FN Thomson Reuters Web of Science™ VR 1.0 PT J AU Schunck, N McDonnell, JD Higdon, D Sarich, J Wild, S AF Schunck, N. McDonnell, J. D. Higdon, D. Sarich, J. Wild, S. TI Quantification of Uncertainties in Nuclear Density Functional Theory SO NUCLEAR DATA SHEETS LA English DT Article; Proceedings Paper CT International Workshop on Nuclear Data Covariances CY APR 28-MAY 01, 2014 CL Santa Fe, NM ID MODELS AB Reliable predictions of nuclear properties are needed as much to answer fundamental science questions as in applications such as reactor physics or data evaluation. Nuclear density functional theory is currently the only microscopic, global approach to nuclear structure that is applicable throughout the nuclear chart. In the past few years, a lot of effort has been devoted to setting up a general methodology to assess theoretical uncertainties in nuclear DFT calculations. In this paper, we summarize some of the recent progress in this direction. Most of the new material discussed here will be be published in separate articles. C1 [Schunck, N.; McDonnell, J. D.] Lawrence Livermore Natl Lab, Div Phys, Livermore, CA 94551 USA. [Higdon, D.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Sarich, J.; Wild, S.] Argonne Natl Lab, Div Math & Comp Sci, Argonne, IL 60439 USA. RP Schunck, N (reprint author), Lawrence Livermore Natl Lab, Div Phys, Livermore, CA 94551 USA. EM schunck1@llnl.gov RI Wild, Stefan/P-4907-2016; OI Wild, Stefan/0000-0002-6099-2772; Schunck, Nicolas/0000-0002-9203-6849 FU U.S. Department of Energy by LLNL [DE-AC52-07NA27344]; SciDAC activity within the U.S. Department of Energy, Office of Science, Advanced Scientific Computing Research program [DE-AC02-06CH11357]; National Center for Computational Sciences (NCCS); National Institute for Computational Sciences (NICS) at ORNL; Livermore Computing Resource Center at LLNL; Laboratory Computing Resource Center at ANL FX This work was partly performed under the auspices of the U.S. Department of Energy by LLNL under Contract DE-AC52-07NA27344. It was supported by the SciDAC activity within the U.S. Department of Energy, Office of Science, Advanced Scientific Computing Research program under contract number DE-AC02-06CH11357. Computational resources were provided through an INCITE award "Computational Nuclear Structure" by the National Center for Computational Sciences (NCCS) and National Institute for Computational Sciences (NICS) at ORNL, through an award by the Livermore Computing Resource Center at LLNL, and through an award by the Laboratory Computing Resource Center at ANL. NR 34 TC 1 Z9 1 U1 0 U2 1 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 0090-3752 EI 1095-9904 J9 NUCL DATA SHEETS JI Nucl. Data Sheets PD JAN PY 2015 VL 123 SI SI BP 115 EP 118 DI 10.1016/j.nds.2014.12.020 PG 4 WC Physics, Nuclear SC Physics GA AZ8UU UT WOS:000348490700022 ER PT J AU Pritychenko, B AF Pritychenko, B. TI Calculations of Nuclear Astrophysics and Californium Fission Neutron Spectrum Averaged Cross Section Uncertainties Using ENDF/B-VII.1, JEFF-3.1.2, JENDL-4.0 and Low-fidelity Covariances SO NUCLEAR DATA SHEETS LA English DT Article; Proceedings Paper CT International Workshop on Nuclear Data Covariances CY APR 28-MAY 01, 2014 CL Santa Fe, NM ID DATA LIBRARY; SCIENCE; COLLABORATION; TECHNOLOGY AB Nuclear astrophysics and californium fission neutron spectrum averaged cross sections and their uncertainties for ENDF materials have been calculated. Absolute values were deduced with Maxwellian and Mannhart spectra, while uncertainties are based on ENDF/B-VII.1, JEFF-3.1.2, JENDL-4.0 and Low-Fidelity covariances. These quantities are compared with available data, independent benchmarks, EXFOR library, and analyzed for a wide range of cases. Recommendations for neutron cross section covariances are given and implications are discussed. C1 Brookhaven Natl Lab, Natl Nucl Data Ctr, Upton, NY 11973 USA. RP Pritychenko, B (reprint author), Brookhaven Natl Lab, Natl Nucl Data Ctr, Upton, NY 11973 USA. EM pritychenko@bnl.gov FU Office of Nuclear Physics, US DoE [DE-AC02-98CH10886]; Brookhaven Science Associates, LLC FX The author thanks M. Herman (BNL) for support of this work, R. Capote, A. Trkov and V. Zerkin (IAEA) for help with Mannhart spectra and data processing, and Mrs. M. Blennau (BNL) for careful reading of the manuscript and useful suggestions. Work at BNL was funded by the Office of Nuclear Physics, US DoE under Contract No. DE-AC02-98CH10886 with Brookhaven Science Associates, LLC. NR 13 TC 1 Z9 1 U1 1 U2 3 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 0090-3752 EI 1095-9904 J9 NUCL DATA SHEETS JI Nucl. Data Sheets PD JAN PY 2015 VL 123 SI SI BP 119 EP 123 DI 10.1016/j.nds.2014.12.021 PG 5 WC Physics, Nuclear SC Physics GA AZ8UU UT WOS:000348490700023 ER PT J AU Tovesson, F AF Tovesson, F. TI Uncertainty Quantification in Fission Cross Section Measurements at LANSCE SO NUCLEAR DATA SHEETS LA English DT Article; Proceedings Paper CT International Workshop on Nuclear Data Covariances CY APR 28-MAY 01, 2014 CL Santa Fe, NM ID CHAMBER AB Neutron-induced fission cross sections have been measured for several isotopes of uranium and plutonium at the Los Alamos Neutron Science Center (LANSCE) over a wide range of incident neutron energies. The total uncertainties in these measurements are in the range 3-5% above 100 keV of incident neutron energy, which results from uncertainties in the target, neutron source, and detector system. The individual sources of uncertainties are assumed to be uncorrelated, however correlation in the cross section across neutron energy bins are considered. The quantification of the uncertainty contributions will be described here. C1 Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Tovesson, F (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM tovesson@lanl.gov FU US Department of Energy; Los Alamos National Security, LLC [DE-AC52-06NA25396] FX This work has benefited from the use of the Los Alamos Neutron Science Center at the Los Alamos National Laboratory. This facility is funded by the US Department of Energy and operated by Los Alamos National Security, LLC under contract DE-AC52-06NA25396. NR 11 TC 0 Z9 0 U1 2 U2 6 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 0090-3752 EI 1095-9904 J9 NUCL DATA SHEETS JI Nucl. Data Sheets PD JAN PY 2015 VL 123 SI SI BP 124 EP 129 DI 10.1016/j.nds.2014.12.022 PG 6 WC Physics, Nuclear SC Physics GA AZ8UU UT WOS:000348490700024 ER PT J AU Haight, RC Wu, CY Lee, HY Taddeucci, TN Perdue, BA O'Donnell, JM Fotiades, N Devlin, M Ullmann, JL Bredeweg, TA Jandel, M Nelson, RO Wender, SA Neudecker, D Rising, ME Mosby, S Sjue, S White, MC Bucher, B Henderson, R AF Haight, R. C. Wu, C. Y. Lee, H. Y. Taddeucci, T. N. Perdue, B. A. O'Donnell, J. M. Fotiades, N. Devlin, M. Ullmann, J. L. Bredeweg, T. A. Jandel, M. Nelson, R. O. Wender, S. A. Neudecker, D. Rising, M. E. Mosby, S. Sjue, S. White, M. C. Bucher, B. Henderson, R. TI The LANL/LLNL Prompt Fission Neutron Spectrum Program at LANSCE and Approach to Uncertainties SO NUCLEAR DATA SHEETS LA English DT Article; Proceedings Paper CT International Workshop on Nuclear Data Covariances CY APR 28-MAY 01, 2014 CL Santa Fe, NM ID QUANTIFICATION; DETECTOR AB New data on the prompt fission neutron spectra (PFNS) from neutron-induced fission with higher accuracies are needed to resolve discrepancies in the literature and to address gaps in the experimental data. The Chi-Nu project, conducted jointly by LANL and LLNL, aims to measure the shape of the PFNS for fission of Pu-239 induced by neutrons from 0.5 to 20 MeV with accuracies of 3-5% in the outgoing energy from 0.1 to 9 MeV and 15% from 9 to 12 MeV and to provide detailed experimental uncertainties. Neutrons from the WNR/LANSCE neutron source are being used to induce fission in a Parallel-Plate Avalanche Counter (PPAC). Two arrays of neutron detectors are used to cover the energy range of neutrons emitted promptly in the fission process. Challenges for the present experiment include background reduction, use of Pu-239 in a PPAC, and understanding neutron detector response. Achieving the target accuracies requires the understanding of many systematic uncertainties. The status and plans for the future will be presented. C1 [Haight, R. C.; Lee, H. Y.; Taddeucci, T. N.; Perdue, B. A.; O'Donnell, J. M.; Fotiades, N.; Devlin, M.; Ullmann, J. L.; Bredeweg, T. A.; Jandel, M.; Nelson, R. O.; Wender, S. A.; Neudecker, D.; Rising, M. E.; Mosby, S.; Sjue, S.; White, M. C.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Wu, C. Y.; Bucher, B.; Henderson, R.] Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. RP Haight, RC (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM haight@lanl.gov RI Devlin, Matthew/B-5089-2013; OI Devlin, Matthew/0000-0002-6948-2154; Fotiadis, Nikolaos/0000-0003-1410-3871; White, Morgan/0000-0003-3876-421X; Wender, Stephen/0000-0002-2446-5115 FU U.S. Department of Energy by Los Alamos National Laboratory [DE-AC52-06NA25396]; Lawrence Livermore National Laboratory [DE-AC52-07NA27344] FX This work was performed under the auspices of the U.S. Department of Energy by Los Alamos National Laboratory under Contract DE-AC52-06NA25396 and the Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344. The experiment benefits from the use of neutrons at the Los Alamos Neutron Science Center. NR 16 TC 3 Z9 3 U1 0 U2 9 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 0090-3752 EI 1095-9904 J9 NUCL DATA SHEETS JI Nucl. Data Sheets PD JAN PY 2015 VL 123 SI SI BP 130 EP 134 DI 10.1016/j.nds.2014.12.023 PG 5 WC Physics, Nuclear SC Physics GA AZ8UU UT WOS:000348490700025 ER PT J AU Taddeucci, TN Haight, RC Lee, HY Neudecker, D O'Donnell, JM White, MC Perdue, BA Devlin, M Fotiadis, N Ullmann, JL Nelson, RO Bredeweg, TA Rising, ME Sjue, SK Wender, SA Wu, CY Henderson, R AF Taddeucci, T. N. Haight, R. C. Lee, H. Y. Neudecker, D. O'Donnell, J. M. White, M. C. Perdue, B. A. Devlin, M. Fotiadis, N. Ullmann, J. L. Nelson, R. O. Bredeweg, T. A. Rising, M. E. Sjue, S. K. Wender, S. A. Wu, C. Y. Henderson, R. TI Multiple-scattering Corrections to Measurements of the Prompt Fission Neutron Spectrum SO NUCLEAR DATA SHEETS LA English DT Article; Proceedings Paper CT International Workshop on Nuclear Data Covariances CY APR 28-MAY 01, 2014 CL Santa Fe, NM ID ENERGY-SPECTRUM; PU-239; CF-252 AB The Chi-Nu project, conducted jointly by LANL and LLNL, aims to measure the shape of the prompt fission neutron spectrum (PFNS) for fission of Pu-239 induced by neutrons from 50 keV to 15 MeV with accuracies of 3-5% in the outgoing energy from 50 keV to 9 MeV and 15% from 9 to 15 MeV. In order to meet this goal, detailed Monte Carlo simulations are being used to assess the importance and effect of every component in the experimental configuration. As part of this effort, we have also simulated some past PFNS measurements to identify possible sources of systematic error. We find that multiple scattering plays an important role in the target geometry, collimators, and detector response and that past experiments probably underestimated the extent of this effect. C1 [Taddeucci, T. N.; Haight, R. C.; Lee, H. Y.; Neudecker, D.; O'Donnell, J. M.; White, M. C.; Perdue, B. A.; Devlin, M.; Fotiadis, N.; Ullmann, J. L.; Nelson, R. O.; Bredeweg, T. A.; Rising, M. E.; Sjue, S. K.; Wender, S. A.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Wu, C. Y.; Henderson, R.] Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. RP Taddeucci, TN (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM taddeucci@lanl.gov RI Devlin, Matthew/B-5089-2013; OI Devlin, Matthew/0000-0002-6948-2154; Fotiadis, Nikolaos/0000-0003-1410-3871; White, Morgan/0000-0003-3876-421X; Wender, Stephen/0000-0002-2446-5115 FU U.S. Department of Energy by Lawrence Livermore National Laboratory [DE-AC52-07NA27344]; Los Alamos National Laboratory [DE-AC52-06NA25396] FX This work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344 and the Los Alamos National Laboratory under Contract DE-AC52-06NA25396. NR 12 TC 9 Z9 9 U1 0 U2 4 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 0090-3752 EI 1095-9904 J9 NUCL DATA SHEETS JI Nucl. Data Sheets PD JAN PY 2015 VL 123 SI SI BP 135 EP 139 DI 10.1016/j.nds.2014.12.024 PG 5 WC Physics, Nuclear SC Physics GA AZ8UU UT WOS:000348490700026 ER PT J AU Burr, T Hoover, A Croft, S Rabin, M AF Burr, T. Hoover, A. Croft, S. Rabin, M. TI Exploring the Impact of Nuclear Data Uncertainties in Ultra-high Resolution Gamma Spectroscopy for Isotopic Analysis Using Approximate Bayesian Computation SO NUCLEAR DATA SHEETS LA English DT Article; Proceedings Paper CT International Workshop on Nuclear Data Covariances CY APR 28-MAY 01, 2014 CL Santa Fe, NM AB High purity germanium (HPGe) currently provides the highest readily available resolution gamma detection for a broad range of radiation measurements, but microcalorimetry is a developing option that has considerably higher resolution even than HPGe. Superior microcalorimetry resolution offers the potential to better distinguish closely spaced X-rays and gamma-rays, a common challenge for the low energy spectral region near 100 keV from special nuclear materials, and the higher signal-to-background ratio also confers an advantage in detection limit. As microcalorimetry continues to develop, it is timely to assess the impact of uncertainties in detector and item response functions and in basic nuclear data, such as branching ratios and half-lives, used to interpret spectra in terms of the contributory radioactive isotopes. We illustrate that a new inference option known as approximate Bayesian computation (ABC) is effective and convenient both for isotopic inference and for uncertainty quantification for microcalorimetry. The ABC approach opens a pathway to new and more powerful implementations for practical applications than currently available. C1 [Burr, T.; Hoover, A.; Rabin, M.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Croft, S.] Oak Ridge Natl Lab, Oak Ridge, TN USA. RP Burr, T (reprint author), Los Alamos Natl Lab, Los Alamos, NM 87545 USA. EM tburr@lanl.gov FU Office of Defense Nuclear Nonproliferation Research and Development FX Office of Defense Nuclear Nonproliferation Research and Development funded this work. NR 10 TC 2 Z9 2 U1 1 U2 5 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 0090-3752 EI 1095-9904 J9 NUCL DATA SHEETS JI Nucl. Data Sheets PD JAN PY 2015 VL 123 SI SI BP 140 EP 145 DI 10.1016/j.nds.2014.12.025 PG 6 WC Physics, Nuclear SC Physics GA AZ8UU UT WOS:000348490700027 ER PT J AU Neudecker, D Talou, P Taddeucci, TN Haight, RC Kawano, T Lee, HY Smith, DL Capote, R Rising, ME White, MC AF Neudecker, D. Talou, P. Taddeucci, T. N. Haight, R. C. Kawano, T. Lee, H. Y. Smith, D. L. Capote, R. Rising, M. E. White, M. C. TI Preliminary Evaluation and Uncertainty Quantification of the Prompt Fission Neutron Spectrum of Pu-239 SO NUCLEAR DATA SHEETS LA English DT Article; Proceedings Paper CT International Workshop on Nuclear Data Covariances CY APR 28-MAY 01, 2014 CL Santa Fe, NM ID NUCLEAR-DATA; MODEL AB Low evaluated uncertainties were obtained in a previous evaluation of the (PU)-P-239 prompt fission neutron spectrum and associated covariances for incident neutrons of 0.5 MeV, which were enlarged a-posteriori before being incorporated into ENDF/B-VII.1. These low evaluated uncertainties triggered an in-depth study and improved estimate of experimental as well as model uncertainties. Here, we will summarize these efforts and show that the improved estimate of experimental and model uncertainties leads to corresponding evaluated uncertainties in good agreement with uncertainties obtained in a statistical analysis based primarily on experimental information. C1 [Neudecker, D.; Talou, P.; Kawano, T.] Los Alamos Natl Lab, Div Theoret, T Nucl & Particle Phys Astrophys & Cosmol 2, Los Alamos, NM 87545 USA. [Taddeucci, T. N.; Haight, R. C.; Lee, H. Y.] Los Alamos Natl Lab, LANSCE NS Neutron & Nucl Sci, Los Alamos, NM 87545 USA. [Smith, D. L.] Argonne Natl Lab, Nucl Engn Div, Coronado, CA 92118 USA. [Capote, R.] IAEA, Nucl Data Sect, A-1400 Vienna, Austria. [Rising, M. E.; White, M. C.] Los Alamos Natl Lab, Div X, Los Alamos, NM 87545 USA. RP Neudecker, D (reprint author), Los Alamos Natl Lab, Div Theoret, T Nucl & Particle Phys Astrophys & Cosmol 2, POB 1663, Los Alamos, NM 87545 USA. EM dneudecker@lanl.gov RI Capote Noy, Roberto/M-1245-2014 OI Capote Noy, Roberto/0000-0002-1799-3438 FU NNSA, US DoE [DE-AC52-06NA25396] FX Work at LANL was sponsored by the NNSA, US DoE under Contract No. DE-AC52-06NA25396. NR 27 TC 5 Z9 5 U1 0 U2 3 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 0090-3752 EI 1095-9904 J9 NUCL DATA SHEETS JI Nucl. Data Sheets PD JAN PY 2015 VL 123 SI SI BP 146 EP 152 DI 10.1016/j.nds.2014.12.026 PG 7 WC Physics, Nuclear SC Physics GA AZ8UU UT WOS:000348490700028 ER PT J AU Kunieda, S Kawano, T Paris, M Hale, GM Shibata, K Fukahori, T AF Kunieda, S. Kawano, T. Paris, M. Hale, G. M. Shibata, K. Fukahori, T. TI Covariance of Neutron Cross Sections for O-16 through R-matrix Analysis SO NUCLEAR DATA SHEETS LA English DT Article; Proceedings Paper CT International Workshop on Nuclear Data Covariances CY APR 28-MAY 01, 2014 CL Santa Fe, NM ID SCIENCE; OXYGEN AB Through the R-matrix analysis, neutron cross sections as well as the covariance are estimated for O-16 in the resolved resonance range. Although we consider the current results are still preliminary, we present the summary of the cross section analysis and the results of data uncertainty/covariance, including those for the differential cross sections. It is found that the values obtained highlight consequences of nature in the theory as well as knowledge from measurements, which gives a realistic quantification of evaluated nuclear data covariances. C1 [Kunieda, S.; Shibata, K.; Fukahori, T.] Japan Atom Energy Agcy, Tokai, Ibaraki 3191195, Japan. [Kawano, T.; Paris, M.; Hale, G. M.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Kunieda, S (reprint author), Japan Atom Energy Agcy, Tokai, Ibaraki 3191195, Japan. EM kunieda.satoshi@jaea.go.jp NR 22 TC 2 Z9 2 U1 1 U2 3 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 0090-3752 EI 1095-9904 J9 NUCL DATA SHEETS JI Nucl. Data Sheets PD JAN PY 2015 VL 123 SI SI BP 159 EP 164 DI 10.1016/j.nds.2014.12.028 PG 6 WC Physics, Nuclear SC Physics GA AZ8UU UT WOS:000348490700030 ER PT J AU Hale, GM Paris, MW AF Hale, G. M. Paris, M. W. TI Data Covariances from R-Matrix Analyses of Light Nuclei SO NUCLEAR DATA SHEETS LA English DT Article; Proceedings Paper CT International Workshop on Nuclear Data Covariances CY APR 28-MAY 01, 2014 CL Santa Fe, NM ID CROSS-SECTION MEASUREMENTS; WHITE NEUTRON SOURCE; SCATTERING; CARBON; RANGE AB After first reviewing the parametric description of light-element reactions in multichannel systems using R-matrix theory and features of the general LANL R-matrix analysis code EDA, we describe how its chi-square minimization procedure gives parameter covariances. This information is used, together with analytically calculated sensitivity derivatives, to obtain cross section covariances for all reactions included in the analysis by first-order error propagation. Examples are given of the covariances obtained for systems with few resonances (He-5) and with many resonances (C-13). We discuss the prevalent problem of this method leading to cross section uncertainty estimates that are unreasonably small for large data sets. The answer to this problem appears to be using parameter confidence intervals in place of standard errors. C1 [Hale, G. M.; Paris, M. W.] Los Alamos Natl Lab, Div Theoret, T Nucl & Particle Phys Astrophys & Cosmol 2, Los Alamos, NM 87545 USA. RP Hale, GM (reprint author), Los Alamos Natl Lab, Div Theoret, T Nucl & Particle Phys Astrophys & Cosmol 2, Los Alamos, NM 87545 USA. EM ghale@lanl.gov OI Paris, Mark/0000-0003-0471-7896 FU NNSA, US DoE [DE-AC52-06NA25396] FX Work sponsored by the NNSA, US DoE, under Contract No. DE-AC52-06NA25396. NR 25 TC 0 Z9 0 U1 0 U2 0 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 0090-3752 EI 1095-9904 J9 NUCL DATA SHEETS JI Nucl. Data Sheets PD JAN PY 2015 VL 123 SI SI BP 165 EP 170 DI 10.1016/j.nds.2014.12.029 PG 6 WC Physics, Nuclear SC Physics GA AZ8UU UT WOS:000348490700031 ER PT J AU Zerovnik, G Trkov, A Kodeli, IA Capote, R Smith, DL AF Zerovnik, G. Trkov, A. Kodeli, I. A. Capote, R. Smith, D. L. TI Random Sampling of Correlated Parameters - a Consistent Solution for Unfavourable Conditions SO NUCLEAR DATA SHEETS LA English DT Article; Proceedings Paper CT International Workshop on Nuclear Data Covariances CY APR 28-MAY 01, 2014 CL Santa Fe, NM ID LARGE UNCERTAINTIES; CROSS-SECTIONS; NUCLEAR-DATA; COVARIANCES AB Two methods for random sampling according to a multivariate lognormal distribution - the correlated sampling method and the method of transformation of correlation coefficients - are briefly presented. The methods are mathematically exact and enable consistent sampling of correlated inherently positive parameters with given information on the first two distribution moments. Furthermore, a weighted sampling method to accelerate the convergence of parameters with extremely large relative uncertainties is described. However, the method is efficient only for a limited number of correlated parameters. C1 [Zerovnik, G.; Trkov, A.; Kodeli, I. A.] Jozef Stefan Inst, SI-1000 Ljubljana, Slovenia. [Trkov, A.; Capote, R.] IAEA, A-1400 Vienna, Austria. [Smith, D. L.] Argonne Natl Lab, Coronado, CA 92118 USA. RP Zerovnik, G (reprint author), Jozef Stefan Inst, Jamova Cesta 39, SI-1000 Ljubljana, Slovenia. EM gasper.zerovnik@ijs.si RI Capote Noy, Roberto/M-1245-2014 OI Capote Noy, Roberto/0000-0002-1799-3438 FU Slovenian Research Agency (ARRS) FX This research was partly supported by the Slovenian Research Agency (ARRS). NR 19 TC 2 Z9 2 U1 0 U2 1 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 0090-3752 EI 1095-9904 J9 NUCL DATA SHEETS JI Nucl. Data Sheets PD JAN PY 2015 VL 123 SI SI BP 185 EP 190 DI 10.1016/j.nds.2014.12.032 PG 6 WC Physics, Nuclear SC Physics GA AZ8UU UT WOS:000348490700034 ER PT J AU Pigni, MT Francis, MW Gauld, IC AF Pigni, M. T. Francis, M. W. Gauld, I. C. TI Investigation of Inconsistent ENDF/B-VII.1 Independent and Cumulative Fission Product Yields with Proposed Revisions SO NUCLEAR DATA SHEETS LA English DT Article; Proceedings Paper CT International Workshop on Nuclear Data Covariances CY APR 28-MAY 01, 2014 CL Santa Fe, NM AB A recent implementation of ENDF/B-VII.1 independent fission product yields and nuclear decay data identified inconsistencies in the data caused by the use of updated nuclear schemes in the decay sub-library that are not reflected in legacy fission product yield data. Recent changes in the decay data sub-library, particularly the delayed neutron branching fractions result in calculated fission product concentrations that do not agree with the cumulative fission yields in the library as well as with experimental measurements. To address these issues, a comprehensive set of independent fission product yields was generated for thermal and fission spectrum neutron-induced fission for U-235,U-238 and Pu-239,Pu-241 in order to provide a preliminary assessment of the updated fission product yield data consistency. These updated independent fission product yields were utilized in the ORIGEN code to compare the calculated fission product inventories with experimentally measured inventories, with particular attention given to the noble gases. Another important outcome of this work is the development of fission product yield covariance data necessary for fission product uncertainty quantification. The evaluation methodology combines a sequential Bayesian method to guarantee consistency between independent and cumulative yields along with the physical constraints on the independent yields. This work was motivated to improve the performance of the ENDF/B-VII.1 library for stable and long-lived fission products. The revised fission product yields and the new covariance data are proposed as a revision to the fission yield data currently in ENDF/B-VII.1. C1 [Pigni, M. T.; Francis, M. W.; Gauld, I. C.] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. RP Pigni, MT (reprint author), Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. EM pignimt@ornl.gov OI Gauld, Ian/0000-0002-3893-7515 FU Defense Threat Reduction Agency Office of Nuclear Forensics Materials Collection, Analysis, Debris Diagnostics Branch; National Nuclear Security Administration, Office of Defense Nuclear Nonproliferation Research and Development FX This work was funded by the Defense Threat Reduction Agency Office of Nuclear Forensics Materials Collection, Analysis, Debris Diagnostics Branch, and the National Nuclear Security Administration, Office of Defense Nuclear Nonproliferation Research and Development. NR 10 TC 4 Z9 4 U1 1 U2 4 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 0090-3752 EI 1095-9904 J9 NUCL DATA SHEETS JI Nucl. Data Sheets PD JAN PY 2015 VL 123 SI SI BP 231 EP 236 DI 10.1016/j.nds.2014.12.040 PG 6 WC Physics, Nuclear SC Physics GA AZ8UU UT WOS:000348490700042 ER PT J AU Sohlberg, K Pennycook, TJ Zhou, W Pennycook, SJ AF Sohlberg, Karl Pennycook, Timothy J. Zhou, Wu Pennycook, Stephen J. TI Insights into the physical chemistry of materials from advances in HAADF-STEM SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Editorial Material ID TRANSMISSION ELECTRON-MICROSCOPY; CADMIUM SELENIDE NANOCRYSTALS; METAL-OXIDE CATALYSTS; HIGH-RESOLUTION; Z-CONTRAST; CDSE NANOCRYSTALS; QUANTUM DOTS; ABERRATION CORRECTION; RHODIUM SESQUIOXIDE; GOLD NANOCLUSTERS AB The observation that, New tools lead to new science[P. S. Weiss, ACS Nano., 2012, 6(3), 18771879], is perhaps nowhere more evident than in scanning transmission electron microscopy (STEM). Advances in STEM have endowed this technique with several powerful and complimentary capabilities. For example, the application of high-angle annular dark-field imaging has made possible real-space imaging at sub-angstrom resolution with Z-contrast (Z = atomic number). Further advances have wrought: simultaneous real-space imaging and elemental identification by using electron energy loss spectroscopy (EELS); 3-dimensional (3D) mapping by depth sectioning; monitoring of surface diffusion by time-sequencing of images; reduced electron energy imaging for probing graphenes; etc. In this paper we review how these advances, often coupled with first-principles theory, have led to interesting and important new insights into the physical chemistry of materials. We then review in detail a few specific applications that highlight some of these STEM capabilities. C1 [Sohlberg, Karl] Drexel Univ, Dept Chem, Philadelphia, PA 19104 USA. [Pennycook, Timothy J.] SuperSTEM Lab, Daresbury, Cheshire, England. [Pennycook, Timothy J.] Univ Oxford, Dept Mat, Oxford OX1 3PH, England. [Zhou, Wu] Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN 37831 USA. [Pennycook, Stephen J.] Univ Tennessee, Dept Mat Sci & Engn, Knoxville, TN 37996 USA. RP Pennycook, SJ (reprint author), Univ Tennessee, Dept Mat Sci & Engn, Knoxville, TN 37996 USA. EM spennyco@utk.edu RI Zhou, Wu/D-8526-2011; Pennycook, Timothy/B-4946-2014 OI Zhou, Wu/0000-0002-6803-1095; Pennycook, Timothy/0000-0002-0008-6516 NR 131 TC 7 Z9 7 U1 11 U2 84 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2015 VL 17 IS 6 BP 3982 EP 4006 DI 10.1039/c4cp04232h PG 25 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA CA6FR UT WOS:000349005900003 PM 25586364 ER PT J AU Rouha, M Cummings, PT AF Rouha, Michael Cummings, Peter T. TI Thickness-dependent structural arrangement in nano-confined imidazolium-based ionic liquid films SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID ROOM-TEMPERATURE; MOLECULAR-DYNAMICS; VIBRATIONAL SPECTROSCOPY; CARBON SUPERCAPACITORS; INTERFACES; SURFACE; HETEROGENEITY; SIMULATION; SCATTERING AB A fundamental understanding of interfacial processes in nano-confined ionic liquids is crucial to increase the performance of modern energy storage devices. It is well-known that interfaces between electrodes and ionic liquids exhibit structures distinct from that of the bulk liquid. Following the recent interest in these systems, we studied the structure of thin ionic liquid films confined in flexible uncharged carbon nano-pores by using fully-atomistic molecular dynamics simulations. We show that the interfacial ions self-assemble into a closely-packed chequerboard-like pattern, formed by both cations and anions in direct contact with the pore wall, and that within this structure we find changes dependent on the thickness of the confined films. At low coverages a dense layer is formed in which both the imidazolium-ring and its alkyl-tail lie parallel to the pore wall. With increasing coverage the alkyl-chains reorient perpendicular to the surface, making space for additional ions until a densified highly ordered layer is formed. This wall-induced self-patterning into interfacial layers with significantly higher than bulk density is consistent with recent experimental and theoretical studies of similar systems. This work reveals additional molecular-level details on the effect of the film-thickness on the structure and density of the ionic liquid. C1 [Rouha, Michael; Cummings, Peter T.] Vanderbilt Univ, Dept Chem & Biomol Engn, Nashville, TN 37235 USA. [Rouha, Michael] Tech Univ Liberec, Inst Nanomat Adv Technol & Innovat, Liberec, Czech Republic. [Cummings, Peter T.] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN USA. RP Rouha, M (reprint author), Vanderbilt Univ, Dept Chem & Biomol Engn, 221 Kirkland Hall, Nashville, TN 37235 USA. EM michael.rouha@tul.cz; peter.cummings@vanderbilt.edu RI Rouha, Michael/N-8187-2013 OI Rouha, Michael/0000-0002-4227-4005 FU Fluid Interface Reactions, Structures and Transport (FIRST) Center, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences; Ministry of Education, Youth and Sports; OPR&DI project Centre for Nanomaterials, Advanced Technologies and Innovation [CZ.1.05/2.1.00/01.0005]; Project Development of Research Teams of R&D Projects at the Technical University of Liberec [CZ.1.07/2.3.00/30.0024] FX This material is based upon work supported as part of the Fluid Interface Reactions, Structures and Transport (FIRST) Center, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences. This research used resources of the National Energy Research Scientific Computing Center. M. R. was in part supported by the Ministry of Education, Youth and Sports in the framework of the targeted support of the National Programme for Sustainability I, the OPR&DI project Centre for Nanomaterials, Advanced Technologies and Innovation CZ.1.05/2.1.00/01.0005 and the Project Development of Research Teams of R&D Projects at the Technical University of Liberec CZ.1.07/2.3.00/30.0024. NR 38 TC 7 Z9 7 U1 5 U2 57 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2015 VL 17 IS 6 BP 4152 EP 4159 DI 10.1039/c4cp05138f PG 8 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA CA6FR UT WOS:000349005900023 PM 25563888 ER PT J AU Pandey, TP Maes, AM Sarode, HN Peters, BD Lavina, S Vezzu, K Yang, Y Poynton, SD Varcoe, JR Seifert, S Liberatore, MW Di Notob, V Herring, AM AF Pandey, Tara P. Maes, Ashley M. Sarode, Himanshu N. Peters, Bethanne D. Lavina, Sandra Vezzu, Keti Yang, Yuan Poynton, Simon D. Varcoe, John R. Seifert, Soenke Liberatore, Matthew W. Di Noto, Vito Herring, Andrew M. TI Interplay between water uptake, ion interactions, and conductivity in an e-beam grafted poly(ethylene-co-tetrafluoroethylene) anion exchange membrane SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID ELECTROLYTE FUEL-CELLS; TRANSPORT-PROPERTIES; AQUEOUS-SOLUTION; CARBON-DIOXIDE; HYDROXIDE; HYDRATION; CHLORIDE; TEMPERATURE; MOLECULES; MECHANISM AB We demonstrate that the true hydroxide conductivity in an e-beam grafted poly(ethylene-co-tetrafluoroethylene) [ETFE] anion exchange membrane (AEM) is as high as 132 mS cm(-1) at 80 degrees C and 95% RH, comparable to a proton exchange membrane, but with very much less water present in the film. To understand this behaviour we studied ion transport of hydroxide, carbonate, bicarbonate and chloride, as well as water uptake and distribution. Water uptake of the AEM in water vapor is an order of magnitude lower than when submerged in liquid water. In addition F-19 pulse field gradient spin echo NMR indicates that there is little tortuosity in the ionic pathways through the film. A complete analysis of the IR spectrum of the AEM and the analyses of water absorption using FT-IR led to conclusion that the fluorinated backbone chains do not interact with water and that two types of water domains exist within the membrane. The reduction in conductivity was measured during exposure of the OH- form of the AEM to air at 95% RH and was seen to be much slower than the reaction of CO2 with OH- as the amount of water in the film determines its ionic conductivity and at relative wet RHs its re-organization is slow. C1 [Pandey, Tara P.; Maes, Ashley M.; Sarode, Himanshu N.; Peters, Bethanne D.; Liberatore, Matthew W.; Herring, Andrew M.] Colorado Sch Mines, Dept Chem & Biol Engn, Golden, CO 80401 USA. [Lavina, Sandra; Vezzu, Keti; Di Noto, Vito] Univ Padua, Dept Chem Sci, I-35131 Padua, Italy. [Vezzu, Keti] Veneto Nanotech, I-351329 Padua, Italy. [Yang, Yuan] Colorado Sch Mines, Dept Chem & Geochem, Golden, CO 80401 USA. [Poynton, Simon D.; Varcoe, John R.] Univ Surrey, Dept Chem, Guildford GU27XH, Surrey, England. [Seifert, Soenke] Xray Sci Div, Argonne Natl Lab, Argonne, IL 60439 USA. RP Herring, AM (reprint author), Colorado Sch Mines, Dept Chem & Biol Engn, Golden, CO 80401 USA. EM aherring@mines.edu RI Liberatore, Matthew/B-6828-2008; OI DI NOTO, VITO/0000-0002-8030-6979; Poynton, Simon/0000-0001-5453-3871; Herring, Andrew/0000-0001-7318-5999; Varcoe, John/0000-0001-9898-0235 FU Army Research Office for support of this research under the MURI program [W911NF-11-1-0462]; Colorado School of Mines NMR facility - National Science Foundation under the an MRI grant [CHE-0923537]; EPSRC [EP/I004882/1]; Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory [DE-AC02-06CH11357] FX The authors would like to thank the Army Research Office for support of this research under the MURI program, grant W911NF-11-1-0462, and The Colorado School of Mines NMR facility funded by National Science Foundation under the an MRI grant CHE-0923537. The anion-exchange membranes were fabricated and characterized using funds from EPSRC Grant EP/I004882/1. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. NR 46 TC 17 Z9 17 U1 10 U2 74 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2015 VL 17 IS 6 BP 4367 EP 4378 DI 10.1039/c4cp05755d PG 12 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA CA6FR UT WOS:000349005900047 PM 25578464 ER PT J AU Wiegel, AA Wilson, KR Hinsberg, WD Houle, FA AF Wiegel, A. A. Wilson, K. R. Hinsberg, W. D. Houle, F. A. TI Stochastic methods for aerosol chemistry: a compact molecular description of functionalization and fragmentation in the heterogeneous oxidation of squalane aerosol by OH radicals SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID VOLATILE ORGANIC-COMPOUNDS; SELF-REACTION KINETICS; AQUEOUS-SOLUTION; PEROXY-RADICALS; RATE CONSTANTS; ATMOSPHERIC CHEMISTRY; HYDROXYL RADICALS; CHEMICAL-REACTIONS; MASS-SPECTROMETRY; CL ATOMS AB The heterogeneous oxidation of organic aerosol by hydroxyl radicals (OH) can proceed through two general pathways: functionalization, in which oxygen functional groups are added to the carbon skeleton, and fragmentation, in which carbon-carbon bonds are broken, producing higher volatility, lower molecular weight products. An ongoing challenge is to develop a quantitative molecular description of these pathways that connects the oxidative evolution of the average aerosol properties (e.g. size and hygroscopicity) to the transformation of free radical intermediates. In order to investigate the underlying molecular mechanism of aerosol oxidation, a relatively compact kinetics model is developed for the heterogeneous oxidation of squalane particles by OH using free radical intermediates that convert reactive hydrogen sites into oxygen functional groups. Stochastic simulation techniques are used to compare calculated system properties over ten oxidation lifetimes with the same properties measured in experiment. The time-dependent average squalane aerosol mass, volume, density, carbon number distribution of scission products, and the average elemental composition are predicted using known rate coefficients. For functionalization, the calculations reveal that the distribution of alcohol and carbonyl groups is controlled primarily by the initial OH abstraction rate and to lesser extent by the branching ratio between secondary peroxy radical product channels. For fragmentation, the calculations reveal that the formation of activated alkoxy radicals with neighboring functional groups controls the molecular decomposition, particularly at high O/C ratios. This kinetic scheme provides a framework for understanding the oxidation chemistry of a model organic aerosol and informs parameterizations of more complex systems. C1 [Wiegel, A. A.; Wilson, K. R.; Houle, F. A.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. [Hinsberg, W. D.] Columbia Hill Tech Consulting, Fremont, CA 94539 USA. RP Wilson, KR (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. EM krwilson@lbl.gov; fahoule@lbl.gov FU Laboratory Directed Research and Development Program of the Department of Energy's Lawrence Berkeley National Laboratory under U.S. Department of Energy Office of Science, Office of Basic Energy Sciences [DE-AC02-05CH11231]; Department of Energy's Office of Science Early Career Research Program; Chemical Sciences Division of the U.S. Department of Energy [DE-AC02-05CH11231]; CHTC FX This material is based upon work supported by the Laboratory Directed Research and Development Program of the Department of Energy's Lawrence Berkeley National Laboratory under U.S. Department of Energy Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-05CH11231. Results were used from past K.R.W. work supported by the Department of Energy's Office of Science Early Career Research Program and by Chemical Sciences Division of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. W.D.H. is supported by CHTC. Special thanks to B. Kirk for help with electronic structure calculations. NR 59 TC 10 Z9 10 U1 6 U2 45 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2015 VL 17 IS 6 BP 4398 EP 4411 DI 10.1039/c4cp04927f PG 14 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA CA6FR UT WOS:000349005900050 PM 25578323 ER PT J AU Houle, FA Hinsberg, WD Wilson, KR AF Houle, F. A. Hinsberg, W. D. Wilson, K. R. TI Oxidation of a model alkane aerosol by OH radical: the emergent nature of reactive uptake SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID SECONDARY ORGANIC AEROSOL; GAS-LIQUID INTERFACES; HETEROGENEOUS OXIDATION; ATMOSPHERIC AEROSOLS; CHEMICAL-REACTIONS; HYDROXYL RADICALS; KINETIC LIMITATIONS; MASS ACCOMMODATION; PARTICLE-PHASE; DIFFUSION AB An accurate description of the evolution of organic aerosol in the Earth's atmosphere is essential for climate models. However, the complexity of multiphase chemical and physical transformations has been challenging to describe at the level required to predict aerosol lifetimes and changes in chemical composition. In this work a model is presented that reproduces experimental data for the early stages of oxidative aging of squalane aerosol by hydroxyl radical (OH), a process governed by reactive uptake of gas phase species onto the particle surface. Simulations coupling free radical reactions and Fickian diffusion are used to elucidate how the measured uptake coefficient reflects the elementary steps of sticking of OH to the aerosol as a result of a gas-surface collision, followed by very rapid abstraction of hydrogen and subsequent free radical reactions. It is found that the uptake coefficient is not equivalent to a sticking coefficient or an accommodation coefficient: it is an intrinsically emergent process that depends upon particle size, viscosity, and OH concentration. An expression is derived to examine how these factors control reactive uptake over a broad range of atmospheric and laboratory conditions, and is shown to be consistent with simulation results. Well-mixed, liquid behavior is found to depend on the reaction conditions in addition to the nature of the organic species in the aerosol particle. C1 [Houle, F. A.; Wilson, K. R.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. [Hinsberg, W. D.] Columbia Hill Tech Consulting, Columbia, CA 94539 USA. RP Houle, FA (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. EM fahoule@lbl.gov; krwilson@lbl.gov FU Laboratory Directed Research and Development Program of the Department of Energy's Lawrence Berkeley National Laboratory under U.S. Department of Energy Office of Science, Office of Basic Energy Sciences [DE-AC02-05CH11231]; Department of Energy's Office of Science Early Career Research Program; Chemical Sciences Division of the U.S. Department of Energy [DE-AC02-05CH11231]; CHTC FX This material is based upon work supported by the Laboratory Directed Research and Development Program of the Department of Energy's Lawrence Berkeley National Laboratory under U.S. Department of Energy Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-05CH11231. Results were used from past K.R.W. work supported by the Department of Energy's Office of Science Early Career Research Program and by Chemical Sciences Division of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. W.D.H. is supported by CHTC. The authors acknowledge DrMichael Ward for valuable discussions. NR 69 TC 17 Z9 17 U1 7 U2 73 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2015 VL 17 IS 6 BP 4412 EP 4423 DI 10.1039/c4cp05093b PG 12 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA CA6FR UT WOS:000349005900051 PM 25578745 ER PT J AU Mamontov, E Zolnierczuk, P Ohl, M AF Mamontov, E. Zolnierczuk, P. Ohl, M. TI Nanometer-sized dynamic entities in an aqueous system SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID NEUTRON SPIN-ECHO; WATER-MOLECULES; GLASS-TRANSITION; IONIC SOLUTION; CROSSOVER; LICL; SPECTROSCOPY; TEMPERATURES; SPECTROMETER; SCATTERING AB Using neutron spin-echo and backscattering spectroscopy, we have found that at low temperatures water molecules in an aqueous solution engage in center-of-mass dynamics that are different from both the main structural relaxations and the well-known localized motions in the transient cages of the nearest neighbor molecules. While the latter localized motions are known to take place on the picosecond time scale and Angstrom length scale, the slower motions that we have observed are found on the nanosecond time scale and nanometer length scale. They are associated with the slow secondary relaxations, or excess wing dynamics, in glass-forming liquids. Our approach, therefore, can be applied to probe the characteristic length scale of the dynamic entities associated with slow dynamics in glass-forming liquids, which presently cannot be studied by other experimental techniques. C1 [Mamontov, E.] Oak Ridge Natl Lab, Neutron Sci Directorate, Oak Ridge, TN 37831 USA. [Zolnierczuk, P.; Ohl, M.] Oak Ridge Natl Lab, Juelich Ctr Neutron Sci, Outstn Spallat Neutron Source, Oak Ridge, TN 37831 USA. RP Mamontov, E (reprint author), Oak Ridge Natl Lab, Neutron Sci Directorate, Oak Ridge, TN 37831 USA. EM mamontove@ornl.gov RI Mamontov, Eugene/Q-1003-2015 OI Mamontov, Eugene/0000-0002-5684-2675 FU Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. DOE; U.S. DOE [DE-AC05-00OR22725] FX The neutron scattering studies were conducted with support from the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. DOE. Oak Ridge National Laboratory is managed by UT-Battelle, LLC, for U.S. DOE under Contract No. DE-AC05-00OR22725. NR 33 TC 2 Z9 2 U1 3 U2 13 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2015 VL 17 IS 6 BP 4466 EP 4471 DI 10.1039/c4cp05081a PG 6 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA CA6FR UT WOS:000349005900057 PM 25578558 ER PT J AU Grimaldo, M Roosen-Runge, F Hennig, M Zanini, F Zhang, FJ Jalarvo, N Zamponi, M Schreiber, F Seydel, T AF Grimaldo, Marco Roosen-Runge, Felix Hennig, Marcus Zanini, Fabio Zhang, Fajun Jalarvo, Niina Zamponi, Michaela Schreiber, Frank Seydel, Tilo TI Hierarchical molecular dynamics of bovine serum albumin in concentrated aqueous solution below and above thermal denaturation SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID ELASTIC NEUTRON-SCATTERING; NUCLEAR-MAGNETIC-RESONANCE; GLOBULAR PROTEIN GELATION; LIGHT-SCATTERING; COOPERATIVE TRANSITIONS; TEMPERATURE-DEPENDENCE; CONFORMATIONAL-CHANGES; ALPHA-LACTALBUMIN; DIFFUSIVE MOTIONS; INTERNAL DYNAMICS AB The dynamics of proteins in solution is a complex and hierarchical process, affected by the aqueous environment as well as temperature. We present a comprehensive study on nanosecond time and nanometer length scales below, at, and above the denaturation temperature T-d. Our experimental data evidence dynamical processes in protein solutions on three distinct time scales. We suggest a consistent physical picture of hierarchical protein dynamics: (i) self-diffusion of the entire protein molecule is confirmed to agree with colloid theory for all temperatures where the protein is in its native conformational state. At higher temperatures T > T-d, the self-diffusion is strongly obstructed by cross-linking or entanglement. (ii) The amplitude of backbone fluctuations grows with increasing T, and a transition in its dynamics is observed above T-d. (iii) The number of mobile side-chains increases sharply at T-d while their average dynamics exhibits only little variations. The combination of quasi-elastic neutron scattering and the presented analytical framework provides a detailed microscopic picture of the protein molecular dynamics in solution, thereby reflecting the changes of macroscopic properties such as cluster formation and gelation. C1 [Grimaldo, Marco; Roosen-Runge, Felix; Hennig, Marcus; Seydel, Tilo] Inst Max von Laue Paul Langevin ILL, F-38042 Grenoble, France. [Grimaldo, Marco; Hennig, Marcus; Zanini, Fabio; Zhang, Fajun; Schreiber, Frank] Univ Tubingen, Inst Angew Phys, D-72076 Tubingen, Germany. [Zanini, Fabio] Max Planck Inst Dev Biol, D-72076 Tubingen, Germany. [Jalarvo, Niina; Zamponi, Michaela] Forschungszentrum Julich, Julich Ctr Neutron Sci, D-52425 Julich, Germany. [Jalarvo, Niina] Oak Ridge Natl Lab, Chem & Engn Mat Div, Neutron Sci Directorate, Oak Ridge, TN 37831 USA. [Jalarvo, Niina] Oak Ridge Natl Lab, JCNS Outstn, Spallat Neutron Source, Oak Ridge, TN 37831 USA. RP Seydel, T (reprint author), Inst Max von Laue Paul Langevin ILL, CS 20156, F-38042 Grenoble, France. EM seydel@ill.eu RI Roosen-Runge, Felix/A-9107-2013; Schreiber, Frank/J-3311-2014; Jalarvo, Niina/Q-1320-2015 OI Roosen-Runge, Felix/0000-0001-5106-4360; Schreiber, Frank/0000-0003-3659-6718; Jalarvo, Niina/0000-0003-0644-6866 FU Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy; Julich Center for Neutron Science (JCNS), Germany; JCNS; Institut Laue-Langevin (ILL); ILL; DFG FX The research at Oak Ridge National Laboratory's Spallation Neutron Source was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy. The spectrometer BASIS is supported by the Julich Center for Neutron Science (JCNS), Germany, via the partner user programme and M.G. and F.Za. acknowledge travel funding by JCNS to conduct the experiments as well as a student grant by the Institut Laue-Langevin (ILL). M.H., M.G. and T.S. have obtained travel funding by ILL. We acknowledge E. Mamontov, H. Schober and S. Da Vela for fruitful discussion and R. Moody for technical assistance. We further acknowledge financial support by the DFG. NR 82 TC 3 Z9 3 U1 2 U2 28 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2015 VL 17 IS 6 BP 4645 EP 4655 DI 10.1039/c4cp04944f PG 11 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA CA6FR UT WOS:000349005900077 PM 25587698 ER PT J AU Arefiev, AV Cochran, GE Schumacher, DW Robinson, APL Chen, GY AF Arefiev, Alexey V. Cochran, Ginevra E. Schumacher, Douglass W. Robinson, Alexander P. L. Chen, Guangye TI Temporal resolution criterion for correctly simulating relativistic electron motion in a high-intensity laser field SO PHYSICS OF PLASMAS LA English DT Article ID IN-CELL ALGORITHM; PLASMA; BEAMS; GENERATION; IMPLICIT AB Particle-in-cell codes are now standard tools for studying ultra-intense laser-plasma interactions. Motivated by direct laser acceleration of electrons in sub-critical plasmas, we examine temporal resolution requirements that must be satisfied to accurately calculate electron dynamics in strong laser fields. Using the motion of a single electron in a perfect plane electromagnetic wave as a test problem, we show surprising deterioration of the numerical accuracy with increasing wave amplitude a(0) for a given time-step. We go on to show analytically that the time-step must be significantly less than lambda/ca(0) to achieve good accuracy. We thus propose adaptive electron sub-cycling as an efficient remedy. (C) 2015 AIP Publishing LLC. C1 [Arefiev, Alexey V.] Univ Texas Austin, Inst Fus Studies, Austin, TX 78712 USA. [Cochran, Ginevra E.; Schumacher, Douglass W.] Ohio State Univ, Dept Phys, Columbus, OH 43210 USA. [Robinson, Alexander P. L.] STFC Rutherford Appleton Lab, Cent Laser Facil, Didcot OX11 0QX, Oxon, England. [Chen, Guangye] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Arefiev, AV (reprint author), Univ Texas Austin, Inst Fus Studies, Austin, TX 78712 USA. RI Chen, Guangye /K-3192-2012; Schumacher, Douglass/J-3454-2015; Arefiev, Alexey/A-8550-2016; OI Chen, Guangye/0000-0002-8800-5791; Schumacher, Douglass/0000-0002-2171-3902; Arefiev, Alexey/0000-0002-0597-0976; Cochran, Ginevra/0000-0001-8959-8341 FU UK EPSRC [EP/G054940/1, EP/G055165/1, EP/G056803/1]; AFOSR [FA9550-14-1-0045]; National Nuclear Security Administration [DE-FC52-08NA28512]; U.S. Department of Energy [DE-FG02-04ER54742]; NNSA [DE-NA0001976] FX A.V.A. would like to thank Dr. S. P. D. Mangles and Dr. V. N. Khudik for stimulating discussions and constructive comments. Simulations for this paper were performed using the EPOCH code (developed under UK EPSRC Grant Nos. EP/G054940/1, EP/G055165/1, and EP/G056803/1) using HPC resources provided by the Texas Advanced Computing Center at The University of Texas. A. V. A. was supported by AFOSR Contract No. FA9550-14-1-0045, National Nuclear Security Administration Contract No. DE-FC52-08NA28512, and U.S. Department of Energy Contract No. DE- FG02-04ER54742. GEC received support from NNSA Contract No. DE-NA0001976. NR 22 TC 9 Z9 9 U1 2 U2 9 PU AMER INST PHYSICS PI MELVILLE PA 1305 WALT WHITMAN RD, STE 300, MELVILLE, NY 11747-4501 USA SN 1070-664X EI 1089-7674 J9 PHYS PLASMAS JI Phys. Plasmas PD JAN PY 2015 VL 22 IS 1 AR 013103 DI 10.1063/1.4905523 PG 11 WC Physics, Fluids & Plasmas SC Physics GA CA8NQ UT WOS:000349178100041 ER PT J AU Berdanier, W Roy, PK Kaganovich, I AF Berdanier, William Roy, Prabir K. Kaganovich, Igor TI Intense ion beam neutralization using underdense background plasma SO PHYSICS OF PLASMAS LA English DT Article ID ELECTRONS; PULSE AB Producing an overdense background plasma for neutralization purposes with a density that is high compared to the beam density is not always experimentally possible. We show that even an underdense background plasma with a small relative density can achieve high neutralization of intense ion beam pulses. Using particle-in-cell simulations, we show that if the total plasma electron charge is not sufficient to neutralize the beam charge, electron emitters are necessary for effective neutralization but are not needed if the plasma volume is so large that the total available charge in the electrons exceeds that of the ion beam. Several regimes of possible underdense/tenuous neutralization plasma densities are investigated with and without electron emitters or dense plasma at periphery regions, including the case of electron emitters without plasma, which does not effectively neutralize the beam. Over 95% neutralization is achieved for even very underdense background plasma with plasma density 1/15th the beam density. We compare results of particle-in-cell simulations with an analytic model of neutralization and find close agreement with the particle-in-cell simulations. Further, we show experimental data from the National Drift Compression experiment-II group that verifies the result that underdense plasma can neutralize intense heavy ion beams effectively. (C) 2015 AIP Publishing LLC. C1 [Berdanier, William] Univ Texas Austin, Dept Phys, Austin, TX 78712 USA. [Berdanier, William; Kaganovich, Igor] Princeton Univ, Princeton Plasma Phys Lab, Princeton, NJ 08543 USA. [Roy, Prabir K.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Berdanier, W (reprint author), Univ Texas Austin, Dept Phys, Austin, TX 78712 USA. FU National Undergraduate Fellowship Program; Department of Energy; Office of Science of the U.S. Department of Energy [DE-AC0205CH11231] FX The authors are grateful to the Heavy Ion Fusion Science Virtual National Laboratory (HIFS-VNL) scientists, engineers, and technologists for their experimental data. This work was supported by the National Undergraduate Fellowship Program and by the Department of Energy. Work at the Lawrence Berkeley Lab was supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC0205CH11231. NR 31 TC 1 Z9 1 U1 1 U2 5 PU AMER INST PHYSICS PI MELVILLE PA 1305 WALT WHITMAN RD, STE 300, MELVILLE, NY 11747-4501 USA SN 1070-664X EI 1089-7674 J9 PHYS PLASMAS JI Phys. Plasmas PD JAN PY 2015 VL 22 IS 1 AR 013104 DI 10.1063/1.4905631 PG 5 WC Physics, Fluids & Plasmas SC Physics GA CA8NQ UT WOS:000349178100042 ER PT J AU Chung, M Qin, H Groening, L Davidson, RC Xiao, C AF Chung, Moses Qin, Hong Groening, Lars Davidson, Ronald C. Xiao, Chen TI Beam envelope calculations in general linear coupled lattices SO PHYSICS OF PLASMAS LA English DT Article AB The envelope equations and Twiss parameters (beta and alpha) provide important bases for uncoupled linear beam dynamics. For sophisticated beam manipulations, however, coupling elements between two transverse planes are intentionally introduced. The recently developed generalized Courant-Snyder theory offers an effective way of describing the linear beam dynamics in such coupled systems with a remarkably similar mathematical structure to the original Courant-Snyder theory. In this work, we present numerical solutions to the symmetrized matrix envelope equation for b which removes the gauge freedom in the matrix envelope equation for w. Furthermore, we construct the transfer and beam matrices in terms of the generalized Twiss parameters, which enables calculation of the beam envelopes in arbitrary linear coupled systems. (C) 2015 AIP Publishing LLC. C1 [Chung, Moses] Ulsan Natl Inst Sci & Technol, Dept Phys, Ulsan 689798, South Korea. [Qin, Hong; Davidson, Ronald C.] Princeton Univ, Plasma Phys Lab, Princeton, NJ 08543 USA. [Qin, Hong] Univ Sci & Technol China, Dept Modern Phys, Hefei 230026, Anhui, Peoples R China. [Groening, Lars; Xiao, Chen] GSI Helmholtzzentrum Schwerionenforsch GmbH, D-64291 Darmstadt, Germany. RP Chung, M (reprint author), Ulsan Natl Inst Sci & Technol, Dept Phys, Ulsan 689798, South Korea. EM mchung@unist.ac.kr FU UNIST (Ulsan National Institute of Science and Technology) [1.140075.01]; U.S. Department of Energy [DE-AC02-09CH11466] FX This work was supported by the 2014 Research Fund (1.140075.01) of UNIST (Ulsan National Institute of Science and Technology). This work was also supported by the U.S. Department of Energy Grant No. DE-AC02-09CH11466. NR 22 TC 2 Z9 2 U1 4 U2 11 PU AMER INST PHYSICS PI MELVILLE PA 1305 WALT WHITMAN RD, STE 300, MELVILLE, NY 11747-4501 USA SN 1070-664X EI 1089-7674 J9 PHYS PLASMAS JI Phys. Plasmas PD JAN PY 2015 VL 22 IS 1 AR 013109 DI 10.1063/1.4903457 PG 6 WC Physics, Fluids & Plasmas SC Physics GA CA8NQ UT WOS:000349178100047 ER PT J AU Friedman, B Carter, TA AF Friedman, B. Carter, T. A. TI A non-modal analytical method to predict turbulent properties applied to the Hasegawa-Wakatani model SO PHYSICS OF PLASMAS LA English DT Article ID DRIFT-WAVE TURBULENCE; PLASMA TURBULENCE; EDGE TURBULENCE; STABILITY; INSTABILITY; FLOW; TRANSITION AB Linear eigenmode analysis often fails to describe turbulence in model systems that have non-normal linear operators and thus nonorthogonal eigenmodes, which can cause fluctuations to transiently grow faster than expected from eigenmode analysis. When combined with energetically conservative nonlinear mode mixing, transient growth can lead to sustained turbulence even in the absence of eigenmode instability. Since linear operators ultimately provide the turbulent fluctuations with energy, it is useful to define a growth rate that takes into account non-modal effects, allowing for prediction of energy injection, transport levels, and possibly even turbulent onset in the subcritical regime. We define such a non-modal growth rate using a relatively simple model of the statistical effect that the nonlinearities have on cross-phases and amplitude ratios of the system state variables. In particular, we model the nonlinearities as delta-function-like, periodic forces that randomize the state variables once every eddy turnover time. Furthermore, we estimate the eddy turnover time to be the inverse of the least stable eigenmode frequency or growth rate, which allows for prediction without nonlinear numerical simulation. We test this procedure on the 2D and 3D Hasegawa-Wakatani model [A. Hasegawa and M. Wakatani, Phys. Rev. Lett. 50, 682 (1983)] and find that the non-modal growth rate is a good predictor of energy injection rates, especially in the strongly non-normal, fully developed turbulence regime. (C) 2015 AIP Publishing LLC. C1 [Friedman, B.; Carter, T. A.] Univ Calif Los Angeles, Dept Phys & Astron, Los Angeles, CA 90095 USA. [Friedman, B.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. RP Friedman, B (reprint author), Univ Calif Los Angeles, Dept Phys & Astron, Los Angeles, CA 90095 USA. EM friedman11@llnl.gov FU U.S. Department of Energy by Lawrence Livermore National Laboratory [DE-AC52-07NA27344]; National Science Foundation [PHY-1202007] FX This work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract No. DE-AC52-07NA27344. This work was supported by the National Science Foundation (Grant No. PHY-1202007). NR 38 TC 1 Z9 1 U1 2 U2 10 PU AMER INST PHYSICS PI MELVILLE PA 1305 WALT WHITMAN RD, STE 300, MELVILLE, NY 11747-4501 USA SN 1070-664X EI 1089-7674 J9 PHYS PLASMAS JI Phys. Plasmas PD JAN PY 2015 VL 22 IS 1 AR 012307 DI 10.1063/1.4905863 PG 10 WC Physics, Fluids & Plasmas SC Physics GA CA8NQ UT WOS:000349178100019 ER PT J AU Kemp, GE Link, A Ping, Y McLean, HS Patel, PK Freeman, RR Schumacher, DW Tiedje, HF Tsui, YY Ramis, R Fedosejevs, R AF Kemp, G. E. Link, A. Ping, Y. McLean, H. S. Patel, P. K. Freeman, R. R. Schumacher, D. W. Tiedje, H. F. Tsui, Y. Y. Ramis, R. Fedosejevs, R. TI On specular reflectivity measurements in high and low-contrast relativistic laser-plasma interactions SO PHYSICS OF PLASMAS LA English DT Article ID MAGNETIC-FIELDS; OVERDENSE PLASMAS; TEMPORAL CONTRAST; SOLID TARGET; PULSE; GENERATION; INTENSITY; HARMONICS; TRANSPORT; DYNAMICS AB Using both experiment and 2D3V particle-in-cell (PIC) simulations, we describe the use of specular reflectivity measurements to study relativistic (I lambda(2) > 10(18) W/cm(2).mu m(2)) laser-plasma interactions for both high and low-contrast 527 nm laser pulses on initially solid density aluminum targets. In the context of hot-electron generation, studies typically rely on diagnostics which, more-often-than-not, represent indirect processes driven by fast electrons transiting through solid density materials. Specular reflectivity measurements, however, can provide a direct measure of the interaction that is highly sensitive to how the EM fields and plasma profiles, critical input parameters for modeling of hot-electron generation, evolve near the interaction region. While the fields of interest occur near the relativistic critical electron density, experimental reflectivity measurements are obtained centimeters away from the interaction region, well after diffraction has fully manifested itself. Using a combination of PIC simulations with experimentally inspired conditions and an analytic, non-paraxial, pulse propagation algorithm, we calculate reflected pulse properties, both near and far from the interaction region, and compare with specular reflectivity measurements. The experiment results and PIC simulations demonstrate that specular reflectivity measurements are an extremely sensitive qualitative, and partially quantitative, indicator of initial laser/target conditions, ionization effects, and other details of intense laser-matter interactions. The techniques described can provide strong constraints on many systems of importance in ultra-intense laser interactions with matter. (C) 2015 AIP Publishing LLC. C1 [Kemp, G. E.; Link, A.; Ping, Y.; McLean, H. S.; Patel, P. K.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. [Kemp, G. E.; Freeman, R. R.; Schumacher, D. W.] Ohio State Univ, Dept Phys, Columbus, OH 43210 USA. [Tiedje, H. F.; Tsui, Y. Y.; Fedosejevs, R.] Univ Alberta, Dept Elect & Comp Engn, Edmonton, AB T6G 2V4, Canada. [Ramis, R.] Univ Politecn Madrid, Madrid, Spain. RP Kemp, GE (reprint author), Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. EM kemp10@llnl.gov RI Schumacher, Douglass/J-3454-2015; Patel, Pravesh/E-1400-2011 OI Schumacher, Douglass/0000-0002-2171-3902; NR 66 TC 1 Z9 1 U1 1 U2 23 PU AMER INST PHYSICS PI MELVILLE PA 1305 WALT WHITMAN RD, STE 300, MELVILLE, NY 11747-4501 USA SN 1070-664X EI 1089-7674 J9 PHYS PLASMAS JI Phys. Plasmas PD JAN PY 2015 VL 22 IS 1 AR 013110 DI 10.1063/1.4906053 PG 13 WC Physics, Fluids & Plasmas SC Physics GA CA8NQ UT WOS:000349178100048 ER PT J AU Korotkevich, AO Lushnikov, PM Rose, HA AF Korotkevich, Alexander O. Lushnikov, Pavel M. Rose, Harvey A. TI Beyond the random phase approximation: Stimulated Brillouin backscatter for finite laser coherence times SO PHYSICS OF PLASMAS LA English DT Article ID HOT-SPOTS; PARAMETRIC-INSTABILITIES; PLASMA; SCATTERING; FILAMENTS; TARGETS; PLATE; BEAMS AB We developed a linear theory of backward stimulated Brillouin scatter (BSBS) of a spatially and temporally random laser beam relevant for laser fusion. Our analysis reveals a new collective regime of BSBS (CBSBS). Its intensity threshold is controlled by diffraction, once cT(c) exceeds a laser speckle length, with T-c the laser coherence time. The BSBS spatial gain rate is approximately the sum of that due to CBSBS, and a part which is independent of diffraction and varies linearly with T-c. The CBSBS spatial gain rate may be reduced significantly by the temporal bandwidth of KrF-based laser systems compared to the bandwidth currently available to temporally smoothed glass-based laser systems. (C) 2015 AIP Publishing LLC. C1 [Korotkevich, Alexander O.; Lushnikov, Pavel M.] Univ New Mexico, Dept Math & Stat, Albuquerque, NM 87131 USA. [Korotkevich, Alexander O.; Lushnikov, Pavel M.] Landau Inst Theoret Phys, Moscow 119334, Russia. [Rose, Harvey A.] Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. [Rose, Harvey A.] New Mexico Consortium, Los Alamos, NM 87544 USA. RP Korotkevich, AO (reprint author), Univ New Mexico, Dept Math & Stat, Albuquerque, NM 87131 USA. EM plushnik@math.unm.edu FU New Mexico Consortium; Department of Energy Award [DE-SCOO02238]; National Science Foundation [PHY 1004118, PHY 1004110, DMS 1412140]; Leading Scientific Schools of Russia [NSh-3753.2014.2] FX We acknowledge helpful discussions with R. Berger and N. Meezan. P.L. and H.R. were supported by the New Mexico Consortium and Department of Energy Award No. DE-SCOO02238 as well as by the National Science Foundation under Grant Nos. PHY 1004118, and PHY 1004110. P.L. was partially supported by the National Science Foundation under Grant No. DMS 1412140. A.K. was partially supported by the "Leading Scientific Schools of Russia" Grant No. NSh-3753.2014.2. NR 28 TC 1 Z9 1 U1 1 U2 9 PU AMER INST PHYSICS PI MELVILLE PA 1305 WALT WHITMAN RD, STE 300, MELVILLE, NY 11747-4501 USA SN 1070-664X EI 1089-7674 J9 PHYS PLASMAS JI Phys. Plasmas PD JAN PY 2015 VL 22 IS 1 AR 012107 DI 10.1063/1.4906057 PG 12 WC Physics, Fluids & Plasmas SC Physics GA CA8NQ UT WOS:000349178100011 ER PT J AU Lee, W Umansky, MV Angus, JR Krasheninnikov, SI AF Lee, Wonjae Umansky, Maxim V. Angus, J. R. Krasheninnikov, Sergei I. TI Electromagnetic effects on dynamics of high-beta filamentary structures SO PHYSICS OF PLASMAS LA English DT Article ID EDGE; TURBULENCE AB The impacts of the electromagnetic effects on blob dynamics are considered. Electromagnetic BOUT++ simulations on seeded high-beta blobs demonstrate that inhomogeneity of magnetic curvature or plasma pressure along the filament leads to bending of the blob filaments and the magnetic field lines due to increased propagation time of plasma current (Alfven time). The bending motion can enhance heat exchange between the plasma facing materials and the inner scrape-off layer (SOL) region. The effects of sheath boundary conditions on the part of the blob away from the boundary are also diminished by the increased Alfven time. Using linear analysis and BOUT++ simulations, it is found that electromagnetic effects in high temperature and high density plasmas reduce the growth rate of resistive drift wave instability when resistivity drops below a certain value. The blobs temperature decreases in the course of its motion through the SOL and so the blob can switch from the electromagnetic to the electrostatic regime where resistive drift waves become important again. (C) 2015 AIP Publishing LLC. C1 [Lee, Wonjae; Krasheninnikov, Sergei I.] Univ Calif San Diego, La Jolla, CA 92093 USA. [Umansky, Maxim V.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. [Angus, J. R.] Naval Res Lab, Washington, DC 20375 USA. RP Lee, W (reprint author), Univ Calif San Diego, 9500 Gilman Dr, La Jolla, CA 92093 USA. EM skrash@mae.ucsd.edu OI Angus, Justin/0000-0003-1474-0002 FU U.S. Department of Energy Office of Science, Office of Fusion Energy Sciences at UCSD [DE-FG02-04ER54739, DE-SC0010413]; Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]; Kwanjeong Educational Foundation FX This material was based upon work supported by the U.S. Department of Energy Office of Science, Office of Fusion Energy Sciences under Award Nos. DE-FG02-04ER54739 and DE-SC0010413 at UCSD. This research used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. This research was also supported by the Kwanjeong Educational Foundation. NR 22 TC 3 Z9 3 U1 2 U2 5 PU AMER INST PHYSICS PI MELVILLE PA 1305 WALT WHITMAN RD, STE 300, MELVILLE, NY 11747-4501 USA SN 1070-664X EI 1089-7674 J9 PHYS PLASMAS JI Phys. Plasmas PD JAN PY 2015 VL 22 IS 1 AR 012505 DI 10.1063/1.4905639 PG 10 WC Physics, Fluids & Plasmas SC Physics GA CA8NQ UT WOS:000349178100027 ER PT J AU Ma, CH Xu, XQ Xi, PW Xia, TY AF Ma, C. H. Xu, X. Q. Xi, P. W. Xia, T. Y. TI Impact of relative phase shift on inward turbulent spreading SO PHYSICS OF PLASMAS LA English DT Article ID TOKAMAKS AB The relative cross-phase between density, temperature, and potential perturbations plays a major role in turbulent spreading and transport. Nonlinear Landau-Fluid simulations show that the electron wave-particle resonances provide a relatively strong parallel damping effect on the electron temperature perturbation and can induce a relative cross-phase shift of smaller than pi/2 angle between E x B velocity and the electron temperature perturbation for large electron temperature gradient, which yields a large spreading for electron. The relative phase for ions is about pi/2 and has no turbulent spreading effect on it. The inward turbulent spreading stops at the position where the radial turbulent correlation length is shorter than the magnetic surface spacing. The temperature pedestal height determines the energy loss due to the turbulent spreading. (C) 2015 AIP Publishing LLC. C1 [Ma, C. H.; Xi, P. W.] Peking Univ, Fus Simulat Ctr, Sch Phys, Beijing 100871, Peoples R China. [Ma, C. H.; Xu, X. Q.; Xi, P. W.; Xia, T. Y.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. [Xia, T. Y.] Chinese Acad Sci, Inst Plasma Phys, Hefei, Peoples R China. RP Ma, CH (reprint author), Peking Univ, Fus Simulat Ctr, Sch Phys, Beijing 100871, Peoples R China. FU U.S. DoE by LLNL [DE-AC52-7NA27344]; ITER-China Program [2013GB111000, 2013GB112006]; NSFC [11261140326, 10935004]; CSC [201206010101] FX The authors wish to acknowledge P. Diamond, A. Dimits, M. V. Umansky, I. Joseph, J. F. Ma, P. Snyder, and X. G. Wang for useful discussions. This work was performed under the auspices of the U.S. DoE by LLNL under Contract No. DE-AC52-7NA27344 and is supported by the ITER-China Program (Nos. 2013GB111000 and 2013GB112006), NSFC (Nos. 11261140326 and 10935004) and CSC (No. 201206010101). Lawrence Livermore National Laboratory IM number: LLNL-JRNL-652541. NR 21 TC 2 Z9 2 U1 1 U2 8 PU AMER INST PHYSICS PI MELVILLE PA 1305 WALT WHITMAN RD, STE 300, MELVILLE, NY 11747-4501 USA SN 1070-664X EI 1089-7674 J9 PHYS PLASMAS JI Phys. Plasmas PD JAN PY 2015 VL 22 IS 1 AR 010702 DI 10.1063/1.4905644 PG 5 WC Physics, Fluids & Plasmas SC Physics GA CA8NQ UT WOS:000349178100002 ER PT J AU Montgomery, DS Albright, BJ Barnak, DH Chang, PY Davies, JR Fiksel, G Froula, DH Kline, JL MacDonald, MJ Sefkow, AB Yin, L Betti, R AF Montgomery, D. S. Albright, B. J. Barnak, D. H. Chang, P. Y. Davies, J. R. Fiksel, G. Froula, D. H. Kline, J. L. MacDonald, M. J. Sefkow, A. B. Yin, L. Betti, R. TI Use of external magnetic fields in hohlraum plasmas to improve laser-coupling SO PHYSICS OF PLASMAS LA English DT Article ID INERTIAL-CONFINEMENT-FUSION; STIMULATED RAMAN-SCATTERING; NATIONAL IGNITION FACILITY; THOMSON-SCATTERING; PHYSICS BASIS; TARGETS AB Efficient coupling of laser energy into hohlraum targets is important for indirect drive ignition. Laser-plasma instabilities can reduce coupling, reduce symmetry, and cause preheat. We consider the effects of an external magnetic field on laser-energy coupling in hohlraum targets. Experiments were performed at the Omega Laser Facility using low-Z gas-filled hohlraum targets which were placed in a magnetic coil with B-z <= 7.5-T. We found that an external field B-z = 7.5-T aligned along the hohlraum axis results in up to a 50% increase in plasma temperature as measured by Thomson scattering. The experiments were modeled using the 2-D magnetohydrodynamics package in HYDRA and were found to be in good agreement. (C) 2015 AIP Publishing LLC. C1 [Montgomery, D. S.; Albright, B. J.; Kline, J. L.; Yin, L.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Barnak, D. H.; Chang, P. Y.; Davies, J. R.; Fiksel, G.; Froula, D. H.; Betti, R.] Univ Rochester, Laser Energet Lab, Rochester, NY 14623 USA. [MacDonald, M. J.] Univ Michigan, Dept Atmospher Ocean & Space Sci, Ann Arbor, MI 48109 USA. [MacDonald, M. J.] SLAC Natl Accelerator Lab, Menlo Pk, CA 94025 USA. [Sefkow, A. B.] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Montgomery, DS (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM montgomery@lanl.gov OI Albright, Brian/0000-0002-7789-6525; MacDonald, Michael/0000-0002-6295-6978; Yin, Lin/0000-0002-8978-5320; Barnak, Daniel/0000-0002-4646-7517; Kline, John/0000-0002-2271-9919 FU Omega Laser Operations team; LANL target fabrication team; U.S. Department of Energy by Los Alamos National Laboratory [DE-AC52-06NA25396] FX The authors would like to acknowledge the support of the Omega Laser Operations team and the LANL target fabrication team. D.S.M. wishes to acknowledge informative discussions with Tom Intrator (LANL, deceased), who helped inspire the formation of this concept through several conversations. A.B.S. acknowledges the simulation support of Joe Koning. The authors would also like to acknowledge discussions with Mordy Rosen, John Perkins, David Strozzi (LLNL), and B. Grant Logan (LBNL). This work performed under the auspices of the U.S. Department of Energy by Los Alamos National Laboratory under Contract No. DE-AC52-06NA25396. NR 24 TC 13 Z9 13 U1 1 U2 20 PU AMER INST PHYSICS PI MELVILLE PA 1305 WALT WHITMAN RD, STE 300, MELVILLE, NY 11747-4501 USA SN 1070-664X EI 1089-7674 J9 PHYS PLASMAS JI Phys. Plasmas PD JAN PY 2015 VL 22 IS 1 AR 010703 DI 10.1063/1.4906055 PG 4 WC Physics, Fluids & Plasmas SC Physics GA CA8NQ UT WOS:000349178100003 ER PT J AU Ott, T Bonitz, M Stanton, LG Murillo, MS AF Ott, T. Bonitz, M. Stanton, L. G. Murillo, M. S. TI Coupling strength in Coulomb and Yukawa one-component plasmas (vol 21, 113704, 2014) SO PHYSICS OF PLASMAS LA English DT Correction C1 [Ott, T.; Bonitz, M.] Univ Kiel, Inst Theoret Phys & Astrophys, D-24098 Kiel, Germany. [Stanton, L. G.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. [Murillo, M. S.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Ott, T (reprint author), Univ Kiel, Inst Theoret Phys & Astrophys, Leibnizstr 15, D-24098 Kiel, Germany. RI Bonitz, Michael/A-6873-2010 OI Bonitz, Michael/0000-0001-7911-0656 NR 1 TC 0 Z9 0 U1 0 U2 6 PU AMER INST PHYSICS PI MELVILLE PA 1305 WALT WHITMAN RD, STE 300, MELVILLE, NY 11747-4501 USA SN 1070-664X EI 1089-7674 J9 PHYS PLASMAS JI Phys. Plasmas PD JAN PY 2015 VL 22 IS 1 AR 019901 DI 10.1063/1.4905185 PG 1 WC Physics, Fluids & Plasmas SC Physics GA CA8NQ UT WOS:000349178100067 ER PT J AU Smirnov, RD Krasheninnikov, SI Pigarov, AY Rognlien, TD AF Smirnov, R. D. Krasheninnikov, S. I. Pigarov, A. Yu. Rognlien, T. D. TI Tungsten dust impact on ITER-like plasma edge SO PHYSICS OF PLASMAS LA English DT Article ID FUSION DEVICES; TOKAMAK; SIMULATION; PARTICLES; OPERATION; ISSUES; CODE AB The impact of tungsten dust originating from divertor plates on the performance of edge plasma in ITER-like discharge is evaluated using computer modeling with the coupled dust-plasma transport code DUSTT-UEDGE. Different dust injection parameters, including dust size and mass injection rates, are surveyed. It is found that tungsten dust injection with rates as low as a few mg/s can lead to dangerously high tungsten impurity concentrations in the plasma core. Dust injections with rates of a few tens of mg/s are shown to have a significant effect on edge plasma parameters and dynamics in ITER scale tokamaks. The large impact of certain phenomena, such as dust shielding by an ablation cloud and the thermal force on tungsten ions, on dust/impurity transport in edge plasma and consequently on core tungsten contamination level is demonstrated. It is also found that high-Z impurities provided by dust can induce macroscopic self-sustained plasma oscillations in plasma edge leading to large temporal variations of edge plasma parameters and heat load to divertor target plates. (C) 2015 AIP Publishing LLC. C1 [Smirnov, R. D.; Krasheninnikov, S. I.; Pigarov, A. Yu.] Univ Calif San Diego, La Jolla, CA 92093 USA. [Rognlien, T. D.] Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. RP Smirnov, RD (reprint author), Univ Calif San Diego, La Jolla, CA 92093 USA. EM rsmirnov@ucsd.edu RI Smirnov, Roman/B-9916-2011 OI Smirnov, Roman/0000-0002-9114-5330 FU U.S. Department of Energy, Office of Science, Office of Fusion Energy Sciences at UCSD [DE-FG02-06ER54852]; U.S. Department of Energy, Office of Science, Office of Fusion Energy Sciences at LLNL [DE-AC52-07NA27344] FX This material is based upon work supported by the U.S. Department of Energy, Office of Science, Office of Fusion Energy Sciences, under Award No. DE-FG02-06ER54852 at UCSD and Contract No. DE-AC52-07NA27344 at LLNL. NR 40 TC 7 Z9 7 U1 3 U2 31 PU AMER INST PHYSICS PI MELVILLE PA 1305 WALT WHITMAN RD, STE 300, MELVILLE, NY 11747-4501 USA SN 1070-664X EI 1089-7674 J9 PHYS PLASMAS JI Phys. Plasmas PD JAN PY 2015 VL 22 IS 1 AR 012506 DI 10.1063/1.4905704 PG 7 WC Physics, Fluids & Plasmas SC Physics GA CA8NQ UT WOS:000349178100028 ER PT J AU Stanier, A Simakov, AN Chacon, L Daughton, W AF Stanier, A. Simakov, Andrei N. Chacon, L. Daughton, W. TI Fast magnetic reconnection with large guide fields SO PHYSICS OF PLASMAS LA English DT Article ID IMPLICIT; SOLVER AB In this letter, it is demonstrated using two-fluid simulations that low-beta magnetic reconnection remains fast, regardless of the presence of fast dispersive waves, which have been previously suggested to play a critical role. To understand these results, a discrete model is constructed that offers scaling relationships for the reconnection rate and dissipation region (DR) thickness in terms of the upstream magnetic field and DR length. We verify these scalings numerically and show how the DR self-adjusts to process magnetic flux at the same rate that it is supplied to a larger region where two-fluid effects become important. The rate is therefore independent of the DR physics and is in good agreement with kinetic results. (C) 2015 AIP Publishing LLC. C1 [Stanier, A.; Simakov, Andrei N.; Chacon, L.; Daughton, W.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Stanier, A (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM stanier@lanl.gov RI Daughton, William/L-9661-2013; OI Simakov, Andrei/0000-0001-7064-9153; Chacon, Luis/0000-0002-4566-8763 FU U.S. Department of Energy, Office of Science; Office of Fusion Energy Sciences; U.S. Department of Energy National Nuclear Security Administration [DE-AC52-06NA25396]; NASA through the Heliospheric Theory Program FX This work was supported by the U.S. Department of Energy, Office of Science, and Office of Fusion Energy Sciences, and used resources provided by the Los Alamos National Laboratory Institutional Computing Program, which was supported by the U.S. Department of Energy National Nuclear Security Administration under Contract No. DE-AC52-06NA25396. Contributions from W.D. were supported by NASA through the Heliospheric Theory Program. A.S. would like to thank Yi-Hsin Liu for helpful discussions and the anonymous referees for their suggestions. NR 38 TC 7 Z9 7 U1 0 U2 4 PU AMER INST PHYSICS PI MELVILLE PA 1305 WALT WHITMAN RD, STE 300, MELVILLE, NY 11747-4501 USA SN 1070-664X EI 1089-7674 J9 PHYS PLASMAS JI Phys. Plasmas PD JAN PY 2015 VL 22 IS 1 AR 010701 DI 10.1063/1.4905629 PG 5 WC Physics, Fluids & Plasmas SC Physics GA CA8NQ UT WOS:000349178100001 ER PT J AU Wang, L Hakim, AH Bhattacharjee, A Germaschewski, K AF Wang, Liang Hakim, Ammar H. Bhattacharjee, A. Germaschewski, K. TI Comparison of multi-fluid moment models with particle-in-cell simulations of collisionless magnetic reconnection SO PHYSICS OF PLASMAS LA English DT Article ID HALL-MAGNETOHYDRODYNAMICS; PRESSURE TENSOR; CURRENT SHEETS; LABORATORY PLASMAS; HYBRID SIMULATIONS; EQUATIONS; MAGNETOTAIL; CHALLENGE; DYNAMICS; GRADIENT AB We introduce an extensible multi-fluid moment model in the context of collisionless magnetic reconnection. This model evolves full Maxwell equations and simultaneously moments of the Vlasov-Maxwell equation for each species in the plasma. Effects like electron inertia and pressure gradient are self-consistently embedded in the resulting multi-fluid moment equations, without the need to explicitly solving a generalized Ohm's law. Two limits of the multi-fluid moment model are discussed, namely, the five-moment limit that evolves a scalar pressures for each species and the ten-moment limit that evolves the full anisotropic, non-gyrotropic pressure tensor for each species. We first demonstrate analytically and numerically that the five-moment model reduces to the widely used Hall magnetohydrodynamics (Hall MHD) model under the assumptions of vanishing electron inertia, infinite speed of light, and quasi-neutrality. Then, we compare ten-moment and fully kinetic particle-in-cell (PIC) simulations of a large scale Harris sheet reconnection problem, where the ten-moment equations are closed with a local linear collisionless approximation for the heat flux. The ten-moment simulation gives reasonable agreement with the PIC results regarding the structures and magnitudes of the electron flows, the polarities and magnitudes of elements of the electron pressure tensor, and the decomposition of the generalized Ohm's law. Possible ways to improve the simple local closure towards a nonlocal fully three-dimensional closure are also discussed. (C) 2015 AIP Publishing LLC. C1 [Wang, Liang; Germaschewski, K.] Univ New Hampshire, Ctr Space Sci, Durham, NH 03824 USA. [Wang, Liang; Germaschewski, K.] Univ New Hampshire, Dept Phys, Durham, NH 03824 USA. [Hakim, Ammar H.; Bhattacharjee, A.] Princeton Plasma Phys Lab, Ctr Heliophys, Princeton, NJ 08543 USA. RP Wang, L (reprint author), Univ New Hampshire, Ctr Space Sci, Durham, NH 03824 USA. EM liang.wang@unh.edu OI Germaschewski, Kai/0000-0002-8495-6354 FU NSF-NASA Collaborative Research on Space Weather [AGS-1338944]; U.S. Department of Energy through the Max-Planck/Princeton Center for Plasma Physics [DE-AC02-09CH11466]; Princeton Plasma Physics Laboratory; U.S. Department of Energy through the Space Science Center of the University of New Hampshire [DE-FG02-07ER46372]; NSF MRI program [PHY-1229408]; U.S. Department of Energy [DE-AC02-05CH11231] FX This research is supported by the NSF-NASA Collaborative Research on Space Weather Grant No. AGS-1338944, the U.S. Department of Energy Contract No. DE-AC02-09CH11466, through the Max-Planck/Princeton Center for Plasma Physics and the Princeton Plasma Physics Laboratory, and the U.S. Department of Energy Contract No. DE-FG02-07ER46372, through the Space Science Center of the University of New Hampshire. Computations were performed on Trillian, a Cray XE6m-200 supercomputer at UNH supported by the NSF MRI program under Grant No. PHY-1229408, on facilities at Research Computing Center of the Princeton Plasma Physics Laboratory, and on facilities at the National Energy Research Scientific Computing Center, supported by the U.S. Department of Energy Contract No. DE-AC02-05CH11231. NR 74 TC 10 Z9 10 U1 2 U2 19 PU AMER INST PHYSICS PI MELVILLE PA 1305 WALT WHITMAN RD, STE 300, MELVILLE, NY 11747-4501 USA SN 1070-664X EI 1089-7674 J9 PHYS PLASMAS JI Phys. Plasmas PD JAN PY 2015 VL 22 IS 1 AR 012108 DI 10.1063/1.4906063 PG 13 WC Physics, Fluids & Plasmas SC Physics GA CA8NQ UT WOS:000349178100012 ER PT J AU Zhou, YL Wang, ZH Xu, XQ Li, HD Feng, H Sun, WG AF Zhou, Y. L. Wang, Z. H. Xu, X. Q. Li, H. D. Feng, H. Sun, W. G. TI Comparisons between tokamak fueling of gas puffing and supersonic molecular beam injection in 2D simulations SO PHYSICS OF PLASMAS LA English DT Article ID HIGH-FIELD SIDE; PLASMA; PHYSICS AB Plasma fueling with high efficiency and deep injection is very important to enable fusion power performance requirements. It is a powerful and efficient way to study neutral transport dynamics and find methods of improving the fueling performance by doing large scale simulations. Two basic fueling methods, gas puffing (GP) and supersonic molecular beam injection (SMBI), are simulated and compared in realistic divertor geometry of the HL-2A tokamak with a newly developed module, named trans-neut, within the framework of BOUT++ boundary plasma turbulence code [Z.H. Wang et al., Nucl. Fusion 54, 043019 (2014)]. The physical model includes plasma density, heat and momentum transport equations along with neutral density, and momentum transport equations. Transport dynamics and profile evolutions of both plasma and neutrals are simulated and compared between GP and SMBI in both poloidal and radial directions, which are quite different from one and the other. It finds that the neutrals can penetrate about four centimeters inside the last closed (magnetic) flux surface during SMBI, while they are all deposited outside of the LCF during GP. It is the radial convection and larger inflowing flux which lead to the deeper penetration depth of SMBI and higher fueling efficiency compared to GP. (C) 2015 AIP Publishing LLC. C1 [Zhou, Y. L.; Sun, W. G.] Sichuan Univ, Inst Atom & Mol Phys, Chengdu 610041, Peoples R China. [Zhou, Y. L.; Wang, Z. H.] Southwestern Inst Phys, Chengdu 610041, Peoples R China. [Xu, X. Q.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. [Li, H. D.; Feng, H.; Sun, W. G.] Xihua Univ, Sch Phys & Chem, Chengdu 610041, Peoples R China. RP Zhou, YL (reprint author), Sichuan Univ, Inst Atom & Mol Phys, Chengdu 610041, Peoples R China. EM zhwang@swip.ac.cn FU NSFC [11205053, 11405112]; China National Magnetic Confinement Fusion Science Program [2013GB107001, 2013GB112005]; Funds of the Youth Innovation Team of Science and Technology in Sichuan Province of China [2014TD0023] FX The authors wish to thank B. D. Dudson and M. V. Umansky for their contributions to BOUT++ framework. We also thank T. D. Rognlien, M. Xu, Y. Zhang, T. Y. Xia, J. Ou, G. S. Xu, B. Gui, C. F. Sang, L. H. Yao, B. B. Feng, C. Y. Chen, S. Y. Chen, and H. H. Wang for their fruitful physical discussions. This work was supported by NSFC, Grant Nos. 11205053 and 11405112, China National Magnetic Confinement Fusion Science Program, Grant Nos. 2013GB107001 and 2013GB112005 and the Funds of the Youth Innovation Team of Science and Technology in Sichuan Province of China (Grant No. 2014TD0023). NR 25 TC 3 Z9 3 U1 3 U2 18 PU AMER INST PHYSICS PI MELVILLE PA 1305 WALT WHITMAN RD, STE 300, MELVILLE, NY 11747-4501 USA SN 1070-664X EI 1089-7674 J9 PHYS PLASMAS JI Phys. Plasmas PD JAN PY 2015 VL 22 IS 1 AR 012503 DI 10.1063/1.4905641 PG 9 WC Physics, Fluids & Plasmas SC Physics GA CA8NQ UT WOS:000349178100025 ER PT J AU Wilke, A Bischof, J Harrison, T Brettin, T D'Souza, M Gerlach, W Matthews, H Paczian, T Wilkening, J Glass, EM Desai, N Meyer, F AF Wilke, Andreas Bischof, Jared Harrison, Travis Brettin, Tom D'Souza, Mark Gerlach, Wolfgang Matthews, Hunter Paczian, Tobias Wilkening, Jared Glass, Elizabeth M. Desai, Narayan Meyer, Folker TI A RESTful API for Accessing Microbial Community Data for MG-RAST SO PLOS COMPUTATIONAL BIOLOGY LA English DT Article ID SERVER AB Metagenomic sequencing has produced significant amounts of data in recent years. For example, as of summer 2013, MG-RAST has been used to annotate over 110,000 data sets totaling over 43 Terabases. With metagenomic sequencing finding even wider adoption in the scientific community, the existing web-based analysis tools and infrastructure in MG-RAST provide limited capability for data retrieval and analysis, such as comparative analysis between multiple data sets. Moreover, although the system provides many analysis tools, it is not comprehensive. By opening MG-RAST up via a web services API (application programmers interface) we have greatly expanded access to MG-RAST data, as well as provided a mechanism for the use of third-party analysis tools with MG-RAST data. This RESTful API makes all data and data objects created by the MG-RAST pipeline accessible as JSON objects. As part of the DOE Systems Biology Knowledgebase project (KBase, http://kbase.us) we have implemented a web services API for MG-RAST. This API complements the existing MG-RAST web interface and constitutes the basis of KBase's microbial community capabilities. In addition, the API exposes a comprehensive collection of data to programmers. This API, which uses a RESTful (Representational State Transfer) implementation, is compatible with most programming environments and should be easy to use for end users and third parties. It provides comprehensive access to sequence data, quality control results, annotations, and many other data types. Where feasible, we have used standards to expose data and metadata. Code examples are provided in a number of languages both to show the versatility of the API and to provide a starting point for users. We present an API that exposes the data in MG-RAST for consumption by our users, greatly enhancing the utility of the MG-RAST service. C1 [Wilke, Andreas; Bischof, Jared; Harrison, Travis; Brettin, Tom; D'Souza, Mark; Gerlach, Wolfgang; Matthews, Hunter; Paczian, Tobias; Wilkening, Jared; Glass, Elizabeth M.; Desai, Narayan; Meyer, Folker] Argonne Natl Lab, Math & Comp Sci Div, Argonne, IL 60439 USA. [Wilke, Andreas; Bischof, Jared; Harrison, Travis; D'Souza, Mark; Gerlach, Wolfgang; Matthews, Hunter; Paczian, Tobias; Wilkening, Jared; Glass, Elizabeth M.; Desai, Narayan; Meyer, Folker] Univ Chicago, Computat Inst, Chicago, IL 60637 USA. RP Meyer, F (reprint author), Argonne Natl Lab, Math & Comp Sci Div, Argonne, IL 60439 USA. EM folker@anl.gov FU Alfred P. Sloan Foundation [2010-12-01]; NIH Human Microbiome Project [UH3 DK083993]; U.S. Department of Energy, Office of Biological and Environmental Research as part of the DOE Systems Biology Knowledgebase [DE-AC02-06CH11357]; U.S. Department of Energy, Office of Science, Advanced Scientific Computing Research [DE-AC02-06CH11357] FX This work was supported in part by the Alfred P. Sloan Foundation grant 2010-12-01, NIH Human Microbiome Project UH3 DK083993 and U.S. Department of Energy, Office of Biological and Environmental Research under Contract DE-AC02-06CH11357 as part of the DOE Systems Biology Knowledgebase. Computing for this work was supported in part by the U.S. Department of Energy, Office of Science, Advanced Scientific Computing Research, under Contract DE-AC02-06CH11357. The funders had no role in study design, data collection and analysis, decision to publish, or preparation of the manuscript. NR 12 TC 5 Z9 7 U1 2 U2 11 PU PUBLIC LIBRARY SCIENCE PI SAN FRANCISCO PA 1160 BATTERY STREET, STE 100, SAN FRANCISCO, CA 94111 USA SN 1553-734X EI 1553-7358 J9 PLOS COMPUT BIOL JI PLoS Comput. Biol. PD JAN PY 2015 VL 11 IS 1 AR e1004008 DI 10.1371/journal.pcbi.1004008 PG 8 WC Biochemical Research Methods; Mathematical & Computational Biology SC Biochemistry & Molecular Biology; Mathematical & Computational Biology GA CB0IO UT WOS:000349309400009 PM 25569221 ER PT J AU Li, F Yager, KG Dawson, NM Jiang, YB Malloy, KJ Qin, Y AF Li, Fei Yager, Kevin G. Dawson, Noel M. Jiang, Ying-Bing Malloy, Kevin J. Qin, Yang TI Nano-structuring polymer/fullerene composites through the interplay of conjugated polymer crystallization, block copolymer self-assembly and complementary hydrogen bonding interactions SO POLYMER CHEMISTRY LA English DT Article ID HETEROJUNCTION SOLAR-CELLS; FIELD-EFFECT TRANSISTORS; FIBER-LIKE MICELLES; ACID METHYL-ESTER; PHOTOVOLTAIC APPLICATIONS; POLY(3-HEXYLTHIOPHENE) NANOFIBERS; POLY(3-BUTYLTHIOPHENE) NANOWIRES; ORGANIC PHOTOVOLTAICS; NANOSCALE MORPHOLOGY; DIBLOCK COPOLYMERS AB We describe a facile strategy of precisely nano-structuring conjugated polymer (CP)/fullerene composites for organic photovoltaics (OPVs). By building in strong complementary hydrogen bonding interactions between CP nanofibers (NFs) and fullerene derivatives, well-defined and stable supramolecular polymer/fullerene composite NFs are obtained. Specifically, a conjugated block copolymer having poly(3-hexylthiophene) (P3HT) backbone selectively functionalized with polar isoorotic acid moieties, P3HT-bP3IOAT, and a diaminopyridine tethered fullerene derivative, PCBP, are used as the building blocks. Selfassembly of P3HT-b-P3IOAT in mixed solvents leads to core-shell micelle-like NFs having IOA groups preferentially located on the periphery of the P3HT NF core, onto which PCBP molecules are subsequently attached non-covalently. Formation of such complex structures are studied in detail and confirmed by NMR spectroscopy, absorption spectroscopy, transmission electron microscopy, atomic force microscopy, and X-ray scattering measurements. Application of these composite NFs in OPV devices is investigated and evaluated, which shows close correlations between device performance and morphology controllability. C1 [Li, Fei; Qin, Yang] Univ New Mexico, Dept Chem & Biol Chem, Albuquerque, NM 87131 USA. [Yager, Kevin G.] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. [Dawson, Noel M.; Malloy, Kevin J.] Univ New Mexico, Ctr High Technol Mat, Albuquerque, NM 87131 USA. [Jiang, Ying-Bing] Univ New Mexico, TEM Lab, Albuquerque, NM 87131 USA. RP Qin, Y (reprint author), Univ New Mexico, Dept Chem & Biol Chem, Albuquerque, NM 87131 USA. EM yangqin@unm.edu RI Li, Fei/D-4426-2015; Yager, Kevin/F-9804-2011; Malloy, Kevin/E-5994-2010 OI Li, Fei/0000-0002-4177-2539; Yager, Kevin/0000-0001-7745-2513; FU University of New Mexico; NSF [IIA-1301346]; Center for Functional Nanomaterials, - U.S. Department of Energy, Office of Basic Energy Sciences [DE-AC02-98CH10886] FX The authors would like to acknowledge University of New Mexico for financial support for this research. Y. Qin acknowledges NSF grant no. IIA-1301346 for financial support. K. Yager is supported by the Center for Functional Nanomaterials, which is funded by the U.S. Department of Energy, Office of Basic Energy Sciences under contract no. DE-AC02-98CH10886. NR 79 TC 11 Z9 11 U1 9 U2 53 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1759-9954 EI 1759-9962 J9 POLYM CHEM-UK JI Polym. Chem. PY 2015 VL 6 IS 5 BP 721 EP 731 DI 10.1039/c4py00934g PG 11 WC Polymer Science SC Polymer Science GA CA6OL UT WOS:000349034300009 ER PT J AU Ahmad, MI Van Campen, DG Fields, JD Yu, JF Pool, VL Parilla, PA Ginley, DS Van Hest, MFAM Toney, MF AF Ahmad, Md Imteyaz Van Campen, Douglas G. Fields, Jeremy D. Yu, Jiafan Pool, Vanessa L. Parilla, Philip A. Ginley, David S. Van Hest, Maikel F. A. M. Toney, Michael F. TI Rapid thermal processing chamber for in-situ x-ray diffraction SO REVIEW OF SCIENTIFIC INSTRUMENTS LA English DT Article ID SOLAR-CELLS; CONTACTS AB Rapid thermal processing (RTP) is widely used for processing a variety of materials, including electronics and photovoltaics. Presently, optimization of RTP is done primarily based on ex-situ studies. As a consequence, the precise reaction pathways and phase progression during the RTP remain unclear. More awareness of the reaction pathways would better enable process optimization and foster increased adoption of RTP, which offers numerous advantages for synthesis of a broad range of materials systems. To achieve this, we have designed and developed a RTP instrument that enables real-time collection of X-ray diffraction data with intervals as short as 100 ms, while heating with ramp rates up to 100 degrees Cs-1, and with a maximum operating temperature of 1200 degrees C. The system is portable and can be installed on a synchrotron beamline. The unique capabilities of this instrument are demonstrated with in-situ characterization of a Bi2O3-SiO2 glass frit obtained during heating with ramp rates 5 degrees Cs-1 and 100 degrees Cs-1, revealing numerous phase changes. (C) 2015 AIP Publishing LLC. C1 [Ahmad, Md Imteyaz; Van Campen, Douglas G.; Yu, Jiafan; Pool, Vanessa L.; Van Hest, Maikel F. A. M.; Toney, Michael F.] SLAC Natl Accelerator Lab, SSRL, Menlo Pk, CA 94025 USA. [Fields, Jeremy D.; Parilla, Philip A.; Ginley, David S.] Natl Renewable Energy Lab, Golden, CO 80401 USA. RP Toney, MF (reprint author), SLAC Natl Accelerator Lab, SSRL, 2575 Sand Hill Rd, Menlo Pk, CA 94025 USA. EM mftoney@slac.stanford.edu RI Ahmad, Mohammad Imteyaz/E-6559-2012; OI Fields, Jeremy/0000-0003-2448-8621 FU Bridging Research Interactions through collaborative the Development Grants in Energy (BRIDGE) program under the SunShot initiative of the Department of Energy [DE-EE0005951]; U.S. Department of Energy, Office of Basic Energy Sciences [DE-AC02-76SF00515] FX This project is funded through the Bridging Research Interactions through collaborative the Development Grants in Energy (BRIDGE) program under the SunShot initiative of the Department of Energy (DE-EE0005951). In-situ measurements were carried out at the Stanford Synchrotron Radiation Laboratory, a national user facility operated by Stanford University on behalf of the U.S. Department of Energy, Office of Basic Energy Sciences, under Contract No. DE-AC02-76SF00515. We thank Ron Marks for assistance with SSRL beam line 7-2. NR 19 TC 2 Z9 2 U1 2 U2 15 PU AMER INST PHYSICS PI MELVILLE PA 1305 WALT WHITMAN RD, STE 300, MELVILLE, NY 11747-4501 USA SN 0034-6748 EI 1089-7623 J9 REV SCI INSTRUM JI Rev. Sci. Instrum. PD JAN PY 2015 VL 86 IS 1 AR 013902 DI 10.1063/1.4904848 PG 7 WC Instruments & Instrumentation; Physics, Applied SC Instruments & Instrumentation; Physics GA CA7AF UT WOS:000349068700029 PM 25638092 ER PT J AU Brejnholt, NF Decker, TA Hill, RM Chen, H Williams, GJ Park, J Alameda, JB Fernandez-Perea, M Pivovaroff, MJ Soufli, R Descalle, MA Peebles, J Kerr, SM AF Brejnholt, N. F. Decker, T. A. Hill, R. M. Chen, H. Williams, G. J. Park, J. Alameda, J. B. Fernandez-Perea, M. Pivovaroff, M. J. Soufli, R. Descalle, M. -A. Peebles, J. Kerr, S. M. TI Reflective multilayer optic as hard X-ray diagnostic on laser-plasma experiment SO REVIEW OF SCIENTIFIC INSTRUMENTS LA English DT Article AB A multilayer-based optic was tested for use as an X-ray diagnostic on a laser-plasma experiment. The multilayer optic was employed to selectively pass X-rays between 55 and 100 keV. An order of magnitude improvement in signal-to-noise ratio is achieved compared to a transmission crystal spectrometer. A multilayer response model, taking into account the source size and spectral content, is constructed and the outlook for application above 500 keV is briefly discussed. LLNL-JRNL-664311. (C) 2015 AIP Publishing LLC. C1 [Brejnholt, N. F.; Decker, T. A.; Hill, R. M.; Chen, H.; Williams, G. J.; Park, J.; Alameda, J. B.; Fernandez-Perea, M.; Pivovaroff, M. J.; Soufli, R.; Descalle, M. -A.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. [Peebles, J.] Univ Calif San Diego, Jacobs Sch Engn, La Jolla, CA 92093 USA. [Kerr, S. M.] Univ Alberta, Edmonton, AB T6G 2R3, Canada. RP Brejnholt, NF (reprint author), Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. EM brejnholt1@llnl.gov OI Kerr, Shaun/0000-0003-4822-564X FU U.S. Department of Energy by Lawrence Livermore National Laboratory [DE-AC52-07NA27344]; Livermore Graduate Scholar Program; LLNL's Laboratory Directed Research and Development Program [13-ERD-048, 12-ERD-062] FX This work performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract No. DE-AC52-07NA27344. Funding was provided by the Livermore Graduate Scholar Program and LLNL's Laboratory Directed Research and Development Program through Project Nos. 13-ERD-048 and 12-ERD-062. The authors gratefully acknowledge support from the staff at the Jupiter Laser Facility and valuable input from Gary F. Stone. NR 24 TC 1 Z9 1 U1 0 U2 8 PU AMER INST PHYSICS PI MELVILLE PA 1305 WALT WHITMAN RD, STE 300, MELVILLE, NY 11747-4501 USA SN 0034-6748 EI 1089-7623 J9 REV SCI INSTRUM JI Rev. Sci. Instrum. PD JAN PY 2015 VL 86 IS 1 AR 013110 DI 10.1063/1.4906509 PG 6 WC Instruments & Instrumentation; Physics, Applied SC Instruments & Instrumentation; Physics GA CA7AF UT WOS:000349068700012 PM 25638075 ER PT J AU Feng, J Nasiatka, J Wan, W Vecchione, T Padmore, HA AF Feng, J. Nasiatka, J. Wan, W. Vecchione, T. Padmore, H. A. TI A novel system for measurement of the transverse electron momentum distribution from photocathodes SO REVIEW OF SCIENTIFIC INSTRUMENTS LA English DT Article ID MICROSCOPY AB The transverse momentum of electrons produced by a photocathode contributes significantly to the performance of several different types of accelerator-based light sources, such as Free Electron Lasers, as well as systems designed for ultrafast electron diffraction and dynamic transmission electron microscopy. Minimization of the transverse emittance from photocathodes is the subject of intensive research, and therefore measurement of this parameter is of great importance. Here, we describe a simple system that offers real time measurements of transverse emittance and can be easily integrated into the photocathode fabrication process. (C) 2015 AIP Publishing LLC. C1 [Feng, J.; Nasiatka, J.; Wan, W.; Padmore, H. A.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Vecchione, T.] SLAC Natl Accelerator Lab, Menlo Pk, CA 94025 USA. RP Feng, J (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. FU Office of Science, Office of Basic Energy Sciences; U.S. Department of Energy [DE-AC02-05CH11231, KC0407-ALSJNT-I0013, DE-SC0005713] FX The authors would like to thank John Smedley, Jared Wong, Susanne Schubert, and Xumin Chen for rewarding discussion. This work was performed at LBNL under the auspices of the Office of Science, Office of Basic Energy Sciences, the U.S. Department of Energy under Contract No. DE-AC02-05CH11231, KC0407-ALSJNT-I0013, and DE-SC0005713. NR 18 TC 9 Z9 9 U1 3 U2 9 PU AMER INST PHYSICS PI MELVILLE PA 1305 WALT WHITMAN RD, STE 300, MELVILLE, NY 11747-4501 USA SN 0034-6748 EI 1089-7623 J9 REV SCI INSTRUM JI Rev. Sci. Instrum. PD JAN PY 2015 VL 86 IS 1 AR 015103 DI 10.1063/1.4904930 PG 5 WC Instruments & Instrumentation; Physics, Applied SC Instruments & Instrumentation; Physics GA CA7AF UT WOS:000349068700055 PM 25638118 ER PT J AU Mitrovic, S Cornell, EW Marcin, MR Jones, RJR Newhouse, PF Suram, SK Jin, J Gregoire, JM AF Mitrovic, Slobodan Cornell, Earl W. Marcin, Martin R. Jones, Ryan J. R. Newhouse, Paul F. Suram, Santosh K. Jin, Jian Gregoire, John M. TI High-throughput on-the-fly scanning ultraviolet-visible dual-sphere spectrometer SO REVIEW OF SCIENTIFIC INSTRUMENTS LA English DT Article ID FILM COMBINATORIAL LIBRARIES; ELECTRONIC STRUCTURE; OPTICAL PROPERTIES; THIN-FILMS; ELECTROCATALYSTS; DISCOVERY AB We have developed an on-the-fly scanning spectrometer operating in the UV-visible and near-infrared that can simultaneously perform transmission and total reflectance measurements at the rate better than 1 sample per second. High throughput optical characterization is important for screening functional materials for a variety of new applications. We demonstrate the utility of the instrument for screening new light absorber materials by measuring the spectral absorbance, which is subsequently used for deriving band gap information through Tauc plot analysis. (C) 2015 AIP Publishing LLC. C1 [Mitrovic, Slobodan; Marcin, Martin R.; Jones, Ryan J. R.; Newhouse, Paul F.; Suram, Santosh K.; Gregoire, John M.] CALTECH, Joint Ctr Artificial Photosynth, Pasadena, CA 91125 USA. [Cornell, Earl W.; Jin, Jian] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Engn, Berkeley, CA 94720 USA. RP Mitrovic, S (reprint author), CALTECH, Joint Ctr Artificial Photosynth, Pasadena, CA 91125 USA. EM mitrovic@caltech.edu; gregoire@caltech.edu RI Mitrovic, Slobodan/E-7847-2010; OI Mitrovic, Slobodan/0000-0001-8913-8505; Jones, Ryan/0000-0002-4629-3115 FU Office of Science of the U.S. Department of Energy [DE-SC0004993] FX This manuscript is based upon work performed by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the U.S. Department of Energy (Award No. DE-SC0004993). NR 16 TC 7 Z9 7 U1 2 U2 8 PU AMER INST PHYSICS PI MELVILLE PA 1305 WALT WHITMAN RD, STE 300, MELVILLE, NY 11747-4501 USA SN 0034-6748 EI 1089-7623 J9 REV SCI INSTRUM JI Rev. Sci. Instrum. PD JAN PY 2015 VL 86 IS 1 AR 013904 DI 10.1063/1.4905365 PG 5 WC Instruments & Instrumentation; Physics, Applied SC Instruments & Instrumentation; Physics GA CA7AF UT WOS:000349068700031 PM 25638094 ER PT J AU Randazzo, JB Tranter, RS AF Randazzo, J. B. Tranter, R. S. TI Note: An improved driver section for a diaphragmless shock tube SO REVIEW OF SCIENTIFIC INSTRUMENTS LA English DT Article AB Improvements to equipment lifetime and measurement reproducibility have been made by modifying the actuating mechanism of a diaphragmless shock tube that is used for high temperature gas kinetic studies. The modifications have two major benefits while retaining the simplicity of the original apparatus. First, the reproducibility of shock wave generation has been greatly improved and is demonstrated with 50 nearly identical experiments on the dissociation of cyclohexene at T-2 = 1765 +/- 13 K and P-2 = 120 +/- 1 Torr, demonstrating the capability for signal averaging over many experiments. Second, the lifetime of the bellows which forms the heart of the actuator is considerably improved, significantly increasing the time between replacements. (C) 2015 AIP Publishing LLC. C1 [Randazzo, J. B.; Tranter, R. S.] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. RP Randazzo, JB (reprint author), Argonne Natl Lab, Chem Sci & Engn Div, 9700 S Cass Ave, Argonne, IL 60439 USA. FU Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences, U.S. Department of Energy [DE-AC02-06CH11357] FX This work was performed under the auspices of the Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences, U.S. Department of Energy, under Contract No. DE-AC02-06CH11357. The authors kindly thank Patrick T. Lynch for the design of the bearing support plate. NR 6 TC 3 Z9 3 U1 0 U2 13 PU AMER INST PHYSICS PI MELVILLE PA 1305 WALT WHITMAN RD, STE 300, MELVILLE, NY 11747-4501 USA SN 0034-6748 EI 1089-7623 J9 REV SCI INSTRUM JI Rev. Sci. Instrum. PD JAN PY 2015 VL 86 IS 1 AR 016117 DI 10.1063/1.4906758 PG 2 WC Instruments & Instrumentation; Physics, Applied SC Instruments & Instrumentation; Physics GA CA7AF UT WOS:000349068700081 PM 25638144 ER PT J AU Repins, IL Egaas, B Mansfield, LM Contreras, MA Muzzillo, CP Beall, C Glynn, S Carapella, J Kuciauskas, D AF Repins, I. L. Egaas, B. Mansfield, L. M. Contreras, M. A. Muzzillo, C. P. Beall, C. Glynn, S. Carapella, J. Kuciauskas, D. TI Fiber-fed time-resolved photoluminescence for reduced process feedback time on thin-film photovoltaics SO REVIEW OF SCIENTIFIC INSTRUMENTS LA English DT Article ID CU(IN,GA)SE-2 SOLAR-CELLS; EFFICIENCY AB Fiber-fed time-resolved photoluminescence is demonstrated as a tool for immediate process feedback after deposition of the absorber layer for CuInxGa1-xSe2 and Cu2ZnSnSe4 photovoltaic devices. The technique uses a simplified configuration compared to typical laboratory time-resolved photoluminescence in the delivery of the exciting beam, signal collection, and electronic components. Correlation of instrument output with completed device efficiency is demonstrated over a large sample set. The extraction of the instrument figure of merit, depending on both the initial luminescence intensity and its time decay, is explained and justified. Limitations in the prediction of device efficiency by this method, including surface effect, are demonstrated and discussed. (C) 2015 AIP Publishing LLC. C1 [Repins, I. L.; Egaas, B.; Mansfield, L. M.; Contreras, M. A.; Beall, C.; Glynn, S.; Carapella, J.; Kuciauskas, D.] Natl Renewable Energy Lab, Golden, CO 80401 USA. [Muzzillo, C. P.] Univ Florida, Dept Chem Engn, Gainesville, FL 32611 USA. RP Repins, IL (reprint author), Natl Renewable Energy Lab, 15013 Denver West Pkwy, Golden, CO 80401 USA. FU U.S. Department of Energy [DE-AC36-08-GO28308]; National Renewable Energy Laboratory; Bayh-Dole funds FX The Alliance for Sustainable Energy, LLC (Alliance), is the manager and operator of the National Renewable Energy Laboratory (NREL). This work was supported by the U.S. Department of Energy under Contract No. DE-AC36-08-GO28308 with the National Renewable Energy Laboratory. Bayh-Dole funds were used to gather data preceding patent application. NR 35 TC 4 Z9 4 U1 5 U2 15 PU AMER INST PHYSICS PI MELVILLE PA 1305 WALT WHITMAN RD, STE 300, MELVILLE, NY 11747-4501 USA SN 0034-6748 EI 1089-7623 J9 REV SCI INSTRUM JI Rev. Sci. Instrum. PD JAN PY 2015 VL 86 IS 1 AR 013907 DI 10.1063/1.4905535 PG 7 WC Instruments & Instrumentation; Physics, Applied SC Instruments & Instrumentation; Physics GA CA7AF UT WOS:000349068700034 PM 25638097 ER PT J AU Zhang, DZ Jackson, JM Zhao, JY Sturhahn, W Alp, EE Toellner, TS Hu, MY AF Zhang, Dongzhou Jackson, Jennifer M. Zhao, Jiyong Sturhahn, Wolfgang Alp, E. Ercan Toellner, Thomas S. Hu, Michael Y. TI Fast temperature spectrometer for samples under extreme conditions SO REVIEW OF SCIENTIFIC INSTRUMENTS LA English DT Article ID DIAMOND-ANVIL CELL; LASER-HEATING SYSTEM; NUCLEAR RESONANT SCATTERING; HIGH-PRESSURE RESEARCH; X-RAY-DIFFRACTION; IRON; CORE; GSECARS AB We have developed a multi-wavelength Fast Temperature Readout (FasTeR) spectrometer to capture a sample's transient temperature fluctuations, and reduce uncertainties in melting temperature determination. Without sacrificing accuracy, FasTeR features a fast readout rate (about 100 Hz), high sensitivity, large dynamic range, and a well-constrained focus. Complimenting a charge-coupled device spectrometer, FasTeR consists of an array of photomultiplier tubes and optical dichroic filters. The temperatures determined by FasTeR outside of the vicinity of melting are, generally, in good agreement with results from the charge-coupled device spectrometer. Near melting, FasTeR is capable of capturing transient temperature fluctuations, at least on the order of 300 K/s. A software tool, SIMFaster, is described and has been developed to simulate FasTeR and assess design configurations. FasTeR is especially suitable for temperature determinations that utilize ultra-fast techniques under extreme conditions. Working in parallel with the laser-heated diamond-anvil cell, synchrotron Mossbauer spectroscopy, and X-ray diffraction, we have applied the FasTeR spectrometer to measure the melting temperature of (Fe0.9Ni0.1)-Fe-57 at high pressure. (C) 2015 AIP Publishing LLC. C1 [Zhang, Dongzhou; Jackson, Jennifer M.; Sturhahn, Wolfgang] CALTECH, Seismol Lab, Pasadena, CA 91125 USA. [Zhang, Dongzhou; Zhao, Jiyong; Alp, E. Ercan; Toellner, Thomas S.; Hu, Michael Y.] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. RP Zhang, DZ (reprint author), CALTECH, Seismol Lab, Pasadena, CA 91125 USA. EM dzzhang@caltech.edu RI Zhang, Dongzhou/D-9604-2017 OI Zhang, Dongzhou/0000-0002-6679-892X FU California Institute of Technology; NSF [EAR-1316362]; U.S. D.O.E., O.S., O.B.E.S. [DE-AC02-06CH11357]; COMPRES under NSF [EAR 06-49658] FX We thank G. Shen, V. B. Prakapenka, M. Rivers, Y. Meng, W. Bi, A. Alatas, and B. Chen for useful discussions and help with commissioning of this system. We are grateful to C. A. Murphy for synthesizing the 57Fe0.9Ni0.1 sample. We thank the California Institute of Technology and NSF (EAR-1316362) for support of this research, GSE-CARS and HP-CAT for the use of the laser drilling and the ruby fluorescence systems, and an anonymous reviewer for his/her thoughtful and constructive comments. Use of the Advanced Photon Source is supported by the U.S. D.O.E., O.S., O.B.E.S. (DE-AC02-06CH11357). Sector 3 operations are supported in part by COMPRES under NSF Cooperative Agreement EAR 06-49658. NR 43 TC 3 Z9 3 U1 7 U2 25 PU AMER INST PHYSICS PI MELVILLE PA 1305 WALT WHITMAN RD, STE 300, MELVILLE, NY 11747-4501 USA SN 0034-6748 EI 1089-7623 J9 REV SCI INSTRUM JI Rev. Sci. Instrum. PD JAN PY 2015 VL 86 IS 1 AR 013105 DI 10.1063/1.4905431 PG 10 WC Instruments & Instrumentation; Physics, Applied SC Instruments & Instrumentation; Physics GA CA7AF UT WOS:000349068700007 PM 25638070 ER PT J AU Wu, TF Zhou, BM Zhu, T Shi, J Xu, ZW Hu, CS Wang, JJ AF Wu, Tengfei Zhou, Baoming Zhu, Ting Shi, Jie Xu, Zhiwei Hu, Chuansheng Wang, Jiajun TI Facile and low-cost approach towards a PVDF ultrafiltration membrane with enhanced hydrophilicity and antifouling performance via graphene oxide/water-bath coagulation SO RSC ADVANCES LA English DT Article ID WALLED CARBON NANOTUBES; MIXED MATRIX MEMBRANE; MECHANICAL-PROPERTIES; COMPOSITE MEMBRANE; PHASE-SEPARATION; FOULING-CONTROL; WASTE-WATER; OXIDE; MORPHOLOGY; SURFACE AB Addressed herein is a facile and low-cost approach to endow hydrophobic polyvinylidene fluoride (PVDF) membranes with reliable hydrophilicity and antifouling properties. Porous asymmetric hydrophilic membranes with tunable morphology were facilely fabricated via phase inversion using an aqueous solution of graphene oxide (GO) as the coagulation bath. An increment in pore size and surface roughness was observed for membranes treated by a GO/water-coagulation bath (GB). The bovine serum albumin rejection of GB-treated membranes increased by 38.99% when the concentration of GO in the coagulation bath was 0.5 g L-1. The contact angle of membranes decreased from 75.9 degrees to 58.8 degrees and the water flux increased by 140% when the dosage of GO was 2 g L-1. Furthermore, fouling resistances of membranes revealed that GB-treated membranes had a higher flux recovery ratio (85.7%) than pristine PVDF (43.3%). Meanwhile, the protein adsorption of GB-treated membranes was decreased by 69.3% compared with that of pristine PVDF membranes. The cost of the membranes can be lowered by using a GB approach compared with GO-mixed matrix membranes because of the reusability of GO in a coagulation bath. This research presents an effective method to tailor membrane performance via GB rather than embedding GO in the membrane matrix. C1 [Wu, Tengfei; Zhou, Baoming; Zhu, Ting; Shi, Jie; Xu, Zhiwei; Hu, Chuansheng] Tianjin Polytech Univ, Sch Text, State Key Lab Hollow Fiber Membrane Mat & Proc, Tianjin 300387, Peoples R China. [Wang, Jiajun] Brookhaven Natl Lab, Photon Sci Directorate, Upton, NY 11973 USA. RP Xu, ZW (reprint author), Tianjin Polytech Univ, Sch Text, State Key Lab Hollow Fiber Membrane Mat & Proc, Tianjin 300387, Peoples R China. EM xuzhiwei@tjpu.edu.cn; jjwang@bnl.gov RI Xu, Zhiwei/A-1313-2015 OI Xu, Zhiwei/0000-0002-8067-5344 FU National Natural Science Foundation of China [11175130]; Petrochemical Joint Funds of National Natural Science Fund Committee - China National Petroleum Corporation [U1362108] FX The work was funded by the National Natural Science Foundation of China (11175130) and the Petrochemical Joint Funds of National Natural Science Fund Committee - China National Petroleum Corporation (U1362108). NR 61 TC 24 Z9 25 U1 12 U2 71 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2046-2069 J9 RSC ADV JI RSC Adv. PY 2015 VL 5 IS 11 BP 7880 EP 7889 DI 10.1039/c4ra13476a PG 10 WC Chemistry, Multidisciplinary SC Chemistry GA AY7DG UT WOS:000347720900011 ER PT J AU Bjorgaard, JA Kose, ME AF Bjorgaard, Josiah A. Kose, Muhammet Erkan TI Simulations of singlet exciton diffusion in organic semiconductors: a review SO RSC ADVANCES LA English DT Review ID CONJUGATED POLYMERS; ENERGY-TRANSFER; THIN-FILMS; EXCITATION TRANSFER; CHARGE-TRANSPORT; SOLAR-CELLS; AB-INITIO; MEH-PPV; REGIOREGULAR POLY(3-HEXYLTHIOPHENE); ELECTRONIC INTERACTIONS AB This review describes exciton diffusion simulation strategies in condensed phase organic semiconductors. Methods for calculating energy transfer rate constants are discussed along with procedures for how to account for energetic disorder. Exciton diffusion can be modelled by using kinetic Monte-Carlo methods or master equations. Recent literature on simulation efforts for estimating exciton diffusion lengths of various conjugated polymers and small molecules is introduced. These studies are discussed in the context of the effects of morphology on exciton diffusion and the necessity of accurate treatment of disorder to accurately reproduce experimental results. C1 [Bjorgaard, Josiah A.] Los Alamos Natl Lab, Ctr Nonlinear Studies, Div Theoret, Los Alamos, NM 87545 USA. [Kose, Muhammet Erkan] TUBITAK Gebze Yerleskesi Marmara Res Ctr, TR-41470 Kocaeli, Turkey. RP Kose, ME (reprint author), Los Alamos Natl Lab, Ctr Nonlinear Studies, Div Theoret, Los Alamos, NM 87545 USA. EM jbjorgaard@lanl.gov; erkan.kose@tubitak.gov.tr FU Center for Nonlinear Studies (CNLS) at Los Alamos National Laboratory (LANL); U.S. Department of Energy; Los Alamos National Security, LLC, for the National Nuclear Security Administration of the U.S. Department of Energy [DE-AC52-06NA25396]; TUBITAK BIDEB Fellowship FX J.A.B. acknowledges the support of the Center for Nonlinear Studies (CNLS) at Los Alamos National Laboratory (LANL) and the U.S. Department of Energy through the LANL LDRD Program. LANL is operated by Los Alamos National Security, LLC, for the National Nuclear Security Administration of the U.S. Department of Energy under contract DE-AC52-06NA25396. M.E.K acknowledges the support by TUBITAK BIDEB Fellowship. NR 108 TC 8 Z9 8 U1 4 U2 55 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2046-2069 J9 RSC ADV JI RSC Adv. PY 2015 VL 5 IS 11 BP 8432 EP 8445 DI 10.1039/c4ra12409j PG 14 WC Chemistry, Multidisciplinary SC Chemistry GA AY7DG UT WOS:000347720900088 ER PT J AU Feng, X Hu, JY Tomiyasu, H Tao, Z Redshaw, C Elsegood, MRJ Horsburgh, L Teat, SJ Wei, XF Yamato, T AF Feng, Xing Hu, Jian-Yong Tomiyasu, Hirotsugu Tao, Zhu Redshaw, Carl Elsegood, Mark R. J. Horsburgh, Lynne Teat, Simon J. Wei, Xian-Fu Yamato, Takehiko TI Iron(III) bromide catalyzed bromination of 2-tert-butylpyrene and corresponding position-dependent aryl-functionalized pyrene derivatives SO RSC ADVANCES LA English DT Article ID POLYCYCLIC AROMATIC-HYDROCARBONS; PHOTOPHYSICAL PROPERTIES; BLUE EMITTERS; EFFICIENT; PI; BORYLATION; SUBSTITUTION; DENDRIMERS AB The present work probes the bromination mechanism of 2-tert-butylpyrene (1), which regioselectively affords mono-, di-, tri- and tetra-bromopyrenes, by theoretical calculation and detailed experimental methods. The bromine atom may be directed to the K-region (positions 5- and 9-) instead of the more reactive 6- and 8-positions in the presence of iron powder. In this process, FeBr3 plays a significant role to release steric hindrance or lower the activation energy of the rearrangement. The intermediate bromopyrene derivatives were isolated and confirmed by H-1 NMR spectrometry, mass spectroscopy and elemental analysis. Further evidence on substitution position originated from a series of aryl substituted pyrene derivatives, which were obtained from the corresponding bromopyrenes on reaction with 4-methoxy-phenylboronic acid by a Suzuki-Miyaura cross-coupling reaction. All position-dependent aryl-functionalized pyrene derivatives are characterized by single X-ray diffraction, H-1/C-13 NMR, FT-IR and MS, and offered straightforward evidence to support our conclusion. Furthermore, the photophysical properties of a series of compounds were confirmed by fluorescence and absorption, as well as by fluorescence lifetime measurements. C1 [Feng, Xing; Wei, Xian-Fu] Beijing Inst Graph Commun, Beijing 102600, Peoples R China. [Feng, Xing; Hu, Jian-Yong; Tomiyasu, Hirotsugu; Yamato, Takehiko] Saga Univ, Fac Sci & Engn, Dept Appl Chem, Saga 8408502, Japan. [Hu, Jian-Yong] RIKEN, CEMS, Emergent Mol Funct Res Grp, Wako, Saitama 3510198, Japan. [Tao, Zhu] Guizhou Univ, Key Lab Macrocycl & Supramol Chem Guizhou Prov, Guiyang 550025, Guizhou, Peoples R China. [Redshaw, Carl] Univ Hull, Dept Chem, Kingston Upon Hull HU6 7RX, Yorks, England. [Elsegood, Mark R. J.; Horsburgh, Lynne] Univ Loughborough, Dept Chem, Loughborough LE11 3TU, Leics, England. [Teat, Simon J.] Berkeley Lab, ALS, Berkeley, CA 94720 USA. RP Yamato, T (reprint author), Saga Univ, Fac Sci & Engn, Dept Appl Chem, Honjo Machi 1, Saga 8408502, Japan. EM yamatot@cc.saga-u.ac.jp RI Redshaw, Carl/C-5644-2009 OI Redshaw, Carl/0000-0002-2090-1688 FU OTEC at Saga University; International Collaborative Project Fund of Guizhou province at Guizhou University; EPSRC; Royal Society of Chemistry; Scientific Research Common Program of Beijing Municipal Commission of Education; Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231] FX This work was performed under the Cooperative Research Program of "Network Joint Research Center for Materials and Devices (Institute for Materials Chemistry and Engineering, Kyushu University)". We would like to thank the OTEC at Saga University and the International Collaborative Project Fund of Guizhou province at Guizhou University for financial support. We also would like to thank the EPSRC and the Royal Society of Chemistry (travel grants to CR) and The Scientific Research Common Program of Beijing Municipal Commission of Education for financial support. Thanks Dr Kai Chen (Nanjing University) for refining the X-ray diffraction data for 3a, 3b and 3d. The Advanced Light Source is supported by the Director, Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract no. DE-AC02-05CH11231. NR 43 TC 2 Z9 2 U1 3 U2 20 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2046-2069 J9 RSC ADV JI RSC Adv. PY 2015 VL 5 IS 12 BP 8835 EP 8848 DI 10.1039/c4ra12216j PG 14 WC Chemistry, Multidisciplinary SC Chemistry GA AY7DK UT WOS:000347721300036 ER PT J AU Zayas, J AF Zayas, Jose TI Strengthening US Ocean Renewable Energy: 2014 Success Stories SO SEA TECHNOLOGY LA English DT Article C1 US DOE, Wind & Water Power Technol Off, Washington, DC 20585 USA. RP Zayas, J (reprint author), US DOE, Wind & Water Power Technol Off, Washington, DC 20585 USA. NR 0 TC 0 Z9 0 U1 0 U2 1 PU COMPASS PUBLICATIONS, INC PI ARLINGTON PA 1501 WILSON BLVD., STE 1001, ARLINGTON, VA 22209-2403 USA SN 0093-3651 J9 SEA TECHNOL JI Sea Technol. PD JAN PY 2015 VL 56 IS 1 BP 19 EP 21 PG 3 WC Engineering, Ocean SC Engineering GA CA4SN UT WOS:000348894800006 ER PT J AU Li, YT Han, JT Vogel, SC Wang, CA AF Li, Yutao Han, Jian-Tao Vogel, Sven C. Wang, Chang-An TI The reaction of Li6.5La3Zr1.5Ta0.5O12 with water SO SOLID STATE IONICS LA English DT Article DE Li-ion solid electrolyte; Garnet; Lithium-ion batteries; Ion exchange ID LITHIUM ION CONDUCTION; GARNET; ELECTROLYTES; LI7LA3ZR2O12; BATTERIES AB The Li-ion conductor "Li6.5La3Zr1.5Ta0.5O12" (LLZT) with garnet structure is prepared by solid-state reaction in an alumina crucible; its stability in water is investigated at room temperature. A Li+/H+ exchange is characterized by TGA, Li-7 and Al-27 MAS NMR, neutron diffraction, and TEM. In water, Li+/H+ exchange leads to a new garnet oxide "Li6.5-xHxLa3Zr1.5Ta0.5O12" (H-LLZT) with space group Ia-3d; the lattice parameter of H-LLZT is increased by the exchanged protons. Both LLZT and a grain boundary phase LiAlO2 are unstable in water. The exchanged protons in H-LLZT displace Li from the octahedral sites bridging the 24d tetrahedral sites; they form a strong O-H bond that distorted the site. The amorphous phase LiAlO2 in the grain boundary dissolves on exposure to water, which inhibits Li-ion transport across the grain boundary. (C) 2014 Elsevier B.V. All rights reserved. C1 [Li, Yutao; Wang, Chang-An] Tsinghua Univ, Sch Mat Sci & Engn, State Key Lab New Ceram & Fine Proc, Beijing 100084, Peoples R China. [Li, Yutao; Han, Jian-Tao] Univ Texas Austin, Mat Res Program, Austin, TX 78712 USA. [Li, Yutao; Han, Jian-Tao] Univ Texas Austin, Texas Mat Inst, Austin, TX 78712 USA. [Vogel, Sven C.] Los Alamos Natl Lab, LANSCE Lujan Ctr, Los Alamos, NM 87545 USA. RP Wang, CA (reprint author), Tsinghua Univ, Sch Mat Sci & Engn, State Key Lab New Ceram & Fine Proc, Beijing 100084, Peoples R China. EM wangca@mail.tsinghua.edu.cn RI Wang, Changan/I-4260-2012; OI Vogel, Sven C./0000-0003-2049-0361 FU National Natural Science Foundation of China (NSFC) [51221291] FX This work was supported by the National Natural Science Foundation of China (NSFC-No. 51221291). NR 18 TC 5 Z9 5 U1 8 U2 62 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0167-2738 EI 1872-7689 J9 SOLID STATE IONICS JI Solid State Ion. PD JAN PY 2015 VL 269 BP 57 EP 61 DI 10.1016/j.ssi.2014.11.010 PG 5 WC Chemistry, Physical; Physics, Condensed Matter SC Chemistry; Physics GA CA4NG UT WOS:000348880700010 ER PT J AU Wang, X Chen, MH Kuo, RC Dey, DK AF Wang, Xia Chen, Ming-Hui Kuo, Rita C. Dey, Dipak K. TI BAYESIAN SPATIAL-TEMPORAL MODELING OF ECOLOGICAL ZERO-INFLATED COUNT DATA SO STATISTICA SINICA LA English DT Article DE Bayesian hierarchical modeling; deviance information criterion; log predictive score; spatial dynamic modeling; zero-inflated Poisson ID LINEAR MIXED MODELS; COD GADUS-MORHUA; ATLANTIC COD; CLIMATE-CHANGE; RESPONSE DATA; R-PACKAGE; POSTERIOR; BINARY AB A Bayesian hierarchical model is developed for count data with spatial and temporal correlations as well as excessive zeros, uneven sampling intensities, and inference on missing spots. Our contribution is to develop a model on zero-inflated count data that provides flexibility in modeling spatial patterns in a dynamic manner and also improves the computational efficiency via dimension reduction. The proposed methodology is of particular importance for studying species presence and abundance in the field of ecological sciences. The proposed model is employed in the analysis of the survey data by the Northeast Fisheries Sciences Center (NEFSC) for estimation and prediction of the Atlantic cod in the Gulf of Maine - Georges Bank region. Model comparisons based on the deviance information criterion and the log predictive score show the improvement by the proposed spatial-temporal model. C1 [Wang, Xia] Univ Cincinnati, Dept Math Sci, Cincinnati, OH 45221 USA. [Chen, Ming-Hui; Dey, Dipak K.] Univ Connecticut, Dept Stat, Storrs, CT 06269 USA. [Kuo, Rita C.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Joint Genome Inst, Berkeley, CA 94720 USA. RP Wang, X (reprint author), Univ Cincinnati, Dept Math Sci, 2815 Commons Way Cincinnati, Cincinnati, OH 45221 USA. EM xia.wang@uc.edu; ming-hui.chen@uconn.edu; chykuo@gmail.com; dipak.dey@uconn.edu FU US National Institutes of Health [GM 70335, CA 74015]; Statistical and Applied Mathematical Sciences Institute (SAMSI) FX We thank the Guest Editor and the referee for their helpful comments and suggestions, which have led to a much improved version of the paper. Dr. Chen's research was partially supported by US National Institutes of Health under Grants #GM 70335 and #CA 74015. Dr. Wang thanks the travel support provided by the Faculty Development Council at the University of Cincinnati. This project benefits from the Statistical and Applied Mathematical Sciences Institute (SAMSI) 2009-2010 and 2012-2013 programs. NR 32 TC 0 Z9 0 U1 1 U2 14 PU STATISTICA SINICA PI TAIPEI PA C/O DR H C HO, INST STATISTICAL SCIENCE, ACADEMIA SINICA, TAIPEI 115, TAIWAN SN 1017-0405 EI 1996-8507 J9 STAT SINICA JI Stat. Sin. PD JAN PY 2015 VL 25 IS 1 BP 189 EP 204 DI 10.5705/ss.2013.212w PG 16 WC Statistics & Probability SC Mathematics GA CA5TC UT WOS:000348969700012 PM 26997848 ER PT J AU Riahi, K Kriegler, E Johnson, N Bertram, C den Elzen, M Eom, J Schaeffer, M Edmonds, J Isaac, M Krey, V Longden, T Luderer, G Mejean, A McCollum, DL Mima, S Turton, H van Vuuren, DP Wada, K Bosetti, V Capros, P Criqui, P Hamdi-Cherif, M Kainuma, M Edenhofer, O AF Riahi, Keywan Kriegler, Elmar Johnson, Nils Bertram, Christoph den Elzen, Michel Eom, Jiyong Schaeffer, Michiel Edmonds, Jae Isaac, Morna Krey, Volker Longden, Thomas Luderer, Gunnar Mejean, Aurelie McCollum, David L. Mima, Silvana Turton, Hal van Vuuren, Detlef P. Wada, Kenichi Bosetti, Valentina Capros, Pantelis Criqui, Patrick Hamdi-Cherif, Meriem Kainuma, Mikiko Edenhofer, Ottmar TI Locked into Copenhagen pledges - Implications of short-term emission targets for the cost and feasibility of long-term climate goals SO TECHNOLOGICAL FORECASTING AND SOCIAL CHANGE LA English DT Article DE Copenhagen pledges; Climate policy; AMPERE; Mitigation; Greenhouse gas emissions ID CARBON-CYCLE MODELS; 2 DEGREES-C; CO2 CONCENTRATIONS; CHANGE MITIGATION; ATMOSPHERE-OCEAN; SIMPLER MODEL; BIO-ENERGY; ECONOMICS; SCENARIOS; INERTIA AB This paper provides an overview of the AMPERE modeling comparison project with focus on the implications of near-term policies for the costs and attainability of long-term climate objectives. Nine modeling teams participated in the project to explore the consequences of global emissions following the proposed policy stringency of the national pledges from the Copenhagen Accord and Cancun Agreements to 2030. Specific features compared to earlier assessments are the explicit consideration of near-term 2030 emission targets as well as the systematic sensitivity analysis for the availability and potential of mitigation technologies. Our estimates show that a 2030 mitigation effort comparable to the pledges would result in a further "lock-in" of the energy system into fossil fuels and thus impede the required energy transformation to reach low greenhouse-gas stabilization levels (450 ppm CO(2)e). Major implications include significant increases in mitigation costs, increased risk that low stabilization targets become unattainable, and reduced chances of staying below the proposed temperature change target of 2 degrees C in case of overshoot. With respect to technologies, we find that following the pledge pathways to 2030 would narrow policy choices, and increases the risks that some currently optional technologies, such as carbon capture and storage (CCS) or the large-scale deployment of bioenergy, will become "a must" by 2030. (C) 2014 The Authors. Published by Elsevier B.V. C1 [Riahi, Keywan; Krey, Volker; McCollum, David L.] Int Inst Appl Syst Anal, Energy Program, A-2361 Laxenburg, Austria. [Johnson, Nils] Int Inst Appl Syst Anal, A-2361 Laxenburg, Austria. [Riahi, Keywan] Graz Univ Technol, A-8010 Graz, Austria. [Kriegler, Elmar; Luderer, Gunnar; Edenhofer, Ottmar] Potsdam Inst Climate Impact Res PIK, Potsdam, Germany. [den Elzen, Michel; Isaac, Morna; van Vuuren, Detlef P.] PBL Netherlands Environm Assessment Agcy, Utrecht, Netherlands. [Eom, Jiyong; Edmonds, Jae] Pacific NW Natl Lab, Joint Global Change Res Inst, College Pk, MD USA. [Schaeffer, Michiel] Climate Analyt, Berlin, Germany. [Longden, Thomas; Bosetti, Valentina] FEEM, Milan, Italy. [Mejean, Aurelie; Hamdi-Cherif, Meriem] CIRED, Nogent Sur Marne, France. [Mima, Silvana; Criqui, Patrick] IEPE, Grenoble, France. [Turton, Hal] Paul Scherrer Inst, Energy Econ Grp, Villigen, Switzerland. [van Vuuren, Detlef P.] Univ Utrecht, Dept Geosci, Utrecht, Netherlands. [Wada, Kenichi] Res Inst Innovat Technol Earth RITE, Syst Anal Grp, Kyoto, Japan. [Capros, Pantelis] NTUA, Dept Elect & Comp Engn, E3M Lab ICCS Lab, Athens, Greece. [Kainuma, Mikiko] NIES, Tsukuba, Ibaraki, Japan. [Bosetti, Valentina] Bocconi Univ, Dept Econ, Milan, Italy. [Edenhofer, Ottmar] Tech Univ Berlin, Berlin, Germany. [Edenhofer, Ottmar] Mercator Res Inst Global Commons & Climate Change, Berlin, Germany. [Bertram, Christoph] Potsdam Inst Climate Impact Res PIK, Global Energy Syst Res Grp, Potsdam, Germany. RP Riahi, K (reprint author), Int Inst Appl Syst Anal, Schlosspl 1, A-2361 Laxenburg, Austria. EM riahi@iiasa.ac.at RI Luderer, Gunnar/G-2967-2012; Edenhofer, Ottmar/E-1886-2013; van Vuuren, Detlef/A-4764-2009; Eom, Jiyong/A-1161-2014; Kriegler, Elmar/I-3048-2016; Longden, Thomas/I-7977-2015; den Elzen, Michel/M-2779-2016; Riahi, Keywan/B-6426-2011; OI Edenhofer, Ottmar/0000-0001-6029-5208; van Vuuren, Detlef/0000-0003-0398-2831; Kriegler, Elmar/0000-0002-3307-2647; Longden, Thomas/0000-0001-7593-659X; den Elzen, Michel/0000-0002-5128-8150; Riahi, Keywan/0000-0001-7193-3498; bosetti, valentina/0000-0003-4970-0027 NR 75 TC 57 Z9 57 U1 8 U2 44 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 0040-1625 EI 1873-5509 J9 TECHNOL FORECAST SOC JI Technol. Forecast. Soc. Chang. PD JAN PY 2015 VL 90 SI SI BP 8 EP 23 DI 10.1016/j.techfore.2013.09.016 PN A PG 16 WC Business; Planning & Development SC Business & Economics; Public Administration GA AY5IG UT WOS:000347605300002 ER PT J AU Kriegler, E Riahi, K Bauer, N Schwanitz, VJ Petermann, N Bosetti, V Marcucci, A Otto, S Paroussos, L Rao, S Curras, TA Ashina, S Bollen, J Eom, J Hamdi-Cherif, M Longden, T Kitous, A Mejean, A Sano, F Schaeffer, M Wada, K Capros, P van Vuuren, DP Edenhofer, O AF Kriegler, Elmar Riahi, Keywan Bauer, Nico Schwanitz, Valeria Jana Petermann, Nils Bosetti, Valentina Marcucci, Adriana Otto, Sander Paroussos, Leonidas Rao, Shilpa Curras, Tabare Arroyo Ashina, Shuichi Bollen, Johannes Eom, Jiyong Hamdi-Cherif, Meriem Longden, Thomas Kitous, Alban Mejean, Aurelie Sano, Fuminori Schaeffer, Michiel Wada, Kenichi Capros, Pantelis van Vuuren, Detlef P. Edenhofer, Ottmar TI Making or breaking climate targets: The AMPERE study on staged accession scenarios for climate policy SO TECHNOLOGICAL FORECASTING AND SOCIAL CHANGE LA English DT Article DE Climate change mitigation; Integrated assessment models; Climate change economics; Carbon leakage; European Union; Regional climate policies ID CARBON LEAKAGE; TECHNOLOGICAL-CHANGE; CHANGE MITIGATION; MODEL; EMISSIONS; MARKETS; REGIMES; EXAMPLE; CHINA; WORLD AB This study explores a situation of staged accession to a global climate policy regime from the current situation of regionally fragmented and moderate climate action. The analysis is based on scenarios in which a front runner coalition - the EU or the EU and China - embarks on immediate ambitious climate action while the rest of the world makes a transition to a global climate regime between 2030 and 2050. We assume that the ensuing regime involves strong mitigation efforts but does not require late joiners to compensate for their initially higher emissions. Thus, climate targets are relaxed, and although staged accession can achieve significant reductions of global warming, the resulting climate outcome is unlikely to be consistent with the goal of limiting global warming to 2 degrees. The addition of China to the front runner coalition can reduce pre-2050 excess emissions by 20-30%, increasing the likelihood of staying below 2 degrees. Not accounting for potential co-benefits, the cost of front runner action is found to be lower for the EU than for China. Regions that delay their accession to the climate regime face a trade-off between reduced short term costs and higher transitional requirements due to larger carbon lock-ins and more rapidly increasing carbon prices during the accession period. (C) 2014 The Authors. Published by Elsevier Inc. C1 [Kriegler, Elmar; Bauer, Nico; Schwanitz, Valeria Jana; Petermann, Nils; Curras, Tabare Arroyo; Edenhofer, Ottmar] Potsdam Inst Climate Impact Res, Potsdam, Germany. [Riahi, Keywan] Int Inst Appl Syst Anal, Energy Program, A-2361 Laxenburg, Austria. [Rao, Shilpa] Int Inst Appl Syst Anal, A-2361 Laxenburg, Austria. [Bosetti, Valentina] Fdn Eni Enrico Mattei, Sustainable Dev Programme, Milan, Italy. [Longden, Thomas] Fdn Eni Enrico Mattei, Milan, Italy. [Marcucci, Adriana] Paul Scherrer Inst, Safety & Environm Technol Grp, Villigen, Switzerland. [Marcucci, Adriana] Paul Scherrer Inst, Energy Econ Grp, Villigen, Switzerland. [Marcucci, Adriana] Swiss Fed Inst Technol, Zurich, Switzerland. [Otto, Sander] Univ Utrecht, Copernicus Inst Sustainable Dev, Global Change Modeling Team, Utrecht, Netherlands. [van Vuuren, Detlef P.] Univ Utrecht, Copernicus Inst Sustainable Dev, Utrecht, Netherlands. [Paroussos, Leonidas; Capros, Pantelis] Inst Commun & Comp Syst, Athens, Greece. [Ashina, Shuichi] Natl Inst Environm Studies, Ctr Social & Environm Syst Res, Tsukuba, Ibaraki, Japan. [Bollen, Johannes] CPB Netherlands Bur Econ Policy Anal, The Hague, Netherlands. [Eom, Jiyong] Pacific NW Natl Lab, Joint Global Change Res Inst, College Pk, MD USA. [Hamdi-Cherif, Meriem; Mejean, Aurelie] Ctr Int Rech Environm & Dev, Paris, France. [Kitous, Alban] European Commiss Joint Res Ctr, Seville, Spain. [Sano, Fuminori] Res Inst Innovat Technol Earth, Kizugawa, Japan. [Wada, Kenichi] Res Inst Innovat Technol Earth, Syst Anal Grp, Kizugawa, Japan. [Schaeffer, Michiel] Climate Analyt, Berlin, Germany. [van Vuuren, Detlef P.] PBL Netherlands Environm Assessment Agcy, Bilthoven, Netherlands. [Edenhofer, Ottmar] Tech Univ Berlin, Berlin, Germany. [Edenhofer, Ottmar] Mercator Res Inst Global Commons & Climate Change, Berlin, Germany. RP Kriegler, E (reprint author), Potsdam Inst Climate Impact Res PIK, Telegraphenberg A31, D-14473 Potsdam, Germany. EM kriegler@pik-potsdam.de RI Edenhofer, Ottmar/E-1886-2013; Schwanitz, Valeria Jana/H-1414-2015; Longden, Thomas/I-7977-2015; van Vuuren, Detlef/A-4764-2009; Eom, Jiyong/A-1161-2014; Kriegler, Elmar/I-3048-2016; Riahi, Keywan/B-6426-2011; OI Edenhofer, Ottmar/0000-0001-6029-5208; Schwanitz, Valeria Jana/0000-0002-8752-2754; Longden, Thomas/0000-0001-7593-659X; van Vuuren, Detlef/0000-0003-0398-2831; Kriegler, Elmar/0000-0002-3307-2647; Riahi, Keywan/0000-0001-7193-3498; Marcucci, Adriana/0000-0002-0427-9120; bosetti, valentina/0000-0003-4970-0027 NR 73 TC 33 Z9 33 U1 5 U2 28 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 0040-1625 EI 1873-5509 J9 TECHNOL FORECAST SOC JI Technol. Forecast. Soc. Chang. PD JAN PY 2015 VL 90 SI SI BP 24 EP 44 DI 10.1016/j.techfore.2013.09.021 PN A PG 21 WC Business; Planning & Development SC Business & Economics; Public Administration GA AY5IG UT WOS:000347605300003 ER PT J AU Bertram, C Johnson, N Luderer, G Riahi, K Isaac, M Eom, J AF Bertram, Christoph Johnson, Nils Luderer, Gunnar Riahi, Keyvvan Isaac, Morna Eom, Jiyong TI Carbon lock-in through capital stock inertia associated with weak near-term climate policies SO TECHNOLOGICAL FORECASTING AND SOCIAL CHANGE LA English DT Article DE Climate change mitigation; Energy systems modeling; Energy efficiency; Carbon dioxide emissions; AMPERE; Integrated assessment ID MODEL; WORLD; COSTS AB Stringent long-term climate targets necessitate a limit on cumulative emissions in this century for which sufficient policy signals are lacking. Using nine energy-economy models, we explore how policies pursued during the next two decades impact long-term transformation pathways towards stringent long-term climate targets. Less stringent near-term policies (i.e., those with larger emissions) consume more of the long-term cumulative emissions budget in the 2010-2030 period, which increases the likelihood of overshooting the budget and the urgency of reducing GHG emissions after 2030. Furthermore, the larger near-term GHG emissions associated with less stringent policies are generated primarily by additional coal-based electricity generation. Therefore, to be successful in meeting the long-term target despite near-term emissions reductions that are weaker than those implied by cost-optimal mitigation pathways, models must prematurely retire significant coal capacity while rapidly ramping up low-carbon technologies between 2030 and 2050 and remove large quantities of CO2 from the atmosphere in the latter half of the century. While increased energy efficiency lowers mitigation costs considerably, even with weak near-term policies, it does not substantially reduce the short-term reliance on coal electricity. However, increased energy efficiency does allow the energy system more flexibility in mitigating emissions and, thus, facilitates the post-2030 transition. (C) 2014 The Authors. Published by Elsevier Inc. C1 [Bertram, Christoph; Luderer, Gunnar] Potsdam Inst Climate Impact Res, D-14473 Potsdam, Germany. [Johnson, Nils; Riahi, Keyvvan] Int Inst Appl Syst Anal, A-2361 Laxenburg, Austria. [Riahi, Keyvvan] Graz Univ Technol, A-8010 Graz, Austria. [Isaac, Morna] Univ Utrecht, Copernicus Inst Sustainable Dev, NL-3584 CS Utrecht, Netherlands. [Eom, Jiyong] Pacific NW Natl Lab, Joint Global Change Res Inst, College Pk, MD 20740 USA. RP Bertram, C (reprint author), POB 601203, D-14412 Potsdam, Germany. EM bertram@pik-potsdam.de RI Luderer, Gunnar/G-2967-2012; Eom, Jiyong/A-1161-2014; Riahi, Keywan/B-6426-2011 OI Riahi, Keywan/0000-0001-7193-3498 NR 31 TC 19 Z9 19 U1 1 U2 12 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 0040-1625 EI 1873-5509 J9 TECHNOL FORECAST SOC JI Technol. Forecast. Soc. Chang. PD JAN PY 2015 VL 90 SI SI BP 62 EP 72 DI 10.1016/j.techfore.2013.10.001 PN A PG 11 WC Business; Planning & Development SC Business & Economics; Public Administration GA AY5IG UT WOS:000347605300005 ER PT J AU Eom, J Edmonds, J Krey, V Johnson, N Longden, T Luderer, G Riahi, K Van Vuuren, DP AF Eom, Jiyong Edmonds, Jae Krey, Volker Johnson, Nils Longden, Thomas Luderer, Gunnar Riahi, Keyvvan Van Vuuren, Detlef P. TI The impact of near-term climate policy choices on technology and emission transition pathways SO TECHNOLOGICAL FORECASTING AND SOCIAL CHANGE LA English DT Article DE Near-term climate policy; Technology deployment; Emission pathway; Technology upscaling ID INTEGRATED ASSESSMENT; CO2 CONCENTRATIONS; MERGE MODEL AB This paper explores the implications of delays (to 2030) in implementing optimal policies for long-term transition pathways to limit climate forcing to 450 ppm CO(2)e on the basis of the AMPERE Work Package 2 model comparison study. The paper highlights the critical importance of the period 2030-2050 for ambitious mitigation strategies. In this period, the most rapid shift to low greenhouse gas emitting technology occurs. In the delayed response emission mitigation scenarios, an even faster transition rate in this period is required to compensate for the additional emissions before 2030. Our physical deployment measures indicate that the availability of CCS technology could play a critical role in facilitating the attainment of ambitious mitigation goals. Without CCS, deployment of other mitigation technologies would become extremely high in the 2030-2050 period. Yet the presence of CCS greatly alleviates the challenges to the transition particularly after the delayed climate policies, lowering the risk that the long-term goal becomes unattainable. The results also highlight the important role of bioenergy with CO2 capture and storage (BECCS), which facilitates energy production with negative carbon emissions. If BECCS is available, transition pathways exceed the emission budget in the mid-term, removing the excess with BECCS in the long term. Excluding either BE or CCS from the technology portfolio implies that emission reductions need to take place much earlier. (C) 2013 Elsevier Inc. C1 [Eom, Jiyong] Sogang Univ, Grad Sch Management Technol, Seoul 121742, South Korea. [Edmonds, Jae] Pacific NW Natl Lab, Joint Global Change Res Inst, College Pk, MD 20740 USA. [Krey, Volker; Johnson, Nils; Riahi, Keyvvan] Int Inst Appl Syst Anal, A-2361 Laxenburg, Austria. [Longden, Thomas] Fdn ENI Enrico Mattei, Venice, Italy. [Longden, Thomas] Euromediterranean Ctr Climate Change, Venice, Italy. [Luderer, Gunnar] Potsdam Inst Climate Impact Res, D-14473 Potsdam, Germany. [Van Vuuren, Detlef P.] PBL Netherlands Environm Assessment Agcy, NL-3720 AH Bilthoven, Netherlands. [Van Vuuren, Detlef P.] Univ Utrecht, Copernicus Inst Sustainable Dev, Utrecht, Netherlands. RP Eom, J (reprint author), Sogang Univ, Grad Sch Management Technol, Seoul 121742, South Korea. EM eomjiyong@sogang.ac.kr RI Luderer, Gunnar/G-2967-2012; Longden, Thomas/I-7977-2015; van Vuuren, Detlef/A-4764-2009; Eom, Jiyong/A-1161-2014; Riahi, Keywan/B-6426-2011 OI Longden, Thomas/0000-0001-7593-659X; van Vuuren, Detlef/0000-0003-0398-2831; Riahi, Keywan/0000-0001-7193-3498 NR 49 TC 19 Z9 19 U1 1 U2 13 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 0040-1625 EI 1873-5509 J9 TECHNOL FORECAST SOC JI Technol. Forecast. Soc. Chang. PD JAN PY 2015 VL 90 SI SI BP 73 EP 88 DI 10.1016/j.techfore.2013.09.017 PN A PG 16 WC Business; Planning & Development SC Business & Economics; Public Administration GA AY5IG UT WOS:000347605300006 ER PT J AU Iyer, G Hultman, N Eom, J McJeon, H Patel, P Clarke, L AF Iyer, Gokul Hultman, Nathan Eom, Jiyong McJeon, Haewon Patel, Pralit Clarke, Leon TI Diffusion of low-carbon technologies and the feasibility of long-term climate targets SO TECHNOLOGICAL FORECASTING AND SOCIAL CHANGE LA English DT Article DE Climate change; Technology diffusion; Carbon-free energy ID RENEWABLE ENERGY TECHNOLOGY; INTEGRATED ASSESSMENT; ENVIRONMENTAL-POLICY; UNITED-KINGDOM; WIND ENERGY; STORAGE CCS; BARRIERS; CAPTURE; STABILIZATION; FRAMEWORK AB Stabilizing the global climate will require large-scale global deployment of low-carbon technologies. Even in the presence of aggressive climate policies, however, the diffusion of such technologies may be limited by several institutional, behavioral, and social factors. In this paper, we review the literature on the sources of such diffusion constraints, and explore the potential implications of such constraints based on the GCAM integrated assessment model. Our analysis highlights that factors that limit technology deployment may have sizeable impacts on the feasibility and mitigation costs of achieving stringent stabilization targets. And such impacts are greatly amplified with major delays in serious climate policies. The results generally indicate that constraints on the expansions of CCS and renewables are more costly than those on nuclear or bioenergy, and jointly constraining these technologies leaves some scenarios infeasible. (C) 2013 Elsevier Inc. All rights reserved. C1 [Iyer, Gokul; Hultman, Nathan] Univ Maryland, Sch Publ Policy, College Pk, MD 20742 USA. [Iyer, Gokul; Hultman, Nathan; McJeon, Haewon; Patel, Pralit; Clarke, Leon] Pacific NW Natl Lab, Joint Global Change Res Inst, College Pk, MD 20740 USA. [Iyer, Gokul; Hultman, Nathan; McJeon, Haewon; Patel, Pralit; Clarke, Leon] Univ Maryland, College Pk, MD 20740 USA. [Eom, Jiyong] Sogang Univ, Grad Sch Management Technol, Seoul 121742, South Korea. RP Iyer, G (reprint author), Pacific NW Natl Lab, Joint Global Change Res Inst, 5825 Univ Res Court,Suite 3500, College Pk, MD 20740 USA. EM giyer@umd.edu; hultman@umd.edu; eomjiyong@sogang.ac.kr; Haewon.Mcjeon@pnnl.gov; pralit.patel@pnnl.gov; leon.clarke@pnnl.gov RI Eom, Jiyong/A-1161-2014 NR 76 TC 18 Z9 18 U1 5 U2 17 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 0040-1625 EI 1873-5509 J9 TECHNOL FORECAST SOC JI Technol. Forecast. Soc. Chang. PD JAN PY 2015 VL 90 SI SI BP 103 EP 118 DI 10.1016/j.techfore.2013.08.025 PN A PG 16 WC Business; Planning & Development SC Business & Economics; Public Administration GA AY5IG UT WOS:000347605300008 ER PT J AU Bauer, N Bosetti, V Hamdi-Cherif, M Kitous, A McCollum, D Mejean, A Rao, CS Turton, H Paroussos, L Ashina, S Calvin, K Wada, K van Vuuren, D AF Bauer, Nico Bosetti, Valentina Hamdi-Cherif, Meriem Kitous, Alban McCollum, David Mejean, Aurelie Rao, C. Shilpa Turton, Hal Paroussos, Leonidas Ashina, Shuichi Calvin, Katherine Wada, Kenichi van Vuuren, Detlef TI CO2 emission mitigation and fossil fuel markets: Dynamic and international aspects of climate policies SO TECHNOLOGICAL FORECASTING AND SOCIAL CHANGE LA English DT Article DE Climate change mitigation policies; Fossil fuel markets; Copenhagen Accord; Carbon leakage; Inter-fuel substitution ID CARBON LEAKAGE; STABILIZATION AB This paper explores a multi-model scenario ensemble to assess the impacts of idealized and non-idealized climate change stabilization policies on fossil fuel markets. Under idealized conditions climate policies significantly reduce coal use in the short- and long-term. Reductions in oil and gas use are much smaller, particularly until 2030, but revenues decrease much more because oil and gas prices are higher than coal prices. A first deviation from optimal transition pathways is delayed action that relaxes global emission targets until 2030 in accordance with the Copenhagen pledges. Fossil fuel markets revert back to the no-policy case: though coal use increases strongest, revenue gains are higher for oil and gas. To balance the carbon budget over the 21st century, the long-term reallocation of fossil fuels is significantly larger twice and more than the short-term distortion. This amplifying effect results from coal lock-in and inter-fuel substitution effects to balance the full-century carbon budget. The second deviation from the optimal transition pathway relaxes the global participation assumption. The result here is less clear-cut across models, as we find carbon leakage effects ranging from positive to negative because trade and substitution patterns of coal, oil, and gas differ across models. In summary, distortions of fossil fuel markets resulting from relaxed short-term global emission targets are more important and less uncertain than the issue of carbon leakage from early mover action. (C) 2014 The Authors. Published by Elsevier B.V. C1 [Bauer, Nico] Potsdam Inst Climate Impact Res PIK, Energy Resources & Technol Grp Sustainable Solut, Potsdam, Germany. [Bosetti, Valentina] FEEM, Sustainable Dev Programme, Milan, Italy. [Hamdi-Cherif, Meriem; Mejean, Aurelie] CIRED, Paris, France. [Kitous, Alban] Joint Res Ctr, Inst Prospect Technol Studies, Seville, Spain. [McCollum, David; Rao, C. Shilpa] Int Inst Appl Syst Anal, Energy Program, A-2361 Laxenburg, Austria. [Turton, Hal] Paul Scherrer Inst, Energy Econ Grp, Villigen, Switzerland. [Paroussos, Leonidas] Natl Tech Univ Athens, GR-10682 Athens, Greece. [Ashina, Shuichi] Natl Inst Environm Studies, Ctr Social & Environm Syst Res, Tsukuba, Ibaraki, Japan. [Calvin, Katherine] Pacific NW Natl Lab, Joint Global Change Res Inst, College Pk, MD USA. [Wada, Kenichi] Res Inst Innovat Technol Earth RITE, Syst Anal Grp, Kyoto, Japan. [van Vuuren, Detlef] Netherlands Environm Assessment Agcy PBL, Bilthoven, Netherlands. [van Vuuren, Detlef] Univ Utrecht, Dept Geosci, Copernicus Inst, Utrecht, Netherlands. RP Bauer, N (reprint author), POB 601203, D-14412 Potsdam, Germany. EM nico.bauer@pik-potsdam.de RI van Vuuren, Detlef/A-4764-2009; OI van Vuuren, Detlef/0000-0003-0398-2831; Bauer, Nico/0000-0002-0211-4162; bosetti, valentina/0000-0003-4970-0027; Calvin, Katherine/0000-0003-2191-4189 NR 28 TC 19 Z9 19 U1 4 U2 22 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 0040-1625 EI 1873-5509 J9 TECHNOL FORECAST SOC JI Technol. Forecast. Soc. Chang. PD JAN PY 2015 VL 90 SI SI BP 243 EP 256 DI 10.1016/j.techfore.2013.09.009 PN A PG 14 WC Business; Planning & Development SC Business & Economics; Public Administration GA AY5IG UT WOS:000347605300018 ER PT J AU Goh, T Huang, JS Bielinski, EA Thompson, BA Tomasulo, S Lee, ML Sfeir, MY Hazari, N Taylor, AD AF Goh, Tenghooi Huang, Jing-Shun Bielinski, Elizabeth A. Thompson, Bennett A. Tomasulo, Stephanie Lee, Minjoo L. Sfeir, Matthew Y. Hazari, Nilay Taylor, Andre D. TI Coevaporated Bisquaraine Inverted Solar Cells: Enhancement Due to Energy Transfer and Open Circuit Voltage Control SO ACS PHOTONICS LA English DT Article DE small-molecule solar cells; Forster resonance energy transfer; open circuit voltage control; thermal coevaporation; photophysics ID POWER-CONVERSION EFFICIENCY; 25TH ANNIVERSARY ARTICLE; SQUARAINE DYES; PHOTOVOLTAIC PERFORMANCE; TERNARY BLENDS; HETEROJUNCTION; BULK; INTERFACE; MECHANISM; ELECTRON AB There is currently enormous interest in the development of small molecule organic solar cells (SMSC), as in principle, these systems offer advantages over both conventional Si photovoltaics and organic polymer solar cells. Here, we report Forster Resonance Energy Transfer (FRET) enhanced inverted SMSC fabricated by coevaporating two different squaraine donors, a symmetrical squaraine (SQ, 2,4-bis-4-[(N,N-diisobutylamino)-2,6-dihydroxyphenyl] squaraine), and an asymmetrical squaraine (ASSQ, 2,4-bis-[(N,N-diisobutylamino)-2,6-dihydroxyphenyl]-4-(4-diphenyliminio) squaraine). ASSQ absorbs blue light (lambda(max) 540 nm) and emits from 550 nm to the near-infrared region, which overlaps with SQ absorption (lambda(max) 690 nm). Therefore, by utilizing a thin film containing the two squaraine donors as the active layer in a SMSC, we can both broaden the photovoltaic absorption spectrum, and reduce recombination loss as a result of FRET. This strategy has resulted in SMSC with power conversion efficiencies (PCE) which are up to 46% greater than those obtained by using a single squaraine donor. Ultrafast time-resolved photoluminescence and transient absorption spectroscopy provide clear evidence of FRET between the small molecules, with a rapid energy transfer time of similar to 1 ps. At optimal blending, which correlates to the highest PCE measured, the efficiency of energy transfer is as high as 85%. Furthermore, in the devices containing two different squaraine molecules, the open circuit voltage (V-OC) is proportional to the fraction of the two donors in the blend, allowing us to predict the V-OC as the ratio of the two donors is changed. SMSC with inverted structures also demonstrate long-term stability in ambient conditions compared to devices employing a conventional architecture. C1 [Goh, Tenghooi; Huang, Jing-Shun; Taylor, Andre D.] Yale Univ, Dept Chem & Environm Engn, New Haven, CT 06511 USA. [Bielinski, Elizabeth A.; Thompson, Bennett A.; Hazari, Nilay] Yale Univ, Dept Chem, New Haven, CT 06511 USA. [Tomasulo, Stephanie; Lee, Minjoo L.] Yale Univ, Dept Elect Engn, New Haven, CT 06511 USA. [Sfeir, Matthew Y.] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. RP Taylor, AD (reprint author), Yale Univ, Dept Chem & Environm Engn, New Haven, CT 06511 USA. EM andre.taylor@yale.edu RI Lee, Minjoo/A-9720-2008; OI Lee, Minjoo/0000-0002-3151-3808; Sfeir, Matthew/0000-0001-5619-5722 FU National Science Foundation [DMR-1410171]; Yale Climate and Energy Institute (YCEI); NSF-CAREER award [CBET-0954985]; U.S. Department of Energy, Office of Basic Energy Sciences [DE-AC02-98CH10886]; YINQE; NSF MRSEC (CRISP) [DMR 1119826] FX The authors gratefully acknowledge the National Science Foundation (DMR-1410171) and the Yale Climate and Energy Institute (YCEI) for partial support of this work. A.D.T. also acknowledges support from the NSF-CAREER award (CBET-0954985). The authors appreciate the help of Dr. Kevin Yager with the GIWAXS experiments. This research was carried out in part at the Center for Functional Nanomaterials, Brookhaven National Laboratory, which is supported by the U.S. Department of Energy, Office of Basic Energy Sciences, under Contract No. DE-AC02-98CH10886. Facilities use was supported by YINQE and NSF MRSEC DMR 1119826 (CRISP). NR 59 TC 16 Z9 17 U1 9 U2 45 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 2330-4022 J9 ACS PHOTONICS JI ACS Photonics PD JAN PY 2015 VL 2 IS 1 BP 86 EP 95 DI 10.1021/ph500282z PG 10 WC Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Optics; Physics, Applied; Physics, Condensed Matter SC Science & Technology - Other Topics; Materials Science; Optics; Physics GA AZ6OS UT WOS:000348339400014 ER PT J AU Zhou, X Deeb, C Kostcheev, S Wiederrecht, GP Adam, PM Beal, J Plain, J Gosztola, DJ Grand, J Felidj, N Wang, H Vial, A Bachelott, R AF Zhou, Xuan Deeb, Claire Kostcheev, Sergei Wiederrecht, Gary P. Adam, Pierre-Michel Beal, Jeremie Plain, Jerome Gosztola, David J. Grand, Johan Felidj, Nordin Wang, Huan Vial, Alexandre Bachelott, Renaud TI Selective Functionalization of the Nanogap of a Plasmonic Dimer SO ACS PHOTONICS LA English DT Article DE photopolymerization; photonics; hybrid nanostructures; surface plasmons; surface-enhanced Raman spectroscopy ID SURFACE-ENHANCED RAMAN; GOLD NANOSTRUCTURES; NANOPARTICLES; SPECTROSCOPY; FLUORESCENCE; RESONANCE; MOLECULE; PHOTOPOLYMERIZATION; QUANTIFICATION; POLARIZATION AB We report a self-developing anisotropic gold/polymer hybrid nanosystem that precisely places dye molecules at the plasmonic hotspot of metal nanostructures for sensing and photonics applications. Unlike conventional molecule-particle configurations, the anisotropic hybrid (AHN) nanosystem introduces an anisotropic spatial distribution of dye-containing active medium. This allows us to precisely overlap the near-field spatial distribution with the active medium and rule out the contribution from the background molecules. This overlap effect selectively highlights the optical response of the molecules of interest, that is, molecules located at the hotspots. Our AHN consists of gold nanodimers whose gaps have been filled with methylene blue molecules. They have been studied by plasmon-enhanced Raman spectroscopy as a probing tool. The AHN opens new doors not only for fundamental studies and photonics applications of molecule-particle interactions, but also for molecular trapping methods at the nanoscale. C1 [Zhou, Xuan; Deeb, Claire; Kostcheev, Sergei; Adam, Pierre-Michel; Beal, Jeremie; Plain, Jerome; Wang, Huan; Vial, Alexandre; Bachelott, Renaud] Univ Technol Troyes, CNRS UMR 6281, Lab Nanotechnol & Instrumentat Opt, F-10004 Troyes, France. [Wiederrecht, Gary P.; Gosztola, David J.] Argonne Natl Lab, Ctr Nanoscale Mat, Argonne, IL 60439 USA. [Grand, Johan; Felidj, Nordin] Univ Paris Diderot, Sorbonne Paris Cite, CNRS UMR 7086, F-75205 Paris 13, France. RP Bachelott, R (reprint author), Univ Technol Troyes, CNRS UMR 6281, Lab Nanotechnol & Instrumentat Opt, 12 Rue Marie Curie CS42060, F-10004 Troyes, France. EM renaud.bachelot@utt.fr RI Vial, Alexandre/I-7894-2012; Gosztola, David/D-9320-2011; OI Vial, Alexandre/0000-0002-7701-0413; Gosztola, David/0000-0003-2674-1379; Deeb, Claire/0000-0002-1323-0660 FU Agence Nationale de la Recherche (ANR) [ANR-12-BS10-0016]; Partner University Fund (PUF) Project; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357] FX The authors would like to thank the platform Nano'mat, the HAPPLE Project (ANR-12-BS10-0016) funded by Agence Nationale de la Recherche (ANR), as well as the Partner University Fund (PUF) Project. Use of the Center for Nanoscale Materials was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. This work has been carried out in the general context of the Labex ACTION. NR 48 TC 11 Z9 11 U1 6 U2 47 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 2330-4022 J9 ACS PHOTONICS JI ACS Photonics PD JAN PY 2015 VL 2 IS 1 BP 121 EP 129 DI 10.1021/ph500331c PG 9 WC Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Optics; Physics, Applied; Physics, Condensed Matter SC Science & Technology - Other Topics; Materials Science; Optics; Physics GA AZ6OS UT WOS:000348339400018 ER PT J AU Fan, YC Shen, NH Koschny, T Soukoulis, CM AF Fan, Yuancheng Shen, Nian-Hai Koschny, Thomas Soukoulis, Costas M. TI Tunable Terahertz Meta-Surface with Graphene Cut-Wires SO ACS PHOTONICS LA English DT Article DE graphene; terahertz; metamaterials; plasmonics; absorption enhancement; effective surface conductivity ID MONOLAYER GRAPHENE; METAMATERIALS; PLASMONICS; POLARIZATION; OPTICS; TRANSPARENCY; METASURFACES; ABSORPTION; CHALLENGES; REFRACTION AB We propose a tunable meta-surface in the terahertz regime by Patterning a graphene sheet in cut-wire array. The enhancement of terahertz absorption of such a graphene meta-surface was studied detailedly via the optimization to the geometry of the structure. Considering the data of graphene in both the experimental and theoretical perspectives, we investigated the performance of the absorbing graphene meta-surface by extracting its effective surface conductivities through a sheet retrieval method. We also specifically considered two sets of well-known experimental graphene data and comparatively studied the properties of graphene meta-surface by changing the graphene parameters in-between. It shows that there has been significant improvement in preparing high-quality graphene samples, which makes it possible to strengthen optical properties of graphene microstructures, and therefore benefits various practical applications. C1 [Fan, Yuancheng] Northwestern Polytech Univ, Minist Educ, Key Lab Space Appl Phys & Chem, Xian 710072, Peoples R China. [Fan, Yuancheng] Northwestern Polytech Univ, Dept Appl Phys, Sch Sci, Xian 710072, Peoples R China. [Shen, Nian-Hai; Koschny, Thomas; Soukoulis, Costas M.] Iowa State Univ, Ames Lab, Ames, IA 50011 USA. [Shen, Nian-Hai; Koschny, Thomas; Soukoulis, Costas M.] Iowa State Univ, Dept Phys & Astron, Ames, IA 50011 USA. [Soukoulis, Costas M.] FORTH, Inst Elect Struct & Laser, Iraklion 71110, Crete, Greece. RP Fan, YC (reprint author), Northwestern Polytech Univ, Minist Educ, Key Lab Space Appl Phys & Chem, Xian 710072, Peoples R China. EM phyfan@nwpu.edu.cn; nhshen@ameslab.gov RI Soukoulis, Costas/A-5295-2008; OI Fan, Yuancheng/0000-0002-7919-4148 FU U.S. Department of Energy (Basic Energy Sciences, Division of Materials Sciences and Engineering) [DE-AC02-07CH11358]; European Research Council under the ERC [320081]; China Scholarship Council [201206260055] FX Work at Ames Laboratory was partially supported by the U.S. Department of Energy (Basic Energy Sciences, Division of Materials Sciences and Engineering) under Contract No. DE-AC02-07CH11358. This work was partially supported by European Research Council under the ERC Advanced Grant No. 320081 (PHOTOMETA). Y.F. acknowledges the China Scholarship Council (No. 201206260055) for financial support. NR 56 TC 36 Z9 36 U1 17 U2 101 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 2330-4022 J9 ACS PHOTONICS JI ACS Photonics PD JAN PY 2015 VL 2 IS 1 BP 151 EP 156 DI 10.1021/ph500366z PG 6 WC Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Optics; Physics, Applied; Physics, Condensed Matter SC Science & Technology - Other Topics; Materials Science; Optics; Physics GA AZ6OS UT WOS:000348339400022 ER PT J AU Dworkowski, FSN Hough, MA Pompidor, G Fuchs, MR AF Dworkowski, Florian S. N. Hough, Michael A. Pompidor, Guillaume Fuchs, Martin R. TI Challenges and solutions for the analysis of in situ, in crystallo micro-spectrophotometric data SO ACTA CRYSTALLOGRAPHICA SECTION D-STRUCTURAL BIOLOGY LA English DT Article DE micro-spectrophotometer; UV-visible absorption; Raman spectroscopy; single-crystal spectroscopy; software toolbox; data analysis; background correction ID X-RAY CRYSTALLOGRAPHY; SWISS LIGHT-SOURCE; RESONANCE RAMAN-SPECTROSCOPY; MACROMOLECULAR CRYSTALLOGRAPHY; RADIATION-DAMAGE; ABSORPTION-SPECTROSCOPY; TRIPLE MONOCHROMATOR; BIOLOGICAL CRYSTALS; PROTEIN CRYSTALS; BEAMLINE X26-C AB Combining macromolecular crystallography with in crystallo micro-spectrophotometry yields valuable complementary information on the sample, including the redox states of metal cofactors, the identification of bound ligands and the onset and strength of undesired photochemistry, also known as radiation damage. However, the analysis and processing of the resulting data differs significantly from the approaches used for solution spectrophotometric data. The varying size and shape of the sample, together with the suboptimal sample environment, the lack of proper reference signals and the general influence of the X-ray beam on the sample have to be considered and carefully corrected for. In the present article, how to characterize and treat these sample-dependent artefacts in a reproducible manner is discussed and the SLS-APEin situ, in crystallo optical spectroscopy data-analysis toolbox is demonstrated. C1 [Dworkowski, Florian S. N.] Paul Scherrer Inst, Swiss Light Source, CH-5232 Villigen, Switzerland. [Hough, Michael A.] Univ Essex, Sch Biol Sci, Colchester CO4 3SQ, Essex, England. [Pompidor, Guillaume] DESY, European Mol Biol Lab Hamburg, D-22603 Hamburg, Germany. [Fuchs, Martin R.] Brookhaven Natl Lab, Upton, NY 11973 USA. RP Dworkowski, FSN (reprint author), Paul Scherrer Inst, Swiss Light Source, CH-5232 Villigen, Switzerland. EM florian.dworkowski@psi.ch RI Dworkowski, Florian/D-2807-2011; OI Dworkowski, Florian/0000-0001-5004-8684; Hough, Michael/0000-0001-7377-6713 FU Max Planck Society (MPG); Novartis; F. Hoffmann-La Roche; EU [2370]; [20111166] FX We would like to thank the X10SA beamline partners for funding: the Max Planck Society (MPG) and the pharmaceutical companies Novartis and F. Hoffmann-La Roche. We would also like to thank our scientific collaborators Hans-Petter Hersleth and Asmund K. Rohr at the University of Oslo, Dominique Bourgeois at Institut de Biologie Structurale Grenoble and Antonello Merlino and Alessandro Vergara at the University of Naples for continuous input, feedback and feature requests, which led to the development of the SLS-APE toolbox. We acknowledge the assistance of Andreea A. Manole at the University of Essex in the preparation of crystals of S. frigidimarina cytochrome c'. Part of this work was carried out under SLS long-term beamtime award 20111166 and was funded in part by EU FP7 BioStructX award 2370. NR 68 TC 4 Z9 4 U1 1 U2 6 PU INT UNION CRYSTALLOGRAPHY PI CHESTER PA 2 ABBEY SQ, CHESTER, CH1 2HU, ENGLAND SN 2059-7983 J9 ACTA CRYSTALLOGR D JI Acta Crystallogr. Sect. D-Struct. Biol. PD JAN PY 2015 VL 71 SI SI BP 27 EP 35 DI 10.1107/S1399004714015107 PN 1 PG 9 WC Biochemical Research Methods; Biochemistry & Molecular Biology; Biophysics; Crystallography SC Biochemistry & Molecular Biology; Biophysics; Crystallography GA AZ9WE UT WOS:000348563900004 PM 25615857 ER PT J AU Cuttitta, CM Ericson, DL Scalia, A Roessler, CG Teplitsky, E Joshi, K Campos, O Agarwal, R Allaire, M Orville, AM Sweet, RM Soares, AS AF Cuttitta, Christina M. Ericson, Daniel L. Scalia, Alexander Roessler, Christian G. Teplitsky, Ella Joshi, Karan Campos, Olven Agarwal, Rakhi Allaire, Marc Orville, Allen M. Sweet, Robert M. Soares, Alexei S. TI Acoustic transfer of protein crystals from agarose pedestals to micromeshes for high-throughput screening SO ACTA CRYSTALLOGRAPHICA SECTION D-STRUCTURAL BIOLOGY LA English DT Article DE macromolecular crystallography; acoustic droplet ejection; crystal mounting; drug discovery; chemical biology; high-throughput screening ID EGG-WHITE LYSOZYME; CRYSTALLIZATION; REFINEMENT; RESOLUTION; BINDING AB Acoustic droplet ejection (ADE) is an emerging technology with broad applications in serial crystallography such as growing, improving and manipulating protein crystals. One application of this technology is to gently transfer crystals onto MiTeGen micromeshes with minimal solvent. Once mounted on a micromesh, each crystal can be combined with different chemicals such as crystal-improving additives or a fragment library. Acoustic crystal mounting is fast (2.33transferss(-1)) and all transfers occur in a sealed environment that is in vapor equilibrium with the mother liquor. Here, a system is presented to retain crystals near the ejection point and away from the inaccessible dead volume at the bottom of the well by placing the crystals on a concave agarose pedestal (CAP) with the same chemical composition as the crystal mother liquor. The bowl-shaped CAP is impenetrable to crystals. Consequently, gravity will gently move the crystals into the optimal location for acoustic ejection. It is demonstrated that an agarose pedestal of this type is compatible with most commercially available crystallization conditions and that protein crystals are readily transferred from the agarose pedestal onto micromeshes with no loss in diffraction quality. It is also shown that crystals can be grown directly on CAPs, which avoids the need to transfer the crystals from the hanging drop to a CAP. This technology has been used to combine thermolysin and lysozyme crystals with an assortment of anomalously scattering heavy atoms. The results point towards a fast nanolitre method for crystal mounting and high-throughput screening. C1 [Cuttitta, Christina M.; Ericson, Daniel L.; Scalia, Alexander; Teplitsky, Ella; Joshi, Karan; Campos, Olven] Brookhaven Natl Lab, Off Educ Programs, Upton, NY 11973 USA. [Cuttitta, Christina M.] CUNY Coll Staten Isl, Ctr Dev Neurosci, Staten Isl, NY 10314 USA. [Cuttitta, Christina M.] CUNY Coll Staten Isl, Dept Biol, Staten Isl, NY 10314 USA. [Ericson, Daniel L.] SUNY Buffalo, Dept Biomed Engn, Buffalo, NY 14260 USA. [Scalia, Alexander] SUNY Binghamton, Dept Biol Sci, Binghamton, NY 11973 USA. [Roessler, Christian G.; Allaire, Marc; Orville, Allen M.; Sweet, Robert M.; Soares, Alexei S.] Brookhaven Natl Lab, Photon Sci Directorate, Upton, NY 11973 USA. [Teplitsky, Ella] SUNY Stony Brook, Dept Biochem & Cell Biol, Stony Brook, NY 11794 USA. [Joshi, Karan] PEC Univ Technol, Dept Elect & Elect Commun Engn, Chandigarh, India. [Campos, Olven] Florida Atlantic Univ, Dept Biol Sci, Boca Raton, FL 33414 USA. [Agarwal, Rakhi; Orville, Allen M.] Brookhaven Natl Lab, Dept Biosci, Upton, NY 11973 USA. RP Soares, AS (reprint author), Brookhaven Natl Lab, Photon Sci Directorate, Upton, NY 11973 USA. EM soares@bnl.gov FU US Department of Energy, Office of Science, Office of Workforce Development for Teachers and Scientists (WDTS); Brookhaven National Laboratory/US Department of Energy, Laboratory Directed Research and Development [11-008]; Office of Biological and Environmental Research; Office of Basic Energy Sciences of the US Department of Energy; National Center for Research Resources [P41RR012408]; National Institute of General Medical Sciences of the National Institutes of Health [P41GM103473]; Louis Stokes Alliances for Minority Participation fellowship FX Personnel for this study were recruited largely through the 2013 spring and summer session and 2014 spring session of the Science Undergraduate Laboratory Internships Program (SULI) and Graduate Research Internship Program (GRIP) supported through the US Department of Energy, Office of Science, Office of Workforce Development for Teachers and Scientists (WDTS). Major ongoing financial support for acoustic droplet ejection applications was through the Brookhaven National Laboratory/US Department of Energy, Laboratory Directed Research and Development Grant 11-008 and from the Offices of Biological and Environmental Research and of Basic Energy Sciences of the US Department of Energy, and from the National Center for Research Resources (P41RR012408) and the National Institute of General Medical Sciences (P41GM103473) of the National Institutes of Health. Additional support was provided by a Louis Stokes Alliances for Minority Participation fellowship. Data for this study were measured on beamlines X12C, X25 and X29 of the National Synchrotron Light Source. We thank Jan Kern and Rosalie Tran for kindly supplying photosystem II crystals and supporting our efforts to determine that these specimens are suitable for serial crystallography with acoustic methods. We thank Labcyte Inc., and particularly Joe Olechno, Richard Stearns and Richard Ellson, for their support and guidance. We thank the coeditor and the reviewers of the manuscript for taking the time to help us to address areas that were outside our expertise. Author contributions: ASS designed the experiment and wrote the paper. CMC, DLE, AS, CGR, ET, OC and ASS grew crystals, obtained data and analyzed data. ASS and KJ designed and built the labware. ASS, CGR and RMS trained and supervised student interns. RA and AMO provided the expressed protein. MA, CGR, AMO and ASS designed a related fragment-screening system that supports the current effort. NR 30 TC 5 Z9 5 U1 2 U2 12 PU INT UNION CRYSTALLOGRAPHY PI CHESTER PA 2 ABBEY SQ, CHESTER, CH1 2HU, ENGLAND SN 2059-7983 J9 ACTA CRYSTALLOGR D JI Acta Crystallogr. Sect. D-Struct. Biol. PD JAN PY 2015 VL 71 SI SI BP 94 EP 103 DI 10.1107/S1399004714013728 PN 1 PG 10 WC Biochemical Research Methods; Biochemistry & Molecular Biology; Biophysics; Crystallography SC Biochemistry & Molecular Biology; Biophysics; Crystallography GA AZ9WE UT WOS:000348563900011 PM 25615864 ER PT J AU Gao, YQ Roslyak, O Dervishi, E Karan, NS Ghosh, Y Sheehan, CJ Wang, F Gupta, G Mohite, A Dattelbaum, AM Doorn, SK Hollingsworth, JA Piryatinski, A Htoon, H AF Gao, Yongqian Roslyak, Oleksiy Dervishi, Enkeleda Karan, Niladri S. Ghosh, Yagnaseni Sheehan, Chris J. Wang, Feng Gupta, Gautam Mohite, Aditya Dattelbaum, Andrew M. Doorn, Stephen K. Hollingsworth, Jennifer A. Piryatinski, Andrei Htoon, Han TI Hybrid Graphene-Giant Nanocrystal Quantum Dot Assemblies with Highly Efficient Biexciton Emission SO Advanced Optical Materials LA English DT Article ID PLASMONICS; BLINKING; GROWTH; OXYGEN; GAIN C1 [Gao, Yongqian; Roslyak, Oleksiy; Dervishi, Enkeleda; Karan, Niladri S.; Ghosh, Yagnaseni; Sheehan, Chris J.; Wang, Feng; Doorn, Stephen K.; Hollingsworth, Jennifer A.; Htoon, Han] Los Alamos Natl Lab, Ctr Integrated Nanotechnol, Los Alamos, NM 87545 USA. [Gupta, Gautam; Mohite, Aditya; Dattelbaum, Andrew M.] Los Alamos Natl Lab, Mat Synth & Integrated Devices Mat Phys & Applica, Los Alamos, NM 87545 USA. [Roslyak, Oleksiy; Piryatinski, Andrei] Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. RP Htoon, H (reprint author), Los Alamos Natl Lab, Ctr Integrated Nanotechnol, Los Alamos, NM 87545 USA. EM htoon@lanl.gov RI Piryatinski, Andrei/B-5543-2009; OI Htoon, Han/0000-0003-3696-2896 FU CINT; OBES, OS, U.S. DOE [2009LANL1096] FX This work was conducted, in part, at the Center for Integrated Nanotechnologies (CINT), a U. S. Department of Energy, Office of Basic Energy Sciences (OBES) user facility. O. R. was supported by CINT. E. D., G. G., A. M., S. K. D., N. S. K., A. P., and Y. Gh. acknowledge Los Alamos National Laboratory Directed Research and Development (LDRD) Funds. Y. Ga., H. H. and J.A.H. acknowledge a Single-Investigator Small-Group Research Award (2009LANL1096), OBES, OS, U.S. DOE. NR 31 TC 10 Z9 10 U1 3 U2 35 PU WILEY-V C H VERLAG GMBH PI WEINHEIM PA BOSCHSTRASSE 12, D-69469 WEINHEIM, GERMANY SN 2195-1071 J9 ADV OPT MATER JI Adv. Opt. Mater. PD JAN PY 2015 VL 3 IS 1 BP 39 EP 43 DI 10.1002/adom.201400362 PG 5 WC Materials Science, Multidisciplinary; Optics SC Materials Science; Optics GA CA2KU UT WOS:000348738300004 ER PT S AU Reu, PL Quintana, E Long, K AF Reu, Phillip L. Quintana, Enrico Long, Kevin BE Jin, H Sciammarella, C Yoshida, S Lamberti, L TI Using Sampling Moire to Extract Displacement Information from X-Ray Images of Molten Salt Batteries SO ADVANCEMENT OF OPTICAL METHODS IN EXPERIMENTAL MECHANICS, VOL 3 SE Conference Proceedings of the Society for Experimental Mechanics Series LA English DT Proceedings Paper CT SEM Annual Conference and Exposition on Experimental and Applied Mechanics CY JUN 02-05, 2014 CL Greenville, SC SP Soc Expt Mech DE Moire; Full-field measurements; X-ray; Battery AB Full-field axial deformation within molten-salt batteries was measured using x-ray imaging with a sampling moire technique. This method worked for in situ testing of the batteries because of the inherent grid pattern of the battery layers when imaged with x-rays. High-speed x-ray imaging acquired movies of the layer deformation during battery activation. Numerical validation of the technique, as implemented in this paper, was done using synthetic and numerically shifted images. Typical results of a battery are shown for one test. Ongoing work on validation and more test results are in progress. C1 [Reu, Phillip L.; Quintana, Enrico; Long, Kevin] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Reu, PL (reprint author), Sandia Natl Labs, POB 5800, Albuquerque, NM 87185 USA. EM plreu@sandia.gov NR 4 TC 0 Z9 0 U1 0 U2 1 PU SPRINGER-VERLAG BERLIN PI BERLIN PA HEIDELBERGER PLATZ 3, D-14197 BERLIN, GERMANY SN 2191-5644 BN 978-3-319-06985-2 J9 C PROC SOC EXP MECH PY 2015 BP 331 EP 336 DI 10.1007/978-3-319-06986-9_38 PG 6 WC Optics; Physics, Applied SC Optics; Physics GA BB8XF UT WOS:000347773500038 ER PT J AU Li, YW Zhang, LJ Ma, YM Singh, DJ AF Li, Yuwei Zhang, Lijun Ma, Yanming Singh, David J. TI Tuning optical properties of transparent conducting barium stannate by dimensional reduction SO APL Materials LA English DT Article ID NEUTRON POWDER DIFFRACTION; BASNO3; OXIDES; SR2SNO4; BA2SNO4; SR AB We report calculations of the electronic structure and optical properties of doped n-type perovskite BaSnO3 and layered perovskites. While doped BaSnO3 retains its transparency for energies below the valence to conduction band onset, the doped layered compounds exhibit below band edge optical conductivity due to transitions from the lowest conduction band. This gives absorption in the visible for Ba2SnO4. Thus, it is important to minimize this phase in transparent conducting oxide (TCO) films. Ba3Sn2O7 and Ba4Sn3O10 have strong transitions only in the red and infrared, respectively. Thus, there may be opportunities for using these as wavelength filtering TCO. (C) 2015 Author(s). C1 [Li, Yuwei; Ma, Yanming] Jilin Univ, State Key Lab Superhard Mat, Changchun 130012, Peoples R China. [Li, Yuwei] Beijing Computat Sci Res Ctr, Beijing 100084, Peoples R China. [Zhang, Lijun] Jilin Univ, Coll Mat Sci & Engn, Changchun 130012, Peoples R China. [Singh, David J.] Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. RP Li, YW (reprint author), Jilin Univ, State Key Lab Superhard Mat, Changchun 130012, Peoples R China. RI Ma, Yanming/A-7297-2008; Ma, Yanming/A-4982-2009; Zhang, Lijun/F-7710-2011 OI Ma, Yanming/0000-0003-3711-0011; FU Natural Science Foundation of China [11025418]; Recruitment Program of Global Experts (Thousand Young Talents Plan); Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences, and Engineering Division FX Y.L. and Y.M. acknowledge funding support from the Natural Science Foundation of China (Grant No. 11025418). L.Z. acknowledges funding from the Recruitment Program of Global Experts (the Thousand Young Talents Plan). Work at ORNL was supported by the Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences, and Engineering Division. NR 49 TC 11 Z9 11 U1 3 U2 53 PU AMER INST PHYSICS PI MELVILLE PA 1305 WALT WHITMAN RD, STE 300, MELVILLE, NY 11747-4501 USA SN 2166-532X J9 APL MATER JI APL Mater. PD JAN PY 2015 VL 3 IS 1 AR 011102 DI 10.1063/1.4906785 PG 9 WC Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Science & Technology - Other Topics; Materials Science; Physics GA CA6CC UT WOS:000348995000002 ER PT J AU Wharton, S Simpson, M Osuna, JL Newman, JF Biraud, SC AF Wharton, Sonia Simpson, Matthew Osuna, Jessica L. Newman, Jennifer F. Biraud, Sebastien C. TI Role of Surface Energy Exchange for Simulating Wind Turbine Inflow: A Case Study in the Southern Great Plains, USA SO ATMOSPHERE LA English DT Article DE WRF; land surface model; Southern Great Plains; ARM; surface energy fluxes; lidar; wind energy; wind shear ID LAND-SURFACE; BOUNDARY-LAYER; SOIL-MOISTURE; ATMOSPHERIC STABILITY; WATER-VAPOR; PART I; METEOROLOGICAL MODEL; FLUX MEASUREMENTS; WRF MODEL; NOAH-MP AB The Weather Research and Forecasting (WRF) model is used to investigate choice of land surface model (LSM) on the near surface wind profile, including heights reached by multi-megawatt (MW) wind turbines. Simulations of wind profiles and surface energy fluxes were made using five LSMs of varying degrees of sophistication in dealing with soil-plant-atmosphere feedbacks for the Department of Energy (DOE) Southern Great Plains (SGP) Atmospheric Radiation Measurement Program (ARM) Central Facility in Oklahoma, USA. Surface flux and wind profile measurements were available for validation. WRF was run for three, two-week periods covering varying canopy and meteorological conditions. The LSMs predicted a wide range of energy flux and wind shear magnitudes even during the cool autumn period when we expected less variability. Simulations of energy fluxes varied in accuracy by model sophistication, whereby LSMs with very simple or no soil-plant-atmosphere feedbacks were the least accurate; however, the most complex models did not consistently produce more accurate results. Errors in wind shear were also sensitive to LSM choice and were partially related to energy flux accuracy. The variability of LSM performance was relatively high suggesting that LSM representation of energy fluxes in WRF remains a large source of model uncertainty for simulating wind turbine inflow conditions. C1 [Wharton, Sonia; Simpson, Matthew; Osuna, Jessica L.] Lawrence Livermore Natl Lab, Atmospher Earth & Energy Div, Livermore, CA 94550 USA. [Newman, Jennifer F.] Univ Oklahoma, Sch Meteorol, Norman, OK 73072 USA. [Biraud, Sebastien C.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, Berkeley, CA 94720 USA. RP Wharton, S (reprint author), Lawrence Livermore Natl Lab, Atmospher Earth & Energy Div, 7000 East Ave,L-103, Livermore, CA 94550 USA. EM wharton4@llnl.gov; simpson35@llnl.gov; osuna2@llnl.gov; jennifer.newman@ou.edu; scbiraud@lbl.gov RI Biraud, Sebastien/M-5267-2013 OI Biraud, Sebastien/0000-0001-7697-933X FU US Department of Energy, Wind and Water Power Technologies Office [WBS 02.07.00.01]; Office of Biological and Environmental Research of the US Department of Energy [DE-AC02-05CH11231]; DOE, National Nuclear Security Administration [DE-AC52-07NA27344. LLNL-JRNL-658967] FX This work was funded by the US Department of Energy, Wind and Water Power Technologies Office under agreement #WBS 02.07.00.01. The flux tower and surface meteorology observations were supported by the Office of Biological and Environmental Research of the US Department of Energy under contract No. DE-AC02-05CH11231 as part of the Atmospheric Radiation Measurement (ARM) and Atmospheric System Research programs. The authors would like to thank the staff at the SGP ARM Central Facility for their help with maintaining the Wind Cube lidar system and their support throughout our study. We'd also like to thank Marc Fischer and Margaret Torn (LBNL) for their support with the flux tower data and Rob Newsom (PNNL) for his support with the Halo lidar data. LLNL is operated by Lawrence Livermore National Security, LLC, for the DOE, National Nuclear Security Administration under contract DE-AC52-07NA27344. LLNL-JRNL-658967 NR 66 TC 0 Z9 0 U1 0 U2 5 PU MDPI AG PI BASEL PA ST ALBAN-ANLAGE 66, CH-4052 BASEL, SWITZERLAND SN 2073-4433 J9 ATMOSPHERE-BASEL JI Atmosphere PD JAN PY 2015 VL 6 IS 1 BP 21 EP 49 DI 10.3390/atmos6010021 PG 29 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA CA0HP UT WOS:000348598500002 ER PT J AU Roland, BP Amrich, CG Kammerer, CJ Stuchul, KA Larsen, SB Rode, S Aslam, AA Heroux, A Wetzel, R VanDemark, AP Palladino, MJ AF Roland, Bartholomew P. Amrich, Christopher G. Kammerer, Charles J. Stuchul, Kimberly A. Larsen, Samantha B. Rode, Sascha Aslam, Anoshe A. Heroux, Annie Wetzel, Ronald VanDemark, Andrew P. Palladino, Michael J. TI Triosephosphate isomerase I170V alters catalytic site, enhances stability and induces pathology in a Drosophila model of TPI deficiency SO BIOCHIMICA ET BIOPHYSICA ACTA-MOLECULAR BASIS OF DISEASE LA English DT Article DE Triosephosphate isomerase; Drosophila; Structure; Triosephosphate isomerase deficiency ID TRIOSE PHOSPHATE ISOMERASE; UNDERSTANDING PROTEIN LIDS; SECONDARY S96P MUTATION; ACTIVE HINGE MUTANTS; CRYSTAL-STRUCTURE; DIMER-INTERFACE; LOOP MOTION; STRUCTURAL BASIS; FLEXIBLE LOOP; TRYPANOSOMA-CRUZI AB Triosephosphate isomerase (TPI) is a glycolytic enzyme which homodimerizes for full catalytic activity. Mutations of the TPI gene elicit a disease known as TPI Deficiency, a glycolytic enzymopathy noted for its unique severity of neurological symptoms. Evidence suggests that TPI Deficiency pathogenesis may be due to conformational changes of the protein, likely affecting dimerization and protein stability. In this report, we genetically and physically characterize a human disease-associated TPI mutation caused by anI170V substitution. Human TPII170V elicits behavioral abnormalities in Drosophila. An examination of hTPI(I170V) enzyme kinetics revealed this substitution reduced catalytic turnover, while assessments of thermal stability demonstrated an increase in enzyme stability. The crystal structure of the homodimeric I170V mutant reveals changes in the geometry of critical residues within the catalytic pocket. Collectively these data reveal new observations of the structural and kinetic determinants of TPI Deficiency pathology, providing new insights into disease pathogenesis. (C) 2014 Elsevier B.V. All rights reserved. C1 [Roland, Bartholomew P.; Kammerer, Charles J.; Stuchul, Kimberly A.; Larsen, Samantha B.; Palladino, Michael J.] Univ Pittsburgh, Sch Med, Dept Pharmacol & Chem Biol, Pittsburgh, PA 15261 USA. [Roland, Bartholomew P.; Kammerer, Charles J.; Stuchul, Kimberly A.; Larsen, Samantha B.; Rode, Sascha; Wetzel, Ronald; Palladino, Michael J.] Univ Pittsburgh, Sch Med, Pittsburgh Inst Neurodegenerat Dis, Pittsburgh, PA 15261 USA. [Amrich, Christopher G.; Aslam, Anoshe A.; VanDemark, Andrew P.] Univ Pittsburgh, Dept Biol Sci, Pittsburgh, PA 15260 USA. [Rode, Sascha; Wetzel, Ronald; VanDemark, Andrew P.] Univ Pittsburgh, Sch Med, Dept Biol Struct, Pittsburgh, PA 15261 USA. [Heroux, Annie] Brookhaven Natl Lab, Dept Biol, Upton, NY 11973 USA. RP Palladino, MJ (reprint author), Univ Pittsburgh, Sch Med, Dept Pharmacol & Chem Biol, 3501 Fifth Ave, Pittsburgh, PA 15261 USA. EM mjp44@pitt.edu RI Wetzel, Ronald/G-7453-2011; OI Roland, Bartholomew/0000-0002-9033-9942 FU Achievement Rewards for College Scientists: Pittsburgh Chapter; National Institutes of Health [R01 GM103369, R01 GM097204, T32 GM8424-17] FX The authors would like to thank Atif Towheed, Kenneth Drombosky, and Aaron Talsma for their helpful discussions. This work was supported by a fellowship from Achievement Rewards for College Scientists: Pittsburgh Chapter [BPR] and the National Institutes of Health [grant numbers R01 GM103369 MJP, APV, R01 GM097204 APV, and T32 GM8424-17 BPR]. NR 70 TC 4 Z9 4 U1 4 U2 25 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0925-4439 EI 0006-3002 J9 BBA-MOL BASIS DIS JI Biochim. Biophys. Acta-Mol. Basis Dis. PD JAN PY 2015 VL 1852 IS 1 BP 61 EP 69 DI 10.1016/j.bbadis.2014.10.010 PG 9 WC Biochemistry & Molecular Biology; Biophysics; Cell Biology SC Biochemistry & Molecular Biology; Biophysics; Cell Biology GA AZ8ST UT WOS:000348485600007 PM 25463631 ER PT J AU Gianetti, TL Nocton, G Minasian, SG Kaltsoyannis, N Kilcoyne, ALD Kozimor, SA Shuh, DK Tyliszczak, T Bergman, RG Arnold, J AF Gianetti, Thomas L. Nocton, Gregory Minasian, Stefan G. Kaltsoyannis, Nikolas Kilcoyne, A. L. David Kozimor, Stosh A. Shuh, David K. Tyliszczak, Tolek Bergman, Robert G. Arnold, John TI Electron localization in a mixed-valence diniobium benzene complex SO CHEMICAL SCIENCE LA English DT Article ID CREUTZ-TAUBE ION; INVERTED-SANDWICH COMPLEXES; N BOND-CLEAVAGE; METAL-COMPLEXES; ARENE; STATE; SPECTROSCOPY; TRANSITION; ZIRCONIUM; CHEMISTRY AB Reaction of the neutral diniobium benzene complex {[Nb(BDI)(NBu)-Bu-t](2)(mu-C6H6)} (BDI = N, N'-diisopropylbenzene- beta-diketiminate) with Ag[B(C6F5) 4] results in a single electron oxidation to produce a cationic diniobium arene complex, {[Nb(BDI)(NBu)-Bu-t](2)(mu-C6H6)}{B(C6F5)(4)}. Investigation of the solid state and solution phase structure using single-crystal X-ray diffraction, cyclic voltammetry, magnetic susceptibility, and multinuclear NMR spectroscopy indicates that the oxidation results in an asymmetric molecule with two chemically inequivalent Nb atoms. Further characterization using density functional theory (DFT) calculations, UV-visible, Nb L-3,L-2-edge X-ray absorption near-edge structure (XANES), and EPR spectroscopies supports assignment of a diniobium complex, in which one Nb atom carries a single unpaired electron that is not largely delocalized on the second Nb atom. During the oxidative transformation, one electron is removed from the delta-bonding HOMO, which causes a destabilization of the molecule and formation of an asymmetric product. Subsequent reactivity studies indicate that the oxidized product allows access to metal-based chemistry with substrates that did not exhibit reactivity with the starting neutral complex. C1 [Gianetti, Thomas L.; Bergman, Robert G.; Arnold, John] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Nocton, Gregory] Ecole Polytech, CNRS, Lab Chim Mol, F-91128 Palaiseau, France. [Minasian, Stefan G.; Shuh, David K.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. [Minasian, Stefan G.; Kozimor, Stosh A.] Los Alamos Natl Lab, Div Chem, Los Alamos, NM 87545 USA. [Kaltsoyannis, Nikolas] UCL, Dept Chem, London WC1H 0AJ, England. [Kilcoyne, A. L. David; Tyliszczak, Tolek] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. RP Nocton, G (reprint author), Ecole Polytech, CNRS, Lab Chim Mol, F-91128 Palaiseau, France. EM greg.nocton@polytechnique.edu; n.kaltsoyannis@ucl.ac.uk; rgbergman@berkeley.edu; arnold@berkeley.edu RI Nocton, Greg/D-4435-2009; Kilcoyne, David/I-1465-2013; Arnold, John/F-3963-2012; OI Arnold, John/0000-0001-9671-227X; Kaltsoyannis, Nikolas/0000-0003-0293-5742 FU AFOSR [FA9550-11-1-0008]; Ecole Polytechnique; CNRS; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences [DE-AC02-05CH11231]; LANL under the Heavy Element Chemistry Program; Los Alamos National Security, LLC, for the National Nuclear Security Administration of U.S. Department of Energy [DE-AC52-06NA25396]; LANL; DOE Office of Science User Facility [DE-AC0205CH11231] FX Work at UC Berkeley is supported by the AFOSR (Grant Number FA9550-11-1-0008). G.N. thanks Ecole Polytechnique and CNRS for funding. Prof R. A. Andersen and Dr W. W. Lukens are thanked for help in measuring and understanding magnetic data and EPR data. This material is based on work supported at LBNL (S.G.M. and D.K.S.) by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences under contract no. DE-AC02-05CH11231, and at LANL under the Heavy Element Chemistry Program by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences. LANL is operated by Los Alamos National Security, LLC, for the National Nuclear Security Administration of U.S. Department of Energy under contract no. DE-AC52-06NA25396. The X-ray absorption work was also supported at LANL by a Glenn T. Seaborg Institute Postdoctoral Fellowship (S.G.M.) This research also used resources of the ALS (A.L.D.K. and T.T.), which is a DOE Office of Science User Facility supported under contract No. DE-AC0205CH11231 at LBNL. N.K. thanks University College London for computing resources via the Research Computing "Legion" cluster (Legion@UCL) and associated services. NR 64 TC 8 Z9 8 U1 1 U2 21 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2041-6520 EI 2041-6539 J9 CHEM SCI JI Chem. Sci. PY 2015 VL 6 IS 2 BP 993 EP 1003 DI 10.1039/c4sc02705a PG 11 WC Chemistry, Multidisciplinary SC Chemistry GA AZ3SN UT WOS:000348147100016 ER PT J AU Lauterbach, L Wang, HX Horch, M Gee, LB Yoda, Y Tanaka, Y Zebger, I Lenz, O Cramer, SP AF Lauterbach, Lars Wang, Hongxin Horch, Marius Gee, Leland B. Yoda, Yoshitaka Tanaka, Yoshihito Zebger, Ingo Lenz, Oliver Cramer, Stephen P. TI Nuclear resonance vibrational spectroscopy reveals the FeS cluster composition and active site vibrational properties of an O-2-tolerant NAD(+)-reducing [NiFe] hydrogenase SO CHEMICAL SCIENCE LA English DT Article ID NAD-LINKED HYDROGENASE; RESPIRATORY COMPLEX-I; RAMAN-SPECTROSCOPY; RALSTONIA-EUTROPHA; 4FE-4S CLUSTER; EPR; FERREDOXIN; DYNAMICS; FTIR; NRVS AB Hydrogenases are complex metalloenzymes that catalyze the reversible splitting of molecular hydrogen into protons and electrons essentially without overpotential. The NAD(+)-reducing soluble hydrogenase (SH) from Ralstonia eutropha is capable of H-2 conversion even in the presence of usually toxic dioxygen. The molecular details of the underlying reactions are largely unknown, mainly because of limited knowledge of the structure and function of the various metal cofactors present in the enzyme. Here, all iron-containing cofactors of the SH were investigated by Fe-57 specific nuclear resonance vibrational spectroscopy (NRVS). Our data provide experimental evidence for one [2Fe2S] center and four [4Fe4S] clusters, which is consistent with the amino acid sequence composition. Only the [2Fe2S] cluster and one of the four [4Fe4S] clusters were reduced upon incubation of the SH with NADH. This finding explains the discrepancy between the large number of FeS clusters and the small amount of FeS cluster-related signals as detected by electron paramagnetic resonance spectroscopic analysis of several NAD(+)-reducing hydrogenases. For the first time, Fe-CO and Fe-CN modes derived from the [NiFe] active site could be distinguished by NRVS through selective C-13 labeling of the CO ligand. This strategy also revealed the molecular coordinates that dominate the individual Fe-CO modes. The present approach explores the complex vibrational signature of the Fe-S clusters and the hydrogenase active site, thereby showing that NRVS represents a powerful tool for the elucidation of complex biocatalysts containing multiple cofactors. C1 [Lauterbach, Lars; Horch, Marius; Zebger, Ingo; Lenz, Oliver] Tech Univ Berlin, Inst Chem, D-10623 Berlin, Germany. [Lauterbach, Lars; Wang, Hongxin; Gee, Leland B.; Cramer, Stephen P.] Univ Calif Davis, Dept Chem, Davis, CA 95616 USA. [Wang, Hongxin; Tanaka, Yoshihito; Cramer, Stephen P.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA 94720 USA. [Yoda, Yoshitaka] JASRI, Mikazuki, Hyogo 6795198, Japan. [Tanaka, Yoshihito] RIKEN, Mikazuki, Hyogo 6795198, Japan. RP Lauterbach, L (reprint author), Tech Univ Berlin, Inst Chem, Str 17 Juni 135, D-10623 Berlin, Germany. EM lars.lauterbach@tu-berlin.de; spcramer@lbl.gov RI Gee, Leland/H-1742-2014; Lauterbach, Lars/L-6671-2014 OI Gee, Leland/0000-0002-5817-3997; Lauterbach, Lars/0000-0002-6601-6473 FU Deutsche Forschungsgemeinschaft (DFG, Cluster of Excellence UniCat); National Institutes of Health [GM-65440] FX The SH biochemistry and IR work (LL, MH, IZ and OL) were supported by the Deutsche Forschungsgemeinschaft (DFG, Cluster of Excellence UniCat). LL received a short-term EMBO scholarship for performing the work in this study. HW, LG and SPC were supported by National Institutes of Health (GM-65440 to SPC). The NRVS experiments were performed at BL09XU and BL19LXU of SPring8 approved under JASRI and RIKEN proposal numbers 2013B0103, 2014B1032 and 20133892). NR 21 TC 6 Z9 6 U1 0 U2 22 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2041-6520 EI 2041-6539 J9 CHEM SCI JI Chem. Sci. PY 2015 VL 6 IS 2 BP 1055 EP 1060 DI 10.1039/c4sc02982h PG 6 WC Chemistry, Multidisciplinary SC Chemistry GA AZ3SN UT WOS:000348147100024 PM 25678951 ER PT J AU Cheruku, P Huang, JH Yen, HJ Iyer, RS Rector, KD Martinez, JS Wang, HL AF Cheruku, Pradeep Huang, Jen-Huang Yen, Hung-Ju Iyer, Rashi S. Rector, Kirk D. Martinez, Jennifer S. Wang, Hsing-Lin TI Tyrosine-derived stimuli responsive, fluorescent amino acids SO CHEMICAL SCIENCE LA English DT Article ID OPTICAL-PROPERTIES; ENANTIOSELECTIVE SYNTHESIS; CHEMICAL BIOLOGY; PROBES; PROTEINS; PALLADIUM; RADICALS; DISEASE; BINDING; ALANINE AB A series of fluorescent unnatural amino acids (UAAs) bearing stilbene and meta-phenylenevinylene (m-PPV) backbone have been synthesized and their optical properties were studied. These novel UAAs were derived from protected diiodo-L-tyrosine using palladium-catalyzed Heck couplings with a series of styrene analogs. Unlike the other fluorescent UAAs, whose emissions are restricted to a narrow range of wavelengths, these new amino acids display the emission peaks at broad range wavelengths (from 400800 nm); including NIR with QY of 4% in HEPES buffer. The incorporation of both pyridine and phenol functional groups leads to distinct red, green, and blue (RGB) emission, in its basic, acidic and neutral states, respectively. More importantly, these amino acids showed reversible pH and redox response showing their promise as stimuli responsive fluorescent probes. To further demonstrate the utility of these UAAs in peptide synthesis, one of the amino acids was incorporated into a cell penetrating peptide (CPP) sequence through standard solid phase peptide synthesis. Resultant CPP was treated with two different cell lines and the internalization was monitored by confocal fluorescence microscopy. C1 [Cheruku, Pradeep; Yen, Hung-Ju; Rector, Kirk D.; Wang, Hsing-Lin] Los Alamos Natl Lab, Div Chem, C PCS, Los Alamos, NM 87545 USA. [Huang, Jen-Huang; Iyer, Rashi S.] Los Alamos Natl Lab, Def Syst & Anal Div, Los Alamos, NM 87545 USA. [Martinez, Jennifer S.] Los Alamos Natl Lab, Ctr Integrated Nanotechnol CINT, Los Alamos, NM 87545 USA. RP Wang, HL (reprint author), Los Alamos Natl Lab, Div Chem, C PCS, POB 1663, Los Alamos, NM 87545 USA. EM hwang@lanl.gov OI Yen, Hung-Ju/0000-0002-6316-9124 FU Laboratory Directed Research and Development (LDRD) program, under the auspices of Department of Energy (DOE) FX This research is supported by the Laboratory Directed Research and Development (LDRD) program, under the auspices of Department of Energy (DOE). Basic Energy Science (BES), Biomolecular Materials Program, Division of Materials Science and Engineering support the synthesis of UAA. NR 56 TC 4 Z9 4 U1 10 U2 43 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2041-6520 EI 2041-6539 J9 CHEM SCI JI Chem. Sci. PY 2015 VL 6 IS 2 BP 1150 EP 1158 DI 10.1039/c4sc02753a PG 9 WC Chemistry, Multidisciplinary SC Chemistry GA AZ3SN UT WOS:000348147100034 ER PT J AU Hart-Cooper, WM Zhao, C Triano, RM Yaghoubi, P Ozores, HL Burford, KN Toste, FD Bergman, RG Raymond, KN AF Hart-Cooper, William M. Zhao, Chen Triano, Rebecca M. Yaghoubi, Parastou Ozores, Haxel Lionel Burford, Kristen N. Toste, F. Dean Bergman, Robert G. Raymond, Kenneth N. TI The effect of host structure on the selectivity and mechanism of supramolecular catalysis of Prins cyclizations SO CHEMICAL SCIENCE LA English DT Article ID CARBONYL-ENE REACTION; CHIRAL LEWIS-ACIDS; MOLECULAR RECOGNITION; BASIC SOLUTION; ENZYME MIMICS; 3,4-DISUBSTITUTED PIPERIDINES; ENANTIOSELECTIVE CATALYSIS; ORTHOFORMATE HYDROLYSIS; COPPER(II) COMPLEXES; NAZAROV CYCLIZATION AB The effect of host structure on the selectivity and mechanism of intramolecular Prins reactions is evaluated using K12Ga4L6 tetrahedral catalysts. The host structure was varied by modifying the structure of the chelating moieties and the size of the aromatic spacers. While variation in chelator substituents was generally observed to affect changes in rate but not selectivity, changing the host spacer afforded differences in efficiency and product diastereoselectivity. An extremely high number of turnovers (up to 840) was observed. Maximum rate accelerations were measured to be on the order of 10(5), which numbers among the largest magnitudes of transition state stabilization measured with a synthetic host-catalyst. Host/guest size effects were observed to play an important role in host-mediated enantioselectivity. C1 [Hart-Cooper, William M.; Zhao, Chen; Triano, Rebecca M.; Yaghoubi, Parastou; Ozores, Haxel Lionel; Burford, Kristen N.; Toste, F. Dean; Bergman, Robert G.; Raymond, Kenneth N.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Dept Chem, Div Chem Sci, Berkeley, CA 94720 USA. RP Toste, FD (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Dept Chem, Div Chem Sci, Berkeley, CA 94720 USA. EM fdtoste@berkeley.edu; rbergman@berkeley.edu; knraymond@socrates.berkeley.edu FU Office of Science of the U.S. Department of Energy at LBNL [DE-AC02-05CH11231]; Division of Chemical Sciences, Geosciences, and Biosciences of the U.S. Department of Energy at LBNL [DE-AC02-05CH11231]; Spanish MEC; NSF [DGE 1106400]; Office of Basic Energy Sciences of the U.S. Department of Energy at LBNL [DE-AC02-05CH11231] FX This research was supported by the Director, Office of Science, Office of Basic Energy Sciences, and the Division of Chemical Sciences, Geosciences, and Biosciences of the U.S. Department of Energy at LBNL (DE-AC02-05CH11231). H.L.O. thanks the Spanish MEC for his FPU fellowship. R. M. T is supported by an NSF graduate research fellowship (DGE 1106400). NR 91 TC 15 Z9 15 U1 8 U2 52 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2041-6520 EI 2041-6539 J9 CHEM SCI JI Chem. Sci. PY 2015 VL 6 IS 2 BP 1383 EP 1393 DI 10.1039/c4sc02735c PG 11 WC Chemistry, Multidisciplinary SC Chemistry GA AZ3SN UT WOS:000348147100067 ER PT J AU Xu, ZJ AF Xu Zhi-Jie TI Phonon Excitation and Energy Redistribution in Phonon Space for Energy Dissipation and Transport in Lattice Structure with Nonlinear Dispersion SO COMMUNICATIONS IN THEORETICAL PHYSICS LA English DT Article DE dispersion; energy dissipation; energy distribution; phonon modes; heat transport; local thermo-dynamic equilibrium; nonequilibrium statistical mechanics ID STATISTICAL-MECHANICAL THEORY; HEAT-CONDUCTION; HETEROGENEOUS MATERIALS; IRREVERSIBLE PROCESSES; HOMOGENIZATION; CRYSTAL; CHAINS; FLOW AB We first propose fundamental solutions of wave propagation in dispersive chain subject to a localized initial perturbation in the displacement. Analytical solutions are obtained for both second order nonlinear dispersive chain and homogenous harmonic chain using stationary phase approximation. Solution is also compared with numerical results from molecular dynamics (MD) simulations. Locally dominant phonon modes (k-space) are introduced based on these solutions. These locally defined spatially and temporally varying phonon modes k(x,t) are critical to the concept of the local thermodynamic equilibrium (LTE). Wave propagation accompanying with the none quilibrium dynamics leads to the excitation of these locally defined phonon modes. It is found that the system energy is gradually redistributed among these excited phonons modes (k-space). This redistribution process is only possible with nonlinear dispersion and requires a finite amount of time to achieve a steady state distribution. This time scale is dependent on the spatial distribution (or frequency content) of the initial perturbation and the dispersion relation. Sharper and more concentrated perturbation leads to a faster energy redistribution and dissipation. This energy redistribution generates localized phonons with various frequencies that can be important for phonon-phonon interaction and energy dissipation in nonlinear systems. Depending on the initial perturbation and temperature, the time scale associated with this energy distribution can be critical for energy dissipation compared to the Umklapp scattering process. Ballistic type of heat transport along the harmonic chain reveals that at any given position, the lowest mode (k = 0) is excited first and gradually expanding to the highest mode (k(max)(x, t)), where kmax(x,t) can only asymptotically approach the maximum mode k(B) of the first Brillouin zone (k(max)(x,t) -> k(B)). No energy distributed into modes with k(max)(x,t) < k < k(B) demonstrates that the local thermodynamic equilibrium cannot be established in harmonic chain. Energy is shown to be uniformly distributed in all available phonon modes k <= k(max)(x, t) at any position with heat transfer along the harmonic chain. The energy flux along the chain is shown to be a constant with time and proportional to the sound speed (ballistic transport). Comparison with the Fourier's law leads to a time-dependent thermal conductivity that diverges with time. C1 Pacific NW Natl Lab, Fundamental & Computat Sci Directorate, Richland, WA 99352 USA. RP Xu, ZJ (reprint author), Pacific NW Natl Lab, Fundamental & Computat Sci Directorate, Richland, WA 99352 USA. EM zhijie.xu@pnnl.gov RI Xu, Zhijie/A-1627-2009 OI Xu, Zhijie/0000-0003-0459-4531 NR 21 TC 0 Z9 0 U1 0 U2 9 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 0253-6102 EI 1572-9494 J9 COMMUN THEOR PHYS JI Commun. Theor. Phys. PD JAN PY 2015 VL 63 IS 1 BP 101 EP 108 PG 8 WC Physics, Multidisciplinary SC Physics GA AZ7YO UT WOS:000348431700016 ER PT J AU McIntyre, NS Ulaganathan, J Simpson, T Qin, J Sherry, N Carcea, AG Newman, RC Kunz, M Tamura, N AF McIntyre, N. S. Ulaganathan, J. Simpson, T. Qin, J. Sherry, N. Carcea, A. G. Newman, R. C. Kunz, M. Tamura, N. TI Microscopic Cracking on Flat Alloy 600 Surfaces Following Accelerated Caustic Corrosion: Mapping of Strains and Microstructure During the Corrosion Process SO CORROSION LA English DT Article DE elastic strain; Laue microdiffraction; stress corrosion cracking; stresses from oxide growth ID X-RAY MICRODIFFRACTION; WHITE-BEAM; DIFFRACTION; SAMPLES; WATER; ORIENTATION; GRADIENTS AB Microscopic distributions of elastic and plastic strains have been studied at three intervals during an electrochemically accelerated corrosion test of a flat, polished surface of a mill-annealed and unstrained sample of Alloy 600 (UNS N06600) in 10% sodium hydroxide (NaOH) at 315 degrees C. Laue microdiffraction was used with a micron-sized polychromatic (white) x-ray beam to map strain changes in the sample as a function of corrosion time. After two 12 h corrosion periods, tensile elastic strains were detected along a grain boundary. After a third 24 h corrosion period, this particular boundary was found to have cracked to a depth of several microns; other adjacent boundaries exhibited tensile elastic strain, but no cracking. No significant changes to plastic strain distributions in the same area could be detected as a function of corrosion exposure. C1 [McIntyre, N. S.; Simpson, T.; Qin, J.; Sherry, N.] Univ Western Ontario, Fac Sci, London, ON N6A 5B7, Canada. [Ulaganathan, J.; Carcea, A. G.; Newman, R. C.; Kunz, M.] Univ Toronto, Dept Chem Engn & Appl Chem, Toronto, ON M5S 3E5, Canada. [Tamura, N.] Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley Hts, CA 94720 USA. RP McIntyre, NS (reprint author), Univ Western Ontario, Fac Sci, London, ON N6A 5B7, Canada. EM smcintyr@uwo.ca FU NSERC; Office of Basic Energy Sciences of the USDOE [DE-AC02-05CH11231]; NSERC-UNENE Senior Industrial Research Chair at the University of Toronto FX We are grateful for the financial assistance of NSERC. The Advanced Light Source is supported by the Director, Office of Basic Energy Sciences of the USDOE, under Contract no. DE-AC02-05CH11231. The contributions of J. Ulaganathan, A.G. Carcea, and R.C. Newman were supported by an NSERC-UNENE Senior Industrial Research Chair at the University of Toronto. We thank J. Chao for some experimental assistance, S. Ramamurthy of Surface Science Western (SSW) for providing the Auger depth profile, and G. Good of SSW for the SIMS imaging. NR 14 TC 1 Z9 1 U1 1 U2 13 PU NATL ASSOC CORROSION ENG PI HOUSTON PA 1440 SOUTH CREEK DRIVE, HOUSTON, TX 77084-4906 USA SN 0010-9312 EI 1938-159X J9 CORROSION JI Corrosion PD JAN PY 2015 VL 71 IS 1 BP 65 EP 70 DI 10.5006/1260 PG 6 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Materials Science; Metallurgy & Metallurgical Engineering GA AZ6DJ UT WOS:000348308500008 ER PT J AU Li, SS Chen, YS Mulfort, KL AF Li, Shenshen Chen, Yu-Sheng Mulfort, Karen L. TI Structural modification in bimetallic Ru(III)-Co(II) metal-organic frameworks SO CRYSTENGCOMM LA English DT Article ID ELECTRON-TRANSFER; ENERGY-TRANSFER; SURFACE-AREA; COMPLEXES; CLUSTERS; CRYSTAL; ACTIVATION; COBALT AB Two new mixed-metal MOFs were synthesized using the same Ru3O(OAc)(6)(+)-based struts and Co(II)-based nodes but variation in synthesis conditions has yielded markedly different topology. C1 [Li, Shenshen; Mulfort, Karen L.] Argonne Natl Lab, Div Chem Sci & Engn, Argonne, IL 60439 USA. [Chen, Yu-Sheng] Adv Photon Source, ChemMatCARS, Argonne, IL 60439 USA. RP Li, SS (reprint author), Argonne Natl Lab, Div Chem Sci & Engn, 9700 South Cass Ave, Argonne, IL 60439 USA. EM mulfort@anl.gov FU U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]; Division of Chemical Sciences and Engineering; National Science Foundation/Department of Energy [NSF/CHE-1346572] FX This material is based upon work supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under contract number DE-AC02-06CH11357. S.L. thanks the Division of Chemical Sciences and Engineering for postdoctoral support. ChemMatCARS Sector 15 is principally supported by the National Science Foundation/Department of Energy under grant number NSF/CHE-1346572. Use of the Advanced Photon Source is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under contract no. DE-AC02-06CH11357. NR 42 TC 0 Z9 0 U1 7 U2 38 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1466-8033 J9 CRYSTENGCOMM JI Crystengcomm PY 2015 VL 17 IS 5 BP 1005 EP 1009 DI 10.1039/c4ce02064b PG 5 WC Chemistry, Multidisciplinary; Crystallography SC Chemistry; Crystallography GA AZ4SZ UT WOS:000348214600005 ER PT J AU Li, T Geier, M Wang, L Ku, XK Gull, BM Lovas, T Shaddix, CR AF Li, Tian Geier, Manfred Wang, Liang Ku, Xiaoke Gull, Berta Matas Lovas, Terese Shaddix, Christopher R. TI Effect of Torrefaction on Physical Properties and Conversion Behavior of High Heating Rate Char of Forest Residue SO ENERGY & FUELS LA English DT Article ID TEMPERATURE ELEMENTAL LOSSES; FLUID-SOLID REACTIONS; 900-1000 DEGREES-C; RANDOM PORE MODEL; PULVERIZED-COAL; GASIFICATION REACTIVITY; LIGNOCELLULOSIC BIOMASS; PYROLYSIS CONDITIONS; STEAM GASIFICATION; ELEVATED PRESSURE AB In the work reported here, both forest residue (FR) and torrefied forest residue (TFR) were devolatilized in a drop tube reactor at 1473 K at a heating rate greater than 10(4) K/s. The physical properties of parent fuel particles and their corresponding char particles were examined by using a scanning electron microscope and a granulometer. After the same milling and sieving process, the TFR particles had a smaller size and smaller aspect ratio than the FR particles. The char particles consisted of two types of particles with different sizes and morphologies: a small particle mode (presumably char fragments) and a large particle mode. The volume fraction of char fragments in the TFR char was considerably less than for the FR char. Both types of char were converted in a drop tube reactor under oxidation and gasification conditions at 1473 and 1573 K, respectively. The total organic mass loss and release of individual organic elements during char conversion were determined using a tracer method. Calcium, manganese, barium, and magnesium were found to be suitable for use as tracers. The fractional carbon conversion rate of TFR char was found to be slower than that of FR char under both oxidation and gasification conditions. The fractional release rate of hydrogen was much higher than that of total organic mass loss, while the corresponding oxygen release was lower for both types of char and for different reactive environments. C1 [Li, Tian; Ku, Xiaoke; Lovas, Terese] Norwegian Univ Sci & Technol, Dept Energy & Proc Engn, N-7491 Trondheim, Norway. [Geier, Manfred; Shaddix, Christopher R.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94550 USA. [Wang, Liang; Gull, Berta Matas] SINTEF Energy Res, N-7465 Trondheim, Norway. RP Li, T (reprint author), Norwegian Univ Sci & Technol, Dept Energy & Proc Engn, Kolbjorn Hejes Vei 1b, N-7491 Trondheim, Norway. EM tian.li@ntnu.no OI Li, Tian/0000-0002-4248-8396; Wang, Liang/0000-0002-1458-7653 FU Research Council of Norway; Sandia's Laboratory Directed Research and Development (LDRD) program; DOE's National Nuclear Security Administration [DE-AC04-94AL85000] FX This work was carried out within the GasBio project, funded by the Research Council of Norway and industry partners. Support was also provided through the Sandia's Laboratory Directed Research and Development (LDRD) program. The authors would like to thank Ethan Hecht from Sandia for providing the schematic of the reactor and for his assistance with the experiments at Sandia. Sandia is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for DOE's National Nuclear Security Administration under Contract DE-AC04-94AL85000. NR 67 TC 11 Z9 11 U1 4 U2 31 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 0887-0624 EI 1520-5029 J9 ENERG FUEL JI Energy Fuels PD JAN PY 2015 VL 29 IS 1 BP 177 EP 184 DI 10.1021/ef5016044 PG 8 WC Energy & Fuels; Engineering, Chemical SC Energy & Fuels; Engineering GA AZ2YB UT WOS:000348094100022 ER PT J AU Ciesielski, PN Crowley, MF Nimlos, MR Sanders, AW Wiggins, GM Robichaud, D Donohoe, BS Foust, TD AF Ciesielski, Peter N. Crowley, Michael F. Nimlos, Mark R. Sanders, Aric W. Wiggins, Gavin M. Robichaud, Dave Donohoe, Bryon S. Foust, Thomas D. TI Biomass Particle Models with Realistic Morphology and Resolved Microstructure for Simulations of Intraparticle Transport Phenomena SO ENERGY & FUELS LA English DT Article ID DILUTE-ACID PRETREATMENT; BUBBLING FLUIDIZED-BEDS; FAST PYROLYSIS; HEAT-TRANSFER; LIGNOCELLULOSIC BIOMASS; WOOD PARTICLES; MASS-TRANSPORT; CORN STOVER; KINETICS; MOMENTUM AB Biomass exhibits a complex microstructure of directional pores that impact how heat and mass are transferred within biomass particles during conversion processes. However, models of biomass particles used in simulations of conversion processes typically employ oversimplified geometries such as spheres and cylinders and neglect intraparticle microstructure. Here we develop 3D models of biomass particles with size, morphology, and microstructure based on parameters obtained from quantitative image analysis. We obtain measurements of particle size and morphology by analyzing large ensembles of particles that result from typical size reduction methods, and we delineate several representative size classes. Microstructural parameters, including cell wall thickness and cell lumen dimensions, are measured directly from micrographs of sectioned biomass. A general constructive solid geometry algorithm is presented that produces models of biomass particles based on these measurements. Next, we employ the parameters obtained from image analysis to construct models of three different particle size classes from two different feedstocks representing a hardwood poplar species (Populus tremuloides, quaking aspen) and a softwood pine (Pinus taeda, loblolly pine). Finally, we demonstrate the utility of the models and the effects explicit microstructure by performing finite-element simulations of intraparticle heat and mass transfer, and the results are compared to similar simulations using traditional simplified geometries. We show how the behavior of particle models with more realistic morphology and explicit microstructure departs from that of spherical models in simulations of transport phenomena and that species-dependent differences in microstructure impact simulation results in some cases. C1 [Ciesielski, Peter N.; Crowley, Michael F.; Donohoe, Bryon S.] Natl Renewable Energy Lab, Biosci Ctr, Golden, CO 80401 USA. [Ciesielski, Peter N.; Nimlos, Mark R.; Robichaud, Dave; Foust, Thomas D.] Natl Renewable Energy Lab, Natl Bioenergy Ctr, Golden, CO 80401 USA. [Sanders, Aric W.] NIST, Quantum Elect & Photon Div, Boulder, CO 80305 USA. [Wiggins, Gavin M.] Oak Ridge Natl Lab, Knoxville, TN 37932 USA. RP Ciesielski, PN (reprint author), Natl Renewable Energy Lab, Biosci Ctr, 15013 Denver West Pkwy, Golden, CO 80401 USA. EM peter.ciesielski@nrel.gov FU Computational Pyrolysis Consortium - U.S. Department of Energy, BioEnergy Technologies Office (BETO); DOE Office of Energy Efficiency and Renewable Energy [DE-AC36-08G028308]; Center for Direct Catalytic Conversion of Biomass to Biofuels (C3Bio), an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0000997] FX The constructive solid geometry algorithm, model visualization methods, and finite-element simulation portions of this work were supported by the Computational Pyrolysis Consortium funded by the U.S. Department of Energy, BioEnergy Technologies Office (BETO). Computational resources were provided by the National Renewable Energy Sciences Center supported by the DOE Office of Energy Efficiency and Renewable Energy under Contract DE-AC36-08G028308. The imaging and image analysis part of this work was supported by the Center for Direct Catalytic Conversion of Biomass to Biofuels (C3Bio), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Award No. DE-SC0000997. NR 40 TC 9 Z9 9 U1 3 U2 23 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 0887-0624 EI 1520-5029 J9 ENERG FUEL JI Energy Fuels PD JAN PY 2015 VL 29 IS 1 BP 242 EP 254 DI 10.1021/ef502204v PG 13 WC Energy & Fuels; Engineering, Chemical SC Energy & Fuels; Engineering GA AZ2YB UT WOS:000348094100030 ER PT J AU Weber, RS Olarte, MV Wang, HM AF Weber, Robert S. Olarte, Mariefel V. Wang, Huamin TI Modeling the Kinetics of Deactivation of Catalysts during the Upgrading of Bio-oil SO ENERGY & FUELS LA English DT Article ID PYROLYSIS OIL; AQUEOUS-PHASE; HYDRODEOXYGENATION; POLYMERIZATION; CONDENSATION; LEVOGLUCOSAN; ZEOLITES AB The fouling of catalysts for the upgrading of bio-oils appears to be very different from the fouling of catalysts for the hydroprocessing of petroleum-derived streams. There are two reasons for the differences: (a) bio-oil contains polarizable components and phases that can stabilize reaction intermediates exhibiting charge separation and (b) bio-oil components contain functional groups that contain O, notably carbonyls (>C-O). Aldol condensation of carbonyls affords very different pathways for the production of oligomeric, refractory deposits than does dehydrogenation/polymerization of petroleum-derived hydrocarbons. Colloquially, we refer to the bio-oil-derived deposits as gunk to discriminate them from coke, the carbonaceous deposits encountered in petroleum refining. Classical gelation appears to be a suitable model for the gunking reaction. Our work has helped explain the temperature range at which bio-oil should be preprocessed (stabilized) to confer longer lifetimes on the catalysts used for more severe processing. Stochastic modeling (kinetic Monte Carlo simulations) appears promising to capture the rates of oligomerization of bio-oil. C1 [Weber, Robert S.; Olarte, Mariefel V.; Wang, Huamin] Pacific NW Natl Lab, Inst Integrated Catalysis, Richland, WA 99352 USA. RP Weber, RS (reprint author), Pacific NW Natl Lab, Inst Integrated Catalysis, POB 999,MS IN K2-12, Richland, WA 99352 USA. EM robert.weber@pnnl.gov RI Olarte, Mariefel/D-3217-2013 OI Olarte, Mariefel/0000-0003-2989-1110 FU U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Bioenergy Technologies Office FX This work was supported by the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Bioenergy Technologies Office. Pacific Northwest National Laboratory (PNNL) is a multiprogram national laboratory operated for DOE by Battelle. NR 26 TC 7 Z9 7 U1 5 U2 40 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 0887-0624 EI 1520-5029 J9 ENERG FUEL JI Energy Fuels PD JAN PY 2015 VL 29 IS 1 BP 273 EP 277 DI 10.1021/ef502483t PG 5 WC Energy & Fuels; Engineering, Chemical SC Energy & Fuels; Engineering GA AZ2YB UT WOS:000348094100033 ER PT J AU Babrauskas, V Singla, V Lucas, D Rich, D AF Babrauskas, Vytenis Singla, Veena Lucas, Donald Rich, David TI Questions About the Conclusions in Blais and Carpenter 2013 SO FIRE TECHNOLOGY LA English DT Letter ID FLAME RETARDANTS; DIBENZOFURANS C1 [Babrauskas, Vytenis] Fire Sci & Technol Inc, Issaquah, WA 98027 USA. [Singla, Veena; Lucas, Donald] Green Sci Policy Inst, Berkeley, CA 94705 USA. [Lucas, Donald] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Rich, David] Univ Calif Berkeley, Berkeley, CA 94720 USA. [Rich, David] Reax Engn Inc, Berkeley, CA 94704 USA. RP Babrauskas, V (reprint author), Fire Sci & Technol Inc, 9000-300th Pl SE, Issaquah, WA 98027 USA. EM vytob@doctorfire.com NR 18 TC 1 Z9 1 U1 1 U2 1 PU SPRINGER PI DORDRECHT PA VAN GODEWIJCKSTRAAT 30, 3311 GZ DORDRECHT, NETHERLANDS SN 0015-2684 EI 1572-8099 J9 FIRE TECHNOL JI Fire Technol. PD JAN PY 2015 VL 51 IS 1 BP 213 EP 217 DI 10.1007/s10694-014-0394-5 PG 5 WC Engineering, Multidisciplinary; Materials Science, Multidisciplinary SC Engineering; Materials Science GA AZ4IY UT WOS:000348185900014 ER PT J AU Kim, Y Salvi, A Stefanopoulou, AG Ersal, T AF Kim, Youngki Salvi, Ashwin Stefanopoulou, Anna G. Ersal, Tulga TI Reducing Soot Emissions in a Diesel Series Hybrid Electric Vehicle Using a Power Rate Constraint Map SO IEEE TRANSACTIONS ON VEHICULAR TECHNOLOGY LA English DT Article DE Diesel engines; discrete optimization; model predictive control (MPC); power management; series hybrid electric vehicles (SHEVs); soot emissions ID IN-THE-LOOP; CONTROL STRATEGY; CONTROL DESIGN; FUEL-ECONOMY; ENGINE; OPTIMIZATION; MANAGEMENT; SIMULATION; ALGORITHM AB This paper considers a diesel series hybrid electric vehicle (SHEV) and proposes the utilization of an engine-generator power rate constraint map to reduce soot emissions without a significant compromise in fuel economy. Specifically, model predictive control (MPC) is used to split the vehicle power demand between the engine-generator unit and the battery. To achieve a reduction in soot, the engine-generator power rate is constrained. Unlike existing strategies, the power rate limit is not a fixed value but varies, depending on the power level, resulting in a map. This constraint map is designed by formulating the soot emission reduction problem as an optimization problem, which is solved through a three-step offline discrete optimization process. The optimization relies on a quasi-static soot emissions map that captures the trends, even during transients, but underestimates the magnitudes. Therefore, to evaluate the performance of the MPC-based power management with the power rate constraint map, experiments are conducted through an engine-in-the-loop simulation framework. Experimental results show that compared with a constant power rate constraint, soot emissions can be reduced by 44.5% while compromising fuel economy by only 0.3% through the proposed approach. As a tradeoff, the ampere-hour (Ah) processed in the battery, which is a variable that has been shown to correlate with battery capacity loss, increases by 5.5%. C1 [Kim, Youngki; Stefanopoulou, Anna G.; Ersal, Tulga] Univ Michigan, Dept Mech Engn, Ann Arbor, MI 48109 USA. [Salvi, Ashwin] US DOE, Adv Res Projects Agcy Energy, Washington, DC 20585 USA. RP Kim, Y (reprint author), Univ Michigan, Dept Mech Engn, Ann Arbor, MI 48109 USA. EM youngki@umich.edu; asalvi@umich.edu; annastef@umich.edu; tersal@umich.edu FU Automotive Research Center of the U.S. Army Tank Automotive Research, Development, and Engineering Center (TARDEC), Warren, MI, USA [W56HZV-04-2-0001] FX This work was supported by the Automotive Research Center in accordance with Cooperative Agreement W56HZV-04-2-0001 of the U.S. Army Tank Automotive Research, Development, and Engineering Center (TARDEC), Warren, MI, USA. The review of this paper was coordinated by Prof. T. M. Guerra. NR 34 TC 8 Z9 8 U1 1 U2 13 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 0018-9545 EI 1939-9359 J9 IEEE T VEH TECHNOL JI IEEE Trans. Veh. Technol. PD JAN PY 2015 VL 64 IS 1 BP 2 EP 12 DI 10.1109/TVT.2014.2321346 PG 11 WC Engineering, Electrical & Electronic; Telecommunications; Transportation Science & Technology SC Engineering; Telecommunications; Transportation GA AZ2HC UT WOS:000348054000002 ER PT J AU Hao, Y Song, JC Yang, F Hao, YY Sun, QJ Guo, JJ Cui, YX Wang, H Zhu, FR AF Hao, Yang Song, Jingcheng Yang, Fan Hao, Yuying Sun, Qinjun Guo, Junjie Cui, Yanxia Wang, Hua Zhu, Furong TI Improved performance of organic solar cells by incorporating silica-coated silver nanoparticles in the buffer layer SO JOURNAL OF MATERIALS CHEMISTRY C LA English DT Article ID HETEROJUNCTION PHOTOVOLTAIC DEVICES; AU NANOPARTICLES; EFFICIENCY ENHANCEMENT; AG NANOPARTICLES; FLUORESCENCE; ARRAYS AB It is demonstrated that the use of silica-coated silver nanoparticles (AgNPs) in the buffer layer improves the performance of organic solar cells (OSCs). It is found that only large sized AgNPs are advantageous for increasing the electric field distribution in the active layer, and therefore, increasing light absorption, caused by the localized surface plasmonic resonance and far-field scattering. Furthermore, the scattering of silica-coated AgNPs is more important to the light harvesting because of the existence of the silica coating. It is also demonstrated that the silica coating is favorable for enhancing the exciton dissociation because of the reduction of the exciton quenching that occurred at the interface between the bare AgNPs and the active layer. Furthermore, silica-coated AgNPs also promote hole transport and extraction, which is presumably explained by the introduction of "dopant" levels within the band gap of the poly(3,4-ethylenedioxythiophene)-poly(styrenesulfonate) and reduction of hole trapping of a bare silver surface. The combination of all these benefits results in a 25.4% improvement in photocurrent density and an increase of 19.2% in power conversion efficiency. This work indicates that using silica-coated AgNPs as light trapping elements is more efficient than using bare AgNPs in plasmonic organic solar cells. The systematic exploration of the optical and electrical effects of silica-coated AgNPs contributes to a more comprehensive understanding of the mechanism of performance improvement of the plasmonic OSCs. C1 [Hao, Yang; Song, Jingcheng; Yang, Fan; Hao, Yuying; Sun, Qinjun; Cui, Yanxia] Taiyuan Univ Technol, Coll Phys & Optoelect, Key Lab Adv Transducers & Intelligent Control Sys, Minist Educ & Shanxi Prov, Taiyuan 030024, Peoples R China. [Guo, Junjie] Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN 37831 USA. [Wang, Hua] Taiyuan Univ Technol, Key Lab Interface Sci & Engn Adv Mat, Taiyuan 030024, Peoples R China. [Zhu, Furong] Hong Kong Baptist Univ, Dept Phys, Kowloon Tong, Hong Kong, Peoples R China. [Zhu, Furong] Hong Kong Baptist Univ, Inst Adv Mat, Kowloon Tong, Hong Kong, Peoples R China. RP Hao, Y (reprint author), Taiyuan Univ Technol, Coll Phys & Optoelect, Key Lab Adv Transducers & Intelligent Control Sys, Minist Educ & Shanxi Prov, Taiyuan 030024, Peoples R China. EM haoyuyinghyy@sina.com; frzhu@hkbu.edu.hk RI guo, junjie/I-3189-2012; Wang, Hua/C-6687-2017; OI guo, junjie/0000-0002-3414-3734; Wang, Hua/0000-0002-2976-9521; Zhu, Furong/0000-0002-6691-1937 FU National Natural Science Foundation of China [61274056, 11204205, 61205179, 21101111, 21071108, 11204202, 91233208]; Key Laboratory of Advanced Display and System Applications; Ministry of Education; Shanghai University; International Science and Technology Cooperation Program of China [2012DFR50460]; Shanxi Natural Science Foundation [2010021023-2, 2011021022-2, 2012011020-4]; New Teachers' Fund [20121402120017]; Hong Kong Scholar Program [XJ2013002]; Talents for Early Career Scheme - Tertiary Education Division, Shanxi Province FX This research work was financially supported by National Natural Science Foundation of China (61274056, 11204205, 61205179, 21101111, 21071108, 11204202, 91233208), Key Laboratory of Advanced Display and System Applications, Ministry of Education, Shanghai University, International Science and Technology Cooperation Program of China (2012DFR50460), Shanxi Natural Science Foundation (2010021023-2, 2011021022-2, 2012011020-4), New Teachers' Fund (20121402120017), Hong Kong Scholar Program (XJ2013002), and Talents for Early Career Scheme - Tertiary Education Division, Shanxi Province. NR 34 TC 10 Z9 11 U1 5 U2 42 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7526 EI 2050-7534 J9 J MATER CHEM C JI J. Mater. Chem. C PY 2015 VL 3 IS 5 BP 1082 EP 1090 DI 10.1039/c4tc01990c PG 9 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA AZ6AM UT WOS:000348300300023 ER PT J AU Anderson, BE Shaw, MD Harker, BM AF Anderson, Brian E. Shaw, Matthew D. Harker, Blaine M. TI Extraction of plate bending stiffness from coincidence angles of sound transmission measurements SO JOURNAL OF THE ACOUSTICAL SOCIETY OF AMERICA LA English DT Article AB The bending stiffness in a homogeneous, isotropic, thin plate is experimentally derived from measurements of coincidence angles extracted from supercritical sound transmission versus frequency measurements. A computer controlled turn table rotates a plate sample and a receiver array, placed in the near field of the plate. The array is used to track the transmitted sound through the plate, generated by a far-field stationary source, using beam forming. The array technique enables measurement of plates measuring only one wavelength in width. Two examples are used for proof of concept, including an aluminum plate in air and an alumina plate under water. (C) 2015 Acoustical Society of America. C1 [Anderson, Brian E.] Los Alamos Natl Lab, Geophys Grp EES 17, Los Alamos, NM 87545 USA. [Shaw, Matthew D.] Penn State Univ, Grad Program Acoust, University Pk, PA 16802 USA. [Harker, Blaine M.] Brigham Young Univ, Acoust Res Grp, Dept Phys & Astron, Provo, UT 84602 USA. RP Anderson, BE (reprint author), Los Alamos Natl Lab, Geophys Grp EES 17, POB 1663, Los Alamos, NM 87545 USA. EM bea@lanl.gov FU Los Alamos National Laboratory; Office of Naval Research [33] FX This research was made possible by funding from the Los Alamos National Laboratory with the use of facilities located on the campus of Brigham Young University, and by funding from the Office of Naval Research Code 33 with the use of facilities located on the campus of the Pennsylvania State University. NR 10 TC 0 Z9 0 U1 1 U2 2 PU ACOUSTICAL SOC AMER AMER INST PHYSICS PI MELVILLE PA STE 1 NO 1, 2 HUNTINGTON QUADRANGLE, MELVILLE, NY 11747-4502 USA SN 0001-4966 EI 1520-8524 J9 J ACOUST SOC AM JI J. Acoust. Soc. Am. PD JAN PY 2015 VL 137 IS 1 BP 498 EP 500 DI 10.1121/1.4904522 PG 3 WC Acoustics; Audiology & Speech-Language Pathology SC Acoustics; Audiology & Speech-Language Pathology GA AZ6ZX UT WOS:000348369000066 PM 25618078 ER PT J AU Speer, JG De Moor, E Clarke, AJ AF Speer, J. G. De Moor, E. Clarke, A. J. TI Critical Assessment 7: Quenching and partitioning SO MATERIALS SCIENCE AND TECHNOLOGY LA English DT Article DE Steel microstructure; Quenching and partitioning; Retained austenite ID Q-AND-P; HIGH-STRENGTH STEEL; MEDIUM-CARBON STEEL; MARTENSITIC STAINLESS-STEEL; INDUCED PLASTICITY STEEL; ATOM-PROBE TOMOGRAPHY; TEMPERING PROCESS; MECHANICAL-PROPERTIES; RETAINED AUSTENITE; HEAT-TREATMENT AB Quenching and partitioning is a relatively new heat treatment concept to generate microstructures containing retained austenite stabilised by carbon partitioning from martensite. Research on quench and partitioning has been conducted by numerous groups, and this critical assessment provides some of the authors' perspectives on progress and understanding in the field, with particular focus on the physical metallurgy and transformation mechanisms, process variations, mechanical behaviour, and industrial implementation. While much progress has been made, the field provides rich opportunity for further understanding and development. C1 [Speer, J. G.; De Moor, E.] Colorado Sch Mines, Adv Steel Proc & Prod Res Ctr, Golden, CO 80401 USA. [Clarke, A. J.] Los Alamos Natl Lab, Mat Sci & Technol Div, Los Alamos, NM 87545 USA. RP Speer, JG (reprint author), Colorado Sch Mines, Adv Steel Proc & Prod Res Ctr, 1500 Illinois St, Golden, CO 80401 USA. EM jspeer@mines.edu RI de moor, emmanuel/E-9373-2012 OI de moor, emmanuel/0000-0001-6538-1121 FU Advanced Steel Processing and Products Research Center; Los Alamos National Security, LLC, operator of the Los Alamos National Laboratory [DE-AC52-06NA25396]; US Department of Energy; US DOE Innovative Manufacturing Initiative [DE-EE0005765] FX JGS and EDM gratefully acknowledge the support of the sponsors of the Advanced Steel Processing and Products Research Center. AJC gratefully acknowledges support from Los Alamos National Security, LLC, operator of the Los Alamos National Laboratory under contract number DE-AC52-06NA25396 with the US Department of Energy. The authors acknowledge support of the US DOE Innovative Manufacturing Initiative through DE-EE0005765. NR 120 TC 14 Z9 14 U1 7 U2 32 PU TAYLOR & FRANCIS LTD PI ABINGDON PA 4 PARK SQUARE, MILTON PARK, ABINGDON OX14 4RN, OXON, ENGLAND SN 0267-0836 EI 1743-2847 J9 MATER SCI TECH-LOND JI Mater. Sci. Technol. PD JAN PY 2015 VL 31 IS 1 BP 3 EP 9 DI 10.1179/1743284714Y.0000000628 PG 7 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Materials Science; Metallurgy & Metallurgical Engineering GA AZ6FI UT WOS:000348314000002 ER PT J AU Baeumer, C Saldana-Greco, D Martirez, JMP Rappe, AM Shim, M Martin, LW AF Baeumer, Christoph Saldana-Greco, Diomedes Martirez, John Mark P. Rappe, Andrew M. Shim, Moonsub Martin, Lane W. TI Ferroelectrically driven spatial carrier density modulation in graphene SO Nature Communications LA English DT Article ID SINGLE-LAYER GRAPHENE; ELECTRON; PSEUDOPOTENTIALS; PHOTORESPONSE; TRANSISTOR; SCATTERING; POINTS AB The next technological leap forward will be enabled by new materials and inventive means of manipulating them. Among the array of candidate materials, graphene has garnered much attention; however, due to the absence of a semiconducting gap, the realization of graphene-based devices often requires complex processing and design. Spatially controlled local potentials, for example, achieved through lithographically defined split-gate configurations, present a possible route to take advantage of this exciting two-dimensional material. Here we demonstrate carrier density modulation in graphene through coupling to an adjacent ferroelectric polarization to create spatially defined potential steps at 180 degrees-domain walls rather than fabrication of local gate electrodes. Periodic arrays of p-i junctions are demonstrated in air (gate tunable to p-n junctions) and density functional theory reveals that the origin of the potential steps is a complex interplay between polarization, chemistry, and defect structures in the graphene/ferroelectric couple. C1 [Baeumer, Christoph; Shim, Moonsub; Martin, Lane W.] Univ Illinois, Dept Mat Sci & Engn, Urbana, IL 61801 USA. [Baeumer, Christoph; Shim, Moonsub; Martin, Lane W.] Univ Illinois, Mat Res Lab, Urbana, IL 61801 USA. [Saldana-Greco, Diomedes; Martirez, John Mark P.; Rappe, Andrew M.] Univ Penn, Makineni Theoret Labs, Dept Chem, Philadelphia, PA 19104 USA. [Martin, Lane W.] Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA. [Martin, Lane W.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. RP Martin, LW (reprint author), Univ Illinois, Dept Mat Sci & Engn, Urbana, IL 61801 USA. EM lwmartin@berkeley.edu RI Martin, Lane/H-2409-2011; Shim, Moonsub/A-7875-2009; OI Martin, Lane/0000-0003-1889-2513; Shim, Moonsub/0000-0001-7781-1029; Baeumer, Christoph/0000-0003-0008-514X FU Army Research Office [W911NF-14-1-0104]; National Science Foundation; Nanoelectronics Research Initiative [DMR-1124696]; Office of Naval Research [N00014-14-1-0761]; Department of Energy Office of Basic Energy Sciences [DE-FG02-07ER15920]; National Energy Research Scientific Computing Center; Office of Science of the US Department of Energy [DE-AC02- 05CH11231] FX C.B. acknowledges support from the Army Research Office under grant W911NF-14-1-0104. D.S.-G., M.S. and L.W.M. acknowledge support from the National Science Foundation and the Nanoelectronics Research Initiative under grant DMR-1124696. J.M.P.M. acknowledges support from the Office of Naval Research under granN00014-14-1-0761. A.M.R. acknowledges support from the Department of Energy Office of Basic Energy Sciences under grant number DE-FG02-07ER15920. Experiments were partially carried out in the Materials Research Laboratory Central Facilities, University of Illinois. D.S.-G., J.M.P.M. and A.M.R. acknowledge computational support from the National Energy Research Scientific Computing Center, which is supported by the Office of Science of the US Department of Energy under Contract No. DE-AC02-05CH11231. NR 50 TC 26 Z9 26 U1 12 U2 81 PU NATURE PUBLISHING GROUP PI LONDON PA MACMILLAN BUILDING, 4 CRINAN ST, LONDON N1 9XW, ENGLAND SN 2041-1723 J9 NAT COMMUN JI Nat. Commun. PD JAN PY 2015 VL 6 AR 6136 DI 10.1038/ncomms7136 PG 8 WC Multidisciplinary Sciences SC Science & Technology - Other Topics GA CA3UM UT WOS:000348832300007 PM 25609217 ER PT J AU Bai, P Jeon, MY Ren, LM Knight, C Deem, MW Tsapatsis, M Siepmann, JI AF Bai, Peng Jeon, Mi Young Ren, Limin Knight, Chris Deem, Michael W. Tsapatsis, Michael Siepmann, J. Ilja TI Discovery of optimal zeolites for challenging separations and chemical transformations using predictive materials modeling SO Nature Communications LA English DT Article ID METAL-ORGANIC FRAMEWORKS; UNITED-ATOM DESCRIPTION; PHASE-EQUILIBRIA; TRANSFERABLE POTENTIALS; SELECTIVE HYDROISOMERIZATION; PROCESS OPTIMIZATION; NANOPOROUS MATERIALS; METHANE STORAGE; N-ALKANES; ADSORPTION AB Zeolites play numerous important roles in modern petroleum refineries and have the potential to advance the production of fuels and chemical feedstocks from renewable resources. The performance of a zeolite as separation medium and catalyst depends on its framework structure. To date, 213 framework types have been synthesized and >330,000 thermodynamically accessible zeolite structures have been predicted. Hence, identification of optimal zeolites for a given application from the large pool of candidate structures is attractive for accelerating the pace of materials discovery. Here we identify, through a large-scale, multi-step computational screening process, promising zeolite structures for two energy-related applications: the purification of ethanol from fermentation broths and the hydroisomerization of alkanes with 18-30 carbon atoms encountered in petroleum refining. These results demonstrate that predictive modelling and data-driven science can now be applied to solve some of the most challenging separation problems involving highly non-ideal mixtures and highly articulated compounds. C1 [Bai, Peng; Jeon, Mi Young; Ren, Limin; Tsapatsis, Michael; Siepmann, J. Ilja] Univ Minnesota, Dept Chem, Ctr Theory, Minneapolis, MN 55455 USA. [Bai, Peng; Jeon, Mi Young; Ren, Limin; Tsapatsis, Michael; Siepmann, J. Ilja] Univ Minnesota, Dept Chem Engn, Ctr Theory, Minneapolis, MN 55455 USA. [Bai, Peng; Jeon, Mi Young; Ren, Limin; Tsapatsis, Michael; Siepmann, J. Ilja] Univ Minnesota, Dept Mat Sci, Ctr Theory, Minneapolis, MN 55455 USA. [Bai, Peng; Jeon, Mi Young; Ren, Limin; Tsapatsis, Michael; Siepmann, J. Ilja] Univ Minnesota, Dept Chem, Ctr Theory, Minneapolis, MN 55455 USA. [Knight, Chris] Argonne Natl Lab, Leadership Comp Facil, Argonne, IL 60439 USA. [Deem, Michael W.] Rice Univ, Dept Bioengn, Houston, TX 77005 USA. [Deem, Michael W.] Rice Univ, Dept Phys & Astron, Houston, TX 77005 USA. RP Siepmann, JI (reprint author), Univ Minnesota, Dept Chem, Ctr Theory, 207 Pleasant St SE, Minneapolis, MN 55455 USA. EM siepmann@umn.edu RI Deem, Michael/P-3595-2014; Bai, Peng/L-8516-2013 OI Deem, Michael/0000-0002-4298-3450; Bai, Peng/0000-0002-6881-4663 FU Department of Energy Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences [DE-FG02-12ER16362]; Office of Science of the Department of Energy [DE-AC02-06CH11357] FX Financial support from the Department of Energy Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences under Award DE-FG02-12ER16362 is gratefully acknowledged. This research used resources of the Argonne Leadership Computing Facility (ALCF) at Argonne National Laboratory, which is supported by the Office of Science of the Department of Energy under contract DE-AC02-06CH11357. Additional computer resources were provided by the Minnesota Super-computing Institute. NR 46 TC 20 Z9 20 U1 11 U2 100 PU NATURE PUBLISHING GROUP PI LONDON PA MACMILLAN BUILDING, 4 CRINAN ST, LONDON N1 9XW, ENGLAND SN 2041-1723 J9 NAT COMMUN JI Nat. Commun. PD JAN PY 2015 VL 6 AR 5912 DI 10.1038/ncomms6912 PG 9 WC Multidisciplinary Sciences SC Science & Technology - Other Topics GA CA2MI UT WOS:000348742100001 PM 25607776 ER PT J AU Balachandran, PV Rondinelli, JM AF Balachandran, Prasanna V. Rondinelli, James M. TI Massive band gap variation in layered oxides through cation ordering SO NATURE COMMUNICATIONS LA English DT Article ID INTERNAL ELECTRIC-FIELD; OPTICAL-PROPERTIES; QUASI-PARTICLE; INTERFACES; ENERGIES; FILMS; PSEUDOPOTENTIALS; ANISOTROPY; SRLAALO4; DENSITY AB The electronic band gap is a fundamental material parameter requiring control for light harvesting, conversion and transport technologies, including photovoltaics, lasers and sensors. Although traditional methods to tune band gaps rely on chemical alloying, quantum size effects, lattice mismatch or superlattice formation, the spectral variation is often limited to < 1 eV, unless marked changes to composition or structure occur. Here we report large band gap changes of up to 200% or similar to 2 eV without modifying chemical composition or use of epitaxial strain in the LaSrAlO4 Ruddlesden-Popper oxide. First-principles calculations show that ordering electrically charged [LaO](1+) and neutral [SrO](0) monoxide planes imposes internal electric fields in the layered oxides. These fields drive local atomic displacements and bond distortions that control the energy levels at the valence and conduction band edges, providing a path towards electronic structure engineering in complex oxides. C1 [Balachandran, Prasanna V.] Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. [Rondinelli, James M.] Northwestern Univ, Dept Mat Sci & Engn, Evanston, IL 60208 USA. RP Rondinelli, JM (reprint author), Northwestern Univ, Dept Mat Sci & Engn, Evanston, IL 60208 USA. EM jrondinelli@northwestern.edu RI Rondinelli, James/A-2071-2009 OI Rondinelli, James/0000-0003-0508-2175 FU DARPA [N66001-12-1-4224]; U.S. DOE, Office of Basic Energy Sciences (BES) [DE-AC02-06CH11357] FX P.V.B. and J.M.R. acknowledge support from DARPA (grant no. N66001-12-1-4224). P.V.B. acknowledges discussions with Dr A. Saxena, J. Young and N. Charles. We thank Professor S. Halasyamani, Professor B. Nelson-Cheeseman, Dr A. Bhattacharya and Dr J. Iniguez for insightful conversations, and gratefully thank Professor L.D. Marks for performing the Wien2k calculations. P.V.B. and J.M.R. acknowledge the help of Dr J. Deslippe and Dr D. Strubbe with the BerkeleyGW code. The computational work made use of the GARNET and SPIRIT clusters at the ERDC and AFRL HPC resources, respectively, under the HPCMP initiative, and facilities available at the Center for Nanoscale Materials (CARBON Cluster) at Argonne National Laboratory, supported by the U.S. DOE, Office of Basic Energy Sciences (BES), DE-AC02-06CH11357. The views, opinions and/or findings reported here are solely those of the authors and do not represent any official views of DARPA. NR 55 TC 9 Z9 9 U1 5 U2 57 PU NATURE PUBLISHING GROUP PI LONDON PA MACMILLAN BUILDING, 4 CRINAN ST, LONDON N1 9XW, ENGLAND SN 2041-1723 J9 NAT COMMUN JI Nat. Commun. PD JAN PY 2015 VL 6 AR 6191 DI 10.1038/ncomms7191 PG 7 WC Multidisciplinary Sciences SC Science & Technology - Other Topics GA CA3WL UT WOS:000348835200001 PM 25635516 ER PT J AU Jiang, YV Freyer, JL Cotanda, P Brucks, SD Killops, KL Bandar, JS Torsitano, C Balsara, NP Lambert, TH Campos, LM AF Jiang, Yivan Freyer, Jessica L. Cotanda, Pepa Brucks, Spencer D. Killops, Kato L. Bandar, Jeffrey S. Torsitano, Christopher Balsara, Nitash P. Lambert, Tristan H. Campos, Luis M. TI The evolution of cyclopropenium ions into functional polyelectrolytes SO Nature Communications LA English DT Article ID LIQUID BLOCK-COPOLYMERS; RADICAL POLYMERIZATION; POLY(IONIC LIQUID)S; PROTON TRANSPORT; FACILE ROUTE; MEMBRANES; POLYMERS; CONDUCTIVITY; CATION; ANION AB Versatile polyelectrolytes with tunable physical properties have the potential to be transformative in applications such as energy storage, fuel cells and various electronic devices. Among the types of materials available for these applications, nanostructured cationic block copolyelectrolytes offer mechanical integrity and well-defined conducting paths for ionic transport. To date, most cationic polyelectrolytes bear charge formally localized on heteroatoms and lack broad modularity to tune their physical properties. To overcome these challenges, we describe herein the development of a new class of functional polyelectrolytes based on the aromatic cyclopropenium ion. We demonstrate the facile synthesis of a series of polymers and nanoparticles based on monomeric cyclopropenium building blocks incorporating various functional groups that affect physical properties. The materials exhibit high ionic conductivity and thermal stability due to the nature of the cationic moieties, thus rendering this class of new materials as an attractive alternative to develop ion-conducting membranes. C1 [Jiang, Yivan; Freyer, Jessica L.; Brucks, Spencer D.; Bandar, Jeffrey S.; Torsitano, Christopher; Lambert, Tristan H.; Campos, Luis M.] Columbia Univ, Dept Chem, New York, NY 10027 USA. [Cotanda, Pepa] Joint Ctr Artificial Photosynth, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Cotanda, Pepa; Balsara, Nitash P.] Univ Calif Berkeley, Dept Chem & Biomol Engn, Berkeley, CA 94720 USA. [Killops, Kato L.] Edgewood Chem Biol Ctr, Aberdeen, MD 21010 USA. Div Mat Sci, Environm Energy Technol Div, Berkeley, CA 94720 USA. [Balsara, Nitash P.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Environm Energy Technol Div, Berkeley, CA 94720 USA. [Balsara, Nitash P.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Joint Ctr Energy Storage, Berkeley, CA 94720 USA. RP Campos, LM (reprint author), Columbia Univ, Dept Chem, New York, NY 10027 USA. EM lcampos@columbia.edu FU National Science Foundation (CAREER) [DMR-1351293, CHE-0953259]; ACS Petroleum Research Fund [54471DNI7] FX This work was supported in part by the National Science Foundation (CAREER, DMR-1351293 to L.M.C. and CHE-0953259 to T.H.L.), ACS Petroleum Research Fund (54471DNI7 to L.M.C.), and 3M Corporation (to L. M. C.). Y.J. thanks the Columbia Amgen Scholars Program and the Columbia Science Research Fellows. J.S.B is grateful for NDSEG and NSF fellowships. K.L.K. thanks the Army Basic Research Program and ECBC for financial support. Transmission electron micrographs were collected at NYSBC, and were made possible by a grant from NYSTAR. The investigation was conducted in a facility constructed with support from Research Facilities Improvement Program Grant number C06 RR017528-01-CEM from the National Center for Research Resources, National Institutes of Health. This material is in part based upon work performed by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the U.S. Department of Energy under Award Number DE-SC0004993. SAXS experiments were performed at Lawrence Berkeley National Laboratory's Advance Light Source, Beamline 7.3.3. Beamline 7.3.3 of the Advanced Light Source is supported by the Director of the Office of Science, Office of Basic Energy Sciences, of the U. S. Department of Energy under Contract No. DE-AC0205CH11231. We thank Dr Jos Paulusse for performing size exclusion chromatography on the homopolymers. We also thank Qi Jiang for performing thermogravimetric analysis on the homopolymers. NR 54 TC 11 Z9 11 U1 4 U2 56 PU NATURE PUBLISHING GROUP PI LONDON PA MACMILLAN BUILDING, 4 CRINAN ST, LONDON N1 9XW, ENGLAND SN 2041-1723 J9 NAT COMMUN JI Nat. Commun. PD JAN PY 2015 VL 6 AR 5950 DI 10.1038/ncomms6950 PG 7 WC Multidisciplinary Sciences SC Science & Technology - Other Topics GA CA3MK UT WOS:000348810700006 PM 25575214 ER PT J AU Li, LZ Schroeder, T Chen, EH Walsh, M Bayn, I Goldstein, J Gaathon, O Trusheim, ME Lu, M Mower, J Cotlet, M Markham, ML Twitchen, DJ Englund, D AF Li, Luozhou Schroeder, Tim Chen, Edward H. Walsh, Michael Bayn, Igal Goldstein, Jordan Gaathon, Ophir Trusheim, Matthew E. Lu, Ming Mower, Jacob Cotlet, Mircea Markham, Matthew L. Twitchen, Daniel J. Englund, Dirk TI Coherent spin control of a nanocavity-enhanced qubit in diamond SO Nature Communications LA English DT Article ID PHOTONIC CRYSTAL CAVITY; NITROGEN-VACANCY CENTERS; COLOR-CENTER; ENTANGLEMENT; ATOM AB A central aim of quantum information processing is the efficient entanglement of multiple stationary quantum memories via photons. Among solid-state systems, the nitrogen-vacancy centre in diamond has emerged as an excellent optically addressable memory with second-scale electron spin coherence times. Recently, quantum entanglement and teleportation have been shown between two nitrogen-vacancy memories, but scaling to larger networks requires more efficient spin-photon interfaces such as optical resonators. Here we report such nitrogen-vacancy-nanocavity systems in the strong Purcell regime with optical quality factors approaching 10,000 and electron spin coherence times exceeding 200 mu s using a silicon hard-mask fabrication process. This spin-photon interface is integrated with on-chip microwave striplines for coherent spin control, providing an efficient quantum memory for quantum networks. C1 [Li, Luozhou; Schroeder, Tim; Chen, Edward H.; Walsh, Michael; Bayn, Igal; Goldstein, Jordan; Gaathon, Ophir; Trusheim, Matthew E.; Mower, Jacob; Englund, Dirk] MIT, Dept Elect Engn & Comp Sci, Cambridge, MA 02139 USA. [Lu, Ming; Cotlet, Mircea] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. [Markham, Matthew L.; Twitchen, Daniel J.] Element Six, Santa Clara, CA 95054 USA. RP Englund, D (reprint author), MIT, Dept Elect Engn & Comp Sci, 77 Massachusetts Ave, Cambridge, MA 02139 USA. EM englund@mit.edu RI Schroder, Tim/M-8624-2014 OI Schroder, Tim/0000-0001-9017-0254 FU Air Force Office of Scientific Research (AFOSR) [FA9550-11-1-0014]; US Department of Energy, Office of Basic Energy Sciences [DE-AC02-98CH10886]; Alexander von Humboldt Foundation; NASA Office of the Chief Technologist's Space Technology Research Fellowship; AFOSR Quantum Memories MURI; NSF IGERT program Interdisciplinary Quantum Information Science and Engineering (iQuISE) FX Fabrication and experiments were supported in part by the Air Force Office of Scientific Research (AFOSR Grant No. FA9550-11-1-0014, supervised by Gernot Pomrenke). Research carried out in part at the Center for Functional Nanomaterials, Brookhaven National Laboratory, which is supported by the US Department of Energy, Office of Basic Energy Sciences, under Contract No. DE-AC02-98CH10886. T.S. was supported by the Alexander von Humboldt Foundation. E.H.C. was supported by the NASA Office of the Chief Technologist's Space Technology Research Fellowship. M.E.T. was supported in part by the AFOSR Quantum Memories MURI. M.E.T. and J.M. were supported by the NSF IGERT program Interdisciplinary Quantum Information Science and Engineering (iQuISE). We would like to thank Fernando Camino, Daniel Kleppner, Hannah Clevenson, Catherine Lee, Sara Mouradian, Ren-Jye Shiue, Aaron Stein, Greg Steinbrecher and Cheng-Chia Tsai for their advice and assistance. We would also like to thank Hassaram Bakhru for nitrogen ion implantation. NR 44 TC 31 Z9 32 U1 3 U2 28 PU NATURE PUBLISHING GROUP PI LONDON PA MACMILLAN BUILDING, 4 CRINAN ST, LONDON N1 9XW, ENGLAND SN 2041-1723 J9 NAT COMMUN JI Nat. Commun. PD JAN PY 2015 VL 6 AR 6173 DI 10.1038/ncomms7173 PG 7 WC Multidisciplinary Sciences SC Science & Technology - Other Topics GA CA3UT UT WOS:000348833000001 PM 25629223 ER PT J AU Liu, Q Li, ZF Liu, YD Zhang, HY Ren, Y Sun, CJ Lu, WQ Zhou, Y Stanciu, L Stach, EA Xie, J AF Liu, Qi Li, Zhe-Fei Liu, Yadong Zhang, Hangyu Ren, Yang Sun, Cheng-Jun Lu, Wenquan Zhou, Yun Stanciu, Lia Stach, Eric A. Xie, Jian TI Graphene-modified nanostructured vanadium pentoxide hybrids with extraordinary electrochemical performance for Li-ion batteries SO Nature Communications LA English DT Article ID RAY-ABSORPTION SPECTROSCOPY; RECHARGEABLE LITHIUM BATTERIES; CATHODE MATERIALS; V2O5 XEROGEL; HOLLOW MICROSPHERES; LIFEPO4 CELLS; OXIDE; NANOCOMPOSITES; INTERCALATION; CAPACITY AB The long-standing issues of low intrinsic electronic conductivity, slow lithium-ion diffusion and irreversible phase transitions on deep discharge prevent the high specific capacity/energy (443 mAhg(-1) and 1,550 Wh kg(-1)) vanadium pentoxide from being used as the cathode material in practical battery applications. Here we develop a method to incorporate graphene sheets into vanadium pentoxide nanoribbons via the sol-gel process. The resulting graphene-modified nanostructured vanadium pentoxide hybrids contain only 2 wt. % graphene, yet exhibits extraordinary electrochemical performance: a specific capacity of 438 mAhg(-1), approaching the theoretical value (443 mAhg(-1)), a long cyclability and significantly enhanced rate capability. Such performance is the result of the combined effects of the graphene on structural stability, electronic conduction, vanadium redox reaction and lithium-ion diffusion supported by various experimental studies. This method provides a new avenue to create nanostructured metal oxide/graphene materials for advanced battery applications. C1 [Liu, Qi; Li, Zhe-Fei; Liu, Yadong; Xie, Jian] Indiana Univ Purdue Univ, Purdue Sch Engn & Technol, Dept Mech Engn, Indianapolis, IN 46202 USA. [Zhang, Hangyu; Zhou, Yun; Stanciu, Lia] Purdue Univ, Sch Mat Engn, W Lafayette, IN 47907 USA. [Ren, Yang; Sun, Cheng-Jun] Argonne Natl Lab, Adv Photon Source, Xray Sci Div, Lemont, IL 60439 USA. [Lu, Wenquan] Argonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USA. [Stanciu, Lia] Purdue Univ, Weldon Sch Biomed Engn, W Lafayette, IN 47907 USA. [Stach, Eric A.] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. RP Xie, J (reprint author), Indiana Univ Purdue Univ, Purdue Sch Engn & Technol, Dept Mech Engn, Indianapolis, IN 46202 USA. EM jianxie@iupui.edu RI Stach, Eric/D-8545-2011; Li, Zhefei/M-1106-2015 OI Stach, Eric/0000-0002-3366-2153; FU U.S. Department of Energy, Office of Science, Office of Basic Energy Science [DE-AC02-06CH11357]; U.S. DOE [DE-AC02-98CH10886] FX We like to express our appreciation for Dr Corinne Renguette's help with editing and Dr Qingliu Wu's help with partially drawing Fig. 4. Use of the Advanced Photon Source was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Science, under Contract No. DE-AC02-06CH11357. This research was also carried out in part at the Center for Functional Nanomaterials at Brookhaven National Laboratory (U.S. DOE contract DE-AC02-98CH10886). A patent has been filed for this novel synthesis method and the corresponding V2O5-G hybrid materials. NR 60 TC 48 Z9 48 U1 33 U2 234 PU NATURE PUBLISHING GROUP PI LONDON PA MACMILLAN BUILDING, 4 CRINAN ST, LONDON N1 9XW, ENGLAND SN 2041-1723 J9 NAT COMMUN JI Nat. Commun. PD JAN PY 2015 VL 6 AR 6127 DI 10.1038/ncomms7127 PG 10 WC Multidisciplinary Sciences SC Science & Technology - Other Topics GA CA3UK UT WOS:000348832100001 PM 25600907 ER PT J AU Perry, SL Leon, L Hoffmann, KQ Kade, MJ Priftis, D Black, KA Wong, D Klein, RA Pierce, CF Margossian, KO Whitmer, JK Qin, J de Pablo, JJ Tirrell, M AF Perry, Sarah L. Leon, Lorraine Hoffmann, Kyle Q. Kade, Matthew J. Priftis, Dimitrios Black, Katie A. Wong, Derek Klein, Ryan A. Pierce, Charles F., III Margossian, Khatcher O. Whitmer, Jonathan K. Qin, Jian de Pablo, Juan J. Tirrell, Matthew TI Chirality-selected phase behaviour in ionic polypeptide complexes SO NATURE COMMUNICATIONS LA English DT Article ID CHARGED BLOCK-COPOLYMERS; FORCE-FIELD; COACERVATION; MICELLES; SIMULATIONS; DYNAMICS; POLYELECTROLYTES; TRANSITIONS; RECOGNITION; STABILITY AB Polyelectrolyte complexes present new opportunities for self-assembled soft matter. Factors determining whether the phase of the complex is solid or liquid remain unclear. Ionic polypeptides enable examination of the effects of stereochemistry on complex formation. Here we demonstrate that chirality determines the state of polyelectrolyte complexes, formed from mixing dilute solutions of oppositely charged polypeptides, via a combination of electrostatic and hydrogen-bonding interactions. Fluid complexes occur when at least one of the polypeptides in the mixture is racemic, which disrupts backbone hydrogen-bonding networks. Pairs of purely chiral polypeptides, of any sense, form compact, fibrillar solids with a beta-sheet structure. Analogous behaviour occurs in micelles formed from polypeptide block copolymers with polyethylene oxide, where assembly into aggregates with either solid or fluid cores, and eventually into ordered phases at high concentrations, is possible. Chirality is an exploitable tool for manipulating material properties in polyelectrolyte complexation. C1 [Perry, Sarah L.; Leon, Lorraine; Hoffmann, Kyle Q.; Kade, Matthew J.; Priftis, Dimitrios; Wong, Derek; Klein, Ryan A.; Pierce, Charles F., III; Margossian, Khatcher O.; Whitmer, Jonathan K.; Qin, Jian; de Pablo, Juan J.; Tirrell, Matthew] Univ Chicago, Inst Mol Engn, Chicago, IL 60637 USA. [Leon, Lorraine; Kade, Matthew J.; Whitmer, Jonathan K.; de Pablo, Juan J.; Tirrell, Matthew] Argonne Natl Lab, Argonne, IL 60439 USA. [Hoffmann, Kyle Q.] Univ Wisconsin, Dept Chem Engn, Madison, WI 53706 USA. [Black, Katie A.] Univ Calif Berkeley, Dept Bioengn, Berkeley, CA 94720 USA. RP Tirrell, M (reprint author), Univ Chicago, Inst Mol Engn, Chicago, IL 60637 USA. EM mtirrell@uchicago.edu OI Perry, Sarah/0000-0003-2301-6710 FU U.S. Department of Energy Office of Science, Program in Basic Energy Sciences, Materials Sciences and Engineering Division FX We thank Dr Carlos Baiz and Dr Denise Schach from the Tokmakoff lab for their assistance and guidance in collecting and analysing the FTIR data. This work also benefited from extensive discussions with Professor Tobin Sosnick. This work was supported by the U.S. Department of Energy Office of Science, Program in Basic Energy Sciences, Materials Sciences and Engineering Division. NR 56 TC 28 Z9 28 U1 11 U2 90 PU NATURE PUBLISHING GROUP PI LONDON PA MACMILLAN BUILDING, 4 CRINAN ST, LONDON N1 9XW, ENGLAND SN 2041-1723 J9 NAT COMMUN JI Nat. Commun. PD JAN PY 2015 VL 6 AR 6052 DI 10.1038/ncomms7052 PG 8 WC Multidisciplinary Sciences SC Science & Technology - Other Topics GA CA3TS UT WOS:000348830100006 PM 25586861 ER PT J AU Ponath, P Fredrickson, K Posadas, AB Ren, Y Wu, XY Vasudevan, RK Okatan, MB Jesse, S Aoki, T McCartney, MR Smith, DJ Kalinin, SV Lai, K Demkov, AA AF Ponath, Patrick Fredrickson, Kurt Posadas, Agham B. Ren, Yuan Wu, Xiaoyu Vasudevan, Rama K. Okatan, M. Baris Jesse, S. Aoki, Toshihiro McCartney, Martha R. Smith, David J. Kalinin, Sergei V. Lai, Keji Demkov, Alexander A. TI Carrier density modulation in a germanium heterostructure by ferroelectric switching SO NATURE COMMUNICATIONS LA English DT Article ID INITIO MOLECULAR-DYNAMICS; TOTAL-ENERGY CALCULATIONS; FIELD-EFFECT TRANSISTORS; AUGMENTED-WAVE METHOD; THIN-FILMS; EPITAXIAL-GROWTH; BEAM EPITAXY; BATIO3 FILMS; BASIS-SET; MICROSCOPY AB The development of non-volatile logic through direct coupling of spontaneous ferroelectric polarization with semiconductor charge carriers is nontrivial, with many issues, including epitaxial ferroelectric growth, demonstration of ferroelectric switching and measurable semiconductor modulation. Here we report a true ferroelectric field effect-carrier density modulation in an underlying Ge(001) substrate by switching of the ferroelectric polarization in epitaxial c-axis-oriented BaTiO3 grown by molecular beam epitaxy. Using the density functional theory, we demonstrate that switching of BaTiO3 polarization results in a large electric potential change in Ge. Aberration-corrected electron microscopy confirms BaTiO3 tetragonality and the absence of any low-permittivity interlayer at the interface with Ge. The non-volatile, switchable nature of the single-domain out-of-plane ferroelectric polarization of BaTiO3 is confirmed using piezoelectric force microscopy. The effect of the polarization switching on the conductivity of the underlying Ge is measured using microwave impedance microscopy, clearly demonstrating a ferroelectric field effect. C1 [Ponath, Patrick; Fredrickson, Kurt; Posadas, Agham B.; Ren, Yuan; Wu, Xiaoyu; Lai, Keji; Demkov, Alexander A.] Univ Texas Austin, Dept Phys, Austin, TX 78712 USA. [Vasudevan, Rama K.; Okatan, M. Baris; Jesse, S.; Kalinin, Sergei V.] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. [Aoki, Toshihiro] Arizona State Univ, Ctr Solid State Sci, Tempe, AZ 85287 USA. [McCartney, Martha R.; Smith, David J.] Arizona State Univ, Dept Phys, Tempe, AZ 85287 USA. RP Demkov, AA (reprint author), Univ Texas Austin, Dept Phys, Austin, TX 78712 USA. EM demkov@physics.utexas.edu RI Aoki, Toshihiro/I-4852-2015; Vasudevan, Rama/Q-2530-2015; Kalinin, Sergei/I-9096-2012; Jesse, Stephen/D-3975-2016; Okatan, M. Baris/E-1913-2016 OI Vasudevan, Rama/0000-0003-4692-8579; Kalinin, Sergei/0000-0001-5354-6152; Jesse, Stephen/0000-0002-1168-8483; Okatan, M. Baris/0000-0002-9421-7846 FU Air Force Office of Scientific Research [FA9550-12-10494]; Office of Naval Research [N000 14-10-1-0489]; NSF [DMR-0821796]; Division of Materials Sciences and Engineering of BES DOE; ORNL by the Scientific User Facilities Division, BES DOE; US Department of Energy, Office of Science, Basic Energy Sciences [DE-SC0010308] FX This work was supported by the Air Force Office of Scientific Research under Grant FA9550-12-10494, and the Office of Naval Research under Grant N000 14-10-1-0489. The acquisition of the JEM-ARM-200F at Arizona State University was supported by NSF Grant DMR-0821796. The research at ORNL was supported by the Division of Materials Sciences and Engineering (R.K.V., M.B.O., S.J. and S.V.K.) of BES DOE. Research was conducted at the CNMS, which is sponsored at ORNL by the Scientific User Facilities Division, BES DOE. The MIM work (Y.R., X.W. and K.L.) was supported by the US Department of Energy, Office of Science, Basic Energy Sciences under Award DE-SC0010308. NR 47 TC 14 Z9 14 U1 10 U2 68 PU NATURE PUBLISHING GROUP PI LONDON PA MACMILLAN BUILDING, 4 CRINAN ST, LONDON N1 9XW, ENGLAND SN 2041-1723 J9 NAT COMMUN JI Nat. Commun. PD JAN PY 2015 VL 6 AR 6067 DI 10.1038/ncomms7067 PG 7 WC Multidisciplinary Sciences SC Science & Technology - Other Topics GA CA3TW UT WOS:000348830600002 PM 25586049 ER PT J AU Wong, CY Cotts, BL Wu, H Ginsberg, NS AF Wong, Cathy Y. Cotts, Benjamin L. Wu, Hao Ginsberg, Naomi S. TI Exciton dynamics reveal aggregates with intermolecular order at hidden interfaces in solution-cast organic semiconducting films SO Nature Communications LA English DT Article ID FIELD-EFFECT TRANSISTORS; TRANSIENT ABSORPTION MICROSCOPY; THIN-FILMS; MOLECULAR PACKING; GRAIN-BOUNDARY; CARRIER TRANSPORT; SINGLE-CRYSTALS; TIPS-PENTACENE; FISSION; TEMPERATURE AB Large-scale organic electronics manufacturing requires solution processing. For small-molecule organic semiconductors, solution processing results in crystalline domains with high charge mobility, but the interfaces between these domains impede charge transport, degrading device performance. Although understanding these interfaces is essential to improve device performance, their intermolecular and electronic structure is unknown: they are smaller than the diffraction limit, are hidden from surface probe techniques, and their nanoscale heterogeneity is not typically resolved using X-ray methods. Here we use transient absorption microscopy to isolate a unique signature of a hidden interface in a TIPS-pentacene thin film, exposing its exciton dynamics and intermolecular structure. Surprisingly, instead of finding an abrupt grain boundary, we reveal that the interface can be composed of nanoscale crystallites interleaved by a web of interfaces that compound decreases in charge mobility. Our novel approach provides critical missing information on interface morphology necessary to correlate solution-processing methods to optimal device performance. C1 [Wong, Cathy Y.; Cotts, Benjamin L.; Wu, Hao; Ginsberg, Naomi S.] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Ginsberg, Naomi S.] Univ Calif Berkeley, Dept Phys, Berkeley, CA 94720 USA. [Ginsberg, Naomi S.] Lawrence Livermore Natl Lab, Phys Biosci & Mat Sci Div, Berkeley, CA 94720 USA. [Ginsberg, Naomi S.] Kavli Energy NanoSci Inst, Berkeley, CA 94720 USA. RP Ginsberg, NS (reprint author), Univ Calif Berkeley, Dept Chem, D64 Hildebrand Hall, Berkeley, CA 94720 USA. EM nsginsberg@berkeley.edu FU Defense Advanced Research Projects Agency Young Faculty Award [N66001-12-1-4228]; Natural Sciences and Engineering Research Council, Canada; National Science Foundation [DGE 1106400] FX This work has been supported by the Defense Advanced Research Projects Agency Young Faculty Award number N66001-12-1-4228. C.Y.W. thanks the Natural Sciences and Engineering Research Council, Canada for a Postdoctoral Fellowship; B. L. C. acknowledges the National Science Foundation Graduate Research Fellowship (DGE 1106400) and N.S.G. acknowledges a David and Lucile Packard Foundation Fellowship for Science and Engineering. We also thank N.A. Switz, S. B. Penwell and L. D. S. Ginsberg for assistance with high-resolution microscopy and analysis. NR 63 TC 18 Z9 18 U1 14 U2 81 PU NATURE PUBLISHING GROUP PI LONDON PA MACMILLAN BUILDING, 4 CRINAN ST, LONDON N1 9XW, ENGLAND SN 2041-1723 J9 NAT COMMUN JI Nat. Commun. PD JAN PY 2015 VL 6 AR 5946 DI 10.1038/ncomms6946 PG 7 WC Multidisciplinary Sciences SC Science & Technology - Other Topics GA CA3MK UT WOS:000348810700002 PM 25581561 ER PT J AU Regaldo, J Whitmore, D Knief, R von Estorff, U Varley, J AF Regaldo, Jacques Whitmore, David Knief, Ronald von Estorff, Ulrik Varley, James TI Outstanding industry training SO NUCLEAR ENGINEERING INTERNATIONAL LA English DT Editorial Material C1 [Regaldo, Jacques] World Assoc Nucl Operators, London, England. [Whitmore, David] Atkins, Epsom, Surrey, England. [Knief, Ronald] Sandia Natl Labs, Livermore, CA 94550 USA. RP Regaldo, J (reprint author), World Assoc Nucl Operators, London, England. NR 0 TC 0 Z9 0 U1 0 U2 0 PU WILMINGTON PUBL PI SIDCUP PA WILMINGTON HOUSE, MAIDSTONE RD, FOOTS CRAY, SIDCUP DA14 SHZ, KENT, ENGLAND SN 0029-5507 J9 NUCL ENG INT JI Nucl. Eng. Int. PD JAN PY 2015 VL 60 IS 726 BP 13 EP 13 PG 1 WC Nuclear Science & Technology SC Nuclear Science & Technology GA AZ2YN UT WOS:000348095300003 ER PT J AU Cecconello, M Jones, OM Boeglin, WU Perez, RV Darrow, DS Klimek, I Sharapov, SE Fitzgerald, M McClements, KG Keeling, DL Allan, SY Michael, CA Akers, RJ Conway, NJ Scannell, R Turnyanskiy, M Ericsson, G AF Cecconello, M. Jones, O. M. Boeglin, W. U. Perez, R. V. Darrow, D. S. Klimek, I. Sharapov, S. E. Fitzgerald, M. McClements, K. G. Keeling, D. L. Allan, S. Y. Michael, C. A. Akers, R. J. Conway, N. J. Scannell, R. Turnyanskiy, M. Ericsson, G. CA MAST Team TI Energetic ion behaviour in MAST SO PLASMA PHYSICS AND CONTROLLED FUSION LA English DT Article; Proceedings Paper CT 41st European-Physical-Society Conference on Plasma Physics CY JUN 23-27, 2014 CL Max Planck Inst Plasma Phys, Berlin, GERMANY HO Max Planck Inst Plasma Phys DE MAST; TAE; fishbones; LLM; sawtooth; fast ion diagnostics ID TOKAMAKS; CODE AB Recent studies of fast ion transport resulting from a range of instabilities, including n = 1 internal kink modes (fishbones and long-lived modes), toroidal Alfven eigenmodes and sawteeth have been carried out at MAST. Strong correlations were found between relative changes in magnetic edge coils signals, edge D a signal a fast ion D a system, a prototype collimated neutron flux monitor and a recently installed prototype charged fusion product detector array, indicating both redistribution and loss of fast ions. Preliminary interpretation of these observations with a suite of stability, modelling and interpretative codes is discussed. C1 [Cecconello, M.; Klimek, I.] Uppsala Univ, Dept Phys & Astron, SE-75105 Uppsala, Sweden. [Jones, O. M.; Sharapov, S. E.; Fitzgerald, M.; McClements, K. G.; Keeling, D. L.; Allan, S. Y.; Akers, R. J.; Conway, N. J.; Scannell, R.; Ericsson, G.; MAST Team] CCFE, Culham Sci Ctr, Abingdon OX14 3DB, Oxon, England. [Jones, O. M.] Univ Durham, Dept Phys, Durham DH1 3LE, England. [Boeglin, W. U.; Perez, R. V.] Florida Int Univ, Dept Phys, Miami, FL 33199 USA. [Darrow, D. S.] Princeton Plasma Phys Lab, Princeton, NJ 08543 USA. [Michael, C. A.] Australian Natl Univ, Canberra, ACT 0200, Australia. [Turnyanskiy, M.] EFDA CSU Garching, ITER Phys Dept, D-85748 Garching, Germany. RP Cecconello, M (reprint author), Uppsala Univ, Dept Phys & Astron, SE-75105 Uppsala, Sweden. EM marco.cecconello@physics.uu.se OI Michael, Clive/0000-0003-1804-870X FU Swedish Research Council; RCUK Energy Programme [EP/I501045]; European Union [633053]; US Department of Energy [DESC0001157, DEAC0209CH11466] FX This work was funded by the Swedish Research Council, the RCUK Energy Programme under grant EP/I501045, the European Union's Horizon 2020 research and innovation programme under grant agreement number 633053 and the US Department of Energy Contract Numbers DESC0001157 and DEAC0209CH11466. The views and opinions expressed herein do not necessarily reflect those of the European Commission. NR 26 TC 8 Z9 8 U1 4 U2 12 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 0741-3335 EI 1361-6587 J9 PLASMA PHYS CONTR F JI Plasma Phys. Control. Fusion PD JAN PY 2015 VL 57 IS 1 AR 014006 DI 10.1088/0741-3335/57/1/014006 PG 11 WC Physics, Fluids & Plasmas SC Physics GA AZ4MG UT WOS:000348194900007 ER PT J AU Gunter, S Yu, Q Lackner, K Bhattacharjee, A Huang, YM AF Guenter, S. Yu, Q. Lackner, K. Bhattacharjee, A. Huang, Y-M TI Fast sawtooth reconnection at realistic Lundquist numbers SO PLASMA PHYSICS AND CONTROLLED FUSION LA English DT Article; Proceedings Paper CT 41st European-Physical-Society Conference on Plasma Physics CY JUN 23-27, 2014 CL Max Planck Inst Plasma Phys, Berlin, GERMANY HO Max Planck Inst Plasma Phys DE magnetic reconnection; sawteeth; plasmoids; two-fluid effects ID HIGH-TEMPERATURE PLASMAS; MAGNETIC RECONNECTION; TOKAMAK; MODES AB Magnetic reconnection, a ubiquitous phenomenon in astrophysics, space science and magnetic confinement research, frequently proceeds much faster than predicted by simple resistive MHD theory. Acceleration can result from the break-up of the thin Sweet-Parker current sheet into plasmoids, or from two-fluid effects decoupling mass and magnetic flux transport over the ion inertial length v(A)/omega(ci) or the drift scale root T-e/m(i)/omega(ci), depending on the absence or presence of a strong magnetic guide field. We describe new results on the modelling of sawtooth reconnection in a simple tokamak geometry (circular cylindrical equilibrium) pushed to realistic Lundquist numbers for present day tokamaks. For the resistive MHD case, the onset criteria and the influence of plasmoids on the reconnection process agree well with earlier results found in the case of vanishing magnetic guide fields. While plasmoids are also observed in two-fluid calculations, they do not dominate the reconnection process for the range of plasma parameters considered in this study. In the two-fluid case they form as a transient phenomenon only. The reconnection times become weakly dependent on the S-value and for the most complete model-including two-fluid effects and equilibrium temperature and density gradients-agree well with those experimentally found on ASDEX Upgrade (<= 100 mu s). C1 [Guenter, S.; Yu, Q.; Lackner, K.] EURATOM, Max Planck Inst Plasmaphys, D-14476 Garching, Germany. [Bhattacharjee, A.; Huang, Y-M] Princeton Plasma Phys Lab, Princeton, NJ 08543 USA. [Guenter, S.; Yu, Q.; Lackner, K.; Bhattacharjee, A.; Huang, Y-M] Max Planck Princeton Ctr Plasma Phys, Berlin, Germany. RP Gunter, S (reprint author), EURATOM, Max Planck Inst Plasmaphys, D-14476 Garching, Germany. EM Sibylle.Guenter@ipp.mpg.de RI Huang, Yi-Min/G-6926-2011 OI Huang, Yi-Min/0000-0002-4237-2211 NR 36 TC 12 Z9 12 U1 4 U2 13 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 0741-3335 EI 1361-6587 J9 PLASMA PHYS CONTR F JI Plasma Phys. Control. Fusion PD JAN PY 2015 VL 57 IS 1 AR 014017 DI 10.1088/0741-3335/57/1/014017 PG 6 WC Physics, Fluids & Plasmas SC Physics GA AZ4MG UT WOS:000348194900018 ER PT J AU Lynch, PT Annesley, CJ Tranter, RS AF Lynch, Patrick T. Annesley, Christopher J. Tranter, Robert S. TI Dissociation of ortho-benzyne radicals in the high temperature fall-off regime SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Phenyl fluoride; Soot formation; Shock tube; Benzyne pyrolysis ID AB-INITIO; UNIMOLECULAR DECOMPOSITION; PHENYL; PYROLYSIS; FLUOROBENZENE; ACETYLENE; ENERGY AB The decomposition of ortho-benzyne radicals (o-C6H4), generated from the dissociation of a new precursor, fluorobenzene (C6H5F), has been investigated in a diaphragmless shock tube in a combined laser schlieren densitometry, LS, (P-2 = 30 +/- 2, 59 +/- 3, 121 +/- 5 Torr, 2050 < T-2 < 2980)/time-of-flight mass spectrometry, TOF-MS (P-5 = 1150 +/- 200 Torr, 2300 < T-5 < 2800 K) study. The LS density gradient profiles were simulated, and excellent agreement was found between simulations and experimental profiles. Rate coefficients for C6H5F -> o-C6H4 + HF, o-C6H4 -> C4H2 + C2H2, and o-C6H4 -> C6H3 + H were obtained. Good agreement with Xu et al. [ Proc. Combust. Inst., 31(2007) 231-239] with respect to the o-benzyne dissociation branching ratio was found. However a strong pressure dependence was also observed in o-benzyne dissociation which was not seen by Xu et al. For o-C6H4 -> C4H2 + C2H2: k(2a,) (120Torr) = (1.2 + 0.4) x 10(63) T-14.27 exp(-52,710/T) k(2a,60Torr) = (1.4 + 0.5) x 10(60) T-13.595 exp(-50,538/T), k(2a,30Torr) = (4.0 +/- 1.3) x 10(57) T-13.015 exp(-48,628/T) s(-1). The inclusion of high temperature o-benzyne abstraction reactions is necessary to simulate the reacting system, and we report estimates of the rate of o-C6H4 + C6H5F. (C) 2013 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Lynch, Patrick T.; Annesley, Christopher J.; Tranter, Robert S.] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. [Lynch, Patrick T.] Univ Michigan, Dept Mech Engn, Dearborn, MI 48128 USA. RP Tranter, RS (reprint author), Argonne Natl Lab, Chem Sci & Engn Div, Bldg 200, Argonne, IL 60439 USA. EM tranter@anl.gov FU Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences, U.S. Department of Energy [DE-AC02-06CH11357] FX This work was performed under the auspices of the Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences, U.S. Department of Energy, under Contract Number DE-AC02-06CH11357. We thank Professor John Kiefer for helpful discussions on this topic. NR 26 TC 1 Z9 1 U1 2 U2 13 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 145 EP 152 DI 10.1016/j.proci.2014.05.049 PN 1 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2EN UT WOS:000348047500006 ER PT J AU Peukert, SL Sivaramakrishnan, R Michael, JV AF Peukert, Sebastian L. Sivaramakrishnan, Raghu Michael, Joe V. TI High temperature rate constants for H/D plus n-C4H10 and i-C4H10 SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Shock tube; Abstraction; Ab initio; Transition state theory; Kinetic isotope effects ID TOTAL ATOMIZATION ENERGIES; PRESSURE RATE-CONSTANT; CH4 DISSOCIATION; SHOCK-WAVES; PHOTOLYSIS; MOLECULES; KINETICS; STATE; FLASH; GAS AB The reactions of D/H with n-C4H10 and i-C4H10 have been studied with both shock-tube experiments and ab initio transition state theoretical calculations. D-atom profiles were measured behind reflected shock waves using D-atom atomic resonance absorption spectrometry (ARAS) in mixtures with C2D5I (D-atom precursor, < 1 ppm) and the alkane of interest in excess (> 200 ppm), over the T-range 1063-1327 K, at pressures congruent to 0.5 atm. D-atom depletion in the present experiments is sensitive only to the reactions, D + n - C4H10 -> products (A) D + i - C4H(10) -> products. (B) Simulations of the measured D-atom profiles allow for determinations of total rate constants for the processes (A) and (B). The experimental rate constants are well represented by the Arrhenius equations, k(A) = 2.11 x 10(-9) exp(-5661 K/T) cm(3) molecules(-1) s(-1) (1074-1253 K) k(B) = 2.57 x 10(-9) exp(-5798 K/T) cm(3) molecules(-1) s(-1) (1063-1327 K) The title reactions have also been characterized using electronic structure theory at the CCSD(T)/cc-pV infinity Z//M06-2X/cc-pvtz level of theory. Over the T-range of the present experiments, the ab initio based transition state theory (TST) kinetics predictions for the isotope effects, k(D)/k(H), are near unity. The theoretical predictions are in good agreement with the experimental results and can be represented by the modified Arrhenius equations, k(A); THEORY = 6.677 x 10(-17) T-2.118 exp(-2700 K/T) cm(3) molecules(-1) s(-1) (500-2000 K) k(B); THEORY = 5.627 x 10(-20) T-2.934 exp(-1225 K/T) cm(3) molecules(-1) s(-1) (500-2000 K) To our knowledge, the present experiments are the first direct measurements for the title reactions and the rate constants from this combined experimental/theoretical effort are recommended for use in combustion modeling. Results from the present studies on n-C4H10 and i-C4H10 along with prior studies on C2H6 and C3H8 suggest the applicability of rate rules for H + Alkanes that are based on generic primary, secondary, and tertiary abstraction sites. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Peukert, Sebastian L.; Sivaramakrishnan, Raghu; Michael, Joe V.] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. RP Sivaramakrishnan, R (reprint author), Argonne Natl Lab, L-117,Bldg 200, Argonne, IL 60439 USA. EM raghu@anl.gov; jmichael@anl.gov RI SIVARAMAKRISHNAN, RAGHU/C-3481-2008 OI SIVARAMAKRISHNAN, RAGHU/0000-0002-1867-1254 FU U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences [DE-AC02-06CH11357]; Argonne-Sandia Consortium on High-Pressure Combustion Chemistry, FWP [2009 ANL 59044] FX This work was supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences, under Contract No. DE-AC02-06CH11357. Support for R. S. and partial support for J. V. M. was provided as part of the Argonne-Sandia Consortium on High-Pressure Combustion Chemistry, FWP# 2009 ANL 59044. NR 32 TC 1 Z9 1 U1 4 U2 13 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 171 EP 179 DI 10.1016/j.proci.2014.05.104 PN 1 PG 9 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2EN UT WOS:000348047500009 ER PT J AU Zador, J Miller, JA AF Zador, Judit Miller, James A. TI Adventures on the C3H5O potential energy surface: OH plus propyne, OH plus allene and related reactions SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Pressure dependence; Propargyl; Master equation ID PHENOMENOLOGICAL RATE COEFFICIENTS; WELL MASTER EQUATION; RATE CONSTANTS; GAS-PHASE; REACTION DYNAMICS; RADICAL REACTION; KINETICS; TEMPERATURE; SERIES; PRESSURE AB We mapped out the stationary points and the corresponding conformational space on the C3H5O potential energy surface relevant for the OH + allene and OH + propyne reactions systematically and automatically using the KinBot software at the UCCSD(T)-F12b/cc-pVQZ-F12//M06-2X/6-311++ G(d,p) level of theory. We used RRKM-based 1-D master equations to calculate pressure-and temperature-dependent, channel-specific phenomenological rate coefficients for the bimolecular reactions propyne + OH and allene + OH, and for the unimolecular decomposition of the CH3CCHOH, CH3C( OH) CH, CH2CCH2OH, CH2C(OH)CH2 primary adducts, and also for the related acetonyl, propionyl, 2-methylvinoxy, and 3-oxo-1-propyl radicals. The major channel of the bimolecular reactions at high temperatures is the formation propargyl + H2O, which makes the title reactions important players in soot formation at high temperatures. However, below similar to 1000 K the chemistry is more complex, involving the competition of stabilization, isomerization and dissociation processes. We found that the OH addition to the central carbon of allene has a particularly interesting and complex pressure dependence, caused by the low-lying exit channel to form ketene + CH3 bimolecular products. We compared our results to a wide range of experimental data and assessed possible uncertainties arising from certain aspects of the theoretical framework. (C) 2013 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Zador, Judit] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. [Miller, James A.] Argonne Natl Lab, Div Chem, Argonne, IL 60439 USA. RP Zador, J (reprint author), Sandia Natl Labs, Combust Res Facil, Mail Stop 9055, Livermore, CA 94551 USA. EM jzador@sandia.gov RI Zador, Judit/A-7613-2008 OI Zador, Judit/0000-0002-9123-8238 FU Division of Chemical Sciences, Geosciences, and Biosciences, the Office of Basic Energy Sciences, the U.S. Department of Energy under DOE [DE-AC02-06CH11357]; ASC-HPCC (ANL FWP) [DE-AC02-2006-CH11357, 59044] FX This work is supported by the Division of Chemical Sciences, Geosciences, and Biosciences, the Office of Basic Energy Sciences, the U.S. Department of Energy under DOE Contract Numbers DE-AC02-06CH11357. Sandia is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the National Nuclear Security Administration. J.A.M. was supported under contract number DE-AC02-2006-CH11357 as part of the ASC-HPCC (ANL FWP #59044). NR 43 TC 9 Z9 9 U1 3 U2 46 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 181 EP 188 DI 10.1016/j.proci.2014.05.103 PN 1 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2EN UT WOS:000348047500010 ER PT J AU Jasper, AW Oana, CM Miller, JA AF Jasper, Ahren W. Oana, C. Melania Miller, James A. TI "Third-Body" collision efficiencies for combustion modeling: Hydrocarbons in atomic and diatomic baths SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Classical trajectory simulations; Unimolecular kinetics; Bath gas efficiencies; Weak collider; Angular momentum ID REVERSIBLE-ARROW CH3; ENERGY-TRANSFER; MASTER EQUATION; UNIMOLECULAR REACTIONS; POLYATOMIC-MOLECULES; CHEMICAL-KINETICS; GAS-PHASE AB The collisional energy transfer dynamics relevant to the unimolecular kinetics of linear, branched, and cyclic hydrocarbons, including both radicals and saturated and unsaturated molecules, in atomic and diatomic baths is studied via classical trajectories. A set of full-dimensional potential energy surfaces (PESs) suitable for efficient trajectory simulations involving large hydrocarbons (CxHy) colliding with any of seven baths (M = He, Ne, Ar, Kr, H-2, N-2, O-2) is validated against direct dynamics calculations for two small systems. The PESs are then used to calculate Lennard-Jones collision parameters, and a general rule for calculating these parameters based only on the number of carbon atoms and the bath gas is obtained. Next, the PESs are used to calculate low-order moments of the collisional energy transfer function relevant to low-pressure-limit unimolecular kinetics for a total of 266 systems (38 unimolecular reactants in 7 baths), with a focus on the average angular momentum and total energy transferred in deactivating collisions. These moments are used to quantify the relative rotational and total collision efficiencies of the 7 baths for the various hydrocarbon reactants. Trends in the collision efficiencies with respect to the chemical structures of the hydrocarbon reactants are discussed. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Jasper, Ahren W.; Oana, C. Melania] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. [Miller, James A.] Argonne Natl Lab, Div Chem, Argonne, IL 60439 USA. RP Jasper, AW (reprint author), Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. EM ajasper@sandia.gov RI Jasper, Ahren/A-5292-2011 FU Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy; National Nuclear Security Administration [DE-AC04-94-AL85000]; Argonne-Sandia Consortium on High-Pressure Combustion Chemistry FX A.W.J. was supported by the Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy. Sandia is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the National Nuclear Security Administration under contract DE-AC04-94-AL85000. C. M. O. and J.A.M. were supported as part of the Argonne-Sandia Consortium on High-Pressure Combustion Chemistry. NR 22 TC 21 Z9 22 U1 4 U2 24 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 197 EP 204 DI 10.1016/j.proci.2014.05.105 PN 1 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2EN UT WOS:000348047500012 ER PT J AU Burke, MP Goldsmith, CF Georgievskii, Y Klippenstein, SJ AF Burke, Michael P. Goldsmith, C. Franklin Georgievskii, Yuri Klippenstein, Stephen J. TI Towards a quantitative understanding of the role of non-Boltzmann reactant distributions in low temperature oxidation SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Low-temperature chemistry; Non-Boltzmann; Hot reactions; Rovibrationally excited states ID MASTER-EQUATION; OH PRODUCTION; O-2; KINETICS AB An essentially universal assumption of chemical kinetics is that bimolecular reactions only occur between reactants of rovibrational energy described by a Boltzmann (thermal) distribution. Given that the O-2 mole fraction is roughly 20% under nearly all relevant low-temperature combustion situations, there is significant potential for molecules to undergo reactive collisions with O-2 on the same time scale as the energy-transferring collisions necessary to achieving a Boltzmann distribution. Within the context of low-temperature combustion, this phenomenon conceivably gives rise to an entirely non-Boltzmann sequence involving multiple reactions of fuel-derived radicals with O-2 to produce multiple OH radicals. Given the complex interplay among simultaneous internal isomerizations, energy-transferring collisions, dissociations and reactive collisions across multiple reaction surfaces, estimating the extent of deviations from conventional thermal assumptions is not straightforward. A novel methodology is presented for coupling multiple master equations and deriving effective phenomenological rate constants for thermal sets of reactants to thermal sets of products in chemically activated sequences that proceed across multiple reaction surfaces. The methodology is used to establish a better understanding of the nature of non-Boltzmann reactant distribution effects and quantify their magnitude. As a case study, we implement the methodology to explore the effect of non-Boltzmann reactants on product branching fractions of the QOOH* + O-2 reaction from n-propyl oxidation as well as its associated dependence with O-2 mole fraction, temperature, and pressure. While it appears that the effect of non-Boltzmann reaction sequences will be considerably smaller at higher pressures (at least for propane), it appears that consideration of non-Boltzmann reaction sequences is likely required for interpretations of experimental measurements commonly used to investigate the R + O-2 and QOOH + O-2 reactions central to engine-relevant ignition behavior. With regard to observable signatures of these effects in experiments, the presence of a stronger-than-usual O-2 mole fraction dependence may be a likely indicator of non-Boltzmann behavior. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Burke, Michael P.; Goldsmith, C. Franklin; Georgievskii, Yuri; Klippenstein, Stephen J.] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. RP Burke, MP (reprint author), Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. EM mpburke@columbia.edu OI Klippenstein, Stephen/0000-0001-6297-9187 FU Argonne National Lab; U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences as part of the Argonne-Sandia Consortium on High-Pressure Combustion Chemistry, (ANL FWP) [DE-AC02-06CH 11357, 59044] FX This work was supported by a Director's Post-doctoral Fellowship from Argonne National Lab (MPB, CFG) and by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences, under Contract No. DE-AC02-06CH 11357 as part of the Argonne-Sandia Consortium on High-Pressure Combustion Chemistry, (ANL FWP # 59044). NR 25 TC 16 Z9 17 U1 9 U2 34 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 205 EP 213 DI 10.1016/j.proci.2014.05.118 PN 1 PG 9 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2EN UT WOS:000348047500013 ER PT J AU Ye, LL Georgievskii, Y Klippenstein, SJ AF Ye, Lili Georgievskii, Yuri Klippenstein, Stephen J. TI Pressure-dependent branching in the reaction of (CH2)-C-1 with C2H4 and other reactions on the C3H6 potential energy surface SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Propene decomposition; Ab initio; Allyl; Rate coefficients; Variable-reaction-coordinate transition state theory ID CORRELATED MOLECULAR CALCULATIONS; RESONANCE-STABILIZED RADICALS; GAUSSIAN-BASIS SETS; PROPENE PYROLYSIS; SHOCK-TUBE; PREDICTIVE THEORY; MASTER EQUATION; PRODUCT YIELDS; RATE CONSTANTS; WAVE-FUNCTIONS AB A number of reactions on the C3H6 potential energy surface (PES) are of central importance to various combustion environments. High level theoretical methods were used to predict the temperature and pressure dependent kinetics for these reactions. The rovibrational properties of the key stationary points in the systems were determined with the CCSD(T)/cc-pVTZ method. High accuracy energies for these stationary points were obtained via the consideration of basis set, higher-order correlation, core-valence, anharmonic vibrational, relativistic, and diagonal Born-Oppenheimer corrections. Variable reaction coordinate transition state theory (VRC-TST) was employed to treat the barrierless channels on the PES, while, for channels possessing a distinct barrier, rate coefficients were instead obtained with conventional transition state theory employing rigid-rotor harmonic oscillator assumptions. For the VRC-TST calculations, the interaction energies required for the evaluation of the reactive flux were evaluated with the CASPT2/cc-pVTZ approach for the orientational sampling, coupled with one-dimensional corrections based on higher accuracy evaluations along the minimum energy path. A priori predictions for the temperature and pressure-dependent rate coefficients were obtained through master-equation calculations incorporating these TST predictions for the microcanonical rate coefficients coupled with a simple model for the collisional energy transfer rates. These theoretical predictions compare favorably with the limited experimental data. The analysis yields modified Arrhenius rate expressions for the (CH2)-C-1 + C2H4, C2H3 + CH3, CH2CHCH2 + H, CH3CCH2 + H, and CH3CHCH + H recombination reactions as well as for the dissociations and isomerizations of propene and cyclopropane. (C) 2013 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Ye, Lili; Georgievskii, Yuri; Klippenstein, Stephen J.] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. [Ye, Lili] Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Anhui, Peoples R China. RP Klippenstein, SJ (reprint author), 9700 S Cass Ave, Argonne, IL 60439 USA. EM sjk@anl.gov FU U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences [DE-AC02-06CH11357] FX This work was supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences, under Contract No. DE-AC02-06CH11357. NR 35 TC 5 Z9 5 U1 4 U2 22 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 223 EP 230 DI 10.1016/j.proci.2014.05.097 PN 1 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2EN UT WOS:000348047500015 ER PT J AU Sarathy, SM Kukkadapu, G Mehl, M Wang, WJ Javed, T Park, S Oehlschlaeger, MA Farooq, A Pitz, WJ Sung, CJ AF Sarathy, S. Mani Kukkadapu, Goutham Mehl, Marco Wang, Weijing Javed, Tamour Park, Sungwoo Oehlschlaeger, Matthew A. Farooq, Aamir Pitz, William J. Sung, Chih-Jen TI Ignition of alkane-rich FACE gasoline fuels and their surrogate mixtures SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Gasoline; Combustion; Chemical kinetics modeling; Surrogate fuels; Ignition ID RAPID COMPRESSION MACHINE; DELAY TIMES; SHOCK-TUBE; 3-METHYLHEPTANE; AUTOIGNITION; OXIDATION AB Petroleum derived gasoline is the most used transportation fuel for light-duty vehicles. In order to better understand gasoline combustion, this study investigated the ignition propensity of two alkane-rich FACE (Fuels for Advanced Combustion Engines) gasoline test fuels and their corresponding PRF (primary reference fuel) blend in fundamental combustion experiments. Shock tube ignition delay times were measured in two separate facilities at pressures of 10, 20, and 40 bar, temperatures from 715 to 1500 K, and two equivalence ratios. Rapid compression machine ignition delay times were measured for fuel/air mixtures at pressures of 20 and 40 bar, temperatures from 632 to 745 K, and two equivalence ratios. Detailed hydrocarbon analysis was also performed on the FACE gasoline fuels, and the results were used to formulate multi-component gasoline surrogate mixtures. Detailed chemical kinetic modeling results are presented herein to provide insights into the relevance of utilizing PRF and multi-component surrogate mixtures to reproduce the ignition behavior of the alkane-rich FACE gasoline fuels. The two FACE gasoline fuels and their corresponding PRF mixture displayed similar ignition behavior at intermediate and high temperatures, but differences were observed at low temperatures. These trends were mimicked by corresponding surrogate mixture models, except for the amount of heat release in the first stage of a two-stage ignition events, when observed. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Sarathy, S. Mani; Javed, Tamour; Park, Sungwoo; Farooq, Aamir] King Abdullah Univ Sci & Technol, Clean Combust Res Ctr, Thuwal 239556900, Saudi Arabia. [Kukkadapu, Goutham; Sung, Chih-Jen] Univ Connecticut, Dept Mech Engn, Storrs, CT USA. [Mehl, Marco; Pitz, William J.] Lawrence Livermore Natl Lab, Livermore, CA USA. [Wang, Weijing; Oehlschlaeger, Matthew A.] Rensselaer Polytech Inst, Troy, NY USA. RP Sarathy, SM (reprint author), King Abdullah Univ Sci & Technol, Clean Combust Res Ctr, Al Kindi Bldg 5 Room 4336, Thuwal 239556900, Saudi Arabia. EM mani.sarathy@kaust.edu.sa RI Farooq, Aamir/B-2550-2013; Sarathy, S. Mani/M-5639-2015; Mehl, Marco/A-8506-2009; OI Farooq, Aamir/0000-0001-5296-2197; Sarathy, S. Mani/0000-0002-3975-6206; Mehl, Marco/0000-0002-2227-5035; Park, Sungwoo/0000-0002-2800-1908 FU Clean Combustion Research Center; Saudi Aramco under the FUELCOM program; Combustion Energy Frontier Research Center, an Energy Frontier Research Center - US Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001198]; U.S. Air Force Office of Scientific Research [FA9550-11-1-0261]; US Department of Energy by Lawrence Livermore National Laboratory [DE-AC52-07NA27344]; U.S. Department of Energy, Office of Vehicle Technologies FX The authors are grateful to Hendrik Muller (Saudi Aramco R&DC), Abdulla Algam (Saudi Aramco R&DC), Mr. Emad Alawi, and Nadim Hourani (KAUST) for the DHA results. The KAUST authors acknowledge funding support from the Clean Combustion Research Center and from Saudi Aramco under the FUELCOM program. The work at the University of Connecticut was supported as part of the Combustion Energy Frontier Research Center, an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, under Award Number DE-SC0001198. The Rensselaer group was supported by the U.S. Air Force Office of Scientific Research (Grant No. FA9550-11-1-0261) with Dr. Chiping Li as technical monitor. The LLNL work was performed under the auspices of the US Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344 and was supported by the U.S. Department of Energy, Office of Vehicle Technologies, Gurpreet Singh, program manager. NR 25 TC 29 Z9 29 U1 4 U2 32 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 249 EP 257 DI 10.1016/j.proci.2014.05.122 PN 1 PG 9 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2EN UT WOS:000348047500018 ER PT J AU Goldsmith, CF Burke, MP Georgievskii, Y Klippenstein, SJ AF Goldsmith, C. Franklin Burke, Michael P. Georgievskii, Yuri Klippenstein, Stephen J. TI Effect of non-thermal product energy distributions on ketohydroperoxide decomposition kinetics SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Low-temperature ignition; Propane oxidation; Master equation; Direct dynamics; Non-Boltzmann effects AB The decomposition of ketohydroperoxides (OQ'OOH) to two radicals is commonly predicted to be the key chain branching step in low-temperature combustion. The possibility of a direct decomposition of the OQ'OOH from its initially produced energy distribution is studied with a combination of master equation (ME) and direct trajectory simulations. The temperature and pressure dependent rate constants for the thermal decomposition of a ketohydroperoxide, HOOCH2CH2CHO, to four product channels were computed using RRKM/ME methods. Direct dynamics calculations were initiated from a transition state in the O-2 + QOOH reaction network to understand the fraction of energy in that transition state that is converted into the internal energy of the OQ'OOH. A novel approach to solving the master equation is used to determine the probability that a vibrationally hot OQ'OOH either will be stabilized to a thermal distribution or will react to form new products. Under most conditions, the majority of vibrationally excited OQ'OOH will be quenched into a thermal distribution. At higher internal energies and lower pressures, however, a significant fraction of the hot OQ'OOH will decompose rather than thermalize. Proper interpretation of low-pressure experiments may require inclusion of vibrationally hot intermediates, particularly if a chemical kinetic mechanism is optimized against the low-pressure data. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Goldsmith, C. Franklin; Burke, Michael P.; Georgievskii, Yuri; Klippenstein, Stephen J.] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. RP Klippenstein, SJ (reprint author), Argonne Natl Lab, Chem Sci & Engn Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM sjk@anl.gov OI Klippenstein, Stephen/0000-0001-6297-9187 FU Division of Chemical Sciences, Geosciences, and Biosciences, the Office of Basic Energy Sciences, the U.S. Department of Energy as part of the Argonne-Sandia Consortium on High-Pressure Combustion Chemistry (FWP) [DE-AC04-94-AL85000, 59044]; Argonne Director's Postdoctoral Fellowship FX This work was supported by the Division of Chemical Sciences, Geosciences, and Biosciences, the Office of Basic Energy Sciences, the U.S. Department of Energy, under contract number DE-AC04-94-AL85000 as part of the Argonne-Sandia Consortium on High-Pressure Combustion Chemistry (FWP # 59044). CFG and MPB gratefully acknowledge financial support from the Argonne Director's Postdoctoral Fellowship. NR 16 TC 13 Z9 13 U1 5 U2 31 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 283 EP 290 DI 10.1016/j.proci.2014.05.006 PN 1 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2EN UT WOS:000348047500022 ER PT J AU Eskola, AJ Welz, O Zador, J Antonov, IO Sheps, L Savee, JD Osborn, DL Taatjes, CA AF Eskola, A. J. Welz, O. Zador, J. Antonov, I. O. Sheps, L. Savee, J. D. Osborn, D. L. Taatjes, C. A. TI Probing the low-temperature chain-branching mechanism of n-butane autoignition chemistry via time-resolved measurements of ketohydroperoxide formation in photolytically initiated n-C4H10 oxidation SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Ketohydroperoxide; n-Butane; Autoignition; Chain branching; Time-resolved ID COMBUSTION; KINETICS AB Ketohydroperoxide formation in Cl-atom initiated low-temperature (550-700 K) oxidation of n-butane was investigated using a time-of-flight mass spectrometer and either tunable synchrotron radiation or a H-2 discharge for photoionization. Experiments were performed at 1-2 atm pressure using a new high-pressure reactor and also at similar to 5 Torr pressure for comparison. Direct kinetic observations of ketohydroperoxide formation qualitatively agree with previous atmospheric pressure jet-stirred reactor studies of Battin-Leclerc et al. (Angew. Chem. Int. Ed., 49 (2010) 3169-3172) where the maximum ketohydroperoxide signal was observed near 600 K. Oxidation of partially deuterated n-butanes provided additional information on the QOOH radical intermediates that proceed to form ketohydroperoxides. The photoionization spectrum of the observed ketohydroperoxide is independent of pressure and is the same when using different deuterium substituted n-butanes, suggesting that one ketohydroperoxide isomer dominates in n-butane oxidation. We conclude that 4-hydroperoxy-2-butyl + O-2 is the main reaction leading to ketohydroperoxide and 3-hydroperoxybutanal is the sole ketohydroperoxide that is observed. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Eskola, A. J.; Welz, O.; Zador, J.; Antonov, I. O.; Sheps, L.; Savee, J. D.; Osborn, D. L.; Taatjes, C. A.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. RP Taatjes, CA (reprint author), Sandia Natl Labs, Combust Res Facil, Mail Stop 9055, Livermore, CA 94551 USA. EM cataatj@sandia.gov RI Welz, Oliver/C-1165-2013; Zador, Judit/A-7613-2008 OI Welz, Oliver/0000-0003-1978-2412; Zador, Judit/0000-0002-9123-8238 FU Saudi Aramco "Kinetics Cluster of Excellence" under a cooperative research and development agreement (CRADA) [CRADA SC10/01773.00, 6500007287]; Office of Science, Office of Basic Energy Sciences of the U.S. Department of Energy (BES/USDOE) [DE-AC02-05CH11231]; Argonne-Sandia Consortium on High-Pressure Combustion Chemistry (SNL FWP) [014544]; Division of Chemical Sciences, Geosciences, and Biosciences, BES/USDOE; National Nuclear Security Administration [DE-AC04-94-AL85000] FX We thank Mr. Howard Johnsen for excellent technical support. This work was supported as part of the Saudi Aramco "Kinetics Cluster of Excellence" under a cooperative research and development agreement (CRADA) between Sandia National Laboratories and Aramco Services Company, a U.S.-based subsidiary of Saudi Aramco, the state-owned national oil company of Saudi Arabia CRADA SC10/01773.00, ASC Contract No. 6500007287). The Advanced Light Source is supported by the Director, Office of Science, Office of Basic Energy Sciences of the U.S. Department of Energy (BES/USDOE) under Contract No. DE-AC02-05CH11231 at Lawrence Berkeley National Laboratory. LS was supported through the Argonne-Sandia Consortium on High-Pressure Combustion Chemistry (SNL FWP #014544). The contributions of JDS, JZ, and DLO, as well as the development and maintenance of the experimental apparatus, are supported by the Division of Chemical Sciences, Geosciences, and Biosciences, BES/USDOE. Sandia is a multi-program laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the National Nuclear Security Administration under contract DE-AC04-94-AL85000. NR 13 TC 9 Z9 10 U1 6 U2 48 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 291 EP 298 DI 10.1016/j.proci.2014.05.011 PN 1 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2EN UT WOS:000348047500023 ER PT J AU Nawdiyal, A Hansen, N Zeuch, T Seidel, L Mauss, F AF Nawdiyal, A. Hansen, N. Zeuch, T. Seidel, L. Mauss, F. TI Experimental and modelling study of speciation and benzene formation pathways in premixed 1-hexene flames SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE 1-Hexene flames; Benzene formation pathways; Molecular beam sampling; Near threshold ionization; Fulvene ID N-HEPTANE OXIDATION; COMBUSTION CHEMISTRY; AROMATIC-COMPOUNDS; ALIPHATIC FUELS; REACTION-MECHANISM; RICH FLAMES; SHOCK-TUBE; ACETYLENE; PRESSURE; CYCLOHEXANE AB An existing detailed and broadly validated kinetic scheme is augmented to capture the flame chemistry of 1-hexene under stoichiometric and fuel rich conditions including benzene formation pathways. In addition, the speciation in a premixed stoichiometric 1-hexene flame (flat-flame McKenna-type burner) has been studied under a reduced pressure of 20-30 mbar applying flame-sampling molecular-beam time-of-flight mass spectrometry and photoionization by tunable vacuum-ultraviolet synchrotron radiation. Mole fraction profiles of 40 different species have been measured and validated against the new detailed chemical reaction model consisting of 275 species and 3047 reversible elementary reactions. A good agreement of modelling results with the experimentally observed mole fraction profiles has been found under both stoichiometric and fuel rich conditions providing a sound basis for analyzing benzene formation pathways during 1-hexene combustion. The analysis clearly shows that benzene formation via the fulvene intermediate is a very important pathway for 1-hexene. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Nawdiyal, A.; Seidel, L.; Mauss, F.] Brandenburg Tech Univ Cottbus, D-03046 Cottbus, Germany. [Hansen, N.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. [Zeuch, T.] Univ Gottingen, Inst Phys Chem, D-37077 Gottingen, Germany. RP Mauss, F (reprint author), Brandenburg Tech Univ Cottbus, Siemens Halske Ring 8, D-03046 Cottbus, Germany. EM Fabian.Mauss@tdtvt.de RI Hansen, Nils/G-3572-2012 FU Office of Science, BES, USDOE [DE-AC02-05CH11231]; National Nuclear Security Administration [DE-AC04-94-AL85000] FX The Advanced Light Source is supported by the Director, Office of Science, BES, USDOE under Contract No. DE-AC02-05CH11231. Sandia is a multi-program laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the National Nuclear Security Administration under contract DE-AC04-94-AL85000. NR 45 TC 6 Z9 6 U1 2 U2 31 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 325 EP 332 DI 10.1016/j.proci.2014.06.047 PN 1 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2EN UT WOS:000348047500027 ER PT J AU Fridlyand, A Goldsborough, SS Brezinsky, K Merchant, SS Green, WH AF Fridlyand, Aleksandr Goldsborough, S. Scott Brezinsky, Kenneth Merchant, Shamel S. Green, William H. TI Influence of the double bond position on the oxidation of decene isomers at high pressures and temperatures SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Decene; Double bond; Oxidation; Shock tube; Kinetic model ID PULSE SHOCK-TUBE; BIODIESEL FUELS; NOX EMISSIONS; COMBUSTION; RECOMBINATION; AUTOIGNITION; PYROLYSIS; SURROGATE; MULTIPLE; RADICALS AB High pressure, single pulse shock tube oxidation experiments were conducted in order to probe the chemical kinetic effects of the double bond position in long alkenes. All oxidation experiments were carried out with approximately 100 ppm of 1-decene, cis-2-decene, cis-5-decene, and trans-5-decene, in argon, at stoichiometric conditions. The experimental conditions covered the pressure range of 40-66 bar and temperature range of 850-1500 K, with an average reaction time of 2 ms. Gas chromatographic measurements of the stable intermediates indicated increased reactivity for the isomers with more centrally located double bonds, with no influence from the cis-trans configuration observed at these conditions. Significantly different yields in most of the intermediate species measured were observed. Chemical kinetic models were assembled with the aid of Reaction Mechanism Generator where these are able to adequately predict the major product species of all isomers investigated. Simulation of the experiments indicates significantly different reaction pathways that each decene isomers undergoes, controlled entirely by the position of the double bond. The implication for fuels with such molecular structure is that reactivity, as well as pollutant formation characteristics can be significantly different depending on the position of the double bond in very similar molecules. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Fridlyand, Aleksandr; Goldsborough, S. Scott; Brezinsky, Kenneth] Univ Illinois, Dept Mech & Ind Engn, Chicago, IL 60607 USA. [Goldsborough, S. Scott] Argonne Natl Lab, Ctr Transportat Res, Argonne, IL 60439 USA. [Merchant, Shamel S.; Green, William H.] MIT, Dept Chem Engn, Cambridge, MA 02139 USA. RP Brezinsky, K (reprint author), 2039 Engn Res Facil M-C 251,842 W Taylor St, Chicago, IL 60607 USA. EM kenbrez@uic.edu OI Fridlyand, Aleksandr/0000-0001-8514-8407 NR 37 TC 7 Z9 7 U1 1 U2 10 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 333 EP 340 DI 10.1016/j.proci.2014.06.020 PN 1 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2EN UT WOS:000348047500028 ER PT J AU Mehl, M Herbinet, O Dirrenberger, P Bounaceur, R Glaude, PA Battin-Leclerc, F Pitz, WJ AF Mehl, Marco Herbinet, Olivier Dirrenberger, Patricia Bounaceur, Roda Glaude, Pierre-Alexandre Battin-Leclerc, Frederique Pitz, William J. TI Experimental and modeling study of burning velocities for alkyl aromatic components relevant to diesel fuels SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Kinetic modeling; Toluene; Ethyl-benzene; Propyl-benzene; Butyl-benzene ID LAMINAR FLAME SPEEDS; RAPID COMPRESSION MACHINE; N-PROPYLBENZENE; SHOCK-TUBE; OXYGEN-NITROGEN; OXIDATION; MIXTURES; BUTYLBENZENE; EXTINCTION; IGNITION AB Aromatic species represent a significant fraction (about one third by weight) of both diesel and gasoline fuels. Much of the aromatics in diesel and gasoline are alkyl-benzene species. Although toluene, the lightest of the alkyl-benzenes, has been the subject of extensive literature investigations, very little experimental data are available for heavier alkyl-benzenes (9-20 carbon atoms) relevant to diesel fuel. In this work, the burning velocity of ethyl-, n-propyl- and n-butyl-benzenes were measured in a premixed flat-flame burner using the heat flux method. The burning velocities were measured as a function of the equivalence ratio at atmospheric pressure and for two unburned gas temperatures (358 and 398 K). These new experiments are compared with burning velocities for toluene previously measured by the authors. The comparisons showed that ethyl-benzene has the highest flame speed, followed by n-propyl- and n-butyl-benzenes which have similar burning velocities. Toluene has the lowest flame speed. Excellent agreement was observed between the new measurements and simulations using a mechanism for alkyl-benzenes recently published by Lawrence Livermore National Laboratory (LLNL) and National University of Ireland. Based on the strong correlation between experiments and calculations, different aspects contributing to the burning speed of the fuels (thermal effects, kinetics,...) were analyzed using the model. A sensitivity analysis was used to determine the reaction rate constants that are most important in determining the flame speed. Reaction path analysis and species profiles in the flame were used to identify the key reaction paths that lead to increase or decrease in the burning velocities. Contrary to what is generally observed for alkanes whose flame speed is controlled by small radical fragments, the flame speed of aromatics is influenced by fuel specific intermediates such as phenyl, benzyl, or even heavier species. The new experimental data and modeling insight generated by this work will support the development of models for heavier alkyl-aromatics of great relevance to diesel fuel. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Mehl, Marco; Pitz, William J.] Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. [Herbinet, Olivier; Dirrenberger, Patricia; Bounaceur, Roda; Glaude, Pierre-Alexandre; Battin-Leclerc, Frederique] Univ Lorraine, Lab React & Genie Proc, UMR CNRS 7274, F-54001 Nancy, France. RP Mehl, M (reprint author), 7000 East Ave L-288, Livermore, CA 94550 USA. EM mehl6@llnl.gov RI Mehl, Marco/A-8506-2009; OI Mehl, Marco/0000-0002-2227-5035; herbinet, olivier/0000-0002-2155-098X; Glaude, Pierre-Alexandre/0000-0001-9166-8388; BOUNACEUR, RODA/0000-0003-4077-6578 FU Saudi Aramco; U.S. Department of Energy, Office of Vehicle Technologies under U.S. Department of Energy by Lawrence Livermore National Laboratory [DE-AC52-07NA27344] FX The work performed at Universite de Lorraine-CNRS was supported by Saudi Aramco. The modeling work performed at LLNL was supported by U.S. Department of Energy, Office of Vehicle Technologies, and performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344. The authors thank the program manager Gurpreet Singh for his support. NR 26 TC 6 Z9 6 U1 3 U2 30 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 341 EP 348 DI 10.1016/j.proci.2014.06.064 PN 1 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2EN UT WOS:000348047500029 ER PT J AU Welz, O Savee, JD Osborn, DL Taatjes, CA AF Welz, Oliver Savee, John D. Osborn, David L. Taatjes, Craig A. TI Chlorine atom-initiated low-temperature oxidation of prenol and isoprenol: The effect of C=C double bonds on the peroxy radical chemistry in alcohol oxidation SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Low-temperature oxidation; Autoignition; Alcohols; Resonance stabilization; Peroxy radicals ID SET MODEL CHEMISTRY; GAS-PHASE OXIDATION; COMBUSTION CHEMISTRY; BIOFUELS PATHWAYS; CL ATOMS; KINETICS; ABSTRACTION; PARAMETERS; CL+C3H6; BUTANOL AB The chlorine atom-initiated oxidation of two unsaturated primary C5 alcohols, prenol (3-methyl-2-buten-1-ol, (CH3)(2)CCHCH2OH) and isoprenol (3-methyl-3-buten-1-ol, CH2C(CH3) CH2CH2OH), is studied at 550 K and low pressure (8 Torr). The time-and isomer-resolved formation of products is probed with multiplexed photoionization mass spectrometry (MPIMS) using tunable vacuum ultraviolet ionizing synchrotron radiation. The peroxy radical chemistry of the unsaturated alcohols appears much less rich than that of saturated C4 and C5 alcohols. The main products observed are the corresponding unsaturated aldehydes -prenal (3-methyl-2-butenal) from prenol oxidation and isoprenal (3-methyl-3-butenal) from isoprenol oxidation. No significant products arising from QOOH chemistry are observed. These results can be qualitatively explained by the formation of resonance stabilized allylic radicals via H-abstraction in the Cl + prenol and Cl + isoprenol initiation reactions. The loss of resonance stabilization upon O-2 addition causes the energies of the intermediate wells, saddle points, and products to increase relative to the energy of the initial radicals and O-2. These energetic shifts make most product channels observed in the peroxy radical chemistry of saturated alcohols inaccessible for these unsaturated alcohols. The experimental findings are underpinned by quantum-chemical calculations for stationary points on the potential energy surfaces for the reactions of the initial radicals with O-2. Under our conditions, the dominant channels in prenol and isoprenol oxidation are the chain-terminating HO2-forming channels arising from radicals, in which the unpaired electron and the -OH group are on the same carbon atom, with stable prenal and isoprenal co-products, respectively. These findings suggest that the presence of C=C double bonds in alcohols will reduce low-temperature reactivity during autoignition. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Welz, Oliver; Savee, John D.; Osborn, David L.; Taatjes, Craig A.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94550 USA. RP Welz, O (reprint author), Univ Duisburg Essen, Inst Combust & Gasdynam, Lotharstr 1, D-47057 Duisburg, Germany. EM oliver.welz@uni-due.de; cataatj@sandia.gov RI Welz, Oliver/C-1165-2013 OI Welz, Oliver/0000-0003-1978-2412 FU Division of Chemical Sciences, Geosciences, and Biosciences, the Office of Basic Energy Sciences, United States Department of Energy (U.S. DOE); U.S. DOE [DE-AC04-94AL85000]; Office of Science, Office of Basic Energy Sciences, of the U.S. DOE [DE-AC02-05CH11231] FX We thank Howard Johnsen (Sandia) and the staff at the Chemical Dynamics Beamline for technical support. This work is funded by the Division of Chemical Sciences, Geosciences, and Biosciences, the Office of Basic Energy Sciences, United States Department of Energy (U.S. DOE). Sandia is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the U.S. DOE, under contract DE-AC04-94AL85000. The Advanced Light Source is supported by the Director, Office of Science, Office of Basic Energy Sciences, of the U.S. DOE, also under contract DE-AC02-05CH11231 between Lawrence Berkeley National Laboratory and the U.S. DOE. NR 33 TC 1 Z9 1 U1 7 U2 35 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 401 EP 408 DI 10.1016/j.proci.2014.05.004 PN 1 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2EN UT WOS:000348047500036 ER PT J AU Labbe, NJ Sivaramakrishnan, R Klippenstein, SJ AF Labbe, Nicole J. Sivaramakrishnan, Raghu Klippenstein, Stephen J. TI The role of radical plus fuel-radical well-skipping reactions in ethanol and methylformate low-pressure flames SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Chemical kinetics; Ab initio; Theory; Rate constants; Biofuels ID TEMPERATURE RATE CONSTANTS; TRANSITION-STATE THEORY; THERMAL-DECOMPOSITION; AB-INITIO; METHYL FORMATE; METHANOL DECOMPOSITION; COMBUSTION CHEMISTRY; PREDICTIVE THEORY; RATE COEFFICIENTS; MASTER EQUATION AB Although the reactions of fuel-radicals with other dominant flame radicals such as H and CH3 are important reactions in low-pressure flames, they have not been well studied. These reactions may occur through either recombination to form stabilized molecular complexes or direct abstractions and chemically activated addition-eliminations to yield bimolecular products. Here, the role of such reactions in low-pressure flames of ethanol and methylformate is studied through a combination of theoretical characterizations of key reactions and detailed kinetic modeling. In particular, H and CH3 + fuel-radical reactions have been characterized theoretically in this work and these are shown to make a pronounced impact on the formation of intermediates. Theoretical calculations for H + CH3CHOH and CH3 + CH3CHOH predict that at low pressures recombinations are minor processes with well-skipping (addition-eliminations) dominating the reaction flux. Direct abstraction was also considered in H + CH3CHOH and theory suggests that abstraction at the CH3-site forming CH2CHOH is the only important channel. Notably, this result is counter to analogy based predictions that CH3CHO should be the dominant abstraction product. Low-pressure ethanol flame simulations indicate that addition-elimination reactions from H + CH3CHOH and CH3 + CH3CHOH are a major source for C2H4 and C3H6 profiles, respectively. Similar results are observed in simulations of a low-pressure methylformate flame, where addition-elimination reactions of H + CH2OCHO and CH3 + CH2OCHO have a significant impact on CH3OH and C2H4 mole fraction profiles, respectively. The present results suggest that the well-skipping reactions of relatively stable fuel-radicals with ubiquitous flame radicals such as H, O, OH, and CH3 should be considered extensively in combustion models. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Labbe, Nicole J.; Sivaramakrishnan, Raghu; Klippenstein, Stephen J.] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. RP Sivaramakrishnan, R (reprint author), Argonne Natl Lab, L-117,Bldg 200, Argonne, IL 60439 USA. EM raghu@anl.gov RI SIVARAMAKRISHNAN, RAGHU/C-3481-2008; OI SIVARAMAKRISHNAN, RAGHU/0000-0002-1867-1254; Klippenstein, Stephen/0000-0001-6297-9187 FU U. S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences [DE-AC0206CH11357] FX This work was supported by the U. S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences, under Contract No. DE-AC0206CH11357. NR 44 TC 8 Z9 8 U1 6 U2 29 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 447 EP 455 DI 10.1016/j.proci.2014.05.107 PN 1 PG 9 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2EN UT WOS:000348047500041 ER PT J AU Niu, YQ Shaddix, CR AF Niu, Yanqing Shaddix, Christopher R. TI A sophisticated model to predict ash inhibition during combustion of pulverized char particles SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Ash; Char; Coal; Combustion; Burnout ID COAL COMBUSTION; OXY-COMBUSTION; BURNOUT; CARBON; CO2 AB Final burnout of char particles from practical fuels such as coal and biomass occurs in the presence of a large ash component. Also, newly utilized coal resources, such as those from India, often contain much larger ash fractions than have traditionally been utilized. In the past, the inhibitory influence of ash on pulverized coal particle combustion has been most frequently modeled using an ash film model, though such films are rarely found when examining partially combusted particles. Conversely, some measurements have suggested that mineral components exposed on the surface of burning pulverized coal (pc) particles may diffuse back into the char matrix, the effect of which can be modeled as an ash dilution effect. To explore the implications of these different ash inhibition models on the temporal evolution of char combustion during burnout, we have developed a new computational model that considers the possibility of an ash film effect, an ash dilution effect, or some arbitrary combination of the two effects acting in tandem, which is the most realistic scenario. This new model predicts that restricted diffusion through the ash film has a significant impact on the char burnout rate throughout its lifetime, whereas char dilution only inhibits combustion significantly when most of the char has been consumed and the combustion mode shifts from predominantly external diffusion control to mixed diffusion control, with sensitivity to both external and internal diffusion resistance. The comparison of the model predictions with experimental results also confirms the previously suggested need to include gasification reaction steps when modeling coal char combustion. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Niu, Yanqing] Xi An Jiao Tong Univ, Key Lab Thermofluid Sci & Engn, Minist Educ, Xian 710049, Peoples R China. [Shaddix, Christopher R.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94550 USA. RP Niu, YQ (reprint author), Xi An Jiao Tong Univ, Key Lab Thermofluid Sci & Engn, Minist Educ, Xian 710049, Peoples R China. EM yqniu85@mail.xjtu.edu.cn OI Niu, Yanqing/0000-0001-7267-9305 FU China Postdoctoral Science Foundation [2013M532046]; National Nature Science Foundation of China [51376147]; U.S. Department of Energy (DOE) National Energy Technology Laboratory's Power Systems Advanced Research Program; U.S. DOE's National Nuclear Security Administration [DE-AC04-94AL85000] FX The present work was supported by the China Postdoctoral Science Foundation funded project (2013M532046), the National Nature Science Foundation of China (51376147) and the U.S. Department of Energy (DOE) National Energy Technology Laboratory's Power Systems Advanced Research Program. The authors gratefully acknowledge the contributions of Ethan Hecht and Manfred Geier for their assistance with laboratory experiments and FORTRAN code writing. Sandia National Laboratories is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for U.S. DOE's National Nuclear Security Administration under contract DE-AC04-94AL85000. NR 19 TC 4 Z9 5 U1 8 U2 22 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 561 EP 569 DI 10.1016/j.proci.2014.05.077 PN 1 PG 9 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2EN UT WOS:000348047500054 ER PT J AU Goldsborough, SS Johnson, MV Banyon, C Pitz, WJ McNenly, MJ AF Goldsborough, S. S. Johnson, M. V. Banyon, C. Pitz, W. J. McNenly, M. J. TI Experimental and modeling study of fuel interactions with an alkyl nitrate cetane enhancer, 2-ethyl-hexyl nitrate SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Rapid compression machine; Cetane enhancer; Alkyl nitrates; Fuel interactions ID RAPID COMPRESSION MACHINE; HIGH-PRESSURE; NITRIC-OXIDE; 2-ETHYLHEXYL NITRATE; EXTENDED TEMPERATURE; MUTUAL SENSITIZATION; BUTYL PEROXIDE; IGNITION; OXIDATION; COMBUSTION AB This study investigates the autoignition behavior of two gasoline surrogates doped with an alkyl nitrate cetane enhancer, 2-ethyl-hexyl nitrate (2EHN) to better understand dopant interactions with the fuels, including influences of accelerating kinetic pathways and enhanced exothermicity. A primary reference fuel (PRF) blend of n-heptane/iso-octane, and a toluene reference fuel (TRF) blend of n-heptane/iso-octane/toluene are used where the aromatic fraction of the latter is set to 20% (liquid volume), while the content of n-heptane is adjusted so that the overall reactivity of the undoped fuels is similar, e.g., Anti-Knock Index (AKI) of similar to 91, Cetane Number (CN) similar to 25. Doping levels of 0.1, 1.0 and 3.0% (liquid volume basis) are used where tests are conducted within a rapid compression machine (RCM) at a compressed pressure of 21 bar, covering temperatures from 675 to 1025 K with stoichiometric fuel-oxygen ratios at O-2 = 11.4%. At the experimental conditions, it is found that the doping effectiveness of 2EHN is fairly similar between the two fuels, though 2EHN is more effective in the aromatic blend at the lowest temperatures, while it is slightly more effective in the non-aromatic blend at intermediate temperatures. Kinetic modeling of the experiments indicates that although some of the reactivity trends can be captured using a detailed model, the extents of predicted Cetane Number enhancement by 2EHN are too large, while differences in fuel interactions for the two fuels result in excessive stimulation of the non-aromatic blend. Sensitivity analysis using the kinetic model indicates that the CH2O and CH3O2 chemistry are very sensitive to the dopant at all conditions. The rate of 2EHN decomposition is only important at low temperatures where its decomposition rate is slow due to the high activation energy of the reaction. At higher temperatures, dopant-derived 3-heptyl radicals are predicted to play an important role stimulating ignition. Finally, nitrogen chemistry is important through the 'NO - NO2 loop' where this can generate substantial amounts of OH. However, at the highest doping levels the formation of methyl and ethyl nitrite, and nitric acid significantly competes with this so that less OH is generated and this constrains the reactivity enhancement of 2EHN. (C) 2014 Published by Elsevier Inc. on behalf of The Combustion Institute. C1 [Goldsborough, S. S.; Johnson, M. V.; Banyon, C.] Argonne Natl Lab, Div Energy Syst, Argonne, IL 60439 USA. [Goldsborough, S. S.] Univ Illinois, Dept Mech & Ind Engn, Chicago, IL 60607 USA. [Pitz, W. J.; McNenly, M. J.] Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. RP Goldsborough, SS (reprint author), Argonne Natl Lab, Div Energy Syst, 9700 S Cass Ave, Argonne, IL 60439 USA. EM scott.goldsborough@anl.gov FU US DOE Vehicle Technology Program; Argonne, a U.S. Department of Energy Office of Science laboratory [DE-AC02-06CH11357]; US Department of Energy by Lawrence Livermore National Laboratory [DE-AC52-07NA27344] FX Timothy Smith and Steve McConnell (ANL) helped maintain and operate the RCM. Funding at ANL and LLNL for this work was provided by the US DOE Vehicle Technology Program with Gurpreet Singh as program manager. This manuscript has been created in part by UChicago Argonne, LLC, Operator of Argonne National Laboratory ("Argonne"). Argonne, a U.S. Department of Energy Office of Science laboratory, is operated under Contract No. DE-AC02-06CH11357. The LLNL work was performed under the auspices of the US Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344. The U.S. Government retains for itself, and others acting on its behalf, a paid-up non-exclusive, irrevocable worldwide license in said article to reproduce, prepare derivative works, distribute copies to the public, and perform publicly and display publicly, by or on behalf of the Government. NR 34 TC 7 Z9 7 U1 0 U2 14 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 571 EP 579 DI 10.1016/j.proci.2014.06.048 PN 1 PG 9 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2EN UT WOS:000348047500055 ER PT J AU McNenly, MJ Whitesides, RA Flowers, DL AF McNenly, Matthew J. Whitesides, Russell A. Flowers, Daniel L. TI Faster solvers for large kinetic mechanisms using adaptive preconditioners SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Chemical kinetics; Sparse matrix; Preconditioner; Ordinary differential equation ID COMBUSTION; OXIDATION; SURROGATE AB The adaptive preconditioners developed in this paper substantially reduce the computational cost of integrating large kinetic mechanisms using implicit ordinary differential equation (ODE) solvers. For a well-stirred reactor, the speedup of the new method is an order of magnitude faster than recent approaches based on direct, sparse linear system solvers. Moreover, the new method is up to three orders of magnitude faster than traditional implementations of the ODE solver where the Jacobian information is generated automatically via finite differences, and the factorization relies on standard, dense matrix operations. Unlike mechanism reduction strategies, the adaptive preconditioners do not alter the underlying system of differential equations. Consequently, the new method achieves its performance gains without any loss of accuracy to within the local error controlled by the ODE solver. Such speedup allows higher fidelity mechanism chemistry to be coupled with multi-dimensional fluid dynamics simulations. (C) 2014 Published by Elsevier Inc. on behalf of The Combustion Institute. C1 [McNenly, Matthew J.; Whitesides, Russell A.; Flowers, Daniel L.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. RP McNenly, MJ (reprint author), Lawrence Livermore Natl Lab, 7000 East Ave,Mail Code L-140, Livermore, CA 94550 USA. EM mcnenly1@llnl.gov FU Advanced Combustion Engine Team Leader for the U.S. Department of Energy Vehicle Technologies Office FX The authors gratefully acknowledge the support of Gurpreet Singh, the Advanced Combustion Engine Team Leader for the U.S. Department of Energy Vehicle Technologies Office. NR 31 TC 10 Z9 10 U1 0 U2 6 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 581 EP 587 DI 10.1016/j.proci.2014.05.113 PN 1 PG 7 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2EN UT WOS:000348047500056 ER PT J AU Yeates, DR Li, W Westmoreland, PR Speight, W Russi, T Packard, A Frenklach, M AF Yeates, Devin R. Li, Wenjun Westmoreland, Phillip R. Speight, William Russi, Trent Packard, Andrew Frenklach, Michael TI Integrated data-model analysis facilitated by an Instrumental Model SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Uncertainty quantification; Model validation; Premixed flame; Data Collaboration; Instrumental Model ID PHOTOIONIZATION CROSS-SECTIONS; COMBUSTION CHEMISTRY; MASS-SPECTROMETRY; CYCLOHEXANE FLAME AB A paradigm is described and demonstrated for rigorously evaluating model-versus-data agreement while extracting new insights for improving the model and experiment. "Bound-to-Bound Data Collaboration" (B2B-DC) is augmented with an Instrumental Model, integrating uncertainty quantification of the reactor model, chemical model, and data analysis. The subject of analysis is a fuel-lean C2H2/O-2/Ar premixed laminar flat flame, mapped with VUV-photoionization molecular-beam mass spectrometry at the Advanced Light Source of Lawrence Berkeley National Laboratory. Experimental signals were modeled with a CHEMKIN flame code augmented with an Instrumental Model. Consistency of the model and raw experimental data are determined as a quantitative measure of their agreement. Features of the mole-fraction profiles are predicted for O, OH, C2H3, and background contributions to H2O measurements. Also computed are posterior distributions of the initial targets and model parameters, as well as their correlations. This approach to model-versus-data assessment promises to advance the science and practical utility of modeling, establishing validity rigorously while identifying and ranking the impacts of specific model and data uncertainties for model and data improvements. Published by Elsevier Inc. on behalf of The Combustion Institute. C1 [Yeates, Devin R.; Speight, William; Russi, Trent; Packard, Andrew; Frenklach, Michael] Univ Calif Berkeley, Dept Mech Engn, Berkeley, CA 94720 USA. [Li, Wenjun; Westmoreland, Phillip R.] N Carolina State Univ, Dept Chem & Biomol Engn, Raleigh, NC 27695 USA. [Frenklach, Michael] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. RP Frenklach, M (reprint author), Univ Calif Berkeley, Dept Mech Engn, 6105B Etcheverry Hall, Berkeley, CA 94720 USA. EM myf@me.berkeley.edu FU NSF [CHE-0535542]; Air Force Office of Scientific Research [FA9550-08-1-0003, FA9550-10-1-0450, FA9550-12-1-0165]; Office of Energy Research, Office of Basic Energy Sciences, Chemical Sciences, Geo-sciences and Biosciences Division of the US Department of Energy [DE-AC03-76F00098] FX Research at the University of California, Berkeley was supported by the NSF Chemistry Division, Cyber-enabled Chemistry, Grant No. CHE-0535542, the Air Force Office of Scientific Research, Grant Nos. FA9550-08-1-0003, FA9550-10-1-0450, and FA9550-12-1-0165, and the Director, Office of Energy Research, Office of Basic Energy Sciences, Chemical Sciences, Geo-sciences and Biosciences Division of the US Department of Energy, under Contract No. DE-AC03-76F00098. PRW gratefully acknowledges ALS collaborators: the late T.A. Cool, N. Hansen (Sandia), K. Kohse-Hoinghaus (Bielefeld University), and the LBNL-ALS staff. The authors thank Mani Sarathy for helpful comments during preparation of the manuscript. NR 41 TC 1 Z9 1 U1 3 U2 13 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 597 EP 605 DI 10.1016/j.proci.2014.05.090 PN 1 PG 9 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2EN UT WOS:000348047500058 ER PT J AU Xin, YX Yoo, CS Chen, JH Law, CK AF Xin, Y. X. Yoo, C. S. Chen, J. H. Law, C. K. TI A DNS study of self-accelerating cylindrical hydrogen-air flames with detailed chemistry SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Cylindrical flame; Hydrogen-air flames; Self-acceleration; Hydrodynamic instability ID DARRIEUS-LANDAU INSTABILITY; DYNAMICS; PROPAGATION; SIMULATIONS; FRONTS; FLOWS AB The self-accelerating expanding cylindrical stoichiometric hydrogen-air flames at eight atmospheres were studied via two-dimensional direct numerical simulation (DNS) of the full compressible NavierStokes equations with detailed chemistry. The flame morphology and propagation were finely resolved by the application of a time step of 2.5 ns and a grid size of 4 mu m. Temporally, the intermittent propagation of the flame front is captured through examining its propagation velocity. Spatially, the flame front is found to be comprised of segments exhibiting similar propagation properties, i.e. the intermittent instantaneous propagation of the flame front is attributed to the development of cellular structures induced by hydrodynamic instability. The long-term average propagation velocity of the flame front is described by a power law, with a self-acceleration exponent of 1.22 for the flame radius with respect to time. The increase in the global flame velocity is shown to be primarily a consequence of increased flame surface area, with the local front propagation velocity remaining largely at the constant laminar flame speed for the near-unity Lewis number mixture studied herein. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Xin, Y. X.; Law, C. K.] Princeton Univ, Dept Mech & Aerosp Engn, Princeton, NJ 08544 USA. [Yoo, C. S.; Chen, J. H.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. [Law, C. K.] Tsinghua Univ, Ctr Combust Energy, Beijing 100084, Peoples R China. [Yoo, C. S.] Ulsan Natl Inst Sci & Technol, Sch Mech & Adv Mat Engn, Usn 689798, South Korea. RP Law, CK (reprint author), Princeton Univ, Dept Mech & Aerosp Engn, Princeton, NJ 08544 USA. EM cklaw@princeton.edu RI Yoo, Chun Sang/E-5900-2010 OI Yoo, Chun Sang/0000-0003-1094-4016 FU Combustion Energy Frontier Research Center, an Energy Frontier Research Center - U.S. Department of Energy, Office of Basic Energy Sciences [DE-SC0001198]; United States Department of Energy [DE-AC04- 94AL85000]; Office of Science of the US DOE [DE-AC03-76SF00098] FX The work at Princeton University and Sandia was supported by the Combustion Energy Frontier Research Center, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Basic Energy Sciences under Award Number DE-SC0001198. Sandia is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the United States Department of Energy under contract DE-AC04- 94AL85000. The authors thank Fujia Wu of Princeton University for his assistance in acquiring the experimental data reported herein. This research used resources of the National Energy Research Computing Center (NERSC) which is supported by the Office of Science of the US DOE under Contract No. DE-AC03-76SF00098. NR 26 TC 3 Z9 3 U1 2 U2 13 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 753 EP 760 DI 10.1016/j.proci.2014.06.076 PN 1 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2EN UT WOS:000348047500076 ER PT J AU Hansen, N Braun-Unkhoff, M Kathrotia, T Lucassen, A Yang, B AF Hansen, N. Braun-Unkhoff, M. Kathrotia, T. Lucassen, A. Yang, B. TI Understanding the reaction pathways in premixed flames fueled by blends of 1,3-butadiene and n-butanol SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Kinetic modeling; Mass spectrometry; Butanol; 1,3-Butadiene; Soot ID PHOTOIONIZATION MASS-SPECTROMETRY; LOW-PRESSURE FLAMES; COMBUSTION CHEMISTRY; RICH FLAMES; EMISSION CHARACTERISTICS; OXIDATION; TEMPERATURE; ISOMERS; IDENTIFICATION; PYROLYSIS AB The oxidation of 1,3-butadiene/n-butanol flames was studied in a combined experimental and modeling work. The goal is to provide a detailed combustion chemistry model that allows for identification of the important pathways for butadiene and butanol oxidation as well as the formation of soot precursors and aromatics. Therefore, the chemical composition has been investigated for three low-pressure (20-30 Torr) premixed flames, with different shares of butanol ranging between 25% and 75% compared to butadiene in 50% argon. Mole fraction profiles of reactants, products, and intermediates including C3Hx and C4Hx radicals as well as mono-aromatics such as benzyl radicals, were measured quantitatively as a function of height above burner surface employing flame-sampled molecular-beam mass spectrometry (MBMS) utilizing photoionization with tunable vacuum-ultraviolet synchrotron radiation. The comparison of measured species profiles with modeling results provides a comprehensive view of the reaction model's quality and predictive capability with respect to the combustion chemistry of 1,3-butadiene and n-butanol under the current low-pressure, high-temperature conditions. In general, a good agreement was found between experimental and modeled results. Reaction flux and sensitivity analysis were used to get more insights into the combustion of the fuels. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Hansen, N.; Lucassen, A.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. [Braun-Unkhoff, M.; Kathrotia, T.] German Aerosp Ctr DLR, Inst Combust Technol, D-70569 Stuttgart, Germany. [Yang, B.] Tsinghua Univ, Ctr Combust Energy, Beijing 100084, Peoples R China. [Yang, B.] Tsinghua Univ, Key Lab Thermal Sci & Power Engn, Minist Educ, Beijing 100084, Peoples R China. RP Hansen, N (reprint author), Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. EM nhansen@sandia.gov; marina.braun-unkhoff@dlr.de RI Hansen, Nils/G-3572-2012; Yang, Bin/A-7158-2008; Lucassen, Arnas/G-3803-2013 OI Yang, Bin/0000-0001-7333-0017; Lucassen, Arnas/0000-0003-2967-2030 FU DAAD (Deutscher Akademischer Austausch Dienst) [56025647]; U.S. Department of Energy (USDOE), Office of Basic Energy Sciences (BES) (Energy Frontier Research Center for Combustion Science) [DE-AC04-94-AL85000, DE-SC0001198]; National Science Foundation of China [51306102]; "National 1000 Young Talents Program" of China; Office of Science, BES, USDOE [DE-AC02-05CH11231]; National Nuclear Security Administration [DE-AC04-94-AL85000] FX The work is supported by the DAAD (Deutscher Akademischer Austausch Dienst) under Grant No. 56025647. NH and AL are supported by the U.S. Department of Energy (USDOE), Office of Basic Energy Sciences (BES) under Grand Nos. DE-AC04-94-AL85000 and DE-SC0001198 (the Energy Frontier Research Center for Combustion Science). BY is supported by the National Science Foundation of China (51306102) and the "National 1000 Young Talents Program" of China. MBU and TK are grateful to the assistance of S. Asenbauer, T. Brandes, and L. Cordes in the modeling work and preparing plots. The measurements were performed within the "Flame Team" collaboration at the Advanced Light Source (ALS), Lawrence Berkeley National Laboratory, Berkeley, USA, and we thank the students and postdocs for the help with the data acquisition. The experiments have profited from the expert technical assistance of Paul Fugazzi. The Advanced Light Source is supported by the Director, Office of Science, BES, USDOE under Contract No. DE-AC02-05CH11231. Sandia is a multi-program laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the National Nuclear Security Administration under contract DE-AC04-94-AL85000. NR 41 TC 7 Z9 7 U1 6 U2 39 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 771 EP 778 DI 10.1016/j.proci.2014.05.005 PN 1 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2EN UT WOS:000348047500078 ER PT J AU Felsmann, D Moshammer, K Kruger, J Lackner, A Brockhinke, A Kasper, T Bierkandt, T Akyildiz, E Hansen, N Lucassen, A Osswald, P Kohler, M Garcia, GA Nahon, L Hemberger, P Bodi, A Gerber, T Kohse-Hoinghaus, K AF Felsmann, Daniel Moshammer, Kai Krueger, Julia Lackner, Alexander Brockhinke, Andreas Kasper, Tina Bierkandt, Thomas Akyildiz, Erdal Hansen, Nils Lucassen, Arnas Osswald, Patrick Koehler, Markus Garcia, Gustavo A. Nahon, Laurent Hemberger, Patrick Bodi, Andras Gerber, Thomas Kohse-Hoeinghaus, Katharina TI Electron ionization, photoionization and photoelectron/photoion coincidence spectroscopy in mass-spectrometric investigations of a low-pressure ethylene/oxygen flame SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Molecular-beam mass spectrometry; Combustion chemistry; Electron ionization; Photoionization; PEPICO ID SYNCHROTRON-RADIATION; COMBUSTION CHEMISTRY; CROSS-SECTIONS AB Quantitative species data for the development and critical examination of combustion mechanisms are in high demand regarding the need for predictive combustion models that may assess the emission potential of current and emerging fuels. Mass spectrometric investigation is one of the often-used techniques to provide mole fractions of stable and reactive intermediates including radicals from specifically designed laboratory experiments. Molecular-beam mass spectrometry (MBMS) has been coupled with electron ionization (EI) and photoionization (PI) to determine the species compositions, and combinations of these techniques have been successful in the investigation of the combustion pathways in flames of numerous hydrocarbon, oxygenated and nitrogenated fuels. Photoelectron/photoion coincidence spectroscopy (PEPICO) has recently emerged as a novel diagnostics to be combined with flame-sampling mass spectrometry, and its potential as a complement of existing techniques is just about being explored. In a multi-laboratory investigation, the present study has thus combined four different MBMS spectrometers (in Bielefeld, Germany, the Advanced Light Source in Berkeley, USA, the Swiss Light Source in Villigen, Switzerland, and the SOLEIL synchrotron in St. Aubin, France) to study a rich premixed argon-diluted low-pressure (40 mbar) ethylene-oxygen flame under comparable conditions. This was done with the aim of illustrating the respective properties and capabilities of the methods under these conditions, with an emphasis on the power offered by the synchrotron-based techniques, including PEPICO, for combustion chemistry studies. Examples include comparisons of selected species quantification as well as PEPICO spectra measured at different instruments. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Felsmann, Daniel; Moshammer, Kai; Krueger, Julia; Lackner, Alexander; Brockhinke, Andreas; Kohse-Hoeinghaus, Katharina] Univ Bielefeld, Dept Chem, Univ Str 25, D-33615 Bielefeld, Germany. [Kasper, Tina; Bierkandt, Thomas; Akyildiz, Erdal] Univ Duisburg Essen, Mass Spectrometry React Flows Thermodynam IVG, Duisburg, Germany. [Hansen, Nils; Lucassen, Arnas] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. [Osswald, Patrick; Koehler, Markus] German Aerosp Ctr DLR, Inst Combust Technol, D-70569 Stuttgart, Germany. [Garcia, Gustavo A.; Nahon, Laurent] Synchrotron SOLEIL, F-91192 Gif Sur Yvette, France. [Hemberger, Patrick; Bodi, Andras; Gerber, Thomas] Paul Scherrer Inst, Swiss Light Source, Mol Dynam Grp, CH-5232 Villigen, Switzerland. RP Moshammer, K (reprint author), Univ Bielefeld, Dept Chem, Univ Str 25, D-33615 Bielefeld, Germany. EM kmoshammer@uni-bielefeld.de RI Hansen, Nils/G-3572-2012; Kohse-Hoinghaus, Katharina/A-3867-2012; Lucassen, Arnas/G-3803-2013; Kasper, Tina/A-2975-2017; Hemberger, Patrick/E-7909-2017; OI Lucassen, Arnas/0000-0003-2967-2030; Kasper, Tina/0000-0003-3993-5316; Hemberger, Patrick/0000-0002-1251-4549; Kohler, Markus/0000-0001-9562-8455; Gerber, Thomas/0000-0001-7027-0477; Garcia, Gustavo/0000-0003-2915-2553; Bodi, Andras/0000-0003-2742-1051 FU Deutsche Forschungsgemeinschaft within the Collaborative Research Center [SFB 686, TP B3]; Swiss Federal Office for Energy (BFE) [101969/152433]; U.S. Department of Energy (USDOE), Office of Basic Energy Sciences (BES) (Energy Frontier Research Center for Combustion Science) [DE-AC04-94-AL85000, DE-SC0001198]; Office of Science, BES, USDOE [DE-AC02-05CH11231] FX The Bielefeld team acknowledges generous partial support by Deutsche Forschungsgemeinschaft within the Collaborative Research Center SFB 686, TP B3. They wish to thank Julia Wullenkord and Harald Waterbor for their support and the general staff at SOLEIL for smoothly running the facility. Some of the experiments were carried out at the VUV beamline of the Swiss Light Source, Paul Scherrer Institute (PSI). The work was financially supported by the Swiss Federal Office for Energy (BFE Contract Number 101969/152433). A. L. and N.H. are supported by the U.S. Department of Energy (USDOE), Office of Basic Energy Sciences (BES) under Grand No. DE-AC04-94-AL85000 and DE-SC0001198 (the Energy Frontier Research Center for Combustion Science). The Advanced Light Source is supported by the Director, Office of Science, BES, USDOE under Contract No. DE-AC02-05CH11231. NR 34 TC 16 Z9 16 U1 9 U2 61 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 779 EP 786 DI 10.1016/j.proci.2014.05.151 PN 1 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2EN UT WOS:000348047500079 ER PT J AU Bierkandt, T Kasper, T Akyildiz, E Lucassen, A Osswald, P Kohler, M Hemberger, P AF Bierkandt, T. Kasper, T. Akyildiz, E. Lucassen, A. Osswald, P. Koehler, M. Hemberger, P. TI Flame structure of a low-pressure laminar premixed and lightly sooting acetylene flame and the effect of ethanol addition SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Acetylene flame structure; Ethanol addition; VUV photoionization; Threshold photoelectron spectroscopy; Soot precursors ID FUEL-RICH FLAMES; PHOTOIONIZATION MASS-SPECTROMETRY; AROMATIC-HYDROCARBONS; REACTION-MECHANISM; BENZENE FLAMES; ARGON FLAME; IDENTIFICATION; COMBUSTION; PRECURSORS; CHEMISTRY AB The flame structure of a fuel-rich (phi = 2.4), laminar premixed, and lightly sooting acetylene flame at 40 mbar and the influence of ethanol addition on the species pool was investigated. Special emphasis was put on the analysis of important soot precursors like propargyl, benzene, and the polyynes. The mole fractions of more than 50 stable and radical species up to m/z = 170 are obtained experimentally in the flames by molecular-beam mass spectrometry (MBMS) in combination with single-photon ionization (SPI) by vacuum ultraviolet (VUV) radiation from the Advanced Light Source (ALS) in Berkeley, CA, USA. For the neat acetylene flame, successful measurements were performed with a combination of MBMS and imaging photoelectron photoion coincidence spectrometry (iPEPICO) at the VUV beamline at the Swiss Light Source (SLS) in Villigen, Switzerland and adding additional species information to the data set. Some interesting isomers (C3H2, C4H5, C4H2O) can be clearly identified by comparison of measured photoionization efficiency (PIE) curves or threshold photoelectron (TPE) spectra with Franck-Condon simulations or literature spectra, respectively. Because of apparatus improvements, the chemical resolution in this study goes beyond prior work and provides a high-quality data set for the development of reaction mechanisms at fuel-rich, low-pressure conditions. (C) 2014 Published by Elsevier Inc. on behalf of The Combustion Institute. C1 [Bierkandt, T.; Kasper, T.; Akyildiz, E.] Univ Duisburg Essen, D-47048 Duisburg, Germany. [Lucassen, A.] Sandia Natl Labs, Livermore, CA USA. [Osswald, P.; Koehler, M.] German Aerosp Ctr DLR, DLR Inst Combust Technol, D-70569 Stuttgart, Germany. [Hemberger, P.] Paul Scherrer Inst, Mol Dynam Grp, CH-5232 Villigen, Switzerland. RP Kasper, T (reprint author), Lotharstr 1, D-47057 Duisburg, Germany. EM tina.kasper@uni-due.de RI Lucassen, Arnas/G-3803-2013; Kasper, Tina/A-2975-2017; Hemberger, Patrick/E-7909-2017; OI Lucassen, Arnas/0000-0003-2967-2030; Kasper, Tina/0000-0003-3993-5316; Hemberger, Patrick/0000-0002-1251-4549; Kohler, Markus/0000-0001-9562-8455 FU MIWF; Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231]; Swiss Federal Office for Energy (BFE) [101969152433]; European Community's Seventh Framework Programme (FP7) [312284]; US Department of Energy, Office of Basic Energy Sciences (BES) (Combustion Energy Frontier Research Center) [DE-SC000119] FX T.B. and T.K. are grateful for financial support from MIWF. All measurements were performed at the ALS and the SLS, respectively. The Advanced Light Source is supported by the Director, Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. The work was financially supported by the Swiss Federal Office for Energy (BFE Contract Number 101969152433). The research leading to these results has received funding from the European Community's Seventh Framework Programme (FP7/2007-2013) under Grant agreement no 312284. A.L. is supported by the US Department of Energy, Office of Basic Energy Sciences (BES) under Grand No. DE-SC0001198 (the Combustion Energy Frontier Research Center). We appreciate support and helpful discussions from Ahren Jasper, Nils Hansen, Phil Westmoreland, Katharina Kohse-Hoinghaus and all other members of the ALS and SLS flame team. NR 44 TC 6 Z9 6 U1 3 U2 26 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 803 EP 811 DI 10.1016/j.proci.2014.05.094 PN 1 PG 9 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2EN UT WOS:000348047500082 ER PT J AU Lucassen, A Park, S Hansen, N Sarathy, SM AF Lucassen, Arnas Park, Sungwoo Hansen, Nils Sarathy, S. Mani TI Combustion chemistry of alcohols: Experimental and modeled structure of a premixed 2-methylbutanol flame SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Alcohol combustion; 2-Methylbutanol; Biofuels; Mass spectrometry; Kinetic modeling ID ISO-BUTANOL; 2-METHYL-1-BUTANOL; DECOMPOSITION; MIXTURES; PATHWAYS; IGNITION; SPEEDS AB This paper presents a detailed investigation of 2-methylbutanol combustion chemistry in low-pressure premixed flames. This chemistry is of particular interest to study because this compound is potentially a lignocellulosic-based, next-generation biofuel. The detailed chemical structure of a stoichiometric low-pressure (25 Torr) flame was determined using flame-sampling molecular-beam mass spectrometry. A total of 55 species were identified and subsequently quantitative mole fraction profiles as function of distance from the burner surface were determined. In an independent effort, a detailed flame chemistry model for 2-methylbutanol was assembled based on recent knowledge gained from combustion chemistry studies for butanol isomers ([Sarathy et al. Combust. Flame 159 (6) (2012) 2028-2055]) and iso-pentanol (3-methylbutanol) [Sarathy et al. Combust. Flame 160 (12) (2013) 2712-2728]. Experimentally determined and modeled mole fraction profiles were compared to demonstrate the model's capabilities. Examples of individual mole fraction profiles are discussed together with the most significant fuel consumption pathways to highlight the combustion chemistry of 2-methylbutanol. Discrepancies between experimental and modeling results are used to suggest areas where improvement of the kinetic model would be needed. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Lucassen, Arnas; Hansen, Nils] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94550 USA. [Park, Sungwoo; Sarathy, S. Mani] King Abdullah Univ Sci & Technol, Thuwal 239556900, Saudi Arabia. RP Lucassen, A (reprint author), Sandia Natl Labs, 7011 East Ave,MS 9055, Livermore, CA 94550 USA. EM arnas.lucassen@gmail.com RI Hansen, Nils/G-3572-2012; Sarathy, S. Mani/M-5639-2015; Lucassen, Arnas/G-3803-2013; OI Sarathy, S. Mani/0000-0002-3975-6206; Lucassen, Arnas/0000-0003-2967-2030; Park, Sungwoo/0000-0002-2800-1908 FU Energy Frontier Research Center for Combustion Science [DE-SC0001198]; Clean Combustion Research Center (CCRC) at KAUST; Office of Science, Basic Energy Sciences, US Department of Energy [DE-AC02-05CH11231]; National Nuclear Security Administration [DE-AC04-94-AL85000] FX The measurements were performed within the "Flame Team" collaboration at the Advanced Light Source and we thank the students and postdocs for the help with the data acquisition. The experiments have profited from the expert technical assistance of Paul Fugazzi. A. L. and N.H. are supported by the Energy Frontier Research Center for Combustion Science (Grant No. DE-SC0001198). S.P. and S.M.S. acknowledge funding from the Clean Combustion Research Center (CCRC) at KAUST. The Advanced Light Source is supported by the Director, Office of Science, Basic Energy Sciences, US Department of Energy, under Contract No. DE-AC02-05CH11231. Sandia is a multi-program laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the National Nuclear Security Administration under contract DE-AC04-94-AL85000. NR 33 TC 10 Z9 10 U1 8 U2 38 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 813 EP 820 DI 10.1016/j.proci.2014.05.008 PN 1 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2EN UT WOS:000348047500083 ER PT J AU Demirgok, B Ugarte, O Valiev, D Akkerman, V AF Demirgok, Berk Ugarte, Orlando Valiev, Damir Akkerman, V'yacheslav TI Effect of thermal expansion on flame propagation in channels with nonslip walls SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Reacting flows; Flame acceleration; Wall friction; Flame-flow feedback; Numerical simulations ID ACCELERATION; TUBES; DETONATION; WAVES AB Propagation of premixed flames in narrow channels is investigated by means of extensive numerical simulations of a complete system of combustion and hydrodynamic equations, incorporating transport properties (thermal conduction, diffusion and viscosity) and Arrhenius chemical kinetics. The system includes mass conservation and Navier-Stokes equations as well as those for the energy and species balance. A flame propagates from the closed end of a channel to the open one. An initially planar flame front gets corrugated due to wall friction and thereby accelerates. It is shown that a flame exhibits an exponential state of acceleration only when the thermal expansion coefficient Theta exceeds a certain critical value Theta > Theta(c). The quantity Theta(c) is tabulated as a function of the Reynolds number related to the flame propagation, Re, being Theta(c) approximate to 6 for Re = 5 similar to 20. The major flame characteristics such as the flame propagation speed and acceleration rate are scrutinized. It is demonstrated that the acceleration promotes with H but weakens with Re. In this respect, the present computational results support the theoretical prediction of Bychkov et al. Physical Review E 72 (2005) 046307 in a wide range of Theta and Re. While very good quantitative and qualitative agreement between numerical and theoretical results is found for realistically large thermal expansion, Theta >= 8, agreement deteriorates with decreasing Theta. Specifically, while the theory and modeling do not quantitatively agree for Theta(c) < Theta < 8, they nevertheless demonstrate a qualitative resemblance (the exponential state of acceleration). Finally, no exponential acceleration at Theta < Theta(c) denotes that the theory completely breaks in that case, but this fits other works in the field and thereby allows reconciling various formulations on the flame acceleration. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Demirgok, Berk; Ugarte, Orlando; Akkerman, V'yacheslav] W Virginia Univ, Dept Mech & Aerosp Engn, CAFEE, Computat Fluid Dynam & Appl Multiphys Ctr CFD & A, Morgantown, WV 26506 USA. [Valiev, Damir] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94550 USA. [Valiev, Damir] Princeton Univ, Dept Mech & Aerosp Engn, Princeton, NJ 08544 USA. RP Akkerman, V (reprint author), W Virginia Univ, Dept Mech & Aerosp Engn, Morgantown, WV 26506 USA. EM Vyacheslav.Akkerman@mail.wvu.edu OI Valiev, Damir/0000-0003-4271-4717 NR 22 TC 4 Z9 4 U1 0 U2 6 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 929 EP 936 DI 10.1016/j.proci.2014.07.031 PN 1 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2EN UT WOS:000348047500097 ER PT J AU Krisman, A Hawkes, ER Talei, M Bhagatwala, A Chen, JH AF Krisman, Alex Hawkes, Evatt R. Talei, Mohsen Bhagatwala, Ankit Chen, Jacqueline H. TI Polybrachial structures in dimethyl ether edge-flames at negative temperature coefficient conditions SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Dimethyl ether; Tribrachial flame; Triple flame; Negative temperature coefficient; Autoignition ID DIRECT NUMERICAL-SIMULATION; TRIPLE FLAME; CO-FLOW; PROPAGATION; IGNITION; AIR; INHOMOGENEITIES; AUTOIGNITION; COUNTERFLOW; OXIDATION AB The structure and stabilisation mechanism of partially premixed, laminar, dimethyl ether (DME) flames are investigated using two-dimensional direct numerical simulation (DNS). The simulations are performed at a pressure of 40 atmospheres and at oxidiser temperatures of 700, 900, 1100, 1300, and 1500 K, while keeping the lift-off length approximately fixed by varying the inlet velocity. At this pressure, DME exhibits two stage ignition below approximately 1100 K and a negative temperature coefficient (NTC) regime from approximately 800-1100 K. The DNS results are investigated by considering the thermochemical structure of the flames and by applying a transport budget analysis to key chemical species. The results show a transition from a lifted flame stabilised by conduction and diffusion-assisted flame propagation to a flame stabilised by autoignition with increasing temperature. At 700 K, the flame has a classical tribrachial structure similar to freely propagating edge flames at non-autoignitive conditions. The intermediate temperature cases reveal a complex transition involving multiple heat release pathways upstream of the stabilisation point. At 900 K, the flame consists of a main-tribrachial structure and an additional upstream branch due to low temperature chemistry: this is termed a tetrabrachial flame. At 1100 and 1300 K, two upstream branches are observed in addition to the main tribrachial structure, one due to low temperature chemistry and the other due to high temperature chemistry, which initiates autoignition and stabilises the flame: these are termed pentabrachial flames. At 1500 K, the low temperature upstream branch is suppressed, so there is only one upstream branch due to high temperature chemistry which proceeds to autoignition, this flame has a tetrabrachial structure, but one which is different from that observed in the 900 K case. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Krisman, Alex; Hawkes, Evatt R.; Talei, Mohsen] Univ New S Wales, Sch Mech & Mfg Engn, Sydney, NSW 2052, Australia. [Hawkes, Evatt R.] Univ New S Wales, Sch Photovolta & Renewable Energy Engn, Sydney, NSW 2052, Australia. [Bhagatwala, Ankit; Chen, Jacqueline H.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 96551 USA. RP Krisman, A (reprint author), Univ New S Wales, Sch Mech & Mfg Engn, Sydney, NSW 2052, Australia. EM a.krisman@unsw.edu.au RI Talei, Mohsen/F-8795-2016; Hawkes, Evatt/C-5307-2012 OI Talei, Mohsen/0000-0001-5923-2461; Hawkes, Evatt/0000-0003-0539-7951 FU Australian Research Council (ARC); Combustion Energy Frontier Research Center, an Energy Frontier Research Center - US Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences [DE-SC0001198]; United States Department of Energy [DE-AC04-94AL85000] FX This work was supported by the Australian Research Council (ARC). The work at Sandia National Laboratories was supported by the Combustion Energy Frontier Research Center, an Energy Frontier Research Center funded by the US Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences under Award No. DE-SC0001198. Sandia is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the United States Department of Energy under contract DE-AC04-94AL85000. The research benefited from computational resources provided through the National Computational Merit Allocation Scheme, supported by the Australian Government. The computational facilities supporting this project included the Australian NCI National Facility, the partner share of the NCI facility provided by Intersect Australia Pty Ltd., the Peak Computing Facility of the Victorian Life Sciences Computation Initiative (VLSCI), iVEC (Western Australia), and the UNSW Faculty of Engineering. NR 33 TC 11 Z9 11 U1 3 U2 8 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 999 EP 1006 DI 10.1016/j.proci.2014.05.129 PN 1 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2EN UT WOS:000348047500105 ER PT J AU Khalil, M Lacaze, G Oefelein, JC Najm, HN AF Khalil, Mohammad Lacaze, Guilhem Oefelein, Joseph C. Najm, Habib N. TI Uncertainty quantification in LES of a turbulent bluff-body stabilized flame SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Uncertainty quantification; Large eddy simulation; Global sensitivity analysis; Turbulent combustion; Model surrogate ID LARGE-EDDY SIMULATION; POLYNOMIAL CHAOS; DIFFERENTIAL-EQUATIONS; SENSITIVITY-ANALYSIS; COMBUSTION; FLOWS; ERRORS; MODEL; JETS AB We address the forward uncertainty quantification problem in large eddy simulation (LES) of a turbulent non-premixed hydrocarbon flame, focusing on parametric uncertainty. More specifically, we examine the effect of uncertainty in the Smagorinsky coefficient and turbulent Prandtl and Schmidt numbers on specific quantities of interest. To conduct this analysis 25 LES simulations are performed, from which a surrogate model is built, based on polynomial chaos expansion, for the quantities of interest. This enables global sensitivity analysis and forward propagation of uncertainty, providing marginal and joint distributions on the quantities of interest. A non-intrusive method is used to construct the surrogate models, avoiding the need to modify the deterministic LES forward solver. The accuracy of the surrogates is examined using global error measures. The results provide insights into the underlying structure of the LES simulation, the impact of varying parameters on specific observables, and correlations among different quantities of interest. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Khalil, Mohammad; Lacaze, Guilhem; Oefelein, Joseph C.; Najm, Habib N.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. RP Khalil, M (reprint author), Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. EM mkhalil@sandia.gov FU US Department of Energy (DOE), Office of Basic Energy Sciences (BES) Division of Chemical Sciences, Geosciences, and Biosciences; United States Department of Energy [DE-AC04 94-AL85000] FX This work was supported by the US Department of Energy (DOE), Office of Basic Energy Sciences (BES) Division of Chemical Sciences, Geosciences, and Biosciences. Sandia National Laboratories is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the United States Department of Energy under contract DE-AC04 94-AL85000. NR 45 TC 1 Z9 1 U1 4 U2 10 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 1147 EP 1156 DI 10.1016/j.proci.2014.05.030 PN 2 PG 10 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2FA UT WOS:000348048800003 ER PT J AU Bhagatwala, A Luo, ZY Shen, H Sutton, JA Lu, TF Chen, JH AF Bhagatwala, Ankit Luo, Zhaoyu Shen, Han Sutton, Jeffrey A. Lu, Tianfeng Chen, Jacqueline H. TI Numerical and experimental investigation of turbulent DME jet flames SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE DNS; Multi-scalar PLIF imaging; Non-premixed; DME; Extinction-reignition ID PREMIXED FLAMES; METHANE; SIMULATIONS; MECHANISMS; REDUCTION AB Results are presented here from a three-dimensional direct numerical simulation of a temporally-evolving planar slot jet flame and experimental measurements within a spatially-evolving axisymmetric jet flame operating with DME (dimethyl ether, CH3OCH3) as the fuel. Both simulation and experiment are conducted at a Reynolds number of 13050. The Damkohler number, stoichiometric mixture fraction and fuel and oxidizer compositions also are matched between simulation and experiment. Simultaneous OH/CH2O PLIF imaging is performed experimentally to characterize the spatial structure of the turbulent DME flames. The simulation shows a fully burning flame initially, which undergoes partial extinction and subsequently, reignition. The scalar dissipation rate (chi) increases to a value much greater than that calculated from near-extinction strained laminar flames, leading to the observed local extinction. As the turbulence decays, the local values of chi decrease and the flame reignites. The reignition process appears to be strongly dependent on the local chi value, which is consistent with previous results for simpler fuels. Statistics of OH and CH2O are compared between simulation and experiment and found to agree. The applicability of OH/CH2O (formaldehyde) product imaging as a surrogate for peak heat release rate is investigated. The concentration product is found to predict peak heat release rate extremely well in the simulation data. When this product imaging is applied to the experimental data, a similar extinction/reignition pattern also is observed in the experiments as a function of axial position. A new 30-species reduced chemical mechanism for DME was also developed as part of this work. Published by Elsevier Inc. on behalf of The Combustion Institute. C1 [Bhagatwala, Ankit; Chen, Jacqueline H.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94550 USA. [Luo, Zhaoyu; Lu, Tianfeng] Univ Connecticut, Dept Mech Engn, Storrs, CT 06269 USA. [Shen, Han; Sutton, Jeffrey A.] Ohio State Univ, Dept Mech & Aerosp Engn, Columbus, OH 43210 USA. RP Bhagatwala, A (reprint author), Sandia Natl Labs, Combust Res Facil, Livermore, CA 94550 USA. EM abhagat@sandia.gov RI Lu, Tianfeng/D-7455-2014 OI Lu, Tianfeng/0000-0001-7536-1976 FU Combustion Energy Frontier Research Center (CEFRC), an Energy Frontier Research Center - U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences (BES) [DE-SC0001198]; United States Department of Energy [DE-AC04-94AL85000]; Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy [DE-SC0008622] FX The research at Sandia and Ohio State is supported by the Combustion Energy Frontier Research Center (CEFRC), an Energy Frontier Research Center funded by the U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences (BES) under Award No. DE-SC0001198. Sandia is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the United States Department of Energy under Contract DE-AC04-94AL85000. The work at University of Connecticut was supported by the Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy under Grant DE-SC0008622. Computer allocations were awarded by the Department of Energy's INCITE award at the Oak Ridge Leadership Computing Facility (OLCF) at the Oak Ridge National Laboratories (ORNL). NR 20 TC 20 Z9 20 U1 8 U2 22 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 1157 EP 1166 DI 10.1016/j.proci.2014.05.147 PN 2 PG 10 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2FA UT WOS:000348048800004 ER PT J AU Fuest, F Magnotti, G Barlow, RS Sutton, JA AF Fuest, F. Magnotti, G. Barlow, R. S. Sutton, J. A. TI Scalar structure of turbulent partially-premixed dimethyl ether/air jet flames SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Dimethyl ether; Partially-premixed; Turbulent flames; 1D Raman scattering; Model validation ID COMBUSTION; DIAGNOSTICS; DISSIPATION; TRANSPORT; LAMINAR AB This work presents results of temperature and major species measurements from two turbulent piloted, partially-premixed dimethyl ether (DME)/air jet flames with Reynolds numbers of 29,300 and 58,600. These results are intended to provide a first set of multi-scalar data from a new flame series for the investigation of turbulence-chemistry interaction and the validation of turbulent combustion models using a complex, oxygenated fuel, DME. The current work investigates two Reynolds number cases from the complete DME flame series (five flames) that were formulated to be similar to the well-known Sydney/Sandia piloted jet burner flame series A-F using methane fuels. The flame structure is examined using ensemble mean and rms radial profiles at various axial positions downstream of the nozzle exit as well as statistics conditioned on mixture fraction. Finally, selected results of the two cases are compared to the original methane-based configurations. Finite-rate chemistry effects such as local extinction and re-ignition and their impact on the scalar flame structure are found to be different in the DME/air jet flames as compared to the methane-based jet flames. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Fuest, F.; Sutton, J. A.] Ohio State Univ, Dept Mech & Aerosp Engn, Columbus, OH 43210 USA. [Magnotti, G.; Barlow, R. S.] Sandia Natl Labs, Livermore, CA USA. RP Fuest, F (reprint author), Ohio State Univ, Dept Mech & Aerosp Engn, 201 W 19th Ave, Columbus, OH 43210 USA. EM fuest.1@osu.edu FU Combustion Energy Frontier Research Center - US Department of Energy, Office of Science, BES [DE-SC0001198]; Division of Chemical Sciences, Geosciences and Biosciences, Office of Basic Energy Sciences, US Department of Energy; United States Department of Energy [DE-AC04-94-AL85000] FX Work at Ohio State University was supported by the Combustion Energy Frontier Research Center funded by the US Department of Energy, Office of Science, BES under Award DE-SC0001198. Work performed at Sandia was supported by the Division of Chemical Sciences, Geosciences and Biosciences, Office of Basic Energy Sciences, US Department of Energy. Sandia National Laboratories is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the United States Department of Energy under contract DE-AC04-94-AL85000. The help of R. Harmon during the experiments is gratefully acknowledged. NR 24 TC 4 Z9 4 U1 5 U2 19 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 1235 EP 1242 DI 10.1016/j.proci.2014.07.062 PN 2 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2FA UT WOS:000348048800013 ER PT J AU Coriton, B Frank, JH AF Coriton, Bruno Frank, Jonathan H. TI High-speed tomographic PIV measurements of strain rate intermittency and clustering in turbulent partially-premixed jet flames SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Tomographic PIV; Turbulent flames; Strain rate; Intermittency ID FLOWS; VORTICITY; GRADIENT AB The effects of combustion on the strain rate field in turbulent jets were studied using 10 kHz tomographic particle image velocimetry (TPIV). Measurements were performed in three turbulent jets: a wellstudied, piloted partially-premixed methane/ air jet flame, Sandia flame C, with low probability of localized extinction; a second piloted jet flame, analogous to flame C but with a reduced pilot flow rate and a high probability of localized extinction; and a non-reacting air jet. Since the jet exit Reynolds number of approximately 13000 was nearly identical in the three jets, differences in the strain rate fields were attributed to the effects of combustion. Spatiotemporal characteristics of the strain rate field were analyzed. Overall, the strain rate norm was larger in the flames than in the non-reacting jet with the most stable flame having the largest values. In all three jets, the compressive strain rate was on average the largest of the three principal strain rates. At high strain rates, the ratios of the compressive and extensive strain rate to the intermediate strain rate were similar to those found in isotropic incompressible turbulent flows. The three-dimensional velocity measurements were used to analyze the spatial distribution of strain rate clusters, defined as singly-connected groups of voxels where the strain rate magnitude exceeded a threshold value. The presence of a stable flame significantly attenuated the number of clusters of intermediate strain rate. Strain rate bursts, corresponding to sudden increases in the number of clusters, were identified in the three jets. Bursts in the non-reacting jet and the unstable flame contained up to twice as many clusters as in the stable flame. The temporal intermittency of intense strain rate clusters was analyzed using the time-series measurements. Clusters with strain rates greater than five times the standard deviation of the strain rate norm were highly intermittent. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Coriton, Bruno; Frank, Jonathan H.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. RP Frank, JH (reprint author), POB 969,MS 9051, Livermore, CA 94551 USA. EM jhfrank@sandia.gov FU U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences; U.S. Department of Energy [DE-AC04-94-AL85000] FX The authors thank Mr. Erxiong Haung for technical assistance in the laboratory. This research was supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences. Sandia National Laboratories is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the U.S. Department of Energy under contract DE-AC04-94-AL85000. NR 18 TC 3 Z9 3 U1 1 U2 7 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 1243 EP 1250 DI 10.1016/j.proci.2014.06.045 PN 2 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2FA UT WOS:000348048800014 ER PT J AU Coriton, B Zendehdel, M Ukai, S Kronenburg, A Stein, OT Im, SK Gamba, M Frank, JH AF Coriton, Bruno Zendehdel, Masoomeh Ukai, Satoshi Kronenburg, Andreas Stein, Oliver T. Im, Seong-Kyun Gamba, Mirko Frank, Jonathan H. TI Imaging measurements and LES-CMC modeling of a partially-premixed turbulent dimethyl ether/air jet flame SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE DME; Turbulent jet flames; PIV; LES-CMC; TNF workshop ID CONDITIONAL MOMENT CLOSURE; LARGE-EDDY SIMULATIONS; DIFFUSION FLAME; COMBUSTION; EXTINCTION; FUEL; DME AB Turbulent dimethyl ether (DME) jet flames provide a canonical flame geometry for studying turbulence-flame interactions in oxygenated fuels and for developing predictive models of these interactions. The development of accurate models for DME/air flames would establish a foundation for studies of more complex oxygenated fuels. We present a joint experimental and computational investigation of the velocity field and OH and CH2O distributions in a piloted, partially-premixed turbulent DME/air jet flame with a jet exit Reynolds number, Re-D, of 29,300. The turbulent DME/air flame is analogous to the well-studied, partially-premixed methane/air jet flame, Sandia Flame D, with identical stoichiometric mixture fraction, xi(st) = 0.35, and bulk jet exit velocity, V-bulk = 45.9 m/s. Measurements include particle image velocimetry (PIV) and simultaneous CH2O and OH laser-induced fluorescence (LIF) imaging. Simulations are performed using a large eddy simulation combined with conditional moment closure (LES-CMC) on an intermediate size grid of 1.3 million cells. Overall, the downstream evolution of the mean and RMS profiles of velocity, OH, and CH2O are well predicted, with the largest discrepancies occurring for CH2O at x/D = 20-25. LES-CMC simulations employing two different chemical reaction mechanisms (Kaiser et al., 2000 [20] and Zhao et al., 2008 [21]) show approximately a factor of two difference in the peak CH2O mole fractions, whereas OH mole fractions are in good agreement between the two mechanisms. The single-shot LIF measurements of OH and CH2O show a wide range of separation distances between the spatial distributions of these intermediate species with gaps on the order of millimeters. The intermittency in the overlap between these species indicates that the consumption rates of formaldehyde by OH in the turbulent DME/air jet flame may be highly intermittent with significant departures from flamelet models. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Coriton, Bruno; Frank, Jonathan H.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. [Zendehdel, Masoomeh; Ukai, Satoshi; Kronenburg, Andreas; Stein, Oliver T.] Univ Stuttgart, Inst Tech Verbrennung, D-70174 Stuttgart, Germany. [Im, Seong-Kyun; Gamba, Mirko] Stanford Univ, Dept Mech Engn, Stanford, CA 94305 USA. RP Frank, JH (reprint author), POB 969,MS 9051, Livermore, CA 94551 USA. EM jhfrank@sandia.gov RI Stein, Oliver/F-2933-2011; Kronenburg, Andreas/F-5567-2017 OI Kronenburg, Andreas/0000-0002-7967-9567 FU U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences; U.S. Department of Energy [DE-AC04-94-AL85000]; DFG [KR3648/1-2]; Department of Energy [DE-FC52-08NA28614] FX The authors thank M.G. Mungal for contributions to the experiments, W.P. Jones for providing the original CFD routines, and E. Huang for technical assistance in the laboratory. The experimental research was supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences. Sandia National Laboratories is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the U.S. Department of Energy under contract DE-AC04-94-AL85000. The Stuttgart group acknowledges the financial support of DFG (grant no. KR3648/1-2), high-performance computing access to HLRS. S.K. Im and M. Gamba were supported by the Department of Energy under Award Number DE-FC52-08NA28614. NR 27 TC 5 Z9 5 U1 7 U2 22 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 1251 EP 1258 DI 10.1016/j.proci.2014.06.042 PN 2 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2FA UT WOS:000348048800015 ER PT J AU Steinberg, AM Coriton, B Frank, JH AF Steinberg, A. M. Coriton, B. Frank, J. H. TI Influence of combustion on principal strain-rate transport in turbulent premixed flames SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Turbulent premixed flames; Strain-rate; High-repetition-rate laser diagnostics; Tomographic PIV; PLIF ID HOMOGENEOUS TURBULENCE; PIV MEASUREMENTS; TOMOGRAPHIC PIV; HEAT RELEASE; OH PLIF; VORTICITY; FLOWS; DYNAMICS AB The transport of principal strain-rates (si) was experimentally investigated using high-repetition-rate (10 kHz) tomographic particle image velocimetry (T-PIV) and OH planar laser induced fluorescence (PLIF) in a Re-j = 13; 000 turbulent premixed flame. These measurements allowed calculation of the source terms in the s(i) transport equation associated with the strain-rate and vorticity fields. Furthermore, the Lagrangian derivatives of s(i) could be calculated by tracking theoretical Lagrangian fluid particles through space and time using the T-PIV data. These Lagrangian derivatives and the resolved source terms allowed the combined effects of the unresolved source terms to be inferred, namely the pressure Hessian, viscous dissipation, density gradients, and viscosity gradients. Statistics conditioned on the location of the Lagrangian fluid particles relative to the flame showed slight reductions in the strain-rate and vorticity source terms in the flame, indicating that these aspects of the turbulence were attenuated by the flame. Comparing the difference between the inferred source terms in the vicinity of the flame to the non-reacting flow showed that attenuation of s(i) arose due to the combined effects of density and pressure gradients in the flame. The effects of flame-induced dilatation were small relative to the turbulent strain-rate and no change was found in the relative alignment of vorticity and strain-rate in the flame. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Steinberg, A. M.] Univ Toronto, Inst Aerosp Studies, Toronto, ON, Canada. [Coriton, B.; Frank, J. H.] Sandia Natl Labs, Combust Res Facil, Livermore, CA USA. RP Steinberg, AM (reprint author), Univ Toronto, Inst Aerosp Studies, Toronto, ON, Canada. EM steinberg@utias.utoroto.ca RI Steinberg, Adam/H-5104-2011 OI Steinberg, Adam/0000-0001-6571-6673 FU US Air Force Office of Scientific Research [FA9550-13-1-0070]; NSERC [RGPIN 413232]; U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences; US Department of Energy [DE-AC04-94-AL85000] FX A. Steinberg acknowledges the support of the US Air Force Office of Scientific Research under Grant No. FA9550-13-1-0070, Project Monitor Dr. Chiping Li, and NSERC under Grant No. RGPIN 413232. The authors acknowledge the support of the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences. Sandia National Laboratories is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the US Department of Energy under contract DE-AC04-94-AL85000. The technical support of Mr. Erxiong Huang also was greatly appreciated. NR 23 TC 7 Z9 7 U1 2 U2 10 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 1287 EP 1294 DI 10.1016/j.proci.2014.06.089 PN 2 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2FA UT WOS:000348048800019 ER PT J AU Amato, A Day, M Cheng, RK Bell, J Lieuwen, T AF Amato, A. Day, M. Cheng, R. K. Bell, J. Lieuwen, T. TI Leading edge statistics of turbulent, lean, H-2-air flames SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Premixed flames; Turbulent combustion; Leading points; Flame stretch ID DIRECT NUMERICAL-SIMULATION; METHANE-AIR FLAMES; BURNING VELOCITY; LEWIS NUMBER; COMBUSTION; PROPAGATION; PRESSURE; SPEED; FLOW AB Several studies have utilized leading points concepts to explain the sensitivity of turbulent burning rates to fuel/oxidizer composition, especially in negative Markstein length mixtures. Leading point theories suggest that the premixed turbulent flame speed is controlled by the flame front characteristics at the flame brush leading edge, or, in other words, by the flamelets that advance farthest into the unburned mixture (the so-called leading points). Furthermore, several authors have postulated that these leading edge flamelets have an inner structure similar to a critically perturbed laminar flame, i.e., the local stretch rate approaches the extinction value, near where the maximum possible laminar burning velocity is reached. In order to investigate these hypotheses for leading points burning rates, this paper analyzes the flame front structure at the leading edge of turbulent, lean (phi = 0.31) premixed H-2/Air flames, utilizing a database of direct numerical simulations (DNS) previously reported by Aspden et al. (2011). We calculate local flame front curvature, thickness, and burning velocity and compare these values to reference quantities obtained from stretched laminar flames computed numerically in different geometrical configurations (a counterflow twin flame, a tubular counterflow flame and an expanding cylindrical flame). These comparisons show that curvatures and burning velocities approach those of "critically" stretched laminar flames for the highest turbulent intensity case, but not for the lower turbulence intensity cases. In all cases, however, the structure of the flame front at the leading edge seems to closely mirror laminar flame calculations. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Amato, A.; Lieuwen, T.] Georgia Inst Technol, Sch Aerosp & Mech Engn, Atlanta, GA 30332 USA. [Day, M.; Bell, J.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Ctr Computat Sci & Engn, Berkeley, CA 94720 USA. [Cheng, R. K.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Amato, A (reprint author), Ben T Zinn Combust Lab, 635 Strong St, Atlanta, GA 30318 USA. EM alberto.amato@gatech.edu FU University Turbine Systems Research program [DE-FC21-92MC29061]; Air Force Office of Scientific Research [FA9550-12-1-0107/RC657] FX This research was supported by the University Turbine Systems Research (contract #DE-FC21-92MC29061) program and the Air Force Office of Scientific Research (contract #FA9550-12-1-0107/RC657), contract monitors are Dr. Mark Freeman and Dr. Chiping Lee, respectively. The authors gratefully acknowledge the help of Prof. C.J. Sung in making available the modified OPPDIF code used to simulate the counterflow tubular flame geometry. NR 32 TC 3 Z9 3 U1 1 U2 11 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 1313 EP 1320 DI 10.1016/j.proci.2014.05.143 PN 2 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2FA UT WOS:000348048800022 ER PT J AU Aspden, AJ Day, MS Bell, JB AF Aspden, A. J. Day, M. S. Bell, J. B. TI Turbulence-chemistry interaction in lean premixed hydrogen combustion SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Turbulent combustion; Premixed hydrogen flames; Low Mach number combustion ID OXYGEN-NITROGEN MIXTURES; NUMERICAL-SIMULATION; COMPLEX CHEMISTRY; FLAMES; FLOWS AB This paper presents three-dimensional direct numerical simulations of lean premixed hydrogen flames at an equivalence ratio of phi = 0.4 over a range of turbulence levels from Ka = 1-36. The simulations form part of a larger effort to construct a DNS database that can be used by the community for model construction and validation. We have focussed on producing well-resolved simulations at conditions representative of atmospheric laboratory-scale flames. After an overview of phenomenological trends with increasing Karlovitz number, we examine the factors that lead to an observed decorrelation between fuel consumption and heat release in the flame at Ka = 36. We show that in this flame the fuel consumption is greatly enhanced in regions of positive curvature. We also show that the radical pool is enriched throughout the entire flame as Ka is increased. In particular, we identify three reactions that, driven by high molar concentrations of radicals at low temperatures, are responsible for high levels of heat release away from regions of fuel consumption, thereby accounting for the observed decorrelation between fuel consumption and heat release. (C) 2014 Published by Elsevier Inc. on behalf of The Combustion Institute. C1 [Aspden, A. J.] Cranfield Univ, Ctr Fluid Mech & Sci Comp, Cranfield MK43 0AL, Beds, England. [Aspden, A. J.; Day, M. S.; Bell, J. B.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Ctr Computat Sci & Engn, Berkeley, CA 94720 USA. RP Aspden, AJ (reprint author), Univ Southampton, Dept Math, Bldg 54, Southampton SO17 1BJ, Hants, England. EM a.j.aspden@soton.ac.uk RI Aspden, Andy/A-7391-2017 OI Aspden, Andy/0000-0002-2970-4824 FU DOE Applied Mathematics Research Program of the DOE Office of Advanced Scientific Computing Research under the U.S. Department of Energy [DE-AC02-05CH11231] FX This work was supported by the DOE Applied Mathematics Research Program of the DOE Office of Advanced Scientific Computing Research under the U.S. Department of Energy Contract No. DE-AC02-05CH11231. NR 13 TC 16 Z9 16 U1 1 U2 18 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 1321 EP 1329 DI 10.1016/j.proci.2014.08.012 PN 2 PG 9 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2FA UT WOS:000348048800023 ER PT J AU Griffiths, RAC Chen, JH Kolla, H Cant, RS Kollmann, W AF Griffiths, R. A. C. Chen, J. H. Kolla, H. Cant, R. S. Kollmann, W. TI Three-dimensional topology of turbulent premixed flame interaction SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Turbulent premixed flame; DNS; Flame structure; Flame topology ID COMBUSTION; SIMULATION; SURFACE; JET AB The topology of turbulent premixed flames is analysed using data from Direct Numerical Simulation (DNS), with emphasis on the statistical geometry of flame-flame interaction. A general method for obtaining the critical points of line, surface and volume fields is outlined, and the method is applied to isosurfaces of reaction progress variable in a DNS configuration involving a pair of freely-propagating hydrogen-air flames in a field of intense shear-generated turbulence. A complete set of possible flame-interaction topologies is derived using the eigenvalues of the scalar Hessian, and the topologies are parametrised using a pair of shape factors. The frequency of occurrence of each type of topology is evaluated from the DNS dataset for two different Damkohler numbers. Different types of flame-interaction topology are found to be favoured in various regions of the turbulent flame, and the physical significance of each interaction is discussed. (C) 2014 Published by Elsevier Inc. on behalf of The Combustion Institute. C1 [Chen, J. H.; Kolla, H.] Sandia Natl Labs, CRF, Livermore, CA 94550 USA. [Griffiths, R. A. C.; Cant, R. S.] Univ Cambridge, Dept Engn, Cambridge CB2 1TN, England. [Griffiths, R. A. C.; Kollmann, W.] Univ Calif Davis, MAE Dept, Davis, CA 95616 USA. RP Griffiths, RAC (reprint author), Univ Cambridge, Dept Engn, Cambridge CB2 1TN, England. EM racg3@cam.ac.uk FU Erasmus Mundus Programme of the European Commission under the Transatlantic Partnership for Excellence in Engineering TEE Project; office of Science of the US Department of Energy [DE- AC05-00OR22725]; Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences of the US Department of Energy; US Department of Energy SciDAC Program FX This paper has been developed as a result of a mobility stay funded by the Erasmus Mundus Programme of the European Commission under the Transatlantic Partnership for Excellence in Engineering TEE Project.; This research used resources of the National Center for Computational Sciences at Oak Ridge National Laboratory, which is supported by the office of Science of the US Department of Energy under contract DE- AC05-00OR22725. The work at Sandia National Laboratories was supported by the Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences of the US Department of Energy and by the US Department of Energy SciDAC Program. NR 30 TC 3 Z9 3 U1 2 U2 9 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 1341 EP 1348 DI 10.1016/j.proci.2014.08.003 PN 2 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2FA UT WOS:000348048800025 ER PT J AU Ansari, N Strakey, PA Goldin, GM Givi, P AF Ansari, N. Strakey, P. A. Goldin, G. M. Givi, P. TI Filtered density function simulation of a realistic swirled combustor SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Large eddy simulation; Filter density function; Turbulent combustion; Monte Carlo methods ID LARGE-EDDY SIMULATION; TURBULENT REACTING FLOWS; FLAME; MODEL AB The scalar filtered mass density function (SFMDF) methodology is employed for large eddy simulation (LES) of the PRECCINSTA burner from DLR. This burner involves a swirling flow configuration and provides a good model of the combustor in gas turbines. In SFMDF, the effects of unresolved scalar fluctuations are taken into account by considering the probability density function of subgrid scale scalar quantities. The modeled SFMDF transport equation is solved numerically via a Lagrangian Monte Carlo scheme coupled with a finite volume flow solver on unstructured grids. The simulated results are assessed via comparison with experimental data and show reasonable agreements. This demonstrates the capability of SFMDF for LES of complex flows, and warrants future applications of the methodology for LES of practical combustor configurations. This work represents one of the first attempts in implementing FDF for LES of a practical gas turbine combustor. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Ansari, N.; Givi, P.] Univ Pittsburgh, Dept Mech Engn & Mat Sci, Pittsburgh, PA 15261 USA. [Strakey, P. A.] Natl Energy Technol Lab, Morgantown, WV 26507 USA. [Ansari, N.; Goldin, G. M.] ANSYS Inc, Canonsburg, PA 15317 USA. RP Ansari, N (reprint author), Univ Pittsburgh, 636 Benedum Hall, Pittsburgh, PA 15261 USA. EM naa56@pitt.edu FU AFOSR [FA9550-12-1-0057]; NSF [CBET-1250171]; NSF Extreme Science and Engineering Discovery Environment (XSEDE) [TG-CTS070055N, TG-CTS120015] FX We are indebted to Dr. Laurent Y.M. Gicquel of CERFACS (Toulouse, France) for his valuable comments and suggestions through the course of this research. We are also grateful to DLR for providing the experimental data on the PRECC-INSTA burner. The work at the University of Pittsburgh is sponsored by AFOSR under Grant FA9550-12-1-0057, by NSF under Grant CBET-1250171, and by the NSF Extreme Science and Engineering Discovery Environment (XSEDE) under Grants TG-CTS070055N & TG-CTS120015. We are thankful to members of the Center for Simulation and Modeling at the University of Pittsburgh for their help with numerous computational issues. NR 42 TC 1 Z9 1 U1 3 U2 11 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 1433 EP 1442 DI 10.1016/j.proci.2014.05.042 PN 2 PG 10 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2FA UT WOS:000348048800036 ER PT J AU Meares, S Prasad, VN Magnotti, G Barlow, RS Masri, AR AF Meares, S. Prasad, V. N. Magnotti, G. Barlow, R. S. Masri, A. R. TI Stabilization of piloted turbulent flames with inhomogeneous inlets SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Turbulent combustion; Inhomogeneous boundary conditions; Flame stabilization ID DISSIPATION; IGNITION; BURNER; FIELD; LES AB This paper investigates the stabilization mechanism of turbulent jet flames with highly inhomogeneous inlet conditions. A modification of the standard piloted burner is employed here with the addition of a central tube (inner) carrying fuel that can slide within the existing (outer) tube carrying air. Both tubes are located within the pilot annulus and inhomogeneity is varied by translating the inner tube upstream of the jet exit plane. Two flames with identical overall air/fuel ratios, bulk jet velocities, and pilot conditions but different levels of homogeneity in the fuel/air mixture are selected for detailed investigations. Measurements are performed using Sandia's Raman-Rayleigh-LIF line facility, and Large Eddy Simulation (LES) using the stochastic fields approach are also conducted for the same flames. Results reported here focus on the early stabilization region. The flame with inhomogeneous inlet conditions is more stable being at 57% of blow-off compared to the homogeneous counterpart, which is at 78% of blow-off. It is found that, very close to the jet exit plane, premixed combustion dominates the flame with an inhomogeneous profile. This is in contrast to the homogeneous case, which behaves like a diffusion flame. Further downstream, but still within the pilot region, partial mixing starts to occur between richer samples and hot combustion products. A comparison of the relative conditional scalar dissipation rates, chi(r) shows that in the upstream region, and within the reactive limits, the homogeneous case has higher values of chi(r). Premixed combustion with higher rates of heat release and lower scalar dissipation rates in the near field are therefore key reasons for the improved stability of the flames with inhomogeneous inlets. These findings are corroborated by results from LES. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Meares, S.; Prasad, V. N.; Masri, A. R.] Univ Sydney, Sch Aerosp Mech & Mechatron Engn, Sydney, NSW 2006, Australia. [Magnotti, G.; Barlow, R. S.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94550 USA. RP Meares, S (reprint author), Univ Sydney, Sch Aerosp Mech & Mechatron Engn, Sydney, NSW 2006, Australia. EM shaun.meares@sydney.edu.au FU Australian Research Council; Division of Chemical Sciences, Geosciences and Biosciences, Office of Basic Energy Sciences, US Department of Energy; United States Department of Energy [DE-AC04-94-AL85000] FX This work is supported by the Australian Research Council. Work at Sandia was supported by the Division of Chemical Sciences, Geosciences and Biosciences, Office of Basic Energy Sciences, US Department of Energy. Sandia National Laboratories is a multi-program laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the United States Department of Energy under contract DE-AC04-94-AL85000. Contributions by Bob Harmon and Dr Mrinal Juddoo in these experiments are highly appreciated. The authors would like to thank Prof. W.P. Jones for providing the original CFD subroutines. NR 23 TC 14 Z9 14 U1 2 U2 9 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 1477 EP 1484 DI 10.1016/j.proci.2014.05.071 PN 2 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2FA UT WOS:000348048800041 ER PT J AU Gruber, A Kerstein, AR Valiev, D Law, CK Kolla, H Chen, JH AF Gruber, A. Kerstein, A. R. Valiev, D. Law, C. K. Kolla, H. Chen, J. H. TI Modeling of mean flame shape during premixed flame flashback in turbulent boundary layers SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Turbulent channel flow; Flame shape model; Turbulent premixed flame; Flame propagation ID DIRECT NUMERICAL-SIMULATION; WALL INTERACTION; BURNER FLAMES; CHANNEL FLOW; COMBUSTION; HYDROGEN; LAMINAR AB Direct numerical simulations of freely-propagating premixed flames in the turbulent boundary layer of fully-developed turbulent channel flows are used for a priori validation of a new model that aims to describe the mean shape of the turbulent flame brush during flashback. Comparison with the DNS datasets, for both fuel-lean and fuel-rich mixture conditions and for Damkohler numbers lower and larger than unity, shows that the model is able to capture the main features of the flame shape. Although further a priori and a posteriori validation is required, particularly at higher Reynolds numbers, this new simple model seems promising and can potentially have impact on the design process of industrial combustion equipment. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Gruber, A.; Kerstein, A. R.] SINTEF Energy Res, Trondheim, Norway. [Valiev, D.; Law, C. K.] Princeton Univ, Princeton, NJ 08544 USA. [Valiev, D.; Kolla, H.; Chen, J. H.] Sandia Natl Labs, Combust Res Facil, Livermore, CA USA. RP Gruber, A (reprint author), SINTEF Energy Res, Trondheim, Norway. EM andrea.gruber@sintef.no OI Valiev, Damir/0000-0003-4271-4717 FU Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences of the US Department of Energy (DOE); US DOE [DE-AC04-94AL85000]; Combustion Energy Frontier Research Center (CEFRC); Energy Frontier Research Center - US DOE, Office of Science, Office of Basic Energy Sciences (BES) [DESC0001198]; Office of Science of the US DOE [DE-AC05-00OR22725]; BIGCCS Centre FX The work at Sandia National Laboratories (SNL) was supported by the Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences of the US Department of Energy (DOE). SNL is a multiprogramme laboratory operated by Sandia Corporation, a Lockheed Martin Company for the US DOE under Contract DE-AC04-94AL85000. Part of the work was supported by the Combustion Energy Frontier Research Center (CEFRC), an Energy Frontier Research Center funded by the US DOE, Office of Science, Office of Basic Energy Sciences (BES) under Award No. DESC0001198. This research used resources of the Oak Ridge Leadership Computing Facility at the Oak Ridge National Laboratory, which is supported by the Office of Science of the US DOE under Contract No. DE-AC05-00OR22725. Finally, this publication has been produced with support from the BIGCCS Centre, performed under the Norwegian research program Centres for Environment-friendly Energy Research (FME). The authors acknowledge the following partners for their contributions: ConocoPhillips, Gassco, Shell, Statoil, TOTAL, GDF SUEZ and the Research Council of Norway (193816/S60). NR 23 TC 8 Z9 9 U1 5 U2 15 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 1485 EP 1492 DI 10.1016/j.proci.2014.06.073 PN 2 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2FA UT WOS:000348048800042 ER PT J AU Dahms, RN Oefelein, JC AF Dahms, Rainer N. Oefelein, Joseph C. TI Non-equilibrium gas-liquid interface dynamics in high-pressure liquid injection systems SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Direct injection; Diesel engine; Supercritical flow; Real fluid model; Nonequilibrium thermodynamics ID UNDERSTANDING IGNITION PROCESSES; FLAME FRONT PROPAGATION; LARGE-EDDY SIMULATION; SURFACE-TENSION; GRADIENT THEORY; SUPERCRITICAL ENVIRONMENTS; CORRESPONDING STATES; TRANSPORT-PROPERTIES; CRYOGENIC FLAMES; BINARY-MIXTURES AB The transition of classical spray atomization processes to single-phase continuous dense-fluid mixing dynamics with diminished surface tension forces is poorly understood. Recently, a theory has been presented that established, based on a Knudsen-number criterion, that the development of such mixing layers is initiated because the multicomponent two-phase interface becomes much wider than the mean free molecular path. This shows that the transition to mixing layers occurs due to interfacial dynamics and not, as conventional wisdom had suggested, because the liquid phase has heated up to supercritical temperatures where surface tension forces diminish. In this paper we focus on the dynamics of this transition process, which still poses many fundamental questions. We show that such dynamics are dictated by substantial statistical fluctuations about the average interface molecule number and the presence of significant interfacial free energy forces. The comprehensive analysis is performed based on a combination of non-equilibrium mean-field thermodynamics and a detailed modified 32-term Benedict-Webb-Rubin mixture state equation. Statistical fluctuations are quantified using the generally accepted model of Poisson-distributions for variances in systems with a small number of molecules. Such fluctuations quantify the range of pressure and temperature conditions under which the gradual transition to dense-fluid mixing dynamics occurs. The interface begins to deteriorate as it broadens substantially. The related interfacial free energy forces do not instantly diminish only because vapor-liquid equilibrium conditions do not apply anymore. Instead, such forces along with the present interfacial statistical fluctuations are shown to gradually decrease as the interface transitions through the molecular chaos regime and to diminish once the interface enters the continuum regime. Then, the interfacial region becomes a continuous gas-liquid mixing layer with diminished free energy forces that is significantly affected by single-phase real-fluid thermodynamics and transport properties. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Dahms, Rainer N.; Oefelein, Joseph C.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94550 USA. RP Dahms, RN (reprint author), Sandia Natl Labs, Combust Res Facil, 7011 East Ave,MS9051, Livermore, CA 94550 USA. EM Rndahms@sandia.gov FU United States Department of Energy [DE-AC04-94-AL85000]; U.S. Department of Energy; Office of Science (SC), Basic Energy Sciences (BES) program [KC0301020] FX Support provided by the U.S. Department of Energy; Office of Science (SC), Basic Energy Sciences (BES) program under Grant No. KC0301020 is gratefully acknowledged. This research was performed at the Combustion Research Facility, Sandia National Laboratories, Livermore, California. Sandia National Laboratories is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the United States Department of Energy under contract DE-AC04-94-AL85000. NR 48 TC 6 Z9 6 U1 3 U2 24 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 1587 EP 1594 DI 10.1016/j.proci.2014.05.155 PN 2 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2FA UT WOS:000348048800051 ER PT J AU Lacaze, G Misdariis, A Ruiz, A Oefelein, JC AF Lacaze, Guilhem Misdariis, Antony Ruiz, Anthony Oefelein, Joseph C. TI Analysis of high-pressure Diesel fuel injection processes using LES with real-fluid thermodynamics and transport SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE LES; Diesel fuel injection; Supercritical fluids; Real-fluid thermodynamics ID LARGE-EDDY SIMULATION; SUBGRID-SCALE MODEL; SUPERCRITICAL-PRESSURE; TURBULENT COMBUSTION; CORRESPONDING STATES; PREDICTION; VISCOSITY; INTERFACE; PRINCIPLE; MIXTURES AB Imaging has long shown that under some high-pressure conditions, the presence of discrete two-phase flow processes becomes diminished. Instead, liquid injection processes transition from classical sprays to dense-fluid jets with no drops present. When and how this transition occurs, however, was not well understood until recently. In this paper, we summarized a new theoretical description that quantifies the effects of real fluid thermodynamics on liquid fuel injection processes as a function of pressure at typical Diesel engine operating conditions. We then apply the Large Eddy Simulation (LES) technique coupled with real-fluid thermodynamics and transport to analyze the flow at conditions when cylinder pressures exceed the thermodynamic critical pressure of the injected fuel. To facilitate the analysis, we use the experimental data posted as part of the Engine Combustion Network (see www.sandia.gov/ECN); namely the "Spray-A" case. Calculations are performed by rigorously treating the experimental operating conditions. Numerical results are in good agreement with available experimental measurements. The high-fidelity simulation is then used to analyze the details of transient mixing and understand the processes leading to auto-ignition. The analysis reveals the profound effect of supercritical fluid phenomena on the instantaneous three-dimensional mixing processes. The large density ratio between the supercritical fuel and the ambient gas leads to significant penetration of the jet with enhanced turbulent mixing at the tip and strong entrainment effects. Using detailed chemistry, a map of the auto-ignition delay time was calculated in simulation results. This map shows that a large flammable region with low velocity and mixture gradients is generated 250 diameters downstream of the injector. In the experiment, the first ignition site is observed at this location. This correspondence seems to indicate that the ignition location is piloted by the efficient mixing operating at the extremity of the jet coupled with long residence times, low strain rates and low scalar gradients. Published by Elsevier Inc. on behalf of The Combustion Institute. C1 [Lacaze, Guilhem; Ruiz, Anthony; Oefelein, Joseph C.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. [Misdariis, Antony] Renault SAS, F-91570 Lardy, France. RP Lacaze, G (reprint author), Sandia Natl Labs, Combust Res Facil, 7011 East Ave,Mail Stop 9051, Livermore, CA 94551 USA. EM gnlacaz@sandia.gov FU U.S. Department of Energy; Office of Science (SC), Basic Energy Sciences (BES) program; Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies (VT) program [KC0301020, VT0401000]; SC-BES program; United States Department of Energy [DE-AC04-94-AL85000]; Office of Science [DE-AC05-00OR22725] FX Support for this research was provided jointly by the U.S. Department of Energy; Office of Science (SC), Basic Energy Sciences (BES) program; and the Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies (VT) program, under grant numbers KC0301020 and VT0401000. Development of the foundational property evaluation schemes for multicomponent hydrocarbon mixtures was supported by the SC-BES program. Application of these tools to advanced engine combustion simulations was supported by the EERE-VT program. Sandia National Laboratories is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the United States Department of Energy under contract DE-AC04-94-AL85000. This research used resources of the Oak Ridge Leadership Computing Facility located in the Oak Ridge National Laboratory, which is supported by the Office of Science under Contract DE-AC05-00OR22725. NR 41 TC 10 Z9 11 U1 6 U2 28 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 1603 EP 1611 DI 10.1016/j.proci.2014.06.072 PN 2 PG 9 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2FA UT WOS:000348048800053 ER PT J AU Schenk, M Hansen, N Vieker, H Beyer, A Golzhauser, A Kohse-Hoinghaus, K AF Schenk, M. Hansen, N. Vieker, H. Beyer, A. Goelzhaeuser, A. Kohse-Hoeinghaus, K. TI PAH formation and soot morphology in flames of C-4 fuels SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE PAH; Soot; Combustion; Mass spectrometry; Helium-ion microscopy ID POLYCYCLIC AROMATIC-HYDROCARBONS; SIZE DISTRIBUTION; COMBUSTION CHEMISTRY; PREMIXED FLAMES; BUTANOL FLAMES; NASCENT SOOT; MECHANISMS; MICROSCOPY; PARTICLES; ETHYLENE AB In this work, we describe experimental studies on the formation of polycyclic aromatic hydrocarbons (PAH's) in opposed-flow atmospheric-pressure flames of n-butane, i-butane, i-butene, and i-butanol and on the morphology of nascent soot particles sampled from premixed atmospheric-pressure flames of the same fuels. To identify the major contributors to the molecular growth mechanism in opposed-flow flames, we employed flame-sampling molecular-beam mass spectrometry with electron ionization (EI) and in situ gas-chromatography (GC) with mass spectrometric detection. The EI and GC-EI mass spectra indicate that several pathways with different building blocks can contribute to molecular growth. Besides the commonly accepted hydrogen-abstraction-C2H2-addition steps, we found reactions of the methyl radical to be important steps. This observation is also supported by the complexity of the mass spectra which indicates that at least one of the building blocks is rather small. The importance of phenyl radicals as building blocks seems to be limited. We also sampled nascent soot particles from premixed atmospheric-pressure flames of the above mentioned fuels and used helium-ion microscopy to unravel the influence of the fuel structure on the morphology of the sampled particles. While differences in flame temperatures and residence times are known to influence the particle sizes, the observed different morphologies are likely due to slightly different C/O ratios and potentially the chemical nature of the fuel. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Schenk, M.; Kohse-Hoeinghaus, K.] Univ Bielefeld, Dept Chem, D-33615 Bielefeld, Germany. [Hansen, N.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. [Vieker, H.; Beyer, A.; Goelzhaeuser, A.] Univ Bielefeld, Dept Phys, D-33615 Bielefeld, Germany. RP Schenk, M (reprint author), Univ Bielefeld, Dept Chem, D-33615 Bielefeld, Germany. EM marina.schenk@uni-bielefeld.de; nhansen@sandia.gov RI Hansen, Nils/G-3572-2012; Kohse-Hoinghaus, Katharina/A-3867-2012; Beyer, Andre/E-5706-2011; Golzhauser, Armin/I-1270-2016 OI Beyer, Andre/0000-0002-9569-0344; Golzhauser, Armin/0000-0002-0838-9028 FU Division of Chemical Sciences, Geosciences and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy [DE-AC04-94-AL85000]; Alexander von Humboldt-Foundation FX The authors thank H. Waterbor for expert technical assistance. N.H. was in part supported by the Division of Chemical Sciences, Geosciences and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy under contract DE-AC04-94-AL85000. N.H. also acknowledges funding through the Alexander von Humboldt-Foundation. NR 41 TC 7 Z9 7 U1 5 U2 45 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 1761 EP 1769 DI 10.1016/j.proci.2014.06.139 PN 2 PG 9 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2FA UT WOS:000348048800071 ER PT J AU Johansson, KO Lai, JYW Skeen, SA Popolan-Vaida, DM Wilson, KR Hansen, N Violi, A Michelsen, HA AF Johansson, K. O. Lai, J. Y. W. Skeen, S. A. Popolan-Vaida, D. M. Wilson, K. R. Hansen, N. Violi, A. Michelsen, H. A. TI Soot precursor formation and limitations of the stabilomer grid SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Soot; Mass spectrometry; Modeling; Acetylene; PAH ID POLYCYCLIC AROMATIC-HYDROCARBONS; GENERATING PARTICLE BEAMS; CONTROLLED DIMENSIONS; AERODYNAMIC LENSES; NOZZLE EXPANSIONS; PREMIXED FLAMES; GROWTH; MECHANISM; COMBUSTION; PATHWAYS AB We have combined experimental and theoretical approaches to gain new insight into the mechanisms of PAH growth and soot formation. The experimental approach involves aerosol-mass spectrometry in conjunction with vacuum-ultraviolet photoionization of volatile species vaporizing from particles sampled from an Ar-diluted C2H2/O-2 counter-flow diffusion flame at nearly atmospheric pressure (700 Torr). We recorded aerosol mass spectra at different distances from the fuel outlet for fixed ionization energies and in a fixed position while tuning the photoionization energy. The mass spectra contain a large distribution of peaks, highlighting the importance of small building blocks and showing a variety of chemical species that extends beyond the traditional classification of PAHs based on thermodynamic stability. In addition, we performed stochastic simulations of PAH growth in the flame in order to provide better insight into the chemical composition of species associated with peaks in the measured mass spectra. These simulations were conducted using a stochastic nanoparticle simulator (SNAPS). Synthesis of experimental and simulated results showed that peaks in the observed mass spectra generally consisted of a mixture of PAH isomers. At m/z = 154 and 202, for example, experiments and simulations suggested that additional isomers than biphenyl and pyrene are important. Furthermore, the results highlight the importance of odd-carbon numbered species and complex growth paths. The experimental results suggest that species of higher masses can build up concentration ahead of species of lower masses. Our experimental results show, for example, that the peak at m/z = 278 appears closer to the burner outlet than the peak at m/z = 202, i.e., suggesting that a single monotonic growth mechanism is not enough. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Johansson, K. O.; Skeen, S. A.; Hansen, N.; Michelsen, H. A.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. [Lai, J. Y. W.; Violi, A.] Univ Michigan, Dept Mech Engn, Ann Arbor, MI 48109 USA. [Popolan-Vaida, D. M.; Wilson, K. R.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. RP Michelsen, HA (reprint author), Sandia Natl Labs, Combust Res Facil, POB 969, Livermore, CA 94551 USA. EM hamiche@sandia.gov RI Hansen, Nils/G-3572-2012 FU U.S. Department of Energy (DOE), Office of Basic Energy Sciences (BES) under the Single Investigator Small Group Research (SISGR) [DE-SC0002619]; DOE BES [DE-AC02-05CH11231]; Alexander von Humboldt Foundation; Division of Chemical Sciences, Geosciences, and Biosciences, DOE BES; National Nuclear Security Administration [DE-AC04-94-AL85000] FX This work has been funded by the U.S. Department of Energy (DOE), Office of Basic Energy Sciences (BES) under the Single Investigator Small Group Research (SISGR), Grant No. DE-SC0002619. Measurements were performed at the Advanced Light Source (ALS) of the Lawrence Berkeley National Laboratory. We are grateful to Paul Fugazzi and Paul Schrader for technical assistance. The ALS, K.R.W., and D.M.P.V. were supported by the Director, DOE BES, under Contract No. DE-AC02-05CH11231. D.M.P.V. is grateful to the Alexander von Humboldt Foundation for a Feodor Lynen fellowship. H.A.M. and N.H. were supported by the Division of Chemical Sciences, Geosciences, and Biosciences, DOE BES. Sandia is a multi-program laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the National Nuclear Security Administration under Contract No. DE-AC04-94-AL85000. NR 38 TC 10 Z9 10 U1 5 U2 34 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 1819 EP 1826 DI 10.1016/j.proci.2014.05.033 PN 2 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2FA UT WOS:000348048800078 ER PT J AU Kislov, VV Singh, RI Edwards, DE Mebel, AM Frenklach, M AF Kislov, V. V. Singh, R. I. Edwards, D. E. Mebel, A. M. Frenklach, M. TI Rate coefficients and product branching ratios for the oxidation of phenyl and naphthyl radicals: A theoretical RRKM-ME study SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Oxidation; Reaction mechanisms; PAH; Soot ID POLYCYCLIC AROMATIC-HYDROCARBONS; POTENTIAL-ENERGY SURFACE; MOLECULAR-OXYGEN O-2; THERMAL-DECOMPOSITION; UNIMOLECULAR DECOMPOSITION; C6H5; INTERMEDIATE; OXYRADICALS; PATHWAYS; KINETICS AB Theoretical VRC-TST/RRKM-ME calculations were performed to evaluate total rate coefficients and product branching ratios for the oxidation of phenyl and 1- and 2-naphthyl radicals with O-2 at temperatures relevant to combustion (1500, 2000, and 2500 K) and pressures of 0.01, 0.1, 1.0, and 10 atm. The results give the rate coefficients in the range of 3.0-5.5 x 10(-11) cm(3) molecule(-1) s(-1) with slightly positive temperature dependence, activation energies varying within 2.3-3.3 kcal/mol, and pre-exponential factors of 7-10 x 10(-11) cm(3) molecule(-1) s(-1). The dominant reaction channel in all three cases is elimination of the oxygen atom from peroxy complexes formed at the initial O-2 addition step and leading to the phenoxy and naphthoxy radical products. The contribution of this channel increases with temperature. Chemically-activated phenoxy and naphthoxy radicals either decompose to the cyclopentadienyl + CO and indenyl + CO products, respectively, or undergo thermal equilibration. The relative yields of the decomposition/equilibration products strongly depend on temperature and pressure in the way that a temperature growth favors decomposition, whereas an increase in pressure favors equilibration. At the lowest temperature considered, 1500 K, the reactions also yield significant amounts of pyranyl + CO (phenyl + O-2) or 1-benzopyranyl + CO (1-naphthyl + O-2). A comparison of the phenyl + O-2 and naphthyl + O-2 reactions reveals that although the general trends in the oxidation kinetics of phenyl and naphthyl radicals are similar, the size and especially the position of the radical site in the aromatic moiety may affect the details of the mechanism and relative product yields. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Kislov, V. V.; Mebel, A. M.] Florida Int Univ, Dept Chem & Biochem, Miami, FL 33199 USA. [Singh, R. I.; Edwards, D. E.; Frenklach, M.] Univ Calif Berkeley, Dept Mech Engn, Berkeley, CA 94720 USA. [Edwards, D. E.; Frenklach, M.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. RP Mebel, AM (reprint author), Florida Int Univ, Dept Chem & Biochem, CP 332,11200 SW 8th St, Miami, FL 33199 USA. EM mebela@fiu.edu RI Mebel, Alexander/A-5234-2009 FU Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Energy Sciences, Office of Sciences of the U.S. Department of Energy [DEFG02-04ER15570, DE-AC03-76F00098]; US Army Corps of Engineers, Humphreys Engineering Center Support Activity [W912HQ-11-C-0035]; Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231] FX This work was funded by the Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Energy Sciences, Office of Sciences of the U.S. Department of Energy (Grant No. DEFG02-04ER15570 to FIU and Contract No. DE-AC03-76F00098 to LBNL) and by the US Army Corps of Engineers, Humphreys Engineering Center Support Activity (Contract No. W912HQ-11-C-0035 to UCB). This research used resources of the National Energy Research Scientific Computing Center, which is supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. NR 33 TC 5 Z9 5 U1 2 U2 24 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 1861 EP 1869 DI 10.1016/j.proci.2014.06.135 PN 2 PG 9 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2FA UT WOS:000348048800083 ER PT J AU Jackson, SI AF Jackson, Scott I. TI An analytic method for two-dimensional wall motion and product isentrope from the detonation cylinder test SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Detonation; Cylinder test; Equation of state AB The cylinder test provides a measurement of detonation product's ability to perform work on adjacent material. Historically, direct numerical simulation has been required to derive the product energy content and isentrope from experiments of cylinder expansion driven by detonation products. One-dimensional analytic methods have not been able to accurately recover these parameters when the cylinder motion is compressible, exhibiting shocks. For incompressible cylinder motion, analytic one-dimensional approximations more accurately recover the isentrope, but still only approximate the two-dimensional cylinder motion and energy. This work provides a fully two-dimensional model that recovers the exact outer cylinder shape from experimental measurements. The inner cylinder shape and product isentrope are also exactly recovered in the limit of incompressible case motion. An alternate methodology also approximates the inner case shape and isentrope for compressible case motion, effectively allowing accurate isentrope determination for any cylinder test. The isentrope derived from a PBX 9502 cylinder test with compressible motion is shown to agree well with a reference isentrope. The errors associated with the one-dimensional flow assumption are also quantified. The incompressible case model can be used to estimate case shape and velocity from a given isentrope, providing a maximum fragment velocity. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Jackson, Scott I.] Los Alamos Natl Lab, Shock & Detonat Phys Grp, Los Alamos, NM 87545 USA. RP Jackson, SI (reprint author), Los Alamos Natl Lab, POB 1663,MS P952, Los Alamos, NM 87545 USA. EM sjackson@lanl.gov OI Jackson, Scott/0000-0002-6814-3468 FU U.S. Department of Energy via Campaign 2, "Dynamic Material Properties" FX This work was supported by the U.S. Department of Energy via Campaign 2, "Dynamic Material Properties" and other programs. NR 10 TC 2 Z9 2 U1 0 U2 2 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 1997 EP 2004 DI 10.1016/j.proci.2014.07.071 PN 2 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2FA UT WOS:000348048800099 ER PT J AU Anderson, EK Aslam, TD Jackson, SI AF Anderson, Eric K. Aslam, Tariq D. Jackson, Scott I. TI The effect of transverse shock propagation on the shock-to-detonation transition process for an insensitive explosive SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Shock; Detonation; Initiation; Transition AB The one-dimensional (1D) shock-to-detonation transition process has been studied extensively for PBX 9502, resulting in a good ability to predict the time or distance to detonation over a range of planar input shock pressures. The results are often represented as run distance or time versus input shock pressure on Pop plots. In practice, however, input shocks to explosives are often not 1D. Instead, they may be oblique or non-planar. Here, we present results from a series of experiments in which a PBX 9502 slab was bonded on one side to a PBX 9501 slab. The faster detonation in the PBX 9501 slab drove an oblique shock in the PBX 9502. The result was a two-dimensional (2D) shock structure consisting of a region of delayed reaction, referred to as an initiating layer, immediately adjacent to the PBX 9501/9502 interface, and a transition to detonation further from the interface. The initiating layer thickness varied with the input shock pressure, which was controlled by the thickness of the PBX 9501 layer. The results of seven such tests are presented in run-time versus input-shock-pressure space and compared to Pop plots generated with data from 1D experiments. Good agreement was observed, with the 2D results showing similar run-times to detonation, but more scatter for a given input shock pressure. The good correlation between the 1D and 2D data suggests the transverse component of the initiating shock does not have a significant effect on the initiation physics. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Anderson, Eric K.; Aslam, Tariq D.; Jackson, Scott I.] Los Alamos Natl Lab, Dynam & Energet Mat Div, Shock & Detonat Phys Grp, Los Alamos, NM 87545 USA. RP Anderson, EK (reprint author), Los Alamos Natl Lab, POB 1663,MS P952, Los Alamos, NM 87545 USA. EM eanderson@lanl.gov OI Jackson, Scott/0000-0002-6814-3468; Aslam, Tariq/0000-0002-4263-0401; Anderson, Eric/0000-0002-5309-5686 FU U.S. Department of Energy Campaign 2: "Dynamic Material Properties" FX This effort was funded by the U.S. Department of Energy Campaign 2: "Dynamic Material Properties." Experiments were assembled and fielded with assistance provided by Sam Vincent and Tim Tucker. NR 10 TC 2 Z9 2 U1 0 U2 14 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 2033 EP 2040 DI 10.1016/j.proci.2014.07.072 PN 2 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2FA UT WOS:000348048800103 ER PT J AU Hill, LG AF Hill, L. G. TI Is the detonation "Dead Zone" really dead? SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Detonation; High Explosive; Dead Zone; Initiation layer; CYLEX test ID PBX-9502 AB This paper explores the Dead Zone (DZ) phenomenon in solid High Explosives (HEs), whereby weaker regions of a detonation shock fail to trigger prompt reaction, leaving behind them isolated pockets of substantially unburned explosive. A key unanswered question is the extent to which DZs react in the following flow, and whether they contribute a significant amount of energy on timescales relevant to system deconsolidation. This paper comprises two parts. The first surveys the DZ phenomenon and discusses (1) the multiple contexts in which it arises, (2) what is observed and believed about it, and (3) how it may be broadly categorized. This general perspective sets the stage for the second part, which examines in detail one particular DZ variant called transverse initiation. This case was not chosen because it is the most common or important, but because it is the most amenable to inquiry. (DZ quantification is quite difficult, and the presented experiment is apparently the first conceived to quantify DZs of any type.) The technique uses a modified Cylinder Expansion (CYLEX) test, wherein a faster HE core (PBX 9501, 95 wt% HMX) is surrounded by a slower HE annulus (PBX 9502, 95 wt% TATB). The fast HE drives detonation in the slow HE faster than the latter would naturally propagate; however, in doing so a largely unreacted initiation layer is left in the slow HE adjacent to the fast HE. Combining the usual CYLEX diagnostics with detonation front curvature measurements and invoking a novel analysis based on the Gurney and Taylor methods, the energy release vs time (and distance) is inferred. The result is a similar to 0.3 mu s induction time (similar to 3 mm induction lag), after which the energy release rises in similar to 2 mu s (15 mm) to half its asymptotic value: similar to 86% of the energy released by a PBX 9502 detonation. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Hill, LG (reprint author), Los Alamos Natl Lab, Mail Stop P918, Los Alamos, NM 87545 USA. EM lgh@lanl.gov FU Campaign 2 of the U.S. Department of Energy FX This project was funded by Campaign 2 of the U.S. Department of Energy (Dan Hooks Project Leader, Rick Martineau Program Manager). Tariq Aslam provided technical advice. Ronnie Olivas, Joe Rael, and Steve Rivera provided fabrication support. Matt Briggs, Bob Mier, John Morris, Mike Shinas, and Larry Vaughan provided shot fielding support. NR 16 TC 1 Z9 1 U1 5 U2 9 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 2041 EP 2049 DI 10.1016/j.proci.2014.10.001 PN 2 PG 9 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2FA UT WOS:000348048800104 ER PT J AU Zeng, W Sjoberg, M Reuss, DL AF Zeng, Wei Sjoeberg, Magnus Reuss, David L. TI Combined effects of flow/spray interactions and EGR on combustion variability for a stratified DISI engine SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Stratified DISI engine; Combustion variability; Flow/spray interactions; EGR; Optical diagnostics AB This study investigates combustion variability of a stratified-charge direct-injection spark ignited (DISI) engine, operated with near-TDC injection of E70 fuel and a spark timing that occurs during the early part of the fuel injection. Using EGR, low engine-out NOx can be achieved, but at the expense of increased combustion variability at higher engine speeds. Initial motored tests at different speeds reveal that the in-cylinder gas flow becomes sufficiently strong at 2000 rpm to cause significant cycle-to-cycle variations of the spray penetration. Hence, the fired tests focus on operation at 2000 rpm with N-2 dilution ([O-2] = 19% and 21%) to simulate EGR. In-cylinder flow, spray, and early-flame measurements are correlated to reveal their effect on the combustion variability. Results reveal two types of flow/spray-interactions that predict the likelihood of a partial burn. (1) Proper flow direction before injection with a more collapsed spray leads to high kinetic energy of the flow during injection, thus generating a rapid early burn, which ensures complete combustion, regardless of the EGR level. (2) Improper flow direction and less collapsed spray generate low flow energy during the early phase of combustion. For this second type of flow/spray-interaction, application of EGR results in a partial-burn frequency of 30%, whereas without EGR, early combustion is shown to be insensitive to flow variations. Flame-probability maps illustrate that the partial-burn cycles for operation with EGR have a weak flame development in that the flame does not develop uniformly and reliably from the spark plug. Without EGR, the flame development is more repeatable regardless of the type of flow/spray-interaction, at the expense of higher NOx emissions. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Zeng, Wei; Sjoeberg, Magnus; Reuss, David L.] Sandia Natl Labs, Livermore, CA 94551 USA. [Reuss, David L.] Univ Michigan, Ann Arbor, MI 48109 USA. RP Zeng, W (reprint author), Sandia Natl Labs, MS 9053,POB 969, Livermore, CA 94551 USA. EM wzeng@sandia.gov FU U.S. Department of Energy, Office of Vehicle Technologies; United States Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX Financial support was provided by the U.S. Department of Energy, Office of Vehicle Technologies. Sandia is a multiprogram laboratory operated by the Sandia Corporation, a Lockheed Martin Company, for the United States Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000. NR 13 TC 7 Z9 7 U1 1 U2 11 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 2907 EP 2914 DI 10.1016/j.proci.2014.06.106 PN 3 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2FH UT WOS:000348049500049 ER PT J AU Wolk, B Chen, JY Dec, JE AF Wolk, Benjamin Chen, Jyh-Yuan Dec, John E. TI Computational study of the pressure dependence of sequential auto-ignition for partial fuel stratification with gasoline SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Gasoline; Reduced; Mechanism; Stratification; Auto-ignition ID HCCI ENGINES; SINGLE-STAGE; HEAT-RELEASE; LOAD LIMITS; COMBUSTION; HEPTANE; 2-STAGE AB Fuel stratification is a potential strategy for reducing the maximum pressure rise rate in HCCI engines. Simulations of Partial Fuel Stratification (PFS) have been performed using CONVERGE with a 96-species reduced mechanism for a 4-component gasoline surrogate. Comparison is made to experimental data from the Sandia HCCI engine at a compression ratio 14: 1 at intake pressures of 1 bar and 2 bar. Analysis of the heat release and temperature in the different equivalence ratio (phi) regions reveals that sequential auto-ignition of the stratified charge occurs in order of increasing phi for 1 bar intake pressure but in order of decreasing phi for 2 bar intake pressure. Increased low-and intermediate-temperature heat release at 2 bar intake pressure compensates for decreased temperatures in higher-phi regions due to evaporative cooling from the liquid fuel spray and decreased compression heating from lower values of the ratio of specific heats. At 1 bar intake pressure, the premixed portion of the charge auto-ignites before the highest-phi regions and the sequential auto-ignition occurs too fast for useful reduction of the maximum pressure rise rate compared to HCCI. Conversely, at 2 bar intake pressure, the premixed portion of the charge auto-ignites last, after the higher-phi regions. More importantly, the sequential auto-ignition occurs over a longer time period than at 1 bar intake pressure such that a sizable reduction in the maximum pressure rise rate compared to HCCI can be achieved. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Wolk, Benjamin; Chen, Jyh-Yuan] Univ Calif Berkeley, Dept Mech Engn, Berkeley, CA 94720 USA. [Dec, John E.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94550 USA. RP Wolk, B (reprint author), Univ Calif Berkeley, 246 Hesse Hall, Berkeley, CA 94720 USA. EM bmwolk@berkeley.edu OI Wolk, Benjamin/0000-0002-9690-9459 FU National Science Foundation; U.S. Department of Energy [CBET-1258653] FX This work at the University of California, Berkeley was partially supported by the National Science Foundation and U.S. Department of Energy under award CBET-1258653. NR 19 TC 3 Z9 3 U1 4 U2 16 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 2993 EP 3000 DI 10.1016/j.proci.2014.05.023 PN 3 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2FH UT WOS:000348049500059 ER PT J AU Leermakers, CAJ Musculus, MPB AF Leermakers, C. A. J. Musculus, M. P. B. TI In-cylinder soot precursor growth in a low-temperature combustion diesel engine: Laser-induced fluorescence of polycyclic aromatic hydrocarbons SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Polycyclic aromatic hydrocarbons; Particulate matter; Laser-induced fluorescence; Laser-induced incandescence; Diesel low-temperature combustion ID DIFFUSION FLAME; EMISSIONS; RATIO AB The growth of poly-cyclic aromatic hydrocarbon (PAH) soot precursors are observed using a two-laser technique combining laser-induced fluorescence (LIF) of PAH with laser-induced incandescence (LII) of soot in a diesel engine under low-temperature combustion (LTC) conditions. The broad mixture distributions and slowed chemical kinetics of LTC "stretch out" soot-formation processes in both space and time, thereby facilitating their study. Imaging PAH-LIF from pulsed-laser excitation at three discrete wavelengths (266, 532, and 633 nm) reveals the temporal growth of PAH molecules, while soot-LII from a 1064-nm pulsed laser indicates inception to soot. The distribution of PAH-LIF also grows spatially within the combustion chamber before soot-LII is first detected. The PAH-LIF signals have broad spectra, much like LII, but typically with spectral profile that is inconsistent with laser-heated soot. Quantitative natural-emission spectroscopy also shows a broad emission spectrum, presumably from PAH chemiluminescence, temporally coinciding with of the PAH-LIF. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Leermakers, C. A. J.] Eindhoven Univ Technol, Dept Mech Engn, NL-5600 MB Eindhoven, Netherlands. [Musculus, M. P. B.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. RP Musculus, MPB (reprint author), Sandia Natl Labs, Combust Res Facil, POB 969,MS 9053, Livermore, CA 94551 USA. EM mpmuscu@sandia.gov FU United States Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000]; U.S. Department of Energy, Office of Vehicle Technologies FX Support for this research at the Combustion Research Facility, Sandia National Laboratories, Livermore, CA, was provided by the U.S. Department of Energy, Office of Vehicle Technologies. Sandia is a multi-program laboratory operated by Sandia Corporation, a Lockheed Martin Company for the United States Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000. Keith Penney and David Cicone are gratefully acknowledged for their assistance with experiments. NR 24 TC 6 Z9 7 U1 1 U2 21 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 3079 EP 3086 DI 10.1016/j.proci.2014.06.101 PN 3 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2FH UT WOS:000348049500069 ER PT J AU Skeen, SA Manin, J Pickett, LM AF Skeen, Scott A. Manin, Julien Pickett, Lyle M. TI Simultaneous formaldehyde PLIF and high-speed schlieren imaging for ignition visualization in high-pressure spray flames SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Spray combustion; Diesel combustion; High-speed imaging; Formaldehyde PLIF; Schlieren imaging ID LASER-INDUCED FLUORESCENCE; COMBUSTION; MODELS; LES AB We applied simultaneous schlieren and formaldehyde (CH2O) planar laser-induced fluorescence (PLIF) imaging to investigate the low-and high-temperature auto-ignition events in a high-pressure (60 bar) spray of n-dodecane. High-speed (150 kHz) schlieren imaging allowed visualization of the temporal progression of the fuel vapor penetration as well as the low-and high-temperature ignition events, while formaldehyde fluorescence was induced by a pulsed (7-ns), 355-nm planar laser sheet at a select time during the same injection. Fluorescence from polycyclic aromatic hydrocarbons (PAH) was also observed and was distinguished from formaldehyde PLIF both temporally and spatially. A characteristic feature previously recorded in schlieren images of similar flames, in which refractive index gradients significantly diminish, has been confirmed to be coincident with large formaldehyde fluorescence signal during low-temperature ignition. Low-temperature reactions initiate near the radial periphery of the spray on the injector side of the spray head. Formaldehyde persists on the injector side of the lift-off length and forms rapidly near the injector following the end of injection. The consumption of formaldehyde coincides with the position and timing of high-temperature ignition and low-density zones that are clearly evident in the schlieren imaging. After the end of injection, the formaldehyde that formed on the injector side of the lift-off length is consumed as a high-temperature ignition front propagates back toward the injector tip. Published by Elsevier Inc. on behalf of The Combustion Institute. C1 [Skeen, Scott A.; Manin, Julien; Pickett, Lyle M.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. RP Skeen, SA (reprint author), PO 969 MS 9055, Livermore, CA 94551 USA. EM sskeen@sandia.gov FU United States Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX We thank Chris Carlen, Dave Cicone, and Keith Penney for technical assistance. The experiments were conducted at the Combustion Research Facility, Sandia National Laboratories, Livermore, CA. Support for this work (SAS) was provided by Sandia National Laboratories under the Early Career Laboratory-Directed Research and Development (EC-LDRD) program and by the U.S. Department of Energy, Office of Vehicle Technologies. Sandia is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the United States Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000. NR 23 TC 29 Z9 31 U1 7 U2 24 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 3167 EP 3174 DI 10.1016/j.proci.2014.06.040 PN 3 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2FH UT WOS:000348049500079 ER PT J AU Bohlin, A Mann, M Patterson, BD Dreizler, A Kliewer, CJ AF Bohlin, Alexis Mann, Markus Patterson, Brian D. Dreizler, Andreas Kliewer, Christopher J. TI Development of two-beam femtosecond/picosecond one-dimensional rotational coherent anti-Stokes Raman spectroscopy: Time-resolved probing of flame wall interactions SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Time-resolved spectroscopy; CARS; Coherent imaging; Flame-wall interaction; Combustion diagnostics ID SINGLE-SHOT THERMOMETRY; SCATTERING THERMOMETRY; CARS THERMOMETRY; LASER-SHOT; TEMPERATURE; N-2; COMBUSTION; LINEWIDTHS; SPECTRA; H-2 AB Hybrid femtosecond/picosecond rotational coherent anti-Stokes Raman spectroscopy (CARS) is developed utilizing a two-beam phase-matching approach for one-dimensional (1D) measurements demonstrated in an impinging jet burner to probe time-resolved head on quenching (HOQ) of a methane/air premixed flame at Phi = 1.0 and Reynolds number = 5000. Single-laser-shot 1D temperature profiles are obtained over a distance of at least 4 mm by fitting the pure-rotational N-2 CARS spectra to a spectral library calculated from a time-domain CARS code. An imaging resolution of similar to 61 lm is obtained in the 1D-CARS measurements. The acquisition of single-shot 1D CARS measurements, as opposed to traditional point-wise CARS techniques, enables new spatially correlated conditional statistics to be determined, such as the position, magnitude, and fluctuations of the instantaneous temperature gradient. The temperature gradient increases as the flame approaches the metal surface, and decreases during quenching. The standard deviation of the temperature gradient follows the same trend as the temperature gradient, increasing as the flame front approaches the surface, and decreasing after quenching. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Bohlin, Alexis; Patterson, Brian D.; Kliewer, Christopher J.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. [Mann, Markus; Dreizler, Andreas] Ctr Smart Interfaces, FG Reakt Stromungen & Messtech, D-64287 Darmstadt, Germany. RP Kliewer, CJ (reprint author), Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. EM cjkliew@sandia.gov RI Bohlin, Alexis/L-8973-2015; Kliewer, Christopher/E-4070-2010 OI Bohlin, Alexis/0000-0003-4383-8332; Kliewer, Christopher/0000-0002-2661-1753 FU U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences; U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000]; DFG (Deutsche Forschungsgemeinschaft), (Center of Smart Interfaces) [EXC 259]; DFG (Deutsche Forschungsgemeinschaft) [GRK 1344] FX Funding for CJK and AB provided by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences. Sandia is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000. AD and MM gratefully acknowledge the financial support of the DFG (Deutsche Forschungsgemeinschaft), EXC 259 (Center of Smart Interfaces) and GRK 1344. NR 38 TC 8 Z9 8 U1 1 U2 26 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 3723 EP 3730 DI 10.1016/j.proci.2014.05.124 PN 3 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2FH UT WOS:000348049500143 ER PT J AU Magnotti, G Geyer, D Barlow, RS AF Magnotti, G. Geyer, D. Barlow, R. S. TI Interference free spontaneous Raman spectroscopy for measurements in rich hydrocarbon flames SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE 1D Raman spectroscopy; Interference; Turbulent flames; Diagnostics ID RAYLEIGH-LIF MEASUREMENTS; NONPREMIXED FLAMES; DIFFUSION FLAME; SCATTERING; EXCITATION; COMBUSTION AB The capability to simultaneously acquire two orthogonal components of a Raman spectrum has been added to the Sandia Raman/Rayleigh/CO-LIF instrument for combustion measurements. This addition allows removing unpolarized fluorescence interference signal from Raman spectra, extending the applicability of the instrument to rich hydrocarbon flames. The optical set-up and the data analysis approach are described. The instrument is tested in challenging rich laminar and turbulent CH4/air flames, deemed inaccessible with the previous instrument. Experimental results show good agreement with laminar calculations performed with Chemkin. The approach also avoids the cumbersome calibration and correction procedures required for data collected with the previous version of the instrument in presence of mild fluorescence interference. The drawback is a drop in the instrument precision, in particular for CO2 and O-2 concentrations. Published by Elsevier Inc. on behalf of The Combustion Institute. C1 [Magnotti, G.; Barlow, R. S.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94550 USA. [Geyer, D.] Hsch Darmstadt, FB Maschinenbau & Kunststofftech, D-64295 Darmstadt, Germany. RP Magnotti, G (reprint author), Sandia Natl Labs, Combust Res Facil, Livermore, CA 94550 USA. EM gmagnot@sandia.gov FU Division of Chemical Sciences, Geosciences and Biosciences, Office of Basic Energy Sciences, US Department of Energy; United States Department of Energy [DE-AC04-94-AL85000] FX Work was supported by the Division of Chemical Sciences, Geosciences and Biosciences, Office of Basic Energy Sciences, US Department of Energy. Sandia National Laboratories is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the United States Department of Energy under contract DE-AC04-94-AL85000. Contributions by Bob Harmon and Chris Carlen in support of these experiments are gratefully acknowledged. NR 18 TC 4 Z9 4 U1 2 U2 11 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 3765 EP 3772 DI 10.1016/j.proci.2014.05.076 PN 3 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2FH UT WOS:000348049500148 ER PT J AU Weinkauff, J Trunk, P Frank, JH Dunn, MJ Dreizler, A Bohm, B AF Weinkauff, J. Trunk, P. Frank, J. H. Dunn, M. J. Dreizler, A. Boehm, B. TI Investigation of flame propagation in a partially premixed jet by high-speed-Stereo-PIV and acetone-PLIF SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE High-speed measurements; Acetone PLIF; Stereo PIV; Flame propagation; Mixture fraction ID LASER-INDUCED FLUORESCENCE; DIFFUSION FLAME; REPETITION-RATE; EDGE-FLAMES; TURBULENT; IGNITION; DIAGNOSTICS; SCATTERING AB This paper presents an experimental study of flame propagation through a partially-premixed flow following ignition. A combination of simultaneous high-speed acetone planar laser induced fluorescence (PLIF) and stereoscopic particle image velocimetry (SPIV) was utilized for time-resolved measurements of mixture fraction, flow field and flame position. This provides access to the major quantities needed to characterize non-premixed flames. High quality mixture fraction measurements with signal-to-noise ratios up to 120 for unity mixture fraction were made feasible using a combination of a conventional high-speed laser at 10 kHz for LIF excitation and a wavelet based de-noising algorithm to reject camera noise. It was observed that flame propagation in the far-field of a partially-premixed jet takes place in a premixed mode, with the flame propagating through highly stratified mixtures until it approaches locations containing mixtures outside the flammability limits. In these areas the flame recedes and further propagation is controlled by mixing processes of air and fuel. Even though flame propagation is then mixing-controlled, the flame is not observed to switch into a non-premixed mode. Instead, mixing ahead of the flame takes place until locally premixed flammable mixtures are recovered for subsequent flame propagation. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Weinkauff, J.; Trunk, P.; Dreizler, A.] Tech Univ Darmstadt, Fachgebiet Reakt Stromungen & Messtech, D-64287 Darmstadt, Germany. [Frank, J. H.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. [Dunn, M. J.] Univ Sydney, Sch Aerosp Mech & Mech Engn, Sydney, NSW 2006, Australia. [Boehm, B.] Tech Univ Darmstadt, Fachgebiet Energie & Kraftwerkstech, D-64287 Darmstadt, Germany. RP Bohm, B (reprint author), Tech Univ Darmstadt, Fachgebiet Energie & Kraftwerkstech, Jovanka Bontschits Str 2, D-64287 Darmstadt, Germany. EM bboehm@ekt.tu-darmstadt.de RI Bohm, Benjamin/I-1666-2012 FU Deutsche Forschungsgemeinschaft [EXC 259]; U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences; U.S. Department of Energy [DE-AC04-94-AL85000] FX Financial support by Deutsche Forschungsgemeinschaft (EXC 259) is gratefully acknowledged. J.H. Frank was supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences. Sandia National Laboratories is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the U.S. Department of Energy under contract DE-AC04-94-AL85000. NR 25 TC 1 Z9 2 U1 0 U2 21 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2015 VL 35 BP 3773 EP 3781 DI 10.1016/j.proci.2014.05.022 PN 3 PG 9 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AZ2FH UT WOS:000348049500149 ER PT J AU Clay, WA Dahl, JEP Carlson, RMK Melosh, NA Shen, ZX AF Clay, W. A. Dahl, J. E. P. Carlson, R. M. K. Melosh, N. A. Shen, Z-X TI Physical properties of materials derived from diamondoid molecules SO REPORTS ON PROGRESS IN PHYSICS LA English DT Review DE diamondoid; nanoparticle; self-assembled monolayer ID SELF-ASSEMBLED MONOLAYERS; METAL-ORGANIC FRAMEWORKS; SECONDARY BUILDING UNITS; CARBON-CARBON BONDS; FUNCTIONALIZED NANODIAMONDS; INFRARED-SPECTROSCOPY; SELECTIVE PREPARATION; REFRACTIVE-INDEX; ADAMANTANE; DIAMANTANE AB Diamondoids are small hydrocarbon molecules which have the same rigid cage structure as bulk diamond. They can be considered the smallest nanoparticles of diamond. They exhibit a mixture of properties inherited from bulk cubic diamond as well as a number of unique properties related to their size and structure. Diamondoids with different sizes and shapes can be separated and purified, enabling detailed studies of the effects of size and structure on the diamondoids' properties and also allowing the creation of chemically functionalized diamondoids which can be used to create new materials. Most notable among these new materials are self-assembled monolayers of diamondoid-thiols, which exhibit a number of unique electron emission properties. C1 [Clay, W. A.; Dahl, J. E. P.; Carlson, R. M. K.; Melosh, N. A.; Shen, Z-X] Stanford Inst Mat & Energy Sci, SLAC, Natl Accelerator Lab, Menlo Pk, CA 94025 USA. [Clay, W. A.; Dahl, J. E. P.; Carlson, R. M. K.; Melosh, N. A.; Shen, Z-X] Stanford Univ, Dept Phys & Appl Phys, Geballe Lab Adv Mat, Stanford, CA 94305 USA. RP Clay, WA (reprint author), Stanford Inst Mat & Energy Sci, SLAC, Natl Accelerator Lab, 2575 Sand Hill Rd, Menlo Pk, CA 94025 USA. EM wclay@alumni.stanford.edu; nmelosh@stanford.edu; zxshen@stanford.edu FU US Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences FX This work is supported by the US Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences. We would like to extend special thanks to Prof P Schreiner for many helpful discussions that contributed to this work. NR 109 TC 9 Z9 9 U1 13 U2 66 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 0034-4885 EI 1361-6633 J9 REP PROG PHYS JI Rep. Prog. Phys. PD JAN PY 2015 VL 78 IS 1 AR 016501 DI 10.1088/0034-4885/78/1/016501 PG 21 WC Physics, Multidisciplinary SC Physics GA CA2TL UT WOS:000348760600003 PM 25551840 ER PT J AU Zhang, J Florita, A Hodge, BM Lu, S Hamann, HF Banunarayanan, V Brockway, AM AF Zhang, Jie Florita, Anthony Hodge, Bri-Mathias Lu, Siyuan Hamann, Hendrik F. Banunarayanan, Venkat Brockway, Anna M. TI A suite of metrics for assessing the performance of solar power forecasting SO SOLAR ENERGY LA English DT Article DE Grid integration; Nonparametric statistical testing; Solar power forecasting; Solar power ramps; Sensitivity analysis ID INTELLIGENCE TECHNIQUES; RADIATION; MULTIVARIATE; SATELLITE; SUPPORT AB Forecasting solar energy generation is a challenging task because of the variety of solar power systems and weather regimes encountered. Inaccurate forecasts can result in substantial economic losses and power system reliability issues. One of the key challenges is the unavailability of a consistent and robust set of metrics to measure the accuracy of a solar forecast. This paper presents a suite of generally applicable and value-based metrics for solar forecasting for a comprehensive set of scenarios (i.e., different time horizons, geographic locations, and applications) that were developed as part of the U.S. Department of Energy SunShot Initiative's efforts to improve the accuracy of solar forecasting. In addition, a comprehensive framework is developed to analyze the sensitivity of the proposed metrics to three types of solar forecasting improvements using a design-of-experiments methodology in conjunction with response surface, sensitivity analysis, and nonparametric statistical testing methods. The three types of forecasting improvements are (i) uniform forecasting improvements when there is not a ramp, (ii) ramp forecasting magnitude improvements, and (iii) ramp forecasting threshold changes. Day-ahead and 1-hour-ahead forecasts for both simulated and actual solar power plants are analyzed. The results show that the proposed metrics can efficiently evaluate the quality of solar forecasts and assess the economic and reliability impacts of improved solar forecasting. Sensitivity analysis results show that (i) all proposed metrics are suitable to show the changes in the accuracy of solar forecasts with uniform forecasting improvements, and (ii) the metrics of skewness, kurtosis, and Renyi entropy are specifically suitable to show the changes in the accuracy of solar forecasts with ramp forecasting improvements and a ramp forecasting threshold. Published by Elsevier Ltd. C1 [Zhang, Jie; Florita, Anthony; Hodge, Bri-Mathias] Natl Renewable Energy Lab, Golden, CO 80401 USA. [Lu, Siyuan; Hamann, Hendrik F.] IBM TJ Watson Res Ctr, Yorktown Hts, NY 10598 USA. [Banunarayanan, Venkat; Brockway, Anna M.] US DOE, Washington, DC 20585 USA. RP Hodge, BM (reprint author), Natl Renewable Energy Lab, Golden, CO 80401 USA. EM bri.mathias.hodge@nrel.gov OI Brockway, Anna/0000-0002-5167-7594 FU U.S. Department of Energy [DE-AC36-08-GO28308]; National Renewable Energy Laboratory FX This work was supported by the U.S. Department of Energy under Contract No. DE-AC36-08-GO28308 with the National Renewable Energy Laboratory as part of the project work performed under the SunShot Initiative's Improving the Accuracy of Solar Forecasting program. Comments and suggestions from the following researchers are also gratefully acknowledged: Dr. Brad Lehman from Northeastern University, Dr. Joseph Simmons from University of Arizona, Dr. Edwin Campos from Argonne National Laboratory, Dr. Melinda Marquis from National Oceanic and Atmospheric Administration, Tara Jensen and Tressa Fowler from National Center for Atmospheric Research, and Jari Miettinen from VTT Technical Research Centre of Finland. NR 49 TC 17 Z9 17 U1 2 U2 7 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0038-092X J9 SOL ENERGY JI Sol. Energy PD JAN PY 2015 VL 111 BP 157 EP 175 DI 10.1016/j.solener.2014.10.016 PG 19 WC Energy & Fuels SC Energy & Fuels GA AZ5KE UT WOS:000348259200015 ER PT J AU Mayes, HB Nolte, MW Beckham, GT Shanks, BH Broadbelt, LJ AF Mayes, Heather B. Nolte, Michael W. Beckham, Gregg T. Shanks, Brent H. Broadbelt, Linda J. TI The Alpha-Bet(a) of Salty Glucose Pyrolysis: Computational Investigations Reveal Carbohydrate Pyrolysis Catalytic Action by Sodium Ions SO ACS CATALYSIS LA English DT Article DE biomass; cellulose; biofuels; 5-HMF; kinetics; dehydration; transition-state stabilization; inorganic salts ID ELECTROCYCLIC FRAGMENTATION MECHANISMS; MOLECULAR-ORBITAL METHODS; CELLULOSE PYROLYSIS; BIOMASS PYROLYSIS; THERMAL-DECOMPOSITION; TRANSPORTATION FUELS; CARBONYL-COMPOUNDS; BIO-OIL; KINETICS; MODEL AB Biomass pyrolysis is a promising technology for the production of renewable fuels and chemicals from nonfood biomass. Given the potential of pyrolysis as a viable, cost-effective biomass deconstruction method, there is active interest in understanding the chemical transformations at the heart of the technology. It has long been known that the presence of alkali- and alkaline-earth-metal ions in biomass, such as Na+, significantly alters product yields of biomass pyrolysis, but the mechanism behind this effect has not been elucidated. In this work, we employ density functional theory (DFT) to reveal the stereoelectronic basis of the effect of sodium ions on several key glucose thermal decomposition reactions, such as the formation of levoglucosan and 5-hydroxymethylfurfural (5-HMF). beta-D-Glucose is of interest for pyrolysis, as it is the monomer of cellulose and a key intermediate in cellulose pyrolysis. alpha-D-Glucose is included in this study, as the two anomers can readily interconvert under pyrolysis conditions. The computational results are consistent with the experimental results for alpha- and beta-D-glucose pyrolysis with NaCl, which demonstrate that the products are the same as those produced in neat pyrolysis, but with differing relative yields. We find that the sodium ion changes the reaction rate coefficients to varying degrees, with approximately 70% of the reactions in this study catalyzed by Na+, approximately 25% inhibited by Na+, and the remainder showing virtually no effect on the rate coefficient. The variations in how the ion modifies the rate coefficient reflect how the particular stereochemistry of the transition state interacts with the ion. The sodium ions have a more subtle effect on reactant electronic structure. The results of this study provide a molecular-level understanding of how naturally occurring salts act as catalysts in biomass pyrolysis. C1 [Mayes, Heather B.; Broadbelt, Linda J.] Northwestern Univ, Dept Chem & Biol Engn, Evanston, IL 60208 USA. [Nolte, Michael W.; Shanks, Brent H.] Iowa State Univ, Dept Chem & Biol Engn, Ames, IA 50011 USA. [Beckham, Gregg T.] Natl Renewable Energy Lab, Natl Bioenergy Ctr, Golden, CO 80401 USA. [Shanks, Brent H.] Iowa State Univ, Ctr Biorenewable Chem CBiRC, Ames, IA 50011 USA. RP Shanks, BH (reprint author), Iowa State Univ, Dept Chem & Biol Engn, Ames, IA 50011 USA. EM bshanks@iastate.edu; broadbelt@northwestern.edu RI Broadbelt, Linda/B-7640-2009; Mayes, Heather/D-8755-2016 OI Mayes, Heather/0000-0001-9373-0106 FU National Advanced Biofuels Consortium (NABC) - Department of Energy (DOE) Office of Energy Efficiency and Renewable Energy through the Office of Biomass Program [DE-EE0003044]; Office of Science of the U.S. DOE [DE-AC02-05CH11231]; NREL Computational Sciences Center - DOE Office of EERE [DE-AC36-08GO28308]; San Diego Supercomputing Center - NSF XSEDE Grant [MCB090159]; DOE Computational Science Graduate Fellowship (CSGF) [DE-FG02-97ER25308]; ARCS Foundation Inc., Chicago Chapter FX This work was supported by the National Advanced Biofuels Consortium (NABC), which is funded by the Department of Energy (DOE) Office of Energy Efficiency and Renewable Energy through the Office of Biomass Program, grant number DE-EE0003044. This research used computational resources of the National Energy Research Scientific Computing Center, which is supported by the Office of Science of the U.S. DOE under Contract No. DE-AC02-05CH11231, the NREL Computational Sciences Center, which is supported by the DOE Office of EERE under Contract No. DE-AC36-08GO28308, and the San Diego Supercomputing Center, which is supported under the NSF XSEDE Grant MCB090159. The authors thank Glen A. Ferguson for valuable discussions and Chris Mayes for helpful scripts. H.B.M. was supported by a DOE Computational Science Graduate Fellowship (CSGF), which is provided under grant number DE-FG02-97ER25308, and the ARCS Foundation Inc., Chicago Chapter. NR 82 TC 7 Z9 7 U1 7 U2 49 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 2155-5435 J9 ACS CATAL JI ACS Catal. PD JAN PY 2015 VL 5 IS 1 BP 192 EP 202 DI 10.1021/cs501125n PG 11 WC Chemistry, Physical SC Chemistry GA AY3XS UT WOS:000347513400024 ER PT J AU Allen, FI Comolli, LR Kusoglu, A Modestino, MA Minor, AM Weber, AZ AF Allen, Frances I. Comolli, Luis R. Kusoglu, Ahmet Modestino, Miguel A. Minor, Andrew M. Weber, Adam Z. TI Morphology of Hydrated As-Cast Nafion Revealed through Cryo Electron Tomography SO ACS MACRO LETTERS LA English DT Article ID FUEL-CELL APPLICATIONS; PROTON-EXCHANGE MEMBRANES; X-RAY-SCATTERING; IONOMER MEMBRANES; THIN-FILMS; TRANSPORT; MICROSCOPY; SIMULATIONS; ANGLE; MICROSTRUCTURE AB Nafion is an ion-containing random copolymer used as a solid electrolyte in many electrochemical applications thanks to its remarkable ionic conductivity and mechanical stability. Understanding the mechanism of ion transport in Nafion, which depends strongly on hydration, therefore requires a complete picture of its morphology in dry and hydrated form. Here we report on a nanoscale study of dry versus hydrated as-cast 100 nm Nafion membranes using analytical transmission electron microscopy (TEM) and cryogenic TEM tomography, respectively. For the dry membrane, spherical clusters similar to 3.5 nm in diameter corresponding to the hydrophilic sulfonic-acid-containing phase are identified. In contrast, cryo TEM tomography of the hydrated membrane reveals an interconnected channel-type network, with a domain spacing of similar to 5 nm, and presents the first nanoscale 3D views of the internal structure of hydrated Nafion obtained by a direct-imaging approach. C1 [Allen, Frances I.; Minor, Andrew M.] Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA. [Modestino, Miguel A.] Univ Calif Berkeley, Dept Chem & Biomol Engn, Berkeley, CA 94720 USA. [Allen, Frances I.; Minor, Andrew M.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mol Foundry, Natl Ctr Electron Microscopy, Berkeley, CA 94720 USA. [Comolli, Luis R.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Life Sci, Berkeley, CA 94720 USA. [Kusoglu, Ahmet; Weber, Adam Z.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. RP Allen, FI (reprint author), Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA. EM fiallen@lbl.gov RI Foundry, Molecular/G-9968-2014; OI Kusoglu, Ahmet/0000-0002-2761-1050 FU Fuel Cell Technologies Office, of the U.S. Department of Energy [DE-AC02-05CH11231]; Office of Science, Office of Basic Energy Sciences, Scientific User Facilities Division, of the U.S. Department of Energy [DE-AC02-05CH11231]; Electron Microscopy of Soft Matter Program - Office of Science, Office of Basic Energy Sciences, Materials Science and Engineering Division, of the U.S. Department of Energy [DE-AC02-05CH11231] FX This work was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Fuel Cell Technologies Office, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. Analytical TEM and portions of the cryo TEM studies were performed at the Molecular Foundry, and the SAXS experiments were performed at the Advanced Light Source (ALS) Beamline 7.3.3, both of which are supported by the Office of Science, Office of Basic Energy Sciences, Scientific User Facilities Division, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. A.M.M. acknowledges support from the Electron Microscopy of Soft Matter Program supported by the Director, Office of Science, Office of Basic Energy Sciences, Materials Science and Engineering Division, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. The authors thank Karen Bustillo for assistance with the XEDS measurements, and Arun Persaud, Alexander Hexemer, and Singanallur Venkatakrishnan for valuable discussions. NR 35 TC 20 Z9 20 U1 6 U2 63 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 2161-1653 J9 ACS MACRO LETT JI ACS Macro Lett. PD JAN PY 2015 VL 4 IS 1 BP 1 EP 5 DI 10.1021/mz500606h PG 5 WC Polymer Science SC Polymer Science GA AZ6OR UT WOS:000348339300003 ER PT J AU Hur, SM Khaira, GS Ramirez-Hernandez, A Muller, M Nealey, PF de Pablo, JJ AF Hur, Su-Mi Khaira, Gurdaman S. Ramirez-Hernandez, Abelardo Mueller, Marcus Nealey, Paul F. de Pablo, Juan J. TI Simulation of Defect Reduction in Block Copolymer Thin Films by Solvent Annealing SO ACS MACRO LETTERS LA English DT Article ID PHASE-BEHAVIOR; MICROPHASE SEPARATION; DILUTION APPROXIMATION; VARYING SELECTIVITY; POLYMER-SOLUTIONS; MORPHOLOGY; PATTERNS; MIXTURES; CRYSTALS AB Solvent annealing provides an effective means to control the self-assembly of block copolymer (BCP) thin films. Multiple effects, including swelling, shrinkage, and morphological transitions, act in concert to yield ordered or disordered structures. The current understanding of these processes is limited; by relying on a theoretically informed coarse-grained model of block copolymers, a conceptual framework is presented that permits prediction and rationalization of experimentally observed behaviors. Through proper selection of several process conditions, it is shown that a narrow window of solvent pressures exists over which one can direct a BCP material to form well-ordered, defect-free structures. C1 [Hur, Su-Mi; Khaira, Gurdaman S.; Ramirez-Hernandez, Abelardo; Nealey, Paul F.; de Pablo, Juan J.] Argonne Natl Lab, Div Mat Sci, Argonne, IL 60439 USA. [Hur, Su-Mi; Ramirez-Hernandez, Abelardo; Nealey, Paul F.; de Pablo, Juan J.] Univ Chicago, Inst Mol Engn, Chicago, IL 60637 USA. [Mueller, Marcus] Univ Gottingen, Inst Theoret Phys, D-37077 Gottingen, Germany. RP de Pablo, JJ (reprint author), Argonne Natl Lab, Div Mat Sci, 9700 S Cass Ave, Argonne, IL 60439 USA. EM depablo@uchicago.edu RI Ramirez-Hernandez, Abelardo/A-1717-2011; Muller, Marcus/B-9898-2009 OI Ramirez-Hernandez, Abelardo/0000-0002-3569-5223; Muller, Marcus/0000-0002-7472-973X FU U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences-Materials Science; European Union [619793] FX This work is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences-Materials Science. Additional support by the Semiconductor Research Corporation for development of fast simulation codes is gratefully acknowledged. M.M. received financial support by the European Union FP7 under Grant Agreement 619793 CoLiSA.MMP. We are grateful for valuable computing resources provided on Blues, a high-performance computing cluster operated by the Laboratory Computing Resource Center at Argonne National Laboratory, for resources provided by the Midway Research Computing Center at the University of Chicago, and by an INCITE Award at Argonne National Laboratory. NR 43 TC 21 Z9 21 U1 14 U2 83 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 2161-1653 J9 ACS MACRO LETT JI ACS Macro Lett. PD JAN PY 2015 VL 4 IS 1 BP 11 EP 15 DI 10.1021/mz500705q PG 5 WC Polymer Science SC Polymer Science GA AZ6OR UT WOS:000348339300005 ER PT J AU Thurber, CM Xu, YW Myers, JC Lodge, TP Macosko, CW AF Thurber, Christopher M. Xu, Yuewen Myers, Jason C. Lodge, Timothy P. Macosko, Christopher W. TI Accelerating Reactive Compatibilization of PE/PLA Blends by an Interfacially Localized Catalyst SO ACS MACRO LETTERS LA English DT Article ID POLYETHYLENE/POLY(METHYL METHACRYLATE) BLENDS; SURFACTANT-COMBINED CATALYST; POLYMER-POLYMER INTERFACES; IN-SITU COMPATIBILIZATION; ADHESION; COPOLYMERS; ACID; WATER; TRANSESTERIFICATION; POLYPROPYLENE AB We show catalyst localized at the interface can compatibilize polyethylene (PE) and polylactide (PLA) blends. Telechelic hydroxyl functional PE was synthesized by ring opening metathesis polymerization, which reacted with PLA in melt mixing (shown by adhesion and droplet size reduction). Lewis acid tin catalysts were examined as interfacial reaction promoters, with the goal of interfacial localization. Stannous octoate was shown to localize at the interface by transmission electron microscopy with energy dispersive X-ray spectroscopy and improved dispersion of PLA in PE as compared to uncatalyzed materials and a nonlocalized tin chloride dihydrate. C1 [Thurber, Christopher M.; Lodge, Timothy P.; Macosko, Christopher W.] Univ Minnesota, Dept Chem Engn & Mat Sci, Minneapolis, MN 55414 USA. [Lodge, Timothy P.] Univ Minnesota, Dept Chem, Minneapolis, MN 55414 USA. [Xu, Yuewen] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. [Myers, Jason C.] Univ Minnesota, Characterizat Facil, Minneapolis, MN 55455 USA. RP Lodge, TP (reprint author), Univ Minnesota, Dept Chem Engn & Mat Sci, Minneapolis, MN 55414 USA. EM lodge@umn.edu; macosko@umn.edu FU Dow Chemical Company; NSF through MRSEC program FX This work was supported by the Dow Chemical Company. The authors would like to thank Dr. Craig Silvis for helpful input in preparation of this work. Parts of this work were carried receives partial support from NSF through the MRSEC program. NR 48 TC 15 Z9 15 U1 5 U2 31 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 2161-1653 J9 ACS MACRO LETT JI ACS Macro Lett. PD JAN PY 2015 VL 4 IS 1 BP 30 EP 33 DI 10.1021/mz500770y PG 4 WC Polymer Science SC Polymer Science GA AZ6OR UT WOS:000348339300009 ER PT J AU Cho, ES Evans, CM Davidson, EC Hoarfrost, ML Modestino, MA Segalman, RA Urban, JJ AF Cho, Eun Seon Evans, Christopher M. Davidson, Emily C. Hoarfrost, Megan L. Modestino, Miguel A. Segalman, Rachel A. Urban, Jeffrey J. TI Enhanced Water Vapor Blocking in Transparent Hybrid Polymer-Nanocrystal Films SO ACS MACRO LETTERS LA English DT Article ID ASYMMETRIC DIBLOCK COPOLYMERS; BARRIER FILMS; COMPOSITE; MIXTURES; SIZE AB Highly transparent and effective encapsulating materials have become increasingly important for photovoltaic (PV) modules to prevent water vapor molecules from permeating PV cells. The composite consists of block copolymer (PS-b-P2VP), comprised of hydrophobic and hydrophilic parts, and hygroscopic nanocrystals (Magnesium Oxide, MgO) incorporated to enhance water vapor blocking by both presenting obstacles for mass transport and also scavenging water molecules. The water vapor transmission rate (WVTR) values were reduced similar to 3000 times, compared to homopolymer (PS), for both polymer and composite samples. Achieving both high transparency and low WVTR, it is expected that the composite materials can function as an excellent water vapor blocking layer for PV modules. C1 [Cho, Eun Seon; Urban, Jeffrey J.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Mol Foundry, Berkeley, CA 94720 USA. [Evans, Christopher M.; Davidson, Emily C.; Segalman, Rachel A.] Univ Calif Santa Barbara, Dept Chem Engn, Santa Barbara, CA 93106 USA. [Davidson, Emily C.; Hoarfrost, Megan L.; Modestino, Miguel A.] Univ Calif Berkeley, Dept Chem & Biomol Engn, Berkeley, CA 94720 USA. RP Urban, JJ (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Mol Foundry, Berkeley, CA 94720 USA. EM jjurban@lbl.gov RI Foundry, Molecular/G-9968-2014; Cho, Eun Seon/D-2658-2017 FU Department of Energy (DOE) through Bay Area Photovoltaic Consortium (BAPVC) [DE-EE0004946]; US-India Partnership to Advance Clean Energy-Research (PACE-R); United States (SERIIUS) - U.S. Department of Energy (Office of Science, Office of Basic Energy Sciences, and Energy Efficiency and Renewable Energy, Solar Energy Technology Program) [DE-AC36-08G028308]; United States (SERIIUS) - Government of India through Department of Science and Technology under IUSSTF/JCERDC-SERIIUS [DE-AC36-08G028308]; Office of Science, Office of Basic Energy Sciences of the U.S. Department of Energy [DE-AC02-05CH11231]; Department of Energy [DE-FG07ER46426]; Bay Area Photovoltaic Consortium (BAPVC) under Sunshot Initiative of DOE; Joint Clean Energy Research and Development Center (JCERDC) - DOE; NSF [NSF-DMR-1206296]; Joint Center for Artificial Photosynthesis (JCAP), DOE Energy Innovation Hub through Office of Science of the U.S. Department of Energy [DE-SC0004993]; Office of Science, Office of Basic Energy Sciences at the U.S. Department of Energy (DOE) FX This material is based upon work supported by the Department of Energy (DOE) through the Bay Area Photovoltaic Consortium (BAPVC) under Award Number DE-EE0004946 and also in part under the US-India Partnership to Advance Clean Energy-Research (PACE-R) for the Solar Energy Research Institute for India and the United States (SERIIUS), funded jointly by the U.S. Department of Energy (Office of Science, Office of Basic Energy Sciences, and Energy Efficiency and Renewable Energy, Solar Energy Technology Program, under Subcontract DE-AC36-08G028308 to the National Renewable Energy Laboratory, Golden, Colorado) and the Government of India, through the Department of Science and Technology under Subcontract IUSSTF/JCERDC-SERIIUS/2012 dated 22nd Nov. 2012. Work at the Molecular Foundry was supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. J.J.U. and R.A.S. conceived of and designed the experiments. E.S.C. performed the materials integration and characterization, supported by Department of Energy Grant no. DE-FG07ER46426, by the Bay Area Photovoltaic Consortium (BAPVC), funded under the Sunshot Initiative of DOE. E.S.C. performed WVTR work using support from the Joint India-US research consortium funded under the Joint Clean Energy Research and Development Center (JCERDC) supported by DOE. E.C.D. and M.L.H were funded by NSF grant no. NSF-DMR-1206296. Polymers were provided by C.M.E. and M.L.H., and SAXS measurements were performed by E.C.D. and M.A.M, supported by the Joint Center for Artificial Photosynthesis (JCAP), a DOE Energy Innovation Hub, supported through the Office of Science of the U.S. Department of Energy under Award Number DE-SC0004993. Work at the Molecular Foundry was supported by the Office of Science, Office of Basic Energy Sciences, at the U.S. Department of Energy (DOE). SAXS measurements were performed at beamline 7.3.3 of the Advanced Light Source (ALS) at Lawrence Berkeley National Laboratory (LBNL) and at beamline 1-5 at Stanford Synchrotron Radiation Laboratory (SSRL). The authors are grateful to Dr. Chris Tassone at SSRL. Also, the authors sincerely appreciate Dr. Tom Mates for assisting SIMS and discussing data analysis and Dr. Jason Forster for ellipsometer. The authors greatly thank Dupont Teijin Films for providing the PET substrate. NR 24 TC 6 Z9 6 U1 5 U2 27 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 2161-1653 J9 ACS MACRO LETT JI ACS Macro Lett. PD JAN PY 2015 VL 4 IS 1 BP 70 EP 74 DI 10.1021/mz500765y PG 5 WC Polymer Science SC Polymer Science GA AZ6OR UT WOS:000348339300017 ER PT J AU Chen, MJ Tompson, AFB Mellors, RJ Abdalla, O AF Chen, Mingjie Tompson, Andrew F. B. Mellors, Robert J. Abdalla, Osman TI An efficient optimization of well placement and control for a geothermal prospect under geological uncertainty SO APPLIED ENERGY LA English DT Article DE Geothermal; Surrogate; Optimization; Uncertainty; Sensitivity ID METAMODELING TECHNIQUES; DESIGN OPTIMIZATION; MODELS AB This study applies an efficient optimization technique based on a multivariate adaptive regression spline (MARS) technique to determine the optimal design and engineering of a potential geothermal production operation at a prospect near Superstition Mountain in Southern California, USA. The faster MARS-based statistical model is used as a surrogate for higher-fidelity physical models within the intensive optimization process. Its use allows for the exploration of the impacts of specific engineering design parameters in the context of geologic uncertainty as a means to both understand and maximize profitability of the production operation. The MARS model is initially developed from a training dataset generated by a finite set of computationally complex hydrothermal models applied to the prospect. Its application reveals that the optimal engineering design variables can differ considerably assuming different choices of hydrothermal flow properties, which, in turn, indicates the importance of reducing the uncertainty of key geologic properties. The major uncertainty sources in the natural-system are identified and ranked first by an efficient MARS-enabled total order sensitivity quantification, which is then used to assist evaluating the effect of geological uncertainties on optimized results. At the Southern California prospect, this parameter sensitivity analysis suggests that groundwater circulation through high permeable structures, rather than heat conduction through impermeable granite, is the primary heat transfer method during geothermal extraction. Reservoir histories simulated using optimal parameters with different constraints are analyzed and compared to investigate the longevity and maximum profit of the geothermal resources. The comparison shows that the longevity and profit are very likely to be overestimated by optimizations without appropriate constraints on natural conditions. In addition to geothermal energy production, this optimization approach can also be used to manage other geologic resource operations, such as hydrocarbon production or CO2 sequestration, under uncertain reservoir conditions. (C) 2014 Elsevier Ltd. All rights reserved. C1 [Chen, Mingjie; Tompson, Andrew F. B.; Mellors, Robert J.] Lawrence Livermore Natl Lab, Atmospher Earth & Energy Div, Livermore, CA USA. [Chen, Mingjie; Abdalla, Osman] Sultan Qaboos Univ, Water Res Ctr, Al Khoud, Oman. RP Chen, MJ (reprint author), Sultan Qaboos Univ, Water Res Ctr, POB 17,PC 123, Al Khoud, Oman. EM cmj1014@yahoo.com RI Mellors, Robert/K-7479-2014; OI Mellors, Robert/0000-0002-2723-5163; Abdalla, Osman/0000-0001-5150-416X FU U.S. Department of Energy by Lawrence Livermore National Laboratory [DE-AC52-07NA27344]; DOE GTO office [DE-EE24675] FX This work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under contract DE-AC52-07NA27344. We would like to thank DOE GTO office for supporting this project under award DE-EE24675. We also appreciate the Navy geothermal program for providing data. We also appreciate the valuable comments from the anonymous reviewers and associated editor, which substantially improved the final paper. NR 31 TC 2 Z9 2 U1 3 U2 23 PU ELSEVIER SCI LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, OXON, ENGLAND SN 0306-2619 EI 1872-9118 J9 APPL ENERG JI Appl. Energy PD JAN 1 PY 2015 VL 137 BP 352 EP 363 DI 10.1016/j.apenergy.2014.10.036 PG 12 WC Energy & Fuels; Engineering, Chemical SC Energy & Fuels; Engineering GA AZ1NY UT WOS:000348006700034 ER PT J AU Steen, D Stadler, M Cardoso, G Groissbock, M DeForest, N Marnay, C AF Steen, David Stadler, Michael Cardoso, Goncalo Groissboeck, Markus DeForest, Nicholas Marnay, Chris TI Modeling of thermal storage systems in MILP distributed energy resource models SO APPLIED ENERGY LA English DT Article DE Distributed energy resources; Investment planning; Renewables; Energy optimization; Thermal energy storage ID PHASE-CHANGE MATERIALS; ABSORPTION CHILLERS; HEAT; TANKS; BUILDINGS; OPERATION; PLANTS AB Thermal energy storage (TES) and distributed generation technologies, such as combined heat and power (CHP) or photovoltaics (PV), can be used to reduce energy costs and decrease CO2 emissions from buildings by shifting energy consumption to times with less emissions and/or lower energy prices. To determine the feasibility of investing in TES in combination with other distributed energy resources (DER), mixed integer linear programming (MILP) can be used. Such a MILP model is the well-established Distributed Energy Resources Customer Adoption Model (DER-CAM); however, it currently uses only a simplified TES model to guarantee linearity and short run-times. Loss calculations are based only on the energy contained in the storage. This paper presents a new DER-CAM TES model that allows improved tracking of losses based on ambient and storage temperatures, and compares results with the previous version. A multi-layer TES model is introduced that retains linearity and avoids creating an endogenous optimization problem. The improved model increases the accuracy of the estimated storage losses and enables use of heat pumps for low temperature storage charging. Results indicate that the previous model overestimates the attractiveness of TES investments for cases without possibility to invest in heat pumps and underestimates it for some locations when heat pumps are allowed. Despite a variation in optimal technology selection between the two models, the objective function value stays quite stable, illustrating the complexity of optimal DER sizing problems in buildings and microgrids. Published by Elsevier Ltd. C1 [Steen, David; Stadler, Michael; Cardoso, Goncalo; Groissboeck, Markus; DeForest, Nicholas; Marnay, Chris] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Steen, David] Chalmers, Environm & Energy Dept, SE-41296 Gothenburg, Sweden. [Stadler, Michael; Groissboeck, Markus] Ctr Energy & Innovat Technol CET, A-3681 Hofamt Priel, Austria. [Cardoso, Goncalo] Univ Lisbon, Inst Super Tecn, P-1049001 Lisbon, Portugal. RP Steen, D (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, 1 Cyclotron Rd MS 90R1121, Berkeley, CA 94720 USA. EM david.steen@chalmers.se; MStadler@lbl.gov FU Office of Electricity Delivery and Energy Reliability; U.S. Department of Energy [DE-AC02-05CH11231] FX DER-CAM has been funded partly by the Office of Electricity Delivery and Energy Reliability, Distributed Energy Program of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. The Distributed Energy Resources Customer Adoption Model (DER-CAM) has been designed at Lawrence Berkeley National Laboratory (LBNL). Furthermore, Chalmers Energy Initiative is greatly acknowledged for funding D. Steen's guest research visit to Lawrence Berkeley National Laboratory. NR 40 TC 16 Z9 16 U1 5 U2 21 PU ELSEVIER SCI LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, OXON, ENGLAND SN 0306-2619 EI 1872-9118 J9 APPL ENERG JI Appl. Energy PD JAN 1 PY 2015 VL 137 BP 782 EP 792 DI 10.1016/j.apenergy.2014.07.036 PG 11 WC Energy & Fuels; Engineering, Chemical SC Energy & Fuels; Engineering GA AZ1NY UT WOS:000348006700073 ER PT J AU Loverro, KL Brown, TN Coyne, ME Schiffman, JM AF Loverro, Kari L. Brown, Tyler N. Coyne, Megan E. Schiffman, Jeffrey M. TI Use of body armor protection with fighting load impacts soldier performance and kinematics SO APPLIED ERGONOMICS LA English DT Article DE Torso load; Gait; Obstacle negotiation ID JOINT COORDINATE SYSTEM; WALKING PATTERNS; CARRIAGE; PARAMETERS; MOTION; STABILITY; GAIT; HIP AB The purpose of this evaluation was to examine how increasing body armor protection with and without a fighting load impacted soldiers' performance and mobility. Thirteen male soldiers performed one performance (repeated 30-m rushing) and three mobility tasks (walk, walk over and walk under) with three different body armor configurations and an anterior fighting load. Increasing body armor protection, decreased soldier performance, as individual and total 30-m rush times were significantly longer with greater protection. While increasing body armor protection had no impact on mobility, i.e. significant effect on trunk and lower limb biomechanics, during the walk and walk over tasks, greater protection did significantly decrease maximum trunk flexion during the walk under task. Adding fighting load may negatively impact soldier mobility, as greater maximum trunk extension was evident during the walk and walk over tasks, and decreased maximum trunk flexion exhibited during the walk under task with the fighting load. (C) 2014 Elsevier Ltd and The Ergonomics Society. All rights reserved. C1 [Loverro, Kari L.; Brown, Tyler N.; Coyne, Megan E.; Schiffman, Jeffrey M.] US Army Natick Soldier Res Dev & Res Ctr, Natick, MA USA. [Loverro, Kari L.] Oak Ridge Inst Sci & Educ ORISE, Belcamp, MD USA. [Schiffman, Jeffrey M.] Liberty Mutual Res Inst Safety, Hopkinton, MA USA. RP Loverro, KL (reprint author), Natick Soldier Res Dev & Engn Ctr, 15 Kansas St R332, Natick, MA 01760 USA. EM kari.l.loverro.ctr@mail.mil NR 31 TC 5 Z9 6 U1 2 U2 21 PU ELSEVIER SCI LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, OXON, ENGLAND SN 0003-6870 EI 1872-9126 J9 APPL ERGON JI Appl. Ergon. PD JAN PY 2015 VL 46 BP 168 EP 175 DI 10.1016/j.apergo.2014.07.015 PN A PG 8 WC Engineering, Industrial; Ergonomics; Psychology, Applied SC Engineering; Psychology GA AY7JO UT WOS:000347736900020 PM 25151315 ER PT J AU Manard, BT Konegger-Kappel, S Gonzalez, JJ Chirinos, J Dong, MR Mao, XL Marcus, RK Russo, RE AF Manard, Benjamin T. Konegger-Kappel, Stefanie Gonzalez, Jhanis J. Chirinos, Jose Dong, Meirong Mao, Xianglei Marcus, R. Kenneth Russo, Richard E. TI Liquid Sampling-Atmospheric Pressure Glow Discharge as a Secondary Excitation Source for Laser Ablation-Generated Aerosols: Parametric Dependence and Robustness to Particle Loading SO APPLIED SPECTROSCOPY LA English DT Article DE Liquid sampling-atmospheric pressure glow discharge; LS-APGD; Laser ablation; Optical emission spectroscopy; Excitation conditions; Robustness; Particle loading ID INDUCTIVELY-COUPLED PLASMA; ATOMIC EMISSION-SPECTROMETRY; ICP-MS MEASUREMENTS; ANALYTICAL-CHEMISTRY; SPECTROSCOPY; MEDIA AB Liquid sampling-atmospheric pressure glow discharge (LS-APGD) microplasma is being developed as a secondary vaporization-excitation source for the optical emission analysis of laser ablation (LA)-generated particle populations. The practicalities of this coupling are evaluated by determining the influence of source parameters on the emission response and the plasma's robustness upon LA introduction of easily ionized elements (EIEs). The influence of discharge current (45-70 mA), LA carrier gas flow rate (0.1-0.8 L min(-1)), and electrode separation distance (0.5-3.5 mm) was studied by measuring Cu emission lines after ablation of a brass sample. Best emission responses were observed for high-discharge currents, low He carrier gas flow rates, and relatively small (<1.5 mm) electrode gaps. Plasma robustness and spectroscopic matrix effects were studied by monitoring Mg(II): Mg(I) intensity ratios and N-2-derived plasma rotational temperatures after the ablation of Sr- and Ca-containing pellets. Plasma robustness investigations showed that the plasma is not appreciably affected by the particle loadings, with the microplasma being slightly more ionizing in the case of Ca introduction. In neither case did the concentration of the concomitant element change the robustness values, implying a high level of robustness. Introduction of the LA particles results in slight increases in the rotational temperatures (similar to 10% relative), with Ca-containing particles having a greater effect than Sr-containing particles. The observed variation of 9% in the plasma rotational temperature is in the same order of magnitude as the short-term reproducibility determined by the proposed LA-LS-APGD system. The determined rotational temperatures ranged from 1047 to 1212 K upon introducing various amounts of Ca and Sr. The relative immunity to LA particle-induced matrix effects is attributed to the relatively long residence times and high power densities (>10 W mm(-3)) of the LS-APGD microplasma. C1 [Manard, Benjamin T.; Konegger-Kappel, Stefanie; Marcus, R. Kenneth] Clemson Univ, Dept Chem, Clemson, SC 29634 USA. [Manard, Benjamin T.; Gonzalez, Jhanis J.; Chirinos, Jose; Dong, Meirong; Mao, Xianglei; Russo, Richard E.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Marcus, RK (reprint author), Clemson Univ, Dept Chem, Biosyst Res Complex,51 New Cherry St, Clemson, SC 29634 USA. EM marcusr@clemson.edu FU U.S. Department of Energy [DE-AC02-05CH11231] FX This work was supported by the Director, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, and the Deputy Administrator for Defense Nuclear Nonproliferation, Assistant Deputy Administrator for Nonproliferation Research and Development of the U.S. Department of Energy under contract DE-AC02-05CH11231. NR 35 TC 5 Z9 5 U1 2 U2 8 PU SOC APPLIED SPECTROSCOPY PI FREDERICK PA 5320 SPECTRUM DRIVE SUITE C, FREDERICK, MD 21703 USA SN 0003-7028 EI 1943-3530 J9 APPL SPECTROSC JI Appl. Spectrosc. PD JAN PY 2015 VL 69 IS 1 BP 58 EP 66 DI 10.1366/14-07585 PG 9 WC Instruments & Instrumentation; Spectroscopy SC Instruments & Instrumentation; Spectroscopy GA AY7MY UT WOS:000347745300008 PM 25506884 ER PT J AU Bleem, LE Stalder, B Brodwin, M Busha, MT Gladders, MD High, FW Rest, A Wechsler, RH AF Bleem, L. E. Stalder, B. Brodwin, M. Busha, M. T. Gladders, M. D. High, F. W. Rest, A. Wechsler, R. H. TI A NEW REDUCTION OF THE BLANCO COSMOLOGY SURVEY: AN OPTICALLY SELECTED GALAXY CLUSTER CATALOG AND A PUBLIC RELEASE OF OPTICAL DATA PRODUCTS SO ASTROPHYSICAL JOURNAL SUPPLEMENT SERIES LA English DT Article DE galaxies: clusters: general; surveys; techniques: photometric ID SOUTH-POLE TELESCOPE; DIGITAL SKY SURVEY; 720 SQUARE DEGREES; X-RAY; PHOTOMETRIC REDSHIFTS; LUMINOSITY FUNCTION; SCALING RELATIONS; RICH CLUSTERS; STELLAR LOCUS; FIELD SURVEY AB The Blanco Cosmology Survey is a four-band (griz) optical-imaging survey of similar to 80 deg(2) of the southern sky. The survey consists of two fields centered approximately at (R.A., decl.) = (23(h), -55 degrees) and (5(h)30(m), -53 degrees) with imaging sufficient for the detection of L-star galaxies at redshift z <= 1. In this paper, we present our reduction of the survey data and describe a new technique for the separation of stars and galaxies. We search the calibrated source catalogs for galaxy clusters at z <= 0.75 by identifying spatial over-densities of red-sequence galaxies and report the coordinates, redshifts, and optical richnesses, lambda , for 764 galaxy clusters at z <= 0.75. This sample, >85% of which are new discoveries, has a median redshift of z = 0.52 and median richness lambda (0.4L L-star) = 16.4. Accompanying this paper we also release full survey data products including reduced images and calibrated source catalogs. These products are available at http://data.rcc.uchicago.edu/dataset/blanco-cosmology-survey. C1 [Bleem, L. E.] Argonne Natl Lab, Argonne, IL 60439 USA. [Bleem, L. E.; Gladders, M. D.; High, F. W.] Univ Chicago, Kavli Inst Cosmol Phys, Chicago, IL 60637 USA. [Stalder, B.] Harvard Smithsonian Ctr Astrophys, Cambridge, MA 02138 USA. [Brodwin, M.] Univ Missouri, Dept Phys & Astron, Kansas City, MO 64110 USA. [Busha, M. T.; Wechsler, R. H.] Stanford Univ, Kavli Inst Particle Astrophys & Cosmol, Stanford, CA 94305 USA. [Busha, M. T.; Wechsler, R. H.] SLAC Natl Accelerator Lab, Menlo Pk, CA 94025 USA. [Gladders, M. D.; High, F. W.] Univ Chicago, Dept Astron & Astrophys, Chicago, IL 60637 USA. [Rest, A.] Space Telescope Sci Inst, Baltimore, MD 21218 USA. [Wechsler, R. H.] Stanford Univ, Dept Phys, Stanford, CA 94305 USA. RP Bleem, LE (reprint author), Argonne Natl Lab, 9700 S Cass Ave, Argonne, IL 60439 USA. FU U.S. Department of Energy, Basic Energy Sciences, Office of Science [DE-AC02-06CH11357]; NSF Physics Frontier Center [PHY-0551142]; NSF [ANT-0638937, AST-1009649, MRI-0723073] FX The authors thank Michael Huff for assistance with flagging spurious objects in the source catalogs and Doug Rudd for his assistance setting up the online data access. L.B. thanks Tom Crawford for useful discussions. L.B. acknowledges support by the U.S. Department of Energy, Basic Energy Sciences, Office of Science, under Contract No. DE-AC02-06CH11357, the NSF Physics Frontier Center award PHY-0551142, and the NSF OPP award ANT-0638937. Galaxy cluster research at SAO is supported in part by NSF grants AST-1009649 and MRI-0723073. This research draws on data provided by NOAO PI 2005B-0043 as distributed by the NOAO Science Archive. NOAO is operated by the Association of Universities for Research in Astronomy (AURA), Inc. under a cooperative agreement with the National Science Foundation. Characterization of the new star-galaxy classifier was based on both data from both AEGIS (a multi-wavelength sky survey conducted with the Chandra, GALEX, Hubble, Keck, CFHT, MMT, Subaru, Palomar, Spitzer, VLA, and other telescopes and supported in part by the NSF, NASA, and the STFC) and on observations obtained with MegaPrime/MegaCam, a joint project of CFHT and CEA/DAPNIA, at the Canada-France-Hawaii Telescope (CFHT) which is operated by the National Research Council (NRC) of Canada, the Institut National des Science de l'Univers of the Centre National de la Recherche Scientifique (CNRS) of France, and the University of Hawaii. This work is based in part on data products produced at the Canadian Astronomy Data Centre as part of the Canada-France-Hawaii Telescope Legacy Survey, a collaborative project of NRC and CNRS. Additionally, this research has made use of the SIMBAD database, operated at CDS, Strasbourg, France. Finally, the authors acknowledge the University of Chicago Research Computing Center for hosting the data products presented in this work. NR 70 TC 10 Z9 10 U1 0 U2 1 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 0067-0049 EI 1538-4365 J9 ASTROPHYS J SUPPL S JI Astrophys. J. Suppl. Ser. PD JAN PY 2015 VL 216 IS 1 AR 20 DI 10.1088/0067-0049/216/1/20 PG 18 WC Astronomy & Astrophysics SC Astronomy & Astrophysics GA AZ3LR UT WOS:000348129600020 ER PT J AU Boyer, ML McQuinn, KBW Barmby, P Bonanos, AZ Gehrz, RD Gordon, KD Groenewegen, MAT Lagadec, E Lennon, D Marengo, M Meixner, M Skillman, E Sloan, GC Sonneborn, G van Loon, JT Zijlstra, A AF Boyer, Martha L. McQuinn, Kristen B. W. Barmby, Pauline Bonanos, Alceste Z. Gehrz, Robert D. Gordon, Karl D. Groenewegen, M. A. T. Lagadec, Eric Lennon, Daniel Marengo, Massimo Meixner, Margaret Skillman, Evan Sloan, G. C. Sonneborn, George van Loon, Jacco Th. Zijlstra, Albert TI AN INFRARED CENSUS OF DUST IN NEARBY GALAXIES WITH SPITZER (DUSTINGS). I. OVERVIEW SO ASTROPHYSICAL JOURNAL SUPPLEMENT SERIES LA English DT Article DE galaxies: dwarf; galaxies: photometry; galaxies: stellar content; infrared: stars; Local Group; stars: AGB and post-AGB; stars: mass-loss; stars: winds, outflows ID LARGE-MAGELLANIC-CLOUD; GIANT BRANCH STARS; DWARF IRREGULAR GALAXIES; YOUNG STELLAR OBJECTS; LOCAL GROUP DWARFS; RICH AGB-STARS; MU-M RANGE; LOW-METALLICITY; EVOLVED STARS; MASS-LOSS AB Nearby resolved dwarf galaxies provide excellent opportunities for studying the dust-producing late stages of stellar evolution over a wide range of metallicity (-2.7 less than or similar to [Fe/H] less than or similar to -1.0). Here, we describe DUSTiNGS (DUST in Nearby Galaxies with Spitzer): a 3.6 and 4.5 mu m post-cryogen Spitzer Space Telescope imaging survey of 50 dwarf galaxies within 1.5 Mpc that is designed to identify dust-producing asymptotic giant branch (AGB) stars and massive stars. The survey includes 37 dwarf spheroidal, 8 dwarf irregular, and 5 transition-type galaxies. This near-complete sample allows for the building of statistics on these rare phases of stellar evolution over the full metallicity range. The photometry is >75% complete at the tip of the red giant branch for all targeted galaxies, with the exception of the crowded inner regions of IC 10, NGC 185, and NGC 147. This photometric depth ensures that the majority of the dust-producing stars, including the thermally pulsing AGB stars, are detected in each galaxy. The images map each galaxy to at least twice the half-light radius to ensure that the entire evolved star population is included and to facilitate the statistical subtraction of background and foreground contamination, which is severe at these wavelengths. In this overview, we describe the survey, the data products, and preliminary results. We show evidence for the presence of dust-producing AGB stars in eight of the targeted galaxies, with metallicities as low as [Fe/H] = -1.9, suggesting that dust production occurs even at low metallicity. C1 [Boyer, Martha L.; Sonneborn, George] NASA, Goddard Space Flight Ctr, Observat Cosmol Lab, Greenbelt, MD 20771 USA. [Boyer, Martha L.] Oak Ridge Associated Univ, Oak Ridge, TN 37831 USA. [McQuinn, Kristen B. W.; Gehrz, Robert D.; Skillman, Evan] Univ Minnesota, Sch Phys & Astron, Minnesota Inst Astrophys, Minneapolis, MN 55455 USA. [Barmby, Pauline] Univ Western Ontario, Dept Phys & Astron, London, ON N6A 3K7, Canada. [Bonanos, Alceste Z.] Natl Observ Athens, IAASARS, GR-15236 Penteli, Greece. [Gordon, Karl D.; Meixner, Margaret] STScI, Baltimore, MD 21218 USA. [Groenewegen, M. A. T.] Royal Observ Belgium, B-1180 Brussels, Belgium. [Lagadec, Eric] Univ Nice Sophia Antipolis, CNRS, Observ Cote Azur, Lab Lagrange,UMR7293, F-06300 Nice, France. [Lennon, Daniel] European Space Astron Ctr, ESA, E-28691 Madrid, Spain. [Marengo, Massimo] Iowa State Univ, Dept Phys & Astron, Ames, IA 50011 USA. [Sloan, G. C.] Cornell Univ, Dept Astron, Ithaca, NY 14853 USA. [van Loon, Jacco Th.] Keele Univ, Lennard Jones Labs, Astrophys Grp, Keele ST5 5BG, Staffs, England. [Zijlstra, Albert] Univ Manchester, Jodrell Bank Ctr Astrophys, Manchester M13 9PL, Lancs, England. RP Boyer, ML (reprint author), NASA, Goddard Space Flight Ctr, Observat Cosmol Lab, Code 665, Greenbelt, MD 20771 USA. EM martha.boyer@nasa.gov RI Bonanos, Alceste/K-5392-2013; Barmby, Pauline/I-7194-2016; OI Bonanos, Alceste/0000-0003-2851-1905; Barmby, Pauline/0000-0003-2767-0090; Lennon, Daniel/0000-0003-3063-4867 FU Spitzer [GO80063]; NASA Astrophysics Data Analysis Program [N3-ADAP13-0058]; NASA Postdoctoral Program at the Goddard Space Flight Center through a contract with NASA; NASA; United States Air Force; European Union (European Social Fund); National Resources under the "ARISTEIA" action of the Operational Programme "Education and Lifelong Learning" in Greece; NSF [AST-1108645] FX Many thanks to Brian Babler for very helpful discussions about IRAC photometry. We also thank the referee for helpful comments. This work is supported by Spitzer via grant GO80063 and by the NASA Astrophysics Data Analysis Program grant number N3-ADAP13-0058. M.L.B. is supported by the NASA Postdoctoral Program at the Goddard Space Flight Center, administered by ORAU through a contract with NASA. R.D.G. was supported by NASA and the United States Air Force. A.Z.B. acknowledges funding by the European Union (European Social Fund) and National Resources under the "ARISTEIA" action of the Operational Programme "Education and Lifelong Learning" in Greece. G.C.S. receives support from the NSF, award AST-1108645. NR 90 TC 12 Z9 12 U1 0 U2 3 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 0067-0049 EI 1538-4365 J9 ASTROPHYS J SUPPL S JI Astrophys. J. Suppl. Ser. PD JAN PY 2015 VL 216 IS 1 AR 10 DI 10.1088/0067-0049/216/1/10 PG 17 WC Astronomy & Astrophysics SC Astronomy & Astrophysics GA AZ3LR UT WOS:000348129600010 ER PT J AU Norman, ML Reynolds, DR So, GC Harkness, RP Wise, JH AF Norman, Michael L. Reynolds, Daniel R. So, Geoffrey C. Harkness, Robert P. Wise, John H. TI FULLY COUPLED SIMULATION OF COSMIC REIONIZATION. I. NUMERICAL METHODS AND TESTS SO ASTROPHYSICAL JOURNAL SUPPLEMENT SERIES LA English DT Article DE cosmology: theory; methods: numerical; radiative transfer ID ADAPTIVE MESH REFINEMENT; COSMOLOGICAL RADIATIVE-TRANSFER; PROBE WMAP OBSERVATIONS; FLUX-LIMITED DIFFUSION; PIECEWISE PARABOLIC METHOD; POPULATION-III STARS; HYDROGEN REIONIZATION; INTERGALACTIC MEDIUM; STELLAR SOURCES; COMPARISON PROJECT AB We describe an extension of the Enzo code to enable fully coupled radiation hydrodynamical simulation of inhomogeneous reionization in large similar to(100 Mpc)(3) cosmological volumes with thousands to millions of point sources. We solve all dynamical, radiative transfer, thermal, and ionization processes self-consistently on the same mesh, as opposed to a postprocessing approach which coarse-grains the radiative transfer. We do, however, employ a simple subgrid model for star formation which we calibrate to observations. The numerical method presented is a modification of an earlier method presented in Reynolds et al. differing principally in the operator splitting algorithm we use to advance the system of equations. Radiation transport is done in the gray flux-limited diffusion (FLD) approximation, which is solved by implicit time integration split off from the gas energy and ionization equations, which are solved separately. This results in a faster and more robust scheme for cosmological applications compared to the earlier method. The FLD equation is solved using the hypre optimally scalable geometric multigrid solver from LLNL. By treating the ionizing radiation as a grid field as opposed to rays, our method is scalable with respect to the number of ionizing sources, limited only by the parallel scaling properties of the radiation solver. We test the speed and accuracy of our approach on a number of standard verification and validation tests. We show by direct comparison with Enzo's adaptive ray tracing method Moray that the well-known inability of FLD to cast a shadow behind opaque clouds has a minor effect on the evolution of ionized volume and mass fractions in a reionization simulation validation test. We illustrate an application of our method to the problem of inhomogeneous reionization in a 80 Mpc comoving box resolved with 3200(3) Eulerian grid cells and dark matter particles. C1 [Norman, Michael L.; So, Geoffrey C.] Univ Calif San Diego, CASS, La Jolla, CA 92093 USA. [Norman, Michael L.; Harkness, Robert P.] Univ Calif San Diego, SDSC, La Jolla, CA 92093 USA. [Reynolds, Daniel R.] So Methodist Univ, Dallas, TX 75205 USA. [Harkness, Robert P.] Oak Ridge Natl Lab, NICS, Oak Ridge, TN 37831 USA. [Wise, John H.] Georgia Inst Technol, Ctr Relativist Astrophys, Atlanta, GA 30332 USA. RP Norman, ML (reprint author), Univ Calif San Diego, CASS, 9500 Gilman Dr, La Jolla, CA 92093 USA. OI Reynolds, Daniel/0000-0002-0911-7841 FU National Science Foundation [AST-0808184, AST-1109243]; NSF [AST-1211626, AST-1333360]; [AST025]; [AST033] FX This research was partially supported by National Science Foundation grants AST-0808184 and AST-1109243 to M.L.N. and D.R.R. J.H.W. acknowledges partial support by NSF grants AST-1211626 and AST-1333360. Simulations were performed on the Kraken supercomputer operated for the Extreme Science and Engineering Discovery Environment (XSEDE) by the National Institute for Computational Science (NICS), ORNL with support from XRAC allocation MCA-TG98N020 to M.L.N., as well as on the Jaguar supercomputer operated for the DOE Office of Science at the National Center for Computational Science (NCCS), ORNL with support from INCITE awards AST025 and AST033 to M.L.N. M.L.N., D.R.R., and G.S. would like to especially acknowledge the tireless devotion to this project by our co-author and dear colleague Robert Harkness, who passed away shortly before this manuscript was completed. NR 97 TC 14 Z9 14 U1 2 U2 5 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 0067-0049 EI 1538-4365 J9 ASTROPHYS J SUPPL S JI Astrophys. J. Suppl. Ser. PD JAN PY 2015 VL 216 IS 1 AR 16 DI 10.1088/0067-0049/216/1/16 PG 24 WC Astronomy & Astrophysics SC Astronomy & Astrophysics GA AZ3LR UT WOS:000348129600016 ER PT J AU Wyant, MC Bretherton, CS Wood, R Carmichael, GR Clarke, A Fast, J George, R Gustafson, WI Hannay, C Lauer, A Lin, Y Morcrette, JJ Mulcahy, J Saide, PE Spak, SN Yang, Q AF Wyant, M. C. Bretherton, C. S. Wood, R. Carmichael, G. R. Clarke, A. Fast, J. George, R. Gustafson, W. I., Jr. Hannay, C. Lauer, A. Lin, Y. Morcrette, J-J Mulcahy, J. Saide, P. E. Spak, S. N. Yang, Q. TI Global and regional modeling of clouds and aerosols in the marine boundary layer during VOCALS: the VOCA intercomparison SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID COMMUNITY ATMOSPHERE MODEL; SOUTHEAST PACIFIC STRATOCUMULUS; GENERAL-CIRCULATION MODELS; WRF-CHEM; CARBONACEOUS AEROSOL; RADIATIVE PROPERTIES; MICROPHYSICS SCHEME; SINGLE-COLUMN; CLIMATE MODEL; FOSSIL-FUEL AB A diverse collection of models are used to simulate the marine boundary layer in the southeast Pacific region during the period of the October-November 2008 VOCALS REx (VAMOS Ocean Cloud Atmosphere Land Study Regional Experiment) field campaign. Regional models simulate the period continuously in boundary-forced free-running mode, while global forecast models and GCMs (general circulation models) are run in forecast mode. The models are compared to extensive observations along a line at 20 degrees S extending westward from the South American coast. Most of the models simulate cloud and aerosol characteristics and gradients across the region that are recognizably similar to observations, despite the complex interaction of processes involved in the problem, many of which are parameterized or poorly resolved. Some models simulate the regional low cloud cover well, though many models underestimate MBL (marine boundary layer) depth near the coast. Most models qualitatively simulate the observed offshore gradients of SO2, sulfate aerosol, CCN (cloud condensation nuclei) concentration in the MBL as well as differences in concentration between the MBL and the free troposphere. Most models also qualitatively capture the decrease in cloud droplet number away from the coast. However, there are large quantitative intermodel differences in both means and gradients of these quantities. Many models are able to represent episodic offshore increases in cloud droplet number and aerosol concentrations associated with periods of offshore flow. Most models underestimate CCN (at 0.1% supersaturation) in the MBL and free troposphere. The GCMs also have difficulty simulating coastal gradients in CCN and cloud droplet number concentration near the coast. The overall performance of the models demonstrates their potential utility in simulating aerosol-cloud interactions in the MBL, though quantitative estimation of aerosol-cloud interactions and aerosol indirect effects of MBL clouds with these models remains uncertain. C1 [Wyant, M. C.; Bretherton, C. S.; Wood, R.; George, R.] Univ Washington, Dept Atmospher Sci, Seattle, WA 98195 USA. [Carmichael, G. R.; Saide, P. E.; Spak, S. N.] Univ Iowa, CGRER, Iowa City, IA USA. [Clarke, A.] Univ Hawaii Manoa, SOEST, Honolulu, HI 96822 USA. [Fast, J.; Gustafson, W. I., Jr.; Yang, Q.] Pacific NW Natl Lab, Richland, WA 99352 USA. [Hannay, C.] Natl Ctr Atmospher Res, Boulder, CO 80307 USA. [Lauer, A.] Univ Hawaii Manoa, Int Pacific Res Ctr, Honolulu, HI 96822 USA. [Lin, Y.] Geophys Fluid Dynam Lab, Princeton, NJ USA. [Morcrette, J-J] European Ctr Medium Range Weather Forecasts, Reading RG2 9AX, Berks, England. [Mulcahy, J.] Met Off, Exeter, Devon, England. RP Wyant, MC (reprint author), Univ Washington, Dept Atmospher Sci, Seattle, WA 98195 USA. EM mwyant@atmos.washington.edu RI Gustafson, William/A-7732-2008; Spak, Scott/B-7331-2008; Yang, Qing/H-3275-2011; Wood, Robert/A-2989-2008; lin, yanluan/A-6333-2015 OI Gustafson, William/0000-0001-9927-1393; Spak, Scott/0000-0002-8545-1411; Yang, Qing/0000-0003-2067-5999; Wood, Robert/0000-0002-1401-3828; FU NASA [NNX08AL05G, NNX11AI52G]; EPA [83503701]; National Center for Research Resources (NCRR), a part of the National Institutes of Health (NIH) [UL1RR024979]; Fulbright-CONICYT [15093810]; US National Oceanic and Atmospheric Administration (NOAA) Atmospheric Composition and Climate Program [NA10AANRG0083/56091]; DOE [DE-AC05-76RL01830] FX The authors wish to thank Grant Allen for his providing of aircraft data for many of the figures. Thanks also to Romain Blot for providing sea-salt measurements. Thanks to Matt Lebsock for providing CloudSat precipitation data and Dan Grosvenor for his assistance. The comments of two anonymous reviewers helped improve this paper. The portion of this work conducted at the University of Iowa was carried out with the aid of NASA grants NNX08AL05G and NNX11AI52G, EPA grant 83503701, grant number UL1RR024979 from the National Center for Research Resources (NCRR), a part of the National Institutes of Health (NIH), and Fulbright-CONICYT scholarship number 15093810. Its contents are solely the responsibility of the authors and do not necessarily represent the official views of the founding institutions. Funding for Pacific Northwest National Laboratory (PNNL) contributions to this research has been provided by the US National Oceanic and Atmospheric Administration (NOAA) Atmospheric Composition and Climate Program (NA10AANRG0083/56091). PNNL is operated for the DOE by Battelle Memorial Institute under contract no. DE-AC05-76RL01830. NR 96 TC 8 Z9 8 U1 3 U2 32 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1680-7316 EI 1680-7324 J9 ATMOS CHEM PHYS JI Atmos. Chem. Phys. PY 2015 VL 15 IS 1 BP 153 EP 172 DI 10.5194/acp-15-153-2015 PG 20 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA AZ0TQ UT WOS:000347958200010 ER PT J AU Canagaratna, MR Jimenez, JL Kroll, JH Chen, Q Kessler, SH Massoli, P Hildebrandt Ruiz, L Fortner, E Williams, LR Wilson, KR Surratt, JD Donahue, NM Jayne, JT Worsnop, DR AF Canagaratna, M. R. Jimenez, J. L. Kroll, J. H. Chen, Q. Kessler, S. H. Massoli, P. Hildebrandt Ruiz, L. Fortner, E. Williams, L. R. Wilson, K. R. Surratt, J. D. Donahue, N. M. Jayne, J. T. Worsnop, D. R. TI Elemental ratio measurements of organic compounds using aerosol mass spectrometry: characterization, improved calibration, and implications SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID HIGH-RESOLUTION; CHEMICAL-CHARACTERIZATION; ATMOSPHERIC AEROSOLS; PARTICLE COMPOSITION; HYDROXYL RADICALS; AMBIENT AEROSOL; RIVER DELTA; SECONDARY; ISOPRENE; OXIDATION AB Elemental compositions of organic aerosol (OA) particles provide useful constraints on OA sources, chemical evolution, and effects. The Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) is widely used to measure OA elemental composition. This study evaluates AMS measurements of atomic oxygen-to-carbon (O : C), hydrogen-to-carbon (H : C), and organic mass-to-organic carbon (OM : OC) ratios, and of carbon oxidation state ((OS) over bar (C))for a vastly expanded laboratory data set of multifunctional oxidized OA standards. For the expanded standard data set, the method introduced by Aiken et al. (2008), which uses experimentally measured ion intensities at all ions to determine elemental ratios (referred to here as "Aiken-Explicit"), reproduces known O: C and H: C ratio values within 20% (average absolute value of relative errors) and 12%, respectively. The more commonly used method, which uses empirically estimated H2O+ and CO+ ion intensities to avoid gas phase air interferences at these ions (referred to here as "Aiken-Ambient"), reproduces O: C and H: C of multifunctional oxidized species within 28 and 14% of known values. The values from the latter method are systematically biased low, however, with larger biases observed for alcohols and simple diacids. A detailed examination of the H2O+, CO+, and CO2+ fragments in the high-resolution mass spectra of the standard compounds indicates that the Aiken-Ambient method underestimates the CO C and especially H2O+ produced from many oxidized species. Combined AMS-vacuum ultraviolet (VUV) ionization measurements indicate that these ions are produced by dehydration and decarboxylation on the AMS vaporizer (usually operated at 600 degrees C). Thermal decomposition is observed to be efficient at vaporizer temperatures down to 200 degrees C. These results are used together to develop an "Improved-Ambient" elemental analysis method for AMS spectra measured in air. The Improved-Ambient method uses specific ion fragments as markers to correct for molecular functionality-dependent systematic biases and reproduces known O : C (H : C) ratios of individual oxidized standards within 28% (13 %) of the known molecular values. The error in Improved-Ambient O : C (H : C) values is smaller for theoretical standard mixtures of the oxidized organic standards, which are more representative of the complex mix of species present in ambient OA. For ambient OA, the Improved-Ambient method produces O : C (H : C) values that are 27% (11 %) larger than previously published Aiken-Ambient values; a corresponding increase of 9% is observed for OM : OC values. These results imply that ambient OA has a higher relative oxygen content than previously estimated. The (OS) over bar (C) values calculated for ambient OA by the two methods agree well, however (average relative difference of 0.06 (OS) over bar (C) units). This indicates that (OS) over bar (C) is a more robust metric of oxidation than O : C, likely since (OS) over bar (C) is not affected by hydration or dehydration, either in the atmosphere or during analysis. C1 [Canagaratna, M. R.; Massoli, P.; Fortner, E.; Williams, L. R.; Jayne, J. T.; Worsnop, D. R.] Aerodyne Res Inc, Billerica, MA 01821 USA. [Jimenez, J. L.] Univ Colorado, Dept Chem & Biochem, Boulder, CO 80309 USA. [Jimenez, J. L.] Univ Colorado, Cooperat Inst Res Environm Sci, Boulder, CO 80309 USA. [Kroll, J. H.; Chen, Q.] MIT, Dept Civil & Environm Engn, Cambridge, MA 02139 USA. [Kroll, J. H.; Kessler, S. H.] MIT, Dept Chem Engn, Cambridge, MA 02139 USA. [Hildebrandt Ruiz, L.] Univ Texas Austin, McKetta Dept Chem Engn, Austin, TX 78712 USA. [Hildebrandt Ruiz, L.] Univ Texas Austin, Ctr Energy & Environm Resources, Austin, TX 78712 USA. [Wilson, K. R.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Surratt, J. D.] Univ N Carolina, Dept Environm Sci & Engn, Chapel Hill, NC USA. [Donahue, N. M.] Carnegie Mellon Univ, Ctr Atmospher Particle Studies, Pittsburgh, PA 15213 USA. RP Canagaratna, MR (reprint author), Aerodyne Res Inc, Billerica, MA 01821 USA. EM mrcana@aerodyne.com RI Jimenez, Jose/A-5294-2008; Hildebrandt Ruiz, Lea/A-4236-2010; Worsnop, Douglas/D-2817-2009; Donahue, Neil/A-2329-2008; Surratt, Jason/D-3611-2009 OI Jimenez, Jose/0000-0001-6203-1847; Worsnop, Douglas/0000-0002-8928-8017; Donahue, Neil/0000-0003-3054-2364; Surratt, Jason/0000-0002-6833-1450 FU NSF [CHE-1012809, AGS-1243354]; NASA [NNX12AC03G]; NOAA [NA13OAR4310063]; National Science Foundation [ATM-1238109, AGS1136479]; Office of Basic Energy Sciences of the US Department of Energy [DE-AC02-05CH11231]; Department of Energy, Office of Science Early Career Research Program; US Department of Energy [DE-FG02-03ER83599, DE-FG02-05ER84269, DE-FG02-07ER84890] FX We thank the participants of AMS Clinic and AMS Users Meetings, Paul Ziemann, and Colette Heald for many useful discussions on these topics. J. H.Kroll, M. R. Canagaratna, and D. R. Worsnop acknowledge support from NSF CHE-1012809. J. L. Jimenez was partially supported by NSF AGS-1243354, NASA NNX12AC03G and NOAA NA13OAR4310063. Q. Chen is supported by the National Science Foundation (ATM-1238109). N. M. Donahue is supported by the National Science foundation (AGS1136479). K. R. Wilson and the Chemical Dynamics Beamline (Advanced Light Source) are supported by the Office of Basic Energy Sciences of the US Department of Energy under contract no. DE-AC02-05CH11231. K. R. Wilson is additionally supported by the Department of Energy, Office of Science Early Career Research Program. E. Fortner, L. R. Williams, and J. T. Jayne acknowledge support from the US Department of Energy (DE-FG02-03ER83599, DE-FG02-05ER84269, DE-FG02-07ER84890) NR 79 TC 127 Z9 128 U1 19 U2 94 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1680-7316 EI 1680-7324 J9 ATMOS CHEM PHYS JI Atmos. Chem. Phys. PY 2015 VL 15 IS 1 BP 253 EP 272 DI 10.5194/acp-15-253-2015 PG 20 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA AZ0TQ UT WOS:000347958200015 ER PT J AU Scanza, RA Mahowald, N Ghan, S Zender, CS Kok, JF Liu, X Zhang, Y Albani, S AF Scanza, R. A. Mahowald, N. Ghan, S. Zender, C. S. Kok, J. F. Liu, X. Zhang, Y. Albani, S. TI Modeling dust as component minerals in the Community Atmosphere Model: development of framework and impact on radiative forcing SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID AEROSOL OPTICAL-PROPERTIES; SKY RADIANCE MEASUREMENTS; EARTH SYSTEM MODEL; SAHARAN DUST; SIZE DISTRIBUTION; CLIMATE MODELS; DESERT DUST; AERONET; CYCLE; WIND AB The mineralogy of desert dust is important due to its effect on radiation, clouds and biogeochemical cycling of trace nutrients. This study presents the simulation of dust radiative forcing as a function of both mineral composition and size at the global scale, using mineral soil maps for estimating emissions. Externally mixed mineral aerosols in the bulk aerosol module in the Community Atmosphere Model version 4 (CAM4) and internally mixed mineral aerosols in the modal aerosol module in the Community Atmosphere Model version 5.1 (CAM5) embedded in the Community Earth System Model version 1.0.5 (CESM) are speciated into common mineral components in place of total dust. The simulations with mineralogy are compared to available observations of mineral atmospheric distribution and deposition along with observations of clear-sky radiative forcing efficiency. Based on these simulations, we estimate the all-sky direct radiative forcing at the top of the atmosphere as + 0.05 W m(-2) for both CAM4 and CAM5 simulations with mineralogy. We compare this to the radiative forcing from simulations of dust in release versions of CAM4 and CAM5 (+0.08 and +0.17 Wm(-2)) and of dust with optimized optical properties, wet scavenging and particle size distribution in CAM4 and CAM5, -0.05 and -0.17 Wm(-2), respectively. The ability to correctly include the mineralogy of dust in climate models is hindered by its spatial and temporal variability as well as insufficient global in situ observations, incomplete and uncertain source mineralogies and the uncertainties associated with data retrieved from remote sensing methods. C1 [Scanza, R. A.; Mahowald, N.; Zhang, Y.; Albani, S.] Cornell Univ, Dept Earth & Atmospher Sci, Ithaca, NY 14850 USA. [Ghan, S.; Liu, X.] Pacific NW Natl Lab, Atmospher Sci & Global Change Div, Richland, WA 99352 USA. [Zender, C. S.] Univ Calif Irvine, Dept Earth Syst Sci, Irvine, CA USA. [Kok, J. F.] Univ Calif Los Angeles, Dept Atmospher & Ocean Sci, Los Angeles, CA USA. [Liu, X.] Univ Wyoming, Dept Atmospher Sci, Laramie, WY 82071 USA. [Zhang, Y.] Fudan Univ, Dept Environm Sci & Engn, Shanghai 200433, Peoples R China. RP Scanza, RA (reprint author), Cornell Univ, Dept Earth & Atmospher Sci, Ithaca, NY 14850 USA. EM ras486@cornell.edu RI Liu, Xiaohong/E-9304-2011; Albani, Samuel/G-5329-2015; Mahowald, Natalie/D-8388-2013; Ghan, Steven/H-4301-2011; Zender, Charles/D-4485-2012; Kok, Jasper/A-9698-2008 OI Liu, Xiaohong/0000-0002-3994-5955; Albani, Samuel/0000-0001-9736-5134; Mahowald, Natalie/0000-0002-2873-997X; Ghan, Steven/0000-0001-8355-8699; Zender, Charles/0000-0003-0129-8024; Kok, Jasper/0000-0003-0464-8325 FU DOE [DE-SC00006735, DE-AC05-76RL01830]; NSF [0932946, 1003509]; US Department of Energy FX We thank Ives Balkanski for his comments and insight which improved the quality of the manuscript. Also, we thank the AERONET program for establishing and maintaining the used sites. These simulations were conducted at the National Center for Atmospheric Research, a National Science Foundation facility. N. Mahowald, R. Scanza and S. Albani would like to acknowledge the support of DOE DE-SC00006735, NSF 0932946 and NSF 1003509.; S. Ghan and X. Liu were funded by the US Department of Energy Atmospheric Systems Research and Climate Modeling programs. The Pacific Northwest National Laboratory (PNNL) is a multiprogram laboratory operated for DOE by Battelle Memorial Institute under contract DE-AC05-76RL01830. NR 77 TC 17 Z9 17 U1 7 U2 41 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1680-7316 EI 1680-7324 J9 ATMOS CHEM PHYS JI Atmos. Chem. Phys. PY 2015 VL 15 IS 1 BP 537 EP 561 DI 10.5194/acp-15-537-2015 PG 25 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA AZ0TQ UT WOS:000347958200030 ER PT J AU Zhang, J Gu, L Bao, F Cao, Y Hao, Y He, J Li, J Li, Y Ren, Y Wang, F Wu, R Yao, B Zhao, Y Lin, G Wu, B Lu, Q Meng, P AF Zhang, J. Gu, L. Bao, F. Cao, Y. Hao, Y. He, J. Li, J. Li, Y. Ren, Y. Wang, F. Wu, R. Yao, B. Zhao, Y. Lin, G. Wu, B. Lu, Q. Meng, P. TI Nitrogen control of C-13 enrichment in heterotrophic organs relative to leaves in a landscape-building desert plant species SO BIOGEOSCIENCES LA English DT Article ID CARBON-ISOTOPE DISCRIMINATION; SOIL CO2 EFFLUX; C-3 PLANTS; PHOSPHOENOLPYRUVATE CARBOXYLASE; TREE STEMS; RESPIRATION; ASSIMILATION; ECOSYSTEM; DIOXIDE; STOICHIOMETRY AB A longstanding puzzle in isotope studies of C-3 plant species is that heterotrophic plant organs (e.g., stems, roots, seeds, and fruits) tend to be enriched in C-13 compared to the autotrophic organ (leaves) that provides them with photosynthate. Our inability to explain this puzzle suggests key deficiencies in understanding post-photosynthetic metabolic processes. It also limits the effectiveness of applications of stable carbon isotope analyses in a variety of scientific disciplines ranging from plant physiology to global carbon cycle studies. To gain insight into this puzzle, we excavated whole plant architectures of Nitraria tangutorum Bobrov, a C-3 species that has an exceptional capability of fixing sands and building sand dunes, in two deserts in northwestern China. We systematically and simultaneously measured carbon isotope ratios and nitrogen and phosphorous contents of different parts of the excavated plants. We also determined the seasonal variations in leaf carbon isotope ratios on nearby intact plants of N. tangutorum. We found, for the first time, that higher nitrogen contents in heterotrophic organs were significantly correlated with increased heterotrophic C-13 enrichment compared to leaves. However, phosphorous contents had no effect on the enrichment. In addition, new leaves had carbon isotope ratios similar to roots but were progressively depleted in C-13 as they matured. We concluded that a nitrogen-mediated process, hypothesized to be the refixation of respiratory CO2 by phosphoenolpyruvate (PEP) carboxylase, was responsible for the differences in C-13 enrichment among different heterotrophic organs, while processes such as fractionating foliar metabolism and preferentially loading into phloem of C-13-enriched sugars may contribute to the overall autotrophic-heterotrophic difference in carbon isotope compositions. C1 [Zhang, J.; Bao, F.; Cao, Y.; He, J.; Li, J.; Li, Y.; Ren, Y.; Wang, F.; Wu, R.; Yao, B.; Wu, B.; Lu, Q.] Chinese Acad Forestry, Inst Desertificat Studies, Beijing, Peoples R China. [Zhang, J.] Chinese Acad Forestry, Res Inst Forestry, Beijing, Peoples R China. [Gu, L.] Oak Ridge Natl Lab, Div Environm Sci, Oak Ridge, TN 37831 USA. [Gu, L.] Oak Ridge Natl Lab, Climate Change Sci Inst, Oak Ridge, TN 37831 USA. [Hao, Y.; Zhao, Y.] Chinese Acad Forestry, Expt Ctr Desert Forestry, Dengkou, Inner Mongolia, Peoples R China. [Lin, G.] Tsinghua Univ, Ctr Earth Syst Sci, Beijing 100084, Peoples R China. [Meng, P.] Chinese Acad Forestry, Beijing, Peoples R China. RP Gu, L (reprint author), Oak Ridge Natl Lab, Div Environm Sci, POB 2008, Oak Ridge, TN 37831 USA. EM lianhong-gu@ornl.gov RI Gu, Lianhong/H-8241-2014 OI Gu, Lianhong/0000-0001-5756-8738 FU Forestry Public Welfare Scientific Research Funding [201104077]; Program of Introducing Advanced Forestry Technologies from Other Countries [2008-4-47]; Science and Technology Foundation [CAFYBB2007008]; Lecture and Study Program for Outstanding Scholars from Home and Abroad of the Chinese Academy of Forestry; National Key Technology R&D Program of the Ministry of Science and Technology of China [2012BAD16B01]; US Department of Energy, Office of Science, Biological and Environmental Research Program, Climate and Environmental Sciences Division; ORNL's Laboratory Directed Research and Development Program; US Department of Energy [DE-AC05-00OR22725] FX Field work, data acquisition and analyses were conducted at the Institute of Desertification Studies, Chinese Academy of Forestry with support in part by grants from the Forestry Public Welfare Scientific Research Funding (201104077), the Program of Introducing Advanced Forestry Technologies from Other Countries (2008-4-47), the Science and Technology Foundation (CAFYBB2007008) and the Lecture and Study Program for Outstanding Scholars from Home and Abroad of the Chinese Academy of Forestry, and the National Key Technology R&D Program of the Ministry of Science and Technology of China (2012BAD16B01). Data analyses and manuscript writing were partly carried out at Oak Ridge National Laboratory (ORNL) with support from US Department of Energy, Office of Science, Biological and Environmental Research Program, Climate and Environmental Sciences Division. It also received support from the ORNL's Laboratory Directed Research and Development Program. ORNL is managed by UT-Battelle, LLC, for the US Department of Energy under contract DE-AC05-00OR22725. NR 47 TC 1 Z9 3 U1 4 U2 26 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1726-4170 EI 1726-4189 J9 BIOGEOSCIENCES JI Biogeosciences PY 2015 VL 12 IS 1 BP 15 EP 27 DI 10.5194/bg-12-15-2015 PG 13 WC Ecology; Geosciences, Multidisciplinary SC Environmental Sciences & Ecology; Geology GA AZ0UR UT WOS:000347960800002 ER PT J AU Gross, E Toste, FD Somorjai, GA AF Gross, Elad Toste, F. Dean Somorjai, Gabor A. TI Polymer-Encapsulated Metallic Nanoparticles as a Bridge Between Homogeneous and Heterogeneous Catalysis SO CATALYSIS LETTERS LA English DT Article DE Heterogeneous catalysis; Homogeneous catalysis; Asymmetric catalysis; Cyclization; Infrared tomography; NEXAFS; Colloidal synthesis ID GENERATION VIBRATIONAL SPECTROSCOPY; SUPPORTED GOLD; CO OXIDATION; NANOCRYSTALLINE CEO2; HYDROGENATION; SELECTIVITY; SIZE; CHEMISTRY; SURFACE; FLOW AB Continuous efforts in catalysis research have been devoted towards the development of heterogeneous catalysts that can activate reactions which are catalyzed by homogeneous catalysts. Replacing homogeneous catalysts with their heterogeneous counterparts will enhance the sustainability of the catalytic system, providing a highly recyclable, scalable and efficient setup. Throughout this review we demonstrate that small (< 2 nm), metallic nanoclusters can catalyze a wide range of pi-bond activation reactions that were previously activated by homogeneous catalysts. The small size of the nanoparticles enables their reversible oxidation into catalytically active metal ions. Encapsulation of the metal within a polymeric matrix severely restricts leaching of the highly oxidized metal ions into the solution phase, inducing high catalytic stability and recyclability. Activation of complex, multistep organic transformations with heterogeneous catalysts provides novel opportunities, not accessible with homogeneous catalysts, to control and tune the products selectivity. By designing the molecular properties of the polymeric matrix that encapsulates the metal cluster, high products selectivity, diastereoselectivity and enantioselectivity can be gained. These results demonstrate the capability of mesoscale catalysts, constructed of metallic nanoparticles and an encapsulating layer, to activate a wide array of catalytic reactions with high reactivity and tunable selectivity. C1 [Gross, Elad; Toste, F. Dean; Somorjai, Gabor A.] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Gross, Elad; Toste, F. Dean; Somorjai, Gabor A.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. [Gross, Elad; Toste, F. Dean; Somorjai, Gabor A.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. RP Gross, E (reprint author), Hebrew Univ Jerusalem, Inst Chem, IL-91904 Jerusalem, Israel. EM elad.gross@mail.huji.ac.il FU Office of Basic Energy Sciences, Materials Science and Engineering Division and the Division of Chemical Sciences, Geological and Biosciences of the U.S. Department of Energy [DE-AC02-05CH11231] FX This work was supported by the Director, Office of Basic Energy Sciences, Materials Science and Engineering Division and the Division of Chemical Sciences, Geological and Biosciences of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. The X-ray absorption and Infrared microspectroscopy studies were performed at the Advanced Light Source, a DOE User facility of the Office of Science, Office of Basic Energy Sciences. NR 64 TC 14 Z9 14 U1 11 U2 66 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1011-372X EI 1572-879X J9 CATAL LETT JI Catal. Lett. PD JAN PY 2015 VL 145 IS 1 BP 126 EP 138 DI 10.1007/s10562-014-1436-9 PG 13 WC Chemistry, Physical SC Chemistry GA AY7BT UT WOS:000347717000008 ER PT J AU Na, K Somorjai, GA AF Na, Kyungsu Somorjai, Gabor A. TI Hierarchically Nanoporous Zeolites and Their Heterogeneous Catalysis: Current Status and Future Perspectives SO CATALYSIS LETTERS LA English DT Article DE Zeolites; Heterogeneous catalysis; Mesoporous materials; Nanoparticles; Acid catalysis ID SUPPORTED RUTHENIUM NANOPARTICLES; SURFACTANT-DIRECTED SYNTHESIS; N-HEPTANE HYDROISOMERIZATION; FISCHER-TROPSCH CATALYSTS; FRIEDEL-CRAFTS ALKYLATION; SINGLE-CRYSTAL CATALYSTS; UNIT-CELL THICKNESS; MESOPOROUS ZEOLITE; MFI ZEOLITE; MOLECULAR-SIEVES AB The research field of hierarchically nanoporous zeolites has been growing at an enormous pace over the past decades. Hierarchically nanoporous zeolites have versatile structural properties such as high surface area and large pore volume that can alleviate diffusional limitations of conventional zeolites with solely microporous framework. In this review, various synthesis strategies to hierarchically nanoporous zeolites and their structural advantages in catalytic reactions will be reviewed. In the first part, many novel synthetic approaches for hierarchically nanoporous zeolites such as post-demetallation, soft-templating, hard-templating, and dual-pore-generating surfactant-directed methods will be introduced. In the second part, catalytic applications of hierarchically nanoporous zeolites on various chemical reactions involving isomerization, cracking, alkylation and oxidation will be discussed. The present comprehensive review will provide future opportunities and perspectives on the research of hierarchically nanoporous zeolites including their applications to catalytic reactions. C1 [Na, Kyungsu; Somorjai, Gabor A.] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Na, Kyungsu; Somorjai, Gabor A.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. RP Somorjai, GA (reprint author), Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. EM Somorjai@berkeley.edu FU Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geological and Biosciences of the US Department of Energy [DE-AC-02-05CH11231]; Chevron Corporation FX This work was supported by the Director, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geological and Biosciences of the US Department of Energy under contract No. DE-AC-02-05CH11231. The nanoparticle synthesis was funded by Chevron Corporation. We thank Walter Ralston for correcting the proof. NR 146 TC 18 Z9 18 U1 13 U2 98 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1011-372X EI 1572-879X J9 CATAL LETT JI Catal. Lett. PD JAN PY 2015 VL 145 IS 1 BP 193 EP 213 DI 10.1007/s10562-014-1411-5 PG 21 WC Chemistry, Physical SC Chemistry GA AY7BT UT WOS:000347717000013 ER PT J AU Zhang, M Frei, H AF Zhang, Miao Frei, Heinz TI Towards a Molecular Level Understanding of the Multi-Electron Catalysis of Water Oxidation on Metal Oxide Surfaces SO CATALYSIS LETTERS LA English DT Article DE Heterogeneous catalysis; Photocatalysis; Water oxidation; Spectroscopy; Surface reaction kinetics; Oxide supports ID OXYGEN EVOLUTION REACTION; CHARGE-TRANSFER CHROMOPHORE; FT-IR SPECTROSCOPY; MESOPOROUS SILICA; COBALT OXIDE; ELECTRON-TRANSFER; PHOTOCATALYTIC OXIDATION; ANODIC CHARACTERISTICS; NANOCLUSTER CATALYST; ACTIVATION-ENERGIES AB Earth abundant metal oxides play a central role as catalysts in the essential chemical transformations of sunlight to fuel conversion, which are the oxidation of water and the reduction of carbon dioxide. The rapidly growing interest in renewable fuel generation by using the energy of the sun has recently led to substantial breakthroughs in the use of first row transition metal oxides as catalysts for oxygen evolution from water. Substantive improvements of rates and lowering of overpotentials have been achieved by exploiting materials properties on the nanoscale, or taking advantage of the synergy of multiple metals. Moreover, knowledge derived from mechanistic investigations with structure specific spectroscopy is accelerating efficiency improvements. Monitoring by time-resolved FT-infrared spectroscopy reveals the molecular nature of active sites, while in situ X-ray and optical spectroscopy under reaction conditions provides insights into the electronic structure of the surface metal centers participating in the catalysis. By combining the bond specificity of vibrational spectroscopy with the metal electronic structure specificity of optical, X-ray absorption or photoelectron spectroscopy, a complete understanding of active surface sites on metal oxides begins to emerge. Charge flow driving the chemical transformations probed by optical spectroscopy across time scales from ultrafast to very slow reveals the processes that control the productive use of charges delivered to the catalyst. Coupling of the water oxidation catalysis at a metal oxide catalyst with carbon dioxide reduction at a heterobinuclear chromophore, which is the goal of the artificial photosystem approach, is demonstrated by a well-defined all-inorganic polynuclear unit. . C1 [Zhang, Miao; Frei, Heinz] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA 94720 USA. RP Frei, H (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA 94720 USA. EM HMFrei@lbl.gov RI Foundry, Molecular/G-9968-2014 FU U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-05CH11231] FX This material is based on work supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under contract No. DE-AC02-05CH11231. This research used resources of the National Center for Electron Microscopy, Lawrence Berkeley National Laboratory, which is a DOE Office of Science User Facility. The authors thank Dr. Christian Kisielowski for imaging at the TEAM0.5 microscope. NR 98 TC 15 Z9 15 U1 12 U2 95 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1011-372X EI 1572-879X J9 CATAL LETT JI Catal. Lett. PD JAN PY 2015 VL 145 IS 1 BP 420 EP 435 DI 10.1007/s10562-014-1437-8 PG 16 WC Chemistry, Physical SC Chemistry GA AY7BT UT WOS:000347717000022 ER PT J AU Xiong, HF DeLaRiva, A Wang, Y Datye, AK AF Xiong, Haifeng DeLaRiva, Andrew Wang, Yong Datye, Abhaya K. TI Low-temperature aqueous-phase reforming of ethanol on bimetallic PdZn catalysts SO CATALYSIS SCIENCE & TECHNOLOGY LA English DT Article ID IMPROVED HYDROTHERMAL STABILITY; OXYGENATED HYDROCARBONS; HYDROGEN; METHANOL; BIOMASS; NIOBIA/CARBON; MECHANISM; ALKANES; SIZE AB Bimetallic PdZn catalysts supported on carbon black (CB) and carbon nanotubes (CNTs) were found to be selective for CO-free H-2 production from ethanol at low temperature (250 degrees C). On Pd, the H-2 yield was low (similar to 0.3 mol H-2/mol ethanol reacted) and the CH4/CO2 ratio was high (similar to 1.7). Addition of Zn to Pd formed the intermetallic PdZn beta phase (atomic ratio of Zn to Pd is 1) with increased H-2 yield (similar to 1.9 mol H-2/mol ethanol reacted) and CH4/CO2 ratio of <1. The higher H-2 yield and low CH4 formation was related to the improved dehydrogenation activity of the L1(0) PdZn beta phase. The TOF increased with particle size and the CNTs provided the most active and selective catalysts, which may be ascribed to pore-confinement effects. Furthermore, no significant changes in either the supports or the PdZn beta particles was found after aqueous-phase reforming (APR) indicating that the metal nanoparticles and the carbon support are hydrothermally stable in the aqueous phase at elevated temperatures and pressures (>200 degrees C, 65 bar). No CO was detected for all the catalysts performed in aqueous-phase reaction, indicating that both monometallic Pd and bimetallic PdZn catalysts have high water-gas shift activity during APR. However, the yield of H-2 is considerably lower than the theoretical value of 6 H-2 per mole ethanol which is due to the presence of oxygenated products and methane on the PdZn catalysts. C1 [Xiong, Haifeng; DeLaRiva, Andrew; Datye, Abhaya K.] Univ New Mexico, Dept Chem & Biol Engn, Albuquerque, NM 87131 USA. [Xiong, Haifeng; DeLaRiva, Andrew; Datye, Abhaya K.] Univ New Mexico, Ctr Microengn Mat, Albuquerque, NM 87131 USA. [Wang, Yong] Pacific NW Natl Lab, Inst Integrated Catalysis, Richland, WA 99352 USA. [Wang, Yong] Washington State Univ, Gene & Linda Voiland Sch Chem Engn & Bioengn, Pullman, WA 99164 USA. RP Xiong, HF (reprint author), Univ New Mexico, Dept Chem & Biol Engn, Albuquerque, NM 87131 USA. EM datye@unm.edu RI xiong, haifeng/F-6638-2016 FU DOE [DE-FG02-05ER15712]; Center for Biorenewable Chemicals (CBiRC) - NSF [EEC-0813570] FX This work is supported by DOE grant DE-FG02-05ER15712 and the Center for Biorenewable Chemicals (CBiRC) supported by NSF under no. EEC-0813570. We thank Eric Peterson for help with XRD, Jay McCabe for CO oxidation reactivity and Dr. H. Pham for assistance with N2 physisorption measurements. NR 24 TC 5 Z9 5 U1 3 U2 43 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2044-4753 EI 2044-4761 J9 CATAL SCI TECHNOL JI Catal. Sci. Technol. PY 2015 VL 5 IS 1 BP 254 EP 263 DI 10.1039/c4cy00914b PG 10 WC Chemistry, Physical SC Chemistry GA AZ6WH UT WOS:000348358200028 ER PT J AU Brambrink, E Amadou, N Benuzzi-Mounaix, A Geissel, M Harmand, M Pelka, A Vinci, T Koenig, M AF Brambrink, E. Amadou, N. Benuzzi-Mounaix, A. Geissel, M. Harmand, M. Pelka, A. Vinci, T. Koenig, M. TI Production and Diagnostics of Dense Matter SO CONTRIBUTIONS TO PLASMA PHYSICS LA English DT Article DE Warm dense matter; high energy density physics; ramp compression ID FACILITY; PLANETS; CURVE; STAR AB High energy lasers are a unique tool to create high pressure states above 10 Mbar at ns time scales, which allow to study material properties under these extreme conditions. These conditions are, for example, comparable with planetary cores, where material properties play an important role for the properties and evolution of a planet. The rapid compression allows also to study dynamic effects of phase transitions as compression times are comparable to relaxation times. We will present recent results of laser compression of iron reaching conditions of so called "super-Earth" cores. A description of the compression schemes as well as present and future diagnostics is presented. (C) 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim C1 [Brambrink, E.; Amadou, N.; Benuzzi-Mounaix, A.; Harmand, M.; Pelka, A.; Vinci, T.; Koenig, M.] Univ Paris 06, Ecole Polytech, CEA, LULI CNRS UMR7605, Palaiseau, France. [Geissel, M.] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Brambrink, E (reprint author), Univ Paris 06, Ecole Polytech, CEA, LULI CNRS UMR7605, Palaiseau, France. EM Erik.Brambrink@polytechnique.edu RI harmand, marion/Q-1248-2016 OI harmand, marion/0000-0003-0713-5824 NR 38 TC 2 Z9 2 U1 2 U2 10 PU WILEY-V C H VERLAG GMBH PI WEINHEIM PA BOSCHSTRASSE 12, D-69469 WEINHEIM, GERMANY SN 0863-1042 EI 1521-3986 J9 CONTRIB PLASM PHYS JI Contrib. Plasma Phys. PD JAN PY 2015 VL 55 IS 1 BP 67 EP 77 DI 10.1002/ctpp.201400029 PG 11 WC Physics, Fluids & Plasmas SC Physics GA AZ3DF UT WOS:000348107200005 ER PT J AU Artioli, G Valentini, L Voltolini, M Dalconi, MC Ferrari, G Russo, V AF Artioli, Gilberto Valentini, Luca Voltolini, Marco Dalconi, Maria C. Ferrari, Giorgio Russo, Vincenzo TI Direct Imaging of Nucleation Mechanisms by Synchrotron Diffraction Micro-Tomography: Superplasticizer-Induced Change of C-S-H Nucleation in Cement SO CRYSTAL GROWTH & DESIGN LA English DT Article ID PORTLAND-CEMENT; HYDRATION KINETICS; CALCIUM SILICATE; PASTES; MODEL AB The properties of cementitious materials are related to the microstructure of their binder matrix, which develops, during cement hydration, by a sequence of dissolution-precipitation reactions. Here, microstructural development is monitored during hydration by synchrotron X-ray diffraction-enhanced computed microtomography (XRD-CT). This innovative, noninvasive technique yields images of the crystallographic phases present in the hydrating cement paste at different stages, which are combined to map the sites where dissolution and precipitation occur. The results indicate that the nucleation mechanism of the main hydration product (a calcium-silicate hydrate commonly referred to as C-S-H) changes in the presence of polycarboxylate ether (PCE) superplasticizers. The observed change is essential to understand the development of the cement microstructure and to provide a direct link between the reaction kinetics and the physicomechanical properties of the system. C1 [Artioli, Gilberto; Valentini, Luca; Dalconi, Maria C.] Univ Padua, Dept Geosci, I-35131 Padua, Italy. [Artioli, Gilberto; Valentini, Luca; Dalconi, Maria C.] Univ Padua, CIRCe Ctr, I-35131 Padua, Italy. [Voltolini, Marco] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Ferrari, Giorgio; Russo, Vincenzo] Mapei SpA, Dept Res & Dev, I-20158 Milan, Italy. RP Valentini, L (reprint author), Univ Padua, Dept Geosci, I-35131 Padua, Italy. EM luca.valentini@unipd.it RI Artioli, Gilberto/F-2149-2015; Voltolini, Marco/G-2781-2015 OI Artioli, Gilberto/0000-0002-8693-7392; FU Mapei S.p.A. through the Mapei-UNIPD; [MA-1063] FX Mapei S.p.A. supports the research through the Mapei-UNIPD agreement.; ESRF is acknowledged for beam time through the Long Term project MA-1063. Remi Tucoulou greatly helped during data collection at ESRF. NR 21 TC 5 Z9 5 U1 5 U2 36 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 1528-7483 EI 1528-7505 J9 CRYST GROWTH DES JI Cryst. Growth Des. PD JAN PY 2015 VL 15 IS 1 BP 20 EP 23 DI 10.1021/cg501466z PG 4 WC Chemistry, Multidisciplinary; Crystallography; Materials Science, Multidisciplinary SC Chemistry; Crystallography; Materials Science GA AY6HK UT WOS:000347667500006 ER PT J AU Hong, MN Moreland, KT Chen, JJ Teng, HH Thalmann, R De Yoreo, JJ AF Hong, Mina Moreland, K. Trent Chen, Jiajun Teng, Henry H. Thalmann, Ruediger De Yoreo, James J. TI Effect of Otoconial Proteins Fetuin A, Osteopontin, and Otoconin 90 on the Nucleation and Growth of Calcite SO CRYSTAL GROWTH & DESIGN LA English DT Article ID OXALATE MONOHYDRATE CRYSTALLIZATION; ATOMIC-FORCE MICROSCOPY; IN-VITRO; KINETICS; MATRIX; INHIBITION; CRYSTALS; THERMODYNAMICS; ACCELERATION; COMPETITION AB We investigated the roles of three proteins associated with the formation of otoconia including fetuin A, osteopontin (OPN), and otoconin 90 (OC90). In situ atomic force microscopy (AFM) studies of the effects of these proteins on the growth of atomic steps on calcite surfaces were performed to obtain insight into their effects on the growth kinetics. We also used scanning electron microscopy to examine the effects of these proteins on crystal morphology. All three proteins were found to be potent inhibitors of calcite growth, although fetuin A promoted growth at concentrations below about 40 nM and only became an inhibitor at higher concentrations. We then used in situ optical microscopy to observe calcite nucleation on films of these proteins adsorbed onto mica surfaces. By measuring the calcite nucleation rate as a function of supersaturation, the value of the interfacial energy that controls the free energy barrier to heterogeneous nucleation was determined for each protein. OPN and OC90 films led to significantly reduced interfacial energies as compared to the value for homogeneous calcite nucleation in bulk solution. The value for fetuin A was equal to that for bulk solution within experimental error. Zeta potential measurements showed all of the proteins possessed negative surface charge and varied in magnitude according to sequence fetuin A > OC90 > OPN. In addition, the interfacial energies exhibited an inverse scaling with the zeta potential. In analogy to previous measurements on polysaccharide films, this scaling indicates the differences between the proteins arise from the effect of protein surface charge on the solutionsubstrate interfacial energy. C1 [Hong, Mina; De Yoreo, James J.] Pacific NW Natl Lab, Phys Sci Div, Richland, WA 99352 USA. [Hong, Mina; Teng, Henry H.] George Washington Univ, Dept Chem, Washington, DC 20052 USA. [Hong, Mina; Chen, Jiajun] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA. [Moreland, K. Trent; Thalmann, Ruediger] Washington Univ, Dept Otolaryngol Head & Neck Surg, St Louis, MO 63110 USA. RP Thalmann, R (reprint author), Washington Univ, Dept Otolaryngol Head & Neck Surg, St Louis, MO 63110 USA. EM thalmannr@ent.wustl.edu; james.deyoreo@pnnl.gov RI Foundry, Molecular/G-9968-2014; Moreland, Trent/I-5497-2013 OI Moreland, Trent/0000-0002-8996-832X FU NIH/NIDCD [RO1 DC011614]; U.S. Department of energy [DE-AC05-76RL01830]; Office of Basic Energy Sciences, Scientific User Facilities Division FX This work was supported by NIH/NIDCD grant number RO1 DC011614. The funders had no role in study design, data collection and analysis, decision to publish, or preparation of the manuscript. This research was performed at Pacific Northwest National Laboratory, which is operated by Battelle for the U.S. Department of energy under Contract DE-AC05-76RL01830, at the Molecular Foundry, Lawrence Berkeley National Laboratory, which is supported by the Office of Basic Energy Sciences, Scientific User Facilities Division, and at the Washington University in St. Louis, Department of Otolaryngology. The authors would like to acknowledge Washington University in St. Louis, Department of Otolaryngology's Electron Microscopy Core. NR 52 TC 2 Z9 2 U1 2 U2 29 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 1528-7483 EI 1528-7505 J9 CRYST GROWTH DES JI Cryst. Growth Des. PD JAN PY 2015 VL 15 IS 1 BP 129 EP 136 DI 10.1021/cg501001r PG 8 WC Chemistry, Multidisciplinary; Crystallography; Materials Science, Multidisciplinary SC Chemistry; Crystallography; Materials Science GA AY6HK UT WOS:000347667500019 PM 25709560 ER PT J AU Custelcean, R Sloop, FV Rajbanshi, A Wan, S Moyer, BA AF Custelcean, Radu Sloop, Frederick V., Jr. Rajbanshi, Arbin Wan, Shun Moyer, Bruce A. TI Sodium Sulfate Separation from Aqueous Alkaline Solutions via Crystalline Urea-Functionalized Capsules: Thermodynamics and Kinetics of Crystallization SO CRYSTAL GROWTH & DESIGN LA English DT Article ID SELECTIVE CRYSTALLIZATION; GROWTH AB The thermodynamics and kinetics of crystallization of sodium sulfate with a tripodal tris-urea receptor (L1) from aqueous alkaline solutions have been measured in the 15-55 degrees C temperature range for a fundamental understanding of the elementary steps involved in this sulfate separation method. The use of radiolabeled (Na2SO4)-S-35 provided a practical way to monitor the sulfate concentration in solution by beta liquid scintillation counting. Our results are consistent with a two-step crystallization mechanism, involving relatively quick dissolution of crystalline L1 followed by the rate-limiting crystallization of the Na2SO4(L1)(2)(H2O)(4) capsules. We found that temperature exerted relatively little influence over the equilibrium sulfate concentration, which ranged between 0.004 and 0.011 M. This corresponds to 77-91% removal of sulfate from a solution containing 0.0475 M initial sulfate concentration, as found in a typical Hanford waste tank. The apparent pseudo-first-order rate constant for sulfate removal increased 20-fold from 15 to 55 degrees C, corresponding to an activation energy of 14.1 kcal/mol. At the highest measured temperature of 55 degrees C, 63% and 75% of sulfate was removed from solution within 8 and 24 h, respectively. These results indicate the capsule crystallization method is a viable approach to sulfate separation from nuclear wastes. C1 [Custelcean, Radu; Sloop, Frederick V., Jr.; Rajbanshi, Arbin; Wan, Shun; Moyer, Bruce A.] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. RP Custelcean, R (reprint author), Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. EM custelceanr@ornl.gov RI Sloop, Jr., Frederick/J-2301-2016; Custelcean, Radu/C-1037-2009; Moyer, Bruce/L-2744-2016 OI Sloop, Jr., Frederick/0000-0001-6473-9507; Custelcean, Radu/0000-0002-0727-7972; Moyer, Bruce/0000-0001-7484-6277 FU Office of Technology Innovation and Development, U.S. Department of Energy; Office of Environmental Management, U.S. Department of Energy FX This research was sponsored by the Office of Technology Innovation and Development, Office of Environmental Management, U.S. Department of Energy. NR 10 TC 6 Z9 6 U1 3 U2 18 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 1528-7483 EI 1528-7505 J9 CRYST GROWTH DES JI Cryst. Growth Des. PD JAN PY 2015 VL 15 IS 1 BP 517 EP 522 DI 10.1021/cg501656s PG 6 WC Chemistry, Multidisciplinary; Crystallography; Materials Science, Multidisciplinary SC Chemistry; Crystallography; Materials Science GA AY6HK UT WOS:000347667500064 ER PT J AU Tomasi, C Kokhanovsky, AA Lupi, A Ritter, C Smirnov, A O'Neill, NT Stone, RS Holben, BN Nyeki, S Wehrli, C Stohl, A Mazzola, M Lanconelli, C Vitale, V Stebel, K Aaltonen, V de Leeuw, G Rodriguez, E Herber, AB Radionov, VF Zielinski, T Petelski, T Sakerin, SM Kabanov, DM Xue, Y Mei, LL Istomina, L Wagener, R McArthur, B Sobolewski, PS Kivi, R Courcoux, Y Larouche, P Broccardo, S Piketh, SJ AF Tomasi, Claudio Kokhanovsky, Alexander A. Lupi, Angelo Ritter, Christoph Smirnov, Alexander O'Neill, Norman T. Stone, Robert S. Holben, Brent N. Nyeki, Stephan Wehrli, Christoph Stohl, Andreas Mazzola, Mauro Lanconelli, Christian Vitale, Vito Stebel, Kerstin Aaltonen, Veijo de Leeuw, Gerrit Rodriguez, Edith Herber, Andreas B. Radionov, Vladimir F. Zielinski, Tymon Petelski, Tomasz Sakerin, Sergey M. Kabanov, Dmitry M. Xue, Yong Mei, Linlu Istomina, Larysa Wagener, Richard McArthur, Bruce Sobolewski, Piotr S. Kivi, Rigel Courcoux, Yann Larouche, Pierre Broccardo, Stephen Piketh, Stuart J. TI Aerosol remote sensing in polar regions SO EARTH-SCIENCE REVIEWS LA English DT Article DE Sun-photometer measurements; Aerosol optical thickness; Polar aerosol optical characteristics; Lidar backscattering coefficient profiles; Satellite aerosol remote sensing; Multimodal aerosol extinction models ID OPTICAL DEPTH RETRIEVAL; RESOLUTION IMAGING SPECTRORADIOMETER; TROPOSPHERIC AEROSOL; BOUNDARY-LAYER; ARCTIC HAZE; AVHRR DATA; ANTARCTIC ATMOSPHERE; SIZE DISTRIBUTIONS; LAND SURFACES; SOUTH-POLE AB Multi-year sets of ground-based sun-photometer measurements conducted at 12 Arctic sites and 9 Antarctic sites were examined to determine daily mean values of aerosol optical thickness tau(lambda) at visible and near-infrared wavelengths, from which best-fit values of Angstrom's exponent alpha were calculated. Analysing these data, the monthly mean values of tau(0.50 mu m) and alpha and the relative frequency histograms of the daily mean values of both parameters were determined for winter spring and summer autumn in the Arctic and for austral summer in Antarctica. The Arctic and Antarctic covariance plots of the seasonal median values of alpha versus tau(0.50 mu m) showed: (i) a considerable increase in tau(0.50 mu m) for the Arctic aerosol from summer to winter spring, without marked changes in alpha; and (ii) a marked increase in tau(0.50 mu m) passing from the Antarctic Plateau to coastal sites, whereas alpha decreased considerably due to the larger fraction of sea-salt aerosol. Good agreement was found when comparing ground-based sun-photometer measurements of tau(lambda) and alpha at Arctic and Antarctic coastal sites with Microtops measurements conducted during numerous AERONET/MAN cruises from 2006 to 2013 in three Arctic Ocean sectors and in coastal and off-shore regions of the Southern Atlantic, Pacific, and Indian Oceans, and the Antarctic Peninsula. Lidar measurements were also examined to characterise vertical profiles of the aerosol backscattering coefficient measured throughout the year at Ny-Alesund. Satellite-based MODIS, MISR, and AATSR retrievals of tau(lambda) over large parts of the oceanic polar regions during spring and summer were in close agreement with ship-borne and coastal ground-based sun-photometer measurements. An overview of the chemical composition of mode particles is also presented, based on in-situ measurements at Arctic and Antarctic sites. Fourteen log-normal aerosol number size-distributions were defined to represent the average features of nuclei, accumulation and coarse mode particles for Arctic haze, summer background aerosol, Asian dust and boreal forest fire smoke, and for various background austral summer aerosol types at coastal and high-altitude Antarctic sites. The main columnar aerosol optical characteristics were determined for all 14 particle modes, based on in-situ measurements of the scattering and absorption coefficients. Diurnally averaged direct aerosol-induced radiative forcing and efficiency were calculated for a set of multimodal aerosol extinction models, using various Bidirectional Reflectance Distribution Function models over vegetation-covered, oceanic and snow-covered surfaces. These gave a reliable measure of the pronounced effects of aerosols on the radiation balance of the surface-atmosphere system over polar regions. (C) 2014 Elsevier B.V. All rights reserved. C1 [Tomasi, Claudio; Lupi, Angelo; Mazzola, Mauro; Lanconelli, Christian; Vitale, Vito] Italian Natl Res Council CNR, Inst Atmospher Sci & Climate ISAC, Climate Change Div, Bologna, Italy. [Kokhanovsky, Alexander A.; Istomina, Larysa] Univ Bremen, Inst Environm Phys IUP, D-28359 Bremen, Germany. [Kokhanovsky, Alexander A.] EUMETSAT, D-64295 Darmstadt, Germany. [Ritter, Christoph] Alfred Wegener Inst Polar & Marine Res, Climate Syst Div, Potsdam, Germany. [Smirnov, Alexander] Sigma Space Corp, Lanham, MD USA. [Smirnov, Alexander] NASA, Goddard Space Flight Ctr, Biospher Sci Branch, Greenbelt, MD 20771 USA. [O'Neill, Norman T.] Univ Sherbrooke, Dept Appl Geomat, Canadian Network Detect Atmospher Change CANDAC, Sherbrooke, PQ J1K 2R1, Canada. [O'Neill, Norman T.] Univ Sherbrooke, Dept Appl Geomat, CARTEL, Sherbrooke, PQ J1K 2R1, Canada. [Stone, Robert S.] NOAA, Global Monitoring Div, Boulder, CO USA. [Stone, Robert S.] Univ Colorado, Cooperat Inst Res Environm Sci, Boulder, CO 80309 USA. [Nyeki, Stephan; Wehrli, Christoph] Phys Meteorol Observ PMOD, World Radiat Ctr, Davos, Switzerland. [Stohl, Andreas; Stebel, Kerstin] Norwegian Inst Air Res NILU, Kjeller, Norway. [Aaltonen, Veijo; Rodriguez, Edith] Finnish Meteorol Inst, Climate & Global Change Div, FIN-00101 Helsinki, Finland. [de Leeuw, Gerrit] Univ Helsinki, Dept Phys, FIN-00014 Helsinki, Finland. [Herber, Andreas B.] Alfred Wegener Inst Polar & Marine Res, Climate Syst Div, Bremerhaven, Germany. [Radionov, Vladimir F.] Arctic & Antarctic Res Inst, St Petersburg 199226, Russia. [Zielinski, Tymon; Petelski, Tomasz] Polish Acad Sci, Inst Oceanol, Sopot, Poland. [Sakerin, Sergey M.; Kabanov, Dmitry M.] Russian Acad Sci, Siberian Branch, VE Zuev Inst Atmospher Opt IAO, Tomsk, Russia. [Xue, Yong] London Metropolitan Univ, Fac Life Sci & Comp, London, England. [Xue, Yong; Mei, Linlu] Chinese Acad Sci, Inst Remote Sensing & Digital Earth, Key Lab Digital Earth Sci, Beijing 100094, Peoples R China. [Wagener, Richard] Brookhaven Natl Lab, Environm & Climate Sci Dept, Upton, NY 11973 USA. [McArthur, Bruce] Environm Canada, N York, ON, Canada. [Sobolewski, Piotr S.] Polish Acad Sci, Inst Geophys, Warsaw 42, Poland. [Kivi, Rigel] Finnish Meteorol Inst, Arctic Res Ctr, Sodankyla, Finland. [Courcoux, Yann] Univ Reunion, CNRS, Inst Atmosphere Reunion OPAR, St Denis, Reunion. [Larouche, Pierre] Inst Maurice Lamontagne, Mont Joli, PQ G5H 3Z4, Canada. [Broccardo, Stephen] Univ Witwatersrand, Johannesburg, South Africa. [Piketh, Stuart J.] North West Univ, Climatol Res Grp, Unit Environm Sci & Management, Potchefstroom, South Africa. RP Tomasi, C (reprint author), Italian Natl Res Council CNR, Inst Atmospher Sci & Climate ISAC, Climate Change Div, Bologna, Italy. EM c.tomasi@isac.cnr.it RI Stohl, Andreas/A-7535-2008; Kokhanovsky, Alexander/C-6234-2016; Mazzola, Mauro/K-9376-2016; OI Stohl, Andreas/0000-0002-2524-5755; Kokhanovsky, Alexander/0000-0001-7370-1164; Mazzola, Mauro/0000-0002-8394-2292; Lanconelli, Christian/0000-0002-9545-1255 FU Italian Research Programme in Antarctica (PNRA); AERONET network in the Arctic and Antarctica; AEROCAN/AERONET sub-network in the Canadian Arctic FX The present study was developed as a part of the CLIMSLIP (Climate Impacts of Short-Lived Pollutants in the Polar Regions) joint project, approved by the European Polar Consortium and coordinated by A. Stohl at NILU (Kjeller, Norway), and supported by the Italian Research Programme in Antarctica (PNRA). The authors gratefully acknowledge the Office of Antarctic Observation of the Japan Meteorological Agency (Tokyo, Japan), for supplying the data-set of EKO sun-photometer measurements carried out at Syowa (Antarctica) from 2000 to 2011. In general we acknowledge the support provided by the AERONET network in the Arctic and Antarctica and the AEROCAN/AERONET sub-network in the Canadian Arctic. The Cimel sun-photometer data at Barrow (Alaska) were collected by the U.S. Department of Energy as part of the Atmospheric Radiation Measurement Program Climate Research Facility (ARM) and processed by AERONET. James H. Butler (Global Monitoring Division, Earth System Research Laboratory (ERL), National Oceanic and Atmospheric Administration (NOAA), Boulder, Colorado, USA) is acknowledged for his effort in establishing and maintaining the activities at the AERONET South Pole Amundsen-Scott base. The colleagues D. G. Chernov, Yu. S. Turchinovich and Victor V. Polkin, (V. E. Zuev Institute of Atmospheric Optics (IAO), Siberian Branch, Russian Academy of Sciences, Tomsk, Russia) are also acknowledged for their participation to field measurements conducted at Barentsburg and in Antarctica. Author's acknowledgements are also due to the managerial and operational support given by M. Fily (LGGE, CNRS, Grenoble, France) at the AERONET Antarctic Dome Concordia station, and to the P.I.s of the AERONET/MAN cruises conducted in the Arctic and Antarctic Oceans, during which Microtops measurements of aerosol optical thickness were performed and examined in the present analysis: Patricia K. Quinn (NOAA Pacific Marine Environmental Laboratory, Seattle, Washington, USA), Andrey Proshutinsky (Woods Hole Oceanographic Institution, Woods Hole, Massachusetts, USA), Carlos Duarte (Instituto Mediterraneo de Estudios Avanzados, Esporles, Mallorca, Spain), Simon Belanger (Universite du Quebec, Rimouski, Quebec, Canada), Elizabeth A. Reid (Naval Research Laboratory, Monterey, California, USA), Gennadi Milinevsky (Space Physics Laboratory, Taras Shevchenko National University of Kyiv, Kyiv, Ukraine), and Heitor Evangelista (Rio de Janeiro State University, Brazil). The analyses and visualisations used in this paper to obtain the sets of MODIS and MISR daily aerosol optical thickness Level-3 data over the Arctic and Antarctic regions were produced with the Giovanni online data system, developed and maintained by the NASA GES DISC. NR 200 TC 12 Z9 13 U1 9 U2 75 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0012-8252 EI 1872-6828 J9 EARTH-SCI REV JI Earth-Sci. Rev. PD JAN PY 2015 VL 140 BP 108 EP 157 DI 10.1016/j.earscirev.2014.11.001 PG 50 WC Geosciences, Multidisciplinary SC Geology GA AY9IJ UT WOS:000347863500006 ER PT J AU Lee, S Gerdes, K AF Lee, Shiwoo Gerdes, Kirk TI Functional Nanostructure Engineering of SOFC Cathode by Solution Infiltration SO ECS ELECTROCHEMISTRY LETTERS LA English DT Article ID OXIDE FUEL-CELLS; PERFORMANCE; ELECTRODES; LACOO3 AB Formation and distribution of infiltrated electrocatalyst were controlled through solution chemistry and correlated cathode performance was investigated for a La0.6Sr0.4Co0.9Pt0.1O3-infiltrated solid-oxide fuel cell (SOFC). Selection of solvent and polymeric additives constituting the slip dramatically affected the infiltrate particles' spatial configuration, and finally determined cathode activity under cell operational conditions. The results imply that microstructural features such as 3-dimensional distribution and interconnectivity of infiltrated nanoparticles must be considered when evaluating activity and stability of cathodes. A modified infiltration process utilizing a mixed solvent of low surface tension and functionally sequenced infiltration was effectively applied to manipulate cathode microstructure. (C) 2015 The Electrochemical Society. C1 [Lee, Shiwoo; Gerdes, Kirk] US DOE, Natl Energy Technol Lab, Morgantown, WV 26507 USA. RP Lee, S (reprint author), US DOE, Natl Energy Technol Lab, Morgantown, WV 26507 USA. EM leesn@contr.netl.doe.gov NR 20 TC 0 Z9 0 U1 5 U2 20 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 2162-8726 EI 2162-8734 J9 ECS ELECTROCHEM LETT JI ECS Electrochem. Lett. PY 2015 VL 4 IS 3 BP F17 EP F20 DI 10.1149/2.0051503eel PG 4 WC Electrochemistry; Materials Science, Multidisciplinary SC Electrochemistry; Materials Science GA AZ9YN UT WOS:000348570700002 ER PT J AU Saad, L Feteha, MY Ebrahim, S Soliman, M Abdel-Fattah, TM AF Saad, Laila Feteha, M. Y. Ebrahim, Sh Soliman, Moataz Abdel-Fattah, Tarek M. TI Dye Sensitized Solar Cell Based on Polyaniline-Carbon Nanotubes/Graphite Composite (vol 3, pg M55, 2014) SO ECS JOURNAL OF SOLID STATE SCIENCE AND TECHNOLOGY LA English DT Correction C1 [Saad, Laila; Feteha, M. Y.; Ebrahim, Sh; Soliman, Moataz] Univ Alexandria, Inst Grad Studies & Res, Dept Mat Sci, Alexandria, Egypt. [Abdel-Fattah, Tarek M.] Christopher Newport Univ, Appl Res Ctr, Thomas Jefferson Natl Accelerator Facil, Newport News, VA 23606 USA. [Abdel-Fattah, Tarek M.] Christopher Newport Univ, Dept Mol Biol & Chem, Newport News, VA 23606 USA. RP Saad, L (reprint author), Univ Alexandria, Inst Grad Studies & Res, Dept Mat Sci, Alexandria, Egypt. NR 1 TC 0 Z9 0 U1 3 U2 9 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 2162-8769 J9 ECS J SOLID STATE SC JI ECS J. Solid State Sci. Technol. PY 2015 VL 4 IS 2 BP X1 EP X1 DI 10.1149/2.0021502jss PG 1 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA AZ7QD UT WOS:000348412100019 ER PT J AU Copping, A Hanna, L Van Cleve, B Blake, K Anderson, RM AF Copping, Andrea Hanna, Luke Van Cleve, Brie Blake, Kara Anderson, Richard M. TI Environmental Risk Evaluation System-an Approach to Ranking Risk of Ocean Energy Development on Coastal and Estuarine Environments SO ESTUARIES AND COASTS LA English DT Article DE Ocean energy devices; Environmental risk assessment; Tidal energy generation; Wave energy generation; Offshore wind energy generation ID WIND FARM CONSTRUCTION; TIDAL CURRENT ENERGY; RENEWABLE ENERGY; POTENTIAL IMPACTS; BOOSTER BIOCIDES; MYOTIS-SODALIS; KILLER WHALES; FISH; DYNAMICS; BARRIERS AB The pressure to develop new and renewable forms of energy to combat climate change, ocean acidification, and energy security has encouraged exploration of sources of power generation from the ocean. One of the major challenges to deploying these devices is discerning the likely effects those devices and associated systems will have on the marine environment. Determining the effects each device design and deployment system may have on specific marine animals and habitats, estimating the extent of those effects upon the resiliency of the ecosystem, and designing appropriate mitigation measures to protect against degradation all pose substantial challenges. With little direct observational or experimental data available on the effects of wave, tidal, and offshore wind devices on marine animals, habitats, and ecosystem processes, researchers have developed the Environmental Risk Evaluation System (ERES) to provide preliminary assessments of these risks and to act as a framework for integrating future data on direct interactions of ocean energy devices with the environment. Using biophysical risk factors, interactions of marine animals and seabirds, with ocean energy devices and systems, are examined; potential effects on habitats, and changes in processes such as sedimentation patterns and water quality, are also considered. The risks associated with specific interactions for which data are more readily available are explored including interactions between ocean energy devices and surface vessels, toxicity of anti-biofouling paints, and potential for harm to animals from turbine blade strike. ERES also examines the effect that environmental regulations have on the deployment and operation of ocean energy devices. C1 [Copping, Andrea; Hanna, Luke; Van Cleve, Brie; Blake, Kara] Pacific NW Natl Lab, Seattle, WA 98109 USA. RP Copping, A (reprint author), Pacific NW Natl Lab, Seattle, WA 98109 USA. EM andrea.copping@pnnl.gov NR 93 TC 6 Z9 6 U1 9 U2 86 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1559-2723 EI 1559-2731 J9 ESTUAR COAST JI Estuaries Coasts PD JAN PY 2015 VL 38 SU 1 BP S287 EP S302 DI 10.1007/s12237-014-9816-3 PG 16 WC Environmental Sciences; Marine & Freshwater Biology SC Environmental Sciences & Ecology; Marine & Freshwater Biology GA AZ0TE UT WOS:000347956700024 ER PT J AU Wang, TP Yang, ZQ Copping, A AF Wang, Taiping Yang, Zhaoqing Copping, Andrea TI A Modeling Study of the Potential Water Quality Impacts from In-Stream Tidal Energy Extraction SO ESTUARIES AND COASTS LA English DT Article DE Tidal energy; Numerical model; Water quality; Flushing rate; Vertical mixing ID EUTROPHICATION MODEL; RENEWABLE ENERGY; CHESAPEAKE BAY; COASTAL OCEAN; MINAS PASSAGE; POWER; ESTUARIES; RESOURCE; NITROGEN; CURRENTS AB To assess the effects of tidal energy extraction on water quality in a simplified estuarine system, which consists of a tidal bay connected to the coastal ocean through a narrow channel where energy is extracted using in-stream tidal turbines, a three-dimensional coastal ocean model with built-in tidal turbine and water quality modules was applied. The effects of tidal energy extraction on water quality were examined for two energy extraction scenarios as compared with the baseline condition. It was found, in general, that the environmental impacts associated with energy extraction depend highly on the amount of power extracted from the system. Model results indicate that, as a result of energy extraction from the channel, the competition between decreased flushing rates in the bay and increased vertical mixing in the channel directly affects water quality responses in the bay. The decreased flushing rates tend to cause a stronger but negative impact on water quality. On the other hand, the increased vertical mixing could lead to higher bottom dissolved oxygen at times. As the first modeling effort directly aimed at examining the impacts of tidal energy extraction on estuarine water quality, this study demonstrates that numerical models can serve as a very useful tool for this purpose. However, more careful efforts are warranted to address system-specific environmental issues in real-world, complex estuarine systems. C1 [Wang, Taiping; Yang, Zhaoqing; Copping, Andrea] Pacific NW Natl Lab, Seattle, WA 98109 USA. RP Wang, TP (reprint author), Pacific NW Natl Lab, 1100 Dexter Ave North,Suite 400, Seattle, WA 98109 USA. EM taiping.wang@pnnl.gov FU Wind and Water Power Program under the Office of Energy Efficiency and Renewable Energy, US Department of Energy FX This study was funded by the Wind and Water Power Program under the Office of Energy Efficiency and Renewable Energy, US Department of Energy. The authors would like to thank the reviewers for their help in improving the quality of the manuscript. Dr. Changsheng Chen at University of Massachusetts Dartmouth is also acknowledged for providing the authors the FVCOM source code. NR 49 TC 3 Z9 3 U1 5 U2 14 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1559-2723 EI 1559-2731 J9 ESTUAR COAST JI Estuaries Coasts PD JAN PY 2015 VL 38 SU 1 BP S173 EP S186 DI 10.1007/s12237-013-9718-9 PG 14 WC Environmental Sciences; Marine & Freshwater Biology SC Environmental Sciences & Ecology; Marine & Freshwater Biology GA AZ0TE UT WOS:000347956700015 ER PT J AU Yang, ZQ Wang, TP AF Yang, Zhaoqing Wang, Taiping TI Modeling the Effects of Tidal Energy Extraction on Estuarine Hydrodynamics in a Stratified Estuary SO ESTUARIES AND COASTS LA English DT Article DE Tidal stream energy; Numerical modeling; Vertical mixing; Stratification; Estuarine circulation ID COASTAL OCEAN MODEL; FINITE-VOLUME; BAY SYSTEM; POWER; CURRENTS; CIRCULATION; CHANNEL; ARRAYS AB A 3-D coastal ocean model with a tidal turbine module was used in this paper to study the effects of tidal energy extraction on temperature and salinity stratification and density-driven two-layer estuarine circulation. Numerical experiments with various turbine array configurations were carried out to investigate the changes in tidally averaged temperature, salinity, and velocity profiles in an idealized stratified estuary that connects to coastal water through a narrow tidal channel. The model was driven by tides, river inflow, and sea surface heat flux. To represent the realistic size of commercial tidal farms, model simulations were conducted based on a small percentage (less than 10 %) of the total number of turbines that would generate the maximum extractable energy in the system. Model results show that extraction of tidal in-stream energy will increase the vertical mixing and decrease the stratification in the estuary. Installation of in-stream tidal farm will cause a phase lag in tidal wave, which leads to large differences in tidal currents between baseline and tidal farm conditions. Extraction of tidal energy in an estuarine system has stronger impact on the tidally averaged salinity, temperature, and velocity in the surface layer than the bottom layer even though the turbine hub height is close to the bottom. Finally, model results also indicate that extraction of tidal energy weakens the two-layer estuarine circulation, especially during neap tides when tidal mixing is weakest and energy extraction is smallest. C1 [Yang, Zhaoqing; Wang, Taiping] Pacific NW Natl Lab, Seattle, WA 98109 USA. RP Yang, ZQ (reprint author), Pacific NW Natl Lab, 1100 Dexter Ave North,Ste 400, Seattle, WA 98109 USA. EM zhaoqing.yang@pnnl.gov FU Wind and Water Power Program under the Office of Energy Efficiency and Renewable Energy, U.S. Department of Energy FX This study is funded by the Wind and Water Power Program under the Office of Energy Efficiency and Renewable Energy, U.S. Department of Energy. The authors thank Dr. Andrea Copping for discussion throughout this study. NR 30 TC 3 Z9 3 U1 2 U2 13 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1559-2723 EI 1559-2731 J9 ESTUAR COAST JI Estuaries Coasts PD JAN PY 2015 VL 38 SU 1 BP S187 EP S202 DI 10.1007/s12237-013-9684-2 PG 16 WC Environmental Sciences; Marine & Freshwater Biology SC Environmental Sciences & Ecology; Marine & Freshwater Biology GA AZ0TE UT WOS:000347956700016 ER PT J AU Zydlewski, GB Copping, AE Redden, AM AF Zydlewski, Gayle Barbin Copping, Andrea E. Redden, Anna M. TI Special Issue: Renewable Ocean Energy Development and the Environment SO ESTUARIES AND COASTS LA English DT Article DE Renewable ocean energy; Tidal energy development; Wave energy development AB Renewable energy harvested from ocean waves, tides, and winds as part of a portfolio of reliable low-carbon energy sources to address climate change and energy security is under consideration by many nations. Engineering designs and characterization of the harvestable resource are moving forward, particularly in Europe, Asia, and North America. At the same time, stakeholders and regulators have expressed the need to understand potential effects on marine animals, habitats, and ecosystem processes. These potential effects are prompting researchers and resource managers to examine interactions of species and ocean areas with energy conversion devices. This volume demonstrates the breadth of disciplines engaged in the quest to understand potential effects and the proactive efforts to develop these new sources of energy to the world, in a responsible manner. C1 [Zydlewski, Gayle Barbin] Univ Maine, Sch Marine Sci, Orono, ME 04469 USA. [Copping, Andrea E.] Pacific NW Natl Lab, Coastal Div, Seattle, WA 98109 USA. [Redden, Anna M.] Acadia Univ, Dept Biol, Wolfville, NS B4P 2R6, Canada. RP Copping, AE (reprint author), Pacific NW Natl Lab, Coastal Div, 1100 Dexter Ave N,Suite 400, Seattle, WA 98109 USA. EM andrea.copping@pnnl.gov NR 11 TC 1 Z9 1 U1 9 U2 25 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1559-2723 EI 1559-2731 J9 ESTUAR COAST JI Estuaries Coasts PD JAN PY 2015 VL 38 SU 1 BP S156 EP S158 DI 10.1007/s12237-014-9922-2 PG 3 WC Environmental Sciences; Marine & Freshwater Biology SC Environmental Sciences & Ecology; Marine & Freshwater Biology GA AZ0TE UT WOS:000347956700013 ER PT J AU Scheibe, TD Murphy, EM Chen, XY Rice, AK Carroll, KC Palmer, BJ Tartakovsky, AM Battiato, I Wood, BD AF Scheibe, Timothy D. Murphy, Ellyn M. Chen, Xingyuan Rice, Amy K. Carroll, Kenneth C. Palmer, Bruce J. Tartakovsky, Alexandre M. Battiato, Ilenia Wood, Brian D. TI An Analysis Platform for Multiscale Hydrogeologic Modeling with Emphasis on Hybrid Multiscale Methods SO GROUNDWATER LA English DT Article ID HETEROGENEOUS POROUS-MEDIA; FINITE-ELEMENT-METHOD; PORE-SCALE MODELS; PARTIAL-DIFFERENTIAL-EQUATIONS; TIME RANDOM-WALKS; MOLECULAR-DYNAMICS; ALGORITHM REFINEMENT; REACTIVE TRANSPORT; FLOW SIMULATIONS; RESERVOIR SIMULATION AB One of the most significant challenges faced by hydrogeologic modelers is the disparity between the spatial and temporal scales at which fundamental flow, transport, and reaction processes can best be understood and quantified (e.g., microscopic to pore scales and seconds to days) and at which practical model predictions are needed (e.g., plume to aquifer scales and years to centuries). While the multiscale nature of hydrogeologic problems is widely recognized, technological limitations in computation and characterization restrict most practical modeling efforts to fairly coarse representations of heterogeneous properties and processes. For some modern problems, the necessary level of simplification is such that model parameters may lose physical meaning and model predictive ability is questionable for any conditions other than those to which the model was calibrated. Recently, there has been broad interest across a wide range of scientific and engineering disciplines in simulation approaches that more rigorously account for the multiscale nature of systems of interest. In this article, we review a number of such approaches and propose a classification scheme for defining different types of multiscale simulation methods and those classes of problems to which they are most applicable. Our classification scheme is presented in terms of a flowchart (Multiscale Analysis Platform), and defines several different motifs of multiscale simulation. Within each motif, the member methods are reviewed and example applications are discussed. We focus attention on hybrid multiscale methods, in which two or more models with different physics described at fundamentally different scales are directly coupled within a single simulation. Very recently these methods have begun to be applied to groundwater flow and transport simulations, and we discuss these applications in the context of our classification scheme. As computational and characterization capabilities continue to improve, we envision that hybrid multiscale modeling will become more common and also a viable alternative to conventional single-scale models in the near future. C1 [Scheibe, Timothy D.; Murphy, Ellyn M.; Chen, Xingyuan; Rice, Amy K.; Carroll, Kenneth C.; Palmer, Bruce J.; Tartakovsky, Alexandre M.] Pacific NW Natl Lab, Richland, WA 99352 USA. [Rice, Amy K.] Colorado Sch Mines, Ctr Expt Study Subsurface Environm Proc, Golden, CO 80401 USA. [Carroll, Kenneth C.] New Mexico State Univ, Las Cruces, NM 88003 USA. [Battiato, Ilenia] Clemson Univ, Dept Mech Engn, Clemson, SC 29631 USA. [Wood, Brian D.] Oregon State Univ, Dept Chem Engn, Corvallis, OR 97331 USA. RP Scheibe, TD (reprint author), Pacific NW Natl Lab, POB 999,MS K9-36, Richland, WA 99352 USA. EM Tim.Scheibe@pnnl.gov RI Carroll, Kenneth/H-5160-2011; Scheibe, Timothy/A-8788-2008; OI Carroll, Kenneth/0000-0003-2097-9589; Scheibe, Timothy/0000-0002-8864-5772; Wood, Brian/0000-0003-3152-7852 FU U.S. Department of Energy, Office of Science; National Science Foundation (NSF); Laboratory-Directed Research and Development program at Pacific Northwest National Laboratory (PNNL) through the Carbon Sequestration Initiative; National Science Foundation [EAR-1246297]; NSF [1141488] FX This work was supported by the U.S. Department of Energy, Office of Science, under the Scientific Discovery through Advanced Computing (SciDAC) and Applied Mathematics programs, by the National Science Foundation (NSF) through the Hydrologic Sciences program in the Division of Earth Sciences, and by the Laboratory-Directed Research and Development program at Pacific Northwest National Laboratory (PNNL) through the Carbon Sequestration Initiative. Ilenia Battiato was supported by the National Science Foundation award EAR-1246297. Dr. Wood's contributions were supported by NSF Grant 1141488. PNNL is operated for the U. S. Department of Energy by Battelle Memorial Institute. NR 157 TC 12 Z9 12 U1 7 U2 33 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0017-467X EI 1745-6584 J9 GROUNDWATER JI Groundwater PD JAN-FEB PY 2015 VL 53 IS 1 BP 38 EP 56 DI 10.1111/gwat.12179 PG 19 WC Geosciences, Multidisciplinary; Water Resources SC Geology; Water Resources GA AZ1EA UT WOS:000347981800010 PM 24628122 ER PT J AU Harrington, AD Smirnov, A Tsirka, SE Schoonen, MAA AF Harrington, Andrea D. Smirnov, Alexander Tsirka, Stella E. Schoonen, Martin A. A. TI Metal-sulfide mineral ores, Fenton chemistry and disease - Particle induced inflammatory stress response in lung cells SO INTERNATIONAL JOURNAL OF HYGIENE AND ENVIRONMENTAL HEALTH LA English DT Article DE Ore minerals; Fenton chemistry; Oxidative stress; Inflammatory stress response; Occupational disease ID HYDROGEN-PEROXIDE; OXIDATIVE STRESS; PARTICULATE MATTER; OXYGEN; TOXICITY; DEATH; SPECTROSCOPY; CHALCOPYRITE; SPHALERITE; EXPOSURE AB The inhalation of mineral particulates and other earth materials, such as coal, can initiate or enhance disease in humans. Workers in occupations with high particulate exposure, such as mining, are particularly at risk. The ability of a material to generate an inflammatory stress response (ISR), a measure of particle toxicity, is a useful tool in evaluating said exposure risk. 1SR is defined as the upregulation of cellular reactive oxygen species (ROS) normalized to cell viability. This study compares the ISR of A549 human lung epithelial cells after exposure to well-characterized common metal-sulfide ore mineral separates. The evaluation of the deleterious nature of ore minerals is based on a range of particle loadings (serial dilutions of 0.002 m(2)/mL stock) and exposure periods (beginning at 30 min and measured systematically for up to 24 h). There is a wide range in ISR values generated by the ore minerals. The ISR values produced by the sphalerite samples are within the range of inert materials. Arsenopyrite generated a small ISR that was largely driven by cell death. Galena showed a similar, but more pronounced response. Copper-bearing ore minerals generated the greatest ISR, both by upregulating cellular ROS and generating substantial and sustained cell death. Chalcopyrite and bornite, both containing ferrous iron, generated the greatest ISR overall. Particles containing Fenton metals as major constituents produce the highest ISR, while other heavy metals mainly generate cell death. This study highlights the importance of evaluating the chemistry, oxidation states and structure of a material when assessing risk management. (C) 2014 Elsevier GmbH. All rights reserved. C1 [Harrington, Andrea D.; Schoonen, Martin A. A.] SUNY Stony Brook, Dept Geosci Earth & Space Sci Bldg, Stony Brook, NY 11784 USA. [Harrington, Andrea D.] NYU, Inst Environm Med, Tuxedo Pk, NY 10987 USA. [Smirnov, Alexander] Dowling Coll, Dept Earth & Marine Sci, Oakdale, NY 11769 USA. [Tsirka, Stella E.] SUNY Stony Brook, Sch Med, Stony Brook, NY 11794 USA. [Schoonen, Martin A. A.] Brookhaven Natl Lab, Dept Environm Sci, Upton, NY 11973 USA. RP Harrington, AD (reprint author), NYU, Inst Environm Med, 57 Old Forge Rd, Tuxedo Pk, NY 10987 USA. EM Andrea.Harrington@nyumc.org; asmirnov@dowling.edu; stella@pharm.stonybrook.edu; martin.schoonen@stonybrook.edu FU Minerals, Metals, Metalloids and Toxicity (3MT) program at Stony Brook University [RO1 NS42168] FX This work was supported by the Minerals, Metals, Metalloids and Toxicity (3MT) program at Stony Brook University, which is funded by NSF-IGERT, and NIH RO1 NS42168 (SET). NR 40 TC 3 Z9 3 U1 4 U2 18 PU ELSEVIER GMBH, URBAN & FISCHER VERLAG PI JENA PA OFFICE JENA, P O BOX 100537, 07705 JENA, GERMANY SN 1438-4639 EI 1618-131X J9 INT J HYG ENVIR HEAL JI Int. J. Hyg. Environ. Health. PD JAN PY 2015 VL 218 IS 1 BP 19 EP 27 DI 10.1016/j.ijheh.2014.07.002 PG 9 WC Public, Environmental & Occupational Health; Infectious Diseases SC Public, Environmental & Occupational Health; Infectious Diseases GA AY6FD UT WOS:000347661800003 PM 25107347 ER PT J AU Giannone, RJ Wurch, LL Heimerl, T Martin, S Yang, ZM Huber, H Rachel, R Hettich, RL Podar, M AF Giannone, Richard J. Wurch, Louie L. Heimerl, Thomas Martin, Stanton Yang, Zamin Huber, Harald Rachel, Reinhard Hettich, Robert L. Podar, Mircea TI Life on the edge: functional genomic response of Ignicoccus hospitalis to the presence of Nanoarchaeum equitans SO ISME JOURNAL LA English DT Article ID PEPTIDE IDENTIFICATION; TRANSCRIPTOME ANALYSIS; ARCHAEAL EVOLUTION; OUTER-MEMBRANE; SP-NOV; INSIGHTS; PROTEOME; HOST; DIVERSITY; ANCESTOR AB The marine hyperthermophilic crenarchaeon Ignicoccus hospitalis supports the propagation on its surface of Nanoarchaeum equitans, an evolutionarily enigmatic archaeon that resembles highly derived parasitic and symbiotic bacteria. The cellular and molecular mechanisms that enable this interarchaea relationship and the intimate physiologic consequences to I. hospitalis are unknown. Here, we used concerted proteomic and transcriptomic analyses to probe into the functional genomic response of I. hospitalis as N. equitans multiplies on its surface. The expression of over 97% of the genes was detected at mRNA level and over 80% of the predicted proteins were identified and their relative abundance measured by proteomics. These indicate that little, if any, of the host genomic information is silenced during growth in the laboratory. The primary response to N. equitans was at the membrane level, with increases in relative abundance of most protein complexes involved in energy generation as well as that of several transporters and proteins involved in cellular membrane stabilization. Similar upregulation was observed for genes and proteins involved in key metabolic steps controlling nitrogen and carbon metabolism, although the overall biosynthetic pathways were marginally impacted. Proliferation of N. equitans resulted, however, in selective downregulation of genes coding for transcription factors and replication and cell cycle control proteins as I. hospitalis shifted its physiology from its own cellular growth to that of its ectosymbiont/parasite. The combination of these multiomic approaches provided an unprecedented level of detail regarding the dynamics of this interspecies interaction, which is especially pertinent as these organisms are not genetically tractable. C1 [Giannone, Richard J.; Martin, Stanton; Yang, Zamin; Hettich, Robert L.; Podar, Mircea] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. [Wurch, Louie L.; Podar, Mircea] Univ Tennessee, Dept Microbiol, Knoxville, TN 37996 USA. [Heimerl, Thomas; Huber, Harald; Rachel, Reinhard] Univ Regensburg, Lehrstuhl Mikrobiol, D-93053 Regensburg, Germany. [Heimerl, Thomas; Huber, Harald; Rachel, Reinhard] Univ Regensburg, Archaeenzentrum, D-93053 Regensburg, Germany. [Martin, Stanton] SAS Inst Inc, Cary, NC USA. RP Podar, M (reprint author), Oak Ridge Natl Lab, Biosci Div, 1 Bethel Valley Rd, Oak Ridge, TN 37831 USA. EM podarm@ornl.gov RI Hettich, Robert/N-1458-2016; OI Hettich, Robert/0000-0001-7708-786X; Podar, Mircea/0000-0003-2776-0205 FU US Department of Energy, Office of Biological and Environmental Research [DE-SC0006654]; Laboratory Directed Research and Development Program of Oak Ridge National Laboratory (ORNL); US Department of Energy; Deutsche Forschungsgemeinschaft FX This research was supported by a grant from the US Department of Energy, Office of Biological and Environmental Research (DE-SC0006654) and by the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory (ORNL). ORNL is managed by UT-Battelle, LLC, for the US Department of Energy. TH, HH and RR were funded by Deutsche Forschungsgemeinschaft. We would like to acknowledge the University of Tennessee Advanced Microscopy and Imaging Center for instrument use, scientific and technical assistance. NR 42 TC 4 Z9 4 U1 2 U2 18 PU NATURE PUBLISHING GROUP PI LONDON PA MACMILLAN BUILDING, 4 CRINAN ST, LONDON N1 9XW, ENGLAND SN 1751-7362 EI 1751-7370 J9 ISME J JI ISME J. PD JAN PY 2015 VL 9 IS 1 BP 101 EP 114 DI 10.1038/ismej.2014.112 PG 14 WC Ecology; Microbiology SC Environmental Sciences & Ecology; Microbiology GA AZ4SK UT WOS:000348212800009 PM 25012904 ER PT J AU Larsen, PE Scott, N Post, AF Field, D Knight, R Hamada, Y Gilbert, JA AF Larsen, Peter E. Scott, Nicole Post, Anton F. Field, Dawn Knight, Rob Hamada, Yuki Gilbert, Jack A. TI Satellite remote sensing data can be used to model marine microbial metabolite turnover SO ISME JOURNAL LA English DT Article ID WESTERN ENGLISH-CHANNEL; SEED BANK; OCEAN; COMMUNITIES; DIVERSITY; BACTERIA; TEMPERATURE; ALGORITHM; WATERS AB Sampling ecosystems, even at a local scale, at the temporal and spatial resolution necessary to capture natural variability in microbial communities are prohibitively expensive. We extrapolated marine surface microbial community structure and metabolic potential from 72 16S rRNA amplicon and 8 metagenomic observations using remotely sensed environmental parameters to create a system- scale model of marine microbial metabolism for 5904 grid cells (49km(2)) in the Western English Chanel, across 3 years of weekly averages. Thirteen environmental variables predicted the relative abundance of 24 bacterial Orders and 1715 unique enzyme-encoding genes that encode turnover of 2893 metabolites. The genes' predicted relative abundance was highly correlated (Pearson Correlation 0.72, P-value <10(-6)) with their observed relative abundance in sequenced metagenomes. Predictions of the relative turnover (synthesis or consumption) of CO2 were significantly correlated with observed surface CO2 fugacity. The spatial and temporal variation in the predicted relative abundances of genes coding for cyanase, carbon monoxide and malate dehydrogenase were investigated along with the predicted inter-annual variation in relative consumption or production of similar to 3000 metabolites forming six significant temporal clusters. These spatiotemporal distributions could possibly be explained by the co-occurrence of anaerobic and aerobic metabolisms associated with localized plankton blooms or sediment resuspension, which facilitate the presence of anaerobic micro-niches. This predictive model provides a general framework for focusing future sampling and experimental design to relate biogeochemical turnover to microbial ecology. C1 [Larsen, Peter E.] Argonne Natl Lab, Biosci Div, Argonne, IL 60439 USA. [Scott, Nicole; Gilbert, Jack A.] Univ Chicago, Dept Ecol & Evolut, Chicago, IL 60637 USA. [Post, Anton F.] Marine Biol Lab, Josephine Bay Paul Ctr Comparat Mol Biol & Evolut, Woods Hole, MA 02543 USA. [Field, Dawn] NERC, Ctr Ecol & Hydrol, Wallingford, Oxon, England. [Knight, Rob] Univ Colorado, Dept Chem & Biochem, BioFrontiers Inst, Boulder, CO 80309 USA. [Hamada, Yuki] Argonne Natl Lab, Div Environm Sci, Argonne, IL 60439 USA. [Gilbert, Jack A.] Argonne Natl Lab, Inst Genom & Syst Biol, Argonne, IL 60439 USA. RP Gilbert, JA (reprint author), Argonne Natl Lab, Inst Genom & Syst Biol, 9700 S Cass Ave, Argonne, IL 60439 USA. EM gilbertjack@anl.gov RI Knight, Rob/D-1299-2010 FU US Department of Energy [DE-AC02-06CH11357]; Howard Hughes Medical Institute FX This work was supported by the US Department of Energy under Contract DE-AC02-06CH11357 and by the Howard Hughes Medical Institute. We also thank the anonymous reviewers from multiple journals who significantly helped us to revise and refine this work to improve the clarity and impact. NR 41 TC 5 Z9 5 U1 3 U2 31 PU NATURE PUBLISHING GROUP PI LONDON PA MACMILLAN BUILDING, 4 CRINAN ST, LONDON N1 9XW, ENGLAND SN 1751-7362 EI 1751-7370 J9 ISME J JI ISME J. PD JAN PY 2015 VL 9 IS 1 BP 166 EP 179 DI 10.1038/ismej.2014.107 PG 14 WC Ecology; Microbiology SC Environmental Sciences & Ecology; Microbiology GA AZ4SK UT WOS:000348212800014 PM 25072414 ER PT J AU Mosier, AC Li, Z Thomas, BC Hettich, RL Pan, CL Banfield, JF AF Mosier, Annika C. Li, Zhou Thomas, Brian C. Hettich, Robert L. Pan, Chongle Banfield, Jillian F. TI Elevated temperature alters proteomic responses of individual organisms within a biofilm community SO ISME JOURNAL LA English DT Article ID IN-SITU DETECTION; TANDEM MASS TAGS; MICROBIAL COMMUNITY; QUANTITATIVE PROTEOMICS; ESCHERICHIA-COLI; PHYLOGENETIC IDENTIFICATION; VIRAL LYSIS; PROTEIN; BACTERIAL; LEPTOSPIRILLUM AB Microbial communities that underpin global biogeochemical cycles will likely be influenced by elevated temperature associated with environmental change. Here, we test an approach to measure how elevated temperature impacts the physiology of individual microbial groups in a community context, using a model microbial-based ecosystem. The study is the first application of tandem mass tag (TMT)-based proteomics to a microbial community. We accurately, precisely and reproducibly quantified thousands of proteins in biofilms growing at 40, 43 and 46 degrees C. Elevated temperature led to upregulation of proteins involved in amino-acid metabolism at the level of individual organisms and the entire community. Proteins from related organisms differed in their relative abundance and functional responses to temperature. Elevated temperature repressed carbon fixation proteins from two Leptospirillum genotypes, whereas carbon fixation proteins were significantly upregulated at higher temperature by a third member of this genus. Leptospirillum group III bacteria may have been subject to viral stress at elevated temperature, which could lead to greater carbon turnover in the microbial food web through the release of viral lysate. Overall, these findings highlight the utility of proteomics-enabled community-based physiology studies, and provide a methodological framework for possible extension to additional mixed culture and environmental sample analyses. C1 [Mosier, Annika C.; Thomas, Brian C.; Banfield, Jillian F.] Univ Calif Berkeley, Dept Earth & Planetary Sci, Berkeley, CA 94720 USA. [Li, Zhou; Hettich, Robert L.; Pan, Chongle] Oak Ridge Natl Lab, Oak Ridge, TN USA. [Li, Zhou] Univ Tennessee, Oak Ridge Natl Lab, Grad Sch Genome Sci & Technol, Knoxville, TN USA. [Banfield, Jillian F.] Univ Calif Berkeley, Dept Environm Sci Policy & Management, Berkeley, CA 94720 USA. RP Mosier, AC (reprint author), Univ Calif Berkeley, Dept Earth & Planetary Sci, 307 McCone Hall,MC4767, Berkeley, CA 94720 USA. EM annika.mosier@gmail.com; jbanfield@berkeley.edu RI Li, Zhou/L-7976-2015; Hettich, Robert/N-1458-2016 OI Hettich, Robert/0000-0001-7708-786X FU U.S. Department of Energy [DE-FG02-10ER64996, DE-SC0004918] FX We thank the late T. W. Arman (President, Iron Mountain Mines) for providing access to the Richmond Mine. We also thank R. Sugarek (Environmental Protection Agency) for site access and R. Carver and M. Jones for on-site assistance. We thank Susan Spaulding, Nicholas Justice and Kyle Frischkorn for laboratory assistance. Funding was provided by the U.S. Department of Energy, through the Carbon-Cycling (DE-FG02-10ER64996) and Knowledgebase (DE-SC0004918) programs. NR 78 TC 9 Z9 9 U1 5 U2 25 PU NATURE PUBLISHING GROUP PI LONDON PA MACMILLAN BUILDING, 4 CRINAN ST, LONDON N1 9XW, ENGLAND SN 1751-7362 EI 1751-7370 J9 ISME J JI ISME J. PD JAN PY 2015 VL 9 IS 1 BP 180 EP 194 DI 10.1038/ismej.2014.113 PG 15 WC Ecology; Microbiology SC Environmental Sciences & Ecology; Microbiology GA AZ4SK UT WOS:000348212800015 PM 25050524 ER PT J AU Wang, GS Jagadamma, S Mayes, MA Schadt, CW Steinweg, JM Gu, LH Post, WM AF Wang, Gangsheng Jagadamma, Sindhu Mayes, Melanie A. Schadt, Christopher W. Steinweg, J. Megan Gu, Lianhong Post, Wilfred M. TI Microbial dormancy improves development and experimental validation of ecosystem model SO ISME JOURNAL LA English DT Article ID CARBON-USE EFFICIENCY; SOIL ORGANIC-MATTER; TEMPERATURE SENSITIVITY; GLOBAL OPTIMIZATION; COMMUNITY STRUCTURE; THERMAL ADAPTATION; THEORETICAL-MODEL; ENZYME-ACTIVITIES; DECOMPOSITION; RESPIRATION AB Climate feedbacks from soils can result from environmental change followed by response of plant and microbial communities, and/or associated changes in nutrient cycling. Explicit consideration of microbial life-history traits and functions may be necessary to predict climate feedbacks owing to changes in the physiology and community composition of microbes and their associated effect on carbon cycling. Here we developed the microbial enzyme-mediated decomposition (MEND) model by incorporating microbial dormancy and the ability to track multiple isotopes of carbon. We tested two versions of MEND, that is, MEND with dormancy (MEND) and MEND without dormancy (MEND_wod), against long-term (270 days) carbon decomposition data from laboratory incubations of four soils with isotopically labeled substrates. MEND_wod adequately fitted multiple observations (total C-CO2 and C-14-CO2 respiration, and dissolved organic carbon), but at the cost of significantly underestimating the total microbial biomass. MEND improved estimates of microbial biomass by 20-71% over MEND_wod. We also quantified uncertainties in parameters and model simulations using the Critical Objective Function Index method, which is based on a global stochastic optimization algorithm, as well as model complexity and observational data availability. Together our model extrapolations of the incubation study show that long-term soil incubations with experimental data for multiple carbon pools are conducive to estimate both decomposition and microbial parameters. These efforts should provide essential support to future field-and global-scale simulations, and enable more confident predictions of feedbacks between environmental change and carbon cycling. C1 [Wang, Gangsheng; Jagadamma, Sindhu; Mayes, Melanie A.; Gu, Lianhong; Post, Wilfred M.] Oak Ridge Natl Lab, Div Environm Sci, Oak Ridge, TN 37831 USA. [Wang, Gangsheng; Jagadamma, Sindhu; Mayes, Melanie A.; Schadt, Christopher W.; Steinweg, J. Megan; Gu, Lianhong; Post, Wilfred M.] Oak Ridge Natl Lab, Climate Change Sci Inst, Oak Ridge, TN 37831 USA. [Schadt, Christopher W.; Steinweg, J. Megan] Oak Ridge Natl Lab, Biosci Div, Oak Ridge, TN 37831 USA. RP Wang, GS (reprint author), Oak Ridge Natl Lab, Div Environm Sci, Bldg 4500N,F129-S,MS-6301, Oak Ridge, TN 37831 USA. EM wangg@ornl.gov RI Schadt, Christopher/B-7143-2008; Gu, Lianhong/H-8241-2014 OI Schadt, Christopher/0000-0001-8759-2448; Gu, Lianhong/0000-0001-5756-8738 FU Laboratory Directed Research and Development Program of the Oak Ridge National Laboratory (ORNL); US Department of Energy (DOE) Biological and Environmental Research (BER) program; US DOE [DE-AC05-00OR22725] FX This research was funded by the Laboratory Directed Research and Development Program of the Oak Ridge National Laboratory (ORNL) and by the US Department of Energy (DOE) Biological and Environmental Research (BER) program. ORNL is managed by UT-Battelle, LLC, for the US DOE under contract DE-AC05-00OR22725. The authors appreciate the insightful reviews of Dr Paul Hanson on earlier drafts of the manuscript. We also thank the two anonymous reviewers for their constructive comments. NR 71 TC 14 Z9 14 U1 11 U2 45 PU NATURE PUBLISHING GROUP PI LONDON PA MACMILLAN BUILDING, 4 CRINAN ST, LONDON N1 9XW, ENGLAND SN 1751-7362 EI 1751-7370 J9 ISME J JI ISME J. PD JAN PY 2015 VL 9 IS 1 BP 226 EP 237 DI 10.1038/ismej.2014.120 PG 12 WC Ecology; Microbiology SC Environmental Sciences & Ecology; Microbiology GA AZ4SK UT WOS:000348212800019 PM 25012899 ER PT J AU Liu, ZY Xu, WQ Yao, SY Johnson-Peck, AC Zhao, FZ Michorczyk, P Kubacka, A Stach, EA Fernandez-Garcia, M Senanayake, SD Rodriguez, JA AF Liu, Zongyuan Xu, Wenqian Yao, Siyu Johnson-Peck, Aaron C. Zhao, Fuzhen Michorczyk, Piotr Kubacka, Anna Stach, Eric A. Fernandez-Garcia, Marcos Senanayake, Sanjaya D. Rodriguez, Jose A. TI Superior performance of Ni-W-Ce mixed-metal oxide catalysts for ethanol steam reforming: Synergistic effects of W- and Ni-dopants SO JOURNAL OF CATALYSIS LA English DT Article DE Steam reforming of ethanol; Lattice strain; Oxygen vacancies; Nickel; Ceria; Tungsten; DRIFTS; XRD; XAFS ID X-RAY-ABSORPTION; GAS SHIFT REACTION; CHEMICAL-PROPERTIES; REACTION-MECHANISM; IN-SITU; STRUCTURAL-CHARACTERIZATION; IR SPECTROSCOPY; THIN-FILMS; HYDROGEN; NANOPARTICLES AB The ethanol steam reforming (ESA) reaction was studied over a series of Ni-W-Ce oxide catalysts. The structures of the catalysts were characterized using in situ techniques including X-ray diffraction, pair distribution function, X-ray absorption fine structure, and transmission electron microscopy; while possible surface intermediates for the ESR reaction were investigated by diffuse reflectance infrared Fourier transform spectroscopy. In these materials, all the W and part of the Ni were incorporated into the CeO2 lattice, with the remaining Ni forming highly dispersed nano-NiO (<2 nm) outside the Ni-W-Ce oxide structure. The nano-NiO was reduced to Ni under ESR conditions. The Ni-W-Ce system exhibited a much larger lattice strain than those seen for Ni-Ce and W-Ce. Synergistic effects between Ni and W inside ceria produced a substantial amount of defects and O vacancies that led to high catalytic activity, selectivity, and stability (i.e., resistance to coke formation) during ethanol steam reforming. (c) 2014 Elsevier Inc. All rights reserved. C1 [Liu, Zongyuan; Xu, Wenqian; Yao, Siyu; Zhao, Fuzhen; Senanayake, Sanjaya D.; Rodriguez, Jose A.] Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA. [Liu, Zongyuan; Rodriguez, Jose A.] SUNY Stony Brook, Dept Chem, Stony Brook, NY 11794 USA. [Johnson-Peck, Aaron C.; Stach, Eric A.] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. [Michorczyk, Piotr; Kubacka, Anna; Fernandez-Garcia, Marcos] CSIC, Inst Catalisis & Petroleoquim, E-28049 Madrid, Spain. [Michorczyk, Piotr] Cracow Univ Technol, Inst Organ Chem & Technol, PL-31155 Krakow, Poland. RP Rodriguez, JA (reprint author), Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA. EM rodrigez@bnl.gov RI Kubacka, Anna /B-8054-2015; Stach, Eric/D-8545-2011; Fernandez-Garcia, Marcos/A-8122-2014; Senanayake, Sanjaya/D-4769-2009; OI Kubacka, Anna /0000-0002-3504-0032; Stach, Eric/0000-0002-3366-2153; Senanayake, Sanjaya/0000-0003-3991-4232; Liu, Zongyuan/0000-0001-8526-5590 FU U.S. Department of Energy, Office of Science [DE-AC02-98CH10886]; U.S. Department of Energy, Office of Basic Energy Sciences [DE-AC02-98CH10886]; National Natural Science Foundation of China [21303272]; China Scholarship Council [201208420304]; Spanish MINECO FX The research carried out at National Synchrotron Light Source, Brookhaven National Laboratory, was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences (DE-AC02-98CH10886 contract). STEEM-EELS data were obtained at the Center for Functional Nanomaterials, supported by the U.S. Department of Energy, Office of Basic Energy Sciences under Contract No. DE-AC02-98CH10886. The financial support from the National Natural Science Foundation of China (Grant 21303272) and China Scholarship Council (File No. 201208420304) is gratefully acknowledged. Anna Kubacka thanks Spanish MINECO for a "Ramon y Cajal" postdoctoral fellowship. NR 50 TC 14 Z9 14 U1 7 U2 78 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 0021-9517 EI 1090-2694 J9 J CATAL JI J. Catal. PD JAN PY 2015 VL 321 BP 90 EP 99 DI 10.1016/j.jcat.2014.10.017 PG 10 WC Chemistry, Physical; Engineering, Chemical SC Chemistry; Engineering GA AZ5PA UT WOS:000348271300011 ER PT J AU Conboy, TM Carlson, MD Rochau, GE AF Conboy, T. M. Carlson, M. D. Rochau, G. E. TI Dry-Cooled Supercritical CO2 Power for Advanced Nuclear Reactors SO JOURNAL OF ENGINEERING FOR GAS TURBINES AND POWER-TRANSACTIONS OF THE ASME LA English DT Article ID DIOXIDE BRAYTON CYCLE; CARBON-DIOXIDE; GAS-TURBINE; PLANT; ENERGY AB Currently, waste heat rejection from electrical power systems accounts for the largest fraction of water withdrawals from the U.S. fresh water table. Siting of nuclear power plants is limited to areas with access to a large natural supply of fresh or sea water. Due to a rise in energy needs and increased concern over environmental impact, dry air cooling systems are poised to play a large role in the future energy economy. In practice, the implementation of dry air-cooled condensing systems at steam plants has proven to be capital-intensive and requires the power cycle to take a significant efficiency penalty. These shortcomings are fundamental to dry-air steam condensation, which must occur at a fixed temperature. Closed-cycle gas turbines are an alternative to the conventional steam Rankine plant that allows for much improved dry heat rejection compatibility. Recent research into advanced nuclear energy systems has identified the supercritical CO2 (s-CO2) Brayton cycle in particular as a viable candidate for many proposed reactor types. The s-CO2 Brayton cycle can maintain superior thermal efficiency over a wide range of ambient temperatures, making these power systems ideally suited for dry air cooling, even in warm climates. For a sodium fast reactor (SFR) operating at 550 degrees C, thermal efficiency is calculated to be 43% with a 50 degrees C compressor inlet temperature. This is achieved by raising CO2 compressor inlet pressure in response to rising ambient temperatures. Preliminary design studies have shown that s-CO2 power cycle hardware will be compact and therefore well-matched to near-term and advanced integral small modular reactor (SMR) designs. These advantages also extend to the cooling plant, where it is estimated that dry cooling towers for an SFR-coupled s-CO2 power cycle will be similar in cost and scale to the evaporative cooling tower for a light-water reactor (LWR). The projected benefits of the s-CO2 power cycle coupled to dry air heat rejection may enable the long-awaited rise of next-generation nuclear energy systems, while redrawing the map for siting of small and large nuclear energy systems. C1 [Conboy, T. M.; Carlson, M. D.; Rochau, G. E.] Sandia Natl Labs, Adv Nucl Concepts, Albuquerque, NM 87185 USA. RP Conboy, TM (reprint author), Sandia Natl Labs, Adv Nucl Concepts, POB 5800,MS1136, Albuquerque, NM 87185 USA. EM tmc@creare.com FU U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX Sandia National Laboratories is a multiprogram laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy's National Nuclear Security Administration under Contract No. DE-AC04-94AL85000. NR 43 TC 0 Z9 0 U1 8 U2 20 PU ASME PI NEW YORK PA TWO PARK AVE, NEW YORK, NY 10016-5990 USA SN 0742-4795 EI 1528-8919 J9 J ENG GAS TURB POWER JI J. Eng. Gas. Turbines Power-Trans. ASME PD JAN PY 2015 VL 137 IS 1 AR 012901 DI 10.1115/1.4028080 PG 10 WC Engineering, Mechanical SC Engineering GA AZ2FP UT WOS:000348050300015 ER PT J AU Ling, M Zhao, H Xiao, XC Shi, FF Wu, MY Qiu, JX Li, S Song, XY Liu, G Zhang, SQ AF Ling, Min Zhao, Hui Xiao, Xingcheng Shi, Feifei Wu, Mingyan Qiu, Jingxia Li, Sheng Song, Xiangyun Liu, Gao Zhang, Shanqing TI Low cost and environmentally benign crack-blocking structures for long life and high power Si electrodes in lithium ion batteries SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID HIGH-CAPACITY; NEGATIVE ELECTRODES; DIFFUSION-COEFFICIENT; SECONDARY BATTERIES; GRAPHITE ELECTRODE; ENERGY-STORAGE; POLYMER BINDER; C COMPOSITE; ANODES; PERFORMANCE AB The high capacity Si (4200 mA h g(-1), Li4.4Si) commonly undergoes cracking and delamination due to drastic volume change (similar to 300%) during lithiation/delithiation processes in lithium ion batteries (LIBs). In this work, abundant and sustainable natural polymer gum arabic (GA) and low cost polyacrylic acid (PAA) are used to fabricate Si anodes with resilient, crack-blocking properties. The esterification reaction between GA and PAA establishes a flexible network resulting in reinforced mechanical strength and enhanced coherent strength. Meanwhile, the water vapour resulting from the esterification reaction generates micron-sized pores which relieves the stress and blocks the formation and propagation of cracks. As a result of the crack-blocking effect, the resultant Si anodes present a superior volumetric capacity of 2890 A h L-1. In addition, charge-discharge cycling for more than 1000 cycles is achieved with the Li insertion capacity limited to 1000 mA h g(-1) at a 1 C rate. C1 [Ling, Min; Qiu, Jingxia; Li, Sheng; Zhang, Shanqing] Griffith Univ, Ctr Clean Environm & Energy, Environm Futures Res Inst, Gold Coast Campus, Australia. [Ling, Min; Qiu, Jingxia; Li, Sheng; Zhang, Shanqing] Griffith Univ, Griffith Sch Environm, Gold Coast Campus, Australia. [Ling, Min; Zhao, Hui; Shi, Feifei; Wu, Mingyan; Song, Xiangyun; Liu, Gao] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. [Xiao, Xingcheng] GM Corp, Global R&D Ctr, Warren, MI 48090 USA. RP Ling, M (reprint author), Griffith Univ, Ctr Clean Environm & Energy, Environm Futures Res Inst, Gold Coast Campus, Australia. RI Li, Sheng/H-6569-2015; Foundry, Molecular/G-9968-2014; Zhang, Shanqing/C-2590-2008; OI Li, Sheng/0000-0003-1645-6865; Zhao, Huijun/0000-0002-3028-0459 FU Australia Research Council; Energy Efficiency, Office of Vehicle Technologies of the U.S. Department of Energy (U.S. DOE) [DE-AC02-05CH11231]; Batteries for Advanced Transportation Technologies (BATT) Program at Lawrence Berkeley National Laboratory FX This work is supported by the Australia Research Council and by the Assistant Secretary for Energy Efficiency, Office of Vehicle Technologies of the U.S. Department of Energy (U.S. DOE) under contract no. DE-AC02-05CH11231 and the Batteries for Advanced Transportation Technologies (BATT) Program at Lawrence Berkeley National Laboratory. NR 55 TC 6 Z9 6 U1 16 U2 73 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7488 EI 2050-7496 J9 J MATER CHEM A JI J. Mater. Chem. A PY 2015 VL 3 IS 5 BP 2036 EP 2042 DI 10.1039/c4ta05817h PG 7 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA AZ3SI UT WOS:000348146600037 ER PT J AU Lee, D Lee, YL Hong, WT Biegalski, MD Morgan, D Shao-Horn, Y AF Lee, Dongkyu Lee, Yueh-Lin Hong, Wesley T. Biegalski, Michael D. Morgan, Dane Shao-Horn, Yang TI Oxygen surface exchange kinetics and stability of (La,Sr)(2)CoO4 +/-delta/La1-xSrxMO3-delta (M = Co and Fe) hetero-interfaces at intermediate temperatures SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID OXIDE FUEL-CELLS; PEROVSKITE-RELATED OXIDES; DOUBLE-LAYER CATHODES; THIN-FILM ELECTRODES; REDUCTION KINETICS; LA1-XSRXMN1-YCOYO3+/-DELTA PEROVSKITES; ELECTRICAL-PROPERTIES; COMPOSITE CATHODE; TRACER DIFFUSION; CGO ELECTROLYTES AB Heterostructured oxide interfaces created by decorating Ruddlesden-Popper (RP) phases on ABO(3) perovskites have shown not only pronounced cation segregation at the interface and in the RP phase but also enhanced kinetics for oxygen electrocatalysis at elevated temperatures. In this study, combining experimental and theoretical approaches, we report and compare the time-dependent surface exchange kinetics and stability of (La0.5Sr0.5)(2)CoO4 +/-delta (LSC214)-decorated La0.6Sr0.4Co0.2Fe0.8O3-delta (LSCF113) and La0.8Sr0.2CoO3-delta (LSC113) thin films. While LSC214 decoration on LSC113 greatly reduced the degradation in the surface exchange kinetics as a function of time relative to undecorated LSC113, LSCF113 with LSC214 coverage showed comparable surface exchange kinetics and stability relative to undecorated LSCF113. This difference is attributed to stabilization of the LSC113 surface by LSC214 decoration and greater stability of LSCF113 against decomposition into secondary phases than LSC113. This hypothesis is supported by density functional theory (DFT) computation, revealing greater surface Sr segregation for LSCF113, which is predicted to have an SrO termination, than LSC113, which is predicted to have a less Sr enriched (La0.25Sr0.75)O termination. Furthermore, DFT also showed a lower energy gain to move Sr from LSCF113 into LSC214 relative to the LSC214-LSC113 surface, and predicted the stability of LSCF113, LSC113, and LSC214 with 100% Sr substitution in their top (001) surface. The stability differences of Sr substitution (with La) in LSCF113, LSC113, and LSC214, along with the assessed DFT decomposition free energies of fully Sr substituted LSCF113, LSC113, and LSC214, correlate with the experimental observation of surface stability trends in surface particle formation of LSCF113 and LSC113 without and with LSC214 decoration. C1 [Lee, Dongkyu; Lee, Yueh-Lin; Hong, Wesley T.; Shao-Horn, Yang] MIT, Electrochem Energy Lab, Cambridge, MA 02139 USA. [Lee, Dongkyu; Lee, Yueh-Lin; Shao-Horn, Yang] MIT, Dept Mech Engn, Cambridge, MA 02139 USA. [Hong, Wesley T.; Shao-Horn, Yang] MIT, Dept Mat Sci & Engn, Cambridge, MA 02139 USA. [Biegalski, Michael D.] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. [Morgan, Dane] Univ Wisconsin, Dept Mat Sci & Engn, Madison, WI 53706 USA. RP Shao-Horn, Y (reprint author), MIT, Dept Mat Sci & Engn, 77 Massachusetts Ave, Cambridge, MA 02139 USA. EM ddmorgan@wisc.edu; shaohorn@mit.edu RI LEE, YUEH-LIN/F-6274-2011 OI LEE, YUEH-LIN/0000-0003-2477-6412 FU Department of Energy (DOE); National Energy Technology Laboratory (NETL); Solid State Energy Conversion Alliance (SECA) Core Technology Program [DEFE0009435]; Skoltech-MIT Center for Electrochemical Energy; Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy; Center for Nanophase Materials Sciences at Oak Ridge National Laboratory [CNMS2013-292] FX This work was supported by the Department of Energy (DOE), the National Energy Technology Laboratory (NETL), the Solid State Energy Conversion Alliance (SECA) Core Technology Program (Funding Opportunity Number DEFE0009435) and the Skoltech-MIT Center for Electrochemical Energy. The PLD and XRD performed were conducted at the Center for Nanophase Materials Sciences, which is sponsored at Oak Ridge National Laboratory by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy, and computations in this work were also benefited from the use of the National Energy Research Scientific Computing Center allocation of the Center for Nanophase Materials Sciences at Oak Ridge National Laboratory, both under grant number CNMS2013-292. NR 78 TC 10 Z9 10 U1 12 U2 67 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7488 EI 2050-7496 J9 J MATER CHEM A JI J. Mater. Chem. A PY 2015 VL 3 IS 5 BP 2144 EP 2157 DI 10.1039/c4ta05795c PG 14 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA AZ3SI UT WOS:000348146600050 ER PT J AU Campbell, JM Ellis, RK AF Campbell, John M. Ellis, R. Keith TI Top-quark processes at NLO in production and decay SO JOURNAL OF PHYSICS G-NUCLEAR AND PARTICLE PHYSICS LA English DT Article DE top quark; collider physics; QCD ID QCD CORRECTIONS; HADRON COLLIDERS; WIDTH AB We describe the implementation of top production and decay processes in the parton-level Monte Carlo program MCFM. By treating the top quark as being on-shell, we can factorize the amplitudes for top-pair production, s-channel single-top production, and t-channel single-top production into the product of an amplitude for production and an amplitude for decay. In this way we can retain all spin correlations. Both the production and the decay amplitudes are calculated consistently at next-to-leading order in alpha(S). The full dependence on the b-quark mass is also kept. Phenomenological results are presented for various kinematic distributions at the LHC and for the top quark forward-backward asymmetry at the Tevatron. C1 [Campbell, John M.; Ellis, R. Keith] Fermilab Natl Accelerator Lab, Batavia, IL 60510 USA. RP Campbell, JM (reprint author), Fermilab Natl Accelerator Lab, Batavia, IL 60510 USA. EM ellis@fnal.gov FU US DOE [DE-AC02-06CH11357] FX We gratefully acknowledge useful conversations with Simon Badger and Markus Schulze. This research is supported by the US DOE under contract DE-AC02-06CH11357. NR 33 TC 16 Z9 16 U1 0 U2 2 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 0954-3899 EI 1361-6471 J9 J PHYS G NUCL PARTIC JI J. Phys. G-Nucl. Part. Phys. PD JAN PY 2015 VL 42 IS 1 AR 015005 DI 10.1088/0954-3899/42/1/015005 PG 38 WC Physics, Nuclear; Physics, Particles & Fields SC Physics GA AZ3LW UT WOS:000348130000006 ER PT J AU Tawfik, AN Magdy, N AF Tawfik, Abdel Nasser Magdy, Niseem TI Thermodynamics and higher order moments in SU(3) linear sigma-model with gluonic quasiparticles SO JOURNAL OF PHYSICS G-NUCLEAR AND PARTICLE PHYSICS LA English DT Article DE chiral lagrangian; quark confinement; quark-gluon plasma; quasiparticle model ID EQUATION-OF-STATE; QCD; FLUCTUATIONS; QUARKS AB In the framework of the linear sigma-model (LSM) with three quark flavors, the chiral phase diagram at finite temperature and density is investigated. For temperatures higher than the critical temperature (T-c), we added to the LSM the gluonic sector from the quasi-particle model (QPM), which assumes that the interacting gluons in the strongly interacting matter, the quark-gluon plasma (QGP), are phenomenologically the same as non-interacting massive quasi-particles. The dependence of the chiral condensates of strange and non-strange quarks on the temperature and chemical potential is analyzed. Then, we calculate the thermodynamics in the new approach (using a combination of the LSM and the QPM). Confronting the results with those from recent lattice quantum chromodynamics simulations reveals an excellent agreement for almost all thermodynamic quantities. The dependences of the first-order and second-order moments of the particle multiplicity on the chemical potential at fixed temperature are studied. These investigations are implemented through characterizing the large fluctuations accompanying the chiral phase transition. The results for the first-order and second-order moments are compared with those from the SU(3) Polyakov linear sigma-model (PLSM). Also, the resulting phase diagrams deduced in the PLSM and the LSM+QPM are compared with each other. C1 [Tawfik, Abdel Nasser] Modern Univ Technol & Informat MTI, Egyptian Ctr Theoret Phys, Cairo 11571, Egypt. [Tawfik, Abdel Nasser; Magdy, Niseem] World Lab Cosmol & Particle Phys WLCAPP, Cairo 11571, Egypt. [Magdy, Niseem] Brookhaven Natl Lab, Dept Phys, Upton, NY 11973 USA. RP Tawfik, AN (reprint author), Modern Univ Technol & Informat MTI, Egyptian Ctr Theoret Phys, Cairo 11571, Egypt. EM atawfik@rcf.rhic.bnl.gov RI Tawfik, Abdel Nasser/M-6220-2013 OI Tawfik, Abdel Nasser/0000-0002-1679-0225 FU World Laboratory for Cosmology and Particle Physics (WLCAPP) FX The present work was supported by the World Laboratory for Cosmology and Particle Physics (WLCAPP) http://wlcapp.net/. NR 37 TC 5 Z9 5 U1 0 U2 1 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 0954-3899 EI 1361-6471 J9 J PHYS G NUCL PARTIC JI J. Phys. G-Nucl. Part. Phys. PD JAN PY 2015 VL 42 IS 1 AR 015004 DI 10.1088/0954-3899/42/1/015004 PG 21 WC Physics, Nuclear; Physics, Particles & Fields SC Physics GA AZ3LW UT WOS:000348130000005 ER PT J AU Xiong, WL Giannone, RJ Morowitz, MJ Banfield, JF Hettich, RL AF Xiong, Weili Giannone, Richard J. Morowitz, Michael J. Banfield, Jillian F. Hettich, Robert L. TI Development of an Enhanced Metaproteomic Approach for Deepening the Microbiome Characterization of the Human Infant Gut SO JOURNAL OF PROTEOME RESEARCH LA English DT Article DE Metaproteome; human infant gut; shotgun proteomics; double filtering ID PEPTIDE-IDENTIFICATION; QUANTITATIVE PROTEOMICS; MASS-SPECTROMETRY; LABEL-FREE; HEALTH; IMPACT; COLONIZATION; PATHOGENESIS; COMMUNITIES; COOPERATE AB The establishment of early life microbiota in the human infant gut is highly variable and plays a crucial role in host nutrient availability/uptake and maturation of immunity. Although high-performance mass spectrometry (MS)-based metaproteomics is a powerful method for the functional characterization of complex microbial communities, the acquisition of comprehensive metaproteomic information in human fecal samples is inhibited by the presence of abundant human proteins. To alleviate this restriction, we have designed a novel metaproteomic strategy based on double filtering (DF) the raw samples, a method that fractionates microbial from human cells to enhance microbial protein identification and characterization in complex fecal samples from healthy premature infants. This method dramatically improved the overall depth of infant gut proteome measurement, with an increase in the number of identified low-abundance proteins and a greater than 2-fold improvement in microbial protein identification and quantification. This enhancement of proteome measurement depth enabled a more extensive microbiome comparison between infants by not only increasing the confidence of identified microbial functional categories but also revealing previously undetected categories. C1 [Xiong, Weili; Giannone, Richard J.; Hettich, Robert L.] Oak Ridge Natl Lab, Chem Sci Div, Oak Ridge, TN 37831 USA. [Xiong, Weili] Univ Tennessee, Grad Sch Genome Sci & Technol, Knoxville, TN 37996 USA. [Morowitz, Michael J.] Univ Pittsburgh, Sch Med, Pittsburgh, PA 15261 USA. [Banfield, Jillian F.] Univ Calif Berkeley, Dept Earth & Planetary Sci, Berkeley, CA 94720 USA. RP Hettich, RL (reprint author), Oak Ridge Natl Lab, Chem Sci Div, Oak Ridge, TN 37831 USA. EM hettichrl@ornl.gov RI Hettich, Robert/N-1458-2016; Xiong, Weili/N-5069-2016 OI Hettich, Robert/0000-0001-7708-786X; Xiong, Weili/0000-0001-7208-917X FU University of Tennessee-Knoxville Genome Science and Technology Program; NIH [1R01-GM-103600] FX We thank Paul Abraham for technical advice and manuscript review. Stipend support for W.X. was provided by the University of Tennessee-Knoxville Genome Science and Technology Program. Research support for the technical project was provided by NIH grant 1R01-GM-103600. Oak Ridge National Laboratory is managed by UT-Battelle, LLC, for the U.S. Department of Energy. NR 32 TC 16 Z9 16 U1 1 U2 16 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 1535-3893 EI 1535-3907 J9 J PROTEOME RES JI J. Proteome Res. PD JAN PY 2015 VL 14 IS 1 BP 133 EP 141 DI 10.1021/pr500936p PG 9 WC Biochemical Research Methods SC Biochemistry & Molecular Biology GA AY3UA UT WOS:000347506600012 PM 25350865 ER PT J AU Xu, Z Wu, CC Xie, F Slysz, GW Tolic, N Monroe, ME Petyuk, VA Payne, SH Fujimoto, GM Moore, RJ Fillmore, TL Schepmoes, AA Levine, DA Townsend, RR Davies, SR Li, SQ Ellis, M Boja, E Rivers, R Rodriguez, H Rodland, KD Liu, T Smith, RD AF Xu, Zhe Wu, Chaochao Xie, Fang Slysz, Gordon W. Tolic, Nikola Monroe, Matthew E. Petyuk, Vladislav A. Payne, Samuel H. Fujimoto, Grant M. Moore, Ronald J. Fillmore, Thomas L. Schepmoes, Athena A. Levine, Douglas A. Townsend, R. Reid Davies, Sherri R. Li, Shunqiang Ellis, Matthew Boja, Emily Rivers, Robert Rodriguez, Henry Rodland, Karin D. Liu, Tao Smith, Richard D. TI Comprehensive Quantitative Analysis of Ovarian and Breast Cancer Tumor Peptidomes SO JOURNAL OF PROTEOME RESEARCH LA English DT Article DE protein degradation; peptidomics; proteases; tumor; ovarian cancer; breast cancer; ischemia ID MOLECULAR-WEIGHT PROTEOME; MASS-SPECTROMETRY; INTRACELLULAR PEPTIDES; CONTROLLED PROTEOLYSIS; SOFTWARE PACKAGE; ACCURATE MASS; PROTEASOME; SERUM; METHIONINE; IDENTIFICATION AB Aberrant degradation of proteins is associated with many pathological states, including cancers. Mass spectrometric analysis of tumor peptidomes, the intracellular and intercellular products of protein degradation, has the potential to provide biological insights on proteolytic processing in cancer. However, attempts to use the information on these smaller protein degradation products from tumors for biomarker discovery and cancer biology studies have been fairly limited to date, largely due to the lack of effective approaches for robust peptidomics identification and quantification and the prevalence of confounding factors and biases associated with sample handling and processing. Herein, we have developed an effective and robust analytical platform for comprehensive analyses of tissue peptidomes, which is suitable for high-throughput quantitative studies. The reproducibility and coverage of the platform, as well as the suitability of clinical ovarian tumor and patient-derived breast tumor xenograft samples with postexcision delay of up to 60 min before freezing for peptidomics analysis, have been demonstrated. Moreover, our data also show that the peptidomics profiles can effectively separate breast cancer subtypes, reflecting tumor-associated protease activities. Peptidomics complements results obtainable from conventional bottom-up proteomics and provides insights not readily obtainable from such approaches. C1 [Xu, Zhe; Wu, Chaochao; Xie, Fang; Slysz, Gordon W.; Monroe, Matthew E.; Petyuk, Vladislav A.; Payne, Samuel H.; Fujimoto, Grant M.; Moore, Ronald J.; Schepmoes, Athena A.; Rodland, Karin D.; Liu, Tao; Smith, Richard D.] Pacific NW Natl Lab, Div Biol Sci, Richland, WA 99354 USA. [Tolic, Nikola; Fillmore, Thomas L.] Pacific NW Natl Lab, Environm Mol Sci Lab, Richland, WA 99354 USA. [Levine, Douglas A.] Mem Sloan Kettering Canc Ctr, Dept Surg, Gynecol Serv, New York, NY 10065 USA. [Townsend, R. Reid; Davies, Sherri R.; Li, Shunqiang; Ellis, Matthew] Washington Univ, Dept Med, St Louis, MO 63130 USA. [Boja, Emily; Rivers, Robert; Rodriguez, Henry] NCI, Off Canc Clin Prote Res, NIH, Bethesda, MD 20892 USA. RP Liu, T (reprint author), Pacific NW Natl Lab, Div Biol Sci, Richland, WA 99354 USA. EM tao.liu@pnnl.gov; dick.smith@pnnl.gov RI Smith, Richard/J-3664-2012; OI Smith, Richard/0000-0002-2381-2349; Petyuk, Vladislav/0000-0003-4076-151X; Payne, Samuel/0000-0002-8351-1994 FU National Cancer Institute Clinical Proteomic Tumor Analysis Consortium (CPTAC), National Institutes of Health [U24CA160019, P41GM103493]; Department of Defense Interagency [MIPR2DO89M2058]; Department of Energy (DOE) Early Career Award; DOE [DE-AC05-76RL0 1830] FX Portions of this work were supported by Grant U24CA160019, from the National Cancer Institute Clinical Proteomic Tumor Analysis Consortium (CPTAC), National Institutes of Health Grant P41GM103493, Department of Defense Interagency Agreement MIPR2DO89M2058, and Department of Energy (DOE) Early Career Award (to S.H.P.). The experimental work described herein was performed in the Environmental Molecular Sciences Laboratory, a national scientific user facility sponsored by the DOE and located at Pacific Northwest National Laboratory, which is operated by Battelle Memorial Institute for the DOE under Contract DE-AC05-76RL0 1830. NR 52 TC 9 Z9 10 U1 1 U2 15 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 1535-3893 EI 1535-3907 J9 J PROTEOME RES JI J. Proteome Res. PD JAN PY 2015 VL 14 IS 1 BP 422 EP 433 DI 10.1021/pr500840w PG 12 WC Biochemical Research Methods SC Biochemistry & Molecular Biology GA AY3UA UT WOS:000347506600036 PM 25350482 ER PT J AU Bryan, AL Love, CN Mills, GL Borkhatada, RR Lance, SL AF Bryan, A. Lawrence, Jr. Love, Cara N. Mills, Gary L. Borkhatada, Rena R. Lance, Stacey L. TI Testing for Associations between Hematozoa Infection and Mercury in Wading Bird Nestlings SO JOURNAL OF WILDLIFE DISEASES LA English DT Article DE Avian malaria; Haemoproteus; Hg; mercury; nestling wading birds; Plasmodium ID SOUTHEASTERN UNITED-STATES; STORKS MYCTERIA-AMERICANA; WOOD STORKS; BLOOD PARASITES; GEORGIA AB Several wading bird species in the southeastern US have a history of infection by hematozoa/avian malaria as well as mercury accumulation through their diet, and thus may be exposed to two, generally sublethal, yet chronic, stressors. We analyzed nestling wading birds (n=171) of varying size and trophic position from the southeastern US, and a smaller sample (n=23) of older, free-ranging birds, to look for potential interrelationships between infection by hematozoa and mercury (Hg) uptake. Only one nestling was PCR positive for hematozoa (Plasmodium/Haemoproteus) whereas nine (39%) of the older wading birds were positive. Sequencing indicated that both nestling and adult positives were infected with Plasmodium. Given the low infection rate of the nestlings, there was no association between Hg and malaria. The older birds exhibited a possible malaria/Hg association, but it may be confounded by their greater potential exposure period and large-scale movements. C1 [Bryan, A. Lawrence, Jr.; Love, Cara N.; Mills, Gary L.; Lance, Stacey L.] Univ Georgia, Savannah River Ecol Lab, Aiken, SC 29802 USA. [Borkhatada, Rena R.] Univ Florida, Everglades Res & Educ Ctr, Belle Glade, FL 33430 USA. RP Bryan, AL (reprint author), Univ Georgia, Savannah River Ecol Lab, PO Drawer E, Aiken, SC 29802 USA. EM lbryan@srel.uga.edu RI Lance, Stacey/K-9203-2013 OI Lance, Stacey/0000-0003-2686-1733 FU US Fish and Wildlife Service Avian Health and Disease Monitoring Program; US Department of Energy [DE-FC09-96SR18546] FX We thank the Georgia DNR (Tim Keyes) and South Carolina DNR (Christy Hand) for assisting with landowner contacts and tissue collecting. Donna Bear provided tissues from the Jacksonville Zoo. Mary Beth Morrison (Palm Beach Solid Waste Authority) and Paul Schoenfeld (Kings Bay Submarine Base) and several private landowners gave us permission to access the wading bird colonies on their properties. Susan Perkins provided helpful discussions and assistance with genus identification. Angela Lindell (Savannah River Ecology Laboratory) assisted with all Hg analyses. This project was funded by the US Fish and Wildlife Service Avian Health and Disease Monitoring Program and received additional support from the US Department of Energy, through Financial Assistance Award DE-FC09-96SR18546 to the University of Georgia Research Foundation. NR 19 TC 0 Z9 0 U1 1 U2 13 PU WILDLIFE DISEASE ASSOC, INC PI LAWRENCE PA 810 EAST 10TH ST, LAWRENCE, KS 66044-8897 USA SN 0090-3558 EI 1943-3700 J9 J WILDLIFE DIS JI J. Wildl. Dis. PD JAN PY 2015 VL 51 IS 1 BP 222 EP 226 DI 10.7589/2013-12-332 PG 5 WC Veterinary Sciences SC Veterinary Sciences GA AZ1LS UT WOS:000348001200024 PM 25375937 ER PT J AU You, Y Yu, XQ Yin, YX Nam, KW Guo, YG AF You, Ya Yu, Xiqian Yin, Yaxia Nam, Kyung-Wan Guo, Yu-Guo TI Sodium iron hexacyanoferrate with high Na content as a Na-rich cathode material for Na-ion batteries SO NANO RESEARCH LA English DT Article DE sodium iron hexacyanoferrate; Na-rich cathode; sodium-ion batteries; Prussian blue analogues ID LONG CYCLE LIFE; PRUSSIAN BLUE ANALOGS; ENERGY-STORAGE; LOW-COST; INTERCALATION CHEMISTRY; ELECTRODE MATERIALS; HOLLOW NANOSPHERES; LITHIUM STORAGE; PERFORMANCE; FRAMEWORK AB Owing to the worldwide abundance and low-cost of Na, room-temperature Na-ion batteries are emerging as attractive energy storage systems for large-scale grids. Increasing the Na content in cathode materials is one of the effective ways to achieve high energy density. Prussian blue and its analogues (PBAs) are promising Na-rich cathode materials since they can theoretically store two Na+ ions per formula unit. However, increasing the Na content in PBAs cathode materials remains a major challenge. Here we show that sodium iron hexacyanoferrate with high Na content can be obtained by simply controlling the reducing agent and reaction atmosphere during synthesis. The Na content can reach as high as 1.63 per formula, which is the highest value for sodium iron hexacyanoferrate. This Na-rich sodium iron hexacyanoferrate demonstrates a high specific capacity of 150 mAh center dot g(-1) and remarkable cycling performance with 90% capacity retention after 200 cycles. Furthermore, the Na intercalation/de-intercalation mechanism has been systematically studied by in situ Raman spectroscopy, X-ray diffraction and X-ray absorption spectroscopy analysis for the first time. The Na-rich sodium iron hexacyanoferrate can function as a plenteous Na reservoir and has great potential as a cathode material for practical Na-ion batteries. C1 [You, Ya; Yin, Yaxia; Guo, Yu-Guo] Chinese Acad Sci, CAS Key Lab Mol Nanostruct & Nanotechnol, Beijing 100190, Peoples R China. [You, Ya; Yin, Yaxia; Guo, Yu-Guo] Chinese Acad Sci, Inst Chem, Beijing Natl Lab Mol Sci, Beijing 100190, Peoples R China. [Yu, Xiqian] Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA. [Nam, Kyung-Wan] Dongguk Univ, Dept Energy & Mat Engn, Seoul 100715, South Korea. RP Nam, KW (reprint author), Dongguk Univ, Dept Energy & Mat Engn, Seoul 100715, South Korea. EM knam@dongguk.edu; ygguo@iccas.ac.cn RI Guo, Yu-Guo/A-1223-2009; You, Ya/F-1270-2015; Nam, Kyung-Wan/E-9063-2015; Yu, Xiqian/B-5574-2014 OI Guo, Yu-Guo/0000-0003-0322-8476; Nam, Kyung-Wan/0000-0001-6278-6369; Yu, Xiqian/0000-0001-8513-518X FU National Natural Science Foundation of China [51225204, 91127044, 21121063]; National Basic Research Program of China [2012CB932900, 2011CB935700]; U.S. Department of Energy, the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies [DE-AC02-98CH10886] FX This work was supported by the National Natural Science Foundation of China (Nos. 51225204, 91127044 and 21121063), the National Basic Research Program of China (Nos. 2012CB932900 and 2011CB935700). The work at BNL was supported by the U.S. Department of Energy, the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies (No. DE-AC02-98CH10886). The authors acknowledge the technical support from beamline scientists at X14A, X18A and X19A (NSLS, BNL). NR 60 TC 44 Z9 44 U1 41 U2 185 PU TSINGHUA UNIV PRESS PI BEIJING PA TSINGHUA UNIV, RM A703, XUEYAN BLDG, BEIJING, 10084, PEOPLES R CHINA SN 1998-0124 EI 1998-0000 J9 NANO RES JI Nano Res. PD JAN PY 2015 VL 8 IS 1 BP 117 EP 128 DI 10.1007/s12274-014-0588-7 PG 12 WC Chemistry, Physical; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA AZ4NX UT WOS:000348200300008 ER PT J AU Yang, Y Fu, Q Wei, MM Bluhm, H Bao, XH AF Yang, Yang Fu, Qiang Wei, Mingming Bluhm, Hendrik Bao, Xinhe TI Stability of BN/metal interfaces in gaseous atmosphere SO NANO RESEARCH LA English DT Article DE h-BN; graphene; intercalation; Ru(0001); PEEM; AP-XPS ID HEXAGONAL BORON-NITRIDE; CHEMICAL-VAPOR-DEPOSITION; UNDERNEATH GRAPHENE; EPITAXIAL GRAPHENE; LARGE-AREA; GROWTH; RU(0001); INTERCALATION; NANOMESH; ADSORPTION AB Hexagonal boron nitride (h-BN) is often prepared by epitaxial growth on metals, and stability of the formed BN/metal interfaces in gaseous environment is a key issue for physicochemical properties of the BN overlayers. As an illustration here, the structural change of a BN/Ru(0001) interface upon exposure to O-2 has been investigated using in situ photoemission electron microscopy (PEEM) and ambient pressure X-ray photoelectron spectroscopy (AP-XPS). We demonstrate the occurrence of oxygen intercalation of the BN overlayers in O-2 atmosphere, which decouples the BN overlayer from the substrate. Comparative studies of oxygen intercalation at BN/Ru(0001) and graphene/Ru(0001) surfaces indicate that the oxygen intercalation of BN overlayers happens more easily than graphene. This finding will be of importance for future applications of BN-based devices and materials under ambient conditions. C1 [Yang, Yang; Fu, Qiang; Wei, Mingming; Bao, Xinhe] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China. [Bluhm, Hendrik] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. RP Fu, Q (reprint author), Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China. EM qfu@dicp.ac.cn; xhbao@dicp.ac.cn RI li, haobo/P-5373-2014; Fu, Qiang/E-7109-2015 OI li, haobo/0000-0002-9215-3754; Fu, Qiang/0000-0001-5316-6758 FU National Natural Science Foundation of China [21222305, 21373208, 21033009]; Ministry of Science and Technology of China [2011CB932704, 2013CB834603]; Chinese Academy of Sciences; Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences and Materials Sciences Division of the US Department of Energy at the Lawrence Berkeley National Laboratory [DE-AC02-05CH11231] FX This work was financially supported by the National Natural Science Foundation of China (Nos. 21222305, 21373208, and 21033009), Ministry of Science and Technology of China (Nos. 2011CB932704 and 2013CB834603), and the Key Research Program of the Chinese Academy of Sciences. The ALS and the MES beamline 11.0.2 are supported by the Director, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences and Materials Sciences Division of the US Department of Energy at the Lawrence Berkeley National Laboratory under Contract No. DE-AC02-05CH11231. NR 46 TC 14 Z9 14 U1 15 U2 86 PU TSINGHUA UNIV PRESS PI BEIJING PA TSINGHUA UNIV, RM A703, XUEYAN BLDG, BEIJING, 10084, PEOPLES R CHINA SN 1998-0124 EI 1998-0000 J9 NANO RES JI Nano Res. PD JAN PY 2015 VL 8 IS 1 BP 227 EP 237 DI 10.1007/s12274-014-0639-0 PG 11 WC Chemistry, Physical; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA AZ4NX UT WOS:000348200300018 ER PT J AU Zhang, LM Liu, C Wong, AB Resasco, J Yang, PD AF Zhang, Liming Liu, Chong Wong, Andrew Barnabas Resasco, Joaquin Yang, Peidong TI MoS2-wrapped silicon nanowires for photoelectrochemical water reduction SO NANO RESEARCH LA English DT Article DE MoS2; Si nanowire array; coaxial heterostructure; photoelectrochemistry; hydrogen evolution reaction (HER) ID HYDROGEN EVOLUTION REACTION; ACTIVE EDGE SITES; SULFIDE CATALYST; H-2 EVOLUTION; MOS2; LAYER; ELECTROCATALYSTS; PHOTOCATHODE; GENERATION; NANOSHEETS AB Integration of molybdenum disulfide (MoS2) onto high surface area photocathodes is highly desired to minimize the overpotential for the solar-powered hydrogen evolution reaction (HER). Semiconductor nanowires (NWs) are beneficial for use in photoelectrochemistry because of their large electrochemically available surface area and inherent ability to decouple light absorption and the transport of minority carriers. Here, silicon (Si) NW arrays were employed as a model photocathode system for MoS2 wrapping, and their solar-driven HER activity was evaluated. The photocathode is made up of a well-defined MoS2/TiO2/Si coaxial NW heterostructure, which yielded photocurrent density up to 15 mA/cm(2) (at 0 V vs. the reversible hydrogen electrode (RHE)) with good stability under the operating conditions employed. This work reveals that earth-abundant electrocatalysts coupled with high surface area NW electrodes can provide performance comparable to noble metal catalysts for photocathodic hydrogen evolution. C1 [Zhang, Liming; Liu, Chong; Wong, Andrew Barnabas; Yang, Peidong] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Resasco, Joaquin] Univ Calif Berkeley, Dept Chem Engn, Berkeley, CA 94720 USA. [Yang, Peidong] Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA. [Wong, Andrew Barnabas; Yang, Peidong] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. RP Yang, PD (reprint author), Stanford Univ, Dept Mat Sci & Engn, Stanford, CA 94305 USA. EM p_yang@berkeley.edu OI Liu, Chong/0000-0001-5546-3852 FU Office of Science, Office of Basic Energy Sciences, Materials Science and Engineering Division, U.S. Department of Energy [DE-AC02-05CH11231]; National Science Foundation Graduate Research Fellowship Program (NSF GRFP) [DGE-0802270] FX This work was supported by the Director, Office of Science, Office of Basic Energy Sciences, Materials Science and Engineering Division, U.S. Department of Energy under Contract No. DE-AC02-05CH11231 (P-Chem). J.R. gratefully acknowledges the support of the National Science Foundation Graduate Research Fellowship Program (NSF GRFP) under Grant No. DGE-0802270. NR 34 TC 14 Z9 14 U1 25 U2 157 PU TSINGHUA UNIV PRESS PI BEIJING PA TSINGHUA UNIV, RM A703, XUEYAN BLDG, BEIJING, 10084, PEOPLES R CHINA SN 1998-0124 EI 1998-0000 J9 NANO RES JI Nano Res. PD JAN PY 2015 VL 8 IS 1 BP 281 EP 287 DI 10.1007/s12274-014-0673-y PG 7 WC Chemistry, Physical; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA AZ4NX UT WOS:000348200300024 ER PT J AU Park, J Mitchel, WC Elhamri, S Grazulis, L Hoelscher, J Mahalingam, K Hwang, C Mo, SK Lee, J AF Park, Jeongho Mitchel, William C. Elhamri, Said Grazulis, Lawrence Hoelscher, John Mahalingam, Krishnamurthy Hwang, Choongyu Mo, Sung-Kwan Lee, Jonghoon TI Observation of the intrinsic bandgap behaviour in as-grown epitaxial twisted graphene SO NATURE COMMUNICATIONS LA English DT Article ID SCANNING-TUNNELING-MICROSCOPY; MULTIWALLED CARBON NANOTUBES; BILAYER GRAPHENE; SUPERLATTICES; GRAPHITE; ENERGIES AB Twisted graphene is of particular interest due to several intriguing characteristics, such as its the Fermi velocity, van Hove singularities and electronic localization. Theoretical studies recently suggested the possible bandgap opening and tuning. Here, we report a novel approach to producing epitaxial twisted graphene on SiC (0001) and the observation of its intrinsic bandgap behaviour. The direct deposition of C-60 on pre-grown graphene layers results in few-layer twisted graphene confirmed by angular resolved photoemission spectroscopy and Raman analysis. The strong enhanced G band in Raman and sp(3) bonding characteristic in X-ray photoemission spectroscopy suggests the existence of interlayer interaction between adjacent graphene layers. The interlayer spacing between graphene layers measured by transmission electron microscopy is 0.352 +/- 0.012 nm. Thermal activation behaviour and nonlinear current-voltage characteristics conclude that an intrinsic bandgap is opened in twisted graphene. Low sheet resistance (similar to 160 Omega square(-1) at 10 K) and high mobility (similar to 2,000 cm(2)V(-1) s(-1) at 10 K) are observed. C1 [Park, Jeongho; Mitchel, William C.; Grazulis, Lawrence; Hoelscher, John; Mahalingam, Krishnamurthy; Lee, Jonghoon] Mat & Mfg Directorate AFRL RXAN Wright Patters AF, Air Force Res Lab, Wright Patterson AFB, OH 45433 USA. [Elhamri, Said] Univ Dayton, Dept Phys, Dayton, OH 45469 USA. [Hwang, Choongyu] Pusan Natl Univ, Dept Phys, Pusan 609735, South Korea. [Mo, Sung-Kwan] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. RP Park, J (reprint author), Mat & Mfg Directorate AFRL RXAN Wright Patters AF, Air Force Res Lab, Wright Patterson AFB, OH 45433 USA. EM jeongho.park.1.ctr@us.af.mil RI Mo, Sung-Kwan/F-3489-2013 OI Mo, Sung-Kwan/0000-0003-0711-8514 FU Air Force office of Scientific Research; Max Planck Korea/POSTECH Research Initiative of the National Research Foundation (NRF) - Ministry of Science, ICT and Future Planning [NRF-2011-0031558] FX This work was supported by the Air Force office of Scientific Research (Dr Harold Weinstock). The authors thank Mr G. Landis, Mr T. Asel and Dr Elizabeth Moore for technical assistance and helpful discussion. C.H. acknowledges financial support from Max Planck Korea/POSTECH Research Initiative of the National Research Foundation (NRF) funded by the Ministry of Science, ICT and Future Planning under Project No. NRF-2011-0031558. NR 35 TC 10 Z9 10 U1 5 U2 55 PU NATURE PUBLISHING GROUP PI LONDON PA MACMILLAN BUILDING, 4 CRINAN ST, LONDON N1 9XW, ENGLAND SN 2041-1723 J9 NAT COMMUN JI Nat. Commun. PD JAN PY 2015 VL 6 AR 5677 DI 10.1038/ncomms6677 PG 8 WC Multidisciplinary Sciences SC Science & Technology - Other Topics GA CA1AJ UT WOS:000348644500001 PM 25562285 ER PT J AU Mudiyanselage, K Xu, F Hoffmann, FM Hrbek, J Waluyo, I Boscoboinik, JA Stacchiola, DJ AF Mudiyanselage, K. Xu, F. Hoffmann, F. M. Hrbek, J. Waluyo, I. Boscoboinik, J. A. Stacchiola, D. J. TI Adsorbate-driven morphological changes on Cu(111) nano-pits SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID GAS SHIFT REACTION; SCANNING-TUNNELING-MICROSCOPY; CARBON-MONOXIDE; ION-BOMBARDMENT; TEMPERATURE-DEPENDENCE; METHANOL SYNTHESIS; SPUTTERING DAMAGE; METAL-OXIDE; IN-SITU; SURFACE AB Adsorbate-driven morphological changes of pitted-Cu(111) surfaces have been investigated following the adsorption and desorption of CO and H. The morphology of the pitted-Cu(111) surfaces, prepared by Ar+ sputtering, exposed a few atomic layers deep nested hexagonal pits of diameters from 8 to 38 nm with steep step bundles. The roughness of pitted-Cu(111) surfaces can be healed by heating to 450-500 K in vacuum. Adsorption of CO on the pitted-Cu(111) surface leads to two infrared peaks at 2089-2090 and 2101-2105 cm(-1) for CO adsorbed on under-coordinated sites in addition to the peak at 2071 cm(-1) for CO adsorbed on atop sites of the close-packed Cu(111) surface. CO adsorbed on under-coordinated sites is thermally more stable than that of atop Cu(111) sites. Annealing of the CO-covered surface from 100 to 300 K leads to minor changes of the surface morphology. In contrast, annealing of a H covered surface to 300 K creates a smooth Cu(111) surface as deduced from infrared data of adsorbed CO and scanning tunnelling microscopy (STM) imaging. The observation of significant adsorbate-driven morphological changes with H is attributed to its stronger modification of the Cu(111) surface by the formation of a sub-surface hydride with a hexagonal structure, which relaxes into the healed Cu(111) surface upon hydrogen desorption. These morphological changes occur similar to 150 K below the temperature required for healing of the pitted-Cu(111) surface by annealing in vacuum. In contrast, the adsorption of CO, which only interacts with the top-most Cu layer and desorbs by 200 K, does not significantly change the morphology of the pitted-Cu(111) surface. C1 [Mudiyanselage, K.; Xu, F.; Hrbek, J.; Waluyo, I.; Stacchiola, D. J.] Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA. [Mudiyanselage, K.; Hoffmann, F. M.] CUNY, BMCC, Dept Sci, New York, NY 10007 USA. [Xu, F.] SUNY Stony Brook, Dept Chem, Stony Brook, NY 11794 USA. [Boscoboinik, J. A.] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. RP Stacchiola, DJ (reprint author), Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA. EM djs@bnl.gov RI Stacchiola, Dario/B-1918-2009; Boscoboinik, Jorge/E-8110-2010; Mudiyanselage, Kumudu/B-2277-2013; OI Stacchiola, Dario/0000-0001-5494-3205; Boscoboinik, Jorge/0000-0002-5090-7079; Mudiyanselage, Kumudu/0000-0002-3539-632X; Xu, Fang/0000-0002-8166-0275 FU U.S. Department of Energy, Office of Science [AC02-98CH10886]; Division of Chemical Sciences, Geosciences, and Biosciences within the Office of Basic Energy Sciences FX This work was carried out at the Chemistry Department, Center for Functional Nanomaterials and National Synchrotron Light Source, Brookhaven National Laboratory, under Contract No. DE-AC02-98CH10886 with the U.S. Department of Energy, Office of Science, and supported by its Division of Chemical Sciences, Geosciences, and Biosciences within the Office of Basic Energy Sciences. NR 46 TC 2 Z9 2 U1 6 U2 35 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2015 VL 17 IS 5 BP 3032 EP 3038 DI 10.1039/c4cp05088f PG 7 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AZ4OW UT WOS:000348203200014 PM 25510404 ER PT J AU Zhang, J Zhou, B Sun, ZR Wang, XB AF Zhang, Jian Zhou, Bin Sun, Zhen-Rong Wang, Xue-Bin TI Photoelectron spectroscopy and theoretical studies of anion-pi interactions: binding strength and anion specificity SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID DENSITY FUNCTIONALS; MOLECULAR-INTERACTIONS; HALIDE RECOGNITION; ELECTRON-TRANSFER; CHARGE-TRANSFER; HALOGEN BONDS; HYDROGEN-BOND; AB-INITIO; COMPLEXES; RECEPTORS AB Proposed in theory and then their existence confirmed, anion-pi interactions have been recognized as new and important non-covalent binding forces. Despite extensive theoretical studies, numerous crystal structural identifications, and a plethora of solution phase investigations, anion-pi interaction strengths that are free from complications of condensed-phase environments have not been directly measured in the gas phase. Herein we present a joint photoelectron spectroscopic and theoretical study on this subject, in which tetraoxacalix[2]arene[2] triazine 1, an electron-deficient and cavity self-tunable macrocyclic, was used as a charge-neutral molecular host to probe its interactions with a series of anions with distinctly different shapes and charge states (spherical halides Cl-, Br-, I-, linear thiocyanate SCN-, trigonal planar nitrate NO3-, pyramidic iodate IO3-, and tetrahedral sulfate SO42-). The binding energies of the resultant gaseous 1 : 1 complexes (1.Cl-, 1.Br-, 1.I-, 1.SCN-, 1.NO3-, 1.IO3- and 1.SO42-) were directly measured experimentally, exhibiting substantial non-covalent interactions with pronounced anion-specific effects. The binding strengths of Cl-, NO3-, IO3- with 1 are found to be strongest among all singly charged anions, amounting to ca. 30 kcal mol(-1), but only about 40% of that between 1 and SO42-. Quantum chemical calculations reveal that all the anions reside in the center of the cavity of 1 with an anion-pi binding motif in the complexes' optimized structures, where 1 is seen to be able to self-regulate its cavity structure to accommodate anions of different geometries and three-dimensional shapes. Electron density surface and charge distribution analyses further support anion-pi binding formation. The calculated binding energies of the anions and 1 nicely reproduce the experimentally estimated electron binding energy increase. This work illustrates that size-selective photoelectron spectroscopy combined with theoretical calculations represents a powerful technique to probe anion-pi interactions and has potential to provide quantitative guest-host molecular binding strengths and unravel fundamental insights in specific anion recognitions. C1 [Zhang, Jian; Zhou, Bin; Sun, Zhen-Rong] E China Normal Univ, State Key Lab Precis Spect, Shanghai 200062, Peoples R China. [Zhang, Jian; Wang, Xue-Bin] Pacific NW Natl Lab, Div Phys Sci, Richland, WA 99352 USA. RP Sun, ZR (reprint author), E China Normal Univ, State Key Lab Precis Spect, Shanghai 200062, Peoples R China. EM zrsun@phy.ecnu.edu.cn; xuebin.wang@pnnl.gov FU U. S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences Biosciences; DOE's Office of Biological and Environmental Research; National Natural Science Foundation of China [11474096] FX We thank Prof. Mei-Xiang Wang (Tsinghua University) and Prof. Haibo Yang (East China Normal University) for providing us the tetraoxacalix[2]arene[2] triazine sample. The NIPES research at PNNL was supported by the U. S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences & Biosciences (X.-B.W.), and was performed at EMSL, a national scientific user facility sponsored by DOE's Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory. The theoretical study performed at ECNU was supported by the National Natural Science Foundation of China (No. 11474096). NR 81 TC 5 Z9 5 U1 1 U2 22 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2015 VL 17 IS 5 BP 3131 EP 3141 DI 10.1039/c4cp04687k PG 11 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AZ4OW UT WOS:000348203200022 PM 25515705 ER PT J AU Islam, MM Ostadhossein, A Borodin, O Yeates, AT Tipton, WW Hennig, RG Kumar, N van Duin, ACT AF Islam, Md Mahbubul Ostadhossein, Alireza Borodin, Oleg Yeates, A. Todd Tipton, William W. Hennig, Richard G. Kumar, Nitin van Duin, Adri C. T. TI ReaxFF molecular dynamics simulations on lithiated sulfur cathode materials SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID REACTIVE FORCE-FIELD; RECHARGEABLE LITHIUM BATTERIES; HIGH SPECIFIC ENERGY; LI-S BATTERIES; SOLID-ELECTROLYTE; ION BATTERIES; AB-INITIO; ENCAPSULATED SULFUR; SILICON ELECTRODES; LIQUID ELECTROLYTE AB Sulfur is a very promising cathode material for rechargeable energy storage devices. However, sulfur cathodes undergo a noticeable volume variation upon cycling, which induces mechanical stress. In spite of intensive investigation of the electrochemical behavior of the lithiated sulfur compounds, their mechanical properties are not very well understood. In order to fill this gap, we developed a ReaxFF interatomic potential to describe Li-S interactions and performed molecular dynamics (MD) simulations to study the structural, mechanical, and kinetic behavior of the amorphous lithiated sulfur (a-LixS) compounds. We examined the effect of lithiation on material properties such as ultimate strength, yield strength, and Young's modulus. Our results suggest that with increasing lithium content, the strength of lithiated sulfur compounds improves, although this increment is not linear with lithiation. The diffusion coefficients of both lithium and sulfur were computed for the a-LixS system at various stages of Li-loading. A grand canonical Monte Carlo (GCMC) scheme was used to calculate the open circuit voltage profile during cell discharge. The Li-S binary phase diagram was constructed using genetic algorithm based tools. Overall, these simulation results provide insight into the behavior of sulfur based cathode materials that are needed for developing lithium-sulfur batteries. C1 [Islam, Md Mahbubul; van Duin, Adri C. T.] Penn State Univ, Dept Mech & Nucl Engn, University Pk, PA 16802 USA. [Ostadhossein, Alireza] Penn State Univ, Dept Engn Sci & Mech, University Pk, PA 16802 USA. [Borodin, Oleg] US Army, Res Lab, Electrochem Branch, Adelphi, MD 20783 USA. [Yeates, A. Todd] US Air Force, Res Lab, Mat & Mfg Directorate, AFRL RXBN, Wright Patterson AFB, OH 45433 USA. [Tipton, William W.; Hennig, Richard G.] Cornell Univ, Dept Mat Sci & Engn, Ithaca, NY 14853 USA. [Kumar, Nitin] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP van Duin, ACT (reprint author), Penn State Univ, Dept Mech & Nucl Engn, University Pk, PA 16802 USA. EM acv13@psu.edu RI Islam, Md Mahbubul/O-9375-2015; Borodin, Oleg/B-6855-2012; Hennig, Richard/A-2978-2008 OI Islam, Md Mahbubul/0000-0003-4584-2204; Borodin, Oleg/0000-0002-9428-5291; Hennig, Richard/0000-0003-4933-7686 FU US Army Research Laboratory through the Collaborative Research Alliance (CRA) for Multi Scale Multidisciplinary Modeling of Electronic Materials (MSME); DoD High Performance Computing (HPC) Productivity Enhancement, Technology Transfer, and Training (PETTT) Program [PP-CCM-KY03-005-P3] FX This work was supported by the grant from the US Army Research Laboratory through the Collaborative Research Alliance (CRA) for Multi Scale Multidisciplinary Modeling of Electronic Materials (MSME) and DoD High Performance Computing (HPC) Productivity Enhancement, Technology Transfer, and Training (PETTT) Program contract number PP-CCM-KY03-005-P3. NR 84 TC 25 Z9 25 U1 10 U2 108 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2015 VL 17 IS 5 BP 3383 EP 3393 DI 10.1039/c4cp04532g PG 11 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AZ4OW UT WOS:000348203200047 PM 25529209 ER PT J AU Chen, JL Chang, CC Ho, YK Chen, CL Hsu, CC Jang, WL Wei, DH Dong, CL Pao, CW Lee, JF Chen, JM Guo, JH Wu, MK AF Chen, Jeng-Lung Chang, Chun-Chieh Ho, Ying-Kai Chen, Chi Liang Hsu, Chih-Chin Jang, Wei-Luen Wei, Da-Hua Dong, Chung-Li Pao, Chih-Wen Lee, Jyh-Fu Chen, Jin-Ming Guo, Jinghua Wu, Maw-Kuen TI Behind the color switching in gasochromic VO2 SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID RAY EMISSION-SPECTROSCOPY; METAL-INSULATOR-TRANSITION; SYNCHROTRON-RADIATION; ELECTRONIC-PROPERTIES; TEMPERATURE; ABSORPTION; SCATTERING; HYDROGEN; SPECTRA; SOLIDS AB Gasochromic VO2 thin films were fabricated by the sol-gel spin-coating technique. The results of X-ray absorption spectroscopy and resonant inelastic X-ray scattering spectroscopy reveal that the origin of gasochromic coloration in VO2 is strongly related to the modulation of its structure and the electron-electron correlation. Upon gasochromic coloration, not only does the valence state change with the incorporation of hydrogen, but also the film undergoes the modification of the local atomic structure. The structural distortion varies the strength of hybridization of the O 2p-V 3d states and the bond distance of V-O and V-O varies. In the hydric process, the local atomic structure of VO2 changes from that of an un-symmetric to that of a symmetric V-O framework. The incorporated hydrogen adds electrons into the V 3d t(2g) orbital, enhancing the electron-electron correlation by reducing the V-V distance. This work presents a new physical insight in which the modulation of the electron-electron correlation is exploited to control the bleached and colored states, giving rise to the gasochromic phenomenon. The strong correlation among atomic spatial rearrangement, electronic structures, and transmittance supports a cooperative mechanism of the VO2 gasochromic transition. These results reveal a clear correlation between the dynamics of the lattice structure and the electronic properties and suggest a possible pathway to gasochromism and elucidation of its mechanism. C1 [Chen, Jeng-Lung; Hsu, Chih-Chin; Jang, Wei-Luen; Dong, Chung-Li; Pao, Chih-Wen; Lee, Jyh-Fu; Chen, Jin-Ming] Natl Synchrotron Radiat Res Ctr, Hsinchu 30076, Taiwan. [Chang, Chun-Chieh; Ho, Ying-Kai; Chen, Chi Liang; Wu, Maw-Kuen] Acad Sinica, Inst Phys, Taipei 11529, Taiwan. [Ho, Ying-Kai; Wei, Da-Hua] Natl Taipei Univ Technol, Dept Mech Engn, Taipei 10608, Taiwan. [Guo, Jinghua] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Chen, CL (reprint author), Acad Sinica, Inst Phys, Taipei 11529, Taiwan. EM clchen@phys.sinica.edu.tw; dong.cl@nsrrc.org.tw FU Ministry of Science and Technology (MOST) [MOST 101-212-M-213-004-MY3, 102-2112-M-001-004-MY3] FX This work is supported by the Ministry of Science and Technology (MOST) (formerly the National Science Council (NSC)) of Taiwan, under contracts no. MOST 101-212-M-213-004-MY3 and 102-2112-M-001-004-MY3. NR 38 TC 6 Z9 6 U1 5 U2 43 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2015 VL 17 IS 5 BP 3482 EP 3489 DI 10.1039/c4cp04623d PG 8 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AZ4OW UT WOS:000348203200060 PM 25533311 ER PT J AU Ma, YC Ghosh, SK Bera, S Jiang, Z Tristram-Nagle, S Lurio, LB Sinha, SK AF Ma, Yicong Ghosh, Sajal K. Bera, Sambhunath Jiang, Zhang Tristram-Nagle, Stephanie Lurio, Laurence B. Sinha, Sunil K. TI Accurate calibration and control of relative humidity close to 100% by X-raying a DOPC multilayer SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID LIPID-BILAYERS; DIFFRACTION; HYDRATION; MEMBRANES; MULTIBILAYERS; FLUCTUATIONS; SCATTERING; PRESSURE; ABSENCE; DMPC AB In this study, we have designed a compact sample chamber that can achieve accurate and continuous control of the relative humidity (RH) in the vicinity of 100%. A 1,2-dioleoyl-sn-glycero-3-phosphocholine (DOPC) multilayer can be used as a humidity sensor by measuring its inter-layer repeat distance (d-spacing) via X-ray diffraction. We convert from DOPC d-spacing to RH according to a theory given in the literature and previously measured data of DOPC multilamellar vesicles in polyvinylpyrrolidone (PVP) solutions. This curve can be used for calibration of RH close to 100%, a regime where conventional sensors do not have sufficient accuracy. We demonstrate that this control method can provide RH accuracies of 0.1 to 0.01%, which is a factor of 10-100 improvement compared to existing methods of humidity control. Our method provides fine tuning capability of RH continuously for a single sample, whereas the PVP solution method requires new samples to be made for each PVP concentration. The use of this cell also potentially removes the need for an X-ray or neutron beam to pass through bulk water if one wishes to work close to biologically relevant conditions of nearly 100% RH. C1 [Ma, Yicong; Ghosh, Sajal K.; Sinha, Sunil K.] Univ Calif San Diego, Dept Phys, La Jolla, CA 92093 USA. [Bera, Sambhunath; Lurio, Laurence B.] No Illinois Univ, Dept Phys, De Kalb, IL 60115 USA. [Jiang, Zhang] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. [Tristram-Nagle, Stephanie] Carnegie Mellon Univ, Dept Phys, Biol Phys Grp, Pittsburgh, PA 15213 USA. RP Sinha, SK (reprint author), Univ Calif San Diego, Dept Phys, La Jolla, CA 92093 USA. EM ssinha@physics.ucsd.edu RI Jiang, Zhang/A-3297-2012; Tristram-Nagle, Prof. Stephanie/N-7811-2014 OI Jiang, Zhang/0000-0003-3503-8909; Tristram-Nagle, Prof. Stephanie/0000-0003-2271-7056 FU U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]; Office of Basic Energy Sciences, U.S. Dept. of Energy under DOE [DE-FG02-04ER46173] FX X-ray data were collected on beamline 33BM at the Advanced Photon Source, Argonne National Laboratory. The authors would like to thank beamline scientists Evguenia Karapetrova and Christian Schlepuetz for their great help. Use of the Advanced Photon Source was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. This work was supported by the Office of Basic Energy Sciences, U.S. Dept. of Energy under DOE Grant number: DE-FG02-04ER46173. NR 23 TC 3 Z9 3 U1 2 U2 16 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2015 VL 17 IS 5 BP 3570 EP 3576 DI 10.1039/c4cp04407j PG 7 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AZ4OW UT WOS:000348203200069 PM 25537423 ER PT J AU Chen, YQ Elshobaki, M Gebhardt, R Bergeson, S Noack, M Park, JM Hillier, AC Ho, KM Biswas, R Chaudhary, S AF Chen, Yuqing Elshobaki, Moneim Gebhardt, Ryan Bergeson, Stephen Noack, Max Park, Joong-Mok Hillier, Andrew C. Ho, Kai-Ming Biswas, Rana Chaudhary, Sumit TI Reducing optical losses in organic solar cells using microlens arrays: theoretical and experimental investigation of microlens dimensions SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID LIGHT-EMITTING-DIODES; MORPHOLOGY EVOLUTION; POLYMER; EXTRACTION; ABSORPTION; EFFICIENCY; ENHANCEMENT; DEVICES; BLENDS; LIMIT AB The performance of organic photovoltaic devices is improving steadily and efficiencies have now exceeded 10%. However, the incident solar spectrum still largely remains poorly absorbed. To reduce optical losses, we employed a microlens array (MLA) layer on the side of the glass substrate facing the incident light; this approach does not interfere with the processing of the active-layer. We observed up to 10% enhancement in the short circuit current of poly({4,8-bis[(2-ethylhexyl)oxy]benzo[1,2-b: 4,5-b']dithiophene-2,6-diyl}{3-fluoro-2-[(2-ethylhexyl)carbonyl] thieno[3,4-b] thiophenediyl}):(6,6)-phenyl C71-butyric acid methyl ester (PTB7: PC71BM) OPV cells. Theoretically and experimentally investigating several MLA dimensions, we found that photocurrent increases with the ratio of the height to the pitch size of MLA. Simulations reveal the enhancement mechanisms: MLA focuses light, and also increases the light path within the active-layer by diffraction. Photocurrent enhancements increase for a polymer system with thinner active-layers, as demonstrated in poly[N-9'-heptadecanyl-2,7-carbazole-alt-5,5-(4',7'-di-2-thienyl-2',1',3'- benzothiadiazole)] (PCDTBT): PC71BM OPVs with 17% improvement in short circuit current. C1 [Chen, Yuqing; Noack, Max; Chaudhary, Sumit] Iowa State Univ, Dept Elect & Comp Engn, Ames, IA 50011 USA. [Elshobaki, Moneim; Gebhardt, Ryan; Chaudhary, Sumit] Iowa State Univ, Dept Mat Sci & Engn, Ames, IA 50011 USA. [Elshobaki, Moneim] Mansoura Univ, Fac Sci, Dept Phys, Mansoura 35516, Egypt. [Gebhardt, Ryan; Park, Joong-Mok; Ho, Kai-Ming; Biswas, Rana] US DOE, Ames Lab, Ames, IA 50011 USA. [Bergeson, Stephen; Ho, Kai-Ming; Biswas, Rana] Iowa State Univ, Dept Phys & Astron, Ames, IA 50011 USA. [Hillier, Andrew C.] Iowa State Univ, Dept Chem & Biol Engn, Ames, IA 50011 USA. RP Chaudhary, S (reprint author), Iowa State Univ, Dept Elect & Comp Engn, Ames, IA 50011 USA. EM sumitc@iastate.edu OI Elshobaki, Moneim/0000-0003-2125-0394 NR 38 TC 9 Z9 9 U1 4 U2 33 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2015 VL 17 IS 5 BP 3723 EP 3730 DI 10.1039/c4cp05221h PG 8 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AZ4OW UT WOS:000348203200086 PM 25556607 ER PT S AU Jellinek, J AF Jellinek, Julius BE Dinner, AR TI TRANSITION FROM ATOMS TO CLUSTERS TO CONDENSED MATTER SO PROCEEDINGS OF THE 240 CONFERENCE: SCIENCE'S GREAT CHALLENGES SE Advances in Chemical Physics LA English DT Review CT 240th Conference on Science's Great Challenges CY SEP 13-15, 2012 CL Univ Chicago, Chicago, IL HO Univ Chicago ID ELECTRONIC SHELL STRUCTURE; METAL-CLUSTERS; MICROCANONICAL ENSEMBLE; MOLECULAR-DYNAMICS; JELLIUM MODEL; SYSTEMS; RANGE; TEMPERATURE; SODIUM C1 Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. RP Jellinek, J (reprint author), Argonne Natl Lab, Chem Sci & Engn Div, 9700 S Cass Ave, Argonne, IL 60439 USA. FU Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences, U.S. Department of Energy [DE-AC02-06CH11357] FX This work was supported by the Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences, U.S. Department of Energy, under Contract No. DE-AC02-06CH11357. I thank Steve Berry and my past and present postdocs and collaborators for stimulating discussions and environment that were conducive to thinking about the ideas presented in this essay. NR 30 TC 0 Z9 0 U1 3 U2 11 PU JOHN WILEY & SONS INC PI HOBOKEN PA 111 RIVER ST, HOBOKEN, NJ 07030 USA SN 0065-2385 BN 978-1-118-95960-2; 978-1-118-95959-6 J9 ADV CHEM PHYS JI Adv. Chem. Phys. PY 2015 VL 157 BP 25 EP 42 PG 18 WC Physics, Atomic, Molecular & Chemical SC Physics GA BB9TT UT WOS:000348650300004 ER PT S AU Young, L AF Young, Linda BE Dinner, AR TI UNDERSTANDING ULTRAINTENSE X-RAY INTERACTIONS WITH MATTER SO PROCEEDINGS OF THE 240 CONFERENCE: SCIENCE'S GREAT CHALLENGES SE Advances in Chemical Physics LA English DT Review CT 240th Conference on Science's Great Challenges CY SEP 13-15, 2012 CL Univ Chicago, Chicago, IL HO Univ Chicago ID FREE-ELECTRON LASER; K-SHELL; PHYSICS; PULSES; REGION; PHOTOIONIZATION; OPERATION; ATOMS; NEON C1 Argonne Natl Lab, Argonne, IL 60439 USA. RP Young, L (reprint author), Argonne Natl Lab, 9700 S Cass Ave, Argonne, IL 60439 USA. NR 47 TC 0 Z9 0 U1 0 U2 2 PU JOHN WILEY & SONS INC PI HOBOKEN PA 111 RIVER ST, HOBOKEN, NJ 07030 USA SN 0065-2385 BN 978-1-118-95960-2; 978-1-118-95959-6 J9 ADV CHEM PHYS JI Adv. Chem. Phys. PY 2015 VL 157 BP 183 EP 194 PG 12 WC Physics, Atomic, Molecular & Chemical SC Physics GA BB9TT UT WOS:000348650300016 ER PT S AU Schneider, BI Bartschat, KR Guan, XX Feder, D Collins, LA AF Schneider, Barry I. Bartschat, Klaus R. Guan, Xiaoxu Feder, David Collins, Lee A. BE Dinner, AR TI TIME-DEPENDENT COMPUTATIONAL METHODS FOR MATTER UNDER EXTREME CONDITIONS SO PROCEEDINGS OF THE 240 CONFERENCE: SCIENCE'S GREAT CHALLENGES SE Advances in Chemical Physics LA English DT Review CT 240th Conference on Science's Great Challenges CY SEP 13-15, 2012 CL Univ Chicago, Chicago, IL HO Univ Chicago C1 [Schneider, Barry I.] Natl Sci Fdn, Off Cyberinfrastruct, Arlington, VA 22230 USA. [Bartschat, Klaus R.; Guan, Xiaoxu] Drake Univ, Dept Phys & Astron, Des Moines, IA 50311 USA. [Feder, David] Univ Calgary, Inst Quantum Sci & Technol, Calgary, AB T2N 1N4, Canada. [Feder, David] Univ Calgary, Dept Phys & Astron, Calgary, AB T2N 1N4, Canada. Los Alamos Natl Lab, Div Theoret, Los Alamos, NM USA. RP Schneider, BI (reprint author), NIST, Appl & Computat Math Div, Gaithersburg, MD 20899 USA. RI Guan, Xiaoxu/A-1299-2013 FU National Science Foundation [PHY-0757755, PHY-1068140, PHY-1430245]; Institutional Computing Program at the Los Alamos National Laboratory; National Nuclear Security Administration of the U.S. Department of Energy [DE-AC52-06NA25396]; XSEDE program [TG-PHY-090031] FX This work was supported, in part, by the National Science Foundation under grants No. PHY-0757755, No. PHY-1068140, and No, PHY-1430245 (KB and XG), and by the Institutional Computing Program at the Los Alamos National Laboratory, operated by Los Alamos National Security, LLC for the National Nuclear Security Administration of the U.S. Department of Energy under Contract No. DE-AC52-06NA25396 (LAC). The authors also thank the National Science Foundation and the XSEDE program for significant computational support under TeraGrid/XSEDE allocation No. TG-PHY-090031. NR 22 TC 0 Z9 0 U1 0 U2 0 PU JOHN WILEY & SONS INC PI HOBOKEN PA 111 RIVER ST, HOBOKEN, NJ 07030 USA SN 0065-2385 BN 978-1-118-95960-2; 978-1-118-95959-6 J9 ADV CHEM PHYS JI Adv. Chem. Phys. PY 2015 VL 157 BP 195 EP 214 PG 20 WC Physics, Atomic, Molecular & Chemical SC Physics GA BB9TT UT WOS:000348650300017 ER PT S AU Beebe, E Alessi, J Binello, S Kanesue, T McCafferty, D Morris, J Okamura, M Pikin, A Ritter, J Schoepfer, R AF Beebe, E. Alessi, J. Binello, S. Kanesue, T. McCafferty, D. Morris, J. Okamura, M. Pikin, A. Ritter, J. Schoepfer, R. BE Lapierre, A Schwarz, S Baumann, TM TI Reliable Operation of the Brookhaven EBIS for Highly Charged Ion Production for RHIC and NSRL SO PROCEEDINGS OF THE XII INTERNATIONAL SYMPOSIUM ON ELECTRON BEAM ION SOURCES AND TRAPS SE AIP Conference Proceedings LA English DT Proceedings Paper CT 12th International Symposium on Electron Beam Ion Sources and Traps CY MAY 18-21, 2014 CL Michigan State Univ, Natl Superconducting Cyclotron Lab, East Lansing, MI SP Facil Rare Isotope Beams, GSI Helmholtz Ctr Heavy Ion Res, Amer Inst Phys, Review Sci Instruments, Agilent Technologies, DREEBIT HO Michigan State Univ, Natl Superconducting Cyclotron Lab AB An Electron Beam Ion Source for the Relativistic Heavy Ion Collider (RHIC EBIS) was commissioned at Brookhaven in September 2010 and since then it routinely supplies ions for RHIC and NASA Space Radiation Laboratory (NSRL) as the main source of highly charged ions from Helium to Uranium. Using three external primary ion sources for 1+ injection into the EBIS and an electrostatic injection beam line, ion species at the EBIS exit can be switched in 0.2 s. A total of 16 different ion species have been produced to date. The length and the capacity of the ion trap have been increased by 20% by extending the trap by two more drift tubes, compared with the original design. The fraction of Au32+ in the EBIS Au spectrum is approximately 12% for 70-80% electron beam neutralization and 8 pulses operation in a 5 Hertz train and 4-5 s super cycle. For single pulse per super cycle operation and 25% electron beam neutralization, the EBIS achieves the theoretical Au32+ fractional output of 18%. Long term stability has been very good with availability of the beam from RHIC EBIS during 2012 and 2014 RHIC runs approximately 99.8%. C1 [Beebe, E.; Alessi, J.; Binello, S.; Kanesue, T.; McCafferty, D.; Morris, J.; Okamura, M.; Pikin, A.; Ritter, J.; Schoepfer, R.] Brookhaven Natl Lab, Upton, NY 11973 USA. RP Beebe, E (reprint author), Brookhaven Natl Lab, Upton, NY 11973 USA. EM beebe@bnl.gov NR 9 TC 1 Z9 1 U1 3 U2 4 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1279-8 J9 AIP CONF PROC PY 2015 VL 1640 DI 10.1063/1.4905394 PG 7 WC Engineering, Electrical & Electronic; Physics, Applied SC Engineering; Physics GA BB8XD UT WOS:000347721900002 ER PT S AU Dickerson, C Peters, C AF Dickerson, Clayton Peters, Christopher BE Lapierre, A Schwarz, S Baumann, TM TI The CARIBU EBIS Control and Synchronization System SO PROCEEDINGS OF THE XII INTERNATIONAL SYMPOSIUM ON ELECTRON BEAM ION SOURCES AND TRAPS SE AIP Conference Proceedings LA English DT Proceedings Paper CT 12th International Symposium on Electron Beam Ion Sources and Traps CY MAY 18-21, 2014 CL Michigan State Univ, Natl Superconducting Cyclotron Lab, East Lansing, MI SP Facil Rare Isotope Beams, GSI Helmholtz Ctr Heavy Ion Res, Amer Inst Phys, Review Sci Instruments, Agilent Technologies, DREEBIT HO Michigan State Univ, Natl Superconducting Cyclotron Lab AB The Californium Rare Isotope Breeder Upgrade (CARIBU) Electron Beam Ion Source (EBIS) charge breeder has been built and tested. The bases of the CARIBU EBIS electrical system are four voltage platforms on which both DC and pulsed high voltage outputs are controlled. The high voltage output pulses are created with either a combination of a function generator and a high voltage amplifier, or two high voltage DC power supplies and a high voltage solid state switch. Proper synchronization of the pulsed voltages, fundamental to optimizing the charge breeding performance, is achieved with triggering from a digital delay pulse generator. The control system is based on National Instruments real-time controllers and LabVIEW software implementing Functional Global Variables (FGV) to store and access instrument parameters. Fiber optic converters enable network communication and triggering across the platforms. C1 [Dickerson, Clayton; Peters, Christopher] Argonne Natl Lab, Argonne, IL 60439 USA. RP Dickerson, C (reprint author), Argonne Natl Lab, 9700 S Cass Ave, Argonne, IL 60439 USA. EM cdickerson@anl.gov NR 3 TC 1 Z9 1 U1 1 U2 1 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1279-8 J9 AIP CONF PROC PY 2015 VL 1640 DI 10.1063/1.4905411 PG 5 WC Engineering, Electrical & Electronic; Physics, Applied SC Engineering; Physics GA BB8XD UT WOS:000347721900019 ER PT S AU Kondrashev, S Barcikowski, A Dickerson, C Ostroumov, PN Sharamentov, S Vondrasek, R Pikin, A AF Kondrashev, S. Barcikowski, A. Dickerson, C. Ostroumov, P. N. Sharamentov, S. Vondrasek, R. Pikin, A. BE Lapierre, A Schwarz, S Baumann, TM TI First Charge Breeding Results at CARIBU EBIS SO PROCEEDINGS OF THE XII INTERNATIONAL SYMPOSIUM ON ELECTRON BEAM ION SOURCES AND TRAPS SE AIP Conference Proceedings LA English DT Proceedings Paper CT 12th International Symposium on Electron Beam Ion Sources and Traps CY MAY 18-21, 2014 CL Michigan State Univ, Natl Superconducting Cyclotron Lab, East Lansing, MI SP Facil Rare Isotope Beams, GSI Helmholtz Ctr Heavy Ion Res, Amer Inst Phys, Review Sci Instruments, Agilent Technologies, DREEBIT HO Michigan State Univ, Natl Superconducting Cyclotron Lab AB The Electron Beam Ion Source (EBIS) developed to breed CARIBU radioactive beams at ATLAS is currently in the off-line commissioning stage. The beam commissioning is being performed using a low emittance surface ionization source producing singly-charged cesium ions. The primary goal of the off-line commissioning is the demonstration of high-efficiency charge breeding in the pulsed injection mode. An overview of the final design of the CARIBU EBIS charge breeder, the off-line commissioning installation and the first results on charge breeding of stable cesium ions are presented and discussed. C1 [Kondrashev, S.; Barcikowski, A.; Dickerson, C.; Ostroumov, P. N.; Sharamentov, S.; Vondrasek, R.] Argonne Natl Lab, 9700 S Cass Ave, Argonne, IL 60439 USA. [Pikin, A.] Brookhaven Natl Lab, Upton, NY 11973 USA. RP Kondrashev, S (reprint author), Argonne Natl Lab, 9700 S Cass Ave, Argonne, IL 60439 USA. EM kondrashev@anl.gov FU U.S. Department of Energy, Office of Nuclear Physics [DE- AC02-06CH11357] FX This work was supported by the U.S. Department of Energy, Office of Nuclear Physics, under contract number DE- AC02-06CH11357. NR 12 TC 3 Z9 3 U1 0 U2 1 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1279-8 J9 AIP CONF PROC PY 2015 VL 1640 DI 10.1063/1.4905400 PG 14 WC Engineering, Electrical & Electronic; Physics, Applied SC Engineering; Physics GA BB8XD UT WOS:000347721900008 ER PT S AU Mertzig, R Shornikov, A Beebe, E Pikin, A Wenander, F AF Mertzig, R. Shornikov, A. Beebe, E. Pikin, A. Wenander, F. BE Lapierre, A Schwarz, S Baumann, TM TI Electron Beam Simulation from Gun to Collector: Towards a Complete Solution SO PROCEEDINGS OF THE XII INTERNATIONAL SYMPOSIUM ON ELECTRON BEAM ION SOURCES AND TRAPS SE AIP Conference Proceedings LA English DT Proceedings Paper CT 12th International Symposium on Electron Beam Ion Sources and Traps CY MAY 18-21, 2014 CL Michigan State Univ, Natl Superconducting Cyclotron Lab, East Lansing, MI SP Facil Rare Isotope Beams, GSI Helmholtz Ctr Heavy Ion Res, Amer Inst Phys, Review Sci Instruments, Agilent Technologies, DREEBIT HO Michigan State Univ, Natl Superconducting Cyclotron Lab ID BACKSCATTERING AB An electron-beam simulation technique for high-resolution complete EBIS/T modelling is presented. The technique was benchmarked on the high compression HEC2 test-stand with an electron beam current, current density and energy of 10 A, 10 kA/cm(2) and 49.2 keV, and on the immersed electron beam at REXEBIS for electron beam characteristics of 0.4 A, 200 A/cm(2) and 4.5 keV. In both Brillouin-like and immersed beams the electron-beam radius varies from several millimeters at the gun, through some hundreds of micrometers in the ionization region to a few centimeters at the collector over a total length of several meters. We report on our approach for finding optimal meshing parameters, based on the local beam properties such as magnetic field-strength, electron energy and beam radius. This approach combined with dividing the problem domain into sub-domains, and subsequent splicing of the local solutions allowed us to simulate the beam propagation in EBISes from the gun to the collector using a conventional PC in about 24-36 h. Brillouin-like electron beams propagated through the complete EBIS were used to analyze the beam behavior within the collector region. We checked whether elastically reflected paraxial electrons from a Brillouin-like beam will escape from the collector region and add to the loss current. We have also studied the power deposition profiles as function of applied potentials using two electrode geometries for a Brillouin-like beam including the effects of backscattered electrons. C1 [Mertzig, R.; Shornikov, A.; Wenander, F.] CERN, CH-1211 Geneva 23, Switzerland. [Beebe, E.; Pikin, A.] Brookhaven Natl Lab, Upton, NY 11973 USA. RP Mertzig, R (reprint author), CERN, CH-1211 Geneva 23, Switzerland. EM robert.mertzig@cern.ch FU HIE-ISOLDE design study; CATHI Marie Curie Initial Training Network [264330] FX We would like to acknowledge financial support by the HIE-ISOLDE design study and by the CATHI Marie Curie Initial Training Network: EU-FP7-PEOPLE-2010-ITN Project number 264330. NR 11 TC 2 Z9 2 U1 0 U2 5 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1279-8 J9 AIP CONF PROC PY 2015 VL 1640 DI 10.1063/1.4905397 PG 10 WC Engineering, Electrical & Electronic; Physics, Applied SC Engineering; Physics GA BB8XD UT WOS:000347721900005 ER PT S AU Perry, A Ostroumov, PN Barcikowski, A Dickerson, C Kondrashev, SA Mustapha, B Savard, G AF Perry, A. Ostroumov, P. N. Barcikowski, A. Dickerson, C. Kondrashev, S. A. Mustapha, B. Savard, G. BE Lapierre, A Schwarz, S Baumann, TM TI Design of the Low Energy Beam Transport Line between CARIBU and the EBIS Charge Breeder SO PROCEEDINGS OF THE XII INTERNATIONAL SYMPOSIUM ON ELECTRON BEAM ION SOURCES AND TRAPS SE AIP Conference Proceedings LA English DT Proceedings Paper CT 12th International Symposium on Electron Beam Ion Sources and Traps CY MAY 18-21, 2014 CL Michigan State Univ, Natl Superconducting Cyclotron Lab, East Lansing, MI SP Facil Rare Isotope Beams, GSI Helmholtz Ctr Heavy Ion Res, Amer Inst Phys, Review Sci Instruments, Agilent Technologies, DREEBIT HO Michigan State Univ, Natl Superconducting Cyclotron Lab AB An Electron Beam Ion Source Charge Breeder (EBIS-CB) has been developed to breed radioactive beams from the CAlifomium Rare isotope Breeder Upgrade (CARIBU) facility at ATLAS. The EBIS-CB will replace the existing ECR charge breeder to increase the intensity and improve the purity of reaccelerated radioactive ion beams. The EBIS-CB is in the final stage of off-line commissioning. Currently, we are developing a low energy beam transport (LEBT) system to transfer CARIBU beams to the EBIS-CB. As was originally planned, an RFQ cooler-buncher will precede the EBIS-CB. Recently, it was decided to include a multi-reflection time-of-flight (MR-TOE) mass-spectrometer following the RFQ. MR-TOF is a relatively new technology used to purify beams with a mass-resolving power up to 3x 10(5) as was demonstrated in experiments at CERN/ISOLDE. Very high purity singly-charged radioactive ion beams will be injected into the EBIS for charge breeding and due to its inherent properties, the EBIS-CB will maintain the purity of the charge bred beams. Possible contamination of residual gas ions will be greatly suppressed by achieving ultra-high vacuum in the EBIS trap. This paper will present and discuss the design of the LEBT and the overall integration of the EBIS-CB into ATLAS. C1 [Perry, A.; Ostroumov, P. N.; Barcikowski, A.; Dickerson, C.; Kondrashev, S. A.; Mustapha, B.; Savard, G.] Argonne Natl Lab, Argonne, IL 60439 USA. RP Perry, A (reprint author), Argonne Natl Lab, 9700 S Cass Ave, Argonne, IL 60439 USA. EM aperry4@hawk.iit.edu NR 15 TC 1 Z9 1 U1 0 U2 2 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1279-8 J9 AIP CONF PROC PY 2015 VL 1640 DI 10.1063/1.4905401 PG 12 WC Engineering, Electrical & Electronic; Physics, Applied SC Engineering; Physics GA BB8XD UT WOS:000347721900009 ER PT S AU Pikin, A Alessi, JG Beebe, EN Shornikov, A Mertzig, R Wenander, F Scrivens, R AF Pikin, Alexander Alessi, James G. Beebe, Edward N. Shornikov, Andrey Mertzig, Robert Wenander, Fredrik Scrivens, Richard BE Lapierre, A Schwarz, S Baumann, TM TI First Test of BNL Electron Beam Ion Source with High Current Density Electron Beam SO PROCEEDINGS OF THE XII INTERNATIONAL SYMPOSIUM ON ELECTRON BEAM ION SOURCES AND TRAPS SE AIP Conference Proceedings LA English DT Proceedings Paper CT 12th International Symposium on Electron Beam Ion Sources and Traps CY MAY 18-21, 2014 CL Michigan State Univ, Natl Superconducting Cyclotron Lab, East Lansing, MI SP Facil Rare Isotope Beams, GSI Helmholtz Ctr Heavy Ion Res, Amer Inst Phys, Review Sci Instruments, Agilent Technologies, DREEBIT HO Michigan State Univ, Natl Superconducting Cyclotron Lab ID TEST EBIS; DESIGN AB A new electron gun with electrostatic compression has been installed at the Electron Beam Ion Source (EBIS) Test Stand at BNL. This is a collaborative effort by BNL and CERN teams with a common goal to study an EBIS with electron beam current up to 10 A, current density up to 10,000 A/cm(2) and energy more than 50 keV. Intensive and pure beams of heavy highly charged ions with mass-to-charge ratio < 4.5 are requested by many heavy ion research facilities including NASA Space Radiation Laboratory (NSRL) at BNL and HIE-ISOLDE at CERN. With a multiampere electron gun, the EBIS should be capable of delivering highly charged ions for both RHIC facility applications at BNL and for ISOLDE experiments at CERN. Details of the electron gun simulations and design, and the Test EBIS electrostatic and magnetostatic structures with the new electron gun are presented. The experimental results of the electron beam transmission are given. C1 [Pikin, Alexander; Alessi, James G.; Beebe, Edward N.] Brookhaven Natl Lab, Upton, NY 11973 USA. [Shornikov, Andrey; Mertzig, Robert; Wenander, Fredrik; Scrivens, Richard] CERN, CH-1211 Geneva 23, Switzerland. RP Pikin, A (reprint author), Brookhaven Natl Lab, Upton, NY 11973 USA. EM pikin@bnl.gov FU US Department of Energy and the National Aeronautic and Space Administration; HIE- ISOLDE design study; CATHI Marie Curie Initial Training Network EU- FP7- PEOPLE- 2010- ITN [264330] FX Work supported under the auspices of the US Department of Energy and the National Aeronautic and Space Administration. A. S., R. M. and F. W. would like to acknowledge support by the HIE- ISOLDE design study and by the CATHI Marie Curie Initial Training Network: EU- FP7- PEOPLE- 2010- ITN Project number 264330. NR 9 TC 3 Z9 3 U1 1 U2 1 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1279-8 J9 AIP CONF PROC PY 2015 VL 1640 DI 10.1063/1.4905395 PG 7 WC Engineering, Electrical & Electronic; Physics, Applied SC Engineering; Physics GA BB8XD UT WOS:000347721900003 ER PT S AU Schenkel, T Weis, CD Lo, CC Persaud, A Chakarov, I Schneider, DH Bokor, J AF Schenkel, T. Weis, C. D. Lo, C. C. Persaud, A. Chakarov, I. Schneider, D. H. Bokor, J. BE Lapierre, A Schwarz, S Baumann, TM TI Deterministic Doping and the Exploration of Spin Qubits SO PROCEEDINGS OF THE XII INTERNATIONAL SYMPOSIUM ON ELECTRON BEAM ION SOURCES AND TRAPS SE AIP Conference Proceedings LA English DT Proceedings Paper CT 12th International Symposium on Electron Beam Ion Sources and Traps CY MAY 18-21, 2014 CL Michigan State Univ, Natl Superconducting Cyclotron Lab, East Lansing, MI SP Facil Rare Isotope Beams, GSI Helmholtz Ctr Heavy Ion Res, Amer Inst Phys, Review Sci Instruments, Agilent Technologies, DREEBIT HO Michigan State Univ, Natl Superconducting Cyclotron Lab DE quantum computing; highly charged ions; ion implantation ID ION-IMPLANTATION; NUCLEAR-SPIN; QUANTUM COMPUTER; ELECTRON-SPIN; SILICON; READOUT AB Deterministic doping by single ion implantation, the precise placement of individual dopant atoms into devices, is a path for the realization of quantum computer test structures where quantum bits (qubits) are based on electron and nuclear spins of donors or color centers. We present a donor - quantum dot type qubit architecture and discuss the use of medium and highly charged ions extracted from an Electron Beam Ion Trap/Source (EBIT/S) for deterministic doping. EBIT/S are attractive for the formation of qubit test structures due to the relatively low emittance of ion beams from an EBIT/S and due to the potential energy associated with the ions' charge state, which can aid single ion imp act detection. Following ion implantation, dopant specific diffusion mechanisms during device processing affect the placement accuracy and coherence properties of donor spin qubits. For bismuth, range straggling is minimal but its relatively low solubility in silicon limits thermal budgets for the formation of qubit test structures. C1 [Schenkel, T.; Weis, C. D.; Lo, C. C.; Persaud, A.; Bokor, J.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Accelerator & Fus Res, Berkeley, CA 94720 USA. [Lo, C. C.; Bokor, J.] Univ Calif Berkeley, Dept Elect Engn & Comp Sci, Berkeley, CA 94720 USA. [Chakarov, I.] Global Foundries, Malta, NY 12020 USA. [Schneider, D. H.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. RP Schenkel, T (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Accelerator & Fus Res, Berkeley, CA 94720 USA. RI Bokor, Jeffrey/A-2683-2011 FU U.S. National Security Agency [100000080295]; Office of Science; U.S. Department of Energy; Laboratory Directed Research and Development Program at Berkeley Lab [DE-AC02-05CH11231] FX This work was supported by the U.S. National Security Agency under 100000080295 and by the Office of Science of the U.S. Department of Energy and by the Laboratory Directed Research and Development Program at Berkeley Lab under contract no. DE-AC02-05CH11231. NR 25 TC 1 Z9 1 U1 2 U2 11 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1279-8 J9 AIP CONF PROC PY 2015 VL 1640 DI 10.1063/1.4905409 PG 5 WC Engineering, Electrical & Electronic; Physics, Applied SC Engineering; Physics GA BB8XD UT WOS:000347721900017 ER PT S AU Shornikov, A Beebe, EN Mertzig, RC Pikin, A Wenander, FJC AF Shornikov, Andrey Beebe, Edward N. Mertzig, Robert C. Pikin, Alexander Wenander, Fredrik J. C. BE Lapierre, A Schwarz, S Baumann, TM TI High Performance Charge Breeder for HIE-ISOLDE and TSR@ISOLDE Applications SO PROCEEDINGS OF THE XII INTERNATIONAL SYMPOSIUM ON ELECTRON BEAM ION SOURCES AND TRAPS SE AIP Conference Proceedings LA English DT Proceedings Paper CT 12th International Symposium on Electron Beam Ion Sources and Traps CY MAY 18-21, 2014 CL Michigan State Univ, Natl Superconducting Cyclotron Lab, East Lansing, MI SP Facil Rare Isotope Beams, GSI Helmholtz Ctr Heavy Ion Res, Amer Inst Phys, Review Sci Instruments, Agilent Technologies, DREEBIT HO Michigan State Univ, Natl Superconducting Cyclotron Lab ID DESIGN AB We report on the development of the HEC2 (High Energy Compression and Current) charge breeder, a possible high performance successor to REXEBIS at ISOLDE. The new breeder would match the performance of the HIE-ISOLDE linac upgrade and make full use of the possible installation of a storage ring at ISOLDE (the TSR@ISOLDE initiative [1]). Dictated by ion beam acceptance and capacity requirements, the breeder features a 2-3.5 A electron beam. In many cases very high charge states, including bare ions up to Z=70 and Li/Na-like up to Z=92 could be requested for experiments in the storage ring, therefore, electron beam energies up to 150 keV are required. The electron-beam current density needed for producing ions with such high charge states at an injection rate into TSR of 0.5-1 Hz is between 10 and 20 kA/cm(2), which agrees with the current density needed to produce A/q<4.5 ions for the HIE-ISOLDE linac with a maximum repetition rate of 100 Hz. The first operation of a prototype electron gun with a pulsed electron beam of 1.5 A and 30 keV was demonstrated in a joint experiment with BNL [2]. In addition, we report on further development aiming to achieve CW operation of an electron beam having a geometrical transverse ion-acceptance matching the injection of 1(+) ions (11.5 mu m), and an emittance/energy spread of the extracted ion beam matching the downstream mass separator and RFQ (0.08 mu m normalized /+/- 1%). C1 [Shornikov, Andrey; Mertzig, Robert C.; Wenander, Fredrik J. C.] CERN, CH-1211 Geneva 23, Switzerland. [Beebe, Edward N.; Pikin, Alexander] Brookhaven Natl Lab, Upton, NY 11973 USA. RP Shornikov, A (reprint author), CERN, CH-1211 Geneva 23, Switzerland. EM andrey.shornikov@cern.ch FU HIE-ISOLDE design study; CATHI Marie Curie Initial Training Network: EU-FP7-PEOPLE-2010-ITN [264330] FX We would like to acknowledge financial support by the HIE-ISOLDE design study and by the CATHI Marie Curie Initial Training Network: EU-FP7-PEOPLE-2010-ITN Project number 264330. The authors want to thank Ivan Podadera-Aliseda and Matthew Fraser for their input on the REXTRAP and REX mass separator/ RFQ. NR 11 TC 2 Z9 2 U1 0 U2 1 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1279-8 J9 AIP CONF PROC PY 2015 VL 1640 DI 10.1063/1.4905396 PG 9 WC Engineering, Electrical & Electronic; Physics, Applied SC Engineering; Physics GA BB8XD UT WOS:000347721900004 ER PT J AU Sridharan, DM Asaithamby, A Bailey, SM Costes, SV Doetsch, PW Dynan, WS Kronenberg, A Rithidech, KN Saha, J Snijders, AM Werner, E Wiese, C Cucinotta, FA Pluth, JM AF Sridharan, D. M. Asaithamby, A. Bailey, S. M. Costes, S. V. Doetsch, P. W. Dynan, W. S. Kronenberg, A. Rithidech, K. N. Saha, J. Snijders, A. M. Werner, E. Wiese, C. Cucinotta, F. A. Pluth, J. M. TI Understanding Cancer Development Processes after HZE-Particle Exposure: Roles of ROS, DNA Damage Repair and Inflammation SO RADIATION RESEARCH LA English DT Review ID DOUBLE-STRAND BREAKS; DEPENDENT PROTEIN-KINASE; INDUCED GENOMIC INSTABILITY; GAP-JUNCTION COMMUNICATION; HUMAN FIBROBLAST-CULTURES; GEV/NUCLEON FE-56 IONS; HIGH-LET RADIATION; INDUCED CHROMOSOMAL INSTABILITY; IRRADIATED HUMAN-CELLS; ATOMIC-BOMB SURVIVORS AB During space travel astronauts are exposed to a variety of radiations, including galactic cosmic rays composed of high-energy protons and high-energy charged (HZE) nuclei, and solar particle events containing low-to medium-energy protons. Risks from these exposures include carcinogenesis, central nervous system damage and degenerative tissue effects. Currently, career radiation limits are based on estimates of fatal cancer risks calculated using a model that incorporates human epidemiological data from exposed populations, estimates of relative biological effectiveness and dose-response data from relevant mammalian experimental models. A major goal of space radiation risk assessment is to link mechanistic data from biological studies at NASA Space Radiation Laboratory and other particle accelerators with risk models. Early phenotypes of HZE exposure, such as the induction of reactive oxygen species, DNA damage signaling and inflammation, are sensitive to HZE damage complexity. This review summarizes our current understanding of critical areas within the DNA damage and oxidative stress arena and provides insight into their mechanistic interdependence and their usefulness in accurately modeling cancer and other risks in astronauts exposed to space radiation. Our ultimate goals are to examine potential links and crosstalk between early response modules activated by charged particle exposure, to identify critical areas that require further research and to use these data to reduced uncertainties in modeling cancer risk for astronauts. A clearer understanding of the links between early mechanistic aspects of high-LET response and later surrogate cancer end points could reveal key nodes that can be therapeutically targeted to mitigate the health effects from charged particle exposures. (C) 2015 by Radiation Research Society. C1 [Sridharan, D. M.; Costes, S. V.; Kronenberg, A.; Snijders, A. M.; Pluth, J. M.] Lawrence Berkeley Natl Lab, Berkeley, CA 94710 USA. [Asaithamby, A.; Saha, J.] Univ Texas SW Med Ctr Dallas, Dallas, TX 75390 USA. [Bailey, S. M.; Wiese, C.] Colorado State Univ, Ft Collins, CO 80523 USA. [Doetsch, P. W.; Dynan, W. S.; Werner, E.] Emory Univ, Atlanta, GA 30322 USA. [Rithidech, K. N.] SUNY Stony Brook, Stony Brook, NY 11794 USA. [Cucinotta, F. A.] Univ Nevada, Las Vegas, NV 89154 USA. RP Pluth, JM (reprint author), Lawrence Berkeley Natl Lab, 717 Potter St, Berkeley, CA 94710 USA. EM jmpluth@lbl.gov FU NASA [NNX13AD57G, NNX08AB65G, NNJ09HC64I, NNX11AC30G, NNJ12HB88I, NNJ06HA33I, NNJ13HA96I, NNX11AK91G, NNJ11HB91I]; NSCOR [NNX11AC54G]; NIH/NIAID [R01080486-02]; Low Dose Scientific Focus Area, U.S. Department of Energy [DE-AC02-05CH11231, DE-AI02-10ER64969] FX We would like to acknowledge that there is a large body of work that has been done in this area and due to space limitations we could not discuss it in its entirety. Thus, we apologize in advance for important works that we were unable to cite in the current review. The authors are members of NASA's Virtual Systems Biology Modeling (VSBM) team on ROS and DNA damage, and wish to thank laboratory members and staff who have assisted in the cited work, as well as the scientists and staff at the NASA Space Radiation Laboratory at Brookhaven National Laboratory. The authors are grateful to Drs. M. Weil (Colorado State University), M. Naidu (Center of Cancer Systems Biology at GeneSys Research Institute (GRI)/Tufts School of Medicine) and E. Azzam (Rutgers New Jersey Medical School) for critical comments on the review and valuable discussions. This work was supported by: NASA NNX13AD57G and NSCOR NNX11AC54G (A. Asaithamby); NASA NNX08AB65G (S. Bailey); NIH/NIAID R01080486-02 (S. Bailey); NASA NNJ09HC64I and the Low Dose Scientific Focus Area, U.S. Department of Energy DE-AC02-05CH11231 (S. V. Costes); NASA NNX11AC30G (W. Dynan, P. Doetsch and E. Werner); NASA NNJ12HB88I (A. Kronenberg); NASA NNJ06HA33I and NNJ13HA96I (J. Pluth, D. Sridharan); NASA NNX11AK91G (K. Rithidech); Low Dose Scientific Focus Area, U.S. Department of Energy DE-AI02-10ER64969 (J. Saha); Low Dose Scientific Focus Area, U.S. Department of Energy DE-AC02-05CH11231 (A. Snijders); NASA NNJ11HB91I (C. Wiese). NR 248 TC 13 Z9 13 U1 0 U2 19 PU RADIATION RESEARCH SOC PI LAWRENCE PA 810 E TENTH STREET, LAWRENCE, KS 66044 USA SN 0033-7587 EI 1938-5404 J9 RADIAT RES JI Radiat. Res. PD JAN PY 2015 VL 183 IS 1 BP 1 EP 26 DI 10.1667/RR13804.1 PG 26 WC Biology; Biophysics; Radiology, Nuclear Medicine & Medical Imaging SC Life Sciences & Biomedicine - Other Topics; Biophysics; Radiology, Nuclear Medicine & Medical Imaging GA AZ0WI UT WOS:000347962400001 PM 25564719 ER PT J AU Shulga, YM Vasilets, VN Kiryukhin, DP Voylov, DN Sokolov, AP AF Shulga, Yury M. Vasilets, Victor N. Kiryukhin, Dmitry P. Voylov, Dmitry N. Sokolov, Alexei P. TI Polymer composites prepared by low-temperature post-irradiation polymerization of C2F4 in the presence of graphene-like material: synthesis and characterization SO RSC ADVANCES LA English DT Article ID INDUCED CROSS-LINKING; X-RAY PHOTOELECTRON; GRAPHITE OXIDE; ATOMIC OXYGEN; CARBON; POLYTETRAFLUOROETHYLENE; REDUCTION; POLY(TETRAFLUOROETHYLENE); FUNCTIONALIZATION; PHOTOEMISSION AB Polymer polytetrafluoroethylene (PTFE)-microwave exfoliated graphene oxide (MEGO) composites containing up to 80 wt% PTFE were prepared by low-temperature post-irradiation polymerization of C2F4 in the presence of the graphene-like material. Composites were characterized by FTIR, NMR, XPS, SEM, TGA, XRD, broadband dielectric spectroscopy and DSC techniques. The melting point of PTFE in the composite (332.5 degrees C) was higher than that of pure PTFE by 8.8 degrees C. The measured values of the melting enthalpy (Delta H-m = 51.5 and 45.4 J g(-1)) were used to calculate the extent of crystallinity in the PTFE and PTFE-MEGO composite (0.63 and 0.55, respectively). No CF3 end groups typical of commercial PTFE have been detected in the PTFE-MEGO composites. C1 [Shulga, Yury M.; Kiryukhin, Dmitry P.] Russian Acad Sci, Inst Problems Chem Phys, Chernogolovka 142432, Moscow Region, Russia. [Vasilets, Victor N.] Russian Acad Sci, Inst Energy Problems Chem Phys, Chernogolovka 142432, Moscow Region, Russia. [Shulga, Yury M.] Natl Univ Sci & Technol MISIS, Moscow 119049, Russia. [Voylov, Dmitry N.; Sokolov, Alexei P.] Univ Tennessee, Dept Chem, Knoxville, TN 37916 USA. [Voylov, Dmitry N.; Sokolov, Alexei P.] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37830 USA. RP Shulga, YM (reprint author), Russian Acad Sci, Inst Problems Chem Phys, Chernogolovka 142432, Moscow Region, Russia. EM shulga@icp.ac.ru RI Voylov, Dmitry/H-4059-2013 OI Voylov, Dmitry/0000-0001-5552-6024 FU Russian Foundation for Basic Research [12-03-00261, 13-03-00398]; RF Ministry of Education and Science [14.594.21.0007, RFMEFI59414X0007, 11.1797.2014/K]; Division of Materials Sciences and Engineering, DOE Office of Basic Energy Sciences FX This work was partially supported by the Russian Foundation for Basic Research (project nos 12-03-00261 and 13-03-00398) and RF Ministry of Education and Science (State Contract no. 14.594.21.0007, RFMEFI59414X0007), State Assignment no. 11.1797.2014/K. US team thanks the Division of Materials Sciences and Engineering, DOE Office of Basic Energy Sciences for financial support. NR 50 TC 2 Z9 2 U1 4 U2 26 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2046-2069 J9 RSC ADV JI RSC Adv. PY 2015 VL 5 IS 13 BP 9865 EP 9874 DI 10.1039/c4ra09074h PG 10 WC Chemistry, Multidisciplinary SC Chemistry GA AZ1BY UT WOS:000347976500071 ER PT J AU Kim, D Roh, HS Kim, Y No, K Hong, S AF Kim, Dongjin Roh, Hee Seok Kim, Yeontae No, Kwangsoo Hong, Seungbum TI Selective current collecting design for spring- type energy harvesters SO RSC ADVANCES LA English DT Article ID GENERATING ELECTRICITY; WALKING AB Here we present a high performance spring-type piezoelectric energy harvester that selectively collects current from the inner part of a spring shell. We analyzed themain reason behind the low efficiency of the initial design using finite element models and proposed a selective current collecting design that can considerably improve the electrical conversion efficiency of the energy harvester. We found that the newly designed energy harvester increases the output voltage by 8 times leading to an output power of 2.21 mW under an impulsive load of 2.18 N when compared with the conventional design. We envision that selective current collecting design will be used in spring-based self-powered active sensors and energy scavenging devices. C1 [Kim, Dongjin; Kim, Yeontae; No, Kwangsoo; Hong, Seungbum] Korea Adv Inst Sci & Technol, Dept Mat Sci & Engn, Taejon 305701, South Korea. [Kim, Dongjin; Hong, Seungbum] Argonne Natl Lab, Div Mat Sci, Lemont, IL 60439 USA. [Roh, Hee Seok] Argonne Natl Lab, Nucl Engn Div, Lemont, IL 60439 USA. RP No, K (reprint author), Korea Adv Inst Sci & Technol, Dept Mat Sci & Engn, Taejon 305701, South Korea. EM ksno@kaist.ac.kr; seungbum@kaist.ac.kr RI Hong, Seungbum/B-7708-2009; No, Kwangsoo/C-1983-2011 OI Hong, Seungbum/0000-0002-2667-1983; FU National Research Foundation (NRF) - Ministry of Education, Science and Technology (MEST), Korea [2011-K000674, 2010-0015063]; UChicago Argonne; U.S. DOE Office of Science Laboratory [DE-AC02-06CH11357] FX This research was supported by the Converging Research Center Program (no. 2011-K000674) and Mid-career Researcher Program (no. 2010-0015063) through the National Research Foundation (NRF) funded by the Ministry of Education, Science and Technology (MEST), Korea. Work at Argonne National Laboratory (D.K., S.H., and H.R., design of selective current collection scheme, simulation of stress and charge, data analysis and writing of manuscript) was supported by UChicago Argonne, a U.S. DOE Office of Science Laboratory, operated under Contract no. DE-AC02-06CH11357. NR 18 TC 7 Z9 7 U1 0 U2 5 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2046-2069 J9 RSC ADV JI RSC Adv. PY 2015 VL 5 IS 14 BP 10662 EP 10666 DI 10.1039/c4ra16443a PG 5 WC Chemistry, Multidisciplinary SC Chemistry GA AZ3RJ UT WOS:000348144100073 ER PT J AU Graves, R Pitarka, A AF Graves, Robert Pitarka, Arben TI Refinements to the Graves and Pitarka (2010) Broadband Ground-Motion Simulation Method SO SEISMOLOGICAL RESEARCH LETTERS LA English DT Article ID CONSTANT STRESS-DROP; SOURCE PARAMETERS; 1994 NORTHRIDGE; RUPTURE LENGTH; TIME HISTORIES; 1988 SAGUENAY; EARTHQUAKE; SLIP; DISPLACEMENT; ATTENUATION C1 [Graves, Robert] US Geol Survey, Pasadena, CA 91106 USA. [Pitarka, Arben] Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. RP Graves, R (reprint author), US Geol Survey, 525 S Wilson Ave, Pasadena, CA 91106 USA. EM rwgraves@usgs.gov; pitarka1@linl.gov RI pitarka, arben/K-5491-2014 FU National Science Foundation (NSF) [EAR-1033462]; United States Geological Survey (USGS) [G12AC20038] FX The authors are very grateful to Fabio Silva, Scott Callaghan, and Phil Maechling of Southern California Earthquake Center (SCEC) for their efforts in implementing the simulation codes on the Broadband Platform (BBP). Constructive reviews by Elizabeth Cochran, Morgan Page, Walter Imperatori, and an anonymous reviewer helped to improve the manuscript. SCEC is funded by National Science Foundation (NSF) Cooperative Agreement EAR-1033462 and United States Geological Survey (USGS) Cooperative Agreement G12AC20038. The SCEC contribution number for this paper is 1947. NR 30 TC 14 Z9 14 U1 0 U2 1 PU SEISMOLOGICAL SOC AMER PI ALBANY PA 400 EVELYN AVE, SUITE 201, ALBANY, CA 94706-1375 USA SN 0895-0695 J9 SEISMOL RES LETT JI Seismol. Res. Lett. PD JAN-FEB PY 2015 VL 86 IS 1 BP 75 EP 80 DI 10.1785/0220140101 PG 6 WC Geochemistry & Geophysics SC Geochemistry & Geophysics GA AZ1QY UT WOS:000348014200011 ER PT J AU Anthony, RE Aster, RC Wiens, D Nyblade, A Anandakrishnan, S Huerta, A Winberry, JP Wilson, T Rowe, C AF Anthony, Robert E. Aster, Richard C. Wiens, Douglas Nyblade, Andrew Anandakrishnan, Sridhar Huerta, Audrey Winberry, J. Paul Wilson, Terry Rowe, Charlotte TI The Seismic Noise Environment of Antarctica SO SEISMOLOGICAL RESEARCH LETTERS LA English DT Article ID STICK-SLIP MOTION; UNITED-STATES; BACKGROUND-NOISE; ICE STREAM; MICROSEISMS; DEPTH C1 [Anthony, Robert E.; Aster, Richard C.] Colorado State Univ, Dept Geosci, Ft Collins, CO 80523 USA. [Wiens, Douglas] Washington Univ, Dept Earth & Planetary Sci, St Louis, MO 63130 USA. [Nyblade, Andrew; Anandakrishnan, Sridhar] Penn State Univ, Dept Geosci, University Pk, PA 16802 USA. [Huerta, Audrey; Winberry, J. Paul] Cent Washington Univ, Dept Geol Sci, Ellensburg, WA 98926 USA. [Wilson, Terry] Ohio State Univ, Dept Geol Sci, Columbus, OH 43210 USA. [Rowe, Charlotte] Los Alamos Natl Lab, Geophys Grp, Los Alamos, NM 87545 USA. RP Anthony, RE (reprint author), Colorado State Univ, Dept Geosci, Ft Collins, CO 80523 USA. EM robertanthony@colostate.edu RI Aster, Richard/E-5067-2013; OI Aster, Richard/0000-0002-0821-4906; Rowe, Charlotte/0000-0001-5803-0147 FU NSF [EAR-1063471, 0632230, 0632239, 0652322, 0632335, 0632136, 0632209, 0632185, 1246776, 1246712, 1419268]; Department of Energy National Nuclear Security Administration FX We express thanks to Tim Parker (Incorporated Research Institutions for Seismology Program for the Array Seismic Studies of the Continental Lithosphere [IRIS-PASSCAL] Instrument Center), Kent Anderson (IRIS), Adam Ringler (US. Geological Survey [USGS] Albuquerque Seismological Laboratory), Dan McNamara (USGS, National Earthquake Information Center), and Susan Bilek and David Reusch (New Mexico Tech) for useful exchanges. The facilities of the IRIS Data Management System, and specifically the IRIS Data Management Center, were used for access to waveform and metadata required in this study. Sea ice concentration data around Antarctica were obtained from The National Snow and Ice Data Center (NSIDC). The Global Seismographic Network (GSN) is a cooperative scientific facility operated jointly by the IRIS, the USGS, and the National Science Foundation (NSF). The facilities of the IRIS Consortium are supported by the NSF under Cooperative Agreement EAR-1063471, NSF Polar Programs, and the Department of Energy National Nuclear Security Administration. POLENET-Antarctica phase 1 was supported by NSF Polar Programs Grant Numbers 0632230, 0632239, 0652322, 0632335, 0632136, 0632209, and 0632185, and POLENET-Antarctica phase 2 is supported by NSF Polar Programs Grant Numbers 1246776, 1246712, and 1419268. Additional funding was provided by Los Alamos National Laboratory through the Institute of Geophysics, Planetary Physics. Additional information regarding the POLENET project, data collection sites, and geophysical data is available at polenet.org (last accessed October 2014). NR 51 TC 10 Z9 10 U1 1 U2 9 PU SEISMOLOGICAL SOC AMER PI ALBANY PA 400 EVELYN AVE, SUITE 201, ALBANY, CA 94706-1375 USA SN 0895-0695 EI 1938-2057 J9 SEISMOL RES LETT JI Seismol. Res. Lett. PD JAN-FEB PY 2015 VL 86 IS 1 BP 89 EP 100 DI 10.1785/0220140109 PG 12 WC Geochemistry & Geophysics SC Geochemistry & Geophysics GA AZ1QY UT WOS:000348014200013 ER PT J AU Kirby, J Nishimoto, M Chow, RWN Baidoo, EEK Wang, G Martin, J Schackwitz, W Chan, R Fortman, JL Keasling, JD AF Kirby, James Nishimoto, Minobu Chow, Ruthie W. N. Baidoo, Edward E. K. Wang, George Martin, Joel Schackwitz, Wendy Chan, Rossana Fortman, Jeffrey L. Keasling, Jay D. TI Enhancing Terpene Yield from Sugars via Novel Routes to 1-Deoxy-D-Xylulose 5-Phosphate SO APPLIED AND ENVIRONMENTAL MICROBIOLOGY LA English DT Article ID 3,4-DIHYDROXY-2-BUTANONE 4-PHOSPHATE SYNTHASE; ESCHERICHIA-COLI; ISOPRENOID BIOSYNTHESIS; SACCHAROMYCES-CEREVISIAE; METABOLIC FLUX; IN-VITRO; PATHWAY; RIBOFLAVIN; BIOFUELS; GENES AB Terpene synthesis in the majority of bacterial species, together with plant plastids, takes place via the 1-deoxy-D-xylulose 5-phosphate (DXP) pathway. The first step of this pathway involves the condensation of pyruvate and glyceraldehyde 3-phosphate by DXP synthase (Dxs), with one-sixth of the carbon lost as CO2. A hypothetical novel route from a pentose phosphate to DXP (nDXP) could enable a more direct pathway from C-5 sugars to terpenes and also circumvent regulatory mechanisms that control Dxs, but there is no enzyme known that can convert a sugar into its 1-deoxy equivalent. Employing a selection for complementation of a dxs deletion in Escherichia coli grown on xylose as the sole carbon source, we uncovered two candidate nDXP genes. Complementation was achieved either via overexpression of the wild-type E. coli yajO gene, annotated as a putative xylose reductase, or via various mutations in the native ribB gene. In vitro analysis performed with purified YajO and mutant RibB proteins revealed that DXP was synthesized in both cases from ribulose 5-phosphate (Ru5P). We demonstrate the utility of these genes for microbial terpene biosynthesis by engineering the DXP pathway in E. coli for production of the sesquiterpene bisabolene, a candidate biodiesel. To further improve flux into the pathway from Ru5P, nDXP enzymes were expressed as fusions to DXP reductase (Dxr), the second enzyme in the DXP pathway. Expression of a Dxr-RibB(G108S) fusion improved bisabolene titers more than 4-fold and alleviated accumulation of intracellular DXP. C1 [Kirby, James; Nishimoto, Minobu; Chow, Ruthie W. N.; Chan, Rossana; Fortman, Jeffrey L.; Keasling, Jay D.] Univ Calif Berkeley, Calif Inst Quantitat Biosci QB3, Berkeley, CA 94720 USA. [Kirby, James; Nishimoto, Minobu; Baidoo, Edward E. K.; Wang, George; Keasling, Jay D.] Joint BioEnergy Inst, Emeryville, CA USA. [Keasling, Jay D.] Univ Calif Berkeley, Dept Biomol & Chem Engn, Berkeley, CA 94720 USA. [Keasling, Jay D.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA 94720 USA. [Martin, Joel; Schackwitz, Wendy] Joint Genome Inst, Walnut Creek, CA USA. RP Keasling, JD (reprint author), Univ Calif Berkeley, Calif Inst Quantitat Biosci QB3, Berkeley, CA 94720 USA. EM keasling@berkeley.edu FU Office of Science, Office of Biological and Environmental Research, of the U.S. Department of Energy [DE-AC02-05CH11231]; U.S. Department of Energy ARPA-E PETRO program [DE-AR0000209] FX The work conducted through the Joint BioEnergy Institute was supported by the Office of Science, Office of Biological and Environmental Research, of the U.S. Department of Energy under contract no. DE-AC02-05CH11231. The work conducted through the University of California at Berkeley was funded through the U.S. Department of Energy ARPA-E PETRO program, under grant no. DE-AR0000209. NR 46 TC 3 Z9 3 U1 2 U2 36 PU AMER SOC MICROBIOLOGY PI WASHINGTON PA 1752 N ST NW, WASHINGTON, DC 20036-2904 USA SN 0099-2240 EI 1098-5336 J9 APPL ENVIRON MICROB JI Appl. Environ. Microbiol. PD JAN PY 2015 VL 81 IS 1 BP 130 EP 138 DI 10.1128/AEM.02920-14 PG 9 WC Biotechnology & Applied Microbiology; Microbiology SC Biotechnology & Applied Microbiology; Microbiology GA AY1TZ UT WOS:000347376200016 PM 25326299 ER PT J AU Hart, R AF Hart, Reid TI Have We Run Out Of Savings Potential In Standard 90.1? SO ASHRAE JOURNAL LA English DT Article AB As part of their support to the ASHRAE Standing Standard Project Committee (SSPC) for Standard 90.1, Energy Standard for Buildings Except Low-Rise Residential Buildings,(1) Pacific Northwest National Laboratory (PNNL) staff members regularly perform a progress indicator analysis to quantitatively measure the progress of Standard 90.1 through its three-year standard development cycle.(2) The standard, which provides the minimum energy-efficiency requirements for design and construction, has produced significant energy savings since the first edition of Standard 90 in 1975. With challenging energy reduction goals ahead of us(3) combined with significant savings already achieved, code developers wonder if we have reached a point of diminishing returns in advancing energy codes and standards. C1 Pacific NW Natl Lab, Richland, WA 99352 USA. RP Hart, R (reprint author), Pacific NW Natl Lab, Richland, WA 99352 USA. FU U.S. Department of Energy's Building Energy Codes Program FX The study is built upon PNNL's code team's Progress Indicator analysis to support Standard 90.1-2013 development. The author would like to acknowledge PNNL commercial code simulation team including Michael Rosenberg, Rahul Athalye, Dr. YuLong Xie, Dr. Weimin Wang, Dr. Jian Zhang, Eric Richman, Mark Halverson, Supriya Goel, and Vrushali Mendon with team leadership by Bing Liu. Members of the ASHRAE SSPC 90.1 provided valuable feedback to development of the prototypes and typical buildings. This analysis was funded by the U.S. Department of Energy's Building Energy Codes Program. The author also acknowledges Mr. Jeremiah Williams from DOE for his technical guidance on this study. NR 10 TC 0 Z9 0 U1 1 U2 1 PU AMER SOC HEATING REFRIGERATING AIR-CONDITIONING ENG, INC, PI ATLANTA PA 1791 TULLIE CIRCLE NE, ATLANTA, GA 30329 USA SN 0001-2491 EI 1943-6637 J9 ASHRAE J JI ASHRAE J. PD JAN PY 2015 VL 57 IS 1 BP 26 EP 38 PG 13 WC Thermodynamics; Construction & Building Technology; Engineering, Mechanical SC Thermodynamics; Construction & Building Technology; Engineering GA AY6IA UT WOS:000347669000009 ER PT J AU Dale, BE AF Dale, Bruce E. TI A New Industry Has Been Launched: The Cellulosic Biofuels Ship (Finally) Sails SO BIOFUELS BIOPRODUCTS & BIOREFINING-BIOFPR LA English DT Editorial Material C1 Michigan State Univ, Dept Chem Engn & Mat Sci, DOE Great Lakes Bioenergy Res Ctr, E Lansing, MI 48824 USA. RP Dale, BE (reprint author), Michigan State Univ, Dept Chem Engn & Mat Sci, DOE Great Lakes Bioenergy Res Ctr, E Lansing, MI 48824 USA. EM bdale@egr.msu.edu NR 0 TC 6 Z9 6 U1 0 U2 7 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 1932-104X EI 1932-1031 J9 BIOFUEL BIOPROD BIOR JI Biofuels Bioprod. Biorefining PD JAN-FEB PY 2015 VL 9 IS 1 BP 1 EP 3 DI 10.1002/bbb.1532 PG 3 WC Biotechnology & Applied Microbiology; Energy & Fuels SC Biotechnology & Applied Microbiology; Energy & Fuels GA AZ0YU UT WOS:000347968600001 ER PT J AU Morgan, WF Sowa, MB AF Morgan, William F. Sowa, Marianne B. TI Non-targeted effects induced by ionizing radiation: Mechanisms and potential impact on radiation induced health effects SO CANCER LETTERS LA English DT Review DE Non-targeted effects; Ionizing radiation; Cell-cell communication ID INDUCED GENOMIC INSTABILITY; ATOMIC-BOMB SURVIVORS; INFLAMMATORY-TYPE RESPONSES; OXIDATIVE STRESS; CHROMOSOMAL INSTABILITY; REACTIVE OXYGEN; IN-VIVO; MITOCHONDRIAL DYSFUNCTION; SIGNAL-TRANSDUCTION; BYSTANDER AB Not-targeted effects represent a paradigm shift from the "DNA centric" view that ionizing radiation only elicits biological effects and subsequent health consequences as a result of an energy deposition event in the cell nucleus. While this is likely true at higher radiation doses (>1 Gy), at low doses (<100 mGy) non-targeted effects associated with radiation exposure might play a significant role. Here definitions of non-targeted effects are presented, the potential mechanisms for the communication of signals and signaling networks from irradiated cells/tissues are proposed, and the various effects of this intra- and intercellular signaling are described. We conclude with speculation on how these observations might lead to and impact long-term human health outcomes. (C) 2013 Elsevier Ireland Ltd. All rights reserved. C1 [Morgan, William F.; Sowa, Marianne B.] Pacific NW Natl Lab, Div Biol Sci, Richland, WA 99352 USA. RP Morgan, WF (reprint author), Pacific NW Natl Lab, Div Biol Sci, 902 Battelle Blvd,POB 999,MSIN J4-02, Richland, WA 99352 USA. EM wfmorgan@pnnl.gov FU Battelle Memorial Institute, Pacific Northwest Division [DE-AC05-76RL0 1830]; US Department of Energy (DOE), Office of Biological and Environmental Research (OBER) Low Dose Radiation Science Program FX Supported by Battelle Memorial Institute, Pacific Northwest Division, under Contract No. DE-AC05-76RL0 1830 with the US Department of Energy (DOE), Office of Biological and Environmental Research (OBER) Low Dose Radiation Science Program. NR 74 TC 22 Z9 22 U1 4 U2 26 PU ELSEVIER IRELAND LTD PI CLARE PA ELSEVIER HOUSE, BROOKVALE PLAZA, EAST PARK SHANNON, CO, CLARE, 00000, IRELAND SN 0304-3835 EI 1872-7980 J9 CANCER LETT JI Cancer Lett. PD JAN 1 PY 2015 VL 356 IS 1 SI SI BP 17 EP 21 DI 10.1016/j.canlet.2013.09.009 PG 5 WC Oncology SC Oncology GA AY4ZP UT WOS:000347583700004 PM 24041870 ER PT J AU White, CE Daemen, LL Hartl, M Page, K AF White, Claire E. Daemen, Luke L. Hartl, Monika Page, Katharine TI Intrinsic differences in atomic ordering of calcium (alumino)silicate hydrates in conventional and alkali-activated cements SO CEMENT AND CONCRETE RESEARCH LA English DT Article DE X-ray diffraction (B); Calcium-silicate-hydrate (C-S-H) (B); Amorphous material (B); Alkali-activated cement; Portland cement (D) ID PAIR DISTRIBUTION FUNCTION; C-S-H; SODIUM ALUMINOSILICATE; TRICALCIUM SILICATE; CRYSTAL-STRUCTURE; PORTLAND-CEMENT; LOCAL-STRUCTURE; ZEOLITE-A; SLAG; GEOPOLYMER AB The atomic structures of calcium silicate hydrate (C-S-H) and calcium (-sodium) aluminosilicate hydrate (C-(N)-A-S-H) gels, and their presence in conventional and blended cement systems, have been the topic of significant debate over recent decades. Previous investigations have revealed that synthetic C-S-H gel is nanocrystalline and due to the chemical similarities between ordinary Portland cement (OPC)-based systems and low-CO2 alkali-activated slags, researchers have inferred that the atomic ordering in alkali-activated slag is the same as in OPC-slag cements. Here, X-ray total scattering is used to determine the local bonding environment and nanostructure of C(-A)-S-H gels present in hydrated tricalcium silicate (C3S), blended C3S-slag and alkali-activated slag, revealing the large intrinsic differences in the extent of nanoscale ordering between C-S-H derived from C3S and alkali-activated slag systems, which may have a significant influence on thermodynamic stability, and material properties at higher length scales, including long term durability of alkali-activated cements. (C) 2014 Elsevier Ltd. All rights reserved. C1 [White, Claire E.] Princeton Univ, Dept Civil & Environm Engn, Princeton, NJ 08544 USA. [White, Claire E.] Princeton Univ, Andlinger Ctr Energy & Environm, Princeton, NJ 08544 USA. [White, Claire E.; Daemen, Luke L.; Hartl, Monika; Page, Katharine] Los Alamos Natl Lab, Manuel Lujan Jr Neutron Scattering Ctr, Los Alamos, NM 87545 USA. [White, Claire E.] Los Alamos Natl Lab, Los Alamos, NM USA. RP White, CE (reprint author), Princeton Univ, Dept Civil & Environm Engn, Princeton, NJ 08544 USA. EM whitece@princeton.edu RI Page, Katharine/C-9726-2009; White, Claire/A-1722-2011; Hartl, Monika/N-4586-2016 OI Page, Katharine/0000-0002-9071-3383; White, Claire/0000-0002-4800-7960; Hartl, Monika/0000-0002-6601-7273 FU Los Alamos National Laboratory; DOE [DE-AC52-06NA25396]; U.S. Department of Energy through the LANL/LDRD Program; U.S. DOE [DE-AC02-06CH11357] FX The participation of all authors in this work was supported by Los Alamos National Laboratory, which is operated by Los Alamos National Security LLC under DOE Contract DE-AC52-06NA25396. Furthermore, CEW gratefully acknowledges the support of the U.S. Department of Energy through the LANL/LDRD Program. The 11-ID-B beam line is located at the Advanced Photon Source, an Office of Science User Facility operated for the U.S. DOE Office of Science by Argonne National Laboratory, under U.S. DOE Contract No. DE-AC02-06CH11357. The authors would like to acknowledge the support and assistance of the beam line staff on 11-ID-B, and access to the beam line via a Partner User Proposal between 11-ID-B and the neutron PDF instrument NOMAD at SNS, ORNL. NR 46 TC 10 Z9 10 U1 6 U2 33 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0008-8846 EI 1873-3948 J9 CEMENT CONCRETE RES JI Cem. Concr. Res. PD JAN PY 2015 VL 67 BP 66 EP 73 DI 10.1016/j.cemconres.2014.08.006 PG 8 WC Construction & Building Technology; Materials Science, Multidisciplinary SC Construction & Building Technology; Materials Science GA AY3SF UT WOS:000347502100007 ER PT J AU Bali, G Meng, XZ Deneff, JI Sun, QN Ragauskas, AJ AF Bali, Garima Meng, Xianzhi Deneff, Jacob I. Sun, Qining Ragauskas, Arthur J. TI The Effect of Alkaline Pretreatment Methods on Cellulose Structure and Accessibility SO CHEMSUSCHEM LA English DT Article DE biomass; cellulose; crystallinity; enzyme catalysis; hydrolysis ID AQUEOUS AMMONIA; ENZYMATIC-HYDROLYSIS; SODIUM-HYDROXIDE; LIGNOCELLULOSIC BIOMASS; BIOFUEL PRODUCTION; HYBRID POPLAR; CORN STOVER; DILUTE-ACID; ETHANOL; SWITCHGRASS AB The effects of different alkaline pretreatments on cellulose structural features and accessibility are compared and correlated with the enzymatic hydrolysis of Populus. The pretreatments are shown to modify polysaccharides and lignin content to enhance the accessibility for cellulase enzymes. The highest increase in the cellulose accessibility was observed in dilute sodium hydroxide, followed by methods using ammonia soaking and lime (Ca(OH)(2)). The biggest increase of cellulose accessibility occurs during the first 10 min of pretreatment, with further increases at a slower rate as severity increases. Low temperature ammonia soaking at longer residence times dissolved a major portion of hemicellulose and exhibited higher cellulose accessibility than high temperature soaking. Moreover, the most significant reduction of degree of polymerization (DP) occurred for dilute sodium hydroxide (NaOH) and ammonia pre-treated Populus samples. The study thus identifies important cellulose structural features and relevant parameters related to biomass recalcitrance. C1 [Bali, Garima; Meng, Xianzhi; Sun, Qining] Georgia Inst Technol, Sch Chem & Biochem, Inst Paper Sci & Technol, Atlanta, GA 30332 USA. [Deneff, Jacob I.] Dept Chem & Biomol Engn, Storrs, CT 06269 USA. [Ragauskas, Arthur J.] Univ Tennessee, Oak Ridge Natl Lab, Dept Forestry Wildlife & Fisheries, Dept Chem & Biomol Engn,BioEnergy Sci Ctr, Knoxville, TN 37996 USA. RP Bali, G (reprint author), Georgia Inst Technol, Sch Chem & Biochem, Inst Paper Sci & Technol, 500,10th St NW, Atlanta, GA 30332 USA. EM aragausk@utk.edu RI Sun, Qining/B-7592-2016; OI Sun, Qining/0000-0002-9678-7834; Ragauskas, Arthur/0000-0002-3536-554X FU Genomic Science Program, Office of Biological and Environmental Research, U. S. Department of Energy [FWP ERKP752]; Office of Biological and Environmental Research [FWP ERKP291]; Office of Biological and Environmental Research in the DOE Office of Science through the BESC, a DOE Bioenergy Research Center; U. S. Department of Energy [DE-AC05-00OR22725]; Paper Science & Engineering fellowship program FX This research was supported, in part, by the Genomic Science Program, Office of Biological and Environmental Research, U. S. Department of Energy, under Contract FWP ERKP752. The research at Oak Ridge National Laboratory's Center for Structural Molecular Biology (CSMB) was supported by the Office of Biological and Environmental Research under Contract FWP ERKP291, using facilities supported by the Office of Basic Energy Sciences, U. S. Department of Energy. This work was also supported, in part, by the Office of Biological and Environmental Research in the DOE Office of Science through the BESC, a DOE Bioenergy Research Center. Oak Ridge National Laboratory is managed by UT-Battelle, LLC, for the U. S. Department of Energy under Contract DE-AC05-00OR22725. Finally, Q.S. wishes to acknowledge Paper Science & Engineering fellowship program and J.D. for NSF-REU support. NR 30 TC 15 Z9 16 U1 9 U2 61 PU WILEY-V C H VERLAG GMBH PI WEINHEIM PA BOSCHSTRASSE 12, D-69469 WEINHEIM, GERMANY SN 1864-5631 EI 1864-564X J9 CHEMSUSCHEM JI ChemSusChem PD JAN PY 2015 VL 8 IS 2 BP 275 EP 279 DI 10.1002/cssc.201402752 PG 5 WC Chemistry, Multidisciplinary; GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY SC Chemistry; Science & Technology - Other Topics GA AY9BE UT WOS:000347843800009 PM 25421020 ER PT J AU Liao, C Guo, BK Sun, XG Dai, S AF Liao, Chen Guo, Bingkun Sun, Xiao-Guang Dai, Sheng TI Synergistic Effects of Mixing Sulfone and Ionic Liquid as Safe Electrolytes for Lithium Sulfur Batteries SO CHEMSUSCHEM LA English DT Article DE electrochemistry; ionic liquids; lithium-sulfur batteries; polymers; sulfones ID ENERGY; CARBON; CATHODE; CELL AB A strategy of mixing both an ionic liquid and sulfone is reported to give synergistic effects of reducing viscosity, increasing ionic conductivity, reducing polysulfide dissolution, and improving safety. The mixtures of ionic liquids and sulfones also show distinctly different physicochemical properties, including thermal properties and crystallization behavior. By using these electrolytes, lithium sulfur batteries assembled with lithium and mesoporous carbon composites show a reversible specific capacity of 1265 mAhg(-1) (second cycle) by using 40% 1.0M lithium bis(trifluoromethylsulfonyl) imide (LiTFSI) in N-methyl-N-propylpyrrolidinium bis(trifluoromethylsulfonyl) imide with 60% 1.0M LiTFSI in methylisopropylsulfone in the first cycle. This capacity is slightly lower than that obtained in pure 1.0m LiTFSI as the sulfone electrolyte; however, it exhibits excellent cycling stability and remains as high as 655 mAhg(-1) even after 50 cycles. This strategy provides a method to alleviate polysulfide dissolution and redox shuttle phenomena, at the same time, with improved ionic conductivity. C1 [Liao, Chen] Argonne Natl Lab, Joint Ctr Energy Storage Res, Argonne, IL 60439 USA. [Guo, Bingkun; Sun, Xiao-Guang; Dai, Sheng] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. [Dai, Sheng] Univ Tennessee, Dept Chem, Knoxville, TN 37996 USA. RP Liao, C (reprint author), Argonne Natl Lab, Joint Ctr Energy Storage Res, 9700 S Cass Ave, Argonne, IL 60439 USA. EM liaoc@anl.gov; sunx@anl.gov; dais@anl.gov RI Guo, Bingkun/J-5774-2014; Dai, Sheng/K-8411-2015; OI Dai, Sheng/0000-0002-8046-3931; Liao, Chen/0000-0001-5168-6493 FU U.S. Department of Energy's Office of Basic Energy Science, Division of Materials Sciences and Engineering; Joint Center for Energy Storage Research, an Energy Innovation Hub - U.S. Department of Energy, Office of Science, Basic Energy Sciences FX This research was supported by the U.S. Department of Energy's Office of Basic Energy Science, Division of Materials Sciences and Engineering. C.L. was supported as part of the Joint Center for Energy Storage Research, an Energy Innovation Hub funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences. NR 24 TC 5 Z9 5 U1 13 U2 66 PU WILEY-V C H VERLAG GMBH PI WEINHEIM PA BOSCHSTRASSE 12, D-69469 WEINHEIM, GERMANY SN 1864-5631 EI 1864-564X J9 CHEMSUSCHEM JI ChemSusChem PD JAN PY 2015 VL 8 IS 2 BP 353 EP 360 DI 10.1002/cssc.201402800 PG 8 WC Chemistry, Multidisciplinary; GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY SC Chemistry; Science & Technology - Other Topics GA AY9BE UT WOS:000347843800019 PM 25427945 ER PT J AU Mara, MW Fransted, KA Chen, LX AF Mara, Michael W. Fransted, Kelly A. Chen, Lin X. TI Interplays of excited state structures and dynamics in copper(I) diimine complexes: Implications and perspectives SO COORDINATION CHEMISTRY REVIEWS LA English DT Review DE Copper diimine; Transition metal complexes; Excited state structure; Solar energy conversion; Ultrafast X-ray absorption; Ultrafast optical transient absorption ID SENSITIZED SOLAR-CELLS; RAY-ABSORPTION SPECTROSCOPY; CU-I COMPLEXES; EXTENDED X-RAY; CHARGE-TRANSFER; MOLECULAR-STRUCTURES; BIS-PHENANTHROLINE; LOCAL-STRUCTURE; FINE-STRUCTURE; PHOTOPHYSICAL PROPERTIES AB Although they were discovered almost four decades ago, Cu(I) diimine complexes have emerged as a group of transition metal complexes that can play important roles in solar energy conversion and utilization, and have potential to replace the quintessential ruthenium polypyridyl complexes as light sensitizers, electron donors and catalytic centers. This review includes some recent photophysical studies and transient structural studies of Cu(I) diimine complexes using ultrafast optical transient absorption and emission as well as X-ray transient absorption spectroscopy. The main focus is on identifying the key structural factors that influence the excited-state properties, such as structural reorganization, intersystem crossing and solvent quenching, with these relatively new techniques on the ultrafast time scales. Ultimately, these structural factors can be used to rationally control the energetics and dynamics of the MLCT state during the light conversion processes. This insight will serve as guidance for material design using Cu(I) diimine complexes as building blocks. (C) 2014 Elsevier B.V. All rights reserved. C1 [Mara, Michael W.; Chen, Lin X.] Northwestern Univ, Dept Chem, Evanston, IL 60208 USA. [Mara, Michael W.; Fransted, Kelly A.; Chen, Lin X.] Argonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USA. RP Chen, LX (reprint author), Argonne Natl Lab, Chem Sci & Engn Div, 9700 S Cass Ave, Lemont, IL 60439 USA. EM lchen@anl.gov FU U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]; U. S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357] FX We thank the support from the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. Use of the Advanced Photon Source at Argonne National Laboratory was supported by the U. S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. The authors would like to thank Drs. Klaus Attenkofer (now at NSLS-II, Brookhaven National Laboratory), Guy Jennings, Xiaoyi Zhang and Mr. Charles Kurtz of the Advanced Photon Source for their contributions to the Beamline 11ID-D facility at the APS. LXC would like to thank her collaborators in the XTA team since 2002, Drs. G. B. Shaw, E. C. Wasinger, J. V. Lockard, M. R. Harpham, A. B. Stickrath, J. Huang, Ms. M. L. Shelby for their contributions to the results included in the review. Our other collaborators contributions and scientific exchanges are also appreciated, Drs. G. Smolentsev, Kristoffer M. Haldrup, Profs. A. Sotadov, G. J. Meyer, F. Castellano, P. Coppens, and many others. The instrumentation supports (to DCC et al.) from the US Department of Energy for purchasing lasers, detectors and other related equipment enabling the initiation and upgrade of XTA experiments at Beamline 11IDD are greatly appreciated. NR 93 TC 32 Z9 32 U1 12 U2 62 PU ELSEVIER SCIENCE SA PI LAUSANNE PA PO BOX 564, 1001 LAUSANNE, SWITZERLAND SN 0010-8545 EI 1873-3840 J9 COORDIN CHEM REV JI Coord. Chem. Rev. PD JAN 1 PY 2015 VL 282 SI SI BP 2 EP 18 DI 10.1016/j.ccr.2014.06.013 PG 17 WC Chemistry, Inorganic & Nuclear SC Chemistry GA AY4ZQ UT WOS:000347583800002 ER PT J AU Gu, J Yan, Y Helbig, BJ Huang, ZQ Lian, TQ Schmehl, RH AF Gu, Jing Yan, Yong Helbig, Brian J. Huang, Zhuangqun Lian, Tianquan Schmehl, Russell H. TI The influence of ligand localized excited states on the photophysics of second row and third row transition metal terpyridyl complexes: Recent examples and a case study SO COORDINATION CHEMISTRY REVIEWS LA English DT Review DE Ruthenium; Terpyridyl complexes; Intraligand; Transient absorption; Diethylenetriamine; Excited state lifetime; MLCT; ILCT ID ENERGY-GAP LAW; TEMPERATURE LUMINESCENCE LIFETIMES; RU(II) COMPLEXES; ROOM-TEMPERATURE; RUTHENIUM(II) COMPLEXES; TRIDENTATE LIGANDS; BIS(TERPYRIDINE) COMPLEXES; MULTICHROMOPHORE APPROACH; POLYPYRIDINE COMPLEXES; ELECTRON-TRANSFER AB The photophysical behavior of Ru(II) and Os(II) diimine complexes having complex aromatic hydrocarbon diimine ligands has received considerable attention as systems exhibiting intramolecular energy transfer to yield excited states with lifetimes much longer than the parent diimine complexes. Here we present a focused discussion of the photophysical behavior of transition metal complexes with modified terpyridyl ligands. The overview includes, as an example of approaches used to evaluate such systems, spectroscopic studies of a pair of Ru(II) mono- and bis-terpyridyl complexes modified with vinylpyrene (Pyr-v-tpy) to have ligand localized excited states that are equal to or lower than the energy of the known MLCT state of the parent complexes, [Ru(Mpt)(2)](2+) and [Ru(Mpt)(dien)](2+) (Mpt = 4'-tolyl-2,2':6',2"-terpyridine, dien = diethylenetriamine). The common observation is that the presence of Pyr-v-tpy serves to lengthen the excited state lifetime of the complex through interaction of MLCT and ligand localized (IL) states. For [Ru(Pyr-v-tpy)(2)](2+) the excited state lifetime increases by a factor of more than 104 relative to [Ru(Mpt)(2)](2+). For [Ru(Pyr-v-tpy)(dien)](2+), the (IL)-I-3 state is close in energy to the MLCT state of the parent [Ru(Mpt)(dien)](2+) and, while the transient absorption spectrum is significantly perturbed relative to [Ru(Mpt)(dien)](2+), the excited state decay rate changes by only a factor of four. The long-lived excited state is formed in less than a ps, indicating strong coupling of the MLCT and ligand localized manifolds. (C) 2014 Elsevier B.V. All rights reserved. C1 [Gu, Jing; Yan, Yong; Helbig, Brian J.; Schmehl, Russell H.] Tulane Univ, Dept Chem, New Orleans, LA 70118 USA. [Huang, Zhuangqun; Lian, Tianquan] Emory Univ, Dept Chem, Atlanta, GA 30322 USA. [Gu, Jing; Yan, Yong] Natl Renewable Energy Lab, Golden, CO 80401 USA. RP Schmehl, RH (reprint author), Tulane Univ, Dept Chem, New Orleans, LA 70118 USA. EM russ@tulane.edu RI Yan, Yong/E-1087-2013 FU U.S. Department of Energy, Office of Basic Energy Sciences [DE-FG-02-96ER14617]; U.S. Department of Energy, Office of Basic Energy Sciences, Solar Photochemistry Program [DE-FG02-12ER16347]; U.S. National Science Foundation [CHE0619770]; IBM Corporation FX RHS wishes to thank the U.S. Department of Energy, Office of Basic Energy Sciences (DE-FG-02-96ER14617). TL is supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Solar Photochemistry Program (DE-FG02-12ER16347). We also thank the U.S. National Science Foundation (grant CHE0619770) for funding the ESI mass spectrometer. J.G. thanks the IBM Corporation for a fellowship in Computational Science administered through the Tulane Center for Computational Science. NR 60 TC 9 Z9 9 U1 4 U2 54 PU ELSEVIER SCIENCE SA PI LAUSANNE PA PO BOX 564, 1001 LAUSANNE, SWITZERLAND SN 0010-8545 EI 1873-3840 J9 COORDIN CHEM REV JI Coord. Chem. Rev. PD JAN 1 PY 2015 VL 282 SI SI BP 100 EP 109 DI 10.1016/j.ccr.2014.06.028 PG 10 WC Chemistry, Inorganic & Nuclear SC Chemistry GA AY4ZQ UT WOS:000347583800010 ER PT J AU Liu, XM Wanner, C Rudnick, RL McDonough, WF AF Liu, Xiao-Ming Wanner, Christoph Rudnick, Roberta L. McDonough, William F. TI Processes controlling delta Li-7 in rivers illuminated by study of streams and groundwaters draining basalts SO EARTH AND PLANETARY SCIENCE LETTERS LA English DT Article DE lithium isotopes; chemical weathering; rivers and groundwaters; reactive transport modeling ID LITHIUM ISOTOPIC COMPOSITION; WEATHERING PROCESSES; CONTINENTAL-CRUST; CO2 CONSUMPTION; FRACTIONATION; BEHAVIOR; LI; SEAWATER; GEOCHEMISTRY; CONSTRAINTS AB We evaluate the factors influencing the abundance, [Li], and isotopic composition of riverine Li delivered to the oceans through analyses and modeling of [Li] and delta Li-7 in streams and groundwaters draining a single continental lithology, the Columbia River Basalts (CRBs). The streams were sampled in different climate zones that lie east (dry), and west (wet) of the Cascades Mountains, and during two different seasons (summer and late winter) in order to evaluate climatic and seasonal influences on Li isotopes in rivers. Dissolved Li (delta Li-7(dis) = +9.3 to +30.4) is systematically heavier than that of fresh or weathered CRBs (-4.7 to +6.0, Liu et al., 2013), suspended loads (-5.9 to -0.3), and shallow groundwaters (+6.7 to +9.4), consistent with previous studies showing that Li isotope fractionation is affected by equilibration between stream water and secondary minerals. However, the lack of correlation between delta Li-7(dis) and climate zone, the uniform secondary minerals and bedrock, coupled with the highly variable (>20 parts per thousand) delta Li-7(dis) indicate that other factors exert a strong control on delta Li-7(dis). In particular, the heavier Li in streams compared to the shallow groundwaters that feed them indicates that continued isotopic fractionation between stream water and suspended and/or bed loads has a major influence on riverine delta Li-7. Seasonal delta Li-7 variation is observed only for streams west of the Cascades, where the difference in precipitation rate between the dry and wet seasons is greatest. Reactive transport model simulations reveal that riverine delta Li-7 is strongly controlled by subsurface residence times and the Li isotope fractionation occurring within rivers. The latter explains why there is no positive correlation between delta Li-7 and traditional weathering proxies such as Si or normalized Si in rivers, as riverine Li isotope fractionation drives delta Li-7 to higher values during transport, whereas the concentrations of major cations and anions are diluted. The varying residence time for groundwaters feeding the western streams in summer (long residence times, higher delta Li-7, greater weathering) and winter (short residence times, lower delta Li-7, less weathering) explains the observed seasonal variations. A global, negative correlation between delta Li-7 and Li/Na for streams and rivers draining basaltic catchments reflects the overall transport time, hence the amount of silicate weathering. Based on our results, the increase of delta Li-7 in seawater during the Cenozoic is unlikely related to changing climate, but may reflect mountain building giving rise to increased silicate weathering. (C) 2014 Elsevier B.V. All rights reserved. C1 [Liu, Xiao-Ming; Rudnick, Roberta L.; McDonough, William F.] Univ Maryland, Dept Geol, College Pk, MD 20742 USA. [Liu, Xiao-Ming] Carnegie Inst Sci, Geophys Lab, Washington, DC 20015 USA. [Wanner, Christoph] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, Berkeley, CA 94720 USA. RP Liu, XM (reprint author), Carnegie Inst Sci, Geophys Lab, 5251 Broad Branch Rd NW, Washington, DC 20015 USA. EM xliu@gl.ciw.edu OI Liu, Xiao-Ming/0000-0001-7904-1056 FU National Science Foundation [EAR 0948549]; University of Maryland; Carnegie Institution of Washington; U.S. Department of Energy, Geothermal Technologies Program, Energy Efficiency and Renewable Energy Office [GT-480010-12] FX We thank Richard Ash for assistance with the ICP-MS/MC-ICP-MS analyses, Igor Puchtel for help in the clean lab, Shuiwang Duan and Tammy Newcomer for major anion analyses, Terry Tolan for sampling guidance and discussion, Marshall Gannett, Steve Hinkle, Steve Cox, and Mike Free for help with fieldwork logistics, and Christie Galen for accompanying up in the field and showing us great birds. Sujay Kaushal kindly provided access to his Biogeochemistry laboratory and provided guidance on water sampling. We are grateful for discussions and comments from Jerome Gaillardet and Cin-Ty Lee. The manuscript benefited greatly from the review comments of three anonymous reviewers. Jean Lynch-Stieglitz is also thanked for her editorial handling and constructive comments. This work was supported by a grant from the National Science Foundation (EAR 0948549 to RLR and WFM) and an Ann G. Wylie Dissertation Fellowship awarded to X-ML from the University of Maryland. X-ML acknowledges postdoctoral fellowship support from the Carnegie Institution of Washington. CW was supported by the U.S. Department of Energy, Geothermal Technologies Program, Energy Efficiency and Renewable Energy Office, Award No GT-480010-12. NR 51 TC 12 Z9 12 U1 3 U2 29 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0012-821X EI 1385-013X J9 EARTH PLANET SC LETT JI Earth Planet. Sci. Lett. PD JAN 1 PY 2015 VL 409 BP 212 EP 224 DI 10.1016/j.epsl.2014.10.032 PG 13 WC Geochemistry & Geophysics SC Geochemistry & Geophysics GA AY7UF UT WOS:000347763500021 ER PT J AU Zhou, N He, G Williams, C Fridley, D AF Zhou, Nan He, Gang Williams, Christopher Fridley, David TI ELITE cities: A low-carbon eco-city evaluation tool for China SO ECOLOGICAL INDICATORS LA English DT Article DE Low-carbon eco-city; Indicator system; Tool; ELITE cities; China AB China is pursuing the development of low-carbon eco-cities to limit carbon dioxide and other greenhouse gases emissions; however, it is unclear what constitutes a low-carbon eco-city and how to evaluate it. The eco and low-carbon indicator tool for evaluating cities (ELITE cities) was developed by researchers at the Lawrence Berkeley National Laboratory in 2012 to evaluate cities' performance by comparing them against benchmark performance goals as well as rank them against other cities in China. ELITE cities measures progress on 33 key indicators selected to represent priority issues within eight primary categories. An excel-based tool was then developed to package the key indicators, indicator benchmarks, explanation of indicators, point calculation functions and transparency-oriented data recording instructions. ELITE cities could be a useful and effective tool for local city government in defining the broad outlines of a low-carbon eco-city and assessing the progress of cities' efforts towards this goal. ELITE cities can also be used by higher-level governments to assess city performance and discern best practices. This paper explains the general framework of the ELITE cities tool, the methods by which the indicators and indicator benchmarks were established, and a detailed guide on tool applications. (C) 2014 Elsevier Ltd. All rights reserved. C1 [Zhou, Nan; He, Gang; Williams, Christopher; Fridley, David] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Energy Anal & Environm Impacts Dept, Environm Energy Technol Div, Berkeley, CA 94720 USA. RP Zhou, N (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Energy Anal & Environm Impacts Dept, Environm Energy Technol Div, 1 Cyclotron Rd,MS 90R4000, Berkeley, CA 94720 USA. EM NZhou@lbl.gov RI He, Gang/N-4549-2013 OI He, Gang/0000-0002-8416-1965 FU U.S. Department of Energy [DE-AC02-05CH11231] FX This work was supported through the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. We appreciate the comments from the anonymous reviewer. The authors would like to thank Lixuan Hong, Qibo Liu, Brian Heimberg and Warren Karlenzig for their input and suggestions. NR 28 TC 13 Z9 15 U1 4 U2 26 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 1470-160X EI 1872-7034 J9 ECOL INDIC JI Ecol. Indic. PD JAN PY 2015 VL 48 BP 448 EP 456 DI 10.1016/j.ecolind.2014.09.018 PG 9 WC Biodiversity Conservation; Environmental Sciences SC Biodiversity & Conservation; Environmental Sciences & Ecology GA AY3PK UT WOS:000347495100048 ER PT J AU McManamay, RA Samu, N Kao, SC Bevelhimer, MS Hetrick, SC AF McManamay, Ryan A. Samu, Nicole Kao, Shih-Chieh Bevelhimer, Mark S. Hetrick, Shelaine C. TI A Multi-scale Spatial Approach to Address Environmental Effects of Small Hydropower Development SO ENVIRONMENTAL MANAGEMENT LA English DT Article DE Dams; Energy policy; Reserve design; Marxan; Landscape ecology ID LIFE-HISTORY STRATEGIES; SERIAL DISCONTINUITY CONCEPT; CONTERMINOUS UNITED-STATES; ALTERED FLOW REGIMES; FRESH-WATER FISHES; LANCANG RIVER; ECOLOGICAL CONSEQUENCES; POPULATION REGULATION; DAM CONSTRUCTION; LAND-USE AB Hydropower development continues to grow worldwide in developed and developing countries. While the ecological and physical responses to dam construction have been well documented, translating this information into planning for hydropower development is extremely difficult. Very few studies have conducted environmental assessments to guide site-specific or widespread hydropower development. Herein, we propose a spatial approach for estimating environmental effects of hydropower development at multiple scales, as opposed to individual site-by-site assessments (e.g., environmental impact assessment). Because the complex, process-driven effects of future hydropower development may be uncertain or, at best, limited by available information, we invested considerable effort in describing novel approaches to represent environmental concerns using spatial data and in developing the spatial footprint of hydropower infrastructure. We then use two case studies in the US, one at the scale of the conterminous US and another within two adjoining rivers basins, to examine how environmental concerns can be identified and related to areas of varying energy capacity. We use combinations of reserve-design planning and multi-metric ranking to visualize tradeoffs among environmental concerns and potential energy capacity. Spatial frameworks, like the one presented, are not meant to replace more in-depth environmental assessments, but to identify information gaps and measure the sustainability of multi-development scenarios as to inform policy decisions at the basin or national level. Most importantly, the approach should foster discussions among environmental scientists and stakeholders regarding solutions to optimize energy development and environmental sustainability. C1 [McManamay, Ryan A.; Samu, Nicole; Kao, Shih-Chieh; Bevelhimer, Mark S.; Hetrick, Shelaine C.] Oak Ridge Natl Lab, Div Environm Sci, Oak Ridge, TN 37831 USA. RP McManamay, RA (reprint author), Oak Ridge Natl Lab, Div Environm Sci, 1 Bethel Valley Rd,MS-6351,POB 2008, Oak Ridge, TN 37831 USA. EM mcmanamayra@ornl.gov RI Kao, Shih-Chieh/B-9428-2012 OI Kao, Shih-Chieh/0000-0002-3207-5328 FU US Department of Energy's (DOE) Office of Energy Efficiency and Renewable Energy, Wind and Water Power Technologies Program; US Department of Energy [DE-AC05-00OR22725] FX This research was sponsored by the US Department of Energy's (DOE) Office of Energy Efficiency and Renewable Energy, Wind and Water Power Technologies Program. This paper has been authored by employees of Oak Ridge National Laboratory, managed by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy. Accordingly, the publisher, by accepting the article for publication, acknowledges that the US Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript or allow others to do so, for US Government purposes. We thank Virginia Dale and three anonymous reviewers for providing comments on an earlier version of this manuscript. Special appreciation goes to Brenna Elrod for assisting with compiling ecological data and Fayzul Pasha, Dilruba Yeasmin, Abdoul A. Oubeidillah, Kevin M. Stewart, Yaxing Wei, and Boualem Hadjerioua for determining energy estimates for new development. Also, we thank Frankie Green, Joan Harn, Timothy McCune, Jim Parham, John Seebach, Jonathan Higgins, Mark Anderson, Mike Sale, Paul Jacobson, and Scott Robinson for providing reviews of methods and suggestions for data sources. Last, we thank Brennan Smith for leadership in the project and Hoyt Battey and TJ Heibel for support and project review. NR 119 TC 4 Z9 5 U1 6 U2 50 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 0364-152X EI 1432-1009 J9 ENVIRON MANAGE JI Environ. Manage. PD JAN PY 2015 VL 55 IS 1 BP 217 EP 243 DI 10.1007/s00267-014-0371-2 PG 27 WC Environmental Sciences SC Environmental Sciences & Ecology GA AY7BG UT WOS:000347715600017 PM 25223621 ER PT J AU Grippo, M Hayse, JW O'Connor, BL AF Grippo, Mark Hayse, John W. O'Connor, Ben L. TI Solar Energy Development and Aquatic Ecosystems in the Southwestern United States: Potential Impacts, Mitigation, and Research Needs SO ENVIRONMENTAL MANAGEMENT LA English DT Article DE Solar energy; Aquatic ecology; Renewable energy; Environmental impacts; Water use; Watershed management ID SAN-PEDRO RIVER; MOJAVE DESERT; ENVIRONMENTAL IMPACTS; RIPARIAN VEGETATION; ADAPTIVE MANAGEMENT; TEMPORAL PATTERNS; BIOTIC INTEGRITY; SEMIARID REGION; WATER RELATIONS; POWER-PLANTS AB The cumulative impacts of utility-scale solar energy facilities on aquatic ecosystems in the Southwestern United States are of concern, considering the many existing regional anthropogenic stressors. We review the potential impacts of solar energy development on aquatic habitat and biota. The greatest potential for impacts is related to the loss, fragmentation, or prolonged drying of ephemeral water bodies and drainage networks resulting from the loss of desert washes within the construction footprint of the facility. Groundwater-dependent aquatic habitat may also be affected by operational groundwater withdrawal in the case of water-intensive solar technologies. Solar panels have also been found to attract aquatic insects and waterbirds, potentially resulting in mortality. Avoiding construction activity near perennial and intermittent surface waters is the primary means of reducing impacts on aquatic habitats, followed by measures to minimize erosion, sedimentation, and contaminant inputs into waterways. Currently, significant data gaps make solar facility impact assessment and mitigation more difficult. Examples include the need for more regional and site-specific studies of surface-groundwater connectivity, more detailed maps of regional stream networks and riparian vegetation corridors, as well as surveys of the aquatic communities inhabiting ephemeral streams. In addition, because they often lack regulatory protection, there is also a need to develop valuation criteria for ephemeral waters based on their ecological and hydrologic function within the landscape. By addressing these research needs, we can achieve the goal of greater reliance on solar energy, while at the same time minimizing impacts on desert ecosystems. C1 [Grippo, Mark; Hayse, John W.] Argonne Natl Lab, Div Environm Sci, Argonne, IL 60439 USA. [O'Connor, Ben L.] Univ Illinois, Dept Civil & Mat Engn, Chicago, IL 60607 USA. RP Grippo, M (reprint author), Argonne Natl Lab, Div Environm Sci, 9700 S Cass Ave,Bldg 240, Argonne, IL 60439 USA. EM mgrippo@anl.gov FU U.S. Department of Energy [DE-AC02-06CH11357]; Bureau of Land Management (BLM), U.S. Department of the Interior (DOI) through U.S. Department of Energy [DE-AC02-06CH11357] FX Argonne National Laboratory's Work was supported by the U.S. Department of Energy, Assistant Secretary for the Office of Energy Efficiency and Renewable Energy (EERE) under contract DE-AC02-06CH11357, and the Bureau of Land Management (BLM), U.S. Department of the Interior (DOI), under interagency agreement, through U.S. Department of Energy contract DE-AC02-06CH11357. NR 92 TC 3 Z9 3 U1 10 U2 52 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 0364-152X EI 1432-1009 J9 ENVIRON MANAGE JI Environ. Manage. PD JAN PY 2015 VL 55 IS 1 BP 244 EP 256 DI 10.1007/s00267-014-0384-x PG 13 WC Environmental Sciences SC Environmental Sciences & Ecology GA AY7BG UT WOS:000347715600018 PM 25331641 ER PT J AU Alaba, OA Bredeson, JV Egesi, CN Esuma, W Ezenwaka, L Ferguson, ME Ha, CM Hall, M Herselman, L Ikpan, A Kafiriti, E Kanju, E Kapinga, F Karugu, A Kawuki, R Kimata, B Kimurto, P Kulakow, P Kulembeka, H Kusolwa, P Lyons, JB Masumba, E van de Merwe, A Mkamilo, G Myburg, AA Nwaogu, A Nzuki, I Olasanmi, B Okogbenin, E Onyegbule, O Owuoche, J Pariyo, A Prochnik, SE Rabbi, IY Rokhsar, DS Rounsley, S Salum, K Shuaibu, KS Sichalwe, C Stephen, M AF Alaba, Oluwafemi A. Bredeson, Jessen V. Egesi, Chiedozie N. Esuma, Williams Ezenwaka, Lydia Ferguson, Morag E. Ha, Cindy M. Hall, Megan Herselman, Liezel Ikpan, Andrew Kafiriti, Elly Kanju, Edward Kapinga, Fortunus Karugu, Arthur Kawuki, Robert Kimata, Bernadetha Kimurto, Paul Kulakow, Peter Kulembeka, Heneriko Kusolwa, Paul Lyons, Jessica B. Masumba, Esther van de Merwe, Albe Mkamilo, Geoffrey Myburg, Alexander A. Nwaogu, Ahamefule Nzuki, Inosters Olasanmi, Bunmi Okogbenin, Emmanuel Onyegbule, Onyeyirichi Owuoche, James Pariyo, Anthony Prochnik, Simon E. Rabbi, Ismail Y. Rokhsar, Daniel S. Rounsley, Steve Salum, Kasele Shuaibu, Kahya S. Sichalwe, Caroline Stephen, Mary CA ICGMC TI High-Resolution Linkage Map and Chromosome-Scale Genome Assembly for Cassava (Manihot esculenta Crantz) from 10 Populations SO G3-GENES GENOMES GENETICS LA English DT Article DE genotyping-by-sequencing; SNP; composite genetic map; pseudomolecules; F1 cross ID MOLECULAR-GENETIC MAP; MARKERS; SNP; ASSOCIATION; DIVERSITY; DISCOVERY AB Cassava (Manihot esculenta Crantz) is a major staple crop in Africa, Asia, and South America, and its starchy roots provide nourishment for 800 million people worldwide. Although native to South America, cassava was brought to Africa 400-500 years ago and is now widely cultivated across sub-Saharan Africa, but it is subject to biotic and abiotic stresses. To assist in the rapid identification of markers for pathogen resistance and crop traits, and to accelerate breeding programs, we generated a framework map for M. esculenta Crantz from reduced representation sequencing [genotyping-by-sequencing (GBS)]. The composite 2412-cM map integrates 10 biparental maps (comprising 3480 meioses) and organizes 22,403 genetic markers on 18 chromosomes, in agreement with the observed karyotype. We used the map to anchor 71.9% of the draft genome assembly and 90.7% of the predicted protein-coding genes. The chromosome-anchored genome sequence will be useful for breeding improvement by assisting in the rapid identification of markers linked to important traits, and in providing a framework for genomic selection-enhanced breeding of this important crop. C1 [Alaba, Oluwafemi A.; Ferguson, Morag E.] IITA, Ibadan, Oyo State, Nigeria. [Bredeson, Jessen V.; Ha, Cindy M.; Hall, Megan; Lyons, Jessica B.; Rokhsar, Daniel S.] Univ Calif Berkeley, Dept Mol & Cell Biol, Berkeley, CA 94720 USA. [Egesi, Chiedozie N.; Ezenwaka, Lydia; Nwaogu, Ahamefule; Okogbenin, Emmanuel; Shuaibu, Kahya S.] NRCRI, Umudike, Nigeria. [Esuma, Williams; Kawuki, Robert; Pariyo, Anthony] Natl Crops Resources Res Inst NaCCRI, Namulonge, Uganda. [Ikpan, Andrew; Kulakow, Peter; Rabbi, Ismail Y.] IITA Nigeria, Ibadan, Oyo State, Nigeria. [Herselman, Liezel] Univ Free State, Dept Plant Sci, Bloemfontein, South Africa. [Kafiriti, Elly; Kimata, Bernadetha] Naliendele Agr Res Inst, Mtwara, Tanzania. [Kanju, Edward] IITA Mikocheni, Dar Es Salaam, Tanzania. [Kapinga, Fortunus] Naliendele Agr Res Inst, Mtwara, Tanzania. [Kimurto, Paul] Egerton Univ, Njoro, Kenya. [Kulembeka, Heneriko] Lake Zonal Agr Res & Dev Inst, Mwanza, Tanzania. [Kusolwa, Paul] Sokoine Univ, Morogoro, Tanzania. [Masumba, Esther; Sichalwe, Caroline] Sugarcane Agr Res Inst, Kibaha, Tanzania. [van de Merwe, Albe; Nzuki, Inosters] Univ Pretoria, Dept Genet, ZA-0002 Pretoria, South Africa. [Mkamilo, Geoffrey] Naliendele Agr Res Inst ARI, Mtwara, Tanzania. [Mkamilo, Geoffrey] ARI, Roots & Tuber Crops Program, New Delhi, India. [Myburg, Alexander A.] Univ Pretoria, Dept Genet Forestry & Biotechnol, ZA-0002 Pretoria, South Africa. [Nzuki, Inosters] Biosci Eastern & Cent Africa BecA, Nairobi 30709001, Kenya. [Olasanmi, Bunmi] Univ Ibadan, Ibadan, Nigeria. [Owuoche, James] Egerton Univ, Njoro, Kenya. [Prochnik, Simon E.; Rokhsar, Daniel S.] Joint Genome Inst, Dept Energy, Walnut Creek, CA USA. [Rounsley, Steve] Univ Arizona, Tucson, AZ USA. [Rounsley, Steve] Dow Agrosci, Indianapolis, IN USA. [Salum, Kasele] Lake Zonal Agr Res & Dev Inst, Mwanza, Tanzania. [Stephen, Mary] Makutupora Agr Res Stn, Dodoma, Tanzania. RP Lyons, JB (reprint author), Univ Calif Berkeley, Dept Mol & Cell Biol, Berkeley, CA 94720 USA. EM O.Alaba@cgiar.org; jessenbredeson@berkeley.edu; cegesi@yahoo.com; esumawilliams@yahoo.co.uk; lydiaezenwaka@yahoo.com; M.Ferguson@cgiar.org; cindy.ha@ucdenver.edu; mhall45@gmail.com; HerselmanL@ufs.ac.za; A.Ikpan@cgiar.org; ekafiriti@gmail.com; e.kanju@cgiar.org; fakapinga@yahoo.com; a.karugu@cgiar.org; kawukisezi@yahoo.com; bkimatha@yahoo.co.uk; kimurtopk@gmail.com; P.Kulakow@cgiar.org; kulembeka@yahoo.com; kusolwap@gmail.com; jblyons@berkeley.edu; emasumba@yahoo.com; albe.vdMerwe@up.ac.za; geoffreymkamilo@yahoo.co.uk; zander.myburg@fabi.up.ac.za; ahamefulenwaogu@yahoo.com; i.nzuki@cgiar.org; bunminadeco@yahoo.com; eokogbenin@cassavacop.org; princessonyin@yahoo.com; owuoche@hotmail.com; tkakau@yahoo.co.uk; seprochnik@lbl.gov; I.RAB-BI@cgiar.org; dsrokhsar@gmail.com; rounsley@email.arizona.edu; kasele_salum@yahoo.com; kahyass@yahoo.com; carosicha@gmail.com; marystephen49@yahoo.com RI Myburg, Alexander/C-5426-2008 OI Myburg, Alexander/0000-0003-0644-5003 FU Bill and Melinda Gates Foundation (BMGF) [OPPGD1493]; CGIAR Research Program on Roots, Tubers, and Bananas; BMGF [OPP1048542, OPPGD1016]; United Kingdom Department for International Development; Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]; National Institutes of Health [S10RR029668, S10RR027303] FX The authors thank Richard Harland and Lisa Brunet for early input into optimization of the GBS protocol; Craig Miller lab/Andrew Glazer for reagents and helpful discussion; Minyong Chung, Justin Choi, Karen Lundy, and other members of the VCGSL at UC Berkeley for advice and technical assistance with sequencing; Jeff Endelman for advice on using LPmerge; and Ed Buckler, Jean-Luc Jannink, and Martha Hamblin, for helpful discussion. J.B.L., J.V.B., C.M.H., and work at UC Berkeley were funded by Bill and Melinda Gates Foundation (BMGF) Grant OPPGD1493 to S.R., D.S.R., and the University of Arizona. Development of populations at IITA Ibadan was funded by the CGIAR Research Program on Roots, Tubers, and Bananas. Next Generation Cassava Breeding grant OPP1048542 from BMGF and the United Kingdom Department for International Development supported S.E.P. and work at NRCRI and IITA. Development of the mapping populations in Tanzania was funded by BMGF grant OPPGD1016 to IITA. The work conducted by the U.S. Department of Energy Joint Genome Institute is supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. This work used the VCGSL at UC Berkeley, supported by National Institutes of Health S10 Instrumentation Grants S10RR029668 and S10RR027303. NR 34 TC 7 Z9 7 U1 6 U2 30 PU GENETICS SOCIETY AMERICA PI BETHESDA PA 9650 ROCKVILLE AVE, BETHESDA, MD 20814 USA SN 2160-1836 J9 G3-GENES GENOM GENET JI G3-Genes Genomes Genet. PD JAN 1 PY 2015 VL 5 IS 1 BP 133 EP 144 DI 10.1534/g3.114.015008 PG 12 WC Genetics & Heredity SC Genetics & Heredity GA AY8TP UT WOS:000347826600014 ER PT J AU Turchi, PJ AF Turchi, Peter J. TI Fusion Rocket Based on Stabilized Liner Implosions SO IEEE TRANSACTIONS ON PLASMA SCIENCE LA English DT Article; Proceedings Paper CT 33rd International Electric Propulsion Conference (IEPC 2013) CY OCT 06-10, 2013 CL George Washington Univ, Washington, DC HO George Washington Univ DE Fusion propulsion; imploding liners; megagauss ID OPERATION AB Examination continues in detail for the use of controlled fusion for high-energy, crewed-missions to the outer planets at significant continual acceleration (>0.01g(0)). Transit times to Jupiter measured in a few months, delivering 200 t of payload, appear possible, but require the use of advanced fuels, e.g., D-He-3, to reduce the excessive burden of radiator mass needed to process the heat of fusion neutrons. Such advanced reactions, however, need plasma temperatures in excess of 100 keV, so adiabatic compression is invoked to match the desired final state to much more modest initial temperature values. This compression would be achieved by stabilized implosion of liquid metal liners, as demonstrated decades ago in the Linus program at the Naval Research Laboratory. Distinctions are drawn between the present propulsion design options and the earlier Linus fusion power reactor based on D-T fuel. C1 Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Turchi, PJ (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM nmturchi1@aol.com NR 15 TC 1 Z9 1 U1 1 U2 5 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 0093-3813 EI 1939-9375 J9 IEEE T PLASMA SCI JI IEEE Trans. Plasma Sci. PD JAN PY 2015 VL 43 IS 1 BP 240 EP 243 DI 10.1109/TPS.2014.2309633 PN 1 PG 4 WC Physics, Fluids & Plasmas SC Physics GA AY8ED UT WOS:000347786300029 ER PT J AU Little, JM Choueiri, EY AF Little, Justin M. Choueiri, Edgar Y. TI Critical Condition for Plasma Confinement in the Source of a Magnetic Nozzle Flow SO IEEE TRANSACTIONS ON PLASMA SCIENCE LA English DT Article; Proceedings Paper CT 33rd International Electric Propulsion Conference (IEPC 2013) CY OCT 06-10, 2013 CL George Washington Univ, Washington, DC HO George Washington Univ DE Cross-field diffusion; helicon plasma; magnetic nozzle (MN); radio-frequency (RF) plasma ID HELICON; FREQUENCY; THRUSTER; PERFORMANCE AB The existence of a theoretically predicted critical magnetic field strength for efficient plasma confinement in helicon plasma thrusters is verified experimentally in the source of a magnetic nozzle (MN) flow. Control of the plasma confinement is crucial for enhancing the mass utilization efficiency of electric propulsion systems that employ MNs. Langmuir probe measurements of the density at the MN throat of a helicon plasma thruster as a function of the applied magnetic field strength indicate a transition from a low-confinement operation mode, in which a majority of the plasma diffuses to the solid walls of the plasma source before emerging from the thruster, to a high-confinement operation mode, in which the plasma preferentially exhausts downstream through the MN. This transition is shown to be governed by the anisotropic Peclet number, Pe(an), which is defined as the ratio of the advective (field aligned) to diffusive (cross field) mass transport rates. Experimental estimations of the mass utilization efficiency of the plasma source for various magnetic field strengths and plasma source lengths are shown to support an analytically derived scaling law, and suggest Pe(an) >> 1 as a design criterion for MN plasma sources. C1 [Little, Justin M.; Choueiri, Edgar Y.] Princeton Univ, Elect Prop & Plasma Dynam Lab, Princeton, NJ 08540 USA. RP Little, JM (reprint author), Princeton Univ, Elect Prop & Plasma Dynam Lab, Princeton, NJ 08540 USA. EM jml@princeton.edu; choueiri@princeton.edu FU Department of Defense through the National Defense Science and Engineering Graduate Fellowship Program; Program in Plasma Science and Technology through DOE [DE-AC02-09CH11466] FX The work of J. M. Little was supported in part by the Department of Defense through the National Defense Science and Engineering Graduate Fellowship Program and in part by the Program in Plasma Science and Technology through DOE under Contract DE-AC02-09CH11466. NR 50 TC 4 Z9 4 U1 3 U2 13 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 0093-3813 EI 1939-9375 J9 IEEE T PLASMA SCI JI IEEE Trans. Plasma Sci. PD JAN PY 2015 VL 43 IS 1 BP 277 EP 286 DI 10.1109/TPS.2014.2322522 PN 1 PG 10 WC Physics, Fluids & Plasmas SC Physics GA AY8ED UT WOS:000347786300033 ER PT J AU Domonkos, MT Struve, KW AF Domonkos, Matthew T. Struve, Kenneth W. TI Guest Editorial Introduction to the Special Issue on Megagauss Magnetic Fields: Production & Application SO IEEE TRANSACTIONS ON PLASMA SCIENCE LA English DT Editorial Material C1 [Domonkos, Matthew T.] Air Force Res Lab, Kirtland AFB, NM 87117 USA. [Struve, Kenneth W.] Sandia Natl Labs, Albuquerque, NM 87123 USA. RP Domonkos, MT (reprint author), Air Force Res Lab, Kirtland AFB, NM 87117 USA. NR 0 TC 0 Z9 0 U1 2 U2 2 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 0093-3813 EI 1939-9375 J9 IEEE T PLASMA SCI JI IEEE Trans. Plasma Sci. PD JAN PY 2015 VL 43 IS 1 BP 333 EP 334 DI 10.1109/TPS.2014.2378532 PN 2 PG 2 WC Physics, Fluids & Plasmas SC Physics GA AY8EL UT WOS:000347787100001 ER PT J AU Turchi, PJ AF Turchi, Peter J. TI Compact Transformer Drive for High-Current Applications SO IEEE TRANSACTIONS ON PLASMA SCIENCE LA English DT Article DE Megampere; pulsed power; transformer ID PLASMA-FLOW SWITCH AB The approach called precision high energy-density liner implosion experiment (PHELIX) provides a technique to allow research on high energy-density phenomena associated with liner implosions in a scaled-down system suitable for use with proton radiography. It has been noted that the ratio of load current to bank energy is almost an order of magnitude higher using the PHELIX transformer technique than achievable with direct drive from high-energy capacitor banks. This increase in current per stored-joule offers the opportunity for using similar transformer arrangements for other applications apart from imploding liners. These potential applications include rail-guns and the dense plasma focus. Results from the dimensionless analyses previously used successfully to design PHELIX will be described for these new applications and design limitations will be discussed. C1 [Turchi, Peter J.] Air Force Weap Lab, Albuquerque, NM USA. [Turchi, Peter J.] Naval Res Lab, Plasma Technol Branch, Washington, DC USA. [Turchi, Peter J.] R&D Associates Inc, Washington Res Lab, Alexandria, VA USA. [Turchi, Peter J.] Ohio State Univ, Columbus, OH 43210 USA. [Turchi, Peter J.] Los Alamos Natl Lab, Los Alamos, NM USA. [Turchi, Peter J.] Amer Inst Aeronaut & Astronaut, Reston, VA 20191 USA. RP Turchi, PJ (reprint author), Amer Inst Aeronaut & Astronaut, Reston, VA 20191 USA. EM nmturchi1@aol.com NR 14 TC 0 Z9 0 U1 1 U2 4 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 0093-3813 EI 1939-9375 J9 IEEE T PLASMA SCI JI IEEE Trans. Plasma Sci. PD JAN PY 2015 VL 43 IS 1 BP 335 EP 338 DI 10.1109/TPS.2014.2375312 PN 2 PG 4 WC Physics, Fluids & Plasmas SC Physics GA AY8EL UT WOS:000347787100002 ER PT J AU Turchi, PJ AF Turchi, Peter J. TI Liner Stability Problems for Megagauss Fusion SO IEEE TRANSACTIONS ON PLASMA SCIENCE LA English DT Article DE Fusion; imploding liners; megagauss ID COMPRESSION AB Megagauss fields obtained by liner implosion may offer controlled fusion at much lower cost, size, and entry power levels than conventional fusion schemes. Such implosions are subject to elastic-plastic instability (for solid-density liners) and Rayleigh-Taylor instability in fluid liners (liquid or plasma). This paper provides budgets on allowable perturbations for the inner surface of the liner to offer a simple guide for researchers. C1 [Turchi, Peter J.] Air Force Weap Lab, Albuquerque, NM USA. [Turchi, Peter J.] Naval Res Lab, Plasma Technol Branch, Washington, DC USA. [Turchi, Peter J.] R&D Associates Inc, Washington Res Lab, Alexandria, VA USA. [Turchi, Peter J.] Ohio State Univ, Columbus, OH 43210 USA. [Turchi, Peter J.] Los Alamos Natl Lab, Los Alamos, NM USA. [Turchi, Peter J.] Amer Inst Aeronaut & Astronaut, Reston, VA 20191 USA. RP Turchi, PJ (reprint author), Amer Inst Aeronaut & Astronaut, Reston, VA 20191 USA. EM nmturchi1@aol.com NR 9 TC 1 Z9 1 U1 1 U2 1 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 0093-3813 EI 1939-9375 J9 IEEE T PLASMA SCI JI IEEE Trans. Plasma Sci. PD JAN PY 2015 VL 43 IS 1 BP 369 EP 373 DI 10.1109/TPS.2014.2375315 PN 2 PG 5 WC Physics, Fluids & Plasmas SC Physics GA AY8EL UT WOS:000347787100009 ER PT J AU Domonkos, MT Degnan, JH Adamson, PE Amdahl, DJ Blasy, B Cooksey, R Grabowski, TC Lehr, FM Robinson, PR Ruden, EL White, WM Frese, MH Frese, SD Coffey, SK Camacho, JF Makhin, V Roderick, N Parker, JV Lerma, A Gale, D Kostora, M McCullough, J Ralph, D Roth, CE Sommars, WE Montoya, T Lynn, AG Turchi, PJ Schroen, D AF Domonkos, Matthew T. Degnan, James H. Adamson, Paul E. Amdahl, David J. Blasy, Brian Cooksey, Rufus Grabowski, Theodore Chris Lehr, Frederick Mark Robinson, Paul Randy Ruden, Edward L. White, William M. Frese, Michael H. Frese, Sherry D. Coffey, Sean K. Camacho, J. Frank Makhin, Vladimir Roderick, Norman Parker, Jerald V. Lerma, Al Gale, Donald Kostora, Mark McCullough, John Ralph, Dale Roth, Chris E. Sommars, Wayne E. Montoya, Thomas Lynn, Alan G. Turchi, Peter J. Schroen, Diana TI Experimental Studies of an Ultrahigh-Speed Plasma Flow SO IEEE TRANSACTIONS ON PLASMA SCIENCE LA English DT Article DE Controlled fusion; imploding liners; magnetized lasma compression; pulsed power ID SWITCH AB In 1991, Turchi et al. reported evidence for a 2000 km/s aluminum plasma that originated from the upstream boundary of a wire array armature in a plasma flow switch (PFS). The 2008 article by Turchi et al. posits that if such high Z plasma could instead be composed of deuterium or a deuterium-tritium mixture, then the resultant multi-keV plasma would make an effective target for magnetized plasma compression to fusion conditions. This report documents several experiments executed in an effort to achieve an ultrahigh-speed flow in a deuterium plasma. The first phase of this research concentrated on extension of the earlier work to a lower current system that would emulate the PFS used in series with an imploding liner load. The apparatus was also modified to permit pulsed injection of deuterium gas along the insulated coaxial electrodes between the PFS armature and the vacuum power feed. The experiments met with limited success, exhibiting evidence of a 550 km/s plasma flow which convected a small fraction of the total magnetic field. Two subsequent tests were conducted using foam armatures. In both cases, current prematurely shunted upstream in the vacuum feed. Several possible causes were explored for the shunting of the current. Among the modifications implemented, the gas injection system was altered to increase both the quantity of gas adjacent to the armature while facilitating an increased pressure gradient between the armature and the current feed. A series of low-energy shots were conducted to examine the impact of several proposed design modifications on current delivery to the armature. These experiments demonstrated that the hardware assembled for this investigation was unlikely to forestall breakdown in the injected gas as required by Turchi et al. Nevertheless, two experiments were conducted to evaluate performance with foam armatures. Both experiments exhibited good current delivery to the armature, behaving initially like the low-energy experiments. The magnetic flux convected downstream was greater than in any of the prior experiments, though significant work remains to demonstrate the ultrahigh-speed plasma flow concept. C1 [Domonkos, Matthew T.; Degnan, James H.; Adamson, Paul E.; Amdahl, David J.; Blasy, Brian; Cooksey, Rufus; Grabowski, Theodore Chris; Lehr, Frederick Mark; Robinson, Paul Randy; Ruden, Edward L.; White, William M.] Air Force Res Lab, Kirtland AFB, NM 87117 USA. [Frese, Michael H.; Frese, Sherry D.; Coffey, Sean K.; Camacho, J. Frank; Makhin, Vladimir; Roderick, Norman] NumerEx LLC, Albuquerque, NM 87106 USA. [Parker, Jerald V.; Lerma, Al; Gale, Donald; Kostora, Mark; McCullough, John; Ralph, Dale; Roth, Chris E.; Sommars, Wayne E.] SAIC, Albuquerque, NM 87106 USA. [Montoya, Thomas] Voss Sci, Albuquerque, NM 87108 USA. [Lynn, Alan G.] Univ New Mexico, Dept Elect & Comp Engn, Albuquerque, NM 87131 USA. [Turchi, Peter J.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Schroen, Diana] Gen Atom Co, Albuquerque, NM 87123 USA. RP Domonkos, MT (reprint author), Air Force Res Lab, Kirtland AFB, NM 87117 USA. EM matthew.domonkos@us.af.mil; james.degnan.2@us.af.mil; paul.adamson.1@us.af.mil; david.amdahl.1@us.af.mil; bryan.blasy@us.af.mil; rufus.cooksey.1@us.af.mil; theodore.grabowski.2@us.af.mil; frederick.lehr@us.af.mil; paul.robinson.13@us.af.mil; edward.ruden@us.af.mil; william.white.48@us.af.mil; michael.frese@numerex-llc.com; sherry.frese@numerex-llc.com; scoffey1357@msn.com; j.camacho.ctr@us.af.mil; vmakhin@techflow.com; nfroder2@comcast.net; jerald.parker.ctr@us.af.mil; albert.lerma.ctr@us.af.mil; donco735@hotmail.com; mark.kostora.ctr@kirtland.af.mil; john.mccullough.8.ctr@us.af.mil; dale.ralph.ctr@kirtland.af.mil; chris.roth.ctr@us.af.mil; wayne.sommars.ctr@us.af.mil; thomas.montoya.ctr@kirtland.af.mil; lynn@ece.unm.edu; nmturchi1@aol.com; dgschro@sandia.gov NR 11 TC 0 Z9 0 U1 0 U2 0 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 0093-3813 EI 1939-9375 J9 IEEE T PLASMA SCI JI IEEE Trans. Plasma Sci. PD JAN PY 2015 VL 43 IS 1 BP 374 EP 388 DI 10.1109/TPS.2014.2360648 PN 2 PG 15 WC Physics, Fluids & Plasmas SC Physics GA AY8EL UT WOS:000347787100010 ER PT J AU Gandavarapu, S Sabolsky, E Sabolsky, K Gerdes, K AF Gandavarapu, Sodith Sabolsky, Edward Sabolsky, Katarzyna Gerdes, Kirk TI In Situ Foaming of Porous (La0.6Sr0.4)(0.98) (Co-0.2 Fe-0.8) O3-delta (LSCF) Cathodes for Solid Oxide Fuel Cell Applications SO INTERNATIONAL JOURNAL OF APPLIED CERAMIC TECHNOLOGY LA English DT Article ID SOFC; ANODE; MICROSTRUCTURE; RESISTANCE; CERMET AB A binder system containing polyurethane precursors was used to in situ foam (direct foam) a (La0.6Sr0.4)(0.98) (Co-0.2 Fe-0.8) O3-delta (LSCF) composition for solid oxide fuel cell (SOFC) cathode applications. The relation between in situ foaming parameters on the final microstructure and electrochemical properties was characterized by microscopy and electrochemical impedance spectroscopy (EIS), respectively. The optimal porous cathode architecture was formed with a 70 vol% solids loading within a polymer precursor composition with a volume ratio of 8:4:1 (isocyanate: PEG: surfactant) in a terpineol-based ink vehicle. The resultant microstructure displayed a broad pore size distribution with highly elongated pore structure. C1 [Gandavarapu, Sodith; Sabolsky, Edward; Gerdes, Kirk] US DOE, Natl Energy Technol Lab, Morgantown, WV 26507 USA. [Gandavarapu, Sodith; Sabolsky, Edward; Sabolsky, Katarzyna] W Virginia Univ, Dept Mech & Aerosp Engn, Morgantown, WV 26506 USA. RP Gandavarapu, S (reprint author), US DOE, Natl Energy Technol Lab, 3610 Collins Ferry Rd,POB 880, Morgantown, WV 26507 USA. EM ed.sabolsky@mail.wvu.edu FU RES [DE-FE0004000]; Department of Energy, National Energy Technology Laboratory, an agency of the United States Government; URS Energy & Construction, Inc. FX As part of the National Energy Technology Laboratory's Regional University Alliance (NETL-RUA), a collaborative initiative of the NETL, this technical effort was performed under the RES contract DE-FE0004000. This project was funded by the Department of Energy, National Energy Technology Laboratory, an agency of the United States Government, through a support contract with URS Energy & Construction, Inc. Neither the United States Government nor any agency thereof, nor any of their employees, nor URS Energy & Construction, Inc., nor any of their employees, makes any warranty, expressed or implied, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. Reference herein to any specific commercial product, process, or service by trade name, trademark, manufacturer, or otherwise, does not necessarily constitute or imply its endorsement, recommendation, or favoring by the United States Government or any agency thereof. The views and opinions of authors expressed herein do not necessarily state or reflect those of the United States Government or any agency thereof. NR 24 TC 0 Z9 0 U1 1 U2 20 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 1546-542X EI 1744-7402 J9 INT J APPL CERAM TEC JI Int. J. Appl. Ceram. Technol. PD JAN-FEB PY 2015 VL 12 IS 1 BP 199 EP 211 DI 10.1111/ijac.12142 PG 13 WC Materials Science, Ceramics SC Materials Science GA AY7BR UT WOS:000347716800024 ER PT J AU Zilla, ML Chan, YGY Lunderberg, JM Schneewind, O Missiakas, D AF Zilla, Megan Liszewski Chan, Yvonne G. Y. Lunderberg, Justin Mark Schneewind, Olaf Missiakas, Dominique TI LytR-CpsA-Psr Enzymes as Determinants of Bacillus anthracis Secondary Cell Wall Polysaccharide Assembly SO JOURNAL OF BACTERIOLOGY LA English DT Article ID RIBITOL TEICHOIC-ACIDS; S-LAYER PROTEINS; STAPHYLOCOCCUS-AUREUS; CAPSULAR POLYSACCHARIDE; STREPTOCOCCUS-PNEUMONIAE; STRUCTURAL-ANALYSIS; FUNCTIONAL-ANALYSIS; CHAIN-LENGTH; SURFACE; SUBTILIS AB Bacillus anthracis, the causative agent of anthrax, replicates as chains of vegetative cells by regulating the separation of septal peptidoglycan. Surface (S)-layer proteins and associated proteins (BSLs) function as chain length determinants and bind to the secondary cell wall polysaccharide (SCWP). In this study, we identified the B. anthracis lcpD mutant, which displays increased chain length and S-layer assembly defects due to diminished SCWP attachment to peptidoglycan. In contrast, the B. anthracis lcpB3 variant displayed reduced cell size and chain length, which could be attributed to increased deposition of BSLs. In other bacteria, LytR-CpsA-Psr (LCP) proteins attach wall teichoic acid (WTA) and polysaccharide capsule to peptidoglycan. B. anthracis does not synthesize these polymers, yet its genome encodes six LCP homologues, which, when expressed in S. aureus, promote WTA attachment. We propose a model whereby B. anthracis LCPs promote attachment of SCWP precursors to discrete locations in the peptidoglycan, enabling BSL assembly and regulated separation of septal peptidoglycan. C1 [Zilla, Megan Liszewski; Lunderberg, Justin Mark; Schneewind, Olaf; Missiakas, Dominique] Argonne Natl Lab, Howard Taylor Ricketts Lab, Lemont, IL USA. [Zilla, Megan Liszewski; Chan, Yvonne G. Y.; Lunderberg, Justin Mark; Schneewind, Olaf; Missiakas, Dominique] Univ Chicago, Dept Microbiol, Chicago, IL 60637 USA. RP Missiakas, D (reprint author), Argonne Natl Lab, Howard Taylor Ricketts Lab, Lemont, IL USA. EM dmissiak@bsd.uchicago.edu FU National Institutes of Health (NIH) [GM07281]; NIH Ruth L. Kirschstein National Research Service award [1F30AI110036-01]; American Heart Association [13POST16980091]; National Institute of Allergy and Infectious Diseases, Infectious Disease Branch [AI069227] FX M.L.Z. and J.M.L. are trainees of the Medical Scientist Training Program at the University of Chicago and are supported by a National Institutes of Health (NIH) training grant (GM07281). J.M.L. is the recipient of NIH Ruth L. Kirschstein National Research Service award 1F30AI110036-01. Y.G.Y.C. is the recipient of American Heart Association award 13POST16980091. This research was supported by grant AI069227 from the National Institute of Allergy and Infectious Diseases, Infectious Disease Branch (to O.S. and D. M.). NR 58 TC 9 Z9 9 U1 0 U2 10 PU AMER SOC MICROBIOLOGY PI WASHINGTON PA 1752 N ST NW, WASHINGTON, DC 20036-2904 USA SN 0021-9193 EI 1098-5530 J9 J BACTERIOL JI J. Bacteriol. PD JAN PY 2015 VL 197 IS 2 BP 343 EP 353 DI 10.1128/JB.02364-14 PG 11 WC Microbiology SC Microbiology GA AY6KX UT WOS:000347676200011 ER PT J AU Xu, C Kaplan, DI Zhang, SJ Athon, M Ho, YF Li, HP Yeager, CM Schwehr, KA Grandbois, R Wellman, D Santschi, PH AF Xu, Chen Kaplan, Daniel I. Zhang, Saijin Athon, Matthew Ho, Yi-Fang Li, Hsiu-Ping Yeager, Chris M. Schwehr, Kathleen A. Grandbois, Russell Wellman, Dawn Santschi, Peter H. TI Radioiodine sorption/desorption and speciation transformation by subsurface sediments from the Hanford Site SO JOURNAL OF ENVIRONMENTAL RADIOACTIVITY LA English DT Article DE Iodine; Iodate; Iodide; Organic carbon; Sorption ID NATURAL ORGANIC-MATTER; SAVANNA RIVER SITE; MOLECULAR ENVIRONMENT; MASS-SPECTROMETRY; CHINESE SOILS; TRACE-METALS; IODINE; I-129; IODATE; GROUNDWATER AB During the last few decades, considerable research efforts have been extended to identify more effective remediation treatment technologies to lower the I-129 concentrations to below federal drinking water standards at the Hanford Site (Richland, USA). Few studies have taken iodate into consideration, though recently iodate, instead of iodide, was identified as the major species in the groundwater of 200-West Area within the Hanford Site. The objective of this study was thus to quantify and understand aqueous radioiodine species transformations and uptake by three sediments collected from the semi-arid, carbonate-rich environment of the Hanford subsurface. All three sediments reduced iodate (IO3-) to iodide (I-), but the loamy-sand sediment reduced more IO3- (100% reduced within 7 days) than the two sand-textured sediments (20% reduced after 28 days). No dissolved organo-iodine species were observed in any of these studies. Iodate uptake K-d values ([I-solid]/[I-aq]; 0.8-7.6 L/kg) were consistently and appreciably greater than iodide K-d values (0-5.6 L/kg). Furthermore, desorption K-d values (11.9-29.8 L/kg) for both iodate and iodide were consistently and appreciably greater than uptake K-d values (0-7.6 L/kg). Major fractions of iodine associated with the sediments were unexpectedly strongly bound, such that only 0.4-6.6 % of the total sedimentary iodine could be exchanged from the surface with KCl solution, and 0-1.2% was associated with Fe or Mn oxides (weak NH2HCl/HNO3 extractable fraction). Iodine incorporated into calcite accounted for 2.9-39.4% of the total sedimentary iodine, whereas organic carbon (OC) is likely responsible for the residual iodine (57.1-90.6%) in sediments. The OC, even at low concentrations, appeared to be controlling iodine binding to the sediments, as it was found that the greater the OC concentrations in the sediments, the greater the values of uptake K-d, desorption K-d, and the greater residual iodine concentrations (non-exchangeable, non-calcite-incorporated and non-Mn, Fe-oxide associated). This finding is of particular interest because it suggests that even very low OC concentrations, <0.2%, may have an impact on iodine geochemistry. The findings that these sediments can readily reduce IO3,- and that IO3- sorbs to a greater extent than I-, sheds light into earlier unexplained Hanford field data that demonstrated increases in groundwater I-127(-)/(IO3-)-I-127 ratios and a decrease groundwater (IO3-)-I-129 concentrations along a transect away from the point sources, where iodine was primarily introduced as IO3-. While a majority of the radioiodine does not bind to these alkaline sediments, there is likely a second smaller iodine fraction in the Hanford subsurface that is strongly bound, presumably to the sediment OC (and carbonate) phases. This second fraction may have an impact on establishing remediation goals and performance assessment calculations. (C) 2014 Elsevier Ltd. All rights reserved. C1 [Xu, Chen; Zhang, Saijin; Athon, Matthew; Ho, Yi-Fang; Li, Hsiu-Ping; Schwehr, Kathleen A.; Grandbois, Russell; Santschi, Peter H.] Texas A&M Univ, Dept Marine Sci, Lab Environm & Oceanog Res, Galveston, TX 77551 USA. [Kaplan, Daniel I.] Savannah River Natl Lab, Aiken, SC 29808 USA. [Wellman, Dawn] Pacific NW Natl Lab, Richland, WA 99354 USA. RP Xu, C (reprint author), Texas A&M Univ, Dept Marine Sci, Lab Environm & Oceanog Res, Bldg 3029, Galveston, TX 77551 USA. EM xuchen66@tamu.edu FU U.S. Department of Energy (DOE) Richland Operations Office; DOE's Office of Science - Subsurface Biogeochemistry Research program [ER65222-1038426-0017532]; DOE's Site Restoration program; Welch Grant [BD0046]; NSF-REU programs; DOE [DE-AD09-96SR18500] FX This work was funded by the U.S. Department of Energy (DOE) Richland Operations Office to the Deep Vadose Zone - Applied Field Research Initiative at Pacific Northwest National Laboratory, DOE's Office of Science - Subsurface Biogeochemistry Research program (Grant No.: ER65222-1038426-0017532), and the DOE's Site Restoration program. Matthew Athon was partially funded by a Welch Grant BD0046 and the NSF-REU programs. Work at the Savannah River National Laboratory was conducted under DOE contract DE-AD09-96SR18500. We greatly thank the two anonymous reviewers and the associate editor for their constructive comments and suggestion. NR 51 TC 6 Z9 6 U1 6 U2 36 PU ELSEVIER SCI LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, OXON, ENGLAND SN 0265-931X EI 1879-1700 J9 J ENVIRON RADIOACTIV JI J. Environ. Radioact. PD JAN PY 2015 VL 139 SI SI BP 43 EP 55 DI 10.1016/j.jenvrad.2014.09.012 PG 13 WC Environmental Sciences SC Environmental Sciences & Ecology GA AY5EN UT WOS:000347596000005 PM 25464040 ER PT J AU Kim, YJ Brooks, SC Zhang, F Parker, JC Moon, JW Roh, Y AF Kim, Young-Jin Brooks, Scott C. Zhang, Fan Parker, Jack C. Moon, Ji-Won Roh, Yul TI Fate and transport of uranium (VI) in weathered saprolite SO JOURNAL OF ENVIRONMENTAL RADIOACTIVITY LA English DT Article DE Uranium(VI); Transport; Modeling; Saprolite ID SURFACE COMPLEXATION MODEL; DOUBLE-LAYER MODEL; SOLUTE TRANSPORT; SUBSURFACE MEDIA; BLIND PREDICTION; METAL SORPTION; ADSORPTION; GOETHITE; URANYL; CARBONATE AB Batch and column experiments were conducted to investigate sorption and transport of uranium (U) in the presence of saprolite derived from interbedded shale, limestone, and sandstone sequences. Sorption kinetics were measured at two initial concentrations (C-0; 1, 10 mu M) and three soil:solution ratios (R-s/w; 0.005, 0.25, 2 kg/L) at pH 4.5 (pH of the saprolite). The rate of U loss from solution (mu mole/L/h) increased with increasing R-s/w. Uranium sorption exhibited a fast phase with 80% sorption in the first eight hours for all C-0 and R-s/w values and a slow phase during which the reaction slowly approached (pseudo) equilibrium over the next seven days. The pH-dependency of U sorption was apparent in pH sorption edges. U(VI) sorption increased over the pH range 4-6, then decreased sharply at pH > 7.5. U(VI) sorption edges were well described by a surface complexation model using calibrated parameters and the reaction network proposed by Waite et al. (1994). Sorption isotherms measured using the same R-s/w and pH values showed a solids concentration effect where U(VI) sorption capacity and affinity decreased with increasing solids concentration. This effect may have been due to either particle aggregation or competition between U(VI) and exchangeable cations for sorption sites. The surface complexation model with calibrated parameters was able to predict the general sorption behavior relatively well, but failed to reproduce solid concentration effects, implying the importance of appropriate design if batch experiments are to be utilized for dynamic systems. Transport of U(VI) through the packed column was significantly retarded. Transport simulations were conducted using the reactive transport model HydroGeoChem (HGC) v5.0 that incorporated the surface complexation reaction network used to model the batch data. Model parameters reported by Waite et al. (1994) provided a better prediction of U transport than optimized parameters derived from our sorption edges. The results presented in this study highlight the challenges in defining appropriate conditions for batch-type experiments used to extrapolate parameters for transport models, and also underline a gap in our ability to transfer batch results to transport simulations. (C) 2014 Elsevier Ltd. All rights reserved. C1 [Kim, Young-Jin] Samsung C&T Corp, Civil Engn Div, Seoul 137956, South Korea. [Brooks, Scott C.] Oak Ridge Natl Lab, Div Environm Sci, Oak Ridge, TN 37831 USA. [Zhang, Fan] Chinese Acad Sci, Inst Tibetan Plateau Res, Key Lab Tibetan Environm Changes & Land Surface P, Beijing 100085, Peoples R China. [Parker, Jack C.] Univ Tennessee, Dept Civil & Environm Engn, Knoxville, TN 37996 USA. [Moon, Ji-Won] Oak Ridge Natl Lab, Biosci Div, Oak Ridge, TN 37831 USA. [Roh, Yul] Chonnam Natl Univ, Fac Earth Syst & Environm Sci, Kwangju 500757, South Korea. RP Brooks, SC (reprint author), Oak Ridge Natl Lab, Div Environm Sci, POB 2008, Oak Ridge, TN 37831 USA. EM brookssc@ornl.gov RI Moon, Ji-Won/A-9186-2011; Brooks, Scott/B-9439-2012 OI Moon, Ji-Won/0000-0001-7776-6889; Brooks, Scott/0000-0002-8437-9788 FU U.S. Department of Energy, Office of Science, Office of Biological and Environmental Research, Subsurface Biogeochemical Research Program; UT-Battelle, LLC [DE-AC05-000R22725]; U.S. Department of Energy FX This work was funded by the U.S. Department of Energy, Office of Science, Office of Biological and Environmental Research, Subsurface Biogeochemical Research Program. The authors would like to thank two anonymous reviewers for their comments. This manuscript has been authored by UT-Battelle, LLC, under contract DE-AC05-000R22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this 161 manuscript, or allow others to do so, for United States Government purposes. NR 61 TC 2 Z9 2 U1 3 U2 17 PU ELSEVIER SCI LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, OXON, ENGLAND SN 0265-931X EI 1879-1700 J9 J ENVIRON RADIOACTIV JI J. Environ. Radioact. PD JAN PY 2015 VL 139 SI SI BP 154 EP 162 DI 10.1016/j.jenvrad.2014.10.008 PG 9 WC Environmental Sciences SC Environmental Sciences & Ecology GA AY5EN UT WOS:000347596000017 PM 25464052 ER PT J AU Deng, B Chen, H Chen, K Chen, J Gong, D Guo, D Hu, X Huang, D Kierstead, J Li, X Liu, C Liu, T Xiang, AC Xu, H Xu, T You, Y Ye, J AF Deng, B. Chen, H. Chen, K. Chen, J. Gong, D. Guo, D. Hu, X. Huang, D. Kierstead, J. Li, X. Liu, C. Liu, T. Xiang, A. C. Xu, H. Xu, T. You, Y. Ye, J. TI The clock distribution system for the ATLAS Liquid Argon Calorimeter Phase-I Upgrade Demonstrator SO JOURNAL OF INSTRUMENTATION LA English DT Article; Proceedings Paper CT Topical Workshop on Electronics for Particle Physics CY SEP 22-26, 2014 CL Aix en Provence, FRANCE DE Radiation-hard electronics; Front-end electronics for detector readout; Detector control systems (detector and experiment monitoring and slow-control systems, architecture, hardware, algorithms, databases) AB A prototype Liquid-argon Trigger Digitizer Board (LTDB), called the LTDB Demonstrator, has been developed to demonstrate the functions of the ATLAS Liquid Argon Calorimeter Phase-I trigger electronics upgrade. Forty Analog-to-Digital converters and four FPGAs with embedded multi-gigabit-transceivers on each Demonstrator need high quality clocks. A clock distribution system based on commercial components has been developed for the Demonstrator. The design of the clock distribution system is presented. The performance of the clock distribution system has been evaluated. The components used in the clock distribution system have been qualified to meet radiation tolerance requirements of the Demonstrator. C1 [Deng, B.] Hubei Polytech Univ, Sch Elect & Elect Informat Engn, Huangshi 435003, Hubei, Peoples R China. [Deng, B.; Gong, D.; Guo, D.; Li, X.; Liu, C.; Liu, T.; Xiang, A. C.; Ye, J.] So Methodist Univ, Dept Phys, Dallas, TX 75275 USA. [Chen, H.; Chen, K.; Hu, X.; Kierstead, J.] Brookhaven Natl Lab, Dept Phys, Upton, NY 11973 USA. [Chen, K.] Univ Houston, Dept Elect Engn, Houston, TX 77004 USA. [Chen, K.; Huang, D.; You, Y.] So Methodist Univ, Dept Elect Engn, Dallas, TX 75275 USA. [Guo, D.] Univ Sci & Technol China, Dept Modern Phys, Hefei 230026, Anhui, Peoples R China. [Li, X.] Cent China Normal Univ, Dept Phys, Wuhan 430079, Hubei, Peoples R China. [Xu, T.] Shandong Univ, MOE Key Lab Particle Phys & Particle Irradiat, Jinan 250100, Shandong, Peoples R China. RP Liu, T (reprint author), So Methodist Univ, Dept Phys, Dallas, TX 75275 USA. FU US-ATLAS RD program; U.S. Department of Energy [DE-FG02-04ER1299]; Hubei Provincial Natural Science Foundation of China [2014CFC1093] FX This work is supported by US-ATLAS R&D program for the upgrade of the LHC, the U.S. Department of Energy Grant DE-FG02-04ER1299 and Hubei Provincial Natural Science Foundation of China (Grant Number 2014CFC1093). The authors would like to express the deepest appreciation to Ms. Tanya Herrera, Dr. Steve Wender, and Dr. Ron Nelson, Dr. Helio Takai, Dr. Mike Wirthlin, Mr. Long Huang, Dr. Ethan Casio for beneficial discussions and kind help during the irradiation tests. NR 12 TC 0 Z9 0 U1 8 U2 14 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 1748-0221 J9 J INSTRUM JI J. Instrum. PD JAN PY 2015 VL 10 AR C01004 DI 10.1088/1748-0221/10/01/C01004 PG 8 WC Instruments & Instrumentation SC Instruments & Instrumentation GA AY7BE UT WOS:000347715400004 ER PT J AU Limburg, KE Walther, BD Lu, ZL Jackman, G Mohan, J Walther, Y Nissling, A Weber, PK Schmitt, AK AF Limburg, Karin E. Walther, Benjamin D. Lu, Zunli Jackman, George Mohan, John Walther, Yvonne Nissling, Anders Weber, Peter K. Schmitt, Axel K. TI In search of the dead zone: Use of otoliths for tracking fish exposure to hypoxia SO JOURNAL OF MARINE SYSTEMS LA English DT Article; Proceedings Paper CT Workshop 1 of IMBIZO III CY JAN, 2013 CL Goa, INDIA DE Fish otoliths; Biogeochemical markers; Hypoxia proxies ID PERCH PERCA-FLAVESCENS; X-RAY-FLUORESCENCE; TRACE-ELEMENTS; WATER CHEMISTRY; BALTIC SEA; CLIMATE VARIABILITY; SULFUR ISOTOPES; NATURAL TAGS; LIFE-HISTORY; MANGANESE AB Otolith chemistry is often useful for tracking provenance of fishes, as well as examining migration histories. Whereas elements such as strontium and barium correlate well with salinity and temperature, experiments that examine manganese uptake as a function of these parameters have found no such correlation. Instead, dissolved manganese is available as a redox product, and as such, is indicative of low-oxygen conditions. Here we present evidence for that mechanism in a range of habitats from marine to freshwater, across species, and also present ancillary proxies that support the mechanism as well. For example, iodine is redox-sensitive and varies inversely with Mn; and sulfur stable isotope ratios provide evidence of anoxic sulfate reduction in some circumstances. Further, S may be incorporated trophically whereas other elements appear to be taken up directly from water. This research suggests a potential means to identify individual fish exposure to hypoxia, over entire lifetimes. With further testing and understanding, in the future fish may be able to be used as "mobile monitors" of hypoxic conditions. (C) 2014 The Authors. Published by Elsevier B.V. C1 [Limburg, Karin E.] SUNY Coll Environm Sci & Forestry, Dept Environm & Forest Biol, Syracuse, NY 13210 USA. [Walther, Benjamin D.; Mohan, John] Univ Texas Austin, Inst Marine Sci, Port Aransas, TX 78373 USA. [Lu, Zunli] Syracuse Univ, Dept Earth Sci, Syracuse, NY 13244 USA. [Jackman, George] CUNY Queens Coll, Dept Biol, Flushing, NY 11367 USA. [Walther, Yvonne] Swedish Univ Agr Sci, Inst Marine Res, SE-37137 Karlskrona, Sweden. [Nissling, Anders] Uppsala Univ, Dept Ecol & Genet, Ar Res Stn, SE-62167 Visby, Sweden. [Weber, Peter K.] Lawrence Livermore Natl Lab, Div Chem Sci, Livermore, CA 94550 USA. [Schmitt, Axel K.] Univ Calif Los Angeles, Dept Earth & Space Sci, Los Angeles, CA 90095 USA. RP Limburg, KE (reprint author), SUNY Coll Environm Sci & Forestry, Dept Environm & Forest Biol, Syracuse, NY 13210 USA. EM klimburg@esf.edu RI Walther, Benjamin/A-7284-2009; UCLA, SIMS/A-1459-2011; OI Walther, Benjamin/0000-0002-2902-4001; Schmitt, Axel/0000-0002-9029-4211 FU National Fish and Wildlife Foundation; FORMAS "Multistressors Project"; National Science Foundation; National Institutes of Health/National Institute of General Medical Sciences under NSF [DMR-00936384] FX We thank AM. Gorman and C. Vandergoot, Ohio Department of Natural Resources, for providing yellow perch otoliths, R. Monteiro for the alewife otolith, D. Dale (Cornell University), D. Driscoll (ESF), and N. Miller (Jackson School of Geoscience) for help with SXFM and LA-ICPMS analyses, and P. Thomas for ship time in the northern Gulf of Mexico. D. Swaney and R. Kraus provided helpful comments on an earlier draft, as did three anonymous reviewers. We thank the National Fish and Wildlife Foundation for partial support; we also thank D. Conley for partial financial support through the FORMAS "Multistressors Project". This work is based in part upon research conducted at the Cornell High Energy Synchrotron Source (CHESS) which is supported by the National Science Foundation and the National Institutes of Health/National Institute of General Medical Sciences under NSF award DMR-00936384. NR 83 TC 22 Z9 22 U1 7 U2 62 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0924-7963 EI 1879-1573 J9 J MARINE SYST JI J. Mar. Syst. PD JAN PY 2015 VL 141 SI SI BP 167 EP 178 DI 10.1016/j.jmarsys.2014.02.014 PG 12 WC Geosciences, Multidisciplinary; Marine & Freshwater Biology; Oceanography SC Geology; Marine & Freshwater Biology; Oceanography GA AY9KM UT WOS:000347868800016 ER PT J AU Ghate, VP Miller, MA Albrecht, BA Fairall, CW AF Ghate, Virendra P. Miller, Mark A. Albrecht, Bruce A. Fairall, Christopher W. TI Thermodynamic and Radiative Structure of Stratocumulus-Topped Boundary Layers SO JOURNAL OF THE ATMOSPHERIC SCIENCES LA English DT Article DE Clouds; Cumulus clouds; Radiative fluxes; Thermodynamics ID SOUTHEAST PACIFIC STRATOCUMULUS; LOWER-TROPOSPHERIC STABILITY; COMMUNITY ATMOSPHERE MODEL; LARGE-EDDY SIMULATIONS; LOW CLOUD COVER; MARINE STRATOCUMULUS; PART I; ACCURATE PARAMETERIZATION; CLIMATE MODELS; CIRRUS CLOUDS AB Stratocumulus-topped boundary layers (STBLs) observed in three different regions are described in the context of their thermodynamic and radiative properties. The primary dataset consists of 131 soundings from the southeastern Pacific (SEP), 90 soundings from the island of Graciosa (GRW) in the North Atlantic, and 83 soundings from the U.S. Southern Great Plains (SGP). A new technique that makes an attempt to preserve the depths of the sublayers within an STBL is proposed for averaging the profiles of thermodynamic and radiative variables. A one-dimensional radiative transfer model known as the Rapid Radiative Transfer Model was used to compute the radiative fluxes within the STBL. The SEP STBLs were characterized by a stronger and deeper inversion, together with thicker clouds, lower free-tropospheric moisture, and higher radiative flux divergence across the cloud layer, as compared to the GRW STBLs. Compared to the STBLs over the marine locations, the STBLs over SGP had higher wind shear and a negligible (-0.41 g kg(-1)) jump in mixing ratio across the inversion. Despite the differences in many of the STBL thermodynamic parameters, the differences in liquid water path at the three locations were statistically insignificant. The soundings were further classified as well mixed or decoupled based on the difference between the surface and cloud-base virtual potential temperature. The decoupled STBLs were deeper than the well-mixed STBLs at all three locations. Statistically insignificant differences in surface latent heat flux (LHF) between well-mixed and decoupled STBLs suggest that parameters other than LHF are responsible for producing decoupling. C1 [Ghate, Virendra P.] Argonne Natl Lab, Div Environm Sci, Argonne, IL 60439 USA. [Miller, Mark A.] Rutgers State Univ, Dept Environm Sci, New Brunswick, NJ 08903 USA. [Albrecht, Bruce A.] Univ Miami, Dept Atmospher Sci, Miami, FL USA. [Fairall, Christopher W.] NOAA, Earth Syst Res Lab, Boulder, CO USA. RP Ghate, VP (reprint author), 9700 S Cass Ave, Argonne, IL 60439 USA. EM vghate@anl.gov FU U.S. Department of Energy's Atmospheric System Research, an Office of Science, Office of Biological and Environmental Research program [DE-AC02-06CH11357]; Atmospheric System Research Grant [DE-FG02-08ER64531]; U.S. Department of Energy, Office of Science, Office of Biological and Environmental Research, Climate and Environmental Sciences Division; NOAA FX The authors wish to thank Dr. Ping Zhu for many helpful discussions about the topic, which led to significant improvement of the manuscript. The authors would also like to thank the anonymous reviewers, particularly reviewer 3, whose comments led to a significant improvement of the manuscript. The authors also would like to thank the crew of R/V Ronald H. Brown for their support in launching the radiosondes and collecting valuable data from multiple cruises. This work was supported primarily by the U.S. Department of Energy's Atmospheric System Research, an Office of Science, Office of Biological and Environmental Research program, under Contract DE-AC02-06CH11357. MAM was supported through the Atmospheric System Research Grant DE-FG02-08ER64531. Some of the data were obtained from the Atmospheric Radiation Measurement Program (ARM) sponsored by the U.S. Department of Energy, Office of Science, Office of Biological and Environmental Research, Climate and Environmental Sciences Division. We thank the NOAA Climate Observation Program (COP) for their funding support. NR 62 TC 6 Z9 6 U1 2 U2 16 PU AMER METEOROLOGICAL SOC PI BOSTON PA 45 BEACON ST, BOSTON, MA 02108-3693 USA SN 0022-4928 EI 1520-0469 J9 J ATMOS SCI JI J. Atmos. Sci. PD JAN PY 2015 VL 72 IS 1 BP 430 EP 451 DI 10.1175/JAS-D-13-0313.1 PG 22 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA AY1WA UT WOS:000347378900025 ER PT J AU Chen, FR Kisielowski, C Van Dyck, D AF Chen, F. -R. Kisielowski, C. Van Dyck, D. TI 3D reconstruction of nanocrystalline particles from a single projection SO MICRON LA English DT Article DE High resolution TEM; 3D reconstruction at atomic resolution; Shape of nanocrystalline particle ID RESOLUTION ELECTRON TOMOGRAPHY; DIFFRACTION; MICROSCOPY; ATOMS; HREM; TEM AB This paper describes an approach to retrieve the three-dimensional atomic structure of a nanocrystalline particle from the reconstructed electron exit wave function in a single projection direction. The method employs wave propagation to determine the local exit surface of each atomic column together with its mass. The exit wave in between colums is used as internal calibration so as to remove the background noise and improve the precision to the level of single atom sensitivity. The validity of the approach is tested with exit wave functions of a gold wedge reconstructed from simulated images containing different levels of noise. (C) 2014 Elsevier Ltd. All rights reserved. C1 [Chen, F. -R.] Natl Tsing Hua Univ Hsin Chu, Hsinchu, Taiwan. [Kisielowski, C.] Natl Ctr Elect Microscopy, Berkeley, CA 94720 USA. [Kisielowski, C.] Joint Ctr Artificial Photosynthesis, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Van Dyck, D.] Univ Antwerp, EMAT, Dept Phys, Antwerp, Belgium. RP Chen, FR (reprint author), Natl Tsing Hua Univ Hsin Chu, Hsinchu, Taiwan. EM fchenl@me.com RI Foundry, Molecular/G-9968-2014 FU Office of Science, Office of Basic Energy Sciences of the U.S. Department of Energy [DE-AC02-05CH11231]; Fund for Scientific Research - Flanders (FWO) [VF04812 N, G.0188.08]; NSC [96-2628-E-007-017-MY3, 101-2120-M-007-012-CC1] FX CK is supported by the Office of Science, Office of Basic Energy Sciences of the U.S. Department of Energy under contract no. DE-AC02-05CH11231. D. Van Dyck acknowledges the financial support from the Fund for Scientific Research - Flanders (FWO) under Project nos. VF04812 N and G.0188.08. F.-R. Chen would like to thank the support from NSC 96-2628-E-007-017-MY3 and NSC 101-2120-M-007-012-CC1. NR 21 TC 4 Z9 4 U1 5 U2 32 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0968-4328 J9 MICRON JI Micron PD JAN PY 2015 VL 68 BP 59 EP 65 DI 10.1016/j.micron.2014.08.009 PG 7 WC Microscopy SC Microscopy GA AZ1RW UT WOS:000348016500009 PM 25306935 ER PT J AU Lin, YY Wen, JG Hu, LH McCarthy, JA Wang, SC Poeppelmeier, KR Marks, LD AF Lin, Yuyuan Wen, Jianguo Hu, Linhua McCarthy, James A. Wang, Shichao Poeppelmeier, Kenneth R. Marks, Laurence D. TI Electron-induced Ti-rich surface segregation on SrTiO3 nanoparticles SO MICRON LA English DT Article DE Beam damage; HREM; Surface structure; Simulation; Strontium titanate; Nanoparticles ID SCANNING-FORCE-MICROSCOPY; ELEVATED-TEMPERATURES; TUNGSTEN TRIOXIDE; PHASE-TRANSITIONS; ISLAND FORMATION; OXIDE SURFACES; DESORPTION; DIET; CHEMISTRY; DIFFUSION AB Atomic surface structures of nanoparticles are of interest in catalysis and other fields. Aberration-corrected HREM facilitates direct imaging of the surfaces of nanoparticles. A remaining concern of surface imaging arises from beam damage. It is important to identify the intrinsic surface structures and the ones created by electron beam irradiation in TEM. In this study, we performed aberration-corrected HREM and EELS to demonstrate that TiO and bcc type Ti islands form due to intense electron irradiation. The formation of Ti-rich islands is in agreement with previous high temperature annealing experiments on the surfaces of SrTiO3 single crystals. (C) 2014 Elsevier Ltd. All rights reserved. C1 [Lin, Yuyuan; Marks, Laurence D.] Northwestern Univ, Dept Mat Sci & Engn, Evanston, IL 60208 USA. [Wen, Jianguo] Argonne Natl Lab, Electron Microscopy Ctr, Argonne, IL 60439 USA. [Hu, Linhua; McCarthy, James A.; Wang, Shichao; Poeppelmeier, Kenneth R.] Northwestern Univ, Dept Chem, Evanston, IL 60208 USA. RP Lin, YY (reprint author), Northwestern Univ, Dept Mat Sci & Engn, Evanston, IL 60208 USA. EM YuyuanLin2014@u.northwestern.edu; L-marks@northwestern.edu RI Wang, Shichao/K-1973-2013; Marks, Laurence/B-7527-2009 OI Wang, Shichao/0000-0003-3632-9193; FU Northwestern University Institute for Catalysis in Energy Processes (ICEP) [DOE DE-FG02-03-ER15457]; UChicago Argonne, LLC [DE-AC02-06CH11357] FX We acknowledge funding from the Northwestern University Institute for Catalysis in Energy Processes (ICEP) on grant number DOE DE-FG02-03-ER15457. The electron microscopy was performed at the Electron Microscopy Center for Materials Research at Argonne National Laboratory, a U.S. Department of Energy Office of Science Laboratory operated under Contract No. DE-AC02-06CH11357 by UChicago Argonne, LLC. NR 46 TC 3 Z9 3 U1 5 U2 54 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0968-4328 J9 MICRON JI Micron PD JAN PY 2015 VL 68 BP 152 EP 157 DI 10.1016/j.micron.2014.05.007 PG 6 WC Microscopy SC Microscopy GA AZ1RW UT WOS:000348016500022 PM 24931386 ER PT J AU Van Dyck, D Lobato, I Chen, FR Kisielowski, C AF Van Dyck, Dirk Lobato, Ivan Chen, Fu-Rong Kisielowski, Christian TI Do you believe that atoms stay in place when you observe them in HREM? SO MICRON LA English DT Article DE Quantitative HREM; TDS; Dose rate dependence ID ELECTRON-MICROSCOPE IMAGES; THERMAL DIFFUSE-SCATTERING; HIGH-RESOLUTION IMAGES; PHONON-SCATTERING; INELASTIC-SCATTERING; CONTRAST; DIFFRACTION; SIMULATIONS; SENSITIVITY; HOLOGRAPHY AB Recent advancements in aberration-corrected electron microscopy allow for an evaluation of unexpectedly large atom displacements beyond a resolution limit of similar to 0.5 angstrom, which are found to be dose-rate dependent in high resolution images. In this paper we outline a consistent description of the electron scattering process, which explains these unexpected phenomena. Our approach links thermal diffuse scattering to electron beam-induced object excitation and relaxation processes, which strongly contribute to the image formation process. The effect can provide an explanation for the well-known contrast mismatch ("Stobbs factor") between image calculations and experiments. (C) 2014 Elsevier Ltd. All rights reserved. C1 [Van Dyck, Dirk; Lobato, Ivan] Univ Antwerp, EMAT, B-2020 Antwerp, Belgium. [Chen, Fu-Rong] Natl Tsing Hua Univ, Dept Engn & Syst Sci, Hsinchu 300, Taiwan. [Kisielowski, Christian] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Natl Ctr Electron Microscopy, Berkeley, CA 94720 USA. [Kisielowski, Christian] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Joint Ctr Artificial Photosynth, Berkeley, CA 94720 USA. RP Van Dyck, D (reprint author), Univ Antwerp, EMAT, Groenenborgerlaan 171, B-2020 Antwerp, Belgium. EM dirk.vandyck@uantwerp.be; ivan.lobato@uantwerp.be; frchen1@me.com; cfkisielowski@lbl.gov RI Foundry, Molecular/G-9968-2014 FU Office of Science of the U.S. Department of Energy [DE-SC0004993]; Fund for Scientific Research Flanders (FWO) [VF04812N, G.0188.08]; NSC [96-2628-E-007-017-MY3, 101-2120-M-007-012-CC1] FX Ck's work was performed for the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the U.S. Department of Energy under Award Number DE-SC0004993. D. Van Dyck acknowledges the financial support from the Fund for Scientific Research Flanders (FWO) under Project nos. VF04812N and G.0188.08. F.-R. Chen would like to thank the support from NSC 96-2628-E-007-017-MY3 and NSC 101-2120-M-007-012-CC1. NR 43 TC 3 Z9 3 U1 3 U2 19 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0968-4328 J9 MICRON JI Micron PD JAN PY 2015 VL 68 BP 158 EP 163 DI 10.1016/j.micron.2014.09.003 PG 6 WC Microscopy SC Microscopy GA AZ1RW UT WOS:000348016500023 PM 25311646 ER PT J AU Calderon, HA Kisielowski, C Specht, P Barton, B Godinez-Salomon, F Solorza-Feria, O AF Calderon, H. A. Kisielowski, C. Specht, P. Barton, B. Godinez-Salomon, F. Solorza-Feria, O. TI Maintaining the genuine structure of 2D materials and catalytic nanoparticles at atomic resolution SO MICRON LA English DT Article DE Electron microscopy; Low dose microscopy; Atomic resolution; Beam damage; Nanoparticles; Graphene; Beam induced transformation ID TRANSMISSION ELECTRON-MICROSCOPY; PARTICLES AB The recent development of atomic resolution, low dose-rate electron microscopy allows investigating 2D materials as well as catalytic nano particles without compromising their structural integrity. For graphene and a variety of nanoparticle compositions, it is shown that a critical dose rate exists of <100 e(-)/angstrom(2) s at 80 keV of electron acceleration that allows maintaining the genuine object structures including their surfaces and edges even if particles are only 3 nm large or smaller. Moreover, it is demonstrated that electron beam-induced phonon excitation from outside the field of view contributes to a contrast degradation in recorded images. These degradation effects can be eliminated by delivering electrons onto the imaged area, only, by using a Nilsonian illumination scheme in combination with a suitable aperture at the electron gun/monochromator assembly. (C) 2014 Elsevier Ltd. All rights reserved. C1 [Calderon, H. A.] UPALM Zacatenco, ESFM IPN, Dept Fis, Mexico City, DF, Mexico. [Kisielowski, C.; Barton, B.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Natl Ctr Electron Microscopy, Berkeley, CA 94720 USA. [Kisielowski, C.; Barton, B.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Joint Ctr Artificial Photosynth, Berkeley, CA 94720 USA. [Specht, P.] UCB, Dept Mat Sci Engn, Berkeley, CA 94720 USA. [Godinez-Salomon, F.; Solorza-Feria, O.] CINVESTAV IPN, Ctr Invest & Estudios Avanzados, Dept Quim, Inst Politecn Nacl, Mexico City 07360, DF, Mexico. RP Calderon, HA (reprint author), UPALM Zacatenco, ESFM IPN, Dept Fis, Ed 9, Mexico City, DF, Mexico. EM hcalder@esfm.ipn.mx RI Foundry, Molecular/G-9968-2014; Barton, Bastian/H-9268-2016 FU Office of Science, Office of Basic Energy Sciences of the U.S. Department of Energy [DE-AC02-05CH11231]; CONACYT [75/2012, 148304, 129207]; IPN; Helios SERC-LBNL FX Electron Microscopy was performed at NCEM, which is supported by the Office of Science, Office of Basic Energy Sciences of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. The research is partially supported by CONACYT (Proyecto FOINST. 75/2012, 148304 and 129207), IPN (COFAA, SIP) and Helios SERC-LBNL. HAC is on sabbatical leave at LBNL. NR 29 TC 3 Z9 3 U1 2 U2 16 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0968-4328 J9 MICRON JI Micron PD JAN PY 2015 VL 68 BP 164 EP 175 DI 10.1016/j.micron.2014.08.007 PG 12 WC Microscopy SC Microscopy GA AZ1RW UT WOS:000348016500024 PM 25240633 ER PT J AU Helveg, S Kisielowski, CF Jinschek, JR Specht, P Yuan, G Frei, H AF Helveg, S. Kisielowski, C. F. Jinschek, J. R. Specht, P. YuaN, G. Frei, H. TI Observing gas-catalyst dynamics at atomic resolution and single-atom sensitivity SO MICRON LA English DT Article DE Transmission electron microscopy; Exit wave reconstruction; In situ studies; Catalysis; Water-splitting; Nanocrystals; Gas-surface interactions; Dynamics ID TRANSMISSION ELECTRON-MICROSCOPY; IN-SITU; HETEROGENEOUS CATALYSTS; MOS2 NANOCATALYSTS; IMAGE-RESOLUTION; DOSE-RATE; TEM; NANOPARTICLES; PRESSURE; BEHAVIOR AB Transmission electron microscopy (TEM) has become an indispensable technique for studying heterogeneous catalysts. In particular, advancements of aberration-Corrected electron optics and data acquisition schemes have made TEM capable of delivering images of catalysts with sub-Angstrom resolution and single-atom sensitivity. Parallel developments of differentially pumped electron microscopes and of gas cells enable in situ observations of catalysts during the exposure to reactive gas environments at pressures of up to atmospheric levels and temperatures of up to several hundred centigrade. Here, we outline how to take advantage of the emerging state-of-the-art instrumentation and methodologies to study surface structures and dynamics to improve the understanding of structure-sensitive catalytic functionality. The concept of using low electron dose-rates in TEM in conjunction with in-line holography and aberration-correction at low voltage (80 kV) is introduced to allow maintaining atomic resolution and sensitivity during in situ observations of catalysts. Benefits are illustrated by exit wave reconstructions of TEM images of a nanocrystalline Co3O4 catalyst material acquired in situ during their exposure to either a reducing or oxidizing gas environment. (C) 2014 Published by Elsevier Ltd. C1 [Kisielowski, C. F.; Frei, H.] JCAP, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Kisielowski, C. F.] Natl Ctr Elect Microscopy, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Jinschek, J. R.] FEI Co, NL-5651 GG Eindhoven, Netherlands. [Specht, P.] Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA. [YuaN, G.; Frei, H.] Phys Biosciences Div, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Helveg, S (reprint author), Haldor Topsoe A-S Nymollevej 55, DK-2800 Lyngby, Denmark. EM sth@topsoe.dk; cfkisielowski@lbl.gov RI Foundry, Molecular/G-9968-2014 FU Joint Center for Artificial Photosynthesis; DOE Energy Innovation Hub; U.S. Department of Energy [DE-SC0004993, DE-AC02-05CH11231] FX TEM measurements were conducted at the electron microscopy facility at Haldor Topsoe A/S. The authors gratefully acknowledge Sven Ullmann (Haldor Topsoe A/S) for support during the experiments. The data acquisition and interpretation were supported by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the U.S. Department of Energy under Award Number DE-SC0004993. Co oxide crystals were prepared by work supported by the Director, Office of Science, Office of Basic Energy Sciences, Division of Chemical, Geological and Biosciences of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. NR 64 TC 8 Z9 8 U1 10 U2 91 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0968-4328 J9 MICRON JI Micron PD JAN PY 2015 VL 68 BP 176 EP 185 DI 10.1016/j.micron.2014.07.009 PG 10 WC Microscopy SC Microscopy GA AZ1RW UT WOS:000348016500025 PM 25245867 ER PT J AU Kisielowski, C Specht, P Gygax, SM Barton, B Calderon, HA Kang, JH Cieslinski, R AF Kisielowski, C. Specht, P. Gygax, S. M. Barton, B. Calderon, H. A. Kang, J. H. Cieslinski, R. TI Instrumental requirements for the detection of electron beam-induced object excitations at the single atom level in high-resolution transmission electron microscopy SO MICRON LA English DT Article DE TEM; Single atom sensitivity; Low dose imaging; Aberration-correction; Catalysis; Functionality ID RECONSTRUCTION; TEM; ABERRATION; MONOCHROMATOR; IMPROVE AB This contribution touches on essential requirements for instrument stability and resolution that allows operating advanced electron microscopes at the edge to technological capabilities. They enable the detection of single atoms and their dynamic behavior on a length scale of picometers in real time. It is understood that the observed atom dynamic is intimately linked to the relaxation and thermalization of electron beam-induced sample excitation. Resulting contrast fluctuations are beam current dependent and largely contribute to a contrast mismatch between experiments and theory if not considered. If explored, they open the possibility to study functional behavior of nanocrystals and single molecules at the atomic level in real time. (C) 2014 Elsevier Ltd. All rights reserved. C1 [Kisielowski, C.] Lawrence Berkeley Natl Lab, Natl Ctr Elect Microscopy, Berkeley, CA 94720 USA. [Kisielowski, C.] Lawrence Berkeley Natl Lab, Joint Ctr Artificial Photosynthesis, Berkeley, CA 94720 USA. [Specht, P.; Gygax, S. M.] Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA. [Barton, B.] Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. [Calderon, H. A.] ESFM IPN, Dept Fis, Mexico City 07300, DF, Mexico. [Kang, J. H.; Cieslinski, R.] Dow Chem Co USA, Midland, MI 48667 USA. RP Specht, P (reprint author), Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA. EM specht@berkeley.edu RI Foundry, Molecular/G-9968-2014; Barton, Bastian/H-9268-2016 FU Office of Science, Office of Basic Energy Sciences of the U.S. Department of Energy [DE-AC02-05CH11231]; Office of Science of the U.S. Department of Energy [DE-SC0004993] FX Electron Microscopy was performed at the NCEM, which is supported by the Office of Science, Office of Basic Energy Sciences of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. Experiments with NiFeOx catalysts were performed for the Joint Center for Artificial Synthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the U.S. Department of Energy under Award Number DE-SC0004993. The Dow Chemical Company supported P. Specht for the investigation of the rhodium catalysts. NR 38 TC 6 Z9 6 U1 3 U2 23 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0968-4328 J9 MICRON JI Micron PD JAN PY 2015 VL 68 BP 186 EP 193 DI 10.1016/j.micron.2014.07.010 PG 8 WC Microscopy SC Microscopy GA AZ1RW UT WOS:000348016500026 PM 25153732 ER PT J AU Septer, AN Bose, JL Lipzen, A Martin, J Whistler, C Stabb, EV AF Septer, Alecia N. Bose, Jeffrey L. Lipzen, Anna Martin, Joel Whistler, Cheryl Stabb, Eric V. TI Bright luminescence of Vibrio fischeri aconitase mutants reveals a connection between citrate and the Gac/Csr regulatory system SO MOLECULAR MICROBIOLOGY LA English DT Article ID SQUID EUPRYMNA-SCOLOPES; ESCHERICHIA-COLI ACONITASES; COGNATE RESPONSE REGULATOR; BARA SENSOR KINASE; POSTTRANSCRIPTIONAL REGULATION; SMALL RNAS; SYMBIOTIC COLONIZATION; OXIDATIVE STRESS; CSRA; GENE AB The Gac/Csr regulatory system is conserved throughout the -proteobacteria and controls key pathways in central carbon metabolism, quorum sensing, biofilm formation and virulence in important plant and animal pathogens. Here we show that elevated intracellular citrate levels in a Vibrio fischeri aconitase mutant correlate with activation of the Gac/Csr cascade and induction of bright luminescence. Spontaneous or directed mutations in the gene that encodes citrate synthase reversed the bright luminescence of aconitase mutants, eliminated their citrate accumulation and reversed their elevated expression of CsrB. Our data elucidate a correlative link between central metabolic and regulatory pathways, and they suggest that the Gac system senses a blockage at the aconitase step of the tricarboxylic acid cycle, either through elevated citrate levels or a secondary metabolic effect of citrate accumulation, and responds by modulating carbon flow and various functions associated with host colonization, including bioluminescence. C1 [Septer, Alecia N.; Bose, Jeffrey L.; Stabb, Eric V.] Univ Georgia, Dept Microbiol, Athens, GA 30602 USA. [Lipzen, Anna; Martin, Joel] DOE Joint Genome Inst, Walnut Creek, CA 94596 USA. [Whistler, Cheryl] Univ New Hampshire, Dept Mol Cellular & Biomed Sci, Durham, NH 03824 USA. RP Stabb, EV (reprint author), Univ Georgia, Dept Microbiol, 120 Cedar St, Athens, GA 30602 USA. EM estabb@uga.edu FU National Science Foundation (NSF) [CAREER MCB-0347317, IOS-0841480, IOS-1121106]; University of Georgia Graduate School; DoD, Air Force Office of Scientific Research, National Defense Science and Engineering Graduate (NDSEG) Fellowship [32 CFR 168a]; Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231] FX We would like to thank Lawrence Shimkets, Diana Downs, Anne Dunn and Jorge Escalante-Semerena for helpful discussions, and Christa Pennacchio, and Wendy Schackwitz at the Joint Genome Institute for assisting with whole-genome resequencing. This research was supported by the National Science Foundation (NSF) under grants CAREER MCB-0347317, IOS-0841480 and IOS-1121106. ANS was supported by funds awarded by the University of Georgia Graduate School and the DoD, Air Force Office of Scientific Research, National Defense Science and Engineering Graduate (NDSEG) Fellowship, 32 CFR 168a. Genome resequencing was conducted by the U.S. Department of Energy Joint Genome Institute supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. NR 70 TC 2 Z9 2 U1 1 U2 19 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0950-382X EI 1365-2958 J9 MOL MICROBIOL JI Mol. Microbiol. PD JAN PY 2015 VL 95 IS 2 BP 283 EP 296 DI 10.1111/mmi.12864 PG 14 WC Biochemistry & Molecular Biology; Microbiology SC Biochemistry & Molecular Biology; Microbiology GA AY8IF UT WOS:000347796700010 PM 25402589 ER PT J AU Hong, MQ Ren, F Wang, YQ Zhang, HX Xiao, XH Fu, DJ Yang, B Jiang, CZ AF Hong, Mengqing Ren, Feng Wang, Yongqiang Zhang, Hongxiu Xiao, Xiangheng Fu, Dejun Yang, Bing Jiang, Changzhong TI Size-dependent radiation tolerance and corrosion resistance in ion irradiated CrN/AlTiN nanofilms SO NUCLEAR INSTRUMENTS & METHODS IN PHYSICS RESEARCH SECTION B-BEAM INTERACTIONS WITH MATERIALS AND ATOMS LA English DT Article DE Radiation tolerance; Corrosion resistance; Multilayered nanofilm ID NANOLAYER FILMS; BEHAVIOR; AMORPHIZATION; TRANSITION; COATINGS; ALLOYS; TIN AB This paper demonstrates a substantial enhancement in radiation tolerance and corrosion resistance for the CrN/AlTiN multilayered nanofilms with the decreasing of period-thickness. After irradiation by 190 keV Ar+ ions to the dose of 81 dpa, the amorphization region in the CrN/AlTiN 3 nm multilayered nanofilm is much smaller than that in the CrN/AlTiN 7 nm multilayered nanofilm and the CrN film based on glancing-incidence X-ray diffraction measurements. Potentiodynamic polarization and impedance measurements show that the CrN/AlTiN multilayered nanofilms have good corrosion resistance to irradiation. With increasing the irradiation fluence, the irradiated samples are more susceptible to corrosive electrolyte. However, the CrN/AlTiN multilayered nanofilm with smaller period-thickness shows significant enhancement of the corrosion resistance under both irradiation and un-irradiation conditions. Under the same irradiation fluence of 5 x 10(16) ions/cm(2), the corrosion current density increased 9.47 times for the CrN film, while it only increased 2.08 times for the CrN/AlTiN 3 nm multilayered nanofilm. The interfaces of multilayered nanofilms act as effective sinks for irradiation-induced defects and are responsible for the enhanced radiation tolerance and corrosion resistance properties. (C) 2014 Elsevier B.V. All rights reserved. C1 [Hong, Mengqing; Ren, Feng; Zhang, Hongxiu; Xiao, Xiangheng; Fu, Dejun; Jiang, Changzhong] Wuhan Univ, Sch Phys & Technol, Wuhan 430072, Peoples R China. [Wang, Yongqiang] Wuhan Univ, Ctr Elect Microscopy, Wuhan 430072, Peoples R China. [Wang, Yongqiang] Los Alamos Natl Lab, Div Mat Sci & Technol, Los Alamos, NM 87545 USA. [Yang, Bing] Wuhan Univ, Sch Power & Mech Engn, Wuhan 430072, Peoples R China. RP Ren, F (reprint author), Wuhan Univ, Sch Phys & Technol, Wuhan 430072, Peoples R China. EM fren@whu.edu.cn RI Ren, Feng/F-9778-2014; OI Ren, Feng/0000-0002-9557-5995; xiao, xiangheng/0000-0001-9111-1619 FU Natural Science Foundation of China [11475129, 11175133, 91026014]; Foundation from Chinese Ministry of Education [20110141130004, NCET-13-0438]; Foundation from Hubei Provincial Natural Science Foundation - China [2012FFA042]; Center for Integrated Nanotechnologies, a DOE nanoscience user facility FX The author thanks the Natural Science Foundation of China (11475129, 11175133, 91026014), the Foundations from Chinese Ministry of Education (20110141130004, NCET-13-0438), Hubei Provincial Natural Science Foundation - China (2012FFA042) for financial support. We thank fruitful discussions with Prof. M. Demkowicz of MIT. YQW acknowledges the partial support from Center for Integrated Nanotechnologies, a DOE nanoscience user facility, jointly operated by Los Alamos and Sandia national Laboratories. NR 27 TC 0 Z9 0 U1 2 U2 20 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0168-583X EI 1872-9584 J9 NUCL INSTRUM METH B JI Nucl. Instrum. Methods Phys. Res. Sect. B-Beam Interact. Mater. Atoms PD JAN 1 PY 2015 VL 342 BP 137 EP 143 DI 10.1016/j.nimb.2014.09.032 PG 7 WC Instruments & Instrumentation; Nuclear Science & Technology; Physics, Atomic, Molecular & Chemical; Physics, Nuclear SC Instruments & Instrumentation; Nuclear Science & Technology; Physics GA AY7YA UT WOS:000347770500021 ER PT J AU Zhang, J Wang, YQ Tang, M Sun, C Yin, DM Li, N AF Zhang, J. Wang, Y. Q. Tang, M. Sun, C. Yin, D. M. Li, N. TI Helium irradiation induced micro-swelling and phase separation in pyrochlore Lu2Ti2O7 SO NUCLEAR INSTRUMENTS & METHODS IN PHYSICS RESEARCH SECTION B-BEAM INTERACTIONS WITH MATERIALS AND ATOMS LA English DT Article DE Ion irradiation; Unit swelling; Ceramics ID SELF-IRRADIATION; NUCLEAR-WASTE; OXIDES; DISORDER; IMMOBILIZATION; ABSORPTION; ACTINIDES; PLUTONIUM; ZIRCONIA; FUEL AB Polycrystalline pyrochlore Lu2Ti2O7 was irradiated with 200 key He+ ions at room temperature to fluences ranging from 2.0 x 10(15) to 2.0 x 10(17) He+/cm(2). Irradiation-induced microstructural evolution was examined by grazing incidence X-ray diffraction and cross-sectional transmission electron microscopy. A micro-swelling (lattice expansion) induced by cation ion disordering was observed, which an obvious swelling was achieved at a fluence of 2.0 x 10(16) He+/cm(2), and saturated at a fluence of 1.0 x 10(17) He+/cm(2) with cation ions fully disordered. Furthermore, during the irradiation process, the pristine pyrochlore phase was found to form by a fluence of 5.0 x 10(16) He+/cm(2), corresponding to an average ballistic damage dose of 0.25 displacements per atom (dpa) for the near surface examined region. No amorphization was observed even to the highest fluence of 2.0 x 10(17) He+/cm(2). The experimental observations are further discussed in the context of antisite formation in the pyrochlore Lu2Ti2O7. (C) 2014 Elsevier B.V. All rights reserved. C1 [Zhang, J.; Yin, D. M.; Li, N.] Xiamen Univ, Coll Energy, Xiamen 361005, Fujian, Peoples R China. [Zhang, J.; Wang, Y. Q.; Tang, M.; Sun, C.] Los Alamos Natl Lab, Mat Sci & Technol Div, Los Alamos, NM 87545 USA. RP Zhang, J (reprint author), Xiamen Univ, Coll Energy, Xiamen 361005, Fujian, Peoples R China. EM zhangjian@xmu.edu.cn OI Zhang, Jianzhong/0000-0001-5508-1782 FU National Natural Science Foundation of China [11205128]; Center for Integrated Nanotechnologies at Los Alamos National Laboratory; DOE-NE Materials Recovery and Waste Form Development program FX This work was sponsored by the National Natural Science Foundation of China with Grant No. 11205128. The work at the Ion Beam Materials Laboratory was partially supported by Center for Integrated Nanotechnologies at Los Alamos National Laboratory. M. Tang would like to thank the financial support of the DOE-NE Materials Recovery and Waste Form Development program including program support from James Bresee, Kimberly Gray, Terry Todd and John Vienna. NR 22 TC 7 Z9 8 U1 1 U2 12 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0168-583X EI 1872-9584 J9 NUCL INSTRUM METH B JI Nucl. Instrum. Methods Phys. Res. Sect. B-Beam Interact. Mater. Atoms PD JAN 1 PY 2015 VL 342 BP 179 EP 183 DI 10.1016/j.nimb.2014.09.036 PG 5 WC Instruments & Instrumentation; Nuclear Science & Technology; Physics, Atomic, Molecular & Chemical; Physics, Nuclear SC Instruments & Instrumentation; Nuclear Science & Technology; Physics GA AY7YA UT WOS:000347770500027 ER PT J AU Xin, XK Li, B Jung, JH Yoon, YJ Biswas, R Lin, ZQ AF Xin, Xukai Li, Bo Jung, Jaehan Yoon, Young Jun Biswas, Rana Lin, Zhiqun TI Ab Initio Simulation of Charge Transfer at the Semiconductor Quantum Dot/TiO2 Interface in Quantum Dot-Sensitized Solar Cells SO PARTICLE & PARTICLE SYSTEMS CHARACTERIZATION LA English DT Article ID PHOTOINDUCED ELECTRON-TRANSFER; MULTIPLE EXCITON GENERATION; ENHANCED PERFORMANCE; TIO2 NANOPARTICLES; OPTICAL-PROPERTIES; ENERGY-TRANSFER; ANATASE TIO2; LOW-COST; CDSE; NANOCRYSTALS AB Quantum dot-sensitized solar cells (QDSSCs) have emerged as a promising solar architecture for next-generation solar cells. The QDSSCs exhibit a remarkably fast electron transfer from the quantum dot (QD) donor to the TiO2 acceptor with size quantization properties of QDs that allows for the modulation of band energies to control photoresponse and photoconversion efficiency of solar cells. To understand the mechanisms that underpin this rapid charge transfer, the electronic properties of CdSe and PbSe QDs with different sizes on the TiO2 substrate are simulated using a rigorous ab initio density functional method. This method capitalizes on localized orbital basis set, which is computationally less intensive. Quite intriguingly, a remarkable set of electron bridging states between QDs and TiO2 occurring via the strong bonding between the conduction bands of QDs and TiO2 is revealed. Such bridging states account for the fast adiabatic charge transfer from the QD donor to the TiO2 acceptor, and may be a general feature for strongly coupled donor/acceptor systems. All the QDs/TiO2 systems exhibit type II band alignments, with conduction band offsets that increase with the decrease in QD size. This facilitates the charge transfer from QDs donors to TiO2 acceptors and explains the dependence of the increased charge transfer rate with the decreased QD size. C1 [Xin, Xukai; Li, Bo; Jung, Jaehan; Yoon, Young Jun; Lin, Zhiqun] Georgia Inst Technol, Sch Mat Sci & Engn, Atlanta, GA 30332 USA. [Biswas, Rana] Iowa State Univ, US DOE, Dept Phys & Astron, Ames, IA 50011 USA. [Biswas, Rana] Iowa State Univ, US DOE, Ames Lab, Ames, IA 50011 USA. RP Xin, XK (reprint author), Georgia Inst Technol, Sch Mat Sci & Engn, Atlanta, GA 30332 USA. EM biswasr@iastate.edu; zhiqun.lin@mse.gatech.edu RI li, bo/I-3282-2014 OI li, bo/0000-0001-9407-9503 FU Air Force Office of Scientific Research [MURI FA9550-14-1-0037]; Key Laboratory of Computational Physical Sciences at Fudan University, Shanghai, China; U.S. Department of Energy, Basic Energy Sciences, Materials Sciences and Engineering Division [DE-AC 02-07CH11358]; Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231] FX This work was supported by the Air Force Office of Scientific Research (MURI FA9550-14-1-0037) (Z.L.), the Key Laboratory of Computational Physical Sciences at Fudan University, Shanghai, China (Z.L); and by the U.S. Department of Energy, Basic Energy Sciences, Materials Sciences and Engineering Division, under contract no. DE-AC 02-07CH11358 (R.B). This research used the resources of the National Energy Research Scientific Computing Center, which is supported by the Office of Science of the U.S. Department of Energy under contract no. DE-AC02-05CH11231. NR 52 TC 7 Z9 7 U1 1 U2 28 PU WILEY-V C H VERLAG GMBH PI WEINHEIM PA BOSCHSTRASSE 12, D-69469 WEINHEIM, GERMANY SN 0934-0866 EI 1521-4117 J9 PART PART SYST CHAR JI Part. Part. Syst. Charact. PD JAN PY 2015 VL 32 IS 1 BP 80 EP 90 DI 10.1002/ppsc.201400111 PG 11 WC Chemistry, Physical; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary SC Chemistry; Science & Technology - Other Topics; Materials Science GA AY7FW UT WOS:000347727600010 ER PT J AU Canto-Pastor, A Molla-Morales, A Ernst, E Dahl, W Zhai, J Yan, Y Meyers, BC Shanklin, J Martienssen, R AF Canto-Pastor, A. Molla-Morales, A. Ernst, E. Dahl, W. Zhai, J. Yan, Y. Meyers, B. C. Shanklin, J. Martienssen, R. TI Efficient transformation and artificial miRNA gene silencing in Lemna minor SO PLANT BIOLOGY LA English DT Article DE AmiRNA; CH42; Lemnaceae; microRNA; RNA silencing; stable transformation ID ARABIDOPSIS-THALIANA; SMALL RNAS; MICRORNAS; DUCKWEED; PLANTS; GIBBA; PCR; DNA; REGENERATION; INDUCTION AB Despite rapid doubling time, simple architecture and ease of metabolic labelling, a lack of genetic tools in the Lemnaceae (duckweed) has impeded the full implementation of this organism as a model for biological research. Here, we present technologies to facilitate high-throughput genetic studies in duckweed. We developed a fast and efficient method for producing Lemna minor stable transgenic fronds via Agrobacterium-mediated transformation and regeneration from tissue culture. Additionally, we engineered an artificial microRNA (amiRNA) gene silencing system. We identified a Lemna gibba endogenous miR166 precursor and used it as a backbone to produce amiRNAs. As a proof of concept we induced the silencing of CH42, a magnesium chelatase subunit, using our amiRNA platform. Expression of CH42 in transgenic L.minor fronds was significantly reduced, which resulted in reduction of chlorophyll pigmentation. The techniques presented here will enable tackling future challenges in the biology and biotechnology of Lemnaceae. C1 [Canto-Pastor, A.; Molla-Morales, A.; Ernst, E.; Dahl, W.; Martienssen, R.] Cold Spring Harbor Lab, Cold Spring Harbor, NY 11724 USA. [Zhai, J.; Meyers, B. C.] Univ Delaware, Newark, DE USA. [Yan, Y.; Shanklin, J.] Brookhaven Natl Lab, Upton, NY 11973 USA. [Martienssen, R.] Cold Spring Harbor Lab, Howard Hughes Med Inst, Gordon & Betty Moore Fdn, Cold Spring Harbor, NY 11724 USA. RP Martienssen, R (reprint author), Cold Spring Harbor Lab, POB 100, Cold Spring Harbor, NY 11724 USA. EM martiens@cshl.edu RI Meyers, Blake/B-6535-2012 OI Meyers, Blake/0000-0003-3436-6097 FU US Department of Energy [DE-EE0003298] FX We thank Vitaly Citovsky for advice on Agrobacterium strains and infection media, and Leo Guthart for his support. This work was supported by a grant from US Department of Energy (DE-EE0003298) to R.A.M. and J.S. NR 35 TC 10 Z9 10 U1 3 U2 28 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 1435-8603 EI 1438-8677 J9 PLANT BIOLOGY JI Plant Biol. PD JAN PY 2015 VL 17 SU 1 SI SI BP 59 EP 65 DI 10.1111/plb.12215 PG 7 WC Plant Sciences SC Plant Sciences GA AY8JE UT WOS:000347799100009 PM 24989135 ER PT J AU Wilson, AD Orme, CJ AF Wilson, Aaron D. Orme, Christopher J. TI Concentration dependent speciation and mass transport properties of switchable polarity solvents SO RSC ADVANCES LA English DT Article ID PRESSURE-RETARDED OSMOSIS; AMMONIA-CARBON DIOXIDE; INTERNAL CONCENTRATION POLARIZATION; BIPHASIC AMINE SOLVENTS; POWER-GENERATION; DRAW SOLUTES; HYDROPHILICITY SOLVENTS; SALINITY GRADIENTS; LIPID EXTRACTION; OSMOTIC POWER AB Tertiary amine switchable polarity solvents (SPS) consisting of predominantly water, tertiary amine, and tertiary ammonium and bicarbonate ions were produced at various concentrations for three different amines: N, N-dimethylcyclohexylamine, N, N-dimethyloctylamine, and 1-cyclohexylpiperidine. These amines exhibit either osmotic or non-osmotic character as observed through forward osmosis, which led to this study to better understand speciation and its influence on water transport through a semipermeable membrane. For all concentrations, several physical properties were measured including viscosity, molecular diffusion coefficients, freezing point depression, and density. Based on these measurements, a variation on the Mark-Houwink equation was developed to predict the viscosity of any tertiary amine SPS as a function of concentration using the amine's molecular mass. The physical properties of osmotic SPS, which are identified as having an amine to carbonic acid salt ratio of similar to 1 : 1, have consistent concentration dependence behavior over a wide range of concentrations, which suggests osmotic pressures based on low concentrations freezing point studies can be extrapolated reliably to higher concentrations. The observed physical properties also allowed the identification of solution state speciation of non-osmotic SPS, where the amine to carbonic acid salts ratio is significantly greater than one. These results indicate that, at most concentrations, the stoichiometric excess of amine is involved in solvating a proton with two amines. C1 [Wilson, Aaron D.; Orme, Christopher J.] Idaho Natl Lab, Idaho Falls, ID 83415 USA. RP Wilson, AD (reprint author), Idaho Natl Lab, POB 1625 MS 2208, Idaho Falls, ID 83415 USA. EM aaron.wilson@inl.gov RI Wilson, Aaron/C-4364-2008 OI Wilson, Aaron/0000-0001-5865-6537 FU United States Department of Energy [DE-AC07-05ID14517]; Idaho National Laboratory via the Laboratory Directed Research and Development program FX This work was supported by the United States Department of Energy through contract DE-AC07-05ID14517. Funding was supplied by Idaho National Laboratory via the Laboratory Directed Research and Development program. The authors thank Nicole K. Kruse of Bruker BioSpin for supplying the 13C DOSY pulse sequence. NR 69 TC 8 Z9 8 U1 6 U2 41 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2046-2069 J9 RSC ADV JI RSC Adv. PY 2015 VL 5 IS 10 BP 7740 EP 7751 DI 10.1039/c4ra08558b PG 12 WC Chemistry, Multidisciplinary SC Chemistry GA AY5JX UT WOS:000347609400091 ER PT J AU Desroches, LB Ganeshalingam, M AF Desroches, Louis-Benoit Ganeshalingam, Mohan TI The dynamics of incremental costs of efficient television display technologies SO TECHNOLOGICAL FORECASTING AND SOCIAL CHANGE LA English DT Article DE Televisions; Efficiency; Experience curves ID EXPERIENCE CURVES; RATES AB We study the evolution of the incremental cost and price of efficiency for televisions in the U.S. market. We focus on televisions due to their rapid technological evolution and large number of annual shipments, such that costs and prices evolve on short timescales as compared to other consumer durable goods. Using the experience curve approach, we compare manufacturing costs and selling prices of two liquid crystal display (LCD) technologies. We find a mean experience rate of 27% for less efficient cold cathode fluorescent lamp LCD televisions and 14% for more efficient light emitting diode LCD televisions, using price data. This corresponds to an annual decline of approximately 17% per year in price for both television types. Our results also suggest that the incremental cost or price of efficiency, holding other major features constant, declines much more rapidly than the baseline cost or price. We find that the incremental cost or price declines at roughly 50% per year. The fitted parameters do depend on the specific technology modeled, as well as on whether cost or price data are used. Our results for LCD televisions are qualitatively similar to other display technologies, even very mature ones, suggesting that the cost and price decline extends many years after a technology is considered mature. We also analyze the selling prices of ENERGY STAR and non-ENERGY STAR televisions, which support our main findings. These results highlight the consumer benefits of efficient display technologies, and how the dynamics of incremental costs differ from baseline costs. (C) 2014 Elsevier Inc. All rights reserved. C1 [Desroches, Louis-Benoit; Ganeshalingam, Mohan] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. RP Desroches, LB (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, 1 Cyclotron Rd, Berkeley, CA 94720 USA. EM ldesroches@lbl.gov NR 20 TC 2 Z9 2 U1 2 U2 9 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 0040-1625 EI 1873-5509 J9 TECHNOL FORECAST SOC JI Technol. Forecast. Soc. Chang. PD JAN PY 2015 VL 90 BP 562 EP 574 DI 10.1016/j.techfore.2014.02.016 PN B PG 13 WC Business; Planning & Development SC Business & Economics; Public Administration GA AY5IH UT WOS:000347605400020 ER PT J AU Payne, SH AF Payne, Samuel H. TI The utility of protein and mRNA correlation SO TRENDS IN BIOCHEMICAL SCIENCES LA English DT Editorial Material DE bioinformatics; systems biology; proteomics; transcriptomics ID GLOBAL ANALYSIS; YEAST; EXPRESSION; ABUNDANCE; CANCER AB Transcriptomic, proteomic, and metabolomic measurements are revolutionizing the way we model and predict cellular behavior, and multi-omic comparisons are being published with increased regularity. Some have expected a trivial and predictable correlation between mRNA and protein; however, the manifest complexity of biological regulation suggests a more nuanced relationship. Indeed, observing this lack of strict correlation provides clues for new research topics, and has the potential for transformative biological insight. C1 Pacific NW Natl Lab, Richland, WA 99354 USA. RP Payne, SH (reprint author), Pacific NW Natl Lab, 902 Battelle Blvd, Richland, WA 99354 USA. EM samuel.payne@pnnl.gov OI Payne, Samuel/0000-0002-8351-1994 FU NCI NIH HHS [U24 CA160019, U24-CA-160019] NR 15 TC 13 Z9 13 U1 3 U2 18 PU ELSEVIER SCIENCE LONDON PI LONDON PA 84 THEOBALDS RD, LONDON WC1X 8RR, ENGLAND SN 0968-0004 J9 TRENDS BIOCHEM SCI JI Trends Biochem.Sci. PD JAN PY 2015 VL 40 IS 1 BP 1 EP 3 DI 10.1016/j.tibs.2014.10.010 PG 3 WC Biochemistry & Molecular Biology SC Biochemistry & Molecular Biology GA AY9ID UT WOS:000347862900001 PM 25467744 ER PT J AU Hochstrasser, ML Doudna, JA AF Hochstrasser, Megan L. Doudna, Jennifer A. TI Cutting it close: CRISPR-associated endoribonuclease structure and function SO TRENDS IN BIOCHEMICAL SCIENCES LA English DT Review DE CRISPR-Cas; crRNA; Cas5; Cas6; endoribonuclease; structure and function ID GUIDED SURVEILLANCE COMPLEX; PROCESSES PRE-CRRNA; CAS SYSTEMS; CRYSTAL-STRUCTURE; IMMUNE-SYSTEM; INTERFERENCE COMPLEX; RNA RECOGNITION; PYROCOCCUS-FURIOSUS; ANTIVIRAL DEFENSE; ADAPTIVE IMMUNITY AB Many bacteria and archaea possess an adaptive immune system consisting of repetitive genetic elements known as clustered regularly interspaced short palindromic repeats (CRISPRs) and CRISPR-associated (Cas) proteins. Similar to RNAi pathways in eukaryotes, CRISPR Cas systems require small RNAs for sequence-specific detection and degradation of complementary nucleic acids. Cas5 and Cas6 enzymes have evolved to specifically recognize and process CRISPR-derived transcripts into functional small RNAs used as guides by interference complexes. Our detailed understanding of these proteins has led to the development of several useful Cas6-based biotechnological methods. Here, we review the structures, functions, mechanisms, and applications of the enzymes responsible for CRISPR RNA (crRNA) processing, highlighting a fascinating family of endonucleases with exquisite RNA recognition and cleavage activities. C1 [Hochstrasser, Megan L.; Doudna, Jennifer A.] Univ Calif Berkeley, Dept Mol & Cell Biol, Berkeley, CA 94720 USA. [Doudna, Jennifer A.] Univ Calif Berkeley, Howard Hughes Med Inst, Berkeley, CA 94720 USA. [Doudna, Jennifer A.] Univ Calif Berkeley, Calif Inst Quantitat Biosci, Berkeley, CA 94720 USA. [Doudna, Jennifer A.] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Doudna, Jennifer A.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA 94720 USA. RP Doudna, JA (reprint author), Univ Calif Berkeley, Dept Mol & Cell Biol, 229 Stanley Hall, Berkeley, CA 94720 USA. EM doudna@berkeley.edu NR 68 TC 16 Z9 18 U1 2 U2 55 PU ELSEVIER SCIENCE LONDON PI LONDON PA 84 THEOBALDS RD, LONDON WC1X 8RR, ENGLAND SN 0968-0004 J9 TRENDS BIOCHEM SCI JI Trends Biochem.Sci. PD JAN PY 2015 VL 40 IS 1 BP 58 EP 66 DI 10.1016/j.tibs.2014.10.007 PG 9 WC Biochemistry & Molecular Biology SC Biochemistry & Molecular Biology GA AY9ID UT WOS:000347862900008 PM 25468820 ER PT J AU Kerfeld, CA Erbilgin, O AF Kerfeld, Cheryl A. Erbilgin, Onur TI Bacterial microcompartments and the modular construction of microbial metabolism SO TRENDS IN MICROBIOLOGY LA English DT Review DE bacterial microcompartments; carboxysomes; metabolosomes; synthetic biology; bacterial organelles ID B-12-DEPENDENT 1,2-PROPANEDIOL DEGRADATION; DEPENDENT DIOL DEHYDRATASE; SALMONELLA-ENTERICA; CARBOXYSOME SHELL; PDU MICROCOMPARTMENT; ESCHERICHIA-COLI; INCREASE PHOTOSYNTHESIS; LACTOBACILLUS-REUTERI; STRUCTURAL INSIGHTS; CRYSTAL-STRUCTURES AB Bacterial microcompartments (BMCs) are protein-bound organelles predicted to be present across 23 bacterial phyla. BMCs facilitate carbon fixation as well as the aerobic and anaerobic catabolism of a variety of organic compounds. These functions have been linked to ecological nutrient cycling, symbiosis, pathogenesis, and cardiovascular disease. Within bacterial cells, BMCs are metabolic modules that can be further dissociated into their constituent structural and functional protein domains. Viewing BMCs as genetic, structural, functional, and evolutionary modules provides a framework for understanding both BMC-mediated metabolism and for adapting their architectures for applications in synthetic biology. C1 [Kerfeld, Cheryl A.] Michigan State Univ, DOE Plant Res Lab, E Lansing, MI 48824 USA. [Kerfeld, Cheryl A.; Erbilgin, Onur] Univ Calif Berkeley, Dept Plant & Microbial Biol, Berkeley, CA 94720 USA. [Kerfeld, Cheryl A.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA 94720 USA. [Kerfeld, Cheryl A.] Berkeley Synthet Biol Inst, Berkeley, CA USA. RP Kerfeld, CA (reprint author), Michigan State Univ, DOE Plant Res Lab, E Lansing, MI 48824 USA. EM ckerfeld@lbl.gov OI erbilgin, onur/0000-0002-6122-6156 FU US Department of Energy, Office of Basic Energy Sciences [DE-AC02 05CH11231]; National Science Foundation [MCB1160614, EF1105892] FX The authors would like to thank members of the Kerfeld laboratory for valuable discussions, and to thank Cristina Iancu and Grant Jensen for providing the micrograph used in Figure 3. This material is based on work supported by the US Department of Energy, Office of Basic Energy Sciences under contract no. DE-AC02 05CH11231 and by grants from the National Science Foundation (MCB1160614 and EF1105892). NR 101 TC 25 Z9 26 U1 11 U2 58 PU ELSEVIER SCI LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, OXON, ENGLAND SN 0966-842X EI 1878-4380 J9 TRENDS MICROBIOL JI Trends Microbiol. PD JAN PY 2015 VL 23 IS 1 BP 22 EP 34 DI 10.1016/j.tim.2014.10.003 PG 13 WC Biochemistry & Molecular Biology; Microbiology SC Biochemistry & Molecular Biology; Microbiology GA AY9JF UT WOS:000347865600006 PM 25455419 ER PT J AU Alammar, T Noei, H Wang, YM Gruner, W Mudring, AV AF Alammar, Tarek Noei, Heshmat Wang, Yuemin Gruener, Wolfgang Mudring, Anja-Verena TI Ionic Liquid-Assisted Sonochemical Preparation of CeO2 Nanoparticles for CO Oxidation SO ACS SUSTAINABLE CHEMISTRY & ENGINEERING LA English DT Article DE Catalysis; Ceria; CO oxidation; Ionic liquids; Nanomaterials ID ROOM-TEMPERATURE; PHOTOCATALYTIC ACTIVITY; CERIUM OXIDE; FILMS; NANORODS; PHOTOLUMINESCENCE; CONDENSATION; NANOCRYSTALS; NANOPOWDERS; DEPENDENCE AB CeO2 nanoparticles were synthesized via a one-step ultrasound synthesis in different kinds of ionic liquids based on bis(trifluoromethanesulfonylamide, [Tf2N](-),in combination with various cations including 1-butyl-3-methylimidazolium ([C(4)mim](+)), 1-ethyl-2,3-dimethylimidazolium ([Edimim](+)), butyl-pyridinium([Py-4](+)), 1-butyl-1-methyl-pyrrolidinium ([Pyrr(14)](+)), and 2-hydroxyethyl-trimethylammonium ([N1112OH](+)). Depending on synthetic parameters, such as ionic liquid, Ce(IV) precursor, heating method, and precipitator, formed ceria exhibits different morphologies, varying from nanospheres, nanorods, nanoribbons, and nanoflowers. The morphology, crystallinity, and chemical composition of the obtained materials were characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy XPS), energy dispersive X-ray spectroscopy (EDX), Raman spectroscopy, and N-2 adsorption. The structural and electronic properties of the as-prepared CeO2 samples were probed by CO adsorption using IR spectroscopy under ultrahigh vacuum conditions. The catalytic activities of CeO2 nanoparticles were investigated in the oxidation of CO. CeO2 nanospheres obtained sonochemically in [C(4)mim] [Tf2N] exhibit the best performance for low-temperature CO oxidation. The superior catalytic performance of this material can be related to its mesoporous structure, small particle size, large surface area, and high number of surface oxygen vacancy sites. C1 [Alammar, Tarek; Mudring, Anja-Verena] Ruhr Univ Bochum, D-44780 Bochum, Germany. [Noei, Heshmat] DESY, D-22607 Hamburg, Germany. [Wang, Yuemin; Gruener, Wolfgang] Ruhr Univ Bochum, Lab Ind Chem, D-44780 Bochum, Germany. [Mudring, Anja-Verena] Iowa State Univ, Ames, IA 50011 USA. [Mudring, Anja-Verena] Ames Lab, Crit Mat Inst, Ames, IA 50011 USA. RP Mudring, AV (reprint author), Ruhr Univ Bochum, D-44780 Bochum, Germany. EM mudring@iastate.edu FU DFG Cluster of Excellence RESOLV; Critical Materials Institute, an Energy Innovation Hub - U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Advanced Manufacturing Office FX We would like to thank Dr. Dennis Gramann for help with the catalytic studies. This work is supported in part by the DFG Cluster of Excellence RESOLV and the Critical Materials Institute, an Energy Innovation Hub funded by the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Advanced Manufacturing Office. NR 66 TC 11 Z9 11 U1 9 U2 58 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 2168-0485 J9 ACS SUSTAIN CHEM ENG JI ACS Sustain. Chem. Eng. PD JAN PY 2015 VL 3 IS 1 BP 42 EP 54 DI 10.1021/sc500387k PG 13 WC Chemistry, Multidisciplinary; GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY; Engineering, Chemical SC Chemistry; Science & Technology - Other Topics; Engineering GA AY3XY UT WOS:000347513900006 ER PT J AU Carpenter, JS McCabe, RJ Mayeur, JR Mara, NA Beyerlein, IJ AF Carpenter, John S. McCabe, Rodney J. Mayeur, Jason R. Mara, Nathan A. Beyerlein, Irene J. TI Interface-Driven Plasticity: The Presence of an Interface Affected Zone in Metallic Lamellar Composites SO ADVANCED ENGINEERING MATERIALS LA English DT Article ID NB NANOLAMELLAR COMPOSITES; MULTILAYER COMPOSITES; MECHANICAL-PROPERTIES; BIMETAL INTERFACES; TEXTURE EVOLUTION; HIGH-STRENGTH; DEFORMATION; STABILITY; MICROSTRUCTURE AB Large strain deformation is used to make fine nanolayered two-phase composites from stacks of conventional polycrystalline sheets. The final materials made by this technique possess a crystallographically highly oriented structure containing nearly atomically perfect interfaces prevailing ubiquitously throughout the material. How this ordered structure evolves with strain from the coarser, more disordered state is not known. Here, using microstructural analysis and computational modeling, we discover a local interface-affected zone (IAZ) possessing the same crystallographically sharp structure in coarse layered composites as the final nanolayered composites. This means that this strongly oriented interface zone survives the mechanical work and overtakes the structure as it refines to the nanoscale. In essence, through the formation of this interface zone, the crossover to a highly oriented nanostructure occurs. Using microstructural analysis and crystal plasticity simulations, we show that the IAZ is a consequence of slip accommodation at the interface. This insight is valuable for developing processing strategies for superior interface-dominated materials. C1 [Carpenter, John S.; McCabe, Rodney J.; Mara, Nathan A.] Los Alamos Natl Lab, Div Mat Sci & Technol, Los Alamos, NM 87545 USA. [Mayeur, Jason R.; Beyerlein, Irene J.] Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. [Mara, Nathan A.] Los Alamos Natl Lab, Mat Phys & Applicat Div, Los Alamos, NM 87545 USA. RP Carpenter, JS (reprint author), Los Alamos Natl Lab, Div Mat Sci & Technol, Los Alamos, NM 87545 USA. EM carpenter@lanl.gov RI Mara, Nathan/J-4509-2014; OI McCabe, Rodney /0000-0002-6684-7410; Carpenter, John/0000-0001-8821-043X FU Los Alamos National Laboratory Directed Research and Development (LDRD) [20140348ER]; Center for Materials at Irradiation and Mechanical Extremes, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [2008LANL1026]; DOE [DEAC5206NA25396] FX J.S.C. and R.J.M. acknowledge the financial support provided by the Los Alamos National Laboratory Directed Research and Development (LDRD) project 20140348ER. J.R.M., I.J.B., and N.A.M. gratefully acknowledge support by the Center for Materials at Irradiation and Mechanical Extremes, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Award Number 2008LANL1026. Los Alamos National Laboratory is operated by Los Alamos National Security LLC under DOE Contract DEAC5206NA25396. Electron microscopy was performed at the Los Alamos Electron Microscopy Laboratory. NR 27 TC 3 Z9 3 U1 4 U2 23 PU WILEY-V C H VERLAG GMBH PI WEINHEIM PA BOSCHSTRASSE 12, D-69469 WEINHEIM, GERMANY SN 1438-1656 EI 1527-2648 J9 ADV ENG MATER JI Adv. Eng. Mater. PD JAN PY 2015 VL 17 IS 1 BP 109 EP 114 DI 10.1002/adem.201400210 PG 6 WC Materials Science, Multidisciplinary SC Materials Science GA AY0RU UT WOS:000347305300015 ER PT J AU Talamo, A AF Talamo, Alberto TI CUDA and MPI performances on the computation of Rossi-alpha distribution from pulsed neutron sources SO ANNALS OF NUCLEAR ENERGY LA English DT Article DE Rossi-alpha; Subcritical; CUDA; MPI; MCNP AB This study presents the methodology to calculate the Rossi-alpha distribution for a subcritical assembly driven by an external pulsed neutron source through MCNP6 computer simulations. The Rossi-alpha distribution is obtained from the signal (e.g., He-3(n,p) reactions) of a neutron detector placed in one experimental channel of the subcritical assembly. The detector signal is obtained from MCNP6 computer simulations modeling a single pulse of the external neutron source. The MCNP6 output data for a single pulse of the external neutron source must be processed to take into account the effect of delayed neutrons born in all previous source pulses. The calculation of the Rossi-a distribution from a pulsed neutron source is time consuming because of the huge amount of processed data. Consequently, the algorithms introduced in this work use parallel computing platforms, e.g., CUDA or MPI, to reduce the computing time. Published by Elsevier Ltd. C1 Argonne Natl Lab, Nucl Engn Div, Argonne, IL 60439 USA. RP Talamo, A (reprint author), Argonne Natl Lab, Nucl Engn Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM alby@anl.gov OI talamo, alberto/0000-0001-5685-0483 FU U.S. Department of Energy [DE-AC02-06CH11357] FX Argonne National Laboratory's work is supported by the U.S. Department of Energy under contract DE-AC02-06CH11357. The author thanks NVIDIA, Silicon Mechanics, and Microway for providing K20 and K40 computing platforms. NR 11 TC 0 Z9 0 U1 1 U2 3 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0306-4549 J9 ANN NUCL ENERGY JI Ann. Nucl. Energy PD JAN PY 2015 VL 75 BP 168 EP 175 DI 10.1016/j.anucene.2014.07.040 PG 8 WC Nuclear Science & Technology SC Nuclear Science & Technology GA AY3OS UT WOS:000347493400020 ER PT J AU Schunert, S Wang, YQ Martineau, R DeHart, MD AF Schunert, Sebastian Wang, Yaqi Martineau, Richard DeHart, Mark D. TI A new mathematical adjoint for the modified SAAF-S-N equations SO ANNALS OF NUCLEAR ENERGY LA English DT Article DE Linear transport equation; Adjoint; SAAF-S-N equations AB We present a new adjoint FEM weak form, which can be directly used for evaluating the mathematical adjoint, suitable for perturbation calculations, of the self-adjoint angular flux S-N equations (SAAF-S-N) without construction and transposition of the underlying coefficient matrix. Stabilization schemes incorporated in the described SAAF-S-N method make the mathematical adjoint distinct from the physical adjoint, i.e. the solution of the continuous adjoint equation with SAAF-S-N. This weak form is implemented into RattleSnake, the MOOSE (Multiphysics Object-Oriented Simulation Environment) based transport solver. Numerical results verify the correctness of the implementation and show its utility both for fixed source and eigenvalue problems. Published by Elsevier Ltd. C1 [Schunert, Sebastian; Wang, Yaqi; DeHart, Mark D.] Idaho Natl Lab, Reactor Phys Anal & Design, Idaho Falls, ID 83415 USA. [Martineau, Richard] Idaho Natl Lab, Fuel Modeling & Simulat, Idaho Falls, ID 83415 USA. RP Schunert, S (reprint author), Idaho Natl Lab, Reactor Phys Anal & Design, 2525 Freemont Ave,POB 1625, Idaho Falls, ID 83415 USA. EM sebastian.schunert@inl.gov; yaqi.wang@inl.gov; richard.martineau@inl.gov; mark.dehart@inl.gov FU Battelle Energy Alliance, LLC [DE-AC07-05ID14517] FX This manuscript has been authored by Battelle Energy Alliance, LLC under Contract No. DE-AC07-05ID14517 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a nonexclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. NR 14 TC 1 Z9 1 U1 1 U2 4 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0306-4549 J9 ANN NUCL ENERGY JI Ann. Nucl. Energy PD JAN PY 2015 VL 75 BP 340 EP 352 DI 10.1016/j.anucene.2014.08.028 PG 13 WC Nuclear Science & Technology SC Nuclear Science & Technology GA AY3OS UT WOS:000347493400042 ER PT J AU George, NM Terrani, K Powers, J Worrall, A Maldonado, I AF George, Nathan Michael Terrani, Kurt Powers, Jeff Worrall, Andrew Maldonado, Ivan TI Neutronic analysis of candidate accident-tolerant cladding concepts in pressurized water reactors SO ANNALS OF NUCLEAR ENERGY LA English DT Article DE Alternate cladding; Accident tolerant fuel; FeCrAl; 310SS; SiC; PWR ID FUEL; OXIDATION; IRRADIATION; COMPOSITE; SCALE; STEAM AB A study analyzed the neutronics of alternate cladding materials in a pressurized water reactor (PWR) environment. Austenitic type 310 (310SS) and 304 stainless steels, ferritic Fe-20Cr-5Al (FeCrAl) and APMT (TM) alloys, and silicon carbide (SiC)-based materials were considered and compared with Zircaloy-4. SCALE 6.1 was used to analyze the associated neutronics penalty/advantage, changes in reactivity coefficients, and spectral variations once a transition in the cladding was made. In the cases examined, materials containing higher absorbing isotopes invoked a reduction in reactivity due to an increase in neutron absorption in the cladding. Higher absorbing materials produced a harder neutron spectrum in the fuel pellet, leading to a slight increase in plutonium production. A parametric study determined the geometric conditions required to match cycle length requirements for each alternate cladding material in a PWR. A method for estimating the end of cycle reactivity was implemented to compare each model to that of standard Zircaloy-4 cladding. By using a thinner cladding of 350 mu m and keeping a constant outer diameter, austenitic stainless steels require an increase of no more than 0.5 wt% enriched U-235 to match fuel cycle requirements, while the required increase for FeCrAl was about 0.1%. When modeling SiC (with slightly lower thermal absorption properties than that of Zircaloy), a standard cladding thickness could be implemented with marginally less enriched uranium (similar to 0.1%). Moderator temperature and void coefficients were calculated throughout the depletion cycle. Nearly identical reactivity responses were found when coolant temperature and void properties were perturbed for each cladding material. By splitting the pellet into 10 equal areal sections, relative fission power as a function of radius was found to be similar for each cladding material. FeCrAl and 310SS cladding have a slightly higher fission power near the pellet's periphery due to the harder neutron spectrum in the system, causing more Pu-239 breeding. An economic assessment calculated the change in fuel pellet production costs for use of each cladding. Implementing FeCrAl alloys would increase fuel pellet production costs about 15% because of increased U-235 enrichment and the additional UO2 pellet volume enabled by using thinner cladding. (C) 2014 Elsevier Ltd. All rights reserved. C1 [George, Nathan Michael; Maldonado, Ivan] Univ Tennessee, Dept Nucl Engn, Knoxville, TN 37996 USA. [Terrani, Kurt] Oak Ridge Natl Lab, Fus & Mat Nucl Syst Div, Oak Ridge, TN 37831 USA. [Powers, Jeff; Worrall, Andrew] Oak Ridge Natl Lab, Reactor & Nucl Syst Div, Oak Ridge, TN 37831 USA. RP George, NM (reprint author), 238 South Purdue Ave, Oak Ridge, TN 37830 USA. EM ngeorge3@utk.edu OI Worrall, Andrew/0000-0003-1580-766X; Powers, Jeffrey/0000-0003-3653-3880 FU Advanced Fuels Campaign of the Fuel Cycle R&D program in the Office of Nuclear Energy, US Department of Energy; U.S. Department of Energy [DE-AC05-00OR22725] FX The aid and technical insight of Jess Gehin and Andrew Godfrey at Oak Ridge National Laboratory are gratefully acknowledged. The work presented in this paper was supported by the Advanced Fuels Campaign of the Fuel Cycle R&D program in the Office of Nuclear Energy, US Department of Energy. This manuscript has been authored by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. NR 30 TC 16 Z9 16 U1 3 U2 47 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0306-4549 J9 ANN NUCL ENERGY JI Ann. Nucl. Energy PD JAN PY 2015 VL 75 BP 703 EP 712 DI 10.1016/j.anucene.2014.09.005 PG 10 WC Nuclear Science & Technology SC Nuclear Science & Technology GA AY3OS UT WOS:000347493400084 ER PT J AU Fiel, JCB da Silva, FC Martinez, AS Leal, LC AF Batista Fiel, Joao Claudio da Silva, Fernando Carvalho Martinez, Aquilino Senra Leal, Luiz C. TI Parameterized representation of macroscopic cross section for PWR reactor SO ANNALS OF NUCLEAR ENERGY LA English DT Article DE Cross-section; Parameterized cross-sections; Chebyshev polynomials; Fuel burnup ID REGRESSION AB The purpose of this work is to describe, by means of Chebyshev polynomials, a parameterized representation of the homogenized macroscopic cross section for PWR fuel element as a function of soluble boron concentration, moderator temperature, fuel temperature, moderator density and U-235(92) enrichment. The cross-section data analyzed are fission, scattering, total, transport, absorption and capture. The parameterization enables a quick and easy determination of problem-dependent cross-sections to be used in few group calculations. The methodology presented in this paper will allow generation of group cross-section data from stored polynomials to perform PWR core calculations without the need to generate them based on computer code calculations using standard steps. The results obtained by the proposed methodology when compared with results from the SCALE code calculations show very good agreement. (C) 2014 Published by Elsevier Ltd. C1 [Batista Fiel, Joao Claudio] Mil Inst Engn, Dept Nucl Engn, Rio De Janeiro, Brazil. [da Silva, Fernando Carvalho; Martinez, Aquilino Senra] Univ Fed Rio de Janeiro, COPPE, Dept Nucl Engn, BR-21945 Rio De Janeiro, Brazil. [Leal, Luiz C.] Oak Ridge Natl Lab, Reactor & Nucl Syst Div, Oak Ridge, TN 37831 USA. RP Fiel, JCB (reprint author), Mil Inst Engn, Dept Nucl Engn, Praca Gen Tibucio,80 Praia Vermelha Urca, Rio De Janeiro, Brazil. NR 10 TC 0 Z9 0 U1 0 U2 2 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0306-4549 J9 ANN NUCL ENERGY JI Ann. Nucl. Energy PD JAN PY 2015 VL 75 BP 736 EP 741 DI 10.1016/j.anucene.2014.07.037 PG 6 WC Nuclear Science & Technology SC Nuclear Science & Technology GA AY3OS UT WOS:000347493400088 ER PT J AU Gibbons, SM Schwartz, T Fouquier, J Mitchell, M Sangwan, N Gilbert, JA Kelley, ST AF Gibbons, Sean M. Schwartz, Tara Fouquier, Jennifer Mitchell, Michelle Sangwan, Naseer Gilbert, Jack A. Kelley, Scott T. TI Ecological Succession and Viability of Human-Associated Microbiota on Restroom Surfaces SO APPLIED AND ENVIRONMENTAL MICROBIOLOGY LA English DT Article ID BACTERIAL COMMUNITY; VAGINAL MICROBIOME; ENVIRONMENT; DIVERSITY; SEQUENCES; VIRUSES; DESIGN; WOMEN AB Human-associated bacteria dominate the built environment (BE). Following decontamination of floors, toilet seats, and soap dispensers in four public restrooms, in situ bacterial communities were characterized hourly, daily, and weekly to determine their successional ecology. The viability of cultivable bacteria, following the removal of dispersal agents (humans), was also assessed hourly. A late-successional community developed within 5 to 8 h on restroom floors and showed remarkable stability over weeks to months. Despite late-successional dominance by skin- and outdoor-associated bacteria, the most ubiquitous organisms were predominantly gut-associated taxa, which persisted following exclusion of humans. Staphylococcus represented the majority of the cultivable community, even after several hours of human exclusion. Methicillin-resistant Staphylococcus aureus (MRSA)-associated virulence genes were found on floors but were not present in assembled Staphylococcus pan-genomes. Viral abundances, which were predominantly enterophages, human papilloma virus, and herpesviruses, were significantly correlated with bacterial abundances and showed an unexpectedly low virus-to-bacterium ratio in surface-associated samples, suggesting that bacterial hosts are mostly dormant on BE surfaces. C1 [Gibbons, Sean M.] Univ Chicago, Grad Program Biophys Sci, Chicago, IL 60637 USA. [Gibbons, Sean M.; Sangwan, Naseer; Gilbert, Jack A.] Argonne Natl Lab, Inst Genom & Syst Biol, Argonne, IL 60439 USA. [Schwartz, Tara; Fouquier, Jennifer; Mitchell, Michelle; Kelley, Scott T.] San Diego State Univ, Dept Biol, San Diego, CA 92182 USA. [Fouquier, Jennifer] San Diego State Univ, Grad Program Bioinformat & Med Informat, San Diego, CA 92182 USA. [Gilbert, Jack A.] Univ Chicago, Dept Ecol & Evolut, Chicago, IL 60637 USA. [Gilbert, Jack A.] Marine Biol Lab, Woods Hole, MA 02543 USA. [Gilbert, Jack A.] Zhejiang Univ, Coll Environm & Resource Sci, Hangzhou 310003, Zhejiang, Peoples R China. RP Gilbert, JA (reprint author), Argonne Natl Lab, Inst Genom & Syst Biol, 9700 S Cass Ave, Argonne, IL 60439 USA. EM gilbertjack@anl.gov OI Gibbons, Sean/0000-0002-8724-7916 FU EPA STAR Graduate Fellowship; National Institutes of Health Training Grant [5T-32EB-009412]; Alfred P. Sloan Foundation's Microbiology of the Built Environment Program FX S.M.G. was supported by an EPA STAR Graduate Fellowship and the National Institutes of Health Training Grant 5T-32EB-009412. We acknowledge funding from the Alfred P. Sloan Foundation's Microbiology of the Built Environment Program. This work was completed in part with resources provided by the University of Chicago Research Computing Center. NR 39 TC 16 Z9 16 U1 2 U2 39 PU AMER SOC MICROBIOLOGY PI WASHINGTON PA 1752 N ST NW, WASHINGTON, DC 20036-2904 USA SN 0099-2240 EI 1098-5336 J9 APPL ENVIRON MICROB JI Appl. Environ. Microbiol. PD JAN PY 2015 VL 81 IS 2 BP 765 EP 773 DI 10.1128/AEM.03117-14 PG 9 WC Biotechnology & Applied Microbiology; Microbiology SC Biotechnology & Applied Microbiology; Microbiology GA AY1UL UT WOS:000347377500032 PM 25398865 ER PT J AU Xu, N Kuhn, K Gallimore, D Martinez, A Schappert, M Montoya, D Lujan, E Garduno, K Tandon, L AF Xu, N. Kuhn, K. Gallimore, D. Martinez, A. Schappert, M. Montoya, D. Lujan, E. Garduno, K. Tandon, L. TI Elemental composition in sealed plutonium-beryllium neutron sources SO APPLIED RADIATION AND ISOTOPES LA English DT Article DE Sealed PuBe neutron source; ICP-MS; ICP-AES; Plutonium assay; Beryllium assay; Trace elements ID ICP-MS; NEPTUNIUM; ASSAY AB Five sealed plutonium-beryllium (PuBe) neutron sources from various manufacturers were disassembled. Destructive chemical analyses for recovered PuBe materials were conducted for disposition purposes. A dissolution method for PuBe alloys was developed for quantitative plutonium (Pu) and beryllium (Be) assay. Quantitation of Be and trace elements was performed using plasma based spectroscopic instruments, namely inductively coupled plasma mass spectrometry (ICP-MS) and atomic emission spectrometry (ICP-AES). Pu assay was accomplished by an electrochemical method. Variations in trace elemental contents among the five PuBe sources are discussed. (C) 2014 Elsevier Ltd. All rights reserved. C1 [Xu, N.; Kuhn, K.; Gallimore, D.; Martinez, A.; Schappert, M.; Montoya, D.; Lujan, E.; Garduno, K.; Tandon, L.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Xu, N (reprint author), Los Alamos Natl Lab, POB 1663,G740, Los Alamos, NM 87545 USA. EM ningxu@lanl.gov FU Department of Homeland Security, Domestic Nuclear Detection Office [IAA HSHQDC-14-X-00028] FX The authors would like to thank the Department of Homeland Security, Domestic Nuclear Detection Office (Grant no. IAA HSHQDC-14-X-00028) for funding the project, and Andres Borrego for assisting in the sample preparation work. This publication is LA-UR-14-21135. NR 18 TC 5 Z9 5 U1 4 U2 16 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0969-8043 J9 APPL RADIAT ISOTOPES JI Appl. Radiat. Isot. PD JAN PY 2015 VL 95 BP 85 EP 89 DI 10.1016/j.apradiso.2014.10.013 PG 5 WC Chemistry, Inorganic & Nuclear; Nuclear Science & Technology; Radiology, Nuclear Medicine & Medical Imaging SC Chemistry; Nuclear Science & Technology; Radiology, Nuclear Medicine & Medical Imaging GA AY5AF UT WOS:000347585200014 ER PT J AU Pauvolid-Correa, A Solberg, O Couto-Lima, D Kenney, J Serra-Freire, N Brault, A Nogueira, R Langevin, S Komar, N AF Pauvolid-Correa, Alex Solberg, Owen Couto-Lima, Dinair Kenney, Joan Serra-Freire, Nicolau Brault, Aaron Nogueira, Rita Langevin, Stanley Komar, Nicholas TI Nhumirim virus, a novel flavivirus isolated from mosquitoes from the Pantanal, Brazil SO ARCHIVES OF VIROLOGY LA English DT Article ID WEST NILE VIRUS; ARBOVIRUS DISEASE; ILHEUS VIRUS; ROCIO VIRUS; CULEX; IDENTIFICATION; EMERGENCE; GENOME; TICKS AB We describe the isolation of a novel flavivirus, isolated from a pool of mosquitoes identified as Culex (Culex) chidesteri collected in 2010 in the Pantanal region of west-central Brazil. The virus is herein designated Nhumirim virus (NHUV) after the name of the ranch from which the mosquito pool was collected. Flavivirus RNA was detected by real-time RT-PCR of homogenized mosquitoes and from the corresponding C6/36 culture supernatant. Based on full-genome sequencing, the virus isolate was genetically distinct from but most closely related to Barkedji virus (BJV), a newly described flavivirus from Senegal. Phylogenetic analysis demonstrated that NHUV grouped with mosquito-borne flaviviruses forming a clade with BJV. This clade may be genetically intermediate between the Culex-borne flaviviruses amplified by birds and the insect-only flaviviruses. C1 [Couto-Lima, Dinair; Nogueira, Rita] Minist Saude, Fundacao Oswaldo Cruz, Inst Oswaldo Cruz, Lab Flavivirus, Rio De Janeiro, RJ, Brazil. [Pauvolid-Correa, Alex; Kenney, Joan; Brault, Aaron; Komar, Nicholas] Ctr Dis Control & Prevent, Div Vector Borne Dis, Ft Collins, CO USA. [Solberg, Owen; Langevin, Stanley] Sandia Natl Labs, Dept Syst Biol, Livermore, CA USA. [Serra-Freire, Nicolau] Minist Saude, Fundacao Oswaldo Cruz, Lab Referencia Nacl Vetores Riquetsioses, Rio De Janeiro, RJ, Brazil. RP Pauvolid-Correa, A (reprint author), Minist Saude, Fundacao Oswaldo Cruz, Inst Oswaldo Cruz, Lab Flavivirus, Rio De Janeiro, RJ, Brazil. EM pauvolid@ioc.fiocruz.br FU ASM; CNPq; CAPES; Fulbright; CDC; FIOCRUZ; FAPERJ FX Special thanks to Zilca Campos from Embrapa Pantanal for her important contribution to this work. We thank Kristy Burkalther, Janae Stovall, Karen Burroughs and Robert Lanciotti from CDC, who provided laboratory assistance. We thank Thierry Tomich, Marcia Furlan, Marcos Tadeu and all staff from Embrapa Pantanal. Special thanks to Helcio Reinaldo Gil-Santana from Diptera Laboratory of FIOCRUZ, and Luiz Pellegrin of Geoprocessing Laboratory of Embrapa Pantanal. Financial support: ASM, CNPq, CAPES, Fulbright, CDC, FIOCRUZ, FAPERJ. NR 46 TC 4 Z9 4 U1 2 U2 8 PU SPRINGER WIEN PI WIEN PA SACHSENPLATZ 4-6, PO BOX 89, A-1201 WIEN, AUSTRIA SN 0304-8608 EI 1432-8798 J9 ARCH VIROL JI Arch. Virol. PD JAN PY 2015 VL 160 IS 1 BP 21 EP 27 DI 10.1007/s00705-014-2219-8 PG 7 WC Virology SC Virology GA AY2FE UT WOS:000347403200003 PM 25252815 ER PT J AU Huang, ZH Fu, JN Zong, WK Wang, LZ Lucas, MM Wang, LF Michael, CBA Cui, XQ Feng, LL Gong, XF Jon, SL Liu, Q Daniel, LV Carl, RP Yang, HG Yuan, XY Donald, GY Zhou, X Zhu, ZX Zhu, ZH AF Huang Zhihua Fu Jianning Zong Weikai Wang Lingzhi Lucas, Macri M. Wang Lifan Michael, Ashley C. B. Cui Xiangqun Feng Long-Long Gong Xuefei Jon, Lawrence S. Liu Qiang Daniel, Luong-Van Carl, Pennypacker R. Yang Huigen Yuan Xiangyan Donald, York G. Zhou Xu Zhu Zhenxi Zhu Zonghong TI PULSATIONS AND PERIOD CHANGES OF THE NON-BLAZHKO RR LYRAE VARIABLE Y OCT OBSERVED FROM DOME A, ANTARCTICA SO ASTRONOMICAL JOURNAL LA English DT Article DE stars: individual (Y Oct); stars: variables: RR Lyrae; techniques: photometric ID ULTRAVIOLET RADIAL-VELOCITIES; SPECTROSCOPIC BINARY ORBITS; BASE-LINE INTERFEROMETRY; CYGNUS OB2 ASSOCIATION; MASSIVE STAR-FORMATION; FINE GUIDANCE SENSOR; O-TYPE STARS; GALACTIC O; SPECKLE INTERFEROMETRY; MAGELLANIC CLOUDS AB During the operation of the Chinese Small Telescope Array (CSTAR) in Dome A of Antarctica in the years 2008, 2009, and 2010, large amounts of photometric data have been obtained for variable stars in the CSTAR field. We present here the study of one of six RR Lyrae variables, Y Oct, observed with CSTAR in Dome A, Antarctica. Photometric data in the i band were obtained in 2008 and 2010, with a duty cycle (defined as the fraction of time representing scientifically available data to CSTAR observation time) of about 44% and 52%, respectively. In 2009, photometric data in the g and r bands were gathered for this star, with a duty cycle of 65% and 60%, respectively. Fourier analysis of the data in the three bands only shows the fundamental frequency and its harmonics, which is characteristic of the non-Blazhko RR Lyrae variables. Values of the fundamental frequency and the amplitudes, as well as the total pulsation amplitude, are obtained from the data in the three bands separately. The amplitude of the fundamental frequency and the total pulsation amplitude in the g band are the largest, and those in the i band the smallest. Two-hundred fifty-one times of maximum are obtained from the three seasons of data, which are analyzed together with 38 maximum times provided in the GEOS RR Lyrae database. A period change rate of -0.96 +/- 0.07 days Myr(-1) is then obtained, which is a surprisingly large negative value. Based on relations available in the literature, the following physical parameters are derived: [Fe/H] = -1.41 +/- 0.14, MV = 0.696 +/- 0.014 mag, V - K = 1.182 +/- 0.028 mag, log T-eff = 3.802 +/- 0.003 K, log g = 2.705 +/- 0.004, logL/L-circle dot = 1.625 +/- 0.013, and logM/M-circle dot = -0.240 +/- 0.019. C1 [Huang Zhihua; Fu Jianning; Zong Weikai; Wang Lingzhi; Zhu Zonghong] Beijing Normal Univ, Dept Astron, Beijing 100875, Peoples R China. [Lucas, Macri M.; Wang Lifan] Texas A&M Univ, Mitchell Inst Fundamental Phys & Astron, Dept Phys & Astron, College Stn, TX USA. [Wang Lingzhi; Wang Lifan; Cui Xiangqun; Feng Long-Long; Gong Xuefei; Liu Qiang; Yang Huigen; Yuan Xiangyan; Zhou Xu; Zhu Zhenxi; Zhu Zonghong] Chinese Ctr Antarctic Astron, Nanjing, Jiangsu, Peoples R China. [Wang Lingzhi; Liu Qiang; Zhou Xu] Chinese Acad Sci, Natl Astron Observ, Beijing, Peoples R China. [Wang Lifan; Feng Long-Long; Zhu Zhenxi] Chinese Acad Sci, Purple Mt Observ, Nanjing, Jiangsu, Peoples R China. [Michael, Ashley C. B.; Jon, Lawrence S.; Daniel, Luong-Van] Univ New S Wales, Sch Phys, Sydney, NSW 2052, Australia. [Cui Xiangqun; Gong Xuefei; Yuan Xiangyan] Nanjing Inst Astron Opt & Technol, Nanjing, Jiangsu, Peoples R China. [Jon, Lawrence S.] Australian Astron Observ, N Ryde, NSW, Australia. [Carl, Pennypacker R.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Ctr Astrophys, Berkeley, CA 94720 USA. [Yang Huigen] Polar Res Inst China, Shanghai, Peoples R China. [Donald, York G.] Univ Chicago, Dept Astron & Astrophys, Chicago, IL 60637 USA. [Donald, York G.] Univ Chicago, Enrico Fermi Inst, Chicago, IL 60637 USA. RP Huang, ZH (reprint author), Beijing Normal Univ, Dept Astron, Beijing 100875, Peoples R China. EM jnfu@bnu.edu.cn OI Macri, Lucas/0000-0002-1775-4859 FU FGS work at Georgia State University; Space Telescope Science Institute; NASA [NAS5-26555]; GSU College of Arts and Sciences; Research Program Enhancement fund of the Board of Regents of the University System of Georgia; Spanish Government Ministerio de Economia y Competitividad (MINECO) [AYA2010-15 081, AYA2010-17 631]; Consejeria de Educacion of the Junta de Andalucia [P08-TIC-4075]; NSERC (Canada); FQRNT (Quebec); CRAQ (Quebec) FX We are grateful to Denise Taylor of STScI for her remarkably effective efforts that made these HST observations possible. We also thank John Subasavage, Sergio Dieterich, and Adric Riedel for their support of the FGS work at Georgia State University. Support for HST proposal numbers GO-11212, 11901, 11943, and 11944 was provided by NASA through a grant from the Space Telescope Science Institute, which is operated by the Association of Universities for Research in Astronomy, Incorporated, under NASA contract NAS5-26555. Institutional support has been provided from the GSU College of Arts and Sciences and from the Research Program Enhancement fund of the Board of Regents of the University System of Georgia, administered through the GSU Office of the Vice President for Research and Economic Development. J.M.A. acknowledges support from the Spanish Government Ministerio de Economia y Competitividad (MINECO) through grants AYA2010-15 081 and AYA2010-17 631 and the Consejeria de Educacion of the Junta de Andalucia through grant P08-TIC-4075. A.F.J.M. is grateful to NSERC (Canada) and FQRNT (Quebec) for financial assistance. N.D.R. gratefully acknowledges his CRAQ (Quebec) fellowship. This research has made use of the WDS Catalog maintained at the U.S. Naval Observatory and the WEBDA database, operated at the Institute for Astronomy of the University of Vienna. NR 88 TC 3 Z9 3 U1 2 U2 7 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 0004-6256 EI 1538-3881 J9 ASTRON J JI Astron. J. PD JAN PY 2015 VL 149 IS 1 AR 25 DI 10.1088/0004-6256/149/1/25 PG 20 WC Astronomy & Astrophysics SC Astronomy & Astrophysics GA AY0SY UT WOS:000347308300024 ER PT J AU Bundy, K Bershady, MA Law, DR Yan, RB Drory, N MacDonald, N Wake, DA Cherinka, B Sanchez-Gallego, JR Weijmans, AM Thomas, D Tremonti, C Masters, K Coccato, L Diamond-Stanic, AM Aragon-Salamanca, A Avila-Reese, V Badenes, C Falcon-Barroso, J Belfiore, F Bizyaev, D Blanc, GA Bland-Hawthorn, J Blanton, MR Brownstein, JR Byler, N Cappellari, M Conroy, C Dutton, AA Emsellem, E Etherington, J Frinchaboy, PM Fu, H Gunn, JE Harding, P Johnston, EJ Kauffmann, G Kinemuchi, K Klaene, MA Knapen, JH Leauthaud, A Li, C Lin, LW Maiolino, R Malanushenko, V Malanushenko, E Mao, S Maraston, C McDermid, RM Merrifield, MR Nichol, RC Oravetz, D Pan, K Parejko, JK Sanchez, SF Schlegel, D Simmons, A Steele, O Steinmetz, M Thanjavur, K Thompson, BA Tinker, JL van den Bosch, RCE Westfall, KB Wilkinson, D Wright, S Xiao, T Zhang, K AF Bundy, Kevin Bershady, Matthew A. Law, David R. Yan, Renbin Drory, Niv MacDonald, Nicholas Wake, David A. Cherinka, Brian Sanchez-Gallego, Jose R. Weijmans, Anne-Marie Thomas, Daniel Tremonti, Christy Masters, Karen Coccato, Lodovico Diamond-Stanic, Aleksandar M. Aragon-Salamanca, Alfonso Avila-Reese, Vladimir Badenes, Carles Falcon-Barroso, Jesus Belfiore, Francesco Bizyaev, Dmitry Blanc, Guillermo A. Bland-Hawthorn, Joss Blanton, Michael R. Brownstein, Joel R. Byler, Nell Cappellari, Michele Conroy, Charlie Dutton, Aaron A. Emsellem, Eric Etherington, James Frinchaboy, Peter M. Fu, Hai Gunn, James E. Harding, Paul Johnston, Evelyn J. Kauffmann, Guinevere Kinemuchi, Karen Klaene, Mark A. Knapen, Johan H. Leauthaud, Alexie Li, Cheng Lin, Lihwai Maiolino, Roberto Malanushenko, Viktor Malanushenko, Elena Mao, Shude Maraston, Claudia McDermid, Richard M. Merrifield, Michael R. Nichol, Robert C. Oravetz, Daniel Pan, Kaike Parejko, John K. Sanchez, Sebastian F. Schlegel, David Simmons, Audrey Steele, Oliver Steinmetz, Matthias Thanjavur, Karun Thompson, Benjamin A. Tinker, Jeremy L. van den Bosch, Remco C. E. Westfall, Kyle B. Wilkinson, David Wright, Shelley Xiao, Ting Zhang, Kai TI OVERVIEW OF THE SDSS-IV MaNGA SURVEY: MAPPING NEARBY GALAXIES AT APACHE POINT OBSERVATORY SO ASTROPHYSICAL JOURNAL LA English DT Article DE galaxies: evolution; galaxies: general; surveys; techniques: imaging spectroscopy ID DIGITAL SKY SURVEY; STAR-FORMING GALAXIES; OSCILLATION SPECTROSCOPIC SURVEY; STELLAR POPULATION GRADIENTS; INITIAL MASS FUNCTION; VIRUS-P EXPLORATION; EARLY DATA RELEASE; TO-LIGHT RATIO; SAURON PROJECT; SPECTRAL CLASSIFICATION AB We present an overview of a new integral field spectroscopic survey called MaNGA (Mapping Nearby Galaxies at Apache Point Observatory), one of three core programs in the fourth-generation Sloan Digital Sky Survey (SDSS-IV) that began on 2014 July 1. MaNGA will investigate the internal kinematic structure and composition of gas and stars in an unprecedented sample of 10,000 nearby galaxies. We summarize essential characteristics of the instrument and survey design in the context of MaNGA's key science goals and present prototype observations to demonstrate MaNGA's scientific potential. MaNGA employs dithered observations with 17 fiber-bundle integral field units that vary in diameter from 12 '' (19 fibers) to 32 '' (127 fibers). Two dual-channel spectrographs provide simultaneous wavelength coverage over 3600-10300 angstrom at R similar to 2000. With a typical integration time of 3 hr, MaNGA reaches a target r-band signal-to-noise ratio of 4-8 (angstrom(-1) per 2 '' fiber) at 23 AB mag arcsec(-2), which is typical for the outskirts of MaNGA galaxies. Targets are selected with M* greater than or similar to 10(9) M-circle dot using SDSS-I redshifts and i-band luminosity to achieve uniform radial coverage in terms of the effective radius, an approximately flat distribution in stellar mass, and a sample spanning a wide range of environments. Analysis of our prototype observations demonstrates MaNGA's ability to probe gas ionization, shed light on recent star formation and quenching, enable dynamical modeling, decompose constituent components, and map the composition of stellar populations. MaNGA's spatially resolved spectra will enable an unprecedented study of the astrophysics of nearby galaxies in the coming 6 yr. C1 [Bundy, Kevin; Leauthaud, Alexie] Univ Tokyo, Todai Inst Adv Study, Univ Kavli IPMU, Kavli Inst Phys & Math,WPI, Kashiwa, Chiba 2778583, Japan. [Bershady, Matthew A.; Wake, David A.; Tremonti, Christy; Diamond-Stanic, Aleksandar M.] Univ Wisconsin, Dept Astron, Madison, WI 53706 USA. [Law, David R.; Cherinka, Brian; Wright, Shelley] Univ Toronto, Dunlap Inst Astron & Astrophys, Toronto, ON M5S 3H4, Canada. [Yan, Renbin; Sanchez-Gallego, Jose R.; Zhang, Kai] Univ Kentucky, Dept Phys & Astron, Lexington, KY 40506 USA. [Drory, Niv] Univ Texas Austin, Dept Astron, McDonald Observ, Austin, TX 78712 USA. [MacDonald, Nicholas; Byler, Nell] Univ Washington, Dept Astron, Seattle, WA 98195 USA. [Weijmans, Anne-Marie] Univ St Andrews, Sch Phys & Astron, St Andrews KY16 9SS, Fife, Scotland. [Thomas, Daniel; Masters, Karen; Coccato, Lodovico; Etherington, James; Maraston, Claudia; Nichol, Robert C.; Steele, Oliver; Wilkinson, David] Univ Portsmouth, Inst Cosmol & Gravitat, Portsmouth, Hants, England. [Masters, Karen] South East Phys Network, SEPNet, Southampton SO17 1BJ, Hants, England. [Coccato, Lodovico; Emsellem, Eric] European So Observ, D-85748 Garching, Germany. [Aragon-Salamanca, Alfonso; Johnston, Evelyn J.; Merrifield, Michael R.] Univ Nottingham, Sch Phys & Astron, Nottingham NG7 2RD, England. [Avila-Reese, Vladimir; Sanchez, Sebastian F.] Univ Nacl Autonoma Mexico, Inst Astron, Mexico City 04510, DF, Mexico. [Badenes, Carles] Univ Pittsburgh, Astrophys & Cosmol Ctr PITT PACC, Dept Phys & Astron & Pittsburgh Particle Phys, Pittsburgh, PA 15260 USA. [Falcon-Barroso, Jesus; Knapen, Johan H.] Inst Astrofis Canarias, E-38200 Tenerife, Spain. [Belfiore, Francesco; Maiolino, Roberto] Univ Cambridge, Cavendish Lab, Cambridge CB3 0HE, England. [Belfiore, Francesco] Univ Cambridge, Kavli Inst Cosmol, Cambridge CB3 0HA, England. [Bizyaev, Dmitry; Kinemuchi, Karen; Klaene, Mark A.; Malanushenko, Viktor; Malanushenko, Elena; Oravetz, Daniel; Pan, Kaike; Simmons, Audrey] Apache Point Observ & New Mexico State, Sunspot, NM 88349 USA. [Blanc, Guillermo A.] Observ Carnegie Inst Sci, Pasadena, CA USA. [Bland-Hawthorn, Joss] Univ Sydney, Sch Phys, Sydney Inst Astron SIfA, Sydney, NSW 2006, Australia. [Brownstein, Joel R.] Univ Utah, Dept Phys & Astron, Salt Lake City, UT 84112 USA. [Cappellari, Michele] Univ Oxford, Dept Phys, Sub Dept Astrophys, Oxford OX1 3RH, England. [Conroy, Charlie] Univ Calif Santa Cruz, Dept Astron & Astrophys, Santa Cruz, CA 95064 USA. [Dutton, Aaron A.; van den Bosch, Remco C. E.] Max Planck Inst Astron, D-69117 Heidelberg, Germany. [Emsellem, Eric] Univ Lyon 1, Observ Lyon, Ctr Rech Astrophys Lyon, F-69561 St Genis Laval, France. [Emsellem, Eric] Ecole Normale Super Lyon, F-69230 St Genis Laval, France. [Frinchaboy, Peter M.; Thompson, Benjamin A.] Texas Christian Univ, Dept Phys & Astron, Ft Worth, TX 76129 USA. [Fu, Hai] Univ Iowa, Dept Phys & Astron, Iowa City, IA 52242 USA. [Gunn, James E.] Princeton Univ, Dept Astrophys Sci, Princeton, NJ 08544 USA. [Harding, Paul] Case Western Reserve Univ, Dept Astron, Cleveland, OH 44106 USA. [Kauffmann, Guinevere] Max Planck Inst Astrophys, D-85748 Garching, Germany. [Knapen, Johan H.] Univ La Laguna, Dept Astrofis, E-38206 San Cristobal la Laguna, Spain. [Li, Cheng; Xiao, Ting] Shanghai Astron Observ, Shanghai 200030, Peoples R China. [Lin, Lihwai] Acad Sinica, Inst Astron & Astrophys, Taipei 106, Taiwan. [Mao, Shude] Natl Astron Observ China, Beijing 100012, Peoples R China. [Mao, Shude] Univ Manchester, Jodrell Bank Ctr Astrophys, Manchester M13 9PL, Lancs, England. [McDermid, Richard M.] Macquarie Univ, Dept Phys & Astron, Sydney, NSW 2109, Australia. [McDermid, Richard M.] Australian Astron Observ, Australian Gemini Off, Sydney, NSW 1670, Australia. [Parejko, John K.] Yale Univ, Dept Phys, New Haven, CT 06520 USA. [Schlegel, David] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Phys, Berkeley, CA 94720 USA. [Steinmetz, Matthias] Leibniz Inst Astrophys Potsdam AIP, D-14482 Potsdam, Germany. [Thanjavur, Karun] Univ Victoria, Dept Phys & Astron, Victoria, BC V8P 5C2, Canada. [Westfall, Kyle B.] Univ Groningen, Kapteyn Astron Inst, NL-9747 AD Groningen, Netherlands. [Wright, Shelley] Univ Toronto, Dept Astron & Astrophys, Toronto, ON M5S 3H4, Canada. RP Bundy, K (reprint author), Univ Tokyo, Todai Inst Adv Study, Univ Kavli IPMU, Kavli Inst Phys & Math,WPI, Kashiwa, Chiba 2778583, Japan. RI Blanc, Guillermo/I-5260-2016; Xiao, Ting/Q-1022-2016; OI Merrifield, Michael/0000-0002-4202-4727; Aragon-Salamanca, Alfonso/0000-0001-8215-1256; van den Bosch, Remco/0000-0002-0420-6159; Cappellari, Michele/0000-0002-1283-8420 FU Alfred P. Sloan Foundation; National Science Foundation; U.S. Department of Energy Office of Science; Carnegie Mellon University; Colorado University; Boulder; Harvard-Smithsonian Center for Astrophysics Participation Group; Johns Hopkins University; Kavli Institute for the Physics and Mathematics of the Universe; Max-Planck-Institut fuer Astrophysik (MPA Garching); Max-Planck-Institut fuer Extraterrestrische Physik (MPE); Max-Planck-Institut fuer Astronomic (MPIA Heidelberg); National Astronomical Observatories of China; New Mexico State University; New York University; Ohio State University; Penn State University; Shanghai Astronomical Observatory; United Kingdom Participation Group; University of Portsmouth; University of Utah; University of Wisconsin; Yale University; World Premier International Research Center Initiative (WPI Initiative), MEXT, Japan; People Programme (Marie Curie Actions) of the European Union's Seventh Framework Programme FP7 under REA [PITN-GA-2011-289313]; Strategic Priority Research Program "The Emergence of Cosmological Structures" of the Chinese Academy of Sciences [XDB09000000]; National Natural Science Foundation of China (NSFC) [11333003]; Royal Society University Research Fellowship; Sloan Foundation; Packard Foundation; Grainger Foundation FX We are grateful for careful comments on the manuscript by Don Schneider and input from the SAMI, CALIFA, and ATLAS3D teams. We also thank Adam Bolton, Stephane Courteau, Natascha Forster-Schreiber, Bruce Gillespie, Gary Hill, Arlette Pecontal, Rob Sharp, Ray Sharples, and Dennis Zaritsky for valuable feedback on the MaNGA instrumentation and survey design. Funding for SDSS-III and SDSS-IV has been provided by the Alfred P. Sloan Foundation and Participating Institutions. Additional funding for SDSS-III comes from the National Science Foundation and the U.S. Department of Energy Office of Science. Further information about both projects is available at www.sdss.org.; The Participating Institutions in SDSS-IV are Carnegie Mellon University, Colorado University, Boulder, Harvard-Smithsonian Center for Astrophysics Participation Group, Johns Hopkins University, Kavli Institute for the Physics and Mathematics of the Universe, Max-Planck-Institut fuer Astrophysik (MPA Garching), Max-Planck-Institut fuer Extraterrestrische Physik (MPE), Max-Planck-Institut fuer Astronomic (MPIA Heidelberg), National Astronomical Observatories of China, New Mexico State University, New York University, The Ohio State University, Penn State University, Shanghai Astronomical Observatory, United Kingdom Participation Group, University of Portsmouth, University of Utah, University of Wisconsin, and Yale University.; This work was supported in part by a World Premier International Research Center Initiative (WPI Initiative), MEXT, Japan. J.H.K. acknowledges financial support to the DAGAL network from the People Programme (Marie Curie Actions) of the European Union's Seventh Framework Programme FP7/2007-2013/under REA grant agreement no. PITN-GA-2011-289313. This work has also been supported by the Strategic Priority Research Program "The Emergence of Cosmological Structures" of the Chinese Academy of Sciences Grant No. XDB09000000 (S.M., C.L.) and by the National Natural Science Foundation of China (NSFC) under grant no. 11333003 (S.M.). M.C. acknowledges support from a Royal Society University Research Fellowship. C.C. acknowledges support from the Sloan and Packard Foundations. A.M.D. acknowledges support from The Grainger Foundation. NR 108 TC 135 Z9 136 U1 8 U2 24 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 0004-637X EI 1538-4357 J9 ASTROPHYS J JI Astrophys. J. PD JAN 1 PY 2015 VL 798 IS 1 AR 7 DI 10.1088/0004-637X/798/1/7 PG 24 WC Astronomy & Astrophysics SC Astronomy & Astrophysics GA AX9TO UT WOS:000347245100007 ER PT J AU Chilcote, J Barman, T Fitzgerald, MP Graham, JR Larkin, JE Macintosh, B Bauman, B Burrows, AS Cardwell, A De Rosa, RJ Dillon, D Doyon, R Dunn, J Erikson, D Gavel, D Goodsell, SJ Hartung, M Hibon, P Ingraham, P Kalas, P Konopacky, Q Maire, J Marchis, F Marley, MS Marois, C Millar-Blanchaer, M Morzinski, K Norton, A Oppenheimer, R Palmer, D Patience, J Perrin, M Poyneer, L Pueyo, L Rantakyro, FT Sadakuni, N Saddlemyer, L Savransky, D Serio, A Sivaramakrishnan, A Song, I Soummer, R Thomas, S Wallace, JK Wiktorowicz, S Wolff, S AF Chilcote, Jeffrey Barman, Travis Fitzgerald, Michael P. Graham, James R. Larkin, James E. Macintosh, Bruce Bauman, Brian Burrows, Adam S. Cardwell, Andrew De Rosa, Robert J. Dillon, Daren Doyon, Rene Dunn, Jennifer Erikson, Darren Gavel, Donald Goodsell, Stephen J. Hartung, Markus Hibon, Pascale Ingraham, Patrick Kalas, Paul Konopacky, Quinn Maire, Jerome Marchis, Franck Marley, Mark S. Marois, Christian Millar-Blanchaer, Max Morzinski, Katie Norton, Andrew Oppenheimer, Rebecca Palmer, David Patience, Jennifer Perrin, Marshall Poyneer, Lisa Pueyo, Laurent Rantakyroe, Fredrik T. Sadakuni, Naru Saddlemyer, Leslie Savransky, Dmitry Serio, Andrew Sivaramakrishnan, Anand Song, Inseok Soummer, Remi Thomas, Sandrine Wallace, J. Kent Wiktorowicz, Sloane Wolff, Schuyler TI THE FIRST H-BAND SPECTRUM OF THE GIANT PLANET beta PICTORIS b SO ASTROPHYSICAL JOURNAL LETTERS LA English DT Article DE infrared: general; instrumentation: adaptive optics; planetary systems; stars: individual (beta Pictoris); techniques: spectroscopic ID DWARF CANDIDATE MEMBER; DIRECTLY IMAGED PLANET; LOW-MASS STARS; BROWN DWARFS; DUST DISK; CONFIRMATION; ATMOSPHERE; EXOPLANET; SPECTROSCOPY; ASYMMETRIES AB Using the recently installed Gemini Planet Imager (GPI), we have obtained the first H-band spectrum of the planetary companion to the nearby young star beta Pictoris. GPI is designed to image and provide low-resolution spectra of Jupiter-sized, self-luminous planetary companions around young nearby stars. These observations were taken covering the H band (1.65 mu m). The spectrum has a resolving power of similar to 45 and demonstrates the distinctive triangular shape of a cool substellar object with low surface gravity. Using atmospheric models, we find an effective temperature of 1600-1700K and a surface gravity of log(g) = 3.5-4.5 (cgs units). These values agree well with "hot-start" predictions from planetary evolution models for a gas giant with mass between 10 and 12 M-Jup and age between 10 and 20 Myr. C1 [Chilcote, Jeffrey; Fitzgerald, Michael P.; Larkin, James E.] Univ Calif Los Angeles, Dept Phys & Astron, Los Angeles, CA 90095 USA. [Chilcote, Jeffrey; Konopacky, Quinn; Maire, Jerome; Millar-Blanchaer, Max] Univ Toronto, Dunlap Inst Astron & Astrophys, Toronto, ON M5S 3H4, Canada. [Barman, Travis] Univ Arizona, Lunar & Planetary Lab, Tucson, AZ 85721 USA. [Graham, James R.; Kalas, Paul] Univ Calif Berkeley, Dept Astron, Berkeley, CA 94720 USA. [Macintosh, Bruce; Ingraham, Patrick] Stanford Univ, Kavli Inst Particle Astrophys & Cosmol, Stanford, CA 94305 USA. [Macintosh, Bruce; Bauman, Brian; Palmer, David; Poyneer, Lisa] Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. [Burrows, Adam S.] Princeton Univ, Dept Astrophys Sci, Princeton, NJ 08544 USA. [Cardwell, Andrew; Hartung, Markus; Hibon, Pascale; Rantakyroe, Fredrik T.; Sadakuni, Naru; Serio, Andrew] Gemini Observ, La Serena, Chile. [De Rosa, Robert J.; Patience, Jennifer] Arizona State Univ, Sch Earth & Space Explorat, Tempe, AZ 85287 USA. [De Rosa, Robert J.] Univ Exeter, Coll Engn Math & Phys Sci, Sch Phys, Exeter EX4 4QL, Devon, England. [Dillon, Daren; Gavel, Donald; Norton, Andrew] Univ Calif Santa Cruz, Univ Calif Observ, Lick Observ, Santa Cruz, CA 95064 USA. [Doyon, Rene] Univ Montreal, Observ Mt Megant, Montreal, PQ H3T 1J4, Canada. [Doyon, Rene] Univ Montreal, Dept Phys, Montreal, PQ H3T 1J4, Canada. [Dunn, Jennifer; Erikson, Darren; Marois, Christian; Saddlemyer, Leslie] Natl Res Council Canada Herzberg, Victoria, BC V9E 2E7, Canada. [Goodsell, Stephen J.] Gemini Observ, Hilo, HI 96720 USA. [Marchis, Franck] SETI Inst, Carl Sagan Ctr, Mountain View, CA 94043 USA. [Marley, Mark S.; Thomas, Sandrine] NASA, Ames Res Ctr, Mountain View, CA 94035 USA. [Morzinski, Katie] Univ Arizona, Steward Observ, Tucson, AZ 85721 USA. [Oppenheimer, Rebecca; Sivaramakrishnan, Anand] Amer Museum Nat Hist, Dept Astrophys, New York, NY 10024 USA. [Perrin, Marshall; Pueyo, Laurent; Sivaramakrishnan, Anand; Soummer, Remi] Space Telescope Sci Inst, Baltimore, MD 21218 USA. [Savransky, Dmitry] Cornell Univ, Sibley Sch Mech & Aerosp Engn, Ithaca, NY 14853 USA. [Song, Inseok] Univ Georgia, Dept Phys & Astron, Athens, GA 30602 USA. [Wallace, J. Kent] CALTECH, Jet Prop Lab, Pasadena, CA 91125 USA. [Wiktorowicz, Sloane] Univ Calif Santa Cruz, Dept Astron, Santa Cruz, CA 95064 USA. [Wolff, Schuyler] Johns Hopkins Univ, Dept Phys & Astron, Baltimore, MD 21218 USA. RP Chilcote, J (reprint author), Univ Calif Los Angeles, Dept Phys & Astron, Los Angeles, CA 90095 USA. EM jchilcote@astro.ucla.edu RI Fitzgerald, Michael/C-2642-2009; Savransky, Dmitry/M-1298-2014; OI Fitzgerald, Michael/0000-0002-0176-8973; Savransky, Dmitry/0000-0002-8711-7206; Oppenheimer, Rebecca/0000-0001-7130-7681 FU Gemini Observatory; NSF Center for Adaptive Optics at UC Santa Cruz; NSF [AST-0909188, AST-1211562, AST-1405505]; NASA [NNX11AD21G, NNX10AH31G, NNX14AC21G]; University of California Office of the President [LFRP-118057]; Science and Technology Facilities Council [ST/H002707/1]; Dunlap Institute, University of Toronto; U.S. Department of Energy by Lawrence Livermore National Laboratory [DE-AC52-07NA27344]; California Institute of Technology/Jet Propulsion Laboratory; NASA Exoplanet Science Institute FX The authors acknowledge the financial support of the Gemini Observatory, the NSF Center for Adaptive Optics at UC Santa Cruz, the NSF (AST-0909188; AST-1211562, AST-1405505), NASA Origins (NNX11AD21G; NNX10AH31G, NNX14AC21G), the University of California Office of the President (LFRP-118057), the Science and Technology Facilities Council (ST/H002707/1), and the Dunlap Institute, University of Toronto. Portions of this work were performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344 and under contract with the California Institute of Technology/Jet Propulsion Laboratory funded by NASA through the Sagan Fellowship Program executed by the NASA Exoplanet Science Institute. We are indebted to the international team of engineers and scientists who worked to make GPI a reality. NR 47 TC 17 Z9 17 U1 0 U2 6 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 2041-8205 EI 2041-8213 J9 ASTROPHYS J LETT JI Astrophys. J. Lett. PD JAN 1 PY 2015 VL 798 IS 1 AR L3 DI 10.1088/2041-8205/798/1/L3 PG 5 WC Astronomy & Astrophysics SC Astronomy & Astrophysics GA AY3CN UT WOS:000347462300003 ER PT J AU Yang, H Apai, D Marley, MS Saumon, D Morley, CV Buenzli, E Artigau, E Radigan, J Metchev, S Burgasser, AJ Mohanty, S Lowrance, PJ Showman, AP Karalidi, T Flateau, D Heinze, AN AF Yang, Hao Apai, Daniel Marley, Mark S. Saumon, Didier Morley, Caroline V. Buenzli, Esther Artigau, Etienne Radigan, Jacqueline Metchev, Stanimir Burgasser, Adam J. Mohanty, Subhanjoy Lowrance, Patrick J. Showman, Adam P. Karalidi, Theodora Flateau, Davin Heinze, Aren N. TI HST ROTATIONAL SPECTRAL MAPPING OF TWO L-TYPE BROWN DWARFS: VARIABILITY IN AND OUT OF WATER BANDS INDICATES HIGH-ALTITUDE HAZE LAYERS SO ASTROPHYSICAL JOURNAL LETTERS LA English DT Article DE brown dwarfs; stars: atmospheres; stars: individual (2MASS J18212815+1414010, 2MASS J15074769-1627386, 2MASS J01365662+0933473); stars: low-mass ID VERY-LOW MASS; T DWARFS; EVOLVING WEATHER; I. DETECTION; ATMOSPHERES; TRANSITION; DUST; PLANETS; PATCHY; CLOUDS AB We present time-resolved near-infrared spectroscopy of two L5 dwarfs, 2MASS J18212815+1414010 and 2MASS J15074759-1627386, observed with the Wide Field Camera 3 instrument on the Hubble Space Telescope (HST). We study the wavelength dependence of rotation-modulated flux variations between 1.1 mu m and 1.7 mu m. We find that the water absorption bands of the two L5 dwarfs at 1.15 mu m and 1.4 mu m vary at similar amplitudes as the adjacent continuum. This differs from the results of previous HST observations of L/T transition dwarfs, in which the water absorption at 1.4 mu m displays variations of about half of the amplitude at other wavelengths. We find that the relative amplitude of flux variability out of the water band with respect to that in the water band shows a increasing trend from the L5 dwarfs toward the early T dwarfs. We utilize the models of Saumon & Marley and find that the observed variability of the L5 dwarfs can be explained by the presence of spatially varying high-altitude haze layers above the condensate clouds. Therefore, our observations show that the heterogeneity of haze layers-the driver of the variability-must be located at very low pressures, where even the water opacity is negligible. In the near future, the rotational spectral mapping technique could be utilized for other atomic and molecular species to probe different pressure levels in the atmospheres of brown dwarfs and exoplanets and uncover both horizontal and vertical cloud structures. C1 [Yang, Hao; Apai, Daniel; Karalidi, Theodora] Univ Arizona, Dept Astron, Tucson, AZ 85721 USA. [Apai, Daniel; Showman, Adam P.; Flateau, Davin] Univ Arizona, Dept Planetary Sci, Tucson, AZ 85721 USA. [Marley, Mark S.] NASA, Ames Res Ctr, Naval Air Stn, Mountain View, CA 94035 USA. [Saumon, Didier] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Morley, Caroline V.] Univ Calif Santa Cruz, Dept Astron & Astrophys, Santa Cruz, CA 95064 USA. [Buenzli, Esther] Max Planck Inst Astron, D-69117 Heidelberg, Germany. [Artigau, Etienne] Univ Montreal, Dept Phys, Montreal, PQ H3C 3J7, Canada. [Radigan, Jacqueline] Space Telescope Sci Inst, Baltimore, MD 21218 USA. [Metchev, Stanimir] Univ Western Ontario, Dept Phys & Astron, London, ON N6A 3K7, Canada. [Burgasser, Adam J.] Univ Calif San Diego, Ctr Astrophys & Space Sci, La Jolla, CA 92093 USA. [Mohanty, Subhanjoy] Univ London Imperial Coll Sci Technol & Med, London SW7 2AZ, England. [Lowrance, Patrick J.] CALTECH, Ctr Infrared Proc & Anal, Pasadena, CA 91125 USA. [Heinze, Aren N.] SUNY Stony Brook, Dept Phys & Astron, Stony Brook, NY 11794 USA. RP Yang, H (reprint author), Univ Arizona, Dept Astron, 933 North Cherry Ave, Tucson, AZ 85721 USA. EM haoyang@email.arizona.edu RI Yang, Hao/F-8396-2014; OI Yang, Hao/0000-0002-9423-2333; Marley, Mark/0000-0002-5251-2943; Buenzli, Esther/0000-0003-3306-1486; Metchev, Stanimir/0000-0003-3050-8203 FU NASA through an award issued by JPL/Caltech; NASA through a grant from the Space Telescope Science Institute [13176, 13280.06-A]; NASA [NAS5-26555]; Swiss National Science Foundation (SNSF) FX This work is part of the Spitzer Cycle-9 Exploration Program Extrasolar Storms. This work is based in part on observations made with the Spitzer Space Telescope, which is operated by the Jet Propulsion Laboratory, California Institute of Technology under a contract with NASA. Support for this work was provided by NASA through an award issued by JPL/Caltech. Support for HST GO programs 13176 and 13280.06-A was provided by NASA through a grant from the Space Telescope Science Institute, which is operated by the Association of Universities for Research in Astronomy, Inc., under NASA contract NAS5-26555. We acknowledge the outstanding help of Patricia Royle (STScI) and the Spitzer Science Center staff, especially Nancy Silbermann, for coordinating the HST and Spitzer observations. E.B. is supported by the Swiss National Science Foundation (SNSF). NR 39 TC 10 Z9 10 U1 0 U2 4 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 2041-8205 EI 2041-8213 J9 ASTROPHYS J LETT JI Astrophys. J. Lett. PD JAN 1 PY 2015 VL 798 IS 1 AR L13 DI 10.1088/2041-8205/798/1/L13 PG 5 WC Astronomy & Astrophysics SC Astronomy & Astrophysics GA AY3CN UT WOS:000347462300013 ER PT J AU Hecker, SS Milani, A AF Hecker, Siegfried S. Milani, Abbas TI Ending the assassination and oppression of Iranian nuclear scientists SO BULLETIN OF THE ATOMIC SCIENTISTS LA English DT Article DE assassination; Fereydoon Abbasi; Iranian nuclear scientists; Majid Shahriari; Omid Kokabee AB Merely for working in their field of expertise, Iranian nuclear scientists face perils and pressures that are nothing less than Shakespearean. The question for them is, in a very real sense, to be or not to be. In the course of the last four decades, these scientists have faced intimidation and severe punishment, including prison terms, at the hands of their own government. In recent years, at least five Iranian nuclear scientists have been the target of assassination attempts often attributed to Israeli intelligence. Regardless of their source, all such threats against scientists are morally indefensible. They offend the scientific spirit, working against the free exchange of ideas that is necessary for humanity to advance. And in the final analysis, the authors assert, these threats against scientists in Iran undermine global peace, targeting experts whose international collaboration is required to deal effectively with the nuclear risks facing the world today. Simply put, killing nuclear scientists makes reducing the threat of nuclear war harder, not easier. C1 [Hecker, Siegfried S.] Stanford Univ, Ctr Int Secur & Cooperat CISAC, Stanford, CA 94305 USA. [Hecker, Siegfried S.] Freeman Spogli Inst Int Studies, Stanford, CA USA. [Hecker, Siegfried S.] Dept Management Sci & Engn, Stanford, CA USA. [Hecker, Siegfried S.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Milani, Abbas] Stanford Univ, Stanford, CA 94305 USA. [Milani, Abbas] Univ Tehran, Fac Law & Polit Sci, Tehran 14174, Iran. RP Hecker, SS (reprint author), Stanford Univ, Ctr Int Secur & Cooperat CISAC, Stanford, CA 94305 USA. NR 6 TC 1 Z9 1 U1 1 U2 6 PU SAGE PUBLICATIONS LTD PI LONDON PA 1 OLIVERS YARD, 55 CITY ROAD, LONDON EC1Y 1SP, ENGLAND SN 0096-3402 EI 1938-3282 J9 B ATOM SCI JI Bull. Atom. Scient. PD JAN-FEB PY 2015 VL 71 IS 1 BP 46 EP 52 DI 10.1177/0096340214564140 PG 7 WC International Relations; Social Issues SC International Relations; Social Issues GA AY0ZC UT WOS:000347322200006 ER PT J AU Yue, YF Zhang, ZY Binder, AJ Chen, JH Jin, XB Overbury, SH Dai, S AF Yue, Yanfeng Zhang, Zhiyong Binder, Andrew J. Chen, Jihua Jin, Xianbo Overbury, Steven H. Dai, Sheng TI Hierarchically Superstructured Prussian Blue Analogues: Spontaneous Assembly Synthesis and Applications as Pseudocapacitive Materials SO CHEMSUSCHEM LA English DT Article DE hierarchical superstructures; prussian blue; prussian blue analogues; pseudocapacitive materials; spontaneous assembly ID SUPERCAPACITOR ELECTRODE MATERIAL; ELECTROCHEMICAL ENERGY-STORAGE; OXIDIZED IRIDIUM ELECTRODES; TEMPLATE-FREE SYNTHESIS; SODIUM-ION BATTERIES; THICK OXIDE-FILMS; NANOPOROUS CARBONS; SINGLE-CRYSTAL; BULK PROCESSES; METAL-OXIDES AB Hierarchically superstructured Prussian blue analogues (hexacyanoferrate, M= Ni-II, Co-II and Cu-II) are synthesized through a spontaneous assembly technique. In sharp contrast to macroporous-only Prussian blue analogues, the hierarchically superstructured porous Prussian blue materials are demonstrated to possess a high capacitance, which is similar to those of the conventional hybrid graphene/MnO2 nanostructured textiles. Because sodium or potassium ions are involved in energy storage processes, more environmentally neutral electrolytes can be utilized, making the superstructured porous Prussian blue analogues a great contender for applications as high-performance pseudocapacitors. C1 [Yue, Yanfeng; Zhang, Zhiyong; Overbury, Steven H.; Dai, Sheng] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. [Binder, Andrew J.] Univ Tennessee, Dept Chem, Knoxville, TN 37996 USA. [Chen, Jihua] Oak Ridge Natl Lab, Ctr Nanophase, Div Mat Sci, Oak Ridge, TN 37831 USA. [Jin, Xianbo] Wuhan Univ, Coll Chem & Mol Sci, Wuhan 430072, Peoples R China. RP Dai, S (reprint author), Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. EM dais@ornl.gov RI Chen, Jihua/F-1417-2011; Dai, Sheng/K-8411-2015; Overbury, Steven/C-5108-2016; Zhang, Zhiyong/H-5611-2012; OI Chen, Jihua/0000-0001-6879-5936; Dai, Sheng/0000-0002-8046-3931; Overbury, Steven/0000-0002-5137-3961; Zhang, Zhiyong/0000-0001-7936-9510; Jin, Xianbo/0000-0002-3095-8979 FU U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences FX The work was supported as part of the Fluid Interface Reactions, Structures, and Transport (FIRST) Center, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences. TEM experiments were conducted at the Center for Nanophase Materials Sciences, which was sponsored at Oak Ridge National Laboratory by the Division of Scientific User Facilities, Office of Basic Energy Sciences, U.S. Department of Energy. NR 61 TC 9 Z9 9 U1 38 U2 156 PU WILEY-V C H VERLAG GMBH PI WEINHEIM PA BOSCHSTRASSE 12, D-69469 WEINHEIM, GERMANY SN 1864-5631 EI 1864-564X J9 CHEMSUSCHEM JI ChemSusChem PD JAN PY 2015 VL 8 IS 1 BP 177 EP 183 DI 10.1002/cssc.201402520 PG 7 WC Chemistry, Multidisciplinary; GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY SC Chemistry; Science & Technology - Other Topics GA AY4IO UT WOS:000347541700022 PM 25385481 ER PT J AU DeRolph, CR Nelson, SAC Kwak, TJ Hain, EF AF DeRolph, Christopher R. Nelson, Stacy A. C. Kwak, Thomas J. Hain, Ernie F. TI Predicting fine-scale distributions of peripheral aquatic species in headwater streams SO ECOLOGY AND EVOLUTION LA English DT Article DE Conservation planning; habitat modeling; headwater streams; landscape variables; peripheral populations; species distributions; topographic gradient; wild trout ID SOUTHERN APPALACHIAN MOUNTAINS; TROUT SALVELINUS-FONTINALIS; MULTIPLE SPATIAL SCALES; NATIVE BROOK TROUT; CLIMATE-CHANGE; FISH ASSEMBLAGES; BROWN TROUT; LANDSCAPE VARIABLES; BIOTIC INTERACTIONS; PRESENCE-ABSENCE AB Headwater species and peripheral populations that occupy habitat at the edge of a species range may hold an increased conservation value to managers due to their potential to maximize intraspecies diversity and species' adaptive capabilities in the context of rapid environmental change. The southern Appalachian Mountains are the southern extent of the geographic range of native Salvelinus fontinalis and naturalized Oncorhynchus mykiss and Salmo trutta in eastern North America. We predicted distributions of these peripheral, headwater wild trout populations at a fine scale to serve as a planning and management tool for resource managers to maximize resistance and resilience of these populations in the face of anthropogenic stressors. We developed correlative logistic regression models to predict occurrence of brook trout, rainbow trout, and brown trout for every interconfluence stream reach in the study area. A streamnetwork was generated to capture a more consistent representation of headwater streams. Each of the final models had four significant metrics in common: stream order, fragmentation, precipitation, and land cover. Strahler stream order was found to be the most influential variable in two of the three final models and the second most influential variable in the other model. Greater than 70% presence accuracy was achieved for all three models. The underrepresentation of headwater streams in commonly used hydrography datasets is an important consideration that warrants close examination when forecasting headwater species distributions and range estimates. Additionally, it appears that a relative watershed position metric (e.g., stream order) is an important surrogate variable (even when elevation is included) for biotic interactions across the landscape in areas where headwater species distributions are influenced by topographical gradients. C1 [DeRolph, Christopher R.; Nelson, Stacy A. C.; Hain, Ernie F.] N Carolina State Univ, Coll Nat Resources, Ctr Geospatial Analyt, Raleigh, NC 27695 USA. [Kwak, Thomas J.] N Carolina State Univ, North Carolina Cooperat Fish & Wildlife Res Unit, US Geol Survey, Raleigh, NC 27695 USA. RP DeRolph, CR (reprint author), Oak Ridge Natl Lab, Div Environm Sci, POB 2008, Oak Ridge, TN 37831 USA. EM chrisderolph@gmail.com FU Federal Aid in Sport Fish Restoration Funds FX This research was funded by Federal Aid in Sport Fish Restoration Funds. NR 72 TC 1 Z9 1 U1 5 U2 26 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 2045-7758 J9 ECOL EVOL JI Ecol. Evol. PD JAN PY 2015 VL 5 IS 1 BP 152 EP 163 DI 10.1002/ece3.1331 PG 12 WC Ecology; Evolutionary Biology SC Environmental Sciences & Ecology; Evolutionary Biology GA AY3ZF UT WOS:000347517300014 PM 25628872 ER PT J AU Saye, RI AF Saye, R. I. TI An algorithm to mesh interconnected surfaces via the Voronoi interface SO ENGINEERING WITH COMPUTERS LA English DT Article DE Interconnected surfaces; Triangulated mesh; Voronoi interface; Multiphase; Multi-material data sets ID LEVEL SET METHOD; GENERATION; QUALITY; FRONTS; MODELS AB Many scientific and engineering problems involve interconnected surfaces meeting at junctions. For example, understanding the dynamics of a soap bubble foam can require modelling the fluid mechanics of liquid inside an intricate network of thin-film membranes. If a mesh of these surfaces is needed, the use of standard meshing algorithms often leads to voids, overlapping elements, or other artefacts near the junctions. Here, we present an algorithm to generate high-quality triangulated meshes of a set of interconnected surfaces with high surface accuracy. By capitalising on mathematical aspects of a geometric construction known as the "Voronoi interface", the algorithm first creates a topologically consistent mesh automatically, without making heuristic or complex decisions about surface topology. In particular, elements that meet at a junction do so by sharing a common edge, leading to simplifications in finite element calculations. In the second stage of the algorithm, mesh quality is improved by applying a short sequence of force-based smoothing, projection, and edge-flipping steps. Efficiency is further enhanced by using a locally adaptive time stepping scheme that prevents inversion of mesh elements, and we also comment on how the algorithm can be parallelised. Results are shown using a variety of examples arising from multiphase curvature flow, geometrically defined objects, surface reconstruction from volumetric point clouds, and a simulation of the multiscale dynamics of a cluster of soap bubbles. In this last example, generating high-quality meshes of evolving interconnected surfaces is crucial in determining thin-film liquid dynamics via finite element methods. C1 [Saye, R. I.] Univ Calif Berkeley, Dept Math, Berkeley, CA 94720 USA. [Saye, R. I.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Saye, RI (reprint author), Univ Calif Berkeley, Dept Math, Berkeley, CA 94720 USA. EM saye@math.berkeley.edu FU Applied Mathematical Sciences subprogram of the Office of Energy Research, US Department of Energy [DE-AC02-05CH11231]; Division of Mathematical Sciences of the National Science Foundation; American Australian Association Sir Keith Murdoch Fellowship FX This research was supported in part by the Applied Mathematical Sciences subprogram of the Office of Energy Research, US Department of Energy, under contract number DE-AC02-05CH11231, by the Division of Mathematical Sciences of the National Science Foundation, and by an American Australian Association Sir Keith Murdoch Fellowship. NR 40 TC 2 Z9 2 U1 4 U2 15 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 0177-0667 EI 1435-5663 J9 ENG COMPUT-GERMANY JI Eng. Comput. PD JAN PY 2015 VL 31 IS 1 BP 123 EP 139 DI 10.1007/s00366-013-0335-9 PG 17 WC Computer Science, Interdisciplinary Applications; Engineering, Mechanical SC Computer Science; Engineering GA AY2FP UT WOS:000347404400009 ER PT J AU Kanchongkittiphon, W Mendell, MJ Gaffin, JM Wang, G Phipatanakul, W AF Kanchongkittiphon, Watcharoot Mendell, Mark J. Gaffin, Jonathan M. Wang, Grace Phipatanakul, Wanda TI Indoor Environmental Exposures and Exacerbation of Asthma: An Update to the 2000 Review by the Institute of Medicine SO ENVIRONMENTAL HEALTH PERSPECTIVES LA English DT Review ID INNER-CITY CHILDREN; EXHALED NITRIC-OXIDE; RANDOMIZED CONTROLLED-TRIAL; VOLATILE ORGANIC-COMPOUNDS; EMERGENCY-DEPARTMENT VISITS; NITROGEN-DIOXIDE EXPOSURE; TOBACCO-SMOKE EXPOSURE; PEAK EXPIRATORY FLOW; DUST-MITE EXPOSURE; RESPIRATORY HEALTH AB BACKGROUND: Previous research has found relationships between specific indoor environmental exposures and exacerbation of asthma. OBJECTIVES: In this review we provide an updated summary of knowledge from the scientific literature on indoor exposures and exacerbation of asthma. METHODS: Peer-reviewed articles published from 2000 to 2013 on indoor exposures and exacerbation of asthma were identified through PubMed, from reference lists, and from authors' files. Articles that focused on modifiable indoor exposures in relation to frequency or severity of exacerbation of asthma were selected for review. Research findings were reviewed and summarized with consideration of the strength of the evidence. RESULTS: Sixty-nine eligible articles were included. Major changed conclusions include a causal relationship with exacerbation for indoor dampness or dampness-related agents (in children); associations with exacerbation for dampness or dampness-related agents (in adults), endotoxin, and environmental tobacco smoke (in preschool children); and limited or suggestive evidence for association with exacerbation for indoor culturable Penicillium or total fungi, nitrogen dioxide, rodents (nonoccupational), feather/down pillows (protective relative to synthetic bedding), and (regardless of specific sensitization) dust mite, cockroach, dog, and dampness-related agents. DISCUSSION: This review, incorporating evidence reported since 2000, increases the strength of evidence linking many indoor factors to the exacerbation of asthma. Conclusions should be considered provisional until all available evidence is examined more thoroughly. CONCLUSION: Multiple indoor exposures, especially dampness-related agents, merit increased attention to prevent exacerbation of asthma, possibly even in nonsensitized individuals. Additional research to establish causality and evaluate interventions is needed for these and other indoor exposures. C1 [Kanchongkittiphon, Watcharoot; Gaffin, Jonathan M.; Phipatanakul, Wanda] Boston Childrens Hosp, Div Allergy & Immunol, Boston, MA USA. [Kanchongkittiphon, Watcharoot; Gaffin, Jonathan M.; Phipatanakul, Wanda] Harvard Univ, Sch Med, Boston, MA USA. [Kanchongkittiphon, Watcharoot] Mahidol Univ, Ramathibodi Hosp, Dept Pediat, Bangkok 10700, Thailand. [Mendell, Mark J.] Calif Dept Publ Hlth, Indoor Air Qual Program, Richmond, CA USA. [Mendell, Mark J.] Lawrence Berkeley Natl Lab, Indoor Environm Grp, Berkeley, CA USA. [Wang, Grace] Amer Inst Res, San Mateo, CA USA. RP Mendell, MJ (reprint author), 819 Everett St, El Cerrito, CA 94530 USA. EM mmendell@pacbell.net FU Indoor Environments Division, Office of Radiation and Indoor Air, of the U.S. Environmental Protection Agency; Ramathibodi Hospital, Mahidol University, Bangkok, Thailand; National Institutes of Health [K23AI106945-01, K24 AI 106822, R01 AI 073964, R01 AI 073964-02S1] FX This study was supported with funding from the Indoor Environments Division, Office of Radiation and Indoor Air, of the U.S. Environmental Protection Agency. Support was also provided by a research scholarship from Ramathibodi Hospital, Mahidol University, Bangkok, Thailand (W.K.) and by grants K23AI106945-01 (J.M.G.) and K24 AI 106822, R01 AI 073964, and R01 AI 073964-02S1 (W.P.) from the National Institutes of Health. NR 115 TC 39 Z9 41 U1 7 U2 48 PU US DEPT HEALTH HUMAN SCIENCES PUBLIC HEALTH SCIENCE PI RES TRIANGLE PK PA NATL INST HEALTH, NATL INST ENVIRONMENTAL HEALTH SCIENCES, PO BOX 12233, RES TRIANGLE PK, NC 27709-2233 USA SN 0091-6765 EI 1552-9924 J9 ENVIRON HEALTH PERSP JI Environ. Health Perspect. PD JAN PY 2015 VL 123 IS 1 BP 6 EP 20 DI 10.1289/ehp.1307922 PG 15 WC Environmental Sciences; Public, Environmental & Occupational Health; Toxicology SC Environmental Sciences & Ecology; Public, Environmental & Occupational Health; Toxicology GA AY1YF UT WOS:000347385000008 PM 25303775 ER PT J AU Zhang, XS Izaurralde, RC Manowitz, DH Sahajpal, R West, TO Thomson, AM Xu, M Zhao, K LeDuc, SD Williams, JR AF Zhang, Xuesong Izaurralde, Roberto C. Manowitz, David H. Sahajpal, Ritvik West, Tristram O. Thomson, Allison M. Xu, Min Zhao, Kaiguang LeDuc, Stephen D. Williams, Jimmy R. TI Regional scale cropland carbon budgets: Evaluating a geospatial agricultural modeling system using inventory data SO ENVIRONMENTAL MODELLING & SOFTWARE LA English DT Article DE Agriculture; Carbon; Climate change; EPIC; Geospatial modeling; Parallel computing ID CLIMATE-CHANGE IMPACTS; ORGANIC-CARBON; INTEGRATED ASSESSMENT; SOIL CARBON; LONG-TERM; CONTERMINOUS USA; UNITED-STATES; RIVER-BASIN; LAND-USE; DYNAMICS AB Accurate quantification and clear understanding of regional scale cropland carbon (C) cycling is critical for designing effective policies and management practices that can contribute toward stabilizing atmospheric CO2 concentrations. However, extrapolating site-scale observations to regional scales represents a major challenge confronting the agricultural modeling community. This study introduces a novel geospatial agricultural modeling system (GAMS) exploring the integration of the mechanistic Environmental Policy Integrated Climate model, spatially-resolved data, surveyed management data, and supercomputing functions for cropland C budgets estimates. This modeling system creates spatially-explicit modeling units at a spatial resolution consistent with remotely-sensed crop identification and assigns cropping systems to each of them by geo-referencing surveyed crop management information at the county or state level. A parallel computing algorithm was also developed to facilitate the computationally intensive model runs and output post-processing and visualization. We evaluated GAMS against National Agricultural Statistics Service (NASS) reported crop yields and inventory estimated county-scale cropland C budgets averaged over 2000-2008. We observed good overall agreement, with spatial correlation of 0.89, 0.90, 0.41, and 0.87, for crop yields, Net Primary Production (NPP), Soil Organic C (SOC) change, and Net Ecosystem Exchange (NEE), respectively. However, we also detected notable differences in the magnitude of NPP and NEE, as well as in the spatial pattern of SOC change. By performing crop-specific annual comparisons, we discuss possible explanations for the discrepancies between GAMS and the inventory method, such as data requirements, representation of agroecosystem processes, completeness and accuracy of crop management data, and accuracy of crop area representation. Based on these analyses, we further discuss strategies to improve GAMS by updating input data and by designing more efficient parallel computing capability to quantitatively assess errors associated with the simulation of C budget components. The modularized design of the GAMS makes it flexible to be updated and adapted for different agricultural models so long as they require similar input data, and to be linked with socio-economic models to understand the effectiveness and implications of diverse C management practices and policies. (C) 2014 Elsevier Ltd. All rights reserved. C1 [Zhang, Xuesong; Manowitz, David H.; West, Tristram O.; Thomson, Allison M.] Pacific NW Natl Lab, Joint Global Change Res Inst, College Pk, MD 20740 USA. [Zhang, Xuesong; Manowitz, David H.; West, Tristram O.; Thomson, Allison M.] Univ Maryland, College Pk, MD 20740 USA. [Izaurralde, Roberto C.; Sahajpal, Ritvik] Univ Maryland, Dept Geog Sci, College Pk, MD 20740 USA. [Xu, Min] Univ Maryland, Earth Syst Sci Interdisciplinary Ctr, College Pk, MD 20740 USA. [Zhao, Kaiguang] Ohio State Univ, Sch Environm & Nat Resources, Ohio Agr Res & Dev Ctr, Wooster, OH 44691 USA. [LeDuc, Stephen D.] US EPA, Natl Ctr Environm Assessment, Arlington, VA 22202 USA. [Izaurralde, Roberto C.; Williams, Jimmy R.] Texas A&M AgriLife Res & Extens Ctr, Temple, TX 76502 USA. RP Zhang, XS (reprint author), Pacific NW Natl Lab, Joint Global Change Res Inst, College Pk, MD 20740 USA. EM xuesong.zhang@pnnl.gov RI zhang, xuesong/B-7907-2009; Zhao, Kaiguang/D-1172-2010; OI Xu, Min/0000-0003-3443-0300 FU DOE Great Lakes Bioenergy Research Center (DOE BER Office of Science) [DE-FC02-07ER64494, KP1601050, DOE EERE OBP 20469-19145]; NASA, North American Carbon Program [NNH12AU03I]; New Investigator Program (NIP) [NNH13ZDA001N] FX We sincerely appreciate the valuable comments provided by the three anonymous reviewers, which have greatly improved the quality of this manuscript. This work was partially funded by the DOE Great Lakes Bioenergy Research Center (DOE BER Office of Science DE-FC02-07ER64494, DOE BER Office of Science KP1601050, DOE EERE OBP 20469-19145), and NASA as part of the North American Carbon Program (NNH12AU03I) and the New Investigator Program (NIP) (NNH13ZDA001N). The views expressed here are those of the authors and do not necessarily represent the views or policies of the U.S. Environmental Protection Agency. NR 78 TC 13 Z9 13 U1 2 U2 38 PU ELSEVIER SCI LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, OXON, ENGLAND SN 1364-8152 EI 1873-6726 J9 ENVIRON MODELL SOFTW JI Environ. Modell. Softw. PD JAN PY 2015 VL 63 BP 199 EP 216 DI 10.1016/j.envsoft.2014.10.005 PG 18 WC Computer Science, Interdisciplinary Applications; Engineering, Environmental; Environmental Sciences SC Computer Science; Engineering; Environmental Sciences & Ecology GA AY1OT UT WOS:000347362900016 ER PT J AU Pan, LH Freifeld, B Doughty, C Zakem, S Sheu, M Cutright, B Terrall, T AF Pan, Lehua Freifeld, Barry Doughty, Christine Zakem, Steven Sheu, Ming Cutright, Bruce Terrall, Tracy TI Fully coupled wellbore-reservoir modeling of geothermal heat extraction using CO2 as the working fluid SO GEOTHERMICS LA English DT Article DE Geothermal electricity; Thermosiphon; CO2; Coupled numerical simulation; Enhanced geothermal system ID SEQUESTRATION; SYSTEMS; CARBON; FLOW AB We consider using CO2 as an alternative to water as a working fluid to produce geothermal electricity through the application of a coupled reservoir, wellbore, and surface power-plant model. Our approach has relaxed some of the simplifying assumptions others have made in previous work, through the application of a subsurface reservoir model fully coupled with a detailed wellbore simulator. We also include a simplified representation of CO2 turbomachinery for a surface plant optimized for direct use of supercritical CO2. The wellbore model includes heat transfer between the fluid in the well and the surrounding formation, in addition to frictional, inertial, and gravitational forces. Our results show that thermophysical operating conditions and the amount of power production are greatly influenced by wellbore flow processes and by wellbore/caprock heat transfer. We investigate competing effects that control development of a thermosiphon, which enables production of geothermal electricity without the need for a continuously operating external pump. (C) 2014 Elsevier Ltd. All rights reserved. C1 [Pan, Lehua; Freifeld, Barry; Doughty, Christine] Lawrence Berkeley Natl Lab, Div Earth Sci, Berkeley, CA 94720 USA. [Zakem, Steven; Sheu, Ming] Echogen Power Syst Inc, Akron, OH 44308 USA. [Cutright, Bruce; Terrall, Tracy] Texas Bur Econ Geol, Austin, TX USA. RP Pan, LH (reprint author), MS 74R0120,One Cyclotron Rd, Berkeley, CA 94720 USA. EM lpan@lbl.gov RI Doughty, Christine/G-2389-2015; Pan, Lehua/G-2439-2015; Freifeld, Barry/F-3173-2010 FU LBNL [DE-AC02-05CH11231] FX This work was funded by the Assistant Secretary for Energy Efficiency and Renewable Energy, Geothermal Technologies Program of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. The authors thank Dan Hawkes (LBNL) for editing the manuscript. NR 15 TC 11 Z9 11 U1 5 U2 22 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0375-6505 EI 1879-3576 J9 GEOTHERMICS JI Geothermics PD JAN PY 2015 VL 53 BP 100 EP 113 DI 10.1016/j.geothermics.2014.05.005 PG 14 WC Energy & Fuels; Geosciences, Multidisciplinary SC Energy & Fuels; Geology GA AY3OX UT WOS:000347493800009 ER PT J AU Dean, C Reimus, P Oates, J Rose, P Newell, D Petty, S AF Dean, Cynthia Reimus, Paul Oates, Jeffrey Rose, Peter Newell, Dennis Petty, Susan TI Laboratory experiments to characterize cation-exchanging tracer behavior for fracture surface area estimation at Newberry Crater, OR SO GEOTHERMICS LA English DT Article DE EGS; Fractures; Tracers; Characterization; Surface area ID TEMPERATURE; TRANSPORT; DEPENDENCE; ADSORPTION; MODEL AB A series of column transport experiments ranging from 25 degrees C to 275 degrees C, as well as batch sorption experiments at 25 degrees C, were conducted to estimate cation exchange parameters for lithium and cesium at the Newberry Crater Enhanced Geothermal System demonstration site. The experiments were designed to facilitate interpretation of single-well field tracer tests to interrogate fracture surface area. Lithium column transport from 125 degrees C to 275 degrees C showed a strong temperature dependence, with much greater cation exchange at higher temperatures than in 25 degrees C experiments. Cesium column transport at 225 degrees C indicated a weaker temperature dependence, and unlike Li+, its exchange decreased at higher temperatures. Published by Elsevier Ltd. C1 [Dean, Cynthia] Los Alamos Natl Lab, Chem Diagnost & Engn Grp, Los Alamos, NM 87545 USA. [Reimus, Paul] Los Alamos Natl Lab, Earth Syst Observat Grp, Los Alamos, NM 87545 USA. [Oates, Jeffrey; Rose, Peter] Univ Utah, Energy & Geosci Inst, Salt Lake City, UT 84112 USA. [Newell, Dennis] Utah State Univ, Dept Geol, Logan, UT 84322 USA. [Petty, Susan] AltaRock Energy Inc, Seattle, WA USA. RP Dean, C (reprint author), Los Alamos Natl Lab, Chem Diagnost & Engn Grp, Los Alamos, NM 87545 USA. EM cdean@lanl.gov FU Institute of Geophysics and Planetary Physics at Los Alamos National Laboratory; U.S. Department of Energy, Geothermal Technologies Program FX This work was supported by the Institute of Geophysics and Planetary Physics at Los Alamos National Laboratory and the U.S. Department of Energy, Geothermal Technologies Program. We would like to acknowledge Michael Rearick, Emily Kluk, Stuart Ware, Jesse Punsal and Brian House of LANL's Earth Systems Observations group for analytical and laboratory support. We would like to acknowledge Kevin Leecaster, formerly of the Energy and Geosciences Institute, University of Utah, for the low-temperature column data. Los Alamos Unlimited Release No. LA-UR-13-26823. NR 21 TC 3 Z9 4 U1 1 U2 11 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0375-6505 EI 1879-3576 J9 GEOTHERMICS JI Geothermics PD JAN PY 2015 VL 53 BP 213 EP 224 DI 10.1016/j.geothermics.2014.05.011 PG 12 WC Energy & Fuels; Geosciences, Multidisciplinary SC Energy & Fuels; Geology GA AY3OX UT WOS:000347493800020 ER PT J AU Lindsey, NJ Newman, GA AF Lindsey, Nathaniel J. Newman, Gregory A. TI Improved workflow for 3D inverse modeling of magnetotelluric data: Examples from five geothermal systems SO GEOTHERMICS LA English DT Article DE Magnetotellurics; Geothermal energy; 3D inversion; Geophysical inverse theory ID ELECTROMAGNETIC INDUCTION; OPTIMIZATION AB Magnetotellurics (MT) is now an important geophysical tool for imaging complex geothermal energy systems, but retrieving realistic three-dimensional (3D) resistivity models is challenging, and computationally intensive. To ameliorate this situation, we develop a sequenced MT inversion workflow that formalizes and improves upon concepts introduced by Rosenkjaer and Oldenberg (2012). We test the performance and reliability of our workflow using five 3D MT datasets from geothermal fields in the United States (Coso, Raft River) and Iceland (Krafla, Hengill and Krysuvik). We compare inversion results from the standard and sequenced workflows for each experiment, and find that the sequenced workflow always retrieves a better-fitting model, specifically at lower frequencies, which is geologically consistent and representative of a high temperature geothermal system. It also uses fewer computational resources. Published by Elsevier Ltd. C1 [Lindsey, Nathaniel J.; Newman, Gregory A.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, Berkeley, CA 94720 USA. RP Lindsey, NJ (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, 1 Cyclotron Rd, Berkeley, CA 94720 USA. EM njlindsey@lbl.gov RI Newman, Gregory/G-2813-2015 FU Department of Energy Geothermal Program Office [GT-480010-19823-10]; Office of Basic Energy Sciences [DE-AC02-05CH11231] FX The authors thank Michael Commer, Erika Gasperikova, and an anonymous reviewer for their helpful suggestions and insight; the Iceland GeoSurvey for sharing data from Krafla, Hengill and Krysuvik geothermal fields; and Phil Wannamaker for sharing data from Raft River geothermal field. This work was carried out at Lawrence Berkeley National Laboratory with funding provided by the Department of Energy Geothermal Program Office under contract GT-480010-19823-10, and Office of Basic Energy Sciences under contract DE-AC02-05CH11231. NR 29 TC 5 Z9 6 U1 1 U2 22 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0375-6505 EI 1879-3576 J9 GEOTHERMICS JI Geothermics PD JAN PY 2015 VL 53 BP 527 EP 532 DI 10.1016/j.geothermics.2014.09.004 PG 6 WC Energy & Fuels; Geosciences, Multidisciplinary SC Energy & Fuels; Geology GA AY3OX UT WOS:000347493800045 ER PT J AU Lippmann, MJ Garg, S AF Lippmann, Marcelo J. Garg, Sabodh TI Alfred H. Truesdell (1933-2044) Obituary SO GEOTHERMICS LA English DT Biographical-Item C1 [Lippmann, Marcelo J.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Garg, Sabodh] Leidos Inc, San Diego, CA 92121 USA. RP Lippmann, MJ (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. EM mjlippmann@lbl.gov; sabodh.k.garg@leidos.com NR 0 TC 0 Z9 0 U1 0 U2 0 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0375-6505 EI 1879-3576 J9 GEOTHERMICS JI Geothermics PD JAN PY 2015 VL 53 BP 554 EP 555 DI 10.1016/j.geothermics.2014.09.006 PG 2 WC Energy & Fuels; Geosciences, Multidisciplinary SC Energy & Fuels; Geology GA AY3OX UT WOS:000347493800050 ER PT J AU Lewis, SM Gross, S Visel, A Kelly, M Morrow, W AF Lewis, Sarah M. Gross, Stephen Visel, Axel Kelly, Maggi Morrow, William TI Fuzzy GIS-based multi-criteria evaluation for US Agave production as a bioenergy feedstock SO GLOBAL CHANGE BIOLOGY BIOENERGY LA English DT Article DE Agave; bioenergy; biofuel; fuzzy logic; geographic information systems; suitability mapping ID BIOFUEL FEEDSTOCK; UNITED-STATES; RESPONSES; TEQUILANA; ENERGY; CO2; SWITCHGRASS; BIOETHANOL AB In the United States, renewable energy mandates calling for increased production of cellulosic biofuels will require a diversity of bioenergy feedstocks to meet growing demands. Within the suite of potential energy crops, plants within the genus Agave promise to be a productive feedstock in hot and arid regions. The potential distributions of Agave tequilana and Agave deserti in the United States were evaluated based on plant growth parameters identified in an extensive literature review. A geospatial suitability model rooted in fuzzy logic was developed that utilized a suite of biophysical criteria to optimize ideal geographic locations for this new crop, and several suitability scenarios were tested for each species. The results of this spatially explicit suitability model suggest that there is potential for Agave to be grown as an energy feedstock in the southwestern region of the United States - particularly in Arizona, California, and Texas - and a significant portion of these areas are proximate to existing transportation infrastructure. Both Agave species showed the highest state-level renewable energy benefit in Arizona, where agave plants have the potential to contribute 4.8-9.6% of the states' ethanol consumption, and 2.5-4.9% of its electricity consumption, for A. deserti and A. tequilana, respectively. This analysis supports the feasibility of Agave as a complementary bioenergy feedstock that can be grown in areas too harsh for conventional energy feedstocks. C1 [Lewis, Sarah M.; Kelly, Maggi] Univ Calif Berkeley, Berkeley, CA 94720 USA. [Gross, Stephen; Visel, Axel] US DOE, Joint Genome Inst, Walnut Creek, CA USA. [Visel, Axel] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Genom Div, Berkeley, CA 94720 USA. [Morrow, William] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Kelly, M (reprint author), Univ Calif Berkeley, 130 Mulford Hall 3114, Berkeley, CA 94720 USA. EM maggi@berkeley.edu RI Visel, Axel/A-9398-2009; OI Visel, Axel/0000-0002-4130-7784; Kelly, Nina Maggi/0000-0002-0198-2822 FU Office of Science, of the US Department of Energy [DE-AC0205CH11231]; Lawrence Berkeley National Laboratory Directed Research and Development Program [LB11036]; US Department of Energy [DEAC02-05CH11231] FX The authors acknowledge Mark Fisher and the University of California Boyd Deep Canyon Natural Reserve for providing climate data used to develop models for A. deserti. This work was supported by the Director, Office of Science, of the US Department of Energy under Contract No. DE-AC0205CH11231. A.V. and S.M.G. were supported by the Lawrence Berkeley National Laboratory Directed Research and Development Program (LB11036) and performed work under the Office of Science of the US Department of Energy Contract No. DEAC02-05CH11231. NR 40 TC 4 Z9 4 U1 2 U2 13 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 1757-1693 EI 1757-1707 J9 GCB BIOENERGY JI GCB Bioenergy PD JAN PY 2015 VL 7 IS 1 BP 84 EP 99 DI 10.1111/gcbb.12116 PG 16 WC Agronomy; Biotechnology & Applied Microbiology; Energy & Fuels SC Agriculture; Biotechnology & Applied Microbiology; Energy & Fuels GA AX1SN UT WOS:000346726500007 ER PT J AU Pinto, AF Romao, CV Pinto, LC Huber, H Saraiva, LM Todorovic, S Cabelli, D Teixeira, M AF Pinto, Ana F. Romao, Celia V. Pinto, Liliana C. Huber, Harald Saraiva, Ligia M. Todorovic, Smilja Cabelli, Diane Teixeira, Miguel TI Superoxide reduction by a superoxide reductase lacking the highly conserved lysine residue SO JOURNAL OF BIOLOGICAL INORGANIC CHEMISTRY LA English DT Article DE Superoxide; Oxidative stress; Superoxide reductase; Ignicoccus ID IRON ACTIVE-SITE; DESULFOARCULUS-BAARSII; ARCHAEOGLOBUS-FULGIDUS; PYROCOCCUS-FURIOSUS; TREPONEMA-PALLIDUM; DESULFOVIBRIO-VULGARIS; PULSE-RADIOLYSIS; MECHANISM; NEELAREDOXIN; PEROXIDE AB Superoxide reductases (SORs) are the most recently identified superoxide detoxification systems, being found in microorganisms from the three domains of life. These enzymes are characterized by a catalytic mononuclear iron site, with one cysteine and four histidine ligands of the ferrous active form. A lysine residue in the -EKHVP- motif, located close to the active site, has been considered to be essential for the enzyme function, by contributing to the positive surface patch that attracts the superoxide anion and by controlling the chemistry of the catalytic mechanism through a hydrogen bond network. However, we show here that this residue is substituted by non-equivalent amino acids in several putative SORs from Archaea and unicellular Eukarya. In this work, we focus on mechanistic and spectroscopic studies of one of these less common enzymes, the SOR from the hyperthermophilic Crenarchaeon Ignicoccus hospitalis. We employ pulse radiolysis fast kinetics and spectroscopic approaches to study the wild-type enzyme (-E23T24HVP-), and two mutants, T24K and E23A, the later mimicking enzymes lacking both the lysine and glutamate (a ferric ion ligand) of the motif. The efficiency of the wild-type protein and mutants in reducing superoxide is comparable to other SORs, revealing the robustness of these enzymes to single mutations. C1 [Pinto, Ana F.; Romao, Celia V.; Pinto, Liliana C.; Saraiva, Ligia M.; Todorovic, Smilja; Teixeira, Miguel] Univ Nova Lisboa, Inst Tecnol Quim & Biol Antonio Xavier, P-2781901 Oeiras, Portugal. [Huber, Harald] Univ Regensburg, Lehrstuhl Mikrobiol, D-93053 Regensburg, Germany. [Cabelli, Diane] Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA. RP Teixeira, M (reprint author), Univ Nova Lisboa, Inst Tecnol Quim & Biol Antonio Xavier, Apartado 127, P-2781901 Oeiras, Portugal. EM miguel@itqb.unl.pt RI Todorovic, Smilja/F-7612-2010; Romao, Celia/G-7013-2011 OI Todorovic, Smilja/0000-0002-0219-6743; Romao, Celia/0000-0002-9474-2405 FU Fundacao para a Ciencia e a Tecnologia (Portugal) [PEst-OE/EQB/LA0004/2013, PTDC/BIA-PRO/67263/2006, PTDC/BIA-PRO/111940/2009, PTDC/SAU-BMA/122444/2010, SFRH/BPD/94050/2013, PTDC/BBB-BQB/0937/2012]; Deutsche Forschungsgemeinschaf [HU 703/2-2]; US DOE Office of Science, Division of Chemical Sciences, Geosciences and Biosciences [DE-AC02-98CH10886] FX This work was supported by Fundacao para a Ciencia e a Tecnologia (Portugal), Grants PEst-OE/EQB/LA0004/2013, PTDC/BIA-PRO/67263/2006 (MT), PTDC/BIA-PRO/111940/2009 (CVR), PTDC/SAU-BMA/122444/2010 (ST), SFRH/BPD/94050/2013 (CVR) and PTDC/BBB-BQB/0937/2012 (LMS), and Deutsche Forschungsgemeinschaf Grant HU 703/2-2. The work at Brookhaven National Laboratory was carried out at the Accelerator Center for Energy Research, which is supported by the US DOE Office of Science, Division of Chemical Sciences, Geosciences and Biosciences under Contract No. DE-AC02-98CH10886. NR 39 TC 0 Z9 0 U1 1 U2 6 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 0949-8257 EI 1432-1327 J9 J BIOL INORG CHEM JI J. Biol. Inorg. Chem. PD JAN PY 2015 VL 20 IS 1 BP 155 EP 164 DI 10.1007/s00775-014-1222-6 PG 10 WC Biochemistry & Molecular Biology; Chemistry, Inorganic & Nuclear SC Biochemistry & Molecular Biology; Chemistry GA AY2GU UT WOS:000347407700013 PM 25476860 ER PT J AU He, YD Huang, JS Sumpter, BG Kornyshev, AA Qiao, R AF He, Yadong Huang, Jingsong Sumpter, Bobby G. Kornyshev, Alexei A. Qiao, Rui TI Dynamic Charge Storage in Ionic Liquids-Filled Nanopores: Insight from a Computational Cyclic Voltammetry Study SO JOURNAL OF PHYSICAL CHEMISTRY LETTERS LA English DT Article ID QUARTZ-CRYSTAL MICROBALANCE; SUBNANOMETER PORES; CARBON ELECTRODES; ENERGY-STORAGE; SUPERCAPACITORS; CAPACITANCE; SIMULATION; BEHAVIOR; MODEL; SIZE AB Understanding the dynamic charge storage in nanoporous electrodes with room-temperature ionic liquid electrolytes is essential for optimizing them to achieve supercapacitors with high energy and power densities. Herein, we report coarse-grained molecular dynamics simulations of the cyclic voltammetry of supercapacitors featuring subnanometer pores and model ionic liquids. We show that the cyclic charging and discharging of nanopores are governed by the interplay between the external field-driven ion transport and the sloshing dynamics of ions inside of the pore. The ion occupancy along the pore length depends strongly on the scan rate and varies cyclically during charging/discharging. Unlike that at equilibrium conditions or low scan rates, charge storage at high scan rates is dominated by counterions while the contribution by co-ions is marginal or negative. These observations help explain the perm-selective charge storage observed experimentally. We clarify the mechanisms underlying these dynamic phenomena and quantify their effects on the efficiency of the dynamic charge storage in nanopores. C1 [He, Yadong; Qiao, Rui] Virginia Tech, Dept Mech Engn, Blacksburg, VA 24061 USA. [Huang, Jingsong; Sumpter, Bobby G.] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci & Comp Sci, Oak Ridge, TN 37831 USA. [Huang, Jingsong; Sumpter, Bobby G.] Oak Ridge Natl Lab, Div Math, Oak Ridge, TN 37831 USA. [Kornyshev, Alexei A.] Univ London Imperial Coll Sci Technol & Med, Fac Nat Sci, Dept Chem, London SW7 2AZ, England. RP Qiao, R (reprint author), Virginia Tech, Dept Mech Engn, Blacksburg, VA 24061 USA. EM ruiqiao@vt.edu RI Sumpter, Bobby/C-9459-2013; Huang, Jingsong/A-2789-2008; Qiao, Rui/B-2350-2009 OI Sumpter, Bobby/0000-0001-6341-0355; Huang, Jingsong/0000-0001-8993-2506; Qiao, Rui/0000-0001-5219-5530 FU NSF [CBET-1461842]; HERE program for faculty at the Oak Ridge National Laboratory (ORNL); Center for Nanophase Materials Sciences, by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy; EPSC FX We thank the Clemson-CCIT and the ARC at Virginia Tech for generous allocation of computer time on the Palmetto cluster and the Blue Ridge cluster, respectively. R.Q. acknowledges the support from NSF (CBET-1461842). R.Q was partially supported by an appointment to the HERE program for faculty at the Oak Ridge National Laboratory (ORNL) administered by ORISE. J.H. and B.G.S. acknowledge support from the Center for Nanophase Materials Sciences, which is sponsored at ORNL by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy. A.A.K acknowledges the former support of EPSC, which helped to start cooperation with R.Q. NR 33 TC 16 Z9 16 U1 9 U2 48 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 1948-7185 J9 J PHYS CHEM LETT JI J. Phys. Chem. Lett. PD JAN 1 PY 2015 VL 6 IS 1 BP 22 EP 30 DI 10.1021/jz5024306 PG 9 WC Chemistry, Physical; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Atomic, Molecular & Chemical SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA AY3XW UT WOS:000347513700004 PM 26263086 ER PT J AU Bai, SR Zhou, DY Davis, MJ Skodje, RT AF Bai, Shirong Zhou, Dingyu Davis, Michael J. Skodje, Rex T. TI Sum over Histories Representation for Chemical Kinetics SO JOURNAL OF PHYSICAL CHEMISTRY LETTERS LA English DT Article ID REACTION-MECHANISMS; SYSTEMS; NETWORKS AB A new representation for chemical kinetics is introduced that is based on a sum over histories formulation that employs chemical pathways defined at a molecular level. The time evolution of a chemically reactive system is described by enumerating the most important pathways followed by a chemical moiety. An explicit formula for the pathway probabilities is derived and takes the form of an integral over a time-ordered product. When evaluating long pathways, the time-ordered product has a simple Monte Carlo representation that is computationally efficient. A small numerical stochastic simulation was used to identify the most important paths to include in the representation. The method was applied to a realistic H-2/O-2 combustion problem and is shown to yield accurate results. C1 [Bai, Shirong; Zhou, Dingyu; Skodje, Rex T.] Univ Colorado, Dept Chem & Biochem, Boulder, CO 80309 USA. [Davis, Michael J.] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. RP Skodje, RT (reprint author), Univ Colorado, Dept Chem & Biochem, Box 215, Boulder, CO 80309 USA. EM Rex.Skodje@colorado.edu FU U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences [DE-AC02-06CH11357] FX The work of D.Y.Z., M.J.D., and S.R.B. was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences, under contract number DE-AC02-06CH11357. NR 22 TC 2 Z9 2 U1 3 U2 13 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 1948-7185 J9 J PHYS CHEM LETT JI J. Phys. Chem. Lett. PD JAN 1 PY 2015 VL 6 IS 1 BP 183 EP 188 DI 10.1021/jz502239v PG 6 WC Chemistry, Physical; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Atomic, Molecular & Chemical SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA AY3XW UT WOS:000347513700028 PM 26263110 ER PT J AU Westbrook, ML Sindelar, RL Fisher, DL AF Westbrook, M. L. Sindelar, R. L. Fisher, D. L. TI Radiolytic hydrogen generation from aluminum oxyhydroxide solids: theory and experiment SO JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY LA English DT Article DE Boehmite; Gibbsite; Density functional theory (DFT); Hydrogen generation; Radiolysis ID BOEHMITE GAMMA-ALOOH; SPACE GROUP; IR-SPECTRA; REFINEMENT; CORROSION; GIBBSITE; DIASPORE; DENSITY; RAMAN AB Exploratory work on gamma exposure to dried solids with chemically-bound water that are typical of those produced on aluminum-clad nuclear fuel in reactor and post-discharge storage has shown a profound production of hydrogen (as the sole gaseous species) from dry boehmite (gamma-AlOOH or Al2O3 center dot H2O) powders and barely observable hydrogen from dry gibbsite (gamma-Al(OH)(3) or Al2O3 center dot 3H(2)O) under gamma irradiation from cobalt-60. A computational investigation of hydrogen bond energies was performed to provide insights to explain the experimental observations. A gas phase or single-molecule model, and a solid phase model were used. For all model reactions, computations indicate hydrogen loss is more favorable for boehmite than for gibbsite, in qualitative agreement with the experimental findings. C1 [Westbrook, M. L.; Sindelar, R. L.; Fisher, D. L.] Savannah River Natl Lab, Aiken, SC 29808 USA. RP Sindelar, RL (reprint author), Savannah River Natl Lab, Aiken, SC 29808 USA. EM robert.sindelar@srnl.doe.gov FU U.S. Department of Energy, Office of Environmental Management; U.S. Department of Energy [DE-AC09-08SR 22470]; agency of the United States Government FX The authors gratefully acknowledge support from the U.S. Department of Energy, Office of Environmental Management. The present work was supported through Contract DE-AC09-08SR 22470 with the U.S. Department of Energy. This report was prepared as an account of work sponsored by an agency of the United States Government. Neither the United States Government nor any agency thereof, nor any of their employees, nor any of their contractors, subcontractors, or their employees, makes any warranty, express or implied, or assumes any legal liability or responsibility for the accuracy, completeness, or any third party's use or the results of such use of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. Reference herein to any specific commercial product, process, or service by trade name, trademark, manufacturer, or otherwise does not necessarily constitute or imply its endorsement, recommendation, or favoring by the United States Government or any agency thereof or its contractors or subcontractors. The views and opinions of the authors expressed herein do not necessarily state or reflect those of the United States Government or any agency thereof. NR 22 TC 2 Z9 2 U1 2 U2 28 PU SPRINGER PI DORDRECHT PA VAN GODEWIJCKSTRAAT 30, 3311 GZ DORDRECHT, NETHERLANDS SN 0236-5731 EI 1588-2780 J9 J RADIOANAL NUCL CH JI J. Radioanal. Nucl. Chem. PD JAN PY 2015 VL 303 IS 1 BP 81 EP 86 DI 10.1007/s10967-014-3563-6 PG 6 WC Chemistry, Analytical; Chemistry, Inorganic & Nuclear; Nuclear Science & Technology SC Chemistry; Nuclear Science & Technology GA AY0OB UT WOS:000347294600010 ER PT J AU Despotopulos, JD Gostic, JM Bennett, ME Gharibyan, N Henderson, RA Moody, KJ Sudowe, R Shaughnessy, DA AF Despotopulos, J. D. Gostic, J. M. Bennett, M. E. Gharibyan, N. Henderson, R. A. Moody, K. J. Sudowe, R. Shaughnessy, D. A. TI Characterization of Group 5 dubnium homologs on diglycolamide extraction chromatography resins from nitric and hydrofluoric acid matrices SO JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY LA English DT Article DE Diglycolamide; Extraction chromatography; Heavy element; Automation; Dubnium ID CHEMICAL-PROPERTIES; AQUEOUS-SOLUTION; ANION-EXCHANGE; ELEMENT 105; N,N,N',N'-TETRAOCTYL DIGLYCOLAMIDE; SOLUTION CHEMISTRY; COMPLEX-FORMATION; FLUORIDE COMPLEXATION; BROMIDE COMPLEXES; HF/HNO3 SOLUTIONS AB A diglycolamide-based resin was characterized for Group 5 (Ta, Nb and pseudo-homolog Pa) separation from Group 4 (Hf and Zr) and tri-valent actinides (Am). The batch uptake of the radionuclides of interest were determined for HNO3/HF matrices and the results were used to develop a column separation method that could be used for element 105 (Db) purification chemistry. Tantalum is significantly retained by the TODGA resin, while Pa/Nb show little to no retention. The affinity for Ta decreases as a function of increased [HNO3], while Zr/Hf (and Am) affinities increase under the same conditions. Adsorption of Ta to polypropylene vials and column frits became a significant focus of this work following several observations made during the course of the column separation method development. All of the Group 5 elements were separated from Group 4 and Am while Ta may be completely isolated from Nb/Pa with the TODGA resin with improvements in column parameters: column height and bed volume. C1 [Despotopulos, J. D.; Gharibyan, N.; Henderson, R. A.; Moody, K. J.; Shaughnessy, D. A.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. [Despotopulos, J. D.; Sudowe, R.] Univ Nevada, Las Vegas, NV 89154 USA. [Gostic, J. M.] Airforce Tech Applicat Ctr, Brevard Country, FL 32925 USA. [Bennett, M. E.] Argonne Natl Lab, Argonne, IL 60439 USA. RP Despotopulos, JD (reprint author), Lawrence Livermore Natl Lab, 7000 East Ave,L-236, Livermore, CA 94550 USA. EM despotopulos1@llnl.gov FU U.S. Department of Energy by Lawrence Livermore National Laboratory [DE-AC52-07NA27344]; Laboratory Directed Research and Development Program at LLNL [11-ERD-011] FX The authors would like to thank Scott Tumey and Thomas Brown for their assistance in producing carrier-free radiotracers at CAMS. This work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344. This work was funded by the Laboratory Directed Research and Development Program at LLNL under project tracking code 11-ERD-011. NR 34 TC 0 Z9 0 U1 4 U2 14 PU SPRINGER PI DORDRECHT PA VAN GODEWIJCKSTRAAT 30, 3311 GZ DORDRECHT, NETHERLANDS SN 0236-5731 EI 1588-2780 J9 J RADIOANAL NUCL CH JI J. Radioanal. Nucl. Chem. PD JAN PY 2015 VL 303 IS 1 BP 485 EP 494 DI 10.1007/s10967-014-3398-1 PG 10 WC Chemistry, Analytical; Chemistry, Inorganic & Nuclear; Nuclear Science & Technology SC Chemistry; Nuclear Science & Technology GA AY0OB UT WOS:000347294600058 ER PT J AU Willingham, D Naes, BE Fahey, AJ AF Willingham, D. Naes, B. E. Fahey, A. J. TI Validating mass spectrometry measurements of nuclear materials via a non-contact volume analysis method of ion sputter craters SO JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY LA English DT Article DE Secondary ion mass spectrometry; Sputter yield; Useful yield; Uranium ID DEPTH PROFILES; ISOTOPE RATIOS; CAMECA IMS-4F; ICP-MS; SIMS; SURFACE; SILICON; ENERGY; IONIZATION; PARTICLES AB A combination of secondary ion mass spectrometry, optical profilometry and a statistically-driven algorithm was used to develop a non-contact volume analysis method to validate the useful yields of nuclear materials. The volume analysis methodology was applied to ion sputter craters created in silicon and uranium substrates sputtered by 18.5 keV O- and 6.0 keV Ar+ ions. Sputter yield measurements were determined from the volume calculations and were shown to be comparable to Monte Carlo calculations and previously reported experimental observations. Additionally, the volume calculations were used to determine the useful yields of Si+, SiO+ and SiO2 (+) ions from the silicon substrate and U+, UO+ and UO2 (+) ions from the uranium substrate under 18.5 keV O- and 6.0 keV Ar+ ion bombardment. This work represents the first steps toward validating the interlaboratory and cross-platform performance of mass spectrometry for the analysis of nuclear materials. C1 [Willingham, D.; Naes, B. E.] Pacific NW Natl Lab, Richland, WA 99352 USA. [Fahey, A. J.] US Naval Res Lab, Washington, DC 20375 USA. RP Willingham, D (reprint author), Pacific NW Natl Lab, 902 Battelle Blvd, Richland, WA 99352 USA. EM david.willingham@pnnl.gov RI Fahey, Albert/C-5611-2015; OI Willingham, David/0000-0002-7166-8994 NR 42 TC 0 Z9 0 U1 1 U2 15 PU SPRINGER PI DORDRECHT PA VAN GODEWIJCKSTRAAT 30, 3311 GZ DORDRECHT, NETHERLANDS SN 0236-5731 EI 1588-2780 J9 J RADIOANAL NUCL CH JI J. Radioanal. Nucl. Chem. PD JAN PY 2015 VL 303 IS 1 BP 655 EP 662 DI 10.1007/s10967-014-3313-9 PG 8 WC Chemistry, Analytical; Chemistry, Inorganic & Nuclear; Nuclear Science & Technology SC Chemistry; Nuclear Science & Technology GA AY0OB UT WOS:000347294600074 ER PT J AU Maxwell, SL Culligan, BK Hutchison, JB Utsey, RC McAlister, DR AF Maxwell, Sherrod L. Culligan, Brian K. Hutchison, Jay B. Utsey, Robin C. McAlister, Daniel R. TI Rapid determination of Sr-90 in seawater samples SO JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY LA English DT Article DE Rapid; Seawater; Sr-90; Radiostrontium; Fission products; Ocean studies AB A rapid method for Sr-90 in large seawater samples has been developed at the Savannah River National Laboratory (SRNL) to assay Sr-90 at very low levels. The new method employs novel pre-concentration steps to collect Y-90 quickly from up to 40 L of seawater to achieve a very low minimum detectable activity (MDA). An MDA for Sr-90 of similar to 150 A mu Bq L-1 may be obtained with this method using a 40 L seawater sample aliquot, counting 1,000 min with gas flow proportional counting. Following the pre-concentration of Y-90 from the seawater, DGA Resin is used to rapidly separate Y-90 from seawater samples and remove additional beta interferences. Gas flow proportional counting, liquid scintillation or Cerenkov counting may be used to count the purified Y-90 and determine Sr-90 present in the seawater sample. This new sample preparation method takes < 8 h. C1 [Maxwell, Sherrod L.; Culligan, Brian K.; Hutchison, Jay B.; Utsey, Robin C.] Savannah River Natl Lab, Aiken, SC 29808 USA. [McAlister, Daniel R.] PG Res Fdn Inc, Lisle, IL 60532 USA. RP Maxwell, SL (reprint author), Savannah River Natl Lab, Bldg 735-B, Aiken, SC 29808 USA. EM sherrod.maxwell@srs.gov FU Department of Energy, DOE [DE-AC09-96SR18500] FX This work was performed under the auspices of the Department of Energy, DOE Contract No. DE-AC09-96SR18500. The authors wish to acknowledge Staci Britt, Phil Demaere, Jack Herrington and Becky Chavous for their assistance with this work. NR 12 TC 4 Z9 4 U1 2 U2 9 PU SPRINGER PI DORDRECHT PA VAN GODEWIJCKSTRAAT 30, 3311 GZ DORDRECHT, NETHERLANDS SN 0236-5731 EI 1588-2780 J9 J RADIOANAL NUCL CH JI J. Radioanal. Nucl. Chem. PD JAN PY 2015 VL 303 IS 1 BP 709 EP 717 DI 10.1007/s10967-014-3391-8 PG 9 WC Chemistry, Analytical; Chemistry, Inorganic & Nuclear; Nuclear Science & Technology SC Chemistry; Nuclear Science & Technology GA AY0OB UT WOS:000347294600080 ER PT J AU Dion, MP Liezers, M Farmer, OT Miller, BW Morley, S Barinaga, C Eiden, G AF Dion, M. P. Liezers, Martin Farmer, Orville T., III Miller, Brian W. Morley, Shannon Barinaga, Charles Eiden, Greg TI Improving alpha spectrometry energy resolution by ion implantation with ICP-MS SO JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY LA English DT Article DE Alpha spectrometry; ICP-MS; Actinide ID DETECTORS; SPECTRA AB We report results of a novel technique using an inductively coupled plasma mass spectrometer as a method of sample preparation for alpha spectrometry. Two samples were produced, a low- and high-bias implant, the potential being the difference between the implant material and the exit ion lens. The two implants were imaged to reveal the geometrical distribution and radiometrically counted and compared to a traditional stipple and electrodeposited Am-241 sample. This method produced thin, contaminant free Am-241 samples which yielded energy resolution of keV full-width at half-maximum which is the lower limit of the large area (450 mm(2)) passivated implanted planar silicon detector used in this research. C1 [Dion, M. P.; Liezers, Martin; Farmer, Orville T., III; Miller, Brian W.; Morley, Shannon; Barinaga, Charles; Eiden, Greg] Pacific NW Natl Lab, Richland, WA 99354 USA. RP Dion, MP (reprint author), Pacific NW Natl Lab, MSIN J4-65,POB 999, Richland, WA 99354 USA. EM michael.dion@pnnl.gov OI Dion, Michael/0000-0002-3030-0050 NR 18 TC 3 Z9 3 U1 0 U2 4 PU SPRINGER PI DORDRECHT PA VAN GODEWIJCKSTRAAT 30, 3311 GZ DORDRECHT, NETHERLANDS SN 0236-5731 EI 1588-2780 J9 J RADIOANAL NUCL CH JI J. Radioanal. Nucl. Chem. PD JAN PY 2015 VL 303 IS 1 BP 877 EP 884 DI 10.1007/s10967-014-3500-8 PG 8 WC Chemistry, Analytical; Chemistry, Inorganic & Nuclear; Nuclear Science & Technology SC Chemistry; Nuclear Science & Technology GA AY0OB UT WOS:000347294600100 ER PT J AU Krogstad, JA Gao, Y Bai, JM Wang, J Lipkin, DM Levi, CG AF Krogstad, Jessica A. Gao, Yan Bai, Jianming Wang, Jun Lipkin, Don M. Levi, Carlos G. TI In Situ Diffraction Study of the High-Temperature Decomposition of t '-Zirconia SO JOURNAL OF THE AMERICAN CERAMIC SOCIETY LA English DT Article ID THERMAL BARRIER COATINGS; UNIT-CELL PARAMETERS; TETRAGONAL ZIRCONIA; POWDER DIFFRACTION; CRYSTAL-STRUCTURE; PHASE-STABILITY; EXPANSION COEFFICIENTS; LATTICE-PARAMETERS; SOLID-SOLUTIONS; ZRO2 AB The mechanisms of phase destabilization upon aging of the metastable t phase of yttria-stabilized zirconia (YSZ) are poorly understood, despite its broad application in thermal barrier coatings. To provide insight, synchrotron X-ray diffraction (XRD) with a quadrupole lamp furnace is used to examine the temperature response, including thermal expansion and phase evolution, of a 9mol% (8wt%) YO(1.5)t-8YSZ. The thermal expansion of equilibrated YSZ powders ranging from 0 to 18.4mol% YO1.5 is also investigated to better understand the effect of composition on the thermal expansion anisotropy. The T-0(c/t) temperature for t-8YSZ is estimated to be 1640 degrees C. Full decomposition of the t phase into a coherent mixture of a Y-lean tetragonal phase (t) and a Y-rich cubic phase (c) that coarsen over time is observed at elevated temperatures; however, upon quenching, the t phase reappears in the diffraction profile. This supports our evolving understanding that the t phase observed by XRD in aged samples is a microstructural artifact due to the coherency strain between the t and c phases. C1 [Krogstad, Jessica A.; Levi, Carlos G.] Univ Calif Santa Barbara, Dept Mat, Santa Barbara, CA 93106 USA. [Gao, Yan; Lipkin, Don M.] Gen Elect Global Res Ctr, Niskayuna, NY USA. [Bai, Jianming; Wang, Jun] Brookhaven Natl Lab, Natl Synchrotron Light Source, Brookhaven, NY USA. RP Krogstad, JA (reprint author), Univ Illinois, Dept Mat Sci & Engn, 1304 W Green St, Urbana, IL 61801 USA. EM jakrogst@illinois.edu RI Bai, Jianming/O-5005-2015 FU National Science Foundation [DMR-1105672, DMR-0605700]; US Department of Energy [DE-FC26-05NT42643]; NSF [DMR-1121053]; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-98CH10886] FX This investigation was supported by the National Science Foundation under Grants DMR-1105672 and DMR-0605700 (JAK, CGL), and by the US Department of Energy via Cooperative Agreement DE-FC26-05NT42643 (YG, DML). Any opinions, findings, conclusions, or other recommendations expressed are those of the authors and do not necessarily reflect the views of the US Department of Energy or the National Science Foundation. The research made use of the UCSB-MRL Central Facilities supported by NSF under grant DMR-1121053. Use of the National Synchrotron Light Source, Brookhaven National Laboratory, was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under contract no. DE-AC02-98CH10886 (JB, JW). Helpful discussions with Prof. R.M. McMeeking (UCSB) are gratefully acknowledged. NR 37 TC 3 Z9 3 U1 5 U2 30 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0002-7820 EI 1551-2916 J9 J AM CERAM SOC JI J. Am. Ceram. Soc. PD JAN PY 2015 VL 98 IS 1 BP 247 EP 254 DI 10.1111/jace.13249 PG 8 WC Materials Science, Ceramics SC Materials Science GA AY0QQ UT WOS:000347302000037 ER PT J AU Xu, HW Costa, GCC Stanek, CR Navrotsky, A AF Xu, Hongwu Costa, Gustavo C. C. Stanek, Christopher R. Navrotsky, Alexandra TI Structural Behavior of Ba1.24Al2.48Ti5.52O16 Hollandite at High Temperature: An In Situ Neutron Diffraction Study SO JOURNAL OF THE AMERICAN CERAMIC SOCIETY LA English DT Article ID SYNROC-TYPE HOLLANDITES; EFFECTIVE IONIC-RADII; BARIUM HOLLANDITES; WASTE FORMS; CESIUM; PHASE; IMMOBILIZATION; CHEMISTRY AB Titanate hollandites comprise a class of potential waste form phases for immobilization of radioactive Cs (and its daughter product Ba) due to their high thermal and aqueous stability. To study their structural behavior at high temperature, we conducted in situ neutron diffraction experiments of a representative tetragonal phase, Ba1.24Al2.48Ti5.52O16, in the temperature range 300-1173K. Rietveld analyses of the obtained data show that on heating, unit-cell parameters a and c increase at similar rates. This isotropic nature of thermal expansion can be explained by the increased volume and regularity of [(Ti,Al)O-6] octahedra and the widening of the Ti/Al-O2-Ti/Al angle (O2 is corner-shared by two [(Ti,Al)O-6] octahedra from neighboring [(Ti,Al)O-6] double chains) with increasing temperature. Practically, this property is advantageous, as hollandite-based ceramic or composite products would, upon heating, be less likely to form microcracks. The amplitudes of thermal vibration for Ba, Ti/Al, and O increase with increasing temperature; however, the rate of increase for Ba is much larger. This behavior is due to the occupancy of the box-shaped cavity site by Ba, which has weaker interactions with its neighboring atoms, compared with those for framework Ti/Al and O. On the other hand, the opening of the oxygen-coordinated cavity box is smaller than the size of Ba, even at high temperature, preventing evaporation of Ba from the hollandite structure. These characteristics render titanate hollandites potentially robust waste forms for Cs/Ba. C1 [Xu, Hongwu] Los Alamos Natl Lab, Div Earth & Environm Sci, Los Alamos, NM 87545 USA. [Costa, Gustavo C. C.; Navrotsky, Alexandra] Univ Calif Davis, Peter A Rock Thermochem Lab, Davis, CA 95616 USA. [Stanek, Christopher R.] Univ Calif Davis, NEAT ORU, Davis, CA 95616 USA. [Stanek, Christopher R.] Los Alamos Natl Lab, Mat Sci & Technol Div, Los Alamos, NM 87545 USA. RP Xu, HW (reprint author), Los Alamos Natl Lab, Div Earth & Environm Sci, Los Alamos, NM 87545 USA. EM hxu@lanl.gov OI Xu, Hongwu/0000-0002-0793-6923 FU Laboratory-Directed Research and Development (LDRD) program of Los Alamos National Laboratory under DOE [DE-AC52-06NA25396]; Department of Energy's Office of Basic Energy Sciences FX This work was supported by the Laboratory-Directed Research and Development (LDRD) program of Los Alamos National Laboratory, which is operated by Los Alamos National Security LLC, under DOE Contract DE-AC52-06NA25396. This work has benefited from the use of the Lujan Neutron Scattering Center at LANSCE, which is funded by the Department of Energy's Office of Basic Energy Sciences. NR 27 TC 3 Z9 3 U1 1 U2 20 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0002-7820 EI 1551-2916 J9 J AM CERAM SOC JI J. Am. Ceram. Soc. PD JAN PY 2015 VL 98 IS 1 BP 255 EP 262 DI 10.1111/jace.13245 PG 8 WC Materials Science, Ceramics SC Materials Science GA AY0QQ UT WOS:000347302000038 ER PT J AU Lim, HJ Battaile, CC Carroll, JD Boyce, BL Weinberger, CR AF Lim, Hojun Battaile, Corbett C. Carroll, Jay D. Boyce, Brad L. Weinberger, Christopher R. TI A physically based model of temperature and strain rate dependent yield in BCC metals: Implementation into crystal plasticity SO JOURNAL OF THE MECHANICS AND PHYSICS OF SOLIDS LA English DT Article DE Kink-pair theory; Temperature; Strain rate; Molybdenum; Tantalum; Tungsten; Niobium ID CENTERED-CUBIC METALS; UNIFIED CONSTITUTIVE MODEL; MOLYBDENUM SINGLE-CRYSTALS; TA-W ALLOYS; FLOW-STRESS; CRYSTALLOGRAPHIC TEXTURE; DEFORMATION-BEHAVIOR; SCREW DISLOCATIONS; LATTICE FRICTION; FCC METALS AB In this work, we develop a crystal plasticity finite element model (CP-FEM) that constitutively captures the temperature and strain rate dependent flow stresses in pure BCC refractory metals. This model is based on the kink-pair theory developed by Seeger (1981) and is calibrated to available data from single crystal experiments to produce accurate and convenient constitutive laws that are implemented into a BCC crystal plasticity model. The model is then used to predict temperature and strain rate dependent yield stresses of single and polycrystal BCC refractory metals (molybdenum, tantalum, tungsten and niobium) and compared with existing experimental data. To connect to larger length scales, classical continuum-scale constitutive models are fit to the CP-FEM predictions of polycrystal yield stresses. The results produced by this model, based on kink-pair theory and with origins in dislocation mechanics, show excellent agreement with the Mechanical Threshold Stress (MIS) model for temperature and strain-rate dependent flow. This framework provides a method to bridge multiple length scales in modeling the deformation of BCC metals. Published by Elsevier Ltd. C1 [Lim, Hojun; Battaile, Corbett C.; Carroll, Jay D.; Boyce, Brad L.] Sandia Natl Labs, Albuquerque, NM 87185 USA. [Weinberger, Christopher R.] Drexel Univ, Dept Mech Engn & Mech, Philadelphia, PA 19104 USA. RP Lim, HJ (reprint author), Sandia Natl Labs, POB 5800, Albuquerque, NM 87185 USA. EM hnlim@sandia.gov RI Carroll, Jay/K-2720-2012 OI Carroll, Jay/0000-0002-5818-4709 FU U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX Sandia National Laboratories is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy's National Nuclear Security Administration under Contract DE-AC04-94AL85000. NR 69 TC 12 Z9 12 U1 7 U2 44 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0022-5096 EI 1873-4782 J9 J MECH PHYS SOLIDS JI J. Mech. Phys. Solids PD JAN PY 2015 VL 74 BP 80 EP 96 DI 10.1016/j.jmps.2014.10.003 PG 17 WC Materials Science, Multidisciplinary; Mechanics; Physics, Condensed Matter SC Materials Science; Mechanics; Physics GA AY1PC UT WOS:000347363700006 ER PT J AU Hollis, K Liu, C Leckie, R Lovato, M AF Hollis, K. Liu, C. Leckie, R. Lovato, M. TI Bulge Testing and Interface Fracture Characterization of Plasma-Sprayed and HIP Bonded Zr Coatings on U-Mo SO JOURNAL OF THERMAL SPRAY TECHNOLOGY LA English DT Article; Proceedings Paper CT International Thermal Spray Conference (ITSC) CY MAY 21-23, 2014 CL German Welding Soc DVS, Barcelona, SPAIN SP ASM Int Thermal Spray Soc, Int Inst Welding HO German Welding Soc DVS DE adhesion test; bulge test; initiation fracture toughness; plasma spray; reactor fuel; transferred arc cleaning ID ZIRCONIUM AB Bulge testing using a pressurized fluid to fracture the interface between bonded material layers along with three-dimensional digital image correlation to measure the sample distortion caused by pressurized fluid was applied to plasma-sprayed coatings. The initiation fracture toughness associated with the bonded materials was measured during the testing. The bulge testing of the uranium-molybdenum alloy plasma sprayed with zirconium and clad in aluminum is presented. The initiation fracture toughness was observed to increase with the increasing cathodic arc-cleaning current and the use of alternating polarity transferred arc current. This dependence was linked to the interface composition of oxide and mixed metal phases along with the interface temperature during spray deposition. C1 [Hollis, K.; Liu, C.; Leckie, R.; Lovato, M.] Los Alamos Natl Lab, Los Alamos, NM USA. EM kjhollis@lanl.gov FU US Department of Energy Global Threat Reduction Initiative Reactor Convert program; National Nuclear Security Administration of the U.S. Department of Energy [DE-AC52-06NA25396] FX The authors gratefully thank Joel Montalvo for the metallographic preparation of the samples, and Beverly Aikin and Victor Vargas for the HIP cladding. The authors would like to acknowledge the financial support of the US Department of Energy Global Threat Reduction Initiative Reactor Convert program. The Los Alamos National Laboratory, an affirmative action, equal-opportunity employer, is operated by the Los Alamos National Security, LLC, for the National Nuclear Security Administration of the U.S. Department of Energy under contract DE-AC52-06NA25396. NR 13 TC 0 Z9 0 U1 3 U2 11 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1059-9630 EI 1544-1016 J9 J THERM SPRAY TECHN JI J. Therm. Spray Technol. PD JAN PY 2015 VL 24 IS 1-2 BP 271 EP 279 DI 10.1007/s11666-014-0198-7 PG 9 WC Materials Science, Coatings & Films SC Materials Science GA AY2JS UT WOS:000347416800032 ER PT J AU Rutqvist, J Dobson, PF Garcia, J Hartline, C Jeanne, P Oldenburg, CM Vasco, DW Walters, M AF Rutqvist, Jonny Dobson, Patrick F. Garcia, Julio Hartline, Craig Jeanne, Pierre Oldenburg, Curtis M. Vasco, Donald W. Walters, Mark TI The Northwest Geysers EGS Demonstration Project, California: Pre-stimulation Modeling and Interpretation of the Stimulation SO MATHEMATICAL GEOSCIENCES LA English DT Article DE EGS; Modeling; Coupled processes; Geomechanics; Induced seismicity; Fluid injection ID GEOTHERMAL-FIELD; FLUID-FLOW; ROCK; DEFORMATION; SEISMICITY; INJECTION; SYSTEM AB The Northwest Geysers Enhanced Geothermal System (EGS) demonstration project aims to create an EGS by directly and systematically injecting cool water at relatively low pressure into a known High Temperature (280-400 A degrees C) Zone (HTZ) located under the conventional (240 A degrees C) geothermal steam reservoir at The Geysers geothermal field in California. In this paper, the results of coupled thermal, hydraulic, and mechanical (THM) analyses made using a model developed as part of the pre-stimulation phase of the EGS demonstration project is presented. The model simulations were conducted in order to investigate injection strategies and the resulting effects of cold-water injection upon the EGS system; in particular to predict the extent of the stimulation zone for a given injection schedule. The actual injection began on October 6, 2011, and in this paper a comparison of pre-stimulation model predictions with micro-earthquake (MEQ) monitoring data over the first few months of a one-year injection program is presented. The results show that, by using a calibrated THM model based on historic injection and MEQ data at a nearby well, the predicted extent of the stimulation zone (defined as a zone of high MEQ density around the injection well) compares well with observed seismicity. The modeling indicates that the MEQ events are related to shear reactivation of preexisting fractures, which is triggered by the combined effects of injection-induced cooling around the injection well and small changes in steam pressure as far as half a kilometer away from the injection well. Pressure-monitoring data at adjacent wells and satellite-based ground-surface deformation data were also used to validate and further calibrate reservoir-scale hydraulic and mechanical model properties. The pressure signature monitored from the start of the injection was particularly useful for a precise back-calculation of reservoir porosity. The first few months of reservoir pressure and surface deformation data were useful for estimating the reservoir-rock permeability and elastic modulus. Finally, although the extent of the calculated stimulation zone matches the field observations over the first few months of injection, the observed surface deformations and MEQ evolution showed more heterogeneous behavior as a result of more complex geology, including minor faults and fracture zones that are important for consideration in the analysis of energy production and the long-term evolution of the EGS system. C1 [Rutqvist, Jonny; Dobson, Patrick F.; Jeanne, Pierre; Oldenburg, Curtis M.; Vasco, Donald W.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Garcia, Julio; Hartline, Craig; Walters, Mark] Calpine Corp, Middletown, CA 95461 USA. RP Rutqvist, J (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. EM Jrutqvist@lbl.gov RI Dobson, Patrick/D-8771-2015; Oldenburg, Curtis/L-6219-2013; Rutqvist, Jonny/F-4957-2015; Jeanne, Pierre/I-2996-2015; Vasco, Donald/I-3167-2016; Vasco, Donald/G-3696-2015; OI Dobson, Patrick/0000-0001-5031-8592; Oldenburg, Curtis/0000-0002-0132-6016; Rutqvist, Jonny/0000-0002-7949-9785; Jeanne, Pierre/0000-0003-1487-8378; Vasco, Donald/0000-0003-1210-8628; Vasco, Donald/0000-0003-1210-8628; Walters, Mark/0000-0001-8458-4813 FU US Department under the US Department of Energy [DE-AC02-05CH11231]; Calpine Corporation FX This work was conducted with funding by the Assistant Secretary for Energy Efficiency and Renewable Energy, Geothermal Technologies Program, of the US Department under the US Department of Energy Contract No. DE-AC02-05CH11231, and by Calpine Corporation. NR 30 TC 14 Z9 15 U1 1 U2 21 PU SPRINGER HEIDELBERG PI HEIDELBERG PA TIERGARTENSTRASSE 17, D-69121 HEIDELBERG, GERMANY SN 1874-8961 EI 1874-8953 J9 MATH GEOSCI JI Math Geosci. PD JAN PY 2015 VL 47 IS 1 SI SI BP 3 EP 29 DI 10.1007/s11004-013-9493-y PG 27 WC Geosciences, Multidisciplinary; Mathematics, Interdisciplinary Applications SC Geology; Mathematics GA AY6SD UT WOS:000347694900002 ER PT J AU Williams, PT Thompson, PD AF Williams, Paul T. Thompson, Paul D. TI In reply-Cardiovascular Disease Mortality and Excessive Exercise in Heart Attack Survivors SO MAYO CLINIC PROCEEDINGS LA English DT Letter ID PHYSICAL-ACTIVITY; RISK-FACTORS; FITNESS; MEN C1 [Williams, Paul T.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Thompson, Paul D.] Hartford Hosp, Hartford, CT 06115 USA. RP Williams, PT (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. NR 8 TC 0 Z9 0 U1 0 U2 1 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 0025-6196 EI 1942-5546 J9 MAYO CLIN PROC JI Mayo Clin. Proc. PD JAN PY 2015 VL 90 IS 1 BP 159 EP 160 DI 10.1016/j.mayocp.2014.11.006 PG 2 WC Medicine, General & Internal SC General & Internal Medicine GA AY2ZW UT WOS:000347455400021 PM 25572201 ER PT J AU Su, JQ Ding, LJ Xue, K Yao, HY Quensen, J Bai, SJ Wei, WX Wu, JS Zhou, JZ Tiedje, JM Zhu, YG AF Su, Jian-Qiang Ding, Long-Jun Xue, Kai Yao, Huai-Ying Quensen, John Bai, Shi-Jie Wei, Wen-Xue Wu, Jin-Shui Zhou, Jizhong Tiedje, James M. Zhu, Yong-Guan TI Long-term balanced fertilization increases the soil microbial functional diversity in a phosphorus-limited paddy soil SO MOLECULAR ECOLOGY LA English DT Article DE 16S rRNA gene pyrosequencing; chemical fertilizer; geochip; long-term fertilization; soil microbial community ID BACTERIAL COMMUNITY STRUCTURE; ORGANIC-MATTER; ENZYME-ACTIVITIES; MINERAL FERTILIZERS; MANURE APPLICATIONS; AGRICULTURAL SOIL; TUNDRA SOIL; ARABLE SOIL; NITROGEN; RESPONSES AB The influence of long-term chemical fertilization on soil microbial communities has been one of the frontier topics of agricultural and environmental sciences and is critical for linking soil microbial flora with soil functions. In this study, 16S rRNA gene pyrosequencing and a functional gene array, geochip 4.0, were used to investigate the shifts in microbial composition and functional gene structure in paddy soils with different fertilization treatments over a 22-year period. These included a control without fertilizers; chemical nitrogen fertilizer (N); N and phosphate (NP); N and potassium (NK); and N, P and K (NPK). Based on 16S rRNA gene data, both species evenness and key genera were affected by P fertilization. Functional gene array-based analysis revealed that long-term fertilization significantly changed the overall microbial functional structures. Chemical fertilization significantly increased the diversity and abundance of most genes involved in C, N, P and S cycling, especially for the treatments NK and NPK. Significant correlations were found among functional gene structure and abundance, related soil enzymatic activities and rice yield, suggesting that a fertilizer-induced shift in the microbial community may accelerate the nutrient turnover in soil, which in turn influenced rice growth. The effect of N fertilization on soil microbial functional genes was mitigated by the addition of P fertilizer in this P-limited paddy soil, suggesting that balanced chemical fertilization is beneficial to the soil microbial community and its functions. C1 [Su, Jian-Qiang; Yao, Huai-Ying; Zhu, Yong-Guan] Chinese Acad Sci, Inst Urban Environm, Key Lab Urban Environm & Hlth, Xiamen 361021, Peoples R China. [Ding, Long-Jun; Zhu, Yong-Guan] Chinese Acad Sci, State Key Lab Urban & Reg Ecol, Res Ctr Ecoenvironm Sci, Beijing 100085, Peoples R China. [Xue, Kai; Bai, Shi-Jie; Zhou, Jizhong] Univ Oklahoma, Inst Environm Genom, Dept Microbiol & Plant Biol, Norman, OK 73019 USA. [Quensen, John; Tiedje, James M.] Michigan State Univ, Dept Plant Soil & Microbial Sci, Ctr Microbial Ecol, E Lansing, MI 48824 USA. [Wei, Wen-Xue; Wu, Jin-Shui] Chinese Acad Sci, Inst Subtrop Agr, Key Lab Agroecol Proc Subtrop Reg, Changsha 410125, Hunan, Peoples R China. [Wei, Wen-Xue; Wu, Jin-Shui] Chinese Acad Sci, Inst Subtrop Agr, Taoyuan Stn Agroecol Res, Changsha 410125, Hunan, Peoples R China. [Zhou, Jizhong] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, Berkeley, CA 94720 USA. [Zhou, Jizhong] Tsinghua Univ, Sch Environm, State Key Joint Lab Environm Simulat & Pollut Con, Beijing 100084, Peoples R China. RP Zhu, YG (reprint author), Chinese Acad Sci, Inst Urban Environm, Key Lab Urban Environm & Hlth, Xiamen 361021, Peoples R China. EM ygzhu@iue.ac.cn RI Zhu, Yong-Guan/A-1412-2009; CAS, KLUEH/G-8978-2016; Su, Jian Qiang/C-2388-2009; SPRP, XDB150200/N-7373-2016 OI Zhu, Yong-Guan/0000-0003-3861-8482; Su, Jian Qiang/0000-0003-1875-249X; FU National Natural Science Foundation of China [41090282, 31270153]; Strategic Priority Research Program of Chinese Academy of Sciences [XDB15020302] FX This work was supported by the National Natural Science Foundation of China (41090282, 31270153) and the Strategic Priority Research Program of Chinese Academy of Sciences, Grant No. XDB15020302. NR 72 TC 22 Z9 25 U1 27 U2 145 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0962-1083 EI 1365-294X J9 MOL ECOL JI Mol. Ecol. PD JAN PY 2015 VL 24 IS 1 BP 136 EP 150 DI 10.1111/mec.13010 PG 15 WC Biochemistry & Molecular Biology; Ecology; Evolutionary Biology SC Biochemistry & Molecular Biology; Environmental Sciences & Ecology; Evolutionary Biology GA AY2WF UT WOS:000347446300011 PM 25410123 ER PT J AU Deng, J Gu, YF Zhang, J Xue, K Qin, YJ Yuan, M Yin, HQ He, ZL Wu, LY Schuur, EAG Tiedje, JM Zhou, J AF Deng, Jie Gu, Yunfu Zhang, Jin Xue, Kai Qin, Yujia Yuan, Mengting Yin, Huaqun He, Zhili Wu, Liyou Schuur, Edward A. G. Tiedje, James M. Zhou, Jizhong TI Shifts of tundra bacterial and archaeal communities along a permafrost thaw gradient in Alaska SO MOLECULAR ECOLOGY LA English DT Article DE 16S rRNA; Illumina MiSeq sequencing; permafrost thaw; soil bacterial and archaeal communities ID SP-NOV.; MICROBIAL COMMUNITIES; WARMING ALTERS; ARCTIC TUNDRA; ACTIVE LAYER; LENA DELTA; SOIL; CARBON; METHANOGENESIS; DIVERSITY AB Understanding the response of permafrost microbial communities to climate warming is crucial for evaluating ecosystem feedbacks to global change. This study investigated soil bacterial and archaeal communities by Illumina MiSeq sequencing of 16S rRNA gene amplicons across a permafrost thaw gradient at different depths in Alaska with thaw progression for over three decades. Over 4.6million passing 16S rRNA gene sequences were obtained from a total of 97 samples, corresponding to 61 known classes and 470 genera. Soil depth and the associated soil physical-chemical properties had predominant impacts on the diversity and composition of the microbial communities. Both richness and evenness of the microbial communities decreased with soil depth. Acidobacteria, Verrucomicrobia, Alpha- and Gamma-Proteobacteria dominated the microbial communities in the upper horizon, whereas abundances of Bacteroidetes, Delta-Proteobacteria and Firmicutes increased towards deeper soils. Effects of thaw progression were absent in microbial communities in the near-surface organic soil, probably due to greater temperature variation. Thaw progression decreased the abundances of the majority of the associated taxa in the lower organic soil, but increased the abundances of those in the mineral soil, including groups potentially involved in recalcitrant C degradation (Actinomycetales, Chitinophaga, etc.). The changes in microbial communities may be related to altered soil C sources by thaw progression. Collectively, this study revealed different impacts of thaw in the organic and mineral horizons and suggests the importance of studying both the upper and deeper soils while evaluating microbial responses to permafrost thaw. C1 [Deng, Jie; Gu, Yunfu; Zhang, Jin; Xue, Kai; Qin, Yujia; Yuan, Mengting; Yin, Huaqun; He, Zhili; Wu, Liyou; Zhou, Jizhong] Univ Oklahoma, Dept Microbiol & Plant Biol, Inst Environm Genom, Norman, OK 73019 USA. [Gu, Yunfu] Sichuan Agr Univ, Coll Resource & Environm, Chengdu, Sichuan, Peoples R China. [Yin, Huaqun] Cent S Univ, Sch Mineral Proc & Bioengn, Changsha, Hunan, Peoples R China. [Schuur, Edward A. G.] Univ Florida, Dept Biol, Gainesville, FL USA. [Tiedje, James M.] Michigan State Univ, Ctr Microbial Ecol, E Lansing, MI 48824 USA. [Zhou, Jizhong] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, Berkeley, CA 94720 USA. [Zhou, Jizhong] Tsinghua Univ, State Key Joint Lab Environm Simulat & Pollut Con, Sch Environm, Beijing 100084, Peoples R China. RP Zhou, JZ (reprint author), Univ Oklahoma, Dept Microbiol & Plant Biol, Inst Environm Genom, Norman, OK 73019 USA. EM jzhou@ou.edu FU Department of Energy (DOE) [DE-FOA-0000866] FX This work is supported by the Department of Energy (DOE) under grant DE-FOA-0000866 aiming to investigate the role of microbial communities in carbon cycling especially under global warming. NR 67 TC 7 Z9 8 U1 13 U2 95 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0962-1083 EI 1365-294X J9 MOL ECOL JI Mol. Ecol. PD JAN PY 2015 VL 24 IS 1 BP 222 EP 234 DI 10.1111/mec.13015 PG 13 WC Biochemistry & Molecular Biology; Ecology; Evolutionary Biology SC Biochemistry & Molecular Biology; Environmental Sciences & Ecology; Evolutionary Biology GA AY2WF UT WOS:000347446300016 PM 25424441 ER PT J AU Buck, PM Chaudhri, A Kumar, S Singh, SK AF Buck, Patrick M. Chaudhri, Anuj Kumar, Sandeep Singh, Satish K. TI Highly Viscous Antibody Solutions Are a Consequence of Network Formation Caused by Domain-Domain Electrostatic Complementarities: Insights from Coarse-Grained Simulations SO MOLECULAR PHARMACEUTICS LA English DT Article DE viscosity; mAB; high concentration; coarse-grained; simulations; drug development ID CONCENTRATED MONOCLONAL-ANTIBODY; REVERSIBLE SELF-ASSOCIATION; ANGLE NEUTRON-SCATTERING; CLUSTER FORMATION; SOLUTION VISCOSITY; DIFFUSION; RHEOLOGY; MODEL AB Therapeutic monoclonal antibody (mAb) candidates that form highly viscous solutions at concentrations above 100 mg/mL can lead to challenges in bioprocessing, formulation development, and subcutaneous drug delivery. Earlier studies of mAbs with concentration-dependent high viscosity have indicated that mAbs with negatively charged Fv regions have a dipole-like quality that increases the likelihood of reversible self-association. This suggests that weak electrostatic intermolecular interactions can form transient antibody networks that participate in resistance to solution deformation under shear stress. Here this hypothesis is explored by parametrizing a coarse-grained (CG) model of an antibody using the domain charges from four different mAbs that have had their concentration-dependent viscosity behaviors previously determined. Multicopy molecular dynamics simulations were performed for these four CG mAbs at several concentrations to understand the effect of surface charge on mass diffusivity, pairwise interactions, and electrostatic network formation. Diffusion coefficients computed from simulations were in qualitative agreement with experimentally determined viscosities for all four mAbs. Contact analysis revealed an overall greater number of pairwise interactions for the two mAbs in this study with high concentration viscosity issues. Further, using equilibrated solution trajectories, the two mAbs with high concentration viscosity issues quantitatively formed more features of an electrostatic network than the other mAbs. The change in the number of these network features as a function of concentration is related to the number of pairwise interactions formed by electrostatic complementarities between antibody domains. Thus, transient antibody network formation caused by domain-domain electrostatic complementarities is the most probable origin of high concentration viscosity for mAbs in this study. C1 [Buck, Patrick M.; Kumar, Sandeep; Singh, Satish K.] Pfizer Inc, Biotherapeut Pharmaceut Sci Res & Dev, Pharmaceut Res & Dev, Chesterfield, MO 63017 USA. [Chaudhri, Anuj] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Computat Res Div, Berkeley, CA 94720 USA. RP Kumar, S (reprint author), Pfizer Inc, Biotherapeut Pharmaceut Sci Res & Dev, Pharmaceut Res & Dev, 700 Chesterfield Pkwy West, Chesterfield, MO 63017 USA. EM sandeep.kumar@pfizer.com FU Pfizer Corporation FX Pfizer Business Technology is thanked for computational facilities. A postdoctoral fellowship to P.M.B. by Pfizer Corporation is gratefully acknowledged. Numerous helpful discussions with Monika Geiger, Pilarin Nichols, Li Li, Donna Luisi, and others on viscosity behaviors of antibodies are acknowledged. NR 25 TC 9 Z9 9 U1 5 U2 19 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 1543-8384 J9 MOL PHARMACEUT JI Mol. Pharm. PD JAN PY 2015 VL 12 IS 1 BP 127 EP 139 DI 10.1021/mp500485w PG 13 WC Medicine, Research & Experimental; Pharmacology & Pharmacy SC Research & Experimental Medicine; Pharmacology & Pharmacy GA AY3TX UT WOS:000347506300013 PM 25383990 ER PT J AU Chen-Wiegart, YCK Figueroa-Santos, MA Petrash, S Garcia-Miralles, J Wang, J AF Chen-Wiegart, Yu-chen Karen Figueroa-Santos, Miriam Aileen Petrash, Stanislas Garcia-Miralles, Jose Wang, Jun TI Critical factors affecting the 3D microstructural formation in hybrid conductive adhesive materials studied by X-ray nano-tomography SO NANOSCALE LA English DT Article ID ELECTRONICS; RESISTANCE AB Conductive adhesives are found favorable in a wide range of applications including a lead-free solder in micro-chips, flexible and printable electronics and enhancing the performance of energy storage devices. Composite materials comprised of metallic fillers and a polymer matrix are of great interest to be implemented as hybrid conductive adhesives. Here we investigated a cost-effective conductive adhesive material consisting of silver-coated copper as micro-fillers using synchrotron-based three-dimensional (3D) X-ray nano-tomography. The key factors affecting the quality and performance of the material were quantitatively studied in 3D on the nanometer scale for the first time. A critical characteristic parameter, defined as a shape-factor, was determined to yield a high-quality silver coating, leading to satisfactory performance. A 'stack-and-screen' mechanism was proposed to elaborate such a phenomenon. The findings and the technique developed in this work will facilitate the future advancement of conductive adhesives to have a great impact in micro-electronics and other applications. C1 [Chen-Wiegart, Yu-chen Karen; Figueroa-Santos, Miriam Aileen; Wang, Jun] Brookhaven Natl Lab, Photon Sci Directorate, Upton, NY 11973 USA. [Figueroa-Santos, Miriam Aileen] Univ Puerto Rico, Dept Mech Engn, Mayaguez, PR 00681 USA. [Petrash, Stanislas; Garcia-Miralles, Jose] Henkel Corp, Bridgewater, NJ 08807 USA. RP Wang, J (reprint author), Brookhaven Natl Lab, Photon Sci Directorate, Upton, NY 11973 USA. EM junwang@bnl.gov NR 11 TC 2 Z9 2 U1 3 U2 17 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2040-3364 EI 2040-3372 J9 NANOSCALE JI Nanoscale PY 2015 VL 7 IS 3 BP 908 EP 913 DI 10.1039/c4nr06068g PG 6 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA AY1SZ UT WOS:000347373500009 PM 25474162 ER PT J AU Kumar, R Bocharova, V Strelcov, E Tselev, A Kravchenko, II Berdzinski, S Strehmel, V Ovchinnikova, OS Minutolo, JA Sangoro, JR Agapov, AL Sokolov, AP Kalinin, SV Sumpter, BG AF Kumar, Rajeev Bocharova, Vera Strelcov, Evgheni Tselev, Alexander Kravchenko, Ivan I. Berdzinski, Stefan Strehmel, Veronika Ovchinnikova, Olga S. Minutolo, Joseph A. Sangoro, Joshua R. Agapov, Alexander L. Sokolov, Alexei P. Kalinin, Sergei V. Sumpter, Bobby G. TI Ion transport and softening in a polymerized ionic liquid SO NANOSCALE LA English DT Article ID POLY(IONIC LIQUID)S; FORCE MICROSCOPY; ELECTROLYTES; INTERFACE; FILMS; CRYSTALLIZATION; CONDUCTIVITY; SPECTROSCOPY; INSTABILITY; FREQUENCY AB Polymerized ionic liquids (PolyILs) are promising materials for various solid state electronic applications such as dye-sensitized solar cells, lithium batteries, actuators, field-effect transistors, light emitting electrochemical cells, and electrochromic devices. However, fundamental understanding of interconnection between ionic transport and mechanical properties in PolyILs is far from complete. In this work, local charge transport and structural changes in films of a PolyIL are studied using an integrated experiment-theory based approach. Experimental data for the kinetics of charging and steady state current-voltage relations can be explained by taking into account the dissociation of ions under an applied electric field (known as the Wien effect). Onsager's theory of the Wien effect coupled with the Poisson-Nernst-Planck formalism for the charge transport is found to be in excellent agreement with the experimental results. The agreement between the theory and experiments allows us to predict structural properties of the PolyIL films. We have observed significant softening of the PolyIL films beyond certain threshold voltages and formation of holes under a scanning probe microscopy (SPM) tip, through which an electric field was applied. The observed softening is explained by the theory of depression in glass transition temperature resulting from enhanced dissociation of ions with an increase in applied electric field. C1 [Kumar, Rajeev; Sumpter, Bobby G.] Oak Ridge Natl Lab, Comp Sci & Math Div, Oak Ridge, TN 37831 USA. [Kumar, Rajeev; Strelcov, Evgheni; Tselev, Alexander; Kravchenko, Ivan I.; Kalinin, Sergei V.; Sumpter, Bobby G.] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. [Bocharova, Vera; Ovchinnikova, Olga S.; Sokolov, Alexei P.] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. [Berdzinski, Stefan; Strehmel, Veronika] Univ Appl Sci, Hsch Niederrhein, Dept Chem, D-47798 Krefeld, Germany. [Berdzinski, Stefan; Strehmel, Veronika] Univ Appl Sci, Hsch Niederrhein, Inst Coatings & Surface Chem, D-47798 Krefeld, Germany. [Minutolo, Joseph A.; Sangoro, Joshua R.] Univ Tennessee, Dept Chem & Biomol Engn, Knoxville, TN 37996 USA. [Agapov, Alexander L.; Sokolov, Alexei P.] Univ Tennessee, Dept Chem, Knoxville, TN 37996 USA. RP Kumar, R (reprint author), Oak Ridge Natl Lab, Comp Sci & Math Div, Oak Ridge, TN 37831 USA. EM kumarr@ornl.gov RI Strelcov, Evgheni/H-1654-2013; Kravchenko, Ivan/K-3022-2015; Tselev, Alexander/L-8579-2015; Sumpter, Bobby/C-9459-2013; Kumar, Rajeev/Q-2255-2015; Kalinin, Sergei/I-9096-2012 OI Kravchenko, Ivan/0000-0003-4999-5822; Tselev, Alexander/0000-0002-0098-6696; Sumpter, Bobby/0000-0001-6341-0355; Kumar, Rajeev/0000-0001-9494-3488; Kalinin, Sergei/0000-0001-5354-6152 FU Laboratory Directed Research and Development (LDRD) Program of Oak Ridge National Laboratory (ORNL); Division of Chemical Sciences, Geosciences, and Bio-sciences, Office of Basic Energy Sciences, United States Department of Energy [DE-AC05-00OR22725]; Oak Ridge National Laboratory (ORNL); Office of Science of the U.S. Department of Energy [DE-AC05-00OR22725]; Division of Materials Sciences and Engineering, DOE Office of Basic Energy Sciences; Science Alliance at the University of Tennessee, Knoxville, through the JDRD Collaborative Cohort Program Fellowship; German Science Foundation (DFG) [SPP 1191] FX This research was sponsored by the Laboratory Directed Research and Development (LDRD) Program of Oak Ridge National Laboratory (ORNL), and managed by UT-Battelle, LLC, for the U.S. Department of Energy. Experimental part of this research was conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility (user proposal #CNMS2013-238). OO acknowledges support by the Division of Chemical Sciences, Geosciences, and Bio-sciences, Office of Basic Energy Sciences, United States Department of Energy under Contract DE-AC05-00OR22725 with Oak Ridge National Laboratory (ORNL), managed and operated by UT-Battelle, LLC. Calculations made use of resources at the Oak Ridge Leadership Computing Facility at the Oak Ridge National Laboratory, which is supported by the Office of Science of the U.S. Department of Energy under Contract DE-AC05-00OR22725. APS acknowledges support from the Division of Materials Sciences and Engineering, DOE Office of Basic Energy Sciences. JAM and JRS acknowledge financial by the Science Alliance at the University of Tennessee, Knoxville, through the JDRD Collaborative Cohort Program Fellowship. SB and VS acknowledge support by the German Science Foundation (DFG) through SPP 1191 program on Ionic Liquids. NR 49 TC 6 Z9 6 U1 4 U2 98 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2040-3364 EI 2040-3372 J9 NANOSCALE JI Nanoscale PY 2015 VL 7 IS 3 BP 947 EP 955 DI 10.1039/c4nr05491a PG 9 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA AY1SZ UT WOS:000347373500015 PM 25463322 ER PT J AU Shen, J Cui, HZ Huang, XP Gong, MG Qin, W Kirkeminde, A Cui, J Ren, SQ AF Shen, Jian Cui, Huizhong Huang, Xiaopeng Gong, Maogang Qin, Wei Kirkeminde, Alec Cui, Jun Ren, Shenqiang TI Synthesis and characterization of rare-earth-free magnetic manganese bismuth nanocrystals SO RSC ADVANCES LA English DT Article ID LOW-TEMPERATURE PHASE; NANOCOMPOSITE MAGNETS; CHEMICAL-SYNTHESIS; PERMANENT-MAGNETS; MNBI; COERCIVITY AB Earth abundant manganese bismuth (MnBi) has long been of interest due to its largemagnetocrystalline anisotropy and high energy density for advanced permanent magnet applications. However, solution synthesis of MnBi phase is challenging due to the reduction potential mismatch between Mn and Bi elements. In this study, we show a versatile MnBi synthesis method involving the metal co-reduction followed by thermal annealing. The magnetically hard MnBi crystalline phase is then exchange coupled with magnetically soft cobalt coating. Our processing approach offers a promising strategy for manufacturing rare-earth-free magnetic nanocrystals. C1 [Shen, Jian; Cui, Huizhong; Huang, Xiaopeng; Gong, Maogang; Qin, Wei; Kirkeminde, Alec; Ren, Shenqiang] Univ Kansas, Dept Chem, Lawrence, KS 66045 USA. [Cui, Jun] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Ren, SQ (reprint author), Univ Kansas, Dept Chem, Lawrence, KS 66045 USA. EM shenqiang@ku.edu RI Gong, Maogang/B-3588-2016 OI Gong, Maogang/0000-0002-2031-781X FU National Science Foundation [NSF-CMMI-1332658]; U.S. Department of Energy's Advanced Research Projects Agency-Energy (ARPA-E) [11/CJ000/09/03] FX S.R. thanks the financial support from the National Science Foundation under Award no. NSF-CMMI-1332658 for material synthesis and assembly. The U.S. Department of Energy's Advanced Research Projects Agency-Energy (ARPA-E) under contract no. 11/CJ000/09/03 is acknowledged (J.C at Pacific Northwest National Laboratory, and S.R. at the University of Kansas). NR 23 TC 4 Z9 4 U1 5 U2 58 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2046-2069 J9 RSC ADV JI RSC Adv. PY 2015 VL 5 IS 8 BP 5567 EP 5570 DI 10.1039/c4ra12440e PG 4 WC Chemistry, Multidisciplinary SC Chemistry GA AY0RQ UT WOS:000347304900012 ER PT J AU Goodwin, A Bobade, S Kang, NG Baskaran, D Hong, KL Mays, J AF Goodwin, Andrew Bobade, Sachin Kang, Nam-Goo Baskaran, Durairaj Hong, Kunlun Mays, Jimmy TI Poly(styrene-graft-hyperbranched polyglycidol): synthesis and solution behavior of a hyperbranched polyelectrolyte SO RSC ADVANCES LA English DT Article ID TRANSFER RADICAL POLYMERIZATION; FRAGMENTATION CHAIN-TRANSFER; DYNAMIC LIGHT-SCATTERING; DENDRITIC SIDE-GROUPS; MOLECULAR-WEIGHT; POLY(ETHYLENE OXIDE); DENDRONIZED POLYMERS; GRAFT-COPOLYMERS; AQUEOUS-SOLUTION; LINEAR-POLYMERS AB This work presents a three-step synthetic procedure to obtain a hypergrafted copolymer composed of a glassy backbone with flexible branched pendant segments. The desired hypergrafted structure was obtained by using a polyfunctional macroinitiator, linear poly(styreneco-4-hydroxystyrene), to yield polystyrene-graft-hyperbranched polyglycidol with randomly placed branch junctions. Atomic force microscopy, dynamic light scattering, and viscometry probed the aggregation and viscometric behavior of the polymer in DMF and DMF-LiBr solutions. The polymer exhibited polyelectrolyte behavior demonstrated by a large increase in the reduced viscosity prior to neutralization with LiBr salt. Additionally, conformational changes were observed by dynamic light scattering in both the average aggregate size and aggregate population with the addition of LiBr salt. C1 [Goodwin, Andrew; Bobade, Sachin; Kang, Nam-Goo; Baskaran, Durairaj; Mays, Jimmy] Univ Tennessee, Dept Chem, Knoxville, TN 37996 USA. [Hong, Kunlun] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. [Mays, Jimmy] Oak Ridge Natl Lab, Chem Sci Div, Oak Ridge, TN 37831 USA. RP Goodwin, A (reprint author), Univ Tennessee, Dept Chem, Knoxville, TN 37996 USA. EM Goodwin@ion.chem.utk.edu; Jimmymays@utk.edu RI Hong, Kunlun/E-9787-2015 OI Hong, Kunlun/0000-0002-2852-5111 FU TN- SCORE program, Thrust 2 [NSF-EPS-1004083]; Oak Ridge National Laboratory by Office of Basic Energy Sciences, U.S. Department of Energy FX The authors would like to thank Kevin Huerto for experimental assistance and the TN- SCORE program, Thrust 2, (NSF-EPS-1004083) for financial support. Andrew Goodwin and Sachin Bobade would like to thank Mr Tom Malmgren, Polymer Characterization Laboratory, University of Tennessee, for assistance in sample characterization. A portion of this research was conducted at the Center for Nanophase Materials Sciences, which is sponsored at Oak Ridge National Laboratory by Office of Basic Energy Sciences, U.S. Department of Energy. NR 43 TC 1 Z9 1 U1 0 U2 32 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2046-2069 J9 RSC ADV JI RSC Adv. PY 2015 VL 5 IS 8 BP 5611 EP 5616 DI 10.1039/c4ra11568f PG 6 WC Chemistry, Multidisciplinary SC Chemistry GA AY0RQ UT WOS:000347304900018 ER PT J AU Yang, N Yee, JK Zhang, ZH Kurmanaeva, L Cappillino, P Stavila, V Lavernia, EJ Marchi, CS AF Yang, Nancy Yee, Joshua K. Zhang, Zhihui Kurmanaeva, Lilia Cappillino, Patrick Stavila, Vitalie Lavernia, Enrique J. Marchi, Chris San TI Hydrogen sorption characteristics of nanostructured Pd-10Rh processed by cryomilling SO ACTA MATERIALIA LA English DT Article DE Palladium; Hydrogen; Cryomilling ID SEVERE PLASTIC-DEFORMATION; METAL-HYDRIDES; PD-RH; NANOCRYSTALLINE PALLADIUM; INTERMETALLIC HYDRIDES; MECHANICAL ATTRITION; STORAGE PROPERTIES; SLOPING PLATEAUS; MISCIBILITY GAP; BEHAVIOR AB Palladium and its alloys are model systems for studying the solid-state storage of hydrogen. Mechanical milling is commonly used to process complex powder systems for solid-state hydrogen storage; however, milling can also be used to evolve nanostructured powder to modify hydrogen sorption characteristics. In the present study, cryomilling (mechanical attrition milling in a cryogenic liquid) is used to produce nanostructured palladium rhodium alloy powder. Characterization of the cryomilled Pd-10Rh using electron microscopy, X-ray diffraction and surface area analysis reveal that (i) particle morphology evolves from spherical to flattened disk-like particles; while (ii) crystallite size decreases from several microns to less than 100 nm; and (iii) dislocation density increases with increased cryomilling time. Hydrogen absorption and desorption isotherms as well as the time scales for absorption were measured for cryomilled Pd-10Rh, and correlated with observed microstructural changes induced by the cryomilling process. In short, as the microstructure of the Pd-10Rh alloy is refined by cryomilling: (i) the maximum hydrogen concentration in the a-phase increases, (ii) the pressure plateau becomes flatter and (iii) the equilibrium hydrogen capacity increases at pressure of 101.3 kPa. Additionally, the rate of hydrogen absorption was reduced by an order of magnitude compared to non-cryomilled (atomized) powder. (C) 2014 Published by Elsevier Ltd. on behalf of Acta Materialia Inc. C1 [Yang, Nancy; Cappillino, Patrick; Stavila, Vitalie; Marchi, Chris San] Sandia Natl Labs, Livermore, CA 94550 USA. [Yee, Joshua K.; Zhang, Zhihui; Kurmanaeva, Lilia; Lavernia, Enrique J.] Univ Calif Davis, Davis, CA 95616 USA. RP Marchi, CS (reprint author), Sandia Natl Labs, Livermore, CA 94550 USA. EM cwsanma@sandia.gov FU Sandia National Laboratories [826008]; US Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX Work at UC Davis was supported by Sandia National Laboratories under contract no. 826008. Sandia National Laboratories is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of the Lockheed Martin Corporation, for the US Department of Energy's National Nuclear Security Administration under contract no. DE-AC04-94AL85000. J.K.Y. would like to acknowledge the support of the Campus Executive Fellowship from Sandia National Laboratories. NR 60 TC 1 Z9 1 U1 6 U2 25 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 1359-6454 EI 1873-2453 J9 ACTA MATER JI Acta Mater. PD JAN 1 PY 2015 VL 82 BP 41 EP 50 DI 10.1016/j.actamat.2014.08.056 PG 10 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Materials Science; Metallurgy & Metallurgical Engineering GA AX6FE UT WOS:000347017800005 ER PT J AU Tourret, D Karma, A AF Tourret, D. Karma, A. TI Growth competition of columnar dendritic grains: A phase-field study SO ACTA MATERIALIA LA English DT Article DE Microstructure selection; Dendritic growth; Directional solidification; Phase-field method ID PRIMARY SPACING SELECTION; NICKEL-BASE SUPERALLOY; DIRECTIONAL-SOLIDIFICATION; ALLOY SOLIDIFICATION; POLYCRYSTALLINE SOLIDIFICATION; INITIAL INSTABILITY; SYMMETRICAL MODEL; PATTERN-FORMATION; EVOLUTION; NOISE AB We report the results of an extensive phase-field study of the growth competition of columnar dendritic grains in two dimensions. We investigate the influence of the temperature gradient and grain bicrystallography on the selection of both grain and microstructure, focusing on a geometry with two grains with principal crystal axes oriented parallel and at a finite misorientation angle with respect to the axis of the temperature gradient. Our first main finding is that, for well-developed dendritic structures forming at a low-temperature gradient, the rate of elimination of the misoriented grain is a non-monotonic function of the difference in undercooling between the dendrite tips of the two grains. Hence this rate cannot be predicted even qualitatively by the common assumption that the elimination rate increases with this undercooling difference. The breakdown of this assumption is particularly striking for highly misoriented dendritic and degenerate structures that persist for very long times despite growing at a substantially larger undercooling than the well-oriented neighboring grains. Our second main finding is that microscopic thermal fluctuations at the origin of sidebranching can induce significant variations in the macroscopic trajectories of grain boundaries (GBs), thereby making grain selection a stochastic process, while yielding limited variations in the selected primary spacings. In contrast, in the absence of fluctuations, GB motion becomes essentially deterministic and grain elimination is suppressed. In addition, our simulations reproduce quantitatively scaling laws deduced from experiments for both the primary dendritic spacing and the dendrite growth direction of misoriented grains. They further reveal that the "intergrain" primary spacing selected by tertiary branching events at GBs is systematically larger than the "intragrain" primary spacing selected by the transient growth competition between primary branches within a single grain, while obeying the same scaling laws. Finally, the fact that the rate of grain elimination is slower in our 2-D simulations than in experiments suggests that the 3-D grain bicrystallography plays a key role in grain selection. This role is interpreted in the light of 2-D simulations that hinder sidebranching on the misoriented grain. (C) 2014 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved. C1 Northeastern Univ, Dept Phys, Boston, MA 02115 USA. Northeastern Univ, Ctr Interdisciplinary Res Complex Syst, Boston, MA 02115 USA. RP Tourret, D (reprint author), Los Alamos Natl Lab, Div Mat Sci & Technol, Los Alamos, NM 87545 USA. EM dtourret@lanl.gov; a.karma@neu.edu RI Tourret, Damien/B-2854-2017 OI Tourret, Damien/0000-0003-4574-7004 FU NASA in the framework of the CETSOL project [NNX11AC09G] FX This research was supported by NASA under award No. NNX11AC09G in the framework of the CETSOL project. The authors are thankful to W. Kurz and Ch.-A. Gandin for stimulating discussions and for providing videos of experiments [10,14], to X. Gong and D. Kaeli of the Northeastern University Computer Architecture Research Laboratory for their help in improving the GPU implementation of our phase-field model, as well as to J.-M. Debierre, J. Ghmadh and R. Guerin for helpful discussions. NR 88 TC 21 Z9 21 U1 7 U2 89 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 1359-6454 EI 1873-2453 J9 ACTA MATER JI Acta Mater. PD JAN 1 PY 2015 VL 82 BP 64 EP 83 DI 10.1016/j.actamat.2014.08.049 PG 20 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Materials Science; Metallurgy & Metallurgical Engineering GA AX6FE UT WOS:000347017800007 ER PT J AU Mason, JK Lind, J Li, SF Reed, BW Kumar, M AF Mason, J. K. Lind, J. Li, S. F. Reed, B. W. Kumar, M. TI Kinetics and anisotropy of the Monte Carlo model of grain growth SO ACTA MATERIALIA LA English DT Article DE Grain growth; Monte Carlo method; MC simulations; Computer simulation ID COMPUTER-SIMULATION; POTTS-MODEL; BOUNDARY ENERGIES; SIZE DISTRIBUTION; ALGORITHM; LATTICE; TEMPERATURE; STATISTICS AB The Monte Carlo model is one of the most frequently used approaches to simulate grain growth, and retains a number of features that derive from the closely related Ising and Potts models. The suitability of these features for the simulation of grain growth is examined, and several modifications to the Hamiltonian and transition probability function are proposed. The resulting model is shown to not only reproduce the usual behaviors of grain growth simulations, but to substantially reduce the effect of the underlying pixel lattice on the microstructure as compared to contemporary simulations. (C) 2014 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved. C1 [Mason, J. K.; Lind, J.; Li, S. F.; Reed, B. W.; Kumar, M.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. [Mason, J. K.] Bogazici Univ, TR-34342 Istanbul, Turkey. RP Lind, J (reprint author), Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. EM jeremy.mason@boun.edu.tr; lind9@llnl.gov; li31@llnl.gov; reed12@llnl.gov; kumar3@llnl.gov RI Mason, Jeremy/P-9567-2015; Mason, Jeremy/P-8188-2014 OI Mason, Jeremy/0000-0002-0425-9816; Mason, Jeremy/0000-0002-0425-9816 FU US Department of Energy by Lawrence Livermore National Laboratory [DE-AC52-07NA27344]; US DOE Office of Basic Energy Sciences, Division of Materials Science and Engineering; Lawrence Postdoctoral Fellowship FX This work was performed under the auspices of the US Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344, and the authors were supported by US DOE Office of Basic Energy Sciences, Division of Materials Science and Engineering. Additional support for J.K.M. in the form of a Lawrence Postdoctoral Fellowship is also acknowledged. NR 31 TC 3 Z9 3 U1 0 U2 16 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 1359-6454 EI 1873-2453 J9 ACTA MATER JI Acta Mater. PD JAN 1 PY 2015 VL 82 BP 155 EP 166 DI 10.1016/j.actamat.2014.08.063 PG 12 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Materials Science; Metallurgy & Metallurgical Engineering GA AX6FE UT WOS:000347017800015 ER PT J AU Yang, L Gao, F Kurtz, RJ Zu, XT AF Yang, L. Gao, F. Kurtz, R. J. Zu, X. T. TI Atomistic simulations of helium clustering and grain boundary reconstruction in alpha-iron SO ACTA MATERIALIA LA English DT Article DE Grain boundary; Atomistic simulation; Nucleation of He clusters; bcc Fe ID DISLOCATION LOOPS; HE INTERSTITIALS; FERRITIC ALLOY; BCC IRON; FE; BUBBLES; NUCLEATION; DIFFUSION; TRANSPORT; GROWTH AB The accumulation and clustering of He atoms at Sigma 3 < 110 >{112) and Sigma 73b < 110 > {661} grain boundaries (GBs) in body-centred cubic Fe, as well as their effects on GB reconstruction, have been investigated using atomic-level computer simulations. The accumulation of He atoms and the evolution of the GB structure all depend on local He concentration, temperature and the original GB structure. At a local He concentration of 1%, small He clusters are formed in the Sigma 3 GB, accompanied by the emission of single self-interstitial Fe atoms (SIAs). At a He concentration of 5%, a large number of SIAs are emitted from He clusters in the Sigma 3 GB and collect at the periphery of these clusters. The SIAs eventually form < 100 > dislocation loops between two He clusters. It is likely that impurities may promote the formation of < 100 > loops and enhance their stabilities in alpha-Fe. At a He concentration of 10%, the large number of emitted SIAs are able to rearrange themselves, forming a new GB plane within the Sigma 3 GB, which results in self-healing of the GB and leads to GB migration. In contrast to the Sigma 3 GB, He clusters are mainly formed along the GB dislocation lines in the Sigma 73b, and the emitted SIAs accumulate at the cores of the GB dislocations, leading to the climb of the dislocations within the GB plane. As compared to bulk Fe, a higher number density of clusters form at GBs, but the average cluster size is smaller. The product of cluster density and average cluster size is roughly constant at a given He level, and is about the same in bulk and GB regions, and varies linearly with the He concentration. (C) 2014 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved. C1 [Yang, L.; Gao, F.; Kurtz, R. J.] Pacific NW Natl Lab, Richland, WA 99352 USA. [Yang, L.; Zu, X. T.] Univ Elect Sci & Technol China, Sch Phys Elect, Chengdu 610054, Peoples R China. [Gao, F.] Univ Michigan, Dept Nucl Engn & Radiol Sci, Ann Arbor, MI 48109 USA. RP Yang, L (reprint author), Pacific NW Natl Lab, MS K8-93,POB 999, Richland, WA 99352 USA. EM yanglildk@uestc.edu.cn; gaofeium@umich.edu FU US Department of Energy, Office of Science, Office of Fusion Energy Science [DE-AC06-76RLO 1830]; National Natural Science Foundation of China-NSAF [10976007] FX F.G. and R.J.K. are grateful for support by the US Department of Energy, Office of Science, Office of Fusion Energy Science under Contract DE-AC06-76RLO 1830. L.Y. and X.T.Z. are grateful for the support by the National Natural Science Foundation of China-NSAF (Grant No. 10976007). The authors acknowledge Dr. W. Setyawan for insightful discussions. NR 33 TC 12 Z9 13 U1 8 U2 46 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 1359-6454 EI 1873-2453 J9 ACTA MATER JI Acta Mater. PD JAN 1 PY 2015 VL 82 BP 275 EP 286 DI 10.1016/j.actamat.2014.09.015 PG 12 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Materials Science; Metallurgy & Metallurgical Engineering GA AX6FE UT WOS:000347017800026 ER PT J AU Zong, HX Ding, XD Lookman, T Li, J Sun, J AF Zong, Hongxiang Ding, Xiangdong Lookman, Turab Li, Ju Sun, Jun TI Uniaxial stress-driven coupled grain boundary motion in hexagonal close-packed metals: A molecular dynamics study SO ACTA MATERIALIA LA English DT Article DE Grain boundary motion; Interface dislocations; Deformation twinning; Molecular dynamics; Titanium ID NANOCRYSTALLINE METALS; ATOMISTIC SIMULATION; PLASTIC-DEFORMATION; MIGRATION; SHEAR; MECHANISM; MOBILITY; MG AB Stress-driven grain boundary (GB) migration has been evident as a dominant mechanism accounting for plastic deformation in crystalline solids. Using molecular dynamics (MD) simulations on a Ti bicrystal model, we show that a uniaxial stress-driven coupling is associated with the recently observed 90 GB reorientation in shock simulations and nanopillar compression measurements. This is not consistent with the theory of shear-induced coupled GB migration. In situ atomic configuration analysis reveals that this GB motion is accompanied by the glide of two sets of parallel dislocation arrays, and the uniaxial stress-driven coupling is explained through a composite action of symmetrically distributed dislocations and deformation twins. In addition, the coupling factor is calculated from MD simulations over a wide range of temperatures. We find that the coupled motion can be thermally damped (i.e., not thermally activated), probably due to the absence of the collective action of interface dislocations. This uniaxial coupled mechanism is believed to apply to other hexagonal close-packed metals. (C) 2014 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved. C1 [Zong, Hongxiang; Lookman, Turab] Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. [Zong, Hongxiang; Ding, Xiangdong; Li, Ju; Sun, Jun] Xi An Jiao Tong Univ, State Key Lab Mech Behav Mat, Xian 710049, Peoples R China. [Li, Ju] MIT, Dept Nucl Sci & Engn, Cambridge, MA 02139 USA. [Li, Ju] MIT, Dept Mat Sci & Engn, Cambridge, MA 02139 USA. RP Ding, XD (reprint author), Xi An Jiao Tong Univ, State Key Lab Mech Behav Mat, Xian 710049, Peoples R China. EM dinxd@mail.xjtu.edu.cn; txl@lanl.gov RI Li, Ju/A-2993-2008; Ding, Xiangdong/K-4971-2013 OI Li, Ju/0000-0002-7841-8058; Ding, Xiangdong/0000-0002-1220-3097 FU US Department of Energy (DOE) at Los Alamos National Laboratory (ASC/PEM); National Basic Research program of China [2010CB631003, 2012CB619402, 2012CB619401]; Program of Introducing Talents of Discipline to Universities in China project [B06025] FX This work was supported by the US Department of Energy (DOE) at Los Alamos National Laboratory (ASC/PEM). We are also grateful to the Natural Science Foundation of China (51171140, 51231008, 51320105014 and 51321003), the National Basic Research program of China (2010CB631003, 2012CB619402, 2012CB619401) and the Program of Introducing Talents of Discipline to Universities in China project (B06025). NR 39 TC 11 Z9 13 U1 9 U2 69 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 1359-6454 EI 1873-2453 J9 ACTA MATER JI Acta Mater. PD JAN 1 PY 2015 VL 82 BP 295 EP 303 DI 10.1016/j.actamat.2014.09.010 PG 9 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Materials Science; Metallurgy & Metallurgical Engineering GA AX6FE UT WOS:000347017800028 ER PT J AU Qian, Y Yasunari, TJ Doherty, SJ Flanner, MG Lau, WKM Ming, J Wang, HL Wang, M Warren, SG Zhang, RD AF Qian, Yun Yasunari, Teppei J. Doherty, Sarah J. Flanner, Mark G. Lau, William K. M. Ming Jing Wang, Hailong Wang, Mo Warren, Stephen G. Zhang, Rudong TI Light-absorbing Particles in Snow and Ice: Measurement and Modeling of Climatic and Hydrological impact SO ADVANCES IN ATMOSPHERIC SCIENCES LA English DT Review DE light-absorbing; aerosol; snow; ice; albedo; measurement; climate; modeling; hydrological cycle ID BLACK CARBON DEPOSITION; INTERCOMPARISON PROJECT ACCMIP; BIOMASS BURNING EMISSIONS; THERMAL-OPTICAL ANALYSIS; ASIAN SUMMER MONSOON; SIERRA-NEVADA SNOW; EARTH SYSTEM MODEL; TIBETAN PLATEAU; ELEMENTAL CARBON; ARCTIC SNOW AB Light absorbing particles (LAP, e.g., black carbon, brown carbon, and dust) influence water and energy budgets of the atmosphere and snowpack in multiple ways. In addition to their effects associated with atmospheric heating by absorption of solar radiation and interactions with clouds, LAP in snow on land and ice can reduce the surface reflectance (a.k.a., surface darkening), which is likely to accelerate the snow aging process and further reduces snow albedo and increases the speed of snowpack melt. LAP in snow and ice (LAPSI) has been identified as one of major forcings affecting climate change, e.g. in the fourth and fifth assessment reports of IPCC. However, the uncertainty level in quantifying this effect remains very high. In this review paper, we document various technical methods of measuring LAPSI and review the progress made in measuring the LAPSI in Arctic, Tibetan Plateau and other mid-latitude regions. We also report the progress in modeling the mass concentrations, albedo reduction, radiative forcing, and climatic and hydrological impact of LAPSI at global and regional scales. Finally we identify some research needs for reducing the uncertainties in the impact of LAPSI on global and regional climate and the hydrological cycle. C1 [Qian, Yun; Wang, Hailong; Wang, Mo; Zhang, Rudong] Pacific NW Natl Lab, Atmospher Sci & Global Change Div, Richland, WA 99352 USA. [Yasunari, Teppei J.] Univ Space Res Assoc, Goddard Earth Sci Technol & Res, Columbia, MD 21046 USA. [Yasunari, Teppei J.] NASA, Goddard Space Flight Ctr, Greenbelt, MD 20771 USA. [Doherty, Sarah J.; Warren, Stephen G.] Univ Washington, Dept Atmospher Sci, Seattle, WA 98195 USA. [Flanner, Mark G.] Univ Michigan, Dept Atmospher Sci, Ann Arbor, MI 48109 USA. [Lau, William K. M.] Univ Maryland, Earth Syst Sci Interdisciplinary Ctr, College Pk, MD 20740 USA. [Lau, William K. M.; Ming Jing] NASA, Earth Sci Div, Goddard Space Flight Ctr, Greenbelt, MD 20771 USA. China Meteorol Adm, Natl Climate Ctr, Beijing 100081, Peoples R China. [Wang, Mo] Chinese Acad Sci, Inst Tibetan Plateau Res, Key Lab Tibetan Environm Changes & Land Surface P, Beijing 100101, Peoples R China. [Zhang, Rudong] Lanzhou Univ, Coll Atmospher Sci, Lanzhou 730000, Peoples R China. RP Qian, Y (reprint author), Pacific NW Natl Lab, Atmospher Sci & Global Change Div, Richland, WA 99352 USA. EM yun.qian@pnnl.gov RI qian, yun/E-1845-2011; Flanner, Mark/C-6139-2011; Doherty, Sarah/D-5592-2015; Yasunari, Teppei/E-5374-2010; Wang, Hailong/B-8061-2010; Lau, William /E-1510-2012; OI Flanner, Mark/0000-0003-4012-174X; Doherty, Sarah/0000-0002-7796-6968; Yasunari, Teppei/0000-0002-9896-9404; Wang, Hailong/0000-0002-1994-4402; Lau, William /0000-0002-3587-3691; Ming, Jing/0000-0001-5527-3768 FU U.S. Department of Energy, Office of Science, Biological and Environmental Research, Earth System Modeling Program; NSF [1253154]; China Scholarship Fund; DOE [DE-AC06-76RLO1830]; NASA Modeling, Analysis, and Prediction (MAP) Program by the Science Mission Directorate at NASA Headquarters FX This study was supported by the U.S. Department of Energy, Office of Science, Biological and Environmental Research, as part of the Earth System Modeling Program. The NASA Modeling, Analysis, and Prediction (MAP) Program by the Science Mission Directorate at NASA Headquarters supported the work contributed by Teppei J. YASUNARI and William K. M. LAU. The NASA GEOS-5 simulation was implemented in the system for NASA Center for Climate Simulation (NCCS). M. G. Flanner was partially supported by NSF 1253154. R. ZHANG acknowledges support from the China Scholarship Fund. The Pacific Northwest National Laboratory is operated for DOE by Battelle Memorial Institute under contract DE-AC06-76RLO1830. NR 226 TC 25 Z9 26 U1 13 U2 76 PU SCIENCE PRESS PI BEIJING PA 16 DONGHUANGCHENGGEN NORTH ST, BEIJING 100717, PEOPLES R CHINA SN 0256-1530 EI 1861-9533 J9 ADV ATMOS SCI JI Adv. Atmos. Sci. PD JAN PY 2015 VL 32 IS 1 BP 64 EP 91 DI 10.1007/s00376-014-0010-0 PG 28 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA AY0JJ UT WOS:000347282700005 ER PT J AU Mahieu, B Gauthier, D Perdrix, M Ge, XY Boutu, W Lepetit, F Wang, F Carre, B Auguste, T Merdji, H Garzella, D Gobert, O AF Mahieu, Benoit Gauthier, David Perdrix, Michel Ge, Xunyou Boutu, Willem Lepetit, Fabien Wang, Fan Carre, Bertrand Auguste, Thierry Merdji, Hamed Garzella, David Gobert, Olivier TI Spatial quality improvement of a Ti:Sapphire laser beam by modal filtering SO APPLIED PHYSICS B-LASERS AND OPTICS LA English DT Article ID ORDER HARMONIC-GENERATION; OPTICAL PULSES; INTERFEROMETRY; OPTIMIZATION; COMPRESSION; FIELD AB We present a study on the improvement of the spatial quality of a laser beam, called modal filtering, suitable to high-energy lasers. The method is theoretically compared with the classical pinhole filtering technique in the case of an astigmatic Gaussian beam, illustrating, in this particular case, its efficiency for filtering low spatial frequencies. Experimental study of the modal filtering of a temporally chirped beam from a Ti:Sapphire chirped-pulse-amplification system is presented. Beam profile, wavefront and pulse duration after compression were measured, showing a dramatic improvement of beam quality and no modifications of the temporal distribution. High-order harmonic generation in a rare gas, a highly nonlinear process which is phase-matching dependent, was used to test the effect of the filter and showed a clear enhancement of the generation. C1 [Mahieu, Benoit; Gauthier, David; Perdrix, Michel; Ge, Xunyou; Boutu, Willem; Lepetit, Fabien; Wang, Fan; Carre, Bertrand; Auguste, Thierry; Merdji, Hamed; Garzella, David; Gobert, Olivier] CEA, Serv Photons Atomes & Mol, Ctr Etud Saclay, F-91191 Gif Sur Yvette, France. [Mahieu, Benoit] Sincrotrone Trieste Elettra, I-34149 Basovizza, Italy. [Mahieu, Benoit] Univ Nova Gorica, Lab Quantum Opt, Ajdovscina 5270, Slovenia. [Merdji, Hamed] SLAC, Stanford PULSE Ctr, Menlo Pk, CA 94025 USA. RP Mahieu, B (reprint author), CEA, Serv Photons Atomes & Mol, Ctr Etud Saclay, Batiment 522, F-91191 Gif Sur Yvette, France. EM benoit.mahieu@ensta-paristech.fr FU Egide agency; Triangle de la Physique network; COST European network FX This work has been sustained by ANR I-NanoX project and FEMTO-X-MAG. We thank Giovanni De Ninno and Romain Bachelard for constructive discussions and are also grateful to the Egide agency, the Triangle de la Physique network and the COST European network for their financial support in the framework of, respectively, the XUV-FISCH project, the XUV-PhLAGH project and the MP1203 action. NR 39 TC 0 Z9 0 U1 1 U2 23 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 0946-2171 EI 1432-0649 J9 APPL PHYS B-LASERS O JI Appl. Phys. B-Lasers Opt. PD JAN PY 2015 VL 118 IS 1 BP 47 EP 60 DI 10.1007/s00340-014-5953-4 PG 14 WC Optics; Physics, Applied SC Optics; Physics GA AX9UO UT WOS:000347247700007 ER PT J AU Kessel, CE Tillack, MS Najmabadi, F Poli, FM Ghantous, K Gorelenkov, N Wang, XR Navaei, D Toudeshki, HH Koehly, C El-Guebaly, L Blanchard, JP Martin, CJ Mynsburge, L Humrickhouse, P Rensink, ME Rognlien, TD Yoda, M Abdel-Khalik, SI Hageman, MD Mills, BH Rader, JD Sadowski, DL Snyder, PB St John, H Turnbull, AD Waganer, LM Malang, S Rowcliffe, AF AF Kessel, C. E. Tillack, M. S. Najmabadi, F. Poli, F. M. Ghantous, K. Gorelenkov, N. Wang, X. R. Navaei, D. Toudeshki, H. H. Koehly, C. El-Guebaly, L. Blanchard, J. P. Martin, C. J. Mynsburge, L. Humrickhouse, P. Rensink, M. E. Rognlien, T. D. Yoda, M. Abdel-Khalik, S. I. Hageman, M. D. Mills, B. H. Rader, J. D. Sadowski, D. L. Snyder, P. B. St. John, H. Turnbull, A. D. Waganer, L. M. Malang, S. Rowcliffe, A. F. TI THE ARIES ADVANCED AND CONSERVATIVE TOKAMAK POWER PLANT STUDY SO FUSION SCIENCE AND TECHNOLOGY LA English DT Article DE ARIES-ACT power plant; engineering and physics design; neutronics ID GREENWALD DENSITY LIMIT; DIVERTOR TARGET PLATE; H-MODE PLASMAS; HIGH-PERFORMANCE; VACUUM VESSEL; RECENT PROGRESS; CURRENT DRIVE; DESIGN; JET; DISCHARGES AB Tokamak power plants are studied with advanced and conservative design philosophies to identify the impacts on the resulting designs and to provide guidance to critical research needs. Incorporating updated physics understanding and using more sophisticated engineering and physics analysis, the tokamak configurations have developed a more credible basis compared with older studies. The advanced configuration assumes a self-cooled lead lithium blanket concept with SiC composite structural material with 58% thermal conversion efficiency. This plasma has a major radius of 6.25 m, a toroidal field of 6.0 T, a q(95) of 4.5, a beta(total)(N) of 5.75, an H-98 of 1.65, an n/n(Gr). of 1.0, and a peak divertor heat flux of 13.7 MW/m(2). The conservative configuration assumes a dual-coolant lead lithium blanket concept with reduced-activation ferritic martensitic steel structural material and helium coolant, achieving a thermal conversion efficiency of 45%. The plasma has a major radius of 9.75 m, a toroidal field of 8.75 T, a q(95) of 8.0, a beta(total)(N) of 2.5, an H-98 of 1.25, an n/n(Gr) of 1.3, and a peak divertor heat flux of 10 MW/m(2). The divertor heat flux treatment with a narrow power scrape-off width has driven the plasmas to larger major radius. Edge and divertor plasma simulations are targeting a basis for high radiated power fraction in the divertor, which is necessary for solutions to keep the peak heat flux in the range 10 to 15 MW/m(2). Combinations of the advanced and conservative approaches show intermediate sizes. A new systems code using a database approach has been used and shows that the operating point is really an operating zone with some range of plasma and engineering parameters and very similar costs of electricity. Other papers in this issue provide more detailed discussion of the work summarized here. C1 [Kessel, C. E.; Poli, F. M.; Ghantous, K.; Gorelenkov, N.] Princeton Plasma Phys Lab, Princeton, NJ 08543 USA. [Tillack, M. S.; Najmabadi, F.; Wang, X. R.; Navaei, D.; Toudeshki, H. H.] Univ Calif San Diego, San Diego, CA 92103 USA. [Koehly, C.] Karlsruhe Inst Technol, D-76021 Karlsruhe, Germany. [El-Guebaly, L.; Blanchard, J. P.; Martin, C. J.; Mynsburge, L.] Univ Wisconsin, Madison, WI USA. [Humrickhouse, P.] Idaho Natl Lab, Idaho Falls, ID 83415 USA. [Rensink, M. E.; Rognlien, T. D.] Lawrence Livermore Natl Lab, Livermore, CA USA. [Yoda, M.; Abdel-Khalik, S. I.; Hageman, M. D.; Mills, B. H.; Rader, J. D.; Sadowski, D. L.] Georgia Inst Technol, Atlanta, GA 30332 USA. [Snyder, P. B.; St. John, H.; Turnbull, A. D.] Gen Atom Co, La Jolla, CA USA. [Malang, S.] Fus Nucl Technol Consulting, D-76351 Linkenheim Hochstetten, Germany. [Rowcliffe, A. F.] Oak Ridge Natl Lab, Oak Ridge, TN USA. RP Kessel, CE (reprint author), Princeton Plasma Phys Lab, POB 451, Princeton, NJ 08543 USA. EM ckessel@pppl.gov FU U.S. Department of Energy [DE-AC02-76CH03073, DE-AC52-07NA27344, DE-FC02-04ER54698] FX This work is partially supported by the U.S. Department of Energy contracts DE-AC02-76CH03073, DE-AC52-07NA27344, and DE-FC02-04ER54698. NR 83 TC 12 Z9 12 U1 3 U2 26 PU AMER NUCLEAR SOC PI LA GRANGE PK PA 555 N KENSINGTON AVE, LA GRANGE PK, IL 60526 USA SN 1536-1055 EI 1943-7641 J9 FUSION SCI TECHNOL JI Fusion Sci. Technol. PD JAN PY 2015 VL 67 IS 1 SI SI BP 1 EP 21 PG 21 WC Nuclear Science & Technology SC Nuclear Science & Technology GA AX5CK UT WOS:000346944500001 ER PT J AU Tillack, MS Wang, XR Navaei, D Toudeshki, HH Rowcliffe, AF Najmabadi, F AF Tillack, M. S. Wang, X. R. Navaei, D. Toudeshki, H. H. Rowcliffe, A. F. Najmabadi, F. CA ARIES TEAM TI DESIGN AND ANALYSIS OF THE ARIES-ACT1 FUSION POWER CORE SO FUSION SCIENCE AND TECHNOLOGY LA English DT Article DE ARIES-ACT power plant; blanket; divertor ID HIGH-PERFORMANCE DIVERTOR; ELASTIC-PLASTIC ANALYSIS; ELECTRICAL-CONDUCTIVITY; STRUCTURAL-MATERIALS; TRANSITION JOINT; COOLED DIVERTORS; RECENT PROGRESS; VACUUM VESSEL; TARGET PLATE; PLANT AB ARIES-ACT1 is the latest in a series of tokamak power plant designs that capitalize on the high-temperature capabilities and attractive safety and environmental characteristics of SiC composites coupled with a self-cooled lead-lithium breeder. This combination offers both design simplicity and high performance, capable of operating at very high coolant outlet temperature in a moderately high-power-density device. Blankets are supported within a poloidally continuous He-cooled steel structural ring, which adds robustness and minimizes loads on the SiC modules. In order to withstand high local surface heat flux in the divertor (of the order of 14 MW/m(2) time averaged), a helium-cooled tungsten-alloy divertor was adopted. About 25% of the total "high-grade" heat is thus removed by helium, to be combined with the blanket heat in order to feed the power cycle. In addition to the in-vessel power-producing elements of the design, this paper also summarizes the key features and analysis of the vacuum vessel and power conversion system. C1 [Tillack, M. S.; Wang, X. R.; Navaei, D.; Toudeshki, H. H.; Najmabadi, F.] Univ Calif San Diego, La Jolla, CA 92093 USA. [Rowcliffe, A. F.] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. RP Tillack, MS (reprint author), Univ Calif San Diego, 9500 Gilman Dr, La Jolla, CA 92093 USA. EM mtillack@ucsd.edu FU U.S. Department of Energy [DE-FG02-04ER54757] FX Financial support was provided by the U.S. Department of Energy under contract DE-FG02-04ER54757. NR 73 TC 6 Z9 6 U1 2 U2 7 PU AMER NUCLEAR SOC PI LA GRANGE PK PA 555 N KENSINGTON AVE, LA GRANGE PK, IL 60526 USA SN 1536-1055 EI 1943-7641 J9 FUSION SCI TECHNOL JI Fusion Sci. Technol. PD JAN PY 2015 VL 67 IS 1 SI SI BP 49 EP 74 PG 26 WC Nuclear Science & Technology SC Nuclear Science & Technology GA AX5CK UT WOS:000346944500003 ER PT J AU Kessel, CE Poli, FM Ghantous, K Gorelenkov, NN Rensink, ME Rognlien, TD Snyder, PB St John, H Turnbull, AD AF Kessel, C. E. Poli, F. M. Ghantous, K. Gorelenkov, N. N. Rensink, M. E. Rognlien, T. D. Snyder, P. B. St. John, H. Turnbull, A. D. TI PHYSICS BASIS FOR AN ADVANCED PHYSICS AND ADVANCED TECHNOLOGY TOKAMAK POWER PLANT CONFIGURATION: ARIES-ACT1 SO FUSION SCIENCE AND TECHNOLOGY LA English DT Article DE ARIES-ACT power plant; plasma physics; tokamak ID EDGE LOCALIZED MODES; ALCATOR C-MOD; PLASMA-FACING COMPONENTS; GREENWALD DENSITY LIMIT; RESISTIVE WALL MODES; HIGH-FIELD SIDE; DIII-D TOKAMAK; ELMY H-MODE; MAGNETOHYDRODYNAMIC STABILITY; HIGH-PERFORMANCE AB The advanced physics and advanced technology tokamak power plant ARIES-ACT1 has a major radius of 6.25 m at an aspect ratio of 4.0, toroidal field of 6.0 T, strong shaping with elongation of 2.2, and triangularity of 0.63. The broadest pressure cases reached wall-stabilized beta(N) similar to 5.75, limited by n = 3 external kink mode requiring a conducting shell at b/a = 0 3, requiring plasma rotation, feedback, and/or kinetic stabilization. The medium pressure peaking case reaches) beta(N) = 5.28 with B-T = 6.75, while the peaked pressure case reaches beta(N) < 5.15. Fast particle magnetohydrodynamic stability shows that the alpha particles are unstable, but this leads to redistribution to larger minor radius rather than loss from the plasma. Edge and divertor plasma modeling shows that 75% of the power to the divertor can be radiated with an ITER-like divertor geometry, while >95% can be radiated in a stable detached mode with an orthogonal target and wide slot geometry. The bootstrap current fraction is 91% with a q(95) of 4.5, requiring similar to 1.1 MA of external current drive. This current is supplied with 5 MW of ion cyclotron radio frequency/fast wave and 40 MW of lower hybrid current drive. Electron cyclotron is most effective for safety factor control over rho similar to 0.2 to 0.6 with 20 MW. The pedestal density is similar to 0.9 X 10(20)/m(3), and the temperature is similar to 4.4 keV. The H-98 factor is 1.65, n/n(Gr) = 1.0, and the ratio of net power to threshold power is 2.8 to 3.0 in the flattop. C1 [Kessel, C. E.; Poli, F. M.; Ghantous, K.; Gorelenkov, N. N.] Princeton Plasma Phys Lab, Princeton, NJ 08543 USA. [Rensink, M. E.; Rognlien, T. D.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. [Snyder, P. B.; St. John, H.; Turnbull, A. D.] Gen Atom Co, San Diego, CA 92121 USA. RP Kessel, CE (reprint author), Princeton Plasma Phys Lab, POB 451, Princeton, NJ 08543 USA. EM ckessel@pppl.gov FU U.S. Department of Energy [DE-AC02-76CH03073, DE-AC52-07NA27344, DE-FC02-04ER54698] FX The work was supported by the U.S. Department of Energy contracts DE-AC02-76CH03073, DE-AC52-07NA27344, and DE-FC02-04ER54698. NR 149 TC 6 Z9 6 U1 0 U2 8 PU AMER NUCLEAR SOC PI LA GRANGE PK PA 555 N KENSINGTON AVE, LA GRANGE PK, IL 60526 USA SN 1536-1055 EI 1943-7641 J9 FUSION SCI TECHNOL JI Fusion Sci. Technol. PD JAN PY 2015 VL 67 IS 1 SI SI BP 75 EP 106 PG 32 WC Nuclear Science & Technology SC Nuclear Science & Technology GA AX5CK UT WOS:000346944500004 ER PT J AU Rensink, ME Rognlien, TD AF Rensink, M. E. Rognlien, T. D. TI PLASMA HEAT-FLUX DISPERSAL FOR ACT1 DIVERTOR CONFIGURATIONS SO FUSION SCIENCE AND TECHNOLOGY LA English DT Article DE ARIES-ACT power plant; UEDGE modeling; edge plasma ID ITER; DETACHMENT; TRANSPORT; POWER; DESIGN; MODEL AB Simulations of the heat flux on plasma-facing components from core exhaust plasma are reported for two possible ACT1 divertor configurations. One configuration uses divertor plates strongly inclined with respect to the poloidal magnetic flux surfaces similar to that planned for ITER and results in a partially detached divertor plasma. The second configuration has divertor plates orthogonal to the flux surfaces, which leads to a fully detached divertor plasma if the width of the divertor region is sufficient. Both configurations use scrape-off layer radiation from seeded impurities to yield an acceptable peak heat flux of similar to 10 MW/m(2) or smaller on the divertor plates and chamber walls. The simulations are performed with the UEDGE two-dimensional transport code to model both plasma and neutral components with some supplementary neutral modeling performed with the DEGAS 2 Monte Carlo code. C1 [Rensink, M. E.; Rognlien, T. D.] Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. RP Rensink, ME (reprint author), Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. EM rognlienl@llnl.gov FU U.S. Department of Energy by Lawrence Livermore National Laboratory [DE-AC5207NA27344] FX The authors would like to acknowledge helpful discussions with D. Stotler regarding neutral particle modeling with the DEGAS 2 code. This work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under contract DE-AC5207NA27344. This material is based upon work supported by the U.S. Department of Energy, Office of Science, Office of Fusion Energy Sciences. NR 28 TC 3 Z9 3 U1 0 U2 5 PU AMER NUCLEAR SOC PI LA GRANGE PK PA 555 N KENSINGTON AVE, LA GRANGE PK, IL 60526 USA SN 1536-1055 EI 1943-7641 J9 FUSION SCI TECHNOL JI Fusion Sci. Technol. PD JAN PY 2015 VL 67 IS 1 SI SI BP 125 EP 141 PG 17 WC Nuclear Science & Technology SC Nuclear Science & Technology GA AX5CK UT WOS:000346944500006 ER PT J AU Humrickhouse, PW Merrill, BJ AF Humrickhouse, Paul W. Merrill, Brad J. TI ARIES-ACT1 SAFETY DESIGN AND ANALYSIS SO FUSION SCIENCE AND TECHNOLOGY LA English DT Article DE ARIES-ACT power plant; MELCOR; fusion safety AB ARIES-ACT1 (Advanced and Conservative Tokamak) is a 1000-MW(electric) tokamak design featuring advanced plasma physics and divertor and blanket engineering. Some relevant features include an advanced SiC blanket with PbLi as coolant and breeder; a helium-cooled steel structural ring and tungsten divertors; a thin-walled, helium-cooled vacuum vessel; and a room-temperature, water-cooled shield outside the vacuum vessel. We consider here some safety aspects of the ARIES-ACT1 design and model a series of design-basis and beyond-design-basis accidents with the MELCOR code modified for fusion. The presence of multiple coolants (PbLi, helium, and water) makes possible a variety of such accidents. We consider here a loss-of-flow accident caused by a long-term station blackout (LTSBO), an ex-vessel helium break into the cryostat, and a beyond-design-basis accident in which a LTSBO is aggravated by a loss-of-coolant accident in ARIES-ACT1's ultimate decay heat removal system, the water-cooled shield. In the design-basis accidents, we find that the secondary confinement boundaries are not challenged, and the structural integrity of in-vessel components is not threatened by high temperatures or pressures; decay heat can be passively removed. C1 [Humrickhouse, Paul W.; Merrill, Brad J.] Idaho Natl Lab, Idaho Falls, ID 83415 USA. RP Humrickhouse, PW (reprint author), Idaho Natl Lab, POB 1625,MS 3840, Idaho Falls, ID 83415 USA. EM paul.humrickhouse@inl.gov FU DOE, Office of Science, Office of Fusion Energy Sciences [DE-AC07-05ID14517] FX This material is based upon work supported by the DOE, Office of Science, Office of Fusion Energy Sciences, under contract DE-AC07-05ID14517. NR 16 TC 4 Z9 4 U1 0 U2 2 PU AMER NUCLEAR SOC PI LA GRANGE PK PA 555 N KENSINGTON AVE, LA GRANGE PK, IL 60526 USA SN 1536-1055 EI 1943-7641 J9 FUSION SCI TECHNOL JI Fusion Sci. Technol. PD JAN PY 2015 VL 67 IS 1 SI SI BP 167 EP 178 PG 12 WC Nuclear Science & Technology SC Nuclear Science & Technology GA AX5CK UT WOS:000346944500009 ER PT J AU Kessel, CE Poli, FM AF Kessel, C. E. Poli, F. M. TI PHYSICS BASIS FOR A CONSERVATIVE PHYSICS AND CONSERVATIVE TECHNOLOGY TOKAMAK POWER PLANT: ARIES-ACT2 SO FUSION SCIENCE AND TECHNOLOGY LA English DT Article DE ARIES-ACT power plant; heating and current drive; transport simulation ID LOWER-HYBRID WAVES; GREENWALD DENSITY LIMIT; RESISTIVE WALL MODES; ALCATOR C-MOD; HIGH-PERFORMANCE; CURRENT DRIVE; DISRUPTION MITIGATION; TRANSPORT BARRIERS; PLASMA ROTATION; ITER AB The conservative physics and conservative technology tokamak power plant ARIES-ACT2 has a major radius of 9.75 m at an aspect ratio of 4.0 and has strong shaping with elongation of 2.2 and triangularity of 0.63. The plasma current is 14 MA, and the toroidal field at the plasma major radius is 8.75 T, making the maximum field at the toroidal field coil 16 T. The no-wall beta(N) reaches similar to 2.4 limited by n = 1 external kink mode, and can be extended to 3.2 with a stabilizing shell behind the ring structure shield. The bootstrap current fraction is 77% with a q(95) of 8.0, requiring similar to 4.0 MA of external current drive. This current is supplied with 30 MW of ion cyclotron radio frequency/fast wave and 80 MW of negative ion neutral beams. Up to 1.0 MA can be driven with lower hybrid (LH) with no wall, and 1.5 or more MA can be driven with a stabilizing shell. Electron cyclotron was examined and is most effective for safety factor control over rho similar to 0.2 to 0.6 with 20 MW. The pedestal density is similar to 0.65 X 10(20)/m(3), and the temperature is similar to 9.0 keV. The H-98 factor is 1.25, n/n(Gr) = 1.3, and the net power to LH threshold power is 1.3 to 1.4 in the flattop. Because of the high toroidal field and high central temperature, the cyclotron radiation loss was found to be high depending on the first-wall reflectivity. C1 [Kessel, C. E.; Poli, F. M.] Princeton Plasma Phys Lab, Princeton, NJ 08543 USA. RP Kessel, CE (reprint author), Princeton Plasma Phys Lab, POB 451, Princeton, NJ 08543 USA. EM ckessel@pppl.gov FU U.S. Department of Energy [DE-AC02-76CH03073] FX We gratefully acknowledge the contribution by P. B. Snyder for the EPED1 analysis to establish the pedestal height. This work is supported by the U.S. Department of Energy contract DE-AC02-76CH03073. NR 76 TC 2 Z9 2 U1 0 U2 5 PU AMER NUCLEAR SOC PI LA GRANGE PK PA 555 N KENSINGTON AVE, LA GRANGE PK, IL 60526 USA SN 1536-1055 EI 1943-7641 J9 FUSION SCI TECHNOL JI Fusion Sci. Technol. PD JAN PY 2015 VL 67 IS 1 SI SI BP 220 EP 239 PG 20 WC Nuclear Science & Technology SC Nuclear Science & Technology GA AX5CK UT WOS:000346944500012 ER PT J AU Goldmann, A Brennecka, G Noordmann, J Weyer, S Wadhwa, M AF Goldmann, Alexander Brennecka, Gregory Noordmann, Janine Weyer, Stefan Wadhwa, Meenakshi TI The uranium isotopic composition of the Earth and the Solar System SO GEOCHIMICA ET COSMOCHIMICA ACTA LA English DT Article ID PLANETARY DIFFERENTIATION; PROTOPLANETARY DISK; CARBONACEOUS CHONDRITES; REFRACTORY INCLUSIONS; IRON-METEORITES; HEAVY-ELEMENTS; LIVE CM-247; PARENT-BODY; FRACTIONATION; HETEROGENEITY AB Recent high-precision mass spectrometric studies of the uranium isotopic composition of terrestrial and meteoritic materials have shown significant variation in the U-238/U-235 ratio, which was previously assumed to be invariant (=137.88). In this study, we have investigated 27 bulk meteorite samples from different meteorite groups and types, including carbonaceous (CM1 and CV3), enstatite (EH4) and ordinary (H-, L-, and LL-) chondrites, as well as a variety of achondrites (angrites, eucrites, and ungrouped) to constrain the distribution of U isotopic heterogeneities and to determine the average U-238/U-235 for the Solar System. The investigated bulk meteorites show a range in U-238/U-235 between 137.711 and 137.891 (1.3 parts per thousand) with the largest variations among ordinary chondrites (OCs). However, the U isotope compositions of 20 of the 27 meteorites analyzed here overlap within analytical uncertainties with the narrow range defined by terrestrial basalts (137.778-137.803), which are likely the best representatives for the U isotope composition of the bulk silicate Earth. Furthermore, the average U-238/U-235 of all investigated meteorite groups overlaps with that of terrestrial basalts (137.795 +/- 0.013). The bulk meteorite samples studied here do not show a negative correlation of U-238/U-235 with Nd/U or Th/U (used as proxies for the Cm/U ratio), as would be expected if radiogenic U-235 was generated by the decay of extant Cm-247 in the early Solar System. Rather, ordinary chondrites show a positive correlation of U-238/U-235 with Nd/U and with 1/U. The following conclusions can be drawn from this study: (1) The Solar System has a broadly homogeneous U isotope composition, and bulk samples of only a limited number of meteorites display detectable U isotope variations; (2) Bulk planetary differentiation has no significant effect on the U-238/U-235 ratio since the Earth, achondrites, and chondrites have indistinguishable U isotope compositions in average. (3) The cause of U isotopic variation in Solar System materials remains enigmatic; however, both the decay of Cm-247 and isotope fractionation are likely responsible for the U isotopic variations observed in CAIs and ordinary chondrites, respectively. The average U-238/U-235 of the investigated meteorite groups (including data compiled from the literature) and terrestrial basalts is 137.794 +/- 0.027 (at a 95% student's t confidence level, including all propagated uncertainties) and represents the best estimate for the Uisotope composition of the Earth and the Solar System. This value may be used for U-Pb and Pb-Pb dating of Solar System materials, provided the precise U isotope composition of the sample is unknown. Compared to Pb-Pb ages that were determined with the previously assumed value for U-238/U-235 (137.88), this new value results in an age adjustment of -0.9 Ma. (C) 2014 Elsevier Ltd. All rights reserved. C1 [Goldmann, Alexander; Weyer, Stefan] Leibniz Univ Hannover, Inst Mineral, D-30167 Hannover, Germany. [Brennecka, Gregory; Wadhwa, Meenakshi] Arizona State Univ, Sch Earth & Space Explorat, Tempe, AZ 85287 USA. [Brennecka, Gregory] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. [Noordmann, Janine] Phys Tech Bundesanstalt, D-38116 Braunschweig, Germany. RP Goldmann, A (reprint author), Leibniz Univ Hannover, Inst Mineral, Callinstr 3, D-30167 Hannover, Germany. FU Deutsche Forschungsgemeinschaft (DFG) [SPP 1385]; NASA [NNX11AK56G, NNX11AK75G] FX We want to thank Jutta Zipfel from the Senckenberg Museum in Frankfurt and Thorsten Kleine from the Westfalische Wilhelms-Universitat Munster for providing meteorite samples and the Goethe Universitat Frankfurt for the analyses of trace element concentrations. We also thank Steve Romaniello (Arizona State University) for assistance with the U isotope analysis of the Stannern homogenized powder. Fruitful discussions with Jutta Zipfel, Steven Galer and Frank Wombacher helped to interpret the findings of this study. The comments of Frederic Moynier, Herbert Palme and two anonymous reviewers significantly helped to improve the manuscript. Frederic Moynier is also thanked for editorial handling. This project was funded by program SPP 1385 of the Deutsche Forschungsgemeinschaft (DFG) and NASA grants NNX11AK56G and NNX11AK75G (M.W.). NR 59 TC 23 Z9 24 U1 0 U2 26 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0016-7037 EI 1872-9533 J9 GEOCHIM COSMOCHIM AC JI Geochim. Cosmochim. Acta PD JAN 1 PY 2015 VL 148 BP 145 EP 158 DI 10.1016/j.gca.2014.09.008 PG 14 WC Geochemistry & Geophysics SC Geochemistry & Geophysics GA AX1ZW UT WOS:000346743900010 ER PT J AU Boyet, M Carlson, RW Borg, LE Horan, M AF Boyet, Maud Carlson, Richard W. Borg, Lars E. Horan, Mary TI Sm-Nd systematics of lunar ferroan anorthositic suite rocks: Constraints on lunar crust formation SO GEOCHIMICA ET COSMOCHIMICA ACTA LA English DT Article ID SM-146 HALF-LIFE; MAGMA-OCEAN; EARLY DIFFERENTIATION; SOLAR-SYSTEM; MANTLE DIFFERENTIATION; METEORITES CONSTRAINTS; ISOTOPIC COMPOSITION; TERRESTRIAL PLANETS; IMPACT HISTORY; FORMATION AGE AB We have measured Sm-Nd systematics, including the short-lived Sm-146-Nd-142 chronometer, in lunar ferroan anorthositic suite (FAS) whole rocks (15415, 62236, 62255, 65315, 60025). At least some members of the suite are thought to be primary crystallization products formed by plagioclase flotation during crystallization of the lunar magma ocean (LMO). Most of these samples, except 62236, have not been exposed to galactic cosmic rays for a long period and thus require minimal correction to their Nd-142 isotope composition. These samples all have measured deficits in Nd-142 relative to the JNdi-1 terrestrial standard in the range -45 to -21 ppm. The range is -45 to -15 ppm once the 62236 Nd-142/Nd-144 ratio is corrected from neutron-capture effects. Analyzed FAS samples do not define a single isochron in either Sm-146-Nd-142 or Sm-147-Nd-143 systematics, suggesting that they either do not have the same crystallization age, come from different sources, or have suffered isotopic disturbance. Because the age is not known for some samples, we explore the implications of their initial isotopic compositions for crystallization ages in the first 400 Ma of solar system history, a timing interval that covers all the ages determined for the ferroan anorthositic suite whole rocks as well as different estimates for the crystallization of the LMO.62255 has the largest deficit in initial Nd-142 and does not appear to have followed the same differentiation path as the other FAS samples. The large deficit in Nd-142 of FAN 62255 may suggest a crystallization age around 60-125 Ma after the beginning of solar system accretion. This result provides essential information about the age of the giant impact forming the Moon. The initial Nd isotopic compositions of FAS samples can be matched either with a bulk-Moon with chondritic Sm/Nd ratio but enstatite-chondrite-like initial Nd-142/Nd-144 (e.g. 10 ppm below modern terrestrial), or a bulk-Moon with superchondritic Sm/Nd ratio and initial Nd-142/Nd-144 similar to ordinary chondrites. (C) 2014 Elsevier Ltd. All rights reserved. C1 [Boyet, Maud] Univ Clermont Ferrand, Univ Blaise Pascal, Lab Magmas & Volcans, UMR 6524, F-63038 Clermont Ferrand, France. [Carlson, Richard W.; Horan, Mary] Carnegie Inst Sci, Dept Terr Magnetism, Washington, DC 20015 USA. [Borg, Lars E.] Lawrence Livermore Natl Lab, Div Chem Sci, Livermore, CA 94550 USA. RP Boyet, M (reprint author), Univ Clermont Ferrand, Univ Blaise Pascal, Lab Magmas & Volcans, UMR 6524, 5 Rue Kessler, F-63038 Clermont Ferrand, France. EM M.Boyet@opgc.univ-bpclermont.fr; rcarlson@carnegiescience.edu; borg5@llnl.gov; mhoran@carnegiescience.edu FU Carnegie Institution of Washington; National Science Foundation [EAR-0320589]; ERC (FP7) [209035]; Laboratory of Excellence ClerVolc [103]; NASA [NNH12AT84I]; U.S. D.O.E. by Lawrence Livermore National Laboratory [DE-AC52-07NA27344] FX We thank T. Mock for having provided support for the mass spectrometer. CAPTEM and the NASA are acknowledged. We further thank Thorsten Kleine, Larry Nyquist and one anonymous reviewer for their constructive reviews. Comments by Marc Norman and Shichun Huang were helpful in improving the manuscript. Funding for this work was provided by Carnegie Institution of Washington, the National Science Foundation (EAR-0320589), the ERC (FP7/2007-2013 Grant Agreement 209035), the Laboratory of Excellence ClerVolc (contribution No. 103), and NASA grant NNH12AT84I to L.E.B. A portion of this work was performed under the auspices of the U.S. D.O.E. by Lawrence Livermore National Laboratory under contract DE-AC52-07NA27344. NR 74 TC 6 Z9 6 U1 7 U2 36 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0016-7037 EI 1872-9533 J9 GEOCHIM COSMOCHIM AC JI Geochim. Cosmochim. Acta PD JAN 1 PY 2015 VL 148 BP 203 EP 218 DI 10.1016/j.gca.2014.09.021 PG 16 WC Geochemistry & Geophysics SC Geochemistry & Geophysics GA AX1ZW UT WOS:000346743900014 ER PT J AU Singh, R Dong, HL Liu, D Zhao, LD Marts, AR Farquhar, E Tierney, DL Almquist, CB Briggs, BR AF Singh, Rajesh Dong, Hailiang Liu, Deng Zhao, Linduo Marts, Amy R. Farquhar, Erik Tierney, David L. Almquist, Catherine B. Briggs, Brandon R. TI Reduction of hexavalent chromium by the thermophilic methanogen Methanothermobacter thermautotrophicus SO GEOCHIMICA ET COSMOCHIMICA ACTA LA English DT Article ID SHEWANELLA-ONEIDENSIS MR-1; CR(VI) UPTAKE MECHANISM; BEARING CLAY-MINERALS; MICROBIAL REDUCTION; REDUCING BACTERIA; THERMOTERRABACTERIUM-FERRIREDUCENS; DISSIMILATORY REDUCTION; METHANOSARCINA-BARKERI; PYROBACULUM-ISLANDICUM; OCHROBACTRUM-ANTHROPI AB Despite significant progress on iron reduction by thermophilic microorganisms, studies on their ability to reduce toxic metals are still limited, despite their common co-existence in high temperature environments (up to 70 degrees C). In this study, Methanothermobacter thermautotrophicus, an obligate thermophilic methanogen, was used to reduce hexavalent chromium. Experiments were conducted in a growth medium with H-2/CO2 as substrate with various Cr6+ concentrations (0.2, 0.4, 1, 3, and 5 mM) in the form of potassium dichromate (K2Cr2O7). Time-course measurements of aqueous Cr6+ concentrations using 1,5-diphenylcarbazide colorimetric method showed complete reduction of the 0.2 and 0.4 mM Cr6+ solutions by this methanogen. However, much lower reduction extents of 43.6%, 13.0%, and 3.7% were observed at higher Cr6+ concentrations of 1, 3 and 5 mM, respectively. These lower extents of bioreduction suggest a toxic effect of aqueous Cr6+ to cells at this concentration range. At these higher Cr6+ concentrations, methanogenesis was inhibited and cell growth was impaired as evidenced by decreased total cellular protein production and live/dead cell ratio. Likewise, Cr6+ bioreduction rates decreased with increased initial concentrations of Cr6+ from 13.3 to 1.9 mu Mh(-1). X-ray absorption near-edge structure (XANES) spectroscopy revealed a progressive reduction of soluble Cr6+ to insoluble Cr3+ precipitates, which was confirmed as amorphous chromium hydroxide by selected area electron diffraction pattern. However, a small fraction of reduced Cr occurred as aqueous Cr3+. Scanning and transmission electron microscope observations of M. thermautotrophicus cells after Cr6+ exposure suggest both extra-and intracellular chromium reduction mechanisms. Results of this study demonstrate the ability of M. thermautotrophicus cells to reduce toxic Cr6+ to less toxic Cr3+ and its potential application in metal bioremediation, especially at high temperature subsurface radioactive waste disposal sites, where the temperature may reach similar to 70 degrees C. (C) 2014 Elsevier Ltd. All rights reserved. C1 [Singh, Rajesh; Dong, Hailiang; Zhao, Linduo; Briggs, Brandon R.] Miami Univ, Dept Geol & Environm Earth Sci, Oxford, OH 45056 USA. [Dong, Hailiang] China Univ Geosci, State Key Lab Biogeol & Environm Geol, Beijing 100083, Peoples R China. [Liu, Deng] China Univ Geosci, State Key Lab Biogeol & Environm Geol, Wuhan 430074, Peoples R China. [Marts, Amy R.; Tierney, David L.] Miami Univ, Dept Chem & Biochem, Oxford, OH 45056 USA. [Farquhar, Erik] Brookhaven Natl Lab, Natl Synchrotron Light Source, Case Western Reserve Univ, Ctr Synchrotron Biosci, Upton, NY 11973 USA. [Almquist, Catherine B.] Miami Univ, Dept Paper & Chem Engn, Oxford, OH 45056 USA. RP Dong, HL (reprint author), Miami Univ, Dept Geol & Environm Earth Sci, Oxford, OH 45056 USA. EM dongh@miamioh.edu FU Subsurface Biogeochemical Research (SBR) Program, Office of Science (BER); U.S. Department of Energy (DOE) [DE-SC0005333]; U.S. National Science Foundation [CHE-1152755] FX This research was supported by the Subsurface Biogeochemical Research (SBR) Program, Office of Science (BER), U.S. Department of Energy (DOE) grant no. DE-SC0005333 to H.D. and by the U.S. National Science Foundation (CHE-1152755 to D.L.T.). The authors are grateful to three anonymous reviewers whose comments improved the quality of the manuscript. NR 84 TC 4 Z9 4 U1 7 U2 48 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0016-7037 EI 1872-9533 J9 GEOCHIM COSMOCHIM AC JI Geochim. Cosmochim. Acta PD JAN 1 PY 2015 VL 148 BP 442 EP 456 DI 10.1016/j.gca.2014.10.012 PG 15 WC Geochemistry & Geophysics SC Geochemistry & Geophysics GA AX1ZW UT WOS:000346743900027 PM 26120143 ER PT J AU Cassata, WS Shuster, DL Renne, PR Weiss, BP AF Cassata, William S. Shuster, David L. Renne, Paul R. Weiss, Benjamin P. TI Evidence for shock heating and constraints on Martian surface temperatures revealed by Ar-40/Ar-39 thermochronometry of Martian meteorites (vol 74, pg 6900, 2010) SO GEOCHIMICA ET COSMOCHIMICA ACTA LA English DT Correction C1 [Cassata, William S.] Lawrence Livermore Natl Lab, Div Chem Sci, Livermore, CA 94550 USA. [Shuster, David L.; Renne, Paul R.] Univ Calif Berkeley, Dept Earth & Planetary Sci, Berkeley, CA 94720 USA. [Shuster, David L.; Renne, Paul R.] Berkeley Geochronol Ctr, Berkeley, CA 94709 USA. [Weiss, Benjamin P.] MIT, Dept Earth Atmospher & Planetary Sci, Cambridge, MA 02139 USA. RP Cassata, WS (reprint author), Lawrence Livermore Natl Lab, Div Chem Sci, 7000 East Ave L-231, Livermore, CA 94550 USA. EM bpweiss@mit.edu RI Shuster, David/A-4838-2011 NR 1 TC 0 Z9 0 U1 0 U2 7 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0016-7037 EI 1872-9533 J9 GEOCHIM COSMOCHIM AC JI Geochim. Cosmochim. Acta PD JAN 1 PY 2015 VL 148 BP 496 EP 498 DI 10.1016/j.gca.2014.09.007 PG 3 WC Geochemistry & Geophysics SC Geochemistry & Geophysics GA AX1ZW UT WOS:000346743900030 ER PT J AU Tan, JG Piao, SL Chen, AP Zeng, ZZ Ciais, P Janssens, IA Mao, JF Myneni, RB Peng, SS Penuelas, J Shi, XY Vicca, S AF Tan, Jianguang Piao, Shilong Chen, Anping Zeng, Zhenzhong Ciais, Philippe Janssens, Ivan A. Mao, Jiafu Myneni, Ranga B. Peng, Shushi Penuelas, Josep Shi, Xiaoying Vicca, Sara TI Seasonally different response of photosynthetic activity to daytime and night-time warming in the Northern Hemisphere SO GLOBAL CHANGE BIOLOGY LA English DT Article DE daytime warming; night-time warming; photosynthesis; seasonal change; vegetation activity ID TERRESTRIAL CARBON-CYCLE; CLIMATE-CHANGE; VEGETATION INDEX; POPULUS-DELTOIDES; GLOBAL PRODUCTS; TIME-SERIES; TEMPERATURE; DROUGHT; ECOSYSTEMS; FEEDBACKS AB Over the last century the Northern Hemisphere has experienced rapid climate warming, but this warming has not been evenly distributed seasonally, as well as diurnally. The implications of such seasonal and diurnal heterogeneous warming on regional and global vegetation photosynthetic activity, however, are still poorly understood. Here, we investigated for different seasons how photosynthetic activity of vegetation correlates with changes in seasonal daytime and night-time temperature across the Northern Hemisphere (>30 degrees N), using Normalized Difference Vegetation Index (NDVI) data from 1982 to 2011 obtained from the Advanced Very High Resolution Radiometer (AVHRR). Our analysis revealed some striking seasonal differences in the response of NDVI to changes in day- vs. night-time temperatures. For instance, while higher daytime temperature (T-max) is generally associated with higher NDVI values across the boreal zone, the area exhibiting a statistically significant positive correlation between T-max and NDVI is much larger in spring (41% of area in boreal zone - total area 12.6x10(6)km(2)) than in summer and autumn (14% and 9%, respectively). In contrast to the predominantly positive response of boreal ecosystems to changes in T-max, increases in T-max tended to negatively influence vegetation growth in temperate dry regions, particularly during summer. Changes in night-time temperature (T-min) correlated negatively with autumnal NDVI in most of the Northern Hemisphere, but had a positive effect on spring and summer NDVI in most temperate regions (e.g., Central North America and Central Asia). Such divergent covariance between the photosynthetic activity of Northern Hemispheric vegetation and day- and night-time temperature changes among different seasons and climate zones suggests a changing dominance of ecophysiological processes across time and space. Understanding the seasonally different responses of vegetation photosynthetic activity to diurnal temperature changes, which have not been captured by current land surface models, is important for improving the performance of next generation regional and global coupled vegetation-climate models. C1 [Tan, Jianguang; Piao, Shilong; Zeng, Zhenzhong; Peng, Shushi] Peking Univ, Sinofrench Inst Earth Syst Sci, Coll Urban & Environm Sci, Beijing 100871, Peoples R China. [Piao, Shilong] Chinese Acad Sci, Inst Tibetan Plateau Res, Key Lab Alpine Ecol & Biodivers, Beijing 100085, Peoples R China. [Chen, Anping] Princeton Univ, Dept Ecol & Evolutionary Biol, Princeton, NJ 08544 USA. [Ciais, Philippe; Peng, Shushi] UMR CEA CNRS, LSCE, F-91191 Gif Sur Yvette, France. [Janssens, Ivan A.; Vicca, Sara] Univ Antwerp, Dept Biol, B-2610 Antwerp, Belgium. [Mao, Jiafu; Shi, Xiaoying] Oak Ridge Natl Lab, Div Environm Sci, Oak Ridge, TN 37831 USA. [Myneni, Ranga B.] Boston Univ, Dept Earth & Environm, Boston, MA 02215 USA. [Penuelas, Josep] CREAF, Barcelona 08193, Catalonia, Spain. [Penuelas, Josep] Global Ecol Unit CREAF CEAB CSIC UAB, CSIC, Barcelona 08193, Catalonia, Spain. RP Piao, SL (reprint author), Peking Univ, Sinofrench Inst Earth Syst Sci, Coll Urban & Environm Sci, Beijing 100871, Peoples R China. EM slpiao@pku.edu.cn RI Janssens, Ivan/P-1331-2014; Chen, Anping/H-9960-2014; Myneni, Ranga/F-5129-2012; Peng, Shushi/J-4779-2014; Penuelas, Josep/D-9704-2011; Vicca, Sara/I-3637-2012; Mao, Jiafu/B-9689-2012 OI Janssens, Ivan/0000-0002-5705-1787; Peng, Shushi/0000-0001-5098-726X; Penuelas, Josep/0000-0002-7215-0150; Vicca, Sara/0000-0001-9812-5837; Mao, Jiafu/0000-0002-2050-7373 FU National Basic Research Program of China [2013CB956303, 2010CB950601]; National Natural Science Foundation of China [41125004, 31321061]; 111 Project [B14001]; US Department of Energy (DOE), Office of Science, Biological and Environmental Research; DOE [DE-AC05-00OR22725] FX This study was supported by the National Basic Research Program of China (Grant No. 2013CB956303 and 2010CB950601), National Natural Science Foundation of China (41125004 and 31321061), and the 111 Project (B14001). Jiafu Mao and Xiaoying Shi1s time is supported by the US Department of Energy (DOE), Office of Science, Biological and Environmental Research. Oak Ridge National Laboratory is managed by UT-BATTELLE for DOE under contract DE-AC05-00OR22725. NR 74 TC 6 Z9 7 U1 9 U2 100 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 1354-1013 EI 1365-2486 J9 GLOBAL CHANGE BIOL JI Glob. Change Biol. PD JAN PY 2015 VL 21 IS 1 BP 377 EP 387 DI 10.1111/gcb.12724 PG 11 WC Biodiversity Conservation; Ecology; Environmental Sciences SC Biodiversity & Conservation; Environmental Sciences & Ecology GA AX1HJ UT WOS:000346698100033 PM 25163596 ER PT J AU Martinez, AD Ortiz, BR Johnson, NE Baranowski, LL Krishna, L Choi, S Dippo, PC To, B Norman, AG Stradins, P Stevanovic, V Toberer, ES Tamboli, AC AF Martinez, Aaron D. Ortiz, Brenden R. Johnson, Nicole E. Baranowski, Lauryn L. Krishna, Lakshmi Choi, Sukgeun Dippo, Patricia C. To, Bobby Norman, Andrew G. Stradins, Paul Stevanovic, Vladan Toberer, Eric S. Tamboli, Adele C. TI Development of ZnSiP2 for Si-Based Tandem Solar Cells SO IEEE JOURNAL OF PHOTOVOLTAICS LA English DT Article DE Density functional theory (DFT); photovoltaic cells; silicon; tandem photovoltaics; ZnSiP2 ID SINGLE-CRYSTALS; EFFICIENCY; PHOTOLUMINESCENCE; SEMICONDUCTORS; COMPOUND; JUNCTION; SPECTRA; SILICON; GROWTH; ZNGEP2 AB A major technological challenge in photovoltaics is the implementation of a lattice matched optically efficient material to be used in conjunction with silicon for tandem photovoltaics. Detailed balance calculations predict an increase in efficiency of up to 12 percentage points for a tandem cell compared with single-junction silicon. Given that the III-V materials currently hold world record efficiencies, both for single and multijunction cells, it would be transformative to develop a material that has similar properties to the III-V's which is also lattice matched to silicon. The II-IV-V-2 chalcopyrites are a promising class of materials that could satisfy these criteria. ZnSiP2 in particular is known to have a bandgap of similar to 2 eV, a lattice mismatch with silicon of 0.5%, and is earth abundant. Its direct bandgap is symmetry-forbidden. We have grown single crystals of ZnSiP2 by a flux growth technique. Structure and phase purity have been confirmed by X-ray diffraction and transmission electron microscopy. Optical measurements, along with a calculation of the absorption spectrum, confirm the similar to 2 eV bandgap. Because of its structural similarity to both crystalline silicon and the III-V's, ZnSiP2 is expected to have good optoelectronic performance. C1 [Martinez, Aaron D.; Ortiz, Brenden R.; Johnson, Nicole E.; Baranowski, Lauryn L.; Krishna, Lakshmi; Stradins, Paul; Stevanovic, Vladan; Toberer, Eric S.; Tamboli, Adele C.] Colorado Sch Mines, Dept Phys, Golden, CO 80401 USA. [Choi, Sukgeun; Dippo, Patricia C.; To, Bobby; Norman, Andrew G.; Stradins, Paul; Stevanovic, Vladan; Toberer, Eric S.; Tamboli, Adele C.] Natl Renewable Energy Lab, Golden, CO 80401 USA. RP Martinez, AD (reprint author), Colorado Sch Mines, Dept Phys, Golden, CO 80401 USA. EM aamartin@mines.edu; bortiz@mymail.mines.edu; nijohnso@mymail.mines.edu; lbaranow@mymail.mines.edu; lkr-ishna@mines.edu; Sukgeun.Choi@nrel.gov; pat.dippo@nrel.gov; Bobby.To@nrel.gov; andrew.norman@nrel.gov; pauls.stradins@nrel.gov; vladan.stevanovic@nrel.gov; etoberer@mines.edu; adele.tamboli@nrel.gov RI Norman, Andrew/F-1859-2010 OI Norman, Andrew/0000-0001-6368-521X FU National Renewable Energy Laboratory through the Laboratory-Directed Research and Development program; National Science Foundation through the Renewable Energy Materials Research and Engineering Center at the Colorado School of Mines under National Science Foundation [DMR-0820518] FX This work was supported by the National Renewable Energy Laboratory through the Laboratory-Directed Research and Development program and by the National Science Foundation through the Renewable Energy Materials Research and Engineering Center at the Colorado School of Mines under National Science Foundation Grant DMR-0820518. NR 39 TC 1 Z9 1 U1 5 U2 35 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 2156-3381 J9 IEEE J PHOTOVOLT JI IEEE J. Photovolt. PD JAN PY 2015 VL 5 IS 1 BP 17 EP 21 DI 10.1109/JPHOTOV.2014.2362305 PG 5 WC Energy & Fuels; Materials Science, Multidisciplinary; Physics, Applied SC Energy & Fuels; Materials Science; Physics GA AX1WA UT WOS:000346732700003 ER PT J AU Hacke, P Terwilliger, K Glick, S Tamizhmani, G Tatapudi, S Stark, C Koch, S Weber, T Berghold, J Hoffmann, S Koehl, M Dietrich, S Ebert, M Mathiak, G AF Hacke, Peter Terwilliger, Kent Glick, Stephen Tamizhmani, Govindasamy Tatapudi, Sai Stark, Cameron Koch, Simon Weber, Thomas Berghold, Juliane Hoffmann, Stephan Koehl, Michael Dietrich, Sascha Ebert, Matthias Mathiak, Gerhard TI Interlaboratory Study to Determine Repeatability of the Damp-Heat Test Method for Potential-Induced Degradation and Polarization in Crystalline Silicon Photovoltaic Modules SO IEEE JOURNAL OF PHOTOVOLTAICS LA English DT Article DE High voltage techniques; photovoltaic systems; solar energy ID SYSTEM VOLTAGE STRESS; SOLAR-CELLS AB To test reproducibility of a technical specification under development for potential-induced degradation (PID) and polarization, three crystalline silicon module types were distributed in five replicas each to five laboratories. Stress tests were performed in environmental chambers at 60 degrees C, 85% relative humidity, 96 h, and with module nameplate system voltage applied. Results from the modules tested indicate that the test protocol can discern susceptibility to PID according to the pass/fail criteria with acceptable consistency fromlab to lab; however, areas for improvement are indicated to achieve better uniformity in temperature and humidity on the module surfaces. In the analysis of variance of the results, 6% of the variance was attributed to laboratory influence, 34% to module design, and 60% to variability in test results within a given design. Testing with the additional factor of illumination with ultraviolet light slowed or arrested the degradation. Testing at 25 degrees C with aluminum foil as the module ground was also examined for comparison. The foil, as tested, did not itself achieve consistent contact to ground at all surfaces, but methods to ensure more consistent grounding were found and proposed. The rates of degradation in each test are compared, and details affecting the rates are discussed. C1 [Hacke, Peter; Terwilliger, Kent; Glick, Stephen] Natl Renewable Energy Lab, Golden, CO 80401 USA. [Tamizhmani, Govindasamy; Tatapudi, Sai; Stark, Cameron] Arizona State Univ, Tempe, AZ 85287 USA. [Koch, Simon; Weber, Thomas; Berghold, Juliane] Photovolta Inst Berlin, D-10997 Berlin, Germany. [Hoffmann, Stephan; Koehl, Michael] Fraunhofer ISE, D-79110 Freiburg, Germany. [Dietrich, Sascha; Ebert, Matthias] Fraunhofer Ctr Silicon Photovolta, Dept Module Reliabil, D-06120 Halle, Germany. [Mathiak, Gerhard] TUV Rheinland Energie & Umwelt GmbH, Dept Solar Energy, D-51105 Cologne, Germany. RP Hacke, P (reprint author), Natl Renewable Energy Lab, Golden, CO 80401 USA. EM peter.hacke@nrel.gov; kent.terwilliger@nrel.gov; Stephen.Glick@nrel.gov; manit@asu.edu; statapud@asu.edu; ceandy@asu.edu; koch@pi-berlin.com; weber@pi-berlin.com; berghold@pi-berlin.com; Stephan.Hoffmann@ise.fraunhofer.de; Michael.Koehl@ise.fraunhofer.de; Sascha.Dietrich@csp.fraunhofer.de; matthias.ebert@csp.fraunhofer.de; gerhard.mathiak@de.tuv.com FU U.S. Department of Energy [DE-AC36-08-GO28308]; National Renewable Energy Laboratory FX This work was supported by the U.S. Department of Energy under Contract DE-AC36-08-GO28308 with the National Renewable Energy Laboratory. NR 21 TC 4 Z9 4 U1 2 U2 11 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 2156-3381 J9 IEEE J PHOTOVOLT JI IEEE J. Photovolt. PD JAN PY 2015 VL 5 IS 1 BP 94 EP 101 DI 10.1109/JPHOTOV.2014.2361650 PG 8 WC Energy & Fuels; Materials Science, Multidisciplinary; Physics, Applied SC Energy & Fuels; Materials Science; Physics GA AX1WA UT WOS:000346732700015 ER PT J AU Sauer, KJ Roessler, T Hansen, CW AF Sauer, Kenneth J. Roessler, Thomas Hansen, Clifford W. TI Modeling the Irradiance and Temperature Dependence of Photovoltaic Modules in PVsyst SO IEEE JOURNAL OF PHOTOVOLTAICS LA English DT Article DE Current-voltage characteristics; mathematical model; minimization; photovoltaic (PV) cells; PV systems; silicon; solar power generation AB In order to reliably simulate the energy yield of photovoltaic (PV) systems, it is necessary to have an accurate model of how the PV modules perform with respect to irradiance and cell temperature. Building on a previous study that addresses the irradiance dependence, two approaches to fit the temperature dependence of module power in PVsyst have been developed and are applied here to recent multi-irradiance and temperature data for a standard Yingli Solar PV module type. The results demonstrate that it is possible to match the measured irradiance and temperature dependence of PV modules in PVsyst. Improvements in energy yield prediction using the optimized models relative to the PVsyst standard model are considered significant for decisions about project financing. C1 [Sauer, Kenneth J.] Yingli Green Energy Amer Inc, San Francisco, CA 94108 USA. [Roessler, Thomas] Yingli Green Energy Int AG, CH-8058 Zurich, Switzerland. [Hansen, Clifford W.] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Sauer, KJ (reprint author), Yingli Green Energy Amer Inc, San Francisco, CA 94108 USA. EM kenneth.sauer@yingliamericas.com; thomas.roessler@yinglisolar.ch; cwhanse@sandia.gov NR 10 TC 14 Z9 14 U1 3 U2 9 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 2156-3381 J9 IEEE J PHOTOVOLT JI IEEE J. Photovolt. PD JAN PY 2015 VL 5 IS 1 BP 152 EP 158 DI 10.1109/JPHOTOV.2014.2364133 PG 7 WC Energy & Fuels; Materials Science, Multidisciplinary; Physics, Applied SC Energy & Fuels; Materials Science; Physics GA AX1WA UT WOS:000346732700022 ER PT J AU Jordan, DC Kurtz, SR AF Jordan, Dirk C. Kurtz, Sarah R. TI Field Performance of 1.7 GW of Photovoltaic Systems SO IEEE JOURNAL OF PHOTOVOLTAICS LA English DT Article DE Durability; field failure; field performance; photovoltaic system; reliability ID CONNECTED PV SYSTEMS AB This paper presents performance data from nearly 50 000 photovoltaic systems totaling 1.7 GW of capacity installed in the USA from 2009 to 2012. Most systems without reported issues, about 90%, produced greater than 90% of the electricity predicted before installation. The data were shown to be consistent with the assumption of historical degradation rates of about 0.5% per year; excessive degradation rates such as 2% or 3% per year were not observed. Large systems showed an insolation-adjusted yield that was about 4% higher than smaller systems. Only 2-4% of the data indicated issues significantly affecting system performance. Delays and interconnections dominate project-related issues particularly in the first year, but were reported in less than 0.5% of all systems. Hardware-related issues are dominated by inverter problems as reported for less than 0.4% and underperforming modules for less than 0.1%. C1 [Jordan, Dirk C.; Kurtz, Sarah R.] Natl Renewable Energy Lab, Golden, CO 80401 USA. RP Jordan, DC (reprint author), Natl Renewable Energy Lab, Golden, CO 80401 USA. EM dirk.jordan@nrel.gov; Sarah.Kurtz@nrel.gov FU U.S. Department of Energy [DE-AC36-08-GO28308]; National Renewable Energy Laboratory FX This work was supported by the U.S. Department of Energy under Contract DE-AC36-08-GO28308 with the National Renewable Energy Laboratory. NR 22 TC 1 Z9 1 U1 2 U2 7 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 2156-3381 J9 IEEE J PHOTOVOLT JI IEEE J. Photovolt. PD JAN PY 2015 VL 5 IS 1 BP 243 EP 249 DI 10.1109/JPHOTOV.2014.2361667 PG 7 WC Energy & Fuels; Materials Science, Multidisciplinary; Physics, Applied SC Energy & Fuels; Materials Science; Physics GA AX1WA UT WOS:000346732700036 ER PT J AU Wang, XF Bhosale, J Moore, J Kapadia, R Bermel, P Javey, A Lundstrom, M AF Wang, Xufeng Bhosale, Jayprakash Moore, James Kapadia, Rehan Bermel, Peter Javey, Ali Lundstrom, Mark TI Photovoltaic Material Characterization With Steady State and Transient Photoluminescence SO IEEE JOURNAL OF PHOTOVOLTAICS LA English DT Article DE Charge carrier lifetime; indium phosphide; photoluminescence (PL); photovoltaic cells ID SURFACE-RECOMBINATION VELOCITY; TIME-RESOLVED PHOTOLUMINESCENCE; SHOCKLEY-QUEISSER LIMIT; INP SINGLE-CRYSTALS; SOLAR-CELLS; LIFETIME; LUMINESCENCE; DEVICES AB In this study, we develop an approach to characterize the surface and bulk properties for thin films of photovoltaic materials by combining two experimental photoluminescence (PL) techniques with one multiphysics simulation. This contactless, in-line characterization technique allows reliable extraction of key lifetime parameters. In this study, we first discuss the strengths and weaknesses of both steady-state and transient PL techniques (specifically, steady-state PL excitation spectroscopy and time-resolved PL) and show that combining them with numerical simulation can be used to extract surface and bulk lifetimes self consistently. The method is applied to InP thin films grown with a novel vapor-liquid-solid method. The InP thin film tested is found to have a bulk Shockley-Read-Hall (SRH) lifetime of 12 ns and a front surface recombination velocity of 5 x 10(4) cm/s. C1 [Wang, Xufeng; Bhosale, Jayprakash; Moore, James; Bermel, Peter; Lundstrom, Mark] Purdue Univ, Sch Elect & Comp Engn, W Lafayette, IN 47907 USA. [Kapadia, Rehan; Javey, Ali] Univ Calif Berkeley, Dept Elect Engn & Comp Sci, Berkeley, CA 94720 USA. [Kapadia, Rehan; Javey, Ali] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. RP Wang, XF (reprint author), Purdue Univ, Sch Elect & Comp Engn, W Lafayette, IN 47907 USA. EM wang159@purdue.edu; jbhosale@purdue.edu; moore32@purdue.edu; rkapadia@eecs.berkeley.edu; pbermel@purdue.edu; ajavey@eecs.berkeley.edu; lundstro@ecn.purdue.edu FU Department of Energyy (DOE) under DOE [DE-EE0004946]; Semiconductor Research Corporation [2110.003] FX This work was supported by the Department of Energyy (DOE), under DOE Cooperative Agreement DE-EE0004946 ("PVMI Bay Area PV Consortium"), and the Semiconductor Research Corporation, under Research Task 2110.003 ("Network for Photovoltaic Technologies"). NR 39 TC 3 Z9 3 U1 4 U2 23 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 2156-3381 J9 IEEE J PHOTOVOLT JI IEEE J. Photovolt. PD JAN PY 2015 VL 5 IS 1 BP 282 EP 287 DI 10.1109/JPHOTOV.2014.2361015 PG 6 WC Energy & Fuels; Materials Science, Multidisciplinary; Physics, Applied SC Energy & Fuels; Materials Science; Physics GA AX1WA UT WOS:000346732700042 ER PT J AU Silverman, TJ Deceglie, MG Marion, B Kurtz, SR AF Silverman, Timothy J. Deceglie, Michael G. Marion, Bill Kurtz, Sarah R. TI Performance Stabilization of CdTe PV Modules Using Bias and Light SO IEEE JOURNAL OF PHOTOVOLTAICS LA English DT Article DE CdTe; light soak; metastability; module; performance; stabilization; thin-film; transient ID SOLAR-CELLS AB Reversible performance changes due to light exposure frustrate repeatable performance measurements on CdTe photovoltaic modules. It is common to use extended light exposure to ensure that measurements are representative of outdoor performance. We quantify the extent to which such a light-exposed state depends on module temperature and consider voltage bias in the dark to aid in stabilization. We evaluate the use of dark forward voltage bias to bring about a performance state equivalent to that obtained with light exposure, as well as to maintain a light-exposed state prior to standard test condition (STC) performance measurement. Our results indicate that the most promising method for measuring a light-exposed state is to use light exposure at controlled temperature followed by prompt STC measurement with a repeatable time interval between exposure and the STC measurement. C1 [Silverman, Timothy J.; Deceglie, Michael G.; Marion, Bill; Kurtz, Sarah R.] Natl Renewable Energy Lab, Golden, CO 80401 USA. RP Silverman, TJ (reprint author), Natl Renewable Energy Lab, Golden, CO 80401 USA. EM timothy.silverman@nrel.gov; michael.deceglie@nrel.gov; bill.marion@nrel.gov; Sarah.Kurtz@nrel.gov FU U.S. Department of Energy [DE-AC36-08GO28308]; National Renewable Energy Laboratory FX This work was supported by the U.S. Department of Energy under Contract DE-AC36-08GO28308 with the National Renewable Energy Laboratory. NR 10 TC 4 Z9 4 U1 1 U2 7 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 2156-3381 J9 IEEE J PHOTOVOLT JI IEEE J. Photovolt. PD JAN PY 2015 VL 5 IS 1 BP 344 EP 349 DI 10.1109/JPHOTOV.2014.2370252 PG 6 WC Energy & Fuels; Materials Science, Multidisciplinary; Physics, Applied SC Energy & Fuels; Materials Science; Physics GA AX1WA UT WOS:000346732700050 ER PT J AU Dall'Anese, E Dhople, SV Johnson, BB Giannakis, GB AF Dall'Anese, Emiliano Dhople, Sairaj V. Johnson, Brian B. Giannakis, Georgios B. TI Optimal Dispatch of Residential Photovoltaic Inverters Under Forecasting Uncertainties SO IEEE JOURNAL OF PHOTOVOLTAICS LA English DT Article DE Conditional value-at-risk (CVaR); distribution networks; forecasting errors; inverter control; microgrids; optimal power flow (OPF); photovoltaic (PV) systems; voltage regulation ID OPF PROBLEM; POWER; SYSTEMS AB Efforts to ensure reliable operation of existing low-voltage distribution systems with high photovoltaic (PV) generation have focused on the possibility of inverters providing ancillary services such as active power curtailment and reactive power compensation. Major benefits include the possibility of averting overvoltages, which may otherwise be experienced when PV generation exceeds the demand. This paper deals with ancillary service procurement in the face of solar irradiance forecasting errors. In particular, assuming that forecasted PV irradiance can be described by a random variable with known (empirical) distribution, the proposed uncertainty-aware optimal inverter dispatch (OID) framework indicates which inverters should provide ancillary services with a guaranteed a priori risk level of PV generation surplus. To capture forecasting errors and strike a balance between risk of overvoltages and (re) active power reserves, the concept of conditional value-at-risk is advocated. Due to AC power balance equations and binary inverter selection variables, the formulated OID involves the solution of a nonconvex mixed-integer nonlinear program. However, a computationally affordable convex relaxation is derived by leveraging sparsity-promoting regularization approaches and semidefinite relaxation techniques. C1 [Dall'Anese, Emiliano; Dhople, Sairaj V.; Giannakis, Georgios B.] Univ Minnesota, Dept Elect & Comp Engn, Minneapolis, MN 55455 USA. [Dall'Anese, Emiliano; Dhople, Sairaj V.; Giannakis, Georgios B.] Univ Minnesota, Digital Technol Ctr, Minneapolis, MN 55455 USA. [Johnson, Brian B.] Natl Renewable Energy Lab, Golden, CO 80401 USA. RP Dall'Anese, E (reprint author), Univ Minnesota, Dept Elect & Comp Engn, Minneapolis, MN 55455 USA. EM emiliano@umn.edu; sdhople@umn.edu; brian.johnson@nrel.gov; georgios@umn.edu FU Institute of Renewable Energy and the Environment, University of Minnesota [RL-0010-13]; Laboratory Directed Research and Development Program at the National Renewable Energy Laboratory; National Science Foundation [CCF 1423316, CyberSEES 1442686] FX This work was supported by the Institute of Renewable Energy and the Environment under Grant RL-0010-13, University of Minnesota, by the Laboratory Directed Research and Development Program at the National Renewable Energy Laboratory, and by the National Science Foundation under Grant CCF 1423316 and Grant CyberSEES 1442686. NR 37 TC 11 Z9 11 U1 1 U2 3 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 2156-3381 J9 IEEE J PHOTOVOLT JI IEEE J. Photovolt. PD JAN PY 2015 VL 5 IS 1 BP 350 EP 359 DI 10.1109/JPHOTOV.2014.2364125 PG 10 WC Energy & Fuels; Materials Science, Multidisciplinary; Physics, Applied SC Energy & Fuels; Materials Science; Physics GA AX1WA UT WOS:000346732700051 ER PT J AU Kuciauskas, D Kanevce, A Dippo, P Seyedmohammadi, S Malik, R AF Kuciauskas, Darius Kanevce, Ana Dippo, Pat Seyedmohammadi, Shahram Malik, Roger TI Minority-Carrier Lifetime and Surface Recombination Velocity in Single-Crystal CdTe SO IEEE JOURNAL OF PHOTOVOLTAICS LA English DT Article DE Cadmium compounds; charge-carrier lifetime; photovoltaic cells; photoluminescence (PL) ID GROWN CDTE; PHOTOLUMINESCENCE; BAND; LUMINESCENCE; INTERFACE AB We apply an earlier developed method [Kuciauskas et al., IEEE J. Photovoltaics, vol. 3, p. 1319, 2013] to analyze surface and bulk recombination in high-quality undoped single-crystal CdTe. By using two-photon excitation time-resolved photoluminescence, we determined a room-temperature minority-carrier lifetime of 360 ns. This lifetime has weak temperature dependence at 202-295 K. We also show that the high surface recombination velocity (> 10(5) cm/s) typical for single-crystal CdTe was reduced by an order of magnitude to approximate to 1 x 10(4) cm/s. C1 [Kuciauskas, Darius; Kanevce, Ana; Dippo, Pat] Natl Renewable Energy Lab, Golden, CO 80401 USA. [Seyedmohammadi, Shahram; Malik, Roger] First Solar, Santa Clara, CA USA. RP Kuciauskas, D (reprint author), Natl Renewable Energy Lab, Golden, CO 80401 USA. EM Darius.Kuciauskas@nrel.gov; Ana.Kanevce@nrel.gov; pat.dippo@nrel.gov; Shahram.S@Firstsolar.com; roger.malik@firstsolar.com FU U.S. Department of Energy [DE-AC36-08-GO28308]; National Renewable Energy Laboratory FX This work was supported in part by the U.S. Department of Energy under Contract DE-AC36-08-GO28308 with the National Renewable Energy Laboratory. NR 27 TC 19 Z9 19 U1 2 U2 24 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 2156-3381 J9 IEEE J PHOTOVOLT JI IEEE J. Photovolt. PD JAN PY 2015 VL 5 IS 1 BP 366 EP 371 DI 10.1109/JPHOTOV.2014.2359738 PG 6 WC Energy & Fuels; Materials Science, Multidisciplinary; Physics, Applied SC Energy & Fuels; Materials Science; Physics GA AX1WA UT WOS:000346732700053 ER PT J AU Siah, SC Jaramillo, R Chakraborty, R Erslev, PT Sun, CJ Weng, TC Toney, MF Teeter, G Buonassisi, T AF Siah, Sin Cheng Jaramillo, R. Chakraborty, Rupak Erslev, Peter T. Sun, Cheng-Jun Weng, Tsu-Chien Toney, Michael F. Teeter, Glenn Buonassisi, Tonio TI X-Ray Absorption Spectroscopy Study of Structure and Stability of Disordered (Cu2SnS3)(1-x)(ZnS)(x) Alloys SO IEEE JOURNAL OF PHOTOVOLTAICS LA English DT Article DE Amorphous semiconductors; annealing; photovoltaic cells; thin films ID SULFUR K-EDGE; CHALCOPYRITE; IFEFFIT; EXAFS AB Secondary phase segregation is hypothesized to have detrimental impacts on Cu2ZnSnS4 (CZTS) thin-film solar cells. In this study, we demonstrate the potential of using kinetic stabilization to inhibit phase decomposition in CZTS. By growing CZTS films at low temperature, we achieve a kinetically stabilized alloy with an expanded solid solution window in the pseudoternary CuSZnS-SnS phase diagram. Using X-ray absorption spectroscopy, we study the structural evolution and stability of this metastable alloy upon annealing. For near-stoichiometric samples, we observe a continuous emergence of short-range order toward crystalline CZTS that is nearly complete after a 1-min anneal at 450 degrees C. For Zn-rich samples, we detect precipitation of ZnS upon annealing, which suggests that the excess Zn exists as cation antisite defects in metastable CZTS. C1 [Siah, Sin Cheng; Jaramillo, R.; Chakraborty, Rupak; Buonassisi, Tonio] MIT, Cambridge, MA 02139 USA. [Erslev, Peter T.; Teeter, Glenn] Natl Renewable Energy Lab, Golden, CO 80401 USA. [Sun, Cheng-Jun] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. [Weng, Tsu-Chien; Toney, Michael F.] Stanford Synchrotron Radiat Lightsource, Menlo Pk, CA 94025 USA. RP Siah, SC (reprint author), MIT, Cambridge, MA 02139 USA. EM sincheng@alum.mit.edu; rjaramil@mit.edu; rupak@mit.edu; pete.erslev@gmail.com; cjsun@aps.anl.gov; tsuchien@slac.stanford.edu; mftoney@slac.stanford.edu; Glenn.Teeter@nrel.gov; buonassisi@mit.edu FU Massachusetts Institute of Technology under the U.S. Department of Energy SunShot Next Generation Photovoltaics II Award [DE-EE00024605]; U.S. DOE [DE-AC02-06CH11357]; U.S. Department of Energy, Office of Basic Energy Sciences [DE-AC02-76SF00515]; Clean Energy Scholarship from National Research Foundation (NRF) of Singapore; DOE (Energy Efficiency and Renewable Energy) EERE Postdoctoral Research Award FX This work was performed at the National Renewable Energy Laboratory and the Massachusetts Institute of Technology under the U.S. Department of Energy SunShot Next Generation Photovoltaics II Award DE-EE00024605. PNC/XSD facilities at the Advanced Photon Source, and research at these facilities, were supported by the U.S. Department of Energy (DOE)-Basic Energy Sciences; the Canadian Light Source and its funding partners; the University of Washington; and the Advanced Photon Source. Use of the Advanced Photon Source, which is an Office of Science User Facility operated for the U.S. Department of Energy Office of Science by Argonne National Laboratory, Argonne, IL, USA, was supported by the U.S. DOE under Contract DE-AC02-06CH11357. Use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, is supported by the U.S. Department of Energy, Office of Basic Energy Sciences, under Contract DE-AC02-76SF00515. This work was also supported by a Clean Energy Scholarship from the National Research Foundation (NRF) of Singapore (S.C. Siah) and a DOE (Energy Efficiency and Renewable Energy) EERE Postdoctoral Research Award (R. Jaramillo). NR 22 TC 3 Z9 3 U1 2 U2 48 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 2156-3381 J9 IEEE J PHOTOVOLT JI IEEE J. Photovolt. PD JAN PY 2015 VL 5 IS 1 BP 372 EP 377 DI 10.1109/JPHOTOV.2014.2360334 PG 6 WC Energy & Fuels; Materials Science, Multidisciplinary; Physics, Applied SC Energy & Fuels; Materials Science; Physics GA AX1WA UT WOS:000346732700054 ER PT J AU Reese, MO Burst, JM Perkins, CL Kanevce, A Johnston, SW Kuciauskas, D Barnes, TM Metzger, WK AF Reese, Matthew O. Burst, James M. Perkins, Craig L. Kanevce, Ana Johnston, Steven W. Kuciauskas, Darius Barnes, Teresa M. Metzger, Wyatt K. TI Surface Passivation of CdTe Single Crystals SO IEEE JOURNAL OF PHOTOVOLTAICS LA English DT Article DE Cadmium compounds; charge carrier lifetime; photoluminescence; photovoltaic cells ID TIME-RESOLVED PHOTOLUMINESCENCE; RECOMBINATION DYNAMICS; CADMIUM TELLURIDE; LIFETIME; CONTACTS; VELOCITY; BULK AB Low open-circuit voltages (850-870 mV), due to excessive bulk and surface recombination, currently limit CdTe photovoltaic efficiencies. Here, we study surface recombination in single crystals with single-photon excitation time-resolved photoluminescence (1PE-TRPL) to measure minority carrier lifetimes. Typically, minority carrier lifetimes of untreated undoped CdTe material as measured by 1PE-TRPL are similar to 100 ps or less, even though their bulk lifetimes as measured by two-photon excitation TRPL can reach 100 ns. Such short 1PE-TRPL lifetimes indicate very high surface recombination velocities exceeding 100 000 cm/s. Here, we examine treatments that can reduce surface recombination and discuss different ways of evaluating their efficacy. C1 [Reese, Matthew O.; Burst, James M.; Perkins, Craig L.; Kanevce, Ana; Johnston, Steven W.; Kuciauskas, Darius; Barnes, Teresa M.; Metzger, Wyatt K.] Natl Renewable Energy Lab, Golden, CO 80401 USA. RP Reese, MO (reprint author), Natl Renewable Energy Lab, Golden, CO 80401 USA. EM Matthew.Reese@nrel.gov; james.burst@nrel.ogv; craig.perkins@nrel.gov; Ana.Kanevce@nrel.gov; steven.johnston@nrel.gov; darius.kuciauskas@nrel.gov; teresa.barnes@nrel.gov; wyatt.metzger@nrel.gov FU U.S. Department of Energy [DE-AC36-08-GO28308]; National Renewable Energy Laboratory FX This work was supported by the U.S. Department of Energy under Contract DE-AC36-08-GO28308 with the National Renewable Energy Laboratory. NR 21 TC 4 Z9 4 U1 5 U2 24 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 2156-3381 J9 IEEE J PHOTOVOLT JI IEEE J. Photovolt. PD JAN PY 2015 VL 5 IS 1 BP 382 EP 385 DI 10.1109/JPHOTOV.2014.2362298 PG 4 WC Energy & Fuels; Materials Science, Multidisciplinary; Physics, Applied SC Energy & Fuels; Materials Science; Physics GA AX1WA UT WOS:000346732700056 ER PT J AU Li, H Jiang, CS Metzger, WK Shih, CK Al-Jassim, M AF Li, Huan Jiang, Chun-Sheng Metzger, Wyatt K. Shih, Chih-Kang Al-Jassim, Mowafak TI Microscopic Real-Space Resistance Mapping Across CdTe Solar Cell Junctions by Scanning Spreading Resistance Microscopy SO IEEE JOURNAL OF PHOTOVOLTAICS LA English DT Article DE CdTe; microelectrical property; solar cell junction; scanning spreading resistance microscopy (SRRM); Thin-film PV ID POLYCRYSTALLINE CDS/CDTE HETEROJUNCTIONS; THIN-FILMS; DIFFUSION; SULFUR AB We report on scanning spreading resistance microscopy on cross sections of thin-film CdTe devices. The results show the capability of identifying the multiple layers, the depletion region, and the nonuniform doping. We observe carrier injection and depletion region movement by laser illumination or by electrically biasing the device, directly revealing the underlying physics of the solar cell junction in real space with resolutions of nanometer scale. C1 [Li, Huan; Jiang, Chun-Sheng; Metzger, Wyatt K.; Al-Jassim, Mowafak] Natl Renewable Energy Lab, Golden, CO 80401 USA. [Li, Huan; Shih, Chih-Kang] Univ Texas Austin, Dept Phys, Austin, TX 78712 USA. RP Li, H (reprint author), Natl Renewable Energy Lab, Golden, CO 80401 USA. EM huan@physics.utexas.edu; chun.sheng.jiang@nrel.gov; wyatt.metzger@nrel.gov; shih@physics.utexas.edu; mowafak.aljassim@nrel.gov RI jiang, chun-sheng/F-7839-2012 FU U.S. Department of Energy [DOE-AC36-08GO28308]; National Renewable Energy Laboratory FX This work was supported by the U.S. Department of Energy under Contract DOE-AC36-08GO28308 with the National Renewable Energy Laboratory. NR 18 TC 2 Z9 2 U1 2 U2 18 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 2156-3381 J9 IEEE J PHOTOVOLT JI IEEE J. Photovolt. PD JAN PY 2015 VL 5 IS 1 BP 395 EP 400 DI 10.1109/JPHOTOV.2014.2363569 PG 6 WC Energy & Fuels; Materials Science, Multidisciplinary; Physics, Applied SC Energy & Fuels; Materials Science; Physics GA AX1WA UT WOS:000346732700059 ER PT J AU Geisz, JF Steiner, MA Garcia, I France, RM Friedman, DJ Kurtz, SR AF Geisz, John F. Steiner, Myles A. Garcia, Ivan France, Ryan M. Friedman, Daniel J. Kurtz, Sarah R. TI Implications of Redesigned, High-Radiative-Efficiency GaInP Junctions on III-V Multijunction Concentrator Solar Cells SO IEEE JOURNAL OF PHOTOVOLTAICS LA English DT Article DE Luminescent coupling; multijunction photovoltaic cells; radiative efficiency; III-V ID OPTIMIZATION; LUMINESCENCE; VOLTAGE; DESIGN; LIMIT AB Nonradiative recombination in inverted GaInP junctions is dramatically reduced using a rear-heterojunction design rather than the more traditional thin-emitter homojunction design. When this GaInP junction design is included in inverted multijunction solar cells, the high radiative efficiency translates into both higher subcell voltage and high luminescence coupling to underlying subcells, both of which contribute to improved performance. Subcell voltages within two and four junction devices are measured by electroluminescence and the internal radiative efficiency is quantified as a function of recombination current using optical modeling. The performance of these concentrator multijunction devices is compared with the Shockley-Queisser detailed-balance radiative limit, as well as an internal radiative limit, which considers the effects of the actual optical environment in which a perfect junction may exist. C1 [Geisz, John F.; Steiner, Myles A.; Garcia, Ivan; France, Ryan M.; Friedman, Daniel J.; Kurtz, Sarah R.] Natl Renewable Energy Lab, Golden, CO 80401 USA. [Garcia, Ivan] Univ Politecn Madrid, Inst Energia Solar, E-28040 Madrid, Spain. RP Geisz, JF (reprint author), Natl Renewable Energy Lab, Golden, CO 80401 USA. EM john.geisz@nrel.gov; myles.steiner@nrel.gov; ivan.garcia@nrel.gov; ryan.france@nrel.gov; daniel.friedman@nrel.gov; Sarah.Kurtz@nrel.gov RI Garcia, Ivan/L-1547-2014 OI Garcia, Ivan/0000-0002-9895-2020 FU U.S. Department of Energy [DE-AC36-08-GO28308]; National Renewable Energy Laboratory; People Programme (Marie Curie Actions) of the European Union [299878] FX This work was supported by the U.S. Department of Energy under Contract DE-AC36-08-GO28308 with the National Renewable Energy Laboratory. The work of I. Garcia was supported by the People Programme (Marie Curie Actions) of the European Union's Seventh Framework Programme (FP7/2007-2013) under REA Grant 299878. NR 29 TC 2 Z9 2 U1 1 U2 15 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 2156-3381 J9 IEEE J PHOTOVOLT JI IEEE J. Photovolt. PD JAN PY 2015 VL 5 IS 1 BP 418 EP 424 DI 10.1109/JPHOTOV.2014.2361014 PG 7 WC Energy & Fuels; Materials Science, Multidisciplinary; Physics, Applied SC Energy & Fuels; Materials Science; Physics GA AX1WA UT WOS:000346732700063 ER PT J AU France, RM Geisz, JF Garcia, I Steiner, MA McMahon, WE Friedman, DJ Moriarty, TE Osterwald, C Ward, JS Duda, A Young, M Olavarria, WJ AF France, Ryan M. Geisz, John F. Garcia, Ivan Steiner, Myles A. McMahon, William E. Friedman, Daniel J. Moriarty, Tom E. Osterwald, Carl Ward, J. Scott Duda, Anna Young, Michelle Olavarria, Waldo J. TI Quadruple-Junction Inverted Metamorphic Concentrator Devices SO IEEE JOURNAL OF PHOTOVOLTAICS LA English DT Article DE Metamorphic; multijunction; III-V ID MULTIJUNCTION SOLAR-CELLS; EFFICIENCY AB We present results for quadruple-junction inverted metamorphic (4J-IMM) devices under the concentrated direct spectrum and analyze the present limitations to performance. The devices integrate lattice-matched subcells with rear heterojunctions, as well as lattice-mismatched subcells with low threading dislocation density. To interconnect the subcells, thermally stable lattice-matched tunnel junctions are used, as well as a metamorphic GaAsSb/GaInAs tunnel junction between the lattice-mismatched subcells. A broadband antireflection coating is used, as well as a front metal grid designed for high concentration operation. The best device has a peak efficiency of (43.8 +/- 2.2)% at 327-sun concentration, as measured with a spectrally adjustable flash simulator, and maintains an efficiency of (42.9 +/- 2.1)% at 869 suns, which is the highest concentration measured. The V-oc increases from 3.445 V at 1-sun to 4.10 V at 327-sun concentration, which indicates high material quality in all of the subcells. The subcell voltages are analyzed using optical modeling, and the present device limitations and pathways to improvement are discussed. Although further improvements are possible, the 4J-IMM structure is clearly capable of very high efficiency at concentration, despite the complications arising from utilizing lattice-mismatched subcells. C1 [France, Ryan M.; Geisz, John F.; Steiner, Myles A.; McMahon, William E.; Friedman, Daniel J.; Moriarty, Tom E.; Osterwald, Carl; Ward, J. Scott; Duda, Anna; Young, Michelle; Olavarria, Waldo J.] Natl Renewable Energy Lab, Golden, CO 80401 USA. [Garcia, Ivan] Univ Politecn Madrid, Inst Energia Solar, E-28040 Madrid, Spain. RP France, RM (reprint author), Natl Renewable Energy Lab, Golden, CO 80401 USA. EM ryan.france@nrel.gov; john.geisz@nrel.gov; ivan.garcia@nrel.gov; myles.steiner@nrel.gov; bill.mcmahon@nrel.gov; daniel.friedman@nrel.gov; Tom.Moriarty@nrel.gov; Carl.Osterwald@nrel.gov; scott.ward@nrel.gov; anna.duda@nrel.gov; michelle.young@nrel.gov; waldo.olavarria@nrel.gov FU U.S. Department of Energy [DE-AC36-08-GO28308]; National Renewable Energy Laboratory; IOF from People Program (Marie Curie Actions) of the European Union [299878] FX This work was supported by the U.S. Department of Energy under Contract DE-AC36-08-GO28308 with the National Renewable Energy Laboratory. The work of I. Garcia was supported by an IOF grant from the People Program (Marie Curie Actions) of the European Union's Seventh Framework Program (FP7/2007-2013) under REA Grant 299878. NR 27 TC 25 Z9 25 U1 2 U2 24 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 2156-3381 J9 IEEE J PHOTOVOLT JI IEEE J. Photovolt. PD JAN PY 2015 VL 5 IS 1 BP 432 EP 437 DI 10.1109/JPHOTOV.2014.2364132 PG 6 WC Energy & Fuels; Materials Science, Multidisciplinary; Physics, Applied SC Energy & Fuels; Materials Science; Physics GA AX1WA UT WOS:000346732700065 ER PT J AU Garcia, I McMahon, WE Steiner, MA Geisz, JF Habte, A Friedman, DJ AF Garcia, Ivan McMahon, William E. Steiner, Myles A. Geisz, John F. Habte, Aron Friedman, Daniel J. TI Optimization of Multijunction Solar Cells Through Indoor Energy Yield Measurements SO IEEE JOURNAL OF PHOTOVOLTAICS LA English DT Article DE Energy yield; luminescence coupling (LC); multijunction solar cell; variable spectrum ID IRRADIANCE; JUNCTION AB The variability of the solar spectra in the fieldmay reduce the annual energy yield of multijunction solar cells. It would, therefore, be desirable to implement a cell design procedure based on the maximization of the annual energy yield. In this study, we present a measurement technique to generate maps of the real performance of the solar cell for a range of light spectrum contents using a solar simulator with a computer-controllable spectral content. These performance maps are demonstrated to be a powerful tool for analyzing the characteristics of any given set of annual spectra representative of a site and their influence on the energy yield of any solar cell. The effect of luminescence coupling on buffering against variations of the spectrum and improving the annual energy yield is demonstrated using this method. C1 [Garcia, Ivan] Univ Politecn Madrid, Inst Energia Solar, E-28040 Madrid, Spain. [Garcia, Ivan; McMahon, William E.; Steiner, Myles A.; Geisz, John F.; Habte, Aron; Friedman, Daniel J.] Natl Renewable Energy Lab, Golden, CO 80401 USA. RP Garcia, I (reprint author), Univ Politecn Madrid, Inst Energia Solar, E-28040 Madrid, Spain. EM igarcia@ies-def.upm.es; bill.mcmahon@nrel.gov; myles.steiner@nrel.gov; john.geisz@nrel.gov; aron.habte@nrel.gov; daniel.friedman@nrel.gov FU U.S. Department of Energy [DE-AC36-08-GO28308]; National Renewable Energy Laboratory; IOF from People Program (Marie Curie Actions) of the European Union [FP7/2007-20a13, 299878] FX This work was supported by the U.S. Department of Energy under Contract DE-AC36-08-GO28308 with the National Renewable Energy Laboratory. The work of I. Garcia was supported by an IOF grant from the People Program (Marie Curie Actions) of the European Union's Seventh Framework Program (FP7/2007-20a13) under REA Grant 299878. NR 16 TC 5 Z9 5 U1 1 U2 5 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 2156-3381 J9 IEEE J PHOTOVOLT JI IEEE J. Photovolt. PD JAN PY 2015 VL 5 IS 1 BP 438 EP 445 DI 10.1109/JPHOTOV.2014.2364128 PG 8 WC Energy & Fuels; Materials Science, Multidisciplinary; Physics, Applied SC Energy & Fuels; Materials Science; Physics GA AX1WA UT WOS:000346732700066 ER PT J AU Abdalah, M Boutchko, R Mitra, D Gullberg, GT AF Abdalah, Mahmoud Boutchko, Rostyslav Mitra, Debasis Gullberg, Grant T. TI Reconstruction of 4-D Dynamic SPECT Images From Inconsistent Projections Using a Spline Initialized FADS Algorithm (SIFADS) SO IEEE TRANSACTIONS ON MEDICAL IMAGING LA English DT Article DE Dynamic single photon emission computed tomography (SPECT); image reconstruction; optimization; regularization ID EMISSION-TOMOGRAPHY; SPATIOTEMPORAL DISTRIBUTIONS; SEGMENTATION; REGULARIZATION; MAXIMUM; PHANTOM AB In this paper, we propose and validate an algorithm of extracting voxel-by-voxel time activity curves directly from inconsistent projections applied in dynamic cardiac SPECT. The algorithm was derived based on factor analysis of dynamic structures (FADS) approach and imposes prior information by applying several regularization functions with adaptively changing relative weighting. The anatomical information of the imaged subject was used to apply the proposed regularization functions adaptively in the spatial domain. The algorithm performance is validated by reconstructing dynamic datasets simulated using the NCAT phantom with a range of different input tissue time-activity curves. The results are compared to the spline-based and FADS methods. The validated algorithm is then applied to reconstruct pre-clinical cardiac SPECT data from canine and murine subjects. Images, generated from both simulated and experimentally acquired data confirm the ability of the new algorithm to solve the inverse problem of dynamic SPECT with slow gantry rotation. C1 [Abdalah, Mahmoud; Mitra, Debasis] Florida Inst Technol, Dept Comp Sci, Melbourne, FL 32901 USA. [Boutchko, Rostyslav; Gullberg, Grant T.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Abdalah, M (reprint author), Florida Inst Technol, Dept Comp Sci, Melbourne, FL 32901 USA. EM mabdalah2009@my.fit.edu FU National Institute of Biomedical Imaging and Bioengineering [R01EB00121]; Heart, Lung, and Blood Institute of the National Institutes of Health [R01HL50663]; Office of Science, Office of Biological and Environmental Research, Medical Sciences Division of the U.S. Department of Energy [DE-AC02-05CH11231] FX This work was supported in part by the National Institute of Biomedical Imaging and Bioengineering under Grant R01EB00121, in part by the Heart, Lung, and Blood Institute of the National Institutes of Health under Grant R01HL50663, and in part by the Director, Office of Science, Office of Biological and Environmental Research, Medical Sciences Division of the U.S. Department of Energy under Contract DE-AC02-05CH11231. Asterisk indicates corresponding author. NR 36 TC 3 Z9 3 U1 0 U2 4 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 0278-0062 EI 1558-254X J9 IEEE T MED IMAGING JI IEEE Trans. Med. Imaging PD JAN PY 2015 VL 34 IS 1 BP 216 EP 228 DI 10.1109/TMI.2014.2352033 PG 13 WC Computer Science, Interdisciplinary Applications; Engineering, Biomedical; Engineering, Electrical & Electronic; Imaging Science & Photographic Technology; Radiology, Nuclear Medicine & Medical Imaging SC Computer Science; Engineering; Imaging Science & Photographic Technology; Radiology, Nuclear Medicine & Medical Imaging GA AX5OJ UT WOS:000346975900021 PM 25167546 ER PT J AU Mousavian, S Valenzuela, J Wang, JH AF Mousavian, Seyedamirabbas Valenzuela, Jorge Wang, Jianhui TI A Probabilistic Risk Mitigation Model for Cyber-Attacks to PMU Networks SO IEEE TRANSACTIONS ON POWER SYSTEMS LA English DT Article DE Cyber-attack; cyber-security; networks; observability; phasor measurement units ID DEFENSE; SIMULATION; PLACEMENT AB The power grid is becoming more dependent on information and communication technologies. Complex networks of advanced sensors such as phasor measurement units (PMUs) are used to collect real time data to improve the observability of the power system. Recent studies have shown that the power grid has significant cyber vulnerabilities which could increase when PMUs are used extensively. Therefore, recognizing and responding to vulnerabilities are critical to the security of the power grid. This paper proposes a risk mitigation model for optimal response to cyber-attacks to PMU networks. We model the optimal response action as a mixed integer linear programming (MILP) problem to prevent propagation of the cyber-attacks and maintain the observability of the power system. C1 [Mousavian, Seyedamirabbas; Valenzuela, Jorge] Auburn Univ, Dept Ind & Syst Engn, Auburn, AL 36849 USA. [Wang, Jianhui] Argonne Natl Lab, Argonne, IL 60439 USA. RP Mousavian, S (reprint author), Auburn Univ, Dept Ind & Syst Engn, Auburn, AL 36849 USA. EM amir@auburn.edu; valenjo@auburn.edu; jianhui.wang@anl.gov FU UChicago Argonne, LLC; [DE-AC02-06CH11357] FX This work was supported by UChicago Argonne, LLC, Operator of Argonne National Laboratory (Argonne). Argonne, a U.S. Department of Energy Office of Science laboratory, is operated under Contract No. DE-AC02-06CH11357. Paper no. TPWRS-00883-2013. NR 31 TC 4 Z9 5 U1 0 U2 3 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 0885-8950 EI 1558-0679 J9 IEEE T POWER SYST JI IEEE Trans. Power Syst. PD JAN PY 2015 VL 30 IS 1 BP 156 EP 165 DI 10.1109/TPWRS.2014.2320230 PG 10 WC Engineering, Electrical & Electronic SC Engineering GA AX1WM UT WOS:000346734000015 ER PT J AU Zhou, N Dagle, J AF Zhou, Ning Dagle, Jeff TI Initial Results in Using a Self-Coherence Method for Detecting Sustained Oscillations SO IEEE TRANSACTIONS ON POWER SYSTEMS LA English DT Article DE Coherence; oscillations; phasor measurement unit (PMU); power spectral density; power system dynamics ID ELECTROMECHANICAL OSCILLATIONS; POWER-SYSTEMS; IDENTIFICATION AB This paper develops a self-coherence method for detecting sustained oscillations using phasor measurement unit (PMU) data. Sustained oscillations decrease system performance and introduce potential reliability issues. Timely detection of the oscillations at an early stage provides the opportunity for taking remedial reaction. Using high-speed time-synchronized PMU data, this paper details a self-coherence method for detecting sustained oscillation, even when the oscillation amplitude is lower than ambient noise. Simulation and field measurement data are used to evaluate the proposed method's performance. It is shown that the proposed method can detect sustained oscillations and estimate oscillation frequencies with a low signal-to-noise ratio. Comparison with a power spectral density method also shows that the proposed self-coherence method performs better. C1 [Zhou, Ning] SUNY Binghamton, Binghamton, NY 13902 USA. [Dagle, Jeff] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Zhou, N (reprint author), SUNY Binghamton, Binghamton, NY 13902 USA. EM ningzhou@binghamton.edu; jeff.dagle@pnnl.gov FU U.S. Department of Energy (DOE) through its Consortium for Electric Reliability Technology Solutions (CERTS) Program; Bonneville Power Administration; DOE [DE-AC05-76RL01830] FX This paper was prepared as a result of work sponsored by the U.S. Department of Energy (DOE) through its Consortium for Electric Reliability Technology Solutions (CERTS) Program. This work was supported by the Bonneville Power Administration. Pacific Northwest National Laboratory (PNNL) is operated by Battelle for DOE under contract DE-AC05-76RL01830. Paper no. TPWRS-00014-2014. NR 18 TC 5 Z9 5 U1 0 U2 4 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 0885-8950 EI 1558-0679 J9 IEEE T POWER SYST JI IEEE Trans. Power Syst. PD JAN PY 2015 VL 30 IS 1 BP 522 EP 530 DI 10.1109/TPWRS.2014.2321225 PG 9 WC Engineering, Electrical & Electronic SC Engineering GA AX1WM UT WOS:000346734000051 ER PT J AU Liu, C Lee, C Shahidehpour, M AF Liu, Cong Lee, Changhyeok Shahidehpour, Mohammad TI Look Ahead Robust Scheduling of Wind-Thermal System With Considering Natural Gas Congestion SO IEEE TRANSACTIONS ON POWER SYSTEMS LA English DT Article DE Natural gas electric coordination; renewable energy; robust optimization; unit commitment AB Natural gas pipeline congestion will impact on the fuel adequacy of several natural gas fired generating units at the same time. This letter focuses on the development of a robust optimization methodology for the scheduling of quick start units when considering natural gas resource availability constraints. Natural gas transmission will be approximated by linear constraints, and the linepack capacity of pipelines will be considered in the proposed model. Case studies show the effectiveness of the proposed model and algorithms. C1 [Liu, Cong] Argonne Natl Lab, Argonne, IL 60439 USA. [Lee, Changhyeok] Northwestern Univ, Evanston, IL 60208 USA. [Shahidehpour, Mohammad] IIT, Chicago, IL 60616 USA. RP Liu, C (reprint author), Argonne Natl Lab, 9700 S Cass Ave, Argonne, IL 60439 USA. FU U.S. Department of Energy Office of Science laboratory [DE-AC02-06CH11357]; U.S. Department of Energy, Office of Electricity Delivery and Energy FX The submitted manuscript has been created by UChicago Argonne, LLC, Operator of Argonne National Laboratory ("Argonne"). Argonne, a U.S. Department of Energy Office of Science laboratory, is operated under Contract No. DE-AC02-06CH11357. This work was supported by the U.S. Department of Energy, Office of Electricity Delivery and Energy. Paper no. PESL-00135-2013. NR 7 TC 2 Z9 2 U1 2 U2 7 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 0885-8950 EI 1558-0679 J9 IEEE T POWER SYST JI IEEE Trans. Power Syst. PD JAN PY 2015 VL 30 IS 1 BP 544 EP 545 DI 10.1109/TPWRS.2014.2326981 PG 2 WC Engineering, Electrical & Electronic SC Engineering GA AX1WM UT WOS:000346734000055 ER PT J AU Carter, JLW Genau, AL Schneider, J Unocic, K Yablinsky, CA Robinson, L AF Carter, Jennifer L. W. Genau, Amber L. Schneider, Judy Unocic, Kinga Yablinsky, Clarissa A. Robinson, Lynne TI DMMM1 Builds on the Strength in Diversity SO JOM LA English DT News Item C1 [Carter, Jennifer L. W.] Case Western Reserve Univ, Dept Mat Sci & Engn, Cleveland, OH 44106 USA. [Genau, Amber L.] Univ Alabama, Tuscaloosa, AL 35487 USA. [Schneider, Judy] Mississippi State Univ, Dept Mech Engn, Mississippi State, MS USA. [Unocic, Kinga] Oak Ridge Natl Lab, Oak Ridge, TN USA. [Yablinsky, Clarissa A.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Carter, JLW (reprint author), Case Western Reserve Univ, Dept Mat Sci & Engn, Cleveland, OH 44106 USA. RI Carter, Jennifer/A-3241-2013; OI Carter, Jennifer/0000-0001-6702-729X; Yablinsky, Clarissa/0000-0001-6162-0949 NR 0 TC 0 Z9 0 U1 0 U2 2 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1047-4838 EI 1543-1851 J9 JOM-US JI JOM PD JAN PY 2015 VL 67 IS 1 BP 13 EP 20 DI 10.1007/s11837-014-1255-x PG 8 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering; Mineralogy; Mining & Mineral Processing SC Materials Science; Metallurgy & Metallurgical Engineering; Mineralogy; Mining & Mineral Processing GA AX8JE UT WOS:000347155100003 ER PT J AU Yan, AD Poole, ZL Chen, RZ Leu, PW Ohodnicki, P Chen, KP AF Yan, Aidong Poole, Zsolt L. Chen, Rongzhang Leu, Paul W. Ohodnicki, Paul Chen, Kevin P. TI Scalable Fabrication of Metal Oxide Functional Materials and Their Applications in High-Temperature Optical Sensing SO JOM LA English DT Article ID GAS SENSOR; HYDROGEN SENSOR; FIBER; NANOSTRUCTURES AB We report a scalable manufacturing approach to produce nano-porous metal oxide films and the dopant variants using a block-copolymer template combined with a sol-gel solution processing approach. The refractive index of the film can be tailored to 1.2-2.4 by 3D nanostructuring in the sub-wavelength regime at scales of 20 nm or less. Based on this approach, this paper reports the synthesis of nanoporous palladium (Pd)-doped titanium dioxide (TiO2) film with refractive index matching the optical fiber material, and its importance on D-shaped fiber Bragg grating for hydrogen sensing at extremely high temperature up to 700A degrees C. The sensor is based on evanescent field interaction in hydrogen-sensitive cladding. The flat side of D-shaped fiber grating was etched to remove a residual 4 mu m cladding material, and thermally stabilized for high-temperature requirements. The peak intensity change of the fiber Bragg wavelength was observed with different hydrogen concentrations from 0.25 vol.% H-2/N-2 to 5 vol.% H-2/N-2. The experimental result shows that the sensor's hydrogen response is reversible and fast. The response time of the hydrogen sensor is < 8 s. C1 [Yan, Aidong; Poole, Zsolt L.; Chen, Rongzhang; Chen, Kevin P.] Univ Pittsburgh, Dept Elect & Comp Engn, Pittsburgh, PA 15261 USA. [Leu, Paul W.] Univ Pittsburgh, Dept Ind Engn, Pittsburgh, PA 15261 USA. [Ohodnicki, Paul] Natl Energy Technol Lab, Pittsburgh, PA 15236 USA. RP Yan, AD (reprint author), Univ Pittsburgh, Dept Elect & Comp Engn, Pittsburgh, PA 15261 USA. EM pec9@pitt.edu RI Leu, Paul/B-9989-2008; Chen, Rongzhang/B-7259-2017 OI Leu, Paul/0000-0002-1599-7144; Chen, Rongzhang/0000-0003-4582-2983 FU National Science Foundation [CMMI-1300273, CMMI-1348591]; Department of Energy [DE-FE0003859] FX This work was supported by the National Science Foundation (CMMI-1300273, CMMI-1348591) and the Department of Energy (DE-FE0003859). This report was prepared as an account of work sponsored by an agency of the United States Government. Neither the United States Government nor any agency thereof, nor any of their employees, makes any warranty, express or implied, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. Reference herein to any specific commercial product, process, or service by trade name, trademark, manufacturer, or otherwise does not necessarily constitute or imply its endorsement, recommendation, or favoring by the United States Government or any agency thereof. The views and opinions of authors expressed herein do not necessarily state or reflect those of the United States Government or any agency thereof. NR 23 TC 2 Z9 2 U1 4 U2 30 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1047-4838 EI 1543-1851 J9 JOM-US JI JOM PD JAN PY 2015 VL 67 IS 1 BP 53 EP 58 DI 10.1007/s11837-014-1235-1 PG 6 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering; Mineralogy; Mining & Mineral Processing SC Materials Science; Metallurgy & Metallurgical Engineering; Mineralogy; Mining & Mineral Processing GA AX8JE UT WOS:000347155100011 ER PT J AU Dryepondt, S Jones, SJ Zhang, Y Maziasz, PJ Pint, BA AF Dryepondt, Sebastien Jones, Samuel J. Zhang, Ying Maziasz, Phillip J. Pint, Bruce A. TI Oxidation, Creep and Fatigue Properties of Bare and Coated 31V Alloy SO JOM LA English DT Article ID PROTECTIVE-COATINGS; ALUMINIDE COATINGS; MECHANICAL-PROPERTIES; SUPERALLOY; BEHAVIOR AB Increasing the efficiency of natural gas reciprocating engines will require materials with better mechanical and corrosion resistance at high temperatures. One solution to increase the lifetime of exhaust valves is to apply an aluminide coating to prevent corrosion assisted fatigue cracking, but the impact of the coating on the valve material mechanical properties needs to be assessed. In addition to cyclic oxidation testing in dry and humid air at 800A degrees C, creep and high cycle fatigue (HCF) testing were conducted at 816A degrees C on bare and slurry or pack-coated 31V alloy. The coated and bare creep specimens exhibited very similar creep rupture lives, as long as the specimens were annealed according to the 31V standard heat treatment before testing. The HCF behavior of the pack-coated alloy was close to the behavior of the bare alloy, but fatigue lifetimes of slurry-coated 31V specimens had higher variability. Aluminide coatings have the potential to improve the valve performance at high temperature, but the coating deposition process needs to be tailored for the substrate standard heat treatment. C1 [Dryepondt, Sebastien; Jones, Samuel J.; Maziasz, Phillip J.; Pint, Bruce A.] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. [Zhang, Ying] Tennessee Technol Univ, Cookeville, TN 38505 USA. RP Dryepondt, S (reprint author), Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. EM dryepondtsn@ornl.gov RI Pint, Bruce/A-8435-2008 OI Pint, Bruce/0000-0002-9165-3335 FU U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Advanced Manufacturing Office FX The authors wish to thank Kevin Hantak at TWR Engine Components for providing the 31V creep and fatigue specimens. They also acknowledge G. Garner, J. Moser, T.L. Jordan, D. McClurg, C.S. Hawkins, D.L. Erdman III, D. Leonard and B.L. Bates for assistance with the experimental work, as well as A. Shyamand D.F. Wilson for reviewing the manuscript. This research was sponsored by the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Advanced Manufacturing Office. NR 23 TC 0 Z9 0 U1 0 U2 10 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1047-4838 EI 1543-1851 J9 JOM-US JI JOM PD JAN PY 2015 VL 67 IS 1 BP 68 EP 76 DI 10.1007/s11837-014-1240-4 PG 9 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering; Mineralogy; Mining & Mineral Processing SC Materials Science; Metallurgy & Metallurgical Engineering; Mineralogy; Mining & Mineral Processing GA AX8JE UT WOS:000347155100014 ER PT J AU Bomberg, M Gibson, M Zhang, J AF Bomberg, Mark Gibson, Michael Zhang, Jian TI A concept of integrated environmental approach for building upgrades and new construction: Part 1-setting the stage SO JOURNAL OF BUILDING PHYSICS LA English DT Article DE Building physics; building science; history of building physics; system integration; thermal upgrade; thermal rehabilitation; ventilated cavities in multi-layered walls; hygrothermal insulations ID ENERGY PERFORMANCE; METHODOLOGY; ENCLOSURES AB This article highlights the need for an active role for building physics in the development of near-zero energy buildings while analyzing an example of an integrated system for the upgrade of existing buildings. The science called either Building Physics in Europe or Building Science in North America has so far a passive role in explaining observed failures in construction practice. In its new role, it would be integrating modeling and testing to provide predictive capability, so much needed in the development of near-zero energy buildings. The authors attempt to create a compact package, applicable to different climates with small modifications of some hygrothermal properties of materials. This universal solution is based on a systems approach that is routine for building physics but in contrast to separately conceived sub-systems that are typical for the design of buildings today. One knows that the building structure, energy efficiency, indoor environmental quality, and moisture management all need to be considered to ensure durability of materials and control cost of near-zero energy buildings. These factors must be addressed through contributions of the whole design team. The same approach must be used for the retrofit of buildings. As this integrated design paradigm resulted from demands of sustainable built environment approach, building physics must drop its passive role and improve two critical domains of analysis: (i) linked, real-time hygrothermal and energy models capable of predicting the performance of existing buildings after renovation and (ii) basic methods of indoor environment and moisture management when the exterior of the building cannot be modified. C1 [Bomberg, Mark] McMaster Univ, Hamilton, ON L8S 4L8, Canada. [Bomberg, Mark] Southeast Univ, Nanjing, Jiangsu, Peoples R China. [Gibson, Michael] Kansas State Univ, Dept Architecture, Manhattan, KS 66506 USA. [Zhang, Jian] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Bomberg, M (reprint author), McMaster Univ, 1280 Main St West, Hamilton, ON L8S 4L8, Canada. EM mark.bomberg@gmail.com NR 61 TC 4 Z9 4 U1 2 U2 15 PU SAGE PUBLICATIONS LTD PI LONDON PA 1 OLIVERS YARD, 55 CITY ROAD, LONDON EC1Y 1SP, ENGLAND SN 1744-2591 EI 1744-2583 J9 J BUILD PHYS JI J. Build Phys. PD JAN PY 2015 VL 38 IS 4 BP 360 EP 385 DI 10.1177/1744259114553728 PG 26 WC Construction & Building Technology SC Construction & Building Technology GA AX5WG UT WOS:000346994900005 ER PT J AU Wang, J Xin, HLL Zhu, J Liu, SF Wu, ZX Wang, DL AF Wang, Jie Xin, Huolin L. Zhu, Jing Liu, Sufen Wu, Zexing Wang, Deli TI 3D hollow structured Co2FeO4/MWCNT as an efficient non-precious metal electrocatalyst for oxygen reduction reaction SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID LITHIUM-ION BATTERIES; MEMBRANE FUEL-CELLS; NITROGEN-DOPED GRAPHENE; SYNERGISTIC CATALYST; CARBON CORROSION; NANOPARTICLES; ELECTRODES; CO3O4; HYBRID; NANOCRYSTALS AB A template- and surfactant-free strategy is developed to prepare a hollow structured Co2FeO4/MWCNT electrocatalyst, which has been successfully used as a highly efficient non-precious metal electrocatalyst for the oxygen reduction reaction (ORR) in alkaline media. The hollow structured Co2FeO4 particles are transformed from solid Co2Fe nanoparticles via the Kirkendall effect, which increases their active sites and improves the contact between the electrolyte and catalyst surfaces and then enhances the electrocatalytic activity. Furthermore, the hollow structured Co2FeO4/MWCNT exhibits excellent Long term stability and high methanol tolerance compared to commercial Pt/C. The hollow structured Co2FeO4/MWCNT electrocatalysts synthesized herein are promising electrode materials for fuel cell applications and the facile synthesis method could be used in low-cost and Large-scale materials production, facilitating the screening of high efficiency catalysts. C1 [Wang, Jie; Zhu, Jing; Liu, Sufen; Wu, Zexing; Wang, Deli] Huazhong Univ Sci & Technol, Key Lab Large Format Battery Mat & Syst, Minist Educ, Sch Chem & Chem Engn, Wuhan 430074, Peoples R China. [Xin, Huolin L.] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. RP Wang, DL (reprint author), Huazhong Univ Sci & Technol, Key Lab Large Format Battery Mat & Syst, Minist Educ, Sch Chem & Chem Engn, Wuhan 430074, Peoples R China. EM wangdl81125@hust.edu.cn RI Wang, Deli/K-5029-2012; Wang, Jie/H-3638-2015; Xin, Huolin/E-2747-2010 OI Wang, Jie/0000-0002-7188-3053; Xin, Huolin/0000-0002-6521-868X FU National Natural Science Foundation [21306060]; Program for New Century Excellent Talents in Universities of China [NCET-13-0237]; Ministry of Education of China [20130142120039]; Fundamental Research Funds for the Central University [2013TS136, 2014YQ009]; U.S. Department of Energy, Office of Basic Energy Sciences [DE-AC02-98CH10886] FX This work was supported by the National Natural Science Foundation (21306060), the Program for New Century Excellent Talents in Universities of China (NCET-13-0237), the Doctoral Fund of Ministry of Education of China (20130142120039), the Fundamental Research Funds for the Central University (2013TS136, 2014YQ009). We thank Analytical and Testing Center of Huazhong University of Science & Technology for allowing us to use its facilities. S/TEM and EELS work was carried out at the Center for Functional Nanomaterials, Brookhaven National Laboratory, which is supported by the U.S. Department of Energy, Office of Basic Energy Sciences, under Contract No. DE-AC02-98CH10886. We also thank Mr. Shaolei Wang in Prof. Tan's group for the BET measurement. NR 51 TC 13 Z9 13 U1 6 U2 85 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7488 EI 2050-7496 J9 J MATER CHEM A JI J. Mater. Chem. A PY 2015 VL 3 IS 4 BP 1601 EP 1608 DI 10.1039/c4ta06265e PG 8 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA AX4MH UT WOS:000346906100031 ER PT J AU Wang, Z Beletskiy, EV Lee, S Hou, XL Wu, YY Li, TH Kung, MC Kung, HH AF Wang, Zhen Beletskiy, Evgeny V. Lee, Sungsik Hou, Xianliang Wu, Yuyang Li, Tiehu Kung, Mayfair C. Kung, Harold H. TI Amine-functionalized siloxane oligomer facilitated synthesis of subnanometer colloidal Au particles SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID PROTECTED GOLD CLUSTERS; ONE-POT PREPARATION; NANOPARTICLE SYNTHESIS; CRYSTAL-STRUCTURE; MONOLAYER; WATER; ACID; HYDROGENATION; COMPLEXES; MOLECULES AB Amine-functionalized siloxane oligomers were synthesized and used successfully to prepare colloidal Au particles smaller than 1 nm. Using NMR to follow the interaction of Au(THT)Cl with the functionalized siloxane, it was determined that the amine ligands displaced the THT ligand effectively. By comparison with other functionalized siloxane oligomers/compound, parameters such as density of ligating groups, oligomer steric barrier and reduction rates were found to be essential for the formation and stability of subnanometer Au particles. Without further treatment, the formed Au particles were active catalysts for the reduction of p-nitrobenzaldehyde by triethylsilane, forming an imine as the major coupling product. Deposition of the Au colloids onto silica, followed by thermal treatment to remove the organic groups resulted in subnanometer Au on silica, indicating this to be a promising method of fabricating subnanometer supported Au catalyst. C1 [Wang, Zhen; Beletskiy, Evgeny V.; Hou, Xianliang; Kung, Mayfair C.; Kung, Harold H.] Northwestern Univ, Chem & Biol Engn Dept, Evanston, IL 60208 USA. [Wang, Zhen; Hou, Xianliang; Li, Tiehu] Northwestern Polytech Univ, Sch Mat Sci & Engn, Xian 710072, Shaanxi, Peoples R China. [Lee, Sungsik] Argonne Natl Lab, Xray Sci Div, Argonne, IL 60439 USA. [Wu, Yuyang] Northwestern Univ, Dept Chem, Evanston, IL 60208 USA. RP Kung, MC (reprint author), Northwestern Univ, Chem & Biol Engn Dept, Evanston, IL 60208 USA. EM m-kung@northwestern.edu; hkung@northwestern.edu RI Kung, Harold/B-7647-2009; Kung, Mayfair/B-7648-2009 FU Department of Energy, Basic Energy Sciences [DE-FG02-01ER15184]; China Scholarship Council; DOE Office of Science by Argonne National Laboratory [DE-AC02-06CH11357] FX This work was supported by the Department of Energy, Basic Energy Sciences, grant no. DE-FG02-01ER15184. Z. W. and X. H. acknowledge funding support from China Scholarship Council. This work made use of the TEM and NMR in the EPIC facility of NUANCE Center and IMSERC facility at Northwestern University. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract no. DE-AC02-06CH11357. NR 46 TC 1 Z9 1 U1 3 U2 32 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7488 EI 2050-7496 J9 J MATER CHEM A JI J. Mater. Chem. A PY 2015 VL 3 IS 4 BP 1743 EP 1751 DI 10.1039/c4ta05954a PG 9 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA AX4MH UT WOS:000346906100050 ER PT J AU Li, XF Budai, JD Liu, F Chen, YS Howe, JY Sun, CJ Tischler, JZ Meltzer, RS Pan, ZW AF Li, Xufan Budai, John D. Liu, Feng Chen, Yu-Sheng Howe, Jane Y. Sun, Chengjun Tischler, Jonathan Z. Meltzer, Richard S. Pan, Zhengwei TI Crystal structures and optical properties of new quaternary strontium europium aluminate luminescent nanoribbons SO JOURNAL OF MATERIALS CHEMISTRY C LA English DT Article ID LED CONVERSION PHOSPHORS; NANOWIRE PHOTONICS; WAVE-GUIDES; LARGE-SCALE; PHOTOLUMINESCENCE; HETEROSTRUCTURES; NANOPHOTONICS; FLUORESCENCE; MULTICOLOR; SCIENCE AB We report the synthesis and characterization of three series of new quaternary strontium europium aluminate (Sr-Eu-Al-O; SEAO) luminescent nanoribbons that show blue, green, and yellow luminescence from localized Eu2+ luminescent centers. These three series of SEAO nanoribbons are: blue luminescent, tetragonal Sr1-xEuxAl6O10 (0 < x < 1) (b-SEAO), green luminescent, monoclinic Sr1-xEuxAl2O4 (0 < x < 1) (g-SEAO), and yellow luminescent, hexagonal Sr1-xEuxAl2O4 (0 < x < 1) (y-SEAO). Among these three series of SEAO nanoribbons, the b-SEAOs and y-SEAOs are new compounds that have not been reported before. The crystal structures of the SEAO nanoribbons were comprehensively studied using various synchrotron X-ray diffraction techniques and the effects of crystal structures on materials' luminescence properties were investigated. These one-dimensional SEAO luminescent nanoribbons can function as both light generators and waveguides, and thus have promising potential as the building blocks in miniaturized photonic circuitry. C1 [Li, Xufan; Liu, Feng; Pan, Zhengwei] Univ Georgia, Coll Engn, Athens, GA 30602 USA. [Li, Xufan; Liu, Feng; Pan, Zhengwei] Univ Georgia, Dept Phys & Astron, Athens, GA 30602 USA. [Budai, John D.; Howe, Jane Y.] Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. [Chen, Yu-Sheng] Univ Chicago, ChemMatCARS, Argonne, IL 60439 USA. [Sun, Chengjun] Argonne Natl Lab, Xray Sci Div, Argonne, IL 60439 USA. [Tischler, Jonathan Z.] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. RP Pan, ZW (reprint author), Univ Georgia, Coll Engn, Athens, GA 30602 USA. EM budaijd@ornl.gov; panz@uga.edu RI Li, Xufan/A-8292-2013; Budai, John/R-9276-2016; OI Li, Xufan/0000-0001-9814-0383; Budai, John/0000-0002-7444-1306; Pan, Zhengwei/0000-0002-3854-958X FU US National Science Foundation (NSF) [DMR-0955908]; Materials Sciences and Engineering Division, Office of Basic Energy Sciences (BES), U.S. Department of Energy (DOE); U.S. DOE [DE-AC02-06CH11357]; Argonne National Laboratory; Divisions of Chemistry and Materials Research, NSF [NSF/CHE-1346572]; Division of Scientific User Facilities of BES, U.S. DOE FX Z.W.P. acknowledges the funding support from the US National Science Foundation (NSF, DMR-0955908). J.D.B. was supported by the Materials Sciences and Engineering Division, Office of Basic Energy Sciences (BES), U.S. Department of Energy (DOE). The use of the APS beamlines 34-ID-E and 11-BM-B (by J.D.B. and J.Z.T.), ChemMatCARS Sector 15 (by Y.S.C. and J.D.B.) and 20-BM-B (by C.J.S.) were supported by U.S. DOE under Contract no. DE-AC02-06CH11357 with Argonne National Laboratory. ChemMatCARS Sector 15 is principally supported by the Divisions of Chemistry and Materials Research, NSF, under grant number NSF/CHE-1346572. The TEM characterization (by J.Y.H.) was conducted at the Oak Ridge National Laboratory ShaRE User Facilities, which is sponsored by the Division of Scientific User Facilities of BES, U.S. DOE. NR 45 TC 1 Z9 1 U1 2 U2 24 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7526 EI 2050-7534 J9 J MATER CHEM C JI J. Mater. Chem. C PY 2015 VL 3 IS 4 BP 778 EP 788 DI 10.1039/c4tc02002b PG 11 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA AX9NL UT WOS:000347229200010 ER PT J AU Wilding, MC Wilson, M McMillan, PF Benmore, CJ Weber, JKR Deschamps, T Champagnon, B AF Wilding, Martin C. Wilson, Mark McMillan, Paul F. Benmore, Chris J. Weber, J. K. R. Deschamps, Thierry Champagnon, Bernard TI Structural properties of Y2O3-Al2O3 liquids and glasses: An overview SO JOURNAL OF NON-CRYSTALLINE SOLIDS LA English DT Article; Proceedings Paper CT 7th International Discussion Meeting on Relaxations in Complex Systems (IDMRCS) CY JUL 21-26, 2013 CL Univ Politecnica Catalunya, Barcelona, SPAIN SP Energia Campus Int Excellence, Barcelona Knowledge Campus, Inst Laue Langevin, Julich Forschungszentrum, CNRS, Lab Leon Brillouin, Int Dielectr Soc, AirLiquide, Almirall, Bruker, Extrasolution, Matgas, Mettler Toledo, Novocontrol Technologies, TA Instruments, Polish Acad Sci, Inst High Pressure Phys HO Univ Politecnica Catalunya DE Polyamorphism; Liquid structure; X-ray diffraction; Container less techniques; Raman spectroscopy ID PRESSURE MOLECULAR-DYNAMICS; RAMAN-SPECTROSCOPY; PHASE-TRANSITIONS; ALUMINATE LIQUIDS; SINGLE-PHASE; X-RAY; YTTRIUM; SIMULATION; SILICATE; DENSITY AB Liquids in the system Y2O3- Al2O3 have been the subject of considerable study because of the reported occurrence of a first-order density and entropy-driven liquid-liquid phase transition (LLPT) in the supercooled liquid state. The observations have become controversial because of the presence of crystalline material that can be formed simultaneously and that can mask the nucleation and growth of the lower density liquid. The previous work is summarized here along with arguments for and against the different viewpoints. Also two studies have been undertaken to investigate the LLPT in this refractory system with emphasis on determining the structure of unequivocally amorphous materials. These include the in situ high energy X-ray diffraction (HEXRD) of supercooled Y2O3 - Al2O3 liquids and the low frequency vibrational dynamics of recovered glasses. Manybody molecular dynamics simulations are also used to interpret the results of both studies. The HEXRD measurements, combined with aerodynamic levitation and rapid data acquisition techniques, show that for the 20 mol% Y2O3 (i.e. AlY20) liquid there is a shift in the position of the first peak in the diffraction pattern over a narrow temperature range (2100-1800 K) prior to crystallization. Microbeam Raman spectroscopy measurements made on AlY20 glasses clearly show contrasting spectra in the low frequency part of the spectrum for low(LDA) and high-density (HDA) glassy regions. The molecular dynamics simulations identify contrasting coordination environments around oxygen anions for the high- (HDL) and low-density (LDL) liquids. (C) 2014 Elsevier B.V. All rights reserved. C1 [Wilding, Martin C.] Aberystwyth Univ, Inst Math & Phys Sci, Aberystwyth SY23 3BZ, Dyfed, Wales. [Wilson, Mark] Univ Oxford, Dept Chem, Phys & Theoret Chem Lab, Oxford OX1 3QZ, England. [McMillan, Paul F.] UCL, Dept Chem, London WC1H 0AJ, England. [Benmore, Chris J.] Argonne Natl Lab, Adv Photon Source, Xray Sci Div, Argonne, IL 60439 USA. [Weber, J. K. R.] Mat Dev Inc, Arlington Hts, WA 6004, Australia. [Deschamps, Thierry] Univ Lyon, CNRS, Ecole Ctr Lyon, Inst Nanotechnol Lyon INL UMR5270, F-69134 Ecully, France. [Champagnon, Bernard] Univ Lyon 1, CNRS, Inst Lumiere Matiere, UMR5306, F-69622 Villeurbanne, France. RP Wilding, MC (reprint author), Aberystwyth Univ, Inst Math & Phys Sci, Aberystwyth SY23 3BZ, Dyfed, Wales. EM mbw@aber.ac.uk; mark.wilson@chem.ox.ac.uk OI Benmore, Chris/0000-0001-7007-7749 NR 44 TC 1 Z9 1 U1 7 U2 45 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0022-3093 EI 1873-4812 J9 J NON-CRYST SOLIDS JI J. Non-Cryst. Solids PD JAN 1 PY 2015 VL 407 SI SI BP 228 EP 234 DI 10.1016/j.jnoncrysol.2014.09.044 PG 7 WC Materials Science, Ceramics; Materials Science, Multidisciplinary SC Materials Science GA AX6FJ UT WOS:000347018300033 ER PT J AU Russina, O Macchiagodena, M Kirchner, B Mariani, A Aoun, B Russina, M Caminiti, R Triolo, A AF Russina, Olga Macchiagodena, Marina Kirchner, Barbara Mariani, Alessandro Aoun, Bachir Russina, Margarita Caminiti, Ruggero Triolo, Alessandro TI Association in ethylammonium nitrate-dimethyl sulfoxide mixtures: First structural and dynamical evidences SO JOURNAL OF NON-CRYSTALLINE SOLIDS LA English DT Article; Proceedings Paper CT 7th International Discussion Meeting on Relaxations in Complex Systems (IDMRCS) CY JUL 21-26, 2013 CL Univ Politecnica Catalunya, Barcelona, SPAIN SP Energia Campus Int Excellence, Barcelona Knowledge Campus, Inst Laue Langevin, Julich Forschungszentrum, CNRS, Lab Leon Brillouin, Int Dielectr Soc, AirLiquide, Almirall, Bruker, Extrasolution, Matgas, Mettler Toledo, Novocontrol Technologies, TA Instruments, Polish Acad Sci, Inst High Pressure Phys HO Univ Politecnica Catalunya DE Protic ionic liquid; Dimethylsulfoxide; X-ray and neutron scattering; Dielectric spectroscopy; Hydrogen bonding ID PROTIC IONIC LIQUIDS; INITIO MOLECULAR-DYNAMICS; X-RAY-DIFFRACTION; WATER MIXTURES; TEMPERATURE-DEPENDENCE; NEUTRON-SCATTERING; MONTE-CARLO; INORGANIC SALTS; MD SIMULATIONS; SELF-DIFFUSION AB Here we report the first structural and dynamic investigation on ethylammonium nitrate, a representative protic Ionic liquid, and dimethylsulfoxide. By using joined x/ray and neutron diffraction, we exploit the EPSR approach to extract structural information at atomistic level. EAN/DMSO turns out to be homogeneous at microscopic scales and indications for the existence of a structural leit motiv with stoichiometric composition 2DMSO:1EAN are found. Dielectric spectroscopy is used to access the relaxation map of the DMSO:EAN = 60:40 mixture. No crystallisation is detected and three relaxation processes could be characterised. Overall this study provides new indications of strict analogies between water and ethylammonium nitrate. (c) 2014 Elsevier B.V. All rights reserved. C1 [Russina, Olga; Mariani, Alessandro; Caminiti, Ruggero] Univ Roma La Sapienza, Dept Chem, I-00185 Rome, Italy. [Macchiagodena, Marina; Kirchner, Barbara] Univ Bonn, Inst Phys & Theoret Chem, Mulliken Ctr Theoret Chem, D-53115 Bonn, Germany. [Mariani, Alessandro; Triolo, Alessandro] CNR, Ist Struttura Mat, Lab Liquidi lonici, I-00133 Rome, Italy. [Aoun, Bachir] Argonne Natl Lab, Lemont, IL 60439 USA. [Russina, Margarita] Helmholtz Zentrum Berlin Mat & Energie, Berlin, Germany. RP Russina, O (reprint author), Univ Roma La Sapienza, Dept Chem, I-00185 Rome, Italy. EM olga.russina@uniroma1.it; triolo@ism.cnr.it RI Triolo, Alessandro/A-4431-2012; Russina, Margarita/E-9886-2016; Russina, Olga/G-9780-2012; OI Triolo, Alessandro/0000-0003-4074-0743; Russina, Margarita/0000-0003-2067-606X; Mariani, Alessandro/0000-0002-3686-2169 NR 79 TC 15 Z9 15 U1 5 U2 40 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0022-3093 EI 1873-4812 J9 J NON-CRYST SOLIDS JI J. Non-Cryst. Solids PD JAN 1 PY 2015 VL 407 SI SI BP 333 EP 338 DI 10.1016/j.jnoncrysol.2014.08.051 PG 6 WC Materials Science, Ceramics; Materials Science, Multidisciplinary SC Materials Science GA AX6FJ UT WOS:000347018300047 ER PT J AU Perticaroli, S Comez, L Sassi, P Paolantoni, M Corezzi, S Caponi, S Morresi, A Fioretto, D AF Perticaroli, S. Comez, L. Sassi, P. Paolantoni, M. Corezzi, S. Caponi, S. Morresi, A. Fioretto, D. TI Hydration and aggregation of lysozyme by extended frequency range depolarized light scattering SO JOURNAL OF NON-CRYSTALLINE SOLIDS LA English DT Article; Proceedings Paper CT 7th International Discussion Meeting on Relaxations in Complex Systems (IDMRCS) CY JUL 21-26, 2013 CL Univ Politecnica Catalunya, Barcelona, SPAIN SP Energia Campus Int Excellence, Barcelona Knowledge Campus, Inst Laue Langevin, Julich Forschungszentrum, CNRS, Lab Leon Brillouin, Int Dielectr Soc, AirLiquide, Almirall, Bruker, Extrasolution, Matgas, Mettler Toledo, Novocontrol Technologies, TA Instruments, Polish Acad Sci, Inst High Pressure Phys HO Univ Politecnica Catalunya DE Hydration water; Biological water; Lysozyme; Depolarized light scattering ID EQUILIBRIUM CLUSTER PHASE; AQUEOUS-SOLUTIONS; WATER DYNAMICS; BIOMOLECULAR HYDRATION; SUPERCOOLED WATER; GLOBULAR-PROTEINS; CELL BIOLOGY; SPECTROSCOPY; RELAXATION; TREHALOSE AB Extended frequency range depolarized light scattering is a spectroscopic technique operating in the GHz-THz range that, applied to aqueous solutions of biomolecules, is able to disentangle the dynamics of the solute from that of water, and relaxation processes of bulk from those of hydration water. Experiments performed on aqueous solution of a variety of biological systems of different nature, such as small hydrophobic and hydrophilic molecules, amino acids, dipeptides, and proteins, have shown that a significant increase in the dynamical retardation and in the extent of the perturbation of water surrounding solute molecules occurs at increasing chemical complexity of the solute. The behavior of aqueous solutions of lysozyme is here analyzed in detail, as a function of solute concentration. Our results provide evidence of a dynamical perturbation extending over more than three water layers in diluted solutions. We find a strong reduction in the average hydration number at increasing solute concentration that cannot be explained by the random superposition of hydration layers among lysozyme molecules in close proximity. This behavior is consistent with the formation of clusters in solution. (c) 2014 Elsevier B.V. All rights reserved. C1 [Perticaroli, S.] Oak Ridge Natl Lab, Joint Inst Neutron Sci, Oak Ridge, TN 37831 USA. [Perticaroli, S.] Oak Ridge Natl Lab, Chem & Mat Sci Div, Oak Ridge, TN 37831 USA. [Perticaroli, S.] Univ Tennessee, Dept Chem, Knoxville, TN 37996 USA. [Comez, L.; Caponi, S.] Univ Perugia, Dipartimento Fis Geol, IOM, CNR, I-06123 Perugia, Italy. [Sassi, P.; Paolantoni, M.; Morresi, A.] Univ Perugia, Dipartimento Chim Biol & Biotecnol, I-06123 Perugia, Italy. [Corezzi, S.; Fioretto, D.] Univ Perugia, Dipartimento Fis Geol, I-06123 Perugia, Italy. [Corezzi, S.] Univ Roma La Sapienza, CNR, ISC, Ist Sistemi Complessi, I-00185 Rome, Italy. [Fioretto, D.] Univ Perugia, CEMIN, I-06123 Perugia, Italy. RP Fioretto, D (reprint author), Univ Perugia, Dipartimento Fis Geol, Via Pascoll, I-06123 Perugia, Italy. EM daniele.fioretto@unipg.it RI Sassi, Paola/F-1141-2014; Paolantoni, Marco /G-1646-2014; Morresi, Assunta/M-7359-2014; Caponi, Silvia/F-9821-2010; Corezzi, Silvia/B-9035-2016 OI Sassi, Paola/0000-0002-4920-2784; Paolantoni, Marco /0000-0002-6266-3497; Morresi, Assunta/0000-0002-0481-6424; Caponi, Silvia/0000-0002-4219-3256; Corezzi, Silvia/0000-0002-3437-5949 NR 60 TC 6 Z9 6 U1 1 U2 23 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0022-3093 EI 1873-4812 J9 J NON-CRYST SOLIDS JI J. Non-Cryst. Solids PD JAN 1 PY 2015 VL 407 SI SI BP 472 EP 477 DI 10.1016/j.jnoncrysol.2014.07.017 PG 6 WC Materials Science, Ceramics; Materials Science, Multidisciplinary SC Materials Science GA AX6FJ UT WOS:000347018300064 ER PT J AU Nakanishi, M Sokolov, AP AF Nakanishi, Masahiro Sokolov, Alexei P. TI Protein dynamics in a broad frequency range: Dielectric spectroscopy studies SO JOURNAL OF NON-CRYSTALLINE SOLIDS LA English DT Article; Proceedings Paper CT 7th International Discussion Meeting on Relaxations in Complex Systems (IDMRCS) CY JUL 21-26, 2013 CL Univ Politecnica Catalunya, Barcelona, SPAIN SP Energia Campus Int Excellence, Barcelona Knowledge Campus, Inst Laue Langevin, Julich Forschungszentrum, CNRS, Lab Leon Brillouin, Int Dielectr Soc, AirLiquide, Almirall, Bruker, Extrasolution, Matgas, Mettler Toledo, Novocontrol Technologies, TA Instruments, Polish Acad Sci, Inst High Pressure Phys HO Univ Politecnica Catalunya DE Protein dynamics; Hydration water; Glass transition; Dielectric spectroscopy; Lysozyme; Myoglobin ID EGG-WHITE LYSOZYME; GOLDSTEIN BETA-RELAXATION; BOVINE SERUM-ALBUMIN; NEUTRON SPIN-ECHO; GLOBULAR-PROTEINS; HYDRATION WATER; GLASS FORMERS; PHOSPHOGLYCERATE KINASE; RIBONUCLEASE-A; WIDE RANGES AB We present detailed dielectric spectroscopy studies of dynamics in two hydrated proteins, lysozyme and myoglobin. We emphasize the importance of explicit account for possible Maxwell-Wagner (MW) polarization effects in protein powder samples. Combining our data with earlier literature results, we demonstrate the existence of three major relaxation processes in globular proteins. To understand the mechanisms of these relaxations we involve literature data on neutron scattering, simulations and NMR studies. The faster process is ascribed to coupled protein-hydration water motions and has relaxation time similar to 10-50 Ps at room temperature. The intermediate process is similar to 10(2)-10(3) times slower than the faster process and might be strongly affected by MW polarizations. Based on the analysis of data obtained by different experimental techniques and simulations, we ascribe this process to large scale domain-like motions of proteins. The slowest observed process is similar to 10(6)-10(7) times slower than the faster process and has anomalously large dielectric amplitude Delta epsilon similar to 10(2)-10(4). The microscopic nature of this process is not clear, but it seems to be related to the glass transition of hydrated proteins. The presentedresults suggest a general classification of the relaxation processes in hydrated proteins. (c) 2014 Elsevier B.V. All rights reserved. C1 [Nakanishi, Masahiro] Hebrew Univ Jerusalem, Dept Appl Phys, IL-91904 Jerusalem, Israel. [Sokolov, Alexei P.] Univ Tennessee, Dept Chem, Knoxville, TN 37996 USA. [Sokolov, Alexei P.] Univ Tennessee, Joint Inst Neutron Sci, Knoxville, TN 37996 USA. [Sokolov, Alexei P.] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. RP Sokolov, AP (reprint author), 1420 Cirde Dr, Knoxville, TN 37996 USA. EM sokolov@utk.edu RI Nakanishi, Masahiro/J-9497-2014 OI Nakanishi, Masahiro/0000-0003-0844-8363 NR 84 TC 11 Z9 11 U1 7 U2 36 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0022-3093 EI 1873-4812 J9 J NON-CRYST SOLIDS JI J. Non-Cryst. Solids PD JAN 1 PY 2015 VL 407 SI SI BP 478 EP 485 DI 10.1016/j.jnoncrysol.2014.08.057 PG 8 WC Materials Science, Ceramics; Materials Science, Multidisciplinary SC Materials Science GA AX6FJ UT WOS:000347018300065 ER PT J AU Miao, YB Beeler, B Deo, C Baskes, MI Okuniewski, MA Stubbins, JF AF Miao, Yinbin Beeler, Benjamin Deo, Chaitanya Baskes, Michael I. Okuniewski, Maria A. Stubbins, James F. TI Defect structures induced by high-energy displacement cascades in gamma uranium SO JOURNAL OF NUCLEAR MATERIALS LA English DT Article ID EMBEDDED-ATOM METHOD; IMPURITIES; POTENTIALS; METALS; DAMAGE; IRON; FUEL AB Displacement cascade simulations were conducted for the gamma uranium system based on molecular dynamics. A recently developed modified embedded atom method (MEAM) potential was employed to replicate the atomic interactions while an embedded atom method (EAM) potential was adopted to help characterize the defect structures induced by the displacement cascades. The atomic displacement process was studied by providing primary knock-on atoms (PKAs) with kinetic energies from 1 key to 50 keV. The influence of the PKA incident direction was examined. The defect structures were analyzed after the systems were fully relaxed. The states of the self-interstitial atoms (SlAs) were categorized into various types of dumbbells, the crowdion, and the octahedral interstitial. The voids were determined to have a polyhedral shape with {110) facets. The size distribution of the voids was also obtained. The results of this study not only expand the knowledge of the microstructural evolution in irradiated gamma uranium, but also provide valuable references for the radiation-induced defects in uranium alloy fuels. (C) 2014 Elsevier B.V. All rights reserved. C1 [Miao, Yinbin; Stubbins, James F.] Univ Illinois, Dept Nucl Plasma & Radiol Engn, Urbana, IL 61801 USA. [Beeler, Benjamin] Univ Calif Davis, Dept Mech & Aerosp Engn, Davis, CA 95616 USA. [Deo, Chaitanya] Georgia Inst Technol, Dept Nucl & Radiol Engn, Atlanta, GA 30332 USA. [Baskes, Michael I.] Mississippi State Univ, Dept Aerosp Engn, Mississippi State, MS 39762 USA. [Baskes, Michael I.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Baskes, Michael I.] Univ Calif San Diego, Dept Mech & Aerosp Engn, La Jolla, CA 92093 USA. [Okuniewski, Maria A.] Idaho Natl Lab, Idaho Falls, ID 83415 USA. RP Miao, YB (reprint author), 216 Talbot Lab, 104 South Wright St, Urbana, IL 61801 USA. EM miao2@illinois.edu OI Miao, Yinbin/0000-0002-3128-4275 FU Taub Cluster in University of Illinois at Urbana-Champaign FX The computing resource was supported by the Taub Cluster in University of Illinois at Urbana-Champaign. Simulation results were visualized by the Open Visual Tool (OVITO)[32]. NR 32 TC 3 Z9 3 U1 3 U2 20 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0022-3115 EI 1873-4820 J9 J NUCL MATER JI J. Nucl. Mater. PD JAN PY 2015 VL 456 BP 1 EP 6 DI 10.1016/j.jnucmat.2014.09.016 PG 6 WC Materials Science, Multidisciplinary; Nuclear Science & Technology SC Materials Science; Nuclear Science & Technology GA AY0GC UT WOS:000347274500001 ER PT J AU Luscher, WG Senor, DJ Clayton, KK Longhurst, GR AF Luscher, Walter G. Senor, David J. Clayton, Kevin K. Longhurst, Glen R. TI In-reactor oxidation of zircaloy-4 under low water vapor pressures SO JOURNAL OF NUCLEAR MATERIALS LA English DT Article ID AUTOCLAVE; CORROSION; ZIRCONIUM; IRRADIATION; EVOLUTION; KINETICS; IMPACT AB Complementary in- and ex-reactor oxidation tests have been performed to evaluate the oxidation and hydrogen absorption performance of Zircaloy-4 (Zr-4) under relatively low partial pressures (300 and 1000 Pa) of water vapor at specified test temperatures (330 and 370 degrees C). Data from these tests will be used to support the fabrication of components intended for isotope-producing targets and provide information regarding the temperature and pressure dependence of oxidation and hydrogen absorption of Zr4 over the specified range of test conditions. Comparisons between in- and ex-reactor test results were performed to evaluate the influence of irradiation. (C) 2014 Elsevier B.V. All rights reserved. C1 [Luscher, Walter G.; Senor, David J.] Pacific NW Natl Lab, Richland, WA 99352 USA. [Clayton, Kevin K.; Longhurst, Glen R.] Idaho Natl Lab, Idaho Falls, ID 83415 USA. RP Luscher, WG (reprint author), Pacific NW Natl Lab, 902 Battelle Blvd, Richland, WA 99352 USA. EM walter.luscher@pnnl.gov; david.senor@pnnl.gov; kevin.clayton@inl.gov; glenlonghurst@suu.edu NR 17 TC 0 Z9 0 U1 0 U2 17 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0022-3115 EI 1873-4820 J9 J NUCL MATER JI J. Nucl. Mater. PD JAN PY 2015 VL 456 BP 17 EP 22 DI 10.1016/j.jnucmat.2014.08.053 PG 6 WC Materials Science, Multidisciplinary; Nuclear Science & Technology SC Materials Science; Nuclear Science & Technology GA AY0GC UT WOS:000347274500003 ER PT J AU Janney, DE Kennedy, JR Madden, JW O'Holleran, TP AF Janney, Dawn E. Kennedy, J. Rory Madden, James W. O'Holleran, Thomas P. TI Am phases in the matrix of a U-Pu-Zr alloy with Np, Am, and rare-earth elements SO JOURNAL OF NUCLEAR MATERIALS LA English DT Article ID X-RAY-DIFFRACTION; MINOR ACTINIDES; ZIRCONIUM SYSTEM; METALLIC FUELS; REDISTRIBUTION; TEMPERATURE; BEHAVIOR; URANIUM AB Phases and microstructures in the matrix of an as-cast U-Pu-Zr alloy with 3 wt% Am, 2% Np, and 8% rare-earth elements were characterized by scanning and transmission electron microscopy. The matrix consists primarily of two phases, both of which contain Am: zeta-(U, Np, Pu, Am) (similar to 70 at.% U, 5% Np, 14% Pu, 1% Am, and 10% Zr) and delta-(U, Np, Pu, Am)Zr-2 (similar to 25% U, 2% Np, 10-15% Pu, 1-2% Am, and 55-60 at.% Zr). These phases are similar to those in U-Pu-Zr alloys, although the Zr content in zeta-(U, Np, Pu, Am) is higher than that in zeta-(U, Pu) and the Zr content in delta-(U, Np, Put Am)Zr-2 is lower than that in delta-UZr2. Nanocrystalline actinide oxides with structures similar to UO2 occurred in some areas, but may have formed by reactions with the atmosphere during sample handling. Planar features consisting of a central zone of zeta-(U, Np, Pu, Am) bracketed by zones of delta-(U, Np, Pu, Am)Zr-2 bound irregular polygons ranging in size from a few micrometers to a few tens of micrometers across. The rest of the matrix consists of elongated domains of Np, Pu, Am) and delta-(U, Np, Pu, Am)Zr-2. Each of these domains is a few tens of nanometers across and a few hundred nanometers long. The domains display strong preferred orientations involving areas a few hundred nanometers to a few micrometers across. (C) 2014 Elsevier B.V. All rights reserved. C1 [Janney, Dawn E.; Kennedy, J. Rory; Madden, James W.; O'Holleran, Thomas P.] Idaho Natl Lab, Idaho Falls, ID 83415 USA. RP Janney, DE (reprint author), Idaho Natl Lab, Mail Stop 6188, Idaho Falls, ID 83415 USA. EM dawn.janney@inl.gov; rory.kennedy@inl.gov; james.madden@inl.gov; thomas.oholleran@inl.gov FU U.S. Department of Energy, Office of Nuclear Energy, under DOE Idaho Operations Office [DE-AC07-051D14517] FX The research presented here was supported by the U.S. Department of Energy, Office of Nuclear Energy, under DOE Idaho Operations Office Contract DE-AC07-051D14517. NR 37 TC 3 Z9 3 U1 2 U2 8 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0022-3115 EI 1873-4820 J9 J NUCL MATER JI J. Nucl. Mater. PD JAN PY 2015 VL 456 BP 46 EP 53 DI 10.1016/j.jnucmat.2014.08.051 PG 8 WC Materials Science, Multidisciplinary; Nuclear Science & Technology SC Materials Science; Nuclear Science & Technology GA AY0GC UT WOS:000347274500007 ER PT J AU He, L Valderrama, B Hassan, AR Yu, J Gupta, M Pakarinen, J Henderson, HB Gan, J Kirk, MA Nelson, AT Manuel, MV El-Azab, A Allen, TR AF He, L. F. Valderrama, B. Hassan, A. -R. Yu, J. Gupta, M. Pakarinen, J. Henderson, H. B. Gan, J. Kirk, M. A. Nelson, A. T. Manuel, M. V. El-Azab, A. Allen, T. R. TI Bubble formation and Kr distribution in Kr-irradiated UO2 SO JOURNAL OF NUCLEAR MATERIALS LA English DT Article ID AUGMENTED-WAVE METHOD; HIGH-RESOLUTION TEM; IN-SITU TEM; FISSION-GAS; URANIUM-DIOXIDE; HIGH-TEMPERATURE; RE-SOLUTION; FUELS; KRYPTON; PRECIPITATION AB In situ and ex situ transmission electron microscopy observation of small Kr bubbles in both single-crystal and polycrystalline UO2 were conducted to understand the inert gas bubble behavior in oxide nuclear fuel. The bubble size and volume swelling are shown as weak functions of ion dose but strongly depend on the temperature. The Kr bubble formation at room temperature was observed for the first time. The depth profiles of implanted Kr determined by atom probe tomography are in good agreement with the calculated profiles by SRIM, but the measured concentration of Kr is about 1/4 of the calculated concentration. This difference is mainly due to low solubility of Kr in UO2 matrix and high release of Kr from sample surface under irradiation. Published by Elsevier B.V. C1 [He, L. F.; Gupta, M.; Pakarinen, J.; Allen, T. R.] Univ Wisconsin, Dept Engn Phys, Madison, WI 53706 USA. [Valderrama, B.; Henderson, H. B.; Manuel, M. V.] Univ Florida, Dept Mat Sci & Engn, Gainesville, FL 32611 USA. [Hassan, A. -R.; El-Azab, A.] Purdue Univ, Sch Nucl Engn, W Lafayette, IN 47907 USA. [Yu, J.; Gan, J.; Allen, T. R.] Idaho Natl Lab, Idaho Falls, ID 83415 USA. [Kirk, M. A.] Argonne Natl Lab, Argonne, IL 60439 USA. [Nelson, A. T.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP He, L (reprint author), Idaho Natl Lab, POB 1625, Idaho Falls, ID 83415 USA. EM Ifhechina@gmail.com RI Manuel, Michele/A-8795-2009; Yu, Jianguo/C-3424-2013; OI Manuel, Michele/0000-0002-3495-7826; Yu, Jianguo/0000-0001-5604-8132; Allen, Todd/0000-0002-2372-7259; He, Lingfeng/0000-0003-2763-1462 FU Center for Materials Science of Nuclear Fuel, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [FWP 1356]; U.S. Department of Energy, Office of Nuclear Energy under DOE Idaho Operations Office, ATR National Scientific User Facility experiments [DE-AC07-051D14517]; U.S. Department of Energy Office of Science Laboratory [DE-ACO2-06CH11357] FX This work was supported as part of the Center for Materials Science of Nuclear Fuel, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under award number FWP 1356. This work was also supported by the U.S. Department of Energy, Office of Nuclear Energy under DOE Idaho Operations Office Contract DE-AC07-051D14517, as part of an ATR National Scientific User Facility experiments. The Kr implantation was accomplished at the Electron Microscopy Center for Materials Research at Argonne National Laboratory, a U.S. Department of Energy Office of Science Laboratory operated under Contract No. DE-ACO2-06CH11357 by UChicago Argonne, LLC. NR 53 TC 3 Z9 3 U1 1 U2 28 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0022-3115 EI 1873-4820 J9 J NUCL MATER JI J. Nucl. Mater. PD JAN PY 2015 VL 456 BP 125 EP 132 DI 10.1016/j.jnucmat.2014.09.026 PG 8 WC Materials Science, Multidisciplinary; Nuclear Science & Technology SC Materials Science; Nuclear Science & Technology GA AY0GC UT WOS:000347274500017 ER PT J AU McMurray, JW Shin, D Besmann, TM AF McMurray, J. W. Shin, D. Besmann, T. M. TI Thermodynamic assessment of the U-La-O system SO JOURNAL OF NUCLEAR MATERIALS LA English DT Article ID URANIUM-OXYGEN SYSTEM; PHASE; DIOXIDE; OXIDES; FUELS; UO2; GD AB The CALPHAD methodology was used to develop a thermodynamic assessment of the U-La-O system. The solid solution and liquid phases are described with the compound energy formalism (CEF) and the partially ionic two-sublattice liquid model, respectively. Experimental thermodynamic and phase equilibria data published in the open literature were then used in optimizations to develop representations of the phases in the system that can be extended to include other actinide and fission products for multi-component models. The models that comprise this assessment very well reproduce experimentally determined oxygen potentials and the observed phase relations for the U-La-O system. (C) 2014 Elsevier B.V. All rights reserved. C1 [McMurray, J. W.; Shin, D.; Besmann, T. M.] Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN 37831 USA. RP McMurray, JW (reprint author), Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN 37831 USA. EM mcmurrayjwl@ornl.gov RI Shin, Dongwon/C-6519-2008; OI Shin, Dongwon/0000-0002-5797-3423; McMurray, Jacob/0000-0001-5111-3054 FU US Department of Energy, Office of Nuclear Energy Fuel Cycle Technology Program FX The authors would like to thank Tom Watkins and Dane Wilson of Oak Ridge National Laboratory for helpful comments. The work was supported by the US Department of Energy, Office of Nuclear Energy Fuel Cycle Technology Program. NR 32 TC 6 Z9 6 U1 2 U2 11 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0022-3115 EI 1873-4820 J9 J NUCL MATER JI J. Nucl. Mater. PD JAN PY 2015 VL 456 BP 142 EP 150 DI 10.1016/j.jnucmat.2014.09.031 PG 9 WC Materials Science, Multidisciplinary; Nuclear Science & Technology SC Materials Science; Nuclear Science & Technology GA AY0GC UT WOS:000347274500019 ER PT J AU Lee, CW Chernatynskiy, A Shukla, P Stoller, RE Sinnott, SB Phillpot, SR AF Lee, C. -W. Chernatynskiy, A. Shukla, P. Stoller, R. E. Sinnott, S. B. Phillpot, S. R. TI Effect of pores and He bubbles on the thermal transport properties of UO2 by molecular dynamics simulation SO JOURNAL OF NUCLEAR MATERIALS LA English DT Article ID MIXED-OXIDE FUELS; URANIUM-DIOXIDE; HIGH BURNUP; GAS BUBBLES; CONDUCTIVITY; POROSITY; HELIUM; BEHAVIOR; CODE; IRRADIATION AB The thermal conductivities of UO2 single crystals containing nanoscale size pores and He gas bubbles are calculated using non-equilibrium molecular dynamics as a function of pore size and gas density in the bubble. As expected, the thermal conductivity decreases as pore size increases, while the decrease in thermal conductivity is determined to be more substantial than the predictions of traditional analytical models by Loeb and Maxwell-Eucken. However, the recent model of Alvarez, which is applicable when the phonon mean-free path is comparable to the pore size, is able to quantitatively reproduce the simulation results. The thermal conductivity of UO2 of the small pores considered here is reduced further when the pore is filled with He gas. This surprising result is due to the penetration of the helium atoms into the lattice where they act as phonon scattering centers. (C) 2014 Elsevier B.V. All rights reserved. C1 [Lee, C. -W.; Chernatynskiy, A.; Shukla, P.; Sinnott, S. B.; Phillpot, S. R.] Univ Florida, Dept Mat Sci & Engn, Gainesville, FL 32611 USA. [Stoller, R. E.] Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN 37831 USA. RP Phillpot, SR (reprint author), Korea Inst Energy Res, Energy Storage Lab, 152 Gajeong Ro, Taejon 305343, South Korea. EM sphil@mse.ufl.edu OI Chernatynskiy, Aleksandr/0000-0001-7431-7201 FU NEAMS FOA; U.S. Government under DOE under the Energy Frontier Research Center (Office of Science, Office of Basic Energy Science) [DE-AC07-05ID14517, FWP 1356]; Air Force Office of Scientific Research [FA9550-12-1-0456]; U.S. Department of Energy, Office of Fusion Energy Sciences under UT-Battelle, LLC FX CWL and SRP were support by the NEAMS FOA Project on Physics-Based Models for 3D Predictive Simulation of Fast Reactor Fuel Performance. This work was co-authored by subcontractor (AC) of the U.S. Government under DOE Contract No. DE-AC07-05ID14517, under the Energy Frontier Research Center (Office of Science, Office of Basic Energy Science, FWP 1356). Accordingly, the U.S. Government retains and the publisher (by accepting the article for publication) acknowledges that the U.S. Government retains a nonexclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for U.S. Government purposes. SBS acknowledges the support of the Air Force Office of Scientific Research through Award Number FA9550-12-1-0456. RES acknowledges the support of U.S. Department of Energy, Office of Fusion Energy Sciences under contract with UT-Battelle, LLC. NR 61 TC 6 Z9 6 U1 2 U2 19 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0022-3115 EI 1873-4820 J9 J NUCL MATER JI J. Nucl. Mater. PD JAN PY 2015 VL 456 BP 253 EP 259 DI 10.1016/j.jnucmat.2014.09.052 PG 7 WC Materials Science, Multidisciplinary; Nuclear Science & Technology SC Materials Science; Nuclear Science & Technology GA AY0GC UT WOS:000347274500032 ER PT J AU Gerczak, TJ Zheng, G Field, KG Allen, TR AF Gerczak, Tyler J. Zheng, Guiqiu Field, Kevin G. Allen, Todd R. TI Effect of exposure environment on surface decomposition of SiC-silver ion implantation diffusion couples SO JOURNAL OF NUCLEAR MATERIALS LA English DT Article ID COATED PARTICLE FUEL; SILICON-CARBIDE; CARBON; IRRADIATION; PERFORMANCE; GRAPHENE; RELEASE; FILMS AB SiC is a promising material for nuclear applications and is a critical component in the construction of tri-structural isotropic (TRISO) fuel. A primary issue with TRISO fuel operation is the observed release of Ag-110m from intact fuel particles. The release of Ag has prompted research efforts to directly measure the transport mechanism of Ag in bulk SiC. Recent experimental efforts have focused primarily on Ag ion implantation designs. The effect of the thermal exposure system on the ion implantation surface has been investigated. Results indicate the utilization of a mated sample geometry and the establishment of a static thermal exposure environment is critical to maintaining an intact surface for diffusion analysis. The nature of the implantation surface and its potential role in Ag diffusion analysis are discussed. Published by Elsevier B.V. C1 [Gerczak, Tyler J.; Zheng, Guiqiu; Field, Kevin G.] Univ Wisconsin, Mat Sci Program, Madison, WI 53706 USA. [Field, Kevin G.] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. [Allen, Todd R.] Univ Wisconsin, Dept Engn Phys, Madison, WI 53706 USA. RP Gerczak, TJ (reprint author), POB 2008, Oak Ridge, TN 37831 USA. EM gerczaktj@ornl.gov; gzheng@wisc.edu; fieldkg@ornl.gov; allen@engr.wisc.edu RI Zheng, Guiqiu/G-7548-2015; OI Zheng, Guiqiu/0000-0002-5783-5848; Allen, Todd/0000-0002-2372-7259; Gerczak, Tyler/0000-0001-9967-3579 FU US DOE, Office of Nuclear Energy Nuclear Energy University Program (NEUP) [11-2988]; US DOE, Office of Nuclear Energy under DOE Idaho Operations Office [DE-AC07-051D14517] FX A portion of this research utilized National Science Foundation (NSF) supported shared facilities at the University of Wisconsin. This work supported by the US DOE, Office of Nuclear Energy Nuclear Energy University Program (NEUP), Award no. 11-2988 and by the US DOE, Office of Nuclear Energy under DOE Idaho Operations Office Contract DE-AC07-051D14517, as part of an ATR-NSUF experiment. The authors would also like to thank Dr. Ovidiu Toader for conducting the Ag implantations at the MIBL and Dr. Jerry Hunter for conducting the SIMS analysis at ICTAS at Va. Tech. NR 33 TC 3 Z9 3 U1 3 U2 21 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0022-3115 EI 1873-4820 J9 J NUCL MATER JI J. Nucl. Mater. PD JAN PY 2015 VL 456 BP 281 EP 286 DI 10.1016/j.jnucmat.2014.09.063 PG 6 WC Materials Science, Multidisciplinary; Nuclear Science & Technology SC Materials Science; Nuclear Science & Technology GA AY0GC UT WOS:000347274500036 ER PT J AU Shao, L Chen, D Wei, CC Martin, MS Wang, XM Park, Y Dein, E Coffey, KR Sohn, Y Sencer, BH Kennedy, JR AF Shao, Lin Chen, Di Wei, Chaochen Martin, Michael S. Wang, Xuemei Park, Youngjoo Dein, Ed Coffey, Kevin R. Sohn, Yongho Sencer, Bulent H. Kennedy, J. Rory TI Radiation effects on interface reactions of U/Fe, U/(Fe plus Cr), and U/(Fe plus Cr plus Ni) SO JOURNAL OF NUCLEAR MATERIALS LA English DT Article ID MECHANICAL-PROPERTIES; STEEL; INTERDIFFUSION; TANTALUM; ALLOY; FE AB We study the effects of radiation damage on interdiffusion and intermetallic phase formation at the interfaces of U/Fe, U/(Fe + Cr), and U/(Fe + Cr + Ni) diffusion couples. Magnetron sputtering is used to deposit thin films of Fe, Fe + Cr, or Fe + Cr + Ni on U substrates to form the diffusion couples. One set of samples are thermally annealed under high vacuum at 450 degrees C or 550 degrees C for one hour. A second set of samples are annealed identically but with concurrent 3.5 MeV Fe++ ion irradiation. The Fe++ ion penetration depth is sufficient to reach the original interfaces. Rutherford backscattering spectrometry analysis with high fidelity spectral simulations is used to obtain interdiffusion profiles, which are used to examine differences in U diffusion and intermetallic phase formation at the buried interfaces. For all three diffusion systems, Fe++ ion irradiations enhance U diffusion. Furthermore, the irradiations accelerate the formation of intermetallic phases. In U/Fe couples, for example, the unirradiated samples show typical interdiffusion governed by Fick's laws, while the irradiated ones show step-like profiles influenced by Gibbs phase rules. (C) 2014 Elsevier B.V. All rights reserved. C1 [Shao, Lin; Chen, Di; Wei, Chaochen; Martin, Michael S.; Wang, Xuemei] Texas A&M Univ, Dept Nucl Engn, College Stn, TX 77843 USA. [Park, Youngjoo; Dein, Ed; Coffey, Kevin R.; Sohn, Yongho] Univ Cent Florida, Mat Sci & Engn, Orlando, FL 32816 USA. [Sencer, Bulent H.; Kennedy, J. Rory] Idaho Natl Lab, Mat & Nucl Fuel Performance, Idaho Falls, ID 83415 USA. RP Shao, L (reprint author), Texas A&M Univ, Dept Nucl Engn, College Stn, TX 77843 USA. EM lshao@tamu.edu RI Sohn, Yongho/A-8517-2010 OI Sohn, Yongho/0000-0003-3723-4743 FU U.S. Department of Energy under DOE-NE Idaho Operations Office [DE-AC07-05ID14517] FX This work was supported by the U.S. Department of Energy under DOE-NE Idaho Operations Office Contract DE-AC07-05ID14517. NR 30 TC 1 Z9 1 U1 2 U2 10 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0022-3115 EI 1873-4820 J9 J NUCL MATER JI J. Nucl. Mater. PD JAN PY 2015 VL 456 BP 302 EP 310 DI 10.1016/j.jnucmat.2014.09.046 PG 9 WC Materials Science, Multidisciplinary; Nuclear Science & Technology SC Materials Science; Nuclear Science & Technology GA AY0GC UT WOS:000347274500039 ER PT J AU Park, Y Keiser, DP Sohn, YH AF Park, Y. Keiser, D. P., Jr. Sohn, Y. H. TI Interdiffusion and reactions between U-Mo and Zr at 650 degrees C as a function of time SO JOURNAL OF NUCLEAR MATERIALS LA English DT Article ID URANIUM-MOLYBDENUM ALLOY; MONOLITHIC FUEL PLATE; DIFFUSION BARRIER; DISPERSION FUEL; THERMODYNAMIC PROPERTIES; PHASE-DIAGRAMS; HIGH-DENSITY; TH-MO AB Development of monolithic U-Mo alloy fuel (typically U-10 wt.%Mo) for the Reduced Enrichment for Research and Test Reactors (RERTR) program entails a use of Zr diffusion barrier to eliminate the interdiffusion-reactions between the fuel alloy and Al-alloy cladding. The application of Zr barrier to the U-Mo fuel system requires a co-rolling process that utilizes a soaking temperature of 650 degrees C, which represents the highest temperature the fuel system is exposed to during both fuel manufacturing and reactor application. Therefore, in this study, development of phase constituents, microstructure and diffusion kinetics of U-10 wt.%Mo and Zr was examined using solid-to-solid diffusion couples annealed at 650 degrees C for 240, 480 and 720 h. Phase constituents and microstructural development were analyzed by scanning electron microscopy (SEM) and transmission electron microscopy (TEM). Concentration profiles were mapped as diffusion paths on the isothermal ternary phase diagram. Within the diffusion zone, single-phase layers of beta-Zr and beta-U were observed along with a discontinuous layer of Mo2Zr between the beta-Zr and beta-U layers. In the vicinity of Mo2Zr phase, islands of alpha-Zr phases were also found. In addition, acicular alpha-Zr and U6Zr3Mo phases were observed within the gamma-U(Mo) terminal alloy. Growth rate of the interdiffusion-reaction zone was determined to be 7.75 (+/- 5.84) x 10(-16) m(2)/s at 650 degrees C, however with an assumption of a certain incubation period. (C) 2014 Elsevier B.V. All rights reserved. C1 [Park, Y.; Sohn, Y. H.] Univ Cent Florida, Adv Mat Proc & Anal Ctr, Dept Mat Sci & Engn, Orlando, FL 32816 USA. [Keiser, D. P., Jr.] Idaho Natl Lab, Nucl Fuels & Mat Div, Idaho Falls, ID 83415 USA. RP Sohn, YH (reprint author), Univ Cent Florida, Adv Mat Proc & Anal Ctr, Dept Mat Sci & Engn, 4000 Cent Florida Blvd, Orlando, FL 32816 USA. EM Yongho.Sohn@ucf.edu RI Sohn, Yongho/A-8517-2010 OI Sohn, Yongho/0000-0003-3723-4743 FU US Department of Energy under DOE-NE Idaho Operations Office [DE-AC07-051D14517]; agency of the U.S. Government FX The work was supported by the US Department of Energy under DOE-NE Idaho Operations Office Contract DE-AC07-051D14517 administered by Battelle Energy Alliance, LLC. The U.S. Government retains and the publisher, by accepting the article for publication, acknowledges that the U.S. Government retains a nonexclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for U.S. Government purposes.; U.S. Department of Energy Disclaimer: This information was prepared as an account of work sponsored by an agency of the U.S. Government. Neither the U.S. Government nor any agency thereof, nor any of their employees, makes any warranty, express or implied, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. References herein to any specific commercial product, process, or service by trade name, trademark, manufacturer, or otherwise, does not necessarily constitute or imply its endorsement, recommendation, or favoring by the U.S. Government or any agency thereof. The views and opinions of authors expressed herein do not necessarily state or reflect those of the U. S. Government or any agency thereof. NR 30 TC 3 Z9 3 U1 4 U2 18 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0022-3115 EI 1873-4820 J9 J NUCL MATER JI J. Nucl. Mater. PD JAN PY 2015 VL 456 BP 351 EP 358 DI 10.1016/j.jnucmat.2014.09.040 PG 8 WC Materials Science, Multidisciplinary; Nuclear Science & Technology SC Materials Science; Nuclear Science & Technology GA AY0GC UT WOS:000347274500046 ER PT J AU Pastore, G Swiler, LP Hales, JD Novascone, SR Perez, DM Spencer, BW Luzzi, L Van Uffelen, P Williamson, RL AF Pastore, Giovanni Swiler, L. P. Hales, J. D. Novascone, S. R. Perez, D. M. Spencer, B. W. Luzzi, L. Van Uffelen, P. Williamson, R. L. TI Uncertainty and sensitivity analysis of fission gas behavior in engineering-scale fuel modeling SO JOURNAL OF NUCLEAR MATERIALS LA English DT Article ID MULTIDIMENSIONAL MULTIPHYSICS SIMULATION; GRAIN-BOUNDARY DIFFUSION; URANIUM-DIOXIDE; RE-SOLUTION; UO2 FUEL; MOLECULAR-DYNAMICS; ROD ANALYSIS; RELEASE; IRRADIATION; BUBBLES AB The role of uncertainties in fission gas behavior calculations as part of engineering-scale nuclear fuel modeling is investigated using the BISON fuel performance code with a recently implemented physics-based model for fission gas release and swelling. Through the integration of BISON with the DAKOTA software, a sensitivity analysis of the results to selected model parameters is carried out based on UO2 single-pellet simulations covering different power regimes. The parameters are varied within ranges representative of the relative uncertainties and consistent with the information in the open literature. The study leads to an initial quantitative assessment of the uncertainty in fission gas behavior predictions with the parameter characterization presently available. Also, the relative importance of the single parameters is evaluated. Moreover, a sensitivity analysis is carried out based on simulations of a fuel rod irradiation experiment, pointing out a significant impact of the considered uncertainties on the calculated fission gas release and cladding diametral strain. The results of the study indicate that the commonly accepted deviation between calculated and measured fission gas release by a factor of 2 approximately corresponds to the inherent modeling uncertainty at high fission gas release. Nevertheless, significantly higher deviations may be expected for values around 10% and lower. Implications are discussed in terms of directions of research for the improved modeling of fission gas behavior for engineering purposes. (C) 2014 Elsevier B.V. All rights reserved. C1 [Pastore, Giovanni; Hales, J. D.; Novascone, S. R.; Perez, D. M.; Spencer, B. W.; Williamson, R. L.] Idaho Natl Lab, Idaho Falls, ID 83415 USA. [Swiler, L. P.] Sandia Natl Labs, Albuquerque, NM 87185 USA. [Luzzi, L.] Politecn Milan, Dept Energy, Nucl Engn Div, I-20156 Milan, Italy. [Van Uffelen, P.] Commiss European Communities, Joint Res Ctr, Inst Transuranium Elements, D-76344 Karlsruhe, Germany. RP Pastore, G (reprint author), Idaho Natl Lab, POB 1625, Idaho Falls, ID 83415 USA. EM Giovanni.Pastore@inl.gov; LPSwile@sandia.gov; jason.Hales@inl.gov; Stephen.Novascone@inl.gov; Danielle.Perez@inl.gov; Benjamin.Spencer@inl.gov; Lelio.Luzzi@polimi.it; Paul.Van-Uffelen@ec.europa.eu; Richard.Williamson@inl.gov OI Hales, Jason/0000-0003-0836-0476; Williamson, Richard/0000-0001-7734-3632; Pastore, Giovanni/0000-0003-2812-506X; Luzzi, Lelio/0000-0002-9754-4535 FU DOE Nuclear Energy Advanced Modeling and Simulation Program; US Government [DE-AC07-05ID14517] FX This work was funded by the DOE Nuclear Energy Advanced Modeling and Simulation Program. The submitted manuscript has been authored by a contractor of the US Government under Contract DE-AC07-05ID14517. Accordingly, the US Government retains a non-exclusive, royalty free license to publish or reproduce the published form of this contribution, or allow others to do so, for US Government purposes. NR 68 TC 11 Z9 11 U1 3 U2 13 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0022-3115 EI 1873-4820 J9 J NUCL MATER JI J. Nucl. Mater. PD JAN PY 2015 VL 456 BP 398 EP 408 DI 10.1016/j.jnucmat.2014.09.077 PG 11 WC Materials Science, Multidisciplinary; Nuclear Science & Technology SC Materials Science; Nuclear Science & Technology GA AY0GC UT WOS:000347274500052 ER PT J AU White, JT Nelson, AT Byler, DD Safarik, DJ Dunwoody, JT McClellan, KJ AF White, J. T. Nelson, A. T. Byler, D. D. Safarik, D. J. Dunwoody, J. T. McClellan, K. J. TI Thermophysical properties of U3Si5 to 1773 K SO JOURNAL OF NUCLEAR MATERIALS LA English DT Article ID U-SI SYSTEM; THERMAL-CONDUCTIVITY; HEAT-CAPACITY; FLASH METHOD; URANIUM; THORIUM; DIFFUSIVITY AB Possible use of U3Si5 as a nuclear reactor fuel requires knowledge of its thermophysical properties as a function of temperature. While limited data is available for U Si compounds containing higher uranium densities, no investigations of U3Si5 have been presented in the literature to date. High purity U3Si5 was fabricated to facilitate a set of experiments to determine the coefficient of thermal expansion, heat capacity, thermal diffusivity, and thermal conductivity from room temperature to 1773 K. Each measurement on nearly stoichiometric U3Si5 showed the existence of a phase transformation at 723 K, which is not consistent with the most recently published phase diagram. (C) 2014 Elsevier B.V. All rights reserved. C1 [White, J. T.; Nelson, A. T.; Byler, D. D.; Safarik, D. J.; Dunwoody, J. T.; McClellan, K. J.] Los Alamos Natl Lab, Div Mat Sci & Technol, Los Alamos, NM 87545 USA. RP White, JT (reprint author), Los Alamos Natl Lab, Div Mat Sci & Technol, Los Alamos, NM 87545 USA. EM jtwhite@lanl.gov FU U.S. Department of Energy, Office of Nuclear Energy Fuel Cycle Research and Development Program FX The support of the U.S. Department of Energy, Office of Nuclear Energy Fuel Cycle Research and Development Program is gratefully acknowledged. This work was performed at Los Alamos National Laboratory under the auspices of the U.S. Department of Energy. NR 24 TC 8 Z9 8 U1 2 U2 18 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0022-3115 EI 1873-4820 J9 J NUCL MATER JI J. Nucl. Mater. PD JAN PY 2015 VL 456 BP 442 EP 448 DI 10.1016/j.jnucmat.2014.10.021 PG 7 WC Materials Science, Multidisciplinary; Nuclear Science & Technology SC Materials Science; Nuclear Science & Technology GA AY0GC UT WOS:000347274500057 ER PT J AU Pillai, MRA Dash, A Knapp, FF AF Pillai, Maroor R. A. Dash, Ashutosh Knapp, Furn F. (Russ), Jr. TI Diversification of Mo-99/Tc-99m Separation: Non-Fission Reactor Production of Mo-99 as a Strategy for Enhancing Tc-99m Availability SO JOURNAL OF NUCLEAR MEDICINE LA English DT Article DE Mo-99; Tc-99m; fission moly; reactor production; cyclotron production AB This paper discusses the benefits of obtaining Tc-99m from non-fission reactor-produced low-specific-activity Mo-99. This scenario is based on establishing a diversified chain of facilities for the distribution of (99)mTc separated from reactor-produced Mo-99 by (n,Y) activation of natural or enriched Mo. Such facilities have expected lower investments than required for the proposed chain of cyclotrons for the production of (99)mTc. Facilities can receive and process reactor-irradiated Mo targets then used for extraction of (99)mTc over a period of 2 wk, with 3 extractions on the same day. Estimates suggest that a center receiving 1.85 TBq (50 Ci) of Mo-99 once every 4 d can provide 1.48-3.33 TBq (40-90 Ci) of (99)mTc daily. This model can use research reactors operating in the United States to supply current Mo-99 needs by applying natural Mo-nat targets. Mo-99 production capacity can be enhanced by using Mo-98-enriched targets. The proposed model reduces the loss of Mo-99 by decay and avoids proliferation as well as waste management issues associated with fission-produced Mo-99. C1 [Pillai, Maroor R. A.] Mol Grp Co, Cochin, Kerala, India. [Dash, Ashutosh] Bhabha Atom Res Ctr, Isotope Prod & Applicat Div, Bombay 400085, Maharashtra, India. [Knapp, Furn F. (Russ), Jr.] Oak Ridge Natl Lab, Med Radioisotope Program, Oak Ridge, TN 27830 USA. RP Knapp, FF (reprint author), Oak Ridge Natl Lab, Mail Stop 6229,Bldg 4501,POB 2008, Oak Ridge, TN 27830 USA. EM knappffjr@ornl.gov NR 10 TC 1 Z9 1 U1 1 U2 10 PU SOC NUCLEAR MEDICINE INC PI RESTON PA 1850 SAMUEL MORSE DR, RESTON, VA 20190-5316 USA SN 0161-5505 EI 1535-5667 J9 J NUCL MED JI J. Nucl. Med. PD JAN PY 2015 VL 56 IS 1 BP 159 EP 161 DI 10.2967/jnumed.114.149609 PG 3 WC Radiology, Nuclear Medicine & Medical Imaging SC Radiology, Nuclear Medicine & Medical Imaging GA AX9PG UT WOS:000347233700045 PM 25537991 ER PT J AU Hernandez, EM Juarez, AM Kilcoyne, ALD Aguilar, A Hernandez, L Antillon, A Macaluso, D Morales-Mori, A Gonzalez-Magana, O Hanstorp, D Covington, AM Davis, V Calabrese, D Hinojosa, G AF Hernandez, E. M. Juarez, A. M. Kilcoyne, A. L. D. Aguilar, A. Hernandez, L. Antillon, A. Macaluso, D. Morales-Mori, A. Gonzalez-Magana, O. Hanstorp, D. Covington, A. M. Davis, V. Calabrese, D. Hinojosa, G. TI Absolute measurements of chlorine Cl+ cation single photoionization cross section SO JOURNAL OF QUANTITATIVE SPECTROSCOPY & RADIATIVE TRANSFER LA English DT Article DE Photoionization of ions; Absorption lines; VUV spectroscopy ID HIGH-RESOLUTION; SHELL PHOTOIONIZATION; OSCILLATOR-STRENGTHS; ELECTRON-IMPACT; ATOMIC CHLORINE; IONS; EXCITATION; ABUNDANCE AB The photoionization of Cl+ leading to Cl2+ was measured in the photon energy range of 19.5-28.0 eV. A spectrum with a photon energy resolution of 15 meV normalized to absolute cross-section measurements is presented. The measurements were carried out by merging a Cl+ ion beam with a photon beam of highly monochromatic synchrotron radiation at the Advanced Light Source at Lawrence Berkeley National Laboratory. The measured photoionization of Cl+ consists of several autoionization resonances surperimposed on the direct photoionization signal. Most of the prominent resonances are assigned to members of Rydberg series originating from the singlet ground state and from metastable triplet levels within the ground-state configuration of Cl+. The direct ionization cross section is no larger than 12 Mb. (C) 2014 Elsevier Ltd. All rights reserved. C1 [Hernandez, E. M.; Juarez, A. M.; Hernandez, L.; Antillon, A.; Morales-Mori, A.; Hinojosa, G.] Univ Nacl Autonoma Mexico, Inst Ciencias Fis Apartado, Cuernavaca 62251, Morelos, Mexico. [Kilcoyne, A. L. D.; Aguilar, A.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Macaluso, D.] Univ Montana, Dept Phys & Astron, Missoula, MT 59812 USA. [Gonzalez-Magana, O.] Univ Groningen, KVI Atom & Mol Phys, NL-9747 AA Groningen, Netherlands. [Hanstorp, D.] Univ Gothenburg, Dept Phys, SE-41296 Gothenburg, Sweden. [Covington, A. M.; Davis, V.] Univ Nevada, Dept Phys, Reno, NV 89557 USA. [Calabrese, D.] Sierra Coll, Dept Phys, Rocklin, CA 95677 USA. [Hernandez, E. M.] Univ Autonoma Estado Morelos, Fac Ciencias, Cuernavaca 62209, Morelos, Mexico. RP Hinojosa, G (reprint author), Univ Nacl Autonoma Mexico, Inst Ciencias Fis Apartado, Postal 48-3, Cuernavaca 62251, Morelos, Mexico. EM hinojosa@fis.unam.mx RI Kilcoyne, David/I-1465-2013; Juarez, Antonio/A-4858-2017; OI Calabrese, Dominic/0000-0003-3933-0739 FU Office of Science, Office of Basic Energy Sciences of the U.S. Department of Energy [DE-AC02-05CH11231]; CONACYT [CB-2011/167631]; Swedish Research Council; Sierra College; [DGAPA-PAPIIT-IN106813] FX The Advanced Light Source is supported by the Director, Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract no. DE-AC02-05CH11231. The authors wish to acknowledge technical support of ALS staff. Grants DGAPA-PAPIIT-IN106813, CONACYT CB-2011/167631. D.H. acknowledges support from the Swedish Research Council. D.C. acknowledges support from Sierra College. NR 25 TC 2 Z9 2 U1 2 U2 10 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0022-4073 EI 1879-1352 J9 J QUANT SPECTROSC RA JI J. Quant. Spectrosc. Radiat. Transf. PD JAN PY 2015 VL 151 BP 217 EP 223 DI 10.1016/j.jqsrt.2014.10.004 PG 7 WC Optics; Spectroscopy SC Optics; Spectroscopy GA AY0BM UT WOS:000347263000023 ER PT J AU Silverstein, HJ Huq, A Lee, M Choi, ES Zhou, HD Wiebe, CR AF Silverstein, Harlyn J. Huq, Ashfia Lee, Minseong Choi, Eun Sang Zhou, Haidong Wiebe, Christopher R. TI Nuclear and magnetic supercells in the multiferroic candidate: Pb3TeMn3P2O14 SO JOURNAL OF SOLID STATE CHEMISTRY LA English DT Article DE Langasite; Dugganite; Multiferroic; Antiferromagnetic; Pb3TeMn3P2O14; Supercell ID CA3GA2GE4O14 STRUCTURE; POWDER DIFFRACTION; CRYSTAL-STRUCTURE; DUGGANITE; BA3NBFE3SI2O14; LANGASITE; PB3TECO3V2O14; DISTORTIONS AB The dugganites, Te6+-containing members of the langasite series, have attracted recent interest due to their complex low-temperature magnetic unit cells, magnetodielectric, and potentially multiferroic properties. For Pb2+-containing dugganites, a large monoclinic supercell was reported and was found to have a profound effect on the low temperature magnetism and spin excitation spectra. Pb3TeMn3P2O14 is another dugganite previously shown to distort away from the canonical P321 langasite unit cell, although this supercell was never fully solved. Here we report the full crystal and magnetic structure solution of Pb3TeMn3P2O14 using synchrotron x-ray and neutron diffraction data: a large trigonal supercell is observed in this material, which is believed to be the first supercell of its kind in the langasite family. Here, the magnetic structure, high-magnetic field behavior, and dielectric properties of Pb3TeMn3P2O14 are presented. In addition to showing weak magnetoelectric behavior similar to other langasites, it was found that a phase transition occurs at 3 T near the antiferromagnetic transition temperature. (C) 2014 Elsevier Inc. All rights reserved. C1 [Silverstein, Harlyn J.; Wiebe, Christopher R.] Univ Manitoba, Dept Chem, Winnipeg, MB R3T 2N2, Canada. [Huq, Ashfia] Oak Ridge Natl Lab, Spallat Neutron Source, Oak Ridge, TN 37831 USA. [Lee, Minseong; Choi, Eun Sang] Natl High Magnet Field Lab, Tallahassee, FL 32310 USA. [Zhou, Haidong] Univ Tennessee, Dept Phys & Astron, Knoxville, TN 37996 USA. [Wiebe, Christopher R.] Univ Winnipeg, Dept Chem, Winnipeg, MB R3B 2E9, Canada. [Wiebe, Christopher R.] McMaster Univ, Dept Phys & Astron, Hamilton, ON L8S 4M1, Canada. RP Silverstein, HJ (reprint author), Univ Manitoba, Dept Chem, Parker Bldg, Winnipeg, MB R3T 2N2, Canada. EM umsilve3@myumanitoba.ca RI Huq, Ashfia/J-8772-2013; Lee, Minseong/D-5371-2016; Zhou, Haidong/O-4373-2016 OI Huq, Ashfia/0000-0002-8445-9649; FU NSERC [3862682010]; ACS Petroleum Research Fund (PRF) [51374-UR10]; CFI [26849]; NSF [DMR-1350002]; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]; Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy; National Science Foundation [DMR-1157490]; State of Florida; U.S. Department of Energy FX This work was supported by NSERC (Application No. 3862682010), The ACS Petroleum Research Fund (PRF No. 51374-UR10), and CFI (Project No. 26849). H.J.S. graciously thanks support from the Vanier CGS and MGS. C.R.W. would like to thank the Canada Research Chair (Tier II) program. H.D.Z. thanks the support of the NSF through award DMR-1350002. Use of the Advanced Photon Source at Argonne National Laboratory was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract no. DE-AC02-06CH11357. A portion of this research at Oak Ridge National Laboratory's Spallation Neutron Source was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy. A portion of this work was performed at the National High Magnetic Field Laboratory, which is supported by National Science Foundation Cooperative Agreement no. DMR-1157490, the State of Florida, and the U.S. Department of Energy. NR 43 TC 1 Z9 1 U1 2 U2 40 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 0022-4596 EI 1095-726X J9 J SOLID STATE CHEM JI J. Solid State Chem. PD JAN PY 2015 VL 221 BP 216 EP 223 DI 10.1016/j.jssc.2014.10.007 PG 8 WC Chemistry, Inorganic & Nuclear; Chemistry, Physical SC Chemistry GA AY0BT UT WOS:000347263700031 ER PT J AU Jin, GB Soderholm, L AF Jin, Geng Bang Soderholm, L. TI Solid-state syntheses and single-crystal characterizations of three tetravalent thorium and uranium silicates SO JOURNAL OF SOLID STATE CHEMISTRY LA English DT Article DE Thorium; Uranium; Silicate; Solid-state syntheses; Single-crystal structure; Raman spectroscopy ID HYDROTHERMAL SYNTHESIS; X-RAY; COFFINITE; HUTTONITE; EKANITE; THSIO4; RAMAN; SPECTROSCOPY; URANOTHORITES; CHEMISTRY AB Colorless crystals of ThSiO4 (huttonite) (1) and (Ca0.5Na0.5)(2)NaThSi8O20 (2) have been synthesized by the solid-state reactions of ThO2, CaSiO3, and Na2WO4 at 1073 K. Green crystals of (Ca0.5Na0.5)(2)NaUSi8O20 (3) have been synthesized by the solid-state reactions of UO2, CaSiO3, and Na2WO4 at 1003 K. All three compounds have been characterized by single-crystal X-ray diffraction. Compound 1 adopts a monazite-type three-dimensional condensed structure, which is built from edge- and corner-shared ThO9 polyhedra and SiO4 tetrahedra. Compounds 2 and 3 are isostructural and they crystallize in a steacyite-type structure. The structure consists of discrete pseudocubic [Si8O20](8-) polyanions, which are connected by An(4+) cations into a three-dimensional framework. Each An atom coordinates to eight monodentate [Si8O20](8-) moieties in a square antiprismatic geometry. Na+ and Ca2+ ions reside in the void within the framework. Raman spectra of 1, 2, and 3 were collected on single crystal samples. 1 displays more complex vibrational bands than thorite. Raman spectra of 2 and 3 are analogous with most of vibrational bands located at almost the same regions. (C) 2014 Elsevier Inc. All rights reserved. C1 [Jin, Geng Bang; Soderholm, L.] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. RP Jin, GB (reprint author), Argonne Natl Lab, CHM 200, 9700 S Cass Ave, Argonne, IL 60439 USA. EM gjin@anl.gov FU U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division [DE-AC02-06CH11357] FX This material is based upon work supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division under contract DE-AC02-06CH11357. NR 48 TC 3 Z9 3 U1 3 U2 23 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 0022-4596 EI 1095-726X J9 J SOLID STATE CHEM JI J. Solid State Chem. PD JAN PY 2015 VL 221 BP 405 EP 410 DI 10.1016/j.jssc.2014.10.018 PG 6 WC Chemistry, Inorganic & Nuclear; Chemistry, Physical SC Chemistry GA AY0BT UT WOS:000347263700057 ER PT J AU Adams, BW Rose-Petruck, C AF Adams, Bernhard W. Rose-Petruck, Christoph TI X-ray focusing scheme with continuously variable lens SO JOURNAL OF SYNCHROTRON RADIATION LA English DT Article DE X-ray focusing; continuously variable focal length ID REFRACTIVE LENSES; OPTICS; SYSTEM AB A novel hybrid X-ray focusing scheme was developed for operation of the X-ray streak camera at the Advanced Photon Source: an X-ray lens focuses vertically from a long distance of 16 m and produces an extended focus that has a small footprint on an inexpensive sagittal mirror. A patented method is used to continuously adjust the focal length of the lens and compensate for chromatic dispersion in energy scans. C1 [Adams, Bernhard W.] Argonne Natl Lab, Argonne, IL 60439 USA. [Rose-Petruck, Christoph] Brown Univ, Providence, RI 02912 USA. RP Adams, BW (reprint author), Argonne Natl Lab, 9700 S Cass Ave, Argonne, IL 60439 USA. EM adams@aps.anl.gov FU US Department of Energy, Office of Basic Energy Sciences [DE-AC02-06CH11357]; US Department of Energy [DE-FG02-08ER15937] FX The work at the Advanced Photon Source was supported by the US Department of Energy, Office of Basic Energy Sciences under Contract No. DE-AC02-06CH11357. CRP acknowledges support from the US Department of Energy under grant DE-FG02-08ER15937. We would like to thank M. C. Chollet for his participation in the early stages of this project. NR 20 TC 1 Z9 1 U1 1 U2 7 PU INT UNION CRYSTALLOGRAPHY PI CHESTER PA 2 ABBEY SQ, CHESTER, CH1 2HU, ENGLAND SN 1600-5775 J9 J SYNCHROTRON RADIAT JI J. Synchrot. Radiat. PD JAN PY 2015 VL 22 BP 16 EP 22 DI 10.1107/S1600577514020451 PN 1 PG 7 WC Instruments & Instrumentation; Optics; Physics, Applied SC Instruments & Instrumentation; Optics; Physics GA AX3PC UT WOS:000346850200004 PM 25537583 ER PT J AU Hudspeth, M Sun, T Parab, N Guo, Z Fezzaa, K Luo, S Chen, W AF Hudspeth, M. Sun, T. Parab, N. Guo, Z. Fezzaa, K. Luo, S. Chen, W. TI Simultaneous X-ray diffraction and phase-contrast imaging for investigating material deformation mechanisms during high-rate loading SO JOURNAL OF SYNCHROTRON RADIATION LA English DT Article DE Kolsky bar; dynamic diffraction ID SHAPE-MEMORY ALLOY; HIGH-STRAIN-RATE; COMPRESSION; PRESSURE; TENSION; BAR AB Using a high-speed camera and an intensified charge-coupled device (ICCD), a simultaneous X-ray imaging and diffraction technique has been developed for studying dynamic material behaviors during high-rate tensile loading. A Kolsky tension bar has been used to pull samples at 1000 s(-1) and 5000 s(-1) strain-rates for super-elastic equiatomic NiTi and 1100-O series aluminium, respectively. By altering the ICCD gating time, temporal resolutions of 100 ps and 3.37 mu s have been achieved in capturing the diffraction patterns of interest, thus equating to single-pulse and 22-pulse X-ray exposure. Furthermore, the sample through-thickness deformation process has been simultaneously imaged via phase-contrast imaging. It is also shown that adequate signal-to-noise ratios are achieved for the detected white-beam diffraction patterns, thereby allowing sufficient information to perform quantitative data analysis diffraction via in-house software (WBXRD_GUI). Of current interest is the ability to evaluate crystal d-spacing, texture evolution and material phase transitions, all of which will be established from experiments performed at the aforementioned elevated strain-rates. C1 [Hudspeth, M.; Parab, N.; Guo, Z.; Chen, W.] Purdue Univ, W Lafayette, IN 47907 USA. [Sun, T.; Fezzaa, K.] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. [Luo, S.] Peac Inst Multiscale Sci, Chengdu 610207, Sichuan, Peoples R China. RP Chen, W (reprint author), Purdue Univ, W Lafayette, IN 47907 USA. EM wchen@purdue.edu RI Luo, Sheng-Nian /D-2257-2010 OI Luo, Sheng-Nian /0000-0002-7538-0541 FU Office of Naval Research [N0014-11-1-0840]; Air Force Research Laboratory [FA8651-13-2-0005]; US DOE [DE-AC02-06CH11357]; Department of Defense (DoD) through National Defense Science and Engineering Graduate Fellowship (NDSEG) Program FX The authors would like to thank B. J. Jensen at Los Alamos National Laboratory for the ICCD camera, and A. Deriy for his assistance with beamline instrumentation. This research was partially supported by Office of Naval Research through a grant (N0014-11-1-0840) and by Air Force Research Laboratory through a cooperative award (FA8651-13-2-0005) to Purdue University. Use of the Advanced Photon Source, an Office of Science User Facility operated for the US Department of Energy (DOE) Office of Science by Argonne National Laboratory, was supported by the US DOE under contract No. DE-AC02-06CH11357. MH was supported by the Department of Defense (DoD) through the National Defense Science and Engineering Graduate Fellowship (NDSEG) Program. NR 22 TC 4 Z9 4 U1 6 U2 25 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0909-0495 EI 1600-5775 J9 J SYNCHROTRON RADIAT JI J. Synchrot. Radiat. PD JAN PY 2015 VL 22 BP 49 EP 58 DI 10.1107/S1600577514022747 PN 1 PG 10 WC Instruments & Instrumentation; Optics; Physics, Applied SC Instruments & Instrumentation; Optics; Physics GA AX3PC UT WOS:000346850200009 PM 25537588 ER PT J AU Gu, WW Wang, HX Wang, K AF Gu, Weiwei Wang, Hongxin Wang, Kun TI Extended X-ray absorption fine structure and multiple-scattering simulation of nickel dithiolene complexes Ni[S2C2(CF3)(2)](2)(n) (n =-2,-1, 0) and an olefin adduct Ni[S2C2(CF3)(2)](2)(1-hexene) SO JOURNAL OF SYNCHROTRON RADIATION LA English DT Article DE Ni dithiolene complexes; olefin adduct; extended X-ray absorption fine structure (EXAFS); X-ray absorption near-edge structure (XANES); single scattering; multiple scattering ID DELOCALIZED GROUND STATES; DENSITY-FUNCTIONAL THEORY; CRYSTAL-STRUCTURE; COORDINATION COMPOUNDS; MODEL COMPOUNDS; K-EDGE; SPECTROSCOPY; HYDROGENASE; STANDARDS; PLATINUM AB A series of Ni dithiolene complexes Ni[S2C2(CF3)](2)(n) (n = -2, -1, 0) (1, 2, 3) and a 1-hexene adduct Ni[S2C2(CF3)(2)](2)(C6H12) (4) have been examined by Ni Kedge X-ray absorption near-edge structure (XANES) and extended X-ray absorption fine-structure (EXAFS) spectroscopies. Ni XANES for 1-3 reveals clear pre-edge features and approximately +0.7 eV shift in the Ni K-edge position for 'one-electron' oxidation. EXAFS simulation shows that the Ni-S bond distances for 1, 2 and 3 (2.11-2.16 angstrom) are within the typical values for square planar complexes and decrease by similar to 0.022 angstrom for each 'one-electron' oxidation. The changes in Ni K-edge energy positions and Ni-S distances are consistent with the 'non-innocent' character of the dithiolene ligand. The Ni-C interactions at similar to 3.0 angstrom are analyzed and the multiple-scattering parameters are also determined, leading to a better simulation for the overall EXAFS spectra. The 1-hexene adduct 4 presents no pre-edge feature, and its Ni K-edge position shifts by -0.8 eV in comparison with its starting dithiolene complex 3. Consistently, EXAFS also showed that the Ni-S distances in 4 elongate by similar to 0.046 angstrom in comparison with 3. The evidence confirms that the neutral complex is 'reduced' upon addition of olefin, presumably by olefin donating the pi-electron density to the LUMO of 3 as suggested by UV/visible spectroscopy in the literature. C1 [Gu, Weiwei; Wang, Hongxin] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA 94720 USA. [Gu, Weiwei] UC Berkeley Extens, Berkeley, CA 94704 USA. [Wang, Hongxin] Univ Calif Davis, Dept Chem, Davis, CA 95616 USA. [Wang, Kun] ExxonMobil Res & Engn Co, Corp Strateg Res, Annandale, NJ 08801 USA. RP Wang, HX (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, 1 Cyclotron Rd, Berkeley, CA 94720 USA. EM hxwang2@lbl.gov NR 39 TC 1 Z9 1 U1 0 U2 16 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0909-0495 EI 1600-5775 J9 J SYNCHROTRON RADIAT JI J. Synchrot. Radiat. PD JAN PY 2015 VL 22 BP 124 EP 129 DI 10.1107/S1600577514025041 PN 1 PG 6 WC Instruments & Instrumentation; Optics; Physics, Applied SC Instruments & Instrumentation; Optics; Physics GA AX3PC UT WOS:000346850200019 PM 25537598 ER PT J AU Rosenbaum, G Ginell, SL Chen, JCH AF Rosenbaum, Gerd Ginell, Stephan L. Chen, Julian C-H. TI Energy optimization of a regular macromolecular crystallography beamline for ultra-high-resolution crystallography SO JOURNAL OF SYNCHROTRON RADIATION LA English DT Article DE undulator; high energy; monochromator; harmonic ID CRYSTAL-STRUCTURE AB A practical method for operating existing undulator synchrotron beamlines at photon energies considerably higher than their standard operating range is described and applied at beamline 19-ID of the Structural Biology Center at the Advanced Photon Source enabling operation at 30 keV. Adjustments to the undulator spectrum were critical to enhance the 30 keV flux while reducing the lower-and higher-energy harmonic contamination. A Pd-coated mirror and Al attenuators acted as effective low-and high-bandpass filters. The resulting flux at 30 keV, although significantly lower than with X-ray optics designed and optimized for this energy, allowed for accurate data collection on crystals of the small protein crambin to 0.38 angstrom resolution. C1 [Rosenbaum, Gerd; Ginell, Stephan L.] Argonne Natl Lab, Struct Biol Ctr, Biosci Div, Argonne, IL 60439 USA. [Rosenbaum, Gerd] Univ Georgia, Dept Biochem & Mol Biol, Athens, GA 30602 USA. [Chen, Julian C-H.] Univ Toledo, Dept Chem, Toledo, OH 43606 USA. [Chen, Julian C-H.] Los Alamos Natl Lab, Biosci Div, Prot Crystallog Stn, Lujan Neutron Scattering Ctr, Los Alamos, NM 87545 USA. RP Chen, JCH (reprint author), Univ Toledo, Dept Chem, Toledo, OH 43606 USA. EM chen_j@lanl.gov FU US DOE-OBER [DE-AC02-06CH11357] FX The authors thank Dr Andrzej Joachimiak for helpful comments and discussions. This work was supported by US DOE-OBER, DE-AC02-06CH11357. NR 5 TC 2 Z9 2 U1 1 U2 2 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0909-0495 EI 1600-5775 J9 J SYNCHROTRON RADIAT JI J. Synchrot. Radiat. PD JAN PY 2015 VL 22 BP 172 EP 174 DI 10.1107/S1600577514022619 PN 1 PG 3 WC Instruments & Instrumentation; Optics; Physics, Applied SC Instruments & Instrumentation; Optics; Physics GA AX3PC UT WOS:000346850200026 PM 25537605 ER PT J AU Li, LC Liu, HH AF Li, Lianchong Liu, Hui-Hai TI EDZ formation and associated hydromechanical behaviour around ED-B tunnel: A numerical study based on a two-part Hooke's model (TPHM) SO KSCE JOURNAL OF CIVIL ENGINEERING LA English DT Article DE numerical simulation; failure process; constitutive model; excavation damaged zone; heterogeneity ID ELASTOPLASTIC CELLULAR-AUTOMATON; LOCAL DEGRADATION APPROACH; EXCAVATION-DISTURBED ZONE; DEPENDENT ELASTIC-MODULI; HETEROGENEOUS ROCKS; STABILITY ANALYSIS; FRACTURED ROCK; OPALINUS CLAY; DAMAGED ZONE; FLUID-FLOW AB The accuracy in modeling coupled processes in a clay/shale repository is largely determined by the validity of the constitutive relationships and related parameter values. As an attempt to more accurately model the Excavation Damaged Zone (EDZ) formation and associated hydromechanical behavior induced by excavation in clay/shale, a recently developed stress-strain relationship (a twopart Hooke's model, abbreviated as TPHM) and associated formulations regarding rock hydraulic/mechanical properties were incorporated and implemented in FLAC3D in detail. TPHM is based on a macroscopic-scale approximation using a natural-strainbased Hooke's law to describe elastic deformation for a fraction of pores subject to a large degree of deformation; an engineeringstrain-based Hooke's law is used for the other part. The usefulness and validity of the TPHM and associated formulations are demonstrated by the consistency between simulation results and field observations from the ED-B tunnel at the Mont Terri site. The simulation results, which are sensitive to the constitutive relationships used in the model, capture both the observed displacements and the size of the damage zone, whereas the approach based on the conventional Hooke's law underestimates both. The fracture modeling provide insight into the evolution of fractured zone that are impossible to be observed in field and are difficult to be considered with static stress analysis approaches. C1 [Li, Lianchong] Dalian Univ Technol, Sch Civil Engn, Dalian 116024, Peoples R China. [Liu, Hui-Hai] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, Berkeley, CA 94720 USA. RP Li, LC (reprint author), Dalian Univ Technol, Sch Civil Engn, Dalian 116024, Peoples R China. EM li_lianchong@yahoo.com; hhliu@lbl.gov FU DOE [DE-AC02-05CH11231] FX The original version of this paper was reviewed by Drs. Daniel Hawkes and Liange Zheng at Lawrence Berkeley National Laboratory. Their constructive comments are appreciated. This work was funded by and conducted for the Used Fuel Disposition Campaign under DOE Contract No. DE-AC02-05CH11231. NR 75 TC 0 Z9 0 U1 5 U2 16 PU KOREAN SOCIETY OF CIVIL ENGINEERS-KSCE PI SEOUL PA 50-7 OGUM-DONG, SONGPA-KU, SEOUL, 138-857, SOUTH KOREA SN 1226-7988 EI 1976-3808 J9 KSCE J CIV ENG JI KSCE J. Civ. Eng. PD JAN PY 2015 VL 19 IS 1 BP 318 EP 331 DI 10.1007/s12205-014-0606-z PG 14 WC Engineering, Civil SC Engineering GA AY0KA UT WOS:000347284300035 ER PT J AU Bailey, JE Nagayama, T Loisel, GP Rochau, GA Blancard, C Colgan, J Cosse, P Faussurier, G Fontes, CJ Gilleron, F Golovkin, I Hansen, SB Iglesias, CA Kilcrease, DP MacFarlane, JJ Mancini, RC Nahar, SN Orban, C Pain, JC Pradhan, AK Sherrill, M Wilson, BG AF Bailey, J. E. Nagayama, T. Loisel, G. P. Rochau, G. A. Blancard, C. Colgan, J. Cosse, Ph. Faussurier, G. Fontes, C. J. Gilleron, F. Golovkin, I. Hansen, S. B. Iglesias, C. A. Kilcrease, D. P. MacFarlane, J. J. Mancini, R. C. Nahar, S. N. Orban, C. Pain, J-C. Pradhan, A. K. Sherrill, M. Wilson, B. G. TI A higher-than-predicted measurement of iron opacity at solar interior temperatures SO NATURE LA English DT Article ID DETAILED CONFIGURATION; PHOTOABSORPTION; RADIATION; MODELS; FILMS; ABUNDANCES; PLASMA; REGION; HOT; CR AB Nearly a century ago it was recognized(1) that radiation absorption by stellar matter controls the internal temperature profiles within stars. Laboratory opacity measurements, however, have never been performed at stellar interior conditions, introducing uncertainties in stellar models(2-5). A particular problem arose(2,3,6-8) when refined photosphere spectral analysis(9,10) led to reductions of 30-50 per cent in the inferred amounts of carbon, nitrogen and oxygen in the Sun. Standard solar models(11) using the revised element abundances disagree with helioseismic observations that determine the internal solar structure using acoustic oscillations. This could be resolved if the true mean opacity for the solar interior matter were roughly 15 per cent higher than predicted(2,3,6-8), because increased opacity compensates for the decreased element abundances. Iron accounts for a quarter of the total opacity(2,12) at the solar radiation/convection zone boundary. Here we report measurements of wavelength-resolved iron opacity at electron temperatures of 1.9-2.3 million kelvin and electron densities of (0.7-4.0) x 10(22) per cubic centimetre, conditions very similar to those in the solar region that affects the discrepancy the most: the radiation/convection zone boundary. The measured wavelength-dependent opacity is 30-400 per cent higher than predicted. This represents roughly half the change in the mean opacity needed to resolve the solar discrepancy, even though iron is only one of many elements that contribute to opacity. C1 [Bailey, J. E.; Nagayama, T.; Loisel, G. P.; Rochau, G. A.; Hansen, S. B.] Sandia Natl Labs, Albuquerque, NM 87185 USA. [Blancard, C.; Cosse, Ph.; Faussurier, G.; Gilleron, F.; Pain, J-C.] Commissariat Energie Atom CEA & Energie Alternat, F-91297 Arpajon, France. [Colgan, J.; Fontes, C. J.; Kilcrease, D. P.; Sherrill, M.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Golovkin, I.; MacFarlane, J. J.] Prism Computat Sci, Madison, WI 53711 USA. [Iglesias, C. A.; Wilson, B. G.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. [Mancini, R. C.] Univ Nevada, Reno, NV 89557 USA. [Nahar, S. N.; Orban, C.; Pradhan, A. K.] Ohio State Univ, Columbus, OH 43210 USA. RP Bailey, JE (reprint author), Sandia Natl Labs, 1515 Eubank SE, Albuquerque, NM 87185 USA. EM jebaile@sandia.gov OI Pain, Jean-Christophe/0000-0002-7825-1315; Kilcrease, David/0000-0002-2319-5934 FU United States Department of Energy [DE-AC04-94AL85000, DE-AC5206NA25396] FX Sandia is a multiprogramme laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the United States Department of Energy under contract DE-AC04-94AL85000. The Los AlamosNational Laboratory is operated by Los Alamos National Security, LLC, for the NNSA of the US DOE under contract number DE-AC5206NA25396. J. E. B. acknowledges support from a DOE High Energy Density Laboratory Plasmas grant. A. K. P. and C. O. also acknowledge support from a DOE High Energy Density Laboratory Plasmas grant. We appreciate the efforts of the entire Z facility team. We thank S. Turck-Chieze, H. Morris, and M. Pinsonneault for discussions. We also thank R. W. Lee for critiquing the manuscript. We appreciate support for the experiments provided by R. J. Leeper, J. L. Porter, M. K. Matzen and M. Herrmann. NR 41 TC 58 Z9 58 U1 6 U2 48 PU NATURE PUBLISHING GROUP PI LONDON PA MACMILLAN BUILDING, 4 CRINAN ST, LONDON N1 9XW, ENGLAND SN 0028-0836 EI 1476-4687 J9 NATURE JI Nature PD JAN 1 PY 2015 VL 517 IS 7532 BP 56 EP U120 DI 10.1038/nature14048 PG 12 WC Multidisciplinary Sciences SC Science & Technology - Other Topics GA AX8SI UT WOS:000347178400033 PM 25557711 ER PT J AU Aggarwal, PK Matsumoto, T Sturchio, NC Chang, HK Gastmans, D Araguas-Araguas, LJ Jiang, W Lu, ZT Mueller, P Yokochi, R Purtschert, R Torgersen, T AF Aggarwal, Pradeep K. Matsumoto, Takuya Sturchio, Neil C. Chang, Hung K. Gastmans, Didier Araguas-Araguas, Luis J. Jiang, Wei Lu, Zheng-Tian Mueller, Peter Yokochi, Reika Purtschert, Roland Torgersen, Thomas TI Continental degassing of He-4 by surficial discharge of deep groundwater SO NATURE GEOSCIENCE LA English DT Article ID NOBLE-GASES; RADIOGENIC HELIUM; OLD GROUNDWATER; TRANSPORT; AQUIFER; CRUST; USA; ACCUMULATION; MARYLAND; BUDGET AB Radiogenic He-4 is produced by the decay of uranium and thorium in the Earths mantle and crust. From here, it is degassed to the atmosphere(1-5) and eventually escapes to space(1,5,6). Assuming that all of the He-4 produced is degassed, about 70% of the total He-4 degassed from Earth comes from the continental crust(2,-5,7). However, the outgoing flux of crustal He-4 has not been directly measured at the Earths surface(2) and the migration pathways are poorly understood(2-4,7,8). Here we present measurements of helium isotopes and the long-lived cosmogenic radio-isotope Kr-81 in the deep, continental-scale Guarani aquifer in Brazil and show that crustal He-4 reaches the atmosphere primarily by the surficial discharge of deep groundwater. We estimate that He-4 in Guarani groundwater discharge accounts for about 20% of the assumed global flux from continental crust, and that other large aquifers may account for about 33%. Old groundwater ages suggest that He-4 in the Guarani aquifer accumulates over half- to one-million-year timescales. We conclude that He-4 degassing from the continents is regulated by groundwater discharge, rather than episodic tectonic events, and suggest that the assumed steady state between crustal production and degassing of He-4, and its resulting atmospheric residence time, should be re-examined. C1 [Aggarwal, Pradeep K.; Matsumoto, Takuya; Araguas-Araguas, Luis J.] IAEA, Isotope Hydrol Sect, A-1400 Vienna, Austria. [Sturchio, Neil C.] Univ Delaware, Dept Geol Sci, Newark, DE 19716 USA. [Chang, Hung K.; Gastmans, Didier] Univ Estadual Paulista, UNESP, CEA, BR-13506900 Rio Claro, SP, Brazil. [Chang, Hung K.; Gastmans, Didier] Univ Estadual Paulista, UNESP, LEBAC, BR-13506900 Rio Claro, SP, Brazil. [Jiang, Wei; Lu, Zheng-Tian; Mueller, Peter] Argonne Natl Lab, Div Phys, Argonne, IL 60439 USA. [Lu, Zheng-Tian] Univ Chicago, Dept Phys, Chicago, IL 60637 USA. [Lu, Zheng-Tian] Univ Chicago, Enrico Fermi Inst, Chicago, IL 60637 USA. [Yokochi, Reika] Univ Chicago, Dept Geophys Sci, Chicago, IL 60637 USA. [Purtschert, Roland] Univ Bern, Inst Phys, CH-3012 Bern, Switzerland. [Torgersen, Thomas] Natl Sci Fdn, Arlington, VA 22230 USA. RP Aggarwal, PK (reprint author), IAEA, Isotope Hydrol Sect, A-1400 Vienna, Austria. EM p.aggarwal@iaea.org RI Jiang, Wei/E-5582-2011; aggarwal, pradeep/C-8367-2016; Mueller, Peter/E-4408-2011; Purtschert, Roland/N-7108-2016 OI aggarwal, pradeep/0000-0001-5970-1408; Mueller, Peter/0000-0002-8544-8191; Purtschert, Roland/0000-0002-4734-7664 FU DOE, Office of Nuclear Physics [DE-AC02-06CH11357]; NSF [EAR-0651161] FX W.J., Z.-T.L, P.M. and the Laboratory Radiokrypton Dating at Argonne are supported by DOE, Office of Nuclear Physics, under contract DE-AC02-06CH11357. Development of the ATTA-3 instrument was supported in part by NSF EAR-0651161. C. Sambandam, L-E Han, D. Hillegonds, P. Klaus, S. Terzer and E. Izweski of IAEA assisted in noble gas analysis or with graphic illustrations. NR 31 TC 6 Z9 6 U1 7 U2 23 PU NATURE PUBLISHING GROUP PI NEW YORK PA 75 VARICK ST, 9TH FLR, NEW YORK, NY 10013-1917 USA SN 1752-0894 EI 1752-0908 J9 NAT GEOSCI JI Nat. Geosci. PD JAN PY 2015 VL 8 IS 1 BP 35 EP 39 DI 10.1038/NGEO2302 PG 5 WC Geosciences, Multidisciplinary SC Geology GA AX3FF UT WOS:000346825000012 ER PT J AU Baek, JS Cuadra, A Cheng, LY Hanson, AL Brown, NR Diamond, DJ AF Baek, J. S. Cuadra, A. Cheng, L. -Y. Hanson, A. L. Brown, N. R. Diamond, D. J. TI ANALYSIS OF LOSS-OF-FLOW ACCIDENTS FOR THE NIST RESEARCH REACTOR WITH FUEL CONVERSION FROM HEU TO LEU SO NUCLEAR TECHNOLOGY LA English DT Article DE loss-of-flow accident; research reactor conversion; NIST research reactor (NBSR) AB A program is underway to convert the current highenriched uranium (HEU) fuel to low-enriched uranium (LEU) fuel in the 20-MW D2O-moderated research reactor (NBSR) at the National Institute of Standards and Technology. A RELAP5 model has been developed to analyze postulated accidents in the NBSR with the present HEU fuel and a proposed LEU fuel. The model includes the reactor vessel, primary pumps, shutdown pumps, various valves, heat exchangers, and average and hottest fuel elements and flow channels in the region where flow enters through an inner plenum (6 fuel elements) and a region where flow enters through an outer plenum (24 elements). The equilibrium cycle power distributions in the fuel elements were determined based on three-dimensional Monte Carlo neutron transport calculations peiformed with the MCNPX code. In this paper we discuss safety analyses conducted for the loss-of-flow accidents resulting from either loss of electrical power or inadvertent throttling of flow control valves at the inlets to the inner and outer plena. The analysis shows that the fuel conversion will not lead to significant changes in the safety analysis and that the calculated maximum clad temperatures, minimum critical heat flux ratios, and minimum onset of flow instability ratios assure that there is adequate margin to fuel failure. C1 [Baek, J. S.; Cuadra, A.; Cheng, L. -Y.; Hanson, A. L.; Brown, N. R.; Diamond, D. J.] Brookhaven Natl Lab, Upton, NY 11973 USA. RP Baek, JS (reprint author), Brookhaven Natl Lab, 33 North Renaissance Rd,Bldg 817, Upton, NY 11973 USA. EM jbaek@bnl.gov FU National Nuclear Security Administration; NIST Center for Neutron Research (NCNR) at NIST FX This work was supported by the National Nuclear Security Administration and the NIST Center for Neutron Research (NCNR) at NIST. The authors appreciate the cooperation of S. O'Kelly and his staff at the NCNR. NR 12 TC 0 Z9 0 U1 1 U2 2 PU AMER NUCLEAR SOC PI LA GRANGE PK PA 555 N KENSINGTON AVE, LA GRANGE PK, IL 60526 USA SN 0029-5450 EI 1943-7471 J9 NUCL TECHNOL JI Nucl. Technol. PD JAN PY 2015 VL 189 IS 1 BP 71 EP 86 PG 16 WC Nuclear Science & Technology SC Nuclear Science & Technology GA AX5CJ UT WOS:000346944400006 ER PT J AU Nguyen, HT Park, H Koster, KL Cahoon, RE Nguyen, HTM Shanklin, J Clemente, TE Cahoon, EB AF Huu Tam Nguyen Park, Hyunwoo Koster, Karen L. Cahoon, Rebecca E. Nguyen, Hanh T. M. Shanklin, John Clemente, Thomas E. Cahoon, Edgar B. TI Redirection of metabolic flux for high levels of omega-7 monounsaturated fatty acid accumulation in camelina seeds SO PLANT BIOTECHNOLOGY JOURNAL LA English DT Article DE omega-7 fatty acid; monounsaturated fatty acid; oilseed; metabolic engineering; fatty acid; camelina ID AGROBACTERIUM-MEDIATED TRANSFORMATION; CAENORHABDITIS-ELEGANS; ARABIDOPSIS SEEDS; PALMITOLEIC ACID; RAPID METHOD; OILS; DESATURASE; SATIVA; TRIACYLGLYCEROLS; PROFILES AB Seed oils enriched in omega-7 monounsaturated fatty acids, including palmitoleic acid (16:19) and cis-vaccenic acid (18:111), have nutraceutical and industrial value for polyethylene production and biofuels. Existing oilseed crops accumulate only small amounts (<2%) of these novel fatty acids in their seed oils. We demonstrate a strategy for enhanced production of omega-7 monounsaturated fatty acids in camelina (Camelina sativa) and soybean (Glycine max) that is dependent on redirection of metabolic flux from the typical 9 desaturation of stearoyl (18:0)-acyl carrier protein (ACP) to 9 desaturation of palmitoyl (16:0)-acyl carrier protein (ACP) and coenzyme A (CoA). This was achieved by seed-specific co-expression of a mutant 9-acyl-ACP and an acyl-CoA desaturase with high specificity for 16:0-ACP and CoA substrates, respectively. This strategy was most effective in camelina where seed oils with similar to 17% omega-7 monounsaturated fatty acids were obtained. Further increases in omega-7 fatty acid accumulation to 60-65% of the total fatty acids in camelina seeds were achieved by inclusion of seed-specific suppression of 3-keto-acyl-ACP synthase II and the FatB 16:0-ACP thioesterase genes to increase substrate pool sizes of 16:0-ACP for the 9-acyl-ACP desaturase and by blocking C18 fatty acid elongation. Seeds from these lines also had total saturated fatty acids reduced to similar to 5% of the seed oil versus similar to 12% in seeds of nontransformed plants. Consistent with accumulation of triacylglycerol species with shorter fatty acid chain lengths and increased monounsaturation, seed oils from engineered lines had marked shifts in thermotropic properties that may be of value for biofuel applications. C1 [Huu Tam Nguyen; Park, Hyunwoo; Cahoon, Rebecca E.; Nguyen, Hanh T. M.; Clemente, Thomas E.; Cahoon, Edgar B.] Univ Nebraska, Ctr Plant Sci Innovat, Lincoln, NE 68588 USA. [Huu Tam Nguyen; Cahoon, Rebecca E.; Cahoon, Edgar B.] Univ Nebraska, Dept Biochem, Lincoln, NE 68583 USA. [Park, Hyunwoo; Nguyen, Hanh T. M.; Clemente, Thomas E.] Univ Nebraska, Dept Agron & Hort, Lincoln, NE USA. [Koster, Karen L.] Univ S Dakota, Dept Biol, Vermillion, SD 57069 USA. [Shanklin, John] Brookhaven Natl Lab, Dept Biosci, Upton, NY 11973 USA. RP Cahoon, EB (reprint author), Univ Nebraska, Ctr Plant Sci Innovat, Lincoln, NE 68588 USA. EM ecahoon2@unl.edu OI Koster, Karen/0000-0002-0462-7244 FU US Department of Agriculture-Agriculture and Food Research Initiative [2009-05988]; Nebraska Soybean Board; US DOE BES FX The project was supported by funding from the US Department of Agriculture-Agriculture and Food Research Initiative 2009-05988 and the Nebraska Soybean Board to TEC and EBC and support from the US DOE BES program to JS. We thank Manuel Rodriguez Rodriguez for expert technical assistance with oil thermal analysis. NR 33 TC 16 Z9 18 U1 4 U2 24 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 1467-7644 EI 1467-7652 J9 PLANT BIOTECHNOL J JI Plant Biotechnol. J. PD JAN PY 2015 VL 13 IS 1 BP 38 EP 50 DI 10.1111/pbi.12233 PG 13 WC Biotechnology & Applied Microbiology; Plant Sciences SC Biotechnology & Applied Microbiology; Plant Sciences GA AX4PW UT WOS:000346915000005 PM 25065607 ER PT J AU Sarma, GN Moody, IS Ilouz, R Phan, RH Sankaran, B Hall, RA Taylor, SS AF Sarma, Ganapathy N. Moody, Issa S. Ilouz, Ronit Phan, Ryan H. Sankaran, Banumathi Hall, Randy A. Taylor, Susan S. TI D-AKAP2:PKA RII:PDZK1 ternary complex structure: Insights from the nucleation of a polyvalent scaffold SO PROTEIN SCIENCE LA English DT Article DE PKA signaling; A-kinase anchoring proteins; D-AKAP2 specificity; AKAP10; PDZK1 crystal structure ID DEPENDENT PROTEIN-KINASE; ALPHA REGULATORY SUBUNIT; A ANCHORING PROTEIN; RECEPTOR CLASS-B; AKAP SPECIFICITY; CARNEY COMPLEX; PDZ DOMAINS; C-TERMINUS; SR-BI; BINDING AB A-kinase anchoring proteins (AKAPs) regulate cAMP-dependent protein kinase (PKA) signaling in space and time. Dual-specific AKAP2 (D-AKAP2/AKAP10) binds with high affinity to both RI and RII regulatory subunits of PKA and is anchored to transporters through PDZ domain proteins. Here, we describe a structure of D-AKAP2 in complex with two interacting partners and the exact mechanism by which a segment that on its own is disordered presents an -helix to PKA and a -strand to PDZK1. These two motifs nucleate a polyvalent scaffold and show how PKA signaling is linked to the regulation of transporters. Formation of the D-AKAP2: PKA binary complex is an important first step for high affinity interaction with PDZK1, and the structure reveals important clues toward understanding this phenomenon. In contrast to many other AKAPs, D-AKAP2 does not interact directly with the membrane protein. Instead, the interaction is facilitated by the C-terminus of D-AKAP2, which contains two binding motifsthe D-AKAP2(AKB) and the PDZ motifthat are joined by a short linker and only become ordered upon binding to their respective partner signaling proteins. The D-AKAP2(AKB) binds to the D/D domain of the R-subunit and the C-terminal PDZ motif binds to a PDZ domain (from PDZK1) that serves as a bridging protein to the transporter. This structure also provides insights into the fundamental question of why D-AKAP2 would exhibit a differential mode of binding to the two PKA isoforms. C1 [Sarma, Ganapathy N.; Moody, Issa S.; Phan, Ryan H.; Taylor, Susan S.] Univ Calif San Diego, Dept Chem & Biochem, La Jolla, CA 92093 USA. [Sarma, Ganapathy N.; Moody, Issa S.; Phan, Ryan H.; Taylor, Susan S.] Univ Calif San Diego, Dept Pharmacol, La Jolla, CA 92093 USA. [Ilouz, Ronit; Taylor, Susan S.] Univ Calif San Diego, Howard Hughes Med Inst, La Jolla, CA 92093 USA. [Sankaran, Banumathi] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley Ctr Struct Biol, Berkeley, CA 94720 USA. [Hall, Randy A.] Emory Univ, Dept Pharmacol, Rollins Res Ctr, Sch Med, Atlanta, GA 30322 USA. RP Taylor, SS (reprint author), Univ Calif San Diego, Dept Chem & Biochem, 9500 Gilman Dr,Mail Code 0654, La Jolla, CA 92093 USA. EM staylor@ucsd.edu FU NIH [DK054441, GM34921]; American Heart Association [0825041F] FX Grant sponsor: NIH; Grant number: DK054441 and GM34921; Grant sponsor: American Heart Association; Grant number: 0825041F. NR 41 TC 1 Z9 1 U1 0 U2 0 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0961-8368 EI 1469-896X J9 PROTEIN SCI JI Protein Sci. PD JAN PY 2015 VL 24 IS 1 BP 105 EP 116 DI 10.1002/pro.2593 PG 12 WC Biochemistry & Molecular Biology SC Biochemistry & Molecular Biology GA AX4PM UT WOS:000346914100011 PM 25348485 ER PT J AU Mikaelian, KO AF Mikaelian, K. O. TI Testing an analytic model for Richtmyer-Meshkov turbulent mixing widths SO SHOCK WAVES LA English DT Article DE Turbulent mix; Shocks; Reshocks; Rayleigh-Taylor; Richtmyer-Meshkov; National Shock-Tube Facility ID RAYLEIGH-TAYLOR INSTABILITY; NUMERICAL SIMULATIONS; AIR/SF6 INTERFACE; FLUIDS; ACCELERATION; PERTURBATIONS AB We discuss a model for the evolution of the turbulent mixing width after a shock or a reshock passes through the interface between two fluids of densities and inducing a velocity jump . In this model, the initial growth rate is independent of the surface finish or initial mixing width , but its duration is directly proportional to it: for , and for . Here is the Atwood number and are dimensionless, -dependent parameters measured in past Rayleigh-Taylor experiments, and is a new dimensionless parameter we introduce via . The mixing width and its derivative remain continuous at since and . We evaluate at from air/SF experiments and propose that the transition at signals isotropication of turbulence. We apply this model to the recent experiments of Jacobs et al. (Shock Waves 23:407-413, 2013) on shock and reshock, and discuss briefly the third wave causing an unstable acceleration of the interface. We also consider the experiments of Weber et al. (Phys Fluids 24:074105, 2012) and argue that their smaller growth rates reflect density gradient stabilization. C1 Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. RP Mikaelian, KO (reprint author), Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. EM mikaelian1@llnl.gov FU U.S. Department of Energy [DE-AC52-07NA27344] FX I am grateful to Jeff Jacobs and Vladimer Tsiklashvili for providing the data in Ref. [28], and to Chris Weber for a discussion of the data in [29,37]. This work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344. NR 60 TC 2 Z9 3 U1 6 U2 28 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 0938-1287 EI 1432-2153 J9 SHOCK WAVES JI Shock Waves PD JAN PY 2015 VL 25 IS 1 BP 35 EP 45 DI 10.1007/s00193-014-0537-0 PG 11 WC Mechanics SC Mechanics GA AX9WY UT WOS:000347251100004 ER PT J AU Grunder, Y Markovic, NM Thompson, P Lucas, CA AF Gruender, Yvonne Markovic, Nenad M. Thompson, Paul Lucas, Christopher A. TI Temperature effects on the atomic structure and kinetics in single crystal electrochemistry SO SURFACE SCIENCE LA English DT Article DE Electrochemistry; Electrodeposition; Gold; Surface structure; X-ray scattering ID X-RAY-SCATTERING; SCANNING-TUNNELING-MICROSCOPY; HIGH-RESOLUTION DIFFRACTION; UNDERPOTENTIAL DEPOSITION; ANION ADSORPTION; AU(111) SURFACE; ELECTROLYTE INTERFACE; ALKALINE ELECTROLYTE; ADSORBED BROMIDE; CARBON-MONOXIDE AB The influence of temperature on the atomic structure at the electrochemical interface has been studied using in-situ surface x-ray scattering (SXS) during the formation of metal monolayers on a Au(111) electrode. For the surface reconstruction of Au(111), higher temperatures increase the mobility of surface atoms in the unreconstructed phase which then determines the surface ordering during the formation of the reconstruction. For the underpotential deposition (UPD) systems, the surface diffusion of the depositing metal adatoms is significantly reduced at low temperatures which results in the frustration of ordered structures in the case of Cu UPD, occurring on a Br-modified surface, and in the formation of a disordered Ag monolayer during Ag UPD. The results indicate that temperature changes affect the mass transport and diffusion of metal adatoms on the electrode surface. This demonstrates the importance of including temperature as a variable in studying surface structure and reactions at the electrochemical interface. (C) 2014 Elsevier B.V. All rights reserved. C1 [Gruender, Yvonne; Thompson, Paul; Lucas, Christopher A.] Univ Liverpool, Dept Phys, Oliver Lodge Lab, Liverpool L69 7ZE, Merseyside, England. [Markovic, Nenad M.] Argonne Natl Lab, Div Mat Sci, Argonne, IL 60439 USA. RP Grunder, Y (reprint author), Univ Liverpool, Dept Phys, Oliver Lodge Lab, Liverpool L69 7ZE, Merseyside, England. EM grunder@liv.ac.uk; clucas@liv.ac.uk RI Grunder, Yvonne/C-6137-2011; OI Grunder, Yvonne/0000-0002-5295-0927; Lucas, Christopher/0000-0001-5743-3868 FU U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-76SF00515]; EPSRC (UK); U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences (BES), Materials Sciences and Engineering Division [DE-AC02-06CH11357]; Royal Society (UK) through a University Research Fellowship [UF120123] FX We would like to thank the XMaS beamline staff for their support of the XMaS beamline, Paul Steadman for his support during the experiments at beamline ID3 at the ESRF, Nadia Leyarovska and Sungsik Lee for their support of BM12-BESSRC at the APS and Sean Brennan for all of the assistance that he has given with the operation of beamline 7-2 at SSRL. The use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515. The XMaS beamline is an EPSRC mid-range facility managed by the University of Liverpool and the University of Warwick We would like to thank a number of PhD students at the University of Liverpool for their contribution to this work In chronological order they are Stuart Medway, Mark Gallagher, Ben Fowler, Dave Mercer, Mick Cormack, Alex Brownrigg and Naomi Sisson. YG, PT and CAL acknowledge the financial support of the EPSRC (UK). NMM is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences (BES), Materials Sciences and Engineering Division, under contract DE-AC02-06CH11357 YG acknowledges the financial support of the Royal Society (UK) through a University Research Fellowship UF120123. NR 63 TC 1 Z9 1 U1 3 U2 46 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0039-6028 EI 1879-2758 J9 SURF SCI JI Surf. Sci. PD JAN PY 2015 VL 631 SI SI BP 123 EP 129 DI 10.1016/j.susc.2014.06.022 PG 7 WC Chemistry, Physical; Physics, Condensed Matter SC Chemistry; Physics GA AY0CR UT WOS:000347266000018 ER PT J AU Anderson, BE Douma, J Ulrich, TJ Snieder, R AF Anderson, Brian E. Douma, Johannes Ulrich, T. J. Snieder, Roel TI Improving spatio-temporal focusing and source reconstruction through deconvolution SO WAVE MOTION LA English DT Article DE Time reversal; Signal processing; Communications ID TIME-REVERSAL; INVERSE FILTER; WAVE-FIELDS; MEDIA AB In this study, a technique is demonstrated to improve the ability of time reversal to both spatially and temporally focus, or compress, elastic wave energy, or to improve the quality of the reconstruction of the source signal. This method utilizes the deconvolution, or inverse filter, in single channel time reversal experiments in solids. Special attention is given to the necessary procedure for improving source signal reconstruction in real experimental conditions. It is also demonstrated theoretically and numerically that good temporal focusing implies that the radius in the spherically symmetric part of the spatial focus is small. (C) 2014 Elsevier B.V. All rights reserved. C1 [Anderson, Brian E.; Ulrich, T. J.] Los Alamos Natl Lab, Geophys Grp EES 17, Los Alamos, NM 87545 USA. [Douma, Johannes; Snieder, Roel] Colorado Sch Mines, Ctr Wave Phenomena, Golden, CO 80401 USA. RP Douma, J (reprint author), Colorado Sch Mines, Ctr Wave Phenomena, 1500 Illinois St, Golden, CO 80401 USA. EM bea@lanl.gov; jdouma@mines.edu FU Los Alamos National Laboratory Institutional Support (LDRD) [20120116ER] FX We would like to thank the anonymous reviewers for their critical and constructive comments. This work was supported by Los Alamos National Laboratory Institutional Support (LDRD), grant #20120116ER. NR 24 TC 6 Z9 6 U1 1 U2 5 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0165-2125 EI 1878-433X J9 WAVE MOTION JI Wave Motion PD JAN PY 2015 VL 52 BP 151 EP 159 DI 10.1016/j.wavemoti.2014.10.001 PG 9 WC Acoustics; Mechanics; Physics, Multidisciplinary SC Acoustics; Mechanics; Physics GA AX6GS UT WOS:000347021700012 ER PT J AU Peng, JH Wang, JS Bi, XT Lim, CJ Sokhansanj, S Peng, HC Jia, DN AF Peng, Jianghong Wang, Jingsong Bi, Xiaotao T. Lim, C. Jim Sokhansanj, Shahab Peng, Hanchao Jia, Dening TI Effects of thermal treatment on energy density and hardness of torrefied wood pellets SO FUEL PROCESSING TECHNOLOGY LA English DT Article DE Pellets; Torrefaction; Effect; Quality ID TORREFACTION; DENSIFICATION; RESIDUES; SAWDUST AB Three types of wood pellets samples, including two types of commercial pellets and one type of lab-made control pellets were torrefied in a fixed bed unit to study the effect of thermal pretreatment on the quality of wood pellets. The quality of wood pellets was mainly characterized by the pellet density, bulk density, higher heating value, Meyer hardness, saturated moisture uptake, volumetric energy density, and energy yield. Results showed that torrefaction significantly decreased the pellet density, hardness, volumetric energy density, and energy yield. The higher heating value increased and the saturated moisture content decreased after torrefaction. In view of the lower density, lower hardness, lower volumetric energy density, and energy yield of torrefied pellets, it is recommended that biomass should be torrefied and then compressed to make strong pellets of high hydrophobicity and volumetric energy density. (C) 2014 Elsevier B.V. All rights reserved. C1 [Peng, Jianghong; Wang, Jingsong; Bi, Xiaotao T.; Lim, C. Jim; Sokhansanj, Shahab; Peng, Hanchao; Jia, Dening] Univ British Columbia, Clean Energy Res Ctr, Vancouver, BC V6T 1Z3, Canada. [Wang, Jingsong] Univ British Columbia, Dept Chem & Biol Engn, Vancouver, BC V6T 1Z3, Canada. [Peng, Jianghong; Wang, Jingsong; Bi, Xiaotao T.; Lim, C. Jim; Sokhansanj, Shahab; Peng, Hanchao; Jia, Dening] Univ Sci & Technol Beijing, Sch Met & Ecol Engn, Beijing 100083, Peoples R China. [Sokhansanj, Shahab] Oak Ridge Natl Lab, Div Environm Sci, Oak Ridge, TN 37831 USA. [Peng, Hanchao] Univ Toronto, Dept Mineral Engn, Toronto, ON M5S 3E3, Canada. RP Bi, XT (reprint author), Univ British Columbia, Clean Energy Res Ctr, Vancouver, BC V6T 1Z3, Canada. EM xbi@chbe.ubc.ca OI Bi, Xiaotao/0000-0001-9514-3685; Jia, Dening/0000-0001-7515-5400 FU Natural Science and Engineering Research Council of Canada (NSERC) [STPGP430177]; University of British Columbia (project: ICON-Bio) FX The authors are grateful to the Natural Science and Engineering Research Council of Canada (NSERC) (project: STPGP430177) and the University of British Columbia (project: ICON-Bio) for financial support. NR 14 TC 2 Z9 2 U1 0 U2 31 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0378-3820 EI 1873-7188 J9 FUEL PROCESS TECHNOL JI Fuel Process. Technol. PD JAN PY 2015 VL 129 BP 168 EP 173 DI 10.1016/j.fuproc.2014.09.010 PG 6 WC Chemistry, Applied; Energy & Fuels; Engineering, Chemical SC Chemistry; Energy & Fuels; Engineering GA AX6HG UT WOS:000347023000021 ER PT J AU Zhang, TY Kumar, R Tsai, YD Elander, RT Wyman, CE AF Zhang, Taiying Kumar, Rajeev Tsai, Yueh-Du Elander, Richard T. Wyman, Charles E. TI Xylose yields and relationship to combined severity for dilute acid post- hydrolysis of xylooligomers from hydrothermal pretreatment of corn stover SO GREEN CHEMISTRY LA English DT Article ID SULFURIC-ACID; SUGAR YIELDS; ENZYMATIC-HYDROLYSIS; FRACTIONATION; CELLULOSE; LIGNOCELLULOSICS; SWITCHGRASS; HEMICELLULOSE; OPTIMIZATION; TECHNOLOGIES AB To maximize yields of fermentable xylose monomer from hydrothermal pretreatment of corn stover at 200 degrees C, the xylooligomers- rich liquor produced was post hydrolyzed with dilute sulfuric acid over a range of times and acid concentrations. The results showed that application of 0.75% H2SO4 at 110 degrees C for 180 min or 0.50% H2SO4 at 110 degrees C for 240 min recovered almost 100% of the total xylose from the oligomers. Furthermore, adjusting one constant in the combined severity parameter ( CSP) provided a rapid and accurate tool for trading off times, temperatures, and acid concentrations to reach the highest xylose yields from xylooligomers in hydrothermal pretreatment solutions. This adjusted CSP showed that an 8.4 degrees C temperature increase has the same impact as doubling the acid concentration or halving reaction time instead of the 10 degrees C change projected by the customary CSP and suggests that xylooligomers bonds are more easily broken than the hemicellulose from which they are derived. C1 [Tsai, Yueh-Du; Wyman, Charles E.] Univ Calif Riverside, Bourns Coll Engn, Dept Chem & Environm Engn, Riverside, CA 92521 USA. [Zhang, Taiying; Kumar, Rajeev; Tsai, Yueh-Du; Wyman, Charles E.] Univ Calif Riverside, Bourns Coll Engn, Ctr Environm Res & Technol CE CERT, Riverside, CA 92507 USA. [Elander, Richard T.] Natl Renewable Energy Lab, Natl Bioenergy Ctr, Golden, CO 80401 USA. RP Zhang, TY (reprint author), Univ Calif Riverside, Bourns Coll Engn, Ctr Environm Res & Technol CE CERT, 1084 Columbia Ave, Riverside, CA 92507 USA. EM charles.wyman@ucr.edu FU National Renewable Energy Laboratory [XGV-2-11467-01]; Ford Motor Company FX We are grateful to National Renewable Energy Laboratory for funding this research through Subcontract no. XGV-2-11467-01. We also acknowledge the Center for Environmental Research and Technology (CE-CERT) of the Bourns College of Engineering for providing facilities used in this research and the Ford Motor Company for funding the Chair in Environmental Engineering that facilitates projects such as this one. NR 45 TC 5 Z9 5 U1 7 U2 22 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9262 EI 1463-9270 J9 GREEN CHEM JI Green Chem. PY 2015 VL 17 IS 1 BP 394 EP 403 DI 10.1039/c4gc01283f PG 10 WC Chemistry, Multidisciplinary; GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY SC Chemistry; Science & Technology - Other Topics GA AX1ZJ UT WOS:000346742600041 ER PT J AU Wang, ZY Chen, BK Wang, JH Begovic, MM Chen, C AF Wang, Zhaoyu Chen, Bokan Wang, Jianhui Begovic, Miroslav M. Chen, Chen TI Coordinated Energy Management of Networked Microgrids in Distribution Systems SO IEEE TRANSACTIONS ON SMART GRID LA English DT Article DE Distributed generator (DG); distribution network; mathematical program with complementarity constraints (MPCC); Microgrid (MG) ID INTELLIGENT MICROGRIDS; MULTI-MICROGRIDS; UNIT COMMITMENT; GENERATION; OPERATION; REDUCTION; MARKET; COST AB This paper proposes a novel control strategy for coordinated operation of networked microgrids (MGs) in a distribution system. The distribution network operator (DNO) and each MG are considered as distinct entities with individual objectives to minimize the operation costs. It is assumed that both the dispatchable and nondispatchable distributed generators (DGs) exist in the networked MGs. In order to achieve the equilibrium among all entities and take into account the uncertainties of DG outputs, we formulate the problem as a stochastic bi-level problem with the DNO in the upper level and MGs in the lower level. Each level consists of two stages. The first stage is to determine base generation setpoints based on the load and nondispatchable DG output forecasts and the second stage is to adjust the generation outputs based on the realized scenarios. A scenario reduction method is applied to enhance a tradeoff between the accuracy of the solution and the computational burden. Case studies of a distribution system with multiple MGs of different types demonstrate the effectiveness of the proposed methodology. The centralized control, deterministic formulation, and stochastic formulation are also compared. C1 [Wang, Zhaoyu; Begovic, Miroslav M.] Georgia Inst Technol, Sch Elect & Comp Engn, Atlanta, GA 30332 USA. [Chen, Bokan] Iowa State Univ, Sch Ind & Mfg Syst Engn, Ames, IA 50014 USA. [Wang, Jianhui; Chen, Chen] Argonne Natl Lab, Decis & Informat Sci Div, Argonne, IL 60439 USA. RP Wang, ZY (reprint author), Georgia Inst Technol, Sch Elect & Comp Engn, Atlanta, GA 30332 USA. EM zhaoyuwang@gatech.edu; bokanc@iastate.edu; jianhui.wang@anl.gov; miroslav@ece.gatech.edu; morningchen@anl.gov FU U.S. Department of Energy Office of Science Laboratory [DE AC02-06CH11357] FX The submitted manuscript has been created by UChicago Argonne, LLC, Operator of Argonne National Laboratory ("Argonne"). Argonne, a U.S. Department of Energy Office of Science Laboratory, is operated under Contract DE AC02-06CH11357. The U.S. Government retains for itself, and others acting on its behalf, a paid-up nonexclusive, irrevocable worldwide license in said article to reproduce, prepare derivative works, distribute copies to the public, and perform publicly and display publicly, by or on behalf of the Government. NR 38 TC 43 Z9 47 U1 5 U2 28 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 1949-3053 EI 1949-3061 J9 IEEE T SMART GRID JI IEEE Trans. Smart Grid PD JAN PY 2015 VL 6 IS 1 BP 45 EP 53 DI 10.1109/TSG.2014.2329846 PG 9 WC Engineering, Electrical & Electronic SC Engineering GA AX1UM UT WOS:000346731400005 ER PT J AU Zhou, N Meng, D Huang, ZY Welch, G AF Zhou, Ning Meng, Da Huang, Zhenyu Welch, Greg TI Dynamic State Estimation of a Synchronous Machine Using PMU Data: A Comparative Study SO IEEE TRANSACTIONS ON SMART GRID LA English DT Article DE Ensemble Kalman filter (EnKF); extended Kalman filter (EKF); particle filter (PF); phasor measurement unit (PMU); power system dynamics; state estimation; unscented Kalman filter (UKF) ID POWER-SYSTEM AB Accurate information about dynamic states is important for efficient control and operation of a power system. This paper compares the performance of four Bayesian-based filtering approaches in estimating dynamic states of a synchronous machine using phasor measurement unit data. The four methods are extended Kalman filter, unscented Kalman filter, ensemble Kalman filter, and particle filter. The statistical performance of each algorithm is compared using Monte Carlo methods and a two-area-four-machine test system. Under the statistical framework, robustness against measurement noise and process noise, sensitivity to sampling interval, and computation time are evaluated and compared for each approach. Based on the comparison, this paper makes some recommendations for the proper use of the methods. C1 [Zhou, Ning] SUNY Binghamton, Dept Elect & Comp Engn, Binghamton, NY 13902 USA. [Meng, Da; Huang, Zhenyu] Pacific NW Natl Lab, Richland, WA 99352 USA. [Welch, Greg] Univ Cent Florida, Orlando, FL 32826 USA. [Welch, Greg] Univ N Carolina, Chapel Hill, NC 27599 USA. RP Zhou, N (reprint author), SUNY Binghamton, Dept Elect & Comp Engn, Binghamton, NY 13902 USA. EM ningzhou@binghamton.edu FU U.S. Department of Energy (DOE); DOE [DE-AC05-76RL01830] FX This work was supported in part by the U.S. Department of Energy (DOE) through its Advanced Grid Modeling Program and its Advanced Scientific Computing Research Applied Mathematics Program; and in part by the Pacific Northwest National Laboratory, operated by Battelle for DOE, under Contract DE-AC05-76RL01830. Paper no. TSG-00923-2013. NR 27 TC 6 Z9 6 U1 0 U2 2 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 1949-3053 EI 1949-3061 J9 IEEE T SMART GRID JI IEEE Trans. Smart Grid PD JAN PY 2015 VL 6 IS 1 BP 450 EP 460 DI 10.1109/TSG.2014.2345698 PG 11 WC Engineering, Electrical & Electronic SC Engineering GA AX1UM UT WOS:000346731400045 ER PT J AU Ke, XD Lu, N Jin, CL AF Ke, Xinda Lu, Ning Jin, Chunlian TI Control and Size Energy Storage Systems for Managing Energy Imbalance of Variable Generation Resources SO IEEE TRANSACTIONS ON SUSTAINABLE ENERGY LA English DT Article DE Ancillary service; energy management; energy storage; operation scheduling; renewable integration; wind forecast ID WIND; BATTERY AB This paper presents control algorithms and sizing strategies for using energy storage to manage energy imbalance for variable generation resources. The control objective is to minimize the hourly generation imbalance between the actual and the scheduled generation of wind farms. Three control algorithms are compared: 1) tracking minute-by-minute power imbalance; 2) postcompensation; and 3) precompensation. Measured data from a wind farm are used in the study. The results show that tracking minute-by-minute power imbalance achieves the best performance by keeping hourly energy imbalance zero. However, the energy storage system (ESS) will be significantly oversized. Postcompensation reduces the power rating of the ESS but the hourly energy imbalance may not be reduced to zero when a large and long-lasting power imbalance occurs. A linear regression forecasting algorithm is developed for a two-stage precompensation algorithm to precharge or predischarge the ESS based on the predicted energy imbalance. An equivalent charge cycle estimation method is proposed to evaluate the effect of providing the energy balancing service on battery life. The performance comparison shows that the precompensation method reduces the size of the ESS by 30% with satisfactory performance. C1 [Ke, Xinda; Lu, Ning] N Carolina State Univ, Dept Elect & Comp Engn, Future Renewable Elect Energy Delivery & Manageme, Raleigh, NC 27606 USA. [Jin, Chunlian] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Ke, XD (reprint author), N Carolina State Univ, Dept Elect & Comp Engn, Future Renewable Elect Energy Delivery & Manageme, Raleigh, NC 27606 USA. EM xke@ncsu.edu; nlu2@ncsu.edu; julie.jin@ercot.com FU U.S. Department of Energy [DE-AC05-76RL01830]; NSF FREEDM Center at North Carolina State University FX This work was supported in part by the U.S. Department of Energy under Grant DE-AC05-76RL01830 and in part by the NSF FREEDM Center at North Carolina State University. Paper no. TSTE-00162-2014. NR 22 TC 12 Z9 12 U1 0 U2 9 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 1949-3029 J9 IEEE T SUSTAIN ENERG JI IEEE Trans. Sustain. Energy PD JAN PY 2015 VL 6 IS 1 BP 70 EP 78 DI 10.1109/TSTE.2014.2355829 PG 9 WC GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY; Energy & Fuels; Engineering, Electrical & Electronic SC Science & Technology - Other Topics; Energy & Fuels; Engineering GA AX1WE UT WOS:000346733200008 ER PT J AU Tucker, MC Cho, KT Weber, AZ Lin, GY Nguyen, TV AF Tucker, Michael C. Cho, Kyu Taek Weber, Adam Z. Lin, Guangyu Trung Van Nguyen TI Optimization of electrode characteristics for the Br-2/H-2 redox flow cell SO JOURNAL OF APPLIED ELECTROCHEMISTRY LA English DT Article DE Redox flow cell; Bromine; Flow battery; Hydrogen bromine ID H-2/BR-2 FUEL-CELL; SCALE ENERGY-STORAGE; BROMINE; BATTERIES; NAFION AB The Br-2/H-2 redox flow cell shows promise as a high-power, low-cost energy storage device. The effect of various aspects of material selection, processing, and assembly of electrodes on the operation, performance, and efficiency of the system is determined. In particular, (+) electrode thickness, cell compression, hydrogen pressure, and (-) electrode architecture are investigated. Increasing hydrogen pressure and depositing the (-) catalyst layer on the membrane instead of on the carbon paper backing layers have a large positive impact on performance, enabling a limiting current density above 2 A cm(-2) and a peak power density of 1.4 W cm(-2). Maximum energy efficiency of 79 % is achieved. In addition, the root cause of limiting-current behavior in this system is elucidated, where it is found that Br- reversibly adsorbs at the Pt (-) electrode for potentials exceeding a critical value, and the extent of Br- coverage is potential-dependent. This phenomenon limits maximum cell current density and must be addressed in system modeling and design. These findings are expected to lower system cost and enable higher efficiency. C1 [Tucker, Michael C.; Weber, Adam Z.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. [Cho, Kyu Taek] No Illinois Univ, Dept Mech Engn, De Kalb, IL 60115 USA. [Lin, Guangyu] TVN Syst Inc, Lawrence, KS USA. [Trung Van Nguyen] Univ Kansas, Lawrence, KS 66045 USA. RP Tucker, MC (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. EM MCTucker@lbl.gov FU Advanced Research Projects Agency-Energy (ARPA-E) of the U.S. Department of Energy [DE-AC02-05CH11231, DE-AR0000262] FX The authors acknowledge helpful discussion with Venkat Srinivasan and Vincent Battaglia. This work was funded by Advanced Research Projects Agency-Energy (ARPA-E) of the U.S. Department of Energy (contract nos. DE-AC02-05CH11231 for LBNL and DE-AR0000262 for TVN Systems, Inc.) with cost share provided by TVN Systems, Inc. NR 22 TC 13 Z9 13 U1 6 U2 38 PU SPRINGER PI DORDRECHT PA VAN GODEWIJCKSTRAAT 30, 3311 GZ DORDRECHT, NETHERLANDS SN 0021-891X EI 1572-8838 J9 J APPL ELECTROCHEM JI J. Appl. Electrochem. PD JAN PY 2015 VL 45 IS 1 BP 11 EP 19 DI 10.1007/s10800-014-0772-1 PG 9 WC Electrochemistry SC Electrochemistry GA AX6JZ UT WOS:000347029900002 ER PT J AU James, LRA Xu, ZQ Sluyter, R Hawksworth, EL Kelso, C Lai, B Paterson, DJ de Jonge, MD Dixon, NE Beck, JL Ralph, SF Dillon, CT AF James, Lloyd R. A. Xu, Zhi-Qiang Sluyter, Ronald Hawksworth, Emma L. Kelso, Celine Lai, Barry Paterson, David J. de Jonge, Martin D. Dixon, Nicholas E. Beck, Jennifer L. Ralph, Stephen F. Dillon, Carolyn T. TI An investigation into the interactions of gold nanoparticles and anti-arthritic drugs with macrophages, and their reactivity towards thioredoxin reductase SO JOURNAL OF INORGANIC BIOCHEMISTRY LA English DT Article DE Gold nanoparticles; Thioredoxin reductase; Macrophages; Rheumatoid arthritis; Gold complexes ID NECROSIS-FACTOR-ALPHA; HUMAN SERUM-ALBUMIN; RHEUMATOID-ARTHRITIS; SODIUM THIOMALATE; MASS-SPECTROMETRY; COORDINATION-COMPLEXES; SILVER NANOPARTICLES; ANTIRHEUMATIC DRUGS; CANCER-CELLS; AURANOFIN AB Gold(I) complexes are an important tool in the arsenal of established approaches for treating rheumatoid arthritis (RA), while some recent studies have suggested that gold nanoparticles (Au NPs) may also be therapeutically efficacious. These observations prompted the current biological studies involving gold(I) anti-RA agents and Au NPs, which are aimed towards improving our knowledge of how they work. The cytotoxicity of auranofin, aurothiomalate, aurothiosulfate and Au NPs towards RAW264.7 macrophages was evaluated using the MIT assay, with the former compound proving to be the most toxic. The extent of cellular uptake of the various gold agents was determined using graphite furnace atomic absorption spectrometry, while their distribution within macrophages was examined using microprobe synchrotron radiation X-ray fluorescence spectroscopy. The latter technique showed accumulation of gold in discrete regions of the cell, and co-localisation with sulfur in the case of cells treated with aurothiomalate or auranofin. Electrospray ionization mass spectrometry was used to characterize thioredoxin reductase (TrxR) in which the penultimate selenocysteine residue was replaced by cysteine. Mass spectra of solutions of TrxR and aurothiomalate, aurothiosulfate or auranofin showed complexes containing bare gold atoms bound to the protein, or protein adducts containing gold atoms retaining some of their initial ligands. These results support TrxR being an important target of gold(I) drugs used to treat RA, while the finding that Au NPs are incorporated into macrophages, but elicit little toxicity, indicates further exploration of their potential for treatment of RA is warranted. (C) 2014 Elsevier Inc. All rights reserved. C1 [James, Lloyd R. A.; Xu, Zhi-Qiang; Sluyter, Ronald; Hawksworth, Emma L.; Kelso, Celine; Dixon, Nicholas E.; Beck, Jennifer L.; Ralph, Stephen F.; Dillon, Carolyn T.] Univ Wollongong, Ctr Med & Mol Biosci, Wollongong, NSW 2522, Australia. [James, Lloyd R. A.; Xu, Zhi-Qiang; Hawksworth, Emma L.; Kelso, Celine; Dixon, Nicholas E.; Beck, Jennifer L.; Ralph, Stephen F.; Dillon, Carolyn T.] Univ Wollongong, Sch Chem, Wollongong, NSW 2522, Australia. [Sluyter, Ronald] Univ Wollongong, Sch Biol Sci, Wollongong, NSW 2522, Australia. [Sluyter, Ronald; Dixon, Nicholas E.; Dillon, Carolyn T.] Illawarra Hlth & Med Res Inst, Wollongong, NSW 2522, Australia. [Lai, Barry] Argonne Natl Lab, Adv Photon Source, Xray Sci Div, Argonne, IL 60439 USA. [Paterson, David J.; de Jonge, Martin D.] Australian Synchrotron, Clayton, Vic 3168, Australia. RP Dillon, CT (reprint author), Univ Wollongong, Sch Chem, Wollongong, NSW 2522, Australia. EM carolynd@uow.edu.au RI de Jonge, Martin/C-3400-2011; Beck, Jennifer/B-6151-2016; Kelso, Celine/E-2679-2016; James, Lloyd/B-7127-2012; OI Beck, Jennifer/0000-0001-6058-4886; James, Lloyd/0000-0002-1163-7395; Dixon, Nicholas/0000-0002-5958-6945; Sluyter, Ronald/0000-0003-4909-686X FU U.S. Department of Energy Office of Science [DE-AC02-06CH11357]; International Synchrotron Access Program; University of Wollongong [LE0453832]; Australian Postgraduate Award FX The use of the XFM beamline at the Australian Synchrotron was supported by that facility. Use of APS was supported by the U.S. Department of Energy Office of Science under Contract No. DE-AC02-06CH11357. CTD acknowledges travel funding provided by the International Synchrotron Access Program managed by the Australian Synchrotron. The authors acknowledge the Australian Research Council and the University of Wollongong for the mass spectrometers used in this work (Q-ToF Ultima, LIEF grant LE0453832), and thank Tony Romeo for performing the FESEM and Yan-Chung Lo and Andrew Wang (Academia Sinica, Taiwan) for the TrxR plasmid. LRAJ was supported by an Australian Postgraduate Award. NR 65 TC 4 Z9 4 U1 2 U2 42 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 0162-0134 EI 1873-3344 J9 J INORG BIOCHEM JI J. Inorg. Biochem. PD JAN PY 2015 VL 142 BP 28 EP 38 DI 10.1016/j.jinorgbio.2014.09.013 PG 11 WC Biochemistry & Molecular Biology; Chemistry, Inorganic & Nuclear SC Biochemistry & Molecular Biology; Chemistry GA AX4CA UT WOS:000346880400004 PM 25306263 ER PT J AU Dassanayake, RS Cabelli, DE Brasch, NE AF Dassanayake, Rohan S. Cabelli, Diane E. Brasch, Nicola E. TI Pulse radiolysis studies of the reactions of nitrogen dioxide with the vitamin B-12 complexes cob(II)alamin and nitrocobalamin SO JOURNAL OF INORGANIC BIOCHEMISTRY LA English DT Article DE Vitamin B-12; Cobalamins; Nitrogen dioxide; Pulse radiolysis; Nitrosative stress ID AQUEOUS-SOLUTION; NITRIC-OXIDE; TYROSINE NITRATION; PEROXYNITROUS ACID; SCARLET PIMPERNEL; HYDROGEN-PEROXIDE; RADICALS; KINETICS; COBALAMINS; MYELOPEROXIDASE AB Although now recognized to be an important reactive nitrogen species in biological systems that modifies the structures of proteins, DNA and lipids, there are few studies on the reactivity of (NO2)-N-center dot, including the reactions between (NO2)-N-center dot and transition metal complexes. We report kinetic studies on the reactions of (NO2)-N-center dot with two forms of vitamin B-12 - cob(II)alamin and nitrocobalamin. UV-visible spectroscopy and HPLC analysis of the product solution show that (NO2)-N-center dot cleanly oxidizes the metal center of cob(II)alamin to form nitrocobalamin, with a second-order rate constant of (3.5 +/- 0.3) x 10(8) M-1 s(-1) (pH 7.0 and 9.0, room temperature, I = 0.20 M). The stoichiometry of the reaction is 1:1. No reaction is detected by UV-visible spectroscopy and HPLC analysis of the product solution when nitrocobalamin is exposed to up to 2.0 mol equiv. (NO2)-N-center dot. (C) 2014 Published by Elsevier Inc. C1 [Dassanayake, Rohan S.] Kent State Univ, Dept Chem & Biochem, Kent, OH 44242 USA. [Cabelli, Diane E.] Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA. [Brasch, Nicola E.] Auckland Univ Technol, Sch Appl Sci, Auckland 1142, New Zealand. RP Brasch, NE (reprint author), Auckland Univ Technol, Sch Appl Sci, Private Bag 92006, Auckland 1142, New Zealand. EM nbrasch@autac.nz FU US National Institute of General Medical Sciences of the National Institutes of Health [1R15GM094707-01A1]; U.S. DOE Office of Science, Division of Chemical Sciences, Geosciences and Biosciences [DE-AC02-98CH10886] FX This research was funded by the US National Institute of General Medical Sciences of the National Institutes of Health under award number 1R15GM094707-01A1. The content is solely the responsibility of the authors and does not necessarily represent the official views of the National Institutes of Health. The work at Brookhaven National lab was carried out at the Accelerator Center for Energy Research, which is supported by the U.S. DOE Office of Science, Division of Chemical Sciences, Geosciences and Biosciences under contract no. DE-AC02-98CH10886. NR 40 TC 4 Z9 4 U1 1 U2 11 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 0162-0134 EI 1873-3344 J9 J INORG BIOCHEM JI J. Inorg. Biochem. PD JAN PY 2015 VL 142 BP 54 EP 58 DI 10.1016/j.jinorgbio.2014.09.014 PG 5 WC Biochemistry & Molecular Biology; Chemistry, Inorganic & Nuclear SC Biochemistry & Molecular Biology; Chemistry GA AX4CA UT WOS:000346880400007 PM 25450018 ER PT J AU Lekivetz, R Sitter, R Bingham, D Hamada, MS Moore, LM Wendelberger, JR AF Lekivetz, R. Sitter, R. Bingham, D. Hamada, M. S. Moore, L. M. Wendelberger, J. R. TI On Algorithms for Obtaining Orthogonal and Near-Orthogonal Arrays for Main-Effects Screening SO JOURNAL OF QUALITY TECHNOLOGY LA English DT Article DE Column-Wise; Near-Orthogonality Criteria; Sequential Element-Wise; Two-Level, Multi-Level, and Mixed-Level Orthogonal Designs ID SUPERSATURATED DESIGNS; MIXED LEVELS; FACTORIAL-DESIGNS; SMALL RUNS; CONSTRUCTION; ABERRATION; SELECTION; LEVEL AB Screening designs for identifying active main effects among a group of factors are frequently used by experimenters. Methods for efficiently designing experiments that estimate main effects are needed, particularly if the experiment involves categorical factors at more than two levels and requires a nonstandard run size. We propose a new and powerful algorithm based on a sequential element-wise-column-wise strategy that focuses on maintaining balance within and between columns. We compare the new algorithm with a column-wise algorithm for finding some selected orthogonal and near-orthogonal arrays. We examine the performance of both algorithms using different criteria and provide a discussion of general strategies in searching for designs. C1 [Lekivetz, R.] JMP Div SAS, Cary, NC 27513 USA. [Sitter, R.; Bingham, D.] Simon Fraser Univ, Dept Stat & Actuarial Sci, Burnaby, BC V5A 1S6, Canada. [Hamada, M. S.; Moore, L. M.; Wendelberger, J. R.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Lekivetz, R (reprint author), JMP Div SAS, Cary, NC 27513 USA. EM ryan.lekivetz@jmp.com; dbingham@stat.sfu.ca; hamada@lanl.gov; lmm.ind1@yahoo.com; joanne@lanl.gov FU Natural Sciences and Engineering Research Council of Canada FX The authors would like to thank C. C. Essix for her encouragement and support. The research of Bingham, Lekivetz and Sitter was supported by grants from the Natural Sciences and Engineering Research Council of Canada. We also thank the editor and an anonymous referee for many insightful comments and suggestions that improved the content and exposition of this article. We note with deep regret that our dear colleague Randy Sitter was tragically lost at sea on September 19, 2007. NR 18 TC 0 Z9 0 U1 2 U2 4 PU AMER SOC QUALITY CONTROL-ASQC PI MILWAUKEE PA 600 N PLANKINTON AVE, MILWAUKEE, WI 53203 USA SN 0022-4065 J9 J QUAL TECHNOL JI J. Qual. Technol. PD JAN PY 2015 VL 47 IS 1 BP 2 EP 13 PG 12 WC Engineering, Industrial; Operations Research & Management Science; Statistics & Probability SC Engineering; Operations Research & Management Science; Mathematics GA AX4EO UT WOS:000346886800002 ER PT J AU Cox, JT Marginean, I Smith, RD Tang, KQ AF Cox, Jonathan T. Marginean, Ioan Smith, Richard D. Tang, Keqi TI On the Ionization and Ion Transmission Efficiencies of Different ESI-MS Interfaces SO JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY LA English DT Article DE Electrospray ionization; Nanoelectrospray; Ion transmission; Ionization efficiency; ESI emitter array ID NANO-ELECTROSPRAY-IONIZATION; NANOELECTROSPRAY MASS-SPECTROMETRY; SUBAMBIENT PRESSURE IONIZATION; ASSISTED INLET IONIZATION; EMITTER ARRAYS; SENSITIVITY; MECHANISM AB The achievable sensitivity of electrospray ionization mass spectrometry (ESI-MS) is largely determined by the ionization efficiency in the ESI source and ion transmission efficiency through the ESI-MS interface. These performance characteristics are difficult to evaluate and compare across multiple platforms as it is difficult to correlate electrical current measurements to actual analyte ions reaching the detector of a mass spectrometer. We present an effective method to evaluate the overall ion utilization efficiency of an ESI-MS interface by measuring the total gas-phase ion current transmitted through the interface and correlating it to the observed ion abundance measured in the corresponding mass spectrum. Using this method, we systematically studied the ion transmission and ionization efficiencies of different ESI-MS interface configurations, including a single emitter/single inlet capillary, single emitter/multi-inlet capillary, and a subambient pressure ionization with nanoelectrospray (SPIN) MS interface with a single emitter and an emitter array, respectively. Our experimental results indicate that the overall ion utilization efficiency of SPIN-MS interface configurations exceeds that of the inlet capillary-based ESI-MS interface configurations. C1 [Cox, Jonathan T.; Marginean, Ioan; Smith, Richard D.; Tang, Keqi] Pacific NW Natl Lab, Div Biol Sci, Richland, WA 99352 USA. RP Tang, KQ (reprint author), Pacific NW Natl Lab, Div Biol Sci, POB 999, Richland, WA 99352 USA. EM keqi.tang@pnnl.gov RI Smith, Richard/J-3664-2012; Marginean, Ioan/A-4183-2008 OI Smith, Richard/0000-0002-2381-2349; Marginean, Ioan/0000-0002-6693-0361 FU NIH National Cancer Institute [1R33CA155252]; General Medical Sciences [GM103493-12]; Laboratory Directed Research and Development Program at Pacific Northwest National Laboratory (PNNL); Department of Energy Office of Biological and Environmental Research Genome Sciences Program under the Pan-omics project; DOE [DE-AC05-76RLO01830] FX The authors thank Dr. Ryan T. Kelly and Dr. Yehia Ibrahim for useful discussions. Portions of this research were supported by the NIH National Cancer Institute (1R33CA155252) and General Medical Sciences (GM103493-12), the Laboratory Directed Research and Development Program at Pacific Northwest National Laboratory (PNNL), and the Department of Energy Office of Biological and Environmental Research Genome Sciences Program under the Pan-omics project. All the experiments were performed in the Environmental Molecular Sciences Laboratory, a US Department of Energy (DOE) national scientific user facility located at PNNL in Richland, Washington. PNNL is a multiprogramming national laboratory operated by Battelle for the DOE under contract DE-AC05-76RLO01830. NR 37 TC 4 Z9 5 U1 9 U2 63 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1044-0305 EI 1879-1123 J9 J AM SOC MASS SPECTR JI J. Am. Soc. Mass Spectrom. PD JAN PY 2015 VL 26 IS 1 BP 55 EP 62 DI 10.1007/s13361-014-0998-5 PG 8 WC Biochemical Research Methods; Chemistry, Analytical; Chemistry, Physical; Spectroscopy SC Biochemistry & Molecular Biology; Chemistry; Spectroscopy GA AX3SN UT WOS:000346859200008 PM 25267087 ER PT J AU Hennessy, C Tsai, CC Beasley, JC Beatty, WS Zollner, PA Rhodes, OE AF Hennessy, Cecilia Tsai, Chia-Chun Beasley, James C. Beatty, William S. Zollner, Patrick A. Rhodes, Olin E., Jr. TI Elucidation of Population Connectivity in Synanthropic Mesopredators: Using Genes to Define Relevant Spatial Scales for Management of Raccoons and Virginia Opossums SO JOURNAL OF WILDLIFE MANAGEMENT LA English DT Article DE Didelphis virginiana; dispersal; Indiana; isolation by distance; population structure; Procyon lotor ID HIGHLY FRAGMENTED LANDSCAPE; DIDELPHIS-VIRGINIANA; PROCYON-LOTOR; MATING SYSTEM; DISTANCE; ATTRIBUTES; DISPERSAL; PATTERNS; RABIES; FLOW AB Raccoons (Procyon lotor) and Virginia opossums (Didelphis virginiana) are highly abundant, synanthropic mesocarnivores that can transmit epizootic diseases of critical importance to human and livestock health such as rabies and tuberculosis. Individuals of both species can exhibit large dispersal distances and our understanding of population connectivity for both of these species is limited. Data on population connectivity and potential for disease transmission are needed for each of these species for the development of data-informed management, control, and vaccination programs. Genetic connectivity among populations can be estimated by evaluation of metrics such as of isolation by distance (IBD) signatures and population structure. Such metrics are influenced not only by geographic distance and barriers to dispersal but also by the life-history characteristics of the species in question. We investigated the scale at which these species exhibited evidence of connectivity via gene flow, using samples collected from 9 sites spanning 254km across north-central, west-central, south-central, and southern Indiana, USA. We evaluated genetic connectivity and signatures of IBD using Bayesian clustering analyses and matrix correlation methods. In the Bayesian model, raccoons were assigned to 3 genetic clusters, whereas Virginia opossums exhibited apparent panmixia. Spatial autocorrelation results indicated a significant positive correlation between genetic and geographic distance for raccoons at distances up to 25km and for Virginia opossums up to 4km. Interspecific differences in reproductive biology, social behavior, and dispersal are likely the causes for differences between these 2 species in the spatial partitioning of populations across broad ranges. In addition, geographic features and past glaciation events may be affecting the genetic characteristics of present-day raccoon populations. Improved information regarding interpopulation distance for these 2 synanthropic species may contribute to more effective management and disease-control programs. (c) 2014 The Wildlife Society. C1 [Hennessy, Cecilia; Tsai, Chia-Chun; Beatty, William S.; Zollner, Patrick A.] Purdue Univ, Dept Forestry & Nat Resources, W Lafayette, IN 47907 USA. [Beasley, James C.; Rhodes, Olin E., Jr.] Univ Georgia, Savannah River Ecol Lab, Aiken, SC 29802 USA. RP Hennessy, C (reprint author), Purdue Univ, Dept Forestry & Nat Resources, 715 W State St, W Lafayette, IN 47907 USA. EM Cecilia.Hennessy@gmail.com RI Zollner, Patrick/A-8727-2010; OI Zollner, Patrick/0000-0001-8263-7029; Beatty, William/0000-0003-0013-3113 FU Indiana Department of Natural Resources Division of Fish and Wildlife [T07R04] FX We would like to thank V. Bennett, M. Cramer, G. Dharmarajan, J. Dumjahn, K. Kuitert, V. Clarkston, J. MacNeil, and V. Filer for assistance with field work. Many thanks to R. Swihart, K. Nichols, N. LaBonte ', E. Latch, and 3 anonymous reviewers for input on earlier versions of this manuscript. We gratefully acknowledge financial support via State Wildlife Research Grant T07R04 from the Indiana Department of Natural Resources Division of Fish and Wildlife, with special thanks to K. Smith, head of the Diversity Section. Purdue Department of Forestry and Natural Resources provided indispensible financial and logistical support. NR 58 TC 3 Z9 4 U1 6 U2 40 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0022-541X EI 1937-2817 J9 J WILDLIFE MANAGE JI J. Wildl. Manage. PD JAN PY 2015 VL 79 IS 1 BP 112 EP 121 DI 10.1002/jwmg.812 PG 10 WC Ecology; Zoology SC Environmental Sciences & Ecology; Zoology GA AW9YT UT WOS:000346611800013 ER PT J AU Vasdekis, AE Stephanopoulos, G AF Vasdekis, Andreas E. Stephanopoulos, Gregory TI Review of methods to probe single cell metabolism and bioenergetics SO METABOLIC ENGINEERING LA English DT Review DE Single cell analysis; Metabolism; Bioenergetics; Microfluidics; Microscopy ID RAMAN-SCATTERING MICROSCOPY; SCANNING ELECTROCHEMICAL MICROSCOPY; STRUCTURED-ILLUMINATION MICROSCOPY; MICROFLUIDIC DISSECTION PLATFORM; SYNAPTIC VESICLE EXOCYTOSIS; GENE-EXPRESSION DYNAMICS; ION MASS-SPECTROMETRY; REAL-TIME DETECTION; RED-BLOOD-CELLS; HIGH-THROUGHPUT AB Single cell investigations have enabled unexpected discoveries, such as the existence of biological noise and phenotypic switching in infection, metabolism and treatment. Herein, we review methods that enable such single cell investigations specific to metabolism and bioenergetics. Firstly, we discuss how to isolate and immobilize individuals from a cell suspension, including both permanent and reversible approaches. We also highlight specific advances in microbiology for its implications in metabolic engineering. Methods for probing single cell physiology and metabolism are subsequently reviewed. The primary focus therein is on dynamic and high-content profiling strategies based on label-free and fluorescence microspectroscopy and microscopy. Non-dynamic approaches, such as mass spectrometry and nuclear magnetic resonance, are also briefly discussed. (C) 2014 international Metabolic Engineering Society. Published by Elsevier Inc. All rights reserved. C1 [Vasdekis, Andreas E.] Pacific NW Natl Lab, Environm Mol Sci Lab, Richland, WA 99354 USA. [Stephanopoulos, Gregory] MIT, Dept Chem Engn, Cambridge, MA 02139 USA. RP Vasdekis, AE (reprint author), Univ Idaho, Dept Phys, Moscow, ID 83844 USA. EM andreasv@uidaho.edu; gregstep@mit.edu OI Vasdekis, Andreas/0000-0003-4315-1047 FU Pacific Northwest National Laboratory (LDRD) [PN12005/2406-Linus Pauling]; DOE, Genomic Sciences program [DE-SC0008744] FX AEV gratefully acknowledges funding support from the Pacific Northwest National Laboratory (LDRD project ID: PN12005/2406-Linus Pauling) and GS from the DOE, Genomic Sciences program Grant no. DE-SC0008744. We also wish to - in advance - apologize to those investigators and colleagues whose work was not cited herein due to space limitations. NR 363 TC 19 Z9 20 U1 17 U2 170 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 1096-7176 EI 1096-7184 J9 METAB ENG JI Metab. Eng. PD JAN PY 2015 VL 27 BP 115 EP 135 DI 10.1016/j.ymben.2014.09.007 PG 21 WC Biotechnology & Applied Microbiology SC Biotechnology & Applied Microbiology GA AX0NN UT WOS:000346649000014 PM 25448400 ER PT J AU Prabhakaran, R AF Prabhakaran, Ramprashad TI TMS 2013: Materials and Fuels for the Current and Advanced Nuclear Reactors II Foreword SO METALLURGICAL AND MATERIALS TRANSACTIONS A-PHYSICAL METALLURGY AND MATERIALS SCIENCE LA English DT Editorial Material C1 Pacific NW Natl Lab, Richland, WA 99352 USA. RP Prabhakaran, R (reprint author), Pacific NW Natl Lab, Richland, WA 99352 USA. EM ramprashad.prabhakaran@pnnl.gov NR 0 TC 0 Z9 0 U1 1 U2 5 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1073-5623 EI 1543-1940 J9 METALL MATER TRANS A JI Metall. Mater. Trans. A-Phys. Metall. Mater. Sci. PD JAN PY 2015 VL 46A IS 1 BP 46 EP 46 DI 10.1007/s11661-014-2626-1 PG 1 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Materials Science; Metallurgy & Metallurgical Engineering GA AX2QI UT WOS:000346788600010 ER PT J AU Park, Y Huang, K Puente, APY Lee, HS Sencer, BH Kennedy, JR Sohn, YH AF Park, Y. Huang, K. Paz y Puente, A. Lee, H. S. Sencer, B. H. Kennedy, J. R. Sohn, Y. H. TI Diffusional Interaction Between U-10 wt pct Zr and Fe at 903 K, 923 K, and 953 K (630 A degrees C, 650 A degrees C, and 680 A degrees C) SO METALLURGICAL AND MATERIALS TRANSACTIONS A-PHYSICAL METALLURGY AND MATERIALS SCIENCE LA English DT Article ID U-ZR; METALLIC FUELS; URANIUM; INTERDIFFUSION; REACTORS; BEHAVIOR; ALLOYS; IRON AB U-Zr metallic fuels cladded in Fe-alloys are being considered for application in an advanced sodium-cooled fast reactor that can recycle the U-Zr fuels and minimize the long-lived actinide waste. To understand the complex fuel-cladding chemical interaction between the U-Zr metallic fuels with Fe-alloys, a systematic multicomponent diffusion study was carried out using solid-to-solid diffusion couples. The U-10 wt pct Zr vs pure Fe diffusion couples were assembled and annealed at temperatures, 903 K, 923 K, and 953 K (630 A degrees C, 650 A degrees C, and 680 A degrees C) for 96 hours. Development of microstructure, phase constituents, and compositions developed during the thermal anneals were examined by scanning electron microscopy, transmission electron microscopy, and X-ray energy dispersive spectroscopy. Complex microstructure consisting of several layers that include phases such as U6Fe, UFe2, ZrFe2, alpha-U, beta-U, Zr-precipitates, chi, epsilon, and lambda were observed. Multi-phase layers were grouped based on phase constituents and microstructure, and the layer thicknesses were measured to calculate the growth constant and activation energy. The local average compositions through the interaction layer were systematically determined, and employed to construct semi-quantitative diffusion paths on isothermal U-Zr-Fe ternary phase diagrams at respective temperatures. The diffusion paths were examined to qualitatively estimate the diffusional behavior of individual components and their interactions. Furthermore, selected area electron diffraction analyses were carried out to determine, for the first time, the exact crystal structure and composition of chi, epsilon, and lambda-phases. The chi, epsilon, and lambda-phases were identified as Pnma(62) Fe(Zr,U), I4/mcm(140) Fe(Zr,U)(2), and P42/mnm(136) U-3(Zr,Fe), respectively. C1 [Park, Y.; Huang, K.; Paz y Puente, A.; Sohn, Y. H.] Univ Cent Florida, Dept Mat Sci & Engn, Adv Mat Proc & Anal Ctr, Orlando, FL 32816 USA. [Paz y Puente, A.] Northwestern Univ, Dept Mat Sci & Engn, Evanston, IL 60208 USA. [Lee, H. S.] Kyungpook Natl Univ, Dept Mat Sci & Met Engn, Taegu, South Korea. [Sencer, B. H.] Idaho Natl Lab, Fundamental Fuel Properties Dept, Nucl Fuel & Mat Div, Idaho Falls, ID USA. [Kennedy, J. R.] Idaho Natl Lab, Adv Test Reactor Natl Sci User Facil, Idaho Falls, ID USA. RP Sohn, YH (reprint author), Univ Cent Florida, Dept Mat Sci & Engn, Adv Mat Proc & Anal Ctr, Orlando, FL 32816 USA. EM yongho.sohn@ucf.edu RI Sohn, Yongho/A-8517-2010; Paz y Puente, Ashley/M-2022-2015 OI Sohn, Yongho/0000-0003-3723-4743; Paz y Puente, Ashley/0000-0001-7108-7164 FU US Department of Energy under DOE-NE Idaho Operations Office [DE-AC07-05ID14517] FX This work was supported by the US Department of Energy under DOE-NE Idaho Operations Office Contract DE-AC07-05ID14517. Accordingly, the US Government retains and the publisher, by accepting the article for publication, acknowledges that the US Government retains a nonexclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US Government purposes. NR 13 TC 1 Z9 1 U1 2 U2 15 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1073-5623 EI 1543-1940 J9 METALL MATER TRANS A JI Metall. Mater. Trans. A-Phys. Metall. Mater. Sci. PD JAN PY 2015 VL 46A IS 1 BP 72 EP 82 DI 10.1007/s11661-014-2277-2 PG 11 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Materials Science; Metallurgy & Metallurgical Engineering GA AX2QI UT WOS:000346788600013 ER PT J AU Westphal, BR Frank, SM Mccartin, WM Cummings, DG Giglio, JJ O'Holleran, TP Hahn, PA Yoo, TS Marsden, KC Bateman, KJ Patterson, MN AF Westphal, Brian R. Frank, S. M. Mccartin, W. M. Cummings, D. G. Giglio, J. J. O'Holleran, T. P. Hahn, P. A. Yoo, T. S. Marsden, K. C. Bateman, K. J. Patterson, M. N. TI Characterization of Irradiated Metal Waste from the Pyrometallurgical Treatment of Used EBR-II Fuel SO METALLURGICAL AND MATERIALS TRANSACTIONS A-PHYSICAL METALLURGY AND MATERIALS SCIENCE LA English DT Article ID STEEL-ZIRCONIUM ALLOYS; NUCLEAR-FUEL; FORMS; MICROSTRUCTURE; TECHNETIUM; PHASE AB As part of the pyrometallurgical treatment of used Experimental Breeder Reactor-II fuel, a metal waste stream is generated consisting primarily of cladding hulls laden with fission products noble to the electrorefining process. Consolidation by melting at high temperature [1873 K (1600 A degrees C)] has been developed to sequester the noble metal fission products (Zr, Mo, Tc, Ru, Rh, Te, and Pd) which remain in the iron-based cladding hulls. Zirconium from the uranium fuel alloy (U-10Zr) is also deposited on the hulls and forms Fe-Zr intermetallics which incorporate the noble metals as well as residual actinides during processing. Hence, Zr has been chosen as the primary indicator for consistency of the metal waste. Recently, the first production-scale metal waste ingot was generated and sampled to monitor Zr content for Fe-Zr intermetallic phase formation and validation of processing conditions. Chemical assay of the metal waste ingot revealed a homogeneous distribution of the noble metal fission products as well as the primary fuel constituents U and Zr. Microstructural characterization of the ingot confirmed the immobilization of the noble metals in the Fe-Zr intermetallic phase. C1 [Westphal, Brian R.; Frank, S. M.; Mccartin, W. M.; Cummings, D. G.; Giglio, J. J.; O'Holleran, T. P.; Hahn, P. A.; Yoo, T. S.; Marsden, K. C.; Bateman, K. J.; Patterson, M. N.] Idaho Natl Lab, Idaho Falls, ID 83415 USA. RP Westphal, BR (reprint author), Idaho Natl Lab, POB 1625, Idaho Falls, ID 83415 USA. EM brian.westphal@inl.gov RI Frank, Steven/B-9046-2017; OI Frank, Steven/0000-0001-8259-6722; Giglio, Jeffrey/0000-0002-0877-927X FU U.S. Department of Energy, Office of Nuclear Energy, Science, and Technology, under DOE-NE Idaho Operations Office [DE-AC07-05ID14517] FX The authors would like to acknowledge the Hot Fuel Examination Facility and Fuel Conditioning Facility operations personnel for their recent contributions and the Analytical Laboratory staff for chemical services. Given the extended history of metal waste form development, the following researchers at Argonne National Laboratory and the Idaho National Laboratory should also be recognized and this by no means represents a complete list: D.P. Abraham, J.P. Ackerman, R.W. Benedict, T.D. DiSanto, N.L. Dietz, W.L. Ebert, R.N. Elliott, T.H. Fanning, J.K. Fink, K.M. Goff, I. Johnson, S.G. Johnson, D.D. Keiser, Jr., C.J. Knight, J.R. Krsul, R.P. Lind, C.D. Morgan, E.E. Morris, S.M. McDeavitt, M. Noy, J.Y. Park, M.C. Petri, J.W. Richardson, Jr., D. Vaden, S. White, and R.A. Wigeland. This work was supported by the U.S. Department of Energy, Office of Nuclear Energy, Science, and Technology, under DOE-NE Idaho Operations Office Contract DE-AC07-05ID14517. NR 39 TC 0 Z9 0 U1 3 U2 8 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1073-5623 EI 1543-1940 J9 METALL MATER TRANS A JI Metall. Mater. Trans. A-Phys. Metall. Mater. Sci. PD JAN PY 2015 VL 46A IS 1 BP 83 EP 92 DI 10.1007/s11661-013-2114-z PG 10 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Materials Science; Metallurgy & Metallurgical Engineering GA AX2QI UT WOS:000346788600014 ER PT J AU Hayes, RW Unocic, RR Nasrollahzadeh, M AF Hayes, Robert W. Unocic, Raymond R. Nasrollahzadeh, Maryam TI Creep Deformation of Allvac 718Plus SO METALLURGICAL AND MATERIALS TRANSACTIONS A-PHYSICAL METALLURGY AND MATERIALS SCIENCE LA English DT Article ID NICKEL-BASE SUPERALLOYS; STEADY-STATE CREEP; DISLOCATION CLIMB; TERTIARY CREEP; STRENGTH; BEHAVIOR; ALLOYS AB The creep deformation behavior of Allvac 718Plus was studied over the temperature range of 923 K to 1005 K (650 A degrees C to 732 A degrees C) at initial applied stress levels ranging from 517 to 655 MPa. Over the entire experimental temperature-stress regime this alloy exhibits Class M-type creep behavior with all creep curves exhibiting a decelerating strain rate with strain or time throughout primary creep. However, unlike pure metals or simple solid solution alloys, this gamma prime strengthened superalloy does not exhibit steady-state creep. Rather, primary creep is instantly followed by a long duration of accelerating strain rate with strain or time. These creep characteristics are common among the gamma prime strengthened superalloys. Allvac 718Plus also exhibits a very high temperature dependence of creep rate. Detailed TEM examination of the deformation structures of selected creep samples reveals dislocation mechanisms similar to those found in high volume fraction gamma prime strengthened superalloys. Strong evidence of microtwinning is found in several of the deformation structures. The presence of microtwinning may account for the strong temperature dependence of creep rate observed in this alloy. In addition, due to the presence of Nb and thus, grain boundary delta phase, matrix dislocation activity which is not present in non-Nb-bearing superalloys occurs in this alloy. The creep characteristics and dislocation mechanisms are presented and discussed in detail. C1 [Hayes, Robert W.; Nasrollahzadeh, Maryam] Met Technol Inc, Northridge, CA 91324 USA. [Unocic, Raymond R.] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. RP Hayes, RW (reprint author), Met Technol Inc, Northridge, CA 91324 USA. EM hayesrw.mtl@gmail.com NR 24 TC 1 Z9 1 U1 2 U2 8 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1073-5623 EI 1543-1940 J9 METALL MATER TRANS A JI Metall. Mater. Trans. A-Phys. Metall. Mater. Sci. PD JAN PY 2015 VL 46A IS 1 BP 218 EP 228 DI 10.1007/s11661-014-2564-y PG 11 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Materials Science; Metallurgy & Metallurgical Engineering GA AX2QI UT WOS:000346788600028 ER PT J AU Chowdhury, SM Surhland, C Sanchez, Z Chaudhary, P Kumar, MAS Lee, S Pena, LA Waring, M Sitharaman, B Naidu, M AF Chowdhury, Sayan Mullick Surhland, Cassandra Sanchez, Zina Chaudhary, Pankaj Kumar, M. A. Suresh Lee, Stephen Pena, Louis A. Waring, Michael Sitharaman, Balaji Naidu, Mamta TI Graphene nanoribbons as a drug delivery agent for lucanthone mediated therapy of glioblastoma multiforme SO NANOMEDICINE-NANOTECHNOLOGY BIOLOGY AND MEDICINE LA English DT Article DE Apurinic endonuclease-1; Thioxanthenones; Lucanthone; Graphene nanoribbons; GBM; CG-4; Rat glial progenitor cells ID APURINIC/APYRIMIDINIC ENDONUCLEASE ACTIVITY; PHOTOTHERMAL THERAPY; OXIDE; NANOPARTICLE; MECHANISMS; RESISTANCE; RADIATION; CARBON; BRAIN AB We report use of PEG-DSPE coated oxidized graphene nanoribbons (O-GNR-PEG-DSPE) as agent for delivery of anti-tumor drug Lucanthone (Luc) into Glioblastoma Multiformae (GBM) cells targeting base excision repair enzyme APE-1 (Apurinic endonuclease-1). Lucanthone, an endonuclease inhibitor of APE-1, was loaded onto O-GNR-PEG-DSPEs using a simple non-covalent method. We found its uptake by GBM cell line U251 exceeding 67% and 60% in APE-1-overexpressing U251, post 24 h. However, their uptake was similar to 38% and 29% by MCF-7 and rat glial progenitor cells (CG-4), respectively. TEM analysis of U251 showed large aggregates of O-GNR-PEG-DSPE in vesicles. Luc-O-GNR-PEG-DSPE was significantly toxic to U251 but showed little/no toxicity when exposed to MCF-7/CG-4 cells. This differential uptake effect can be exploited to use O-GNR-PEG-DSPEs as a vehicle for Luc delivery to GBM, while reducing nonspecific cytotoxicity to the surrounding healthy tissue. Cell death in U251 was necrotic, probably due to oxidative degradation of APE-1. From the Clinical Editor: This study reports on the utility of PEG-DSPE coated oxidized graphene nanoribbons as anti-tumor drug delivery agents of Lucanthone into Glioblastoma Multiformae cells targeting base excision repair enzyme APE-1, demonstrating promising anti-tumor effects with good preservation of healthy cells. (C) 2015 Elsevier Inc. All rights reserved. C1 [Sanchez, Zina; Kumar, M. A. Suresh] SUNY Stony Brook, Dept Pharmacol Sci, Stony Brook, NY 11794 USA. [Chowdhury, Sayan Mullick; Surhland, Cassandra; Lee, Stephen; Pena, Louis A.; Sitharaman, Balaji] SUNY Stony Brook, Dept Biomed Engn, Stony Brook, NY 11794 USA. [Chaudhary, Pankaj] Queens Univ Belfast, Ctr Canc Res & Cell Biol, Belfast, Antrim, North Ireland. [Pena, Louis A.] Brookhaven Natl Lab, Dept Biosci, Upton, NY 11973 USA. [Waring, Michael] Univ Cambridge, Dept Pharmacol, Cambridge, England. [Naidu, Mamta] Tufts Sch Med, Ctr Canc Syst Biol, GeneSys Res Inst, Boston, MA USA. RP Sitharaman, B (reprint author), Tufts Univ, Sch Med, Ctr Canc Syst Biol, GeneSys Res Inst, Boston, MA 02135 USA. EM balaji.sitharaman@stonybrook.edu; mamta.naidu@steward.org OI Naidu, Mamta/0000-0002-2754-2470 FU DOE [KP-1401020/MO-079]; NIH [1DP2OD007394-01] FX This work was supported by DOE grant to LP (DOE grant KP-1401020/MO-079) and NIH grant to SB (1DP2OD007394-01). NR 28 TC 10 Z9 10 U1 10 U2 48 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 1549-9634 EI 1549-9642 J9 NANOMED-NANOTECHNOL JI Nanomed.-Nanotechnol. Biol. Med. PD JAN PY 2015 VL 11 IS 1 BP 109 EP 118 DI 10.1016/j.nano.2014.08.001 PG 10 WC Nanoscience & Nanotechnology; Medicine, Research & Experimental SC Science & Technology - Other Topics; Research & Experimental Medicine GA AX3NQ UT WOS:000346846500011 PM 25131339 ER PT J AU Krasnoslobodtsev, AV Torres, MP Kaur, S Vlassiouk, IV Lipert, RJ Jain, M Batra, SK Lyubchenko, YL AF Krasnoslobodtsev, Alexey V. Torres, Maria P. Kaur, Sukhwinder Vlassiouk, Ivan V. Lipert, Robert J. Jain, Maneesh Batra, Surinder K. Lyubchenko, Yuri L. TI Nano-immunoassay with improved performance for detection of cancer biomarkers SO NANOMEDICINE-NANOTECHNOLOGY BIOLOGY AND MEDICINE LA English DT Article DE Nano-immunoassay; Cancer biomarkers; Nanodiagnostics; Pancreatic cancer; Surface-enhanced Raman scattering (SERS); AFM ID ENHANCED RAMAN-SPECTROSCOPY; SURFACE-PLASMON RESONANCE; SERS; NANOPARTICLES; GRAPHENE; SCATTERING; SUBSTRATE AB Nano-immunoassay utilizing surface-enhanced Raman scattering (SERS) effect is a promising analytical technique for early detection of cancer. In its current standing the assay is capable of discriminating samples of healthy individuals from samples of pancreatic cancer patients. Further improvements in sensitivity and reproducibility will extend practical applications of the SERS-based detection platforms to wider range of problems. In this report, we discuss several strategies designed to improve performance of the SERS-based detection system. We demonstrate that reproducibility of the platform is enhanced by using atomically smooth mica surface as a template for preparation of capture surface in SERS sandwich immunoassay. Furthermore, assay's stability and sensitivity can be further improved by using either polymer or graphene monolayer as a thin protective layer applied on top of the assay addresses. The protective layer renders signal to be more stable against photo-induced damage and carbonaceous contamination. From the Clinical Editor: This study discusses strategies to improve the performance of nano-immunoassays utilizing surface-enhanced Raman scattering (SERS) effect, an analytical technique with high sensitivity that holds a great promise for early cancer biomarker detection. (C) 2015 Elsevier Inc. All rights reserved. C1 [Krasnoslobodtsev, Alexey V.; Lyubchenko, Yuri L.] Univ Nebraska, Med Ctr, Dept Pharmaceut Sci, Omaha, NE 68182 USA. [Torres, Maria P.; Kaur, Sukhwinder; Jain, Maneesh; Batra, Surinder K.] Univ Nebraska, Med Ctr, Dept Biochem & Mol Biol, Omaha, NE 68182 USA. [Vlassiouk, Ivan V.] Oak Ridge Natl Lab, Oak Ridge, TN USA. [Lipert, Robert J.] Iowa State Univ, Ames, IA USA. [Krasnoslobodtsev, Alexey V.] Univ Nebraska, Dept Phys, Omaha, NE 68182 USA. RP Krasnoslobodtsev, AV (reprint author), Univ Nebraska, Dept Phys, Omaha, NE 68182 USA. EM akrasnos@gmail.com; sbatra@unmc.edu; ylyubchenko@unmc.edu RI Vlassiouk, Ivan/F-9587-2010 OI Vlassiouk, Ivan/0000-0002-5494-0386 FU NSF [EPS-1004094]; National Institutes of Health [5R01GM096039-04]; National Institutes of Health (EDRN) [UO1 CA111294, P50 CA 127297]; Nebraska Research Initiative (NRI) FX The work was supported by grants EPS-1004094 (NSF) and 5R01GM096039-04 (National Institutes of Health) to Y.L.L.; National Institutes of Health (EDRN UO1 CA111294, P50 CA 127297) to S.K.B. and Nebraska Research Initiative (NRI) grant to M.J., Y.L.L. and A.V. NR 22 TC 7 Z9 7 U1 2 U2 49 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 1549-9634 EI 1549-9642 J9 NANOMED-NANOTECHNOL JI Nanomed.-Nanotechnol. Biol. Med. PD JAN PY 2015 VL 11 IS 1 BP 167 EP 173 DI 10.1016/j.nano.2014.08.012 PG 7 WC Nanoscience & Nanotechnology; Medicine, Research & Experimental SC Science & Technology - Other Topics; Research & Experimental Medicine GA AX3NQ UT WOS:000346846500017 PM 25200613 ER PT J AU Lukyanchuk, I Vinokur, VM Rydh, A Xie, R Milosevic, MV Welp, U Zach, M Xiao, ZL Crabtree, GW Bending, SJ Peeters, FM Kwok, WK AF Lukyanchuk, I. Vinokur, V. M. Rydh, A. Xie, R. Milosevic, M. V. Welp, U. Zach, M. Xiao, Z. L. Crabtree, G. W. Bending, S. J. Peeters, F. M. Kwok, W. K. TI Rayleigh instability of confined vortex droplets in critical superconductors SO NATURE PHYSICS LA English DT Article ID MAGNETIZATION; TRANSITIONS; STABILITY; STRINGS; LEAD AB Depending on the Ginzburg-Landau parameter kappa, superconductors can either be fully diamagnetic if kappa < 1/root 2 (type I superconductors) or allow magnetic flux to penetrate through Abrikosov vortices if kappa > 1/root 2 (type II superconductors; refs 1,2). At the Bogomolny critical point, kappa = kappa(c) = 1/root 2, a state that is infinitely degenerate with respect to vortex spatial configurations arises(3,4). Despite in-depth investigations of conventional type I and type II superconductors, a thorough understanding of the magnetic behaviour in the near-Bogomolny critical regime at kappa similar to kappa(c) remains lacking. Here we report that in confined systems the critical regime expands over a finite interval of kappa forming a critical superconducting state. We show that in this state, in a sample with dimensions comparable to the vortex core size, vortices merge into a multi-quanta droplet, which undergoes Rayleigh instability(5) on increasing kappa and decays by emitting single vortices. Superconducting vortices realize Nielsen-Olesen singular solutions of the Abelian Higgs model, which is pervasive in phenomena ranging from quantum electrodynamics to cosmology(6-9). Our study of the transient dynamics of Abrikosov-Nielsen-Olesen vortices in systems with boundaries promises access to non-trivial effects in quantum field theory by means of bench-top laboratory experiments. C1 [Lukyanchuk, I.] Univ Picardie, Lab Condensed Matter Phys, F-80000 Amiens, France. [Vinokur, V. M.; Xie, R.; Welp, U.; Zach, M.; Xiao, Z. L.; Crabtree, G. W.; Kwok, W. K.] Argonne Natl Lab, Div Mat Sci, Argonne, IL 60439 USA. [Rydh, A.] Stockholm Univ, Albanova Univ Ctr, Dept Phys, SE-10691 Stockholm, Sweden. [Milosevic, M. V.; Peeters, F. M.] Univ Antwerp, Dept Phys, B-2020 Antwerp, Belgium. [Bending, S. J.] Univ Bath, Dept Phys, Bath BA2 7AY, Avon, England. RP Lukyanchuk, I (reprint author), Univ Picardie, Lab Condensed Matter Phys, F-80000 Amiens, France. EM lukyanc@ferroix.net RI Milosevic, Milorad/H-9393-2012; Rydh, Andreas/A-7068-2012; CMT, UAntwerpen Group/A-5523-2016; Igor, Lukyanchuk/C-4206-2008; Zach, Michael/D-4160-2009; OI Rydh, Andreas/0000-0001-6641-4861; Zach, Michael/0000-0002-4409-3419; Xie, Ruobing/0000-0003-0266-9122 FU US Department of Energy, Office of Science Materials Sciences and Engineering Division (Materials Theory Institute); FP7-IRSES-SIMTECH program; ITN-NOTEDEV program; Flemish Science Foundation (FWO-Vlaanderen) FX We would like to thank N. Nekrasov for illuminating discussions. The work was supported by the US Department of Energy, Office of Science Materials Sciences and Engineering Division (V.M.V., W.K.K., U.W., R.X., M.Z., Z.L.X., G.W.C. and partially I.L. through the Materials Theory Institute), by FP7-IRSES-SIMTECH and ITN-NOTEDEV programs (I.L.), and by the Flemish Science Foundation (FWO-Vlaanderen) (M.V.M. and F.M.P.). NR 24 TC 9 Z9 9 U1 1 U2 32 PU NATURE PUBLISHING GROUP PI LONDON PA MACMILLAN BUILDING, 4 CRINAN ST, LONDON N1 9XW, ENGLAND SN 1745-2473 EI 1745-2481 J9 NAT PHYS JI Nat. Phys. PD JAN PY 2015 VL 11 IS 1 BP 21 EP 25 DI 10.1038/NPHYS3146 PG 5 WC Physics, Multidisciplinary SC Physics GA AX3HQ UT WOS:000346831100018 ER PT J AU Li, YZ Lewis, EE Smith, MA Wu, HC Cao, LZ AF Li, Yunzhao Lewis, E. E. Smith, Micheal A. Wu, Hongchun Cao, Liangzhi TI Preconditioned Multigroup GMRES Algorithms for the Variational Nodal Method SO NUCLEAR SCIENCE AND ENGINEERING LA English DT Article ID STRATEGIES; ITERATION AB Combinations of three approaches are examined as options to replace the algorithms presently employed in the variational nodal code VARIANT. They are preconditioned Generalized Minimal Residual (GMRES) algorithms, parallelism in energy, and Wielandt acceleration. Together with partitioned matrix and Gauss-Seidel (GS) preconditioners, two GMRES algorithms are formulated to replace the upscattering iteration and facilitate energy parallelism and Wielandt acceleration. The GMRES algorithms are tested on two-dimensional thermal and fast reactor diffusion problems. The two GMRES algorithms yield higher efficiencies in energy group parallelization and Wielandt acceleration than simple parallelization of the existing GS algorithm. With preconditioning the GMRES algorithms reduce the total computing time by a factor of 2 to 4 and in some cases by a factor of >10. A multilevel iteration optimization scheme is investigated that automatically adjusts the relative error tolerance of the inner iterations according to the estimated convergence rate of the corresponding outer iterations and updates the Wielandt shift magnitude as the calculations progress. Numerical results based on large two-dimensional thermal and fast reactor diffusion problems demonstrate that automated optimization of the multilevel iterative processes reduces iteration numbers by as much as an order of magnitude. C1 [Li, Yunzhao; Wu, Hongchun; Cao, Liangzhi] Xi An Jiao Tong Univ, Sch Nucl Sci & Technol, Xian 710049, Shaanxi, Peoples R China. [Lewis, E. E.] Northwestern Univ, Dept Mech Engn, Evanston, IL 60208 USA. [Smith, Micheal A.] Argonne Natl Lab, Nucl Engn Div, Argonne, IL 60439 USA. RP Li, YZ (reprint author), Xi An Jiao Tong Univ, Sch Nucl Sci & Technol, 28 West Xianning Rd, Xian 710049, Shaanxi, Peoples R China. EM yunzhao@mail.xjtu.edu.cn RI Cao, Liangzhi/N-5471-2014 OI Cao, Liangzhi/0000-0002-2872-011X FU National Natural Science Foundation of China [11305123]; State Scholarship Fund of China [2010628100]; U.S. Department of Energy [DE-AC02-06CH11357] FX This work is supported by the National Natural Science Foundation of China (No. 11305123), the State Scholarship Fund of China (No. 2010628100), and the U.S. Department of Energy (No. DE-AC02-06CH11357). NR 20 TC 1 Z9 1 U1 0 U2 3 PU AMER NUCLEAR SOC PI LA GRANGE PK PA 555 N KENSINGTON AVE, LA GRANGE PK, IL 60526 USA SN 0029-5639 EI 1943-748X J9 NUCL SCI ENG JI Nucl. Sci. Eng. PD JAN PY 2015 VL 179 IS 1 BP 42 EP 58 PG 17 WC Nuclear Science & Technology SC Nuclear Science & Technology GA AX4BZ UT WOS:000346880300003 ER PT J AU Ouisloumen, M Ougouag, AM Ghrayeb, SZ AF Ouisloumen, Mohamed Ougouag, Abderrafi M. Ghrayeb, Shadi Z. TI Anisotropic Elastic Resonance Scattering Model for the Neutron Transport Equation SO NUCLEAR SCIENCE AND ENGINEERING LA English DT Article ID KERNEL; IMPACT; GAS AB The resonance scattering transfer cross section has been reformulated to account for anisotropic scattering in the center of mass of the neutron-nucleus system. The main innovation over previous implementations is the relaxation of the ubiquitous assumption of isotropic scattering in the center of mass and the actual effective use of scattering angle distributions from evaluated nuclear data files in the computation of the angular moments of the resonant scattering kernels. The formulas for the high-order an isotropic moments in the laboratory system are also derived. A multigroup numerical formulation is derived and implemented into a module incorporated within the NJOY nuclear data processing code. An ultrafine-energy-mesh cross-section library was generated using these new theoretical models and then was used for fuel assembly calculations with the PARAGON lattice physics code. The results obtained indicate that this new model makes a significant difference to predictions of reactivity, multigroup fluxes, and isotopic inventory during depletion. C1 [Ouisloumen, Mohamed] Westinghouse Elect Co LLC, Nucl Fuel, Cranberry Township, PA 16066 USA. [Ougouag, Abderrafi M.] Idaho Natl Lab, Idaho Falls, ID 83415 USA. [Ghrayeb, Shadi Z.] US Nucl Regulatory Commiss, Washington, DC 20555 USA. RP Ouisloumen, M (reprint author), Westinghouse Elect Co LLC, Nucl Fuel, Cranberry Township, PA 16066 USA. EM ouislom@westinghouse.com OI Ougouag, Abderrafi/0000-0003-4436-380X FU Westinghouse; Idaho National Laboratory; U.S. Department of Energy FX The development and implementation of this project were funded by Westinghouse. The theoretical developments were carried out jointly at Westinghouse and at Idaho National Laboratory. The bulk of the funding, from Westinghouse, is gratefully acknowledged. Support for the second and third authors (AMO and SZG, respectively), from Idaho National Laboratory and the U.S. Department of Energy, respectively, is also gratefully acknowledged. The authors would like to express their gratitude to R. L. Oelrich, Jr., for his support. We also thank H. Huria for his help with NJOY modifications, J. R. Seeker and D. R. Gibson for reviewing this paper, and the anonymous peer reviewers for many valuable suggestions for improving the quality of this paper. The first author (MO) would like to thank H. Ouisloumen for her help in editing this paper. NR 30 TC 2 Z9 2 U1 2 U2 3 PU AMER NUCLEAR SOC PI LA GRANGE PK PA 555 N KENSINGTON AVE, LA GRANGE PK, IL 60526 USA SN 0029-5639 EI 1943-748X J9 NUCL SCI ENG JI Nucl. Sci. Eng. PD JAN PY 2015 VL 179 IS 1 BP 59 EP 84 PG 26 WC Nuclear Science & Technology SC Nuclear Science & Technology GA AX4BZ UT WOS:000346880300004 ER PT J AU Kitamura, A Kurikami, H Yamaguchi, M Oda, Y Saito, T Kato, T Niizato, T Iijima, K Sato, H Yui, M Machida, M Yamada, S Itakura, M Okumura, M Onishi, Y AF Kitamura, Akihiro Kurikami, Hiroshi Yamaguchi, Masaaki Oda, Yoshihiro Saito, Tatsuo Kato, Tomoko Niizato, Tadafumi Iijima, KaZuki Sato, Haruo Yui, Mikazu Machida, Masahiko Yamada, Susumu Itakura, Mitsuhiro Okumura, Masahiko Onishi, Yasuo TI Mathematical Modeling of Radioactive Contaminants in the Fukushima Environment SO NUCLEAR SCIENCE AND ENGINEERING LA English DT Article ID SUBSURFACE SEDIMENTS; HANFORD SITE; RADIOCESIUM; SORPTION; ILLITE; USA AB Significant amounts of radioactive materials were released to the atmosphere from the Fukushima Daiichi nuclear power plant after the accident caused by the major earthquake and devastating tsunami on March 11, 2011. Accurate and efficient prediction of the distribution and fate of radioactive materials eventually deposited at the surface in the Fukushima area is of primary importance. In order to make such a prediction, it is important to gather information regarding the main migration pathways for radioactive materials in the environment and the time dependences of radioactive material transport over the long term. The radionuclide of most concern in the Fukushima case is radioactive cesium. Previous surveys indicate that the primary transportation mechanisms of cesium are either soil erosion and water transport of sediment-sorbed contaminants or transport of dissolved cesium in the water drainage system such as by rivers. A number of mathematical models of radioactive contaminants, with particular attention paid to radiocesium, on the land and in rivers, reservoirs, and estuaries in the Fukushima area are developed. Simulation results are examined while simultaneously implementing field investigations. For example, the orders of magnitude of the radiocesium concentration on the flood plain of the Ukedo River by model prediction and field investigation results were both 10(5) Bq/kg. Microscopic studies of the adsorption/desorption mechanism of cesium and soils have been performed to shed light on the mechanisms of macroscopic diffusive transport of radiocesium through soil. The maximum exchange energy between cesium and prelocated potassium in the frayed edge site was simulated to be 27 kJ/mol, which reproduces the corresponding value previously achieved by experiments. These predictions will be utilized for assessment of dose from the environmental contamination and proposed countermeasures to limit dispersion of the contaminants. C1 [Kitamura, Akihiro; Kurikami, Hiroshi; Yamaguchi, Masaaki; Oda, Yoshihiro; Saito, Tatsuo; Kato, Tomoko; Niizato, Tadafumi; Iijima, KaZuki; Sato, Haruo; Yui, Mikazu] Japan Atom Energy Agcy, Fukushima Environm Safety Ctr, Fukushima, Japan. [Kitamura, Akihiro; Kurikami, Hiroshi; Yamaguchi, Masaaki; Oda, Yoshihiro; Saito, Tatsuo; Kato, Tomoko; Niizato, Tadafumi; Iijima, KaZuki; Sato, Haruo; Yui, Mikazu] Geol Isolat Res & Dev Directorate, Ibaraki, Japan. [Machida, Masahiko; Yamada, Susumu; Itakura, Mitsuhiro; Okumura, Masahiko] Japan Atom Energy Agcy, Ctr Computat Sci & E Syst, Chiba, Japan. [Onishi, Yasuo] Pacific NW Natl Lab, Energy & Environm Directorate, Richland, WA 99352 USA. RP Kitamura, A (reprint author), Japan Atom Energy Agcy, Fukushima Environm Safety Ctr, Fukushima, Japan. EM kitamura.akihiro@jaea.go.jp NR 26 TC 1 Z9 1 U1 4 U2 12 PU AMER NUCLEAR SOC PI LA GRANGE PK PA 555 N KENSINGTON AVE, LA GRANGE PK, IL 60526 USA SN 0029-5639 EI 1943-748X J9 NUCL SCI ENG JI Nucl. Sci. Eng. PD JAN PY 2015 VL 179 IS 1 BP 104 EP 118 PG 15 WC Nuclear Science & Technology SC Nuclear Science & Technology GA AX4BZ UT WOS:000346880300006 ER PT J AU Green, MA Emery, K Hishikawa, Y Warta, W Dunlop, ED AF Green, Martin A. Emery, Keith Hishikawa, Yoshihiro Warta, Wilhelm Dunlop, Ewan D. TI Solar cell efficiency tables (Version 45) SO PROGRESS IN PHOTOVOLTAICS LA English DT Article DE solar cell efficiency; photovoltaic efficiency; energy conversion efficiency ID CONCENTRATOR; STABILITY AB Consolidated tables showing an extensive listing of the highest independently confirmed efficiencies for solar cells and modules are presented. Guidelines for inclusion of results into these tables are outlined and new entries since July 2014 are reviewed. Copyright (c) 2014 John Wiley & Sons, Ltd. C1 [Green, Martin A.] Univ New S Wales, Australian Ctr Adv Photovolta, Sydney, NSW 2052, Australia. [Emery, Keith] Natl Renewable Energy Lab, Golden, CO 80401 USA. [Hishikawa, Yoshihiro] Natl Inst Adv Ind Sci & Technol, Res Ctr Photovolta Technol RCPVT, Tsukuba, Ibaraki 3058568, Japan. [Warta, Wilhelm] Fraunhofer Inst Solar Energy Syst, Dept Solar Cells Mat & Technol, D-79110 Freiburg, Germany. [Dunlop, Ewan D.] Commiss European Communities, Joint Res Ctr, Renewable Energy Unit, Inst Energy, IT-21027 Ispra, Italy. RP Green, MA (reprint author), Univ New S Wales, Sch Photovolta & Renewable Energy Engn, Sydney, NSW 2052, Australia. EM m.green@unsw.edu.au FU U.S. Department of Energy [DE-AC36-08-GO28308]; National Renewable Energy Laboratory FX The Australian Centre for Advanced Photovoltaics commenced operation in February 2013 with support from the Australian Government through the Australian Renewable Energy Agency (ARENA). The Australian Government does not accept responsibility for the views, information or advice expressed herein. The work by K. Emery was supported by the U.S. Department of Energy under Contract No. DE-AC36-08-GO28308 with the National Renewable Energy Laboratory. NR 54 TC 740 Z9 753 U1 64 U2 423 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 1062-7995 EI 1099-159X J9 PROG PHOTOVOLTAICS JI Prog. Photovoltaics PD JAN PY 2015 VL 23 IS 1 BP 1 EP 9 DI 10.1002/pip.2573 PG 9 WC Energy & Fuels; Materials Science, Multidisciplinary; Physics, Applied SC Energy & Fuels; Materials Science; Physics GA AX0NX UT WOS:000346650000001 ER PT J AU Biagioni, D Graham, RL Albin, DS Jones, WB Suh, C AF Biagioni, David Graham, Rebekah L. Albin, David S. Jones, Wesley B. Suh, Changwon TI Analysis of governing factors for photovoltaic loss mechanism of n-CdS/p-CdTe heterojunction via multi-way data decomposition SO PROGRESS IN PHOTOVOLTAICS LA English DT Article DE CdTe; thin film solar cells; C-V; reliability; degradation; multi-way PLS ID SOLAR-CELLS; MULTIVARIATE REGRESSION; STABILITY; BARRIER; VOLTAGE AB An analytical framework for identifying key factors of the degradation of photovoltaic efficiency over time is presented. We demonstrate that, in many photovoltaic experimental settings, reliability data sets are easily cast in a multi- or N-way format. We adopt a statistical technique, N-way partial least squares, that generates a multi-linear model using all of the data simultaneously. With this approach, we are able to model variables of interest such as cell efficiency while representing the data in a lower-dimensional space in which salient features are more easily identified. We illustrate our approach with reliability data for CdS/CdTe heterojunction solar cell devices. Even with the inclusion of a noisy parameter such as the net acceptor density, and with a relatively small number of devices, we automatically identify key factors that are highly related to performance degradation. In particular, the conductance at the back contact is related to short stress-time degradation (0-300h), whereas the net acceptor density near the junction (at +0.08VDC bias) is correlated with more gradual, long stress-time degradation (300-1000h). These notable degradation modes are explained with respect to our processing conditions and Cu-diffusion in the cells. Copyright (c) 2013 John Wiley & Sons, Ltd. C1 [Biagioni, David; Graham, Rebekah L.; Albin, David S.; Jones, Wesley B.; Suh, Changwon] Natl Renewable Energy Lab, Golden, CO 80401 USA. [Biagioni, David] Univ Colorado, Dept Appl Math, Boulder, CO 80309 USA. [Suh, Changwon] Harvard Univ, Dept Chem & Chem Biol, Cambridge, MA 02138 USA. RP Suh, C (reprint author), Natl Renewable Energy Lab, 15013 Denver West Pkwy, Golden, CO 80401 USA. EM csuh@fas.harvard.edu FU US Department of Energy [DE-AC36-08-GO28308]; National Renewable Energy Laboratory FX This work was supported by the US Department of Energy under Contract No. DE-AC36-08-GO28308 with the National Renewable Energy Laboratory. NR 29 TC 4 Z9 4 U1 1 U2 17 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 1062-7995 EI 1099-159X J9 PROG PHOTOVOLTAICS JI Prog. Photovoltaics PD JAN PY 2015 VL 23 IS 1 BP 49 EP 60 DI 10.1002/pip.2394 PG 12 WC Energy & Fuels; Materials Science, Multidisciplinary; Physics, Applied SC Energy & Fuels; Materials Science; Physics GA AX0NX UT WOS:000346650000006 ER PT J AU Li, CB Shi, HQ Cao, YJ Wang, JH Kuang, YH Tan, Y Wei, J AF Li, Canbing Shi, Haiqing Cao, Yijia Wang, Jianhui Kuang, Yonghong Tan, Yi Wei, Jing TI Comprehensive review of renewable energy curtailment and avoidance: A specific example in China SO RENEWABLE & SUSTAINABLE ENERGY REVIEWS LA English DT Review DE Curtailed electric energy; Carbon capture and storage; Emission reduction; Renewable energy sources ID WIND POWER; DEMAND RESPONSE; CARBON CAPTURE; COMBINED HEAT; OPTIMIZATION; TURBINES; SYSTEMS; STORAGE; OPERATION AB Concerns over climate change (global warming) are driving innovation for stabilizing and reducing greenhouse gas (GHG) emissions. Technologies like carbon capture and storage (CCS) as well as renewable energy sources including wind and solar have been increasingly used and integrated into existing energy systems. The global installed renewable energy capacity booms, but many problems regarding grid integration appears due to the variability and uncertainty in the output of renewable energy generation. Therefore, large amount of curtailed electric energy (CEE) exists, which means some of the renewable energy generation must be wasted to keep real-time balance between load and generation in power system. In this paper, the definition of CEE is introduced, and the main causes for CEE are discussed. Then, the worldwide CEE is estimated, especially in China. Moreover, to evaluate the utilization priority of various generation resources, the potential of reducing fossil fuel consumption, GHG emissions and air pollutants as well as the potential of capturing CO2 with CEE are analyzed. Possible CEE reduction strategies are also presented. (C) 2014 Published by Elsevier Ltd. C1 [Li, Canbing; Shi, Haiqing; Cao, Yijia; Kuang, Yonghong; Tan, Yi; Wei, Jing] Hunan Univ, Coll Elect & Informat Engn, Changsha 410082, Hunan, Peoples R China. [Wang, Jianhui] Argonne Natl Lab, Decis & Informat Sci Div, Lemont, IL USA. RP Li, CB (reprint author), Hunan Univ, Coll Elect & Informat Engn, Changsha 410082, Hunan, Peoples R China. EM licanbing@gmail.com; yjcao@hnu.edu.cn FU National High Technology Research and Development of China (863 Program) [2011AA050203]; Program for New Century Excellent Talents in Chinese Universities [NCET-12-0167] FX The authors gratefully acknowledge the support provided by the National High Technology Research and Development of China (863 Program, Grant no. 2011AA050203) and Program for New Century Excellent Talents in Chinese Universities (Grant no. NCET-12-0167). The authors also sincerely thank the organizations and individuals, whose work has been cited in this article. NR 83 TC 22 Z9 22 U1 7 U2 55 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 1364-0321 J9 RENEW SUST ENERG REV JI Renew. Sust. Energ. Rev. PD JAN PY 2015 VL 41 BP 1067 EP 1079 DI 10.1016/j.rser.2014.09.009 PG 13 WC GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY; Energy & Fuels SC Science & Technology - Other Topics; Energy & Fuels GA AX0DA UT WOS:000346622400079 ER PT J AU Kim, J Haberkorn, N Gofryk, K Graf, MJ Ronning, F Sefat, AS Movshovich, R Civale, L AF Kim, Jeehoon Haberkorn, N. Gofryk, K. Graf, M. J. Ronning, F. Sefat, A. S. Movshovich, R. Civale, L. TI Superconducting properties in heavily overdoped Ba(Fe0.86Co0.14)(2)As-2 single crystals SO SOLID STATE COMMUNICATIONS LA English DT Article DE Iron arsenide superconductors; Upper critical field; Magnetic penetration depth; Vortex pinning ID HIGH-TEMPERATURE SUPERCONDUCTORS; II SUPERCONDUCTORS AB We report the intrinsic superconducting parameters in a heavily overdoped Ba(Fe1-xCox)(2)As-2 (x=0.14) single crystal and their influence in the resulting vortex dynamics. We find a bulk superconducting critical temperature of 9.8 K, magnetic penetration depth lambda(ab) (0)=660 +/- 50 nm, coherence length xi(ab) (0)=6.4 +/- 0.2 nm, and the upper critical field anisotropy gamma(T -> Tc) approximate to 3.7. The vortex phase diagram, in comparison with the optimally doped compound, presents a narrow collective creep regime. The intrinsic pinning energy plays an important role in the resulting vortex dynamics as compared with similar pinning landscape and comparable intrinsic thermal fluctuations. (C) 2014 Elsevier Ltd. All rights reserved. C1 [Kim, Jeehoon] Inst for Basic Sci Korea, CALDES, Pohang, South Korea. [Kim, Jeehoon] Pohang Univ Sci & Technol, Dept Phys, Pohang, South Korea. [Haberkorn, N.] Ctr Atom Bariloche, RA-8400 San Carlos De Bariloche, Rio Negro, Argentina. [Gofryk, K.; Graf, M. J.; Ronning, F.; Movshovich, R.; Civale, L.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Sefat, A. S.] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. RP Kim, J (reprint author), Inst for Basic Sci Korea, CALDES, Pohang, South Korea. EM jeehoon@postech.ac.kr; haberkornn@yahoo.com.ar; krzysztof.gofryk@in1.gov; graf@lanl.gov; fronning@lanl.gov; sefata@ornl.gov; roman@lanl.gov; lcivale@lanl.gov RI Sefat, Athena/R-5457-2016; OI Sefat, Athena/0000-0002-5596-3504; Gofryk, Krzysztof/0000-0002-8681-6857 FU U.S. Department of Energy, Office; Institute for Basic Science [IBS-R015-D1] FX Research at LANL was supported by the U.S. Department of Energy, Office of and was supported by Institute for Basic Science by Project Code (IBS-R015-D1). N.H. is a member of CONICET (Argentina). NR 40 TC 1 Z9 1 U1 2 U2 16 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0038-1098 EI 1879-2766 J9 SOLID STATE COMMUN JI Solid State Commun. PD JAN PY 2015 VL 201 BP 20 EP 24 DI 10.1016/j.ssc.2014.09.016 PG 5 WC Physics, Condensed Matter SC Physics GA AX2FY UT WOS:000346760100005 ER PT J AU Keck, RE de Mare, M Churchfield, MJ Lee, S Larsen, G Madsen, HA AF Keck, Rolf-Erik de Mare, Martin Churchfield, Matthew J. Lee, Sang Larsen, Gunner Madsen, Helge Aagaard TI Two improvements to the dynamic wake meandering model: including the effects of atmospheric shear on wake turbulence and incorporating turbulence build-up in a row of wind turbines SO WIND ENERGY LA English DT Article DE Dynamic wake meandering; DWM; Wake modelling; Actuator line model; Wind turbine wake; wake-added turbuelnce; Wake turbulence; Wind farm modelling AB The dynamic wake meandering (DWM) model is an engineering wake model designed to physically model the wake deficit evolution and the unsteady meandering that occurs in wind turbine wakes. The present study aims at improving two features of the model: 1. The effect of the atmospheric boundary layer shear on the wake deficit evolution by including a strain-rate contribution in the wake turbulence calculation. 2. The method to account for the increased turbulence at a wake-affected turbine by basing the wake-added turbulence directly on the Reynolds stresses of the oncoming wake. This also allows the model to simulate the build-up of turbulence over a row of turbines in a physically consistent manner. The performance of the modified model is validated against actuator line (AL) model results and field data from the Lillgrund offshore wind farm. Qualitatively, the modified DWM model is in fair agreement with the reference data. A quantitative comparison between the mean flow field of the DWM model with and without the suggested improvements, to that of the AL model, shows that the root-mean-square difference in terms of wind speed and turbulence intensity is reduced on the order of 30% and 40%, respectively, by including the proposed corrections for a row of eight turbines. Furthermore, it is found that the root-mean-square difference between the AL model and the modified DWM model in terms of wind speed and turbulence intensity does not increase over a row of turbines compared with the root-mean-square difference of a single turbine. Copyright (c) 2013 John Wiley & Sons, Ltd. C1 [Keck, Rolf-Erik; de Mare, Martin] Vestas Wind Syst AS, Rotor Syst, DK-4000 Roskilde, Denmark. [Keck, Rolf-Erik; de Mare, Martin; Larsen, Gunner; Madsen, Helge Aagaard] Riso DTU Natl Lab Sustainable Energy, Wind Energy Dept, DK-4000 Roskilde, Denmark. [Churchfield, Matthew J.; Lee, Sang] Natl Renewable Energy Lab, Golden, CO 80401 USA. RP Keck, RE (reprint author), Riso DTU Natl Lab Sustainable Energy, Wind Energy Dept, DK-4000 Roskilde, Denmark. EM rolf.keck@gmail.com OI Aagaard Madsen , Helge/0000-0002-4647-3706 NR 25 TC 5 Z9 5 U1 0 U2 10 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 1095-4244 EI 1099-1824 J9 WIND ENERGY JI Wind Energy PD JAN PY 2015 VL 18 IS 1 BP 111 EP 132 DI 10.1002/we.1686 PG 22 WC Energy & Fuels; Engineering, Mechanical SC Energy & Fuels; Engineering GA AX1HM UT WOS:000346698400007 ER PT J AU Hausler, I Atkins, R Falmbigl, M Rudin, SP Neumann, W Johnson, DC AF Haeusler, Ines Atkins, Ryan Falmbigl, Matthias Rudin, Sven P. Neumann, Wolfgang Johnson, David C. TI Insights from STEM and NBED studies into the local structure and growth mechanism of misfit layered compounds prepared using modulated reactants SO ZEITSCHRIFT FUR KRISTALLOGRAPHIE LA English DT Article DE ferecrystal; modulated elemental reactants; nano-beam electron diffraction; transmission electron microscopy ID COMPOSITE CRYSTALS; FERECRYSTALLINE COMPOUNDS; MULTIDIMENSIONAL SPACE; ELECTRICAL-PROPERTIES; SUPERSPACE GROUPS; SYMMETRY; SYSTEM; FAMILY AB X-ray diffraction and transmission electron microscopy were used to probe the structure of the misfit compound [(SnSe)(1.15)](1)(VSe2)(1) grown using an elementally modulated precursor. The specular X-ray diffraction pattern contained only 00l reflections, which yielded a c lattice parameter of 1.203(1) nm. Cross-section STEM revealed alternating layers of SnSe and VSe2, in agreement with the structure model refined from the X-ray diffraction pattern using Rietveld refinement. Plan-view transmission electron microscopy revealed the in-plane grain structure of the films, yielding grain sizes in agreement with previously reported in plane X-ray diffraction studies and the cross-section STEM images. The plan view images also contained Moire fringes resulting from grains with different relative tilting on both sides of interfaces as well as Moire fringes resulting from different relative rotations between domains. An energy-filtered nano-beam electron diffraction pattern obtained from at least one domain in the [(SnSe)(1.15)](1) (VSe2)(1) sample investigated in cross section contained a series of resolvable supercell reflections along the c axis that indicated that the supercell c-axis lattice parameter was a multiple of three times that determined using X-ray diffraction. Energy filtered NBED of plan-view samples showed diffraction patterns from select regions with 12-fold symmetry, indicating that the arrangement of the layers is not rotationally random from layer to layer. This suggests that during the self-assembly of the amorphous modulated elemental precursor, the SnSe and VSe2 constituent layers must nucleate off the adjacent interfaces of the growing crystal, yielding layers that are locally rotationally aligned with growing crystal. Different processing conditions during the precursor to crystal self-assembly might enable the domain size and/or the extent of order to be controlled. C1 [Neumann, Wolfgang] Humboldt Univ, Inst Phys, D-12489 Berlin, Germany. [Neumann, Wolfgang] Univ Oregon, Dept Chem, Eugene, OR 97401 USA. [Haeusler, Ines] Humboldt Univ, Inst Phys, D-12489 Berlin, Germany. [Atkins, Ryan; Falmbigl, Matthias; Johnson, David C.] Univ Oregon, Dept Chem, Eugene, OR 97401 USA. [Rudin, Sven P.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Neumann, W (reprint author), Humboldt Univ, Inst Phys, Newtonstr 15, D-12489 Berlin, Germany. EM wolfgang.neumann@physik.hu-berlin FU National Science Foundation [DMR-1266217]; National Science Foundation through CCI grant [CHE-1102637]; U.S. Department of Energy [LDRD-DR 20140025] FX The authors acknowledge support from the National Science Foundation under grant DMR-1266217. Coauthors RA and MF acknowledge support from the National Science Foundation through CCI grant number CHE-1102637. Coauthor SPR acknowledges support from the U.S. Department of Energy under Grant No. LDRD-DR 20140025. NR 31 TC 2 Z9 2 U1 1 U2 19 PU WALTER DE GRUYTER GMBH PI BERLIN PA GENTHINER STRASSE 13, D-10785 BERLIN, GERMANY SN 0044-2968 J9 Z KRISTALLOGR JI Z. Kristall. PD JAN PY 2015 VL 230 IS 1 BP 45 EP 54 DI 10.1515/zkri-2014-1761 PG 10 WC Crystallography SC Crystallography GA AX2HS UT WOS:000346764800007 ER PT J AU Eddaoudi, M Sava, DF Eubank, JF Adil, K Guillerm, V AF Eddaoudi, Mohamed Sava, Dorina F. Eubank, Jarrod F. Adil, Karim Guillerm, Vincent TI Zeolite-like metal-organic frameworks (ZMOFs): design, synthesis, and properties SO CHEMICAL SOCIETY REVIEWS LA English DT Review ID CARBON-DIOXIDE CAPTURE; MOLECULAR BUILDING-BLOCKS; HYDROGEN STORAGE; IMIDAZOLATE FRAMEWORKS; GAS-ADSORPTION; SODALITE-TYPE; COORDINATION POLYMERS; CRYSTAL-STRUCTURE; THERMAL-STABILITY; STRUCTURAL-CHARACTERIZATION AB This review highlights various design and synthesis approaches toward the construction of ZMOFs, which are metal-organic frameworks (MOFs) with topologies and, in some cases, features akin to traditional inorganic zeolites. The interest in this unique subset of MOFs is correlated with their exceptional characteristics arising from the periodic pore systems and distinctive cage-like cavities, in conjunction with modular intra- and/or extra-framework components, which ultimately allow for tailoring of the pore size, pore shape, and/or properties towards specific applications. C1 [Eddaoudi, Mohamed; Adil, Karim; Guillerm, Vincent] King Abdullah Univ Sci & Technol, Div Phys Sci & Engn, Adv Membranes & Porous Mat Ctr AMPM, Funct Mat Design Discovery & Dev Res Grp FMD3, Thuwal 239556900, Saudi Arabia. [Eddaoudi, Mohamed; Sava, Dorina F.; Eubank, Jarrod F.] Univ S Florida, Dept Chem, Tampa, FL 33620 USA. [Sava, Dorina F.] Sandia Natl Labs, Nanoscale Sci Dept, Albuquerque, NM 87185 USA. [Eubank, Jarrod F.] Florida Southern Coll, Dept Chem & Phys, Lakeland, FL 33801 USA. RP Eddaoudi, M (reprint author), King Abdullah Univ Sci & Technol, Div Phys Sci & Engn, Adv Membranes & Porous Mat Ctr AMPM, Funct Mat Design Discovery & Dev Res Grp FMD3, Thuwal 239556900, Saudi Arabia. EM mohamed.eddaoudi@kaust.edu.sa RI Eddaoudi, Mohamed/D-2298-2009; Sava Gallis, Dorina/D-2827-2015; Guillerm, Vincent/G-4545-2011 OI Eddaoudi, Mohamed/0000-0003-1916-9837; Guillerm, Vincent/0000-0003-3460-223X FU King Abdullah University of Science and Technology (KAUST) FX This work was supported by the King Abdullah University of Science and Technology (KAUST). NR 151 TC 165 Z9 166 U1 71 U2 488 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 0306-0012 EI 1460-4744 J9 CHEM SOC REV JI Chem. Soc. Rev. PY 2015 VL 44 IS 1 BP 228 EP 249 DI 10.1039/c4cs00230j PG 22 WC Chemistry, Multidisciplinary SC Chemistry GA AX1JL UT WOS:000346703400012 PM 25341691 ER PT J AU Mariette, C Guerin, L Rabiller, P Chen, YS Bosak, A Popov, A Hollingsworth, MD Toudic, B AF Mariette, Celine Guerin, Laurent Rabiller, Philippe Chen, Yu-Sheng Bosak, Alexei Popov, Alexander Hollingsworth, Mark D. Toudic, Bertrand TI The creation of modulated monoclinic aperiodic composites in n-alkane/urea compounds SO ZEITSCHRIFT FUR KRISTALLOGRAPHIE-CRYSTALLINE MATERIALS LA English DT Article DE alkane/urea crystals; aperiodic crystals; crystallographic superspace; diffraction; phase transitions ID UREA INCLUSION-COMPOUNDS; ELASTIC NEUTRON-SCATTERING; X-RAY-SCATTERING; PHASE-TRANSITION; STRUCTURAL-PROPERTIES; COMPOUNDS OC(NH2)2+CNH2N+2; DISORDERED STRUCTURE; DIFFUSE-SCATTERING; NMR-SPECTROSCOPY; GUEST MOLECULES AB n-Dodecane/urea is a member of the prototype series of n-alkane/urea inclusion compounds. At room temperature, it presents a quasi-one dimensional liquid-like state for the confined guest molecules within the rigid, hexagonal framework of the urea host. At lower temperatures, we report the existence of two other phases. Below T-c=248 K there appears a phase with rank four superspace group P6(1)22(00 gamma), the one typically observed at room temperature in n-alkane/urea compounds with longer guest molecules. A misfit parameter, defined by the ratio gamma=C-h/C-g (C-host/C-guest), is found to be 0.632 +/- 0.005. Below T-c1=123 K, a monoclinic modulated phase is created with a constant shift along c of the guest molecules in adjacent channels. The maximal monoclinic space group for this structure is P12(1)1(alpha 0 gamma). Analogies and differences with n-heptane/urea, which also presents a monoclinic, modulated low-temperature phase, are discussed. C1 [Toudic, Bertrand] Univ Rennes 1, CNRS, Dept Phys, Rennes, France. [Mariette, Celine; Guerin, Laurent; Rabiller, Philippe] Univ Rennes 1, Inst Phys Rennes, CNRS 6251, UMR UR1, F-35042 Rennes, France. [Chen, Yu-Sheng] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. [Bosak, Alexei; Popov, Alexander] European Synchrotron Radiat Facil, F-38043 Grenoble, France. [Hollingsworth, Mark D.] Kansas State Univ, Dept Chem, Manhattan, KS 66506 USA. RP Toudic, B (reprint author), Univ Rennes 1, CNRS, Dept Phys, Campus Beaulieu, Rennes, France. EM bertrand.toudic@univ-rennes1.fr RI Guerin, Laurent/C-4353-2015 FU NSF [CHE-0809845]; DOE [DE-AC02-06CH11357] FX We thank Shane M. Nichols, Bo Wang, Robert Henning, and Vukica Srager for their help with this work, which was supported by the NSF (CHE-0809845). Portions of this research were carried out at the Advanced Photon Source (beamline 14-BM-C) at Argonne National Laboratory, under DOE Contract No. DE-AC02-06CH11357. NR 45 TC 1 Z9 1 U1 0 U2 19 PU WALTER DE GRUYTER GMBH PI BERLIN PA GENTHINER STRASSE 13, D-10785 BERLIN, GERMANY SN 2194-4946 EI 2196-7105 J9 Z KRIST-CRYST MATER JI Z. Krist.-Cryst. Mater. PD JAN PY 2015 VL 230 IS 1 BP 5 EP 11 DI 10.1515/zkri-2014-1773 PG 7 WC Crystallography SC Crystallography GA AX2HS UT WOS:000346764800003 PM 26213678 ER PT J AU Peterson, C Grosse, SD Li, R Sharma, AJ Razzaghi, H Herman, WH Gilboa, SM AF Peterson, Cora Grosse, Scott D. Li, Rui Sharma, Andrea J. Razzaghi, Hilda Herman, William H. Gilboa, Suzanne M. TI Preventable health and cost burden of adverse birth outcomes associated with pregestational diabetes in the United States SO AMERICAN JOURNAL OF OBSTETRICS AND GYNECOLOGY LA English DT Article DE diabetes mellitus; economic analysis; pregnancy complications ID FACTOR SURVEILLANCE SYSTEM; POPULATION-BASED COHORT; PRECONCEPTION CARE; CONGENITAL-ANOMALIES; RESOURCE UTILIZATION; REPRODUCTIVE AGE; ECONOMIC COSTS; WOMEN; PREGNANCY; TYPE-1 AB OBJECTIVE: Preconception care for women with diabetes can reduce the occurrence of adverse birth outcomes. We aimed to estimate the preconception care (PCC)epreventable health and cost burden of adverse birth outcomes associated with diagnosed and undiagnosed pregestational diabetes mellitus (PGDM) in the United States. STUDY DESIGN: Among women of reproductive age (15-44 years), we estimated age-and race/ethnicity-specific prevalence of diagnosed and undiagnosed diabetes. We applied age and race/ethnicity-specific pregnancy rates, estimates of the risk reduction from PCC for 3 adverse birth outcomes (preterm birth, major birth defects, and perinatal mortality), and lifetime medical and lost productivity costs for children with those outcomes. Using a probabilistic model, we estimated the reduction in adverse birth outcomes and costs associated with universal PCC compared with no PCC among women with PGDM. We did not assess maternal outcomes and associated costs. RESULTS: We estimated 2.2% of US births are to women with PGDM. Among women with diagnosed diabetes, universal PCC might avert 8397 (90% prediction interval [PI], 5252-11,449) preterm deliveries, 3725 (90% PI, 3259-4126) birth defects, and 1872 (90% PI, 1239-2415) perinatal deaths annually. Associated discounted lifetime costs averted for the affected cohort of children could be as high as $4.3 billion (90% PI, 3.4-5.1 billion) (2012 US dollars). PCC among women with undiagnosed diabetes could yield an additional $1.2 billion (90% PI, 951 million-1.4 billion) in averted cost. CONCLUSION: Results suggest a substantial health and cost burden associated with PGDM that could be prevented by universal PCC, which might offset the cost of providing such care. C1 [Peterson, Cora; Grosse, Scott D.; Razzaghi, Hilda; Gilboa, Suzanne M.] CDC, Natl Ctr Birth Defects & Dev Disabil, Ctr Dis Control & Prevent, Atlanta, GA 30333 USA. [Li, Rui; Sharma, Andrea J.] CDC, Natl Ctr Chron Dis Prevent & Hlth Promot, Ctr Dis Control & Prevent, Atlanta, GA 30333 USA. [Sharma, Andrea J.] US Public Hlth Serv Commissioned Corps, Atlanta, GA USA. [Razzaghi, Hilda] Oak Ridge Inst Sci & Educ, Oak Ridge, TN USA. [Herman, William H.] Univ Michigan, Sch Med, Dept Internal Med, Ann Arbor, MI USA. [Herman, William H.] Univ Michigan, Sch Med, Dept Epidemiol, Ann Arbor, MI USA. RP Peterson, C (reprint author), CDC, Natl Ctr Injury Prevent & Control, Atlanta, GA 30333 USA. EM cora.peterson@cdc.hhs.gov OI Peterson, Cora/0000-0001-7955-0977; Sharma, Andrea/0000-0003-0385-0011 FU Intramural CDC HHS [CC999999]; NIDDK NIH HHS [P30 DK020572, P30 DK092926] NR 57 TC 6 Z9 6 U1 1 U2 8 PU MOSBY-ELSEVIER PI NEW YORK PA 360 PARK AVENUE SOUTH, NEW YORK, NY 10010-1710 USA SN 0002-9378 EI 1097-6868 J9 AM J OBSTET GYNECOL JI Am. J. Obstet. Gynecol. PD JAN PY 2015 VL 212 IS 1 AR 74.e1 DI 10.1016/j.ajog.2014.09.009 PG 9 WC Obstetrics & Gynecology SC Obstetrics & Gynecology GA AW9OA UT WOS:000346585700024 PM 25439811 ER PT J AU Zhang, HL Fontes, CJ AF Zhang, Hong Lin Fontes, Christopher J. TI Relativistic distorted-wave collision strengths and oscillator strengths for the 185 Delta n=0 transitions with n=2 in the 67 C-like ions with 26 <= Z <= 92 SO ATOMIC DATA AND NUCLEAR DATA TABLES LA English DT Article DE Electron-impact excitation collision strengths; Relativistic distorted-wave theory; Carbon-like ions; Improved top-up method ID ELECTRON-IMPACT EXCITATION; HIGHLY-CHARGED IONS; B-LIKE IONS; OPTICALLY ALLOWED TRANSITIONS; POSSIBLE N=2-N=3 TRANSITIONS; CROSS-SECTION MEASUREMENT; ATOMIC DATA; FE-XXI; LINE EMISSION; IRON PROJECT AB Relativistic distorted-wave collision strengths have been calculated for the 185 Delta n = 0 transitions with n = 2 in the 67 C-like ions with nuclear charge number Z in the range 26 <= Z <= 92. The calculations were made for the six final, or scattered, electron energies E' = 0.03, 0.08, 0.20, 0.42, 0.80, and 1.40, where E' is in units of Z(eff)(2) Ry with Z(eff) = Z-4.17. In addition, electric dipole oscillator strengths are provided. In the present collision-strength calculations, an improved "top-up" method, which employs relativistic plane waves, was used to obtain the high partial-wave contribution for each transition, in contrast to the partial-relativistic Coulomb-Bethe approximation used in previous work by Zhang and Sampson [H.L. Zhang, D.H. Sampson, At. Data Nucl. Data Tables 63 (1996) 275]. In that earlier work, collision strengths were also provided for the same 185 Delta n = 0 transitions in C-like ions, but for the more limited list of 46 ions with Z in the range 9 <= Z <= 54. The collision strengths covered in the present work, particularly those for optically allowed transitions, should be more accurate than the corresponding data given by Zhang and Sampson [H.L. Zhang, D.H. Sampson, At. Data Nucl. Data Tables 63 (1996) 275] and are presented here to replace those earlier results. (C) 2014 Elsevier Inc. All rights reserved. C1 [Zhang, Hong Lin; Fontes, Christopher J.] Los Alamos Natl Lab, Computat Phys Div, Los Alamos, NM 87545 USA. RP Fontes, CJ (reprint author), Los Alamos Natl Lab, Computat Phys Div, POB 1663, Los Alamos, NM 87545 USA. EM cjf@lanl.gov FU U.S. Department of Energy, Los Alamos National Laboratory [DE-AC52-06NA25396] FX We would like to thank Kris Eriksen for helpful conversations concerning the modeling of low density plasmas. This work was performed under the auspices of the U.S. Department of Energy by Los Alamos National Laboratory under Contract No. DE-AC52-06NA25396. NR 45 TC 2 Z9 2 U1 2 U2 8 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 0092-640X EI 1090-2090 J9 ATOM DATA NUCL DATA JI Atom. Data Nucl. Data Tables PD JAN PY 2015 VL 101 BP 41 EP 142 DI 10.1016/j.adt.2014.08.001 PG 102 WC Physics, Atomic, Molecular & Chemical; Physics, Nuclear SC Physics GA AW8WN UT WOS:000346540300002 ER PT J AU Fontes, CJ Zhang, HL AF Fontes, Christopher J. Zhang, Hong Lin TI Relativistic distorted-wave collision strengths for the 16 Delta n=0 optically allowed transitions with n=2 in the 67 O-like ions with 26 <= Z <= 92 SO ATOMIC DATA AND NUCLEAR DATA TABLES LA English DT Article DE Electron-impact excitation collision strengths; Relativistic distorted-wave theory; Oxygen-like ions; Improved top-up method ID HIGHLY-CHARGED IONS; ELECTRON-IMPACT EXCITATION; B-LIKE IONS; POSSIBLE N=2-N=3 TRANSITIONS; N-LIKE IONS; C-LIKE IONS; OSCILLATOR-STRENGTHS; ATOMIC DATA; IRON PROJECT; 8-LESS-THAN-OR-EQUAL-TO-Z-LESS-THAN-OR-EQUAL-TO-92 AB Relativistic distorted-wave collision strengths have been calculated for the 16 Delta n = 0 optically allowed transitions with n = 2 in the 67 O-like ions with nuclear charge number Z in the range 26 <= Z <= 92. The calculations were made for the four final, or scattered, electron energies E' = 0.20, 0.42, 0.80, and 1.40, where E' is in units of Z(eff)(2) Ry with Z(eff) = Z - 5.83. In the present calculations, an improved "top-up" method, which employs relativistic plane waves, was used to obtain the high partial-wave contribution for each transition, in contrast to the partial-relativistic Coulomb-Bethe approximation used in previous work by Zhang and Sampson [H.L. Zhang, D.H. Sampson, At. Data Nucl. Data Tables 82 (2002) 357]. In that earlier work, collision strengths were also provided for O-like ions, but for a more comprehensive data set consisting of all possible 45 Delta n = 0 transitions, six scattered energies, and the 79 ions with Z in the range 14 <= Z <= 92. The collision strengths covered in the present work should be more accurate than the corresponding data given by Zhang and Sampson [H.L. Zhang, D.H. Sampson, At. Data Nucl. Data Tables 82 (2002) 357] and are presented here to replace those earlier results. (C) 2014 Elsevier Inc. All rights reserved. C1 [Fontes, Christopher J.; Zhang, Hong Lin] Los Alamos Natl Lab, Computat Phys Div, Los Alamos, NM 87545 USA. RP Fontes, CJ (reprint author), Los Alamos Natl Lab, Computat Phys Div, POB 1663, Los Alamos, NM 87545 USA. EM cjf@lanl.gov FU US Department of Energy, Los Alamos National Laboratory [DE-AC52-06NA25396] FX We would like to thank Kris Eriksen for helpful conversations concerning the modeling of astrophysical plasmas. This work was performed under the auspices of the US Department of Energy by Los Alamos National Laboratory under Contract No. DE-AC52-06NA25396. NR 39 TC 2 Z9 2 U1 1 U2 8 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 0092-640X EI 1090-2090 J9 ATOM DATA NUCL DATA JI Atom. Data Nucl. Data Tables PD JAN PY 2015 VL 101 BP 143 EP 157 DI 10.1016/j.adt.2014.08.002 PG 15 WC Physics, Atomic, Molecular & Chemical; Physics, Nuclear SC Physics GA AW8WN UT WOS:000346540300003 ER PT J AU Sugama, T Pyatina, T AF Sugama, T. Pyatina, T. TI Effect of sodium carboxymethyl celluloses on water-catalyzed self-degradation of 200 degrees C-heated alkali-activated cement SO CEMENT & CONCRETE COMPOSITES LA English DT Article DE Sodium carboxymethyl cellulose; Enhanced geothermal system; Self-degradation; Alkali-activated cement; Fly ash; Slag ID CALCIUM-PHOSPHATE CEMENT; BONE CEMENTS; GEOTHERMAL WELLS; MUD ADDITIVES; MICROSPHERES; SPECTROSCOPY; TEMPERATURE; ADSORPTION; GEOPOLYMER; FILLERS AB This paper investigates the usefulness of sodium carboxymethyl celluloses (CMC) in promoting self-degradation of 200 degrees C-heated sodium silicate-activated slag/Class C fly ash cementitious material after contact with water. CMC emitted two major volatile compounds, CO2 and acetic acid, creating a porous structure in cement. CMC also reacted with NaOH from sodium silicate to form three solid reaction products, disodium glycolate salt, sodium glucosidic salt, and sodium bicarbonate. Other solid reaction products, such as sodium polysilicate and sodium carbonate, were derived from hydrolysates of sodium silicate. Dissolution of these products upon contact with water generated heat that promoted cement's self-degradation. Thus, CMC of high molecular weight rendered two important features to the water-catalyzed self-degradation of heated cement: one was the high heat generated in exothermic reactions in cement; the other was the introduction of extensive porosity into cement. (C) 2014 The Authors. Published by Elsevier Ltd. C1 [Sugama, T.; Pyatina, T.] Brookhaven Natl Lab, Upton, NY 11973 USA. RP Pyatina, T (reprint author), Brookhaven Natl Lab, Bldg 734,Brookhaven Ave, Upton, NY 11973 USA. EM sugama@bnl.gov; tpyatina@bnl.gov FU US Department of Energy Geothermal Technology Program in the Office of Energy Efficiency and Renewable Energy; U.S. Department of Energy, Office of Basic Energy Sciences [DE-AC02-98CH10886] FX The authors would like to acknowledge the funding of the Project by the US Department of Energy Geothermal Technology Program in the Office of Energy Efficiency and Renewable Energy. The authors also would like to thank the Center for Functional Nanomaterials, Brookhaven National Laboratory, which is supported by the U.S. Department of Energy, Office of Basic Energy Sciences, under Contract No. DE-AC02-98CH10886. NR 41 TC 3 Z9 3 U1 4 U2 30 PU ELSEVIER SCI LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, OXON, ENGLAND SN 0958-9465 EI 1873-393X J9 CEMENT CONCRETE COMP JI Cem. Concr. Compos. PD JAN PY 2015 VL 55 BP 281 EP 289 DI 10.1016/j.cemconcomp.2014.09.015 PG 9 WC Construction & Building Technology; Materials Science, Composites SC Construction & Building Technology; Materials Science GA AW4AS UT WOS:000346224600031 ER PT J AU Kim, YM Zhou, Y Gao, Y Fu, JS Johnson, BA Huang, C Liu, Y AF Kim, Young-Min Zhou, Ying Gao, Yang Fu, Joshua S. Johnson, Brent A. Huang, Cheng Liu, Yang TI Spatially resolved estimation of ozone-related mortality in the United States under two representative concentration pathways (RCPs) and their uncertainty SO CLIMATIC CHANGE LA English DT Article ID GREENHOUSE-GAS EMISSIONS; CLIMATE-CHANGE; HEALTH IMPACTS; AMBIENT OZONE; AIR-POLLUTION; EXPOSURE AB The spatial pattern of the uncertainty in air pollution-related health impacts due to climate change has rarely been studied due to the lack of high-resolution model simulations, especially under the Representative Concentration Pathways (RCPs), the latest greenhouse gas emission pathways. We estimated future tropospheric ozone (O-3) and related excess mortality and evaluated the associated uncertainties in the continental United States under RCPs. Based on dynamically downscaled climate model simulations, we calculated changes in O-3 level at 12 km resolution between the future (2057 and 2059) and base years (2001-2004) under a low-to-medium emission scenario (RCP4.5) and a fossil fuel intensive emission scenario (RCP8.5). We then estimated the excess mortality attributable to changes in O-3. Finally, we analyzed the sensitivity of the excess mortality estimates to the input variables and the uncertainty in the excess mortality estimation using Monte Carlo simulations. O-3-related premature deaths in the continental U.S. were estimated to be 1312 deaths/year under RCP8.5 (95 % confidence interval (CI): 427 to 2198) and -2118 deaths/year under RCP4.5 (95 % CI: -3021 to -1216), when allowing for climate change and emissions reduction. The uncertainty of O-3-related excess mortality estimates was mainly caused by RCP emissions pathways. Excess mortality estimates attributable to the combined effect of climate and emission changes on O-3 as well as the associated uncertainties vary substantially in space and so do the most influential input variables. Spatially resolved data is crucial to develop effective community level mitigation and adaptation policy. C1 [Kim, Young-Min; Zhou, Ying; Liu, Yang] Emory Univ, Rollins Sch Publ Hlth, Dept Environm Hlth, Atlanta, GA 30322 USA. [Gao, Yang] Pacific NW Natl Lab, Atmospher Sci & Global Change Div, Richland, WA 99352 USA. [Fu, Joshua S.] Univ Tennessee, Dept Civil & Environm Engn, Knoxville, TN USA. [Johnson, Brent A.] Emory Univ, Rollins Sch Publ Hlth, Dept Biostat & Bioinformat, Atlanta, GA 30322 USA. [Huang, Cheng] George Washington Univ, Sch Publ Hlth, Milken Inst, Dept Global Hlth, Washington, DC USA. [Huang, Cheng] George Washington Univ, Sch Publ Hlth, Milken Inst, Dept Environm & Occupat Hlth, Washington, DC USA. RP Liu, Y (reprint author), Emory Univ, Rollins Sch Publ Hlth, Dept Environm Hlth, 1518 Clifton Rd NE, Atlanta, GA 30322 USA. EM yang.liu@emory.edu FU Centers for Disease Control and Prevention (CDC) [5 U01 EH000405]; National Institutes of Health (NIH) [1R21ES020225]; Office of Science of the U.S. Department of Energy [DEAC05-00OR22725]; Office of Science of the U.S. Department of Energy as part of the Regional and Global Climate Modeling Program FX This study was supported by the Centers for Disease Control and Prevention (CDC) (Grant No. 5 U01 EH000405) and by the National Institutes of Health (NIH) (Grant No. 1R21ES020225). National Science Foundation through TeraGrid resources provided by National Institute for Computational Sciences (NICS) (TG-ATM110009 and UT-TENN0006) and resources of the Oak Ridge Leadership Computing Facility at the Oak Ridge National Laboratory supported by the Office of Science of the U.S. Department of Energy (DEAC05-00OR22725) were used for the climate and air pollution model simulations. Yang Gao was partly supported by the Office of Science of the U.S. Department of Energy as part of the Regional and Global Climate Modeling Program. The Pacific Northwest National Laboratory is operated for DOE by Battelle Memorial Institute (DE-AC05-76RL01830). NR 27 TC 3 Z9 3 U1 4 U2 26 PU SPRINGER PI DORDRECHT PA VAN GODEWIJCKSTRAAT 30, 3311 GZ DORDRECHT, NETHERLANDS SN 0165-0009 EI 1573-1480 J9 CLIMATIC CHANGE JI Clim. Change PD JAN PY 2015 VL 128 IS 1-2 BP 71 EP 84 DI 10.1007/s10584-014-1290-1 PG 14 WC Environmental Sciences; Meteorology & Atmospheric Sciences SC Environmental Sciences & Ecology; Meteorology & Atmospheric Sciences GA AW4FO UT WOS:000346236800005 PM 25530644 ER PT J AU Magnotti, G Barlow, RS AF Magnotti, Gaetano Barlow, Robert S. TI Effects of high shear on the structure and thickness of turbulent premixed methane/air flames stabilized on a bluff-body burner SO COMBUSTION AND FLAME LA English DT Article DE Turbulent premixed flames; Bluff-body flames; Differential diffusion; Preferential transport; Multiscalar diagnostics ID AIR FLAMES; PREFERENTIAL DIFFUSION; FRONT STRUCTURE; SWIRLING FLOWS; CH4/AIR FLAMES; BUNSEN FLAMES; LEWIS NUMBER; COMBUSTION; TRANSPORT; RAMAN AB The effects of preferential transport and strain on the scalar structure (profiles of major species, elemental ratios) of turbulent premixed bluff-body stabilized flames are examined using line-imaged Raman/Rayleigh/CO-LIF diagnostics combined with crossed-planar Rayleigh imaging to determine the 3D flame orientation. Comparison of the experimental measurements with laminar flame calculations shows strong effects of preferential diffusion on the flame structure and the product state in lean and rich flames. Measurements of the flame orientation show a strong correlation between the flame-front normal angle and the strength of the preferential transport effects. As the flame-front angle decreases (by increasing the reactant velocity or decreasing the distance from the surface), the coupling between the preferential diffusion through the flame brush and the recirculation region is increased, enhancing the preferential transport effects. Spatial profiles and flame thickness measurements are discussed to evaluate how the strain and the turbulence affect the flame. In fuel-lean flames, as the velocity increases, eddies smaller than the flame thickness, but larger than the reaction layer, penetrate the preheat zone, improving the mixing and thickening the flame. Higher velocities are associated with higher levels of strain, which mitigate the thickening effect of the turbulence. Increases of the flame thickness up to 10% were observed. In fuel-rich flames, both the strain and the turbulence contribute to the thickening of the flame, and a flame thickness up to 2.5 times larger than the unstrained laminar thickness is observed. Changes are not limited to the preheat zone, but affect the entire flame structure. Progress variable scalar dissipation rate profiles are also discussed. Published by Elsevier Inc. on behalf of The Combustion Institute. C1 [Magnotti, Gaetano; Barlow, Robert S.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94550 USA. RP Magnotti, G (reprint author), Sandia Natl Labs, Combust Res Facil, Livermore, CA 94550 USA. EM gmagnot@sandia.gov OI Magnotti, Gaetano/0000-0002-1723-5258 FU Division of Chemical Sciences, Geosciences and Biosciences, Office of Basic Energy Sciences, US Department of Energy; United States Department of Energy [DE-AC04-94-AL85000] FX This research was funded by the Division of Chemical Sciences, Geosciences and Biosciences, Office of Basic Energy Sciences, US Department of Energy. Sandia National Laboratories is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the United States Department of Energy under contract DE-AC04-94-AL85000. Contributions by Bob Harmon in support of these experiments are gratefully acknowledged. NR 44 TC 9 Z9 9 U1 3 U2 12 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 0010-2180 EI 1556-2921 J9 COMBUST FLAME JI Combust. Flame PD JAN PY 2015 VL 162 IS 1 BP 100 EP 114 DI 10.1016/j.combustflame.2014.06.015 PG 15 WC Thermodynamics; Energy & Fuels; Engineering, Multidisciplinary; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA AW6QL UT WOS:000346393600010 ER PT J AU Junghans, A Chellappa, R Wang, P Majewski, J Luciano, G Marcelli, R Proietti, E AF Junghans, A. Chellappa, R. Wang, P. Majewski, J. Luciano, G. Marcelli, R. Proietti, E. TI Neutron reflectometry studies of aluminum-saline water interface under hydrostatic pressure SO CORROSION SCIENCE LA English DT Article DE Passive Films; Modelling studies; interfaces; Oxidation ID SEA-WATER; CORROSION AB The structural stability of Al layers in contact with 3.5 wt.% NaCl water solution was investigated at a temperature of 25 degrees C and hydrostatic pressures from 1 to 600 atm using neutron reflectometry. A pressure-temperature (P-T) Neutron Reflectometry (NR) cell developed at Los Alamos National Laboratory (LANL) was used to understand the behavior of thin (similar to 900 angstrom) aluminum layers in contact with saline liquid. Experimental results suggest that in the preliminary stages of corrosion the influence of pressure accelerates the mechanism of interactions of the oxide film with Cl- and H2O with lower speed compared to results found in the literature. (C) 2014 Elsevier Ltd. All rights reserved. C1 [Junghans, A.; Chellappa, R.; Wang, P.; Majewski, J.] Los Alamos Natl Lab, Los Alamos Neutron Sci Ctr, Los Alamos, NM 87545 USA. [Luciano, G.] CNR, ISMAR, Marine Sci Inst Genoa, Natl Res Council Italy, Venice, Italy. [Marcelli, R.; Proietti, E.] CNR, Inst Microelect & Microsyst, I-00133 Rome, Italy. RP Junghans, A (reprint author), Los Alamos Natl Lab, Los Alamos Neutron Sci Ctr, POB 1663, Los Alamos, NM 87545 USA. EM jarek@lanl.gov; giorgio.luciano@ge.ismar.cnr.it RI Junghans, Ann/A-4257-2011; Luciano, Giorgio/O-6330-2014 OI Junghans, Ann/0000-0001-7061-4663; Luciano, Giorgio/0000-0001-6353-8711 FU DOE Office of Basic Energy Sciences; Los Alamos National Laboratory under DOE [DE-AC52-06NA25396] FX This work benefited from the use of the Lujan Neutron Scattering Center at Los Alamos Neutron Science Center funded by the DOE Office of Basic Energy Sciences and Los Alamos National Laboratory under DOE Contract DE-AC52-06NA25396. NR 11 TC 4 Z9 4 U1 0 U2 11 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0010-938X EI 1879-0496 J9 CORROS SCI JI Corrosion Sci. PD JAN PY 2015 VL 90 BP 101 EP 106 DI 10.1016/j.corsci.2014.10.001 PG 6 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Materials Science; Metallurgy & Metallurgical Engineering GA AW9AC UT WOS:000346549200010 ER PT J AU Cao, FY Shi, ZM Song, GL Liu, M Dargusch, MS Atrens, A AF Cao, Fuyong Shi, Zhiming Song, Guang-Ling Liu, Ming Dargusch, Matthew S. Atrens, Andrej TI Influence of hot rolling on the corrosion behavior of several Mg-X alloys SO CORROSION SCIENCE LA English DT Article DE Magnesium; SEM; Weight loss ID HIGH-PURITY MAGNESIUM; IN-VITRO CORROSION; AZ31; PERFORMANCE; AZ91; MICROSTRUCTURE; RESISTANCE; SURFACE AB The influence of hot rolling on the corrosion of Mg-X alloys (X = Gd, Ca, Al, Mn, Sn, Sr, Nd, La, Ce, Zr or Si) was investigated by immersion tests in 3.5% NaCl solution saturated with Mg(OH)(2). The corrosion rates for all Mg-X alloys (except Mg0.1Zr and Mg0.3Si) decreased after hot rolling, attributed to fine-grained alloys having a more homogeneous microstructure, and fewer, smaller second-phase particles. For Mg0.1Zr and Mg0.3Si, the corrosion rate increased after hot rolling. There were a number of possible reasons, one of which was a greater sensitivity to the precipitation of deleterious Fe-rich particles. (C) 2014 Elsevier Ltd. All rights reserved. C1 [Cao, Fuyong; Shi, Zhiming; Song, Guang-Ling; Dargusch, Matthew S.; Atrens, Andrej] Univ Queensland, Sch Mech & Min Engn, Brisbane, Qld 4072, Australia. [Shi, Zhiming; Dargusch, Matthew S.] Univ Queensland, Ctr Adv Mat Proc & Mfg AMPAM, Brisbane, Qld 4072, Australia. [Song, Guang-Ling] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. [Liu, Ming] GM China Sci Lab, Shanghai 201206, Peoples R China. RP Atrens, A (reprint author), Univ Queensland, Sch Mech & Min Engn, Brisbane, Qld 4072, Australia. EM Andrejs.Atrens@uq.edu.au RI Song, Guang-Ling/D-9540-2013; Atrens, Andrejs/I-5850-2013; OI Song, Guang-Ling/0000-0002-9802-6836; Atrens, Andrejs/0000-0003-0671-4082; Dargusch, Matthew/0000-0003-4336-5811 FU Australian Research Council Centre of Excellence Design of Light Alloys; China Scholarship Council under the State Scholarship Fund FX This research was supported by the Australian Research Council Centre of Excellence Design of Light Alloys. Thanks to the China Scholarship Council to provide a scholarship under the State Scholarship Fund to Fuyong Cao. The authors acknowledge the facilities, and the scientific and technical assistance, of the Australian Microscopy & Microanalysis Research Facility at the Centre for Microscopy & Microanalysis, The University of Queensland. Thanks are expressed for the hot rolling which was arranged by Nicole Stanford, Institute for Frontier Materials, Deakin University, Geelong Waum Ponds Campus, Locked Bag 20000, Geelong, VIC 3220 and carried out by Mohan Setty. NR 40 TC 16 Z9 17 U1 4 U2 31 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0010-938X EI 1879-0496 J9 CORROS SCI JI Corrosion Sci. PD JAN PY 2015 VL 90 BP 176 EP 191 DI 10.1016/j.corsci.2014.10.012 PG 16 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Materials Science; Metallurgy & Metallurgical Engineering GA AW9AC UT WOS:000346549200018 ER PT J AU Telang, A Gill, AS Teysseyre, S Mannava, SR Qian, D Vasudevan, VK AF Telang, Abhishek Gill, Amrinder S. Teysseyre, Sebastien Mannava, Seetha R. Qian, Dong Vasudevan, Vijay K. TI Effects of laser shock peening on SCC behavior of Alloy 600 in tetrathionate solution SO CORROSION SCIENCE LA English DT Article DE Nickel; X-ray diffraction; TEM; Intergranular corrosion; Stress corrosion ID STRESS-CORROSION CRACKING; AUSTENITIC STAINLESS-STEEL; SENSITIZED ALLOY-600; INCONEL-600; SUSCEPTIBILITY; THIOSULFATE; FAILURE AB In this study, the effects of laser shock peening (LSP) on stress corrosion cracking (SCC) behavior of nickel based Alloy 600 in tetrathionate solution were investigated. The LSP induced compressive residual stresses and changes in the near surface microstructure, hardness were characterized. The effects of LSP on SCC susceptibility of Alloy 600 in tetrathionate solution were evaluated by slow strain rate tests and constant load tests. The results indicate a significantly longer time to failure and decreased susceptibility to SCC. These improvements were attributed to LSP induced compressive residual stresses, increased yield strength and hardening caused by near-surface microstructural changes. (C) 2014 Elsevier Ltd. All rights reserved. C1 [Telang, Abhishek; Mannava, Seetha R.; Vasudevan, Vijay K.] Univ Cincinnati, Dept Mech & Mat Engn, Cincinnati, OH 45221 USA. [Gill, Amrinder S.] AK Steel, Res Ctr, Middletown, OH 45044 USA. [Teysseyre, Sebastien] Idaho Natl Lab, Idaho Falls, ID 83415 USA. [Qian, Dong] Univ Texas Dallas, Dept Mech Engn, Richardson, TX 75080 USA. RP Telang, A (reprint author), Univ Cincinnati, Dept Mech & Mat Engn, 415 Rhodes Hall,2901 Woodside Dr, Cincinnati, OH 45221 USA. EM telangam@mail.uc.edu RI Qian, Dong/B-2326-2008 OI Qian, Dong/0000-0001-9367-0924 FU Nuclear Energy University Program (NEUP) of the US Department of Energy [102835, DE-AC07-051D14517]; State of Ohio, Department of Development and Third Frontier Commission FX The authors are grateful for financial support of this research by the Nuclear Energy University Program (NEUP) of the US Department of Energy contract #102835 issued under prime contract DE-AC07-051D14517 to Battelle Energy Alliance, LLC. We also gratefully acknowledge the contribution of the State of Ohio, Department of Development and Third Frontier Commission, which provided funding in support of "Ohio Center for Laser Shock Processing for Advanced Materials and Devices" equipment in the Center that was used in this work. The authors are also grateful for the support of David Simmermon (Cincinnati State Technical and Community College) for LSP setup. Any opinions, findings, conclusions, or recommendations expressed in these documents are those of the author(s) and do not necessarily reflect the views of the DOE, State of Ohio, Department of Development. NR 26 TC 11 Z9 11 U1 6 U2 33 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0010-938X EI 1879-0496 J9 CORROS SCI JI Corrosion Sci. PD JAN PY 2015 VL 90 BP 434 EP 444 DI 10.1016/j.corsci.2014.10.045 PG 11 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Materials Science; Metallurgy & Metallurgical Engineering GA AW9AC UT WOS:000346549200043 ER PT J AU Antonio, MR McAlister, DR Horwitz, EP AF Antonio, Mark R. McAlister, Daniel R. Horwitz, E. Philip TI An europium(III) diglycolamide complex: insights into the coordination chemistry of lanthanides in solvent extraction SO DALTON TRANSACTIONS LA English DT Article ID F-ELEMENT CATIONS; N-DODECANE; TODGA; ACTINIDES; TETRAALKYLDIGLYCOLAMIDE; AGGREGATION; ENHANCEMENT; SYSTEM; LIGAND; MEDIA AB The synthesis, stoichiometry, and structural characterization of a homoleptic, cationic europium(III) complex with three neutral tetraalkyldiglycolamide ligands are reported. The tri(bismuth tetrachloride) tris(N,N,N',N'-tetra-n-octyldiglycolamide)Eu salt, [Eu(TODGA)(3)][(BiCl4)(3)] obtained from methanol was examined by Eu L-3-edge X-ray absorption spectroscopy (XAS) to reveal an inner-sphere coordination of Eu3+ that arises from 9 O atoms and two next-nearest coordination spheres that arise from 6 carbon atoms each. A structural model is proposed in which each TODGA ligand with its O=C-a-C-b-O-C-b-C-a=O backbone acts as a tridentate O donor, where the two carbonyl O atoms and the one ether O atom bond to Eu3+. Given the structural rigidity of the tridentate coordination motif in [Eu(TODGA)(3)](3+) with six 5-membered chelate rings, the six Eu-Ca and six Eu-Cb interactions are readily resolved in the EXAFS (extended X-ray absorption fine structure) spectrum. The three charge balancing [BiCl4](-) anions are beyond the cationic [Eu(TODGA)(3)](3+) cluster in an outer sphere environment that is too distant to be detected by XAS. Despite their sizeable length and propensity for entanglement, the four n-octyl groups of each TODGA (for a total of twelve) do not perturb the Eu3+ coordination environment over that seen from previously reported single-crystal structures of tripositive lanthanide (Ln(3+)) complexes with tetraalkyldiglycolamide ligands (of the same 1 : 3 metal-to-ligand ratio stoichiometry) but having shorter i-propyl and i-butyl groups. The present results set the foundation for understanding advanced solvent extraction processes for the separation of the minor, tripositive actinides (Am, Cm) from the Ln(3+) ions in terms of the local structure of Eu3+ in a solid state coordination complex with TODGA. C1 [Antonio, Mark R.] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. [McAlister, Daniel R.; Horwitz, E. Philip] PG Res Fdn, Lisle, IL 60532 USA. RP Antonio, MR (reprint author), Argonne Natl Lab, Chem Sci & Engn Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM mantonio@anl.gov OI Antonio, Mark/0000-0002-1208-4534 FU U.S. DOE, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Biosciences and Geosciences [DE-AC02-06CH11357] FX This material and the use of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility at the Argonne National Laboratory, are based upon work supported by the U.S. DOE, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Biosciences and Geosciences, under contract no. DE-AC02-06CH11357. NR 35 TC 11 Z9 11 U1 8 U2 61 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1477-9226 EI 1477-9234 J9 DALTON T JI Dalton Trans. PY 2015 VL 44 IS 2 BP 515 EP 521 DI 10.1039/c4dt01775g PG 7 WC Chemistry, Inorganic & Nuclear SC Chemistry GA AW6YW UT WOS:000346412500015 PM 25310364 ER PT J AU Peterson, SM Helm, ML Appel, AM AF Peterson, Sonja M. Helm, Monte L. Appel, Aaron M. TI Nickel complexes of a binucleating ligand derived from an SCS pincer SO DALTON TRANSACTIONS LA English DT Article ID ORGANOPALLADIUM CROWN-ETHER; CARBON-DIOXIDE; CO2 REDUCTION; 2ND-SPHERE COORDINATION; SIMULTANEOUS 1ST-SPHERE; ELECTROCHEMICAL REACTIONS; HYDRAZINIUM ION; X-RAY; ACTIVATION; ELECTROCATALYSTS AB A binucleating ligand has been prepared that contains an SCS pincer and three oxygen donor atoms in a partial crown ether loop. To enable metalation with Ni-0, a bromoarene precursor was used and resulted in the formation of a nickel-bromide complex in the SCS pincer portion of the ligand. Reaction of the nickel complex with a lithium salt yielded a heterobimetallic complex with bromide bridging the two metal centers. The solid-state structures were determined for this heterobimetallic complex and the nickel-bromide precursor, and the two complexes were characterized electrochemically to determine the influence of coordinating the second metal. C1 [Peterson, Sonja M.; Helm, Monte L.; Appel, Aaron M.] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Appel, AM (reprint author), Pacific NW Natl Lab, POB 999,MS K2-57, Richland, WA 99352 USA. EM aaron.appel@pnnl.gov OI Appel, Aaron/0000-0002-5604-1253 FU US Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences Biosciences; Center for Molecular Electrocatalysis, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science FX The research by SMP and AMA was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences & Biosciences. The research by MLH was supported as part of the Center for Molecular Electrocatalysis, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science. Pacific Northwest National Laboratory (PNNL) is a multiprogram national laboratory operated for DOE by Battelle. NR 46 TC 3 Z9 3 U1 4 U2 29 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1477-9226 EI 1477-9234 J9 DALTON T JI Dalton Trans. PY 2015 VL 44 IS 2 BP 747 EP 752 DI 10.1039/c4dt02718c PG 6 WC Chemistry, Inorganic & Nuclear SC Chemistry GA AW6YW UT WOS:000346412500042 PM 25407101 ER PT J AU Dunn, JB Gaines, L Kelly, JC James, C Gallagher, KG AF Dunn, J. B. Gaines, L. Kelly, J. C. James, C. Gallagher, K. G. TI The significance of Li-ion batteries in electric vehicle life-cycle energy and emissions and recycling's role in its reduction SO ENERGY & ENVIRONMENTAL SCIENCE LA English DT Article ID LITHIUM-ION; ENVIRONMENTAL-IMPACT; SYSTEMS; PRICES; COBALT AB Three key questions have driven recent discussions of the energy and environmental impacts of automotive lithium-ion batteries. We address each of them, beginning with whether the energy intensity of producing all materials used in batteries or that of battery assembly is greater. Notably, battery assembly energy intensity depends on assembly facility throughput because energy consumption of equipment, especially the dry room, is mainly throughput-independent. Low-throughput facilities therefore will have higher energy intensities than near-capacity facilities. In our analysis, adopting an assembly energy intensity reflective of a low-throughput plant caused the assembly stage to dominate cradle-to-gate battery energy and environmental impact results. Results generated with an at-capacity assembly plant energy intensity, however, indicated cathode material production and aluminium use as a structural material were the drivers. Estimates of cradle-to-gate battery energy and environmental impacts must therefore be interpreted in light of assumptions made about assembly facility throughput. The second key question is whether battery recycling is worthwhile if battery assembly dominates battery cradle-to-gate impacts. In this case, even if recycled cathode materials are less energy and emissions intensive than virgin cathode materials, little energy and environmental benefit is obtained from their use because the energy consumed in assembly is so high. We reviewed the local impacts of metals recovery for cathode materials and concluded that avoiding or reducing these impacts, including SOx emissions and water contamination, is a key motivator of battery recycling regardless of the energy intensity of assembly. Finally, we address whether electric vehicles (EV) offer improved energy and environmental performance compared to internal combustion-engine vehicles (ICV). This analysis illustrated that, even if a battery assembly energy reflective of a low-throughput facility is adopted, EVs consume less petroleum and emit fewer greenhouse gases (GHG) than an ICV on a life-cycle basis. The only scenario in which an EV emitted more GHGs than an ICV was when it used solely coal-derived electricity as a fuel source. SOx emissions, however, were up to four times greater for EVs than ICVs. These emissions could be reduced through battery recycling. C1 [Dunn, J. B.; Gaines, L.; Kelly, J. C.] Argonne Natl Lab, Div Energy Syst, Argonne, IL 60439 USA. [James, C.] Michigan State Univ, Dept Chem Engn & Mat Sci, E Lansing, MI 48824 USA. [Gallagher, K. G.] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. RP Dunn, JB (reprint author), Argonne Natl Lab, Div Energy Syst, 9700 S Cass Ave, Argonne, IL 60439 USA. EM jdunn@anl.gov FU Vehicle Technologies Office of the Office of Energy Efficiency and Renewable Energy of the United States Department of Energy [DE-AC02-06CH11357] FX The authors are very grateful to Michael Wang, Amgad Elgowainy, and Jeongwoo Han for helpful communication and discussions. This work was supported by the Vehicle Technologies Office of the Office of Energy Efficiency and Renewable Energy of the United States Department of Energy, under contract DE-AC02-06CH11357. We acknowledge Dave Howell of this office for support and guidance. NR 45 TC 32 Z9 32 U1 17 U2 148 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1754-5692 EI 1754-5706 J9 ENERG ENVIRON SCI JI Energy Environ. Sci. PY 2015 VL 8 IS 1 BP 158 EP 168 DI 10.1039/c4ee03029j PG 11 WC Chemistry, Multidisciplinary; Energy & Fuels; Engineering, Chemical; Environmental Sciences SC Chemistry; Energy & Fuels; Engineering; Environmental Sciences & Ecology GA AW9FT UT WOS:000346563600009 ER PT J AU Tan, GJ Shi, FY Doak, JW Sun, H Zhao, LD Wang, PL Uher, C Wolverton, C Dravid, VP Kanatzidis, MG AF Tan, Gangjian Shi, Fengyuan Doak, Jeff W. Sun, Hui Zhao, Li-Dong Wang, Pengli Uher, Ctirad Wolverton, Chris Dravid, Vinayak P. Kanatzidis, Mercouri G. TI Extraordinary role of Hg in enhancing the thermoelectric performance of p-type SnTe SO ENERGY & ENVIRONMENTAL SCIENCE LA English DT Article ID LATTICE THERMAL-CONDUCTIVITY; INITIO MOLECULAR-DYNAMICS; TOTAL-ENERGY CALCULATIONS; AUGMENTED-WAVE METHOD; POWER-GENERATION; LEAD-TELLURIDE; BAND-STRUCTURE; BULK THERMOELECTRICS; VALENCE-BAND; PANOSCOPIC APPROACH AB We report several synergistic effects in Hg alloying of SnTe to enhance the power factor and overall figure of merit ZT. Hg alloying decreases the energy separation between the two valence bands, leading to pronounced band convergence that improves the Seebeck coefficient. Hg alloying of SnTe also significantly enlarges the band gap thereby effectively suppressing the bipolar diffusion. Collectively, this results in high ZT of similar to 1.35 at 910 K for 2% Bi-doped SnTe with 3% HgTe. The solubility limit of Hg in SnTe is less than 3 mol%, and above this level we observe HgTe precipitates in the SnTe matrix, typically trapped at grain boundary triple junctions. The strong point defect scattering of phonons caused by Hg alloying coupled with mesoscale scattering via grain boundaries contributes to a great reduction of lattice thermal conductivity. The multiple synergistic roles that Hg plays in regulating the electron and phonon transport in SnTe provide important new insights into continued optimization of SnTe-based and related materials. C1 [Tan, Gangjian; Zhao, Li-Dong; Wang, Pengli; Kanatzidis, Mercouri G.] Northwestern Univ, Dept Chem, Evanston, IL 60208 USA. [Shi, Fengyuan; Doak, Jeff W.; Wolverton, Chris; Dravid, Vinayak P.] Northwestern Univ, Dept Mat Sci & Engn, Evanston, IL 60208 USA. [Sun, Hui; Uher, Ctirad] Univ Michigan, Dept Phys, Ann Arbor, MI 48109 USA. [Kanatzidis, Mercouri G.] Argonne Natl Lab, Div Mat Sci, Argonne, IL 60439 USA. RP Tan, GJ (reprint author), Northwestern Univ, Dept Chem, 2145 Sheridan Rd, Evanston, IL 60208 USA. EM m-kanatzidis@northwestern.edu RI Sun, Hui/D-3411-2014; Dravid, Vinayak/B-6688-2009; Wolverton, Christopher/B-7542-2009; Shi, Fengyuan/Q-2584-2015; OI Sun, Hui/0000-0002-9745-3510; Shi, Fengyuan/0000-0001-9769-3824; Tan, Gangjian/0000-0002-9087-4048 FU Revolutionary Materials for Solid State Energy Conversion, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, and Office of Basic Energy Sciences [DE-SC0001054] FX This work was supported as part of the Revolutionary Materials for Solid State Energy Conversion, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, and Office of Basic Energy Sciences under Award Number DE-SC0001054. Transmission electron microscopy work was partially performed in the EPIC facility of the NUANCE Center at Northwestern University. NR 77 TC 55 Z9 55 U1 24 U2 172 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1754-5692 EI 1754-5706 J9 ENERG ENVIRON SCI JI Energy Environ. Sci. PY 2015 VL 8 IS 1 BP 267 EP 277 DI 10.1039/c4ee01463d PG 11 WC Chemistry, Multidisciplinary; Energy & Fuels; Engineering, Chemical; Environmental Sciences SC Chemistry; Energy & Fuels; Engineering; Environmental Sciences & Ecology GA AW9FT UT WOS:000346563600023 ER PT J AU Ritenour, AJ Boucher, JW DeLancey, R Greenaway, AL Aloni, S Boettcher, SW AF Ritenour, Andrew J. Boucher, Jason W. DeLancey, Robert Greenaway, Ann L. Aloni, Shaul Boettcher, Shannon W. TI Doping and electronic properties of GaAs grown by close-spaced vapor transport from powder sources for scalable III-V photovoltaics SO ENERGY & ENVIRONMENTAL SCIENCE LA English DT Article ID EPITAXIAL LAYERS; PHOTOELECTROCHEMICAL BEHAVIOR; SEMICONDUCTOR ELECTRODES; GALLIUM-ARSENIDE; WATER-VAPOR; N-GAAS; CELLS; GAP; ACETONITRILE; JUNCTIONS AB We report the use of a simple close-spaced vapor transport technique for the growth of high-quality epitaxial GaAs films using potentially inexpensive GaAs powders as precursors. The free carrier type and density (10(16) to 10(19) cm(-3)) of the films were adjusted by addition of Te or Zn powder to the GaAs source powder. We show using photoelectrochemical and electron beam-induced current analyses that the minority carrier diffusion lengths of the n- and p-GaAs films reached similar to 3 mu m and similar to 8 mu m, respectively. Hall mobilities approach those achieved for GaAs grown by metal-organic chemical vapor deposition, 1000-4200 cm(2) V-1 s(-1) for n-GaAs and 50-240 cm V-1 s(-1) for p-GaAs depending on doping level. We conclude that the electronic quality of GaAs grown by close-spaced vapor transport is similar to that of GaAs made using conventional techniques and is thus sufficient for high-performance photovoltaic applications. C1 [Ritenour, Andrew J.; Greenaway, Ann L.; Boettcher, Shannon W.] Univ Oregon, Dept Chem & Biochem, Eugene, OR 97403 USA. [Boucher, Jason W.; DeLancey, Robert] Univ Oregon, Dept Phys, Eugene, OR 97403 USA. [Aloni, Shaul] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA. RP Ritenour, AJ (reprint author), Univ Oregon, Dept Chem & Biochem, Eugene, OR 97403 USA. EM swb@uoregon.edu RI Foundry, Molecular/G-9968-2014; OI Greenaway, Ann/0000-0001-6681-9965 FU Department of Energy (DOE) SunShot Initiative BRIDGE program [DE-EE0005957]; Julie and Rocky Dixon Graduate Innovation Fellowship; NSF [DGE-0829517]; Research Corporation for Science Advancement as a Cottrell Scholar; Molecular Foundry; Lawrence Berkeley National Laboratory; U.S. DOE Office of Science, Office of Basic Energy Sciences [DE-AC02-05CH1123]; W.M Keck Foundation; M.J. Murdock Charitable Trust; ONAMI; Oregon Built Environment and Sustainable Technologies FX This work was supported by the Department of Energy (DOE) SunShot Initiative BRIDGE program (DE-EE0005957). AR acknowledges support from the Julie and Rocky Dixon Graduate Innovation Fellowship. AG acknowledges support from a NSF Graduate Research Fellowship (DGE-0829517). SB acknowledges support from Research Corporation for Science Advancement as a Cottrell Scholar. We acknowledge support from the user program at the Molecular Foundry, Lawrence Berkeley National Laboratory, with funding from the U.S. DOE Office of Science, Office of Basic Energy Sciences under Contract DE-AC02-05CH1123. The CAMCOR shared instrument facilities are supported by grants from the W.M Keck Foundation, the M.J. Murdock Charitable Trust, ONAMI, and NSF. The SUNRISE Photovoltaic Laboratory is supported by Oregon Built Environment and Sustainable Technologies. Assistance from Fuding Lin, Adam Smith, Stephen Golledge, Fred Stevie, Kris Johnson, Jeff Garmin, John Boosinger, Cliff Dax, Alex Negrete, Richard Cramer, Solomon Levinrad, Athavan Nadarajah, Lena Trotochaud, Matthew Kast, Sangeun Chun, Michaela Burke, T.J. Mills, Adam Batchellor and David Senkovich is acknowledged. NR 61 TC 12 Z9 12 U1 0 U2 21 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1754-5692 EI 1754-5706 J9 ENERG ENVIRON SCI JI Energy Environ. Sci. PY 2015 VL 8 IS 1 BP 278 EP 285 DI 10.1039/c4ee01943a PG 8 WC Chemistry, Multidisciplinary; Energy & Fuels; Engineering, Chemical; Environmental Sciences SC Chemistry; Energy & Fuels; Engineering; Environmental Sciences & Ecology GA AW9FT UT WOS:000346563600024 ER PT J AU Scofield, ME Koenigsmann, C Wang, L Liu, HQ Wong, SS AF Scofield, Megan E. Koenigsmann, Christopher Wang, Lei Liu, Haiqing Wong, Stanislaus S. TI Tailoring the composition of ultrathin, ternary alloy PtRuFe nanowires for the methanol oxidation reaction and formic acid oxidation reaction SO ENERGY & ENVIRONMENTAL SCIENCE LA English DT Article ID OXYGEN REDUCTION REACTION; TEMPERATURE FUEL-CELLS; ELECTROCATALYTIC PERFORMANCE; CATALYTIC PERFORMANCE; QUANTITATIVE DEMS; CARBON-MONOXIDE; ANODE CATALYSTS; ELECTROOXIDATION; NI; NANOPARTICLES AB In the search for alternatives to conventional Pt electrocatalysts, we have synthesized ultrathin, ternary PtRuFe nanowires (NW), possessing different chemical compositions in order to probe their CO tolerance as well as electrochemical activity as a function of composition for both (i) the methanol oxidation reaction (MOR) and (ii) the formic acid oxidation reaction (FAOR). As-prepared 'multifunctional' ternary NW catalysts exhibited both higher MOR and FAOR activity as compared with mono-metallic Pt NWs, binary Pt7Ru3 and Pt7Fe3 NWs, and commercial catalyst control samples. In terms of synthetic novelty, we utilized a sustainably mild, ambient wet-synthesis method never previously applied to the fabrication of crystalline, pure ternary systems in order to fabricate ultrathin, homogeneous alloy PtRuFe NWs with a range of controlled compositions. These NWs were subsequently characterized using a suite of techniques including XRD, TEM, SAED, and EDAX in order to verify not only the incorporation of Ru and Fe into the Pt lattice but also their chemical homogeneity, morphology, as well as physical structure and integrity. Lastly, these NWs were electrochemically tested in order to deduce the appropriateness of conventional explanations such as (i) the bi-functional mechanism as well as (ii) the ligand effect to account for our MOR and FAOR reaction data. Specifically, methanol oxidation appears to be predominantly influenced by the Ru content, whereas formic acid oxidation is primarily impacted by the corresponding Fe content within the ternary metal alloy catalyst itself. C1 [Scofield, Megan E.; Koenigsmann, Christopher; Wang, Lei; Liu, Haiqing; Wong, Stanislaus S.] SUNY Stony Brook, Dept Chem, Stony Brook, NY 11794 USA. [Wong, Stanislaus S.] Brookhaven Natl Lab, Condensed Matter Phys & Mat Sci Dept, Upton, NY 11973 USA. RP Scofield, ME (reprint author), SUNY Stony Brook, Dept Chem, Stony Brook, NY 11794 USA. EM stanislaus.wong@stonybrook.edu FU U.S. Department of Energy, Basic Energy Sciences, Materials Sciences and Engineering Division; U.S. Department of Energy [DE-AC02-98CH10886] FX Research for all authors was supported by the U.S. Department of Energy, Basic Energy Sciences, Materials Sciences and Engineering Division. Experiments for this manuscript were performed in part at the Center for Functional Nanomaterials located at Brookhaven National Laboratory, which is supported by the U.S. Department of Energy under Contract no. DE-AC02-98CH10886. We thank James Quinn (SUNY Stony Brook) for assistance with EDAX measurements. NR 52 TC 55 Z9 55 U1 29 U2 149 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1754-5692 EI 1754-5706 J9 ENERG ENVIRON SCI JI Energy Environ. Sci. PY 2015 VL 8 IS 1 BP 350 EP 363 DI 10.1039/c4ee02162b PG 14 WC Chemistry, Multidisciplinary; Energy & Fuels; Engineering, Chemical; Environmental Sciences SC Chemistry; Energy & Fuels; Engineering; Environmental Sciences & Ecology GA AW9FT UT WOS:000346563600031 ER PT J AU Chabaud, BM Brock, JS Williams, TO AF Chabaud, Brandon M. Brock, Jerry S. Williams, Todd O. TI Benchmark analytic solution of the dynamic sphere problem for Bodner-Partom elastic-viscoplastic materials SO EUROPEAN JOURNAL OF MECHANICS A-SOLIDS LA English DT Article DE Dynamic sphere problem; Bodner-Partom viscoplasticity; Benchmark analytic solution ID RADIATIVE SHOCK SOLUTIONS; DIFFUSION; MODEL AB Developing benchmark analytic solutions for problems in solid and fluid mechanics is important for the purpose of testing and verifying computational physics codes. In order to test the numerical results of physics codes that predict the response of elastic-viscoplastic materials, we consider the geometrically linear dynamic sphere problem. We present an exact solution for the dynamic response of a spherical shell composed of a linearly elastic-viscoplastic material exhibiting isotropic symmetry. The solution takes the form of an infinite series of eigenfunctions. We demonstrate, both qualitatively and quantitatively, the convergence of the computed benchmark solution under spatial, temporal, and eigenmode refinement. We also use our computational benchmark solution to compute viscoplastic strains on a spherical shell composed of titanium. (C) 2014 Elsevier Masson SAS. All rights reserved. C1 [Chabaud, Brandon M.; Brock, Jerry S.; Williams, Todd O.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Chabaud, BM (reprint author), Los Alamos Natl Lab, MS B-259, Los Alamos, NM 87545 USA. EM chabaud@lanl.gov; jsbrock@lanl.gov; oakhill@lanl.gov NR 25 TC 1 Z9 1 U1 0 U2 1 PU GAUTHIER-VILLARS/EDITIONS ELSEVIER PI PARIS PA 23 RUE LINOIS, 75015 PARIS, FRANCE SN 0997-7538 EI 1873-7285 J9 EUR J MECH A-SOLID JI Eur. J. Mech. A-Solids PD JAN-FEB PY 2015 VL 49 BP 114 EP 124 DI 10.1016/j.euromechsol.2014.07.006 PG 11 WC Mechanics SC Mechanics GA AW8XG UT WOS:000346542100010 ER PT J AU Tomasi, D Wang, GJ Wang, RL Caparelli, EC Logan, J Volkow, ND AF Tomasi, Dardo Wang, Gene-Jack Wang, Ruiliang Caparelli, Elisabeth C. Logan, Jean Volkow, Nora D. TI Overlapping Patterns of Brain Activation to Food and Cocaine Cues in Cocaine Abusers: Association to Striatal D2/D3 Receptors SO HUMAN BRAIN MAPPING LA English DT Review DE reward; addiction; obesity; fMRI; PET ID NUCLEUS-ACCUMBENS CORE; VENTRAL TEGMENTAL AREA; DOPAMINE RELEASE; SEEKING BEHAVIOR; MESOLIMBIC DOPAMINE; SYNAPTIC PLASTICITY; DEPENDENT PATIENTS; CAUDATE-NUCLEUS; DORSAL STRIATUM; C-11 RACLOPRIDE AB Cocaine, through its activation of dopamine (DA) signaling, usurps pathways that process natural rewards. However, the extent to which there is overlap between the networks that process natural and drug rewards and whether DA signaling associated with cocaine abuse influences these networks have not been investigated in humans. We measured brain activation responses to food and cocaine cues with fMRI, and D2/D3 receptors in the striatum with [C-11]raclopride and Positron emission tomography in 20 active cocaine abusers. Compared to neutral cues, food and cocaine cues increasingly engaged cerebellum, orbitofrontal, inferior frontal, and premotor cortices and insula and disengaged cuneus and default mode network (DMN). These fMRI signals were proportional to striatal D2/D3 receptors. Surprisingly cocaine and food cues also deactivated ventral striatum and hypothalamus. Compared to food cues, cocaine cues produced lower activation in insula and postcentral gyrus, and less deactivation in hypothalamus and DMN regions. Activation in cortical regions and cerebellum increased in proportion to the valence of the cues, and activation to food cues in somatosensory and orbitofrontal cortices also increased in proportion to body mass. Longer exposure to cocaine was associated with lower activation to both cues in occipital cortex and cerebellum, which could reflect the decreases in D2/D3 receptors associated with chronicity. These findings show that cocaine cues activate similar, though not identical, pathways to those activated by food cues and that striatal D2/D3 receptors modulate these responses, suggesting that chronic cocaine exposure might influence brain sensitivity not just to drugs but also to food cues. Hum Brain Mapp, 36:120-136, 2015. (c) 2014 Wiley Periodicals, Inc. C1 [Tomasi, Dardo; Wang, Gene-Jack; Volkow, Nora D.] NIAAA, NIH, Bethesda, MD USA. [Wang, Ruiliang] Brookhaven Natl Lab, Dept Med, Upton, NY 11973 USA. [Caparelli, Elisabeth C.; Volkow, Nora D.] NIDA, NIH, Bethesda, MD 20892 USA. [Logan, Jean] NYU, Dept Psychiat, New York, NY 10016 USA. RP Tomasi, D (reprint author), 5635 Fishers Lane, Bethesda, MD 20892 USA. EM tomasidg@mail.nih.gov RI Tomasi, Dardo/J-2127-2015; OI Logan, Jean/0000-0002-6993-9994 FU National Institutes of Alcohol Abuse and Alcoholism; Intramural Research Program National Institute on Alcohol Abuse and Alcoholism (NIAAA) [Y1AA3009] FX Contract grant sponsor: National Institutes of Alcohol Abuse and Alcoholism; Intramural Research Program National Institute on Alcohol Abuse and Alcoholism (NIAAA) #Y1AA3009. NR 101 TC 20 Z9 20 U1 3 U2 22 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 1065-9471 EI 1097-0193 J9 HUM BRAIN MAPP JI Hum. Brain Mapp. PD JAN PY 2015 VL 36 IS 1 BP 120 EP 136 DI 10.1002/hbm.22617 PG 17 WC Neurosciences; Neuroimaging; Radiology, Nuclear Medicine & Medical Imaging SC Neurosciences & Neurology; Radiology, Nuclear Medicine & Medical Imaging GA AW3ML UT WOS:000346190800010 PM 25142207 ER PT J AU Liu, GX Shen, HY Ward, L AF Liu, Guoxin Shen, Haiying Ward, Lee TI An Efficient and Trustworthy P2P and Social Network Integrated File Sharing System SO IEEE TRANSACTIONS ON COMPUTERS LA English DT Article DE Peer-to-peer (P2P) systems; file searching; file replication; social networks; proximity; churn ID TO-PEER SYSTEM; SMALL-WORLD; SEARCH; LOCALITY; OVERLAY AB Efficient and trustworthy file querying is important to the overall performance of peer-to-peer (P2P) file sharing systems. Emerging methods are beginning to address this challenge by exploiting online social networks (OSNs). However, current OSN-based methods simply cluster common-interest nodes for high efficiency or limit the interaction between social friends for high trustworthiness, which provides limited enhancement or contradicts the open and free service goal of P2P systems. Little research has been undertaken to fully and cooperatively leverage OSNs with integrated consideration of proximity and interest. In this work, we analyze a BitTorrent file sharing trace, which proves the necessity of proximity-and interest-aware clustering. Based on the trace study and OSN properties, we propose a social network integrated P2P file sharing system with enhanced efficiency and trustworthiness (SOCNET) to fully and cooperatively leverage the common-interest, proximity-close, and trust properties of OSN friends. SOCNET uses a hierarchical distributed hash table (DHT) to cluster common-interest nodes, then further cluster proximity-close nodes into a subcluster, and connects the nodes in a subcluster with social links. Thus, when queries travel along trustable social links, they also gain higher probability of being successfully resolved by proximity-close nodes, and it simultaneously enhances efficiency and trustworthiness. We further propose different strategies to guide nodes to forward a file query to friends that are more trustworthy and more likely to resolve the queries or forward the query to file holders. We also propose follower-and cluster-based file replication algorithms to enhance file search efficiency. The results of trace-driven experiments on the real-world PlanetLab testbed demonstrate the higher efficiency, trustworthiness, and dynamism-resilience of SOCNET compared with other systems. Experimental results also confirm the effectiveness of the proposed strategies to improve SOCNET's performance. C1 [Liu, Guoxin; Shen, Haiying] Clemson Univ, Dept Elect & Comp Engn, Clemson, SC 29634 USA. [Ward, Lee] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Liu, GX (reprint author), Clemson Univ, Dept Elect & Comp Engn, Clemson, SC 29634 USA. EM guoxinl@clemson.edu; shenh@clemson.edu; lee@sandia.gov FU U.S. NSF [IIS-1354123, CNS-1254006, CNS-1249603, OCI-1064230, CNS-1049947, CNS-0917056, CNS-1025652]; Microsoft Research Faculty Fellowship [8300751]; U.S. Department of Energy's Oak Ridge National Laboratory; Extreme Scale Systems Center located at ORNL; DoD [4000111689] FX We would like to thank Dr. Andy Pavlo in Brown University for providing the BitTorrent trace data. This research was supported in part by U.S. NSF Grants IIS-1354123, CNS-1254006, CNS-1249603, OCI-1064230, CNS-1049947, CNS-0917056, and CNS-1025652, Microsoft Research Faculty Fellowship 8300751, and U.S. Department of Energy's Oak Ridge National Laboratory including the Extreme Scale Systems Center located at ORNL and DoD 4000111689. An early version of this work was presented in the Proceedings of the IEEE International Conference on Peer-to-Peer Computing (P2P'12) [51]. NR 48 TC 4 Z9 7 U1 0 U2 9 PU IEEE COMPUTER SOC PI LOS ALAMITOS PA 10662 LOS VAQUEROS CIRCLE, PO BOX 3014, LOS ALAMITOS, CA 90720-1314 USA SN 0018-9340 EI 1557-9956 J9 IEEE T COMPUT JI IEEE Trans. Comput. PD JAN PY 2015 VL 64 IS 1 BP 54 EP 70 DI 10.1109/TC.2013.201 PG 17 WC Computer Science, Hardware & Architecture; Engineering, Electrical & Electronic SC Computer Science; Engineering GA AW9JB UT WOS:000346572100007 ER PT J AU Gundlach-Graham, A Dennis, EA Ray, SJ Enke, CG Barinaga, CJ Koppenaal, DW Hieftje, GM AF Gundlach-Graham, Alexander Dennis, Elise A. Ray, Steven J. Enke, Christie G. Barinaga, Charles J. Koppenaal, David W. Hieftje, Gary M. TI Laser-ablation sampling for inductively coupled plasma distance-of-flight mass spectrometry SO JOURNAL OF ANALYTICAL ATOMIC SPECTROMETRY LA English DT Article ID HIGH-SPATIAL-RESOLUTION; X-RAY FLUORESCENCE; ICP-MS; GEOLOGICAL-MATERIALS; TRANSIENT SIGNALS; ARRAY DETECTOR; 266 NM; CAPABILITIES; SPECTROGRAPH; PERFORMANCE AB An inductively coupled plasma distance-of-flight mass spectrometer (ICP-DOFMS) has been coupled with laser-ablation (LA) sample introduction for the elemental analysis of solids. ICP-DOFMS is well suited for the analysis of laser-generated aerosols because it offers both high-speed mass analysis and simultaneous multi-elemental detection. Here, we evaluate the analytical performance of the LA-ICP-DOFMS instrument, equipped with a microchannel plate-based imaging detector, for the measurement of steady-state LA signals, as well as transient signals produced from single LA events. Steady-state detection limits are 1 mu g g(-1), and absolute single-pulse LA detection limits are 200 fg for uranium; the system is shown capable of performing time-resolved single-pulse LA analysis. By leveraging the benefits of simultaneous multi-elemental detection, we also attain a good shot-to-shot reproducibility of 6% relative standard deviation (RSD) and isotope-ratio precision of 0.3% RSD with a 10 s integration time. C1 [Gundlach-Graham, Alexander; Dennis, Elise A.; Ray, Steven J.; Enke, Christie G.; Hieftje, Gary M.] Indiana Univ, Dept Chem, Bloomington, IN 47405 USA. [Enke, Christie G.] Univ New Mexico, Dept Chem, Albuquerque, NM 87131 USA. [Barinaga, Charles J.; Koppenaal, David W.] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Hieftje, GM (reprint author), Indiana Univ, Dept Chem, Bloomington, IN 47405 USA. EM hieftje@indiana.edu RI Gundlach-Graham, Alexander/B-6069-2011; OI Gundlach-Graham, Alexander/0000-0003-4806-6255; Ray, Steven/0000-0001-5675-1258 FU Division of Analytical Chemistry (DAC) of the American Chemistry Society; Indiana University, Department of Chemistry under the Briscoe Teacher-Scholar fellowship program; U.S. Department of Energy [DE-FG02-98ER14890]; National Science Foundation [DBI-1062846]; US DOE [DE-AC06-76RLO-1830op]; Agilent Technologies FX Alexander Gundlach-Graham thanks the Division of Analytical Chemistry (DAC) of the American Chemistry Society and Agilent Technologies for a DAC graduate-research fellowship. AGG also thanks Indiana University, Department of Chemistry for support under the Briscoe Teacher-Scholar fellowship program. Partial salary support was provided by the U.S. Department of Energy through grant DE-FG02-98ER14890. This research was also supported in part by the National Science Foundation through Grant DBI-1062846 and performed in collaboration with Pacific Northwest National Laboratory, operated for the US DOE by Battelle Memorial Institute under Contract DE-AC06-76RLO-1830op. NR 54 TC 7 Z9 7 U1 2 U2 21 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 0267-9477 EI 1364-5544 J9 J ANAL ATOM SPECTROM JI J. Anal. At. Spectrom. PY 2015 VL 30 IS 1 BP 139 EP 147 DI 10.1039/c4ja00231h PG 9 WC Chemistry, Analytical; Spectroscopy SC Chemistry; Spectroscopy GA AW4LE UT WOS:000346251800008 ER PT J AU Konegger-Kappel, S Manard, BT Zhang, LX Konegger, T Marcus, RK AF Konegger-Kappel, Stefanie Manard, Benjamin T. Zhang, Lynn X. Konegger, Thomas Marcus, R. Kenneth TI Liquid sampling-atmospheric pressure glow discharge excitation of atomic and ionic species SO JOURNAL OF ANALYTICAL ATOMIC SPECTROMETRY LA English DT Article ID LINE INTENSITY RATIOS; LASER-INDUCED PLASMA; OPTICAL-EMISSION SPECTROMETRY; APGD IONIZATION SOURCE; MASS-SPECTROMETRY; ELEMENTAL FRACTIONATION; SPECTROSCOPY; ABLATION; MICROPLASMAS; BRASS AB The liquid sampling-atmospheric pressure glow discharge (LS-APGD) was characterized with respect to the effects of interrelated operational source parameters on the excitation of atomic (I) and ionic (II) states for expanding the fundamental understanding of this microplasma's characteristics as an excitation source for optical emission spectroscopy (OES) analyses. Parameters that were investigated for identifying the key driving forces for atomic and ionic excitation conditions were discharge current, interelectrode gap, and He sheath and counter gas flows. The addition of the He counter gas flow allowed assessment of the additional parameter relevant when aerosol samples are introduced following laser ablation sampling of solid matrices. The introduction of the analytes (500 mu g g(-1) copper and zinc in 2% HNO3) in liquid form through the solution capillary permitted the investigation of source parameter effects, without introducing additional influences from solid sampling such as heterogeneous particle populations. Individual driving forces for excitation/ionization conditions and inter-parametric dependencies were assessed by changing the operating conditions according to a design of experiment (DOE) plan and monitoring Zn and Cu atomic and ionic emission lines (Zn I 213.9 nm, Cu I 324.7 nm, Zn I 481.1 nm, and Zn II 202.5 nm). Pareto plots of standardized effects were used for evaluating levels of significance as well as magnitudes of both individual and inter-active parametric effects on emission responses, background emissions and signal-to-background ratios as well as the LS-APGD's tolerance against changes in excitation conditions (i.e. robustness). The results indicate that parameter settings leading to high plasma power density are the key driving forces for enhanced analyte emission, with the interelectrode distances showing the most pronounced influences for the investigated parameter space. C1 [Konegger-Kappel, Stefanie; Zhang, Lynn X.; Marcus, R. Kenneth] Clemson Univ, Dept Chem, Clemson, SC 29634 USA. [Manard, Benjamin T.] Los Alamos Natl Lab, Chem Div Actinide Analyt Chem, Los Alamos, NM 87544 USA. [Konegger, Thomas] Clemson Univ, Dept Mat Sci & Engn, Clemson, SC 29634 USA. RP Marcus, RK (reprint author), Clemson Univ, Dept Chem, Clemson, SC 29634 USA. EM marcusr@clemson.edu FU Defense Threat Reduction Agency, Basic Research Award [HDTRA1-14-1-0010] FX This work was supported by the Defense Threat Reduction Agency, Basic Research Award # HDTRA1-14-1-0010, to Clemson University. NR 42 TC 4 Z9 4 U1 3 U2 32 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 0267-9477 EI 1364-5544 J9 J ANAL ATOM SPECTROM JI J. Anal. At. Spectrom. PY 2015 VL 30 IS 1 BP 285 EP 295 DI 10.1039/c4ja00302k PG 11 WC Chemistry, Analytical; Spectroscopy SC Chemistry; Spectroscopy GA AW4LE UT WOS:000346251800024 ER PT J AU Lin, Z Liang, CD AF Lin, Zhan Liang, Chengdu TI Lithium-sulfur batteries: from liquid to solid cells SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Review ID LI-S BATTERIES; COMPOSITE CATHODE MATERIALS; CAPACITY FADING MECHANISMS; HIGH-PERFORMANCE CATHODE; GEL POLYMER ELECTROLYTE; GLYCOL) DIMETHYL ETHER; HIGH SPECIFIC ENERGY; HIGH-RATE CAPABILITY; X-RAY-DIFFRACTION; LONG CYCLE LIFE AB Lithium-sulfur (Li-S) batteries supply a theoretical specific energy 5 times higher than that of lithium-ion batteries (2500 vs. similar to 500 W h kg(-1)). However, the insulating properties and polysulfide shuttle effects of the sulfur cathode and safety concerns of the lithium anode in liquid electrolytes are still key limitations to practical use of traditional Li-S batteries. In this review, we start with a brief discussion on fundamentals of Li-S batteries and key challenges associated with conventional liquid cells. We then introduce the most recent progress in liquid systems, including sulfur positive electrodes, lithium negative electrodes, and electrolytes and binders. We discuss the significance of investigating electrode reaction mechanisms in liquid cells using in situ techniques to monitor the compositional and morphological changes. We also discuss the importance of this game-changing shift, moving from traditional liquid cells to recently developed solid cells, with positive advances in both solid electrolytes and electrode materials. Finally, the opportunities and perspectives for future research on Li-S batteries are presented. C1 [Lin, Zhan] Zhejiang Univ, Coll Chem & Biol Engn, Hangzhou 310027, Zhejiang, Peoples R China. [Liang, Chengdu] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. RP Liang, CD (reprint author), Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. EM liangcn@ornl.gov RI Lin, Zhan/C-6806-2011 OI Lin, Zhan/0000-0001-5009-8198 FU Division of Materials Sciences and Engineering, Office of Basic Energy Sciences, US Department of Energy (DOE) FX This work was sponsored by the Division of Materials Sciences and Engineering, Office of Basic Energy Sciences, US Department of Energy (DOE). NR 185 TC 85 Z9 85 U1 82 U2 611 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7488 EI 2050-7496 J9 J MATER CHEM A JI J. Mater. Chem. A PY 2015 VL 3 IS 3 BP 936 EP 958 DI 10.1039/c4ta04727c PG 23 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA AW6YB UT WOS:000346410400001 ER PT J AU Jang, GG Jacobs, CB Gresback, RG Ivanov, IN Meyer, HM Kidder, M Joshi, PC Jellison, GE Phelps, TJ Graham, DE Moon, JW AF Jang, Gyoung Gug Jacobs, Christopher B. Gresback, Ryan G. Ivanov, Ilia N. Meyer, Harry M., III Kidder, Michelle Joshi, Pooran C. Jellison, Gerald E., Jr. Phelps, Tommy J. Graham, David E. Moon, Ji-Won TI Size tunable elemental copper nanoparticles: extracellular synthesis by thermoanaerobic bacteria and capping molecules SO JOURNAL OF MATERIALS CHEMISTRY C LA English DT Article ID OXIDE NANOPARTICLES; CU NANOPARTICLES; METAL; ENVIRONMENTS; FABRICATION; FILMS; INK AB Bimodal sized elemental copper (Cu) nanoparticles (NPs) were synthesized from inexpensive oxidized copper salts by an extracellular metal-reduction process using anaerobic Thermoanaerobacter sp. X513 bacteria in aqueous solution. The bacteria nucleate NPs outside of the cell, and they control the Cu2+ reduction rate to form uniform crystallites with an average diameter of 1.75 + 0.46 mu m after 3 days incubation. To control the size and enhance the air stability of Cu NPs, the reaction mixtures were supplemented with nitrilotriacetic acid as a chelator, and the surfactant capping agents oleic acid, oleylamine, ascorbic acid, or L-cysteine. Time-dependent UV-visible absorption measurements and XPS studies indicated well-suspended, bimodal colloidal Cu NPs (70-150 and 5-10 nm) with extended air-stability up to 300 min and stable Cu NP film surfaces with 14% oxidation after 20 days. FTIR spectroscopy suggested that these capping agents were effectively adsorbed on the NP surface providing oxidation resistance under aqueous and dry conditions. Compared to previously reported Cu NP syntheses, this biological process substantially reduced the requirement for hazardous organic solvents and chemical reducing agents, while reducing the levels of Cu oxide impurities in the product. This process was highly reproducible and scalable from 0.01 to 1 L batches. C1 [Jang, Gyoung Gug; Phelps, Tommy J.; Graham, David E.; Moon, Ji-Won] Oak Ridge Natl Lab, Biosci Div, Oak Ridge, TN 37831 USA. [Jacobs, Christopher B.; Gresback, Ryan G.; Ivanov, Ilia N.] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci Div, Oak Ridge, TN 37831 USA. [Meyer, Harry M., III; Joshi, Pooran C.; Jellison, Gerald E., Jr.] Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. [Kidder, Michelle] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. RP Moon, JW (reprint author), Oak Ridge Natl Lab, Biosci Div, Oak Ridge, TN 37831 USA. EM moonj@ornl.gov RI ivanov, ilia/D-3402-2015; Graham, David/F-8578-2010; Moon, Ji-Won/A-9186-2011; OI ivanov, ilia/0000-0002-6726-2502; Graham, David/0000-0001-8968-7344; Moon, Ji-Won/0000-0001-7776-6889; Jacobs, Christopher/0000-0001-7906-6368 FU US Department of Energy (DOE); Advanced Manufacturing Office, Low Temperature Material Synthesis Program [CPS 24762]; Oak Ridge National Laboratory (ORNL); ORNL Scientific User Facilities Division; DOE Office of Basic Research Sciences; US DOE, Office of Science, Basic Energy Sciences [ERKCC96]; UT-Battelle, LLC, for DOE [DE-AC05-00OR22725] FX The authors gratefully acknowledge the support from the US Department of Energy (DOE), Advanced Manufacturing Office, Low Temperature Material Synthesis Program (CPS 24762) and the Oak Ridge National Laboratory (ORNL). Part of this research was conducted at the Center for Nanophase Materials Sciences, which is sponsored by the ORNL Scientific User Facilities Division and DOE Office of Basic Research Sciences. FTIR work provided by M. K. K. was supported by the US DOE, Office of Science, Basic Energy Sciences under Award ERKCC96. We appreciate helpful comments about NP properties from Beth Armstrong. ORNL is managed by UT-Battelle, LLC, for DOE under contract DE-AC05-00OR22725. The U.S. Government is authorized to reproduce and distribute reprints for Government purposes notwithstanding any copyright notation hereon. G.G.J. performed synthesis experiments, analyzed data, and prepared text for the manuscript. C. B. J., R. G. G. and I.N.I. carried out SEM, TEM, TGA and other imaging experiments. H. M. M. assisted in XPS and analysis of its results. M. K. performed FTIR and its analysis. P. C. J. and G. E. J. assisted in developing electrical analysis apparatus and methods and reviewing electrical analysis. T. J. P. provided constructive guidance and comments about the manuscript. D. E. G. and J. M. directed the work, organized its presentation and finalized the text. NR 34 TC 8 Z9 8 U1 5 U2 41 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7526 EI 2050-7534 J9 J MATER CHEM C JI J. Mater. Chem. C PY 2015 VL 3 IS 3 BP 644 EP 650 DI 10.1039/c4tc02356k PG 7 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA AW9ID UT WOS:000346569700020 ER PT J AU Sistrunk, E Guhr, M AF Sistrunk, Emily Guehr, Markus TI Extreme ultraviolet spectrometer based on a transmission electron microscopy grid SO JOURNAL OF OPTICS LA English DT Article DE high harmonic generation; extreme ultraviolet; ultrafast optics ID ACHROMATIC INTERFEROMETRIC LITHOGRAPHY; ORDER HARMONIC-GENERATION; DYNAMICS; GRATINGS; LASER AB We performed extreme ultraviolet spectroscopy using an 80 lines/mm transmission electron microscope mesh as the dispersive element. We present the usefulness of this instrument for dispersing a high harmonic spectrum from the 13th to the 29th harmonic of a Ti: sapph laser, corresponding to a wavelength range from 60 to 27 nm. The resolution of the instrument is limited by the image size of the high harmonic generation region on the detector. The resolution in first order diffraction is under 2 nm over the entire spectral range with a resolving power around 30. C1 [Sistrunk, Emily; Guehr, Markus] SLAC Natl Accelerator Lab, PULSE Inst, Menlo Pk, CA 94025 USA. [Sistrunk, Emily] Lawrence Livermore Natl Lab, NIF, Livermore, CA 94550 USA. [Sistrunk, Emily] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. RP Sistrunk, E (reprint author), SLAC Natl Accelerator Lab, PULSE Inst, 2575 Sand Hill Rd, Menlo Pk, CA 94025 USA. EM mguehr@stanford.edu RI Guehr, Markus/B-7446-2015 OI Guehr, Markus/0000-0002-9111-8981 FU Office of Science Early Career Research Program through the Office of Basic Energy Sciences, US Department of Energy; AMOS program within the Chemical Sciences, Geosciences, and Biosciences Division of the Office of Basic Energy Sciences, Office of Science, US Department of Energy FX We acknowledge discussions and/or experimental support with/from J Grilj, TJA Wolf, M Koch and A Belkacem. MG acknowledges funding via the Office of Science Early Career Research Program through the Office of Basic Energy Sciences, US Department of Energy. This work was supported by the AMOS program within the Chemical Sciences, Geosciences, and Biosciences Division of the Office of Basic Energy Sciences, Office of Science, US Department of Energy. NR 28 TC 0 Z9 0 U1 2 U2 13 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 2040-8978 EI 2040-8986 J9 J OPTICS-UK JI J. Opt. PD JAN PY 2015 VL 17 IS 1 AR 015502 DI 10.1088/2040-8978/17/1/015502 PG 4 WC Optics SC Optics GA AW7XD UT WOS:000346473900010 ER PT J AU Barrett, RF Crozier, PS Doerfler, DW Heroux, MA Lin, PT Thornquist, HK Trucano, TG Vaughan, CT AF Barrett, R. F. Crozier, P. S. Doerfler, D. W. Heroux, M. A. Lin, P. T. Thornquist, H. K. Trucano, T. G. Vaughan, C. T. TI Assessing the role of mini-applications in predicting key performance characteristics of scientific and engineering applications SO JOURNAL OF PARALLEL AND DISTRIBUTED COMPUTING LA English DT Article DE High performance computing; Validation; Scientific computing AB Computational science and engineering application programs are typically large, complex, and dynamic, and are often constrained by distribution limitations. As a means of making tractable rapid explorations of scientific and engineering application programs in the context of new, emerging, and future computing architectures, a suite of "miniapps" has been created to serve as proxies for full scale applications. Each miniapp is designed to represent a key performance characteristic that does or is expected to significantly impact the runtime performance of an application program. In this paper we introduce a methodology for assessing the ability of these miniapps to effectively represent these.performance issues. We applied this methodology to three miniapps, examining the linkage between them and an application they are intended to represent. Herein we evaluate the fidelity of that linkage. This work represents the initial steps required to begin to answer the question, "Under what conditions does a miniapp represent a key performance characteristic in a full app?" (C) 2014 Elsevier Inc. All rights reserved. C1 [Barrett, R. F.; Crozier, P. S.; Doerfler, D. W.; Heroux, M. A.; Lin, P. T.; Thornquist, H. K.; Trucano, T. G.; Vaughan, C. T.] Sandia Natl Labs, Ctr Res Comp, Albuquerque, NM 87185 USA. RP Barrett, RF (reprint author), Sandia Natl Labs, Ctr Res Comp, POB 5800, Albuquerque, NM 87185 USA. EM rfbarre@sandia.gov OI Heroux, Michael/0000-0002-5893-0273 FU Advanced Simulation and Computing (ASC) program - US Department of Energy's National Nuclear Security Agency; US Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX Support for this work was provided through the Advanced Simulation and Computing (ASC) program funded by US Department of Energy's National Nuclear Security Agency. This effort was greatly enhanced by interactions with staff throughout Sandia as well as many external organizations. It is heartening to discover the active interests in this work, supported by broad and deep expertise, of the computational science community.; Sandia National Laboratories is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the US Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000. NR 34 TC 2 Z9 2 U1 0 U2 4 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 0743-7315 EI 1096-0848 J9 J PARALLEL DISTR COM JI J. Parallel Distrib. Comput. PD JAN PY 2015 VL 75 BP 107 EP 122 DI 10.1016/j.jpdc.2014.09.006 PG 16 WC Computer Science, Theory & Methods SC Computer Science GA AW9BK UT WOS:000346552500010 ER PT J AU Aartsen, MG Abbasi, R Ackermann, M Adams, J Aguilar, JA Ahlers, M Altmann, D Arguelles, C Auffenberg, J Bai, X Baker, M Barwick, SW Baum, V Bay, R Beatty, JJ Tjus, JB Becker, KH BenZvi, S Berghaus, P Berley, D Bernardini, E Bernhard, A Besson, DZ Binder, G Bindig, D Bissok, M Blaufuss, E Blumenthal, J Boersma, DJ Bohm, C Bose, D Boser, S Botner, O Brayeur, L Bretz, HP Brown, AM Bruijn, R Casey, J Casier, M Chirkin, D Christov, A Christy, B Clark, K Classen, L Clevermann, F Coenders, S Cohen, S Cowen, DF Silva, AHC Danninger, M Daughhetee, J Davis, JC Day, M De Clercq, C De Ridder, S Desiati, P de Vries, KD de With, M DeYoung, T Diaz-Velez, JC Dunkman, M Eagan, R Eberhardt, B Eichmann, B Eisch, J Euler, S Evenson, PA Fadiran, O Fazely, AR Fedynitch, A Feintzeig, J Feusels, T Filimonov, K Finley, C Fischer-Wasels, T Flis, S Franckowiak, A Frantzen, K Fuchs, T Gaisser, TK Gallagher, J Gerhardt, L Gladstone, L Glusenkamp, T Goldschmidt, A Golup, G Gonzalez, JG Goodman, JA Gora, D Grandmont, DT Grant, D Gretskov, P Groh, JC Gross, A Ha, C Ismail, AH Hallen, P Hallgren, A Halzen, F Hanson, K Hebecker, D Heereman, D Heinen, D Helbing, K Hellauer, R Hickford, S Hill, GC Hoffman, KD Hoffmann, R Homeier, A Hoshina, K Huang, F Huelsnitz, W Hulth, PO Hultqvist, K Hussain, S Ishihara, A Jacobi, E Jacobsen, J Jagielski, K Japaridze, GS Jero, K Jlelati, O Kaminsky, B Kappes, A Karg, T Karle, A Kauer, M Kelley, JL Kiryluk, J Klas, J Klein, SR Kohne, JH Kohnen, G Kolanoski, H Kopke, L Kopper, C Kopper, S Koskinen, DJ Kowalski, M Krasberg, M Kriesten, A Krings, K Kroll, G Kunnen, J Kurahashi, N Kuwabara, T Labare, M Landsman, H Larson, MJ Lesiak-Bzdak, M Leuermann, M Leute, J Lunemann, J Macias, O Madsen, J Maggi, G Maruyama, R Mase, K Matis, HS McNally, F Meagher, K Merck, M Merino, G Meures, T Miarecki, S Middell, E Milke, N Miller, J Mohrmann, L Montaruli, T Morse, R Nahnhauer, R Naumann, U Niederhausen, H Nowicki, SC Nygren, DR Obertacke, A Odrowski, S Olivas, A Omairat, A O'Murchadha, A Paul, L Pepper, JA de los Heros, CP Pfendner, C Pieloth, D Pinat, E Posselt, J Price, PB Przybylski, GT Quinnan, M Radel, L Rae, I Rameez, M Rawlins, K Redl, P Reimann, R Resconi, E Rhode, W Ribordy, M Richman, M Riedel, B Rodrigues, JP Rott, C Ruhe, T Ruzybayev, B Ryckbosch, D Saba, SM Sander, HG Santander, M Sarkar, S Schatto, K Scheriau, F Schmidt, T Schmitz, M Schoenen, S Schoneberg, S Schonwald, A Schukraft, A Schulte, L Schultz, D Schulz, O Secke, D Sestayo, Y Seunarine, S Shanidze, R Sheremata, C Smith, MWE Soldin, D Spiczak, GM Spiering, C Stamatikos, M Stanev, T Stanisha, NA Stasik, A Stezelberger, T Stokstad, RG Stossl, A Strahler, EA Strom, R Strotjohann, NL Sullivan, GW Taavola, H Taboada, I Tamburro, A Tepe, A Ter-Antonyan, S Tesic, G Tilav, S Toale, PA Tobin, MN Toscano, S Tselengidou, M Unger, E Usner, M Vallecorsa, S van Eijndhoven, N van Overloop, A van Santen, J Vehring, M Voge, M Vraeghe, M Walck, C Waldenmaier, T Wallraff, M Weaver, C Wellons, M Wendt, C Westerhoff, S Whitehorn, N Wiebe, K Wiebusch, CH Williams, DR Wissing, H Wolf, M Wood, TR Woschnagg, K Xu, DL Xu, XW Yanez, JP Yodh, G Yoshida, S Zarzhitsky, P Ziemann, J Zierke, S Zoll, M AF Aartsen, M. G. Abbasi, R. Ackermann, M. Adams, J. Aguilar, J. A. Ahlers, M. Altmann, D. Arguelles, C. Auffenberg, J. Bai, X. Baker, M. Barwick, S. W. Baum, V. Bay, R. Beatty, J. J. Tjus, J. Becker Becker, K. -H. BenZvi, S. Berghaus, P. Berley, D. Bernardini, E. Bernhard, A. Besson, D. Z. Binder, G. Bindig, D. Bissok, M. Blaufuss, E. Blumenthal, J. Boersma, D. J. Bohm, C. Bose, D. Boeser, S. Botner, O. Brayeur, L. Bretz, H. -P. Brown, A. M. Bruijn, R. Casey, J. Casier, M. Chirkin, D. Christov, A. Christy, B. Clark, K. Classen, L. Clevermann, F. Coenders, S. Cohen, S. Cowen, D. F. Silva, A. H. Cruz Danninger, M. Daughhetee, J. Davis, J. C. Day, M. De Clercq, C. De Ridder, S. Desiati, P. de Vries, K. D. de With, M. DeYoung, T. Diaz-Velez, J. C. Dunkman, M. Eagan, R. Eberhardt, B. Eichmann, B. Eisch, J. Euler, S. Evenson, P. A. Fadiran, O. Fazely, A. R. Fedynitch, A. Feintzeig, J. Feusels, T. Filimonov, K. Finley, C. Fischer-Wasels, T. Flis, S. Franckowiak, A. Frantzen, K. Fuchs, T. Gaisser, T. K. Gallagher, J. Gerhardt, L. Gladstone, L. Glusenkamp, T. Goldschmidt, A. Golup, G. Gonzalez, J. G. Goodman, J. A. Gora, D. Grandmont, D. T. Grant, D. Gretskov, P. Groh, J. C. Gross, A. Ha, C. Ismail, A. Haj Hallen, P. Hallgren, A. Halzen, F. Hanson, K. Hebecker, D. Heereman, D. Heinen, D. Helbing, K. Hellauer, R. Hickford, S. Hill, G. C. Hoffman, K. D. Hoffmann, R. Homeier, A. Hoshina, K. Huang, F. Huelsnitz, W. Hulth, P. O. Hultqvist, K. Hussain, S. Ishihara, A. Jacobi, E. Jacobsen, J. Jagielski, K. Japaridze, G. S. Jero, K. Jlelati, O. Kaminsky, B. Kappes, A. Karg, T. Karle, A. Kauer, M. Kelley, J. L. Kiryluk, J. Klaes, J. Klein, S. R. Koehne, J. -H. Kohnen, G. Kolanoski, H. Koepke, L. Kopper, C. Kopper, S. Koskinen, D. J. Kowalski, M. Krasberg, M. Kriesten, A. Krings, K. Kroll, G. Kunnen, J. Kurahashi, N. Kuwabara, T. Labare, M. Landsman, H. Larson, M. J. Lesiak-Bzdak, M. Leuermann, M. Leute, J. Luenemann, J. Macias, O. Madsen, J. Maggi, G. Maruyama, R. Mase, K. Matis, H. S. McNally, F. Meagher, K. Merck, M. Merino, G. Meures, T. Miarecki, S. Middell, E. Milke, N. Miller, J. Mohrmann, L. Montaruli, T. Morse, R. Nahnhauer, R. Naumann, U. Niederhausen, H. Nowicki, S. C. Nygren, D. R. Obertacke, A. Odrowski, S. Olivas, A. Omairat, A. O'Murchadha, A. Paul, L. Pepper, J. A. de los Heros, C. Perez Pfendner, C. Pieloth, D. Pinat, E. Posselt, J. Price, P. B. Przybylski, G. T. Quinnan, M. Raedel, L. Rae, I. Rameez, M. Rawlins, K. Redl, P. Reimann, R. Resconi, E. Rhode, W. Ribordy, M. Richman, M. Riedel, B. Rodrigues, J. P. Rott, C. Ruhe, T. Ruzybayev, B. Ryckbosch, D. Saba, S. M. Sander, H. -G. Santander, M. Sarkar, S. Schatto, K. Scheriau, F. Schmidt, T. Schmitz, M. Schoenen, S. Schoeneberg, S. Schoenwald, A. Schukraft, A. Schulte, L. Schultz, D. Schulz, O. Secke, D. Sestayo, Y. Seunarine, S. Shanidze, R. Sheremata, C. Smith, M. W. E. Soldin, D. Spiczak, G. M. Spiering, C. Stamatikos, M. Stanev, T. Stanisha, N. A. Stasik, A. Stezelberger, T. Stokstad, R. G. Stoessl, A. Strahler, E. A. Stroem, R. Strotjohann, N. L. Sullivan, G. W. Taavola, H. Taboada, I. Tamburro, A. Tepe, A. Ter-Antonyan, S. Tesic, G. Tilav, S. Toale, P. A. Tobin, M. N. Toscano, S. Tselengidou, M. Unger, E. Usner, M. Vallecorsa, S. van Eijndhoven, N. van Overloop, A. van Santen, J. Vehring, M. Voge, M. Vraeghe, M. Walck, C. Waldenmaier, T. Wallraff, M. Weaver, Ch. Wellons, M. Wendt, C. Westerhoff, S. Whitehorn, N. Wiebe, K. Wiebusch, C. H. Williams, D. R. Wissing, H. Wolf, M. Wood, T. R. Woschnagg, K. Xu, D. L. Xu, X. W. Yanez, J. P. Yodh, G. Yoshida, S. Zarzhitsky, P. Ziemann, J. Zierke, S. Zoll, M. TI The IceProd framework: Distributed data processing for the IceCube neutrino observatory SO JOURNAL OF PARALLEL AND DISTRIBUTED COMPUTING LA English DT Article DE Data management; Grid computing; Monitoring; Distributed computing AB IceCube is a one-gigaton instrument located at the geographic South Pole, designed to detect cosmic neutrinos, identify the particle nature of dark matter, and study high-energy neutrinos themselves. Simulation of the IceCube detector and processing of data require a significant amount of computational resources. This paper presents the first detailed description of IceProd, a lightweight distributed management system designed to meet these requirements. It is driven by a central database in order to manage mass production of simulations and analysis of data produced by the IceCube detector. IceProd runs as a separate layer on top of other middleware and can take advantage of a variety of computing resources, including grids and batch systems such as CREAM, HTCondor, and PBS. This is accomplished by a set of dedicated daemons that process job submission in a coordinated fashion through the use of middleware plugins that serve to abstract the details of job submission and job management from the framework. (C) 2014 Elsevier Inc. All rights reserved. C1 [Bissok, M.; Blumenthal, J.; Coenders, S.; Euler, S.; Gretskov, P.; Hallen, P.; Heinen, D.; Jagielski, K.; Kriesten, A.; Krings, K.; Leuermann, M.; Paul, L.; Raedel, L.; Reimann, R.; Schoenen, S.; Schukraft, A.; Vehring, M.; Wallraff, M.; Wiebusch, C. H.; Zierke, S.] Rhein Westfal TH Aachen, Inst Phys 3, D-52056 Aachen, Germany. [Aartsen, M. G.; Hill, G. C.] Univ Adelaide, Sch Chem & Phys, Adelaide, SA 5005, Australia. [Rawlins, K.] Univ Alaska Anchorage, Dept Phys & Astron, Anchorage, AK 99508 USA. [Japaridze, G. S.] Clark Atlanta Univ, CTSPS, Atlanta, GA 30314 USA. [Bruijn, R.; Casey, J.; Daughhetee, J.; Taboada, I.] Georgia Inst Technol, Sch Phys, Atlanta, GA 30332 USA. [Bruijn, R.; Casey, J.; Daughhetee, J.; Taboada, I.] Georgia Inst Technol, Ctr Relativist Astrophys, Atlanta, GA 30332 USA. [Fazely, A. R.; Ter-Antonyan, S.; Xu, X. W.] Southern Univ, Dept Phys, Baton Rouge, LA 70813 USA. [Bay, R.; Binder, G.; Filimonov, K.; Gerhardt, L.; Ha, C.; Klein, S. R.; Miarecki, S.; Price, P. B.; Woschnagg, K.] Univ Calif Berkeley, Dept Phys, Berkeley, CA 94720 USA. [Binder, G.; Gerhardt, L.; Goldschmidt, A.; Ha, C.; Klein, S. R.; Matis, H. S.; Miarecki, S.; Nygren, D. R.; Przybylski, G. T.; Stezelberger, T.; Stokstad, R. G.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [de With, M.; Kolanoski, H.; Waldenmaier, T.] Humboldt Univ, Inst Phys, D-12489 Berlin, Germany. [Tjus, J. Becker; Eichmann, B.; Fedynitch, A.; Saba, S. M.; Schoeneberg, S.; Unger, E.] Ruhr Univ Bochum, Fak Phys & Astron, D-44780 Bochum, Germany. [Boeser, S.; Franckowiak, A.; Hebecker, D.; Homeier, A.; Kowalski, M.; Schulte, L.; Stasik, A.; Strotjohann, N. L.; Usner, M.; Voge, M.] Univ Bonn, Inst Phys, D-53115 Bonn, Germany. [Hanson, K.; Heereman, D.; Meures, T.; O'Murchadha, A.; Pinat, E.] Univ Libre Bruxelles, Sci Fac CP230, B-1050 Brussels, Belgium. [Brayeur, L.; Casier, M.; De Clercq, C.; de Vries, K. D.; Golup, G.; Kunnen, J.; Maggi, G.; Miller, J.; Strahler, E. A.; van Eijndhoven, N.] Vrije Univ Brussel, Dienst ELEM, B-1050 Brussels, Belgium. [Ishihara, A.; Mase, K.; Yoshida, S.] Chiba Univ, Dept Phys, Chiba 260, Japan. [Adams, J.; Hickford, S.; Macias, O.] Univ Canterbury, Dept Phys & Astron, Christchurch 1, New Zealand. [Brayeur, L.; Casier, M.; De Clercq, C.; de Vries, K. D.; Golup, G.; Kunnen, J.; Maggi, G.; Miller, J.; Olivas, A.; Strahler, E. A.; van Eijndhoven, N.] Univ Maryland, Dept Phys, College Pk, MD 20742 USA. [Beatty, J. J.; Davis, J. C.; Pfendner, C.; Stamatikos, M.] Ohio State Univ, Dept Phys, Columbus, OH 43210 USA. [Beatty, J. J.; Davis, J. C.; Pfendner, C.; Stamatikos, M.] Ohio State Univ, Ctr Cosmol & Astroparticle Phys, Columbus, OH 43210 USA. [Beatty, J. J.] Ohio State Univ, Dept Astron, Columbus, OH 43210 USA. [Sarkar, S.] Univ Copenhagen, Niels Bohr Inst, DK-2100 Copenhagen, Denmark. [Clevermann, F.; Frantzen, K.; Fuchs, T.; Koehne, J. -H.; Milke, N.; Pieloth, D.; Rhode, W.; Ruhe, T.; Scheriau, F.; Schmitz, M.; Ziemann, J.] TU Dortmund Univ, Dept Phys, D-44221 Dortmund, Germany. [Grandmont, D. T.; Grant, D.; Nowicki, S. C.; Odrowski, S.; Sheremata, C.; Wood, T. R.] Univ Alberta, Dept Phys, Edmonton, AB T6G 2E1, Canada. [Altmann, D.; Classen, L.; Gora, D.; Kappes, A.; Tselengidou, M.] Univ Erlangen Nurnberg, Erlangen Ctr Astroparticle Phys, D-91058 Erlangen, Germany. [Aguilar, J. A.; Christov, A.; Montaruli, T.; Rameez, M.; Vallecorsa, S.] Univ Geneva, Dept Phys Nucl & Corpusculaire, CH-1211 Geneva, Switzerland. [De Ridder, S.; Feusels, T.; Ismail, A. Haj; Jlelati, O.; Labare, M.; Ryckbosch, D.; van Overloop, A.; Vraeghe, M.] Univ Ghent, Dept Phys & Astron, B-9000 Ghent, Belgium. [Barwick, S. W.; Yodh, G.] Univ Calif Irvine, Dept Phys & Astron, Irvine, CA 92697 USA. [Brown, A. M.; Cohen, S.; Ribordy, M.] Ecole Polytech Fed Lausanne, Lab High Energy Phys, CH-1015 Lausanne, Switzerland. [Besson, D. Z.] Univ Kansas, Dept Phys & Astron, Lawrence, KS 66045 USA. [Gallagher, J.] Univ Wisconsin, Dept Astron, Madison, WI 53706 USA. [Abbasi, R.; Ahlers, M.; Arguelles, C.; Auffenberg, J.; Baker, M.; BenZvi, S.; Chirkin, D.; Day, M.; Desiati, P.; Diaz-Velez, J. C.; Eisch, J.; Fadiran, O.; Feintzeig, J.; Gladstone, L.; Halzen, F.; Hoshina, K.; Jacobsen, J.; Jero, K.; Karle, A.; Kauer, M.; Kelley, J. L.; Kopper, C.; Krasberg, M.; Kurahashi, N.; Landsman, H.; Maruyama, R.; McNally, F.; Merck, M.; Merino, G.; Morse, R.; Riedel, B.; Rodrigues, J. P.; Santander, M.; Schultz, D.; Tobin, M. N.; Toscano, S.; van Santen, J.; Weaver, Ch.; Wellons, M.; Wendt, C.; Westerhoff, S.; Whitehorn, N.] Univ Wisconsin, Dept Phys, Madison, WI 53706 USA. [Abbasi, R.; Ahlers, M.; Arguelles, C.; Auffenberg, J.; Baker, M.; BenZvi, S.; Chirkin, D.; Day, M.; Desiati, P.; Diaz-Velez, J. C.; Eisch, J.; Fadiran, O.; Feintzeig, J.; Gladstone, L.; Halzen, F.; Hoshina, K.; Jacobsen, J.; Jero, K.; Karle, A.; Kauer, M.; Kelley, J. L.; Kopper, C.; Krasberg, M.; Kurahashi, N.; Landsman, H.; Maruyama, R.; McNally, F.; Merck, M.; Merino, G.; Morse, R.; Riedel, B.; Rodrigues, J. P.; Santander, M.; Schultz, D.; Tobin, M. N.; Toscano, S.; van Santen, J.; Weaver, Ch.; Wellons, M.; Wendt, C.; Westerhoff, S.; Whitehorn, N.] Univ Wisconsin, Wisconsin IceCube Particle Astrophys Ctr, Madison, WI 53706 USA. [Rae, I.] Univ Wisconsin, Dept Comp Sci, Madison, WI 53706 USA. [Baum, V.; Eberhardt, B.; Koepke, L.; Kroll, G.; Luenemann, J.; Sander, H. -G.; Schatto, K.; Wiebe, K.] Johannes Gutenberg Univ Mainz, Inst Phys, D-55099 Mainz, Germany. [Kohnen, G.] Univ Mons, B-7000 Mons, Belgium. [Bernhard, A.; Gross, A.; Leute, J.; Resconi, E.; Schulz, O.; Sestayo, Y.] Tech Univ Munich, D-85748 Garching, Germany. [Bai, X.; Evenson, P. A.; Gaisser, T. K.; Gonzalez, J. G.; Hussain, S.; Kuwabara, T.; Ruzybayev, B.; Secke, D.; Stanev, T.; Tamburro, A.; Tilav, S.] Univ Delaware, Bartol Res Inst, Newark, DE 19716 USA. [Bai, X.; Evenson, P. A.; Gaisser, T. K.; Gonzalez, J. G.; Hussain, S.; Kuwabara, T.; Ruzybayev, B.; Secke, D.; Stanev, T.; Tamburro, A.; Tilav, S.] Univ Delaware, Dept Phys & Astron, Newark, DE 19716 USA. [Sarkar, S.] Univ Oxford, Dept Phys, Oxford OX1 3NP, England. [Bernhard, A.; Madsen, J.; Seunarine, S.; Spiczak, G. M.] Univ Wisconsin, Dept Phys, River Falls, WI 54022 USA. [Bohm, C.; Danninger, M.; Finley, C.; Flis, S.; Hulth, P. O.; Hultqvist, K.; Walck, C.; Wolf, M.; Zoll, M.] Stockholm Univ, Oskar Klein Ctr, SE-10691 Stockholm, Sweden. [Bohm, C.; Danninger, M.; Finley, C.; Flis, S.; Hulth, P. O.; Hultqvist, K.; Walck, C.; Wolf, M.; Zoll, M.] Stockholm Univ, Dept Phys, SE-10691 Stockholm, Sweden. [Kiryluk, J.; Lesiak-Bzdak, M.; Niederhausen, H.] SUNY Stony Brook, Dept Phys & Astron, Stony Brook, NY 11794 USA. [Bose, D.; Rott, C.] Sungkyunkwan Univ, Dept Phys, Suwon 440746, South Korea. [Clark, K.] Univ Toronto, Dept Phys, Toronto, ON M5S 1A7, Canada. [Larson, M. J.; Pepper, J. A.; Toale, P. A.; Williams, D. R.; Xu, D. L.; Zarzhitsky, P.] Univ Alabama, Dept Phys & Astron, Tuscaloosa, AL 35487 USA. [Cowen, D. F.] Penn State Univ, Dept Astron & Astrophys, University Pk, PA 16802 USA. [Cowen, D. F.; DeYoung, T.; Dunkman, M.; Eagan, R.; Groh, J. C.; Huang, F.; Quinnan, M.; Smith, M. W. E.; Stanisha, N. A.; Tesic, G.] Penn State Univ, Dept Phys, University Pk, PA 16802 USA. [Boersma, D. J.; Botner, O.; Hallgren, A.; de los Heros, C. Perez; Stroem, R.; Taavola, H.] Uppsala Univ, Dept Phys & Astron, S-75120 Uppsala, Sweden. [Becker, K. -H.; Bindig, D.; Fischer-Wasels, T.; Helbing, K.; Hoffmann, R.; Klaes, J.; Kopper, S.; Naumann, U.; Obertacke, A.; Omairat, A.; Posselt, J.; Soldin, D.; Tepe, A.] Univ Wuppertal, Dept Phys, D-42119 Wuppertal, Germany. [Ackermann, M.; Berghaus, P.; Bernardini, E.; Bretz, H. -P.; Silva, A. H. Cruz; Glusenkamp, T.; Jacobi, E.; Kaminsky, B.; Karg, T.; Middell, E.; Mohrmann, L.; Nahnhauer, R.; Schoenwald, A.; Shanidze, R.; Spiering, C.; Stoessl, A.; Yanez, J. P.] DESY, D-15735 Zeuthen, Germany. RP Desiati, P (reprint author), Univ Wisconsin, Dept Phys, Madison, WI 53706 USA. EM desiati@icecube.wisc.edu; juancarlos@wipac.wisc.edu; ofadiran@icecube.wisc.edu; ian@cs.wisc.edu; dschultz@icecube.wisc.edu RI Auffenberg, Jan/D-3954-2014; Maruyama, Reina/A-1064-2013; Wiebusch, Christopher/G-6490-2012; Taavola, Henric/B-4497-2011; Koskinen, David/G-3236-2014; Aguilar Sanchez, Juan Antonio/H-4467-2015; Tjus, Julia/G-8145-2012; Beatty, James/D-9310-2011; Sarkar, Subir/G-5978-2011 OI Auffenberg, Jan/0000-0002-1185-9094; Maruyama, Reina/0000-0003-2794-512X; Wiebusch, Christopher/0000-0002-6418-3008; Taavola, Henric/0000-0002-2604-2810; Merino, Gonzalo/0000-0002-9540-5742; Arguelles Delgado, Carlos/0000-0003-4186-4182; Koskinen, David/0000-0002-0514-5917; Aguilar Sanchez, Juan Antonio/0000-0003-2252-9514; Beatty, James/0000-0003-0481-4952; Sarkar, Subir/0000-0002-3542-858X FU U.S. National Science Foundation-Office of Polar Programs; U.S. National Science Foundation-Physics Division; University of Wisconsin Alumni Research Foundation; Grid Laboratory Of Wisconsin (GLOW) grid infrastructure at the University of Wisconsin Madison; Open Science Grid (OSG) grid infrastructure; U.S. Department of Energy, and National Energy Research Scientific Computing Center; Louisiana Optical Network Initiative (LONI) grid computing resources; Natural Sciences and Engineering Research Council of Canada; WestGrid and Compute/Calcul Canada; Swedish Research Council; Swedish Polar Research Secretariat; Swedish National Infrastructure for Computing (SNIC); Knut and Alice Wallenberg Foundation, Sweden; German Ministry for Education and Research (BMBF); Deutsche Forschungsgemeinschaft (DFG); Helmholtz Alliance for Astroparticle Physics (HAP); Research Department of Plasmas with Complex Interactions (Bochum), Germany; Fund for Scientific Research (FNRS-FWO); FWO Odysseus programme; Flanders Institute to encourage scientific and technological research in industry (IWT); Belgian Federal Science Policy Office (Belspo); University of Oxford, United Kingdom; Marsden Fund, New Zealand; Australian Research Council; Japan Society for Promotion of Science (JSPS); Swiss National Science Foundation (SNSF), Switzerland; National Research Foundation of Korea (NRF); Danish National Research Foundation, Denmark (DNRF) FX We acknowledge the support from the following agencies: U.S. National Science Foundation-Office of Polar Programs, U.S. National Science Foundation-Physics Division, University of Wisconsin Alumni Research Foundation, the Grid Laboratory Of Wisconsin (GLOW) grid infrastructure at the University of Wisconsin Madison, the Open Science Grid (OSG) grid infrastructure; U.S. Department of Energy, and National Energy Research Scientific Computing Center, the Louisiana Optical Network Initiative (LONI) grid computing resources; Natural Sciences and Engineering Research Council of Canada, WestGrid and Compute/Calcul Canada; Swedish Research Council, Swedish Polar Research Secretariat, Swedish National Infrastructure for Computing (SNIC), and Knut and Alice Wallenberg Foundation, Sweden; German Ministry for Education and Research (BMBF), Deutsche Forschungsgemeinschaft (DFG), Helmholtz Alliance for Astroparticle Physics (HAP), Research Department of Plasmas with Complex Interactions (Bochum), Germany; Fund for Scientific Research (FNRS-FWO), FWO Odysseus programme, Flanders Institute to encourage scientific and technological research in industry (IWT), Belgian Federal Science Policy Office (Belspo); University of Oxford, United Kingdom; Marsden Fund, New Zealand; Australian Research Council; Japan Society for Promotion of Science (JSPS); the Swiss National Science Foundation (SNSF), Switzerland; National Research Foundation of Korea (NRF); Danish National Research Foundation, Denmark (DNRF). NR 18 TC 2 Z9 2 U1 0 U2 11 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 0743-7315 EI 1096-0848 J9 J PARALLEL DISTR COM JI J. Parallel Distrib. Comput. PD JAN PY 2015 VL 75 BP 198 EP 211 DI 10.1016/j.jpdc.2014.08.001 PG 14 WC Computer Science, Theory & Methods SC Computer Science GA AW9BK UT WOS:000346552500017 ER PT J AU Razzaghi, H Oster, M Reefhuis, J AF Razzaghi, Hilda Oster, Matthew Reefhuis, Jennita TI Long-Term Outcomes in Children with Congenital Heart Disease: National Health Interview Survey SO JOURNAL OF PEDIATRICS LA English DT Article ID QUALITY-OF-LIFE; NEURODEVELOPMENTAL OUTCOMES; SPECTRUM DISORDERS; FOLLOW-UP; SURGERY; DEFECTS; ADULTS; CARE; POPULATION; REPAIR AB Objective To assess the extent of long-term morbidity in children with congenital heart disease (CHD). Study design We used data from the 1997-2011 National Health Interview Survey to study long-term outcomes in children aged 0-17 years with CHD. Parents were asked whether their child was diagnosed with CHD. We assessed for comorbidities, including autism/autism spectrum disorders; healthcare utilization, including number of emergency room visits; and daily life aspects, including number of days of school missed. These outcomes were compared between children with and without reported CHD using ORs and chi(2) statistics. Results The study included 420 children with reported CHD and 180 048 children without CHD, with no significant between-group differences in age and sex. The odds of reporting worse health and more than 10 days of school/daycare missed in the previous year were 3 times higher for the children with CHD compared with those without CHD. Children aged 2-17 with CHD were more likely than those without CHD to have had a diagnosis of autism spectrum disorder (crude OR, 4.6; 95% CI, 1.9-11.0) or intellectual disability (crude OR, 9.1; 95% CI, 5.4-15.4). The rates of emergency room, home, and doctors' office visits were significantly higher in the children with CHD. Conclusion Reported adverse outcomes were more prevalent in the children with CHD. Our findings, particularly those regarding neurodevelopmental outcomes, may be helpful for parents, healthcare providers, and others in assessing the specific needs of children and teenagers with CHD. C1 [Razzaghi, Hilda; Oster, Matthew; Reefhuis, Jennita] Ctr Dis Control & Prevent, Natl Ctr Birth Defects & Dev Disabil, Atlanta, GA 30333 USA. [Razzaghi, Hilda] Oak Ridge Inst Sci & Educ, Oak Ridge, TN USA. [Oster, Matthew] Emory Univ, Sch Med, Childrens Healthcare Atlanta, Atlanta, GA USA. RP Razzaghi, H (reprint author), Ctr Dis Control & Prevent, Mail Stop E86,1600 Clifton Rd, Atlanta, GA 30333 USA. EM hir2@cdc.gov FU Research Participation program for the Centers for Disease Control and Prevention FX H.R. was supported by an appointment to the Research Participation program for the Centers for Disease Control and Prevention administered by the Oak Ridge Institute for Science and Education through an agreement between the Department of Energy and Centers for Disease Control and Prevention. The findings and conclusions in this report are those of the authors and do not necessarily represent the official position of Centers for Disease Control and Prevention. The authors declare no conflicts of interest. NR 38 TC 5 Z9 5 U1 2 U2 15 PU MOSBY-ELSEVIER PI NEW YORK PA 360 PARK AVENUE SOUTH, NEW YORK, NY 10010-1710 USA SN 0022-3476 EI 1097-6833 J9 J PEDIATR-US JI J. Pediatr. PD JAN PY 2015 VL 166 IS 1 BP 119 EP + DI 10.1016/j.jpeds.2014.09.006 PG 7 WC Pediatrics SC Pediatrics GA AW9NI UT WOS:000346584000026 PM 25304924 ER PT J AU Azimi, N Xue, Z Rago, ND Takoudis, C Gordin, ML Song, JX Wang, DH Zhang, ZC AF Azimi, Nasim Xue, Zheng Rago, Nancy Dietz Takoudis, Christos Gordin, Mikhail L. Song, Jiangxuan Wang, Donghai Zhang, Zhengcheng TI Fluorinated Electrolytes for Li-S Battery: Suppressing the Self-Discharge with an Electrolyte Containing Fluoroether Solvent SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID LITHIUM-SULFUR BATTERIES; ELECTROCHEMICAL PROPERTIES; LIQUID ELECTROLYTES; POLYSULFIDE SHUTTLE; THERMAL-STABILITY; CATHODE MATERIAL; ION BATTERIES; PERFORMANCE; CAPACITY; MECHANISM AB The fluorinated electrolyte containing a fluoroether 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether (TTE) was investigated as a new electrolyte for lithium-sulfur (Li-S) batteries. The low solubility of lithium polysulfides (LiPS) in the fluorinated electrolyte reduced the parasitic reactions with Li anode and mitigated the self-discharge by limiting their diffusion from the cathode to the anode. The use of fluorinated ether as a co-solvent and LiNO3 as an additive in the electrolyte shows synergetic effect in suppressing the self-discharge of Li-S battery due to the formation of the solid electrolyte interphase (SEI) on both sulfur cathode and the lithium anode. The Li-S cell with the fluorinated electrolyte showed prolonged shelf life at fully charged state. (C) The Author(s) 2014. Published by ECS. This is an open access article distributed under the terms of the Creative Commons Attribution 4.0 License (CC BY, http://creativecommons.org/licenses/by/4.0/), which permits unrestricted reuse of the work in any medium, provided the original work is properly cited. All rights reserved. C1 [Azimi, Nasim; Xue, Zheng; Rago, Nancy Dietz; Zhang, Zhengcheng] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. [Azimi, Nasim; Takoudis, Christos] Univ Illinois, Dept Chem Engn, Chicago, IL 60607 USA. [Azimi, Nasim; Takoudis, Christos] Univ Illinois, Dept Bioengn, Chicago, IL 60607 USA. [Gordin, Mikhail L.; Song, Jiangxuan; Wang, Donghai] Penn State Univ, Dept Mech & Nucl Engn, University Pk, PA 16802 USA. RP Azimi, N (reprint author), Argonne Natl Lab, Chem Sci & Engn Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM zzhang@anl.gov RI Song, Jiangxuan/G-8536-2015; Wang, Donghai/L-1150-2013 OI Wang, Donghai/0000-0001-7261-8510 FU Vehicle Technologies Office, U.S. Department of Energy, Argonne, a U.S. Department of Energy laboratory [DE-AC02-06CH11357] FX This research is supported by the Vehicle Technologies Office, U.S. Department of Energy, Argonne, a U.S. Department of Energy laboratory, is operated by UChicago Argonne, LLC under contract DE-AC02-06CH11357. Z.Z. thank Dr. Shengshui Zhang from US Army Research Laboratory for the technical discussions. NR 29 TC 18 Z9 18 U1 10 U2 113 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 EI 1945-7111 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2015 VL 162 IS 1 BP A64 EP A68 DI 10.1149/2.0431501jes PG 5 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA AW0JZ UT WOS:000345979700030 ER PT J AU Dogan, F Croy, JR Balasubramanian, M Slater, MD Iddir, H Johnson, CS Vaughey, JT Key, B AF Dogan, Fulya Croy, Jason R. Balasubramanian, Mahalingam Slater, Michael D. Iddir, Hakim Johnson, Christopher S. Vaughey, John T. Key, Baris TI Solid State NMR Studies of Li2MnO3 and Li-Rich Cathode Materials: Proton Insertion, Local Structure, and Voltage Fade SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID X-RAY-ABSORPTION; PAIR DISTRIBUTION FUNCTION; ELECTROCHEMICAL ACTIVITY; CHEMICAL DELITHIATION; LITHIUM INTERCALATION; ELECTRODE MATERIAL; BATTERY CATHODE; OXIDE CATHODES; ION BATTERIES; DIFFRACTION AB High energy densities of lithium-rich transition metal oxides cannot be sufficiently maintained on cycling due to high-voltage first-cycle activation and the subsequent structural changes. These changes can be seen as a continuous decrease of the average voltage with cycling, known as voltage fade. Electrochemical and chemical insertion of protons has been reported suggesting that protons generated in the electrolyte could be involved in electrochemical cycling which could play a similar role in the "Li2MnO3 component" of lithium rich transition metal oxides. Here, electrochemical insertion of structural protons, changes in lithium occupancy at various states of charge, and changes in local structure have been investigated via a combination of local probes including solid state NMR, X-ray absorption spectroscopy and first principle calculations. While significant evidence is found for the deposition of non-structural proton-bearing species on electrodes, which accumulate with extensive cycling, structural proton insertion is not found to be a significant process directly effecting voltage fade. The electrochemical activity of disordered Li2MnO3, synthesized at low temperature, is also investigated and its Li removal/insertion properties measured quantitatively with NMR. Major reordering of Li sites and subsequent local structural transitions are observed by NMR and are found to be synchronous with voltage fade. (C) 2014 The Electrochemical Society. All rights reserved. C1 [Dogan, Fulya; Croy, Jason R.; Slater, Michael D.; Johnson, Christopher S.; Vaughey, John T.; Key, Baris] Argonne Natl Lab, Electrochem Energy Storage Dept, Chem Sci & Engn Div, Argonne, IL 60439 USA. [Balasubramanian, Mahalingam] Argonne Natl Lab, Xray Sci Div, Adv Photon Source, Argonne, IL 60439 USA. [Iddir, Hakim] Argonne Natl Lab, Mat Sci Div, Argonne, IL 60439 USA. RP Dogan, F (reprint author), Argonne Natl Lab, Electrochem Energy Storage Dept, Chem Sci & Engn Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM bkey@anl.gov FU U.S. Department of Energy's Vehicle Technologies Program; U.S. DOE, Basic Energy Sciences; National Sciences and Engineering Research Council of Canada; U.S. Department of Energy Office of Science laboratory [DE-AC02-06CH11357]; U.S. Government FX Support from the U.S. Department of Energy's Vehicle Technologies Program, specifically from Peter Faguy, Tien Duong and David Howell, is gratefully acknowledged. We also acknowledge valuable feedback from Kevin Gallagher and many useful discussions within the Argonne Voltage Fade Team (A. Abouimrane, I. Belharouak, R. Benedek, T. Burrell, Z. Chen, D. Dees, B. Ingram, E. Lee, B. Long, D. Miller, M. Thackeray, L. Trahey) and Yang Ren for synchrotron XRD support at the Advanced Photon Source, sector 11-ID-C. Sector 20 facilities at the Advanced Photon Source of Argonne National Laboratory, and research at these facilities, are supported by the U.S. DOE, Basic Energy Sciences, and National Sciences and Engineering Research Council of Canada and its founding institutions. The submitted manuscript has been created by UChicago Argonne, LLC, Operator of Argonne National Laboratory. Argonne, a U.S. Department of Energy Office of Science laboratory, is operated under Contract No. DE-AC02-06CH11357. The U.S. Government retains for itself, and others acting on its behalf, a paid-up non-exclusive, irrevocable worldwide license in said article to reproduce, prepare derivative works, distribute copies to the public, and perform publicly and display publicly, by or on behalf of the Government. NR 37 TC 20 Z9 20 U1 11 U2 156 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 EI 1945-7111 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2015 VL 162 IS 1 BP A235 EP A243 DI 10.1149/2.1041501jes PG 9 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA AW0JZ UT WOS:000345979700022 ER PT J AU Gallaway, JW Menard, M Hertzberg, B Zhong, Z Croft, M Sviridov, LA Turney, DE Banerjee, S Steingart, DA Erdonmez, CK AF Gallaway, Joshua W. Menard, Melissa Hertzberg, Benjamin Zhong, Zhong Croft, Mark Sviridov, Lev A. Turney, Damon E. Banerjee, Sanjoy Steingart, Daniel A. Erdonmez, Can K. TI Hetaerolite Profiles in Alkaline Batteries Measured by High Energy EDXRD SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID MANGANESE-DIOXIDE ELECTRODE; X-RAY-DIFFRACTION; ZINC CELLS; ELECTROCHEMICAL REDUCTION; CATHODIC REDUCTION; DISCHARGE PROCESS; REDOX PROCESSES; MNO2; GAMMA-MNO2; MECHANISM AB Energy dispersive X-ray diffraction (EDXRD) with photons of high energy and high flux is used to map crystalline discharge products within alkaline AA cells following discharge at various rates: C/160, C/80, C/40, C/20, C/10, and C/5. During the study, the sealed cells are never opened and thus never exposed to air. The technique's resolution allows the various manganese oxide discharge products to be distinguished, which has previously proven difficult. In particular, colocalized Mn3O4 (hausmannite) and ZnMn2O4 (hetaerolite) phases are resolved at C/160, C/80, and C/40 rates. Following more rapid discharge at C/20, no hausmannite is observed: instead, two well-defined zones result, one consisting only of hetaerolite, and the other only of alpha-MnOOH (groutite), with a small transition region where both phases are detected. Modeling suggests the observed hetaerolite-groutite boundary positions are consistent with hetaerolite formation in regions of greater active material utilization. Radial hetaerolite and hausmannite profiles are calculated and found to be a function of the discharge current, which also determines discharge capacity. Results also show formation of a alpha-MnOOH phase from oxidation states MnO(1.)7 to MnO(1.)53 with relatively little gamma-MnOOH character. (C) 2014 The Electrochemical Society. All rights reserved. C1 [Gallaway, Joshua W.; Sviridov, Lev A.; Turney, Damon E.; Banerjee, Sanjoy] CUNY, Energy Inst, Dept Chem Engn, New York, NY 10031 USA. [Menard, Melissa] Urban Elect Power LLC, New York, NY 10027 USA. [Hertzberg, Benjamin; Steingart, Daniel A.] Princeton Univ, Dept Mech & Aerosp Engn, Princeton, NJ 08544 USA. [Hertzberg, Benjamin; Steingart, Daniel A.] Princeton Univ, Andlinger Ctr Energy & Environm, Princeton, NJ 08544 USA. [Zhong, Zhong; Croft, Mark] Brookhaven Natl Lab, Photon Sci Directorate, Upton, NY 11973 USA. [Croft, Mark] Rutgers State Univ, Dept Phys & Astron, Piscataway, NJ 08854 USA. [Erdonmez, Can K.] Brookhaven Natl Lab, Energy Storage Grp, Upton, NY 11973 USA. RP Gallaway, JW (reprint author), CUNY, Energy Inst, Dept Chem Engn, New York, NY 10031 USA. EM jgallaway@che.ccny.cuny.edu FU Laboratory Directed Research and Development Program of Brookhaven National Laboratory (LDRD-BNL) [DE-AC02-98CH 10866]; U.S. Department of Energy; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-98CH10886] FX The authors thank Hui Zhong for assistance at the beamline and Eric Rus for helpful thoughts while editing the manuscript. This work was supported by the Laboratory Directed Research and Development Program of Brookhaven National Laboratory (LDRD-BNL) Under Contract No. DE-AC02-98CH 10866 with the U.S. Department of Energy. Use of the National Synchrotron Light Source, Brookhaven National Laboratory, was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-98CH10886. NR 57 TC 9 Z9 9 U1 4 U2 18 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 EI 1945-7111 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2015 VL 162 IS 1 BP A162 EP A168 DI 10.1149/2.0811501jes PG 7 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA AW0JZ UT WOS:000345979700009 ER PT J AU Lee, SH DeMayo, RA Takeuchi, KJ Takeuchi, ES Marschilok, AC AF Lee, Shu Han DeMayo, Rachel A. Takeuchi, Kenneth J. Takeuchi, Esther S. Marschilok, Amy C. TI Progress toward Metal-Air Batteries: Mechanistic Investigation of the Effect of Water on the Oxygen Reduction Reaction at Carbon-Conductive Polymer-Silver Composite Air Electrodes SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID SUPEROXIDE ION; ELECTROCHEMICAL REDUCTION; CYCLIC VOLTAMMETRY; APROTIC-SOLVENTS; ANODIC FILMS; ELECTROLYTES; ACETONITRILE; DIOXYGEN; MEDIA; ELECTROREDUCTION AB The oxygen reduction reaction (ORR) at the carbon-conductive polymer-silver (C-cp-Ag) composite electrode in non-aqueous electrolyte with small amounts of added water is the subject of this study. The contributions of the various components of the composite electrode were assessed by employing four electrodes: (1) glassy carbon (C), (2) polypyrrole coated glassy carbon (C-cp), (3) silver disk (Ag), and (4) carbon-polypyrrole-silver composite (C-cp-Ag). Notably, with 5000 ppm of water in non-aqueous solution, the ORR reaction at Ag and C-cp-Ag shows an n = 4 reduction, while ORR at C and C-cp display an n = 1 reduction. The results show that the use of a multilayer C-cp-Ag composite electrode provides the opportunity to achieve the four electron reduction of one O-2 molecule, with a low precious metal (Ag) loading. (C) The Author(s) 2014. Published by ECS. This is an open access article distributed under the terms of the Creative Commons Attribution Non-Commercial No Derivatives 4.0 License (CC BY-NC-ND, http://creativecommons.org/licenses/by-nc-nd/4.0/), which permits non-commercial reuse, distribution, and reproduction in any medium, provided the original work is not changed in any way and is properly cited. For permission for commercial reuse, please email: oa@electrochem.org. All rights reserved. C1 [Lee, Shu Han] SUNY Buffalo, Dept Chem & Biol Engn, Buffalo, NY 14260 USA. [DeMayo, Rachel A.] SUNY Buffalo, Dept Chem, Buffalo, NY 14260 USA. [Takeuchi, Kenneth J.; Takeuchi, Esther S.; Marschilok, Amy C.] SUNY Stony Brook, Dept Chem, Stony Brook, NY 11794 USA. [Takeuchi, Esther S.; Marschilok, Amy C.] SUNY Stony Brook, Dept Mat Sci & Engn, Stony Brook, NY 11794 USA. [Takeuchi, Esther S.] Brookhaven Natl Lab, Upton, NY 11973 USA. RP Lee, SH (reprint author), SUNY Buffalo, Dept Chem & Biol Engn, Buffalo, NY 14260 USA. EM kenneth.takeuchi.1@stonybrook.edu; esther.takeuchi@stonybrook.edu; amy.marschilok@stonybrook.edu FU Air Force Office of Scientific Research [FA9550-09-1-0334]; Department of Energy, Office of Electricity [1275961] FX Studies involving mechanistic interrogation in moderate water (500 ppm) containing hybrid electrolytes were supported by the Air Force Office of Scientific Research under Award No. FA9550-09-1-0334. Studies involving mechanistic interrogation in higher water (5000 ppm) containing hybrid electrolytes were supported by the Department of Energy, Office of Electricity, administered through Sandia National Laboratories, Purchase Order #1275961. NR 41 TC 0 Z9 0 U1 4 U2 44 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 EI 1945-7111 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2015 VL 162 IS 1 BP A69 EP A76 DI 10.1149/2.0351501jes PG 8 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA AW0JZ UT WOS:000345979700031 ER PT J AU Li, Y Bareno, J Bettge, M Abraham, DP AF Li, Yan Bareno, Javier Bettge, Martin Abraham, Daniel P. TI Unexpected Voltage Fade in LMR-NMC Oxides Cycled below the "Activation" Plateau SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID LITHIUM-ION BATTERIES; CATHODE MATERIALS; ELECTRON-MICROSCOPY; LOCAL-STRUCTURE; POSITIVE ELECTRODE; LAYERED OXIDES; NI; PERFORMANCE; CELLS; OXYGEN AB A common feature of lithium-excess layered oxides, nominally of composition xLi(2)MnO(3)center dot(1-x)LiMO2 (M = transition metal) is a high-voltage plateau (similar to 4.5 V vs. Li/Li+) in their capacity-voltage profile during the first delithiation cycle. This plateau is believed to result from activation of the Li2MnO3 component, which makes additional lithium available for electrochemical cycling. However, oxides cycled beyond this activation plateau are known to display voltage fade which is a continuous reduction in their equilibrium potential. In this article we show that these oxides display gradual voltage fade even on electrochemical cycling in voltage ranges well below the activation plateau. The average fade is similar to 0.08 mV-cycle(-1) for Li(1.2)Ni(0.1)5Mn(0.5)5Co(0.1)O(2) vs. Li cells after 20 cycles in the 2-4.1 V range at 55 degrees C; a similar to 54 mV voltage hysteresis, expressed as the difference in average cell voltage between charge and discharge cycles, is also observed. The voltage fade results from a gradual accumulation of local spinel environments in the crystal structure. Some of these spinel sites result from lithium deficiencies during oxide synthesis and are likely to be at the particle surfaces; other sites result from the migration of transition metal atoms in the partially-delithiated LiMO2 component into the lithium planes during electrochemical cycling. The observed rate of voltage fade depends on a combination of factors that includes the phase equilibrium between the layered and spinel components and the kinetics of transition metal migration. (C) The Author(s) 2014. Published by ECS. This is an open access article distributed under the terms of the Creative Commons Attribution 4.0 License (CC BY, http://creativecommons.org/licenses/by/4.0/), which permits unrestricted reuse of the work in any medium, provided the original work is properly cited. All rights reserved. C1 [Li, Yan; Bareno, Javier; Bettge, Martin; Abraham, Daniel P.] Argonne Natl Lab, Argonne, IL 60439 USA. [Li, Yan] Univ Rochester, Rochester, NY 14627 USA. RP Li, Y (reprint author), Argonne Natl Lab, 9700 S Cass Ave, Argonne, IL 60439 USA. EM abraham@anl.gov RI Li, Yan/H-2957-2012; OI Li, Yan/0000-0002-9801-7243; Bareno, Javier/0000-0003-1230-9278 FU U.S. Department of Energy's Vehicle Technologies Program; DOE Vehicle Technologies Program (VTP) within Applied Battery Research (ABR) for Transportation Program; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]; U.S. Department of Energy Office of Science laboratory [DE-AC02-06CH11357]; U.S. Government FX Support from the U.S. Department of Energy's Vehicle Technologies Program, specifically from Peter Faguy and Dave Howell, is gratefully acknowledged. We are grateful to A. Jansen, B. Polzin, and S. Trask from the U.S. Department of Energy's (DOE) CAMP Facility, Argonne for the electrodes used in this study. The CAMP is fully supported by the DOE Vehicle Technologies Program (VTP) within the core funding of the Applied Battery Research (ABR) for Transportation Program. Use of the Advanced Photon Source (APS) was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. We are grateful to Matt Suchomel at APS beam line 11-BM for obtaining the high-resolution powder diffraction data. We are also grateful for the support and feedback from members of the Argonne Voltage Fade Team (A. Abouimrane, M. Balasubramanian, R. Benedek, I. Bloom, T. Burrell, Z. Chen J. Croy, D. Dees, F. Dogan, K. Gallagher, H. Iddir, B. Ingram, C. Johnson, B. Key, E. Lee, B. Long, W. Lu, D. Miller, M. Thackeray, Y. Ren, L. Trahey, Q. Wu, J. Vaughey).; The submitted manuscript has been created by UChicago Argonne, LLC, Operator of Argonne National Laboratory ("Argonne"). Argonne, a U.S. Department of Energy Office of Science laboratory, is operated under Contract No. DE-AC02-06CH11357. The U.S. Government retains for itself, and others acting on its behalf, a paid-up non-exclusive, irrevocable worldwide license in said article to reproduce, prepare derivative works, distribute copies to the public, and perform publicly and display publicly, by or on behalf of the Government. NR 49 TC 18 Z9 18 U1 5 U2 59 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 EI 1945-7111 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2015 VL 162 IS 1 BP A155 EP A161 DI 10.1149/2.0741501jes PG 7 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA AW0JZ UT WOS:000345979700007 PM 25560671 ER PT J AU Moy, D Manivannan, A Narayanan, SR AF Moy, Derek Manivannan, A. Narayanan, S. R. TI Direct Measurement of Polysulfide Shuttle Current: A Window into Understanding the Performance of Lithium-Sulfur Cells SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID LI-S BATTERIES; LIQUID ELECTROLYTE; CARBON NANOTUBES; FUNDAMENTAL CHEMISTRY; HIGH-CAPACITY; CATHODE; COMPOSITE; DENSITY AB The shuttling of polysulfide ions between the electrodes in a lithium-sulfur battery is a major technical issue limiting the self-discharge and cycle life of this high-energy rechargeable battery. Although there have been attempts to suppress the shuttling process, there has not been a direct measurement of the rate of shuttling. We report here a simple and direct measurement of the rate of the shuttling (that we term "shuttle current"), applicable to the study of any type of lithium-sulfur cell. We demonstrate the effectiveness of this measurement technique using cells with and without lithium nitrate (a widely-used shuttle suppressor additive). We present a phenomenological analysis of the shuttling process and simulate the shuttle currents as a function of the state-of-charge of a cell. We also demonstrate how the rate of decay of the shuttle current can be used to predict the capacity fade in a lithium-sulfur cell due to the shuttle process. We expect that this new ability to directly measure shuttle currents will provide greater insight into the performance differences observed with various additives and electrode modifications that are aimed at suppressing the rate of shuttling of polysulfide ions and increasing the cycle life of lithium-sulfur cells. (C) The Author(s) 2014. Published by ECS. This is an open access article distributed under the terms of the Creative Commons Attribution 4.0 License (CC BY, http://creativecommons.org/licenses/by/4.0/), which permits unrestricted reuse of the work in any medium, provided the original work is properly cited. All rights reserved. C1 [Moy, Derek; Narayanan, S. R.] Univ So Calif, Dept Chem, Loker Hydrocarbon Res Inst, Los Angeles, CA 90089 USA. [Manivannan, A.] US DOE, Natl Energy Technol Lab, Morgantown, WV 26507 USA. RP Moy, D (reprint author), Univ So Calif, Dept Chem, Loker Hydrocarbon Res Inst, Los Angeles, CA 90089 USA. EM sri.narayan@usc.edu FU Loker Hydrocarbon Research Institute, University of Southern California; U.S. Department of Energy - PIP Program FX The research reported here was supported by the Loker Hydrocarbon Research Institute, University of Southern California, and the U.S. Department of Energy - PIP Program for financial support to Derek Moy during the summer semester of 2013. NR 47 TC 23 Z9 23 U1 4 U2 68 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 EI 1945-7111 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2015 VL 162 IS 1 BP A1 EP A7 DI 10.1149/2.0181501jes PG 7 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA AW0JZ UT WOS:000345979700015 ER PT J AU Ruther, RE Callender, AF Zhou, H Martha, SK Nanda, J AF Ruther, Rose E. Callender, Andrew F. Zhou, Hui Martha, Surendra K. Nanda, Jagjit TI Raman Microscopy of Lithium-Manganese-Rich Transition Metal Oxide Cathodes SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID X-RAY-DIFFRACTION; ION BATTERY CATHODE; LOCAL-STRUCTURE; VOLTAGE FADE; COMPOSITION LI1.2MN0.525NI0.175CO0.1O2; ELECTROCHEMICAL ACTIVITY; ELECTRON-MICROSCOPY; LATTICE-VIBRATIONS; SITU; LI2MNO3 AB Lithium-rich and manganese-rich (LMR) layered transition metal (TM) oxide composites with general formula xLi(2)MnO(3) center dot (1-x)LiMO2 (M = Ni, Co, Mn) are promising cathode candidates for high energy density lithium ion batteries. Lithium-manganese-rich TM oxides crystallize as a nanocomposite layered phase whose structure further evolves with electrochemical cycling. Raman spectroscopy is a powerful tool to monitor the crystal chemistry and correlate phase changes with electrochemical behavior. While several groups have reported Raman spectra of lithium rich TM oxides, the data show considerable variability in terms of both the vibrational features observed and their interpretation. In this study, Raman microscopy is used to investigate lithium-rich and manganese-rich TM cathodes as a function of voltage and electrochemical cycling at various temperatures. No growth of a spinel phase is observed within the cycling conditions. However, analysis of the Raman spectra does indicate the structure of LMR-NMC deviates significantly from an ideal layered phase. The results also highlight the importance of using low laser power and large sample sizes to obtain consistent data sets. (C) The Author(s) 2014. Published by ECS. This is an open access article distributed under the terms of the Creative Commons Attribution Non-Commercial No Derivatives 4.0 License (CC BY-NC-ND, http://creativecommons.org/licenses/by-nc-nd/4.0/), which permits non-commercial reuse, distribution, and reproduction in any medium, provided the original work is not changed in any way and is properly cited. For permission for commercial reuse, please email: oa@electrochem.org. All rights reserved. C1 [Ruther, Rose E.; Zhou, Hui; Nanda, Jagjit] Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. [Callender, Andrew F.] Tennessee Technol Univ, Dept Chem, Cookeville, TN 38505 USA. [Martha, Surendra K.] Indian Inst Technol Hyderabad, Dept Chem, Yeddumailaram 502205, Telangana, India. RP Ruther, RE (reprint author), Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. EM rutherre@ornl.gov; nandaj@ornl.gov RI Ruther, Rose/I-9207-2016 OI Ruther, Rose/0000-0002-1391-902X FU U.S. Department of Energy [DE-AC05 00OR22725] FX This work was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the U.S. Department of Energy under the Batteries for Advanced Transportation Technologies (BATT) Program. Oak Ridge National Laboratory is managed by UT-Battelle, LLC, for the U.S. Department of Energy under contract no. DE-AC05 00OR22725. NR 59 TC 18 Z9 18 U1 18 U2 97 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 EI 1945-7111 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2015 VL 162 IS 1 BP A98 EP A102 DI 10.1149/2.0361501jes PG 5 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA AW0JZ UT WOS:000345979700036 ER PT J AU Seshadri, D Shirpour, M Doeff, M AF Seshadri, Dhruv Shirpour, Mona Doeff, Marca TI Electrochemical Properties of Electrodes Derived from NaTi3O6OH center dot 2H(2)O in Sodium and Lithium Cells SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID ION-EXCHANGE; INTERCALATION PROPERTIES; LAYERED STRUCTURE; TITANATE; LI; DIFFRACTION; STRONTIUM; BATTERIES; NA2TI3O7; CATHODE AB Materials derived from the layered compound NaTi3O6OH center dot 2H(2)O, also known as "sodium nonatitanate" or NNT, have recently been found to undergo reversible sodium or lithium intercalation processes at very low potentials. While practical discharge capacities in lithium cells can be above 200 mAh/g, making them of interest for high-energy applications, the presence of mobile sodium in the materials complicates the cycling behavior. A simple ion-exchange process prior to incorporation in electrochemical cells removes all sodium ions, producing the lithiated form of the material. The lithiated material (LNT) performs similarly to NNT in lithium cells, although coulombic inefficiencies are somewhat higher. A comparison is made between the behavior of NNT in sodium cells and that of NNT and the lithiated analog in lithium cells. (C) The Author(s) 2014. Published by ECS. This is an open access article distributed under the terms of the Creative Commons Attribution 4.0 License (CC BY, http://creativecommons.org/licenses/by/4.0/), which permits unrestricted reuse of the work in any medium, provided the original work is properly cited. All rights reserved. C1 [Seshadri, Dhruv; Shirpour, Mona; Doeff, Marca] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. RP Seshadri, D (reprint author), Texas A&M Univ, Dept Biomed Engn, College Stn, TX 77843 USA. EM mmdoeff@lbl.gov FU Laboratory Directed Research and Development Program of Lawrence Berkeley National Laboratory under U.S. Department of Energy [DE-AC02- 05CH11231]; U.S. Department of Energy FX This work was supported by the Laboratory Directed Research and Development Program of Lawrence Berkeley National Laboratory under U.S. Department of Energy Contract DE-AC02- 05CH11231. Portions of this research were carried out at the Stanford Synchrotron Radiation Lightsource, a Directorate of SLAC National Accelerator Laboratory and an Office of Science User Facility operated for the U.S. Department of Energy Office of Science by Stanford University. D.S. thank the Science Undergraduate Laboratory Internship (SULI) program sponsored by the U.S. Department of Energy for a summer internship spent at Lawrence Berkeley National Laboratory. NR 19 TC 3 Z9 3 U1 5 U2 32 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 EI 1945-7111 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2015 VL 162 IS 1 BP A52 EP A59 DI 10.1149/2.0391501jes PG 8 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA AW0JZ UT WOS:000345979700028 ER PT J AU Zheng, D Zhang, XR Li, C McKinnon, ME Sadok, RG Qu, DY Yu, XQ Lee, HS Yang, XQ Qu, DY AF Zheng, Dong Zhang, Xuran Li, Chao McKinnon, Meaghan E. Sadok, Rachel G. Qu, Deyu Yu, Xiqian Lee, Hung-Sui Yang, Xiao-Qing Qu, Deyang TI Quantitative Chromatographic Determination of Dissolved Elemental Sulfur in the Non-Aqueous Electrolyte for Lithium-Sulfur Batteries SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID PERFORMANCE LIQUID-CHROMATOGRAPHY; POLYSULFIDES; REDUCTION; SOLVENTS AB A fast and reliable analytical method is reported for the quantitative determination of dissolved elemental sulfur in non-aqueous electrolytes for Li-S batteries. By using high performance liquid chromatography with a UV detector, the solubility of S in 12 different pure solvents and in 22 different electrolytes was determined. It was found that the solubility of elemental sulfur is dependent on the Lewis basicity, the polarity of solvents and the salt concentration in the electrolytes. In addition, the S content in the electrolyte recovered from a discharged Li-S battery was successfully determined by the proposed HPLC/UV method. Thus, the feasibility of the method to the online analysis for a Li-S battery is demonstrated. Interestingly, the S was found super-saturated in the electrolyte recovered from a discharged Li-S cell. (C) 2014 The Electrochemical Society. All rights reserved. C1 [Zheng, Dong; Li, Chao; McKinnon, Meaghan E.; Sadok, Rachel G.; Qu, Deyang] Univ Massachusetts, Dept Chem, Boston, MA 02125 USA. [Zhang, Xuran; Qu, Deyu] Wuhan Univ Technol, Sch Sci, Dept Chem, Wuhan 430070, Hubei, Peoples R China. [Yu, Xiqian; Lee, Hung-Sui; Yang, Xiao-Qing] Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA. RP Zheng, D (reprint author), Univ Massachusetts, Dept Chem, Boston, MA 02125 USA. EM deyang.qu@umb.edu RI Zheng, Dong/J-9975-2015; Yu, Xiqian/B-5574-2014 OI Zheng, Dong/0000-0002-5824-3270; Yu, Xiqian/0000-0001-8513-518X FU Office of Vehicle Technologies of the U.S. Department of Energy; Office of Vehicle Technologies under program of Vehicle Technology Program [DEAC02-98CH10886]; Fundamental Research Fund for the Central Universities China [2013-Ia-016, 2013-Ia-034, 2014-Ia-033, 2014-zy-166, 2014-LX-B1-11] FX The authors from UMB are indebted to the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the U.S. Department of Energy for financial support and the work done at Brookhaven National Lab. is supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies, under the program of Vehicle Technology Program, under Contract Number DEAC02-98CH10886. The work done in WUT was partially financially supported by the Fundamental Research Fund for the Central Universities China 2013-Ia-016, 2013-Ia-034, 2014-Ia-033, 2014-zy-166 and 2014-LX-B1-11. NR 21 TC 11 Z9 11 U1 9 U2 59 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 EI 1945-7111 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2015 VL 162 IS 1 BP A203 EP A206 DI 10.1149/2.1011501jes PG 4 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA AW0JZ UT WOS:000345979700016 ER PT J AU Gao, PP Lara-Curzio, E Trejo, R Radovic, M AF Gao, Peipei Lara-Curzio, Edgar Trejo, Rosa Radovic, Miladin TI Dynamic Mechanical Analysis of Phase Transformations and Anelastic Relaxation in Stabilized Zirconias SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID ION-CONDUCTING MEMBRANES; OXIDE FUEL-CELLS; ELECTRICAL-CONDUCTIVITY; DIELECTRIC-RELAXATION; ELEVATED-TEMPERATURES; LOCALIZED RELAXATION; INTERNAL-FRICTION; DEFECT STRUCTURE; DOPED ZIRCONIA; CUBIC ZIRCONIA AB Elastic properties of polycrystalline stabilized zirconias, namely Yttria Stabilized Zirconia (YSZ) and Scandia, Ceria Stabilized Zirconia (SCSZ), were studied by Dynamic Mechanical Analyzer (DMA) in air. Changes of storage modulus E ', loss modulus E '' and mechanical damping (tan delta) with temperature were simultaneously monitored at various frequencies. In 8 mol% (8YSZ) and 10 mol% (10YSZ) Yttria Stabilized Zirconia, a drop in storage modulus of similar to 37% was observed in the 30 degrees C to 400 degrees C temperature range, together with two frequency dependent damping peaks. While the first tan delta peak can be attributed to the anelastic relaxation of (Y-Zr'V-O(center dot center dot))(center dot) elastic (and dielectric) dipoles, the second one is probably the result of local ordering of oxygen vacancies and/or relaxation of (2Y(Zr)' V-O(center dot center dot))(x) dipoles. For cubic SCSZ, four damping peaks were observed in the similar temperature regime accompanied by significant nonlinear drop of the storage modulus. The first tan delta is attributed to anealstic relaxation of (Sc-Zr' V-O(center dot center dot))(center dot). It was also found that stress induced phase transformation from cubic to rhombohedral structure is the reason for the frequency dependent third peak in the tan delta spectra while the fourth frequency independent peak was found to be the result of the phase transformation from rhombohedral to cubic structure. (C) 2014 The Electrochemical Society. All rights reserved. C1 [Gao, Peipei; Radovic, Miladin] Texas A&M Univ, Dept Mech Engn, College Stn, TX 77843 USA. [Lara-Curzio, Edgar; Trejo, Rosa] Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. [Radovic, Miladin] Texas A&M Univ, Dept Mat Sci & Engn, College Stn, TX 77843 USA. RP Gao, PP (reprint author), Texas A&M Univ, Dept Mech Engn, College Stn, TX 77843 USA. EM mradovic@tamu.edu FU U.S. National Science Foundation [DMR-1057155] FX The authors are grateful to U.S. National Science Foundation, for supporting this work under the grant DMR-1057155 awarded to Texas A&M University. NR 47 TC 1 Z9 1 U1 2 U2 15 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 EI 1945-7111 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2015 VL 162 IS 1 BP F14 EP F22 DI 10.1149/2.0941414jes PG 9 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA AW0JZ UT WOS:000345979700074 ER PT J AU Veal, BW Baldo, PM Paulikas, AP Eastman, JA AF Veal, B. W. Baldo, P. M. Paulikas, A. P. Eastman, J. A. TI Understanding Artifacts in Impedance Spectroscopy SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID YTTRIA-STABILIZED ZIRCONIA; THIN-FILMS; EXPERIMENTAL LIMITATIONS; REFERENCE ELECTRODE; IONIC-CONDUCTIVITY; THERMAL-EXPANSION; SRTIO3; TRANSPORT; SYSTEM AB Four-terminal measurements of impedance spectra have long been troubled by the presence of high frequency artifacts that typically indicate unphysically large inductive behavior. We follow up on the observation of Fleig et al., that voltage and current are necessarily measured in different locations of the potentiostat circuit, and that, typically, the electrometer input is a virtual ground. In this case, the capacitance of coaxial cables that connect sample electrodes to the potentiostat provides a high frequency conduction path to ground, so that some of the current that passes through the sample bypasses the electrometer. In four-electrode measurements, this mechanism produces the observed inductive artifacts. We examine a variety of simulated samples, with calculations compared to measurements of relevant circuits, to quantitatively investigate the nature of the artifacts. Model results agree with measurements when the leakage capacitances are properly included in the circuit analyses. With understanding of the origin of the inductive artifacts, the four-electrode method can be effectively utilized, enabling a combination of two-, three-and four-electrode measurements to be used to best advantage. Using this combination of electrode configurations, temperature dependent measurements of SrTiO3, Y2O3-stabilized ZrO2, and In2O3 films deposited on YSZ substrates are presented. (C) The Author(s) 2014. Published by ECS. This is an open access article distributed under the terms of the Creative Commons Attribution Non-Commercial No Derivatives 4.0 License (CC BY-NC-ND, http://creativecommons.org/licenses/by-nc-nd/4.0/), which permits non-commercial reuse, distribution, and reproduction in any medium, provided the original work is not changed in any way and is properly cited. For permission for commercial reuse, please email: oa@electrochem.org. All rights reserved. C1 [Veal, B. W.; Baldo, P. M.; Paulikas, A. P.; Eastman, J. A.] Argonne Natl Lab, Div Mat Sci, Argonne, IL 60439 USA. RP Veal, BW (reprint author), Argonne Natl Lab, Div Mat Sci, 9700 S Cass Ave, Argonne, IL 60439 USA. EM jeastman@anl.gov OI Eastman, Jeff/0000-0002-0847-4265 FU U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division FX This work was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division. Helpful discussions with P. Zapol are gratefully acknowledged. NR 24 TC 2 Z9 2 U1 0 U2 26 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 EI 1945-7111 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2015 VL 162 IS 1 BP H47 EP H57 DI 10.1149/2.0791501jes PG 11 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA AW0JZ UT WOS:000345979700103 ER PT J AU Davis, MJ Janke, R AF Davis, Michael J. Janke, Robert TI Influence of Network Model Detail on Estimated Health Effects of Drinking Water Contamination Events SO JOURNAL OF WATER RESOURCES PLANNING AND MANAGEMENT LA English DT Article DE Water distribution systems; Simulation; Water quality; Drinking water; Public health ID DISTRIBUTION-SYSTEMS AB Network model detail can influence the accuracy of results from analyses of water distribution systems. Previous work has shown the limitations of skeletonized network models when considering water quality and hydraulic effects. Loss of model detail is potentially less important for aggregated effects such as the systemwide health effects associated with a contamination event, but has received limited attention. The influence of model detail on such effects is examined here by comparing results obtained for contamination events using three large network models and several skeletonized versions of the models. Loss of model detail decreases the accuracy of estimated aggregated adverse effects related to contamination events. It has the potential to have a large negative influence on the results of consequence assessments and the design of contamination warning systems. However, the adverse influence on analysis results can be minimized by restricting attention to high percentile effects (i.e.,95th percentile or higher). C1 [Davis, Michael J.] Argonne Natl Lab, Div Environm Sci, Argonne, IL 60439 USA. [Janke, Robert] US EPA, Natl Homeland Secur Res Ctr, Cincinnati, OH 45268 USA. RP Davis, MJ (reprint author), Argonne Natl Lab, Div Environm Sci, 9700 S Cass Ave, Argonne, IL 60439 USA. EM mike_davis@anl.gov; janke.robert@epa.gov FU U.S. Environmental Protection Agency's (EPA's) Office of Research and Development; EPA under U.S. Department of Energy [DE-AC02-06CH11357] FX The U.S. Environmental Protection Agency's (EPA's) Office of Research and Development funded, managed, and participated in the research described here under an interagency agreement. The views expressed in this paper are those of the authors and do not necessarily reflect the views or policies of EPA. Mention of trade names or commercial products does not constitute endorsement or recommendation for use. Work at Argonne National Laboratory was sponsored by the EPA under an interagency agreement through U.S. Department of Energy Contract DE-AC02-06CH11357. NR 23 TC 1 Z9 1 U1 0 U2 4 PU ASCE-AMER SOC CIVIL ENGINEERS PI RESTON PA 1801 ALEXANDER BELL DR, RESTON, VA 20191-4400 USA SN 0733-9496 EI 1943-5452 J9 J WATER RES PLAN MAN JI J. Water Resour. Plan. Manage.-ASCE PD JAN PY 2015 VL 141 IS 1 AR UNSP 04014044 DI 10.1061/(ASCE)WR.1943-5452.0000436 PG 9 WC Engineering, Civil; Water Resources SC Engineering; Water Resources GA AW5WX UT WOS:000346342800003 ER PT J AU Jebrail, MJ Renzi, RF Sinha, A Van De Vreugde, J Gondhalekar, C Ambriz, C Meagher, RJ Branda, SS AF Jebrail, Mais J. Renzi, Ronald F. Sinha, Anupama Van De Vreugde, Jim Gondhalekar, Carmen Ambriz, Cesar Meagher, Robert J. Branda, Steven S. TI A solvent replenishment solution for managing evaporation of biochemical reactions in air-matrix digital microfluidics devices SO LAB ON A CHIP LA English DT Article ID ELECTROWETTING-BASED ACTUATION; ON-CHIP; CHEMISTRY; DROPLETS; EXTRACTION; INTERFACE; BIOLOGY; RNA AB Digital microfluidics (DMF) is a powerful technique for sample preparation and analysis for a broad range of biological and chemical applications. In many cases, it is desirable to carry out DMF on an open surface, such that the matrix surrounding the droplets is ambient air. However, the utility of the air-matrix DMF format has been severely limited by problems with droplet evaporation, especially when the droplet-based biochemical reactions require high temperatures for long periods of time. We present a simple solution for managing evaporation in air-matrix DMF: just-in-time replenishment of the reaction volume using droplets of solvent. We demonstrate that this solution enables DMF-mediated execution of several different biochemical reactions (RNA fragmentation, first-strand cDNA synthesis, and PCR) over a range of temperatures (4-95 degrees C) and incubation times (up to 1 h or more) without use of oil, humidifying chambers, or off-chip heating modules. Reaction volumes and temperatures were maintained roughly constant over the course of each experiment, such that the reaction kinetics and products generated by the air-matrix DMF device were comparable to those of conventional benchscale reactions. This simple yet effective solution for evaporation management is an important advance in developing air-matrix DMF for a wide variety of new, high-impact applications, particularly in the biomedical sciences. C1 [Jebrail, Mais J.; Renzi, Ronald F.; Sinha, Anupama; Van De Vreugde, Jim; Gondhalekar, Carmen; Ambriz, Cesar; Meagher, Robert J.; Branda, Steven S.] Sandia Natl Labs, Livermore, CA 94551 USA. RP Branda, SS (reprint author), Sandia Natl Labs, Livermore, CA 94551 USA. EM sbranda@sandia.gov FU Sandia National Laboratories (SNL) Laboratory-Directed Research and Development (LDRD) program [158814]; U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX This work was funded by the Sandia National Laboratories (SNL) Laboratory-Directed Research and Development (LDRD) program (grant 158814). SNL is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000. NR 27 TC 11 Z9 11 U1 2 U2 26 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1473-0197 EI 1473-0189 J9 LAB CHIP JI Lab Chip PY 2015 VL 15 IS 1 BP 151 EP 158 DI 10.1039/c4lc00703d PG 8 WC Biochemical Research Methods; Chemistry, Multidisciplinary; Nanoscience & Nanotechnology SC Biochemistry & Molecular Biology; Chemistry; Science & Technology - Other Topics GA AW7YQ UT WOS:000346478100019 PM 25325619 ER PT J AU Shih, SCC Gach, PC Sustarich, J Simmons, BA Adams, PD Singh, S Singh, AK AF Shih, Steve C. C. Gach, Philip C. Sustarich, Jess Simmons, Blake A. Adams, Paul D. Singh, Seema Singh, Anup K. TI A droplet-to-digital (D2D) microfluidic device for single cell assays SO LAB ON A CHIP LA English DT Article ID IONIC LIQUID PRETREATMENT; PLURONIC ADDITIVES; BIOFUEL PRODUCTION; LIPID PRODUCTION; GROWTH; PLATFORM; YEAST; SACCHARIFICATION; ENCAPSULATION; SWITCHGRASS AB We have developed a new hybrid droplet-to-digital microfluidic platform (D2D) that integrates droplet-in-channel microfluidics with digital microfluidics (DMF) for performing multi-step assays. This D2D platform combines the strengths of the two formats-droplets-in-channel for facile generation of droplets containing single cells, and DMF for on-demand manipulation of droplets including control of different droplet volumes (pL-mu L), creation of a dilution series of ionic liquid (IL), and parallel single cell culturing and analysis for IL toxicity screening. This D2D device also allows for automated analysis that includes a feedback-controlled system for merging and splitting of droplets to add reagents, an integrated Peltier element for parallel cell culture at optimum temperature, and an impedance sensing mechanism to control the flow rate for droplet generation and preventing droplet evaporation. Droplet-in-channel is well-suited for encapsulation of single cells as it allows the careful manipulation of flow rates of aqueous phase containing cells and oil to optimize encapsulation. Once single cell containing droplets are generated, they are transferred to a DMF chip via a capillary where they are merged with droplets containing IL and cultured at 30 degrees C. The DMF chip, in addition to permitting cell culture and reagent (ionic liquid/salt) addition, also allows recovery of individual droplets for off-chip analysis such as further culturing and measurement of ethanol production. The D2D chip was used to evaluate the effect of IL/salt type (four types: NaOAc, NaCl, [C(2)mim] [OAc], [C(2)mim] [Cl]) and concentration (four concentrations: 0, 37.5, 75, 150 mM) on the growth kinetics and ethanol production of yeast and as expected, increasing IL concentration led to lower biomass and ethanol production. Specifically, [C(2)mim] [OAc] had inhibitory effects on yeast growth at concentrations 75 and 150 mM and significantly reduced their ethanol production compared to cells grown in other ILs/salts. The growth curve trends obtained by D2D matched conventional yeast culturing in microtiter wells, validating the D2D platform. We believe that our approach represents a generic platform for multi-step biochemical assays such as drug screening, digital PCR, enzyme assays, immunoassays and cell-based assays. C1 [Shih, Steve C. C.; Gach, Philip C.; Sustarich, Jess; Simmons, Blake A.; Singh, Seema; Singh, Anup K.] Sandia Natl Labs, Livermore, CA 94551 USA. [Shih, Steve C. C.; Gach, Philip C.; Sustarich, Jess; Simmons, Blake A.; Adams, Paul D.; Singh, Seema; Singh, Anup K.] Joint Bioenergy Inst JBEI, Emeryville, CA USA. [Adams, Paul D.] LBNL, Berkeley, CA 94720 USA. [Adams, Paul D.] Univ Calif Berkeley, Dept Bioengn, Berkeley, CA 94720 USA. RP Singh, AK (reprint author), Sandia Natl Labs, 7011 East Ave, Livermore, CA 94551 USA. EM aksingh@sandia.gov RI Adams, Paul/A-1977-2013; OI Adams, Paul/0000-0001-9333-8219; Simmons, Blake/0000-0002-1332-1810; Shih, Steve/0000-0003-3540-0808 FU US Department of Energy, Office of Science, Office of Biological and Environmental Research [DE-AC02-05CH11231]; United States Department of Energy's Nuclear Security Administration [DE-AC04-94AL85000] FX The authors thank Marijke Frederix and Dr. Aindrila Mukhopadhyay for the yeast isolate; Susan Yilmaz for initial help with microscopy; Jennifer Gin, Edward Baidoo, Helcio Burd for their assistance with operating the HPLC and chromatogram analysis; This work was part of the DOE Joint BioEnergy Institute (www.jbei.org), supported by the US Department of Energy, Office of Science, Office of Biological and Environmental Research, through contract DE-AC02-05CH11231 between Lawrence Berkeley National Laboratory and the US Department of Energy. Sandia is a multi-program laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the United States Department of Energy's Nuclear Security Administration under contract DE-AC04-94AL85000. NR 64 TC 20 Z9 20 U1 24 U2 172 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1473-0197 EI 1473-0189 J9 LAB CHIP JI Lab Chip PY 2015 VL 15 IS 1 BP 225 EP 236 DI 10.1039/c4lc00794h PG 12 WC Biochemical Research Methods; Chemistry, Multidisciplinary; Nanoscience & Nanotechnology SC Biochemistry & Molecular Biology; Chemistry; Science & Technology - Other Topics GA AW7YQ UT WOS:000346478100027 PM 25354549 ER PT J AU Lee, J Wall, JJ Rogers, JR Rathz, TJ Choo, H Liaw, PK Hyers, RW AF Lee, J. Wall, J. J. Rogers, J. R. Rathz, T. J. Choo, H. Liaw, P. K. Hyers, R. W. TI Non-contact measurements of creep properties of niobium at 1985 degrees C SO MEASUREMENT SCIENCE AND TECHNOLOGY LA English DT Article DE creep; electrostatic levitation; refractory metals; high temperature deformation ID HIGH-TEMPERATURE MATERIALS; NICKEL-BASE SUPERALLOY; FINITE-ELEMENT MODEL; SI-B ALLOY; REFRACTORY-METALS; MELTING-POINT; CRACK-GROWTH; BEHAVIOR; LEVITATION; COMPOSITE AB The stress exponent in the power-law creep of niobium at 1985 degrees C was measured by a non-contact technique using an electrostatic levitation facility at NASA MSFC. This method employs a distribution of stress to allow the stress exponent to be determined from each test, rather than from the curve fit through measurements from multiple samples that is required by conventional methods. The sample is deformed by the centripetal acceleration from the rapid rotation, and the deformed shapes are analyzed to determine the strain. Based on a mathematical proof, which revealed that the stress exponent was determined uniquely by the ratio of the polar to equatorial strains, a series of finite-element analyses with the models of different stress exponents were also performed to determine the stress exponent corresponding to the measured strain ratio. The stress exponent from the ESL experiment showed a good agreement with those from the literature and the conventional creep test. C1 [Lee, J.; Hyers, R. W.] Univ Massachusetts, Amherst, MA 01003 USA. [Wall, J. J.] Los Alamos Natl Lab, LANSCE LC, Los Alamos, NM 87545 USA. [Wall, J. J.; Choo, H.; Liaw, P. K.] Univ Tennessee, Knoxville, TN 37996 USA. [Rogers, J. R.] NASA, George C Marshall Space Flight Ctr, Huntsville, AL 35812 USA. [Rathz, T. J.] Univ Alabama, Huntsville, AL 35899 USA. RP Lee, J (reprint author), Univ Massachusetts, Amherst, MA 01003 USA. EM jonghyunlee@ecs.umass.edu RI Choo, Hahn/A-5494-2009 OI Choo, Hahn/0000-0002-8006-8907 FU NASA [NNM04AA78G, NNM04AA19A] FX This research has been sponsored in part by NASA under grants NNM04AA78G and NNM04AA19A. The experimental portion of this work was performed at the NASA MSFC Electrostatic Levitation Facility. The authors thank Trudy Allen and Glenn Fountain at NASA MSFC for their technical support. NR 52 TC 0 Z9 0 U1 2 U2 19 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 0957-0233 EI 1361-6501 J9 MEAS SCI TECHNOL JI Meas. Sci. Technol. PD JAN PY 2015 VL 26 IS 1 AR 015901 DI 10.1088/0957-0233/26/1/015901 PG 8 WC Engineering, Multidisciplinary; Instruments & Instrumentation SC Engineering; Instruments & Instrumentation GA AW6DS UT WOS:000346360300027 ER PT J AU Aetukuri, NB McCloskey, BD Garcia, JM Krupp, LE Viswanathan, V Luntz, AC AF Aetukuri, Nagaphani B. McCloskey, Bryan D. Garcia, Jeannette M. Krupp, Leslie E. Viswanathan, Venkatasubramanian Luntz, Alan C. TI Solvating additives drive solution-mediated electrochemistry and enhance toroid growth in non-aqueous Li-O-2 batteries SO NATURE CHEMISTRY LA English DT Article ID LI-AIR BATTERIES; CHARGE-TRANSPORT; CARBON CATHODE; LI2O2; LITHIUM; ELECTROLYTE; LIMITATIONS; MORPHOLOGY; STABILITY; DISCHARGE AB Given their high theoretical specific energy, lithium-oxygen batteries have received enormous attention as possible alternatives to current state-of-the-art rechargeable Li-ion batteries. However, the maximum discharge capacity in nonaqueous lithium-oxygen batteries is limited to a small fraction of its theoretical value due to the build-up of insulating lithium peroxide (Li2O2), the battery's primary discharge product. The discharge capacity can be increased if Li2O2 forms as large toroidal particles rather than as a thin conformal layer. Here, we show that trace amounts of electrolyte additives, such as H2O, enhance the formation of Li2O2 toroids and result in significant improvements in capacity. Our experimental observations and a growth model show that the solvating properties of the additives prompt a solution-based mechanism that is responsible for the growth of Li2O2 toroids. We present a general formalism describing an additive's tendency to trigger the solution process, providing a rational design route for electrolytes that afford larger lithium-oxygen battery capacities. C1 [Aetukuri, Nagaphani B.; McCloskey, Bryan D.; Garcia, Jeannette M.; Krupp, Leslie E.; Luntz, Alan C.] IBM Corp, Almaden Res Ctr, San Jose, CA 95120 USA. [McCloskey, Bryan D.] Univ Calif Berkeley, Dept Chem & Biomol Engn, Berkeley, CA 94720 USA. [McCloskey, Bryan D.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. [Viswanathan, Venkatasubramanian] Carnegie Mellon Univ, Dept Mech Engn, Pittsburgh, PA 15213 USA. [Luntz, Alan C.] SLAC Natl Accelerator Lab, SUNCAT, Menlo Pk, CA 94025 USA. RP Aetukuri, NB (reprint author), IBM Corp, Almaden Res Ctr, 650 Harry Rd, San Jose, CA 95120 USA. EM phani@alumni.stanford.edu; venkvis@cmu.edu RI Aetukuri, Nagaphani/A-2107-2015; McCloskey, Bryan/A-6556-2015; OI Aetukuri, Nagaphani/0000-0001-7269-5057; McCloskey, Bryan/0000-0001-6599-2336; Viswanathan, Venkatasubramanian/0000-0003-1060-5495 FU IBM model shop; Carnegie Mellon University FX The authors thank R. Shelby for Raman measurements, D. Bethune and G. Wallraff for discussions and help with experiments and the IBM model shop for support with the DEMS system. N.B.A. acknowledges guidance from H.C. Kim and W.W. Wilcke. V.V. is supported by a faculty startup grant from Carnegie Mellon University. NR 42 TC 168 Z9 168 U1 39 U2 311 PU NATURE PUBLISHING GROUP PI LONDON PA MACMILLAN BUILDING, 4 CRINAN ST, LONDON N1 9XW, ENGLAND SN 1755-4330 EI 1755-4349 J9 NAT CHEM JI Nat. Chem. PD JAN PY 2015 VL 7 IS 1 BP 50 EP 56 DI 10.1038/NCHEM.2132 PG 7 WC Chemistry, Multidisciplinary SC Chemistry GA AW6XQ UT WOS:000346409400012 PM 25515890 ER PT J AU Tang, JY Riley, WJ AF Tang, Jinyun Riley, William J. TI Weaker soil carbon-climate feedbacks resulting from microbial and abiotic interactions SO NATURE CLIMATE CHANGE LA English DT Article ID ORGANIC-MATTER; TEMPERATURE SENSITIVITY; RESPIRATION; DECOMPOSITION; DEPENDENCE; DYNAMICS; COMPLEX; MODELS; FOREST AB The large uncertainty in soil carbon-climate feedback predictions has been attributed to the incorrect parameterization of decomposition temperature sensitivity (Q(10); ref. 1) and microbial carbon use effciency(2). Empirical experiments have found that these parameters vary spatiotemporally(3-6), but such variability is not included in current ecosystem models(7-13). Here we use a thermodynamically based decomposition model to test the hypothesis that this observed variability arises from interactions between temperature, microbial biogeochemistry, and mineral surface sorptive reactions. We show that because mineral surfaces interact with substrates, enzymes and microbes, both Q(10) and microbial carbon use effciency are hysteretic (so that neither can be represented by a single static function) and the conventional labile and recalcitrant substrate characterization with static temperature sensitivity is flawed. In a 4-K temperature perturbation experiment, our fully dynamic model predicted more variable but weaker soil carbon-climate feedbacks than did the static Q(10) and static carbon use effciency model when forced with yearly, daily and hourly variable temperatures. These results imply that current Earth system models probably overestimate the response of soil carbon stocks to global warming. Future ecosystem models should therefore consider the dynamic interactions between sorptive mineral surfaces, substrates and microbial processes. C1 [Tang, Jinyun; Riley, William J.] Lawrence Berkeley Natl Lab LBL, Div Earth Sci, Berkeley, CA 94720 USA. RP Tang, JY (reprint author), Lawrence Berkeley Natl Lab LBL, Div Earth Sci, Berkeley, CA 94720 USA. EM jinyuntang@lbl.gov RI Tang, Jinyun/M-4922-2013; Riley, William/D-3345-2015 OI Tang, Jinyun/0000-0002-4792-1259; Riley, William/0000-0002-4615-2304 FU Office of Science, Office of Biological and Environmental Research of the US Department of Energy as part of their Regional and Global Climate Modeling (RGCM) Program [DE-AC02-05CH11231]; Next-Generation Ecosystem Experiments (NGEE Arctic) project; Early Career Development Grant by Earth Sciences Division of Lawrence Berkeley National Laboratory FX This research was supported by the Director, Office of Science, Office of Biological and Environmental Research of the US Department of Energy, under contract no. DE-AC02-05CH11231, as part of their Regional and Global Climate Modeling (RGCM) Program; and by the Next-Generation Ecosystem Experiments (NGEE Arctic) project. J.Y.T. is also supported by an Early Career Development Grant provided by the Earth Sciences Division of Lawrence Berkeley National Laboratory. NR 29 TC 34 Z9 34 U1 15 U2 113 PU NATURE PUBLISHING GROUP PI LONDON PA MACMILLAN BUILDING, 4 CRINAN ST, LONDON N1 9XW, ENGLAND SN 1758-678X EI 1758-6798 J9 NAT CLIM CHANGE JI Nat. Clim. Chang. PD JAN PY 2015 VL 5 IS 1 BP 56 EP 60 DI 10.1038/NCLIMATE2438 PG 5 WC Environmental Sciences; Environmental Studies; Meteorology & Atmospheric Sciences SC Environmental Sciences & Ecology; Meteorology & Atmospheric Sciences GA AW8LQ UT WOS:000346513900019 ER PT J AU Cademartiri, L Bishop, KJM AF Cademartiri, Ludovico Bishop, Kyle J. M. TI Programmable self-assembly SO NATURE MATERIALS LA English DT Article ID NANOPARTICLE SUPERLATTICES; COMPLEX STRUCTURES; PATCHY PARTICLES; BUILDING-BLOCKS; DNA; NANOWIRES; CRYSTALS; COLLOIDS; FORCES; CRYSTALLIZATION C1 [Cademartiri, Ludovico] Iowa State Univ Sci & Technol, Dept Mat Sci & Engn, Ames, IA 50011 USA. [Cademartiri, Ludovico] Iowa State Univ Sci & Technol, Dept Chem & Biol Engn, Ames, IA 50011 USA. [Cademartiri, Ludovico] US DOE, Ames Lab, Ames, IA 50011 USA. [Bishop, Kyle J. M.] Penn State Univ, Dept Chem Engn, University Pk, PA 16802 USA. RP Cademartiri, L (reprint author), Iowa State Univ Sci & Technol, Dept Mat Sci & Engn, 2240J Hoover Hall, Ames, IA 50011 USA. EM lcademar@iastate.edu RI Bishop, Kyle/F-1742-2010; Cademartiri, Ludovico/A-4142-2008 OI Cademartiri, Ludovico/0000-0001-8805-9434 NR 75 TC 56 Z9 56 U1 35 U2 274 PU NATURE PUBLISHING GROUP PI LONDON PA MACMILLAN BUILDING, 4 CRINAN ST, LONDON N1 9XW, ENGLAND SN 1476-1122 EI 1476-4660 J9 NAT MATER JI Nat. Mater. PD JAN PY 2015 VL 14 IS 1 BP 2 EP 9 DI 10.1038/nmat4184 PG 8 WC Chemistry, Physical; Materials Science, Multidisciplinary; Physics, Applied; Physics, Condensed Matter SC Chemistry; Materials Science; Physics GA AW7FM UT WOS:000346430100002 PM 25515989 ER PT J AU Wegst, UGK Bai, H Saiz, E Tomsia, AP Ritchie, RO AF Wegst, Ulrike G. K. Bai, Hao Saiz, Eduardo Tomsia, Antoni P. Ritchie, Robert O. TI Bioinspired structural materials SO NATURE MATERIALS LA English DT Review ID DENTIN-ENAMEL JUNCTION; CALCIUM-PHOSPHATE MINERALIZATION; SYNTHETIC-POLYMER SCAFFOLDS; HUMAN CORTICAL BONE; MECHANICAL-PROPERTIES; BIOMIMETIC MATERIALS; CERAMIC STRUCTURES; NATURAL MATERIALS; HYBRID MATERIALS; NACRE FORMATION AB Natural structural materials are built at ambient temperature from a fairly limited selection of components. They usually comprise hard and soft phases arranged in complex hierarchical architectures, with characteristic dimensions spanning from the nanoscale to the macroscale. The resulting materials are lightweight and often display unique combinations of strength and toughness, but have proven difficult to mimic synthetically. Here, we review the common design motifs of a range of natural structural materials, and discuss the difficulties associated with the design and fabrication of synthetic structures that mimic the structural and mechanical characteristics of their natural counterparts. C1 [Wegst, Ulrike G. K.] Dartmouth Coll, Thayer Sch Engn, Hanover, NH 03755 USA. [Bai, Hao; Tomsia, Antoni P.; Ritchie, Robert O.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. [Saiz, Eduardo] Univ London Imperial Coll Sci Technol & Med, Ctr Adv Struct Ceram, Dept Mat, London SW7 2AZ, England. [Ritchie, Robert O.] Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA. RP Wegst, UGK (reprint author), Dartmouth Coll, Thayer Sch Engn, Hanover, NH 03755 USA. EM ulrike.wegst@dartmouth.edu; roritchie@lbl.gov RI Ritchie, Robert/A-8066-2008; Bai, Hao/J-5255-2012; Bai, Hao/D-1713-2017; OI Ritchie, Robert/0000-0002-0501-6998; Bai, Hao/0000-0002-1707-4976; Bai, Hao/0000-0002-3348-6129; Wegst, Ulrike G.K./0000-0002-9057-415X FU Mechanical Behavior of Materials Program at Lawrence Berkeley National Laboratory - U.S. Department of Energy, Office of Basic Energy Sciences, Materials Sciences and Engineering Division [DE-AC02-05CH11231]; National Science Foundation [CMMI-1200408]; European Commission (FP7 Programme, reintegration grant BISM) FX This work was supported by the Mechanical Behavior of Materials Program at Lawrence Berkeley National Laboratory, funded by the U.S. Department of Energy, Office of Basic Energy Sciences, Materials Sciences and Engineering Division, under Contract No. DE-AC02-05CH11231. U.G.K.W. acknowledges support from the National Science Foundation through CMMI-1200408. E.S. acknowledges support from the European Commission (FP7 Programme, reintegration grant BISM). We are grateful to many colleagues and collaborators, J. Kerr and M. Snead in particular, for helpful discussions. We would also like to thank S. Russell for helpful comments in editing this manuscript, and A. Lapp and Z. Deretsky from LevelFive.com for help with the figures. NR 138 TC 302 Z9 306 U1 183 U2 870 PU NATURE PUBLISHING GROUP PI LONDON PA MACMILLAN BUILDING, 4 CRINAN ST, LONDON N1 9XW, ENGLAND SN 1476-1122 EI 1476-4660 J9 NAT MATER JI Nat. Mater. PD JAN PY 2015 VL 14 IS 1 BP 23 EP 36 DI 10.1038/NMAT4089 PG 14 WC Chemistry, Physical; Materials Science, Multidisciplinary; Physics, Applied; Physics, Condensed Matter SC Chemistry; Materials Science; Physics GA AW7FM UT WOS:000346430100010 PM 25344782 ER PT J AU Hashimoto, M Nowadnick, EA He, RH Vishik, IM Moritz, B He, Y Tanaka, K Moore, RG Lu, DH Yoshida, Y Ishikado, M Sasagawa, T Fujita, K Ishida, S Uchida, S Eisaki, H Hussain, Z Devereaux, TP Shen, ZX AF Hashimoto, Makoto Nowadnick, Elizabeth A. He, Rui-Hua Vishik, Inna M. Moritz, Brian He, Yu Tanaka, Kiyohisa Moore, Robert G. Lu, Donghui Yoshida, Yoshiyuki Ishikado, Motoyuki Sasagawa, Takao Fujita, Kazuhiro Ishida, Shigeyuki Uchida, Shinichi Eisaki, Hiroshi Hussain, Zahid Devereaux, Thomas P. Shen, Zhi-Xun TI Direct spectroscopic evidence for phase competition between the pseudogap and superconductivity in Bi2Sr2CaCu2O8+delta SO NATURE MATERIALS LA English DT Article ID T-C SUPERCONDUCTOR; HIGH-TEMPERATURE SUPERCONDUCTOR; ORDER; STATE; BI2SR2-XLAXCUO6+DELTA; TRANSITIONS; SYMMETRY; DENSITY AB In the high-temperature (T-c) cuprate superconductors, a growing body of evidence suggests that the pseudogap phase(1), existing below the pseudogap temperature T*, is characterized by some broken electronic symmetries distinct from those associated with superconductivity(2-21). In particular, recent scattering experiments have suggested that charge ordering competes with superconductivity(18-21). However, no direct link of an interplay between the two phases has been identified from the important low-energy excitations. Here, we report an antagonistic singularity at T-c in the spectral weight of Bi2Sr2CaCu2O8+delta as compelling evidence for phase competition, which persists up to a high hole concentration p similar to 0.22. Comparison with theoretical calculations confirms that the singularity is a signature of competition between the order parameters for the pseudogap and superconductivity. The observation of the spectroscopic singularity at finite temperatures over a wide doping range provides new insights into the nature of the competitive interplay between the two orders and the complex phase diagram near the pseudogap critical point. C1 [Hashimoto, Makoto; Moore, Robert G.; Lu, Donghui] SLAC Natl Accelerator Lab, Stanford Synchrotron Radiat Lightsource, Menlo Pk, CA 94025 USA. [Nowadnick, Elizabeth A.; He, Rui-Hua; Vishik, Inna M.; Moritz, Brian; He, Yu; Tanaka, Kiyohisa; Moore, Robert G.; Devereaux, Thomas P.; Shen, Zhi-Xun] SLAC Natl Accelerator Lab, Stanford Inst Mat & Energy Sci, Menlo Pk, CA 94025 USA. [Nowadnick, Elizabeth A.; He, Rui-Hua; Vishik, Inna M.; He, Yu; Tanaka, Kiyohisa; Devereaux, Thomas P.; Shen, Zhi-Xun] Stanford Univ, Geballe Lab Adv Mat, Stanford, CA 94305 USA. [Nowadnick, Elizabeth A.; He, Rui-Hua; Vishik, Inna M.; He, Yu; Tanaka, Kiyohisa; Shen, Zhi-Xun] Stanford Univ, Dept Phys, Stanford, CA 94305 USA. [Nowadnick, Elizabeth A.; He, Rui-Hua; Vishik, Inna M.; He, Yu; Tanaka, Kiyohisa; Shen, Zhi-Xun] Stanford Univ, Dept Appl Phys, Stanford, CA 94305 USA. [He, Rui-Hua; Hussain, Zahid] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. [Moritz, Brian] Univ N Dakota, Dept Phys & Astrophys, Grand Forks, ND 58202 USA. [Tanaka, Kiyohisa] Osaka Univ, Dept Phys, Toyonaka, Osaka 5600043, Japan. [Yoshida, Yoshiyuki; Ishikado, Motoyuki; Eisaki, Hiroshi] Natl Inst Adv Ind Sci & Technol, Tsukuba, Ibaraki 3058568, Japan. [Ishikado, Motoyuki] Japan Atom Energy Agcy, Quantum Beam Sci Directorate, Tokai, Ibaraki 3191195, Japan. [Sasagawa, Takao] Tokyo Inst Technol, Mat & Struct Lab, Yokohama, Kanagawa 2268503, Japan. [Fujita, Kazuhiro; Ishida, Shigeyuki; Uchida, Shinichi] Univ Tokyo, Dept Phys, Bunkyo Ku, Tokyo 1130033, Japan. [Fujita, Kazuhiro] Cornell Univ, Dept Phys, Atom & Solid State Phys Lab, Ithaca, NY 14853 USA. RP Hashimoto, M (reprint author), SLAC Natl Accelerator Lab, Stanford Synchrotron Radiat Lightsource, Menlo Pk, CA 94025 USA. EM mhashi@slac.stanford.edu; zxshen@stanford.edu RI Sasagawa, Takao/E-6666-2014; Moritz, Brian/D-7505-2015 OI Sasagawa, Takao/0000-0003-0149-6696; Moritz, Brian/0000-0002-3747-8484 FU DOE Office of Basic Energy Sciences, Materials Sciences and Engineering Division [DE-AC02-76SF00515] FX We thank S. Kivelson, H. Yao, A. Millis, D. Scalapino, P. Hirshfeld, B. Markiewicz, D-H. Lee, L. Yu, A. Fujimori and N. Nagaosa for fruitful discussions. ARPES experiments were performed at the Stanford Synchrotron Radiation Lightsource, operated by the Office of Basic Energy Science, US DOE. This work is supported by DOE Office of Basic Energy Sciences, Materials Sciences and Engineering Division, under Contract DE-AC02-76SF00515. NR 36 TC 26 Z9 26 U1 12 U2 95 PU NATURE PUBLISHING GROUP PI LONDON PA MACMILLAN BUILDING, 4 CRINAN ST, LONDON N1 9XW, ENGLAND SN 1476-1122 EI 1476-4660 J9 NAT MATER JI Nat. Mater. PD JAN PY 2015 VL 14 IS 1 BP 37 EP 42 DI 10.1038/NMAT4116 PG 6 WC Chemistry, Physical; Materials Science, Multidisciplinary; Physics, Applied; Physics, Condensed Matter SC Chemistry; Materials Science; Physics GA AW7FM UT WOS:000346430100011 PM 25362356 ER PT J AU Xu, RJ Liu, S Grinberg, I Karthik, J Damodaran, AR Rappe, AM Martin, LW AF Xu, Ruijuan Liu, Shi Grinberg, Ilya Karthik, J. Damodaran, Anoop R. Rappe, Andrew M. Martin, Lane W. TI Ferroelectric polarization reversal via successive ferroelastic transitions SO NATURE MATERIALS LA English DT Article ID ZIRCONATE-TITANATE FILMS; ATOMIC-LEVEL SIMULATION; THIN-FILMS; DOMAIN-WALL; OXIDES; MECHANISMS; DYNAMICS AB Switchable polarization makes ferroelectrics a critical component in memories, actuators and electro-optic devices, and potential candidates for nanoelectronics. Although many studies of ferroelectric switching have been undertaken, much remains to be understood about switching in complex domain structures and in devices. In this work, a combination of thin-film epitaxy, macro- and nanoscale property and switching characterization, and molecular dynamics simulations are used to elucidate the nature of switching in PbZr0.2Ti0.8O3 thin films. Differences are demonstrated between (001)-/(101)- and (111)- oriented films, with the latter exhibiting complex, nanotwinned ferroelectric domain structures with high densities of 90 degrees domain walls and considerably broadened switching characteristics. Molecular dynamics simulations predict both 180 degrees (for (001)-/(101)- oriented films) and 90 degrees multi-step switching (for (111)- oriented films) and these processes are subsequently observed in stroboscopic piezoresponse force microscopy. These results have implications for our understanding of ferroelectric switching and offer opportunities to change domain reversal speed. C1 [Xu, Ruijuan; Karthik, J.; Damodaran, Anoop R.; Martin, Lane W.] Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA. [Liu, Shi; Grinberg, Ilya; Rappe, Andrew M.] Univ Penn, Dept Chem, Makineni Theoret Labs, Philadelphia, PA 19104 USA. [Martin, Lane W.] Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. RP Martin, LW (reprint author), Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA. EM lwmartin@berkeley.edu RI LIU, SHI/I-5494-2013; Martin, Lane/H-2409-2011 OI LIU, SHI/0000-0002-8488-4848; Martin, Lane/0000-0003-1889-2513 FU National Science Foundation; Nanoelectronics Research Initiative [DMR-1124696]; US DOE [DE-FG02-07ER46431]; National Science Foundation [DMR-1451219]; Army Research Office [W911NF-14-1-0104]; Office of Naval Research [N00014-12-1-1033] FX R.X. and S.L. acknowledge support from the National Science Foundation and the Nanoelectronics Research Initiative under grant DMR-1124696. I.G. acknowledges support from the US DOE under grant DE-FG02-07ER46431. J.K. acknowledges support from the National Science Foundation under grant DMR-1451219. A.R.D. and L.W.M. acknowledge support from the Army Research Office under grant W911NF-14-1-0104. A.M.R. acknowledges support from the Office of Naval Research under grant N00014-12-1-1033. The authors acknowledge computational support from the High-Performance Computing Modernization Office of the Department of Defense, and from the National Energy Research Scientific, Computing Center of the Department of Energy. NR 46 TC 49 Z9 49 U1 31 U2 199 PU NATURE PUBLISHING GROUP PI LONDON PA MACMILLAN BUILDING, 4 CRINAN ST, LONDON N1 9XW, ENGLAND SN 1476-1122 EI 1476-4660 J9 NAT MATER JI Nat. Mater. PD JAN PY 2015 VL 14 IS 1 BP 79 EP 86 DI 10.1038/NMAT4119 PG 8 WC Chemistry, Physical; Materials Science, Multidisciplinary; Physics, Applied; Physics, Condensed Matter SC Chemistry; Materials Science; Physics GA AW7FM UT WOS:000346430100018 PM 25344784 ER PT J AU Engel, M Damasceno, PF Phillips, CL Glotzer, SC AF Engel, Michael Damasceno, Pablo F. Phillips, Carolyn L. Glotzer, Sharon C. TI Computational self-assembly of a one-component icosahedral quasicrystal SO NATURE MATERIALS LA English DT Article ID NANOPARTICLE SUPERLATTICES; METALLIC PHASE; GROWTH; ORDER; SIMULATIONS AB Icosahedral quasicrystals (IQCs) are a form of matter that is ordered but not periodic in any direction. All reported IQCs are intermetallic compounds and either of face-centred-icosahedral or primitive-icosahedral type, and the positions of their atoms have been resolved from diffraction data. However, unlike axially symmetric quasicrystals, IQCs have not been observed in non-atomic (that is, micellar or nanoparticle) systems, where real-space information would be directly available. Here, we show that an IQC can be assembled by means of molecular dynamics simulations from a one-component system of particles interacting via a tunable, isotropic pair potential extending only to the third-neighbour shell. The IQC is body-centred, self-assembles from a fluid phase, and in parameter space neighbours clathrates and other tetrahedrally bonded crystals. Our findings elucidate the structure and dynamics of the IQC, and suggest routes to search for it and design it in soft matter and nanoscale systems. C1 [Engel, Michael; Glotzer, Sharon C.] Univ Michigan, Dept Chem Engn, Ann Arbor, MI 48109 USA. [Damasceno, Pablo F.; Glotzer, Sharon C.] Univ Michigan, Appl Phys Program, Ann Arbor, MI 48109 USA. [Phillips, Carolyn L.] Argonne Natl Lab, Argonne, IL 60439 USA. [Glotzer, Sharon C.] Univ Michigan, Dept Mat Sci & Engn, Ann Arbor, MI 48109 USA. RP Engel, M (reprint author), Univ Michigan, Dept Chem Engn, Ann Arbor, MI 48109 USA. EM engelmm@umich.edu; sglotzer@umich.edu RI Engel, Michael/G-1778-2010 OI Engel, Michael/0000-0002-7031-3825 FU DOD/ASD(RE) [N00244-09-1-0062]; US Army Research Office [W911NF-10-1-0518]; University of Michigan CEMRI for Photonics and Multiscale Nanomaterials (C-PHOM) - National Science Foundation Materials Research Science and Engineering Center [DMR 1120923]; Simons Foundation; Office of Science of the US Department of Energy [DE-AC02-06CH11357]; Office of the Director through Argonne National Laboratory FX This material is based on work supported in part by the DOD/ASD(R&E) under Award No. N00244-09-1-0062 (M.E. and S.C.G.), by the US Army Research Office under Grant Award No. W911NF-10-1-0518 (S.C.G.), by the University of Michigan CEMRI for Photonics and Multiscale Nanomaterials (C-PHOM) funded by the National Science Foundation Materials Research Science and Engineering Center program DMR 1120923 (P.F.D.), and by a Simons Investigator award from the Simons Foundation to S.C.G. Simulations were performed on a GPU cluster managed by the University of Michigan's Center for advanced computing and also on resources of the Argonne Leadership Computing Facility at Argonne National Laboratory, which is supported by the Office of Science of the US Department of Energy under contract DE-AC02-06CH11357 (C.L.P.). C.L.P. was funded by the Office of the Director through the Named Postdoctoral Fellowship Program (Aneesur Rahman Postdoctoral Fellowship), Argonne National Laboratory. Any opinions, findings, and conclusions or recommendations expressed in this publication are those of the authors and do not necessarily reflect the views of the DOD/ASD(R&E). NR 52 TC 30 Z9 31 U1 8 U2 90 PU NATURE PUBLISHING GROUP PI LONDON PA MACMILLAN BUILDING, 4 CRINAN ST, LONDON N1 9XW, ENGLAND SN 1476-1122 EI 1476-4660 J9 NAT MATER JI Nat. Mater. PD JAN PY 2015 VL 14 IS 1 BP 109 EP 116 DI 10.1038/NMAT4152 PG 8 WC Chemistry, Physical; Materials Science, Multidisciplinary; Physics, Applied; Physics, Condensed Matter SC Chemistry; Materials Science; Physics GA AW7FM UT WOS:000346430100022 PM 25485986 ER PT J AU Cappa, JJ Yetter, C Fakra, S Cappa, PJ DeTar, R Landes, C Pilon-Smits, EAH Simmons, MP AF Cappa, Jennifer J. Yetter, Crystal Fakra, Sirine Cappa, Patrick J. DeTar, Rachael Landes, Corbett Pilon-Smits, Elizabeth A. H. Simmons, Mark P. TI Evolution of selenium hyperaccumulation in Stanleya (Brassicaceae) as inferred from phylogeny, physiology and X-ray microprobe analysis SO NEW PHYTOLOGIST LA English DT Article DE ancestral reconstruction; evolution; hyperaccumulation; phylogenetics; selenium (Se); Stanleya; X-ray microprobe analysis ID LOCATING SELENIFEROUS AREAS; WESTERN UNITED-STATES; THLASPI-CAERULESCENS BRASSICACEAE; PRAIRIE DOG HERBIVORY; INDICATOR PLANTS; NICKEL HYPERACCUMULATION; SULFUR ACCUMULATION; MAXIMUM-LIKELIHOOD; PROTECTS PLANTS; DNA-SEQUENCES AB Past studies have identified herbivory as a likely selection pressure for the evolution of hyperaccumulation, but few have tested the origin(s) of hyperaccumulation in a phylogenetic context. We focused on the evolutionary history of selenium (Se) hyperaccumulation in Stanleya (Brassicaceae). Multiple accessions were collected for all Stanleya taxa and two outgroup species. We sequenced four nuclear gene regions and performed a phylogenetic analysis. Ancestral reconstruction was used to predict the states for Se-related traits in a parsimony framework. Furthermore, we tested the taxa for Se localization and speciation using X-ray microprobe analyses. True hyperaccumulation was found in three taxa within the S.pinnata/bipinnata clade. Tolerance to hyperaccumulator Se concentrations was found in several taxa across the phylogeny, including the hyperaccumulators. X-ray analysis revealed two distinct patterns of leaf Se localization across the genus: marginal and vascular. All taxa accumulated predominantly (65-96%) organic Se with the C-Se-C configuration. These results give insight into the evolution of Se hyperaccumulation in Stanleya and suggest that Se tolerance and the capacity to produce organic Se are likely prerequisites for Se hyperaccumulation in Stanleya. C1 [Cappa, Jennifer J.; Yetter, Crystal; DeTar, Rachael; Pilon-Smits, Elizabeth A. H.; Simmons, Mark P.] Colorado State Univ, Dept Biol, Ft Collins, CO 80523 USA. [Fakra, Sirine] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. [Cappa, Patrick J.] Univ Colorado, Inst Arctic & Alpine Res, Boulder, CO 80309 USA. [Landes, Corbett] Prescott Coll, Prescott, AZ 86303 USA. RP Pilon-Smits, EAH (reprint author), Colorado State Univ, Dept Biol, Ft Collins, CO 80523 USA. EM epsmits@lamar.colostate.edu RI Simmons, Mark/F-7157-2013 OI Simmons, Mark/0000-0003-3896-4633 FU Doctoral Dissertation Improvement Grant [DEB-1210752]; American Society for Plant Taxonomists FX The authors thank Ihsan Al-Shehbaz (MO) for helpful discussion regarding the morphological characters, phylogeny, and for donating leaf material. The authors also thank Richard Halse (OSU), and Ron Hartman (RM) for generously donating the necessary leaf material. This work was funded by Doctoral Dissertation Improvement Grant # DEB-1210752 to J.J.C., and the American Society for Plant Taxonomists. NR 85 TC 6 Z9 6 U1 4 U2 42 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0028-646X EI 1469-8137 J9 NEW PHYTOL JI New Phytol. PD JAN PY 2015 VL 205 IS 2 BP 583 EP 595 DI 10.1111/nph.13071 PG 13 WC Plant Sciences SC Plant Sciences GA AW9NO UT WOS:000346584600017 PM 25262627 ER PT J AU Wiedemeier, DB Abiven, S Hockaday, WC Keiluweit, M Kleber, M Masiello, CA McBeath, AV Nico, PS Pyle, LA Schneider, MPW Smernik, RJ Wiesenberg, GLB Schmidt, MWI AF Wiedemeier, Daniel B. Abiven, Samuel Hockaday, William C. Keiluweit, Marco Kleber, Markus Masiello, Caroline A. McBeath, Anna V. Nico, Peter S. Pyle, Lacey A. Schneider, Maximilian P. W. Smernik, Ronald J. Wiesenberg, Guido L. B. Schmidt, Michael W. I. TI Aromaticity and degree of aromatic condensation of char SO ORGANIC GEOCHEMISTRY LA English DT Article DE Pyrogenic organic matter; Char; Aromaticity; Aromatic condensation; Pyrolysis; Stability; Heat treatment temperature; Biochar ID PAST FIRE REGIMES; BLACK CARBON; PYROLYSIS TEMPERATURE; CHEMICAL-COMPOSITION; CURRENT KNOWLEDGE; PYROGENIC CARBON; ORGANIC TRACERS; BIOCHAR; WOOD; BIOMASS AB The aromatic carbon structure is a defining property of chars and is often expressed with the help of two concepts: (i) aromaticity and (ii) degree of aromatic condensation. The varying extent of these two features is assumed to largely determine the relatively high persistence of charred material in the environment and is thus of interest for, e.g., biochar characterization or carbon cycle studies. Consequently, a variety of methods has been used to assess the aromatic structure of chars, which has led to interesting insights but has complicated the comparison of data acquired with different methods. We therefore used a suite of seven methods (elemental analysis, MIR spectroscopy, NEXAFS spectroscopy, C-13 NMR spectroscopy, BPCA analysis, lipid analysis and helium pycnometry) and compared 13 measurements from them using a diverse sample set of 38 laboratory chars. Our results demonstrate that most of the measurements could be categorized either into those which assess aromaticity or those which assess the degree of aromatic condensation. A variety of measurements, including relatively inexpensive and simple ones, reproducibly captured the two aromatic features in question, and data from different methods could therefore be compared. Moreover, general patterns between the two aromatic features and the pyrolysis conditions were revealed, supporting reconstruction of the highest heat treatment temperature (HTT) of char. (C) 2014 Elsevier Ltd. All rights reserved. C1 [Wiedemeier, Daniel B.; Abiven, Samuel; Schneider, Maximilian P. W.; Wiesenberg, Guido L. B.; Schmidt, Michael W. I.] Univ Zurich, Dept Geog, CH-8057 Zurich, Switzerland. [Hockaday, William C.] Baylor Univ, Dept Geol, Waco, TX 76798 USA. [Keiluweit, Marco; Kleber, Markus] Oregon State Univ, Dept Crop & Soil Sci, Corvallis, OR 97331 USA. [Kleber, Markus] Inst Soil Landscape Res, Leibniz Ctr Agr Landscape Res ZALF, D-15374 Muncheberg, Germany. [Masiello, Caroline A.; Pyle, Lacey A.] Rice Univ, Dept Earth Sci, Houston, TX 77005 USA. [McBeath, Anna V.; Smernik, Ronald J.] Univ Adelaide, Sch Agr Food & Wine, Adelaide, SA 5064, Australia. [Nico, Peter S.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, Berkeley, CA 94720 USA. RP Wiedemeier, DB (reprint author), Univ Zurich, Dept Geog, CH-8057 Zurich, Switzerland. EM daniel.wiedemeier@geo.uzh.ch RI Wiesenberg, Guido/A-3883-2009; Nico, Peter/F-6997-2010; Masiello, Caroline/A-2653-2011; Pyle, Lacey/I-2981-2015; McBeath, Anna/E-3548-2012; Schmidt, Michael W. I./G-5186-2012; OI Wiesenberg, Guido/0000-0003-2738-5775; Nico, Peter/0000-0002-4180-9397; Abiven, Samuel/0000-0002-5663-0912; Masiello, Caroline/0000-0003-2102-6229; Pyle, Lacey/0000-0001-5928-8609; McBeath, Anna/0000-0003-1608-8150; Hockaday, William/0000-0002-0501-0393; Schmidt, Michael W. I./0000-0002-7227-0646; Smernik, Ronald/0000-0001-6033-5855 FU U.S. Department of Energy [DE-AC02-05CH11231]; NSF [EAR-0911685] FX Support for M.W.I.S. was also provided by the U.S. Department of Energy (Contract No. DE-AC02-05CH11231). B.H. Meier (Laboratory of Physical Chemistry ETH) made available NMR instruments. C.A.M acknowledges support from NSF EAR-0911685. We thank S. Derenne and an anonymous reviewer for providing constructive comments that improved the manuscript. NR 58 TC 30 Z9 30 U1 12 U2 107 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0146-6380 J9 ORG GEOCHEM JI Org. Geochem. PD JAN PY 2015 VL 78 BP 135 EP 143 DI 10.1016/j.orggeochem.2014.10.002 PG 9 WC Geochemistry & Geophysics SC Geochemistry & Geophysics GA AW6OX UT WOS:000346389700013 ER PT J AU Erickson, DJ Sulzberger, B Zepp, RG Austin, AT AF Erickson, David J., III Sulzberger, Barbara Zepp, Richard G. Austin, Amy T. TI Effects of stratospheric ozone depletion, solar UV radiation, and climate change on biogeochemical cycling: interactions and feedbacks SO PHOTOCHEMICAL & PHOTOBIOLOGICAL SCIENCES LA English DT Review ID DISSOLVED ORGANIC-MATTER; PLANT LITTER DECOMPOSITION; CARBON-DIOXIDE UPTAKE; ARCTIC SEA-ICE; MARINE-PHYTOPLANKTON; OCEAN ACIDIFICATION; GREENHOUSE GASES; ATMOSPHERIC CO2; TIPPING POINTS; SURFACE WATERS AB Climate change modulates the effects of solar UV radiation on biogeochemical cycles in terrestrial and aquatic ecosystems, particularly for carbon cycling, resulting in UV-mediated positive or negative feedbacks on climate. Possible positive feedbacks discussed in this assessment include: (i) enhanced UV-induced mineralisation of above ground litter due to aridification; (ii) enhanced UV-induced mineralisation of photoreactive dissolved organic matter (DOM) in aquatic ecosystems due to changes in continental runoff and ice melting; (iii) reduced efficiency of the biological pump due to UV-induced bleaching of coloured dissolved organic matter (CDOM) in stratified aquatic ecosystems, where CDOM protects phytoplankton from the damaging solar UV-B radiation. Mineralisation of organic matter results in the production and release of CO2, whereas the biological pump is the main biological process for CO2 removal by aquatic ecosystems. This paper also assesses the interactive effects of solar UV radiation and climate change on the biogeochemical cycling of aerosols and trace gases other than CO2, as well as of chemical and biological contaminants. Interacting effects of solar UV radiation and climate change on biogeochemical cycles are particularly pronounced at terrestrial-aquatic interfaces. C1 [Erickson, David J., III] Oak Ridge Natl Lab, Comp Earth Sci Grp, Div Math & Comp Sci, Oak Ridge, TN 37831 USA. [Sulzberger, Barbara] Eawag Swiss Fed Inst Aquat Sci & Technol, CH-8600 Dubendorf, Switzerland. [Zepp, Richard G.] US EPA, Athens, GA 30605 USA. [Austin, Amy T.] Univ Buenos Aires, Inst Invest Fisiol & Ecol Vinculadas Agr IFEVA, Buenos Aires, DF, Argentina. [Austin, Amy T.] Univ Buenos Aires, CONICET, Buenos Aires, DF, Argentina. RP Erickson, DJ (reprint author), Oak Ridge Natl Lab, Comp Earth Sci Grp, Div Math & Comp Sci, POB 2008,MS 6016, Oak Ridge, TN 37831 USA. EM d.j.erickson@tds.net OI Austin, Amy/0000-0002-7468-5861 FU U.S. Global Change Research Program; Oak Ridge National Laboratory; Office of Science of the U.S. Department of Energy [DE-AC05-00OR22725]; Eawag: Swiss Federal Institute of Aquatic Science and Technology; National Exposure Research Laboratory, Ecosystems Research Division, U.S. Environmental Protection Agency; National Agency of Science and Technology of Argentina (ANPCyT) FX D. E. was supported by the U.S. Global Change Research Program and by the Oak Ridge National Laboratory, which is supported by the Office of Science of the U.S. Department of Energy under Contract Number DE-AC05-00OR22725. B. S. was supported by Eawag: Swiss Federal Institute of Aquatic Science and Technology. R. Z. was supported by the National Exposure Research Laboratory, Ecosystems Research Division, U.S. Environmental Protection Agency, and A. A. was supported by grants from the National Agency of Science and Technology of Argentina (ANPCyT). NR 251 TC 16 Z9 16 U1 10 U2 94 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1474-905X EI 1474-9092 J9 PHOTOCH PHOTOBIO SCI JI Photochem. Photobiol. Sci. PY 2015 VL 14 IS 1 BP 127 EP 148 DI 10.1039/c4pp90036g PG 22 WC Biochemistry & Molecular Biology; Biophysics; Chemistry, Physical SC Biochemistry & Molecular Biology; Biophysics; Chemistry GA AW9HC UT WOS:000346567000008 PM 25380348 ER PT J AU Yoon, HJ Xu, AR Sterbinsky, GE Arena, DA Wang, ZY Stephens, PW Meng, YS Carroll, KJ AF Yoon, Hyojung Xu, Aoran Sterbinsky, George E. Arena, Dario A. Wang, Ziying Stephens, Peter W. Meng, Ying Shirley Carroll, Kyler J. TI In situ non-aqueous nucleation and growth of next generation rare-earth-free permanent magnets SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID POLYOL PROCESS; FERROMAGNETIC PARTICLES; PHASE-CHANGE; NANOPARTICLES; PHOTOREDUCTION; MECHANISM; KINETICS AB Using a controllable wet chemical approach, the polyol process, we developed a cobalt carbide nanomagnet consisting of an assembly of Co2C and Co3C nanoparticles as an alternative to rare earth permanent magnets (PMs). The thermodynamically stable mixed phase cobalt carbide nanoparticles are shown to be acicular in morphology. Their exchange-coupled magnetic interaction possessing high maximum energy product of 20.7 kJ m(-3) and room temperature coercivity (2.9 kOe) has been confirmed through vibrating sample magnetometer (VSM) and first order reversal curves (FORCs). These metastable carbide nanoparticles offer improved magnetic properties compared to their pure bulk form. An understanding of the formation mechanism, using in situ time-resolved X-ray spectroscopy (TR-XAS), and the correlation between phase contributions to the properties are described in detail. Our strategy presents a controllable route to preparing the cobalt carbide nanomagnets, which could be potentially useful in permanent magnet clean energy applications. Additionally, the in situ apparatus offers a promising way to directly explore the effects of reaction variables for high-temperature wet chemical reactions. C1 [Yoon, Hyojung; Xu, Aoran; Wang, Ziying; Meng, Ying Shirley; Carroll, Kyler J.] Univ Calif San Diego, Dept NanoEngn, La Jolla, CA 92093 USA. [Yoon, Hyojung; Meng, Ying Shirley] Univ Calif San Diego, Mat Sci & Engn Program, La Jolla, CA 92093 USA. [Sterbinsky, George E.; Arena, Dario A.] Brookhaven Natl Lab, Natl Synchrotron Light Source, Upton, NY 11973 USA. [Stephens, Peter W.] SUNY Stony Brook, Dept Phys & Astron, Stony Brook, NY 11794 USA. [Carroll, Kyler J.] MIT, Cambridge, MA 01239 USA. RP Meng, YS (reprint author), Univ Calif San Diego, Dept NanoEngn, La Jolla, CA 92093 USA. EM shmeng@ucsd.edu; kcarroll@mit.edu FU U. S. Department of Energy, Office of Basic Energy Science [DE-AC02-98CH10886]; U.S. Department of Energy Advanced Research Project Agency - Energy (ARPA-E) [DE-AR0000192] FX H. Yoon and K. Carroll acknowledge S. Khalid for technical assistance at the National Synchrotron Light Source and for the use of beamline X18B, where all the in situ measurements were taken. The National Synchrotron Light Source, Brookhaven National Laboratory, was supported by the U. S. Department of Energy, Office of Basic Energy Sciences, under Contract No. DE-AC02-98CH10886. We thank W. Nielson for his guidance in the design of the in situ reactor. We thank E. Carpenter and Z. Huba for their valuable discussions on the nucleation and growth of magnetic nanoparticles. We also thank Y. Zhu and S. Pollard for their assistance on collection of HR-TEM data. We also acknowledges the support from the U.S. Department of Energy Advanced Research Project Agency - Energy (ARPA-E) under the contract # DE-AR0000192. NR 39 TC 3 Z9 3 U1 4 U2 41 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2015 VL 17 IS 2 BP 1070 EP 1076 DI 10.1039/c4cp04451g PG 7 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AW4FH UT WOS:000346236000040 PM 25412691 ER PT J AU Feng, X Yang, ZZ Tang, DC Kong, QY Gu, L Wang, ZX Chen, LQ AF Feng, Xin Yang, Zhenzhong Tang, Daichun Kong, Qingyu Gu, Lin Wang, Zhaoxiang Chen, Liquan TI Performance improvement of Li-rich layer-structured Li1.2Mn0.54Ni0.13Co0.13O2 by integration with spinel LiNi0.5Mn1.5O4 SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID LITHIUM-ION BATTERIES; CATHODE MATERIALS; ELECTROCHEMICAL PROPERTIES; PHASE-TRANSFORMATION; SURFACE MODIFICATION; ELECTRON-MICROSCOPY; COMPOSITE CATHODE; OXIDE ELECTRODES; CAPACITY FADE; OXYGEN LOSS AB Li-rich layered Li1+xMnyM1-x-yO2 (or denoted xLi(2)MnO(3)center dot(1-x)LiMO2, M = Ni, Co, Mn, etc.) are promising cathode materials for high energy-density Li-ion batteries. However, their commercial applications suffer from problems such as a drop in the capacity and discharge voltage during cycling. In this work, the cycling performance of a layered oxide Li1.2Ni0.13Co0.13Mn0.54O2 is improved by integration with spinel LiNi0.5Mn1.5O4 to obtain a layered-spinel composite. Characterization by powder X-ray diffraction (XRD), high resolution transmission electron microscopy (HRTEM) as well as cyclic voltammetry (CV) indicates that delayed degradation of layered Li2MnO3 and the suppressed growth of LiMn2O4-like spinel are responsible for the performance improvement. C1 [Feng, Xin; Yang, Zhenzhong; Tang, Daichun; Gu, Lin; Wang, Zhaoxiang; Chen, Liquan] Chinese Acad Sci, Inst Phys, Beijing 100190, Peoples R China. [Kong, Qingyu] Argonne Natl Lab, Xray Sci Div, Argonne, IL 60439 USA. RP Wang, ZX (reprint author), Chinese Acad Sci, Inst Phys, POB 603, Beijing 100190, Peoples R China. EM zxwang@aphy.iphy.ac.cn RI Gu, Lin/D-9631-2011; Yang, Zhenzhong/O-2344-2014 OI Gu, Lin/0000-0002-7504-031X; Yang, Zhenzhong/0000-0002-7226-7973 FU National Natural Science Foundation of China (NSFC) [51372268] FX This work was financially supported by the National Natural Science Foundation of China (NSFC No. 51372268). NR 42 TC 24 Z9 24 U1 12 U2 230 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2015 VL 17 IS 2 BP 1257 EP 1264 DI 10.1039/c4cp04087b PG 8 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AW4FH UT WOS:000346236000062 PM 25420544 ER PT J AU Agosta, L Zollo, G Arcangeli, C Buonocore, F Gala, F Celino, M AF Agosta, Lorenzo Zollo, Giuseppe Arcangeli, Caterina Buonocore, Francesco Gala, Fabrizio Celino, Massimo TI Water driven adsorption of amino acids on the (101) anatase TiO2 surface: an ab initio study SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID MOLECULAR-DYNAMICS; OXIDE SURFACES; TITANIUM; FERRITIN; BINDING; METAL; MOTIF AB Arg, Lys and Asp amino acids are known to play a critical role in the adhesion of the RKLPDA engineered peptide on the (101) surface of the titania anatase phase. To understand their contribution to peptide adhesion, we have considered the relevant charge states due to protonation (Arg and Lys) or deprotonation (Asp) occurring in neutral water solution, and studied their adsorption on the (101) anatase TiO2 surface by ab initio total energy calculations based on density functional theory. The adsorption configurations on the hydrated surface are compared to those on the dry surface considering also the presence of the hydration shell around amino acid side-chains. This study explains how water molecules mediate the adsorption of charged amino acids showing that protonated amino acids are chemically adsorbed much more strongly than de-protonated Asp. Moreover it is shown that the polar screening of the hydration shell reduces the adsorption energy of the protonated amino acids to a small extent, thus evidencing that both Arg and Lys strongly adhere on the (101) anatase TiO2 surface in neutral water solution and that they play a major role in the adhesion of the RKLPDA peptide. C1 [Agosta, Lorenzo; Zollo, Giuseppe; Gala, Fabrizio] Univ Roma La Sapienza, Dipartimento Sci Base & Applicate Ingn, Sez Fis, I-00161 Rome, Italy. [Agosta, Lorenzo; Arcangeli, Caterina; Buonocore, Francesco; Celino, Massimo] Univ Roma Tor Vergata, NAST Ctr, Dept Phys, I-00133 Rome, Italy. [Agosta, Lorenzo; Buonocore, Francesco] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN USA. [Arcangeli, Caterina; Buonocore, Francesco; Celino, Massimo] CR Casaccia, ENEA Italian Natl Agcy New Technol Energy & Susta, I-00123 Rome, Italy. RP Zollo, G (reprint author), Univ Roma La Sapienza, Dipartimento Sci Base & Applicate Ingn, Sez Fis, Via A Scarpa 14-16, I-00161 Rome, Italy. EM giuseppe.zollo@uniroma1.it RI Zollo, Giuseppe/N-9816-2016; OI Zollo, Giuseppe/0000-0001-6082-8844; Buonocore, Francesco/0000-0001-5028-4468; Celino, Massimo/0000-0002-9707-991X; Gala, Fabrizio/0000-0002-2172-5815 FU META-Materials Enhancement for Technological Application-Project [PIRSES-GA-2010-269182] FX Computational resources were provided by the Italian National Agency for New Technology, Energy and Sustainable Economic Development (ENEA) under the ENEA-GRID CRESCO project. We warmly acknowledge this institution for contributing to the present article. We thank Dr Simone Giusepponi for his support for the efficient implementation of the AIMD simulations. This work was partly supported by META-Materials Enhancement for Technological Application-Project (FP7-PEOPLE-2010-IRSES-Marie Curie Actions, PIRSES-GA-2010-269182). NR 33 TC 11 Z9 11 U1 5 U2 46 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2015 VL 17 IS 3 BP 1556 EP 1561 DI 10.1039/c4cp03056g PG 6 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AW7XA UT WOS:000346473600003 PM 25434879 ER PT J AU Leung, K AF Leung, Kevin TI Predicting the voltage dependence of interfacial electrochemical processes at lithium-intercalated graphite edge planes SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID ION BATTERIES; MOLECULAR-DYNAMICS; ELECTRON-TRANSFER; DEPOSITION; SURFACE; STABILITY; CHEMISTRY; WATER AB The applied potential governs lithium-intercalation and electrode passivation reactions in lithium ion batteries, but are challenging to calibrate in condensed phase DFT calculations. In this work, the "anode potential'' of charge-neutral lithium-intercalated graphite (LiC6) with oxidized edge planes is computed as a function of Li-content (n(Li)) at edge planes, using ab initio molecular dynamics (AIMD), a previously introduced Li+ transfer free energy method, and the experimental Li+/Li(s) value as reference. The voltage assignments are corroborated using explicit electron transfer from fluoroethylene carbonate radical anion markers. PF6- is shown to decompose electrochemically (i.e., not just thermally) at low potentials imposed by our voltage calibration technique. We demonstrate that excess electrons reside in localized states-in-the-gap in the organic carbonate liquid region, which is not semiconductor-like (band-state-like) as widely assumed in the literature. C1 Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Leung, K (reprint author), Sandia Natl Labs, MS 1415, Albuquerque, NM 87185 USA. EM kleung@sandia.gov FU Nanostructures for Electrical Energy Storage (NEES); U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DESC0001160]; U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX We thank Kevin Zavadil and Jun Cheng for interesting discussions. This work was supported by Nanostructures for Electrical Energy Storage (NEES), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Award Number DESC0001160. Sandia National Laboratories is a multiprogram laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000. NR 36 TC 14 Z9 14 U1 3 U2 60 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2015 VL 17 IS 3 BP 1637 EP 1643 DI 10.1039/c4cp04494k PG 7 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AW7XA UT WOS:000346473600015 PM 25438093 ER PT J AU Watson, Z Keinan, S Kanai, Y AF Watson, Zoe Keinan, Shahar Kanai, Yosuke TI Electronic and optical properties of polypyridylruthenium derivatized polystyrenes: multi-level computational analysis of metallo-polymeric chromophore assemblies SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID ARTIFICIAL PHOTOSYNTHESIS; DYNAMICS; ACID; CHALLENGES; COMPLEXES; TRANSPORT; SOLVENT; CELLS; STATE; WATER AB Great effort is geared toward investigation of new materials for solar energy conversion in recent years. Polymeric chromophore assemblies consisting of [Ru(bpy)(3)] (2+) complexes attached to a polystyrene backbone have gained considerable interest in recent years because of their structural flexibility combined with their ability to efficiently capture solar energy and transport the captured energy in the form of exciton or charges. We employ a combination of computational methods to examine how opto-electronic properties of [Ru(bpy)(3)](2+) complexes are influenced by the polymer dynamics in these polymeric chromophore assemblies. The covalent linker between the polymer and the light-absorbing Ru complex is thought to play an important role in optimizing the assemblies for solar energy conversion and transport. We find that the presence of -CH2- groups in the linker has a significant impact on the Highest Occupied Molecular Orbital (HOMO) and Lowest Unoccupied Molecular Orbital (LUMO) energies of the pendants. Generally speaking, a longer linker leads to higher HOMO energies. Without the presence of -CH2- groups, a mixture of cis and trans amide bond in the covalent linker leads to a bimodal distribution for both HOMO and LUMO energies. Importantly, we find that distributions of orbital energies from individual [Ru(bpy)(3)](2+) pendants have the maximum overlap when there is only one -CH2- group in the linker. Such an isotropic energy distribution is likely to be important for charge transport within the assemblies. We also find that in contrast to the isolated [Ru(bpy)(3)](2+) complex, the HOMO is generally found on the linker rather than on Ru atom. This does not change the character of the metal- to- ligand charge transfer (MLCT) excited states, as these excitations in the pendants do not derive from HOMO/LUMO transitions but rather from HOMO - 2/LUMO transition since HOMO - 2 is located on the Ru atom. C1 [Watson, Zoe; Keinan, Shahar; Kanai, Yosuke] Univ N Carolina, Dept Chem, Chapel Hill, NC 27599 USA. [Kanai, Yosuke] Lawrence Livermore Natl Lab, Condensed Matter & Mat Div, Livermore, CA 27333 USA. RP Keinan, S (reprint author), Univ N Carolina, Dept Chem, Chapel Hill, NC 27599 USA. EM skeinan@gmail.com; ykanai@ad.unc.edu RI Kanai, Yosuke/B-5554-2016 FU U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001011, DE-AC0205CH11231] FX This material is based upon work solely supported as part of the UNC EFRC: Center for Solar Fuels, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Award Number DE-SC0001011. We thank National Energy Research Scientific Computing Center, which is supported by the Office of Science of the U.S. Department of Energy under contract No. DE-AC0205CH11231 for computational resources. NR 27 TC 0 Z9 0 U1 1 U2 10 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2015 VL 17 IS 3 BP 1776 EP 1784 DI 10.1039/c4cp04043k PG 9 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AW7XA UT WOS:000346473600030 PM 25463448 ER PT J AU Bera, PP Peverati, R Head-Gordon, M Lee, TJ AF Bera, Partha P. Peverati, Roberto Head-Gordon, Martin Lee, Timothy J. TI Hydrocarbon growth via ion-molecule reactions: computational studies of the isomers of C4H2+, C6H2+ and C6H4+ and their formation paths from acetylene and its fragments SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID FOCK PERTURBATION-THEORY; ELECTRONIC-TRANSITIONS; INTERSTELLAR-MEDIUM; SPIN ORBITALS; CHEMISTRY; DENSITY; SPECTROSCOPY; ELEMENTS; BENZENE; MATRIX AB We seek insight into the origin of observations made in plasma experiments mimicking interstellar and circumstellar conditions. To this end theory is applied to the low-energy isomers of C4H2+, C6H2+ and C6H4+ and their formation paths from acetylene and its fragments. Ab initio molecular dynamics trajectories are performed to explore which isomers are readily accessible from acetylene and its ion fragments. Structural information at a high level of electronic structure theory [CCSD(T)/cc-pVTZ], as well as information on the vibrational [UMP2] and electronic spectra [omega B97X] of the low-energy isomers is reported. C1 [Bera, Partha P.; Lee, Timothy J.] NASA, Ames Res Ctr, Mountain View, CA 94035 USA. [Bera, Partha P.] Bay Area Environm Res Inst, Petaluma, CA 94952 USA. [Peverati, Roberto; Head-Gordon, Martin] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Peverati, Roberto; Head-Gordon, Martin] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. RP Lee, TJ (reprint author), NASA, Ames Res Ctr, MS 245-1, Mountain View, CA 94035 USA. EM Timothy.J.Lee@nasa.gov RI Lee, Timothy/K-2838-2012; Bera, Partha /K-8677-2012; OI Peverati, Roberto/0000-0001-7774-9923 FU NASA Carbon in the Galaxy consortium [NNH10ZDA001N]; BAER Institute FX The authors gratefully acknowledge financial support from the NASA Carbon in the Galaxy consortium grant NNH10ZDA001N, and PPB acknowledges support from the BAER Institute. PPB and TJL gratefully acknowledge helpful discussions with Dr Cesar Contreras and Dr Farid Salama throughout this project. NR 45 TC 5 Z9 5 U1 3 U2 20 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2015 VL 17 IS 3 BP 1859 EP 1869 DI 10.1039/c4cp04480k PG 11 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AW7XA UT WOS:000346473600039 PM 25474483 ER PT J AU Bock, DC Takeuchi, KJ Marschilok, AC Takeuchi, ES AF Bock, David C. Takeuchi, Kenneth J. Marschilok, Amy C. Takeuchi, Esther S. TI Structural and silver/vanadium ratio effects on silver vanadium phosphorous oxide solution formation kinetics: Impact on battery electrochemistry SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID LITHIUM-ION BATTERIES; LI-ION; CATHODE MATERIAL; DISSOLUTION KINETICS; CAPACITY LOSSES; RELEASE; PERFORMANCE; ELECTRODES; TEMPERATURE; MECHANISMS AB The detailed understanding of non-faradaic parasitic reactions which diminish battery calendar life is essential to the development of effective batteries for use in long life applications. The dissolution of cathode materials including manganese, cobalt and vanadium oxides in battery systems has been identified as a battery failure mechanism, yet detailed dissolution studies including kinetic analysis are absent from the literature. The results presented here provide a framework for the quantitative and kinetic analyses of the dissolution of cathode materials which will aid the broader community in more fully understanding this battery failure mechanism. In this study, the dissolution of silver vanadium oxide, representing the primary battery powering implantable cardioverter defibrillators (ICD), is compared with the dissolution of silver vanadium phosphorous oxide (AgwVxPyOz) materials which were targeted as alternatives to minimize solubility. This study contains the first kinetic analyses of silver and vanadium solution formation from Ag0.48VOPO4 center dot 1.9H(2)O and Ag2VP2O8, in a non-aqueous battery electrolyte. The kinetic results are compared with those of Ag2VO2PO4 and Ag2V4O11 to probe the relationships among crystal structure, stoichiometry, and solubility. For vanadium, significant dissolution was observed for Ag2V4O11 as well as for the phosphate oxide Ag0.49VOPO4 center dot 1.9H(2)O, which may involve structural water or the existence of multiple vanadium oxidation states. Notably, the materials from the SVPO family with the lowest vanadium solubility are Ag2VO2PO4 and Ag2VP2O8. The low concentrations and solution rates coupled with their electrochemical performance make these materials interesting alternatives to Ag2V4O11 for the ICD application. C1 [Bock, David C.; Takeuchi, Kenneth J.; Marschilok, Amy C.; Takeuchi, Esther S.] SUNY Stony Brook, Dept Chem, Stony Brook, NY 11794 USA. [Takeuchi, Kenneth J.; Marschilok, Amy C.; Takeuchi, Esther S.] SUNY Stony Brook, Dept Mat Sci & Engn, Stony Brook, NY 11794 USA. [Takeuchi, Esther S.] Brookhaven Natl Lab, Upton, NY 11973 USA. RP Takeuchi, KJ (reprint author), SUNY Stony Brook, Dept Chem, Stony Brook, NY 11794 USA. EM kenneth.takeuchi.1@stonybrook.edu; amy.marschilok@stonybrook.edu; esther.takeuchi@stonybrook.edu FU Department of Energy, Office of Basic Energy Sciences, Division of Materials Science [DE-SC0002460]; National Institutes of Health from the National Heart, Lung, and Blood Institute [1R01HL093044-01A1] FX The authors acknowledge the financial support for the material preparation and characterization from the Department of Energy, Office of Basic Energy Sciences, Division of Materials Science, DE-SC0002460. The solubility studies were supported by the National Institutes of Health under Grant 1R01HL093044-01A1 from the National Heart, Lung, and Blood Institute. Brookhaven National Laboratory is acknowledged for the SmartLab X-ray Diffractometer. NR 54 TC 8 Z9 8 U1 2 U2 45 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2015 VL 17 IS 3 BP 2034 EP 2042 DI 10.1039/c4cp04819a PG 9 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AW7XA UT WOS:000346473600058 PM 25478865 ER PT J AU Phillips, JL Gnanakaran, S AF Phillips, Joshua L. Gnanakaran, S. TI A data-driven approach to modeling the tripartite structure of multidrug resistance efflux pumps SO PROTEINS-STRUCTURE FUNCTION AND BIOINFORMATICS LA English DT Article DE efflux pump; drug resistance; drug translocation; tripartite structures; geometrical simulations; FRODAN; membrane transporter; MexAB-OprM; AmrAB-OprA; Burkholderia pseudomallei ID GRAM-NEGATIVE BACTERIA; PSEUDOMONAS-AERUGINOSA; CRYSTAL-STRUCTURE; ESCHERICHIA-COLI; OUTER-MEMBRANE; ROTATING MECHANISM; TRANSPORTER ACRB; DRUG-RESISTANCE; PROTEIN; CHANNEL AB Many bacterial pathogens are becoming increasingly resistant to antibiotic treatments, and a detailed understanding of the molecular basis of antibiotic resistance is critical for the development of next-generation approaches for combating bacterial infections. Studies focusing on pathogens have revealed the profile of resistance in these organisms to be due primarily to the presence of multidrug resistance efflux pumps: tripartite protein complexes which span the periplasm bridging the inner and outer membranes of Gram-negative bacteria. An atomic-level resolution tripartite structure remains imperative to advancing our understanding of the molecular mechanisms of pump function using both theoretical and experimental approaches. We develop a fast and consistent method for constructing tripartite structures which leverages existing data-driven models and provide molecular modeling approaches for constructing tripartite structures of multidrug resistance efflux pumps. Our modeling studies reveal that conformational changes in the inner membrane component responsible for drug translocation have limited impact on the conformations of the other pump components, and that two distinct models derived from conflicting experimental data are both consistent with all currently available measurements. Additionally, we investigate putative drug translocation pathways via geometric simulations based on the available crystal structures of the inner membrane pump component, AcrB, bound to two drugs which occupy distinct binding sites: doxorubicin and linezolid. These simulations suggest that smaller drugs may enter the pump through a channel from the cytoplasmic leaflet of the inner membrane, while both smaller and larger drug molecules may enter through a vestibule accessible from the periplasm. Proteins 2015; 83:46-65. (c) 2014 Wiley Periodicals, Inc. C1 [Phillips, Joshua L.; Gnanakaran, S.] Los Alamos Natl Lab, Theoret Biol & Biophys Grp T6, Los Alamos, NM 87545 USA. [Phillips, Joshua L.] Middle Tennessee State Univ, Dept Comp Sci, Murfreesboro, TN 37132 USA. RP Gnanakaran, S (reprint author), Los Alamos Natl Labs, T-6,MS K710, Los Alamos, NM 87545 USA. EM gnana@lanl.gov OI Gnanakaran, S/0000-0002-9368-3044 FU LANL/DOE LDRD [20140121DR]; LANL Institutional Computing and Metropolis Postdoctoral Fellowship; LANL Center for Nonlinear Studies FX Grant sponsor: LANL/DOE LDRD; grant number: 20140121DR; Grant sponsors: LANL Institutional Computing and Metropolis Postdoctoral Fellowship and the LANL Center for Nonlinear Studies (to JLP). NR 40 TC 4 Z9 4 U1 2 U2 15 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0887-3585 EI 1097-0134 J9 PROTEINS JI Proteins PD JAN PY 2015 VL 83 IS 1 BP 46 EP 65 DI 10.1002/prot.24632 PG 20 WC Biochemistry & Molecular Biology; Biophysics SC Biochemistry & Molecular Biology; Biophysics GA AW7WF UT WOS:000346471600004 PM 24957790 ER PT J AU Hu, HY Yuan, W Jia, Z Baker, GL AF Hu, Heyi Yuan, Wen Jia, Zhe Baker, Gregory L. TI Ionic liquid-based random copolymers: a new type of polymer electrolyte with low glass transition temperature SO RSC ADVANCES LA English DT Article ID SENSITIZED SOLAR-CELL; SILICA NANOPARTICLES; CONDUCTION; BRUSH AB A new type of polymer electrolyte has been prepared from the side-chains of ionic liquids (IL) and an analogue of ethylene oxide (EO) directly grafted on a polyethylene oxide backbone. By tuning the two types of monomer composition during polymerization, a series of copolymers with different monomer ratios between IL : EO = 8 : 1 to 1 : 4 have been synthesized. All copolymerized polyionic liquids showed higher ionic conductivity than an IL homopolymer. By choosing a composition with IL : EO = 1 : 1, the corresponding polymer gave the highest conductivity, 1.2 x 10(-4) S cm(-1) at room temperature, compared to 9.3 x 10(-6) S cm(-1) from a homopolymer. We attribute this to one order of magnitude improvement of conductivity from a low glass transition temperature (T-g) below -40 degrees C. C1 [Hu, Heyi; Yuan, Wen; Jia, Zhe; Baker, Gregory L.] Michigan State Univ, Dept Chem, E Lansing, MI 48824 USA. [Yuan, Wen] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. RP Yuan, W (reprint author), Michigan State Univ, Dept Chem, E Lansing, MI 48824 USA. EM yuanwen@msu.edu RI Yuan, Wen/G-7141-2015 OI Yuan, Wen/0000-0002-1812-9588 FU National Science Foundation [DMR-0934568]; MSU Center for Alternative Energy Storage Research and Technology (CAESRT) FX This study was supported financially by the National Science Foundation (DMR-0934568) and the MSU Center for Alternative Energy Storage Research and Technology (CAESRT). W.Y. is also indebted to Dr James McCusker, Dr Keith Promislow and Dr Lawrence Drzal for valuable discussions. NR 20 TC 15 Z9 15 U1 6 U2 50 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2046-2069 J9 RSC ADV JI RSC Adv. PY 2015 VL 5 IS 5 BP 3135 EP 3140 DI 10.1039/c4ra13432j PG 6 WC Chemistry, Multidisciplinary SC Chemistry GA AW6WC UT WOS:000346405200004 ER PT J AU Swenson, TL Jenkins, S Bowen, BP Northen, TR AF Swenson, Tami L. Jenkins, Stefan Bowen, Benjamin P. Northen, Trent R. TI Untargeted soil metabolomics methods for analysis of extractable organic matter SO SOIL BIOLOGY & BIOCHEMISTRY LA English DT Article DE Soil organic matter; Metabolomics; Gas chromatography/mass spectrometry; Fumigation ID CHLOROFORM FUMIGATION-EXTRACTION; MICROBIAL BIOMASS CARBON; MASS-SPECTROMETRY; GAS-CHROMATOGRAPHY; NITROGEN; PLANT; METABOLITES; SORPTION; RELEASE; WATER AB The cycling of soil organic matter (SOM) by microorganisms is a critical component of the global carbon cycle but remains poorly understood. There is an emerging view that much of SOM, and especially the dissolved fraction (DOM), is composed of small molecules of plant and microbial origin resulting from lysed cells and released metabolites. Unfortunately, little is known about the small molecule composition of soils and how these molecules are cycled (by microbes or plants or by adsorption to mineral surfaces). The water-extractable organic matter (WEOM) fraction is of particular interest given that this is presumably the most biologically-accessible component of SOM. Here we describe the development of a simple soil metabolomics workflow and a novel spike recovery approach using C-13 bacterial lysates to assess the types of metabolites remaining in the WEOM fraction. Soil samples were extracted with multiple mass spectrometry-compatible extraction buffers (water, 10 mM K2SO4 or NH4HCO3, 10-100% methanol or isopropanol/methanol/water [3:3:2 v/v/v]) with and without prior chloroform vapor fumigation. Profiling of derivatized extracts was performed using gas chromatography/mass spectrometry (GC/MS) with 55 metabolites identified by comparing fragmentation patterns and retention times with authentic standards. As expected, fumigation, which is thought to lyse microbial cells, significantly increased the range and abundance of metabolites relative to unfumigated samples. To assess the types of microbial metabolites from lysed bacterial cells that remain in the WEOM fraction, an extract was prepared from the soil bacterium Pseudomonas stutzerii RCH2 grown on C-13 acetate. This approach produced highly labeled metabolites that were easily discriminated from the endogenous soil metabolites. Comparing the composition of the fresh bacterial extract with what was recovered following a 15 min incubation with soil revealed that only 27% of the metabolites showed >50% recovery in the WEOM. Many, especially cations (polyamines) and anions, showed <10% recovery. These represent metabolites that may be inaccessible to microbes in this environment and would be most likely to accumulate as SOM presumably due to binding with minerals and negatively-charged clay particles. This study presents a simple untargeted metabolomics workflow for extractable organic matter and an approach to estimate microbial metabolite availability in soils. These methods can be used to further our understanding of SOM and DOM composition and examine the link between metabolic pathways and microbial communities to terrestrial carbon cycling. Published by Elsevier Ltd. C1 [Swenson, Tami L.; Jenkins, Stefan; Bowen, Benjamin P.; Northen, Trent R.] Lawrence Berkeley Natl Lab, Div Life Sci, Berkeley, CA 94720 USA. RP Northen, TR (reprint author), Lawrence Berkeley Natl Lab, Div Life Sci, 1 Cyclotron Rd, Berkeley, CA 94720 USA. EM TRNorthen@lbl.gov OI Northen, Trent/0000-0001-8404-3259 FU U.S. Department of Energy, Office of Science, Biological and Environmental Research, Genomic Science Program, Carbon Cycling Research [DE-SC0010566]; Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231] FX We thank Jill Banfield (University of California, Berkeley) and her lab (especially Susan Spaulding and David Burstein) for assisting in soil collection, Zachary Aanderud (Brigham Young University) for providing essential guidance on soil extraction methodology, Peter Nico (LBNL) for providing critical feedback on this manuscript and Alexandra Walling for preparing and analyzing the authentic standards. This work was funded by the U.S. Department of Energy, Office of Science, Biological and Environmental Research, Genomic Science Program, as part of the Carbon Cycling Research (DE-SC0010566). Lawrence Berkeley National Laboratory is supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. NR 61 TC 4 Z9 4 U1 12 U2 104 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0038-0717 J9 SOIL BIOL BIOCHEM JI Soil Biol. Biochem. PD JAN PY 2015 VL 80 BP 189 EP 198 DI 10.1016/j.soilbio.2014.10.007 PG 10 WC Soil Science SC Agriculture GA AW8YS UT WOS:000346545800022 ER PT J AU Li, CP Engtrakul, C Tenent, RC Wolden, CA AF Li, Chi-Ping Engtrakul, Chaiwat Tenent, Robert C. Wolden, Colin A. TI Scalable synthesis of improved nanocrystalline, mesoporous tungsten oxide films with exceptional electrochromic performance SO SOLAR ENERGY MATERIALS AND SOLAR CELLS LA English DT Article DE Electrochromic; Mesoporous; Sol gel; Templated; Tungsten oxide; Ultrasonic spray deposition ID ULTRASONIC SPRAY DEPOSITION; WO3 THIN-FILMS; BLOCK-COPOLYMER; NANOPARTICLES; NANOSTRUCTURES; DURABILITY; COATINGS; SILICA AB Templated sol gel chemistry provides a versatile approach to introduce order and porosity into nanostructured materials. However conventional evaporation induced self assembly techniques are not easily scaled to produce films with sufficient thickness over large areas at the throughput required by electrochromic windows. Here we demonstrate that the principles of sol gel chemistry may be deployed using ultrasonic spray deposition (USD) for scalable synthesis of nanocrystalline WO3 films with unrivaled electrochromic performance. Systematic manipulation of sol chemistry enabled the production of mesoporous films with high specific surface area ( > 100 m(2)/g), mean pore sizes of similar to 5 nm, and narrow pore size distributions. Film thickness is found to be proportional to the sol concentration and number of spray passes, and various combinations are shown to produce films capable of modulating >98% of incident solar radiation in the visible spectrum (450-900 nm). Elimination of haze enables full transmission in the bleached state, while the broadband coloration is attributed to the exceptionally high charge density ( > 120 mC/cm(2)). The materials have good switching speeds which improve with specific surface area, and the long term durability is promising. (C) 2014 Elsevier B.V. All rights reserved. C1 [Li, Chi-Ping; Wolden, Colin A.] Colorado Sch Mines, Dept Chem & Biol Engn, Golden, CO 80401 USA. [Li, Chi-Ping; Wolden, Colin A.] Colorado Sch Mines, Mat Sci Program, Golden, CO 80401 USA. [Li, Chi-Ping; Engtrakul, Chaiwat; Tenent, Robert C.] Natl Renewable Energy Lab, Golden, CO 80401 USA. RP Wolden, CA (reprint author), Colorado Sch Mines, Dept Chem & Biol Engn, Golden, CO 80401 USA. EM cwolden@mines.edu FU National Science Foundation [DMR-0820518]; Department of Energy [DE-AC36-08GO28308] FX This research was founded by National Science Foundation through award DMR-0820518 and the Department of Energy under subcontract DE-AC36-08GO28308. NR 41 TC 10 Z9 10 U1 6 U2 78 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0927-0248 EI 1879-3398 J9 SOL ENERG MAT SOL C JI Sol. Energy Mater. Sol. Cells PD JAN PY 2015 VL 132 BP 6 EP 14 DI 10.1016/j.solmat.2014.08.014 PG 9 WC Energy & Fuels; Materials Science, Multidisciplinary; Physics, Applied SC Energy & Fuels; Materials Science; Physics GA AW9AE UT WOS:000346549400002 ER PT J AU Jiang, CS Repins, IL Beall, C Moutinho, HR Ramanathan, K Al-Jassim, MM AF Jiang, C. -S. Repins, I. L. Beall, C. Moutinho, H. R. Ramanathan, K. Al-Jassim, M. M. TI Investigation of micro-electrical properties of Cu2ZnSnSe4 thin films using scanning probe microscopy SO SOLAR ENERGY MATERIALS AND SOLAR CELLS LA English DT Article DE CZTSe; Solar cell, thin film; Grain boundary; Scanning Kelvin probe force microscopy; Scanning spreading resistance microscopy ID SOLAR-CELL; FORCE MICROSCOPY; EFFICIENCY; DEPOSITION; CUINSE2; SILICON AB We report on a local potential and resistance mapping of Cu2ZnSnSe4 (CZTSe) films using nm-resolution electrical scanning probe microscopies of scanning Kelvin probe force microscopy and scanning spreading resistance microscopy. We have conducted a comparative study with high-performance Cu-2(In,Ga)Se-2 (CIGSe) film. Both CZTSe and CIGSe were deposited by co-evaporation of elements in vacuum. The results show that the microelectrical properties of the two polycrystalline materials are similar-higher potential and lower resistance on the grain boundaries (GBs) than on grain surfaces-suggesting inverted GB carrier polarity of these films. The consistent GB properties in contrast to the large difference in photovoltaic output of the two materials suggest that factors other than the GBs are responsible for the low photovoltaic output of CZTSe device. (C) 2014 Elsevier B.V. All rights reserved. C1 [Jiang, C. -S.; Repins, I. L.; Beall, C.; Moutinho, H. R.; Ramanathan, K.; Al-Jassim, M. M.] Natl Renewable Energy Lab, Golden, CO 80401 USA. RP Jiang, CS (reprint author), Natl Renewable Energy Lab, Golden, CO 80401 USA. EM chun.shengjiang@nrel.gov RI jiang, chun-sheng/F-7839-2012 FU U.S. Department of Energy [DOE-AC36-08G028308]; National Renewable Energy Laboratory FX The authors thank C. DeHart and J. Carapella at NREL for the assistances in making solar cells samples. This work was supported by the U.S. Department of Energy under Contract no. DOE-AC36-08G028308 with the National Renewable Energy Laboratory. NR 29 TC 10 Z9 10 U1 1 U2 28 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0927-0248 EI 1879-3398 J9 SOL ENERG MAT SOL C JI Sol. Energy Mater. Sol. Cells PD JAN PY 2015 VL 132 BP 342 EP 347 DI 10.1016/j.solmat.2014.08.046 PG 6 WC Energy & Fuels; Materials Science, Multidisciplinary; Physics, Applied SC Energy & Fuels; Materials Science; Physics GA AW9AE UT WOS:000346549400048 ER PT J AU Dupont, SR Voroshazi, E Nordlund, D Dauskardt, RH AF Dupont, Stephanie R. Voroshazi, Eszter Nordlund, Dennis Dauskardt, Reinhold H. TI Morphology and interdiffusion control to improve adhesion and cohesion properties in inverted polymer solar cells SO SOLAR ENERGY MATERIALS AND SOLAR CELLS LA English DT Article DE Adhesion and delamination; Cohesion; Reliability; Polymer solar cells; Annealing; NEXAFS ID X-RAY; HETEROJUNCTION AB The role of pre-electrode deposition annealing on the morphology and the fracture properties of polymer solar cells is discussed. We found an increase in adhesion at the weak P3HT:PCBM/PEDOT:PSS interface with annealing temperature, caused by increased interdiffusion between the organic layers. The formation of micrometer sized PCBM crystallites, which occurs with annealing above the crystallization temperature of PCBM, initially weakened the P3HT:PCBM layer itself. Further annealing improved the cohesion, due to a pull-out toughening mechanism of the growing PCBM clusters. Understanding how the morphology, tuned by annealing, affects the adhesive and cohesive properties in these organic films is essential for the mechanical integrity of OPV devices. (C) 2014 Elsevier B.V. All rights reserved. C1 [Dupont, Stephanie R.; Dauskardt, Reinhold H.] Stanford Univ, Dept Mat Sci & Engn, Stanford, CA 94305 USA. [Voroshazi, Eszter] IMEC VZW, B-3000 Louvain, Belgium. [Nordlund, Dennis] SLAC, Synchrotron Radiat Lightsource, Menlo Pk, CA USA. RP Dauskardt, RH (reprint author), Stanford Univ, Dept Mat Sci & Engn, Stanford, CA 94305 USA. EM dauskardt@stanford.edu RI Nordlund, Dennis/A-8902-2008 OI Nordlund, Dennis/0000-0001-9524-6908 FU Center for Advanced Molecular Photovoltaics (CAMP), King Abdullah University of Science and Technology (KAUST) [KUS-C1-015-21] FX This research was supported by the Center for Advanced Molecular Photovoltaics (CAMP) supported by King Abdullah University of Science and Technology (KAUST) under Award no. KUS-C1-015-21. Portions of this research were carried out at the Stanford Synchrotron Radiation Lightsource, a Directorate of SLAC National Accelerator Laboratory and an Office of Science User Facility operated for the U.S. Department of Energy Office of Science by Stanford University. NR 23 TC 9 Z9 9 U1 3 U2 39 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0927-0248 EI 1879-3398 J9 SOL ENERG MAT SOL C JI Sol. Energy Mater. Sol. Cells PD JAN PY 2015 VL 132 BP 443 EP 449 DI 10.1016/j.solmat.2014.09.013 PG 7 WC Energy & Fuels; Materials Science, Multidisciplinary; Physics, Applied SC Energy & Fuels; Materials Science; Physics GA AW9AE UT WOS:000346549400061 ER PT J AU Burrows, K Fthenakis, V AF Burrows, Keith Fthenakis, Vasilis TI Glass needs for a growing photovoltaics industry SO SOLAR ENERGY MATERIALS AND SOLAR CELLS LA English DT Article DE Photovoltaics; Glass; Forecasts; Economics AB With the projected growth in photovoltaics the demand of glass for the solar industry will far exceed the current supply, and thousands of new float-glass plants will have to be built to meet its needs over the next 20 years. Such expansion will provide an opportunity for the solar industry to obtain products better suited to their needs, such as low-iron glass and borosilicate glass at the lowest possible price. While there are no significant technological hurdles that would prevent the flat glass industry from meeting the solar industry's projected needs, to do so will require advance planning and substantial investments. (C) 2014 Elsevier B.V. All rights reserved. C1 [Burrows, Keith; Fthenakis, Vasilis] Columbia Univ, Ctr Life Cycle Anal, New York, NY 10027 USA. [Fthenakis, Vasilis] Brookhaven Natl Lab, Photovolta Environm Res Ctr, Upton, NY 11973 USA. RP Fthenakis, V (reprint author), Columbia Univ, Ctr Life Cycle Anal, 926 SW Mudd,500 West 120th St, New York, NY 10027 USA. EM vmf5@columbia.edu NR 22 TC 5 Z9 5 U1 1 U2 6 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0927-0248 EI 1879-3398 J9 SOL ENERG MAT SOL C JI Sol. Energy Mater. Sol. Cells PD JAN PY 2015 VL 132 BP 455 EP 459 DI 10.1016/j.solmat.2014.09.028 PG 5 WC Energy & Fuels; Materials Science, Multidisciplinary; Physics, Applied SC Energy & Fuels; Materials Science; Physics GA AW9AE UT WOS:000346549400063 ER PT J AU Welch, AW Zawadzki, PP Lany, S Wolden, CA Zakutayev, A AF Welch, Adam W. Zawadzki, Pawel P. Lany, Stephan Wolden, Cohn A. Zakutayev, Andriy TI Self-regulated growth and tunable properties of CuSbS2 solar absorbers SO SOLAR ENERGY MATERIALS AND SOLAR CELLS LA English DT Article DE Chalcogenide; Earth abundant; CuSbS2; Chalcostibite; Sputter deposition; Antimony; Layered structure; Combinatorial ID OF-THE-ART; THIN-FILMS; ELECTRONIC-STRUCTURE; PHASE-RELATIONS; CELLS; COPPER; SB2S3; SB; TETRAHEDRITE; CU2S-SB2S3 AB Polycrystalline thin film copper chalcogenide solar cells show remarkable efficiencies, and analogous but less-explored semiconducting materials may hold similar promise. With consideration of elemental abundance and process scalability, we explore the potential of the Cu-Sb-S material system for photovoltaic applications. Using a high-throughput combinatorial approach, Cu-Sb-S libraries were synthesized by magnetron co-sputtering of Cu2S and Sb2S3 targets and evaluated by a suite of spatially resolved characterization techniques. The resulting compounds include Cu1.8S (digenite), Cu12Sb4S13 (tetrahedrite), CuSbS2 (chalcostibite), and Sb2S3 (stibnite). Of the two ternary phases synthesized, CuSbS2 was found to have the most potential, however, when deposited at low temperatures its electrical conductivity varied by several orders of magnitude due to the presence of impurities. To address this issue, we developed a self-regulated approach to synthesize stoichiometric CuSbS2 films using excess Sb2S3 vapor at elevated substrate temperatures. Theoretical calculations explain that phase-pure CuSbS2 is expected to be formed over a relatively wide range of temperatures and pressures, bound by the sublimation of Sb2S3 and decomposition of CuSbS2. The carrier concentration of CuSbS2 films produced within this regime was tunable from 10(16)-10(18) cm(-3) through appropriate control of Sb2S3 flux rate and substrate temperature. CuSbS2 displayed a sharp optical absorption onset indicative of a direct transition at 1.5 eV and an absorption coefficient of 10(5) cm(-1) within 0.3 eV of the onset. The results of this study suggest that CuSbS2 holds promise for solar energy conversion due to its tolerant processing window, tunable carrier concentration, solar-matched band gap, and high absorption coefficient. (C) 2014 Elsevier B.V. All rights reserved. C1 [Welch, Adam W.; Zawadzki, Pawel P.; Lany, Stephan; Zakutayev, Andriy] Natl Renewable Energy Lab, Golden, CO 80401 USA. [Welch, Adam W.; Wolden, Cohn A.] Colorado Sch Mines, Golden, CO 80401 USA. RP Welch, AW (reprint author), Natl Renewable Energy Lab, Golden, CO 80401 USA. EM adam.welch@nrel.gov OI Lany, Stephan/0000-0002-8127-8885; Zakutayev, Andriy/0000-0002-3054-5525 FU US Department of Energy, Office of Energy Efficiency and Renewable Energy, "Rapid Development of Earth-Abundant Thin Film Solar Cells" [DE-AC36-08GO28308] FX This work was supported by the US Department of Energy, Office of Energy Efficiency and Renewable Energy, as a part of the "Rapid Development of Earth-Abundant Thin Film Solar Cells" agreement, under contract No. DE-AC36-08GO28308 to NREL. We thank David S. Ginley and William Tumas at NREL for useful strategic discussions. NR 74 TC 28 Z9 28 U1 12 U2 92 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0927-0248 EI 1879-3398 J9 SOL ENERG MAT SOL C JI Sol. Energy Mater. Sol. Cells PD JAN PY 2015 VL 132 BP 499 EP 506 DI 10.1016/j.solmat.2014.09.041 PG 8 WC Energy & Fuels; Materials Science, Multidisciplinary; Physics, Applied SC Energy & Fuels; Materials Science; Physics GA AW9AE UT WOS:000346549400069 ER PT J AU Desai, MS Lee, SW AF Desai, Malav S. Lee, Seung-Wuk TI Protein-based functional nanomaterial design for bioengineering applications SO WILEY INTERDISCIPLINARY REVIEWS-NANOMEDICINE AND NANOBIOTECHNOLOGY LA English DT Review ID RECOMBINANT SPIDER SILK; ELASTIN-LIKE POLYPEPTIDES; TISSUE ENGINEERING APPLICATIONS; INVERSE TEMPERATURE TRANSITION; EXTRACELLULAR-MATRIX PROTEINS; RESILIN-BASED MATERIALS; EPITHELIAL-CELL GROWTH; SPIDROIN 1 SCAFFOLDS; II COLLAGEN GEL; CROSS-LINKING AB In this review article, we describe recent progress in the field of protein-based bionanomaterial design with focus on the four well-characterized proteins: mammalian elastin and collagen, and insect-derived silk and resilin. These proteins are important structural components and understanding their physical and biochemical properties has allowed us to not only replicate them but also create novel smart materials. The smart' properties of a material include its ability to self-assemble, respond to stimuli, and/or promote cell interactions. Such properties can be attributed to unique structural modules from elastin, collagen, silk, and resilin as well as functional modules identified from other proteins directly or using display techniques such as phage display. Thus, the goal of this article is to not only emphasize the types of protein-based peptide modules and their uses but also encourage and inspire the reader to create new toolsets of smart polypeptides to overcome their challenges. WIREs Nanomed Nanobiotechnol 2015, 7:69-97. doi: 10.1002/wnan.1303 For further resources related to this article, please visit the . Conflict of interest: The authors have declared no conflicts of interest for this article. C1 [Desai, Malav S.; Lee, Seung-Wuk] Univ Calif Berkeley, Dept Bioengn, Berkeley, CA 94720 USA. [Desai, Malav S.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA 94720 USA. RP Lee, SW (reprint author), Univ Calif Berkeley, Dept Bioengn, Berkeley, CA 94720 USA. EM leesw@berkeley.edu OI Desai, Malav/0000-0002-4160-6944 FU National Science Foundation Center of Integrated Nanomechanical Systems [EEC-0832819]; NIH ARRA supplement [DE 018360-02] FX This work was supported by National Science Foundation Center of Integrated Nanomechanical Systems (EEC-0832819), and NIH ARRA supplement to an NIDCR R21 grant (DE 018360-02). NR 235 TC 9 Z9 9 U1 10 U2 88 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 1939-5116 EI 1939-0041 J9 WIRES NANOMED NANOBI JI Wiley Interdiscip. Rev.-Nanomed. Nanobiotechnol. PD JAN-FEB PY 2015 VL 7 IS 1 BP 69 EP 97 DI 10.1002/wnan.1303 PG 29 WC Nanoscience & Nanotechnology; Medicine, Research & Experimental SC Science & Technology - Other Topics; Research & Experimental Medicine GA AW4WG UT WOS:000346277700004 PM 25392986 ER PT J AU Cui, WP Liu, R Manna, E Park, JM Fungura, F Shinar, J Shinar, R AF Cui, Weipan Liu, Rui Manna, Eeshita Park, Joong-Mok Fungura, Fadzai Shinar, Joseph Shinar, Ruth TI Oxygen and relative humidity monitoring with films tailored for enhanced photoluminescence SO ANALYTICA CHIMICA ACTA LA English DT Article DE O-2 sensor; Porous sensing films; Photoluminescence enhancement; Light scattering; Relative humidity effect ID RESPONSE CHARACTERISTICS; PHASE-SEPARATION; POLYMER-FILMS; BLEND FILM; SENSORS; LUMINESCENCE; CONVECTION; PORPHYRIN; PHOTODETECTORS; PATTERNS AB Approaches to generate porous or doped sensing films, which significantly enhance the photoluminescence (PL) of oxygen optical sensors, and thus improve the signal-to-noise (S/N) ratio, are presented. Tailored films, which enable monitoring the relative humidity (RH) as well, are also presented. Effective porous structures, in which the O-2-sensitive dye Pt octaethylporphyrin (PtOEP) or the Pd analog PdOEP was embedded, were realized by first generating blend films of polyethylene glycol (PEG) with polystyrene (PS) or with ethyl cellulose (EC), and then immersing the dried films in water to remove the water-soluble PEG. This approach creates pores (voids) in the sensing films. The dielectric contrast between the films' constituents and the voids increases photon scattering, which in turn increases the optical path of the excitation light within the film, and hence light absorption by the dye, and its PL. Optimized sensing films with a PEG: PS ratio of 1:4 (PEG's molecular weight M-w similar to 8000) led to similar to 4.4 x enhancement in the PL (in comparison to PS films). Lower M-w similar to 200 PEG with a PEG:EC ratio of 1:1 led to a PL enhancement of similar to 4.7 x. Film-dependent PL enhancements were observed at all oxygen concentrations. The strong PL enhancement enables (i) using lower dye (luminophore) concentrations, (ii) reducing power consumption and enhancing the sensor's operational lifetime when using organic light emitting diodes (OLEDs) as excitation sources, (iii) improving performance when using compact photodetectors with no internal gain, and (iv) reliably extending the dynamic range. The effect of RH on O-2 sensing is also presented. Dye: EC films are sensitive to the RH, as shown by the change of the dye's PL decay time with RH at a given O-2 concentration. Surprisingly, this RH sensitivity vanishes by adding PEG to EC, including by washing PEG off. In contrast, doping EC with TiO2 nanoparticles maintains the RH effect with the advantage of significant PL enhancement. This enhancement enables differentiation of < 10% changes in the RH, which is unattained with the dye: EC sensing films. The results are discussed in terms of the composition, thickness, and microstructure, whether porous or nanoparticle doped, of the composite films. (C) 2014 Published by Elsevier B.V. C1 [Cui, Weipan; Liu, Rui; Manna, Eeshita; Park, Joong-Mok; Fungura, Fadzai; Shinar, Joseph] US DOE, Ames Lab, Washington, DC 20585 USA. [Manna, Eeshita; Shinar, Ruth] Iowa State Univ, Microelect Res Ctr, Ames, IA 50011 USA. [Manna, Eeshita; Shinar, Ruth] Iowa State Univ, Dept Elect & Comp Engn, Ames, IA 50011 USA. RP Shinar, J (reprint author), US DOE, Ames Lab, Washington, DC 20585 USA. EM jshinar@iastate.edu FU US Department of Energy (USDOE) [DE-AC 02-07CH11358]; Basic Energy Sciences, Division of Materials Science and Engineering, USDOE FX We thank Geyuan Liu for assistance in transmission measurements. Ames Laboratory is operated by Iowa State University for the US Department of Energy (USDOE) under Contract No. DE-AC 02-07CH11358. RL, EM, JMP, and FF were supported by Basic Energy Sciences, Division of Materials Science and Engineering, USDOE. NR 50 TC 0 Z9 0 U1 5 U2 43 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0003-2670 EI 1873-4324 J9 ANAL CHIM ACTA JI Anal. Chim. Acta PD JAN 1 PY 2015 VL 853 BP 563 EP 571 DI 10.1016/j.aca.2014.10.035 PG 9 WC Chemistry, Analytical SC Chemistry GA AU5MT UT WOS:000345652000059 PM 25467504 ER PT J AU Throckmorton, HM Bird, JA Monte, N Doane, T Firestone, MK Horwath, WR AF Throckmorton, Heather M. Bird, Jeffrey A. Monte, Nick Doane, Tad Firestone, Mary K. Horwath, William R. TI The soil matrix increases microbial C stabilization in temperate and tropical forest soils SO BIOGEOCHEMISTRY LA English DT Article DE Microorganisms; Fungi; Bacteria; Carbon; Soil organic matter; Mineral protection; Stabilization ID PARTICULATE ORGANIC-MATTER; CARBON TURNOVER; NMR-SPECTROSCOPY; MINERAL CONTROL; CONIFER FOREST; DYNAMICS; C-13; SEDIMENTS; POOLS; FRACTIONATION AB Microbial biomass represents a substantial source of labile C contributing to soil organic matter (SOM) maintenance. Microbial residues may associate with the soil matrix through a variety of mechanisms, reducing its bioavailability and increasing its persistence in soil. Our objective was to examine soil matrix effects on the stability of non-living microbial C inputs in two contrasting forest ecosystems by following microbial residues (Fungi, Actinobacteria, Gram-positive bacteria (Gm +), Gram-negative bacteria (Gm -)) into SOM fractions in a temperate forest in California (CA) and a tropical forest in Puerto Rico (PR) for 3 and 2 years, respectively. We isolated 3 SOM fractions: (i) free light fraction (FLF), (ii) occluded light fraction (OLF), and (iii) dense fraction (DF). Additionally, we characterized SOM fraction chemistry to infer quality and source of native fraction SOM. Our results showed greater stabilization as mineral-associated microbial C (i.e., as DF and OLF), compared with loose detrital C (i.e., FLF). There was no microbial group effect (i.e., differences in fraction C recovery among different microbial cell types). Our findings suggest that mineral association is more important for stabilizing non-living microbial C in soil than the cellular structure of the initial source of microbial inputs, with site specific edaphic factors as the major controllers of the amount of microbial residues stabilized. C1 [Throckmorton, Heather M.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Bird, Jeffrey A.] CUNY Queens Coll, Flushing, NY 11367 USA. [Monte, Nick; Doane, Tad; Horwath, William R.] Univ Calif Davis, Davis, CA 95616 USA. [Firestone, Mary K.] Univ Calif Berkeley, Berkeley, CA 94720 USA. RP Throckmorton, HM (reprint author), Los Alamos Natl Lab, MS 495, Los Alamos, NM 87545 USA. EM hthrockmorton@lanl.gov; jbird@qc.cuny.edu; mkfstone@berkeley.edu; wrhorwath@ucdavis.edu RI Bird, Jeffrey/H-8751-2012 OI Bird, Jeffrey/0000-0002-0939-0637 FU National Science Foundation's Division of Environmental Biology, Ecosystem Science Cluster [324002]; Kearney Foundation of Soil Science; J. G. Boswell Endowed Chair in Soil Science FX This research was funded by The National Science Foundation's Division of Environmental Biology, Ecosystem Science Cluster (Award No. 324002), The Kearney Foundation of Soil Science and the J. G. Boswell Endowed Chair in Soil Science. We are grateful for contributions from researchers J. Braun, L. Dane, E. Dubinsky, J. Fortney, D. Herman, J. Pett-Ridge and W. Silver, as well as the research staff of the UC Blodgett Forest Research Station and the Luquillo Experimental Forest. NR 46 TC 7 Z9 7 U1 5 U2 58 PU SPRINGER PI DORDRECHT PA VAN GODEWIJCKSTRAAT 30, 3311 GZ DORDRECHT, NETHERLANDS SN 0168-2563 EI 1573-515X J9 BIOGEOCHEMISTRY JI Biogeochemistry PD JAN PY 2015 VL 122 IS 1 BP 35 EP 45 DI 10.1007/s10533-014-0027-6 PG 11 WC Environmental Sciences; Geosciences, Multidisciplinary SC Environmental Sciences & Ecology; Geology GA AW3CS UT WOS:000346163800003 ER PT J AU Kudahettige-Nilsson, RL Helmerius, J Nilsson, RT Sojblom, M Hodge, DB Rova, U AF Kudahettige-Nilsson, Rasika L. Helmerius, Jonas Nilsson, Robert T. Soejblom, Magnus Hodge, David B. Rova, Ulrika TI Biobutanol production by Clostridium acetobutylicum using xylose recovered from birch Kraft black liquor SO BIORESOURCE TECHNOLOGY LA English DT Article DE ABE fermentation; Birch wood Kraft black liquor; Lignin precipitation; Fermentation inhibitors; Detoxification ID ACETONE-BUTANOL FERMENTATION; BEIJERINCKII; ETHANOL; WOOD; DETOXIFICATION; WASTE; ACID; PRETREATMENT; HYDROLYSATE; LIGNIN AB Acetone-butanol-ethanol (ABE) fermentation was studied using acid-hydrolyzed xylan recovered from hardwood Kraft black liquor by CO2 acidification as the only carbon source. Detoxification of hydrolyzate using activated carbon was conducted to evaluate the impact of inhibitor removal and fermentation. Xylose hydrolysis yields as high as 18.4% were demonstrated at the highest severity hydrolysis condition. Detoxification using active carbon was effective for removal of both phenolics (76-81%) and HMF (38-52%). Batch fermentation of the hydrolyzate and semi-defined P2 media resulted in a total solvent yield of 0.12-0.13 g/g and 0.34 g/g, corresponding to a butanol concentration of 1.8-2.1 g/L and 7.3 g/L respectively. This work is the first study of a process for the production of a biologically-derived biofuel from hemicelluloses solubilized during Kraft pulping and demonstrates the feasibility of utilizing xylan recovered directly from industrial Kraft pulping liquors as a feedstock for biological production of biofuels such as butanol. (C) 2014 The Authors. Published by Elsevier Ltd. C1 [Kudahettige-Nilsson, Rasika L.; Helmerius, Jonas; Nilsson, Robert T.; Soejblom, Magnus; Hodge, David B.; Rova, Ulrika] Lulea Univ Technol, Div Chem Engn, SE-97187 Lulea, Sweden. [Hodge, David B.] Michigan State Univ, Dept Chem Engn & Mat Sci, E Lansing, MI 48824 USA. [Hodge, David B.] Michigan State Univ, Dept Biosyst & Agr Engn, E Lansing, MI 48824 USA. [Hodge, David B.] Michigan State Univ, DOE Great Lakes Bioenergy Res Ctr, E Lansing, MI 48824 USA. RP Rova, U (reprint author), Lulea Univ Technol, Div Chem Engn, SE-97187 Lulea, Sweden. EM ulrika.rova@ltu.se OI Rova, Ulrika/0000-0001-7500-2367 FU Swedish Energy Agency; VINNO-VA (Swedish Governmental Agency for Innovation Systems); Smurfit Kappa; Bio4Energy, Swedish government FX The authors wish to thank the Swedish Energy Agency, VINNO-VA (Swedish Governmental Agency for Innovation Systems), Smurfit Kappa and Bio4Energy, a strategic research environment appointed by the Swedish government, for financially supporting this work. NR 37 TC 15 Z9 15 U1 2 U2 54 PU ELSEVIER SCI LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, OXON, ENGLAND SN 0960-8524 EI 1873-2976 J9 BIORESOURCE TECHNOL JI Bioresour. Technol. PD JAN PY 2015 VL 176 BP 71 EP 79 DI 10.1016/j.biortech.2014.11.012 PG 9 WC Agricultural Engineering; Biotechnology & Applied Microbiology; Energy & Fuels SC Agriculture; Biotechnology & Applied Microbiology; Energy & Fuels GA AW0LE UT WOS:000345982900010 PM 25460986 ER PT J AU Reiche, HM Carpenter, JS Stein, F Tomida, T Vogel, SC AF Reiche, H. M. Carpenter, J. S. Stein, F. Tomida, T. Vogel, S. C. TI Metallurgical studies with the HIPPO diffractometer at LANSCE SO CANADIAN METALLURGICAL QUARTERLY LA English DT Article DE Low carbon steel; Texture memory effect; Nanocomposites; Multilayer; Variant selection; Creep furnace; Neutron diffraction ID NB NANOLAMELLAR COMPOSITES; BONDING ARB PROCESS; FE-AL SYSTEM; ENGINEERING MATERIALS; NEUTRON-DIFFRACTION; PHASE-EQUILIBRIA; HIGH-STRENGTH; TEXTURE; INTERFACES; EVOLUTION AB Advantages of neutron diffraction for metallurgical studies are highlighted with research examples performed on the High Pressure -Preferred Orientation diffractometerat the Los Alamos Neutron Science Center. The previously inconclusive crystallographic structure of the Fe-Al epsilon-phase, stable between 1095 and 1231 degrees C, was determined by in situ neutron diffraction to have the formula Fe5Al8 with a body centred cubic structure of the Hume-Rothery Cu5Zn8 type at 1120 degrees C. As a second example, the effect of variations in accumulative roll bonding processing parameters on interfacial structure, hardness, and thermal stability are explored for lamellar Cu-Nb multilayers with individual layer thicknesses of 20 nm. Furthermore, we derive an explanation for observed texture memory effects during the alpha ->gamma ->alpha transformation cycle in a 0.1% C-1% Mn hot rolled steel sheet from the double Kurdjumov-Sachs relationship. Finally, we present in situ results of a Zr-2.5Nb sample heated into the beta-field and subsequently compressed by 20% via our recently developed creep furnace which uniquely allows deconvolution of the effects of heating, phase transformations, deformation and cooling on the texture evolution. C1 [Reiche, H. M.; Vogel, S. C.] Los Alamos Natl Lab, Los Alamos Neutron Scattering Ctr, Los Alamos, NM 87545 USA. [Carpenter, J. S.] Los Alamos Natl Lab, Mat Sci & Technol Div, Los Alamos, NM 87545 USA. [Stein, F.] Max Planck Inst Eisenforsch GmbH, D-40237 Dusseldorf, Germany. [Tomida, T.] Nippon Steel & Sumitomo Met Corp, Steel Res Labs, Tech Res & Dev Bur, Amagasaki, Hyogo 6600891, Japan. RP Reiche, HM (reprint author), Los Alamos Natl Lab, Los Alamos Neutron Scattering Ctr, Los Alamos, NM 87545 USA. EM reiche@lanl.gov OI Vogel, Sven C./0000-0003-2049-0361; Carpenter, John/0000-0001-8821-043X FU US Department of Energy's Office of Basic Energy Science; Center for Materials at Irradiation and Mechanical Extremes, an Energy Frontier Research Center - US Department of Energy, Office of Science, Office of Basic Energy Sciences [2008LANL1026]; DOE [DE-AC52-06NA25396] FX This work benefited from the Lujan Neutron Scattering Center at the Los Alamos Neutron Science Center which was funded by the US Department of Energy's Office of Basic Energy Science. The authors gratefully acknowledge support from the Center for Materials at Irradiation and Mechanical Extremes, an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Office of Basic Energy Sciences under Award Number 2008LANL1026. This work was performed, in part, at the Center for Integrated Nanotechnologies, an Office of Science User Facility operated by the US Department of Energy, Office of Science. The Los Alamos National Laboratory is operated by the Los Alamos National Security LLC under the DOE Contract DE-AC52-06NA25396. NR 34 TC 0 Z9 0 U1 1 U2 9 PU MANEY PUBLISHING PI LEEDS PA STE 1C, JOSEPHS WELL, HANOVER WALK, LEEDS LS3 1AB, W YORKS, ENGLAND SN 0008-4433 EI 1879-1395 J9 CAN METALL QUART JI Can. Metall. Q. PD JAN PY 2015 VL 54 IS 1 BP 2 EP 8 DI 10.1179/1879139514Y.0000000157 PG 7 WC Metallurgy & Metallurgical Engineering SC Metallurgy & Metallurgical Engineering GA AW2NT UT WOS:000346126000002 ER PT J AU Richter, K Lorbeer, C Mudring, AV AF Richter, K. Lorbeer, C. Mudring, A. -V. TI A novel approach to prepare optically active ion doped luminescent materials via electron beam evaporation into ionic liquids SO CHEMICAL COMMUNICATIONS LA English DT Article ID UP-CONVERSION PHOSPHORS; CDSE QUANTUM DOTS; FLUORIDE NANOPARTICLES; ANTIREFLECTIVE COATINGS; METAL NANOPARTICLES; LAF3 NANOPARTICLES; ALKALINE-EARTH; THIN-FILMS; MGF2; PARTICLES AB A novel approach to prepare luminescent materials via electron-beam evaporation into ionic liquids is presented which even allows doping of host lattices with ions that have a strong size mismatch. To prove this, MgF2 nanoparticles doped with Eu3+ were fabricated. The obtained nanoparticles featured an unusually high luminescence lifetime and the obtained material showed a high potential for application. C1 [Richter, K.; Lorbeer, C.; Mudring, A. -V.] Ruhr Univ Bochum, D-44801 Bochum, Germany. [Mudring, A. -V.] Iowa State Univ, Dept Mat Sci & Engn, Ames, IA 50010 USA. [Mudring, A. -V.] Ames Lab DOE, Crit Mat Inst, Ames, IA 50010 USA. RP Mudring, AV (reprint author), Ruhr Univ Bochum, Univ Str 150, D-44801 Bochum, Germany. EM anja.mudring@rub.de FU Critical Materials Institute, an Energy Innovation Hub - U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Advanced Manufacturing Office FX This work was supported in part by the Critical Materials Institute, an Energy Innovation Hub funded by the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Advanced Manufacturing Office. NR 51 TC 1 Z9 1 U1 2 U2 33 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1359-7345 EI 1364-548X J9 CHEM COMMUN JI Chem. Commun. PY 2015 VL 51 IS 1 BP 114 EP 117 DI 10.1039/c4cc05817h PG 4 WC Chemistry, Multidisciplinary SC Chemistry GA AU9JW UT WOS:000345909400021 PM 25383750 ER PT J AU Chee, SW Pratt, SH Hattar, K Duquette, D Ross, FM Hull, R AF Chee, See Wee Pratt, Sarah H. Hattar, Khalid Duquette, David Ross, Frances M. Hull, Robert TI Studying localized corrosion using liquid cell transmission electron microscopy SO CHEMICAL COMMUNICATIONS LA English DT Article ID PITTING CORROSION; GROWTH; COPPER; ALUMINUM; BEHAVIOR AB Localized corrosion of Cu and Al thin films exposed to aqueous NaCl solutions was studied using liquid cell transmission electron microscopy (LCTEM). We demonstrate that potentiostatic control can be used to initiate pitting and that local compositional changes, due to focused ion beam implantation of Au+ ions, can modify the corrosion susceptibility of Al films. C1 [Chee, See Wee; Duquette, David; Hull, Robert] Rensselaer Polytech Inst, Dept Mat Sci & Engn, Troy, NY 12180 USA. [Pratt, Sarah H.; Hattar, Khalid] Sandia Natl Labs, Albuquerque, NM 87123 USA. [Ross, Frances M.] IBM Corp, Thomas J Watson Res Ctr, Yorktown Hts, NY 10598 USA. RP Chee, SW (reprint author), Rensselaer Polytech Inst, Dept Mat Sci & Engn, Troy, NY 12180 USA. EM see.wee.chee@gmail.com RI Chee, See Wee/C-6052-2008; Ross, Frances/P-8919-2015 OI Chee, See Wee/0000-0003-0095-3242; Ross, Frances/0000-0003-0838-9770 FU National Science Foundation [DMR-1309509]; Division of Materials Science and Engineering; U.S. Department of Energy's Office of Basic Energy Sciences; Office of Energy and Renewable Energy Water Power Program; U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX S.W.C, D.D., F.M. R. and R.H. acknowledge Dr Joseph Grogan and Dr Jeung-Hun Park for discussions on beam effects, Mr Nicholas Scheidner for modelling the radiolysis species and Ms Ainsley Pinkowitz for her assistance with electrochemistry experiments. Funding at Rensselaer Polytechnic Institute is provided by the National Science Foundation, grant number DMR-1309509. K.H. and S.H.P acknowledge Ms Aubrianna Kinghorn and Dr Bernadette Hernandez-Sanchez for their assistance and the Division of Materials Science and Engineering, the U.S. Department of Energy's Office of Basic Energy Sciences along with Office of Energy and Renewable Energy Water Power Program for partial support. Sandia National Laboratories is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000. NR 27 TC 4 Z9 4 U1 10 U2 46 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1359-7345 EI 1364-548X J9 CHEM COMMUN JI Chem. Commun. PY 2015 VL 51 IS 1 BP 168 EP 171 DI 10.1039/c4cc06443g PG 4 WC Chemistry, Multidisciplinary SC Chemistry GA AU9JW UT WOS:000345909400035 PM 25388023 ER PT J AU Conato, MT Oleksiak, MD McGrail, BP Motkuri, RK Rimer, JD AF Conato, Marlon T. Oleksiak, Matthew D. McGrail, B. Peter Motkuri, Radha K. Rimer, Jeffrey D. TI Framework stabilization of Si-rich LTA zeolite prepared in organic-free media SO CHEMICAL COMMUNICATIONS LA English DT Article ID STRUCTURE-DIRECTING AGENTS; PRESSURE SWING ADSORPTION; SEED-ASSISTED SYNTHESIS; SYNTHETIC ZEOLITE; ION-EXCHANGE; CRYSTALLINE ZEOLITES; ORGANOTEMPLATE-FREE; SI/AL RATIOS; SEPARATION; MIXTURES AB Zeolite HOU-2 (LTA type) is prepared with the highest silica content (Si/Al = 2.1) reported for Na-LTA zeolites without the use of an organic structure-directing agent. The rational design of Si-rich zeolites has the potential to improve their thermal stability for applications in catalysis, gas storage, and selective separations. C1 [Conato, Marlon T.; Oleksiak, Matthew D.; Rimer, Jeffrey D.] Univ Houston, Dept Chem & Biomol Engn, Houston, TX 77204 USA. [McGrail, B. Peter; Motkuri, Radha K.] Pacific NW Natl Lab, Richland, WA 99354 USA. RP Rimer, JD (reprint author), Univ Houston, Dept Chem & Biomol Engn, 4800 Calhoun Rd, Houston, TX 77204 USA. EM jrimer@central.uh.edu RI Motkuri, Radha/F-1041-2014; OI Motkuri, Radha/0000-0002-2079-4798; Oleksiak, Matthew/0000-0002-0419-2092 FU National Science Foundation [CAREER 1151098]; Norman Hackerman Advanced Research Program [003652-0024-2011]; Welch Foundation [E-1794]; U.S. Department of Energy (DOE); U.S. DOE [DE-AC05-76RL01830] FX This work has been supported by the National Science Foundation (CAREER 1151098), the Norman Hackerman Advanced Research Program (003652-0024-2011), and the Welch Foundation (Award E-1794). The CO2 sorption work was performed at Pacific Northwest National Laboratory (PNNL) and has been supported by the U.S. Department of Energy (DOE). PNNL is operated by Battelle for the U.S. DOE under Contract DE-AC05-76RL01830. NR 52 TC 8 Z9 8 U1 15 U2 74 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1359-7345 EI 1364-548X J9 CHEM COMMUN JI Chem. Commun. PY 2015 VL 51 IS 2 BP 269 EP 272 DI 10.1039/c4cc07396g PG 4 WC Chemistry, Multidisciplinary SC Chemistry GA AW0IK UT WOS:000345975000003 PM 25347029 ER PT J AU Deng, Y Zhang, GH Qi, XT Liu, C Miller, JT Kropf, AJ Bunel, EE Lan, Y Lei, AW AF Deng, Yi Zhang, Guanghui Qi, Xiaotian Liu, Chao Miller, Jeffrey T. Kropf, A. Jeremy Bunel, Emilio E. Lan, Yu Lei, Aiwen TI Revealing the halide effect on the kinetics of the aerobic oxidation of Cu(I) to Cu(II) SO CHEMICAL COMMUNICATIONS LA English DT Article ID COPPER-CATALYZED OXIDATION; ALCOHOL OXIDATION; END-ON; COMPLEXES; FUNCTIONALIZATION; MECHANISM; DIOXYGEN; 2,6-DIMETHYLPHENOL; POLYMERIZATION; CHEMISTRY AB In situ infrared (IR) and X-ray absorption near-edge structure (XANES) spectroscopic investigations reveal that different halide ligands have distinct effects on the aerobic oxidation of Cu(I) to Cu(II) in the presence of TMEDA (tetramethylethylenediamine). The iodide ligand gives the lowest rate and thus leads to the lowest catalytic reaction rate of aerobic oxidation of hydroquinone to benzoquinone. Further DFT calculations suggest that oxidation of CuI-TMEDA involves a side-on transition state, while oxidation of CuCl-TMEDA involves an end-on transition state which has a lower activation energy. C1 [Deng, Yi; Zhang, Guanghui; Liu, Chao; Lei, Aiwen] Wuhan Univ, Coll Chem & Mol Sci, Wuhan 430072, Hubei, Peoples R China. [Deng, Yi; Zhang, Guanghui; Miller, Jeffrey T.; Kropf, A. Jeremy; Bunel, Emilio E.; Lei, Aiwen] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. [Qi, Xiaotian; Lan, Yu] Chongqing Univ, Sch Chem & Chem Engn, Chongqing 400030, Peoples R China. RP Lan, Y (reprint author), Chongqing Univ, Sch Chem & Chem Engn, Chongqing 400030, Peoples R China. EM lanyu@cqu.edu.cn; aiwenlei@whu.edu.cn RI Zhang, Guanghui/C-4747-2008; ID, MRCAT/G-7586-2011; Lan, Yu/A-8146-2016; OI Zhang, Guanghui/0000-0002-5854-6909; Lan, Yu/0000-0002-2328-0020; Liu, Chao/0000-0002-2521-924X; Lei, Aiwen/0000-0001-8417-3061 FU 973 Program [2011CB808600, 2012CB725302]; National Natural Science Foundation of China [21390400, 21025206, 21272180, 21302148, 21372266, 51302327]; Research Fund for the Doctoral Program of Higher Education of China [20120141130002]; Program for Changjiang Scholars and Innovative Research Team in University [IRT1030]; U. S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]; Department of Energy; MRCAT member institutions; Chemical Sciences and Engineering Division at Argonne National Laboratory FX This work was supported by the 973 Program (2011CB808600 and 2012CB725302), the National Natural Science Foundation of China (21390400, 21025206, 21272180, 21302148, 21372266, and 51302327), the Research Fund for the Doctoral Program of Higher Education of China (20120141130002) and the Program for Changjiang Scholars and Innovative Research Team in University (IRT1030). The Program of Introducing Talents of Discipline to Universities of China (111 Program) is also appreciated. Use of the Advanced Photon Source was supported by the U. S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. MRCAT operations are supported by the Department of Energy and the MRCAT member institutions. This work was also funded by the Chemical Sciences and Engineering Division at Argonne National Laboratory. In addition, we thank Prof. Mei-Xiang Wang (Tsinghua University) for providing the Cu(III) sample. NR 44 TC 10 Z9 10 U1 15 U2 92 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1359-7345 EI 1364-548X J9 CHEM COMMUN JI Chem. Commun. PY 2015 VL 51 IS 2 BP 318 EP 321 DI 10.1039/c4cc05720a PG 4 WC Chemistry, Multidisciplinary SC Chemistry GA AW0IK UT WOS:000345975000016 PM 25407986 ER PT J AU Yuan, JW Wang, J Zhang, GH Liu, C Qi, XT Lan, Y Miller, JT Kropf, AJ Bunel, EE Lei, AW AF Yuan, Jiwen Wang, Jing Zhang, Guanghui Liu, Chao Qi, Xiaotian Lan, Yu Miller, Jeffrey T. Kropf, A. Jeremy Bunel, Emilio E. Lei, Aiwen TI Bimetallic zinc complex - active species in coupling of terminal alkynes with aldehydes via nucleophilic addition/Oppenauer oxidation SO CHEMICAL COMMUNICATIONS LA English DT Article ID MANNICH-TYPE REACTION; CATALYZED CHEMOSELECTIVE REDUCTION; ASYMMETRIC MICHAEL ADDITION; ENANTIOSELECTIVE SYNTHESIS; PROPARGYLIC ALCOHOLS; ALDOL ADDITIONS; AQUEOUS-MEDIA; BETA-AMINO; ACETYLENES; NITROALKENES AB A mechanistic study on the zinc-promoted coupling between aldehydes and terminal alkynes via nucleophilic addition/Oppenauer oxidation using operando IR, XANES/EXAFS techniques and DFT calculations was demonstrated. It was determined that a bimetallic zinc complex was the active species. C1 [Yuan, Jiwen; Wang, Jing; Zhang, Guanghui; Liu, Chao; Lei, Aiwen] Wuhan Univ, Coll Chem & Mol Sci, Wuhan 430072, Hubei, Peoples R China. [Zhang, Guanghui; Miller, Jeffrey T.; Kropf, A. Jeremy; Bunel, Emilio E.; Lei, Aiwen] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. [Qi, Xiaotian; Lan, Yu] Chongqing Univ, Sch Chem & Chem Engn, Chongqing 400030, Peoples R China. RP Liu, C (reprint author), Wuhan Univ, Coll Chem & Mol Sci, Wuhan 430072, Hubei, Peoples R China. EM chao.liu@whu.edu.cn; lanyu@cqu.edu.cn; aiwenlei@whu.edu.cn RI Zhang, Guanghui/C-4747-2008; ID, MRCAT/G-7586-2011; Lei, Aiwen/G-8033-2015; Lan, Yu/A-8146-2016; OI Zhang, Guanghui/0000-0002-5854-6909; Lei, Aiwen/0000-0001-8417-3061; Lan, Yu/0000-0002-2328-0020; Liu, Chao/0000-0002-2521-924X FU 973 Program [2012CB725302]; National Natural Science Foundation of China [21390400, 21025206, 21272180, 21302148, 21372266]; Program for Changjiang Scholars and Innovative Research Team in University [IRT1030]; Research Fund for the Doctoral Program of Higher Education of China [20120141130002]; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]; Department of Energy; MRCAT member institutions FX This work was supported by the 973 Program (2012CB725302), the National Natural Science Foundation of China (21390400, 21025206, 21272180, 21302148 and 21372266), and the Program for Changjiang Scholars and Innovative Research Team in University (IRT1030) and the Research Fund for the Doctoral Program of Higher Education of China (20120141130002). The Program of Introducing Talents of Discipline to Universities of China (111 Program) is also appreciated. The use of the Advanced Photon Source was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. MRCAT operations are supported by the Department of Energy and the MRCAT member institutions. NR 51 TC 18 Z9 18 U1 10 U2 65 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1359-7345 EI 1364-548X J9 CHEM COMMUN JI Chem. Commun. PY 2015 VL 51 IS 3 BP 576 EP 579 DI 10.1039/c4cc08152h PG 4 WC Chemistry, Multidisciplinary SC Chemistry GA AW1RU UT WOS:000346068200031 PM 25413491 ER PT J AU Velasco, V Aguila, D Barrios, LA Borilovic, I Roubeau, O Ribas-Arino, J Fumanal, M Teat, SJ Aromi, G AF Velasco, V. Aguila, D. Barrios, L. A. Borilovic, I. Roubeau, O. Ribas-Arino, J. Fumanal, M. Teat, S. J. Aromi, G. TI New coordination features; a bridging pyridine and the forced shortest non-covalent distance between two CO32- species SO CHEMICAL SCIENCE LA English DT Article ID BETA-DIKETONATE LIGAND; MAGNETIC-PROPERTIES; CRYSTAL-STRUCTURE; CREVICE COORDINATION; MOLECULAR-STRUCTURES; COMPLEXES; FIXATION; CLUSTER; SERIES; DINUCLEAR AB The aerobic reaction of the multidentate ligand 2,6-bis-(3-oxo-3-(2-hydroxyphenyl)-propionyl)-pyridine, H4L, with Co(II) salts in strong basic conditions produces the clusters [Co-4(L)(2)(OH)(py)(7)]NO3 (1) and [Co8Na4(L)(4)(OH)(2)(CO3)(2)(py)(10)](BF4)(2) (2). Analysis of their structure unveils unusual coordination features including a very rare bridging pyridine ligand or two trapped carbonate anions within one coordination cage, forced to stay at an extremely close distance (d(O center dot center dot center dot O) = 1.946 angstrom). This unprecedented non-bonding proximity represents a meeting point between long covalent interactions and "intermolecular" contacts. These original motifs have been analysed here through DFT calculations, which have yielded interaction energies and the reduced repulsion energy experimented by both CO32 anions when located in close proximity inside the coordination cage. C1 [Velasco, V.; Aguila, D.; Barrios, L. A.; Borilovic, I.; Aromi, G.] Univ Barcelona, Dept Quim Inorgan, E-08028 Barcelona, Spain. [Roubeau, O.] CSIC, Inst Ciencia Mat Aragon, E-50009 Zaragoza, Spain. [Roubeau, O.] Univ Zaragoza, E-50009 Zaragoza, Spain. [Ribas-Arino, J.; Fumanal, M.] Univ Barcelona, Dept Quim Fis, Barcelona 08028, Spain. [Ribas-Arino, J.; Fumanal, M.] Univ Barcelona, IQTCUB, Barcelona 08028, Spain. [Teat, S. J.] Berkeley Lab, Adv Light Source, Berkeley, CA 94720 USA. RP Aromi, G (reprint author), Univ Barcelona, Dept Quim Inorgan, Diagonal 645, E-08028 Barcelona, Spain. EM guillem.aromi@qi.ub.es RI Ribas, Jordi/G-8076-2011; Aromi, Guillem/I-2483-2015; Roubeau, Olivier/A-6839-2010; BARRIOS MORENO, LEONI ALEJANDRA/E-5413-2017; OI Ribas, Jordi/0000-0003-4088-6187; Aromi, Guillem/0000-0002-0997-9484; Roubeau, Olivier/0000-0003-2095-5843; BARRIOS MORENO, LEONI ALEJANDRA/0000-0001-7075-9950; Fumanal, Maria/0000-0002-4175-8876 FU ERC [258060]; Spanish MICINN [CTQ2009-06959, MAT2011-24284]; University of Barcelona; Office of Science, Office of Basic Energy Sciences of the U.S. Department of Energy [DE-AC02-05CH11231]; "Ramon y Cajal" Fellowship FX G.A. thanks the Generalitat de Catalunya for the prize ICREA Academia 2008 and 2013, for excellence in research and the ERC for a Starting Grant (258060 FuncMolQIP). The authors thank the Spanish MICINN for funding through CTQ2009-06959 (GA, LAB, DA), MAT2011-24284 (OR) and a "Ramon y Cajal" Fellowship (JRA), the ERC for a Predoctoral Fellowship under grant 258060 FuncMolQIP (VV and IB) and University of Barcelona for a Ph-D grant (MF). Data for H4L and 1 were collected through access to ALS beamline 11.3.1. The Advanced Light Source is supported by the Director, Office of Science, Office of Basic Energy Sciences of the U.S. Department of Energy under contract no. DE-AC02-05CH11231. NR 62 TC 4 Z9 4 U1 3 U2 21 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2041-6520 EI 2041-6539 J9 CHEM SCI JI Chem. Sci. PY 2015 VL 6 IS 1 BP 123 EP 131 DI 10.1039/c4sc02491e PG 9 WC Chemistry, Multidisciplinary SC Chemistry GA AU9HD UT WOS:000345901600007 ER PT J AU Kline, MA Wei, XX Horner, IJ Liu, R Chen, S Chen, S Yung, KY Yamato, K Cai, ZH Bright, FV Zeng, XC Gong, B AF Kline, Mark A. Wei, Xiaoxi Horner, Ian J. Liu, Rui Chen, Shuang Chen, Si Yung, Ka Yi Yamato, Kazuhiro Cai, Zhonghou Bright, Frank V. Zeng, Xiao Cheng Gong, Bing TI Extremely strong tubular stacking of aromatic oligoamide macrocycles SO CHEMICAL SCIENCE LA English DT Article ID HYDROGEN-BONDING INTERACTIONS; ASSEMBLING ORGANIC NANOTUBES; SHAPE-PERSISTENT MACROCYCLES; ONE-POT FORMATION; CARBON NANOTUBES; LIQUID-CRYSTAL; MASS-TRANSPORT; BETA-BARRELS; SOLID-STATE; MOLECULES AB As the third-generation rigid macrocycles evolved from progenitor 1, cyclic aromatic oligoamides 3, with a backbone of reduced constraint, exhibit extremely strong stacking with an astoundingly high affinity (estimated lower limit of K-dimer > 10(13) M-1 in CHCl3), which leads to dispersed tubular stacks that undergo further assembly in solution. Computational study reveals a very large binding energy (-49.77 kcal mol(-1)) and indicates highly cooperative local dipole interactions that account for the observed strength and directionality for the stacking of 3. In the solid-state, X-ray diffraction (XRD) confirms that the aggregation of 3 results in well-aligned tubular stacks. The persistent tubular assemblies of 3, with their non-deformable sub-nm pore, are expected to possess many interesting functions. One such function, transmembrane ion transport, is observed for 3. C1 [Kline, Mark A.; Wei, Xiaoxi; Horner, Ian J.; Liu, Rui; Yung, Ka Yi; Yamato, Kazuhiro; Bright, Frank V.; Gong, Bing] SUNY Buffalo, Dept Chem, Buffalo, NY 14260 USA. [Chen, Shuang; Zeng, Xiao Cheng] Univ Nebraska, Dept Chem, Lincoln, NE 68588 USA. [Chen, Si; Cai, Zhonghou] Argonne Natl Lab, Xray Sci Div, Argonne, IL 60439 USA. [Gong, Bing] Beijing Normal Univ, Coll Chem, Beijing 100875, Peoples R China. RP Gong, B (reprint author), SUNY Buffalo, Dept Chem, Buffalo, NY 14260 USA. EM bgong@buffalo.edu RI Yamato, Kazuhiro/G-4213-2013; Chen, Shuang/N-7917-2015; OI Yamato, Kazuhiro/0000-0001-9592-0739; Bright, Frank/0000-0002-1500-5969 FU National Science Foundation [CHE-1306326]; Natural Science Foundation of China [91227109]; US Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357] FX We thank the support of the National Science Foundation (CHE-1306326) and the Natural Science Foundation of China (91227109). Use of the Advanced Photon Source was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, under contract no. DE-AC02-06CH11357. NR 87 TC 9 Z9 9 U1 5 U2 49 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2041-6520 EI 2041-6539 J9 CHEM SCI JI Chem. Sci. PY 2015 VL 6 IS 1 BP 152 EP 157 DI 10.1039/c4sc02380c PG 6 WC Chemistry, Multidisciplinary SC Chemistry GA AU9HD UT WOS:000345901600011 ER PT J AU Park, YI Postupna, O Zhugayevych, A Shin, H Park, YS Kim, B Yen, HJ Cheruku, P Martinez, JS Park, JW Tretiak, S Wang, HL AF Park, Y. I. Postupna, O. Zhugayevych, A. Shin, H. Park, Y. -S. Kim, B. Yen, H. -J. Cheruku, P. Martinez, J. S. Park, J. W. Tretiak, S. Wang, H. -L. TI A new pH sensitive fluorescent and white light emissive material through controlled intermolecular charge transfer SO CHEMICAL SCIENCE LA English DT Article ID SINGLE-EMITTING-COMPONENT; DENSITY-FUNCTIONAL THEORY; CONJUGATED POLYMERS; PUSH-PULL; DIODES; MOLECULES; ELECTROLUMINESCENCE; EXCITON; WATER; CHROMOPHORES AB A new, pH dependent and water-soluble, conjugated oligomer (amino, trimethylammonium oligophenylene vinylene, ATAOPV) was synthesized with a quaternary ammonium salt and an aromatic amine at the two ends of a pi-conjugated oligomer, thus creating a strong dipole across the molecule. A unique white light LED is successfully fabricated from a stimuli responsive organic molecule whose emission properties are dominated by the pH value of the solution through controlled intermolecular charge transfer. C1 [Park, Y. I.; Park, Y. -S.; Yen, H. -J.; Cheruku, P.; Wang, H. -L.] Los Alamos Natl Lab, Div Chem, Phys Chem & Appl Spect C PCS, Los Alamos, NM 87545 USA. [Postupna, O.; Zhugayevych, A.; Tretiak, S.] Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. [Shin, H.; Kim, B.; Park, J. W.] Catholic Univ Korea, Display Res Ctr, Dept Chem, Puchon 420743, South Korea. [Martinez, J. S.] Los Alamos Natl Lab, Ctr Integrated Nanotechnol, Mat Phys & Applicat Div, Los Alamos, NM 87545 USA. RP Wang, HL (reprint author), Los Alamos Natl Lab, Div Chem, Phys Chem & Appl Spect C PCS, Los Alamos, NM 87545 USA. EM serg@lanl.gov; hwang@lanl.gov RI Tretiak, Sergei/B-5556-2009; OI Tretiak, Sergei/0000-0001-5547-3647; Park, Young-Shin/0000-0003-4204-1305; Yen, Hung-Ju/0000-0002-6316-9124 FU Laboratory Directed Research and Development program; National Research Foundation of Korea (NRF) - Korea government (MEST) [2012001846]; U.S. Department of Energy [DE-AC52-06NA25396] FX The authors would like to acknowledge financial support by the Laboratory Directed Research and Development program, (YIP, HLW, ST, OP and AZ), for the synthesis and theoretical consideration of conjugated oligomers. Photophysical characterization of conjugated oligomers was supported by the Basic Energy Science, Biomolecular Materials Program, Division of Materials Science and Engineering (H.-L Wang and J. S. Martinez). A.Z. thanks Troy van Voorhis for discussion on charge transfer states and Jason Keith for helpful suggestions on computational methodology. (BJK, HGS, J. W. Park) was supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MEST) (No. 2012001846). This work was performed, in part, at the Center for Integrated Nanotechnologies, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science. Los Alamos National Laboratory, an affirmative action equal opportunity employer, is operated by Los Alamos National Security, LLC, for the National Nuclear Security Administration of the U.S. Department of Energy under contract DE-AC52-06NA25396. NR 63 TC 29 Z9 29 U1 7 U2 64 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2041-6520 EI 2041-6539 J9 CHEM SCI JI Chem. Sci. PY 2015 VL 6 IS 1 BP 789 EP 797 DI 10.1039/c4sc01911c PG 9 WC Chemistry, Multidisciplinary SC Chemistry GA AU9HD UT WOS:000345901600096 ER PT J AU Allendorf, MD Stavila, V AF Allendorf, Mark D. Stavila, Vitalie TI Crystal engineering, structure-function relationships, and the future of metal-organic frameworks SO CRYSTENGCOMM LA English DT Article ID POROUS COORDINATION POLYMER; ZEOLITIC IMIDAZOLATE FRAMEWORKS; HYDROGEN STORAGE; DRUG-DELIVERY; MOLECULAR-DYNAMICS; METHANE STORAGE; CARBON-DIOXIDE; GAS-ADSORPTION; HETEROGENEOUS CATALYST; NANOPOROUS MATERIALS AB Metal-Organic Frameworks (MOFs) are a rapidly expanding class of hybrid organic-inorganic materials that can be rationally designed and assembled through crystal engineering. The explosion of interest in this subclass of coordination polymers results from their outstanding properties and myriad possible applications, which include traditional uses of microporous materials, such as gas storage, separations, and catalysis, as well as new realms in biomedicine, electronic devices, and information storage. The objective of this Highlight article is to provide the reader with a sense of where the field stands after roughly fifteen years of research. Remarkable progress has been made, but the barriers to practical and commercial advances are also evident. We discuss the basic elements of MOF assembly and present a conceptual hierarchy of structural elements that assists in understanding how unique properties in these materials can be achieved. Structure-function relationships are then discussed; several are now well understood, as a result of the focused efforts of many research groups over the past decade. Prospects for the use of MOFs in membranes, catalysis, biomedicine, and as active components in electronic and photonic devices are also discussed. Finally, we identify the most pressing challenges in our view that must be addressed for these materials to realize their full potential in the marketplace. C1 [Allendorf, Mark D.; Stavila, Vitalie] Sandia Natl Labs, Livermore, CA 94551 USA. RP Allendorf, MD (reprint author), Sandia Natl Labs, Livermore, CA 94551 USA. EM mdallen@sandia.gov FU Sandia Laboratory Directed Research and Development Program; U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX The writing of this article was enabled by the support of the Sandia Laboratory Directed Research and Development Program. Sandia National Laboratories is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000. NR 178 TC 66 Z9 66 U1 26 U2 255 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1466-8033 J9 CRYSTENGCOMM JI Crystengcomm PY 2015 VL 17 IS 2 BP 229 EP 246 DI 10.1039/c4ce01693a PG 18 WC Chemistry, Multidisciplinary; Crystallography SC Chemistry; Crystallography GA AW3GB UT WOS:000346173200004 ER PT J AU Serra-Crespo, P Dikhtiarenko, A Stavitski, E Juan-Alcaniz, J Kapteijn, F Coudert, FX Gascon, J AF Serra-Crespo, Pablo Dikhtiarenko, Alla Stavitski, Eli Juan-Alcaniz, Jana Kapteijn, Freek Coudert, Francois-Xavier Gascon, Jorge TI Experimental evidence of negative linear compressibility in the MIL-53 metal-organic framework family SO CRYSTENGCOMM LA English DT Article ID IMIDAZOLATE FRAMEWORK; SINGLE-CRYSTAL; PRESSURE; DIFFRACTION; SEPARATION; SOLIDS AB We report a series of powder X-ray diffraction experiments performed on the soft porous crystals MIL-53(Al) and NH2-MIL-53(Al) in a diamond anvil cell under different pressurization media. Systematic refinements of the obtained powder patterns demonstrate that these materials expand along a specific direction while undergoing total volume reduction under an increasing hydrostatic pressure. The results confirm for the first time the negative linear compressibility behaviour of this family of materials, recently predicted from quantum chemical calculations. C1 [Serra-Crespo, Pablo; Dikhtiarenko, Alla; Juan-Alcaniz, Jana; Kapteijn, Freek; Gascon, Jorge] Delft Univ Technol, NL-2628 BL Delft, Netherlands. [Stavitski, Eli] Brookhaven Natl Lab, Natl Synchrotron Light Source, Upton, NY 11973 USA. [Coudert, Francois-Xavier] CNRS Chim ParisTech, Inst Rech Chim Paris, F-75005 Paris, France. RP Serra-Crespo, P (reprint author), Delft Univ Technol, Julianalaan 136, NL-2628 BL Delft, Netherlands. EM P.SerraCrespo@tudelft.nl; J.Gascon@tudelft.nl RI Gascon, Jorge/E-8798-2010; Group, CE/C-3853-2009; Serra-Crespo, Pablo/A-3170-2012; Kapteijn, Frederik /F-2031-2010; Coudert, Francois-Xavier/C-1374-2008; OI Gascon, Jorge/0000-0001-7558-7123; Kapteijn, Frederik /0000-0003-0575-7953; Coudert, Francois-Xavier/0000-0001-5318-3910; Serra Crespo, Pablo/0000-0002-5106-0527 FU COMPRES; Consortium for Materials Properties Research in Earth Sciences, under NSF [EAR 10-43050]; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-98CH10886]; European Research Council under the European Union's Seventh Framework Programme/ERC [335746]; CrystEng-MOF-MMM FX We are grateful to Zhiqiang Chen for his help with XRD experiments. This research was partially supported by COMPRES, the Consortium for Materials Properties Research in Earth Sciences, under NSF Cooperative Agreement EAR 10-43050. Use of the National Synchrotron Light Source, Brookhaven National Laboratory, was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under contract no. DE-AC02-98CH10886. The research leading to these results has received funding from the European Research Council under the European Union's Seventh Framework Programme (FP/2007-2013)/ERC grant agreement no. 335746, CrystEng-MOF-MMM. NR 39 TC 33 Z9 33 U1 7 U2 60 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1466-8033 J9 CRYSTENGCOMM JI Crystengcomm PY 2015 VL 17 IS 2 BP 276 EP 280 DI 10.1039/c4ce00436a PG 5 WC Chemistry, Multidisciplinary; Crystallography SC Chemistry; Crystallography GA AW3GB UT WOS:000346173200007 PM 25722647 ER PT J AU Qu, L Long, FH Peng, HC AF Qu, Lei Long, Fuhui Peng, Hanchuan TI 3-D Registration of Biological Images and Models [Registration of microscopic images and its uses in segmentation and annotation] SO IEEE SIGNAL PROCESSING MAGAZINE LA English DT Article ID C. ELEGANS; DROSOPHILA; BRAINS; REPRESENTATION; RECOGNITION; ALGORITHM; ALIGNMENT; ATLAS; FRUIT C1 [Qu, Lei; Long, Fuhui] Howard Hughes Med Inst, Ashburn, VA USA. [Long, Fuhui] Lawrence Berkeley Natl Lab, Berkeley, CA USA. [Long, Fuhui] Duke Univ, Durham, NC 27706 USA. [Peng, Hanchuan] Allen Inst Brain Sci, Res Grp, Seattle, WA USA. RP Qu, L (reprint author), Anhui Univ, Hefei, Peoples R China. EM qulei@ahu.edu.cn; fuhuil@alleninstitute.org; hanchuanp@alleninstitute.org RI Magazine, Signal Processing/E-9947-2015 FU Chinese Natural Science Foundation [61201396, 61301296, 61377006, U1201255]; Scientific Research Foundation for the Returned Overseas Chinese Scholars, State Education Ministry; Technology Foundation for Selected Overseas Chinese Scholar, Ministry of Personnel of China FX We thank Xindi Ai, Katie Lin, and Rummi Ganguly for proofreading this manuscript during revision. Lei Qu was partially supported by Chinese Natural Science Foundation Project (61201396, 61301296, 61377006, U1201255); Scientific Research Foundation for the Returned Overseas Chinese Scholars, State Education Ministry; and the Technology Foundation for Selected Overseas Chinese Scholar, Ministry of Personnel of China. NR 47 TC 8 Z9 8 U1 1 U2 8 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 1053-5888 EI 1558-0792 J9 IEEE SIGNAL PROC MAG JI IEEE Signal Process. Mag. PD JAN PY 2015 VL 32 IS 1 BP 70 EP 77 DI 10.1109/MSP.2014.2354060 PG 8 WC Engineering, Electrical & Electronic SC Engineering GA AW1IR UT WOS:000346043800013 ER PT J AU Christensen, GA Zane, GM Kazakov, AE Li, X Rodionov, DA Novichkov, PS Dubchak, I Arkin, AP Wall, JD AF Christensen, G. A. Zane, G. M. Kazakov, A. E. Li, X. Rodionov, D. A. Novichkov, P. S. Dubchak, I. Arkin, A. P. Wall, J. D. TI Rex (Encoded by DVU_0916) in Desulfovibrio vulgaris Hildenborough Is a Repressor of Sulfate Adenylyl Transferase and Is Regulated by NADH SO JOURNAL OF BACTERIOLOGY LA English DT Article ID DISSIMILATORY SULFITE REDUCTASE; PHENOL-CHLOROFORM EXTRACTION; SINGLE-STEP METHOD; REDUCING BACTERIA; BACILLUS-SUBTILIS; FAMILY REPRESSOR; RELATIVE QUANTIFICATION; ARCHAEOGLOBUS-FULGIDUS; CRYSTAL-STRUCTURE; RNA ISOLATION AB Although the enzymes for dissimilatory sulfate reduction by microbes have been studied, the mechanisms for transcriptional regulation of the encoding genes remain unknown. In a number of bacteria the transcriptional regulator Rex has been shown to play a key role as a repressor of genes producing proteins involved in energy conversion. In the model sulfate-reducing microbe Desulfovibrio vulgaris Hildenborough, the gene DVU_0916 was observed to resemble other known Rex proteins. Therefore, the DVU_0916 protein has been predicted to be a transcriptional repressor of genes encoding proteins that function in the process of sulfate reduction in D. vulgaris Hildenborough. Examination of the deduced DVU_0916 protein identified two domains, one a winged helix DNA-binding domain common for transcription factors, and the other a Rossman fold that could potentially interact with pyridine nucleotides. A deletion of the putative rex gene was made in D. vulgaris Hildenborough, and transcript expression studies of sat, encoding sulfate adenylyl transferase, showed increased levels in the D. vulgaris Hildenborough Rex (Rex(DvH)) mutant relative to the parental strain. The Rex(DvH)-binding site upstream of sat was identified, confirming RexDvH to be a repressor of sat. We established in vitro that the presence of elevated NADH disrupted the interaction between Rex(DvH) and DNA. Examination of the 5' transcriptional start site for the sat mRNA revealed two unique start sites, one for respiring cells that correlated with the Rex(DvH)-binding site and a second for fermenting cells. Collectively, these data support the role of RexDvH as a transcription repressor for sat that senses the redox status of the cell. C1 [Christensen, G. A.; Zane, G. M.; Wall, J. D.] Univ Missouri, Dept Biochem, Columbia, MO 65211 USA. [Christensen, G. A.; Zane, G. M.; Kazakov, A. E.; Novichkov, P. S.; Dubchak, I.; Arkin, A. P.; Wall, J. D.] Ecosyst & Networks Integrated Genes & Mol Assembl, Berkeley, CA USA. [Kazakov, A. E.; Novichkov, P. S.; Dubchak, I.; Arkin, A. P.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA 94720 USA. [Li, X.; Rodionov, D. A.] Sanford Burnham Med Res Inst, La Jolla, CA USA. [Rodionov, D. A.] Russian Acad Sci, AA Kharkevich Inst Informat Transmiss Problems, Moscow, Russia. RP Wall, JD (reprint author), Univ Missouri, Dept Biochem, Columbia, MO 65211 USA. EM wallj@missouri.edu RI Arkin, Adam/A-6751-2008; OI Arkin, Adam/0000-0002-4999-2931; Christensen, Geoffrey/0000-0003-1360-0729 FU Office of Science, Office of Biological and Environmental Research, of the U.S. Department of Energy [DE-AC02- 05CH11231] FX This research, conducted by ENIGMA-Ecosystems and Networks Integrated with Genes and Molecular Assemblies (http://enigma.lbl.gov/), a Scientific Focus Area Program at Lawrence Berkeley National Laboratory, was supported by the Office of Science, Office of Biological and Environmental Research, of the U.S. Department of Energy under contract DE-AC02- 05CH11231. NR 49 TC 4 Z9 5 U1 4 U2 14 PU AMER SOC MICROBIOLOGY PI WASHINGTON PA 1752 N ST NW, WASHINGTON, DC 20036-2904 USA SN 0021-9193 EI 1098-5530 J9 J BACTERIOL JI J. Bacteriol. PD JAN PY 2015 VL 197 IS 1 BP 29 EP 39 DI 10.1128/JB.02083-14 PG 11 WC Microbiology SC Microbiology GA AW1KP UT WOS:000346048700006 PM 25313388 ER PT J AU Killikelly, A Benson, MA Ohneck, EA Sampson, JM Jakoncic, J Spurrier, B Torres, VJ Kong, XP AF Killikelly, April Benson, Meredith A. Ohneck, Elizabeth A. Sampson, Jared M. Jakoncic, Jean Spurrier, Brett Torres, Victor J. Kong, Xiang-Peng TI Structure-Based Functional Characterization of Repressor of Toxin (Rot), a Central Regulator of Staphylococcus aureus Virulence SO JOURNAL OF BACTERIOLOGY LA English DT Article ID ANTIMICROBIAL SURVEILLANCE PROGRAM; GLOBAL REGULATOR; GENE-EXPRESSION; UNITED-STATES; IN-VIVO; RNAIII; AGR; DNA; PROTEINS; IDENTIFICATION AB Staphylococcus aureus is responsible for a large number of diverse infections worldwide. In order to support its pathogenic lifestyle, S. aureus has to regulate the expression of virulence factors in a coordinated fashion. One of the central regulators of the S. aureus virulence regulatory networks is the transcription factor repressor of toxin (Rot). Rot plays a key role in regulating S. aureus virulence through activation or repression of promoters that control expression of a large number of critical virulence factors. However, the mechanism by which Rot mediates gene regulation has remained elusive. Here, we have determined the crystal structure of Rot and used this information to probe the contribution made by specific residues to Rot function. Rot was found to form a dimer, with each monomer harboring a winged helix-turn-helix (WHTH) DNA-binding motif. Despite an overall acidic pI, the asymmetric electrostatic charge profile suggests that Rot can orient the WHTH domain to bind DNA. Structure-based site-directed mutagenesis studies demonstrated that R-91, at the tip of the wing, plays an important role in DNA binding, likely through interaction with the minor groove. We also found that Y-66, predicted to bind within the major groove, contributes to Rot interaction with target promoters. Evaluation of Rot binding to different activated and repressed promoters revealed that certain mutations on Rot exhibit promoter-specific effects, suggesting for the first time that Rot differentially interacts with target promoters. This work provides insight into a precise mechanism by which Rot controls virulence factor regulation in S. aureus. C1 [Killikelly, April; Sampson, Jared M.; Spurrier, Brett; Kong, Xiang-Peng] NYU, Sch Med, Dept Mol Pharmacol & Biochem, New York, NY 10016 USA. [Benson, Meredith A.; Ohneck, Elizabeth A.; Torres, Victor J.] NYU, Sch Med, Dept Microbiol, New York, NY 10016 USA. [Jakoncic, Jean] Brookhaven Natl Lab, Photon Sci Directorate, Upton, NY 11973 USA. RP Torres, VJ (reprint author), NYU, Sch Med, Dept Microbiol, New York, NY 10016 USA. EM Victor.Torres@nyumc.org; Xiangpeng.Kong@med.nyu.edu OI Kong, Xiang-Peng/0000-0001-5773-2681; Torres, Victor/0000-0002-7126-0489 FU National Science and Engineering Research Council of Canada; National Institute of Allergy and Infectious Diseases of the National Institutes of Health [R21AI101533]; NIH training grant [GM088118] FX Research reported in this publication was supported in part by funds of a Graduate Research Fellowship to A.K. from the National Science and Engineering Research Council of Canada and by the National Institute of Allergy and Infectious Diseases of the National Institutes of Health under award number R21AI101533 to V.J.T. B.S. was supported by NIH training grant GM088118. V.J.T. is a Burroughs Wellcome Fund Investigator in the Pathogenesis of Infectious Diseases. NR 57 TC 3 Z9 3 U1 9 U2 26 PU AMER SOC MICROBIOLOGY PI WASHINGTON PA 1752 N ST NW, WASHINGTON, DC 20036-2904 USA SN 0021-9193 EI 1098-5530 J9 J BACTERIOL JI J. Bacteriol. PD JAN PY 2015 VL 197 IS 1 BP 188 EP 200 DI 10.1128/JB.02317-14 PG 13 WC Microbiology SC Microbiology GA AW1KP UT WOS:000346048700021 PM 25331435 ER PT J AU Laprade, EJ Liaw, CY Jiang, Z Shull, KR AF Laprade, Evan J. Liaw, Chya-Yan Jiang, Zhang Shull, Kenneth R. TI Mechanical and Microstructural Characterization of Sulfonated Pentablock Copolymer Membranes SO JOURNAL OF POLYMER SCIENCE PART B-POLYMER PHYSICS LA English DT Article DE block copolymers; creep; membranes ID PROTON-EXCHANGE MEMBRANES; CREEP AB Creep experiments utilizing a membrane inflation geometry were used to characterize the mechanical properties of pentablock copolymer membranes designed for water purification applications. Membranes were formed by casting from micellar solutions, and structure development during the casting process was followed in real time with grazing incidence small angle X-ray scattering. The thin film morphologies were consistent with previously published results obtained for much thicker solvent cast films. The biaxial creep compliance of the films for applied stresses in the megapascal range increased substantially as the degree of sulfonation and consequent hydration of the middle block was increased. The sulfonation level was much more important than the overall degree of ordering in determining the creep compliance of the hydrated membranes. (C) 2014 Wiley Periodicals, Inc. C1 [Laprade, Evan J.; Liaw, Chya-Yan; Shull, Kenneth R.] Northwestern Univ, Dept Mat Sci & Engn, Evanston, IL 60208 USA. [Liaw, Chya-Yan; Jiang, Zhang] Argonne Natl Lab, Adv Photon Source, Xray Sci Div, Argonne, IL 60439 USA. RP Shull, KR (reprint author), Northwestern Univ, Dept Mat Sci & Engn, Evanston, IL 60208 USA. EM k-shull@northwestern.edu RI Jiang, Zhang/A-3297-2012; Shull, Kenneth/B-7536-2009 OI Jiang, Zhang/0000-0003-3503-8909; FU U.S. DOE [DE-AC02-06CH11357] FX Use of the Advanced Photon Source, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science by Argonne National Laboratory, was supported by the U.S. DOE under Contract No. DE-AC02-06CH11357. Nexar solutions were kindly provided by Dr. Carl Willis at Kraton Polymers. NR 22 TC 4 Z9 4 U1 2 U2 22 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0887-6266 EI 1099-0488 J9 J POLYM SCI POL PHYS JI J. Polym. Sci. Pt. B-Polym. Phys. PD JAN 1 PY 2015 VL 53 IS 1 BP 39 EP 47 DI 10.1002/polb.23623 PG 9 WC Polymer Science SC Polymer Science GA AW1XA UT WOS:000346080500003 ER PT J AU Gong, CH Zhang, Y Shankaran, H Resat, H AF Gong, Chunhong Zhang, Yi Shankaran, Harish Resat, Haluk TI Integrated analysis reveals that STAT3 is central to the crosstalk between HER/ErbB receptor signaling pathways in human mammary epithelial cells SO MOLECULAR BIOSYSTEMS LA English DT Article ID EPIDERMAL-GROWTH-FACTOR; MODULAR RESPONSE ANALYSIS; ACTIVATED PROTEIN-KINASE; BREAST-CANCER CELLS; LUNG-CANCER; ERBB RECEPTORS; EGF-RECEPTOR; PHOSPHATIDYLINOSITOL 3-KINASE; DEPENDENT ACTIVATION; P38 MAPK AB Human epidermal growth factor receptors (HER, also known as ErbB) drive cellular proliferation, pro-survival and stress responses by activating several downstream kinases, in particular ERK, p38 MAPK, JNK (SAPK), the PI3K/AKT, as well as various transcriptional regulators such as STAT3. When co-expressed, the first three members of HER family (HER1-3) can form homo- and hetero-dimers, and there is considerable evidence suggesting that the receptor dimers differentially activate intracellular signaling pathways. To better understand the interactions in this system, we pursued multi-factorial experiments where HER dimerization patterns and signaling pathways were rationally perturbed. We measured the activation of HER1-3 receptors and of the sentinel signaling proteins ERK, AKT, p38 MAPK, JNK, STAT3 as a function of time in a panel of human mammary epithelial (HME) cells expressing different levels of HER1-3 stimulated with various ligand combinations. We hypothesized that the HER dimerization pattern is a better predictor of downstream signaling than the total receptor activation levels. We validated this hypothesis using a combination of model-based analysis to quantify the HER dimerization patterns, and by clustering the activation data in multiple ways to confirm that the HER receptor dimer is a better predictor of the signaling through p38 MAPK, ERK and AKT pathways than the total HER receptor expression and activation levels. We then pursued combinatorial inhibition studies to identify the causal regulatory interactions between sentinel signaling proteins. Quantitative analysis of the collected data using the modular response analysis (MRA) and its Bayesian Variable Selection Algorithm (BVSA) version allowed us to obtain a consensus regulatory interaction model, which revealed that STAT3 occupies a central role in the crosstalk between the studied pathways in HME cells. Results of the BVSA/MRA and cluster analysis were in agreement with each other. C1 [Gong, Chunhong; Zhang, Yi; Shankaran, Harish; Resat, Haluk] Pacific NW Natl Lab, Computat Biol & Bioinformat Grp, Richland, WA 99352 USA. [Resat, Haluk] Washington State Univ, Sch Chem Engn & Bioengn, Pullman, WA 99164 USA. [Resat, Haluk] Washington State Univ, Sch Elect Engn & Comp Sci, Pullman, WA 99164 USA. RP Resat, H (reprint author), Washington State Univ, Sch Chem Engn & Bioengn, POB 646515, Pullman, WA 99164 USA. EM haluk.resat@wsu.edu FU National Institutes of Health [5R01GM072821-07]; U.S. Department of Energy [DE-AC06-76RL01830] FX The research described in this paper was funded by the National Institutes of Health Grant 5R01GM072821-07 to H.R. Pacific Northwest National Laboratory is a multiprogram national laboratory operated by Battelle for the U.S. Department of Energy under Contract DE-AC06-76RL01830. NR 96 TC 2 Z9 2 U1 0 U2 8 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1742-206X EI 1742-2051 J9 MOL BIOSYST JI Mol. Biosyst. PD JAN PY 2015 VL 11 IS 1 BP 146 EP 158 DI 10.1039/c4mb00471j PG 13 WC Biochemistry & Molecular Biology SC Biochemistry & Molecular Biology GA AU9FQ UT WOS:000345897600014 PM 25315124 ER PT J AU Carmona, C Langan, P Smith, JC Petridis, L AF Carmona, Christopher Langan, Paul Smith, Jeremy C. Petridis, Loukas TI Why genetic modification of lignin leads to low-recalcitrance biomass SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID CINNAMYL ALCOHOL-DEHYDROGENASE; MOLECULAR-DYNAMICS SIMULATION; BOND-DISSOCIATION ENTHALPIES; PARTICLE MESH EWALD; FORCE-FIELD; DOWN-REGULATION; CELL-WALLS; MODEL; BIOSYNTHESIS; ARABIDOPSIS AB Genetic modification of plants via down-regulation of cinnamyl alcohol dehydrogenase leads to incorporation of aldehyde groups in the lignin polymer. The resulting lignocellulosic biomass has increased bioethanol yield. However, a molecular-scale explanation of this finding is currently lacking. Here, we perform molecular dynamics simulation of the copolymer with hemicellulose of wild type and the genetically modified lignin, in aqueous solution. We find that the non-covalent association with hemicellulose of lignin containing aldehyde groups is reduced compared to the wild-type. This phase separation may increase the cell wall porosity in the mutant plants, thus explaining their easier deconstruction to biofuels. The thermodynamic origin of the reduced lignin-hemicellulose association is found to be a more favorable self-interaction energy and less favorable interaction with hemicellulose for the mutant lignin. Furthermore, reduced hydration water density fluctuations are found for the mutant lignin, implying a more hydrophobic lignin surface. The results provide a detailed description of how aldehyde incorporation makes lignin more hydrophobic and reduces its association with hemicellulose, thus suggesting that increased lignin hydrophobicity may be an optimal characteristic required for improved biofuel production. C1 [Carmona, Christopher] Univ Calif Los Angeles, Los Angeles, CA 90095 USA. [Carmona, Christopher; Smith, Jeremy C.; Petridis, Loukas] Oak Ridge Natl Lab, Ctr Biophys Mol, Oak Ridge, TN 37831 USA. [Langan, Paul] Biol & Soft Matter Div, Oak Ridge, TN 37831 USA. [Smith, Jeremy C.] Univ Tennessee, Dept Biochem & Cellular & Mol Biol, Knoxville, TN 37996 USA. RP Petridis, L (reprint author), Oak Ridge Natl Lab, Ctr Biophys Mol, Oak Ridge, TN 37831 USA. EM petridisl@ornl.gov RI Langan, Paul/N-5237-2015; smith, jeremy/B-7287-2012; Petridis, Loukas/B-3457-2009 OI Langan, Paul/0000-0002-0247-3122; smith, jeremy/0000-0002-2978-3227; Petridis, Loukas/0000-0001-8569-060X FU BioEnergy Science Center; U.S. Department of Energy (DOE) Bioenergy Research Center; Office of Biological and Environmental Research in the DOE Office of Science; Office of Science of the U.S. Department of Energy [DE-AC05-00OR22725] FX We thank Drs Brian H. Davison and Amandeep Sangha for useful discussions. This research is funded by the BioEnergy Science Center, a U.S. Department of Energy (DOE) Bioenergy Research Center supported by the Office of Biological and Environmental Research in the DOE Office of Science. This research used resources of the Oak Ridge Leadership Computing Facility at the Oak Ridge National Laboratory, which is supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC05-00OR22725. NR 53 TC 5 Z9 6 U1 1 U2 35 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2015 VL 17 IS 1 BP 358 EP 364 DI 10.1039/c4cp05004e PG 7 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AW4FD UT WOS:000346235600037 PM 25384960 ER PT J AU Pham, HH Wang, LW AF Pham, Hieu H. Wang, Lin-Wang TI Oxygen vacancy and hole conduction in amorphous TiO2 SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID DENSITY-FUNCTIONAL THEORY; CATHODIC VACUUM-ARC; TITANIUM-DIOXIDE; RUTILE TIO2; STRUCTURAL-PROPERTIES; MOLECULAR-DYNAMICS; PLUS U; FILMS; ELECTRON; ANATASE AB The amorphous titanium dioxide (a-TiO2) has drawn attention recently due to the finding that it holds promise for coating conventional photoelectrodes for corrosion protection while still allowing the holes to transport to the surface. The mechanism of hole conductivity at a level much higher than the edge of the valence band is still a mystery. In this work, an amorphous TiO2 model is obtained from molecular dynamics employing the "melt-and-quench'' technique. The electronic properties, polaronic states and the hole conduction mechanism in amorphous structure were investigated by means of density functional theory with Hubbard's energy correction (DFT + U) and compared to those in crystalline (rutile) TiO2. The formation energy of the oxygen vacancy was found to reduce significantly (by a few eV) upon amorphization. Our theoretical study suggested that the oxygen vacancies and their defect states provide hopping channels, which are comparable to experimental observations and could be responsible for hole conduction in the "leaky'' TiO2 recently discovered for the photochemical water-splitting applications. C1 [Wang, Lin-Wang] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Joint Ctr Artificial Photosynthesis, Berkeley, CA 94720 USA. Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. RP Wang, LW (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Joint Ctr Artificial Photosynthesis, Berkeley, CA 94720 USA. EM lwwang@lbl.gov RI Pham, Hieu/C-6436-2015 FU Office of Science of the U.S. Department of Energy [DE-SC0004993] FX We would like to thank Dr S. Hu for very helpful discussions. This material is based on the work performed by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the U.S. Department of Energy under Award number DE-SC0004993. We use the resource of National Energy Research Scientific Computing center (NERSC) located in the Lawrence Berkeley National Laboratory. NR 71 TC 32 Z9 32 U1 25 U2 137 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2015 VL 17 IS 1 BP 541 EP 550 DI 10.1039/c4cp04209c PG 10 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AW4FD UT WOS:000346235600058 PM 25406575 ER PT J AU Clikeman, TT Deng, SHM Popov, AA Wang, XB Strauss, SH Boltalina, OV AF Clikeman, Tyler T. Deng, Shihu H. M. Popov, Alexey A. Wang, Xue-Bin Strauss, Steven H. Boltalina, Olga V. TI Fullerene cyanation does not always increase electron affinity: an experimental and theoretical study SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID BASIS-SETS; ACCEPTORS; ISOMERS; DENSITY; C60F36; DERIVATIVES; RADICALS; EXCHANGE; DIAMOND; C-60 AB The electron affinities of C-70 derivatives with trifluoromethyl, methyl and cyano groups were studied experimentally and theoretically using low-temperature photoelectron spectroscopy (LT PES) and density functional theory (DFT). The electronic effects of these functional groups were determined and found to be highly dependent on the addition patterns. Substitution of CF3 for CN for the same addition pattern increases the experimental electron affinity by 70 meV per substitution. The synthesis of a new fullerene derivative, C-70(CF3)(10)(CN)(2), is reported for the first time. C1 [Clikeman, Tyler T.; Strauss, Steven H.; Boltalina, Olga V.] Colorado State Univ, Dept Chem, Ft Collins, CO 80523 USA. [Deng, Shihu H. M.; Wang, Xue-Bin] Pacific NW Natl Lab, Div Phys Sci, Richland, WA 99352 USA. [Popov, Alexey A.] Leibniz Inst Solid State & Mat Res, Dept Elect & Conducting Polymers, D-01069 Dresden, Germany. RP Popov, AA (reprint author), Leibniz Inst Solid State & Mat Res, Dept Elect & Conducting Polymers, D-01069 Dresden, Germany. EM steven.strauss@colostate.edu; olga.boltalina@colostate.edu RI Popov, Alexey/A-9937-2011 OI Popov, Alexey/0000-0002-7596-0378 FU U.S [NSF/CHE-1362302, NSF/CHE-1346572]; National Institute of Health [R21CA140080]; Colorado State University Research Foundation; US Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences Biosciences; US Department of Energy's Office of Biological and Environmental Research; DFG [PO 1602/1-1] FX We thank the U.S. NSF/CHE-1362302, NSF/CHE-1346572, National Institute of Health (grant R21CA140080), and the Colorado State University Research Foundation for partial financial support. The LT PES work was supported by the US Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences & Biosciences (X.-B.W.) and was performed at EMSL, a national scientific user facility sponsored by the US Department of Energy's Office of Biological and Environmental Research and located at PNNL. Popov acknowledges DFG (PO 1602/1-1) for financial support. The Research Computing Center of the Moscow State University is gratefully acknowledged for the computational facilities at the supercomputer "Chebyshev SKIF-MSU''.32 NR 39 TC 3 Z9 3 U1 2 U2 28 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2015 VL 17 IS 1 BP 551 EP 556 DI 10.1039/c4cp04287e PG 6 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AW4FD UT WOS:000346235600059 PM 25407600 ER PT J AU Yu, R Chong, XY Jiang, YH Zhou, R Yuan, W Feng, J AF Yu, Ran Chong, Xiaoyu Jiang, Yehua Zhou, Rong Yuan, Wen Feng, Jing TI The stability, electronic structure, elastic and metallic properties of manganese nitrides SO RSC ADVANCES LA English DT Article ID 1ST-PRINCIPLES CALCULATIONS; MAGNETIC-PROPERTIES; THERMAL-PROPERTIES; CRYSTAL-STRUCTURE; 1ST PRINCIPLES; NB; COMPOUND; NACL; TA; ZR AB The phase stability, electronic structure, elastic and metallic properties of manganese nitrides (Mn4N, Mn2N0.86, Mn3N2, and MnN) were extensively studied by first principles calculations. The negative values of cohesive energy and formation enthalpy show that these compounds are thermodynamically stable. The bonding of Manganese nitrides is the combinations of covalent and metallic bonds. In addition, a strong hybridization exists nearby the Fermi level, being characteristic of N-p and Mn-d states. The elastic properties of these nitrides (Mn4N, Mn2N0.86, and MnN) were calculated, which included bulk modulus, shear modulus, Young's modulus, Poisson's ratio, and hardness. The calculated results reveal that Mn2N0.86 and MnN are ductile while Mn4N is brittle, and the hardness values of these nitrides are 24.35 GPa, 12.01 GPa, and 17.06 GPa, respectively. The MnN compound has the highest Debye temperature (632.1 K), while Mn2N0.86 has the lowest Debye temperature (390.5 K). The anisotropy of Young's modulus for Mn4N and MnN compounds is more prominent than Mn2N0.86 at the three crystalline planes. Moreover, the compound of Mn3N2 has an unstable structure in mechanical stability. C1 [Yu, Ran; Chong, Xiaoyu; Jiang, Yehua; Zhou, Rong] Kunming Univ Sci & Technol, Fac Mat Sci & Engn, Kunming 650093, Peoples R China. [Feng, Jing] Harvard Univ, Sch Engn & Appl Sci, Cambridge, MA 02138 USA. [Yuan, Wen] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. RP Jiang, YH (reprint author), Kunming Univ Sci & Technol, Fac Mat Sci & Engn, Kunming 650093, Peoples R China. EM jiangyehua@kmust.edu.cn; jfeng@seas.harvard.edu RI Yuan, Wen/G-7141-2015 OI Yuan, Wen/0000-0002-1812-9588 FU National Natural Science Foundation [51171074, 51261013] FX This work is supported by National Natural Science Foundation (no.: 51171074 and 51261013). NR 26 TC 9 Z9 9 U1 15 U2 79 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2046-2069 J9 RSC ADV JI RSC Adv. PY 2015 VL 5 IS 2 BP 1620 EP 1627 DI 10.1039/c4ra10914g PG 8 WC Chemistry, Multidisciplinary SC Chemistry GA AW1WT UT WOS:000346079900097 ER PT J AU Pan, JJ Cheng, XL Sharp, M Ho, CS Khadka, N Katsaras, J AF Pan, Jianjun Cheng, Xiaolin Sharp, Melissa Ho, Chian-Sing Khadka, Nawal Katsaras, John TI Structural and mechanical properties of cardiolipin lipid bilayers determined using neutron spin echo, small angle neutron and X-ray scattering, and molecular dynamics simulations SO SOFT MATTER LA English DT Article ID PARTICLE MESH EWALD; CONSTANT-PRESSURE; FLUID BILAYER; FORCE-FIELD; MEMBRANES; TEMPERATURE; ORGANIZATION; CHOLESTEROL; DIFFRACTION; ELASTICITY AB The detailed structural and mechanical properties of a tetraoleoyl cardiolipin (TOCL) bilayer were determined using neutron spin echo (NSE) spectroscopy, small angle neutron and X-ray scattering (SANS and SAXS, respectively), and molecular dynamics (MD) simulations. We used MD simulations to develop a scattering density profile (SDP) model, which was then utilized to jointly refine SANS and SAXS data. In addition to commonly reported lipid bilayer structural parameters, component distributions were obtained, including the volume probability, electron density and neutron scattering length density. Of note, the distance between electron density maxima D-HH (39.4 angstrom) and the hydrocarbon chain thickness 2D(C) (29.1 angstrom) of TOCL bilayers were both found to be larger than the corresponding values for dioleoyl phosphatidylcholine (DOPC) bilayers. Conversely, TOCL bilayers have a smaller overall bilayer thickness D-B (36.7 angstrom), primarily due to their smaller headgroup volume per phosphate. SDP analysis yielded a lipid area of 129.8 angstrom(2), indicating that the cross-sectional area per oleoyl chain in TOCL bilayers (i.e., 32.5 angstrom(2)) is smaller than that for DOPC bilayers. Multiple sets of MD simulations were performed with the lipid area constrained at different values. The calculated surface tension versus lipid area resulted in a lateral area compressibility modulus K-A of 342 mN m(-1), which is slightly larger compared to DOPC bilayers. Model free comparison to experimental scattering data revealed the best simulated TOCL bilayer from which detailed molecular interactions were determined. Specifically, Na+ cations were found to interact most strongly with the glycerol hydroxyl linkage, followed by the phosphate and backbone carbonyl oxygens. Inter-and intra-lipid interactions were facilitated by hydrogen bonding between the glycerol hydroxyl and phosphate oxygen, but not with the backbone carbonyl. Finally, analysis of the intermediate scattering functions from NSE spectroscopy measurements of TOCL bilayers yielded a bending modulus K-C of 1.06 x 10(-19) J, which was larger than that observed in DOPC bilayers. Our results show the physicochemical properties of cardiolin bilayers that may be important in explaining their functionality in the inner mitochondrial membrane. C1 [Pan, Jianjun; Ho, Chian-Sing; Khadka, Nawal] Univ S Florida, Dept Phys, Tampa, FL 33620 USA. [Cheng, Xiaolin] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. [Cheng, Xiaolin] Univ Tennessee, Dept Biochem & Cellular & Mol Biol, Knoxville, TN 37996 USA. [Sharp, Melissa] European Spallat Source ESS AB, Lund, Sweden. [Katsaras, John] Oak Ridge Natl Lab, Neutron Sci Directorate, Oak Ridge, TN 37831 USA. [Katsaras, John] Univ Tennessee, Dept Phys & Astron, Knoxville, TN 37996 USA. [Katsaras, John] Oak Ridge Natl Lab, Joint Inst Neutron Sci, Oak Ridge, TN 37831 USA. RP Pan, JJ (reprint author), Univ S Florida, Dept Phys, Tampa, FL 33620 USA. EM panj@usf.edu; katsarasj@ornl.gov OI Katsaras, John/0000-0002-8937-4177 FU Scientific User Facilities Division, Office of Basic Energy Sciences, US Department of Energy [IPTS 7168, IPTS 5975, IPTS 6192]; NSF; NIH/NIGMS via NSF [DMR-1332208]; Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]; Scientific User Facilities Division of the DOE Office of Basic Energy Sciences (BES); Laboratory Directed Research and Development Program of Oak Ridge National Laboratory (ORNL); U.S. Department of Energy (DOE) [DE-AC05-00OR2275]; University of South Florida FX Part of the research conducted at ORNL's High Flux Isotope Reactor (IPTS 7168) and Spallation Neutron Source (IPTS 5975 and IPTS 6192) was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, US Department of Energy. CHESS is supported by the NSF & NIH/NIGMS via NSF award DMR-1332208. Part of the computation used the resources of the National Energy Research Scientific Computing Center, which is supported by the Office of Science of the U.S. Department of Energy under Contract no. DE-AC02-05CH11231. J. Katsaras is supported through the Scientific User Facilities Division of the DOE Office of Basic Energy Sciences (BES), and from the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory (ORNL), managed by UT-Battelle, LLC, for the U.S. Department of Energy (DOE) under contract no. DE-AC05-00OR2275. J. Pan is supported by a startup fund from the University of South Florida. NR 60 TC 11 Z9 11 U1 4 U2 41 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1744-683X EI 1744-6848 J9 SOFT MATTER JI Soft Matter PY 2015 VL 11 IS 1 BP 130 EP 138 DI 10.1039/c4sm02227k PG 9 WC Chemistry, Physical; Materials Science, Multidisciplinary; Physics, Multidisciplinary; Polymer Science SC Chemistry; Materials Science; Physics; Polymer Science GA AW0KD UT WOS:000345980100013 PM 25369786 ER EF