FN Thomson Reuters Web of Science™ VR 1.0 PT S AU Doppner, T Kritcher, AL Kraus, D Glenzer, SH Bachmann, BL Chapman, D Collins, GW Falcone, RW Hawreliak, J Landen, OL Lee, HJ Le Pape, S Ma, T Neumayer, P Redmer, R Swift, DC AF Doeppner, T. Kritcher, A. L. Kraus, D. Glenzer, S. H. Bachmann, B. L. Chapman, D. Collins, G. W. Falcone, R. W. Hawreliak, J. Landen, O. L. Lee, H. J. Le Pape, S. Ma, T. Neumayer, P. Redmer, R. Swift, D. C. BE Buttler, W Furlanetto, M Evans, W TI X-ray Thomson scattering as a temperature probe for Gbar shock experiments SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID NATIONAL IGNITION FACILITY AB In X-ray Thomson scattering (XRTS), spectrally-resolved spectrometry of probe x-rays scattered from matter gives an elastic (ionic) and an inelastic (electronic) feature, whose location, width, and amplitude can be analyzed for electron density and temperature. This diagnostic is complementary to traditional, mechanical EOS measurements which do not directly constrain temperature. XRTS has been demonstrated on planar dynamic-loading experiments at the Omega laser, and a spectrometer has been constructed for use at the National Ignition Facility (NIF). We plan to obtain XRTS measurements into the Gbar regime using hohlraum-driven converging shocks at NIF. In these experiments, the radial profile through the sample at any instant of time varies greatly, though the XRTS signal is dominated by the densest region, which is close to the shock front where simultaneous radiography obtains an EOS measurement. C1 [Doeppner, T.; Kritcher, A. L.; Bachmann, B. L.; Collins, G. W.; Hawreliak, J.; Landen, O. L.; Le Pape, S.; Ma, T.; Swift, D. C.] Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. [Kraus, D.; Falcone, R. W.] Univ Calif Berkeley, Berkeley, CA 94720 USA. [Glenzer, S. H.; Lee, H. J.] SLAC Natl Accelerator Lab, Menlo Pk, CA 94025 USA. [Chapman, D.] AWE plc, Plasma Phys Grp, Reading RG7 4PR, Berks, England. [Falcone, R. W.] Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Neumayer, P.] Gesell Schwerionenphys, Darmstadt, Germany. [Redmer, R.] Univ Rostock, D-18051 Rostock, Germany. RP Doppner, T (reprint author), Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. EM doeppner1@llnl.gov RI lepape, sebastien/J-3010-2015 FU U. S. Department of Energy by Lawrence Livermore National Laboratory [DE- AC52- 07NA27344]; Laboratory Directed Research and Development [13- ERD- 073]; SSAA program [DE- FG52- 06NA26212] FX This work performed under the auspices of the U. S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE- AC52- 07NA27344 and supported by Laboratory Directed Research and Development Grant No. 13- ERD- 073. RWF acknowledges support from SSAA program Contract No. DE- FG52- 06NA26212. Special thanks go to Scott Burns and Allen house who designed and built the MACS spectrometer, and to Dan Kalantar, Tom McCarvillle and Reg Wood who worked out critically important alignment procedures. NR 17 TC 11 Z9 11 U1 3 U2 22 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR UNSP 192019 DI 10.1088/1742-6596/500/19/192019 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900310 ER PT S AU Erskine, DJ Smith, RF Bolme, C Ali, S Celliers, PM Collins, GW AF Erskine, David J. Smith, R. F. Bolme, C. Ali, S. Celliers, P. M. Collins, G. W. BE Buttler, W Furlanetto, M Evans, W TI Numerical refocusing of 2d-VISAR data SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID INTERFEROMETER AB Two dimensional velocity interferometer (2d-VISAR) data can be treated as a kind of hologram, since fringes recorded by the interferometer manifest both phase and magnitude information about changes in the optical field of the target, over an image. By the laws of diffraction, knowledge of the optical field at one focal plane can be used to calculate the optical field at another focal plane. Hence a numerical re-focusing operation can be performed on the data post-experiment, which can bring into focus narrow features that were recorded in an out of focus configuration. Demonstration on shocked Si data is shown. C1 [Erskine, David J.; Smith, R. F.; Celliers, P. M.; Collins, G. W.] Lawrence Livermore Natl Lab, POB 808, Livermore, CA 94551 USA. [Bolme, C.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Ali, S.] Univ Calif Berkeley, Dept Earth & Planetary Sci, Berkeley, CA 94720 USA. RP Erskine, DJ (reprint author), Lawrence Livermore Natl Lab, POB 808, Livermore, CA 94551 USA. EM erskine1@llnl.gov OI Bolme, Cynthia/0000-0002-1880-271X FU U.S. Department of Energy by Lawrence Livermore National Laboratory [DE-AC52-07NA27344] FX This work performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344. NR 15 TC 1 Z9 1 U1 2 U2 8 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR UNSP 142013 DI 10.1088/1742-6596/500/14/142013 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900193 ER PT S AU Fensin, SJ Valone, SM Cerreta, EK Gray, GT AF Fensin, S. J. Valone, S. M. Cerreta, E. K. Gray, G. T., III BE Buttler, W Furlanetto, M Evans, W TI Predicting failure stress for grain boundaries using average and local properties SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID DYNAMIC FRACTURE; INTERFACES; METALS; ENERGY; COPPER; NUCLEATION; STRENGTH; BEHAVIOR; SOLIDS; MODELS AB Several factors can affect the failure stress of a grain boundary, such as grain boundary structure, energy and excess volume, in addition to its interactions with dislocations. In this paper, we focus on the influence of grain boundary energy, excess volume and plasticity at the boundary on the failure stress of a grain boundary, in copper from molecular-dynamics simulations. Flyer plate simulations were carried out for four boundary types with different energies and excess volumes. These boundaries were chosen as model systems to represent various boundaries observed in "real" materials. Simulations indicate that there is no direct correlation between the void nucleation stress of a boundary and either its energy and excess volume. This result suggests that average properties of grain boundaries alone are not sufficient indicators of the failure strength of a boundary. However, local boundary properties related to the ability of a grain boundary to undergo plastic deformation are better markers of its strength. C1 [Fensin, S. J.; Valone, S. M.; Cerreta, E. K.; Gray, G. T., III] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Fensin, SJ (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM saryuj@lanl.gov NR 28 TC 0 Z9 0 U1 0 U2 5 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 112024 DI 10.1088/1742-6596/500/11/112024 PG 5 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900126 ER PT S AU Francois, EG Morris, JS Lieber, M AF Francois, E. G. Morris, J. S. Lieber, M. BE Buttler, W Furlanetto, M Evans, W TI Three dimensional hemispherical test development to evaluate detonation wave breakout SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing AB The Onionskin test has been the standard test to evaluate detonation wave breakout over a hemispherical surface for decades. It has been an effective test used in a variety of applications to qualify main charge materials, evaluate different boosters, and compare different detonators. It is not without its shortfalls however. It only images a small portion of the explosive and requires very precise alignment and camera requirements to make sense of the results. Asymmetry in explosive behavior cannot be pinpointed or evaluated effectively. We have developed a new diagnostic using fiber optics covering the surface of the explosive to yield a 3D representation of the detonation wave behavior. Precise timing mapping of the detonation over the hemispherical surface is generated which can be converted to detonation wave breakout behavior using Huygens' wave reconstruction. This report will include the results of a recent suite of tests on PBX 9501, and discussion of how the test was developed for this explosive and contrasting previous work on PBX 9502. The results of these tests will describe the effects on detonation wave breakout symmetry when Sylgard 184 is placed between the detonator and booster. The effects on symmetry and timing when the Sylgard gap thickness is increased and the detonator is canted will be shown. C1 [Francois, E. G.; Morris, J. S.; Lieber, M.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Francois, EG (reprint author), Los Alamos Natl Lab, WX 7, Los Alamos, NM 87545 USA. EM elizabethf@lanl.gov NR 7 TC 0 Z9 0 U1 0 U2 1 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 142015 DI 10.1088/1742-6596/500/14/142015 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900195 ER PT S AU Fredenburg, DA Koller, DD AF Fredenburg, D. A. Koller, D. D. BE Buttler, W Furlanetto, M Evans, W TI Interpreting the shock response of porous oxide systems SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID EQUATION; HUGONIOT; MODEL; STATE AB An energy based model is developed to described the shock compression response of phase transitioning porous materials. Assuming the solid and porous materials transform to the same high pressure phase (HPP), the shock response of the solid material is used to define the energy limits E-1, the energy at which the shocked solid begins to deviate from the Hugoniot of the low pressure phase, and E-2, the energy at which the shocked solid begins to asymptote to the equilibrium HPP. With the Hugoniot of the HPP solid known, the porous Hugoniot is calculated using an isobaric (constant pressure) approach, with at present two variable parameters. The parameters are the thermodynamic value of the initial Gruneisen constant, gamma(0), and the yield/transition strength parameter, sigma(Y). The approach is demonstrated for several different initial distentions of SiO2. C1 [Fredenburg, D. A.; Koller, D. D.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Fredenburg, DA (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM dafreden@lanl.gov; ddennis@lanl.gov NR 15 TC 0 Z9 0 U1 0 U2 1 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 112025 DI 10.1088/1742-6596/500/11/112025 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900127 ER PT S AU Garcia, F Vandersall, KS Tarver, CM AF Garcia, Frank Vandersall, Kevin S. Tarver, Craig M. BE Buttler, W Furlanetto, M Evans, W TI Shock initiation experiments with ignition and growth modeling on low density HMX SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID MANGANIN AB Shock initiation experiments on low density (similar to 1.2 and similar to 1.6 g/cm(3)) HMX were performed to obtain in-situ pressure gauge data, characterize the run-distance-to-detonation behavior, and provide a basis for Ignition and Growth reactive flow modeling. A 101 mm diameter gas gun was utilized to initiate the explosive charges with manganin piezoresistive pressure gauge packages placed between packed layers (similar to 1.2 g/cm(3)) or sample disks pressed to low density (similar to 1.6 g/cm(3)). The measured shock sensitivity of the similar to 1.2 g/cm(3) HMX was similar to that previously measured by Sheffield et al. and the similar to 1.6 g/cm(3) HMX was measured to be much less shock sensitive. Ignition and Growth model parameters were utilized that yielded good agreement with the experimental data at both initial densities. C1 [Garcia, Frank; Vandersall, Kevin S.; Tarver, Craig M.] Lawrence Livermore Natl Lab, Energet Mat Ctr, Livermore, CA 94550 USA. RP Garcia, F (reprint author), Lawrence Livermore Natl Lab, Energet Mat Ctr, 7000 East Ave,L-282, Livermore, CA 94550 USA. EM vandersall1@llnl.gov NR 10 TC 5 Z9 5 U1 1 U2 22 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 052048 DI 10.1088/1742-6596/500/5/052048 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900082 ER PT S AU Gibson, LL Dattelbaum, DM Bartram, BD Sheffield, SA Gustavsen, RL Brown, GW Sandstrom, MM Giambra, AM Handley, CA AF Gibson, L. L. Dattelbaum, D. M. Bartram, B. D. Sheffield, S. A. Gustavsen, R. L. Brown, G. W. Sandstrom, M. M. Giambra, A. M. Handley, C. A. BE Buttler, W Furlanetto, M Evans, W TI Shock initiation sensitivity and Hugoniot-based equation of state of Composition B obtained using in situ electromagnetic gauging SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID EXPLOSIVES AB A series of gas gun-driven plate impact experiments were performed on vacuum melt-cast Composition B to obtain new Hugoniot states and shock sensitivity (run-distance-to-detonation) information. The Comp B (rho(0) = 1.713 g/cm(3)) consisted of 59.5% RDX, 39.5% TNT, and 1% wax, with similar to 6.5% HMX in the RDX. The measured Hugoniot states were found to be consistent with earlier reports, with the compressibility on the shock adiabat softer than that of a 63% RDX material reported by Marsh.[4] The shock sensitivity was found to be more sensitive (shorter run distance to detonation at a given shock input condition) than earlier reports for Comp B-3 and a lower density (1.68-1.69 g/cm(3)) Comp B formulation. The reactive flow during the shock-to-detonation transition was marked by heterogeneous, hot spot-driven growth both in and behind the leading shock front. C1 [Gibson, L. L.; Dattelbaum, D. M.; Bartram, B. D.; Sheffield, S. A.; Gustavsen, R. L.; Brown, G. W.; Sandstrom, M. M.; Giambra, A. M.] Los Alamos Natl Lab, Weap Expt, POB 1663, Los Alamos, NM 87545 USA. [Handley, C. A.] Atom Weap Estab, Aldermaston, England. RP Dattelbaum, DM (reprint author), Los Alamos Natl Lab, Weap Expt, POB 1663, Los Alamos, NM 87545 USA. EM danadat@lanl.gov OI Gustavsen, Richard/0000-0002-2281-2742 NR 16 TC 0 Z9 0 U1 1 U2 13 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR UNSP 192004 DI 10.1088/1742-6596/500/19/192004 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900295 ER PT S AU Glover, BB Daily, ME Son, SF Groven, LJ AF Glover, B. B. Daily, M. E. Son, S. F. Groven, L. J. BE Buttler, W Furlanetto, M Evans, W TI Microwave frequency material properties of PBS 9501 and PBX 9501 and small scale heating experiments SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing AB This work reports the microwave frequency dielectric properties of PBX 9501 and one of its representative mocks, PBS 9501, within 1-20 GHz. From these measurements it is shown that the binder system has a strong influence on microwave heating of such compositions resulting in significant temperature gradients within the individual HMX or sugar crystals at high microwave heating rates. Using the measured dielectric properties, COMSOL 4.3 Multiphysics was used to simulate and optimize a microwave applicator with a high electric field to input power ratio. The simulated applicator design indicated subsecond heating to decomposition for PBX 9501 and was validated with small scale experiments on both PBS 9501 and PBX 9501. At approximately 2.45 GHz and 100 W applied power, PBS 9501 decomposition was observed shortly (<34 ms) after a measured surface temperature of 70 degrees C (binder system melts). Finally, rapid heating of PBX 9501 was also shown in the optimized cavity. C1 [Glover, B. B.; Groven, L. J.] Los Alamos Natl Lab, WX 6, Los Alamos, NM 87545 USA. [Daily, M. E.; Son, S. F.; Groven, L. J.] Purdue Univ, Sch Mech Engn, W Lafayette, IN USA. [Groven, L. J.] South Dakota Sch Mines & Technol, Chem & Biol Engn, Rapid City, SD USA. RP Glover, BB (reprint author), Los Alamos Natl Lab, WX 6, Los Alamos, NM 87545 USA. EM lori.groven@sdsmt.edu FU Office of Naval Research [N00014-11-1-0466] FX Funded by the Office of Naval Research under project manager Dr. Michael Shlesinger, grant No. N00014-11-1-0466. NR 13 TC 0 Z9 0 U1 1 U2 7 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR UNSP 052040 DI 10.1088/1742-6596/500/5/052040 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900074 ER PT S AU Goff, M Burns, M Gustavsen, R Stennett, C Hazell, PJ Appleby-Thomas, GJ AF Goff, M. Burns, M. Gustavsen, R. Stennett, C. Hazell, P. J. Appleby-Thomas, G. J. BE Buttler, W Furlanetto, M Evans, W TI Effects observed when using metallic flyers and barriers with the embedded particle velocity gauge technique SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID INITIATION AB A number of experiments were carried out using a modified version of the standard particle velocity gauge technique in plate impact experiments with inert targets. Unusually these utilised dynamic metallic elements. Traditional methodology advises against the use of metallic flyers/barriers with this technique as conductive objects moving in the magnetic field produce perturbations in the output gauge voltage leading to inaccuracies in the derived particle velocities. This body of work investigated the causes of the perturbation effect, methods of minimising its magnitude and possible post-processing correction methods. In experiments with Al flyers, perturbations on the order of 10-15% of signal strength were observed. While the magnitude of the voltage traces were distorted, key features such as shock impact could still be observed, and shock tracker gauges were still effective. The case of metallic barriers was also examined and similar effects observed. This study has indicated that while a coarse empirical correction is possible, uncertainty in the validity of the correction would preclude the use of dynamic metallic elements in experiments where high fidelity data is required. C1 [Goff, M.; Stennett, C.; Appleby-Thomas, G. J.] Cranfield Univ, Swindon SN6 8LA, Wilts, England. [Goff, M.; Burns, M.] AWE, Reading RG7 4PR, Berks, England. [Gustavsen, R.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Hazell, P. J.] UNSW Canberra, Univ New S Wales, Sch Engn & Informat Technol, Canberra, ACT 2600, Australia. RP Goff, M (reprint author), Cranfield Univ, Swindon SN6 8LA, Wilts, England. EM m.goff@cranfield.ac.uk OI Hazell, Paul/0000-0002-8302-3173; Gustavsen, Richard/0000-0002-2281-2742 FU ISP ( Imperial College, London, UK); PhD FX The metallic flyer work was carried out in support of an ISP ( Imperial College, London, UK) funded PhD. The authors would like to thank A Roberts (Cranfield) and B Bartram (LANL) for invaluable technical assistance and also L Markland ( AWE) for assistance with hydrocode modelling. NR 4 TC 0 Z9 0 U1 0 U2 6 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR UNSP 142017 DI 10.1088/1742-6596/500/14/142017 PG 5 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900197 ER PT S AU Goodwin, PM Bartram, BD Gibson, LL Wu, M Dattelbaum, DM AF Goodwin, P. M. Bartram, B. D. Gibson, L. L. Wu, M. Dattelbaum, D. M. BE Buttler, W Furlanetto, M Evans, W TI Non-invasive timing of gas gun projectiles with light detection and ranging SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing AB We have developed a Light Detection and Ranging (LIDAR) diagnostic to track the position of a projectile inside of a gas gun launch tube in real-time. This capability permits the generation of precisely timed trigger pulses useful for triggering high-latency diagnostics such as a flash lamp-pumped laser. An initial feasibility test was performed using a 72 mm bore diameter single-stage gas gun routinely used for dynamic research at Los Alamos. A 655 nm pulsed diode laser operating at a pulse repetition rate of 100 kHz was used to interrogate the position of the moving projectile in real-time. The position of the projectile in the gun barrel was tracked over a distance of similar to 3 meters prior to impact. The position record showed that the projectile moved at a velocity of 489 m/s prior to impacting the target. This velocity was in good agreement with independent measurements of the projectile velocity by photon Doppler velocimetry and timing of the passage of the projectile through optical marker beams positioned at the muzzle of the gun. The time-to-amplitude conversion electronics used enable the LIDAR data to be processed in real-time to generate trigger pulses at preset separations between the projectile and target. C1 [Goodwin, P. M.] Los Alamos Natl Lab, Ctr Integrated Nanotechnol, POB 1663, Los Alamos, NM 87545 USA. [Bartram, B. D.; Gibson, L. L.; Dattelbaum, D. M.] Los Alamos Natl Lab, Shock & Detonat Phys, Los Alamos, NM 87545 USA. [Wu, M.] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Goodwin, PM (reprint author), Los Alamos Natl Lab, Ctr Integrated Nanotechnol, POB 1663, Los Alamos, NM 87545 USA. EM pmg@lanl.gov FU LANL Laboratory Directed Research and Development [2011012DR]; DOE/NNSA; [LA-UR-13-27770] FX We gratefully acknowledge the Chamber 9 gas gun team for help with the experiments. Los Alamos National Laboratory is operated by LANS LLC for DOE and NNSA. Support for this work was provided by LANL Laboratory Directed Research and Development Project 2011012DR and DOE/NNSA Campaign 2 funds. LA-UR-13-27770, approved for public release; distribution is unlimited. NR 7 TC 0 Z9 0 U1 0 U2 5 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR UNSP 142009 DI 10.1088/1742-6596/500/14/142009 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900189 ER PT S AU Grady, D Fenton, G Vogler, T AF Grady, Dennis Fenton, Gregg Vogler, Tracy BE Buttler, W Furlanetto, M Evans, W TI Equation of state for shock compression of distended solids SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing AB Shock Hugoniot data for full-density and porous compounds of boron carbide, silicon dioxide, tantalum pentoxide, uranium dioxide and playa alluvium are investigated for the purpose of equation-of-state representation of intense shock compression. Complications of multivalued Hugoniot behavior characteristic of highly distended solids are addressed through the application of enthalpy-based equations of state of the form originally proposed by Rice and Walsh in the late 1950's. Additive measures of cold and thermal pressure intrinsic to the Mie-Gruneisen EOS framework is replaced by isobaric additive functions of the cold and thermal specific volume components in the enthalpy-based formulation. Additionally, experimental evidence reveals enhancement of shock-induced phase transformation on the Hugoniot with increasing levels of initial distension for silicon dioxide, uranium dioxide and possibly boron carbide. Methods for addressing this experimentally observed feature of the shock compression are incorporated into the EOS model. C1 [Grady, Dennis; Fenton, Gregg] Appl Res Associates, Southwest Div, 4300 San Mateo Blvd NE, Albuquerque, NM 87110 USA. [Vogler, Tracy] Sandia Natl Labs, Livermore, CA 94550 USA. RP Grady, D (reprint author), Appl Res Associates, Southwest Div, 4300 San Mateo Blvd NE, Albuquerque, NM 87110 USA. EM dgrady@ara.com NR 10 TC 1 Z9 1 U1 0 U2 8 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR UNSP 152007 DI 10.1088/1742-6596/500/15/152007 PG 8 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900221 ER PT S AU Gray, GT Bourne, NK Livescu, V Trujillo, CP MacDonald, S Withers, P AF Gray, G. T., III Bourne, N. K. Livescu, V. Trujillo, C. P. MacDonald, S. Withers, P. BE Buttler, W Furlanetto, M Evans, W TI The influence of shock-loading path on the spallation response of Ta SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID DYNAMIC FRACTURE; METALS AB Spallation is well known to be a complex process strongly influenced by microstructure, loading path, and the loading profile yet often a singular "spall strength" is utilized in hydrocodes to quantify the dynamic fracture behavior of a material. In the current study, the influence of loading path on the "spall strength" and damage evolution in high-purity Ta is presented. Tantalum samples where shock loaded to three different peak shock stresses using both symmetric impact, and two different composite flyer plate configurations such that upon unloading the three samples displayed nearly identical "pull-back" signals as measured via rear-surface velocimetry. While the "pull-back" signals observed are similar in magnitude, the highest peak stressed sample resulted in complete spall scab separation while the two lower peak stresses resulted in incipient spall. The damage evolution in the "soft" recovered Ta samples was quantified using optical metallography, electron-back-scatter diffraction, and tomography. The effect of loading path on spallation and its ramifications for the stress and kinetic dependency of dynamic damage evolution is discussed. C1 [Gray, G. T., III; Livescu, V.; Trujillo, C. P.] Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. [Bourne, N. K.] AWE Aldermaston Reading, Berkshire RG7 4PR, England. [MacDonald, S.; Withers, P.] Univ Manchester, Manchester M60 1QD, Lancs, England. RP Gray, GT (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM rusty@lanl.gov FU US Department of Energy [06NA25396]; DoD/ DOE Munitions Program FX Los Alamos National Laboratory is operated by LANS, LLC, for the NNSA of the US Department of Energy under Contract No. DE- AC52- 06NA25396. This research was supported under the auspices of the US Department of Energy and the Joint DoD/ DOE Munitions Program. NR 15 TC 4 Z9 4 U1 1 U2 14 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR UNSP 112031 DI 10.1088/1742-6596/500/11/112031 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900133 ER PT S AU Gustavsen, RL Aslam, TD Bartram, BD Hollowell, BC AF Gustavsen, R. L. Aslam, T. D. Bartram, B. D. Hollowell, B. C. BE Buttler, W Furlanetto, M Evans, W TI Plate impact experiments on the TATB based explosive PBX 9502 at pressures near the Chapman-Jouguet state SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing AB A series of two-stage gus-gun driven plate impact experiments on PBX 9502 (95 wt.% tri-amino-trinitro-benzene, 5 wt.% Kel-F800 plastic binder) was completed in the 28 34 GPa pressure range. This is just above the Chapman-Jouguet state of approximate to 28 GPa. The experiments consisted of a thick oxygen free high conductivity copper (OFHC Cu) flyer plate impacting a PBX 9502 sample backed by a Lithium Fluoride (LiF) window. Photonic Doppler Velocimetry (PDV) was used to measure velocity histories (wave profiles) at the PBX 9502/LiF interface. Shock transit times and sample thicknesses were converted to shock velocities, Us. Particle velocities, up, were calculated by way of impedance matching. Lastly, the measured wave profiles were compared with numerical simulations of the experiments using the Wescott-Stewart-Davis reactive-burn model. C1 [Gustavsen, R. L.; Aslam, T. D.; Bartram, B. D.; Hollowell, B. C.] Los Alamos Natl Lab, Shock & Detonat Phys Grp, Los Alamos, NM 87545 USA. RP Gustavsen, RL (reprint author), Los Alamos Natl Lab, Shock & Detonat Phys Grp, POB 1663, Los Alamos, NM 87545 USA. EM rgus@lanl.gov OI Aslam, Tariq/0000-0002-4263-0401; Gustavsen, Richard/0000-0002-2281-2742 NR 15 TC 0 Z9 0 U1 2 U2 15 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 052015 DI 10.1088/1742-6596/500/5/052015 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900049 ER PT S AU Hammerberg, JE Milhans, JL Ravelo, RJ Germann, TC AF Hammerberg, J. E. Milhans, J. L. Ravelo, R. J. Germann, T. C. BE Buttler, W Furlanetto, M Evans, W TI Frictional interactions at high velocity ductile metal interfaces SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing AB We have examined the effect of evolution of grain morphology on the frictional force at polycrystalline Al-Al and Al-Ta interfaces as a function of grain size and sliding velocity. We present the results of 8M, 26M and 138M particle NonEquilibrium Molecular Dynamics (NEMD) simulations for grain sizes of 13 and 20 nm. Sample sizes consisted of 3x3x3 and 5x5x5 grains on each side of a sliding interface. We have considered sliding velocities from 20 to 4000 m/s. For velocities below a size dependent critical velocity above which a fluid layer forms, we find enhanced grain coarsening leading to a highly strained, graded final steady state microstructure that exhibits a dynamic morphology for times greater than 5-10 ns. We find that the frictional force is insensitive to the initial grain size distribution due to the evolution of the initial distribution to a new nonequilibrium steady state. We discuss the relationship of these results to single crystal interfaces and the mechanisms for grain size and shape evolution. C1 [Hammerberg, J. E.; Milhans, J. L.; Germann, T. C.] Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. [Ravelo, R. J.] Univ Texas El Paso, Dept Phys, El Paso, TX USA. RP Hammerberg, JE (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM jeh@lanl.gov OI Germann, Timothy/0000-0002-6813-238X FU U. S. Dept. of Energy [DEAC52- 06NA25396]; LANL ASC- PEM program FX It is a pleasure to acknowledge very useful discussions with B. L. Holian during the course of this work. This work was performed under the auspices of the U. S. Dept. of Energy under contract DEAC52- 06NA25396. The support of the LANL ASC- PEM program is gratefully acknowledged. NR 6 TC 1 Z9 1 U1 1 U2 3 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR UNSP 172003 DI 10.1088/1742-6596/500/17/172003 PG 5 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900239 ER PT S AU Hobbs, ML Kaneshige, MJ AF Hobbs, M. L. Kaneshige, M. J. BE Buttler, W Furlanetto, M Evans, W TI Effect of confinement during cookoff of TATB SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing AB In practical scenarios, cookoff of explosives is a three-dimensional transient phenomenon where the rate limiting reactions may occur either in the condensed or gas phase. The effects of confinement are more dramatic when the rate-limiting reactions occur in the gas phase. Explosives can be self-confined, where the decomposing gases are contained within non-permeable regions of the explosive, or confined by a metal or composite container. In triaminotrinitrobenzene (TATB) based explosives, self-confinement is prevalent in plastic bonded explosives at full density. The time-to-ignition can be delayed by orders of magnitude if the reactive gases leave the confining apparatus. Delays in ignition can also occur when the confining apparatus has excess gas volume or ullage. Understanding the effects of confinement is required to accurately model explosive cookoff at various scales ranging from small laboratory experiments to large real systems. C1 [Hobbs, M. L.] Sandia Natl Labs, Engn Sci Ctr, POB 5800, Albuquerque, NM 87185 USA. [Kaneshige, M. J.] Sandia Natl Labs, Energet Components Ctr, Albuquerque, NM 87185 USA. RP Hobbs, ML (reprint author), Sandia Natl Labs, Engn Sci Ctr, POB 5800, Albuquerque, NM 87185 USA. EM mlhobbs@sandia.gov FU DE-AC04-94AL85000; [2013-5318C] FX 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. SAND NO. 2013-5318C. We would also like to thank Shane Snedigar for running all of the SITI experiments, Bill Erikson for reducing the SITI data to determine thermal conductivity, Tolulope Okusanya for helping to implement the pressure dependent model, Eric Harstad for leading the energetics team and obtaining funding, and Marty Pilch, Leanna Minier for their constant interest and enthusiasm regarding our experimental and modeling activities. NR 6 TC 0 Z9 0 U1 1 U2 8 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR UNSP 052017 DI 10.1088/1742-6596/500/5/052017 PG 8 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900051 ER PT S AU Hollowell, BC Gustavsen, RL Dattelbaum, DM Bartram, BD AF Hollowell, B. C. Gustavsen, R. L. Dattelbaum, D. M. Bartram, B. D. BE Buttler, W Furlanetto, M Evans, W TI Shock initiation of the TATB-based explosive PBX 9502 cooled to 77 Kelvin SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing AB We present gas-gun driven plate impact shock initiation experiments on the explosive PBX 9502 (95 weight percent triaminotrinitrobenzene, 5 weight percent Kel-F 800 binder) cooled to liquid nitrogen temperature, 77K. PBX 9502 samples were cooled by flowing liquid nitrogen through a sample mounting plate and surrounding coil. Temperatures were monitored using embedded and surface mounted thermocouples. Reactive flow was measured with embedded electromagnetic particle velocity gauges. Wave profiles from the particle velocity gauges show that, even at 77K, shock initiation in PBX 9502 retains a heterogeneous or "hot-spot" character. The "Pop-plot," or distance to detonation, x(D), vs. impact pressure, P, is log(10)(x(D)) = 4.9 - 3.3log(10)(P). C1 [Hollowell, B. C.; Gustavsen, R. L.; Dattelbaum, D. M.; Bartram, B. D.] Los Alamos Natl Lab, Shock & Detonat Phys Grp, Los Alamos, NM 87545 USA. RP Hollowell, BC (reprint author), Los Alamos Natl Lab, Shock & Detonat Phys Grp, Mail Stop P952, Los Alamos, NM 87545 USA. EM rgus@lanl.gov OI Gustavsen, Richard/0000-0002-2281-2742 NR 15 TC 0 Z9 0 U1 2 U2 13 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 182014 DI 10.1088/1742-6596/500/18/182014 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900260 ER PT S AU Hsu, PC Hust, G Zhang, MX Lorenz, TK Reynolds, JG Fried, L Springer, HK Maienschein, JL AF Hsu, P. C. Hust, G. Zhang, M. X. Lorenz, T. K. Reynolds, J. G. Fried, L. Springer, H. K. Maienschein, J. L. BE Buttler, W Furlanetto, M Evans, W TI Study of thermal sensitivity and thermal explosion violence of energetic materials in the LLNL ODTX system SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID DECOMPOSITION AB Incidents caused by fire and combat operations can heat energetic materials that may lead to thermal explosion and result in structural damage and casualty. Some explosives may thermally explode at fairly low temperatures (<100 degrees C) and the violence from thermal explosion may cause significant damage. Thus it is important to understand the response of energetic materials to thermal insults. The One Dimensional Time to Explosion (ODTX) system at the Lawrence Livermore National Laboratory has been used for decades to measure times to explosion, threshold thermal explosion temperature, and determine kinetic parameters of energetic materials. Samples of different configurations (pressed part, powder, paste, and liquid) can be tested in the system. The ODTX testing can also provide useful data for assessing the thermal explosion violence of energetic materials. Recent ODTX experimental data are reported in the paper. C1 [Hsu, P. C.; Hust, G.; Zhang, M. X.; Lorenz, T. K.; Reynolds, J. G.; Fried, L.; Springer, H. K.; Maienschein, J. L.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. RP Hsu, PC (reprint author), Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. EM hsu7@llnl.gov RI Fried, Laurence/L-8714-2014 OI Fried, Laurence/0000-0002-9437-7700 NR 12 TC 1 Z9 1 U1 1 U2 4 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 052019 DI 10.1088/1742-6596/500/5/052019 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900053 ER PT S AU Hull, L Gray, G Faulkner, J Briggs, M AF Hull, L. Gray, G. Faulkner, J. Briggs, M. BE Buttler, W Furlanetto, M Evans, W TI Damage in low alloy steel produced by sweeping, interacting detonation waves SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing AB Detonation waves that sweep along the surface of a metal plate induce reduced pressure and enhanced shear, relative to the same detonation at normal incidence. Detonation waves at intermediate obliquity impress intermediate combined stress states. Release waves from the free surfaces may enter into play and contribute to the damage. Initiation of explosive at discrete points produces strong pressure, density, and velocity gradients in the gaseous explosive products in areas where the waves collide, are impressed in an adjacent metal, causing similar stress gradients within the metal that often leading to intense damage. In this work, we investigate damage generated in AISI 4130 steel by the combined effects of oblique drive and interacting detonation waves. The experimental data consist of multipoint velocimetry points probing the free surface in regions loaded by interacting detonation waves and regions between the interactions. Metallography on recovered plate records the plastic flow and damage correlated with the velocimetry data. Spall is indicated in most regions, but not some, and the alpha-epsilon stress-induced phase transformation appears in most regions, but not all. C1 [Hull, L.; Gray, G.; Faulkner, J.; Briggs, M.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Hull, L (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM lh@lanl.gov NR 1 TC 1 Z9 1 U1 0 U2 2 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 112034 DI 10.1088/1742-6596/500/11/112034 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900136 ER PT S AU Jackson, SI Short, M AF Jackson, Scott I. Short, Mark BE Buttler, W Furlanetto, M Evans, W TI Experimental measurement of the scaling of the diameter- and thickness-effect curves for ideal, insensitive, and non-ideal explosives SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID DETONATION; INITIATION; VELOCITY AB Numerous two-dimensional high-explosive slab tests were fielded for explosives that exhibit ideal (PBX 9501), slightly non-ideal (PBX 9502), and highly non-ideal (ANFO) detonation. Detonation velocity versus slab thickness t (thickness-effect curves) are compared to previous diameter-effect measurements obtained by varying the diameter d of cylindrical rate sticks. The scale factors dlt necessary to overlay the diameter- and thickness-effect curves were computed for each explosive formulation. We observe that the scale factor varies with detonation velocity (or level of detonation "ideality"). The measured scale factors range from 1.89-2.20, 1.25-1.87, and 1.79-1.05 for PBX 9501, PBX 9502, and ANFO formulations, respectively, as detonation velocity varies from the (near failure) critical velocity to the Chapman-Jouguet velocity. These results support our previous theoretical prediction that the scale factor relating the diameter- and thickness-effect curves will increasingly deviate from two as the detonation structure becomes increasingly non-ideal. C1 [Jackson, Scott I.; Short, Mark] Los Alamos Natl Lab, Shock & Detonation Phys Grp, Los Alamos, NM 87544 USA. RP Jackson, SI (reprint author), Los Alamos Natl Lab, Shock & Detonation Phys Grp, POB 1663, Los Alamos, NM 87544 USA. EM sjackson@lanl.gov OI Jackson, Scott/0000-0002-6814-3468 NR 12 TC 1 Z9 1 U1 0 U2 8 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 052020 DI 10.1088/1742-6596/500/5/052020 PG 5 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900054 ER PT S AU Jensen, BJ Ramos, KJ Iverson, AJ Bernier, J Carlson, CA Yeager, JD Fezzaa, K Hooks, DE AF Jensen, B. J. Ramos, K. J. Iverson, A. J. Bernier, J. Carlson, C. A. Yeager, J. D. Fezzaa, K. Hooks, D. E. BE Buttler, W Furlanetto, M Evans, W TI Dynamic experiment using IMPULSE at the Advanced Photon Source SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID PHASE-TRANSITION; KCL AB The ability to examine the dynamic response of materials at extreme conditions requires diagnostics that can provide real-time, in situ, spatially resolved measurements at the appropriate length scale. Recent advances in synchrotron sources and diagnostics coupled to dynamic loading platforms are transforming the dynamic compression field to allow for such investigations. In the current work, recent experimental efforts on the IMPULSE (IMPact System for ULtrafast Synchrotron Experiments) capability at the Advanced Photon Source (Argonne, IL) will be highlighted to describe its development and use to examine phenomena including jet-formation in metals, compaction, crack formation and propagation, and material strength and failure. These experimental results have relied in part on: 1) the development of a robust optically multiplexed intensified detector configuration to obtain the first shock movies and 2) gun system improvements to better synchronize the impact event with the 80-ps width X-ray bunch. The IMPULSE capability is expected to continue to reveal novel phenomena for materials subjected to high strain rate loading while developing the required knowledge base to ensure success for future facilities including the Dynamic Compression Sector at the Advanced Photon Source and LANL's MaRIE. C1 [Jensen, B. J.; Ramos, K. J.; Yeager, J. D.; Hooks, D. E.] Los Alamos Natl Lab, WX-9, Los Alamos, NM 87544 USA. [Iverson, A. J.; Carlson, C. A.] Natl Secur Technol LLC, Los Alamos, NM 87544 USA. [Bernier, J.] Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. [Fezzaa, K.] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. RP Jensen, BJ (reprint author), Los Alamos Natl Lab, WX-9, Los Alamos, NM 87544 USA. EM bjjensen@lanl.gov OI Yeager, John/0000-0002-3121-6053 FU LANL's MaRIE; Science Campaign programs and National Security Technologies (NSTec); Shock Wave Physics Related Diagnostics (SWRD); DOE [DEAC52-06NA25396]; U. S. DOE [DE-AC02-06CH11357] FX This work was supported by LANL's MaRIE and Science Campaign programs and National Security Technologies (NSTec) Shock Wave Physics Related Diagnostics (SWRD) program. LANL is operated by Los Alamos National Security, LLC for the U. S. Department of Energy (DOE) under Contract No. DEAC52-06NA25396. Use of the Advanced Photon Source, an Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory, was supported by the U. S. DOE under Contract No. DE-AC02-06CH11357. NR 20 TC 3 Z9 3 U1 4 U2 24 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR UNSP 042001 DI 10.1088/1742-6596/500/4/042001 PG 8 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900034 ER PT S AU Key, CT Schumacher, SC Ruggirello, KP Alexander, CS AF Key, C. T. Schumacher, S. C. Ruggirello, K. P. Alexander, C. S. BE Buttler, W Furlanetto, M Evans, W TI A multiphase approach for modelling the shock response of composite materials SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing AB The shock response of unidirectional fiber reinforced composite materials is inherently anisotropic due to their microstructural geometric configuration. Unlike typical elastic-plastic materials, composite materials form the observed two-wave structure under longitudinal shocks due to a precursor wave travelling through the fibers ahead of a bulk wave in the resin constituent. The nature of this response presents a problem in traditional hydrocode frameworks where each cell or material point tracks only a single velocity field. This paper outlines an adaptation of the Baer and Nunziato multi-phase model in CTH where a mixture rule is used to determine the velocity field of each constituent (fiber and matrix) of the composite material. The model modifies the momentum exchange term to represent the frictional drag forces between the fiber and matrix constituents, while assuming no mass or energy exchange. The momentum drag model is dependent not only upon the pressure difference between the constituents but also the directional dependence of the shock response. Finally, the model is implemented and the sensitivity of the solution to the interaction parameters demonstrated. C1 [Key, C. T.] Appl Technol Grp, HI TEST Labs, POB 87, Arvonia, VA 23004 USA. [Schumacher, S. C.; Ruggirello, K. P.; Alexander, C. S.] Sandia Natl Labs, Mech Engn, Albuquerque, NM 87123 USA. RP Key, CT (reprint author), Appl Technol Grp, HI TEST Labs, POB 87, Arvonia, VA 23004 USA. EM chris.key@hitestlabs.com FU [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 4 TC 0 Z9 0 U1 1 U2 4 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR UNSP 112056 DI 10.1088/1742-6596/500/11/112056 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900158 ER PT S AU Kohl, I Jilek, B Farrow, D Urayama, J Kearney, S AF Kohl, I. Jilek, B. Farrow, D. Urayama, J. Kearney, S. BE Buttler, W Furlanetto, M Evans, W TI Development of spectral interferometry for shock characterization in energetic materials SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID THIN-FILMS AB Ultrafast laser diagnostics have opened new pathways for investigation of shock physics and initiation of energetic materials. Short laser pulses on the time scale of 100s of picoseconds can be utilized for direct laser drive and coupled with imaging, spectroscopic, and interferometric tools at femtosecond scales for studies of dynamic loading during shock transit. At Sandia National Laboratories, we are implementing diagnostic platforms which extend the recent development of Ultrafast Shock Interrogation (USI) by Armstrong et al. [1] for table top measurement of Hugoniot/Equation-of-state data and characterization of shock structure with micron spatial resolution and picosecond time resolution. We present bare aluminium ablator data and initial data for pentaerythritol tetranitrate (PETN) as well as describe our experimental setup. C1 [Kohl, I.; Jilek, B.; Farrow, D.; Urayama, J.; Kearney, S.] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Kohl, I (reprint author), Sandia Natl Labs, POB 5800, Albuquerque, NM 87185 USA. EM spkearn@sandia.gov NR 22 TC 1 Z9 1 U1 0 U2 4 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 022005 DI 10.1088/1742-6596/500/2/022005 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900006 ER PT S AU Lam, K AF Lam, Kin BE Buttler, W Furlanetto, M Evans, W TI Modeling of propellant flow and explosively-driven valve for the Large-Bore Powder Gun SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing AB The Large-Bore Powder Gun is being developed to provide impact experiments on physics samples at the Nevada Test Site. A confinement system is required to seal the target chamber from the gun system to keep it free of hazardous materials from the impact event. A key component of the confinement system is an explosively driven valve (EDV), which uses a small amount of explosive to drive an aluminum piston perpendicular to the barrel axis into a tapered hole. The objective of this study is to evaluate designs of the confinement system via computational simulations using models validated with prototype experiments. A novel approach is adopted for this work, in which an energy source developed based on interior ballistic calculations was implemented in a hydrocodc, which in turn was used to model the propellant flow, EDV operation, and their interactions. This paper describes the models and some simulation results leading to a proposed confinement system design. C1 Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Lam, K (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM klam@lanl.gov NR 4 TC 0 Z9 0 U1 0 U2 1 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 152008 DI 10.1088/1742-6596/500/15/152008 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900222 ER PT S AU Lemke, RW Knudson, MD Cochrane, KR Desjarlais, MP Asay, JR AF Lemke, R. W. Knudson, M. D. Cochrane, K. R. Desjarlais, M. P. Asay, J. R. BE Buttler, W Furlanetto, M Evans, W TI On the scaling of the magnetically accelerated flyer plate technique to currents greater than 20 MA SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing AB In this article we discuss scaling the magnetically accelerated flyer plate technique to currents greater than is available on the Z accelerator. Peak flyer plate speeds in the range 746 km/s are achieved in pulsed power driven, hyper-velocity impact experiments on Z for peak currents in the range 8-20 MA. The highest (lowest) speeds are produced using aluminum (aluminum-copper) flyer plates. In either case, the approximate to 1 mm thick flyer plate is shocklessly accelerated by magnetic pressure to ballistic speed in approximate to 400 ns; it arrives at the target with a fraction of material at standard density. During acceleration a melt front, due to resistive heating, moves from the drive-side toward the target-side of the flyer plate; the speed of the melt front increases with increasing current. Peak flyer speeds on Z scale quadratically (linearly) with current at the low (high) end of the range. Magnetohydrodynamic simulation shows that the change in scaling is due to geometric deformation, and that linear scaling continues as current increases. However, the combined effects of shockless acceleration and resistive heating lead to an upper bound on the magnetic field feasible for pulsed power driven flyer plate experiments, which limits the maximum possible speed of a useful flyer plate to < 100 km/s. C1 [Lemke, R. W.; Knudson, M. D.; Cochrane, K. R.; Desjarlais, M. P.; Asay, J. R.] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Lemke, RW (reprint author), Sandia Natl Labs, POB 5800, Albuquerque, NM 87185 USA. EM rwlemke@sandia.gov NR 14 TC 1 Z9 1 U1 0 U2 4 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 152009 DI 10.1088/1742-6596/500/15/152009 PG 5 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900223 ER PT S AU Levesque, GA Vitello, P Nichols, AL Tarver, C Willey, T Friedman, G Oppelstrup, T AF Levesque, G. A. Vitello, P. Nichols, A. L., III Tarver, C. Willey, T. Friedman, G. Oppelstrup, T. BE Buttler, W Furlanetto, M Evans, W TI Analyses on the effect of hot spot density on material consumption rate SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID EXPLOSIVES AB There is an observed effect of an explosive's constituent grain size and density on its performance. At the mesoscale, it is the outward burning of hot spots that controls observed performance. While statistical hot spot models can integrate the mesoscale behaviour to macroscale simulations, it is unknown what the density of created hot spots is as a function of grain size and porosity. Simulating mesoscale hot spot distributions and varying hot spot density, we discuss the resultant performance as influenced by inter-pore distance and pore distribution. C1 [Levesque, G. A.; Vitello, P.; Nichols, A. L., III; Tarver, C.; Willey, T.; Friedman, G.; Oppelstrup, T.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. RP Levesque, GA (reprint author), Lawrence Livermore Natl Lab, 7000 East Ave, Livermore, CA 94550 USA. EM levesque6@llnl.gov RI Willey, Trevor/A-8778-2011 OI Willey, Trevor/0000-0002-9667-8830 NR 10 TC 0 Z9 0 U1 1 U2 10 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 152010 DI 10.1088/1742-6596/500/15/152010 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900224 ER PT S AU Lipp, MJ Jenei, Z Ruddle, D Aracne-Ruddle, C Cynn, H Evans, WJ Kono, Y Kenney-Benson, C Park, C AF Lipp, M. J. Jenei, Zs Ruddle, D. Aracne-Ruddle, C. Cynn, H. Evans, W. J. Kono, Y. Kenney-Benson, C. Park, C. BE Buttler, W Furlanetto, M Evans, W TI Equation of state measurements by radiography provide evidence for a liquid-liquid phase transition in cerium SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID ALPHA-GAMMA-TRANSITION; VOLUME-COLLAPSE; PRESSURE AB A pressure-volume isotherm in cerium metal at 1100 K was measured in a large volume press of the Paris-Edinburgh type up to 6 GPa. The volume was determined by imaging a rectangular shape of the sample via white X-ray radiography. Energy dispersive x-ray diffraction spectra were recorded to ensure that the highly reactive cerium in the cell assembly remained pure at this temperature. Even at 1100 K the p-V equation of state of liquid cerium shows a pronounced decrease of the bulk modulus above the gamma-phase region similar to the 775 K isotherm in the solid that also shows an inflection point between gamma-and alpha-type cerium. The inflection point in the 1100 K isotherm indicating the minimum in the bulk modulus separating the gamma- from the alpha-type liquid is located at approximately 3.5 GPa. C1 [Lipp, M. J.; Jenei, Zs; Ruddle, D.; Aracne-Ruddle, C.; Cynn, H.; Evans, W. J.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. [Kono, Y.; Kenney-Benson, C.; Park, C.] Carnegie Inst Sci, Geophys Lab, HPCAT, Argonne, IL 60439 USA. RP Lipp, MJ (reprint author), Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. EM lipp1@llnl.gov RI Jenei, Zsolt/B-3475-2011 FU US Department of Energy; Lawrence Livermore National Laboratory [DE-AC52-07NA27344]; Laboratory Directed Research [12-LW-014]; DOE- NNSA [DE-NA0001974]; DOE-BES [DE-FG02-99ER45775, DE-AC02-06CH11357]; NSF FX This work was performed under the auspices of the US Department of Energy by Lawrence Livermore National Laboratory under Contract No. DE-AC52-07NA27344 and funded by the Laboratory Directed Research and Development Program under project tracking code 12-LW-014. Portions of this work were performed at HPCAT (Sector 16), Advanced Photon Source (APS), Argonne National Laboratory. HPCAT operations are supported by DOE- NNSA under Award No. DE-NA0001974 and DOE-BES under Award No. DE-FG02-99ER45775, with partial instrumentation funding by NSF. APS is supported by DOE-BES, under Contract No. DE-AC02-06CH11357. NR 25 TC 1 Z9 2 U1 4 U2 10 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR UNSP 032011 DI 10.1088/1742-6596/500/3/032011 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900023 ER PT S AU Lloyd, JT Clayton, JD Austin, RA McDowell, DL AF Lloyd, J. T. Clayton, J. D. Austin, R. A. McDowell, D. L. BE Buttler, W Furlanetto, M Evans, W TI Modeling single-crystal microstructure evolution due to shock loading SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID CONSTITUTIVE MODEL; ALUMINUM; METALS AB An existing high strain rate viscoplastic (HSRVP) model is extended to address single-crystal anisotropic, elastic-plastic material response and is implemented into a steady plastic wave formulation in the weak shock regime. The single-crystal HSRVP model tracks the nucleation, multiplication, annihilation, and trapping of dislocations, as well as thermally activated and phonon drag limited glide kinetics. The steady plastic wave formulation is used to model the elastic-plastic response with respect to a propagating longitudinal wave, and assumes that the magnitudes of quasi-transverse waves are negligible. This steady wave analysis does not require specification of artificial viscosity, which can give rise to spurious dissipative effects. The constitutive model and its numerical implementation are applied to single-crystal pure Al and results are compared with existing experimental data. Dislocation density evolution, lattice reorientation, and macroscopic velocity-time histories are tracked for different initial orientations subjected to varying peak shock pressures. Results suggest that initial material orientation can significantly influence microstructure evolution, which can be captured using the modified Taylor factor. C1 [Lloyd, J. T.; McDowell, D. L.] Georgia Inst Technol, Woodruff Sch Mech Engn, Atlanta, GA 30332 USA. [Clayton, J. D.] US Army Res Lab, Impact Phys Branch, Aberdeen Proving Ground, MD USA. [Austin, R. A.] Lawrence Livermore Natl Lab, Mater Modeling & Simulat Grp, Livermore, CA USA. [McDowell, D. L.] Georgia Inst Technol, Sch Mater Sci & Engn, Atlanta, GA 30332 USA. RP Lloyd, JT (reprint author), Georgia Inst Technol, Woodruff Sch Mech Engn, Atlanta, GA 30332 USA. EM jeff.lloyd@gatech.edu RI Austin, Ryan/J-9003-2014; Clayton, John/C-7760-2009 NR 13 TC 1 Z9 1 U1 0 U2 7 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 112040 DI 10.1088/1742-6596/500/11/112040 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900142 ER PT S AU Maienschein, JL AF Maienschein, J. L. BE Buttler, W Furlanetto, M Evans, W TI Research topics in explosives - a look at explosives behaviors SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing AB The behaviors of explosives under many conditions - e.g., sensitivity to inadvertent reactions, explosion, detonation - are controlled by the chemical and physical properties of the explosive materials. Several properties are considered for a range of improvised and conventional explosives. Here I compare these properties across a wide range of explosives to develop an understanding of explosive behaviors. For improvised explosives, which are generally heterogeneous mixtures of ingredients, a range of studies is identified as needed to more fully understand their behavior and properties. For conventional explosives, which are generally comprised of crystalline explosive molecules held together with a binder, I identify key material properties that determine overall sensitivity, including the extremely safe behavior of Insensitive High Explosives, and discuss an approach to predicting the sensitivity or insensitivity of an explosive. C1 Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. RP Maienschein, JL (reprint author), Lawrence Livermore Natl Lab, POB 808,L-282, Livermore, CA 94551 USA. EM maienschein1@llnl.gov NR 14 TC 1 Z9 1 U1 0 U2 4 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 052027 DI 10.1088/1742-6596/500/5/052027 PG 8 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900061 ER PT S AU Manner, VW Pemberton, SJ Brown, GW Tappan, BC Hill, LG Preston, DN Neuscamman, SJ Glascoe, LG AF Manner, V. W. Pemberton, S. J. Brown, G. W. Tappan, B. C. Hill, L. G. Preston, D. N. Neuscamman, S. J. Glascoe, L. G. BE Buttler, W Furlanetto, M Evans, W TI Measurements of near-field blast effects using kinetic plates SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID EXPLOSIVES AB Few tests have been designed to measure the near-field blast impulse of ideal and non-ideal explosives, mostly because of the inherent experimental difficulties due to nontransparent fireballs and thermal effects on gauges. In order to measure blast impulse in the near-field, a new test has been developed by firing spherical charges at 152 mm (6 in) from steel plates and probing acceleration using laser velocimetry. Tests measure the velocity imparted to the steel plate in the 50 - 300 mu s timeframe, and are compared with free-field overpressure measurements at 1.52 m (5 ft) and ms timescales using piezoelectric pencil gauges. Specifically, tests have been performed with C4 to probe the contributions of ideal explosives and charge size effects. Non-ideal aluminized explosive formulations have been studied to explore the role of aluminum in near-field blast effects and far-field pressure, and are compared with formulations using LiF as an inert surrogate replacement for Al. The results are compared with other near-field blast tests and cylinder tests, and the validity of this test is explored with modeling and basic theory. C1 [Manner, V. W.; Pemberton, S. J.; Brown, G. W.; Tappan, B. C.; Hill, L. G.; Preston, D. N.] Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. [Neuscamman, S. J.; Glascoe, L. G.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. RP Manner, VW (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM vwmanner@lanl.gov FU National Explosives Engineering Science Security (NEXESS); Sandia National Laboratories; Los Alamos National Laboratory; Lawrence Livermore National Laboratory; U. S. Department of Homeland Security; Science and Technology Directorate; Explosives Division FX The work was performed by the National Explosives Engineering Science Security (NEXESS) Center, a tri-lab effort supported by Sandia National Laboratories, Los Alamos National Laboratory, and Lawrence Livermore National Laboratory under sponsorship of the U. S. Department of Homeland Security, Science and Technology Directorate, Explosives Division. NR 7 TC 0 Z9 0 U1 0 U2 4 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR UNSP 052029 DI 10.1088/1742-6596/500/5/052029 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900063 ER PT S AU Manner, VW Barker, BJ Sanders, VE Laintz, KE Scott, BL Preston, DN Sandstrom, M Reardon, BL AF Manner, V. W. Barker, B. J. Sanders, V. E. Laintz, K. E. Scott, B. L. Preston, D. N. Sandstrom, M. Reardon, B. L. BE Buttler, W Furlanetto, M Evans, W TI Energetic lanthanide complexes: coordination chemistry and explosives applications SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID TRANSITION-METAL SALTS; CRYSTAL-STRUCTURE; 5-NITRO-2,4-DIHYDRO-3H-1,2,4-TRIAZOLE-3-ONE NTO; LUMINESCENCE; STATE AB Metals are generally added to organic molecular explosives in a heterogeneous composite to improve overall heat and energy release. In order to avoid creating a mixture that can vary in homogeneity, energetic organic molecules can be directly bonded to high molecular weight metals, forming a single metal complex with Angstrom-scale separation between the metal and the explosive. To probe the relationship between the structural properties of metal complexes and explosive performance, a new series of energetic lanthanide complexes has been prepared using energetic ligands such as NTO (5-nitro-2,4-dihydro-1,2,4-triazole-3-one). These are the first examples of lanthanide NTO complexes where no water is coordinated to the metal, demonstrating novel control of the coordination environment. The complexes have been characterized by X-ray crystallography, NMR and IR spectroscopies, photoluminescence, and sensitivity testing. The structural and energetic properties are discussed in the context of enhanced blast effects and detection. Cheetah calculations have been performed to fine-tune physical properties, creating a systematic method for producing explosives with 'tailor made' characteristics. These new complexes will be benchmarks for further study in the field of metalized high explosives. C1 [Manner, V. W.; Barker, B. J.; Sanders, V. E.; Laintz, K. E.; Scott, B. L.; Preston, D. N.; Sandstrom, M.; Reardon, B. L.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Manner, VW (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM vwmanner@lanl.gov RI Barker, Beau/S-5494-2016; Scott, Brian/D-8995-2017 OI Barker, Beau/0000-0001-6680-6814; Scott, Brian/0000-0003-0468-5396 NR 25 TC 0 Z9 0 U1 0 U2 7 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 182028 DI 10.1088/1742-6596/500/18/182028 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900274 ER PT S AU May, CM Tarver, CM AF May, Chadd M. Tarver, Craig M. BE Buttler, W Furlanetto, M Evans, W TI Short pulse duration shock initiation experiments plus ignition and growth modeling on Composition B SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing AB Composition B (63% RDX, 36% TNT, 1% wax) is still a widely used energetic material whose shock initiation characteristics are necessary to understand. It is now possible to shock initiate Composition B and other secondary explosives at diameters well below their characteristic failure diameters for unconfined self-sustaining detonation. This is done using very high velocity, very thin, small diameter flyer plates accelerated by electric or laser power sources. Recently experimental detonation versus failure to detonate threshold flyer velocity curves for Composition B using several Kapton (TM) flyer thicknesses and diameters were measured. Flyer plates with diameters of 2 mm successfully detonated Composition B, which has a nominal failure diameter of 4.3 mm. The shock pressures required for these initiations are greater than the Chapman-Jouguet (C-J) pressure in self-sustaining Composition B detonation waves. The initiation process is two-dimensional, because both rear and side rarefactions can affect the shocked Composition B reaction rates. The Ignition and Growth reactive flow model for Composition B is extended to yield accurate simulations of this new threshold velocity data for various flyer thicknesses. C1 [May, Chadd M.; Tarver, Craig M.] Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. RP May, CM (reprint author), Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. EM tarver1@llnl.gov NR 9 TC 1 Z9 1 U1 1 U2 16 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 052045 DI 10.1088/1742-6596/500/5/052045 PG 5 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900079 ER PT S AU McGrane, SD Brown, KE Dang, NC Bolme, CA Moore, DS AF McGrane, S. D. Brown, K. E. Dang, N. C. Bolme, C. A. Moore, D. S. BE Buttler, W Furlanetto, M Evans, W TI Coherent Raman studies of shocked liquids SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID INDUCED DECOMPOSITION; VIBRATIONAL SPECTROSCOPY; NANOENERGETIC MATERIALS; MOLECULAR MATERIALS; CHEMICAL-REACTION; INDUCED CHEMISTRY; NITROMETHANE; COMPRESSION; SCATTERING; TEMPERATURE AB Coherent anti-Stokes Raman spectroscopy (CARS) is reported following shock loading for the liquids phenylacetylene (18 and 13 GPa), cyclohexane (17 GPa), and acrylonitrile (17 GPa). The evolution of the spectra over the first 300 ps was recorded in each case. All spectra show monotonic decay of all peaks with increasing time after shock. No new peaks due to either chemical reaction or pressure shifting of the vibrational frequencies were observable. This loss of signal after shock is attributed to the decreased coherence time in the shock heated liquids, which leads to rapid signal loss in the nonresonant background free version of CARS used in the measurements. These results suggest that more complex methods may be required to measure picosecond shock induced chemistry with coherent Raman techniques that are free of nonresonant background interference. C1 [McGrane, S. D.; Brown, K. E.; Bolme, C. A.; Moore, D. S.] Los Alamos Natl Lab, Shock & Detonat Phys Grp, MS P952, Los Alamos, NM 87544 USA. [Dang, N. C.] US Army Res Lab, Aberdeen, MD 21005 USA. RP McGrane, SD (reprint author), Los Alamos Natl Lab, Shock & Detonat Phys Grp, MS P952, Los Alamos, NM 87544 USA. EM mcgrane@lanl.gov OI Mcgrane, Shawn/0000-0002-2978-3980; Bolme, Cynthia/0000-0002-1880-271X FU High Explosive Science and Laboratory Directed Research and Development programs at Los Alamos National Laboratory FX The authors acknowledge support from the Campaign 2: High Explosive Science and Laboratory Directed Research and Development programs at Los Alamos National Laboratory. NR 38 TC 1 Z9 1 U1 0 U2 18 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR UNSP 142021 DI 10.1088/1742-6596/500/14/142021 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900201 ER PT S AU Millett, JCF Whiteman, G Bourne, NK Case, S Gray, GT AF Millett, J. C. F. Whiteman, G. Bourne, N. K. Case, S. Gray, G. T., III BE Buttler, W Furlanetto, M Evans, W TI Shear strength developments during shock loading in tantalum alloys: Effects of cold work and alloying SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID LATERAL STRESS; PEAK PRESSURE; DEFORMATION; BEHAVIOR AB The development of shear strength behind the shock front in tantalum alloys of 2.5 and 10wt% tungsten has been monitored by the use of laterally mounted stress gauges. Results show that in common with pure tantalum, shear strength decreases behind the shock front. At 2.5wt%, we believe that tungsten modifies the mechanical response by mitigating the effects of interstitial solute atoms, thus easing dislocation motion, as evidenced by the smaller reduction in shear strength compared to pure tantalum. At higher tungsten levels, it would appear that this is overcome by an overall increase in Peierls stress, which renders dislocation motion more difficult, thus giving the alloy a response more in common with that of the pure metal. Cold rolling of the 2.5% W alloy also appears to increase shear strength reduction behind the shock front (compared to the annealed alloy), although at present the reasons for this are unclear. C1 [Millett, J. C. F.; Whiteman, G.; Bourne, N. K.; Case, S.] AWE, Reading RG7 4PR, Berks, England. [Gray, G. T., III] Los Alamos Natl Lab, MST 8, Los Alamos, NM 87545 USA. RP Millett, JCF (reprint author), AWE, Reading RG7 4PR, Berks, England. EM jeremy.millett@awe.co.uk NR 17 TC 0 Z9 0 U1 0 U2 6 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR UNSP 112046 DI 10.1088/1742-6596/500/11/112046 PG 5 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900148 ER PT S AU Moore, DS McGrane, SD AF Moore, D. S. McGrane, S. D. BE Buttler, W Furlanetto, M Evans, W TI Raman temperature measurement SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID SCATTERING AB We are examining the experimental trade-offs for the use of the spontaneous Raman Stokes/anti-Stokes intensity ratio as a fundamental temperature measurement at static and dynamic extreme conditions. The trade-off space includes spatial resolution and temperature range versus vibrational frequency, as well as heating of the sample and nonlinear damage caused by the excitation laser. The experiments are being performed under a range of experimental conditions from nanoseconds to seconds and from cryogenic (77 K) to elevated (ca. 1000 K) temperatures. The results are being compared to calculations for transparent metal oxide and polymer materials, with the aim to demonstrate their potential as temperature reporters when used as thin windows on opaque materials. C1 [Moore, D. S.; McGrane, S. D.] Los Alamos Natl Lab, Shock & Detonat Phys Grp, Los Alamos, NM 87545 USA. RP Moore, DS (reprint author), Los Alamos Natl Lab, Shock & Detonat Phys Grp, POB 1663, Los Alamos, NM 87545 USA. EM moored@lanl.gov OI Mcgrane, Shawn/0000-0002-2978-3980 NR 10 TC 2 Z9 2 U1 1 U2 17 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 192011 DI 10.1088/1742-6596/500/19/192011 PG 5 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900302 ER PT S AU Moro, EA AF Moro, E. A. BE Buttler, W Furlanetto, M Evans, W TI New developments in photon Doppler velocimetry SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing AB Photon Doppler velocimetry (PDV) has made the transition among many experimental groups from being a new diagnostic to being routinely fielded as a means of obtaining velocity data in high-speed test applications. Indeed, research groups both within and outside of the shock physics community have taken note of PDV's robust, high-performance measurement capabilities. As PDV serves as the primary diagnostic in an increasing number of experiments, it will continue to find new applications and enable the measurement of previously un-measurable phenomena. This paper provides a survey of recent developments in PDV system design and feature extraction as well as a discussion of new applications for PDV. More specifically, changes at the system level have enabled the collection of data sets that are far richer than those previously attainable in terms of spatial and temporal coverage as well as improvements over PDV's previously measurable velocity ranges. And until recently, PDV data have been analyzed almost exclusively in the frequency-domain; although the use of additional data analysis techniques is beginning to show promise, particularly as it pertains to extracting information from a PDV signal about surface motion that is not along the beam's axis. C1 Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Moro, EA (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM moro@lanl.gov NR 25 TC 7 Z9 7 U1 1 U2 2 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 142023 DI 10.1088/1742-6596/500/14/142023 PG 8 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900203 ER PT S AU Mulford, R Swift, DC Hamel, S AF Mulford, R. Swift, D. C. Hamel, S. BE Buttler, W Furlanetto, M Evans, W TI Equation of state of ammonia SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID WATER AB Ammonia and water are critical components of extraterrestrial bodies, determining the density and physical properties of the Outer Planets, their moons, and of extrasolar planets. Ammonia is unusual in having a high heat capacity relative to other molecular species. Equations of state (EOS) are presented for ammonia and for mixtures of ammonia and water. Their properties are discussed in terms of chemical compositions that evolve as pressure and temperature are varied. The NH4OH hydrate of ammonia is known to exist as a separate molecular species at pressures above about 5 GPa, and an effort was made to include reaction between NH3 and H2O in the mixture EOS. The EOS are suitable for calculating structures of icy planets and exoplanets, and of impacts. mass-radius relations which bound the possible interpretations of composition and structure for extraterrestrial bodies of unknown composition, such as exoplanets. C1 [Mulford, R.] Los Alamos Natl Lab, MS E502, Los Alamos, NM 87544 USA. [Swift, D. C.; Hamel, S.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. RP Mulford, R (reprint author), Los Alamos Natl Lab, MS E502, Los Alamos, NM 87544 USA. EM mulford@lanl.gov NR 15 TC 2 Z9 2 U1 2 U2 9 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR UNSP 072001 DI 10.1088/1742-6596/500/7/072001 PG 5 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900093 ER PT S AU Murphy, MJ Johnson, CE AF Murphy, M. J. Johnson, C. E. BE Buttler, W Furlanetto, M Evans, W TI Preliminary investigations of HE performance characterization using SWIFT SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing AB Preliminary experiments are performed to assess the utility of using the shock wave image framing technique (SWIFT) to characterize high explosive (HE) performance on detonator length and time scales. Columns of XTX 8004, an extrudable RDX-based high explosive, are cured directly within polymethylmethacrylate (PMMA) dynamic witness plates, and SWIFT is employed to directly visualize shock waves driven into PMMA through detonation interaction. Current experiments investigate two-dimensional, axisymmetric test geometries that resemble historic aquarium tests, but on millimeter length scales, and the SWIFT system records 16-frame, time-resolved image sequences at 190 ns inter-framing. Detonation wave velocities are accurately calculated from the time-resolved images, and standard aquarium-test analysis is evaluated to investigate calculated shock pressures at the HE/PMMA interface. Experimental SWIFT results are discussed where the charge diameter of XTX 8004 is varied from 2.0 mm to 6.5 mm. C1 [Murphy, M. J.; Johnson, C. E.] Los Alamos Natl Lab, Detonator Technol W6, Los Alamos, NM 87545 USA. RP Murphy, MJ (reprint author), Los Alamos Natl Lab, Detonator Technol W6, POB 1663, Los Alamos, NM 87545 USA. EM mjmurphy@lanl.gov NR 9 TC 0 Z9 0 U1 0 U2 3 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 142024 DI 10.1088/1742-6596/500/14/142024 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900204 ER PT S AU Neuscamman, SJ Manner, VW Brown, GW Glascoe, LG AF Neuscamman, S. J. Manner, V. W. Brown, G. W. Glascoe, L. G. BE Buttler, W Furlanetto, M Evans, W TI Numerical simulations of near-field blast effects using kinetic plates SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing AB Numerical simulations using two hydrocodes were compared to near-field measurements of blast impulse associated with ideal and non-ideal explosives to gain insight into testing results and predict untested configurations. The recently developed kinetic plate test was designed to measure blast impulse in the near-field by firing spherical charges in close range from steel plates and probing plate acceleration using laser velocimetry. Plate velocities for ideal, non-ideal and aluminized explosives tests were modeled using a three dimensional hydrocode. The effects of inert additives in the explosive formulation were modeled using a 1-D hydrocode with multiphase flow capability using Lagrangian particles. The relative effect of particle impact on the plate compared to the blast wave impulse is determined and modeling is compared to free field pressure results. C1 [Neuscamman, S. J.; Glascoe, L. G.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. [Manner, V. W.; Brown, G. W.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Neuscamman, SJ (reprint author), Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. EM neuscamman1@llnl.gov FU STUN; NEXESS Center; Los Alamos National Laboratory (LANL); Lawrence Livermore National Laboratory (LLNL); Sandia National Laboratories (SNL); US Department of Homeland Security Science & Technology Directorate Explosives Division (DHSSTEXD); U.S. Department of Energy; Lawrence Livermore National Laboratory [DE-AC52-07NA27344, LLNL-PROC-641774] FX The authors wish to acknowledge Lew Glennand Ilya Lomov for the adaptation and parameterization of STUN to multiphase flow problems as used here. This work was performed by the NEXESS Center, a tri-lab effort supported by Los Alamos National Laboratory (LANL), Lawrence Livermore National Laboratory (LLNL), and Sandia National Laboratories (SNL), under the sponsorship of the US Department of Homeland Security Science & Technology Directorate, Explosives Division (DHSS&TEXD). This work is performed under the auspice sof the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344. LLNL-PROC-641774 NR 7 TC 0 Z9 0 U1 1 U2 2 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR UNSP 052033 DI 10.1088/1742-6596/500/5/052033 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900067 ER PT S AU Olson, RT Cerreta, EK Morris, C Montoya, AM Mariam, FG Saunders, A King, RS Brown, EN Gray, GT Bingert, JF AF Olson, R. T. Cerreta, E. K. Morris, C. Montoya, A. M. Mariam, F. G. Saunders, A. King, R. S. Brown, E. N. Gray, G. T. Bingert, J. F. BE Buttler, W Furlanetto, M Evans, W TI The effect of microstructure on Rayleigh-Taylor instability growth in solids SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID ELASTIC-PLASTIC SOLIDS; STRAIN-RATE; DEFORMATION; ACCELERATION; COPPER; MODEL AB The effect that grain size and material processing have on high-strain rate deformation of copper has been assessed through measurements of unstable Rayleigh-Taylor (RT) perturbation growth. The dynamic loading conditions and initial sinusoidal perturbations imposed on the samples are kept constant while the microstructure of the sample material is varied. Different polycrystalline grain-sizes, single-crystal orientations, and strain-hardened samples have all been dynamically tested. The RT perturbation growth is measured by acquiring a time-sequence of radiographs using the Los Alamos National Laboratory Proton Radiography (pRad) Facility. Single-crystal orientation and stain hardening due to material processing are both observed to affect the perturbation growth. However, polycrystalline grain size variations in copper samples do not influence the growth rate under the loading conditions investigated. C1 [Olson, R. T.; Cerreta, E. K.; Morris, C.; Montoya, A. M.; Mariam, F. G.; Saunders, A.; King, R. S.; Brown, E. N.; Gray, G. T.; Bingert, J. F.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Olson, RT (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM rtolson@lanl.gov OI Brown, Eric/0000-0002-6812-7820; Morris, Christopher/0000-0003-2141-0255 NR 19 TC 3 Z9 3 U1 2 U2 14 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 112048 DI 10.1088/1742-6596/500/11/112048 PG 8 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900150 ER PT S AU Pacheco, AH Dattelbaum, DM Orler, EB Bartram, BD Gustavsen, RL AF Pacheco, Adam H. Dattelbaum, Dana M. Orler, E. Bruce Bartram, Brian D. Gustavsen, Richard L. BE Buttler, W Furlanetto, M Evans, W TI Hugoniot-based equations of state for two filled EPDM rubbers SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing AB Particle-filled elastomers are commonly used as engineering components due to their ability to provide structural support via their elastic mechanical response. Even small amounts of particle fillers are known to increase the mechanical strength of elastomers due to polymer-filler interactions. In this work, the shock response of two filled (SiO2 or silica and Kevlar (TM) fillers) ethylene-propylene-diene (EPDM) rubbers were studied using single and two-stage gas gun-driven plate impact experiments. Hugoniot states were determined using standard plate impact methods. Both filled-EPDM elastomers exhibit high compressibility under shock loading and have a response similar to adiprene rubber. C1 [Pacheco, Adam H.; Dattelbaum, Dana M.; Bartram, Brian D.; Gustavsen, Richard L.] Los Alamos Natl Lab, Shock & Detonat Phys Grp, POB 1663, Los Alamos, NM 87545 USA. [Orler, E. Bruce] Virginia Tech, Dept Chem, Blacksburg, VA 24061 USA. RP Pacheco, AH (reprint author), Los Alamos Natl Lab, Shock & Detonat Phys Grp, POB 1663, Los Alamos, NM 87545 USA. EM danadat@lanl.gov OI Gustavsen, Richard/0000-0002-2281-2742 FU DOE/DoD; DOE/NNSA FX The authors acknowledge funding from the DOE/DoD Joint Munitions Program, DOE/NNSA, and the help of Ben Hollowell and Lee Gibson in firing the gas guns. NR 7 TC 0 Z9 0 U1 0 U2 2 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR UNSP 182015 DI 10.1088/1742-6596/500/18/182015 PG 5 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900261 ER PT S AU Preston, DN Hill, LG Tappan, BC AF Preston, D. N. Hill, L. G. Tappan, B. C. BE Buttler, W Furlanetto, M Evans, W TI The Los Alamos detonating pellet test (DPT): PBX 9501 evaluation tests SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing AB High explosive (HE) Velocity of Detonation (VOD) measurements are usually conducted using rate-stick-type tests. This method is highly accurate if carefully implemented, but is relatively costly and may require kilograms or more of HE depending on its sensitivity. We present a novel technique for inferring VOD using a single HE pellet, which for Conventional High Explosives (CHEs) can use 10 gm of HE or even less. This attribute makes the Detonating Pellet Test (DPT) ideal for the preliminary performance characterization of newly synthesized HE materials. On the other end of the size spectrum, the DPT can be scaled to very large dimensions so as to minimize the HE load necessary to characterize highly insensitive HEs such as ANFO. The DPT exploits the fact that the detonation emerging from the pellet face can be made highly spherical over some central region. Spherical detonation breakout on the Sample Pellet (SP) face is described by a simple analytic equation, which depends on the VOD and the Center Of Initiation (COI). The latter is determined by separate characterization of the detonator, with a wave refraction correction at the detonator/SP interface. The SP VOD is then determined by fitting the ideal breakout equation, with specified detonator COI, to detonation breakout data obtained via streak camera. We develop the DPT method and appraise it using sample PBX 9501 data in particular, while discussing its benefits and limitations in general. C1 [Preston, D. N.; Hill, L. G.; Tappan, B. C.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Preston, DN (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM dpreston@lanl.gov NR 4 TC 0 Z9 0 U1 0 U2 2 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 052035 DI 10.1088/1742-6596/500/5/052035 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900069 ER PT S AU Preston, DN Brown, GW Tappan, BC Oshwald, DM Koby, JR Schoonover, ML AF Preston, D. N. Brown, G. W. Tappan, B. C. Oshwald, D. M. Koby, J. R. Schoonover, M. L. BE Buttler, W Furlanetto, M Evans, W TI Drop weight impact measurements of HE sensitivity: modified detection methods SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID EXPLOSIVES AB High explosives small-scale sensitivity testing has been a hallmark of safety screening since WWII. Sensitivity testing was once crude and simple; broom sticks were used to scrape explosives on the floor while experimenters would look, listen, and smell for signs of a reaction. Since then, a wide variety of testing apparatus have been developed to explore the effects of different stimuli on explosives. In concert with the development of the machines themselves, the reaction detection methods have also evolved. This paper's focus is on the Los Alamos National Laboratory's (LANL) drop weight impact machine and reaction detection methods. A critical evaluation of results is presented with cautionary examples of false positives that can occur with non-explosive materials. C1 [Preston, D. N.; Brown, G. W.; Tappan, B. C.; Oshwald, D. M.; Koby, J. R.; Schoonover, M. L.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Preston, DN (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM dpreston@lanl.gov NR 7 TC 1 Z9 1 U1 2 U2 6 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 182033 DI 10.1088/1742-6596/500/18/182033 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900279 ER PT S AU Prime, MB Vaughan, DE Preston, DL Buttler, WT Chen, SR Oro, DM Pack, C AF Prime, M. B. Vaughan, D. E. Preston, D. L. Buttler, W. T. Chen, S. R. Oro, D. M. Pack, C. BE Buttler, W Furlanetto, M Evans, W TI Using growth and arrest of Richtmyer-Meshkov instabilities and Lagrangian simulations to study high-rate material strength SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID MODEL AB Experiments applying a supported shock through mating surfaces (Atwood number = 1) with geometrical perturbations have been proposed for studying strength at strain rates up to 10(7)/s using Richtmyer-Meshkov (RM) instabilities. Buttler et al. recently reported experimental results for RM instability growth in copper but with an unsupported shock applied by high explosives and the geometrical perturbations on the opposite free surface (Atwood number = -1). This novel configuration allowed detailed experimental observation of the instability growth and arrest. We present results and interpretation from numerical simulations of the Buttler RM instability experiments. Highly-resolved, two-dimensional simulations were performed using a Lagrangian hydrocode and the Preston-Tonks-Wallace (PTW) strength model. The model predictions show good agreement with the data. The numerical simulations are used to examine various assumptions previously made in an analytical model and to estimate the sensitivity of such experiments to material strength. C1 [Prime, M. B.; Vaughan, D. E.; Preston, D. L.; Buttler, W. T.; Chen, S. R.; Oro, D. M.; Pack, C.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Prime, MB (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM prime@lanl.gov OI Prime, Michael/0000-0002-4098-5620 NR 12 TC 2 Z9 2 U1 1 U2 5 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 112051 DI 10.1088/1742-6596/500/11/112051 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900153 ER PT S AU Rae, PJ Baca, EV Cartelli, AR Holmes, MD Kuiper, TA AF Rae, P. J. Baca, E. V. Cartelli, A. R. Holmes, M. D. Kuiper, T. A. BE Buttler, W Furlanetto, M Evans, W TI The increased shock sensitivity of PBX 9502 at high temperature SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing AB A modified gap test using brass attenuators has been designed that can significantly heat explosive samples prior to testing. The sensitivity of PBX 9502 when heated to 180, 200, 230 & 260 degrees C and soaked for 30 minutes was investigated. It was discovered that under the moderate confinement (0.46 MPa) of this test, the sensitivity of the material did increase close to literature data for LX-17 (a very similar composition) heated to 250 degrees C under numerically unquantified 'heavy confinement'. C1 [Rae, P. J.; Baca, E. V.; Cartelli, A. R.; Holmes, M. D.; Kuiper, T. A.] Los Alamos Natl Lab, Los Alamos, NM 87544 USA. RP Rae, PJ (reprint author), Los Alamos Natl Lab, WX 6, Los Alamos, NM 87544 USA. EM prae@lanl.gov NR 5 TC 0 Z9 0 U1 0 U2 3 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 052036 DI 10.1088/1742-6596/500/5/052036 PG 5 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900070 ER PT S AU Ramos, KJ Jensen, BJ Iverson, AJ Yeager, JD Carlson, CA Montgomery, DS Thompson, DG Fezzaa, K Hooks, DE AF Ramos, K. J. Jensen, B. J. Iverson, A. J. Yeager, J. D. Carlson, C. A. Montgomery, D. S. Thompson, D. G. Fezzaa, K. Hooks, D. E. BE Buttler, W Furlanetto, M Evans, W TI In situ investigation of the dynamic response of energetic materials using IMPULSE at the Advanced Photon Source SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID X-RAY-DIFFRACTION AB The mechanical and chemical response of energetic materials is controlled by a convolution of deformation mechanisms that span length scales and evolve during impact. Traditional methods use continuum measurements to infer the microstructural response whereas advances in synchrotron capabilities and diagnostics are providing new, unique opportunities to interrogate materials in real time and in situ. Experiments have been performed on a new gas-gun system (IMPact system for Ultrafast Synchrotron Experiments) using single X-ray bunch phase contrast imaging (PCI) and Laue diffraction at the Advanced Photon Source (APS). The low absorption of molecular materials maximizes x-ray beam penetration, allowing measurements in transmission using the brilliance currently available at APS Sector 32. The transmission geometry makes it possible to observe both average lattice response and spatially heterogeneous, continuum response (1-4 um spatial resolution over similar to 2 x 2 mm area, 80 ps exposure, 153 ns frame-rate) in energetic materials ranging from single crystals to plastic-bonded composites. The current work describes our progress developing and using these diagnostics to observe deformation mechanisms relevant to explosives and the first experiments performed with explosives on IMPULSE at APS. C1 [Ramos, K. J.; Jensen, B. J.; Yeager, J. D.; Montgomery, D. S.; Thompson, D. G.; Hooks, D. E.] Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. [Fezzaa, K.] Argonne Natl Lab, APS, Argonne, IL 60439 USA. [Iverson, A. J.; Carlson, C. A.] Natl Secur Technol LLC, Los Alamos, NM 87544 USA. RP Ramos, KJ (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM kramos@lanl.gov OI Yeager, John/0000-0002-3121-6053 FU U. S. Department of Energy through LANL's MaRIE; Science Campaigns; Joint Munitions and LDRD programs and National Security Technologies (NSTec) Shock Wave Related Diagnostics (SWRD) program; U. S. DOE [DE-AC02-06CH11357] FX The authors wish to thank T. H. Pierce, C. T. Owens, V. T. Hamilton, R. Valdiviez, C. A. Bolme, R. L. Sandberg, C. Liu, and C. M. Cady from LANL, J. A. Young and A. H. Curtis from NSTec LLC, and A. Deriy from ANL for their many contributions to this work. D. A. Frendenburg from LANL is thanked for the experiment illustrated in figure 6 (a). This work was supported by the U. S. Department of Energy through LANL's MaRIE, Science Campaigns, Joint Munitions and LDRD programs and National Security Technologies (NSTec) Shock Wave Related Diagnostics (SWRD) program. LANL is operated by Los Alamos National Security, LLC for the U. S. Department of Energy under contract DE- AC52-06NA25396. National Security Technologies, LLC, performed this work under Contract No. DE- AC52-06NA25946. 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. NR 22 TC 6 Z9 6 U1 3 U2 27 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR UNSP 142028 DI 10.1088/1742-6596/500/14/142028 PG 8 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900208 ER PT S AU Resnyansky, AD McDonald, SA Withers, PJ Bourne, NK Millett, JCF Brown, EN Rae, PJ AF Resnyansky, A. D. McDonald, S. A. Withers, P. J. Bourne, N. K. Millett, J. C. F. Brown, E. N. Rae, P. J. BE Buttler, W Furlanetto, M Evans, W TI Three-dimensional characterisation and simulation of deformation and damage during Taylor impact in PTFE SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID STRAIN-RATE; POLYTETRAFLUOROETHYLENE; POLYETHYLENE; TEMPERATURE; TENSILE; PHASE AB The current work presents Taylor impact experiments interrogating the effect of dynamic, high-pressure loading on polytetrafluoroethylene (PTFE). In particular, X-ray microtomography has been used to characterise the damage imparted to cylindrical samples due to impact at different velocities. Distinct regions of deformation are present and controlled by fracture within the polymer, with the extent of the deformed region and increasing propagation of fractures from the impact face showing a clear trend with increasing impact velocity. A two-phase rate sensitive strength model is implemented in the CTH hydrocode and used for simulation of the problem. The high-pressure phase transition of PTFE into Phase III within the crystalline domains from the polymer at normal conditions is managed by suitable phase transition kinetics within the model. The experimental observations are discussed with respect to the multi-phase model hydrocode predictions of the shock response from Taylor impact simulations. The damage and its progress are shown to correlate well with the onset of the phase transition and its evolution following the impact velocity increase. C1 [Resnyansky, A. D.] DSTO, Weapons & Countermeasures Div, POB 1500, Edinburgh, SA 5111, Australia. [McDonald, S. A.; Withers, P. J.; Bourne, N. K.] Univ Manchester, Sch Mat, Manchester M13 9PL, Lancs, England. [Bourne, N. K.; Millett, J. C. F.] AWE, Reading RG7 4PR, Berks, England. [Brown, E. N.; Rae, P. J.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Resnyansky, AD (reprint author), DSTO, Weapons & Countermeasures Div, POB 1500, Edinburgh, SA 5111, Australia. RI Resnyansky, Anatoly/H-6399-2013; OI Resnyansky, Anatoly/0000-0003-2573-1005; Brown, Eric/0000-0002-6812-7820 NR 16 TC 0 Z9 0 U1 0 U2 8 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR UNSP 182035 DI 10.1088/1742-6596/500/18/182035 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900281 ER PT S AU Reynolds, JG Sandstrom, MM Brown, GW Warner, KF Phillips, JJ Shelley, TJ Reyes, JA Hsu, PC AF Reynolds, J. G. Sandstrom, M. M. Brown, G. W. Warner, K. F. Phillips, J. J. Shelley, T. J. Reyes, J. A. Hsu, P. C. BE Buttler, W Furlanetto, M Evans, W TI DHS small-scale safety and thermal testing of improvised explosives-comparison of testing performance SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing AB One of the first steps in establishing safe handling procedures for explosives is small-scale safety and thermal (SSST) testing. To better understand the response of improvised materials or homemade explosives (HMEs) to SSST testing, 16 HME materials were compared to three standard military explosives in a proficiency-type round robin study among five laboratories-two DoD and three DOE-sponsored by DHS. The testing matrix has been designed to address problems encountered with improvised materials-powder mixtures, liquid suspensions, partially wetted solids, immiscible liquids, and reactive materials. More than 30 issues have been identified that indicate standard test methods may require modification when applied to HMEs to derive accurate sensitivity assessments needed for developing safe handling and storage practices. This paper presents a generalized comparison of the results among the testing participants, comparison of friction results from BAM (German Bundesanstalt fur Materialpr fung) and ABL (Allegany Ballistics Laboratory) designed testing equipment, and an overview of the statistical results from the RDX (1,3,5-Trinitroperhydro-1,3,5-triazine) standard tested throughout the proficiency test. C1 [Reynolds, J. G.; Hsu, P. C.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. [Sandstrom, M. M.; Brown, G. W.] Los Alamos Natl Lab, Los Alamos, NM USA. [Warner, K. F.] Naval Surface Warfare Ctr, Indian Head, MD USA. [Phillips, J. J.] Sandia Natl Labs, Albuquerque, NM USA. [Shelley, T. J.] Bureau Alcohol Tobacco & Firearms, Redstone Arsenal, AL USA. [Reyes, J. A.] Tyndall AFB, Appl Res Associate, Tyndall, FL USA. RP Reynolds, JG (reprint author), Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. EM reynolds3@llnl.gov FU Integrated Data Collection Analysis (IDCA); Los Alamos National Laboratory; Lawrence Livermore National Laboratory; Sandia National Laboratories; Air Force Research Laboratory; Indian Head Division; Naval Surface Warfare; U. S. Department of Homeland Security; Science and Technology Directorate; Explosives Division; Los Alamos National Security, LLC; U. S. Department of Energy [DE-AC52-06NA25396]; National Nuclear Security Administration [DE-AC0494AL85000]; Lawrence Livermore National Laboratory [DE-AC52-07NA27344]; The Air Force Research Laboratory and Indian Head Division; AFRL/RXQL; NSWC IHD [LLNLPROC-641023, (760210)] FX This work was performed by the Integrated Data Collection Analysis (IDCA) Program, a five- lab effort supported by Los Alamos National Laboratory, Lawrence Livermore National Laboratory, Sandia National Laboratories, the Air Force Research Laboratory, and Indian Head Division, Naval Surface Warfare under sponsorship of the U. S. Department of Homeland Security, Science and Technology Directorate, Explosives Division. Los Alamos National Laboratory is operated by Los Alamos National Security, LLC, for the U. S. Department of Energy under Contract DE-AC52-06NA25396. Sandia is a multi- program laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the U. S. Department of Energy's National Nuclear Security Administration under Contract DE-AC0494AL85000. This work was performed under the auspices of the U. S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344. The Air Force Research Laboratory and Indian Head Division, Naval Surface Warfare also performed work in support of this effort. The work performed by AFRL/RXQL and NSWC IHD is under sponsorship of the U. S. Department of Homeland Security, Science and Technology Directorate, Explosives Division. LLNLPROC-641023 (760210). NR 7 TC 3 Z9 3 U1 0 U2 6 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR UNSP 052037 DI 10.1088/1742-6596/500/5/052037 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900071 ER PT S AU Rigg, PA Saavedra, RA Scharff, RJ AF Rigg, P. A. Saavedra, R. A. Scharff, R. J. BE Buttler, W Furlanetto, M Evans, W TI Sound speed measurements in zirconium using the front surface impact technique SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID COMPRESSION AB We have performed a series of experiments impacting zirconium samples of varying purity level directly onto lithium fluoride (LiF) windows to determine both the Hugoniot and sound speed as a function of stress up to 70 GPa. This front surface impact (FSI) geometry is useful for determining sound speed in shock-compression experiments because wave interactions are mostly eliminated and multiple sample thicknesses are not needed in each experiment. The experimental results show two kinks in the sound speed which correlate well with the location of the alpha --> omega and omega --> beta transitions, respectively. A rarefaction shock also forms in the release wave in experiments conducted at 31 GPa giving further evidence that this phase transition is being observed. C1 [Rigg, P. A.; Saavedra, R. A.; Scharff, R. J.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Rigg, PA (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM parigg@lanl.gov OI Scharff, Robert/0000-0002-1708-8964 NR 14 TC 2 Z9 2 U1 0 U2 3 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 032014 DI 10.1088/1742-6596/500/3/032014 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900026 ER PT S AU Rigg, PA Scharff, RJ Hixson, RS AF Rigg, P. A. Scharff, R. J. Hixson, R. S. BE Buttler, W Furlanetto, M Evans, W TI Sound speed measurements in tantalum using the front surface impact technique SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID EQUATION-OF-STATE; VELOCITIES; COMPRESSION; GPA AB Shock compression experiments were performed on tantalum to determine the longitudinal sound speed on the Hugoniot from 36 to 105 GPa. Tantalum samples were impacted directly on to lithium fluoride windows at velocities ranging from 2.5 to 5.0 km/s and the resulting particle velocity profiles at the sample/window interface were recorded using optical velocimetry techniques. The time of arrival of the rarefaction wave from the back surface of the tantalum sample was then used to determine the longitudinal sound speed at the corresponding impact stress. In contrast to recently reported work, we see no evidence of a phase transition in the tantalum in this stress range. C1 [Rigg, P. A.; Scharff, R. J.; Hixson, R. S.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Rigg, PA (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM prigg@lanl.gov OI Scharff, Robert/0000-0002-1708-8964 NR 26 TC 6 Z9 6 U1 0 U2 5 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 032018 DI 10.1088/1742-6596/500/3/032018 PG 8 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900030 ER PT S AU Rodriguez, G Sandberg, RL Jackson, SI Vincent, SW Gilbertson, SM Udd, E AF Rodriguez, G. Sandberg, R. L. Jackson, S. I. Vincent, S. W. Gilbertson, S. M. Udd, E. BE Buttler, W Furlanetto, M Evans, W TI Fiber Bragg sensing of high explosive detonation experiments at Los Alamos National Laboratory SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing AB An all optical-fiber-based approach to measuring high explosive detonation front position and velocity is demonstrated. By measuring total light return using an incoherent light source reflected from a fiber Bragg grating sensor in contact with the explosive, dynamic mapping of the detonation front position and velocity versus time is obtained. We demonstrate two examples of detonation front measurements: PETN detasheet test and detonation along a multi-HE cylindrical rate stick containing sections of PBX 9501, Comp B, TNT, PBX 9407, PBX 9520, and inert PMMA. In the PETN detasheet measurement, excellent agreement with complementary diagnostics (electrical pins) is achieved, with accuracy in the detonation front velocity at the 0.13% level when compared to the results from the pin data. C1 [Rodriguez, G.; Sandberg, R. L.; Gilbertson, S. M.] Los Alamos Natl Lab, Mat Phys & Applicat Div, POB 1663, Los Alamos, NM 87545 USA. [Jackson, S. I.; Vincent, S. W.] Los Alamos Natl Lab, Weapons Expt Div, Los Alamos, NM 87545 USA. [Udd, E.] Columbia Gorge Res LLC, Fairview, OR 97024 USA. RP Rodriguez, G (reprint author), Los Alamos Natl Lab, Mat Phys & Applicat Div, POB 1663, Los Alamos, NM 87545 USA. EM rodrigeo@lanl.gov RI Rodriguez, George/G-7571-2012; OI Rodriguez, George/0000-0002-6044-9462; Jackson, Scott/0000-0002-6814-3468; Sandberg, Richard/0000-0001-9719-8188 FU Los Alamos National Laboratory; Department of Energy for Los Alamos National Security LLC [DE-AC52-06NA25396] FX This work is funded at the Los Alamos National Laboratory under the auspices of the Department of Energy for Los Alamos National Security LLC under Contract no. DE-AC52-06NA25396. NR 2 TC 4 Z9 4 U1 3 U2 13 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR UNSP 142030 DI 10.1088/1742-6596/500/14/142030 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900210 ER PT S AU Rothman, S Davis, JP Gooding, S Knudson, M Ao, T AF Rothman, S. Davis, J-P Gooding, S. Knudson, M. Ao, T. BE Buttler, W Furlanetto, M Evans, W TI Measurement of the principal quasi-isentrope of lead to similar to 3Mbar using the "Z" machine SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID HIGHLY PLASTICIZED METALS; EQUATION-OF-STATE; COMPRESSION AB We have measured the principal quasi-isentrope of pure lead to similar to 3 Mbar, using magnetically-driven ramp compression on SNL's "Z" machine. Multiple point-VISARs were used to measure the surface velocities of the compressed samples, and iterative Lagrangian analysis was used to find the wave speed as a function of ramp velocity to an accuracy of <2%. This was then integrated to longitudinal stress as a function of volume on the quasi-isentrope. The experiment used a stripline configuration with samples arranged in pairs at each of 4 vertical positions on opposite drive panels: three of the four pair positions held two lead samples of different thicknesses, while the fourth consisted of one lead sample and a bare panel for drive measurement. The thicker samples of the 3 pairs experienced weak shocks at low stress so their quasi-isentrope data is unreliable there. The single-sample data was good at low stress but affected at high stress by either effects of closure of the stripline gap and / or reflections of the compression pulse from the drive-panel rear surfaces. Data from both methods overlapped at intermediate stresses so have been combined to give the required quasi-isentrope data. C1 [Rothman, S.; Gooding, S.] AWE Aldermaston, Reading RG7 4PR, Berks, England. [Davis, J-P; Knudson, M.; Ao, T.] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Rothman, S (reprint author), AWE Aldermaston, Reading RG7 4PR, Berks, England. EM steve.rothman@awe.co.uk NR 11 TC 2 Z9 2 U1 0 U2 0 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR UNSP 032016 DI 10.1088/1742-6596/500/3/032016 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900028 ER PT S AU Rudd, RE Arsenlis, A Barton, NR Cavallo, RM Comley, AJ Maddox, BR Marian, J Park, HS Prisbrey, ST Wehrenberg, CE Zepeda-Ruiz, L Remington, BA AF Rudd, R. E. Arsenlis, A. Barton, N. R. Cavallo, R. M. Comley, A. J. Maddox, B. R. Marian, J. Park, H-S Prisbrey, S. T. Wehrenberg, C. E. Zepeda-Ruiz, L. Remington, B. A. BE Buttler, W Furlanetto, M Evans, W TI Multiscale strength (MS) models: their foundation, their successes, and their challenges SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID TRANSITION-METALS; INTERATOMIC POTENTIALS; PLASTIC-DEFORMATION; TAYLOR INSTABILITY; TANTALUM; COMPRESSION; SIMULATION; DYNAMICS; SOLIDS; FLOW AB Multiscale strength (MS) models are constructed to capture a natural hierarchy in the deformation of metals such as V and Ta starting with atomic bonding and extending up through the mobility of individual dislocations, the evolution of dislocation networks and so on until the ultimate material response at the scale of an experiment. In practice, the hierarchy is described by quantum mechanics, molecular dynamics, dislocation dynamics, and so on, ultimately parameterizing a continuum constitutive model. We review the basic models and describe how they operate at extremely high pressures and strain rates, such as in Rayleigh-Taylor plastic flow experiments. The models use dislocation density as a state variable, and describe time-dependent, as well as rate-dependent, plasticity. They make interesting and testable predictions about transients in plastic flow. There are also clear challenges, however. The current MS models do not include a variety of mechanisms known to be important at low rates. Still, MS models provide compelling insight into plastic deformation of metals under extreme pressures and strain rates. C1 [Rudd, R. E.; Arsenlis, A.; Barton, N. R.; Cavallo, R. M.; Maddox, B. R.; Marian, J.; Park, H-S; Prisbrey, S. T.; Wehrenberg, C. E.; Zepeda-Ruiz, L.; Remington, B. A.] Lawrence Livermore Natl Lab, 7000 East Ave,L-367, Livermore, CA 94550 USA. [Comley, A. J.] AWE, Reading RG7 4PR, Berks, England. RP Rudd, RE (reprint author), Lawrence Livermore Natl Lab, 7000 East Ave,L-367, Livermore, CA 94550 USA. FU LDRD program at Lawrence Livermore National Laboratory (LLNL) [09-SI-010]; Computing Grand Challenge program at LLNL; U.S. Department of Energy by Lawrence Livermore National Laboratory [DE-AC52-07NA27344] FX We appreciate support from the LDRD program at Lawrence Livermore National Laboratory (LLNL) under project 09-SI-010 and supercomputer time from the Computing Grand Challenge program at LLNL. 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 36 TC 2 Z9 2 U1 1 U2 25 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR UNSP 112055 DI 10.1088/1742-6596/500/11/112055 PG 8 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900157 ER PT S AU Ruggirello, KP Schumacher, SC AF Ruggirello, K. P. Schumacher, S. C. BE Buttler, W Furlanetto, M Evans, W TI A comparison of the shock response of the Material Point Method SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing AB The Lagrangian Material Point Method (MPM) [1, 2] has been implemented into the Eulerian shock physics code CTH [3] at Sandia National Laboratories. Eulerian hydrodynamic methods are useful for large deformation problems, where mesh tangling typically leads to difficulties for Lagrangian finite element methods. However, Eulerian techniques suffer from numerical diffusion due to advection, which can be problematic for many material models requiring the transport of a damage parameter or other state variables that need to remain sharp [4]. The inclusion of the MPM in CTH allows for the accurate simulation of structural response to shock loading in a single framework. This paper presents a comparison of the shock response of the MPM and CPDI to the CTH hydrodynamics code. C1 [Ruggirello, K. P.; Schumacher, S. C.] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Ruggirello, KP (reprint author), Sandia Natl Labs, POB 5800 MS 0828, Albuquerque, NM 87185 USA. EM kruggir@sandia.gov NR 6 TC 0 Z9 0 U1 0 U2 6 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 152013 DI 10.1088/1742-6596/500/15/152013 PG 5 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900227 ER PT S AU Sandberg, RL Rodriguez, G Gibson, LL Dattelbaum, DM Stevens, GD Grover, M Lalone, BM Udd, E AF Sandberg, R. L. Rodriguez, G. Gibson, L. L. Dattelbaum, D. M. Stevens, G. D. Grover, M. Lalone, B. M. Udd, E. BE Buttler, W Furlanetto, M Evans, W TI Embedded optical probes for simultaneous pressure and temperature measurement of materials in extreme conditions SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID SENSORS AB We present recent efforts at Los Alamos National Laboratory (LANL) to develop sensors for simultaneous, in situ pressure and temperature measurements under dynamic conditions by using an all-optical fiber-based approach While similar tests have been done previously in deflagration-to-detonation tests (DDT), where pressure and temperature were measured to 82 kbar and 400 degrees C simultaneously, here we demonstrate the use of embedded fiber grating sensors to obtain high temporal resolution, in situ pressure measurements in inert materials. We present two experimental demonstrations of pressure measurements: (1) under precise shock loading from a gas-gun driven plate impact and (2) under high explosive driven shock in a water filled vessel. The system capitalizes on existing telecom components and fast transient digitizing recording technology. It operates as a relatively inexpensive embedded probe (single-mode 1550 nm fiber-based Bragg grating) that provides a continuous fast pressure record during shock and/or detonation. By applying well-controlled shock wave pressure profiles to these inert materials, we study the dynamic pressure response of embedded fiber Bragg gratings to extract pressure amplitude of the shock wave and compare our results with particle velocity wave profiles measured simultaneously. C1 [Sandberg, R. L.; Rodriguez, G.] Los Alamos Natl Lab, Mat Phys & Applicat Div, POB 1663, Los Alamos, NM 87545 USA. [Gibson, L. L.; Dattelbaum, D. M.] Los Alamos Natl Lab, Weapons Expt Div, Los Alamos, NM 87545 USA. [Stevens, G. D.; Grover, M.; Lalone, B. M.] Special Technol Lab, Natl Secur Technol, Santa Barbara, CA 93111 USA. [Udd, E.] Columbia Gorge Res LLC, Columbia, OR 97024 USA. RP Sandberg, RL (reprint author), Los Alamos Natl Lab, Mat Phys & Applicat Div, POB 1663, Los Alamos, NM 87545 USA. EM sandberg@lanl.gov RI Rodriguez, George/G-7571-2012; OI Rodriguez, George/0000-0002-6044-9462; Sandberg, Richard/0000-0001-9719-8188 FU Department of Energy; Los Alamos National Security LLC FX We thank B. Bartram, A. Pacheco, and P. Ellsworth for help in fielding the experiments at Chamber 9. Funding for this work was provided by the DOE/ NNSA Campaign 2 and Gemini Project at Los Alamos National Laboratory under the auspices of the Department of Energy for Los Alamos National Security LLC. NR 10 TC 3 Z9 3 U1 1 U2 10 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR UNSP 142031 DI 10.1088/1742-6596/500/14/142031 PG 5 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900211 ER PT S AU Shan, TR Thompson, AP AF Shan, Tzu-Ray Thompson, Aidan P. BE Buttler, W Furlanetto, M Evans, W TI Shock-induced hotspot formation and chemical reaction initiation in PETN containing a spherical void SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID MOLECULAR-DYNAMICS SIMULATIONS; HOT-SPOT FORMATION; PENTAERYTHRITOL TETRANITRATE; FORCE-FIELD; SOLIDS; CRYSTALS; CAVITIES; COLLAPSE; REAXFF; SHEAR AB We present results of reactive molecular dynamics simulations of hotspot formation and chemical reaction initiation in shock-induced compression of pentaerythritol tetranitrate (PETN) with the ReaxFF reactive force field. A supported shockwave is driven through a PETN crystal containing a 20 nm spherical void at a sub-threshold impact velocity of 2 km/s. Formation of a hotspot due to shock-induced void collapse is observed. During void collapse, NO2 is the dominant species ejected from the upstream void surface. Once the ejecta collide with the downstream void surface and the hotspot develops, formation of final products such as N-2 and H2O is observed. The simulation provides a detailed picture of how void collapse and hotspot formation leads to initiation at sub-threshold impact velocities. C1 [Shan, Tzu-Ray; Thompson, Aidan P.] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Shan, TR (reprint author), Sandia Natl Labs, POB 5800, Albuquerque, NM 87185 USA. EM tnshan@sandia.gov NR 23 TC 6 Z9 7 U1 0 U2 8 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 172009 DI 10.1088/1742-6596/500/17/172009 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900245 ER PT S AU Springer, HK Tarver, CM Reaugh, JE May, CM AF Springer, H. K. Tarver, C. M. Reaugh, J. E. May, C. M. BE Buttler, W Furlanetto, M Evans, W TI Investigating short-pulse shock initiation in HMX-based explosives with reactive meso-scale simulations SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID ENERGETIC MATERIALS AB We performed reactive meso-scale simulations of short-pulse experiments to study the influence of flyer velocity and pore structure on shock initiation of LX-10 (95wt% HMX, 5wt% Viton A). Our calculations show that the reaction evolution fit a power law relationship in time and increases with increasing porosity, decreasing pore size, and increasing flyer velocity. While heterogeneous shock initiation modes, dependent on hot spot mechanisms, are predicted at lower flyer velocities, mixed heterogeneous-homogeneous shock initiation modes, less dependent on hot spots, are predicted at higher velocities. These studies are important because they enable the development of predictive shock initiation models that incorporate complex microstructure and can be used to optimize performance-safety characteristics of explosives. C1 [Springer, H. K.; Tarver, C. M.; Reaugh, J. E.; May, C. M.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. RP Springer, HK (reprint author), Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. EM keo@llnl.gov NR 21 TC 5 Z9 5 U1 4 U2 25 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 052041 DI 10.1088/1742-6596/500/5/052041 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900075 ER PT S AU Tappan, BC Hill, LG Manner, VW Pemberton, SJ Lieber, MA Johnson, CE Sanders, VE AF Tappan, B. C. Hill, L. G. Manner, V. W. Pemberton, S. J. Lieber, M. A. Johnson, C. E. Sanders, V. E. BE Buttler, W Furlanetto, M Evans, W TI High-temperature and pressure aluminum reactions in carbon dioxide rich post-detonation environments SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing AB Powdered aluminum is a common additive to energetic materials, but little is understood regarding its reaction rate at very high temperatures and pressures in specific oxidizing gases such as carbon dioxide. Aluminum reaction kinetics in carbon dioxide have been studied in various reaction conditions, but difficulties arise in the more specific study of Al oxidation at the high pressures and temperatures in detonation reactions. To study these reactions, small particle size Al or the inert surrogate, LiF, was added to the energetic material benzotrifuroxan (BTF). BTF is a hydrogen-free material that selectively forms CO2 as the major oxidizing species for post-detonation Al oxidation. High-fidelity PDV measurements were utilized for early wall velocity expansion measurements in 12.7 mm copper cylinders. The JWL equation of state was solved to determine temperature, pressure and energies at specific time periods. A genetic algorithm was used in conjunction with a numerical simulation hydrocode, ALE3D, which enables the elucidation of aluminum reaction extent. By comparison of the Al oxidation with LiF, data indicate that Al oxidation occurs on an extremely fast time scale, beginning and completing between 1 and 25 microseconds. Unconfined, 6.4 mm diameter rate-sticks were also utilized to determine the effect of Al compared to LiF on detonation velocity. C1 [Tappan, B. C.; Hill, L. G.; Manner, V. W.; Pemberton, S. J.; Lieber, M. A.; Johnson, C. E.; Sanders, V. E.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Tappan, BC (reprint author), Los Alamos Natl Lab, Los Alamos, NM 87545 USA. EM btappan@lanl.gov NR 5 TC 0 Z9 0 U1 0 U2 3 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 052043 DI 10.1088/1742-6596/500/5/052043 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900077 ER PT S AU Tarver, CM Chidester, SK AF Tarver, Craig M. Chidester, Steven K. BE Buttler, W Furlanetto, M Evans, W TI Ignition and growth modeling of short pulse shock initiation experiments on fine particle Hexanitrostilbene (HNS) SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing AB Hexanitrostilbene (HNS) is a booster explosive that is usually initiated using short pulse duration shock waves produced by high velocity impacts with thin flyer plates. HNS is generally used at a density of 1.60 g/cm(3), which implies a porosity of 8%. It has been produced in several forms (I -IV, ultrafine, etc.) with various particle surface areas. The threshold flyer velocities for shock induced detonation versus failure to detonate for these different surface area materials vary slightly, but, in this paper, an average Ignition and Growth reactive flow model parameter set was determined using all of the experimental data from several aluminium and Kapton (TM) flyer plate studies. This data ranged from shock pressures of 4 GPa to above the Chapman-Jouguet (C-J) detonation pressure (similar to 20 GPa) and from 1 to 120 nanoseconds in time duration. Good agreement was obtained for the available short pulse duration detonation verses failure to threshold flyer velocity data using the Ignition and Growth model, C1 [Tarver, Craig M.; Chidester, Steven K.] Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. RP Tarver, CM (reprint author), Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. EM tarver1@llnl.gov NR 13 TC 1 Z9 1 U1 0 U2 10 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 052044 DI 10.1088/1742-6596/500/5/052044 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900078 ER PT S AU Thompson, AP Shan, TR AF Thompson, Aidan P. Shan, Tzu-Ray BE Buttler, W Furlanetto, M Evans, W TI Reactive atomistic simulations of shock-induced initiation processes in mixtures of ammonium nitrate and fuel oil SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID MOLECULAR-DYNAMICS; FORCE-FIELD; TEMPERATURE; STATE; REAXFF; ND4NO3; H2O-N2 AB Ammonium nitrate mixed with fuel oil (ANFO) is a commonly used blasting agent. In this paper we investigated the shock properties of pure ammonium nitrate (AN) and two different mixtures of ammonium nitrate and n-dodecane by characterizing their Hugoniot states. We simulated shock compression of pure AN and ANFO mixtures using the Multi-scale Shock Technique, and observed differences in chemical reaction. We also performed a large-scale explicit sub-threshold shock of AN crystal with a 10 nm void filled with 4.4 wt% of n-dodecane. We observed the formation of hotspots and enhanced reactivity at the interface region between AN and n-dodecane molecules. C1 [Thompson, Aidan P.; Shan, Tzu-Ray] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Thompson, AP (reprint author), Sandia Natl Labs, POB 5800, Albuquerque, NM 87185 USA. EM athomps@sandia.gov NR 28 TC 2 Z9 2 U1 2 U2 6 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 DI 10.1088/1742-6596/500/5/052046 PG 8 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900080 ER PT S AU Thompson, DG DeLuca, R Archuleta, J Brown, GW Koby, J AF Thompson, Darla Graff DeLuca, Racci Archuleta, Jose Brown, Geoff W. Koby, Joseph BE Buttler, W Furlanetto, M Evans, W TI Taylor impact tests on PBX composites: imaging and analysis SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing AB A series of Taylor impact tests were performed on three plastic bonded explosive (PBX) formulations: PBX 9501, PBXN-9 and HPP (propellant). The first two formulations are HMX-based, and all three have been characterized quasi-statically in tension and compression. The Taylor impact tests use a 500 psi gas gun to launch PBX projectiles (approximately 30 grams, 16 mm diameter, 76 mm long), velocities as high as 215 m/s, at a steel anvil. Tests were performed remotely and no sign of ignition/reaction have been observed to date. Highspeed imaging was used to capture the impact of the specimen onto anvil surface. Side-view contour images have been analyzed using dynamic stress equations from the literature, and additionally, front-view images have been used to estimate a tensile strain failure criterion for initial specimen fracture. Post-test sieve analysis of specimen debris correlates fragmentation with projectile velocity, and these data show interesting differences between composites. Along with other quasi-static and dynamic measurements, Taylor impact images and fragmentation data provide a useful metric for the calibration or evaluation of intermediate-rate model predictions of PBX constituitive response and failure/fragmentation. Intermediate-rate tests involving other impact configurations are being considered. C1 [Thompson, Darla Graff; DeLuca, Racci; Archuleta, Jose; Brown, Geoff W.; Koby, Joseph] Los Alamos Natl Lab, High Explos Sci & Technol, Los Alamos, NM 87545 USA. RP Thompson, DG (reprint author), Los Alamos Natl Lab, High Explos Sci & Technol, WX-7, Los Alamos, NM 87545 USA. EM dkgraff@lanl.gov NR 5 TC 0 Z9 0 U1 1 U2 10 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 112062 DI 10.1088/1742-6596/500/11/112062 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900164 ER PT S AU Tringe, JW Kane, RJ Lorenz, KT Baluyot, EV Vandersall, KS AF Tringe, J. W. Kane, R. J. Lorenz, K. T. Baluyot, E. V. Vandersall, K. S. BE Buttler, W Furlanetto, M Evans, W TI Dielectric characterization and microwave interferometry in HMX-based explosives SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID POROUS-MEDIA; SHOCK-WAVES; DETONATION AB Microwave interferometry is a useful technique for understanding the development and propagation of detonation waves. The velocity of the front can be determined directly with the dielectric constant of the explosive and the instantaneous phase difference of the reflected microwave signal from the detonation front. However, the dielectric constant of HMX-based explosives has been measured only over a small range of wavelengths. Here we employ an open-ended coaxial probe to determine the complex dielectric constant for LX-10 and other HMX-based explosives over the 5-20 GHz range. The propagation of a detonation wave in a lightly-confined cylindrical charge geometry is described where the microwave-reflective properties of the detonation front are characterized with a waveguide. For comparison, piezoelectric pins were used to measure the detonation velocity and indirectly estimate the dielectric constant of LX-10 at 26.5 GHz. Future work in this area will also be discussed. C1 [Tringe, J. W.; Kane, R. J.; Lorenz, K. T.; Baluyot, E. V.; Vandersall, K. S.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. RP Tringe, JW (reprint author), Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. EM tringe2@llnl.gov NR 12 TC 0 Z9 0 U1 0 U2 5 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 142033 DI 10.1088/1742-6596/500/14/142033 PG 5 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900213 ER PT S AU Vandersall, KS Garcia, F Fried, LE Tarver, CM AF Vandersall, Kevin S. Garcia, Frank Fried, Laurence E. Tarver, Craig M. BE Buttler, W Furlanetto, M Evans, W TI Double shock experiments and reactive flow modeling on LX-17 to understand the reacted equation of state SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing AB Experimental data from measurements of the reacted state of an energetic material are desired to incorporate reacted states in modeling by computer codes. In a case such as LX-17 (92.5% TATB and 7.5% Kel-F by weight), where the time dependent kinetics of reaction is still not fully understood and the reacted state may evolve over time, this information becomes even more vital. Experiments were performed to measure the reacted state of LX-17 using a double shock method involving the use of two flyer materials (with known properties) mounted on the projectile that send an initial shock through the material close to or above the Chapman-Jouguet (CJ) state followed by a second shock at a higher magnitude into the detonated material. By measuring the parameters of the first and second shock waves, information on the reacted state can be obtained. The LX-17 detonation reaction zone profiles plus the arrival times and amplitudes of reflected shocks in LX-17 detonation reaction products were measured using Photonic Doppler Velocimetry (PDV) probes and an aluminum foil coated LiF window. A discussion of this work will include the experimental parameters, velocimetry profiles, data interpretation, reactive CHEETAH and Ignition and Growth modeling, as well as detail on possible future experiments. C1 [Vandersall, Kevin S.; Garcia, Frank; Fried, Laurence E.; Tarver, Craig M.] Lawrence Livermore Natl Lab, Energet Mat Ctr, Livermore, CA 94550 USA. RP Vandersall, KS (reprint author), Lawrence Livermore Natl Lab, Energet Mat Ctr, 7000 East Ave,L-282, Livermore, CA 94550 USA. EM vandersall1@llnl.gov RI Fried, Laurence/L-8714-2014 OI Fried, Laurence/0000-0002-9437-7700 NR 11 TC 0 Z9 0 U1 0 U2 13 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR 052047 DI 10.1088/1742-6596/500/5/052047 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900081 ER PT S AU Velisavljevic, N Sinogeikin, S Saavedra, R Chellappa, RS Rothkirch, A Dattelbaum, DM Konopkova, Z Liermann, HP Bishop, M Tsoi, GM Vohra, YK AF Velisavljevic, N. Sinogeikin, S. Saavedra, R. Chellappa, R. S. Rothkirch, A. Dattelbaum, D. M. Konopkova, Z. Liermann, H-P Bishop, M. Tsoi, G. M. Vohra, Y. K. BE Buttler, W Furlanetto, M Evans, W TI Time-resolved x-ray diffraction and electrical resistance measurements of structural phase transitions in zirconium SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID PRESSURE; METAL AB We have designed a portable pressure controller module to tune compression rates and maximum pressures attainable in a standard gas-membrane diamond anvil cell (DAC). During preliminary experiments, performed on zirconium (Zr) metal sample, pressure jumps of up to 80 GPa were systematically obtained in less than 0.2s (resulting in compression rate of few GPa/s up to more than 400 GPa/s). In-situ x-ray diffraction and electrical resistance measurements were performed simultaneously during this rapid pressure increase to provide the first time resolved data on alpha --> omega --> beta structural evolution in Zr at high pressures. Direct control of compression rates and peak pressures, which can be held for prolonged time, allows for investigation of structural evolution and kinetics of structural phase transitions of materials under previously unexplored compression rate-pressure conditions that bridge traditional static and shock/dynamic experimental platforms. C1 [Velisavljevic, N.; Saavedra, R.; Chellappa, R. S.; Dattelbaum, D. M.] Los Alamos Natl Lab, Los Alamos, NM 87544 USA. [Sinogeikin, S.] Carnegie Inst Sci, Geophys Lab, HPCAT, Argonne, IL USA. [Rothkirch, A.; Konopkova, Z.; Liermann, H-P] Deutsch Elektronen Synchrotron DESY, Hamburg, Germany. [Bishop, M.; Tsoi, G. M.; Vohra, Y. K.] Univ Alabama Birmingham, Dept Phys, Birmingham, AL USA. RP Velisavljevic, N (reprint author), Los Alamos Natl Lab, Los Alamos, NM 87544 USA. EM nenad@lanl.gov FU DOE- NNSA [DE-AC52-06NA25396, DE-NA0001974]; DOE/NNSA [DENA0002014]; DOE- BES [DE-FG02-99ER45775, DE-AC0206CH11357]; NSF; Bundesministerium fur Bildung und Forschung [05KS7RF1] FX Los Alamos National Laboratory (LANL) is operated by LANS, LLC for the DOE- NNSA under contract # DE-AC52-06NA25396. YKV is supported by the DOE/ NNSA under Award No. DENA0002014. Portions of this work were performed at HPCAT (Sector 16), Advanced Photon Source (APS), Argonne National Laboratory. HPCAT operations are supported by DOE-NNSA under Award No. DE-NA0001974 and DOE- BES under Award No. DE- FG02- 99ER45775, with partial instrumentation funding by NSF. APS is supported by DOE-BES, under Contract No. DE-AC0206CH11357. ECB- DESY was funded by the " Bundesministerium fur Bildung und Forschung" under contract 05KS7RF1 " Verbundprojekt: Messeinrichtungen fur die Material-und Strukturforschung an PETRAIII, Teilprojekt 2: Laserheizung fu"r die ' Extreme Conditions'-Station." We would also like to thank the HPCAT and ECB staff for their assistance. NR 12 TC 7 Z9 7 U1 1 U2 9 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR UNSP 032020 DI 10.1088/1742-6596/500/3/032020 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900032 ER PT S AU Wang, J Smith, RF Coppari, F Eggert, JH Boehly, TR Collins, GW Duffy, TS AF Wang, J. Smith, R. F. Coppari, F. Eggert, J. H. Boehly, T. R. Collins, G. W. Duffy, T. S. BE Buttler, W Furlanetto, M Evans, W TI Ramp compression of magnesium oxide to 234 GPa SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID EQUATION-OF-STATE; ISENTROPIC COMPRESSION; SOLIDS; TEMPERATURES; DYNAMICS; WAVES AB Single-crystal magnesium oxide (MgO) samples were ramp compressed to above 200 GPa pressure at the Omega laser facility. Multi-stepped MgO targets were prepared using lithography and wet etching techniques. Free surface velocities of ramp-compressed MgO were measured with a VISAR. The sound velocity and stress-density response were determined using an iterative Lagrangian analysis. The measured equation of state is consistent with expectations from previous shock and static data as well as with a recent X-ray diffraction measurement under ramp loading. The peak elastic stresses observed in our samples have amplitudes of 3-5.5 GPa, decreasing with propagation distance. C1 [Wang, J.; Duffy, T. S.] Princeton Univ, Dept Geosci, Princeton, NJ 08544 USA. [Smith, R. F.; Coppari, F.; Eggert, J. H.; Collins, G. W.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. [Boehly, T. R.] Univ Rochester, Laser Energet Lab, Rochester, NY 14623 USA. RP Wang, J (reprint author), Princeton Univ, Dept Geosci, Princeton, NJ 08544 USA. EM juewang@princeton.edu RI Duffy, Thomas/C-9140-2017 OI Duffy, Thomas/0000-0002-5357-1259 FU DOE [DE- NA000085, DEFG52- 09NA29037]; LLNL under LDRD [12- SI- 007] FX We acknowledge the Omega staff at LLE for their assistance and the Micro/ Nano fabrication laboratory staff ( Joe Palmer and George Watson) at Princeton University and the Target Engineering Team ( Stephanie Uhlich, Walt Unites, Timothy Uphaus and Russell Wallace) at LLNL for fabrication and metrology of the targets. The research was supported by DOE under DE- NA0000856 and DEFG52- 09NA29037 and LLNL under LDRD 12- SI- 007. NR 33 TC 0 Z9 1 U1 1 U2 11 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR UNSP 062002 DI 10.1088/1742-6596/500/6/062002 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900089 ER PT S AU Wehrenberg, C Comley, AJ Rudd, RE Terry, M Hawreliak, J Maddox, BR Prisbrey, ST Park, HS Remington, BA AF Wehrenberg, C. Comley, A. J. Rudd, R. E. Terry, M. Hawreliak, J. Maddox, B. R. Prisbrey, S. T. Park, H-S Remington, B. A. BE Buttler, W Furlanetto, M Evans, W TI Strain anisotropy and shear strength of shock compressed tantalum from in-situ Laue diffraction SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing AB Laser driven shock experiments were performed at the Omega facility to study the dynamic yield strength of similar to 5 mu m thick single crystal tantalum using in-situ Laue diffraction. Tantalum samples were shocked along the [001] direction to peak stresses up to 50 GPa and probed using a 150 ps pulse of bremsstrahlung radiation from an imploding CH capsule x-ray source timed for when the shock was halfway through the sample. The capsule implosion was monitored by a combination of pinhole cameras and DANTE x-ray diode scopes. Diffraction spots for both the undriven and driven regions of the sample were recorded simultaneously on image plate detectors. The strain state of the material was found by combining the strain anisotropy found from the driven diffraction pattern and with simultaneous VISAR measurements. C1 [Wehrenberg, C.; Rudd, R. E.; Terry, M.; Hawreliak, J.; Maddox, B. R.; Prisbrey, S. T.; Park, H-S; Remington, B. A.] Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. [Comley, A. J.] Atom Weap Estab, Reading RG7 4PR, Berks, England. RP Wehrenberg, C (reprint author), Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. EM wehrenberg1@llnl.gov FU U.S. Dept. of Energy (DOE); LLNL [DE-AC52-07NA27344] FX This work was performed under the auspices of the U.S. Dept. of Energy (DOE) by LLNL under Contract DE-AC52-07NA27344. NR 9 TC 2 Z9 2 U1 0 U2 9 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR UNSP 112064 DI 10.1088/1742-6596/500/11/112064 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900166 ER PT S AU White, BW Springer, HK Reaugh, JE AF White, B. W. Springer, H. K. Reaugh, J. E. BE Buttler, W Furlanetto, M Evans, W TI Computational studies of the skid test: Evaluation of the non-shock ignition of LX-10 using HERMES SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing AB We perform computational studies to evaluate the non-shock ignition response of LX-10 (95wt.% HMX, 5wt.% Viton A) during a skid impact test. We employ the HERMES (High Explosive Response to MEchanical Stimuli) model for LX-10 for Skid test calculations investigating the influence of drop height and angle on the pressure, strain-rate, strain, and ignition states. While grit is typically present in skid tests, it was not considered in these continuum-scale calculations. We found that the incident angle has a much more significant influence on pressure, strain-rate, strain, and ignition states than drop height. The peak HERMES ignition parameter value, Ign, is nearly one order of magnitude higher for an incident angle of 45 degrees than for 14 degrees. Peak Ign values occur at the contact patch where shear deformation is highest and is a result of the shear-dependence in the ignition criteria. While peak Ign values for Steven Tests were approximately 60, the skid test had a much smaller value < 2 for the scenarios considered in this study. The discrepancy in ignition values suggest that grit-explosive interactions play a significant role in skid test response. Since the peak ignition values are much less for the 14 degrees impact angles, the role of the grit may be more important at lower incident angles. Future work should include meso-scale calculations to resolve the localized grit interactions that underpins these shear ignition mechanisms. C1 [White, B. W.] Lawrence Livermore Natl Lab, Computat Engn Div, 7000 East Ave, Livermore, CA 94550 USA. [Springer, H. K.; Reaugh, J. E.] Lawrence Livermore Natl Lab, Div Chem Sci, Livermore, CA 94550 USA. RP White, BW (reprint author), Lawrence Livermore Natl Lab, Computat Engn Div, 7000 East Ave, Livermore, CA 94550 USA. EM white234@llnl.gov FU U. S. Department of Energy by Lawrence Livermore National Laboratory [AC52- 07NA27344]; DoD- DOE Munitions Technology Development Program 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. This work was supported by the Joint DoD- DOE Munitions Technology Development Program. NR 5 TC 0 Z9 0 U1 0 U2 5 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR UNSP 192021 DI 10.1088/1742-6596/500/19/192021 PG 6 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900312 ER PT S AU Yarrington, CD Kittell, D Wixom, RR Damm, DL AF Yarrington, C. D. Kittell, D. Wixom, R. R. Damm, D. L. BE Buttler, W Furlanetto, M Evans, W TI A Mie-Griineisen EOS with non-constant specific heat SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID SHOCK INITIATION; EXPLOSIVES; MODEL AB A complete and consistent equation of state based on Mie-Gruneisen assumptions was developed. This EOS assumes constant Gruneisen coefficient, but a variable specific heat that is modeled using Einstein's theory of heat capacities using two oscillators. The shock velocity particle velocity Hugoniot (Us-up) was derived from density functional theory molecular dynamics (DFT-MD). The EOS was formatted as a tabular EOS and checked for consistency using one-dimensional impact simulations in CTH. C1 [Yarrington, C. D.; Wixom, R. R.; Damm, D. L.] Sandia Natl Labs, POB 5800, Albuquerque, NM 87185 USA. [Kittell, D.] Purdue Univ, Dept Engn Mech, W Lafayette, IN USA. RP Yarrington, CD (reprint author), Sandia Natl Labs, POB 5800, Albuquerque, NM 87185 USA. EM cdyarri@sandia.gov FU U. S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX The authors wish to thank M. R. Baer for many fruitful discussions and continued technical contributions to this theory. 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 11 TC 0 Z9 0 U1 2 U2 6 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 DI 10.1088/1742-6596/500/5/052053 PG 5 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900087 ER PT S AU Zong, HX Xue, DZ Ding, XD Lookman, T AF Zong, Hongxiang Xue, Dezhen Ding, Xiangdong Lookman, Turab BE Buttler, W Furlanetto, M Evans, W TI Phase transformations in Titanium: Anisotropic deformation of omega phase SO 18TH APS-SCCM AND 24TH AIRAPT, PTS 1-19 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th Joint Int Conf of the APS Topical-Grp on Shock Compress of Condensed Matter / 24th Int Conf of the Int-Assoc-for-the-Advancement-of-High-Pressure-Sci-and-Technol CY JUL 07-12, 2013 CL Seattle, WA SP APS, Top Grp, Int Assoc Advancement High Pressure Sci & Technol, Aldermaston Weap Estab, Def Threat Reduct Agcy, Lawrence Livermore Natl Lab, Los Alamos Natl Lab, Sandia Natl Lab, Vis Res, NAC Image Technol, Specialized Imaging, Almax EasyLab, SMS Safety Management Serv, IOP Publishing ID HIGH-PRESSURE TORSION; ALLOYS; ZIRCONIUM; BEHAVIOR; ZR; TRANSITION; STRESS; METAL AB We study the plastic deformation of the omega phase which is obtained when Titanium undergoes a phase transformation under pressure. We perform molecular dynamics simulations under uniaxial loading and find that the omega phase not only shows brittle fracture upon loading in the [0001] direction, but also exhibits "superplastic" deformation features along the [10 (1) over bar0] direction. The brittle fracture is analogous to that which occurs in metallic glass by means of shear banding whereas the ductility is mediated by the a (hcp) to alpha (hexagonal) phase transformation. We further show that the elastic deformation of the omega phase is anisotropic; it can be non-uniform upon [0001] uniaxial compression. Our results provide insight into the mechanical behaviour of the omega phase and imply that the transformation mediated ductility can lead to improvement of the plasticity of omega-containing Titanium alloys. C1 [Zong, Hongxiang; Xue, Dezhen; Ding, Xiangdong] Xi An Jiao Tong Univ, State Key Lab Mech Behav Mat, Xian 710049, Peoples R China. [Zong, Hongxiang; Xue, Dezhen; Ding, Xiangdong; Lookman, Turab] Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. RP Zong, HX (reprint author), Xi An Jiao Tong Univ, State Key Lab Mech Behav Mat, Xian 710049, Peoples R China. EM txl@lanl.gov RI XUE, Dezhen/A-6062-2010; Ding, Xiangdong/K-4971-2013 OI XUE, Dezhen/0000-0001-6132-1236; Ding, Xiangdong/0000-0002-1220-3097 FU NSFC [51171140, 51231008]; 973 Program of China [2010CB631003, 2012CB619402]; 111 project [B06025]; US DOE at LANL [DE- AC52- 06NA25396] FX This work was supported by NSFC ( 51171140, 51231008), the 973 Program of China ( 2010CB631003, 2012CB619402) and 111 project ( B06025), as well as US DOE at LANL ( DE- AC52- 06NA25396). NR 32 TC 0 Z9 0 U1 0 U2 16 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 500 AR UNSP 112042 DI 10.1088/1742-6596/500/11/112042 PG 8 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA7QL UT WOS:000337722900144 ER PT S AU De Andrade, V Ganne, J Dubacq, B Ryan, CG Bourdelle, F Plunder, A Falkenberg, G Thieme, J AF De Andrade, V. Ganne, J. Dubacq, B. Ryan, C. G. Bourdelle, F. Plunder, A. Falkenberg, G. Thieme, J. GP IOP TI Retrieving past geodynamic events by unlocking rock archives with mu-XRF and mu-spectroscopy SO 22ND INTERNATIONAL CONGRESS ON X-RAY OPTICS AND MICROANALYSIS SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 22nd International Congress on X-Ray Optics and Microanalysis (ICXOM) CY SEP 02-06, 2013 CL Univ Hamburg, Hamburg, GERMANY SP DESY, TU Dresden, Helmholtz Zentrum Geesthacht HO Univ Hamburg ID PHASE-EQUILIBRIUM EXPERIMENTS; NATURAL PELITIC ASSEMBLAGES; X-RAY; THERMODYNAMIC MODEL; SILICATE-GLASSES; DETECTOR ARRAY; CHLORITE; MICROPROBE; XANES; THERMOBAROMETRY AB Rocks are commonly polycrystalline systems presenting multi-scale chemical and structural heterogeneities inherited from crystallization processes or successive metamorphic events. This work illustrates how spatially resolved analytical techniques coupled with thermodynamic approaches allow rock compositional variations to be related to large-scale geodynamic processes. Emphasis is placed on the contribution of quantitative chemical imaging to the study of 2.2-2.0 Gy old metamorphic rocks from the West African Craton. A thorough analysis of elemental chemical maps acquired on rock thin sections enabled high pressure relic minerals to be located and re-analyzed later with precise point analyses. The pressure-temperature conditions of crystallization calculated from these analyses are typical of modern subduction zones. These results push back the onset of modern-style plate tectonics to 2.15 Gy, i.e. more than one billion years earlier than was consensually accepted. The second part of the paper describes the imaging capabilities offered by the new ultra-bright diffraction limited synchrotron sources. Experimental data acquired with the Maia detector at beamline P06 at Petra III as well as simulations of mu-XRF spectra that will be generated at the SRX beamline at NSLS-II are presented. These results demonstrate that cm(2) large chemical maps can be acquired with submicron spatial resolution and a precision suitable for thermobarometric estimates, with dwell time smaller than 1 millisecond. The last part of the paper discusses the relevance of utilizing recent X-ray fluorescence nanoprobes for diagenetic to low grade metamorphism applications. C1 [De Andrade, V.] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. [De Andrade, V.; Thieme, J.] Brookhaven Natl Lab, Photon Sci, NSLS II, Upton, NY 11793 USA. [Ganne, J.] Univ Toulouse 3, IRD, UR 234, GET, F-31400 Toulouse, France. [Dubacq, B.; Plunder, A.] Univ Paris 06, ISTEP, UMR 7193, UPMC, F-75005 Paris, France. [Dubacq, B.; Plunder, A.] CNRS, ISTEP, UMR 7193, F-75005 Paris, France. [Ryan, C. G.] CSIRO, Earth Sci Resource Engn, Clayton, Vic 3168, Australia. [Bourdelle, F.] Univ Lorraine, GeoRessources, UMR 7359, F-54506 Vandoeuvre Les Nancy, France. [Plunder, A.] UMR CNRS 8538 Lab, Geol ENS, F-75005 F- Paris, France. [Falkenberg, G.] Photon Sci, Deutsch Elektronen Synchrotron DESY, Notkestr 85, D-22603 Hamburg, Germany. RP De Andrade, V (reprint author), Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. EM vdeandrade@anl.gov FU NSLS-II project; US department of Energy, Office of Science and Office of Basic Energy Sciences FX This work was financially supported by the NSLS-II project, itself funded by the US department of Energy, Office of Science and Office of Basic Energy Sciences. We are grateful to Ulrike Boesenberg and Gerd Wellenreuther from the P06 beamline team at Petra III, who helped setting up the experiment aiming to test the new Maia 384 detector. We also want to thank Robin Kirkham & Pete Siddons for their support and advices concerning the Maia. At last, thanks to Tom Schoonjans for his support in configuring the XMIMSIM software and the SRX team endeavoring to build an outstanding instrument. NR 40 TC 3 Z9 3 U1 0 U2 6 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 499 AR UNSP 012012 DI 10.1088/1742-6596/499/1/012012 PG 13 WC Optics; Physics, Applied SC Optics; Physics GA BA8FS UT WOS:000338041300012 ER PT S AU Ryan, CG Siddons, DP Kirkham, R Li, ZY de Jonge, MD Paterson, DJ Kuczewski, A Howard, DL Dunn, PA Falkenberg, G Boesenberg, U De Geronimo, G Fisher, LA Halfpenny, A Lintern, MJ Lombi, E Dyl, KA Jensen, M Moorhead, GF Cleverley, JS Hough, RM Godel, B Barnes, SJ James, SA Spiers, KM Alfeld, M Wellenreuther, G Vukmanovic, Z Borg, S AF Ryan, C. G. Siddons, D. P. Kirkham, R. Li, Z. Y. de Jonge, M. D. Paterson, D. J. Kuczewski, A. Howard, D. L. Dunn, P. A. Falkenberg, G. Boesenberg, U. De Geronimo, G. Fisher, L. A. Halfpenny, A. Lintern, M. J. Lombi, E. Dyl, K. A. Jensen, M. Moorhead, G. F. Cleverley, J. S. Hough, R. M. Godel, B. Barnes, S. J. James, S. A. Spiers, K. M. Alfeld, M. Wellenreuther, G. Vukmanovic, Z. Borg, S. GP IOP TI Maia X-ray fluorescence imaging: Capturing detail in complex natural samplesF SO 22ND INTERNATIONAL CONGRESS ON X-RAY OPTICS AND MICROANALYSIS SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 22nd International Congress on X-Ray Optics and Microanalysis (ICXOM) CY SEP 02-06, 2013 CL Univ Hamburg, Hamburg, GERMANY SP DESY, TU Dresden, Helmholtz Zentrum Geesthacht HO Univ Hamburg ID QUANTITATIVE PIXE MICROANALYSIS; NUCLEAR MICROPROBE; PROTON MICROPROBE; SOUTH-AUSTRALIA; GOLD PROSPECT; SYNCHROTRON; DETECTOR; SPECIATION; SPECTRA; COWPEA AB Motivated by the challenge of capturing complex hierarchical chemical detail in natural material from a wide range of applications, the Maia detector array and integrated real-time processor have been developed to acquire X-ray fluorescence images using X-ray Fluorescence Microscopy (XFM). Maia has been deployed initially at the XFM beamline at the Australian Synchrotron and more recently, demonstrating improvements in energy resolution, at the P06 beamline at Petra III in Germany. Maia captures fine detail in element images beyond 100 M pixels. It combines a large solid-angle annular energy-dispersive 384 detector array, stage encoder and flux counter inputs and dedicated FPGA-based real-time event processor with embedded spectral deconvolution. This enables high definition imaging and enhanced trace element sensitivity to capture complex trace element textures and place them in a detailed spatial context. Maia hardware and software methods provide per pixel correction for dwell, beam flux variation, dead-time and pileup, as well as off-line parallel processing for enhanced throughput. Methods have been developed for real-time display of deconvoluted SXRF element images, depth mapping of rare particles and the acquisition of 3D datasets for fluorescence tomography and XANES imaging using a spectral deconvolution method that tracks beam energy variation. C1 [Ryan, C. G.; Fisher, L. A.; Halfpenny, A.; Lintern, M. J.; Cleverley, J. S.; Hough, R. M.; Godel, B.; Barnes, S. J.; Vukmanovic, Z.; Borg, S.] CSIRO Earth Sci & Resource Engn, 26 Dick Perry Ave, Kensington, WA 6151, Australia. [Siddons, D. P.; Li, Z. Y.; Kuczewski, A.; De Geronimo, G.] Brookhaven Natl Lab, Upton, NY USA. [Kirkham, R.; Jensen, M.; Moorhead, G. F.; James, S. A.] CSIRO Mat Sci & Engn, Clayton, Vic 3168, Australia. [de Jonge, M. D.; Paterson, D. J.; Howard, D. L.; James, S. A.; Spiers, K. M.] Australian Synchrotron, Blackburn, Lancs, Australia. [Falkenberg, G.; Boesenberg, U.; Alfeld, M.] Photon Sci, DESY, D-22603 D- Hamburg, Germany. [Lombi, E.] Univ South Australia, Ctr Environm Risk Assessment & Remediat, Mawson Lakes, SA 5095, Australia. [Dyl, K. A.; Vukmanovic, Z.] Curtin Univ, Dept Appl Geol, Perth, WA 6845, Australia. [Wellenreuther, G.] European XFEL, Albert Einstein Ring 19, D-22761 Hamburg, Germany. RP Ryan, CG (reprint author), CSIRO Earth Sci & Resource Engn, 26 Dick Perry Ave, Kensington, WA 6151, Australia. EM chris.ryan@csiro.au RI Moorhead, Gareth/B-6634-2009; Kirkham, Robin/C-9786-2010; Halfpenny, Angela/G-3975-2011; Lombi, Enzo/F-3860-2013; Alfeld, Matthias/L-6748-2016; Barnes, Steve/A-6083-2011; James, Simon/J-5320-2012 OI Moorhead, Gareth/0000-0002-9299-9549; Kirkham, Robin/0000-0003-1012-3496; Halfpenny, Angela/0000-0001-6560-3134; Lombi, Enzo/0000-0003-3384-0375; Alfeld, Matthias/0000-0001-7974-9564; Barnes, Steve/0000-0002-4912-9177; James, Simon/0000-0001-9369-3288 NR 53 TC 25 Z9 25 U1 2 U2 25 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 499 AR UNSP 012002 DI 10.1088/1742-6596/499/1/012002 PG 12 WC Optics; Physics, Applied SC Optics; Physics GA BA8FS UT WOS:000338041300002 ER PT S AU Siddons, DP Kirkham, R Ryan, CG De Geronimo, G Dragone, A Kuczewski, AJ Li, ZY Carini, GA Pinelli, D Beuttenmuller, R Elliott, D Pfeffer, M Tyson, TA Moorhead, GF Dunn, PA AF Siddons, D. P. Kirkham, R. Ryan, C. G. De Geronimo, G. Dragone, A. Kuczewski, A. J. Li, Z. Y. Carini, G. A. Pinelli, D. Beuttenmuller, R. Elliott, D. Pfeffer, M. Tyson, T. A. Moorhead, G. F. Dunn, P. A. GP IOP TI Maia X-ray Microprobe Detector Array System SO 22ND INTERNATIONAL CONGRESS ON X-RAY OPTICS AND MICROANALYSIS SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 22nd International Congress on X-Ray Optics and Microanalysis (ICXOM) CY SEP 02-06, 2013 CL Univ Hamburg, Hamburg, GERMANY SP DESY, TU Dresden, Helmholtz Zentrum Geesthacht HO Univ Hamburg AB Maia is an advanced system designed specifically for scanning x-ray fluorescence microprobe applications. It consists of a large array of photodiode detectors and associated signal processing, closely coupled to an FPGA-based control and analysis system. In this paper we will describe the architecture and construction of the system. C1 [Siddons, D. P.; De Geronimo, G.; Kuczewski, A. J.; Pinelli, D.; Beuttenmuller, R.; Elliott, D.; Pfeffer, M.] Brookhaven Natl Lab, Upton, NY 11973 USA. [Dragone, A.; Carini, G. A.] SLAC Natl Accelerator Lab, Menlo Pk, CA 94025 USA. [Li, Z. Y.; Tyson, T. A.] New Jersey Inst Technol, Newark, NJ 07102 USA. [Ryan, C. G.] CSIRO Earth Sci & Resource Engn, Kensington, WA 6151, Australia. [Kirkham, R.; Moorhead, G. F.; Dunn, P. A.] CSIRO Mat Sci & Engn, Clayton, Vic 3168, Australia. RP Siddons, DP (reprint author), Brookhaven Natl Lab, Upton, NY 11973 USA. EM siddons@bnl.gov RI Moorhead, Gareth/B-6634-2009; Kirkham, Robin/C-9786-2010 OI Moorhead, Gareth/0000-0002-9299-9549; Kirkham, Robin/0000-0003-1012-3496 FU U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-ACO2-98CH10886]; National Science Foundation, Major Research Instrumentation [DMR 0722730]; U.S. Department of Energy [DE-ACO2-76SF00515] FX This work was supported at BNL by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-ACO2-98CH10886. The CSIRO work took place within the CSIRO Sensors and Sensor Networks Transformational Capability Platform. NJIT authors were supported by the National Science Foundation, Major Research Instrumentation Grant. DMR 0722730. SLAC is supported by the U.S. Department of Energy under contract number DE-ACO2-76SF00515. NR 12 TC 9 Z9 9 U1 1 U2 9 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 499 AR UNSP 012001 DI 10.1088/1742-6596/499/1/012001 PG 10 WC Optics; Physics, Applied SC Optics; Physics GA BA8FS UT WOS:000338041300001 ER PT J AU Lanekoff, I Stevens, SL Stenzel-Poore, MP Laskin, J AF Lanekoff, Ingela Stevens, Susan L. Stenzel-Poore, Mary P. Laskin, Julia TI Matrix effects in biological mass spectrometry imaging: identification and compensation SO ANALYST LA English DT Article ID DESORPTION ELECTROSPRAY-IONIZATION; RAT-BRAIN SECTIONS; CEREBRAL-ISCHEMIA; TISSUE-SECTIONS; WHITE-MATTER; FATTY-ACID; PHOSPHOLIPIDS; STROKE; LIPIDS; QUANTIFICATION AB Matrix effects in mass spectrometry imaging (MSI) may affect the observed molecular distribution in chemical and biological systems. In this study, we use mouse brain tissue of a middle cerebral artery occlusion (MCAO) stroke model to examine matrix effects in nanospray desorption electrospray ionization MSI (nano-DESI MSI). This is achieved by normalizing the intensity of the sodium and potassium adducts of endogenous phosphatidylcholine (PC) species to the intensity of the corresponding adduct of the PC standard supplied at a constant rate with the nano-DESI solvent. The use of MCAO model with an ischemic region localized to one hemisphere of the brain enables immediate comparison of matrix effects within one ion image. Furthermore, significant differences in sodium and potassium concentrations in the ischemic region in comparison with the healthy tissue allowed us to distinguish between two types of matrix effects. Specifically, we discuss matrix effects originating from variations in alkali metal concentrations and matrix effects originating from variations in the molecular composition of the tissue. Compensation for both types of matrix effects was achieved by normalizing the signals corresponding to endogenous PC to the signals of the standards. This approach, which does not introduce any complexity in sample preparation, efficiently compensates for signal variations resulting from differences in the local concentrations of sodium and potassium in tissue sections and from the complexity of the extracted analyte mixture derived from local variations in molecular composition. C1 [Lanekoff, Ingela; Laskin, Julia] Pacific NW Natl Lab, Div Phys Sci, Richland, WA 99352 USA. [Stevens, Susan L.; Stenzel-Poore, Mary P.] Oregon Hlth & Sci Univ, Dept Mol Microbiol & Immunol, Portland, OR 97201 USA. RP Laskin, J (reprint author), Pacific NW Natl Lab, Div Phys Sci, POB 999,K8-88, Richland, WA 99352 USA. EM Julia.Laskin@pnnl.gov RI Laskin, Julia/H-9974-2012 OI Laskin, Julia/0000-0002-4533-9644 FU Chemical Imaging Initiative, at Pacific Northwest National Laboratory (PNNL); U.S. Department of Energy (DOE) [DE-AC05-76RL01830]; DOE's Office of Biological and Environmental Research; NIH-NINDS [NS062381] FX The research described in this paper is part of the Chemical Imaging Initiative, at Pacific Northwest National Laboratory (PNNL) supported under the PNNL's Laboratory Directed Research and Development Program. PNNL is operated by Battelle for the U.S. Department of Energy (DOE) under Contract DE-AC05-76RL01830. The research was performed using EMSL, a national scientific user facility sponsored by the DOE's Office of Biological and Environmental Research and located at PNNL. Research performed at OHSU was supported by the NIH-NINDS NS062381 (MSP). We thank Dr Mingyue Liu and Valerie Conrad for excellent technical support. NR 52 TC 15 Z9 15 U1 4 U2 38 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 0003-2654 EI 1364-5528 J9 ANALYST JI Analyst PY 2014 VL 139 IS 14 BP 3528 EP 3532 DI 10.1039/c4an00504j PG 5 WC Chemistry, Analytical SC Chemistry GA AJ9LO UT WOS:000338032500004 PM 24802717 ER PT J AU Yu, Y Koller, J Jordanova, VK Zaharia, SG Godinez, HC AF Yu, Y. Koller, J. Jordanova, V. K. Zaharia, S. G. Godinez, H. C. TI Radiation belt data assimilation of a moderate storm event using a magnetic field configuration from the physics-based RAM-SCB model SO ANNALES GEOPHYSICAE LA English DT Article DE Magnetospheric physics; energetic particles, trapped ID PHASE-SPACE DENSITY; KALMAN FILTER; PARTICLE DATA; CODE; MAGNETOSPHERE; ENVIRONMENT; SHEET AB Data assimilation using Kalman filters provides an effective way of understanding both spatial and temporal variations in the outer electron radiation belt. Data assimilation is the combination of in situ observations and physical models, using appropriate error statistics to approximate the uncertainties in both the data and the model. The global magnetic field configuration is one essential element in determining the adiabatic invariants for the phase space density (PSD) data used for the radiation belt data assimilation. The lack of a suitable global magnetic field model with high accuracy is still a long-lasting problem. This paper employs a physics-based magnetic field configuration for the first time in a radiation belt data assimilation study for a moderate storm event on 19 December 2002. The magnetic field used in our study is the magnetically self-consistent inner magnetosphere model RAM-SCB, developed at Los Alamos National Laboratory (LANL). Furthermore, we apply a cubic spline interpolation method in converting the differential flux measurements within the energy spectrum, to obtain a more accurate PSD input for the data assimilation than the commonly used linear interpolation approach. Finally, the assimilation is done using an ensemble Kalman filter (EnKF), with a localized adaptive inflation (LAI) technique to appropriately account for model errors in the assimilation and improve the performance of the Kalman filter. The assimilative results are compared with results from another assimilation experiment using the Tsyganenko 2001S (T01S) magnetic field model, to examine the dependence on a magnetic field model. Results indicate that the data assimilations using different magnetic field models capture similar features in the radiation belt dynamics, including the temporal evolution of the electron PSD during a storm and the location of the PSD peak. The assimilated solution predicts the energy differential flux to a relatively good degree when compared with independent LANL-GEO in situ observations. A closer examination suggests that for the chosen storm event, the assimilation using the RAM-SCB predicts a better flux at most energy levels during storm recovery phase but is slightly worse in the storm main phase than the assimilation using the T01S model. C1 [Yu, Y.; Koller, J.; Jordanova, V. K.; Zaharia, S. G.; Godinez, H. C.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Yu, Y (reprint author), Los Alamos Natl Lab, Los Alamos, NM 87545 USA. EM yiqun@lanl.gov RI Koller, Josef/C-5591-2009; Yu, Yiqun/E-2710-2012; OI Koller, Josef/0000-0002-6770-4980; Yu, Yiqun/0000-0002-1013-6505; Jordanova, Vania/0000-0003-0475-8743 FU US Department of Energy; Los Alamos National Laboratory Directed Research and Development program FX This work was conducted under the auspices of the US Department of Energy, with support from the Los Alamos National Laboratory Directed Research and Development program. The authors thank Yue Chen and Geoff Reeves for helpful discussion. NR 36 TC 2 Z9 2 U1 0 U2 6 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 0992-7689 EI 1432-0576 J9 ANN GEOPHYS-GERMANY JI Ann. Geophys. PY 2014 VL 32 IS 5 BP 473 EP 483 DI 10.5194/angeo-32-473-2014 PG 11 WC Astronomy & Astrophysics; Geosciences, Multidisciplinary; Meteorology & Atmospheric Sciences SC Astronomy & Astrophysics; Geology; Meteorology & Atmospheric Sciences GA AJ8IQ UT WOS:000337947100001 ER PT J AU Scarino, AJ Obland, MD Fast, JD Burton, SP Ferrare, RA Hostetler, CA Berg, LK Lefer, B Haman, C Hair, JW Rogers, RR Butler, C Cook, AL Harper, DB AF Scarino, A. J. Obland, M. D. Fast, J. D. Burton, S. P. Ferrare, R. A. Hostetler, C. A. Berg, L. K. Lefer, B. Haman, C. Hair, J. W. Rogers, R. R. Butler, C. Cook, A. L. Harper, D. B. TI Comparison of mixed layer heights from airborne high spectral resolution lidar, ground-based measurements, and the WRF-Chem model during CalNex and CARES SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID AEROSOL OPTICAL-PROPERTIES; BOUNDARY-LAYER; MIXING HEIGHT; VALIDATION; PROFILES; WEATHER AB The California Research at the Nexus of Air Quality and Climate Change (CalNex) and Carbonaceous Aerosol and Radiative Effects Study (CARES) field campaigns during May and June 2010 provided a data set appropriate for studying the structure of the atmospheric boundary layer (BL). The NASA Langley Research Center (LaRC) airborne high spectral resolution lidar (HSRL) was deployed to California onboard the NASA LaRC B-200 aircraft to aid in characterizing aerosol properties during these two field campaigns. Measurements of aerosol extinction (532 nm), backscatter (532 and 1064 nm), and depolarization (532 and 1064 nm) profiles during 31 flights, many in coordination with other research aircraft and ground sites, constitute a diverse data set for use in characterizing the spatial and temporal distribution of aerosols, as well as the depth and variability of the daytime mixed layer (ML) height. The paper describes the modified Haar wavelet covariance transform method used to derive the ML heights from HSRL backscatter profiles. HSRL ML heights are validated using ML heights derived from two radiosonde profile sites during CARES. Comparisons between ML heights from HSRL and a Vaisala ceilometer operated during CalNex were used to evaluate the representativeness of a fixed measurement over a larger region. In the Los Angeles basin, comparisons of ML heights derived from HSRL measurements and ML heights derived from the ceilometer result in a very good agreement (mean bias difference of 10 m and correlation coefficient of 0.89) up to 30 km away from the ceilometer site, but are essentially uncorrelated for larger distances, indicating that the spatial variability of the ML height is significant over these distances and not necessarily well captured by limited ground stations. The HSRL ML heights are also used to evaluate the performance in simulating the temporal and spatial variability of ML heights from the Weather Research and Forecasting Chemistry (WRF-Chem) community model. When compared to aerosol ML heights from HSRL, thermodynamic ML heights from WRF-Chem were underpredicted in the CalNex and CARES regions, shown by a bias difference value of -157 m and -29 m, respectively. Better agreement over the Central Valley than in mountainous regions suggests that some variability in the ML height is not well captured at the 4 km grid resolution of the model. A small but significant number of cases have poor agreement when WRF-Chem consistently overestimates the ML height in the late afternoon. Additional comparisons with WRF-Chem aerosol mixed layer heights show no significant improvement over thermodynamic ML heights, confirming that any differences between measurement and model are not due to the methodology of ML height determination. C1 [Scarino, A. J.; Butler, C.] Sci Syst & Applicat Inc, Hampton, VA 23666 USA. [Obland, M. D.; Burton, S. P.; Ferrare, R. A.; Hostetler, C. A.; Hair, J. W.; Rogers, R. R.; Cook, A. L.; Harper, D. B.] NASA, Langley Res Ctr, Hampton, VA 23665 USA. [Fast, J. D.; Berg, L. K.] Pacific NW Natl Lab, Richland, WA 99352 USA. [Lefer, B.] Univ Houston, Dept Earth & Atmospher Sci, Houston, TX USA. [Haman, C.] Trinity Consultants, Baton Rouge, LA USA. RP Scarino, AJ (reprint author), Sci Syst & Applicat Inc, Hampton, VA 23666 USA. EM amy.jo.scarino@nasa.gov RI Berg, Larry/A-7468-2016; Scarino, Angela/F-3593-2013 OI Berg, Larry/0000-0002-3362-9492; Scarino, Angela/0000-0001-7389-3717 FU NASA Science Mission Directorate; Department of Energy Atmospheric Systems Research program [DE-AI02-05ER63985]; Office of Science, Office of Biological and Environmental Research (OBER); NASA CALIPSO project FX The funding for this research came from the NASA Science Mission Directorate, the Department of Energy Atmospheric Systems Research program (interagency agreement DE-AI02-05ER63985), the Office of Science, Office of Biological and Environmental Research (OBER), and the NASA CALIPSO project. DOE's ARM Climate Research Facility supported logistics and data collection during CARES. We would also like to thank Dave Turner for writing a significant amount of the code for the Haar Wavelet Covariance program that is applied to the HSRL aerosol backscatter. The authors would also like to thank the NASA Langley King Air B-200 flight crew for their outstanding work supporting these flights and measurements. NR 40 TC 13 Z9 14 U1 1 U2 20 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 2014 VL 14 IS 11 BP 5547 EP 5560 DI 10.5194/acp-14-5547-2014 PG 14 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA AJ6KO UT WOS:000337803100016 ER PT J AU Li, M Zhang, Q Streets, DG He, KB Cheng, YF Emmons, LK Huo, H Kang, SC Lu, Z Shao, M Su, H Yu, X Zhang, Y AF Li, M. Zhang, Q. Streets, D. G. He, K. B. Cheng, Y. F. Emmons, L. K. Huo, H. Kang, S. C. Lu, Z. Shao, M. Su, H. Yu, X. Zhang, Y. TI Mapping Asian anthropogenic emissions of non-methane volatile organic compounds to multiple chemical mechanisms SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID AIR-POLLUTION SOURCES; PEARL RIVER-DELTA; BIOMASS-BURNING EMISSIONS; SOURCE APPORTIONMENT; PART II; HYDROCARBONS NMHCS; MOTOR-VEHICLES; UNITED-STATES; SURFACE OZONE; VERSION 2 AB An accurate speciation mapping of non-methane volatile organic compounds (NMVOC) emissions has an important impact on the performance of chemical transport models (CTMs) in simulating ozone mixing ratios and secondary organic aerosols. Taking the INTEX-B Asian NMVOC emission inventory as the case, we developed an improved speciation framework to generate model-ready anthropogenic NMVOC emissions for various gas-phase chemical mechanisms commonly used in CTMs in this work, by using an explicit assignment approach and updated NMVOC profiles. NMVOC profiles were selected and aggregated from a wide range of new measurements and the SPECIATE database v.4.2. To reduce potential uncertainty from individual measurements, composite profiles were developed by grouping and averaging source profiles from the same category. The fractions of oxygenated volatile organic compounds (OVOC) were corrected during the compositing process for those profiles which used improper sampling and analyzing methods. Emissions of individual species were then lumped into species in different chemical mechanisms used in CTMs by applying mechanism-dependent species mapping tables, which overcomes the weakness of inaccurate mapping in previous studies. Emission estimates for individual NMVOC species differ between one and three orders of magnitude for some species when different sets of profiles are used, indicating that source profile is the most important source of uncertainties of individual species emissions. However, those differences are diminished in lumped species as a result of the lumping in the chemical mechanisms. Gridded emissions for eight chemical mechanisms at 30 min x 30 min resolution as well as the auxiliary data are available at < a href='http://mic.greenresource.cn/intex-b2006'target='_blank'> http://mic.greenresource.cn/intex-b2006 . The framework proposed in this work can be also used to develop speciated NMVOC emissions for other regions. C1 [Li, M.; Zhang, Q.] Tsinghua Univ, Minist Educ Key Lab Earth Syst Modeling, Ctr Earth Syst Sci, Beijing 100084, Peoples R China. [Li, M.; He, K. B.; Kang, S. C.] Tsinghua Univ, State Key Joint Lab Environm Simulat & Pollut Con, Sch Environm, Beijing 100084, Peoples R China. [Streets, D. G.; Lu, Z.] Argonne Natl Lab, Decis & Informat Sci Div, Argonne, IL 60439 USA. [Cheng, Y. F.; Su, H.] Max Planck Inst Chem, Multiphase Chem Dept, D-55128 Mainz, Germany. [Emmons, L. K.] Natl Ctr Atmospher Res, Div Atmospher Chem, Boulder, CO 80307 USA. [Huo, H.] Tsinghua Univ, Inst Energy Environm & Econ, Beijing 100084, Peoples R China. [Shao, M.] Peking Univ, State Key Joint Lab Environm Simulat & Pollut Con, Coll Environm Sci & Engn, Beijing 100871, Peoples R China. [Yu, X.] Beijing Green Resource Res Co Ltd, Beijing, Peoples R China. [Zhang, Y.] N Carolina State Univ, Dept Marine Earth & Atmospher Sci, Raleigh, NC 27695 USA. RP Zhang, Q (reprint author), Tsinghua Univ, Minist Educ Key Lab Earth Syst Modeling, Ctr Earth Syst Sci, Beijing 100084, Peoples R China. EM qiangzhang@tsinghua.edu.cn RI Su, Hang/A-6226-2010; Zhang, Qiang/D-9034-2012; Cheng, Yafang/F-9362-2010; Emmons, Louisa/R-8922-2016 OI Su, Hang/0000-0003-4889-1669; Cheng, Yafang/0000-0003-4912-9879; Emmons, Louisa/0000-0003-2325-6212 FU China's National Basic Research Program [2010CB951803, 2014CB441301]; National Science Foundation of China [41222036, 21221004]; Tsinghua University Initiative Research Program [2011Z01026]; US EPA STAR at Argonne National Laboratory [R83337601]; North Carolina State University FX The work was supported by China's National Basic Research Program (2010CB951803 and 2014CB441301), the National Science Foundation of China (41222036 and 21221004), and the Tsinghua University Initiative Research Program (2011Z01026). This work was partly sponsored by the US EPA STAR grant R83337601 at Argonne National Laboratory and North Carolina State University. NR 70 TC 33 Z9 34 U1 9 U2 47 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 2014 VL 14 IS 11 BP 5617 EP 5638 DI 10.5194/acp-14-5617-2014 PG 22 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA AJ6KO UT WOS:000337803100020 ER PT J AU Yan, F Winijkul, E Streets, DG Lu, Z Bond, TC Zhang, Y AF Yan, F. Winijkul, E. Streets, D. G. Lu, Z. Bond, T. C. Zhang, Y. TI Global emission projections for the transportation sector using dynamic technology modeling SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID EXHAUST PARTICULATE MATTER; SULFUR-DIOXIDE EMISSIONS; DUTY DIESEL VEHICLES; BLACK CARBON; SHIPPING EMISSIONS; NO(X) EMISSIONS; AIR-POLLUTANTS; CLIMATE; ROAD; INVENTORY AB In this study, global emissions of gases and particles from the transportation sector are projected from the year 2010 to 2050. The Speciated Pollutant Emission Wizard (SPEW)-Trend model, a dynamic model that links the emitter population to its emission characteristics, is used to project emissions from on-road vehicles and non-road engines. Unlike previous models of global emission estimates, SPEW-Trend incorporates considerable detail on the technology stock and builds explicit relationships between socioeconomic drivers and technological changes, such that the vehicle fleet and the vehicle technology shares change dynamically in response to economic development. Emissions from shipping, aviation, and rail are estimated based on other studies so that the final results encompass the entire transportation sector. The emission projections are driven by four commonly-used IPCC (Intergovernmental Panel on Climate Change) scenarios (A1B, A2, B1, and B2). With global fossil-fuel use (oil and coal) in the transportation sector in the range of 128-171 EJ across the four scenarios, global emissions are projected to be 101-138 Tg of carbon monoxide (CO), 44-54 Tg of nitrogen oxides (NOx), 14-18 Tg of non-methane total hydrocarbons (THC), and 3.6-4.4 Tg of particulate matter (PM) in the year 2030. At the global level, a common feature of the emission scenarios is a projected decline in emissions during the first one or two decades (2010-2030), because the effects of stringent emission standards offset the growth in fuel use. Emissions increase slightly in some scenarios after 2030, because of the fast growth of on-road vehicles with lax or no emission standards in Africa and increasing emissions from non-road gasoline engines and shipping. On-road vehicles and non-road engines contribute the most to global CO and THC emissions, while on-road vehicles and shipping contribute the most to NOx and PM emissions. At the regional level, Latin America and East Asia are the two largest contributors to global CO and THC emissions in the year 2010; this dominance shifts to Africa and South Asia in the future. By the year 2050, for CO and THC emissions, non-road engines contribute the greatest fraction in Asia and the former USSR, while on-road vehicles make the largest contribution in Latin America, Africa, and the Middle East; for NOx and PM emissions, shipping controls the trend in most regions. These forecasts include a formal treatment of the factors that drive technology choices in the global vehicle sector and therefore represent a robust and plausible projection of what future emissions may be. These results have important implications for emissions of gases and aerosols that influence air quality, human health, and climate change. C1 [Yan, F.; Winijkul, E.; Streets, D. G.; Lu, Z.] Argonne Natl Lab, Decis & Informat Sci Div, Argonne, IL 60439 USA. [Yan, F.; Streets, D. G.; Lu, Z.] Univ Chicago, Computat Inst, Chicago, IL 60637 USA. [Winijkul, E.; Bond, T. C.] Univ Illinois, Dept Civil & Environm Engn, Urbana, IL 61801 USA. [Zhang, Y.] N Carolina State Univ, Dept Marine Earth & Atmospher Sci, Raleigh, NC 27695 USA. RP Yan, F (reprint author), Argonne Natl Lab, Decis & Informat Sci Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM fangyan@anl.gov RI Bond, Tami/A-1317-2013 OI Bond, Tami/0000-0001-5968-8928 FU US Department of Agriculture; National Institute of Food and Agriculture [2012-67003-30192]; National Science Foundation EaSM program at NCSU [AGS-1049200]; US Department of Energy [DE-AC02-06CH11357] FX This work is supported by the US Department of Agriculture, National Institute of Food and Agriculture, through the award number 2012-67003-30192 to the University of Chicago and by the National Science Foundation EaSM program, through the award number AGS-1049200 at NCSU. We are grateful for the support of the USDA Project Officer, L. M. Tupas, and the NSF Program Director, A. S. Bamzai. Argonne National Laboratory is operated by UChicago Argonne, LLC under Contract no. DE-AC02-06CH11357 with the US Department of Energy. NR 111 TC 11 Z9 11 U1 9 U2 44 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 2014 VL 14 IS 11 BP 5709 EP 5733 DI 10.5194/acp-14-5709-2014 PG 25 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA AJ6KO UT WOS:000337803100025 ER PT J AU Liu, M Rajagopalan, K Chung, SH Jiang, X Harrison, J Nergui, T Guenther, A Miller, C Reyes, J Tague, C Choate, J Salathe, EP Stockle, CO Adam, JC AF Liu, M. Rajagopalan, K. Chung, S. H. Jiang, X. Harrison, J. Nergui, T. Guenther, A. Miller, C. Reyes, J. Tague, C. Choate, J. Salathe, E. P. Stoeckle, C. O. Adam, J. C. TI What is the importance of climate model bias when projecting the impacts of climate change on land surface processes? SO BIOGEOSCIENCES LA English DT Article ID SYSTEMS SIMULATION-MODEL; WESTERN UNITED-STATES; DAILY SOLAR-RADIATION; LONG-TERM TRENDS; PACIFIC-NORTHWEST; COASTAL ZONE; SPATIALLY EXPLICIT; GLOBAL-MODEL; BIOGENIC EMISSIONS; FIELD SIGNIFICANCE AB Regional climate change impact (CCI) studies have widely involved downscaling and bias correcting (BC) global climate model (GCM)-projected climate for driving land surface models. However, BC may cause uncertainties in projecting hydrologic and biogeochemical responses to future climate due to the impaired spatiotemporal covariance of climate variables and a breakdown of physical conservation principles. Here we quantify the impact of BC on simulated climate-driven changes in water variables (evapotranspiration (ET), runoff, snow water equivalent (SWE), and water demand for irrigation), crop yield, biogenic volatile organic compounds (BVOC), nitric oxide (NO) emissions, and dissolved inorganic nitrogen (DIN) export over the Pacific Northwest (PNW) region. We also quantify the impacts on net primary production (NPP) over a small watershed in the region (HJ-Andrews). Simulation results from the coupled ECHAM5-MPI-OM model with A1B emission scenario were first dynamically downscaled to 12 km resolution with the WRF model. Then a quantile-mapping-based statistical downscaling model was used to downscale them into 1/16 degrees resolution daily climate data over historical and future periods. Two climate data series were generated, with bias correction (BC) and without bias correction (NBC). Impact models were then applied to estimate hydrologic and biogeochemical responses to both BC and NBC meteorological data sets. These impact models include a macroscale hydrologic model (VIC), a coupled cropping system model (VIC-CropSyst), an ecohydrological model (RHESSys), a biogenic emissions model (MEGAN), and a nutrient export model (Global-NEWS). Results demonstrate that the BC and NBC climate data provide consistent estimates of the climate-driven changes in water fluxes (ET, runoff, and water demand), VOCs (isoprene and monoterpenes) and NO emissions, mean crop yield, and river DIN export over the PNW domain. However, significant differences rise from projected SWE, crop yield from dry lands, and HJ-Andrews's ET between BC and NBC data. Even though BC post-processing has no significant impacts on most of the studied variables when taking PNW as a whole, their effects have large spatial variations and some local areas are substantially influenced. In addition, there are months during which BC and NBC post-processing produces significant differences in projected changes, such as summer runoff. Factor-controlled simulations indicate that BC post-processing of precipitation and temperature both substantially contribute to these differences at regional scales. We conclude that there are trade-offs between using BC climate data for offline CCI studies versus directly modeled climate data. These trade-offs should be considered when designing integrated modeling frameworks for specific applications; for example, BC may be more important when considering impacts on reservoir operations in mountainous watersheds than when investigating impacts on biogenic emissions and air quality, for which VOCs are a primary indicator. C1 [Liu, M.; Rajagopalan, K.; Chung, S. H.; Nergui, T.; Guenther, A.; Reyes, J.; Adam, J. C.] Washington State Univ, Pullman, WA 99164 USA. [Jiang, X.] NCAR Earth Syst Lab, Div Atmospher Chem, Boulder, CO USA. [Harrison, J.; Miller, C.] Washington State Univ, Sch Environm, Vancouver, WA USA. [Guenther, A.] Pacific NW Natl Lab, Richland, WA 99352 USA. [Tague, C.; Choate, J.] Univ Calif Santa Barbara, Bren Sch Environm Sci & Management, Santa Barbara, CA 93106 USA. [Salathe, E. P.] Univ Washington, Sch Sci Technol Engn & Math, Bothell, WA USA. [Stoeckle, C. O.] Washington State Univ, Dept Biol Syst Engn, Pullman, WA 99164 USA. RP Adam, JC (reprint author), Washington State Univ, Pullman, WA 99164 USA. EM jcadam@wsu.edu RI Liu, Mingliang/B-1361-2009; Guenther, Alex/B-1617-2008 OI Guenther, Alex/0000-0001-6283-8288 FU United States Department of Agriculture [20116700330346]; National Science Foundation [0903714] FX This study has been supported by the United States Department of Agriculture (grant no. 20116700330346 for the Biosphere-relevant Earth system modeling project, BioEarth) and the National Science Foundation (grant no. 0903714 for Nitrogen Systems: Policy-oriented Integrated Research and Education program, NSPIRE). NR 108 TC 6 Z9 6 U1 9 U2 46 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1726-4170 EI 1726-4189 J9 BIOGEOSCIENCES JI Biogeosciences PY 2014 VL 11 IS 10 BP 2601 EP 2622 DI 10.5194/bg-11-2601-2014 PG 22 WC Ecology; Geosciences, Multidisciplinary SC Environmental Sciences & Ecology; Geology GA AJ8IU UT WOS:000337947500004 ER PT J AU Vicca, S Bahn, M Estiarte, M van Loon, EE Vargas, R Alberti, G Ambus, P Arain, MA Beier, C Bentley, LP Borken, W Buchmann, N Collins, SL de Dato, G Dukes, JS Escolar, C Fay, P Guidolotti, G Hanson, PJ Kahmen, A Kroel-Dulay, G Ladreiter-Knauss, T Larsen, KS Lellei-Kovacs, E Lebrija-Trejos, E Maestre, FT Marhan, S Marshall, M Meir, P Miao, Y Muhr, J Niklaus, PA Ogaya, R Penuelas, J Poll, C Rustad, LE Savage, K Schindlbacher, A Schmidt, IK Smith, AR Sotta, ED Suseela, V Tietema, A van Gestel, N van Straaten, O Wan, S Weber, U Janssens, IA AF Vicca, S. Bahn, M. Estiarte, M. van Loon, E. E. Vargas, R. Alberti, G. Ambus, P. Arain, M. A. Beier, C. Bentley, L. P. Borken, W. Buchmann, N. Collins, S. L. de Dato, G. Dukes, J. S. Escolar, C. Fay, P. Guidolotti, G. Hanson, P. J. Kahmen, A. Kroel-Dulay, G. Ladreiter-Knauss, T. Larsen, K. S. Lellei-Kovacs, E. Lebrija-Trejos, E. Maestre, F. T. Marhan, S. Marshall, M. Meir, P. Miao, Y. Muhr, J. Niklaus, P. A. Ogaya, R. Penuelas, J. Poll, C. Rustad, L. E. Savage, K. Schindlbacher, A. Schmidt, I. K. Smith, A. R. Sotta, E. D. Suseela, V. Tietema, A. van Gestel, N. van Straaten, O. Wan, S. Weber, U. Janssens, I. A. TI Can current moisture responses predict soil CO2 efflux under altered precipitation regimes? A synthesis of manipulation experiments SO BIOGEOSCIENCES LA English DT Article ID TEMPERATE FOREST SOIL; CLIMATE-CHANGE; CARBON-DIOXIDE; SUMMER DROUGHT; HETEROTROPHIC RESPIRATION; TERRESTRIAL ECOSYSTEMS; ROOT RESPIRATION; FLUXES; GRASSLAND; PRODUCTIVITY AB As a key component of the carbon cycle, soil CO2 efflux (SCE) is being increasingly studied to improve our mechanistic understanding of this important carbon flux. Predicting ecosystem responses to climate change often depends on extrapolation of current relationships between ecosystem processes and their climatic drivers to conditions not yet experienced by the ecosystem. This raises the question of to what extent these relationships remain unaltered beyond the current climatic window for which observations are available to constrain the relationships. Here, we evaluate whether current responses of SCE to fluctuations in soil temperature and soil water content can be used to predict SCE under altered rainfall patterns. Of the 58 experiments for which we gathered SCE data, 20 were discarded because either too few data were available or inconsistencies precluded their incorporation in the analyses. The 38 remaining experiments were used to test the hypothesis that a model parameterized with data from the control plots (using soil temperature and water content as predictor variables) could adequately predict SCE measured in the manipulated treatment. Only for 7 of these 38 experiments was this hypothesis rejected. Importantly, these were the experiments with the most reliable data sets, i.e., those providing high-frequency measurements of SCE. Regression tree analysis demonstrated that our hypothesis could be rejected only for experiments with measurement intervals of less than 11 days, and was not rejected for any of the 24 experiments with larger measurement intervals. This highlights the importance of high-frequency measurements when studying effects of altered precipitation on SCE, probably because infrequent measurement schemes have insufficient capacity to detect shifts in the climate dependencies of SCE. Hence, the most justified answer to the question of whether current moisture responses of SCE can be extrapolated to predict SCE under altered precipitation regimes is 'no' - as based on the most reliable data sets available. We strongly recommend that future experiments focus more strongly on establishing response functions across a broader range of precipitation regimes and soil moisture conditions. Such experiments should make accurate measurements of water availability, should conduct high-frequency SCE measurements, and should consider both instantaneous responses and the potential legacy effects of climate extremes. This is important, because with the novel approach presented here, we demonstrated that, at least for some ecosystems, current moisture responses could not be extrapolated to predict SCE under altered rainfall conditions. C1 [Vicca, S.; Janssens, I. A.] Univ Antwerp, Res Grp Plant & Vegetat Ecol, Dept Biol, B-2610 Antwerp, Belgium. [Bahn, M.; Ladreiter-Knauss, T.] Univ Innsbruck, Inst Ecol, A-6020 Innsbruck, Austria. [Estiarte, M.; Ogaya, R.; Penuelas, J.] CREAF CEAB UAB, Global Ecol Unit, CSIC, Cerdanyola Del Valles 08913, Catalonia, Spain. [Estiarte, M.; Ogaya, R.; Penuelas, J.] CREAF, Cerdanyola Del Valles 08193, Catalonia, Spain. [van Loon, E. E.; Tietema, A.] Univ Amsterdam, Inst Biodivers & Ecosyst Dynam, NL-1012 WX Amsterdam, Netherlands. [Vargas, R.] Univ Delaware, Dept Plant & Soil Sci, Delaware Environm Inst, Newark, DE 19717 USA. [Alberti, G.] Univ Udine, I-33100 Udine, Italy. [Alberti, G.] European Forest Inst, MOUNTFOR Project Ctr, San Michele All Adige, Trento, Italy. [Ambus, P.; Beier, C.; Larsen, K. S.] Tech Univ Denmark, Dept Chem & Biochem Engn, DK-2800 Lyngby, Denmark. [Arain, M. A.] McMaster Univ, McMaster Ctr Climate Change, Hamilton, ON, Canada. [Arain, M. A.] McMaster Univ, Sch Geog & Earth Sci, Hamilton, ON, Canada. [Beier, C.] NIVA Norwegian Inst Water Res, N-0349 Oslo, Norway. [Bentley, L. P.] Texas Tech Univ, Dept Biol Sci, Lubbock, TX 79409 USA. [Borken, W.] Univ Bayreuth, D-95448 Bayreuth, Germany. [Buchmann, N.] ETH, Dept Environm Syst Sci, Zurich, Switzerland. [Collins, S. L.] Univ New Mexico, Dept Biol, Albuquerque, NM 87131 USA. [de Dato, G.; Guidolotti, G.] Univ Tuscia, Dept Innovat Biol Agrofood & Forest Syst, Viterbo, Italy. [Dukes, J. S.; Suseela, V.] Purdue Univ, Dept Forestry & Nat Resources, W Lafayette, IN 47907 USA. [Dukes, J. S.] Univ Massachusetts, Dept Biol, Boston, MA 02125 USA. [Dukes, J. S.] Purdue Univ, Dept Biol Sci, W Lafayette, IN 47907 USA. [Escolar, C.; Maestre, F. T.] Univ Rey Juan Carlos, Area Biodiversidad & Conservac, Dept Biol & Geol, Escuela Super Ciencias Expt & Tecnol, Mostoles 28933, Spain. [Fay, P.] USDA ARS, Grassland Soil & Water Res Lab, Temple, TX 76502 USA. [Hanson, P. J.] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. [Kahmen, A.] ETH, Inst Agr Sci, CH-8092 Zurich, Switzerland. [Kroel-Dulay, G.; Lellei-Kovacs, E.; Lebrija-Trejos, E.] MTA Ctr Ecol Res, H-2163 Vacratot, Hungary. [Lebrija-Trejos, E.] Tel Aviv Univ, Dept Mol Biol & Ecol Plants, IL-69978 Tel Aviv, Israel. [Marhan, S.; Poll, C.] Univ Hohenheim, Inst Soil Sci & Land Evaluat, D-70599 Stuttgart, Germany. [Marshall, M.; Smith, A. R.] Environm Ctr Wales, Ctr Ecol & Hydrol, Bangor LL57 2UW, Gwynedd, Wales. [Meir, P.] Univ Edinburgh, Sch Geosci, Edinburgh, Midlothian, Scotland. [Meir, P.] Australian Natl Univ, Res Sch Biol, Canberra, ACT, Australia. [Miao, Y.; Wan, S.] Henan Univ, Coll Life Sci, State Key Lab Cotton Biol, Kaifeng 475004, Henan, Peoples R China. [Muhr, J.] Max Planck Inst Biogeochem, Dept Biogeochem Proc, D-07701 Jena, Germany. [Niklaus, P. A.] Univ Zurich, Inst Evolutionary Biol & Environm Studies, CH-8057 Zurich, Switzerland. [Savage, K.] USFS Northern Res Stn, Durham, NH 03824 USA. [Schindlbacher, A.] Woods Hole Res Ctr, Falmouth, MA 02540 USA. [Schmidt, I. K.] Nat Hazards & Landscape BFW, Fed Res & Training Ctr Forests, Dept Forest Ecol, A-1131 Vienna, Austria. [Smith, A. R.] Univ Copenhagen, Dept Geosci & Nat Resource Management, DK-1168 Copenhagen, Denmark. [Sotta, E. D.] Bangor Univ, Sch Environm Nat Resources & Geog, Bangor LL57 2UW, Gwynedd, Wales. [Suseela, V.] Embrapa Amapa, BR-68906970 Macapa, AP, Brazil. [van Gestel, N.] Clemson Univ, Sch Agr Forest & Environm Sci, Clemson, SC 29634 USA. [van Straaten, O.] Texas Tech Univ, Dept Biol Sci, Lubbock, TX 79409 USA. [Weber, U.] Univ Gottingen, Buesgen Inst, D-37077 Gottingen, Germany. Max Planck Inst Biogeochem, Dept Biogeochem Integrat BGI, D-07745 Jena, Germany. RP Vicca, S (reprint author), Univ Antwerp, Res Grp Plant & Vegetat Ecol, Dept Biol, Univ Pl 1, B-2610 Antwerp, Belgium. EM sara.vicca@uantwerpen.be RI de Dato, Giovanbattista/F-9693-2014; Bahn, Michael/I-3536-2013; Wan, Shiqiang/B-5799-2009; Beier, Claus/C-1789-2016; Ambus, Per/B-2514-2015; Marshall, Miles/G-5410-2011; Maestre, Fernando/A-6825-2008; Young, Kristina/M-3069-2014; Smith, Andy/A-7512-2011; Larsen, Klaus/C-7549-2015; Schmidt, Inger /A-6230-2015; Hanson, Paul J./D-8069-2011; Buchmann, Nina/E-6095-2011; Penuelas, Josep/D-9704-2011; Estiarte, Marc/G-2001-2016; Dukes, Jeffrey/C-9765-2009; Vicca, Sara/I-3637-2012; Collins, Scott/P-7742-2014; Vargas, Rodrigo/C-4720-2008; Meir, Patrick/J-8344-2012; Niklaus, Pascal/G-5786-2010; Janssens, Ivan/P-1331-2014; OI de Dato, Giovanbattista/0000-0003-0289-1727; Bahn, Michael/0000-0001-7482-9776; Beier, Claus/0000-0003-0348-7179; Ambus, Per/0000-0001-7580-524X; Maestre, Fernando/0000-0002-7434-4856; Smith, Andy/0000-0001-8580-278X; Larsen, Klaus/0000-0002-1421-6182; Schmidt, Inger /0000-0003-3880-2060; Hanson, Paul J./0000-0001-7293-3561; Penuelas, Josep/0000-0002-7215-0150; Estiarte, Marc/0000-0003-1176-8480; Dukes, Jeffrey/0000-0001-9482-7743; Vicca, Sara/0000-0001-9812-5837; Collins, Scott/0000-0002-0193-2892; Vargas, Rodrigo/0000-0001-6829-5333; Niklaus, Pascal/0000-0002-2360-1357; Janssens, Ivan/0000-0002-5705-1787; Poll, Christian/0000-0002-9674-4447; Fay, Philip/0000-0002-8291-6316; Alberti, Giorgio/0000-0003-2422-3009 FU European Community [FP7-ENV-2008-1-226701]; ESF network CLIMMANI; EU [INCREASE FP7-INFRASTRUCTURE-2008-1, 227628]; studies at Stubai from Carbo-Extreme; Austrian Science Fund (FWF) project [P22214-B17]; ERA-Net Circle Mountain project CAMELEON; EU project Carbo-Extreme [226701]; BIOLOG project (BMBF); NCCR Climate; U.S. NSF; US Department of Energy's Office of Science (BER), through the Northeastern Regional Center of the National Institute for Climatic Change Research; NSF LTER; DoE NICCR; NSF; USDA; Konza LTER program; European Research Council under the European Community [242658]; British Ecological Society [231/1975]; NERC [NE/J011002/1]; ARC [FT110100457]; USGS Global Climate Change Small Watershed Project grant; National Park Service grant; United States Environmental Protection Agency (EPA) under the Greater Research Opportunities (GRO) graduate program; EU FW5 VULCAN project; Hungarian Government [NKFP-3B/0008/2002]; Spanish government [CGL2010-17172]; Spanish government grant Consolider Ingenio MONTES [CSD2008-00040]; Catalan government [SGR2009-458]; Villum Foundation FX This work emerged from the Carbo-Extreme project, funded by the European Community's Seventh Framework Programme under grant agreement (FP7-ENV-2008-1-226701). We also acknowledge support of the ESF network CLIMMANI and of the EU-funded INCREASE FP7-INFRASTRUCTURE-2008-1 (grant agreement no. 227628) project for data exchange. S. Vicca is a postdoctoral research associate of the Fund for Scientific Research - Flanders. M. Bahn and T. Ladreiter-Knauss acknowledge funding of the studies at Stubai from Carbo-Extreme, the Austrian Science Fund (FWF) project P22214-B17 and the ERA-Net Circle Mountain project CAMELEON. N. Buchmann acknowledges funding from the EU project Carbo-Extreme (grant agreement no. 226701) as well as from the BIOLOG project (BMBF) and NCCR Climate. J. S. Dukes acknowledges support for the Boston-Area Climate Experiment from the U.S. NSF and by the US Department of Energy's Office of Science (BER), through the Northeastern Regional Center of the National Institute for Climatic Change Research. Research at Sevilleta was supported by NSF LTER and DoE NICCR. P. Fay acknowledges funding from NSF, USDA and the Konza LTER program. USDA is an equal opportunity provider and employer. F. T. Maestre and C. Escolar were supported by the European Research Council under the European Community's Seventh Framework Programme (FP7/2007-2013/ERC grant agreement 242658) and by the British Ecological Society (studentship 231/1975), respectively. P. Meir was supported by NERC NE/J011002/1 and ARC FT110100457. Financial support for the Big Bend project came from a USGS Global Climate Change Small Watershed Project grant to John Zak and a National Park Service grant to John Zak and David Tissue. L. P. Bentley was funded by the United States Environmental Protection Agency (EPA) under the Greater Research Opportunities (GRO) graduate program. E. Lellei-Kovacs acknowledges support provided through the research grant of the EU FW5 VULCAN project and the NKFP-3B/0008/2002 grant from the Hungarian Government. The research of M. Estiarte and J. Penuelas was supported by the Spanish government grants CGL2010-17172 and Consolider Ingenio MONTES (CSD2008-00040), and by the Catalan government grant SGR2009-458. The Brandbjerg experiment (Climaite) was funded by the Villum Foundation. I thank Lola and Mauro for making my life more colorful. Lastly, we wish to thank the editor and three anonymous reviewers for their positive assessment of our work and the insightful suggestions that improved this paper. NR 85 TC 18 Z9 19 U1 12 U2 126 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1726-4170 EI 1726-4189 J9 BIOGEOSCIENCES JI Biogeosciences PY 2014 VL 11 IS 11 BP 2991 EP 3013 DI 10.5194/bg-11-2991-2014 PG 23 WC Ecology; Geosciences, Multidisciplinary SC Environmental Sciences & Ecology; Geology GA AJ8JZ UT WOS:000337950900007 ER PT J AU McDermott, JE Huang, YF Zhang, B Xu, H Zhao, ZM AF McDermott, Jason E. Huang, Yufei Zhang, Bing Xu, Hua Zhao, Zhongming TI Integrative Genomics and Computational Systems Medicine SO BIOMED RESEARCH INTERNATIONAL LA English DT Editorial Material C1 [McDermott, Jason E.] Pacific NW Natl Lab, Computat Biol & Bioinformat Grp, Richland, WA 99352 USA. [Huang, Yufei] Univ Texas San Antonio, Dept Elect & Comp Engn, San Antonio, TX 78249 USA. [Zhang, Bing; Zhao, Zhongming] Vanderbilt Univ, Sch Med, Dept Biomed Informat, Nashville, TN 37203 USA. [Zhang, Bing; Zhao, Zhongming] Vanderbilt Univ, Med Ctr, Ctr Quantitat Sci, Nashville, TN 37232 USA. [Zhang, Bing; Zhao, Zhongming] Vanderbilt Univ, Med Ctr, Dept Canc Biol, Nashville, TN 37232 USA. [Xu, Hua] Univ Texas Hlth Sci Ctr Houston, Sch Biomed Informat, Houston, TX 77030 USA. RP Zhao, ZM (reprint author), Vanderbilt Univ, Sch Med, Dept Biomed Informat, Nashville, TN 37203 USA. EM zhongming.zhao@vanderbilt.edu NR 0 TC 0 Z9 0 U1 0 U2 0 PU HINDAWI PUBLISHING CORPORATION PI NEW YORK PA 410 PARK AVENUE, 15TH FLOOR, #287 PMB, NEW YORK, NY 10022 USA SN 2314-6133 EI 2314-6141 J9 BIOMED RES INT JI Biomed Res. Int. PY 2014 AR 945253 DI 10.1155/2014/945253 PG 3 WC Biotechnology & Applied Microbiology; Medicine, Research & Experimental SC Biotechnology & Applied Microbiology; Research & Experimental Medicine GA AK0JZ UT WOS:000338100100001 ER PT J AU Lapresta-Fernandez, A Salinas-Castillo, A de la Llana, SA Costa-Fernandez, JM Dominguez-Meister, S Cecchini, R Capitan-Vallvey, LF Moreno-Bondi, MC Marco, MP Sanchez-Lopez, JC Anderson, IS AF Lapresta-Fernandez, A. Salinas-Castillo, A. de la Llana, S. Anderson Costa-Fernandez, J. M. Dominguez-Meister, S. Cecchini, R. Capitan-Vallvey, L. F. Moreno-Bondi, M. C. Marco, M. -Pilar Sanchez-Lopez, J. C. Anderson, I. S. TI A General Perspective of the Characterization and Quantification of Nanoparticles: Imaging, Spectroscopic, and Separation Techniques SO CRITICAL REVIEWS IN SOLID STATE AND MATERIALS SCIENCES LA English DT Review DE nanoparticles; characterization techniques; imaging; spectroscopic; separation ID FIELD-FLOW FRACTIONATION; TRANSMISSION ELECTRON-MICROSCOPY; ATOMIC-FORCE MICROSCOPY; SIZE-EXCLUSION CHROMATOGRAPHY; ENHANCED RAMAN-SCATTERING; NATURAL AQUATIC COLLOIDS; X-RAY MICROSCOPY; BREAKDOWN-DETECTION LIBD; HIGHLY SENSITIVE QUANTIFICATION; TOF MASS-SPECTROMETRY AB This article gives an overview of the different techniques used to identify, characterize, and quantify engineered nanoparticles (ENPs). The state-of-the-art of the field is summarized, and the different characterization techniques have been grouped according to the information they can provide. In addition, some selected applications are highlighted for each technique. The classification of the techniques has been carried out according to the main physical and chemical properties of the nanoparticles such as morphology, size, polydispersity characteristics, structural information, and elemental composition. Microscopy techniques including optical, electron and X-ray microscopy, and separation techniques with and without hyphenated detection systems are discussed. For each of these groups, a brief description of the techniques, specific features, and concepts, as well as several examples, are described. C1 [Lapresta-Fernandez, A.; Salinas-Castillo, A.; Capitan-Vallvey, L. F.] Univ Granada, Dept Analyt Chem, ECsens, E-18071 Granada, Spain. [de la Llana, S. Anderson] Hop Cantonal Univ Geneva, Serv Neonatol & Soins Intensifs Pediat, Dept Enfant & Adolescent, CH-1205 Geneva, Switzerland. [Costa-Fernandez, J. M.] Univ Oviedo, Fac Chem, Dept Phys & Analyt Chem, E-33006 Oviedo, Spain. [Dominguez-Meister, S.; Sanchez-Lopez, J. C.] Univ Seville, CSIC, Inst Ciencia Mat Sevilla, Seville 41092, Spain. [Cecchini, R.] CNR, Ist Lo, Studio Mat Nanostrutturati, I-40129 Bologna, Italy. [Moreno-Bondi, M. C.] Univ Complutense, Dept Analyt Chem, Optochem Sensors & Appl Photochem Grp GSOLFA, E-28040 Madrid, Spain. [Marco, M. -Pilar] CSIC, IQAC, Nanobiotechnol Diagnost Grp AMRg, CIBER Bioingn Biomat & Nanomed CIBER BBN, ES-08034 Barcelona, Spain. [Anderson, I. S.] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. RP Lapresta-Fernandez, A (reprint author), Univ Granada, Dept Analyt Chem, ECsens, Campus Fuentenueva, E-18071 Granada, Spain. EM lapresta@ugr.es RI Sanchez-Lopez, Juan Carlos/K-3424-2014; Moreno-Bondi, Maria/H-3138-2011; MARCO, M-Pilar/A-9836-2015; Salinas-Castillo, Alfonso/N-1335-2015; Lapresta-Fernandez, Alejandro/K-9138-2016; Cecchini, Raimondo/J-7059-2012 OI Sanchez-Lopez, Juan Carlos/0000-0002-3490-6455; Moreno-Bondi, Maria/0000-0002-3612-0675; MARCO, M-Pilar/0000-0002-4064-1668; Salinas-Castillo, Alfonso/0000-0002-1360-6699; Lapresta-Fernandez, Alejandro/0000-0002-0641-9887; Cecchini, Raimondo/0000-0003-3650-2478 FU Junta de Andalucia, (Spain) [P10-FQM-5974]; CEI-Biotic Granada start-up Micro-projects for young researchers [CEI2013-MP-10] FX The work was funded in part by the Junta de Andalucia, (Spain) (Proyecto de Excelencia P10-FQM-5974) and CEI-Biotic Granada start-up Micro-projects for young researchers (CEI2013-MP-10). NR 278 TC 20 Z9 20 U1 6 U2 90 PU TAYLOR & FRANCIS INC PI PHILADELPHIA PA 530 CHESTNUT STREET, STE 850, PHILADELPHIA, PA 19106 USA SN 1040-8436 EI 1547-6561 J9 CRIT REV SOLID STATE JI Crit. Rev. Solid State Mat. Sci. PY 2014 VL 39 IS 6 BP 423 EP 458 DI 10.1080/10408436.2014.899890 PG 36 WC Materials Science, Multidisciplinary; Physics, Condensed Matter SC Materials Science; Physics GA AJ7VP UT WOS:000337908400002 ER PT J AU Fowler, DA Pfeiffer, CR Teat, SJ Beavers, CM Baker, GA Atwood, JL AF Fowler, Drew A. Pfeiffer, Constance R. Teat, Simon J. Beavers, Christine M. Baker, Gary A. Atwood, Jerry L. TI Illuminating host-guest cocrystallization between pyrogallol[4]arenes and the ionic liquid 1-ethyl-3-methylimidazolium ethylsulfate SO CRYSTENGCOMM LA English DT Article ID MOLECULAR CAPSULES; C-METHYL; NANOCAPSULES; IMIDAZOLIUM; CRYSTALLIZATION; COMPLEXATION; ORGANIZATION; CATIONS; SALTS AB The host-guest complexes of seven unique cocrystals containing pyrogallol[4]arenes and the ionic liquid 1-ethyl-3-methylimidazolium ethylsulfate are fully described. The investigation of these cocrystals is directed at expanding the control of the solid-state structures of these unique host-guest assemblies. The effects of varying conditions such as solvent choice and aliphatic tail length appended on the host macrocycle are explored and shed new light on the resultant supramolecular structures. C1 [Fowler, Drew A.; Pfeiffer, Constance R.; Baker, Gary A.; Atwood, Jerry L.] Univ Missouri, Columbia, MO 65211 USA. [Teat, Simon J.; Beavers, Christine M.] Adv Light Source, Berkeley, CA USA. RP Fowler, DA (reprint author), Univ Missouri, 601 South Coll, Columbia, MO 65211 USA. EM sjteat@lbl.gov; bakergar@missouri.edu; AtwoodJ@misssouri.edu RI Beavers, Christine/C-3539-2009; Baker, Gary/H-9444-2016 OI Beavers, Christine/0000-0001-8653-5513; Baker, Gary/0000-0002-3052-7730 FU ACS PRF grant [51865-DNI10]; Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231] FX Financial support from an ACS PRF grant (51865-DNI10) to GAB is acknowledged. JLA thanks NSF. 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 36 TC 9 Z9 9 U1 2 U2 5 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 2014 VL 16 IS 27 BP 6010 EP 6022 DI 10.1039/c4ce00359d PG 13 WC Chemistry, Multidisciplinary; Crystallography SC Chemistry; Crystallography GA AJ9MV UT WOS:000338036400008 ER PT J AU Quy, VC Carnevale, V Manganaro, L Lusic, M Rossetti, G Leone, V Fenollar-Ferrer, C Raugei, S Del Sal, G Giacca, M Carloni, P AF Vo Cam Quy Carnevale, Vincenzo Manganaro, Lara Lusic, Marina Rossetti, Giulia Leone, Vanessa Fenollar-Ferrer, Cristina Raugei, Simone Del Sal, Giannino Giacca, Mauro Carloni, Paolo TI HIV-1 Integrase Binding to its Cellular Partners: A Perspective from Computational Biology SO CURRENT PHARMACEUTICAL DESIGN LA English DT Article DE HIV-1 integrase; human Pin1; protein - protein interaction; class II mutant ID IMMUNODEFICIENCY-VIRUS TYPE-1; MULTIPLE SEQUENCE ALIGNMENT; REFINED SOLUTION STRUCTURE; CARBOXYL-TERMINAL DOMAIN; CATALYTIC CORE DOMAIN; DNA-BINDING; RETROVIRAL INTEGRASE; PROTEIN STRUCTURES; ISOMERASE PIN1; REGULATORY MECHANISM AB Viral DNA integration into the infected cell genome is an essential step in the HIV-1 life cycle. Hence, the viral integrase enzyme has become an important target for antiviral therapy. The integrase's activity action relies on the binding to its cellular partners, therefore the knowledge of the structural determinants is very important from a therapeutic perspective. Here we first review published computer-aided structural predictions of HIV-1 integrase in complex with its interactors. These include DNA and the human HAT protein. Next, we present a prediction of the complex between HIV-1 integrase with the human prolyl-isomerase-1 (hPin1) enzyme. Interaction with hPin1 is crucial for efficient HIV-1 infection and it increases integrase stability (Manganaro et. al 2010, Nat. Med. 16, 329). The modeling presented here, which is validated against experimental data, provides a rationale for a variety of viral protein's mutations which impair protein function and HIV-1 virus replication in vivo without significantly affecting enzymatic activity. C1 [Vo Cam Quy; Rossetti, Giulia; Carloni, Paolo] Forschungszentrum Julich, German Res Sch Simulat Sci, Inst Adv Simulat IAS 5, D-52425 Julich, Germany. [Carnevale, Vincenzo] Temple Univ, Inst Computat Mol Sci, Philadelphia, PA 19122 USA. [Manganaro, Lara; Lusic, Marina; Giacca, Mauro] Int Ctr Genet Engn & Biotechnol, I-34149 Trieste, Italy. [Leone, Vanessa; Fenollar-Ferrer, Cristina; Raugei, Simone] Scuola Int Super Studi Avanzati, I-34136 Trieste, Italy. [Leone, Vanessa] Max Planck Inst Biophys, Theoret Mol Biophys Grp, D-60438 Frankfurt, Germany. [Fenollar-Ferrer, Cristina] Max Planck Inst Biophys, Computat Struct Biol Grp, D-60438 Frankfurt, Germany. [Raugei, Simone] Pacific NW Natl Lab, Richland, WA 99352 USA. [Rossetti, Giulia] Inst Res Biomed, ES-08028 Barcelona, Spain. [Rossetti, Giulia] Barcelona Supercomp Ctr, Joint Res Program Computat Biol, ES-08028 Barcelona, Spain. [Rossetti, Giulia] Forschungszentrum Julich, Julich Supercomp Ctr, D-52425 Julich, Germany. [Del Sal, Giannino] Lab Nazl CIB, I-34012 Trieste, Italy. [Del Sal, Giannino] Univ Trieste, Dipartimento Sci Vita, I-34100 Trieste, Italy. RP Carloni, P (reprint author), Forschungszentrum Julich, German Res Sch Simulat Sci, Inst Adv Simulat IAS 5, D-52425 Julich, Germany. EM p.carloni@grs-sim.de RI Carnevale, Vincenzo/D-8015-2014; Giacca, Mauro/J-9287-2016; OI Carnevale, Vincenzo/0000-0002-1918-8280; Giacca, Mauro/0000-0003-2927-7225; DEL SAL, GIANNINO/0000-0003-2185-6003; Rossetti, Giulia/0000-0002-2032-4630 FU BANDO AIDS Grant from the Italian Government for "Targeting HIV transcription to control infection and to purge post-integrative latency" FX This work was supported by the BANDO AIDS Grant from the Italian Government for "Targeting HIV transcription to control infection and to purge post-integrative latency". NR 121 TC 0 Z9 0 U1 0 U2 6 PU BENTHAM SCIENCE PUBL LTD PI SHARJAH PA EXECUTIVE STE Y-2, PO BOX 7917, SAIF ZONE, 1200 BR SHARJAH, U ARAB EMIRATES SN 1381-6128 EI 1873-4286 J9 CURR PHARM DESIGN JI Curr. Pharm. Design PY 2014 VL 20 IS 21 BP 3412 EP 3421 PG 10 WC Pharmacology & Pharmacy SC Pharmacology & Pharmacy GA AJ7TE UT WOS:000337899300004 PM 24001231 ER PT J AU Choi, SH Kim, JS Lee, JY Jeon, JS Kim, JW Russo, RE Gonzalez, J Yoo, JH Kim, KS Yang, JS Park, KS AF Choi, Sung Hwa Kim, Jae Sung Lee, Ji Yeon Jeon, Ji Suk Kim, Ju Wan Russo, Richard E. Gonzalez, Jhanis Yoo, Jong Hyun Kim, Kyong Su Yang, Jung Seok Park, Kyung Su TI Analysis of arsenic in rice grains using ICP-MS and fs LA-ICP-MS SO JOURNAL OF ANALYTICAL ATOMIC SPECTROMETRY LA English DT Article ID LASER-ABLATION; FEMTOSECOND; WHITE; GLASS AB With rice being the main staple crop in Asian countries such as China, Korea and Japan, the detection of arsenic (As), an element known to be carcinogenic to humans, has been the topic of high public interest. In this study, the total arsenic content in 200 white and 104 brown rice samples collected in Korea was analyzed using a Quadrupole Inductively Coupled Plasma-Mass Spectrometer (ICP-MS). One of the rice grain samples was polished with 3, 5, 7, 9 and 11 degrees of milling and arsenic concentration variance from the surface to the inner core region was investigated. Furthermore, spatial distribution of arsenic over the cross-section of a brown rice grain was obtained using femtosecond Laser Ablation-Inductively Coupled Plasma-Mass Spectrometry (fs LA-ICP-MS). For the total arsenic content analysis, 91.7 +/- 28.1 and 101 +/- 33.6 mu g(-1) kg(-1) of arsenic were measured in the white and the brown rice, respectively. The fs LA-ICP-MS mapping image explains that the higher arsenic concentration in the brown rice is due to high arsenic distribution in the rice husk (protective covering of rice). Consequently, some degree of rice milling may be effective in the reduction of arsenic intake. C1 [Choi, Sung Hwa; Kim, Jae Sung; Lee, Ji Yeon; Jeon, Ji Suk; Park, Kyung Su] Korea Inst Sci & Technol, Adv Anal Ctr, Seoul 136791, South Korea. [Kim, Ju Wan] Joong Ang Univ, Dept Mech Engn, Seoul 156756, South Korea. [Russo, Richard E.; Gonzalez, Jhanis] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Yoo, Jong Hyun] Appl Spectra Inc, Fremont, CA 94538 USA. [Kim, Kyong Su] Chosun Univ, Dept Food & Nutr, Kwangju 501759, South Korea. [Yang, Jung Seok] Korea Inst Sci & Technol, Adv Anal Ctr, Kangnung 210340, South Korea. RP Park, KS (reprint author), Korea Inst Sci & Technol, Adv Anal Ctr, Seoul 136791, South Korea. EM pks6475@kist.re.kr FU Ministry of Food and Drug Safety [12162MFDS014] FX This research was supported by a grant (12162MFDS014) from the Ministry of Food and Drug Safety in 2012-2016. NR 24 TC 8 Z9 8 U1 10 U2 56 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 2014 VL 29 IS 7 BP 1233 EP 1237 DI 10.1039/c4ja00069b PG 5 WC Chemistry, Analytical; Spectroscopy SC Chemistry; Spectroscopy GA AJ6FR UT WOS:000337786400008 ER PT J AU Chirinos, JR Oropeza, DD Gonzalez, JJ Hou, HM Morey, M Zorba, V Russo, RE AF Chirinos, Jose R. Oropeza, Dayana D. Gonzalez, Jhanis J. Hou, Huaming Morey, Mark Zorba, Vassilia Russo, Richard E. TI Simultaneous 3-dimensional elemental imaging with LIBS and LA-ICP-MS SO JOURNAL OF ANALYTICAL ATOMIC SPECTROMETRY LA English DT Article ID PLASMA-MASS SPECTROMETRY; INDUCED BREAKDOWN SPECTROSCOPY; LASER-ABLATION; PEGMATITE AB Laser Induced Breakdown Spectroscopy (LIBS) and Laser Ablation Inductively Coupled Plasma-Mass Spectrometry (LA-ICP-MS) are used simultaneously for spatially resolved mapping of major and trace elements and isotopes within a Bastnasite rare earth ore sample. The combination of the two techniques provides complementary measurements for elements that are separately unattainable due to low sensitivity and/or strong interferences. Two dimensional (2D) layer-by-layer mapping, 2D cross-sectional imaging and three-dimensional (3D) volume rendering of elements and isotopes in the Bastnasite matrix are presented. These results pave the way for improved 3D elemental imaging through simultaneously acquired LIBS and LA-ICP-MS measurements. C1 [Chirinos, Jose R.; Oropeza, Dayana D.; Gonzalez, Jhanis J.; Hou, Huaming; Zorba, Vassilia; Russo, Richard E.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Gonzalez, Jhanis J.; Russo, Richard E.] Appl Spectra, Fremont, CA 94538 USA. [Morey, Mark] Special Technol Lab, Santa Barbara, CA 93111 USA. RP Russo, RE (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. EM rerusso@lbl.gov RI Zorba, Vassilia/C-4589-2015 FU Chemical Science Division, Office of Basic Energy Sciences of the U.S. Department of Energy at the Lawrence Berkeley National Laboratory [DE-AC02-05CH11231]; U.S. Department of Energy's National Nuclear Security Administration, Office of Defense Nuclear Nonproliferation Research and Development; Special Technologies Laboratory FX This work has been support by the Chemical Science Division, Office of Basic Energy Sciences of the U.S. Department of Energy under contract number DE-AC02-05CH11231 at the Lawrence Berkeley National Laboratory. The Special Technologies Laboratory thanks the U.S. Department of Energy's National Nuclear Security Administration, Office of Defense Nuclear Nonproliferation Research and Development, for financial support. Applied Spectra, Inc. acknowledges support from the Special Technologies Laboratory. NR 25 TC 21 Z9 21 U1 2 U2 59 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 2014 VL 29 IS 7 BP 1292 EP 1298 DI 10.1039/c4ja00066h PG 7 WC Chemistry, Analytical; Spectroscopy SC Chemistry; Spectroscopy GA AJ6FR UT WOS:000337786400016 ER PT J AU Graff, DL Love, SP AF Graff, David L. Love, Steven P. TI Toward real-time spectral imaging for chemical detection with a digital micromirror device-based programmable spectral filter SO JOURNAL OF MICRO-NANOLITHOGRAPHY MEMS AND MOEMS LA English DT Article DE hyperspectral imaging; Hadamard spectroscopy; spectral-matched filters; chemical detection; real-time spectral imaging; micromirror array; DLP; digital micromirror device ID SPECTROMETER AB Hyperspectral imaging sensors have proven to be powerful tools for highly selective and sensitive chemical detection applications, but they have significant operational drawbacks including slow line-scanning acquisition, large data volume of the resulting images, and a detection time lag due to the computational overhead of the matched-filter analysis. We have recently developed and demonstrated a high-speed, high-resolution, programmable spectral filter based on the Texas Instruments DLP digital micromirror device (DMD) that is capable of performing matched-filter image processing across a two-dimensional (2-D) field-of-view directly in the optical hardware and will enable real-time chemical detection without slow scanning, large data volumes or expensive postprocessing requirements. Based on traditional optical techniques, our spectral filter encodes the spectral information orthogonal to the spatial image information, enabling the DMD to encode matched-filter information into the spectral content of the scene without disturbing the underlying 2-D image. With this new technology, everything from simple multiband filters to very complicated hyperspectral matched filters can be implemented directly in the optical train of the sensor, producing an image highlighting a target signature within a spectrally cluttered scene in real time without further processing. We will first describe the implementation of a DMD as a multiplexing spectral selector for a 2-D field-of-view, discuss its utility as a multiband spectral filter, and show how the DLP's duty cycle-based grayscale capability enables the direct measurement of the adaptive matched filter. We will also show examples of multispectral and hyperspectral matched-filter images recorded with our visible spectrum prototype. (C) 2014 Society of Photo-Optical Instrumentation Engineers (SPIE) C1 [Graff, David L.; Love, Steven P.] Los Alamos Natl Lab, Space & Remote Sensing Grp, Los Alamos, NM 87544 USA. RP Graff, DL (reprint author), Los Alamos Natl Lab, Space & Remote Sensing Grp, Mail Stop B244, Los Alamos, NM 87544 USA. EM dlgraff@lanl.gov OI Love, Steven/0000-0003-0588-9622 FU Los Alamos National Laboratory [20110267ER] FX The authors gratefully acknowledge James Theiler and Bernard Foy of Los Alamos National Laboratory for their insight and shared expertise in both spectral image processing and multispectral filter design. This work was performed as part of an Exploratory Research project (20110267ER) under the Laboratory-Directed Research and Development (LDRD) program at Los Alamos National Laboratory. NR 16 TC 3 Z9 3 U1 0 U2 7 PU SPIE-SOC PHOTO-OPTICAL INSTRUMENTATION ENGINEERS PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98225 USA SN 1932-5150 EI 1932-5134 J9 J MICRO-NANOLITH MEM JI J. Micro-Nanolithogr. MEMS MOEMS PD JAN-MAR PY 2014 VL 13 IS 1 AR 011111 DI 10.1117/1.JMM.13.1.011111 PG 8 WC Engineering, Electrical & Electronic; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Optics SC Engineering; Science & Technology - Other Topics; Materials Science; Optics GA AK7TL UT WOS:000338630500020 ER PT J AU Love, SP Graff, DL AF Love, Steven P. Graff, David L. TI Full-frame programmable spectral filters based on micromirror arrays SO JOURNAL OF MICRO-NANOLITHOGRAPHY MEMS AND MOEMS LA English DT Article DE spectral imager; micromirror array; digital micromirror device; Hadamard; hyperspectral; matched filter; programmable spectral imager ID SPECTROMETER AB Rapidly programmable micromirror arrays, such as the Texas Instruments Digital Light Processor (DLP) digital micromirror device (DMD), have opened an exciting new arena in spectral imaging: rapidly reprogrammable, high spectral resolution, multiband spectral filters that perform spectral processing directly in the optical hardware. Such a device is created by placing a DMD at the spectral plane of an imaging spectrometer and by using it as a spectral selector that passes some wavelengths down the optical train to the final image and rejects others. Although simple in concept, realizing a truly practical DMD-based spectral filter has proved challenging. Versions described to date have been limited by the intertwining of image position and spectral propagation direction common to most imaging spectrometers, reducing these instruments to line-by-line scanning imagers rather than true spectral cameras that collect entire two-dimensional (2-D) images at once. Here, we report several optical innovations that overcome this limitation and allow us to construct full-frame programmable filters that spectrally manipulate every pixel, simultaneously and without spectral shifts, across a full 2-D image. So far, our prototype, which can be programmed either as a matched-filter imager for specific target materials or as a fully hyperspectral multiplexing Hadamard transform imager, has demonstrated over 100 programmable spectral bands while maintaining good spatial image quality. We discuss how diffraction-mediated trades between spatial and spectral resolution determine achievable performance. Finally, we describe methods for dealing with the DLP's 2-D diffractive effects and suggest a simple modification to the DLPs that would eliminate their impact for this application. (C) 2014 Society of Photo-Optical Instrumentation Engineers (SPIE) C1 [Love, Steven P.; Graff, David L.] Los Alamos Natl Lab, Space & Remote Sensing Grp ISR 2, Los Alamos, NM 87544 USA. RP Love, SP (reprint author), Los Alamos Natl Lab, Space & Remote Sensing Grp ISR 2, Mail Stop B244, Los Alamos, NM 87544 USA. EM splove@lanl.gov OI Love, Steven/0000-0003-0588-9622 FU Los Alamos National Laboratory [20110267ER] FX The authors gratefully acknowledge Tom Hale for his valuable assistance in constructing the early capillary-array/LCD prototype. This work was performed as part of an Exploratory Research project (20110267ER) under the Laboratory-Directed Research and Development (LDRD) program at Los Alamos National Laboratory. NR 18 TC 2 Z9 2 U1 0 U2 5 PU SPIE-SOC PHOTO-OPTICAL INSTRUMENTATION ENGINEERS PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98225 USA SN 1932-5150 EI 1932-5134 J9 J MICRO-NANOLITH MEM JI J. Micro-Nanolithogr. MEMS MOEMS PD JAN-MAR PY 2014 VL 13 IS 1 AR 011108 DI 10.1117/1.JMM.13.1.011108 PG 11 WC Engineering, Electrical & Electronic; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Optics SC Engineering; Science & Technology - Other Topics; Materials Science; Optics GA AK7TL UT WOS:000338630500017 ER PT J AU Bhattacharyya, S Mastai, Y Panda, RN Yeon, SH Hu, MZ AF Bhattacharyya, Sayan Mastai, Yitzhak Panda, Rabi Narayan Yeon, Sun-Hwa Hu, Michael Z. TI Advanced Nanoporous Materials: Synthesis, Properties, and Applications SO JOURNAL OF NANOMATERIALS LA English DT Editorial Material C1 [Bhattacharyya, Sayan] Indian Inst Sci Educ & Res IISER Kolkata, Dept Chem Sci, Mohanpur 741246, India. [Mastai, Yitzhak] Bar Ilan Univ, Dept Chem, IL-52900 Ramat Gan, Israel. [Mastai, Yitzhak] Bar Ilan Univ, Inst Nanotechnol, IL-52900 Ramat Gan, Israel. [Panda, Rabi Narayan] Birla Inst Technol & Sci Pilani, Dept Chem, Zuari Nagar 403726, Goa, India. [Yeon, Sun-Hwa] Korea Inst Energy Res, Distributed Power Generat & Energy Storage Grp, Taejon 305343, South Korea. [Hu, Michael Z.] Oak Ridge Natl Lab, Energy & Transportat Sci Div, Oak Ridge, TN 37831 USA. RP Bhattacharyya, S (reprint author), Indian Inst Sci Educ & Res IISER Kolkata, Dept Chem Sci, Mohanpur 741246, India. EM sayanb@iiserkol.ac.in OI Hu, Michael/0000-0001-8461-9684 NR 0 TC 0 Z9 0 U1 1 U2 8 PU HINDAWI PUBLISHING CORPORATION PI NEW YORK PA 410 PARK AVENUE, 15TH FLOOR, #287 PMB, NEW YORK, NY 10022 USA SN 1687-4110 EI 1687-4129 J9 J NANOMATER JI J. Nanomater. PY 2014 AR 275796 DI 10.1155/2014/275796 PG 2 WC Nanoscience & Nanotechnology; Materials Science, Multidisciplinary SC Science & Technology - Other Topics; Materials Science GA AJ9WY UT WOS:000338065200001 ER PT J AU Yang, SX Tongay, S Li, Y Yue, Q Xia, JB Li, SS Li, JB Wei, SH AF Yang, Shengxue Tongay, Sefaattin Li, Yan Yue, Qu Xia, Jian-Bai Li, Shun-Shen Li, Jingbo Wei, Su-Huai TI Layer-dependent electrical and optoelectronic responses of ReSe2 nanosheet transistors SO NANOSCALE LA English DT Article ID TRANSITION-METAL DICHALCOGENIDES; HYDROGEN EVOLUTION REACTION; FIELD-EFFECT TRANSISTORS; HEXAGONAL BORON-NITRIDE; BAND-EDGE TRANSITIONS; SINGLE-LAYER; MOS2; NANOSTRUCTURES; PHOTODETECTOR; DISELENIDE AB The ability to control the appropriate layer thickness of transition-metal dichalcogenides (TMDs) affords the opportunity to engineer many properties for a variety of applications in possible technological fields. Here we demonstrate that band-gap and mobility of ReSe2 nanosheet, a new member of the TMDs, increase when the layer number decreases, thus influencing the performances of ReSe2 transistors with different layers. A single-layer ReSe2 transistor shows much higher device mobility of 9.78 cm(2) V-1 s(-1) than few-layer transistors (0.10 cm(2) V-1 s(-1)). Moreover, a single-layer device shows high sensitivity to red light (633 nm) and has a light-improved mobility of 14.1 cm(2) V-1 s(-1). Molecular physisorption is used as "gating" to modulate the carrier density of our single-layer transistors, resulting in a high photoresponsivity (R-lambda) of 95 AW(-1) and external quantum efficiency (EQE) of 18 645% in O-2 environment. This work highlights the fact that the properties of ReSe2 can be tuned in terms of the number of layers and gasmolecule gating, and single-layer ReSe2 with appropriate band-gap is a promising material for future functional device applications. C1 [Yang, Shengxue; Tongay, Sefaattin; Li, Yan; Xia, Jian-Bai; Li, Shun-Shen; Li, Jingbo] Chinese Acad Sci, Inst Semicond, State Key Lab Superlattices & Microstruct, Beijing 100083, Peoples R China. [Tongay, Sefaattin] Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA. [Yue, Qu] Natl Univ Def Technol, Coll Sci, Changsha 410073, Hunan, Peoples R China. [Xia, Jian-Bai; Li, Shun-Shen; Li, Jingbo] Univ Sci & Technol China, Synerget Innovat Ctr Quantum Informat & Quantum P, Hefei 230026, Anhui, Peoples R China. [Wei, Su-Huai] Natl Renewable Energy Lab, Golden, CO 80401 USA. RP Li, JB (reprint author), Chinese Acad Sci, Inst Semicond, State Key Lab Superlattices & Microstruct, POB 912, Beijing 100083, Peoples R China. EM jbli@semi.ac.cn; swei@nrel.gov FU National Natural Science Foundation of China [91233120]; National Basic Research Program of China [2011CB921901]; US DOE through NREL [DE-AC36-08GO28308]; China Postdoctoral Science Foundation [2013M540127] FX This work is supported by the National Natural Science Foundation of China (91233120) and the National Basic Research Program of China (2011CB921901). S. H. Wei acknowledges financial support from US DOE through NREL (Grant no. DE-AC36-08GO28308). S. Yang acknowledges financial support from China Postdoctoral Science Foundation (no. 2013M540127). NR 39 TC 35 Z9 35 U1 9 U2 101 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 2014 VL 6 IS 13 BP 7226 EP 7231 DI 10.1039/c4nr01741b PG 6 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA AJ6FU UT WOS:000337786700013 PM 24882603 ER PT J AU Wang, HT Cui, XQ Guan, WM Zheng, XL Zhao, HT Wang, Z Wang, QY Xue, TY Liu, C Singh, DJ Zheng, WT AF Wang, Haitao Cui, Xiaoqiang Guan, Weiming Zheng, Xianliang Zhao, Hetong Wang, Zhao Wang, Qiyu Xue, Tianyu Liu, Chang Singh, David J. Zheng, Weitao TI Kinetic effects in the photomediated synthesis of silver nanodecahedra and nanoprisms: combined effect of wavelength and temperature SO NANOSCALE LA English DT Article ID PLASMON-MEDIATED SYNTHESIS; SHAPE-CONTROLLED SYNTHESIS; NOBLE-METAL NANOPARTICLES; OPTICAL-PROPERTIES; CHEMICAL-SYNTHESIS; GROWTH; NANOCRYSTALS; MORPHOLOGY; NANOSTRUCTURES; EXCITATION AB Photomediated synthesis is a reliable, high yield method for the production of a variety of morphologies of silver nanoparticles. Here, we report synthesis of silver nanoprisms and nanodecahedra with tunable sizes via control of the reaction temperature and the irradiation wavelength. The results show that shorter excitation wavelengths and lower reaction temperatures result in high yields of nanodecahedra, while longer excitation wavelengths and higher reaction temperatures result in the formation of nanoprisms. The mechanism for the growth condition dependent evolution in the morphology of the silver particles is discussed as a kinetically controlled process. This is based on analysis of the reaction kinetics at various excitation wavelengths and temperatures. The energy barrier for the transformation from seeds to nanodecahedra is relatively high and requires a shorter wavelength. Thus longer wavelength illumination leads to the formation of nanoprisms. Thermodynamically stable five-fold twinning structures are shown to evolve from twin plane structures. The fast reaction rate at higher temperature favors the growth of nanoprisms by preferential Ag deposition on planar structures in a kinetics-controlled mode, while slower rates yield thermodynamically favored nanodecahedra. C1 [Wang, Haitao; Cui, Xiaoqiang; Zheng, Xianliang; Zhao, Hetong; Wang, Zhao; Wang, Qiyu; Xue, Tianyu; Liu, Chang; Singh, David J.; Zheng, Weitao] Jilin Univ, MOE, Key Lab Automobile Mat, Changchun 130012, Peoples R China. [Wang, Haitao; Cui, Xiaoqiang; Zheng, Xianliang; Zhao, Hetong; Wang, Zhao; Wang, Qiyu; Xue, Tianyu; Liu, Chang; Singh, David J.; Zheng, Weitao] Jilin Univ, Dept Mat Sci, State Key Lab Superhard Mat, Changchun 130012, Peoples R China. [Guan, Weiming] State Key Lab Adv Technol Comprehens Utilizat Pla, Kunming 650106, Peoples R China. [Singh, David J.] Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN 37831 USA. RP Cui, XQ (reprint author), Jilin Univ, MOE, Key Lab Automobile Mat, Changchun 130012, Peoples R China. EM xqcui@jlu.edu.cn; wtzheng@jlu.edu.cn OI zheng, weitao/0000-0002-9028-278X FU National Natural Science Foundation of China [21275064, 21075051]; Program for New Century Excellent Talents in University [NCET-10-0433]; State Key Laboratory of Advanced Technologies for Comprehensive Utilization of Platinum Metals [SKL-SPM-201207]; Fundamental Research Funds for the Jilin University [200903020]; Jilin University, China; Department of Energy, Basic Energy Sciences, Materials Sciences and Technology Division FX This work was financially supported by the National Natural Science Foundation of China (no. 21275064, 21075051), the Program for New Century Excellent Talents in University (NCET-10-0433), the fund of the State Key Laboratory of Advanced Technologies for Comprehensive Utilization of Platinum Metals (SKL-SPM-201207), the Fundamental Research Funds for the Jilin University (Grant no. 200903020), and the "211" and "985" projects of Jilin University, China. Work at ORNL was supported by the Department of Energy, Basic Energy Sciences, Materials Sciences and Technology Division. NR 40 TC 7 Z9 7 U1 3 U2 61 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 2014 VL 6 IS 13 BP 7295 EP 7302 DI 10.1039/c4nr01442a PG 8 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA AJ6FU UT WOS:000337786700023 PM 24848449 ER PT J AU Na, H Jeong, JS Chang, HJ Kim, HY Woo, K Lim, K Mkhoyan, KA Jang, HS AF Na, Hyejin Jeong, Jong Seok Chang, Hye Jung Kim, Hyun You Woo, Kyoungja Lim, Kipil Mkhoyan, K. Andre Jang, Ho Seong TI Facile synthesis of intense green light emitting LiGdF4:Yb,Er-based upconversion bipyramidal nanocrystals and their polymer composites SO NANOSCALE LA English DT Article ID EARTH FLUORIDE NANOCRYSTALS; DOPED NAYF4 NANOCRYSTALS; CORE/SHELL NANOCRYSTALS; NAGDF4 NANOPARTICLES; CRYSTAL-STRUCTURE; IN-VIVO; LUMINESCENCE; EMISSION; NANOPHOSPHORS; PHOSPHORS AB A pathway for achieving intense green light emitting LiGdF4:Yb,Er upconversion nanophosphors (UCNPs) via Y3+ doping is demonstrated. It was revealed that Y3+ doping initiated the formation of a tetragonal phase and affected the particle size. Single tetragonal-phase LiGd0.4Y0.4F4:Yb(18%),Er(2%) (LGY(0.4)F:Yb,Er) UCNPs exhibited strong upconversion (UC) green luminescence and tetragonal bipyramidal morphologies. They showed 1325 and 325-fold higher photoluminescence intensity than the 0 and 80 mol% Y3+-doped LiGdF4:Yb,Er UCNPs, respectively. Additionally the particle size (edge length) of LiGdF4:Yb,Er-based upconversion tetragonal bipyramids (UCTBs) was controlled from 60.5 nm to an ultrasmall size of 9.3 nm with varying Y3+ doping concentration. In an LGY(0.4)F:Yb,Er UCTB, uniform distribution of all constituent elements was directly confirmed by using high-angle annular dark-field scanning transmission electron microscopy and energy-filtered transmission electron microscopy (EFTEM) image analyses. In particular, existence of activator Er3+ ions with extremely small quantity was clearly seen over a particle on the EFTEM image. Moreover, the LGY(0.4)F:Yb,Er UCTBs were successfully incorporated into the polydimethylsiloxane (PDMS) polymer and the highly transparent UCTB-PDMS composites showed bright green light under the excitation of 980 nm infrared light. C1 [Na, Hyejin; Woo, Kyoungja; Lim, Kipil; Jang, Ho Seong] Korea Inst Sci & Technol, Mol Recognit Res Ctr, Seoul 136791, South Korea. [Jeong, Jong Seok; Mkhoyan, K. Andre] Univ Minnesota, Dept Chem Engn & Mat Sci, Minneapolis, MN 55455 USA. [Chang, Hye Jung] Korea Inst Sci & Technol, Adv Anal Ctr, Seoul 136791, South Korea. [Kim, Hyun You] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. [Kim, Hyun You] Chungnam Natl Univ, Dept Nanomat Engn, Taejon 305764, South Korea. RP Jang, HS (reprint author), Korea Inst Sci & Technol, Ctr Mat Architecturing, Hwarangno 14 Gil 5, Seoul 136791, South Korea. EM msekorea@kist.re.kr RI Jeong, Jong Seok/G-5022-2010; Jang, Ho Seong/C-3941-2013; OI Jeong, Jong Seok/0000-0002-5570-748X; Jang, Ho Seong/0000-0002-2031-1303; Mkhoyan, Andre/0000-0003-3568-5452 FU Dream project [2V03410]; Flagship project - Korea Institute of Science and Technology (KIST) [2E24572]; Pioneer Research Center Program through the National Research Foundation of Korea; Ministry of Science, ICT & Future Planning [NRF-2013M3C1A3065040]; MRSEC Program of the National Science Foundation (NSF) [DMR-0819885]; U.S. Department of Energy, Office of Basic Energy Sciences [DE-AC02-98CH10886]; NSF through the MRSEC program FX This work was supported in part by the Dream project (2V03410) and Flagship project (2E24572) funded by the Korea Institute of Science and Technology (KIST), the Pioneer Research Center Program through the National Research Foundation of Korea funded by the Ministry of Science, ICT & Future Planning (NRF-2013M3C1A3065040), the MRSEC Program of the National Science Foundation (NSF) under Award number DMR-0819885, and the U.S. Department of Energy, Office of Basic Energy Sciences, under Contract DE-AC02-98CH10886 (H.Y.K.), and parts of this work were carried out in the Characterization Facility, University of Minnesota, which receives partial support from the NSF through the MRSEC program. We thank Seo Kyoung Ryu and Min Kyoung Cho for their technical help for EFTEM analysis (2V02951). NR 48 TC 12 Z9 12 U1 3 U2 53 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 2014 VL 6 IS 13 BP 7461 EP 7468 DI 10.1039/c4nr00857j PG 8 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA AJ6FU UT WOS:000337786700045 PM 24882742 ER PT J AU Yu, Q Mishra, RK Morris, JW Minor, AM AF Yu, Qian Mishra, Raja K. Morris, John W., Jr. Minor, Andrew M. TI The effect of size on dislocation cell formation and strain hardening in aluminium SO PHILOSOPHICAL MAGAZINE LA English DT Article DE aluminium; dislocation cell; dimensional restriction; strain hardening ID MECHANICAL-PROPERTIES; PLASTIC-DEFORMATION; SINGLE-CRYSTALS; ALLOYS; METALS; AL AB The formation of dislocation cells has a significant impact on the strain hardening behaviour of metals. Dislocation cells can form in metals with a characteristic size defined by three-dimensional tangles of dislocations that serve as "walls" and less dense internal regions. It has been proposed that inhibiting the formation of dislocation cells could improve the strain hardening behaviour of metals such as Al. Here we employ in situ scanning electron microscope compression testing of pure Al single crystal pillars with physical dimensions larger, close to and smaller than the reported cell size in Al, respectively, to investigate the possible size effect on the formation of dislocation cell and the consequent change of mechanical properties. We observed that the formation of dislocation cells is inhibited as the pillar size decreases to a critical value and simultaneously both the strength and the strain hardening behaviour become strongly enhanced. This phenomenon is discussed in terms of the effect of dimensional restriction on the formation of dislocation cells. The reported mechanism could be applied in polycrystalline Al where the tunable physical dimension could be grain size instead of sample size, providing insight into Al alloy design. C1 [Yu, Qian; Morris, John W., Jr.; Minor, Andrew M.] Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA. [Yu, Qian; Minor, Andrew M.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Natl Ctr Electron Microscopy, Berkeley, CA 94720 USA. [Mishra, Raja K.] Gen Motors Res & Dev Ctr, Warren, WI USA. RP Minor, AM (reprint author), Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA. EM aminor@berkeley.edu RI Foundry, Molecular/G-9968-2014 FU General Motors Research and Development Center; National Center for Electron Microscopy at Lawrence Berkeley National Laboratory by the US Department of Energy [DE-AC02-05CH11231] FX This research was supported by the General Motors Research and Development Center and the National Center for Electron Microscopy at Lawrence Berkeley National Laboratory, which is supported by the US Department of Energy under Contract # DE-AC02-05CH11231. NR 25 TC 8 Z9 8 U1 3 U2 25 PU TAYLOR & FRANCIS LTD PI ABINGDON PA 4 PARK SQUARE, MILTON PARK, ABINGDON OX14 4RN, OXON, ENGLAND SN 1478-6435 EI 1478-6443 J9 PHILOS MAG JI Philos. Mag. PY 2014 VL 94 IS 18 BP 2062 EP 2071 DI 10.1080/14786435.2014.906755 PN A PG 10 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering; Physics, Applied; Physics, Condensed Matter SC Materials Science; Metallurgy & Metallurgical Engineering; Physics GA AJ7VA UT WOS:000337905400007 ER PT J AU Costantini, JM Beuneu, F Weber, WJ AF Costantini, Jean-Marc Beuneu, Francois Weber, William J. TI Annealing of paramagnetic centres in electron-and ion-irradiated yttria-stabilized zirconia: effect of yttria content SO PHILOSOPHICAL MAGAZINE LA English DT Article DE yttria-stabilized zirconia; electron irradiation; ion irradiation; colour centres; electron paramagnetic resonance ID CHARGED-PARTICLE IRRADIATIONS; OPTICAL-PROPERTIES; DEFECTS; ZRO2; TRANSPORT; OXIDE AB We have studied the effect of yttria content on the recovery of paramagnetic centres in electron- and ion-irradiated yttria-stabilized zirconia (ZrO2: Y3+). Single crystals with 9.5 or 18 mol% Y2O3 were irradiated with 1.0-2.5 MeV electrons, 145-MeV carbon ions, 200-MeV iodine ions, 1.45-GeV xenon ions and 2.25-GeV gold ions at various fluences. Thermal annealing of electron (F+-type and T) centres and hole centres was studied by X-band electron paramagnetic resonance spectroscopy. Hole centres are found to anneal more quickly for 18 mol% than for 9.5 mol% Y2O3. At long annealing times, a non-zero asymptotic behaviour is observed in the isothermal annealing curves of hole centres and F+-type centres between 300 and 500 K. For the electron-irradiated samples, the asymptotic concentration of both defect types normalized by the values prior to annealing has a maximum value of similar to 0.5 for annealing temperatures below the onset of the (isochronal) recovery stage (400 K), regardless of the yttria content. For the ion-irradiated samples, larger normalized asymptotic values (similar to 0.8) at high annealing temperature are found for the F+-type centres with a similar recovery process. Such an uncommon behaviour is analysed on the basis of a model using equilibrated reactions between point defects with different charge states. C1 [Costantini, Jean-Marc] CEA, DEN, SRMA, F-91191 Gif Sur Yvette, France. [Beuneu, Francois] Ecole Polytech, CNRS, CEA, LSI, F-91128 Palaiseau, France. [Weber, William J.] Univ Tennessee, Dept Mat Sci & Engn, Knoxville, TN 37996 USA. [Weber, William J.] Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN 37831 USA. RP Costantini, JM (reprint author), CEA, DEN, SRMA, F-91191 Gif Sur Yvette, France. EM jean-marc.costantini@cea.fr RI Weber, William/A-4177-2008 OI Weber, William/0000-0002-9017-7365 FU US Department of Energy, Basic Energy Sciences, Materials Science and Engineering Division FX Authors are indebted to the late Prof A.M. Stoneham (University College London, UK) for fruitful discussions and advice. One of the authors (W.J. Weber) was supported by the US Department of Energy, Basic Energy Sciences, Materials Science and Engineering Division. C. Trautmann (Helmholtzzentrum fur Schwerionenforschung, Darmstadt, Germany) and M. Toulemonde (CIMAP, Caen, France) are warmly thanked for the irradiations at GSUUNILAC and GANIL. NR 26 TC 2 Z9 2 U1 1 U2 7 PU TAYLOR & FRANCIS LTD PI ABINGDON PA 4 PARK SQUARE, MILTON PARK, ABINGDON OX14 4RN, OXON, ENGLAND SN 1478-6435 EI 1478-6443 J9 PHILOS MAG JI Philos. Mag. PY 2014 VL 94 IS 20 BP 2281 EP 2296 DI 10.1080/14786435.2014.913107 PG 16 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering; Physics, Applied; Physics, Condensed Matter SC Materials Science; Metallurgy & Metallurgical Engineering; Physics GA AJ8SO UT WOS:000337978000004 ER PT J AU Jesche, A Canfield, PC AF Jesche, A. Canfield, P. C. TI Single crystal growth from light, volatile and reactive materials using lithium and calcium flux SO PHILOSOPHICAL MAGAZINE LA English DT Article DE crystal growth; solution growth; nitrides; X-ray diffraction; magnetic properties ID INTERMETALLIC COMPOUNDS; DICALCIUM NITRIDE; SYSTEM; TRANSITION; PHASE; Y2NI7; NI; FERROMAGNETISM; HYDRIDE; ALLOYS AB We present a method for the solution growth of single crystals from reactive Li and Ca melts and its application to the synthesis of several, representative compounds. Among these, single crystalline Li3N, Li-2(Li1-xTx) N with T = {Mn, Fe, Co}, LiCaN, Li2C2, LiRh and LiIr from Li-rich flux, as well as Ca2N, CaNi2, CaNi3, YbNi2, Y2Ni7 and LaNi5 from Ca-rich flux could be obtained. Special emphasize is given on the growth of nitrides using commercially available Li3N and Ca3N2 powders as the nitrogen source instead of N-2 gas. C1 [Jesche, A.; Canfield, P. C.] Iowa State Univ, Ames Lab, Ames, IA 50011 USA. [Canfield, P. C.] Iowa State Univ, Dept Phys & Astron, Ames, IA USA. RP Jesche, A (reprint author), Iowa State Univ, Ames Lab, Ames, IA 50011 USA. EM jesche@ameslab.gov FU US Department of Energy, Office of Basic Energy Science, Division of Materials Sciences and Engineering (BES-DMSE); US Department of Energy by Iowa State University [DE-AC02-07CH11358] FX S.L. Bud'ko, P. Hohn, R. S. Houk, J.L. Jacobs and A. Kreyssig are acknowledged for comments and discussions. The authors thank F. Laabs and W. E. Straszheim for assistance with energy dispersive X-ray analysis. This work was supported by the US Department of Energy, Office of Basic Energy Science, Division of Materials Sciences and Engineering (BES-DMSE). The research was performed at the Ames Laboratory. Ames Laboratory is operated for the US Department of Energy by Iowa State University under Contract No. DE-AC02-07CH11358. The authors would like to acknowledge supplemental support from BES-DMSE for the acquisition of a Inert Gas Atmosphere system that was instrumental in the synthesis and characterization of the materials prepared for this research. NR 45 TC 9 Z9 9 U1 4 U2 46 PU TAYLOR & FRANCIS LTD PI ABINGDON PA 4 PARK SQUARE, MILTON PARK, ABINGDON OX14 4RN, OXON, ENGLAND SN 1478-6435 EI 1478-6443 J9 PHILOS MAG JI Philos. Mag. PY 2014 VL 94 IS 21 BP 2372 EP 2402 DI 10.1080/14786435.2014.913114 PG 31 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering; Physics, Applied; Physics, Condensed Matter SC Materials Science; Metallurgy & Metallurgical Engineering; Physics GA AJ8SS UT WOS:000337978400002 ER PT J AU Scheer, AM Welz, O Zador, J Osborn, DL Taatjes, CA AF Scheer, Adam M. Welz, Oliver Zador, Judit Osborn, David L. Taatjes, Craig A. TI Low-temperature combustion chemistry of novel biofuels: resonance-stabilized QOOH in the oxidation of diethyl ketone SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID SET MODEL CHEMISTRY; GAS-PHASE REACTIONS; MOLECULAR-OXYGEN; CHLORINE ATOMS; KINETICS; ETHYL; 3-PENTANONE; MECHANISM; RADICALS; FUTURE AB The Cl-center dot initiated oxidation reactions of diethyl ketone (DEK; 3-pentanone; (CH3CH2)(2)C=O), 2,2,4,4-d4-diethyl ketone (d(4)-DEK; (CH3CD2)(2)C=O) and 1,1,1,5,5,5-d(6)-diethyl ketone (d(6)-DEK; (CD3CH2)(2)C=O) are studied at 8 Torr and 550-650 K using Cl-2 as a source for the pulsed-photolytic generation of Cl-center dot. Products are monitored as a function of reaction time, mass, and photoionization energy using multiplexed photoionization mass spectrometry with tunable synchrotron radiation. Adding a large excess of O-2 to the reacting flow allows determination of products resulting from oxidation of the initial primary (R-p) and secondary (R-s) radicals formed via the Cl-center dot + DEK reaction. Because of resonance stabilization, the secondary DEK radical (3-oxopentan-2-yl) reaction with O-2 has a shallow alkyl peroxy radical (RsO2) well and no energetically low-lying product channels. This leads to preferential back dissociation of RsO2 and a greater likelihood of consumption of R-s by competing radical-radical reactions. On the other hand, reaction of the primary DEK radical (3-oxopentan-1-yl) with O-2 has several accessible bimolecular product channels. Vinyl ethyl ketone is observed from HO2-elimination from the DEK alkylperoxy radicals, and small-molecule products are identified from beta-scission reactions and decomposition reactions of oxy radical secondary products. Although channels yielding OH + 3-, 4-, 5-and 6-membered ring cyclic ether products are possible in the oxidation of DEK, at the conditions of this study (8 Torr, 550-650 K) only the 5-membered ring, 2-methyltetrahydrofuran-3-one, is observed in significant quantities. Computation of relevant stationary points on the potential energy surfaces for the reactions of R-p and R-s with O-2 indicates this cyclic ether is formed via a resonance-stabilized hydroperoxyalkyl radical (QOOH) intermediate, formed from isomerization of the RpO2 radical. C1 [Scheer, Adam M.; Welz, Oliver; Zador, Judit; Osborn, David L.; Taatjes, Craig A.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. RP Taatjes, CA (reprint author), Sandia Natl Labs, Combust Res Facil, MS 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 Laboratory Directed Research and Development program at Sandia National Laboratories; multiprogram laboratory; Lockheed Martin Company, for the United States Department of Energy (USDOE)'s National Nuclear Security Administration [DEAC04-94AL85000]; Division of Chemical Sciences, Geosciences, and Biosciences, the Office of Basic Energy Sciences (BES), USDOE; Office of Science, BES/USDOE [DE-AC020-5CH11231] FX We thank Dr John D. Savee and Dr Brandon Rotavera for useful discussions and Mr Howard Johnsen for technical support of these experiments. This work is supported by the Laboratory Directed Research and Development program at Sandia National Laboratories, a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the United States Department of Energy (USDOE)'s National Nuclear Security Administration under contract DEAC04-94AL85000. The development of the experimental apparatus and the participation of JZ, OW, & DLO were supported by the Division of Chemical Sciences, Geosciences, and Biosciences, the Office of Basic Energy Sciences (BES), USDOE. The Advanced Light Source is supported by the Director, Office of Science, BES/USDOE, under contract DE-AC020-5CH11231 between Lawrence Berkeley National Laboratory and the USDOE. NR 36 TC 7 Z9 7 U1 3 U2 62 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 2014 VL 16 IS 26 BP 13027 EP 13040 DI 10.1039/c3cp55468f PG 14 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AJ6FJ UT WOS:000337785400002 PM 24585023 ER PT J AU Wang, WJ Kuzmenko, I Vaknin, D AF Wang, Wenjie Kuzmenko, Ivan Vaknin, David TI Iron near absorption edge X-ray spectroscopy at aqueous-membrane interfaces SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID REFLECTIVITY; FLUORESCENCE; MONOLAYER; FE3+ AB Employing synchrotron X-ray scattering, we systematically determine the absorption near-edge spectra (XANES) of iron in its ferrous (Fe2+) and ferric (Fe3+) states both as ions in aqueous solutions and as they bind to form a single layer to anionic templates that consist of carboxyl or phosphate groups at aqueous/vapor interfaces. While the XANES of bulk iron ions show that the electronic state and coordination of iron complexes in the bulk are isotropic, the interfacial bound ions show a signature of a broken inversion-symmetry environment. The XANES of Fe2+ and Fe3+ in the bulk possess distinct profiles however, upon binding they practically exhibit similar patterns. This indicates that both bound ions settle into a stable electronic and coordination configuration with an effective fractional valence (for example, Fe[2+nu]+, 0 < nu < 1) at charged organic templates. Such two dimensional properties may render interfacial iron, abundant in living organisms, a more efficient and versatile catalytic behavior. C1 [Wang, Wenjie; Vaknin, David] Iowa State Univ, Ames Lab, Ames, IA 50011 USA. [Wang, Wenjie; Vaknin, David] Iowa State Univ, Dept Phys & Astron, Ames, IA 50011 USA. [Kuzmenko, Ivan] Argonne Natl Lab, Adv Photon Source, Xray Sci Div, Argonne, IL 60439 USA. RP Vaknin, D (reprint author), Iowa State Univ, Ames Lab, Ames, IA 50011 USA. EM vaknin@ameslab.gov RI Vaknin, David/B-3302-2009 OI Vaknin, David/0000-0002-0899-9248 FU Office of Basic Energy Sciences, U.S. Department of Energy [DE-AC02-07CH11358]; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357] FX We thank R.Y. Park (Ames Laboratory, Iowa State University) for technical support at APS. The work at the Ames Laboratory was supported by the Office of Basic Energy Sciences, U.S. Department of Energy under Contract No. DE-AC02-07CH11358. 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. NR 35 TC 1 Z9 1 U1 0 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 2014 VL 16 IS 26 BP 13517 EP 13522 DI 10.1039/c4cp00657g PG 6 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AJ6FJ UT WOS:000337785400058 PM 24890972 ER PT J AU Hu, B Liao, HX Alam, SM Goldstein, B AF Hu, Bin Liao, Hua-Xin Alam, S. Munir Goldstein, Byron TI Estimating the Probability of Polyreactive Antibodies 4E10 and 2F5 Disabling a gp41 Trimer after T Cell-HIV Adhesion SO PLOS COMPUTATIONAL BIOLOGY LA English DT Article ID IMMUNODEFICIENCY-VIRUS TYPE-1; BROADLY NEUTRALIZING ANTIBODIES; PROXIMAL EXTERNAL REGION; COMPLEMENTARITY-DETERMINING REGION; HEAVY-CHAIN; MEMBRANE; ENTRY; EPITOPE; INHIBITION; MECHANISMS AB A few broadly neutralizing antibodies, isolated from HIV-1 infected individuals, recognize epitopes in the membrane proximal external region (MPER) of gp41 that are transiently exposed during viral entry. The best characterized, 4E10 and 2F5, are polyreactive, binding to the viral membrane and their epitopes in the MPER. We present a model to calculate, for any antibody concentration, the probability that during the pre-hairpin intermediate, the transient period when the epitopes are first exposed, a bound antibody will disable a trivalent gp41 before fusion is complete. When 4E10 or 2F5 bind to the MPER, a conformational change is induced that results in a stably bound complex. The model predicts that for these antibodies to be effective at neutralization, the time to disable an epitope must be shorter than the time the antibody remains bound in this conformation, about five minutes or less for 4E10 and 2F5. We investigate the role of avidity in neutralization and show that 2F5 IgG, but not 4E10, is much more effective at neutralization than its Fab fragment. We attribute this to 2F5 interacting more stably than 4E10 with the viral membrane. We use the model to elucidate the parameters that determine the ability of these antibodies to disable epitopes and propose an extension of the model to analyze neutralization data. The extended model predicts the dependencies of IC50 for neutralization on the rate constants that characterize antibody binding, the rate of fusion of gp41, and the number of gp41 bridging the virus and target cell at the start of the pre-hairpin intermediate. Analysis of neutralization experiments indicate that only a small number of gp41 bridges must be disabled to prevent fusion. However, the model cannot determine the exact number from neutralization experiments alone. C1 [Hu, Bin; Goldstein, Byron] Los Alamos Natl Lab, Div Theoret, Theoret Biol & Biophys Grp, Los Alamos, NM 87545 USA. [Liao, Hua-Xin; Alam, S. Munir] Duke Univ, Med Ctr, Human Vaccine Inst, Durham, NC USA. RP Hu, B (reprint author), Los Alamos Natl Lab, Div Theoret, Theoret Biol & Biophys Grp, Los Alamos, NM 87545 USA. EM bxg@lanl.gov FU National Institute of General Medical Sciences of the National Institutes of Health [R37-GM035556]; Department of Energy [DEAC52-06NA25396] FX The research reported in this publication was supported by the National Institute of General Medical Sciences of the National Institutes of Health under award number R37-GM035556 and by the Department of Energy contract DEAC52-06NA25396. The content is solely the responsibility of the authors and does not necessarily represent the official views of the National Institutes of Health. The funders had no role in study design, data collection and analysis, decision to publish, or preparation of the manuscript. NR 46 TC 3 Z9 3 U1 0 U2 2 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 2014 VL 10 IS 1 AR e1003431 DI 10.1371/journal.pcbi.1003431 PG 11 WC Biochemical Research Methods; Mathematical & Computational Biology SC Biochemistry & Molecular Biology; Mathematical & Computational Biology GA AJ8JE UT WOS:000337948500031 PM 24499928 ER PT J AU Harmon, JE AF Harmon, Joseph E. TI Rhetorical Style: The Uses of Language in Persuasion SO RHETORIC SOCIETY QUARTERLY LA English DT Book Review C1 [Harmon, Joseph E.] Argonne Natl Lab, Argonne, IL 60439 USA. RP Harmon, JE (reprint author), Argonne Natl Lab, Argonne, IL 60439 USA. NR 1 TC 0 Z9 0 U1 1 U2 1 PU ROUTLEDGE JOURNALS, TAYLOR & FRANCIS LTD PI ABINGDON PA 4 PARK SQUARE, MILTON PARK, ABINGDON OX14 4RN, OXFORDSHIRE, ENGLAND SN 0277-3945 EI 1930-322X J9 RHETOR SOC Q JI Rhetor. Soc. Q. PY 2014 VL 44 IS 3 SI SI BP 293 EP 296 PG 4 WC Communication; Literature; Philosophy SC Communication; Literature; Philosophy GA AJ8GR UT WOS:000337941600010 ER PT J AU Heinson, WR Pierce, F Sorensen, CM Chakrabarti, A AF Heinson, W. R. Pierce, F. Sorensen, C. M. Chakrabarti, A. TI Crossover from Ballistic to Epstein Diffusion in the Free-Molecular Regime SO AEROSOL SCIENCE AND TECHNOLOGY LA English DT Article ID TRANSITION REGIME; FRACTAL DIMENSION; AEROSOL; FLAMES; AGGLOMERATION; MOBILITY AB We investigate, through simulation, a system of aggregating particles in the free molecular regime that undergoes a crossover from ballistic to diffusive motion. As the aggregates grow, the aggregate mean free path becomes smaller and the motion between collisions becomes more diffusive. From growth kinetics, we find that when the ratio of the aggregate mean path to the mean aggregate nearest neighbor separation reaches of the order of unity, a crossover to diffusive motion occurs. This ratio, called the nearest neighbor Knudsen number, becomes an important parameter in understanding aerosol aggregation in the free molecular regime. C1 [Heinson, W. R.; Sorensen, C. M.; Chakrabarti, A.] Kansas State Univ, Dept Phys, Manhattan, KS 66506 USA. [Pierce, F.] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Chakrabarti, A (reprint author), Kansas State Univ, Dept Phys, Cardwell Hall, Manhattan, KS 66506 USA. EM amitc@phys.ksu.edu FU National Science Foundation [AGS 1261651] FX This material is based upon work supported by the National Science Foundation under grant no. AGS 1261651. NR 25 TC 2 Z9 2 U1 0 U2 8 PU TAYLOR & FRANCIS INC PI PHILADELPHIA PA 530 CHESTNUT STREET, STE 850, PHILADELPHIA, PA 19106 USA SN 0278-6826 EI 1521-7388 J9 AEROSOL SCI TECH JI Aerosol Sci. Technol. PY 2014 VL 48 IS 7 BP 738 EP 746 DI 10.1080/02786826.2014.922677 PG 9 WC Engineering, Chemical; Engineering, Mechanical; Environmental Sciences; Meteorology & Atmospheric Sciences SC Engineering; Environmental Sciences & Ecology; Meteorology & Atmospheric Sciences GA AJ4TY UT WOS:000337670400006 ER PT J AU Datskos, P Chen, JH Sharma, J AF Datskos, Panos Chen, Jihua Sharma, Jaswinder TI Synthesis of very small diameter silica nanofibers using sound waves SO CHEMICAL COMMUNICATIONS LA English DT Article ID ULTRASOUND; GROWTH; FIBERS AB Silica nanofibers of an average diameter approximate to 30 nm and length approximate to 100 mu m have been synthesized using an unprecedented strategy: sound waves. A new phenomenon, spinning off the nanofibers at silica rod tips, is also observed. C1 [Datskos, Panos; Sharma, Jaswinder] Oak Ridge Natl Lab, Nanosyst Separat & Mat Res Grp, Energy & Transportat Sci Div, Oak Ridge, TN 37831 USA. [Chen, Jihua] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. RP Sharma, J (reprint author), Oak Ridge Natl Lab, Nanosyst Separat & Mat Res Grp, Energy & Transportat Sci Div, One Bethel Valley Rd, Oak Ridge, TN 37831 USA. EM sharmajk@ornl.gov RI Chen, Jihua/F-1417-2011 OI Chen, Jihua/0000-0001-6879-5936 FU U.S. Department of Energy [DE-AC05-00OR22725]; Laboratory Director's Research and Development Program of the Oak Ridge National Laboratory; Oak Ridge National Laboratory by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy FX J. Sharma is a Eugene P. Wigner Fellow at the Oak Ridge National Laboratory managed by UT-Battelle, LLC, for the U.S. Department of Energy under Contract DE-AC05-00OR22725. The work was supported by the Laboratory Director's Research and Development Program of the Oak Ridge National Laboratory. A portion of this research was 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. NR 30 TC 2 Z9 2 U1 4 U2 29 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 2014 VL 50 IS 55 BP 7277 EP 7279 DI 10.1039/c4cc03206c PG 3 WC Chemistry, Multidisciplinary SC Chemistry GA AJ5XT UT WOS:000337764300012 PM 24872205 ER PT J AU Permana, ADC Nugroho, A Lee, HS Bak, SM Chung, KY Min, BK Kim, J AF Permana, Antonius Dimas Chandra Nugroho, Agung Lee, Hong-Shik Bak, Seong-Min Chung, Kyung Yoon Min, Byoung Koun Kim, Jaehoon TI Synthesis of Hydrous Ruthenium Oxide Nanoparticles in Sub- and Supercritical Water and Their Capacitive Properties SO CHEMICAL ENGINEERING COMMUNICATIONS LA English DT Article DE Ruthenium oxide; Subcritical water; Supercapacitor; Supercritical water ID HYDROTHERMAL SYNTHESIS; ELECTROCHEMICAL CAPACITORS; SUPERCAPACITORS; PARTICLES; RUO2; REACTIVITY; DIOXIDE; SIZE AB Hydrous ruthenium oxide (RuO2 center dot nH(2)O) nanoparticles with various particle sizes and water contents were synthesized in sub- and supercritical water in a very short reaction time of 15min. The particle size, surface area, morphology, crystalline structure, and electrochemical properties were analyzed and compared with those of commercial RuO2 particles. Ultrafine spherical RuO2 center dot 0.6H(2)O nanoparticles with an average size of 4.2nm were produced in subcritical water (250 degrees C, 300bar), while larger and more highly crystalline rod-shaped RuO2 center dot(0.3-0.5)H2O particles were produced in supercritical water (400 degrees C, 300bar). The use of NaOH under the supercritical water conditions resulted in a decrease in particle size. The hydrous RuO2 nanoparticles synthesized in subcritical water exhibited a much higher specific capacitance (255Fg(-1)) at a scan rate of 10mVs(-1) than those synthesized in supercritical water (77Fg(-1)) and commercial RuO2 (8Fg(-1)). C1 [Permana, Antonius Dimas Chandra; Nugroho, Agung; Lee, Hong-Shik; Min, Byoung Koun] Korea Inst Sci & Technol, Clean Energy Res Ctr, Seoul, South Korea. [Bak, Seong-Min] Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA. [Bak, Seong-Min; Chung, Kyung Yoon] Korea Inst Sci & Technol, Ctr Energy Convergence, Seoul, South Korea. [Min, Byoung Koun] Korea Univ, Green Sch, Seoul, South Korea. [Kim, Jaehoon] Sungkyunkwan Univ, Sch Mech Engn, Suwon 440746, Gyeong Gi Do, South Korea. [Kim, Jaehoon] SKKU Adv Inst Nano Technol SAINT, Suwon, South Korea. RP Kim, J (reprint author), Sungkyunkwan Univ, Sch Mech Engn, 2066 Seobu Ro, Suwon 440746, Gyeong Gi Do, South Korea. EM jaehoonkim@skku.edu RI Kim, Jaehoon/G-6116-2014; Chung, Kyung Yoon/E-4646-2011; Bak, Seong Min/J-4597-2013; OI Kim, Jaehoon/0000-0001-6188-7571; Chung, Kyung Yoon/0000-0002-1273-746X; Bak, Seong-Min/0000-0002-1626-5949 FU National Research Foundation of Korea; Ministry of Science, ICT & Future Planning [NRF-2013R1A1A2061020]; Korean Government (MSIP) FX This work was supported by the National Research Foundation of Korea grant, funded by the Ministry of Science, ICT & Future Planning (NRF-2013R1A1A2061020). The authors also acknowledge the support from the the University-Institute cooperation program of the National Research Foundation of Korea grant, funded by the Korean Government (MSIP). NR 30 TC 1 Z9 1 U1 7 U2 30 PU TAYLOR & FRANCIS INC PI PHILADELPHIA PA 530 CHESTNUT STREET, STE 850, PHILADELPHIA, PA 19106 USA SN 0098-6445 EI 1563-5201 J9 CHEM ENG COMMUN JI Chem. Eng. Commun. PY 2014 VL 201 IS 10 BP 1259 EP 1269 DI 10.1080/00986445.2013.805127 PG 11 WC Engineering, Chemical SC Engineering GA AJ4AR UT WOS:000337611900001 ER PT J AU Pumera, M Polsky, R Bonanni, A AF Pumera, Martin Polsky, Ronen Bonanni, Alessandra TI Electrochemistry of Graphene SO ELECTROANALYSIS LA English DT Editorial Material C1 [Pumera, Martin; Bonanni, Alessandra] Nanyang Technol Univ, Singapore 639798, Singapore. [Polsky, Ronen] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Pumera, M (reprint author), Nanyang Technol Univ, Singapore 639798, Singapore. RI Bonanni, Alessandra/G-8192-2011; Pumera, Martin/F-2724-2010 OI Pumera, Martin/0000-0001-5846-2951 NR 0 TC 0 Z9 0 U1 0 U2 16 PU WILEY-V C H VERLAG GMBH PI WEINHEIM PA BOSCHSTRASSE 12, D-69469 WEINHEIM, GERMANY SN 1040-0397 EI 1521-4109 J9 ELECTROANAL JI Electroanalysis PD JAN PY 2014 VL 26 IS 1 SI SI BP 4 EP 4 DI 10.1002/elan.201480001 PG 1 WC Chemistry, Analytical; Electrochemistry SC Chemistry; Electrochemistry GA AJ5CT UT WOS:000337699600002 ER PT J AU Xiao, XY Miller, PR Narayan, RJ Brozik, SM Wheeler, DR Brener, I Wang, J Burckel, DB Polsky, R AF Xiao, Xiaoyin Miller, Philip R. Narayan, Roger J. Brozik, Susan M. Wheeler, David R. Brener, Igal Wang, Joseph Burckel, D. Bruce Polsky, Ronen TI Simultaneous Detection of Dopamine, Ascorbic Acid and Uric Acid at Lithographically-Defined 3D Graphene Electrodes SO ELECTROANALYSIS LA English DT Article DE Dopamine; Ascorbic acid; Uric acid; Graphene electrodes ID POROUS CARBON ELECTRODES; ELECTROCHEMISTRY; TRANSPORT; GRAPHITE; FOAM AB Three dimensional graphene electrodes are presented as highly sensitive electrochemical transducers for the detection of dopamine, ascorbic acid, and uric acid. The detection limits for each separate analyte is approximately 5 mu M. In addition the oxidative peak potentials for each are sufficiently separated such that the simultaneous detection of a mixture can be accomplished without any modification steps leading to three well resolved peaks. Increased steady state mass transport profiles due to enhanced diffusion effects at the open porous three dimensional graphene electrodes are also observed. C1 [Xiao, Xiaoyin; Miller, Philip R.; Brozik, Susan M.; Wheeler, David R.; Brener, Igal; Burckel, D. Bruce; Polsky, Ronen] Sandia Natl Labs, Albuquerque, NM 87185 USA. [Miller, Philip R.; Narayan, Roger J.] Univ N Carolina, Joint Dept Biomed Engn, Raleigh, NC 27695 USA. [Miller, Philip R.; Narayan, Roger J.] N Carolina State Univ, Raleigh, NC 27695 USA. [Wang, Joseph] Univ Calif San Diego, Dept NanoEngn, La Jolla, CA 92093 USA. RP Burckel, DB (reprint author), Sandia Natl Labs, POB 5800, Albuquerque, NM 87185 USA. EM rpolsky@sandia.gov RI Wang, Joseph/C-6175-2011 FU United States Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX Sandia is 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. The authors acknowledge the Sandia National Laboratories' Laboratory Directed Research & Development (LDRD) program. NR 18 TC 10 Z9 11 U1 4 U2 38 PU WILEY-V C H VERLAG GMBH PI WEINHEIM PA BOSCHSTRASSE 12, D-69469 WEINHEIM, GERMANY SN 1040-0397 EI 1521-4109 J9 ELECTROANAL JI Electroanalysis PD JAN PY 2014 VL 26 IS 1 SI SI BP 52 EP 56 DI 10.1002/elan.201300253 PG 5 WC Chemistry, Analytical; Electrochemistry SC Chemistry; Electrochemistry GA AJ5CT UT WOS:000337699600005 ER PT J AU Davis, DJ Raji, ARO Lambert, TN Vigil, JA Li, L Nan, KW Tour, JM AF Davis, Danae J. Raji, Abdul-Rahman O. Lambert, Timothy N. Vigil, Julian A. Li, Lei Nan, Kewang Tour, James M. TI Silver-Graphene Nanoribbon Composite Catalyst for the Oxygen Reduction Reaction in Alkaline Electrolyte SO ELECTROANALYSIS LA English DT Article DE Silver nanoparticles; Graphene nanoribbons; Oxygen reduction reaction; Catalysis ID AG NANOPARTICLES; FUNCTIONALIZATION; ELECTROCATALYSIS; HYBRIDS; STACKS; MEDIA; STATE; PT/C; AU AB Silver-graphene nanoribbons (Ag-GNRs) were prepared from the chemical unzipping of multiwalled carbon nanotubes (MWCNTs) by reaction with Na/K alloy, Ag(O2CCH3) and then CH3OH. Ag-GNRs exhibited improved electrocatalytic ability for the oxygen reduction reaction (ORR) in 0.1 M KOH as compared to the underlying GNR substrate alone and displayed an earlier onset and higher currents than a commercial Ag/Carbon (Ag/C) catalyst. The Ag-GNR hybrid demonstrates an outstanding tolerance to CH3OH crossover which exceeds that of the commercial benchmark, 20% Pt/C. C1 [Davis, Danae J.; Lambert, Timothy N.; Vigil, Julian A.] Sandia Natl Labs, Dept Mat Devices & Energy Technol, Albuquerque, NM 87185 USA. [Raji, Abdul-Rahman O.; Li, Lei; Tour, James M.] Rice Univ, Dept Chem, Houston, TX 77005 USA. [Nan, Kewang; Tour, James M.] Rice Univ, Houston, TX 77005 USA. [Tour, James M.] Rice Univ, Richard E Smalley Inst Nanoscale Sci & Technol, Houston, TX 77005 USA. RP Lambert, TN (reprint author), Sandia Natl Labs, Dept Mat Devices & Energy Technol, POB 5800, Albuquerque, NM 87185 USA. EM tnlambe@sandia.gov; tour@rice.edu RI Nan, Kewang /D-9478-2017; Li, Lei /E-4677-2017; OI Nan, Kewang /0000-0002-2745-0656; Tour, James/0000-0002-8479-9328 FU Sandia National Laboratories; United States Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000]; AFOSR [FA9550-09-1-0581]; AFOSR MURI Program [FA9550-12-1-0035] FX The work conducted at Sandia National Laboratories was supported by Sandia National Laboratories: 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. The work at Rice University was supported by Sandia National Laboratories, the AFOSR (FA9550-09-1-0581), and the AFOSR MURI Program (FA9550-12-1-0035). NR 31 TC 28 Z9 28 U1 5 U2 52 PU WILEY-V C H VERLAG GMBH PI WEINHEIM PA BOSCHSTRASSE 12, D-69469 WEINHEIM, GERMANY SN 1040-0397 EI 1521-4109 J9 ELECTROANAL JI Electroanalysis PD JAN PY 2014 VL 26 IS 1 SI SI BP 164 EP 170 DI 10.1002/elan.201300254 PG 7 WC Chemistry, Analytical; Electrochemistry SC Chemistry; Electrochemistry GA AJ5CT UT WOS:000337699600019 ER PT J AU Zhang, WY Du, D Gunaratne, D Colby, R Lin, YH Laskin, J AF Zhang, Weiying Du, Dan Gunaratne, Don Colby, Robert Lin, Yuehe Laskin, Julia TI Polyoxometalate-Graphene Nanocomposite Modified Electrode for Electrocatalytic Detection of Ascorbic Acid SO ELECTROANALYSIS LA English DT Article DE Ascorbic acid; Polyoxometalate; Graphene; Nanocomposites ID GLASSY-CARBON ELECTRODE; NANOPARTICLES; BIOSENSORS; NANOTUBES; ENZYME; COMPOSITES; SENSORS; OXIDE AB Phosphomolybdate functionalized graphene nanocomposite (PMo12-GS) has been successfully formed on a glassy carbon electrode (GCE) for the detection of ascorbic acid (AA). The obtained PMo12-GS modified GCE, was characterized by cyclic voltammetry, electrochemical impedance spectroscopy, scanning electron microscopy (SEM) and Fourier transform infrared (FT-IR) spectroscopy and compared with GCE, GS modified GCE, and PMo12 modified GCE. It shows an increased current and a decrease in over-potential of similar to 210 mV. The amperometric signals are linearly proportional to the AA concentration in a wide concentration range from 1 x 10(-6) M to 8 x 10(-3) M, with a detection limit of 0.5 x 10(-6) M. The PMo12-GS modified electrode was employed for the determination of the AA level in vitamin C tablets, with recoveries between 96.3 and 100.8%. C1 [Zhang, Weiying; Du, Dan; Gunaratne, Don; Lin, Yuehe; Laskin, Julia] Pacific NW Natl Lab, Div Phys Sci, Richland, WA 99352 USA. [Colby, Robert] Pacific NW Natl Lab, Environm Mol Sci Lab, Richland, WA 99352 USA. RP Lin, YH (reprint author), Pacific NW Natl Lab, Div Phys Sci, Richland, WA 99352 USA. EM yuehe.lin@pnnl.gov; julia.laskin@pnnl.gov RI Laskin, Julia/H-9974-2012; Du, Dan (Annie)/G-3821-2012; Lin, Yuehe/D-9762-2011 OI Laskin, Julia/0000-0002-4533-9644; Lin, Yuehe/0000-0003-3791-7587 FU Office of Basic Energy Science, Division of Chemical Sciences, and Geosciences & Biosciences of U.S. Department of Energy (DOE); DOE's Office of Biological and Environmental Research; US-DOE [DE-AC05-76RL01830] FX This research was performed at the Pacific Northwest National Laboratory (PNNL) and supported by the Office of Basic Energy Science, Division of Chemical Sciences, and Geosciences & Biosciences of U.S. Department of Energy (DOE). Part of this work was performed using EMSL, a national scientific user facility sponsored by the DOE's Office of Biological and Environmental Research and located at PNNL. PNNL is operated by Battelle for US-DOE under Contract DE-AC05-76RL01830. NR 29 TC 14 Z9 14 U1 9 U2 57 PU WILEY-V C H VERLAG GMBH PI WEINHEIM PA BOSCHSTRASSE 12, D-69469 WEINHEIM, GERMANY SN 1040-0397 EI 1521-4109 J9 ELECTROANAL JI Electroanalysis PD JAN PY 2014 VL 26 IS 1 SI SI BP 178 EP 183 DI 10.1002/elan.201300343 PG 6 WC Chemistry, Analytical; Electrochemistry SC Chemistry; Electrochemistry GA AJ5CT UT WOS:000337699600021 ER PT J AU Kauffman, JL Lesieutre, GA Babuska, V AF Kauffman, Jeffrey L. Lesieutre, George A. Babuska, Vit TI Damping Models for Shear Beams with Applications to Spacecraft Wiring Harnesses SO JOURNAL OF SPACECRAFT AND ROCKETS LA English DT Article ID TIMOSHENKO BEAM; EXPERIMENTAL VALIDATION; VIBRATION; STABILITY; SYSTEMS AB Spacecraft wiring harnesses can fundamentally alter a spacecraft's structural dynamics, necessitating a model to predict the coupled dynamic response of the structure and attached cabling. Although a beam model including first-order transverse shear can accurately predict vibration resonance frequencies, current time domain damping models are inadequate. For example, common proportional damping models result modal damping that depends unrealistically on the frequency. Inspired by a geometric rotation-based viscous damping model that provides frequency independent modal damping in an Euler-Bernoulli formulation, a viscous damping model with terms associated with the shear and bending angles is presented. The model provides modal damping that is approximately constant in the bending-dominated regime (low mode numbers), increasing by at most 6% for a particular selection of bending and shear angle-based damping coefficients. In the shear-dominated regime (high mode numbers), damping values increase linearly with mode number and in proportion to the shear angle-based damping coefficient. A key feature of this shear beam damping model is its ready finite element implementation using only matrices commonly developed for an Euler-Bernoulli beam. Such an analysis using empirically determined damping coefficients generates damping values that agree well with existing spacecraft wiring harness cable data. C1 [Kauffman, Jeffrey L.] Univ Cent Florida, Dept Mech & Aerosp Engn, Orlando, FL 32816 USA. [Lesieutre, George A.] Penn State Univ, Dept Aerosp Engn, University Pk, PA 16802 USA. [Babuska, Vit] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Kauffman, JL (reprint author), Univ Cent Florida, Dept Mech & Aerosp Engn, POB 162450, Orlando, FL 32816 USA. RI Kauffman, Jeffrey/G-3811-2012; OI Kauffman, Jeffrey/0000-0003-1980-9865; Lesieutre, George/0000-0003-4547-5379 FU Sandia National Laboratories; United States Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX This work was supported by Sandia National Laboratories. Sandia National Laboratories is a multiprogram laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the United States Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000. The authors also thank Hartono "Anton" Sumali as well as Emil Ardelean, Douglas Coombs, and James Goodding for thoroughly explaining the experimental process and indicating the most useful and robust cable data, and Randy Mayes for his helpful review and comments in preparing this article. NR 21 TC 0 Z9 0 U1 5 U2 12 PU AMER INST AERONAUTICS ASTRONAUTICS PI RESTON PA 1801 ALEXANDER BELL DRIVE, STE 500, RESTON, VA 22091-4344 USA SN 0022-4650 EI 1533-6794 J9 J SPACECRAFT ROCKETS JI J. Spacecr. Rockets PD JAN-FEB PY 2014 VL 51 IS 1 BP 16 EP 22 DI 10.2514/1.A32440 PG 7 WC Engineering, Aerospace SC Engineering GA AJ6JY UT WOS:000337800900003 ER PT J AU Yoo, SY Merzlyak, A Lee, SW AF Yoo, So Young Merzlyak, Anna Lee, Seung-Wuk TI Synthetic Phage for Tissue Regeneration SO MEDIATORS OF INFLAMMATION LA English DT Review ID GENETICALLY-ENGINEERED VIRUSES; FILAMENTOUS PHAGE; GENE DELIVERY; MAMMALIAN-CELLS; LANDSCAPE PHAGE; DRUG-DELIVERY; GROWTH-FACTOR; DISPLAY; RECEPTOR; PEPTIDE AB Controlling structural organization and signaling motif display is of great importance to design the functional tissue regenerating materials. Synthetic phage, genetically engineered M13 bacteriophage has been recently introduced as novel tissue regeneration materials to display a high density of cell-signaling peptides on their major coat proteins for tissue regeneration purposes. Structural advantages of their long-rod shape and monodispersity can be taken together to construct nanofibrous scaffolds which support cell proliferation and differentiation as well as direct orientation of their growth in two or three dimensions. This review demonstrated how functional synthetic phage is designed and subsequently utilized for tissue regeneration that offers potential cell therapy. C1 [Yoo, So Young] Pusan Natl Univ, Sch Med, Med Res Inst, Convergence Stem Cell Res Ctr, Yangsan 626870, South Korea. [Merzlyak, Anna; Lee, Seung-Wuk] Univ Calif Berkeley, Dept Bioengn, Berkeley, CA 94720 USA. [Merzlyak, Anna; Lee, Seung-Wuk] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA 94720 USA. RP Yoo, SY (reprint author), Pusan Natl Univ, Sch Med, Med Res Inst, Convergence Stem Cell Res Ctr, Yangsan 626870, South Korea. EM yoosy2@gmail.com OI Yoo, So Young/0000-0001-8875-9289 FU National Research Foundation of Korea (NRF); Ministry of Science, ICT and Future Planning [2013R1A1A3008484] FX This research was supported by Basic Science Research Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Science, ICT and Future Planning (2013R1A1A3008484). NR 96 TC 3 Z9 3 U1 5 U2 19 PU HINDAWI LTD PI LONDON PA ADAM HOUSE, 3RD FLR, 1 FITZROY SQ, LONDON, WIT 5HE, ENGLAND SN 0962-9351 EI 1466-1861 J9 MEDIAT INFLAMM JI Mediat. Inflamm. PY 2014 AR 192790 DI 10.1155/2014/192790 PG 11 WC Cell Biology; Immunology SC Cell Biology; Immunology GA AJ1TQ UT WOS:000337439100001 ER PT S AU Yoon, HJ Carmichael, TR Tourassi, G AF Yoon, Hong-Jun Carmichael, Tandy R. Tourassi, Georgia BE MelloThoms, CR Kupinski, MA TI Gaze as a Biometric SO MEDICAL IMAGING 2014: IMAGE PERCEPTION, OBSERVER PERFORMANCE, AND TECHNOLOGY ASSESSMENT SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Medical Imaging - Image Perception, Observer Performance, and Technology Assessment CY FEB 16-17, 2014 CL San Diego, CA SP SPIE, Modus Med Devices Inc, XIFIN Inc, Ventana Med Syst Inc, Intrace Med DE eye tracking; perceptual organization; user modeling ID EYE-MOVEMENTS AB Two people may analyze a visual scene in two completely different ways. Our study sought to determine whether human gaze may be used to establish the identity of an individual. To accomplish this objective we investigated the gaze pattern of twelve individuals viewing still images with different spatial relationships. Specifically, we created 5 visual "dot-pattern" tests to be shown on a standard computer monitor. These tests challenged the viewer's capacity to distinguish proximity, alignment, and perceptual organization. Each test included 50 images of varying difficulty (total of 250 images). Eye-tracking data were collected from each individual while taking the tests. The eye-tracking data were converted into gaze velocities and analyzed with Hidden Markov Models to develop personalized gaze profiles. Using leave-one-out cross-validation, we observed that these personalized profiles could differentiate among the 12 users with classification accuracy ranging between 53% and 76%, depending on the test. This was statistically significantly better than random guessing (i.e., 8.3% or 1 out of 12). Classification accuracy was higher for the tests where the users' average gaze velocity per case was lower. The study findings support the feasibility of using gaze as a biometric or personalized biomarker. These findings could have implications in Radiology training and the development of personalized e-learning environments. C1 [Yoon, Hong-Jun; Tourassi, Georgia] Oak Ridge Natl Lab, Hlth Data Sci Inst, Biomed Sci & Engn Ctr, One Bethel Valley Rd, Oak Ridge, TN 37830 USA. [Carmichael, Tandy R.] Tennessee Technol Univ, Dept Elect & Comp Engn, Cookeville, TN 38505 USA. RP Yoon, HJ (reprint author), Oak Ridge Natl Lab, Hlth Data Sci Inst, Biomed Sci & Engn Ctr, One Bethel Valley Rd, Oak Ridge, TN 37830 USA. EM tourassig@ornl.gov OI Tourassi, Georgia/0000-0002-9418-9638 FU U. S. Department of Energy [DE- AC05 00OR22725] FX This manuscript has been authored by UT- Battelle, LLC, under Contract No. 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 18 TC 1 Z9 1 U1 0 U2 1 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9830-4 J9 PROC SPIE PY 2014 VL 9037 AR UNSP 903707 DI 10.1117/12.2044303 PG 7 WC Optics; Radiology, Nuclear Medicine & Medical Imaging SC Optics; Radiology, Nuclear Medicine & Medical Imaging GA BA7IZ UT WOS:000337585600006 ER PT S AU Sukumar, SR Ainsworth, KC AF Sukumar, Sreenivas R. Ainsworth, Keela C. BE Law, MY Cook, TS TI Pattern Search in Multi-structure Data: A Framework for the Next-Generation Evidence-based Medicine SO MEDICAL IMAGING 2014: PACS AND IMAGING INFORMATICS: NEXT GENERATION AND INNOVATIONS SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Medical Imaging - PACS and Imaging Informatics - Next Generation and Innovations CY FEB 18-20, 2014 CL San Diego, CA SP SPIE, Modus Med Devices Inc, XIFIN Inc, Ventana Med Syst Inc, Intrace Med DE pattern search; hypothesis discovery; structured data; unstructured data; multi-structure data analysis ID DISCOVERY; ARROWSMITH AB With the impetus towards personalized and evidence-based medicine, the need for a framework to analyze/interpret quantitative measurements (blood work, toxicology, etc.) with qualitative descriptions (specialist reports after reading images, bio-medical knowledgebase, etc.) to predict diagnostic risks is fast emerging. Addressing this need, we pose and answer the following questions: (i) How can we jointly analyze and explore measurement data in context with qualitative domain knowledge? (ii) How can we search and hypothesize patterns (not known apriori) from such multi-structure data? (iii) How can we build predictive models by integrating weakly-associated multi-relational multi-structure data? We propose a framework towards answering these questions. We describe a software solution that leverages hardware for scalable in-memory analytics and applies next-generation semantic query tools on medical data. C1 [Sukumar, Sreenivas R.; Ainsworth, Keela C.] Oak Ridge Natl Lab, Computat Sci & Engn Div, Oak Ridge, TN 37831 USA. RP Sukumar, SR (reprint author), Oak Ridge Natl Lab, Computat Sci & Engn Div, 1 Bethel Valley Rd, Oak Ridge, TN 37831 USA. EM sukumarsr@ornl.gov NR 24 TC 0 Z9 0 U1 0 U2 1 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9832-8 J9 PROC SPIE PY 2014 VL 9039 AR 90390O DI 10.1117/12.2044378 PG 6 WC Optics; Radiology, Nuclear Medicine & Medical Imaging SC Optics; Radiology, Nuclear Medicine & Medical Imaging GA BA7IY UT WOS:000337584000021 ER PT B AU Christ-Lakin, H Hess, DR AF Christ-Lakin, Heather Hess, Darlene R. BE Svyantek, DJ Mahoney, KT TI TRANSFORMATIONAL LEADERSHIP AND SPIRITUAL INTELLIGENCE SO ORGANIZATIONAL PROCESSES AND RECEIVED WISDOM SE Research in Organizational Sciences LA English DT Article; Book Chapter ID WORKPLACE SPIRITUALITY; SPECIAL-ISSUE; ORGANIZATIONS; PERSPECTIVE; PERFORMANCE; MANAGEMENT; PARADIGM; SEEKING; IMPACT; VALUES C1 [Christ-Lakin, Heather] Sandia Natl Labs, Livermore, CA 94550 USA. [Christ-Lakin, Heather] Univ Phoenix, Houston, TX USA. RP Christ-Lakin, H (reprint author), Sandia Natl Labs, Livermore, CA 94550 USA. NR 171 TC 0 Z9 0 U1 0 U2 3 PU INFORMATION AGE PUBLISHING-IAP PI CHARLOTTE PA PO BOX 79049, CHARLOTTE, NC 28271-7047 USA BN 978-1-62396-550-1; 978-1-62396-551-8 J9 RES ORG SCI PY 2014 BP 71 EP 99 PG 29 WC Psychology, Applied; Management SC Psychology; Business & Economics GA BA4SJ UT WOS:000336233900005 ER PT S AU Lany, S AF Lany, Stephan BE Teherani, FH Look, DC Rogers, DJ TI Polymorphism, band-structure, band-lineup, and alloy energetics of the group II oxides and sulfides MgO, ZnO, CdO, MgS, ZnS, CdS SO OXIDE-BASED MATERIALS AND DEVICES V SE Proceedings of SPIE LA English DT Proceedings Paper CT Annual Conference on Oxide-Based Materials and Devices V held at SPIE Photonics West CY FEB 02-05, 2014 CL San Francisco, CA SP SPIE DE Transparent conducting oxides; functional materials; polymorphism; band-structure; ionization potential; semiconductor alloys; mixing enthalpy; surface energies ID SEMICONDUCTORS; SURFACE; POTENTIALS; MGXZN1-XO; OFFSETS; ENERGY AB The group II chalcogenides are an important class of functional semiconductor materials exhibiting a remarkable diversity in terms of structure and properties. In order to aid the materials design, a consistent set of electronic structure calculations is presented, including data on the polymorphic energy ordering, the band-structures, the band-lineups relative to the vacuum level, surface energies, as well as on the alloy energetics. To this end, current state-of-the-art electronic structure tools are employed, which, besides standard density functional theory (DFT), include total-energy calculation in the random phase approximation and GW quasiparticle energy calculations. The ionization potentials and electron affinities are obtained by combining the results of bulk GW and surface DFT calculations. Considering both octahedral and tetrahedral coordination symmetries, exemplified by the rock-salt and zinc-blende lattices, respectively, this data reveals both the chemical and structural trends within this materials family. C1 Natl Renewable Energy Lab, Golden, CO 80401 USA. RP Lany, S (reprint author), Natl Renewable Energy Lab, 15013 Denver West Blvd, Golden, CO 80401 USA. EM Stephan.Lany@NREL.gov OI Lany, Stephan/0000-0002-8127-8885 NR 41 TC 1 Z9 1 U1 4 U2 21 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9900-4 J9 PROC SPIE PY 2014 VL 8987 AR 89870K DI 10.1117/12.2043587 PG 8 WC Optics; Physics, Applied SC Optics; Physics GA BA7IW UT WOS:000337582100015 ER PT J AU Kramer, MJ Mendelev, MI Asta, M AF Kramer, M. J. Mendelev, M. I. Asta, M. TI Structure of liquid Al and Al67Mg33 alloy: comparison between experiment and simulation SO PHILOSOPHICAL MAGAZINE LA English DT Article DE liquid metals; molecular dynamic simulations; X-ray diffraction ID INTERATOMIC POTENTIALS APPROPRIATE; UNIVERSAL SCALING LAW; AUGMENTED-WAVE METHOD; MOLECULAR-DYNAMICS; ENERGY CALCULATIONS; ELECTRON-GAS; METALS; DIFFRACTION; ALUMINUM; DISTRIBUTIONS AB We report data on the structure of liquid Al and an Al67Mg33 alloy obtained from state-of-the-art X-ray diffraction experiments and ab initio molecular dynamics (AIMD) simulations. To facilitate a direct comparison between these data, we develop a method to elongate the AIMD pair correlation function in order to obtain reliable AIMD structure factors. The comparison reveals an appreciable level of discrepancy between experimental and AIMD liquid structures, with the latter being consistently more ordered than the former at the same temperature. The discrepancy noted in this study is estimated to have significant implications for simulation-based calculations of liquid transport properties and solid-liquid interface kinetic properties. C1 [Kramer, M. J.; Mendelev, M. I.] Iowa State Univ, Ames Lab, Div Mat Sci & Engn, Ames, IA 50011 USA. [Asta, M.] Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA. RP Mendelev, MI (reprint author), Iowa State Univ, Ames Lab, Div Mat Sci & Engn, Ames, IA 50011 USA. EM mendelev@ameslab.gov FU Department of Energy, Office of Basic Energy Sciences [DE-AC02-07CH11358]; US Department of Energy, Office of Science and Basic Energy Sciences [DE-AC02-06CH11357]; Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division, of the US Department of Energy (DOE) [DE-FG02-06ER46282] FX Work at the Ames Laboratory was supported by the Department of Energy, Office of Basic Energy Sciences [Contract number DE-AC02-07CH11358]. The high-energy X-ray work at the MUCAT sector of the APS was supported by the US Department of Energy, Office of Science and Basic Energy Sciences [Contract number DE-AC02-06CH11357]. MA acknowledges support from the Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division, of the US Department of Energy (DOE) [Contract number DE-FG02-06ER46282]. NR 46 TC 6 Z9 6 U1 4 U2 21 PU TAYLOR & FRANCIS LTD PI ABINGDON PA 4 PARK SQUARE, MILTON PARK, ABINGDON OX14 4RN, OXON, ENGLAND SN 1478-6435 EI 1478-6443 J9 PHILOS MAG JI Philos. Mag. PY 2014 VL 94 IS 17 BP 1876 EP 1892 DI 10.1080/14786435.2014.886786 PG 17 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering; Physics, Applied; Physics, Condensed Matter SC Materials Science; Metallurgy & Metallurgical Engineering; Physics GA AJ3YU UT WOS:000337605100002 ER PT J AU Planes, A Castan, T Saxena, A AF Planes, A. Castan, T. Saxena, A. TI Thermodynamics of multicaloric effects in multiferroics SO PHILOSOPHICAL MAGAZINE LA English DT Article DE ferroelectrics; ferromagnetism; functional materials; thermodynamics ID ADIABATIC TEMPERATURE-CHANGE; GD5SI2GE2; POLARIZATION AB We provide a general thermodynamic framework to study multicaloric effects in multiferroic materials. This is applied to the case of a magnetoelectric multiferroic such as BiFeO3, which is described by means of a Landau free energy with a biquadratic coupling between polarization and magnetization. We obtain a phase diagram, the isothermal entropy change and the adiabatic temperature change across different continuous and first-order phase transitions as the applied electric and magnetic fields are varied. The multicaloric effects are suitably decomposed into the corresponding electrocaloric and magnetocaloric contributions. C1 [Planes, A.; Castan, T.] Univ Barcelona, Fac Fis, Dept Estruct & Constituents Mat, E-08028 Barcelona, Catalonia, Spain. [Saxena, A.] Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. RP Planes, A (reprint author), Univ Barcelona, Fac Fis, Dept Estruct & Constituents Mat, Diagonal 647, E-08028 Barcelona, Catalonia, Spain. EM toni@ecm.ub.edu RI Planes, Antoni/O-1904-2015 OI Planes, Antoni/0000-0001-5213-5714 FU CICyT (Spain) [MAT2013-40590-P]; US Department of Energy FX This work was supported by CICyT (Spain) through project MAT2013-40590-P and in part by the US Department of Energy. NR 26 TC 21 Z9 21 U1 3 U2 45 PU TAYLOR & FRANCIS LTD PI ABINGDON PA 2-4 PARK SQUARE, MILTON PARK, ABINGDON OR14 4RN, OXON, ENGLAND SN 1478-6435 EI 1478-6443 J9 PHILOS MAG JI Philos. Mag. PY 2014 VL 94 IS 17 BP 1893 EP 1908 DI 10.1080/14786435.2014.899438 PG 16 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering; Physics, Applied; Physics, Condensed Matter SC Materials Science; Metallurgy & Metallurgical Engineering; Physics GA AJ3YU UT WOS:000337605100003 ER PT J AU Lawson, AC AF Lawson, A. C. TI Gruneisen analysis of thermodynamic properties of delta-phase Pu-Ga alloys SO PHILOSOPHICAL MAGAZINE LA English DT Article DE actinides; thermal expansion; elasticity ID THERMAL-EXPANSION; ELASTIC-CONSTANTS; PLUTONIUM; TEMPERATURE AB We present a Gruneisen analysis of the intriguing temperature dependence of the thermal expansion and bulk modulus of delta phase plutonium alloys. This analysis exploits the thermodynamic relationship between these quantities and the heat capacity and reduces the description of complicated behaviour to the determination of a manageable number of numerical constants. We conclude from the analysis (1) that there is a small Schottky-like heat capacity anomaly at high temperatures and (2) that the size of this anomaly depends strongly on alloy concentration. Gruneisen analysis provides an economical description of the thermal expansion and bulk modulus of delta-Pu. C1 Los Alamos Natl Lab, Manuel Lujan Jr Neutron Scattering Ctr, Los Alamos, NM 87545 USA. RP Lawson, AC (reprint author), Los Alamos Natl Lab, Manuel Lujan Jr Neutron Scattering Ctr, Los Alamos, NM 87545 USA. EM aclawson@cybermesa.com FU United States Department of Energy; DOE [DE-AC52-06NA25396] FX We are pleased to thank Tongsik Lee and Gerry Lander for many useful discussions. Research was performed under the auspices of the United States Department of Energy. This work has benefited from the use of NPD at the Lujan Center at Los Alamos Neutron Science Center, funded by DOE Office of Basic Energy Sciences. Los Alamos National Laboratory is operated by Los Alamos National Security LLC under DOE Contract DE-AC52-06NA25396. NR 29 TC 2 Z9 2 U1 2 U2 12 PU TAYLOR & FRANCIS LTD PI ABINGDON PA 4 PARK SQUARE, MILTON PARK, ABINGDON OX14 4RN, OXON, ENGLAND SN 1478-6435 EI 1478-6443 J9 PHILOS MAG JI Philos. Mag. PY 2014 VL 94 IS 19 BP 2150 EP 2161 DI 10.1080/14786435.2014.906759 PG 12 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering; Physics, Applied; Physics, Condensed Matter SC Materials Science; Metallurgy & Metallurgical Engineering; Physics GA AJ4CJ UT WOS:000337617600003 ER PT J AU Barenblatt, GI Chorin, AJ Prostokishin, VM AF Barenblatt, G. I. Chorin, A. J. Prostokishin, V. M. TI Turbulent flows at very large Reynolds numbers: new lessons learned SO PHYSICS-USPEKHI LA English DT Review AB The universal (Reynolds-number-independent) von Karman Prandt1 logarithmic law for the velocity distribution in the basic intermediate region of a turbulent shear flow is generally considered to be one of the fundamental laws of engineering science and is taught universally in fluid mechanics and hydraulics courses. We show here that this law is based on an assumption that cannot be considered to be correct and which does not correspond to experiment. Nor is Landau's derivation of this law quite correct. In this paper, an alternative scaling law explicitly incorporating the influence of the Reynolds number is discussed, as is the corresponding drag law. The study uses the concept of intermediate asymptotics and that of incomplete similarity in the similarity parameter. Yakov Borisovich Zeldovich played an outstanding role in the development of these ideas. This work is a tribute to his glowing memory. C1 [Barenblatt, G. I.; Prostokishin, V. M.] Russian Acad Sci, PP Shirshov Oceanol Inst, Moscow 119997, Russia. [Barenblatt, G. I.; Chorin, A. J.] Univ Calif Berkeley, Berkeley, CA 94720 USA. [Barenblatt, G. I.; Chorin, A. J.; Prostokishin, V. M.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Prostokishin, V. M.] Natl Res Nucl Univ MEPhI, Moscow 115409, Russia. RP Barenblatt, GI (reprint author), Russian Acad Sci, PP Shirshov Oceanol Inst, Nakhimovskii Prosp 36, Moscow 119997, Russia. EM gibar@math.berkeley.edu; chorin@math.berkeley.edu; VMProstokishin@mephi.ru OI Prostokishin, Valeriy/0000-0001-6185-9642 NR 21 TC 8 Z9 9 U1 3 U2 8 PU TURPION LTD PI BRISTOL PA C/O TURPION LTD, IOP PUBLISHING, TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6HG, ENGLAND SN 1063-7869 EI 1468-4780 J9 PHYS-USP+ JI Phys. Usp. PY 2014 VL 57 IS 3 BP 250 EP 256 DI 10.3367/UFNr.0184.201403d.0265 PG 7 WC Physics, Multidisciplinary SC Physics GA AJ0QN UT WOS:000337360600004 ER PT S AU Hong, TZ Yang, L Xia, JJ Feng, W AF Hong, Tianzhen Yang, Le Xia, Jianjun Feng, Wei BE Li, A Zhu, Y Li, Y TI Building Energy Benchmarking Between the United States and China: Methods and Challenges SO PROCEEDINGS OF THE 8TH INTERNATIONAL SYMPOSIUM ON HEATING, VENTILATION AND AIR CONDITIONING, VOL 3: BUILDING SIMULATION AND INFORMATION MANAGEMENT SE Lecture Notes in Electrical Engineering LA English DT Proceedings Paper CT 8th International Symposium on Heating, Ventilation, and Air Conditioning (ISHVAC) CY OCT 19-21, 2013 CL Xian, PEOPLES R CHINA SP Xian Univ Architecture & Technol, Tsinghua Univ, Univ Hong Kong DE Benchmarking; Buildings; China; Data analysis; Data model; Energy data; United States AB Currently, buildings in the U. S. account for more than 40 % of total primary energy. In China, the same figure is 20 %. Detailed building energy analysis and benchmarking based on energy monitoring are becoming vitally important for the evaluation of energy-efficient technologies and related policy making. This paper focuses on methods and challenges in energy benchmarking of office buildings between the U. S. and China, based on the experiences and outcomes of a joint research project under the U.S.-China Clean Energy Research Center for Building Energy Efficiency (CERC-BEE). First, benchmarking methods were presented, including data analysis methods, required data, building selection criteria, and a standard data model for building energy use. Annual electricity use benchmarking was performed from a sample of selected office buildings in both countries, with the aim of identifying and understanding the main discrepancies and key driving factors. Benchmarking challenges were then summarized and discussed, and some potential solutions were proposed, including the process of building selection, data collection and clean-up, and specific analysis techniques. Recommendations were proposed for future work to improve the process and outcomes of building energy benchmarking between the two countries. C1 [Hong, Tianzhen] Lawrence Berkeley Natl Lab, Simulat Res Grp, Berkeley, CA 94720 USA. [Hong, Tianzhen; Feng, Wei] Lawrence Berkeley Natl Lab LBNL, Berkeley, CA 94720 USA. [Yang, Le; Xia, Jianjun] Tsinghua Univ, Beijing 100084, Peoples R China. RP Hong, TZ (reprint author), Lawrence Berkeley Natl Lab, Simulat Res Grp, Berkeley, CA 94720 USA. EM thong@lbl.gov FU U. S.- China Clean Energy Research Center for Building Energy Efficiency FX This work was supported by the U. S.- China Clean Energy Research Center for Building Energy Efficiency. The authors appreciate the building owners, facility managers, and a few LBNL researchers for providing building data and related information for the project. NR 15 TC 2 Z9 2 U1 0 U2 3 PU SPRINGER-VERLAG BERLIN PI BERLIN PA HEIDELBERGER PLATZ 3, D-14197 BERLIN, GERMANY SN 1876-1100 BN 978-3-642-39578-9; 978-3-642-39577-2 J9 LECT NOTES ELECTR EN PY 2014 VL 263 BP 473 EP 486 DI 10.1007/978-3-642-39578-9_50 PG 14 WC Construction & Building Technology SC Construction & Building Technology GA BA7JF UT WOS:000337595000050 ER PT J AU Carrington, DB Munoz, DA Heinrich, JC AF Carrington, David B. Munoz, Dominic A. Heinrich, Juan C. TI Modelling fluid flow in domains containing moving interfaces SO PROGRESS IN COMPUTATIONAL FLUID DYNAMICS LA English DT Article DE fluid flow; moving interfaces; arbitrary Lagrangian-Eulerian; ALE; fixed mesh; local mesh adaptation ID FINITE-ELEMENT METHOD; DENDRITIC SOLIDIFICATION; ALE; COMPUTATIONS; STRATEGIES; BOUNDARIES; SCHEMES; ENGINE; CODE AB A method for the numerical simulations of fluid flow in domains containing moving rigid objects or boundaries is presented, which falls into the general category of arbitrary Lagrangian-Eulerian methods. The method is based on a fixed mesh that is modified locally both in space and time to describe the moving interfaces that are allowed to displace independently of the mesh. It results in a fully robust formulation capable of calculating in irregular meshes on domains of complex geometry containing moving devises without danger of the mesh becoming unsuitable due to its continuous deformation. This work presents the ideas in the context of two space dimensions, and constitutes the first stage in the development of a three-dimensional model to interface with the KIVA simulator developed by Los Alamos National Laboratory. The method's capabilities and accuracy are assessed using several examples including a case that has an analytical solution. C1 [Carrington, David B.] Los Alamos Natl Lab, Theoret Div Fluid Dynam T 03, Los Alamos, NM 87545 USA. [Munoz, Dominic A.] Alion Sci & Technol, Albuquerque, NM 87110 USA. [Heinrich, Juan C.] Univ New Mexico, Dept Mech Engn, Albuquerque, NM 87131 USA. RP Carrington, DB (reprint author), Los Alamos Natl Lab, Theoret Div Fluid Dynam T 03, POB 1663,MS B216, Los Alamos, NM 87545 USA. EM dcarring@lanl.gov; dmunoz@alionscience.com; heinrich@unm.edu FU LLC for the National Nuclear Security Administration of the U.S. Department of Energy (DOE) [DE-AC52-06NA25396]; Los Alamos National Laboratory; DOE's Office of Energy Efficiency and Renewable Energy (EERE) Advanced Combustion Programme FX The DOE's Office of Energy Efficiency and Renewable Energy (EERE) Advanced Combustion Programme (Gurpreet Singh) is supporting this effort. 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 (DOE) under contract DE-AC52-06NA25396. Los Alamos National Laboratory strongly supports academic freedom and a researcher's right to publish; as an institution, however, the Laboratory does not endorse the viewpoint of a publication or guarantee its technical correctness. NR 27 TC 1 Z9 1 U1 0 U2 1 PU INDERSCIENCE ENTERPRISES LTD PI GENEVA PA WORLD TRADE CENTER BLDG, 29 ROUTE DE PRE-BOIS, CASE POSTALE 856, CH-1215 GENEVA, SWITZERLAND SN 1468-4349 EI 1741-5233 J9 PROG COMPUT FLUID DY JI Prog. Comput. Fluid Dyn. PY 2014 VL 14 IS 3 BP 139 EP 150 DI 10.1504/PCFD.2014.062429 PG 12 WC Thermodynamics; Mechanics SC Thermodynamics; Mechanics GA AJ4YT UT WOS:000337687100001 ER PT J AU Chapman, JL Lu, L Anderson-Cook, CM AF Chapman, Jessica L. Lu, Lu Anderson-Cook, Christine M. TI Process Optimization for Multiple Responses Utilizing the Pareto Front Approach SO QUALITY ENGINEERING LA English DT Article DE graphical summary; multiple response optimization; response surface; trade-offs ID DESIGN AB In many optimization situations, there are several responses associated with a product or process that need to be jointly considered. In this article we present Pareto front multiple objective optimization as an option to complement other statistical and mathematical methods in the response surface methodology toolkit. We demonstrate the Pareto front approach for multiple response process optimization based on evaluating a fine grid of input variable combinations within the range of operating conditions, as well as the use of a set of graphical tools to aid in decision making, with an example process involving two inputs and three responses of interest. We also discuss a simple way to examine the impact that variability in the responses can have on the solution by considering the estimated mean and worst-case response values. R code for implementing the methods discussed in this article is available upon request (jchapman@stlawu.edu). C1 [Chapman, Jessica L.] St Lawrence Univ, Dept Math Comp Sci & Stat, Canton, NY 13617 USA. [Lu, Lu] Univ S Florida, Dept Math & Stat, Tampa, FL USA. [Anderson-Cook, Christine M.] Los Alamos Natl Lab, Stat Sci Grp, Los Alamos, NM USA. RP Chapman, JL (reprint author), St Lawrence Univ, Dept Math Comp Sci & Stat, 23 Romoda Dr, Canton, NY 13617 USA. EM jchapman@stlawu.edu NR 14 TC 11 Z9 11 U1 3 U2 5 PU TAYLOR & FRANCIS INC PI PHILADELPHIA PA 530 CHESTNUT STREET, STE 850, PHILADELPHIA, PA 19106 USA SN 0898-2112 EI 1532-4222 J9 QUAL ENG JI Qual. Eng. PY 2014 VL 26 IS 3 BP 253 EP 268 DI 10.1080/08982112.2013.852681 PG 16 WC Engineering, Industrial; Statistics & Probability SC Engineering; Mathematics GA AJ3PW UT WOS:000337580200001 ER PT J AU Lu, L Johnson, ME Anderson-Cook, CM AF Lu, Lu Johnson, Mark E. Anderson-Cook, Christine M. TI Selecting a Best Two-Level 16-Run Screening Design from the Catalog of Nonisomorphic Regular and Nonregular Designs for Six to Eight Factors SO QUALITY ENGINEERING LA English DT Article DE alias patterns; design generators; desirability functions; nondominated designs; Pareto front optimization; supersaturated ID RESPONSE-SURFACE DESIGN; MULTIPLE CRITERIA; PARETO FRONTIER; OPTIMIZATION AB When exploring first-order models including two-factor interactions for six to eight factors using a 16-run design, there are many possible model choices. Building on the Johnson and Jones (2010) catalog of the nonisomorphic regular and nonregular design alternatives, we summarize which of these design options are most promising based on two common design criteria. The Pareto fronts based on the criteria E(s(2)) and tr(AA') suggest that only a handful of the possible designs should be considered further, and the best design depends on the relative emphasis given each of the two criteria. This article considers each case of six, seven, and eight factors for 16-run two-level designs and provides numerical and graphical comparisons between the alternatives to highlight the merits of the leading candidates. C1 [Lu, Lu] Univ S Florida, Dept Math & Stat, Tampa, FL USA. [Johnson, Mark E.] Univ Cent Florida, Dept Stat, Orlando, FL 32816 USA. [Anderson-Cook, Christine M.] Los Alamos Natl Lab, Stat Sci Grp, Los Alamos, NM USA. RP Lu, L (reprint author), 4202 E Fowler Ave, Tampa, FL 33620 USA. EM icyemma@gmail.com NR 13 TC 1 Z9 1 U1 0 U2 2 PU TAYLOR & FRANCIS INC PI PHILADELPHIA PA 530 CHESTNUT STREET, STE 850, PHILADELPHIA, PA 19106 USA SN 0898-2112 EI 1532-4222 J9 QUAL ENG JI Qual. Eng. PY 2014 VL 26 IS 3 BP 269 EP 284 DI 10.1080/08982112.2013.854903 PG 16 WC Engineering, Industrial; Statistics & Probability SC Engineering; Mathematics GA AJ3PW UT WOS:000337580200002 ER PT J AU Hamada, MS Kelly, E Buxton, T AF Hamada, M. S. Kelly, E. Buxton, T. TI Understanding the Rule of 7: Statistical Properties for Various Sample Sizes SO QUALITY ENGINEERING LA English DT Article DE confidence interval; coverage probability; range; relative length distribution; tolerance interval AB Motivated by an engineer's question to understand the "Rule of 7'' sample size rule of thumb, this article studies the statistical properties for a sample size of 7 and well as other sample sizes. Properties of ranges, tolerance intervals and confidence intervals, are considered. Sample size recommendations are made. C1 [Hamada, M. S.; Kelly, E.] Los Alamos Natl Lab, Stat Sci Grp, Los Alamos, NM 87545 USA. [Buxton, T.] Los Alamos Natl Lab, Oversight Surveillance Grp, Los Alamos, NM 87545 USA. RP Hamada, MS (reprint author), Los Alamos Natl Lab, Stat Sci Grp, POB 1663, Los Alamos, NM 87545 USA. EM hamada@lanl.gov NR 3 TC 0 Z9 0 U1 0 U2 2 PU TAYLOR & FRANCIS INC PI PHILADELPHIA PA 530 CHESTNUT STREET, STE 850, PHILADELPHIA, PA 19106 USA SN 0898-2112 EI 1532-4222 J9 QUAL ENG JI Qual. Eng. PY 2014 VL 26 IS 3 BP 285 EP 289 DI 10.1080/08982112.2013.805780 PG 5 WC Engineering, Industrial; Statistics & Probability SC Engineering; Mathematics GA AJ3PW UT WOS:000337580200003 ER PT S AU Chou, J Valley, GC Hernandez, VJ Bennett, CV Pelz, L Heebner, J Di Nicola, JM Rever, M Bowers, M AF Chou, Jason Valley, George C. Hernandez, Vincent J. Bennett, Corey V. Pelz, Larry Heebner, John Di Nicola, J. M. Rever, Matthew Bowers, Mark BE Sadwick, LP OSullivan, CM TI RF-Photonic Wideband Measurements of Energetic Pulses on NIF Enhanced by Compressive Sensing Algorithms SO TERAHERTZ, RF, MILLIMETER, AND SUBMILLIMETER-WAVE TECHNOLOGY AND APPLICATIONS VII SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Terahertz, RF, Millimeter, and Submillimeter-Wave Technology and Applications VII CY FEB 04-06, 2014 CL San Francisco, CA SP SPIE, Hubner GmbH & Co KG DE RF signal processing; RF photonics; single-shot; real-time; FM-AM conversion; compressive sensing ID ORTHOGONAL MATCHING PURSUIT AB At the National Ignition Facility (NIF), home of the world's largest laser, a critical pulse screening process is used to ensure safe operating conditions for amplifiers and target optics. To achieve this, high speed recording instrumentation up to 34 GHz measures pulse shape characteristics throughout a facility the size of three football fields-which can be a time consuming procedure. As NIF transitions to higher power handling and increased wavelength flexibility, this lengthy and extensive process will need to be performed far more frequently. We have developed an accelerated high-throughput pulse screener that can identify nonconforming pulses across 48 locations using a single, real-time 34-GHz oscilloscope. Energetic pulse shapes from anywhere in the facility are imprinted onto telecom wavelengths, multiplexed, and transported over fiber without distortion. The critical pulse-screening process at high-energy laser facilities can be reduced from several hours just seconds-allowing greater operational efficiency, agility to system modifications, higher power handling, and reduced costs. Typically, the sampling noise from the oscilloscope places a limit on the achievable signal-to-noise ratio of the measurement, particularly when highly shaped and/or short duration pulses are required by target physicists. We have developed a sophisticated signal processing algorithm for this application that is based on orthogonal matching pursuit (OMP). This algorithm, developed for recovering signals in a compressive sensing system, enables high fidelity single shot screening even for low signal-to-noise ratio measurements. C1 [Chou, Jason; Hernandez, Vincent J.; Bennett, Corey V.; Pelz, Larry; Heebner, John; Di Nicola, J. M.; Rever, Matthew; Bowers, Mark] Lawrence Livermore Natl Lab, 7000 East Ave, Livermore, CA 94550 USA. [Valley, George C.] Aerosp Corp, El Segundo, CA 90245 USA. RP Chou, J (reprint author), Lawrence Livermore Natl Lab, 7000 East Ave, Livermore, CA 94550 USA. EM chou8@llnl.gov NR 8 TC 0 Z9 0 U1 1 U2 10 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9898-4 J9 PROC SPIE PY 2014 VL 8985 AR UNSP 898511 DI 10.1117/12.2042361 PG 10 WC Optics; Physics, Applied SC Optics; Physics GA BA7AS UT WOS:000337347500020 ER PT S AU Burton, T AF Burton, Thomas BE Evans, D Hands, S Lietava, R Romita, R Baillie, OV TI eRHIC: A Precision Tool for Studying Nuclear Structure SO 14TH INTERNATIONAL CONFERENCE ON STRANGENESS IN QUARK MATTER (SQM2013) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 14th International Conference on Strangeness in Quark Matter (SQM) CY JUL 22-27, 2013 CL Univ Birmingham, Birmingham, ENGLAND HO Univ Birmingham AB eRHIC is a proposed electron-ion collider to be located at Brookhaven National Lab. This high-luminosity electron-hadron machine will provide unprecedented precision and versatility in studying features of QCD and the structure of nucleons and nuclei. We describe some key features of the eRHIC proposal, focusing on its potential for understanding the gluon structure of nuclei. C1 Brookhaven Natl Lab, Upton, NY 11973 USA. RP Burton, T (reprint author), Brookhaven Natl Lab, Upton, NY 11973 USA. EM tpb@bnl.gov NR 2 TC 0 Z9 0 U1 0 U2 0 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 509 AR 012057 DI 10.1088/1742-6596/509/1/012057 PG 4 WC Astronomy & Astrophysics; Physics, Applied SC Astronomy & Astrophysics; Physics GA BA6OE UT WOS:000337194300057 ER PT S AU Hao, Q AF Hao, Qiu CA STAR Collaboration BE Evans, D Hands, S Lietava, R Romita, R Baillie, OV TI Status and Physics Opportunities of the STAR Heavy Flavor Tracker and the Muon Telescope Detector Upgrades SO 14TH INTERNATIONAL CONFERENCE ON STRANGENESS IN QUARK MATTER (SQM2013) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 14th International Conference on Strangeness in Quark Matter (SQM) CY JUL 22-27, 2013 CL Univ Birmingham, Birmingham, ENGLAND HO Univ Birmingham ID COLLISIONS AB The STAR Collaboration will complete the Heavy Flavor Tracker (HFT) and the Muon Telescope Detector (MTD) upgrades by 2014. HFT utilizes the state-of-art active pixel detector technology, which will greatly enhance the STAR physics capabilities by measuring heavy quark yield, collectivity and correlations via the topological reconstruction of charmed hadrons over a wide momentum range. The MTD is based on the long Multi-Gap Resistive Plate Chamber detector technology designed to measure muons penetrating the bulk of other detectors and the magnet yoke. It will enable STAR to study di-muon and electron-muon correlations and enhance heavy quarkonium studies. With the addition of these upgrades, STAR is well suited to perform precise measurements of production as well as correlations of rare probes (heavy flavors, dileptons) to systematically investigate the quark-gluon plasma properties at RHIC. For Run 13 63% of the MTD has been installed and data have been taken. Prototype PXL sectors (30% coverage) have also been installed and commissioned. Anticipated physics results and current status of these upgrades is reported. C1 [Hao, Qiu; STAR Collaboration] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Hao, Q (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, 1 Cyclotron Rd, Berkeley, CA 94720 USA. EM hqiu@lbl.gov NR 10 TC 0 Z9 0 U1 0 U2 0 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 509 AR 012026 DI 10.1088/1742-6596/509/1/012026 PG 5 WC Astronomy & Astrophysics; Physics, Applied SC Astronomy & Astrophysics; Physics GA BA6OE UT WOS:000337194300026 ER PT S AU Ploskon, M AF Ploskon, Mateusz CA ALICE Collaboration BE Evans, D Hands, S Lietava, R Romita, R Baillie, OV TI Overview of results from ALICE SO 14TH INTERNATIONAL CONFERENCE ON STRANGENESS IN QUARK MATTER (SQM2013) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 14th International Conference on Strangeness in Quark Matter (SQM) CY JUL 22-27, 2013 CL Univ Birmingham, Birmingham, ENGLAND HO Univ Birmingham ID RANGE ANGULAR-CORRELATIONS; P-PB COLLISIONS; TEV; LHC AB ALICE is a dedicated experiment for measurements of heavy-ion collisions at the Large Hadron Collider (LHC). A wealth of experimental data recorded in 2010, 2011 and 2012 suggests that a strongly interacting de-confined medium is created in collisions of lead ions at a centre-of-mass energy \/(NN)-N-s = 2.76 TeV. In order to quantify the properties of this hot and dense matter, measurements were performed in smaller systems, such as proton-proton and proton-lead, where effects related to the medium are expected to be negligible. We present an overview of recent measurements of particle production and particle correlations in protonproton, Pb Pb and p Pb collisions at the LHC by ALICE Collaboration. C1 [Ploskon, Mateusz; ALICE Collaboration] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Ploskon, M (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, 1 Cyclotron Rd, Berkeley, CA 94720 USA. EM MPloskon@lbl.gov NR 36 TC 0 Z9 0 U1 0 U2 3 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 509 AR 012003 DI 10.1088/1742-6596/509/1/012003 PG 7 WC Astronomy & Astrophysics; Physics, Applied SC Astronomy & Astrophysics; Physics GA BA6OE UT WOS:000337194300003 ER PT S AU Vogt, R AF Vogt, Ramona BE Evans, D Hands, S Lietava, R Romita, R Baillie, OV TI Open and Hidden Heavy Flavor Production in pp, pA and AA Collisions SO 14TH INTERNATIONAL CONFERENCE ON STRANGENESS IN QUARK MATTER (SQM2013) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 14th International Conference on Strangeness in Quark Matter (SQM) CY JUL 22-27, 2013 CL Univ Birmingham, Birmingham, ENGLAND HO Univ Birmingham ID J/PSI; SUPPRESSION; DEPENDENCE; PHYSICS AB In these proceedings we present a brief overview of recent open heavy flavor and quarkonium production theory in proton-proton (pp), proton/deuteron-nucleus (pA, dA) and nucleus-nucleus collisions. C1 Lawrence Livermore Natl Lab, Div Phys, Livermore, CA 94551 USA. RP Vogt, R (reprint author), Lawrence Livermore Natl Lab, Div Phys, Livermore, CA 94551 USA. EM vogt@physics.ucdavis.edu NR 44 TC 2 Z9 2 U1 0 U2 2 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 509 AR 012007 DI 10.1088/1742-6596/509/1/012007 PG 6 WC Astronomy & Astrophysics; Physics, Applied SC Astronomy & Astrophysics; Physics GA BA6OE UT WOS:000337194300007 ER PT S AU Wiranata, A Koch, V Prakash, M Wang, XN AF Wiranata, A. Koch, V. Prakash, M. Wang, X. N. BE Evans, D Hands, S Lietava, R Romita, R Baillie, OV TI Shear viscosity of a multi-component hadronic system SO 14TH INTERNATIONAL CONFERENCE ON STRANGENESS IN QUARK MATTER (SQM2013) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 14th International Conference on Strangeness in Quark Matter (SQM) CY JUL 22-27, 2013 CL Univ Birmingham, Birmingham, ENGLAND HO Univ Birmingham ID KINETIC GAS THEORY AB The shear viscosity eta and entropy density 8 of a hadron gas with zero baryon number density are calculated using the Chapman-Enskog and virial expansion approaches, respectively. Interactions are included via the K-matrix parametrization of cross sections preserving the unitarity of the S-matrix. In the four component mixture (pi - K - N - eta), a total of 57 resonances up to 2 GeV mass are included. Interactions forming resonances reduce the magnitude of eta and increase 8, both effects serving to progressively reduce eta/s as the temperature nears the QCD phase transition temperature. C1 [Wiranata, A.; Wang, X. N.] Cent China Normal Univ, Inst Particle Phys, Wuhan 430079, Peoples R China. [Koch, V.; Wang, X. N.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Nucl Sci, Berkeley, CA 94720 USA. [Prakash, M.] Ohio Univ, Dept Phys & Astron, Athens, OH 45701 USA. RP Wiranata, A (reprint author), Cent China Normal Univ, Inst Particle Phys, Wuhan 430079, Peoples R China. RI Prakash, Madappa/D-9820-2016; OI Wang, Xin-Nian/0000-0002-9734-9967 FU NSFC [11221504, 1350110493]; US DOE [DE-AC02-05CH11231, DE-FG02-93ER-40756] FX This work is supported by the NSFC under grant No. 11221504 & No. 1350110493, and by the US DOE under contracts #DE-AC02-05CH11231 and #DE-FG02-93ER-40756. NR 18 TC 1 Z9 1 U1 0 U2 0 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 509 AR UNSP 012049 DI 10.1088/1742-6596/509/1/012049 PG 4 WC Astronomy & Astrophysics; Physics, Applied SC Astronomy & Astrophysics; Physics GA BA6OE UT WOS:000337194300049 ER PT S AU Zhang, XM AF Zhang, Xiaoming CA ALICE Collaboration BE Evans, D Hands, S Lietava, R Romita, R Baillie, OV TI Nuclear modification factor and elliptic flow of muons from heavy-flavour decays in Pb-Pb collisions at root s(NN)=2.76 TeV SO 14TH INTERNATIONAL CONFERENCE ON STRANGENESS IN QUARK MATTER (SQM2013) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 14th International Conference on Strangeness in Quark Matter (SQM) CY JUL 22-27, 2013 CL Univ Birmingham, Birmingham, ENGLAND HO Univ Birmingham AB We report on the latest results from ALICE on the measurement of the nuclear modification factor and elliptic flow of muons from heavy-flavour decays at forward rapidity in Pb-Pb collisions at root s(NN) = 2.76 TeV. A strong suppression of muons from heavy-flavour decays is observed at high transverse momentum, p(T), in the most central collisions compared to the binary-scaled expectation from pp events at the same energy, while a positive elliptic flow is observed at intermediate p(T) in semi-central collisions. Comparisons with model predictions are presented. C1 [Zhang, Xiaoming] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Zhang, XM (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, 1 Cyclotron Rd, Berkeley, CA 94720 USA. EM xmzhang@lbl.gov NR 16 TC 1 Z9 1 U1 0 U2 5 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 509 AR 012045 DI 10.1088/1742-6596/509/1/012045 PG 4 WC Astronomy & Astrophysics; Physics, Applied SC Astronomy & Astrophysics; Physics GA BA6OE UT WOS:000337194300045 ER PT S AU Klimov, VI AF Klimov, Victor I. BE Langer, JS TI Multicarrier Interactions in Semiconductor Nanocrystals in Relation to the Phenomena of Auger Recombination and Carrier Multiplication SO ANNUAL REVIEW OF CONDENSED MATTER PHYSICS, VOL 5 SE Annual Review of Condensed Matter Physics LA English DT Review; Book Chapter ID MULTIPLE EXCITON GENERATION; COLLOIDAL QUANTUM DOTS; LIGHT-EMITTING-DIODES; AMPLIFIED SPONTANEOUS EMISSION; EFFICIENCIES EXCEEDING UNITY; CORE-SHELL INTERFACE; SOLAR-CELLS; SILICON NANOCRYSTALS; CDSE NANOCRYSTALS; MULTIEXCITON GENERATION AB Chemically synthesized semiconductor nanocrystals (NCs) have been extensively studied as a test bed for exploring the physics of strong quantum confinement and as a highly flexible materials platform for the realization of a new generation of solution-processed optical, electronic, and optoelectronic devices. Because of readily tunable, size-dependent emission and absorption spectra, colloidal NCs are especially attractive for applications in light-emitting diodes, solid-state lighting, lasing, and solar cells. It is universally recognized that the realization of these and other prospective applications of NCs requires a detailed understanding of carrier-carrier interactions in these structures, as they have a strong effect on both recombination and photogeneration dynamics of charge carriers. For example, non-radiative Auger recombination is one of the key factors limiting the performance of NC-based lasers and light-emitting diodes. The inverse of this process, carrier multiplication, plays a beneficial role in light harvesting and can be used to boost the efficiency of photovoltaics through increased photocurrent. This article reviews recent progress in the understanding of multicarrier processes in NCs of various complexities, including zero-dimensional spherical quantum dots, quasi-one-dimensional nanorods, and various types of core-shell heterostructures. This review's specific focus is on recent efforts toward controlling multicarrier interactions using traditional approaches, such as size and shape control, as well as newly developed methods involving interface engineering for suppression of Auger decay and engineering of intraband cooling rates for enhancement of carrier multiplication. C1 Los Alamos Natl Lab, Div Chem, C PCS, Los Alamos, NM 87545 USA. RP Klimov, VI (reprint author), Los Alamos Natl Lab, Div Chem, C PCS, POB 1663, Los Alamos, NM 87545 USA. EM klimov@lanl.gov OI Klimov, Victor/0000-0003-1158-3179 NR 131 TC 43 Z9 43 U1 10 U2 92 PU ANNUAL REVIEWS PI PALO ALTO PA 4139 EL CAMINO WAY, PO BOX 10139, PALO ALTO, CA 94303-0897 USA SN 1947-5454 BN 978-0-8243-5005-5 J9 ANNU REV CONDEN MA P JI Annu. Rev. Condens. Matter Phys. PY 2014 VL 5 BP 285 EP 316 DI 10.1146/annurev-conmatphys-031113-133900 PG 32 WC Physics, Condensed Matter SC Physics GA BA6SI UT WOS:000337270800013 ER PT S AU Pokharel, R Lind, J Kanjarla, AK Lebensohn, RA Li, SF Kenesei, P Suter, RM Rollett, AD AF Pokharel, Reeju Lind, Jonathan Kanjarla, Anand K. Lebensohn, Ricardo A. Li, Shiu Fai Kenesei, Peter Suter, Robert M. Rollett, Anthony D. BE Langer, JS TI Polycrystal Plasticity: Comparison Between Grain-Scale Observations of Deformation and Simulations SO ANNUAL REVIEW OF CONDENSED MATTER PHYSICS, VOL 5 SE Annual Review of Condensed Matter Physics LA English DT Review; Book Chapter DE nf-HEDM; plastic deformation; microstructure; texture; micromechanical modeling ID ENERGY DIFFRACTION MICROSCOPY; X-RAY-DIFFRACTION; DISCRETE DISLOCATION PLASTICITY; FINITE-ELEMENT; SINGLE-CRYSTALS; TEXTURE DEVELOPMENT; INTRAGRANULAR BEHAVIOR; CONSTITUTIVE MODEL; LATTICE ROTATIONS; FCC POLYCRYSTALS AB The response of polycrystals to plastic deformation is studied at the level of variations within individual grains, and comparisons are made to theoretical calculations using crystal plasticity (CP). We provide a brief overview of CP and a review of the literature, which is dominated by surface observations. The motivating question asks how well CP represents the mesoscale behavior of large populations of dislocations (as carriers of plastic strain). The literature shows consistently that only moderate agreement is found between experiment and calculation. We supplement this with a current example of microstructure evolution in the interior of a copper sample subjected to tensile deformation. Nondestructive measurements of orientation fields were performed using the near-field highenergy X-ray diffraction microscopy (nf-HEDM) technique at the Advanced Photon Source (APS). Starting at highly ordered grains, a single two-dimensional slice of microstructure containing similar to 150 grains was followed through multiple strain states, where it tracked lattice rotations and defect accumulation of up to 14% elongation. In accord with the literature, at the scale of individual grains, comparison of observations with CP models indicates reasonable qualitative agreement but significant variations between simulation and experiment are apparent. The conclusion is that in order to be able to quantify the effects of microstructure on the distributions of slip, orientation change, and damage accumulation, the empirically derived constitutive relations used in continuum-scale simulations need to be improved. Equally important will be the development of large-scale simulations of polycrystals that directly model dislocations. C1 [Pokharel, Reeju; Li, Shiu Fai; Rollett, Anthony D.] Carnegie Mellon Univ, Dept Mat Sci & Engn, Pittsburgh, PA 15213 USA. [Lind, Jonathan; Suter, Robert M.] Carnegie Mellon Univ, Dept Phys, Pittsburgh, PA 15213 USA. [Li, Shiu Fai] Lawrence Livermore Natl Lab, Div Mat Sci & Engn, Livermore, CA 94550 USA. [Pokharel, Reeju; Kanjarla, Anand K.; Lebensohn, Ricardo A.] Los Alamos Natl Lab, Div Mat Sci & Technol, Los Alamos, NM 87544 USA. [Kenesei, Peter] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. [Kanjarla, Anand K.] IIT Madras, Dept Met & Mat Engn, Madras 60036, Tamil Nadu, India. RP Pokharel, R (reprint author), Carnegie Mellon Univ, Dept Mat Sci & Engn, Pittsburgh, PA 15213 USA. EM reeju@lanl.gov RI Lebensohn, Ricardo/A-2494-2008; Suter, Robert/P-2541-2014; Rollett, Anthony/A-4096-2012 OI Lebensohn, Ricardo/0000-0002-3152-9105; Suter, Robert/0000-0002-0651-0437; Rollett, Anthony/0000-0003-4445-2191 NR 117 TC 38 Z9 38 U1 8 U2 52 PU ANNUAL REVIEWS PI PALO ALTO PA 4139 EL CAMINO WAY, PO BOX 10139, PALO ALTO, CA 94303-0897 USA SN 1947-5454 BN 978-0-8243-5005-5 J9 ANNU REV CONDEN MA P JI Annu. Rev. Condens. Matter Phys. PY 2014 VL 5 BP 317 EP 346 DI 10.1146/annurev-conmatphys-031113-133846 PG 30 WC Physics, Condensed Matter SC Physics GA BA6SI UT WOS:000337270800014 ER PT S AU Armijo, LM Kopciuch, M Olszowka, Z Wawrzyniec, SJ Rivera, AC Plumley, JB Cook, NC Brandt, YI Huber, DL Smolyakov, GA Adolphi, NL Smyth, HDC Osinski, M AF Armijo, Leisha M. Kopciuch, Michael Olszowka, Zuzia Wawrzyniec, Stephen J. Rivera, Antonio C. Plumley, John B. Cook, Nathaniel C. Brandt, Yekaterina I. Huber, Dale L. Smolyakov, Gennady A. Adolphi, Natalie L. Smyth, Hugh D. C. Osinski, Marek BE Parak, WJ Osinski, M Yamamoto, KI TI Delivery of antibiotics coupled to iron oxide nanoparticles across the biofilm of mucoid Pseudonomas aeruginosa and investigation of their efficacy SO COLLOIDAL NANOPARTICLES FOR BIOMEDICAL APPLICATIONS IX SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Colloidal Nanoparticles for Biomedical Applications IX CY FEB 01-04, 2014 CL San Francisco, CA SP SPIE DE Nanoparticles; Fe3O4; magnetite; ferrofluid; drug delivery; antibiotic; Pseudomonas aeruginosa; biofilm; antibiotic sensitivities ID BIOMEDICAL APPLICATIONS; PSEUDOMONAS-AERUGINOSA; MAGNETIC NANOPARTICLES; CYSTIC-FIBROSIS; IN-VIVO; NANOCRYSTALS; HYPERTHERMIA; THERMOTHERAPY AB Pseudomonas aeruginosa bacterium is a deadly pathogen, leading to respiratory failure in cystic fibrosis and nosocomial pneumonia, and responsible for high mortality rates in these diseases. P. aeruginosa has inherent as well as acquired resistance to many drug classes. In this paper, we investigate the effectiveness of two classes; aminoglycoside (tobramycin) and fluoroquinolone (ciprofloxacin) administered alone, as well as conjugated to iron oxide (magnetite) nanoparticles. P. aeruginosa possesses the ability to quickly alter its genetics to impart resistance to the presence of new, unrecognized treatments. As a response to this impending public health threat, we have synthesized and characterized magnetite nanoparticles capped with biodegradable short-chain carboxylic acid derivatives conjugated to common antibiotic drugs. The functionalized nanoparticles may carry the drug past the mucus and biofilm layers to target the bacterial colonies via magnetic gradient-guided transport. Additionally, the magnetic ferrofluid may be used under application of an oscillating magnetic field to raise the local temperature, causing biofilm disruption, slowed growth, and mechanical disruption. These abilities of the ferrofluid would also treat multi-drug resistant strains, which appear to be increasing in many nosocomial as well as acquired opportunistic infections. In this in vitro model, we show that the iron oxide alone can also inhibit bacterial growth and biofilm formation. C1 [Armijo, Leisha M.; Kopciuch, Michael; Olszowka, Zuzia; Wawrzyniec, Stephen J.; Rivera, Antonio C.; Plumley, John B.; Cook, Nathaniel C.; Brandt, Yekaterina I.; Smolyakov, Gennady A.; Osinski, Marek] Univ New Mexico, Ctr High Technol Mat, 1313 Goddard SE, Albuquerque, NM 87106 USA. [Olszowka, Zuzia] Albuquerque Inst Math & Sci, Albuquerque, NM 87106 USA. [Huber, Dale L.] Sandia Natl Labs, Ctr Integrated Nanotechnol, Albuquerque, NM 87123 USA. [Adolphi, Natalie L.] Univ New Mexico Hlth Sci Ctr, Dept Biochem & Mol Biol, Albuquerque, NM 87131 USA. [Smyth, Hugh D. C.] Univ Texas, Coll Pharm, Austin, TX 78712 USA. [Osinski, Marek] Univ Carlos III Madrid, Dept Tecnologia Elect, On leave Grupo Optoelectron Tecnologia Laser GOTL, Madrid, Spain. RP Armijo, LM (reprint author), Univ New Mexico, Ctr High Technol Mat, 1313 Goddard SE, Albuquerque, NM 87106 USA. RI Parak, Wolfgang J./M-3998-2014; Huber, Dale/A-6006-2008 OI Parak, Wolfgang J./0000-0003-1672-6650; Huber, Dale/0000-0001-6872-8469 FU NIH [1R21HL092812- 01A1, 060201]; Nano- Pullies for Enhanced Drug Delivery to the Lung; NSF IGERT program on " Integrating Nanotechnology with Cell Biology and Neuroscience [DGE- 0549500]; CINT/ SNL [U2010B1079]; DoE [DE- AC04- 94AL85000] FX This work was supported by NIH under the Grant No. 1R21HL092812- 01A1 " Multifunctional Nanoparticles: Nano- Knives and Nano- Pullies for Enhanced Drug Delivery to the Lung", by NIH under the Grant No. GM- 060201 " Initiatives to Maximize Student Diversity", and by the NSF IGERT program on " Integrating Nanotechnology with Cell Biology and Neuroscience", Grant No. DGE- 0549500. This work was performed in part at CINT/ SNL under Project No. U2010B1079 " Characterization of Multifunctional Nanoparticles for Enhanced Drug Delivery to the Lung", funded by DoE contract No. DE- AC04- 94AL85000. NR 36 TC 0 Z9 0 U1 3 U2 10 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9868-7 J9 PROC SPIE PY 2014 VL 8955 AR UNSP 89550I DI 10.1117/12.2043340 PG 12 WC Engineering, Biomedical; Nanoscience & Nanotechnology; Optics SC Engineering; Science & Technology - Other Topics; Optics GA BA6UN UT WOS:000337284100008 ER PT J AU Ozdol, VB Tyutyunnikov, D Koch, CT van Aken, PA AF Oezdoel, V. B. Tyutyunnikov, D. Koch, C. T. van Aken, P. A. TI Strain mapping for advanced CMOS technologies SO CRYSTAL RESEARCH AND TECHNOLOGY LA English DT Article; Proceedings Paper CT 21st Annual Meeting of the German-Crystallographic-Society CY MAR 19-22, 2013 CL Freiberg, GERMANY DE Strain mapping; Dark-field inline electron holography; Strain-engineering; CMOS ID ALGORITHM AB The ability to measure strain quantitatively has become an important tool for characterizing strain-engineered CMOS devices. We report on nanometer scale strain measurements performed on off-the-shelf 32-nm node device structures. We show that the two-dimensional deformation tensor in NMOS channels can be mapped using high resolution transmission electron microscopy. We also demonstrate the application of our recently developed dark-field inline holography technique on an array of PMOS transistors, showing that this technique is capable of combining a large field of view of 1 micrometer with a spatial resolution better than 1 nm, and very high precision (around 10(-4)). Also, the experimental requirements for implementing this technique are easily met on most modern TEMs, without any modification to the hardware or alignment of the microscope. C1 [Oezdoel, V. B.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Natl Ctr Electron Microscopy, Berkeley, CA 94720 USA. [Tyutyunnikov, D.; van Aken, P. A.] Max Planck Inst Intelligent Syst, Stuttgart Ctr Electron Microscopy, D-70569 Stuttgart, Germany. [Koch, C. T.] Univ Ulm, Inst Expt Phys, D-89081 Ulm, Germany. RP van Aken, PA (reprint author), Max Planck Inst Intelligent Syst, Stuttgart Ctr Electron Microscopy, D-70569 Stuttgart, Germany. EM vanaken@is.mpg.de RI Koch, Christoph/E-9689-2011; Foundry, Molecular/G-9968-2014 OI Koch, Christoph/0000-0002-3984-1523; FU Carl Zeiss Foundation; German Research Foundation (DFG) [KO2911/7-1]; European Union [312483] FX CTK acknowledges the Carl Zeiss Foundation as well as the German Research Foundation (DFG, grant nr. KO2911/7-1). The research leading to these results has received funding from the European Union Seventh Framework Programme [FP7/2007-2013] under grant agreement no 312483 (ESTEEM2). NR 15 TC 1 Z9 1 U1 2 U2 21 PU WILEY-V C H VERLAG GMBH PI WEINHEIM PA POSTFACH 101161, 69451 WEINHEIM, GERMANY SN 0232-1300 EI 1521-4079 J9 CRYST RES TECHNOL JI Cryst. Res. Technol. PD JAN PY 2014 VL 49 IS 1 BP 38 EP 42 DI 10.1002/crat.201300226 PG 5 WC Crystallography SC Crystallography GA AI9XA UT WOS:000337297500007 ER PT J AU Wolfson, O Xu, B AF Wolfson, Ouri Xu, Bo TI A New Paradigm for Querying Blobs in Vehicular Networks SO IEEE MULTIMEDIA LA English DT Article ID DISSEMINATION AB A novel paradigm and several derived strategies that query binary large objects in a wireless vehicular network reveal the answer throughput and communication overhead of various approaches. C1 [Wolfson, Ouri] Univ Illinois, Chicago, IL 60680 USA. [Wolfson, Ouri] Univ Illinois, Urbana, IL USA. [Xu, Bo] Argonne Natl Lab, Res & Anal Comp Ctr, Argonne, IL 60439 USA. [Xu, Bo] Univ Illinois, Dept Comp Sci, Chicago, IL 60680 USA. RP Wolfson, O (reprint author), Univ Illinois, Chicago, IL 60680 USA. EM wolfson@cs.uic.edu; boxu08@gmail.com FU US Department of Transportation National University Rail Center (NURAIL); Illinois Department of Transportation (METSI); National Science Foundation [IIS-1213013, CCF-1216096, DGE-0549489, IIP-1315169] FX This research was supported in part by the US Department of Transportation National University Rail Center (NURAIL); Illinois Department of Transportation (METSI); and National Science Foundation grants IIS-1213013, CCF-1216096, DGE-0549489, and IIP-1315169. NR 15 TC 2 Z9 2 U1 0 U2 0 PU IEEE COMPUTER SOC PI LOS ALAMITOS PA 10662 LOS VAQUEROS CIRCLE, PO BOX 3014, LOS ALAMITOS, CA 90720-1314 USA SN 1070-986X EI 1941-0166 J9 IEEE MULTIMEDIA JI IEEE Multimedia PD JAN-MAR PY 2014 VL 21 IS 1 BP 48 EP 58 PG 11 WC Computer Science, Hardware & Architecture; Computer Science, Information Systems; Computer Science, Software Engineering; Computer Science, Theory & Methods SC Computer Science GA AI8LU UT WOS:000337168200008 ER PT J AU Bae, WK Lim, J Zorn, M Kwak, J Park, YS Lee, D Lee, S Char, K Zentel, R Lee, C AF Bae, Wan Ki Lim, Jaehoon Zorn, Matthias Kwak, Jeonghun Park, Young-Shin Lee, Donggu Lee, Seonghoon Char, Kookheon Zentel, Rudolf Lee, Changhee TI Reduced efficiency roll-off in light-emitting diodes enabled by quantum dot-conducting polymer nanohybrids SO JOURNAL OF MATERIALS CHEMISTRY C LA English DT Article ID NANOCRYSTAL SOLIDS; CHARGE INJECTION; DEVICES; LAYERS AB We demonstrate QLEDs implementing wider active layers (50 nm) based on QD-conducting polymer nanohybrids, which exhibit a stable operational device performance across a wide range of current densities and brightness. A comparative study reveals that the significant suppression of efficiency roll-off in the high current density regime is primarily attributed to a sufficient charge carrier distribution over the wider active layer and improved charge carrier balance within QDs enabled by the hybridization of QDs with conducting polymers. Utilization of this finding in future studies should greatly facilitate the development of high performance, stable QLEDs at high current density or luminance regime toward displays or solid-state lighting applications. C1 [Bae, Wan Ki] Korea Inst Sci & Technol, Natl Agenda Agenda Res Div, Photoelect Hybrids Res Ctr, Seoul 136791, South Korea. [Lim, Jaehoon; Park, Young-Shin] Los Alamos Natl Lab, Div Chem, Los Alamos, NM 87544 USA. [Zorn, Matthias; Lee, Donggu; Zentel, Rudolf] Johannes Gutenberg Univ Mainz, Inst Organ Chem, D-55099 Mainz, Germany. [Kwak, Jeonghun] Dong A Univ, Dept Elect Engn, Pusan 604714, South Korea. [Lee, Changhee] Seoul Natl Univ, ISRC, Dept Elect Engn & Comp Sci, Seoul 151742, South Korea. [Lee, Seonghoon] Seoul Natl Univ, Dept Chem, Seoul 151742, South Korea. [Char, Kookheon] Seoul Natl Univ, Natl Creat Res Initiat Ctr Intelligent Hybrids, Sch Chem & Biol Engn, Seoul 151742, South Korea. RP Zentel, R (reprint author), Johannes Gutenberg Univ Mainz, Inst Organ Chem, Duesbergweg 10-14, D-55099 Mainz, Germany. EM khchar@plaza.snu.ac.kr; zentel@uni-mainz.de; chlee7@snu.ac.kr RI Kwak, Jeonghun/C-6191-2009; Lee, Changhee/A-2471-2009; Zentel, Rudolf/D-4542-2011; OI Kwak, Jeonghun/0000-0002-4037-8687; Lee, Changhee/0000-0003-2800-8250; Park, Young-Shin/0000-0003-4204-1305 FU KIST internal project [2E24821]; National Research Foundation of Korea (NRF) - Korea Ministry of Education, Science, and Technology (MEST) through the National Creative Research Initiative Center for Intelligent Hybrids [2010-0018290]; Technology Development Program to Solve Climate Changes [NRF-2009C1AAA001-2009-0093282]; Industrial Strategic Technology Development Program [10045145]; International Research Training Group: Self Organized Materials for Optoelectronics; DFG (Germany); NRF (Korea) FX This research was financially supported by KIST internal project (2E24821). This work was also financially supported by the National Research Foundation of Korea (NRF) funded by the Korea Ministry of Education, Science, and Technology (MEST) through the National Creative Research Initiative Center for Intelligent Hybrids (no. 2010-0018290), and Technology Development Program to Solve Climate Changes (no. NRF-2009C1AAA001-2009-0093282). This work was also supported by the Industrial Strategic Technology Development Program (10045145, Development of high performance chalcogenide TFT backplane and cadmium-free highly efficient hybrid EL material/devices). This work was in part supported by the International Research Training Group: Self Organized Materials for Optoelectronics, jointly supported by the DFG (Germany) and NRF (Korea). NR 24 TC 10 Z9 11 U1 1 U2 35 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 2014 VL 2 IS 25 BP 4974 EP 4979 DI 10.1039/c4tc00232f PG 6 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA AI8BP UT WOS:000337129700010 ER PT J AU Grahame, TJ Klemm, R Schlesinger, RB AF Grahame, Thomas J. Klemm, Rebecca Schlesinger, Richard B. TI Public health and components of particulate matter: The changing assessment of black carbon SO JOURNAL OF THE AIR & WASTE MANAGEMENT ASSOCIATION LA English DT Review ID DIESEL EXHAUST PARTICLES; POLYCYCLIC AROMATIC-HYDROCARBONS; CORONARY-HEART-DISEASE; INDOOR AIR-POLLUTION; LONG-TERM EXPOSURE; WOOD SMOKE EXPOSURE; IMPAIRED ENDOGENOUS FIBRINOLYSIS; CONCENTRATED AMBIENT PARTICLES; ENDOTHELIAL GROWTH-FACTOR; INDUCE OXIDATIVE STRESS AB In 2012, the WHO classified diesel emissions as carcinogenic, and its European branch suggested creating a public health standard for airborne black carbon (BC). In 2011, EU researchers found that life expectancy could be extended four to nine times by reducing a unit of BC, vs reducing a unit of PM2.5. Only recently could such determinations be made. Steady improvements in research methodologies now enable such judgments.In this Critical Review, we survey epidemiological and toxicological literature regarding carbonaceous combustion emissions, as research methodologies improved over time. Initially, we focus on studies of BC, diesel, and traffic emissions in the Western countries (where daily urban BC emissions are mainly from diesels). We examine effects of other carbonaceous emissions, e.g., residential burning of biomass and coal without controls, mainly in developing countries.Throughout the 1990s, air pollution epidemiology studies rarely included species not routinely monitored. As additional PM2.5. chemical species, including carbonaceous species, became more widely available after 1999, they were gradually included in epidemiological studies. Pollutant species concentrations which more accurately reflected subject exposure also improved models.Natural interventions - reductions in emissions concurrent with fuel changes or increased combustion efficiency; introduction of ventilation in highway tunnels; implementation of electronic toll payment systems - demonstrated health benefits of reducing specific carbon emissions. Toxicology studies provided plausible biological mechanisms by which different PM species, e.g., carbonaceous species, may cause harm, aiding interpretation of epidemiological studies.Our review finds that BC from various sources appears to be causally involved in all-cause, lung cancer, and cardiovascular mortality, morbidity, and perhaps adverse birth and nervous system effects. We recommend that the U.S. EPA rubric for judging possible causality of PM2.5. mass concentrations, be used to assess which PM2.5. species are most harmful to public health.Implications: Black carbon (BC) and correlated co-emissions appear causally related with all-cause, cardiovascular, and lung cancer mortality, and perhaps with adverse birth outcomes and central nervous system effects. Such findings are recent, since widespread monitoring for BC is also recent. Helpful epidemiological advances (using many health relevant PM2.5 species in models; using better measurements of subject exposure) have also occurred. Natural intervention studies also demonstrate harm from partly combusted carbonaceous emissions. Toxicology studies consistently find biological mechanisms explaining how such emissions can cause these adverse outcomes. A consistent mechanism for judging causality for different PM2.5 species is suggested.A list of acronyms will be found at the end of the article. C1 [Grahame, Thomas J.] US DOE, Washington, DC 20585 USA. [Klemm, Rebecca] Klemm Anal Grp, Washington, DC USA. [Schlesinger, Richard B.] Pace Univ, Dept Biol & Hlth Sci, New York, NY USA. RP Grahame, TJ (reprint author), US DOE, Room 4G 036,1000 Independence Ave,SW, Washington, DC 20585 USA. EM thomas.grahame@hq.doe.gov NR 311 TC 41 Z9 41 U1 108 U2 242 PU TAYLOR & FRANCIS INC PI PHILADELPHIA PA 530 CHESTNUT STREET, STE 850, PHILADELPHIA, PA 19106 USA SN 1096-2247 EI 2162-2906 J9 J AIR WASTE MANAGE JI J. Air Waste Manage. Assoc. PY 2014 VL 64 IS 6 BP 620 EP 660 DI 10.1080/10962247.2014.912692 PG 41 WC Engineering, Environmental; Environmental Sciences; Meteorology & Atmospheric Sciences SC Engineering; Environmental Sciences & Ecology; Meteorology & Atmospheric Sciences GA AI9IV UT WOS:000337247200002 PM 25039199 ER PT S AU Demos, SG Urayama, S AF Demos, Stavros G. Urayama, Shiro BE Alfano, RR Demos, SG TI Enhanced visualization of the Bile Duct via parallel white light and indocyanine green fluorescence laparoscopic imaging SO OPTICAL BIOPSY XII SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Optical Biopsy XII CY FEB 04-05, 2014 CL San Francisco, CA SP SPIE, BaySpec Inc, Energy Res Co, Hamamatsu Corp, PerkinElmer Inc, Intuit Surg, Inc, Coherent Inc, Corning Inc, Fianium Ltd, LEUKOS, NKT Photon A S, ThorLabs Inc DE Laparoscopic imaging; fluorescence endoscopic imaging; laparoscopic cholecystectomy; ICG ID CHOLANGIOGRAPHY; CHOLECYSTECTOMY AB Despite best efforts, bile duct injury during laparoscopic cholecystectomy is a major potential complication. Precise detection method of extrahepatic bile duct during laparoscopic procedures would minimize the risk of injury. Towards this goal, we have developed a compact imaging instrumentation designed to enable simultaneous acquisition of conventional white color and NIR fluorescence endoscopic/laparoscopic imaging using ICG as contrast agent. The capabilities of this system, which offers optimized sensitivity and functionality, are demonstrated for the detection of the bile duct in an animal model. This design could also provide a low-cost real-time surgical navigation capability to enhance the efficacy of a variety of other image-guided minimally invasive procedures. C1 [Demos, Stavros G.] Lawrence Livermore Natl Lab, 7000 East Ave, Livermore, CA 94550 USA. [Urayama, Shiro] Calif State Univ Sacramento, Davis Med Ctr, Div Gastroenterol & Hepatol, Sacramento, CA 95817 USA. RP Demos, SG (reprint author), Lawrence Livermore Natl Lab, 7000 East Ave, Livermore, CA 94550 USA. FU Battelle Memorial Institute and the Center for Biophotonics; NSF Science and Technology Center; University of California Davis [PHY 0120999]; Division of Gastroenterology and Hepatology, University of California, Davis; U. S. Department of Energy; Lawrence Livermore National Laboratory [DE-AC52-07NA27344] FX This research was supported in part by funding from the Battelle Memorial Institute and the Center for Biophotonics, an NSF Science and Technology Center, is managed by the University of California, Davis, under Cooperative Agreement No. PHY 0120999. Additional support provided from Division of Gastroenterology and Hepatology, University of California, Davis (for S. U.). This work was performed in part under the auspices of the U. S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344. NR 6 TC 0 Z9 0 U1 0 U2 2 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9853-3 J9 PROC SPIE PY 2014 VL 8940 AR UNSP 89400R DI 10.1117/12.2044271 PG 6 WC Oncology; Optics; Radiology, Nuclear Medicine & Medical Imaging SC Oncology; Optics; Radiology, Nuclear Medicine & Medical Imaging GA BA6GZ UT WOS:000337140700013 ER PT S AU Wang, LP AF Wang, Liping BE Li, A Zhu, Y Li, Y TI Window Operation and Its Impacts on Thermal Comfort and Energy Use SO PROCEEDINGS OF THE 8TH INTERNATIONAL SYMPOSIUM ON HEATING, VENTILATION AND AIR CONDITIONING, VOL 2: HVAC&R COMPONENT AND ENERGY SYSTEM SE Lecture Notes in Electrical Engineering LA English DT Proceedings Paper CT 8th International Symposium on Heating, Ventilation, and Air Conditioning (ISHVAC) CY OCT 19-21, 2013 CL Xian, PEOPLES R CHINA SP Xian Univ Architecture & Technol, Tsinghua Univ, Univ Hong Kong DE Natural ventilation; Mixed mode; Window operation; Energy; Thermal comfort ID HYBRID VENTILATION AB Operable windows provide occupants' ability to control over local environment and satisfy human's expectation to access to outdoor environment. Operation strategies for operable windows can have significant impacts on indoor thermal comfort and energy consumption of building performance. It is not uncommon that building facility managers complain that operable windows were left open in buildings with a conventional HVAC system. However, optimum control strategies of window operation can improve thermal comfort and reduce energy consumption for building using natural ventilation or mixed mode ventilation. The study focuses on the investigation of the impacts of window operations on building performance for different types of building systems including natural ventilation, mixed mode ventilation, and conventional HVAC systems in a medium-size reference office building. Building performance simulation tool EnergyPlus is used to simulate window operations for each system in three different climates. Various control strategies of window operations for building operation systems, implemented using (EMS) in EnergyPlus, are evaluated based on the criteria of thermal comfort and energy consumption. The results highlight the impacts of window operations on thermal comfort and energy use and identify that hybrid ventilation for perimeter zones has 12-20 % saving potentials of annual HVAC site energy consumption. C1 Lawrence Berkeley Natl Lab, Berkeley, CA 94706 USA. RP Wang, LP (reprint author), Lawrence Berkeley Natl Lab, 1 Cyclotron Rd,Bldg 90,MS90-3145, Berkeley, CA 94706 USA. EM lwang@lbl.gov NR 6 TC 0 Z9 0 U1 0 U2 3 PU SPRINGER-VERLAG BERLIN PI BERLIN PA HEIDELBERGER PLATZ 3, D-14197 BERLIN, GERMANY SN 1876-1100 BN 978-3-642-39581-9; 978-3-642-39580-2 J9 LECT NOTES ELECTR EN PY 2014 VL 262 BP 259 EP 266 DI 10.1007/978-3-642-39581-9_26 PG 8 WC Construction & Building Technology; Energy & Fuels SC Construction & Building Technology; Energy & Fuels GA BA6IC UT WOS:000337148000026 ER PT J AU Nakagawa, T Burrell, AK Del Sesto, RE Janicke, MT Nekimken, AL Purdy, GM Paik, B Zhong, RQ Semelsberger, TA Davis, BL AF Nakagawa, Tessui Burrell, Anthony K. Del Sesto, Rico E. Janicke, Michael T. Nekimken, Adam L. Purdy, Geraldine M. Paik, Biswajit Zhong, Rui-Qin Semelsberger, Troy A. Davis, Benjamin L. TI Physical, structural, and dehydrogenation properties of ammonia borane in ionic liquids SO RSC ADVANCES LA English DT Article ID HYDROGEN STORAGE MATERIAL; THERMAL-DECOMPOSITION; IMIDAZOLIUM; AMIDOTRIHYDROBORATE; CATALYSTS; RELEASE AB Ionic liquids (ILs) are excellent solvents for the dehydrogenation of ammonia borane (AB); however, the basic properties that allow efficient dehydrogenation are still unclear. In this report, density, viscosity, melting/freezing/glass transition temperature, solubility, and the dehydrogenation properties, including impurity gas quantification, of AB-imidazolium-based IL solutions were studied. Note that ILs can solubilize 32-35 wt% of AB, and the liquid AB-IL solutions have densities of similar to 0.9 g cm(-3), viscosities similar to motor oil (100-250 cP), and glass transition temperatures below -50 degrees C. AB-ILs are stable at room temperature for several weeks with minimal hydrogen generation, although some hydrolysis occurs immediately upon mixing as a result of trace water content. Between 80 and 130 degrees C, more than 2 mol H-2/AB are desorbed from AB-ILs with limited impurity emissions. Furthermore, there is no reaction between AB and ILs upon dehydrogenation, and structural analysis reveals a complex solid solution. C1 [Nakagawa, Tessui; Burrell, Anthony K.; Del Sesto, Rico E.; Purdy, Geraldine M.; Paik, Biswajit; Zhong, Rui-Qin; Semelsberger, Troy A.; Davis, Benjamin L.] Los Alamos Natl Lab, Mat Phys & Applicat Div, Los Alamos, NM 87544 USA. [Janicke, Michael T.] Los Alamos Natl Lab, Div Chem, Los Alamos, NM 87545 USA. [Nekimken, Adam L.] Stanford Univ, Dept Mech Engn, Stanford, CA 94305 USA. RP Nakagawa, T (reprint author), Univ Ryukyus, Fac Sci, 1 Senbaru, Nishihara, Okinawa 9030213, Japan. EM tessui@sci.u-ryukyu.ac.jp; bldavis@lanl.gov RI Paik, Biswajit/A-5943-2010; Davis, Benjamin /I-7897-2015; OI Davis, Benjamin/0000-0001-5439-0751; Janicke, Michael/0000-0002-3139-2882 FU DOE office of EERE (Energy Efficiency and Renewable Energy) [NA25396, DE-EE-0005658] FX This work was supported by the DOE office of EERE (Energy Efficiency and Renewable Energy) under contract numbers NA25396 and DE-EE-0005658. NR 33 TC 6 Z9 6 U1 4 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 2014 VL 4 IS 42 BP 21681 EP 21687 DI 10.1039/c4ra01455c PG 7 WC Chemistry, Multidisciplinary SC Chemistry GA AI8AB UT WOS:000337123100002 ER PT J AU Baggetto, L Mohanty, D Meisner, RA Bridges, CA Daniel, C Wood, DL Dudney, NJ Veith, GM AF Baggetto, Loic Mohanty, Debasish Meisner, Roberta A. Bridges, Craig A. Daniel, Claus Wood, David L., III Dudney, Nancy J. Veith, Gabriel M. TI Degradation mechanisms of lithium-rich nickel manganese cobalt oxide cathode thin films SO RSC ADVANCES LA English DT Article ID X-RAY-DIFFRACTION; LI-ION BATTERIES; COMPOSITION LI1.2MN0.525NI0.175CO0.1O2; PHOTOELECTRON-SPECTROSCOPY; XPS SPECTRA; MN; NI; ELECTRODES; TRANSFORMATION; PERFORMANCE AB This paper reports a method to prepare Li-rich NMC (Li1.2Mn0.55Ni0.15Co0.1O2) thin film cathodes for Li-ion batteries using RF magnetron sputtering and post-annealing in O-2. Thin film cathodes with high reversible capacities (260 mA h g(-1)) and potential profiles similar to those of the powder material have been obtained. Structural and electrochemical studies show that the grown materials consist of a layered structure with trigonal symmetry in which Li/TM ordering is partially achieved. Using XPS we determine that the surface is comprised of Mn4+, Co3+ and Ni2+ cations inside an O2- framework. The loss mechanisms of these electrodes have been studied after 184 cycles. The data after cycling shows the absence of Li/TM ordering, confirming that Li2MnO3 activation is irreversible, while electron diffraction data indicates extensive structural modifications upon cycling. In addition, we identified that the surface chemistry is dominated by inorganic species (LiF, Lix'POy'Fz', LixPFy), along with small amounts of organic species with C-O and O-C=O groups such as PEO, LiOR and RCO2Li. Moreover, XPS results indicate that Ni and Co migrate into the bulk while the reduction of Mn4+ into Mn3+ is clearly evidenced, as expected from the activation of Li2MnO3 domains and discharging to 2.5 V. C1 [Baggetto, Loic; Mohanty, Debasish; Meisner, Roberta A.; Dudney, Nancy J.; Veith, Gabriel M.] Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. [Bridges, Craig A.] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. [Daniel, Claus; Wood, David L., III] Oak Ridge Natl Lab, Energy & Transportat Sci Div, Oak Ridge, TN 37831 USA. [Daniel, Claus] Univ Tennessee, Bredesen Ctr Interdisciplinary Res & Grad Educ, Knoxville, TN 37996 USA. RP Baggetto, L (reprint author), Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. EM loic_baggetto@yahoo.fr; veithgm@ornl.gov RI Daniel, Claus/A-2060-2008; Dudney, Nancy/I-6361-2016; Baggetto, Loic/D-5542-2017; OI Daniel, Claus/0000-0002-0571-6054; Dudney, Nancy/0000-0001-7729-6178; Baggetto, Loic/0000-0002-9029-2363; Wood, David/0000-0002-2471-4214 FU U.S. Department of Energy (DOE); Basic Energy Sciences (BES); Materials Sciences and Engineering Division; Vehicle Technologies Office of the Office of Energy Efficiency and Renewable Energy at the U.S. Department of Energy; ORNL's Shared Research Equipment (ShaRE) User Program - DOE-BES FX Dr Daniel Abraham, ANL, is thankfully acknowledged for providing the powder material. Drs Sergiy Kalnaus and Lynn Trahey are gratefully acknowledged for fruitful discussions. This work was support by the U.S. Department of Energy (DOE), Basic Energy Sciences (BES), Materials Sciences and Engineering Division (LB, GMV, NJD - Synthesis, XRD, electrochemistry, XPS) and by the Vehicle Technologies Office (program managers Peter Faguy and David Howell) of the Office of Energy Efficiency and Renewable Energy at the U.S. Department of Energy (DM, CD, RAM, DLW - XRD, Microscopy). Microscopy research was supported via a user project supported by ORNL's Shared Research Equipment (ShaRE) User Program, which is also supported by DOE-BES. NR 38 TC 10 Z9 10 U1 7 U2 84 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 2014 VL 4 IS 45 BP 23364 EP 23371 DI 10.1039/c4ra03674c PG 8 WC Chemistry, Multidisciplinary SC Chemistry GA AI8FT UT WOS:000337145900002 ER PT J AU Nelson, KM Qiao, ZA Mahurin, SM Mayes, RT Bridges, CA Dai, S AF Nelson, Kimberly M. Qiao, Zhen-An Mahurin, Shannon M. Mayes, Richard T. Bridges, Craig A. Dai, Sheng TI A non-micellar synthesis of mesoporous carbon via spinodal decomposition SO RSC ADVANCES LA English DT Article ID MOLECULAR-SIEVES; PHASE-SEPARATION; ADSORPTION; TRANSFORMATION; TEMPERATURE; POLYMERS; RESIN AB Mesoporous carbons were prepared via spinodal decomposition of non-amphiphilic linear polyethylene glycol with phloroglucinol-formaldehyde resin under refluxing acidic ethanol conditions. By shifting the molecular weight and the concentration of polyethylene glycol, both mesopore size and volume can be tuned. C1 [Nelson, Kimberly M.; Dai, Sheng] Univ Tennessee, Dept Chem, Knoxville, TN 37996 USA. [Qiao, Zhen-An; Mahurin, Shannon M.; Mayes, Richard T.; Bridges, Craig A.; Dai, Sheng] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. RP Dai, S (reprint author), Univ Tennessee, Dept Chem, Knoxville, TN 37996 USA. EM dais@orl.gov RI Dai, Sheng/K-8411-2015; OI Dai, Sheng/0000-0002-8046-3931; Mayes, Richard/0000-0002-7457-3261; Qiao, Zhen-An/0000-0001-6064-9360 FU Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy FX This work was fully sponsored by the Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy. NR 29 TC 2 Z9 2 U1 1 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 2014 VL 4 IS 45 BP 23703 EP 23706 DI 10.1039/c4ra03558e PG 4 WC Chemistry, Multidisciplinary SC Chemistry GA AI8FT UT WOS:000337145900045 ER PT S AU Atanassova, ID Doerr, SH Mills, GL AF Atanassova, Irena D. Doerr, Stefan H. Mills, Gary L. BE Hartemink, AE McSweeney, K TI Hot-Water-Soluble Organic Compounds Related to Hydrophobicity in Sandy Soils SO SOIL CARBON SE Progress in Soil Science LA English DT Proceedings Paper CT International-Union-of-Soil-Sciences Global Soil Carbon Conference CY JUN 03-06, 2013 CL Madison, WI SP Int Union Soil Sci, Univ Wisconsin, Coll Agr & Life Sci, Dept Soil Sci ID CHEMICAL-COMPOSITION; FOREST SOIL; HUMIC-ACID; MATTER; REPELLENCY; SORPTION; CARBON AB Soil water repellency (WR) reduces mineralization of soil organic matter (SOM) and has the potential to sequester soil carbon. However, predicted climate change events such as decreased rainfall and droughts can cause changes in WR influencing water storage and plant productivity. Hot-water-soluble carbon (HWSC) is a sensitive indicator of ecosystem changes. It contains binding agents influencing soil aggregate stability, which is mainly controlled by soil WR levels. Here we characterize the link between WR and the organic compounds composition in hot water extracts from accelerated solvent extraction (ASE) of sandy soils. Extracts were lyophilized, fractionated and measured by GC/MS. Dominant compounds were phenolic acids, short chain dicarboxylic acids (C-4-C-9), saccharides, glycosides, (C-8-C-18) fatty acids, and esters of oleic, stearic and palmitic acids. We speculate that the complete elimination of WR by hot water was due to: (i) critical quantity of HWSC extracted, necessary to disaggregate soil particles; (ii) removal of sugars and aromatics; (iii) removal of hydrophobic fatty acid esters (C-16 and C-18); (iv) enhanced desorption of complex DOC fractions in water at high T and pressure; (v) exposure of greater proportion of hydrophilic sites. The polarity and aromaticity of HWSC can play a critical role in stabilization and destabilization of soil organic matter (SOM), particle wettability and C dynamics in soils. C1 [Atanassova, Irena D.] N Poushkarov Inst Soil Sci Agrotechnol & Plant Pr, 7 Shosse Bankya, Sofia 1080, Bulgaria. [Atanassova, Irena D.; Mills, Gary L.] Univ Georgia, Savannah River Ecol Lab, Aiken, SC 29802 USA. [Doerr, Stefan H.] Swansea Univ, Inst Environm Sustainabil, Swansea SA2 8PP, W Glam, Wales. RP Atanassova, ID (reprint author), N Poushkarov Inst Soil Sci Agrotechnol & Plant Pr, 7 Shosse Bankya, Sofia 1080, Bulgaria. EM i.d.atanassova@abv.bg RI Doerr, Stefan/G-5456-2012 OI Doerr, Stefan/0000-0002-8700-9002 NR 21 TC 0 Z9 0 U1 0 U2 9 PU SPRINGER PI DORDRECHT PA PO BOX 17, 3300 AA DORDRECHT, NETHERLANDS SN 2352-4774 BN 978-3-319-04084-4; 978-3-319-04083-7 J9 PROGR SOIL SCI PY 2014 BP 137 EP 146 DI 10.1007/978-3-319-04084-4_14 PG 10 WC Soil Science SC Agriculture GA BA6KO UT WOS:000337169400016 ER PT B AU Sanford, GR AF Sanford, Gregg R. BE Hartemink, AE McSweeney, K TI Perennial Grasslands Are Essential for Long Term SOC Storage in the Mollisols of the North Central USA SO SOIL CARBON SE Progress in Soil Science LA English DT Proceedings Paper CT International-Union-of-Soil-Sciences Global Soil Carbon Conference CY JUN 03-06, 2013 CL Madison, WI SP Int Union Soil Sci, Univ Wisconsin, Coll Agr & Life Sci, Dept Soil Sci ID SOIL CARBON SEQUESTRATION; EUROPEAN GRASSLANDS; ORGANIC-MATTER; MANAGEMENT; TILLAGE; IMPACTS; BIODIVERSITY; TEMPERATE; DIVERSITY; BENEFITS AB Long-term agricultural research sites like the Wisconsin Integrated Cropping Systems Trial (WICST), with annual and perennial cropping systems growing alongside rotationally grazed pasture and native prairie plantings, provide invaluable insight into the carbon sequestration potential of agriculture in the North Central USA. Analysis of soil organic C (SOC) stocks during the first 20 years of the WICST study showed that annual row crop agriculture lost 5.5 Mg C ha(-1), while rotationally grazed pasture was a significant sink to 0-60 cm depth (5.1 Mg ha(-1)). While SOC changes for the Prairie, Conservation Reserve Program planting (CRP), and forage systems were not significantly different from zero when considered independently of one another, differences between systems suggest a trend of SOC accumulation in Prairie and loss in the CRP and forage systems. Carbon stabilization and accretion on the fine textured Mollisols of the North Central U. S. may not be possible, even under agricultural best management practices, without the inclusion of perennial grasses. RP Sanford, GR (reprint author), Great Lakes Bioenergy Res Ctr, 1552 Univ Ave, Madison, WI 53726 USA. EM gregg.r.sanford@gmail.com NR 32 TC 3 Z9 3 U1 2 U2 16 PU SPRINGER PI DORDRECHT PA PO BOX 17, 3300 AA DORDRECHT, NETHERLANDS BN 978-3-319-04084-4; 978-3-319-04083-7 J9 PROGR SOIL SCI PY 2014 BP 281 EP 288 DI 10.1007/978-3-319-04084-4_29 PG 8 WC Soil Science SC Agriculture GA BA6KO UT WOS:000337169400031 ER PT J AU Krejci, AJ Gebre, T Ruggiero, CA Mochena, MD Dickerson, JH AF Krejci, A. J. Gebre, T. Ruggiero, C. A. Mochena, M. D. Dickerson, J. H. TI Kinetics of monolayer and bilayer nanoparticle film formation during electrophoretic deposition SO ADVANCES IN APPLIED CERAMICS LA English DT Article DE Electrophoretic deposition; Directed assembly; Iron oxide; Monolayer; Time-resolved ID CDSE NANOCRYSTAL FILMS; THIN-FILMS AB The kinetics of electrophoretic deposition are studied for the growth of monolayers and bilayers of similar to 10 nm iron oxide nanoparticles. The net deposited nanoparticle film is measured as a function of time for five voltages through analysis of scanning electron microcopy images of the films. The collected data suggest that films deposited at different voltages have different kinetic behaviours. Additionally, we observe monolayer and bilayer growth separately, from which we assert that the initiation of the bilayer may be the source of variation in kinetic behaviour. C1 [Krejci, A. J.; Dickerson, J. H.] Vanderbilt Univ, Dept Phys & Astron, Nashville, TN 37235 USA. [Krejci, A. J.; Dickerson, J. H.] Vanderbilt Univ, Vanderbilt Inst Nanoscale Sci & Engn, Nashville, TN 37235 USA. [Gebre, T.; Mochena, M. D.] Florida A&M Univ, Dept Phys, Tallahassee, FL 32307 USA. [Ruggiero, C. A.; Dickerson, J. H.] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. [Dickerson, J. H.] Vanderbilt Univ, Dept Chem, Nashville, TN 37235 USA. RP Dickerson, JH (reprint author), Vanderbilt Univ, Dept Phys & Astron, Nashville, TN 37235 USA. EM jdickerson@bnl.gov RI Dickerson, James/F-7950-2013 OI Dickerson, James/0000-0001-9636-6303 FU United States Army Research Office [W911NF-12-1-0047]; United States National Science Foundation (NSF) CAREER Award [DMR-1054161]; US Department of Energy, Office of Basic Energy Sciences [DE-AC02-98CH10886] FX This research is partially supported by the United States Army Research Office, Award W911NF-12-1-0047, and the United States National Science Foundation (NSF) CAREER Award DMR-1054161. Research was carried out 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. NR 24 TC 2 Z9 2 U1 1 U2 12 PU MANEY PUBLISHING PI LEEDS PA STE 1C, JOSEPHS WELL, HANOVER WALK, LEEDS LS3 1AB, W YORKS, ENGLAND SN 1743-6753 EI 1743-6761 J9 ADV APPL CERAM JI Adv. Appl. Ceram. PD JAN PY 2014 VL 113 IS 1 BP 50 EP 54 DI 10.1179/1743676113Y.0000000124 PG 5 WC Materials Science, Ceramics SC Materials Science GA AI6XR UT WOS:000337021500009 ER PT J AU Liu, Z Mehran, A Phillips, TJ AghaKouchak, A AF Liu, Zhu Mehran, Ali Phillips, Thomas J. AghaKouchak, Amir TI Seasonal and regional biases in CMIP5 precipitation simulations SO CLIMATE RESEARCH LA English DT Article DE Precipitation; Climate; CMIP5 ID CLIMATE MODELS; EXTREMES; TEMPERATURE; ENSEMBLE; VARIABILITY; RESOLUTION; INDEXES; EVENTS; EXPECT; GRIDS AB This study provides insight into how CMIP5 climate models perform in simulating summer and winter precipitation at different geographical locations and climate conditions. Precipitation biases in the CMIP5 historical (1901 to 2005) simulations relative to the Climatic Research Unit (CRU) observations are evaluated over 8 regions exhibiting distinct seasonal hydroclimates: moist tropical (Amazonia and central Africa), monsoonal (southern China), moist continental (central Europe), semi-arid (western United States and eastern Australia), and polar (Siberia and Canada). While the bias and monthly quantile bias (MQB) reflect no substantial differences in CMIP5 summer and winter precipitation simulations at the global scale, strong seasonality and high inter-model variability are found over the selected moist tropical regions (i.e. Amazonia and central Africa). In the semi-arid regions, high inter-model precipitation variability is also displayed, especially in summer, while the median of simulations is an overestimate of both winter and summer precipitation. In Siberia and central Europe, most CMIP5 models underestimate summer precipitation, and overestimate it in winter. Also, the MQB values decrease as the choice of quantile thresholds increase, implying that the underestimation of summer precipitation is primarily associated with biases in lower quantiles of the precipitation distribution. While the CMIP5 models exhibit similar behaviors in simulating high-latitude winter precipitation, they differ substantially in summer simulations for the selected Canadian and Siberian regions. Finally, in the monsoonal southern China region, CMIP5 models exhibit large overall precipitation biases in both summer and winter, as well as at higher quantiles. C1 [Liu, Zhu; Mehran, Ali; AghaKouchak, Amir] Univ Calif Irvine, Irvine, CA 92697 USA. [Phillips, Thomas J.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. RP AghaKouchak, A (reprint author), Univ Calif Irvine, E4130 Engn Gateway, Irvine, CA 92697 USA. EM amir.a@uci.edu FU United States Bureau of Reclamation (USBR) [R11AP81451]; National Science Foundation (NSF) [EAR-1316536, OISE-1243543]; US Department of Energy at Lawrence Livermore National Laboratory [DE-AC52-07NA27344] FX We thank the Editor and the 3 anonymous reviewers for their thoughtful comments which led to significant improvements in the current version of the paper. The financial support for authors A.A., Z.L. and A.M. was made available from the United States Bureau of Reclamation (USBR) Award No. R11AP81451, and the National Science Foundation (NSF) Awards No. EAR-1316536 and OISE-1243543. The contributions of author T.J.P. were performed under the auspices of the US Department of Energy at Lawrence Livermore National Laboratory under contract DE-AC52-07NA27344. We acknowledge the World Climate Research Programme's Working Group on Coupled Modelling, which is responsible for CMIP, and we thank the climate-modeling groups (listed in Table 1 of this paper) for producing and making available their model output. For CMIP, the US Department of Energy's Program for Climate Model Diagnosis and Intercomparison provides coordinating support and leads the development of software infrastructure in partnership with the Global Organization for Earth System Science Portals. NR 68 TC 12 Z9 14 U1 0 U2 17 PU INTER-RESEARCH PI OLDENDORF LUHE PA NORDBUNTE 23, D-21385 OLDENDORF LUHE, GERMANY SN 0936-577X EI 1616-1572 J9 CLIM RES JI Clim. Res. PY 2014 VL 60 IS 1 BP 35 EP 50 DI 10.3354/cr01221 PG 16 WC Environmental Sciences; Meteorology & Atmospheric Sciences SC Environmental Sciences & Ecology; Meteorology & Atmospheric Sciences GA AI7GR UT WOS:000337053900004 ER PT J AU Jakubowski, AR Jackson, RD Casler, MD AF Jakubowski, Andrew R. Jackson, Randall D. Casler, Michael D. TI The History of Reed Canarygrass in North America: Persistence of Natives among Invading Eurasian Populations SO CROP SCIENCE LA English DT Article ID GRASS PHALARIS-ARUNDINACEA; PLANT INVASIONS; DNA; BIOENERGY; DOMESTICATION; AMPLIFICATION; EVOLUTIONARY; NUTRIENTS; SEQUENCES; NETWORKS AB Reed canarygrass (Phalaris arundinacea L.) is a major invader in North American wetlands that has also been planted as a forage crop for nearly a century. While the species is native to both North America and Eurasia, the geographic origin of invaders has remained unknown due to the previous inability to distinguish North American and Eurasian populations. The goals of this study were to (i) identify extant native North American populations if they exist, (ii) determine the geographic origin of present-day populations in North America, and (iii) compare the diversity among Eurasian and North American populations to determine whether there is evidence of a genetic bottleneck in North America. A total of 987 individuals from 373 accessions were investigated using 15 microsatellite markers. A subset of 37 individuals was sequenced at four chloroplast regions. The population structure of the species was inferred using Bayesian clustering approaches and a median joining tree. Native North American populations of reed canarygrass are still present in North America. However, only 3 of the 235 North American accessions sampled were of North American origin. All Eurasian subpopulations were present in North America and invading populations in North America were as diverse as populations in the Eurasian range. The Eurasian populations are far more common in North American wetlands today and suggest introduced Eurasian populations are more invasive than their North American counterparts although the mechanisms for the differences in invasibility remain a mystery. C1 [Jakubowski, Andrew R.; Jackson, Randall D.] Univ Wisconsin, Dep Agron, Madison, WI 53706 USA. [Jackson, Randall D.; Casler, Michael D.] Univ Wisconsin, DOE Great Lakes Bioenergy Res Ctr, Madison, WI 53706 USA. [Casler, Michael D.] ARS, USDA, US Dairy Forage Res Ctr, Madison, WI 53706 USA. RP Jakubowski, AR (reprint author), Univ Wisconsin, Dep Agron, 1575 Linden Dr, Madison, WI 53706 USA. EM Jakubowski@wisc.edu FU Grazing Lands Conservation Initiative [941-3]; USDA-ARS FX This work was funded in part by Grazing Lands Conservation Initiative grant 941-3 and by USDA-ARS funds. We are grateful to the University of Alaska Museum of the North (ALA) (in particular, Matt Carlson of the University of Alaska-Anchorage), the Bell Museum of Natural History at the University of Minnesota (MIN), The University of Wisconsin Herbarium (WIS), Agriculture and Agri-Food Canada DAO Herbarium, the University Laval Herbarium (QFA), and the Iowa State University Herbarium (ISC) for allowing us to sample tissue from specimens. We are grateful to Jerry Cherney and Nick Baker for assistance with plant and seed collection. We also wish to thank Dr. Hasan Khatib for the use of his lab for herbarium specimen DNA extractions and PCR setup. NR 56 TC 3 Z9 3 U1 5 U2 29 PU CROP SCIENCE SOC AMER PI MADISON PA 677 S SEGOE ROAD, MADISON, WI 53711 USA SN 0011-183X EI 1435-0653 J9 CROP SCI JI Crop Sci. PD JAN-FEB PY 2014 VL 54 IS 1 BP 210 EP 219 DI 10.2135/cropsci2013.05.0342 PG 10 WC Agronomy SC Agriculture GA AI3FG UT WOS:000336745400018 ER PT J AU Donahue, CM Pacheco, JSL Keith, JM Daly, SR AF Donahue, Courtney M. Pacheco, Juan S. Lezama Keith, Jason M. Daly, Scott R. TI Sulfur K-edge X-ray absorption spectroscopy and time-dependent density functional theory of arsenic dithiocarbamates SO DALTON TRANSACTIONS LA English DT Article ID EFFECTIVE CORE POTENTIALS; ELECTRONIC-STRUCTURE; MASS-SPECTROMETRY; AS(III) BINDING; COMPLEXES; LIGANDS; COVALENCY; PROTEINS; CHROMATOGRAPHY; MOLECULES AB S K-edge X-ray absorption spectroscopy (XAS) and time-dependent density functional theory (TDDFT) calculations were performed on a series of As[S2CNR2](3) complexes, where R-2 = Et-2, (CH2)(5) and Ph-2, to determine how dithiocarbamate substituents attached to N affect As[S2CNR2](3) electronic structure. Complimentary [PPh4][S2CNR2] salts were also studied to compare dithiocarbamate bonding in the absence of As. The XAS results indicate that changing the orientation of the alkyl substituents from trans to cis (R-2 = Et-2 vs. (CH2)(5)) yields subtle variations whereas differences associated with a change from alkyl to aryl are much more pronounced. For example, despite the differences in As 4p mixing, the first features in the S K-edge XAS spectra of [PPh4][S2CNPh2] and As[S2CNPh2](3) were both shifted by 0.3 eV compared to their alkyl-substituted derivatives. DFT calculations revealed that the unique shift observed for [PPh4] [S2CNPh2] is due to phenyl-induced splitting of the pi* orbitals delocalized over N, C and S. A similar phenomenon accounts for the shift observed for As[S2CNPh2](3), but the presence of two unique S environments (As-S and As center dot center dot center dot S) prevented reliable analysis of As-S covalency from the XAS data. In the absence of experimental values, DFT calculations revealed a decrease in As-S orbital mixing in As[S2CNPh2](3) that stems from a redistribution of electron density to S atoms participating in weaker As center dot center dot center dot S interactions. Simulated spectra obtained from TDDFT calculations reproduce the experimental differences in the S K-edge XAS data, which suggests that the theory is accurately modeling the experimental differences in As-S orbital mixing. The results highlight how S K-edge XAS and DFT can be used cooperatively to understand the electronic structure of low symmetry coordination complexes containing S atoms in different chemical environments. C1 [Donahue, Courtney M.; Daly, Scott R.] George Washington Univ, Dept Chem, Washington, DC 20052 USA. [Pacheco, Juan S. Lezama] Stanford Univ, Environm Earth Syst Sci Dept, Sch Earth Sci, Stanford, CA 94305 USA. [Keith, Jason M.] Colgate Univ, Dept Chem, Hamilton, NY 13346 USA. [Keith, Jason M.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Keith, JM (reprint author), Colgate Univ, Dept Chem, 13 Oak Dr, Hamilton, NY 13346 USA. EM srdaly@gwu.edu FU George Washington University; Colgate University; Los Alamos National Laboratory; National Nuclear Security Administration of the Department of Energy [DEAC52-06NA25396] FX We would like to thank Drs Stosh Kozimor and Angela Olsen for help collecting portions of the XAS data, and Dr Beau Ballard for helpful discussions. This work was supported by start-up funds at the George Washington University and Colgate University as well as the Director's Postdoctoral Fellowship at Los Alamos National Laboratory (JMK). Portions of this research were carried out at the Stanford Synchrotron Radiation Laboratory (SSRL), which is a national user facility supported by the U.S. Department of Energy, Office of Basic Energy Sciences. Los Alamos National Laboratory is operated by Los Alamos National Security, LLC, for the National Nuclear Security Administration of the Department of Energy under Contract DEAC52-06NA25396. NR 51 TC 4 Z9 4 U1 1 U2 12 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 2014 VL 43 IS 24 BP 9189 EP 9201 DI 10.1039/c4dt00078a PG 13 WC Chemistry, Inorganic & Nuclear SC Chemistry GA AI4NA UT WOS:000336840900027 PM 24811926 ER PT J AU Shen, YL Li, WK Wu, JR Li, S Luo, HM Dai, S Wu, WS AF Shen, Yinglin Li, Wenkui Wu, Jianrong Li, Shun Luo, Huimin Dai, Sheng Wu, Wangsuo TI Solvent extraction of lanthanides and yttrium from aqueous solution with methylimidazole in an ionic liquid SO DALTON TRANSACTIONS LA English DT Article ID METAL-IONS; ACTINIDE EXTRACTION; COMPLEXES; SEPARATION; TODGA; MECHANISMS; MALONAMIDE; SOLVATION; REMOVAL; DILUENT AB 1-Methylimidazole (1-MIM) and 2-methylimidazole (2-MIM) are miscible in water and imidazolium based ionic liquids (ILs), and can coordinate with soft metal ions. This paper reports a novel solvent extraction process for trivalent lanthanides and yttrium from aqueous solutions into ILs, which was promoted by a hydrophilic 1-MIM or 2-MIM. Slope analysis confirmed that MIM in ILs formed a 1 : 1 complex with La3+ and Y3+ and a 1 : 4 complex with Eu3+ and Lu3+, depending on the atomic number of the metal and the metal-ligand interactions that have been characterized by FTIR spectroscopy and ESI-MS. The effect of nitrate concentration on the extraction of lanthanides with 1-MIM in ILs was analysed. It indicated that nitrate anions were involved in the extraction process. Under the same conditions, the extraction of lanthanides with MIM into n-pentanol was carried out. The extractability was by far lower than that obtained in ILs. Both cationic exchange and neutral solvation mechanisms occurred in ILs and only the neutral solvation mechanism occurred in n-pentanol, which were demonstrated by the extraction tests and the structure of extracted species determined by ESI-MS. The competitive extraction in ILs showed good selectivity for lanthanides compared to alkali metals and alkaline earth cations. After extraction, lanthanides could be stripped very easily from the ionic liquid phase with dilute nitric acid. From the temperature dependence data, the thermodynamic parameter values (Delta H,Delta S and Delta G) were calculated. The results indicated that the extraction reactions were spontaneous and went through an endothermic process. C1 [Shen, Yinglin; Li, Wenkui; Wu, Jianrong; Li, Shun; Wu, Wangsuo] Lanzhou Univ, Radiochem Lab, Lanzhou 730000, Peoples R China. [Luo, Huimin] Oak Ridge Natl Lab, Energy & Transportat Sci Div, Oak Ridge, TN USA. [Dai, Sheng] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN USA. RP Shen, YL (reprint author), Lanzhou Univ, Radiochem Lab, Lanzhou 730000, Peoples R China. EM shenyl@lzu.edu.cn; dais@ornl.gov RI Dai, Sheng/K-8411-2015 OI Dai, Sheng/0000-0002-8046-3931 FU Ph.D. Programs Foundation of the Ministry of Education of China [20090211120026]; National Natural Science Foundation of China [J1210001]; US DOE, Office of Science, Division of Chemical Sciences, Geosciences and Biosciences [DE-AC05-0096OR22725] FX This research was supported by the Ph.D. Programs Foundation of the Ministry of Education of China (20090211120026) and the National Natural Science Foundation of China (J1210001). HML and SD were supported by US DOE, Office of Science, Division of Chemical Sciences, Geosciences and Biosciences under Contract DE-AC05-0096OR22725 with Oak Ridge National Laboratory, managed by UT-Battelle, LLC. NR 46 TC 19 Z9 20 U1 3 U2 46 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 2014 VL 43 IS 26 BP 10023 EP 10032 DI 10.1039/c4dt00747f PG 10 WC Chemistry, Inorganic & Nuclear SC Chemistry GA AI8DG UT WOS:000337135600026 PM 24854623 ER PT J AU Szovenyi, P Devos, N Weston, DJ Yang, XH Hock, Z Shaw, JA Shimizu, KK McDaniel, SF Wagner, A AF Szoevenyi, Peter Devos, Nicolas Weston, David J. Yang, Xiaohan Hock, Zsofia Shaw, Jonathan A. Shimizu, Kentaro K. McDaniel, Stuart F. Wagner, Andreas TI Efficient Purging of Deleterious Mutations in Plants with Haploid Selfing SO GENOME BIOLOGY AND EVOLUTION LA English DT Article DE high throughput sequencing; haploid; diploid; haploid-dominant life cycle; intragametophytic selfing; outcrossing; deleterious mutations ID EFFECTIVE POPULATION-SIZE; SPOROPHYTIC INBREEDING DEPRESSION; MOSS PHYSCOMITRELLA-PATENS; MATING SYSTEM; GENETIC LOAD; GENOMIC CONSEQUENCES; MOLECULAR EVOLUTION; SUBSTITUTION RATES; NATURAL-SELECTION; CAPSELLA-GRANDIFLORA AB In diploid organisms, selfing reduces the efficiency of selection in removing deleterious mutations from a population. This need not be the case for all organisms. Some plants, for example, undergo an extreme form of selfing known as intragametophytic selfing, which immediately exposes all recessive deleterious mutations in a parental genome to selective purging. Here, we ask how effectively deleterious mutations are removed from such plants. Specifically, we study the extent to which deleterious mutations accumulate in a predominantly selfing and a predominantly outcrossing pair of moss species, using genome-wide transcriptome data. We find that the selfing species purge significantly more nonsynonymous mutations, as well as a greater proportion of radical amino acid changes which alter physicochemical properties of amino acids. Moreover, their purging of deleterious mutation is especially strong in conserved regions of protein-coding genes. Our observations show that selfing need not impede but can even accelerate the removal of deleterious mutations, and do so on a genome-wide scale. C1 [Szoevenyi, Peter; Shimizu, Kentaro K.; Wagner, Andreas] Univ Zurich, Inst Evolutionary Biol & Environm Studies, CH-8006 Zurich, Switzerland. [Szoevenyi, Peter; Hock, Zsofia] Univ Zurich, Inst Systemat Bot, CH-8006 Zurich, Switzerland. [Szoevenyi, Peter; Wagner, Andreas] Swiss Inst Bioinformat, Lausanne, Switzerland. [Szoevenyi, Peter] Inst Biol, MTA ELTE MTM Ecol Res Grp, ELTE, Budapest, Hungary. [Devos, Nicolas; Shaw, Jonathan A.] Duke Univ, Dept Biol, Durham, NC 27706 USA. [Weston, David J.; Yang, Xiaohan] Oak Ridge Natl Lab, Biosci Div, Oak Ridge, TN USA. [McDaniel, Stuart F.] Univ Florida, Dept Biol, Gainesville, FL 32611 USA. [Wagner, Andreas] ASTAR, Bioinformat Inst, Singapore, Singapore. [Wagner, Andreas] Santa Fe Inst, Santa Fe, NM 87501 USA. RP Szovenyi, P (reprint author), Univ Zurich, Inst Evolutionary Biol & Environm Studies, CH-8006 Zurich, Switzerland. EM peter.szoevenyi@uzh.ch RI McDaniel, Stuart/L-5197-2014; Devos, Nicolas/E-7490-2015; Yang, Xiaohan/A-6975-2011 OI Yang, Xiaohan/0000-0001-5207-4210 FU Swiss National Science Foundation, Ambizione [PZ00P3_131726]; URPP pilot grant of the Systems Biology/Functional Genomics priority program of the University of Zurich; Swiss National Science Foundation [315230-129708, 31003A_140917]; University Priority Research Program in Evolutionary Biology at the University of Zurich; NSF [DEB-0918998] FX Three anonymous reviewers provided helpful comments on an earlier version of this manuscript. This work was supported by the Swiss National Science Foundation, Ambizione grant number PZ00P3_131726 to P.S.Z. and by a URPP pilot grant of the Systems Biology/Functional Genomics priority program of the University of Zurich to P.S.Z. This work also received support through Swiss National Science Foundation grants 315230-129708 to A. W., and grant 31003A_140917 to K. K. S., as well as by the University Priority Research Program in Evolutionary Biology at the University of Zurich to A. W. and K. K. S. This work was also supported by an NSF grant no. DEB-0918998 to A.J.S. and Blanka Shaw. NR 89 TC 15 Z9 15 U1 4 U2 21 PU OXFORD UNIV PRESS PI OXFORD PA GREAT CLARENDON ST, OXFORD OX2 6DP, ENGLAND SN 1759-6653 J9 GENOME BIOL EVOL JI Genome Biol. Evol. PY 2014 VL 6 IS 5 BP 1238 EP 1252 DI 10.1093/gbe/evu099 PG 15 WC Evolutionary Biology; Genetics & Heredity SC Evolutionary Biology; Genetics & Heredity GA AI7BY UT WOS:000337037100020 PM 24879432 ER PT J AU Hubbard, CG West, LJ Rodriguez-Blanco, JD Shaw, S AF Hubbard, Christopher G. West, L. Jared Rodriguez-Blanco, Juan Diego Shaw, Samuel TI Laboratory study of spectral induced polarization responses of magnetite - Fe2+ redox reactions in porous media SO GEOPHYSICS LA English DT Article ID FREQUENCY ELECTRICAL-PROPERTIES; ATOM EXCHANGE; SEDIMENTS; URANIUM; IRON; BIOREMEDIATION; PRECIPITATION; SIGNATURES; COMPLEXATION; REACTIVITY AB Spectral induced polarization (SIP) phase anomalies in field surveys at contaminated sites have previously been shown to correlate with the occurrence of chemically reducing conditions and/or semiconductive minerals, but the reasons for this are not fully understood. We report a systematic laboratory investigation of the role of the semiconductive mineral magnetite and its interaction with redox-active versus redox-inactive ions in producing such phase anomalies. The SIP responses of quartz sand with 5% magnetite in solutions containing redox-inactive Ca2+ and Ni2+ versus redox-active Fe2+ were measured across the pH ranges corresponding to adsorption of these metals to magnetite. With redox inactive ions Ca2+ and Ni2+, SIP phase response showed no changes across the pH range 4-10, corresponding to their adsorption, showing similar to 30 mrad anomalies peaking at similar to 59-74 Hz. These large phase anomalies are probably caused by polarization of the magnetite-solution interfaces. With the redox-active ion Fe2+, frequency of peak phase response decreased progressively from similar to 46 to similar to 3 Hz as effluent pH increased from four to seven, corresponding to progressive adsorption of Fe2+ to the magnetite surface. The latter frequency (3 Hz) corresponds approximately with those of phase anomalies detected in field surveys reported elsewhere. We conclude that pH sensitivity arises from redox reactions between Fe2+ and magnetite surfaces, with transfer of electrical charge through the bulk mineral, as reported in other laboratory investigations. Our results confirm that SIP measurements are sensitive to redox reactions involving charge transfers between adsorbed ions and semiconductive minerals. Phase anomalies seen in field surveys of groundwater contamination and biostimulation may therefore be indicative of iron-reducing conditions, when semiconductive iron minerals such as magnetite are present. C1 [Hubbard, Christopher G.; West, L. Jared; Rodriguez-Blanco, Juan Diego; Shaw, Samuel] Univ Leeds, Sch Earth & Environm, Leeds, W Yorkshire, England. RP Hubbard, CG (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, Berkeley, CA 94720 USA. EM cghubbard@lbl.gov; L.J.West@leeds.ac.uk; jblanco@nano.ku.dk; sam.shaw@manchester.ac.uk RI Rodriguez-Blanco, Juan Diego/D-5197-2013; Hubbard, Christopher/J-6150-2014; Shaw, Sam/A-3528-2017 OI Rodriguez-Blanco, Juan Diego/0000-0001-5978-3001; Hubbard, Christopher/0000-0002-8217-8122; Shaw, Sam/0000-0002-6353-5454 FU Royal Society [RG2010R1]; NERC [NE/D014026/1] FX Funding was provided by Royal Society grant RG2010R1 and NERC grant NE/D014026/1. We thank Lee Slater, Dimitrios Ntarlagiannis, and Jeff Heenan for assistance in setting up the SIP equipment; Tony Windross and Rhys Moore for constructing the sample holder; Kath Morris, Dimitrios Ntarlagiannis, and Yuxin Wu for their assistance with manuscript preparation; and the reviewers for their insightful comments, which helped improve the manuscript. NR 55 TC 10 Z9 10 U1 1 U2 10 PU SOC EXPLORATION GEOPHYSICISTS PI TULSA PA 8801 S YALE ST, TULSA, OK 74137 USA SN 0016-8033 EI 1942-2156 J9 GEOPHYSICS JI Geophysics PD JAN-FEB PY 2014 VL 79 IS 1 BP D21 EP D30 DI 10.1190/GEO2013-0079.1 PG 10 WC Geochemistry & Geophysics SC Geochemistry & Geophysics GA AI5MU UT WOS:000336912400007 ER PT J AU Wu, YX Surasani, VK Li, L Hubbard, SS AF Wu, Yuxin Surasani, Vikranth Kumar Li, Li Hubbard, Susan Sharpless TI Geophysical monitoring and reactive transport simulations of bioclogging processes induced by Leuconostoc mesenteroides SO GEOPHYSICS LA English DT Article ID SATURATED HYDRAULIC CONDUCTIVITY; INDUCED-POLARIZATION; POROUS-MEDIA; MICROBIAL-GROWTH; SAND COLUMNS; UNCONSOLIDATED SEDIMENTS; ELECTRON-MICROSCOPY; CHEMICAL-REACTIONS; DISSOLUTION RATES; MASS-TRANSPORT AB Although bioclogging has been used for various applications, its performance has been unpredictable. We carried out a bioclogging experiment and developed a reactive transport model to understand and quantify geophysical responses to the production of a biopolymer (dextran) in a silica sand porous medium. The developed model was used to predict effectiveness of bioclogging and the associated geophysical signature under different treatment conditions. The porosity reduction calculated from the reactive transport modeling matched the concurrent increase in electrical resistivity and confirmed the dominant contribution of pore fluid conductivity to the bulk electrical conductivity. Correlations between measured electrical phase signals and predicted mineral surface area reduction indicated the controlling effect of mineral surface area on polarization. The joint use of the two methods quantitatively estimated the extent of decrease in porosity as well as effective mineral surface area, both of which are challenging to measure nondestructively in biological systems. The joint use of the geophysical methods and reactive transport modeling provided a better understanding of the dominant processes that govern dextran-based bioclogging and the associated geophysical responses. This opens new opportunities for quantifying changes associated with bioclogging processes and can potentially lead to new conceptual models that relate hydraulic property changes to the porosity and mineral surface area, which will enhance prediction, monitoring, and control of applications that use bioclogging. C1 [Wu, Yuxin; Hubbard, Susan Sharpless] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, Berkeley, CA 94720 USA. [Surasani, Vikranth Kumar; Li, Li] Penn State Univ, John & Willie Leone Family Dept Energy & Mineral, University Pk, PA 16802 USA. [Surasani, Vikranth Kumar] Birla Inst Sci & Technol, Dept Chem Engn, Hyderabad, Andhra Pradesh, India. RP Wu, YX (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, Berkeley, CA 94720 USA. EM ywu3@lbl.gov; surasani@psu.edu; lili@eme.psu.edu; sshubbard@lbl.gov RI Hubbard, Susan/E-9508-2010; Wu, Yuxin/G-1630-2012; Li, Li/A-6077-2008 OI Wu, Yuxin/0000-0002-6953-0179; Li, Li/0000-0002-1641-3710 FU Energy Bioscience Institute FX Funding for this research is provided by Energy Bioscience Institute. The authors wish to thank T.-H. Kwon (Washington State University) for the preparation of the microbes and growth media and R. Chakraborty (Lawrence Berkeley National Laboratory) for microbial cell counts and imaging. We thank the associate editor J. Carcione and three reviewers (D. Ntarlagiannis at Rutgers University and two anonymous reviewers) for their helpful comments. NR 97 TC 4 Z9 4 U1 2 U2 10 PU SOC EXPLORATION GEOPHYSICISTS PI TULSA PA 8801 S YALE ST, TULSA, OK 74137 USA SN 0016-8033 EI 1942-2156 J9 GEOPHYSICS JI Geophysics PD JAN-FEB PY 2014 VL 79 IS 1 BP E61 EP E73 DI 10.1190/GEO2013-0121.1 PG 13 WC Geochemistry & Geophysics SC Geochemistry & Geophysics GA AI5MU UT WOS:000336912400013 ER PT J AU Mirtchev, P Liao, K Jaluague, E Qiao, Q Tian, Y Varela, M Burch, KS Pennycook, SJ Perovic, DD Ozin, G AF Mirtchev, Peter Liao, Kristine Jaluague, Elizabeth Qiao, Qiao Tian, Yao Varela, Maria Burch, Kenneth S. Pennycook, Stephen J. Perovic, Doug D. Ozin, Geoffrey TI Fe2O3/Cu2O heterostructured nanocrystals SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID CORE-SHELL NANOPARTICLES; HYBRID NANOCRYSTALS; NANOROD HETEROSTRUCTURES; OPTICAL-PROPERTIES; SEEDED GROWTH; CUPROUS-OXIDE; NANOSTRUCTURES; CDSE; NANOHETEROSTRUCTURES; NANOARCHITECTURES AB We report the synthesis of colloidal gamma-Fe2O3/Cu2O hetero-nanocrystals (HNCs) using a solution-phase seeded-growth approach. gamma-Fe2O3 nanocrystals were used as seeds for the nucleation of metallic Cu followed by oxidation of the Cu domain to Cu2O upon exposure to air. The resulting dimer, trimer, and oligomer HNCs were characterized by high resolution electron microscopy, energy dispersive X-ray spectroscopy, and powder X-ray diffraction. The iron oxide component was found to be mainly gamma-Fe2O3 using a combination of Raman and X-ray photoelectron spectroscopy. A maximal HNC yield of 72% was achieved by reducing particle growth time to a lower growth temperature with respect to the individual component particles. Size-selective precipitation was used to enrich the nanoparticle mixture in gamma-Fe2O3/Cu2O dimers by removing the larger aggregates. Ultraviolet photoelectron spectroscopy was used to determine that gamma-Fe2O3 and Cu2O are n-doped and p-doped respectively and form a staggered, type II band alignment. As such, gamma-Fe2O3/Cu2O HNCs may be attractive candidates for applications in solar energy conversion and represent a valuable addition to the growing library of oxide-oxide hetero-nanocrystals. C1 [Mirtchev, Peter; Liao, Kristine; Ozin, Geoffrey] Univ Toronto, Dept Chem, Toronto, ON M5S 3H6, Canada. [Jaluague, Elizabeth] Queens Univ, Dept Chem, Kingston, ON K7L 3N6, Canada. [Qiao, Qiao; Varela, Maria] Univ Complutense Madrid, Dept Fis Aplicada 3, E-28040 Madrid, Spain. [Qiao, Qiao; Varela, Maria] Univ Complutense Madrid, Inst Pluridisciplinar, E-28040 Madrid, Spain. [Tian, Yao; Varela, Maria] Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. [Burch, Kenneth S.] Univ Toronto, Dept Phys, Toronto, ON M5S 1A7, Canada. [Pennycook, Stephen J.] Univ Tennessee, Dept Mat Sci & Engn, Knoxville, TN 37996 USA. [Perovic, Doug D.] Univ Toronto, Dept Mat Sci & Engn, Toronto, ON M5S 3E4, Canada. RP Ozin, G (reprint author), Univ Toronto, Dept Chem, 80 St George St, Toronto, ON M5S 3H6, Canada. EM gozin@chem.utoronto.ca RI Varela, Maria/E-2472-2014 OI Varela, Maria/0000-0002-6582-7004 FU Natural Sciences and Engineering Research Council; Ministry of Research Innovation (MRI); University of Toronto; NSERC CGS-D Graduate Scholarship; U.S. Department of Energy (DOE), Basic Energy Sciences (BES), Materials Sciences and Engineering Division; U.S. Department of Energy (DOE), Basic Energy Sciences (BES), Materials Sciences and Engineering Division through the Center for Nanophase Materials Sciences (CNMS); Scientific User Facilities Division, DOE-BES; European Research Council [239739] FX We would like to acknowledge the Natural Sciences and Engineering Research Council, the Ministry of Research Innovation (MRI) and the University of Toronto for financial support of this work. G.A.O. is the Government of Canada Research Chair in Materials Chemistry and Nanochemistry. K. S. B. is the Canada Research Chair in the Spectroscopy of Novel Materials. P. M. is a holder of an NSERC CGS-D Graduate Scholarship. We would like to thank Tornado Spectral Systems for the use of the U1 Raman spectrometer. The authors would also like to acknowledge Dr Neil Coombs, Ilya Gourevich, and the Canadian and Japanese offices of Hitachi High Technologies for assistance with TEM imaging, EELS, and EDX acquisition. Research at ORNL was supported by the U.S. Department of Energy (DOE), Basic Energy Sciences (BES), Materials Sciences and Engineering Division, and through the Center for Nanophase Materials Sciences (CNMS), which is sponsored by the Scientific User Facilities Division, DOE-BES. Research at UCM supported by the European Research Council Starting Investigator Award STEMX #239739. NR 58 TC 4 Z9 4 U1 7 U2 108 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 2014 VL 2 IS 22 BP 8525 EP 8533 DI 10.1039/c4ta01757a PG 9 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA AI4PT UT WOS:000336848000047 ER PT J AU Lekse, JW Haycock, BJ Lewis, JP Kauffman, DR Matranga, C AF Lekse, Jonathan W. Haycock, Barry J. Lewis, James P. Kauffman, Douglas R. Matranga, Christopher TI The effect of electronic structure changes in NaInO2 and NaIn0.9Fe0.1O2 on the photoreduction of methylene blue SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID PHOTOCATALYTIC DEGRADATION; DOPED TIO2; WATER; SEMICONDUCTOR; DECOMPOSITION; CUGA1-XFEXO2; DELAFOSSITES; CARBON; STATES AB Photochemical dye degradation is a promising method for organic pollutant remediation; however, this process has been limited by the efficiency of the catalyst materials with respect to photon absorption. An ideal catalyst would be capable of using as much of the solar spectrum as possible, in particular the visible region. One interesting class of materials that have the potential to provide this photoactivity is known as delafossites. These materials have the general formula ABO(2) and are based on the mineral CuFeO2, also known as delafossite. They are especially interesting due to the ability to alter the band structure of these materials using chemical substitution. In particular, substitution on the B-site in these materials can be used to tune the physical properties of delafossites for specific applications. In this work, NaInO2 and NaIn0.9Fe0.1O2 have been studied and Fe substitution was found to decrease the band gap energy from 3.9 eV to 2.8 eV. The catalytic activity, measured by methylene blue dye degradation, of these delafossite materials was analysed and the reduction in band gap energy was found to result in increased visible light photoactivity. Computationally, thousands of supercells were examined in order to determine the most energetically favourable substituted structures and generate density of states plots in order to determine that the experimentally observed results were due to Fe-states increasing the energy of the highest occupied molecular orbitals. C1 [Lekse, Jonathan W.; Haycock, Barry J.; Lewis, James P.; Kauffman, Douglas R.; Matranga, Christopher] US DOE, Natl Energy Technol Lab, Pittsburgh, PA 15236 USA. [Lekse, Jonathan W.] URS, South Pk, PA 15129 USA. [Haycock, Barry J.; Lewis, James P.] W Virginia Univ, Dept Phys, Morgantown, WV 26506 USA. RP Lekse, JW (reprint author), US DOE, Natl Energy Technol Lab, Pittsburgh, PA 15236 USA. EM Jonathan.Lekse@CONTR.NETL.DOE.GOV RI Matranga, Christopher/E-4741-2015; OI Matranga, Christopher/0000-0001-7082-5938; Kauffman, Douglas/0000-0002-7855-3428 FU RES [DE-FE0004000]; National Science Foundation [NSF DMR 09-03225]; agency of the United States Government 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 work was also supported, in part, by the National Science Foundation through NSF DMR 09-03225. 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 favouring by the United States Government or any agency thereof. The views and opinions of authors expressed herein for not necessarily state or reflect those of the United States Government or any agency thereof. NR 42 TC 3 Z9 3 U1 4 U2 22 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 2014 VL 2 IS 24 BP 9331 EP 9337 DI 10.1039/c4ta00906a PG 7 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA AI4QT UT WOS:000336850600049 ER PT J AU Vasdekis, AE Wilkins, MJ Grate, JW Kelly, RT Konopka, AE Xantheas, SS Chang, TM AF Vasdekis, A. E. Wilkins, M. J. Grate, J. W. Kelly, R. T. Konopka, A. E. Xantheas, S. S. Chang, T. -M. TI Solvent immersion imprint lithography SO LAB ON A CHIP LA English DT Article ID MICROFLUIDIC DEVICES; SOFT LITHOGRAPHY; CAPILLARY-ELECTROPHORESIS; NANOIMPRINT LITHOGRAPHY; POLYMERS; DISSOLUTION; FABRICATION; SYSTEMS; POLYSTYRENE; TECHNOLOGY AB We present Solvent Immersion Imprint Lithography (SIIL), a technique for polymer functionalization and microsystem prototyping. SIIL is based on polymer immersion in commonly available solvents. This was experimentally and computationally analyzed, uniquely enabling two practical aspects. The first is imprinting and bonding deep features that span the 1 to 100 mu m range, which are unattainable with existing solvent-based methods. The second is a functionalization scheme characterized by a well-controlled, 3D distribution of chemical moieties. SIIL is validated by developing microfluidics with embedded 3D oxygen sensors and microbioreactors for quantitative metabolic studies of a thermophile anaerobe microbial culture. Polystyrene (PS) was employed in the aforementioned applications; however all soluble polymers - including inorganic ones - can be employed with SIIL under no instrumentation requirements and typical processing times of less than two minutes. C1 [Vasdekis, A. E.; Kelly, R. T.] Pacific NW Natl Lab, Environm Mol Sci Lab, Richland, WA 99352 USA. [Wilkins, M. J.; Konopka, A. E.] Pacific NW Natl Lab, Div Biol Sci, Richland, WA 99352 USA. [Grate, J. W.; Xantheas, S. S.] Pacific NW Natl Lab, Div Phys Sci, Richland, WA 99352 USA. [Chang, T. -M.] Univ Wisconsin Parkside, Kenosha, WI 53141 USA. RP Vasdekis, AE (reprint author), Pacific NW Natl Lab, Environm Mol Sci Lab, POB 999, Richland, WA 99352 USA. EM andreas.vasdekis@pnnl.gov RI Xantheas, Sotiris/L-1239-2015; Kelly, Ryan/B-2999-2008; Wilkins, Michael/A-9358-2013; OI Kelly, Ryan/0000-0002-3339-4443; Vasdekis, Andreas/0000-0003-4315-1047; Xantheas, Sotiris/0000-0002-6303-1037 FU Pacific Northwest National Laboratory (Linus Pauling Fellowship - LDRD) [PN12005/2406]; Department of Energy's Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory [48924]; National Energy Research Scientific Computing Center - the Office of Science of the U. S. Department of Energy [DE-AC02-05CH11231]; US Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences FX AEV gratefully acknowledges funding from the Pacific Northwest National Laboratory (Linus Pauling Fellowship - LDRD project ID: PN12005/2406). Part of the research was performed using EMSL, a national scientific user facility sponsored by the Department of Energy's Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory (proposal ID: 48924). The experimental work was conducted under the Laboratory Directed Research and Development Program at PNNL, a multiprogram national laboratory operated by Battelle for the U. S. Department of Energy. The computational part of this work was supported by the US Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences (TMC and SSX). Computer resources were provided by 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. Additionally, the kind supply of the engineered Flavobacterium strain by Shicheng Chen (Michigan State University), the Yarrowia Lipolytica by Gregory Stephanopoulos (MIT) are gratefully acknowledged. NR 54 TC 9 Z9 9 U1 3 U2 31 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 2014 VL 14 IS 12 BP 2072 EP 2080 DI 10.1039/c4lc00226a PG 9 WC Biochemical Research Methods; Chemistry, Multidisciplinary; Nanoscience & Nanotechnology SC Biochemistry & Molecular Biology; Chemistry; Science & Technology - Other Topics GA AI3DG UT WOS:000336738900013 PM 24789571 ER PT J AU Romero-Severson, EO Meadors, GD Volz, EM AF Romero-Severson, E. O. Meadors, G. D. Volz, E. M. TI A Generating Function Approach to HIV Transmission with Dynamic Contact Rates SO MATHEMATICAL MODELLING OF NATURAL PHENOMENA LA English DT Article DE HIV; transmission model; R-0; generating functions; branching process ID INFECTION; EPIDEMIC; GONORRHEA; NETWORKS; MODELS; UGANDA; RAKAI; STAGE; MEN; SEX AB The basic reproduction number, R-0, is often defined as the average number of infections generated by a newly infected individual in a fully susceptible population. The interpretation, meaning, and derivation of R-0 are controversial. However, in the context of mean field models, R-0 demarcates the epidemic threshold below which the infected population approaches zero in the limit of time. In this manner, R-0 has been proposed as a method for understanding the relative impact of public health interventions with respect to disease eliminations from a theoretical perspective. The use of R-0 is made more complex by both the strong dependency of R-0 on the model form and the stochastic nature of transmission. A common assumption in models of HIV transmission that have closed form expressions for R-0 is that a single individual's behavior is constant over time. In this paper we derive expressions for both R-0 and probability of an epidemic in a finite population under the assumption that people periodically change their sexual behavior over time. We illustrate the use of generating functions as a general framework to model the effects of potentially complex assumptions on the number of transmissions generated by a newly infected person in a susceptible population. We find that the relationship between the probability of an epidemic and R-0 is not straightforward, but, that as the rate of change in sexual behavior increases both R-0 and the probability of an epidemic also decrease. C1 [Romero-Severson, E. O.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Meadors, G. D.] Univ Michigan, Dept Phys, Ann Arbor, MI 48109 USA. [Volz, E. M.] Univ Michigan, Dept Epidemiol, Ann Arbor, MI 48109 USA. RP Romero-Severson, EO (reprint author), Los Alamos Natl Lab, Los Alamos, NM 87545 USA. EM eoromero@lanl.gov FU NIH [R01AI087520, R01AI78752, K01-AI-091440-03]; NSF [0855422, 1205173] FX EORS was supported by NIH grants R01AI087520 and R01AI78752. GDM was supported by NSF awards 0855422 and 1205173. EMV was supported by NIH Career Development Award K01-AI-091440-03. NR 28 TC 2 Z9 2 U1 1 U2 6 PU EDP SCIENCES S A PI LES ULIS CEDEX A PA 17, AVE DU HOGGAR, PA COURTABOEUF, BP 112, F-91944 LES ULIS CEDEX A, FRANCE SN 0973-5348 EI 1760-6101 J9 MATH MODEL NAT PHENO JI Math. Model. Nat. Phenom. PY 2014 VL 9 IS 2 BP 121 EP 135 DI 10.1051/mmnp/20149208 PG 15 WC Mathematical & Computational Biology; Mathematics, Interdisciplinary Applications; Multidisciplinary Sciences SC Mathematical & Computational Biology; Mathematics; Science & Technology - Other Topics GA AI6CO UT WOS:000336957600008 PM 27087760 ER PT J AU McMahon, BH Manore, CA Hyman, JM LaBute, MX Fair, JM AF McMahon, B. H. Manore, C. A. Hyman, J. M. LaBute, M. X. Fair, J. M. TI Coupling Vector-host Dynamics with Weather Geography and Mitigation Measures to Model Rift Valley Fever in Africa SO MATHEMATICAL MODELLING OF NATURAL PHENOMENA LA English DT Article DE epidemiology; rift valley fever; mitigation; vaccination; geography; weather; network model ID WEST-AFRICA; BORNE DISEASES; VIRUS; TRANSMISSION; OUTBREAK; CLIMATE; MOSQUITOS; EPIDEMIOLOGY; POPULATIONS; EMERGENCE AB We present and characterize a multi-host epidemic model of Rift Valley fever (RVF) virus in East Africa with geographic spread on a network, rule-based mitigation measures, and mosquito infection and population dynamics. Susceptible populations are depleted by disease and vaccination and are replenished with the birth of new animals. We observe that the severity of the epidemics is strongly correlated with the duration of the rainy season and that even severe epidemics are abruptly terminated when the rain stops. Because naturally acquired herd immunity is established, total mortality across 25 years is relatively insensitive to many mitigation approaches. Strong reductions in cattle mortality are expected, however, with sufficient reduction in population densities of either vectors or susceptible (ie. unvaccinated) hosts. A better understanding of RVF epidemiology would result from serology surveys to quantify the importance of herd immunity in epidemic control, and sequencing of virus from representative animals to quantify the realative importance of transportation and local reservoirs in nucleating yearly epidemics. Our results suggest that an effective multi-layered mitigation strategy would include vector control, movement control, and vaccination of young animals yearly, even in the absence of expected rainfall. C1 [McMahon, B. H.; Fair, J. M.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Manore, C. A.; Hyman, J. M.] Tulane Univ, Dept Math, New Orleans, LA 70118 USA. [Manore, C. A.] Tulane Univ, Ctr Computat Sci, New Orleans, LA 70118 USA. [LaBute, M. X.] Lawrence Livermore Natl Lab, Appl Stat Grp, Computat Engn Div, Livermore, CA 94550 USA. RP Fair, JM (reprint author), Los Alamos Natl Lab, K404, Los Alamos, NM 87545 USA. EM fmfair@lanl.gov FU US Department of Energy [DE-AC52-06NA25396]; NIH/NIGMS grant in the Models of Infectious Disease Agent Study (MIDAS) program [U01-GM097661-01]; NSF MPS Division of Mathematical Sciences NSF/MPS/DMS [DMS-1122666] FX We thank Dennis Powell, Leslie Moore, Mac Brown, Joel Berendzen, and Mary Green for assistance with data collection and analysis. This work was performed in part by Defense Threat Reduction Agency (DTRA) CBT-09-IST-05-1-0092. Los Alamos National Security, LLC, is operator of the Los Alamos National Laboratory (LANL) under Contract No. DE-AC52-06NA25396 with the US Department of Energy. This work was also supported in part by an NIH/NIGMS grant in the Models of Infectious Disease Agent Study (MIDAS) program, U01-GM097661-01 and by the NSF MPS Division of Mathematical Sciences NSF/MPS/DMS grant DMS-1122666. NR 49 TC 4 Z9 4 U1 0 U2 11 PU EDP SCIENCES S A PI LES ULIS CEDEX A PA 17, AVE DU HOGGAR, PA COURTABOEUF, BP 112, F-91944 LES ULIS CEDEX A, FRANCE SN 0973-5348 EI 1760-6101 J9 MATH MODEL NAT PHENO JI Math. Model. Nat. Phenom. PY 2014 VL 9 IS 2 BP 161 EP 177 DI 10.1051/mmnp/20149211 PG 17 WC Mathematical & Computational Biology; Mathematics, Interdisciplinary Applications; Multidisciplinary Sciences SC Mathematical & Computational Biology; Mathematics; Science & Technology - Other Topics GA AI6CO UT WOS:000336957600011 PM 25892858 ER PT J AU Ho, SF Mendoza-Garcia, A Guo, SJ He, K Su, D Liu, S Metin, O Sun, SH AF Ho, Sally Fae Mendoza-Garcia, Adriana Guo, Shaojun He, Kai Su, Dong Liu, Sheng Metin, Onder Sun, Shouheng TI A facile route to monodisperse MPd (M = Co or Cu) alloy nanoparticles and their catalysis for electrooxidation of formic acid SO NANOSCALE LA English DT Article ID PD NANOPARTICLES; PALLADIUM NANOPARTICLES; CARBON NANOTUBES; AMMONIA BORANE; ELECTROCATALYTIC ACTIVITIES; OXIDATION; DEHYDROGENATION; REDUCTION; EFFICIENT; GRAPHENE AB MPd (M = Co, or Cu) nanoparticles (NPs) were synthesized by borane-amine reduction of metal acetylacetonates. The size of the MPd NPs was controlled at 3.5 nm and their compositions were tuned by the molar ratios of the metal precursors. These MPd NPs were active catalysts for electrochemical oxidation of formic acid and the Cu30Pd70 NPs showed the highest mass activity at 1192.9 A g(Pd)(-1), much higher than 552.6 A g(Pd)(-1) obtained from the 3.5 nm Pd NPs. Our synthesis provides a facile route to MPd NPs, allowing further investigation of MPd NP catalysts for electrochemical oxidation and many other chemical reactions. C1 [Ho, Sally Fae; Mendoza-Garcia, Adriana; Guo, Shaojun; Liu, Sheng; Metin, Onder; Sun, Shouheng] Brown Univ, Dept Chem, Providence, RI 02912 USA. [He, Kai; Su, Dong] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. [Metin, Onder] Ataturk Univ, Fac Sci, Dept Chem, TR-25240 Erzurum, Turkey. RP Sun, SH (reprint author), Brown Univ, Dept Chem, Providence, RI 02912 USA. EM ssun@brown.edu RI Guo, Shaojun/A-8449-2011; He, Kai/B-9535-2011; Su, Dong/A-8233-2013 OI Guo, Shaojun/0000-0002-5941-414X; He, Kai/0000-0003-4666-1800; Su, Dong/0000-0002-1921-6683 FU U.S. Army Research Laboratory; U.S. Army Research Office under the Multi University Research Initiative MURI grant [W911NF-11-1-0353]; U.S. Department of Energy, Office of Basic Energy Sciences [DE-AC02-98CH10886] FX This work was supported by the U.S. Army Research Laboratory and the U.S. Army Research Office under the Multi University Research Initiative MURI grant number W911NF-11-1-0353 on "Stress-Controlled Catalysis via Engineered Nanostructures". TEM work carried out at the Center for Functional Nanomaterials, Brookhaven National Laboratory, was supported by the U.S. Department of Energy, Office of Basic Energy Sciences, under Contract No. DE-AC02-98CH10886. NR 30 TC 28 Z9 28 U1 26 U2 125 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 2014 VL 6 IS 12 BP 6970 EP 6973 DI 10.1039/c4nr01107d PG 4 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA AI8FI UT WOS:000337143900090 PM 24838646 ER PT J AU Kim, BJ Kim, MW Jang, JS Stach, EA AF Kim, B. J. Kim, M. W. Jang, J. S. Stach, E. A. TI Real time observation of ZnO nanostructure formation via the solid-vapor and solid-solid-vapor mechanisms SO NANOSCALE LA English DT Article ID ZINC-OXIDE NANOWIRES; GROWTH; SURFACE; TEMPERATURE; ENERGY; NUCLEATION; NANOBELTS; DRIVEN; MODEL AB We report in situ transmission electron microscopy studies of the formation of ZnO nanostructures - nanoscale depressions, nanoholes, nanoribbons, and nanosheets - and the phase stability and kinetics of Au catalysts on ZnO. During annealing, the ZnO Layer produces hexagonally shaped, vertical nanoscale depressions, which increase in size along the (0001) growth direction through preferential dissociation from the {10 (1) over bar0} facet and which subsequently form hexagonal islands at their six-fold junctions. Real time observations of the annealing of Au deposited on ZnO show that the catalysts remain solid up to 900 C, an observation that has implications regarding ZnO nanowire growth via the vapor-solid-solid mechanism (VSS). The Au aka creates hexagonal nanoscale holes orgy at the Location of solid Au catalysts, via the solid-solid-vapor (SSV) mechanism. Importantly, coarsening of the Au particles is negligible due to Limited Au diffusion on the side facets of the nanoscale depressions, suggesting an approach to the growth of uniform hybrid nanowires with control over both diameter and Location. Furthermore, we directly monitor the evolution of the transformation of a nanoribbon into a nanosheet with {1010} facets. This process takes place through a periodic, kinetic roughening transition of the surface, which is controlled by the kinetic competition between surface growth and the transfer of evaporated gases. In total, these observations give new insights into multiple growth processes occurring in this important materials system. C1 [Kim, B. J.; Kim, M. W.] Gwangju Inst Sci & Technol, Sch Mat Sci & Engn, Kwangju, South Korea. [Jang, J. S.] Yeungnam Univ, Dept Elect Engn, LED IT Fus Technol Res Ctr LIFTRC, Gyeongbuk 712749, South Korea. [Stach, E. A.] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. RP Kim, BJ (reprint author), Gwangju Inst Sci & Technol, Sch Mat Sci & Engn, Kwangju, South Korea. EM kimbj@gist.ac.kr; jsjang@ynu.ac.kr; estach@bnl.gov RI Stach, Eric/D-8545-2011 OI Stach, Eric/0000-0002-3366-2153 FU Research Institute for Solar and Sustainable Energies (RISE) at Gwangju Institute of Science and Technology (GIST); National Research Foundation of Korea (NRF) - Korea government [2013R1A1A1007978]; Ministry of Trade, Industry and Energy (MTIE) through the industrial infrastructure program [10033630]; Center for Functional Nanomaterials, Brookhaven National Laboratory; U.S. Department of Energy, Office of Basic Energy Sciences [DE-AC02-98CH10886] FX B. J. Kim acknowledges the support from the Research Institute for Solar and Sustainable Energies (RISE) at Gwangju Institute of Science and Technology (GIST), and the support from the National Research Foundation of Korea (NRF) grant funded by the Korea government (2013R1A1A1007978). B. J. Kim and J. S. Jang acknowledge the support from the Ministry of Trade, Industry and Energy (MTIE) through the industrial infrastructure program under Grant no. 10033630. E.A.S. acknowledges support from 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 30 TC 2 Z9 2 U1 2 U2 42 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 2014 VL 6 IS 12 BP 6984 EP 6990 DI 10.1039/c3nr06628b PG 7 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA AI8FI UT WOS:000337143900092 PM 24837497 ER PT S AU Akl, TJ Wilson, MA Ericson, MN Cote, GL AF Akl, Tony J. Wilson, Mark A. Ericson, M. Nance Cote, Gerard L. BE Cote, GL TI Photoplethysmography beyond Perfusion and Oxygenation Monitoring: Pulse Wave Analysis for Hepatic Graft Monitoring SO OPTICAL DIAGNOSTICS AND SENSING XIV: TOWARD POINT-OF-CARE DIAGNOSTICS SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Optical Diagnostics and Sensing XIV - Toward Point-of-Care Diagnostics CY FEB 03-06, 2014 CL San Francisco, CA SP SPIE DE Photoplethysmography; Pulse waveform; Pulse analysis; Compliance; Graft monitoring ID LIVER-TRANSPLANTATION; IMPLANTABLE SENSOR; CONTOUR ANALYSIS; DISEASE; MICROCIRCULATION; QUANTIFICATION; ELASTOGRAPHY; FIBROSIS; FINGER AB Photoplethysmography is a technique widely used in monitoring perfusion and blood oxygen saturation based on the amplitude of the pulsatile signal at one or multiple wavelengths. However, the pulsatile signal carries in its waveform a substantial amount of information about the mechanical properties of the tissue and vasculature under investigation that is still yet to be utilized to its full potential. In this work, we present the feasibility of pulse wave analysis for the application of monitoring hepatic implants and diagnosing graft complications. In particular, we demonstrate the utility of computing the slope of the pulse during the diastole phase to assess compliance changes in tissue. This hypothesis was tested in a series of in vitro experiments using a polydimethylsiloxane based phantom mimicking the optical and mechanical properties of the portal vein. The emptying time decreased from 148.1 ms for phantoms with compliance of 12 KPa to 97.5 ms for phantoms with compliance of 61 KPa. These compliance levels mimic those seen for normal and fibrotic hepatic tissue respectively. C1 [Akl, Tony J.; Cote, Gerard L.] Texas A&M Univ, Dept Biomed Engn, College Stn, TX 77843 USA. [Wilson, Mark A.] Univ Pittsburgh, Dept Surg, Pittsburgh, PA USA. [Wilson, Mark A.] VA Pittsburgh Healthcare Syst, Pittsburgh, PA USA. [Ericson, M. Nance] Oak Ridge Natl Lab, Oak Ridge, TN USA. RP Akl, TJ (reprint author), Texas A&M Univ, Dept Biomed Engn, College Stn, TX 77843 USA. RI Ericson, Milton/H-9880-2016 OI Ericson, Milton/0000-0002-6628-4865 FU bioengineering research partnership (BRP); NIH [5R01-GM077150] FX This research was funded by a bioengineering research partnership (BRP) grant from NIH, (#5R01-GM077150). NR 28 TC 0 Z9 0 U1 0 U2 2 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9864-9 J9 PROC SPIE PY 2014 VL 8951 AR UNSP 895103 DI 10.1117/12.2039611 PG 6 WC Optics; Radiology, Nuclear Medicine & Medical Imaging SC Optics; Radiology, Nuclear Medicine & Medical Imaging GA BA5JX UT WOS:000336740800002 ER PT J AU Iftekharuddin, KM Awwal, AAS Young, SS Abdulla, GM AF Iftekharuddin, Khan M. Awwal, Abdul A. S. Young, S. Susan Abdulla, Ghaleb M. TI Optical and Hybrid Imaging and Processing for Big Data Problems SO OPTICAL ENGINEERING LA English DT Editorial Material C1 [Iftekharuddin, Khan M.] Old Dominion Univ, Dept Elect & Comp Engn, Norfolk, VA 23529 USA. [Awwal, Abdul A. S.] Lawrence Livermore Natl Lab, NIF, Livermore, CA 94551 USA. [Young, S. Susan] US Army Res Lab, Adelphi, MD 20783 USA. [Abdulla, Ghaleb M.] Lawrence Livermore Natl Lab, Ctr Appl Sci Comp, Livermore, CA 94551 USA. RP Iftekharuddin, KM (reprint author), Old Dominion Univ, Dept Elect & Comp Engn, 231 Kaufman Hall, Norfolk, VA 23529 USA. EM iftekhar@odu.edu; awwal1@llnl.gov; shiqiong.susan.young@us.army.mil; abdulla1@llnl.gov NR 0 TC 0 Z9 0 U1 2 U2 11 PU SPIE-SOC PHOTO-OPTICAL INSTRUMENTATION ENGINEERS PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98225 USA SN 0091-3286 EI 1560-2303 J9 OPT ENG JI Opt. Eng. PD JAN PY 2014 VL 53 IS 1 AR 011001 DI 10.1117/1.OE.53.1.011001 PG 2 WC Optics SC Optics GA AI8LW UT WOS:000337168500003 ER PT J AU Kim, HJ Park, SH Lee, CS AF Kim, Hyung Jun Park, Su Han Lee, Chang Sik TI Light intensity and image visualization of GDI injector sprays according to nozzle hole arrangements SO OPTIK LA English DT Article DE Gasoline direct injection (GDI); Multi-hole injector; Spray characteristics; Atomization ID ENGINE; ATOMIZATION; SYSTEM; MODEL AB The light intensity measurement and image visualization of multi-hole injection spray due to different hole arrangements and hole numbers were investigated. The light intensities and behavior characteristics of the GDI spray were analyzed through the axial and diagonal spray penetration, cone angle, and spray area from the spray images by using the image visualization system and image analysis system. The atomization performance of GDI injectors was analyzed by the local and overall Sauter mean diameter (SMD) measurement. It is revealed that the higher injection pressure shows higher light intensity levels due to the strong vortices and collision by a high injection pressure. The light intensity level at the outer and end region of the spray shows lower value compared to that at the center spray region. In all of test injectors, the increased injection pressure leads to the decrease of the droplet size distribution in the initial spray. But, there is little difference of the droplet size at low and high injection pressure in middle and latter period after the injection. The overall SMD of GDI injectors showed from 14 to 23.14 mu m. (C) 2013 Elsevier GmbH. All rights reserved. C1 [Kim, Hyung Jun] Natl Inst Environm Res, Transportat Pollut Res Ctr, Inchon 404170, South Korea. [Park, Su Han] Argonne Natl Lab, Adv Photon Source, Lemont, IL 60439 USA. [Lee, Chang Sik] Hanyang Univ, Sch Mech Engn, Seoul 133791, South Korea. RP Lee, CS (reprint author), Hanyang Univ, Sch Mech Engn, 17 Haengdang Dong, Seoul 133791, South Korea. EM cslee@hanyang.ac.kr FU National Research Foundation of Korea (NRF) - Korea government (MEST) [2012007015]; Second Brain Korea 21 Project a FX This work was supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MEST) (2012007015) and was supported by the Second Brain Korea 21 Project a. NR 18 TC 1 Z9 1 U1 2 U2 12 PU ELSEVIER GMBH, URBAN & FISCHER VERLAG PI JENA PA OFFICE JENA, P O BOX 100537, 07705 JENA, GERMANY SN 0030-4026 J9 OPTIK JI Optik PY 2014 VL 125 IS 12 BP 2763 EP 2767 DI 10.1016/j.ijleo.2013.11.030 PG 5 WC Optics SC Optics GA AI6AI UT WOS:000336951800010 ER PT J AU Yu, Y Mao, BH Geller, A Chang, R Gaskell, K Liu, Z Eichhorn, BW AF Yu, Yi Mao, Baohua Geller, Aaron Chang, Rui Gaskell, Karen Liu, Zhi Eichhorn, Bryan W. TI CO2 activation and carbonate intermediates: an operando AP-XPS study of CO2 electrolysis reactions on solid oxide electrochemical cells SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID RAY PHOTOELECTRON-SPECTROSCOPY; DOPED CERIA; THIN-FILMS; FUEL-CELL; IN-SITU; TEMPERATURE; REDUCTION; CEO2; ADSORPTION; DIOXIDE AB Through the use of ambient pressure X-ray photoelectron spectroscopy and specially designed ceria-based solid oxide electrochemical cells, carbon dioxide (CO2) electrolysis reactions (CO2 + 2e(-) -> CO + O2-) and carbon monoxide (CO) electro-oxidation reactions (CO + O2- -CO2 + 2e(-)) over cerium oxide electrodes have been investigated in the presence of 0.5 Torr CO-CO2 gas mixtures at similar to 600 degrees C. Carbonate species (CO32-) are identified on the ceria surface as reaction intermediates. When CO2 electrolysis is promoted on ceria electrodes at + 2.0 V applied bias, we observe a higher concentration of CO32- over a 400 mu m-wide active region on the ceria surface, accompanied by Ce3+/Ce4+ redox changes. This increase in the CO32- steady-state concentration suggests that the process of pre-coordination of CO2 to the ceria surface to form a CO32- intermediate (CO2(g) + O-(surface)(2-) -> CO32- ((surface))) precedes a rate-limiting electron transfer process involving CO32- reduction to give CO and oxide ions (CO32- ((surface)) + 2Ce(3+) -> CO(g) + 2O(2-) ((surface)) + 2Ce(4+)). When the applied bias is switched to -1.5 V to promote CO electro-oxidation on ceria, the surface CO32- concentration slightly decreases from the equilibrium value, suggesting that the electron transfer process is also a rate-limiting process in the reverse direction. C1 [Yu, Yi; Geller, Aaron; Gaskell, Karen; Eichhorn, Bryan W.] Univ Maryland, Dept Chem & Biochem, College Pk, MD 20742 USA. [Mao, Baohua; Chang, Rui; Liu, Zhi] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. RP Liu, Z (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. EM zliu2@lbl.gov; eichhorn@umd.edu RI Liu, Zhi/B-3642-2009 OI Liu, Zhi/0000-0002-8973-6561 FU Office of Naval Research [N000140510711]; University of Maryland Nanocenter; University of Maryland Energy Research Center (UMERC); Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC0205CH11231]; National Natural Science Foundation of China [11227902] FX This work was funded through the support of the Office of Naval Research through Contract No. N000140510711 (Dr Michele Anderson program manager). We thank the University of Maryland Nanocenter and the University of Maryland Energy Research Center (UMERC) for their support. 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-AC0205CH11231. R. C. and B. M. thank National Natural Science Foundation of China (No. 11227902) for its support. NR 51 TC 14 Z9 14 U1 12 U2 95 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 2014 VL 16 IS 23 BP 11633 EP 11639 DI 10.1039/c4cp01054j PG 7 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AI3WU UT WOS:000336796800064 PM 24806971 ER PT J AU Han, G Huang, Y Koua, FHM Shen, JR Westlund, PO Messinger, J AF Han, Guangye Huang, Yang Koua, Faisal Hammad Mekky Shen, Jian-Ren Westlund, Per-Olof Messinger, Johannes TI Hydration of the oxygen-evolving complex of photosystem II probed in the dark-stable S-1 state using proton NMR dispersion profiles SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID PHOTOSYNTHETIC WATER OXIDATION; MAGNETIC-RELAXATION DISPERSION; PANCREATIC TRYPSIN-INHIBITOR; ELECTRON-PARAMAGNETIC-RESONANCE; MOLECULAR-DYNAMICS SIMULATIONS; FLASH-INDUCED ENHANCEMENTS; NUCLEAR-SPIN RELAXATION; EPR MULTILINE SIGNAL; SUBSTRATE-WATER; MANGANESE CLUSTER AB The hydration of the oxygen-evolving complex (OEC) was characterized in the dark stable S-1 state of photosystem II using water R-1(omega) NMR dispersion (NMRD) profiles. The R-1(omega) NMRD profiles were recorded over a frequency range from 0.01 MHz to 40 MHz for both intact and Mn-depleted photosystem II core complexes from Thermosynechococcus vulcanus (T. vulcanus). The intact-minus-(Mn)-depleted difference NMRD profiles show a characteristic dispersion from approximately 0.03 MHz to 1 MHz, which is interpreted on the basis of the Solomon-Bloembergen-Morgan (SBM) and the slow motion theories as being due to a paramagnetic enhanced relaxation (PRE) of water protons. Both theories are qualitatively consistent with the S-T = 1, g = 4.9 paramagnetic state previously described for the S-1 state of the OEC; however, an alternative explanation involving the loss of a separate class of long-lived internal waters due to the Mn-depletion procedure can presently not be ruled out. Using a point-dipole approximation the PRE-NMRD effect can be described as being caused by 1-2 water molecules that are located about 10 angstrom away from the spin center of the Mn4CaO5 cluster in the OEC. The application of the SBM theory to the dispersion observed for PSII in the S-1 state is questionable, because the parameters extracted do not fulfil the presupposed perturbation criterion. In contrast, the slow motion theory gives a consistent picture indicating that the water molecules are in fast chemical exchange with the bulk (tau(w) < 1 mu s). The modulation of the zero-field splitting (ZFS) interaction suggests a (restricted) reorientation/ structural equilibrium of the Mn4CaO5 cluster with a characteristic time constant of tau(ZFS) = 0.6-0.9 mu s. C1 [Han, Guangye; Huang, Yang; Westlund, Per-Olof; Messinger, Johannes] Umea Univ, Kemiskt Biol Ctr, Dept Chem, S-90187 Umea, Sweden. [Han, Guangye] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA 94720 USA. [Koua, Faisal Hammad Mekky; Shen, Jian-Ren] Okayama Univ, Fac Sci, Grad Sch Nat Sci & Technol, Dept Biol, Okayama 7008530, Japan. RP Westlund, PO (reprint author), Umea Univ, Kemiskt Biol Ctr, Dept Chem, Linnaeus Vag 6, S-90187 Umea, Sweden. EM perolof.westlund@chem.umu.se; johannes.messinger@chem.umu.se RI Shen, Jian-Ren/B-2558-2011; OI Koua, Faisal Hammad Mekky/0000-0001-8371-9587 FU Artificial Leaf Project Umea (K&A Wallenberg foundation); Solar Fuels strong research environment Umea (Umea University); Energimyndigheten; MEXT/JSPS of Japan [24000018] FX The authors thank Tobias Sparrman and Dmitriy Shevela for technical support. The Kempe foundation is acknowledged for supporting the purchase of the NMRD field cycling instrument and for a postdoc stipend to GH. Further financial support was provided by the Artificial Leaf Project Umea (K&A Wallenberg foundation; JM), the Solar Fuels strong research environment Umea (Umea University; JM), VR (YH, POW, JM) and Energimyndigheten (JM). JRS was supported by a Grant-in-Aid for Specially Promoted Research No. 24000018 from MEXT/JSPS of Japan. Author contributions: JM conceived the experiment, FHMK prepared the PSIIcc in the lab of JRS, GH performed all NMRD and EPR experiments, YH and POW performed the theoretical analysis, the manuscript was written by GH, POW and JM, with contributions from all other authors. NR 102 TC 0 Z9 0 U1 5 U2 14 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 2014 VL 16 IS 24 BP 11924 EP 11935 DI 10.1039/c3cp55232b PG 12 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AI7ZR UT WOS:000337122000012 PM 24695863 ER PT J AU Lewandowska-Andralojc, A Polyansky, DE Wang, CH Wang, WH Himeda, Y Fujita, E AF Lewandowska-Andralojc, Anna Polyansky, Dmitry E. Wang, Chiu-Hui Wang, Wan-Hui Himeda, Yuichiro Fujita, Etsuko TI Efficient water oxidation with organometallic iridium complexes as precatalysts SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID HALF-SANDWICH COMPLEXES; CARBON-DIOXIDE; HETEROGENEOUS CATALYSIS; RUTHENIUM COMPLEXES; ELECTRON-TRANSFER; AMMONIUM-NITRATE; OXIDE CLUSTERS; LIGANDS; HYDROGENATION; OXYGEN AB Catalytic water oxidation has been investigated using five iridium complexes as precatalysts and NaIO4 as an oxidant at various pH conditions. An increase in the activity of all complexes was observed with increasing pH. A detailed analysis of spectroscopic data together with O-2-evolution experiments using Cp*Ir(6,6'-dihydroxy-2,2'-bipyridine)(OH2)(2+) as a precatalyst indicate that the high catalytic activity is closely connected with transient species (A) that exhibits an absorption band at lambda(max) 590 nm. The formation of this active form is strongly dependent on reaction conditions, and the species was distinctly observed using a small excess of periodate. However, another species absorbing at 600 nm (B), which seems to be a less active catalyst, was also observed and was more prominent at high oxidant concentration. Dynamic light scattering analysis and transmission electron microscopy have identified species B as 120 nm nanoparticles. The ultrafiltration method has revealed that species A can be attributed to particles with size in the range of 0.5-2 nm, possibly small IrOx clusters similar to those described previously by Harriman and co-workers C1 [Lewandowska-Andralojc, Anna; Polyansky, Dmitry E.; Wang, Chiu-Hui; Fujita, Etsuko] Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA. [Wang, Wan-Hui; Himeda, Yuichiro] Natl Inst Adv Ind Sci & Technol, Tsukuba, Ibaraki 3058565, Japan. [Wang, Wan-Hui; Himeda, Yuichiro] Japan Sci & Technol Agcy, ACT C, Kawaguchi, Saitama 3320012, Japan. RP Fujita, E (reprint author), Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA. EM fujita@bnl.gov RI Polyansky, Dmitry/C-1993-2009; Lewandowska-Andralojc, Anna/A-8149-2012; Wang, Wan-Hui/J-8773-2012 OI Polyansky, Dmitry/0000-0002-0824-2296; Wang, Wan-Hui/0000-0002-5943-4589 FU U.S. Department of Energy [DE-AC02-98CH10886]; Division of Chemical Sciences, Geosciences, & Biosciences, Office of Basic Energy Sciences; Japan Science and Technology Agency (JST); ACT-C FX We thank Dr James T. Muckerman for a careful reading of this manuscript. Dr Yimei Zhu is acknowledged for providing access to a JEOL JEM3000F TEM. We thank Dr Sergei Lymar for help with calculations of one-electron reduction potentials of periodate. The work at BNL was carried out under contract DE-AC02-98CH10886 with the U.S. Department of Energy and supported by its Division of Chemical Sciences, Geosciences, & Biosciences, Office of Basic Energy Sciences. Y. H. and W.-H. W. thank the Japan Science and Technology Agency (JST), ACT-C for financial support. NR 69 TC 25 Z9 25 U1 1 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 2014 VL 16 IS 24 BP 11976 EP 11987 DI 10.1039/c3cp55101f PG 12 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AI7ZR UT WOS:000337122000017 PM 24549266 ER PT J AU Kharche, N Hybertsen, MS Muckerman, JT AF Kharche, Neerav Hybertsen, Mark S. Muckerman, James T. TI Computational investigation of structural and electronic properties of aqueous interfaces of GaN, ZnO, and a GaN/ZnO alloy SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID DENSITY-FUNCTIONAL THEORY; SOLID-SOLUTION PHOTOCATALYST; INITIO MOLECULAR-DYNAMICS; AUGMENTED-WAVE METHOD; (GA1-XZNX)(N1-XOX) PHOTOCATALYSTS; SURFACE-STRUCTURE; LIQUID WATER; BASIS-SET; OXIDE; 1ST-PRINCIPLES AB The GaN/ZnO alloy functions as a visible-light photocatalyst for splitting water into hydrogen and oxygen. As a first step toward understanding the mechanism and energetics of water-splitting reactions, we investigate the microscopic structure of the aqueous interfaces of the GaN/ZnO alloy and compare them with the aqueous interfaces of pure GaN and ZnO. Specifically, we have studied the (10(1) over bar0) surface of GaN and ZnO and the (10(1) over bar0) and (1(2) over bar10) surfaces of the 1 : 1 GaN/ZnO alloy. The calculations are carried out using first-principles density functional theory based molecular dynamics (DFT-MD). The structure of water within a 3 A distance from the semiconductor surface is significantly altered by the acid/base chemistry of the aqueous interface. Water adsorption on all surfaces is substantially dissociative such that the surface anions (N or O) act as bases accepting protons from dissociated water molecules while the corresponding hydroxide ions bond with surface cations (Ga or Zn). Additionally, the hard-wall interface presented by the semiconductor imparts ripples in the density of water. Beyond a 3 A distance from the semiconductor surface, water exhibits a bulk-like hydrogen bond network and oxygen-oxygen radial distribution function. Taken together, these characteristics represent the resting (or "dark") state of the catalytic interface. The electronic structure analysis of the aqueous GaN/ZnO interface suggests that the photogenerated holes may get trapped on interface species other than the adsorbed OH- ions. This suggests additional dynamical steps in the water oxidation process. C1 [Kharche, Neerav; Muckerman, James T.] Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA. [Hybertsen, Mark S.] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. RP Kharche, N (reprint author), Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA. EM nkharche@bnl.gov; mhyberts@bnl.gov; muckerma@bnl.gov RI Kharche, Neerav/F-4331-2015; OI Kharche, Neerav/0000-0003-1014-6022; Hybertsen, Mark S/0000-0003-3596-9754 FU U.S. Department of Energy [DE-AC02-98CH10886]; Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231] FX We thank P. B. Allen and M. Fernandez-Serra for valuable discussions. This work was carried out at Brookhaven National Laboratory under contract No. DE-AC02-98CH10886 with the U.S. Department of Energy and supported by its Office of Basic Energy Sciences, its Division of Chemical Sciences, its Computational Materials and Chemical Sciences Network program, and its Scientific User Facilities Division. This research utilized resources at the Center for Functional Nanomaterials at Brookhaven National Laboratory and the National Energy Research Scientific Computing Center at Lawrence Berkeley National Laboratory, which is supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. NR 57 TC 7 Z9 7 U1 0 U2 82 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 2014 VL 16 IS 24 BP 12057 EP 12066 DI 10.1039/c4cp00486h PG 10 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AI7ZR UT WOS:000337122000026 PM 24686328 ER PT J AU Salvador, JR Cho, JY Ye, ZX Moczygemba, JE Thompson, AJ Sharp, JW Koenig, JD Maloney, R Thompson, T Sakamoto, J Wang, H Wereszczak, AA AF Salvador, James R. Cho, Jung Y. Ye, Zuxin Moczygemba, Joshua E. Thompson, Alan J. Sharp, Jeffrey W. Koenig, Jan D. Maloney, Ryan Thompson, Travis Sakamoto, Jeffrey Wang, Hsin Wereszczak, Andrew A. TI Conversion efficiency of skutterudite-based thermoelectric modules SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID FIGURE; TESTS; MERIT AB Presently, the only commercially available power generating thermoelectric (TE) modules are based on bismuth telluride (Bi2Te3) alloys and are limited to a hot side temperature of 250 degrees C due to the melting point of the solder interconnects and/ or generally poor power generation performance above this point. For the purposes of demonstrating a TE generator or TEG with higher temperature capability, we selected skutterudite based materials to carry forward with module fabrication because these materials have adequate TE performance and are mechanically robust. We have previously reported the electrical power output for a 32 couple skutterudite TE module, a module that is type identical to ones used in a high temperature capable TEG prototype. The purpose of this previous work was to establish the expected power output of the modules as a function of varying hot and cold side temperatures. Recent upgrades to the TE module measurement system built at the Fraunhofer Institute for Physical Measurement Techniques allow for the assessment of not only the power output, as previously described, but also the thermal to electrical energy conversion efficiency. Here we report the power output and conversion efficiency of a 32 couple, high temperature skutterudite module at varying applied loading pressures and with different interface materials between the module and the heat source and sink of the test system. We demonstrate a 7% conversion efficiency at the module level when a temperature difference of 460 degrees C is established. Extrapolated values indicate that 7.5% is achievable when proper thermal interfaces and loading pressures are used. C1 [Salvador, James R.] GM Global Res & Dev, Chem & Mat Syst Lab, Warren, MI 48090 USA. [Cho, Jung Y.; Ye, Zuxin] Optimal Inc, Plymouth, MI 48170 USA. [Moczygemba, Joshua E.; Thompson, Alan J.; Sharp, Jeffrey W.] Marlow Ind Inc, Dallas, TX 75238 USA. [Koenig, Jan D.] Fraunhofer Inst Phys Measurement Tech, D-79110 Freiburg, Germany. [Maloney, Ryan; Thompson, Travis; Sakamoto, Jeffrey] Michigan State Univ, Dept Chem Engn & Mat Sci, E Lansing, MI 48824 USA. [Wang, Hsin; Wereszczak, Andrew A.] Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. RP Salvador, JR (reprint author), GM Global Res & Dev, Chem & Mat Syst Lab, MC 480-106-224,30500 Mound Rd, Warren, MI 48090 USA. RI Wang, Hsin/A-1942-2013; Wereszczak, Andrew/I-7310-2016 OI Wang, Hsin/0000-0003-2426-9867; Wereszczak, Andrew/0000-0002-8344-092X FU GM; Marlow Industries; DOE [DE-FC26-04NT42278, DE-EE0005432]; Revolutionary Materials for Solid State Energy Conversion, an Energy Frontier Research Center - US Department of Energy, Office of Science, Office of Basic Energy Science [DE-SC001054]; GM Global R&D under the Materials Science and Technology Division; Work-for-Others (WFO) Program [14687701, NFE-12-03934]; U.S. Department of Energy FX JRS, JYC, and ZY would like to thank J. F. Herbst and M. W. Verbrugge for their continued support and encouragement. This work is supported by GM, Marlow Industries (a subsidiary of II-VI Inc.), and by DOE under corporate agreement DE-FC26-04NT42278 and DE-EE0005432. TT and J. Sakamoto would like to acknowledge support from the Revolutionary Materials for Solid State Energy Conversion, an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Office of Basic Energy Science under Award Number DE-SC001054. This research was partially performed at the Oak Ridge National Laboratory (ORNL) and sponsored GM Global R&D under the Materials Science and Technology Division, Work-for-Others (WFO) Program, IAM: 14687701, and DOE agreement: NFE-12-03934, with the U.S. Department of Energy. NR 31 TC 30 Z9 30 U1 7 U2 67 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 2014 VL 16 IS 24 BP 12510 EP 12520 DI 10.1039/c4cp01582g PG 11 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AI7ZR UT WOS:000337122000074 PM 24830880 ER PT J AU van Swol, F Petsev, DN AF van Swol, Frank Petsev, Dimiter N. TI Molecular dynamics simulation of binary hard sphere colloids near the glass transition SO RSC ADVANCES LA English DT Article ID SUPERCOOLED LIQUIDS; HETEROGENEOUS DYNAMICS; CHARACTERISTIC LENGTH; MICROSCOPIC DYNAMICS; RELAXATION; MOTION; MIXTURES; ATOMS; MODEL; TIME AB This study reports on molecular dynamics simulations of concentrated binary hard sphere colloids near the glass transition. We present the three-dimensional mean square displacements for systems that increase in density, into the glass transition region. The molecular dynamics simulations probe wider time scales than the experimentally assessable range. They cover the short time scale that corresponds to ballistic motion, the intermediate scale that corresponds to caged Brownian motion, and the long time diffusion described by the Einstein-Smoluchowski limit. We report results for alpha(2), the non-Gaussian parameter, which captures the details of the mean square displacements around the time that, on average, rearrangements of the particle cages occur. The dynamic temporal correlations were examined in terms of the four point susceptibility. The implications for ageing are also discussed. C1 [van Swol, Frank] Sandia Natl Labs, Albuquerque, NM 87185 USA. [Petsev, Dimiter N.] Univ New Mexico, Dept Chem & Nucl Engn, Albuquerque, NM 87131 USA. RP van Swol, F (reprint author), Sandia Natl Labs, POB 5800, Albuquerque, NM 87185 USA. EM fbvansw@sandia.gov; dimiter@unm.edu FU NSF [CBET 0844645]; Sandia National Laboratories' LDRD program; U.S. Department of Energy's National Nuclear Security Administration [DEAC04-94AL85000] FX The authors are grateful to Dr Christine Roberts for bringing ref. 5 to our attention. This work was funded by NSF (CBET 0844645) and by Sandia National Laboratories' LDRD 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 DEAC04-94AL85000. Finally the authors wish to thank the reviewer for the helpful comments that lead to a much improved final version of this article. NR 37 TC 1 Z9 1 U1 7 U2 19 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 2014 VL 4 IS 41 BP 21631 EP 21637 DI 10.1039/c4ra02391a PG 7 WC Chemistry, Multidisciplinary SC Chemistry GA AI4LO UT WOS:000336837100065 ER PT S AU Lentine, AL Cox, JA Zortman, WA Savignon, DJ AF Lentine, Anthony L. Cox, Jonathan A. Zortman, William A. Savignon, Daniel J. BE Eldada, LA Lee, EH He, S TI Electronic Interfaces to Silicon Photonics SO SMART PHOTONIC AND OPTOELECTRONIC INTEGRATED CIRCUITS XVI SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Smart Photonic and Optoelectronic Integrated Circuits XVI CY FEB 05-06, 2014 CL San Francisco, CA SP SPIE DE Optical interconnects; silicon photonics; optoelectronics ID OPTICAL MODULATORS; HIGH-PERFORMANCE; PHOTODETECTORS; COMPACT; STABILIZATION; RESONATOR; FILTERS; ENERGY; VLSI AB We describe the interface circuits to silicon photonics modulators, optical filters, and detectors that will be required to enable silicon photonics micro-ring and micro-disk devices to be integrated in dense wavelength division multiplexing circuitry C1 [Lentine, Anthony L.; Cox, Jonathan A.; Zortman, William A.; Savignon, Daniel J.] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Lentine, AL (reprint author), Sandia Natl Labs, POB 5800, Albuquerque, NM 87185 USA. NR 54 TC 1 Z9 1 U1 1 U2 3 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9902-8 J9 PROC SPIE PY 2014 VL 8989 AR 89890F DI 10.1117/12.2045696 PG 10 WC Engineering, Electrical & Electronic; Optics SC Engineering; Optics GA BA5MU UT WOS:000336802200010 ER PT S AU Young, AL Hunker, JD Ellis, AR Samora, S Wendt, JR Stick, DL AF Young, Amber L. Hunker, Jeffery D. Ellis, A. Robert Samora, Sally Wendt, Joel R. Stick, Daniel L. BE Eldada, LA Lee, EH He, S TI Precision alignment of integrated optics in surface electrode ion traps for quantum information processing SO SMART PHOTONIC AND OPTOELECTRONIC INTEGRATED CIRCUITS XVI SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Smart Photonic and Optoelectronic Integrated Circuits XVI CY FEB 05-06, 2014 CL San Francisco, CA SP SPIE DE micro-optic integration; off-axis Fresnel zone plates; optical alignment; non-contact alignment; hybrid microsystems; surface electrode ion trap; diffractive optics AB The integration of optics for efficient light delivery and the collection of fluorescence from trapped ions in surface electrode ion traps is a key component to achieving scalability for quantum information processing. Diffractive optical elements (DOEs) present a promising approach as compared to bulk optics because of their small physical profile and their flexibility in tailoring the optical wavefront. The precise alignment of the optics for coupling fluorescence to and from the ions, however, poses a particular challenge. Excitation and manipulation of the ions requires a high degree of optical access, significantly restricting the area available for mounting components. The ion traps, DOEs, and other components are compact, constraining the manipulation of various elements. For efficient fluorescence collection from the ions the DOE must be have a large numerical aperture (NA), which results in greater sensitivity to misalignment. The ion traps are sensitive devices, a mechanical approach to alignment such as contacting the trap and using precision motors to back-off a set distance not only cannot achieve the desired alignment precision, but risks damage to the ion trap. We have developed a non-contact precision optical alignment technique. We use line foci produced by off-axis linear Fresnel zone plates (FZPs) projected on alignment targets etched in the top metal layer of the ion trap and demonstrate micron-level alignment accuracy. C1 [Young, Amber L.; Hunker, Jeffery D.; Ellis, A. Robert; Samora, Sally; Wendt, Joel R.; Stick, Daniel L.] Sandia Natl Labs, Albuquerque, NM 87111 USA. RP Young, AL (reprint author), Sandia Natl Labs, POB 5800, Albuquerque, NM 87111 USA. EM alyoun@sandia.gov NR 7 TC 0 Z9 0 U1 0 U2 3 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9902-8 J9 PROC SPIE PY 2014 VL 8989 AR 89890L DI 10.1117/12.2040795 PG 8 WC Engineering, Electrical & Electronic; Optics SC Engineering; Optics GA BA5MU UT WOS:000336802200016 ER PT J AU Pan, JJ Cheng, XL Monticelli, L Heberle, FA Kucerka, N Tieleman, DP Katsaras, J AF Pan, Jianjun Cheng, Xiaolin Monticelli, Luca Heberle, Frederick A. Kucerka, Norbert Tieleman, D. Peter Katsaras, John TI The molecular structure of a phosphatidylserine bilayer determined by scattering and molecular dynamics simulations SO SOFT MATTER LA English DT Article ID X-RAY-SCATTERING; PARTICLE MESH EWALD; SMALL-ANGLE NEUTRON; LIPID-BILAYERS; CONSTANT-PRESSURE; FORCE-FIELD; PLASMA-MEMBRANE; SURFACE-TENSION; NA+ COUNTERIONS; HYDRATION AB Phosphatidylserine (PS) lipids play essential roles in biological processes, including enzyme activation and apoptosis. We report on the molecular structure and atomic scale interactions of a fluid bilayer composed of 1-palmitoyl-2-oleoyl-sn-glycero-3-phosphatidylserine (POPS). A scattering density profile model, aided by molecular dynamics (MD) simulations, was developed to jointly refine different contrast small-angle neutron and X-ray scattering data, which yielded a lipid area of 62.7 angstrom(2) at 25 degrees C. MD simulations with POPS lipid area constrained at different values were also performed using all-atom and aliphatic united-atom models. The optimal simulated bilayer was obtained using a model-free comparison approach. Examination of the simulated bilayer, which agrees best with the experimental scattering data, reveals a preferential interaction between Na+ ions and the terminal serine and phosphate moieties. Long-range inter-lipid interactions were identified, primarily between the positively charged ammonium, and the negatively charged carboxylic and phosphate oxygens. The area compressibility modulus K-A of the POPS bilayer was derived by quantifying lipid area as a function of surface tension from area-constrained MD simulations. It was found that POPS bilayers possess a much larger K-A than that of neutral phosphatidylcholine lipid bilayers. We propose that the unique molecular features of POPS bilayers may play an important role in certain physiological functions. C1 [Pan, Jianjun] Univ S Florida, Dept Phys, Tampa, FL 33620 USA. [Cheng, Xiaolin; Heberle, Frederick A.; Katsaras, John] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. [Cheng, Xiaolin] Univ Tennessee, Dept Biochem & Cellular & Mol Biol, Knoxville, TN 37996 USA. [Monticelli, Luca] INSERM, UMR S665, F-75015 Paris, France. [Monticelli, Luca] INTS, Paris, France. [Kucerka, Norbert] CNR, Canadian Neutron Beam Ctr, Chalk River, ON K0J 1J0, Canada. [Kucerka, Norbert] Comenius Univ, Fac Pharm, Dept Phys Chem Drugs, Bratislava 83232, Slovakia. [Tieleman, D. Peter] Univ Calgary, Dept Biol Sci, Calgary, AB T2N 1N4, Canada. [Tieleman, D. Peter] Univ Calgary, Ctr Mol Simulat, Calgary, AB T2N 1N4, Canada. [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 RI Tieleman, D. Peter/A-4790-2011; OI Tieleman, D. Peter/0000-0001-5507-0688; Katsaras, John/0000-0002-8937-4177; Monticelli, Luca/0000-0002-6352-4595 FU GENCI-CINES [2012-076353]; Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]; Laboratory Directed Research and Development Program of Oak Ridge National Laboratory (ORNL); U.S. Department of Energy (DOE) [DE-AC05-00OR2275]; DOE Office of Biological and Environmental Research (BER); Scientific User Facilities Division of the DOE Office of Basic Energy Sciences (BES); National Science Foundation; National Institutes of Health/National Institute of General Medical Sciences under NSF [DMR-0936384]; Natural Sciences and Engineering Research Council (Canada) FX We thank John Nagle and Drew Marquardt for discussions. Simulations using the GROMACS force field were performed partly using HPC resources from GENCI-CINES (Grant 2012-076353). Simulations using the CHARMM force field 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. Support was received from the Laboratory Directed Research and Development Program (J.K.) 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. This work acknowledges additional support from the DOE Office of Biological and Environmental Research (BER), for use of the Bio-SANS instrument at the ORNL Center for Structural Molecular Biology (CSMB), and from the Scientific User Facilities Division of the DOE Office of Basic Energy Sciences (BES), for use of the EQ-SANS instrument at the ORNL Spallation Neutron Source. SAXS data were collected 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-0936384. DPT is an Alberta Innovates Health Solutions Scientist and Alberta Innovate Technology Futures Strategic Chair in (Bio) Molecular Simulation. Work in DPT's group is supported by the Natural Sciences and Engineering Research Council (Canada). NR 53 TC 25 Z9 25 U1 5 U2 49 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 2014 VL 10 IS 21 BP 3716 EP 3725 DI 10.1039/c4sm00066h PG 10 WC Chemistry, Physical; Materials Science, Multidisciplinary; Physics, Multidisciplinary; Polymer Science SC Chemistry; Materials Science; Physics; Polymer Science GA AI4OT UT WOS:000336845400004 PM 24807693 ER PT J AU Lee, H Tsouris, V Lim, Y Mustafa, R Choi, J Choi, YH Park, HW Meron, M Lin, BH Won, YY AF Lee, Hoyoung Tsouris, Vasilios Lim, Yunho Mustafa, Rafid Choi, Je Choi, Yun Hwa Park, Hae-Woong Meron, Mati Lin, Binhua Won, You-Yeon TI Macroscopic lateral heterogeneity observed in a laterally mobile immiscible mixed polyelectrolyte-neutral polymer brush SO SOFT MATTER LA English DT Article ID CONSISTENT-FIELD THEORY; OPPOSITELY CHARGED POLYMERS; AIR-WATER-INTERFACE; NANOSCALE HETEROGENEITIES; COLLOID STABILIZATION; DIBLOCK COPOLYMER; COATED SURFACES; SOLVENT; SEGREGATION; LAYERS AB We studied mixed poly(ethylene oxide) (PEO) and poly(2-(dimethylamino) ethyl methacrylate) (PDMAEMA) brushes. The question we attempted to answer was: when the chain grafting points are laterally mobile, how will this lateral mobility influence the structure and phase behavior of the mixed brush? Three different model mixed PEO/PDMAEMA brush systems were prepared: (1) a laterally mobile mixed brush by spreading onto the air-water interface a mixture of poly(ethylene oxide)-poly(n-butyl acrylate) (PEO-PnBA) and poly(2-(dimethylamino) ethyl methacrylate)-poly(n-butyl acrylate) (PDMAEMA-PnBA) diblock copolymers (the specific diblock copolymers used will be denoted as PEO113-PnBA(100) and PDMAEMA(118)-PnBA(100), where the subscripts refer to the number-average degrees of polymerization of the individual blocks), (2) a mobility-restricted (inseparable) version of the above mixed brush prepared using a PEO-PnBA-PDMAEMA triblock copolymer (denoted as PEO113-PnBA(89)-PDMAEMA(120)) having respective brush molecular weights matched with those of the diblock copolymers, and (3) a different laterally mobile mixed PEO and PDMAEMA brush prepared from a PEO113-PnBA(100) and PDMAEMA(200)-PnBA(103) diblock copolymer combination, which represents a further more height-mismatched mixed brush situation than described in (1). These three mixed brush systems were investigated by surface pressure-area isotherm and X-ray (XR) reflectivity measurements. These experimental data were analyzed within the theoretical framework of a continuum self-consistent field (SCF) polymer brush model. The combined experimental and theoretical results suggest that the mobile mixed brush derived using the PEO113-PnBA(100) and PDMAEMA(118)-PnBA(100) combination (i.e., mixed brush System #1) undergoes a lateral macroscopic phase separation at high chain grafting densities, whereas the more height-mismatched system (System #3) is only microscopically phase separated under comparable brush density conditions even though the lateral mobility of the grafted chains is unrestricted. The macroscopic phase separation observed in the laterally mobile mixed brush system is in contrast with the microphase separation behavior commonly observed in two-dimensional laterally mobile charged small molecule mixtures. Further study is needed to determine the detailed morphologies of the macro- and microphase-separated mixed PEO/PDMAEMA brushes. C1 [Lee, Hoyoung; Tsouris, Vasilios; Lim, Yunho; Mustafa, Rafid; Choi, Je; Choi, Yun Hwa; Park, Hae-Woong; Won, You-Yeon] Purdue Univ, Sch Chem Engn, W Lafayette, IN 47907 USA. [Meron, Mati; Lin, Binhua] Univ Chicago, Adv Photon Source, Argonne, IL 60439 USA. RP Won, YY (reprint author), Purdue Univ, Sch Chem Engn, W Lafayette, IN 47907 USA. EM yywon@ecn.purdue.edu FU National Science Foundation (NSF) [DMR-0906567, CBET-1264336]; National Science Foundation/Department of Energy [NSF/CHE-0822838]; U. S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357] FX The authors would like to thank the National Science Foundation (NSF) for providing financial support for this research (DMR-0906567, and CBET-1264336). ChemMatCARS Sector 15 at the Advanced Photon Source of Argonne National Laboratory (where the XR measurements reported in this paper were made) is principally supported by the National Science Foundation/Department of Energy under grant number NSF/CHE-0822838. 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. NR 71 TC 5 Z9 5 U1 4 U2 37 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 2014 VL 10 IS 21 BP 3771 EP 3782 DI 10.1039/c4sm00022f PG 12 WC Chemistry, Physical; Materials Science, Multidisciplinary; Physics, Multidisciplinary; Polymer Science SC Chemistry; Materials Science; Physics; Polymer Science GA AI4OT UT WOS:000336845400010 PM 24695635 ER PT J AU Lin, YH Yager, KG Stewart, B Verduzco, R AF Lin, Yen-Hao Yager, Kevin G. Stewart, Bridget Verduzco, Rafael TI Lamellar and liquid crystal ordering in solvent-annealed all-conjugated block copolymers SO SOFT MATTER LA English DT Article ID ROD-COIL; MICROPHASE SEPARATION; MAGNETIC ALIGNMENT; DIBLOCK COPOLYMER; THIN-FILMS; POLY(3-HEXYLTHIOPHENE); POLY(9,9-DI-N-OCTYL-2,7-FLUORENE); CRYSTALLIZATION; MORPHOLOGY; MOBILITY AB All-conjugated block copolymers are an emerging class of polymeric materials promising for organic electronic applications, but further progress requires a better understanding of their microstructure including crystallinity and self-assembly through micro-phase segregation. Here, we demonstrate remarkable changes in the thin film structure of a model series of all-conjugated block copolymers with varying processing conditions. Under thermal annealing, poly(3-hexylthiophene)-b-poly(9',9'-dioctylfluorene) (P3HT-b-PF) all-conjugated block copolymers exhibit crystalline features of P3HT or PF, depending on the block ratio, and poor pi-pi stacking. Under chloroform solvent annealing, the block copolymers exhibit lamellar ordering, as evidenced by multiple reflections in grazing incidence wide- and small-angle X-ray scattering (GIWAXS and GISAXS), including an in-plane reflection indicative of order along the pi-pi stacking direction for both P3HT and PF blocks. The lamellae have a characteristic domain size of 4.2 nm, and this domain size is found to be independent of block copolymer molecular weight and block ratio. This suggests that lamellar self-assembly arises due to a combination of polymer block segregation and pi-pi stacking of both P3HT and PF polymer blocks. Strategies for predicting the microstructure of all-conjugated block copolymers must take into account intermolecular pi-pi stacking and liquid crystalline interactions not typically found in flexible coil block copolymers. C1 [Lin, Yen-Hao; Stewart, Bridget; Verduzco, Rafael] Rice Univ, Dept Chem & Biomol Engn, Houston, TX 77005 USA. [Yager, Kevin G.] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. RP Verduzco, R (reprint author), Rice Univ, Dept Chem & Biomol Engn, MS-362,6100 Main St, Houston, TX 77005 USA. EM rafaelv@rice.edu RI Yager, Kevin/F-9804-2011 OI Yager, Kevin/0000-0001-7745-2513 FU National Science Foundation [CBET-1264703]; Louis and Peaches Owen; U.S. Department of Energy, Office of Basic Energy Sciences [DE-AC02-98CH10886]; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]; Department of Homeland Security, Office of Science and Technology [2009-ST-000031] FX This work was supported by the National Science Foundation under Grant no. CBET-1264703 and Louis and Peaches Owen. Research carried out in part at the Center for Functional Nanomaterials and National Synchrotron Light Source, Brookhaven National Laboratory, which is supported by the U.S. Department of Energy, Office of Basic Energy Sciences, under Contract no. DE-AC02-98CH10886. Use of 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. B.S. acknowledges the support of the Department of Homeland Security, Office of Science and Technology, Award # 2009-ST-000031. NR 48 TC 13 Z9 13 U1 6 U2 82 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 2014 VL 10 IS 21 BP 3817 EP 3825 DI 10.1039/c3sm53090f PG 9 WC Chemistry, Physical; Materials Science, Multidisciplinary; Physics, Multidisciplinary; Polymer Science SC Chemistry; Materials Science; Physics; Polymer Science GA AI4OT UT WOS:000336845400014 PM 24718905 ER PT J AU Deshmukh, SA Kamath, G Sankaranarayanan, SKRS AF Deshmukh, Sanket A. Kamath, Ganesh Sankaranarayanan, Subramanian K. R. S. TI Comparison of the interfacial dynamics of water sandwiched between static and free-standing fully flexible graphene sheets SO SOFT MATTER LA English DT Article ID INITIO MOLECULAR-DYNAMICS; EMPIRICAL FORCE-FIELD; LIQUID WATER; MONTE-CARLO; AB-INITIO; X-RAY; VIBRATIONAL-SPECTRA; NUCLEIC-ACIDS; SIMULATION; TEMPERATURE AB Classical molecular dynamics simulations are used to present a detailed atomistic picture of the instantaneous local structures of water and the structural evolution of stationary and dynamically evolving graphene-water interfaces. The confinement effects are strongly coupled to the nature of the interface, which eventually governs its nanoscopic structural arrangements and interface dynamics. We show that the structure, transport properties, and vibrational densities of states of proximal water molecules are strongly correlated with the nature of the graphene-water interface. We identify and correlate features in vibrational spectra with characteristic structural features observed at the atomic scale for the confined water molecules near a stationary and dynamically evolving hydrophobic surface such as graphene. Our simulations indicate that the local orientation, ordering, and solvation dynamics of interfacial water molecules are a strong function of the graphene slit-width, which is controlled by the nature of the interface (fully flexible vs. static). A monotonic decrease in local ordering with increasing slit-width was observed for the static graphene-water interface, whereas a non-monotonic variation was seen for its fully flexible counterpart. The simulation results offer useful insights into the effect of interfacial dynamics in defining the structure and transport properties at graphene-aqueous media interfaces. Finally these simulations provide a molecular level interpretation of the differential confinement effects arising from the dynamically evolving graphene-water interface. C1 [Deshmukh, Sanket A.; Sankaranarayanan, Subramanian K. R. S.] Argonne Natl Lab, Ctr Nanoscale Mat, Argonne, IL 60439 USA. [Kamath, Ganesh] Univ Missouri, Dept Chem, Columbia, MO 65211 USA. RP Sankaranarayanan, SKRS (reprint author), Argonne Natl Lab, Ctr Nanoscale Mat, 9700 S Cass Ave, Argonne, IL 60439 USA. EM skrssank@anl.gov FU U. S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357] FX 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. The authors thank the computational facilities provided by CNM-ANL. NR 62 TC 2 Z9 2 U1 3 U2 28 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 2014 VL 10 IS 23 BP 4067 EP 4083 DI 10.1039/c3sm53044b PG 17 WC Chemistry, Physical; Materials Science, Multidisciplinary; Physics, Multidisciplinary; Polymer Science SC Chemistry; Materials Science; Physics; Polymer Science GA AI4PE UT WOS:000336846500004 PM 24845025 ER PT J AU Wang, Z Chiang, WS Le, PS Fratini, E Li, MD Alatas, A Baglioni, P Chen, SH AF Wang, Zhe Chiang, Wei-Shan Le, Peisi Fratini, Emiliano Li, Mingda Alatas, Ahmet Baglioni, Piero Chen, Sow-Hsin TI One role of hydration water in proteins: key to the "softening" of short time intraprotein collective vibrations of a specific length scale SO SOFT MATTER LA English DT Article ID X-RAY-SCATTERING; DYNAMICS; MOTIONS; RESOLUTION; EXCITATION; SOLVATION; MYOGLOBIN; POWDERS; MODEL; DNA AB High resolution inelastic X-ray scattering (IXS) experiments show that the "phonon energy softening" and "phonon population enhancement"observed in a hydrated native protein when increasing the temperature from 200 K to physiological temperature are not directly related to the protein structure. Such phenomena were also observed in a denatured sample without a defined tertiary structure and with a limited residual secondary structure. However, in a dry sample, such "softening" is strongly suppressed. These facts suggest that the above-mentioned protein "softening" phenomenon is water-induced. In addition, increasing the hydration level can also induce "phonon energy softening" at room temperature, but not at 200 K. This change may be due to a qualitative difference in the dynamics of hydration water at 200 K and at room temperature. C1 [Wang, Zhe; Chiang, Wei-Shan; Le, Peisi; Li, Mingda; Chen, Sow-Hsin] MIT, Dept Nucl Sci & Engn, Cambridge, MA 02139 USA. [Fratini, Emiliano; Baglioni, Piero] Univ Florence, Dept Chem, I-50019 Florence, Italy. [Fratini, Emiliano; Baglioni, Piero] Univ Florence, CSGI, I-50019 Florence, Italy. [Alatas, Ahmet] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. RP Chen, SH (reprint author), MIT, Dept Nucl Sci & Engn, 77 Massachusetts Ave, Cambridge, MA 02139 USA. EM sowhsin@mit.edu RI Baglioni, Piero/B-1208-2011; OI Baglioni, Piero/0000-0003-1312-8700; Wang, Zhe/0000-0003-4103-0751 FU Basic Energy Sciences Division of US DOE [DE-FG02-90ER45429]; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]; Ministero dell'Istruzione, dell'Universita e della Ricerca Scientica (MiUR); Consorzio Interuniversitario per lo Sviluppo dei Sistemi a Grande Interfase (CSGI) FX The research at MIT was supported by a grant from the Basic Energy Sciences Division of US DOE DE-FG02-90ER45429. The work at 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. E.F. and P.B. acknowledge financial support from Ministero dell'Istruzione, dell'Universita e della Ricerca Scientica (MiUR), and Consorzio Interuniversitario per lo Sviluppo dei Sistemi a Grande Interfase (CSGI). NR 37 TC 4 Z9 4 U1 0 U2 18 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 2014 VL 10 IS 24 BP 4298 EP 4303 DI 10.1039/c4sm00257a PG 6 WC Chemistry, Physical; Materials Science, Multidisciplinary; Physics, Multidisciplinary; Polymer Science SC Chemistry; Materials Science; Physics; Polymer Science GA AI7WP UT WOS:000337112600009 PM 24789017 ER PT S AU Mniszewski, SM Del Valle, SY Priedhorsky, R Hyman, JM Hickman, KS AF Mniszewski, Susan M. Del Valle, Sara Y. Priedhorsky, Reid Hyman, James M. Hickman, Kyle S. BE Dabbaghian, V Mago, VK TI Understanding the Impact of Face Mask Usage Through Epidemic Simulation of Large Social Networks SO THEORIES AND SIMULATIONS OF COMPLEX SOCIAL SYSTEMS SE Intelligent Systems Reference Library LA English DT Article; Book Chapter ID PANDEMIC INFLUENZA; SURGICAL MASKS; N95 RESPIRATORS; PERFORMANCE; OUTBREAK; FILTER AB Evidence from the 2003 SARS epidemic and 2009 H1N1 pandemic shows that face masks can be an effective non-pharmaceutical intervention in minimizing the spread of airborne viruses. Recent studies have shown that using face masks is correlated to an individual's age and gender, where females and older adults are more likely to wear a mask than males or youths. There are only a few studies quantifying the impact of using face masks to slow the spread of an epidemic at the population level, and even fewer studies that model their impact in a population where the use of face masks depends upon the age and gender of the population. We use a state-of- the-art agent-based simulation to model the use of face masks and quantify their impact on three levels of an influenza epidemic and compare different mitigation scenarios. These scenarios involve changing the demographics of mask usage, the adoption of mask usage in relation to a perceived threat level, and the combination of masks with other non-pharmaceutical interventions such as hand washing and social distancing. Our results shows that face masks alone have limited impact on the spread of influenza. However, when face masks are combined with other interventions such as hand sanitizer, they can be more effective. We also observe that monitoring social internet systems can be a useful technique to measure compliance. We conclude that educating the public on the effectiveness of masks to increase compliance can reduce morbidity and mortality. C1 [Mniszewski, Susan M.; Del Valle, Sara Y.; Priedhorsky, Reid] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Hyman, James M.; Hickman, Kyle S.] Tulane Univ, New Orleans, LA 70118 USA. RP Mniszewski, SM (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM smm@lanl.gov; sdelvall@lanl.gov; reidpr@lanl.gov; myhyman@tulane.edu; khickman@tulane.edu NR 46 TC 3 Z9 3 U1 0 U2 0 PU SPRINGER-VERLAG BERLIN PI BERLIN PA HEIDELBERGER PLATZ 3, D-14197 BERLIN, GERMANY SN 1868-4394 BN 978-3-642-39149-1; 978-3-642-39148-4 J9 INTEL SYST REF LIBR PY 2014 VL 52 BP 97 EP 115 DI 10.1007/978-3-642-39149-1_8 D2 10.1007/978-3-642-39149-1 PG 19 WC Computer Science, Artificial Intelligence SC Computer Science GA BA3KB UT WOS:000334314900008 ER PT J AU Liu, J Ruhl, E Hitchcock, AP Mcllroy, DN Bozek, JD Tyliszczak, T Knop-Gericke, A Boag, NM Dowben, PA AF Liu, Jing Ruehl, Eckart Hitchcock, Adam P. Mcllroy, David N. Bozek, John D. Tyliszczak, Tolek Knop-Gericke, Axel Boag, Neil M. Dowben, Peter A. TI Double Cation Formation from the Photo-Fragmentation of the closo-Carboranes SO ZEITSCHRIFT FUR PHYSIKALISCHE CHEMIE-INTERNATIONAL JOURNAL OF RESEARCH IN PHYSICAL CHEMISTRY & CHEMICAL PHYSICS LA English DT Article DE Decomposition; Ionic Fragmentation; closo-Carboranes; Ionic Fragmentation Energetics; PEPIPICO ID INNER-SHELL EXCITATION; CORE-LEVEL EXCITATION; MASS-SPECTROMETRY; DOUBLE PHOTOIONIZATION; DISSOCIATION DYNAMICS; IONIC FRAGMENTATION; CHARGE SEPARATION; ARGON CLUSTERS; BORON-CARBIDE; 30.4 NM AB Time-of-flight mass analysis with multi-stop coincidence detection has been used to study the multi-cation ionic fragmentation via fission of three isomeric carborane icosahedral cage compounds closo-1,2-orthocarborane, closo-1,7-metacarborane, closo-1,12-paracarborane (C2B10H12) following inner-shell excitation at or above the B is regime. Photoelectron-photoion-photoion coincidence (PEPIPICO) spectroscopy was used to study the dominant fission routes in the core level excitation regime. Series of ion pairs are identified, where asymmetric fission dominates, leading to ion pairs of different mass. The fragmentation yields and charge separation mass spectra of all three isomers are generally quite similar in that the ion pairs (H+, Y+), Y-11(+)), and (Y-3(+), Y-9(+)) dominate, where denotes the mass region from B+ to CH. Slight differences are observed at the B 1s-threshold, where the H+ and BH2+/CH+ ion pairs dominate for ortho-and metacarborane, while (Y+, Y-11(+)) ion pairs dominate the multi-photofragment ion yield of paracarborane. These similarities and distinct differences in charge separation are discussed by considering the energetics of these three major species of ion pairs, as well as charge distributions in closo-carboranes and charge distributions in the carborane cage. It is shown that product formation via charge separation is driven by electronic relaxation, so that the lowest energy products are not necessarily formed. C1 [Ruehl, Eckart] Free Univ Berlin, Inst Chem & Biochem, D-14195 Berlin, Germany. [Liu, Jing; Dowben, Peter A.] Univ Nebraska, Dept Phys & Astron, Lincoln, NE 68588 USA. [Liu, Jing; Dowben, Peter A.] Univ Nebraska, Nebraska Ctr Mat & Nanosci, Lincoln, NE 68588 USA. [Hitchcock, Adam P.] McMaster Univ, Dept Chem & Chem Biol, Hamilton, ON L8S 4M1, Canada. [Mcllroy, David N.] Univ Idaho, Dept Phys, Moscow, ID 83844 USA. [Bozek, John D.] LCLS Project, Stanford Linear Accelerator, Menlo Pk, CA 94025 USA. [Tyliszczak, Tolek] Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 91420 USA. [Knop-Gericke, Axel] Max Planck Gesell, Fritz Haber Inst, D-14195 Berlin, Germany. [Boag, Neil M.] Univ Salford, Mat & Phys Res Ctr, Salford M5 4WT, Lancs, England. RP Ruhl, E (reprint author), Free Univ Berlin, Inst Chem & Biochem, Takustr 3, D-14195 Berlin, Germany. EM ruehl@zedat.fu-berlin.de RI Liu, Jing/E-7184-2016; Bozek, John/E-9260-2010 OI Bozek, John/0000-0001-7486-7238 FU Defense Threat Reduction Agency [HDTRA1-09-1-0060]; Deutsche Forschungsgemeinschaft [RU 420/8-1]; National Aeronautics and Space Administration [13-EPSCoR-0012]; Office of Energy Research, Office of Basic Energy Sciences, Materials Sciences Division of the US Department of Energy [DE-AC02-05CH11231]; Fonds der Chemischen Industrie FX Die Autoren mochten die Atmosphare und die engagierten Diskussionen in den Kellerburos und Laboren der Takustrafsse 3 wurdigen. Spezieller Dank gebuhrt Klaus Rademann fur seine grundlegende Rolle in der Clusterchemie, fortfuhrt von einigen Autoren dieses Artikels (P. A. D. + E. R). This work was supported by the Defense Threat Reduction Agency (Grant No. HDTRA1-09-1-0060), the Deutsche Forschungsgemeinschaft through grant RU 420/8-1, the Fonds der Chemischen Industrie and the National Aeronautics and Space Administration through grant 13-EPSCoR-0012. Data were acquired at ALS beamline 9.1. The Advanced Light Source is supported by the Director, Office of Energy Research, Office of Basic Energy Sciences, Materials Sciences Division of the US Department of Energy, under Contract No. DE-AC02-05CH11231. The authors thank David Kilcoyne for his contributions to the PEPIPICO instrumentation. NR 37 TC 1 Z9 1 U1 0 U2 8 PU WALTER DE GRUYTER GMBH PI BERLIN PA GENTHINER STRASSE 13, D-10785 BERLIN, GERMANY SN 0942-9352 J9 Z PHYS CHEM JI Z. Phys. Chemie-Int. J. Res. Phys. Chem. Chem. Phys. PY 2014 VL 228 IS 4-5 SI SI BP 421 EP 436 DI 10.1515/zpch-2014-0447 PG 16 WC Chemistry, Physical SC Chemistry GA AI5YY UT WOS:000336948100008 ER PT J AU Lane, JMD Grest, GS AF Lane, J. Matthew D. Grest, Gary S. TI Assembly of responsive-shape coated nanoparticles at water surfaces SO NANOSCALE LA English DT Article ID MOLECULAR-DYNAMICS; GOLD NANOPARTICLES; SIMULATIONS; MEMBRANES; POLYMER; MONOLAYERS; MODEL AB Nanoparticle (NP) assembly and aggregation can be controlled using a variety of organic coatings that bind to the nanoparticle surface and alter its affinity for solvent and other particles. We show that surprisingly simple short chain polymer coatings can be effectively used to selectively control the aggregation of very small nanoparticles by taking advantage of the environment-responsive shape produced by the coating's spontaneous asymmetry on high-curvature nanoparticles. Using extremely long molecular dynamics simulations of alkanethiol coated Au nanoparticles, we show that varying the terminal groups of a nanoparticle coating dramatically alters the coating shape at the water liquid-vapor interface, producing very different assembly morphologies. NPs with CH3-terminated coatings assemble into short linear groupings with a highly aligned structure at early time and then form more disordered clusters as these linear groupings further assemble. NPs with COOH-terminated coatings assemble into dimers and disordered clumps with no preferred alignment at short time and longer disordered chains of particles at longer times. We also find that the responsive shape of the coating continues to adapt to local environment during assembly. The orientations of chains within NP coatings are significantly different when the NPs are arranged in aggregates than when they are isolated. C1 [Lane, J. Matthew D.; Grest, Gary S.] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Lane, JMD (reprint author), Sandia Natl Labs, POB 5800, Albuquerque, NM 87185 USA. EM jlane@sandia.gov FU Office of Science of the United States Department of Energy [DE-AC02-05CH11231]; Lockheed Martin Corporation; U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX This work was performed, in part, at the Center for Integrated Nanotechnology, a U.S. Department of Energy and Office of Basic Energy Sciences user facility. This research used resources obtained through the Advanced Scientific Computing Research (ASCR) Leadership Computing Challenge (ALCC) at the National Energy Research Scientific Computing Center (NERSC), which is supported by the Office of Science of the United States Department of Energy under Contract no. DE-AC02-05CH11231. 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 29 TC 12 Z9 12 U1 1 U2 58 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 2014 VL 6 IS 10 BP 5132 EP 5137 DI 10.1039/c3nr04658c PG 6 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA AG1BB UT WOS:000335148800017 PM 24503935 ER PT J AU Birarda, G Bedolla, DE Mitri, E Pacor, S Grenci, G Vaccari, L AF Birarda, Giovanni Bedolla, Diana E. Mitri, Elisa Pacor, Sabrina Grenci, Gianluca Vaccari, Lisa TI Apoptotic pathways of U937 leukemic monocytes investigated by infrared microspectroscopy and flow cytometry SO ANALYST LA English DT Article ID PROGRAMMED CELL-DEATH; MEMBRANE-FLUIDITY; LIVE CELLS; MICRO-SPECTROSCOPY; CYCLE; FTIR; DISEASES; ABSORPTION; TRANSITION; MECHANISMS AB Apoptosis is a strictly regulated cell death mechanism that plays a pivotal role in the normal evolution of multicellular organisms. Its misregulation has been associated with many diseases, making its early and reliable detection a key point for modern cellular biology. In this paper, we propose the use of infrared microspectroscopy (IRMS) as a label-free methodology for the detection of apoptotic-related biochemical processes induced on U937 leukemic monocytes by serum starvation and CCCP-exposure. The spectroscopic results are in agreement with parallel Flow Cytometry (FC) experiments, where plasma membrane integrity and mitochondrial activity were assessed. Spectroscopic outcomes complement FC data and allow drawing a more complete picture of the apoptotic pathways. In particular, we established that the two apoptosis-inducing treatments, cell starvation and CCCP exposure, affect the cell cycle in a different way. With the former, cell death is preceded by a cell cycle arrest, whereas the latter causes an increased cell cycle progression. Spectral data demonstrate that for both conditions apoptosis proceeds through the accumulation of lipid droplets within cells. Moreover, we were able to establish a spectral marker for DNA condensation/ fragmentation: the enhancement of the PhI band component centred at similar to 1206 cm(-1), which is more sensitive than the relative intensity of the PhII band to which phospholipids and carbohydrates also contribute significantly. In conclusion, we demonstrate that the intrinsic multi-parametric nature of IRMS and its application on cells under physiological conditions can be well exploited for the investigation of apoptotic pathways. C1 [Birarda, Giovanni; Bedolla, Diana E.; Vaccari, Lisa] SISSI Beamline, Elettra Sincrotrone Trieste, I-34149 Trieste, Italy. [Birarda, Giovanni] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Mitri, Elisa; Pacor, Sabrina] Univ Trieste, I-34100 Trieste, Italy. [Mitri, Elisa; Grenci, Gianluca] CNR, IOM, TASC Lab, I-34149 Trieste, Italy. [Grenci, Gianluca] Natl Univ Singapore, Mechanobiol Inst MBI, Singapore 117548, Singapore. RP Vaccari, L (reprint author), SISSI Beamline, Elettra Sincrotrone Trieste, SS 14 Km 163-5, I-34149 Trieste, Italy. EM lisa.vaccari@elettra.eu OI PACOR, SABRINA/0000-0001-8043-6725; Bedolla Orozco, Diana Eva/0000-0003-1902-1517 NR 70 TC 9 Z9 9 U1 2 U2 14 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 0003-2654 EI 1364-5528 J9 ANALYST JI Analyst PY 2014 VL 139 IS 12 BP 3097 EP 3106 DI 10.1039/c4an00317a PG 10 WC Chemistry, Analytical SC Chemistry GA AI3CZ UT WOS:000336737900022 PM 24781500 ER PT J AU Gunsolus, IL Hu, DH Mihai, C Lohse, SE Lee, CS Torelli, MD Hamers, RJ Murhpy, CJ Orr, G Haynes, CL AF Gunsolus, Ian L. Hu, Dehong Mihai, Cosmin Lohse, Samuel E. Lee, Chang-soo Torelli, Marco D. Hamers, Robert J. Murhpy, Catherine J. Orr, Galya Haynes, Christy L. TI Facile method to stain the bacterial cell surface for super-resolution fluorescence microscopy SO ANALYST LA English DT Article ID OPTICAL RECONSTRUCTION MICROSCOPY; LOCALIZATION ANALYSIS; ESCHERICHIA-COLI; NANOPARTICLES; PROBES; LIMIT AB A method to fluorescently stain the surfaces of both Gram-negative and Gram-positive bacterial cells compatible with super-resolution fluorescence microscopy is presented. This method utilizes a commercially-available fluorescent probe to label primary amines at the surface of the cell. We demonstrate efficient staining of two bacterial strains, the Gram-negative Shewanella oneidensis MR-1 and the Gram-positive Bacillus subtilis 168. Using structured illumination microscopy and stochastic optical reconstruction microscopy, which require high quantum yield or specialized dyes, we show that this staining method may be used to resolve the bacterial cell surface with sub-diffraction-limited resolution. We further use this method to identify localization patterns of nanomaterials, specifically cadmium selenide quantum dots, following interaction with bacterial cells. C1 [Gunsolus, Ian L.; Haynes, Christy L.] Univ Minnesota, Dept Chem, Minneapolis, MN 55455 USA. [Hu, Dehong; Mihai, Cosmin; Orr, Galya] Pacific NW Natl Lab, Environm Mol Sci Lab, Richland, WA 99354 USA. [Lohse, Samuel E.; Murhpy, Catherine J.] Univ Illinois, Dept Chem, Urbana, IL 61801 USA. [Lee, Chang-soo; Torelli, Marco D.; Hamers, Robert J.] Univ Wisconsin, Dept Chem, Madison, WI 53706 USA. RP Haynes, CL (reprint author), Univ Minnesota, Dept Chem, 207 Pleasant St SE, Minneapolis, MN 55455 USA. EM chaynes@umn.edu RI Hu, Dehong/B-4650-2010; Hamers, Robert/C-6466-2008; OI Hu, Dehong/0000-0002-3974-2963; Hamers, Robert/0000-0003-3821-9625; Haynes, Christy/0000-0002-5420-5867 FU National Science Foundation [CHE-1240151]; NIEHS [1RC2ES018786-01]; University of Minnesota Biotechnology Institute; Department of Energy's Office of Biological and Environmental Research and located at PNNL FX This work was funded by a grant from the National Science Foundation to the Center for Sustainable Nanotechnology, CHE-1240151. Galya Orr acknowledges partial support from NIEHS grant 1RC2ES018786-01. I. L. G. acknowledges partial support from a training grant from the University of Minnesota Biotechnology Institute. We wish to thank the Jeff Gralnick lab at the University of Minnesota for their donation of Shewanella oneidensis MR-1. A portion of the research was performed at EMSL, a national scientific user facility sponsored by the Department of Energy's Office of Biological and Environmental Research and located at PNNL. CSL acknowledges the Bionanotechnology Research Center, Korea Research Institute of Bioscience and Biotechnology (KRIBB), 125 Gwahangno, Yuseong-gu, Daejeon 305-806, Korea. NR 22 TC 7 Z9 7 U1 1 U2 27 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 0003-2654 EI 1364-5528 J9 ANALYST JI Analyst PY 2014 VL 139 IS 12 BP 3174 EP 3178 DI 10.1039/c4an00574k PG 5 WC Chemistry, Analytical SC Chemistry GA AI3CZ UT WOS:000336737900032 PM 24816810 ER PT J AU Mann, GW Carslaw, KS Reddington, CL Pringle, KJ Schulz, M Asmi, A Spracklen, DV Ridley, DA Woodhouse, MT Lee, LA Zhang, K Ghan, SJ Easter, RC Liu, X Stier, P Lee, YH Adams, PJ Tost, H Lelieveld, J Bauer, SE Tsigaridis, K van Noije, TPC Strunk, A Vignati, E Bellouin, N Dalvi, M Johnson, CE Bergman, T Kokkola, H von Salzen, K Yu, F Luo, G Petzold, A Heintzenberg, J Clarke, A Ogren, A Gras, J Baltensperger, U Kaminski, U Jennings, SG O'Dowd, CD Harrison, RM Beddows, DCS Kulmala, M Viisanen, Y Ulevicius, V Mihalopoulos, N Zdimal, V Fiebig, M Hansson, HC Swietlicki, E Henzing, JS AF Mann, G. W. Carslaw, K. S. Reddington, C. L. Pringle, K. J. Schulz, M. Asmi, A. Spracklen, D. V. Ridley, D. A. Woodhouse, M. T. Lee, L. A. Zhang, K. Ghan, S. J. Easter, R. C. Liu, X. Stier, P. Lee, Y. H. Adams, P. J. Tost, H. Lelieveld, J. Bauer, S. E. Tsigaridis, K. van Noije, T. P. C. Strunk, A. Vignati, E. Bellouin, N. Dalvi, M. Johnson, C. E. Bergman, T. Kokkola, H. von Salzen, K. Yu, F. Luo, G. Petzold, A. Heintzenberg, J. Clarke, A. Ogren, A. Gras, J. Baltensperger, U. Kaminski, U. Jennings, S. G. O'Dowd, C. D. Harrison, R. M. Beddows, D. C. S. Kulmala, M. Viisanen, Y. Ulevicius, V. Mihalopoulos, N. Zdimal, V. Fiebig, M. Hansson, H-C Swietlicki, E. Henzing, J. S. TI Intercomparison and evaluation of global aerosol microphysical properties among AeroCom models of a range of complexity SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID CLOUD CONDENSATION NUCLEI; MARINE BOUNDARY-LAYER; NUMBER SIZE DISTRIBUTIONS; GENERAL-CIRCULATION MODEL; OFF-LINE MODEL; CLIMATE MODEL; BLACK CARBON; PARTICLE FORMATION; MIXING STATE; ATMOSPHERIC AEROSOL AB Many of the next generation of global climate models will include aerosol schemes which explicitly simulate the microphysical processes that determine the particle size distribution. These models enable aerosol optical properties and cloud condensation nuclei (CCN) concentrations to be determined by fundamental aerosol processes, which should lead to a more physically based simulation of aerosol direct and indirect radiative forcings. This study examines the global variation in particle size distribution simulated by 12 global aerosol microphysics models to quantify model diversity and to identify any common biases against observations. Evaluation against size distribution measurements from a new European network of aerosol supersites shows that the mean model agrees quite well with the observations at many sites on the annual mean, but there are some seasonal biases common to many sites. In particular, at many of these European sites, the accumulation mode number concentration is biased low during winter and Aitken mode concentrations tend to be overestimated in winter and underestimated in summer. At high northern latitudes, the models strongly underpredict Aitken and accumulation particle concentrations compared to the measurements, consistent with previous studies that have highlighted the poor performance of global aerosol models in the Arctic. In the marine boundary layer, the models capture the observed meridional variation in the size distribution, which is dominated by the Aitken mode at high latitudes, with an increasing concentration of accumulation particles with decreasing latitude. Considering vertical profiles, the models reproduce the observed peak in total particle concentrations in the upper troposphere due to new particle formation, although modelled peak concentrations tend to be biased high over Europe. Overall, the multimodel-mean data set simulates the global variation of the particle size distribution with a good degree of skill, suggesting that most of the individual global aerosol microphysics models are performing well, although the large model diversity indicates that some models are in poor agreement with the observations. Further work is required to better constrain size-resolved primary and secondary particle number sources, and an improved understanding of nucleation and growth (e. g. the role of nitrate and secondary organics) will improve the fidelity of simulated particle size distributions. C1 [Mann, G. W.] Univ Leeds, Natl Ctr Atmospher Sci, Leeds, W Yorkshire, England. [Mann, G. W.; Carslaw, K. S.; Reddington, C. L.; Pringle, K. J.; Spracklen, D. V.; Ridley, D. A.; Woodhouse, M. T.; Lee, L. A.] Univ Leeds, Sch Earth & Environm, Leeds, W Yorkshire, England. [Schulz, M.] Norwegian Meteorol Inst, Oslo, Norway. [Asmi, A.; Viisanen, Y.] Univ Helsinki, Helsinki, Finland. [Pringle, K. J.; Tost, H.; Lelieveld, J.] Max Planck Inst Chem, D-55128 Mainz, Germany. [Ridley, D. A.] MIT, Cambridge, MA 02139 USA. [Zhang, K.] Max Planck Inst Meteorol, D-20146 Hamburg, Germany. [Zhang, K.; Ghan, S. J.; Easter, R. C.] Pacific NW Natl Lab, Richland, WA 99352 USA. [Stier, P.] Univ Oxford, Dept Phys, Oxford, England. [Lee, Y. H.; Adams, P. J.] Carnegie Mellon Univ, Pittsburgh, PA 15213 USA. [Bauer, S. E.; Tsigaridis, K.] Columbia Univ, Ctr Climate Syst Res, New York, NY USA. [Lelieveld, J.] Cyprus Inst, Nicosia, Cyprus. [Lee, Y. H.; Bauer, S. E.; Tsigaridis, K.] NASA, Goddard Inst Space Studies, New York, NY 10025 USA. [van Noije, T. P. C.; Strunk, A.] Royal Netherlands Meteorol Inst KNMI, De Bilt, Netherlands. [Vignati, E.] EU Joint Res Ctr JRC, Ispra, Italy. [Bellouin, N.] Univ Reading, Dept Meteorol, Reading, Berks, England. [Dalvi, M.; Johnson, C. E.] Met Off Hadley Ctr, Exeter, Devon, England. [Bergman, T.; Kokkola, H.] Finnish Meteorol Inst, Kuopio Unit, Kuopio, Finland. [von Salzen, K.] Environm Canada, Canadian Ctr Climate Modelling & Anal, Gatineau, PQ, Canada. [Yu, F.; Luo, G.] SUNY Albany, Dept Earth & Atmospher Sci, Albany, NY 12222 USA. [Petzold, A.] DLR, Inst Atmospher Phys, Oberpfaffenhofen, Germany. [Heintzenberg, J.] Leibniz Inst Tropospher Res, Leipzig, Germany. [Clarke, A.] Univ Hawaii, Dept Oceanog, Honolulu, HI 96822 USA. [Ogren, A.] NOAA, Earth Syst Res Lab, Boulder, CO USA. [Woodhouse, M. T.; Gras, J.] CSIRO Marine & Atmospher Res, Aspendale, Vic, Australia. [Baltensperger, U.] Paul Scherrer Inst, Villigen, Switzerland. [Kaminski, U.] Deutsch Wetterdienst DWD, Offenbach, Germany. [Jennings, S. G.; O'Dowd, C. D.] Natl Univ Ireland Galway, Galway, Ireland. [Harrison, R. M.; Beddows, D. C. S.] Univ Birmingham, Natl Ctr Atmospher Sci, Birmingham, W Midlands, England. [Kulmala, M.] Univ Helsinki, Dept Phys, Helsinki, Finland. [Ulevicius, V.] Ctr Phys Sci & Technol, Vilnius, Lithuania. [Tost, H.] Johannes Gutenberg Univ Mainz, Inst Phys Atmosphere, D-55122 Mainz, Germany. [Petzold, A.] Forschungszentrum Julich, IEK Troposphere 8, D-52425 Julich, Germany. [Harrison, R. M.] King Abdulaziz Univ, Dept Environm Sci, Jeddah 21589, Saudi Arabia. [Mihalopoulos, N.] Univ Crete, Dept Chem, Iraklion, Greece. [Zdimal, V.] Acad Sci Czech Republic, Inst Chem Proc Fundamentals, CR-16502 Prague, Czech Republic. [Liu, X.] Univ Wyoming, Dept Atmospher Sci, Laramie, WY 82071 USA. [Fiebig, M.] Norwegian Inst Air Res NILU, Dept Atmospher & Climate Res, Oslo, Norway. [Hansson, H-C] Stockholm Univ, Dept Appl Environm Sci, Stockholm, Sweden. [Swietlicki, E.] Lund Univ, Dept Phys, S-22362 Lund, Sweden. [Henzing, J. S.] Netherlands Org Appl Sci Res TNO, Utrecht, Netherlands. RP Mann, GW (reprint author), Univ Leeds, Natl Ctr Atmospher Sci, Leeds, W Yorkshire, England. EM gmann@env.leeds.ac.uk RI Liu, Xiaohong/E-9304-2011; Swietlicki, Erik/B-9426-2014; Harrison, Roy/A-2256-2008; Kokkola, Harri/J-5993-2014; Fiebig, Markus/I-4872-2012; Petzold, Andreas/J-2347-2012; Bergman, Tommi/C-2445-2009; Carslaw, Ken/C-8514-2009; O'Dowd , Colin/K-8904-2012; Spracklen, Dominick/B-4890-2014; Bauer, Susanne/P-3082-2014; Yu, Fangqun/F-3708-2011; Adams, Peter/D-7134-2013; Reddington, Carly/I-3390-2015; Woodhouse, Matthew/E-4808-2013; Zhang, Kai/F-8415-2010; Ogren, John/M-8255-2015; Schulz, Michael/A-6930-2011; Zdimal, Vladimir/H-3434-2014; Ghan, Steven/H-4301-2011; Mihalopoulos, Nikolaos/H-5327-2016; Kulmala, Markku/I-7671-2016; Stier, Philip/B-2258-2008; Lelieveld, Johannes/A-1986-2013; Tost, Holger/C-3812-2017; OI Liu, Xiaohong/0000-0002-3994-5955; Harrison, Roy/0000-0002-2684-5226; Fiebig, Markus/0000-0002-3380-3470; Petzold, Andreas/0000-0002-2504-1680; Bergman, Tommi/0000-0002-6133-2231; Carslaw, Ken/0000-0002-6800-154X; O'Dowd , Colin/0000-0002-3068-2212; Yu, Fangqun/0000-0003-0874-4883; Adams, Peter/0000-0003-0041-058X; Woodhouse, Matthew/0000-0002-9892-4492; Zhang, Kai/0000-0003-0457-6368; Ogren, John/0000-0002-7895-9583; Schulz, Michael/0000-0003-4493-4158; Ghan, Steven/0000-0001-8355-8699; Mihalopoulos, Nikolaos/0000-0002-1282-0896; Kulmala, Markku/0000-0003-3464-7825; Stier, Philip/0000-0002-1191-0128; Tost, Holger/0000-0002-3105-4306; Lee, Yunha/0000-0001-7478-2672 FU National Centre for Atmospheric Science, one of the UK Natural Environment Research Council (NERC) research centres; NERC [NE/G015015/1, NE/G006172/1]; NERC Doctoral Training Grant; EU from the European Research Council (ERC) [218793, 283576, FP7-280025]; ERC [265148, 226144]; UK Integrated Climate Programme - Department for Energy and Climate Change (DECC); Department for Environment Food and Rural Affairs - DECC/Defra [GA01101]; US Department of Energy (DOE) Scientific Discoveries through Advanced Computing program; DOE by Battelle Memorial Institute [DE-AC06-76RLO 1830]; NASA Modeling, Analysis and Prediction Program [NASA NNX09AK66G]; NERC project AEROS [NE/G006148/1]; Max Planck Society; Canadian Foundation for Climate and Atmospheric Sciences (CFCAS); Environment Canada; Flemish agency for Innovation by Science and Technology (IWT) through the Climate and Air Quality Modelling for Policy Support (CLIMAQS) project; NASA [NNX11AQ72G]; NSF [0942106]; EU [RII3-CT-2006-026140]; Swedish Environmental Protection Agency; UK Department for Environment, Food and Rural Affairs; EPA; Met Eireann; Department of the Environment; European Union; German Ministry of Education and Science [AFO 2000]; European Commission FX G. W. Mann and K. S. Carslaw received funding from the National Centre for Atmospheric Science, one of the UK Natural Environment Research Council (NERC) research centres. NERC research grants funded D. V. Spracklen (NE/G015015/1) and L. A. Lee (NE/G006172/1), while D. A. Ridley was funded via an NERC Doctoral Training Grant. M. T. Wood-house and G. W. Mann received EU funding from the European Research Council (ERC) under Seventh Framework Programme (FP7) consortium projects MACC and MACC-II (grant agreements 218793 and 283576 respectively). C. L. Reddington, K. J. Pringle and K. S. Carslaw also received ERC FP7 funding under the PE-GASOS Integrated Project (grant agreement 265148). N. Bellouin, M. Dalvi, C. E. Johnson were supported as part the UK Integrated Climate Programme funded by the Department for Energy and Climate Change (DECC) and Department for Environment Food and Rural Affairs - DECC/Defra (GA01101). S. J. Ghan, R. C. Easter and X. Liu were supported by the US Department of Energy (DOE) Scientific Discoveries through Advanced Computing program. The Pacific Northwest National Laboratory (PNNL) is operated for the DOE by Battelle Memorial Institute under contract DE-AC06-76RLO 1830. S. E. Bauer and K. Tsigaridis were supported by the NASA Modeling, Analysis and Prediction Program (NASA NNX09AK66G) with supercomputing resourced via the NASA High-End Computing (HEC) Program through the NASA Center for Climate Simulation (NCCS) at Goddard Space Flight Center. P. Stier has been supported by the NERC project AEROS (NE/G006148/1) and received EU funding from the European Research Council (ERC) under FP7 grant agreement FP7-280025. K. J. Pringle, H. Tost and J. Lelieveld received funding from the ERC (grant agreement 226144). K. Zhang was supported by funding from the Max Planck Society. Simulations with ECHAM5-HAM2 were performed at the German Climate Computing Center (Deutsches Klimarechenzentrum GmbH, DKRZ). K. von Salzen was supported by the Canadian Foundation for Climate and Atmospheric Sciences (CFCAS) and Environment Canada. A. Strunk acknowledges financial support from the Flemish agency for Innovation by Science and Technology (IWT) through the Climate and Air Quality Modelling for Policy Support (CLIMAQS) project. F. Yu and G. Luo were supported by NASA under grant NNX11AQ72G and NSF under grant 0942106. The EUSAAR network of aerosol supersites were established with EU funding from the Research Infrastructure Action under the FP6 Structuring the European Research Area Programme, Contract RII3-CT-2006-026140. Data for the Aspvreten and Zeppelin sites were provided by the Atmospheric Science Unit, Department of Applied Env. Sci, Stockholm University with financial support from the Swedish Environmental Protection Agency. The Harwell station is operated with financial support from the UK Department for Environment, Food and Rural Affairs. The Mace Head station received support from several Irish Government Agencies including the EPA, Met Eireann, and Department of the Environment. S. G. Jennings and C. D. O'Dowd would like to acknowledge the support of the European Union, through various projects within the 5th, 6th and 7th Framework programmes. J. Heintzenberg gratefully acknowledges financial support from the German Ministry of Education and Science (AFO 2000 programme) and from the European Commission's DGXII Environment RTD 4th, 5th, 6th and 7th framework programmes. Airborne data provided by A.; Clarke, University of Hawaii, represent about 2 decades of approximately equal support from the NSF-Atmospheric Chemistry Program and the NASA-Earth Science Division. We are also grateful to the two anonymous reviewers whose comments have improved the paper considerably. NR 158 TC 38 Z9 38 U1 4 U2 79 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 2014 VL 14 IS 9 BP 4679 EP 4713 DI 10.5194/acp-14-4679-2014 PG 35 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA AI3DN UT WOS:000336739700020 ER PT J AU Lee, YN Springston, S Jayne, J Wang, J Hubbe, J Senum, G Kleinman, L Daum, PH AF Lee, Y. -N. Springston, S. Jayne, J. Wang, J. Hubbe, J. Senum, G. Kleinman, L. Daum, P. H. TI Chemical composition and sources of coastal marine aerosol particles during the 2008 VOCALS-REx campaign SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID BOUNDARY-LAYER; SOUTHEAST PACIFIC; SIZE DISTRIBUTION; CLOUD; EVOLUTION AB The chemical composition of aerosol particles (D-p <= 1.5 mu m) was measured over the southeast Pacific Ocean during the VAMOS (Variability of the American Monsoon Systems) Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-Rex) between 16 October and 15 November 2008 using the US Department of Energy (DOE) G-1 aircraft. The objective of these flights was to gain an understanding of the sources and evolution of these aerosols, and of how they interact with the marine stratus cloud layer that prevails in this region of the globe. Our measurements showed that the marine boundary layer (MBL) aerosol mass was dominated by non-sea-salt SO42-, followed by Na+, Cl-, Org (total organics), NH4+, and NO3-, in decreasing order of importance; CH3SO3- (MSA), Ca2+, and K+ rarely exceeded their limits of detection. Aerosols were strongly acidic with a NH4+ to SO42- equivalents ratio typically < 0.3. Sea-salt aerosol (SSA) particles, represented by NaCl, exhibited Cl- deficits caused by both HNO3 and H2SO4, but for the most part were externally mixed with particles, mainly SO42-. SSA contributed only a small fraction of the total accumulation mode particle number concentration. It was inferred that all aerosol species (except SSA) were of predominantly continental origin because of their strong land-to-sea concentration gradient. Comparison of relative changes in median values suggests that (1) an oceanic source of NH3 is present between 72A degrees W and 76A degrees W, (2) additional organic aerosols from biomass burns or biogenic precursors were emitted from coastal regions south of 31A degrees S, with possible cloud processing, and (3) free tropospheric (FT) contributions to MBL gas and aerosol concentrations were negligible. The very low levels of CH3SO3- observed as well as the correlation between SO42- and NO3- (which is thought primarily anthropogenic) suggest a limited contribution of DMS to SO42- aerosol production during VOCALS. C1 [Lee, Y. -N.; Springston, S.; Wang, J.; Senum, G.; Kleinman, L.; Daum, P. H.] Brookhaven Natl Lab, Div Atmospher Sci, Upton, NY 11973 USA. [Jayne, J.] Aerodyne Res Inc, Bellerica, MA 01821 USA. [Hubbe, J.] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Daum, PH (reprint author), Brookhaven Natl Lab, Div Atmospher Sci, Upton, NY 11973 USA. EM phdaum@bnl.gov RI Wang, Jian/G-9344-2011 FU DOE Office of Biological and Environmental Research FX The Atmospheric Sciences Program within the DOE Office of Biological and Environmental Research, which has since been merged into the Atmospheric System Research Program, supported this research. The authors gratefully acknowledge the DOE G-1 flight crew led by Chief Pilot Bob Hannigan for their dedication and professionalism that ensured a safe and productive scientific mission. NR 26 TC 3 Z9 3 U1 1 U2 27 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 2014 VL 14 IS 10 BP 5057 EP 5072 DI 10.5194/acp-14-5057-2014 PG 16 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA AI3DQ UT WOS:000336740000013 ER PT J AU Zaveri, RA Easter, RC Shilling, JE Seinfeld, JH AF Zaveri, R. A. Easter, R. C. Shilling, J. E. Seinfeld, J. H. TI Modeling kinetic partitioning of secondary organic aerosol and size distribution dynamics: representing effects of volatility, phase state, and particle-phase reaction SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID CLOUD CONDENSATION NUCLEI; ALPHA-PINENE; HETEROGENEOUS REACTIONS; ATMOSPHERIC PARTICLES; AQUEOUS-PHASE; GROWTH; CHEMISTRY; CCN; EVAPORATION; ABSORPTION AB This paper describes and evaluates a new framework for modeling kinetic gas-particle partitioning of secondary organic aerosol (SOA) that takes into account diffusion and chemical reaction within the particle phase. The framework uses a combination of (a) an analytical quasi-steady-state treatment for the diffusion-reaction process within the particle phase for fast-reacting organic solutes, and (b) a two-film theory approach for slow- and nonreacting solutes. The framework is amenable for use in regional and global atmospheric models, although it currently awaits specification of the various gas- and particle-phase chemistries and the related physicochemical properties that are important for SOA formation. Here, the new framework is implemented in the computationally efficient Model for Simulating Aerosol Interactions and Chemistry (MOSAIC) to investigate the competitive growth dynamics of the Aitken and accumulation mode particles. Results show that the timescale of SOA partitioning and the associated size distribution dynamics depend on the complex interplay between organic solute volatility, particle-phase bulk diffusivity, and particle-phase reactivity (as exemplified by a pseudo-first-order reaction rate constant), each of which can vary over several orders of magnitude. In general, the timescale of SOA partitioning increases with increase in volatility and decrease in bulk diffusivity and rate constant. At the same time, the shape of the aerosol size distribution displays appreciable narrowing with decrease in volatility and bulk diffusivity and increase in rate constant. A proper representation of these physicochemical processes and parameters is needed in the next generation models to reliably predict not only the total SOA mass, but also its composition- and number-diameter distributions, all of which together determine the overall optical and cloud-nucleating properties. C1 [Zaveri, R. A.; Easter, R. C.; Shilling, J. E.] Pacific NW Natl Lab, Atmospher Sci & Global Change Div, Richland, WA 99352 USA. [Seinfeld, J. H.] CALTECH, Div Chem & Chem Engn, Pasadena, CA 91125 USA. [Seinfeld, J. H.] CALTECH, Div Engn & Appl Sci, Pasadena, CA 91125 USA. RP Zaveri, RA (reprint author), Pacific NW Natl Lab, Atmospher Sci & Global Change Div, Richland, WA 99352 USA. EM rahul.zaveri@pnnl.gov RI Shilling, John/L-6998-2015; Zaveri, Rahul/G-4076-2014 OI Shilling, John/0000-0002-3728-0195; Zaveri, Rahul/0000-0001-9874-8807 FU US Department of Energy (DOE) Atmospheric System Research (ASR) Program at Pacific Northwest National Laboratory (PNNL) [DE-AC06-76RLO 1830]; DOE [DE-SC0006626]; National Science Foundation [AGS-1057183] FX R. A. Zaveri thanks M. Shiraiwa (Max Planck Institute for Chemistry), A. Zelenyuk, M. Shrivastava (Pacific Northwest National Laboratory), J. Wang (Brookhaven National Laboratory), M. West (University of Illinois at Urbana-Champaign), and A. S. Wexler (University of California, Davis) for stimulating discussions. The authors thank A. Carlton for editing this paper. This research was supported by the US Department of Energy (DOE) Atmospheric System Research (ASR) Program under contract DE-AC06-76RLO 1830 at Pacific Northwest National Laboratory (PNNL). Participation of J. H. Seinfeld in this research was supported by DOE grant DE-SC0006626 and National Science Foundation grant AGS-1057183. PNNL is operated for the US DOE by Battelle Memorial Institute. NR 66 TC 24 Z9 24 U1 10 U2 65 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 2014 VL 14 IS 10 BP 5153 EP 5181 DI 10.5194/acp-14-5153-2014 PG 29 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA AI3DQ UT WOS:000336740000018 ER PT J AU Taylor, PA Ludwigsen, JS Ford, CC AF Taylor, Paul A. Ludwigsen, John S. Ford, Corey C. TI Investigation of blast-induced traumatic brain injury SO BRAIN INJURY LA English DT Article DE Blast; mild traumatic brain injury; modelling; simulation ID WHITE-MATTER; SYSTEM; MODEL AB Objective: Many troops deployed in Iraq and Afghanistan have sustained blast-related, closed-head injuries from being within non-lethal distance of detonated explosive devices. Little is known, however, about the mechanisms associated with blast exposure that give rise to traumatic brain injury (TBI). This study attempts to identify the precise conditions of focused stress wave energy within the brain, resulting from blast exposure, which will correlate with a threshold for persistent brain injury. Methods: This study developed and validated a set of modelling tools to simulate blast loading to the human head. Using these tools, the blast-induced, early-time intracranial wave motions that lead to focal brain damage were simulated. Results: The simulations predict the deposition of three distinct wave energy components, two of which can be related to injury-inducing mechanisms, namely cavitation and shear. Furthermore, the results suggest that the spatial distributions of these damaging energy components are independent of blast direction. Conclusions: The predictions reported herein will simplify efforts to correlate simulation predictions with clinical measures of TBI and aid in the development of protective headwear. C1 [Taylor, Paul A.; Ludwigsen, John S.] Sandia Natl Labs, Terminal Ballist Technol, Albuquerque, NM 87185 USA. [Ford, Corey C.] Univ New Mexico, Dept Neurol, Albuquerque, NM 87131 USA. RP Taylor, PA (reprint author), Sandia Natl Labs, Terminal Ballist Technol, POB 5800, Albuquerque, NM 87185 USA. EM pataylo@sandia.gov NR 31 TC 14 Z9 14 U1 1 U2 8 PU INFORMA HEALTHCARE PI LONDON PA TELEPHONE HOUSE, 69-77 PAUL STREET, LONDON EC2A 4LQ, ENGLAND SN 0269-9052 EI 1362-301X J9 BRAIN INJURY JI Brain Inj. PY 2014 VL 28 IS 7 BP 879 EP 895 DI 10.3109/02699052.2014.888478 PG 17 WC Neurosciences; Rehabilitation SC Neurosciences & Neurology; Rehabilitation GA AH9XL UT WOS:000336498600001 PM 24766453 ER PT J AU Clikeman, TT Bukovsky, EV Kuvychko, IV San, LK Deng, SHM Wang, XB Chen, YS Strauss, SH Boltalina, OV AF Clikeman, Tyler T. Bukovsky, Eric V. Kuvychko, Igor V. San, Long K. Deng, Shihu H. M. Wang, Xue-Bin Chen, Yu-Sheng Strauss, Steven H. Boltalina, Olga V. TI Poly(trifluoromethyl) azulenes: structures and acceptor properties SO CHEMICAL COMMUNICATIONS LA English DT Article ID 2,4,6,8-TETRACYANOAZULENE; DERIVATIVES; POLYAZULENE; COMPLEXES; MOLECULES; BEHAVIOR AB Six new poly(trifluoromethyl) azulenes prepared in a single high-temperature reaction exhibit strong electron accepting properties in the gas phase and in solution and demonstrate the propensity to form regular pi-stacked columns in donor-acceptor crystals when mixed with pyrene as a donor. C1 [Clikeman, Tyler T.; Bukovsky, Eric V.; Kuvychko, Igor V.; San, Long K.; 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. [Chen, Yu-Sheng] Univ Chicago, Adv Photon Source, ChemMatCARS, Argonne, IL 60439 USA. RP Wang, XB (reprint author), Pacific NW Natl Lab, Div Phys Sci, POB 999,MS K8-88, Richland, WA 99352 USA. EM steven.strauss@colostate.edu; olga.boltalina@colostate.edu FU U.S. NSF [CHE-1346572]; Colorado State University Research Foundation; US Department of Energy (DOE), Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences; DOE Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory; National Science Foundation [NSF/CHE-1346572]; U.S. Department of Energy, Office of Science, and Office of Basic Energy Sciences [DE-AC02-06CH11357] FX Natalia Shustova and Dmitry Peryshkov are greatly acknowledged for assistance with X-ray crystallography of AZUL-4-1. We thank the U.S. NSF/CHE-1346572, and the Colorado State University Research Foundation for partial financial support. The photoelectron spectra work was supported by the US Department of Energy (DOE), Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences, and was performed at the EMSL, a national scientific user facility sponsored by DOE Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory. ChemMatCARS Sector 15 is principally supported by the National Science Foundation under grant number NSF/CHE-1346572. Use of the Advanced Photon Source was supported by the U.S. Department of Energy, Office of Science, and Office of Basic Energy Sciences under Contract DE-AC02-06CH11357. NR 29 TC 5 Z9 5 U1 4 U2 23 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 2014 VL 50 IS 47 BP 6263 EP 6266 DI 10.1039/c4cc00510d PG 4 WC Chemistry, Multidisciplinary SC Chemistry GA AI3VM UT WOS:000336793100021 PM 24788399 ER PT J AU Davenport, TC Ahn, HS Ziegler, MS Tilley, TD AF Davenport, Timothy C. Ahn, Hyun S. Ziegler, Micah S. Tilley, T. Don TI A molecular structural analog of proposed dinuclear active sites in cobalt-based water oxidation catalysts SO CHEMICAL COMMUNICATIONS LA English DT Article ID OXYGEN-EVOLVING CATALYST; PHOTOSYSTEM-II; COMPLEXES; PHOSPHATE; MECHANISM; EVOLUTION; CENTERS; DIMER; FUEL AB The compound [Co-2(mu-OH)(2)(OH2)(2)(DPFN)][NO3](4) is a molecular structural analog of proposed active sites of cobalt phosphate water oxidation catalysts. Computational studies on this system indicate feasible catalytic pathways to oxygen formation, despite the low electrocatalytic activity observed for [Co-2(mu-OH)(2)(OH2)(2)(DPFN)][NO3](4). Electrochemical and reactivity studies implicate the binding of phosphate to the dicobalt core, which may inhibit water oxidation catalysis. C1 [Davenport, Timothy C.; Ahn, Hyun S.; Ziegler, Micah S.; Tilley, T. Don] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Davenport, Timothy C.; Ahn, Hyun S.; Ziegler, Micah S.; Tilley, T. Don] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. RP Tilley, TD (reprint author), Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. EM tdtilley@berkeley.edu FU National Science Foundation [CHE-0840505]; University of California; Helios Solar Energy Research Center; Office of Energy Research, Office of Basic Energy Sciences, Chemical Sciences Division, of the U.S. Department of Energy [DE-AC02-05CH11231] FX We acknowledge Dr Xinzheng Yang for assistance with computational work and Dr Christopher Letko for helpful discussions. Support for T. C. D. was provided by a National Science Foundation Graduate Research Fellowship and a University of California Chancellor's Fellowship. Funding for this work was provided by the Helios Solar Energy Research Center, and the support of the Director, Office of Energy Research, Office of Basic Energy Sciences, Chemical Sciences Division, of the U.S. Department of Energy under contract DE-AC02-05CH11231. Support for the Molecular Graphics and Computation Facility at UC Berkeley is provided by the National Science Foundation under grant CHE-0840505. NR 24 TC 13 Z9 13 U1 1 U2 41 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 2014 VL 50 IS 48 BP 6326 EP 6329 DI 10.1039/c3cc46865h PG 4 WC Chemistry, Multidisciplinary SC Chemistry GA AI3VU UT WOS:000336794000007 PM 24797957 ER PT J AU Saito, T Perkins, JH Vautard, F Meyer, HM Messman, JM Tolnai, B Naskar, AK AF Saito, Tomonori Perkins, Joshua H. Vautard, Frederic Meyer, Harry M. Messman, Jamie M. Tolnai, Balazs Naskar, Amit K. TI Methanol Fractionation of Softwood Kraft Lignin: Impact on the Lignin Properties SO CHEMSUSCHEM LA English DT Article DE biomass; carbon; polymers; renewable resources; waste prevention ID SEQUENTIAL SOLVENT-EXTRACTION; MILLED WOOD LIGNIN; ALCELL(R) LIGNIN; ORGANOSOLV LIGNINS; CONTROLLED-RELEASE; CARBON-FIBER; ETHANOL; SPECTROSCOPY; TEMPERATURE; HERBICIDE AB The development of technologies to tune lignin properties for high-performance lignin-based materials is crucial for the utilization of lignin in various applications. Here, the effect of methanol (MeOH) fractionation on the molecular weight, molecular weight distribution, glass transition temperature (T-g), thermal decomposition, and chemical structure of lignin were investigated. Repeated MeOH fractionation of softwood Kraft lignin successfully removed the low-molecular-weight fraction. The separated high-molecular-weight lignin showed a T-g of 211 degrees C and a char yield of 47%, much higher than those of as-received lignin (T-g 153 degrees C, char yield 41%). The MeOH-soluble fraction of lignin showed an increased low-molecular-weight fraction and a lower T-g (117 degrees C) and char yield (32%). The amount of low-molecular-weight fraction showed a quantitative correlation with both 1/T-g and char yield in a linear regression. This study demonstrated the efficient purification or fractionation technology for lignin; it also established a theoretical and empirical correlation between the physical characteristics of fractionated lignins. C1 [Saito, Tomonori] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. [Perkins, Joshua H.; Vautard, Frederic; Meyer, Harry M.; Naskar, Amit K.] Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN 37831 USA. [Messman, Jamie M.] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. [Tolnai, Balazs] Kruger Inc, Ind Prod Div, Montreal, PQ H3S 1G5, Canada. RP Saito, T (reprint author), Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. EM saitot@ornl.gov; naskarak@ornl.gov RI Saito, Tomonori/M-1735-2016 OI Saito, Tomonori/0000-0002-4536-7530 FU Laboratory Directed Research and Development Program of Oak Ridge National Laboratory; U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Advanced Manufacturing Office [DE-AC05-00O30725]; UT-Battelle, LLC; Division of Scientific User Facilities, U.S. Department of Energy; U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Program FX This research was sponsored by the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory, managed by UT-Battelle, LLC, for the U.S. Department of Energy. J.H.P. acknowledges support by the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Advanced Manufacturing Office, under contract DE-AC05-00O30725 with UT-Battelle, LLC. Part of the polymer characterization work was conducted at the Center for Nanophase Materials Sciences, which is sponsored at Oak Ridge National Laboratory by the Division of Scientific User Facilities, U.S. Department of Energy. A part of this research was done through the Oak Ridge National Laboratory's High Temperature Materials Laboratory User Program, sponsored by the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Program. NR 39 TC 40 Z9 40 U1 8 U2 53 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 2014 VL 7 IS 1 BP 221 EP 228 DI 10.1002/cssc.201300509 PG 8 WC Chemistry, Multidisciplinary; GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY SC Chemistry; Science & Technology - Other Topics GA AI3YR UT WOS:000336802400026 PM 24458739 ER PT J AU Shen, B Dai, F Price, L Lu, HY AF Shen, Bo Dai, Fan Price, Lynn Lu, Hongyou TI CALIFORNIA'S CAP-AND-TRADE PROGRAMME AND INSIGHTS FOR CHINA'S PILOT SCHEMES SO ENERGY & ENVIRONMENT LA English DT Article DE Cap-and-trade; greenhouse gas emissions trading; climate change; China ID CLIMATE-CHANGE; LESSONS AB California's cap-and-trade programme under the Assembly Bill 32 is a key element in California's comprehensive plan for reducing its greenhouse gas (GHG) emissions to 1990 levels by 2020. In China, separate local cap-and-trade pilot schemes are being developed to explore a market-based solution for addressing the country's increasing GHG emissions. The Californian cap-and-trade scheme and China's local pilots are similar in that both have been developed in the absence of a national emissions trading scheme. This paper reviews the Californian scheme and draws insights for China's pilots from various perspectives including the legal basis, institutional arrangement, programme structure, market design, the implementation process, and mechanisms for ensuring compliance. C1 [Shen, Bo; Dai, Fan; Price, Lynn; Lu, Hongyou] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, China Energy Grp, Berkeley, CA 94720 USA. [Dai, Fan] SUNY Coll Environm Sci & Forestry, Syracuse, NY 13210 USA. RP Shen, B (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, China Energy Grp, 1 Cyclotron Rd, Berkeley, CA 94720 USA. EM boshen@lbl.gov NR 31 TC 4 Z9 4 U1 2 U2 13 PU MULTI-SCIENCE PUBL CO LTD PI BRENTWOOD PA 5 WATES WAY, BRENTWOOD CM15 9TB, ESSEX, ENGLAND SN 0958-305X J9 ENERG ENVIRON-UK JI Energy Environ. PY 2014 VL 25 IS 3-4 SI SI BP 551 EP 575 PG 25 WC Environmental Studies SC Environmental Sciences & Ecology GA AI1UZ UT WOS:000336642000003 ER PT S AU Sopori, B Mehta, V Devayajanam, S Seacrist, M Shi, G Chen, J Deshpande, A Binns, J Appel, J AF Sopori, Bhushan Mehta, Vishal Devayajanam, Srinivas Seacrist, M. Shi, G. Chen, J. Deshpande, A. Binns, J. Appel, J. BE Murphy, JD TI y Defect generation and propagation in mc-Si ingots: Influence on the performance of solar cells SO GETTERING AND DEFECT ENGINEERING IN SEMICONDUCTOR TECHNOLOGY XV SE Solid State Phenomena LA English DT Proceedings Paper CT 15th International Conference on Gettering and Defect Engineering in Semiconductor Technology (GADEST) CY SEP 22-27, 2013 CL St Johns Coll, Oxford, ENGLAND SP European Mat Res Soc HO St Johns Coll DE dislocations; defects; solar cell; silicon; network model ID MISFIT DISLOCATIONS; TEMPERATURE; EPILAYERS AB This paper describes results of our study aimed at understanding mechanism(s) of dislocation generation and propagation in multi-crystalline silicon (mc-Si) ingots, and evaluating their influence on the solar cell performance. This work was done in two parts: (i) Measurement of dislocation distributions along various bricks, selected from strategic locations within several ingots; and (ii) Theoretical modeling of the cell performance corresponding to the measured dislocation distributions. Solar cells were fabricated on wafers of known dislocation distribution, and the results were compared with the theory. These results show that cell performance can be accurately predicted from the dislocation distribution, and the changes in the dislocation distribution are the primary cause for variations in the cell-to-cell performance. The dislocation generation and propagation mechanisms, suggested by our results, are described in this paper. C1 [Sopori, Bhushan; Mehta, Vishal; Devayajanam, Srinivas] Natl Renewable Energy Lab, Golden, CO 80401 USA. [Seacrist, M.; Shi, G.; Chen, J.; Deshpande, A.; Binns, J.; Appel, J.] MEMC Elect Mat, St Peters, MO USA. RP Sopori, B (reprint author), Natl Renewable Energy Lab, Golden, CO 80401 USA. EM bhushan.sopori@nrel.gov FU U.S. Department of Energy [DE-AC36-08G028308] FX This work was supported by the U.S. Department of Energy under Contract No. DE-AC36-08G028308 with the National Renewable Energy Laboratory. NR 11 TC 2 Z9 2 U1 0 U2 6 PU TRANS TECH PUBLICATIONS LTD PI DURNTEN-ZURICH PA KREUZSTRASSE 10, 8635 DURNTEN-ZURICH, SWITZERLAND SN 1012-0394 J9 SOLID STATE PHENOMEN PY 2014 VL 205-206 BP 55 EP + DI 10.4028/www.scientific.net/SSP.205-206.55 PG 2 WC Physics, Applied; Physics, Condensed Matter SC Physics GA BA4VK UT WOS:000336338000008 ER PT J AU Mante, OD Agblevor, FA AF Mante, Ofei D. Agblevor, F. A. TI Catalytic pyrolysis for the production of refinery-ready biocrude oils from six different biomass sources SO GREEN CHEMISTRY LA English DT Article ID FIXED-BED REACTOR; HZSM-5 ZEOLITE; OXYGENATE COMPONENTS; MESOPOROUS MATERIALS; HYDROCARBON FUELS; VAPORS; CONVERSION; TRANSFORMATION; FEEDSTOCK; STABILITY AB This study focused on understanding the impact of catalytic pyrolysis and biomass feedstock on the physicochemical properties of upgraded bio-oils. Results from catalytic conversion of different types of biomass feedstocks (woody: pine, hybrid poplar and pinyon-juniper; herbaceous: switchgrass; agricultural residue: corn stover; and forest residue: pine bark) with HZSM-5 zeolite to biocrude oils are presented. The study showed that the source of biomass plays an important role in catalytic pyrolysis products. Significant differences were observed in product distribution, selectivity to aromatic hydrocarbons and physicochemical properties of the biocrude oils. The pyroprobe-GC/MS experiment showed that pine and pinyon-juniper produced the highest carbon yield of monoaromatic hydrocarbons. C-13 NMR analysis revealed that aromatic hydrocarbon content of the oils followed this order: pinyon-juniper > corn stover > pine > poplar > switchgrass > pine bark. The chemical composition and the physicochemical properties indicated that it is critical to reduce carbonyls to achieve stable oils. Also, it was found that elimination of sugars (levoglucosan) and phenolics would improve oil specific gravity and viscosity. Furthermore, reducing the acidity of oils by catalytic pyrolysis appeared to be very challenging. Hence, phenols (weak acids) may have to be minimized in addition to other acids to increase the pH. The nitrogen contents correlated with pH values. Thus, feedstocks with high nitrogen content produced less acidic oils. Nonetheless, high content of nitrogenous compounds could make the biocrude oil highly unstable. The effects of the bio-oil chemical composition on the physicochemical properties are discussed as well as opportunities and challenges of utilizing biocrude oil as feed for standard refinery units. C1 [Mante, Ofei D.] Brookhaven Natl Lab, Dept Sustainable Energy Technol, Upton, NY 11973 USA. [Agblevor, F. A.] Utah State Univ, Dept Biol Engn, USTAR Bioenergy Ctr, Logan, UT 84322 USA. RP Mante, OD (reprint author), Brookhaven Natl Lab, Dept Sustainable Energy Technol, Upton, NY 11973 USA. EM nmante@bnl.gov RI Mante, Ofei/E-8513-2014 OI Mante, Ofei/0000-0002-0960-2943 FU Utah Science Technology and Research (USTAR) Program; BNL Laboratory-Directed Research and development Program, LDRD Project [12-024] FX The Utah Science Technology and Research (USTAR) Program is acknowledged for funding support for the pilot scale work. The pyroprobe-GC/MS studies were performed under the BNL Laboratory-Directed Research and development Program, LDRD Project #12-024. The authors would like to thank Mr Guevara Che Nyendu (USU) for the viscosity measurements and Mr Bhuvanesh Yathavan (USU) for the organic elemental analysis. Dr Seung-Soo Kim (Kangwon National University) is also acknowledged for the TGA work on the biocrude oils. NR 57 TC 15 Z9 15 U1 2 U2 24 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 2014 VL 16 IS 6 BP 3364 EP 3377 DI 10.1039/c4gc00555d PG 14 WC Chemistry, Multidisciplinary; GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY SC Chemistry; Science & Technology - Other Topics GA AI4LF UT WOS:000336836100054 ER PT S AU Dingley, KH Ubick, EA Vogel, JS Ognibene, TJ Malfatti, MA Kulp, K Haack, KW AF Dingley, Karen H. Ubick, Esther A. Vogel, John S. Ognibene, Ted J. Malfatti, Michael A. Kulp, Kristen Haack, Kurt W. BE Keohavong, P Grant, SG TI DNA Isolation and Sample Preparation for Quantification of Adduct Levels by Accelerator Mass Spectrometry SO MOLECULAR TOXICOLOGY PROTOCOLS, 2ND EDITION SE Methods in Molecular Biology LA English DT Article; Book Chapter DE Accelerator mass spectroscopy (AMS); DNA damage; DNA adduct; Carbon-14; Tritium; DNA isolation; Risk assessment ID HUMANS; CARCINOGEN; EXPOSURE; COLON; C-14; AMS; TISSUE; CELLS AB Accelerator mass spectrometry (AMS) is a highly sensitive technique used for the quantification of adducts following exposure to carbon-14- or tritium-labeled chemicals, with detection limits in the range of one adduct per 10(11)-10(12) nucleotides. The protocol described in this chapter provides an optimal method for isolating and preparing DNA samples to measure isotope-labeled DNA adducts by AMS. When preparing samples, special precautions must be taken to avoid cross-contamination of isotope among samples and produce a sample that is compatible with AMS. The DNA isolation method described is based upon digestion of tissue with proteinase K, followed by extraction of DNA using Qiagen isolation columns. The extracted DNA is precipitated with isopropanol, washed repeatedly with 70 % ethanol to remove salt, and then dissolved in water. DNA samples are then converted to graphite or titanium hydride and the isotope content measured by AMS to quantify adduct levels. This method has been used to reliably generate good yields of uncontaminated, pure DNA from animal and human tissues for analysis of adduct levels. C1 [Dingley, Karen H.; Ubick, Esther A.; Vogel, John S.; Ognibene, Ted J.; Malfatti, Michael A.; Kulp, Kristen] Lawrence Livermore Natl Lab, Biol & Biotechnol Res Program, Ctr Accelerator Mass Spect, Livermore, CA 94550 USA. RP Dingley, KH (reprint author), Lawrence Livermore Natl Lab, Biol & Biotechnol Res Program, Ctr Accelerator Mass Spect, Livermore, CA 94550 USA. FU NCRR NIH HHS [RR13461]; NIGMS NIH HHS [P41 GM103483] NR 30 TC 0 Z9 0 U1 1 U2 6 PU HUMANA PRESS INC PI TOTOWA PA 999 RIVERVIEW DR, STE 208, TOTOWA, NJ 07512-1165 USA SN 1064-3745 BN 978-1-62703-739-6; 978-1-62703-738-9 J9 METHODS MOL BIOL JI Methods Mol. Biol. PY 2014 VL 1105 BP 147 EP 157 DI 10.1007/978-1-62703-739-6_12 D2 10.1007/978-1-62703-739-6 PG 11 WC Biochemical Research Methods; Biochemistry & Molecular Biology; Pharmacology & Pharmacy; Toxicology SC Biochemistry & Molecular Biology; Pharmacology & Pharmacy; Toxicology GA BA2SX UT WOS:000333851000013 PM 24623226 ER PT J AU Longerich, S Kwon, Y Tsai, MS Hlaing, AS Kupfer, GM Sung, P AF Longerich, Simonne Kwon, Youngho Tsai, Miaw-Sheue Hlaing, Aye Su Kupfer, Gary M. Sung, Patrick TI Regulation of FANCD2 and FANCI monoubiquitination by their interaction and by DNA SO NUCLEIC ACIDS RESEARCH LA English DT Article ID CROSS-LINK REPAIR; ANEMIA PATHWAY; S-PHASE; PROTEIN; COMPLEX; IDENTIFICATION; RECRUITMENT; ACTIVATION; CHROMATIN; MEMBER AB FANCD2 and FANCI function together in the Fanconi anemia network of deoxyribonucleic acid (DNA) crosslink repair. These proteins form the dimeric ID2 complex that binds DNA and becomes monoubiquitinated upon exposure of cells to DNA crosslinking agents. The monoubiquitinated ID2 complex is thought to facilitate DNA repair via recruitment of specific nucleases, translesion DNA polymerases and the homologous recombination machinery. Using the ubiquitin conjugating enzyme (E2) UBE2T and ubiquitin ligase (E3) FANCL, monoubiquitination of human FANCD2 and FANCI was examined. The ID2 complex is a poor substrate for monoubiquitination, consistent with the published crystal structure showing the solvent inaccessibility of the target lysines. Importantly, FANCD2 monoubiquitination within the ID2 complex is strongly stimulated by duplex or branched DNA, but unstructured single-stranded DNA or chromatinized DNA is ineffective. Interaction of FANCL with the ID2 complex is indispensable for its E3 ligase efficacy. Interestingly, mutations in FANCI that impair its DNA binding activity compromise DNA-stimulated FANCD2 monoubiquitination. Moreover, we demonstrate that in the absence of FANCD2, DNA also stimulates FANCI monoubiquitination, but in a FANCL-independent manner. These results implicate the role of a proper DNA ligand in FANCD2 and FANCI monoubiquitination, and reveal regulatory mechanisms that are dependent on protein-protein and protein-DNA interactions. C1 [Longerich, Simonne; Kwon, Youngho; Sung, Patrick] Yale Univ, Dept Mol Biophys & Biochem, New Haven, CT 06520 USA. [Tsai, Miaw-Sheue; Hlaing, Aye Su] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Life Sci Div, Berkeley, CA 94720 USA. [Kupfer, Gary M.] Yale Univ, Sch Med, Dept Pathol, New Haven, CT 06520 USA. RP Sung, P (reprint author), Yale Univ, Dept Mol Biophys & Biochem, New Haven, CT 06520 USA. EM patrick.sung@yale.edu FU National Institutes of Health [RO1CA168635, RO1ES015252, PO1CA92584, RO1-HL063776]; Leukemia and Lymphoma Society [5279-08] FX National Institutes of Health [RO1CA168635 to P. S and G. M. K, RO1ES015252, PO1CA92584 to P. S., RO1-HL063776 to G. M. K.]; Career Development Award from the Leukemia and Lymphoma Society (5279-08 to S.L.). NR 32 TC 21 Z9 21 U1 2 U2 10 PU OXFORD UNIV PRESS PI OXFORD PA GREAT CLARENDON ST, OXFORD OX2 6DP, ENGLAND SN 0305-1048 EI 1362-4962 J9 NUCLEIC ACIDS RES JI Nucleic Acids Res. PY 2014 VL 42 IS 9 BP 5657 EP 5670 DI 10.1093/nar/gku198 PG 14 WC Biochemistry & Molecular Biology SC Biochemistry & Molecular Biology GA AH9WI UT WOS:000336495400030 PM 24623813 ER PT J AU Jung, YL Luquette, LJ Ho, JWK Ferrari, F Tolstorukov, M Minoda, A Issner, R Epstein, CB Karpen, GH Kuroda, MI Park, PJ AF Jung, Youngsook L. Luquette, Lovelace J. Ho, Joshua W. K. Ferrari, Francesco Tolstorukov, Michael Minoda, Aki Issner, Robbyn Epstein, Charles B. Karpen, Gary H. Kuroda, Mitzi I. Park, Peter J. TI Impact of sequencing depth in ChIP-seq experiments SO NUCLEIC ACIDS RESEARCH LA English DT Article ID HUMAN GENOME AB In a chromatin immunoprecipitation followed by high-throughput sequencing (ChIP-seq) experiment, an important consideration in experimental design is the minimum number of sequenced reads required to obtain statistically significant results. We present an extensive evaluation of the impact of sequencing depth on identification of enriched regions for key histone modifications (H3K4me3, H3K36me3, H3K27me3 and H3K9me2/me3) using deep-sequenced datasets in human and fly. We propose to define sufficient sequencing depth as the number of reads at which detected enrichment regions increase < 1% for an additional million reads. Although the required depth depends on the nature of the mark and the state of the cell in each experiment, we observe that sufficient depth is often reached at < 20 million reads for fly. For human, there are no clear saturation points for the examined datasets, but our analysis suggests 40-50 million reads as a practical minimum for most marks. We also devise a mathematical model to estimate the sufficient depth and total genomic coverage of a mark. Lastly, we find that the five algorithms tested do not agree well for broad enrichment profiles, especially at lower depths. Our findings suggest that sufficient sequencing depth and an appropriate peak-calling algorithm are essential for ensuring robustness of conclusions derived from ChIP-seq data. C1 [Jung, Youngsook L.; Luquette, Lovelace J.; Ho, Joshua W. K.; Ferrari, Francesco; Park, Peter J.] Harvard Univ, Sch Med, Ctr Biomed Informat, Boston, MA 02115 USA. [Jung, Youngsook L.; Ho, Joshua W. K.; Tolstorukov, Michael; Kuroda, Mitzi I.; Park, Peter J.] Brigham & Womens Hosp, Div Genet, Boston, MA 02115 USA. [Jung, Youngsook L.; Ho, Joshua W. K.; Tolstorukov, Michael; Kuroda, Mitzi I.; Park, Peter J.] Harvard Univ, Sch Med, Boston, MA 02115 USA. [Tolstorukov, Michael] Massachusetts Gen Hosp, Dept Mol Biol, Boston, MA 02114 USA. [Minoda, Aki; Karpen, Gary H.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Life Sci, Dept Genome Dynam, Berkeley, CA 94720 USA. [Minoda, Aki; Karpen, Gary H.] Univ Calif Berkeley, Dept Mol & Cell Biol, Berkeley, CA 94720 USA. [Issner, Robbyn; Epstein, Charles B.] Broad Inst MIT & Harvard, Cambridge, MA 02142 USA. [Park, Peter J.] Childrens Hosp, Informat Program, Boston, MA 02115 USA. RP Park, PJ (reprint author), Harvard Univ, Sch Med, Ctr Biomed Informat, Boston, MA 02115 USA. EM peter_park@harvard.edu RI Ferrari, Francesco/H-5007-2012; Minoda, Aki/D-5335-2017 OI Ferrari, Francesco/0000-0002-9811-3753; Minoda, Aki/0000-0002-2927-5791 FU [U01HG004258]; [R01GM101958]; [R01GM082798] FX This work was supported by U01HG004258 to G.K., R01GM101958 to M.K., and R01GM082798 to P.J.P. Funding for open access charge: institutional grant to P.J.P. NR 19 TC 15 Z9 15 U1 2 U2 13 PU OXFORD UNIV PRESS PI OXFORD PA GREAT CLARENDON ST, OXFORD OX2 6DP, ENGLAND SN 0305-1048 EI 1362-4962 J9 NUCLEIC ACIDS RES JI Nucleic Acids Res. PY 2014 VL 42 IS 9 AR e74 DI 10.1093/nar/gku178 PG 10 WC Biochemistry & Molecular Biology SC Biochemistry & Molecular Biology GA AH9WI UT WOS:000336495400001 PM 24598259 ER PT J AU Xiao, XC Liu, ZY Baggetto, L Veith, GM More, KL Unocic, RR AF Xiao, Xingcheng Liu, Zhongyi Baggetto, Loic Veith, Gabriel M. More, Karren L. Unocic, Raymond R. TI Unraveling manganese dissolution/deposition mechanisms on the negative electrode in lithium ion batteries SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article AB The structure, chemistry, and spatial distribution of Mn-bearing nanoparticles dissolved from the Li1.05Mn2O4 cathode during accelerated electrochemical cycling tests at 55 degrees C and deposited within the solid electrolyte interphase (SEI) are directly characterized through HRTEM imaging and XPS. Here we use air protection and vacuum transfer systems to transport cycled electrodes for imaging and analytical characterization. From HRTEM imaging, we find that a band of individual metallic Mn nanoparticles forms locally at the SEI/graphite interface while the internal and outermost layer of the SEI contains a mixture of LiF and MnF2 nanoparticles, which is confirmed with XPS. Based on our experimental findings we propose a new interpretation of how Mn is reduced from the cathode and how metallic Mn and Mn-bearing nanoparticles form within the SEI during electrochemical cycling. C1 [Xiao, Xingcheng; Liu, Zhongyi] Gen Motors Res & Dev Ctr, Warren, MI USA. [Baggetto, Loic; Veith, Gabriel M.] Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN USA. [More, Karren L.; Unocic, Raymond R.] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN USA. RP Xiao, XC (reprint author), Gen Motors Res & Dev Ctr, Warren, MI USA. EM xingcheng.xiao@gm.com; unocicrr@ornl.gov RI More, Karren/A-8097-2016; Baggetto, Loic/D-5542-2017; OI More, Karren/0000-0001-5223-9097; Baggetto, Loic/0000-0002-9029-2363; Unocic, Raymond/0000-0002-1777-8228 FU Oak Ridge National Laboratory's Center for Nanophase Materials Sciences; Scientific User Facilities Division, BES-DOE; U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering under UT-Battelle, LLC FX Materials characterization research was supported by Oak Ridge National Laboratory's Center for Nanophase Materials Sciences, which is sponsored by the Scientific User Facilities Division, BES-DOE (RRU and KLM). LB and GMV were supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering, under contract with UT-Battelle, LLC. The authors gratefully acknowledge the expertise of Dorothy W. Coffey for FIB-TEM specimen preparation. NR 15 TC 12 Z9 12 U1 2 U2 38 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 2014 VL 16 IS 22 BP 10398 EP 10402 DI 10.1039/c4cp00833b PG 5 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AI3SF UT WOS:000336781500012 PM 24733563 ER PT J AU Flores, JM Washenfelder, RA Adler, G Lee, HJ Segev, L Laskin, J Laskin, A Nizkorodov, SA Brown, SS Rudich, Y AF Flores, J. M. Washenfelder, R. A. Adler, G. Lee, H. J. Segev, L. Laskin, J. Laskin, A. Nizkorodov, S. A. Brown, S. S. Rudich, Y. TI Complex refractive indices in the near-ultraviolet spectral region of biogenic secondary organic aerosol aged with ammonia SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID POLYCYCLIC AROMATIC-HYDROCARBONS; ENHANCED ABSORPTION-SPECTROSCOPY; IONIZATION-MASS-SPECTROMETRY; LIGHT-ABSORBING IMPURITIES; SULFURIC-ACID-SOLUTIONS; BROWN CARBON; ALPHA-PINENE; OPTICAL-PROPERTIES; BLACK CARBON; REACTION-PRODUCTS AB Atmospheric absorption by brown carbon aerosol may play an important role in global radiative forcing. Brown carbon arises from both primary and secondary sources, but the mechanisms and reactions of the latter are highly uncertain. One proposed mechanism is the reaction of ammonia or amino acids with carbonyl products in secondary organic aerosol (SOA). We generated SOA in situ by reacting biogenic alkenes (alpha-pinene, limonene, and alpha-humulene) with excess ozone, humidifying the resulting aerosol, and reacting the humidified aerosol with gaseous ammonia. We determined the complex refractive indices (RI) in the 360-420 nm range for these aerosols using broadband cavity enhanced spectroscopy (BBCES). The average real part (n) of the measured spectral range of the NH3-aged alpha-pinene SOA increased from n = 1.50 (+/- 0.01) for the unreacted SOA to n = 1.57 (+/- 0.01) after 1.5 h of exposure to 1.9 ppm NH3, whereas the imaginary component (k) remained below k < 0.001 ((+0.002)(-0.001)) For the limonene and alpha-humulene SOA the real part did not change significantly, and we observed a small change in the imaginary component of the RI. The imaginary component increased from k = 0.000 to an average k = 0.029 (+/- 0.021) for alpha-humulene SOA, and from k < 0.001((+0.002)(-0.001)) to an average k = 0.032 (+/- 0.019) for limonene SOA after 1.5 h of exposure to 1.3 and 1.9 ppm of NH3, respectively. Collected filter samples of the aged and unreacted alpha-pinene SOA and limonene SOA were analyzed off-line by nanospray desorption electrospray ionization high resolution mass spectrometry (nano-DESI/HR-MS), and in situ using a Time-of-Flight Aerosol Mass Spectrometer (ToF-AMS), confirming that the SOA reacted and that various nitrogen-containing reaction products formed. If we assume that NH3 aging reactions scale linearly with time and concentration, which will not necessarily be the case in the atmosphere, then a 1.5 h reaction with 1 ppm NH3 in the laboratory is equivalent to 24 h reaction with 63 ppbv NH3, indicating that the observed aerosol absorption will be limited to atmospheric regions with high NH3 concentrations. C1 [Flores, J. M.; Adler, G.; Segev, L.; Rudich, Y.] Weizmann Inst Sci, Dept Earth & Planetary Sci, IL-76100 Rehovot, Israel. [Washenfelder, R. A.] Univ Colorado, Cooperat Inst Res Environm Sci, Boulder, CO 80309 USA. [Washenfelder, R. A.; Brown, S. S.] Natl Ocean & Atmospher Adm, Earth Syst Res Lab, Div Chem Sci, Boulder, CO 80305 USA. [Lee, H. J.; Nizkorodov, S. A.] Univ Calif Irvine, Dept Chem, Irvine, CA 92697 USA. [Laskin, J.] Pacific NW Natl Lab, Div Phys Sci, Richland, WA 99352 USA. [Laskin, A.] Pacific NW Natl Lab, Environm Mol Sci Lab, Richland, WA 99352 USA. RP Rudich, Y (reprint author), Weizmann Inst Sci, Dept Earth & Planetary Sci, IL-76100 Rehovot, Israel. EM yinon.rudich@weizmann.ac.il RI Washenfelder, Rebecca/E-7169-2010; Laskin, Julia/H-9974-2012; Rudich, Yinon/K-1498-2012; Brown, Steven/I-1762-2013; Laskin, Alexander/I-2574-2012; Nizkorodov, Sergey/I-4120-2014; Manager, CSD Publications/B-2789-2015; OI Washenfelder, Rebecca/0000-0002-8106-3702; Laskin, Julia/0000-0002-4533-9644; Laskin, Alexander/0000-0002-7836-8417; Nizkorodov, Sergey/0000-0003-0891-0052; Rudich, Yinon/0000-0003-3149-0201 FU USA-Israel Binational Science Foundation (BSF) [2012013]; German Israel Science Foundation [1136-26.8/2011]; U.S. Department of Commerce, National Oceanic and Atmospheric Administration through Climate Program Office's Atmospheric Chemistry, Carbon Cycle and Climate (AC4) Program; NOAA AC4 program [NA13OAR4310066, NA13OAR4310062]; U.S. DOE's Office of Biological and Environmental Research; U.S. DOE by Battelle Memorial Institute [DE-AC06-76RL0 1830]; Jinich Postdoctoral Fellowship FX This research was supported by research grants from the USA-Israel Binational Science Foundation (BSF) grant #2012013 and by the German Israel Science Foundation (grant #1136-26.8/2011). We thank Avi Lavi for his help with the ToF-AMS measurements, and John Nowak and Charles Brock for their helpful suggestions. RAW and SSB acknowledge financial support from the U.S. Department of Commerce, National Oceanic and Atmospheric Administration through Climate Program Office's Atmospheric Chemistry, Carbon Cycle and Climate (AC4) Program. The PNNL and UCI groups acknowledge support by the NOAA AC4 program, awards NA13OAR4310066 (PNNL) and NA13OAR4310062 (UCI). The nano-DESI/HR-MS experiments described in this paper were performed at the Environmental Molecular Sciences Laboratory, a national scientific user facility sponsored by U.S. DOE's Office of Biological and Environmental Research and located at the Pacific Northwest National Laboratory (PNNL). PNNL is operated for U.S. DOE by Battelle Memorial Institute under Contract No. DE-AC06-76RL0 1830. JMF is supported by a research grant from the Jinich Postdoctoral Fellowship. NR 98 TC 24 Z9 25 U1 10 U2 75 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 2014 VL 16 IS 22 BP 10629 EP 10642 DI 10.1039/c4cp01009d PG 14 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AI3SF UT WOS:000336781500042 PM 24752662 ER PT J AU Vijayakumar, M Govind, N Walter, E Burton, SD Shukla, A Devaraj, A Xiao, J Liu, J Wang, CM Karim, A Thevuthasan, S AF Vijayakumar, M. Govind, Niranjan Walter, Eric Burton, Sarah D. Shukla, Anil Devaraj, Arun Xiao, Jie Liu, Jun Wang, Chongmin Karim, Ayman Thevuthasan, S. TI Molecular structure and stability of dissolved lithium polysulfide species SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID RAY-ABSORPTION SPECTROSCOPY; DENSITY-FUNCTIONAL THEORY; LI-S BATTERIES; SULFUR BATTERIES; LIQUID ELECTROLYTES; GRAPHENE OXIDE; IONIC LIQUIDS; RADICAL-ANION; CARBON PAPER; BASIS-SET AB The ability to predict the solubility and stability of lithium polysulfide is vital in realizing longer lasting lithium-sulfur batteries. Herein we report combined experimental and computational analyses to understand the dissolution mechanism of lithium polysulfide species in an aprotic solvent medium. Multi-uclear NMR, variable temperature ESR and sulfur K-edge XAS analyses reveal that the lithium exchange between polysulfide species and solvent molecules constitutes the first step in the dissolution process. Lithium exchange leads to de-lithiated polysulfide ions (S-n(2-)) which subsequently form highly reactive free radicals through dissociation reaction (S-n(2-) -> 2S(n/2)(center dot-)). The energy required for the dissociation and possible dimer formation reactions of the polysulfide species is analyzed using density functional theory (DFT) based calculations. Based on these findings, we discuss approaches to optimize the electrolyte in order to control the polysulfide solubility. C1 [Vijayakumar, M.; Govind, Niranjan; Walter, Eric; Burton, Sarah D.; Shukla, Anil; Devaraj, Arun; Xiao, Jie; Liu, Jun; Wang, Chongmin; Karim, Ayman; Thevuthasan, S.] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Vijayakumar, M (reprint author), Pacific NW Natl Lab, Richland, WA 99352 USA. EM Vijay@pnnl.gov RI Murugesan, Vijayakumar/C-6643-2011; Karim, Ayman/G-6176-2012; Walter, Eric/P-9329-2016 OI Murugesan, Vijayakumar/0000-0001-6149-1702; Karim, Ayman/0000-0001-7449-542X; FU U.S. Department of Energy (DOE) [DE-AC05-76RLO1830]; Joint Center for Energy Storage Research (JCESR), an Energy Innovation Hub - U.S. Department of Energy, Office of Science, Basic Energy Sciences (BES); DOE's Office of Biological and Environmental Research; US Department of Energy, Office of Basic Energy Sciences [DE-FG02-05ER15688]; Synchrotron Catalysis Consortium FX We thank Drs Karl T. Mueller and Jianzhi Hu for their support and fruitful discussions. The research described in this paper is part of the Chemical Imaging Initiative led by Dr Lou Terminello at Pacific Northwest National Laboratory (PNNL). It was conducted under the Laboratory Directed Research and Development Program at PNNL, a multi-program national laboratory operated by Battelle under Contract DE-AC05-76RLO1830 for the U.S. Department of Energy (DOE). The synthesis part of this work is supported by the Joint Center for Energy Storage Research (JCESR), an Energy Innovation Hub funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences (BES). The NMR, MS and DFT computation work was carried out at EMSL (www.emsl.pnl.gov), a national scientific user facility sponsored by the DOE's Office of Biological and Environmental Research. Use of the National Synchrotron Light Source, at Brookhaven National Laboratory, for the XANES experiments was supported by the US Department of Energy, Office of Basic Energy Sciences (Grant# DE-FG02-05ER15688). Beamline X-19A is supported, in part, by the Synchrotron Catalysis Consortium. NR 59 TC 41 Z9 41 U1 14 U2 151 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 2014 VL 16 IS 22 BP 10923 EP 10932 DI 10.1039/c4cp00889h PG 10 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AI3SF UT WOS:000336781500076 PM 24770561 ER PT J AU Ortega, C Liao, RL Anderson, LN Rustad, T Ollodart, AR Wright, AT Sherman, DR Grundner, C AF Ortega, Corrie Liao, Reiling Anderson, Lindsey N. Rustad, Tige Ollodart, Anja R. Wright, Aaron T. Sherman, David R. Grundner, Christoph TI Mycobacterium tuberculosis Ser/Thr Protein Kinase B Mediates an Oxygen-Dependent Replication Switch SO PLOS BIOLOGY LA English DT Article ID ACCURATE MASS; PKNB; IDENTIFICATION; LATENCY; RESPIRATION; INHIBITORS; DORMANCY; PHOSPHORYLATION; PERSISTENCE; ACTIVATION AB The majority of Mycobacterium tuberculosis (Mtb) infections are clinically latent, characterized by drug tolerance and little or no bacterial replication. Low oxygen tension is a major host factor inducing bacteriostasis, but the molecular mechanisms driving oxygen-dependent replication are poorly understood. Here, we tested the role of serine/threonine phosphorylation in the Mtb response to altered oxygen status, using an in vitro model of latency (hypoxia) and reactivation (reaeration). Broad kinase inhibition compromised survival of Mtb in reaeration. Activity-based protein profiling and genetic mutation identified PknB as the kinase critical for surviving hypoxia. Mtb replication was highly sensitive to changes in PknB levels in aerated culture, and even more so in hypoxia. A mutant overexpressing PknB specifically in hypoxia showed a 10-fold loss in viability and gross morphological defects in low oxygen conditions. In contrast, chemically reducing PknB activity during hypoxia specifically compromised resumption of growth during reaeration. These data support a model in which PknB activity is reduced to achieve bacteriostasis, and elevated when replication resumes. Together, these data show that phosphosignaling controls replicative transitions associated with latency and reactivation, that PknB is a major regulator of these transitions, and that PknB could provide a highly vulnerable therapeutic target at every step of the Mtb life cycle-active disease, latency, and reactivation. C1 [Ortega, Corrie; Liao, Reiling; Rustad, Tige; Ollodart, Anja R.; Sherman, David R.; Grundner, Christoph] Seattle Biomed Res Inst, Seattle, WA 98109 USA. [Ortega, Corrie; Sherman, David R.; Grundner, Christoph] Univ Washington, Dept Global Hlth, Seattle, WA 98195 USA. [Anderson, Lindsey N.; Wright, Aaron T.] Pacific NW Natl Lab, Div Biol Sci, Richland, WA 99352 USA. RP Ortega, C (reprint author), Seattle Biomed Res Inst, 4 Nickerson St, Seattle, WA 98109 USA. EM Christoph.Grundner@seattlebiomed.org RI Anderson, Lindsey /S-6375-2016; OI Anderson, Lindsey /0000-0002-8741-7823; Wright, Aaron/0000-0002-3172-5253 FU Paul G. Allen Family Foundation [8999]; American Lung Association; University of Washington Center for AIDS Research, an NIH [P30AI027757]; NIAID; NCI; NIMH; NIDA; NICHD; NHLBI; NIA; American Society of Microbiology Robert D. Watkins Graduate Research Fellowship; Laboratory Directed Research and Development Program at PNNL; NIGMS [P41 GM103493] FX C.G. was supported by the Paul G. Allen Family Foundation (8999); the American Lung Association; and a New Investigator Award by the University of Washington Center for AIDS Research, an NIH-funded program (P30AI027757) that is supported by the following NIH Institutes and Centers: NIAID, NCI, NIMH, NIDA, NICHD, NHLBI, and NIA. C.O. is the recipient of an American Society of Microbiology Robert D. Watkins Graduate Research Fellowship. A. T. W. and L.N.A. were supported by the Laboratory Directed Research and Development Program at PNNL and the NIGMS (P41 GM103493). This research used instrumentation and capabilities developed under support from the NIGMS and the U.S. DOE. Proteomic measurements were made in the Environmental Molecular Sciences Laboratory, a DOE-BER national scientific user facility at PNNL. The funders had no role in study design, data collection and analysis, decision to publish, or preparation of the manuscript. NR 49 TC 17 Z9 18 U1 1 U2 12 PU PUBLIC LIBRARY SCIENCE PI SAN FRANCISCO PA 1160 BATTERY STREET, STE 100, SAN FRANCISCO, CA 94111 USA SN 1545-7885 J9 PLOS BIOL JI PLoS. Biol. PD JAN PY 2014 VL 12 IS 1 AR e1001746 DI 10.1371/journal.pbio.1001746 PG 11 WC Biochemistry & Molecular Biology; Biology SC Biochemistry & Molecular Biology; Life Sciences & Biomedicine - Other Topics GA AI4JT UT WOS:000336832200003 PM 24409094 ER PT S AU Perillo, EP De Haro, L Phipps, ME Martinez, JS Yeh, HC Dunn, AK Shepherd, DP Werner, JH AF Perillo, Evan P. De Haro, Leyma Phipps, Mary E. Martinez, Jennifer S. Yeh, Hsin-Chih Dunn, Andrew K. Shepherd, Douglas P. Werner, James H. BE Enderlein, J Gregor, I Gryczynski, ZK Erdmann, R Koberling, F TI Enhanced 3D localization of individual RNA transcripts via astigmatic imaging SO SINGLE MOLECULE SPECTROSCOPY AND SUPERRESOLUTION IMAGING VII SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Single Molecule Spectroscopy and Superresolution Imaging VII CY FEB 01-02, 2014 CL San Francisco, CA SP SPIE DE smFISH; single-molecule localization; astigmatic imaging; fluorescence microscopy; gene expression ID OPTICAL RECONSTRUCTION MICROSCOPY; GENE-EXPRESSION; IN-SITU; OSTEOCLAST DIFFERENTIATION; SINGLE CELLS; STEM-CELLS; OSTEOBLAST; REVEALS; YEAST; PARTICLES AB Here we present an automated microscope capable of 3D multi-color single molecule localization of individual messenger RNA molecules in a wide range of cell types. We have implemented astigmatic imaging with a cylindrical lens to improve z-localization, and a maximum likelihood estimator on a graphics processing unit to improve localization precision and speed. This microscope will aid in gene expression analysis by its capability to perform high throughput imaging of thick cells and tissues while still maintaining sufficient z resolution to resolve single RNA transcripts in three dimensions. Enhanced z-localization allows for resolving membrane localized and co-localized transcripts. C1 [Perillo, Evan P.; Yeh, Hsin-Chih; Dunn, Andrew K.] Univ Texas Austin, Dept Biomed Engn, Austin, TX 78712 USA. [De Haro, Leyma; Phipps, Mary E.; Martinez, Jennifer S.; Shepherd, Douglas P.; Werner, James H.] Los Alamos Natl Lab, Ctr Intergrated Nanotechnol, Los Alamos, NM 87544 USA. [Shepherd, Douglas P.] Univ Colorado, Dept Phys, Denver, CO 80204 USA. RP Perillo, EP (reprint author), Univ Texas Austin, Dept Biomed Engn, Austin, TX 78712 USA. EM douglas.shepherd@ucdenver.edu; jwerner@lanl.gov RI Dunn, Andrew/I-9527-2014 FU Los Alamos National Laboratory Directed Research and Development (LDRD); Center for Integrated Nanotechnologies; U.S.Department of Energy; Office of Basic Energy Science suserfacility at Los Alamos National Laboratory [DE-AC5206NA25396]; Sandia National Laboratories [DE-AC04-94AL85000] FX This work was supported through Los Alamos National Laboratory Directed Research and Development (LDRD) and was performed at the Center for Integrated Nanotechnologies ,a U.S.Department of Energy, Office of Basic Energy Science suserfacility at Los Alamos National Laboratory (Contract DE-AC5206NA25396) and Sandia National Laboratories (Contract DE-AC04-94AL85000). NR 39 TC 0 Z9 0 U1 1 U2 8 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9863-2 J9 PROC SPIE PY 2014 VL 8950 AR UNSP 895003 DI 10.1117/12.2038197 PG 11 WC Instruments & Instrumentation; Optics; Spectroscopy SC Instruments & Instrumentation; Optics; Spectroscopy GA BA4ZV UT WOS:000336479700001 ER PT J AU Martin, JE Solis, KJ AF Martin, James E. Solis, Kyle J. TI Symmetry-breaking magnetic fields create a vortex fluid that exhibits a negative viscosity, active wetting, and strong mixing SO SOFT MATTER LA English DT Article ID MICROFLUIDIC SYSTEMS; APPLIED PHYSICS; MICRODROPLETS; CHIP; MANIPULATION; MICROMIXERS; INTERFACES; DROPLETS; LAB AB There are many areas of science and technology where being able to generate vigorous, noncontact flow would be desirable. We have discovered that three dimensional, time-dependent electric or magnetic fields having key symmetries can be used to generate controlled fluid motion by the continuous injection of energy. Unlike natural convection, this approach does not require a thermal gradient as an energy source, nor does it require gravity, so space applications are feasible. The result is a highly active material we call a vortex fluid. The homogeneous torque density of this fluid enables it to climb walls, induce ballistic droplet motion, and mix vigorously, even in such complex geometries as porous media. This vortex fluid can also exhibit a negative viscosity, which can immeasurably extend the control range of the "smart fluids" used in electro- and magnetorheological devices and can thus significantly increase their performance. Because the applied fields are uniform and modest in strength, vortex fluids of any scale can be created, making applications of any size, from directing microdroplet motion to controlling damping in magnetorheological dampers that protect bridges and buildings from earthquakes, feasible. C1 [Martin, James E.; Solis, Kyle J.] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Martin, JE (reprint author), Sandia Natl Labs, POB 5800, Albuquerque, NM 87185 USA. EM jmartin@sandia.gov; kjsolis@sandia.gov FU U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000]; Division of Materials Science, Office of Basic Energy Sciences, U.S. Department of Energy (DOE) 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. This work was supported by the Division of Materials Science, Office of Basic Energy Sciences, U.S. Department of Energy (DOE). We thank Vladimir Raksha, Paul Coombs, Tom Markantes, Bill Kittler, and Kees-Jan Delst at JDSU and Matt Groo at Novamet for supplying the magnetic platelets used in these experiments. NR 48 TC 12 Z9 12 U1 3 U2 26 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 2014 VL 10 IS 22 BP 3993 EP 4002 DI 10.1039/c4sm00280f PG 10 WC Chemistry, Physical; Materials Science, Multidisciplinary; Physics, Multidisciplinary; Polymer Science SC Chemistry; Materials Science; Physics; Polymer Science GA AI4OY UT WOS:000336845900013 PM 24733404 ER PT S AU Yeats, C Dessailly, BH Glass, EM Fremont, DH Orengo, CA AF Yeats, Corin Dessailly, Benoit H. Glass, Elizabeth M. Fremont, Daved H. Orengo, Christine A. BE Anderson, WF TI Target Selection for Structural Genomics of Infectious Diseases SO STRUCTURAL GENOMICS AND DRUG DISCOVERY: METHODS AND PROTOCOLS SE Methods in Molecular Biology LA English DT Article; Book Chapter DE Target selection; Vaccine and virulence targets; Essential proteins; Drug targets; Domain annotation; Structure homologue recognition; Secondary structure and disorder prediction; Construct boundary identification ID TRANSMEMBRANE PROTEIN TOPOLOGY; LOUIS ENCEPHALITIS-VIRUS; GRAM-NEGATIVE BACTERIA; MONOCLONAL-ANTIBODIES; MOLECULAR EVOLUTION; COWPOX INFECTION; RNA REPLICATION; VACCINIA VIRUS; E-GLYCOPROTEIN; WEB SERVICES AB This chapter describes the protocols used to identify, filter, and annotate potential protein targets from an organism associated with infectious diseases. Protocols often combine computational approaches for mining information in public databases or for checking whether the protein has already been targeted for structure determination, with manual strategies that examine the literature for information on the biological role of the protein or the experimental strategies that explore the effects of knocking out the protein. Publicly available computational tools have been cited as much as possible. Where these do not exist, the concepts underlying in-house tools developed for the Center for Structural Genomics of Infectious Diseases have been described. C1 [Yeats, Corin; Dessailly, Benoit H.; Orengo, Christine A.] UCL, Ctr Struct Genom Infect Dis, Dept Struct & Mol Biol, London, England. [Glass, Elizabeth M.] Argonne Natl Lab, Math & Comp Sci Div, Ctr Struct Genom Infect Dis, Argonne, IL 60439 USA. [Fremont, Daved H.] Ctr Struct Genom Infect Dis, St Louis, MO USA. [Fremont, Daved H.] Washington Univ, Dept Pathol & Immunol, St Louis, MO USA. [Fremont, Daved H.] Washington Univ, Dept Biochem & Mol Biophys, St Louis, MO USA. RP Yeats, C (reprint author), UCL, Ctr Struct Genom Infect Dis, Dept Struct & Mol Biol, London, England. FU PHS HHS [272201200026C, 272200700058C] NR 41 TC 0 Z9 0 U1 0 U2 11 PU HUMANA PRESS INC PI TOTOWA PA 999 RIVERVIEW DR, STE 208, TOTOWA, NJ 07512-1165 USA SN 1064-3745 BN 978-1-4939-0354-2; 978-1-4939-0353-5 J9 METHODS MOL BIOL JI Methods Mol. Biol. PY 2014 VL 1140 BP 35 EP 51 DI 10.1007/978-1-4939-0354-2_3 D2 10.1007/978-1-4939-0354-2 PG 17 WC Biochemical Research Methods; Biochemistry & Molecular Biology; Pharmacology & Pharmacy SC Biochemistry & Molecular Biology; Pharmacology & Pharmacy GA BA2NQ UT WOS:000333708800004 PM 24590707 ER PT S AU Makowska-Grzyska, M Kim, Y Maltseva, N Li, H Zhou, M Joachimiak, G Babnigg, G Joachimiak, A AF Makowska-Grzyska, Magdalena Kim, Youngchang Maltseva, Natalia Li, Hui Zhou, Min Joachimiak, Grazyna Babnigg, Gyorgy Joachimiak, Andrzej BE Anderson, WF TI Protein Production for Structural Genomics Using E. coli Expression SO STRUCTURAL GENOMICS AND DRUG DISCOVERY: METHODS AND PROTOCOLS SE Methods in Molecular Biology LA English DT Article; Book Chapter DE Protein expression; Protein purification; Disposable vessel fermentation; Selenomethionine-labeling; IMAC; His-tag; High-throughput ID ETCH VIRUS PROTEASE; HIGH-THROUGHPUT; RECOMBINANT PROTEINS; LARGE-SCALE; PURIFICATION; PIPELINE; NMR; CRYSTALLIZATION; QUALITY; CLONING AB The goal of structural biology is to reveal details of the molecular structure of proteins in order to understand their function and mechanism. X-ray crystallography and NMR are the two best methods for atomic level structure determination. However, these methods require milligram quantities of proteins. In this chapter a reproducible methodology for large-scale protein production applicable to a diverse set of proteins is described. The approach is based on protein expression in E. coli as a fusion with a cleavable affinity tag that was tested on over 20,000 proteins. Specifically, a protocol for fermentation of large quantities of native proteins in disposable culture vessels is presented. A modified protocol that allows for the production of selenium-labeled proteins in defined media is also offered. Finally, a method for the purification of His(6) -tagged proteins on immobilized metal affinity chromatography columns that generates highpurity material is described in detail. C1 [Makowska-Grzyska, Magdalena; Kim, Youngchang; Maltseva, Natalia; Zhou, Min] Univ Chicago, Ctr Struct Genom Infect Dis, Chicago, IL 60637 USA. [Kim, Youngchang; Li, Hui; Zhou, Min] Argonne Natl Lab, Midwest Ctr Struct Genom, Argonne, IL 60439 USA. [Kim, Youngchang] Argonne Natl Lab, Struct Biol Ctr, Argonne, IL 60439 USA. [Joachimiak, Grazyna; Babnigg, Gyorgy; Joachimiak, Andrzej] Argonne Natl Lab, Midwest Ctr Struct Genom, Biosci Div, Argonne, IL 60439 USA. [Babnigg, Gyorgy; Joachimiak, Andrzej] Univ Chicago, Computat Inst, Ctr Struct Genom Infect Dis, Chicago, IL 60637 USA. [Joachimiak, Andrzej] Univ Chicago, Chicago, IL 60637 USA. RP Makowska-Grzyska, M (reprint author), Univ Chicago, Ctr Struct Genom Infect Dis, Chicago, IL 60637 USA. FU NIAID NIH HHS [HHSN272200700058C, HHSN272201200026C]; NIGMS NIH HHS [U54 GM094585, GM094585]; PHS HHS [272201200026C, 272200700058C] NR 29 TC 5 Z9 6 U1 2 U2 6 PU HUMANA PRESS INC PI TOTOWA PA 999 RIVERVIEW DR, STE 208, TOTOWA, NJ 07512-1165 USA SN 1064-3745 BN 978-1-4939-0354-2; 978-1-4939-0353-5 J9 METHODS MOL BIOL JI Methods Mol. Biol. PY 2014 VL 1140 BP 89 EP 105 DI 10.1007/978-1-4939-0354-2_7 D2 10.1007/978-1-4939-0354-2 PG 17 WC Biochemical Research Methods; Biochemistry & Molecular Biology; Pharmacology & Pharmacy SC Biochemistry & Molecular Biology; Pharmacology & Pharmacy GA BA2NQ UT WOS:000333708800008 PM 24590711 ER PT S AU Tan, KM Kim, Y Hatzos-Skintges, C Chang, C Cuff, M Chhor, G Osipiuk, J Michalska, K Nocek, B An, H Babnigg, G Bigelow, L Joachimiak, G Li, H Mack, J Makowska--Grzyska, M Maltseva, N Mulligan, R Tesar, C Zhou, M Joachimiak, A AF Tan, Kemin Kim, Youngchang Hatzos-Skintges, Catherine Chang, Changsoo Cuff, Marianne Chhor, Gekleng Osipiuk, Jerzy Michalska, Karolina Nocek, Boguslaw An, Hao Babnigg, Gyorgy Bigelow, Lance Joachimiak, Grazyna Li, Hui Mack, Jamey Makowska--Grzyska, Magdalena Maltseva, Natalia Mulligan, Rory Tesar, Christine Zhou, Min Joachimiak, Andrzej BE Anderson, WF TI Salvage of Failed Protein Targets by Reductive Alkylation SO STRUCTURAL GENOMICS AND DRUG DISCOVERY: METHODS AND PROTOCOLS SE Methods in Molecular Biology LA English DT Article; Book Chapter DE Chemical modification; Lysine reductive alkylation; Methylation; Ethylation; Isopropylation; Protein crystallization ID LYSINE RESIDUES; CRYSTALLIZATION; METHYLATION; INTERFACES; RESOLUTION; LYSOZYME AB The growth of diffraction-quality single crystals is of primary importance in protein X-ray crystallography. Chemical modification of proteins can alter their surface properties and crystallization behavior. The Midwest Center for Structural Genomics (MCSG) has previously reported how reductive methylation of lysine residues in proteins can improve crystallization of unique proteins that initially failed to produce diffraction-quality crystals. Recently, this approach has been expanded to include ethylation and isopropylation in the MCSG protein crystallization pipeline. Applying standard methods, 180 unique proteins were alkylated and screened using standard crystallization procedures. Crystal structures of 12 new proteins were determined, including the first ethylated and the first isopropylated protein structures. In a few cases, the structures of native and methylated or ethylated states were obtained and the impact of reductive alkylation of lysine residues was assessed. Reductive methylation tends to be more efficient and produces the most alkylated protein structures. Structures of methylated proteins typically have higher resolution limits. A number of well-ordered alkylated lysine residues have been identified, which make both intermolecular and intramolecular contacts. The previous report is updated and complemented with the following new data; a description of a detailed alkylation protocol with results, structural features, and roles of alkylated lysine residues in protein crystals. These contribute to improved crystallization properties of some proteins. C1 [Tan, Kemin; Hatzos-Skintges, Catherine; Chang, Changsoo; Cuff, Marianne; Chhor, Gekleng; Osipiuk, Jerzy; Michalska, Karolina; Nocek, Boguslaw; An, Hao; Babnigg, Gyorgy; Bigelow, Lance; Joachimiak, Grazyna; Mack, Jamey; Tesar, Christine; Joachimiak, Andrzej] Argonne Natl Lab, Midwest Ctr Struct Genom, Biosci Div, Argonne, IL 60439 USA. [Tan, Kemin; Chang, Changsoo; Cuff, Marianne; Osipiuk, Jerzy; Michalska, Karolina; Nocek, Boguslaw] Argonne Natl Lab, Struct Biol Ctr, Biosci Div, Argonne, IL 60439 USA. [Tan, Kemin; Osipiuk, Jerzy; Nocek, Boguslaw; Babnigg, Gyorgy; Mulligan, Rory; Joachimiak, Andrzej] Univ Chicago, Computat Inst, Ctr Struct Genom Infect Dis, Chicago, IL 60637 USA. [Kim, Youngchang; Makowska--Grzyska, Magdalena; Maltseva, Natalia; Zhou, Min] Univ Chicago, Ctr Struct Genom Infect Dis, Chicago, IL 60637 USA. [Kim, Youngchang; Li, Hui; Zhou, Min] Argonne Natl Lab, Midwest Ctr Struct Genom, Argonne, IL 60439 USA. [Kim, Youngchang] Argonne Natl Lab, Struct Biol Ctr, Argonne, IL 60439 USA. [Joachimiak, Andrzej] Univ Chicago, Chicago, IL 60637 USA. RP Tan, KM (reprint author), Argonne Natl Lab, Midwest Ctr Struct Genom, Biosci Div, 9700 S Cass Ave, Argonne, IL 60439 USA. FU NIAID NIH HHS [HHSN272200700058C, HHSN272201200026C]; NIGMS NIH HHS [U54 GM094585, GM094585, U54 GM074942]; PHS HHS [272200700058C, 272201200026C] NR 26 TC 2 Z9 2 U1 0 U2 3 PU HUMANA PRESS INC PI TOTOWA PA 999 RIVERVIEW DR, STE 208, TOTOWA, NJ 07512-1165 USA SN 1064-3745 BN 978-1-4939-0354-2; 978-1-4939-0353-5 J9 METHODS MOL BIOL JI Methods Mol. Biol. PY 2014 VL 1140 BP 189 EP 200 DI 10.1007/978-1-4939-0354-2_15 D2 10.1007/978-1-4939-0354-2 PG 12 WC Biochemical Research Methods; Biochemistry & Molecular Biology; Pharmacology & Pharmacy SC Biochemistry & Molecular Biology; Pharmacology & Pharmacy GA BA2NQ UT WOS:000333708800016 PM 24590719 ER PT S AU Goldschmidt, L Eisenberg, D Derewenda, ZS AF Goldschmidt, Lukasz Eisenberg, David Derewenda, Zygmunt S. BE Anderson, WF TI Salvage or Recovery of Failed Targets by Mutagenesis to Reduce Surface Entropy SO STRUCTURAL GENOMICS AND DRUG DISCOVERY: METHODS AND PROTOCOLS SE Methods in Molecular Biology LA English DT Article; Book Chapter DE Protein crystallization; Surface entropy reduction; Site-directed mutagenesis; Protein engineering; Crystal contacts ID RATIONAL PROTEIN CRYSTALLIZATION; SYNTHASE; RESOLUTION; MUTATIONS; MECHANISM; RESIDUES; RHOGDI AB The success of macromolecular crystallization depends on the protein's ability to form specific, cohesive intermolecular interactions that serve as crystal contacts. In the cases where the protein lacks surface patches conducive to such interactions, crystallization may not occur. However, it is possible to enhance the likelihood of crystallization by engineering such patches through site-directed mutagenesis, targeting specifically residues with high side chain entropy and replacing them with small amino acids (i.e., surface entropy reduction, SER). This method has proven successful in hundreds of crystallographic analyses of proteins otherwise recalcitrant to crystallization. Three representative cases of the application of the SER strategy, assisted by the automated prediction of the mutation sites using the SER prediction (SERp) server are described. C1 [Goldschmidt, Lukasz; Eisenberg, David] Univ Calif Los Angeles, Howard Hughes Med Inst, UCLA DOE Inst Genom & Prote, Los Angeles, CA 90024 USA. [Derewenda, Zygmunt S.] Univ Virginia, Sch Med, Dept Mol Physiol & Biol Phys, Charlottesville, VA 22908 USA. RP Goldschmidt, L (reprint author), Univ Calif Los Angeles, Howard Hughes Med Inst, UCLA DOE Inst Genom & Prote, Los Angeles, CA 90024 USA. FU NIGMS NIH HHS [GM095847] NR 19 TC 5 Z9 5 U1 0 U2 2 PU HUMANA PRESS INC PI TOTOWA PA 999 RIVERVIEW DR, STE 208, TOTOWA, NJ 07512-1165 USA SN 1064-3745 BN 978-1-4939-0354-2; 978-1-4939-0353-5 J9 METHODS MOL BIOL JI Methods Mol. Biol. PY 2014 VL 1140 BP 201 EP 209 DI 10.1007/978-1-4939-0354-2_16 D2 10.1007/978-1-4939-0354-2 PG 9 WC Biochemical Research Methods; Biochemistry & Molecular Biology; Pharmacology & Pharmacy SC Biochemistry & Molecular Biology; Pharmacology & Pharmacy GA BA2NQ UT WOS:000333708800017 PM 24590720 ER PT S AU Rajashankar, K Dauter, Z AF Rajashankar, Kanagalaghatta Dauter, Zbigniew BE Anderson, WF TI Data Collection for Crystallographic Structure Determination SO STRUCTURAL GENOMICS AND DRUG DISCOVERY: METHODS AND PROTOCOLS SE Methods in Molecular Biology LA English DT Article; Book Chapter DE Diffraction data collection; Diffraction data quality; Rotation method; Strategy ID MACROMOLECULAR CRYSTALLOGRAPHY; RADIATION-DAMAGE; STRATEGIES; QUALITY AB Diffraction data measurement is the final experimental step of crystal structure analysis; all subsequent stages are computational. Good-quality data, optimized for a particular application, make the structure solution and refinement easier and enhance the accuracy of the final models. This chapter describes the principles of the rotation method of data collection and discusses various scenarios that are useful for different types of applications, such as anomalous phasing, molecular replacement, ligand identification, etc. Some typical problems encountered in practice are also discussed. C1 [Rajashankar, Kanagalaghatta] Cornell Univ, Argonne Natl Lab, NE CAT, Argonne, IL 60439 USA. [Rajashankar, Kanagalaghatta] Cornell Univ, Argonne Natl Lab, Dept Chem & Chem Biol, Argonne, IL USA. [Dauter, Zbigniew] NCI, Synchrotron Radiat Res Sect, Macromol Crystallog Lab, Argonne Natl Lab, Argonne, IL USA. RP Rajashankar, K (reprint author), Cornell Univ, Argonne Natl Lab, NE CAT, Argonne, IL 60439 USA. FU Intramural NIH HHS; NIGMS NIH HHS [8 P41 GM103403-10] NR 24 TC 0 Z9 0 U1 0 U2 0 PU HUMANA PRESS INC PI TOTOWA PA 999 RIVERVIEW DR, STE 208, TOTOWA, NJ 07512-1165 USA SN 1064-3745 BN 978-1-4939-0354-2; 978-1-4939-0353-5 J9 METHODS MOL BIOL JI Methods Mol. Biol. PY 2014 VL 1140 BP 211 EP 237 DI 10.1007/978-1-4939-0354-2_17 D2 10.1007/978-1-4939-0354-2 PG 27 WC Biochemical Research Methods; Biochemistry & Molecular Biology; Pharmacology & Pharmacy SC Biochemistry & Molecular Biology; Pharmacology & Pharmacy GA BA2NQ UT WOS:000333708800018 PM 24590721 ER PT S AU Binkowski, TA Jiang, W Roux, B Anderson, WF Joachimiak, A AF Binkowski, T. Andrew Jiang, Wei Roux, Benoit Anderson, Wayne F. Joachimiak, Andrzej BE Anderson, WF TI Virtual High-Throughput Ligand Screening SO STRUCTURAL GENOMICS AND DRUG DISCOVERY: METHODS AND PROTOCOLS SE Methods in Molecular Biology LA English DT Article; Book Chapter DE Protein; Ligand; High-throughput screening; Docking; Molecular modeling ID FREE-ENERGY CALCULATIONS; BINDING FREE-ENERGIES; MOLECULAR-DYNAMICS; COMPUTER-SIMULATIONS; ANALYTICAL SHAPE; T4 LYSOZYME; COMPUTATION; PROTEINS; DOCKING; MODEL AB In Structural Genomics projects, virtual high-throughput ligand screening can be utilized to provide important functional details for newly determined protein structures. Using a variety of publicly available software tools, it is possible to computationally model, predict, and evaluate how different ligands interact with a given protein. At the Center for Structural Genomics of Infectious Diseases (CSGID) a series of protein analysis, docking and molecular dynamics software is scripted into a single hierarchical pipeline allowing for an exhaustive investigation of protein-ligand interactions. The ability to conduct accurate computational predictions of protein-ligand binding is a vital component in improving both the efficiency and economics of drug discovery. Computational simulations can minimize experimental efforts, the slowest and most cost prohibitive aspect of identifying new therapeutics. C1 [Binkowski, T. Andrew; Joachimiak, Andrzej] Univ Chicago, Ctr Struct Genom Infect Dis, Computat Inst, Chicago, IL 60637 USA. [Jiang, Wei] Argonne Natl Lab, Argonne Leadership Comp Facil, Argonne, IL 60439 USA. [Roux, Benoit] Univ Chicago, Dept Biochem & Mol Biol, Chicago, IL 60637 USA. [Anderson, Wayne F.] Northwestern Univ, Feinberg Sch Med, Ctr Struct Genom Infect Dis, Chicago, IL 60611 USA. [Anderson, Wayne F.] Northwestern Univ, Feinberg Sch Med, Midwest Ctr Struct Genom, Chicago, IL 60611 USA. [Joachimiak, Andrzej] Argonne Natl Lab, Midwest Ctr Struct Genom, Biosci Div, Argonne, IL 60439 USA. [Joachimiak, Andrzej] Univ Chicago, Chicago, IL 60637 USA. RP Binkowski, TA (reprint author), Univ Chicago, Ctr Struct Genom Infect Dis, Computat Inst, Chicago, IL 60637 USA. FU NIAID NIH HHS [HHSN272201200026C, HHSN272200700058C]; NIGMS NIH HHS [GM094585, U54 GM074942, U54 GM094585]; PHS HHS [272200700058C, 272201200026C] NR 42 TC 2 Z9 2 U1 0 U2 2 PU HUMANA PRESS INC PI TOTOWA PA 999 RIVERVIEW DR, STE 208, TOTOWA, NJ 07512-1165 USA SN 1064-3745 BN 978-1-4939-0354-2; 978-1-4939-0353-5 J9 METHODS MOL BIOL JI Methods Mol. Biol. PY 2014 VL 1140 BP 251 EP 261 DI 10.1007/978-1-4939-0354-2_19 D2 10.1007/978-1-4939-0354-2 PG 11 WC Biochemical Research Methods; Biochemistry & Molecular Biology; Pharmacology & Pharmacy SC Biochemistry & Molecular Biology; Pharmacology & Pharmacy GA BA2NQ UT WOS:000333708800020 PM 24590723 ER PT S AU Sulakhe, D Balasubramanian, S Xie, BQ Berrocal, E Feng, B Taylor, A Chitturi, B Dave, U Agam, G Xu, JB Bornigen, D Dubchak, I Gilliam, TC Maltsev, N AF Sulakhe, Dinanath Balasubramanian, Sandhya Xie, Bingqing Berrocal, Eduardo Feng, Bo Taylor, Andrew Chitturi, Bhadrachalam Dave, Utpal Agam, Gady Xu, Jinbo Boernigen, Daniela Dubchak, Inna Gilliam, T. Conrad Maltsev, Natalia BE Maltsev, N Rzhetsky, A Gilliam, TC TI High-Throughput Translational Medicine: Challenges and Solutions SO SYSTEMS ANALYSIS OF HUMAN MULTIGENE DISORDERS SE Advances in Experimental Medicine and Biology LA English DT Article; Book Chapter ID GENE-EXPRESSION DATA; NEURAL-TUBE DEFECTS; CANDIDATE DISEASE GENES; SET ENRICHMENT ANALYSIS; VITAMIN B-12 RECEPTOR; SPINA-BIFIDA; ENVIRONMENT INTERACTIONS; COMPUTATIONAL TOOLS; SEQUENCE DATABASE; MICROARRAY DATA AB Recent technological advances in genomics now allow producing biological data at unprecedented tera- and petabyte scales. Yet, the extraction of useful knowledge from this voluminous data presents a significant challenge to a scientific community. Efficient mining of vast and complex data sets for the needs of biomedical research critically depends on seamless integration of clinical, genomic, and experimental information with prior knowledge about genotype-phenotype relationships accumulated in a plethora of publicly available databases. Furthermore, such experimental data should be accessible to a variety of algorithms and analytical pipelines that drive computational analysis and data mining. Translational projects require sophisticated approaches that coordinate and perform various analytical steps involved in the extraction of useful knowledge from accumulated clinical and experimental data in an orderly semiautomated manner. It presents a number of challenges such as (1) high-throughput data management involving data transfer, data storage, and access control; (2) scalable computational infrastructure; and (3) analysis of large-scale multidimensional data for the extraction of actionable knowledge. We present a scalable computational platform based on crosscutting requirements from multiple scientific groups for data integration, management, and analysis. The goal of this integrated platform is to address the challenges and to support the end-to-end analytical needs of various translational projects. C1 [Sulakhe, Dinanath; Dave, Utpal; Gilliam, T. Conrad; Maltsev, Natalia] Univ Chicago, Computat Inst, Argonne Natl Lab, Chicago, IL 60637 USA. [Balasubramanian, Sandhya; Xie, Bingqing; Berrocal, Eduardo; Feng, Bo; Taylor, Andrew; Boernigen, Daniela; Gilliam, T. Conrad; Maltsev, Natalia] Univ Chicago, Dept Human Genet, Chicago, IL 60637 USA. [Xie, Bingqing; Berrocal, Eduardo; Feng, Bo; Agam, Gady] IIT, Dept Comp Sci, Chicago, IL 60616 USA. [Chitturi, Bhadrachalam] Amrita Vishwa Vidyapeetham Univ, Dept Comp Sci, Kollam, Kerala, India. [Xu, Jinbo; Boernigen, Daniela] Toyota Technol Inst, Chicago, IL USA. [Dubchak, Inna] Berkley Natl Lab, Genom Div, Walnut Creek, CA USA. RP Sulakhe, D (reprint author), Univ Chicago, Computat Inst, Argonne Natl Lab, 5735 S Ellis Ave, Chicago, IL 60637 USA. EM sulakhe@mcs.anl.gov; Maltsev@uchicago.edu FU NHLBI NIH HHS [R01 HL091495]; NINDS NIH HHS [NS050375] NR 110 TC 4 Z9 5 U1 1 U2 5 PU SPRINGER PI NEW YORK PA 233 SPRING STREET, NEW YORK, NY 10013, UNITED STATES SN 0065-2598 BN 978-1-4614-8777-7; 978-1-4614-8778-4 J9 ADV EXP MED BIOL JI Adv.Exp.Med.Biol. PY 2014 VL 799 BP 39 EP 67 DI 10.1007/978-1-4614-8778-4_3 D2 10.1007/978-1-4614-8778-4 PG 29 WC Genetics & Heredity; Medicine, Research & Experimental SC Genetics & Heredity; Research & Experimental Medicine GA BA2PX UT WOS:000333762700004 PM 24292961 ER PT J AU Hou, WT Lancaster, L Li, DS Bowlus, A Bozhilov, K Kisailus, D AF Hou, Wenting Lancaster, Louis Li, Dongsheng Bowlus, Ana Bozhilov, Krassimir Kisailus, David TI Biologically inspired synthesis of highly branched zinc oxide nanowires SO BIOINSPIRED BIOMIMETIC AND NANOBIOMATERIALS LA English DT Article DE bioinspired; crystal growth; nanomaterial; nanowire; photocatalyst; semiconductor; solar; synthesis ID SENSITIZED SOLAR-CELLS; ZNO NANOSTRUCTURES; VAPOR-DEPOSITION; NANOTREE ARRAYS; LOW-TEMPERATURE; THIN-FILMS; GROWTH; NANOPARTICLES; NANORODS; ORIENTATION AB Biological mineralization demonstrates how nature can produce elegant structures through controlled organic-mineral interactions. These organics are often used to control shape, size and orientation of mineral. Inspired from nature, the authors utilize an organic agent, ethylenediamine, as a mineralizer to inhibit rapid hydrolysis and condensation of zinc oxide, and thus control crystal growth behavior. Through adjustment of synthesis parameters, such as precursor concentration and the molar ratio of the inorganic precursor and organic ligands, the authors investigate the mechanism of formation of highly branched zinc oxide nanostructures, which can be used for improving efficiency in energy conversion and water purification applications. C1 [Hou, Wenting; Lancaster, Louis; Li, Dongsheng; Bowlus, Ana; Kisailus, David] Univ Calif Riverside, Dept Chem & Environm Engn, Riverside, CA 92521 USA. [Li, Dongsheng] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. [Bozhilov, Krassimir] Univ Calif Riverside, Mat Sci & Engn Program, Cent Facil Adv Microscopy & Microanal, Riverside, CA 92521 USA. [Kisailus, David] Univ Calif Riverside, Riverside, CA 92521 USA. RP Kisailus, D (reprint author), Univ Calif Riverside, Dept Chem & Environm Engn, Riverside, CA 92521 USA. EM david@engr.ucr.edu NR 54 TC 1 Z9 1 U1 1 U2 28 PU ICE PUBLISHING PI WESTMINISTER PA INST CIVIL ENGINEERS, 1 GREAT GEORGE ST, WESTMINISTER SW 1P 3AA, ENGLAND SN 2045-9858 EI 2045-9866 J9 BIOINSPIR BIOMIM NAN JI Bioinspired Biomim. Nanobiomat. PY 2014 VL 3 IS 1 BP 10 EP 18 DI 10.1680/bbn.13.00019 PG 9 WC Engineering, Biomedical; Materials Science, Biomaterials SC Engineering; Materials Science GA AH8ZS UT WOS:000336428400004 ER PT J AU Davis, EB Richard, TL AF Davis, Ethan B. Richard, Tom L. TI Biomass energy and the implications for climate and food The US response SO BULLETIN OF THE ATOMIC SCIENTISTS LA English DT Article DE agricultural production; bioenergy; carbon sequestration; climate change; consumption; food security; greenhouse gases; income; meat; perennial grasses AB Many experts have concluded that, if greenhouse gas concentrations are to be limited while the world's energy demands are nonetheless met, biomass energy will be an indispensable resource. At the same time, climate change is expected to affect agricultural productivity adverselyand 15 percent of people in developing countries, according to the UN's Food and Agriculture Organization, already suffer from extreme food insecurity. Authors from three countriesJose R. Moreira of Brazil (2014), Roberto Bissio of Uruguay (2014), and Ethan B. Davis and Tom L. Richard of the United Statesexplore how the potential climate mitigation benefits of devoting arable land to the production of biomass energy can be achieved without further undermining food security in the developing world. C1 [Davis, Ethan B.] Penn State Univ, University Pk, PA 16802 USA. [Davis, Ethan B.] Dartmouth Coll, Thayer Sch Engn, Hanover, NH 03755 USA. [Davis, Ethan B.] Oak Ridge Natl Lab, Dept Energy, Oak Ridge, TN USA. [Richard, Tom L.] Penn States Inst Energy & Environm, University Pk, PA USA. RP Davis, EB (reprint author), Penn State Univ, University Pk, PA 16802 USA. NR 12 TC 2 Z9 2 U1 3 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 PY 2014 VL 70 IS 1 BP 16 EP 20 DI 10.1177/0096340213516739 PG 5 WC International Relations; Social Issues SC International Relations; Social Issues GA AH1PD UT WOS:000335892400004 ER PT J AU Mossine, AV Mayhan, CM Fowler, DA Teat, SJ Deakyne, CA Atwood, JL AF Mossine, Andrew V. Mayhan, Collin M. Fowler, Drew A. Teat, Simon J. Deakyne, Carol A. Atwood, Jerry L. TI Zinc-seamed pyrogallol[4]arene dimers as structural components in a two-dimensional MOF SO CHEMICAL SCIENCE LA English DT Article ID MOLECULAR CAPSULES; COORDINATION; NANOCAPSULES; GEOMETRIES; FERROCENE; COMPLEXES; GUEST AB The synthesis of a two-dimensional (2D) metal-organic framework (MOF) is described wherein Zn-seamed pyrogallol[4] arene (PgC(x)) nanocapsules are utilized as supramolecular building blocks with 4,4'-bipyridine (bpy) linkers. The choice of linker and of crystallization solvent (DMSO) was guided by electronic structure calculations on the zinc model complexes Zn(C2H3O2)(2)L, which showed that bpy and DMSO have similar Zn-L binding strengths and that there is little drop-off in binding strength when bpy is bound to a second Zn(C2H3O2)(2) moiety. The MOF features unusual coordination geometries at the zinc centres along the nanocapsular periphery when compared to previous examples of zinc-seamed nanocapsules. The change in coordination geometry leads to a compulsory change in the internal volume of the nanocapsule as well as the behaviour of the encapsulated guest molecule. There are also several well defined voids and channels within the structure. C1 [Mossine, Andrew V.; Mayhan, Collin M.; Fowler, Drew A.; Deakyne, Carol A.; Atwood, Jerry L.] Univ Missouri, Dept Chem, Columbia, MO 65211 USA. [Teat, Simon J.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Deakyne, CA (reprint author), Univ Missouri, Dept Chem, Columbia, MO 65211 USA. EM sjteat@lbl.gov; DeakyneC@missouri.edu; atwoodj@missouri.edu FU NSF; NIBIB [T21 EB004822]; Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231] FX We thank NSF for support of this work (J.L.A.) as well as NIBIB training grant T21 EB004822 (A.V.M.). The computations were performed on the HPC resources at the University of Missouri Bioinformatics Consortium (UMBC). 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 27 TC 6 Z9 6 U1 11 U2 44 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 2014 VL 5 IS 6 BP 2297 EP 2303 DI 10.1039/c4sc00462k PG 7 WC Chemistry, Multidisciplinary SC Chemistry GA AH6QA UT WOS:000336254500023 ER PT J AU Ouizem, S Rosario-Amorin, D Dickie, DA Paine, RT de Bettencourt-Dias, A Hay, BP Podair, J Delmau, LH AF Ouizem, Sabrina Rosario-Amorin, Daniel Dickie, Diane A. Paine, Robert T. de Bettencourt-Dias, A. Hay, Benjamin P. Podair, Julien Delmau, Ltitia H. TI Synthesis and f-element ligation properties of NCMPO-decorated pyridine N-oxide platforms SO DALTON TRANSACTIONS LA English DT Article ID LANTHANIDE COORDINATION CHEMISTRY; MM3 FORCE-FIELD; MOLECULAR-STRUCTURES; EXTRACTION PROPERTIES; NITRIC-ACID; WIDE RIM; MULTICOORDINATE LIGANDS; SOLVENT-EXTRACTION; FISSION-PRODUCTS; WATER-MOLECULES AB Stepwise syntheses of 2-{[2-(diphenylphosphoryl)acetamido]methyl}pyridine 1-oxide, 2-[Ph2P(O)CH2C(O)N( H)CH2]C5H4NO (6), 2-{[2-(diphenylphosphoryl)acetamido]methyl}-6-[(diphenylphosphoryl)methyl]pyridine 1-oxide, 2-[Ph2P(O)CH2C(O)N(H)CH2]-6-[Ph2P(O)CH2]C5H3NO (7) and 2,6-bis{[2-(diphenylphosphoryl) acetamido] methyl} pyridine 1-oxide, 2,6-[Ph2P(O)CH2C(O)N(H)CH2](2)C5H3NO (8), are reported along with spectroscopic characterization data and single crystal X-ray diffraction structure determination for 6 center dot 2H(2)O, 7 and 2,6-[Ph2P(O)CH2C(O)N(H)CH2](2)C5H3N center dot MeOH 18 center dot MeOH, the pyridine precursor of 8. Molecular mechanics computations indicate that 6, 7 and 8 should experience minimal steric hindrance to donor group reorganization that would permit tridentate, tetradentate and pentadentate docking structures for the respective ligands on lanthanide cations. However, crystal structure determination for the lanthanide complexes, {[Yb(6)(NO3)(3)]center dot(MeOH)}(n), {[Lu(6)(NO3)(3)]center dot(MeOH)}(n), [Er(6)(2)(H2O)(2)](NO3)(3)center dot(H2O)(4)}(n), {[La(13)(NO3)(3)(MeOH)]center dot(MeOH)}(n), {[Eu(7){NO3)(2)(EtOAc)(0.5)(H2O)(0.5)](NO3)}(2)center dot MeOH and [Dy-3(7)(4)(NO3)(4)(H2O)(2)](NO3)(5)center dot(MeOH)(5)center dot(H2O)(2) reveal solid-state structures with mixed chelating/bridging ligand : Ln(III) interactions that employ lower than the maximal denticity. The binding of 6 and 7 with Eu(III) in the solid state and in MeOH solutions is also accessed by emission spectroscopy. The acid dependence for solvent extractions with 6 and 7 in 1,2-dichloroethane for Eu(III) and Am(III) in nitric acid solutions is described and compared with the behavior of n-octyl(phenyl)-N, N-diisobutylcarbamoylmethylphosphine oxide (OPhDiBCMPO, 1b) and 2-[(diphenyl) phosphinoylmethyl] pyridine N-oxide (DPhNOPO, 4a). C1 [Ouizem, Sabrina; Rosario-Amorin, Daniel; Dickie, Diane A.; Paine, Robert T.] Univ New Mexico, Dept Chem & Chem Biol, Albuquerque, NM 87131 USA. [de Bettencourt-Dias, A.] Univ Nevada, Dept Chem, Reno, NV 89557 USA. [Hay, Benjamin P.; Podair, Julien; Delmau, Ltitia H.] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. RP Paine, RT (reprint author), Univ New Mexico, Dept Chem & Chem Biol, Albuquerque, NM 87131 USA. EM rtpaine@unm.edu RI Dickie, Diane/B-1647-2010 OI Dickie, Diane/0000-0003-0939-3309 FU University of New Mexico; Division of Chemical Sciences, Geosciences and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy [DE-FG02-03ER15419]; National Science Foundation [CHE-0443580]; NMR spectrometers [CHE-0840523, -0946690]; NSF [CHE-1058805] FX Financial support for this study at the University of New Mexico was provided by the Division of Chemical Sciences, Geosciences and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy (Grant DE-FG02-03ER15419 (R.T.P)). In addition, funds from the National Science Foundation assisted with the purchases of the X-ray diffractometer (CHE-0443580) and NMR spectrometers (CHE-0840523 and -0946690) are acknowledged. B.P.H. and L.H.D. acknowledge support from the Division of Chemical Sciences, Geosciences and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy. AdBD acknowledges financial support from the NSF (CHE-1058805) and thanks Jorge Monteiro for assistance with photophysical data collection. NR 105 TC 7 Z9 7 U1 0 U2 18 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 2014 VL 43 IS 22 BP 8368 EP 8386 DI 10.1039/c3dt53611d PG 19 WC Chemistry, Inorganic & Nuclear SC Chemistry GA AH6PW UT WOS:000336254100030 PM 24733501 ER PT J AU Socol, Y Dobrzynski, L Doss, M Feinendegen, LE Janiak, MK Miller, ML Sanders, CL Scott, BR Ulsh, B Vaiserman, A AF Socol, Yehoshua Dobrzynski, Ludwik Doss, Mohan Feinendegen, Ludwig E. Janiak, Marek K. Miller, Mark L. Sanders, Charles L. Scott, Bobby R. Ulsh, Brant Vaiserman, Alexander TI COMMENTARY: ETHICAL ISSUES OF CURRENT HEALTH-PROTECTION POLICIES ON LOW-DOSE IONIZING RADIATION SO DOSE-RESPONSE LA English DT Editorial Material DE low-dose radiation; risk; hormesis; adaptive response ID LIFE-SPAN; IRRADIATION; RISK; RADON; CANCER; MODEL AB The linear no-threshold (LNT) model of ionizing-radiation-induced cancer is based on the assumption that every radiation dose increment constitutes increased cancer risk for humans. The risk is hypothesized to increase linearly as the total dose increases. While this model is the basis for radiation safety regulations, its scientific validity has been questioned and debated for many decades. The recent memorandum of the International Commission on Radiological Protection admits that the LNT-model predictions at low doses are "speculative, unproven, undetectable and 'phantom'. "Moreover, numerous experimental, ecological, and epidemiological studies show that low doses of sparsely-ionizing or sparsely-ionizing plus highly-ionizing radiation may be beneficial to human health (hormesis/adaptive response). The present LNT-model-based regulations impose excessive costs on the society. For example, the median-cost medical program is 5000 times more cost-efficient in saving lives than controlling radiation emissions. There are also lives lost: e.g., following Fukushima accident, more than 1000 disaster-related yet non-radiogenic premature deaths were officially registered among the population evacuated due to radiation concerns. Additional negative impacts of LNT-model-inspired radiophobia include: refusal of some patients to undergo potentially life-saving medical imaging; discouragement of the study of low-dose radiation therapies; motivation for radiological terrorism and promotion of nuclear proliferation. C1 [Socol, Yehoshua] Acad Forum Nucl Awareness, Karney Shomron, Israel. [Dobrzynski, Ludwik] Natl Ctr Nucl Res, Otwock, Poland. [Doss, Mohan] Fox Chase Canc Ctr, Philadelphia, PA 19111 USA. [Feinendegen, Ludwig E.] Univ Dusseldorf, Dusseldorf, Germany. [Janiak, Marek K.] Mil Inst Hyg & Epidemiol, Warsaw, Poland. [Miller, Mark L.] Sandia Natl Labs, Livermore, CA 94550 USA. [Scott, Bobby R.] Lovelace Resp Res Inst, Albuquerque, NM USA. [Ulsh, Brant] MH Chew & Associates, Livermore, CA USA. [Vaiserman, Alexander] Inst Gerontol, Kiev, Ukraine. RP Socol, Y (reprint author), Acad Forum Nucl Awareness, POB 3067 Karney Shomron, Karney Shomron, Israel. EM socol@FalconAnalytics.com NR 39 TC 3 Z9 3 U1 2 U2 10 PU INT DOSE-RESPONSE SOC PI AMHERST PA UNIV MASSACHUSETTS SPH, MORRILL SCI CTR 1, N344, 639 N PLEASANT ST, AMHERST, MA 01003-9298 USA SN 1559-3258 J9 DOSE-RESPONSE JI Dose-Response PY 2014 VL 12 IS 2 BP 342 EP 348 DI 10.2203/dose-response.13-044.Socol PG 7 WC Pharmacology & Pharmacy; Radiology, Nuclear Medicine & Medical Imaging; Toxicology SC Pharmacology & Pharmacy; Radiology, Nuclear Medicine & Medical Imaging; Toxicology GA AH9RG UT WOS:000336478900009 PM 24910586 ER PT J AU Marcus, MA Lam, PJ AF Marcus, Matthew A. Lam, Phoebe J. TI Visualising Fe speciation diversity in ocean particulate samples by micro X-ray absorption near-edge spectroscopy SO ENVIRONMENTAL CHEMISTRY LA English DT Article ID NONLINEAR DIMENSIONALITY REDUCTION; NORTH PACIFIC; IRON; AVAILABILITY AB It is a well known truism that natural materials are inhomogeneous, so analysing them on a point-by-point basis can generate a large volume of data, from which it becomes challenging to extract understanding. In this paper, we show an example in which particles taken from the ocean in two different regions (the Western Subarctic Pacific and the Australian sector of the Southern Ocean, south of Tasmania) are studied by Fe K-edge micro X-ray absorption near-edge spectroscopy (mXANES). The resulting set of data consists of 209 spectra from the Western Subarctic Pacific and 126 from the Southern Ocean. We show the use of principal components analysis with an interactive projection visualisation tool to reduce the complexity of the data to something manageable. The Western Subarctic Pacific particles were grouped into four main populations, each of which was characterised by spectra consistent with mixtures of 1-3 minerals: (1) Fe3+ oxyhydroxides+Fe3+ clays+Fe2+ phyllosilicates, (2) Fe3+ clays, (3) mixed-valence phyllosilicates and (4) magnetite+Fe3+ clays+Fe2+ silicates, listed in order of abundance. The Southern Ocean particles break into three clusters: (1) Fe3+-bearing clays+Fe3+ oxyhydroxides, (2) Fe2+ silicates+Fe(3+)Z oxyhydroxides and (3) Fe3+ oxides+Fe3+-bearing clays+Fe2+ silicates, in abundance order. Although there was some overlap between the two regions, this analysis shows that the particulate Fe mineral assemblage is distinct between the Western Subarctic Pacific and the Southern Ocean, with potential implications for the bioavailability of particulate Fe in these two iron-limited regions. We then discuss possible advances in the methods, including automatic methods for characterising the structure of the data. C1 [Marcus, Matthew A.] Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. [Lam, Phoebe J.] Woods Hole Oceanog Inst, Dept Marine Chem & Geochem, Woods Hole, MA 02543 USA. RP Marcus, MA (reprint author), Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. EM mamarcus@lbl.gov FU Office of Science, Office of Basic Energy Sciences, US Department of Energy [DE-AC02-05CH11231]; Australian Government Cooperative Research Centres Programme; WHOI Independent Study Award FX The operations of the Advanced Light Source at Lawrence Berkeley National Laboratory are supported by the Director, Office of Science, Office of Basic Energy Sciences, US Department of Energy under contract number DE-AC02-05CH11231. Collection of samples for the VERTIGO project was supported by the US National Science Foundation Program in Chemical Oceanography to Ken Buesseler and the US Department of Energy, Office of Science, Biological and Environmental Research Program to Jim Bishop. The SAZ-SENSE project was supported by the Australian Government Cooperative Research Centres Programme. Collection of spectroscopic data by PJL was supported through the WHOI Postdoctoral Scholar Program, WHOI Independent Study Award and NSF Chemical Oceanography. Thanks to S. Fakra, S. Bone and D. Ohnemus for assistance at the beamline. The authors thank Thomas Borch, Jakob Frommer and Andreas Voegelin for the use of several of their Fe reference spectra, as well as those sources acknowledged in Marcus et al.[18] NR 27 TC 6 Z9 6 U1 3 U2 13 PU CSIRO PUBLISHING PI CLAYTON PA UNIPARK, BLDG 1, LEVEL 1, 195 WELLINGTON RD, LOCKED BAG 10, CLAYTON, VIC 3168, AUSTRALIA SN 1448-2517 EI 1449-8979 J9 ENVIRON CHEM JI Environ. Chem. PY 2014 VL 11 IS 1 BP 10 EP 17 DI 10.1071/EN13075 PG 8 WC Chemistry, Analytical; Environmental Sciences SC Chemistry; Environmental Sciences & Ecology GA AI0FN UT WOS:000336521700003 ER PT S AU Efimov, A Velizhanin, K Gelikonov, G AF Efimov, Anatoly Velizhanin, Kirill Gelikonov, Grigory BE Hemmati, H Boroson, DM TI Simultaneous scintillation measurements of coherent and partially coherent beams in an open atmosphere experiment SO FREE-SPACE LASER COMMUNICATION AND ATMOSPHERIC PROPAGATION XXVI SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Free-Space Laser Communication and Atmospheric Propagation XXVI CY FEB 02-04, 2014 CL San Francisco, CA SP SPIE DE Scintillations; Atmospheric turbulence; Free-Space Optical Communication; Partially coherent beam; Multimode fiber ID REDUCTION AB Scintillation indices, probability distribution functions and signal spectra are measured simultaneously for spatially coherent and partially coherent optical beams propagating through various distances in an open atmosphere. The partially coherent beam is produced by coupling the broadband output of a superluminescent diode to a multimode optical fiber. A simple system to adjust the coherence radius by controlling the numerical aperture at the fiber output is implemented. Substantial reduction of the scintillation index and signal fade probability as compared to a slightly diverging coherent Gaussian beam are observed at all propagation distances studied up to 6.5 km. C1 [Efimov, Anatoly; Velizhanin, Kirill] Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. [Gelikonov, Grigory] RAS, Inst Appl Phys, Novgorod 603950, Russia. RP Efimov, A (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM efimov@lanl.gov RI Velizhanin, Kirill/C-4835-2008; OI Efimov, Anatoly/0000-0002-5559-4147 FU National Nuclear Security Administration of the U. S. Department of Energy [DE- AC52- 06NA25396] FX This work was performed, in part, at the Center for Integrated Nanotechnologies, a U. S. Department of Energy, Office of Basic Energy Sciences user facility. 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 13 TC 3 Z9 3 U1 0 U2 5 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9884-7 J9 PROC SPIE PY 2014 VL 8971 AR UNSP 897105 DI 10.1117/12.2037416 PG 8 WC Engineering, Electrical & Electronic; Optics; Physics, Applied SC Engineering; Optics; Physics GA BA4QB UT WOS:000336122300004 ER PT S AU Davis, RW Wu, HW Singh, S AF Davis, Ryan W. Wu, Hauwen Singh, Seema BE Farkas, DL Nicolau, DV Leif, RC TI Multispectral sorter for rapid, nondestructive optical bioprospecting for algae biofuels SO IMAGING, MANIPULATION, AND ANALYSIS OF BIOMOLECULES, CELLS, AND TISSUES XII SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Imaging, Manipulation, and Analysis of Biomolecules, Cells, and Tissues XII CY FEB 03-06, 2014 CL San Francisco, CA SP SPIE DE cell sorting; laser trap; micro-Raman; PAM fluorometry; algae biofuels ID DUNALIELLA-SALINA; TEMPERATURE; BIODIESEL; STATE AB Microalgal biotechnology is a nascent yet burgeoning field for developing the next generation of sustainable feeds, fuels, and specialty chemicals. Among the issues facing the algae bioproducts industry, the lack of efficient means of cultivar screening and phenotype selection represents a critical hurdle for rapid development and diversification. To address this challenge, we have developed a multi-modal and label-free optical tool which simultaneously assesses the photosynthetic productivity and biochemical composition of single microalgal cells, and provides a means for actively sorting attractive specimen (bioprospecting) based on the spectral readout. The device integrates laser-trapping micro-Raman spectroscopy and pulse amplitude modulated (PAM) fluorometry of microalgal cells in a flow cell. Specifically, the instrument employs a dual-purpose epi-configured IR laser for single-cell trapping and Raman spectroscopy, and a high-intensity VIS-NIR trans-illumination LED bank for detection of variable photosystem II (PSII) fluorescence. Micro-Raman scatter of single algae cells revealed vibrational modes corresponding to the speciation and total lipid content, as well as other major biochemical pools, including total protein, carbohydrates, and carotenoids. PSII fluorescence dynamics provide a quantitative estimate of maximum photosynthetic efficiency and regulated and non-regulated non-photochemical quenching processes. The combined spectroscopic readouts provide a set of metrics for subsequent optical sorting of the cells by the laser trap for desirable biomass properties, e. g. the combination of high lipid productivity and high photosynthetic yield. Thus the device provides means for rapid evaluation and sorting of algae cultures and environmental samples for biofuels development. C1 [Davis, Ryan W.] Sandia Natl Labs, Livermore, CA 94550 USA. Joint BioEnergy Inst, Emeryville, CA USA. RP Davis, RW (reprint author), Sandia Natl Labs, Livermore, CA 94550 USA. NR 22 TC 1 Z9 1 U1 6 U2 15 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9860-1 J9 PROC SPIE PY 2014 VL 8947 AR UNSP 89471E DI 10.1117/12.2040538 PG 11 WC Cell & Tissue Engineering; Optics; Radiology, Nuclear Medicine & Medical Imaging SC Cell Biology; Optics; Radiology, Nuclear Medicine & Medical Imaging GA BA4NO UT WOS:000336037200030 ER PT S AU Zhang, PF Goodwin, PM Werner, JH AF Zhang, Pengfei Goodwin, Peter M. Werner, James H. BE Farkas, DL Nicolau, DV Leif, RC TI Fast, 3D imaging via confocal line scanning of a Bessel beam using a single galvo mirror SO IMAGING, MANIPULATION, AND ANALYSIS OF BIOMOLECULES, CELLS, AND TISSUES XII SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Imaging, Manipulation, and Analysis of Biomolecules, Cells, and Tissues XII CY FEB 03-06, 2014 CL San Francisco, CA SP SPIE DE light-sheet microscopy; line scanning; Bessel beam; confocal microscopy ID LIGHT-SHEET MICROSCOPY; FLUORESCENCE MICROSCOPY; MOLECULE LOCALIZATION; PLANE ILLUMINATION; THICK MEDIA; EXCITATION; CELLS AB We developed a light-sheet illumination microscope that can perform fast 3D imaging of transparent biological samples. The light-sheet is created by raster scanning of a Bessel Beam with one galvo-mirror. Fluorescence excited from the thin layer of the sample is de-scanned by the same galvo-mirror, and then spatially filtered by a slit so that out-of-focus fluorescence generated by the side lobes of the Bessel beam is rejected. The spatially filtered fluorescence is returned by a series of optics and is re-scanned by the same galvo-mirror across the chip of a camera such that the fluorescence image is constructed in real-time. Compared to two-photon Bessel beam excitation or other confocal line scanning approaches, our method is of lower cost, simpler, and doesn't require calibration and synchronization of multiple galvo mirrors. We demonstrated the capability of fast 3D imaging and background rejection capabilities of this microscope with fluorescent beads embedded in PDMS. C1 [Zhang, Pengfei; Goodwin, Peter M.; Werner, James H.] Los Alamos Natl Lab, Ctr Integrated Nanotechnol, Los Alamos, NM 87545 USA. RP Zhang, PF (reprint author), Los Alamos Natl Lab, Ctr Integrated Nanotechnol, POB 1663, Los Alamos, NM 87545 USA. NR 20 TC 2 Z9 2 U1 1 U2 7 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9860-1 J9 PROC SPIE PY 2014 VL 8947 AR 89471K DI 10.1117/12.2036848 PG 8 WC Cell & Tissue Engineering; Optics; Radiology, Nuclear Medicine & Medical Imaging SC Cell Biology; Optics; Radiology, Nuclear Medicine & Medical Imaging GA BA4NO UT WOS:000336037200035 ER PT J AU Feng, CC Sorokine, A AF Feng, Chen-Chieh Sorokine, Alexandre TI Comparing English, Mandarin, and Russian hydrographic and terrain categories SO INTERNATIONAL JOURNAL OF GEOGRAPHICAL INFORMATION SCIENCE LA English DT Article DE cross-linguistic comparison; landscape category; data standard; interoperability; ontology ID SEMANTIC SIMILARITY; ONTOLOGIES; LANDSCAPE; LANGUAGE; TERMS AB The paper compares hydrographic and terrain categories in the geospatial data standards of the United States, Taiwan, and Russian Federation where the dominant languages used are from different language families. It aims to identify structural and semantic differences between similar categories across three geospatial data standards. By formalizing the data standard structures and identifying the properties that differentiate sibling categories in each geospatial data standard using well-known formal relations and quality universals, we develop a common basis on which hydrographic and terrain categories in the three data standards can be compared. The result suggests that all the three data standards structure categories with a mixture of relations even though most of them are well-known relations in top-level ontologies. Similar categories can be found across all the three standards. Cases of categories from different standards carrying identical meaning are rare. Partial overlaps in the meaning of the similar categories can be a direct result of different quality universals at work in defining and distinguishing these categories, or in the case of these categories being ordered by size, the threshold values for distinguishing the categories are ambiguous and language-dependent. Understanding these differences avoids incorrect mappings of categories in multilingual applications. More importantly, it provides a starting point for more effective mapping between hydrographic and terrain categories between English, Mandarin, and Russian. C1 [Feng, Chen-Chieh] Natl Univ Singapore, Dept Geog, Singapore 117548, Singapore. [Sorokine, Alexandre] Oak Ridge Natl Lab, Computat Sci & Engn Div, Oak Ridge, TN USA. RP Feng, CC (reprint author), Natl Univ Singapore, Dept Geog, Singapore 117548, Singapore. EM geofcc@nus.edu.sg RI Feng, Chen-Chieh/F-9993-2012 OI Feng, Chen-Chieh/0000-0003-0410-714X FU National University of Singapore Academic Research Fund [R-109-000-112-112] FX Support by the National University of Singapore Academic Research Fund [grant number R-109-000-112-112] is appreciated. NR 44 TC 0 Z9 0 U1 0 U2 4 PU TAYLOR & FRANCIS LTD PI ABINGDON PA 4 PARK SQUARE, MILTON PARK, ABINGDON OX14 4RN, OXON, ENGLAND SN 1365-8816 EI 1362-3087 J9 INT J GEOGR INF SCI JI Int. J. Geogr. Inf. Sci. PY 2014 VL 28 IS 6 SI SI BP 1294 EP 1315 DI 10.1080/13658816.2013.831420 PG 22 WC Computer Science, Information Systems; Geography; Geography, Physical; Information Science & Library Science SC Computer Science; Geography; Physical Geography; Information Science & Library Science GA AH8HX UT WOS:000336379300007 ER PT J AU Tarefder, RA Sumee, N Storlie, C AF Tarefder, Rafiqul A. Sumee, Nasrin Storlie, Curtis TI Study of MEPDG Sensitivity Using Nonparametric Regression Procedures SO JOURNAL OF COMPUTING IN CIVIL ENGINEERING LA English DT Article DE Sensitivity analysis; Statistics; Sampling; Pavements; Mechanistic-Empirical Pavement Design Guide; Sensitivity analysis; Advanced statistical analysis; Latin hypercube sampling; Nonparametric regression; Confidence intervals AB Because the new Mechanistic-Empirical Pavement Design Guide (MEPDG) includes numerous inputs, a sensitivity analysis using the Monte Carlo approach is not practical because it requires thousands of MEPDG runs. Instead, nonparametric regression procedures can be very useful to perform MEPDG sensitivity analysis. In this study, nonparametric regression procedures such as multivariate adaptive regression splines and gradient boosting machine are employed to identify inputs that contribute significantly to the outputs. Thirty inputs are used to randomly generate 750 input combinations by using Latin hypercube sampling. Using four-layer pavement geometry [two asphalt concrete (AC), base, and subgrade layers], simulations are run in MEPDG software to produce a time series of predicted distresses such as roughness, rutting, and cracking. Sensitivity analysis resulted in three groups of inputs to which the output is (1)highly sensitive, (2)moderately sensitive, and (3)minimally sensitive. Results show that roughness is highly sensitive to traffic input variables such as annual average daily truck traffic (AADTT), percentage of trucks in the design lane, and thickness of bottom AC layer. AC rutting is highly affected by AADTT, percentage of trucks in design direction, and tire pressure. Three major factors for total rutting, longitudinal cracking, and alligator cracking are AADTT, percentage of trucks in design direction, and thickness of bottom AC layer. In addition to these, alligator cracking is highly sensitive to percentage of air voids in the bottom AC layer. Transverse cracking is highly sensitive to the percentage of trucks in the design lane, percentage of Class 11 vehicles, plastic limit, thickness of base layer, effective binder content of top AC layer, and climate. Among all of the inputs, the thickness of the AC layer is highly interactive with other input variables. C1 [Tarefder, Rafiqul A.; Sumee, Nasrin] Univ New Mexico, Dept Civil Engn, Albuquerque, NM 87131 USA. [Sumee, Nasrin] N Carolina State Univ, Dept Civil Construct & Environm Engn, Raleigh, NC 27695 USA. [Storlie, Curtis] Los Alamos Natl Lab, Stat Sci Grp CCS 6, Los Alamos, NM 87545 USA. RP Tarefder, RA (reprint author), Univ New Mexico, Dept Civil Engn, MSC01 1070, Albuquerque, NM 87131 USA. EM tarefder@unm.edu; nsumee@ncsu.edu; storlie@lanl.gov FU New Mexico Department of Transportation FX The authors would like to thank the New Mexico Department of Transportation for funding this study. NR 18 TC 0 Z9 0 U1 0 U2 0 PU ASCE-AMER SOC CIVIL ENGINEERS PI RESTON PA 1801 ALEXANDER BELL DR, RESTON, VA 20191-4400 USA SN 0887-3801 EI 1943-5487 J9 J COMPUT CIVIL ENG JI J. Comput. Civil. Eng. PD JAN 1 PY 2014 VL 28 IS 1 BP 134 EP 144 DI 10.1061/(ASCE)CP.1943-5487.0000239 PG 11 WC Computer Science, Interdisciplinary Applications; Engineering, Civil SC Computer Science; Engineering GA AD7LT UT WOS:000333446100014 ER PT J AU Hoffman, MJ Fountain, AG Liston, GE AF Hoffman, Matthew J. Fountain, Andrew G. Liston, Glen E. TI Near-surface internal melting: a substantial mass loss on Antarctic Dry Valley glaciers SO JOURNAL OF GLACIOLOGY LA English DT Article DE Antarctic glaciology; energy balance; glacier ablation phenomena; ice/atmosphere interactions; surface melt ID GREENLAND ICE-SHEET; AERODYNAMIC ROUGHNESS LENGTH; ENERGY-BALANCE; TAYLOR VALLEY; SEA ICE; OPTICAL-PROPERTIES; SPATIAL VARIATIONS; ABLATION ZONE; BLUE ICE; SNOW AB The McMurdo Dry Valleys, southern Victoria Land, East Antarctica, are a polar desert, and melt from glacial ice is the primary source of water to streams, lakes and associated ecosystems. Previous work found that to adequately model glacier ablation and subsurface ice temperatures with a surface energy-balance model required including the transmission of solar radiation into the ice. Here we investigate the contribution of subsurface melt to the mass balance of (and runoff from) Dry Valley glaciers by including a drainage process in the model and applying the model to three glacier sites using 13 years of hourly meteorological data. Model results for the smooth glacier surfaces common to many glaciers in the Dry Valleys showed that sublimation was typically the largest component of surface lowering, with rare episodes of surface melting, consistent with anecdotal field observations. Results also showed extensive internal melting 5-15 cm below the ice surface, the drainage of which accounted for similar to 50% of summer ablation. This is consistent with field observations of subsurface streams and formation of a weathering crust. We identify an annual cycle of weathering crust formation in summer and its removal during the 10 months of winter sublimation. C1 [Hoffman, Matthew J.] Los Alamos Natl Lab, Fluid Dynam & Solid Mech Grp, Los Alamos, NM 87545 USA. [Fountain, Andrew G.] Portland State Univ, Dept Geol, Portland, OR 97207 USA. [Liston, Glen E.] Colorado State Univ, Cooperat Inst Res Atmosphere, Ft Collins, CO 80523 USA. RP Hoffman, MJ (reprint author), Los Alamos Natl Lab, Fluid Dynam & Solid Mech Grp, Los Alamos, NM 87545 USA. EM mhoffman@lanl.gov FU US National Science Foundation (NSF) Office of Polar Programs [ANT-0423595, ANT-0233823]; Earth System Modeling program of the Office of Biological and Environmental Research within the US Department of Energy's Office of Science; NSF grant [ANT-0424589] FX This work was funded by US National Science Foundation (NSF) Office of Polar Programs grants ANT-0423595 and ANT-0233823, the Earth System Modeling program of the Office of Biological and Environmental Research within the US Department of Energy's Office of Science, and by NSF grant No. ANT-0424589 to the Center for Remote Sensing of Ice Sheets (CReSIS). We thank Hassan Basagic, Thomas Nylen and Liz Bagshaw for assistance in the field. NR 67 TC 6 Z9 6 U1 2 U2 18 PU INT GLACIOL SOC PI CAMBRIDGE PA LENSFIELD RD, CAMBRIDGE CB2 1ER, ENGLAND SN 0022-1430 EI 1727-5652 J9 J GLACIOL JI J. Glaciol. PY 2014 VL 60 IS 220 BP 361 EP 374 DI 10.3189/2014JoG13J095 PG 14 WC Geography, Physical; Geosciences, Multidisciplinary SC Physical Geography; Geology GA AH5VB UT WOS:000336198100016 ER PT J AU Ma, L Chen, W Schatte, G Wang, W Joly, AG Huang, YN Sammynaiken, R Hossu, M AF Ma, Lun Chen, Wei Schatte, Gabriele Wang, Wei Joly, Alan G. Huang, Yining Sammynaiken, Ramaswami Hossu, Marius TI A new Cu-cysteamine complex: structure and optical properties SO JOURNAL OF MATERIALS CHEMISTRY C LA English DT Article ID MULTIPLE-STATE EMISSION; METAL-COMPLEX; SOLID-STATE; LUMINESCENCE; LIGAND; PHOTOLUMINESCENCE; COPPER(II); CYSTAMINE; MN2+ AB Here we report the structure and optical properties of a new Cu-cysteamine complex (Cu-Cy) with a formula of Cu3Cl(SR)(2) (R = CH2CH2NH2). This Cu-Cy has a different structure from a previous Cu-Cy complex, in which both thio and amine groups from cysteamine bond with copper ions. Single-crystal X-ray diffraction and solid-state nuclear magnetic resonance results show that the oxidation state of copper in Cu3Cl(SR)(2) is +1 rather than +2. Further, Cu3Cl(SR)(2) has been observed to show intense photoluminescence and X-ray excited luminescence. More interesting is that Cu3Cl(SR)(2) particles can produce singlet oxygen under irradiation by light or X-ray. This indicates that Cu3Cl(SR)(2) is a new photosensitizer that can be used for deep cancer treatment as X-ray can penetrate soft tissues. All these findings mean that Cu3Cl(SR)(2) is a new material with potential applications for lighting, radiation detection and cancer treatment. C1 [Ma, Lun; Chen, Wei; Hossu, Marius] Univ Texas Arlington, Dept Phys, Arlington, TX 76019 USA. [Ma, Lun; Chen, Wei; Hossu, Marius] Univ Texas Arlington, SAVANT Ctr, Arlington, TX 76019 USA. [Schatte, Gabriele; Sammynaiken, Ramaswami] Univ Saskatchewan, Saskatchewan Struct Sci Ctr, Saskatoon, SK S7N 5C9, Canada. [Wang, Wei; Huang, Yining] Univ Western Ontario, Dept Chem, London, ON N6A 3K7, Canada. [Joly, Alan G.] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Chen, W (reprint author), Univ Texas Arlington, Dept Phys, POB 19059, Arlington, TX 76019 USA. EM weichen@uta.edu OI 王, 伟/0000-0003-2864-5102 FU U.S. Army Medical Research Acquisition Activity (USAMRAA) [W81XWH-10-1-0279, W81XWH-10-1-0234]; NSF; DHS joint ARI program [2011-DN-077-ARI053-02, 2011-DN-077-ARI053-03, 2011-DN-077-ARI053-04] FX We would like to acknowledge the support from the U.S. Army Medical Research Acquisition Activity (USAMRAA) under Contracts of W81XWH-10-1-0279 and W81XWH-10-1-0234 and partially the NSF and DHS joint ARI program (2011-DN-077-ARI053-02, 3&4). NR 40 TC 6 Z9 7 U1 7 U2 28 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 2014 VL 2 IS 21 BP 4239 EP 4246 DI 10.1039/c4tc00114a PG 8 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA AH3PZ UT WOS:000336038400019 ER PT S AU Bender, DA DeRose, CT Starbuck, A Verley, JC Jenkins, MW AF Bender, Daniel A. DeRose, Christopher T. Starbuck, Andrew Verley, Jason C. Jenkins, Mark W. BE Nakata, Y Xu, X Roth, S Neuenschwander, B TI Precision Laser Annealing of Silicon devices for Enhanced Electro-Optic Performance SO LASER APPLICATIONS IN MICROELECTRONIC AND OPTOELECTRONIC MANUFACTURING (LAMOM) XIX SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Laser Applications in Microelectronic and Optoelectronic Manufacturing (LAMOM) XIX CY FEB 03-06, 2014 CL San Francisco, CA SP SPIE, Okamoto Opt AB We present results from laser annealing experiments in Si using a passively Q-switched Nd:YAG microlaser. Exposure with laser at fluence values above the damage threshold of commercially available photodiodes results in electrical damage (as measured by an increase in photodiode dark current). We show that increasing the laser fluence to values in excess of the damage threshold can result in annealing of a damage site and a reduction in detector dark current by as much as 100x in some cases. A still further increase in fluence results in irreparable damage. Thus we demonstrate the presence of a laser annealing window over which performance of damaged detectors can be at least partially reconstituted. Moreover dark current reduction is observed over the entire operating range of the diode indicating that device performance has been improved for all values of reverse bias voltage. Additionally, we will present results of laser annealing in Si waveguides. By exposing a small (<10 um) length of a Si waveguide to an annealing laser pulse, the longitudinal phase of light acquired in propagating through the waveguide can be modified with high precision, <15 milliradian per laser pulse. Phase tuning by 180 degrees is exhibited with multiple exposures to one arm of a Mach-Zehnder interferometer at fluence values below the morphological damage threshold of an etched Si waveguide. No reduction in optical transmission at 1550 nm was found after 220 annealing laser shots. C1 [Bender, Daniel A.; DeRose, Christopher T.; Starbuck, Andrew; Verley, Jason C.; Jenkins, Mark W.] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Bender, DA (reprint author), Sandia Natl Labs, POB 5800, Albuquerque, NM 87185 USA. NR 3 TC 0 Z9 0 U1 0 U2 1 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9880-9 J9 PROC SPIE PY 2014 VL 8967 AR 89670S DI 10.1117/12.2037339 PG 9 WC Engineering, Electrical & Electronic; Optics; Physics, Applied SC Engineering; Optics; Physics GA BA4PE UT WOS:000336082300020 ER PT J AU D'Angelo, S Glanville, J Ferrara, F Naranjo, L Gleasner, CD Shen, XH Bradbury, ARM Kiss, C AF D'Angelo, Sara Glanville, Jacob Ferrara, Fortunato Naranjo, Leslie Gleasner, Cheryl D. Shen, Xiaohong Bradbury, Andrew R. M. Kiss, Csaba TI The antibody mining toolbox An open source tool for the rapid analysis of antibody repertoires SO MABS LA English DT Article DE HCDR3; antibody library; deep sequencing; regular expression; AbMining ToolBox ID PHAGE DISPLAY; GENERATION; DIVERSITY; GENE; TECHNOLOGIES; LIBRARIES; SELECTION; AFFINITY; REGION; RECOMBINATION AB In vitro selection has been an essential tool in the development of recombinant antibodies against various antigen targets. Deep sequencing has recently been gaining ground as an alternative and valuable method to analyze such antibody selections. The analysis provides a novel and extremely detailed view of selected antibody populations, and allows the identification of specific antibodies using only sequencing data, potentially eliminating the need for expensive and laborious low-throughput screening methods such as enzyme-linked immunosorbant assay. The high cost and the need for bioinformatics experts and powerful computer clusters, however, have limited the general use of deep sequencing in antibody selections. Here, we describe the AbMining ToolBox, an open source software package for the straightforward analysis of antibody libraries sequenced by the three main next generation sequencing platforms (454, Ion Torrent, MiSeq). The ToolBox is able to identify heavy chain CDR3s as effectively as more computationally intense software, and can be easily adapted to analyze other portions of antibody variable genes, as well as the selection outputs of libraries based on different scaffolds. The software runs on all common operating systems (Microsoft Windows, Mac OS X, Linux), on standard personal computers, and sequence analysis of 1-2 million reads can be accomplished in 10-15 min, a fraction of the time of competing software. Use of the ToolBox will allow the average researcher to incorporate deep sequence analysis into routine selections from antibody display libraries. C1 [D'Angelo, Sara; Ferrara, Fortunato] New Mexico Consortium, Los Alamos, NM USA. [Glanville, Jacob] Stanford Univ, Stanford, CA 94305 USA. [Naranjo, Leslie; Gleasner, Cheryl D.; Shen, Xiaohong; Bradbury, Andrew R. M.; Kiss, Csaba] Los Alamos Natl Lab, Div B, Los Alamos, NM 87545 USA. RP Kiss, C (reprint author), Los Alamos Natl Lab, Div B, Los Alamos, NM 87545 USA. EM csaba.kiss@lanl.gov OI Bradbury, Andrew/0000-0002-5567-8172 FU National Institutes of Health [5U54DK093500-02]; Los Alamos National Laboratory Directed Research Development Directed Research funds [20120029DR] FX This work was supported by the National Institutes of Health [5U54DK093500-02 to ARMB]; and Los Alamos National Laboratory Directed Research Development Directed Research [20120029DR] funds. NR 40 TC 14 Z9 14 U1 1 U2 8 PU LANDES BIOSCIENCE PI AUSTIN PA 1806 RIO GRANDE ST, AUSTIN, TX 78702 USA SN 1942-0862 EI 1942-0870 J9 MABS-AUSTIN JI mAbs PD JAN-FEB PY 2014 VL 6 IS 1 BP 160 EP 172 DI 10.4161/mabs.27105 PG 13 WC Medicine, Research & Experimental SC Research & Experimental Medicine GA AH6HH UT WOS:000336230800014 PM 24423623 ER PT J AU Mayeur, JR Beyerlein, IJ Bronkhorst, CA Mourad, HM AF Mayeur, Jason R. Beyerlein, Irene J. Bronkhorst, Curt A. Mourad, Hashem M. TI The Influence of Grain Interactions on the Plastic Stability of Heterophase Interfaces SO MATERIALS LA English DT Article DE crystal plasticity; rolling texture; nanolamellar composites; interface stability; grain interactions ID ROLLING TEXTURE DEVELOPMENT; NB NANOLAMELLAR COMPOSITES; CU/NB-LAYERED COMPOSITES; HIGH-STRENGTH; NANOCOMPOSITE WIRES; BIMETAL INTERFACES; DEFORMATION; EVOLUTION; MULTILAYERS; DISLOCATION AB Two-phase bimetal composites contain both grain boundaries and bi-phase interfaces between dissimilar crystals. In this work, we use a crystal plasticity finite element framework to explore the effects of grain boundary interactions on the plastic stability of bi-phase interfaces. We show that neighboring grain interactions do not significantly alter interface plastic stability during plane strain compression. The important implications are that stable orientations at bimetal interfaces can be different than those within the bulk layers. This finding provides insight into bi-phase microstructural development and suggests a pathway for tuning interface properties via severe plastic deformation. C1 [Mayeur, Jason R.; Beyerlein, Irene J.; Bronkhorst, Curt A.; Mourad, Hashem M.] Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. RP Mayeur, JR (reprint author), Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. EM jmayeur@lanl.gov; irene@lanl.gov; cabronk@lanl.gov; hmourad@lanl.gov RI Bronkhorst, Curt/B-4280-2011 OI Bronkhorst, Curt/0000-0002-2709-1964 FU 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]; National Nuclear Security Administration of the US Department of Energy [DE-AC52-06NA25396]; Los Alamos National Laboratory Directed Research and Development (LDRD) [DR20110029]; DOE [DE AC52 06NA25396] FX Jason R. Mayeur and Irene J. Beyerlein gratefully acknowledge support by 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. 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 US Department of Energy under Contract DE-AC52-06NA25396. Curt A. Bronkhorst and Hashem M. Mourad acknowledge the support of the Los Alamos National Laboratory Directed Research and Development (LDRD) Project DR20110029. Los Alamos National Laboratory is operated by Los Alamos National Security LLC under DOE Contract DE AC52 06NA25396. NR 41 TC 10 Z9 10 U1 1 U2 13 PU MDPI AG PI BASEL PA ST ALBAN-ANLAGE 66, CH-4052 BASEL, SWITZERLAND SN 1996-1944 J9 MATERIALS JI Materials PD JAN PY 2014 VL 7 IS 1 BP 302 EP 322 DI 10.3390/ma7010302 PG 21 WC Materials Science, Multidisciplinary SC Materials Science GA AH4HR UT WOS:000336088500023 ER PT J AU Samudrala, GK Vohra, YK Walock, MJ Miles, R AF Samudrala, Gopi K. Vohra, Yogesh K. Walock, Michael J. Miles, Robin TI Rapid Growth of Nanostructured Diamond Film on Silicon and Ti-6Al-4V Alloy Substrates SO MATERIALS LA English DT Article DE MPCVD; nanostructured diamond; film growth; thin film structure and morphology ID CHEMICAL-VAPOR-DEPOSITION; GAS-PHASE; MICROWAVE PLASMA; NITROGEN; NANODIAMOND; CVD AB Nanostructured diamond (NSD) films were grown on silicon and Ti-6Al-4V alloy substrates by microwave plasma chemical vapor deposition (MPCVD). NSD Growth rates of 5 mu m/h on silicon, and 4 mu m/h on Ti-6Al-4V were achieved. In a chemistry of H-2/CH4/N-2, varying ratios of CH4/H-2 and N-2/CH4 were employed in this research and their effect on the resulting diamond films were studied by X-ray photoelectron spectroscopy, Raman spectroscopy, scanning electron microscopy, and atomic force microscopy. As a result of modifying the stock cooling stage of CVD system, we were able to utilize plasma with high power densities in our NSD growth experiments, enabling us to achieve high growth rates. Substrate temperature and N-2/CH4 ratio have been found to be key factors in determining the diamond film quality. NSD films grown as part of this study were shown to contain 85% to 90% sp(3) bonded carbon. C1 [Samudrala, Gopi K.; Vohra, Yogesh K.; Walock, Michael J.] Univ Alabama Birmingham, Dept Phys, Birmingham, AL 35294 USA. [Miles, Robin] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. RP Samudrala, GK (reprint author), Univ Alabama Birmingham, Dept Phys, Birmingham, AL 35294 USA. EM gopi@uab.edu; ykvohra@uab.edu; mwalock@uab.edu; miles7@llnl.gov RI Walock, Michael/H-5540-2013 OI Walock, Michael/0000-0002-0403-4510 FU National Science Foundation Partnerships for Innovation: Building Innovation Capacity (PFI: BIC) subprogram [IIP-1317210]; Laser Inertial Fusion Energy (LIFE) program at the Lawrence Livermore National Laboratory [DE-AC52-07NA27344] FX Our research results are based upon work supported by the National Science Foundation Partnerships for Innovation: Building Innovation Capacity (PFI: BIC) subprogram under Grant No. IIP-1317210. Any opinions, findings, and conclusions or recommendations expressed in this material are those of the author(s) and do not necessarily reflect the views of the National Science Foundation. The authors would also like to acknowledge support from the Laser Inertial Fusion Energy (LIFE) program at the Lawrence Livermore National Laboratory under Grant No. DE-AC52-07NA27344. NR 20 TC 4 Z9 4 U1 3 U2 11 PU MDPI AG PI BASEL PA POSTFACH, CH-4005 BASEL, SWITZERLAND SN 1996-1944 J9 MATERIALS JI Materials PD JAN PY 2014 VL 7 IS 1 BP 365 EP 374 DI 10.3390/ma7010365 PG 10 WC Materials Science, Multidisciplinary SC Materials Science GA AH4HR UT WOS:000336088500026 ER PT S AU Thomas, SJ Macintosh, B Belikov, R AF Thomas, Sandrine J. Macintosh, Bruce Belikov, Ruslan BE Bifano, TG Kubby, J Gigan, S TI MEMS and the direct detection of exoplanets SO MEMS ADAPTIVE OPTICS VIII SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on MEMS Adaptive Optics VIII CY FEB 02, 2014 CL San Francisco, CA SP SPIE, Samsung Adv Inst Technol DE MEMS; High-Contrast imaging; Extreme Adaptive Optics; Extrasolar planets ID EXTREME ADAPTIVE OPTICS; DEFORMABLE MIRROR; CORONAGRAPH; APERTURES; STAR AB Deformable mirrors, and particularly MEMS, are crucial components for the direct imaging of exoplanets for both ground-based and space-based instruments. Without deformable mirrors, coronagraphs are incapable of reaching contrasts required to image Jupiter-like planets. The system performance is limited by image quality degradation resulting from wavefront error introduced from multiple effects including: atmospheric turbulence, static aberrations in the system, non-common-path aberrations, all of which vary with time. Correcting for these effects requires a deformable mirror with fast response and numerous actuators having moderate stroke. Not only do MEMS devices fulfill this requirement but their compactness permits their application in numerous space- and ground-based instruments, which are often volume- and mass-limited. In this paper, I will briefly explain how coronagraphs work and their requirements. I then will discuss the Extreme Adaptive Optics needed to compensate for the introduced wavefront error and how MEMS devices are a good choice to achieve the performance needed to produce the contrasts necessary to detect exoplanets. As examples, I will discuss a facility instrument for the Gemini Observatory, called the Gemini Planet Imager, that will detect Jupiter-like planets and present recent results from the NASA Ames Coronagraph Experiment laboratory, in the context of a proposed space-based mission called EXCEDE. EXCEDE is planned to focus on protoplanetary disks. C1 [Thomas, Sandrine J.] UARC NASA Ames Res Ctr, Moffett Field, CA 94035 USA. [Macintosh, Bruce] LLNL, Livermore, CA USA. [Belikov, Ruslan] NASA, Ames Res Ctr, Moffett Field, CA USA. RP Thomas, SJ (reprint author), UARC NASA Ames Res Ctr, Moffett Field, CA 94035 USA. EM sandrie.thomas77@nasa.gov FU National Aeronautics and Space Administration under Prime [NAS2-03144]; University of California, Santa Cruz; University Affiliated Research Center; National Aeronautics and Space Administration's Ames Research Center; NASA; Technology Development for Exoplanet Missions (TDEM) [NNH10ZDA001N-SAT]; NASA's Science Mission Directorate; NASA Ames Research Center FX The material is based upon work supported by the National Aeronautics and Space Administration under Prime Contract Number NAS2-03144 awarded to the University of California, Santa Cruz, University Affiliated Research Center. This work was supported in part by the National Aeronautics and Space Administration's Ames Research Center, as well as the NASA Explorer program and the Technology Development for Exoplanet Missions (TDEM) program through solicitation NNH10ZDA001N-SAT at NASA's Science Mission Directorate. It was carried out at the NASA Ames Research Center. Any opinions, findings, and conclusions or recommendations expressed in this article are those of the authors and do not necessarily reflect the views of the National Aeronautics and Space Administration. We also acknowledge all the GPI team members and ACE/EXCEDE team members. NR 33 TC 0 Z9 0 U1 0 U2 0 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9891-5 J9 PROC SPIE PY 2014 VL 8978 AR UNSP 897806 DI 10.1117/12.2044134 PG 15 WC Engineering, Electrical & Electronic; Optics SC Engineering; Optics GA BA4PD UT WOS:000336081700005 ER PT S AU Wilcox, CC Santiago, F Jungwirth, ME Martinez, T Restaino, SR Bagwell, B Romeo, R AF Wilcox, Christopher C. Santiago, Freddie Jungwirth, Matthew E. Martinez, Ty Restaino, Sergio R. Bagwell, Brett Romeo, Robert BE Bifano, TG Kubby, J Gigan, S TI First light with a carbon fiber reinforced polymer 0.4 meter telescope SO MEMS ADAPTIVE OPTICS VIII SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on MEMS Adaptive Optics VIII CY FEB 02, 2014 CL San Francisco, CA SP SPIE, Samsung Adv Inst Technol AB For the passed several years, the Naval Research Laboratory (NRL) has been investigating the use of Carbon Fiber Reinforced Polymer (CFRP) material in the construction of a telescope assembly including the optical components. The NRL, Sandia National Laboratories (SNL), and Composite Mirror Applications, Inc. (CMA) have jointly assembled a prototype telescope and achieved "first light" images with a CFRP 0.4 m aperture telescope. CFRP offers several advantages over traditional materials such as creating structures that are lightweight and low coefficient of thermal expansion and conductivity. The telescope's primary and secondary mirrors are not made from glass, but CFRP, as well. The entire telescope weighs approximately 10 kg while a typical telescope of this size would weigh quite a bit more. We present the achievement of "first light" with this telescope demonstrating the imaging capabilities of this prototype and the optical surface quality of the mirrors with images taken during a day's quiescent periods. C1 [Wilcox, Christopher C.; Martinez, Ty; Restaino, Sergio R.] US Naval Res Lab, 4555 Overlook Ave SW, Washington, DC 20375 USA. [Santiago, Freddie; Jungwirth, Matthew E.; Bagwell, Brett] Sandia Natl Labs, Albuquerque, NM 87123 USA. [Romeo, Robert] Composite Mirror Applicat Inc, Tucson, AZ 85710 USA. RP Wilcox, CC (reprint author), US Naval Res Lab, 4555 Overlook Ave SW, Washington, DC 20375 USA. EM chris.wilcox@nrl.navy.mil NR 5 TC 0 Z9 0 U1 0 U2 5 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9891-5 J9 PROC SPIE PY 2014 VL 8978 AR UNSP 897805 DI 10.1117/12.2042105 PG 8 WC Engineering, Electrical & Electronic; Optics SC Engineering; Optics GA BA4PD UT WOS:000336081700004 ER PT S AU Ai, Y Marrone, BL AF Ai, Ye Marrone, Babetta L. BE Gray, BL Becker, H TI Separation of Biological Cells in a Microfluidic Device Using Surface Acoustic Waves (SAWs) SO MICROFLUIDICS, BIOMEMS, AND MEDICAL MICROSYSTEMS XII SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Microfluidics, BioMEMS, and Medical Microsystems XII CY FEB 02-04, 2014 CL San Francisco, CA SP SPIE, Samsung Adv Inst Technol, Microfluid ChipShop GmbH, Univ Cincinnati, Ohio Ctr Microfluid Innovat DE Microfluidics; Lab on a Chip; Surface Acoustic Wave (SAW); Cell Separation ID PARTICLES; CAPTURE AB In this study, a surface acoustic wave (SAW)-based microfluidic device has been developed to separate heterogeneous particle or cell mixtures in a continuous flow using acoustophoresis. The microfluidic device is comprised of two components, a SAW transducer and a microfluidic channel made of polydimethylsiloxane (PDMS). The SAW transducer was fabricated by patterning two pairs of interdigital electrodes on a lithium niobate (LiNbO3) piezoelectric substrate. When exciting the SAW transducer by AC signals, a standing SAW is generated along the cross-section of the channel. Solid particles immersed in the standing SAW field are accordingly pushed to the pressure node arising from the acoustic radiation force acting on the particles, referring to the acoustic particle-focusing phenomenon. Acoustic radiation force highly depends on the particle properties, resulting in different acoustic responses for different types of cells. A numerical model, coupling the piezoelectric effect in the solid substrate and acoustic pressure in the fluid, was developed to provide a better understanding of SAW-based particle manipulation. Separation of two types of fluorescent particles has been demonstrated using the developed SAW-based microfluidic device. An efficient separation of E. coli bacteria from peripheral blood mononuclear cell (PBMC) samples has also been successfully achieved. The purity of separated E. coli bacteria and separated PBMCs were over 95% and 91%, respectively, obtained by a flow cytometric analysis. The developed microfluidic device can efficiently separate E. coli bacteria from biological samples, which has potential applications in biomedical analysis and clinical diagnosis. C1 [Ai, Ye] Singapore Univ Technol & Design, Singapore, Singapore. [Marrone, Babetta L.] Los Alamos Natl Lab, Biosci Div, Los Alamos, NM 87545 USA. RP Ai, Y (reprint author), Singapore Univ Technol & Design, Singapore, Singapore. EM aiye@sutd.edu.sg RI Ai, Ye/F-3411-2011 OI Ai, Ye/0000-0001-8638-1649 FU National Center for Research Resources; National Institute of General Medical Sciences of the National Institutes of Health [P41 RR01315]; National Flow Cytometry Resource (BLM); Laboratory Directed Research and Development [20130239ER]; Los Alamos National Laboratory (BLM); SUTD- MIT International Design Center [IDG11300101] FX This work was supported, in part, by the National Center for Research Resources and the National Institute of General Medical Sciences of the National Institutes of Health (P41 RR01315) through the National Flow Cytometry Resource (BLM), the Laboratory Directed Research and Development award (20130239ER) from Los Alamos National Laboratory (BLM), and SUTD- MIT International Design Center IDG11300101 (YA). NR 18 TC 0 Z9 0 U1 3 U2 35 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9889-2 J9 PROC SPIE PY 2014 VL 8976 AR UNSP 89760O DI 10.1117/12.2035952 PG 7 WC Engineering, Biomedical; Optics SC Engineering; Optics GA BA4NJ UT WOS:000336033500016 ER PT S AU Xie, JQ Demarteau, M Wagner, R Ruiz-Oses, M Liang, X Ben-Zvi, I Attenkofer, K Schubert, S Smedley, J Wong, J Padmore, H Woll, A AF Xie, Junqi Demarteau, Marcel Wagner, Robert Ruiz-Oses, Miguel Liang, Xue Ben-Zvi, Ilan Attenkofer, Klaus Schubert, Susanne Smedley, John Wong, Jared Padmore, Howard Woll, Arthur BE Digonnet, MJF Jiang, S TI Study of Bi-alkali Photocathode Growth on Glass by X-ray Techniques for Fast Timing Response Photomultipliers SO OPTICAL COMPONENTS AND MATERIALS XI SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Optical Components and Materials XI CY FEB 03-05, 2014 CL San Francisco, CA SP SPIE DE Photomultipliers; Photocathode; Alkali Antimonide; X-ray diffraction; X-ray reflectivity AB Bi-alkali antimonide photocathode is an essential component in fast timing response photomultipliers. Real-time in-situ grazing incidence x-ray diffraction and post-growth x-ray reflectivity measurement were performed to study the photocathode deposition process on glass substrate. Grazing incidence x-ray diffraction patterns show the formation of Sb crystalline, dissolution of crystalline phase Sb by the application of K vapor and reformation of refined crystal textures. XRR result exhibits that the film thickness increases similar to 4.5 times after K diffusion and almost have no change after Cs diffusion. Further investigation is expected to understand the photocathode growth process and provide guidelines for photocathode development. C1 [Xie, Junqi; Demarteau, Marcel; Wagner, Robert] Argonne Natl Lab, 9700 S Cass Ave, Lemont, IL 60439 USA. [Ruiz-Oses, Miguel; Liang, Xue; Ben-Zvi, Ilan] SUNY Stony Brook, Stony Brook, NY 11794 USA. [Attenkofer, Klaus; Schubert, Susanne; Smedley, John] Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Wong, Jared; Padmore, Howard] Helmholtz Zentrum, D-12489 Berlin, Germany. [Woll, Arthur] Cornell Univ, Cornell High Energy Synchrotron Source, Ithaca, NY 14850 USA. RP Xie, JQ (reprint author), Argonne Natl Lab, 9700 S Cass Ave, Lemont, IL 60439 USA. EM jxie@anl.gov FU Director, Office of Science, Office of Basic Energy Sciences; U. S. Department of Energy [DE-AC02-05CH11231, DE-AC02-98CH10886, KC0407-ALSJNT-I0013, DESC0005713]; U. S. Department of Energy; Office of Science; Office of Basic Energy Sciences; Office of High Energy Physics [DE-AC02-06CH11357]; NSF [DMR-0936384] FX This work was 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, DE-AC02-98CH10886, KC0407-ALSJNT-I0013 and DESC0005713. Work at Argonne National Laboratory was supported by the U. S. Department of Energy, Office of Science, Office of Basic Energy Sciences and Office of High Energy Physics under contract DE-AC02-06CH11357. Use of CHESS is supported by NSF award DMR-0936384. NR 12 TC 0 Z9 0 U1 0 U2 2 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9895-3 J9 PROC SPIE PY 2014 VL 8982 AR UNSP 89821O DI 10.1117/12.2037367 PG 6 WC Materials Science, Multidisciplinary; Optics; Physics, Applied SC Materials Science; Optics; Physics GA BA4NN UT WOS:000336036800048 ER PT S AU Peters, DW Davids, PS Kim, JK Leonhardt, D Beechem, TE Howell, SW Ohta, T Wendt, JR Montoya, JA AF Peters, David W. Davids, Paul S. Kim, Jin K. Leonhardt, Darin Beechem, Thomas E., III Howell, Stephen W. Ohta, Taisuke Wendt, Joel R. Montoya, John A. BE Adibi, A Lin, SY Scherer, A TI Application of plasmonic subwavelength structuring to enhance infrared detection SO PHOTONIC AND PHONONIC PROPERTIES OF ENGINEERED NANOSTRUCTURES IV SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Photonic and Phononic Properties of Engineered Nanostructures IV CY FEB 03-06, 2014 CL San Francisco, CA SP SPIE DE nanoantenna; infrared; detector; metasurface; metamaterial AB Nanoantennas are an enabling technology for visible to terahertz components and may be used with a variety of detector materials. We have integrated subwavelength patterned metal nanoantennas with various detector materials for infrared detection: midwave infrared indium gallium arsenide antimonide detectors, longwave infrared graphene detectors, and shortwave infrared germanium detectors. Nanoantennas offer a means to make infrared detectors much thinner, thus lowering the dark current and improving performance. The nanoantenna converts incoming plane waves to more tightly bound and concentrated surface waves. The active material only needs to extend as far as these bound fields. In the case of graphene detectors, which are only one or two atomic layers thick, such field concentration is a necessity for usable device performance, as single pass absorption is insufficient. The nanoantenna is thus the enabling component of these thin devices. However nanoantenna integration and fabrication vary considerably across these platforms as do the considerations taken into account during design. Here we discuss the motivation for these devices and show examples for the three material systems. Characterization results are included for the midwave infrared detector. C1 [Peters, David W.; Davids, Paul S.; Kim, Jin K.; Leonhardt, Darin; Beechem, Thomas E., III; Howell, Stephen W.; Ohta, Taisuke; Wendt, Joel R.; Montoya, John A.] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Peters, DW (reprint author), Sandia Natl Labs, POB 5800, Albuquerque, NM 87185 USA. EM dwpeter@sandia.gov NR 5 TC 2 Z9 2 U1 2 U2 22 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9907-3 J9 PROC SPIE PY 2014 VL 8994 AR 899419 DI 10.1117/12.2040727 PG 6 WC Nanoscience & Nanotechnology; Optics SC Science & Technology - Other Topics; Optics GA BA4NM UT WOS:000336036300014 ER PT S AU Romano, S De Tommasi, E De Luca, AC Rendina, I Cabrini, S Mocella, V AF Romano, S. De Tommasi, E. De Luca, A. C. Rendina, I. Cabrini, S. Mocella, V. BE Adibi, A Lin, SY Scherer, A TI The negative refraction under out-of-plane incident condition: an experimental study SO PHOTONIC AND PHONONIC PROPERTIES OF ENGINEERED NANOSTRUCTURES IV SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Photonic and Phononic Properties of Engineered Nanostructures IV CY FEB 03-06, 2014 CL San Francisco, CA SP SPIE DE photonic crystal; guided resonance; plasmon resonance; negative refractive index ID PHOTONIC CRYSTALS; SURFACE; RESONANCE; METAMATERIAL; BIOSENSOR; GRATINGS; LIGHT AB In this work, resonance phenomena in a negative photonic crystal are experimentally detected and discussed. Localized surface modes and guided mode resonances appear in the reflection spectrum of a photonic crystal slab interacting with external infrared radiation and can be connected with the negative refractive index of the sample. These phenomena can provide an efficient way to confine the radiation into the structure, with an high field enhancement and a strong sensibility of the resonance position to the refractive index variations. C1 [Romano, S.; De Tommasi, E.; Rendina, I.; Mocella, V.] CNR, IMM, Unita Napoli, Via P Castellino 111, I-80131 Naples, Italy. [Cabrini, S.] Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA USA. [De Luca, A. C.] CNR IBP, I-80131 Naples, Italy. RP Romano, S (reprint author), CNR, IMM, Unita Napoli, Via P Castellino 111, I-80131 Naples, Italy. RI Foundry, Molecular/G-9968-2014; De Luca, Anna Chiara/B-4730-2012; rendina, ivo/F-8266-2013; OI De Luca, Anna Chiara/0000-0002-3696-8465; rendina, ivo/0000-0002-3861-373X; Mocella, Vito/0000-0001-8793-0486; DE TOMMASI, EDOARDO/0000-0003-2030-4557 FU Office of Science; Office of Basic Energy Sciences; U.S. Depaetment of Energy [DE-AC02-05CH11231]; ACDL; AIRC start-up [11454]; EDT; FIR; Italian Ministry of Education, Universities and Research FX Portions of this work were performed at the Molecular Foundry, Lawrence Berkeley National Laboratory, which is supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Depaetment of Energy under Conteact No. DE-AC02-05CH11231. ACDL was supported by an AIRC start-up Grant 11454. ACDL and EDT were supported by a FIR project RBFR12WAY of Italian Ministry of Education, Universities and Research. NR 26 TC 0 Z9 0 U1 0 U2 3 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9907-3 J9 PROC SPIE PY 2014 VL 8994 AR UNSP 89941D DI 10.1117/12.2039721 PG 8 WC Nanoscience & Nanotechnology; Optics SC Science & Technology - Other Topics; Optics GA BA4NM UT WOS:000336036300016 ER PT S AU Michael, S Chow, WW Schneider, HC AF Michael, Stephan Chow, Weng W. Schneider, Hans Christian BE Witzigmann, B Osinski, M Henneberger, F Arakawa, Y TI Group-velocity slowdown in quantum-dots and quantum-dot molecules SO PHYSICS AND SIMULATION OF OPTOELECTRONIC DEVICES XXII SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Physics and Simulation of Optoelectronic Devices XXII CY FEB 03-06, 2014 CL San Francisco, CA SP SPIE ID ELECTROMAGNETICALLY INDUCED TRANSPARENCY; OPTICAL BUFFER; LIGHT; INVERSION; COHERENCE; INTERFERENCE; STATES; MEDIA; WELL AB We investigate theoretically the slowdown of optical pulses due to quantum-coherence effects in In GaAs-based quantum dots and quantum dot molecules. Simple models for the electronic structure of quantum dots and, in particular, quantum-dot molecules are described and calibrated using numerical simulations. It is shown how these models can be used to design optimized quantum-dot molecules for quantum coherence applications. The wave functions and energies obtained from the optimizations are used as input for a microscopic calculation of the quantum-dot material dynamics including carrier scattering and polarization dephasing. The achievable group velocity slowdown in quantum-coherence V schemes consisting of quantum-dot molecule states is shown to be substantially higher than what is achievable from similar transitions in typical In GaAs-based single quantum dots. C1 [Michael, Stephan; Schneider, Hans Christian] Univ Kaiserslautern, Dept Phys, POB 3049, D-67653 Kaiserslautern, Germany. [Chow, Weng W.] Sandia Natl Labs, Semicond Mat & Dev Sci Dept, Albuquerque, NM 87185 USA. RP Michael, S (reprint author), Univ Kaiserslautern, Dept Phys, POB 3049, D-67653 Kaiserslautern, Germany. RI Schneider, Hans Christian/B-9450-2009 OI Schneider, Hans Christian/0000-0001-7656-4919 FU U. S. Department of Energy, Office of Science, Office of Basic Energy Sciences; [SFB787] FX This work was supported in part by Sandia's LDRD program and Energy Frontier Research Center ( EFRC) for Solid- State Lighting Science, funded by U. S. Department of Energy, Office of Science, Office of Basic Energy Sciences. WWC thanks the hospitality of the Technical University Berlin and travel support provided by SFB787. NR 37 TC 0 Z9 0 U1 0 U2 1 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9893-9 J9 PROC SPIE PY 2014 VL 8980 DI 10.1117/12.2042412 PG 16 WC Engineering, Electrical & Electronic; Optics; Physics, Applied SC Engineering; Optics; Physics GA BA4NS UT WOS:000336039900041 ER PT S AU Krishna, L Martinez, AD Baranowski, LL Brawand, NP Koh, CA Stevanovic, V Lusk, MT Toberer, ES Tamboli, AC AF Krishna, Lakshmi Martinez, Aaron D. Baranowski, Lauryn L. Brawand, Nicholas P. Koh, Carolyn A. Stevanovic, Vladan Lusk, Mark T. Toberer, Eric S. Tamboli, Adele C. BE Freundlich, A Guillemoles, JF TI Group IV clathrates: synthesis, optoelectronic properties, and photovoltaic applications SO PHYSICS, SIMULATION, AND PHOTONIC ENGINEERING OF PHOTOVOLTAIC DEVICES III SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Physics, Simulation, and Photonic Engineering of Photovoltaic Devices III CY 2014 CL San Francisco, CA SP SPIE DE clathrate; density functional theory; film; Si; SiGe; type II clathrates; band gap; absorption ID OPTICAL BAND-GAP; II CLATHRATE; SILICON; SI; GERMANIUM; FRAMEWORK; NAXSI136; SUPERCONDUCTIVITY; 1ST-PRINCIPLES; DECOMPOSITION AB Group IV clathrates are a unique class of guest/framework type compounds that are considered potential candidates for a wide range of applications (superconductors to semiconductors). To date, most of the research on group IV clathrates has focused heavily on thermoelectric applications. Recently, these materials have attracted attention as a result of their direct, wide band gaps for possible use in photovoltaic applications. Additionally, framework alloying has been shown to result in tunable band gaps. In this review, we discuss the current work and future opportunities concerning the synthesis and optical characterization of group IV clathrates for optoelectronics applications. C1 [Krishna, Lakshmi; Martinez, Aaron D.; Baranowski, Lauryn L.; Brawand, Nicholas P.; Stevanovic, Vladan; Lusk, Mark T.; Toberer, Eric S.; Tamboli, Adele C.] Colorado Sch Mines, Dept Phys, Golden, CO 80401 USA. [Koh, Carolyn A.] Colarado Sch Mines, Chem Biol Engn, Golden, CO USA. [Toberer, Eric S.; Tamboli, Adele C.] Natl Renewable Energy Lab, Golden, CO USA. RP Krishna, L (reprint author), Colorado Sch Mines, Dept Phys, Golden, CO 80401 USA. EM atamboli@mines.edu FU NSF [DMR-0820518, CNS-0722415]; Colorado School of Mines; Department of Defense (DoD) through the National Defense Science and Engineering Graduate Fellowship (NDSEG); Center for Revolutionary Solar Photoconversion FX We thank Reuben T. Collins and P. Craig Taylor for insightful discussions on optical properties of clathrates. We acknowledge the Renewable Energy MRSEC program (NSF Grant No. DMR-0820518) at the Colorado School of Mines for financial support. The calculations were carried out using the high performance computing resources provided by the Golden Energy Computing Organization at the Colorado School of Mines (NSF Grant No. CNS-0722415). Additional funding was received from the Center for Revolutionary Solar Photoconversion. LLB was supported by the Department of Defense (DoD) through the National Defense Science and Engineering Graduate Fellowship (NDSEG) Program. NR 58 TC 1 Z9 1 U1 1 U2 8 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9894-6 J9 PROC SPIE PY 2014 VL 8981 AR UNSP 898108 DI 10.1117/12.2040056 PG 11 WC Energy & Fuels; Optics; Physics, Applied SC Energy & Fuels; Optics; Physics GA BA4NT UT WOS:000336040600005 ER PT S AU Lumb, MP Steiner, MA Geisz, JF Walters, RJ AF Lumb, Matthew P. Steiner, Myles A. Geisz, John F. Walters, Robert J. BE Freundlich, A Guillemoles, JF TI Analytical modeling of III-V solar cells close to the fundamental limit SO PHYSICS, SIMULATION, AND PHOTONIC ENGINEERING OF PHOTOVOLTAIC DEVICES III SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Physics, Simulation, and Photonic Engineering of Photovoltaic Devices III CY 2014 CL San Francisco, CA SP SPIE DE Photovoltaics; Modeling; Reflector; High efficiency; GaAs; InP; Solar Cell ID LUMINESCENCE AB A highly effective strategy of photon management is to use a back surface reflector. In this work, we present a full analytical model incorporating effects from both the modified generation function and photon recycling in GaAs solar cells with a BSR. We discuss the impact of doping concentration, non-radiative recombination, solar cell dimensions and BSR reflectivity on the efficiency, and compare the prediction of the device models to experimental data measured on GaAs devices. We use the model to predict the performance of alternative III-V materials, such as InP, comparing the predicted performance to state-of-the-art GaAs solar cells. C1 [Lumb, Matthew P.] George Washington Univ, 2121 I St NW, Washington, DC 20037 USA. [Walters, Robert J.] US Naval Res Lab, Washington, DC 20375 USA. [Steiner, Myles A.; Geisz, John F.] Natl Renewable Energy Lab, Golden, CO 80401 USA. RP Lumb, MP (reprint author), George Washington Univ, 2121 I St NW, Washington, DC 20037 USA. NR 20 TC 0 Z9 0 U1 1 U2 8 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9894-6 J9 PROC SPIE PY 2014 VL 8981 AR UNSP 898114 DI 10.1117/12.2041359 PG 9 WC Energy & Fuels; Optics; Physics, Applied SC Energy & Fuels; Optics; Physics GA BA4NT UT WOS:000336040600022 ER PT S AU Xu, WH Hadim, H Chu, YS Shi, Y Nazaretski, E AF Xu, Weihe Hadim, Hamid Chu, Yong S. Shi, Yong Nazaretski, Evgeny BE Shea, HR Ramesham, R TI Measurements of thermal conductivity of La0.95Sr0.05CoO3 nanofibers using MEMS devices SO RELIABILITY, PACKAGING, TESTING, AND CHARACTERIZATION OF MOEMS/MEMS, NANODEVICES, AND NANOMATERIALS XIII SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Reliability, Packaging, Testing, and Characterization of MOEMS/MEMS, Nanodevices, and Nanomaterials XIII CY FEB 03-04, 2014 CL San Francisco, CA SP SPIE, Samsung Adv Inst Technol DE Thermoelectric; Heat Transfer; Thermal Conductivity; Nanoscale; MEMS ID DIMENSIONAL THERMOELECTRIC-MATERIALS; SILICON NANOWIRES; NANOSTRUCTURES; MERIT; PERFORMANCE; FIGURE; OXIDE AB Thermoelectric oxide nanofibers prepared by electrospinning are expected to have reduced thermal conductivity when compared to bulk samples. Measurements of nanofibers' thermal conductivity is challenging since it involves sophisticated sample preparation methods. In this work, we present a novel method suitable for measurements of thermal conductivity in a single nanofiber. A microelectro-mechanical (MEMS) device has been designed and fabricated to perform thermal conductivity measurements on a single nanofiber. A special Si template was designed to collect and transfer individual nanofibers onto a MEMS device. Pt was deposited by Focused Ion Beam to reduce the effective length of a prepared nanofiber. A single La0.95Sr0.05CoO3 nanofiber with a diameter of 140 nm was studied and characterized using this approach. Measured thermal conductivity of a nanofiber was determined to be 0.7 W/m.K, which is 23% of the value reported for bulk La0.95Sr0.05CoO3 samples. C1 [Xu, Weihe; Chu, Yong S.; Nazaretski, Evgeny] Brookhaven Natl Lab, Upton, NY 11973 USA. [Xu, Weihe; Hadim, Hamid; Shi, Yong] Stevens Inst Technol, Dept Mech Engn, Hoboken, NJ 07030 USA. RP Xu, WH (reprint author), Brookhaven Natl Lab, Upton, NY 11973 USA. FU US Department of Energy, Office of Basic Energy Sciences [DE-AC02-98CH10886] FX This work was carried out in part at Brookhaven National Laboratory, Center for Functional Nanomaterials at Brookhaven National Laboratory, supported by the US Department of Energy, Office of Basic Energy Sciences, under contract no. DE-AC02-98CH10886. NR 34 TC 0 Z9 0 U1 2 U2 4 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9888-5 J9 PROC SPIE PY 2014 VL 8975 AR UNSP 89750D DI 10.1117/12.2054464 PG 6 WC Nanoscience & Nanotechnology; Materials Science, Characterization & Testing; Optics SC Science & Technology - Other Topics; Materials Science; Optics GA BA4NQ UT WOS:000336038300010 ER PT J AU Zhou, JG Hu, YF Li, XL Wang, CM Zuin, L AF Zhou, Jigang Hu, Yongfeng Li, Xiaolin Wang, Chongmin Zuin, Lucia TI Chemical bonding in amorphous Si-coated carbon nanotubes as anodes for Li ion batteries: a XANES study SO RSC ADVANCES LA English DT Article ID X-RAY-ABSORPTION; ELECTROLYTE INTERPHASE SEI; NANORODS-GRAPHENE HYBRID; OXYGEN REDUCTION; COBALT OXIDE; NANOCRYSTALS; SILICON; SPECTROSCOPY; PERFORMANCE; EVOLUTION AB The nature of the chemical bonding in an amorphous Si-coated carbon nanotube (Si-CNT) anode, and its evolution upon electrochemical cycling, have been investigated using comprehensive X-ray absorption spectroscopy (XANES) at the Si L-and K-edges, along with the C and O K-edges. The Si nanolayer on the CNT is found to be anchored to the CNT via Si-O-C bonding. This bond weakens upon electrochemical cycling, accompanied by the generation of Li2CO3 on the surface of the Si-CNT. These findings are crucial in designing further improved Si-C composite anodes for lithium ion batteries. C1 [Zhou, Jigang; Hu, Yongfeng; Zuin, Lucia] Canadian Light Source Inc, Saskatoon, SK, Canada. [Li, Xiaolin; Wang, Chongmin] Pacific NW Natl Lab, Richland, WA 99354 USA. RP Zhou, JG (reprint author), Canadian Light Source Inc, Saskatoon, SK, Canada. EM jigang.zhou@lightsource.ca; Chongmin.wang@pnnl.gov RI Zhou, Jigang/N-6831-2014 OI Zhou, Jigang/0000-0001-6644-2862 FU NSERC; NRC; CIHR; University of Saskatchewan; DOE's Office of Biological and Environmental Research and located at PNNL FX Thanks to Drs J. Dynes and T. Regier at CLS for technical assistance. CLS is supported by NSERC, NRC, CIHR and the University of Saskatchewan. We thank Dr D. J. Burton of Applied Science for providing the Si-CNT sample. CW is grateful for the support of the Chemical Imaging Initiative of Paci. c Northwest National Laboratory. Part of this work was conducted in the William R. Wiley Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility sponsored by the DOE's Office of Biological and Environmental Research and located at PNNL. PNNL is operated by Battelle for the Department of Energy under Contract DE-AC0576RLO1830. NR 22 TC 6 Z9 6 U1 7 U2 70 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 2014 VL 4 IS 39 BP 20226 EP 20229 DI 10.1039/c4ra01332h PG 4 WC Chemistry, Multidisciplinary SC Chemistry GA AH4EI UT WOS:000336079200019 ER PT J AU Breslow, AD Tiwari, A Schulz, M Carrington, L Tang, LJ Mars, J AF Breslow, Alex D. Tiwari, Ananta Schulz, Martin Carrington, Laura Tang, Lingjia Mars, Jason TI Enabling fair pricing on high performance computer systems with node sharing SO SCIENTIFIC PROGRAMMING LA English DT Article DE Online pricing; supercomputer accounting; resource sharing; chip multiprocessor; contention; computer systems management AB Co-location, where multiple jobs share compute nodes in large-scale HPC systems, has been shown to increase aggregate throughput and energy efficiency by 10-20%. However, system operators disallow co-location due to fair-pricing concerns, i.e., a pricing mechanism that considers performance interference from co-running jobs. In the current pricing model, application execution time determines the price, which results in unfair prices paid by the minority of users whose jobs suffer from co-location. This paper presents POPPA, a runtime system that enables fair pricing by delivering precise online interference detection and facilitates the adoption of supercomputers with co-locations. POPPA leverages a novel shutter mechanism - a cyclic, fine-grained interference sampling mechanism to accurately deduce the interference between co-runners - to provide unbiased pricing of jobs that share nodes. POPPA is able to quantify inter-application interference within 4% mean absolute error on a variety of co-located benchmark and real scientific workloads. C1 [Breslow, Alex D.] Univ Calif San Diego, San Diego, CA 92103 USA. [Tiwari, Ananta; Carrington, Laura] San Diego Supercomp Ctr, La Jolla, CA USA. [Schulz, Martin] Lawrence Livermore Natl Lab, Livermore, CA USA. [Tang, Lingjia; Mars, Jason] Univ Michigan, Ann Arbor, MI 48109 USA. RP Breslow, AD (reprint author), Univ Calif San Diego, San Diego, CA 92103 USA. EM abreslow@cs.ucsd.edu; tiwari@sdsc.edu; schulzm@llnl.gov; lcarring@sdsc.edu; lingjia@eecs.umich.edu; profmars@eecs.umich.edu FU U.S. Department of Energy by Lawrence Livermore National Laboratory [DE-AC52-07NA27344 (LLNL-CONF-635977)]; DOE Office of Science, Advanced Scientific Computing Research [62855]; National Science Foundation [CCF-1302682] FX The authors thank the anonymous reviewers for their time and feedback. In addition, they thank Professor Mike Norman of UCSD, Professor Leo Porter of Skidmore College, and Terri Quinn of LLNL. Some of the ideas in this paper were inspired by discussions with the late Allan Snavely. Part of this work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344 (LLNL-CONF-635977). This work was supported in part by the DOE Office of Science, Advanced Scientific Computing Research, under award number 62855 "Beyond the Standard Model - Towards an Integrated Modeling Methodology for the Performance and Power"; PNNL lead institution; Program Manager Sonia Sachs. The authors acknowledge National Science Foundation support under CCF-1302682. NR 56 TC 0 Z9 0 U1 0 U2 1 PU IOS PRESS PI AMSTERDAM PA NIEUWE HEMWEG 6B, 1013 BG AMSTERDAM, NETHERLANDS SN 1058-9244 EI 1875-919X J9 SCI PROGRAMMING-NETH JI Sci. Program. PY 2014 VL 22 IS 2 BP 59 EP 74 DI 10.3233/SPR-140387 PG 16 WC Computer Science, Software Engineering SC Computer Science GA AH8ZY UT WOS:000336429300002 ER PT J AU Warren, MS AF Warren, Michael S. TI 2HOT: An improved parallel hashed oct-tree N-body algorithm for cosmological simulation SO SCIENTIFIC PROGRAMMING LA English DT Article DE Computational cosmology; N-body; fast multipole method ID HALO MASS FUNCTION; MULTIPOLE METHOD; 3 DIMENSIONS; CODE; UNIVERSALITY; PARAMETERS; EVOLUTION; TOOLKIT; SPHERE AB We report on improvements made over the past two decades to our adaptive treecode N-body method (HOT). A mathematical and computational approach to the cosmological N-body problem is described, with performance and scalability measured up to 256k (2(18)) processors. We present error analysis and scientific application results from a series of more than ten 69 billion (4096(3)) particle cosmological simulations, accounting for 4x10(20) floating point operations. These results include the first simulations using the new constraints on the standard model of cosmology from the Planck satellite. Our simulations set a new standard for accuracy and scientific throughput, while meeting or exceeding the computational efficiency of the latest generation of hybrid TreePM N-body methods. C1 Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. RP Warren, MS (reprint author), Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. EM msw@lanl.gov FU Office of Science of the Department of Energy [DE-AC05-00OR22725]; Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]; National Nuclear Security Administration of the U.S. Department of Energy [DE-AC52-06NA25396] FX We gratefully acknowledge John Salmon for his many contributions to the initial version of HOT, and helpful comments on a draft version of this manuscript. We thank Mark Galassi for his memory management improvements to 2HOT and Ben Bergen for assistance with the OpenCL implementation. We thank the Institutional Computing Program at LANL for providing the computing resources used for our production simulations. This research used resources of the Oak Ridge Leadership Computing Facility at Oak Ridge National Laboratory, which is supported by the Office of Science of the Department of Energy under Contract DE-AC05-00OR22725. This research also 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. This research was performed under the auspices of the National Nuclear Security Administration of the U.S. Department of Energy under Contract DE-AC52-06NA25396. NR 75 TC 0 Z9 0 U1 1 U2 2 PU HINDAWI PUBLISHING CORPORATION PI NEW YORK PA 410 PARK AVENUE, 15TH FLOOR, #287 PMB, NEW YORK, NY 10022 USA SN 1058-9244 EI 1875-919X J9 SCI PROGRAMMING-NETH JI Sci. Program. PY 2014 VL 22 IS 2 BP 109 EP 124 DI 10.3233/SPR-140385 PG 16 WC Computer Science, Software Engineering SC Computer Science GA AH8ZY UT WOS:000336429300005 ER PT J AU Jung, M Wilson, EH Choi, W Shalf, J Aktulga, HM Yang, C Saule, E Catalyurek, UV Kandemir, M AF Jung, Myoungsoo Wilson, Ellis H., III Choi, Wonil Shalf, John Aktulga, Hasan Metin Yang, Chao Saule, Erik Catalyurek, Umit V. Kandemir, Mahmut TI Exploring the future of out-of-core computing with compute-local non-volatile memory SO SCIENTIFIC PROGRAMMING LA English DT Article DE High performance computing; scientific application; non-volatile memory; solid state disk; out-of-core computing ID FILE SYSTEM; FLASH; EIGENSOLVER; PARALLELISM; I/O AB Drawing parallels to the rise of general purpose graphical processing units (GPGPUs) as accelerators for specific high-performance computing (HPC) workloads, there is a rise in the use of non-volatile memory (NVM) as accelerators for I/O-intensive scientific applications. However, existing works have explored use of NVM within dedicated I/O nodes, which are distant from the compute nodes that actually need such acceleration. As NVM bandwidth begins to out-pace point-to-point network capacity, we argue for the need to break from the archetype of completely separated storage. Therefore, in this work we investigate co-location of NVM and compute by varying I/O interfaces, file systems, types of NVM, and both current and future SSD architectures, uncovering numerous bottlenecks implicit in these various levels in the I/O stack. We present novel hardware and software solutions, including the new Unified File System (UFS), to enable fuller utilization of the new compute-local NVM storage. Our experimental evaluation, which employs a real-world Out-of-Core (OoC) HPC application, demonstrates throughput increases in excess of an order of magnitude over current approaches. C1 [Jung, Myoungsoo; Choi, Wonil] Univ Texas Dallas, Dept Elect Engn, Richardson, TX 75083 USA. [Wilson, Ellis H., III; Choi, Wonil; Kandemir, Mahmut] Penn State Univ, Dept Comp Sci & Engn, University Pk, PA 16802 USA. [Shalf, John; Aktulga, Hasan Metin; Yang, Chao] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Computat Res Div, Berkeley, CA 94720 USA. [Shalf, John] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Natl Energy Res Sci Comp Ctr, Berkeley, CA 94720 USA. [Saule, Erik; Catalyurek, Umit V.] Ohio State Univ, Columbus, OH 43210 USA. RP Jung, M (reprint author), Univ Texas Dallas, Dept Elect Engn, Richardson, TX 75083 USA. EM jung@utdallas.edu; ellis@cse.psu.edu; wonil.choi@utdallas.edu; jshalf@lbl.gov; hmaktulga@lbl.gov; cyang@lbl.gov; esaule@bmi.osu.edu; umit@bmi.osu.edu; kandemir@cse.psu.edu OI Catalyurek, Umit/0000-0002-5625-3758 FU NSF [1017882, 0937949, 0833126, OCI-0904809]; DOE [DE-SC0002156]; ASCR Office in the DOE Office of Science [DE-AC02-05CH11231]; Scientific Discovery through Advanced Computing program - U.S. Department of Energy, Office of Science, Advanced Scientific Computing Research and Nuclear Physics; U.S. Department of Energy [DE-AC02-05CH11231]; University of Texas at Dallas FX This research is supported in part by University of Texas at Dallas, NSF grants 1017882, 0937949, 0833126, OCI-0904809 and DOE grant DE-SC0002156. This work was also supported by the ASCR Office in the DOE Office of Science under contract number DE-AC02-05CH11231 and partially supported by Scientific Discovery through Advanced Computing program funded by U.S. Department of Energy, Office of Science, Advanced Scientific Computing Research and Nuclear Physics.; This manuscript has been authored by an author at Lawrence Berkeley National Laboratory under Contract No. DE-AC02-05CH11231 with the U.S. Department of Energy. The U.S. Government retains, and the publisher, by accepting the article for publication, acknowledges, that the U.S. 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 U.S. Government purposes. NR 43 TC 0 Z9 0 U1 0 U2 3 PU IOS PRESS PI AMSTERDAM PA NIEUWE HEMWEG 6B, 1013 BG AMSTERDAM, NETHERLANDS SN 1058-9244 EI 1875-919X J9 SCI PROGRAMMING-NETH JI Sci. Program. PY 2014 VL 22 IS 2 BP 125 EP 139 DI 10.3233/SPR-140384 PG 15 WC Computer Science, Software Engineering SC Computer Science GA AH8ZY UT WOS:000336429300006 ER PT J AU Laney, D Langer, S Weber, C Lindstrom, P Wegener, A AF Laney, Daniel Langer, Steven Weber, Christopher Lindstrom, Peter Wegener, Al TI Assessing the effects of data compression in simulations using physically motivated metrics SO SCIENTIFIC PROGRAMMING LA English DT Article DE Data compression; high performance computing ID RAYLEIGH-TAYLOR INSTABILITY; FLOATING-POINT DATA AB This paper examines whether lossy compression can be used effectively in physics simulations as a possible strategy to combat the expected data-movement bottleneck in future high performance computing architectures. We show that, for the codes and simulations we tested, compression levels of 3-5X can be applied without causing significant changes to important physical quantities. Rather than applying signal processing error metrics, we utilize physics-based metrics appropriate for each code to assess the impact of compression. We evaluate three different simulation codes: a Lagrangian shock-hydrodynamics code, an Eulerian higher-order hydrodynamics turbulence modeling code, and an Eulerian coupled laser-plasma interaction code. We compress relevant quantities after each time-step to approximate the effects of tightly coupled compression and study the compression rates to estimate memory and disk-bandwidth reduction. We find that the error characteristics of compression algorithms must be carefully considered in the context of the underlying physics being modeled. C1 [Laney, Daniel; Langer, Steven; Weber, Christopher; Lindstrom, Peter] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. [Wegener, Al] Samplify, Campbell, CA 95008 USA. RP Laney, D (reprint author), Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. EM dlaney@llnl.gov; langer1@llnl.gov; weber30@llnl.gov; pl@llnl.gov; awegener@samplify.com OI Lindstrom, Peter/0000-0003-3817-4199 FU U.S. Department of Energy by Lawrence Livermore National Laboratory [DE-AC52-07NA27344]; Defense Advanced Research Projects Agency [HR0011-07-9-0001] FX This document was released as LLNL-CONF-642236. This work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344. Some of this material is based upon work supported by the Defense Advanced Research Projects Agency under its Agreement No. HR0011-07-9-0001. NR 35 TC 0 Z9 0 U1 0 U2 4 PU HINDAWI PUBLISHING CORPORATION PI NEW YORK PA 410 PARK AVENUE, 15TH FLOOR, #287 PMB, NEW YORK, NY 10022 USA SN 1058-9244 EI 1875-919X J9 SCI PROGRAMMING-NETH JI Sci. Program. PY 2014 VL 22 IS 2 BP 141 EP 155 DI 10.3233/SPR-140386 PG 15 WC Computer Science, Software Engineering SC Computer Science GA AH8ZY UT WOS:000336429300007 ER PT J AU Dart, E Rotman, L Tierney, B Hester, M Zurawski, J AF Dart, Eli Rotman, Lauren Tierney, Brian Hester, Mary Zurawski, Jason TI The Science DMZ: A network design pattern for data-intensive science SO SCIENTIFIC PROGRAMMING LA English DT Article DE High performance networking; perfsonar; data-intensive science; network architecture; measurement AB The ever-increasing scale of scientific data has become a significant challenge for researchers that rely on networks to interact with remote computing systems and transfer results to collaborators worldwide. Despite the availability of high-capacity connections, scientists struggle with inadequate cyberinfrastructure that cripples data transfer performance, and impedes scientific progress. The Science DMZ paradigm comprises a proven set of network design patterns that collectively address these problems for scientists. We explain the Science DMZ model, including network architecture, system configuration, cybersecurity, and performance tools, that creates an optimized network environment for science. We describe use cases from universities, supercomputing centers and research laboratories, highlighting the effectiveness of the Science DMZ model in diverse operational settings. In all, the Science DMZ model is a solid platform that supports any science workflow, and flexibly accommodates emerging network technologies. As a result, the Science DMZ vastly improves collaboration, accelerating scientific discovery. C1 [Dart, Eli; Rotman, Lauren; Tierney, Brian; Hester, Mary] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Energy Sci Network, Berkeley, CA 94720 USA. [Zurawski, Jason] Internet2, Off CTO, Washington, DC USA. RP Dart, E (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Energy Sci Network, Berkeley, CA 94720 USA. EM eddart@lbl.gov; lbrotman@lbl.gov; bltierney@lbl.gov; mchester@lbl.gov; zurawski@internet2.edu FU National Science Foundation; U.S. Department of Energy [DE-AC02-05CH11231] FX The authors wish to acknowledge the vision of the National Science Foundation for its support of the CC-NIE program.; This manuscript has been authored by an author at Lawrence Berkeley National Laboratory under Contract No. DE-AC02-05CH11231 with the U.S. Department of Energy. The U.S. Government retains, and the publisher, by accepting the article for publication, acknowledges, that the U.S. 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 U.S. Government purposes. NR 17 TC 3 Z9 3 U1 1 U2 5 PU IOS PRESS PI AMSTERDAM PA NIEUWE HEMWEG 6B, 1013 BG AMSTERDAM, NETHERLANDS SN 1058-9244 EI 1875-919X J9 SCI PROGRAMMING-NETH JI Sci. Program. PY 2014 VL 22 IS 2 BP 173 EP 185 DI 10.3233/SPR-140382 PG 13 WC Computer Science, Software Engineering SC Computer Science GA AH8ZY UT WOS:000336429300009 ER PT J AU Cyr, EC Shadid, J Wildey, T AF Cyr, Eric C. Shadid, John Wildey, Tim TI APPROACHES FOR ADJOINT-BASED A POSTERIORI ANALYSIS OF STABILIZED FINITE ELEMENT METHODS SO SIAM JOURNAL ON SCIENTIFIC COMPUTING LA English DT Article DE stabilized methods; adjoint problem; error analysis; adjoint consistency; convection-diffusion; Stokes; Navier-Stokes ID COMPUTATIONAL FLUID-DYNAMICS; NAVIER-STOKES EQUATIONS; ERROR ESTIMATION; HEAT-TRANSFER; FORMULATION AB This study derives a posteriori error estimates for linear functionals of the solution of systems of partial differential equations discretized using stabilized continuous Galerkin methods. We investigate a convection-diffusion equation, the Stokes equations, and incompressible low Reynolds number flow governed by the Navier-Stokes equations. We consider three well-known stabilization methods and show that only one of the three is adjoint consistent and that even this case is contingent upon a proper treatment of the adjoint data. A standard approach for a posteriori error analysis uses the adjoint of the stabilized formulation, which inherits the difficulties induced by the lack of adjoint consistency. We introduce and analyze two alternative approaches. The first is based on the addition of stabilization terms to the adjoint data, while the second is based on a stabilized formulation of the formal adjoint problem. We show that any of the three approaches can be used to derive a fully computable error representation. However, numerical results show that these new alternative approaches result in more accurate error estimates for a variety of problems. C1 [Cyr, Eric C.] Sandia Natl Labs, Scalable Algorithms Dept, Albuquerque, NM 87185 USA. [Shadid, John] Sandia Natl Labs, Multiphys Simulat Technol Dept, Albuquerque, NM 87185 USA. [Wildey, Tim] Sandia Natl Labs, Optimizat & Uncertainty Quantificat Dept, Albuquerque, NM 87185 USA. RP Cyr, EC (reprint author), Sandia Natl Labs, Scalable Algorithms Dept, POB 5800, Albuquerque, NM 87185 USA. EM eccyr@sandia.gov; jnshadi@sandia.gov; tmwilde@sandia.gov FU U.S. Department of Energy Office of Science, Advanced Scientific Computing Research-Applied Mathematics Program at Sandia National Laboratories; U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX This work was partially supported by the U.S. Department of Energy Office of Science, Advanced Scientific Computing Research-Applied Mathematics Program at Sandia National Laboratories. 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 28 TC 4 Z9 4 U1 0 U2 1 PU SIAM PUBLICATIONS PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA SN 1064-8275 EI 1095-7197 J9 SIAM J SCI COMPUT JI SIAM J. Sci. Comput. PY 2014 VL 36 IS 2 BP A766 EP A791 DI 10.1137/120895822 PG 26 WC Mathematics, Applied SC Mathematics GA AH0NU UT WOS:000335817600020 ER PT J AU Haut, T Wingate, B AF Haut, Terry Wingate, Beth TI AN ASYMPTOTIC PARALLEL-IN-TIME METHOD FOR HIGHLY OSCILLATORY PDES SO SIAM JOURNAL ON SCIENTIFIC COMPUTING LA English DT Article DE parallel-in-time; asymptotic; heterogeneous multiscale method ID HETEROGENEOUS MULTISCALE METHODS; ORDINARY DIFFERENTIAL-EQUATIONS; HAMILTONIAN-SYSTEMS; ROTATING-FLOWS; INITIAL DATA; PARAREAL; DISCRETIZATION; ALGORITHMS; DYNAMICS; NUMBER AB We present a new time-stepping algorithm for nonlinear PDEs that exhibit scale separation in time of a highly oscillatory nature. The algorithm combines the parareal method-a parallel-in-time scheme introduced in [J.-L. Lions, Y. Maday, and G. Turinici, C. R. Acad. Sci. Paris Ser. I Math., 332 (2001), pp. 661-668]-with techniques from the heterogeneous multiscale method (cf. [W. E and B. Engquist, Notices Amer. Math. Soc., 50 (2003), pp. 1062-1070]), which make use of the slow asymptotic structure of the equations [A. J. Majda and P. Embid, Theoret. Comput. Fluid Dyn., 11 (1998), pp. 155-169]. We present error bounds, based on the analysis in [M. J. Gander and E. Hairer, in Domain Decomposition Methods in Science and Engineering XVII, Springer, Berlin, 2008, pp. 45-56] and [G. Bal, in Domain Decomposition Methods in Science and Engineering, Springer, Berlin, 2005, pp. 425-432], that demonstrate convergence of the method. A complexity analysis also demonstrates that the parallel speedup increases arbitrarily with greater scale separation. Finally, we demonstrate the accuracy and efficiency of the method on the (onedimensional) rotating shallow water equations, which is a standard test problem for new algorithms in geophysical fluid problems. Compared to exponential integrators such as ETDRK4 and Strang splitting-which solve the stiff oscillatory part exactly-we find that we can use coarse time steps that are orders of magnitude larger (for a comparable accuracy), yielding an estimated parallel speedup of approximately 100 for physically realistic parameter values. For the (one-dimensional) shallow water equations, we also show that the estimated parallel speedup of this " asymptotic parareal method" is more than a factor of 10 greater than the speedup obtained from the standard parareal method. C1 [Haut, Terry; Wingate, Beth] Los Alamos Natl Lab, CNLS, Los Alamos, NM 87545 USA. RP Haut, T (reprint author), Los Alamos Natl Lab, CNLS, MS B258, Los Alamos, NM 87545 USA. EM terryhaut@gmail.com; wingate@lanl.gov NR 38 TC 9 Z9 9 U1 0 U2 4 PU SIAM PUBLICATIONS PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA SN 1064-8275 EI 1095-7197 J9 SIAM J SCI COMPUT JI SIAM J. Sci. Comput. PY 2014 VL 36 IS 2 BP A693 EP A713 DI 10.1137/130914577 PG 21 WC Mathematics, Applied SC Mathematics GA AH0NU UT WOS:000335817600017 ER PT J AU Rubensson, EH Niklasson, AMN AF Rubensson, Emanuel H. Niklasson, Anders M. N. TI INTERIOR EIGENVALUES FROM DENSITY MATRIX EXPANSIONS IN QUANTUM MECHANICAL MOLECULAR DYNAMICS SO SIAM JOURNAL ON SCIENTIFIC COMPUTING LA English DT Article DE Born-Oppenheimer molecular dynamics; density functional theory; density matrix purification; Fermi operator expansion; homo-lumo gap; interior eigenvalues; linear scaling electronic structure theory; matrix functions; nonmonotonic expansion; recursive expansion; scale-and-fold acceleration; trace-correcting purification ID ELECTRONIC-STRUCTURE CALCULATIONS; CONSISTENT-FIELD THEORY; TIGHT-BINDING METHOD; SYSTEM-SIZE; PURIFICATION; SIMULATIONS; MINIMIZATION; CONVERGENCE; STATES; ATOMS AB An accelerated polynomial expansion scheme to construct the density matrix in quantum mechanical molecular dynamics simulations is proposed. The scheme is based on recursive density matrix expansions, e. g., [A. M. N. Niklasson, Phys. Rev. B, 66 (2002), 155115], which are accelerated by a scale-and-fold technique [E. H. Rubensson, J. Chem. Theory Comput., 7 (2011), pp. 1233-1236]. The acceleration scheme requires interior eigenvalue estimates, which may be expensive and cumbersome to come by. Here we show how such eigenvalue estimates can be extracted from the recursive expansion by a simple and robust procedure at a negligible computational cost. Our method is illustrated with density functional tight-binding Born-Oppenheimer molecular dynamics simulations, where the computational effort is dominated by the density matrix construction. In our analysis we identify two different phases of the recursive polynomial expansion, the conditioning and purification phases, and we show that the acceleration represents an improvement of the conditioning phase, which typically gives a significant reduction of the computational cost. C1 [Rubensson, Emanuel H.] Uppsala Univ, Dept Informat Technol, Div Comp Sci, SE-75105 Uppsala, Sweden. [Niklasson, Anders M. N.] Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. RP Rubensson, EH (reprint author), Uppsala Univ, Dept Informat Technol, Div Comp Sci, Box 337, SE-75105 Uppsala, Sweden. EM emanuel.rubensson@it.uu.se; amn@lanl.gov FU Goran Gustafsson Foundation; Swedish Research Council [621-2012-3861]; Lisa and Carl-Gustav Esseen Foundation; Swedish National Strategic e-Science Research Program (eSSENCE); United States Department of Energy Office of Basic Energy Sciences; International Ten Bar Java Group FX This work was supported by the Goran Gustafsson Foundation, the Swedish Research Council (grant 621-2012-3861), the Lisa and Carl-Gustav Esseen Foundation, the Swedish National Strategic e-Science Research Program (eSSENCE), the United States Department of Energy Office of Basic Energy Sciences, and the International Ten Bar Java Group of T. Peery. NR 67 TC 3 Z9 3 U1 0 U2 10 PU SIAM PUBLICATIONS PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA SN 1064-8275 EI 1095-7197 J9 SIAM J SCI COMPUT JI SIAM J. Sci. Comput. PY 2014 VL 36 IS 2 BP B147 EP B170 DI 10.1137/130911585 PG 24 WC Mathematics, Applied SC Mathematics GA AH0NU UT WOS:000335817600025 ER PT J AU Petra, CG Schenk, O Lubin, M Gaeertner, K AF Petra, Cosmin G. Schenk, Olaf Lubin, Miles Gaeertner, Klaus TI AN AUGMENTED INCOMPLETE FACTORIZATION APPROACH FOR COMPUTING THE SCHUR COMPLEMENT IN STOCHASTIC OPTIMIZATION SO SIAM JOURNAL ON SCIENTIFIC COMPUTING LA English DT Article DE parallel linear algebra; stochastic programming; stochastic optimization; parallel-interior point; economic dispatch; unit commitment ID SYMMETRIC INDEFINITE SYSTEMS; SPARSE LINEAR-SYSTEMS; UNIT COMMITMENT; PRECONDITIONER; ALGORITHMS; SOLVER; MARKET AB We present a scalable approach and implementation for solving stochastic optimization problems on high-performance computers. In this work we revisit the sparse linear algebra computations of the parallel solver PIPS with the goal of improving the shared-memory performance and decreasing the time to solution. These computations consist of solving sparse linear systems with multiple sparse right-hand sides and are needed in our Schur-complement decomposition approach to compute the contribution of each scenario to the Schur matrix. Our novel approach uses an incomplete augmented factorization implemented within the PARDISO linear solver and an outer BiCGStab iteration to efficiently absorb pivot perturbations occurring during factorization. This approach is capable of both efficiently using the cores inside a computational node and exploiting sparsity of the right-hand sides. We report on the performance of the approach on high-performance computers when solving stochastic unit commitment problems of unprecedented size (billions of variables and constraints) that arise in the optimization and control of electrical power grids. Our numerical experiments suggest that supercomputers can be efficiently used to solve power grid stochastic optimization problems with thousands of scenarios under the strict "real-time" requirements of power grid operators. To our knowledge, this has not been possible prior to the present work. C1 [Petra, Cosmin G.] Argonne Natl Lab, Math & Comp Sci Div, Argonne, IL 60439 USA. [Schenk, Olaf] Univ Svizzera Italiana, Inst Computat Sci, CH-6900 Lugano, Switzerland. [Lubin, Miles] MIT, Ctr Operat Res, Cambridge, MA 02139 USA. [Gaeertner, Klaus] Weierstrass Inst Appl Anal & Stochast, D-10117 Berlin, Germany. RP Petra, CG (reprint author), Argonne Natl Lab, Math & Comp Sci Div, Argonne, IL 60439 USA. EM petra@mcs.anl.gov; olaf.schenk@usi.ch; mlubin@mit.edu; klaus.gaertner@wias-berlin.de OI Lubin, Miles/0000-0001-6781-9633 FU U.S. Department of Energy [DE-AC02-06CH11357]; Office of Science of the U.S. Department of Energy [DE-AC02-06CH11357]; Department of Energy INCITE award "Optimization of Complex Energy Systems under Uncertainty," FX This work was supported by the U.S. Department of Energy under contract DE-AC02-06CH11357. This research used resources of the Laboratory Computing Resource Center and the Argonne Leadership Computing Facility at Argonne National Laboratory, which is supported by the Office of Science of the U.S. Department of Energy under contract DE-AC02-06CH11357. Computing time on Intrepid was granted by a 2012 Department of Energy INCITE award "Optimization of Complex Energy Systems under Uncertainty," PI Mihai Anitescu, Co-PI Cosmin G. Petra. 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 43 TC 12 Z9 13 U1 0 U2 2 PU SIAM PUBLICATIONS PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA SN 1064-8275 EI 1095-7197 J9 SIAM J SCI COMPUT JI SIAM J. Sci. Comput. PY 2014 VL 36 IS 2 BP C139 EP C162 DI 10.1137/130908737 PG 24 WC Mathematics, Applied SC Mathematics GA AH0NU UT WOS:000335817600032 ER PT S AU Antoniadou, I Worden, K Manson, G Dervilis, N Taylor, SG Farrar, CR AF Antoniadou, I. Worden, K. Manson, G. Dervilis, N. Taylor, S. G. Farrar, Charles R. BE Uhl, T TI Damage detection in RAPTOR telescope systems using time-frequency analysis methods SO SMART DIAGNOSTICS V SE Key Engineering Materials LA English DT Proceedings Paper CT 5th International Congress of Technical Diagnostics CY SEP 03-05, 2012 CL Krakow, POLAND SP Famur, EC Test Syst, EC Syst DE RAPTOR telescope; empirical mode decomposition; Hilbert transform; Teager-Kaiser energy operator; energy separation algorithms ID EMPIRICAL MODE DECOMPOSITION; FAULT-DETECTION; GEAR AB The RAPTOR telescope systems are astronomical observatories that operate in remote locations in New Mexico searching for astrophysical transients called gamma-ray bursts. Their operating condition should remain at good levels in order to have accurate observations. Currently, the first component of the RAPTOR telescopes to fail is a capstan driving mechanism that operates in a run-to failure mode. The capstans wear relatively frequently because of their manufacturing material and can cause damage to other more expensive components, such as the drive wheels and the telescope optics. Monitoring the condition of these systems seems a reasonable solution since the unpredictable rate at which the capstans experience wear, in combination with the remote locations and high duty cycles of these telescope systems, make it unprofitable to choose a strategy of replacing the capstans at chosen intervals. Experimental tests of the telescope systems reported here recorded vibration signals during clockwise and counterclockwise rotations, similar to a motion known as "homing-sequence". The Empirical Mode Decomposition (EMD) method in combination with the Hilbert Transform (HT) and a new alternative method for the estimation of the instantaneous features of a signal that applies an energy tracking operator, called Teager-Kaiser Energy operator, and an energy separation algorithm to the data being analysed, are the time-frequency analysis methods used for analysis here. C1 [Antoniadou, I.; Worden, K.; Manson, G.; Dervilis, N.] Univ Sheffield, Dept Mech Engn, Dynam Res Grp, Mappin St, Sheffield S1 3JD, S Yorkshire, England. [Taylor, S. G.; Farrar, Charles R.] Los Alamos Natl Lab, Engn Sci & Applicat Div, Los Alamos, NM 87545 USA. RP Antoniadou, I (reprint author), Univ Sheffield, Dept Mech Engn, Dynam Res Grp, Mappin St, Sheffield S1 3JD, S Yorkshire, England. EM I.Antoniadou@sheffield.ac.uk OI Manson, Graeme/0000-0001-7484-5127; Farrar, Charles/0000-0001-6533-6996 FU European Commission FX This work is part of the SYSWND project, operated under the Marie Curie Network Scheme, and funded by the European Commission Seventh Framework Program. In addition the authors want to thank especially prof. Wieslaw Staszewski of the Faculty Mechanical Engineering and Robotics, of AGH University, for his help on time-frequency analysis methods on this paper. NR 24 TC 0 Z9 0 U1 0 U2 1 PU TRANS TECH PUBLICATIONS LTD PI DURNTEN-ZURICH PA KREUZSTRASSE 10, 8635 DURNTEN-ZURICH, SWITZERLAND SN 1013-9826 J9 KEY ENG MATER PY 2014 VL 588 BP 43 EP + DI 10.4028/www.scientific.net/KEM.588.43 PG 3 WC Engineering, Civil; Engineering, Mechanical; Materials Science, Multidisciplinary SC Engineering; Materials Science GA BA4SM UT WOS:000336234700005 ER PT S AU Dervilis, N Choi, M Antoniadou, I Farinholt, KM Taylor, SG Barthorpe, RJ Park, G Farrar, CR Worden, K AF Dervilis, N. Choi, M. Antoniadou, I. Farinholt, K. M. Taylor, S. G. Barthorpe, R. J. Park, G. Farrar, C. R. Worden, K. BE Uhl, T TI Machine Learning Applications for a Wind Turbine Blade under Continuous Fatigue Loading SO SMART DIAGNOSTICS V SE Key Engineering Materials LA English DT Proceedings Paper CT 5th International Congress of Technical Diagnostics CY SEP 03-05, 2012 CL Krakow, POLAND SP Famur, EC Test Syst, EC Syst DE Damage detection; Novelty analysis; Radial Basis Function Networks; Auto-associative Neural Networks; Fatigue test; Wind turbine blade ID HEALTH MONITORING METHODOLOGY; NOVELTY DETECTION; EXPERIMENTAL VALIDATION AB Structural health monitoring (SHM) systems will be one of the leading factors in the successful establishment of wind turbines in the energy arena. Detection of damage at an early stage is a vital issue as blade failure would be a catastrophic result for the entire wind turbine. In this study the SHM analysis will be based on experimental measurements of vibration analysis, extracted of a 9m CX-100 blade under fatigue loading. For analysis, machine learning techniques utilised for failure detection of wind turbine blades will be applied, like non-linear Neural Networks, including Auto-Associative Neural Network (AANN) and Radial Basis Function (RBF) networks models. C1 [Dervilis, N.; Antoniadou, I.; Barthorpe, R. J.; Worden, K.] Univ Sheffield, Dept Mech Engn, Dynam Res Grp, Mappin St, Sheffield S1 3JD, S Yorkshire, England. [Farinholt, K. M.; Taylor, S. G.; Park, G.; Farrar, C. R.] Los Alamos Natl Lab, Engn Inst, Los Alamos, NM 87545 USA. [Choi, M.] Chonbuk Natl Univ, Dept Aerosp Engn, Jeonju, South Korea. RP Dervilis, N (reprint author), Univ Sheffield, Dept Mech Engn, Dynam Res Grp, Mappin St, Sheffield S1 3JD, S Yorkshire, England. EM N.Dervilis@sheffield.ac.uk RI Barthorpe, Robert/D-8959-2016; OI Barthorpe, Robert/0000-0002-6645-8482; Farrar, Charles/0000-0001-6533-6996 FU Department of Energy at Los Alamos National Laboratory FX The research was funded by the Department of Energy through the Laboratory Directed Research and Development program at Los Alamos National Laboratory. The authors would also like to acknowledge Scott Hughes and Mike Desmond from the National Renewable Energy Laboratory, and Mark Rumsey and Jon White from the Sandia National Laboratory for their support and guidance on this study. The authors gratefully acknowledge the support of the EU Marie Curie scheme through the Initial Training Network SYS WIND. NR 22 TC 0 Z9 0 U1 0 U2 6 PU TRANS TECH PUBLICATIONS LTD PI DURNTEN-ZURICH PA KREUZSTRASSE 10, 8635 DURNTEN-ZURICH, SWITZERLAND SN 1013-9826 J9 KEY ENG MATER PY 2014 VL 588 BP 166 EP + DI 10.4028/www.scientific.net/KEM.588.166 PG 3 WC Engineering, Civil; Engineering, Mechanical; Materials Science, Multidisciplinary SC Engineering; Materials Science GA BA4SM UT WOS:000336234700019 ER PT S AU Puretzky, AA Geohegan, DB Pannala, S Rouleau, CM AF Puretzky, A. A. Geohegan, D. B. Pannala, S. Rouleau, C. M. BE Geohegan, DB Trager, F Dubowski, JJ TI Exploring growth kinetics of carbon nanotube arrays by in situ optical diagnostics and modeling SO SYNTHESIS AND PHOTONICS OF NANOSCALE MATERIALS XI SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Synthesis and Photonics of Nanoscale Materials XI CY FEB 02-04, 2014 CL San Francisco, CA SP SPIE DE Carbon nanotubes; vertically aligned carbon nanotube arrays; chemical vapor deposition; growth kinetics; in situ diagnostics ID CHEMICAL-VAPOR-DEPOSITION; RAMAN-SPECTROSCOPY; FILAMENT GROWTH; REAL-TIME; NUCLEATION; SCALE; TEMPERATURE; TERMINATION; ACETYLENE; CATALYSTS AB Simple kinetic models of carbon nanotube growth have been able to successfully link together many experimental parameters involved in the growth of carbon nanotubes for practical applications including the prediction of growth rates, terminal lengths, number of walls, activation energies, and their dependences on the growth environment. The implications of recent experiments utilizing in situ monitoring of carbon nanotube growth on our past kinetic model are first reviewed. Then, sub-second pulsed feedstock gas introduction is discussed to explore the nucleation and initial growth of carbon nanotubes in the context of the kinetic model. Moreover, kinetic effects in "pulsed CVD" - using repeated pulsed gas introduction to stop and restart nanotube growth - are explored to understand renucleation, the origin of alignment in nanotube arrays, and incremental growth. Time-resolved reflectivity of the surface is used to remotely understand the kinetics of nucleation and the coordinated growth of arrays. This approach demonstrates that continuous vertically aligned single wall carbon nanotubes can be grown incrementally by pulsed CVD, and that the first exposure of fresh catalyst to feedstock gas is critical to nanotubes site density required for coordinated growth. Aligned nanotube arrays (as short as 60 nm) are shown to nucleate and grow within single, sub-second gas pulses. The multiple-pulse growth experiments (> 100 pulses) show that a high fraction of nanotubes renucleate on subsequent gas pulses. C1 [Puretzky, A. A.; Geohegan, D. B.; Pannala, S.; Rouleau, C. M.] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. RP Puretzky, AA (reprint author), Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. RI Rouleau, Christopher/Q-2737-2015; Puretzky, Alexander/B-5567-2016; Geohegan, David/D-3599-2013 OI Rouleau, Christopher/0000-0002-5488-3537; Puretzky, Alexander/0000-0002-9996-4429; Geohegan, David/0000-0003-0273-3139 NR 49 TC 0 Z9 0 U1 1 U2 11 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9882-3 J9 PROC SPIE PY 2014 VL 8969 AR 896904 DI 10.1117/12.2045949 PG 12 WC Nanoscience & Nanotechnology; Optics; Physics, Applied SC Science & Technology - Other Topics; Optics; Physics GA BA4QD UT WOS:000336124900002 ER PT S AU Rouleau, CM Tian, M Puretzky, AA Mahjouri-Samani, M Duscher, G Geohegan, DB AF Rouleau, C. M. Tian, M. Puretzky, A. A. Mahjouri-Samani, M. Duscher, G. Geohegan, D. B. BE Geohegan, DB Trager, F Dubowski, JJ TI Catalytic nanoparticles for carbon nanotube growth synthesized by through thin film femtosecond laser ablation SO SYNTHESIS AND PHOTONICS OF NANOSCALE MATERIALS XI SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Synthesis and Photonics of Nanoscale Materials XI CY FEB 02-04, 2014 CL San Francisco, CA SP SPIE DE femtosecond laser vaporization; through thin film laser ablation; nanoparticle synthesis; nanotube growth ID ARRAYS AB The synthesis of metal nanoparticles by femtosecond laser vaporization of nm-thickness metal films is explored with the goal of comparing the salient features of femtosecond-based through thin film laser ablation (TTFA) to that of ns TTFA, and testing the feasibility of direct synthesis of clean nanoparticle alloys to explore the synthesis of carbon nanotubes by chemical vapor deposition. It is demonstrated that evaporated metal films are cleanly removed from quartz substrates using the technique, producing a highly forward-directed plume of nanoparticles (angle of divergence of similar to 2.5 degrees) which were cleanly deposited onto different supports for analysis. TEM showed the nanoparticles were spherical with diameters that ranged from a few nm to hundreds of nm in a bimodal fashion. Unlike ns-TTFA, it was found that raising the pressure had no effect on the intensity of the smaller mode within the distribution, suggesting that nanoparticle formation by gas phase condensation was not at play under the present conditions. Close examination of size distributions from a 20 and 10nm Pt film revealed an 80nm downshift in the position of the large mode within the distribution, suggesting film thickness may provide a route to controlling the modal distribution of nanoparticles produced by this method. Lastly, particles sourced by a Fe/Mo bilayer film were found to be effective in growing single wall carbon nanotubes by atmospheric chemical vapor deposition, indicating sufficiently small and catalytically active particles were produced. C1 [Rouleau, C. M.; Puretzky, A. A.; Mahjouri-Samani, M.; Geohegan, D. B.] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. [Tian, M.; Duscher, G.] Univ Tennessee Knoxville, Dept Mat Sci & Engn, Knoxville, TN 37996 USA. RP Rouleau, CM (reprint author), Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. EM rouleaucm@ornl.gov RI Mahjouri-Samani, Masoud/Q-2239-2015; Rouleau, Christopher/Q-2737-2015; Puretzky, Alexander/B-5567-2016; Duscher, Gerd/G-1730-2014; Geohegan, David/D-3599-2013 OI Mahjouri-Samani, Masoud/0000-0002-6080-7450; Rouleau, Christopher/0000-0002-5488-3537; Puretzky, Alexander/0000-0002-9996-4429; Duscher, Gerd/0000-0002-2039-548X; Geohegan, David/0000-0003-0273-3139 FU Materials Sciences and Engineering MSE Division; Office of Basic Energy Sciences; U. S. Department of Energy; Scientific User Facilities SUF Division FX This work was sponsored by the Materials Sciences and Engineering ( MSE) Division, Office of Basic Energy Sciences, U. S. Department of Energy. A portion of this research was conducted at the Center for Nanophase Materials Sciences user facility, which is sponsored at Oak Ridge National Laboratory by the Scientific User Facilities ( SUF) Division, U. S.Department of Energy. NR 11 TC 1 Z9 1 U1 2 U2 7 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9882-3 J9 PROC SPIE PY 2014 VL 8969 AR UNSP 896907 DI 10.1117/12.2045951 PG 6 WC Nanoscience & Nanotechnology; Optics; Physics, Applied SC Science & Technology - Other Topics; Optics; Physics GA BA4QD UT WOS:000336124900004 ER PT S AU Albrecht, AR Seletskiy, DV Wang, Y Cederberg, JG Sheik-Bahae, M AF Albrecht, Alexander R. Seletskiy, Denis V. Wang, Yi Cederberg, Jeffrey G. Sheik-Bahae, Mansoor BE Moloney, JV TI Exploring ultrafast negative Kerr Effect for self-mode-locking vertical external-cavity surface-emitting lasers SO VERTICAL EXTERNAL CAVITY SURFACE EMITTING LASERS (VECSELS) IV SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Vertical External Cavity Surface Emitting Lasers (VECSELs) IV CY FEB 02-04, 2014 CL San Francisco, CA SP SPIE, Coherent Inc DE Semiconductor lasers; mode-locked lasers; Kerr effect ID SEMICONDUCTOR DISK LASER; HIGH-POWER; NONLINEAR REFRACTION; GENERATION; AMPLIFIERS; INDEX; DISPERSION; DYNAMICS; ALGAAS; PULSES AB Quasi-stable self-mode-locking of an InGaAs vertical external-cavity surface-emitting laser (VECSEL) emitting around 1020 nm has been observed, resulting in 500 fs pulses at a repetition rate of 1 GHz. The mechanism is attributed to negative ultrafast Kerr lensing in the semiconductor gain structure. Our calculations show that a mode narrowing on the order of 0.5% can be obtained at the concave cavity end-mirror or at the gain medium. This is consistent with experimental observations, as mode-locking can be achieved by placing a (hard) aperture before the concave cavity end mirror inside the VECSEL cavity, or by the soft aperture created by changing the pump spot size in relation to the lasing mode on the gain chip. The pulse train generated by the VECSEL has been analyzed by a fast InGaAs photo diode and oscilloscope, RF spectrum analyzer, and second harmonic intensity autocorrelation. The effect of dispersion on pulse width has been studied, hinting at soliton-like pulse formation. C1 [Albrecht, Alexander R.; Wang, Yi; Sheik-Bahae, Mansoor] Univ New Mexico, Dept Phys & Astron, 1919 Lomas Blvd NE, Albuquerque, NM 87131 USA. [Seletskiy, Denis V.] Univ Konstanz, Depat Phys & Ctr Appl Photon, D-78464 Constance, Germany. [Cederberg, Jeffrey G.] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Albrecht, AR (reprint author), Univ New Mexico, Dept Phys & Astron, 1919 Lomas Blvd NE, Albuquerque, NM 87131 USA. EM alex2@unm.edu FU US Air Force Research Laboratory ( AFRL); National Science Foundation [1160764]; Sandia's Laboratory Directed Research and Development Office; Sandia Corporation [DE-AC04-94AL85000] FX Work at UNM was partially supported by grants from US Air Force Research Laboratory ( AFRL). DVS acknowledges support by the National Science Foundation under Grant No. 1160764. VECSEL growth was supported by Sandia's Laboratory Directed Research and Development Office. 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 30 TC 1 Z9 1 U1 1 U2 5 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9879-3 J9 PROC SPIE PY 2014 VL 8966 AR UNSP 896604 DI 10.1117/12.2040072 PG 9 WC Engineering, Electrical & Electronic; Optics; Physics, Applied SC Engineering; Optics; Physics GA BA4NU UT WOS:000336041100002 ER PT S AU Fuchs, MR Sweet, RM Berman, LE Hendrickson, WA Chubar, O Canestrari, N Idir, M Yang, L Schneider, DK AF Fuchs, M. R. Sweet, R. M. Berman, L. E. Hendrickson, W. A. Chubar, O. Canestrari, N. Idir, M. Yang, L. Schneider, D. K. BE Arp, U Reversz, P Williams, GP TI NSLS-II Biomedical Beamlines for Macromolecular Crystallography, FMX and AMX, and for X-ray Scattering, LIX: Current Developments SO 17TH PAN-AMERICAN SYNCHROTRON RADIATION INSTRUMENTATION CONFERENCE SRI2013 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 17th Pan-American Synchrotron Radiation Instrumentation Conference (SRI) CY JUN 19-21, 2013 CL Natl Inst Stand & Technol, Synchrotron Ultraviolet Radiat Facil, Gaithersburg, MD SP Cornell Univ Cornell High Energy Synchrotron Source, Thomas Jefferson Natl Accelerator Facil HO Natl Inst Stand & Technol, Synchrotron Ultraviolet Radiat Facil ID SYNCHROTRON; OPTICS AB We present the current status of development of the two macromolecular crystallography (MX) beamlines, FMX and AMX, and the X-ray scattering beamline LIX, at the National Synchrotron Light Source-II (NSLS-II) [1]. Together, FMX and AMX will cover a broad range of use cases from serial crystallography on micron sized crystals, to very large unit cell complexes, to rapid sample screening, e. g. for the always-hard-to-grow membrane proteins and for ligand binding studies. The LIX beamline will support a variety of X-ray scattering measurements for studies on proteins in solution, lipid membranes and biological tissues. We have performed Synchrotron Radiation Workshop (SRW) [2] and Shadow[3] simulations to help select optimal methods to modify the size of the beam easily and smoothly at both FMX and AMX. The very low emittance of the NSLS-II storage ring and the resulting low divergence of the X-ray beam, as well as the long optical path lengths in the photon delivery systems lead to stringent requirements e. g. for vibrational stability and mirror quality. We discuss beamline design considerations addressing these challenges, such as combining mirror optics with compound refractive lenses (CRLs). C1 [Fuchs, M. R.; Sweet, R. M.; Berman, L. E.; Hendrickson, W. A.; Chubar, O.; Canestrari, N.; Idir, M.; Yang, L.; Schneider, D. K.] Brookhaven Natl Lab, Upton, NY 11973 USA. RP Fuchs, MR (reprint author), Brookhaven Natl Lab, Upton, NY 11973 USA. EM mfuchs@bnl.gov NR 6 TC 5 Z9 5 U1 0 U2 4 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 493 AR 012021 DI 10.1088/1742-6596/493/1/012021 PG 4 WC Instruments & Instrumentation; Optics; Physics, Applied SC Instruments & Instrumentation; Optics; Physics GA BA4LZ UT WOS:000336000800021 ER PT S AU Gofron, KJ Lauer, K Nazaretski, E Yan, H Kalbfleisch, S Greer, A Dalesio, B Chu, YS AF Gofron, K. J. Lauer, K. Nazaretski, E. Yan, H. Kalbfleisch, S. Greer, A. Dalesio, B. Chu, Y. S. BE Arp, U Reversz, P Williams, GP TI Piezo control for 1 nm spatial resolution synchrotron X-ray microscopy SO 17TH PAN-AMERICAN SYNCHROTRON RADIATION INSTRUMENTATION CONFERENCE SRI2013 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 17th Pan-American Synchrotron Radiation Instrumentation Conference (SRI) CY JUN 19-21, 2013 CL Natl Inst Stand & Technol, Synchrotron Ultraviolet Radiat Facil, Gaithersburg, MD SP Cornell Univ Cornell High Energy Synchrotron Source, Thomas Jefferson Natl Accelerator Facil HO Natl Inst Stand & Technol, Synchrotron Ultraviolet Radiat Facil ID MULTILAYER LAUE LENSES AB A novel motion control system which utilizes the Power PMAC controller from Delta Tau Data Systems Inc., has been developed for positioning with 1 nm spatial resolution. Present work is a significant step forward towards commissioning of the X-ray microscope which will operate at the Hard X-ray Nanoprobe (HXN) beamline at the NSLS-II. The control system is capable of performing high-speed / high-accuracy on-the-fly scans of the sample with respect to the nano-focusing optics e.g. Multilayer Laue Lenses (MLL) or Fresnel X-ray Zone Plates (ZP) [1]. The Power PMAC controls piezoelectric-based nano-positioning stages using piezo-expansion for short range motion and stick-slip motion for longer travel distances. An EPICS interface to the Power PMAC has been developed allowing for easy integration into a beamline control environment. C1 [Gofron, K. J.; Lauer, K.; Nazaretski, E.; Yan, H.; Kalbfleisch, S.; Dalesio, B.; Chu, Y. S.] Brookhaven Natl Lab, Natl Synchrotron Light Source 2, Upton, NY 11973 USA. [Greer, A.] Observ Sci Ltd, Cambridge CB4 0WX, England. RP Gofron, KJ (reprint author), Brookhaven Natl Lab, Natl Synchrotron Light Source 2, Upton, NY 11973 USA. EM kgofron@bnl.gov FU Department of Energy [DE-AC-02-98CH10886]; Office of Basic Energy Sciences [DE-AC-02-98CH10886] FX Work at Brookhaven was supported by the Department of Energy, Office of Basic Energy Sciences under contract DE-AC-02-98CH10886. We; thank Dennis Kuhne and James Biancarosa for experimental support. We thank Deming Shu at APS for collaborating on developing the HXN MLL microscope. NR 4 TC 2 Z9 3 U1 0 U2 10 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 493 AR UNSP 012026 DI 10.1088/1742-6596/493/1/012026 PG 4 WC Instruments & Instrumentation; Optics; Physics, Applied SC Instruments & Instrumentation; Optics; Physics GA BA4LZ UT WOS:000336000800026 ER PT S AU Huang, R Szebenyi, T Pfeifer, M Woll, A Smilgies, DM Finkelstein, K Dale, D Wang, YX Vila-Comamala, J Gillilan, R Cook, M Bilderback, DH AF Huang, Rong Szebenyi, Thomas Pfeifer, Mark Woll, Arthur Smilgies, Detlef-M. Finkelstein, Kenneth Dale, Darren Wang, Yuxin Vila-Comamala, Joan Gillilan, Richard Cook, Michael Bilderback, Donald H. BE Arp, U Reversz, P Williams, GP TI Application of CHESS single-bounce capillaries at synchrotron beamlines SO 17TH PAN-AMERICAN SYNCHROTRON RADIATION INSTRUMENTATION CONFERENCE SRI2013 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 17th Pan-American Synchrotron Radiation Instrumentation Conference (SRI) CY JUN 19-21, 2013 CL Natl Inst Stand & Technol, Synchrotron Ultraviolet Radiat Facil, Gaithersburg, MD SP Cornell Univ Cornell High Energy Synchrotron Source, Thomas Jefferson Natl Accelerator Facil HO Natl Inst Stand & Technol, Synchrotron Ultraviolet Radiat Facil ID X-RAY-FLUORESCENCE; IN-SITU; XRF; MICROSCOPY AB Single-bounce capillaries are achromatic X-ray focusing optics that can provide efficient and high demagnification focusing with large numerical apertures. Capillary fabrication at CHESS can be customized according to specific application requirements. Exemplary applications are reviewed in this paper, as well as recent progress on condensers for high-resolution transmission X-ray microscopy and small focal size capillaries. C1 [Huang, Rong; Szebenyi, Thomas; Pfeifer, Mark; Woll, Arthur; Smilgies, Detlef-M.; Finkelstein, Kenneth; Dale, Darren; Bilderback, Donald H.] Cornell Univ, Cornell High Energy Synchrotron Source, Ithaca, NY 14853 USA. [Wang, Yuxin; Vila-Comamala, Joan] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. [Gillilan, Richard; Cook, Michael] MacCHESS Macromolecular Diffract facil CHESS, Ithaca, NY 14853 USA. [Bilderback, Donald H.] Cornell Univ, Sch Appl Engn Phys, Ithaca, NY 14853 USA. RP Huang, R (reprint author), Cornell Univ, Cornell High Energy Synchrotron Source, Ithaca, NY 14853 USA. EM rh66@cornell.edu RI ID, BioCAT/D-2459-2012; Vila-Comamala, Joan/E-2106-2017; OI Smilgies, Detlef/0000-0001-9351-581X FU NSF; NIH/NIGMS via NSF [DMR-0936384, DMR-0807731]; NIGMS [GM-103485] FX CHESS is supported by the NSF & NIH/NIGMS via NSF award DMR-0936384 and NSF DMR-0807731, and the MacCHESS resource is supported by NIGMS award GM-103485. NR 18 TC 2 Z9 2 U1 1 U2 8 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 493 AR UNSP 012034 DI 10.1088/1742-6596/493/1/012034 PG 4 WC Instruments & Instrumentation; Optics; Physics, Applied SC Instruments & Instrumentation; Optics; Physics GA BA4LZ UT WOS:000336000800034 ER PT S AU Keister, JW Siddons, DP Kuczewski, A Coburn, DS Beuttenmuller, R Rumaiz, A Cai, YQ AF Keister, J. W. Siddons, D. P. Kuczewski, A. Coburn, D. S. Beuttenmuller, R. Rumaiz, A. Cai, Y. Q. BE Arp, U Reversz, P Williams, GP TI Compact pseudo-2D strip detector system for sub-meV IXS SO 17TH PAN-AMERICAN SYNCHROTRON RADIATION INSTRUMENTATION CONFERENCE SRI2013 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 17th Pan-American Synchrotron Radiation Instrumentation Conference (SRI) CY JUN 19-21, 2013 CL Natl Inst Stand & Technol, Synchrotron Ultraviolet Radiat Facil, Gaithersburg, MD SP Cornell Univ Cornell High Energy Synchrotron Source, Thomas Jefferson Natl Accelerator Facil HO Natl Inst Stand & Technol, Synchrotron Ultraviolet Radiat Facil AB A dual 32 strip sensor array is realized for use at the IXS (inelastic x-ray scattering) beamline of NSLS-II. By making use of established controls methods and sensor device recipes, our new geometry is realized quickly and at minimal cost. The detector geometry is chosen to match the output of a multi-element high-resolution energy analyzer, while the pulse thresholding is optimized for an ultra-low noise floor at a pass energy of 9.13 keV. Detector subsystems and integration are described, including sensor geometry and silicon device processing, cooling and thermal readback, bias and threshold optimizations, readout ASIC and controls, vacuum enclosure and x-ray window, mounting and positioning, and assembly procedure and testing. C1 [Keister, J. W.; Siddons, D. P.; Kuczewski, A.; Coburn, D. S.; Rumaiz, A.; Cai, Y. Q.] Brookhaven Natl Lab, Photon Sci Directorate, Upton, NY 11973 USA. [Beuttenmuller, R.] Brookhaven Natl Lab, Instrumentat Div, Upton, NY 11973 USA. RP Keister, JW (reprint author), Brookhaven Natl Lab, Photon Sci Directorate, Upton, NY 11973 USA. EM jkeister@bnl.gov RI Cai, Yong/C-5036-2008 OI Cai, Yong/0000-0002-9957-6426 FU U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DEAC02-98CH10886] FX The authors wish to thank L. Reffi and D. Levy for detailed design and fabrication of the Tagma mechanical components, and D. Pinelli and D. Poshka for electronics assembly. 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. DEAC02-98CH10886. NR 5 TC 0 Z9 0 U1 0 U2 2 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 493 AR UNSP 012015 DI 10.1088/1742-6596/493/1/012015 PG 4 WC Instruments & Instrumentation; Optics; Physics, Applied SC Instruments & Instrumentation; Optics; Physics GA BA4LZ UT WOS:000336000800015 ER PT S AU Kujala, N Erdmann, M Goetze, K Sullivan, J Huang, XR Macrander, A AF Kujala, Naresh Erdmann, Mark Goetze, Kurt Sullivan, Joseph Huang, Xianrong Macrander, Albert BE Arp, U Reversz, P Williams, GP TI A fast white-beam shutter for hard x-ray topography at beamline 1-BM of the Advanced Photon Source SO 17TH PAN-AMERICAN SYNCHROTRON RADIATION INSTRUMENTATION CONFERENCE SRI2013 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 17th Pan-American Synchrotron Radiation Instrumentation Conference (SRI) CY JUN 19-21, 2013 CL Natl Inst Stand & Technol, Synchrotron Ultraviolet Radiat Facil, Gaithersburg, MD SP Cornell Univ Cornell High Energy Synchrotron Source, Thomas Jefferson Natl Accelerator Facil HO Natl Inst Stand & Technol, Synchrotron Ultraviolet Radiat Facil AB Beamline 1-BM at the Advanced Photon Source (APS) delivers a white beam from a bending magnet with very intense x-ray photon flux. One important application of this beamline is white-beam x-ray topography imaging for crystal-based x-ray optics development and for industrial characterization of single crystals and epitaxial materials. Due to the intense photon flux from the third-generation synchrotron source of the APS, the exposure time of the imaging process should be accurately controlled down to the millisecond level. For this purpose we have designed and implemented a fast shutter that is vacuum compatible to 10(-8) torr. The aperture is a copper block with a 70 mm horizontal and 5 mm vertical opening and is water cooled. The aperture is moved vertically up and down by means of a linear voice-coil actuator. The aperture's position is controlled using encoder feedback in a servo loop running on an industrial motion controller. A shutter opening response time of 32 milliseconds was measured. In this paper, we describe the shutter mechanics and its associated electronics installed at the 1-BM, and we report example white-beam topographs of diamond type IIa crystals. C1 [Kujala, Naresh; Erdmann, Mark; Goetze, Kurt; Sullivan, Joseph; Huang, Xianrong; Macrander, Albert] Argonne Natl Lab, Adv Photon Source, Lemont, IL 60439 USA. RP Kujala, N (reprint author), Argonne Natl Lab, Adv Photon Source, Lemont, IL 60439 USA. EM kujala@aps.anl.gov NR 6 TC 2 Z9 2 U1 1 U2 5 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 493 AR 012007 DI 10.1088/1742-6596/493/1/012007 PG 4 WC Instruments & Instrumentation; Optics; Physics, Applied SC Instruments & Instrumentation; Optics; Physics GA BA4LZ UT WOS:000336000800007 ER PT S AU Liu, ZP Rosenbaum, G Navrotski, G AF Liu, Zunping Rosenbaum, Gerd Navrotski, Gary BE Arp, U Reversz, P Williams, GP TI Performance Prediction for a Hockey-Puck Silicon Crystal Monochromator at the Advanced Photon Source SO 17TH PAN-AMERICAN SYNCHROTRON RADIATION INSTRUMENTATION CONFERENCE SRI2013 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 17th Pan-American Synchrotron Radiation Instrumentation Conference (SRI) CY JUN 19-21, 2013 CL Natl Inst Stand & Technol, Synchrotron Ultraviolet Radiat Facil, Gaithersburg, MD SP Cornell Univ Cornell High Energy Synchrotron Source, Thomas Jefferson Natl Accelerator Facil HO Natl Inst Stand & Technol, Synchrotron Ultraviolet Radiat Facil ID HEAT LOADS; SYNCHROTRON AB One of the Key Performance Parameters of the upgrade of the Advanced Photon Source (APS) is the increase of the storage ring current from 100 to 150 mA. In order to anticipate the impact of this increased heat load on the X-ray optics of the beamlines, the APS has implemented a systematic review, by means of finite element analysis and computational fluid dynamics, of the thermal performance of the different types of monochromators installed at the highest-heat-load insertion device beamlines. We present here simulations of the performance of a directly liquid nitrogen-cooled silicon crystal, the hockey-puck design. Calculations of the temperature and slope error at multiple ring currents under multiple operational conditions, including the influence of power, cooling, and diffraction surface thickness are included. C1 [Liu, Zunping; Navrotski, Gary] Argonne Natl Lab, Adv Photon Source, 9700 S Cass Ave, Lemont, IL 60439 USA. [Rosenbaum, Gerd] Univ Georgia, Dept Biochem, Argonne Natl Lab, Struct Biol Ctr, Lemont, IL 60439 USA. RP Liu, ZP (reprint author), Argonne Natl Lab, Adv Photon Source, 9700 S Cass Ave, Lemont, IL 60439 USA. EM zpliu@anl.gov FU U.S. Department of Energy, Office of Science and Office of Biological and Environmental Research by Argonne National Laboratory [DE-AC02-06CH11357] FX The authors thank Mati Meron for utilizing his code SRUFF and Catherine Eyberger for edit. The Advanced Photon Source and the Structural Biology Center at Sector 19 are Office of Science User Facilities operated for the U.S. Department of Energy, Office of Science and Office of Biological and Environmental Research by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. NR 9 TC 2 Z9 2 U1 1 U2 3 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 493 AR UNSP 012009 DI 10.1088/1742-6596/493/1/012009 PG 4 WC Instruments & Instrumentation; Optics; Physics, Applied SC Instruments & Instrumentation; Optics; Physics GA BA4LZ UT WOS:000336000800009 ER PT S AU Madden, T Baldwin, J Von Dreele, R Suchomel, M Toby, BH AF Madden, T. Baldwin, J. Von Dreele, R. Suchomel, M. Toby, B. H. BE Arp, U Reversz, P Williams, GP TI Scanning CCD Detector for X-ray Powder Diffraction SO 17TH PAN-AMERICAN SYNCHROTRON RADIATION INSTRUMENTATION CONFERENCE SRI2013 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 17th Pan-American Synchrotron Radiation Instrumentation Conference (SRI) CY JUN 19-21, 2013 CL Natl Inst Stand & Technol, Synchrotron Ultraviolet Radiat Facil, Gaithersburg, MD SP Cornell Univ Cornell High Energy Synchrotron Source, Thomas Jefferson Natl Accelerator Facil HO Natl Inst Stand & Technol, Synchrotron Ultraviolet Radiat Facil ID LIGHT-SOURCE AB We discuss the design, fabrication and use of a custom CCD detector for x-ray powder diffraction measurements. The detector is mounted on a diffractometer arm, where line-by-line readout of the CCD is coupled to continuous motion of the arm. As the arm moves, the data from the CCD detector are accumulated and can be viewed as if it were a "film strip" with partial powder diffraction rings. Because of the unique design of the camera, both high-resolution and rapid measurements can be performed. Powder diffraction patterns are collected with speeds of a few minutes, or less, with many of the advantages of large area position-sensitive detectors, for example amorphous silicon flat panels, such as high sensitivity, direct evidence of grainy samples and freedom from low-angle asymmetry, but with resolution better than linear position-sensitive detectors and nearly as good as the ultimate in resolution, analyser-crystal detection [2,3]. C1 [Madden, T.; Baldwin, J.; Von Dreele, R.; Suchomel, M.; Toby, B. H.] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. RP Madden, T (reprint author), Argonne Natl Lab, Adv Photon Source, 9700 S Cass Ave, Argonne, IL 60439 USA. EM tmadden@aps.anl.gov RI Toby, Brian/F-3176-2013; Suchomel, Matthew/C-5491-2015; OI Toby, Brian/0000-0001-8793-8285; SUCHOMEL, Matthew/0000-0002-9500-5079 NR 5 TC 1 Z9 1 U1 0 U2 4 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 493 AR 012016 DI 10.1088/1742-6596/493/1/012016 PG 4 WC Instruments & Instrumentation; Optics; Physics, Applied SC Instruments & Instrumentation; Optics; Physics GA BA4LZ UT WOS:000336000800016 ER PT S AU Madden, T Baldwin, J AF Madden, T. Baldwin, J. BE Arp, U Reversz, P Williams, GP TI 50 MHz Voltage-to-Frequency Converter SO 17TH PAN-AMERICAN SYNCHROTRON RADIATION INSTRUMENTATION CONFERENCE SRI2013 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 17th Pan-American Synchrotron Radiation Instrumentation Conference (SRI) CY JUN 19-21, 2013 CL Natl Inst Stand & Technol, Synchrotron Ultraviolet Radiat Facil, Gaithersburg, MD SP Cornell Univ Cornell High Energy Synchrotron Source, Thomas Jefferson Natl Accelerator Facil HO Natl Inst Stand & Technol, Synchrotron Ultraviolet Radiat Facil AB The Voltage-to-Frequency Converter (V2F) is an instrument commonly used in synchrotron beam line experiments for converting a slowly varying voltage signal representing x-ray flux to a high frequency pulse train, with each pulse representing a packet of x-ray energy. The pulses are commonly integrated with a digital counter to calculate total x-ray energy incident on a sample during an exposure. As x-ray experiment data is taken faster and faster and exposure times shrink, V2F frequencies must necessarily increase to preserve precision in measuring total x-ray energy. The APS Detector Group have designed and built two custom 50MHz V2F instruments for APS beam line experiments. The instruments are designed according to the Nuclear Instrument Module (NIM) standard and respectively reside at APS Sector 12-BM, and in the APS Detector Pool [1]. C1 [Madden, T.; Baldwin, J.] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. RP Madden, T (reprint author), Argonne Natl Lab, Adv Photon Source, 9700 S Cass Ave, Argonne, IL 60439 USA. EM tmadden@aps.anl.gov NR 2 TC 0 Z9 0 U1 0 U2 0 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 493 AR 012008 DI 10.1088/1742-6596/493/1/012008 PG 4 WC Instruments & Instrumentation; Optics; Physics, Applied SC Instruments & Instrumentation; Optics; Physics GA BA4LZ UT WOS:000336000800008 ER PT S AU Marton, Z Nagarkar, VV Miller, SR Brecher, C Bhandari, HB Kenesei, P Ross, SK Almer, JD Singh, B AF Marton, Z. Nagarkar, Vivek V. Miller, Stuart R. Brecher, Charles Bhandari, Harish B. Kenesei, Peter Ross, Stephen K. Almer, Jonathan D. Singh, Bipin BE Arp, U Reversz, P Williams, GP TI Novel High Efficiency Microcolumnar LuI3:Ce for Hard X-ray Imaging SO 17TH PAN-AMERICAN SYNCHROTRON RADIATION INSTRUMENTATION CONFERENCE SRI2013 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 17th Pan-American Synchrotron Radiation Instrumentation Conference (SRI) CY JUN 19-21, 2013 CL Natl Inst Stand & Technol, Synchrotron Ultraviolet Radiat Facil, Gaithersburg, MD SP Cornell Univ Cornell High Energy Synchrotron Source, Thomas Jefferson Natl Accelerator Facil HO Natl Inst Stand & Technol, Synchrotron Ultraviolet Radiat Facil ID DETECTOR AB We have developed a structured scintillator using a vacuum deposition technique that is suitable for manufacturing large area scintillators in a microcolumnar form. While providing high absorption efficiency, it also allows great temporal and spatial resolution X-ray imaging. Microcolumnar films of extremely fast and bright cerium-doped lutetium iodide (LuI3:Ce) scintillator were synthesized. It has high density (similar to 5.6 g/cm(3)), high effective atomic number (59.7), bright green emission (540 nm range, well matched to commercial optics and CCD sensors), light yield exceeding 115,000 ph/MeV, and rapid, afterglow-free decay (similar to 28 ns). This new scintillator could resolve the 153 ns bunch structure of the Advanced Photon Source (APS) at Argonne National Laboratory (ANL). Due to the fast, afterglow-free decay, and high efficiency of LuI3:Ce, during the experiments performed at the 1-ID hard X-ray beamline at the APS, single 65 keV X-ray photons could be resolved with high signal-to-noise ratio and with temporal resolution better than 20ns. In the future, it will enable a wide range of hard X-ray (20 keV to 100 keV) imaging and/or high frame-rate applications such as dynamic studies of the structural and electrochemical properties of batteries using microtomographic X-ray imaging, internal corrosion in fuel cells, and time-resolved muscle diffraction experiments. C1 [Marton, Z.; Nagarkar, Vivek V.; Miller, Stuart R.; Brecher, Charles; Bhandari, Harish B.; Singh, Bipin] Radiat Monitoring Dev Inc, Watertown, MA 02472 USA. [Kenesei, Peter; Ross, Stephen K.; Almer, Jonathan D.] Argonne Natl Lab, X ray Sci Div, Adv Photon Source, Argonne, IL 60439 USA. RP Marton, Z (reprint author), Radiat Monitoring Dev Inc, Watertown, MA 02472 USA. FU US Department of Energy [DE-SC0007549]; US Department of Energy, Basic Energy Sciences, Office of Science [W-31-109-ENG-38]; U.S. DOE [DEAC02-06CH11357] FX We thank Dr. Steve K. Ross and Dr. Peter Kenesei and Dr. Jonathan D. Almer at Argonne National Laboratory for carrying out hard X-ray imaging experiments at the 1-ID beamline of APS as well as for valuable discussions. This work was supported in part by the US Department of Energy under Grant DE-SC0007549. Use of the APS was supported by the US Department of Energy, Basic Energy Sciences, Office of Science, under Contract No. W-31-109-ENG-38. 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. DEAC02-06CH11357. NR 10 TC 1 Z9 1 U1 2 U2 9 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 493 AR UNSP 012017 DI 10.1088/1742-6596/493/1/012017 PG 4 WC Instruments & Instrumentation; Optics; Physics, Applied SC Instruments & Instrumentation; Optics; Physics GA BA4LZ UT WOS:000336000800017 ER PT S AU Pardini, T Poyneer, LA McCarville, TJ Macintosh, B Bauman, B Pivavaroff, MJ AF Pardini, T. Poyneer, L. A. McCarville, T. J. Macintosh, B. Bauman, B. Pivavaroff, M. J. BE Arp, U Reversz, P Williams, GP TI The adaptive x-ray optic project at the Lawrence Livermore National Laboratory SO 17TH PAN-AMERICAN SYNCHROTRON RADIATION INSTRUMENTATION CONFERENCE SRI2013 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 17th Pan-American Synchrotron Radiation Instrumentation Conference (SRI) CY JUN 19-21, 2013 CL Natl Inst Stand & Technol, Synchrotron Ultraviolet Radiat Facil, Gaithersburg, MD SP Cornell Univ Cornell High Energy Synchrotron Source, Thomas Jefferson Natl Accelerator Facil HO Natl Inst Stand & Technol, Synchrotron Ultraviolet Radiat Facil ID FREE-ELECTRON LASER AB Deformable mirrors (DMs) have been successfully used in astronomical adaptive optics at near-infrared wavelengths, greatly reducing atmospheric-induced aberrations [1]. Extending this capability to the soft and hard x-ray regime is now required in order to take full advantage of the beam quality characteristic of new generation synchrotron facilities and X-ray Free Electron Lasers (XFELs). Achieving this goal challenges both current mirror manufacturing techniques and physical optics modeling. The Lawrence Livermore National Laboratory (LLNL) is currently developing an x-ray DM to correct wavefront aberrations introduced along the beam path of a typical x-ray beam-line [2]. To model the expected performance of such a mirror, we have also developed simulation code based on the wavefront propagation library of functions PROPER [3]. Here we present the current status of the project, including metrology done on the mirror substrate. Additionally we report on results from our wavefront simulation code, which have proven very useful in predicting technical aspects of mirror deployment at a typical x-ray facility. C1 [Pardini, T.; Poyneer, L. A.; McCarville, T. J.; Macintosh, B.; Bauman, B.; Pivavaroff, M. J.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. RP Pardini, T (reprint author), Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. EM pardini2@llnl.gov RI Pivovaroff, Michael/M-7998-2014 OI Pivovaroff, Michael/0000-0001-6780-6816 NR 8 TC 0 Z9 0 U1 1 U2 7 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 493 AR 012022 DI 10.1088/1742-6596/493/1/012022 PG 4 WC Instruments & Instrumentation; Optics; Physics, Applied SC Instruments & Instrumentation; Optics; Physics GA BA4LZ UT WOS:000336000800022 ER PT S AU Schmidt, O DeBartolo, J Kurtz, C Lee, B Seifert, S Winans, R Zuo, X AF Schmidt, O. DeBartolo, J. Kurtz, C. Lee, B. Seifert, S. Winans, R. Zuo, X. BE Arp, U Reversz, P Williams, GP TI Variable q-range x-ray scattering chamber for chemical and materials science at the Advanced Photon Source SO 17TH PAN-AMERICAN SYNCHROTRON RADIATION INSTRUMENTATION CONFERENCE SRI2013 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 17th Pan-American Synchrotron Radiation Instrumentation Conference (SRI) CY JUN 19-21, 2013 CL Natl Inst Stand & Technol, Synchrotron Ultraviolet Radiat Facil, Gaithersburg, MD SP Cornell Univ Cornell High Energy Synchrotron Source, Thomas Jefferson Natl Accelerator Facil HO Natl Inst Stand & Technol, Synchrotron Ultraviolet Radiat Facil AB We present here the design of a novel variable q-range x-ray scattering instrument recently installed at Sector 12 of the Advanced Photon Source. This device provides automated, computer-controlled q-range changes for x-ray scattering experiments by varying the sample-to-detector distance within a large vacuum chamber. Eliminating the need to vent the system when changing camera lengths allows for quick and efficient change-overs between experimental setups. The detector cannot operate in a vacuum environment; therefore it is housed within an air chamber open to atmospheric pressure. A large carbon window isolates the detector from vacuum while allowing high x-ray transmission. An array of motorized beam stops mounted directly upstream of the window protects the detector from the direct x-ray beam for various types of scattering experiments. A smaller detector protrudes into the lower front section for simultaneous wide-angle x-ray scattering data collection. A fully automated support structure aligns the vacuum chamber to the x-ray trajectory. C1 [Schmidt, O.] Argonne Natl Lab, Engn Support Div, 9700 S Cass Ave, Argonne, IL 60439 USA. [DeBartolo, J.; Kurtz, C.; Lee, B.; Seifert, S.; Winans, R.; Zuo, X.] Argonne Natl Lab, X Ray Sci Div, Argonne, IL USA. RP Schmidt, O (reprint author), Argonne Natl Lab, Engn Support Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM oschmidt@aps.anl.gov NR 2 TC 0 Z9 0 U1 0 U2 2 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 493 AR UNSP 012010 DI 10.1088/1742-6596/493/1/012010 PG 4 WC Instruments & Instrumentation; Optics; Physics, Applied SC Instruments & Instrumentation; Optics; Physics GA BA4LZ UT WOS:000336000800010 ER PT S AU Shaban, EH Siddons, DP Seifu, D AF Shaban, E. H. Siddons, D. P. Seifu, D. BE Arp, U Reversz, P Williams, GP TI 10 cm x 10 cm Single Gas Electron Multiplier (GEM) X-ray Fluorescence Detector for Dilute Elements SO 17TH PAN-AMERICAN SYNCHROTRON RADIATION INSTRUMENTATION CONFERENCE SRI2013 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 17th Pan-American Synchrotron Radiation Instrumentation Conference (SRI) CY JUN 19-21, 2013 CL Natl Inst Stand & Technol, Synchrotron Ultraviolet Radiat Facil, Gaithersburg, MD SP Cornell Univ Cornell High Energy Synchrotron Source, Thomas Jefferson Natl Accelerator Facil HO Natl Inst Stand & Technol, Synchrotron Ultraviolet Radiat Facil AB We have built and tested a 10 cm x 10 cm single Gas Electron Multiplier (GEM) X-ray detector to probe dilute amounts of Fe in a prepared sample. The detector uses Argon/Carbon Dioxide (75/25) gas mixture flowing at a slow rate through a leak proof Plexi-glass enclosure held together by O-rings and screws. The Fluorescence X-ray emitted by the element under test is directed through a Mylar window into the drift region of the detector where abundant gas is flowing. The ionized electrons are separated, drifted into the high electric field of the GEM, and multiplied by impact ionization. The amplified negatively charged electrons are collected and further amplified by a Keithley amplifier to probe the absorption edge of the element under test using X-ray absorption spectroscopy technique. The results show that the GEM detector provided good results with less noise as compared with a Silicon drift detector (SDD). C1 [Shaban, E. H.] Southern Univ, Baton Rouge, LA 70813 USA. [Siddons, D. P.] Brookhaven Natl Lab, NSLS, Upton, NY 11973 USA. [Seifu, D.] Morgan State Univ, Dept Phys, Baltimore, MD 21251 USA. RP Shaban, EH (reprint author), Southern Univ, Baton Rouge, LA 70813 USA. EM elhag_shaban@subr.edu FU NSF [DMR-1126444]; LEQSF-EPS [2012-PFUND-290]; NSLS; Instrumentation Department at Brookhaven National Lab, NSLS workshop, and Morgan State University FX This work is supported by NSF award DMR-1126444, and partly by LEQSF-EPS (2012)-PFUND-290. This work was done in collaboration with NSLS, the Instrumentation Department at Brookhaven National Lab, NSLS workshop, and Morgan State University. We thank the students Goings, Leonard, Driggs, Berthe, Bamagu, and Carriere for the help. We thank CAMD/LSU for providing the beamtime at DCM hutch, Dr. Roy, Merchant, and Jiles for the help & assistance, and 3M Corporation for providing the GEMs. NR 3 TC 0 Z9 0 U1 0 U2 0 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 493 AR UNSP 012018 DI 10.1088/1742-6596/493/1/012018 PG 4 WC Instruments & Instrumentation; Optics; Physics, Applied SC Instruments & Instrumentation; Optics; Physics GA BA4LZ UT WOS:000336000800018 ER PT S AU Shu, D Kalbfleisch, S Kearney, S Anton, J Chu, YS AF Shu, D. Kalbfleisch, S. Kearney, S. Anton, J. Chu, Y. S. BE Arp, U Reversz, P Williams, GP TI Optomechanical design of a high-precision detector robot arm system for x-ray nano-diffraction with x-ray nanoprobe SO 17TH PAN-AMERICAN SYNCHROTRON RADIATION INSTRUMENTATION CONFERENCE SRI2013 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 17th Pan-American Synchrotron Radiation Instrumentation Conference (SRI) CY JUN 19-21, 2013 CL Natl Inst Stand & Technol, Synchrotron Ultraviolet Radiat Facil, Gaithersburg, MD SP Cornell Univ Cornell High Energy Synchrotron Source, Thomas Jefferson Natl Accelerator Facil HO Natl Inst Stand & Technol, Synchrotron Ultraviolet Radiat Facil AB Collaboration between Argonne National Laboratory and Brookhaven National Laboratory has created a design for the high-precision detector robot arm system that will be used in the x-ray nano-diffraction experimental station at the Hard X-ray Nanoprobe (HXN) beamline for the NSLS-II project. The robot arm system is designed for positioning and manipulating an x-ray detector in three-dimensional space for nano-diffraction data acquisition with the HXN x-ray microscope. It consists of the following major component groups: a granite base with air-bearing support, a 2-D horizontal base stage, a vertical axis goniometer, a 2-D vertical plane robot arm, a 3-D fast scanning stages group, and a 2-D x-ray pixel detector. The design specifications and unique optomechanical structure of this novel high-precision detector robot arm system will be presented in this paper. C1 [Shu, D.; Kearney, S.; Anton, J.] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. [Kalbfleisch, S.; Chu, Y. S.] Brookhaven Natl Lab, Natl Synchrotron Light Source, Upton, NY 11973 USA. [Kearney, S.; Anton, J.] Univ Illinois, Chicago, IL 60607 USA. RP Shu, D (reprint author), Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. EM shu@aps.anl.gov FU U.S. Department of Energy, Office of Science [DE-AC02-06CH11357]; [DE-AC02-98CH10886] FX The work at Argonne is supported by the U.S. Department of Energy, Office of Science, under Contract No. DE-AC02-06CH11357. The work at Brookhaven is supported by the U.S. Department of Energy, Office of Science, under Contract No. DE-AC02-98CH10886. NR 3 TC 0 Z9 0 U1 0 U2 3 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 493 AR UNSP 012027 DI 10.1088/1742-6596/493/1/012027 PG 4 WC Instruments & Instrumentation; Optics; Physics, Applied SC Instruments & Instrumentation; Optics; Physics GA BA4LZ UT WOS:000336000800027 ER PT S AU Steier, C Madur, A Bailey, B Berg, K Biocca, A Black, A Casey, P Colomb, D Gunion, B Li, N Marks, S Nishimura, H Pappas, C Peterman, K Portsmann, G Prestemon, S Rawlins, A Robin, D Rossi, S Scarvie, T Schlueter, R Sun, C Tarawneh, H Wan, W Williams, E Yin, L Zhou, Q Jin, J Zhang, J Cheng, C Wen, Y Wu, J AF Steier, C. Madur, A. Bailey, B. Berg, K. Biocca, A. Black, A. Casey, P. Colomb, D. Gunion, B. Li, N. Marks, S. Nishimura, H. Pappas, C. Peterman, K. Portsmann, G. Prestemon, S. Rawlins, A. Robin, D. Rossi, S. Scarvie, T. Schlueter, R. Sun, C. Tarawneh, H. Wan, W. Williams, E. Yin, L. Zhou, Q. Jin, J. Zhang, J. Cheng, C. Wen, Y. Wu, J. BE Arp, U Reversz, P Williams, GP TI Completion of the Brightness Upgrade of the ALS SO 17TH PAN-AMERICAN SYNCHROTRON RADIATION INSTRUMENTATION CONFERENCE SRI2013 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 17th Pan-American Synchrotron Radiation Instrumentation Conference (SRI) CY JUN 19-21, 2013 CL Natl Inst Stand & Technol, Synchrotron Ultraviolet Radiat Facil, Gaithersburg, MD SP Cornell Univ Cornell High Energy Synchrotron Source, Thomas Jefferson Natl Accelerator Facil HO Natl Inst Stand & Technol, Synchrotron Ultraviolet Radiat Facil AB The Advanced Light Source (ALS) at Berkeley Lab remains one of the brightest sources for soft x-rays worldwide. A multiyear upgrade of the ALS is underway, which includes new and replacement x-ray beamlines, a replacement of many of the original insertion devices and many upgrades to the accelerator. The accelerator upgrade that affects the ALS performance most directly is the ALS brightness upgrade [1], which reduces the horizontal emittance from 6.3 to 2.0 nm (2.5 nm effective). Magnets for this upgrade were installed in late 2012 and early 2013 followed by user operation with the reduced emittance. C1 [Steier, C.; Madur, A.; Bailey, B.; Berg, K.; Biocca, A.; Black, A.; Casey, P.; Colomb, D.; Gunion, B.; Li, N.; Marks, S.; Nishimura, H.; Pappas, C.; Peterman, K.; Portsmann, G.; Prestemon, S.; Rawlins, A.; Robin, D.; Rossi, S.; Scarvie, T.; Schlueter, R.; Sun, C.; Tarawneh, H.; Wan, W.; Williams, E.] LBNL, Berkeley, CA 94720 USA. [Yin, L.; Zhou, Q.; Jin, J.; Zhang, J.; Cheng, C.; Wen, Y.; Wu, J.] SINAP, Shanghai, Peoples R China. RP Steier, C (reprint author), LBNL, Berkeley, CA 94720 USA. EM CSteier@lbl.gov FU U.S. Department of Energy [DE-AC02-05CH11231] 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. NR 7 TC 1 Z9 1 U1 0 U2 3 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 493 AR UNSP 012030 DI 10.1088/1742-6596/493/1/012030 PG 4 WC Instruments & Instrumentation; Optics; Physics, Applied SC Instruments & Instrumentation; Optics; Physics GA BA4LZ UT WOS:000336000800030 ER PT S AU Storns, P Khounsary, A Antimonov, M Dufresne, EM Reininger, R AF Storns, Philip Khounsary, Ali Antimonov, Mikhail Dufresne, Eric M. Reininger, Ruben BE Arp, U Reversz, P Williams, GP TI A Sagittally Bent Crystal for the Short Pulse X-ray Beam line at the Advanced Photon Source SO 17TH PAN-AMERICAN SYNCHROTRON RADIATION INSTRUMENTATION CONFERENCE SRI2013 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 17th Pan-American Synchrotron Radiation Instrumentation Conference (SRI) CY JUN 19-21, 2013 CL Natl Inst Stand & Technol, Synchrotron Ultraviolet Radiat Facil, Gaithersburg, MD SP Cornell Univ Cornell High Energy Synchrotron Source, Thomas Jefferson Natl Accelerator Facil HO Natl Inst Stand & Technol, Synchrotron Ultraviolet Radiat Facil ID SYNCHROTRON-RADIATION AB The Short Pulse X-ray Imaging and Microscopy (SPXIM) Beam line at the Advanced Photon Source (APS) is being designed to provide a short-pulse focused beam at the sample some 60 m from the source. The second crystal in the horizontally diffracting double-crystal monochromator system is sagittally bent to focus the full vertical fan of the beam, preserving the flux of a typical undulator beamline at the APS, while providing a time-angle correlated beam on the sample with a few-picosecond pulse duration. An energy scan using this system requires changing the bent radius of the second crystal. Undesirable distortions in the sagittally bent second crystal are due to anticlastic deformations. In this paper, the analysis and design of the bent crystal is presented including an examination of the mechanical interaction between the crystal and the two pairs of rollers used to bend it. Ray tracings including the anticlastic deformations obtained from an optimized finite element model show a minimal effect on the spot size at the sample position. C1 [Storns, Philip; Khounsary, Ali; Antimonov, Mikhail; Dufresne, Eric M.; Reininger, Ruben] Argonne Natl Lab, Argonne, IL 60439 USA. RP Storns, P (reprint author), Argonne Natl Lab, 9700 S Cass Ave, Argonne, IL 60439 USA. EM amk@aps.anl.gov RI Antimonov, Mikhail/P-2064-2016 OI Antimonov, Mikhail/0000-0002-5769-0132 NR 6 TC 0 Z9 0 U1 0 U2 0 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 493 AR 012023 DI 10.1088/1742-6596/493/1/012023 PG 4 WC Instruments & Instrumentation; Optics; Physics, Applied SC Instruments & Instrumentation; Optics; Physics GA BA4LZ UT WOS:000336000800023 ER PT S AU Tanabe, T Kitegi, C He, P Musardo, M Rank, OCJ Cappadoro, P Fernandes, H Harder, D Corwin, T AF Tanabe, Toshi Kitegi, Charles He, Ping Musardo, Marco Rank, Oleg Chubar James Cappadoro, Peter Fernandes, Huston Harder, David Corwin, Todd BE Arp, U Reversz, P Williams, GP TI The Latest Status of NSLS-II Insertion Devices SO 17TH PAN-AMERICAN SYNCHROTRON RADIATION INSTRUMENTATION CONFERENCE SRI2013 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 17th Pan-American Synchrotron Radiation Instrumentation Conference (SRI) CY JUN 19-21, 2013 CL Natl Inst Stand & Technol, Synchrotron Ultraviolet Radiat Facil, Gaithersburg, MD SP Cornell Univ Cornell High Energy Synchrotron Source, Thomas Jefferson Natl Accelerator Facil HO Natl Inst Stand & Technol, Synchrotron Ultraviolet Radiat Facil AB The National Synchrotron Light Source-II (NSLS-II) project is now in the final stage of construction. The Linac, the Booster synchrotron, and the Storage Ring magnets girder assemblies have been installed. The first damping wiggler has been delivered and its field characteristics are carefully measured. A Three Pole Wiggler (3PW) and Apple-II type elliptically polarizing undulators (EPUs) have been fabricated by the vendors. Two 3.0m long in-vacuum undulators (IVUs) and one 1.5m long IVU are almost complete and waiting for factory acceptance tests. One 3.0m long IVU for Inelastic X-ray Scattering beamline is in fabrication by a different vendor. Recently two 2.8m long IVUs for long straight sections (LSSs) have been added to the project for "future beamlines". In addition, two 1.5m long IVUs and one 2.8m long IVU for LSSs have been procured for Advanced Beamlines for Biological Investigations with X-rays (ABBIX) project funded by National Institure of Health (NIH). Further, two 3.5m long EPUs for LSSs are being designed for NSLS-II Experimental Tools (NEXT) -Major Item of Equipment (MIE) project. To succeed these conventional IVUs, PrFeB based cryo-permanent magnet undulator (CPMU) is considered as next generation device of hard X-ray sources. An In-Vacuum Magnetic Measurement System (IVMMS) for cold in-situ Hall probe mapping of CPMUs up to 1.5m in length has been developed. Summary of the current status of each project and future plans for the NSLS-II ring will be discussed. C1 [Tanabe, Toshi; Kitegi, Charles; He, Ping; Musardo, Marco; Rank, Oleg Chubar James; Cappadoro, Peter; Fernandes, Huston; Harder, David; Corwin, Todd] Brookhaven Natl Lab, Photon Sci Directorate, Upton, NY 11973 USA. RP Tanabe, T (reprint author), Brookhaven Natl Lab, Photon Sci Directorate, Upton, NY 11973 USA. EM ttanabe@bnl.gov NR 3 TC 0 Z9 0 U1 0 U2 5 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 493 AR 012031 DI 10.1088/1742-6596/493/1/012031 PG 4 WC Instruments & Instrumentation; Optics; Physics, Applied SC Instruments & Instrumentation; Optics; Physics GA BA4LZ UT WOS:000336000800031 ER PT S AU Tarawneh, H Steier, C Falcone, R Robin, D Nishimura, H Sun, C Wan, W AF Tarawneh, H. Steier, C. Falcone, R. Robin, D. Nishimura, H. Sun, C. Wan, W. BE Arp, U Reversz, P Williams, GP TI ALS-II, a Potential Soft X-ray, Diffraction Limited Upgrade of the Advanced Light Source SO 17TH PAN-AMERICAN SYNCHROTRON RADIATION INSTRUMENTATION CONFERENCE SRI2013 SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 17th Pan-American Synchrotron Radiation Instrumentation Conference (SRI) CY JUN 19-21, 2013 CL Natl Inst Stand & Technol, Synchrotron Ultraviolet Radiat Facil, Gaithersburg, MD SP Cornell Univ Cornell High Energy Synchrotron Source, Thomas Jefferson Natl Accelerator Facil HO Natl Inst Stand & Technol, Synchrotron Ultraviolet Radiat Facil AB The Advanced Light Source (ALS) at Berkeley Lab has seen many upgrades over the years, keeping it one of the brightest sources for soft x-rays worldwide. Recent developments in magnet technology and lattice design appear to open the door for very large further increases in brightness [1], particularly by reducing the horizontal emittance, even within the space constraints of the existing tunnel. Initial studies for possible lattices will be presented that could approach the soft x-ray diffraction limit around 2 keV in both planes within the ALS footprint. Emerging scientific applications and experimental methods that would greatly benefit from ring based sources having much higher brightness and transverse coherence than present or near future storage ring facilities include nanometer imaging applications, X-ray correlation spectroscopy, diffraction microscopy, holography, ptychography, and resonant inelastic soft X-ray scattering at high resolution. C1 [Tarawneh, H.; Steier, C.; Falcone, R.; Robin, D.; Nishimura, H.; Sun, C.; Wan, W.] Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Tarawneh, H (reprint author), Lawrence Berkeley Natl Lab, 1 Cyclotron Rd, Berkeley, CA 94720 USA. EM hitarawneh@lbl.gov NR 10 TC 2 Z9 2 U1 0 U2 0 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 493 AR 012020 DI 10.1088/1742-6596/493/1/012020 PG 4 WC Instruments & Instrumentation; Optics; Physics, Applied SC Instruments & Instrumentation; Optics; Physics GA BA4LZ UT WOS:000336000800020 ER PT J AU Schie, IW Alber, L Gryshuk, AL Chan, JW AF Schie, Iwan W. Alber, Lucas Gryshuk, Amy L. Chan, James W. TI Investigating drug induced changes in single, living lymphocytes based on Raman micro-spectroscopy SO ANALYST LA English DT Article ID CELL-CYCLE; APOPTOTIC CELLS; T-LYMPHOCYTES; MICROSPECTROSCOPY; IDENTIFICATION; CYTOMETRY; CANCER AB Raman spectroscopy is a powerful tool for label-free, single cell characterization. In many reported studies, a Raman spectrum is acquired from a fraction of the cell volume and used as a representative signature of the whole cell to identify and discriminate between cell populations. It has remained an open question whether this is the most suitable approach since the spectra may not truly represent the cell as a whole and critical biochemical information could therefore be lost. To address this question, we developed a line-scan Raman microscope to acquire Raman images of single lymphocytes exposed to the chemotherapeutic drug doxorubicin for 24 to 96 hours. Principal component analysis was able to separate cells based on their drug-exposure times. Difference spectra on the mean data for the different time-points revealed that changes are related to a decrease in mean nucleic acid content and an increase in mean protein and lipid content. Vertex component analysis was used to extract the pure component spectra of lipids, nucleic acids, and proteins. Quantitative analysis of the data revealed that biochemical changes occurred at both local subcellular (i.e. molecular density) and global cellular (i.e. total observable molecular content) levels. However, significant differences between the trends in the local and global changes were observed. While local nucleic acid content decreased with increasing drug exposure time, the total cellular nucleic acid content remained relatively constant. For protein, local content remained relatively constant for all exposure times while the total protein content in the cell increased similar to 3 fold. Lipid content in the entire cell increased similar to 5 fold, compared to a smaller increase in lipid at the local level. These results show that valuable information about the biochemical changes throughout the entire cell can be missed if only Raman spectra of localized cell regions are used. These findings are expected to have a major impact on the future development of Raman spectroscopy for cytometry applications. C1 [Schie, Iwan W.; Chan, James W.] Univ Calif Davis, Ctr Biophoton Sci & Technol, Sacramento, CA 95817 USA. [Alber, Lucas] Heidelberg Univ, Dept Phys, D-69117 Heidelberg, Germany. [Gryshuk, Amy L.] Lawrence Livermore Natl Lab, Biosci & Biotechnol Div, Livermore, CA 94550 USA. [Chan, James W.] Univ Calif Davis, Dept Pathol & Lab Med, Sacramento, CA 95817 USA. RP Schie, IW (reprint author), Univ Calif Davis, Ctr Biophoton Sci & Technol, Sacramento, CA 95817 USA. EM iwan.schie@ipht-jena.de; jwjchan@ucdavis.edu RI Chan, James/J-3829-2014 FU National Science Foundation, Center for Biophotonics Sensors and Systems NSF award [1068109]; Creation of an Ecosystem for Biophotonics Innovation NSF award [1127888]; Ecosystem for Biophotonic Innovation: Building Sustainability NSF award [1343479]; Keaton Raphael Memorial Foundation FX We would like to thank Drs Kris Kulp and Mike Malfatti from Lawrence Livermore National Laboratory for fruitful discussions on this project. This work has been funded in part by the National Science Foundation, Center for Biophotonics Sensors and Systems NSF award 1068109, the Creation of an Ecosystem for Biophotonics Innovation NSF award 1127888, Ecosystem for Biophotonic Innovation: Building Sustainability NSF award 1343479, and by the Keaton Raphael Memorial Foundation. NR 39 TC 15 Z9 15 U1 4 U2 29 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 0003-2654 EI 1364-5528 J9 ANALYST JI Analyst PY 2014 VL 139 IS 11 BP 2726 EP 2733 DI 10.1039/c4an00250d PG 8 WC Chemistry, Analytical SC Chemistry GA AH2CS UT WOS:000335928900017 PM 24756205 ER PT J AU Wang, H Shen, J Li, YY Wei, ZY Cao, GX Gai, Z Hong, KL Banerjee, P Zhou, SQ AF Wang, Hui Shen, Jing Li, Yingyu Wei, Zengyan Cao, Guixin Gai, Zheng Hong, Kunlun Banerjee, Probal Zhou, Shuiqin TI Magnetic iron oxide-fluorescent carbon dots integrated nanoparticles for dual-modal imaging, near-infrared light-responsive drug carrier and photothermal therapy SO BIOMATERIALS SCIENCE LA English DT Article ID HYBRID NANOPARTICLES; QUANTUM DOTS; CORE-SHELL; BIFUNCTIONAL NANOPARTICLES; INORGANIC NANOPARTICLES; EMERGENT NANOLIGHTS; FACILE SYNTHESIS; IN-VIVO; PROBES; NANOSTRUCTURES AB Multifunctional hybrid nanoparticles (NPs, similar to 100 nm) that combine magnetic Fe3O4 nanocrystals and fluorescent carbon dots (CDs) in porous carbon (C) were successfully synthesized using a one-pot solvothermal method by simply increasing the H2O2 concentration. The resultant Fe3O4@C-CDs hybrid NPs not only demonstrate excellent magnetic responsive properties (M-s = 32.5 emu g(-1)) and magnetic resonance imaging ability (r(2)(star) = 674.4 mM(-1) s(-1)) from the Fe3O4 nanocrystal core, but also exhibit intriguing photoluminescent (quantum yield similar to 6.8%) properties including upconversion fluorescence and excellent photostability from the CDs produced in the porous carbon. The hybrid NPs can enter the intracellular region and illuminate mouse melanoma B16F10 cells under different excitation wavelengths. Meanwhile, the mesoporous carbon shell and hydrophilic surface functional groups endow the hybrid NPs with high loading capacity (835 mg g(-1)) for the anti-cancer drug doxorubicin and excellent stability in aqueous solutions. More importantly, the hybrid NPs can absorb and convert near-infrared (NIR) light to heat due to the existence of CDs, and thus, can realise NIR-controlled drug release and combined photothermo/chemotherapy for high therapeutic efficacy. Such nanostructured Fe3O4@C-CDs hybrid NPs demonstrate great promise towards advanced nanoplatforms for simultaneous imaging diagnostics and high efficacy therapy. C1 [Wang, Hui; Shen, Jing; Li, Yingyu; Banerjee, Probal; Zhou, Shuiqin] CUNY Coll Staten Isl, Dept Chem, Staten Isl, NY 10314 USA. [Wang, Hui; Shen, Jing; Li, Yingyu; Banerjee, Probal; Zhou, Shuiqin] CUNY, Grad Ctr, Staten Isl, NY 10314 USA. [Wei, Zengyan] CUNY Hunter Coll, Dept Chem & Biochem, New York, NY 10065 USA. [Cao, Guixin; Gai, Zheng; Hong, Kunlun] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. [Cao, Guixin; Gai, Zheng; Hong, Kunlun] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. RP Wang, H (reprint author), CUNY Coll Staten Isl, Dept Chem, Staten Isl, NY 10314 USA. EM shuiqin.zhou@csi.cuny.edu RI Gai, Zheng/B-5327-2012; wang, hui/G-6433-2015; Cao, Guixin/G-4452-2015; Wei, Zengyan/B-1548-2012; Hong, Kunlun/E-9787-2015 OI Gai, Zheng/0000-0002-6099-4559; Cao, Guixin/0000-0002-9252-1158; Wei, Zengyan/0000-0001-6948-7572; Hong, Kunlun/0000-0002-2852-5111 FU American Diabetes Association [1-12-BS-243]; PSC-CUNY [66076-00 44]; Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy FX We gratefully acknowledge the financial support from the American Diabetes Association (Basic Science Award 1-12-BS-243) and PSC-CUNY Research Award (66076-00 44). A portion of this research was 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. NR 68 TC 36 Z9 37 U1 18 U2 210 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2047-4830 EI 2047-4849 J9 BIOMATER SCI-UK JI Biomater. Sci. PY 2014 VL 2 IS 6 BP 915 EP 923 DI 10.1039/c3bm60297d PG 9 WC Materials Science, Biomaterials SC Materials Science GA AH2WZ UT WOS:000335984000012 ER PT J AU Zang, HD Routh, PK Alam, R Maye, MM Cotlet, M AF Zang, Huidong Routh, Prahlad K. Alam, Rabeka Maye, Mathew M. Cotlet, Mircea TI Core size dependent hole transfer from a photoexcited CdSe/ZnS quantum dot to a conductive polymer SO CHEMICAL COMMUNICATIONS LA English DT Article ID POWER-LAW BEHAVIOR; ENERGY-TRANSFER; PHOTOLUMINESCENCE BLINKING; FLUORESCENCE INTERMITTENCY; SOLAR-CELLS; NANOCRYSTALS; ELECTROLUMINESCENCE; NANOPARTICLES; INTENSITY; SERIES AB Photoinduced hole transfer from a CdSe/ZnS quantum dot to a conjugated polymer is tuned by varying the quantum dot core size. Hole transfer affects the photoluminescence blinking of the quantum dot, increasing the duration of the on-states and decreasing that of the off-states. C1 [Zang, Huidong; Routh, Prahlad K.; Cotlet, Mircea] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. [Alam, Rabeka; Maye, Mathew M.] Syracuse Univ, Dept Chem, Syracuse, NY 13224 USA. RP Zang, HD (reprint author), Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. EM cotlet@bnl.gov OI Routh, Prahlad Kumar/0000-0002-0629-3743 FU U.S. Department of Energy, Office of Basic Energy Sciences [DE-AC02-98CH10886]; AFOSR [FA9550-10-1-0033] FX Research carried out in part at the Center for Functional Nanomaterials at Brookhaven National Laboratory and sponsored by the U.S. Department of Energy, Office of Basic Energy Sciences, (Contract No. DE-AC02-98CH10886). M.M.M. acknowledges support from AFOSR (FA9550-10-1-0033). We thank Dr H.L. Wang from Los Alamos National Laboratory in New Mexico and Dr H.Y. Woo from Pusan National University in South Korea for providing FHQ. NR 33 TC 12 Z9 13 U1 1 U2 27 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 2014 VL 50 IS 45 BP 5958 EP 5960 DI 10.1039/c3cc47975g PG 3 WC Chemistry, Multidisciplinary SC Chemistry GA AH2XG UT WOS:000335984700002 PM 24301881 ER PT J AU Steiner, AL Tawfik, AB Shalaby, A Zakey, AS Abdel-Wahab, MM Salah, Z Solmon, F Sillman, S Zaveri, RA AF Steiner, A. L. Tawfik, A. B. Shalaby, A. Zakey, A. S. Abdel-Wahab, M. M. Salah, Z. Solmon, F. Sillman, S. Zaveri, R. A. TI Climatological simulations of ozone and atmospheric aerosols in the Greater Cairo region SO CLIMATE RESEARCH LA English DT Article DE Ozone; Mediterranean; Urban; Air quality ID CLIMATE MODEL; INTERANNUAL VARIABILITY; NITROGEN-DIOXIDE; URBAN AREA; EGYPT; EMISSIONS; POLLUTION; AFRICA; DUST; TRANSPORT AB An integrated chemistry-climate model (RegCM4-CHEM) simulates present-day climate, ozone and tropospheric aerosols over Egypt with a focus on northern Africa and the Greater Cairo (GC) region. The densely populated GC region is known for its severe air quality issues driven by high levels of anthropogenic pollution in conjunction with natural sources such as dust, and agricultural burning events. We find that current global emission inventories underestimate key pollutants such as nitrogen oxides and anthropogenic aerosol species. In the GC region, average ground-based observations of the daily July maximum nitrogen dioxide (NO2)are 40 to 60 parts per billion by volume (ppbv) and are about 10 ppbv higher than modeled estimates, likely due to model grid cell resolution, improper boundary layer representation, and poor emissions inventories. Observed July daily maximum ozone concentrations range from 30 ppbv (winter) to 90 ppbv (summer). The model reproduces the seasonal cycle fairly well, but modeled July ozone is underestimated by approximately 10 ppbv and exhibits little interannual variability. For aerosols, springtime dust events dominate the seasonal aerosol cycle. The chemistry-climate model captures the springtime peak aerosol optical depth (AOD) of 0.7 to 1 but is slightly greater than satellite-derived AOD. Observed AOD decreases in the summer and increases again in the fall due to agricultural burning events in the Nile Delta; however, the model underestimates this observed AOD peak in fall, as standard emissions inventories underestimate the extent of this burning and the resulting aerosol emissions. Our comparison of modeled gas and particulate phase atmospheric chemistry in the GC region indicates that improved emissions inventories of mobile sources and other anthropogenic activities, specifically NOx and organic aerosols, are needed to improve air quality simulations in this region. C1 [Steiner, A. L.; Tawfik, A. B.; Sillman, S.] Univ Michigan, Dept Atmospher Ocean & Space Sci, Ann Arbor, MI 48109 USA. [Shalaby, A.; Zakey, A. S.; Salah, Z.] Egyptian Meteorol Author, Cairo, Egypt. [Abdel-Wahab, M. M.] Cairo Univ, Dept Methodol, Cairo, Egypt. [Solmon, F.] Abdus Salaam Int Ctr Theoret Phys, Earth Syst Phys Grp, I-34151 Trieste, Italy. [Zaveri, R. A.] Pacific NW Natl Lab, Atmospher Sci & Global Change Div, Richland, WA 99352 USA. RP Steiner, AL (reprint author), Univ Michigan, Dept Atmospher Ocean & Space Sci, Ann Arbor, MI 48109 USA. EM alsteiner@umich.edu RI Tawfik, Ahmed/D-3683-2015; Zaveri, Rahul/G-4076-2014; Steiner, Allison/F-4942-2011 OI Tawfik, Ahmed/0000-0002-6631-9300; Zaveri, Rahul/0000-0001-9874-8807; FU US-Egypt Joint Board on Scientific and Technological Collaboration [NSF AGS-0809255]; European Union [212520]; US Department of Energy's Atmospheric System Research (ASR) program FX This work was supported through a grant from the US-Egypt Joint Board on Scientific and Technological Collaboration to A.S.Z. and A. L. S. (NSF AGS-0809255) and the European Union's Seventh Framework Programme (FP/2007-2011) within the project MEGAPOLI (grant agreement no. 212520). We thank the International Centre for Theoretical Physics, Trieste, Italy and the Earth System Physics group for providing administrative and computational support for this project. Participation of R.A.Z. in this study was partially supported by the US Department of Energy's Atmospheric System Research (ASR) program. We also gratefully acknowledge Louisa Emmons at NCAR for providing MOZART chemical boundary conditions for these simulations. Additionally, we thank Olivier Favez, Stephane Alfaro, and Jean Sciare for graciously providing CACHE observational data. NR 62 TC 2 Z9 2 U1 0 U2 9 PU INTER-RESEARCH PI OLDENDORF LUHE PA NORDBUNTE 23, D-21385 OLDENDORF LUHE, GERMANY SN 0936-577X EI 1616-1572 J9 CLIM RES JI Clim. Res. PY 2014 VL 59 IS 3 BP 207 EP 228 DI 10.3354/cr01211 PG 22 WC Environmental Sciences; Meteorology & Atmospheric Sciences SC Environmental Sciences & Ecology; Meteorology & Atmospheric Sciences GA AH0RO UT WOS:000335828100003 ER PT J AU Polat, BD Eryilmaz, OL Keles, O AF Polat, B. Deniz Eryilmaz, O. Levent Keles, Ozgul TI Si Based Anodes via Magnetron Sputtering for LIB SO ECS ELECTROCHEMISTRY LETTERS LA English DT Article ID LITHIUM-ION BATTERIES; THIN-FILM; SILICON; COPPER AB The reversible cyclability of Si based anodes is greatly improved by tuning the atomic ratio of Cu/Si and the thickness of films fabricated via magnetron sputtering. High electrochemical performance is achieved when the thin film made of 10% at.Cu-90% at.Si is used. 1100 mAhg(-1) specific capacity is delivered after the 100th cycles with 99.7% Coulombic efficiency. This remarkable performance is the result of the amorphous structure and enhanced physical and mechanical properties of the thin film. (C) 2014 The Electrochemical Society. All rights reserved. C1 [Polat, B. Deniz; Keles, Ozgul] Istanbul Tech Univ, Dept Met & Mat Engn, TR-34469 Istanbul, Turkey. [Eryilmaz, O. Levent] Argonne Natl Lab, Div Energy Syst, Argonne, IL 60439 USA. RP Polat, BD (reprint author), Istanbul Tech Univ, Dept Met & Mat Engn, TR-34469 Istanbul, Turkey. EM b.denizpolat@gmail.com NR 8 TC 6 Z9 6 U1 3 U2 13 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 2014 VL 3 IS 6 BP A45 EP A49 DI 10.1149/2.009405eel PG 5 WC Electrochemistry; Materials Science, Multidisciplinary SC Electrochemistry; Materials Science GA AH3GT UT WOS:000336012400003 ER PT S AU Drachenberg, DR Messerly, MJ Pax, PH Sridharan, AK Tassano, JB Dawson, JW AF Drachenberg, Derrek R. Messerly, Michael J. Pax, Paul H. Sridharan, Arun K. Tassano, John B. Dawson, Jay W. BE Ramachandran, S TI Yb3+doped ribbon fiber for high average power lasers and amplifiers SO FIBER LASERS XI: TECHNOLOGY, SYSTEMS, AND APPLICATIONS SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Fiber Lasers XI - Technology, Systems, and Applications CY FEB 03-06, 2014 CL San Francisco, CA SP SPIE, NKT Photon A S, PolarOnyx, Inc ID ORDER MODE AB Diffraction-limited high power lasers in the region of 10s of kW to greater than 100 kW are needed for defense, manufacturing and future science applications. A balance of thermal lensing and Stimulated Brillouin Scattering (SBS) for narrowband amplifiers and Stimulated Raman Scattering (SRS) for broadband amplifiers is likely to limit the average power of circular core fiber amplifiers to 2 kW (narrowband) or 36 kW (broadband). A ribbon fiber, which has a rectangular core, operating in a high order mode can overcome these obstacles by increasing mode area without becoming thermal lens limited and without the on-axis intensity peak associated with circular high order modes. High order ribbon fiber modes can also be converted to a fundamental Gaussian mode with high efficiency for applications in which this is necessary. We present an Yb-doped, air clad, optical fiber having an elongated, ribbon-like core having an effective mode area of area of 600 mu m(2) and an aspect ratio of 13:1. As an amplifier, the fiber produced 50% slope efficiency and a seed-limited power of 10.5 W, a gain of 24 dB. As an oscillator, the fiber produced multimode power above 40 W with 71% slope efficiency and single mode power above 5 W with 44% slope efficiency. The multimode M-2 beam quality factor of the fiber was 1.6 in the narrow dimension and 15 in the wide dimension. C1 [Drachenberg, Derrek R.; Messerly, Michael J.; Pax, Paul H.; Sridharan, Arun K.; Tassano, John B.; Dawson, Jay W.] Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. RP Drachenberg, DR (reprint author), Lawrence Livermore Natl Lab, L-491,POB 808, Livermore, CA 94551 USA. EM drachenberg1@llnl.gov RI Chen, Ru/A-5105-2015 NR 13 TC 1 Z9 1 U1 0 U2 8 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9874-8 J9 PROC SPIE PY 2014 VL 8961 AR 89610T DI 10.1117/12.2040792 PG 10 WC Engineering, Electrical & Electronic; Optics; Physics, Applied SC Engineering; Optics; Physics GA BA4KL UT WOS:000335903300017 ER PT S AU Moore, SW Patterson, BD Soh, DBS Bisson, SE AF Moore, Sean W. Patterson, Brian D. Soh, Daniel B. S. Bisson, Scott E. BE Ramachandran, S TI An all-fiber high-energy cladding-pumped 93 nanosecond Q-switched fiber laser using an Yb3+-doped fiber saturable absorber SO FIBER LASERS XI: TECHNOLOGY, SYSTEMS, AND APPLICATIONS SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Fiber Lasers XI - Technology, Systems, and Applications CY FEB 03-06, 2014 CL San Francisco, CA SP SPIE, NKT Photon A S, PolarOnyx, Inc ID DOPED FIBER AB We report an all-fiber passively Q-switched laser using a large mode area (LMA) Yb3+-doped fiber cladding-pumped at 915 nm and an unpumped single-mode (SM) Yb3+-doped fiber as the saturable absorber (SA). The saturable absorber SM fiber and LMA gain fiber were coupled with a fiber taper designed to match the fundamental spatial mode of the LMA fiber and the expanded LP01 mode of the single mode fiber. The amplified spontaneous (ASE) intensity propagating in the single mode SA saturates the absorption before the onset of gain depletion in the pumped fiber, switching the fiber cavity to a high Q-state and producing a pulse. Using this scheme we demonstrate a Q-switched all-fiber oscillator with 32 mu J 93 ns pulses at 1030 nm. The associated peak power is nearly two orders of magnitude larger than that reported in previous experimental studies using a single Yb+3 saturable absorber fiber. The pulse energy was amplified to 0.230 mJ using an Yb3+-doped cladding pumped fiber amplifier fusion spliced to the fiber oscillator, increasing the energy by eight fold while preserving the all-fiber architecture. C1 [Moore, Sean W.; Patterson, Brian D.; Soh, Daniel B. S.; Bisson, Scott E.] Sandia Natl Labs, Livermore, CA 94550 USA. RP Moore, SW (reprint author), Sandia Natl Labs, 7011 East Ave, Livermore, CA 94550 USA. RI Chen, Ru/A-5105-2015 NR 6 TC 0 Z9 0 U1 0 U2 1 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9874-8 J9 PROC SPIE PY 2014 VL 8961 AR 896113 DI 10.1117/12.2040813 PG 4 WC Engineering, Electrical & Electronic; Optics; Physics, Applied SC Engineering; Optics; Physics GA BA4KL UT WOS:000335903300026 ER PT J AU Adzima, BJ Venna, SR Klara, SS He, HK Zhong, MJ Luebke, DR Mauter, MS Matyjaszewski, K Nulwala, HB AF Adzima, Brian J. Venna, Surendar R. Klara, Steven S. He, Hongkun Zhong, Mingjiang Luebke, David R. Mauter, Meagan S. Matyjaszewski, Krzysztof Nulwala, Hunaid B. TI Modular polymerized ionic liquid block copolymer membranes for CO2/N-2 separation SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID ABA TRIBLOCK COPOLYMERS; EPOXY CLICK CHEMISTRY; RADICAL POLYMERIZATION; POLY(IONIC LIQUID)S; PHASE-BEHAVIOR; MULTIFUNCTIONAL POLYMERS; RAFT POLYMERIZATION; THERMAL-PROPERTIES; CO2 SEPARATION; CARBON-DIOXIDE AB The continuing discovery of broad classes of materials, such as ionic liquids, zeolites, metal-organic frameworks, and block copolymers, presents an enormous opportunity in developing materials for new applications. Polymerized ionic liquid block copolymers (PIL-BCPs) fall at the union of two already large sets of materials, and are an emerging class of materials useful in gas separation membranes, ion and electron conducting materials, and as mechanical actuators. A wide range of ionic liquid moieties can be used as pendant groups along the polymer backbone, potentially allowing for a wide variation in the resulting material properties; however in practice the range of ionic liquids explored is hindered by the need to optimize polymerization conditions for each new monomer. Here, we present a modular approach to PIL-BCP synthesis where a variety of olefin bearing cations are readily conjugated to polymers using thiol-Michael click chemistry. This approach allowed for the rapid development of a diverse material library including phase separated thin films, ion-gels, and liquid PIL-BCPs, with a reduced investment in synthetic time. Finally, we demonstrate that this approach identified PIL-BCPs with increased CO2 permeability relative to PILs, which could find use in carbon capture from flue gas. C1 [Adzima, Brian J.; Venna, Surendar R.; Luebke, David R.; Nulwala, Hunaid B.] Natl Energy Technol Lab, Pittsburgh, PA 15236 USA. [Klara, Steven S.; Mauter, Meagan S.] Carnegie Mellon Univ, Dept Chem Engn, Pittsburgh, PA 15213 USA. [He, Hongkun; Zhong, Mingjiang; Matyjaszewski, Krzysztof; Nulwala, Hunaid B.] Carnegie Mellon Univ, Dept Chem, Pittsburgh, PA 15213 USA. RP Mauter, MS (reprint author), Carnegie Mellon Univ, Dept Chem Engn, 5000 Forbes Ave, Pittsburgh, PA 15213 USA. EM mauter@cmu.edu; km3@andrew.cmu.edu; hnulwala@andrew.cmu.edu RI Nulwala, Hunaid/G-8126-2012; He, Hongkun/B-4759-2011; Zhong, Mingjiang/F-3470-2011; Matyjaszewski, Krzysztof/A-2508-2008; OI Nulwala, Hunaid/0000-0001-7481-3723; He, Hongkun/0000-0002-7214-3313; Zhong, Mingjiang/0000-0001-7533-4708; Matyjaszewski, Krzysztof/0000-0003-1960-3402; Mauter, Meagan/0000-0002-4932-890X FU U.S. Department of Energy's National Energy Technology Laboratory [DE-FE0004000] FX This technical effort was also performed in support of the U.S. Department of Energy's National Energy Technology Laboratory's on-going research on CO2 capture under the contract DE-FE0004000. NR 63 TC 26 Z9 26 U1 9 U2 127 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 2014 VL 2 IS 21 BP 7967 EP 7972 DI 10.1039/c4ta00661e PG 6 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA AH2AW UT WOS:000335924100046 ER PT J AU Ho, CC Chen, CA Chang, CY Darling, SB Su, WF AF Ho, Chun-Chih Chen, Chien-An Chang, Chun-Yu Darling, Seth B. Su, Wei-Fang TI Isoindigo-based copolymers for polymer solar cells with efficiency over 7% SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID FIELD-EFFECT TRANSISTORS; CONJUGATED POLYMERS; PHOTOVOLTAIC APPLICATIONS; ACCEPTOR; DESIGN; MOLECULE; DENSITY; IMPACT AB A series of isoindigo-based low-band-gap copolymers (PnTI) containing an extended thiophene unit in the donor segment of the polymer were synthesized. The results show that the extended thiophene unit with centrosymmetric conformation simultaneously broadens the polymer absorption and enhances the crystallinity and, thus, hole mobility. Consequently, with additional improved solubility, the polymer P6TI exhibits the highest PCE of 7.25% (and a high J(sc) of 16.24 mA cm(-2)) among isoindigo-based low-band-gap copolymers. This work demonstrates that by simply adjusting the donor segment and with relatively simple synthetic schemes, a material for high-performance and scalable PSCs will become available. C1 [Ho, Chun-Chih; Chang, Chun-Yu; Su, Wei-Fang] Natl Taiwan Univ, Dept Mat Sci & Engn, Taipei 10617, Taiwan. [Chen, Chien-An; Su, Wei-Fang] Natl Taiwan Univ, Inst Polymer Sci & Engn, Taipei 10617, Taiwan. [Darling, Seth B.] Argonne Natl Lab, Ctr Nanoscale Mat, Lemont, IL 60439 USA. [Darling, Seth B.] Univ Chicago, Inst Mol Engn, Chicago, IL USA. RP Su, WF (reprint author), Natl Taiwan Univ, Dept Mat Sci & Engn, Taipei 10617, Taiwan. EM suwf@ntu.edu.tw RI Su, Wei-Fang/C-2646-2009 FU National Science Council of Taiwan [NSC 99-2221-E-002-020-MY3, 101-2120-M-002-003, 101-3113-E-002-010, 102-3113-P-002-027]; US Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357] FX We gratefully acknowledge the financial support from the National Science Council of Taiwan (NSC 99-2221-E-002-020-MY3, 101-2120-M-002-003, 101-3113-E-002-010, and 102-3113-P-002-027). We also thank the Department of Chemistry of National Taiwan University for use of their NMR spectrometer. Use of the Center for Nanoscale Materials at Argonne National Laboratory was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract no. DE-AC02-06CH11357. NR 39 TC 22 Z9 22 U1 3 U2 24 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 2014 VL 2 IS 21 BP 8026 EP 8032 DI 10.1039/c4ta01083c PG 7 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA AH2AW UT WOS:000335924100054 ER PT J AU Nikodinovic-Runic, J Mojic, M Kang, YJ Maksimovic-Ivanic, D Mijatovic, S Vasiljevic, B Stamenkovic, VR Senerovic, L AF Nikodinovic-Runic, Jasmina Mojic, Marija Kang, Yijin Maksimovic-Ivanic, Danijela Mijatovic, Sanja Vasiljevic, Branka Stamenkovic, Vojislav R. Senerovic, Lidija TI Undecylprodigiosin conjugated monodisperse gold nanoparticles efficiently cause apoptosis in colon cancer cells in vitro SO JOURNAL OF MATERIALS CHEMISTRY B LA English DT Article ID TARGETED DRUG-DELIVERY; ANTICANCER ACTIVITY; BACTERIAL PRODIGININES; PRODIGIOSIN ANALOGS; RESISTANCE; SIZE; BIOSYNTHESIS; THERAPY; AGENTS; RED AB Bacterial pigment undecylprodigiosin (UP) was produced using Streptomyces sp. JS520 and conjugated to monodisperse gold nanoparticles (UP-Au). Both UP and UP-Au showed cytocidal activity towards melanoma (A375), lung carcinoma (A549), breast cancer (MCF-7) and colon cancer (HCT-116) cells, inducing apoptosis with IC50 values ranging from 0.4 to 4 mu g ml(-1). Unconjugated UP had a tendency to lose its activity over time and to change biophysical characteristics over pH. The loss of the pigment potency was overcome by conjugation with gold nanoparticles. UP-Au exhibited high stability over pH 3.8 to 7.4 and its activity remained unaffected in time. Nano-packing changed the mechanism of UP toxicity by converting the intracellular signals from a mitochondrial dependent to a mitochondrial independent apoptotic process. The availability of nonpyrogenic UP in high amounts, together with specific anticancer activity and improved stability in the complex with gold nanoparticles, presents a novel platform for further development of UP-Au complexes as an anticancer drug suitable for clinical applications. C1 [Nikodinovic-Runic, Jasmina; Vasiljevic, Branka; Senerovic, Lidija] Univ Belgrade, Inst Mol Genet & Genet Engn, Belgrade 11010, Serbia. [Mojic, Marija; Maksimovic-Ivanic, Danijela; Mijatovic, Sanja] Univ Belgrade, Dept Immunol, Inst Biol Res Sinisa Stankov, Belgrade 11060, Serbia. [Kang, Yijin; Stamenkovic, Vojislav R.] Argonne Natl Lab, Div Mat Sci, Argonne, IL 60439 USA. RP Senerovic, L (reprint author), Univ Belgrade, Inst Mol Genet & Genet Engn, Vojvode Stepe 444a,POB 23, Belgrade 11010, Serbia. EM vrstamenkovic@anl.gov; seneroviclidija@imgge.bg.ac.rs RI Vasiljevic, Branka/H-6890-2012; Maksimovic-Ivanic, Danijela/E-7246-2015; Mijatovic, Sanja/E-7662-2015; Mojic, Marija/E-8729-2015 OI Vasiljevic, Branka/0000-0002-2315-3590; Maksimovic-Ivanic, Danijela/0000-0002-8006-5079; Mijatovic, Sanja/0000-0001-9509-9098; Mojic, Marija/0000-0002-4906-9880 FU Ministry of Education, Science and Technological Development of Serbia [173048, 173013]; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357] FX Part of the work performed at the University of Belgrade, Institute of Molecular Genetics and Genetic Engineering and Institute for Biological Research "Sinisa Stankovic" was supported by the Ministry of Education, Science and Technological Development of Serbia (Project no. 173048 and 173013). Part of the work performed at Argonne National Laboratory was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract DE-AC02-06CH11357. NR 59 TC 3 Z9 3 U1 0 U2 14 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-750X EI 2050-7518 J9 J MATER CHEM B JI J. Mat. Chem. B PY 2014 VL 2 IS 21 BP 3271 EP 3281 DI 10.1039/c4tb00300d PG 11 WC Materials Science, Biomaterials SC Materials Science GA AH4CE UT WOS:000336072400012 ER PT J AU Jiao, TF Yan, XB Balan, L Stepanov, AL Chen, XQ Hu, MZ AF Jiao, Tifeng Yan, Xingbin Balan, Lavinia Stepanov, Andrey L. Chen, Xinqing Hu, Michael Z. TI Chemical Functionalization, Self-Assembly, and Applications of Nanomaterials and Nanocomposites SO JOURNAL OF NANOMATERIALS LA English DT Editorial Material C1 [Jiao, Tifeng] Yanshan Univ, Sch Environm & Chem Engn, Qinhuangdao 066004, Peoples R China. [Yan, Xingbin] Chinese Acad Sci, Lanzhou Inst Chem Phys, Lab Clean Energy Chem & Mat, Lanzhou 730000, Peoples R China. [Balan, Lavinia] Inst Mat Sci Mulhouse IS2M, F-68057 Mulhouse, France. [Stepanov, Andrey L.] Russian Acad Sci, Kazan Phys Tech Inst, Kazan 420029, Russia. [Chen, Xinqing] Hong Kong Univ Sci & Technol, Dept Chem & Biomol Engn, Kowloon, Hong Kong, Peoples R China. [Hu, Michael Z.] Oak Ridge Natl Lab, Energy & Transportat Sci Div, Oak Ridge, TN 37831 USA. RP Yan, XB (reprint author), Chinese Acad Sci, Lanzhou Inst Chem Phys, Lab Clean Energy Chem & Mat, Lanzhou 730000, Peoples R China. EM xbyan@licp.cas.cn RI Yan, Xingbin/B-2408-2014; Balan, Lavinia/L-5866-2016; OI Yan, Xingbin/0000-0002-9976-8815; Hu, Michael/0000-0001-8461-9684 NR 0 TC 0 Z9 0 U1 1 U2 14 PU HINDAWI PUBLISHING CORPORATION PI NEW YORK PA 410 PARK AVENUE, 15TH FLOOR, #287 PMB, NEW YORK, NY 10022 USA SN 1687-4110 EI 1687-4129 J9 J NANOMATER JI J. Nanomater. PY 2014 AR 291013 DI 10.1155/2014/291013 PG 2 WC Nanoscience & Nanotechnology; Materials Science, Multidisciplinary SC Science & Technology - Other Topics; Materials Science GA AH7GO UT WOS:000336301300001 ER PT J AU Veneziani, M Griffa, A Garraffo, Z Mensa, JA AF Veneziani, Milena Griffa, Annalisa Garraffo, Zulema Mensa, Jean A. TI Barrier Layers in the Tropical South Atlantic: Mean Dynamics and Submesoscale Effects SO JOURNAL OF PHYSICAL OCEANOGRAPHY LA English DT Article DE Geographic location; entity; Tropics; Circulation; Dynamics; Atmosphere-ocean interaction; Eddies; Ocean dynamics; Atm; Ocean Structure; Phenomena; Oceanic mixed layer; Models and modeling; Ocean models ID CALIFORNIA CURRENT SYSTEM; EQUATORIAL WESTERN PACIFIC; SEA-SURFACE TEMPERATURE; MIXED-LAYER; PART I; 2-DIMENSIONAL TURBULENCE; BULK PARAMETERIZATION; OCEAN CIRCULATION; TOGA DECADE; VARIABILITY AB Barrier layers are generated when the surface mixed layer is shallower than the layer where temperature is well mixed, in geographical regions where salinity plays a key role in setting up upper-ocean density stratification. In the tropical oceans, thick barrier layers are also found in a latitude range where spiraling trajectories from surface in situ drifters suggest the presence of predominantly cyclonic submesoscale-like vortices. The authors explore these dynamical processes and their interplay in the present paper, focusing on the tropical South Atlantic Ocean and using a high-resolution modeling approach. The objective is threefold: to investigate the mean dynamics contributing to barrier-layer formation in this region, to study the distribution and seasonality of submesoscale features, and to verify whether and how the submesoscale impacts barrier-layer thickness. The model used is the Regional Ocean Modeling System (ROMS) in its Adaptive Grid Refinement in Fortran (AGRIF) online-nested configuration with a horizontal resolution ranging between 9 and 1 km. The simulated circulation is first described in terms of mean and submesoscale dynamics, and the associated seasonal cycle. Mechanisms for barrier-layer formation are then investigated. The results confirm previous hypotheses by Mignot et al. on the relevance of enhanced winter mixing deepening the isothermal layer, whereas the salinity stratification is sustained by advection of surface fresh waters and subsurface salinity maxima. Finally, submesoscale effects on barrier-layer thickness are studied, quantifying their contribution to vertical fluxes of temperature and salinity. Submesoscale vortices associated with salinity fronts are found to have a significant effect, producing thicker barrier layers (by similar to 20%-35%) and a shallower mixed layer because of their restratifying effect on salinity. C1 [Veneziani, Milena] Univ Calif Santa Cruz, Inst Marine Sci, Santa Cruz, CA 95064 USA. [Griffa, Annalisa] CNR, ISMAR, Pozzuolo Di Lerici, Italy. [Griffa, Annalisa; Garraffo, Zulema; Mensa, Jean A.] Univ Miami, Rosenstiel Sch Marine & Atmospher Sci, Miami, FL 33149 USA. [Garraffo, Zulema] NCWCP, NOAA EMC, IMSG, College Pk, MD USA. RP Veneziani, M (reprint author), Los Alamos Natl Lab, Fluid Dynam & Solid Mech Div, MS B216,POB 1663, Los Alamos, NM 87545 USA. EM milena@lanl.gov RI CNR, Ismar/P-1247-2014 OI CNR, Ismar/0000-0001-5351-1486 FU National Science Foundation [OCE-0850690, OCE-0850714] FX We gratefully acknowledge the support of the National Science Foundation through Grants OCE-0850690 and OCE-0850714. Computations were performed on the ShaRCS, UC Shared Research Computing Services Cluster, which is technically supported by multiple UC IT divisions and managed by the University of California, Office of the President. MV specifically acknowledges the technical assistance of Yon Qin and Krishna Muriki. We also thank Gualtiero Badin, Jeroen Molemaker, and Vincent Combes for interesting scientific discussions. NR 82 TC 2 Z9 2 U1 4 U2 24 PU AMER METEOROLOGICAL SOC PI BOSTON PA 45 BEACON ST, BOSTON, MA 02108-3693 USA SN 0022-3670 EI 1520-0485 J9 J PHYS OCEANOGR JI J. Phys. Oceanogr. PD JAN PY 2014 VL 44 IS 1 BP 265 EP 288 DI 10.1175/JPO-D-13-064.1 PG 24 WC Oceanography SC Oceanography GA AH0IH UT WOS:000335802100023 ER PT S AU Glavicic, M Brown, DW Clausen, B Sisneros, T Holden, TM AF Glavicic, M. Brown, D. W. Clausen, B. Sisneros, T. Holden, T. M. BE Holden, TM Muransky, O Hamelin, CJ TI Load-sharing in delta-processed Inconel 718 SO MECHANICAL STRESS EVALUATION BY NEUTRONS AND SYNCHROTRON RADIATION VII SE Materials Science Forum LA English DT Proceedings Paper CT 7th International Conference on Mechanical Stress Evaluation by Neutrons and Synchrotron Radiation CY SEP 10-12, 2013 CL Sydney, AUSTRALIA DE load-sharing; strain; neutron diffraction; nickel-based superalloy ID PLASTIC-DEFORMATION; NEUTRON-DIFFRACTION; SUPERALLOY; ALLOYS; NI3NB AB Time-of-flight neutron measurements have been made at 20, 400 and 650 degrees C on delta-processed Inconel 718 in order to measure the load sharing between the gamma-phase matrix and the orthorhombic delta-phase. The strain response parallel and perpendicular to the applied stress was measured for seven gamma-phase reflections and five delta-phase reflections. The latter were about 50 times weaker than the former suggesting a 2.0% concentration of the delta-phase. At all temperatures the delta-phase strain becomes strongly tensile parallel to the loading direction but also exhibits plastic deformation. However, the nature of the three orthorhombic strains changes with temperature. C1 [Glavicic, M.] Rolls Royce Corp, Indianapolis, IN 46206 USA. [Brown, D. W.; Clausen, B.; Sisneros, T.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Holden, T. M.] Northern Stress Technol, Deep River, ON KOJ1PO, Canada. RP Glavicic, M (reprint author), Rolls Royce Corp, Indianapolis, IN 46206 USA. EM michael.glavicic@rolls-royce.com; dbrown@lanl.gov; clausen@lanl.gov; tsisneros@lanl.gov; holdent@magma.ca RI Clausen, Bjorn/B-3618-2015 OI Clausen, Bjorn/0000-0003-3906-846X FU MAT (Metals Affordability Initiative) program [GE7]; Department of Energy's Office of Basic Energy Sciences; Los Alamos National Security LLC under DOE [DE-AC5206NA25396] FX We wish to acknowledge useful conversations with Dr. M. R. Hill of Hill Engineering and Dr. S. Vogel at LANSCE. Dr. O. Muransky brought the authors' attention to the slip modes in Ni3Nb and their effect in this case. The authors would like to acknowledge James Castle of the Boeing Company and Dr. Shesh Srivatsa of GE Aviation for their participation in the discussions that led to this work being conducted and partly funded in the MAT (Metals Affordability Initiative) program GE7. This work has benefifted 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. Los Alamos National Laboratory is operated by Los Alamos National Security LLC under DOE Contract DE-AC5206NA25396. NR 13 TC 0 Z9 0 U1 0 U2 4 PU TRANS TECH PUBLICATIONS LTD PI DURNTEN-ZURICH PA KREUZSTRASSE 10, 8635 DURNTEN-ZURICH, SWITZERLAND SN 0255-5476 J9 MATER SCI FORUM PY 2014 VL 777 BP 52 EP + DI 10.4028/www.scientific.net/MSF.777.52 PG 2 WC Materials Science, Multidisciplinary; Materials Science, Characterization & Testing SC Materials Science GA BA4MW UT WOS:000336006800010 ER PT S AU Brown, DW Balogh, L Byler, D Hefferan, CM Hunter, JF Kenesei, P Li, SF Lind, J Niezgoda, SR Suter, RM AF Brown, D. W. Balogh, L. Byler, D. Hefferan, C. M. Hunter, J. F. Kenesei, P. Li, S. F. Lind, J. Niezgoda, S. R. Suter, R. M. BE Holden, TM Muransky, O Hamelin, CJ TI Demonstration of Near Field High Energy X-Ray Diffraction Microscopy on High-Z Ceramic Nuclear Fuel Material SO MECHANICAL STRESS EVALUATION BY NEUTRONS AND SYNCHROTRON RADIATION VII SE Materials Science Forum LA English DT Proceedings Paper CT 7th International Conference on Mechanical Stress Evaluation by Neutrons and Synchrotron Radiation CY SEP 10-12, 2013 CL Sydney, AUSTRALIA DE Urania; Porosity; Tomography; High Energy X-ray Diffraction Microscopy ID THERMAL-CONDUCTIVITY; PARALLEL ALGORITHMS; UO2; SOFTWARE; MICROSTRUCTURE; RECONSTRUCTION; MIGRATION; POROSITY; KINETICS AB Near-field high energy x-ray diffraction microscopy (nf-HEDM) and high energy x-ray micro-tomography (mu T) have been utilized to characterize the pore structure and grain morphology in sintered ceramic UO2 nuclear fuel material. mu T successfully images pores to 2-3 mu m diameters and is analyzed to produce a pore size distribution. It is apparent that the largest number of pores and pore volume in the sintered ceramic are below the current resolution of the technique, which might be more appropriate to image cracks in the same ceramics. Grain orientation maps of slices determined by nf-HEDM at 25 pm intervals are presented and analyzed in terms of grain boundary misorientation angle. The benefit of these two techniques is that they are non-destructive and thus could be performed before and after processes (such as time at temperature or in-reactor) or even in-situ. C1 [Brown, D. W.; Byler, D.; Hunter, J. F.] Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87544 USA. [Balogh, L.] Queens Univ, Kingston, ON K7L 3N6, Canada. [Hefferan, C. M.] R J Lee Grp, Pittsburgh, PA 15146 USA. [Kenesei, P.] Argonne Natl Lab, Argonne, IL 60439 USA. [Li, S. F.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. [Lind, J.; Suter, R. M.] Carnegie Mellon Univ, Pittsburgh, PA 15213 USA. [Niezgoda, S. R.] Ohio State Univ, Columbus, OH 43210 USA. RP Brown, DW (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87544 USA. EM dbrown@lanl.gov RI Niezgoda, Stephen/I-6750-2013; Balogh, Levente/S-1238-2016 OI Niezgoda, Stephen/0000-0002-7123-466X; NR 27 TC 3 Z9 3 U1 0 U2 7 PU TRANS TECH PUBLICATIONS LTD PI DURNTEN-ZURICH PA KREUZSTRASSE 10, 8635 DURNTEN-ZURICH, SWITZERLAND SN 0255-5476 J9 MATER SCI FORUM PY 2014 VL 777 BP 112 EP + DI 10.4028/www.scientific.net/MSF.777.112 PG 3 WC Materials Science, Multidisciplinary; Materials Science, Characterization & Testing SC Materials Science GA BA4MW UT WOS:000336006800019 ER PT S AU Lee, SY Woo, W Gharghouri, MA Yoon, C An, K AF Lee, Soo Yeol Woo, Wanchuck Gharghouri, Michael A. Yoon, Cheol An, Ke BE Holden, TM Muransky, O Hamelin, CJ TI Micromechanical Behavior of Solid-Solution-Strengthened Mg-1wt.%Al Alloy Investigated by In-Situ Neutron Diffraction SO MECHANICAL STRESS EVALUATION BY NEUTRONS AND SYNCHROTRON RADIATION VII SE Materials Science Forum LA English DT Proceedings Paper CT 7th International Conference on Mechanical Stress Evaluation by Neutrons and Synchrotron Radiation CY SEP 10-12, 2013 CL Sydney, AUSTRALIA DE Magnesium; Internal strain; Twinning; Texture; Neutron diffraction ID MAGNESIUM ALLOY; DEFORMATION; AZ31B; SLIP AB In-situ neutron diffraction experiments were employed to investigate the micromechanical behavior of solid-solution-strengthened Mg-1wt.%Al alloy. Two starting textures were used: 1) as-extruded then solutionized texture, T1, in which the basal poles of most grains are tilted around 70 similar to 85 degrees from the extrusion axis, and 2) a reoriented texture, T2, in which the basal poles of most gains are tilted around 10 similar to 20 degrees from the extrusion axis. Lattice strains and diffraction peak intensity variations were measured in situ during loading-unloading cycles in uniaxial tension. Twinning activities and stress states for various grain orientations were revealed. The results show that the soft grain orientations, favorably oriented for either extension twinning or basal slip, exhibit stress relaxation, resulting in compressive residual strain after unloading. On the other hand, the hard grain orientations, unfavorably oriented for both extension twinning and basal slip, carry more applied load, leading to much higher lattice strains during loading followed by tensile residual strains upon unloading. C1 [Lee, Soo Yeol; Yoon, Cheol] Chungnam Natl Univ, Dept Mat Sci & Engn, Taejon 305764, South Korea. [Woo, Wanchuck] Korea Atom Energy Res Inst, Div Neutron Sci, Taejon 305353, South Korea. [Gharghouri, Michael A.] Chalk River Labs, Canadian Neutron Beam Ctr, Chalk River, ON K0J 1J0, Canada. [An, Ke] Oak Ridge Natl Lab, Chem & Engn Mat Div, Oak Ridge, TN 37831 USA. RP Lee, SY (reprint author), Chungnam Natl Univ, Dept Mat Sci & Engn, Taejon 305764, South Korea. EM sylee2012@cnu.ac.kr; chuckwoo@kaeri.re.kr; Michael.Gharghouri@nrc.gc.ca; yc2013@cnu.ac.kr; kean@ornl.gov OI WOO, Wanchuck/0000-0003-0350-5357; An, Ke/0000-0002-6093-429X FU National Research Foundation of Korea (NRF); Korean government (MSIP) [2012M2B2A4029572]; Office of Basic Energy Sciences; Department of Energy (DOE) FX This work was supported by the National Research Foundation of Korea (NRF) grant funded by the Korean government (MSIP) (No. 2012M2B2A4029572). Research conducted at SNS was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, Department of Energy (DOE). The authors would like to thank Mr. W. Wu, Mr. H. Skorpenske and Dr. L. Yang for their help during experiments. NR 13 TC 1 Z9 1 U1 1 U2 4 PU TRANS TECH PUBLICATIONS LTD PI DURNTEN-ZURICH PA KREUZSTRASSE 10, 8635 DURNTEN-ZURICH, SWITZERLAND SN 0255-5476 J9 MATER SCI FORUM PY 2014 VL 777 BP 130 EP + DI 10.4028/www.scientific.net/MSF.777.130 PG 3 WC Materials Science, Multidisciplinary; Materials Science, Characterization & Testing SC Materials Science GA BA4MW UT WOS:000336006800022 ER PT J AU Zhou, XW Jones, RE Hopkins, PE Beechem, TE AF Zhou, Xiao-wang Jones, Reese E. Hopkins, Patrick E. Beechem, Thomas E. TI Thermal boundary conductance between Al films and GaN nanowires investigated with molecular dynamics SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID SOLID-SOLID INTERFACES; PHONON-SCATTERING; SINGLE GAN; TRANSPORT; CONDUCTIVITY; SIMULATION; NANOSTRUCTURES; RESISTANCE AB GaN nanowires are being pursued for optoelectronic and high-power applications. In either use, increases in operating temperature reduce both performance and reliability making it imperative to minimize thermal resistances. Since interfaces significantly influence the thermal response of nanosystems, the thermal boundary resistance between GaN nanowires and metal contacts has major significance. In response, we have performed systematic molecular dynamics simulations to study the thermal boundary conductance between GaN nanowires and Al films as a function of nanowire dimensions, packing density, and the depth the nanowire is embedded into the metal contact. At low packing densities, the apparent Kapitza conductance between GaN nanowires and an aluminum film is shown to be larger than when contact is made between films of these same materials. This enhancement decreases toward the film-film limit, however, as the packing density increases. For densely packed nanowires, maximizing the Kapitza conductance can be achieved by embedding the nanowires into the films, as the conductance is found to be proportional to the total contact area. C1 [Zhou, Xiao-wang; Jones, Reese E.] Sandia Natl Labs, Mech Mat Dept, Livermore, CA 94550 USA. [Hopkins, Patrick E.] Univ Virginia, Dept Mech & Aerosp Engn, Charlottesville, VA 22904 USA. [Beechem, Thomas E.] Sandia Natl Labs, Nanoscale Sci Dept, Albuquerque, NM 87185 USA. RP Jones, RE (reprint author), Sandia Natl Labs, Mech Mat Dept, Livermore, CA 94550 USA. EM rjones@sandia.gov FU Office of Naval Research Young Investigator Program [N00014-3-0528]; Commonwealth Research Commercialization Fund of Virginia; 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. This work was performed under a Laboratory Directed Research and Development (LDRD) project. PEH is also appreciative for funding from the Office of Naval Research Young Investigator Program (N00014-3-0528) and support from the Commonwealth Research Commercialization Fund of Virginia. NR 57 TC 5 Z9 5 U1 5 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 2014 VL 16 IS 20 BP 9403 EP 9410 DI 10.1039/c4cp00261j PG 8 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AH0OC UT WOS:000335818600023 PM 24722642 ER PT J AU Darkins, R Sushko, ML Liu, J Duffy, DM AF Darkins, Robert Sushko, Maria L. Liu, Jun Duffy, Dorothy M. TI Stress in titania nanoparticles: an atomistic study SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID MOLECULAR-DYNAMICS SIMULATIONS; DECAHEDRAL GOLD NANOPARTICLES; MECHANICAL DEFORMATION; OPTICAL-PROPERTIES; ELASTIC STRAIN; VIRIAL STRESS; TIO2; NANOCRYSTALS; ENERGY; GAN AB Stress engineering is becoming an increasingly important method for controlling electronic, optical, and magnetic properties of nanostructures, although the concept of stress is poorly defined at the nanoscale. We outline a procedure for computing bulk and surface stress in nanoparticles using atomistic simulation. The method is applicable to ionic and non-ionic materials alike and may be extended to other nanostructures. We apply it to spherical anatase nanoparticles ranging from 2 to 6 nm in diameter and obtain a surface stress of 0.89 N m(-1), in agreement with experimental measurements. Based on the extent that stress inhomogeneities at the surface are transmitted into the bulk, two characteristic length-scales are identified: below 3 nm bulk and surface regions cannot be defined and the available analytic theories for stress are not applicable, and above about 5 nm the stress becomes well-described by the theoretical Young-Laplace equation. The effect of a net surface charge on the bulk stress is also investigated. It is found that moderate surface charges can induce significant bulk stresses, on the order of 100 MPa, in nanoparticles within this size range. C1 [Darkins, Robert; Duffy, Dorothy M.] UCL, UCL Phys & Astron, London, England. [Sushko, Maria L.; Liu, Jun] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Duffy, DM (reprint author), UCL, UCL Phys & Astron, London, England. EM d.duffy@ucl.ac.uk RI Sushko, Maria/C-8285-2014 OI Sushko, Maria/0000-0002-7229-7072 FU EPSRC under the Molecular Modelling and Materials Science Industrial Doctorate Centre for developing methodology for stress simulations in nanoparticles; US Department of Energy (DOE), Office of Basic Energy Sciences, Division of Materials Sciences and Engineering [KC020105-FWP12152]; DOE; Battelle [DE-AC05-76RL01830] FX RD acknowledges funding from EPSRC under the Molecular Modelling and Materials Science Industrial Doctorate Centre for developing methodology for stress simulations in nanoparticles and the US Department of Energy (DOE), Office of Basic Energy Sciences, Division of Materials Sciences and Engineering, under Award KC020105-FWP12152 for studying titania nanoparticles. MLS and JL acknowledge DOE support under the same award. PNNL is a multiprogram national laboratory operated for DOE by Battelle under Contract DE-AC05-76RL01830. NR 59 TC 4 Z9 4 U1 1 U2 27 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 2014 VL 16 IS 20 BP 9441 EP 9447 DI 10.1039/c3cp54357a PG 7 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AH0OC UT WOS:000335818600027 PM 24724152 ER PT J AU Baggetto, L Hah, HY Johnson, CE Bridges, CA Johnson, JA Veith, GM AF Baggetto, Loic Hah, Hien-Yoong Johnson, Charles E. Bridges, Craig A. Johnson, Jacqueline A. Veith, Gabriel M. TI The reaction mechanism of FeSb2 as anode for sodium-ion batteries SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID X-RAY-DIFFRACTION; LI-ION; NEGATIVE ELECTRODES; THIN-FILMS; MOSSBAUER-SPECTROSCOPY; CRYSTAL STRUCTURE; HIGH-CAPACITY; MARCASITE; SYSTEM; TIN AB The electrochemical reaction of FeSb2 with Na is reported for the first time. The first discharge (sodiation) potential profile of FeSb2 is characterized by a gentle slope centered at 0.25 V. During charge (Na removal) and the subsequent discharge, the main reaction takes place near 0.7 V and 0.4 V, respectively. The reversible storage capacity amounts to 360 mA h g(-1), which is smaller than the theoretical value of 537 mA h g(-1). The reaction, studied by ex situ and in situ X-ray diffraction, is found to proceed by the consumption of crystalline FeSb2 to form an amorphous phase. Upon further sodiation, the formation of nanocrystalline Na3Sb domains is evidenced. During desodiation, Na3Sb domains convert into an amorphous phase. The chemical environment of Fe, probed by Fe-57 Mossbauer spectroscopy, undergoes significant changes during the reaction. During sodiation, the well-resolved doublet of FeSb2 with an isomer shift around 0.45 mm s(-1) and a quadrupole splitting of 1.26 mm s(-1) is gradually converted into a doublet line centered at about 0.15 mm s(-1) along with a singlet line around 0 mm s(-1). The former signal results from the formation of a Fe-rich FexSb alloy with an estimated composition of 'Fe4Sb' while the latter signal corresponds to superparamagnetic Fe due to the formation of nanosized pure Fe domains. Interestingly the signal of 'Fe4Sb' remains unaltered during desodiation. This mechanism is substantially different than that observed during the reaction with Li. The irreversible formation of a Fe-rich 'Fe4Sb' alloy and the absence of full desodiation of Sb domains explain the lower than theoretical practical storage capacity. C1 [Baggetto, Loic; Veith, Gabriel M.] Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. [Hah, Hien-Yoong; Johnson, Charles E.] Univ Tennessee, Inst Space, Ctr Laser Applicat, Tullahoma, TN 37388 USA. [Hah, Hien-Yoong; Johnson, Jacqueline A.] Univ Tennessee, Inst Space, Dept Mech Aeronaut & Biomed Engn, Tullahoma, TN 37388 USA. [Bridges, Craig A.] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. RP Baggetto, L (reprint author), Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. EM loic_baggetto@yahoo.fr; veithgm@ornl.gov RI Johnson, Jacqueline/P-4844-2014; Baggetto, Loic/D-5542-2017 OI Johnson, Jacqueline/0000-0003-0830-9275; Baggetto, Loic/0000-0002-9029-2363 FU U.S. Department of Energy (DOE), Basic Energy Sciences (BES), Materials Sciences and Engineering Division; Center for Laser Applications; University of Tennessee Space Institute FX LB, CAB and GMV acknowledge the support of the U.S. Department of Energy (DOE), Basic Energy Sciences (BES), Materials Sciences and Engineering Division. HYH, CEJ and JAJ would like to acknowledge support from the Center for Laser Applications and the University of Tennessee Space Institute. NR 43 TC 24 Z9 24 U1 13 U2 109 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 2014 VL 16 IS 20 BP 9538 EP 9545 DI 10.1039/c4cp00738g PG 8 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AH0OC UT WOS:000335818600038 PM 24727860 ER PT J AU Mardirossian, N Head-Gordon, M AF Mardirossian, Narbe Head-Gordon, Martin TI omega B97X-V: A 10-parameter, range-separated hybrid, generalized gradient approximation density functional with nonlocal correlation, designed by a survival-of-the-fittest strategy SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID CONSISTENT BASIS-SETS; GAUSSIAN-BASIS SETS; HOLE DIPOLE-MOMENT; EXCHANGE-CORRELATION FUNCTIONALS; BENCHMARK INTERACTION ENERGIES; INHOMOGENEOUS ELECTRON-GAS; MAIN-GROUP THERMOCHEMISTRY; MOLECULAR-ORBITAL METHODS; COORDINATE-SPACE MODEL; HARTREE-FOCK MODEL AB A 10-parameter, range-separated hybrid (RSH), generalized gradient approximation (GGA) density functional with nonlocal correlation (VV10) is presented. Instead of truncating the B97-type power series inhomogeneity correction factors (ICF) for the exchange, same-spin correlation, and opposite-spin correlation functionals uniformly, all 16383 combinations of the linear parameters up to fourth order (m = 4) are considered. These functionals are individually fit to a training set and the resulting parameters are validated on a primary test set in order to identify the 3 optimal ICF expansions. Through this procedure, it is discovered that the functional that performs best on the training and primary test sets has 7 linear parameters, with 3 additional nonlinear parameters from range-separation and nonlocal correlation. The resulting density functional, omega B97X-V, is further assessed on a secondary test set, the parallel-displaced coronene dimer, as well as several geometry datasets. Furthermore, the basis set dependence and integration grid sensitivity of omega B97X-V are analyzed and documented in order to facilitate the use of the functional. C1 [Head-Gordon, Martin] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. RP Head-Gordon, M (reprint author), Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. EM mhg@cchem.berkeley.edu FU Director, Office of Energy Research, Office of Basic Energy Sciences, Chemical Sciences Division of the U.S. Department of Energy [DE-AC0376SF00098]; SciDac Program; NSF [CHE-1048789] FX This work was supported by the Director, Office of Energy Research, Office of Basic Energy Sciences, Chemical Sciences Division of the U.S. Department of Energy under Contract DE-AC0376SF00098, and by a grant from the SciDac Program. We acknowledge computational resources obtained under NSF award CHE-1048789. NR 140 TC 70 Z9 70 U1 5 U2 49 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 2014 VL 16 IS 21 BP 9904 EP 9924 DI 10.1039/c3cp54374a PG 21 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AH2BD UT WOS:000335924800018 PM 24430168 ER PT J AU Panchenko, A Tartakovsky, A Cooper, K AF Panchenko, Alexander Tartakovsky, Alexandre Cooper, Kevin TI DISCRETE MODELS OF FLUIDS: SPATIAL AVERAGING, CLOSURE, AND MODEL REDUCTION SO SIAM JOURNAL ON APPLIED MATHEMATICS LA English DT Article DE multiscale computational methods; upscaling; model reduction; dimension reduction; Irving-Kirkwood procedure; Hardy-Murdoch averaging; deconvolution closure ID SMOOTHED PARTICLE HYDRODYNAMICS; MICROSCOPIC PERSPECTIVE; DIFFERENTIAL-EQUATIONS; PHYSICAL FOUNDATIONS; CONTINUUM-MECHANICS; MOLECULAR-DYNAMICS; REACTIVE TRANSPORT; FLOWS; SIMULATIONS; SEPARATION AB We consider semidiscrete ODE models of single-phase fluids and two-fluid mixtures. In the presence of multiple fine-scale heterogeneities, the size of these ODE systems can be very large. Spatial averaging is then a useful tool for reducing computational complexity of the problem. The averages satisfy exact balance equations of mass, momentum, and energy. These equations do not form a satisfactory continuum model because evaluation of stress and heat flux requires solving the underlying ODEs. To produce continuum equations that can be simulated without resolving microscale dynamics, we recently proposed a closure method based on the use of regularized deconvolution. Here we continue the investigation of deconvolution closure with the long term objective of developing consistent computational upscaling for multiphase particle methods. The structure of the fine-scale particle solvers is reminiscent of molecular dynamics. For this reason we use nonlinear averaging introduced for atomistic systems by Noll, Hardy, and Murdoch-Bedeaux. We also consider a simpler linear averaging originally developed in large eddy simulation of turbulence. We present several simple but representative examples of spatially averaged ODEs, where the closure error can be analyzed. Based on this analysis we suggest a general strategy for reducing the relative error of approximate closure. For problems with periodic highly oscillatory material parameters we propose a spectral boosting technique that augments the standard deconvolution and helps to correctly account for dispersion effects. We also conduct several numerical experiments, one of which is a complete mesoscale simulation of a stratified two-fluid flow in a channel. In this simulation, the operation count per coarse time step scales sublinearly with the number of particles. C1 [Panchenko, Alexander; Cooper, Kevin] Washington State Univ, Dept Math, Pullman, WA 99164 USA. [Tartakovsky, Alexandre] Pacific NW Natl Lab, Computat Math Grp, Richland, WA 99352 USA. RP Panchenko, A (reprint author), Washington State Univ, Dept Math, Pullman, WA 99164 USA. EM panchenko@math.wsu.edu; alexandre.tartakovsky@pnl.gov; kcooper@math.wsu.edu NR 68 TC 1 Z9 1 U1 1 U2 11 PU SIAM PUBLICATIONS PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA SN 0036-1399 EI 1095-712X J9 SIAM J APPL MATH JI SIAM J. Appl. Math. PY 2014 VL 74 IS 2 BP 477 EP 515 DI 10.1137/12089346X PG 39 WC Mathematics, Applied SC Mathematics GA AH0PE UT WOS:000335821700012 ER PT J AU Sangoro, JR Iacob, C Agapov, AL Wang, Y Berdzinski, S Rexhausen, H Strehmel, V Friedrich, C Sokolov, AP Kremer, F AF Sangoro, J. R. Iacob, C. Agapov, A. L. Wang, Y. Berdzinski, S. Rexhausen, H. Strehmel, V. Friedrich, C. Sokolov, A. P. Kremer, F. TI Decoupling of ionic conductivity from structural dynamics in polymerized ionic liquids SO SOFT MATTER LA English DT Article ID VISCOELASTIC BEHAVIOR; POLY(IONIC LIQUID)S; CHARGE-TRANSPORT AB Charge transport and structural dynamics in low molecular weight and polymerized 1-vinyl-3-pentylimidazolium bis(trifluoromethylsulfonyl) imide ionic liquids (ILs) are investigated by a combination of broadband dielectric spectroscopy, dynamic mechanical spectroscopy and differential scanning calorimetry. While the dc conductivity and fluidity exhibit practically identical temperature dependence for the non-polymerized IL, a significant decoupling of ionic conduction from structural dynamics is observed for the polymerized IL. In addition, the dc conductivity of the polymerized IL exceeds that of its molecular counterpart by four orders of magnitude at their respective calorimetric glass transition temperatures. This is attributed to the unusually high mobility of the anions especially at lower temperatures when the structural dynamics is significantly slowed down. A simple physical explanation of the possible origin of the remarkable decoupling of ionic conductivity from structural dynamics is proposed. C1 [Sangoro, J. R.] Univ Tennessee, Dept Chem & Biomol Engn, Knoxville, TN 37996 USA. [Iacob, C.; Kremer, F.] Univ Leipzig, Inst Expt Phys 1, D-04103 Leipzig, Germany. [Berdzinski, S.; Strehmel, V.] Hsch Niederrhein Univ Appl Sci, Dept Chem, D-47798 Krefeld, Germany. [Berdzinski, S.; Strehmel, V.] Hsch Niederrhein Univ Appl Sci, Inst Coatings & Surface Chem, D-47798 Krefeld, Germany. [Rexhausen, H.] Univ Potsdam, Inst Chem, D-14476 Potsdam, Germany. [Wang, Y.; Sokolov, A. P.] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37830 USA. [Agapov, A. L.; Sokolov, A. P.] Univ Tennessee, Dept Chem, Knoxville, TN 37996 USA. [Agapov, A. L.; Sokolov, A. P.] Univ Tennessee, Dept Phys & Astron, Knoxville, TN 37996 USA. [Friedrich, C.] Univ Freiburg I Br, Freiburger Mat Forschungszentrum, Freiburg, Germany. [Friedrich, C.] Univ Freiburg I Br, Inst Makromol Chem Albert Ludwigs, Freiburg, Germany. RP Sangoro, JR (reprint author), Univ Tennessee, Dept Chem & Biomol Engn, Knoxville, TN 37996 USA. EM jsangoro@utk.edu RI Wang, Yangyang/A-5925-2010; Iacob, Ciprian/Q-7812-2016; Sangoro, Joshua/A-6573-2011 OI Wang, Yangyang/0000-0001-7042-9804; Sangoro, Joshua/0000-0002-5483-9528 FU Deutsche Forschungsgemeinschaft under the DFG SPP 1191 Priority Program on Ionic Liquids; NSF Chemistry program [CHE-1213444]; University of Potsdam for mass spectrometric investigation; Fraunhofer Institute for Applied Polymer Research Potsdam-Golm FX JRS acknowledges The University of Tennessee-Knoxville for tenure-track faculty start-up funds. CI, SB, RH, VS, and FK gratefully acknowledge financial support from the Deutsche Forschungsgemeinschaft under the DFG SPP 1191 Priority Program on Ionic Liquids. ALA, YW and APS thanks NSF Chemistry program (grant CHE-1213444) for financial support. The authors also thank Jorg Karger and Rustem Valliulin for PFG NMR measurement of the PIL reported in this article. JRS thanks T. Saito for critically reading the manuscript. Furthermore, VS and SB would like gratefully to acknowledge the group of E. Kleinpeter, especially I. Starke and S. Furstenberg from the University of Potsdam for mass spectrometric investigation, E. Gornitz and K. Blumel (Fraunhofer Institute for Applied Polymer Research Potsdam-Golm) for support during viscosity measurements, and H. Wetzel (Fraunhofer Institute for Applied Polymer Research Potsdam-Golm) for analysis of the water content in the ionic liquid by Karl-Fischer analysis. NR 28 TC 22 Z9 22 U1 9 U2 73 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 2014 VL 10 IS 20 BP 3536 EP 3540 DI 10.1039/c3sm53202j PG 5 WC Chemistry, Physical; Materials Science, Multidisciplinary; Physics, Multidisciplinary; Polymer Science SC Chemistry; Materials Science; Physics; Polymer Science GA AH2CD UT WOS:000335927400002 PM 24718358 ER PT J AU Zhang, XH Yager, KG Douglas, JF Karim, A AF Zhang, Xiaohua Yager, Kevin G. Douglas, Jack F. Karim, Alamgir TI Suppression of target patterns in domain aligned cold-zone annealed block copolymer films with immobilized film-spanning nanoparticles SO SOFT MATTER LA English DT Article ID THIN-FILMS; DIBLOCK COPOLYMERS; ORDER; TEMPERATURE; BLENDS; AGGREGATION; CONFINEMENT; ALIGNMENT; POLYMERS; DISORDER AB We examine the effect of a moving in-plane temperature gradient on the ordering of cylinder- forming block-copolymers (BCP) in films containing immobilized nanoparticles that span the film thickness. In a previous paper, we reported the effect of static step oven-annealing of these films above the glass transition temperature T-g for a long period before ordering the BCP film at a much higher temperature. In the dynamic film annealing method of the present work, termed cold zone annealing (CZA), the material is continuously raised to a temperature somewhat above the glass transition temperature and then well above it, with a control of the heating time and thermal gradient. Oven annealing before ordering has been found to relieve residual stresses in the film associated with large thermal expansion of the film upon heating, eliminating the large scale target patterns induced by stresses effects associated with residual solvent and thermal expansion. By comparison, CZA naturally suppresses undesirable target patterning with enhanced ordering kinetics created through this thermal history. C1 [Zhang, Xiaohua] Soochow Univ, Ctr Soft Condensed Matter Phys & Interdisciplinar, Suzhou 215006, Peoples R China. [Yager, Kevin G.] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. [Douglas, Jack F.] NIST, Div Engn & Mat Sci, Mat Measurement Lab, Gaithersburg, MD 20899 USA. [Karim, Alamgir] Univ Akron, Dept Polymer Engn, Akron, OH 44325 USA. RP Zhang, XH (reprint author), Soochow Univ, Ctr Soft Condensed Matter Phys & Interdisciplinar, Suzhou 215006, Peoples R China. EM zhangxiaohua@suda.edu.cn; alamgir@uakron.edu RI Yager, Kevin/F-9804-2011 OI Yager, Kevin/0000-0001-7745-2513 FU National Basic Research Program of China (973 Program) [2012CB821505]; National Natural Science Foundation of China [91027040, 21274103, 21104054]; U.S. Department of Energy, Office of Basic Energy Sciences [DE-AC02-98CH10886]; National Science Foundation, Division of Materials Research [NSF DMR-1006421] FX The authors acknowledge financial support of National Basic Research Program of China (973 Program) (no. 2012CB821505), and National Natural Science Foundation of China (no. 91027040, no. 21274103, and no. 21104054). The Center for Functional Nanomaterials, Brookhaven National Laboratory, is supported by the U.S. Department of Energy, Office of Basic Energy Sciences, under Contract no. DE-AC02-98CH10886. This CZA work was supported by the National Science Foundation, Division of Materials Research, Grant NSF DMR-1006421. We also wish to thank Brian Berry for help with the CZA measurements. NR 40 TC 3 Z9 3 U1 0 U2 14 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 2014 VL 10 IS 20 BP 3656 EP 3666 DI 10.1039/c4sm00238e PG 11 WC Chemistry, Physical; Materials Science, Multidisciplinary; Physics, Multidisciplinary; Polymer Science SC Chemistry; Materials Science; Physics; Polymer Science GA AH2CD UT WOS:000335927400014 PM 24676041 ER PT S AU Crainic, TG Gobbato, L Perboli, G Rei, W Watson, JP Woodruff, DL AF Crainic, Teodor Gabriel Gobbato, Luca Perboli, Guido Rei, Walter Watson, Jean-Paul Woodruff, David L. BE DeSousa, JF DeSousa, JP Costa, A Farias, T Melo, S TI Bin Packing Problems with uncertainty on item characteristics: an application to capacity planning in logistics SO TRANSPORTATION: CAN WE DO MORE WITH LESS RESOURCES? - 16TH MEETING OF THE EURO WORKING GROUP ON TRANSPORTATION - PORTO 2013 SE Procedia Social and Behavioral Sciences LA English DT Proceedings Paper CT 16th Meeting of the Euro-Working-Group-in-Transportation CY SEP, 2013 CL Porto, PORTUGAL SP Euro Working Grp Transportat DE Stochastic Bin Packing; logistics capacity planning; supply chain; third party logistic AB Most modem companies are part of international economic networks, where goods are produced under different strategies, then transported over long distances and stored for variable periods of time at different locations along the considered network. These activities are often performed by first consolidating goods in appropriate bins, which are then stored at warehouses and shipped using multiple vehicles through various transportation modes. Companies thus face the problem of planning for sufficient capacity, e.g., negotiating it with third party logistic firms (3PLs) that specify both the capacity to be used and the logistical services to be performed. Given the time lag that usually exists between the capacity-planning decisions and the operational decisions that define how the planned capacity is used, the common assumption that all information concerning the parameters of the model is known is unlikely to be observed. We therefore propose a new stochastic problem, named the Variable Cost and Size Bin Packing Problem with Stochastic Items. The problem considers a company making a tactical capacity plan by choosing a set of appropriate bins, which are defined according to their specific volume and fixed cost. Bins included in the capacity plan are chosen in advance without the exact knowledge of what items will be available for the dispatching. When, during the operational phase, the planned capacity is not sufficient, extra capacity must be purchased. An extensive experimental plan is used to analyze the impact that diversity in instance structure has on the capacity planning and the effect of considering different levels of variability and correlation of the stochastic parameters related to items. (C) 2013 The Authors. Published by Elsevier Ltd. C1 [Gobbato, Luca; Perboli, Guido] DAUIN Politecn Torino, Turin, Italy. [Crainic, Teodor Gabriel; Perboli, Guido; Rei, Walter] CIRRELT, Montreal, PQ, Canada. [Rei, Walter] Univ Quebec Montreal, Sch Management, Montreal, PQ, Canada. [Crainic, Teodor Gabriel; Rei, Walter; Woodruff, David L.] Sandia Natl Labs, Albuquerque, NM 87185 USA. [Woodruff, David L.] Univ Calif Davis, Grad Sch Management, Davis, CA USA. RP Gobbato, L (reprint author), DAUIN Politecn Torino, Turin, Italy. EM luca.gobbato@polito.it FU Minister dell'Istruzione; Univers ta c Ricerca - MIUR (Italian Ministry of University and Research); Natural Sciences and Engineering Council of Canada (NSERC) FX Partial funding was provided by the Minister dell'Istruzione, Univers ta c Ricerca - MIUR (Italian Ministry of University and Research), under the 2009 PRIN Project "Methods and Algorithms for the Logistics Optimization", by the Natural Sciences and Engineering Council of Canada (NSERC), and the Fonds de recherche du Quebec-Nature et technologies (FRONT). NR 19 TC 1 Z9 1 U1 1 U2 5 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA SARA BURGERHARTSTRAAT 25, PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 1877-0428 J9 PROCD SOC BEHV PY 2014 VL 111 BP 654 EP 662 DI 10.1016/j.sbspro.2014.01.099 PG 9 WC Transportation SC Transportation GA BA4FG UT WOS:000335582500067 ER PT S AU Manaa, MR Fried, LE AF Manaa, M. Riad Fried, Laurence E. BE Sabin, JR TI The Reactivity of Energetic Materials Under High Pressure and Temperature SO ADVANCES IN QUANTUM CHEMISTRY, VOL 69 SE Advances in Quantum Chemistry LA English DT Review; Book Chapter ID MOLECULAR-DYNAMICS SIMULATIONS; TIGHT-BINDING METHOD; CONDENSED-PHASE DECOMPOSITION; HMX PYROLYSIS PRODUCTS; EQUATION-OF-STATE; THERMAL-DECOMPOSITION; PENTAERYTHRITOL TETRANITRATE; HYDROSTATIC COMPRESSION; LIQUID NITROMETHANE; SOLID EXPLOSIVES AB Chemical transformations that occur at the reactive shock front of energetic materials determine many aspects of material properties and performance. One major shortcoming of current explosive models is the lack of chemical kinetics data of the reacting explosive at the high pressures and, temperatures experienced under detonation conditions. In the absence of experimental data, long time-scale atomistic molecular dynamics simulations with reactive chemistry provide insight into the decomposition mechanisms of explosives and allow us to obtain effective reaction rates. These rates can then be incorporated into a thermochemical continuum code for accurate and predictive description of grain- and continuum-scale dynamics of reacting explosives. During the course of the past decade, we have examined the chemistry of several reacting explosive materials, such as the high-performing HMX and the very insensitive TATB explosives, both of which are organic molecular solids at ambient conditions. We have used quantum-based, self-consistent charge density functional tight-binding method to calculate the interatomic forces in molecular dynamics simulations either for thermal decomposition studies (constant volume temperature) or dynamical shock studies using the multiscale shock simulation technique (MSST). These studies allow us to investigate the chemical reactivity of explosives and to examine electronic properties at extreme conditions of temperature and pressure for a relatively long timescale on the order of several hundreds of picoseconds. In this chapter, we discuss challenges in simulating the reactions of shocked energetic materials and review specific examples of our recent simulations on HMX, PETN, and shocked TATB. Each of these studies revealed interesting aspects associated with known macroscopic properties of these materials. We also discuss simulations on nonenergetic materials such as shocked carbon and methane. C1 [Manaa, M. Riad; Fried, Laurence E.] Lawrence Livermore Natl Lab, Energet Mat Ctr, Livermore, CA USA. RP Fried, LE (reprint author), Lawrence Livermore Natl Lab, Energet Mat Ctr, Livermore, CA USA. EM fried1@llnl.gov RI Fried, Laurence/L-8714-2014 OI Fried, Laurence/0000-0002-9437-7700 NR 90 TC 10 Z9 10 U1 11 U2 75 PU ELSEVIER ACADEMIC PRESS INC PI SAN DIEGO PA 525 B STREET, SUITE 1900, SAN DIEGO, CA 92101-4495 USA SN 0065-3276 BN 978-0-12-800345-9 J9 ADV QUANTUM CHEM JI Adv. Quantum Chem. PY 2014 VL 69 BP 221 EP 252 DI 10.1016/B978-0-12-800345-9.00006-4 PG 32 WC Chemistry, Physical SC Chemistry GA BA1PN UT WOS:000332802600006 ER PT J AU Cui, YJ Abouimrane, A Sun, CJ Ren, Y Amine, K AF Cui, Yanjie Abouimrane, Ali Sun, Cheng-Jun Ren, Yang Amine, Khalil TI Li-Se battery: absence of lithium polyselenides in carbonate based electrolyte SO CHEMICAL COMMUNICATIONS LA English DT Article ID X-RAY-ABSORPTION; LIQUID ELECTROLYTES; SELENIUM BATTERIES; CATHODE MATERIAL; SPECTROSCOPY; COMPOSITE; SULFUR; DIFFRACTION; PERFORMANCE; DISCHARGE AB The lithiation mechanism of the Li-Se cell in a carbonate-based electrolyte is discussed. It is found that Se is directly reduced to Li2Se in discharge without intermediate phases detected by in situ X-ray diffraction or X-ray absorption spectroscopy. The reason is that the redox products Se and Li2Se, as well as lithium polyselenides are insoluble in the electrolyte. C1 [Cui, Yanjie; Abouimrane, Ali; Amine, Khalil] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. [Sun, Cheng-Jun; Ren, Yang] Argonne Natl Lab, Xray Sci Div, Adv Photon Source, Argonne, IL 60439 USA. RP Abouimrane, A (reprint author), Argonne Natl Lab, Chem Sci & Engn Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM abouimrane@anl.gov FU U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]; U.S. DOE - Basic Energy Sciences; Canadian Light Source; University of Washington; APS; DOE Vehicle Technologies Program within the core funding of the Applied Battery Research for Transportation Program FX Work done at Argonne National Laboratory and use of the Advanced Photon Source (APS) and the Raman instrument at the Center for Nanoscale Materials are supported by the U. S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. PNC/XSD facilities at the APS, and research at these facilities, are supported by the U.S. DOE - Basic Energy Sciences, the Canadian Light Source and its funding partners, the University of Washington, and the APS. The pouch cells were produced at the U.S. DOE Cell Fabrication Facility (CFF), ANL. The CFF is fully supported by the DOE Vehicle Technologies Program within the core funding of the Applied Battery Research for Transportation Program. NR 22 TC 36 Z9 36 U1 15 U2 107 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 2014 VL 50 IS 42 BP 5576 EP 5579 DI 10.1039/c4cc00934g PG 4 WC Chemistry, Multidisciplinary SC Chemistry GA AG5LP UT WOS:000335460800010 PM 24722685 ER PT S AU Bingham, PR Santos-Villalobos, H Lavrik, N Bilheux, H Gregor, J AF Bingham, Philip R. Santos-Villalobos, Hector Lavrik, Nickolay Bilheux, Hassina Gregor, Jens BE Bouman, CA Sauer, KD TI Magnified neutron radiography with coded sources SO COMPUTATIONAL IMAGING XII SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Computational Imaging XII CY FEB 05-06, 2014 CL San Francisco, CA SP Soc Imaging Sci & Technol, SPIE AB A coded source imaging system has been developed to improve resolution for neutron radiography through magnification and demonstrated at the High Flux Isotope Reactor (HFIR) CG-1D instrument. Without magnification, the current resolution at CG-1D is 80 mu m using a charge-coupled device (CCD) equipped with a lens. As for all neutron imaging instruments, magnification is limited by a large source size. At CG-1D the size is currently limited to 12mm with a circular aperture. Coded source imaging converts this large aperture into a coded array of smaller apertures to achieve high resolution without the loss of flux for a single pinhole aperture, but requires a decoding step. The developed system has demonstrated first magnified radiographic imaging at magnifications as high as 25x using coded apertures with holes as small as 10 mu m. Such a development requires a team with a broad base of expertise including imaging systems design, neutron physics, microelectronics manufacturing methods, reconstruction algorithms, and high performance computing. The paper presents the system design, discusses implementation challenges, and presents imaging results. C1 [Bingham, Philip R.; Santos-Villalobos, Hector; Lavrik, Nickolay; Bilheux, Hassina] Oak Ridge Natl Lab, Oak Ridge, TN 37830 USA. [Gregor, Jens] Univ Tennessee, Knoxville, TN USA. RP Bingham, PR (reprint author), Oak Ridge Natl Lab, Oak Ridge, TN 37830 USA. RI Bilheux, Hassina/H-4289-2012; Lavrik, Nickolay/B-5268-2011; OI Bilheux, Hassina/0000-0001-8574-2449; Lavrik, Nickolay/0000-0002-9543-5634; Bingham, Philip/0000-0003-4616-6084 NR 12 TC 0 Z9 0 U1 0 U2 3 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9937-0 J9 PROC SPIE PY 2014 VL 9020 AR UNSP 90200A DI 10.1117/12.2044587 PG 10 WC Optics; Imaging Science & Photographic Technology SC Optics; Imaging Science & Photographic Technology GA BA4EF UT WOS:000335494800008 ER PT S AU Kallman, JS DePiero, S Azevedo, S Martz, HE AF Kallman, Jeffrey S. DePiero, Sabrina Azevedo, Stephen Martz, Harry E., Jr. BE Bouman, CA Sauer, KD TI Effects of Powder Morphology and Particle Size on CT Number Estimates SO COMPUTATIONAL IMAGING XII SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Computational Imaging XII CY FEB 05-06, 2014 CL San Francisco, CA SP Soc Imaging Sci & Technol, SPIE DE X-ray attenuation; particle size; powder packing; electron density AB We performed experiments and data analysis to determine how powder morphology and particle size affect X-ray attenuation (CT number or CTN). These experiments were performed on a CT system with an isotropic resolution of (0.15 mm)(3), and an endpoint energy of 160kV. Powders with effective atomic number (Z(e)) within +/- 0.2 of water were found to have CTN more directly related to electron density than to bulk physical density. Variations in mean particle size ranging between 2 mu m and 44 mu m were found to have no effect on specimen mean CTN. C1 [Kallman, Jeffrey S.; DePiero, Sabrina; Azevedo, Stephen; Martz, Harry E., Jr.] Lawrence Livermore Natl Lab, LLNL PROC 658150, Livermore, CA 94551 USA. RP Kallman, JS (reprint author), Lawrence Livermore Natl Lab, LLNL PROC 658150, POB 808, Livermore, CA 94551 USA. EM kallman1@llnl.gov NR 3 TC 1 Z9 1 U1 1 U2 1 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9937-0 J9 PROC SPIE PY 2014 VL 9020 AR 90200K DI 10.1117/12.2048876 PG 13 WC Optics; Imaging Science & Photographic Technology SC Optics; Imaging Science & Photographic Technology GA BA4EF UT WOS:000335494800016 ER PT S AU Kracher, A AF Kracher, Alfred BE Vakoch, DA TI Evolutionary Perspectives on Interstellar Communication: Images of Altruism SO EXTRATERRESTRIAL ALTRUISM: EVOLUTION AND ETHICS IN THE COSMOS SE Frontiers Collection LA English DT Article; Book Chapter DE Aesthetic strategy; Art; Convergent evolution; Iconography; Imagination; Layered messages; Madonna images ID LIFE AB At least some part of an interstellar message of altruism will be in the form of images. Designing such iconic messages will require a comprehensive dialogue among representatives of science, arts and humanities, and include non-Western traditions. As a basis for discussing the likely success (or failure) of communicating cultural concepts to extraterrestrials, we can first look at some examples how this has been done across cultures here on Earth. I use the example of religious icons on altruism, because it is an area where the repertoire of iconic messages has been studied in some detail. We can then address particular questions about using this approach in interstellar messages. How much terrestrial experience can help depends on how human-like the recipients of our message are thought to be. Some conclusions are: (a) Images have to be combined with other forms of communication. (b) Terrestrial experience can be valuable for alien recipients that are human-like, but even in this case the difference in evolutionary history is a significant barrier to understanding. (c) In the case of aliens that are not human-like it is unclear what the equivalent of altruism would be for them. (d) Sending multiple diverse messages increases our chances to be understood, but also to be misunderstood. (e) A serious effort at designing interstellar messages of altruism will have positive consequences for humanity even if no alien civilization acknowledges our transmission. C1 [Kracher, Alfred] Iowa State Univ, Ames Lab, Ames, IA USA. [Kracher, Alfred] Univ Arkansas, Arkansas Ctr Space & Planetary Sci, Fayetteville, AR 72701 USA. RP Kracher, A (reprint author), 15837 Garden View Dr, Apple Valley, MN 55124 USA. EM akracher1945@gmail.com NR 20 TC 1 Z9 1 U1 0 U2 1 PU SPRINGER PI NEW YORK PA 233 SPRING STREET, NEW YORK, NY 10013, UNITED STATES SN 1612-3018 BN 978-3-642-37749-5 J9 FRONT COLLECT PY 2014 BP 295 EP 308 DI 10.1007/978-3-642-37750-1_19 D2 10.1007/978-3-642-37750-1 PG 14 WC Astronomy & Astrophysics; Ethics SC Astronomy & Astrophysics; Social Sciences - Other Topics GA BA1NH UT WOS:000332728100020 ER PT J AU Sautter, V Fabre, C Forni, O Toplis, MJ Cousin, A Ollila, AM Meslin, PY Maurice, S Wiens, RC Baratoux, D Mangold, N Le Mouelic, S Gasnault, O Berger, G Lasue, J Anderson, RA Lewin, E Schmidt, M Dyar, D Ehlmann, BL Bridges, J Clark, B Pinet, P AF Sautter, V. Fabre, C. Forni, O. Toplis, M. J. Cousin, A. Ollila, A. M. Meslin, P. Y. Maurice, S. Wiens, R. C. Baratoux, D. Mangold, N. Le Mouelic, S. Gasnault, O. Berger, G. Lasue, J. Anderson, R. A. Lewin, E. Schmidt, M. Dyar, D. Ehlmann, B. L. Bridges, J. Clark, B. Pinet, P. TI Igneous mineralogy at Bradbury Rise: The first ChemCam campaign at Gale crater SO JOURNAL OF GEOPHYSICAL RESEARCH-PLANETS LA English DT Article DE Curiosity; Gale Crater; igneous rocks; feldspar; laser-induced breakdown spectroscopy (LIBS); ChemCam ID INSTRUMENT SUITE; MARS; SCIENCE; ROVER; CRUST; GEOCHEMISTRY; METEORITES; TARGETS; UNIT AB Textural and compositional analyses using Chemistry Camera (ChemCam) remote microimager and laser-induced breakdown spectroscopy (LIBS) have been performed on five float rocks and coarse gravels along the first 100 m of the Curiosity traverse at Bradbury Rise. ChemCam, the first LIBS instrument sent to another planet, offers the opportunity to assess mineralogic diversity at grain-size scales (similar to 100 mu m) and, from this, lithologic diversity. Depth profiling indicates that targets are relatively free of surface coatings. One type of igneous rock is volcanic and includes both aphanitic (Coronation) and porphyritic (Mara) samples. The porphyritic sample shows dark grains that are likely pyroxene megacrysts in a fine-grained mesostasis containing andesine needles. Both types have magnesium-poor basaltic compositions and in this respect are similar to the evolved Jake Matijevic rock analyzed further along the Curiosity traverse both with Alpha-Particle X-ray Spectrometer and ChemCam instruments. The second rock type encountered is a coarse-grained intrusive rock (Thor Lake) showing equigranular texture with millimeter size crystals of feldspars and Fe-Ti oxides. Such a rock is not unique at Gale as the surrounding coarse gravels (such as Beaulieu) and the conglomerate Link are dominated by feldspathic (andesine-bytownite) clasts. Finally, alkali feldspar compositions associated with a silica polymorph have been analyzed in fractured filling material of Preble rock and in Stark, a putative pumice or an impact melt. These observations document magmatic diversity at Gale and describe the first fragments of feldspar-rich lithologies (possibly an anorthosite) that may be ancient crust transported from the crater rim and now forming float rocks, coarse gravel, or conglomerate clasts. C1 [Sautter, V.] MNHN, CNRS UMR 7202, LMCM, FR-75005 Paris, France. [Fabre, C.] Univ Lorraine, CNRS UMR GeoRessources 7359, Nancy, France. [Forni, O.; Toplis, M. J.; Meslin, P. Y.; Maurice, S.; Baratoux, D.; Gasnault, O.; Berger, G.; Lasue, J.; Pinet, P.] Univ Toulouse, CNRS UMR IRAP 7277, Toulouse, France. [Cousin, A.; Wiens, R. C.] Los Alamos Natl Lab, Los Alamos, NM USA. [Ollila, A. M.] Univ New Mexico, Inst Meteorit, Albuquerque, NM 87131 USA. [Mangold, N.; Le Mouelic, S.] LPG Nantes, CNRS UMR 6112, Nantes, France. [Anderson, R. A.] US Geol Survey, Flagstaff, AZ 86001 USA. [Lewin, E.] Univ Grenoble, CNRS UMR 5275, ISTerre, Grenoble, France. [Schmidt, M.] Brock Univ, Dept Earth Sci, St Catharines, ON L2S 3A1, Canada. [Dyar, D.] Mt Holyoke Coll, Dept Astron, S Hadley, MA 01075 USA. [Ehlmann, B. L.] CALTECH, Div Geol & Planetary Sci, Pasadena, CA 91125 USA. [Bridges, J.] Univ Leicester, SRC, Leicester, Leics, England. [Clark, B.] Space Sci Inst, Boulder, CO USA. RP Sautter, V (reprint author), MNHN, CNRS UMR 7202, LMCM, 61 Rue Buffon, FR-75005 Paris, France. EM vsautter@mnhn.fr RI BERGER, Gilles/F-7118-2016; LEWIN, Eric/F-1451-2017; OI Gasnault, Olivier/0000-0002-6979-9012 FU NASA's Mars Exploration Program in the US; NASA's Mars Exploration Program in the France; Centre National d'Etudes Spatiales (CNES) FX The MSL team is gratefully acknowledged. The manuscript was greatly improved by the reviews of H.Y. McSween, M. McCanta, and H. Nekvasil, as well as editorial comments by J. Filiberto. All are warmly thanked for their help. This research was carried out with funding from NASA's Mars Exploration Program in the US and in France with the Centre National d'Etudes Spatiales (CNES). NR 58 TC 55 Z9 55 U1 3 U2 28 PU AMER GEOPHYSICAL UNION PI WASHINGTON PA 2000 FLORIDA AVE NW, WASHINGTON, DC 20009 USA SN 2169-9097 EI 2169-9100 J9 J GEOPHYS RES-PLANET JI J. Geophys. Res.-Planets PD JAN PY 2014 VL 119 IS 1 BP 30 EP 46 DI 10.1002/2013JE004472 PG 17 WC Geochemistry & Geophysics SC Geochemistry & Geophysics GA AD1YA UT WOS:000333028400003 ER PT J AU Schmidt, ME Campbell, JL Gellert, R Perrett, GM Treiman, AH Blaney, DL Olilla, A Calef, FJ Edgar, L Elliott, BE Grotzinger, J Hurowitz, J King, PL Minitti, ME Sautter, V Stack, K Berger, JA Bridges, JC Ehlmann, BL Forni, O Leshin, LA Lewis, KW McLennan, SM Ming, DW Newsom, H Pradler, I Squyres, SW Stolper, EM Thompson, L VanBommel, S Wiens, RC AF Schmidt, M. E. Campbell, J. L. Gellert, R. Perrett, G. M. Treiman, A. H. Blaney, D. L. Olilla, A. Calef, F. J., III Edgar, L. Elliott, B. E. Grotzinger, J. Hurowitz, J. King, P. L. Minitti, M. E. Sautter, V. Stack, K. Berger, J. A. Bridges, J. C. Ehlmann, B. L. Forni, O. Leshin, L. A. Lewis, K. W. McLennan, S. M. Ming, D. W. Newsom, H. Pradler, I. Squyres, S. W. Stolper, E. M. Thompson, L. VanBommel, S. Wiens, R. C. TI Geochemical diversity in first rocks examined by the Curiosity Rover in Gale Crater: Evidence for and significance of an alkali and volatile-rich igneous source SO JOURNAL OF GEOPHYSICAL RESEARCH-PLANETS LA English DT Article DE Mars geochemistry; Mars Science Laboratory; APXS; Gale Crater ID X-RAY SPECTROMETER; CHEMCAM INSTRUMENT SUITE; MEDUSAE FOSSAE FORMATION; MARTIAN MANTLE; MERIDIANI-PLANUM; GUSEV CRATER; ISOTOPIC SYSTEMATICS; PETROGENETIC MODEL; LANDING SITE; MARS AB The first four rocks examined by the Mars Science Laboratory Alpha Particle X-ray Spectrometer indicate that Curiosity landed in a lithologically diverse region of Mars. These rocks, collectively dubbed the Bradbury assemblage, were studied along an eastward traverse (sols 46-102). Compositions range from Na- and Al-rich mugearite Jake_Matijevic to Fe-, Mg-, and Zn-rich alkali-rich basalt/hawaiite Bathurst_Inlet and span nearly the entire range in FeO* and MnO of the data sets from previous Martian missions and Martian meteorites. The Bradbury assemblage is also enriched in K and moderately volatile metals (Zn and Ge). These elements do not correlate with Cl or S, suggesting that they are associated with the rocks themselves and not with salt-rich coatings. Three out of the four Bradbury rocks plot along a line in elemental variation diagrams, suggesting mixing between Al-rich and Fe-rich components. ChemCam analyses give insight to their degree of chemical heterogeneity and grain size. Variations in trace elements detected by ChemCam suggest chemical weathering (Li) and concentration in mineral phases (e.g., Rb and Sr in feldspars). We interpret the Bradbury assemblage to be broadly volcanic and/or volcaniclastic, derived either from near the Gale crater rim and transported by the Peace Vallis fan network, or from a local volcanic source within Gale Crater. High Fe and Fe/Mn in Et_Then likely reflect secondary precipitation of Fe3+ oxides as a cement or rind. The K-rich signature of the Bradbury assemblage, if igneous in origin, may have formed by small degrees of partial melting of metasomatized mantle. . C1 [Schmidt, M. E.] Brock Univ, Dept Earth Sci, St Catharines, ON L2S 3A1, Canada. [Campbell, J. L.; Gellert, R.; Perrett, G. M.; Pradler, I.; VanBommel, S.] Univ Guelph, Dept Phys, Guelph, ON N1G 2W1, Canada. [Treiman, A. H.] Lunar Planetary Sci Inst, Houston, TX USA. [Blaney, D. L.; Calef, F. J., III; Grotzinger, J.; Ehlmann, B. L.] CALTECH, Jet Prop Lab, Pasadena, CA USA. [Olilla, A.] Univ New Mexico, Inst Meteorit, Albuquerque, NM 87131 USA. [Edgar, L.] Arizona State Univ, Tempe, AZ USA. [Elliott, B. E.; Thompson, L.] Univ New Brunswick, Dept Earth Sci, Fredericton, NB, Canada. [Grotzinger, J.; Stack, K.; Ehlmann, B. L.; Stolper, E. M.] CALTECH, Pasadena, CA 91125 USA. [Hurowitz, J.] SUNY Stony Brook, Dept Geosci, Stony Brook, NY 11794 USA. [King, P. L.] Australian Natl Univ, Res Sch Earth Sci, Canberra, ACT, Australia. [Minitti, M. E.] Johns Hopkins Univ, Appl Phys Lab, Laurel, MD USA. [Sautter, V.] Museum Natl Hist Nat, F-75231 Paris, France. [Berger, J. A.] Univ Western Ontario, Dept Earth Sci, London, ON, Canada. [Bridges, J. C.] Univ Leicester, Dept Phys & Astron, Space Res Ctr, Leicester LE1 7RH, Leics, England. [Forni, O.] Univ Toulouse 3, UPS OMP, Inst Rech Astrophys & Planetol, F-31062 Toulouse, France. [Leshin, L. A.] Rensselaer Polytech Inst, Sch Sci, Troy, NY USA. [Lewis, K. W.; McLennan, S. M.] Princeton Univ, Princeton, NJ 08544 USA. [Ming, D. W.] NASA, Lyndon B Johnson Space Ctr, Houston, TX 77058 USA. [Squyres, S. W.] Cornell Univ, Dept Astron, Ithaca, NY 14853 USA. [Wiens, R. C.] Los Alamos Natl Lab, Los Alamos, NM USA. RP Schmidt, ME (reprint author), Brock Univ, Dept Earth Sci, St Catharines, ON L2S 3A1, Canada. EM mschmidt2@brocku.ca RI King, Penelope/A-1791-2011 OI King, Penelope/0000-0002-8364-9168 FU Canadian Space Agency (CSA); NASA MSL mission FX This work was funded by the Canadian Space Agency (CSA) support for the APXS instrument and Participating Scientist grant to Schmidt, and by the NASA MSL mission. Thoughtful reviews by Brian Balta, Cerena Goodrich, and Christian Schrader improved the manuscript. We sincerely thank the many engineers and scientists who have contributed to the great success of the MSL mission. NR 96 TC 48 Z9 49 U1 6 U2 48 PU AMER GEOPHYSICAL UNION PI WASHINGTON PA 2000 FLORIDA AVE NW, WASHINGTON, DC 20009 USA SN 2169-9097 EI 2169-9100 J9 J GEOPHYS RES-PLANET JI J. Geophys. Res.-Planets PD JAN PY 2014 VL 119 IS 1 BP 64 EP 81 DI 10.1002/2013JE004481 PG 18 WC Geochemistry & Geophysics SC Geochemistry & Geophysics GA AD1YA UT WOS:000333028400005 ER PT J AU Ollila, AM Newsom, HE Clark, B Wiens, RC Cousin, A Blank, JG Mangold, N Sautter, V Maurice, S Clegg, SM Gasnault, O Forni, O Tokar, R Lewin, E Dyar, MD Lasue, J Anderson, R McLennan, SM Bridges, J Vaniman, D Lanza, N Fabre, C Melikechi, N Perrett, GM Campbell, JL King, PL Barraclough, B Delapp, D Johnstone, S Meslin, PY Rosen-Gooding, A Williams, J AF Ollila, Ann M. Newsom, Horton E. Clark, Benton, III Wiens, Roger C. Cousin, Agnes Blank, Jen G. Mangold, Nicolas Sautter, Violaine Maurice, Sylvestre Clegg, Samuel M. Gasnault, Olivier Forni, Olivier Tokar, Robert Lewin, Eric Dyar, M. Darby Lasue, Jeremie Anderson, Ryan McLennan, Scott M. Bridges, John Vaniman, Dave Lanza, Nina Fabre, Cecile Melikechi, Noureddine Perrett, Glynis M. Campbell, John L. King, Penelope L. Barraclough, Bruce Delapp, Dorothea Johnstone, Stephen Meslin, Pierre-Yves Rosen-Gooding, Anya Williams, Josh CA MSL Sci Team TI Trace element geochemistry ( Li, Ba, Sr, and Rb) using Curiosity's ChemCam: Early results for Gale crater from Bradbury Landing Site to Rocknest SO JOURNAL OF GEOPHYSICAL RESEARCH-PLANETS LA English DT Article DE laser-induced breakdown spectroscopy; Mars; Gale crater; trace elements; ChemCam; Mars Science Laboratory ID INDUCED BREAKDOWN SPECTROSCOPY; X-RAY SPECTROMETER; LIGHT LITHOPHILE ELEMENTS; CHEMICAL-COMPOSITION; MARTIAN SOIL; SM-ND; ISOTOPIC COMPOSITION; INSTRUMENT SUITE; SELF-ABSORPTION; SOUTH-AFRICA AB The ChemCam instrument package on the Mars rover, Curiosity, provides new capabilities to probe the abundances of certain trace elements in the rocks and soils on Mars using the laser-induced breakdown spectroscopy technique. We focus on detecting and quantifying Li, Ba, Rb, and Sr in targets analyzed during the first 100 sols, from Bradbury Landing Site to Rocknest. Univariate peak area models and multivariate partial least squares models are presented. Li, detected for the first time directly on Mars, is generally low (<15 ppm). The lack of soil enrichment in Li, which is highly fluid mobile, is consistent with limited influx of subsurface waters contributing to the upper soils. Localized enrichments of up to similar to 60 ppm Li have been observed in several rocks but the host mineral for Li is unclear. Bathurst_Inlet is a fine-grained bedrock unit in which several analysis locations show a decrease in Li and other alkalis with depth, which may imply that the unit has undergone low-level aqueous alteration that has preferentially drawn the alkalis to the surface. Ba (similar to 1000 ppm) was detected in a buried pebble in the Akaitcho sand ripple and it appears to correlate with Si, Al, Na, and K, indicating a possible feldspathic composition. Rb and Sr are in the conglomerate Link at abundances >100 ppm and >1000 ppm, respectively. These analysis locations tend to have high Si and alkali abundances, consistent with a feldspar composition. Together, these trace element observations provide possible evidence of magma differentiation and aqueous alteration. C1 [Ollila, Ann M.; Newsom, Horton E.; Williams, Josh] Univ New Mexico, Dept Earth & Planetary Sci, Inst Meteorit, Albuquerque, NM 87131 USA. [Clark, Benton, III] Space Sci Inst, Boulder, CO USA. [Wiens, Roger C.; Cousin, Agnes; Clegg, Samuel M.; Lanza, Nina; Delapp, Dorothea; Johnstone, Stephen] Los Alamos Natl Lab, Los Alamos, NM USA. [Blank, Jen G.] NASA, Ames Res Ctr, Moffett Field, CA 94035 USA. [Mangold, Nicolas] Univ Nantes, CNRS, UMR6112, LPGN, Nantes, France. [Sautter, Violaine] Museum Natl Hist Nat, Lab Mineral & Cosmochim Museum, F-75231 Paris, France. [Maurice, Sylvestre; Gasnault, Olivier; Forni, Olivier; Lasue, Jeremie; Meslin, Pierre-Yves] Univ Toulouse 3, Inst Rech Astrophys & Planetol, F-31062 Toulouse, France. [Tokar, Robert; Vaniman, Dave; Barraclough, Bruce] Planetary Sci Inst, Tucson, AZ USA. [Lewin, Eric] ISTerre, Grenoble, France. [Dyar, M. Darby] Mt Holyoke Coll, Dept Astron, S Hadley, MA 01075 USA. [Anderson, Ryan] US Geol Survey, Astrogeol Sci Ctr, Flagstaff, AZ 86001 USA. [McLennan, Scott M.] SUNY Stony Brook, Dept Geosci, Stony Brook, NY 11794 USA. [Bridges, John] Univ Leicester, Dept Phys & Astron, Space Res Ctr, Leicester LE1 7RH, Leics, England. [Fabre, Cecile] Univ Lorraine, CNRS, UMR7356, GeoResources, Vandoeuvre Les Nancy, France. [Melikechi, Noureddine] Delaware State Univ, Opt Sci Ctr Appl Res, Dover, DE USA. [Perrett, Glynis M.; Campbell, John L.; King, Penelope L.] Univ Guelph, Dept Phys, Guelph, ON N1G 2W1, Canada. [King, Penelope L.] Australian Natl Univ, Res Sch Earth Sci, Canberra, ACT, Australia. [Rosen-Gooding, Anya] Albuquerque Acad, Albuquerque, NM USA. RP Ollila, AM (reprint author), Univ New Mexico, Dept Earth & Planetary Sci, Inst Meteorit, 1 Univ New Mexico,MSC03-2050, Albuquerque, NM 87131 USA. EM aollila@unm.edu RI Gonzalez, Rafael/D-1748-2009; Rodriguez-Manfredi, Jose/L-8001-2014; King, Penelope/A-1791-2011; Ramos, Miguel/K-2230-2014; LEWIN, Eric/F-1451-2017; OI Rodriguez-Manfredi, Jose/0000-0003-0461-9815; King, Penelope/0000-0002-8364-9168; Ramos, Miguel/0000-0003-3648-6818; Gasnault, Olivier/0000-0002-6979-9012; Clegg, Sam/0000-0002-0338-0948 FU Zonta International Foundation; New Mexico Space Grant Consortium; Chateaubriand Fellowship; Canadian Space Agency FX A. Ollila would like to thank the Zonta International Foundation, the New Mexico Space Grant Consortium, and the Chateaubriand Fellowship for their support. P. King acknowledges support from the Canadian Space Agency. We would also like to thank NASA and the numerous scientists and engineers that have worked on MSL throughout the years. NR 127 TC 28 Z9 28 U1 6 U2 35 PU AMER GEOPHYSICAL UNION PI WASHINGTON PA 2000 FLORIDA AVE NW, WASHINGTON, DC 20009 USA SN 2169-9097 EI 2169-9100 J9 J GEOPHYS RES-PLANET JI J. Geophys. Res.-Planets PD JAN PY 2014 VL 119 IS 1 BP 255 EP 285 DI 10.1002/2013JE004517 PG 31 WC Geochemistry & Geophysics SC Geochemistry & Geophysics GA AD1YA UT WOS:000333028400017 ER PT S AU Quach, TT AF Quach, Tu-Thach BE Alattar, AM Memon, ND Heitzenrater, CD TI Cover Estimation and Payload Location using Markov Random Fields SO MEDIA WATERMARKING, SECURITY, AND FORENSICS 2014 SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Media Watermarking, Security, and Forensics CY FEB 03-05, 2014 CL San Francisco, CA SP Soc Imaging Sci & Technol, SPIE DE Steganalysis; Cover Estimation; Payload Location; Markov Random Fields ID GRAPH CUTS; STEGANOGRAPHY AB Payload location is an approach to find the message bits hidden in steganographic images, but not necessarily their logical order. Its success relies primarily on the accuracy of the underlying cover estimators and can be improved if more estimators are used. This paper presents an approach based on Markov random field to estimate the cover image given a stego image. It uses pairwise constraints to capture the natural two-dimensional statistics of cover images and forms a basis for more sophisticated models. Experimental results show that it is competitive against current state-of-the-art estimators and can locate payload embedded by simple LSB steganography and group-parity steganography. Furthermore, when combined with existing estimators, payload location accuracy improves significantly. C1 Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Quach, TT (reprint author), Sandia Natl Labs, POB 5800, Albuquerque, NM 87185 USA. EM tong@sandia.gov NR 20 TC 0 Z9 0 U1 0 U2 1 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9945-5 J9 PROC SPIE PY 2014 VL 9028 DI 10.1117/12.2032711 PG 9 WC Mathematical & Computational Biology; Optics SC Mathematical & Computational Biology; Optics GA BA4EE UT WOS:000335494300016 ER PT S AU Finnerty, P Aguayo, E Amman, M Avignone, FT Barabash, AS Barton, PJ Beene, JR Bertrand, FE Boswell, M Brudanin, V Busch, M Chan, YD Christofferson, CD Collar, JI Combs, DC Cooper, RJ Detwiler, JA Doe, PJ Efremenko, Y Egorov, V Ejiri, H Elliott, SR Esterline, J Fast, JE Fields, N Fraenkle, FM Galindo-Uribarri, A Gehman, M Giovanetti, GK Green, MP Guiseppe, VE Gusey, K Hallin, AL Hazama, R Henning, R Hoppe, EW Horton, M Howard, S Howe, MA Johnson, RA Keeter, KJ Kidd, MF Knecht, A Kochetov, O Konovalov, SI Kouzes, RT LaFerriere, BD Leon, J Leviner, LE Loach, JC Luke, PN MacMullin, S Marino, MG Martin, RD Merriman, JH Miller, ML Mizouni, L Nomachi, M Orrell, JL Overman, NR Perumpilly, G Phillips, DG Poon, AWP Radford, DC Rielage, K Robertson, RGH Ronquest, MC Schubert, AG Shima, T Shirchenko, M Snavely, KJ Steele, D Strain, J Timkin, V Tornow, W Varner, RL Vetter, K Vorren, K Wilkerson, JF Yakushev, E Yaver, H Young, AR Yu, CH Yumatov, V AF Finnerty, P. Aguayo, E. Amman, M. Avignone, F. T., III Barabash, A. S. Barton, P. J. Beene, J. R. Bertrand, F. E. Boswell, M. Brudanin, V. Busch, M. Chan, Y-D Christofferson, C. D. Collar, J. I. Combs, D. C. Cooper, R. J. Detwiler, J. A. Doe, P. J. Efremenko, Yu Egorov, V. Ejiri, H. Elliott, S. R. Esterline, J. Fast, J. E. Fields, N. Fraenkle, F. M. Galindo-Uribarri, A. Gehman, M. Giovanetti, G. K. Green, M. P. Guiseppe, V. E. Gusey, K. Hallin, A. L. Hazama, R. Henning, R. Hoppe, E. W. Horton, M. Howard, S. Howe, M. A. Johnson, R. A. Keeter, K. J. Kidd, M. F. Knecht, A. Kochetov, O. Konovalov, S. I. Kouzes, R. T. LaFerriere, B. D. Leon, J. Leviner, L. E. Loach, J. C. Luke, P. N. MacMullin, S. Marino, M. G. Martin, R. D. Merriman, J. H. Miller, M. L. Mizouni, L. Nomachi, M. Orrell, J. L. Overman, N. R. Perumpilly, G. Phillips, D. G., II Poon, A. W. P. Radford, D. C. Rielage, K. Robertson, R. G. H. Ronquest, M. C. Schubert, A. G. Shima, T. Shirchenko, M. Snavely, K. J. Steele, D. Strain, J. Timkin, V. Tornow, W. Varner, R. L. Vetter, K. Vorren, K. Wilkerson, J. F. Yakushev, E. Yaver, H. Young, A. R. Yu, C-H Yumatov, V. CA Majorana Collaboration GP IOP TI The MAJORANA DEMONSTRATOR: Progress towards showing the feasibility of a tonne-scale Ge-76 neutrinoless double-beta decay experiment SO PASCOS 2012 - 18TH INTERNATIONAL SYMPOSIUM ON PARTICLES STRINGS AND COSMOLOGY SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th International Symposium on Particles Strings and Cosmology (PASCOS) CY JUN 03-08, 2012 CL Merida, MEXICO SP Consejo Nacl Ciencia & Tecnologia, Univ Nacl Autonoma Mexico, Consejo Tecnico Investigac Cientifica, Univ Nacl Autonoma Mexico, Inst Ciencias Nucl, Univ Nacl Autonoma Mexico, Inst Fisica, Centro Estudios Avanzados IPN, Inst Cientifico & Tecnologico D F, Univ Guanajuato, Programa Integral Fortalecimiento Instituc, Soc Mexicana Fisica, Int Ctr Theoret Phys, Benemerita Univ Autonoma Puebla, Govt State Yucatan, Univ Hamburg, Telmex ID GERMANIUM DETECTOR; FRAMEWORK; SEARCH; MASSES AB The MAJORANA DEMONSTRATOR will search for the neutrinoless double-beta decay (0 nu beta beta) of the Ge-76 isotope with a mixed array of enriched and natural germanium detectors. The observation of this rare decay would indicate the neutrino is its own anti-particle, demonstrate that lepton number is not conserved, and provide information on the absolute mass-scale of the neutrino. The DEMONSTRATOR is being assembled at the 4850 foot level of the Sanford Underground Research Facility in Lead, South Dakota. The array will be contained in a low-background environment and surrounded by passive and active shielding. The goals for the DEMONSTRATOR are: demonstrating a background rate less than 3 t(-1) y(-1) in the 4 keV region of interest (ROT) surrounding the 2039 keV Ge-76 endpoint energy; establishing the technology required to build a tonne-scale germanium based double-beta decay experiment; testing the recent claim of observation of 0 nu beta beta [I]; and performing a direct search for light WIMPs (3-10 GeV/c(2)). C1 [Finnerty, P.; Fraenkle, F. M.; Giovanetti, G. K.; Green, M. P.; Henning, R.; Howe, M. A.; Kouzes, R. T.; MacMullin, S.; Snavely, K. J.; Strain, J.; Vorren, K.; Wilkerson, J. F.] Univ N Carolina, Dept Phys & Astron, Chapel Hill, NC 27514 USA. [Finnerty, P.; Busch, M.; Combs, D. C.; Esterline, J.; Fraenkle, F. M.; Giovanetti, G. K.; Green, M. P.; Henning, R.; Howe, M. A.; Leviner, L. E.; MacMullin, S.; Phillips, D. G., II; Snavely, K. J.; Strain, J.; Tornow, W.; Varner, R. L.; Wilkerson, J. F.; Young, A. R.] Triangle Univ, Nucl Lab, Durham, NC 27703 USA. [Aguayo, E.; Fast, J. E.; Hoppe, E. W.; Kouzes, R. T.; LaFerriere, B. D.; Merriman, J. H.; Mizouni, L.; Orrell, J. L.; Overman, N. R.] Pacific Northwest Natl Lab, Richland, WA 99353 USA. [Amman, M.; Luke, P. N.; Yaver, H.] Lawrence Berkeley Natl Lab, Div Engn, Berkeley, CA 94702 USA. [Avignone, F. T., III; Mizouni, L.] Univ South Carolina, Dept Phys & Astron, Columbia, SC 29203 USA. [Avignone, F. T., III; Beene, J. R.; Bertrand, F. E.; Cooper, R. J.; Galindo-Uribarri, A.; Radford, D. C.; Varner, R. L.; Wilkerson, J. F.; Yu, C-H] Oak Ridge Natl Lab, Oak Ridge, TN 37830 USA. [Barabash, A. S.; Konovalov, S. I.; Yumatov, V.] Inst Theoret & Expt Phys, Moscow, Russia. [Barton, P. J.; Chan, Y-D; Detwiler, J. A.; Loach, J. C.; Martin, R. D.; Poon, A. W. P.; Vetter, K.] Lawrence Berkeley Natl Lab, Div Nucl Sci, Berkeley, CA 94702 USA. [Boswell, M.; Elliott, S. R.; Gehman, M.; Kidd, M. F.; Rielage, K.; Ronquest, M. C.; Steele, D.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Egorov, V.; Gusey, K.; Kochetov, O.; Shirchenko, M.; Timkin, V.; Yakushev, E.] Joint Nucl Res Inst, Dubna, Russia. [Busch, M.; Esterline, J.; Tornow, W.] Duke Univ, Dept Phys, Durham, NC 27706 USA. [Horton, M.; Howard, S.] South Dakota Sch Mines & Technol, Rapid City, SD 57701 USA. [Fields, N.] Univ Chicago, Dept Phys, Chicago, IL 60637 USA. [Combs, D. C.; Leviner, L. E.; Phillips, D. G., II; Young, A. R.] North Carolina State Univ, Dept Phys, Raleigh, NC USA. [Doe, P. J.; Johnson, R. A.; Knecht, A.; Leon, J.; Marino, M. G.; Miller, M. L.; Robertson, R. G. H.; Schubert, A. G.] Univ Washington, Ctr Expt Nucl Phys & Astrophys, Dept Phys, Seattle, WA 98195 USA. [Efremenko, Yu] Univ Tennessee, Dept Phys & Astron, Knoxville, TN 37996 USA. [Ejiri, H.; Hazama, R.; Nomachi, M.; Shima, T.] Osaka Univ, Res Ctr Nucl Phys, Dept Phys, Suita, Osaka 565, Japan. [Guiseppe, V. E.; Perumpilly, G.] Univ S Dakota, Dept Phys, Vermillion, SD 57069 USA. [Hallin, A. L.] Univ Alberta, Ctr Particle Phys, Edmonton, AB T6G 2M7, Canada. [Keeter, K. J.] Black Hills State Univ, Dept Phys, Spearfish, SD USA. [Vetter, K.] Univ Calif Berkeley, Dept Nucl Engn, Berkeley, CA 94720 USA. RP Finnerty, P (reprint author), Univ N Carolina, Dept Phys & Astron, Chapel Hill, NC 27514 USA. EM paddy@unc.edu RI radford, David/A-3928-2015; Barabash, Alexander/S-8851-2016; OI Green, Matthew/0000-0002-1958-8030; Marino, Michael/0000-0003-1226-6036; Rielage, Keith/0000-0002-7392-7152 FU Office of Nuclear Physics in DOE Office of Science [DE-AC02-05CH11231, DE-FG02-97ER41041, DE-FG02-97ER41033, DE-FG02-97ER4104, DE-FG02-97ER41042, DE-SCOO05054, DE-FG02-10ER41715, DE-FG0297ER41020]; Nuclear Astrophysics Program of National Science Foundation [PHY-0919270, PHY-1003940, 0855314, 1003399]; Russian Federal Agency for Atomic Energy; U.S.Department of Energy through LANL/LDRD Program; DOE/NNSASSGF; Department of Energy Office of Science Graduate Fellowship Program DOESCGF; ORISE-ORAU [DE-AC05-06OR23100] FX We acknowledge support from the Office of Nuclear Physics in the DOE Office of Science under grant numbers DE-AC02-05CH11231, DE-FG02-97ER41041, DE-FG02-97ER41033, DE-FG02-97ER4104, DE-FG02-97ER41042,DE-SCOO05054, DE-FG02-10ER41715, andDE-FG0297ER41020. We acknowledge support from the Particle and Nuclear Astrophysics Program of the National Science Foundation through grant numbers PHY-0919270, PHY-1003940, 0855314, and 1003399. We gratefully acknowledge support from the Russian Federal Agency for Atomic Energy. We gratefully acknowledge the support of the U.S.Department of Energy through the LANL/LDRD Program. N. Fields is supported by the DOE/NNSASSGF program.G.K. Giovanetti is supported by the Department of Energy Office of Science Graduate Fellowship Program (DOESCGF), made possible in part by the American Recovery and Reinvestment Act of 2009, administered by ORISE-ORAU under contract no.DE-AC05-06OR23100. NR 25 TC 0 Z9 0 U1 1 U2 3 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 485 AR UNSP 012042 DI 10.1088/1742-6596/485/1/012042 PG 6 WC Astronomy & Astrophysics; Physics, Multidisciplinary; Physics, Particles & Fields SC Astronomy & Astrophysics; Physics GA BA4EW UT WOS:000335557100042 ER PT S AU Kopp, J AF Kopp, Joachim GP IOP TI New signals in dark matter detectors SO PASCOS 2012 - 18TH INTERNATIONAL SYMPOSIUM ON PARTICLES STRINGS AND COSMOLOGY SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 18th International Symposium on Particles Strings and Cosmology (PASCOS) CY JUN 03-08, 2012 CL Merida, MEXICO SP Consejo Nacl Ciencia & Tecnologia, Univ Nacl Autonoma Mexico, Consejo Tecnico Investigac Cientifica, Univ Nacl Autonoma Mexico, Inst Ciencias Nucl, Univ Nacl Autonoma Mexico, Inst Fisica, Centro Estudios Avanzados IPN, Inst Cientifico & Tecnologico D F, Univ Guanajuato, Programa Integral Fortalecimiento Instituc, Soc Mexicana Fisica, Int Ctr Theoret Phys, Benemerita Univ Autonoma Puebla, Govt State Yucatan, Univ Hamburg, Telmex ID OSCILLATIONS; SOLAR AB We investigate the scattering of solar neutrinos on electrons and nuclei in dark matter direct detection experiments. The rates of these processes are small in the Standard Model, but can be enhanced by several orders of magnitude if the neutrino sector is slightly non-minimal. This makes even the current generation of dark matter detectors very sensitive to non-standard neutrino physics. Examples discussed here are neutrino magnetic moments and toy models with a simple hidden sector containing a sterile neutrino and a light new gauge boson ("dark photon"). We discuss the expected event spectra and temporal modulation effects, as well as constraints from a variety of astrophysical, cosmological, and laboratory experiments. C1 Fermilab Natl Accelerator Lab, Batavia, IL 60510 USA. RP Kopp, J (reprint author), Fermilab Natl Accelerator Lab, POB 500, Batavia, IL 60510 USA. EM jkopp@mpi-hd.mpg.de NR 29 TC 0 Z9 0 U1 0 U2 0 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 485 AR 012032 DI 10.1088/1742-6596/485/1/012032 PG 6 WC Astronomy & Astrophysics; Physics, Multidisciplinary; Physics, Particles & Fields SC Astronomy & Astrophysics; Physics GA BA4EW UT WOS:000335557100032 ER PT J AU Wan, W Lee, H Yu, XQ Wang, C Nam, KW Yang, XQ Zhou, HH AF Wan, Wang Lee, Hungsui Yu, Xiqian Wang, Chao Nam, Kyung-Wan Yang, Xiao-Qing Zhou, Henghui TI Tuning the electrochemical performances of anthraquinone organic cathode materials for Li-ion batteries through the sulfonic sodium functional group SO RSC ADVANCES LA English DT Article ID RECHARGEABLE LITHIUM BATTERIES; STORAGE MATERIALS; ELECTRODES; COMPOUND; CAPACITY; SALT AB The effects on electrochemical performance of C14H8O2 organic cathode materials with and without SO3Na- functional groups for lithium ion batteries were investigated. The Na2C14H6O8S2 with two SO3Na- shows the best cycle performance and highest lithium storage voltage, while an outstanding rate performance is also achieved after combination with graphene paper. C1 [Wan, Wang; Wang, Chao; Zhou, Henghui] Peking Univ, Coll Chem & Mol Engn, Beijing 100871, Peoples R China. [Lee, Hungsui; Yu, Xiqian; Yang, Xiao-Qing] Brookhaven Natl Lab, Upton, NY 11973 USA. [Nam, Kyung-Wan] Dongguk Univ Seoul, Dept Energy & Mat Engn, Seoul 100715, South Korea. RP Yu, XQ (reprint author), Brookhaven Natl Lab, Upton, NY 11973 USA. EM xyu@bnl.gov; xyang@bnl.gov; hhzhou@pku.edu.cn RI Nam, Kyung-Wan/B-9029-2013; Nam, Kyung-Wan/E-9063-2015; Yu, Xiqian/B-5574-2014; OI Nam, Kyung-Wan/0000-0001-6278-6369; Nam, Kyung-Wan/0000-0001-6278-6369; Yu, Xiqian/0000-0001-8513-518X; zhou, henghui/0000-0003-0317-1756 FU A*Star Singapore-China Joint Research Program [2012DFG52130]; U.S. Department of Energy; Office of Vehicle Technologies [DEAC02-98CH10886] FX We appreciate financial support from the A*Star Singapore-China Joint Research Program (no. 2012DFG52130). This 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 under Contract Number DEAC02-98CH10886. The support provided by the China Scholarship Council (CSC) during a visit of Wang Wan to Brookhaven National Lab is acknowledged. The authors acknowledge technical support by the beamline scientist Dr Jianming Bai at X14A (NSLS, BNL). NR 28 TC 19 Z9 19 U1 7 U2 75 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 2014 VL 4 IS 38 BP 19878 EP 19882 DI 10.1039/c4ra01166j PG 5 WC Chemistry, Multidisciplinary SC Chemistry GA AH2AK UT WOS:000335922900043 ER PT S AU Perera, D Landau, DP Nicholson, DM Stocks, GM Eisenbach, M Yin, JQ Brown, G AF Perera, Dilina Landau, David P. Nicholson, Don M. Stocks, G. Malcolm Eisenbach, Markus Yin, Junqi Brown, Gregory GP IOP TI Combined molecular dynamics-spin dynamics simulations of bcc iron SO VII BRAZILIAN MEETING ON SIMULATIONAL PHYSICS SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 7th Brazilian Meeting on Simulational Physics CY AUG 05-10, 2013 CL Joao Pessoa, BRAZIL SP Brazilian Agcy CNPq, Brazilian Agcy CAPES, Brazilian Agcy FAPESQ, Federal Univ UFPB, Federal Univ UFMG ID AB-INITIO; SYSTEMS AB Using a classical model that treats translational and spin degrees of freedom on an equal footing, we study phonon-magnon interactions in BCC iron with combined molecular and spin dynamics methods. The atomic interactions are modeled via an empirical many-body potential while spin dependent interactions are established through a Hamiltonian of the Heisenberg form with a distance dependent magnetic exchange interaction obtained from first principles electronic structure calculations. The temporal evolution of translational and spin degrees of freedom was determined by numerically solving the coupled equations of motion, using an algorithm based on the second order Suzuki-Trotter decomposition of the exponential operators. By calculating Fourier transforms of space- and time-displaced correlation functions, we demonstrate that the the presence of lattice vibrations leads to noticeable softening and damping of spin wave modes. As a result of the interplay between lattice and spin subsystems, we also observe additional longitudinal spin wave excitations, with frequencies which coincide with that of the longitudinal lattice vibrations. C1 [Perera, Dilina; Landau, David P.] Univ Georgia, Ctr Simulat Phys, Athens, GA 30602 USA. [Nicholson, Don M.; Stocks, G. Malcolm; Eisenbach, Markus; Yin, Junqi] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. [Brown, Gregory] Florida State Univ, Tallahassee, FL 32306 USA. RP Perera, D (reprint author), Univ Georgia, Ctr Simulat Phys, Athens, GA 30602 USA. EM dilinanp@physast.uga.edu RI Stocks, George Malcollm/Q-1251-2016; OI Stocks, George Malcollm/0000-0002-9013-260X; Eisenbach, Markus/0000-0001-8805-8327; Yin, Junqi/0000-0003-3843-5520 FU U.S.Department of Energy, Office of Basic Energy Sciences, Materials Sciences and Engineering Division, Center for Defect Physics; Energy Frontier Research Center; Georgia Advanced Computing Resource Center FX Authors wish to thank Shan-Ho Tsai and Stefan Schnabel for informative discussions. This research was sponsored by the U.S.Department of Energy, Office of Basic Energy Sciences, Materials Sciences and Engineering Division, "Center for Defect Physics ", an Energy Frontier Research Center. We also acknowledge the computational resources and technical expertise provided by the Georgia Advanced Computing Resource Center, a partnership between the University of Georgia's Office of the Vice President for Research and Office of the Vice President for Information Technology NR 22 TC 4 Z9 4 U1 1 U2 5 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 487 AR UNSP 012007 DI 10.1088/1742-6596/487/1/012007 PG 9 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA4DV UT WOS:000335442800007 ER PT S AU Vogel, T Li, YW Wust, T Landau, DP AF Vogel, Thomas Li, Ying Wai Wuest, Thomas Landau, David P. GP IOP TI Exploring new frontiers in statistical physics with a new, parallel Wang-Landau framework SO VII BRAZILIAN MEETING ON SIMULATIONAL PHYSICS SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 7th Brazilian Meeting on Simulational Physics CY AUG 05-10, 2013 CL Joao Pessoa, BRAZIL SP Brazilian Agcy CNPq, Brazilian Agcy CAPES, Brazilian Agcy FAPESQ, Federal Univ UFPB, Federal Univ UFMG ID DENSITY-OF-STATES; RANDOM-WALK; ALGORITHM; SIMULATIONS; PERCOLATION AB Combining traditional Wang-Landau sampling for multiple replica systems with an exchange of densities of states between replicas, we describe a general framework for simulations on massively parallel Petaflop supercomputers. The advantages and general applicability of the method for simulations of complex systems are demonstrated for the classical 2D Potts spin model featuring a strong first-order transition and the self-assembly of lipid bilayers in amphiphilic solutions in a continuous model. C1 [Vogel, Thomas] Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. [Vogel, Thomas; Li, Ying Wai; Landau, David P.] Univ Georgia, Ctr Simulat Phys, Athens, GA 30602 USA. [Wuest, Thomas] Oak Ridge Natl Lab, Natl Ctr Computat, Oak Ridge, TN 37831 USA. [Wuest, Thomas] Swiss Fed Res Inst WSL, CH-8903 Birmensdorf, Switzerland. RP Vogel, T (reprint author), Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. EM thomasvogel@physast.uga.edu RI Vogel, Thomas/A-7570-2014 OI Vogel, Thomas/0000-0003-0205-3205 FU National Science Foundation [DMR-0810223, OCI-0904685]; Office of Advanced Scientific Computing Research; U.S. Department of Energy; TACC under XSEDE [PHY130009, PHY 130014]; [LA-UR-13-26563] FX This work was supported by the National Science Foundation under Grants DMR-0810223 and OCI-0904685. Y.W. Li was partly sponsored by the Office of Advanced Scientific Computing Research; U.S. Department of Energy. Supercomputer time was provided by TACC under XSEDE grants PHY130009 and PHY 130014. Assigned : LA-UR-13-26563. NR 35 TC 5 Z9 5 U1 0 U2 8 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 487 AR UNSP 012001 DI 10.1088/1742-6596/487/1/012001 PG 10 WC Physics, Applied; Physics, Multidisciplinary SC Physics GA BA4DV UT WOS:000335442800001 ER PT J AU Ha, JW Fang, N AF Ha, Ji Won Fang, Ning TI Defocused differential interference contrast microscopy imaging of single plasmonic anisotropic nanoparticles SO CHEMICAL COMMUNICATIONS LA English DT Article ID GOLD NANORODS; ORIENTATION SENSORS; 3-DIMENSIONAL ORIENTATION; METAL NANOPARTICLES; ROTATIONAL-DYNAMICS; ABSORPTION; MOLECULE; SIZE AB We present the defocused differential interference contrast (DIC) imaging of gold nanorods. We found that the scattered light and the defocus aberration play an important role in the formation of orientation-dependent DIC image patterns of a gold nanorod. Interestingly, the scattered light from a gold nanorod aligned closer to the polarization directions enables us to directly resolve its spatial orientation under a defocused DIC microscope. C1 [Fang, Ning] Iowa State Univ, US Dept Energy, Ames Lab, Ames, IA 50011 USA. Iowa State Univ, Dept Chem, Ames, IA 50011 USA. RP Fang, N (reprint author), Iowa State Univ, US Dept Energy, Ames Lab, Ames, IA 50011 USA. EM nfang@iastate.edu FU U.S. Department of Energy, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division; U.S. Department of Energy [DE-AC02-07CH11358] FX This work was supported by U.S. Department of Energy, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division. The Ames Laboratory is operated for the U.S. Department of Energy by Iowa State University under contract no. DE-AC02-07CH11358. NR 22 TC 2 Z9 2 U1 4 U2 23 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 2014 VL 50 IS 41 BP 5500 EP 5502 DI 10.1039/c4cc01567c PG 3 WC Chemistry, Multidisciplinary SC Chemistry GA AG3QE UT WOS:000335333700022 PM 24722924 ER PT J AU Wang, L Han, J Hoy, J Hu, F Liu, HQ Gentleman, MM Sfeir, MY Misewich, JA Wong, SS AF Wang, Lei Han, Jinkyu Hoy, Jessica Hu, Fang Liu, Haiqing Gentleman, Molly M. Sfeir, Matthew Y. Misewich, James A. Wong, Stanislaus S. TI Probing differential optical and coverage behavior in nanotube-nanocrystal heterostructures synthesized by covalent versus non-covalent approaches SO DALTON TRANSACTIONS LA English DT Article ID WALL CARBON NANOTUBES; CDSE QUANTUM DOTS; ELECTRON-TRANSFER; PHOTOLUMINESCENCE; GRAPHENE; GROWTH; FUNCTIONALIZATION; ASSEMBLIES AB Double-walled carbon nanotube (DWNT)-CdSe heterostructures with the individual nanoscale building blocks linked together by 4-aminothiophenol (4-ATP) have been successfully synthesized using two different and complementary routes, i.e. covalent attachment and non-covalent p-p stacking. Specifically, using a number of characterization methods, we have probed the effects of these differential synthetic coupling approaches on the resulting CdSe quantum dot (QD) coverage on the underlying nanotube template as well as the degree of charge transfer between the CdSe QDs and the DWNTs. In general, based on microscopy and spectroscopy data collectively, we noted that heterostructures generated by noncovalent p-p stacking interactions evinced not only higher QD coverage density but also possibly more efficient charge transfer behavior as compared with their counterparts produced using covalent linker-mediated protocols. C1 [Wang, Lei; Liu, Haiqing; Wong, Stanislaus S.] SUNY Stony Brook, Dept Chem, Stony Brook, NY 11794 USA. [Han, Jinkyu; Hoy, Jessica; Misewich, James A.; Wong, Stanislaus S.] Brookhaven Natl Lab, Condensed Matter Phys & Mat Sci Dept, Upton, NY 11973 USA. [Hu, Fang; Gentleman, Molly M.] SUNY Stony Brook, Mat Sci Dept, Stony Brook, NY 11794 USA. [Hoy, Jessica; Sfeir, Matthew Y.] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. RP Wong, SS (reprint author), SUNY Stony Brook, Dept Chem, Stony Brook, NY 11794 USA. EM sswong@bnl.gov RI Han, Jinkyu/B-6522-2013; OI Sfeir, Matthew/0000-0001-5619-5722 FU U.S. Department of Energy [DE-AC02-98CH10886]; U.S. Department of Energy Office of Basic Energy Sciences [DE-AC02-98CH10886] FX Research (including support for LW, JKH, JH, HL, and SSW) was provided by the U.S. Department of Energy, Basic Energy Sciences, Materials Sciences and Engineering Division at Brookhaven National Laboratory, which is supported by the U.S. Department of Energy under Contract No. DE-AC02-98CH10886. Research (i.e. PL measurements) 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. NR 44 TC 2 Z9 2 U1 2 U2 24 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 2014 VL 43 IS 20 BP 7480 EP 7490 DI 10.1039/c3dt53405g PG 11 WC Chemistry, Inorganic & Nuclear SC Chemistry GA AG4HS UT WOS:000335380900019 PM 24658386 ER PT J AU Mandalika, A Qin, L Sato, TK Runge, T AF Mandalika, Anurag Qin, Li Sato, Trey K. Runge, Troy TI Integrated biorefinery model based on production of furans using open-ended high yield processes SO GREEN CHEMISTRY LA English DT Article ID LIQUID HOT-WATER; VAPOR-PHASE HYDROGENATION; YEAST PICHIA-STIPITIS; SACCHAROMYCES-CEREVISIAE; FURFURYL ALCOHOL; ETHANOL FERMENTATION; SELECTIVE HYDROGENATION; SUPPORTED COPPER; BATCH CULTURE; CORN STOVER AB The biodetoxification pathway for the reduction of the fermentation inhibitor furfural was utilized to produce furfuryl alcohol using both a commercial Bakers' yeast and six other native strains selected for their high tolerance towards the inhibitory effects of furfural. This study explores the potential of the microbial method as an environmentally-benign alternative to the conventional catalytic hydrogenation process for producing furfuryl alcohol used extensively in industry. The microbial method for furfuryl alcohol production provides the benefit of a homogeneous biochemical conversion devoid of chemical catalysis in conjunction with other carbohydrate-based processes (e.g. production of ethanol). Results showed that the yields of furfuryl alcohol using the laboratory yeast strains exceeded 90% of the theoretical yield at a furfural concentration of 25 g l(-1) which are comparable to yields obtained using the catalyticprocess. Furfuryl alcohol yields progressively declined as the furfural concentration was increased up to 65 g l(-1) where the yields averaged over 37%. Piecing together novel high-yield conversion processes for furfural and furfuryl alcohol an integrated biorefinery model based on the production of furans has been envisioned. Such a facility bypasses the need for high pressure hydrogenation using copper chromite catalysts and hydrogen and azeotropic distillation of furfural to produce dilute streams of both notable platform chemicals. C1 [Mandalika, Anurag] Louisiana State Univ, Ctr Agr, Baton Rouge, LA 70803 USA. [Qin, Li; Sato, Trey K.] Univ Wisconsin, DOE Great Lakes Bioenergy Res Ctr, Madison, WI 53726 USA. [Runge, Troy] Univ Wisconsin, Madison, WI 53706 USA. RP Mandalika, A (reprint author), Louisiana State Univ, Ctr Agr, Baton Rouge, LA 70803 USA. EM trunge@wisc.edu FU National Institute of Food and Agriculture, United States Department of Agriculture [WIS01521]; DOE Great Lakes Bioenergy Research Center (DOE BER Office of Science) [DE-FC02-07ER64494] FX This material is based upon work support by the National Institute of Food and Agriculture, United States Department of Agriculture, under ID number WIS01521, and the DOE Great Lakes Bioenergy Research Center (DOE BER Office of Science DE-FC02-07ER64494). The authors would like to acknowledge Zhouyang Xiang and Yi-Kai Su for development of the analytical and fermentation methods utilized in this work. The authors are also grateful to the Wisconsin Energy Institute at the University of Wisconsin, for support of this work, and assistance provided by Drs JunYong Zhu and Carl Houtman of the USDA Forest Products Lab in Madison, WI. NR 62 TC 8 Z9 10 U1 4 U2 21 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 2014 VL 16 IS 5 BP 2480 EP 2489 DI 10.1039/c3gc42424c PG 10 WC Chemistry, Multidisciplinary; GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY SC Chemistry; Science & Technology - Other Topics GA AF8ZT UT WOS:000335005200017 ER PT J AU Sun, N Parthasarathi, R Socha, AM Shi, J Zhang, S Stavila, V Sale, KL Simmons, BA Singh, S AF Sun, Ning Parthasarathi, Ramakrishnan Socha, Aaron M. Shi, Jian Zhang, Sonny Stavila, Vitalie Sale, Kenneth L. Simmons, Blake A. Singh, Seema TI Understanding pretreatment efficacy of four cholinium and imidazolium ionic liquids by chemistry and computation SO GREEN CHEMISTRY LA English DT Article ID 1-ETHYL-3-METHYLIMIDAZOLIUM ACETATE; LIGNOCELLULOSIC BIOMASS; CELLULOSE; DISSOLUTION; SOLVENT; LIGNIN; REGENERATION; SACCHARIFICATION; SWITCHGRASS; EXTRACTION AB Certain ionic liquids (ILs) offer a potentially more sustainable and environmentally responsible alternative to organic solvents for many industrial applications, including biorefineries, where they are used to pretreat lignocellulose. To gain a more robust understanding of the roles of cations and anions in the process, we monitored the impact of the respective ILs on Panicum virgatum (switchgrass) in terms of lignin content, cellulose crystallinity, and enzymatic digestibility. The behaviors of four ILs, based on one of two cations, 1-ethyl-3-methylimidazolium ([C(2)mim](+)) and cholinium ([Ch](+)), and one of two anions, acetate ([OAc](-)) and lysinate ([Lys](-)), were compared. While all four ILs were effective in pretreating switchgrass, ILs containing [Lys](-)anions provided greater delignification (70-80% vs. 16-50%) after addition of water as an anti-solvent and higher glucose yields (78-96% vs. 56-90%) compared to those obtained by the use of ILs containing [OAc]-anions. Measurements of the Kamlet-Taft parameters using a series of dyes indicated a greater hydrogen bond basicity for the ILs with [Lys](-)anions as compared to acetate ILs. To understand the effective delignification ability of lysinate-based ILs, interaction energies of individual ions and ion pairs with a model dilignol substrate were determined by quantum chemical calculations. The results show that the addition of antisolvent significantly influenced the interaction energies governing lignin removal during the process. C1 [Sun, Ning; Parthasarathi, Ramakrishnan; Socha, Aaron M.; Shi, Jian; Zhang, Sonny; Sale, Kenneth L.; Simmons, Blake A.; Singh, Seema] Joint BioEnergy Inst, Deconstruct Div, Emeryville, CA 94608 USA. [Sun, Ning] Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA USA. [Parthasarathi, Ramakrishnan; Socha, Aaron M.; Shi, Jian; Stavila, Vitalie; Sale, Kenneth L.; Simmons, Blake A.; Singh, Seema] Biol & Mat Sci Ctr, Sandia Natl Labs, Livermore, CA USA. [Socha, Aaron M.] CUNY Bronx Community Coll, Dept Chem & Chem Technol, Bronx, NY USA. RP Sun, N (reprint author), Joint BioEnergy Inst, Deconstruct Div, Emeryville, CA 94608 USA. EM seesing@sandia.gov RI Parthasarathi, Ramakrishnan/C-2093-2008; OI Parthasarathi, Ramakrishnan/0000-0001-5417-5867; Simmons, Blake/0000-0002-1332-1810 FU Office of Science, Office of Biological and Environmental Research; National Energy Research Scientific Computing Center (NERSC); [DE-AC02-05CH11231] FX This work conducted by 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. This research used resources of the National Energy Research Scientific Computing Center (NERSC) and the authors thank Francesca Verdier, Department Head, NERSC Services for the timely help. The authors also thank Dr Dong Wu for providing the cell wall image in the graphical table of contents entry. NR 41 TC 30 Z9 30 U1 6 U2 63 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 2014 VL 16 IS 5 BP 2546 EP 2557 DI 10.1039/c3gc42401d PG 12 WC Chemistry, Multidisciplinary; GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY SC Chemistry; Science & Technology - Other Topics GA AF8ZT UT WOS:000335005200025 ER PT J AU Ciesielski, PN Resch, MG Hewetson, B Killgore, JP Curtin, A Anderson, N Chiaramonti, AN Hurley, DC Sanders, A Himmel, ME Chapple, C Mosier, N Donohoe, BS AF Ciesielski, Peter N. Resch, Michael G. Hewetson, Barron Killgore, Jason P. Curtin, Alexandra Anderson, Nick Chiaramonti, Ann N. Hurley, Donna C. Sanders, Aric Himmel, Michael E. Chapple, Clint Mosier, Nathan Donohoe, Bryon S. TI Engineering plant cell walls: tuning lignin monomer composition for deconstructable biofuel feedstocks or resilient biomaterials SO GREEN CHEMISTRY LA English DT Article ID ARABIDOPSIS-THALIANA; FERULATE 5-HYDROXYLASE; BIOMASS RECALCITRANCE; HYBRID POPLAR; LIGNIFICATION; HEMICELLULOSE; DIGESTIBILITY; PRETREATMENT; SWITCHGRASS; HYDROLYSIS AB Advances in genetic manipulation of the biopolymers that compose plant cell walls will facilitate more efficient production of biofuels and chemicals from biomass and lead to specialized biomaterials with tailored properties. Here we investigate several genetic variants of Arabidopsis: the wild type, which makes a lignin polymer of primarily guaiacyl (G) and syringyl (S) monomeric units, the fah1 mutant, which makes lignin from almost exclusively G subunits, and a ferulate 5-hydroxylase (F5H) overexpressing line (C4H: F5H) that makes lignin from S subunits. We employ multiscale, multimodal imaging techniques that reveal the biomass of the C4H: F5H transgenic to be more susceptible to deconstruction by maleic acid treatment than the other variants. Enzymatic saccharification assays of the treated materials show that C4H: F5H transgenic tissue is significantly more digestible than the wild type, while the fah1 mutant is clearly the least digestible of these materials. Finally, we show by contact resonance force microscopy, an atomic force microscopy technique, that F5H overexpression in C4H: F5H transgenic plants significantly reduces the stiffness of the cell walls in the region of the compound middle lamella relative to wild type and fah1. C1 [Ciesielski, Peter N.; Resch, Michael G.; Himmel, Michael E.; Donohoe, Bryon S.] Natl Renewable Energy Lab, Biosci Ctr, Golden, CO 80401 USA. [Hewetson, Barron; Mosier, Nathan] Purdue Univ, Dept Agr & Biol Engn, W Lafayette, IN 47907 USA. [Killgore, Jason P.; Curtin, Alexandra; Chiaramonti, Ann N.; Hurley, Donna C.] NIST, Appl Chem & Mat Div, Boulder, CO 80305 USA. [Curtin, Alexandra; Sanders, Aric] NIST, Quantum Elect & Photon Div, Boulder, CO 80305 USA. [Anderson, Nick; Chapple, Clint] Purdue Univ, Dept Biochem, W Lafayette, IN 47907 USA. RP Ciesielski, PN (reprint author), Natl Renewable Energy Lab, Biosci Ctr, 15013 Denver West Pkwy, Golden, CO 80401 USA. EM bryon.donohoe@nrel.gov FU Center for Direct Catalytic Conversion of Biomass to Biofuels (C3Bio) FX This work was supported as part of 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, Award Number DE-SC0000997. NREL is a national laboratory of the US Department of Energy, Office of Energy Efficiency and Renewable Energy, operated by the Alliance for Sustainable Energy, LLC. The authors would like to acknowledge the role of the Renewable & Sustainable Energy Institute (RASEI) in facilitating the collaboration between NREL and NIST-Boulder. Partial contribution of NIST, not subject to copyright. NR 34 TC 19 Z9 20 U1 3 U2 57 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 2014 VL 16 IS 5 BP 2627 EP 2635 DI 10.1039/c3gc42422g PG 9 WC Chemistry, Multidisciplinary; GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY SC Chemistry; Science & Technology - Other Topics GA AF8ZT UT WOS:000335005200035 ER PT J AU Ertsen, MW Murphy, JT Purdue, LE Zhu, T AF Ertsen, M. W. Murphy, J. T. Purdue, L. E. Zhu, T. TI A journey of a thousand miles begins with one small step - human agency, hydrological processes and time in socio-hydrology SO HYDROLOGY AND EARTH SYSTEM SCIENCES LA English DT Article ID USA; PRECIPITATION; HOHOKAM AB When simulating social action in modeling efforts, as in socio-hydrology, an issue of obvious importance is how to ensure that social action by human agents is well-represented in the analysis and the model. Generally, human decision-making is either modeled on a yearly basis or lumped together as collective social structures. Both responses are problematic, as human decision-making is more complex and organizations are the result of human agency and cannot be used as explanatory forces. A way out of the dilemma of how to include human agency is to go to the largest societal and environmental clustering possible: society itself and climate, with time steps of years or decades. In the paper, another way out is developed: to face human agency squarely, and direct the modeling approach to the agency of individuals and couple this with the lowest appropriate hydrological level and time step. This approach is supported theoretically by the work of Bruno Latour, the French sociologist and philosopher. We discuss irrigation archaeology, as it is in this discipline that the issues of scale and explanatory force are well discussed. The issue is not just what scale to use: it is what scale matters. We argue that understanding the arrangements that permitted the management of irrigation over centuries requires modeling and understanding the small-scale, day-to-day operations and personal interactions upon which they were built. This effort, however, must be informed by the longer-term dynamics, as these provide the context within which human agency is acted out. C1 [Ertsen, M. W.; Zhu, T.] Delft Univ Technol, Water Resources Dept, Delft, Netherlands. [Murphy, J. T.] Argonne Natl Lab, Argonne, IL 60439 USA. [Murphy, J. T.] Univ Chicago, Computat Inst, Chicago, IL 60637 USA. [Purdue, L. E.] Arizona State Univ, Sch Sustainabil, Tempe, AZ USA. RP Ertsen, MW (reprint author), Delft Univ Technol, Water Resources Dept, Delft, Netherlands. EM m.w.ertsen@tudelft.nl FU Soil System Inc. (Paleowest); GEOPHEN laboratory (University of Caen Basse-Normandie, France); Fyssen Foundation; Desert Archaeology, Inc, Pima County, Arizona FX Authors would like to thank the School of Human Evolution and Social Change and well as the School of Sustainability at Arizona State University (Tempe, Arizona) for their support in the collection of the data. Louise Purdue would also like to thank Soil System Inc. (Paleowest) and the GEOPHEN laboratory (University of Caen Basse-Normandie, France) for the support they provided in collecting and preparing the data as well as the Fyssen Foundation for its financial support in the development of this project. Fieldwork at the Las Capas site in 2008 and 2009 was undertaken by Desert Archaeology, Inc, and was funded by Pima County, Arizona, bonds as part of the Ina Road Regional Wastewater Reclamation Facility Upgrade Project. All photos and source data are courtesy of Desert Archaeology, Inc., Tucson, Arizona, and we gratefully acknowledge the opportunity to work with the data their excavations have collected and the effort they made in providing the data in a useful format. Special thanks are due to Desert Archaeology's James Vint and Fred Nials; without their contributions of materials, data, and insight this project would not have been possible. All errors are our own. NR 41 TC 10 Z9 10 U1 1 U2 15 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1027-5606 EI 1607-7938 J9 HYDROL EARTH SYST SC JI Hydrol. Earth Syst. Sci. PY 2014 VL 18 IS 4 BP 1369 EP 1382 DI 10.5194/hess-18-1369-2014 PG 14 WC Geosciences, Multidisciplinary; Water Resources SC Geology; Water Resources GA AG4FS UT WOS:000335375300010 ER PT J AU Konca, YU Kirshenbaum, K Zuckermann, RN AF Konca, Yeliz Utku Kirshenbaum, Kent Zuckermann, Ronald N. TI Nanometer-scale siRNA carriers incorporating peptidomimetic oligomers: physical characterization and biological activity SO INTERNATIONAL JOURNAL OF NANOMEDICINE LA English DT Article DE lipitoid; siRNA delivery; therapeutic oligonucleotides; peptoid ID CAVEOLAE-MEDIATED ENDOCYTOSIS; CELL-PENETRATING PEPTIDE; LIPID-LIKE MATERIALS; GENE DELIVERY; IN-VIVO; RNAI THERAPEUTICS; CURRENT PROGRESS; MAMMALIAN-CELLS; CATIONIC LIPIDS; DRUG-DELIVERY AB Synthetic short interfering RNA (siRNA) oligonucleotides can trigger the RNA interference pathway and lead to selective gene silencing. Despite considerable enthusiasm and investment, formidable challenges remain that may deter translating this breakthrough discovery into clinical applications. In particular, the development of efficient, nontoxic, nonimmunogenic methods for delivering siRNA in vivo has proven to be exceptionally challenging. Thorough analysis of the relationship between the structure and function of siRNA carrier systems, both in isolation and in complex with RNA, will facilitate the design of efficient nonviral siRNA delivery vehicles. In this study, we explore the relationship between the physicochemical characteristics and the biological activity of "lipitoid" compounds as potent siRNA delivery vehicles. Lipitoids are cationic peptidomimetic oligomers incorporating a peptoid and a phospholipid moiety. Lipitoids can associate with siRNA oligonucleotides and self-assemble into spherical lipitoid-based nanoparticles (LNPs), with dimensions that are dependent upon the medium and the stoichiometric ratio between the cationic monomers of the lipitoid and anionic siRNA oligonucleotides. The morphology, gene silencing efficiency, and cytotoxicity of the siRNA-loaded LNPs are similarly sensitive to the stoichiometry of the complexes. The medium in which the LNPs are formed affects the assembled cargo particles' characteristics such as particle size, transfection efficiency, and stability. Formation of the LNPs in the biological, serum-free medium OptiMEM resulted in LNPs an order of magnitude larger than LNPs formed in water, and were twice as efficient in siRNA transfection compared to LNPs formed in water. Inhibitor studies were conducted to elucidate the efficiency of lysosomal escape and the uptake mechanism of the siRNA-loaded LNPs. Our results suggest that these lipitoid-based, siRNA-loaded spherical LNPs are internalized through a lipid raft-dependent and dynaminmediated pathway, circumventing endosomal and lysosomal encapsulation. The lipitoid-siRNA nanospheres proved to be suitable platforms for investigating the critical parameters determining the efficiency of transfection agents, revealing the necessity for conducting characterization studies in biological media. The investigation of the LNP internalization pathway points to an alternative uptake route that bypasses the lysosome, explaining the surprisingly high efficiency of LNPs and suggesting that the uptake mechanism should be probed rather than assumed for the next generation of rationally designed -transfection agents. C1 [Konca, Yeliz Utku] Koc Univ, Dept Chem, TR-34450 Istanbul, Turkey. [Kirshenbaum, Kent] NYU, Dept Chem, New York, NY 10003 USA. [Zuckermann, Ronald N.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA. RP Konca, YU (reprint author), Koc Univ, Dept Chem, TR-34450 Istanbul, Turkey. EM ykonca@ku.edu.tr RI Foundry, Molecular/G-9968-2014 FU Office of Science, Office of Basic Energy Sciences of the Department of Energy [DE-AC02-05CH11231]; National Science Foundation (NSF) [CHE-#1152317]; MacCracken Full Fellowship awarded by New York University; Horizon Travel Award for Research; Margaret and Herman Sokol Travel/Research Award FX Portions of this work were performed as a User Project at the Molecular Foundry, Lawrence Berkeley National Laboratory, which is supported by the Office of Science, Office of Basic Energy Sciences of the Department of Energy under Contract No DE-AC02-05CH11231. The support of the National Science Foundation (NSF), through award CHE-#1152317 to KK, is gratefully acknowledged. This work would not be possible without the Horizon Travel Award for Research, the Margaret and Herman Sokol Travel/Research Award, and MacCracken Full Fellowship awarded by New York University to YUK. NR 47 TC 4 Z9 4 U1 3 U2 21 PU DOVE MEDICAL PRESS LTD PI ALBANY PA PO BOX 300-008, ALBANY, AUCKLAND 0752, NEW ZEALAND SN 1178-2013 J9 INT J NANOMED JI Int. J. Nanomed. PY 2014 VL 9 BP 2271 EP 2284 DI 10.2147/IJN.S57449 PG 14 WC Nanoscience & Nanotechnology; Pharmacology & Pharmacy SC Science & Technology - Other Topics; Pharmacology & Pharmacy GA AG7BU UT WOS:000335573800001 PM 24872690 ER PT J AU Zhong, X Liu, L Wang, XD Yu, HY Zhuang, GL Mei, DH Li, XN Wang, JG AF Zhong, Xing Liu, Lin Wang, Xinde Yu, Huiyou Zhuang, Guilin Mei, Donghai Li, Xiaonian Wang, Jian-guo TI A radar-like iron based nanohybrid as an efficient and stable electrocatalyst for oxygen reduction SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID NONPRECIOUS-METAL-CATALYSTS; DENSITY-FUNCTIONAL THEORY; FUEL-CELLS; CATHODE CATALYST; GRAPHENE; PHTHALOCYANINE; PERFORMANCE; COMPOSITE; POLYANILINE AB A new type of hybrid material consisting of iron phthalocyanine (FePc) coordinated with pyridyne cycloaddition of graphene sheets (PyNGs) as a high-performance electrocatalyst for ORR was fabricated. The Fe-PyNG hybrid has a similar overpotential but has a higher current density and superior stability compared to Pt/C in alkaline solutions for ORR. C1 [Zhong, Xing; Liu, Lin; Wang, Xinde; Yu, Huiyou; Zhuang, Guilin; Li, Xiaonian; Wang, Jian-guo] Zhejiang Univ Technol, Coll Chem Engn, Hangzhou 310014, Zhejiang, Peoples R China. [Mei, Donghai] Pacific NW Natl Lab, Inst Integrated Catalysis, Richland, WA 99352 USA. RP Wang, JG (reprint author), Zhejiang Univ Technol, Coll Chem Engn, Hangzhou 310014, Zhejiang, Peoples R China. EM jgw@zjut.edu.cn RI Mei, Donghai/A-2115-2012; Li, Xiaonian/G-2026-2011; Mei, Donghai/D-3251-2011; Zhuang, Gui-lin/G-6531-2016 OI Mei, Donghai/0000-0002-0286-4182; FU National Basic Research Program of China (973 Program) [2013CB733501]; National Natural Science Foundation of China [NSFC-21306169, 21176221, 21136001, 21101137, 91334103]; Zhejiang Provincial Natural Science Foundation of China [ZJNSF-R4110345]; New Century Excellent Talents in University Program [NCET-10-0979] FX This work was supported by the National Basic Research Program of China (973 Program) (2013CB733501), the National Natural Science Foundation of China (NSFC-21306169, 21176221, 21136001, 21101137 and 91334103), Zhejiang Provincial Natural Science Foundation of China (ZJNSF-R4110345) and the New Century Excellent Talents in University Program (NCET-10-0979). We thank Prof. Youqun Zhu for Instruments support. NR 38 TC 8 Z9 8 U1 2 U2 31 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 2014 VL 2 IS 19 BP 6703 EP 6707 DI 10.1039/c4ta00647j PG 5 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA AF6PA UT WOS:000334835800002 ER PT J AU Sun, XG Liao, C Baggetto, L Guo, BK Unocic, RR Veith, GM Dai, S AF Sun, Xiao-Guang Liao, Chen Baggetto, Loic Guo, Bingkun Unocic, Raymond R. Veith, Gabriel M. Dai, Sheng TI Bis(fluoromalonato)borate (BFMB) anion based ionic liquid as an additive for lithium-ion battery electrolytes SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID PROPYLENE CARBONATE SOLUTIONS; GRAPHITE-ELECTRODES; INTERFACIAL REACTIONS; SULFONE ELECTROLYTES; LIBOB; BIS(OXALATO)BORATE; INTERCALATION; CONDUCTIVITY; DEPENDENCE; STABILITY AB Propylene carbonate (PC) is a good solvent for lithium ion battery applications due to its low melting point and high dielectric constant. However, PC is easily intercalated into graphite causing it to exfoliate, killing its electrochemical performance. Here we report on the synthesis of a new ionic liquid electrolyte based on partially fluorinated borate anion, 1-butyl-1,2-dimethylimidazolium bis(fluoromalonato)borate (BDMIm center dot BFMB), which can be used as an additive in 1 M LiPF6/PC electrolyte to suppress graphite exfoliation and improve cycling performance. In addition, both PC and BDMIm center dot BFMB can be used synergistically as additive to 1.0 M LiPF6/methyl isopropyl sulfone (MIPS) to dramatically improve its cycling performance. It is also found that the chemistry nature of the ionic liquids has dramatic effect on their role as additive in PC based electrolyte. C1 [Sun, Xiao-Guang; Liao, Chen; Guo, Bingkun; Dai, Sheng] Oak Ridge Natl Lab, Chem Sci Div, Oak Ridge, TN 37831 USA. [Baggetto, Loic; Veith, Gabriel M.] Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN 37831 USA. [Unocic, Raymond R.] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. [Dai, Sheng] Univ Tennessee, Dept Chem, Knoxville, TN 37996 USA. RP Sun, XG (reprint author), Oak Ridge Natl Lab, Chem Sci Div, One Bethel Valley Rd, Oak Ridge, TN 37831 USA. EM sunx@ornl.gov RI Guo, Bingkun/J-5774-2014; Dai, Sheng/K-8411-2015; Baggetto, Loic/D-5542-2017; OI Dai, Sheng/0000-0002-8046-3931; Baggetto, Loic/0000-0002-9029-2363; Liao, Chen/0000-0001-5168-6493; Unocic, Raymond/0000-0002-1777-8228 FU U.S. Department of Energy's Office of Basic Energy Science, Division of Materials Sciences and Engineering; ORNL's Center for Nanophase Materials Sciences (CNMS); Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy FX This research was supported by the U.S. Department of Energy's Office of Basic Energy Science, Division of Materials Sciences and Engineering and through a user project supported by ORNL's Center for Nanophase Materials Sciences (CNMS), which is sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy. NR 33 TC 8 Z9 8 U1 8 U2 54 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 2014 VL 2 IS 20 BP 7606 EP 7614 DI 10.1039/c3ta14943a PG 9 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA AF8XH UT WOS:000334998400062 ER PT J AU Saha, A Chattopadhyay, S Shibata, T Viswanatha, R AF Saha, Avijit Chattopadhyay, Soma Shibata, Tomohiro Viswanatha, Ranjani TI The curious case of CdTe/CdS: photoabsorption versus photoemission SO JOURNAL OF MATERIALS CHEMISTRY C LA English DT Article ID LIGHT-EMITTING DEVICES; QUANTUM DOTS; SEMICONDUCTOR NANOCRYSTALS; HIGHLY LUMINESCENT; NANOPARTICLES; IFEFFIT; DIODES AB The potential of nanomaterials arises from the fine tuning of material properties by changing their composition, size and shape. Here, we show that by varying the local Cd and Te/S environment using CdTe/CdS as the host, a highly promising photovoltaicmaterial can be easily converted to an efficient photo-emitting material. Thus we demonstrate for the first time that the internal structure can be used to tune the properties of the nanomaterial leading to competing and contrasting applications. C1 [Saha, Avijit; Viswanatha, Ranjani] Jawaharlal Nehru Ctr Adv Sci Res, New Chem Unit, Bangalore 560064, Karnataka, India. [Chattopadhyay, Soma; Shibata, Tomohiro] Argonne Natl Lab, MRCAT, CSRRI IIT, Argonne, IL 60439 USA. [Chattopadhyay, Soma; Shibata, Tomohiro] Illinois Inst Technol, Dept Phys, Adv Mat Grp, Chicago, IL 60616 USA. [Viswanatha, Ranjani] Jawaharlal Nehru Ctr Adv Sci Res, Int Ctr Mat Sci, Bangalore 560064, Karnataka, India. RP Viswanatha, R (reprint author), Jawaharlal Nehru Ctr Adv Sci Res, New Chem Unit, Bangalore 560064, Karnataka, India. EM rv@jncasr.ac.in RI ID, MRCAT/G-7586-2011 FU JNCASR; Sheikh Saqr Laboratory; Department of Science and Technology, Government of India; CSIR; U.S. DOE [DE-AC02-06CH11357] FX AS and RV thank JNCASR, Sheikh Saqr Laboratory and Department of Science and Technology, Government of India for financial support. AS thanks CSIR for a research fellowship. We thank Dr Vladislav Zyryanov for designing the sample cells for EXAFS. MRCAT operations were supported by the Department of Energy and the MRCAT member institutions. Use of the Advanced Photon Source, an Office of Science User Facilities 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. NR 32 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 2050-7526 EI 2050-7534 J9 J MATER CHEM C JI J. Mater. Chem. C PY 2014 VL 2 IS 20 BP 3868 EP 3872 DI 10.1039/c4tc00300d PG 5 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA AG2DL UT WOS:000335226100001 ER PT J AU Pol, VG Wen, JG Miller, DJ Thackeray, MM AF Pol, Vilas G. Wen, Jianguo Miller, Dean J. Thackeray, Michael M. TI Sonochemical Deposition of Sn, SnO2 and Sb on Spherical Hard Carbon Electrodes for Li-Ion Batteries SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID RECHARGEABLE LITHIUM BATTERIES; ANODE MATERIAL; ELECTROCHEMICAL PERFORMANCE; INSERTION ELECTRODE; OPTICAL-PROPERTIES; C NANOCOMPOSITE; LOW-TEMPERATURE; ALLOY ANODES; SPHERES; NANOPARTICLES AB Sonochemical deposition of Sn, SnO2 and Sb nanoparticles on the surface of autogenically-prepared hard carbon spheres increases their capacity for accommodating lithium, thereby rendering these carbon composite materials promising negative electrodes for advanced lithium-ion electrochemical cells. Preliminary data indicate that the carbon spheres, which offer a base capacity of similar to 250 mAh/g, can provide between 300 and 400 mAh/g with excellent cycling stability when decorated with 10-15 wt% Sn, SnO2 and Sb nanoparticles. The latter value exceeds the theoretical capacity of conventional graphite electrodes (LiC6, 372 mAh/g), suggesting that the Sn, SnO2 and Sb nanoparticles remain tethered to, and maintain electrical connectivity with, the carbon substrate during electrochemical cycling. Compositional, morphological, structural and electrochemical properties of these carbon composite materials are presented and discussed with respect to other types of previously reported architectures composed of carbon, tin and/or antimony. (C) 2014 The Electrochemical Society. All rights reserved. C1 [Pol, Vilas G.; Thackeray, Michael M.] Argonne Natl Lab, Chem Sci & Engn Div, Electrochem Energy Storage Dept, Lemont, IL 60439 USA. [Wen, Jianguo; Miller, Dean J.] Argonne Natl Lab, Electron Microscopy Ctr, Lemont, IL 60439 USA. RP Pol, VG (reprint author), Purdue Univ, Sch Chem Engn, W Lafayette, IN 47907 USA. EM vpol@purdue.edu; thackeray@anl.gov FU Center for Electrical Energy Storage - Tailored Interfaces, an Energy Frontier Research Center; Office of Science, Office of Basic Energy Sciences; U.S. Department of Energy Office of Science laboratory [DE-AC02-06CH11357] FX The initial work on the preparation and electrochemical characterization of the carbon spheres and tin-coated samples was supported by DOE-EERE, Office of Vehicle Technologies; the later work on the synthesis of the Sn/Sb-coated spheres and SEM/TEM characterization was funded by the Center for Electrical Energy Storage - Tailored Interfaces, an Energy Frontier Research Center funded by the Office of Science, Office of Basic Energy Sciences. Superior Graphite is thanked for undertaking the high-temperature heating of the spherical carbon particles. Use of the FE-SEM facilities at Argonne's Center for Nano-scale Materials (CNM) and SEM/TEM facilities at Electron Microscopy Center (EMC) is also gratefully acknowledged.; 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, 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 50 TC 5 Z9 5 U1 8 U2 57 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 2014 VL 161 IS 5 BP A777 EP A782 DI 10.1149/2.064405jes PG 6 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA AG3CD UT WOS:000335292500018 ER PT J AU Woo, JJ Maroni, VA Liu, G Vaughey, JT Gosztola, DJ Amine, K Zhang, ZC AF Woo, Jung-Je Maroni, Victor A. Liu, Gao Vaughey, John T. Gosztola, David J. Amine, Khalil Zhang, Zhengcheng TI Symmetrical Impedance Study on Inactivation Induced Degradation of Lithium Electrodes for Batteries Beyond Lithium-Ion SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID SURFACE-MORPHOLOGY; CYCLING EFFICIENCY; LI; METAL; ELECTROLYTES; SPECTROSCOPY; PERFORMANCE; CARBONATE; INSIGHTS AB The degradation of the lithium (Li) electrode was investigated based on its structural transformation due to the inactivation of deposited Li using a Copper/LiNi1/3Mn1/3Co1/3O2 (NMC) cell and a Li vertical bar Li symmetrical cell. Depletion of active Li turned out to be the major reason for the failure of the Li electrode under our experimental conditions. Following the first charging (Li-deposition) of the Copper/NMC cell, the discharge process only recovered 23% of the total deposited Li back to the NMC cathode. Electrochemical impedance spectroscopy (EIS) experiments of the Li vertical bar Li symmetric cell demonstrated that the repeated inactivation during the deposition process leads to the growth of the deposited Li layer thereby forming three interfacial structures most likely originating from (i) residual Li vertical bar liquid electrolyte, (ii) cycled Li in the inner deposited Li layer vertical bar liquid electrolyte, and (iii) cycled Li on the outer deposited Li layer vertical bar liquid electrolyte. The voltage profile and EIS of the symmetric cell could be correlated with the degradation behavior exhibited by the Li electrode. (C) 2014 The Electrochemical Society. All rights reserved. C1 [Woo, Jung-Je; Maroni, Victor A.; Vaughey, John T.; Amine, Khalil; Zhang, Zhengcheng] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. [Liu, Gao] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. [Gosztola, David J.] Argonne Natl Lab, Nanosci & Technol Div, Argonne, IL 60439 USA. RP Woo, JJ (reprint author), Argonne Natl Lab, Chem Sci & Engn Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM zzhang@anl.gov RI Gosztola, David/D-9320-2011; OI Gosztola, David/0000-0003-2674-1379; Vaughey, John/0000-0002-2556-6129 FU Integrated Laboratory/Industry Research Project (ILIRP), Vehicle Technologies office, U.S. Department of Energy; U.S. Department of Energy by UChicago Argonne, LLC [DE-AC02-06CH11357] FX This research was supported by the Integrated Laboratory/Industry Research Project (ILIRP), Vehicle Technologies office, U.S. Department of Energy. The Raman spectroscopy measurements were performed at the Center for Nanoscale Materials (CNM) at Argonne National Laboratory. Use of the CNM was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences. Argonne National Laboratory is operated for the U.S. Department of Energy by UChicago Argonne, LLC, under contract DE-AC02-06CH11357. JJ Woo thanks Dr. Dennis W. Dees for insightful discussions. NR 25 TC 5 Z9 5 U1 3 U2 39 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 2014 VL 161 IS 5 BP A827 EP A830 DI 10.1149/2.089405jes PG 4 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA AG3CD UT WOS:000335292500025 ER PT J AU Papandrew, AB Wilson, DL Cantillo, NM Hawks, S Atkinson, RW Goenaga, GA Zawodzinski, TA AF Papandrew, Alexander B. Wilson, David L., III Cantillo, Nelly M. Hawks, Samantha Atkinson, Robert W., III Goenaga, Gabriel A. Zawodzinski, Thomas A., Jr. TI Electrochemical Hydrogen Separation via Solid Acid Membranes SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID ELECTROLYTE FUEL-CELL; EVOLUTION REACTIONS; PROTON CONDUCTORS; CARBON-MONOXIDE; CO; OXIDATION; STEAM; ELECTROOXIDATION; PERFORMANCE; REFORMATE AB The inorganic proton conductor CsH2PO4 (CDP) was investigated as a proton exchange membrane for electrochemical hydrogen separation at temperatures from 230 degrees C to 250 degrees C. Carbon-supported Pt and Pd were synthesized via vapor deposition and evaluated as hydrogen oxidation catalysts in hydrogen pump electrodes. The hydrogen oxidation and evolution reactions were reversible on Pt in 100% H-2, and a cell current of 300 mA cm(-2) was produced at a 25 mV overpotential after correction for the membrane ohmic resistance. Anodes were also exposed to hydrogen-containing gas mixtures to simulate reformed fuels. In the case of a stream containing 7% CO (75% H-2, balance CO2), a 300 mA cm(-2) cell current required 45 mV electrode polarization, and in a stream containing 10% CO and 0.25% CH4 (43% H-2, balance N-2, CO2), 75 mV polarization was required to obtain the same current. The performance of carbon-supported Pd was virtually identical to that of Pt under each of these conditions. (C) 2014 The Electrochemical Society. All rights reserved. C1 [Papandrew, Alexander B.; Wilson, David L., III; Cantillo, Nelly M.; Hawks, Samantha; Atkinson, Robert W., III; Goenaga, Gabriel A.; Zawodzinski, Thomas A., Jr.] Univ Tennessee, Dept Chem & Biomol Engn, Knoxville, TN 37996 USA. [Zawodzinski, Thomas A., Jr.] Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. [Zawodzinski, Thomas A., Jr.] King Abdulaziz Univ, Dept Chem, Jeddah 21413, Saudi Arabia. RP Papandrew, AB (reprint author), Univ Tennessee, Dept Chem & Biomol Engn, Knoxville, TN 37996 USA. EM apapandrew@utk.edu RI Cantillo, Nelly/B-4672-2016 OI Cantillo, Nelly/0000-0002-9616-4135 FU Office of Naval Research [N000141210887]; Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy FX This work was supported by the Office of Naval Research (Award N000141210887). A portion of this research was 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. NR 35 TC 9 Z9 9 U1 3 U2 28 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 2014 VL 161 IS 5 BP F679 EP F685 DI 10.1149/2.078405jes PG 7 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA AG3CD UT WOS:000335292500074 ER PT J AU Lancaster, WA Menon, AL Scott, I Poole, FL Vaccaro, BJ Thorgersen, MP Geller, J Hazen, TC Hurt, RA Brown, SD Elias, DA Adams, MWW AF Lancaster, W. Andrew Menon, Angeli Lal Scott, Israel Poole, Farris L. Vaccaro, Brian J. Thorgersen, Michael P. Geller, Jil Hazen, Terry C. Hurt, Richard A., Jr. Brown, Steven D. Elias, Dwayne A. Adams, Michael W. W. TI Metallomics of two microorganisms relevant to heavy metal bioremediation reveal fundamental differences in metal assimilation and utilization SO METALLOMICS LA English DT Article ID DESULFOVIBRIO-VULGARIS HILDENBOROUGH; SULFATE-REDUCING BACTERIA; ENTEROBACTER-CLOACAE COMPLEX; MICROBIAL COMMUNITY; URANIUM REDUCTION; STRAIN; REMOVAL; EXPRESSION; CHROMATE; GENOME AB Although as many as half of all proteins are thought to require a metal cofactor, the metalloproteomes of microorganisms remain relatively unexplored. Microorganisms from different environments are likely to vary greatly in the metals that they assimilate, not just among the metals with well-characterized roles but also those lacking any known function. Herein we investigated the metal utilization of two microorganisms that were isolated from very similar environments and are of interest because of potential roles in the immobilization of heavy metals, such as uranium and chromium. The metals assimilated and their concentrations in the cytoplasm of Desulfovibrio vulgaris strain Hildenborough (DvH) and Enterobacter cloacae strain Hanford (EcH) varied dramatically, with a larger number of metals present in Enterobacter. For example, a total of 9 and 19 metals were assimilated into their cytoplasmic fractions, respectively, and DvH did not assimilate significant amounts of zinc or copper whereas EcH assimilated both. However, bioinformatic analysis of their genome sequences revealed a comparable number of predicted metalloproteins, 813 in DvH and 953 in EcH. These allowed some rationalization of the types of metal assimilated in some cases (Fe, Cu, Mo, W, V) but not in others (Zn, Nd, Ce, Pr, Dy, Hf and Th). It was also shown that U binds an unknown soluble protein in EcH but this incorporation was the result of extracellular U binding to cytoplasmic components after cell lysis. C1 [Lancaster, W. Andrew; Menon, Angeli Lal; Scott, Israel; Poole, Farris L.; Vaccaro, Brian J.; Thorgersen, Michael P.; Adams, Michael W. W.] Univ Georgia, Dept Biochem & Mol Biol, Athens, GA 30602 USA. [Geller, Jil] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, Berkeley, CA 94720 USA. [Hazen, Terry C.] Univ Tennessee, Dept Earth & Planetary Sci, Knoxville, TN 37996 USA. [Hazen, Terry C.; Hurt, Richard A., Jr.; Brown, Steven D.; Elias, Dwayne A.] Oak Ridge Natl Lab, Biosci Div, Oak Ridge, TN 37831 USA. RP Adams, MWW (reprint author), Univ Georgia, Dept Biochem & Mol Biol, Life Sci Bldg, Athens, GA 30602 USA. EM adams@bmb.uga.edu RI Brown, Steven/A-6792-2011; Hazen, Terry/C-1076-2012 OI Brown, Steven/0000-0002-9281-3898; Hazen, Terry/0000-0002-2536-9993 FU ENIGMA - Ecosystems and Networks Integrated with Genes and Molecular Assemblies; Office of Science, Office of Biological and Environmental Research, of the U. S. Department of Energy [DE-AC02-05CH11231] FX This research was funded 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 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. NR 55 TC 6 Z9 6 U1 3 U2 32 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1756-5901 EI 1756-591X J9 METALLOMICS JI Metallomics PY 2014 VL 6 IS 5 BP 1004 EP 1013 DI 10.1039/c4mt00050a PG 10 WC Biochemistry & Molecular Biology SC Biochemistry & Molecular Biology GA AG1BF UT WOS:000335149200004 PM 24706256 ER PT J AU Jiang, DE Wu, JZ AF Jiang, De-en Wu, Jianzhong TI Unusual effects of solvent polarity on capacitance for organic electrolytes in a nanoporous electrode SO NANOSCALE LA English DT Article ID DOUBLE-LAYER CAPACITORS; IONIC LIQUID ELECTROLYTE; CARBON SUPERCAPACITORS; ELECTROCHEMICAL CAPACITORS; SUBNANOMETER PORES; ENERGY-STORAGE; NONAQUEOUS ELECTROLYTES; ACYLAMINO GROUP; GRAPHENE; SIZE AB The interplay between ions and solvent molecules inside the nanoporous electrodes of a supercapacitor has not been well understood but could be a fertile ground for new insights into the device's performance. By tuning the dipole moment of the solvent in an organic electrolyte, we find, from classical density functional theory calculations, pronounced oscillation of capacitance with the pore size for a moderately to weakly polar solvent. A quantitative analysis of the electric-double-layer (EDL) structure indicates that the capacitance oscillation shares a similar physical origin to that of an ionic liquid electrolyte: the oscillatory behavior arises from the formation of alternating layers of counterions and coions near strongly charged surfaces. More interestingly, we find that in the large-pore region, the capacitance versus the pore size has a volcano-shaped trend; in other words, there exists a solvent dipole moment that yields a maximal capacitance. These theoretical predictions can be validated with future experiments and highlight the great potential in tuning the organic solvent to achieve optimal performance of EDL capacitors. C1 [Jiang, De-en] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. [Wu, Jianzhong] Univ Calif Riverside, Dept Chem & Environm Engn, Riverside, CA 92521 USA. RP Jiang, DE (reprint author), Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. EM jiangd@ornl.gov; jwu@engr.ucr.edu RI Jiang, De-en/D-9529-2011; OI Jiang, De-en/0000-0001-5167-0731; Wu, Jianzhong/0000-0002-4582-5941 FU Fluid Interface Reactions, Structures, and Transport (FIRST) Center, an Energy Frontier Research Center - U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences FX This work was supported by the Fluid Interface Reactions, Structures, and Transport (FIRST) Center, an Energy Frontier Research Center funded by the U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences. NR 58 TC 16 Z9 16 U1 5 U2 46 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 2014 VL 6 IS 10 BP 5545 EP 5550 DI 10.1039/c4nr00046c PG 6 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA AG1BB UT WOS:000335148800070 PM 24733527 ER PT J AU Li, MY Pattathil, S Hahn, MG Hodge, DB AF Li, Muyang Pattathil, Sivakumar Hahn, Michael G. Hodge, David B. TI Identification of features associated with plant cell wall recalcitrance to pretreatment by alkaline hydrogen peroxide in diverse bioenergy feedstocks using glycome profiling SO RSC ADVANCES LA English DT Article ID ENZYMATIC-HYDROLYSIS; CORN STOVER; BIOMASS; DIGESTIBILITY; GRASSES; POPLAR; XYLOSE; DECONSTRUCTION; ACCESSIBILITY; FERMENTATION AB A woody dicot (hybrid poplar), an herbaceous dicot (goldenrod), and a graminaceous monocot (corn stover) were subjected to alkaline hydrogen peroxide (AHP) pretreatment and subsequent enzymatic hydrolysis in order to assess how taxonomically and structurally diverse biomass feedstocks respond to a mild alkaline oxidative pretreatment and how differing features of the cell wall matrix contribute to its recalcitrance. Using glycome profiling, we determined changes in the extractability of non-cellulosic glucans following pretreatment by screening extracts of the pretreated walls with a panel of 155 cell wall glycan-directed monoclonal antibodies to determine differences in the abundance and distribution of non-cellulosic glycan epitopes in these extracts and assess pretreatment-induced changes in the structural integrity of the cell wall. Two taxonomically-dependent outcomes of pretreatment were identified that both improved the subsequent enzymatic hydrolysis yields but differed in their impacts on cell wall structural integrity. Specifically, it was revealed that goldenrod walls exhibited decreases in all classes of alkali-extractable glycans indicating their solubilization during pretreatment, which was accompanied by an improvement in the subsequent extractability of the remaining cell wall glycans. The corn stover walls did not show the same decreases in glycan abundance in extracts following pretreatment, but rather mild increases in all classes of cell wall glycans, indicating overall weaker associations between cell wall polymers and improved extractability. The hybrid poplar walls were relatively unaffected by pretreatment in terms of composition, enzymatic hydrolysis, and the extractability of cell wall glycans due presumably to their higher lignin content and denser vascular structure. C1 [Li, Muyang; Hodge, David B.] Michigan State Univ, Dept Biosyst & Agr Engn, E Lansing, MI 48824 USA. [Li, Muyang; Hodge, David B.] Michigan State Univ, Great Lakes Bioenergy Res Ctr, E Lansing, MI 48824 USA. [Pattathil, Sivakumar; Hahn, Michael G.] Univ Georgia, Complex Carbohydrate Res Ctr, Athens, GA 30602 USA. [Pattathil, Sivakumar; Hahn, Michael G.] Oak Ridge Natl Lab, BioEnergy Sci Ctr BESC, Oak Ridge, TN 37831 USA. [Hahn, Michael G.] Univ Georgia, Dept Plant Biol, Athens, GA 30602 USA. [Hodge, David B.] Michigan State Univ, Dept Mat Sci & Chem Engn, E Lansing, MI 48824 USA. [Hodge, David B.] Lulea Univ Technol, Div Sustainable Proc Engn, S-95187 Lulea, Sweden. RP Hodge, DB (reprint author), Michigan State Univ, Dept Biosyst & Agr Engn, E Lansing, MI 48824 USA. EM hodgeda@egr.msu.edu OI , Sivakumar Pattathil/0000-0003-3870-4137 FU DOE Great Lakes Bioenergy Research Center (DOE BER Office of Science) [DE-FC02-07ER64494, DE-AC05-00OR22725]; BioEnergy Science Center administered by Oak Ridge National Laboratory; NSF Plant Genome Program [DBI-0421683, IOS-0923992, 1336622] FX This work was funded by the DOE Great Lakes Bioenergy Research Center (DOE BER Office of Science DE-FC02-07ER64494) and the BioEnergy Science Center administered by Oak Ridge National Laboratory, and funded by a grant (DOE BER Office of Science DE-AC05-00OR22725). The generation of the CCRC series of plant cell wall glycan-directed monoclonal antibodies used in this work was supported by the NSF Plant Genome Program (DBI-0421683 and IOS-0923992). Muyang Li was supported in part by a grant from NSF (NSF CBET 1336622). NR 52 TC 10 Z9 10 U1 2 U2 19 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 2014 VL 4 IS 33 BP 17282 EP 17292 DI 10.1039/c4ra00824c PG 11 WC Chemistry, Multidisciplinary SC Chemistry GA AG2DR UT WOS:000335226700057 ER PT J AU Gulliver, DM Lowry, GV Gregory, KB AF Gulliver, Djuna M. Lowry, Gregory V. Gregory, Kelvin B. TI CO2 concentration and pH alters subsurface microbial ecology at reservoir temperature and pressure SO RSC ADVANCES LA English DT Article ID 16S RIBOSOMAL-RNA; LONG-TERM EXPERIMENTS; IN-SITU CONDITIONS; CARBON-DIOXIDE; SUBSEAFLOOR SEDIMENTS; PHYLOGENETIC ANALYSES; PETROLEUM RESERVOIRS; CALCIUM-CARBONATE; SP. NOV.; DEEP-SEA AB The security of long-term CO2 storage following geologic carbon sequestration may be impacted by biogeochemical reactions in the formation; yet little understanding exists about the impact of CO2 gradients on microorganisms that drive biogeochemistry in the deep subsurface. The effect of CO2 gradients on the microbial community from a brine aquifer was examined at reservoir pressure (14 MPa) and temperature (40 degrees C). The community was exposed to pCO(2) at 0, 0.1, 1.4 and 14 MPa for up to 56 days and was examined using 16S rRNA gene clone libraries and qPCR. Diversity indices (equitability) were also determined. In addition, the effect of lowered pH without CO2 exposure was examined. Exposure to CO2 resulted in a decrease in microbial diversity and a decrease in 16S rRNA gene concentrations. After 56 days, no 16S genes were recovered following exposure to 1.4 MPa pCO(2) or greater. Exposure to 0.1 MPa pCO(2) resulted in 16S gene concentrations an order of magnitude less than 0 MPa pCO(2). The equitability of 0 MPa exposure (0.54) decreased with 0.1 MPa exposure to 0.29. Microbial community with the lowered pH (pH = 4.4) and 0 MPa pCO(2) resulted in 5 orders of magnitude increased 16S gene concentration than reactors with CO2 exposure, indicating that CO2 was detrimental independent of pH. This suggests that even buffered reservoirs may have a decreased microbial population due to injected CO2. Halotolerant strains Halomonas and Marinobacter appeared to be the most tolerant to CO2 exposure and decreased pH. This is the first study to examine the initial microbial community response to a gradient of CO2 that would follow geologic carbon sequestration. C1 [Gulliver, Djuna M.; Lowry, Gregory V.; Gregory, Kelvin B.] Natl Energy Technol Lab, Off Res & Dev, Pittsburgh, PA 15236 USA. [Gulliver, Djuna M.; Lowry, Gregory V.; Gregory, Kelvin B.] Carnegie Mellon Univ, Dept Civil & Environm Engn, Pittsburgh, PA 15213 USA. RP Gregory, KB (reprint author), Natl Energy Technol Lab, Off Res & Dev, Pittsburgh, PA 15236 USA. EM kelvin@cmu.edu RI Gulliver, Djuna/H-8182-2014; OI Gulliver, Djuna/0000-0003-4219-5849; Gregory, Kelvin/0000-0001-5488-2297 NR 72 TC 4 Z9 5 U1 3 U2 23 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 2014 VL 4 IS 34 BP 17443 EP 17453 DI 10.1039/c4ra02139h PG 11 WC Chemistry, Multidisciplinary SC Chemistry GA AG2EA UT WOS:000335227700006 ER PT J AU Rahman, A Sarma, A Gayen, S Sanyal, MK AF Rahman, Atikur Sarma, Abhisakh Gayen, Sirshendu Sanyal, Milan K. TI Asymmetric water diffusion driven nanotube actuator SO RSC ADVANCES LA English DT Article ID SHAPE-MEMORY POLYMERS; ARTIFICIAL MUSCLES; CARBON NANOTUBES; CHANNELS; LIGHT; FILMS; FLOW AB Here we report, water vapor driven actuation of polymer nanotubes, embedded in a nanoporous membrane with one end attached to a surface deposited thin polymer layer. The nanotube composite shows oscillatory motion when placed near water. Permeation of water vapor through these nanotube embedded membranes is found to be direction dependent. With the water vapor as the driving force, the actuator can lift a mass 1000 times heavier than itself with a change in relative humidity of less than 40%. The actuation mechanism arises due to efficient absorption of water molecules by polymer nanotubes and their rapid evaporation through the surface deposited polymer layer. This actuator can be used as artificial muscle and the direction dependent water transport may help in understanding the activities of transmembrane channels and pumps of biological cells. With the aid of a nanowire generator, the oscillatory motion can be used to generate electricity too. C1 [Rahman, Atikur; Sarma, Abhisakh; Gayen, Sirshendu; Sanyal, Milan K.] Saha Inst Nucl Phys, Surface Phys Div, Kolkata 700064, W Bengal, India. RP Rahman, A (reprint author), Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. EM arahman@bnl.gov; milank.sanyal@saha.ac.in RI sanyal, milan/J-2527-2015; OI sanyal, milan/0000-0002-3847-8793; Rahman, Atikur/0000-0002-1275-7129 NR 34 TC 3 Z9 3 U1 7 U2 35 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 2014 VL 4 IS 34 BP 17573 EP 17578 DI 10.1039/c4ra00153b PG 6 WC Chemistry, Multidisciplinary SC Chemistry GA AG2EA UT WOS:000335227700022 ER PT B AU Clark, RM Hakim, S AF Clark, Robert M. Hakim, Simon BE Clark, RM Hakim, S TI Securing Water and Wastewater Systems: Global Perspectives SO SECURING WATER AND WASTEWATER SYSTEMS: GLOBAL EXPERIENCES SE Protecting Critical Infrastructure LA English DT Article; Book Chapter ID CLIMATE-CHANGE; OUTBREAK; MILWAUKEE; QUALITY; IMPACTS C1 [Clark, Robert M.] Univ Cincinnati, Cincinnati, OH 45221 USA. [Clark, Robert M.] Sandia Natl Labs, Livermore, CA 94550 USA. [Clark, Robert M.] US EPA, Washington, DC USA. [Clark, Robert M.] Rutgers State Univ, Piscataway, NJ 08855 USA. [Clark, Robert M.] US PHS, Rockville, MD USA. [Clark, Robert M.] US EPA, WSWRD, Washington, DC USA. [Hakim, Simon] Ctr Competit Govt, Fox Sch Business & Management, Philadelphia, PA 19122 USA. [Hakim, Simon] Temple Univ, Philadelphia, PA 19122 USA. RP Clark, RM (reprint author), 9627 Lansford Dr, Cincinnati, OH 45242 USA. EM rmclark@fuse.net; hakim@temple.edu NR 19 TC 0 Z9 0 U1 1 U2 1 PU SPRINGER-VERLAG BERLIN PI BERLIN PA HEIDELBERGER PLATZ 3, D-14197 BERLIN, GERMANY BN 978-3-319-01092-2; 978-3-319-01091-5 J9 PROT CRIT INFRASTRUC PY 2014 VL 2 BP 1 EP 27 DI 10.1007/978-3-319-01092-2_1 D2 10.1007/978-3-319-01092-2 PG 27 WC Engineering, Environmental; Engineering, Civil; Water Resources SC Engineering; Water Resources GA BA1ET UT WOS:000332421800001 ER PT B AU Janke, R Tryby, ME Clark, RM AF Janke, Robert Tryby, Michael E. Clark, Robert M. BE Clark, RM Hakim, S TI Protecting Water Supply Critical Infrastructure: An Overview SO SECURING WATER AND WASTEWATER SYSTEMS: GLOBAL EXPERIENCES SE Protecting Critical Infrastructure LA English DT Article; Book Chapter ID CONTAMINATION SOURCE IDENTIFICATION; DISTRIBUTION-SYSTEM CONTAMINATION; DRINKING-WATER; DISTRIBUTION NETWORKS; SENSOR PLACEMENT; WARNING SYSTEMS; PATHOGEN INTRUSION; UNITED-STATES; OUTBREAK; MODEL C1 [Janke, Robert] US EPA, Off Res & Dev, Natl Homeland Secur Res Ctr, Water Infrastruct & Protect Div, Cincinnati, OH 45268 USA. [Tryby, Michael E.] US EPA, Natl Risk Management Res Lab, Water Supply & Water Resources Div, Cincinnati, OH 45268 USA. [Clark, Robert M.] Univ Cincinnati, Cincinnati, OH 45221 USA. [Clark, Robert M.] Sandia Natl Labs, Livermore, CA 94550 USA. [Clark, Robert M.] US EPA, Washington, DC USA. [Clark, Robert M.] Rutgers State Univ, Piscataway, NJ 08855 USA. [Clark, Robert M.] US PHS, Rockville, MD USA. [Clark, Robert M.] US EPA, WSWRD, Washington, DC USA. RP Janke, R (reprint author), US EPA, Off Res & Dev, Natl Homeland Secur Res Ctr, Water Infrastruct & Protect Div, Cincinnati, OH 45268 USA. EM janke.robert@epa.gov; tryby.michael@epa.gov; rmclark@fuse.net NR 138 TC 1 Z9 1 U1 1 U2 7 PU SPRINGER-VERLAG BERLIN PI BERLIN PA HEIDELBERGER PLATZ 3, D-14197 BERLIN, GERMANY BN 978-3-319-01092-2; 978-3-319-01091-5 J9 PROT CRIT INFRASTRUC PY 2014 VL 2 BP 29 EP 85 DI 10.1007/978-3-319-01092-2_2 D2 10.1007/978-3-319-01092-2 PG 57 WC Engineering, Environmental; Engineering, Civil; Water Resources SC Engineering; Water Resources GA BA1ET UT WOS:000332421800002 ER PT B AU Clark, RM AF Clark, Robert M. BE Clark, RM Hakim, S TI The Impacts of Global Climate Change on Water Treatment Design and Operations SO SECURING WATER AND WASTEWATER SYSTEMS: GLOBAL EXPERIENCES SE Protecting Critical Infrastructure LA English DT Article; Book Chapter ID SEA-LEVEL RISE; ACTIVATED CARBON; SYSTEMS; GAC; PERFORMANCE; REMOVAL; QUALITY; COST C1 [Clark, Robert M.] Univ Cincinnati, Cincinnati, OH 45221 USA. [Clark, Robert M.] Sandia Natl Labs, Livermore, CA 94550 USA. [Clark, Robert M.] US EPA, Washington, DC USA. [Clark, Robert M.] Rutgers State Univ, Piscataway, NJ 08855 USA. [Clark, Robert M.] US PHS, Rockville, MD USA. [Clark, Robert M.] US EPA, WSWRD, Washington, DC USA. RP Clark, RM (reprint author), 9627 Lansford Dr, Cincinnati, OH 45242 USA. EM rmclark@fuse.net NR 31 TC 0 Z9 0 U1 0 U2 0 PU SPRINGER-VERLAG BERLIN PI BERLIN PA HEIDELBERGER PLATZ 3, D-14197 BERLIN, GERMANY BN 978-3-319-01092-2; 978-3-319-01091-5 J9 PROT CRIT INFRASTRUC PY 2014 VL 2 BP 251 EP 272 DI 10.1007/978-3-319-01092-2_12 D2 10.1007/978-3-319-01092-2 PG 22 WC Engineering, Environmental; Engineering, Civil; Water Resources SC Engineering; Water Resources GA BA1ET UT WOS:000332421800012 ER PT S AU Waychunas, GA AF Waychunas, Glenn A. BE Henderson, GS Neuville, DR Downs, RT TI Luminescence Spectroscopy SO SPECTROSCOPIC METHODS IN MINERALOLOGY AND MATERIALS SCIENCES SE Reviews in Mineralogy & Geochemistry LA English DT Review; Book Chapter ID DISSOLVED ORGANIC-MATTER; TIME-RESOLVED LUMINESCENCE; OPTICALLY STIMULATED LUMINESCENCE; LASER FLUORESCENCE SPECTROSCOPY; THERMO-LUMINESCENCE; ALKALI FELDSPARS; NATURAL FLUORITE; ALPHA-QUARTZ; ACTIVATED CATHODOLUMINESCENCE; PETROLOGICAL SIGNIFICANCE C1 EO Lawrence Berkeley Natl Lab, Dept Geochem, Div Earth Sci, Berkeley, CA 94720 USA. RP Waychunas, GA (reprint author), EO Lawrence Berkeley Natl Lab, Dept Geochem, Div Earth Sci, One Cyclotron Rd,MS 74-316C, Berkeley, CA 94720 USA. EM gawaychunas@lbl.gov NR 177 TC 1 Z9 1 U1 2 U2 27 PU MINERALOGICAL SOC AMER PI CHANTILLY PA 3635 CONCORDE PKWY STE 500, CHANTILLY, VA 20151-1125 USA SN 1529-6466 BN 978-0-939950-93-5 J9 REV MINERAL GEOCHEM JI Rev. Mineral. Geochem. PY 2014 VL 78 BP 175 EP 217 DI 10.2138/rmg.2014.78.5 PG 43 WC Geochemistry & Geophysics; Mineralogy SC Geochemistry & Geophysics; Mineralogy GA BA3NO UT WOS:000334387700005 ER PT S AU Linder, EV AF Linder, E. V. BE Sathyaprakash, BS Singh, TP TI The direction of gravity SO VISHWA MIMANSA: AN INTERPRETATIVE EXPOSITION OF THE UNIVERSE. PROCEEDINGS OF THE 7TH INTERNATIONAL CONFERENCE ON GRAVITATION AND COSMOLOGY SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 7th International Conference on Gravitation and Cosmology (ICGC) CY DEC 14-19, 2011 CL INDIA SP Inter Univ Ctr Astronomy & Astrophys, Assoc Friends Astronomy, SINP, Ctr AstroParticle Phys, Dept Sci, Technol & Environm, Foundat Quest Inst, Harish Chandra Res Inst, Infosys Sci Fdn, Inst Math Sci, TATA Inst Fundamental Res, Int Ctr Theoret Sci, Indian Assoc Gen Relat & Gravitat AB Gravity directs the paths of light rays and the growth of structure. Moreover, gravity on cosmological scales does not simply point down: It accelerates the universal expansion by pulling outward, either due to a highly negative pressure dark energy or an extension of general relativity. We have examined methods to test the properties of gravity through cosmological measurements. We have then considered specific possibilities for a sound gravitational theory based on the Galilean shift symmetry. The evolution of the laws of gravity from the early universe to the present acceleration to the future fate - the paths of gravity carries rich information on this fundamental force of physics, and on the mystery of dark energy. C1 Berkeley Lab, Berkeley, CA 94720 USA. RP Linder, EV (reprint author), Berkeley Lab, Berkeley, CA 94720 USA. EM evlinder@lbl.gov NR 14 TC 0 Z9 0 U1 0 U2 1 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 484 AR 012006 DI 10.1088/1742-6596/484/1/012006 PG 8 WC Astronomy & Astrophysics SC Astronomy & Astrophysics GA BA4BF UT WOS:000335317500008 ER PT S AU Janjusic, T Kavi, K AF Janjusic, Tomislav Kavi, Krishna BE Hurson, A TI Hardware and Application Profiling Tools SO ADVANCES IN COMPUTERS, VOL 92 SE Advances in Computers LA English DT Article; Book Chapter ID SYSTEM SIMULATION; TIME MODEL; INSTRUMENTATION; FRAMEWORK; ACCURATE; MEMORY; ACCESS AB This chapter describes hardware and application profiling tools used by researchers and application developers. With over 30 years of research, there have been numerous tools developed and used, and it will be too difficult to include all of them here. Therefore, in this chapter, we describe various areas with a selection of widely accepted and recent tools. This chapter is intended for the beginning reader interested in exploring more about these topics. Numerous references are provided to help jump-start the interested reader into the area of hardware simulation and application profiling. We make an effort to clarify and correctly classify application profiling tools based on their scope, interdependence, and operation mechanisms. To visualize these features, we provide diagrams that explain various development relationships between interdependent tools. Hardware simulation tools are described into categories that elaborate on their scope. Therefore, we have covered areas of single to full-system simulation, power modeling, and network processors. C1 [Janjusic, Tomislav] Oak Ridge Natl Lab, Oak Ridge, TN 37830 USA. [Kavi, Krishna] Univ N Texas, NSF Ind Univ Cooperat Res Ctr Net Centr Software, Denton, TX 76203 USA. RP Janjusic, T (reprint author), Oak Ridge Natl Lab, Oak Ridge, TN 37830 USA. NR 71 TC 0 Z9 0 U1 1 U2 3 PU ELSEVIER ACADEMIC PRESS INC PI SAN DIEGO PA 525 B STREET, SUITE 1900, SAN DIEGO, CA 92101-4495 USA SN 0065-2458 BN 978-0-12-420232-0 J9 ADV COMPUT JI Adv. Comput. PY 2014 VL 92 BP 105 EP 160 DI 10.1016/B978-0-12-420232-0.00003-9 PG 56 WC Computer Science, Hardware & Architecture; Computer Science, Software Engineering; Computer Science, Theory & Methods SC Computer Science GA BA0CO UT WOS:000331017000003 ER PT J AU Ewing, RG Heredia-Langner, A Warner, MG AF Ewing, Robert G. Heredia-Langner, Alejandro Warner, Marvin G. TI Optimizing detection of RDX vapors using designed experiments for remote sensing SO ANALYST LA English DT Article ID REACTION-MASS-SPECTROMETRY; REAL-TIME DETECTION; VOLATILE ORGANIC-COMPOUNDS; ION MOBILITY SPECTROMETRY; ELECTROSPRAY-IONIZATION; PTR-MS; EXPLOSIVES; AIR; EXTRACTION AB This paper presents results of designed experiments performed to study the effect of four factors on the detection of RDX vapors from desorption into an atmospheric flow tube mass spectrometer (AFT- MS). The experiments initially included four independent factors: gas flow rate, desorption current, solvent evaporation time and RDX mass. The values of three detection responses, peak height, peak width, and peak area were recorded but only the peak height response was analyzed. Results from the first block of experiments indicated that solvent evaporation time was not statistically significant at the 95% confidence level. A second round of experiments was designed and executed using flow rate, current, and RDX mass as factors and the results were used to create a model to predict conditions resulting in maximum peak height. Those conditions were confirmed experimentally and used to obtain data for a calibration model. The calibration model represented RDX amounts ranging from 1 to 25 pg desorbed into an air flow of 7 L min(-1). Air samples from a shipping container that held 2 closed explosive storage magazines were collected on metal filaments for varying amounts for time ranging from 5 to 90 minutes. RDX was detected from all of the filaments sampled by desorption into the AFT- MS. From the calibration model, RDX vapor concentrations within the shipping container were calculated to be in the range of 1 to 50 parts-per-quadrillion (ppq(v)) from data collected on 2 separate days. C1 [Ewing, Robert G.; Heredia-Langner, Alejandro; Warner, Marvin G.] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Ewing, RG (reprint author), Pacific NW Natl Lab, 902 Battelle Blvd,POB 999, Richland, WA 99352 USA. EM robert.ewing@pnnl.gov FU Laboratory Directed Research and Development funding at Pacific Northwest National Laboratory FX This work was funded in part by Laboratory Directed Research and Development funding at Pacific Northwest National Laboratory. The Pacific Northwest National Laboratory is a multiprogram national laboratory operated for the U.S. Department of Energy by Battelle Memorial Institute. NR 33 TC 0 Z9 0 U1 2 U2 27 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 0003-2654 EI 1364-5528 J9 ANALYST JI Analyst PY 2014 VL 139 IS 10 BP 2440 EP 2448 DI 10.1039/c4an00125g PG 9 WC Chemistry, Analytical SC Chemistry GA AF5DM UT WOS:000334734200022 PM 24695634 ER PT J AU Fan, J Leung, LR DeMott, PJ Comstock, JM Singh, B Rosenfeld, D Tomlinson, JM White, A Prather, KA Minnis, P Ayers, JK Min, Q AF Fan, J. Leung, L. R. DeMott, P. J. Comstock, J. M. Singh, B. Rosenfeld, D. Tomlinson, J. M. White, A. Prather, K. A. Minnis, P. Ayers, J. K. Min, Q. TI Aerosol impacts on California winter clouds and precipitation during CalWater 2011: local pollution versus long-range transported dust (vol 14, pg 81, 2014) SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Correction C1 [Fan, J.; Leung, L. R.; Comstock, J. M.; Singh, B.; Tomlinson, J. M.] Pacific NW Natl Lab, Richland, WA 99352 USA. [DeMott, P. J.] Colorado State Univ, Dept Atmospher Sci, Ft Collins, CO 80523 USA. [Rosenfeld, D.] Hebrew Univ Jerusalem, Inst Earth Sci, IL-91904 Jerusalem, Israel. [White, A.] NOAA ESRL, R PSD2, Boulder, CO 80305 USA. [Prather, K. A.] Univ Calif San Diego, Scripps Inst Oceanog, Dept Chem & Biochem, La Jolla, CA 92093 USA. [Minnis, P.] NASA Langley Res Ctr LaRC, Hampton, VA USA. [Ayers, J. K.] Sci Syst & Applicat Inc, Hampton, VA USA. [Min, Q.] SUNY Albany, Atmospher Sci Res Ctr, Albany, NY 12203 USA. RP Fan, J (reprint author), Pacific NW Natl Lab, Richland, WA 99352 USA. EM jiwen.fan@pnnl.gov RI Fan, Jiwen/E-9138-2011; DeMott, Paul/C-4389-2011; Rosenfeld, Daniel/F-6077-2016 OI DeMott, Paul/0000-0002-3719-1889; Rosenfeld, Daniel/0000-0002-0784-7656 NR 1 TC 2 Z9 2 U1 1 U2 13 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 2014 VL 14 IS 6 BP 3063 EP 3064 DI 10.5194/acp-14-3063-2014 PG 2 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA AE6LP UT WOS:000334104700018 ER PT J AU Long, MS Keene, WC Easter, RC Sander, R Liu, X Kerkweg, A Erickson, D AF Long, M. S. Keene, W. C. Easter, R. C. Sander, R. Liu, X. Kerkweg, A. Erickson, D. TI Sensitivity of tropospheric chemical composition to halogen-radical chemistry using a fully coupled size-resolved multiphase chemistry-global climate system: halogen distributions, aerosol composition, and sensitivity of climate-relevant gases SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID MARINE BOUNDARY-LAYER; SEA-SALT AEROSOLS; COMMUNITY ATMOSPHERE MODEL; TROPICAL ATLANTIC-OCEAN; BROMINE CHEMISTRY; OZONE DESTRUCTION; ATOMIC CHLORINE; HALOCARBON MEASUREMENTS; NUMBER CONCENTRATIONS; REACTIVE CHLORINE AB Observations and model calculations indicate that highly non-linear multiphase atmospheric processes involving inorganic Cl and Br significantly impact tropospheric chemistry and composition, aerosol evolution, and radiative transfer. The sensitivity of global atmospheric chemistry to the production of marine aerosol and the associated activation and cycling of inorganic Cl and Br was investigated using a size-resolved multiphase coupled chemistry-global climate model (National Center for Atmospheric Research's Community Atmosphere Model (CAM) v3.6.33). Simulated results revealed strong meridional and vertical gradients in Cl and Br species. They also point to possible physicochemical mechanisms that may account for several previously unexplained phenomena, including the enrichment of Br- in submicron aerosol and the presence of a BrO maximum in the polar free troposphere. However, simulated total volatile inorganic Br mixing ratios in the troposphere were generally higher than observed, due in part to the overly efficient net production of BrCl. In addition, the emission scheme for marine aerosol and associated Br-, which is the only source for Br in the model, overestimates emission fluxes from the high-latitude Southern Ocean. Br in the stratosphere was lower than observed due to the lack of long-lived precursor organobromine species in the simulation. Comparing simulations using chemical mechanisms with and without reactive Cl and Br species demonstrates a significant temporal and spatial sensitivity of primary atmospheric oxidants (O-3, HOx, NOx), CH4, non-methane hydrocarbons (NMHCs), and dimethyl sulfide (DMS) to halogen cycling. Globally, halogen chemistry had relatively less impact on SO2 and non-sea-salt (nss) SO42- although significant regional differences were evident. Although variable geographically, much of this sensitivity is attributable to either over-vigorous activation of Br (primarily BrCl) via the chemical mechanism or overproduction of sea-salt aerosol simulated under higher-wind regimes. In regions where simulated mixing ratios of reactive Br and Cl fell within observed ranges, though, halogen chemistry drove large changes in oxidant fields and associated chemical processes relative to simulations with no halogens. However, the overall simulated impacts of Br chemistry globally are overestimated and thus caution is warranted in their interpretation. C1 [Long, M. S.] Harvard Univ, Sch Engn & Appl Sci, Cambridge, MA 02138 USA. [Keene, W. C.] Univ Virginia, Dept Environm Sci, Charlottesville, VA 22904 USA. [Easter, R. C.] Pacific NW Natl Lab, Atmospher Sci & Global Change Div, Richland, WA 99352 USA. [Sander, R.] Max Planck Inst Chem, Air Chem Dept, D-55020 Mainz, Germany. [Liu, X.] Univ Wyoming, Dept Atmospher, Laramie, WY 82071 USA. [Kerkweg, A.] Johannes Gutenberg Univ Mainz, Inst Atmospher Phys, D-55099 Mainz, Germany. [Erickson, D.] Oak Ridge Natl Lab, Comp Sci & Math Div, Oak Ridge, TN 37830 USA. RP Long, MS (reprint author), Harvard Univ, Sch Engn & Appl Sci, Cambridge, MA 02138 USA. EM mlong@seas.harvard.edu RI Liu, Xiaohong/E-9304-2011; Sander, Rolf/A-5725-2011 OI Liu, Xiaohong/0000-0002-3994-5955; Sander, Rolf/0000-0001-6479-2092 FU US Department of Energy's (DOE's) Office of Science through the Office of Biological and Environmental Research (BER) [DE-FG02-07ER64442, DE-SC0007120]; National Center for Computational Sciences at Oak Ridge National Laboratory; DOE's Office of Science (BER) [DE-AC05-00OR22725]; National Science Foundation; DOE's Office of Science (BER); US Department of Energy, Office of Science, Scientific Discovery through Advanced Computing (SciDAC) program; DOE [DE-AC06-76RLO 1830] FX The three reviewers and the editor provided constructive suggestions for improving the manuscript. Financial support was provided by the US Department of Energy's (DOE's) Office of Science through the Office of Biological and Environmental Research (BER, grant numbers DE-FG02-07ER64442 and DE-SC0007120 to the University of Virginia), a Global Change Education Program Graduate Research Environmental Fellowship, and the National Center for Computational Sciences at Oak Ridge National Laboratory, which is supported by DOE's Office of Science (BER) under contract DE-AC05-00OR22725. The CESM project is supported by the National Science Foundation and the DOE's Office of Science (BER). PNNL authors were funded by the US Department of Energy, Office of Science, Scientific Discovery through Advanced Computing (SciDAC) program. The Pacific Northwest National Laboratory is operated for DOE by Battelle Memorial Institute under contract DE-AC06-76RLO 1830. NR 101 TC 14 Z9 14 U1 5 U2 44 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 2014 VL 14 IS 7 BP 3397 EP 3425 DI 10.5194/acp-14-3397-2014 PG 29 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA AF3JO UT WOS:000334608400013 ER PT J AU Chin, M Diehl, T Tan, Q Prospero, JM Kahn, RA Remer, LA Yu, H Sayer, AM Bian, H Geogdzhayev, IV Holben, BN Howell, SG Huebert, BJ Hsu, NC Kim, D Kucsera, TL Levy, RC Mishchenko, MI Pan, X Quinn, PK Schuster, GL Streets, DG Strode, SA Torres, O Zhao, XP AF Chin, Mian Diehl, T. Tan, Q. Prospero, J. M. Kahn, R. A. Remer, L. A. Yu, H. Sayer, A. M. Bian, H. Geogdzhayev, I. V. Holben, B. N. Howell, S. G. Huebert, B. J. Hsu, N. C. Kim, D. Kucsera, T. L. Levy, R. C. Mishchenko, M. I. Pan, X. Quinn, P. K. Schuster, G. L. Streets, D. G. Strode, S. A. Torres, O. Zhao, X. -P. TI Multi-decadal aerosol variations from 1980 to 2009: a perspective from observations and a global model SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID NORTH-ATLANTIC OSCILLATION; LONG-TERM RECORD; OPTICAL DEPTH; AFRICAN DUST; TROPOSPHERIC AEROSOL; UNITED-STATES; GOCART MODEL; INTERCONTINENTAL TRANSPORT; AERONET MEASUREMENTS; TOMS OBSERVATIONS AB Aerosol variations and trends over different land and ocean regions from 1980 to 2009 are analyzed with the Goddard Chemistry Aerosol Radiation and Transport (GOCART) model and observations from multiple satellite sensors and available ground-based networks. Excluding time periods with large volcanic influence, aerosol optical depth (AOD) and surface concentration over polluted land regions generally vary with anthropogenic emissions, but the magnitude of this association can be dampened by the presence of natural aerosols, especially dust. Over the 30-year period in this study, the largest reduction in aerosol levels occurs over Europe, where AOD has decreased by 40-60% on average and surface sulfate concentrations have declined by a factor of up to 3-4. In contrast, East Asia and South Asia show AOD increases, but the relatively high level of dust aerosols in Asia reduces the correlation between AOD and pollutant emission trends. Over major dust source regions, model analysis indicates that the change of dust emissions over the Sahara and Sahel has been predominantly driven by the change of near-surface wind speed, but over Central Asia it has been largely influenced by the change of the surface wetness. The decreasing dust trend in the North African dust outflow region of the tropical North Atlantic and the receptor sites of Barbados and Miami is closely associated with an increase of the sea surface temperature in the North Atlantic. This temperature increase may drive the decrease of the wind velocity over North Africa, which reduces the dust emission, and the increase of precipitation over the tropical North Atlantic, which enhances dust removal during transport. Despite significant trends over some major continental source regions, the model-calculated global annual average AOD shows little change over land and ocean in the past three decades, because opposite trends in different land regions cancel each other out in the global average, and changes over large open oceans are negligible. This highlights the necessity for regional-scale assessment of aerosols and their climate impacts, as global-scale average values can obscure important regional changes. C1 [Chin, Mian; Diehl, T.; Tan, Q.; Kahn, R. A.; Yu, H.; Sayer, A. M.; Bian, H.; Holben, B. N.; Hsu, N. C.; Kim, D.; Kucsera, T. L.; Levy, R. C.; Pan, X.; Strode, S. A.; Torres, O.] NASA, Goddard Space Flight Ctr, Greenbelt, MD 20771 USA. [Diehl, T.; Tan, Q.; Sayer, A. M.; Kim, D.; Kucsera, T. L.; Strode, S. A.] Univ Space Res Assoc, Columbia, MD USA. [Prospero, J. M.] Univ Miami, Miami, FL USA. [Remer, L. A.; Bian, H.] Univ Maryland Baltimore Cty, Baltimore, MD 21228 USA. [Yu, H.] Univ Maryland, College Pk, MD 20742 USA. [Geogdzhayev, I. V.; Mishchenko, M. I.] NASA, Goddard Inst Space Studies, New York, NY 10025 USA. [Geogdzhayev, I. V.] Columbia Univ, New York, NY USA. [Howell, S. G.; Huebert, B. J.] Univ Hawaii, Honolulu, HI 96822 USA. [Quinn, P. K.] NOAA, Pacific Marine Environm Lab, Seattle, WA 98115 USA. [Schuster, G. L.] NASA, Langley Res Ctr, Hampton, VA 23665 USA. [Streets, D. G.] Argonne Natl Lab, Argonne, IL 60439 USA. [Zhao, X. -P.] NOAA, Natl Climat Data Ctr, Asheville, NC USA. RP Chin, M (reprint author), NASA, Goddard Space Flight Ctr, Greenbelt, MD 20771 USA. EM mian.chin@nasa.gov RI Torres, Omar/G-4929-2013; Mishchenko, Michael/D-4426-2012; Kim, Dongchul/H-2256-2012; Quinn, Patricia/R-1493-2016; Chin, Mian/J-8354-2012; Sayer, Andrew/H-2314-2012; Levy, Robert/M-7764-2013; Kahn, Ralph/D-5371-2012; Strode, Sarah/H-2248-2012; Yu, Hongbin/C-6485-2008 OI Kim, Dongchul/0000-0002-5659-1394; Quinn, Patricia/0000-0003-0337-4895; Prospero, Joseph/0000-0003-3608-6160; Sayer, Andrew/0000-0001-9149-1789; Levy, Robert/0000-0002-8933-5303; Kahn, Ralph/0000-0002-5234-6359; Strode, Sarah/0000-0002-8103-1663; Yu, Hongbin/0000-0003-4706-1575 FU NASA's Modeling, Analysis, and Prediction (MAP) program; Atmospheric Composition, Modeling, and Analysis Program (ACMAP); NASA Postdoctoral Program FX We thank the IMPROVE, EMEP, and AERONET networks for making their data available on line. Site PIs and data managers of these networks are gratefully acknowledged. We also thank the Goddard Earth Science Data and Information Services Center for providing gridded satellite products of SeaWiFS, MISR, and MODIS through their Giovanni website. We are grateful to three anonymous reviewers for their very constructive, helpful comments. This work is supported by NASA's Modeling, Analysis, and Prediction (MAP) program and the Atmospheric Composition, Modeling, and Analysis Program (ACMAP). X. Pan is supported by the NASA Postdoctoral Program, administrated by the Oak Ridge Associated University (ORAU). NR 109 TC 66 Z9 68 U1 4 U2 67 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 2014 VL 14 IS 7 BP 3657 EP 3690 DI 10.5194/acp-14-3657-2014 PG 34 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA AF3JO UT WOS:000334608400028 ER PT J AU Wang, YP Chen, BC Wieder, WR Leite, M Medlyn, BE Rasmussen, M Smith, MJ Agusto, FB Hoffman, F Luo, YQ AF Wang, Y. P. Chen, B. C. Wieder, W. R. Leite, M. Medlyn, B. E. Rasmussen, M. Smith, M. J. Agusto, F. B. Hoffman, F. Luo, Y. Q. TI Oscillatory behavior of two nonlinear microbial models of soil carbon decomposition SO BIOGEOSCIENCES LA English DT Article ID LAND-USE CHANGE; ORGANIC-MATTER; TERRESTRIAL ECOSYSTEMS; LITTER DECOMPOSITION; BACTERIAL-POPULATIONS; NITROGEN DYNAMICS; TALLGRASS PRAIRIE; THEORETICAL-MODEL; STORAGE CAPACITY; GLOBAL PATTERNS AB A number of nonlinear models have recently been proposed for simulating soil carbon decomposition. Their predictions of soil carbon responses to fresh litter input and warming differ significantly from conventional linear models. Using both stability analysis and numerical simulations, we showed that two of those nonlinear models (a two-pool model and a three-pool model) exhibit damped oscillatory responses to small perturbations. Stability analysis showed the frequency of oscillation is proportional to root(epsilon(-1) - 1) K-s/V-s in the two-pool model, and to root(epsilon(-1) - 1) K-l/V-l in the three-pool model, where epsilon is microbial growth efficiency, K-s and K-l are the half saturation constants of soil and litter carbon, respectively, and V-s and V-l are the maximal rates of carbon decomposition per unit of microbial biomass for soil and litter carbon, respectively. For both models, the oscillation has a period of between 5 and 15 years depending on other parameter values, and has smaller amplitude at soil temperatures between 0 and 15 degrees C. In addition, the equilibrium pool sizes of litter or soil carbon are insensitive to carbon inputs in the nonlinear model, but are proportional to carbon input in the conventional linear model. Under warming, the microbial biomass and litter carbon pools simulated by the nonlinear models can increase or decrease, depending whether epsilon varies with temperature. In contrast, the conventional linear models always simulate a decrease in both microbial and litter carbon pools with warming. Based on the evidence available, we concluded that the oscillatory behavior and insensitivity of soil carbon to carbon input are notable features in these nonlinear models that are somewhat unrealistic. We recommend that a better model for capturing the soil carbon dynamics over decadal to centennial timescales would combine the sensitivity of the conventional models to carbon influx with the flexible response to warming of the nonlinear model. C1 [Wang, Y. P.] CSIRO Marine & Atmospher Res, Aspendale, Vic 3195, Australia. [Chen, B. C.] Univ Texas Arlington, Dept Math, Arlington, TX 76019 USA. [Wieder, W. R.] Natl Ctr Atmospher Res, Boulder, CO 80307 USA. [Leite, M.] Univ Toledo, Dept Math & Stat, Toledo, OH 43606 USA. [Medlyn, B. E.] Macquarie Univ, Fac Sci, Dept Biol Sci, N Ryde, NSW 2109, Australia. [Rasmussen, M.] Univ London Imperial Coll Sci Technol & Med, Dept Math, London, England. [Smith, M. J.] Microsoft Res, Computat Sci Lab, Cambridge, England. [Agusto, F. B.] Austin Peay State Univ, Dept Math & Stat, Clarksville, TN 37044 USA. [Hoffman, F.] Oak Ridge Natl Lab, Computat Earth Sci Grp, Oak Ridge, TN 37831 USA. [Luo, Y. Q.] Univ Oklahoma, Dept Microbiol & Plant Biol, Norman, OK 73019 USA. RP Wang, YP (reprint author), CSIRO Marine & Atmospher Res, Private Bag 1, Aspendale, Vic 3195, Australia. EM yingping.wang@csiro.au RI Rasmussen, Martin/J-4479-2014; wang, yp/A-9765-2011; Hoffman, Forrest/B-8667-2012; OI Rasmussen, Martin/0000-0002-7366-4719; Hoffman, Forrest/0000-0001-5802-4134; Medlyn, Belinda/0000-0001-5728-9827; WIEDER, WILLIAM/0000-0001-7116-1985 FU National Science Foundation; US Department of Homeland Security; US Department of Agriculture through NSF [EF-0832858]; University of Tennessee, Knoxville FX This work was assisted through participation of the authors in the working group Nonautonomous Systems and Terrestrial Carbon Cycle, at the National Institute for Mathematical and Biological Synthesis, an institute sponsored by the National Science Foundation, the US Department of Homeland Security, and the US Department of Agriculture through NSF award no. EF-0832858, with additional support from The University of Tennessee, Knoxville. NR 50 TC 17 Z9 17 U1 2 U2 24 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1726-4170 EI 1726-4189 J9 BIOGEOSCIENCES JI Biogeosciences PY 2014 VL 11 IS 7 BP 1817 EP 1831 DI 10.5194/bg-11-1817-2014 PG 15 WC Ecology; Geosciences, Multidisciplinary SC Environmental Sciences & Ecology; Geology GA AF3JT UT WOS:000334609000010 ER PT J AU Abellan, P Woehl, TJ Parent, LR Browning, ND Evans, JE Arslan, I AF Abellan, P. Woehl, T. J. Parent, L. R. Browning, N. D. Evans, J. E. Arslan, I. TI Factors influencing quantitative liquid (scanning) transmission electron microscopy SO CHEMICAL COMMUNICATIONS LA English DT Article ID IN-SITU OBSERVATION; IMAGING PROTEIN; GROWTH; WATER; CELL; NANOPARTICLES; NANOMATERIALS; NUCLEATION; RESOLUTION; DYNAMICS AB One of the experimental challenges in the study of nanomaterials in liquids in the (scanning) transmission electron microscope ((S) TEM) is gaining quantitative information. A successful experiment in the fluid stage will depend upon the ability to plan for sensitive factors such as the electron dose applied, imaging mode, acceleration voltage, beam-induced solution chemistry changes, and the specifics of solution reactivity. In this paper, we make use of a visual approach to show the extent of damage of different instrumental and experimental factors in liquid samples imaged in the (S) TEM. Previous results as well as new insights are presented to create an overview of beam-sample interactions identified for changing imaging and experimental conditions. This work establishes procedures to understand the effect of the electron beam on a solution, provides information to allow for a deliberate choice of the optimal experimental conditions to enable quantification, and identifies the experimental factors that require further analysis for achieving fully quantitative results in the liquid (S) TEM. C1 [Abellan, P.; Parent, L. R.; Browning, N. D.] Pacific NW Natl Lab, Fundamental & Computat Sci Directorate, Richland, WA 99352 USA. [Woehl, T. J.] Univ Calif Davis, Dept Chem Engn & Mat Sci, Davis, CA 95616 USA. [Evans, J. E.] Pacific NW Natl Lab, Environ Mol Sci Lab, Richland, WA 99352 USA. [Arslan, I.] Pacific NW Natl Lab, Energy & Environm Directorate, Richland, WA 99352 USA. RP Abellan, P (reprint author), Pacific NW Natl Lab, Fundamental & Computat Sci Directorate, POB 999, Richland, WA 99352 USA. EM Patricia.abellanbaeza@pnnl.gov RI Abellan, Patricia/G-4255-2011; OI Abellan, Patricia/0000-0002-5797-1102; Browning, Nigel/0000-0003-0491-251X FU Chemical Imaging Initiative; U.S. Department of Energy [DE-AC05-76RL01830] FX The in situ stage development was supported by the Chemical Imaging Initiative, under the Laboratory Directed Research and Development Program at Pacific Northwest National Laboratory (PNNL). PNNL is a multiprogram national laboratory operated by Battelle for the U.S. Department of Energy under Contract DE-AC05-76RL01830. A portion of the research was performed using EMSL, a national scientific user facility sponsored by the Department of Energy's Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory. We thank J. A. Lercher for providing the zeolite samples used in this study. NR 33 TC 33 Z9 33 U1 10 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 2014 VL 50 IS 38 BP 4873 EP 4880 DI 10.1039/c3cc48479c PG 8 WC Chemistry, Multidisciplinary SC Chemistry GA AF5EN UT WOS:000334736900001 PM 24643324 ER PT J AU Hu, N Shao, RF Zhu, CH Shen, YQ Park, C Korblova, E Guerra, C Rego, JA Hexemer, A Clark, NA Walba, DM AF Hu, Nan Shao, Renfan Zhu, Chenhui Shen, Yongqiang Park, Cheol Korblova, Eva Guerra, Carlos Rego, James A. Hexemer, Alexander Clark, Noel A. Walba, David M. TI Ferroelectric and antiferroelectric odd-even behavior in a tricarbosilane-terminated liquid crystal homologous series SO CHEMICAL SCIENCE LA English DT Article ID BENT-CORE MOLECULES; POLAR ORDER; PHASES; CHIRALITY; MESOGENS AB A new class of polyphilic mesogens composed of a tolanphenyl carboxylate core, a chiral alkoxy tail, and a tricarbosilane terminated alkoxy tail was synthesized, and shown to self-organize into nanophase segregated, smectic liquid crystalline ( LC) phases. It was found that the number of carbons in the alkyl spacer between the tricarbosilane and the core controlled the observed phase with perfect fidelity: oddcarbon spacers gave antiferroelectric phases, and even-carbon spacers gave ferroelectric phases. Even more interestingly, homologues with odd carbon number show the rare and useful chiral orthoconic antiferroelectric SmCA phase, where the optic axis tilt alternates from layer to layer between + 45 degrees and -45 degrees, making the molecular directors in adjacent layers orthogonal. The even-carbon homologues exhibit the SmC phase with close to 45 degrees tilt. The findings demonstrate that the supramolecular self-organization of polyphilic mesogens may be controlled by the length of hydrocarbon spacers. C1 [Hu, Nan; Korblova, Eva; Walba, David M.] Univ Colorado, Dept Chem & Biochem, Liquid Crystal Mat Res Ctr, Boulder, CO 80309 USA. [Shao, Renfan; Zhu, Chenhui; Shen, Yongqiang; Park, Cheol; Clark, Noel A.] Univ Colorado, Dept Phys, Liquid Crystal Mat Res Ctr, Boulder, CO 80309 USA. [Guerra, Carlos; Rego, James A.] Calif State Polytech Univ Pomona, Dept Chem, Pomona, CA 91768 USA. [Zhu, Chenhui; Hexemer, Alexander] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. RP Walba, DM (reprint author), Univ Colorado, Dept Chem & Biochem, Liquid Crystal Mat Res Ctr, 125 UCB, Boulder, CO 80309 USA. EM Walba@colorado.edu RI Clark, Noel/E-9011-2010; Shen, Yongqiang/N-7902-2013; Walba, David/F-7284-2013 OI Shen, Yongqiang/0000-0001-8696-5433; FU Liquid Crystal Materials Research Center (NSF MRSEC award) [DMR-0820579]; Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231] FX We thank the Liquid Crystal Materials Research Center (NSF MRSEC award no. DMR-0820579) for financial support of this work. We also acknowledge Beamline 7.3.3 of the Advanced Light Source 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-AC02-05CH11231. We thank Dr Per Rudquist for valuable discussions. NR 38 TC 4 Z9 4 U1 6 U2 25 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 2014 VL 5 IS 5 BP 1869 EP 1874 DI 10.1039/c3sc53353k PG 6 WC Chemistry, Multidisciplinary SC Chemistry GA AF1SC UT WOS:000334492700023 ER PT J AU Foster, ME Azoulay, JD Wong, BM Allendorf, MD AF Foster, Michael E. Azoulay, Jason D. Wong, Bryan M. Allendorf, Mark D. TI Novel metal-organic framework linkers for light harvesting applications SO CHEMICAL SCIENCE LA English DT Article ID DENSITY-FUNCTIONAL THEORY; GENERALIZED-GRADIENT-APPROXIMATION; BRILLOUIN-ZONE INTEGRATIONS; INITIO MOLECULAR-DYNAMICS; TOTAL-ENERGY CALCULATIONS; AUGMENTED-WAVE METHOD; CHARGE-TRANSFER; SELECTIVE SEPARATION; CARBON-DIOXIDE; SOLAR-CELLS AB Metal-organic frameworks (MOFs) are composed of organic linkers and coordinating metals that selfassemble to form a crystalline material with tunable nanoporosity. Their synthetic modularity and inherent long-range order create opportunities for use as new functional electronic materials. Using quantum mechanical computational methodologies we propose novel conjugated organic linkers that are capable of forming the same one-dimensional infinite metal-oxide secondary building units (SBUs) as the well-known IRMOF-74. This structural arrangement allows for the formation of a continuous p-p stacking network that should enable charge transport in fashion analogous to organic semiconductors. The structural and electronic properties (fundamental and optical gaps) of the isolated proposed linkers were modeled using a non-empirically tuned long-range corrected functional that leads to significantly improved results compared with experimental benchmarks. In addition, periodic hybrid density functional calculations were employed to model the extended MOF systems. Our results demonstrate how the electronic properties of MOFs can be readily modified to have favorable orbital alignments with known electron acceptors that should facilitate charge transfer. The predicted properties are in good agreement with experiment (i.e. UV-Vis absorption spectra), demonstrating the power of this computational approach for MOF design. C1 [Foster, Michael E.; Azoulay, Jason D.] Sandia Natl Labs, Dept Chem Mat, Livermore, CA 94551 USA. [Wong, Bryan M.] Drexel Univ, Dept Chem, Dept Mat Sci & Engn, Philadelphia, PA 19104 USA. [Allendorf, Mark D.] Sandia Natl Labs, Ctr Biol & Mat Sci, Livermore, CA 94551 USA. RP Allendorf, MD (reprint author), Sandia Natl Labs, Ctr Biol & Mat Sci, Livermore, CA 94551 USA. EM mdallen@sandia.gov RI Wong, Bryan/B-1663-2009 OI Wong, Bryan/0000-0002-3477-8043 FU U.S. Department of Energy Office of Energy Efficiency and Renewable Energy SunShot Program [DE-FOA-0000387-1923]; Sandia National Laboratories' Laboratory Directed Research and Development (LDRD) Program; U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX This work was supported by the U.S. Department of Energy Office of Energy Efficiency and Renewable Energy SunShot Program under award number DE-FOA-0000387-1923 and Sandia National Laboratories' Laboratory Directed Research and Development (LDRD) 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 72 TC 42 Z9 42 U1 19 U2 170 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 2014 VL 5 IS 5 BP 2081 EP 2090 DI 10.1039/c4sc00333k PG 10 WC Chemistry, Multidisciplinary SC Chemistry GA AF1SC UT WOS:000334492700051 ER PT J AU Kennedy, S Beavers, CM Teat, SJ Dalgarno, SJ AF Kennedy, Stuart Beavers, Christine M. Teat, Simon J. Dalgarno, Scott J. TI Salt formation affects the conformational and assembly properties of p-carboxylatocalix[4]arenes SO CRYSTENGCOMM LA English DT Article ID METAL-ORGANIC FRAMEWORKS; CALIXARENE NANOTUBES; POROUS MATERIALS; CRYSTALS AB The conformational properties and self-assembly behaviour of the p-carboxylatocalix[4]arenes, when in the presence of a pyridine template, are well understood. Salt formation with these molecules, a process driven by the introduction of an amino group to the 2-position of the pyridine template, has dramatic consequences on both building block conformation and the resulting self-assembly. C1 [Kennedy, Stuart; Dalgarno, Scott J.] Heriot Watt Univ, Inst Chem Sci, Edinburgh EH14 4AS, Midlothian, Scotland. [Beavers, Christine M.; Teat, Simon J.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Kennedy, S (reprint author), Heriot Watt Univ, Inst Chem Sci, Edinburgh EH14 4AS, Midlothian, Scotland. EM S.J.Dalgarno@hw.ac.uk RI Kennedy, Stuart/D-5248-2014; Beavers, Christine/C-3539-2009; Dalgarno, Scott/A-7358-2010 OI Kennedy, Stuart/0000-0002-1769-8797; Beavers, Christine/0000-0001-8653-5513; Dalgarno, Scott/0000-0001-7831-012X FU EPSRC; Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231] FX We thank the EPSRC for financial support of this work. 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 28 TC 4 Z9 4 U1 2 U2 15 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 2014 VL 16 IS 18 BP 3712 EP 3717 DI 10.1039/c3ce42523a PG 6 WC Chemistry, Multidisciplinary; Crystallography SC Chemistry; Crystallography GA AF2XC UT WOS:000334574800010 ER PT J AU Abellan, G Carrasco, JA Coronado, E Romero, J Varela, M AF Abellan, Gonzalo Carrasco, Jose A. Coronado, Eugenio Romero, Jorge Varela, Maria TI Alkoxide-intercalated CoFe-layered double hydroxides as precursors of colloidal nanosheet suspensions: structural, magnetic and electrochemical properties SO JOURNAL OF MATERIALS CHEMISTRY C LA English DT Article ID WATER OXIDATION; ELECTRODE MATERIALS; THIN-FILMS; NI-AL; NANOPARTICLES; EXFOLIATION; GRAPHENE; OXIDES AB Alkoxide-intercalated CoFe-layered double hydroxides (CoFe-LDHs) were synthesized via the nonaqueous methanolic route. According to powder X-ray diffraction and field emission scanning electron microscopy, they exhibit a nanosized plate-like morphology with a basal space of 9.21 A. The hydrolysis of the material in water leads to colloidal suspensions of nanosheets with lateral dimensions of about 20 nm and thicknesses of ca. 4 nm as demonstrated by atomic force microscopy and dynamic light scattering. Atomic resolution scanning transmission electron microscopy combined with electron energy-loss spectroscopy confirm the high crystalline quality of the crystals and the proper Co/Fe stoichiometry. The magnetic properties of the CoFe-LDH have been investigated by means of DC and AC magnetic susceptibility measurements and isothermal magnetisation, showing a low-temperature magnetic ordering below ca. 7 K with a size-dependent spin-glass like behaviour, and displaying hysteresis cycles at 2 K with a coercive field of 402 G. Moreover, the sample has been tested as an electrode material for supercapacitors in a three-electrode system by means of cyclic voltammetry and galvanostatic charge-discharge experiments, showing high capacitances and stability. Finally, we have explored the electrocatalytic behaviour towards water oxidation, demonstrating its efficient and persistent performance at basic pHs, highlighting their tremendous potential in energy storage devices. C1 [Abellan, Gonzalo; Carrasco, Jose A.; Coronado, Eugenio; Romero, Jorge] Univ Valencia, Inst Ciencia Mol ICMol, Valencia 46980, Paterna, Spain. [Varela, Maria] Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN 37830 USA. [Varela, Maria] Univ Complutense Madrid, Dpt Fis Aplicada 3, E-28040 Madrid, Spain. [Varela, Maria] Univ Complutense Madrid, Inst Pluridisciplinar, E-28040 Madrid, Spain. RP Coronado, E (reprint author), Univ Valencia, Inst Ciencia Mol ICMol, Catedrat Jose Beltran 2, Valencia 46980, Paterna, Spain. EM eugenio.coronado@uv.es RI Varela, Maria/H-2648-2012; Coronado, Eugenio/E-8960-2014; Varela, Maria/E-2472-2014; icmol, icmol/I-5784-2015; Abellan, Gonzalo/B-3451-2013 OI Varela, Maria/0000-0002-6582-7004; Abellan, Gonzalo/0000-0003-1564-6210 FU EU (Projects HINTS and ERC Advanced Grant SPINMOL); Spanish MINECO (Projects Consolider-Ingenio in Molecular Nanoscience) [MAT2011-22785, CTQ-2011-26507]; Generalitat Valenciana (Prometeo Program, ISIC-Nano and Geronimo Forteza Program); VLC/CAMPUS; INNCIDE program through Vicerectorat d'lnvestigacio i Politica Cienti. ca of the University of Valencia; Office of Basic Energy Sciences, Division of Materials Sciences and Engineering, U.S. Department of Energy; ERC Starting Investigator Award [239739] FX Financial support from the EU (Projects HINTS and ERC Advanced Grant SPINMOL), the Spanish MINECO (Projects Consolider-Ingenio in Molecular Nanoscience, MAT2011-22785, and CTQ-2011-26507), and the Generalitat Valenciana (Prometeo Program, ISIC-Nano and Geronimo Forteza Program) is gratefully acknowledged. Support from VLC/CAMPUS and INNCIDE program through Vicerectorat d'lnvestigacio i Politica Cienti. ca of the University of Valencia is also acknowledged. We also acknowledge E. Tormos and A. Lopez for their help with the experimental work, and J. M. Martinez and G. Agusti for magnetic measurements. This research was sponsored by the Office of Basic Energy Sciences, Division of Materials Sciences and Engineering, U.S. Department of Energy (M. V.). Electron microscopy was performed at the Centro Nacional de Microscopia Electronica (UCM) sponsored by the ERC Starting Investigator Award STEMOX# 239739. NR 50 TC 38 Z9 38 U1 20 U2 132 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 2014 VL 2 IS 19 BP 3723 EP 3731 DI 10.1039/c3tc32578d PG 9 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA AF8XZ UT WOS:000335000300007 ER PT J AU Hu, MZ Shi, DL Blom, DA AF Hu, Michael Z. Shi, Donglu Blom, Douglas A. TI Nanostructured Mesoporous Silica Wires with Intrawire Lamellae via Evaporation-Induced Self-Assembly in Space-Confined Channels SO JOURNAL OF NANOMATERIALS LA English DT Article ID NANOWIRE ARRAYS; NANOFIBERS; TEMPLATES; MEMBRANES; AAO AB Evaporation-induced self-assembly (EISA) of silica sol-gel ethanol-water solution mixtures with block-copolymer were studied inside uniform micro/nano-channels. Nanostructured mesoporous silica wires, with various intrawire self-assembly structures including lamellae, were prepared via EISA process but in space-confined channels with the diameter ranging from 50 nm to 200 nm. Membranes made of anodized aluminum oxide (AAO) and track-etched polycarbonate (EPC) were utilized as the arrays of space-confined channels (i. e., 50, 100, and 200 nm EPC and 200 nm AAO) for infiltration and drying of mixture solutions; these substrate membranes were submerged in mixture solutions consisting of a silica precursor, a structure-directing agent, ethanol, and water. After the substrate channels were filled with the solution under vacuum impregnation, the membrane was removed from the solution and dried in air. The silica precursor used was tetraethyl othosilicate (TEOS), and the structure-directing agent employed was triblock copolymer Pluronic-123 (P123). It was found that the formation of the mesoporous nanostructures in silica wires within uniform channels were significantly affected by the synthesis conditions including (1) preassemble TEOS aging time, (2) the evaporation rate during the vacuum impregnation, and (3) the air-dry temperature. The obtained intrawire structures, including 2D hexagonal rods and lamellae, were studied by scanning transmission electron microscopy (STEM). A steric hindrance effect seems to explain well the observed polymer-silica mesophase formation tailored by TEOS aging time. The evaporation effect, air-drying effect, and AAO versus EPC substrate effect on the mesoporous structure of the formed silica wires were also presented and discussed. C1 [Hu, Michael Z.] Oak Ridge Natl Lab, Energy & Transportat Sci Div, Oak Ridge, TN 37831 USA. [Shi, Donglu] Univ Cincinnati, Dept Mech & Mat Engn, Mat Sci & Engn Program, Cincinnati, OH 45221 USA. [Blom, Douglas A.] Univ S Carolina, Columbia, SC 29208 USA. RP Hu, MZ (reprint author), Oak Ridge Natl Lab, Energy & Transportat Sci Div, Oak Ridge, TN 37831 USA. EM hum1@ornl.gov OI Hu, Michael/0000-0001-8461-9684 FU ORNL LDRD-SEED; DOE/EERE/BETO; Division of Materials Science [KC 02 03 01 0]; Office of Science; U.S. Department of Energy; Assistant Secretary for Energy Efficiency and Renewable Energy; Office of Transportation Technologies; High Temperature Materials Laboratory; U.S. Department of Energy [DE-AC-05-00OR22725] FX The authors acknowledge Peng Lai for her involvement of conducting some hands-on experiments and discussions during her postmaster work at the Oak Ridge National Laboratory (ORNL). This work on nanostructure control inside the nanochannel array membranes is partially supported by the ORNL LDRD-SEED Money Program Fund, partially by the DOE/EERE/BETO Program Fund, and partially by the Division of Materials Science (KC 02 03 01 0), Office of Science, the U.S. Department of Energy. The STEM characterization was sponsored in part by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Transportation Technologies, as part of the High Temperature Materials Laboratory, managed by UT-Battelle, LLC, for the U.S. Department of Energy under contract DE-AC-05-00OR22725. NR 16 TC 1 Z9 1 U1 4 U2 43 PU HINDAWI PUBLISHING CORPORATION PI NEW YORK PA 410 PARK AVENUE, 15TH FLOOR, #287 PMB, NEW YORK, NY 10022 USA SN 1687-4110 EI 1687-4129 J9 J NANOMATER JI J. Nanomater. PY 2014 AR 932160 DI 10.1155/2014/932160 PG 8 WC Nanoscience & Nanotechnology; Materials Science, Multidisciplinary SC Science & Technology - Other Topics; Materials Science GA AF5MP UT WOS:000334757900001 ER PT J AU Kashyap, S Woehl, T Valverde-Tercedor, C Sanchez-Quesada, M Lopez, CJ Prozorov, T AF Kashyap, Sanjay Woehl, Taylor Valverde-Tercedor, Carmen Sanchez-Quesada, Miguel Jimenez Lopez, Concepcion Prozorov, Tanya TI Visualization of Iron-Binding Micelles in Acidic Recombinant Biomineralization Protein, MamC SO JOURNAL OF NANOMATERIALS LA English DT Article ID TRANSMISSION ELECTRON-MICROSCOPY; IN-SITU TEM; SURFACE PATTERNING TOOLS; MAGNETOTACTIC BACTERIA; MAGNETIC NANOPARTICLES; MAGNETOSOME MEMBRANE; PROTEOMIC ANALYSIS; MMS6; NANOCRYSTALS; FERRITIN AB Biological macromolecules are utilized in low-temperature synthetic methods to exert precise control over nanoparticle nucleation and placement. They enable low-temperature formation of a variety of functional nanostructured materials with properties often not achieved via conventional synthetic techniques. Here we report on the in situ visualization of a novel acidic bacterial recombinant protein, MamC, commonly present in the magnetosome membrane of several magnetotactic bacteria, including Magnetococcus marinus, strain MC-1. Our findings provide an insight into the self-assembly of MamC and point to formation of the extended protein surface, which is assumed to play an important role in the formation of biotemplated inorganic nanoparticles. The self-organization of MamC is compared to the behavior of another acidic recombinant iron-binding protein, Mms6. C1 [Kashyap, Sanjay; Woehl, Taylor; Prozorov, Tanya] US DOE, Ames Lab, Ames, IA 50011 USA. [Valverde-Tercedor, Carmen; Sanchez-Quesada, Miguel; Jimenez Lopez, Concepcion] Univ Granada, Dept Microbiol, E-18071 Granada, Spain. RP Prozorov, T (reprint author), US DOE, Ames Lab, Ames, IA 50011 USA. EM tprozoro@ameslab.gov FU U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division; U.S. Department of Energy by Iowa State University [DE-AC02-07CH11358]; Spanish Government [CGL2010-18274]; program Salvador de Madariaga FX This work was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. The research was performed at the Ames Laboratory, which is operated for the U.S. Department of Energy by Iowa State University under Contract no. DE-AC02-07CH11358. MamC cloning and purification were done at the University of Granada, Spain. Concepcion Jimenez Lopez acknowledges the support from the Spanish Government through Grant CGL2010-18274 and the program Salvador de Madariaga. The authors thank the Laboratory of Professor Marit Nilsen-Hamilton for providing the recombinant biomineralization protein, Mms6. NR 64 TC 8 Z9 9 U1 1 U2 17 PU HINDAWI PUBLISHING CORPORATION PI NEW YORK PA 410 PARK AVENUE, 15TH FLOOR, #287 PMB, NEW YORK, NY 10022 USA SN 1687-4110 EI 1687-4129 J9 J NANOMATER JI J. Nanomater. PY 2014 AR 320124 DI 10.1155/2014/320124 PG 7 WC Nanoscience & Nanotechnology; Materials Science, Multidisciplinary SC Science & Technology - Other Topics; Materials Science GA AF5KT UT WOS:000334753100001 ER PT J AU Trebbin, M Kruger, K DePonte, D Roth, SV Chapman, HN Forster, S AF Trebbin, Martin Krueger, Kilian DePonte, Daniel Roth, Stephan V. Chapman, Henry N. Foerster, Stephan TI Microfluidic liquid jet system with compatibility for atmospheric and high-vacuum conditions SO LAB ON A CHIP LA English DT Article ID X-RAY-SCATTERING; FREE-ELECTRON LASERS; LARGE-SCALE INTEGRATION; PROTEIN NANOCRYSTALLOGRAPHY; SOFT LITHOGRAPHY; ROOM-TEMPERATURE; PHOTOSYSTEM-II; DIFFRACTION; GENERATION; DEVICES AB We present microfluidic chip based devices that produce liquid jets with micrometer diameters while operating at very low flow rates. The chip production is based on established soft-lithographical techniques employing a three-layer design protocol. This allows the exact, controlled and reproducible design of critical parts such as nozzles and the production of nozzle arrays. The microfluidic chips reproducibly generate liquid jets exiting at perfect right angles with diameters between 20 mu m and 2 mu m, and under special circumstances, even down to 0.9 mu m. Jet diameter, jet length, and the domain of the jetting/dripping instability can be predicted and controlled based on the theory for liquid jets in the plate-orifice configuration described by Ganan-Calvo et al. Additionally, conditions under which the device produces highly reproducible monodisperse droplets at exact and predictable rates can be achieved. The devices operate under atmospheric and under vacuum conditions making them highly relevant for a wide range of applications, for example, for free-electron lasers. Further, the straightforward integration of additional features such as a jet-in-jet is demonstrated. This device design has the potential to integrate more features based on established microfluidic components and may become a standard device for small liquid jet production. C1 [Trebbin, Martin; Krueger, Kilian; Foerster, Stephan] Univ Bayreuth, D-95447 Bayreuth, Germany. [DePonte, Daniel] SLAC, Stanford, CA USA. [DePonte, Daniel; Chapman, Henry N.] DESY, CFEL, Hamburg, Germany. [Roth, Stephan V.] DESY, HASYLAB, Hamburg, Germany. RP Forster, S (reprint author), Univ Bayreuth, Univ Str 30, D-95447 Bayreuth, Germany. EM stephan.foerster@uni-bayreuth.de RI Forster, Stephan/B-2180-2015; Trebbin, Martin/A-5281-2015; Chapman, Henry/G-2153-2010 OI Trebbin, Martin/0000-0001-8278-5865; Chapman, Henry/0000-0002-4655-1743 FU European Research Council [291211]; Federal Ministry of Research (BMBF) [05K13WC5] FX We thank the European Research Council for financial support within the ERC Advanced Grant project STREAM (#291211) and the Federal Ministry of Research (BMBF, #05K13WC5). Very helpful discussions with Joachim Schulz (XFEL, Hamburg, Germany), Kenneth Beyerlein and Dominik Oberthur (both CFEL/DESY, Hamburg, Germany) are gratefully acknowledged. NR 116 TC 15 Z9 15 U1 9 U2 41 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 2014 VL 14 IS 10 BP 1733 EP 1745 DI 10.1039/c3lc51363g PG 13 WC Biochemical Research Methods; Chemistry, Multidisciplinary; Nanoscience & Nanotechnology SC Biochemistry & Molecular Biology; Chemistry; Science & Technology - Other Topics GA AF7AT UT WOS:000334866500011 PM 24671443 ER PT J AU Harris, WM Brinkman, KS Lin, Y Su, D Cocco, AP Nakajo, A DeGostin, MB Chen-Wiegart, YCK Wang, J Chen, FL Chu, YS Chiu, WKS AF Harris, William M. Brinkman, Kyle S. Lin, Ye Su, Dong Cocco, Alex P. Nakajo, Arata DeGostin, Matthew B. Chen-Wiegart, Yu-chen Karen Wang, Jun Chen, Fanglin Chu, Yong S. Chiu, Wilson K. S. TI Characterization of 3D interconnected microstructural network in mixed ionic and electronic conducting ceramic composites SO NANOSCALE LA English DT Article ID X-RAY MICROSCOPY; OXYGEN PERMEABILITY; OXIDE; TRANSMISSION; MEMBRANE; FILMS; CERIA; TECHNOLOGY; SEPARATION; NANOSCALE AB The microstructure and connectivity of the ionic and electronic conductive phases in composite ceramic membranes are directly related to device performance. Transmission electron microscopy (TEM) including chemical mapping combined with X-ray nano-tomography (XNT) have been used to characterize the composition and 3-D microstructure of a MIEC composite model system consisting of a Ce0.8Gd0.2O2 (GDC) oxygen ion conductive phase and a CoFe2O4 (CFO) electronic conductive phase. The microstructural data is discussed, including the composition and distribution of an emergent phase which takes the form of isolated and distinct regions. Performance implications are considered with regards to the design of new material systems which evolve under non-equilibrium operating conditions. C1 [Harris, William M.; Cocco, Alex P.; Nakajo, Arata; DeGostin, Matthew B.; Chiu, Wilson K. S.] Univ Connecticut, Dept Mech Engn, Storrs, CT 06269 USA. [Brinkman, Kyle S.] Clemson Univ, Dept Mat Sci & Engn, Clemson, SC 29634 USA. [Su, Dong] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. [Chen-Wiegart, Yu-chen Karen; Wang, Jun] Brookhaven Natl Lab, Photon Sci Directorate, Upton, NY 11973 USA. [Lin, Ye] Univ S Carolina, Dept Mech Engn, Columbia, SC 29208 USA. [Chu, Yong S.] Brookhaven Natl Lab, Natl Synchrotron Light Source 2, Upton, NY 11973 USA. EM wchiu@engr.uconn.edu RI Chen, Fanglin/K-1039-2012; Su, Dong/A-8233-2013; OI Chen, Fanglin/0000-0001-9942-8872; Su, Dong/0000-0002-1921-6683; Lin, Ye/0000-0003-4289-894X; Brinkman, Kyle/0000-0002-2219-1253 FU Energy Frontier Research Center on Science Based Nano-Structure Design and Synthesis of Heterogeneous Functional Materials for Energy Systems (HeteroFoaM Center) - U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001061]; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-98CH10886]; U.S. Department of Energy, Office of Basic Energy Sciences [DE-AC02-98CH10886] FX The authors acknowledge financial support from an Energy Frontier Research Center on Science Based Nano-Structure Design and Synthesis of Heterogeneous Functional Materials for Energy Systems (HeteroFoaM Center) funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences (Award no. DE-SC0001061). 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. Electron microscopy research has been partially 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. NR 32 TC 6 Z9 6 U1 5 U2 35 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 2014 VL 6 IS 9 BP 4480 EP 4485 DI 10.1039/c3nr06684c PG 6 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA AF6WO UT WOS:000334855500005 PM 24615571 ER PT J AU Bai, P Kao, J Chen, JH Mickelson, W Zettl, A Xu, T AF Bai, Peter Kao, Joseph Chen, Jian-Hao Mickelson, William Zettl, Alex Xu, Ting TI Nanostructures on graphene using supramolecule and supramolecular nanocomposites SO NANOSCALE LA English DT Article ID BLOCK-COPOLYMER LITHOGRAPHY; MAGNETIC-FIELD ALIGNMENT; THIN-FILMS; ACTIVE CATALYSTS; METAL NANOPARTICLES; OXIDE NANOSHEETS; SUZUKI REACTION; GRAPHITE OXIDE; CARBON SUPPORT; LARGE-AREA AB Nanopatterning and functionalizing of graphene is often required to tune or enhance its unique physical properties. However, complex processes are needed to overcome the chemical incompatibilities between the patterning template, the functional small molecules or nanoparticles, and the underlying graphene. We present a block copolymer (BCP)-based supramolecular thin film as a versatile platform for the generation of periodic patterns of small molecules and ordered assemblies of nanoparticles on top of a graphene substrate without chemical modification of any components. The present approach opens opportunities to readily pattern and functionalize graphene, and to investigate the structure-property correlations of graphene/nanoparticle and graphene/small molecule composite materials. C1 [Bai, Peter; Kao, Joseph; Xu, Ting] Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA. [Chen, Jian-Hao; Mickelson, William; Zettl, Alex] Univ Calif Berkeley, Dept Phys, Berkeley, CA 94720 USA. [Zettl, Alex; Xu, Ting] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. [Xu, Ting] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. RP Xu, T (reprint author), Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA. EM tingxu@berkeley.edu RI Bai, Peter/J-9084-2014; Zettl, Alex/O-4925-2016; Chen, Jian-Hao/C-6983-2009 OI Zettl, Alex/0000-0001-6330-136X; Chen, Jian-Hao/0000-0002-9485-1759 FU COINS NSF [EEC-0832819]; Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231] FX This work was supported by the COINS NSF award EEC-0832819. 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 DE-AC02-05CH11231. NR 49 TC 2 Z9 2 U1 7 U2 52 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 2014 VL 6 IS 9 BP 4503 EP 4507 DI 10.1039/c4nr00420e PG 5 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA AF6WO UT WOS:000334855500009 PM 24647721 ER PT J AU Ermanoski, I Miller, JE Allendorf, MD AF Ermanoski, I. Miller, J. E. Allendorf, M. D. TI Efficiency maximization in solar-thermochemical fuel production: challenging the concept of isothermal water splitting SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID THERMODYNAMIC PROPERTIES; NONSTOICHIOMETRIC CERIA; OXIDE; ENERGY; SYSTEM; CO2; TEMPERATURE; OXALATE; CEO2-X; CYCLE AB Widespread adoption of solar-thermochemical fuel production depends on its economic viability, largely driven by the efficiency of use of the available solar resource. Herein, we analyze the efficiency of two-step cycles for thermochemical hydrogen production, with emphasis on efficiency. Owing to water thermodynamics, isothermal H-2 production is shown to be impractical and inefficient, irrespective of reactor design or reactive oxide properties, but an optimal temperature difference between cycle steps, for which efficiency is the highest, can be determined for a wide range of other operating parameters. A combination of well-targeted pressure and temperature swing, rather than either individually, emerges as the most efficient mode of operation of a two-step thermochemical cycle for solar fuel production. C1 [Ermanoski, I.; Miller, J. E.] Sandia Natl Labs, Albuquerque, NM 87185 USA. [Allendorf, M. D.] Sandia Natl Labs, Livermore, CA 94551 USA. RP Ermanoski, I (reprint author), Sandia Natl Labs, POB 5800, Albuquerque, NM 87185 USA. EM iermano@sandia.gov FU U.S. Department of Energy Fuel Cell Technologies Program via the Solar Thermochemical Hydrogen (STCH) directive; Advanced Materials for Next Generation High Efficiency Thermochemistry LDRD project; United States Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX The authors would like to thank Dr T. M. Besmann of Oak Ridge National Laboratory, who provided the CeO2-x model, based on data from Zinkevich et al. 20 Many useful discussions with Anthony McDaniel of Sandia National Laboratories and Nathan Siegel of Bucknell University are gratefully acknowledged as well. This work was supported by the U.S. Department of Energy Fuel Cell Technologies Program via the Solar Thermochemical Hydrogen (STCH) directive, and the Advanced Materials for Next Generation High Efficiency Thermochemistry LDRD project. 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 33 TC 36 Z9 36 U1 5 U2 56 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 2014 VL 16 IS 18 BP 8418 EP 8427 DI 10.1039/c4cp00978a PG 10 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AF3HP UT WOS:000334602900026 PM 24668070 ER PT J AU Nicolai, A Sumpter, BG Meuniera, V AF Nicolai, Adrien Sumpter, Bobby G. Meunier, Vincent TI Tunable water desalination across graphene oxide framework membranes SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID REVERSE-OSMOSIS DESALINATION; HIGH PERMEABILITY; CARBON NANOTUBE; DYNAMICS; SIMULATIONS; FUTURE; ENERGY; FILMS; ART AB The performance of graphene oxide framework (GOF) membranes for water desalination is assessed using classical molecular dynamics (MD) simulations. The coupling between water permeability and salt rejection of GOF membranes is studied as a function of linker concentration n, thickness h and applied pressure Delta P. The simulations reveal that water permeability in GOF-(n,h) membranes can be tuned from similar to 5 (n = 32 and h = 6.5 nm) to 400 L cm(-2) day(-1) MPa-1 (n = 64 and h = 2.5 nm) and follows a C(n)h(-alpha n) an law. For a given pore size (n = 16 or 32), water permeability of GOF membranes increases when the pore spacing decreases, whereas for a given pore spacing (n = 32 or 64), water permeability increases by up to two orders of magnitude when the pore size increases. Furthermore, for linker concentrations n <= 32, the high water permeability corresponds to a 100% salt rejection, elevating this type of GOF membrane as an ideal candidate for water desalination. Compared to experimental performance of reverse osmosis membranes, our calculations suggest that under the same conditions of applied pressure and characteristics of membranes (Delta P similar to 10 MPa and h similar to 100 nm), one can expect a perfect salt rejection coupled to a water permeability two orders of magnitude higher than existing technologies, i.e., from a few cL cm(-2) day(-1) MPa-1 to a few L cm(-2) day(-1) MPa-1. C1 [Nicolai, Adrien; Meunier, Vincent] Rensselaer Polytech Inst, Dept Phys Appl Phys & Astron, Troy, NY 12180 USA. [Sumpter, Bobby G.] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. [Sumpter, Bobby G.] Oak Ridge Natl Lab, Div Math & Comp Sci, Oak Ridge, TN 37831 USA. RP Nicolai, A (reprint author), Rensselaer Polytech Inst, Dept Phys Appl Phys & Astron, Troy, NY 12180 USA. EM adrien.nicolai@gmail.com RI Meunier, Vincent/F-9391-2010; Sumpter, Bobby/C-9459-2013 OI Meunier, Vincent/0000-0002-7013-179X; Sumpter, Bobby/0000-0001-6341-0355 FU Office of Naval Research; Center for Nanophase Materials Sciences; Oak Ridge National Laboratory by the Scientific User Facilities Division, Basic Energy Sciences, U.S. Department of Energy FX Work at Rensselaer Polytechnic Institute (RPI) was supported by the Office of Naval Research. Calculations were done on the Center for Computational Innovations (CCI) cluster, at RPI. BGS was supported by the Center for Nanophase Materials Sciences, which is sponsored at Oak Ridge National Laboratory by the Scientific User Facilities Division, Basic Energy Sciences, U.S. Department of Energy. NR 40 TC 36 Z9 37 U1 20 U2 181 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 2014 VL 16 IS 18 BP 8646 EP 8654 DI 10.1039/c4cp01051e PG 9 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AF3HP UT WOS:000334602900053 PM 24675972 ER PT J AU Chen, CW Huang, ZY Lin, YM Huang, WC Chen, YH Strzalka, J Chang, AY Schaller, RD Lee, CK Pao, CW Lin, HW AF Chen, Chang-Wen Huang, Zheng-Yu Lin, Yi-Min Huang, Wei-Ching Chen, Yi-Hong Strzalka, Joseph Chang, Angela Y. Schaller, Richard D. Lee, Cheng-Kuang Pao, Chun-Wei Lin, Hao-Wu TI Morphology, molecular stacking, dynamics and device performance correlations of vacuum-deposited small-molecule organic solar cells SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID POLYMER PHOTOVOLTAIC CELLS; OPEN-CIRCUIT VOLTAGE; IMPEDANCE SPECTROSCOPY; CHARGE-TRANSPORT; BIMOLECULAR RECOMBINATION; CONJUGATED POLYMERS; BLOCKING LAYER; EFFICIENCY; HETEROJUNCTIONS; MOBILITY AB The "all carbon'' organic solar cells (OSCs) based on the homocyclic molecule tetraphenyldibenzoperiflanthene (DBP) as a donor and C-60 as an acceptor were comprehensively characterized. The optimized planar-mixed heterojunction device with a DBP: C-60 mixture ratio of DBP:C-60 (1:2) exhibited a power conversion efficiency of 4.47%. To understand why DBP possesses such advantageous characteristics, the correlations of the morphology, molecular stacking, carrier dynamics and performance of DBP: fullerene-based devices have been systematically studied. First, the face- on stacked DBP molecules could enhance both the absorption of light and the charge carrier mobility. Second, DBP : C-60 (1:2) thin films with optimized domain sizes and partially interconnected acceptor grains led to the most balanced carrier mobility and the lowest bimolecular recombination in devices. Finally, the DBP molecules were found to stack closely using grazing incidence wide-angle X-ray scattering measurements, with a pi-pi stacking spacing of 4.58 A, indicating an effective molecular orbital overlap in DBP. The study not only reveals the promising characteristics of DBP as a donor in OSCs but the clear correlations of the thin-film nano-morphology, molecular stacking, carrier mobility and charge recombination found here could also provide insights into the characterization methodology and optimization of the small molecule OSCs. C1 [Chen, Chang-Wen; Huang, Zheng-Yu; Lin, Yi-Min; Huang, Wei-Ching; Chen, Yi-Hong; Lin, Hao-Wu] Natl Tsing Hua Univ, Dept Mat Sci & Engn, Hsinchu 30013, Taiwan. [Strzalka, Joseph] Argonne Natl Lab, Xray Sci Div, Argonne, IL 60439 USA. [Chang, Angela Y.; Schaller, Richard D.] Northwestern Univ, Dept Chem, Evanston, IL 60208 USA. [Schaller, Richard D.] Argonne Natl Lab, Ctr Nanoscale Mat, Argonne, IL 60439 USA. [Lee, Cheng-Kuang; Pao, Chun-Wei] Acad Sinica, Res Ctr Appl Sci, Taipei 115, Taiwan. RP Lin, HW (reprint author), Natl Tsing Hua Univ, Dept Mat Sci & Engn, 101,Sect 2,Kuang Fu Rd, Hsinchu 30013, Taiwan. EM hwlin@mx.nthu.edu.tw RI Lee, Cheng-Kuang/G-6390-2010; Pao, Chun-Wei/D-3307-2009; Lin, Hao-Wu/I-5871-2013 OI Pao, Chun-Wei/0000-0003-0821-7856; Lin, Hao-Wu/0000-0003-4216-7995 FU National Science Council of Taiwan [NSC 101-2112-M-007-017-MY3, NSC 102-2221-E- 007-125-MY3, NSC-102-2633-M-007-002]; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357] FX The work was financially supported by the National Science Council of Taiwan (NSC 101-2112-M-007-017-MY3, NSC 102-2221-E- 007-125-MY3, NSC-102-2633-M-007-002). 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. NR 85 TC 5 Z9 5 U1 3 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 2014 VL 16 IS 19 BP 8852 EP 8864 DI 10.1039/c3cp55385j PG 13 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AF9DN UT WOS:000335015700018 PM 24683598 ER PT J AU Koo, J Park, M Hwang, S Huang, B Jang, B Kwon, Y Lee, H AF Koo, Jahyun Park, Minwoo Hwang, Seunghyun Huang, Bing Jang, Byungryul Kwon, Yongkyung Lee, Hoonkyung TI Widely tunable band gaps of graphdiyne: an ab initio study SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID HYDROGEN STORAGE; DECORATED GRAPHYNE; CARBON; LITHIUM; CAPACITY; GRAPHENE; FAMILY; FORMS AB Functionalization of graphdiyne, a two-dimensional atomic layer of sp-sp(2) hybrid carbon networks, was investigated through first-principles calculations. Hydrogen or halogen atoms preferentially adsorb on sp-bonded carbon atoms rather than on sp(2)-bonded carbon atoms, forming sp(2)- or sp(3)-hybridization. The energy band gap of graphdiyne is increased from similar to 0.5 eV to similar to 5.2 eV through the hydrogenation or halogenation. Unlike graphene, segregation of adsorbing atoms is energetically unfavourable. Our results show that hydrogenation or halogenation can be utilized for modifying the electronic properties of graphdiyne for applications to nano-electronics and -photonics. C1 [Koo, Jahyun; Park, Minwoo; Hwang, Seunghyun; Jang, Byungryul; Kwon, Yongkyung; Lee, Hoonkyung] Konkuk Univ, Sch Phys, Seoul 143701, South Korea. [Huang, Bing] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37830 USA. RP Lee, H (reprint author), Konkuk Univ, Sch Phys, Seoul 143701, South Korea. EM hkiee3@konkuk.ac.kr RI Huang, Bing/D-8941-2011 OI Huang, Bing/0000-0001-6735-4637 FU National Research Foundation of Korea - Ministry of Education, Science and Technology [KRF-2012R1A1A1013124] FX This work was supported by the Basic Science Research Program (Grant No. KRF-2012R1A1A1013124) through the National Research Foundation of Korea, funded by the Ministry of Education, Science and Technology. NR 45 TC 10 Z9 10 U1 9 U2 91 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 2014 VL 16 IS 19 BP 8935 EP 8939 DI 10.1039/c4cp00800f PG 5 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AF9DN UT WOS:000335015700028 PM 24691588 ER PT J AU Yun, WS Lee, JD AF Yun, Won Seok Lee, J. D. TI Unexpected strong magnetism of Cu doped single-layer MoS2 and its origin SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID AUGMENTED-WAVE METHOD; MOLYBDENUM-DISULFIDE; MONOLAYER MOS2; FUNCTIONALIZATION; 1ST-PRINCIPLES; MECHANISM; GRAPHENE AB The magnetism of the 3d transition-metal (TM) doped single-layer (1L) MoS2, where the Mo atom is partially replaced by the 3d TM atom, is investigated using the first-principles density functional calculations. In a series of 3d TM doped 1L-MoS2's, the induced spin polarizations are negligible for Sc, Ti, and Cr dopings, while the induced spin polarizations are confirmed for V, Mn, Fe, Co, Ni, Cu, and Zn dopings and the systems become magnetic. Especially, the Cu doped system shows unexpectedly strong magnetism although Cu is nonmagnetic in its bulk state. The driving force is found to be a strong hybridization between Cu 3d states and 3p states of neighboring S, which results in an extreme unbalanced spin-population in the spin-split impurity bands near the Fermi level. Finally, we also discuss further issues of the Cu induced magnetism of 1L-MoS2 such as investigation of additional charge states, the Cu doping at the S site instead of the Mo site, and the Cu adatom on the layer (i.e., 1L-MoS2). C1 [Yun, Won Seok; Lee, J. D.] DGIST, Dept Emerging Mat Sci, Taegu 711873, South Korea. [Yun, Won Seok] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Ctr Xray Opt, Berkeley, CA 94720 USA. RP Lee, JD (reprint author), DGIST, Dept Emerging Mat Sci, Taegu 711873, South Korea. EM jdlee@dgist.ac.kr RI Yun, Won Seok/B-4962-2014 OI Yun, Won Seok/0000-0002-6710-9807 FU National Research Foundation of Korea - Ministry of Education, Science and Technology [2012K1A4A3053565, 2013R1A1A2007388] FX This work was supported by the Leading Foreign Research Institute Recruitment Program (Grant No. 2012K1A4A3053565) and the Basic Science Research Program (Grant No. 2013R1A1A2007388) through the National Research Foundation of Korea (NRF) funded by the Ministry of Education, Science and Technology (MEST). NR 46 TC 33 Z9 33 U1 16 U2 168 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 2014 VL 16 IS 19 BP 8990 EP 8996 DI 10.1039/c4cp00247d PG 7 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AF9DN UT WOS:000335015700034 PM 24695769 ER PT J AU Wojnarowska, Z Wang, YY Paluch, KJ Sokolov, AP Paluch, M AF Wojnarowska, Zaneta Wang, Yangyang Paluch, Krzysztof J. Sokolov, Alexei P. Paluch, Marian TI Observation of highly decoupled conductivity in protic ionic conductors SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID PHOSPHORIC-ACID; FUEL-CELLS; LIQUIDS; ELECTROLYTES; RELAXATION; GROTTHUSS; LIDOCAINE; MECHANISM; MIXTURES; FUTURE AB Ionic liquids (ILs) are key materials for the development of a wide range of emerging technologies. Protic ionic liquids, an important class of ILs, have long been envisioned as promising anhydrous electrolytes for fuel cells. It is well known that in comparison to all other cations, protons exhibit abnormally high conductivity in water. Such superprotonic dynamics was expected in protic ionic conductors as well. However, many years of extensive studies led to the disappointing conclusion that this is not the case and most protic ionic liquids display subionic behavior. Therefore, the relatively low conductivity seems to be the main obstacle for the application of protic ionic liquids in fuel cells. Using dielectric spectroscopy, herein we report the observation of highly decoupled conductivity in a newly synthesized protic ionic conductor. We show that its proton transport is strongly decoupled from the structural relaxation, in terms of both temperature dependence and characteristic rates. This finding offers a fresh look on the charge transport mechanism in PILs and also provides new ideas for design of anhydrous materials with exceptionally high proton conductivity. C1 [Wojnarowska, Zaneta; Paluch, Marian] Univ Silesia, Inst Phys, PL-40007 Katowice, Poland. [Wojnarowska, Zaneta; Paluch, Marian] SMCEBI, PL-41500 Chorzow, Poland. [Wang, Yangyang; Sokolov, Alexei P.] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. [Paluch, Krzysztof J.] Univ Dublin Trinity Coll, Sch Pharm & Pharmaceut Sci, Dublin 2, Ireland. [Sokolov, Alexei P.] Univ Tennessee, Dept Chem, Knoxville, TN 37996 USA. RP Wojnarowska, Z (reprint author), Univ Silesia, Inst Phys, Uniwersytecka 4, PL-40007 Katowice, Poland. EM zaneta.wojnarowska@us.edu.pl RI Wang, Yangyang/A-5925-2010; OI Wang, Yangyang/0000-0001-7042-9804; Paluch, Krzysztof Jan/0000-0001-7293-7394 FU National Science Centre within the framework of the Opus [DEC 2011/03/B/ST3/02072]; FNP START; LDRD Program of ORNL; NSF [CHE-1213444] FX Z.W. and M.P. are deeply grateful for the financial support by the National Science Centre within the framework of the Opus project (Grant No. DEC 2011/ 03/ B/ ST3/ 02072). Z.W. acknowledges financial assistance from FNP START. Y.W. acknowledges the LDRD Program of ORNL, managed by UT-Battelle, LLC, for the U.S. DOE. A.P.S. thanks the support from the NSF under grant CHE-1213444. NR 31 TC 13 Z9 13 U1 7 U2 40 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 2014 VL 16 IS 19 BP 9123 EP 9127 DI 10.1039/c4cp00899e PG 5 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AF9DN UT WOS:000335015700049 PM 24699717 ER PT J AU Kirshenbaum, KC Bock, DC Zhong, Z Marschilok, AC Takeuchi, KJ Takeuchi, ES AF Kirshenbaum, Kevin C. Bock, David C. Zhong, Zhong Marschilok, Amy C. Takeuchi, Kenneth J. Takeuchi, Esther S. TI In situ profiling of lithium/Ag2VP2O8 primary batteries using energy dispersive X-ray diffraction SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID SILVER VANADIUM-OXIDE; ELECTROCHEMICAL IMPEDANCE SPECTROSCOPY; LITHIUM BATTERIES; MECHANISTIC INSIGHTS; LIFEPO4; CATHODE; ELECTRODES; RECRYSTALLIZATION; ELECTROLYTES; PERFORMANCES AB In situ, in operando characterization of electrochemical cells can provide insight into the complex discharge chemistries of batteries which may not be available with destructive methods. In this study, in situ energy-dispersive X-ray spectroscopy (EDXRD) measurements are conducted for the first time on active lithium/silver vanadium diphosphate, Li/Ag2VP2O8, electrochemical cells at several depths of discharge allowing depth profiling analysis of the reduction process. This technique enables non-destructive, in operando imaging of the reduction process within a battery electrode over a millimeter scale interrogation area with micron scale resolution. The discharge of Ag2VP2O8 progresses via a reduction displacement reaction forming conductive silver metal as a discharge product, a high Z material which can be readily detected by diffraction-based methods. The high energy X-ray capabilities of NSLS beamline X17B1 allowed spatially resolved detection of the reduction products forming conductive pathways providing insight into the discharge mechanism of Ag(2)VP2(O8). C1 [Kirshenbaum, Kevin C.; Takeuchi, Esther S.] Brookhaven Natl Lab, Upton, NY 11973 USA. [Bock, David C.; Marschilok, Amy C.; Takeuchi, Kenneth J.; Takeuchi, Esther S.] SUNY Stony Brook, Dept Chem, Stony Brook, NY 11794 USA. [Zhong, Zhong] Brookhaven Natl Lab, Upton, NY 11973 USA. [Marschilok, Amy C.; Takeuchi, Kenneth J.; Takeuchi, Esther S.] SUNY Stony Brook, Dept Mat Sci & Engn, Stony Brook, NY 11794 USA. RP Marschilok, AC (reprint author), SUNY Stony Brook, Dept Chem, Stony Brook, NY 11794 USA. EM amy.marschilok@stonybrook.edu; kenneth.takeuchi.1@stonybrook.edu; esther.takeuchi@stonybrook.edu FU Department of Energy, Office of Basic Energy Sciences [DE-SC0008512]; U.S. Department of Energy [DE-AC02-98CH10886]; Brookhaven National Laboratory; Gertrude and Maurice Goldhaber Distinguished Fellowship Program FX E. Takeuchi, K. Takeuchi, A. Marschilok and D. Bock acknowledge funding from the Department of Energy, Office of Basic Energy Sciences, under grant DE-SC0008512. Utilization of the National Synchrotron Light Source (NSLS) beamline X17B1 was supported by U.S. Department of Energy Contract DE-AC02-98CH10886. K. Kirshenbaum acknowledges Postdoctoral support from Brookhaven National Laboratory and the Gertrude and Maurice Goldhaber Distinguished Fellowship Program. The authors also acknowledge Mark C. Croft for helpful discussions. NR 49 TC 14 Z9 14 U1 4 U2 47 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 2014 VL 16 IS 19 BP 9138 EP 9147 DI 10.1039/c4cp01220h PG 10 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AF9DN UT WOS:000335015700051 PM 24705594 ER PT J AU Choi, SW Farinholt, KM Taylor, SG Light-Marquez, A Park, G AF Choi, Seong-Won Farinholt, Kevin M. Taylor, Stuart G. Light-Marquez, Abraham Park, Gyuhae TI Damage Identification of Wind Turbine Blades Using Piezoelectric Transducers SO SHOCK AND VIBRATION LA English DT Article ID ACTIVE-SENSORS; VALIDATION AB This paper presents the experimental results of active-sensing structural health monitoring (SHM) techniques, which utilize piezoelectric transducers as sensors and actuators, for determining the structural integrity of wind turbine blades. Specifically, Lamb wave propagations and frequency response functions at high frequency ranges are used to estimate the condition of wind turbine blades. For experiments, a 1 m section of a CX-100 blade is used. The goal of this study is to assess and compare the performance of each method in identifying incipient damage with a consideration given to field deployability. Overall, these methods yielded a sufficient damage detection capability to warrant further investigation. This paper also summarizes the SHM results of a full-scale fatigue test of a 9 m CX-100 blade using piezoelectric active sensors. This paper outlines considerations needed to design such SHM systems, experimental procedures and results, and additional issues that can be used as guidelines for future investigations. C1 [Choi, Seong-Won; Park, Gyuhae] Chonnam Natl Univ, Sch Mech Syst Engn, Kwangju 500757, South Korea. [Farinholt, Kevin M.; Taylor, Stuart G.; Light-Marquez, Abraham; Park, Gyuhae] Los Alamos Natl Lab, Engn Inst, Los Alamos, NM 87545 USA. RP Park, G (reprint author), Chonnam Natl Univ, Sch Mech Syst Engn, Kwangju 500757, South Korea. EM gpark@chonnam.ac.kr FU Department of Energy through the Laboratory Directed Research and Development Program at Los Alamos National Laboratory; Leading Foreign Research Institute Recruitment Program through the National Research Foundation of Korea - Ministry of Education, Science and Technology [2011-0030065]; "Leaders Industry-University Cooperation" Project - Ministry of Education, Science and Technology (MEST), Republic of Korea FX This work was funded by the Department of Energy through the Laboratory Directed Research and Development Program at Los Alamos National Laboratory. This research was also partially supported by the Leading Foreign Research Institute Recruitment Program through the National Research Foundation of Korea funded by the Ministry of Education, Science and Technology (2011-0030065). G. Park acknowledges the partial support of the "Leaders Industry-University Cooperation" Project, supported by the Ministry of Education, Science and Technology (MEST), Republic of Korea. The authors also would like to acknowledge Mark Rumsey and Jon White from Sandia National Laboratory for their support and guidance on this study. NR 18 TC 1 Z9 1 U1 0 U2 14 PU HINDAWI PUBLISHING CORPORATION PI NEW YORK PA 410 PARK AVENUE, 15TH FLOOR, #287 PMB, NEW YORK, NY 10022 USA SN 1070-9622 EI 1875-9203 J9 SHOCK VIB JI Shock Vib. PY 2014 AR 430854 DI 10.1155/2014/430854 PG 9 WC Acoustics; Engineering, Mechanical; Mechanics SC Acoustics; Engineering; Mechanics GA AF6OL UT WOS:000334834300001 ER PT J AU Reichhardt, C Reichhardt, CJO AF Reichhardt, C. Reichhardt, C. J. Olson TI Aspects of jamming in two-dimensional athermal frictionless systems SO SOFT MATTER LA English DT Review ID PHASE-TRANSITIONS; GRANULAR MATERIAL; DYNAMICS; CHAINS; CRYSTALS; PARTICLE; LATTICE; ARRAYS; FOAMS; SHEAR AB In this work we provide an overview of jamming transitions in two dimensional systems focusing on the limit of frictionless particle interactions in the absence of thermal fluctuations. We first discuss jamming in systems with short range repulsive interactions, where the onset of jamming occurs at a critical packing density and where certain quantities show a divergence indicative of critical behavior. We describe how aspects of the dynamics change as the jamming density is approached and how these dynamics can be explored using externally driven probes. Different particle shapes can produce jamming densities much lower than those observed for disk-shaped particles, and we show how jamming exhibits fragility for some shapes while for other shapes this is absent. Next we describe the effects of long range interactions and jamming behavior in systems such as charged colloids, vortices in type-II superconductors, and dislocations. We consider the effect of adding obstacles to frictionless jamming systems and discuss connections between this type of jamming and systems that exhibit depinning transitions. Finally, we discuss open questions such as whether the jamming transition in all these different systems can be described by the same or a small subset of universal behaviors, as well as future directions for studies of jamming transitions in two dimensional systems, such as jamming in self-driven or active matter systems. C1 [Reichhardt, C.; Reichhardt, C. J. Olson] Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. RP Reichhardt, C (reprint author), Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. EM reichhardt@lanl.gov FU NNSA of the U.S. DoE at LANL [DE-AC52-06NA25396] FX This work was carried out under the auspices of the NNSA of the U.S. DoE at LANL under Contract no. DE-AC52-06NA25396. NR 94 TC 13 Z9 14 U1 6 U2 50 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 2014 VL 10 IS 17 BP 2932 EP 2944 DI 10.1039/c3sm53154f PG 13 WC Chemistry, Physical; Materials Science, Multidisciplinary; Physics, Multidisciplinary; Polymer Science SC Chemistry; Materials Science; Physics; Polymer Science GA AF1SO UT WOS:000334494000002 PM 24695520 ER PT J AU Washington, AL Li, X Schofield, AB Hong, K Fitzsimmons, MR Dalgliesh, R Pynn, R AF Washington, A. L. Li, X. Schofield, A. B. Hong, K. Fitzsimmons, M. R. Dalgliesh, R. Pynn, R. TI Inter-particle correlations in a hard-sphere colloidal suspension with polymer additives investigated by Spin Echo Small Angle Neutron Scattering (SESANS) SO SOFT MATTER LA English DT Article ID EQUATION; POLYSTYRENE; LATTICES AB Using a neutron scattering technique that measures a statistically-averaged density correlation function in real space rather than the conventional reciprocal-space structure factor, we have measured correlations between poly(methyl-methacrylate) (PMMA) colloidal particles of several sizes suspended in decalin. The new method, called Spin Echo Small Angle Neutron Scattering (SESANS) provides accurate information about particle composition, including the degree of solvent penetration into the polymer brush grafted on to the PMMA spheres to prevent aggregation. It confirms for particles, between 85 nm and 150 nm in radius that inter-particle correlations closely follow the Percus-Yevick hard- sphere model when the colloidal volume-fraction is between 30% and 50% provided the volume-fraction is used as a fitted parameter. No particle aggregation occurs in these systems. When small amounts of polystyrene are added as a depletant to a concentrated suspension of PMMA particles, short-range clustering of the particles occurs and there is an increase in the frequency of near-neighbor contacts. Within a small range of depletant concentration, near-neighbor correlations saturate and large aggregates with power law density correlations are formed. SESANS clearly separates the short-and long-range correlations and shows that, in this case, the power-law correlations are visible for inter-particle distances larger than roughly two particle diameters. In some cases, aggregate sizes are within our measurement window, which can extend out to 16 microns in favorable cases. We discuss the advantages of SESANS for measurements of the structure of concentrated colloidal systems and conclude that the method offers several important advantages. C1 [Washington, A. L.; Li, X.; Pynn, R.] Indiana Univ, Ctr Explorat Energy & Matter, Bloomington, IN 47405 USA. [Li, X.; Pynn, R.] Oak Ridge Natl Lab, Neutron Scattering Sci Directorate, Oak Ridge, TN USA. [Schofield, A. B.] Univ Edinburgh, Sch Phys & Astron, Edinburgh, Midlothian, Scotland. [Hong, K.] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN USA. [Fitzsimmons, M. R.] Los Alamos Natl Lab, Manual Lujan Neutron Scattering Ctr, Los Alamos, NM USA. [Dalgliesh, R.] Rutherford Appleton Lab, Chilton OX11 0QX, Oxon, England. RP Washington, AL (reprint author), Indiana Univ, Ctr Explorat Energy & Matter, Bloomington, IN 47405 USA. EM rpynn@indiana.edu RI Hong, Kunlun/E-9787-2015; OI Hong, Kunlun/0000-0002-2852-5111; Washington, Adam/0000-0002-3243-1556 FU U.S. Department of Energy through its Office of Basic Energy Sciences, Division of Material Science and Engineering [DE-FG02-09ER46279]; UK Engineering and Physical Sciences Research Council [EP/J007404/1]; Oak Ridge National Laboratory by Office of Basic Energy Sciences, U. S. Department of Energy; Los Alamos National Security LLC under DOE [DE-AC52-06NA25396] FX We thank Chris Duif of the Interfaculty Reactor Institute in Del. for carrying out several SESANS measurements on our samples and Wim Bouwman of the same institute for helpful comments on the manuscript. This work was supported by the U.S. Department of Energy through its Office of Basic Energy Sciences, Division of Material Science and Engineering (grant no. DE-FG02-09ER46279). ABS is partially funded by the UK Engineering and Physical Sciences Research Council grant EP/J007404/1. 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. We thank the ISIS facility in the UK and the Los Alamos Neutron Science Center (LANSCE) for the award of beam time. Los Alamos National Laboratory is operated by Los Alamos National Security LLC under DOE Contract DE-AC52-06NA25396. NR 24 TC 9 Z9 9 U1 0 U2 14 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 2014 VL 10 IS 17 BP 3016 EP 3026 DI 10.1039/c3sm53027b PG 11 WC Chemistry, Physical; Materials Science, Multidisciplinary; Physics, Multidisciplinary; Polymer Science SC Chemistry; Materials Science; Physics; Polymer Science GA AF1SO UT WOS:000334494000012 PM 24695952 ER PT S AU Favela, JF Shapira, D Chavez, E Ortiz, ME Andrade, E de Lucio, OG Huerta, A AF Favela, J. F. Shapira, D. Chavez, E. Ortiz, M. E. Andrade, E. de Lucio, O. G. Huerta, A. BE BarronPalos, L MartinezQuiroz, E MoralesAgiss, I TI Nuclear physics experiments with a windowless supersonic gas jet target SO XXXVI SYMPOSIUM ON NUCLEAR PHYSICS (COCOYOC 2013) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 36th Symposium on Nuclear Physics CY JAN 07-10, 2013 CL Cocoyoc, MEXICO SP Mexican Phys Soc, Div Nucl Phys AB A new windowless gas target has been developed in Mexico. It is a supersonic gas jet flow produced inside a vacuum chamber which can be coupled to a regular beam line in an accelerator laboratory as a differential pumping system brings the pressure of the gas target system down to a microTorr, or better, at the connecting stage. In this work, we present the system as it was designed and constructed as well as the first results using air, Nitrogen and Argon. C1 [Favela, J. F.; Chavez, E.; Ortiz, M. E.; Andrade, E.; de Lucio, O. G.; Huerta, A.] Univ Nacl Autonoma Mexico, Inst Fis, Mexico City 04510, DF, Mexico. [Shapira, D.] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. RP Favela, JF (reprint author), Univ Nacl Autonoma Mexico, Inst Fis, Mexico City 04510, DF, Mexico. EM ffavela@gmail.com FU CONACYT [82692]; PAPIIT [IN-118310]; IFUNAM FX This work was supported by CONACYT 82692, PAPIIT IN-118310, the shop at IFUNAM and Dr. Roberto Gleason's support for the improvement of our facility. NR 11 TC 0 Z9 0 U1 0 U2 1 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2014 VL 492 AR UNSP 012010 DI 10.1088/1742-6596/492/1/012010 PG 7 WC Physics, Nuclear SC Physics GA BA3ZP UT WOS:000335222900010 ER PT J AU Wong, J Piceno, YM DeSantis, TZ Pahl, M Andersen, GL Vaziri, ND AF Wong, Jakk Piceno, Yvette M. DeSantis, Todd Z. Pahl, Madeleine Andersen, Gary L. Vaziri, Nosratola D. TI Expansion of Urease- and Uricase-Containing, Indole- and p-Cresol-Forming and Contraction of Short-Chain Fatty Acid-Producing Intestinal Microbiota in ESRD SO AMERICAN JOURNAL OF NEPHROLOGY LA English DT Article DE Chronic kidney disease; Hemodialysis; Inflammation; Uric acid; Uremic toxins; Microbiome; Malnutrition; Gastrointestinal tract ID CHRONIC KIDNEY-DISEASE; EPITHELIAL TIGHT JUNCTION; CHRONIC-RENAL-FAILURE; CLOSTRIDIUM-DIFFICILE; GASTROINTESTINAL-TRACT; HEMODIALYSIS-PATIENTS; OXIDATIVE STRESS; UREMIC TOXICITY; EXHALED BREATH; INFLAMMATION AB Background: Intestinal microbiome constitutes a symbiotic ecosystem that is essential for health, and changes in its composition/function cause various illnesses. Biochemical milieu shapes the structure and function of the microbiome. Recently, we found marked differences in the abundance of numerous bacterial taxa between ESRD and healthy individuals. Influx of urea and uric acid and dietary restriction of fruits and vegetables to prevent hyperkalemia alter ESRD patients' intestinal milieu. We hypothesized that relative abundances of bacteria possessing urease, uricase, and p-cresol- and indoleproducing enzymes is increased, while abundance of bacteria containing enzymes converting dietary fiber to shortchain fatty acids (SCFA) is reduced in ESRD. Methods: Reference sets of bacteria containing genes of interest were compiled to family, and sets of intestinal bacterial families showing differential abundances between 12 healthy and 24 ESRD individuals enrolled in our original study were compiled. Overlap between sets was assessed using hypergeometric distribution tests. Results: Among 19 microbial families that were dominant in ESRD patients, 12 possessed urease, 5 possessed uricase, and 4 possessed indole and p-cresol-forming enzymes. Among 4 microbial families that were diminished in ESRD patients, 2 possessed butyrateforming enzymes. Probabilities of these overlapping distributions were <0.05. Conclusions: ESRD patients exhibited significant expansion of bacterial families possessing urease, uricase, and indole and p-cresol forming enzymes, and contraction of families possessing butyrate-forming enzymes. Given the deleterious effects of indoxyl sulfate, p-cresol sulfate, and urea-derived ammonia, and beneficial actions of SCFA, these changes in intestinal microbial metabolism contribute to uremic toxicity and inflammation. (C) 2014 S. Karger AG, Basel C1 [Wong, Jakk; Piceno, Yvette M.; Andersen, Gary L.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Ctr Environm Biotechnol, Berkeley, CA 94720 USA. [DeSantis, Todd Z.] Second Genome, San Bruno, CA USA. [Pahl, Madeleine; Vaziri, Nosratola D.] Univ Calif Irvine, Div Nephrol & Hypertens, Irvine, CA 92868 USA. RP Vaziri, ND (reprint author), Univ Calif Irvine, Sch Med, Div Nephrol & Hypertens, Irvine, CA 92868 USA. EM ndvaziri@uci.edu RI Andersen, Gary/G-2792-2015; Piceno, Yvette/I-6738-2016 OI Andersen, Gary/0000-0002-1618-9827; Piceno, Yvette/0000-0002-7915-4699 FU National Center for Research Resources; National Center for Advancing Translational Sciences, National Institutes of Health [UL1 TR000153] FX The authors have no conflict of interest to declare. This project was, in part, supported by the National Center for Research Resources and the National Center for Advancing Translational Sciences, National Institutes of Health, through Grant UL1 TR000153. NR 45 TC 50 Z9 51 U1 1 U2 27 PU KARGER PI BASEL PA ALLSCHWILERSTRASSE 10, CH-4009 BASEL, SWITZERLAND SN 0250-8095 EI 1421-9670 J9 AM J NEPHROL JI Am. J. Nephrol. PY 2014 VL 39 IS 3 BP 230 EP 237 DI 10.1159/000360010 PG 8 WC Urology & Nephrology SC Urology & Nephrology GA AE7DK UT WOS:000334156700006 PM 24643131 ER PT J AU Phillips, MC Taubman, MS Bernacki, BE Cannon, BD Stahl, RD Schiffern, JT Myers, TL AF Phillips, Mark C. Taubman, Matthew S. Bernacki, Bruce E. Cannon, Bret D. Stahl, Robert D. Schiffern, John T. Myers, Tanya L. TI Real-time trace gas sensing of fluorocarbons using a swept-wavelength external cavity quantum cascade laser SO ANALYST LA English DT Article ID LEAST-SQUARES METHODS; PHOTOACOUSTIC-SPECTROSCOPY; FREQUENCY COMB; SINGLE-MODE; MU-M; CALIBRATION; SENSOR AB We present results demonstrating real-time sensing of four different fluorocarbons at low part-per billion (ppb) concentrations using an external cavity quantum cascade laser (ECQCL) designed for infrared vibrational spectroscopy of molecules with broad absorption features. The ECQCL was repeatedly swept at 20 Hz over its full tuning range of 1145-1265 cm(-1) providing a scan rate of 3535 cm(-1) s(-1), and a detailed characterization of the ECQCL scan stability and repeatability is presented. The ECQCL was combined with a 100 meter path length multi-pass cell for direct absorption spectroscopy. A portable sensor system is described, which was deployed on a mobile automotive platform to provide spatially-resolved detection of fluorocarbons in outdoor experiments. Noise-equivalent detection limits of 8001000 parts-per-trillion (ppt) are demonstrated for 1 s integration times. C1 [Phillips, Mark C.; Taubman, Matthew S.; Bernacki, Bruce E.; Cannon, Bret D.; Stahl, Robert D.; Schiffern, John T.; Myers, Tanya L.] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Phillips, MC (reprint author), Pacific NW Natl Lab, Richland, WA 99352 USA. EM mark.phillips@pnnl.gov FU DOE/NNSA Office of Nonproliferation and Verification Research and Development [NA-22]; Air Force Academy; U.S. Department of Energy (DOE) [DE-AC05-76RL01830] FX We thank Bob Sams, Tom Blake, and Tim Johnson for measurement of the PFT quantitative absorption spectra for the NWIR spectral library. This work was supported by the DOE/NNSA Office of Nonproliferation and Verification Research and Development (NA-22) and the Air Force Academy. The Pacific Northwest National Laboratory is operated for the U.S. Department of Energy (DOE) by the Battelle Memorial Institute under Contract no. DE-AC05-76RL01830. NR 44 TC 20 Z9 20 U1 2 U2 29 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 0003-2654 EI 1364-5528 J9 ANALYST JI Analyst PY 2014 VL 139 IS 9 BP 2047 EP 2056 DI 10.1039/c3an01642k PG 10 WC Chemistry, Analytical SC Chemistry GA AE7KJ UT WOS:000334176400003 PM 24384671 ER PT J AU Hiranuma, N Hoffmann, N Kiselev, A Dreyer, A Zhang, K Kulkarni, G Koop, T Mohler, O AF Hiranuma, N. Hoffmann, N. Kiselev, A. Dreyer, A. Zhang, K. Kulkarni, G. Koop, T. Moehler, O. TI Influence of surface morphology on the immersion mode ice nucleation efficiency of hematite particles SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID MINERAL DUST PARTICLES; AEROSOL CHAMBER AIDA; WATER-ADSORPTION; MICROPHYSICS; ALPHA-FE2O3; CRYSTALS; SAMPLES AB In this paper, the effect of the morphological modification of aerosol particles with respect to heterogeneous ice nucleation is comprehensively investigated for laboratorygenerated hematite particles as a model substrate for atmospheric dust particles. The surface-area-scaled ice nucleation efficiencies of monodisperse cubic hematite particles and milled hematite particles were measured with a series of expansion cooling experiments using the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) cloud simulation chamber. Complementary offline characterization of physico-chemical properties of both hematite subsets were also carried out with scanning electron microscopy (SEM), energy dispersive X-ray (EDX) spectroscopy, dynamic light scattering (DLS), and an electro-kinetic particle charge detector to further constrain droplet-freezing measurements of hematite particles. Additionally, an empirical parameterization derived from our laboratory measurements was implemented in the single-column version of the Community Atmospheric Model version 5 (CAM5) to investigate the model sensitivity in simulated ice crystal number concentration on different ice nucleation efficiencies. From an experimental perspective, our results show that the immersion mode ice nucleation efficiency of milled hematite particles is almost an order of magnitude higher at -35.2 degrees C < T < -33.5 degrees C than that of the cubic hematite particles, indicating a substantial effect of morphological irregularities on immersion mode freezing. Our modeling results similarly show that the increased droplet- freezing rates of milled hematite particles lead to about one order magnitude higher ice crystal number in the upper troposphere than cubic hematite particles. Overall, our results suggest that the surface irregularities and associated active sites lead to greater ice activation through droplet freezing. C1 [Hiranuma, N.; Hoffmann, N.; Kiselev, A.; Moehler, O.] Karlsruhe Inst Technol, Inst Meteorol & Climate Res Atmospher Aerosol Res, D-76021 Karlsruhe, Germany. [Dreyer, A.; Koop, T.] Univ Bielefeld, Fac Chem, Bielefeld, Germany. [Zhang, K.; Kulkarni, G.] Pacific NW Natl Lab, Atmospher Sci & Global Change Div, Richland, WA 99352 USA. RP Hiranuma, N (reprint author), Karlsruhe Inst Technol, Inst Meteorol & Climate Res Atmospher Aerosol Res, D-76021 Karlsruhe, Germany. EM seong.moon@kit.edu RI Koop, Thomas/B-7861-2008; Hiranuma, Naruki/D-3780-2014; Kiselev, Alexei/A-3036-2013; Mohler, Ottmar/J-9426-2012; Zhang, Kai/F-8415-2010 OI Koop, Thomas/0000-0002-7571-3684; Hiranuma, Naruki/0000-0001-7790-4807; Kiselev, Alexei/0000-0003-0136-2428; Zhang, Kai/0000-0003-0457-6368 FU German Research Society (DfG) [MO668/4-1, KO2944/2-1, FOR 1525 INUIT]; Department of Energy Atmospheric System Research Program; DOE by Battelle Memorial Institute [DE-AC05-76RLO 1830]; Deutsche Forschungsgemeinschaft; Open Access Publishing Fund of the Karlsruhe Institute of Technology FX The authors gratefully acknowledge financial support provided by the German Research Society (DfG) under contracts MO668/4-1 and KO2944/2-1 within FOR 1525 INUIT. G. Kulkarni and K. Zhang acknowledge support from the Department of Energy Atmospheric System Research Program and thank J. Fast for providing an opportunity to integrate measurements into the model. K. Zhang thanks X. Liu for his help on the model setup and S. Xie for providing the atmospheric forcing data used in this study. We thank the AIDA technicians, R. Buschbacher, T. Chudy, E. Kranz, G. Scheurig, and S. Vogt, for their continuous and dedicated support for the operation of AIDA. Technical support from M. Schnaiter for the SIMONE measurements and data processing is appreciated. The expertise of T. Kisely for the BET measurements is gratefully acknowledged. We thank P. Weidler and S. Jaeger for the preparation of the hematite particles. We also thank P. Alpert and D. Knopf for useful discussions. The Pacific Northwest National Laboratory is operated for DOE by Battelle Memorial Institute under contract DE-AC05-76RLO 1830.; We acknowledge support by Deutsche Forschungsgemeinschaft and the Open Access Publishing Fund of the Karlsruhe Institute of Technology. NR 36 TC 21 Z9 21 U1 2 U2 37 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 2014 VL 14 IS 5 BP 2315 EP 2324 DI 10.5194/acp-14-2315-2014 PG 10 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA AE6LK UT WOS:000334104200007 ER PT J AU Jiao, C Flanner, MG Balkanski, Y Bauer, SE Bellouin, N Berntsen, TK Bian, H Carslaw, KS Chin, M De Luca, N Diehl, T Ghan, SJ Iversen, T Kirkevag, A Koch, D Liu, X Mann, GW Penner, JE Pitari, G Schulz, M Seland, O Skeie, RB Steenrod, SD Stier, P Takemura, T Tsigaridis, K van Noije, T Yun, Y Zhang, K AF Jiao, C. Flanner, M. G. Balkanski, Y. Bauer, S. E. Bellouin, N. Berntsen, T. K. Bian, H. Carslaw, K. S. Chin, M. De Luca, N. Diehl, T. Ghan, S. J. Iversen, T. Kirkevag, A. Koch, D. Liu, X. Mann, G. W. Penner, J. E. Pitari, G. Schulz, M. Seland, O. Skeie, R. B. Steenrod, S. D. Stier, P. Takemura, T. Tsigaridis, K. van Noije, T. Yun, Y. Zhang, K. TI An AeroCom assessment of black carbon in Arctic snow and sea ice SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID AEROSOL-CLIMATE INTERACTIONS; CLOUD CONDENSATION NUCLEI; GLOBAL-MODELS; LIGHT-ABSORPTION; FUTURE CLIMATE; ECHAM-HAM; EMISSIONS; TRANSPORT; SENSITIVITY; PREINDUSTRIAL AB Though many global aerosols models prognose surface deposition, only a few models have been used to directly simulate the radiative effect from black carbon (BC) deposition to snow and sea ice. Here, we apply aerosol deposition fields from 25 models contributing to two phases of the Aerosol Comparisons between Observations and Models (AeroCom) project to simulate and evaluate within-snow BC concentrations and radiative effect in the Arctic. We accomplish this by driving the offline land and sea ice components of the Community Earth System Model with different deposition fields and meteorological conditions from 2004 to 2009, during which an extensive field campaign of BC measurements in Arctic snow occurred. We find that models generally underestimate BC concentrations in snow in northern Russia and Norway, while overestimating BC amounts elsewhere in the Arctic. Although simulated BC distributions in snow are poorly correlated with measurements, mean values are reasonable. The multi-model mean (range) bias in BC concentrations, sampled over the same grid cells, snow depths, and months of measurements, are -4.4 (-13.2 to + 10.7) ng g(-1) for an earlier phase of AeroCom models (phase I), and + 4.1 (-13.0 to + 21.4) ng g(-1) for a more recent phase of AeroCom models (phase II), compared to the observational mean of 19.2 ng g(-1). Factors determining model BC concentrations in Arctic snow include Arctic BC emissions, transport of extra-Arctic aerosols, precipitation, deposition efficiency of aerosols within the Arctic, and meltwater removal of particles in snow. Sensitivity studies show that the model-measurement evaluation is only weakly affected by meltwater scavenging efficiency because most measurements were conducted in non-melting snow. The Arctic (60-90 degrees N) atmospheric residence time for BC in phase II models ranges from 3.7 to 23.2 days, implying large inter-model variation in local BC deposition efficiency. Combined with the fact that most Arctic BC deposition originates from extra-Arctic emissions, these results suggest that aerosol removal processes are a leading source of variation in model performance. The multi-model mean (full range) of Arctic radiative effect from BC in snow is 0.15 (0.07-0.25) W m(-2) and 0.18 (0.06-0.28) W m(-2) in phase I and phase II models, respectively. After correcting for model biases relative to observed BC concentrations in different regions of the Arctic, we obtain a multi-model mean Arctic radiative effect of 0.17W m(-2) for the combined AeroCom ensembles. Finally, there is a high correlation between modeled BC concentrations sampled over the observational sites and the Arctic as a whole, indicating that the field campaign provided a reasonable sample of the Arctic. C1 [Jiao, C.; Flanner, M. G.; Penner, J. E.] Univ Michigan, Dept Atmospher Ocean & Space Sci, Ann Arbor, MI 48109 USA. [Balkanski, Y.] CEA CNRS UVSQ, Lab Sci Climat & Environm, Gif Sur Yvette, France. [Bauer, S. E.; Tsigaridis, K.] Columbia Univ, Ctr Climate Syst Res, New York, NY USA. [Bauer, S. E.; Tsigaridis, K.] NASA, Goddard Inst Space Studies, New York, NY 10025 USA. [Bellouin, N.] Met Off Hadley Ctr, Exeter, Devon, England. [Berntsen, T. K.] Univ Oslo, Dept Geosci, Oslo, Norway. [Bian, H.] Univ Maryland Baltimore Cty, Baltimore, MD 21228 USA. [Carslaw, K. S.; Mann, G. W.] Univ Leeds, Sch Earth & Environm, Inst Climate & Atmospher Sci, Leeds, W Yorkshire, England. [Chin, M.; Diehl, T.] NASA, Goddard Space Flight Ctr, Greenbelt, MD 20771 USA. [De Luca, N.; Pitari, G.] Univ Aquila, Dipartimento Sci Fis & Chim, I-67100 Laquila, Italy. [Ghan, S. J.; Liu, X.; Zhang, K.] Pacific NW Natl Lab, Richland, WA 99352 USA. [Iversen, T.; Kirkevag, A.; Schulz, M.; Seland, O.] Norwegian Meteorol Inst, Oslo, Norway. [Liu, X.] Univ Wyoming, Dept Atmospher Sci, Laramie, WY 82071 USA. [Skeie, R. B.] Ctr Int Climate & Environm Res Oslo CICERO, Oslo, Norway. [Steenrod, S. D.] Univ Space Res Assoc, Columbia, MD USA. [Stier, P.] Univ Oxford, Dept Phys, Oxford, England. [Takemura, T.] Kyushu Univ, Appl Mech Res Inst, Fukuoka 8168580, Japan. [van Noije, T.] Royal Netherlands Meteorol Inst, NL-3730 AE De Bilt, Netherlands. [Yun, Y.] NOAA, Geophys Fluid Dynam Lab, Princeton, NJ USA. [Zhang, K.] Max Planck Inst Meteorol, D-20146 Hamburg, Germany. RP Jiao, C (reprint author), Univ Michigan, Dept Atmospher Ocean & Space Sci, Ann Arbor, MI 48109 USA. EM chaoyij@umich.edu RI Ghan, Steven/H-4301-2011; Stier, Philip/B-2258-2008; Pitari, Giovanni/O-7458-2016; Chin, Mian/J-8354-2012; Carslaw, Ken/C-8514-2009; Bauer, Susanne/P-3082-2014; Penner, Joyce/J-1719-2012; Kyushu, RIAM/F-4018-2015; Jiao, Chaoyi/F-9065-2015; Zhang, Kai/F-8415-2010; Skeie, Ragnhild/K-1173-2015; Schulz, Michael/A-6930-2011; U-ID, Kyushu/C-5291-2016; Liu, Xiaohong/E-9304-2011; Flanner, Mark/C-6139-2011; Balkanski, Yves/A-6616-2011; Takemura, Toshihiko/C-2822-2009 OI Ghan, Steven/0000-0001-8355-8699; Stier, Philip/0000-0002-1191-0128; Pitari, Giovanni/0000-0001-7051-9578; Carslaw, Ken/0000-0002-6800-154X; Zhang, Kai/0000-0003-0457-6368; Skeie, Ragnhild/0000-0003-1246-4446; Schulz, Michael/0000-0003-4493-4158; Liu, Xiaohong/0000-0002-3994-5955; Flanner, Mark/0000-0003-4012-174X; Balkanski, Yves/0000-0001-8241-2858; Takemura, Toshihiko/0000-0002-2859-6067 FU NSF [ATM-0852775, ARC-1023387]; Joint DECC/Defra Met Office Hadley Centre Climate Programme [GA01101]; US Department of Energy, Office of Science, Scientific Discoveries through Advanced Computing program; DOE by Battelle Memorial Institute [DE-AC06-76RLO 1830]; Research Council of Norway through the RegClim project; Research Council of Norway through NorClim project; Research Council of Norway through EarthClim project [207711/E10]; Research Council of Norway through NOTUR/NorStore project; Norwegian Space Centre through PM-VRAE; EU project PEGASOS; EU project ACCESS; Norwegian Research Council through the project SLAC (Short Lived Atmospheric Components); EU project ECLIPSE; UK Natural Environment Research Council project AEROS [NE/G006148/1]; Max Planck Society FX This research was partially supported by NSF ATM-0852775 and ARC-1023387. N. Bellouin was supported by the Joint DECC/Defra Met Office Hadley Centre Climate Programme (GA01101). S. Ghan and X. Liu were supported by the US Department of Energy, Office of Science, Scientific Discoveries through Advanced Computing program. The Pacific Northwest National Laboratory (PNNL) is operated for the DOE by Battelle Memorial Institute under contract DE-AC06-76RLO 1830. T. Iversen, A. Kirkevag and O. Seland have been funded by the Research Council of Norway through the RegClim, NorClim, EarthClim (207711/E10) and NOTUR/NorStore projects, by the Norwegian Space Centre through PM-VRAE, and by the EU projects PEGASOS and ACCESS. R. B. Skeie has been funded by the Norwegian Research Council through the project SLAC (Short Lived Atmospheric Components) and the EU project ECLIPSE. P. Stier acknowledges support from the UK Natural Environment Research Council project AEROS [NE/G006148/1]. K. Zhang was supported by funding from the Max Planck Society. NR 91 TC 22 Z9 23 U1 4 U2 42 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 2014 VL 14 IS 5 BP 2399 EP 2417 DI 10.5194/acp-14-2399-2014 PG 19 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA AE6LK UT WOS:000334104200013 ER PT J AU Kangasluoma, J Kuang, C Wimmer, D Rissanen, MP Lehtipalo, K Ehn, M Worsnop, DR Wang, J Kulmala, M Petaja, T AF Kangasluoma, J. Kuang, C. Wimmer, D. Rissanen, M. P. Lehtipalo, K. Ehn, M. Worsnop, D. R. Wang, J. Kulmala, M. Petaja, T. TI Sub-3 nm particle size and composition dependent response of a nano-CPC battery SO ATMOSPHERIC MEASUREMENT TECHNIQUES LA English DT Article ID DIFFERENTIAL MOBILITY ANALYZERS; ATMOSPHERIC AEROSOL NUCLEATION; ION SPECTROMETER NAIS; BOREAL FOREST; SULFURIC-ACID; NEUTRAL CLUSTER; CHEMICAL-COMPOSITION; MASS-SPECTROMETER; HIGH-RESOLUTION; NANOPARTICLES AB In this study we built a nano-CPC (condensation particle counter) battery, consisting of four ultrafine CPCs optimized for the detection of sub-3 nm particles. Two of the CPCs use diethylene glycol as a working fluid: a laminar type diethlylene glycol CPC and a mixing type Airmodus A09 particle size magnifier. The other two CPCs are a laminar type TSI 3025A and a TSI 3786 with butanol and water as the working fluids, respectively. The nano-CPC battery was calibrated with seven different test aerosols: tetraheptyl ammonium bromide, ammonium sulfate, sodium chloride, tungsten oxide, sucrose, candle flame products and limonene ozonolysis products. The results show that ammonium sulfate and sodium chloride have a higher activation efficiency with the water-based 3786 than with the butanol-based 3025A, whereas the other aerosols were activated better with butanol than with water as the working fluid. It is worthwhile to mention that sub-2 nm limonene ozonolysis products were detected very poorly with all of the CPCs, butanol being the best fluid to activate the oxidation products. To explore how the detection efficiency is affected if the aerosol is an internal mixture of two different chemical substances, we made the first attempt to control the mixing state of sub-3 nm laboratory generated aerosol. We show that we generated an internally mixed aerosol of ammonium sulfate nucleated onto tungsten oxide seed particles, and observed that the activation efficiency of the internally mixed clusters was a function of the internal mixture composition. C1 [Kangasluoma, J.; Wimmer, D.; Rissanen, M. P.; Lehtipalo, K.; Ehn, M.; Worsnop, D. R.; Kulmala, M.; Petaja, T.] Univ Helsinki, Dept Phys, Helsinki 00014, Finland. [Kuang, C.; Wang, J.] Brookhaven Natl Lab, Atmospher Sci Div, Upton, NY 11789 USA. [Lehtipalo, K.] Airmodus Ltd, Helsinki 00560, Finland. [Worsnop, D. R.] Aerodyne Res Inc, Billerica, MA USA. RP Kuang, C (reprint author), Brookhaven Natl Lab, Atmospher Sci Div, Upton, NY 11789 USA. EM ckuang@bnl.gov RI Worsnop, Douglas/D-2817-2009; Wang, Jian/G-9344-2011; Petaja, Tuukka/A-8009-2008; Kulmala, Markku/I-7671-2016; Ehn, Mikael/N-2571-2016 OI Lehtipalo, Katrianne/0000-0002-1660-2706; Rissanen, Matti/0000-0003-0463-8098; Worsnop, Douglas/0000-0002-8928-8017; Petaja, Tuukka/0000-0002-1881-9044; Kangasluoma, Juha/0000-0002-1639-1187; Kulmala, Markku/0000-0003-3464-7825; Ehn, Mikael/0000-0002-0215-4893 FU European Research Council (ATMNUCLE) [227463]; Academy of Finland (Center of Excellence Program projects) [1118615, 139656]; Nordic Center for Excellence (CRAICC); European Commission seventh Framework program (ACTRIS) [262254]; European Commission seventh Framework program (PEGASOS) [265148]; Maj and Tor Nessling Foundation FX This work was partly funded by the European Research Council (ATMNUCLE, 227463), Academy of Finland (Center of Excellence Program projects 1118615 and 139656), Nordic Center for Excellence (CRAICC), European Commission seventh Framework program (ACTRIS, contract no. 262254; PEGASOS, contract no. 265148) and Maj and Tor Nessling Foundation. Also we want to thank the tofTools team for providing tools for mass spectrometry analysis and M. Attoui for providing the wire generator and electrospray source. NR 46 TC 20 Z9 20 U1 1 U2 25 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1867-1381 EI 1867-8548 J9 ATMOS MEAS TECH JI Atmos. Meas. Tech. PY 2014 VL 7 IS 3 BP 689 EP 700 DI 10.5194/amt-7-689-2014 PG 12 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA AE6LX UT WOS:000334105700001 ER PT J AU Jayakaran, AD Williams, TM Ssegane, H Amatya, DM Song, B Trettin, CC AF Jayakaran, A. D. Williams, T. M. Ssegane, H. Amatya, D. M. Song, B. Trettin, C. C. TI Hurricane impacts on a pair of coastal forested watersheds: implications of selective hurricane damage to forest structure and streamflow dynamics SO HYDROLOGY AND EARTH SYSTEM SCIENCES LA English DT Article ID ADAPTIVE REGRESSION SPLINES; SOUTHEASTERN UNITED-STATES; SPECIES EUCALYPT FOREST; AGE-RELATED-CHANGES; SOUTH-CAROLINA; NORTH-CAROLINA; CATASTROPHIC WIND; PINE PLANTATIONS; TIME-SERIES; HYDROLOGY AB Hurricanes are infrequent but influential disruptors of ecosystem processes in the southeastern Atlantic and Gulf coasts. Every southeastern forested wetland has the potential to be struck by a tropical cyclone. We examined the impact of Hurricane Hugo on two paired coastal South Carolina watersheds in terms of streamflow and vegetation dynamics, both before and after the hurricane's passage in 1989. The study objectives were to quantify the magnitude and timing of changes including a reversal in relative streamflow difference between two paired watersheds, and to examine the selective impacts of a hurricane on the vegetative composition of the forest. We related these impacts to their potential contribution to change watershed hydrology through altered evapotranspiration processes. Using over 30 years of monthly rainfall and streamflow data we showed that there was a significant transformation in the hydrologic character of the two watersheds - a transformation that occurred soon after the hurricane's passage. We linked the change in the rainfall-runoff relationship to a catastrophic change in forest vegetation due to selective hurricane damage. While both watersheds were located in the path of the hurricane, extant forest structure varied between the two watersheds as a function of experimental forest management techniques on the treatment watershed. We showed that the primary damage was to older pines, and to some extent larger hardwood trees. We believe that lowered vegetative water use impacted both watersheds with increased outflows on both watersheds due to loss of trees following hurricane impact. However, one watershed was able to recover to pre hurricane levels of evapotranspiration at a quicker rate due to the greater abundance of pine seedlings and saplings in that watershed. C1 [Jayakaran, A. D.; Williams, T. M.; Song, B.] Clemson Univ, Baruch Inst Coastal Ecol & Forest Sci, Georgetown, SC USA. [Ssegane, H.] Argonne Natl Lab, Div Energy Syst, Argonne, IL 60439 USA. [Amatya, D. M.; Trettin, C. C.] USDA Forest Serv, Ctr Forested Wetlands Res, Cordesville, SC USA. RP Jayakaran, AD (reprint author), Clemson Univ, Baruch Inst Coastal Ecol & Forest Sci, Georgetown, SC USA. EM ajayaka@clemson.edu RI Ssegane, Herbert/K-8098-2014; Jayakaran, Anand/M-2441-2016 OI Jayakaran, Anand/0000-0003-2605-9759 FU NIFA/USDA [SC1700394] FX The authors thank Andy Harrison for his significant contributions in assembling streamflow and rainfall data for watersheds 77 and 80. Dr. Jayakaran's contribution is based upon work supported by NIFA/USDA project number SC1700394, technical contribution number 6165 of the Clemson University Experiment Station. NR 90 TC 1 Z9 1 U1 2 U2 16 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1027-5606 EI 1607-7938 J9 HYDROL EARTH SYST SC JI Hydrol. Earth Syst. Sci. PY 2014 VL 18 IS 3 BP 1151 EP 1164 DI 10.5194/hess-18-1151-2014 PG 14 WC Geosciences, Multidisciplinary; Water Resources SC Geology; Water Resources GA AF1VJ UT WOS:000334501700017 ER PT S AU Karakaya, M Bolme, D Boehnen, C AF Karakaya, Mahmut Bolme, David Boehnen, Christopher BE Niel, KS Bingham, PR TI Eye Gaze Tracking using Correlation Filters SO IMAGE PROCESSING: MACHINE VISION APPLICATIONS VII SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Image Processing - Machine Vision Applications VII CY FEB 03-04, 2014 CL San Francisco, CA SP Soc Imaging Sci & Technol, SPIE DE Eye tracking; correlation filters; gaze estimation AB In this paper, we studied a method for eye gaze tracking that provide gaze estimation from a standard webcam with a zoom lens and reduce the setup and calibration requirements for new users. Specifically, we have developed a gaze estimation method based on the relative locations of points on the top of the eyelid and eye corners. Gaze estimation method in this paper is based on the distances between top point of the eyelid and eye corner detected by the correlation filters. Advanced correlation filters were found to provide facial landmark detections that are accurate enough to determine the subjects gaze direction up to angle of approximately 4-5 degrees although calibration errors often produce a larger overall shift in the estimates. This is approximately a circle of diameter 2 inches for a screen that is arm's length from the subject. At this accuracy it is possible to figure out what regions of text or images the subject is looking but it falls short of being able to determine which word the subject has looked at. C1 [Karakaya, Mahmut] Meliksah Univ, Mevlana Mahallesi, TR-38030 Talas Kayseri, Turkey. [Bolme, David; Boehnen, Christopher] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. RP Karakaya, M (reprint author), Meliksah Univ, Mevlana Mahallesi, TR-38030 Talas Kayseri, Turkey. EM mkarakaya@meliksah.edu.tr NR 15 TC 0 Z9 0 U1 0 U2 3 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9941-7 J9 PROC SPIE PY 2014 VL 9024 AR UNSP 90240U DI 10.1117/12.2040266 PG 12 WC Engineering, Electrical & Electronic; Optics; Imaging Science & Photographic Technology SC Engineering; Optics; Imaging Science & Photographic Technology GA BA2ZS UT WOS:000334026000023 ER PT S AU Porter, R Harvey, N Ruggiero, C AF Porter, Reid Harvey, Neal Ruggiero, Christy BE Niel, KS Bingham, PR TI Investigation of Segmentation Based Pooling for Image Quantification SO IMAGE PROCESSING: MACHINE VISION APPLICATIONS VII SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Image Processing - Machine Vision Applications VII CY FEB 03-04, 2014 CL San Francisco, CA SP Soc Imaging Sci & Technol, SPIE DE segmentation; semantic segmentation; feature pooling; image quantification; microscopy ID CLASSIFICATION; RECOGNITION AB A key step in many image quantification solutions is feature pooling, where subsets of lower-level features are combined so that higher-level, more invariant predictions can be made. The pooling region, which defines the subsets, often has a fixed spatial size and geometry, but data-adaptive pooling regions have also been used. In this paper we investigate pooling strategies for the data-adaptive case and suggest a new framework for pooling that uses multiple sub-regions instead of a single region. We show that this framework can help represent the shape of the pooling region and also produce useful pairwise features for adjacent pooling regions. We demonstrate the utility of the framework in a number of classification tasks relevant to image quantification in digital microscopy. C1 [Porter, Reid; Harvey, Neal; Ruggiero, Christy] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Porter, R (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM rporter@lanl.gov; harve@lanl.gov; ruggiero@lanl.gov NR 32 TC 0 Z9 0 U1 0 U2 0 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9941-7 J9 PROC SPIE PY 2014 VL 9024 AR 90240F DI 10.1117/12.2038707 PG 11 WC Engineering, Electrical & Electronic; Optics; Imaging Science & Photographic Technology SC Engineering; Optics; Imaging Science & Photographic Technology GA BA2ZS UT WOS:000334026000013 ER PT J AU Lu, Q Hutchings, GS Zhou, Y Xin, HLL Zheng, HM Jiao, F AF Lu, Qi Hutchings, Gregory S. Zhou, Yang Xin, Huolin L. Zheng, Haimei Jiao, Feng TI Nanostructured flexible Mg-modified LiMnPO4 matrix as high-rate cathode materials for Li-ion batteries SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID RECHARGEABLE LITHIUM BATTERIES; LIFEPO4 CATHODE; PERFORMANCE; ELECTRODES; ANODES; NANOCOMPOSITE; CAPACITY AB One-dimensional (1D) electrode materials have attracted much attention recently because of their potential application in flexible battery technology. Many 1D anode materials based on carbon and metal oxides have been synthesized for flexible batteries, however only limited studies on the cathode side have been conducted. Here, we report the synthesis of high-rate cathode electrodes based on Mg-modified LiMnPO4 nanofibers. The nanofibers are embedded inside a nanostructured conducting carbon matrix to enhance their electronic conductivity and structural integrity while retaining flexibility. As a result, a 50% increase in capacity is obtained, achieving an outstanding performance of 135 mA h g (-1) at a C/10 rate (15 mA g (-1)). This nanostructured Mg-modified LiMnPO4 matrix also exhibited superior rate capability and much better cycleability compared to its LiMnPO4 counterpart. Even at a high charge/discharge rate of 5C (750 mA g (-1)), 80% of the capacity (107 mA h g (-1)) is still retained, representing, to the best of our knowledge, the best rate performance for LiMnPO4-based electrodes. More importantly, such a superior rate capability is achieved with an excellent cycleability (no capacity fading for 200 deep cycles). C1 [Lu, Qi; Hutchings, Gregory S.; Jiao, Feng] Univ Delaware, Dept Chem & Biomol Engn, Newark, DE 19716 USA. [Zhou, Yang] Univ Delaware, Dept Phys & Astron, Newark, DE 19716 USA. [Xin, Huolin L.; Zheng, Haimei] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. RP Jiao, F (reprint author), Univ Delaware, Dept Chem & Biomol Engn, Newark, DE 19716 USA. EM jiao@udel.edu RI Hutchings, Gregory/B-5620-2012; Xin, Huolin/E-2747-2010; Lu, Qi/P-7477-2016; OI Hutchings, Gregory/0000-0002-0819-9654; Xin, Huolin/0000-0002-6521-868X; Jiao, Feng/0000-0002-3335-3203 FU University of Delaware Research Foundation (UDRF); U.S. Department of Energy (DOE) [DE-AC02-05CH11231] FX The authors are grateful to the University of Delaware Research Foundation (UDRF) for financial support. H. L. Xin and H. M. Zheng acknowledge the support from U.S. Department of Energy (DOE) under Contract # DE-AC02-05CH11231. H. L. Xin thanks Haiyan Tan for supplying the MnO reference spectrum. NR 38 TC 24 Z9 27 U1 8 U2 81 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 2014 VL 2 IS 18 BP 6368 EP 6373 DI 10.1039/c4ta00654b PG 6 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA AE6RW UT WOS:000334123100017 ER PT J AU Lee, D Lee, YL Grimaud, A Hong, WT Biegalski, MD Morgan, D Shao-Horn, Y AF Lee, Dongkyu Lee, Yueh-Lin Grimaud, Alexis Hong, Wesley T. Biegalski, Michael D. Morgan, Dane Shao-Horn, Yang TI Strontium influence on the oxygen electrocatalysis of La2-xSrxNiO4 +/-delta (0.0 <= x(Sr) <= 1.0) thin films SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID OXIDE FUEL-CELLS; SURFACE EXCHANGE KINETICS; TRANSPORT-PROPERTIES; NEUTRON-DIFFRACTION; LA1-XSRXMN1-YCOYO3+/-DELTA PEROVSKITES; ELECTROCHEMICAL PROPERTIES; ELECTRICAL-PROPERTIES; REDUCTION KINETICS; TRACER DIFFUSION; TEMPERATURE AB Substitution of lanthanum by strontium (Sr) in the A-site of cobalt-containing perovskites can greatly promote oxygen surface exchange kinetics at elevated temperatures. Little is known about the effect of A-site substitution on the oxygen electrocatalysis of Ruddlesden-Popper (RP) oxides. In this study, we report, for the first time, the growth and oxygen surface exchange kinetics of La2-xSrxNiO4 +/-delta (LSNO, 0.0 <= x(Sr) <= 1.0) thin films grown on (001)(cubic)-Y2O3-stabilized ZrO2 (YSZ) by pulsed laser deposition. Highresolution X-ray diffraction analysis revealed that the LSNO film orientation was changed gradually from the (100)(tetra). (in-plane) to the (001)(tetra). (out-of-plane) orientation in the RP structure with increasing Sr from La2NiO4+delta (x(Sr) (=) 0) to LaSrNiO4 +/-delta (x(Sr) = 1.0). Such a change in the LSNO film orientation was accompanied by reduction in the oxygen surface exchange kinetics by two orders of magnitude as shown from electrochemical impedance spectroscopy results. Density functional theory (DFT) calculations showed that Sr substitution could stabilize the (001)(tetra). surface relative to the (100)(tetra). surface and both Sr substitution and increasing (001)(tetra). surface could greatly weaken adsorption of molecular oxygen in the La-La bridge sites in the RP structure, which can reduce oxygen surface exchange kinetics. C1 [Lee, Dongkyu; Lee, Yueh-Lin; Grimaud, Alexis; Hong, Wesley T.; Shao-Horn, Yang] MIT, Electrochem Energy Lab, Cambridge, MA 02139 USA. [Lee, Dongkyu; Lee, Yueh-Lin; Grimaud, Alexis; 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 Lee, D (reprint author), MIT, Electrochem Energy Lab, 77 Massachusetts Ave, Cambridge, MA 02139 USA. EM shaohorn@mit.edu RI Hong, Wesley/H-1102-2014; LEE, YUEH-LIN/F-6274-2011 OI LEE, YUEH-LIN/0000-0003-2477-6412 FU DOE [SISGR DESC0002633]; King Abdullah University of Science and Technology; King Fahd University of Petroleum and Minerals in Dharam, Saudi Arabia through the Center for Clean Water and Clean Energy; U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering [DESC0001284]; National Science Foundation [OCI-1053575]; Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy FX This work was supported in part by DOE (SISGR DESC0002633) and King Abdullah University of Science and Technology. The authors would like to thank the King Fahd University of Petroleum and Minerals in Dharam, Saudi Arabia, for funding the research reported in this paper through the Center for Clean Water and Clean Energy at MIT and KFUPM. Funding for D. Morgan and partial support for Y.-L. Lee provided by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering under award number DESC0001284. This work also benefitted from the use of the Extreme Science and Engineering Discovery Environment (XSEDE), which is supported by National Science Foundation grant number OCI-1053575. PLD was 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. NR 63 TC 16 Z9 16 U1 6 U2 47 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 2014 VL 2 IS 18 BP 6480 EP 6487 DI 10.1039/c3ta14918h PG 8 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA AE6RW UT WOS:000334123100032 ER PT J AU Cottingham, P Miller, DC Sheckelton, JP Neilson, JR Feygenson, M Huq, A McQueen, TM AF Cottingham, Patrick Miller, David C. Sheckelton, John P. Neilson, James R. Feygenson, Mikhail Huq, Ashfia McQueen, Tyrel M. TI Dynamic charge disproportionation in the 1D chain material PdTeI SO JOURNAL OF MATERIALS CHEMISTRY C LA English DT Article ID DENSITY-WAVE; TRANSITION; METAL AB PdTeI features quasi-1D -Pd-Te-Pd-Te- chains with palladium formally in the 3+ oxidation state. Using pair distribution function analysis of X-ray and neutron total scattering data, we find that there is a local charge-density wave arising from the disproportionation of Pd3+ towards Pd2+ in pseudo-square planar, and Pd4+ in pseudo-octahedral, coordination. The magnitude and coherence length for this distortion is small, such that the average structure determined by Bragg diffraction techniques possesses higher symmetry than the local structure at all temperatures. Temperature-dependent resistivity measurements show a transport anomaly at T-CDW = 50 K, corresponding to the reduced fluctuations of the charge separated Pd2+ and Pd4+ sites. At higher temperatures, the charge separation is dynamic, with local Pd2+/Pd4+ pairs persisting up to room temperature. C1 [Cottingham, Patrick; Miller, David C.; Sheckelton, John P.; Neilson, James R.; McQueen, Tyrel M.] Johns Hopkins Univ, Dept Chem, Baltimore, MD 21218 USA. [Feygenson, Mikhail; Huq, Ashfia] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. RP McQueen, TM (reprint author), Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. EM mcqueen@jhu.edu RI Feygenson, Mikhail /H-9972-2014; Huq, Ashfia/J-8772-2013; OI Feygenson, Mikhail /0000-0002-0316-3265; Huq, Ashfia/0000-0002-8445-9649; Neilson, James/0000-0001-9282-5752 FU American Chemical Society Petroleum Research Fund; National Science Foundation (NSF), Division of Materials Research (DMR), CAREER [1253562]; U. S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]; Division of Scientific User Facilities, Office of Basic Energy Sciences, U.S. Department of Energy [DE-AC05-00OR22725]; UT-Battelle, LLC FX Acknowledgment is made to the donors of the American Chemical Society Petroleum Research Fund and the National Science Foundation (NSF), Division of Materials Research (DMR), CAREER grant #1253562 for support of this research. Use of the Advanced Photon Source (APS) 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 thank Matthew Suchomel (11-BM) and Karena Chapman (11-ID-B) for their assistance with experiments at the APS. Use of the Spallation Neutron Source (SNS) is supported by the Division of Scientific User Facilities, Office of Basic Energy Sciences, U.S. Department of Energy, under contract DE-AC05-00OR22725 with UT-Battelle, LLC. Patrick Cottingham acknowledges the assistance of Mark Koontz with EDX/SEM measurements. NR 41 TC 3 Z9 3 U1 1 U2 20 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 2014 VL 2 IS 17 BP 3238 EP 3246 DI 10.1039/c3tc32051k PG 9 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA AE6SL UT WOS:000334124800019 ER PT J AU Williams, TE Chang, CM Rosen, EL Garcia, G Runnerstrom, EL Williams, BL Koo, B Buonsanti, R Milliron, DJ Helms, BA AF Williams, Teresa E. Chang, Christina M. Rosen, Evelyn L. Garcia, Guillermo Runnerstrom, Evan L. Williams, Bradley L. Koo, Bonil Buonsanti, Raffaella Milliron, Delia J. Helms, Brett A. TI NIR-Selective electrochromic heteromaterial frameworks: a platform to understand mesoscale transport phenomena in solid-state electrochemical devices SO JOURNAL OF MATERIALS CHEMISTRY C LA English DT Article ID DOPED SEMICONDUCTOR NANOCRYSTALS; TUNABLE INFRARED-ABSORPTION; OXIDE NANOCRYSTALS; COLLOIDAL NANOCRYSTALS; OPTICAL-PROPERTIES; PLASMON RESONANCE; THIN-FILMS; ARCHITECTURES AB We report here the first solid-state, NIR-selective electrochromic devices. Critical to device performance is the arrangement of nanocrystal-derived electrodes into heteromaterial frameworks, where hierarchically porous ITO nanocrystal active layers are infiltrated by an ion-conducting polymer electrolyte with mesoscale periodicity. Enhanced coloration efficiency and transport are realized over unarchitectured electrodes in devices, paving the way towards new smart windows technologies. C1 [Williams, Teresa E.; Chang, Christina M.; Rosen, Evelyn L.; Runnerstrom, Evan L.; Williams, Bradley L.; Milliron, Delia J.; Helms, Brett A.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA. [Williams, Teresa E.] Univ Calif Berkeley, Grad Grp Appl Sci & Technol, Berkeley, CA 94720 USA. [Garcia, Guillermo; Koo, Bonil] Heliotrope Technol, Berkeley, CA 94705 USA. [Runnerstrom, Evan L.] Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA. [Buonsanti, Raffaella] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Joint Ctr Artificial Photosynth, Berkeley, CA 94720 USA. [Buonsanti, Raffaella] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. [Milliron, Delia J.] Univ Texas Austin, Dept Chem Engn, Austin, TX 78712 USA. RP Helms, BA (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mol Foundry, 1 Cyclotron Rd, Berkeley, CA 94720 USA. EM milliron@che.utexas.edu; bahelms@lbl.gov RI Milliron, Delia/D-6002-2012; Foundry, Molecular/G-9968-2014; OI Helms, Brett/0000-0003-3925-4174 FU Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231]; ARPA-E [DE-AR0000334]; U.S Department of Energy [DE-SC0009472]; Office of Science of the U.S. Department of Energy [DE-SC0004993] FX GISAXS data were acquired at the Advanced Light Source and all other work was performed at the Molecular Foundry; both are 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.J.M. and E. L. R. were supported by ARPA-E under contract DE-AR0000334. G. G. and B. K. were supported by U.S Department of Energy, STTR grant no. DE-SC0009472. R. B. is supported by the Office of Science of the U.S. Department of Energy under award number DE-SC0004993. A. Wills and E. Schaible are thanked for assistance with GISAXS at ALS beamline 7.3.3. S. Doris is also thanked for helpful discussions. D.J.M. discloses a financial interest in Heliotrope Technologies, a company pursuing commercial development of electrochromic devices. NR 29 TC 12 Z9 12 U1 5 U2 38 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 2014 VL 2 IS 17 BP 3328 EP 3335 DI 10.1039/c3tc32247e PG 8 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA AE6SL UT WOS:000334124800029 ER PT J AU Lee, H Zhang, Y Zhang, L Mirabito, T Burnett, EK Trahan, S Mohebbi, AR Mannsfeld, SCB Wudl, F Briseno, AL AF Lee, Hyunbok Zhang, Yue Zhang, Lei Mirabito, Timothy Burnett, Edmund K. Trahan, Stefan Mohebbi, Ali Reza Mannsfeld, Stefan C. B. Wudl, Fred Briseno, Alejandro L. TI Rubicene:a molecular fragment of C-70 for use in organic field-effect transistors SO JOURNAL OF MATERIALS CHEMISTRY C LA English DT Article ID ENERGY-LEVEL ALIGNMENT; THIN-FILM TRANSISTORS; PHOTOPHYSICAL PROPERTIES; ELECTRONIC-STRUCTURE; CRYSTAL-STRUCTURES; CHARGE-TRANSPORT; INTERFACES; SEMICONDUCTORS; DENSITY; SPECTROSCOPIES AB Rubicene, a molecular fragment of C-70, is a promising organic semiconductor material that displays excellent electronic characteristics for use in organic field-effect transistors (OFETs). Bottom-gate/ bottom-contact polycrystalline thin-film OFETs using rubicene exhibit a saturation hole mobility of 0.20 cm(2) V-1 s-(1) and a current on/off ratio ( (I)on/ (I)off) of 1.0 Chi 104. In addition, the device performance can be improved with a mobility of 0.32 cm2 V-1 s-(1) and Ion/ Ioff of 2.5 Chi 104 with pentafluorobenzenethiol (PFBT) self-assembled monolayer (SAM) treatment on Au electrodes. To characterize the interfacial electronic structure and morphology of rubicene on Au and PFBT/ Au, ultraviolet photoelectron spectroscopy (UPS), theoretical calculation with density functional theory (DFT) and grazing incidence X-ray diffraction (GIXD) were performed. With PFBT SAM treatment, the hole injection barrier from Au to rubicene is significantly decreased from 1.15 to 0.48 eV due to the formation of a large interface dipole on Au that increased its work function from 4.33 to 5.67 eV. Furthermore, PFBT SAM treatment also induces an "edge-on" configuration of rubicene, which can lead to the increase in carrier mobility. These results indicate that rubicene can serve as a benchmark organic semiconductor for model charge transport studies and in various organic electronic devices. C1 [Lee, Hyunbok; Zhang, Yue; Zhang, Lei; Mirabito, Timothy; Burnett, Edmund K.; Trahan, Stefan; Briseno, Alejandro L.] Univ Massachusetts, Dept Polymer Sci & Engn, Amherst, MA 01003 USA. [Mohebbi, Ali Reza; Wudl, Fred] Univ Calif Santa Barbara, Dept Chem & Biochem, Santa Barbara, CA 93106 USA. [Mannsfeld, Stefan C. B.] Stanford Synchrotron Radiat Lab, SLAC Natl Accelerator Lab, Menlo Pk, CA 94025 USA. RP Briseno, AL (reprint author), Univ Massachusetts, Dept Polymer Sci & Engn, 120 Governors Dr, Amherst, MA 01003 USA. EM abriseno@mail.pse.umass.edu FU Office of Naval Research [N000141110636]; U.S. Department of Energy, Office of Basic Energy Sciences [DE-SC0001087]; Department of Energy [DE-FG02-08ER46535] FX A. L. B acknowledges support by the Office of Naval Research (N000141110636). UPS measurements were carried out as part of the Polymer-Based Materials for Harvesting Solar Energy laboratory, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Basic Energy Sciences under Award number DE-SC0001087. F. W and A. R. M thank the Department of Energy through Grant # DE-FG02-08ER46535. The authors thank Volodimyr V. Duzhko and Jayanta K. Baral for valuable discussion and support in the initial experimental setup and Dr. Sean Parkin for helping explain the crystal structure refinement data. NR 48 TC 16 Z9 16 U1 3 U2 26 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 2014 VL 2 IS 17 BP 3361 EP 3366 DI 10.1039/c3tc32117g PG 6 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA AE6SL UT WOS:000334124800032 ER PT J AU Palermo, EF Darling, SB McNeil, AJ AF Palermo, Edmund F. Darling, Seth B. McNeil, Anne J. TI pi-Conjugated gradient copolymers suppress phase separation and improve stability in bulk heterojunction solar cells SO JOURNAL OF MATERIALS CHEMISTRY C LA English DT Article ID CURRENT-VOLTAGE CHARACTERISTICS; CRITICAL MICELLE CONCENTRATIONS; POLYMER PHOTOVOLTAIC DEVICES; STATE SHEAR PULVERIZATION; BLOCK-COPOLYMERS; FUNCTIONALIZED POLYTHIOPHENE; ORGANIC PHOTOVOLTAICS; MORPHOLOGY CONTROL; DISPERSED PHASE; BLENDS AB Gradient sequence copolymers of 3-hexylthiophene (90 mol%) and 3-(6-bromohexyl) thiophene (10 mol%) were synthesized by catalyst transfer polycondensation. Post-polymerization conversion of the side-chain bromides into azides and subsequent Cu-catalyzed azide-alkyne cycloaddition installed C60-functional groups. Comparing blends of poly(3- hexylthiophene) (P3HT) and phenyl-C61-butyric acid methyl ester (PCBM) with and without the gradient copolymer additive revealed that, when the gradient copolymer was present, micron-scale phase separation was not observed even after prolonged thermal annealing times. In addition, the PCBM was still able to quench the P3HT emission after thermal annealing, indicating that the donor-acceptor interfacial area is maintained. Together, these data suggest that the gradient copolymers are an effective compatibilizer for P3HT/PCBM physical blends. This stabilized film morphology led to stable power conversion efficiencies (PCE) of the corresponding bulk heterojunction solar cells even upon extended thermal annealing. Nevertheless, the short circuit current and fill factor were reduced when the gradient copolymer was present, leading to a lower PCE. Overall, these gradient copolymer additives represent a promising tool for inhibiting micron-scale phase separation and producing robust polymer/fullerene-based solar cells. C1 [Palermo, Edmund F.; McNeil, Anne J.] Univ Michigan, Dept Chem, Ann Arbor, MI 48109 USA. [Palermo, Edmund F.; McNeil, Anne J.] Univ Michigan, Macromol Sci & Engn Program, Ann Arbor, MI 48109 USA. [Darling, Seth B.] Argonne Natl Lab, Ctr Nanoscale Mat, Argonne, IL 60439 USA. [Darling, Seth B.] Univ Chicago, Inst Mol Engn, Chicago, IL 60637 USA. RP McNeil, AJ (reprint author), Univ Michigan, Dept Chem, 930 North Univ Ave, Ann Arbor, MI 48109 USA. EM ajmcneil@umich.edu FU Army Research Office [ARO 58200-CH-PCS]; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]; Camille and Henry Dreyfus Foundation FX We thank the Army Research Office (ARO 58200-CH-PCS) for support of this work. Use of the Center for Nanoscale Materials 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. J. M. thanks the Camille and Henry Dreyfus Foundation for a research fellowship. We also gratefully acknowledge Dr Chun-Chih Ho, Dr Matthew Pelton and Dr David Gosztola for assistance with device fabrication testing and PL measurements. NR 62 TC 22 Z9 22 U1 3 U2 49 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 2014 VL 2 IS 17 BP 3401 EP 3406 PG 6 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA AE6SL UT WOS:000334124800037 ER PT J AU Karimi, S Jiang, XQ Cosman, P Martz, H AF Karimi, Seemeen Jiang, Xiaoqian Cosman, Pamela Martz, Harry TI Flexible methods for segmentation evaluation: Results from CT-based luggage screening SO JOURNAL OF X-RAY SCIENCE AND TECHNOLOGY LA English DT Article DE Segmentation evaluation; computed tomography; luggage screening; feature recovery ID IMAGE SEGMENTATION; ALGORITHMS; TRUTH AB BACKGROUND: Imaging systems used in aviation security include segmentation algorithms in an automatic threat recognition pipeline. The segmentation algorithms evolve in response to emerging threats and changing performance requirements. Analysis of segmentation algorithms' behavior, including the nature of errors and feature recovery, facilitates their development. However, evaluation methods from the literature provide limited characterization of the segmentation algorithms. OBJECTIVE: To develop segmentation evaluation methods that measure systematic errors such as oversegmentation and undersegmentation, outliers, and overall errors. The methods must measure feature recovery and allow us to prioritize segments. METHODS: We developed two complementary evaluation methods using statistical techniques and information theory. We also created a semi-automatic method to define ground truth from 3D images. We applied our methods to evaluate five segmentation algorithms developed for CT luggage screening. We validated our methods with synthetic problems and an observer evaluation. RESULTS: Both methods selected the same best segmentation algorithm. Human evaluation confirmed the findings. The measurement of systematic errors and prioritization helped in understanding the behavior of each segmentation algorithm. CONCLUSIONS: Our evaluation methods allow us to measure and explain the accuracy of segmentation algorithms. C1 [Karimi, Seemeen; Jiang, Xiaoqian; Cosman, Pamela] Univ Calif San Diego, San Diego, CA 92103 USA. [Martz, Harry] Lawrence Livermore Natl Lab, Livermore, CA USA. RP Karimi, S (reprint author), Univ Calif San Diego, San Diego, CA 92103 USA. EM seemeen.karimi@gmail.com FU Lawrence Livermore National Laboratories; Science and Technology Directorate of the Department of Homeland Security; Northeastern University FX The authors thank Dr. J. Beaty and the ALERT group at Northeastern University for supplying the image sets. The authors are very grateful to Jihoon Kim for help with the statistical testing, and to Drs. A. Boxwala, J. Kallman, S. Azevedo, K. Bond, and C. Crawford. This work was performed under the auspices of Lawrence Livermore National Laboratories, the Science and Technology Directorate of the Department of Homeland Security, and Northeastern University. NR 41 TC 1 Z9 1 U1 1 U2 6 PU IOS PRESS PI AMSTERDAM PA NIEUWE HEMWEG 6B, 1013 BG AMSTERDAM, NETHERLANDS SN 0895-3996 EI 1095-9114 J9 J X-RAY SCI TECHNOL JI J. X-Ray Sci. Technol. PY 2014 VL 22 IS 2 BP 175 EP 195 DI 10.3233/XST-140418 PG 21 WC Instruments & Instrumentation; Optics; Physics, Applied SC Instruments & Instrumentation; Optics; Physics GA AE9TS UT WOS:000334353600004 PM 24699346 ER PT J AU Choi, YJ Ronnebro, ECE Rassat, S Karkamkar, A Maupin, G Holladay, J Simmons, K Brooks, K AF Choi, Young Joon Roennebro, Ewa C. E. Rassat, Scot Karkamkar, Abhi Maupin, Gary Holladay, Jamie Simmons, Kevin Brooks, Kriston TI Kinetics study of solid ammonia borane hydrogen release - modeling and experimental validation for chemical hydrogen storage SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID THERMAL-DECOMPOSITION; ALUMINUM-HYDRIDE; REQUIREMENTS; REGENERATION AB Ammonia borane (AB), NH3BH3, is a promising material for chemical hydrogen storage with 19.6 wt% gravimetric hydrogen capacity of which maximum 16.2 wt% hydrogen can be released via an exothermic thermal decomposition below 200 degrees C. We have investigated the kinetics of hydrogen release from AB and from an AB-methyl cellulose (AB/MC) composite at temperatures of 160-300 degrees C using both experiments and modeling. The hydrogen release rate at 300 degrees C is twice as fast as at 160 degrees C. The purpose of our study was to show safe hydrogen release without thermal runaway effects and to validate system model kinetics. AB/MC released hydrogen at similar to 20 degrees C lower than neat AB and at a faster release rate in that temperature range. Based on the experimental results, the kinetics equations were revised to better represent the growth and nucleation process during decomposition of AB. We explored two different reactor concepts; auger and fixed bed. The current auger reactor concept turned out to not be appropriate, however, we demonstrated safe self-propagation of the hydrogen release reaction of solid AB/MC in a fixed bed reactor. C1 [Choi, Young Joon; Roennebro, Ewa C. E.; Rassat, Scot; Karkamkar, Abhi; Maupin, Gary; Holladay, Jamie; Simmons, Kevin; Brooks, Kriston] Pacific NW Natl Lab, Richland, WA 99352 USA. [Choi, Young Joon] Globalfoundries, Malta, NY 12020 USA. RP Ronnebro, ECE (reprint author), Pacific NW Natl Lab, 902 Battelle Blvd, Richland, WA 99352 USA. EM youngjoon.choi@globalfoundries.com; ewa.ronnebro@pnnl.gov FU U.S. Department of Energy's Fuel Cell Technology Office; U.S. Department of Energy's Office of Biological and Environmental Research FX The authors acknowledge support from the U.S. Department of Energy's Fuel Cell Technology Office. This work was performed as part of the Center of Excellence in Hydrogen Storage Engineering. Troy Semelsberger of LANL, Donald Anton of SRNL and Tom Autrey of PNNL are acknowledged for fruitful discussions. Timothy Peters of PNNL is acknowledged for valuable work on the fixed bed reactor. A portion of the research described in this paper was performed in the Environmental Molecular Science Laboratory, a national scientific user facility sponsored by the U.S. Department of Energy's Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory. Pacific Northwest National Laboratory is operated for U.S. DOE by Battelle. NR 22 TC 8 Z9 8 U1 0 U2 34 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 2014 VL 16 IS 17 BP 7959 EP 7968 DI 10.1039/c3cp55280b PG 10 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AE7SY UT WOS:000334200400036 PM 24647627 ER PT J AU Zhang, YW Aidhy, DS Varga, T Moll, S Edmondson, PD Namavar, F Jin, K Ostrouchov, CN Weber, WJ AF Zhang, Yanwen Aidhy, Dilpuneet S. Varga, Tamas Moll, Sandra Edmondson, Philip D. Namavar, Fereydoon Jin, Ke Ostrouchov, Christopher N. Weber, William J. TI The effect of electronic energy loss on irradiation-induced grain growth in nanocrystalline oxides SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID CERIA; SIMULATION; NANOPORES; PHASE; CEO2 AB Grain growth of nanocrystalline materials is generally thermally activated, but can also be driven by irradiation at much lower temperature. In nanocrystalline ceria and zirconia, energetic ions deposit their energy to both atomic nuclei and electrons. Our experimental results have shown that irradiation-induced grain growth is dependent on the total energy deposited, where electronic energy loss and elastic collisions between atomic nuclei both contribute to the production of disorder and grain growth. Our atomistic simulations reveal that a high density of disorder near grain boundaries leads to locally rapid grain movement. The additive effect from both electronic excitation and atomic collision cascades on grain growth demonstrated in this work opens up new possibilities for controlling grain sizes to improve functionality of nanocrystalline materials. C1 [Zhang, Yanwen; Aidhy, Dilpuneet S.; Weber, William J.] Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. [Zhang, Yanwen; Jin, Ke; Ostrouchov, Christopher N.; Weber, William J.] Univ Tennessee, Dept Mat Sci & Engn, Knoxville, TN 37996 USA. [Varga, Tamas] Pacific NW Natl Lab, Richland, WA 99352 USA. [Moll, Sandra] TN Int AREVA, F-78182 Montigny Le Bretonneux, France. [Edmondson, Philip D.] Univ Oxford, Dept Mat, Oxford OX1 3PH, England. [Namavar, Fereydoon] Univ Nebraska Med Ctr, Omaha, NE 68198 USA. RP Zhang, YW (reprint author), Oak Ridge Natl Lab, Div Mat Sci & Technol, 4500S A148,MS 6138, Oak Ridge, TN 37831 USA. EM Zhangy1@ornl.gov RI Weber, William/A-4177-2008; Edmondson, Philip/O-7255-2014 OI Weber, William/0000-0002-9017-7365; Edmondson, Philip/0000-0001-8990-0870 FU Materials Science of Actinides, an Energy Frontier Research Center; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences; Department of Energy's Office of Biological and Environmental Research FX This work was supported as part of the Materials Science of Actinides, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences. A portion of research was performed at the UT-ORNL Ion Beam Materials Laboratory (IBML, http://ibml.utk.edu/) located at the University of Tennessee, Knoxville and the Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility sponsored by the Department of Energy's Office of Biological and Environmental Research located at Pacific Northwest National Laboratory. The MD simulations were performed at the National Energy Research Scientific Computing Center at Lawrence Berkeley National Laboratory. NR 42 TC 19 Z9 19 U1 3 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 2014 VL 16 IS 17 BP 8051 EP 8059 DI 10.1039/c4cp00392f PG 9 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AE7SY UT WOS:000334200400046 PM 24651953 ER PT J AU Sai, N Leung, K Zador, J Henkelman, G AF Sai, Na Leung, Kevin Zador, Judit Henkelman, Graeme TI First principles study of photo-oxidation degradation mechanisms in P3HT for organic solar cells SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID DENSITY-FUNCTIONAL THEORY; INTER-LABORATORY COLLABORATION; SOLID-STATE PHOTOCHEMISTRY; FINDING SADDLE-POINTS; PHOTOELECTRON-SPECTROSCOPY; PHOTOVOLTAIC DEVICES; POLYMER; OXYGEN; POLY(3-HEXYLTHIOPHENE); POLY(3-ALKYLTHIOPHENES) AB We present a theoretical study of degradation mechanisms for photoinduced oxidation in organic polymers in the condensed phase, using poly(3-hexylthiophene) (P3HT) as an example. Applying density functional theory with a hybrid density functional and periodic boundary conditions that account for steric effects and permit the modeling of interchain chemical reactions, we investigate reaction pathways that may lead to the oxidation of the thiophene backbone as a critical step toward disrupting the polymer conjugation. We calculate energy barriers for reactions of the P3HT backbone with oxidizing agents including the hydroxyl radical (OH center dot), hydroperoxide (ROOH), and the peroxyl radical (ROO center dot), following a UV-driven radical reaction starting at the alpha-carbon of the alkyl side chain as suggested by infrared (IR) and X-ray photoemission (XPS) spectrosocopy studies. The results strongly suggest that an attack of OH center dot on sulfur in P3HT is unlikely to be thermodynamically favored. On the other hand, an attack of a peroxyl radical on the side chain on the P3HT backbone may provide low barrier reaction pathways to photodegradation of P3HT and other polymers with side chains. The condensed phase setting is found to qualitatively affect predictions of degradation processes. C1 [Sai, Na; Henkelman, Graeme] Univ Texas Austin, Energy Frontier Res Ctr EFRC CST, Austin, TX 78712 USA. [Sai, Na; Henkelman, Graeme] Univ Texas Austin, Inst Computat Engn & Sci, Austin, TX 78712 USA. [Sai, Na] Univ Texas Austin, Dept Phys, Austin, TX 78712 USA. [Leung, Kevin] Sandia Natl Labs, Albuquerque, NM 87185 USA. [Zador, Judit] Sandia Natl Labs, Livermore, CA 94550 USA. RP Sai, N (reprint author), Univ Texas Austin, Energy Frontier Res Ctr EFRC CST, Austin, TX 78712 USA. EM nsai@physics.utexas.edu RI Zador, Judit/A-7613-2008 OI Zador, Judit/0000-0002-9123-8238 FU Understanding Charge Separation and Transfer at Interfaces in Energy Materials (EFRC:CST); US Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001091]; Division of Chemical Sciences, Geosciences, and Biosciences; Office of Basic Energy Sciences; U.S. Department of Energy; National Nuclear Security Administration [DEAC04-94-AL85000] FX NS thanks Christopher W. Bielawski, Bradley J. Holliday, and Peter J. Rossky for valuable conversations. This work was supported as part of the Understanding Charge Separation and Transfer at Interfaces in Energy Materials (EFRC:CST), an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Office of Basic Energy Sciences under Award Number DE-SC0001091. Computing resources were provided by the National Energy Research Scientific Computing Center (NERSC) and the Texas Advanced Computing Center (TACC). J.Z. is supported by the Division of Chemical Sciences, Geosciences, and Biosciences, the Office of Basic Energy Sciences, the 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 DEAC04-94-AL85000. NR 55 TC 25 Z9 25 U1 4 U2 76 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 2014 VL 16 IS 17 BP 8092 EP 8099 DI 10.1039/c4cp00146j PG 8 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AE7SY UT WOS:000334200400051 PM 24652517 ER PT J AU Hopkins, JC Carr, AB AF Hopkins, John C. Carr, Alan B. TI Harold Melvin Agnew Obituary SO PHYSICS TODAY LA English DT Biographical-Item C1 [Hopkins, John C.; Carr, Alan B.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Hopkins, JC (reprint author), Los Alamos Natl Lab, Los Alamos, NM 87545 USA. NR 1 TC 0 Z9 0 U1 0 U2 0 PU AMER INST PHYSICS PI MELVILLE PA CIRCULATION & FULFILLMENT DIV, 2 HUNTINGTON QUADRANGLE, STE 1 N O 1, MELVILLE, NY 11747-4501 USA SN 0031-9228 EI 1945-0699 J9 PHYS TODAY JI Phys. Today PD JAN PY 2014 VL 67 IS 1 BP 56 EP 56 PG 1 WC Physics, Multidisciplinary SC Physics GA AE8IR UT WOS:000334244000016 ER PT J AU Kogan, V Prozorov, R Huebener, R AF Kogan, Vladimir Prozorov, Ruslan Huebener, Rudolf TI John Richard Clem Obituary SO PHYSICS TODAY LA English DT Biographical-Item C1 [Kogan, Vladimir; Prozorov, Ruslan] Iowa State Univ, Ames Lab, Ames, IA 50011 USA. [Huebener, Rudolf] Univ Tubingen, Tubingen, Germany. RP Kogan, V (reprint author), Iowa State Univ, Ames Lab, Ames, IA 50011 USA. NR 1 TC 0 Z9 0 U1 0 U2 1 PU AMER INST PHYSICS PI MELVILLE PA CIRCULATION & FULFILLMENT DIV, 2 HUNTINGTON QUADRANGLE, STE 1 N O 1, MELVILLE, NY 11747-4501 USA SN 0031-9228 EI 1945-0699 J9 PHYS TODAY JI Phys. Today PD JAN PY 2014 VL 67 IS 1 BP 56 EP 57 PG 2 WC Physics, Multidisciplinary SC Physics GA AE8IR UT WOS:000334244000017 ER PT S AU Perakis, IE Lingos, PC Wang, J AF Perakis, I. E. Lingos, P. C. Wang, J. BE Betz, M Elezzabi, AY Song, JJ Tsen, KT TI Quantum tricks with femtosecond light pulses teach magnetic devices to think ultrafast SO ULTRAFAST PHENOMENA AND NANOPHOTONICS XVIII SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Ultrafast Phenomena and Nanophotonics XVIII CY FEB 02-05, 2014 CL San Francisco, CA SP SPIE, Femtolasers, Inc DE Femtosecond Magnetism; ultrafast nonlinear optical response; quantum spin dynamics; non-equilibrium materials manipulation; all-optical switching; Photoinduced Nonequilibrium Phase Transitions; coherent control ID PHASE-SEPARATION; MANGANITE; SPIN AB The technological demand to push the gigahertz switching speed limit of today's magnetic memory/logic devices into the terahertz (1THz=1ps(-1)) regime underlies the entire field of spin-electronics and integrated multifunctional devices. This challenge is met by all-optical magnetic switching based on coherent spin manipulation By analogy to femto-chemistry and photosynthetic dynamics where photo-products of chemical/biochemical reactions can be influenced by creating suitable superpositions of molecular states, femtosecond (fs) laser-excited coherence between spin/orbital/charge states can switch magnetic orders, by "suddenly" breaking the delicate balance between competing phases of correlated materials, e.g., the colossal magneto-resistive (CMR) manganites suitable for applications. Here we discuss femtosecond (fs) all-optical switching from antiferro- to ferromagnetic ordering via establishment of a magnetization increase within similar to 100 fs, while the laser field still interacts with the system. Such non-equilibrium ferromagnetic correlations arise from quantum spin-flip fluctuations correlated with coherent superpositions of electronic states. The development of ferromagnetic correlations during the fs laser pulse reveals an initial quantum coherent regime of magnetism, clearly distinguished from the picosecond lattice-heating regime characterized by phase separation. We summarize a microscopic theory based on density matrix equations of motion for composite fermion Hubbard operators, instead of bare electrons, that take into account the strong spin and charge local correlations. Our work merges two fields, femto-magnetism in metals/band insulators and non-equilibrium phase transitions of strongly correlated electrons, where local interactions exceeding the kinetic energy produce a complex balance of competing orders. C1 [Perakis, I. E.; Lingos, P. C.] Univ Crete, Dept Phys, Iraklion 71003, Crete, Greece. [Perakis, I. E.] Fdn Res & Technol Hellas, Inst Elect Strut & Laser, Iraklion 71003, Crete, Greece. [Wang, J.] Iowa State Univ, Dept Phys & Astron, Ames, IA 50011 USA. [Wang, J.] Iowa State Univ, Ames Lab US DOE, Ames, IA 50011 USA. RP Perakis, IE (reprint author), Univ Crete, Dept Phys, Iraklion 71003, Crete, Greece. FU European Union's Seventh Framework Programme [316165]; National Science Foundation [DMR-1055352]; Ames Laboratory's LDRD program; Iowa State University [#DE-AC02-07CH11358] FX This work was supported by the European Union's Seventh Framework Programme(FP7-REGPOT201220131)undergrantagreementNo.316165(theoretical/c omputationalstudies),by the National Science Foundation Contract No. DMR-1055352 (laserspectroscopy), and by the Ames Laboratory's LDRD program(materials synthesis and sample characterization).Ames Laboratory is operated for the U.S.DOE by Iowa State University under contract #DE-AC02-07CH11358. NR 20 TC 0 Z9 0 U1 0 U2 9 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9897-7 J9 PROC SPIE PY 2014 VL 8984 AR UNSP 898417 DI 10.1117/12.2034297 PG 8 WC Nanoscience & Nanotechnology; Optics; Physics, Applied SC Science & Technology - Other Topics; Optics; Physics GA BA2ZG UT WOS:000334021100023 ER PT J AU Li, F Bond-Lamberty, B Levis, S AF Li, F. Bond-Lamberty, B. Levis, S. TI Quantifying the role of fire in the Earth system - Part 2: Impact on the net carbon balance of global terrestrial ecosystems for the 20th century SO BIOGEOSCIENCES LA English DT Article ID CLIMATE-VEGETATION SYSTEM; BIOMASS BURNING EMISSIONS; COMMUNITY LAND MODEL; DYNAMIC VEGETATION; INTERANNUAL VARIABILITY; PONDEROSA PINE; WOOD-HARVEST; FOREST; BOREAL; ATMOSPHERE AB Fire is the primary form of terrestrial ecosystem disturbance on a global scale. It affects the net carbon balance of terrestrial ecosystems by emitting carbon directly and immediately into the atmosphere from biomass burning (the fire direct effect), and by changing net ecosystem productivity and land-use carbon loss in post-fire regions due to biomass burning and fire-induced vegetation mortality ( the fire indirect effect). Here, we provide the first quantitative assessment of the impact of fire on the net carbon balance of global terrestrial ecosystems during the 20th century, and investigate the roles of fire's direct and indirect effects. This is done by quantifying the difference between the 20th century fire-on and fire-off simulations with the NCAR Community Land Model CLM4.5 (prescribed vegetation cover and uncoupled from the atmospheric model) as a model platform. Results show that fire decreases the net carbon gain of global terrestrial ecosystems by 1.0 Pg Cyr(-1) averaged across the 20th century, as a result of the fire direct effect (1.9 Pg Cyr(-1)) partly offset by the indirect effect (-0.9 Pg Cyr(-1)). Post-fire regions generally experience decreased carbon gains, which is significant over tropical savannas and some North American and East Asian forests. This decrease is due to the direct effect usually exceeding the indirect effect, while they have similar spatial patterns and opposite sign. The effect of fire on the net carbon balance significantly declines until similar to 1970 with a trend of 8 Tg Cyr(-1) due to an increasing indirect effect, and increases subsequently with a trend of 18 Tg Cyr(-1) due to an increasing direct effect. These results help constrain the global-scale dynamics of fire and the terrestrial carbon cycle. C1 [Li, F.] Chinese Acad Sci, Inst Atmospher Phys, Int Ctr Climate & Environm Sci, Beijing, Peoples R China. [Bond-Lamberty, B.] Univ Maryland, Joint Global Change Res Inst, Pacific NW Natl Lab, College Pk, MD 20742 USA. [Levis, S.] Natl Ctr Atmospher Res, Climate & Global Dynam Div, Terr Sci Sect, Boulder, CO 80307 USA. RP Li, F (reprint author), Chinese Acad Sci, Inst Atmospher Phys, Int Ctr Climate & Environm Sci, Beijing, Peoples R China. EM lifang@mail.iap.ac.cn RI Bond-Lamberty, Ben/C-6058-2008 OI Bond-Lamberty, Ben/0000-0001-9525-4633 FU Strategic Priority Research Program of the Chinese Academy of Sciences [XDA05110201]; State Key Project for Basic Research Program of China (973) [2010CB951801]; National Natural Science Foundation [41005052]; National Science Foundation; DOE Office of Science Integrated Assessment Research Program; Earth System Modeling Program, as part of the integrated Earth System Modeling Project FX This study is co-supported by the Strategic Priority Research Program of the Chinese Academy of Sciences under grant no. XDA05110201, the State Key Project for Basic Research Program of China (973) under grant no. 2010CB951801, and the National Natural Science Foundation under grant no. 41005052. We are grateful to D. S. Ward from Cornell University, X.-D. Zeng and Z.-D. Lin from the Institute of Atmospheric Physics, Chinese Academy of Sciences, D. M. J. S. Bowman from the University of Tasmania, C. D. Koven from the Lawrence Berkeley National Lab, and K. Trenberth from the National Center for Atmospheric Research (NCAR) for helpful discussions. We thank L. Giglio from the NASA Goddard Space Flight, G. R. van der Werf from VU University, M. Jung and C. Roedenbeck from the Max Planck Institute for Biogeochemistry, M.-S. Zhao from the University of Montana, and F. Chevallier from the Laboratory of Sciences of the Climate and Environment (LSCE) for making their data available. We also thank the two anonymous reviewers for their valuable comments and suggestions, Editor S. Liu for handling this paper, and J. Xiao, S. Liu and P. Story for organizing the special issue. Computing resources were provided by the NCAR, which is sponsored by the National Science Foundation. B. Bond-Lamberty is funded by the DOE Office of Science Integrated Assessment Research Program and Earth System Modeling Program, as part of the integrated Earth System Modeling Project. NR 107 TC 18 Z9 21 U1 8 U2 56 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1726-4170 EI 1726-4189 J9 BIOGEOSCIENCES JI Biogeosciences PY 2014 VL 11 IS 5 BP 1345 EP 1360 DI 10.5194/bg-11-1345-2014 PG 16 WC Ecology; Geosciences, Multidisciplinary SC Environmental Sciences & Ecology; Geology GA AE6KI UT WOS:000334100700003 ER PT J AU Yang, X Thornton, PE Ricciuto, DM Post, WM AF Yang, X. Thornton, P. E. Ricciuto, D. M. Post, W. M. TI The role of phosphorus dynamics in tropical forests - a modeling study using CLM-CNP SO BIOGEOSCIENCES LA English DT Article ID CARBON-NITROGEN INTERACTIONS; N-P STOICHIOMETRY; TERRESTRIAL ECOSYSTEMS; HEDLEY FRACTIONATION; SOIL-PHOSPHORUS; NATURAL ECOSYSTEMS; AMAZONIAN FORESTS; GLOBAL PATTERNS; C-3 PLANTS; LAND-USE AB Tropical forests play a significant role in the global carbon cycle and global climate. However, tropical carbon cycling and the feedbacks from tropical ecosystems to the climate system remain critical uncertainties in the current generation of carbon-climate models. One of the major uncertainties comes from the lack of representation of phosphorus (P), currently believed to be the most limiting nutrient in tropical regions. Here we introduce P dynamics and C-N-P interactions into the CLM4-CN (Community Land Model version 4 with prognostic Carbon and Nitrogen) model and investigate the role of P cycling in controlling the productivity of tropical ecosystems. The newly developed CLM-CNP model includes all major biological and geochemical processes controlling P availability in soils and the interactions between C, N, and P cycles. Model simulations at sites along a Hawaiian soil chronosequence indicate that the introduction of P limitation greatly improved the model performance at the P-limited site. The model is also able to capture the shift in nutrient limitation along this chronosequence (from N limited to P limited), as shown in the comparison of model simulated plant responses to fertilization with the observed data. Model simulations at Amazonian forest sites show that CLM-CNP is capable of capturing the overall trend in NPP (net primary production) along the P availability gradient. This comparison also suggests a significant interaction between nutrient limitation and land use history. Model experiments under elevated atmospheric CO2 ([CO2]) conditions suggest that tropical forest responses to increasing [CO2] will interact strongly with changes in the P cycle. We highlight the importance of two feedback pathways (biochemical mineralization and desorption of secondary mineral P) that can significantly affect P availability and determine the extent of P limitation in tropical forests under elevated [CO2]. Field experiments with elevated CO2 are therefore needed to help quantify these important feedbacks. CO2 doubling model experiments show that tropical forest response to elevated [CO2] can only be predicted if the interactions between C cycle and nutrient dynamics are well understood and represented in models. Predictive modeling of C-nutrient interactions will have important implications for the prediction of future carbon uptake and storage in tropical ecosystems and global climate change. C1 [Yang, X.; Thornton, P. E.; Ricciuto, D. M.; Post, W. M.] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. RP Yang, X (reprint author), Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. EM yangx2@ornl.gov RI Thornton, Peter/B-9145-2012; Yang, Xiaojuan/I-3643-2016; Ricciuto, Daniel/I-3659-2016 OI Thornton, Peter/0000-0002-4759-5158; Yang, Xiaojuan/0000-0002-2686-745X; Ricciuto, Daniel/0000-0002-3668-3021 FU US Department of Energy, Office of Science, Biological and Environmental Research (BER) programs; US Department of Energy [DE-AC05-00OR22725] FX This research was sponsored by the US Department of Energy, Office of Science, Biological and Environmental Research (BER) programs and performed at Oak Ridge National Laboratory (ORNL). ORNL is managed by UT-Battelle, LLC, for the US Department of Energy under contract no. DE-AC05-00OR22725. We would like to thank Kirsten Thonicke, Sonke Zaehle and one anonymous reviewer for their constructive comments and suggestions. NR 61 TC 22 Z9 22 U1 5 U2 79 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1726-4170 EI 1726-4189 J9 BIOGEOSCIENCES JI Biogeosciences PY 2014 VL 11 IS 6 BP 1667 EP 1681 DI 10.5194/bg-11-1667-2014 PG 15 WC Ecology; Geosciences, Multidisciplinary SC Environmental Sciences & Ecology; Geology GA AE6KK UT WOS:000334100900014 ER PT J AU Yan, H Qian, Y Lin, G Leung, LR Yang, B Fu, Q AF Yan, H. Qian, Y. Lin, G. Leung, L. R. Yang, B. Fu, Q. TI Parametric sensitivity and calibration for the Kain-Fritsch convective parameterization scheme in the WRF model SO CLIMATE RESEARCH LA English DT Article DE Sensitivity; Convection scheme; Parameters; Calibration; Optimization; Regional climate model; WRF ID CLIMATE MODEL; UNCERTAINTY QUANTIFICATION; RADIATIVE-TRANSFER; SURFACE FLUXES; SOIL-MOISTURE; PART I; CLOUD; MESOSCALE; ENSEMBLE; VARIABILITY AB Convective parameterizations used in climate models display sensitivity to model resolution and variable skill in different climatic regimes. Although parameters in convective schemes can be calibrated using observations to reduce model errors, it is not clear if the optimal parameters calibrated based on regional data can robustly improve model skill across different model resolutions and climatic regimes. In this study, this issue is investigated using a regional modeling framework based on the Weather Research and Forecasting (WRF) model. To quantify the response and sensitivity of model performance to model parameters, we identified 5 key input parameters and specified their ranges in the Kain-Fritsch (KF) convection scheme in WRF, and calibrated them across different spatial resolutions, climatic regimes, and radiation schemes using observed precipitation data. Results show that the optimal values for 5 input parameters in the KF scheme are similar, and model sensitivity and error exhibit similar dependence on the input parameters for all experiments conducted in this study, despite differences in the precipitation climatology. We found that the model overall performances in simulating precipitation are relatively more sensitive to the coefficients of downdraft and entrainment mass flux, as well as to the starting height of downdraft. However, we found that rainfall biases-which are probably more related to structural errors-still exist over some regions in the simulation, even with the optimal para meters. This suggests that further studies are needed to identify the sources of uncertainties, as well as to reduce the model biases or structural errors, both of which are associated with missed or misrepresented physical processes and/or potential problems with the modeling. C1 [Yan, H.; Fu, Q.] Lanzhou Univ, Sch Atmospher Sci, Lanzhou 730000, Peoples R China. [Yan, H.; Qian, Y.; Lin, G.; Leung, L. R.] Pacific NW Natl Lab, Richland, WA 99354 USA. [Yang, B.] Nanjing Univ, Sch Atmospher Sci, Nanjing 210000, Jiangsu, Peoples R China. [Fu, Q.] Univ Washington, Dept Atmospher Sci, Seattle, WA 98105 USA. RP Qian, Y (reprint author), Pacific NW Natl Lab, Richland, WA 99354 USA. EM yun.qian@pnnl.gov RI qian, yun/E-1845-2011; Yan, Huiping/C-6847-2015; Yang, Ben/O-8548-2015 FU US Department of Energy (DOE) Office of Science's Advanced Scientific Computing Research program; Pacific Northwest National Laboratory [DE-AC05-76RL01830] FX This work was supported by the Applied Mathematics program of the US Department of Energy (DOE) Office of Science's Advanced Scientific Computing Research program. The computations were performed using resources of the National Energy Research Scientific Computing Center (NERSC) at Lawrence Berkeley National Laboratory (LBNL). Pacific Northwest National Laboratory is operated by Battelle for the DOE under Contract DE-AC05-76RL01830. NR 36 TC 6 Z9 6 U1 0 U2 10 PU INTER-RESEARCH PI OLDENDORF LUHE PA NORDBUNTE 23, D-21385 OLDENDORF LUHE, GERMANY SN 0936-577X EI 1616-1572 J9 CLIM RES JI Clim. Res. PY 2014 VL 59 IS 2 BP 135 EP 147 DI 10.3354/cr01213 PG 13 WC Environmental Sciences; Meteorology & Atmospheric Sciences SC Environmental Sciences & Ecology; Meteorology & Atmospheric Sciences GA AE4NE UT WOS:000333958300005 ER PT J AU Flynn, RW Lance, SL AF Flynn, R. W. Lance, S. L. TI Copper tolerance in the southern toad, Anaxyrus terrestris: a quantitative genetic approach SO INTEGRATIVE AND COMPARATIVE BIOLOGY LA English DT Meeting Abstract CT Annual Meeting of the Society-for-Integrative-and-Comparative-Biology CY JAN 03-07, 2014 CL Austin, TX SP Soc Integrat & Comparat Biol C1 Univ Georgia, Athens, GA 30602 USA. Savannah River Ecol Lab, Aiken, SC 29802 USA. EM wflynn@srel.uga.edu NR 0 TC 0 Z9 0 U1 1 U2 4 PU OXFORD UNIV PRESS INC PI CARY PA JOURNALS DEPT, 2001 EVANS RD, CARY, NC 27513 USA SN 1540-7063 EI 1557-7023 J9 INTEGR COMP BIOL JI Integr. Comp. Biol. PY 2014 VL 54 SU 1 BP E65 EP E65 PG 1 WC Zoology SC Zoology GA AD2FP UT WOS:000333049500261 ER PT J AU Love, CN Scott, DE Nunziata, SO Winzeler, ME Lance, SL AF Love, C. N. Scott, D. E. Nunziata, S. O. Winzeler, M. E. Lance, S. L. TI Prevalence of the amphibian disease chytridiomycosis in contaminated and uncontaminated wetlands on the Savannah River Site, South Carolina SO INTEGRATIVE AND COMPARATIVE BIOLOGY LA English DT Meeting Abstract CT Annual Meeting of the Society-for-Integrative-and-Comparative-Biology CY JAN 03-07, 2014 CL Austin, TX SP Soc Integrat & Comparat Biol C1 Univ Georgia, Savannah River Ecol Lab, Aiken, SC 29802 USA. Univ Kentucky, Dept Biol, Lexington, KY 40506 USA. EM love@srel.uga.edu NR 0 TC 0 Z9 0 U1 1 U2 1 PU OXFORD UNIV PRESS INC PI CARY PA JOURNALS DEPT, 2001 EVANS RD, CARY, NC 27513 USA SN 1540-7063 EI 1557-7023 J9 INTEGR COMP BIOL JI Integr. Comp. Biol. PY 2014 VL 54 SU 1 BP E127 EP E127 PG 1 WC Zoology SC Zoology GA AD2FP UT WOS:000333049501038 ER PT J AU Porter, ME Wainwright, DK Lowe, AT Halvorsen, MB Summers, AP AF Porter, M. E. Wainwright, D. K. Lowe, A. T. Halvorsen, M. B. Summers, A. P. TI Anisotropy in the skin and blubber of killer whales suggest no hydrostatic function SO INTEGRATIVE AND COMPARATIVE BIOLOGY LA English DT Meeting Abstract CT Annual Meeting of the Society-for-Integrative-and-Comparative-Biology CY JAN 03-07, 2014 CL Austin, TX SP Soc Integrat & Comparat Biol C1 Florida Atlantic Univ, Boca Raton, FL 33431 USA. Harvard Univ, Cambridge, MA 02138 USA. Univ Washington, Seattle, WA 98195 USA. Pacific NW Natl Lab, Richland, WA 99352 USA. Friday Harbor Labs, Friday Harbor, WA USA. EM me.porter@fau.edu NR 0 TC 0 Z9 0 U1 0 U2 0 PU OXFORD UNIV PRESS INC PI CARY PA JOURNALS DEPT, 2001 EVANS RD, CARY, NC 27513 USA SN 1540-7063 EI 1557-7023 J9 INTEGR COMP BIOL JI Integr. Comp. Biol. PY 2014 VL 54 SU 1 BP E167 EP E167 PG 1 WC Zoology SC Zoology GA AD2FP UT WOS:000333049501198 ER PT J AU Rumrill, CT Flynn, RW Scott, DE Lance, SL AF Rumrill, C. T. Flynn, R. W. Scott, D. E. Lance, S. L. TI Latent effects of multiple stressors on southern toads, Anaxyrus terrestris SO INTEGRATIVE AND COMPARATIVE BIOLOGY LA English DT Meeting Abstract CT Annual Meeting of the Society-for-Integrative-and-Comparative-Biology CY JAN 03-07, 2014 CL Austin, TX SP Soc Integrat & Comparat Biol C1 [Rumrill, C. T.; Flynn, R. W.; Scott, D. E.; Lance, S. L.] Univ Georgia, Savannah River Ecol Lab, Aiken, SC USA. EM rumrill@srel.uga.edu NR 0 TC 0 Z9 0 U1 1 U2 4 PU OXFORD UNIV PRESS INC PI CARY PA JOURNALS DEPT, 2001 EVANS RD, CARY, NC 27513 USA SN 1540-7063 EI 1557-7023 J9 INTEGR COMP BIOL JI Integr. Comp. Biol. PY 2014 VL 54 SU 1 BP E341 EP E341 PG 1 WC Zoology SC Zoology GA AD2FP UT WOS:000333049502428 ER PT J AU Tran, T Boughton, R Wilcoxen, T Fair, J Hofmeister, E Grindstaff, J Owen, J Fassbinder-Orth, C AF Tran, T. Boughton, R. Wilcoxen, T. Fair, J. Hofmeister, E. Grindstaff, J. Owen, J. Fassbinder-Orth, C. TI Expanding our toolbox in avian ecological immunology: effectiveness of a new anti-passerine IgY detecting antibody in wild birds SO INTEGRATIVE AND COMPARATIVE BIOLOGY LA English DT Meeting Abstract CT Annual Meeting of the Society-for-Integrative-and-Comparative-Biology CY JAN 03-07, 2014 CL Austin, TX SP Soc Integrat & Comparat Biol C1 Creighton Univ, Omaha, NE 68178 USA. Archbold Biol Stn, Venus, FL USA. Millikin Univ, Decatur, IL USA. Los Alamos Natl Lab, Los Alamos, NM 87545 USA. USGS Natl Wildlife Hlth Ctr, Madison, WI USA. Oklahoma State Univ, Stillwater, OK 74078 USA. Michigan State Univ, E Lansing, MI 48824 USA. EM carolfassbinder-orth@creighton.edu NR 0 TC 0 Z9 0 U1 2 U2 2 PU OXFORD UNIV PRESS INC PI CARY PA JOURNALS DEPT, 2001 EVANS RD, CARY, NC 27513 USA SN 1540-7063 EI 1557-7023 J9 INTEGR COMP BIOL JI Integr. Comp. Biol. PY 2014 VL 54 SU 1 BP E359 EP E359 PG 1 WC Zoology SC Zoology GA AD2FP UT WOS:000333049502498 ER PT J AU Winzeler, ME Lance, SL Love, CN Nunziata, SO Scott, DE AF Winzeler, M. E. Lance, S. L. Love, C. N. Nunziata, S. O. Scott, D. E. TI Prevalence of Ranavirus in Contaminated and Uncontaminated Sites on the Savannah River Site SO INTEGRATIVE AND COMPARATIVE BIOLOGY LA English DT Meeting Abstract CT Annual Meeting of the Society-for-Integrative-and-Comparative-Biology CY JAN 03-07, 2014 CL Austin, TX SP Soc Integrat & Comparat Biol C1 Univ Georgia, Savannah River Ecol Lab, Aiken, SC USA. Univ Kentucky, Dept Biol, Lexington, KY USA. EM meganwinzeler@gmail.com NR 0 TC 0 Z9 0 U1 1 U2 7 PU OXFORD UNIV PRESS INC PI CARY PA JOURNALS DEPT, 2001 EVANS RD, CARY, NC 27513 USA SN 1540-7063 EI 1557-7023 J9 INTEGR COMP BIOL JI Integr. Comp. Biol. PY 2014 VL 54 SU 1 BP E370 EP E370 PG 1 WC Zoology SC Zoology GA AD2FP UT WOS:000333049502543 ER PT S AU Ghasemkhani, M Albrecht, AR Melgaard, SD Seletskiy, DV Cederberg, JG Sheik-Bahae, M AF Ghasemkhani, Mohammadreza Albrecht, Alexander R. Melgaard, Seth D. Seletskiy, Denis V. Cederberg, Jeffrey G. Sheik-Bahae, Mansoor BE Epstein, RI Seletskiy, DV SheikBahae, M TI Intracavity optical refrigeration to 131 K using high-power vertical external-cavity surface-emitting lasers (VECSELs) SO LASER REFRIGERATION OF SOLIDS VII SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Laser Refrigeration of Solids VII CY FEB 05-06, 2014 CL San Francisco, CA SP SPIE DE Anti-Stokes fluorescence; laser cooling of solids; vertical external-cavity surface-emitting lasers; birefringent filter AB Laser cooling of Yb:YLF crystal to 131 K from room temperature has been demonstrated in an active intracavity arrangement for enhanced pump absorption. The laser is a high-power, broadly-tunable InGaAs/GaAs MQW VECSEL capable of producing 20 Watts at 1020 nm, directly at the E4-E5 transition of the Yb-ion. This is the coldest temperature achieved to date in an intracavity geometry and without sophisticated heat load management of the crystal. This progress presents a significant advancement towards an all-solid-state compact cryocooler. C1 [Ghasemkhani, Mohammadreza; Albrecht, Alexander R.; Melgaard, Seth D.; Seletskiy, Denis V.; Sheik-Bahae, Mansoor] Univ New Mexico, Dept Phys & Astron, 1919 Lomas Blvd NE MSC 07-4220, Albuquerque, NM 87131 USA. [Melgaard, Seth D.] Air Force Res Lab, Kirtland AFB, NM USA. [Cederberg, Jeffrey G.] Sandia Natl Labs, POB 5800, Albuquerque, NM 87185 USA. [Seletskiy, Denis V.] Univ Konstanz, Ctr Appl Photon, Dept Phys, Constance, Germany. RP Ghasemkhani, M (reprint author), Univ New Mexico, Dept Phys & Astron, 1919 Lomas Blvd NE MSC 07-4220, Albuquerque, NM 87131 USA. EM mrghasem@unm.edu FU DARPA [10669320]; Thermo Dynamic Films (TDF) through an STTR; AFRL [FA94531310223]; National Research Council Research Associateship Award at the Air Force Research Laboratory; National Science Foundation [1160764]; EU FP7 Marie Curie Zukunftskolleg Incoming Fellowship Programme; University of Konstanz [291784]; Sandia's Laboratory Directed Research and Development Office; U. S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX The authors thank Richard Epstein and Markus Hehlen for useful discussions, and AC Materials (Tarpon Springs, FL) for customized sample growth and preparation. The work at UNM was supported by DARPA (GRANT 10669320), Thermo Dynamic Films (TDF) through an STTR Grant, AFRL (FA94531310223). SDM acknowledges the support of a National Research Council Research Associateship Award at the Air Force Research Laboratory. DVS acknowledges support by the National Science Foundation under Grant No. 1160764 and partial support by the EU FP7 Marie Curie Zukunftskolleg Incoming Fellowship Programme, University of Konstanz (Grant No. 291784). VECSEL growth was supported by Sandia's Laboratory Directed Research and Development Office. 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 15 TC 1 Z9 1 U1 3 U2 5 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9913-4 J9 PROC SPIE PY 2014 VL 9000 AR UNSP 900005 DI 10.1117/12.2040116 PG 7 WC Optics; Physics, Applied SC Optics; Physics GA BA2ZR UT WOS:000334025900004 ER PT S AU Hehlen, MP Boncher, WL Melgaard, SD Blair, MW Jackson, RA Littleford, TE Love, SP AF Hehlen, Markus P. Boncher, William L. Melgaard, Seth D. Blair, Michael W. Jackson, Robert A. Littleford, Thomas E. Love, Steven P. BE Epstein, RI Seletskiy, DV SheikBahae, M TI Preparation of high-purity LiF, YF3, and YbF3 for laser refrigeration SO LASER REFRIGERATION OF SOLIDS VII SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Laser Refrigeration of Solids VII CY FEB 05-06, 2014 CL San Francisco, CA SP SPIE DE Solid-state optical refrigeration; ytterbium doped fluoride crystals; lattice defect modeling; EPR spectroscopy; chelate-assisted solvent extraction purification ID SIMULATION; SOLIDS AB The role of transition-metal impurities in Yb3+-doped YLiF4 (YLF) laser-cooling crystals is studied. Divalent 3d transition-metal ions, in particular Fe2+, are found to have strong absorptions at the laser cooling pump wavelength and degrade the cooling efficiency by introducing background absorption. A set of eight substitutional and charge-compensated defects that form upon introduction of 1+, 2+, and 3+ transition-metal ions into the YLF crystal lattice is proposed. A calculation of solution energies for each defect type and for a range of 3d ions is carried out. It indicates that divalent 3d ions preferentially substitute for Y3+ accompanied by a fluoride vacancy for charge compensation. An electron paramagnetic resonance (EPR) study of a YLF crystal identifies Fe2+ in the crystal lattice, in agreement with the elemental analysis and the computational results. A strategy for purifying the YF3, LiF, and YbF3 starting materials for the YLF:Yb crystal growth is discussed. Chelate-assisted solvent extraction purification with pyrrolidine dithiocarbamate (APDC) for Y, Li, and Yb as well as ethylenediaminetetraacetic acid (EDTA) for Li was carried out. C1 [Hehlen, Markus P.; Boncher, William L.; Blair, Michael W.; Love, Steven P.] Los Alamos Natl Lab, Mailstop E546, Los Alamos, NM 87545 USA. [Melgaard, Seth D.] BAir Force Res Lab, Kirtland AFB, Albuquerque, NM USA. [Jackson, Robert A.; Littleford, Thomas E.] Keele Univ, Keele UK ST5 5BG, Staffs, England. RP Hehlen, MP (reprint author), Los Alamos Natl Lab, Mailstop E546, Los Alamos, NM 87545 USA. EM hehlen@lanl.gov OI Boncher, William/0000-0001-9155-5527; Love, Steven/0000-0003-0588-9622 FU LANL/LDRD [20140275ER]; National Research Council Research Associateship Award at the Air Force Research Laboratory FX This work was carried out under the auspices of the National Nuclear Security Administration of the Department of Energy ( DOE) at Los Alamos National Laboratory and supported by the LANL/LDRD program (20140275ER). SDM acknowledges the support of a National Research Council Research Associateship Award at the Air Force Research Laboratory. NR 23 TC 0 Z9 0 U1 2 U2 14 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9913-4 J9 PROC SPIE PY 2014 VL 9000 AR UNSP 900004 DI 10.1117/12.2039547 PG 11 WC Optics; Physics, Applied SC Optics; Physics GA BA2ZR UT WOS:000334025900003 ER PT S AU Kao, TY Cai, XW Hu, Q Reno, JL AF Kao, Tsung-Yu Cai, Xiaowei Hu, Qing Reno, John L. BE Razeghi, M Tournie, E Brown, GJ TI Microstrip Antenna Coupled Distributed Feedback Terahertz Quantum-Cascade Lasers SO QUANTUM SENSING AND NANOPHOTONIC DEVICES XI SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Quantum Sensing and Nanophotonic Devices XI CY FEB 02-06, 2014 CL San Francisco, CA SP SPIE DE Terahertz; Quantum Cascade Laser; DFB; Microwave Engineering; Integrated Antenna; Microstrip Transmission Line; Linear Antenna Array AB By introducing coupled microstrip antennas on THz Distributed Feedback (DFB) Quantum Cascade Lasers (QCLs), the radiation efficiency of each feedback aperture is greatly enhanced. Single mode emission similar to 3 THz from a 31-period antenna-coupled third-order DFB laser yields similar to 4 times improvement in output power comparing with a corrugated third-order device fabricated on the same gain medium. This 31-period device has similar to 15x25 degrees beam divergence and 4 mW pulsed power (4%) at 10 K with maximum lasing temperature (T-max) at 134 K (pulsed). When phase matching condition is met, emissions from 81 apertures (4-mm long) are coherently combined to form a narrow beam with 12.5 degrees divergence. Further experiment demonstrated the new device at 4 THz (25-period, similar to 18 mu mx1-mm long. The 4 THz device reaches >8 mW pulsed power (10%) at 12 K with T-max 109 K (pulsed) and >77 K (cw). The slope efficiency is 450 mW/A with 0.57% wall-plug. It is worth pointing out although the antennas would be excited differently, similar enhancement in out-coupling efficiency can also be observed in second-order surface-emitting THz DFB lasers. Begin the abstract two lines below author names and addresses. C1 [Kao, Tsung-Yu; Cai, Xiaowei; Hu, Qing] MIT, Dept Elect Engn & Comp Sci, Cambridge, MA 02139 USA. [Reno, John L.] Sandia Natl Labs, Ctr Integrated Nanotechnol, Albuquerque, NM 87185 USA. RP Kao, TY (reprint author), MIT, Dept Elect Engn & Comp Sci, Cambridge, MA 02139 USA. EM wilt_kao@mit.edu FU NASA; NSF; U. S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX This work is supported by NASA and NSF, and also performed at the Center for Integrated Nanotechnologies, a U. S. Department of Energy, Office of Basic Energy Sciences user facility. Sandia National Laboratories is a multi- program laboratory 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 6 TC 0 Z9 0 U1 0 U2 6 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9906-6 J9 PROC SPIE PY 2014 VL 8993 AR UNSP 89930E DI 10.1117/12.2036604 PG 9 WC Engineering, Electrical & Electronic; Optics; Physics, Applied SC Engineering; Optics; Physics GA BA2ZQ UT WOS:000334025500009 ER PT S AU Kelly, JF Sams, RL Blake, TA Kriesel, JM AF Kelly, J. F. Sams, R. L. Blake, T. A. Kriesel, J. M. BE Razeghi, M Tournie, E Brown, GJ TI Further developments of capillary absorption spectrometers using small hollow-waveguide fibers SO QUANTUM SENSING AND NANOPHOTONIC DEVICES XI SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Quantum Sensing and Nanophotonic Devices XI CY FEB 02-06, 2014 CL San Francisco, CA SP SPIE DE mid-infrared (IR); hollow-waveguides; quantum cascade (QC) lasers; FM spectroscopy; tunable laser; absorption spectroscopy; Liouville's Theorem ID QUANTUM CASCADE LASERS; SPECTROSCOPY; DOPPLER AB Our objective is to enhance quantification of stable carbon and oxygen isotope ratios to better than 1 parts per thousand relative isotope precision for sample sizes < 1 pico-mole. A newer variant Capillary Absorption Spectrometer (CAS) is described using a proprietary linear-taper hollow waveguide in conjunction with wavelength and frequency modulation techniques of tunable laser absorption spectrometry. Previous work used circular capillaries with uniform 1 mm ID to measure C-13/C-12 ratios with >= 20 pico-mole samples to <= 10 ppm (1 parts per thousand precision against standards) [1]. While performing fairly well, it generated residual modal noise due to multipath propagation in the hollow-waveguides (HWGs). This system has been used with laser ablation-catalytic combustion techniques to analyze small resolution (similar to 25 mu m spot diameter) laser ablation events on solids. Using smaller ID capillary waveguides could improve detection limits and spatial resolutions. Reducing an IR-compatible hollow waveguide's inner diameter (ID) to < 300 mu m decreases modal noise significantly for mid-IR operation, but feedback noise with high gain semiconductor lasers can become problematic. A proprietary linear-taper small waveguide (mean ID = 0.35 mm, L = 1 m) was tested to understand whether modal noise and optical feedback effects could be simultaneously reduced. We see better mode filtering and, significant reductions of feedback noise under favorable coupling of a multi-spatial mode QC laser to the smaller ID of the linear-tapered HWG. We demonstrate that better modal coupling operation is consistent with Liouville's theorem, where greater suppression of feedback from spurious scatter within the HWG occurs by injecting the laser into the smaller ID port. Our progress on developing lighter-weight, potentially fieldable alternatives to Isotope Ratio Mass Spectrometers (IRMS) with a small volume (<= 0.1 cm(3)) CAS system will be discussed and compared to other competitive systems. C1 [Kelly, J. F.; Sams, R. L.; Blake, T. A.] Pacific NW Natl Lab, POB 999, Richland, WA 99352 USA. [Kriesel, J. M.] Opto Knowledge Syst Inc, Torrance, CA 90502 USA. RP Kelly, JF (reprint author), Pacific NW Natl Lab, POB 999, Richland, WA 99352 USA. EM jfk@pnnl.gov; ta.blake@pnnl.gov RI Razeghi, Manijeh/B-7265-2009 FU U. S. Department of Energy, using Laboratory Directed R D ( LDRD); Pacific Northwest National Laboratory; U. S. Department of Energy by Battelle Memorial Institute [DE-AC05-76RL01830] FX This work was supported by the U. S. Department of Energy, using Laboratory Directed R& D ( LDRD) funding. The authors would like to thank Drs ML Alexander, H Kruezer, and JJ Moran for their support through LDRD funding for the continued work discussed herein. Pacific Northwest National Laboratory is operated for the U. S. Department of Energy by Battelle Memorial Institute under Contract No. DE-AC05-76RL01830. NR 22 TC 0 Z9 0 U1 1 U2 3 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9906-6 J9 PROC SPIE PY 2014 VL 8993 AR UNSP 89931O DI 10.1117/12.2042734 PG 16 WC Engineering, Electrical & Electronic; Optics; Physics, Applied SC Engineering; Optics; Physics GA BA2ZQ UT WOS:000334025500034 ER PT S AU Macfaden, AJ Reno, JL Brener, I Mitrofanov, O AF Macfaden, Alexander J. Reno, John L. Brener, Igal Mitrofanov, Oleg BE Razeghi, M Tournie, E Brown, GJ TI Terahertz near-field probe incorporating lambda/100 aperture for time-domain spectroscopy and imaging SO QUANTUM SENSING AND NANOPHOTONIC DEVICES XI SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Quantum Sensing and Nanophotonic Devices XI CY FEB 02-06, 2014 CL San Francisco, CA SP SPIE DE terahertz; near-field; time-domain spectroscopy; photonic nanostructure; FDTD ID DIFFRACTION; MICROSCOPE; PULSES AB Achieving high spatial resolutions for imaging with terahertz (THz) waves requires near-field probes, such as a sub-wavelength aperture probe. Bethe's theory of transmission through a sub-wavelength aperture of size a predicts that the transmitted electric field scales as E alpha a(3). This strong dependence limits the size of apertures that can be employed and hence the spatial resolution. This dependence however changes for the evanescent field components in very close proximity (similar to 1 mu m for THz waves) to the aperture, as shown by electromagnetic simulations. To exploit this effect in a THz near-field probe, we developed a photoconductive THz near-field detector structure, which incorporates a thinned photo-conductive detector region and a distributed Bragg reflector between the detector and the aperture plane. Near-field probes are manufactured with different aperture sizes to investigate transmission of THz pulses through apertures as small as 3 mu m. The experimental results confirm that the transmitted field amplitude, and therefore the sensitivity, increases by about one order of magnitude for the new probes. A 3 mu m aperture probe with a spatial resolution of lambda/100 at 1THz is demonstrated. C1 [Macfaden, Alexander J.; Mitrofanov, Oleg] UCL, Dept Elect & Elect Engn, London WC1E 7JE, England. [Reno, John L.; Brener, Igal; Mitrofanov, Oleg] Sandia Natl Labs, Ctr Integrated Nanotechnol, Albuquerque, NM 87185 USA. [Reno, John L.; Brener, Igal] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Macfaden, AJ (reprint author), UCL, Dept Elect & Elect Engn, London WC1E 7JE, England. EM o.mitrofanov@ucl.ac.uk RI Mitrofanov, Oleg/C-1938-2008 OI Mitrofanov, Oleg/0000-0003-3510-2675 FU Royal Society [UF080745]; Center for Integrated Nanotechnologies; Office of Science User Facility; U. S. Department of Energy ( DOE) Office of Science; Sandia National Laboratories; Sandia Corporation; Lockheed Martin Corporation; U. S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX We would like to thank Prof. Paul Planken for useful discussions of wave transmission through small apertures and gratefully acknowledge the support of the Royal Society [Grant No. UF080745]. 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. 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 16 TC 0 Z9 0 U1 0 U2 10 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9906-6 J9 PROC SPIE PY 2014 VL 8993 AR UNSP 89931D DI 10.1117/12.2039364 PG 7 WC Engineering, Electrical & Electronic; Optics; Physics, Applied SC Engineering; Optics; Physics GA BA2ZQ UT WOS:000334025500030 ER PT S AU Mitrofanov, O Yu, WL Thompson, RJ Jiang, YX Brener, I Pan, W Berger, C de Heer, WA Jiang, ZG AF Mitrofanov, Oleg Yu, Wenlong Thompson, Robert J. Jiang, Yuxuan Brener, Igal Pan, Wei Berger, Claire de Heer, Walter A. Jiang, Zhigang BE Razeghi, M Tournie, E Brown, GJ TI THz near-field microscopy of graphene structures SO QUANTUM SENSING AND NANOPHOTONIC DEVICES XI SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Quantum Sensing and Nanophotonic Devices XI CY FEB 02-06, 2014 CL San Francisco, CA SP SPIE DE graphene; terahertz; near-field microscopy; plasmons; surface waves; time-domain spectroscopy; ribbon; array AB Properties of graphene can be tuned electrically and chemically, providing a promising system for application in terahertz (THz) devices. Graphene response can be enhanced even further by means of coupling electromagnetic waves into plasmon modes, frequency of which is controlled by geometrical parameters. To probe excitation of confined plasmon modes and surface wave excitation, epitaxial graphene and its structures are investigated using THz near-field microscopy. Detected near-field images suggest excitation of THz surface waves occurring at graphene edges, similar to that observed at metallic edges, and excitation of confined plasmon modes. We will also discuss the impact of graphene inhomogeneity on local THz transmission properties on the sub-wavelength scale. C1 [Mitrofanov, Oleg; Thompson, Robert J.] UCL, London WC1E 7JE, England. [Mitrofanov, Oleg; Brener, Igal] Sandia Natl Labs, Ctr Integrated Nanotechnol, Albuquerque, NM 87185 USA. [Jiang, Yuxuan; Berger, Claire; de Heer, Walter A.; Jiang, Zhigang] Georgia Inst Technol, Sch Phys, Atlanta, GA 30332 USA. [Brener, Igal; Pan, Wei] Sandia Natl Labs, POB 5800, Albuquerque, NM 87185 USA. [Brener, Igal; Pan, Wei] CNRS, F-38042 Grenoble, France. RP Mitrofanov, O (reprint author), UCL, London WC1E 7JE, England. RI Mitrofanov, Oleg/C-1938-2008 OI Mitrofanov, Oleg/0000-0003-3510-2675 FU Royal Society [UF080745]; UCL and at the Center for Integrated Nanotechnologies; Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science by SNL [DE-AC04-94AL85000]; NSF [DMR-0820382]; DOE Office of Basic Energy Sciences (BES) through a contract with SNL; LDRD FX This work is supported by the Royal Society [grant number UF080745] and performed at UCL and at the Center for Integrated Nanotechnologies, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science by SNL [contract DE-AC04-94AL85000]. Epitaxial graphene growth and device fabrication are carried out at GaTech, supported by the NSF [DMR-0820382] and the DOE Office of Basic Energy Sciences (BES) through a contract with SNL. The work at SNL is supported by LDRD NR 7 TC 0 Z9 0 U1 2 U2 12 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9906-6 J9 PROC SPIE PY 2014 VL 8993 AR UNSP 89932A DI 10.1117/12.2041790 PG 6 WC Engineering, Electrical & Electronic; Optics; Physics, Applied SC Engineering; Optics; Physics GA BA2ZQ UT WOS:000334025500045 ER PT S AU Perkins, JJ Newell, RT Schabacker, CR Richardson, C AF Perkins, Jeffrey J. Newell, Raymond T. Schabacker, Charles R. Richardson, Craig BE Razeghi, M Tournie, E Brown, GJ TI Novel fiber-optic geometries for fast quantum communication SO QUANTUM SENSING AND NANOPHOTONIC DEVICES XI SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Quantum Sensing and Nanophotonic Devices XI CY FEB 02-06, 2014 CL San Francisco, CA SP SPIE ID ORBITAL ANGULAR-MOMENTUM; GAUSSIAN LASER MODES; OPTICAL-FIBERS; POYNTING VECTOR; POWER TRANSFER; LIGHT-BEAMS C1 [Perkins, Jeffrey J.; Schabacker, Charles R.; Richardson, Craig] Fiberguide Ind, 3409 E Linden St, Caldwell, ID 83605 USA. [Newell, Raymond T.] Los Alamos Natl Lab, Los Alamos, NM USA. RP Perkins, JJ (reprint author), Fiberguide Ind, 3409 E Linden St, Caldwell, ID 83605 USA. NR 37 TC 0 Z9 0 U1 0 U2 5 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9906-6 J9 PROC SPIE PY 2014 VL 8993 AR UNSP 89930J DI 10.1117/12.2039917 PG 10 WC Engineering, Electrical & Electronic; Optics; Physics, Applied SC Engineering; Optics; Physics GA BA2ZQ UT WOS:000334025500012 ER PT S AU Yang, RQ Lotfi, H Li, L Hinkey, RT Ye, H Klem, JF Lei, L Mishima, TD Keay, JC Santos, MB Johnson, MB AF Yang, Rui Q. Lotfi, Hossein Li, Lu Hinkey, Robert T. Ye, Hao Klem, J. F. Lei, L. Mishima, T. D. Keay, J. C. Santos, M. B. Johnson, M. B. BE Razeghi, M Tournie, E Brown, GJ TI Quantum-Engineered Interband Cascade Photovoltaic Devices SO QUANTUM SENSING AND NANOPHOTONIC DEVICES XI SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Quantum Sensing and Nanophotonic Devices XI CY FEB 02-06, 2014 CL San Francisco, CA SP SPIE DE photovoltaics; semiconductors; quantum wells; type-II heterostructures ID THERMOPHOTOVOLTAIC DEVICES; EFFICIENCY; TEMPERATURE; CONVERSION; LASERS; LIMIT AB Quantum-engineered multiple stage photovoltaic (PV) devices are explored based on InAs/GaSb/AlSb interband cascade (IC) structures. These ICPV devices employ multiple discrete absorbers that are connected in series by wide-bandgap unipolar barriers using type-II heterostructure interfaces for facilitating carrier transport between cascade stages similar to IC lasers. The discrete architecture is beneficial for improving the collection efficiency and for spectral splitting by utilizing absorbers with different bandgaps. As such, the photo-voltages from each individual cascade stage in an ICPV device add together, creating a high overall open-circuit voltage, similar to conventional multi-junction tandem solar cells. Furthermore, photo-generated carriers can be collected with nearly 100% efficiency in each stage. This is because the carriers travel over only a single cascade stage, designed to be shorter than a typical diffusion length. The approach is of significant importance for operation at high temperatures where the diffusion length is reduced. Here, we will present our recent progress in the study of ICPV devices, which includes the demonstration of ICPV devices at room temperature and above with narrow bandgaps (e.g. 0.23 eV) and high open-circuit voltages. C1 [Yang, Rui Q.; Lotfi, Hossein; Li, Lu; Hinkey, Robert T.; Ye, Hao] Univ Oklahoma, Sch Elect & Comp Engn, Norman, OK 73019 USA. [Klem, J. F.] Sandia Natl Labs, Albuquerque, NM 87185 USA. [Lei, L.; Mishima, T. D.; Keay, J. C.; Santos, M. B.; Johnson, M. B.] Univ Oklahoma, Dept Phys & Astron, Norman, OK 73019 USA. RP Yang, RQ (reprint author), Univ Oklahoma, Sch Elect & Comp Engn, Norman, OK 73019 USA. FU DoE EPSCoR program [DE-SC0004523]; C-SPIN; Oklahoma/Arkansas MRSEC [DMR- 0520550]; U. S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX We are grateful to Yuchao Jiang, Lihua Zhao, Chao Niu, and Ernest S. Sanchez for technical assistance. This work was supported in part by the DoE EPSCoR program (Award No. DE-SC0004523) and by C-SPIN, the Oklahoma/Arkansas MRSEC (DMR- 0520550). 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 28 TC 2 Z9 2 U1 3 U2 8 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9906-6 J9 PROC SPIE PY 2014 VL 8993 AR UNSP 899310 DI 10.1117/12.2040746 PG 10 WC Engineering, Electrical & Electronic; Optics; Physics, Applied SC Engineering; Optics; Physics GA BA2ZQ UT WOS:000334025500022 ER PT J AU Cihan, A Birkholzer, J Illangasekare, TH Zhou, QL AF Cihan, Abdullah Birkholzer, Jens Illangasekare, Tissa H. Zhou, Quanlin TI A modeling approach to represent hysteresis in capillary pressuresaturation relationship based on fluid connectivity in void space SO WATER RESOURCES RESEARCH LA English DT Article DE hysteresis; capillary pressure; saturation; capillary trapping; residual saturation ID SOIL HYDRAULIC-PROPERTIES; PREFRACTAL POROUS-MEDIA; RELATIVE PERMEABILITY; SIMILARITY HYPOTHESIS; INVASION PERCOLATION; WATER HYSTERESIS; BEREA SANDSTONE; DOMAIN THEORY; PORE WATER; FLOW AB This study presents a new model for description of hysteretic constitutive relationships between capillary pressure and saturation under capillary-dominated multiphase flow conditions in porous media. Hysteretic relationships are required for accurate prediction of spatial and temporal distribution of multiphase fluids in response to successively occurring drainage and imbibition events in porous media. In addition to contact angle effects, connectivity of the void space in the porous medium plays a central role for the macroscopic manifestation of hysteresis behavior and capillary entrapment of wetting and nonwetting fluids. The hysteretic constitutive model developed in this work uses void-size distribution and a measure of connectivity for void space to compute the hysteretic curves and to predict entrapped fluid-phase saturations. Two functions, the drainage connectivity function and the wetting connectivity function, are introduced to characterize connectivity of fluids in void space during drainage and wetting processes. These functions can be estimated through pore-scale simulations in computer-generated porous media or from traditional experimental measurements of primary drainage and main wetting curves. The hysteresis model results are verified by comparing the model predicted scanning curves with 3-D pore-scale simulations as well as with actual data sets obtained from column experiments found in the literature. C1 [Cihan, Abdullah; Birkholzer, Jens; Zhou, Quanlin] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, Berkeley, CA 94720 USA. [Illangasekare, Tissa H.] Colorado Sch Mines, Ctr Expt Study Subsurface Environm Proc, Golden, CO 80401 USA. RP Cihan, A (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, One Cyclotron Rd,Mail Stop 74R316C, Berkeley, CA 94720 USA. EM acihan@lbl.gov RI Zhou, Quanlin/B-2455-2009; Birkholzer, Jens/C-6783-2011; Cihan, Abdullah/D-3704-2015 OI Zhou, Quanlin/0000-0001-6780-7536; Birkholzer, Jens/0000-0002-7989-1912; FU National Energy Technology Laboratory, National Risk Assessment Partnership of the US Department of Energy at Lawrence Berkeley National Laboratory, under U.S. Department of Energy [DE-AC02-05CH11231]; Office of Sequestration, Hydrogen, and Clean Coal Fuels, through the National Energy Technology Laboratory, under the U.S. Department of Energy [FE0004630]; National Science Foundation/EAR [1045282] FX The authors wish to thank three anonymous reviewers, as well as Tetsu K. Tokunaga of Lawrence Berkeley National Laboratory (LBNL), for their careful review of the manuscript and the suggestion of improvements. This work was funded by the Assistant Secretary for Fossil Energy, National Energy Technology Laboratory, National Risk Assessment Partnership of the US Department of Energy at Lawrence Berkeley National Laboratory, under U.S. Department of Energy contract DE-AC02-05CH11231. Supplementary funding was provided by the Assistant Secretary for Fossil Energy, Office of Sequestration, Hydrogen, and Clean Coal Fuels, through the National Energy Technology Laboratory, under the U.S. Department of Energy contract FE0004630. This work was in part based upon work supported by the National Science Foundation/EAR under award 1045282. NR 45 TC 7 Z9 7 U1 0 U2 18 PU AMER GEOPHYSICAL UNION PI WASHINGTON PA 2000 FLORIDA AVE NW, WASHINGTON, DC 20009 USA SN 0043-1397 EI 1944-7973 J9 WATER RESOUR RES JI Water Resour. Res. PD JAN PY 2014 VL 50 IS 1 BP 119 EP 131 DI 10.1002/2013WR014280 PG 13 WC Environmental Sciences; Limnology; Water Resources SC Environmental Sciences & Ecology; Marine & Freshwater Biology; Water Resources GA AB4ZN UT WOS:000331798800009 ER PT J AU Liu, XY Zhou, QL Kitanidis, PK Birkholzer, JT AF Liu, Xiaoyi Zhou, Quanlin Kitanidis, Peter K. Birkholzer, Jens T. TI Fast iterative implementation of large-scale nonlinear geostatistical inverse modeling SO WATER RESOURCES RESEARCH LA English DT Article DE geostatistical inverse modeling; Krylov subspace methods; large-scale inversion; MINRES ID STEADY-STATE; HYDRAULIC TOMOGRAPHY; TRANSMISSIVITY; MOMENTS; FIELDS; HEAD AB In nonlinear geostatistical inverse problems, it often takes a significant amount of computational cost to form linear geostatistical inversion systems by linearizing the forward model. More specifically, the storage cost associated with the sensitivity matrix H (m x n, where m and n are the numbers of measurements and unknowns, respectively) is high, especially when both m and n are large in for instance, 3-D tomography problems. In this research, instead of explicitly forming and directly solving the linear geostatistical inversion system, we use MINRES, a Krylov subspace method, to solve it iteratively. During each iteration in MINRES, we only compute the products Hx and H(T)x for any appropriately sized vectors x, for which we solve the forward problem twice. As a result, we reduce the memory requirement from O(mn) to O(m)+O(n). This iterative methodology is combined with the Bayesian inverse method in Kitanidis (1996) to solve large-scale inversion problems. The computational advantages of our methodology are demonstrated using a large-scale 3-D numerical hydraulic tomography problem with transient pressure measurements (250,000 unknowns and approximate to 100,000 measurements). In this case, approximate to 200 GB of memory would otherwise be required to fully compute and store the sensitivity matrix H at each Newton step during optimization. The CPU cost can also be significantly reduced in terms of the total number of forward simulations. In the end, we discuss potential extension of the methodology to other geostatistical methods such as the Successive Linear Estimator. C1 [Liu, Xiaoyi; Zhou, Quanlin; Birkholzer, Jens T.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, Berkeley, CA 94720 USA. [Kitanidis, Peter K.] Stanford Univ, Dept Civil & Environm Engn, Stanford, CA 94305 USA. RP Liu, XY (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, One Cyclotron Rd, Berkeley, CA 94720 USA. EM XiaoyiLiu@lbl.gov RI Zhou, Quanlin/B-2455-2009; Birkholzer, Jens/C-6783-2011 OI Zhou, Quanlin/0000-0001-6780-7536; Birkholzer, Jens/0000-0002-7989-1912 FU Office of Sequestration, Hydrogen, and Clean Coal Fuels, National Energy Technology Laboratory, of the U.S. Department of Energy [DE-AC02-05CH11231]; Earth Sciences Division of Lawrence Berkeley National Laboratory through Early Career Development Grants FX This work was funded by the Assistant Secretary for Fossil Energy, Office of Sequestration, Hydrogen, and Clean Coal Fuels, National Energy Technology Laboratory, of the U.S. Department of Energy under contract DE-AC02-05CH11231. Additional funding was provided by the Earth Sciences Division of Lawrence Berkeley National Laboratory through Early Career Development Grants. We also thank Michael Cardiff, Dmitry B. Avdeev, and the other anonymous reviewer for their valuable comments and suggestions. NR 24 TC 6 Z9 6 U1 0 U2 11 PU AMER GEOPHYSICAL UNION PI WASHINGTON PA 2000 FLORIDA AVE NW, WASHINGTON, DC 20009 USA SN 0043-1397 EI 1944-7973 J9 WATER RESOUR RES JI Water Resour. Res. PD JAN PY 2014 VL 50 IS 1 BP 198 EP 207 DI 10.1002/2012WR013241 PG 10 WC Environmental Sciences; Limnology; Water Resources SC Environmental Sciences & Ecology; Marine & Freshwater Biology; Water Resources GA AB4ZN UT WOS:000331798800014 ER PT J AU Hammond, GE Lichtner, PC Mills, RT AF Hammond, G. E. Lichtner, P. C. Mills, R. T. TI Evaluating the performance of parallel subsurface simulators: An illustrative example with PFLOTRAN SO WATER RESOURCES RESEARCH LA English DT Article DE high performance computing; biogeochemical transport; groundwater flow ID VARIABLY SATURATED FLOW; FREE NEWTON-KRYLOV; HANFORD 300 AREA; REACTIVE TRANSPORT; MIGRATION; PRECONDITIONERS; MEDIA; MODEL AB To better inform the subsurface scientist on the expected performance of parallel simulators, this work investigates performance of the reactive multiphase flow and multicomponent biogeochemical transport code PFLOTRAN as it is applied to several realistic modeling scenarios run on the Jaguar supercomputer. After a brief introduction to the code's parallel layout and code design, PFLOTRAN's parallel performance (measured through strong and weak scalability analyses) is evaluated in the context of conceptual model layout, software and algorithmic design, and known hardware limitations. PFLOTRAN scales well (with regard to strong scaling) for three realistic problem scenarios: (1) in situ leaching of copper from a mineral ore deposit within a 5-spot flow regime, (2) transient flow and solute transport within a regional doublet, and (3) a real-world problem involving uranium surface complexation within a heterogeneous and extremely dynamic variably saturated flow field. Weak scalability is discussed in detail for the regional doublet problem, and several difficulties with its interpretation are noted. C1 [Hammond, G. E.] Sandia Natl Labs, Albuquerque, NM 87185 USA. [Lichtner, P. C.] OFM Res, Santa Fe, NM USA. [Mills, R. T.] Oak Ridge Natl Lab, Div Environm Sci, Oak Ridge, TN 37831 USA. [Mills, R. T.] Univ Tennessee, Elect Engn & Comp Sci Dept, Knoxville, TN USA. [Mills, R. T.] Univ Tennessee, Earth & Planetary Sci Dept, Knoxville, TN USA. RP Hammond, GE (reprint author), Sandia Natl Labs, POB 5800,MS 0747, Albuquerque, NM 87185 USA. EM gehammo@sandia.gov FU U.S. Department of Energy (DOE) through the Office of Biological & Environmental Research, Subsurface Biogeochemical Research, PNNL Science Focus Area under DOE [DE-AC05-76RL01830]; OFM Research FX We thank two anonymous reviewers that greatly improved the manuscript. This research was funded by the U.S. Department of Energy (DOE) through the Office of Biological & Environmental Research, Subsurface Biogeochemical Research, PNNL Science Focus Area under DOE contract DE-AC05-76RL01830. Additional support was provided by OFM Research. Supercomputing resources were provided by the DOE Office of Science Innovative and Novel Computational Impact on Theory and Experiment (INCITE) program with allocations on OLCF Jaguar at Oak Ridge National Laboratory. NR 57 TC 22 Z9 22 U1 2 U2 17 PU AMER GEOPHYSICAL UNION PI WASHINGTON PA 2000 FLORIDA AVE NW, WASHINGTON, DC 20009 USA SN 0043-1397 EI 1944-7973 J9 WATER RESOUR RES JI Water Resour. Res. PD JAN PY 2014 VL 50 IS 1 BP 208 EP 228 DI 10.1002/2012WR013483 PG 21 WC Environmental Sciences; Limnology; Water Resources SC Environmental Sciences & Ecology; Marine & Freshwater Biology; Water Resources GA AB4ZN UT WOS:000331798800015 ER PT J AU O'Malley, D Vesselinov, VV AF O'Malley, D. Vesselinov, V. V. TI Groundwater remediation using the information gap decision theory SO WATER RESOURCES RESEARCH LA English DT Article DE decision theory; uncertainty analysis; groundwater remediation ID UNSATURATED FRACTURED TUFF; SPATIAL VARIABILITY; UNCERTAINTY; FLOW; MANAGEMENT; PROBABILITIES; PARAMETERS; TRANSPORT; MODELS AB One of the challenges in the design and selection of remediation activities for subsurface contamination is dealing with manifold uncertainties. A scientifically defensible decision process demands consideration of the uncertainties involved. A nonprobabilistic approach based on information gap (info-gap) decision theory is employed to study the robustness of alternative remediation activities. This approach incorporates both parametric and nonparametric (conceptual) uncertainty in predicting contaminant concentrations that are effected by natural processes and the remediation activities. Two remedial scenarios are explored to demonstrate the applicability of the info-gap approach to decision making related to groundwater remediation. C1 [O'Malley, D.; Vesselinov, V. V.] Los Alamos Natl Lab, Div Earth & Environm Sci, Computat Earth Sci Grp, Los Alamos, NM 87545 USA. RP O'Malley, D (reprint author), Los Alamos Natl Lab, Div Earth & Environm Sci, Computat Earth Sci Grp, Los Alamos, NM 87545 USA. EM omalled@lanl.gov RI Vesselinov, Velimir/P-4724-2016; OI Vesselinov, Velimir/0000-0002-6222-0530; O'Malley, Daniel/0000-0003-0432-3088 FU Environmental Programs Directorate of the Los Alamos National Laboratory; Advanced Simulation Capability for Environmental Management (ASCEM) project, Department of Energy, Environmental Management; Integrated Multifaceted Approach to Mathematics at the Interfaces of Data, Models, and Decisions (DiaMonD) project, Department of Energy, Office of Science FX The authors wish to thank Y. Ben-Haim for helpful discussions in the preparation of this manuscript. The authors also wish to thank the anonymous reviewers who provided useful comments that improved the manuscript. This research was funded by the Environmental Programs Directorate of the Los Alamos National Laboratory; the Advanced Simulation Capability for Environmental Management (ASCEM) project, Department of Energy, Environmental Management; and the Integrated Multifaceted Approach to Mathematics at the Interfaces of Data, Models, and Decisions (DiaMonD) project, Department of Energy, Office of Science. NR 34 TC 7 Z9 7 U1 2 U2 12 PU AMER GEOPHYSICAL UNION PI WASHINGTON PA 2000 FLORIDA AVE NW, WASHINGTON, DC 20009 USA SN 0043-1397 EI 1944-7973 J9 WATER RESOUR RES JI Water Resour. Res. PD JAN PY 2014 VL 50 IS 1 BP 246 EP 256 DI 10.1002/2013WR014718 PG 11 WC Environmental Sciences; Limnology; Water Resources SC Environmental Sciences & Ecology; Marine & Freshwater Biology; Water Resources GA AB4ZN UT WOS:000331798800017 ER PT J AU Cihan, A Zhou, QL Birkholzer, JT Kraemer, SR AF Cihan, Abdullah Zhou, Quanlin Birkholzer, Jens T. Kraemer, Stephen R. TI Flow in horizontally anisotropic multilayered aquifer systems with leaky wells and aquitards SO WATER RESOURCES RESEARCH LA English DT Article DE analytical solution; anisotropy; multilayered aquifers; groundwater flow; abandoned well; leakage ID CO2 STORAGE; SALINE FORMATIONS; GROUND-WATER AB Flow problems in an anisotropic domain can be transformed into ones in an equivalent isotropic domain by coordinate transformations. Once analytical solutions are obtained for the equivalent isotropic domain, they can be back transformed to the original anisotropic domain. The existing solutions presented by Cihan et al. (2011) for isotropic multilayered aquifer systems with alternating aquitards and multiple injection/pumping wells and leaky wells were modified to account for horizontal anisotropy in aquifers. The modified solutions for pressure buildup distribution and leakage rates through leaky wells can be used when the anisotropy direction and ratio ( Kx/Ky) are assumed to be identical for all aquifers alternating with aquitards. However, for multilayered aquifers alternating with aquicludes, both the principal direction of the anisotropic horizontal conductivity and the anisotropy ratio can be different in each aquifer. With coordinate transformation, a circular well with finite radius becomes an ellipse, and thus in the transformed domain the head contours in the immediate vicinity of the well have elliptical shapes. Through a radial flow approximation around the finite radius wells, the elliptical well boundaries in the transformed domain are approximated by an effective well radius expression. The analytical solutions with the effective radius approximations were compared with exact solutions as well as a numerical solution for elliptic flow. The effective well radius approximation is sufficiently accurate to predict the head buildup at the well bore of the injection/pumping wells for moderately anisotropic systems ( Kx/Ky25). The effective radius approximation gives satisfactory results for predicting head buildup at observation points and leakage through leaky wells away from the injection/pumping wells even for highly anisotropic aquifer systems (Kx/Ky1000). Key Points Anisotropic multilayered aquifer systems A new effective radius approximations to well in anisotropic systems Verification with existing solutions and numerical solutions C1 [Cihan, Abdullah; Zhou, Quanlin; Birkholzer, Jens T.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, Berkeley, CA 94720 USA. [Kraemer, Stephen R.] US EPA, Natl Exposure Res Lab, Ecosyst Res Div, Athens, GA USA. RP Cihan, A (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, 1 Cyclotron Rd,Mail Stop 74R316C, Berkeley, CA 94720 USA. EM acihan@lbl.gov RI Zhou, Quanlin/B-2455-2009; Birkholzer, Jens/C-6783-2011; Cihan, Abdullah/D-3704-2015 OI Zhou, Quanlin/0000-0001-6780-7536; Birkholzer, Jens/0000-0002-7989-1912; FU U.S. Environmental Protection Agency (EPA) [DW89922359-01-0]; Office of Sequestration, Hydrogen, and Clean Coal Fuels, through the National Energy Technology Laboratory, under the USDOE [DE-AC02-05CH11231] FX The authors wish to thank three anonymous reviewers as well as Marco Bianchi of Lawrence Berkeley National Laboratory (LBNL) and Junqi Huang of U.S. Environmental Protection Agency for their careful reviews of the manuscript and suggestions of improvements. The research described in this article has been funded in part by the U.S. Environmental Protection Agency (EPA) through the Interagency agreement DW89922359-01-0 to the U.S. Department of Energy (DOE), Lawrence Berkeley National Laboratory. The views expressed in this article are those of the author(s) and do not necessarily reflect the views or policies of the EPA. Mention of trade names or commercial products does not constitute endorsement or recommendation for use. Supplementary funding was provided by the Assistant Secretary for Fossil Energy, Office of Sequestration, Hydrogen, and Clean Coal Fuels, through the National Energy Technology Laboratory, under the USDOE contract DE-AC02-05CH11231. NR 29 TC 1 Z9 2 U1 1 U2 21 PU AMER GEOPHYSICAL UNION PI WASHINGTON PA 2000 FLORIDA AVE NW, WASHINGTON, DC 20009 USA SN 0043-1397 EI 1944-7973 J9 WATER RESOUR RES JI Water Resour. Res. PD JAN PY 2014 VL 50 IS 1 BP 741 EP 747 DI 10.1002/2013WR013867 PG 7 WC Environmental Sciences; Limnology; Water Resources SC Environmental Sciences & Ecology; Marine & Freshwater Biology; Water Resources GA AB4ZN UT WOS:000331798800050 ER PT J AU Jager, HI McManamay, RA AF Jager, Henriette I. McManamay, Ryan A. TI Comment on "Cumulative biophysical impact of small and large hydropower development in Nu River, China'' by Kelly M. Kibler and Desiree D. Tullos SO WATER RESOURCES RESEARCH LA English DT Editorial Material DE sustainability; indicators C1 [Jager, Henriette I.; McManamay, Ryan A.] Oak Ridge Natl Lab, Div Environm Sci, Oak Ridge, TN 37831 USA. RP Jager, HI (reprint author), Oak Ridge Natl Lab, Div Environm Sci, POB 2008, Oak Ridge, TN 37831 USA. EM jagerhi@ornl.gov OI Jager, Henriette/0000-0003-4253-533X NR 2 TC 1 Z9 1 U1 1 U2 12 PU AMER GEOPHYSICAL UNION PI WASHINGTON PA 2000 FLORIDA AVE NW, WASHINGTON, DC 20009 USA SN 0043-1397 EI 1944-7973 J9 WATER RESOUR RES JI Water Resour. Res. PD JAN PY 2014 VL 50 IS 1 BP 758 EP 759 DI 10.1002/2013WR014378 PG 2 WC Environmental Sciences; Limnology; Water Resources SC Environmental Sciences & Ecology; Marine & Freshwater Biology; Water Resources GA AB4ZN UT WOS:000331798800053 ER PT J AU Cadenas, JJG Alvarez, V Borges, FIG Carcel, S Castel, J Cebrian, S Cervera, A Conde, CAN Dafni, T Dias, THVT Diaz, J Egorov, M Esteve, R Evtoukhovitch, P Fernandes, LMP Ferrario, P Ferreira, AL Freitas, EDC Gehman, VM Gil, A Goldschmidt, A Gomez, H Gonzalez-Diaz, D Gutierrez, RM Hauptman, J Morata, JAH Herrera, DC Iguaz, FJ Irastorza, IG Jinete, MA Labarga, L Laing, A Liubarsky, I Lopes, JAM Lorca, D Losada, M Luzon, G Mari, A Martin-Albo, J Martinez, A Miller, T Moiseenko, A Monrabal, F Monserrate, M Monteiro, CMB Mora, FJ Moutinho, LM Vidal, JM da Luz, HN Navarro, G Nebot-Guinot, M Nygren, D Oliveira, CAB Palma, R Perez, J Perez-Aparicio, JL Renner, J Ripoll, L Rodriguez, A Rodriguez, J Santos, FP dos Santos, JMF Segui, L Serra, L Shuman, D Simon, A Sofka, C Sorel, M Toledo, JF Tomas, A Torrent, J Tsamalaidze, Z Veloso, JFCA Villar, JA Webb, R White, J Yahlali, N AF Gomez Cadenas, J. J. Alvarez, V. Borges, F. I. G. Carcel, S. Castel, J. Cebrian, S. Cervera, A. Conde, C. A. N. Dafni, T. Dias, T. H. V. T. Diaz, J. Egorov, M. Esteve, R. Evtoukhovitch, P. Fernandes, L. M. P. Ferrario, P. Ferreira, A. L. Freitas, E. D. C. Gehman, V. M. Gil, A. Goldschmidt, A. Gomez, H. Gonzalez-Diaz, D. Gutierrez, R. M. Hauptman, J. Hernando Morata, J. A. Herrera, D. C. Iguaz, F. J. Irastorza, I. G. Jinete, M. A. Labarga, L. Laing, A. Liubarsky, I. Lopes, J. A. M. Lorca, D. Losada, M. Luzon, G. Mari, A. Martin-Albo, J. Martinez, A. Miller, T. Moiseenko, A. Monrabal, F. Monserrate, M. Monteiro, C. M. B. Mora, F. J. Moutinho, L. M. Munoz Vidal, J. Natal da Luz, H. Navarro, G. Nebot-Guinot, M. Nygren, D. Oliveira, C. A. B. Palma, R. Perez, Javier Perez-Aparicio, J. L. Renner, J. Ripoll, L. Rodriguez, A. Rodriguez, J. Santos, F. P. dos Santos, J. M. F. Segui, L. Serra, L. Shuman, D. Simon, A. Sofka, C. Sorel, M. Toledo, J. F. Tomas, A. Torrent, J. Tsamalaidze, Z. Veloso, J. F. C. A. Villar, J. A. Webb, R. White, J. Yahlali, N. TI Present Status and Future Perspectives of the NEXT Experiment SO ADVANCES IN HIGH ENERGY PHYSICS LA English DT Review ID DOUBLE-BETA DECAY AB NEXT is an experiment dedicated to neutrinoless double beta decay searches in xenon. The detector is a TPC, holding 100 kg of high-pressure xenon enriched in the Xe-136 isotope. It is under construction in the Laboratorio Subterraneo de Canfranc in Spain, and it will begin operations in 2015. The NEXT detector concept provides an energy resolutionbetter than 1% FWHM and a topological signal that can be used to reduce the background. Furthermore, the NEXT technology can be extrapolated to a 1 ton-scale experiment. C1 [Gomez Cadenas, J. J.; Alvarez, V.; Carcel, S.; Cervera, A.; Diaz, J.; Ferrario, P.; Gil, A.; Laing, A.; Liubarsky, I.; Lorca, D.; Martin-Albo, J.; Martinez, A.; Monrabal, F.; Monserrate, M.; Munoz Vidal, J.; Nebot-Guinot, M.; Rodriguez, J.; Serra, L.; Simon, A.; Sorel, M.; Yahlali, N.] Univ Valencia, CSIC, Inst Fis Corpuscular IFIC, Valencia 46980, Spain. [Borges, F. I. G.; Conde, C. A. N.; Dias, T. H. V. T.; Fernandes, L. M. P.; Freitas, E. D. C.; Lopes, J. A. M.; Monteiro, C. M. B.; Natal da Luz, H.; Santos, F. P.; dos Santos, J. M. F.] Univ Coimbra, Dept Fis, P-3004516 Coimbra, Portugal. [Castel, J.; Cebrian, S.; Dafni, T.; Gomez, H.; Gonzalez-Diaz, D.; Herrera, D. C.; Iguaz, F. J.; Irastorza, I. G.; Luzon, G.; Rodriguez, A.; Segui, L.; Tomas, A.; Villar, J. A.] Univ Zaragoza, Lab Fis Nucl & Astroparticulas, E-50009 Zaragoza, Spain. [Egorov, M.; Gehman, V. M.; Goldschmidt, A.; Miller, T.; Nygren, D.; Oliveira, C. A. B.; Renner, J.; Shuman, D.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Esteve, R.; Mari, A.; Mora, F. J.; Toledo, J. F.] Univ Politecn Valencia, I3M, Valencia 46022, Spain. [Evtoukhovitch, P.; Moiseenko, A.; Tsamalaidze, Z.] Joint Inst Nucl Res, Dubna 141980, Russia. [Ferreira, A. L.; Moutinho, L. M.; Veloso, J. F. C. A.] Univ Aveiro, I3N, P-3810193 Aveiro, Portugal. [Gutierrez, R. M.; Jinete, M. A.; Losada, M.; Navarro, G.] Univ Antonio Narino, Ctr Invest, Bogota, Colombia. [Hauptman, J.] Iowa State Univ, Dept Phys & Astron, Ames, IA 50011 USA. [Hernando Morata, J. A.] Univ Santiago de Compostela, IGFAE, Santiago De Compostela 15782, Spain. [Labarga, L.] Univ Autonoma Madrid, Dept Fis Teor, E-28049 Madrid, Spain. [Palma, R.; Perez-Aparicio, J. L.] Univ Politecn Valencia, Dept Mecan Medios Continuos & Teor Estruct, E-46071 Valencia, Spain. [Perez, Javier] UAM, CSIC, Inst Fis Teor, Madrid 28049, Spain. [Ripoll, L.; Torrent, J.] Univ Girona, Escola Politecn Super, Girona 17071, Spain. [Sofka, C.; Webb, R.; White, J.] Texas A&M Univ, Dept Phys & Astron, College Stn, TX 77843 USA. RP Ferrario, P (reprint author), Univ Valencia, CSIC, Inst Fis Corpuscular IFIC, Calle Catedrat Jose Beltran 2, Valencia 46980, Spain. EM paola.ferrario@ific.uv.es RI YAHLALI, NADIA/L-1880-2014; Monrabal, Francesc/A-5880-2015; Ripoll, Lluis/A-8413-2015; dos Santos, Joaquim/B-3058-2015; Perez-Aparicio, Jose/H-7053-2015; Natal da Luz, Hugo/F-6460-2013; Fernandes, Luis/E-2372-2011; Moutinho, Luis/J-6021-2013; Iguaz Gutierrez, Francisco Jose/F-4117-2016; Gil Ortiz, Alejandro/M-1671-2014; Dafni, Theopisti /J-9646-2012; matias-lopes, jose/H-6074-2012; AMADE Research Group, AMADE/B-6537-2014; Villar, Jose Angel/K-6630-2014; Gonzalez Diaz, Diego/K-7265-2014; Diaz, Jose/B-3454-2012; veloso, joao/J-4478-2013; Irastorza, Igor/B-2085-2012; Gomez Cadenas, Juan Jose/L-2003-2014; Hernando Morata, Jose Angel/L-7642-2014 OI Veloso, Joao/0000-0002-7107-7203; Munoz Vidal, Javier/0000-0002-9649-2251; Toledo Alarcon, Jose Francisco/0000-0002-9782-4510; Freitas, Elisabete/0000-0001-8235-3229; Santos, Filomena/0000-0002-0214-4185; Martin-Albo, Justo/0000-0002-7318-1469; dos Santos, Joaquim Marques Ferreira/0000-0002-8841-6523; Monteiro, Cristina Maria Bernardes/0000-0002-1912-2804; Palma, Roberto/0000-0002-4047-381X; Luzon Marco, Gloria/0000-0002-5352-1884; YAHLALI, NADIA/0000-0003-2184-0132; Monrabal, Francesc/0000-0002-4047-5620; Ripoll, Lluis/0000-0001-8194-5396; Perez-Aparicio, Jose/0000-0003-2884-6991; Natal da Luz, Hugo/0000-0003-1177-870X; Fernandes, Luis/0000-0002-7061-8768; Moutinho, Luis/0000-0001-9074-4449; Iguaz Gutierrez, Francisco Jose/0000-0001-6327-9369; Gil Ortiz, Alejandro/0000-0002-0852-412X; Dafni, Theopisti /0000-0002-8921-910X; matias-lopes, jose/0000-0002-6366-2963; AMADE Research Group, AMADE/0000-0002-5778-3291; Villar, Jose Angel/0000-0003-0228-7589; Gonzalez Diaz, Diego/0000-0002-6809-5996; Diaz, Jose/0000-0002-7239-223X; Irastorza, Igor/0000-0003-1163-1687; Gomez Cadenas, Juan Jose/0000-0002-8224-7714; Hernando Morata, Jose Angel/0000-0002-8683-5142 FU Ministerio de Economia y Competitividad of Spain [CSD20080037 FPA2009-13697-C04-04 FIS2012-37947C04]; Office of Science; Office of Basic Energy Sciences of the US Department of Energy [DE-AC02-05CH11231]; Portuguese FCT and FEDER [PTDC/FIS/103860/2008 PTDC/FIS/112272/2009]; US DOE NNSA Stewardship Science Graduate Fellowship [DE-FC52-08NA28752] FX This work was supported by the following agencies and institutions: the Ministerio de Economia y Competitividad of Spain under Grants CONSOLIDER-Ingenio 2010 CSD2008-0037 (CUP), FPA2009-13697-C04-04, and FIS2012-37947-C04; the Director, Office of Science, Office of Basic Energy Sciences of the US Department of Energy under Contract no. DE-AC02-05CH11231; and the Portuguese FCT and FEDER through the program COMPETE, Projects PTDC/FIS/103860/2008 and PTDC/FIS/112272/2009. J. Renner (LBNL) acknowledges the support of a US DOE NNSA Stewardship Science Graduate Fellowship under Contract no. DE-FC52-08NA28752. J. J. Gomez-Cadenas is a spokes person. NR 41 TC 1 Z9 1 U1 3 U2 22 PU HINDAWI PUBLISHING CORPORATION PI NEW YORK PA 410 PARK AVENUE, 15TH FLOOR, #287 PMB, NEW YORK, NY 10022 USA SN 1687-7357 EI 1687-7365 J9 ADV HIGH ENERGY PHYS JI Adv. High. Energy Phys. PY 2014 AR 907067 DI 10.1155/2014/907067 PG 22 WC Physics, Particles & Fields SC Physics GA AD9YN UT WOS:000333620700001 ER PT J AU Ghosal, S Weber, PK Laskin, A AF Ghosal, Sutapa Weber, Peter K. Laskin, Alexander TI Spatially resolved chemical imaging of individual atmospheric particles using nanoscale imaging mass spectrometry: insight into particle origin and chemistry SO ANALYTICAL METHODS LA English DT Article ID SULFUR ISOTOPE FRACTIONATION; MEXICO-CITY; ENVIRONMENTAL PARTICLES; AEROSOLSURECENT DEVELOPMENTS; ELECTRON-MICROSCOPY; MINERAL DUST; AEROSOL; MICROANALYSIS; OXIDATION; CATALYSIS AB Knowledge of the spatially resolved composition of atmospheric particles is essential for differentiating between their surface versus bulk chemistry and understanding particle reactivity and the potential environmental impact. We demonstrate the application of nanometer-scale secondary ion mass spectrometry (CAMECA NanoSIMS 50 ion probe) for 3D chemical imaging of individual atmospheric particles without any sample pre-treatment, such as sectioning of particles. Use of NanoSIMS depth profile analysis enables elemental mapping of particles with nanometer spatial resolution over a broad range of particle sizes. We have used this technique to probe the spatially resolved composition of ambient particles collected during a field campaign in Mexico City. Particles collected during this campaign have been extensively characterized in the past using other particle analysis techniques and hence offer a unique opportunity for exploring the utility of depth-resolved chemical imaging in ambient particle research. Particles examined in this study include those collected during a pollution episode related to urban waste incineration as well as background particles from the same location before the episode. Particles from the pollution episode show substantial intra-particle compositional variability typical of particles resulting from multiple emission sources. In contrast, the background particles have relatively homogeneous compositions with enhanced presence of nitrogen, oxygen, and chlorine at the particle surface. The observed surface enhancement of nitrogen and oxygen species is consistent with the presence of surface nitrates resulting from gas-particle heterogeneous interactions and is indicative of atmospheric ageing of the particles. The results presented here illustrate 3D characterization of ambient particles for insight into their chemical history. C1 [Ghosal, Sutapa] Calif Dept Publ Hlth, Environm Hlth Lab, Richmond, CA 94804 USA. [Weber, Peter K.] Lawrence Livermore Natl Lab, Glenn T Seaborg Inst, Livermore, CA 94550 USA. [Laskin, Alexander] Pacific NW Natl Lab, William R Wiley Environm Mol Sci Lab, Richland, WA 99352 USA. RP Ghosal, S (reprint author), Calif Dept Publ Hlth, Environm Hlth Lab, Richmond, CA 94804 USA. EM Sutapa.Ghosal@cdph.ca.gov RI Ghosal, Sandip/B-7595-2009; Laskin, Alexander/I-2574-2012 OI Laskin, Alexander/0000-0002-7836-8417 FU Chemical Imaging Initiative under the Laboratory Directed Research and Development funds of Pacific Northwest National Laboratory (PNNL); U.S. Department of Energy at the Lawrence Livermore National Laboratory [DEAC52-07NA27344] FX AL acknowledges support by the Chemical Imaging Initiative under the Laboratory Directed Research and Development funds of Pacific Northwest National Laboratory (PNNL). This work was performed under the auspices of the U.S. Department of Energy at the Lawrence Livermore National Laboratory under Contract DEAC52-07NA27344. NR 35 TC 6 Z9 6 U1 3 U2 41 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1759-9660 EI 1759-9679 J9 ANAL METHODS-UK JI Anal. Methods PY 2014 VL 6 IS 8 BP 2444 EP 2451 DI 10.1039/c3ay42012d PG 8 WC Chemistry, Analytical; Food Science & Technology; Spectroscopy SC Chemistry; Food Science & Technology; Spectroscopy GA AD8NZ UT WOS:000333524200004 ER PT J AU Kastengren, AL Tilocco, FZ Duke, D Powell, CF Zhang, XS Moon, S AF Kastengren, A. L. Tilocco, F. Z. Duke, D. Powell, C. F. Zhang, Xusheng Moon, Seoksu TI TIME-RESOLVED X-RAY RADIOGRAPHY OF SPRAYS FROM ENGINE COMBUSTION NETWORK SPRAY A DIESEL INJECTORS SO ATOMIZATION AND SPRAYS LA English DT Article DE sprays; x-ray; radiography; engine combustion network; diesel; Spray A ID AMBIENT DENSITY AB A significant hurdle to the understanding of sprays is the link between nozzle geometry and the fluid distribution in the spray. X-ray radiography can help to clarify this link by providing quantitative measurements of the spray density in the near-nozzle region, including at the exit plane. The current work describes x-ray radiography measurements performed at Argonne National Laboratory under the "Spray A" conditions of the Engine Combustion Network. Four injector samples have been studied, and model-dependent reconstructions have been used to generate 3D maps of the average fuel density as a function of time. These measurements reveal differences between the sprays from nominally identical injectors that can be interpreted in terms of previously measured geometric differences in the injector nozzles. C1 [Kastengren, A. L.; Tilocco, F. Z.; Duke, D.; Powell, C. F.] Argonne Natl Lab, Div Energy Syst, Argonne, IL 60439 USA. [Zhang, Xusheng; Moon, Seoksu] Argonne Natl Lab, Adv Photon Source, Xray Sci Div, Argonne, IL 60439 USA. RP Kastengren, AL (reprint author), Argonne Natl Lab, Div Energy Syst, 9700 S Cass Ave, Argonne, IL 60439 USA. EM akastengren@anl.gov FU US Department of Energy [DE-AC02-06CH11357]; DOE Vehicle Technologies Program FX This work was performed at the 7-BM beamline of the Advanced Photon Source (APS), Argonne National Laboratory. The use of the APS is supported by the US Department of Energy under Contract No. DE-AC02-06CH11357 and by the DOE Vehicle Technologies Program, with Gurpreet Singh as team leader. The authors also wish to acknowledge Lyle Pickett for performing the optical microscopy measurements shown in Table 3. NR 16 TC 13 Z9 13 U1 0 U2 8 PU BEGELL HOUSE INC PI REDDING PA 50 CROSS HIGHWAY, REDDING, CT 06896 USA SN 1044-5110 EI 1936-2684 J9 ATOMIZATION SPRAY JI Atom. Sprays PY 2014 VL 24 IS 3 BP 251 EP 272 PG 22 WC Engineering, Multidisciplinary; Engineering, Chemical; Engineering, Mechanical; Materials Science, Multidisciplinary; Physics, Applied SC Engineering; Materials Science; Physics GA AE1HK UT WOS:000333720200003 ER PT S AU Gonzalez, JM Fisher, SZ AF Gonzalez, Javier M. Fisher, S. Zoe BE Frost, SC McKenna, R TI Carbonic Anhydrases in Industrial Applications SO CARBONIC ANHYDRASE: MECHANISM, REGULATION, LINKS TO DISEASE, AND INDUSTRIAL APPLICATIONS SE Subcellular Biochemistry LA English DT Article; Book Chapter DE Carbon sequestration; Green house gas; Biomimetic; Biofuel; Thermophiles; Medical applications ID CO2 SEQUESTRATION; DIOXIDE CAPTURE; BIOMIMETIC SEQUESTRATION; CARBONATION REACTION; BACILLUS-SUBTILIS; ARTIFICIAL LUNGS; CLIMATE-CHANGE; IMMOBILIZATION; PROTEIN; ENZYME AB Carbonic anhydrases (CAs) catalyze a fundamental reaction: the reversible hydration and dehydration of carbon dioxide (CO2) and bicarbonate (HCO3-), respectively. Current methods for CO2 capture and sequestration are harsh, expensive, and require prohibitively large energy inputs, effectively negating the purpose of removing CO2 from the atmosphere. Due to CA's activity on CO2 there is increasing interest in using CAs for industrial applications such as carbon sequestration and biofuel production. A lot of work in the last decade has focused on immobilizing CA onto various supports for incorporation into CO2 scrubbing applications or devices. Although the proof of principle has been validated, current CAs being tested do not withstand the harsh industrial conditions. The advent of large-scale genome sequencing projects has resulted in several emerging efforts seeking out novel CAs from a variety of microorganisms, including bacteria, micro-, and macro-algae. CAs are also being investigated for their use in medical applications, such drug delivery systems and artificial lungs. This review also looks at possible downstream uses of captured and sequestered CO2, from using it to enhance oil recovery to incorporating it into useful and financially viable products. C1 [Gonzalez, Javier M.; Fisher, S. Zoe] Los Alamos Natl Lab, Biosci Div, Los Alamos, NM 87701 USA. RP Fisher, SZ (reprint author), Los Alamos Natl Lab, Biosci Div, Los Alamos, NM 87701 USA. EM javierg@lanl.gov; zfisher@lanl.gov OI Gonzalez, Javier M./0000-0002-3298-2235 NR 88 TC 3 Z9 3 U1 0 U2 16 PU SPRINGER PI NEW YORK PA 233 SPRING STREET, NEW YORK, NY 10013, UNITED STATES SN 0306-0225 BN 978-94-007-7359-2; 978-94-007-7358-5 J9 SUBCELL BIOCHEM JI Subcell. Biochem. PY 2014 VL 75 BP 405 EP 426 DI 10.1007/978-94-007-7359-2_20 D2 10.1007/978-94-007-7359-2 PG 22 WC Biochemistry & Molecular Biology; Genetics & Heredity SC Biochemistry & Molecular Biology; Genetics & Heredity GA BA0QY UT WOS:000332111800020 PM 24146390 ER PT J AU Gu, WW Wang, HX Wang, K AF Gu, Weiwei Wang, Hongxin Wang, Kun TI Nickel L-edge and K-edge X-ray absorption spectroscopy of non-innocent Ni[S2C2(CF3)(2)]2(n) series (n =-2,-1, 0): direct probe of nickel fractional oxidation state changes SO DALTON TRANSACTIONS LA English DT Article ID DELOCALIZED GROUND STATES; ELECTRONIC-STRUCTURE; CRYSTAL-STRUCTURE; COORDINATION COMPOUNDS; DITHIOLENE COMPLEXES; ORBITAL MAGNETISM; METAL-COMPLEXES; SPECTRES-L; HYDROGENASES; COVALENCY AB A series of nickel dithiolene complexes Ni[S2C2(CF3)(2)]2(n) (n = -2, -1, 0) has been investigated using Ni L-and K-edge X-ray absorption spectroscopy (XAS). The L-3 centroid shifts about 0.3 eV for a change of one unit in the formal oxidation state (or 0.3 eV per oxi), corresponding to similar to 33% of the shift for Ni oxides or fluorides (about 0.9 eV per oxi). The K-edge XAS edge position shifts about 0.7 eV per oxi, corresponding to similar to 38% of that for Ni oxides (1.85 eV per oxi). In addition, Ni L sum rule analysis found the Ni(3d) ionicity in the frontier orbitals being 50.5%, 44.0% and 38.5% respectively (for n = -2, -1, 0), in comparison with their formal oxidation states (of Ni(II), Ni(III), and Ni(IV)). For the first time, direct and quantitative measurement of the Ni fractional oxidation state changes becomes possible for Ni dithiolene complexes, illustrating the power of L-edge XAS and L sum rule analysis in such a study. The Ni L-edge and K-edge XAS can be used in a complementary manner to better assess the oxidation states for Ni. C1 [Gu, Weiwei; Wang, Hongxin] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA 94720 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 FU National Institutes of Health [GM-65440]; Department of Energy, Office of Basic Energy Sciences; U.S. Department of Energy, Office of Biological and Environmental Research; DOE/LBNL [DE-AC02-05CH11231] FX The research is supported by the National Institutes of Health (GM-65440, to Prof. Stephen P. Cramer at University of California at Davis). We thank Prof. Cramer for the overall support for this work, Prof. C. G. Riordon of University of Delaware for providing the reference sample [PhTttBu] Ni(I)CO. ALS and SSRL are supported by the Department of Energy, Office of Basic Energy Sciences. This research is also part of the advanced biological experimental X-ray spectroscopy program (ABEX), which is supported by the U.S. Department of Energy, Office of Biological and Environmental Research. All the LBNL work is under the DOE/LBNL contract DE-AC02-05CH11231. NR 58 TC 11 Z9 11 U1 0 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 2014 VL 43 IS 17 BP 6406 EP 6413 DI 10.1039/c4dt00308j PG 8 WC Chemistry, Inorganic & Nuclear SC Chemistry GA AD9JG UT WOS:000333580600017 PM 24604143 ER PT J AU Brown, MA Kropf, AJ Paulenova, A Gelis, AV AF Brown, M. Alex Kropf, A. Jeremy Paulenova, Alena Gelis, Artem V. TI Aqueous complexation of citrate with neodymium(III) and americium(III): a study by potentiometry, absorption spectrophotometry, microcalorimetry, and XAFS SO DALTON TRANSACTIONS LA English DT Article ID EQUILIBRIUM-CONSTANTS; CARBOXYLIC-ACIDS; IONIC-STRENGTH; LANTHANIDE; TALSPEAK; SYSTEMS; THERMODYNAMICS; EUROPIUM(III); SPECTROSCOPY; ENTHALPIES AB The aqueous complexation of Nd(III) and Am(III) with anions of citrate was studied by potentiometry, absorption spectrophotometry, microcalorimetry, and X-ray absorption fine structure (XAFS). Using potentiometric titration data fitting the metal-ligand (L) complexes that were identified for Nd(III) were NdHL, NdL, NdHL2, and NdL2; a review of trivalent metal-citrate complexes is also included. Stability constants for these complexes were calculated from potentiometric and spectrophotometric titrations. Microcalorimetric results concluded that the entropy term of complex formation is much more dominant than the enthalpy. XAFS results showed a dependence in the Debye-Waller factor that indicated Nd(III)citrate complexation over the pH range of 1.56-6.12. C1 [Brown, M. Alex; Kropf, A. Jeremy; Gelis, Artem V.] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. [Paulenova, Alena] Oregon State Univ, Dept Nucl Engn & Radiat Hlth Phys, Corvallis, OR 97330 USA. RP Gelis, AV (reprint author), Argonne Natl Lab, Chem Sci & Engn Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM gelis@anl.gov RI BM, MRCAT/G-7576-2011 FU Department of Energy Nuclear Energy University Programs Graduate Fellowship; Fuel Cycle Research and Development Program FX This material is based upon work supported under a Department of Energy Nuclear Energy University Programs Graduate Fellowship and Fuel Cycle Research and Development Program, Sigma Team for Minor Actinide Separation. The authors thank Peter Gans (Protonic Software) for his assistance with the modelling software, Peter Zalupski (INL) and Joseph Lapka (OSU) for discussions on microcalorimetry, Mark Jensen (ANL) for discussions on potentiometry, and the Oregon State University Radiochemistry group for their reviews. We would also like to thank an anonymous reviewer for further enhancing our discussions on the chemical speciation in this work. NR 44 TC 2 Z9 2 U1 5 U2 19 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 2014 VL 43 IS 17 BP 6446 EP 6454 DI 10.1039/c4dt00343h PG 9 WC Chemistry, Inorganic & Nuclear SC Chemistry GA AD9JG UT WOS:000333580600021 PM 24619154 ER PT J AU Kusoglu, A Calabrese, M Weber, AZ AF Kusoglu, Ahmet Calabrese, Michelle Weber, Adam Z. TI Effect of Mechanical Compression on Chemical Degradation of Nafion Membranes SO ECS ELECTROCHEMISTRY LETTERS LA English DT Article ID FUEL-CELL MEMBRANES; POLYMER ELECTROLYTE MEMBRANE; COVALENT BONDS; PFSA MEMBRANES; STRESS; DURABILITY; BEHAVIOR; WATER; ACTIVATION; IONOMERS AB The effect of compression on the chemical degradation of Nafion is investigated. Results indicate a nonlinear dependence of chemical degradation on compression level, with a slight decrease at 1 MPa and then increase up to 10MPa. The results confirm the synergistic nature of mechanical effects on chemical fuel-cell membrane degradation, which are expected to occur in operando. The impact of compression is also shown to change the nano-domain structure, consistent with the increase in chemical decomposition. Thus, deformation energy accumulated in the membrane due to mechanical loads seemingly accelerates the chemical reactions driving the decomposition of the polymer membrane. (C) 2014 The Electrochemical Society. All rights reserved. C1 [Kusoglu, Ahmet; Calabrese, Michelle; Weber, Adam Z.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. RP Kusoglu, A (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. EM akusoglu@lbl.gov OI Kusoglu, Ahmet/0000-0002-2761-1050 FU Science Undergraduate Laboratory Internship (SULI) program of the U. S. Department of Energy; Fuel Cell Technologies Office, of the U. S. Department of Energy [DE-AC02-05CH11231]; Department of Energy, Office of Basic Energy Sciences [DE-AC02-05CH11231] FX Authors thank Dr. Wonseok Yoon for his help with the preparation of test setup and for helpful discussions. ME acknowledges support from the Science Undergraduate Laboratory Internship (SULI) program of the U. S. Department of Energy. This work was funded by the Assistant Secretary for Energy Efficiency and Renewable Energy, Fuel Cell Technologies Office, of the U. S. Department of Energy under contract number DE-AC02-05CH11231. SAXS experiments were performed at beamline 7.3.3 at the Advanced Light Source (ALS), Lawrence Berkeley National Laboratory, which is a national user facility funded by the Department of Energy, Office of Basic Energy Sciences under contract number DE-AC02-05CH11231. NR 32 TC 12 Z9 12 U1 3 U2 12 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 2014 VL 3 IS 5 BP F33 EP F36 DI 10.1149/2.008405eel PG 4 WC Electrochemistry; Materials Science, Multidisciplinary SC Electrochemistry; Materials Science GA AE2LL UT WOS:000333804400009 ER PT J AU Thomson, AM Kyle, GP Zhang, X Bandaru, V West, TO Wise, MA Izaurralde, RC Calvin, KV AF Thomson, A. M. Kyle, G. P. Zhang, X. Bandaru, V. West, T. O. Wise, M. A. Izaurralde, R. C. Calvin, K. V. TI The contribution of future agricultural trends in the US Midwest to global climate change mitigation SO GLOBAL ENVIRONMENTAL CHANGE-HUMAN AND POLICY DIMENSIONS LA English DT Article DE Integrated assessment; Climate mitigation; Agriculture ID LAND-USE CHANGE; ORGANIC-CARBON SEQUESTRATION; INTEGRATED ASSESSMENT; HIGH-RESOLUTION; LONG-TERM; EMISSIONS; BIOFUELS; MANAGEMENT; CROPLANDS; DYNAMICS AB Land use change is a complex response to changing environmental and socioeconomic systems. Historical drivers of land use change include changes in the natural resource availability of a region, changes in economic conditions for production of certain products and changing policies. Most recently, introduction of policy incentives for biofuel production have influenced land use change in the US Midwest, leading to concerns that bioenergy production systems may compete with food production and land conservation. Here we explore how land use may be impacted by future climate mitigation measures by nesting a high resolution agricultural model (EPIC - Environmental Policy Indicator Climate) for the US Midwest within a global integrated assessment model (GCAM - Global Change Assessment Model). This approach is designed to provide greater spatial resolution and detailed agricultural practice information by focusing on the climate mitigation potential of agriculture and land use in a specific region, while retaining the global economic context necessary to understand the far ranging effects of climate mitigation targets. We find that until the simulated carbon prices are very high, the US Midwest has a comparative advantage in producing traditional food and feed crops over bioenergy crops. Overall, the model responds to multiple pressures by adopting a mix of future responses. We also find that the GCAM model is capable of simulations at multiple spatial scales and agricultural technology resolution, which provides the capability to examine regional response to global policy and economic conditions in the context of climate mitigation. (C) 2014 Elsevier Ltd. All rights reserved. C1 [Thomson, A. M.; Kyle, G. P.; Zhang, X.; Bandaru, V.; West, T. O.; Wise, M. A.; Izaurralde, R. C.; Calvin, K. V.] Pacific NW Natl Lab, Joint Global Change Res Inst, College Pk, MD 20740 USA. RP Thomson, AM (reprint author), Pacific NW Natl Lab, Joint Global Change Res Inst, 5825 Univ Res Court,Suite 3500, College Pk, MD 20740 USA. EM allison.thomson@pnnl.gov RI Thomson, Allison/B-1254-2010; zhang, xuesong/B-7907-2009; OI Calvin, Katherine/0000-0003-2191-4189 FU PNNL Laboratory Directed Research and Development program as part of the Platform for Regional Integrated Modeling and Assessment; NASA [NNH12AU031]; DOE by Battelle Memorial Institute [DE-AC05-76RL01830] FX This research was funded through the PNNL Laboratory Directed Research and Development program as part of the Platform for Regional Integrated Modeling and Assessment. Longterm support for GCAM development is provided by the Integrated Assessment Research Program in the DOE Office of Science and additional support for EPIC development was provided by NASA (NNH12AU031). This research used Evergreen computing resources at PNNL's Joint Global Change Research Institute at the University of Maryland in College Park. PNNL is operated for DOE by Battelle Memorial Institute under contract DE-AC05-76RL01830. We thank Stephanie Waldhoff for valuable feedback on earlier versions of the manuscript. NR 73 TC 7 Z9 7 U1 3 U2 32 PU ELSEVIER SCI LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, OXON, ENGLAND SN 0959-3780 EI 1872-9495 J9 GLOBAL ENVIRON CHANG JI Glob. Environ. Change-Human Policy Dimens. PD JAN PY 2014 VL 24 BP 143 EP 154 DI 10.1016/j.gloenvcha.2013.11.019 PG 12 WC Environmental Sciences; Environmental Studies; Geography SC Environmental Sciences & Ecology; Geography GA AD8HC UT WOS:000333506100015 ER PT J AU Smith, AM Kast, MG Nail, BA Aloni, S Boettcher, SW AF Smith, Adam M. Kast, Matthew G. Nail, Benjamin A. Aloni, Shaul Boettcher, Shannon W. TI A planar-defect-driven growth mechanism of oxygen deficient tungsten oxide nanowires SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID LOW-TEMPERATURE; ELECTRON-MICROSCOPY; SCREW DISLOCATIONS; NANOTUBES; FILMS; CONVERSION; TRIOXIDE; NANORODS; ARRAYS; SCALE AB Tungsten oxide nanowires (NWs) have many applications and can be grown simply via vapor transport from solid WO3, but the mechanism by which they form is not well understood. We performed a series of vapor transport tungsten oxide growth experiments with controlled oxygen partial pressures, source-to-substrate temperature differences, and with W or WO3 substrates. The resulting films were analyzed using electron microscopy, diffraction, and photoelectron spectroscopy. NWs formed only under sufficiently reducing conditions where substoichiometric compositions (e. g. similar to WO2.9) were obtained. Transmission electron microscopy (TEM) analysis of the NWs revealed extended defects parallel to the (010) NW growth direction, similar to those found in bulk samples that are associated with ordered O vacancies. Cross-sectional TEM analysis showed that the defects appear to bound, and thus potentially stabilize the nanowire surface to preference the 1D growth. NWs annealed in air show decreasing defect concentrations with increasing temperature and a progressive collapse of the 1D morphology. These results support a mechanism where oxygen-deficient substoichiometric planar defects oriented parallel to the NW long axis direct the NW growth. This mechanism is likely relevant to other oxide nanomaterials that form extended defects due to oxygen non-stoichiometry. The role of defects in controlling the growth morphology is also important for NW applications because the defects may be beneficial (e. g. for thermoelectrics) or detrimental (e. g. for photoelectrochemical cells) to device performance. C1 [Smith, Adam M.; Kast, Matthew G.; Nail, Benjamin A.; Boettcher, Shannon W.] Univ Oregon, Dept Chem & Biochem, Eugene, OR 97403 USA. [Kast, Matthew G.; Boettcher, Shannon W.] Univ Oregon, Ctr Sustainable Mat Chem, Eugene, OR 97403 USA. [Aloni, Shaul] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA. RP Boettcher, SW (reprint author), Univ Oregon, Dept Chem & Biochem, Eugene, OR 97403 USA. EM swb@uoregon.edu RI Foundry, Molecular/G-9968-2014 FU Office of Naval Research, through the Oregon Nanoscience and Microtechnologies Institute; Center for Sustainable Materials Chemistry through the National Science Foundation grant [CHE-1102637]; user program at the Molecular Foundry, Lawrence Berkeley National Laboratory; U.S. Department of Energy Office of Science, Office of Basic Energy Sciences [DE-AC02-05CH1123]; National Science Foundation [DGE-0742540]; McNair Scholars Program; W.M. Keck Foundation; M.J. Murdock Charitable Trust; ONAMI; Air Force Research Laboratory [FA8650-05-1-5041]; NSF [0923577, 0421086]; University of Oregon; DuPont Young Professors program FX This work was partially supported by the Office of Naval Research, through the Oregon Nanoscience and Microtechnologies Institute. M.G.K. and the XPS analysis portion of the study was supported by the Center for Sustainable Materials Chemistry through the National Science Foundation grant CHE-1102637. We also acknowledge support from the user program at the Molecular Foundry, Lawrence Berkeley National Laboratory, with funding from the U.S. Department of Energy Office of Science, Office of Basic Energy Sciences under Contract DE-AC02-05CH1123. A.M.S. acknowledges support from the National Science Foundation grant DGE-0742540 as a GK-12 teaching fellow. B.A.N. acknowledges support from the McNair Scholars Program. The CAMCOR shared instrument facilities are supported by grants from the W.M. Keck Foundation, the M.J. Murdock Charitable Trust, ONAMI, the Air Force Research Laboratory (FA8650-05-1-5041), NSF (0923577 and 0421086) and the University of Oregon. S.W.B. acknowledges support from the DuPont Young Professors program. NR 61 TC 14 Z9 14 U1 3 U2 59 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 2014 VL 2 IS 17 BP 6121 EP 6129 DI 10.1039/c3ta14163b PG 9 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA AD9JH UT WOS:000333580700021 ER PT J AU Xia, H Hu, MZ Meng, YS Xie, JP Zhao, XY AF Xia, Hui Hu, Michael Z. Meng, Ying Shirley Xie, Jianping Zhao, Xiangyu TI Nanostructured Materials for Clean Energy and Environmental Challenges SO JOURNAL OF NANOMATERIALS LA English DT Editorial Material C1 [Xia, Hui] Nanjing Univ Sci & Technol, Sch Mat Sci & Engn, Nanjing 210094, Jiangsu, Peoples R China. [Hu, Michael Z.] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. [Meng, Ying Shirley] Univ Calif San Diego, Dept NanoEngn, San Diego, CA 92103 USA. [Xie, Jianping] Natl Univ Singapore, Dept Chem & Biomol Engn, Singapore 117576, Singapore. [Zhao, Xiangyu] Inst Technol, Inst Nanotechnol, Karlsruhe, Germany. RP Xia, H (reprint author), Nanjing Univ Sci & Technol, Sch Mat Sci & Engn, Nanjing 210094, Jiangsu, Peoples R China. EM xiahui@njust.edu.cn OI Hu, Michael/0000-0001-8461-9684; Xie, Jianping/0000-0002-3254-5799 NR 0 TC 0 Z9 0 U1 1 U2 14 PU HINDAWI PUBLISHING CORPORATION PI NEW YORK PA 410 PARK AVENUE, 15TH FLOOR, #287 PMB, NEW YORK, NY 10022 USA SN 1687-4110 EI 1687-4129 J9 J NANOMATER JI J. Nanomater. PY 2014 AR 675859 DI 10.1155/2014/675859 PG 2 WC Nanoscience & Nanotechnology; Materials Science, Multidisciplinary SC Science & Technology - Other Topics; Materials Science GA AE2SP UT WOS:000333823600001 ER PT J AU Zhu, HP Hu, MZ Shao, L Yu, K Dabestani, R Zaman, MB Liao, SJ AF Zhu, Huaping Hu, Michael Z. Shao, Lei Yu, Kui Dabestani, Reza Zaman, Md. Badruz Liao, Shijun TI Synthesis and Optical Properties of Thiol Functionalized CdSe/ZnS (Core/Shell) Quantum Dots by Ligand Exchange SO JOURNAL OF NANOMATERIALS LA English DT Article ID SEMICONDUCTOR NANOCRYSTALS; COMPOSITE NANOSTRUCTURES; PHOTOPHYSICAL PROPERTIES; GOLD NANOCRYSTALS; NANOPARTICLES; PHOTOLUMINESCENCE; BLINKING; CLUSTERS; LUMINESCENCE; SUPPRESSION AB The colloidal photoluminescent quantum dots (QDs) of CdSe (core) and CdSe/ZnS (core/shell) were synthesized at different temperatures with different growth periods. Optical properties (i.e., UV/Vis spectra and photoluminescent emission spectra) of the resulting QDs were investigated. The shell-protected CdSe/ZnS QDs exhibited higher photoluminescent (PL) efficiency and stability than their corresponding CdSe core QDs. Ligand exchange with various thiol molecules was performed to replace the initial surface passivation ligands, that is, trioctylphosphine oxide (TOPO) and trioctylphosphine (TOP), and the optical properties of the surface-modified QDs were studied. The thiol ligand molecules in this study included 1,4-benzenedimethanethiol, 1,16-hexadecanedithiol, 1,11-undecanedithiol, biphenyl-4,4'-dithiol, 11-mercapto-1-undecanol, and 1,8-octanedithiol. After the thiol functionalization, the CdSe/ZnSQDs exhibited significantly enhanced PL efficiency and storage stability. Besides surface passivation effect, such enhanced performance of thiol-functionalized QDs could be due to cross-linked assembly formation of dimer/trimer clusters, in which QDs are linked by dithiol molecules. Furthermore, effects of ligand concentration, type of ligand, and heating on the thiol stabilization of QDs were also discussed. C1 [Zhu, Huaping; Hu, Michael Z.; Dabestani, Reza] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. [Zhu, Huaping; Liao, Shijun] S China Univ Technol, Sch Chem & Chem Engn, Guangzhou 510641, Guangdong, Peoples R China. [Shao, Lei] Beijing Univ Chem Technol, Key Lab Nanomat, Minist Educ, Minist Educ High Grav Engn & Technol,Res Ctr, Beijing 100029, Peoples R China. [Yu, Kui; Zaman, Md. Badruz] Natl Res Council Canada, Steacie Inst Mol Sci, Ottawa, ON K1A 0R6, Canada. RP Hu, MZ (reprint author), Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. EM hum1@ornl.gov RI Liao, Shijun/C-1745-2012; OI Hu, Michael/0000-0001-8461-9684 FU Laboratory Directed Research and Development Program (Seed Money project) of ORNL; China Scholarship Council; China National Natural Science Foundation FX The authors would like to thank their colleagues at the Oak Ridge National Laboratory (ORNL), particularly Edward {Ed} W. Hagaman and Jian Jiao for providing NMR measurements and Reza T. Dabestani for giving access to the UV-Vis absorption and photoluminescence spectrometers. Thanks are also due to E. Andrew Payzant for XRD data, Lawrence Frederick Allard Jr. for data obtained from the ACEM at the ORNL HTML user facility, and David C. Joy for data obtained from the STEM at the ORNL/CNMS user facility. This work was supported in part by the Laboratory Directed Research and Development Program (Seed Money project) of ORNL, which is managed by UT-Battelle, LLC, for the U.S. Department of Energy, and NA22 program. The authors would also like to acknowledge China Scholarship Council and China National Natural Science Foundation for providing the financial support to Ph.D. student candidate Huaping Zhu. NR 54 TC 3 Z9 3 U1 6 U2 91 PU HINDAWI PUBLISHING CORPORATION PI NEW YORK PA 410 PARK AVENUE, 15TH FLOOR, #287 PMB, NEW YORK, NY 10022 USA SN 1687-4110 EI 1687-4129 J9 J NANOMATER JI J. Nanomater. PY 2014 AR 324972 DI 10.1155/2014/324972 PG 14 WC Nanoscience & Nanotechnology; Materials Science, Multidisciplinary SC Science & Technology - Other Topics; Materials Science GA AD9NS UT WOS:000333592400001 ER PT J AU Collins, E Pantoya, M Neuber, AA Daniels, M AF Collins, Eric Pantoya, Michelle Neuber, Andreas A. Daniels, Michael TI Piezoelectric Ignition of Nanocomposite Energetic Materials SO JOURNAL OF PROPULSION AND POWER LA English DT Article ID ELECTRIC-POWER GENERATION; RANDOM PACKING; SPHERICAL-PARTICLES; SIZE DISTRIBUTIONS; THERMITES; ALUMINUM; SPHERES; COMBUSTION; SIMULATION; CERAMICS AB Piezoelectric initiators are a unique form of ignition for energetic material because the current and voltage are tied together by impact loading on the crystal. This study examines the ignition response of an energetic composite composed of aluminum and molybdenum trioxide nanopowders to the arc generated from a lead zirconate and lead titanate piezocrystal. The mechanical stimuli used to activate the piezocrystal varied to assess ignition voltage, power, and delay time of aluminum-molybdenum trioxide for a range of bulk powder densities. Results show a high dielectric strength leads to faster ignition times because of the higher voltage delivered to the energetic. Ignition delay is under 0.4ms, which is faster than observed with thermal or shock ignition. Electric ignition of composite energetic materials is a strong function of interparticle connectivity, and thus the role of bulk density on electrostatic discharge ignition sensitivity is a focus of this study. Results show that the ignition delay times are dependent on the powder bulk density with an optimum bulk density of 50%. Packing fractions and electrical conductivity were analyzed and aid in explaining the resulting ignition behavior as a function of bulk density. C1 [Collins, Eric; Pantoya, Michelle] Texas Tech Univ, Dept Mech Engn, Lubbock, TX 79409 USA. [Neuber, Andreas A.] Texas Tech Univ, Dept Elect Engn, Lubbock, TX 79409 USA. [Daniels, Michael] Idaho Natl Lab, Idaho Falls, ID 83415 USA. RP Pantoya, M (reprint author), Texas Tech Univ, Dept Mech Engn, Lubbock, TX 79409 USA. EM michelle.pantoya@ttu.edu FU Army Research Office [W911NF-11-1-0439]; Idaho National Laboratory; Laboratory Directed Research and Development program FX Authors M. Pantoya and E. Collins are grateful for support from the Army Research Office contract W911NF-11-1-0439 and for encouragement from our program manager, Ralph Anthenien. Idaho National Laboratory is also gratefully acknowledged for supporting this collaborative work with internal funds via the Laboratory Directed Research and Development program. NR 22 TC 1 Z9 1 U1 1 U2 10 PU AMER INST AERONAUTICS ASTRONAUTICS PI RESTON PA 1801 ALEXANDER BELL DRIVE, STE 500, RESTON, VA 22091-4344 USA SN 0748-4658 EI 1533-3876 J9 J PROPUL POWER JI J. Propul. Power PD JAN-FEB PY 2014 VL 30 IS 1 BP 15 EP 18 DI 10.2514/1.B35034 PG 4 WC Engineering, Aerospace SC Engineering GA AD9SK UT WOS:000333604600001 ER PT J AU Liu, YD Liu, Q Li, ZF Ren, Y Xie, J He, H Xu, F AF Liu, Yadong Liu, Qi Li, Zhefei Ren, Yang Xie, Jian He, Hao Xu, Fan TI Failure Study of Commercial LiFePO4 Cells in over-Discharge Conditions Using Electrochemical Impedance Spectroscopy SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID LITHIUM-ION BATTERIES; SAFETY; OVERCHARGE; MECHANISMS; ISSUES AB Electrochemical impedance spectroscopy (EIS) studies were carried out on commercial 18650 LiFePO4 cells at different States of Charge (SOCs) to investigate failure in over-discharge conditions. The charge/discharge curves, capacity, charge acceptance, temperature, and impedance were characterized and analyzed. The EIS results show that the de-convoluted Ohmic resistance, R-0, solid electrolyte interphase (SEI) resistance, R-SEI, and Warburg Coefficient, sigma, change with cycle number in some patterns, indicating the occurrence of corrosion of the current collector, SEI breakdown/decomposition and reformation, and the development of diffusion barriers of Li+ in the electrode, respectively. These parameters, R-0, R-SEI, and sigma are associated with failure and can be used as indicators of incoming failure. The EIS results from the three-electrode system verify that the EIS results from the two-electrode system (practical 18650 cells) are reliable, which lays the foundation for the use of electrochemical impedance on practical applications of LIB cells. Overall, electrochemical impedance spectroscopy can be used as an effective and reliable tool to monitor the state of health, predict incoming failure of the cell, and issue a warning before failure without disturbing the operation of the cell. (C) 2014 The Electrochemical Society. All rights reserved. C1 [Liu, Yadong; Liu, Qi; Li, Zhefei; Xie, Jian; He, Hao; Xu, Fan] Indiana Univ Purdue Univ, Purdue Sch Engn & Technol, Dept Mech Engn, Indianapolis, IN 46202 USA. [Ren, Yang] Argonne Natl Lab, Xray Sci Div, Argonne, IL 60439 USA. RP Liu, YD (reprint author), Indiana Univ Purdue Univ, Purdue Sch Engn & Technol, Dept Mech Engn, Indianapolis, IN 46202 USA. EM jianxie@iupui.edu RI Li, Zhefei/M-1106-2015 FU U.S. Navy [N00164-09-C-GS42]; U.S. Department of Energy, Office of Science, Office of Basic Energy Science [DE-AC02-06CH11357] FX This work was financially supported by the U.S. Navy under contract N00164-09-C-GS42. The authors would also like to express appreciation to A123 Systems for providing the 18650 LiFePO4 cells for testing. 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. NR 27 TC 9 Z9 9 U1 12 U2 65 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 2014 VL 161 IS 4 BP A620 EP A632 DI 10.1149/2.090404jes PG 13 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA AD8XR UT WOS:000333549500024 ER PT J AU Sacci, RL Adamczyk, LA Veith, GM Dudney, NJ AF Sacci, Robert L. Adamczyk, Leslie A. Veith, Gabriel M. Dudney, Nancy J. TI Dry Synthesis of Lithium Intercalated Graphite Powder and Fiber SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID ION BATTERIES; LITHIATED GRAPHITE; CARBON AB Herein we describe the direct synthesis of lithium intercalated graphite by heating under vacuum or ball milling under pressurized Ar(g). Both methods allow for stoichometric control of Li-C ratio in battery-grade graphites and carbon fibers prior to formation of a solid electrolyte interphase. The products' surface chemistries, as probed by XPS, suggest that LiC6 are extremely reactive with trace amounts of moisture or oxygen. The open circuit potential and SEM data show that the reactivity of the lithiated battery-grade graphite and the carbon fiber can be related to the density of edge/defect sites on the surfaces. Preliminary results of spontaneous delithiation of Li-graphite in electrolyte are also given. (C) 2014 The Electrochemical Society. All rights reserved. C1 [Sacci, Robert L.; Adamczyk, Leslie A.; Veith, Gabriel M.; Dudney, Nancy J.] Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. RP Sacci, RL (reprint author), Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. EM saccirl@ornl.gov; dadneynj@ornl.gov RI Dudney, Nancy/I-6361-2016 OI Dudney, Nancy/0000-0001-7729-6178 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; U.S. Department of Energy, Office of Basic Energy Sciences, Materials Sciences and Engineering Division FX Research was supported by 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 (RLS, LAA, NJD). XPS analysis was done with support of the U.S. Department of Energy, Office of Basic Energy Sciences, Materials Sciences and Engineering Division (GMV). The authors thank Applied Science, Inc. for samples of the Pyrograf I carbon fibers and Pred Materials International for the MGPA. NR 16 TC 5 Z9 5 U1 6 U2 35 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 2014 VL 161 IS 4 BP A614 EP A619 DI 10.1149/2.082404jes PG 6 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA AD8XR UT WOS:000333549500023 ER PT J AU Saha, P Jampani, PH Datta, MK Okoli, CU Manivannan, A Kumta, PN AF Saha, Partha Jampani, Prashanth H. Datta, Moni Kanchan Okoli, Chris U. Manivannan, Ayyakkannu Kumta, Prashant N. TI A Convenient Approach to Mo6S8 Chevrel Phase Cathode for Rechargeable Magnesium Battery SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID ELECTROLYTE-SOLUTIONS; MG BATTERIES; ORGANIC-SOLVENTS; PERFORMANCE; TECHNOLOGY; DEPOSITION; INSERTION; COMPOUND; CU2MO6S8; PROGRESS AB A two-step solution chemistry route was used to synthesize ternary Chevrel phase (Cu2Mo6S8) with 5 h annealing at 1000 degrees C under reducing atmosphere. The approach marks a synthesis route different from hitherto described conventional solid-state methods. X-ray diffraction and scanning electron micrograph shows the formation of similar to 1-1.5 mu m size cuboidal shape Cu2Mo6S8 crystals with unit cell dimensions a similar to 0.96245 nm and c similar to 1.01987 nm of molar volume similar to 818.14 x 10(-3) nm(3). De-cuprated Mo6S8 exhibits a discharge capacity similar to 76 mAhg(-1) with good capacity retention up to similar to 50 cycles when cycled at the current rate of 20 mA/g (similar to C/6). The excellent rate capability and high Coulombic efficiency (similar to 99.3% at similar to 1.5C rate) of the Mo6S8 cathode renders the solution chemistry route an alternative approach for the synthesis of cuprated Chevrel phase: a known cathode system for magnesium battery. (C) 2014 The Electrochemical Society. All rights reserved. C1 [Saha, Partha; Datta, Moni Kanchan; Kumta, Prashant N.] Univ Pittsburgh, Swanson Sch Engn, Dept Bioengn, Pittsburgh, PA 15261 USA. [Jampani, Prashanth H.; Okoli, Chris U.; Kumta, Prashant N.] Univ Pittsburgh, Swanson Sch Engn, Pittsburgh, PA 15261 USA. [Datta, Moni Kanchan; Kumta, Prashant N.] Univ Pittsburgh, Ctr Complex Engn Multifunct Mat, Pittsburgh, PA 15261 USA. [Manivannan, Ayyakkannu; Kumta, Prashant N.] US DOE, Natl Energy Technol Lab, Morgantown, WV 26507 USA. [Kumta, Prashant N.] Univ Pittsburgh, Sch Dent Med, Pittsburgh, PA 15261 USA. RP Saha, P (reprint author), Univ Pittsburgh, Swanson Sch Engn, Dept Bioengn, Pittsburgh, PA 15261 USA. EM pkumta@pitt.edu RI Jampani Hanumantha, Prashanth/A-9840-2013 OI Jampani Hanumantha, Prashanth/0000-0001-7159-1993 FU Department of Energy's National Energy Technology Laboratory's program DOE-NETL) [DE-FE0004000]; Edward R. Weidlein Chair Professorship funds; Center for Complex Engineered Multifunctional Materials (CCEMM); United States Government FX The authors gratefully acknowledge the financial support as part of the Department of Energy's National Energy Technology Laboratory's program DOE-NETL) (contract number DE-FE0004000). PNK also acknowledge the Edward R. Weidlein Chair Professorship funds and the Center for Complex Engineered Multifunctional Materials (CCEMM) for partial support of this research.; 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 31 TC 17 Z9 17 U1 11 U2 87 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 2014 VL 161 IS 4 BP A593 EP A598 DI 10.1149/2.061404jes PG 6 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA AD8XR UT WOS:000333549500020 ER PT J AU Banga, D Perdue, B Stickney, J AF Banga, Dhego Perdue, Brian Stickney, John TI Formation of CuIn(1-x)GaxSe2 (CIGS) by Electrochemical Atomic Layer Deposition (ALD) SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID SILICON SOLAR-CELLS; UNDERPOTENTIAL DEPOSITION; MODULATED REACTANTS; THIN-FILMS; CU(IN,GA)SE-2; ELECTRODEPOSITION; STM; SUPERLATTICES; PRECURSORS; AU(100) AB The formation of CuIn(1-x)GaxSe2 (CIGS) by electrochemical atomic layer deposition (E-ALD) is reported. Two different CIGS E-ALD cycle programs were investigated. The first consisted of the sequential deposition of alternating atomic layers (AL) metal and Se. That is, AL of Cu, In and Ga were alternated with AL of Se, in what is referred to as a quaternary CIGS program. The second was a superlattice program, composed of differing numbers of the binary compound cycles repeated in a period. The use of the superlattice program allowed better control of the overall stoichiometry. Electron probe microanalysis was used to characterize deposit compositions. A discussion of how variations in the deposition programs affected the resulting deposit compositions is presented. Deposits were formed with the classic CIGS stoichiometry (CuIn0.7Ga0.3Se2) using the superlattice program. XRD patterns for the E-ALD deposited chalcopyrite CIGS are reported as deposited, no annealing. (C) 2014 The Electrochemical Society. All rights reserved. C1 [Banga, Dhego] Sandia Natl Labs, Dept Mat Phys, Livermore, CA 94550 USA. [Banga, Dhego; Perdue, Brian; Stickney, John] Univ Georgia, Dept Chem, Athens, GA 30602 USA. RP Banga, D (reprint author), Sandia Natl Labs, Dept Mat Phys, Livermore, CA 94550 USA. EM stickney@chem.uga.edu FU National Science foundation, Division of Materials Research [1006747] FX Support from the National Science foundation, Division of Materials Research #1006747, is gratefully acknowledged. NR 39 TC 2 Z9 2 U1 2 U2 22 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 2014 VL 161 IS 4 BP D141 EP D146 DI 10.1149/2.031404jes PG 6 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA AD8XR UT WOS:000333549500042 ER PT J AU Zhang, MQ Watson, JS Counce, RM Trulove, PC Zawodzinski, TA AF Zhang, Mengqi Watson, Jack S. Counce, Robert M. Trulove, Paul C. Zawodzinski, Thomas A., Jr. TI Electrochemistry and Morphology Studies of Aluminum Plating/Stripping in a Chloroaluminate Ionic Liquid on Porous Carbon Materials SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID ELECTRODEPOSITION; NUCLEATION; CHLORIDE AB Aluminum electrodeposition and electrodissolution in mixtures of AlCl3 and 1-ethyl-3-methylimidazolium chloride on carbon paper electrodes consisting of graphitized fibers were investigated. Porous electrodes, such as carbon paper electrodes, often offer possible advantages such as higher nominal current densities and less dendrite formation, over solid planar electrodes. Cyclic voltammetry, chronoamperometry and pulse current deposition were used to investigate Al plating and stripping on this porous structure. The Al morphology on the carbon paper was probed using SEM. Composition and temperature affect the Al electrode performance through their influence on the diffusivity of ions. Therefore, control of the diffusion process during Al plating/stripping is essential. (C) 2014 The Electrochemical Society. All rights reserved. C1 [Zhang, Mengqi; Watson, Jack S.; Counce, Robert M.; Zawodzinski, Thomas A., Jr.] Univ Tennessee, Dept Chem & Biomol Engn, Knoxville, TN 37996 USA. [Trulove, Paul C.] US Naval Acad, Dept Chem, Annapolis, MD 21402 USA. [Zawodzinski, Thomas A., Jr.] Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. [Zawodzinski, Thomas A., Jr.] King Abdulaziz Univ, Dept Chem, Jeddah 21413, Saudi Arabia. RP Zhang, MQ (reprint author), Univ Tennessee, Dept Chem & Biomol Engn, Knoxville, TN 37996 USA. EM mzhang17@utk.edu FU TNSCORE program, NSF [EPS-1004083] FX We thank the TNSCORE program, NSF EPS-1004083, for funding this work. NR 13 TC 3 Z9 3 U1 2 U2 38 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 2014 VL 161 IS 4 BP D163 EP D167 DI 10.1149/2.048404jes PG 5 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA AD8XR UT WOS:000333549500046 ER PT J AU Rowlett, JR Chen, Y Shaver, AT Fahs, GB Sundell, BJ Li, Q Kim, YS Zelenay, P Moore, RB Mecham, S McGrath, JE AF Rowlett, Jarrett R. Chen, Yu Shaver, Andrew T. Fahs, Gregory B. Sundell, Benjamin J. Li, Qing Kim, Yu Seung Zelenay, Piotr Moore, Robert B. Mecham, Sue McGrath, James E. TI Multiblock Copolymers Based upon Increased Hydrophobicity Bisphenol A Moieties for Proton Exchange Membranes SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID POLY(ARYLENE ETHER SULFONE)S; FUEL-CELL APPLICATION; RANDOM STATISTICAL COPOLYMERS; POLYMER ELECTROLYTE MEMBRANE; ACID GROUPS; BENZONITRILE) COPOLYMERS; HYDROCARBON MEMBRANES; PERFORMANCE; NITRILE)S; TEMPERATURE AB Increasing hydrophobicity multiblock copolymers were synthesized by altering the copolymer composition of the hydrophobic segments. A series of nitrile-containing hydrophobic oligomers consisting of bisphenol A (Bis A), dimethylbisphenol A (DMBPA), and tetramethylbisphenol A (TMBPA) moieties were reacted with a disulfonated poly (arylene ether sulfone) hydrophilic segment to form the multiblock copolymer series. H-1 and F-19 NMR spectroscopy were used to monitor the progress of the copolymerization reactions and confirm the desired compositions. Membranes cast from the resultant multiblock copolymers had high molecular weight as measured by size-exclusion chromatography (SEC), and showed strong mechanical properties. As the hydrophobicity of the polymers increased from the Bis A, to the DMBPA, and to the TMBPA systems, the membranes showed a corresponding decrease in water uptake. The reduced water uptake and limited fluorine content produced membranes with significantly reduced methanol permeabilities over that of Nafion or other similar multiblock copolymer membranes. Electrochemical testing showed that the more hydrophobic TMBPA systems showed improved performance at higher methanol concentrations. (C) 2014 The Electrochemical Society. C1 [Rowlett, Jarrett R.; Chen, Yu; Shaver, Andrew T.; Fahs, Gregory B.; Sundell, Benjamin J.; Moore, Robert B.; Mecham, Sue; McGrath, James E.] Virginia Polytech Inst & State Univ, Macromol & Intofaces Inst, Dept Chem, Blacksburg, VA 24061 USA. [Li, Qing; Kim, Yu Seung; Zelenay, Piotr] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Rowlett, JR (reprint author), Virginia Polytech Inst & State Univ, Macromol & Intofaces Inst, Dept Chem, Blacksburg, VA 24061 USA. EM jmcgrath@vt.edu RI Moore, Robert/E-9619-2011; Li, Qing/G-4502-2011; Rowlett, Jarrett/B-8115-2017 OI Moore, Robert/0000-0001-9057-7695; Li, Qing/0000-0003-4807-030X; Rowlett, Jarrett/0000-0003-2775-696X FU US Department of Energy; LANL [DE-AC52-06NA25396]; National Science Foundation [DMR-1126534, DMR-0923107] FX The authors appreciate the support of this research by the US Department of Energy, in collaboration with LANL, under Contract DE-AC52-06NA25396. Additionally, for the SEC and SAXS experiments, the authors greatly acknowledge the financial support by the National Science Foundation under the grant No. DMR-1126534 (SEC) and DMR-0923107 (SAXS). NR 44 TC 7 Z9 7 U1 2 U2 25 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 2014 VL 161 IS 4 BP F535 EP F543 DI 10.1149/2.086404jes PG 9 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA AD8XR UT WOS:000333549500076 ER PT J AU Su, Q Gong, WQ Yoon, D Jacob, C Jia, QX Manthiram, A Jacobson, AJ Wang, HY AF Su, Qing Gong, Wenquan Yoon, Daeil Jacob, Clement Jia, Quanxi Manthiram, Arumugam Jacobson, Allan J. Wang, Haiyan TI Interlayer Effects on Oxygen Reduction Kinetics in Porous Electrodes of La0.5Sr0.5CoO3-delta SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID OXIDE FUEL-CELLS; THIN-FILM; SURFACE EXCHANGE; ELECTROCHEMICAL CHARACTERIZATION; LA0.6SR0.4CO0.2FE0.8O3 CATHODES; TEMPERATURE SOFCS; DIFFUSION; PEROVSKITES; NANOSCALE; MECHANISM AB Thick La0.5Sr0.5CoO3-delta (LSCO) cathodes (similar to 30 mu m) have been successfully fabricated with and without nanoporous LSCO interlayers on both sides of a dense polycrystalline gadolinia-doped ceria (CGO) substrate by combining screen printing and pulsed laser deposition (PLD) methods. The electrochemical properties of these LSCO cathodes for oxygen reduction reaction have been determined by electrochemical impedance spectroscopy (EIS) at different interlayer thicknesses, temperatures, and oxygen partial pressures. The oxygen reduction reaction on the LSCO electrode with and without the interlayer has been found to be mainly limited by the surface exchange process. By fitting the power density data by Butler-Volmer equation, it demonstrates that as the thickness of the PLD interlayer increases, the surface exchange resistance of the cathode decreases due to a significant increase in the number of reaction sites obtained by inserting the nanoporous LSCO interlayer. (C) 2014 The Electrochemical Society. All rights reserved. C1 [Su, Qing; Wang, Haiyan] Texas A&M Univ, Dept Mat Sci & Engn, College Stn, TX 77843 USA. [Gong, Wenquan; Jacobson, Allan J.] Univ Houston, Dept Chem, Houston, TX 77204 USA. [Gong, Wenquan; Jacobson, Allan J.] Univ Houston, Texas Ctr Superconduct, Houston, TX 77204 USA. [Yoon, Daeil; Manthiram, Arumugam] Univ Texas Austin, Electrochem Energy Lab, Austin, TX 78712 USA. [Yoon, Daeil; Manthiram, Arumugam] Univ Texas Austin, Mat Sci & Engn Program, Austin, TX 78712 USA. [Jacob, Clement; Wang, Haiyan] Texas A&M Univ, Dept Elect & Comp Engn, College Stn, TX 77843 USA. [Jia, Quanxi] Los Alamos Natl Lab, Ctr Integrated Nanotechnol CINT, Los Alamos, NM 87545 USA. RP Su, Q (reprint author), Texas A&M Univ, Dept Mat Sci & Engn, College Stn, TX 77843 USA. EM ajjacob@uh.edu; wangh@ece.tamu.edu RI Jia, Q. X./C-5194-2008; Su, Qing/N-2518-2014; Wang, Haiyan/P-3550-2014; Albe, Karsten/F-1139-2011 OI Wang, Haiyan/0000-0002-7397-1209; FU U.S. National Science Foundation [NSF-0846504, NSF 1007969]; Robert A. Welch Foundation [E-0024, F-1254]; U.S. Department of Energy (U.S. DOE), Office of Basic Energy Sciences, Division of Materials Sciences and Engineering [DESC0001284] FX The work was supported by the U.S. National Science Foundation (NSF-0846504 and NSF 1007969). A. J. J and W. G acknowledge the support from the Robert A. Welch Foundation (Grant No. E-0024) and the U.S. Department of Energy (U.S. DOE), Office of Basic Energy Sciences, Division of Materials Sciences and Engineering (under Award No. DESC0001284, impedance measurements and analysis). A. M. and D. Y acknowledge the support by the Robert A. Welch Foundation (Grant No. F-1254). The work at Los Alamos 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. NR 43 TC 1 Z9 1 U1 3 U2 20 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 2014 VL 161 IS 4 BP F398 EP F404 DI 10.1149/2.026404jes PG 7 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA AD8XR UT WOS:000333549500059 ER PT J AU Small, LJ Wheeler, DR AF Small, L. J. Wheeler, D. R. TI Influence of Analysis Method on the Experimentally Observed Capacitance at the Gold-Ionic Liquid Interface SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID CONSTANT-PHASE-ELEMENT; DOUBLE-LAYER CAPACITANCE; ELECTRICAL DOUBLE-LAYER; DIFFERENTIAL CAPACITANCE; IMPEDANCE SPECTROSCOPY; TEMPERATURE; ELECTRODE; SURFACE; RELAXATION; THICKNESS AB Diverse results have been reported on the differential capacitance of the metal-ionic liquid interface. Here the effect of the analysis method on the experimentally observed double layer capacitance is evaluated. A fast Fourier transform impedance spectroscopy technique allows the impedance-DC bias landscape of three 1-alkyl-3-methylimidazolium salts to be explored over a wide range of frequencies in a fraction of the time required for traditional impedance techniques. Analysis of this data set using four different methods found in the literature demonstrates how the assumptions inherent to each method alter the capacitance-DC bias curve. Careful consideration of these assumptions is necessary to compare results across the literature and understand the properties inherent to the solid-ionic liquid interface. (C) 2014 The Electrochemical Society. C1 [Small, L. J.; Wheeler, D. R.] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Small, LJ (reprint author), Sandia Natl Labs, POB 5800, Albuquerque, NM 87185 USA. EM ljsmall@sandia.gov OI Small, Leo/0000-0003-0404-6287 FU Laboratory Directed Research and Development (LDRD) program at Sandia National Laboratories; U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX This work was supported by the Laboratory Directed Research and Development (LDRD) program at Sandia National Laboratories. 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 32 TC 2 Z9 2 U1 0 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 2014 VL 161 IS 4 BP H260 EP H263 DI 10.1149/2.094404jes PG 4 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA AD8XR UT WOS:000333549500100 ER PT J AU Zhang, HJ Yuan, XX Ma, ZF Wen, W Yang, JH AF Zhang, Hui-Juan Yuan, Xianxia Ma, Zi-Feng Wen, Wen Yang, Junhe TI Investigation of Non-Precious Metal CoN4-Based Oxygen Reduction Catalyst by Electrochemical and X-ray Absorption Spectroscopy Techniques SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID PEM FUEL-CELLS; NITROGEN-CONTAINING CARBON; COBALT COMPOUNDS; O-2 REDUCTION; ACTIVE-SITES; ELECTROCATALYSTS; PERFORMANCE; POLYANILINE; PARTICLES; PYROLYSIS AB Electrochemical and X-ray absorption techniques are applied to determine the influence of pyrolysis and nitrogen-containing precursor loading on the catalytic activity and structure of carbon-supported cobalt triethylenetetramine (CoTETA/C) catalyst. These CoTETA/C catalysts with different nitrogen-containing precursor loadings are synthesized from pyrolyzing cobalt triethylenetetramine supported on carbon at 800 degrees C in Ar atmosphere. For comparison, the as-prepared (without pyrolysis) is also studied. Cyclic voltammograms and rotating disk electrode measurements indicate that the as-prepared presents very low activity, while the CoTETA/C catalysts. with different nitrogen-containing precursor loadings show good catalytic activity and the maximum is found for CoTETA/C catalyst with Co:TETA = 1:4. X-ray absorption measurements at Co and N K edges show that after pyrolysis the CoN4 centers are no longer detected along with little nitrogen atoms inserted into carbon matrix and nanometallic alpha-Co clusters are formed. X-ray diffraction also confirms the presence of nanometallic alpha-Co particles on the catalysts. (c) 2014 The Electrochemical Society. C1 [Zhang, Hui-Juan; Yang, Junhe] Univ Shanghai Sci & Technol, Sch Mat Sci & Engn, Shanghai 200093, Peoples R China. [Yuan, Xianxia; Ma, Zi-Feng] Shanghai Jiao Tong Univ, Dept Chem Engn, Shanghai 200240, Peoples R China. [Wen, Wen] Brookhaven Natl Lab, Upton, NY 11973 USA. RP Zhang, HJ (reprint author), Univ Shanghai Sci & Technol, Sch Mat Sci & Engn, Shanghai 200093, Peoples R China. EM zfma@sjtu.edu.cn; jhyang@usst.edu.cn RI Yuan, Xianxia/A-4256-2009 FU National Science Foundation of China [51102169, 51272157, 21176155]; Shanghai Science and Technology Program [13ZR1429000]; Shanghai College Teacher Scheme [slg 11028] FX This work is financial supported by the National Science Foundation of China (51102169, 51272157 and 21176155), Shanghai Science and Technology Program (13ZR1429000), and Shanghai College Teacher Scheme (slg 11028). NR 26 TC 1 Z9 1 U1 4 U2 27 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 2014 VL 161 IS 4 BP H155 EP H160 DI 10.1149/2.003404jes PG 6 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA AD8XR UT WOS:000333549500082 ER PT J AU Krejci, AJ Yager, KG Ruggiero, C Dickerson, JH AF Krejci, Alex J. Yager, Kevin. G. Ruggiero, Christopher Dickerson, James H. TI X-ray scattering as a liquid and solid phase probe of ordering within sub-monolayers of iron oxide nanoparticles fabricated by electrophoretic deposition SO NANOSCALE LA English DT Article ID MONODISPERSE NANOCRYSTALS; COLLOID MONOLAYERS; SUPERLATTICES; COATINGS; CDSE; TRANSPORT; CERAMICS; CRYSTALS; POWDER; SCALES AB Order within sub-monolayers of nanoparticles, fabricated by electrophoretic deposition, was assessed during nanoparticle deposition in a liquid suspension and after the films had dried by grazing-incidence small-angle X-ray scattering. Experiments were performed in a custom-made, liquid-phase cell. The results indicated that ordering occurred during the drying event. C1 [Krejci, Alex J.; Dickerson, James H.] Vanderbilt Univ, Dept Phys & Astron, Nashville, TN 37235 USA. [Krejci, Alex J.; Dickerson, James H.] Vanderbilt Univ, Vanderbilt Inst Nanoscale Sci & Engn, Nashville, TN 37235 USA. [Yager, Kevin. G.; Ruggiero, Christopher; Dickerson, James H.] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. RP Dickerson, JH (reprint author), Vanderbilt Univ, Dept Phys & Astron, Nashville, TN 37235 USA. EM jdickerson@bnl.gov RI Dickerson, James/F-7950-2013; Yager, Kevin/F-9804-2011 OI Dickerson, James/0000-0001-9636-6303; Yager, Kevin/0000-0001-7745-2513 FU United States National Science Foundation [DMR-1054161]; U.S. Department of Energy, Office of Basic Energy Sciences [DE-AC02-98CH10886] FX This research was supported by the United States National Science Foundation CAREER Award (DMR-1054161). Research carried out in part at the Center for Functional Nanomaterials and the National Synchrotron Light Source, Brookhaven National Laboratory, which are supported by the U.S. Department of Energy, Office of Basic Energy Sciences, under contract no. DE-AC02-98CH10886. NR 43 TC 3 Z9 3 U1 2 U2 10 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 2014 VL 6 IS 8 BP 4047 EP 4051 DI 10.1039/c4nr00645c PG 5 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA AD9EJ UT WOS:000333567300018 PM 24599306 ER PT J AU Annesley, CJ Goldsmith, CF Tranter, RS AF Annesley, Christopher J. Goldsmith, C. Franklin Tranter, Robert S. TI A shock tube laser schlieren study of methyl acetate dissociation in the fall-off regime SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID RATE CONSTANTS; RATE COEFFICIENTS; DECOMPOSITION; COMBUSTION; OXIDATION; RADICALS; METHANOL; BIODIESEL; MECHANISM; PATHWAYS AB The pyrolysis of methyl acetate, 2% and 4% dilute in krypton, was investigated in a diaphragmless shock tube (DFST) using laser schlieren densitometry (LS). Experiments were performed at 122 +/- 3 and 63 +/- 2 Torr over the temperature range of 1492-2266 K. Master equation models for the four main dissociation paths of methyl acetate based on a prior study by Peukert et al. [S. Peukert, R. Sivaramakrishnan, M. Su and J. Michael, Combust. Flame, 2012, 159, 2312-2323] were refined and formed the basis for simulating the LS experiments. The density gradient profiles from the LS experiments indicate that the initial dissociation proceeds predominantly by breakage of the C-O bond leading ultimately to two methyl radicals and CO2, accounting for 83-88% of the methyl acetate loss over this temperature range. Rate coefficients for dissociation of methyl acetate were satisfactorily simulated with a master equation model, with modelled rate coefficients of k(120) Torr = 9.06 x 10(81) x T-19.07 x exp(-61600K/T) s(-1), k(60) Torr = 3.71 x 10(82) x T-19.34 x exp(-61200K/T) s(-1), and of k(infinity) = 1.97 x 10(30) x T-3.80 x exp(-47900K/T) s(-1) for the major channel, based on fitting to 120 Torr and 60 Torr data taken in this study. The model also captures the pressure dependency of methyl acetate dissociation and resolves an earlier discrepancy concerning the mechanism of dissociation of methyl acetate. C1 [Annesley, Christopher J.; Goldsmith, C. Franklin; Tranter, Robert S.] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. RP Tranter, RS (reprint author), Argonne Natl Lab, Chem Sci & Engn Div, 9700 S Cass Ave, 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]; Argonne Director's Postdoctoral Fellowship 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. CFG gratefully acknowledges financial support from the Argonne Director's Postdoctoral Fellowship. The authors kindly thank Dr Raghu Sivaramakrishnan for sharing the RRKM/ME input files and many helpful discussions. We are grateful to Prof. Ronald K. Hanson and Dr David F Davidson for providing the experimental data in Fig. 8. NR 31 TC 3 Z9 3 U1 3 U2 24 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 2014 VL 16 IS 16 BP 7241 EP 7250 DI 10.1039/c3cp55297g PG 10 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AD8NS UT WOS:000333523500010 PM 24608752 ER PT J AU Cui, GF Liu, SF Wang, KM Li, Q Wu, G AF Cui, Guofeng Liu, Shaofang Wang, Kaiming Li, Qing Wu, Gang TI Discovering p-doped mechanism in non-magnetic Ni-P films for HDD substrate: a combined experimental and theoretical study SO RSC ADVANCES LA English DT Article ID ELECTROLESS DEPOSITION PROCESS; OXIDATION MECHANISM; DIMETHYLAMINE BORANE; AMMONIACAL SOLUTIONS; REDUCTANT; DENSITY; ALLOYS; NICKEL; ELECTRODEPOSITION; EXCHANGE AB In this work, a new mechanism is proposed for the redox of hypophosphorous acid catalyzed by a nickel cluster through a combined study of density functional theory (DFT) calculations and electrochemical impedance spectroscopy (EIS) measurements. The DFT results indicate that the concentration of OH- is a crucial species to control the oxidation and reduction of hypophosphorous acid. The oxidation of hypophosphorous acid takes place preferably at higher OH- concentration, as OH- can combine directly with H3PO2 and hydrogen radical (H-center dot). In contrast, reduction is inhibited in this case because the hydrogen radical preferably combines with OH- rather than H3PO2. Thus, pH serves as a key switch to control the pathways of the coupling reaction. EIS results demonstrated that the electroless nickel process includes three electrochemical processes: charge-discharge of electrical double layer, Ni(I) transforming to Ni(II) or Ni(0), and specific adsorption of intermediate products. In good agreement with theoretical prediction, the experimental measurements indicated that an electroless nickel coating with high phosphorus content was successfully synthesized at a low pH, exhibiting non-magnetic properties and enabling its use as a non-magnetic coating for hard disk drive substrates. C1 [Cui, Guofeng; Liu, Shaofang] Sun Yat Sen Univ, Sch Chem & Chem Engn, Key Lab Low Carbon Chem & Energy Conservat Guangd, Guangzhou 510275, Guangdong, Peoples R China. [Wang, Kaiming] Shanghai Jiao Tong Univ, Sch Elect Informat & Elect Engn, Shanghai 200240, Peoples R China. [Li, Qing; Wu, Gang] Los Alamos Natl Lab, Mat Phys & Applicat Div, Los Alamos, NM 87545 USA. RP Cui, GF (reprint author), Sun Yat Sen Univ, Sch Chem & Chem Engn, Key Lab Low Carbon Chem & Energy Conservat Guangd, Guangzhou 510275, Guangdong, Peoples R China. EM cuigf@mail.sysu.edu.cn RI Wu, Gang/E-8536-2010; Li, Qing/G-4502-2011 OI Wu, Gang/0000-0003-4956-5208; Li, Qing/0000-0003-4807-030X FU National Natural Science Foundation of China [51271205]; "Fundamental Research Funds for the Central Universities" [11lgpy08]; "GuangZhou Pearl Technology the Nova Special Project" [2012J2200058]; "Research and Application of Key Technologies Oriented the Industrial Development" [90035-3283309, 90035-3283321]; "Plan of Science and Technology Project" of the DaYa Gulf District in Huizhou City [31000-4207387] FX Dr G. F. Cui gratefully acknowledges the financial support from the National Natural Science Foundation of China (51271205), the "Fundamental Research Funds for the Central Universities" (11lgpy08), the "GuangZhou Pearl Technology the Nova Special Project" (2012J2200058), the "Research and Application of Key Technologies Oriented the Industrial Development" (90035-3283309, 90035-3283321), and the "Plan of Science and Technology Project" of the DaYa Gulf District in Huizhou City (31000-4207387). NR 22 TC 0 Z9 0 U1 1 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 2014 VL 4 IS 28 BP 14663 EP 14672 DI 10.1039/c3ra47217e PG 10 WC Chemistry, Multidisciplinary SC Chemistry GA AD8OX UT WOS:000333526600049 ER PT J AU Quiroz-Guzman, M Fagnant, DP Chen, XY Shi, CJ Brennecke, JF Goff, GS Runde, W AF Quiroz-Guzman, Mauricio Fagnant, Daniel P., Jr. Chen, Xiao-Yan Shi, Chaojun Brennecke, Joan F. Goff, George S. Runde, Wolfgang TI Synthesis and characterization of the thermodynamic and electrochemical properties of tetra-alkyl phosphonium oxalate ionic liquids SO RSC ADVANCES LA English DT Article ID MOLECULAR-STRUCTURE; CRYSTAL-STRUCTURE; HYDROGEN-BOND; COMPLEXES; AMMONIUM; LITHIUM; SALTS; CATALYSIS; RAMAN; ELECTRODEPOSITION AB Ionic liquids (ILs) are attractive alternatives to water, high temperature molten salts or conventional organic solvents for electrodeposition of technologically important metals. Designing ILs containing functional groups specifically targeted to interact with or even chelate metals, such as carboxylate, may increase the metal solubility and affect thermodynamic and electrochemical properties. This paper reports the synthesis and characterization of three ionic liquids comprised of one or two tetra-alkyl phosphonium cations paired with a hydrogen oxalate or oxalate anion, with the general formula [(P-RRRR')(x)][C2O4H2-x], R = 4,6 and R' = 4, 14. These compounds were characterized by H-1, C-13, P-31 NMR, and Raman spectroscopy. Electrochemical windows, electrical conductivities, densities and viscosities were also determined experimentally. Thermal gravimetric analysis (TGA) revealed decomposition temperatures above 200 degrees C and differential scanning calorimetry (DSC) analysis revealed that the two [(P-66614)(x)][C2O4H2-x] salts have similar glass transition temperatures while [(P-4444)(2)][C2O4] has a melting point above room temperature. Raman and powder X-ray diffraction spectroscopy confirm that Nd2O3 dissolves and complexes with [P-66614][C2O4]. C1 [Quiroz-Guzman, Mauricio; Fagnant, Daniel P., Jr.; Shi, Chaojun; Brennecke, Joan F.] Univ Notre Dame, Dept Chem & Biomol Engn, Notre Dame, IN 46556 USA. [Chen, Xiao-Yan; Goff, George S.] Los Alamos Natl Lab, Div Chem, Los Alamos, NM 87545 USA. [Chen, Xiao-Yan; Goff, George S.; Runde, Wolfgang] Los Alamos Natl Lab, Sci Program Off, Los Alamos, NM 87545 USA. RP Brennecke, JF (reprint author), Univ Notre Dame, Dept Chem & Biomol Engn, 182 Fitzpatrick Hall, Notre Dame, IN 46556 USA. EM mquirozg@nd.edu; jfb@nd.edu; georgeg@lanl.gov; runde@lanl.gov FU Los Alamos Laboratory Directed Research and Development Program; G. T. Seaborg Institute for Transactinium Science at Los Alamos National Laboratory FX The authors gratefully acknowledge the Los Alamos Laboratory Directed Research and Development Program and the G. T. Seaborg Institute for Transactinium Science at Los Alamos National Laboratory for financial support during this project. NR 62 TC 4 Z9 4 U1 3 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 2014 VL 4 IS 29 BP 14840 EP 14846 DI 10.1039/c4ra01467g PG 7 WC Chemistry, Multidisciplinary SC Chemistry GA AD8PU UT WOS:000333528900005 ER PT J AU Nguyen, MC Zhao, X Wang, CZ Ho, KM AF Manh Cuong Nguyen Zhao, Xin Wang, Cai-Zhuang Ho, Kai-Ming TI New Be-intercalated hexagonal boron layer structure of BeB2 SO RSC ADVANCES LA English DT Article ID AUGMENTED-WAVE METHOD; BERYLLIUM-BORON; SUPERCONDUCTIVITY; SYSTEMS; CAB2 AB Using a genetic algorithm method and first-principle calculations, we performed searches for low-energy crystal structures of BeB2. We found a new family of structures, where the B atoms form hexagonal layers intercalated by Be atoms. The lowest-energy structure has a formation energy of -99.47 meV per atom with 4 formula units in the unit cell, which is much more stable than the models proposed before. The formation energies of structures in the new structure family can be well described by an Ising-like model with "anti-ferromagnetic" coupling between the displacements of Be atoms from the mid-plane between two B layers. We also performed phonon calculations as well as electronic band structure calculations to verify the stability and investigate the electronic properties of the newly found structure. C1 [Manh Cuong Nguyen] Iowa State Univ, Ames Lab, US DOE, Ames, IA 50011 USA. Iowa State Univ, Dept Phys & Astron, Ames, IA 50011 USA. RP Nguyen, MC (reprint author), Iowa State Univ, Ames Lab, US DOE, Ames, IA 50011 USA. EM mcnguyen@ameslab.gov RI Nguyen, Manh Cuong/G-2783-2015; OI Nguyen, Manh Cuong/0000-0001-8027-9029; Zhao, Xin/0000-0002-3580-512X FU U.S. Department of Energy, Office of Basic Energy Science, Division of Materials Science and Engineering; DOE [DE-AC02-07CH11358]; National Energy Research Scientific Computing Center (NERSC) FX The U.S. Department of Energy, Office of Basic Energy Science, Division of Materials Science and Engineering supported the research at the Ames Laboratory, which is operated for the DOE by Iowa State University under Contract No. DE-AC02-07CH11358, with an additional computing grant through the National Energy Research Scientific Computing Center (NERSC). NR 33 TC 1 Z9 1 U1 3 U2 22 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 2014 VL 4 IS 29 BP 15061 EP 15065 DI 10.1039/c4ra00114a PG 5 WC Chemistry, Multidisciplinary SC Chemistry GA AD8PU UT WOS:000333528900038 ER PT J AU Luce, R Ng, EG AF Luce, Robert Ng, Esmond G. TI ON THE MINIMUM FLOPS PROBLEM IN THE SPARSE CHOLESKY FACTORIZATION SO SIAM JOURNAL ON MATRIX ANALYSIS AND APPLICATIONS LA English DT Article DE sparse Cholesky factorization; minimum fill; minimum operation count; computational complexity ID DEGREE ORDERING ALGORITHM; FILL-IN; ELIMINATION; GRAPHS; TREE AB Prior to computing the Cholesky factorization of a sparse symmetric positive definite matrix, a reordering of the rows and columns is computed so as to reduce both the number of fill elements in Cholesky factor and the number of arithmetic operations (FLOPs) in the numerical factorization. These two metrics are clearly somehow related and yet it is suspected that these two problems are different. However, no rigorous theoretical treatment of the relation of these two problems seems to have been given yet. In this paper we show by means of an explicit, scalable construction that the two problems are different in a very strict sense: no ordering is optimal for both fill and FLOPs in the constructed graph. Further, it is commonly believed that minimizing the number of FLOPs is no easier than minimizing the fill (in the complexity sense), but so far no proof appears to be known. We give a reduction chain that shows the NP hardness of minimizing the number of arithmetic operations in the Cholesky factorization. C1 [Luce, Robert] TU Berlin, Inst Math, D-10623 Berlin, Germany. [Ng, Esmond G.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Computat Res Div, Berkeley, CA 94720 USA. RP Luce, R (reprint author), TU Berlin, Inst Math, MA 3-3, D-10623 Berlin, Germany. EM luce@math.tu-berlin.de; EGNg@lbl.gov OI Luce, Robert/0000-0001-6960-9656 FU Deutsche Forschungsgemeinschaft, Cluster of Excellence "UniCat"; Scientific Discovery through Advanced Computing Program in the Offices of Advanced Scientific Computing Research in the Office of Science, US Department of Energy under Lawrence Berkeley National Laboratory [DE-AC02-05CH11231] FX This work was supported by Deutsche Forschungsgemeinschaft, Cluster of Excellence "UniCat".; This work was supported in part by the Scientific Discovery through Advanced Computing Program in the Offices of Advanced Scientific Computing Research in the Office of Science, US Department of Energy under contract no. DE-AC02-05CH11231 at Lawrence Berkeley National Laboratory. NR 24 TC 3 Z9 3 U1 0 U2 2 PU SIAM PUBLICATIONS PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA SN 0895-4798 EI 1095-7162 J9 SIAM J MATRIX ANAL A JI SIAM J. Matrix Anal. Appl. PY 2014 VL 35 IS 1 BP 1 EP 21 DI 10.1137/130912438 PG 21 WC Mathematics, Applied SC Mathematics GA AE0YW UT WOS:000333693300001 ER PT J AU Vassilevski, PS Villa, U AF Vassilevski, Panayot S. Villa, Umberto TI A MIXED FORMULATION FOR THE BRINKMAN PROBLEM SO SIAM JOURNAL ON NUMERICAL ANALYSIS LA English DT Article DE Brinkman problem; Stokes-Darcy coupling; saddle point problems; block preconditioners; algebraic multigrid ID ELEMENT EXTERIOR CALCULUS; NAVIER-STOKES EQUATIONS; AUXILIARY SPACE AMG; MAXWELL EQUATIONS; VOLUME DISTRIBUTION; HODGE THEORY; TINY HOLES; FINITE; H(DIV); HOMOGENIZATION AB The Brinkman model is a unified law governing the flow of a viscous fluid in an inhomogeneous medium, where fractures, bubbles, or channels alternate inside a porous matrix. In this work, we explore a novel mixed formulation of the Brinkman problem based on the Hodge decomposition of the vector Laplacian. Introducing the flow's vorticity as an additional unknown, this formulation allows for a uniformly stable and conforming discretization by standard finite elements (Nedelec, Raviart-Thomas, piecewise discontinuous). A priori error estimates for the discretization error in the H(curl; Omega)-H(div; Omega)-L-2(Omega) norm of the solution, which are optimal with respect to the approximation properties of finite element spaces, are obtained. The theoretical results are illustrated with numerical experiments. Finally, the proposed formulation allows for a scalable block diagonal preconditioner which takes advantage of the auxiliary space algebraic multigrid solvers for H(curl) and H(div) problems available in the preconditioning library hypre (http://llnl.gov/CASC/hypre), as shown in a follow-up paper [P. S. Vassilevski and U. Villa, SIAM J. Sci. Comput., 35 (2013), pp. S3-S17]. C1 [Vassilevski, Panayot S.; Villa, Umberto] Lawrence Livermore Natl Lab, Ctr Appl Sci Comp, Livermore, CA 94551 USA. RP Vassilevski, PS (reprint author), Lawrence Livermore Natl Lab, Ctr Appl Sci Comp, Livermore, CA 94551 USA. EM panayot@llnl.gov; villa13@llnl.gov RI Villa, Umberto/C-7956-2014 FU U.S. Department of Energy by the Lawrence Livermore National Laboratory [DE-AC52-07NA27344] FX This work was performed under the auspices of the U.S. Department of Energy by the Lawrence Livermore National Laboratory under contract DE-AC52-07NA27344. NR 49 TC 6 Z9 6 U1 0 U2 5 PU SIAM PUBLICATIONS PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA SN 0036-1429 EI 1095-7170 J9 SIAM J NUMER ANAL JI SIAM J. Numer. Anal. PY 2014 VL 52 IS 1 BP 258 EP 281 DI 10.1137/120884109 PG 24 WC Mathematics, Applied SC Mathematics GA AD7CP UT WOS:000333419300015 ER PT J AU Anitescu, M Zeng, XY Constantinescu, EM AF Anitescu, Mihai Zeng, Xiaoyan Constantinescu, Emil M. TI A LOW-MEMORY APPROACH FOR BEST-STATE ESTIMATION OF HIDDEN MARKOV MODELS WITH MODEL ERROR SO SIAM JOURNAL ON NUMERICAL ANALYSIS LA English DT Article DE data assimilation; weakly constrained 4D-Var; hidden Markov models; limited-memory methods; quasi-Newton methods ID DATA ASSIMILATION; THEORETICAL ASPECTS; 4D-VAR; UNCERTAINTY; ALGORITHMS; WEATHER; SYSTEM; FLOW AB We present a low-memory approach for the best-state estimate (data assimilation) of hidden Markov models where model error is considered. In particular, our findings apply to the 4D-Var framework. The novelty of our approach resides in the fact that the storage needed by our estimation framework, while including model error, is dramatically reduced from O(number of time steps) to O(1). The main insight is that we can restate the objective function of the state estimation (the likelihood function) from a function of all states to a function of the initial state only. We do so by restricting the other states by recursively enforcing the optimality conditions. This results in a regular nonlinear equation or an optimization problem for which a descent direction can be computed using only a forward sweep. In turn, the best estimate can be obtained locally by limited-memory quasi-Newton algorithms that need only O(1) storage with respect to the time steps. Our findings are demonstrated by numerical experiments on Burgers' equations. C1 [Anitescu, Mihai; Zeng, Xiaoyan; Constantinescu, Emil M.] Argonne Natl Lab, Math & Comp Sci Div, Argonne, IL 60439 USA. [Zeng, Xiaoyan] Shanghai Univ, Dept Math, Shanghai, Peoples R China. RP Zeng, XY (reprint author), Shanghai Univ, Dept Math, Shanghai, Peoples R China. EM anitescu@mcs.anl.gov; cherryzxy@shu.edu.cn; emconsta@mcs.anl.gov FU Department of Energy [DE-AC02-06CH11357] FX This work was supported by the Department of Energy under contract DE-AC02-06CH11357. NR 28 TC 1 Z9 1 U1 1 U2 1 PU SIAM PUBLICATIONS PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA SN 0036-1429 EI 1095-7170 J9 SIAM J NUMER ANAL JI SIAM J. Numer. Anal. PY 2014 VL 52 IS 1 BP 468 EP 495 DI 10.1137/120870451 PG 28 WC Mathematics, Applied SC Mathematics GA AD7CP UT WOS:000333419300025 ER PT J AU Zavala, VM Anitescu, M AF Zavala, Victor M. Anitescu, Mihai TI SCALABLE NONLINEAR PROGRAMMING VIA EXACT DIFFERENTIABLE PENALTY FUNCTIONS AND TRUST-REGION NEWTON METHODS SO SIAM JOURNAL ON OPTIMIZATION LA English DT Article DE scalable; nonlinear programming; exact differentiable penalty; trust region; Newton; iterative linear algebra ID MODEL-PREDICTIVE CONTROL; LINEAR COMPLEMENTARITY-PROBLEMS; CONSTRAINED OPTIMIZATION; ALGORITHM; CONVERGENCE; STRATEGIES; EQUATIONS; SYSTEMS AB We present an approach for nonlinear programming based on the direct minimization of an exact differentiable penalty function using trust-region Newton techniques. The approach provides desirable features required for scalability: it can detect and exploit directions of negative curvature, it is superlinearly convergent, and it enables the scalable computation of the Newton step through iterative linear algebra. Moreover, it presents features that are desirable for parametric optimization problems that must be solved in a latency-limited environment, as is the case for model predictive control and mixed-integer nonlinear programming. These features are fast detection of activity, efficient warm starting, and progress on a primal-dual merit function at every iteration. We note that other algorithmic approaches fail to satisfy at least one of these features. We derive general convergence results for our approach and demonstrate its behavior through numerical studies. C1 [Zavala, Victor M.; Anitescu, Mihai] Argonne Natl Lab, Div Math & Comp Sci, Argonne, IL 60439 USA. RP Zavala, VM (reprint author), Argonne Natl Lab, Div Math & Comp Sci, 9700 S Cass Ave, Argonne, IL 60439 USA. EM vzavala@mcs.anl.gov; anitescu@mcs.anl.gov NR 50 TC 3 Z9 3 U1 1 U2 4 PU SIAM PUBLICATIONS PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA SN 1052-6234 EI 1095-7189 J9 SIAM J OPTIMIZ JI SIAM J. Optim. PY 2014 VL 24 IS 1 BP 528 EP 558 DI 10.1137/120888181 PG 31 WC Mathematics, Applied SC Mathematics GA AE1WF UT WOS:000333761700021 ER PT J AU Chen, J Wang, L Anitescu, M AF Chen, Jie Wang, Lei Anitescu, Mihai TI A FAST SUMMATION TREE CODE FOR MATERN KERNEL SO SIAM JOURNAL ON SCIENTIFIC COMPUTING LA English DT Article DE Matern kernel; Gaussian process; fast summation; tree code ID MULTIPOLE ALGORITHM; CARTESIAN TREECODE; INTEGRAL-EQUATIONS; 3 DIMENSIONS; MATRICES; APPROXIMATION; SOLVER AB The Matern family of functions is a widely used covariance kernel in spatial statistics for Gaussian process modeling, which in many instances requires calculations with a covariance matrix. In this paper, we design a fast summation algorithm for the Matern kernel in order to efficiently perform matrix-vector multiplications. This algorithm is based on the Barnes-Hut tree code framework and addresses several practical issues: the anisotropy of the kernel, the nonuniform distribution of the point set, and a tight error estimate of the approximation. Even though the algorithmic details differ from the standard tree code in several aspects, empirically the computational cost of our algorithm scales as O(n log n) for n points. Comprehensive numerical experiments are shown to demonstrate the practicality of the design. C1 [Chen, Jie; Anitescu, Mihai] Argonne Natl Lab, Div Math & Comp Sci, Argonne, IL 60439 USA. [Wang, Lei] Univ Wisconsin, Dept Math Sci, Milwaukee, WI 53211 USA. RP Chen, J (reprint author), Argonne Natl Lab, Div Math & Comp Sci, 9700 S Cass Ave, Argonne, IL 60439 USA. EM jiechen@mcs.anl.gov; wang256@uwm.edu; anitescu@mcs.anl.gov FU U.S. Department of Energy [DE-AC02-06CH11357] FX The submitted manuscript was created by the University of Chicago as an operator of Argonne National Laboratory under contract DE-AC02-06CH11357 with the U.S. Department of Energy. 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 35 TC 6 Z9 6 U1 0 U2 4 PU SIAM PUBLICATIONS PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA SN 1064-8275 EI 1095-7197 J9 SIAM J SCI COMPUT JI SIAM J. Sci. Comput. PY 2014 VL 36 IS 1 BP A289 EP A309 DI 10.1137/120903002 PG 21 WC Mathematics, Applied SC Mathematics GA AD7BI UT WOS:000333415500014 ER PT J AU Vecharynski, E Saad, Y Sosonkina, M AF Vecharynski, Eugene Saad, Yousef Sosonkina, Masha TI GRAPH PARTITIONING USING MATRIX VALUES FOR PRECONDITIONING SYMMETRIC POSITIVE DEFINITE SYSTEMS SO SIAM JOURNAL ON SCIENTIFIC COMPUTING LA English DT Article DE graph partitioning; iterative linear system solution; preconditioning; Cauchy-Bunyakowski-Schwarz (CBS) constant; symmetric positive definite; spectral partitioning ID IRREGULAR GRAPHS; EIGENVECTORS; SCHEME AB Prior to the parallel solution of a large linear system, it is required to perform a partitioning of its equations/unknowns. Standard partitioning algorithms are designed using the considerations of the efficiency of the parallel matrix-vector multiplication, and typically disregard the information on the coefficients of the matrix. This information, however, may have a significant impact on the quality of the preconditioning procedure used within the chosen iterative scheme. In the present paper, we suggest a spectral partitioning algorithm, which takes into account the information on the matrix coefficients and constructs partitions with respect to the objective of enhancing the quality of the nonoverlapping additive Schwarz (block Jacobi) preconditioning for symmetric positive definite linear systems. For a set of test problems with large variations in magnitudes of matrix coefficients, our numerical experiments demonstrate a noticeable improvement in the convergence of the resulting solution scheme when using the new partitioning approach. C1 [Vecharynski, Eugene] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Computat Res Div, Berkeley, CA 94720 USA. [Saad, Yousef] Univ Minnesota, Dept Comp Sci & Engn, Minneapolis, MN 55455 USA. [Sosonkina, Masha] Old Dominion Univ, Dept Modeling Simulat & Visualizat Engn, Norfolk, VA 23529 USA. RP Vecharynski, E (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Computat Res Div, Berkeley, CA 94720 USA. EM eugene.vecharynski@gmail.com; saad@cs.umn.edu; msosonki@odu.edu FU Iowa State University [DE-AC02-07CH11358]; Office of Science, Division of Mathematical, Information, and Computational Sciences of the U.S. Department of Energy [DE-AC02-05CH11231]; U.S. Department of Energy [DE-FG-08ER25841] FX This work was supported in part by Iowa State University under the contract DE-AC02-07CH11358 with the U.S. Department of Energy and by the Director, Office of Science, Division of Mathematical, Information, and Computational Sciences of the U.S. Department of Energy under contract number DE-AC02-05CH11231 and by the U.S. Department of Energy under grant DE-FG-08ER25841. NR 39 TC 8 Z9 8 U1 0 U2 2 PU SIAM PUBLICATIONS PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA SN 1064-8275 EI 1095-7197 J9 SIAM J SCI COMPUT JI SIAM J. Sci. Comput. PY 2014 VL 36 IS 1 BP A63 EP A87 DI 10.1137/120898760 PG 25 WC Mathematics, Applied SC Mathematics GA AD7BI UT WOS:000333415500004 ER PT J AU Ahn, HS Davenport, TC Tilley, TD AF Ahn, Hyun S. Davenport, Timothy C. Tilley, T. Don TI Molecular cobalt electrocatalyst for proton reduction at low overpotential SO CHEMICAL COMMUNICATIONS LA English DT Article ID HYDROGEN-PRODUCTION; COMPLEXES; EVOLUTION AB Linear trimetallic Co-III/Co-II/Co-III cobalt complexes with bridging acyl-alkoxy ligands are electrocatalysts for the reduction of tosic acid in acetonitrile. The -OCMe2CH2COMe complex appears to operate homogeneously, and at a modest onset overpotential of 175 mV. A turnover frequency of ca. 80 s(-1) was observed at an overpotential of 300 mV. C1 [Ahn, Hyun S.; Davenport, Timothy C.; Tilley, T. Don] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Ahn, Hyun S.; Davenport, Timothy C.; Tilley, T. Don] Univ Calif Berkeley, Dept Chem Engn, Berkeley, CA 94720 USA. [Ahn, Hyun S.; Davenport, Timothy C.; Tilley, T. Don] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. RP Tilley, TD (reprint author), Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. EM tdtilley@berkeley.edu FU Office of Science, Office of Basic Energy Sciences of the U.S. Department of Energy [DE-AC0205CH11231] FX This work was supported by the Director, Office of Science, Office of Basic Energy Sciences of the U.S. Department of Energy under Contract No. DE-AC0205CH11231. The authors would like to acknowledge Professor Peidong Yang for the use of TEM. The authors also thank Dr Pascual Ona-Burgos for helpful discussions and advice. NR 21 TC 8 Z9 8 U1 2 U2 23 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 2014 VL 50 IS 29 BP 3834 EP 3837 DI 10.1039/c3cc49682a PG 4 WC Chemistry, Multidisciplinary SC Chemistry GA AD2BE UT WOS:000333037000017 PM 24589710 ER PT J AU Tulli, LG Moridi, N Wang, WJ Helttunen, K Neuburger, M Vaknin, D Meier, W Shahgaldian, P AF Tulli, Ludovico G. Moridi, Negar Wang, Wenjie Helttunen, Kaisa Neuburger, Markus Vaknin, David Meier, Wolfgang Shahgaldian, Patrick TI Polymorphism control of an active pharmaceutical ingredient beneath calixarene-based Langmuir monolayers SO CHEMICAL COMMUNICATIONS LA English DT Article ID CRYSTALLIZATION; ACETAMINOPHEN; NUCLEATION; CACO3 AB This communication demonstrates the possibility to nucleate and grow different crystalline polymorphic forms of gabapentin (GBP) using, as nucleation templates, Langmuir monolayers of an amphiphilic calixarene at different packing densities. C1 [Tulli, Ludovico G.; Moridi, Negar; Shahgaldian, Patrick] Univ Appl Sci & Arts Northwestern Switzerland, Sch Life Sci, Inst Chem & Bioanalyt, Muttenz, Switzerland. [Wang, Wenjie; Vaknin, David] Iowa State Univ, Ames Lab, Ames, IA USA. [Wang, Wenjie; Vaknin, David] Iowa State Univ, Dept Phys & Astron, Ames, IA USA. [Helttunen, Kaisa] Univ Jyvaskyla, Dept Chem, Nanosci Ctr, SF-40351 Jyvaskyla, Finland. [Neuburger, Markus; Meier, Wolfgang] Univ Basel, Dept Chem, CH-4003 Basel, Switzerland. RP Shahgaldian, P (reprint author), Univ Appl Sci & Arts Northwestern Switzerland, Sch Life Sci, Inst Chem & Bioanalyt, Muttenz, Switzerland. EM patrick.shahgaldian@fhnw.ch RI Helttunen, Kaisa/F-5615-2014; Shahgaldian, Patrick/C-2928-2015; Vaknin, David/B-3302-2009 OI Helttunen, Kaisa/0000-0001-7455-4207; Shahgaldian, Patrick/0000-0002-1743-0387; Vaknin, David/0000-0002-0899-9248 FU Swiss Nanoscience Institute (SNI); Swiss National Science Foundation (SNSF); Office of Basic Energy Sciences, U.S. Department of Energy [DEAC02-07CH11358]; U.S. Department of Energy, Basic Energy Sciences, Office of Science [DE-AC02-06CH11357] FX The financial support from the Swiss Nanoscience Institute (SNI) and the Swiss National Science Foundation (SNSF) is gratefully acknowledged. The work at the Ames Laboratory is supported by the Office of Basic Energy Sciences, U.S. Department of Energy under Contract No. DEAC02-07CH11358. X-ray diffraction at the Advanced Photon Source is supported by the U.S. Department of Energy, Basic Energy Sciences, Office of Science, under Contract No. DE-AC02-06CH11357. NR 20 TC 5 Z9 5 U1 1 U2 24 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 2014 VL 50 IS 30 BP 3938 EP 3940 DI 10.1039/c4cc00928b PG 3 WC Chemistry, Multidisciplinary SC Chemistry GA AD3EY UT WOS:000333122300010 PM 24599407 ER PT J AU Harschneck, T Zhou, NJ Manley, EF Lou, SJ Yu, XG Butler, MR Timalsina, A Turrisi, R Ratner, MA Chen, LX Chang, RPH Facchetti, A Marks, TJ AF Harschneck, Tobias Zhou, Nanjia Manley, Eric F. Lou, Sylvia J. Yu, Xinge Butler, Melanie R. Timalsina, Amod Turrisi, Riccardo Ratner, Mark A. Chen, Lin X. Chang, Robert P. H. Facchetti, Antonio Marks, Tobin J. TI Substantial photovoltaic response and morphology tuning in benzo[ 1,2-b: 6,5-b']-dithiophene (bBDT) molecular donors SO CHEMICAL COMMUNICATIONS LA English DT Article ID ORGANIC SOLAR-CELLS; BACKBONE CURVATURE; EFFICIENCY; DIKETOPYRROLOPYRROLE; ADDITIVES; POLYMERS; BANDGAP; LEVEL AB The influence of solubilizing substituents on the photovoltaic performance and thin-film blend morphology of new benzo[ 1,2-b: 6,5-b']dithiophene (bBDT) based small molecule donor semiconductors is investigated. Solar cells based on bBDT(TDPP) (2)- PC71BM with two different types of side chains exhibit high power conversion efficiencies, up to 5.53%. C1 [Harschneck, Tobias; Zhou, Nanjia; Manley, Eric F.; Lou, Sylvia J.; Yu, Xinge; Butler, Melanie R.; Timalsina, Amod; Turrisi, Riccardo; Ratner, Mark A.; Chen, Lin X.; Facchetti, Antonio; Marks, Tobin J.] Northwestern Univ, Dept Chem, Evanston, IL 60208 USA. [Manley, Eric F.; Lou, Sylvia J.; Yu, Xinge; Butler, Melanie R.; Timalsina, Amod; Ratner, Mark A.; Chen, Lin X.; Facchetti, Antonio; Marks, Tobin J.] Northwestern Univ, Argonne Northwestern Solar Energy Res Ctr, Evanston, IL 60208 USA. [Chen, Lin X.] Argonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USA. [Chang, Robert P. H.] Northwestern Univ, Dept Mat Sci & Engn, Evanston, IL 60208 USA. [Facchetti, Antonio] Polyera Corp, Skokie, IL 60077 USA. RP Ratner, MA (reprint author), Northwestern Univ, Dept Chem, 2145 Sheridan Rd, Evanston, IL 60208 USA. RI Zhou, Nanjia/F-5820-2014; Chang, R.P.H/B-7505-2009 OI Zhou, Nanjia/0000-0003-4493-1264; FU ANSER Center, an Energy Frontier Research Center; U. S. Department of Energy, Office of Science, and Office of Basic Energy Sciences [DE-SC0001059]; NSF; DAAD FX T. H. thanks DAAD for a postdoctoral fellowship. N.Z., E. F. M., A.T., and S. J. L. were supported as part of the ANSER Center, 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-SC0001059. M. R. B. thanks NSF for a predoctoral fellowship. NR 20 TC 25 Z9 25 U1 4 U2 40 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 2014 VL 50 IS 31 BP 4099 EP 4101 DI 10.1039/c3cc49620a PG 3 WC Chemistry, Multidisciplinary SC Chemistry GA AD3SP UT WOS:000333166700020 PM 24619285 ER PT J AU Jin, P Kumari, H Kennedy, S Barnes, CL Teat, SJ Dalgarno, SJ Atwood, JL AF Jin, Ping Kumari, Harshita Kennedy, Stuart Barnes, Charles L. Teat, Simon J. Dalgarno, Scott J. Atwood, Jerry L. TI Structural alteration of the metal-organic pyrogallol[4]arene nano-capsule motif by incorporation of large metal centres SO CHEMICAL COMMUNICATIONS LA English DT Article ID MOLECULAR CAPSULES; HYDROGEN-BONDS; ION-TRANSPORT; COORDINATION; NANOCAPSULES; ASSEMBLIES; GUEST; ENCAPSULATION; COMPLEX; ROBUST AB Addition of cadmium(II) nitrate to gallium-coordinated metal-organic C-alkylpyrogallol[4]arene nano-capsules affords a variation of the near spherical hexamer motif, structural changes in which are induced by the markedly different nature of the secondary incorporated metal. C1 [Jin, Ping; Kumari, Harshita; Kennedy, Stuart; Barnes, Charles L.; Atwood, Jerry L.] Univ Missouri, Dept Chem, Columbia, MO 65211 USA. [Teat, Simon J.] Berkeley Lab, Adv Light Source, Berkeley, CA 94720 USA. [Dalgarno, Scott J.] Heriot Watt Univ, Inst Chem Sci, Edinburgh EH14 4AS, Midlothian, Scotland. RP Atwood, JL (reprint author), Univ Missouri, Dept Chem, 601 S Coll Ave, Columbia, MO 65211 USA. EM AtwoodJ@missouri.edu RI Kennedy, Stuart/D-5248-2014; Dalgarno, Scott/A-7358-2010 OI Kennedy, Stuart/0000-0002-1769-8797; Dalgarno, Scott/0000-0001-7831-012X FU Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231] 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. NR 28 TC 3 Z9 3 U1 2 U2 30 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 2014 VL 50 IS 34 BP 4508 EP 4510 DI 10.1039/c4cc00202d PG 3 WC Chemistry, Multidisciplinary SC Chemistry GA AD9JF UT WOS:000333580500027 PM 24667819 ER PT J AU Izatt, RM Izatt, SR Bruening, RL Izatta, NE Moyer, BA AF Izatt, Reed M. Izatt, Steven R. Bruening, Ronald L. Izatta, Neil E. Moyer, Bruce A. TI Challenges to achievement of metal sustainability in our high-tech society SO CHEMICAL SOCIETY REVIEWS LA English DT Review ID E-WASTE; RECOVERY; SYSTEMS; EXTRACTION; RESOURCES; INDUSTRY AB Achievement of sustainability in metal life cycles from mining of virgin ore to consumer and industrial devices to end-of-life products requires greatly increased recycling rates and improved processing of metals using conventional and green chemistry technologies. Electronic and other high-tech products containing precious, toxic, and specialty metals usually have short lifetimes and low recycling rates. Products containing these metals generally are incinerated, discarded as waste in landfills, or dismantled in informal recycling using crude and environmentally irresponsible procedures. Low recycling rates of metals coupled with increasing demand for high-tech products containing them necessitate increased mining with attendant environmental, health, energy, water, and carbon-footprint consequences. In this tutorial review, challenges to achieving metal sustainability, including projected use of urban mining, in present high-tech society are presented; health, environmental, and economic incentives for various government, industry, and public stakeholders to improve metal sustainability are discussed; a case for technical improvements, including use of molecular recognition, in selective metal separation technology, especially for metal recovery from dilute feed stocks is given; and global consequences of continuing on the present path are examined. C1 [Izatt, Reed M.; Izatt, Steven R.; Bruening, Ronald L.; Izatta, Neil E.] IBC Adv Technol Inc, Amer Fork, UT 84003 USA. [Izatt, Reed M.] Brigham Young Univ, Dept Chem & Biochem, Provo, UT 84602 USA. [Moyer, Bruce A.] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37830 USA. RP Izatt, RM (reprint author), IBC Adv Technol Inc, 856 East Utah Valley Dr, Amer Fork, UT 84003 USA. EM reedmizatt@gmail.com RI Izatt, Reed/F-3284-2014; Moyer, Bruce/L-2744-2016 OI Izatt, Reed/0000-0003-0943-5097; Moyer, Bruce/0000-0001-7484-6277 FU IBC Advanced Technologies, Inc; Critical Materials Institute, an Energy Innovation Hub; U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Advanced Manufacturing Office; Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy FX We acknowledge and appreciate the valuable assistance of Krystyna Pawlak, Anne Marie Izatt, Janet Spilsbury Izatt, and David W. De Paoli in preparing this manuscript. We are grateful for the support of IBC Advanced Technologies, Inc. The participation of BAM 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; and in part by the Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy. NR 53 TC 31 Z9 31 U1 4 U2 69 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 2014 VL 43 IS 8 BP 2451 EP 2475 DI 10.1039/c3cs60440c PG 25 WC Chemistry, Multidisciplinary SC Chemistry GA AD5YT UT WOS:000333330200006 PM 24464346 ER PT J AU Yang, Y Ren, Y Sun, CJ Hao, SJ AF Yang, Ying Ren, Yang Sun, Chengjun Hao, Shijie TI Facile route fabrication of nickel based mesoporous carbons with high catalytic performance towards 4-nitrophenol reduction SO GREEN CHEMISTRY LA English DT Article ID RAY-ABSORPTION SPECTROSCOPY; P-NITROPHENOL HYDROGENATION; ONE-POT SYNTHESIS; SILICA NANOCOMPOSITES; NI CATALYSTS; NANOPARTICLES; OXIDATION; POLYMER; CONVERSION; COMPLEXES AB Novel nickel based mesoporous carbons are firstly in situ fabricated via pyrolysis of CTAB-chitosan-nickel supramolecular aggregates, which are pre-constructed by CTAB-directed self-assembly of 8-quinolinol modified chitosan and nickel acetate under basic conditions. This facile route fabrication method renders smart and homogeneously dispersed Ni nanoparticles (NPs) on the mesoporous carbonaceous framework without using any stabilizer and additional reductant, verified by high-energy X-ray diffraction, TEM, X-ray absorption fine structure, N-2 adsorption/desorption and Raman spectroscopy. Moreover, it is found that the morphology of Ni NPs, the textural property of carbonaceous supports, and the corresponding catalytic performance towards 4-nitrophenol reduction vary with the pyrolysis temperature. It is suggested that the nickel based mesoporous carbon pyrolyzed at 750 degrees C (Ni/MC-750) simultaneously possessing uniform spherical Ni NPs (24.5 nm) and bottle-neck mesopores exhibits the largest activity factor of 20.9 s(-1) g(-1) of any nickel catalysts. C1 [Yang, Ying; Hao, Shijie] China Univ Petr, State Key Lab Heavy Oil Proc, Beijing 102249, Peoples R China. [Ren, Yang; Sun, Chengjun] Argonne Natl Lab, Xray Div Sci, Argonne, IL 60439 USA. RP Yang, Y (reprint author), China Univ Petr, State Key Lab Heavy Oil Proc, Beijing 102249, Peoples R China. EM catalyticscience@163.com FU U.S. Department of Energy - Basic Energy Sciences; Canadian Light Source and its funding partners; University of Washington; Advanced Photon Source; U.S. DOE [DE-AC02-06CH11357]; National Natural Science Foundation of China [21303229]; Science Foundation of China University of Petroleum, Beijing [2462013YJRC018] FX PNC/XSD facilities at the Advanced Photon Source, and research at these facilities, are supported by the U.S. Department of Energy - 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, 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. Financial support for this research work from the National Natural Science Foundation of China (21303229) and the Science Foundation of China University of Petroleum, Beijing (2462013YJRC018) is also acknowledged. NR 47 TC 30 Z9 30 U1 9 U2 63 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 2014 VL 16 IS 4 BP 2273 EP 2280 DI 10.1039/c3gc42121j PG 8 WC Chemistry, Multidisciplinary; GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY SC Chemistry; Science & Technology - Other Topics GA AD5ZC UT WOS:000333331200066 ER PT J AU Hasegawa, H Sonnerup, BUO Hu, Q Nakamura, T AF Hasegawa, Hiroshi Sonnerup, Bengt U. OE. Hu, Qiang Nakamura, Takuma TI Reconstruction of an evolving magnetic flux rope in the solar wind: Decomposing spatial and temporal variations from single-spacecraft data SO JOURNAL OF GEOPHYSICAL RESEARCH-SPACE PHYSICS LA English DT Article DE Grad-Shafranov equilibrium; magnetic flux rope; magnetic cloud; solar wind; magnetic reconnection ID CLUSTER; MAGNETOPAUSE; CLOUDS; FIELD AB We present a novel single-spacecraft method for decomposing spatial and temporal variations of physical quantities at points along the path of a spacecraft in space-time. The method is designed for use in the reconstruction of evolving two-dimensional, approximately magnetohydrostatic structures in a space plasma. It is an extension of the one developed by Sonnerup and Hasegawa (2010) and Hasegawa et al. (2010), in which it was assumed that variations in the time series of data, recorded as the structures move past the spacecraft, are all due to spatial effects. In reality, some of the observed variations are usually caused by temporal evolution of the structure during the time it moves past the observing spacecraft; the information in the data about the spatial structure is aliased by temporal effects. The purpose here is to remove this time aliasing from the reconstructed maps of field and plasma properties. Benchmark tests are performed by use of synthetic data taken by a virtual spacecraft as it traverses, at a constant velocity, a magnetic flux rope growing sufficiently slowly (relative to the Alfven speed) in a two-dimensional magnetohydrodynamic simulation of magnetic reconnection. These tests show that the new method can better recover the space-time behavior of the flux rope than does the original version, in which time-aliasing effects had not been removed. An application of the new method to a solar wind flux rope, observed by the ACE spacecraft, suggests that the cross-sectional shape of the core part of the flux rope was varying. Key Points Recovery of evolving 2-D magnetohydrostatic structure from in situ measurements Decomposing spatial and temporal variations from single-spacecraft data Evolving cross-sectional shape of a solar wind magnetic cloud C1 [Hasegawa, Hiroshi] Japan Aerosp Explorat Agcy, Inst Space & Astronaut Sci, Sagamihara, Kanagawa 2298510, Japan. [Sonnerup, Bengt U. OE.] Dartmouth Coll, Thayer Sch Engn, Hanover, NH 03755 USA. [Hu, Qiang] Univ Alabama, CSPAR, Huntsville, AL 35899 USA. [Nakamura, Takuma] Los Alamos Natl Lab, X Computat Phys Div, Los Alamos, NM USA. RP Hasegawa, H (reprint author), Japan Aerosp Explorat Agcy, Inst Space & Astronaut Sci, 3-1-1 Yoshinodai, Sagamihara, Kanagawa 2298510, Japan. EM hase@stp.isas.jaxa.jp RI Hasegawa, Hiroshi/A-1192-2007 OI Hasegawa, Hiroshi/0000-0002-1172-021X FU [KAKENHI 24740337] FX We are grateful to both reviewers for their constructive comments. We thank R. Skoug at LANL for the use of electron data from the ACE SWEPAM instrument. Work by H.H. at JAXA was supported by grant-in-aid for Scientific Research KAKENHI 24740337. NR 29 TC 1 Z9 1 U1 1 U2 4 PU AMER GEOPHYSICAL UNION PI WASHINGTON PA 2000 FLORIDA AVE NW, WASHINGTON, DC 20009 USA SN 2169-9380 EI 2169-9402 J9 J GEOPHYS RES-SPACE JI J. Geophys. Res-Space Phys. PD JAN PY 2014 VL 119 IS 1 BP 97 EP 114 DI 10.1002/2013JA019180 PG 18 WC Astronomy & Astrophysics SC Astronomy & Astrophysics GA AD1YC UT WOS:000333028600010 ER PT J AU Birn, J Hesse, M AF Birn, J. Hesse, M. TI Forced reconnection in the near magnetotail: Onset and energy conversion in PIC and MHD simulations SO JOURNAL OF GEOPHYSICAL RESEARCH-SPACE PHYSICS LA English DT Article DE entropy conservation; energy transfer; magnetotail reconnection ID THIN CURRENT SHEETS; MAGNETIC RECONNECTION; CURRENT DISRUPTION; NEUTRAL SHEETS; PLASMA SHEET; SMALL-SCALE; SUBSTORM; RESISTIVITY; FIELD; CONFIGURATIONS AB Using two-dimensional particle-in-cell (PIC) together with magnetohydrodynamic (MHD) simulations of magnetotail dynamics, we investigate the evolution toward onset of reconnection and the subsequent energy transfer and conversion. In either case, reconnection onset is preceded by a driven phase, during which magnetic flux is added to the tail at the high-latitude boundaries, followed by a relaxation phase, during which the configuration continues to respond to the driving. The boundary deformation leads to the formation of thin embedded current sheets, which are bifurcated in the near tail, converging to a single sheet farther out in the MHD simulations. The thin current sheets in the PIC simulation are carried by electrons and are associated with a strong perpendicular electrostatic field, which may provide a connection to parallel potentials and auroral arcs and an ionospheric signal even prior to the onset of reconnection. The PIC simulation very well satisfies integral entropy conservation (intrinsic to ideal MHD) during this phase, supporting ideal ballooning stability. Eventually, the current intensification leads to the onset of reconnection, the formation and ejection of a plasmoid, and a collapse of the inner tail. The earthward flow shows the characteristics of a dipolarization front: enhancement of B-z, associated with a thin vertical electron current sheet in the PIC simulation. Both MHD and PIC simulations show a dominance of energy conversion from incoming Poynting flux to outgoing enthalpy flux, resulting in heating of the inner tail. Localized Joule dissipation plays only a minor role. C1 [Birn, J.] Space Sci Inst, Boulder, CO 80301 USA. [Birn, J.] Los Alamos Natl Lab, Los Alamos, NM USA. [Hesse, M.] NASA, Goddard Space Flight Ctr, Greenbelt, MD 20771 USA. RP Birn, J (reprint author), Space Sci Inst, Boulder, CO 80301 USA. EM jbirn@spacescience.org RI feggans, john/F-5370-2012; NASA MMS, Science Team/J-5393-2013 OI NASA MMS, Science Team/0000-0002-9504-5214 FU US Department of Energy; NSF grant [GEM1203711]; NASA grants [NNX13AD10G, NNX13AD21G, NNX12AO98G] FX Part of this work was performed at Los Alamos under the auspices of the US Department of Energy, supported by NSF grant GEM1203711 and NASA grants NNX13AD10G, NNX13AD21G, and NNX12AO98G. NR 56 TC 13 Z9 13 U1 0 U2 12 PU AMER GEOPHYSICAL UNION PI WASHINGTON PA 2000 FLORIDA AVE NW, WASHINGTON, DC 20009 USA SN 2169-9380 EI 2169-9402 J9 J GEOPHYS RES-SPACE JI J. Geophys. Res-Space Phys. PD JAN PY 2014 VL 119 IS 1 BP 290 EP 309 DI 10.1002/2013JA019354 PG 20 WC Astronomy & Astrophysics SC Astronomy & Astrophysics GA AD1YC UT WOS:000333028600026 ER PT J AU Yoon, S Ha, J Chae, SR Kilcoyne, DA Monteiro, PJM AF Yoon, Seyoon Ha, Juyoung Chae, Sejung Rosie Kilcoyne, David A. Monteiro, Paulo J. M. TI X-ray spectromicroscopic study of interactions between NaCl and calcium silicate hydrates SO MAGAZINE OF CONCRETE RESEARCH LA English DT Article ID C-S-H; ADVANCED LIGHT-SOURCE; PHOTOELECTRON-SPECTROSCOPY; SODIUM-CHLORIDE; DISSOLUTION; PHASES AB X-ray diffraction (XRD), scanning transmission X-ray microscopy (STXM) and X-ray absorption near edge structure (XANES) spectra were used to investigate the interactions between sodium chloride (NaCl) and calcium silicate hydrate (C-S-H), the primary binding phase of hydrated Portland cement. XRD analysis indicates the interlayer expansion of C-S-H with a high Ca/Si ratio. Contrast maps of STXM images collected from C-S-Hs with different Ca/Si ratios reacted with NaCl solution reveal that sodium interacts with C-S-H with a low Ca/Si ratio, while chloride is intercalated into the interlayer of C-S-H with a high Ca/Si ratio. Silicon K-edge XANES spectra were analysed to understand the variation in the structure of silicate chains. This revealed that the interaction with the sodium cations depolymerises the silicate chains of C-S-H with a low Ca/Si ratio. The mechanism involved for the selection of adsorbed ions is probably due to the residual charge between the positive charge of interlayer calcium ions and the negative charge of the end group of silicate chains in C-S-H. C1 [Yoon, Seyoon] Univ Aberdeen, Kings Coll, Sch Engn, Aberdeen, Scotland. [Ha, Juyoung] Rutgers State Univ, Dept Environm Sci, New Brunswick, NJ 08903 USA. [Chae, Sejung Rosie; Monteiro, Paulo J. M.] Univ Calif Berkeley, Dept Civil & Environm Engn, Berkeley, CA 94720 USA. [Kilcoyne, David A.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. RP Yoon, S (reprint author), Univ Aberdeen, Kings Coll, Sch Engn, Aberdeen, Scotland. RI Yoon, Seyoon/N-5936-2014; Kilcoyne, David/I-1465-2013 OI Yoon, Seyoon/0000-0002-3451-5518; FU Office of Science, Department of Energy [DE-AC02-05CH11231] FX Data were acquired at beamlines BL5.3.2.1 and BL11.0.2.2 at the Advanced Light Source, supported by the Director of the Office of Science, Department of Energy, under contract no. DE-AC02-05CH11231. NR 23 TC 3 Z9 3 U1 1 U2 16 PU ICE PUBLISHING PI WESTMINISTER PA INST CIVIL ENGINEERS, 1 GREAT GEORGE ST, WESTMINISTER SW 1P 3AA, ENGLAND SN 0024-9831 EI 1751-763X J9 MAG CONCRETE RES JI Mag. Concr. Res. PY 2014 VL 66 IS 3 BP 141 EP 149 DI 10.1680/macr.13.00244 PG 9 WC Construction & Building Technology; Materials Science, Multidisciplinary SC Construction & Building Technology; Materials Science GA AD4UW UT WOS:000333247700003 ER PT J AU Lee, KH Kao, J Parizi, SS Caruntu, G Xu, T AF Lee, Keun Hyung Kao, Joseph Parizi, Saman Salemizadeh Caruntu, Gabriel Xu, Ting TI Dielectric properties of barium titanate supramolecular nanocomposites SO NANOSCALE LA English DT Article ID POLYMER NANOCOMPOSITES; ENERGY DENSITY; COMPOSITES; CONSTANT; FILMS; NANOPARTICLES; PERMITTIVITY; PERCOLATION; STRATEGIES AB Nanostructured dielectric composites can be obtained by dispersing high permittivity fillers, barium titanate (BTO) nanocubes, within a supramolecular framework. Thin films of BTO supramolecular nanocomposites exhibit a dielectric permittivity (epsilon(r)) as high as 15 and a relatively low dielectric loss of similar to 0.1 at 1 kHz. These results demonstrate a new route to control the dispersion of high permittivity fillers toward high permittivity dielectric nanocomposites with low loss. Furthermore, the present study shows that the size distribution of nanofillers plays a key role in their spatial distribution and local ordering and alignment within supramolecular nanostructures. C1 [Lee, Keun Hyung; Kao, Joseph; Xu, Ting] Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA. [Parizi, Saman Salemizadeh; Caruntu, Gabriel] Cent Michigan Univ, Dept Chem, Mt Pleasant, MI 48858 USA. [Parizi, Saman Salemizadeh; Caruntu, Gabriel] Cent Michigan Univ, Sci Adv Mat Program, Mt Pleasant, MI 48858 USA. [Xu, Ting] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Xu, Ting] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mat Sci Div, Berkeley, CA 94720 USA. RP Xu, T (reprint author), Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA. EM tingxu@berkeley.edu FU Office of Naval Research Young Investigator program; Central Michigan University; Macromolecular, Supramolecular and Nanochemistry Division of the National Science Foundation [1157300] FX The authors thank Prof. Jean M. J. Frechet for access to his metal evaporator and impedance spectroscopy equipment. This work was supported by the Office of Naval Research Young Investigator program. GC thanks the Central Michigan University for supporting this work through start-up funds and the Macromolecular, Supramolecular and Nanochemistry Division of the National Science Foundation (CAREER award no. 1157300). NR 40 TC 12 Z9 12 U1 3 U2 37 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 2014 VL 6 IS 7 BP 3526 EP 3531 DI 10.1039/c3nr05535c PG 6 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA AD2DD UT WOS:000333042500012 PM 24584569 ER PT J AU Fei, L Xu, Y Wu, XF Chen, G Li, YL Li, BS Deng, SG Smirnov, S Fan, HY Luo, HM AF Fei, Ling Xu, Yun Wu, Xiaofei Chen, Gen Li, Yuling Li, Binsong Deng, Shuguang Smirnov, Sergei Fan, Hongyou Luo, Hongmei TI Instant gelation synthesis of 3D porous MoS2@C nanocomposites for lithium ion batteries SO NANOSCALE LA English DT Article ID STORAGE PROPERTIES; ANODE MATERIAL; FACILE SYNTHESIS; ASSISTED SYNTHESIS; MESOPOROUS CARBON; MOS2; GRAPHENE; NANOPARTICLES; NANOSHEETS; PERFORMANCES AB Three-dimensional (3D) nanoporous architectures, possessing high surface area, massive pores, and excellent structural stability, are highly desirable for many applications including catalysts and electrode materials in lithium ion batteries. However, the preparation of such materials remains a major challenge. Here, we introduce a novel method, instant gelation, for the synthesis of such materials. The as-prepared porous 3D MoS2@C nanocomposites, with layered MoS2 clusters or strips ingrained in porous and conductive 3D carbon matrix, indeed showed excellent electrochemical performance when applied as anode materials for lithium ion batteries. Its interconnected carbon network ensures good conductivity and fast electron transport; the micro-, and mesoporous nature effectively shortens the lithium ion diffusion path and provides room necessary for volume expansion. The large specific surface area is beneficial for a better contact between electrode materials and electrolyte. C1 [Fei, Ling; Xu, Yun; Wu, Xiaofei; Chen, Gen; Li, Yuling; Deng, Shuguang; Luo, Hongmei] New Mexico State Univ, Dept Chem Engn, Las Cruces, NM 88003 USA. [Li, Binsong; Fan, Hongyou] Sandia Natl Labs, Adv Mat Lab, Albuquerque, NM 87106 USA. [Smirnov, Sergei] New Mexico State Univ, Dept Chem & Biochem, Las Cruces, NM 88003 USA. RP Luo, HM (reprint author), New Mexico State Univ, Dept Chem Engn, Las Cruces, NM 88003 USA. EM hluo@nmsu.edu RI CHEN, GEN/K-9436-2014; Deng, Shuguang/G-5926-2011; Smirnov, Sergei/H-8774-2016 OI CHEN, GEN/0000-0003-3504-3572; Deng, Shuguang/0000-0003-2892-3504; FU NSF/CMMI Nano-Manufacturing Program [1131290]; office of Vice President for Research at NMSU; U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering; U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX We acknowledge the funding support from NSF/CMMI Nano-Manufacturing Program under Grant no. 1131290 and the office of Vice President for Research at NMSU. L.F. acknowledges the Preparing Future Faculty Graduate Assistantship Award. This work is partially supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering. Sandia is a multiprogram laboratory 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 29 TC 24 Z9 24 U1 10 U2 178 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 2014 VL 6 IS 7 BP 3664 EP 3669 DI 10.1039/c3nr05815h PG 6 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA AD2DD UT WOS:000333042500032 PM 24567121 ER PT J AU Mangum, BD Sampat, S Ghosh, Y Hollingsworth, JA Htoon, H Malko, AV AF Mangum, Benjamin D. Sampat, Siddharth Ghosh, Yagnaseni Hollingsworth, Jennifer A. Htoon, Han Malko, Anton V. TI Influence of the core size on biexciton quantum yield of giant CdSe/CdS nanocrystals SO NANOSCALE LA English DT Article ID PHOTON-COUNTING STATISTICS; LIGHT-EMITTING-DIODES; LEVY WALK PROCESS; AUGER RECOMBINATION; SEMICONDUCTOR NANOCRYSTALS; BLINKING SUPPRESSION; SHELL-THICKNESS; DOT BLINKING; PHOTOLUMINESCENCE; EMISSION AB We present a systematic study of photoluminescence (PL) emission intensity and biexciton (BX) quantum yields (QYBX) in individual "giant" CdSe/CdS nanocrystals (g-NCs) as a function of g-NC core size and shell thickness. We show that g-NC core size significantly affects QYBX and can be utilized as an effective tuning parameter towards higher QYBX while keeping the total volume of the g-NC constant. Specifically, we observe that small-core (2.2 nm diameter) CdSe/CdS NCs with a volume of similar to 200 nm(3) (shell comprises 4 CdS monolayers) show very low average and maximum QYBX's of similar to 3 and 7%, respectively. In contrast, same-volume medium-core (3 nm diameter) NCs afford higher average values of similar to 10%, while QYBX's of similar to 30% are achieved for same-volume large-core (5.5 nm diameter) CdSe/CdS NCs, with some approaching similar to 80%. These observations underline the influence of the g-NC core size on the evolution of PL emissive states in multi-shell NCs. Moreover, our study also reveals that the use of long anneal times in the growth of CdS shells plays a critical role in achieving high QYBX. C1 [Mangum, Benjamin D.; Ghosh, Yagnaseni; Hollingsworth, Jennifer A.; Htoon, Han] Los Alamos Natl Lab, Mat Phys & Applicat Div, Ctr Integrated Nanotechnol, Los Alamos, NM 87545 USA. [Sampat, Siddharth; Malko, Anton V.] Univ Texas Dallas, Dept Phys, Richardson, TX 75080 USA. RP Malko, AV (reprint author), Univ Texas Dallas, Dept Phys, Richardson, TX 75080 USA. EM htoon@lanl.gov; anton.malko@utdallas.edu OI Htoon, Han/0000-0003-3696-2896 FU DOE/BES [DE-SC0010697]; Single Investigator Small Group Research Grant [2009LANL1096]; Office of Basic Energy Sciences (OBES); Office of Science (OS); U.S. Department of Energy (DOE); Los Alamos National Laboratory Directed Research and Development (LDRD) Program FX UT Dallas group (A. V. M. and S. S.) acknowledges partial support from the DOE/BES grant (DE-SC0010697), while B. D. M., J.A.H. and H. H. acknowledge partial support by a Single Investigator Small Group Research Grant (2009LANL1096), Office of Basic Energy Sciences (OBES), Office of Science (OS), U.S. Department of Energy (DOE). This work was performed, in part, at the Center for Integrated Nanotechnologies (CINT), a U.S. DOE, OBES User Facility and Nanoscale Science Research Center. Y.G. acknowledges support by the Los Alamos National Laboratory Directed Research and Development (LDRD) Program. NR 45 TC 14 Z9 14 U1 1 U2 43 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 2014 VL 6 IS 7 BP 3712 EP 3720 DI 10.1039/c3nr06558h PG 9 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA AD2DD UT WOS:000333042500038 PM 24569861 ER PT J AU Si, LP He, HS Zhu, K AF Si, Liping He, Hongshan Zhu, Kai TI 8-Hydroxylquinoline-conjugated porphyrins as broadband light absorbers for dye-sensitized solar cells SO NEW JOURNAL OF CHEMISTRY LA English DT Article ID TIO2 FILMS; ANCHORING GROUP; EFFICIENCY; TRANSPORT; ENERGY; SPECTROSCOPY; CHROMOPHORES; DESIGN; LENGTH; COST AB Three porphyrin dyes, DPZn-HOQ, PZn-HOQ and DPZn-COOH, were synthesized and characterized for dyesensitized solar cells. Both DPZn-HOQ and DPZn-COOH exhibited a donor-p-acceptor configuration with N,N-dimethylaniline as a donor and 8-hydroxylquinoline (HOQ) and para-benzoic acid (BZA) as acceptors, respectively. PZn-HOQ is an analogue of DPZn-HOQ without a donor. It was found that DPZn-HOQ exhibited broader and stronger light absorption capability in the red region than DPZn-COOH. Theoretical calculations showed that the electrons were delocalized to the 8-hydroxylquinoline ring in DPZN-HOQ. The DPZn-HOQ-sensitized solar cells exhibited higher energy conversion efficiency (3.09%) than DPZn-COOH-sensitized solar cells (1.76%) under the same conditions. The results were consistent with the incident photon to current conversion efficiency (IPCE) spectra. The electrochemical impedance spectroscopy studies revealed that HOQ-conjugated porphyrin exhibited high electron recombination resistance and a long electron lifetime, which was attributed to the effective shielding of DPZn-HOQ from the electrolyte due to its tilted orientation on the surface of TiO2 nanoparticles. The efficiency of DPZn-HOQ-sensitized solar cells was further increased to 3.41% when a complementary dye BET was used. C1 [Si, Liping; He, Hongshan] Eastern Illinois Univ, Dept Chem, Charleston, IL 62910 USA. [Si, Liping; He, Hongshan] S Dakota State Univ, Ctr Adv Photovolta, Brookings, SD 57006 USA. [Zhu, Kai] Natl Renewable Energy Lab, Golden, CO 80401 USA. RP He, HS (reprint author), Eastern Illinois Univ, Dept Chem, Charleston, IL 62910 USA. EM hhe@eiu.edu; kai.zhu@nrel.gov OI He, Hongshan/0000-0002-7462-1366 FU Council on Faculty Research Grant, Eastern Illinois University; National Science Foundation/EPSCoR [0903804]; Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy [DE-AC36-08GO28308] FX This work was partially supported by the Council on Faculty Research Grant, Eastern Illinois University (H.H.) and the National Science Foundation/EPSCoR, Grant No. 0903804 (H.H.). This work was also supported by the Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy, under contract No. DE-AC36-08GO28308 (K.Z.). NR 38 TC 8 Z9 8 U1 0 U2 14 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1144-0546 EI 1369-9261 J9 NEW J CHEM JI New J. Chem. PY 2014 VL 38 IS 4 BP 1565 EP 1572 DI 10.1039/c3nj01643a PG 8 WC Chemistry, Multidisciplinary SC Chemistry GA AD2RX UT WOS:000333083900030 ER PT J AU Shao, N Wu, Q AF Shao, Nan Wu, Qin TI Charge self-localization in pi-conjugated polymers by long range corrected hybrid functionals SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID 2ND-ORDER PERTURBATION-THEORY; DENSITY FUNCTIONALS; HARTREE-FOCK; POLYACETYLENE CHAINS; CONDUCTING POLYMERS; SEPARATED HYBRIDS; RADICAL CATIONS; OLIGOMERS; EXCHANGE; DESIGN AB We systematically investigate the capability of hybrid functionals for describing charge self-localization in conjugated polymers, using the critical test that the spatial extension of a localized charge should be polymer length independent. We first compare the new long-range corrected (LRC) hybrids with conventional global hybrids and find that the former has a clear and important advantage over the latter in being significantly less spin contaminated. We then focus on LRC hybrids and investigate in detail the dependence of charge localization on the range parameter. We show that this parameter consistently needs to be about 0.2 bohr(-1) or larger to produce self-localized charges across different polymers. We introduce a new measure to determine the charge localization length, and then consider how properties related to localized charges converge with the polymer length and how they depend on the range parameter. These properties include the reorganization energy in the Marcus theory for electron transfer and the lowest excitation energy of a polaron. We discuss parameter tuning to experimental results and also suggest 0.2 bohr(-1) without tuning for exploratory studies based on the preference for least spin contaminations. C1 [Shao, Nan; Wu, Qin] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. RP Wu, Q (reprint author), Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. EM qinwu@bnl.gov RI Wu, Qin/C-9483-2009 OI Wu, Qin/0000-0001-6350-6672 FU U. S. Department of Energy, Office of Basic Energy Sciences [DE-AC02-98CH10886] FX All calculations were performed on the computer clusters 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. NR 45 TC 5 Z9 5 U1 1 U2 18 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 2014 VL 16 IS 14 BP 6700 EP 6708 DI 10.1039/c3cp54515f PG 9 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AD3DZ UT WOS:000333119800041 PM 24584767 ER PT J AU Zhou, J AF Zhou, Jia TI Stacking interactions of nickel bis(dithiolene) with graphene and beyond SO RSC ADVANCES LA English DT Article ID SCANNING-TUNNELING-MICROSCOPY; INITIO MOLECULAR-DYNAMICS; TOTAL-ENERGY CALCULATIONS; HEXAGONAL BORON-NITRIDE; AUGMENTED-WAVE METHOD; EPITAXIAL-GROWTH; BERRYS PHASE; BASIS-SET; METALS; APPROXIMATION AB Density functional theory (DFT) with dispersion correction has been used to study the stacking interactions of the nickel bis(dithiolene) molecule and graphene. As in our previous study of the nickel bis(dithiolene) molecule and benzene, two different configurations were considered for the nickel bis(dithiolene) molecule and graphene, and the whole potential energy surface (PES) was explored for each of them. The stacking interaction energy is comparable with other similar systems in the experiments, and it is shown that the surface-mediated interactions play a role in determining molecular orientation. Based on the results of the nickel bis(dithiolene) molecule and graphene, we also studied a new two-dimensional (2D) heterobilayered material consisting of a 2D nickel bis(dithiolene) sheet and graphene or hexagonal boron nitride (h-BN). It turns out that h-BN is a good substrate for the 2D nickel bis(dithiolene) sheet, an organic topological insulator, to maintain its original properties, while the 2D nickel bis( dithiolene) sheet behaves like a metal when forming a new 2D heterobilayered material with graphene. These observations would undoubtedly enrich the current study of 2D heterobilayered materials. C1 Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. RP Zhou, J (reprint author), Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. EM zhouj1@ornl.gov FU Office of Science of the U.S. Department of Energy [DE-AC05-00OR22750, DE-AC02-05CH11231]; Center for Nanophase Materials Sciences; Scientific User Facilities Division, U.S. Department of Energy FX This work used computational resources of the National Center for Computational Sciences at Oak Ridge National laboratory and of the National Energy Research Scientific Computing Center, which are supported by the Office of Science of the U.S. Department of Energy under Contract no. DE-AC05-00OR22750 and DE-AC02-05CH11231, respectively. We also acknowledge the support from the Center for Nanophase Materials Sciences, which is sponsored at ORNL by the Scientific User Facilities Division, U.S. Department of Energy. NR 39 TC 2 Z9 2 U1 7 U2 44 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 2014 VL 4 IS 26 BP 13361 EP 13366 DI 10.1039/c3ra48058e PG 6 WC Chemistry, Multidisciplinary SC Chemistry GA AD2RL UT WOS:000333082700019 ER PT J AU Mruetusatorn, P Boreyko, JB Venkatesan, GA Sarles, SA Hayes, DG Collier, CP AF Mruetusatorn, Prachya Boreyko, Jonathan B. Venkatesan, Guru A. Sarles, Stephen A. Hayes, Douglas G. Collier, C. Patrick TI Dynamic morphologies of microscale droplet interface bilayers SO SOFT MATTER LA English DT Article ID SUPPORTED PHOSPHOLIPID-BILAYERS; LIPID-BILAYERS; SHAPE TRANSFORMATIONS; SPONTANEOUS-CURVATURE; UNILAMELLAR VESICLES; MOLECULAR-MECHANISM; GIANT VESICLES; MEMBRANE; MONOLAYERS; FISSION AB Droplet interface bilayers (DIBs) are a powerful platform for studying the dynamics of synthetic cellular membranes; however, very little has been done to exploit the unique dynamical features of DIBs. Here, we generate microscale droplet interface bilayers (mu DIBs) by bringing together femtoliter-volume water droplets in a microfluidic oil channel, and characterize morphological changes of the mDIBs as the droplets shrink due to evaporation. By varying the initial conditions of the system, we identify three distinct classes of dynamic morphology. (1) Buckling and fission: when forming mDIBs using the lipid-out method (lipids in oil phase), lipids in the shrinking monolayers continually pair together and slide into the bilayer to conserve their mass. As the bilayer continues to grow, it becomes confined, buckles, and eventually fissions one or more vesicles. (2) Uniform shrinking: when using the lipid-in method (lipids in water phase) to form mDIBs, lipids uniformly transfer from the monolayers and bilayer into vesicles contained inside the water droplets. (3) Stretching and unzipping: finally, when the droplets are pinned to the wall(s) of the microfluidic channel, the droplets become stretched during evaporation, culminating in the unzipping of the bilayer and droplet separation. These findings offer a better understanding of the dynamics of coupled lipid interfaces. C1 [Mruetusatorn, Prachya; Hayes, Douglas G.] Univ Tennessee, Dept Biosyst Engn & Soil Sci, Knoxville, TN 37996 USA. [Boreyko, Jonathan B.; Collier, C. Patrick] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. [Venkatesan, Guru A.; Sarles, Stephen A.] Univ Tennessee, Dept Mech Aerosp & Biomed Engn, Knoxville, TN 37996 USA. RP Collier, CP (reprint author), Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. EM colliercp@ornl.gov RI Collier, Charles/C-9206-2016 OI Collier, Charles/0000-0002-8198-793X FU Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy; Air Force Office of Scientific Research Basic Research Initiative [11157642] FX This research was 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. G. Venkatesan and A. Sarles are funded by the Air Force Office of Scientific Research Basic Research Initiative grant number 11157642. NR 70 TC 10 Z9 10 U1 3 U2 44 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 2014 VL 10 IS 15 BP 2530 EP 2538 DI 10.1039/c3sm53032a PG 9 WC Chemistry, Physical; Materials Science, Multidisciplinary; Physics, Multidisciplinary; Polymer Science SC Chemistry; Materials Science; Physics; Polymer Science GA AD3CY UT WOS:000333116700005 PM 24647872 ER PT J AU Armstrong, CL Haussler, W Seydel, T Katsaras, J Rheinstadter, MC AF Armstrong, Clare L. Haeussler, Wolfgang Seydel, Tilo Katsaras, John Rheinstaedter, Maikel C. TI Nanosecond lipid dynamics in membranes containing cholesterol SO SOFT MATTER LA English DT Article ID X-RAY-SCATTERING; NEUTRON SPIN-ECHO; COLLECTIVE DYNAMICS; PHOSPHOLIPID-BILAYERS; BIOLOGICAL-MEMBRANES; MOLECULAR-STRUCTURE; LATERAL DIFFUSION; LIQUID DOMAINS; PHASE-DIAGRAMS; RIPPLE PHASE AB Lipid dynamics in the cholesterol-rich (40 mol%) liquid-ordered (l(o)) phase of dimyristoylphosphatidylcholine membranes were studied using neutron spin-echo and neutron backscattering. Recent theoretical and experimental evidence supports the notion of the liquid-ordered phase in phospholipid membranes as a locally structured liquid, with small ordered 'domains' of a highly dynamic nature in equilibrium with a disordered matrix [S. Meinhardt, R. L. C. Vink and F. Schmid, Proc. Natl. Acad. Sci. U. S. A., 2013, 110(12), 4476-4481, C. L. Armstrong et al., PLoS One, 2013, 8(6), e66162]. This local structure was found to have a pronounced impact on the membranes' dynamical properties. We found that the long-wavelength dynamics in the liquid-ordered phase, associated with the elastic properties of the membranes, were faster by two orders of magnitude as compared to the liquid disordered phase. At the same time, collective nanoscale diffusion was significantly slower. The presence of a soft-mode (a slowing down) in the long-wavelength dispersion relationship suggests an upper size limit for the ordered lipid domain of approximate to 220 angstrom. Moreover, from the relaxation rate of the collective lipid diffusion of lipid-lipid distances, the lifetime of these domains was estimated to be about 100 nanoseconds. C1 [Armstrong, Clare L.; Rheinstaedter, Maikel C.] McMaster Univ, Dept Phys & Astron, Hamilton, ON L8S 4M1, Canada. [Haeussler, Wolfgang] Tech Univ Munich, FRM II & E21, Garching, Germany. [Seydel, Tilo] Inst Max Von Laue Paul Langevin, F-38042 Grenoble, France. [Katsaras, John] Oak Ridge Natl Lab, Neutron Sci Directorate, Oak Ridge, TN USA. [Katsaras, John; Rheinstaedter, Maikel C.] Canadian Neutron Beam Ctr, Chalk River, ON, Canada. [Katsaras, John] Joint Inst Neutron Sci, Oak Ridge, TN USA. RP Rheinstadter, MC (reprint author), McMaster Univ, Dept Phys & Astron, Hamilton, ON L8S 4M1, Canada. EM rheinstadter@mcmaster.ca OI Katsaras, John/0000-0002-8937-4177 FU Natural Sciences and Engineering Research Council (NSERC) of Canada; National Research Council (NRC); Canada Foundation for Innovation (CFI); Ontario Ministry of Economic Development and Innovation; Scientific User Facilities Division of the Office of Basic Energy Sciences (BES); Laboratory Directed Research and Development (LDRD) program of Oak Ridge National Laboratory; U.S. Department of Energy (DOE) [DE-AC05-00OR2275]; Province of Ontario FX This research was funded by the Natural Sciences and Engineering Research Council (NSERC) of Canada, the National Research Council (NRC), the Canada Foundation for Innovation (CFI), and the Ontario Ministry of Economic Development and Innovation. J.K. acknowledges support from the Scientific User Facilities Division of the Office of Basic Energy Sciences (BES), and the Laboratory Directed Research and Development (LDRD) program of Oak Ridge National Laboratory, managed by UT-Battelle, LLC, for the U.S. Department of Energy (DOE) under contract no. DE-AC05-00OR2275. M.C.R. is the recipient of an Early Researcher Award from the Province of Ontario. NR 75 TC 21 Z9 21 U1 2 U2 32 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 2014 VL 10 IS 15 BP 2600 EP 2611 DI 10.1039/c3sm51757h PG 12 WC Chemistry, Physical; Materials Science, Multidisciplinary; Physics, Multidisciplinary; Polymer Science SC Chemistry; Materials Science; Physics; Polymer Science GA AD3CY UT WOS:000333116700013 PM 24647350 ER PT J AU Trabert, E AF Traebert, Elmar TI Measurement of femtosecond atomic lifetimes using ion traps SO APPLIED PHYSICS B-LASERS AND OPTICS LA English DT Article ID HIGHLY-CHARGED IONS; MAGNETIC TRAPPING MODE; BEAM; SPECTROSCOPY; TRANSITION; COLD AB Two types of experiment are described that both employ an electron beam ion trap for the production of highly charged ion species with the aim of then measuring atomic level lifetimes in the femtosecond range. In one experiment (done by Beiersdorfer et al. some time ago), the lifetime measurement depends on the associated line broadening. In a recent string of experiments at Linac Coherent Light Source Stanford, the HI-LIGHT collaboration employed pump-probe excitation using the FEL as a short-pulse X-ray laser. C1 [Traebert, Elmar] Ruhr Univ Bochum, Fak Phys & Astron, Astron Inst, D-44780 Bochum, Germany. [Traebert, Elmar] Lawrence Livermore Natl Lab, Div Phys, Livermore, CA 94550 USA. RP Trabert, E (reprint author), Ruhr Univ Bochum, Fak Phys & Astron, Astron Inst, D-44780 Bochum, Germany. EM traebert@astro.rub.de FU U.S. Department of Energy by Lawrence Livermore National Laboratory [DE-AC52-07NA27344]; German Research Association (DFG) [Tr171-19] FX The author appreciates thankfully the hospitality and support experienced at the Livermore EBIT laboratory and the work experience in the HI-LIGHT collaboration. Part of this work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344. Support by the German Research Association (DFG) is gratefully acknowledged (Tr171-19). NR 29 TC 1 Z9 1 U1 1 U2 7 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 2014 VL 114 IS 1-2 BP 167 EP 172 DI 10.1007/s00340-013-5586-z PG 6 WC Optics; Physics, Applied SC Optics; Physics GA AC9JO UT WOS:000332850800018 ER PT J AU Klebe, DI Blatherwick, RD Morris, VR AF Klebe, D. I. Blatherwick, R. D. Morris, V. R. TI Ground-based all-sky mid-infrared and visible imagery for purposes of characterizing cloud properties SO ATMOSPHERIC MEASUREMENT TECHNIQUES LA English DT Article ID COVER; FRACTION AB This paper describes the All Sky Infrared Visible Analyzer (ASIVA), a multi-purpose visible and infrared sky imaging and analysis instrument whose primary function is to provide radiometrically calibrated imagery in the mid-infrared (mid-IR) atmospheric window. This functionality enables the determination of diurnal fractional sky cover and estimates of sky/cloud temperature from which one can derive estimates of sky/cloud emissivity and cloud height. This paper describes the calibration methods and performance of the ASIVA instrument with particular emphasis on data products being developed for the meteorological community. Data presented here were collected during the Solmirus' ASIVA campaign conducted at the Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) Climate Research Facility from 21 May to 27 July 2009. The purpose of this campaign was to determine the efficacy of IR technology in providing reliable nighttime sky cover data. Significant progress has been made in the analysis of the campaign data over the past several years and the ASIVA has proven to be an excellent instrument for determining sky cover as well as the potential for determining sky/cloud temperature, sky/cloud emissivity, precipitable water vapor (PWV), and ultimately cloud height. C1 [Klebe, D. I.] Denver Museum Nat & Sci, Denver, CO 80205 USA. [Blatherwick, R. D.] Univ Denver, Denver, CO USA. [Morris, V. R.] Pacific NW Natl Lab, Richland, WA 99352 USA. [Blatherwick, R. D.] Solmirus Corp, Woodland Park, CO USA. RP Klebe, DI (reprint author), Denver Museum Nat & Sci, Denver, CO 80205 USA. EM dimitri.klebe@dmns.org FU US Department of Energy's (DOE) Atmospheric System Research Program, an Office of Science, Office of Biological and Environmental Research program FX This research was supported in part by the US Department of Energy's (DOE) Atmospheric System Research Program, an Office of Science, Office of Biological and Environmental Research program, under Grant DE-SC-0008650. We acknowledge the cooperation of the DOE Atmospheric Radiation Measurement Climate Research Facility Southern Great Plains site and thank those responsible for the operation and maintenance of the instruments that produced the data used in this study. NR 20 TC 13 Z9 13 U1 1 U2 4 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1867-1381 EI 1867-8548 J9 ATMOS MEAS TECH JI Atmos. Meas. Tech. PY 2014 VL 7 IS 2 BP 637 EP 645 DI 10.5194/amt-7-637-2014 PG 9 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA AC3AF UT WOS:000332386700020 ER PT J AU Andrews, AE Kofler, JD Trudeau, ME Williams, JC Neff, DH Masarie, KA Chao, DY Kitzis, DR Novelli, PC Zhao, CL Dlugokencky, EJ Lang, PM Crotwell, MJ Fischer, ML Parker, MJ Lee, JT Baumann, DD Desai, AR Stanier, CO De Wekker, SFJ Wolfe, DE Munger, JW Tans, PP AF Andrews, A. E. Kofler, J. D. Trudeau, M. E. Williams, J. C. Neff, D. H. Masarie, K. A. Chao, D. Y. Kitzis, D. R. Novelli, P. C. Zhao, C. L. Dlugokencky, E. J. Lang, P. M. Crotwell, M. J. Fischer, M. L. Parker, M. J. Lee, J. T. Baumann, D. D. Desai, A. R. Stanier, C. O. De Wekker, S. F. J. Wolfe, D. E. Munger, J. W. Tans, P. P. TI CO2, CO, and CH4 measurements from tall towers in the NOAA Earth System Research Laboratory's Global Greenhouse Gas Reference Network: instrumentation, uncertainty analysis, and recommendations for future high-accuracy greenhouse gas monitoring efforts SO ATMOSPHERIC MEASUREMENT TECHNIQUES LA English DT Article ID CARBON-DIOXIDE EXCHANGE; ATMOSPHERIC CO2; MOLE FRACTIONS; AIR; SCALE; SPECTROSCOPY; INVERSION; ANALYZER; METHANE; DESIGN AB A reliable and precise in situ CO2 and CO analysis system has been developed and deployed at eight sites in the NOAA Earth System Research Laboratory's (ESRL) Global Greenhouse Gas Reference Network. The network uses very tall (> 300 m) television and radio transmitter towers that provide a convenient platform for mid-boundary-layer trace-gas sampling. Each analyzer has three sample inlets for profile sampling, and a complete vertical profile is obtained every 15 min. The instrument suite at one site has been augmented with a cavity ring-down spectrometer for measuring CO2 and CH4. The long-term stability of the systems in the field is typically better than 0.1 ppm for CO2, 6 ppb for CO, and 0.5 ppb for CH4, as determined from repeated standard gas measurements. The instrumentation is fully automated and includes sensors for measuring a variety of status parameters, such as temperatures, pressures, and flow rates, that are inputs for automated alerts and quality control algorithms. Detailed and time-dependent uncertainty estimates have been constructed for all of the gases, and the uncertainty framework could be readily adapted to other species or analysis systems. The design emphasizes use of off-theshelf parts and modularity to facilitate network operations and ease of maintenance. The systems report high-quality data with > 93% uptime. Recurrent problems and limitations of the current system are discussed along with general recommendations for high-accuracy trace-gas monitoring. The network is a key component of the North American Carbon Program and a useful model for future research-grade operational greenhouse gas monitoring efforts. C1 [Andrews, A. E.; Kofler, J. D.; Trudeau, M. E.; Williams, J. C.; Neff, D. H.; Masarie, K. A.; Chao, D. Y.; Kitzis, D. R.; Novelli, P. C.; Zhao, C. L.; Dlugokencky, E. J.; Lang, P. M.; Crotwell, M. J.; Wolfe, D. E.; Tans, P. P.] NOAA, Earth Syst Res Lab, Boulder, CO 80305 USA. [Kofler, J. D.; Trudeau, M. E.; Neff, D. H.; Chao, D. Y.; Kitzis, D. R.; Zhao, C. L.; Crotwell, M. J.] Univ Colorado, Cooperat Inst Res Environm Sci, Boulder, CO 80309 USA. [Trudeau, M. E.] Colorado State Univ, Cooperat Inst Res Atmosphere, Ft Collins, CO 80523 USA. [Williams, J. C.] Sci & Technol Corp, Boulder, CO USA. [Fischer, M. L.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. [Crotwell, M. J.] Savannah River Natl Lab, Aiken, SC USA. [Crotwell, M. J.] Savannah River Nucl Solut LLC, Aiken, SC USA. [Lee, J. T.] Univ Maine, Sch Forestry, Ctr Res Sustainable Forestry, Orono, ME USA. [Baumann, D. D.] US Forest Serv, Inst Appl Ecosyst Studies, No Res Stn, Rhinelander, WI USA. [Desai, A. R.] Univ Wisconsin, Atmospher & Ocean Sci Dept, Madison, WI USA. [Stanier, C. O.] Univ Iowa, Dept Chem & Biochem Engn, Iowa City, IA 52242 USA. [De Wekker, S. F. J.] Univ Virginia, Dept Environm Sci, Charlottesville, VA 22903 USA. [Munger, J. W.] Harvard Univ, Sch Engn & Appl Sci, Cambridge, MA 02138 USA. RP Andrews, AE (reprint author), NOAA, Earth Syst Res Lab, Boulder, CO 80305 USA. EM arlyn.andrews@noaa.gov RI Andrews, Arlyn/K-3427-2012; Desai, Ankur/A-5899-2008; Stanier, Charles/D-4307-2016; Munger, J/H-4502-2013 OI Desai, Ankur/0000-0002-5226-6041; Stanier, Charles/0000-0001-9924-0853; Munger, J/0000-0002-1042-8452 FU WKT with cooperation from the Blackland Research and Extension Center; WBI has been provided by students from the University of Iowa; NASA Iowa Space Grant Consortium; National Science Foundation Biocomplexity in the Environment Program [ATM-0221850]; DOE Office of Science-Terrestrial Carbon Processes program [DE-AC09-08SR22470]; LLC [DE-AC09-08SR22470]; US Department of Energy; California Energy Commission (CEC) Public Interest Environmental Research Program and the Director, Office of Science, Office of Basic Energy Sciences, of the US Department of Energy [DE-AC02-05CH11231]; NSF [DEB-0845166] FX We thank Peter Bakwin for valuable advice based on his experiences as lead scientist for the NOAA tall tower network. Aris Legoretta and David (Zim) Sherman contributed to design and testing of the CO2/CO system. Ron Teclaw helped to establish the LEF site and assisted with operations for more than a decade. Ranjan Muttiah, Joaquin Sanabria, and Onyango Okello provided support at WKT with cooperation from the Blackland Research and Extension Center. Local support at WBI has been provided by students from the University of Iowa, including Alicia Pettibone, Adam Beranek-Collins, Jameson Schoenfelder, Alex Bender, Robert Bullard, Ben Behrendt, and Andrew Hesselink, several of whom were sponsored by the NASA Iowa Space Grant Consortium. Site support at SNP has been provided by Temple Lee. Sonja Wolter, Jack Higgs, Doug Guenther, and Kelly Sours have contributed substantially to tower PFP sampling efforts. Colm Sweeney, Anna Karion, Huilin Chen, and Tim Newberger loaned Picarro CRDS analyzers for testing and provided advice particularly regarding installation and calibration of Picarro analyzers, uncertainty estimation, and PFP comparisons. Jeff Peischl and Tom Ryerson contributed data and results from comparisons with the NOAA P-3 CO2 analyzer. Scott Richardson and Tasha Miles carried out and analyzed data from the WBI CRDS comparison. Installation of equipment at AMT was made possible by a grant from the National Science Foundation Biocomplexity in the Environment Program (ATM-0221850). We thank Verizon Wireless for continuing support at AMT and Steve Wofsy and David Hollinger for assistance with establishing the AMT site. Installation of equipment at SCT was accomplished with funding provided by the DOE Office of Science-Terrestrial Carbon Processes program and performed under contract no. DE-AC09-08SR22470. The Savannah River National Laboratory is operated by Savannah River Nuclear Solutions, LLC under Contract No. DE-AC09-08SR22470 with the US Department of Energy. Roger Strand and others at Wisconsin Public Television have facilitated installation and maintenance of equipment at LEF. Deployment and operation of the Picarro analyzer at WGC is collaboration between NOAA ESRL and LBNL and has been supported by the California Energy Commission (CEC) Public Interest Environmental Research Program and the Director, Office of Science, Office of Basic Energy Sciences, of the US Department of Energy under contract no. DE-AC02-05CH11231. Ankur Desai's work at LEF has been supported by NSF grant no. DEB-0845166. Anna Karion, Huilin Chen, Colm Sweeney, Andrew Crotwell, and two anonymous reviewers provided many helpful suggestions for improving the paper. Referee # 1 provided an especially thorough review that motivated additional testing of our analytical system and more careful description of the uncertainty framework. NR 50 TC 42 Z9 43 U1 7 U2 59 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1867-1381 EI 1867-8548 J9 ATMOS MEAS TECH JI Atmos. Meas. Tech. PY 2014 VL 7 IS 2 BP 647 EP 687 DI 10.5194/amt-7-647-2014 PG 41 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA AC3AF UT WOS:000332386700021 ER PT J AU Stolley, RM Darmon, JM Helm, ML AF Stolley, Ryan M. Darmon, Jonathan M. Helm, Monte L. TI Solvent and electrolyte effects on Ni((P2NR)-N-R '(2))(2)-catalyzed electrochemical oxidation of hydrogen SO CHEMICAL COMMUNICATIONS LA English DT Article ID ELECTROCATALYTIC OXIDATION; PENDANT AMINES; PROTON RELAYS; CATALYSTS; WATER; CHALLENGES; REDUCTION; COMPLEXES; ANIONS; 2ND AB We report solvent and electrolyte effects on the electrocatalytic oxidation of H-2 using Ni((P2N2R')-N-Cy)(2) (R' = Bn, Bu-t) complexes. A turnover frequency of 46 s(-1) for Ni((P2N2Bn)-N-Cy)(2) was obtained using 0.2 M [(Bu4N)-Bu-n][BF4] in THF. A turnover frequency of 51 s(-1) was observed for Ni((P2N2tBu)-N-Cy)(2) using 0.2 M [(Bu4N)-Bu-n][B(C6F5)(4)] in fluorobenzene. These observations, in conjunction with previous studies, indicate nitrile binding inhibits catalysis supported by Ni((P2N2Bn)-N-Cy)(2). C1 [Stolley, Ryan M.; Darmon, Jonathan M.; Helm, Monte L.] Pacific NW Natl Lab, Ctr Mol Electrocatalysis, Div Phys Sci, Richland, WA 99352 USA. RP Helm, ML (reprint author), Pacific NW Natl Lab, Ctr Mol Electrocatalysis, Div Phys Sci, POB 999,K2-57, Richland, WA 99352 USA. EM monte.helm@pnnl.gov FU Center for Molecular Electrocatalysis; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences. Pacific Northwest National Laboratory FX This research 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, Office of Basic Energy Sciences. Pacific Northwest National Laboratory is operated by Battelle for the U.S. Department of Energy. NR 33 TC 9 Z9 9 U1 1 U2 12 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 2014 VL 50 IS 28 BP 3681 EP 3684 DI 10.1039/c4cc00295d PG 4 WC Chemistry, Multidisciplinary SC Chemistry GA AD0MF UT WOS:000332927500008 PM 24554087 ER PT J AU Udovic, TJ Matsuo, M Unemoto, A Verdal, N Stavila, V Skripov, AV Rush, JJ Takamura, H Orimo, S AF Udovic, Terrence J. Matsuo, Motoaki Unemoto, Atsushi Verdal, Nina Stavila, Vitalie Skripov, Alexander V. Rush, John J. Takamura, Hitoshi Orimo, Shin-ichi TI Sodium superionic conduction in Na2B12H12 SO CHEMICAL COMMUNICATIONS LA English DT Article ID BATTERIES; LI2B12H12; SYSTEM AB Impedance measurements indicate that Na2B12H12 exhibits dramatic Na+ conductivity (on the order of 0.1 S cm(-1)) above its order-disorder phase-transition at approximate to 529 K, rivaling that of current, solid-state, ceramic-based, Na-battery electrolytes. Superionicity may be aided by the large size, quasispherical shape, and high rotational mobility of the B12H122- anions. C1 [Udovic, Terrence J.; Verdal, Nina; Rush, John J.] NIST, NIST Ctr Neutron Res, Gaithersburg, MD 20899 USA. [Matsuo, Motoaki; Orimo, Shin-ichi] Tohoku Univ, Inst Mat Res, Sendai, Miyagi 9808577, Japan. [Unemoto, Atsushi; Orimo, Shin-ichi] Tohoku Univ, WPI Adv Inst Mat Res, Sendai, Miyagi 9808577, Japan. [Verdal, Nina; Rush, John J.] Univ Maryland, Dept Mat Sci & Engn, College Pk, MD 20742 USA. [Stavila, Vitalie] Sandia Natl Labs, Livermore, CA 94551 USA. [Skripov, Alexander V.] Russian Acad Sci, Inst Met Phys, Ural Branch, Ekaterinburg 620990, Russia. [Takamura, Hitoshi] Tohoku Univ, Grad Sch Engn, Sendai, Miyagi 9808579, Japan. RP Udovic, TJ (reprint author), NIST, NIST Ctr Neutron Res, Gaithersburg, MD 20899 USA. EM udovic@nist.gov; orimo@imr.tohoku.ac.jp RI ORIMO, Shin-ichi/A-4971-2011; matsuo, motoaki/M-9636-2014; Unemoto, Atsushi/D-3051-2013; Takamura, Hitoshi/B-9514-2014; Skripov, Alexander/K-4525-2013 OI ORIMO, Shin-ichi/0000-0002-4216-0446; matsuo, motoaki/0000-0002-3454-7018; Takamura, Hitoshi/0000-0002-4841-4582; Skripov, Alexander/0000-0002-0610-5538 FU DOE EERE [DE-EE0002978, DE-AC04-94AL85000]; Russian Foundation for Basic Research [12-03-00078]; U.S. Civilian Research & Development Foundation (CRDF Global) [RUP1-7076-EK-12]; National Science Foundation under Cooperative Agreement [OISE-9531011]; Integrated Materials Research Center for the Low-Carbon Society (LC-IMR), Tohoku University; Japan Science and Technology Agency (JST); JSPS KAKENHI [25220911] FX This work was performed, in part, in collaboration between members of IEA HIA Task 32-Hydrogen-based Energy Storage. The authors gratefully acknowledge support from DOE EERE through Grant No. DE-EE0002978 and DE-AC04-94AL85000; the Russian Foundation for Basic Research under Grant No. 12-03-00078; the U.S. Civilian Research & Development Foundation (CRDF Global) under Award No. RUP1-7076-EK-12; the National Science Foundation under Cooperative Agreement No. OISE-9531011; the Integrated Materials Research Center for the Low-Carbon Society (LC-IMR), Tohoku University; the Advanced Low Carbon Technology Research and Development Program (ALCA) from the Japan Science and Technology Agency (JST); and JSPS KAKENHI under Grant No. 25220911. The authors also thank Andrew J. Udovic for valuable discussions concerning this work. NR 21 TC 45 Z9 45 U1 7 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 2014 VL 50 IS 28 BP 3750 EP 3752 DI 10.1039/c3cc49805k PG 3 WC Chemistry, Multidisciplinary SC Chemistry GA AD0MF UT WOS:000332927500029 PM 24584582 ER PT J AU McCleskey, TM Shi, P Bauer, E Highland, MJ Eastman, JA Bi, ZX Fuoss, PH Baldo, PM Ren, W Scott, BL Burrell, AK Jia, QX AF McCleskey, T. M. Shi, P. Bauer, E. Highland, M. J. Eastman, J. A. Bi, Z. X. Fuoss, P. H. Baldo, P. M. Ren, W. Scott, B. L. Burrell, A. K. Jia, Q. X. TI Nucleation and growth of epitaxial metal-oxide films based on polymer-assisted deposition SO CHEMICAL SOCIETY REVIEWS LA English DT Review ID CHEMICAL SOLUTION DEPOSITION; THIN-FILMS AB Polymer-assisted deposition (PAD) is one of the chemical solution deposition methods which have been successfully used to grow films, form coatings, and synthesize nanostructured materials. In comparison with other conventional solution-based deposition techniques, PAD differs in its use of water-soluble polymers in the solution that prevent the metal ions from unwanted chemical reactions and keep the solution stable. Furthermore, filtration to remove non-coordinated cations and anions in the PAD process ensures well controlled nucleation, which enables the growth of high quality epitaxial films with desired structural and physical properties. The precursor solution is prepared by mixing water-soluble polymer(s) with salt(s). Thermal treatment of the precursor films in a controlled environment leads to the formation of desired materials. Using BaTiO3 grown on SrTiO3 and LaMnO3 on LaAlO3 as model systems, we show the effect of filtration on the nucleation and growth of epitaxial complex metal-oxide films based on the PAD process. C1 [McCleskey, T. M.; Bauer, E.; Bi, Z. X.; Scott, B. L.; Jia, Q. X.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Shi, P.; Ren, W.] Xi An Jiao Tong Univ, Sch Elect & Informat Eng, Xian 710049, Peoples R China. [Highland, M. J.; Eastman, J. A.; Fuoss, P. H.; Baldo, P. M.; Burrell, A. K.] Argonne Natl Lab, Argonne, IL 60439 USA. RP McCleskey, TM (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM tmark@lanl.gov; qxjia@lanl.gov RI Jia, Q. X./C-5194-2008; shi, peng/C-8551-2011; Scott, Brian/D-8995-2017; OI shi, peng/0000-0003-2217-8486; Scott, Brian/0000-0003-0468-5396; Eastman, Jeff/0000-0002-0847-4265; Mccleskey, Thomas/0000-0003-3750-3245 FU U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division; U. S. DOE [DE-C02- 06CH11357]; U.S. Department of Energy [DE-AC52-06NA25396] FX 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. The work at Argonne National Laboratory was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division. 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-C02- 06CH11357. NR 25 TC 9 Z9 9 U1 12 U2 85 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 2014 VL 43 IS 7 BP 2141 EP 2146 DI 10.1039/c3cs60285k PG 6 WC Chemistry, Multidisciplinary SC Chemistry GA AC4KH UT WOS:000332489400012 PM 24158602 ER PT J AU Orikasa, Y Crumlin, EJ Sako, S Amezawa, K Uruga, T Biegalski, MD Christen, HM Uchimoto, Y Shao-Horn, Y AF Orikasa, Yuki Crumlin, Ethan J. Sako, Shinnosuke Amezawa, Koji Uruga, Tomoya Biegalski, Michael D. Christen, Hans M. Uchimoto, Yoshiharu Shao-Horn, Yang TI Surface Strontium Segregation of Solid Oxide Fuel Cell Cathodes Proved by In Situ Depth-Resolved X-ray Absorption Spectroscopy SO ECS ELECTROCHEMISTRY LETTERS LA English DT Article ID PEROVSKITE THIN-FILMS; OXYGEN-REDUCTION ACTIVITY; ACTIVITY ENHANCEMENT; SR SEGREGATION; LA0.6SR0.4COO3-DELTA; LA1-XSRXCOO3-DELTA; NONSTOICHIOMETRY; ELECTROCATALYSIS; CONDUCTIVITY; DEGRADATION AB Little is known about the structures and chemistry of perovskites, occurring from the surface to the bulk, at high temperatures and ambient oxygen pressures. Changes in the composition and electronic structure of (001)-oriented La0.8Sr0.2CoO3-delta (LSC) films were investigated by using in situ depth-resolved X-ray adsorption (XAS) under practical operating conditions of solid oxide fuel cells. Depth-resolved XAS spectra of LSC films, with a depth resolution of similar to 2 nm, revealed that the surface regions of similar to 10 nm were considerably different from the film bulk. The surface regions were enriched in strontium, which can play an important role in governing the oxygen exchange kinetics at the surface. (C) 2014 The Electrochemical Society. All rights reserved. C1 [Orikasa, Yuki; Sako, Shinnosuke; Uchimoto, Yoshiharu] Kyoto Univ, Grad Sch Human & Environm Studies, Sakyo Ku, Kyoto 6068501, Japan. [Crumlin, Ethan J.; Shao-Horn, Yang] MIT, Dept Chem Engn, Cambridge, MA 02139 USA. [Amezawa, Koji] Tohoku Univ, Inst Multidisciplinary Res Adv Mat, Aoba Ku, Sendai, Miyagi 9808577, Japan. [Uruga, Tomoya] Japan Synchrotron Radiat Res Inst, Sayo, Hyogo 6795198, Japan. [Biegalski, Michael D.; Christen, Hans M.] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. RP Orikasa, Y (reprint author), Kyoto Univ, Grad Sch Human & Environm Studies, Sakyo Ku, Yoshida Nihonmatsu Cho, Kyoto 6068501, Japan. EM orikasa.yuuki.2a@kyoto-u.ac.jp; shaohorn@mit.edu RI Christen, Hans/H-6551-2013 OI Christen, Hans/0000-0001-8187-7469 FU Oak Ridge National Laboratory by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy FX The synchrotron radiation experiments were performed at SPring-8 with the approval of the Japan Synchrotron Radiation Research Institute (JASRI) (Proposal Nos. 2009B1607, 2009B1613, 2011B1908, 2012A1675, 2012A1678). A portion of this research was 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. The authors thank Dr. Sung-Jin Ahn for the XRD measurement. NR 43 TC 12 Z9 12 U1 5 U2 58 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 2014 VL 3 IS 4 BP F23 EP F26 DI 10.1149/2.006404eel PG 4 WC Electrochemistry; Materials Science, Multidisciplinary SC Electrochemistry; Materials Science GA AD2MI UT WOS:000333069400008 ER PT J AU Stewart, SM Spernjak, D Borup, R Datye, A Garzon, F AF Stewart, S. Michael Spernjak, Dusan Borup, Rodney Datye, Abhaya Garzon, Fernando TI Cerium Migration through Hydrogen Fuel Cells during Accelerated Stress Testing SO ECS ELECTROCHEMISTRY LETTERS LA English DT Article ID DEGRADATION MITIGATION; PEROXIDE AB Component durability of polymer-electrolyte membrane (PEM) fuel cells can be improved by adding cerium cations, which serve to scavenge harmful free radicals and selectively decompose hydrogen peroxide, which are formed during the oxidation reduction reaction (ORR). We have investigated the change in distribution of cerium cations in a hydrogen fuel cell as a function of operating time, considering both cerium containing membranes (commercial XL by DuPont) as well as fuel cells with CeO2 in the cathode catalyst layer. Our results show cerium cations are very mobile in Nafion, and migrate into both the anode and cathode catalyst layers. (C) 2014 The Electrochemical Society. All rights reserved. C1 [Stewart, S. Michael; Datye, Abhaya] Univ New Mexico, Dept Chem Engn, Albuquerque, NM 87131 USA. [Spernjak, Dusan; Borup, Rodney; Garzon, Fernando] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Stewart, SM (reprint author), Univ New Mexico, Dept Chem Engn, Albuquerque, NM 87131 USA. EM garzon@lanl.gov FU U.S. DOE, Energy Efficiency and Renewable Energy, Fuel Cell Technologies Office and Technology Development Manager Nancy Garland FX The authors wish to acknowledge the financial support of the U.S. DOE, Energy Efficiency and Renewable Energy, Fuel Cell Technologies Office and Technology Development Manager Nancy Garland. Special thanks is owed to Aaron Jenkins of UNM for his help mounting and measuring samples at Argonne, as well as Dr. Barry Lai and Dr. Zhonghou Cai of Argonne APS for their help in setting up the experiments at the APS beam line. NR 13 TC 13 Z9 13 U1 4 U2 26 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 2014 VL 3 IS 4 BP F19 EP F22 DI 10.1149/2.008404eel PG 4 WC Electrochemistry; Materials Science, Multidisciplinary SC Electrochemistry; Materials Science GA AD2MI UT WOS:000333069400007 ER PT J AU Claps, G Murtas, F Pietropaolo, A Celentano, G Vannozzi, A Santoni, A Quintieri, L Riedel, RA AF Claps, G. Murtas, F. Pietropaolo, A. Celentano, G. Vannozzi, A. Santoni, A. Quintieri, L. Riedel, R. A. TI He-3-free triple GEM thermal neutron detector SO EPL LA English DT Article ID READOUT AB A novel type of thermal neutron detector based on the gas electron multiplier (GEM) technology is presented in the framework of the research and development activity on the 3 He replacement for neutron detection. The device relies on a series of boron-coated alumina sheets placed perpendicularly to the incident neutron beam direction. The detector, named side-on GEM (S-GEM), was tested on beam at the High Flux Isotope Reactor at the Oak Ridge National Laboratory (US) to assess its performance in terms of beam position resolution, efficiency and signal-to-background (S/B) ratio as compared to a 10 bar 3 He tube for sub-thermal neutrons. Using 3mm wide PADs, a sub-millimeter position resolution was obtained. The achieved efficiency is about 30% with a quite good S/B ratio. The obtained results demonstrate the effectiveness of the proposed detector configuration to achieve a good spatial resolution and, in the perspective, a higher thermal neutron efficiency, comparable to 3 He tubes typically used for diagnostic in nuclear reactors. The main issues to be addressed to reach the goal, mostly related to boron coating procedures and characterization, are also pointed out. Copyright (c) EPLA, 2014 C1 [Claps, G.; Murtas, F.] Ist Nazl Fis Nucl, Lab Nazl Frascati, I-00044 Rome, Italy. [Murtas, F.] CERN, CH-1211 Geneva 23, Switzerland. [Pietropaolo, A.; Celentano, G.; Vannozzi, A.; Santoni, A.] ENEA, Ctr Ric Frascati, I-00044 Rome, Italy. [Pietropaolo, A.] Mediterranean Inst Fundamental Phys, MIFP, I-00040 Rome, Italy. [Quintieri, L.] ENEA, Ctr Ric Casaccia, I-00123 Rome, Italy. [Riedel, R. A.] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. RP Claps, G (reprint author), Ist Nazl Fis Nucl, Lab Nazl Frascati, Via Enrico Fermi 40, I-00044 Rome, Italy. EM antonino.pietropaolo@enea.it RI Murtas, Fabrizio/B-5729-2012; OI Murtas, Fabrizio/0000-0002-7041-6541; Quintieri, Lina/0000-0002-7547-9429; Vannozzi, Angelo/0000-0003-4628-4312 FU MEPA FX The authors warmly acknowledge A. Balla, G. Corradi and D. Tagnani from the electronic group of Istituto Nazionale di Fisica Nucleare (Laboratori Nazionali di Frascati), F. Loprete for the mechanical machining of the cathodes. Mr V. Orsetti (ENEA CR Frascati) is thanked for technical support in XPS measurements. The financial support from the MEPA project is also acknowledged. NR 20 TC 5 Z9 5 U1 0 U2 12 PU EPL ASSOCIATION, EUROPEAN PHYSICAL SOCIETY PI MULHOUSE PA 6 RUE DES FRERES LUMIERE, MULHOUSE, 68200, FRANCE SN 0295-5075 EI 1286-4854 J9 EPL-EUROPHYS LETT JI EPL PD JAN PY 2014 VL 105 IS 2 AR 22002 DI 10.1209/0295-5075/105/22002 PG 6 WC Physics, Multidisciplinary SC Physics GA AC6FT UT WOS:000332617600007 ER PT J AU Li, FX Ren, J Sinitsyn, NA AF Li, Fuxiang Ren, Jie Sinitsyn, Nikolai A. TI Quantum Zeno effect as a topological phase transition in full counting statistics and spin noise spectroscopy SO EPL LA English DT Article ID SINGLE-ELECTRON SPIN; DOT; DYNAMICS AB When the interaction of a quantum system with a detector changes from weak to strong-coupling limits, the system experiences a transition from the regime with quantum-mechanical coherent oscillations to the regime with a frozen dynamics. In addition to this quantum Zeno transition, we show that the full counting statistics of detector signal events experiences a topological phase transition at the boundary between two phases at intermediate coupling of a quantum system to the detector. We demonstrate that this transition belongs to the class of topological phase transitions that can be classified by elements of the braid group. We predict that this transition can be explored experimentally by means of the optical spin noise spectroscopy. Copyright (c) EPLA, 2014 C1 [Li, Fuxiang] Texas A&M Univ, Dept Phys, College Stn, TX 77840 USA. [Li, Fuxiang; Ren, Jie; Sinitsyn, Nikolai A.] Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. RP Li, FX (reprint author), Texas A&M Univ, Dept Phys, College Stn, TX 77840 USA. EM lifuxiang225@gmail.com; renjie@lanl.gov; nsinitsyn@lanl.gov RI Ren, Jie/G-5314-2010; Li, Fuxiang/O-9132-2015 OI Ren, Jie/0000-0003-2806-7226; FU National Nuclear Security Administration of the U. S. Department of Energy at Los Alamos National Laboratory [DE-AC52-06NA25396] FX We thank Yan Li and S. A. Crooker for useful discussions. Work at LANL was carried out under the auspices of the National Nuclear Security Administration of the U. S. Department of Energy at Los Alamos National Laboratory under Contract No. DE-AC52-06NA25396. NR 34 TC 2 Z9 2 U1 2 U2 9 PU EPL ASSOCIATION, EUROPEAN PHYSICAL SOCIETY PI MULHOUSE PA 6 RUE DES FRERES LUMIERE, MULHOUSE, 68200, FRANCE SN 0295-5075 EI 1286-4854 J9 EPL-EUROPHYS LETT JI EPL PD JAN PY 2014 VL 105 IS 2 AR 27001 DI 10.1209/0295-5075/105/27001 PG 6 WC Physics, Multidisciplinary SC Physics GA AC6FT UT WOS:000332617600017 ER PT J AU Wong, PC Huang, ZY Chen, YS Mackey, P Jin, SS AF Wong, Pak Chung Huang, Zhenyu Chen, Yousu Mackey, Patrick Jin, Shuangshuang TI Visual Analytics for Power Grid Contingency Analysis SO IEEE COMPUTER GRAPHICS AND APPLICATIONS LA English DT Article C1 [Wong, Pak Chung; Huang, Zhenyu; Chen, Yousu; Mackey, Patrick; Jin, Shuangshuang] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Wong, PC (reprint author), Pacific NW Natl Lab, Richland, WA 99352 USA. EM pak.wong@pnnl.gov; zhenyu.huang@pnnl.gov; yousu.chen@pnnl.gov; patrick.mackey@pnnl.gov; shuangshuang@pnnl.gov FU US Department of Energy (DOE) Office of Electricity Delivery & Energy Reliability through its Advanced Modeling Grid Research Program; Center for Adaptive Supercomputing Software-Multithreaded Architectures at the Pacific Northwest National Laboratory (PNNL); US Department of Homeland Security Science and Technology Directorate; DOE [DE-AC05-76RL01830] FX This research has been supported partly by the US Department of Energy (DOE) Office of Electricity Delivery & Energy Reliability through its Advanced Modeling Grid Research Program, the Center for Adaptive Supercomputing Software-Multithreaded Architectures at the Pacific Northwest National Laboratory (PNNL), and the US Department of Homeland Security Science and Technology Directorate. Battelle manages the PNNL for the DOE under contract DE-AC05-76RL01830. NR 17 TC 1 Z9 1 U1 0 U2 3 PU IEEE COMPUTER SOC PI LOS ALAMITOS PA 10662 LOS VAQUEROS CIRCLE, PO BOX 3014, LOS ALAMITOS, CA 90720-1314 USA SN 0272-1716 EI 1558-1756 J9 IEEE COMPUT GRAPH JI IEEE Comput. Graph. Appl. PD JAN-FEB PY 2014 VL 34 IS 1 BP 42 EP 51 PG 10 WC Computer Science, Software Engineering SC Computer Science GA AC8EB UT WOS:000332764800007 ER PT J AU Lee, SH Kim, CK Shim, HS Yoo, JH Russo, RE Jeong, S AF Lee, Seok-Hee Kim, Chan-Kyu Shim, Hee-Sang Yoo, Jong-Hyun Russo, Richard E. Jeong, Sungho TI Ablation and Spectroscopic Characteristics of Thin CuIn1-xGaxSe2 Solar Cell Films Fabricated by Co-Evaporation and Co-Sputtering Processes SO INTERNATIONAL JOURNAL OF PRECISION ENGINEERING AND MANUFACTURING-GREEN TECHNOLOGY LA English DT Article ID INDUCED BREAKDOWN SPECTROSCOPY; LASER-INDUCED PLASMA; ECHELLE SPECTROMETER; CU(IN,GA)SE-2; SILICON; SAMPLES; SUBSTRATE; POWDERS AB The influence of fabrication processes on the LIBS (Laser Induced Breakdown Spectroscopy) spectra of major and minor chemical constituents in CuIn1-xGaxSe2 (CIGS) absorber films produced by co-sputtering and co-evaporation techniques on Mo-coated soda lime glass (SLG) is reported. It was found that the ablation rate per pulse of CIGS layers fabricated by the co-sputtering technique is higher than those fabricated by the co-evaporation technique, resulting in higher LIBS signal intensities of the constituent elements. The examination of surface morphology of irradiated surfaces and changes in LIBS signal intensities revealed evidences of elemental fractionation for the CIGS films fabricated by co-sputtering technique but not for those by co-evaporation technique. From x-ray diffraction measurements, it was confirmed that the differences in the ablation and spectroscopic characteristics of the two different types of CIGS absorber films were contributed to the differences in crystalline properties. Furthermore, it was demonstrated that LIBS can effectively determine a depth profile of sodium concentration in CIGS thin films, diffused from SLG. C1 [Lee, Seok-Hee; Kim, Chan-Kyu; Jeong, Sungho] Gwangju Inst Sci & Technol, Sch Mechatron, Kwangju 500712, South Korea. [Shim, Hee-Sang] Gwangju Inst Sci & Technol, Res Inst Solar & Sustainable Energies, Kwangju 500712, South Korea. [Yoo, Jong-Hyun; Russo, Richard E.] Appl Spectra Inc, Fremont, CA 94538 USA. [Russo, Richard E.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Jeong, S (reprint author), Gwangju Inst Sci & Technol, Sch Mechatron, 1 Oryong Dong, Kwangju 500712, South Korea. EM shjeong@gist.ac.kr FU National Research Foundation of Korea (NRF); Korea government (MEST) [2013-064113] FX This work was supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MEST) (No. 2013-064113). NR 55 TC 2 Z9 2 U1 2 U2 20 PU KOREAN SOC PRECISION ENG PI SEOUL PA RM 306, KWANGMYUNG BLDG, 5-4 NONHYUN-DONG, KANGNAM-GU, SEOUL, 135-010, SOUTH KOREA SN 2288-6206 EI 2198-0810 J9 INT J PR ENG MAN-GT JI Int. J. Precis Eng Manuf-Green Technol. PD JAN PY 2014 VL 1 IS 1 BP 17 EP 24 DI 10.1007/s40684-014-0003-6 PG 8 WC GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY; Engineering, Manufacturing; Engineering, Mechanical SC Science & Technology - Other Topics; Engineering GA AC6PR UT WOS:000332646800003 ER PT J AU Falcini, F Piliouras, A Garra, R Guerin, A Jerolmack, DJ Rowland, J Paola, C AF Falcini, F. Piliouras, A. Garra, R. Guerin, A. Jerolmack, D. J. Rowland, J. Paola, C. TI Hydrodynamic and suspended sediment transport controls on river mouth morphology SO JOURNAL OF GEOPHYSICAL RESEARCH-EARTH SURFACE LA English DT Article DE river mouth; suspended sediment; potential vorticity ID MISSISSIPPI DELTA; DEPOSITION; FLOWS; JET AB River mouths building into standing bodies of water have strikingly varied growth habits. This presents a compelling pattern formation problem that is also of great practical relevance for subsurface prediction and managing coastal wetlands. Here we present a generalized 2.5-dimensional potential vorticity (PV) theory that explains sedimentation patterns of a sediment-laden stationary jet by coupling an understanding of vorticity with suspended sediment concentration fields. We explore the physical meaning of this new sediment-PV definition, and its impact on outflow depositional patterns, by analyzing data from a shallow wall-bounded plane jet experiment and by discussing new theoretical insights. A key result is that lateral advection and diffusion of suspended sediment are directly proportional to jet vorticity, a feature that reveals the mechanistic process that forms elongated channels by focused levee deposition. The new PV theory constitutes a more generalized mathematical framework that expands the Rouse theory for the equilibrium of suspended sediment. Key Points Lateral advection/diffusion of suspended sediment are proportional to vorticity Our mathematical framework generalizes the Rouse theory for suspended sediment We probe processes that lead to the formation of various channel patterns C1 [Falcini, F.] CNR, Ist Sci Atmosfera & Clima, Rome, Italy. [Piliouras, A.] Univ Texas Austin, Dept Geol Sci, Austin, TX USA. [Garra, R.] Univ Roma La Sapienza, Dipartimento Sci Base & Applicate Ingn, Rome, Italy. [Guerin, A.] Univ Paris Diderot, Inst Phys Globe Paris, Equipe Dynam Fluides Geol, Paris, France. [Jerolmack, D. J.] Univ Penn, Dept Earth & Environm Sci, Philadelphia, PA 19104 USA. [Rowland, J.] Los Alamos Natl Lab, Div Earth & Environm Sci, Los Alamos, NM 87545 USA. [Paola, C.] Univ Minnesota, Dept Geol & Geophys, Minneapolis, MN USA. RP Falcini, F (reprint author), CNR, Ist Sci Atmosfera & Clima, Rome, Italy. EM f.falcini@isac.cnr.it OI Falcini, Federico/0000-0001-8105-2491 FU National Science Foundation through National Center for Earth-surface Dynamics (NCED), a Science and Technology Center [EAR-0746138, EAR-0120914]; FESD: A Delta Dynamics Collaboratory under Italian National Flag Project RITMARE (Marine Italian Research) [EAR-1135427]; Italian Ministry of Education, University and Research within the National Research Program; National Center for Earth-surface Dynamics FX We gratefully acknowledge the support by the National Science Foundation through contract EAR-0746138 to D.J.J., via the National Center for Earth-surface Dynamics (NCED), a Science and Technology Center funded under agreement EAR-0120914, and by FESD: A Delta Dynamics Collaboratory under agreement EAR-1135427 to C. P., via the Italian National Flag Project RITMARE (Marine Italian Research) funded by the Italian Ministry of Education, University and Research within the National Research Program 2011-2013 to FF. This work was inspired by discussions at the Doolin "deltas workshop" with A. Fowler, C. Stark, J. Swenson, and V. Voller, sponsored by the National Center for Earth-surface Dynamics. NR 38 TC 3 Z9 4 U1 0 U2 15 PU AMER GEOPHYSICAL UNION PI WASHINGTON PA 2000 FLORIDA AVE NW, WASHINGTON, DC 20009 USA SN 2169-9003 EI 2169-9011 J9 J GEOPHYS RES-EARTH JI J. Geophys. Res.-Earth Surf. PD JAN PY 2014 VL 119 IS 1 BP 1 EP 11 DI 10.1002/2013JF002831 PG 11 WC Geosciences, Multidisciplinary SC Geology GA AD1YL UT WOS:000333029500001 ER PT J AU Huff, AG Kircher, A Hodges, JS Kennedy, S AF Huff, Andrew G. Kircher, Amy Hodges, James S. Kennedy, Shaun TI State Officials' Perceptions of the Food and Agriculture Sector Criticality Assessment Tool (FASCAT), Food-system Risk, and Food Defense Funding SO JOURNAL OF HOMELAND SECURITY AND EMERGENCY MANAGEMENT LA English DT Article DE cognitive bias; criticality assessment; food defense funding; resource allocation; risk perception ID BIAS; ANXIETY AB Determining food system criticality is necessary to mitigate risks to the nation's food supply and prioritize and allocate funding. The Food and Agriculture Sector Criticality Assessment Tool (FASCAT) is a tool used broadly by state governments to determine the criticality of food systems throughout the US State officials (SOs) responsible for food defense (n=32) were surveyed to determine whether FASCAT is of value to food defense and to determine SOs' security beliefs, values, and practices related to food defense. Results indicated that: (1) SOs believe FASCAT is easier to use than other forms of risk assessment; (2) FASCAT training may have introduced bias into assessment of probability, threat, vulnerability, and consequences; (3) FASCAT is valuable to SOs; (4) SOs do not routinely follow security management best practices; (5) SOs believe that intentional biological threats to the food system are the most probable threats, though without supporting evidence; and (6) SOs believe food defense risk mitigation is not adequately funded by state or federal governments. These findings indicate that even though bias was potentially introduced to FASCAT assessments, SOs believe FASCAT has been useful to them in determining food system criticality. SOs indicate that more funding is needed from state and federal governments to adequately mitigate and manage food defense risks, and that they require more comprehensive training from food defense subject matter experts in threat assessment, risk mitigation, and security management to reduce the possibility of bias from FASCAT training. C1 [Huff, Andrew G.] Sandia Natl Labs, Natl Infrastruct Simulat & Anal Ctr, Albuquerque, NM 87185 USA. [Kircher, Amy] Univ Minnesota, Natl Ctr Food Protect & Def, St Paul, MN 55108 USA. [Hodges, James S.] Univ Minnesota, Minneapolis, MN USA. [Kennedy, Shaun] Univ Minnesota, St Paul, MN 55108 USA. RP Huff, AG (reprint author), Sandia Natl Labs, Natl Infrastruct Simulat & Anal Ctr, POB 5800, Albuquerque, NM 87185 USA. EM aghuff@sandia.gov NR 27 TC 1 Z9 1 U1 3 U2 9 PU WALTER DE GRUYTER GMBH PI BERLIN PA GENTHINER STRASSE 13, D-10785 BERLIN, GERMANY SN 2194-6361 EI 1547-7355 J9 J HOMEL SECUR EMERG JI J. Homel. Secur. Emerg. Manag. PY 2014 VL 11 IS 1 BP 101 EP 116 DI 10.1515/jhsem-2013-0063 PG 16 WC Public Administration SC Public Administration GA AC4XT UT WOS:000332525300007 ER PT J AU Lerner, K Bertram, K AF Lerner, Ken Bertram, Ken TI Common Issues in Emergency Public Information as Identified in CSEPP Exercises SO JOURNAL OF HOMELAND SECURITY AND EMERGENCY MANAGEMENT LA English DT Article DE crisis communications; emergency public information; media; media relations; public warning AB The US Chemical Stockpile Emergency Preparedness Program (CSEPP) has been holding multiple large hazmat exercises every year for over 20 years. A sample of CSEPP after-action reports were surveyed to extract issues relating to emergency public information. Analysis showed four themes among the identified issues, relating to accuracy of public warnings and news releases; coordination of information among jurisdictions; internal communications; and accuracy/completeness of information provided to individual callers. These issues and the solutions suggested by exercise evaluators are consistent with the current body of knowledge in crisis communications. While these themes emerged from study of particular traditional emergency public information techniques and situations, the lessons they give may be applied to a variety of emergency public information channels including social media. C1 [Lerner, Ken; Bertram, Ken] Argonne Natl Lab, Div Decis & Informat Sci, Argonne, IL 60439 USA. RP Lerner, K (reprint author), Argonne Natl Lab, Div Decis & Informat Sci, Bldg 221 9700 S Cass Ave, Argonne, IL 60439 USA. EM klerner@anl.gov NR 22 TC 2 Z9 2 U1 1 U2 6 PU WALTER DE GRUYTER GMBH PI BERLIN PA GENTHINER STRASSE 13, D-10785 BERLIN, GERMANY SN 2194-6361 EI 1547-7355 J9 J HOMEL SECUR EMERG JI J. Homel. Secur. Emerg. Manag. PY 2014 VL 11 IS 1 BP 155 EP 168 DI 10.1515/jhsem-2013-0059 PG 14 WC Public Administration SC Public Administration GA AC4XT UT WOS:000332525300010 ER PT J AU Rangasamy, E Sahu, G Keum, JK Rondinone, AJ Dudney, NJ Liang, CD AF Rangasamy, Ezhiylmurugan Sahu, Gayatri Keum, Jong Kahk Rondinone, Adam J. Dudney, Nancy J. Liang, Chengdu TI A high conductivity oxide-sulfide composite lithium superionic conductor SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID SPACE-CHARGE REGIONS; SOLID 2-PHASE SYSTEMS; IONIC-CONDUCTIVITY; TETRAGONAL LI7LA3ZR2O12; SULFUR BATTERIES; ELECTROLYTES; PHASE; AL; SUBSTITUTION; ENHANCEMENT AB Best of both worlds: a composite electrolyte of LLZO and LPS successfully combines low grain boundary resistance, room temperature processability and low interfacial resistance of LPS with the excellent electrochemical stability and ionic conductivity of LLZO. The composite electrolyte improves the ionic conductivity of parent electrolytes and augments exceptional compatibility with metallic lithium, thereby making the electrolyte attractive for practical solid-state batteries. C1 [Rangasamy, Ezhiylmurugan; Sahu, Gayatri; Keum, Jong Kahk; Rondinone, Adam J.; Liang, Chengdu] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. [Dudney, Nancy J.] Oak Ridge Natl Lab, Div Mat Sci & Technol, 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 Keum, Jong/N-4412-2015; Rondinone, Adam/F-6489-2013; Dudney, Nancy/I-6361-2016 OI Keum, Jong/0000-0002-5529-1373; Rondinone, Adam/0000-0003-0020-4612; Dudney, Nancy/0000-0001-7729-6178 FU Division of Materials sciences and Engineering, Office of Basic Energy Sciences U.S. Department of Energy (DOE); Oak Ridge National Laboratory by the Division of Scientific User Facilities, U.S. DOE; U.S. Department of Energy (DOE)/Energy Efficiency and Renewable Energy (EERE) through the Office of Vehicle Technologies FX This work was sponsored by the Division of Materials sciences and Engineering, Office of Basic Energy Sciences U.S. Department of Energy (DOE). The synthesis and characterization of materials were conducted at the Center for Nanophase Materials Sciences, which is sponsored at Oak Ridge National Laboratory by the Division of Scientific User Facilities, U.S. DOE. Potential use of this solid electrolyte in lithium-sulfur batteries was supported by the U.S. Department of Energy (DOE)/Energy Efficiency and Renewable Energy (EERE) through the Office of Vehicle Technologies. NR 37 TC 14 Z9 14 U1 17 U2 166 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 2014 VL 2 IS 12 BP 4111 EP 4116 DI 10.1039/c3ta15223e PG 6 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA AC3BB UT WOS:000332388900002 ER PT J AU Jiang, XY Pan, YX Huang, SM Chen, X Wang, JG Liu, GK AF Jiang, Xianyu Pan, Yuexiao Huang, Shaoming Chen, Xi'an Wang, Jiaguo Liu, Guokui TI Hydrothermal synthesis and photoluminescence properties of red phosphor BaSiF6:Mn4+ for LED applications SO JOURNAL OF MATERIALS CHEMISTRY C LA English DT Article ID MAGNESIUM FLUOROGERMANATE PHOSPHORS; LIGHT-EMITTING-DIODES; LUMINESCENCE PROPERTIES; CAAL12O19/MN4+; MG2+ AB An efficient red phosphor, BaSiF6:Mn4+ free of manganese oxide impurities, has been synthesized by using a one-step hydrothermal method at 120 degrees C for 12 h. The synthesis and chemical reactions have been investigated in detail and it includes: (a) influence of starting materials, concentrations of KMnO4 and HF, reaction temperature and time on products; (b) redox reaction of KMnO4 by HF; (c) chemical reaction mechanism for red phosphor BaSiF6:Mn4+center dot Mn4+ ions, acting as activators in the phosphor, originated from KMnO4 reduced by HF. The composition and crystal structure were determined with XRD, EDS and XPS. The morphology and thermal stability were investigated by SEM and TG-DSC, respectively. The maximum absorption band (at 460 nm) of the phosphor overlaps well with the blue emission of commercial InGaN LED. The room temperature emission spectrum of the phosphor shows a typical emission (centered at 632 nm) of Mn4+ in complex fluorides. The characteristic broad excitation band and sharp emission peaks of this red phosphor are desirable for potential applications as a red phosphor or for improving the color rendering index of conventional white LEDs. C1 [Jiang, Xianyu; Pan, Yuexiao; Huang, Shaoming; Chen, Xi'an; Wang, Jiaguo] Wenzhou Univ, Fac Chem & Mat Engn, Nanomat & Chem Key Lab, Wenzhou 325027, Zhejiang, Peoples R China. [Liu, Guokui] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. RP Pan, YX (reprint author), Wenzhou Univ, Fac Chem & Mat Engn, Nanomat & Chem Key Lab, Wenzhou 325027, Zhejiang, Peoples R China. EM yxpan8@gmail.com; gkliu@anl.gov FU Chinese NSF [51102185]; Zhejiang Provincial Science and Technology [KZ1209005]; Qianjiang Talents Project [QJD1302005]; U.S. Department of Energy, Office of Basic Sciences [DE-AC02-06CH11357] FX This research was jointly supported by Chinese NSF (Grant no. 51102185), Zhejiang Provincial Science and Technology (Grant no. KZ1209005) and, Qianjiang Talents Project (Grant no. QJD1302005). Work performed at ANL was supported by the U.S. Department of Energy, Office of Basic Sciences, under contract DE-AC02-06CH11357. NR 27 TC 54 Z9 54 U1 10 U2 96 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 2014 VL 2 IS 13 BP 2301 EP 2306 DI 10.1039/c3tc31878h PG 6 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA AC4HR UT WOS:000332482400003 ER PT J AU Pasquarelli, RM van Hest, MFAM Parilla, PA Perkins, JD O'Hayre, R Ginley, DS AF Pasquarelli, Robert M. van Hest, Maikel F. A. M. Parilla, Philip A. Perkins, John D. O'Hayre, Ryan Ginley, David S. TI Processing-phase diagrams: a new tool for solution-deposited thin-film development applied to the In5O(OPri)(13)-In2O3 system SO JOURNAL OF MATERIALS CHEMISTRY C LA English DT Article ID TRANSPARENT CONDUCTING OXIDES; INDIUM-TIN-OXIDE; PULSED-LASER DEPOSITION; IN2O3 FILMS; LOW-TEMPERATURE; SOL-GEL; CRYSTALLIZATION; TRANSISTORS; ISOPROPOXIDES; ALUMINUM AB Understanding processing-property relationships of a precursor is important for achieving the desired properties in opto-electronic thin-films. This work highlights the construction of a processing-phase diagram of the novel In2O3 precursor In5O(OPri)(13) for transparent conducting oxide applications. The decomposition behavior of the precursor was profiled with thermogravimetry, differential scanning calorimetry, and temperature programmed desorption mass spectroscopy. Decomposition occurred at 150-230 degrees C. Higher temperature exothermic reactions were identified as structural rearrangement/ordering processes. The precursor powder was found to crystallize into the bixbyite structure at 300-350 degrees C, presenting a non-crystalline phase-processing window for the material. Crystallization of a film was monitored with in situ X-ray diffraction annealing, which showed a markedly higher crystallization onset of 500 degrees C and a much larger non-crystalline oxide window. The decomposition and crystallization behavior of the precursor powders and films were combined into a master processing-phase diagram. Solution deposited, crystalline In2O3 films annealed under Ar-4%H-2 achieved a conductivity of 165 S cm(-1) with high visible transparency (80%) and exhibited a mobility of 9.6 cm(2) V-1 s(-1) with a carrier concentration of 1.1 x 10(20) cm(-3). C1 [Pasquarelli, Robert M.; O'Hayre, Ryan] Colorado Sch Mines, Dept Met & Mat Engn, Golden, CO 80401 USA. [van Hest, Maikel F. A. M.; Parilla, Philip A.; Perkins, John D.; Ginley, David S.] Natl Renewable Energy Lab, Golden, CO 80401 USA. RP Pasquarelli, RM (reprint author), Colorado Sch Mines, Dept Met & Mat Engn, Golden, CO 80401 USA. EM robert.pasquarelli@gmail.com FU SunShot Initiative by the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Office of Solar Energy Technology [DE-AC36-08GO28308] FX This work was supported as part of the SunShot Initiative by the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Office of Solar Energy Technology under Award Number DE-AC36-08GO28308 to the National Renewable Energy Laboratory (NREL). The authors thank Calvin Curtis and Alexander Miedaner for their chemistry assistance in the laboratory and Harvey Guthrey for help with TEM preparation and imaging. NR 42 TC 0 Z9 0 U1 0 U2 7 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 2014 VL 2 IS 13 BP 2360 EP 2367 DI 10.1039/c3tc31930j PG 8 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA AC4HR UT WOS:000332482400013 ER PT S AU Zerbs, S Giuliani, S Collart, F AF Zerbs, Sarah Giuliani, Sarah Collart, Frank BE Lorsch, J TI Small-Scale Expression of Proteins in E. coli SO LABORATORY METHODS IN ENZYMOLOGY: PROTEIN PT A SE Methods in Enzymology LA English DT Review; Book Chapter ID ESCHERICHIA-COLI; IMPROVE; AUTOINDUCTION; MEMBRANE; SYSTEMS; GENES AB Proteins participate in virtually every cellular activity, and a knowledge of protein function is essential for an understanding of biological systems. However, protein diversity necessitates the application of an array of in vivo and in vitro approaches for characterization of the functional and biochemical properties of proteins. Methods that enable production of proteins for in vitro studies are critical for determination of the molecular, kinetic, and thermodynamic properties of these molecules. Ideally, proteins could be purified from the original source; however, the native host is often unsuitable for a number. of reasons. Consequently, systems for heterologous protein production are commonly used to produce large amounts of protein. Heterologous expression hosts are chosen using a number of criteria, including genetic tractability, advantageous production or processing characteristics (secretion or posttranslational modifications), or economy of time and growth requirements. The subcloning process also provides an opportunity to introduce purification tags, epitope tags, fusions, truncations, and mutations into the coding sequence that may be useful in downstream purification or characterization applications. Bacterial systems for heterologous protein expression have advantages in ease of use, cost, short generation times, and scalability. These expression systems have been widely used by high-throughput protein production projects and often represent an initial experiment for any expression target. Escherichia coli has been studied for many years as a model bacterial organism and is one of the most popular hosts for heterologous protein expression (Terpe, 2006). Its protein production capabilities have been intensively studied, and the ease of genetic manipulation in this organism has led to the development of strains engineered exclusively for use in protein expression. These resources are widely available from commercial sources and public repositories. Despite these advantages, many targets are unsuitable for expression in E. coli, and attempts will not yield protein that can be utilized in downstream applications. A thorough understanding of the protein target, the requirements of the final application, and available tools are all essential for planning a successful expression experiment. This protocol is designed to optimize expression and solubility using an E. coli host and expression vector with an IPTG-inducible T7 promoter. The general features of the method are easily extended to other organisms and expression systems. Small-scale expression cultures are used to identify the optimum expression parameters for a given target. Thorough analysis of the total cell content and soluble fraction is used to screen out failed targets and those unlikely to succeed in large-scale purification cultures. The protocol listed here can be used in individual tubes for a small number of targets or adapted for use in 48-well plates for high throughput applications (Abdullah et al., 2009). Using the same culture for initial expression analysis and solubility analysis reduces variability between expression trials and saves the time required to produce separate cultures. C1 [Zerbs, Sarah; Giuliani, Sarah; Collart, Frank] Argonne Natl Lab, Biosci Div, Lemont, IL 60439 USA. RP Collart, F (reprint author), Argonne Natl Lab, Biosci Div, Lemont, IL 60439 USA. EM fcollart@anl.gov OI Collart, Frank/0000-0001-6942-4483 NR 14 TC 2 Z9 2 U1 6 U2 57 PU ELSEVIER ACADEMIC PRESS INC PI SAN DIEGO PA 525 B STREET, SUITE 1900, SAN DIEGO, CA 92101-4495 USA SN 0076-6879 BN 978-0-12-420070-8 J9 METHOD ENZYMOL JI Methods Enzymol. PY 2014 VL 536 BP 117 EP 131 DI 10.1016/B978-0-12-420070-8.00011-8 PG 15 WC Biochemical Research Methods; Biochemistry & Molecular Biology SC Biochemistry & Molecular Biology GA BA0TV UT WOS:000332260100012 PM 24423272 ER PT J AU Nguyen, TD Carrillo, JMY Matheson, MA Brown, WM AF Trung Dac Nguyen Carrillo, Jan-Michael Y. Matheson, Michael A. Brown, W. Michael TI Rupture mechanism of liquid crystal thin films realized by large-scale molecular simulations SO NANOSCALE LA English DT Article ID NEMATIC-ISOTROPIC TRANSITION; DISJOINING-PRESSURE ISOTHERMS; POLYMER-FILMS; COMPUTER-SIMULATION; PATTERN-FORMATION; PHASE-DIAGRAM; METAL-FILMS; DYNAMICS; INSTABILITY; MODEL AB The ability of liquid crystal (LC) molecules to respond to changes in their environment makes them an interesting candidate for thin film applications, particularly in bio-sensing, bio-mimicking devices, and optics. Yet the understanding of the (in) stability of this family of thin films has been limited by the inherent challenges encountered by experiment and continuum models. Using unprecedented large-scale molecular dynamics (MD) simulations, we address the rupture origin of LC thin films wetting a solid substrate at length scales similar to those in experiment. Our simulations show the key signatures of spinodal instability in isotropic and nematic films on top of thermal nucleation, and importantly, for the first time, evidence of a common rupture mechanism independent of initial thickness and LC orientational ordering. We further demonstrate that the primary driving force for rupture is closely related to the tendency of the LC mesogens to recover their local environment in the bulk state. Our study not only provides new insights into the rupture mechanism of liquid crystal films, but also sets the stage for future investigations of thin film systems using peta-scale molecular dynamics simulations. C1 [Trung Dac Nguyen; Carrillo, Jan-Michael Y.; Matheson, Michael A.; Brown, W. Michael] Oak Ridge Natl Lab, Natl Ctr Computat Sci, Oak Ridge, TN 37831 USA. RP Nguyen, TD (reprint author), Oak Ridge Natl Lab, Natl Ctr Computat Sci, Oak Ridge, TN 37831 USA. EM nguyentd@ornl.gov; brownw@ornl.gov RI Carrillo, Jan-Michael/K-7170-2013; Nguyen, Trung/H-7008-2012 OI Carrillo, Jan-Michael/0000-0001-8774-697X; Nguyen, Trung/0000-0002-5076-264X FU Office of Advanced Scientific Computing Research, Office of Science, U.S. Department of Energy [DE-AC05-00OR22725]; UT-Battelle, LLC. FX This research used resources of the Leadership Computing Facility at Oak Ridge National Laboratory and was conducted under the auspices of the Office of Advanced Scientific Computing Research, Office of Science, U.S. Department of Energy under Contract no. DE-AC05-00OR22725 with UT-Battelle, LLC. Accordingly, the U. S. Government retains a nonexclusive, royalty-free license to publish or reproduce the published form of this contribution, or allow others to do so, for U. S. Government purposes. NR 94 TC 8 Z9 8 U1 1 U2 28 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 2014 VL 6 IS 6 BP 3083 EP 3096 DI 10.1039/c3nr05413f PG 14 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA AC6AY UT WOS:000332604200012 PM 24264516 ER PT J AU Yang, M Campbell, PS Santini, CC Mudring, AV AF Yang, Mei Campbell, Paul S. Santini, Catherine C. Mudring, Anja-Verena TI Small nickel nanoparticle arrays from long chain imidazolium ionic liquids SO NANOSCALE LA English DT Article ID METAL NANOPARTICLES; CATALYTIC-PROPERTIES; CARBON NANOTUBES; CRYSTALS; STABILIZATION; HYDROGENATION; METALLIZATION; NANOCRYSTALS; PRECURSOR; VERSATILE AB A series of six long chain alkyl mono-and bi-cationic imidazolium based salts with bis(trifluoromethylsulfonyl) imide (NTf2-) as the anion were synthesized and characterized. The single crystal structure of 1-methyl-3-octadecylimidazolium bis(trifluoromethylsulfonyl) imide could be obtained by X-ray analysis. All these long chain alkyl imidazolium based ILs were applied in the synthesis of nickel nanoparticles via chemical decomposition of an organometallic precursor of nickel. In these media, spontaneous decomposition of Ni(COD)(2) (COD = 1,5-cyclooctadiene) in the absence of H-2 occurred giving small NPs (<= 4 nm) with narrow size distributions. Interestingly, formation of regularly interspaced NP arrays was also observed in long chain ILs. Such array formation could be interesting for potential applications such as carbon nanotube growth. C1 [Yang, Mei; Campbell, Paul S.; Mudring, Anja-Verena] Ruhr Univ Bochum, Fak Chem Biochem, D-44780 Bochum, Germany. [Santini, Catherine C.] Univ Lyon 1, Inst Chim Lyon, UMR CNRS 5265, ESCPE Lyon,C2P2,Equipe Chim Organometall Surface, F-69616 Villeurbanne, France. [Mudring, Anja-Verena] Iowa State Univ, Dept Mat Sci & Engn, Ames, IA 50010 USA. [Mudring, Anja-Verena] US DOE, Ames Lab, Ames, IA 50010 USA. RP Mudring, AV (reprint author), Ruhr Univ Bochum, Fak Chem Biochem, D-44780 Bochum, Germany. EM catherine.santini@univ-lyon1.fr; anja.mudring@ruhr-uni-bochum.de FU German Science Foundation DFG through the priority program 1191; DFG Cluster of Excellence RESOLV; DESY (Deutsches Elektronensynchrotron) [I-20100011]; Alexander von Humboldt foundation FX This work was supported by the German Science Foundation DFG through the priority program 1191 "Ionic Liquids", the DFG Cluster of Excellence RESOLV and the DESY (Deutsches Elektronensynchrotron proposal no. I-20100011). We thank Dr Sergio Funari for support during the SAXS measurements. The authors would like to thank Philippe Arquilliere and Inga S. Helgadottir for TEM measurements. P. C. also acknowledges funding from the Alexander von Humboldt foundation. NR 43 TC 15 Z9 15 U1 7 U2 70 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 2014 VL 6 IS 6 BP 3367 EP 3375 DI 10.1039/c3nr05048c PG 9 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA AC6AY UT WOS:000332604200047 PM 24526274 ER PT J AU McInnes, LC Smith, B Zhang, H Mills, RT AF McInnes, Lois Curfman Smith, Barry Zhang, Hong Mills, Richard Tran TI Hierarchical Krylov and nested Krylov methods for extreme-scale computing SO PARALLEL COMPUTING LA English DT Article DE Hierarchical; Nested; Krylov methods; Variable preconditioner ID NONSYMMETRIC LINEAR-SYSTEMS; ALGORITHM; INNER; GMRES AB The solution of large, sparse linear systems is often a dominant phase of computation for simulations based on partial differential equations, which are ubiquitous in scientific and engineering applications. While preconditioned Krylov methods are widely used and offer many advantages for solving sparse linear systems that do not have highly convergent, geometric multigrid solvers or specialized fast solvers, Krylov methods encounter well-known scaling difficulties for over 10,000 processor cores because each iteration requires at least one vector inner product, which in turn requires a global synchronization that scales poorly because of internode latency. To help overcome these difficulties, we have developed hierarchical Krylov methods and nested Krylov methods in the PETSc library that reduce the number of global inner products required across the entire system (where they are expensive), though freely allow vector inner products across smaller subsets of the entire system (where they are inexpensive) or use inner iterations that do not invoke vector inner products at all. Nested Krylov methods are a generalization of inner-outer iterative methods with two or more layers. Hierarchical Krylov methods are a generalization of block Jacobi and overlapping additive Schwarz methods, where each block itself is solved by Krylov methods on smaller blocks. Conceptually, the hierarchy can continue recursively to an arbitrary number of levels of smaller and smaller blocks. As a specific case, we introduce the hierarchical FGMRES method, or h-FGMRES, and we demonstrate the impact of two-level h-FGMRES with a variable preconditioner on the PFLOTRAN subsurface flow application. We also demonstrate the impact of nested FGMRES, BiCGStab and Chebyshev methods. These hierarchical Krylov methods and nested Krylov methods significantly reduced overall PFLOTRAN simulation time on the Cray XK6 when using 10,000 through 224,000 cores through the combined effects of reduced global synchronization due to fewer global inner products and stronger inner hierarchical or nested preconditioners. (C) 2013 Elsevier B.V. All rights reserved. C1 [McInnes, Lois Curfman; Smith, Barry; Zhang, Hong] Argonne Natl Lab, Math & Comp Sci Div, Argonne, IL 60439 USA. [Zhang, Hong] IIT, Dept Comp Sci, Chicago, IL 60616 USA. [Mills, Richard Tran] Oak Ridge Natl Lab, Div Environm Sci, Oak Ridge, TN 37831 USA. [Mills, Richard Tran] Univ Tennessee, Dept Elect Engn & Comp Sci, Dept Earth & Planetary Sci, Knoxville, TN 37936 USA. RP Zhang, H (reprint author), Argonne Natl Lab, Math & Comp Sci Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM mcinnes@mcs.anl.gov; smith@mcs.anl.gov; hzhang@mcs.anl.gov; rmills@ornl.gov FU Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]; Office of Science of the Department of Energy [DE-AC05-00OR22725]; Office of Advanced Scientific Computing Research, Office of Science, U.S. Department of Energy [DE-AC02-06CH11357]; Climate and Environmental Sciences Division of the Office of Biological and Environmental Research (BER); Computational Science Research and Partnerships Division of the Office of Advanced Scientific Computing Research within the U.S. Department of Energy's Office of Science FX 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. We gratefully acknowledge the use of the Cray XE6 at NERSC for preliminary studies on hierarchical Krylov methods and the three-layer nested Krylov experiments that are summarized in Table 5. This research also used resources of the National Center for Computational Sciences at Oak Ridge National Laboratory, which is supported by the Office of Science of the Department of Energy under Contract DE-AC05-00OR22725.; L.C. McInnes, B. Smith, and H. Zhang were supported by the Office of Advanced Scientific Computing Research, Office of Science, U.S. Department of Energy, under Contract DE-AC02-06CH11357. R. Mills was partially supported by the Climate and Environmental Sciences Division of the Office of Biological and Environmental Research (BER) and the Computational Science Research and Partnerships Division of the Office of Advanced Scientific Computing Research within the U.S. Department of Energy's Office of Science. NR 46 TC 7 Z9 7 U1 1 U2 7 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0167-8191 EI 1872-7336 J9 PARALLEL COMPUT JI Parallel Comput. PD JAN PY 2014 VL 40 IS 1 BP 17 EP 31 DI 10.1016/j.parco.2013.10.001 PG 15 WC Computer Science, Theory & Methods SC Computer Science GA AD0HB UT WOS:000332914000002 ER PT J AU Dong, Y Wang, H Nolas, GS AF Dong, Yongkwan Wang, Hsin Nolas, George S. TI Synthesis and thermoelectric properties of Cu excess Cu2ZnSnSe4 SO PHYSICA STATUS SOLIDI-RAPID RESEARCH LETTERS LA English DT Article DE stannites; thermoelectrics; semiconductors; Cu2ZnSnSe4 ID BULK THERMOELECTRICS; NANOCRYSTALS; CU2CDSNSE4 AB Quaternary stannites with an excess of copper were successfully synthesized by reacting the constituent elements and subsequent solid state annealing, followed by densification by hot-pressing. The composition for each specimen was confirmed with a combination of Rietveld refinement and elemental analysis. Their high temperature thermoelectric properties were measured from 300 K to 800 K and compared with that of Cu2ZnSnSe4. The thermal conductivity decreases significantly with increasing Cu content at elevated temperatures due to the crystal structure of this material system. A maximum ZT value of 0.86 was obtained at 800 K for the specimen with the highest Cu content, Cu2.2Zn0.8SnSe4. ((c) 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim) C1 [Dong, Yongkwan; Nolas, George S.] Univ S Florida, Dept Phys, Tampa, FL 33620 USA. [Wang, Hsin] Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN 37831 USA. RP Nolas, GS (reprint author), Univ S Florida, Dept Phys, Tampa, FL 33620 USA. EM gnolas@usf.edu RI Wang, Hsin/A-1942-2013 OI Wang, Hsin/0000-0003-2426-9867 FU National Science Foundation [1048796]; Department of Energy [1048796]; UT-Battelle LLC [DE-AC05000OR22725] FX Y.D. and G.S.N. gratefully acknowledge financial support from the National Science Foundation and Department of Energy Partnership on Thermoelectric Devices for Vehicle Applications (Grant No. 1048796). H.W. would like to thank the support of the assistant secretary for Energy Efficiency and Renewable Energy of the Department of Energy and the Propulsion Materials program under the Vehicle Technologies program. Oak Ridge National Laboratory is managed by UT-Battelle LLC under contract DE-AC05000OR22725. NR 22 TC 18 Z9 18 U1 5 U2 42 PU WILEY-V C H VERLAG GMBH PI WEINHEIM PA BOSCHSTRASSE 12, D-69469 WEINHEIM, GERMANY SN 1862-6254 EI 1862-6270 J9 PHYS STATUS SOLIDI-R JI Phys. Status Solidi-Rapid Res. Lett. PD JAN PY 2014 VL 8 IS 1 BP 61 EP 64 DI 10.1002/pssr.201308274 PG 4 WC Materials Science, Multidisciplinary; Physics, Applied; Physics, Condensed Matter SC Materials Science; Physics GA AA4SO UT WOS:000331086600010 ER PT J AU Kim, YS Welch, CF Mack, NH Hjelm, RP Orler, EB Hawley, ME Lee, KS Yim, SD Johnston, CM AF Kim, Y. S. Welch, C. F. Mack, N. H. Hjelm, R. P. Orler, E. B. Hawley, M. E. Lee, K. S. Yim, S. -D. Johnston, C. M. TI Highly durable fuel cell electrodes based on ionomers dispersed in glycerol SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID CATALYSTS; DEGRADATION; DURABILITY; SCATTERING; INTERFACE; PEFCS; ELECTROCATALYSTS; ALLOY AB A major, unprecedented improvement in the durability of polymer electrolyte membrane fuel cells is obtained by tuning the properties of the interface between the catalyst and the ionomer by choosing the appropriate dispersing medium. While a fuel cell cathode prepared from aqueous dispersion showed 90 mV loss at 0.8 A cm(-2) after 30000 potential cycles (0.6-1.0 V), a fuel cell cathode prepared from glycerol dispersion exhibited only 20 mV loss after 70000 cycles. This minimum performance loss occurs even though there was an over 80% reduction of electrochemical surface area of the Pt catalyst. These findings indicate that a proper understanding and control of the catalyst-water-ionomer (three-phase) interfaces is even more important for maintaining fuel cell durability in typical electrodes than catalyst agglomeration, and this opens up a novel path for tailoring the functional properties of electrified interfaces. C1 [Kim, Y. S.; Lee, K. S.; Yim, S. -D.; Johnston, C. M.] Los Alamos Natl Lab, Sensors & Electrochem Devices Grp, Los Alamos, NM 87545 USA. [Welch, C. F.; Orler, E. B.; Hawley, M. E.] Los Alamos Natl Lab, Polymers & Coatings Grp, Los Alamos, NM 87545 USA. [Mack, N. H.] Los Alamos Natl Lab, Phys Chem & Appl Spect Grp, Los Alamos, NM 87545 USA. [Hjelm, R. P.] Los Alamos Natl Lab, Los Alamos Neutron Sci Ctr, Los Alamos, NM 87545 USA. RP Kim, YS (reprint author), Los Alamos Natl Lab, Sensors & Electrochem Devices Grp, POB 1663, Los Alamos, NM 87545 USA. EM yskim@lanl.gov; cjohnston2005@gmail.com OI Lee, Kwan Soo/0000-0002-5315-3487; Welch, Cynthia/0000-0002-4638-6434 FU Korea Institute of Energy Research; Los Alamos National Security LLC under DOE [DE-AC52-06NA25396]; U. S. Department of Energy Fuel Cell Technologies program FX We thank the U. S. Department of Energy Fuel Cell Technologies program for funding this work. We thank Jerzy Chilistunoff for the microelectrode experimental set-up. We thank Andrea Labouriau for NMR measurement. We thank Karen More (ORNL) for assisting in TEM measurements. K. S. Lee acknowledges the research grant from Gwangju Institute of Science and Technology. S.-D. Yim acknowledges the support from Korea Institute of Energy Research. Los Alamos National Laboratory is operated by Los Alamos National Security LLC under DOE Contract DE-AC52-06NA25396. NR 26 TC 12 Z9 12 U1 1 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 2014 VL 16 IS 13 BP 5927 EP 5932 DI 10.1039/c4cp00496e PG 6 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AC4EW UT WOS:000332474700005 PM 24569648 ER PT J AU Miliordos, E Xantheas, SS AF Miliordos, Evangelos Xantheas, Sotiris S. TI Elucidating the mechanism behind the stabilization of multi-charged metal cations in water: a case study of the electronic states of microhydrated Mg2+, Ca2+ and Al3+ SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID MOLECULAR-DYNAMICS SIMULATION; GAS-PHASE ION; DENSITY-FUNCTIONAL THEORY; X-RAY-DIFFRACTION; INFRARED RADIATIVE DISSOCIATION; COLLISION-INDUCED DISSOCIATION; HYDRATED CALCIUM-ION; GAUSSIAN-BASIS SETS; AB-INITIO; ALKALINE-EARTH AB Metal atoms typically have second and higher ionization potentials (IPs) that are larger than the IP of water, resulting in the Coulombic explosion of the first few [M(H2O)(n)](+q) (q >= 2) gas phase clusters as the M+(q-1) + (H2O)(n) + or MOH+(q-1) + H3O+(H2O)(n-2) energy levels are energetically more stable than the Mq+ + (H2O)(n) ones for small n. We present a theoretical analysis of the various electronic states arising from the sequential hydration of the Ca2+, Mg2+ and Al3+ cations with up to six water molecules. Our results quantify the relative shift of those electronic states with the degree of solvation, identify their complex interaction with other states arising from different dissociation channels and shed light on the mechanism behind the energetic stabilization of the multi-charged hydrated M+q(H2O) n complexes observed in aqueous solution with respect to the water ionization products. C1 [Miliordos, Evangelos; Xantheas, Sotiris S.] Pacific NW Natl Lab, Div Phys Sci, Richland, WA 99352 USA. RP Xantheas, SS (reprint author), Pacific NW Natl Lab, Div Phys Sci, 902 Battelle Blvd,POB 999,MS K1-83, Richland, WA 99352 USA. EM sotiris.xantheas@pnnl.gov RI Xantheas, Sotiris/L-1239-2015 FU US Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences; Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231] FX This work was supported by the US Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences. Pacific Northwest National Laboratory (PNNL) is a multiprogram national laboratory operated for DOE by Battelle. 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 85 TC 5 Z9 5 U1 2 U2 31 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 2014 VL 16 IS 15 BP 6886 EP 6892 DI 10.1039/c3cp53636j PG 7 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AD3EO UT WOS:000333121300006 PM 24131940 ER PT J AU Gowda, SR Gallagher, KG Croy, JR Bettge, M Thackeray, MM Balasubramanian, M AF Gowda, Sanketh R. Gallagher, Kevin G. Croy, Jason R. Bettge, Martin Thackeray, Michael M. Balasubramanian, Mahalingam TI Oxidation state of cross-over manganese species on the graphite electrode of lithium-ion cells SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID SPINEL CELLS; BATTERIES; CAPACITY; DISSOLUTION; INTERPHASE; ELECTROCHEMISTRY; DEGRADATION; DEPOSITION; INSERTION; CATHODE AB It is well known that Li-ion cells containing manganese oxide-based positive electrodes and graphite-based negative electrodes suffer accelerated capacity fade, which has been attributed to the deposition of dissolved manganese on the graphite electrodes during electrochemical cell cycling. However, the reasons for the accelerated capacity fade are still unclear. This stems, in part, from conflicting reports of the oxidation state of the manganese species in the negative electrode. In this communication, the oxidation state of manganese deposited on graphite electrodes has been probed by X-ray absorption near edge spectroscopy (XANES). The XANES features confirm, unequivocally, the presence of fully reduced manganese (Mn-0) on the surface of graphite particles. The deposition of Mn-0 on the graphite negative electrode acts as a starting point to understand the consequent electrochemical behavior of these electrodes; possible reasons for the degradation of cell performance are proposed and discussed. C1 [Gowda, Sanketh R.; Gallagher, Kevin G.; Croy, Jason R.; Bettge, Martin; Thackeray, Michael M.] Argonne Natl Lab, Chem Sci & Engn Div, Electrochem Energy Storage Dept, Argonne, IL 60439 USA. [Balasubramanian, Mahalingam] Argonne Natl Lab, Adv Photon Source, Xray Sci Div, Argonne, IL 60439 USA. RP Gallagher, KG (reprint author), Argonne Natl Lab, Chem Sci & Engn Div, Electrochem Energy Storage Dept, 9700 S Cass Ave, Argonne, IL 60439 USA. EM kevin.gallagher@anl.gov; mali@aps.anl.gov FU Center for Electrical Energy Storage (CEES), an Energy Frontier Research Center; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences (U.S. DOE-BES); Argonne National Laboratory; U.S. DOE-BES [DE-AC02-06CH11357] FX This project was supported by the Center for Electrical Energy Storage (CEES), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences (U.S. DOE-BES). S. R. G. was supported by a Director's Postdoctoral Fellowship at Argonne National Laboratory. Use of sector 20 facilities at the Advanced Photon Source (APS) and microscopy facilities at the Center for Nanoscale Materials (CNM) at Argonne, supported by U.S. DOE-BES under Contract No. DE-AC02-06CH11357, is acknowledged. Electrodes for cell fabrication were obtained from Argonne's Cell Analysis, Modeling and Prototyping Facility (CAMP). Yuzi Liu is acknowledged for help with the TEM studies. NR 27 TC 16 Z9 16 U1 4 U2 37 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 2014 VL 16 IS 15 BP 6898 EP 6902 DI 10.1039/c4cp00764f PG 5 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AD3EO UT WOS:000333121300008 PM 24608259 ER PT J AU Nanba, Y Asakura, D Okubo, M Zhou, HS Amemiya, K Okada, K Glans, PA Jenkins, CA Arenholz, E Guo, JH AF Nanba, Yusuke Asakura, Daisuke Okubo, Masashi Zhou, Haoshen Amemiya, Kenta Okada, Kozo Glans, Per-Anders Jenkins, Catherine A. Arenholz, Elke Guo, Jinghua TI Anisotropic charge-transfer effects in the asymmetric Fe(CN)(5)NO octahedron of sodium nitroprusside: a soft X-ray absorption spectroscopy study SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID TRANSITION-METAL COMPOUNDS; METASTABLE STATES; POLARIZATION DEPENDENCE; OPTICAL SPECTROSCOPY; EMISSION SPECTRA; SINGLE-CRYSTALS; CENTER-DOT; COMPLEXES; FE; SCATTERING AB The electronic structure of Na-2[ Fe(CN)(5)NO]center dot 2H(2)O (sodium nitroprusside: SNP) was investigated by using soft X-ray absorption (XA) spectroscopy. The Fe L-2,L-3-edge XA spectrum of SNP exhibited distinct and very large satellite peaks for L-3 and L-2 regions, which is different from the spectra of hexacyanoferrates and the other iron compounds. A configuration-interaction full-multiplet calculation, in which the ligand molecular orbitals for the C-4v symmetry were taken into account, revealed the Fe2+ low-spin state with very strong effects of metal-to-ligand charge-transfer from the Fe 3d to NO 2p orbitals. C1 [Nanba, Yusuke; Asakura, Daisuke; Okubo, Masashi; Zhou, Haoshen] Natl Inst Adv Ind Sci & Technol, Energy Technol Res Inst, Tsukuba, Ibaraki 3058568, Japan. [Amemiya, Kenta] High Energy Accelerator Res Org, IMSS, Photon Factory, Tsukuba, Ibaraki 3050801, Japan. [Okada, Kozo] Okayama Univ, Grad Sch Nat Sci & Technol, Okayama 7008530, Japan. [Glans, Per-Anders; Jenkins, Catherine A.; Arenholz, Elke; Guo, Jinghua] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. RP Asakura, D (reprint author), Natl Inst Adv Ind Sci & Technol, Energy Technol Res Inst, Tsukuba, Ibaraki 3058568, Japan. EM daisuke-asakura@aist.go.jp RI OKADA, Kozo/B-1464-2011; Glans, Per-Anders/G-8674-2016; Okubo, Masashi/C-6360-2011; Jenkins, Catherine/A-7740-2012 FU Office of Science, Office of Basic Energy Science, of the U.S. Department of Energy [DE-AC02-05CH11231] FX This work was carried out under the approvals of the Photon Factory Program Advisory Committee (Proposal No. 2010G038 and 2012G107) and of the Advanced Light Source (Proposal No. 04907R). This work was also conducted based on the Japan-U.S. cooperation project for research and standardization of Clean Energy Technologies. The Advanced Light Source is supported by the Director, Office of Science, Office of Basic Energy Science, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. NR 36 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 2014 VL 16 IS 15 BP 7031 EP 7036 DI 10.1039/c3cp55471f PG 6 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AD3EO UT WOS:000333121300026 PM 24603987 ER PT J AU Hirsch, CN Foerster, JM Johnson, JM Sekhon, RS Muttoni, G Vaillancourt, B Penagaricano, F Lindquist, E Pedraza, MA Barry, K de Leon, N Kaeppler, SM Buell, CR AF Hirsch, Candice N. Foerster, Jillian M. Johnson, James M. Sekhon, Rajandeep S. Muttoni, German Vaillancourt, Brieanne Penagaricano, Francisco Lindquist, Erika Pedraza, Mary Ann Barry, Kerrie de Leon, Natalia Kaeppler, Shawn M. Buell, C. Robin TI Insights into the Maize Pan-Genome and Pan-Transcriptome SO PLANT CELL LA English DT Article ID ARABIDOPSIS-THALIANA; WIDE ASSOCIATION; FLOWERING-TIME; RNA-SEQ; GENETIC ARCHITECTURE; EUKARYOTIC GENOMES; MASS SELECTION; INBRED LINES; RICE GENOME; F-1 HYBRID AB Genomes at the species level are dynamic, with genes present in every individual (core) and genes in a subset of individuals (dispensable) that collectively constitute the pan-genome. Using transcriptome sequencing of seedling RNA from 503 maize (Zea mays) inbred lines to characterize the maize pan-genome, we identified 8681 representative transcript assemblies (RTAs) with 16.4% expressed in all lines and 82.7% expressed in subsets of the lines. Interestingly, with linkage disequilibrium mapping, 76.7% of the RTAs with at least one single nucleotide polymorphism (SNP) could be mapped to a single genetic position, distributed primarily throughout the nonpericentromeric portion of the genome. Stepwise iterative clustering of RTAs suggests, within the context of the genotypes used in this study, that the maize genome is restricted and further sampling of seedling RNA within this germplasm base will result in minimal discovery. Genome-wide association studies based on SNPs and transcript abundance in the pan-genome revealed loci associated with the timing of the juvenile-to-adult vegetative and vegetative-to-reproductive developmental transitions, two traits important for fitness and adaptation. This study revealed the dynamic nature of the maize pan-genome and demonstrated that a substantial portion of variation may lie outside the single reference genome for a species. C1 [Hirsch, Candice N.; Vaillancourt, Brieanne; Buell, C. Robin] Michigan State Univ, Dept Plant Biol, E Lansing, MI 48824 USA. [Hirsch, Candice N.; Vaillancourt, Brieanne; Buell, C. Robin] Michigan State Univ, Dept Energy, Great Lakes Bioenergy Res Ctr, E Lansing, MI 48824 USA. [Foerster, Jillian M.; Johnson, James M.; Sekhon, Rajandeep S.; Muttoni, German; de Leon, Natalia; Kaeppler, Shawn M.] Univ Wisconsin, Dept Agron, Madison, WI 53706 USA. [Sekhon, Rajandeep S.; de Leon, Natalia; Kaeppler, Shawn M.] Univ Wisconsin, Dept Energy, Great Lakes Bioenergy Res Ctr, Madison, WI 53706 USA. [Penagaricano, Francisco] Univ Wisconsin, Dept Anim Sci, Madison, WI 53706 USA. [Lindquist, Erika; Pedraza, Mary Ann; Barry, Kerrie] Joint Genome Inst, Dept Energy, Walnut Creek, CA 94598 USA. RP Buell, CR (reprint author), Michigan State Univ, Dept Plant Biol, E Lansing, MI 48824 USA. EM buell@msu.edu RI Penagaricano, Francisco/C-8083-2015; OI Penagaricano, Francisco/0000-0001-6661-3991; Kaeppler, Shawn/0000-0002-5964-1668 FU Department of Energy Great Lakes Bioenergy Research Center (DOE BER Office of Science) [DE-FC02-07ER64494]; Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231] FX This work was funded by the Department of Energy Great Lakes Bioenergy Research Center (DOE BER Office of Science DE-FC02-07ER64494). 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 DE-AC02-05CH11231. NR 84 TC 58 Z9 60 U1 9 U2 53 PU AMER SOC PLANT BIOLOGISTS PI ROCKVILLE PA 15501 MONONA DRIVE, ROCKVILLE, MD 20855 USA SN 1040-4651 EI 1532-298X J9 PLANT CELL JI Plant Cell PD JAN PY 2014 VL 26 IS 1 BP 121 EP 135 DI 10.1105/tpc.113.119982 PG 15 WC Biochemistry & Molecular Biology; Plant Sciences; Cell Biology SC Biochemistry & Molecular Biology; Plant Sciences; Cell Biology GA AC0ZE UT WOS:000332223200012 PM 24488960 ER PT J AU Leverenz, RL Jallet, D Li, MD Mathies, RA Kirilovsky, D Kerfeld, CA AF Leverenz, Ryan L. Jallet, Denis Li, Ming-De Mathies, Richard A. Kirilovsky, Diana Kerfeld, Cheryl A. TI Structural and Functional Modularity of the Orange Carotenoid Protein: Distinct Roles for the N- and C-Terminal Domains in Cyanobacterial Photoprotection SO PLANT CELL LA English DT Article ID SYNECHOCYSTIS PCC 6803; PHOTOACTIVE YELLOW PROTEIN; EXCITED-STATE PROPERTIES; CRYSTAL-STRUCTURE; SPECTROSCOPIC PROPERTIES; ARTHROSPIRA-MAXIMA; CIRCULAR-DICHROISM; BETA-CAROTENE; ACTIVE-SITE; LIGHT AB The orange carotenoid protein (OCP) serves as a sensor of light intensity and an effector of phycobilisome (PB)-associated photoprotection in cyanobacteria. Structurally, the OCP is composed of two distinct domains spanned by a single carotenoid chromophore. Functionally, in response to high light, the OCP converts from a dark-stable orange form, OCPO, to an active red form, OCPR. The C-terminal domain of the OCP has been implicated in the dynamic response to light intensity and plays a role in switching off the OCP's photoprotective response through its interaction with the fluorescence recovery protein. The function of the N-terminal domain, which is uniquely found in cyanobacteria, is unclear. To investigate its function, we isolated the N-terminal domain in vitro using limited proteolysis of native OCP. The N-terminal domain retains the carotenoid chromophore; this red carotenoid protein (RCP) has constitutive PB fluorescence quenching activity comparable in magnitude to that of active, full-length OCPR. A comparison of the spectroscopic properties of the RCP with OCPR indicates that critical proteinchromophore interactions within the C-terminal domain are weakened in the OCPR form. These results suggest that the C-terminal domain dynamically regulates the photoprotective activity of an otherwise constitutively active carotenoid binding N-terminal domain. C1 [Jallet, Denis; Kirilovsky, Diana] CEA, Inst Biol & Technol Saclay, F-91191 Gif Sur Yvette, France. [Jallet, Denis; Kirilovsky, Diana] CNRS, Unite Mixte Rech 8221, F-91191 Gif Sur Yvette, France. [Li, Ming-De; Mathies, Richard A.] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Kerfeld, Cheryl A.] US Dept Energy Joint Genome Inst, Walnut Creek, CA 94598 USA. [Kerfeld, Cheryl A.] Univ Calif Berkeley, Berkeley Synthet Biol Inst, Berkeley, CA 94720 USA. [Leverenz, Ryan L.; Kerfeld, Cheryl A.] Univ Calif Berkeley, Dept Plant & Microbial Biol, Berkeley, CA 94720 USA. RP Kerfeld, CA (reprint author), Michigan State Univ, MSU Dept Energy, Plant Res Lab, E Lansing, MI 48824 USA. EM ckerfeld@lbl.gov FU National Science Foundation [MCB 0851094, MCB1160614]; Agence Nationale de la Recherche (Project CYANOPROTECT); Centre National de la Recherche Scientifique; Commissariat a l'Energie Atomique; HARVEST EU FP7 Marie Curie Research Training Network; University Paris XI; Mathies Royalty Fund FX C.A.K. and R.L.L. acknowledge the support of the National Science Foundation (MCB 0851094 and MCB1160614). The research of D.K. and D.J. was supported by grants from the Agence Nationale de la Recherche (Project CYANOPROTECT), the Centre National de la Recherche Scientifique, the Commissariat a l'Energie Atomique, and HARVEST EU FP7 Marie Curie Research Training Network. D.J. has a fellowship of the University Paris XI. R.L.L., M.-D.L., and R.A.M. acknowledge financial support from the Mathies Royalty Fund. NR 34 TC 30 Z9 31 U1 3 U2 29 PU AMER SOC PLANT BIOLOGISTS PI ROCKVILLE PA 15501 MONONA DRIVE, ROCKVILLE, MD 20855 USA SN 1040-4651 EI 1532-298X J9 PLANT CELL JI Plant Cell PD JAN PY 2014 VL 26 IS 1 BP 426 EP 437 DI 10.1105/tpc.113.118588 PG 12 WC Biochemistry & Molecular Biology; Plant Sciences; Cell Biology SC Biochemistry & Molecular Biology; Plant Sciences; Cell Biology GA AC0ZE UT WOS:000332223200031 PM 24399299 ER PT J AU He, HK Adzima, B Zhong, MJ Averick, S Koepsel, R Murata, H Russell, A Luebke, D Takahara, A Nulwala, H Matyjaszewski, K AF He, Hongkun Adzima, Brian Zhong, Mingjiang Averick, Saadyah Koepsel, Richard Murata, Hironobu Russell, Alan Luebke, David Takahara, Atsushi Nulwala, Hunaid Matyjaszewski, Krzysztof TI Multifunctional photo-crosslinked polymeric ionic hydrogel films SO POLYMER CHEMISTRY LA English DT Article ID POLY(ETHYLENE GLYCOL DIACRYLATE); TRANSFER RADICAL POLYMERIZATION; POLYURETHANE ACRYLATE NETWORKS; IONOMER MEMBRANES; MECHANICAL-PROPERTIES; BLOCK-COPOLYMERS; FUEL-CELLS; ANTIBACTERIAL ACTIVITY; BIOCIDAL ACTIVITY; MOLECULAR-WEIGHT AB A facile approach was developed to prepare crosslinked ionic polymer hydrogel films by photo-crosslinking utilizing p-vinylbenzyl trimethylammonium chloride (VBTMACl) or p-vinylbenzyl trimethylammonium hydroxide (VBTMAOH) as the monomer and poly(ethylene oxide) dimethacrylate (PEODMA, M-n = 750) as the crosslinker. The films with different crosslinking degrees (20%, 40%, 60%, 80%, and 100%) were prepared and characterized by swelling measurements, scanning electron microscopy (SEM), UV-visible spectroscopy, attenuated total reflection Fourier transform infrared (ATR-FTIR) spectroscopy, dynamic mechanical analysis (DMA), thermogravimetric analysis (TGA), and small-angle X-ray scattering (SAXS). It was found that the mechanical and thermal properties of the films were largely influenced by the contents of the crosslinker in the films. By ion-exchange of the anions in the films with various other anions, the hydrophobicity/hydrophilicity of the films was changed. In addition, fluorescent films were prepared by treatment with fluorescein, and paramagnetic films with FeCl4- as a counter anion showed catalytic activity for Friedel-Crafts alkylation. The ionic films with quaternary ammonium chloride groups displayed antimicrobial activity against Escherichia coli (E. coli) with almost 100% killing efficiency. Multifunctional films with various tunable properties have significant potential for a wide range of applications. C1 [He, Hongkun; Zhong, Mingjiang; Averick, Saadyah; Nulwala, Hunaid; Matyjaszewski, Krzysztof] Carnegie Mellon Univ, Dept Chem, Ctr Macromol Engn, Pittsburgh, PA 15213 USA. [He, Hongkun; Adzima, Brian; Luebke, David; Nulwala, Hunaid; Matyjaszewski, Krzysztof] Natl Energy Technol Lab, Pittsburgh, PA 15236 USA. [Koepsel, Richard; Murata, Hironobu; Russell, Alan] Carnegie Mellon Univ, Inst Complex Engineered Syst, Pittsburgh, PA 15213 USA. [Takahara, Atsushi] Kyushu Univ, Inst Mat Chem & Engn, Fukuoka 8190395, Japan. RP Nulwala, H (reprint author), Carnegie Mellon Univ, Dept Chem, Ctr Macromol Engn, 4400 5th Ave, Pittsburgh, PA 15213 USA. EM hnulwala@andrew.cmu.edu; km3b@andrew.cmu.edu RI Nulwala, Hunaid/G-8126-2012; He, Hongkun/B-4759-2011; U-ID, Kyushu/C-5291-2016; Zhong, Mingjiang/F-3470-2011; Matyjaszewski, Krzysztof/A-2508-2008; Averick, Saadyah/A-9999-2015; OI Nulwala, Hunaid/0000-0001-7481-3723; He, Hongkun/0000-0002-7214-3313; Zhong, Mingjiang/0000-0001-7533-4708; Matyjaszewski, Krzysztof/0000-0003-1960-3402; Russell, Alan/0000-0001-5101-4371; Koepsel, Richard/0000-0002-6780-4914 FU NSF [CHE-1039870, DMR-0969301]; DoE [ER-45998]; U.S. Department of Energy's National Energy Technology Laboratory [DE-FE0004000] FX We acknowledged NSF support (CHE-1039870 and DMR-0969301) and DoE support (ER-45998) is acknowledged. This technical effort was also performed in support of U.S. Department of Energy's National Energy Technology Laboratory's ongoing research on CO2 capture under the contract DE-FE0004000. We would like to gratefully thank Dr Noboru Ohta (JASRI/SPring-8) for his helpful assistance in the SAXS measurements. NR 99 TC 8 Z9 8 U1 7 U2 90 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 2014 VL 5 IS 8 BP 2824 EP 2835 DI 10.1039/c3py01708g PG 12 WC Polymer Science SC Polymer Science GA AD3FB UT WOS:000333122600020 ER PT S AU Chang, C Xu, W Chen-Wiegart, YCK Wang, J Yu, DT AF Chang, Cheng Xu, Wei Chen-Wiegart, Yu-chen Karen Wang, Jun Yu, Dantong BE Wong, PC Kao, DL Hao, MC Chen, C TI Improving Chemical Mapping Algorithm and Visualization in Full-field Hard X-ray Spectroscopic Imaging SO VISUALIZATION AND DATA ANALYSIS 2014 SE Proceedings of SPIE LA English DT Proceedings Paper CT IS and T/SPIE 21st Annual Conference on Visualization and Analysis (VDA) CY FEB 03-05, 2014 CL San Francisco, CA SP Soc Imaging Sci & Technol, SPIE, Kitware Inc DE XANES; Spectroscopy; Chemical mapping; Spectra fitting; Parallel computing; Visualization AB X-ray Absorption Near Edge Structure (XANES) imaging, an advanced absorption spectroscopy technique, at the Transmission X-ray Microscopy (TXM) Beamline X8C of NSLS enables high-resolution chemical mapping (a.k.a. chemical composition identification or chemical spectra fitting). Two-Dimensional (2D) chemical mapping has been successfully applied to study many functional materials to decide the percentages of chemical components at each pixel position of the material images. In chemical mapping, the attenuation coefficient spectrum of the material (sample) can be fitted with the weighted sum of standard spectra of individual chemical compositions, where the weights are the percentages to be calculated. In this paper, we first implemented and compared two fitting approaches: (i) a brute force enumeration method, and (ii) a constrained least square minimization algorithm proposed by us. Next, as 2D spectra fitting can be conducted pixel by pixel, so theoretically, both methods can be implemented in parallel. In order to demonstrate the feasibility of parallel computing in the chemical mapping problem and investigate how much efficiency improvement can be achieved, we used the second approach as an example and implemented a parallel version for a multi-core computer cluster. Finally we used a novel way to visualize the calculated chemical compositions, by which domain scientists could grasp the percentage difference easily without looking into the real data. C1 [Chang, Cheng; Xu, Wei; Yu, Dantong] Brookhaven Natl Lab, Computat Sci Ctr, Upton, NY 11973 USA. [Chen-Wiegart, Yu-chen Karen; Wang, Jun] Brookhaven Natl Lab, Photon Sci Directorate, Upton, NY 11973 USA. RP Chang, C (reprint author), Brookhaven Natl Lab, Computat Sci Ctr, Upton, NY 11973 USA. EM cchang@bnl.gov; xuw@bnl.gov; ycchen@bnl.gov; junwang@bnl.gov; dtyu@bnl.gov NR 7 TC 0 Z9 0 U1 1 U2 5 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9934-9 J9 PROC SPIE PY 2014 VL 9017 AR UNSP 90170S DI 10.1117/12.2041109 PG 8 WC Engineering, Electrical & Electronic; Optics SC Engineering; Optics GA BA1SU UT WOS:000333055000026 ER PT S AU Harvey, N Porter, R AF Harvey, Neal Porter, Reid BE Wong, PC Kao, DL Hao, MC Chen, C TI User-Driven Sampling Strategies in Image Exploitation SO VISUALIZATION AND DATA ANALYSIS 2014 SE Proceedings of SPIE LA English DT Proceedings Paper CT IS and T/SPIE 21st Annual Conference on Visualization and Analysis (VDA) CY FEB 03-05, 2014 CL San Francisco, CA SP Soc Imaging Sci & Technol, SPIE, Kitware Inc DE visual analytics; interactive machine learning; active learning; relevance feedback AB Visual analytics and interactive machine learning both try to leverage the complementary strengths of humans and machines to solve complex data exploitation tasks. These fields overlap most significantly when training is involved: the visualization or machine learning tool improves over time by exploiting observations of the human-computer interaction. This paper focuses on one aspect of the human-computer interaction that we call user-driven sampling strategies Unlike relevance feedback and active learning sampling strategies, where the computer selects which data to label at each iteration, we investigate situations where the user selects which data is to be labeled at each iteration. User-driven sampling strategies can emerge in many visual analytics applications but they have not been fully developed in machine learning. User-driven sampling strategies suggest new theoretical and practical research questions for both visualization science and machine learning. In this paper we identify and quantify the potential benefits of these strategies in a practical image analysis application. We find user-driven sampling strategies can sometimes provide significant performance gains by steering tools towards local minima that have lower error than tools trained with all of the data. In preliminary experiments we find these performance gains are particularly pronounced when the user is experienced with the tool and application domain C1 [Harvey, Neal; Porter, Reid] Los Alamos Natl Lab, Intelligence & Space Res Div, Los Alamos, NM 87545 USA. RP Harvey, N (reprint author), Los Alamos Natl Lab, Intelligence & Space Res Div, POB 1663, Los Alamos, NM 87545 USA. EM harve@lanl.gov; rporter@lanl.gov NR 16 TC 0 Z9 0 U1 0 U2 0 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9934-9 J9 PROC SPIE PY 2014 VL 9017 AR 90170B DI 10.1117/12.2038581 PG 8 WC Engineering, Electrical & Electronic; Optics SC Engineering; Optics GA BA1SU UT WOS:000333055000010 ER PT J AU Renslow, RS Babauta, JT Majors, PD Mehta, HS Ewing, RJ Ewing, TW Mueller, KT Beyenal, H AF Renslow, R. S. Babauta, J. T. Majors, P. D. Mehta, H. S. Ewing, R. J. Ewing, T. W. Mueller, K. T. Beyenal, H. TI A biofilm microreactor system for simultaneous electrochemical and nuclear magnetic resonance techniques SO WATER SCIENCE AND TECHNOLOGY LA English DT Article DE biofilm; electrochemistry; Geobacter; magnetic resonance; NMR; reactor ID MICROBIAL FUEL-CELL; GEOBACTER-SULFURREDUCENS BIOFILMS; ONEIDENSIS MR-1 BIOFILMS; REMOTE POWER-GENERATION; WASTE-WATER TREATMENT; DESALINATION CELL; ELECTRON-TRANSFER; IMAGING MRI; NMR; ELECTRICITY AB Nuclear magnetic resonance (NMR) techniques are ideally suited for the study of biofilms and for probing their microenvironments because these techniques allow for noninvasive interrogation and in situ monitoring with high resolution. By combining NMR with simultaneous electrochemical techniques, it is possible to sustain and study live biofilms respiring on electrodes. Here, we describe a biofilm microreactor system, including a reusable and a disposable reactor, that allows for simultaneous electrochemical and NMR techniques (EC-NMR) at the microscale. Microreactors were designed with custom radio frequency resonator coils, which allowed for NMR measurements of biofilms growing on polarized gold electrodes. For an example application of this system we grew Geobacter sulfurreducens biofilms on electrodes. EC-NMR was used to investigate growth medium flow velocities and depth-resolved acetate concentration inside the biofilm. As a novel contribution we used Monte Carlo error analysis to estimate the standard deviations of the acetate concentration measurements. Overall, we found that the disposable EC-NMR microreactor provided a 9.7 times better signal-to-noise ratio over the reusable reactor. The EC-NMR biofilm microreactor system can ultimately be used to correlate extracellular electron transfer rates with metabolic reactions and explore extracellular electron transfer mechanisms. C1 [Renslow, R. S.; Mehta, H. S.; Ewing, R. J.; Mueller, K. T.] Pacific NW Natl Lab, Environm Mol Sci Lab, Richland, WA 99352 USA. [Babauta, J. T.; Ewing, R. J.; Beyenal, H.] Washington State Univ, Gene & Linda Voiland Sch Chem Engn & Bioengn & Bi, Pullman, WA 99164 USA. [Majors, P. D.] Bruker BioSpin Corp, Billerica, MA 01821 USA. [Mueller, K. T.] Penn State Univ, Dept Chem, University Pk, PA 16802 USA. RP Renslow, RS (reprint author), Pacific NW Natl Lab, Environm Mol Sci Lab, Richland, WA 99352 USA. EM ryan.renslow@pnnl.gov RI Mueller, Karl/A-3637-2010 FU United States Office of Naval Research (ONR) [N00014-09-1-0090]; National Institutes of Health (NIDCR) [R21 DE017232]; Department of Energy's Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory; NSF-CAREER award [0954186]; NIH Protein Biotechnology Training Grant [T32-GM008336]; Linus Pauling Distinguished Postdoctoral Fellowship at Pacific Northwest National Laboratory FX This research was financially supported by the United States Office of Naval Research (ONR) (Grant no. N00014-09-1-0090). The custom-built EC-NMR biofilm microreactor hardware development was supported by the National Institutes of Health (NIDCR) (Grant no. R21 DE017232). All NMR experiments were performed at the Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility sponsored by the Department of Energy's Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory. T. Ewing was supported by NSF-CAREER award #0954186. NIH Protein Biotechnology Training Grant T32-GM008336 helped fund R. Renslow and J. Babauta during this project. R. Renslow was also supported by a Linus Pauling Distinguished Postdoctoral Fellowship at Pacific Northwest National Laboratory. We thank M. Townsend and R. May for building the reusable microreactors. NR 47 TC 3 Z9 3 U1 3 U2 29 PU IWA PUBLISHING PI LONDON PA ALLIANCE HOUSE, 12 CAXTON ST, LONDON SW1H0QS, ENGLAND SN 0273-1223 EI 1996-9732 J9 WATER SCI TECHNOL JI Water Sci. Technol. PY 2014 VL 69 IS 5 BP 966 EP 973 DI 10.2166/wst.2013.802 PG 8 WC Engineering, Environmental; Environmental Sciences; Water Resources SC Engineering; Environmental Sciences & Ecology; Water Resources GA AD0RC UT WOS:000332940800009 PM 24622544 ER PT J AU Crumeyrolle, S Chen, G Ziemba, L Beyersdorf, A Thornhill, L Winstead, E Moore, RH Shook, MA Hudgins, C Anderson, BE AF Crumeyrolle, S. Chen, G. Ziemba, L. Beyersdorf, A. Thornhill, L. Winstead, E. Moore, R. H. Shook, M. A. Hudgins, C. Anderson, B. E. TI Factors that influence surface PM2.5 values inferred from satellite observations: perspective gained for the US Baltimore-Washington metropolitan area during DISCOVER-AQ SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID AEROSOL OPTICAL DEPTH; PARTICULATE MATTER; LIGHT-SCATTERING; AIR-QUALITY; RELATIVE-HUMIDITY; UNITED-STATES; IN-SITU; RADIATIVE PROPERTIES; RESEARCH AIRCRAFT; ACE 1 AB During the NASA DISCOVER-AQ campaign over the US Baltimore, MD-Washington, D. C., metropolitan area in July 2011, the NASA P-3B aircraft performed extensive profiling of aerosol optical, chemical, and microphysical properties. These in situ profiles were coincident with ground-based remote sensing (AERONET) and in situ (PM2.5) measurements. Here, we use this data set to study the correlation between the PM2.5 observations at the surface and the column integrated measurements. Aerosol optical depth (AOD(550) (nm)) calculated with the extinction (550 nm) measured during the in situ profiles was found to be strongly correlated with the volume of aerosols present in the boundary layer (BL). Despite the strong correlation, some variability remains, and we find that the presence of aerosol layers above the BL (in the buffer layer - BuL) introduces significant uncertainties in PM2.5 estimates based on column-integrated measurements (overestimation of PM2.5 by a factor of 5). This suggests that the use of active remote sensing techniques would dramatically improve air quality retrievals. Indeed, the relationship between the AOD(550 nm) and the PM2.5 is strongly improved by accounting for the aerosol present in and above the BL (i.e., integrating the aerosol loading from the surface to the top of the BuL). Since more than 15% of the AOD values observed during DISCOVER-AQ are dominated by aerosol water uptake, the f(RH)(amb) (ratio of scattering coefficient at ambient relative humidity (RH) to scattering coefficient at low RH; see Sect. 3.2) is used to study the impact of the aerosol hygroscopicity on the PM2.5 retrievals. The results indicate that PM2.5 can be predicted within a factor up to 2 even when the vertical variability of the f(RH)(amb) is assumed to be negligible. Moreover, f(RH = 80 %) and RH measurements performed at the ground may be used to estimate the f(RH)(amb) during dry conditions (RHBL < 55 %). C1 [Crumeyrolle, S.; Moore, R. H.] Oak Ridge Associated Univ, NASA, Postdoctoral program, Oak Ridge, TN 37831 USA. [Crumeyrolle, S.; Chen, G.; Ziemba, L.; Beyersdorf, A.; Thornhill, L.; Winstead, E.; Moore, R. H.; Shook, M. A.; Hudgins, C.; Anderson, B. E.] NASA, Langley Res Ctr, Hampton, VA 23681 USA. [Crumeyrolle, S.] Univ Lille 1, CNRS, LOA, UMR8518, F-59655 Villeneuve Dascq, France. [Thornhill, L.; Winstead, E.; Shook, M. A.] Sci Syst & Applicat SSAI, Hampton, VA 23666 USA. RP Crumeyrolle, S (reprint author), Oak Ridge Associated Univ, NASA, Postdoctoral program, Oak Ridge, TN 37831 USA. EM suzanne.crumeyrolle@gmail.com FU NASA through the Earth System Science Pathfinder Program Office; ESSP Program Office; NASA Postdoctoral Program fellowship FX This research was funded by NASA's Earth Venture-1 Program through the Earth System Science Pathfinder Program Office. The authors wish to thank the ESSP Program Office for their support throughout the first DISCOVER-AQ deployment. We would also like to express our deep appreciation to Mary Kleb as well as the pilots and flight crews of NASA's P-3B and UC-12 for their important contributions. We thank B. Holben (NASA-GSFC) for providing the Sun photometer within the framework of the AERONET program. Finally, we would like to thank the Maryland Department of Environment and EPA for making the PM2.5 and the ozone measurements available and sharing their data with DISCOVER-AQ. Suzanne Crumeyrolle and Richard H. Moore have been supported by the NASA Postdoctoral Program fellowship. NR 68 TC 15 Z9 15 U1 5 U2 36 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 2014 VL 14 IS 4 BP 2139 EP 2153 DI 10.5194/acp-14-2139-2014 PG 15 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA AC2ZZ UT WOS:000332386100023 ER PT J AU Schmokel, MS Bjerg, L Cenedese, S Jorgensen, MRV Chen, YS Overgaard, J Iversen, BB AF Schmokel, Mette S. Bjerg, Lasse Cenedese, Simone Jorgensen, Mads R. V. Chen, Yu-Sheng Overgaard, Jacob Iversen, Bo B. TI Atomic properties and chemical bonding in the pyrite and marcasite polymorphs of FeS2: a combined experimental and theoretical electron density study SO CHEMICAL SCIENCE LA English DT Article ID X-RAY-DIFFRACTION; EXPERIMENTAL CHARGE-DENSITY; ARSENOPYRITE TYPE STRUCTURES; TRANSITION-METAL-COMPLEXES; DARWIN TRANSFER EQUATIONS; COPPENS MULTIPOLE MODEL; D-ORBITAL OCCUPANCIES; TOPOLOGICAL ANALYSIS; CRYSTAL-STRUCTURES; SHELL STRUCTURE AB The electron density distributions in both polymorphs of the promising photovoltaic material iron disulfide have been determined by multipole modelling against state-of-the-art synchrotron X-ray diffraction data collected at 10 K using minute single crystals with dimensions less than 10 mm. Charge density analysis of FeS2 pyrite and marcasite offers a unique opportunity to relate local atomic properties, such as 2-center chemical bonding, atomic charges and d-orbital populations, to polymorphism in extended crystal structures. In combination with results from periodic calculations on the compounds in the experimental geometries using WIEN2k, the study provides unambiguous answers to a number of unsolved issues regarding the nature of the bonding in FeS2. The Fe-S bonds exhibit all the virtues of polar covalent bonds, with only minor charge accumulation but significantly negative energy densities at the bond critical points. Compared to a non-interacting model, the density is found to be concentrated along the Fe-S interaction line in support of a partial covalent bonding description. The homopolar covalent S-S interaction is seemingly stronger in pyrite than in marcasite, determined not only from the shorter distance but also from all topological indicators. The study also clarifies that the atomic charges are significantly smaller than the estimation based on crystal-field theory of Fe2+, S-1. The experimentally derived Fe d-orbital populations are found to deviate from the commonly assumed full t(2g) set, empty e(g) set, and they fit exceptionally well with the theoretical individual atomic orbitals projected density of states showing a higher d(xy) participation in the valence band in marcasite compared with pyrite. Thus, the differences between the two polymorphic compounds are directly reflected in their valence density distributions and d-orbital populations. C1 [Schmokel, Mette S.; Bjerg, Lasse; Jorgensen, Mads R. V.; Overgaard, Jacob; Iversen, Bo B.] Aarhus Univ, Ctr Mat Crystallog, Dept Chem, DK-8000 Aarhus C, Denmark. [Schmokel, Mette S.; Bjerg, Lasse; Jorgensen, Mads R. V.; Overgaard, Jacob; Iversen, Bo B.] Aarhus Univ, iNANO, DK-8000 Aarhus C, Denmark. [Cenedese, Simone] Univ Toledo, Toledo, OH 43606 USA. [Chen, Yu-Sheng] Univ Chicago, ChemMatCARS, Adv Photon Source, Argonne, IL 60439 USA. [Cenedese, Simone] Univ Milan, CNR, ISTM, I-20133 Milan, Italy. [Cenedese, Simone] Univ Milan, Dipartimento Chim, I-20133 Milan, Italy. RP Overgaard, J (reprint author), Aarhus Univ, Ctr Mat Crystallog, Dept Chem, Langelandsgade 140, DK-8000 Aarhus C, Denmark. RI Jorgensen, Mads Ry Vogel/C-6109-2017 OI Jorgensen, Mads Ry Vogel/0000-0001-5507-9615 FU Danish National Research Foundation [DNRF93]; Danish Research Council for Nature and Universe (Danscatt); National Science Foundation/Department of Energy [NSF/CHE-0822838]; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357] FX This work was supported by the Danish National Research Foundation (DNRF93), and the Danish Research Council for Nature and Universe (Danscatt). ChemMatCARS Sector 15 is principally supported by the National Science Foundation/Department of Energy under Grant NSF/CHE-0822838. 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. NR 104 TC 11 Z9 11 U1 9 U2 58 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 2014 VL 5 IS 4 BP 1408 EP 1421 DI 10.1039/c3sc52977k PG 14 WC Chemistry, Multidisciplinary SC Chemistry GA AC4CE UT WOS:000332467400019 ER PT J AU Simon, JI Weis, D DePaolo, DJ Renne, PR Mundil, R Schmitt, AK AF Simon, Justin I. Weis, Dominique DePaolo, Donald J. Renne, Paul R. Mundil, Roland Schmitt, Axel K. TI Assimilation of preexisting Pleistocene intrusions at Long Valley by periodic magma recharge accelerates rhyolite generation: rethinking the remelting model SO CONTRIBUTIONS TO MINERALOGY AND PETROLOGY LA English DT Article DE Long Valley; Timescales; Silicic magma processes; Isotopes; Geochronology; Supervolcano ID FISH CANYON SANIDINE; U-PB AGES; K-40 DECAY CONSTANTS; BISHOP-TUFF; SILICIC MAGMA; RESIDENCE TIMES; GLASS MOUNTAIN; AR-40/AR-39 GEOCHRONOLOGY; MELT INCLUSIONS; VOLCANIC FIELD AB Rhyolite flows and tuffs from the Long Valley area of California, which were erupted over a two-million-year time period, exhibit systematic trends in Nd, Hf, and Pb isotopes, trace element composition, erupted volume, and inferred magma residence time that provide evidence for a new model for the production of large volumes of silica-rich magma. Key constraints come from geochronology of zircon crystal populations combined with a refined eruption chronology from Ar-Ar geochronology; together these data give better estimates of magma residence time that can be evaluated in the context of changing magma compositions. Here, we report Hf, Nd, and Sr isotopes, major and trace element compositions, Ar-40/Ar-39 ages, and U-Pb zircon ages that combined with existing data suggest that the chronology and geochemistry of Long Valley rhyolites can be explained by a dynamic interaction of crustal and mantle-derived magma. The large volume Bishop Tuff represents the culmination of a period of increased mantle-derived magma input to the Long Valley volcanic system; the effect of this input continued into earliest postcaldera time. As the postcaldera evolution of the system continued, new and less primitive crustal-derived magmas dominated the system. A mixture of varying amounts of more mafic mantle-derived and felsic crustal-derived magmas with recently crystallized granitic plutonic materials offers the best explanation for the observed chronology, secular shifts in Hf and Nd isotopes, and the apparently low zircon crystallization and saturation temperatures as compared to Fe-Ti oxide eruption temperatures. This scenario in which transient crustal magma bodies remained molten for varying time periods, fed eruptions before solidification, and were then remelted by fresh recharge provides a realistic conceptual framework that can explain the isotopic and geochemical evidence. General relationships between crustal residence times and magma sources are that: (1) precaldera rhyolites had long crustal magma residence times and high crustal affinity, (2) the caldera-related Bishop Tuff and early postcaldera rhyolites have lower crustal affinity and short magma residence times, and (3) later postcaldera rhyolites again have stronger crustal signatures and longer magma residence times. C1 [Simon, Justin I.] NASA, Lyndon B Johnson Space Ctr, Ctr Isotope Cosmochem & Geochronol, Houston, TX 77058 USA. [Weis, Dominique] Univ British Columbia, Pacific Ctr Isotope & Geochem Res, Dept Earth Ocean & Atmospher Sci, Vancouver, BC V5Z 1M9, Canada. [DePaolo, Donald J.] Univ Calif Berkeley, Ctr Isotope Geochem, Dept Earth & Planetary Sci, Berkeley, CA 94720 USA. [DePaolo, Donald J.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Renne, Paul R.; Mundil, Roland] Berkeley Geochronol Ctr, Berkeley, CA 94709 USA. [Renne, Paul R.] Univ Calif Berkeley, Dept Earth & Planetary Sci, Berkeley, CA 94720 USA. [Schmitt, Axel K.] Univ Calif Los Angeles, Dept Earth & Space Sci, Los Angeles, CA 90095 USA. RP Simon, JI (reprint author), NASA, Lyndon B Johnson Space Ctr, Ctr Isotope Cosmochem & Geochronol, Astromat Res Off KR111, Houston, TX 77058 USA. EM Justin.I.Simon@NASA.gov RI Weis, Dominique/Q-7658-2016; UCLA, SIMS/A-1459-2011; OI Weis, Dominique/0000-0002-6638-5543; Schmitt, Axel/0000-0002-9029-4211 FU Instrumentation and Facilities Program, Division of Earth Sciences, National Science Foundation FX We value the technical assistance of J. Barling, T. Becker, S. Brown, R. Friedman, B. Kieffer, and T. Owens. Informal reviews by R. Mills and M. Tappa are greatly appreciated. This contribution benefits from two anonymous reviewers and the efforts of AE T. Grove. The ion microprobe facility at UCLA is partly supported by a grant from the Instrumentation and Facilities Program, Division of Earth Sciences, National Science Foundation. NR 109 TC 14 Z9 14 U1 1 U2 30 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 0010-7999 EI 1432-0967 J9 CONTRIB MINERAL PETR JI Contrib. Mineral. Petrol. PD JAN PY 2014 VL 167 IS 1 AR 955 DI 10.1007/s00410-013-0955-5 PG 34 WC Geochemistry & Geophysics; Mineralogy SC Geochemistry & Geophysics; Mineralogy GA AC5TI UT WOS:000332583200004 ER PT J AU Prime, MB DeWald, AT Hill, MR Clausen, B Tran, M AF Prime, Michael B. DeWald, Adrian T. Hill, Michael R. Clausen, Bjorn Minh Tran TI Forensic determination of residual stresses and K-1 from fracture surface mismatch SO ENGINEERING FRACTURE MECHANICS LA English DT Article DE Fracture; Residual stress; Fractography; Failure analysis; Fracture surface mismatch; Conjugate surface; Crack closure; Aluminum ID NEUTRON-DIFFRACTION; ALLOY; WELD; REFINEMENT; TOUGHNESS; CONTOUR; PROFILE AB Residual stresses can be a main cause of fractures, but forensic failure analysis is difficult because the residual stresses are relaxed after fracture because of the new free surface. In this paper, a method is presented for a posteriori determination of the residual stresses by measuring the geometric mismatch between the mating fracture surfaces. Provided the fracture is not overly ductile, so that plasticity may be neglected, a simple, elastic calculation based on Bueckner's principle gives the original residual stresses normal to the fracture plane. The method was demonstrated on a large 7000 series aluminum alloy forging that fractured during an attempt to cut a section into two pieces. Neutron diffraction measurements on another section of the same forging convincingly validated the residual stresses determined from the fracture surface mismatch. After accounting for closure, an analysis of the residual stress intensity factor based on the measured residual stress agreed with the material's fracture toughness and fractographic evidence of the failure initiation site. The practicality of the fracture surface method to investigate various failures is discussed in light of the required assumptions. (C) 2013 Elsevier Ltd. All rights reserved. C1 [Prime, Michael B.; Clausen, Bjorn] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [DeWald, Adrian T.] Hill Engn LLC, Rancho Cordova, CA 95670 USA. [Hill, Michael R.; Minh Tran] Univ Calif Davis, Mech & Aerosp Engn Dept, Davis, CA 95616 USA. RP Prime, MB (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM prime@lanl.gov RI Clausen, Bjorn/B-3618-2015; Hill, Michael/A-2525-2016; OI Clausen, Bjorn/0000-0003-3906-846X; Hill, Michael/0000-0002-9168-211X; Prime, Michael/0000-0002-4098-5620 FU Los Alamos National Security, LLC for the National Nuclear Security Administration of the U.S. Department of Energy [DE-AC52-06NA25396]; Office of Basic Energy Sciences (DOE) FX The authors would like to thank Tom Holden and Don Brown for extensive consultation on texture and microstress effects in the neutron data, Jeremy Robinson of the University of Limerick for discussions on the stresses in 7000 series aluminum alloys, James Castle and The Boeing Company for providing the material and its pedigree for this paper from Boeing's internal study, and Mark James of the Alcoa Technical Center for technical discussions. Some of this work was performed at Los Alamos National Laboratory, 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. This work has benefited from the use of the Lujan Neutron Scattering Center at LANSCE, which is funded by the Office of Basic Energy Sciences (DOE). NR 49 TC 7 Z9 8 U1 1 U2 6 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0013-7944 EI 1873-7315 J9 ENG FRACT MECH JI Eng. Fract. Mech. PD JAN PY 2014 VL 116 BP 158 EP 171 DI 10.1016/j.engfracmech.2013.12.008 PG 14 WC Mechanics SC Mechanics GA AC4NE UT WOS:000332497200012 ER PT J AU Wu, JY Zhou, Y Gao, Y Fu, JS Johnson, BA Huang, C Kim, YM Liu, Y AF Wu, Jianyong Zhou, Ying Gao, Yang Fu, Joshua S. Johnson, Brent A. Huang, Cheng Kim, Young-Min Liu, Yang TI Estimation and Uncertainty Analysis of Impacts of Future Heat Waves on Mortality in the Eastern United States SO ENVIRONMENTAL HEALTH PERSPECTIVES LA English DT Article ID HEALTH WARNING SYSTEMS; CLIMATE-CHANGE; CITIES; RISK AB BACKGROUND: Climate change is anticipated to influence heat-related mortality in the future. However, estimates of excess mortality attributable to future heat waves are subject to large uncertainties and have not been projected under the latest greenhouse gas emission scenarios. OBJECTIVES: We estimated future heat wave mortality in the eastern United States (approximately 1,700 counties) under two Representative Concentration Pathways (RCPs) and investigated sources of uncertainty. METHODS: Using dynamically downscaled hourly temperature projections for 2057-2059, we projected heat wave days that were defined using four heat wave metrics and estimated the excess mortality attributable to them. We apportioned the sources of uncertainty in excess mortality estimates using a variance-decomposition method. RESULTS: Estimates suggest that excess mortality attributable to heat waves in the eastern United States would result in 200-7,807 deaths/year (mean 2,379 deaths/year) in 2057-2059. Average excess mortality projections under RCP4.5 and RCP8.5 scenarios were 1,403 and 3,556 deaths/year, respectively. Excess mortality would be relatively high in the southern states and eastern coastal areas (excluding Maine). The major sources of uncertainty were the relative risk estimates for mortality on heat wave versus non-heat wave days, the RCP scenarios, and the heat wave definitions. CONCLUSIONS: Mortality risks from future heat waves may be an order of magnitude higher than the mortality risks reported in 2002-2004, with thousands of heat wave-related deaths per year in the study area projected under the RCP8.5 scenario. Substantial spatial variability in county-level heat mortality estimates suggests that effective mitigation and adaptation measures should be developed based on spatially resolved data. C1 [Wu, Jianyong; Zhou, Ying; Kim, Young-Min; Liu, Yang] Emory Univ, Rollins Sch Publ Hlth, Dept Environm Hlth, Atlanta, GA 30322 USA. [Gao, Yang; Fu, Joshua S.] Univ Tennessee, Dept Civil & Environm Engn, Knoxville, TN USA. [Gao, Yang] Pacific NW Natl Lab, Atmospher Sci & Global Change Div, Richland, WA 99352 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 & Hlth Serv, Dept Global 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 RI Wu, Jianyong/A-6854-2011 OI Wu, Jianyong/0000-0002-5864-3186 FU Climate and Health Program at the Centers for Disease Control and Prevention (CDC)5 U01 EH000405; National Institutes of Health [1R21ES020225]; National Science Foundation [TG-ATM110009, UT-TENN0006]; Office of Science of the U.S. Department of Energy (DOE) [DE-AC05-00OR22725]; Office of Science of the U.S. Department of Energy as part of the Regional and Global Climate Modeling Program; Pacific Northwest National Laboratory [DE-AC05-76RL01830] FX The study was supported mainly by the Climate and Health Program at the Centers for Disease Control and Prevention (CDC; grant 5 U01 EH000405 managed by G. Luber) and by the National Institutes of Health (grant 1R21ES020225). The climate model simulations were supported in part by the National Science Foundation through TeraGrid resources provided by National Institute for Computational Sciences (grants TG-ATM110009 and UT-TENN0006). The data simulations 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 (DOE) (contract DE-AC05-00OR22725). Y.G. was supported in part 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 (contract DE-AC05-76RL01830). NR 37 TC 22 Z9 22 U1 4 U2 29 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 2014 VL 122 IS 1 BP 10 EP 16 DI 10.1289/ehp.1306670 PG 7 WC Environmental Sciences; Public, Environmental & Occupational Health; Toxicology SC Environmental Sciences & Ecology; Public, Environmental & Occupational Health; Toxicology GA AC6OT UT WOS:000332644200013 PM 24192064 ER PT J AU Logue, JM Klepeis, NE Lobscheid, AB Singer, BC AF Logue, Jennifer M. Klepeis, Neil E. Lobscheid, Agnes B. Singer, Brett C. TI Pollutant Exposures from Natural Gas Cooking Burners: A Simulation-Based Assessment for Southern California SO ENVIRONMENTAL HEALTH PERSPECTIVES LA English DT Article ID INDOOR AIR-QUALITY; NITROGEN-DIOXIDE; RESPIRATORY SYMPTOMS; NO2 CONCENTRATIONS; ENVIRONMENTS; ASSOCIATION; PERFORMANCE; VENTILATION; HOMES AB BACKGROUND: Residential natural gas cooking burners (NGCBs) can emit substantial quantities of pollutants, and they are typically used without venting range hoods. OBJECTIVE: We quantified pollutant concentrations and occupant exposures resulting from NGCB use in California homes. METHODS: A mass-balance model was applied to estimate time-dependent pollutant concentrations throughout homes in Southern California and the exposure concentrations experienced by individual occupants. We estimated nitrogen dioxide (NO2), carbon monoxide (CO), and formaldehyde (HCHO) concentrations for 1 week each in summer and winter for a representative sample of Southern California homes. The model simulated pollutant emissions from NGCBs as well as NO2 and CO entry from outdoors, dilution throughout the home, and removal by ventilation and deposition. Residence characteristics and outdoor concentrations of NO2 and CO were obtained from available databases. We inferred ventilation rates, occupancy patterns, and burner use from household characteristics. We also explored proximity to the burner(s) and the benefits of using venting range hoods. Replicate model executions using independently generated sets of stochastic variable values yielded estimated pollutant concentration distributions with geometric means varying by < 10%. RESULTS: The simulation model estimated that-in homes using NGCBs without coincident use of venting range hoods-62%, 9%, and 53% of occupants are routinely exposed to NO2, CO, and HCHO levels that exceed acute health-based standards and guidelines. NGCB use increased the sample median of the highest simulated 1-hr indoor concentrations by 100, 3,000, and 20 ppb for NO2, CO, and HCHO, respectively. CONCLUSIONS: Reducing pollutant exposures from NGCBs should be a public health priority. Simulation results suggest that regular use of even moderately effective venting range hoods would dramatically reduce the percentage of homes in which concentrations exceed health-based standards. C1 [Logue, Jennifer M.; Lobscheid, Agnes B.; Singer, Brett C.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Indoor Environm Grp, Berkeley, CA 94720 USA. [Logue, Jennifer M.; Singer, Brett C.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Residential Bldg Syst Grp, Berkeley, CA 94720 USA. [Klepeis, Neil E.] Stanford Univ, Dept Civil & Environm Engn, Stanford, CA 94305 USA. [Klepeis, Neil E.] San Diego State Univ, Res Fdn, Ctr Behav Epidemiol & Community Hlth C BEACH, Grad Sch Publ Hlth, San Diego, CA 92182 USA. RP Logue, JM (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, 1 Cyclotron Rd, Berkeley, CA 94720 USA. EM jmlogue@lbl.gov FU U.S. Department of Energy (DOE) Building America Program, Office of Energy Efficiency and Renewable Energy under DOE [DE-AC02-05CH11231]; U.S. Department of Housing and Urban Development, Office of Healthy Homes and Lead Hazard Control [I-PHI-01070]; U.S. Environmental Protection Agency Indoor Environments Division [DW-89-92322201-0]; California Energy Commission [500-05-026, 500-08-061] FX Funding for this research was provided by the U.S. Department of Energy (DOE) Building America Program, Office of Energy Efficiency and Renewable Energy under DOE contract DE-AC02-05CH11231; by the U.S. Department of Housing and Urban Development, Office of Healthy Homes and Lead Hazard Control through interagency agreement I-PHI-01070; by the U.S. Environmental Protection Agency Indoor Environments Division through interagency agreement DW-89-92322201-0; and by the California Energy Commission through contracts 500-05-026 and 500-08-061. NR 46 TC 11 Z9 11 U1 7 U2 39 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 2014 VL 122 IS 1 BP 43 EP 50 DI 10.1289/ehp.1306673 PG 8 WC Environmental Sciences; Public, Environmental & Occupational Health; Toxicology SC Environmental Sciences & Ecology; Public, Environmental & Occupational Health; Toxicology GA AC6OT UT WOS:000332644200017 PM 24192135 ER PT J AU Sathitsuksanoh, N Holtman, KM Yelle, DJ Morgan, T Stavila, V Pelton, J Blanch, H Simmons, BA George, A AF Sathitsuksanoh, Noppadon Holtman, Kevin M. Yelle, Daniel J. Morgan, Trevor Stavila, Vitalie Pelton, Jeffrey Blanch, Harvey Simmons, Blake A. George, Anthe TI Lignin fate and characterization during ionic liquid biomass pretreatment for renewable chemicals and fuels production SO GREEN CHEMISTRY LA English DT Article ID STATE 2D NMR; ENZYMATIC-HYDROLYSIS; DILUTE-ACID; WOOD LIGNIN; CELLULOSE; SPECTROSCOPY; SWITCHGRASS; SACCHARIFICATION; DELIGNIFICATION; LIGNOCELLULOSE AB The fate of lignin from wheat straw, Miscanthus, and Loblolly pine after pretreatment by a non-toxic and recyclable ionic liquid (IL), [C(2)mim][OAc], followed by enzymatic hydrolysis was investigated. The lignin partitioned into six process streams, each of which was quantified and analyzed by a combination of a novel solution-state two-dimensional (2D) nuclear magnetic resonance (NMR) method, and size exclusion chromatography (SEC). Pretreatment of biomass samples by [C(2)mim][OAc] at 120 and 160 degrees C enhances hydrolysis rates and enzymatic glucan digestions compared to those of untreated biomass samples. Lignin partitioning into the different streams can be controlled by altering the ionic liquid pre-treatment conditions, with higher temperatures favoring higher lignin partitioning to the IL stream. 2D NMR bond abundance data and SEC results reveal that lignin is depolymerized during ionic liquid pretreatment, and lignin of different molecular masses can be isolated in the different process streams. SEC suggested that higher molecular mass lignin was precipitated from the ionic liquid, leaving smaller molecular mass lignin in solution for further extraction. Lignin obtained as a residue of enzymatic hydrolysis contained the highest molecular mass molecules, similar in structure to the control lignin. The results suggest that isolated lignins via IL pretreatment from all three feedstocks were both depolymerized and did not contain new condensed structures. This finding leads to the possibility that lignin obtained from this IL pretreatment process may be more amenable to upgrading, thereby enhancing biorefinery economics. C1 [Sathitsuksanoh, Noppadon; Blanch, Harvey; Simmons, Blake A.; George, Anthe] Joint BioEnergy Inst, Emeryville, CA 94608 USA. [Holtman, Kevin M.] ARS, USDA, Western Reg Res Ctr, Albany, CA 94710 USA. [Yelle, Daniel J.] US Forest Serv, Forest Prod Lab, Madison, WI 53705 USA. [Morgan, Trevor] Univ Hawaii, Hawaii Nat Energy Inst, Honolulu, HI 96822 USA. [Stavila, Vitalie; Simmons, Blake A.; George, Anthe] Sandia Natl Labs, Livermore, CA USA. [Pelton, Jeffrey] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA 94720 USA. [Blanch, Harvey] Univ Calif Berkeley, Dept Chem & Biomol Engn, Berkeley, CA 94720 USA. RP Sathitsuksanoh, N (reprint author), Joint BioEnergy Inst, 5885 Hollis St, Emeryville, CA 94608 USA. EM ageorge@lbl.gov RI sathitsuksanoh, noppadon/O-6305-2014; OI sathitsuksanoh, noppadon/0000-0003-1521-9155; Simmons, Blake/0000-0002-1332-1810 FU Total; Office of Science, Office of Biological and Environmental Research, of the U.S. DOE [DE-AC02-05CH11231] FX This work was performed as part of a collaboration program between JBEI and Total. Noppadon Sathitsuksanoh's and Anthe George's work in this program is funded by Total. Angelique Chanal, Vineet Rajgarhia, Laurent Fourage and Henri Strub, Total New Energies - R&D, are acknowledged for their contribution to this collaborative program. The portion of the work conducted by the Joint BioEnergy Institute was supported by the Office of Science, Office of Biological and Environmental Research, of the U.S. DOE under Contract no. DE-AC02-05CH11231. NR 42 TC 28 Z9 29 U1 6 U2 84 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 2014 VL 16 IS 3 BP 1236 EP 1247 DI 10.1039/c3gc42295j PG 12 WC Chemistry, Multidisciplinary; GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY SC Chemistry; Science & Technology - Other Topics GA AB8KO UT WOS:000332039200033 ER PT J AU Mukarakate, C Zhang, XD Stanton, AR Robichaud, DJ Ciesielski, PN Malhotra, K Donohoe, BS Gjersing, E Evans, RJ Heroux, DS Richards, R Iisa, K Nimlos, MR AF Mukarakate, Calvin Zhang, Xiaodong Stanton, Alexander R. Robichaud, David J. Ciesielski, Peter N. Malhotra, Kara Donohoe, Bryon S. Gjersing, Erica Evans, Robert J. Heroux, David S. Richards, Ryan Iisa, Kristiina Nimlos, Mark R. TI Real-time monitoring of the deactivation of HZSM-5 during upgrading of pine pyrolysis vapors SO GREEN CHEMISTRY LA English DT Article ID FRACTIONAL CATALYTIC PYROLYSIS; FLUIDIZED-BED REACTOR; CRUDE BIO-OIL; COKE FORMATION; BIOMASS PYROLYSIS; MOLECULAR CHARACTERIZATION; ZEOLITE CATALYST; CONVERSION; HYDROCARBONS; METHANOL AB The conversion of pine pyrolysis vapors over fixed beds of HZSM-5 catalyst was studied as a function of deactivation of the catalyst, presumably by coking. Small laboratory reactors were used in this study in which the products were identified using a molecular beam mass spectrometer (MBMS) and gas chromatography mass spectrometry (GCMS). In all of these experiments, real-time measurements of the products formed were conducted as the catalyst aged and deactivated during upgrading. The results from these experiments showed the following: (1) Fresh catalyst produces primarily aromatic hydrocarbons and olefins with no detectable oxygen-containing species. (2) After pyrolysis of roughly the same weight of biomass as weight of catalyst, oxygenated products begin to appear in the product stream. This suite of oxygen containing products appears different from the products formed when the catalyst is fresh and when the catalyst is completely deactivated. In particular, phenol and cresols are measured while upgrading pine, cellulose and lignin pyrolysis vapors, suggesting that these products are intermediates or side products formed during upgrading. (3) After the addition of more pyrolysis vapors, the product stream consists of primary vapors from pine pyrolysis. Catalyst samples collected at various points during deactivation were analyzed using a variety of tools. The results show that carbon build-up is correlated with catalyst deactivation, suggesting that deactivation is due to coking. Further, studies of nitrogen adsorption on the used catalyst suggest that coking initially occurs on the outside of the catalyst, leaving the micropores largely intact. From a practical point of view, it appears that based upon this study and others in the literature, the amount of oxygen in the upgraded products can be related to the level of deactivation of the HZSM-5 catalyst, which can be determined by how much pyrolysis vapor is run over the catalyst. C1 [Mukarakate, Calvin; Robichaud, David J.; Gjersing, Erica; Iisa, Kristiina; Nimlos, Mark R.] Natl Renewable Energy Lab, Natl Bioenergy Ctr, Golden, CO 80401 USA. [Zhang, Xiaodong] Acad Sci, Energy Res Inst Shadong, Jinan 250014, Peoples R China. [Stanton, Alexander R.] Colorado State Univ, Dept Chem & Biol Engn, Ft Collins, CO 80523 USA. [Ciesielski, Peter N.; Donohoe, Bryon S.] Natl Renewable Energy Lab, Biosci Ctr, Golden, CO 80401 USA. [Malhotra, Kara] Cornell Univ, Dept Mech & Aerosp Engn, Ithaca, NY 14853 USA. [Evans, Robert J.] MicroChem Technol Inc, Boulder, CO 80301 USA. [Heroux, David S.] St Michaels Coll, Dept Chem, Colchester, VT 05439 USA. [Richards, Ryan] Colorado Sch Mines, Dept Chem & Geochem, Golden, CO 80401 USA. RP Mukarakate, C (reprint author), Natl Renewable Energy Lab, Natl Bioenergy Ctr, 15013 Denver West Pkwy, Golden, CO 80401 USA. EM calvin.mukarakate@nrel.gov RI Richards, Ryan/B-3513-2008 FU U.S. Department of Energy's Bioenergy Technologies Office (DOE-BETO) [DE-AC36-08GO28308]; National Renewable Energy Laboratory FX This work was supported by the U.S. Department of Energy's Bioenergy Technologies Office (DOE-BETO) Contract No. DE-AC36-08GO28308 with the National Renewable Energy Laboratory. Albemarle is acknowledged for providing the catalyst sample. The authors would like to thank, Lynn Gedvilas, Kristen Ryan, John Yarbrough, Sridhar Budhi, Daniel Carpenter, Rick French, and Stefan Czernik for stimulating discussions. NR 70 TC 30 Z9 30 U1 4 U2 58 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 2014 VL 16 IS 3 BP 1444 EP 1461 DI 10.1039/c3gc42065e PG 18 WC Chemistry, Multidisciplinary; GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY SC Chemistry; Science & Technology - Other Topics GA AB8KO UT WOS:000332039200056 ER PT J AU Vardon, DR Sharma, BK Jaramillo, H Kim, D Choe, JK Ciesielski, PN Strathmann, TJ AF Vardon, Derek R. Sharma, Brajendra K. Jaramillo, Humberto Kim, Dongwook Choe, Jong Kwon Ciesielski, Peter N. Strathmann, Timothy J. TI Hydrothermal catalytic processing of saturated and unsaturated fatty acids to hydrocarbons with glycerol for in situ hydrogen production SO GREEN CHEMISTRY LA English DT Article ID PLATINUM-RHENIUM CATALYSTS; CARBON-SUPPORTED PLATINUM; PD(111) MODEL SURFACES; MODIFIED NI CATALYSTS; AQUEOUS-PHASE; OXYGENATED HYDROCARBONS; VEGETABLE-OILS; BIODIESEL PRODUCTION; SUPERCRITICAL WATER; REACTION PATHWAYS AB Lipids are a promising feedstock to produce renewable hydrocarbon fuels and H-2 via catalytic hydrothermal processing. Upon exposure to hydrothermal media (e.g., 300 degrees C, 8-11 MPa), lipids rapidly hydrolyze to produce saturated and unsaturated free fatty acids in varying ratios, depending on the feedstock, as well as glycerol. This report demonstrates the potential of Pt-Re/C for the hydrothermal conversion of saturated and unsaturated fatty acids to hydrocarbons, using glycerol reforming for in situ H2 production to meet process demands. Experiments showed that deoxygenation of stearic acid, a model saturated fatty acid, was significantly enhanced with Pt-Re/C under a reducing atmosphere compared to Pt/C. The coupled hydrogenation and deoxygenation (HYD-DOX) of oleic aid, a model unsaturated fatty acid, was also moderately enhanced under an inert atmosphere using glycerol for in situ H-2 production, with DOX as the rate-limiting step. Characterization of Pt-Re/C showed that Re had a significant effect on CO: H uptake ratio (2.2) compared to commercial Pt/C (1.3), with the metals dispersed as small crystallites (similar to 3-4 nm) throughout carbon support. Experiments revealed that the initial system H-2 headspace loading <3.45 MPa greatly enhances fatty acid DOX kinetics via decarboxylation/decarbonylation without net H2 consumption. At higher initial H2 loadings (>= 3.45 MPa), fatty acid reduction was also observed as a minor DOX pathway. Experiments also showed that oleic acid HYD-DOX and glycerol reforming are affected by initial glycerol concentration and catalyst loading. Under optimized process conditions, complete HYD-DOX of oleic acid to heptadecane was achieved within 2 h with a net-zero H2 consumption using a 1 : 3 glycerol-to-fatty acid ratio (i.e., the native ratio in triacylglycerides). X-ray photoelectron spectroscopy showed that H2 in the reactor headspace results in lower oxidation states of Pt and Re, suggesting a possible mechanism for enhanced DOX kinetics. This approach holds promise for overcoming the high external H2 demands of conventional lipid hydrotreatment processes. C1 [Vardon, Derek R.; Jaramillo, Humberto; Choe, Jong Kwon; Strathmann, Timothy J.] Univ Illinois, Dept Civil & Environm Engn, Urbana, IL 61801 USA. [Sharma, Brajendra K.] Univ Illinois, Illinois Sustainable Technol Ctr, Champaign, IL 61820 USA. [Kim, Dongwook] Korea Mil Acad, Dept Chem, Seoul 139799, South Korea. [Ciesielski, Peter N.] Natl Renewable Energy Lab, Golden, CO 80401 USA. RP Vardon, DR (reprint author), Univ Illinois, Dept Civil & Environm Engn, 205 N Mathews Ave, Urbana, IL 61801 USA. EM dvardon2@illinois.edu RI Strathmann, Timothy/K-7606-2012; Vardon, Derek/B-8249-2017 OI Strathmann, Timothy/0000-0002-7299-3115; Vardon, Derek/0000-0002-0199-4524 FU United States Environmental Protection Agency (EPA) under the Science to Achieve Results (STAR) Graduate Fellowship Program; National Science Foundation Graduate Research Fellowship [DGE-1144245]; Department of Civil and Environmental Engineering at the University of Illinois; National Science Foundation Division of Chemical, Bioengineering, Environmental, and Transport Systems [CBET-0746453]; U.S. Department of Energy [DEFG02-91-ER45439]; Center for Direct Catalytic Conversion of Biomass to Biofuels [C3Bio]; Energy Frontier Research Center; U.S. DOE, Office of Science, Office of Basic Energy Sciences [DE-SC0000997] FX The research described in this paper has been funded in part by the United States Environmental Protection Agency (EPA) under the Science to Achieve Results (STAR) Graduate Fellowship Program. The EPA has not officially endorsed this publication and the views expressed herein may not reflect the views of the EPA. This material is also based upon work supported by the National Science Foundation Graduate Research Fellowship (DGE-1144245). Any opinion, findings, and conclusions or recommendations expressed in this material are those of the authors and do not necessarily reflect the views of the National Science Foundation. In addition, financial support was provided by the Department of Civil and Environmental Engineering at the University of Illinois and the National Science Foundation Division of Chemical, Bioengineering, Environmental, and Transport Systems (CBET-0746453).; We thank Rick Haasch for assistance with XPS analysis at the Center of Microanalysis of Materials (UIUC), which is supported by the U.S. Department of Energy under grant DEFG02-91-ER45439. Catalyst characterization was also supported in part by the Center for Direct Catalytic Conversion of Biomass to Biofuels (C3Bio), an Energy Frontier Research Center funded by the U.S. DOE, Office of Science, Office of Basic Energy Sciences, Award Number DE-SC0000997. Additionally, we would like to thank Martin Menart at the Colorado School of Mines for assistance with catalyst chemisorption measurements. NR 46 TC 18 Z9 19 U1 9 U2 77 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 2014 VL 16 IS 3 BP 1507 EP 1520 DI 10.1039/c3gc41798k PG 14 WC Chemistry, Multidisciplinary; GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY SC Chemistry; Science & Technology - Other Topics GA AB8KO UT WOS:000332039200062 ER PT J AU Han, JJ Kunde, YA Hong-Geller, E Werner, JH AF Han, Jason J. Kunde, Yuliya A. Hong-Geller, Elizabeth Werner, James H. TI Actin restructuring during Salmonella typhimurium infection investigated by confocal and super-resolution microscopy SO JOURNAL OF BIOMEDICAL OPTICS LA English DT Article DE super-resolution; fluorescence microscopy; host-pathogen; bacteria; protein ID STRUCTURED ILLUMINATION MICROSCOPY; SINGLE-MOLECULE LOCALIZATION; FLUORESCENT-PROBES; HOST-CELLS; RESOLUTION LIMIT; EPITHELIAL-CELLS; III SECRETION; 3 DIMENSIONS; PROTEINS; TRACKING AB We have used super-resolution optical microscopy and confocal microscopy to visualize the cytoskeletal restructuring of HeLa cells that accompanies and enables Salmonella typhimurium internalization. Herein, we report the use of confocal microscopy to verify and explore infection conditions that would be compatible with super-resolution optical microscopy, using Alexa-488 labeled phalloidin to stain the actin cytoskeletal network. While it is well known that actin restructuring and cytoskeletal rearrangements often accompany and assist in bacterial infection, most studies have employed conventional diffraction-limited fluorescence microscopy to explore these changes. Here we show that the superior spatial resolution provided by single-molecule localization methods (such as direct stochastic optical reconstruction microscopy) enables more precise visualization of the nanoscale changes in the actin cytoskeleton that accompany bacterial infection. In particular, we found that a thin (100-nm) ring of actin often surrounds an invading bacteria 10 to 20 min postinfection, with this ring being transitory in nature. We estimate that a few hundred monofilaments of actin surround the S. typhimurium in this heretofore unreported bacterial internalization intermediate. (C) The Authors. Published by SPIE under a Creative Commons Attribution 3.0 Unported License. Distribution or reproduction of this work in whole or in part requires full attribution of the original publication, including its DOI. C1 [Han, Jason J.; Werner, James H.] Los Alamos Natl Lab, Ctr Integrated Nanotechnol, Los Alamos, NM 87545 USA. [Kunde, Yuliya A.; Hong-Geller, Elizabeth] Los Alamos Natl Lab, Biosci Div, Los Alamos, NM 87545 USA. RP Werner, JH (reprint author), Los Alamos Natl Lab, Ctr Integrated Nanotechnol, POB 1663, Los Alamos, NM 87545 USA. EM jwerner@lanl.gov FU Los Alamos National Laboratory Directed Research and Development (LDRD) program; Los Alamos National Laboratory [DE-AC52-06NA25396] FX This work was supported by the Los Alamos National Laboratory Directed Research and Development (LDRD) program and was in part performed at the Center for Integrated Nanotechnologies, a U.S. Department of Energy, Office of Basic Energy Sciences user facility at Los Alamos National Laboratory (Contract DE-AC52-06NA25396). NR 44 TC 5 Z9 5 U1 2 U2 10 PU SPIE-SOC PHOTO-OPTICAL INSTRUMENTATION ENGINEERS PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98225 USA SN 1083-3668 EI 1560-2281 J9 J BIOMED OPT JI J. Biomed. Opt. PD JAN PY 2014 VL 19 IS 1 AR 016011 DI 10.1117/1.JBO.19.1.016011 PG 8 WC Biochemical Research Methods; Optics; Radiology, Nuclear Medicine & Medical Imaging SC Biochemistry & Molecular Biology; Optics; Radiology, Nuclear Medicine & Medical Imaging GA AB6IZ UT WOS:000331892700043 PM 24413454 ER PT J AU Tavakoli, M Cholis, I Evoli, C Ullio, P AF Tavakoli, Maryam Cholis, Ilias Evoli, Carmelo Ullio, Piero TI Constraints on dark matter annihilations from diffuse gamma-ray emission in the Galaxy SO JOURNAL OF COSMOLOGY AND ASTROPARTICLE PHYSICS LA English DT Article DE dark matter theory; gamma ray theory; gamma ray experiments; cosmic ray theory ID INTERSTELLAR RADIATION-FIELD; STAR-FORMING GALAXIES; MILKY-WAY; FERMI-LAT; BACKGROUND-RADIATION; MOLECULAR GAS; 3-DIMENSIONAL DISTRIBUTION; EMPIRICAL-MODELS; HELIUM SPECTRA; COSMIC-RAYS AB Recent advances in gamma-ray cosmic ray, infrared and radio astronomy have allowed us to develop a significantly better understanding of the galactic medium properties in the last few years. In this work using the DRAGON code, that numerically solves the GR propagation equation and calculating gamma-ray emissivities in a 2-dimensional grid enclosing the Galaxy, we study in a self consistent manner models for the galactic diffuse gamma-ray emission. Our models are cross-checked to both the available CR and gamma-ray data We address the extend to which dark matter annihilations in the Galaxy can contribute to the diffuse gamma-ray flux towards different directions on the sky. Moreover we discuss the impact that astrophysical uncertainties of non DM nature. have on the derived gamma-ray limits. Such uncertainties are related to the diffusion properties on the Galaxy, the interstellar gas and the interstellar radiation field energy densities. Light similar to 10 GeV dark matter annihilating dominantly to hadrons is more strongly constrained by gamma-ray observations towards the inner parts of the Galaxy and influenced the most by assumptions of the gas distribution; while TeV scale DM annihilating dominantly to leptons has its tightest constraints from observations towards the galactic center avoiding the galactic disk plane, with the main astrophysical uncertainty being the radiation field energy density. In addition, we present a method of deriving constraints on the dark matter distribution profile from the diffuse gamma-ray spectra. These results critically depend on the assumed mass of the dark matter particles and the type of its end annihilation products. C1 [Tavakoli, Maryam; Evoli, Carmelo] Univ Hamburg, Inst Theoret Phys 2, D-22761 Hamburg, Germany. [Tavakoli, Maryam] Inst Res Fundamental Sci IPM, Sch Astron, Tehran, Iran. [Cholis, Ilias] Fermilab Natl Accelerator Lab, Ctr Particle Astrophys, Batavia, IL 60510 USA. [Ullio, Piero] SISSA, I-34136 Trieste, Italy. [Ullio, Piero] Ist Nazl Fis Nucl, Sez Trieste, I-34136 Trieste, Italy. RP Tavakoli, M (reprint author), Univ Hamburg, Inst Theoret Phys 2, Luruper Chaussee 149, D-22761 Hamburg, Germany. EM maryam.tavakoli@desy.de; cholis@fnal.gov; carmelo.evoli@desy.de; ullio@sissa.it OI Evoli, Carmelo/0000-0002-6023-5253 FU German Science Foundation (DFG) under the Collaborative Research Center [(SFB) 676]; Helmholtz Alliance for Astro-particle Physics; Initiative and Networking Fund of the Helmholtz Association; US Department of Energy FX The authors acknowledge the use of the Fermi-LAT: data and parts of the "FermiTools" publicly available at http://fermi.gsfc.nasa.gov/ssc/. We also acknowledge using HEALPix [167]. We would like to thank Alessandro Cuoco, Dan Hooper, Hani Nurbiantoro Santosa, Meng Su and Gabrijela Zaharijas for the valuable discussions we have shared. The work of MT is supported by the German Science Foundation (DFG) under the Collaborative Research Center (SFB) 676 Particles, Strings and the Early Universe. MT also thanks ICTP-SAIFR. for its hospitality during the final stages of this work. CE acknowledges support from the Helmholtz Alliance for Astro-particle Physics funded by the Initiative and Networking Fund of the Helmholtz Association. This work has been supported in part by the US Department of Energy (IC). NR 191 TC 17 Z9 17 U1 1 U2 8 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 1475-7516 J9 J COSMOL ASTROPART P JI J. Cosmol. Astropart. Phys. PD JAN PY 2014 IS 1 AR 017 DI 10.1088/1475-7516/2014/01/017 PG 38 WC Astronomy & Astrophysics; Physics, Particles & Fields SC Astronomy & Astrophysics; Physics GA AA5JZ UT WOS:000331134400018 ER PT J AU Lorbeer, C Cybinska, J Mudring, AV AF Lorbeer, Chantal Cybinska, Joanna Mudring, Anja-Verena TI Reaching quantum yields >> 100% in nanomaterials SO JOURNAL OF MATERIALS CHEMISTRY C LA English DT Article ID IONIC LIQUIDS; RUTHENIUM NANOPARTICLES; DOWNCONVERSION; NANOSTRUCTURES; LUMINESCENCE; NANOCRYSTALS; TRIFLUORIDES; LIGDF4-EU3+; CRYSTALS; ROUTE AB For the first time, it has been realized that trigonal GdF3:Eu, which is usually only accessible at high temperatures and very high pressures, has a superior capability as a host material for quantum-cutting materials compared to orthorhombic phase GdF3:Eu. Synthesis of these materials from ionic liquids does not only allow us to obtain oxygen-free, nanoscale fluorides - a prerequisite for fluoride quantum cutters, but by changing the ionic liquid it becomes also possible to tune the phase of the nanoparticles and thus, most importantly, the quantum cutting efficiency of the final material. C1 [Lorbeer, Chantal; Cybinska, Joanna; Mudring, Anja-Verena] Ruhr Univ Bochum, Fak Chem & Biochem, D-44780 Bochum, Germany. [Cybinska, Joanna] Univ Wroclaw, Fac Chem, PL-50383 Wroclaw, Poland. [Mudring, Anja-Verena] Iowa State Univ, Dept Mat Sci & Engn, Ames, IA 50010 USA. [Mudring, Anja-Verena] Ames Lab DOE, Crit Mat Inst, Ames, IA 50010 USA. RP Mudring, AV (reprint author), Ruhr Univ Bochum, Fak Chem & Biochem, D-44780 Bochum, Germany. EM anja.mudring@ruhr-uni-bochum.de FU European Research Council through an ERC [200475]; DESY [II-20090181]; Fonds der Chemischen Industrie; 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 acknowledge support by the European Research Council through an ERC Starting Grant ("EMIL", contract no. 200475) and DESY (proposal no. II-20090181). The Fonds der Chemischen Industrie is acknowledged for a Dozentenstipendium for AVM and a Doktorandenstipendium for CL. This work is also 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 38 TC 13 Z9 13 U1 4 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 2014 VL 2 IS 10 BP 1862 EP 1868 DI 10.1039/c3tc31662a PG 7 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA AB8GI UT WOS:000332027800013 ER PT J AU Simon, CM Kim, J Lin, LC Martin, RL Haranczyk, M Smit, B AF Simon, Cory M. Kim, Jihan Lin, Li-Chiang Martin, Richard L. Haranczyk, Maciej Smit, Berend TI Optimizing nanoporous materials for gas storage SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID METAL-ORGANIC FRAMEWORKS; CRYSTALLINE POROUS MATERIALS; METHANE STORAGE; NATURAL-GAS; HYDROGEN STORAGE; ISOSTERIC HEAT; ADSORPTION; ZEOLITES; CARBON; SCALE AB In this work, we address the question of which thermodynamic factors determine the deliverable capacity of methane in nanoporous materials. The deliverable capacity is one of the key factors that determines the performance of a material for methane storage in automotive fuel tanks. To obtain insights into how the molecular characteristics of a material are related to the deliverable capacity, we developed several statistical thermodynamic models. The predictions of these models are compared with the classical thermodynamics approach of Bhatia and Myers [Bhatia and Myers, Langmuir, 2005, 22, 1688] and with the results of molecular simulations in which we screen the International Zeolite Association (IZA) structure database and a hypothetical zeolite database of over 100 000 structures. Both the simulations and our models do not support the rule of thumb that, for methane storage, one should aim for an optimal heat of adsorption of 18.8 kJ mol(-1). Instead, our models show that one can identify an optimal heat of adsorption, but that this optimal heat of adsorption depends on the structure of the material and can range from 8 to 23 kJ mol(-1). The different models we have developed are aimed to determine how this optimal heat of adsorption is related to the molecular structure of the material. C1 [Simon, Cory M.; Lin, Li-Chiang; Smit, Berend] Univ Calif Berkeley, Dept Chem & Biomol Engn, Berkeley, CA 94720 USA. [Kim, Jihan] Korea Adv Inst Sci & Technol, Dept Chem & Biomol Engn, Taejon 305701, South Korea. [Martin, Richard L.; Haranczyk, Maciej] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Simon, CM (reprint author), Univ Calif Berkeley, Dept Chem & Biomol Engn, Berkeley, CA 94720 USA. EM CoryMSimon@gmail.com RI Smit, Berend/B-7580-2009; Martin, Richard/C-7129-2013; Kim, Jihan/H-8002-2013; Lin, Li-Chiang/J-8120-2014; Haranczyk, Maciej/A-6380-2014; OI Smit, Berend/0000-0003-4653-8562; Martin, Richard/0000-0001-9858-2608; Haranczyk, Maciej/0000-0001-7146-9568; Lin, Li-Chiang/0000-0002-2821-9501; Simon, Cory/0000-0002-8181-9178 FU U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences [DE-FG02-12ER16362]; Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231] FX Thanks to Lev Sarkisov for statistical mechanics discussions and Stack Overflow for answering plotting questions. This work is supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences under Award DE-FG02-12ER16362. 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 46 TC 17 Z9 17 U1 2 U2 49 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 2014 VL 16 IS 12 BP 5499 EP 5513 DI 10.1039/c3cp55039g PG 15 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA AC3DZ UT WOS:000332396500007 PM 24394864 ER PT J AU Wilson, AD Stewart, FF AF Wilson, Aaron D. Stewart, Frederick F. TI Structure-function study of tertiary amines as switchable polarity solvents SO RSC ADVANCES LA English DT Article ID CARBON-DIOXIDE ABSORPTION; DRIVEN MEMBRANE PROCESSES; ROOM-TEMPERATURE; IONIC LIQUIDS; LIPID EXTRACTION; DRAW SOLUTES; GREEN CHEMISTRY; OSMOSIS; CAPTURE; AMIDINES AB A series of tertiary amines have been screened for their function as switchable polarity solvents (SPS). The relative ratios of tertiary amine and carbonate species as well as maximum possible concentration were determined through quantitative H-1 and C-13 NMR spectroscopy. The viscosities of the polar SPS solutions were measured and ranged from near water in dilute systems through to gel formation at high concentrations. The van't Hoff indices for SPS solutions were measured through freezing point depression studies as a proxy for osmotic pressures. A new form of SPS with an amine : carbonate ratio significantly greater than unity has been identified. Tertiary amines that function as SPS at ambient pressures appear to be limited to molecules with fewer than 12 carbons. The N,N-dimethyl-n-alkylamine structure has been identified as important to the function of an SPS. C1 [Wilson, Aaron D.; Stewart, Frederick F.] 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 Fund (LDRD) [14-079] 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 Fund (LDRD) under project 14-079. NR 55 TC 16 Z9 16 U1 7 U2 64 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 2014 VL 4 IS 22 BP 11039 EP 11049 DI 10.1039/c3ra47724j PG 11 WC Chemistry, Multidisciplinary SC Chemistry GA AC4CZ UT WOS:000332469500003 ER PT J AU Thompson, RL Shi, W Albenze, E Kusuma, VA Hopkinson, D Damodaran, K Lee, AS Kitchin, JR Luebke, DR Nulwala, H AF Thompson, Robert L. Shi, Wei Albenze, Erik Kusuma, Victor A. Hopkinson, David Damodaran, Krishnan Lee, Anita S. Kitchin, John R. Luebke, David R. Nulwala, Hunaid TI Probing the effect of electron donation on CO2 absorbing 1,2,3-triazolide ionic liquids SO RSC ADVANCES LA English DT Article ID CARBON-DIOXIDE; STRONG BASES; CAPTURE; ANION; TEMPERATURE; PHASE; TAUTOMERISM; ABSORPTION; SEPARATION; CHEMISTRY AB Development of the next generation materials for effective separation of gases is required to address various issues in energy and environmental applications. Ionic liquids (ILs) are among the most promising material types. To overcome the many hurdles in making a new class of materials technologically applicable, it is necessary to identify, access, and scale up a range of representative substances. In this work, CO2 reactive triazolide ILs were synthesized and characterized with the aim of developing a deeper understanding of how structural changes affect the overall properties of these substances. It was found that substituents on the anion play a crucial role in dictating the physical properties for CO2 capture. Depending upon the anion substituent, CO2 capacities between 0.07 and 0.4 mol CO2 per mol IL were observed. It was found that less sterically-hindered anions and anions containing electron donating groups were more reactive towards CO2. Detailed spectroscopic, CO2 absorption, rheological, and simulation studies were carried out to understand the nature and influence of these substituents. The effect of water content was also evaluated, and it was found that water had an unexpected impact on the properties of these materials, resulting in an increased viscosity, but little change in the CO2 reactivity. C1 [Thompson, Robert L.; Shi, Wei; Albenze, Erik; Kusuma, Victor A.; Hopkinson, David; Luebke, David R.; Nulwala, Hunaid] US DOE, Natl Energy Technol Lab, Pittsburgh, PA 15236 USA. [Thompson, Robert L.; Shi, Wei; Albenze, Erik] URS Corp, South Pk, PA 15129 USA. [Damodaran, Krishnan] Univ Pittsburgh, Dept Chem, Pittsburgh, PA 15260 USA. [Lee, Anita S.; Kitchin, John R.] Carnegie Mellon Univ, Dept Chem Engn, Pittsburgh, PA 15213 USA. [Nulwala, Hunaid] Carnegie Mellon Univ, Dept Chem, Pittsburgh, PA 15213 USA. RP Thompson, RL (reprint author), US DOE, Natl Energy Technol Lab, 626 Cochrans Mill Rd, Pittsburgh, PA 15236 USA. EM robert.thompson@contr.netl.doe.gov; hnulwala@andrew.cmu.edu RI Kitchin, John/A-2363-2010; Nulwala, Hunaid/G-8126-2012; OI Kitchin, John/0000-0003-2625-9232; Nulwala, Hunaid/0000-0001-7481-3723; Kusuma, Victor/0000-0002-7881-4536 FU Department of Energy, National Energy Technology Laboratory, an agency of the United States Government, through URS Energy & Construction, Inc. FX 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 39 TC 7 Z9 7 U1 6 U2 34 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 2014 VL 4 IS 25 BP 12748 EP 12755 DI 10.1039/c3ra47097k PG 8 WC Chemistry, Multidisciplinary SC Chemistry GA AC4IQ UT WOS:000332485000017 ER PT J AU Ebeida, MS Patney, A Mitchell, SA Dalbey, KR Davidson, AA Owens, JD AF Ebeida, Mohamed S. Patney, Anjul Mitchell, Scott A. Dalbey, Keith R. Davidson, Andrew A. Owens, John D. TI k-d Darts: Sampling by k-Dimensional Flat Searches SO ACM TRANSACTIONS ON GRAPHICS LA English DT Article DE Algorithms; Theory; Sampling; dimension; line search; thin regions; rendering; depth-of-field; Poisson-disk sampling; Monte Carlo integration; Latin hypercube sampling; uncertainty quantification ID ALGORITHM AB We formalize sampling a function using k-d darts. A k-d dart is a set of independent, mutually orthogonal, k-dimensional hyperplanes called k-d flats. A dart has d choose k flats, aligned with the coordinate axes for efficiency. We show k-d darts are useful for exploring a function's properties, such as estimating its integral, or finding an exemplar above a threshold. We describe a recipe for converting some algorithms from point sampling to k-d dart sampling, if the function can be evaluated along a k-d flat. We demonstrate that k-d darts are more efficient than point-wise samples in high dimensions, depending on the characteristics of the domain: for example, the subregion of interest has small volume and evaluating the function along a flat is not too expensive. We present three concrete applications using line darts (1-d darts): relaxed maximal Poisson-disk sampling, high-quality rasterization of depth-of-field blur, and estimation of the probability of failure from a response surface for uncertainty quantification. Line darts achieve the same output fidelity as point sampling in less time. For Poisson-disk sampling, we use less memory, enabling the generation of larger point distributions in higher dimensions. Higher-dimensional darts provide greater accuracy for a particular volume estimation problem. C1 [Ebeida, Mohamed S.; Mitchell, Scott A.; Dalbey, Keith R.] Sandia Natl Labs, Albuquerque, NM 87123 USA. [Patney, Anjul; Davidson, Andrew A.; Owens, John D.] Univ Calif Davis, Davis, CA 95616 USA. RP Mitchell, SA (reprint author), Sandia Natl Labs, 1515 Eubank, Albuquerque, NM 87123 USA. EM samitch@sandia.gov FU Sandia's Validation and Verification program; Computer Science Research Institute; National Science Foundation [CCF-1017399]; Sandia LDRD award [13-0144]; UC Lab Fees Research Program [12-LR-238449]; NVIDIA; Intel; Intel Science and Technology Center for Visual Computing; U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX M. S. Ebeida, S. A. Mitchell, and K. R. Dalbey thank Sandia's Validation and Verification program, and Computer Science Research Institute for supporting this work. A. Patney, A. A. Davidson, and J. D. Owens thank the National Science Foundation (grant no. CCF-1017399), Sandia LDRD award no. 13-0144, UC Lab Fees Research Program award no. 12-LR-238449, NVIDIA and Intel Graduate Fellowships, and the Intel Science and Technology Center for Visual Computing for supporting this work. 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 34 TC 2 Z9 2 U1 0 U2 1 PU ASSOC COMPUTING MACHINERY PI NEW YORK PA 2 PENN PLAZA, STE 701, NEW YORK, NY 10121-0701 USA SN 0730-0301 EI 1557-7368 J9 ACM T GRAPHIC JI ACM Trans. Graph. PD JAN PY 2014 VL 33 IS 1 AR 3 DI 10.1145/2522528 PG 16 WC Computer Science, Software Engineering SC Computer Science GA AB9MM UT WOS:000332118300003 ER PT J AU Dissanayake, DMNM Ashraf, A Pang, YT Eisaman, MD AF Dissanayake, D. M. Nanditha M. Ashraf, Ahsan Pang, Yutong Eisaman, Matthew D. TI Mapping Spatially Resolved Charge Collection Probability within P3HT:PCBM Bulk Heterojunction Photovoltaics SO ADVANCED ENERGY MATERIALS LA English DT Article DE charge transport; solar cells; conjugated polymers; fullerenes; thin films ID ORGANIC SOLAR-CELLS; SELF-ORGANIZATION; POLYMER; TRANSPORT; MORPHOLOGY; FILMS; BLENDS; METHANOFULLERENE; CRYSTALLINITY; DISSOCIATION AB Material properties in polymer and fullerene bulk heterojunctions (BHJs) such as donor to acceptor volume fraction, morphology, and molecular orientation critically influence light absorption, exciton dissociation, charge transport, and recombination, all of which are crucial device properties in organic photovoltaics (OPV). Spatial variation of BHJ properties normal to the substrate, caused by phase segregation, can thereby create corresponding spatial variations in the OPVs optoelectronic properties. Here, normally incident and wave-guided optical modes are used to selectively excite localized regions within an inverted poly(3-hexythiophene-2,5-diyl) and phenyl-C61-butyric acid methyl ester BHJ OPV and corresponding internal quantum efficiencies are measured to study the spatial-dependent charge carrier collection probability within the BHJ. An electron-limited charge collection profile is observed for a thick (920 nm) BHJ due to fullerene-poor regions as a result of phase segregation. As the thickness of the BHJ is reduced (100 nm), charge transport is seen to be unaffected by the phase segregation. This has the potential to be a versatile non-destructive characterization technique for measuring the spatially varying charge collection probability in thin film photovoltaics and will help enable optimum device design and characterization. C1 [Dissanayake, D. M. Nanditha M.; Ashraf, Ahsan; Pang, Yutong; Eisaman, Matthew D.] Brookhaven Natl Lab, Sustainable Energy Technol Dept, Upton, NY 11973 USA. [Ashraf, Ahsan; Pang, Yutong; Eisaman, Matthew D.] SUNY Stony Brook, Dept Phys & Astron, Stony Brook, NY 11794 USA. RP Dissanayake, DMNM (reprint author), Brookhaven Natl Lab, Sustainable Energy Technol Dept, Upton, NY 11973 USA. EM ndissanayake@bnl.gov FU U.S. Department of Energy, Office of Basic Energy Sciences [DE-AC02-98CH10886]; U.S. Department of Energy, Sustainable Energy Technologies Department [DE-AC02-98CH10886]; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-ACO2-98CH10886] FX 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. This work was also partially supported by the U.S. Department of Energy, Sustainable Energy Technologies Department under contract DE-AC02-98CH10886. NEXAFS was performed at National Institute of Standards and Technology beamline U7A at the National Synchrotron Light Source. 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-ACO2-98CH10886. The authors would like to thank Dr. Conan R. Weiland for help with NEXAFS measurements. NR 24 TC 4 Z9 4 U1 3 U2 33 PU WILEY-V C H VERLAG GMBH PI WEINHEIM PA BOSCHSTRASSE 12, D-69469 WEINHEIM, GERMANY SN 1614-6832 EI 1614-6840 J9 ADV ENERGY MATER JI Adv. Energy Mater. PD JAN PY 2014 VL 4 IS 2 AR 1300525 DI 10.1002/aenm.201300525 PG 9 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary; Physics, Applied; Physics, Condensed Matter SC Chemistry; Energy & Fuels; Materials Science; Physics GA AB6LQ UT WOS:000331900400002 ER PT J AU Miller, JE McDaniel, AH Allendorf, MD AF Miller, James E. McDaniel, Anthony H. Allendorf, Mark D. TI Considerations in the Design of Materials for Solar-Driven Fuel Production Using Metal-Oxide Thermochemical Cycles SO ADVANCED ENERGY MATERIALS LA English DT Article DE carbon dioxide; ceria; ferrite; gas splitting; hydrogen ID YTTRIA-STABILIZED ZIRCONIA; NONSTOICHIOMETRIC CERIUM DIOXIDE; FEO/FE3O4 REDOX REACTIONS; OXYGEN STORAGE CAPACITY; HYDROGEN-PRODUCTION; SOLID-SOLUTIONS; THERMODYNAMIC ANALYSIS; H-2 GENERATION; THERMAL-ENERGY; IRON-OXIDE AB With demand for energy increasing worldwide and an ever-stronger case building for anthropogenic climate change, the need for carbon-neutral fuels is becoming an imperative. Extensive transportation infrastructure based on liquid hydrocarbon fuels motivates development of processes using solar energy to convert CO2 and H2O to fuel precursors such as synthesis gas. Here, perspectives concerning the use of solar-driven thermochemical cycles using metal oxides to produce fuel precursors are given and, in particular, the important relationship between reactor design and material selection is discussed. Considering both a detailed thermodynamic analysis and factors such as reaction kinetics, volatility, and phase stability, an integrated analytical approach that facilitates material design is presented. These concepts are illustrated using three oxide materials currently receiving considerable attention: metal-substituted ferrites, ceria, and doped cerias. Although none of these materials is ideal, the tradeoffs made in selecting any one of them are clearly indicated, providing a starting point for assessing the feasibility of alternative materials developed in the future. C1 [Miller, James E.] Sandia Natl Labs, Albuquerque, NM 87185 USA. [McDaniel, Anthony H.; Allendorf, Mark D.] Sandia Natl Labs, Livermore, CA 94551 USA. RP Miller, JE (reprint author), Sandia Natl Labs, POB 5800, Albuquerque, NM 87185 USA. EM jemille@sandia.gov; mdallen@sandia.gov FU U.S. Department of Energy Fuel Cell Technologies Program; Laboratory Directed Research and Development Program at Sandia National Laboratories; United States Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX This work was supported by the U.S. Department of Energy Fuel Cell Technologies Program as part of the Production technology development area and by the Laboratory Directed Research and Development Program at Sandia National Laboratories. 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 99 TC 35 Z9 35 U1 2 U2 68 PU WILEY-V C H VERLAG GMBH PI WEINHEIM PA POSTFACH 101161, 69451 WEINHEIM, GERMANY SN 1614-6832 EI 1614-6840 J9 ADV ENERGY MATER JI Adv. Energy Mater. PD JAN PY 2014 VL 4 IS 2 AR 1300469 DI 10.1002/aenm.201300469 PG 19 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary; Physics, Applied; Physics, Condensed Matter SC Chemistry; Energy & Fuels; Materials Science; Physics GA AB6LQ UT WOS:000331900400010 ER PT J AU Hua, X Yu, XY Wang, ZY Yang, L Liu, BW Zhu, ZH Tucker, AE Chrisler, WB Hill, EA Thevuthasan, T Lin, YH Liu, SQ Marshall, MJ AF Hua, Xin Yu, Xiao-Ying Wang, Zhaoying Yang, Li Liu, Bingwen Zhu, Zihua Tucker, Abigail E. Chrisler, William B. Hill, Eric A. Thevuthasan, Theva Lin, Yuehe Liu, Songqin Marshall, Matthew J. TI In situ molecular imaging of a hydrated biofilm in a microfluidic reactor by ToF-SIMS SO ANALYST LA English DT Article ID ION MASS-SPECTROMETRY; SURFACES; SHEWANELLA; INTERFACE; ROLES; CELLS; TIME AB A novel microfluidic reactor for biofilm growth and in situ characterization using time-of-flight secondary ion mass spectrometry (ToF-SIMS) was constructed to enable two-dimensional chemical imaging of hydrated biofilms. We demonstrate the detection of characteristic fatty acid fragments from microfluidic reactor-grown biofilms and illustrate advantages of hydrated-state ToF-SIMS imaging. C1 [Hua, Xin; Yu, Xiao-Ying; Liu, Bingwen] Pacific NW Natl Lab, Richland, WA 99352 USA. [Hua, Xin; Liu, Songqin] Southeast Univ, Sch Chem & Chem Engn, Nanjing 211189, Jiangsu, Peoples R China. [Wang, Zhaoying; Yang, Li; Zhu, Zihua; Thevuthasan, Theva] Pacific NW Natl Lab, WR Wiley Environm Mol Sci Lab, Richland, WA 99352 USA. [Tucker, Abigail E.; Chrisler, William B.; Hill, Eric A.; Marshall, Matthew J.] Pacific NW Natl Lab, Biol Sci Div, Richland, WA 99352 USA. [Lin, Yuehe] Pacific NW Natl Lab, Phys Sci Div, Richland, WA 99352 USA. [Lin, Yuehe] Washington State Univ, Sch Mech & Mat Engn, Pullman, WA 99164 USA. RP Yu, XY (reprint author), Pacific NW Natl Lab, Richland, WA 99352 USA. EM xiaoying.yu@pnnl.gov; matthew.marshall@pnnl.gov RI Zhu, Zihua/K-7652-2012; Yu, Xiao-Ying/L-9385-2013; Liu, Shu/B-7626-2009; Lin, Yuehe/D-9762-2011; Liu, Songqin/O-2680-2013; OI Yu, Xiao-Ying/0000-0002-9861-3109; Lin, Yuehe/0000-0003-3791-7587; Marshall, Matthew J/0000-0002-2402-8003 FU Pacific Northwest National Laboratory (PNNL) Chemical Imaging Initiative-Laboratory Directed Research and Development (CII-LDRD) fund; Use at Facility Funds (UAFF); U.S. DOE Office of Science Early Career Research Award [60385]; DOE [DE-AC05-76RL01830] FX We are grateful to the Pacific Northwest National Laboratory (PNNL) Chemical Imaging Initiative-Laboratory Directed Research and Development (CII-LDRD) fund and the Use at Facility Funds (UAFF) for support in the design and construction of the microfluidic reactor. Biofilm studies were funded by a U.S. DOE Office of Science Early Career Research Award (project no. 60385) and instrument time was provided through an Environmental Molecular Sciences Laboratory (EMSL) Science Themed Proposal. A US patent application (14/050,144) including the particular application of biofilm growth and molecular imaging using the microfluidic flow reactor described in this work was filed. PNNL is operated by Battelle for the DOE under contract DE-AC05-76RL01830. NR 25 TC 8 Z9 8 U1 4 U2 53 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 0003-2654 EI 1364-5528 J9 ANALYST JI Analyst PY 2014 VL 139 IS 7 BP 1609 EP 1613 DI 10.1039/c3an02262e PG 5 WC Chemistry, Analytical SC Chemistry GA AC3MB UT WOS:000332422400003 PM 24571001 ER PT J AU Roscioli, KM Tufariello, JA Zhang, X Li, SX Goetz, GH Cheng, GL Siems, WF Hill, HH AF Roscioli, Kristyn M. Tufariello, Jessica A. Zhang, Xing Li, Shelly X. Goetz, Gilles H. Cheng, Guilong Siems, William F. Hill, Herbert H., Jr. TI Desorption electrospray ionization (DESI) with atmospheric pressure ion mobility spectrometry for drug detection SO ANALYST LA English DT Article ID THIN-LAYER-CHROMATOGRAPHY; TRAP MASS-SPECTROMETRY; PHARMACEUTICAL SAMPLES; RAPID ANALYSIS; ANTIMALARIALS; FORMULATIONS; TABLETS; URINE AB Desorption electrospray ionization (DESI) was coupled to an ambient pressure drift tube ion mobility time-of-flight mass spectrometer (IM-TOFMS) for the direct analysis of active ingredients in pharmaceutical samples. The DESI source was also coupled with a standalone IMS demonstrating potential of portable and inexpensive drug-quality testing platforms. The DESI-IMS required no sample pretreatment as ions were generated directly from tablets and cream formulations. The analysis of a range of over-the-counter and prescription tablet formations was demonstrated for amphetamine (methylphenidate), antidepressant (venlafaxine), barbiturate (Barbituric acid), depressant (alprazolam), narcotic (3-methylmorphine) and sympatholytic (propranolol) drugs. Active ingredients from soft and liquid formulations, such as Icy Hot cream (methyl salicylate) and Nyquil cold medicine (acetaminophen, dextromethorphan, doxylamine) were also detected. Increased sensitivity for selective drug responses was demonstrated through the formation of sodiated adduct ions by introducing small quantities of NaCl into the DESI solvent. Of the drugs and pharmaceuticals tested in this study, 68% (22 total samples) provided a clear ion mobility response at characteristic mobilities either as (M + H)(+), (M - H)(-), or (M + Na)(+) ions. C1 [Roscioli, Kristyn M.] Pacific NW Natl Lab, Richland, WA 99352 USA. [Tufariello, Jessica A.; Zhang, Xing; Siems, William F.; Hill, Herbert H., Jr.] Washington State Univ, Dept Chem, Pullman, WA 99164 USA. [Li, Shelly X.; Goetz, Gilles H.; Cheng, Guilong] Pfizer Inc, Groton Labs, Pfizer Global Res & Dev, Groton, CT 06340 USA. RP Roscioli, KM (reprint author), Pacific NW Natl Lab, Richland, WA 99352 USA. EM kristyn.roscioli@pnnl.gov OI Goetz, Gilles/0000-0001-5316-1586 FU Pfizer Inc. FX We wish to acknowledge Pfizer Inc. for providing the funding for this research. Thank you to Frederick Antosz, Stephen R. Brune and Laurence Philippe for their support and assistance in obtaining funding, thank you to Zhongli Zhang for his contribution to the research proposal and for critical review of the manuscript. NR 26 TC 8 Z9 8 U1 3 U2 49 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 0003-2654 EI 1364-5528 J9 ANALYST JI Analyst PY 2014 VL 139 IS 7 BP 1740 EP 1750 DI 10.1039/c3an02113k PG 11 WC Chemistry, Analytical SC Chemistry GA AC3MB UT WOS:000332422400023 PM 24551872 ER PT J AU Manoharan, VS Kotamarthi, R Feng, Y Cadeddu, MP AF Manoharan, V. S. Kotamarthi, R. Feng, Y. Cadeddu, M. P. TI Increased absorption by coarse aerosol particles over the Gangetic-Himalayan region SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID BROWN CARBON AB Each atmospheric aerosol type has distinctive light-absorption characteristics related to its physical/chemical properties. Climate models treat black carbon as the main light-absorbing component of carbonaceous atmospheric aerosols, while absorption by some organic aerosols is also considered, particularly at ultraviolet wavelengths. Most absorbing aerosols are assumed to be <1 mu m in diameter (sub-micron). Here we present results from a recent field study in India, primarily during the post-monsoon season (October-November), suggesting the presence of absorbing aerosols sized 1-10 mu m. Absorption due to super-micron-sized particles was nearly 30% greater than that due to smaller particles. Periods of increased absorption by larger particles ranged from a week to a month. Radiative forcing calculations under clear-sky conditions show that super-micron particles account for nearly 44% of the total aerosol forcing. The origin of the large aerosols is unknown, but meteorological conditions indicate that they are of local origin. Such economic and habitation conditions exist throughout much of the developing world. Hence, large absorbing particles could be an important component of the regional-scale atmospheric energy balance. C1 [Manoharan, V. S.; Kotamarthi, R.; Feng, Y.; Cadeddu, M. P.] Argonne Natl Lab, Div Environm Sci, Argonne, IL 60439 USA. RP Manoharan, VS (reprint author), Argonne Natl Lab, Div Environm Sci, 9700 S Cass Ave, Argonne, IL 60439 USA. EM vmanoharan@anl.gov FU US Department of Energy, Office of Biological and Environmental Research [DE-AC02-06CH11357] FX This work was supported by the US Department of Energy, Office of Biological and Environmental Research, under contract DE-AC02-06CH11357. NR 20 TC 9 Z9 9 U1 0 U2 14 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 2014 VL 14 IS 3 BP 1159 EP 1165 DI 10.5194/acp-14-1159-2014 PG 7 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA AC2ZN UT WOS:000332384900002 ER PT J AU Williams, IN Riley, WJ Torn, MS Biraud, SC Fischer, ML AF Williams, I. N. Riley, W. J. Torn, M. S. Biraud, S. C. Fischer, M. L. TI Biases in regional carbon budgets from covariation of surface fluxes and weather in transport model inversions SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID ATMOSPHERIC BOUNDARY-LAYER; SOUTHERN GREAT-PLAINS; TALL TOWER; DIOXIDE EXCHANGE; CO2; CYCLE; CONVECTION; REANALYSIS; CHEMISTRY; PROFILES AB Recent advances in atmospheric transport model inversions could significantly reduce uncertainties in land carbon uptake through the assimilation of CO2 concentration measurements at weekly and shorter timescales. The potential of these measurements for reducing biases in estimated land carbon sinks depends on the strength of covariation between surface fluxes and atmospheric transport at these timescales and how well transport models represent this covariation. Daily to seasonal covariation of surface fluxes and atmospheric transport was estimated in observations at the US Southern Great Plains Atmospheric Radiation Measurement Climate Research Facility, and compared to an atmospheric transport model inversion (CarbonTracker). Covariation of transport and surface fluxes was stronger in CarbonTracker than in observations on synoptic (daily to weekly) timescales, with a wet year (2007) having significant covariation compared to a dry year (2006). Differences between observed and CarbonTracker synoptic covariation resulted in a 0.3 ppm CO2 enhancement in boundary layer concentrations during the growing season, and a corresponding enhancement in carbon uptake by 13% of the seasonal cycle amplitude in 2007, as estimated by an offline simplified transport model. This synoptic rectification of surface flux variability was of similar magnitude to the interannual variability in carbon sinks alone, and indicates that interannual variability in the inversions can be affected by biases in simulated synoptic rectifier effects. The most significant covariation of surface fluxes and transport had periodicities of 10 days and greater, suggesting that surface flux inversions would benefit from improved simulations of the effects of soil moisture on boundary layer heights and surface CO2 fluxes. Soil moisture remote sensing could be used along with CO2 concentration measurements to further constrain atmospheric transport model inversions. C1 [Williams, I. N.; Riley, W. J.; Torn, M. S.; Biraud, S. C.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, Berkeley, CA 94720 USA. [Fischer, M. L.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. RP Williams, IN (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, Berkeley, CA 94720 USA. EM inwilliams@lbl.gov RI Williams, Ian/G-3256-2015; Riley, William/D-3345-2015; Torn, Margaret/D-2305-2015; Biraud, Sebastien/M-5267-2013 OI Williams, Ian/0000-0003-0355-1310; Riley, William/0000-0002-4615-2304; Biraud, Sebastien/0000-0001-7697-933X FU Office of Biological and Environmental Research of the US Department of Energy [DE-AC02-05CH11231]; Terrestrial Ecosystem Science Program; ARM Aerial Facility FX This research was 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 Program (ARM), ARM Aerial Facility, and Terrestrial Ecosystem Science Program. The LISA Technology Package Data Analysis (LTPDA) Toolbox (http://www.lisa.aei-hannover.de/ltpda/) was used in developing the stochastic model presented in this paper. NR 53 TC 1 Z9 1 U1 0 U2 17 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 2014 VL 14 IS 3 BP 1571 EP 1585 DI 10.5194/acp-14-1571-2014 PG 15 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA AC2ZN UT WOS:000332384900027 ER PT J AU Bartels-Rausch, T Jacobi, HW Kahan, TF Thomas, JL Thomson, ES Abbatt, JPD Ammann, M Blackford, JR Bluhm, H Boxe, C Domine, F Frey, MM Gladich, I Guzman, MI Heger, D Huthwelker, T Klan, P Kuhs, WF Kuo, MH Maus, S Moussa, SG McNeill, VF Newberg, JT Pettersson, JBC Roeselova, M Sodeau, JR AF Bartels-Rausch, T. Jacobi, H. -W. Kahan, T. F. Thomas, J. L. Thomson, E. S. Abbatt, J. P. D. Ammann, M. Blackford, J. R. Bluhm, H. Boxe, C. Domine, F. Frey, M. M. Gladich, I. Guzman, M. I. Heger, D. Huthwelker, Th. Klan, P. Kuhs, W. F. Kuo, M. H. Maus, S. Moussa, S. G. McNeill, V. F. Newberg, J. T. Pettersson, J. B. C. Roeselova, M. Sodeau, J. R. TI A review of air-ice chemical and physical interactions (AICI): liquids, quasi-liquids, and solids in snow SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Review ID ATMOSPHERIC TRACE GASES; SUPERCOOLED AQUEOUS-SOLUTIONS; SCANNING-ELECTRON-MICROSCOPY; OZONE DEPLETION EVENTS; DIFFERENT WATER MODELS; TO-FIRN TRANSFER; MOLECULAR-DYNAMICS; HYDROGEN-PEROXIDE; HEXAGONAL ICE; NITRIC-ACID AB Snow in the environment acts as a host to rich chemistry and provides a matrix for physical exchange of contaminants within the ecosystem. The goal of this review is to summarise the current state of knowledge of physical processes and chemical reactivity in surface snow with relevance to polar regions. It focuses on a description of impurities in distinct compartments present in surface snow, such as snow crystals, grain boundaries, crystal surfaces, and liquid parts. It emphasises the microscopic description of the ice surface and its link with the environment. Distinct differences between the disordered air-ice interface, often termed quasi-liquid layer, and a liquid phase are highlighted. The reactivity in these different compartments of surface snow is discussed using many experimental studies, simulations, and selected snow models from the molecular to the macro-scale. Although new experimental techniques have extended our knowledge of the surface properties of ice and their impact on some single reactions and processes, others occurring on, at or within snow grains remain unquantified. The presence of liquid or liquid-like compartments either due to the formation of brine or disorder at surfaces of snow crystals below the freezing point may strongly modify reaction rates. Therefore, future experiments should include a detailed characterisation of the surface properties of the ice matrices. A further point that remains largely unresolved is the distribution of impurities between the different domains of the condensed phase inside the snowpack, i.e. in the bulk solid, in liquid at the surface or trapped in confined pockets within or between grains, or at the surface. While surface-sensitive laboratory techniques may in the future help to resolve this point for equilibrium conditions, additional uncertainty for the environmental snowpack may be caused by the highly dynamic nature of the snowpack due to the fast metamorphism occurring under certain environmental conditions. Due to these gaps in knowledge the first snow chemistry models have attempted to reproduce certain processes like the long-term incorporation of volatile compounds in snow and firn or the release of reactive species from the snowpack. Although so far none of the models offers a coupled approach of physical and chemical processes or a detailed representation of the different compartments, they have successfully been used to reproduce some field experiments. A fully coupled snow chemistry and physics model remains to be developed. C1 [Bartels-Rausch, T.; Ammann, M.] Paul Scherrer Inst, Lab Radio & Environm Chem, CH-5232 Villigen, Switzerland. [Jacobi, H. -W.] CNRS, Lab Glaciol & Geophys Environnm UMR5183, F-38041 Grenoble, France. [Jacobi, H. -W.] Univ Grenoble Alpes, LGGE UMR5183, F-38041 Grenoble, France. [Kahan, T. F.] Syracuse Univ, Dept Chem, Syracuse, NY USA. [Thomas, J. L.] Univ Paris 06, CNRS INSU, LATMOS IPSL, UMR8190, Paris, France. [Thomas, J. L.] Univ Calif Los Angeles, Dept Atmospher & Ocean Sci, Los Angeles, CA 90095 USA. [Thomson, E. S.; Pettersson, J. B. C.] Univ Gothenburg, Dept Chem & Mol Biol Atmospher Sci, S-41296 Gothenburg, Sweden. [Abbatt, J. P. D.] Univ Toronto, Dept Chem, Toronto, ON M5S 3H6, Canada. [Blackford, J. R.] Univ Edinburgh, Sch Engn, Inst Mat & Proc, Edinburgh EH9 3JL, Midlothian, Scotland. [Bluhm, H.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. [Boxe, C.] CUNY, Medgar Evers Coll, Dept Chem & Environm Sci, Brooklyn, NY 11235 USA. [Boxe, C.] CUNY, Grad Ctr, Dept Chem, Dept Earth & Environm Sci, New York, NY 10016 USA. [Domine, F.] Univ Laval, Takuvik Joint Int Lab, Quebec City, PQ G1V 0A6, Canada. [Domine, F.] CNRS, Quebec City, PQ G1V 0A6, Canada. [Domine, F.] Dept Chem, Quebec City, PQ G1V 0A6, Canada. [Frey, M. M.] British Antarctic Survey, Nat Environm Res Council, Cambridge CB3 0ET, England. [Gladich, I.] Acad Sci Czech Republic, Inst Organ Chem & Biochem, Prague 16610 6, Czech Republic. [Guzman, M. I.] Univ Kentucky, Dept Chem, Lexington, KY 40506 USA. [Heger, D.; Klan, P.] Masaryk Univ, Fac Sci, Dept Chem, Brno 62500, Czech Republic. [Heger, D.; Klan, P.] Masaryk Univ, Fac Sci, RECETOX, Brno 62500, Czech Republic. [Huthwelker, Th.] Paul Scherrer Inst, Swiss Light Source, CH-5232 Villigen, Switzerland. [Kuhs, W. F.] Univ Gottingen, GZG Abt Kristallographie, D-37077 Gottingen, Germany. [Kuo, M. H.; Moussa, S. G.; McNeill, V. F.] Columbia Univ, Dept Chem Engn, New York, NY USA. [Maus, S.] Univ Bergen, Inst Geophys, N-5007 Bergen, Norway. [Newberg, J. T.] Univ Delaware, Dept Chem & Biochem, Newark, DE 19716 USA. [Sodeau, J. R.] Univ Coll Cork, Dept Chem, Cork, Ireland. [Sodeau, J. R.] Univ Coll Cork, Environm Res Inst, Cork, Ireland. RP Bartels-Rausch, T (reprint author), Paul Scherrer Inst, Lab Radio & Environm Chem, CH-5232 Villigen, Switzerland. EM thorsten.bartels-rausch@psi.ch RI Klan, Petr/H-1189-2012; Frey, Markus/G-1756-2012; Thomson, Erik/C-6187-2014; Heger, Dominik/H-9934-2012; Guzman, Marcelo/C-5966-2008; Bartels-Rausch, Thorsten/A-7651-2008; Pettersson, Jan/D-2250-2009; Ammann, Markus/E-4576-2011 OI Klan, Petr/0000-0001-6287-2742; Frey, Markus/0000-0003-0535-0416; Heger, Dominik/0000-0002-6881-8699; Guzman, Marcelo/0000-0002-6730-7766; Bartels-Rausch, Thorsten/0000-0002-7548-2572; Ammann, Markus/0000-0001-5922-9000 FU IGAC; Columbia University School of Engineering and Applied Sciences; Swiss National Science Foundation [121857, 125179, 140400, 149629]; LEFE-CHAT program of INSU-CNRS; NSF [ATM-0845043, ANT-1019347]; Czech Science Foundation [P208/10/1724, P503/10/0947]; project CETOCOEN [CZ.1.05/2.1.00/01.0001]; U.S. National Science Foundation [CHE-1255290]; Division of Chemical Sciences, Geosciences, and Biosciences of the U.S. Department of Energy [DE-AC02-05CH11231]; European Regional Development Fund; [RVO 61388963] FX This review was initiated and planned during the 3rd Workshop on Air-Ice Chemical Interactions held in June 2011, in New York, NY. The workshop was sponsored in part by IGAC and the Columbia University School of Engineering and Applied Sciences. T. Bartels-Rausch and M. Ammann appreciate support by the Swiss National Science Foundation (grants 121857, 125179, 140400, and 149629) and valuable input to this review by Sepp Schreiber. H.-W. Jacobi acknowledges support by the LEFE-CHAT program of INSU-CNRS. E. S. Thomson and J. B. C. Pettersson benefit from the scientific support of the Swedish Research Council and the Nordic top-level research initiative CRAICC. M. H. Kuo, V. F. McNeill, and S. G. Moussa acknowledge a NSF CAREER award for V. F. McNeill (ATM-0845043). M. Roeselova acknowledges support from the Czech Science Foundation (grant P208/10/1724) and RVO 61388963. P. Klan and D. Heger appreciate support by the Czech Science Foundation (P503/10/0947), and the project CETOCOEN (CZ.1.05/2.1.00/01.0001) granted by the European Regional Development Fund. M. I. Guzman thanks the U.S. National Science Foundation for a CAREER award (CHE-1255290). F. Domine thanks the French Polar Institute (IPEV) for continuous support. H. Bluhm acknowledges support from the Director, Office of Science, Office of Basic Energy Sciences, and by the Division of Chemical Sciences, Geosciences, and Biosciences of the U.S. Department of Energy under Contract Nr. DE-AC02-05CH11231. J. T. Newberg acknowledges support from an NSF Postdoctoral Fellowship (ANT-1019347). NR 354 TC 45 Z9 46 U1 12 U2 187 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 2014 VL 14 IS 3 BP 1587 EP 1633 DI 10.5194/acp-14-1587-2014 PG 47 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA AC2ZN UT WOS:000332384900028 ER PT J AU Gan, CM Pleim, J Mathur, R Hogrefe, C Long, CN Xing, J Roselle, S Wei, C AF Gan, C. -M. Pleim, J. Mathur, R. Hogrefe, C. Long, C. N. Xing, J. Roselle, S. Wei, C. TI Assessment of the effect of air pollution controls on trends in shortwave radiation over the United States from 1995 through 2010 from multiple observation networks SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID SURFACE SOLAR-RADIATION; BUDGET NETWORK; OPTICAL DEPTH; AEROSOL; RADIOMETER; EMISSIONS; SURFRAD AB Long-term data sets of all-sky and clear-sky downwelling shortwave (SW) radiation, cloud cover fraction, and aerosol optical depth (AOD) were analyzed together with surface concentrations from several networks (e. g., Surface Radiation Budget Network (SURFRAD), Clean Air Status and Trend Network (CASTNET), Interagency Monitoring of Protection Visual Environments (IMPROVE) and Atmospheric Radiation Measurement (ARM)) in the United States (US). Seven states with varying climatology were selected to better understand the effects of aerosols and clouds on SW radiation. This analysis aims to assess the effects of reductions in anthropogenic aerosol burden resulting from substantial reductions in emissions of sulfur dioxide (SO2) and nitrogen oxides (NOx) over the past 16 yr across the US, based on trends in SW radiation. The SO2 and NOx emission data show decreasing trends from 1995 to 2010, which indirectly validates the effects of the Clean Air Act (CAA) in the US. Meanwhile, the total column AOD and surface total PM2.5 observations also show decreasing trends in the eastern US but slightly increasing trends in the western US. Moreover, measured surface concentrations of several other pollutants (i.e., SO2, SO4 and NOx) have similar behavior to AOD and total PM2.5. Analysis of the observed data shows strong increasing trends in all-sky downwelling SW radiation with decreasing trends in cloud cover. However, since observations of both all-sky direct and diffuse SW radiation show increasing trends, there may be other factors contributing to the radiation trends in addition to the decreasing trends in overall cloud cover. To investigate the role of direct radiative effects of aerosols, clear-sky downwelling radiation is analyzed so that cloud effects are eliminated. However, similar increasing trends in clear-sky total and diffuse SW radiation are observed. While significantly decreasing trends in AOD and surface PM2.5 concentrations along with increasing SW radiation (both all-sky and clear-sky) in the eastern US during 1995-2010 imply the occurrence of direct aerosol mediated "brightening", the increasing trends of both all-sky and clear-sky diffuse SW radiation contradicts this conclusion since diffuse radiation would be expected to decrease as aerosols direct effects decrease and cloud cover decreases. After investigating several confounding factors, the increasing trend in clear-sky diffuse SW may be due to more high-level cirrus from increasing air traffic over the US. The clear-sky radiation observations in the western US also show indications of "brightening" even though the AOD, PM2.5 and surface concentration do not vary drastically. This outcome was not unexpected because the CAA controls were mainly aimed at reducing air pollutant emissions in the eastern US and air pollutant levels in the western US were much lower at the onset. This suggests other factors affect the "brightening" especially in the western US. C1 [Gan, C. -M.; Pleim, J.; Mathur, R.; Hogrefe, C.; Xing, J.; Roselle, S.; Wei, C.] US EPA, Atmospher Modeling & Anal Div, Natl Exposure Res Lab, Res Triangle Pk, NC 27711 USA. [Long, C. N.] Pacific NW Natl Lab, Climate Phys Grp, Richland, WA 99352 USA. RP Gan, CM (reprint author), US EPA, Atmospher Modeling & Anal Div, Natl Exposure Res Lab, Res Triangle Pk, Res Triangle Pk, NC 27711 USA. EM chuenmeei@gmail.com RI xing, jia/O-1784-2014; wei, chao/E-4379-2011; Pleim, Jonathan Pleim/C-1331-2017 OI Pleim, Jonathan Pleim/0000-0001-6190-6082 FU US Department of Energy [IA DE-SC0003782]; US Environmental Protection Agency [IA RW-89-9233260]; Climate Change Research Division of the US Department of Energy as part of the Atmospheric System Research (ASR) Program FX This research was performed while C.-M. Gan held a National Research Council Research Associateship Award at US EPA. The research presented in this study was supported through an interagency agreement between the US Department of Energy (funding IA DE-SC0003782) and the US Environmental Protection Agency (funding IA RW-89-9233260). It has been subject to the US EPA's administrative review and approved for publication. The author also would like thank J. Augustine from NOAA-SURFRAD for his support and assistance in obtaining the SURFRAD data. C. N. Long acknowledges the support of the Climate Change Research Division of the US Department of Energy as part of the Atmospheric System Research (ASR) Program. We also appreciate the comments of three reviewers and the editor, which have significantly improved this paper. NR 42 TC 16 Z9 16 U1 0 U2 21 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 2014 VL 14 IS 3 BP 1701 EP 1715 DI 10.5194/acp-14-1701-2014 PG 15 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA AC2ZN UT WOS:000332384900034 ER PT J AU Jin, SE Jin, HE Hong, SS AF Jin, Su-Eon Jin, Hyo-Eon Hong, Soon-Sun TI Targeted Delivery System of Nanobiomaterials in Anticancer Therapy: From Cells to Clinics SO BIOMED RESEARCH INTERNATIONAL LA English DT Review ID IRON-OXIDE NANOPARTICLES; INCORPORATING MICELLAR NANOPARTICLE; PLGA-BASED NANOPARTICLES; TOBACCO-MOSAIC-VIRUS; IN-VIVO EVALUATION; DRUG-DELIVERY; GENE DELIVERY; PHASE-I; CARBON NANOTUBES; PROSTATE-CANCER AB Targeted delivery systems of nanobiomaterials are necessary to be developed for the diagnosis and treatment of cancer. Nanobiomaterials can be engineered to recognize cancer-specific receptors at the cellular levels and to deliver anticancer drugs into the diseased sites. In particular, nanobiomaterial-based nanocarriers, so-called nanoplatforms, are the design of the targeted delivery systems such as liposomes, polymeric nanoparticles/micelles, nanoconjugates, norganic materials, carbon-based nanobiomaterials, and bioinspired phage system, which are based on the nanosize of 1-100 nmin diameter. In this review, the design and the application of these nanoplatforms are discussed at the cellular levels as well as in the clinics. We believe that this review can offer recent advances in the targeted delivery systems of nanobiomaterials regarding in vitro and in vivo applications and the translation of nanobiomaterials to nanomedicine in anticancer therapy. C1 [Jin, Su-Eon; Hong, Soon-Sun] Inha Univ, Coll Med, Dept Drug Dev, Inchon 400712, South Korea. [Jin, Hyo-Eon] Univ Calif Berkeley, Dept Bioengn, Berkeley, CA 94720 USA. [Jin, Hyo-Eon] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA 94720 USA. RP Hong, SS (reprint author), Inha Univ, Coll Med, Dept Drug Dev, 3 Ga, Inchon 400712, South Korea. EM hongs@inha.ac.kr FU Korean Health Technology R&D Project, Ministry of Health and Welfare [A120266]; National Research Foundation of Korea (NRF); Ministry of Education, Science and Technology [NRF-2012-0002988, 2012R1A2A2A01045602]; Inha University FX This work is supported by Korean Health Technology R&D Project (A120266), Ministry of Health and Welfare, the National Research Foundation of Korea (NRF) funded by the Ministry of Education, Science and Technology (NRF-2012-0002988, 2012R1A2A2A01045602), and Inha University grant. NR 206 TC 21 Z9 21 U1 6 U2 81 PU HINDAWI LTD PI LONDON PA ADAM HOUSE, 3RD FLR, 1 FITZROY SQ, LONDON, WIT 5HE, ENGLAND SN 2314-6133 EI 2314-6141 J9 BIOMED RES INT JI Biomed Res. Int. PY 2014 AR 814208 DI 10.1155/2014/814208 PG 23 WC Biotechnology & Applied Microbiology; Medicine, Research & Experimental SC Biotechnology & Applied Microbiology; Research & Experimental Medicine GA AC1YI UT WOS:000332293500001 ER PT J AU Veith, GM Baggetto, L Sacci, RL Unocic, RR Tenhaeff, WE Browning, JF AF Veith, Gabriel M. Baggetto, Loic Sacci, Robert L. Unocic, Raymond R. Tenhaeff, Wyatt E. Browning, James F. TI Direct measurement of the chemical reactivity of silicon electrodes with LiPF6-based battery electrolytes SO CHEMICAL COMMUNICATIONS LA English DT Article ID LITHIUM-ION BATTERIES; PHOTOELECTRON-SPECTROSCOPY; NEUTRON REFLECTOMETRY; INTERPHASE; REFLECTION; LITHIATION; INTERFACES; LIQUID; ANODES; MODEL AB We report the first direct measurement of the extent of the spontaneous non-electrochemically driven reaction between a lithium ion battery electrode surface ( Si) and a liquid electrolyte (1.2 M LiPF6-3:7 wt% ethylene carbonate : dimethyl carbonate). This layer is estimated to be 35 angstrom thick with a SLD of similar to 4 x 10(-6) angstrom(-2) and likely originates from the consumption of the silicon surface. C1 [Veith, Gabriel M.; Baggetto, Loic; Sacci, Robert L.] Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. [Unocic, Raymond R.] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Natl Lab, Oak Ridge, TN 37831 USA. [Tenhaeff, Wyatt E.] Univ Rochester, Dept Chem Engn, Rochester, NY 14627 USA. [Browning, James F.] Oak Ridge Natl Lab, Neutron Sci Directorate, Chem & Engn Mat Div, Oak Ridge, TN 37831 USA. RP Veith, GM (reprint author), Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. EM veithgm@ornl.gov; browningjf@ornl.gov RI Browning, James/C-9841-2016; Baggetto, Loic/D-5542-2017; OI Browning, James/0000-0001-8379-259X; Baggetto, Loic/0000-0002-9029-2363; Unocic, Raymond/0000-0002-1777-8228 FU Materials Sciences and Engineering Division, Office of Basic Energy Sciences, U.S. Department of Energy under UT-Battelle, LLC; Fluid Interface Reactions, Structures, and Transport (FIRST) Center; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences; Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy FX This research was supported by the Materials Sciences and Engineering Division, Office of Basic Energy Sciences, U.S. Department of Energy under contract with UT-Battelle, LLC (LB, GMV) and 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 (RLS, RRU - PAS, SEM). Neutron reflectometry measurements were carried out on the Liquids Reflectometer at the Spallation Neutron Source which is sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy. A portion of the research was performed by Oak Ridge National Laboratory's Center for Nanophase Materials Science (CNMS) (SEM), which is sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy. NR 29 TC 11 Z9 11 U1 5 U2 71 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 2014 VL 50 IS 23 BP 3081 EP 3084 DI 10.1039/c3cc49269a PG 4 WC Chemistry, Multidisciplinary SC Chemistry GA AB8GB UT WOS:000332027100030 PM 24513965 ER EF