FN Thomson Reuters Web of Science™ VR 1.0 PT J AU Hu, SC Shiue, A Chuang, HC Xu, TF AF Hu, Shih-Cheng Shiue, Angus Chuang, Hsien-Chou Xu, Tengfang TI Life cycle assessment of high-technology buildings: Energy consumption and associated environmental impacts of wafer fabrication plants SO ENERGY AND BUILDINGS LA English DT Article DE High-technology buildings; Life cycle assessment; Wafer fabrication; DRAM; Environmental impact; Energy use ID SEMICONDUCTOR INDUSTRY; PERFORMANCE; MINIENVIRONMENTS; MICROCHIP AB Effective environmental control and energy efficiency in high-technology buildings have become an important subject of investigations across continents since the last decades. This study aims to quantify energy use and associated environmental impact of four high-technology buildings for wafer fabrication in a subtropical region of Asia using life cycle assessment techniques. Wafer fabrication process and its energy and steam consumption were associated with "summer smog," "heavy metals," and "acidification potential" on the environment. All fabs used natural gas, diesel oil, and steam, which together accounted for about 5% of the total energy consumption. Two metrics - production efficiency index (PEI) and the electricity utilization index (EUI) were used to characterize and normalize environmental impact of each of the four high-technology buildings within which dynamic random access memory (DRAM) wafers were manufactured. The GHG emissions in PEI and EUI have declined from 601 g to 367 g (by 39%) and from 28.9 g to 13.7 g (by 53%), respectively, between 1999 and 2007. Energy intensity per unit area of wafer production has increased from 195 to 268 associated with a 37% increase in emission rate of CO2-equivalent greenhouse gas (GHG) from 195 kg to 268 kg (by 73 kg) per unit area of wafers produced. (c) 2012 Elsevier B.V. All rights reserved. C1 [Hu, Shih-Cheng; Shiue, Angus; Chuang, Hsien-Chou] Natl Taipei Univ Technol, Dept Energy & Refrigerating Air Conditioning Engn, Taipei, Taiwan. [Xu, Tengfang] Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Int Energy Studies Grp, Berkeley, CA USA. RP Shiue, A (reprint author), 1,Sec 3,Chung Hsiao E Rd, Taipei 10608, Taiwan. EM angusshiue@gmail.com NR 22 TC 2 Z9 2 U1 2 U2 26 PU ELSEVIER SCIENCE SA PI LAUSANNE PA PO BOX 564, 1001 LAUSANNE, SWITZERLAND SN 0378-7788 EI 1872-6178 J9 ENERG BUILDINGS JI Energy Build. PD JAN PY 2013 VL 56 BP 126 EP 133 DI 10.1016/j.enbuild.2012.09.023 PG 8 WC Construction & Building Technology; Energy & Fuels; Engineering, Civil SC Construction & Building Technology; Energy & Fuels; Engineering GA 082FU UT WOS:000314378500015 ER PT J AU Ban-Weiss, G Wray, C Delp, W Ly, P Akbari, H Levinson, R AF Ban-Weiss, George Wray, Craig Delp, Woody Ly, Peter Akbari, Hashem Levinson, Ronnen TI Electricity production and cooling energy savings from installation of a building-integrated photovoltaic roof on an office building SO ENERGY AND BUILDINGS LA English DT Article DE Photovoltaic; Building integrated photovoltaic (BIPV); Building energy; White roof; Reflective roof; Building heat transfer ID AIR-QUALITY; SOLAR REFLECTANCE; ALBEDO; IMPACTS AB Reflective roofs can reduce demand for air conditioning and warming of the atmosphere. Roofs can also host photovoltaic (PV) modules that convert sunlight to electricity. In this study we assess the effects of installing a building integrated photovoltaic (BIPV) roof on an office building in Yuma, AZ. The system consists of thin film PV laminated to a white membrane, which lies above a layer of insulation. The solar absorptance of the roof decreased to 0.38 from 0.75 after installation of the BIPV, lowering summertime daily mean roof upper surface temperatures by about 5 degrees C. Summertime daily heat influx through the roof deck fell to +/- 0.1 kWh/m(2) from 0.3-1.0 kWh/m(2). However, summertime daily heat flux from the ventilated attic into the conditioned space was minimally affected by the BIPV, suggesting that the roof was decoupled from the conditioned space. Daily PV energy production was about 25% of building electrical energy use in the summer. For this building the primary benefit of the BIPV appeared to be its capacity to generate electricity and not its ability to reduce heat flows into the building. Building energy simulations were used to estimate the cooling energy savings and heating energy penalties for more typical buildings. (c) 2012 Elsevier B.V. All rights reserved. C1 [Ban-Weiss, George; Wray, Craig; Delp, Woody; Levinson, Ronnen] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. [Ly, Peter] USN, Naval Facil Engn & Expeditionary Ctr, Port Hueneme, CA 93043 USA. [Akbari, Hashem] Concordia Univ, Dept Bldg Civil & Environm Engn, Montreal, PQ, Canada. RP Ban-Weiss, G (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, 1 Cyclotron Rd, Berkeley, CA 94720 USA. EM georgebw@berkeley.edu OI Ban-Weiss, George/0000-0001-8211-2628 FU Department of Defense Environmental Security Technology Certification Program [SI-200813]; Energy Efficiency and Renewable Energy, Office of Building Technology, State, and Community Programs, of the U.S. Department of Energy [DE-AC02-05CH11231] FX This work was supported by the Department of Defense Environmental Security Technology Certification Program under Project No. SI-200813. It was also supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Building Technology, State, and Community Programs, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. We wish to thank Luke O'Dea of Unisolar for technical information on the PV; Michael Boyd and Ronald Durfey of MCAS Yuma for technical assistance; and Jordan Woods of Lawrence Berkeley National Laboratory. NR 25 TC 13 Z9 13 U1 1 U2 28 PU ELSEVIER SCIENCE SA PI LAUSANNE PA PO BOX 564, 1001 LAUSANNE, SWITZERLAND SN 0378-7788 J9 ENERG BUILDINGS JI Energy Build. PD JAN PY 2013 VL 56 BP 210 EP 220 DI 10.1016/j.enbuild.2012.06.032 PG 11 WC Construction & Building Technology; Energy & Fuels; Engineering, Civil SC Construction & Building Technology; Energy & Fuels; Engineering GA 082FU UT WOS:000314378500024 ER PT J AU Jo, S Jiang, W Lee, HS Roux, B Im, W AF Jo, Sunhwan Jiang, Wei Lee, Hui Sun Roux, Benoit Im, Wonpil TI CHARMM-GUI Ligand Binder for Absolute Binding Free Energy Calculations and Its Application SO JOURNAL OF CHEMICAL INFORMATION AND MODELING LA English DT Article ID HISTOGRAM ANALYSIS METHOD; DRUG DESIGN; COMPUTER-SIMULATIONS; T4 LYSOZYME; MOLECULAR-MECHANICS; FORCE-FIELD; DYNAMICS; SOLVENT; COMPUTATION; AFFINITIES AB Advanced free energy perturbation molecular dynamics (FEP/MD) simulation methods are available to accurately calculate absolute binding free energies of protein ligand complexes. However, these methods rely on several sophisticated command scripts implementing various biasing energy restraints to enhance the convergence of the FEP/MD calculations, which must all be handled properly to yield correct results. Here, we present a user-friendly Web interface, CHARMM-GUI Ligand Binder (http://www.charmm-gui.org/input/gbinding), to provide standardized CHARMM input files for calculations of absolute binding free energies using the FEP/MD simulations. A number of features are implemented to conveniently set up the FEP/MD simulations in highly customizable manners, thereby permitting an accelerated throughput of this important class of computations while decreasing the possibility of human errors. The interface and a series of input files generated by the interface are tested with illustrative calculations of absolute binding free energies of three nonpolar aromatic ligands to the L99A mutant of 14 lysozyme and three FK506-related ligands to FKBP12. Statistical errors within individual calculations are found to be small (similar to 1 kcal/mol), and the calculated binding free energies generally agree well with the experimental measurements and the previous computational studies (within similar to 2 kcal/mol). Therefore, CHARMM-GUI Ligand Binder provides a convenient and reliable way to set up the ligand binding free energy calculations and can be applicable to pharmaceutically important protein-ligand systems. C1 [Jo, Sunhwan; Lee, Hui Sun; Im, Wonpil] Univ Kansas, Dept Mol Biosci, Lawrence, KS 66047 USA. [Jo, Sunhwan; Lee, Hui Sun; Im, Wonpil] Univ Kansas, Ctr Bioinformat, Lawrence, KS 66047 USA. [Jiang, Wei] Argonne Natl Lab, Leadership Comp Facil, Argonne, IL 60439 USA. [Roux, Benoit] Gordon Ctr Integrat Sci, Dept Biochem & Mol Biol, Chicago, IL 60637 USA. [Roux, Benoit] Argonne Natl Lab, Biosci Div, Argonne, IL 60439 USA. RP Roux, B (reprint author), Gordon Ctr Integrat Sci, Dept Biochem & Mol Biol, 929 E 57th St, Chicago, IL 60637 USA. EM roux@uchicago.edu; wonpil@ku.edu FU University of Kansas General Research Fund [2301388-003]; NSF [ABI-1145987, MCB-0920261]; NIH [U54 GM087519-01]; TeraGrid/XSEDE resources [TG-MCB070009] FX This work was supported by the University of Kansas General Research Fund allocation #2301388-003, NSF ABI-1145987, NIH U54 GM087519-01, TeraGrid/XSEDE resources (TG-MCB070009) (to W.I.), and NSF MCB-0920261 (to B.R.). NR 42 TC 14 Z9 14 U1 2 U2 29 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 1549-9596 EI 1549-960X J9 J CHEM INF MODEL JI J. Chem Inf. Model. PD JAN PY 2013 VL 53 IS 1 BP 267 EP 277 DI 10.1021/ci300505n PG 11 WC Chemistry, Medicinal; Chemistry, Multidisciplinary; Computer Science, Information Systems; Computer Science, Interdisciplinary Applications SC Pharmacology & Pharmacy; Chemistry; Computer Science GA 081OV UT WOS:000314332400023 PM 23205773 ER PT J AU Reedy, ED Cox, JV AF Reedy, E. D., Jr. Cox, J. V. TI Hierarchical Analysis of the Release Step in a Nanofabrication Process Using an Adhesion/Atomistic Friction Surface Interaction Model SO JOURNAL OF ENGINEERING MATERIALS AND TECHNOLOGY-TRANSACTIONS OF THE ASME LA English DT Article ID NANOIMPRINT LITHOGRAPHY; TEMPERATURE; FABRICATION; FRACTURE; GROWTH AB Finite element analysis techniques were used to study the release step in a nanofabrication process. These calculations employed a novel adhesion/atomistic friction surface interaction model to define how the glassy polymer interacts with the hard mold. This model is applicable to solids that interact via relatively weak, van der Waals forces and is applicable to intentionally weakened interfaces (e.g., when a mold release is used). The goal of this effort is to simulate the entire separation process. The release step was studied by performing unit cell calculations for a pattern composed of identical, parallel channels. The interface between the mold and the glassy polymer did not unzip in a continuous, quasi-static manner in these simulations. Instead, there was a complex failure sequence that included multiple dynamic separations and arrest events as well as adhesive reattachment. The sensitivity of the release process to interface and bulk material properties, polymer shrinkage, and feature geometry was then quantified by examining variations from a baseline configuration. Finally, the feasibility of a hierarchical analysis that represents the nanometer-scale pattern by a pattern traction-separation (T-U) relationship, which is defined by a unit cell analysis, was demonstrated. [DOI: 10.1115/1.4023042] C1 [Reedy, E. D., Jr.; Cox, J. V.] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Reedy, ED (reprint author), Sandia Natl Labs, POB 5800, Albuquerque, NM 87185 USA. EM edreedy@sandia.gov FU Laboratory Directed Research and Development 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 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 No. DE-AC04-94AL85000. NR 19 TC 1 Z9 1 U1 0 U2 9 PU ASME PI NEW YORK PA TWO PARK AVE, NEW YORK, NY 10016-5990 USA SN 0094-4289 J9 J ENG MATER-T ASME JI J. Eng. Mater. Technol.-Trans. ASME PD JAN PY 2013 VL 135 IS 1 AR 011008 DI 10.1115/1.4023042 PG 9 WC Engineering, Mechanical; Materials Science, Multidisciplinary SC Engineering; Materials Science GA 087FN UT WOS:000314746800008 ER PT J AU Fulvio, PF Hillesheim, PC Bauer, JC Mahurin, SM Dai, S AF Fulvio, Pasquale Fernando Hillesheim, Patrick Christopher Bauer, John Christopher Mahurin, Shannon Mark Dai, Sheng TI Magadiite templated high surface area graphene-type carbons from metal-halide based ionic liquids SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID GRAPHITE OXIDE; EXFOLIATION; PRECURSORS; NANOSHEETS AB Dispersible graphene-type carbon powders were prepared with metal halide-ionic liquids as the carbon source and Magadiite, a layered sodium silicate, as the template. The metal halide has a major impact on the graphene yield, ordering of the carbon lattice, and adsorption properties. C1 [Fulvio, Pasquale Fernando; Hillesheim, Patrick Christopher; Bauer, John Christopher; Mahurin, Shannon Mark; Dai, Sheng] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. [Dai, Sheng] Univ Tennessee, Dept Chem, Knoxville, TN 37996 USA. RP Fulvio, PF (reprint author), Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. EM fulviopf@ornl.gov; dais@ornl.gov RI Bauer, John/J-3150-2012; Fulvio, Pasquale/B-2968-2014; Dai, Sheng/K-8411-2015 OI Fulvio, Pasquale/0000-0001-7580-727X; Dai, Sheng/0000-0002-8046-3931 FU Fluid Interface Reactions, Structures and Transport (FIRST) Center; US Department of Energy, Office of Science, Office of Basic Energy Sciences FX This work was supported as part of the Fluid Interface Reactions, Structures and Transport (FIRST) Center, an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Office of Basic Energy Sciences. NR 29 TC 7 Z9 7 U1 0 U2 48 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7488 J9 J MATER CHEM A JI J. Mater. Chem. A PY 2013 VL 1 IS 1 BP 59 EP 62 DI 10.1039/c2ta00634k PG 4 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA 085EY UT WOS:000314598400008 ER PT J AU Cappillino, PJ Hattar, KM Clark, BG Hartnett, RJ Stavila, V Hekmaty, MA Jacobs, BW Robinson, DB AF Cappillino, Patrick J. Hattar, Khalid M. Clark, Blythe G. Hartnett, Ryan J. Stavila, Vitalie Hekmaty, Michelle A. Jacobs, Benjamin W. Robinson, David B. TI Synthesis of mesoporous palladium with tunable porosity and demonstration of its thermal stability by in situ heating and environmental transmission electron microscopy SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID LYOTROPIC LIQUID-CRYSTALS; HYDROGEN-STORAGE; CATALYZED DEPOLYMERIZATION; DIBLOCK COPOLYMERS; NANOPARTICLE; PD; SURFACTANT; PLATINUM; ALLOY; MORPHOLOGIES AB Palladium and its alloys have high-value applications as materials for high-performance hydrogen storage, chromatographic separation of hydrogen isotopes, electrocatalysis and catalysis. These materials can be formed by chemical or electrochemical reduction in a lyotropic liquid crystalline template that constrains their growth on the nanometer scale. This approach works for a variety of metals, but Pd presents special challenges due to the autocatalytic nature of its growth, which can disrupt the template structure, resulting in disordered pores. Presented herein is a scaleable synthesis that overcomes these challenges, yielding mesoporous Pd powder having pore diameters of 7 or 13 nm. Pore size control is effected by varying the size of the molecular template, polystyrene-block-polyethylene oxide. We have used heated-stage TEM for in situ observation of the materials in vacuum and in the presence of H-2 gas, demonstrating that both pore diameter and the chemical state of the surface play important roles in determining thermal stability. Improved stability compared to previously reported examples facilitates preparation of scalable quantities of regularly mesoporous Pd that retains porosity at the elevated temperatures required for applications in hydrogen charge/discharge and catalysis. C1 [Cappillino, Patrick J.; Hartnett, Ryan J.; Stavila, Vitalie; Hekmaty, Michelle A.; Robinson, David B.] Sandia Natl Labs, Livermore, CA USA. [Hattar, Khalid M.; Clark, Blythe G.] Sandia Natl Labs, Albuquerque, NM 87185 USA. [Jacobs, Benjamin W.] Protochips Inc, Raleigh, NC USA. RP Cappillino, PJ (reprint author), Sandia Natl Labs, POB 969,Mail Stop 9291, Livermore, CA USA. EM drobins@sandia.gov RI Stavila, Vitalie/B-6464-2008 OI Stavila, Vitalie/0000-0003-0981-0432 FU U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX Sandia National Laboratories is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000. NR 43 TC 13 Z9 13 U1 4 U2 83 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7488 J9 J MATER CHEM A JI J. Mater. Chem. A PY 2013 VL 1 IS 3 BP 602 EP 610 DI 10.1039/c2ta00190j PG 9 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA 085RN UT WOS:000314632100023 ER PT J AU Hai, B Shukla, AK Duncan, H Chen, GY AF Hai, Bin Shukla, Alpesh K. Duncan, Hugues Chen, Guoying TI The effect of particle surface facets on the kinetic properties of LiMn1.5Ni0.5O4 cathode materials SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID LI-ION BATTERIES; PULSED-LASER DEPOSITION; MOLTEN-SALT SYNTHESIS; SINGLE-CRYSTAL; LINI0.5MN1.5O4 CATHODES; ELECTRODE MATERIALS; SPINEL CATHODES; LOCAL-STRUCTURE; X-RAY; PERFORMANCE AB Large LiMn1.5Ni0.5O4 single crystals in plate shape with (112) surface facets and octahedral shape with (111) surface facets were obtained by molten-salt synthesis. The presence of transition-metal ordering in both samples was independently confirmed by SAED, FTIR, NMR, and electrochemical studies, demonstrating the excellent capability of each technique in distinguishing the ordered and disordered phases. The apparent chemical diffusion minima during Li extraction and insertion were correlated with the occurrence of the first-order phase transition, implying that phase boundary movement limits Li transport in the spinel cathodes. Despite a more ordered structure, nearly ten times less Mn3+ content, and increased two-phase boundary movement during delithiation and relithiation, the octahedral crystals exhibited superior rate capability and a larger chemical diffusion coefficient, suggesting the kinetic preeminence of (111) surface facets over (112). The dominating effect of particle morphology and the importance of morphology design in achieving optimal performance of the LiMn1.5Ni0.5O4 spinel are clearly demonstrated for the first time. C1 [Hai, Bin; Shukla, Alpesh K.; Duncan, Hugues; Chen, Guoying] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. RP Hai, B (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. EM gchen@lbl.gov RI Foundry, Molecular/G-9968-2014 FU National Center for Electron Microscopy at Lawrence Berkeley National Laboratory and Stanford Synchrotron Radiation Lightsource; U.S. Department of Energy [DE-AC02-05CH11231] FX The authors acknowledge the support of the National Center for Electron Microscopy at Lawrence Berkeley National Laboratory and Stanford Synchrotron Radiation Lightsource, a Directorate of SLAC National Accelerator Laboratory and an Office of Science User Facility operated for the U.S. Department of Energy Office of Science by Stanford University. We thank Dr Michal Leskes for collecting 6Li MAS NMR data, and Dr Jordi Cabana for assisting with the synchrotron experiments. This work was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of FreedomCAR and Vehicle Technologies of the U.S. Department of Energy under contract no. DE-AC02-05CH11231. NR 42 TC 65 Z9 69 U1 8 U2 136 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7488 J9 J MATER CHEM A JI J. Mater. Chem. A PY 2013 VL 1 IS 3 BP 759 EP 769 DI 10.1039/c2ta00212d PG 11 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA 085RN UT WOS:000314632100043 ER PT J AU Wang, C Krishnan, V Wu, DS Bledsoe, R Paddison, SJ Duscher, G AF Wang, Chen Krishnan, Veena Wu, Dongsheng Bledsoe, Rylan Paddison, Stephen J. Duscher, Gerd TI Evaluation of the microstructure of dry and hydrated perfluorosulfonic acid ionomers: microscopy and simulations SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID NAFION PERFLUORINATED MEMBRANES; DISSIPATIVE PARTICLE DYNAMICS; PROTON-EXCHANGE MEMBRANES; FUEL-CELL MEMBRANES; ANGLE X-RAY; ELECTRON-MICROSCOPY; POLYMER MEMBRANES; MORPHOLOGY; SCATTERING; TRANSPORT AB The morphology of dry and hydrated perfluorosulfonic acid (PFSA) ionomers at cryo and room temperature is examined using TEM/STEM with EELS capability. Z-contrast imaging was utilized to identify the micro-phase separation of the hydrophilic side chains containing water and the hydrophobic polytetrafluoroethylene (PTFE) backbones. The results compare very favourably with hydrated morphologies obtained through mesoscale dissipative particle dynamics (DPD) simulations. The cryo-STEM images of plunge-frozen samples was also found to agree with morphologies based on SAXS experiments. C1 [Wang, Chen; Wu, Dongsheng; Paddison, Stephen J.] Univ Tennessee, Dept Chem & Biomol Engn, Knoxville, TN USA. [Krishnan, Veena; Bledsoe, Rylan; Duscher, Gerd] Univ Tennessee, Dept Mat Sci & Engn, Knoxville, TN USA. [Duscher, Gerd] Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN USA. RP Wang, C (reprint author), Univ Tennessee, Dept Chem & Biomol Engn, Knoxville, TN USA. EM spaddison@utk.edu RI Paddison, Stephen/B-2935-2014; Duscher, Gerd/G-1730-2014; Wang, Chen/I-3748-2014 OI Duscher, Gerd/0000-0002-2039-548X; Wang, Chen/0000-0002-2343-339X FU Office of Basic Energy Sciences, U.S. Department of Energy [DE-AC05-00OR22725]; Shared Research Equipment (SHaRE) user facility at Oak Ridge National Laboratory (ORNL); Sustainable Energy and Education Research Center (SEERC) FX This research was supported by Office of Basic Energy Sciences, U.S. Department of Energy (Contract no. DE-AC05-00OR22725), Shared Research Equipment (SHaRE) user facility at Oak Ridge National Laboratory (ORNL) and Sustainable Energy and Education Research Center (SEERC). We would also like to thank Houston Dycus and Joshua R. Garcia for their help with valuable data analysis. NR 40 TC 11 Z9 11 U1 2 U2 55 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7488 J9 J MATER CHEM A JI J. Mater. Chem. A PY 2013 VL 1 IS 3 BP 938 EP 944 DI 10.1039/c2ta01034h PG 7 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA 085RN UT WOS:000314632100066 ER PT J AU Wang, WC Chen, SY Yang, PX Duan, CG Wang, LW AF Wang, Weichao Chen, Shiyou Yang, Ping-Xiong Duan, Chun-Gang Wang, Lin-Wang TI Si:WO3 heterostructure for Z-scheme water splitting: an ab initio study SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID TOTAL-ENERGY CALCULATIONS; WAVE BASIS-SET; HYDROGEN GENERATION; SOLAR-ENERGY; WO3; OXYGEN; DEPOSITION; DIFFUSION; OXIDATION; SEMICONDUCTORS AB The Si:WO3 heterostructure is expected to have suitable band alignment for the Z-scheme water splitting, but the heterostructure interfaces have been scarcely studied. In this work, a series of interfaces between the WO3 (100) and Si (001) surfaces, which have a small lattice-mismatch, are studied using ab initio calculations. When there is no atom diffusion across the interface, a Si-O bonded interface with Si dimers is the most stable. Analysis of the electronic structure shows that the interfacial Si and O atoms are fully saturated, leading to a clean interface without localized gap states. O diffusion from WO3 into Si is found to be thermodynamically possible, but it does not affect the full bond saturation of the interfacial atoms. A type-II band alignment exists between Si and WO3, with the WO3 conduction band about 0.5 eV higher than the Si valence band, which is not influenced by O diffusion. A band diagram is plotted for the Si: WO3 heterostructure to evaluate its photocatalytic capability, and the influence of the small Schottky barrier and the interface amorphous layer is discussed. C1 [Wang, Weichao; Chen, Shiyou; Yang, Ping-Xiong; Duan, Chun-Gang] E China Normal Univ, Key Lab Polar Mat & Devices MOE, Shanghai 200241, Peoples R China. [Chen, Shiyou; Wang, Lin-Wang] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mat Sci Div, Berkeley, CA 94720 USA. [Chen, Shiyou; Wang, Lin-Wang] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, JCAP, Berkeley, CA 94720 USA. RP Wang, WC (reprint author), E China Normal Univ, Key Lab Polar Mat & Devices MOE, Shanghai 200241, Peoples R China. EM shiyouchen@lbl.gov; lwwang@lbl.gov RI Duan, Chun-Gang/D-2755-2013 FU NSF of China [61106087, 10934002, 61076060]; Special Funds for Major State Basic Research [2012CB921401]; Science and Technology Commission of Shanghai Municipality [10JC1404600]; PCSIRT; CC of ECNU; Office of Science of the U.S. Department of Energy [DE-SC0004993.] FX S.C. and L.W.W. acknowledge Dr Jian-Wei Sun, Le Chen, Joel W. Ager, David Grauer, Junjun Zhang and Ty Matthews for their helpful discussion. The work at ECNU is supported by the NSF of China (no. 61106087, 10934002 and 61076060), the Special Funds for Major State Basic Research (no. 2012CB921401), the Science and Technology Commission of Shanghai Municipality (10JC1404600), PCSIRT and CC of ECNU. This paper is based upon work performed by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, as follows: The data analysis and manuscript modification were supported through the Office of Science of the U.S. Department of Energy under Award no. DE-SC0004993. NR 42 TC 12 Z9 14 U1 2 U2 109 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 2013 VL 1 IS 4 BP 1078 EP 1085 DI 10.1039/c2ta00441k PG 8 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA 085SB UT WOS:000314633500014 ER PT J AU Jurow, MJ Hageman, BA DiMasi, E Nam, CY Pabon, C Black, CT Drain, CM AF Jurow, Matthew J. Hageman, Brian A. DiMasi, Elaine Nam, Chang-Yong Pabon, Cesar Black, Charles T. Drain, Charles Michael TI Controlling morphology and molecular packing of alkane substituted phthalocyanine blend bulk heterojunction solar cells SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID DISCOTIC LIQUID-CRYSTALS; ORGANIC PHOTOVOLTAIC CELLS; ELECTROCHEMICAL PROPERTIES; CONVERSION EFFICIENCY; ZINC PHTHALOCYANINE; PHOTONIC MATERIALS; SELF-ORGANIZATION; PORPHYRIN ARRAYS; DYE; ENERGY AB Systematic changes in the exocyclic substitution of a core phthalocyanine platform tune the absorption properties to yield commercially viable dyes that function as the primary light absorbers in organic bulk heterojunction solar cells. Blends of these complementary phthalocyanines absorb a broader portion of the solar spectrum compared to a single dye, thereby improving solar cell performance. We correlate grazing incidence small angle X-ray scattering data with solar cell performance to elucidate the role of the nanomorphology of active layers composed of blends of phthalocyanines and a fullerene derivative. A highly reproducible device architecture is used to ensure accuracy and is relevant to films for solar windows in urban settings. We demonstrate that the number and structure of the exocyclic motifs dictate phase formation, hierarchical organization, and nanostructure, thus can be employed to tailor active layer morphology to enhance exciton dissociation and charge collection efficiencies in the photovoltaic devices. These studies reveal that disordered films make better solar cells, short alkanes increase the optical density of the active layer, and branched alkanes inhibit unproductive homogeneous molecular alignment. C1 [Jurow, Matthew J.; Hageman, Brian A.; Pabon, Cesar; Drain, Charles Michael] CUNY, Hunter Coll, Dept Chem, New York, NY 10065 USA. [DiMasi, Elaine] Brookhaven Natl Lab, Photon Sci Div BLDG 728M, Upton, NY 11973 USA. [Nam, Chang-Yong; Black, Charles T.] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. [Drain, Charles Michael] Rockefeller Univ, New York, NY 10065 USA. RP Jurow, MJ (reprint author), CUNY, Hunter Coll, Dept Chem, New York, NY 10065 USA. EM DiMasi@bnl.gov; Cdrain@hunter.cuny.edu RI Nam, Chang-Yong/D-4193-2009; OI Nam, Chang-Yong/0000-0002-9093-4063; Jurow, Matthew/0000-0003-3943-4765 FU National Science Foundation (NSF) [CHE-0847997, 0848602]; National Institutes of Health [RR003037, MD007599]; CUNY; U.S. Department of Energy, Office of Basic Energy Sciences [DE-AC02-98CH10886] FX We thank Dr R. Gearba and Dr A. Varotto for assistance with experimental design, and Dr L. Yang, Dr K. Yager, and Dr V. Stanic for assistance with the X-ray beam. We also thank Mr J. Baris for helping to facilitate research, and N.P. Drain for the photos of the solar cells. This work was supported by the National Science Foundation (NSF, CHE-0847997 and 0848602 to C.M.D.). Hunter College Science infrastructure is supported by the NSF, the National Institutes of Health (including the RCMI program RR003037 and MD007599), and CUNY. This Research was carried out in part at the Center for Functional Nanomaterials and the National Synchrotron Light Source, Brookhaven National Laboratory supported by the U.S. Department of Energy, Office of Basic Energy Sciences, under Contract no. DE-AC02-98CH10886. NR 80 TC 16 Z9 16 U1 4 U2 101 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7488 J9 J MATER CHEM A JI J. Mater. Chem. A PY 2013 VL 1 IS 5 BP 1557 EP 1565 DI 10.1039/c2ta00415a PG 9 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA 085UP UT WOS:000314640100007 PM 23589766 ER PT J AU Sattayasamitsathit, S Gu, YE Kaufmann, K Jia, WZ Xiao, XY Rodriguez, M Minteer, S Cha, J Burckel, DB Wang, CM Polsky, R Wang, J AF Sattayasamitsathit, Sirilak Gu, Yonge Kaufmann, Kevin Jia, Wenzhao Xiao, Xiaoyin Rodriguez, Mark Minteer, Shelley Cha, Jennifer Burckel, D. Bruce Wang, Chunming Polsky, Ronen Wang, Joseph TI Highly ordered multilayered 3D graphene decorated with metal nanoparticles SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID FUEL-CELLS; INTERCONNECTED GRAPHENE; METHANOL OXIDATION; CARBON SUPPORT; PLATINUM; ELECTRODES; NANOCRYSTALS; TRANSPARENT; PERFORMANCE; DEPOSITION AB Highly ordered multi-layered three-dimensional (3D) graphene structures decorated with Pd, Pt and Au metal nanoparticles are prepared and characterized. The ability to control the morphology, distribution and size of the metal nanoparticles on the 3D graphene support upon changing the electro- and electroless-deposition conditions is demonstrated. Tailor-made Pt nanostructures, with nanospike and nanoparticle shapes, are prepared using electroless deposition techniques. Au nanoflowers and nanoparticle structures and Pd nanocubes are obtained following electrodeposition onto the 3D graphene support. The deposition patterns and trends are characterized. The greatly enhanced electrocatalytic activity of the metal-NP-graphene surfaces has been illustrated in connection to voltammetric measurements of ORR and hydrogen peroxide at 3D-graphene coated with Pt and Pd nanoparticles, respectively. Such metal nanoparticles decorated multi-layer 3D graphene allows for high mass transport access and catalytic activity for a diverse range of applications, including sensor and fuel-cell technologies. C1 [Sattayasamitsathit, Sirilak; Gu, Yonge; Kaufmann, Kevin; Jia, Wenzhao; Cha, Jennifer; Wang, Joseph] Univ Calif San Diego, Dept Nanoengn, La Jolla, CA 92093 USA. [Gu, Yonge; Wang, Chunming] Lanzhou Univ, Dept Chem, Lanzhou 730000, Peoples R China. [Xiao, Xiaoyin; Rodriguez, Mark; Burckel, D. Bruce; Polsky, Ronen] Sandia Natl Labs, Dept Biosensors & Nanomat, Albuquerque, NM 87185 USA. [Minteer, Shelley] Univ Utah, Dept Chem & Mat Sci & Engn, Salt Lake City, UT 84112 USA. RP Sattayasamitsathit, S (reprint author), Univ Calif San Diego, Dept Nanoengn, La Jolla, CA 92093 USA. EM rpolsky@sandia.gov; josephwang@ucsd.edu RI Sattayasamitsathit, Sirilak/A-6883-2010; Jia, Wenzhao/F-6168-2013; Minteer, Shelley/C-4751-2014; Wang, Joseph/C-6175-2011 OI Sattayasamitsathit, Sirilak/0000-0003-0349-3333; Jia, Wenzhao/0000-0003-1387-5407; Minteer, Shelley/0000-0002-5788-2249; FU United Stated Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000]; Sandia National Laboratories' Laboratory Directed Research & Development (LDRD); National Science Foundation [CHE-1057562]; U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering [DE-SC0004937]; China Scholarship Council (CSC) FX Sandia is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the United Stated 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), National Science Foundation under award no. CHE-1057562 ( material synthesis and characterization), and the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering under award no. DE-SC0004937 (electrocatalytic behavior and energy applications). Y.G. acknowledges the China Scholarship Council (CSC) for the financial support. The authors thank P. Xu for her help. NR 35 TC 49 Z9 49 U1 5 U2 226 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7488 J9 J MATER CHEM A JI J. Mater. Chem. A PY 2013 VL 1 IS 5 BP 1639 EP 1645 DI 10.1039/c2ta00954d PG 7 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA 085UP UT WOS:000314640100017 ER PT J AU Gorka, J Mayes, RT Baggetto, L Veith, GM Dai, S AF Gorka, Joanna Mayes, Richard T. Baggetto, Loic Veith, Gabriel M. Dai, Sheng TI Sonochemical functionalization of mesoporous carbon for uranium extraction from seawater SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID GROUP-CONTAINING ADSORBENT; SURFACE FUNCTIONALIZATION; SEA-WATER; POLYMER; STABILITY; RECOVERY; POLYACRYLONITRILE; ADSORPTION; SILICAS; URANYL AB Extracting uranium from seawater is challenging due to its low concentration (3.3 ppb) and the myriad of competing ions. Mesoporous carbon materials provide a high surface area alternative to the traditional polymeric fiber braids developed for seawater extractions, specifically uranium extraction. In this work, sonochemical grafting of acrylonitrile onto the pores of soft-templated mesoporous carbons followed by its conversion to amidoxime functionalities was used to prepare an effective sorbent material with a high density of binding sites. Pore blockage, often observed for free radical polymerization, leads to poor adsorbent performance but can be easily overcome by the use of ultrasound during polymerization. Parameters such as surface area and surface pre-treatment, sonication intensity, solvent system, and monomer/initiator ratios were varied to optimize the polymerization and uranium adsorption capacity while not blocking the porosity, a significant hurdle in the utilization of functionalized porous materials. The results show that neither the surface oxidation with nitric acid nor CO2 activation alone is sufficient to cause significant improvement in grafting and uranium uptake. However, when coupled together, a greatly enhanced performance of the adsorbent materials was observed. C1 [Gorka, Joanna; Mayes, Richard T.; Dai, Sheng] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. [Baggetto, Loic; Veith, Gabriel M.] Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. [Dai, Sheng] Univ Tennessee, Dept Chem, Knoxville, TN 37996 USA. RP Gorka, J (reprint author), Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. EM dais@ornl.gov RI Dai, Sheng/K-8411-2015; Mayes, Richard/G-1499-2016; Baggetto, Loic/D-5542-2017 OI Dai, Sheng/0000-0002-8046-3931; Mayes, Richard/0000-0002-7457-3261; Baggetto, Loic/0000-0002-9029-2363 FU Fuel Resources Campaign in the Fuel Cycle Research and Development Program, Office of Nuclear Energy, U.S. Department of Energy (DOE) FX We thank the Fuel Resources Campaign in the Fuel Cycle Research and Development Program, Office of Nuclear Energy, U.S. Department of Energy (DOE), for support of this work. NR 41 TC 57 Z9 59 U1 18 U2 172 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 2013 VL 1 IS 9 BP 3016 EP 3026 DI 10.1039/c2ta01008a PG 11 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA 085XQ UT WOS:000314648000012 ER PT J AU Cox-Galhotra, RA Huq, A Hodges, JP Kim, JH Yu, CF Wang, XQ Jacobson, AJ McIntosh, S AF Cox-Galhotra, Rosemary A. Huq, Ashfia Hodges, Jason P. Kim, Jung-Hyun Yu, Chengfei Wang, Xiqu Jacobson, Allan J. McIntosh, Steven TI Visualizing oxygen anion transport pathways in NdBaCo2O5+delta by in situ neutron diffraction SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID OXIDE FUEL-CELLS; ELECTRICAL-CONDUCTIVITY; LAYERED COBALTITES; HIGH-TEMPERATURE; CATHODES; LNBACO(2)O(5+DELTA); PRBACO2O5+DELTA; DIFFUSION; MEMBRANES; CRYSTAL AB The layered perovskite NdBaCo2O5+delta (NBCO) was characterized using neutron powder diffraction under in situ conditions from 577-852 degrees C and in 10(-1) to 10(-4) atm oxygen. The best fit to the data was obtained in the tetragonal (P4/mmm) space group. No oxygen atom vacancy ordering was observed that warranted a lowering of the symmetry to orthorhombic (Pmmm). Two P4/mmm structural models were investigated: Model 1 (no split sites) and Model 2 (split Nd and O2 sites). Transport of oxygen through the material via the vacancy hopping mechanism likely involves the nearest-neighbor oxygen atom sites in the Nd layer. Total oxygen stoichiometry values were in the range 5.51 <= delta <= 5.11. The tetragonal lattice parameters increased with temperature as expected. However, the a-axis expands while the c-axis contracts with decreasing pO(2) at a given temperature due to increasing vacancy concentration in the Nd layer. C1 [Cox-Galhotra, Rosemary A.; McIntosh, Steven] Univ Virginia, Dept Chem Engn, Charlottesville, VA 22904 USA. [Huq, Ashfia; Hodges, Jason P.; Kim, Jung-Hyun] Oak Ridge Natl Lab, Spallat Neutron Source, Oak Ridge, TN 37830 USA. [Yu, Chengfei; Wang, Xiqu; Jacobson, Allan J.] Univ Houston, Dept Chem, Houston, TX 77204 USA. [McIntosh, Steven] Lehigh Univ, Dept Chem Engn, Bethlehem, PA 18015 USA. RP Cox-Galhotra, RA (reprint author), Univ Virginia, Dept Chem Engn, Charlottesville, VA 22904 USA. EM mcintosh@lehigh.edu RI Kim, Jung-Hyun/I-5273-2013; Huq, Ashfia/J-8772-2013; Hodges, Jason/K-1421-2013; Albe, Karsten/F-1139-2011; OI Kim, Jung-Hyun/0000-0002-4598-4686; Huq, Ashfia/0000-0002-8445-9649; Hodges, Jason/0000-0003-3016-4578 FU Division of Scientific User Facilities, Office of Basic Energy Sciences, U.S. Department of Energy [DE-AC05-00OR22725]; U.S. National Science Foundation; Robert A Welch Foundation [E-0024]; U.S. Department of Energy (U.S. DOE), Office of Basic Energy Sciences, Division of Materials Sciences and Engineering [DE-SC0001284] FX Use of the Spallation Neutron Source 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. Rosemary Cox-Galhotra is supported by the U.S. National Science Foundation Graduate Research Fellowship. AJJ, CY and XW acknowledge support from the Robert A Welch Foundation (Grant no. E-0024, XW) and the U.S. Department of Energy (U.S. DOE), Office of Basic Energy Sciences, Division of Materials Sciences and Engineering (under Award no. DE-SC0001284, sample preparation, neutron experiments). NR 43 TC 20 Z9 20 U1 3 U2 53 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 2013 VL 1 IS 9 BP 3091 EP 3100 DI 10.1039/c3ta01308a PG 10 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA 085XQ UT WOS:000314648000022 ER PT J AU Schudel, BR Harmon, B Abhyankar, VV Pruitt, BW Negrete, OA Singh, AK AF Schudel, Benjamin R. Harmon, Brooke Abhyankar, Vinay V. Pruitt, Benjamin W. Negrete, Oscar A. Singh, Anup K. TI Microfluidic platforms for RNA interference screening of virus-host interactions SO LAB ON A CHIP LA English DT Article ID CELL ARRAYS; MICROSCOPY; GENE; EXPRESSION; INFECTION; ENDOCYTOSIS; PROTEINS AB RNA interference (RNAi) is a powerful tool for functional genomics with the capacity to comprehensively analyze host-pathogen interactions. High-throughput RNAi screening is used to systematically perturb cellular pathways and discover therapeutic targets, but the method can be tedious and requires extensive capital equipment and expensive reagents. To aid in the development of an inexpensive miniaturized RNAi screening platform, we have developed a two part microfluidic system for patterning and screening gene targets on-chip to examine cellular pathways involved in virus entry and infection. First, a multilayer polydimethylsiloxane (PDMS)-based spotting device was used to array siRNA molecules into 96 microwells targeting markers of endocytosis, along with siRNA controls. By using a PDMS-based spotting device, we remove the need for a microarray printer necessary to perform previously described small scale (e. g. cellular microarrays) and microchip-based RNAi screening, while still minimizing reagent usage tenfold compared to conventional screening. Second, the siRNA spotted array was transferred to a reversibly sealed PDMS-based screening platform containing microchannels designed to enable efficient cell loading and transfection of mammalian cells while preventing cross-contamination between experimental conditions. Validation of the screening platform was examined using Vesicular stomatitis virus and emerging pathogen Rift Valley fever virus, which demonstrated virus entry pathways of clathrin-mediated endocytosis and caveolae-mediated endocytosis, respectively. The techniques here are adaptable to other well-characterized infection pathways with a potential for large scale screening in high containment biosafety laboratories. C1 [Schudel, Benjamin R.; Harmon, Brooke; Abhyankar, Vinay V.; Pruitt, Benjamin W.; Negrete, Oscar A.; Singh, Anup K.] Sandia Natl Labs, Dept Biotechnol & Bioengn, Livermore, CA 94551 USA. RP Negrete, OA (reprint author), Sandia Natl Labs, Dept Biotechnol & Bioengn, POB 969, Livermore, CA 94551 USA. EM onegret@sandia.gov; aksingh@sandia.gov OI Pruitt, Benjamin/0000-0001-7532-7081 FU U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000]; Laboratory Directed Research and Development grant 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 a Laboratory Directed Research and Development grant given to O.A.N. at Sandia National Laboratories. NR 33 TC 8 Z9 9 U1 2 U2 31 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1473-0197 J9 LAB CHIP JI Lab Chip PY 2013 VL 13 IS 5 BP 811 EP 817 DI 10.1039/c2lc41165b PG 7 WC Biochemical Research Methods; Chemistry, Multidisciplinary; Nanoscience & Nanotechnology SC Biochemistry & Molecular Biology; Chemistry; Science & Technology - Other Topics GA 085YU UT WOS:000314651000008 PM 23361404 ER PT J AU Fowlkes, JD Collier, CP AF Fowlkes, Jason D. Collier, C. Patrick TI Single-molecule mobility in confined and crowded femtolitre chambers SO LAB ON A CHIP LA English DT Article ID FLUORESCENCE CORRELATION SPECTROSCOPY; CROSS-CORRELATION SPECTROSCOPY; FLUIDIC CHANNELS; DIFFUSION; DYNAMICS; CELLS; PROBE AB The effects of increased crowding and confinement on the mobility of individual fluorescent molecules were studied using Fluorescence Correlation Spectroscopy (FCS) in a microfluidic device with sealable femtolitre-volume chambers, and compared to three dimensional stochastic Monte Carlo simulations. When crowding and the degree of confinement were increased simultaneously, extended correlation times of fluorescent intensity fluctuations were observed with FCS compared to varying either crowding or confinement alone. Both experimental data and simulation suggest these extended correlation times were due to increased fluorophore adsorption-desorption events at the chamber lid in the presence of crowders. The data in increasingly confined and crowded chambers described here captures some of the salient features of crowding in cell-like environments. C1 [Fowlkes, Jason D.; Collier, C. Patrick] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 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 Oak Ridge National Laboratory by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy 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. NR 40 TC 6 Z9 6 U1 1 U2 24 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 2013 VL 13 IS 5 BP 877 EP 885 DI 10.1039/c2lc40907k PG 9 WC Biochemical Research Methods; Chemistry, Multidisciplinary; Nanoscience & Nanotechnology SC Biochemistry & Molecular Biology; Chemistry; Science & Technology - Other Topics GA 085YU UT WOS:000314651000016 PM 23303284 ER PT J AU Haroz, EH Duque, JG Tu, XM Zheng, M Walker, ARH Hauge, RH Doorn, SK Kono, J AF Haroz, Erik H. Duque, Juan G. Tu, Xiaomin Zheng, Ming Walker, Angela R. Hight Hauge, Robert H. Doorn, Stephen K. Kono, Junichiro TI Fundamental optical processes in armchair carbon nanotubes SO NANOSCALE LA English DT Article ID MANY-FERMION SYSTEM; ELECTRONIC-STRUCTURE; RAMAN-SCATTERING; QUANTUM WIRES; DENSITY DIFFERENTIATION; ABSORPTION-SPECTRA; SOMMERFELD FACTORS; RESONANCE RAMAN; SINGLE; DNA AB Single-wall carbon nanotubes provide ideal model one-dimensional (1-D) condensed matter systems in which to address fundamental questions in many-body physics, while, at the same time, they are leading candidates for building blocks in nanoscale optoelectronic circuits. Much attention has been recently paid to their optical properties, arising from 1-D excitons and phonons, which have been revealed via photoluminescence, Raman scattering, and ultrafast optical spectroscopy of semiconducting carbon nanotubes. On the other hand, dynamical properties of metallic nanotubes have been poorly explored, although they are expected to provide a novel setting for the study of electron-hole pairs in the presence of degenerate 1-D electrons. In particular, (n,n)-chirality, or armchair, metallic nanotubes are truly gapless with massless carriers, ideally suited for dynamical studies of Tomonaga-Luttinger liquids. Unfortunately, progress towards such studies has been slowed by the inherent problem of nanotube synthesis whereby both semiconducting and metallic nanotubes are produced. Here, we use post-synthesis separation methods based on density gradient ultracentrifugation and DNA-based ion-exchange chromatography to produce aqueous suspensions strongly enriched in armchair nanotubes. Through resonant Raman spectroscopy of the radial breathing mode phonons, we provide macroscopic and unambiguous evidence that density gradient ultracentrifugation can enrich ensemble samples in armchair nanotubes. Furthermore, using conventional, optical absorption spectroscopy in the near-infrared and visible range, we show that interband absorption in armchair nanotubes is strongly excitonic. Lastly, by examining the G-band mode in Raman spectra, we determine that observation of the broad, lower frequency (G(-)) feature is a result of resonance with non-armchair "metallic" nanotubes. These findings regarding the fundamental optical absorption and scattering processes in metallic carbon nanotubes lay the foundation for further spectroscopic studies to probe many-body physical phenomena in one dimension. C1 [Haroz, Erik H.] Rice Univ, Dept Elect & Comp Engn, Houston, TX 77005 USA. [Haroz, Erik H.; Hauge, Robert H.; Kono, Junichiro] Rice Univ, Richard E Smalley Inst Nanoscale Sci & Technol, Houston, TX 77005 USA. [Duque, Juan G.] Los Alamos Natl Lab, Div Chem, Phys Chem & Appl Spect C PCS, Los Alamos, NM 87545 USA. [Tu, Xiaomin; Zheng, Ming] NIST, Div Polymers, Gaithersburg, MD 20899 USA. [Walker, Angela R. Hight] NIST, Opt Technol Div, Gaithersburg, MD 20899 USA. [Hauge, Robert H.] Rice Univ, Dept Chem, Houston, TX 77005 USA. [Doorn, Stephen K.] Los Alamos Natl Lab, Ctr Integrated Nanotechnol, Los Alamos, NM 87545 USA. [Kono, Junichiro] Rice Univ, Dept Phys & Astron, Houston, TX 77005 USA. RP Kono, J (reprint author), Rice Univ, Dept Elect & Comp Engn, 6100 Main St,MS-378, Houston, TX 77005 USA. EM kono@rice.edu RI Hight Walker, Angela/C-3373-2009; Hauge, Robert/A-7008-2011 OI Hight Walker, Angela/0000-0003-1385-0672; Hauge, Robert/0000-0002-3656-0152 FU National Science Foundation [CHE-0809020, CMS-060950]; Department of Energy BES Program [DEFG02-06ER46308]; Air Force Research Laboratories [FA8650-05-D-5807]; Los Alamos National Laboratory LDRD Program; Robert A. Welch Foundation [C-1509, C-0807]; National Aeronautics and Space Administration [NNJ05HI05C]; World Class University Program at Sungkyunkwan University [R31-2008-000-10029-0] FX This work was supported by the National Science Foundation through Grant no. CHE-0809020 and CMS-060950, the Department of Energy BES Program through Grant no. DEFG02-06ER46308, the Air Force Research Laboratories under contract number FA8650-05-D-5807, the Los Alamos National Laboratory LDRD Program, the Robert A. Welch Foundation through Grant no. C-1509 and C-0807, the National Aeronautics and Space Administration (NNJ05HI05C), and the World Class University Program at Sungkyunkwan University (R31-2008-000-10029-0). This work was performed in part at the Center for Integrated Nanotechnologies, a US Department of Energy, Office of Basic Energy Sciences user facility. We thank our collaborators who contributed to the work presented in this feature article: B. Y. Lu, W. D. Rice, S. Ghosh, R. B. Weisman, P. Nikolaev, S. Arepalli, C. G. Densmore, A. Jagota, D. Roxbury, C. Y. Khripin and J. A. Fagan. We would also like to thank K. Yanagi, C. Kittrell, W. Adams, N. Alvarez, C. Pint, B. Dan, K. Sato, R. Saito, and A. Imambekov for useful and stimulating discussions. NR 166 TC 19 Z9 19 U1 2 U2 79 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2040-3364 J9 NANOSCALE JI Nanoscale PY 2013 VL 5 IS 4 BP 1411 EP 1439 DI 10.1039/c2nr32769d PG 29 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA 083PM UT WOS:000314477300020 PM 23340668 ER PT J AU Forssen, C Hagen, G Hjorth-Jensen, M Nazarewicz, W Rotureau, J AF Forssen, C. Hagen, G. Hjorth-Jensen, M. Nazarewicz, W. Rotureau, J. TI Living on the edge of stability, the limits of the nuclear landscape SO PHYSICA SCRIPTA LA English DT Article; Proceedings Paper CT 152nd Nobel Symposium on Physics with Radioactive Beams CY JUN 11-15, 2012 CL Goteborg, SWEDEN ID MATRIX RENORMALIZATION-GROUP; MONTE-CARLO DIAGONALIZATION; SHELL-MODEL; MEAN-FIELD; DRIP-LINE; QUANTUM-SYSTEMS; CONTINUUM; FORCES; ENERGY; MATTER AB A first-principles description of nuclear systems along the drip lines presents a substantial theoretical and computational challenge. In this paper, we discuss the nuclear theory roadmap, some of the key theoretical approaches, and present selected results with a focus on long isotopic chains. An important conclusion, which consistently emerges from these theoretical analyses, is that three-nucleon forces are crucial for both global nuclear properties and detailed nuclear structure, and that many-body correlations due to the coupling to the particle continuum are essential as one approaches particle drip lines. In the quest for a comprehensive nuclear theory, high performance computing plays a key role. C1 [Forssen, C.; Rotureau, J.] Chalmers, Dept Fundamental Phys, SE-41296 Gothenburg, Sweden. [Hagen, G.; Nazarewicz, W.] Oak Ridge Natl Lab, Div Phys, Oak Ridge, TN 37831 USA. [Hagen, G.; Nazarewicz, W.] Univ Tennessee, Dept Phys & Astron, Knoxville, TN 37996 USA. [Hjorth-Jensen, M.] Michigan State Univ, Natl Superconducting Cyclotron Lab, E Lansing, MI 48824 USA. [Hjorth-Jensen, M.] Michigan State Univ, Dept Phys & Astron, E Lansing, MI 48824 USA. [Hjorth-Jensen, M.] Univ Oslo, Dept Phys, N-0316 Oslo, Norway. [Hjorth-Jensen, M.] Univ Oslo, Ctr Math Applicat, N-0316 Oslo, Norway. [Nazarewicz, W.] Warsaw Univ, Inst Theoret Phys, PL-00681 Warsaw, Poland. RP Forssen, C (reprint author), Chalmers, Dept Fundamental Phys, SE-41296 Gothenburg, Sweden. EM morten.hjorth-jensen@fys.uio.no RI Forssen, Christian/C-6093-2008; rotureau, jimmy/B-2365-2013 OI Forssen, Christian/0000-0003-3458-0480; FU European Research Council under European Community [240603]; US Department of Energy [DE-AC05-00OR22725, DE-FG02-96ER40963, DE-FG05-87ER40361, DE-SC0008499, DE-FG02-04ER41338]; US NSF [PHY-0854912]; Swedish Research Council [2007-4078]; Research Council of Norway via Notur project [NN2977K]; Office of Nuclear Physics, US Department of Energy (Oak Ridge National Laboratory) FX We are much indebted to Carlo Barbieri, Bruce Barrett, Scott Bogner, Alex Brown, David Dean, Jacek Dobaczewski, Thomas Duguet, Dick Furnstahl, Alexandra Gade, Mihai Horoi, Gustav Jansen, Robert Janssens, Oyvind Jensen, Bjorn Jonson, Simen Kvaal, Augusto Macchiavelli, Pieter Maris, Nicolas Michel, Petr Navratil, Thomas Nilsson, Filomena Nunes, Takaharu Otsuka, George Papadimitriou, Thomas Papenbrock, Lucas Platter, Marek Ploszajczak, Sofia Quaglioni, Robert Roth, Achim Schwenk, Brad Sherill, Olivier Sorlin, Artemisia Spyrou, Michael Thoennessen, Jeff Tostevin, Koshiroh Tsukiyama and James Vary for the many stimulating discussions on nuclear physics, many-body physics, shell-model and coupled-cluster calculations, nuclear density functional theory, and open quantum systems. The research leading to these results has received funding from the European Research Council under the European Community's Seventh Framework Programme (FP7/2007-2013)/ERC grant agreement no. 240603. This work was supported by the US Department of Energy under contract nos. DE-AC05-00OR22725 (Oak Ridge National Laboratory, managed by UT-Battelle, LLC), DE-FG02-96ER40963 (University of Tennessee), DE-FG05-87ER40361 (Joint Institute for Heavy Ion Research), DE-SC0008499 (NUCLEI SciDAC Collaboration), DE-FG02-04ER41338, the US NSF under grant number PHY-0854912, and by the Swedish Research Council (dnr. 2007-4078). Computational resources were provided by the Oak Ridge Leadership Class Computing Facility, the National Energy Research Scientific Computing Facility and the Research Council of Norway via the Notur project (Supercomputing grant number NN2977K). This work was supported by the Office of Nuclear Physics, US Department of Energy (Oak Ridge National Laboratory). An award of computer time was provided by the Innovative and Novel Computational Impact on Theory and Experiment (INCITE) program. NR 198 TC 25 Z9 25 U1 1 U2 23 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 0031-8949 EI 1402-4896 J9 PHYS SCRIPTA JI Phys. Scr. PD JAN PY 2013 VL T152 AR 014022 DI 10.1088/0031-8949/2013/T152/014022 PG 19 WC Physics, Multidisciplinary SC Physics GA 078MT UT WOS:000314103800023 ER PT J AU Janssens, RVF AF Janssens, Robert V. F. TI Tracking changes in shell structure in neutron-rich nuclei as a function of spin SO PHYSICA SCRIPTA LA English DT Article; Proceedings Paper CT 152nd Nobel Symposium on Physics with Radioactive Beams CY JUN 11-15, 2012 CL Goteborg, SWEDEN ID EXCITED-STATES; MODEL; ISOTOPES; NI-68; N=40; CLOSURES; MASSES; TI-55; CORE; N=32 AB Taking advantage of the resolving power of modern gamma-ray spectrometers in combination with different types of nuclear reactions, it has been possible to investigate to fairly high-spin neutron-rich nuclei in a number of regions of the nuclear chart. The primary motivations for such studies are to characterize changes in shell structure as a function of the neutron-to-proton ratio and to document the impact of a large neutron excess on global properties, such as the nuclear shape. Recent data on nuclei close to the 'island of inversion' near Mg-32 are discussed first. They highlight challenges in describing the observations with modern effective interactions. Subsequently, the nature of excitations in neutron-rich fpg-shell nuclei between Ca and Ni is reviewed. A neutron sub-shell closure at N = 32 has been attributed to the monopole tensor force. Furthermore, the presence of collective excitations at moderate spin in neutron-rich Cr and Fe isotopes illustrates the role of the g(9/2) orbital in driving the nuclear shape. The observations suggest that mixing between 'deformed' and 'shell-model' states needs to be considered. Finally, recent results in the direct vicinity of Ni-68 indicate that the impact of the N = 40 neutron shell closure is rather modest. C1 Argonne Natl Lab, Div Phys, Argonne, IL 60439 USA. RP Janssens, RVF (reprint author), Argonne Natl Lab, Div Phys, 9700 S Cass Ave, Argonne, IL 60439 USA. EM janssens@anl.gov FU US Department of Energy, Office of Nuclear Physics [DE-AC02-06CH11357] FX The author would like to express his gratitude to the organizing committee of the Nobel Symposium for the opportunity to attend the meeting and to present this contribution. He is also indebted to his many collaborators: without their hard work and effort, the results presented above would not have materialized. He gratefully acknowledges constant fruitful interactions with A Gade, C Chiara, S Freeman, B Fornal, W Walters, as well as with his ANL collaborators M P Carpenter and S Zhu. This work was supported by the US Department of Energy, Office of Nuclear Physics, under contract no. DE-AC02-06CH11357. NR 64 TC 4 Z9 4 U1 1 U2 2 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 0031-8949 EI 1402-4896 J9 PHYS SCRIPTA JI Phys. Scr. PD JAN PY 2013 VL T152 AR 014005 DI 10.1088/0031-8949/2013/T152/014005 PG 10 WC Physics, Multidisciplinary SC Physics GA 078MT UT WOS:000314103800006 ER PT J AU Jones, KL AF Jones, Kate L. TI Transfer reaction experiments with radioactive beams: from halos to the r-process SO PHYSICA SCRIPTA LA English DT Article; Proceedings Paper CT 152nd Nobel Symposium on Physics with Radioactive Beams CY JUN 11-15, 2012 CL Goteborg, SWEDEN ID SINGLE-PARTICLE STATES; INVERSE KINEMATICS; DETECTOR ARRAY; REX-ISOLDE; SPECTROMETER; BE-11; NUCLEI; PB-208; CARBON; RADII AB Transfer reactions are a powerful probe of the properties of atomic nuclei. When used in inverse kinematics with radioactive ion beams they can provide detailed information on the structure of exotic nuclei and can inform nucleosynthesis calculations. There are a number of groups around the world who use these reactions, usually with particle detection in large silicon arrays. Sometimes these arrays are coupled to gamma-ray detectors, and occasionally smaller arrays of silicon detectors are mounted within a solenoid magnet. Modern techniques using transfer reactions in inverse kinematics are covered, with specific examples, many from measurements made with beams from the Holifield Radioactive Ion Beam Facility at Oak Ridge National Laboratory. C1 [Jones, Kate L.] Univ Tennessee, Dept Phys & Astron, Knoxville, TN 37996 USA. [Jones, Kate L.] Oak Ridge Natl Lab, Div Phys, Oak Ridge, TN 37831 USA. RP Jones, KL (reprint author), Univ Tennessee, Dept Phys & Astron, Knoxville, TN 37996 USA. EM kgrzywac@utk.edu RI Jones, Katherine/B-8487-2011 OI Jones, Katherine/0000-0001-7335-1379 FU US Department of Energy [DE-FG02-96ER40983, DE-SC0001174] FX I would like to thank all of my collaborators on the experiments described here, especially James Allmond, Daniel Bardayan, James Beene, Anissa Bey, Jolie Cizewski, Alfredo Galindo-Uribarri, Ray Kozub, Brett Manning, Filomena Nunes, Steven Pain, David Radford, Kyle Schmitt and the ORRUBA-RIBENS and CLARION-HYBALL collaborations. Additionally I would like to thank Jacob Johansen, Karsten Riisager and their collaborators for allowing their data to be presented here. This work was supported by the US Department of Energy under contract numbers DE-FG02-96ER40983 (UT), DE-SC0001174 (UT). NR 77 TC 7 Z9 7 U1 0 U2 3 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 0031-8949 EI 1402-4896 J9 PHYS SCRIPTA JI Phys. Scr. PD JAN PY 2013 VL T152 AR 014020 DI 10.1088/0031-8949/2013/T152/014020 PG 10 WC Physics, Multidisciplinary SC Physics GA 078MT UT WOS:000314103800021 ER PT J AU Cabot, W Zhou, Y AF Cabot, W. Zhou, Ye TI Statistical measurements of scaling and anisotropy of turbulent flows induced by Rayleigh-Taylor instability SO PHYSICS OF FLUIDS LA English DT Article ID DIRECT NUMERICAL SIMULATIONS; VARIABLE-DENSITY TURBULENCE; ISOTROPIC TURBULENCE; REYNOLDS-NUMBER; MIXING TRANSITION; ENERGY-TRANSFER; LOCAL ISOTROPY; VORTICITY; DISSIPATION; SKEWNESS AB This work investigates several key statistical measurements of turbulence induced by Rayleigh-Taylor instability using data from well resolved numerical simulations at moderate Reynolds number with the goal of determining the degree of departure of this inhomogeneous flow from that of homogeneous, isotropic turbulence. The simulations use two miscible fluids with unity Schmidt number and moderate density contrast (3/2 to 9). The results of this study should find application in subgrid-scale modeling for large-eddy simulations and Reynolds-averaged Navier-Stokes modeling used in many engineering and scientific problems. (C) 2013 American Institute of Physics. [http://dx.doi.org/10.1063/1.4774338] C1 [Cabot, W.; Zhou, Ye] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. RP Cabot, W (reprint author), Lawrence Livermore Natl Lab, 7000 East Ave, Livermore, CA 94550 USA. FU Lawrence Livermore National Security, LLC [DE-AC52-07NA27344] FX This work was performed under the auspices of the Lawrence Livermore National Security, LLC under Contract No. DE-AC52-07NA27344. NR 40 TC 10 Z9 10 U1 0 U2 17 PU AMER INST PHYSICS PI MELVILLE PA CIRCULATION & FULFILLMENT DIV, 2 HUNTINGTON QUADRANGLE, STE 1 N O 1, MELVILLE, NY 11747-4501 USA SN 1070-6631 J9 PHYS FLUIDS JI Phys. Fluids PD JAN PY 2013 VL 25 IS 1 AR 015107 DI 10.1063/1.4774338 PG 18 WC Mechanics; Physics, Fluids & Plasmas SC Mechanics; Physics GA 086ZC UT WOS:000314728200032 ER PT J AU Loxley, PN Nadiga, BT AF Loxley, P. N. Nadiga, B. T. TI Bistability and hysteresis of maximum-entropy states in decaying two-dimensional turbulence SO PHYSICS OF FLUIDS LA English DT Article ID STATISTICAL-MECHANICS; RELAXATION; EQUATIONS; FLOWS AB We propose a theory that qualitatively predicts the stability and equilibrium structure of long-lived, quasi-steady flow states in decaying two-dimensional turbulence. This theory combines a maximum entropy principal with a nonlinear parameterization of the vorticity-stream-function dependency of such long-lived states. In particular, this theory predicts unidirectional-flow states that are bistable, exhibit hysteresis, and undergo large abrupt changes in flow topology; and a vortex-pair state that undergoes continuous changes in flow topology. These qualitative predictions are confirmed in numerical simulations of the two-dimensional Navier-Stokes equation. We discuss limitations of the theory, and why a reduced quantitative theory of long-lived flow states is difficult to obtain. We also provide a partial theoretical justification for why certain sets of initial conditions go to certain long-lived flow states. (C) 2013 American Institute of Physics. [http://dx.doi.org/10.1063/1.4774348] C1 [Loxley, P. N.] Los Alamos Natl Lab, Ctr Nonlinear Studies, Los Alamos, NM 87545 USA. [Loxley, P. N.] Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. [Nadiga, B. T.] Los Alamos Natl Lab, Comp Computat & Stat Sci Div, Los Alamos, NM 87545 USA. RP Loxley, PN (reprint author), Los Alamos Natl Lab, Ctr Nonlinear Studies, Los Alamos, NM 87545 USA. OI Loxley, Peter/0000-0003-3659-734X FU U.S. Department of Energy (DOE) through the LANL/LDRD Program [20110150ER]; Center for Nonlinear Studies; NSF [1066293] FX We thank D. Montgomery and F. Bouchet for informative discussions on topics closely related to this work. We gratefully acknowledge the support of the U.S. Department of Energy (DOE) through the LANL/LDRD Program Project No. 20110150ER for this work. P.N.L. was also supported by the Center for Nonlinear Studies. B.T.N. thanks the Aspen Center for Physics (supported in part by NSF Grant No. 1066293) for its hospitality during the summer 2012 workshop on "Stochastic Flows and Climate Modeling." NR 19 TC 3 Z9 3 U1 1 U2 11 PU AMER INST PHYSICS PI MELVILLE PA CIRCULATION & FULFILLMENT DIV, 2 HUNTINGTON QUADRANGLE, STE 1 N O 1, MELVILLE, NY 11747-4501 USA SN 1070-6631 J9 PHYS FLUIDS JI Phys. Fluids PD JAN PY 2013 VL 25 IS 1 AR 015113 DI 10.1063/1.4774348 PG 17 WC Mechanics; Physics, Fluids & Plasmas SC Mechanics; Physics GA 086ZC UT WOS:000314728200038 ER PT J AU Bennun, SV Yarema, KJ Betenbaugh, MJ Krambeck, FJ AF Bennun, Sandra V. Yarema, Kevin J. Betenbaugh, Michael J. Krambeck, Frederick J. TI Integration of the Transcriptome and Glycome for Identification of Glycan Cell Signatures SO PLOS COMPUTATIONAL BIOLOGY LA English DT Article ID PROSTATE-SPECIFIC ANTIGEN; GENE-EXPRESSION DATA; CARBOHYDRATE ANTIGENS; MATHEMATICAL-MODEL; SEMINAL PLASMA; CANCER CELLS; LNCAP CELLS; GLYCOSYLATION; CARCINOMA; LECTIN AB Abnormalities in glycan biosynthesis have been conclusively linked to many diseases but the complexity of glycosylation has hindered the analysis of glycan data in order to identify glycoforms contributing to disease. To overcome this limitation, we developed a quantitative N-glycosylation model that interprets and integrates mass spectral and transcriptomic data by incorporating key glycosylation enzyme activities. Using the cancer progression model of androgen-dependent to androgen-independent Lymph Node Carcinoma of the Prostate (LNCaP) cells, the N-glycosylation model identified and quantified glycan structural details not typically derived from single-stage mass spectral or gene expression data. Differences between the cell types uncovered include increases in H(II) and Le(y) epitopes, corresponding to greater activity of alpha 2-Fuc-transferase (FUT1) in the androgen-independent cells. The model further elucidated limitations in the two analytical platforms including a defect in the microarray for detecting the GnTV (MGAT5) enzyme. Our results demonstrate the potential of systems glycobiology tools for elucidating key glycan biomarkers and potential therapeutic targets. The integration of multiple data sets represents an important application of systems biology for understanding complex cellular processes. C1 [Bennun, Sandra V.; Betenbaugh, Michael J.; Krambeck, Frederick J.] Johns Hopkins Univ, Dept Chem & Biomol Engn, Baltimore, MD USA. [Bennun, Sandra V.; Krambeck, Frederick J.] ReacTech Inc, Alexandria, VA USA. [Yarema, Kevin J.] Johns Hopkins Univ, Dept Biomed Engn, Baltimore, MD USA. RP Bennun, SV (reprint author), Sandia Natl Labs, POB 5800, Albuquerque, NM 87185 USA. EM svbennun@gmail.com RI Betenbaugh, Michael J./A-3252-2010 OI Betenbaugh, Michael J./0000-0002-6336-4659 FU National Cancer Institute Awards [5R41CA127885-02, R01CA112314]; Consortium of Functional Glycomics; Bridging Grant [U54-GM062116-10] FX This work was supported by the National Cancer Institute Awards 5R41CA127885-02 and R01CA112314, and the Consortium of Functional Glycomics (http://www.functionalglycomics.org), Bridging Grant Number U54-GM062116-10. The funders had no role in study design, data collection and analysis, decision to publish, or preparation of the manuscript. NR 42 TC 21 Z9 21 U1 2 U2 8 PU PUBLIC LIBRARY SCIENCE PI SAN FRANCISCO PA 1160 BATTERY STREET, STE 100, SAN FRANCISCO, CA 94111 USA SN 1553-7358 J9 PLOS COMPUT BIOL JI PLoS Comput. Biol. PD JAN PY 2013 VL 9 IS 1 AR e1002813 DI 10.1371/journal.pcbi.1002813 PG 18 WC Biochemical Research Methods; Mathematical & Computational Biology SC Biochemistry & Molecular Biology; Mathematical & Computational Biology GA 085ED UT WOS:000314595600003 PM 23326219 ER PT J AU Nowak-Lovato, K Alexandrov, LB Banisadr, A Bauer, AL Bishop, AR Usheva, A Mu, FP Hong-Geller, E Rasmussen, KO Hlavacek, WS Alexandrov, BS AF Nowak-Lovato, Kristy Alexandrov, Ludmil B. Banisadr, Afsheen Bauer, Amy L. Bishop, Alan R. Usheva, Anny Mu, Fangping Hong-Geller, Elizabeth Rasmussen, Kim O. Hlavacek, William S. Alexandrov, Boian S. TI Binding of Nucleoid-Associated Protein Fis to DNA Is Regulated by DNA Breathing Dynamics SO PLOS COMPUTATIONAL BIOLOGY LA English DT Article ID CARCINOGENIC LESION O-6-METHYLGUANINE; GLOBAL GENE-EXPRESSION; GENOME-WIDE ANALYSIS; ESCHERICHIA-COLI; TRANSCRIPTION-FACTOR; BASAL TRANSCRIPTION; SEQUENCE; SITES; INITIATION; DENATURATION AB Physicochemical properties of DNA, such as shape, affect protein-DNA recognition. However, the properties of DNA that are most relevant for predicting the binding sites of particular transcription factors (TFs) or classes of TFs have yet to be fully understood. Here, using a model that accurately captures the melting behavior and breathing dynamics (spontaneous local openings of the double helix) of double-stranded DNA, we simulated the dynamics of known binding sites of the TF and nucleoid-associated protein Fis in Escherichia coli. Our study involves simulations of breathing dynamics, analysis of large published in vitro and genomic datasets, and targeted experimental tests of our predictions. Our simulation results and available in vitro binding data indicate a strong correlation between DNA breathing dynamics and Fis binding. Indeed, we can define an average DNA breathing profile that is characteristic of Fis binding sites. This profile is significantly enriched among the identified in vivo E. coli Fis binding sites. To test our understanding of how Fis binding is influenced by DNA breathing dynamics, we designed base-pair substitutions, mismatch, and methylation modifications of DNA regions that are known to interact (or not interact) with Fis. The goal in each case was to make the local DNA breathing dynamics either closer to or farther from the breathing profile characteristic of a strong Fis binding site. For the modified DNA segments, we found that Fis-DNA binding, as assessed by gel-shift assay, changed in accordance with our expectations. We conclude that Fis binding is associated with DNA breathing dynamics, which in turn may be regulated by various nucleotide modifications. C1 [Nowak-Lovato, Kristy; Banisadr, Afsheen; Hong-Geller, Elizabeth] Los Alamos Natl Lab, Biosci Div, Los Alamos, NM USA. [Alexandrov, Ludmil B.] Wellcome Trust Sanger Inst, Canc Genome Project, Cambridge, England. [Bauer, Amy L.] Los Alamos Natl Lab, X Theoret Design Div, Los Alamos, NM USA. [Bishop, Alan R.; Mu, Fangping; Rasmussen, Kim O.; Hlavacek, William S.; Alexandrov, Boian S.] Los Alamos Natl Lab, Div Theoret, Los Alamos, NM USA. [Usheva, Anny] Harvard Univ, Beth Israel Deaconess Med Ctr, Sch Med, Boston, MA 02215 USA. RP Nowak-Lovato, K (reprint author), Los Alamos Natl Lab, Biosci Div, Los Alamos, NM USA. EM wish@lanl.gov; boian@lanl.gov RI Rasmussen, Kim/B-5464-2009; Alexandrov, Boian/D-2488-2010; Alexandrov, Ludmil/B-6582-2014; OI Rasmussen, Kim/0000-0002-4029-4723; Alexandrov, Boian/0000-0001-8636-4603; Alexandrov, Ludmil/0000-0003-3596-4515; Hlavacek, William/0000-0003-4383-8711 FU National Nuclear Security Administration of the US Department of Energy at Los Alamos National Laboratory [DE-AC52-06NA25396] FX This work was carried out under the auspices of the National Nuclear Security Administration of the US Department of Energy at Los Alamos National Laboratory under Contract No. DE-AC52-06NA25396. The funders had no role in study design, data collection and analysis, decision to publish, or preparation of the manuscript. NR 99 TC 12 Z9 12 U1 0 U2 25 PU PUBLIC LIBRARY SCIENCE PI SAN FRANCISCO PA 1160 BATTERY STREET, STE 100, SAN FRANCISCO, CA 94111 USA SN 1553-7358 J9 PLOS COMPUT BIOL JI PLoS Comput. Biol. PD JAN PY 2013 VL 9 IS 1 AR e1002881 DI 10.1371/journal.pcbi.1002881 PG 14 WC Biochemical Research Methods; Mathematical & Computational Biology SC Biochemistry & Molecular Biology; Mathematical & Computational Biology GA 085ED UT WOS:000314595600036 PM 23341768 ER PT J AU Condon, BJ Leng, YQ Wu, DL Bushley, KE Ohm, RA Otillar, R Martin, J Schackwitz, W Grimwood, J MohdZainudin, N Xue, CS Wang, R Manning, VA Dhillon, B Tu, ZJ Steffenson, BJ Salamov, A Sun, H Lowry, S LaButti, K Han, J Copeland, A Lindquist, E Barry, K Schmutz, J Baker, SE Ciuffetti, LM Grigoriev, IV Zhong, S Turgeon, BG AF Condon, Bradford J. Leng, Yueqiang Wu, Dongliang Bushley, Kathryn E. Ohm, Robin A. Otillar, Robert Martin, Joel Schackwitz, Wendy Grimwood, Jane MohdZainudin, NurAinIzzati Xue, Chunsheng Wang, Rui Manning, Viola A. Dhillon, Braham Tu, Zheng Jin Steffenson, Brian J. Salamov, Asaf Sun, Hui Lowry, Steve LaButti, Kurt Han, James Copeland, Alex Lindquist, Erika Barry, Kerrie Schmutz, Jeremy Baker, Scott E. Ciuffetti, Lynda M. Grigoriev, Igor V. Zhong, Shaobin Turgeon, B. Gillian TI Comparative Genome Structure, Secondary Metabolite, and Effector Coding Capacity across Cochliobolus Pathogens SO PLOS GENETICS LA English DT Article ID NONRIBOSOMAL PEPTIDE SYNTHETASES; HOST-SELECTIVE TOXINS; POLYKETIDE VIRULENCE FACTOR; DISEASE-RESISTANCE GENE; RICE BLAST FUNGUS; HC-TOXIN; T-TOXIN; VICTORIN SENSITIVITY; ELECTROPHORETIC KARYOTYPE; LEPTOSPHAERIA-MACULANS AB The genomes of five Cochliobolus heterostrophus strains, two Cochliobolus sativus strains, three additional Cochliobolus species (Cochliobolus victoriae, Cochliobolus carbonum, Cochliobolus miyabeanus), and closely related Setosphaeria turcica were sequenced at the Joint Genome Institute (JGI). The datasets were used to identify SNPs between strains and species, unique genomic regions, core secondary metabolism genes, and small secreted protein (SSP) candidate effector encoding genes with a view towards pinpointing structural elements and gene content associated with specificity of these closely related fungi to different cereal hosts. Whole-genome alignment shows that three to five percent of each genome differs between strains of the same species, while a quarter of each genome differs between species. On average, SNP counts among field isolates of the same C. heterostrophus species are more than 25x higher than those between inbred lines and 50x lower than SNPs between Cochliobolus species. The suites of nonribosomal peptide synthetase (NRPS), polyketide synthase (PKS), and SSP-encoding genes are astoundingly diverse among species but remarkably conserved among isolates of the same species, whether inbred or field strains, except for defining examples that map to unique genomic regions. Functional analysis of several strain-unique PKSs and NRPSs reveal a strong correlation with a role in virulence. C1 [Condon, Bradford J.; Wu, Dongliang; MohdZainudin, NurAinIzzati; Xue, Chunsheng; Turgeon, B. Gillian] Cornell Univ, Dept Plant Pathol & Plant Microbe Biol, Ithaca, NY 14850 USA. [Leng, Yueqiang; Wang, Rui; Zhong, Shaobin] N Dakota State Univ, Dept Plant Pathol, Fargo, ND 58105 USA. [Bushley, Kathryn E.; Manning, Viola A.; Ciuffetti, Lynda M.] Oregon State Univ, Dept Bot & Plant Pathol, Corvallis, OR 97331 USA. [Ohm, Robin A.; Otillar, Robert; Martin, Joel; Schackwitz, Wendy; Salamov, Asaf; Sun, Hui; Lowry, Steve; LaButti, Kurt; Han, James; Copeland, Alex; Lindquist, Erika; Barry, Kerrie; Schmutz, Jeremy; Grigoriev, Igor V.] US Dept Energy DOE, Joint Genome Inst JGI, Walnut Creek, CA USA. [Grimwood, Jane; Schmutz, Jeremy] HudsonAlpha Inst Biotechnol, Huntsville, AL USA. [MohdZainudin, NurAinIzzati] Univ Putra Malaysia, Dept Biol, Fac Sci, Serdang, Selangor, Malaysia. [Xue, Chunsheng] Shenyang Agr Univ, Coll Plant Protect, Shenyang, Peoples R China. [Dhillon, Braham] Univ British Columbia, Dept Forest Sci, Vancouver, BC V6T 1W5, Canada. [Tu, Zheng Jin] Univ Minnesota, Supercomp Inst Adv Computat Res, Minneapolis, MN USA. [Steffenson, Brian J.] Univ Minnesota, Dept Plant Pathol, St Paul, MN USA. [Baker, Scott E.] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Condon, BJ (reprint author), Cornell Univ, Dept Plant Pathol & Plant Microbe Biol, Ithaca, NY 14850 USA. EM shaobin.zhong@ndsu.edu; bgt1@cornell.edu RI Ohm, Robin/I-6689-2016; OI Condon, Bradford/0000-0003-4377-9205; Mohd Zainudin, Nur Ain Izzati/0000-0002-4648-1503; Steffenson, Brian/0000-0001-7961-5363 FU Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]; Triticeae-CAP project from the USDA National Institute of Food and Agriculture [2011-68002-30029]; Lieberman-Okinow Endowment of the University of Minnesota FX The work conducted by the U.S. Department of Energy Joint Genome Institute is supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. Partial support is provided by the Triticeae-CAP project (2011-68002-30029) from the USDA National Institute of Food and Agriculture to SZ and the Lieberman-Okinow Endowment of the University of Minnesota to BJS. The funders had no role in study design, data collection and analysis, decision to publish, or preparation of the manuscript. NR 123 TC 48 Z9 58 U1 3 U2 75 PU PUBLIC LIBRARY SCIENCE PI SAN FRANCISCO PA 1160 BATTERY STREET, STE 100, SAN FRANCISCO, CA 94111 USA SN 1553-7404 J9 PLOS GENET JI PLoS Genet. PD JAN PY 2013 VL 9 IS 1 AR e1003233 DI 10.1371/journal.pgen.1003233 PG 29 WC Genetics & Heredity SC Genetics & Heredity GA 085YZ UT WOS:000314651500070 PM 23357949 ER PT J AU Shi, WB Xie, SX Chen, XY Sun, S Zhou, X Liu, LT Gao, P Kyrpides, NC No, EG Yuan, JS AF Shi, Weibing Xie, Shangxian Chen, Xueyan Sun, Su Zhou, Xin Liu, Lantao Gao, Peng Kyrpides, Nikos C. No, En-Gyu Yuan, Joshua S. TI Comparative Genomic Analysis of the Endosymbionts of Herbivorous Insects Reveals Eco-Environmental Adaptations: Biotechnology Applications SO PLOS GENETICS LA English DT Article ID TERMITE RETICULITERMES-FLAVIPES; PROTEIN FAMILIES DATABASE; PHOSPHOTRANSFERASE SYSTEM; CLOSTRIDIUM-LJUNGDAHLII; BACTERIAL ENDOSYMBIONT; ABC TRANSPORTERS; GUT; SYMBIONTS; GENE; EVOLUTION AB Metagenome analysis of the gut symbionts of three different insects was conducted as a means of comparing taxonomic and metabolic diversity of gut microbiomes to diet and life history of the insect hosts. A second goal was the discovery of novel biocatalysts for biorefinery applications. Grasshopper and cutworm gut symbionts were sequenced and compared with the previously identified metagenome of termite gut microbiota. These insect hosts represent three different insect orders and specialize on different food types. The comparative analysis revealed dramatic differences among the three insect species in the abundance and taxonomic composition of the symbiont populations present in the gut. The composition and abundance of symbionts was correlated with their previously identified capacity to degrade and utilize the different types of food consumed by their hosts. The metabolic reconstruction revealed that the gut metabolome of cutworms and grasshoppers was more enriched for genes involved in carbohydrate metabolism and transport than wood-feeding termite, whereas the termite gut metabolome was enriched for glycosyl hydrolase (GH) enzymes relevant to lignocellulosic biomass degradation. Moreover, termite gut metabolome was more enriched with nitrogen fixation genes than those of grasshopper and cutworm gut, presumably due to the termite's adaptation to the high fiber and less nutritious food types. In order to evaluate and exploit the insect symbionts for biotechnology applications, we cloned and further characterized four biomass-degrading enzymes including one endoglucanase and one xylanase from both the grasshopper and cutworm gut symbionts. The results indicated that the grasshopper symbiont enzymes were generally more efficient in biomass degradation than the homologous enzymes from cutworm symbionts. Together, these results demonstrated a correlation between the composition and putative metabolic functionality of the gut microbiome and host diet, and suggested that this relationship could be exploited for the discovery of symbionts and biocatalysts useful for biorefinery applications. C1 [Shi, Weibing; Xie, Shangxian; Sun, Su; Liu, Lantao; Gao, Peng; Yuan, Joshua S.] Texas A&M Univ, Dept Plant Pathol & Microbiol, College Stn, TX 77843 USA. [Shi, Weibing; Xie, Shangxian; Chen, Xueyan; Sun, Su; Zhou, Xin; Liu, Lantao; Gao, Peng; No, En-Gyu; Yuan, Joshua S.] Texas A&M Univ, Inst Plant Genom & Biotechnol, College Stn, TX USA. [Xie, Shangxian] Huazhong Univ Sci & Technol, Sch Life Sci & Technol, Wuhan 430074, Hubei, Peoples R China. [Chen, Xueyan] Texas A&M Univ, Dept Vet Pathol, College Stn, TX 77843 USA. [Kyrpides, Nikos C.] DOE Joint Genomes Inst, Walnut Creek, CA USA. RP Shi, WB (reprint author), Texas A&M Univ, Dept Plant Pathol & Microbiol, College Stn, TX 77843 USA. EM syuan@tamu.edu RI Xie, Shangxian/P-7175-2016; Kyrpides, Nikos/A-6305-2014 OI Kyrpides, Nikos/0000-0002-6131-0462 FU SouthCentral Sungrant; Texas Agrilife Bioenergy Research Initiative FX The research is funded by SouthCentral Sungrant and Texas Agrilife Bioenergy Research Initiative. The funders had no role in study design, data collection and analysis, decision to publish, or preparation of the manuscript. NR 92 TC 17 Z9 17 U1 2 U2 71 PU PUBLIC LIBRARY SCIENCE PI SAN FRANCISCO PA 1160 BATTERY STREET, STE 100, SAN FRANCISCO, CA 94111 USA SN 1553-7404 J9 PLOS GENET JI PLoS Genet. PD JAN PY 2013 VL 9 IS 1 AR e1003131 DI 10.1371/journal.pgen.1003131 PG 12 WC Genetics & Heredity SC Genetics & Heredity GA 085YZ UT WOS:000314651500006 PM 23326236 ER PT J AU Price, AD Huber, DL AF Price, Andrew D. Huber, Dale L. TI Controlled polymer monolayer synthesis by radical transfer to surface immobilized transfer agents SO POLYMER CHEMISTRY LA English DT Article ID SELF-ASSEMBLED MONOLAYERS; CHAIN-TRANSFER; MOLECULAR-WEIGHT; SOLID SUBSTRATE; SILICA; BRUSHES; GLASS; MICROARRAYS; ADSORPTION; STYRENE AB Radical chain transfer from solution-generated free radicals to thiol transfer agents bound to the surfaces of planar silicon and silica particles was investigated as a method to generate surface-bound polymer brushes. Both conventional radical and reversible addition-fragmentation chain transfer (RAFT) polymerizations created polymer films with molecular weights dependent on the details of the reaction. In the presence of high free radical concentrations or RAFT agent modifiers, the surface had minimal influence on the growth of grafted polymer chains following the initial radical transfer to the surface. Notably, excellent control of film thickness was achieved in the absence of surface-bound initiators or RAFT agents, thereby simplifying the synthesis of immobilized brush architectures. On the other hand, low concentrations of solution free radicals in conventional radical polymerization generated grafted polymers with lengths varying considerably from polymers in solution. Despite the simplicity and versatility of this technique for creating polymer-modified surfaces by surface initiated polymerization (SIP), it has been under-utilized; likely due to the absence of a framework for the rational design of the brush. The details of this investigation should allow surface modification by polymer films to become accessible to researchers without the need to create complex precursor surface chemistries. C1 [Price, Andrew D.; Huber, Dale L.] Sandia Natl Labs, Ctr Integrated Nanotechnol, Albuquerque, NM 87185 USA. RP Huber, DL (reprint author), Sandia Natl Labs, Ctr Integrated Nanotechnol, POB 5800, Albuquerque, NM 87185 USA. EM Dale.Huber@sandia.gov RI Huber, Dale/A-6006-2008 OI Huber, Dale/0000-0001-6872-8469 FU Division of Materials Sciences and Engineering, Office of Basic Energy Sciences, United States Department of Energy; U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX This work was supported by the Division of Materials Sciences and Engineering, Office of Basic Energy Sciences, United States Department of Energy. 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 35 TC 2 Z9 2 U1 3 U2 45 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1759-9954 J9 POLYM CHEM-UK JI Polym. Chem. PY 2013 VL 4 IS 5 BP 1565 EP 1574 DI 10.1039/c2py20955a PG 10 WC Polymer Science SC Polymer Science GA 083PZ UT WOS:000314478800033 ER PT J AU Yang, ZB Chen, T He, RX Li, HP Lin, HJ Li, L Zou, GF Jia, QX Peng, HS AF Yang, Zhibin Chen, Tao He, Ruixuan Li, Houpu Lin, Huijuan Li, Li Zou, Guifu Jia, Quanxi Peng, Huisheng TI A novel carbon nanotube/polymer composite film for counter electrodes of dye-sensitized solar cells SO POLYMER CHEMISTRY LA English DT Article ID POLYMER NANOCOMPOSITES; NANOTUBES; FIBERS; FABRICATION AB In the development of optoelectronic and electronic devices, it is critically important, but remains challenging to discover new electrode materials to replace the conventional indium and platinum which have obvious disadvantages including high cost, complex fabrication, and chemical instability during the use. To this end, carbon nanotube (CNT)/polymer composite materials may represent one of the most promising candidates due to the combined advantages including high surface area, excellent electrical and electrocatalytic properties, and high stability from CNTs while good flexibility, abundant supply, and easy fabrication from polymers. In the current composite electrodes, however, CNTs are typically interconnected to form networks, and the generated charges have to hop through a lot of boundaries among CNTs. The resulting organic solar cells based on the CNT/polymer composite electrodes showed low efficiencies. Here we have developed a perpendicularly aligned and penetrated CNT/polymer composite film through a simple slicing technique. This novel composite film exhibits good transparency, high flexibility, excellent electrical conductivity, and remarkable electrocatalytic activity, and may be widely used for various electrode materials. As a demonstration, it was used as a counter electrode to fabricate dye-sensitized solar cells with high efficiency. C1 [Yang, Zhibin; Chen, Tao; He, Ruixuan; Li, Houpu; Lin, Huijuan; Li, Li; Peng, Huisheng] Fudan Univ, State Key Lab Mol Engn Polymers, Dept Macromol Sci, Shanghai 200438, Peoples R China. [Yang, Zhibin; Chen, Tao; He, Ruixuan; Li, Houpu; Lin, Huijuan; Li, Li; Peng, Huisheng] Fudan Univ, Adv Mat Lab, Shanghai 200438, Peoples R China. [Zou, Guifu; Jia, Quanxi] Los Alamos Natl Lab, Ctr Integrated Nanotechnol, Los Alamos, NM 87545 USA. RP Peng, HS (reprint author), Fudan Univ, State Key Lab Mol Engn Polymers, Dept Macromol Sci, Shanghai 200438, Peoples R China. EM penghs@fudan.edu.cn RI ZOU, GUIFU/C-8498-2011; Jia, Q. X./C-5194-2008; Yang, Zhibin/F-6212-2015; Peng, Huisheng/G-8867-2011 OI Yang, Zhibin/0000-0003-4036-9446; FU NSFC [20904006, 91027025]; MOST [2011CB932503, 2011DFA51330]; STCSM [1052nm01600, 11520701400]; MOE [NCET-09-0318]; Li Foundation Heritage Prize; Fudan University; Los Alamos National Security, LLC for the National Nuclear Security Administration of the U.S. Department of Energy [DE-AC52-06NA25396] FX This work was supported by NSFC (20904006, 91027025), MOST (2011CB932503, 2011DFA51330), STCSM (1052nm01600, 11520701400), MOE (NCET-09-0318), Li Foundation Heritage Prize, and Fudan University. The work at Los Alamos was performed 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 36 TC 15 Z9 15 U1 3 U2 71 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 2013 VL 4 IS 5 BP 1680 EP 1684 DI 10.1039/c2py21021e PG 5 WC Polymer Science SC Polymer Science GA 083PZ UT WOS:000314478800046 ER PT J AU Boggs, MA Islam, M Dong, W Wall, NA AF Boggs, M. A. Islam, M. Dong, W. Wall, N. A. TI Complexation of Tc(IV) with EDTA at varying ionic strength of NaCl SO RADIOCHIMICA ACTA LA English DT Article DE Technetium; EDTA; Complexation; Solvent extraction; PHREEQC ID ORGANIC-LIGANDS; TECHNETIUM(IV); PERTECHNETATE; REDUCTION; SOLUBILITY; CHEMISTRY; COLLOIDS; FE(II); WASTE; OXIDE AB The stability constant for Tc(IV)/EDTA complexes were determined using a solvent extraction technique at varying ionic strength (NaCl) and the specific ion interaction theory model allowed for calculating stability constants at zero ionic strength. The stability constants at zero ionic strength for the formation of the TcOEDTA(2-) and TcOHEDTA(-) complexes are 10(20.0 +/- 0.4) and 10(25.3 +/- 0.5), respectively. The modeled Tc(IV) solubility was calculated to be 3.9 x 10(-7) M at near-neutral pH and in presence of 2.5 mM EDTA, a result found to be in good agreement with published solubility experimental data. Speciation calculations showed that TcOEDTA(2-) is the predominant species between pH 4 and 7.5 in presence of 0.171 mM EDTA, while TcO(OH)(2)(0) is predominant in basic solution. These studies show that EDTA has a very strong affinity for complexation with Tc(IV) and can increase the environmental mobility of Tc(IV). C1 [Boggs, M. A.; Islam, M.; Wall, N. A.] Washington State Univ, Dept Chem, Pullman, WA 99164 USA. [Dong, W.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Wall, NA (reprint author), Washington State Univ, Dept Chem, Pullman, WA 99164 USA. EM nawall@wsu.edu RI Boggs, Mark/I-6954-2012; Dong, Wenming/G-3221-2015 OI Dong, Wenming/0000-0003-2074-8887 FU US DOE (Office of the Biological and Environmental Research, Office of Science) [DE-FG02-08ER64696]; US NRC [NRC3808953] FX The authors wish to thank Cytec Industries for the opportunity to use Cyanex 272. This work was supported by the US DOE (Office of the Biological and Environmental Research, Office of Science) under the grant DE-FG02-08ER64696 and by the US NRC under the grant NRC3808953. NR 31 TC 6 Z9 7 U1 3 U2 26 PU OLDENBOURG VERLAG PI MUNICH PA LEKTORAT MINT, POSTFACH 80 13 60, D-81613 MUNICH, GERMANY SN 0033-8230 J9 RADIOCHIM ACTA JI Radiochim. Acta PY 2013 VL 101 IS 1 BP 13 EP 18 DI 10.1524/ract.2013.2000 PG 6 WC Chemistry, Inorganic & Nuclear; Nuclear Science & Technology SC Chemistry; Nuclear Science & Technology GA 085NE UT WOS:000314620700003 ER PT J AU Devanathan, R Gao, F Sundgren, CJ AF Devanathan, Ram Gao, Fei Sundgren, Christina J. TI Role of cation choice in the radiation tolerance of pyrochlores SO RSC ADVANCES LA English DT Article ID MOLECULAR-DYNAMICS SIMULATIONS; HEAVY-ION IRRADIATION; STRUCTURAL MODIFICATIONS; PHASE-TRANSITIONS; OXIDES; DISORDER; DAMAGE; AMORPHIZATION; ACTINIDES; MIGRATION AB We have used atomistic computer simulations to study anion diffusion coefficients and the response to swift heavy ion irradiation of Gd2TixZr2-xO7 pyrochlore for x values of 0, 0.5, 1, 1.5 and 2. In Gd2Ti2O7, a thermal energy deposition per unit length of 12 keV nm(-1) results in a cylindrical amorphous track of radius 2 nm in good agreement with experiment. The volume swelling of the track is 4%, which suggests that it is partially amorphous. Gd vacancies and Ti interstitials along with cation exchange play a role in damage accumulation in the titanate. In sharp contrast, Gd2Zr2O7 does not swell and merely transforms from pyrochlore to fluorite under the same conditions. The activation energy barrier for oxygen hopping by the vacancy mechanism in these pyrochlores is 0.26-0.44 eV. The radiation tolerance of gadolinium zirconate pyrochlore is related to the efficient annihilation of cation Frenkel pairs, the low energy cost and negligible volume expansion associated with the resulting cation exchange, and efficient annealing of anion sublattice damage. C1 [Devanathan, Ram; Gao, Fei; Sundgren, Christina J.] Pacific NW Natl Lab, Div Phys Sci, Richland, WA 99352 USA. RP Devanathan, R (reprint author), Pacific NW Natl Lab, Div Phys Sci, MS K2-01, Richland, WA 99352 USA. EM ram.devanathan@pnnl.gov RI Devanathan, Ram/C-7247-2008 OI Devanathan, Ram/0000-0001-8125-4237 FU Materials Science and Engineering Division, Office of Basic Energy Sciences, US Department of Energy (DOE) [DE-AC05-76RL01830]; DOE Summer Undergraduate Laboratory Internship Program; DOE's Office of Biological and Environmental Research; Office of Science of the DOE [DE-AC02-05CH11231] FX This work was supported by the Materials Science and Engineering Division, Office of Basic Energy Sciences, US Department of Energy (DOE) under Contract DE-AC05-76RL01830. Christina J. Sundgren was supported by the DOE Summer Undergraduate Laboratory Internship Program. This research was performed using Environmental Molecular Sciences Laboratory, a national scientific user facility sponsored by DOE's Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory. This work used resources of the National Energy Research Scientific Computing Center, which is supported by the Office of Science of the DOE under Contract No. DE-AC02-05CH11231. NR 41 TC 11 Z9 11 U1 6 U2 46 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 2013 VL 3 IS 9 BP 2901 EP 2909 DI 10.1039/c2ra22745b PG 9 WC Chemistry, Multidisciplinary SC Chemistry GA 083OZ UT WOS:000314475700008 ER PT J AU Thomasson, A Ibrahim, F Lefevre, C Autissier, E Roulland, F Meny, C Leuvrey, C Choi, S Jo, W Cregut, O Versini, G Barre, S Alouani, M Viart, N AF Thomasson, Alexandre Ibrahim, Fatima Lefevre, Christophe Autissier, Emmanuel Roulland, Francois Meny, Christian Leuvrey, Cedric Choi, Sukgeun Jo, William Cregut, Olivier Versini, Gilles Barre, Sophie Alouani, Mebarek Viart, Nathalie TI Effects of iron concentration and cationic site disorder on the optical properties of magnetoelectric gallium ferrite thin films SO RSC ADVANCES LA English DT Article ID SOLID-STATE REACTION; MULTIFERROIC GAFEO3; MAGNETIC-PROPERTIES; GEL AB Room-temperature dielectric function epsilon = epsilon(1) + i epsilon(2) spectra of magnetoelectric Ga2-xFexO3 (x = 0.9, 1.0, and 1.4) thin films are determined by spectroscopic ellipsometry (SE) as a function of Fe concentration x. The SE data are analysed by a multilayer model with a series of Tauc-Lorentz oscillators. While the threshold energies slightly decrease as x increases, the oscillator strength shows a strong composition-dependence for the major optical structure at similar to 3.5 eV. The experimental data are compared to the epsilon spectra obtained by density functional theory ( DFT) calculations. Even though the overall shape of epsilon spectra is consistent, the experimental data and calculated spectra show a clear discrepancy in the oscillator's strength ratio of the two optical structures at similar to 3.5 and similar to 6.0 eV. The DFT calculations suggest that a significant disordering in the cationic (Ga and Fe) sites in Ga2-xFexO3 is present in thin films, which influences their optical properties. This work demonstrates a successful application of optical characterization for determining the cationic sites occupation in thin films, which in turn improves our understanding of Physics and Chemistry in Ga2-xFexO3 thin films and paves a pathway to the development of new multifunctional devices. C1 [Thomasson, Alexandre; Ibrahim, Fatima; Lefevre, Christophe; Autissier, Emmanuel; Roulland, Francois; Meny, Christian; Leuvrey, Cedric; Cregut, Olivier; Versini, Gilles; Barre, Sophie; Alouani, Mebarek; Viart, Nathalie] Inst Phys & Chim Mat Strasbourg, UMR CNRS UdS 7504, F-67034 Strasbourg 2, France. [Choi, Sukgeun] Natl Renewable Energy Lab, Golden, CO 80401 USA. [Jo, William] Ewha Womans Univ, Dept Phys, Seoul 120750, South Korea. RP Thomasson, A (reprint author), Inst Phys & Chim Mat Strasbourg, UMR CNRS UdS 7504, 23 Rue Loess,BP 43, F-67034 Strasbourg 2, France. EM Sukgeun.Choi@nrel.gov; wmjo@ewha.ac.kr; viart@unistra.fr RI Choi, Sukgeun/J-2345-2014; OI Lefevre, Christophe/0000-0002-2962-3426; Viart, Nathalie/0000-0002-7851-017X FU international ANR DFG Chemistry project GALIMEO [2011-INTB-1006-01]; CNRS - PICS program [5733]; HPC resources from GENCI-CINES Grant [2012-gem1100]; U.S. Department of Energy [DE-AC36-08-GO28308] FX This work has been carried out in the framework of the French-Korean International Laboratory "CNRS-EWHA Research Center for Ultrafast Optics and Nanoelectronics of Functional Nanostructures''. It was done with the financial support from the international ANR DFG Chemistry project GALIMEO #2011-INTB-1006-01 and from the CNRS - PICS program 5733. The calculations were performed using HPC resources from GENCI-CINES Grant 2012-gem1100. The work done at NREL was supported by the U.S. Department of Energy under Contract no. DE-AC36-08-GO28308. The authors wish to thank Guillaume Rogez and Jonathan Alaria for their help in preliminary optical measurements. NR 33 TC 6 Z9 6 U1 1 U2 39 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 2013 VL 3 IS 9 BP 3124 EP 3130 DI 10.1039/c2ra22681b PG 7 WC Chemistry, Multidisciplinary SC Chemistry GA 083OZ UT WOS:000314475700034 ER PT J AU Kim, D Hong, S Li, D Roh, HS Ahn, G Kim, J Park, M Hong, J Sung, TH No, K AF Kim, Dongjin Hong, Seungbum Li, Dongjun Roh, Hee Seok Ahn, Gun Kim, Jiyoon Park, Moonkyu Hong, Jongin Sung, Tae-hyun No, Kwangsoo TI A spring-type piezoelectric energy harvester SO RSC ADVANCES LA English DT Article ID VINYLIDENE FLUORIDE; TRIFLUOROETHYLENE COPOLYMER; GENERATING ELECTRICITY; FILMS; PIEZORESPONSE; CRYSTALLINE; WALKING AB We developed a three-dimensional spring-type piezoelectric energy harvester using a dip-coating method and multi-directional electrode deposition. The energy harvester consists of a bi-layered structure composed of a surface electrode and a ferroelectric polymer, on a conventional spring which has two roles - the core electrode and the mechanical substrate for the ferroelectric polymer. The energy harvester generated an output voltage of up to 88 mV as a function of cycling compression stress, which leads to a piezoelectric constant of 28.55 pC N-1 for unpoled P(VDF-TrFE) films. Since the spring structure significantly decreases the resonance frequency of the harvester, the spring-type energy harvester can effectively generate electricity using low-frequency vibration energy abundant in the nature. C1 [Kim, Dongjin; Hong, Seungbum; Li, Dongjun; Ahn, Gun; Kim, Jiyoon; Park, Moonkyu; No, Kwangsoo] Korea Adv Inst Sci & Technol, Dept Mat Sci & Engn, Taejon 305701, South Korea. [Kim, Dongjin; Hong, Seungbum] Argonne Natl Lab, Div Mat Sci, Argonne, IL 60439 USA. [Roh, Hee Seok] Argonne Natl Lab, Nucl Engn Div, Argonne, IL 60439 USA. [Hong, Jongin] Chung Ang Univ, Dept Chem, Seoul 156756, South Korea. [Sung, Tae-hyun] Hanyang Univ, Dept Elect Engn, Seoul 133791, South Korea. RP Kim, D (reprint author), Korea Adv Inst Sci & Technol, Dept Mat Sci & Engn, Taejon 305701, South Korea. EM seungbum@kaist.ac.kr; ksno@kaist.ac.kr RI Kim, Dongjin/B-5624-2012; Hong, Jongin/B-4504-2009; No, Kwangsoo/C-1983-2011; Hong, Seungbum/B-7708-2009 OI Hong, Jongin/0000-0002-2891-5785; Hong, Seungbum/0000-0002-2667-1983 FU Mid-career Researcher Program through the National Research Foundation of Korea (NRF) [2010-0015063]; Conversion Research Center Program through the National Research Foundation of Korea (NRF) [2011K000674]; Ministry of Education, Science and Technology (MEST); New & Renewable Energy of the Korea Institute of Energy Technology Evaluation and Planning (KETEP) grant [20103020060010]; Ministry of Knowledge Economy, Korea; UChicago Argonne; U.S. DOE Office of Science Laboratory [DE-AC02-06CH11357] FX This research was supported by the Mid-career Researcher Program (No. 2010-0015063) and Conversion Research Center Program (No. 2011K000674) through the National Research Foundation of Korea (NRF) funded by the Ministry of Education, Science and Technology (MEST) and the New & Renewable Energy of the Korea Institute of Energy Technology Evaluation and Planning (KETEP) grant (No. 20103020060010) funded by the Ministry of Knowledge Economy, Korea. Work at Argonne National Laboratory (S. H. and D. K., data analysis and writing of manuscript) was supported by UChicago Argonne, a U.S. DOE Office of Science Laboratory, operated under Contract No. DE-AC02-06CH11357. J. H. acknowledges the Chung-Ang University Research Grants in 2011. NR 29 TC 15 Z9 15 U1 0 U2 40 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 2013 VL 3 IS 10 BP 3194 EP 3198 DI 10.1039/c2ra22554a PG 5 WC Chemistry, Multidisciplinary SC Chemistry GA 086QR UT WOS:000314701800005 ER PT J AU Oikawa, A Lund, CH Sakuragi, Y Scheller, HV AF Oikawa, Ai Lund, Christian Have Sakuragi, Yumiko Scheller, Henrik V. TI Golgi-localized enzyme complexes for plant cell wall biosynthesis SO TRENDS IN PLANT SCIENCE LA English DT Review ID PROTEIN-PROTEIN INTERACTIONS; GLYCOSYLTRANSFERASE FAMILY 8; IN-VIVO; ARABIDOPSIS; XYLAN; IDENTIFICATION; XYLOGLUCAN; DOMAIN; ALPHA-2,6-SIALYLTRANSFERASE; EVOLUTION AB The plant cell wall mostly comprises complex glycans, which are synthesized by numerous enzymes located in the Golgi apparatus and plasma membrane. Protein protein interactions have been shown to constitute an important organizing principle for glycan biosynthetic enzymes in mammals and yeast Recent genetic and biochemical data also indicate that such interactions could be common in plant cell wall biosynthesis. In this review, we examine the new findings in protein protein interactions among plant cell wall biosynthetic enzymes and discuss the possibilities for enzyme complexes in the Golgi apparatus. These new insights in the field may contribute to novel strategies for molecular engineering of the cell wall. C1 [Oikawa, Ai; Scheller, Henrik V.] Joint BioEnergy Inst, Feedstocks Div, Emeryville, CA 94608 USA. [Oikawa, Ai; Scheller, Henrik V.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA 94720 USA. [Lund, Christian Have; Sakuragi, Yumiko] Univ Copenhagen, Dept Plant Biol & Biotechnol, DK-1871 Frederiksberg, Denmark. [Lund, Christian Have; Sakuragi, Yumiko] Villum Kann Rasmussen Res Ctr Proact Plants, DK-1871 Frederiksberg, Denmark. [Scheller, Henrik V.] Univ Calif Berkeley, Dept Plant & Microbial Biol, Berkeley, CA 94720 USA. RP Sakuragi, Y (reprint author), Univ Copenhagen, Dept Plant Biol & Biotechnol, DK-1871 Frederiksberg, Denmark. EM ysa@life.ku.dk; hscheller@lbl.gov RI Sakuragi, Yumiko/E-9707-2012; Scheller, Henrik/A-8106-2008 OI Sakuragi, Yumiko/0000-0002-9405-5197; Scheller, Henrik/0000-0002-6702-3560 FU US Department of Energy, Office of Science, Office of Biological and Environmental Research [AC02-05CH11231]; Lawrence Berkeley National Laboratory; Villum-Kann Rasmussen grant; Danish National Advanced Technology Foundation for the platform Biomass for the 21st Century [j. 001-2011-4]; European Union [256808] FX This work was funded by the US Department of Energy, Office of Science, Office of Biological and Environmental Research, through contract DE-AC02-05CH11231 with Lawrence Berkeley National Laboratory, by the Villum-Kann Rasmussen grant to the Pro-Active Plant Centre, by the Danish National Advanced Technology Foundation for the platform Biomass for the 21st Century (j. 001-2011-4), and by the European Union 7th Framework Programme (grant # 256808). NR 54 TC 30 Z9 30 U1 7 U2 73 PU ELSEVIER SCIENCE LONDON PI LONDON PA 84 THEOBALDS RD, LONDON WC1X 8RR, ENGLAND SN 1360-1385 J9 TRENDS PLANT SCI JI Trends Plant Sci. PD JAN PY 2013 VL 18 IS 1 BP 49 EP 58 DI 10.1016/j.tplants.2012.07.002 PG 10 WC Plant Sciences SC Plant Sciences GA 077BF UT WOS:000314002200007 PM 22925628 ER PT J AU Shvartsburg, AA Smith, RD AF Shvartsburg, Alexandre A. Smith, Richard D. TI High-Resolution Differential Ion Mobility Spectrometry of a Protein SO ANALYTICAL CHEMISTRY LA English DT Article ID GAS-PHASE SEPARATIONS; UBIQUITIN CONFORMERS; MASS SPECTROMETRY; CROSS-SECTIONS; FIELD; ANALYZERS; CONFORMATIONS; TEMPERATURE; DISTORTION AB Use of elevated electric fields and helium-rich gases has recently enabled differential ion mobility spectrometry (IMS) with a resolving power up to R 300. Here we applied that technique to a protein (ubiquitin), achieving R up to 80 and separating previously unresolved conformers. While still limited by conformational multiplicity, this resolution is some 4 times greater than that previously reported using either conventional (drift-tube or traveling-wave) or differential IMS. The capability for fine resolution of protein conformers may open new avenues for proteoform separations in top-down and intact-protein proteomics. C1 [Shvartsburg, Alexandre A.; Smith, Richard D.] Pacific NW Natl Lab, Div Biol Sci, Richland, WA 99352 USA. RP Shvartsburg, AA (reprint author), Pacific NW Natl Lab, Div Biol Sci, POB 999, Richland, WA 99352 USA. EM alexandre.shvartsburg@pnnl.gov RI Smith, Richard/J-3664-2012 OI Smith, Richard/0000-0002-2381-2349 FU NIH NIGMS [8 P41 GM103493-10]; U.S. Department of Energy Office of Biological and Environmental Research FX We thank Dr. Keqi Tang and Ron Moore for experimental help and Prof. David Clemmer for insightful discussions. This work was supported by NIH NIGMS (Grant 8 P41 GM103493-10) and the U.S. Department of Energy Office of Biological and Environmental Research and carried out in the Environmental Molecular Sciences Laboratory, a DOE national scientific user facility at PNNL. NR 34 TC 15 Z9 16 U1 2 U2 72 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 0003-2700 EI 1520-6882 J9 ANAL CHEM JI Anal. Chem. PD JAN 1 PY 2013 VL 85 IS 1 BP 10 EP 13 DI 10.1021/ac3029129 PG 4 WC Chemistry, Analytical SC Chemistry GA 065NZ UT WOS:000313156500003 PM 23244633 ER PT J AU McClintock, CS Hettich, RL AF McClintock, Carlee S. Hettich, Robert L. TI Experimental Approach to Controllably Vary Protein Oxidation While Minimizing Electrode Adsorption for Boron-Doped Diamond Electrochemical Surface Mapping Applications SO ANALYTICAL CHEMISTRY LA English DT Article ID INDUCED CONFORMATIONAL-CHANGES; MASS-SPECTROMETRY; CIRCULAR-DICHROISM; HYDROXYL RADICALS; CYSTEINE; REAGENT AB Oxidative protein surface mapping has become a powerful approach for measuring the solvent accessibility of folded protein structures. A variety of techniques exist for generating the key reagent (i.e., hydroxyl radicals) for these measurements; however, these approaches range significantly in their complexity and expense of operation. This research expands upon earlier work to enhance the controllability of boron-doped diamond (BDD) electrochemistry as an easily accessible tool for producing hydroxyl radicals in order to oxidize a range of intact proteins. Efforts to modulate the oxidation level while minimizing the adsorption of protein to the electrode involved the use of relatively high flow rates to reduce protein residence time inside the electrochemical flow chamber. Additionally, a different cell activation approach using variable voltage to supply a controlled current allowed us to precisely tune the extent of oxidation in a protein-dependent manner. In order to gain perspective on the level of protein adsorption onto the electrode surface, studies were conducted to monitor protein concentration during electrolysis and gauge changes in the electrode surface between cell activation events. This report demonstrates the successful use of BDD electrochemistry for greater precision in generating a target number of oxidation events upon intact proteins. C1 [McClintock, Carlee S.; Hettich, Robert L.] Univ Tennessee, Oak Ridge Natl Lab, Grad Sch Genome Sci & Technol, Oak Ridge, TN 37830 USA. [Hettich, Robert L.] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. RP Hettich, RL (reprint author), Univ Tennessee, Oak Ridge Natl Lab, Grad Sch Genome Sci & Technol, 1060 Commerce Pk, Oak Ridge, TN 37830 USA. EM hettichrl@ornl.gov RI Hettich, Robert/N-1458-2016 OI Hettich, Robert/0000-0001-7708-786X FU UTK-ORNL Graduate School of Genome Science and Technology; National Institutes of Health General Medicine Section [R0I-GM070754] FX The authors extend thanks to Dr. Vilmos Kertesz for providing electrochemical expertise. C.M. acknowledges financial support from the UTK-ORNL Graduate School of Genome Science and Technology. This research was supported by the National Institutes of Health General Medicine Section under Grant R0I-GM070754. Oak Ridge National Laboratory is managed by University of Tennessee Battelle LLC for the Department of Energy. NR 28 TC 5 Z9 5 U1 0 U2 25 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 0003-2700 J9 ANAL CHEM JI Anal. Chem. PD JAN 1 PY 2013 VL 85 IS 1 BP 213 EP 219 DI 10.1021/ac302418t PG 7 WC Chemistry, Analytical SC Chemistry GA 065NZ UT WOS:000313156500032 PM 23210708 ER PT J AU Ewing, RG Atkinson, DA Clowers, BH AF Ewing, Robert G. Atkinson, David A. Clowers, Brian H. TI Direct Real-Time Detection of RDX Vapors Under Ambient Conditions SO ANALYTICAL CHEMISTRY LA English DT Article ID REACTION-MASS-SPECTROMETRY; ION MOBILITY SPECTROMETRY; VOLATILE ORGANIC-COMPOUNDS; EXPLOSIVES DETECTION; CHEMICAL SENSORS; PTR-MS; POLYMERS; AIR AB The results in this manuscript represent a demonstration of RDX vapor detection in real time at ambient temperature without sample preconcentration. The detection of vapors from the low volatility explosive compound RDX was achieved through selective atmospheric pressure chemical ionization using nitrate reactant ions (NO3-) and NO3-center dot HNO3 adducts generated in an electrical discharge source. The RDX vapors were ionized in a reaction region, which provided a variable (up to several seconds) reaction time. The reaction times were controlled either by flow in an atmospheric flow tube (AFT) or by an electric field in an atmospheric drift tube (ADT). Both AFT and ADT were interfaced to a quadrupole mass spectrometer for ion detection and identification. Recorded signals were observed for RDX concentrations below 25 ppq using selected ion monitoring (SIM) of the RDX-nitrate adduct at m/z 284. C1 [Ewing, Robert G.; Atkinson, David A.; Clowers, Brian H.] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Ewing, RG (reprint author), Pacific NW Natl Lab, 902 Battelle Blvd, Richland, WA 99352 USA. EM robert.ewing@pnnl.gov FU Laboratory Directed Research and Development funding at the Pacific Northwest National Laboratory FX This work was funded in part by Laboratory Directed Research and Development funding at the 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 44 TC 19 Z9 19 U1 3 U2 87 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 0003-2700 J9 ANAL CHEM JI Anal. Chem. PD JAN 1 PY 2013 VL 85 IS 1 BP 389 EP 397 DI 10.1021/ac302828g PG 9 WC Chemistry, Analytical SC Chemistry GA 065NZ UT WOS:000313156500058 PM 23215531 ER PT J AU Kumar, R Klug, DD Ratcliffe, CI Tulk, CA Ripmeester, JA AF Kumar, Rajnish Klug, Dennis D. Ratcliffe, Christopher I. Tulk, Christopher A. Ripmeester, John A. TI Low-Pressure Synthesis and Characterization of Hydrogen-Filled Ice Ic SO ANGEWANDTE CHEMIE-INTERNATIONAL EDITION LA English DT Article DE clathrates; cubic ice; hydrates; hydrogen ID AMORPHOUS SOLID WATER; CLATHRATE HYDRATE; NEUTRON-DIFFRACTION; HIGH RESOLUTION; LIQUID; H-2; POLYMORPHS; SPECTRA; NMR; H2 C1 [Klug, Dennis D.; Ratcliffe, Christopher I.; Ripmeester, John A.] Natl Res Council Canada, Ottawa, ON K1A 0R6, Canada. [Kumar, Rajnish] CSIR Natl Chem Lab, Chem Engn & Proc Dev Div, Pune 411008, Maharashtra, India. [Tulk, Christopher A.] Oak Ridge Natl Lab, Neutron Scattering Sci Div, Oak Ridge, TN 37831 USA. RP Ripmeester, JA (reprint author), Natl Res Council Canada, 100 Sussex Dr, Ottawa, ON K1A 0R6, Canada. EM john.ripmeester@nrc-cnrc.gc.ca RI Kumar, Rajnish/C-9749-2013; Tulk, Chris/R-6088-2016 OI Kumar, Rajnish/0000-0002-7749-3515; Tulk, Chris/0000-0003-3400-3878 FU Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy FX A part of this research at ORNL's Spallation Neutron Source was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy. The authors also thank G. McLaurin and S. Lang for technical assistance. NR 28 TC 3 Z9 3 U1 0 U2 48 PU WILEY-V C H VERLAG GMBH PI WEINHEIM PA BOSCHSTRASSE 12, D-69469 WEINHEIM, GERMANY SN 1433-7851 J9 ANGEW CHEM INT EDIT JI Angew. Chem.-Int. Edit. PY 2013 VL 52 IS 5 BP 1531 EP 1534 DI 10.1002/anie.201208367 PG 4 WC Chemistry, Multidisciplinary SC Chemistry GA 075UV UT WOS:000313913300036 PM 23280637 ER PT J AU Kerfeld, CA AF Kerfeld, Cheryl A. TI Introduction: Sequences and consequences SO BIOCHEMISTRY AND MOLECULAR BIOLOGY EDUCATION LA English DT Review DE Active learning; computational biology; computers in research and teaching; curriculum design development and implementation; genomics proteomics bioinformatics; inquiry based teaching C1 [Kerfeld, Cheryl A.] Joint Genome Inst, Dept Energy, Walnut Creek, CA 94598 USA. [Kerfeld, Cheryl A.] Univ Calif Berkeley, Dept Plant & Microbial Biol, Berkeley, CA 94720 USA. [Kerfeld, Cheryl A.] Univ Calif Berkeley, Synthet Biol Inst, Berkeley, CA 94720 USA. RP Kerfeld, CA (reprint author), Joint Genome Inst, Dept Energy, 2800 Mitchell Dr, Walnut Creek, CA 94598 USA. EM ckerfeld@berkeley.edu FU U.S. Department of Energy [DE-AC02-05CH11231]; NSF [MCB0851094, EF1105897] FX This work is supported by U.S. Department of Energy Under Contract No. DE-AC02-05CH11231 and by NSF (MCB0851094 and EF1105897). NR 6 TC 2 Z9 2 U1 2 U2 17 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 1470-8175 J9 BIOCHEM MOL BIOL EDU JI Biochem. Mol. Biol. Educ. PD JAN-FEB PY 2013 VL 41 IS 1 BP 12 EP 15 DI 10.1002/bmb.20660 PG 4 WC Biochemistry & Molecular Biology; Education, Scientific Disciplines SC Biochemistry & Molecular Biology; Education & Educational Research GA 079KP UT WOS:000314169300004 PM 23382121 ER PT J AU Goh, CS Junginger, M Cocchi, M Marchal, D Thran, D Hennig, C Heinimo, J Nikolaisen, L Schouwenberg, PP Bradley, D Hess, R Jacobson, J Ovard, L Deutmeyer, M AF Goh, Chun Sheng Junginger, Martin Cocchi, Maurizio Marchal, Didier Thraen, Daniela Hennig, Christiane Heinimo, Jussi Nikolaisen, Lars Schouwenberg, Peter-Paul Bradley, Douglas Hess, Richard Jacobson, Jacob Ovard, Leslie Deutmeyer, Michael TI Wood pellet market and trade: a global perspective SO BIOFUELS BIOPRODUCTS & BIOREFINING-BIOFPR LA English DT Article DE wood pellet; trade; global perspective; market ID BIOENERGY AB This perspective provides an overview of wood pellet markets in a number of countries of high significance, together with an inventory of market factors and relevant past or existing policies. In 2010, the estimated global wood pellet production and consumption were close to 14.3 Mt (million metric tonnes) and 13.5 Mt, respectively, while the global installed production capacity had reached over 28 Mt. Two types of pellets are mainly traded (i) for residential heating and (ii) for large-scale district heating or co-firing installations. The EU was the primary market, responsible for nearly 61% and 85% of global production and consumption, respectively in 2010. EU markets were divided according to end use: (i) residential and district heating, (ii) power plants driven market, (iii) mixed market, and (iv) export-driven countries. North America basically serves as an exporter, but also with significant domestic consumption in USA. East Asia is predicted to become the second-largest consumer after the EU in the near future. The development perspective in Latin America remains unclear. Five factors that determine the market characteristics are: (i) the existence of coal-based power plants, (ii) the development of heating systems, (iii) feedstock availability, (iv) interactions with wood industry, and (v) logistics factor. Furthermore, intervention policies play a pivotal role in market development. The perspective of wood pellets industry was also analyzed from four major aspects: (i) supply potential, (ii) logistics issues, (iii) sustainability considerations, and (iv) technology development. (C) 2013 Society of Chemical Industry and John Wiley & Sons, Ltd C1 [Goh, Chun Sheng] Univ Utrecht, Fac Geosci, Dept Innovat Environm & Energy Sci, Copernicus Inst, NL-3584 CD Utrecht, Netherlands. [Cocchi, Maurizio] ETA Florence Renewable Energies, Florence, Italy. [Marchal, Didier] Walloon Agr Res Ctr, Dept Agr Engn, Gembloux, Belgium. [Thraen, Daniela] Helmholtz Zentrum Umweltforsch GmbH UFZ, Leipzig, Germany. [Hennig, Christiane] Deutsch Biomasseforschungszentrum gGmbH DBFZ, Leipzig, Germany. [Heinimo, Jussi] Lappeenranta Univ Technol, Varkaus, Finland. [Nikolaisen, Lars] Danish Technol Inst, Dept Renewable Energy & Transport, Aarhus, Denmark. [Schouwenberg, Peter-Paul] RWE Essent, sHertogenbosch, Netherlands. [Bradley, Douglas] Climate Change Solut, Ottawa, ON, Canada. [Hess, Richard] Idaho Natl Lab, Energy Syst & Technol Div, Biofuels & Renewable Energy Technol Dept, Idaho Falls, ID 83415 USA. [Deutmeyer, Michael] Green Carbon Grp, Hamburg, Germany. RP Goh, CS (reprint author), Univ Utrecht, Fac Geosci, Dept Innovat Environm & Energy Sci, Copernicus Inst, Budapestlaan 6, NL-3584 CD Utrecht, Netherlands. EM c.s.goh@uu.nl RI Goh, Chun Sheng/K-3364-2012; Junginger, Martin/A-2687-2009; OI Junginger, Martin/0000-0002-5010-2051; Goh, Chun Sheng/0000-0003-1209-6591; Ovard, Leslie/0000-0002-9021-8286 NR 22 TC 48 Z9 48 U1 5 U2 46 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 1932-104X J9 BIOFUEL BIOPROD BIOR JI Biofuels Bioprod. Biorefining PD JAN-FEB PY 2013 VL 7 IS 1 BP 24 EP 42 DI 10.1002/bbb.1366 PG 19 WC Biotechnology & Applied Microbiology; Energy & Fuels SC Biotechnology & Applied Microbiology; Energy & Fuels GA 074BE UT WOS:000313786100006 ER PT J AU English, A Tyner, WE Sesmero, J Owens, P Muth, DJ AF English, Alicia Tyner, Wallace E. Sesmero, Juan Owens, Phillip Muth, David J., Jr. TI Environmental tradeoffs of stover removal and erosion in Indiana SO BIOFUELS BIOPRODUCTS & BIOREFINING-BIOFPR LA English DT Article DE production; environment; biomass; erosion ID SOIL ORGANIC-MATTER; CORN STOVER; CONSERVATION TILLAGE; BIOMASS; CARBON AB When considering the market for biomass from corn stover resources, the consequences of soil erosion and soil quality issues are important considerations. Removal of stover can be beneficial in some areas, especially when coordinated with other conservation practices, such as vegetative barrier strips and cover crops. However, benefits are highly dependent on several factors, namely if farmers see costs and benefits associated with erosion and the tradeoffs with the removal of biomass. Although typically considered an internal cost, the implication is important to policy and contracting for biomass. This paper uses results from an integrated RUSLE2/WEPS model to incorporate six different regime choices, covering management, harvest, and conservation, into a simple profit maximization model to show these tradeoffs explicitly. The results of this work show how different costs for erosion, biomass, and conservation management will affect behavior. If the private costs of erosion are low and no conservation requirement exists, biomass removal will significantly increase erosion, but only in some areas. Alternatively, when erosion prices are high, farmers will parallel socially optimal levels of erosion, and conservation management practices can be incentivized through access to a market for stover. (C) 2013 Society of Chemical Industry and John Wiley & Sons, Ltd C1 [English, Alicia; Sesmero, Juan; Owens, Phillip] Purdue Univ, Dept Agr Econ, W Lafayette, IN 47907 USA. [Owens, Phillip] Purdue Univ, Dept Agron, W Lafayette, IN 47907 USA. [Muth, David J., Jr.] Idaho Natl Lab, Idaho Falls, ID 83415 USA. RP English, A (reprint author), Purdue Univ, Dept Agr Econ, Krannert 613, W Lafayette, IN 47907 USA. EM english2@purdue.edu NR 36 TC 5 Z9 5 U1 3 U2 20 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 1932-104X J9 BIOFUEL BIOPROD BIOR JI Biofuels Bioprod. Biorefining PD JAN-FEB PY 2013 VL 7 IS 1 BP 78 EP 88 DI 10.1002/bbb.1375 PG 11 WC Biotechnology & Applied Microbiology; Energy & Fuels SC Biotechnology & Applied Microbiology; Energy & Fuels GA 074BE UT WOS:000313786100010 ER PT J AU Sperling, M Piontek, J Gerdts, G Wichels, A Schunck, H Roy, AS La Roche, J Gilbert, J Nissimov, JI Bittner, L Romac, S Riebesell, U Engel, A AF Sperling, M. Piontek, J. Gerdts, G. Wichels, A. Schunck, H. Roy, A. -S. La Roche, J. Gilbert, J. Nissimov, J. I. Bittner, L. Romac, S. Riebesell, U. Engel, A. TI Effect of elevated CO2 on the dynamics of particle-attached and free-living bacterioplankton communities in an Arctic fjord SO BIOGEOSCIENCES LA English DT Article ID INTERGENIC SPACER ANALYSIS; DIFFERENT PCO(2) LEVELS; PHYTOPLANKTON BLOOM; HETEROTROPHIC BACTERIA; OCEAN ACIDIFICATION; ANTAGONISTIC INTERACTIONS; ENZYME-ACTIVITIES; MESOCOSM; CARBON; BIODIVERSITY AB In the frame of the European Project on Ocean Acidification (EPOCA), the response of an Arctic pelagic community (<3 mm) to a gradient of seawater pCO(2) was investigated. For this purpose 9 large-scale in situ mesocosms were deployed in Kongsfjorden, Svalbard (78 degrees 56.2' N, 11 degrees 53.6' E), in 2010. The present study investigates effects on the communities of particle-attached (PA; >3 mu m) and free-living (FL; <3 mu m > 0.2 mu m) bacteria by Automated Ribosomal Intergenic Spacer Analysis (ARISA) in 6 of the mesocosms, ranging from 185 to 1050 mu atm initial pCO(2), and the surrounding fjord. ARISA was able to resolve, on average, 27 bacterial band classes per sample and allowed for a detailed investigation of the explicit richness and diversity. Both, the PA and the FL bacterioplankton community exhibited a strong temporal development, which was driven mainly by temperature and phytoplankton development. In response to the breakdown of a picophytoplankton bloom, numbers of ARISA band classes in the PA community were reduced at low and medium CO2 (similar to 185-685 mu atm) by about 25 %, while they were more or less stable at high CO2 (similar to 820-1050 mu atm). We hypothesise that enhanced viral lysis and enhanced availability of organic substrates at high CO2 resulted in a more diverse PA bacterial community in the post-bloom phase. Despite lower cell numbers and extracellular enzyme activities in the post-bloom phase, bacterial protein production was enhanced in high CO2 mesocosms, suggesting a positive effect of community richness on this function and on carbon cycling by bacteria. C1 [Sperling, M.; Piontek, J.; Engel, A.] Alfred Wegener Inst Polar & Marine Res, D-27570 Bremerhaven, Germany. [Sperling, M.; Gerdts, G.; Wichels, A.] Alfred Wegener Inst, D-27498 Helgoland, Germany. [Sperling, M.; Piontek, J.; Schunck, H.; Roy, A. -S.; La Roche, J.; Riebesell, U.; Engel, A.] GEOMAR Helmholtz Ctr Ocean Res Kiel, D-24105 Kiel, Germany. [Gilbert, J.; Nissimov, J. I.] Plymouth Marine Lab, Plymouth PL1 3DH, Devon, England. [Gilbert, J.] Argonne Natl Lab, Argonne, IL 60439 USA. [Bittner, L.; Romac, S.] CNRS, UMR7144, Roscoff, France. [Bittner, L.; Romac, S.] Univ Paris 06, Stn Biol Roscoff, Roscoff, France. RP Sperling, M (reprint author), Alfred Wegener Inst Polar & Marine Res, Handelshafen 12, D-27570 Bremerhaven, Germany. EM martin.sperling@awi.de RI LaRoche, Julie/A-1109-2010; OI , Anja/0000-0002-1042-1955 FU European Community [211384]; EU EraNet BiodivErsA program BioMarKs; Helmholtz Graduate School for Polar and Marine Research (POLMAR) FX This work is a contribution to the "European Project on Ocean Acidification" (EPOCA), which received funding from the European Community's Seventh Framework Programme (FP7/2007-2013) under grant agreement no. 211384. This work was also partly funded by the EU EraNet BiodivErsA program BioMarKs (SR and LB). We gratefully acknowledge the logistical support of Greenpeace International for its assistance with the transport of the mesocosm facility from Kiel to Ny-Alesund and back to Kiel. We also thank the captains and crews of M/V Esperanza of Greenpeace and R/V Viking Explorer of the University Centre in Svalbard (UNIS) for assistance during mesocosm transport and during deployment and recovery in Kongsfjorden. We thank the staff of the French-German Arctic Research Base (AWIPEV) at Ny-Alesund, in particular Marcus Schumacher, for on-site logistical support. We thank Tina Baustian for help with DNA extraction. Two anonymous referees are thanked for improvement of the manuscript. Mesoaqua supported the field trip of J. I. N. on grant METAEPOCA. Financial support for the work of M. S. was provided through a stipend and a travel grant by the Helmholtz Graduate School for Polar and Marine Research (POLMAR). NR 56 TC 14 Z9 14 U1 0 U2 67 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1726-4170 J9 BIOGEOSCIENCES JI Biogeosciences PY 2013 VL 10 IS 1 BP 181 EP 191 DI 10.5194/bg-10-181-2013 PG 11 WC Ecology; Geosciences, Multidisciplinary SC Environmental Sciences & Ecology; Geology GA 079ME UT WOS:000314173700012 ER PT J AU Hudiburg, TW Law, BE Thornton, PE AF Hudiburg, T. W. Law, B. E. Thornton, P. E. TI Evaluation and improvement of the Community Land Model (CLM4) in Oregon forests SO BIOGEOSCIENCES LA English DT Article ID OLD-GROWTH FORESTS; CARBON STORAGE; UNITED-STATES; BIOMASS; PATTERNS; FLUXES; STOCKS AB Ecosystem process models are important tools for determining the interactive effects of global change and disturbance on forest carbon dynamics. Here we evaluated and improved terrestrial carbon cycling simulated by the Community Land Model (CLM4), the land model portion of the Community Earth System Model (CESM1.0.4). Our analysis was conducted primarily in Oregon forests using FLUXNET and forest inventory data for the period 2001-2006. We go beyond prior modeling studies in the region by incorporating regional variation in physiological parameters from > 100 independent field sites in the region. We also compare spatial patterns of simulated forest carbon stocks and net primary production (NPP) at 15 km resolution using data collected from federal forest inventory plots (FIA) from > 3000 plots in the study region. Finally, we evaluate simulated gross primary production (GPP) with FLUXNET eddy covariance tower data at wet and dry sites in the region. We improved model estimates by making modifications to CLM4 to allow physiological parameters (e. g., foliage carbon to nitrogen ratios and specific leaf area), mortality rate, biological nitrogen fixation, and wood allocation to vary spatially by plant functional type (PFT) within an ecoregion based on field plot data in the region. Prior to modifications, default parameters resulted in underestimation of stem biomass in all forested ecoregions except the Blue Mountains and annual NPP was both over-and underestimated. After modifications, model estimates of mean NPP fell within the observed range of uncertainty in all ecoregions (two-sided P value = 0.8), and the underestimation of stem biomass was reduced. This was an improvement from the default configuration by 50% for stem biomass and 30% for NPP. At the tower sites, modeled monthly GPP fell within the observed range of uncertainty at both sites for the majority of the year, however summer GPP was underestimated at the Metolius semi-arid pine site and spring GPP was overestimated at the Campbell River mesic Douglas-fir site, indicating GPP may be an area for further improvement. The low bias in summer maximum GPP at the semi-arid site could be due to seasonal response of V-cmax to temperature and precipitation while overestimated spring values at the mesic site could be due to response of V-cmax to temperature and day length. C1 [Hudiburg, T. W.] Univ Illinois, Dept Plant Biol, Urbana, IL 61801 USA. [Law, B. E.] Oregon State Univ, Dept Forest Ecosyst & Soc, Corvallis, OR 97331 USA. [Thornton, P. E.] Oak Ridge Natl Lab, Climate & Ecosyst Proc Environm Sci Div, Oak Ridge, TN 37831 USA. RP Hudiburg, TW (reprint author), Univ Illinois, Dept Plant Biol, 1206 W Gregory Dr, Urbana, IL 61801 USA. EM hudiburg@illinois.edu; bev.law@oregonstate.edu; thorntonpe@ornl.gov RI Thornton, Peter/B-9145-2012; Law, Beverly/G-3882-2010 OI Thornton, Peter/0000-0002-4759-5158; Law, Beverly/0000-0002-1605-1203 FU US Department of Energy; Oak Ridge Associated Universities; Environmental Research Terrestrial Carbon Program [DE-FG02-04ER64361] FX This research was performed under an appointment to the Global Change Education Program administered by the Oak Ridge Institute for Science and Education, under contract between the US Department of Energy and Oak Ridge Associated Universities and the Environmental Research Terrestrial Carbon Program (Award # DE-FG02-04ER64361). We would like to thank J. Martin for data contribution, the FLUXNET database, and A. Black for use of the Campbell River site data. NR 44 TC 19 Z9 21 U1 1 U2 51 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1726-4170 J9 BIOGEOSCIENCES JI Biogeosciences PY 2013 VL 10 IS 1 BP 453 EP 470 DI 10.5194/bg-10-453-2013 PG 18 WC Ecology; Geosciences, Multidisciplinary SC Environmental Sciences & Ecology; Geology GA 079ME UT WOS:000314173700029 ER PT J AU Roy, AS Gibbons, SM Schunck, H Owens, S Caporaso, JG Sperling, M Nissimov, JI Romac, S Bittner, L Muhling, M Riebesell, U LaRoche, J Gilbert, JA AF Roy, A. -S. Gibbons, S. M. Schunck, H. Owens, S. Caporaso, J. G. Sperling, M. Nissimov, J. I. Romac, S. Bittner, L. Muehling, M. Riebesell, U. LaRoche, J. Gilbert, J. A. TI Ocean acidification shows negligible impacts on high-latitude bacterial community structure in coastal pelagic mesocosms SO BIOGEOSCIENCES LA English DT Article ID DIFFERENT PCO(2) LEVELS; METHYLOTENERA-MOBILIS; MICROBIAL COMMUNITIES; N-2 FIXATION; PHYTOPLANKTON; DYNAMICS; BACTERIOPLANKTON; DIVERSITY; BIOSPHERE; TAXONOMY AB The impact of ocean acidification and carbonation on microbial community structure was assessed during a large-scale in situ costal pelagic mesocosm study, included as part of the EPOCA 2010 Arctic campaign. The mesocosm experiment included ambient conditions (fjord) and nine mesocosms with pCO(2) levels ranging from similar to 145 to similar to 1420 mu atm. Samples for the present study were collected at ten time points (t-1, t1, t5, t7, t12, t14, t18, t22, t26 to t28) in seven treatments (ambient fjord (similar to 145), 2x similar to 185, similar to 270, similar to 685, similar to 820, similar to 1050 mu atm) and were analysed for "small" and "large" size fraction microbial community composition using 16S rRNA (ribosomal ribonucleic acid) amplicon sequencing. This high-throughput sequencing analysis produced similar to 20 000 000 16S rRNA V4 reads, which comprised 7000OTUs. The main variables structuring these communities were sample origins (fjord or mesocosms) and the community size fraction (small or large size fraction). The community was significantly different between the unenclosed fjord water and enclosed mesocosms (both control and elevated CO2 treatments) after nutrients were added to the mesocosms, suggesting that the addition of nutrients is the primary driver of the change in mesocosm community structure. The relative importance of each structuring variable depended greatly on the time at which the community was sampled in relation to the phytoplankton bloom. The sampling strategy of separating the small and large size fraction was the second most important factor for community structure. When the small and large size fraction bacteria were analysed separately at different time points, the only taxon pCO(2) was found to significantly affect were the Gammaproteobacteria after nutrient addition. Finally, pCO(2) treatment was found to be significantly correlated (non-linear) with 15 rare taxa, most of which increased in abundance with higher CO2. C1 [Roy, A. -S.; Schunck, H.; Sperling, M.; Riebesell, U.; LaRoche, J.] GEOMAR Helmholtz Ctr Ocean Res Kiel, D-24105 Kiel, Germany. [Gibbons, S. M.; Owens, S.; Caporaso, J. G.; Gilbert, J. A.] Argonne Natl Lab, Inst Genom & Syst Biol, Argonne, IL 60439 USA. [Gibbons, S. M.] Univ Chicago, Grad Program Biophys Sci, Chicago, IL 60637 USA. [Caporaso, J. G.] Univ Arizona, Dept Comp Sci, Flagstaff, AZ 86001 USA. [Nissimov, J. I.] Plymouth Marine Lab, Plymouth PL1 3DH, Devon, England. [Romac, S.; Bittner, L.] Univ Paris 06, CNRS, Paris 6 UMR7144, F-29682 Roscoff, France. [Gilbert, J. A.] Univ Chicago, Dept Ecol & Evolut, Chicago, IL 60637 USA. [Owens, S.] Univ Chicago, Computat Inst, Chicago, IL 60637 USA. [Sperling, M.] Alfred Wegener Inst Polar & Marine Res, D-27570 Bremerhaven, Germany. [Muehling, M.] TU Bergakad Freiberg, Inst Biol Sci, D-09599 Freiberg, Germany. RP Roy, AS (reprint author), GEOMAR Helmholtz Ctr Ocean Res Kiel, Dusternbrooker Weg 20, D-24105 Kiel, Germany. EM sroy@geomar.de RI LaRoche, Julie/A-1109-2010 FU European Community's Seventh Framework Programme [211384]; NIH [5T-32EB-009412] FX This work is a contribution to the "European Project on Ocean Acidification" (EPOCA), which received funding from the European Community's Seventh Framework Programme (FP7/2007-2013) under grant agreement no. 211384. We gratefully acknowledge the logistical support of Greenpeace International for its assistance with the transport of the mesocosm facility from Kiel to Ny-A lesund and back to Kiel. We also thank the captains and crews of M/V ESPERANZA of Greenpeace and R/V Viking Explorer of the University Centre in Svalbard (UNIS) for assistance during mesocosm transport and during deployment and recovery in Kongsfjorden. We thank the staff of the French-German Arctic Research Base at Ny-A lesund, in particular Marcus Schumacher, for on-site logistical support. We would like to thank Mesoaqua for supporting J. I. N. in the field trip time to Svalbard on grant METAEPOCA. We also want to thank Tina Baustian for her help during the RNA/DNA extraction. Finally, the funding for S. M. G. was provided by NIH Training Grant 5T-32EB-009412. NR 47 TC 19 Z9 20 U1 3 U2 69 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1726-4170 J9 BIOGEOSCIENCES JI Biogeosciences PY 2013 VL 10 IS 1 BP 555 EP 566 DI 10.5194/bg-10-555-2013 PG 12 WC Ecology; Geosciences, Multidisciplinary SC Environmental Sciences & Ecology; Geology GA 079ME UT WOS:000314173700036 ER PT S AU Vineyard, CM Aimone, JB Emmanuel, GR AF Vineyard, Craig M. Aimone, James B. Emmanuel, Glory R. BE Chella, A Pirrone, R Sorbello, R Johannsdottir, KR TI Neurogenesis in a High Resolution Dentate Gyrus Model SO BIOLOGICALLY INSPIRED COGNITIVE ARCHITECTURES 2012 SE Advances in Intelligent Systems and Computing LA English DT Proceedings Paper CT Annual International Conference on Biologically Inspired Cognitive Architectures (BICA) CY OCT 31-NOV 03, 2012 CL Palermo, ITALY SP Dept Chem, management, Comp, Mech Engn, Univ Palermo, BICA Soc DE Neurogenesis; dentate gyrus; computational neural network model; spiking neuron model C1 [Vineyard, Craig M.; Aimone, James B.; Emmanuel, Glory R.] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Vineyard, CM (reprint author), Sandia Natl Labs, POB 5800, Albuquerque, NM 87185 USA. EM cmviney@sandia.gov RI Aimone, James/H-4694-2016 OI Aimone, James/0000-0002-7361-253X NR 0 TC 1 Z9 1 U1 0 U2 0 PU SPRINGER-VERLAG BERLIN PI BERLIN PA HEIDELBERGER PLATZ 3, D-14197 BERLIN, GERMANY SN 2194-5357 BN 978-3-642-34273-8 J9 ADV INTELL SYST PY 2013 VL 196 BP 371 EP 372 PG 2 WC Computer Science, Artificial Intelligence; Mathematical & Computational Biology SC Computer Science; Mathematical & Computational Biology GA BDN04 UT WOS:000313923100065 ER PT S AU Vineyard, CM Emmanuel, GR Verzi, SJ Heileman, GL AF Vineyard, Craig M. Emmanuel, Glory R. Verzi, Stephen J. Heileman, Gregory L. BE Chella, A Pirrone, R Sorbello, R Johannsdottir, KR TI A Game Theoretic Model of Neurocomputation SO BIOLOGICALLY INSPIRED COGNITIVE ARCHITECTURES 2012 SE Advances in Intelligent Systems and Computing LA English DT Proceedings Paper CT Annual International Conference on Biologically Inspired Cognitive Architectures (BICA) CY OCT 31-NOV 03, 2012 CL Palermo, ITALY SP Dept Chem, management, Comp, Mech Engn, Univ Palermo, BICA Soc DE Neuron modeling; neurocomputation; game theory; chip-firing game C1 [Vineyard, Craig M.; Emmanuel, Glory R.; Verzi, Stephen J.; Heileman, Gregory L.] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Vineyard, CM (reprint author), Sandia Natl Labs, POB 5800, Albuquerque, NM 87185 USA. EM cmviney@sandia.gov NR 0 TC 0 Z9 0 U1 0 U2 1 PU SPRINGER-VERLAG BERLIN PI BERLIN PA HEIDELBERGER PLATZ 3, D-14197 BERLIN, GERMANY SN 2194-5357 BN 978-3-642-34273-8 J9 ADV INTELL SYST PY 2013 VL 196 BP 373 EP 374 PG 2 WC Computer Science, Artificial Intelligence; Mathematical & Computational Biology SC Computer Science; Mathematical & Computational Biology GA BDN04 UT WOS:000313923100066 ER PT J AU Bushuyev, OS Peterson, GR Brown, P Maiti, A Gee, RH Weeks, BL Hope-Weeks, LJ AF Bushuyev, Oleksandr S. Peterson, Geneva R. Brown, Preston Maiti, Amitesh Gee, Richard H. Weeks, Brandon L. Hope-Weeks, Louisa J. TI Metal-Organic Frameworks (MOFs) as Safer, Structurally Reinforced Energetics SO CHEMISTRY-A EUROPEAN JOURNAL LA English DT Article DE coordination polymers; crystal engineering; density functional calculations; energetic materials; metal-organic frameworks ID NICKEL HYDRAZINE NITRATE; MOLECULAR STRUCTURE; CRYSTAL-STRUCTURE; PRIMARY EXPLOSIVES; PERCHLORATE; DIHYDRATE; COMPLEXES; SALTS; AZIDE; NHN AB Second-generation cobalt and zinc coordination architectures were obtained through efforts to stabilize extremely sensitive and energetic transition-metal hydrazine perchlorate ionic polymers. Partial ligand substitution by the tridentate hydrazinecarboxylate anion afforded polymeric 2D-sheet structures never before observed for energetic materials. Carefully balanced reaction conditions allowed the retention of the noncoordinating perchlorate anion in the presence of a strongly chelating hydrazinecarboxylate ligand. High-quality X-ray single-crystal structure determination revealed that the metal coordination preferences lead to different structural motifs and energetic properties, despite the nearly isoformulaic nature of the two compounds. Energetic tests indicate highly decreased sensitivity and DFT calculations suggest a high explosive performance for these remarkable structures. C1 [Bushuyev, Oleksandr S.; Peterson, Geneva R.; Brown, Preston; Hope-Weeks, Louisa J.] Texas Tech Univ, Dept Chem & Biochem, Lubbock, TX 79409 USA. [Maiti, Amitesh; Gee, Richard H.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. [Weeks, Brandon L.] Texas Tech Univ, Dept Chem Engn, Lubbock, TX 79409 USA. RP Hope-Weeks, LJ (reprint author), Texas Tech Univ, Dept Chem & Biochem, Lubbock, TX 79409 USA. EM louisa.hope-weeks@ttu.edu RI Weeks, Brandon/P-6331-2014 OI Weeks, Brandon/0000-0003-2552-4129 FU U.S. Department of Homeland Security [2008-ST-061-ED0001]; U.S. Department of Energy by Lawrence Livermore National Laboratory [DE-AC52-07A27344]; U.S. Department of State Fulbright Graduate Program FX This material is based upon work supported by the U.S. Department of Homeland Security under award number 2008-ST-061-ED0001. Part of this work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07A27344. This work was also partially supported by the U.S. Department of State Fulbright Graduate Program (studentship to O.S.B.). The authors thank Peter Muller for helpful advice. NR 27 TC 41 Z9 43 U1 6 U2 90 PU WILEY-V C H VERLAG GMBH PI WEINHEIM PA BOSCHSTRASSE 12, D-69469 WEINHEIM, GERMANY SN 0947-6539 J9 CHEM-EUR J JI Chem.-Eur. J. PD JAN PY 2013 VL 19 IS 5 BP 1706 EP 1711 DI 10.1002/chem.201203610 PG 6 WC Chemistry, Multidisciplinary SC Chemistry GA 074BT UT WOS:000313787700026 PM 23239142 ER PT J AU Tomasi, D Volkow, ND AF Tomasi, Dardo Volkow, Nora D. TI Striatocortical pathway dysfunction in addiction and obesity: differences and similarities SO CRITICAL REVIEWS IN BIOCHEMISTRY AND MOLECULAR BIOLOGY LA English DT Review DE Alcohol; cocaine; methamphetamine; marijuana; obesity; eating disorders; networks; receptors; dopamine; striatum ID METHAMPHETAMINE-DEPENDENT SUBJECTS; POSITRON-EMISSION-TOMOGRAPHY; ANTERIOR CINGULATE CORTEX; D-2/D-3 RECEPTOR AVAILABILITY; ADOLESCENT MARIJUANA USERS; ABSTINENT COCAINE ABUSERS; STRIATAL DOPAMINE RELEASE; MEDIAL PREFRONTAL CORTEX; BINGE-EATING DISORDER; WORKING-MEMORY TASK AB Neuroimaging techniques are starting to reveal significant overlap in the brain circuitry underlying addiction and disorders of dyscontrol over rewarding behaviors (such as binge eating disorder and obesity). Positron emission tomography (PET) has demonstrated impaired striatal dopamine (DA) signaling (decreased D2 receptors) in drug addiction and obesity that is associated with reduced baseline glucose metabolism in medial and ventral prefrontal brain regions. Functional magnetic resonance imaging (fMRI) has documented brain activation abnormalities that also implicate DA-modulated striato-cortical pathways. In this review we map findings from recent neuroimaging studies that differentiate brain activation in drug/food addiction from those in controls within brain networks functionally connected with ventral and dorsal striatum. We show that regions found to be abnormal in addiction and obesity frequently emerge at the overlap of the dorsal and the ventral striatal networks. Medial temporal and superior frontal regions functionally connected with dorsal striatum display greater vulnerability in obesity and eating disorders than in drug addictions, indicating more widespread abnormalities for obesity and eating disorders than for addictions. This corroborates involvement of both ventral striatal (predominantly associated with reward and motivation) and dorsal striatal networks (associated with habits or stimulus response learning) in addiction and obesity but also identify distinct patterns between these two disorders. C1 [Tomasi, Dardo; Volkow, Nora D.] NIAAA, Bethesda, MD USA. [Volkow, Nora D.] NIDA, Bethesda, MD 20892 USA. RP Tomasi, D (reprint author), Brookhaven Natl Lab, Dept Med, Lab Neuroimaging LNI NIAAA, Bldg 490,30 Bell Ave, Upton, NY 11973 USA. EM tomasi@bnl.gov RI Tomasi, Dardo/J-2127-2015 FU National Institutes of Alcohol Abuse and Alcoholism [2RO1AA09481] FX This work was accomplished with support from the National Institutes of Alcohol Abuse and Alcoholism (2RO1AA09481). NR 177 TC 61 Z9 61 U1 6 U2 44 PU INFORMA HEALTHCARE PI LONDON PA TELEPHONE HOUSE, 69-77 PAUL STREET, LONDON EC2A 4LQ, ENGLAND SN 1040-9238 EI 1549-7798 J9 CRIT REV BIOCHEM MOL JI Crit. Rev. Biochem. Mol. Biol. PD JAN-FEB PY 2013 VL 48 IS 1 BP 1 EP 19 DI 10.3109/10409238.2012.735642 PG 19 WC Biochemistry & Molecular Biology SC Biochemistry & Molecular Biology GA 078AO UT WOS:000314070700001 PM 23173916 ER PT J AU Novak, DM Smirnov, LS Kolesnikov, AI Voronin, VI Berger, IF Laptash, NM Vasil'ev, AD Flerov, IN AF Novak, D. M. Smirnov, L. S. Kolesnikov, A. I. Voronin, V. I. Berger, I. F. Laptash, N. M. Vasil'ev, A. D. Flerov, I. N. TI Refinement of the crystal structure of the high-temperature phase G (0) in (NH4)(2)WO2F4 (powder, X-ray, and neutron scattering) SO CRYSTALLOGRAPHY REPORTS LA English DT Article ID ORIENTATIONALLY DISORDERED STRUCTURES; TRANSITIONS; OXYFLUORIDE AB The (NH4)(2)WO2F4 compound undergoes a series of phase transitions: G (0) -> 201, K -> G (1) -> 160, and K -> G (2), with a significant change in entropy (Delta S (1) Rln10 at the G (0) -> G (1) transition), which indicates significant orientational disordering in the G (0) phase and the order-disorder type of the phase transition. X-ray diffraction is used to identify the crystal structure of the G (0) phase as rhombohedral (sp. gr. Cmcm, Z = 4), determine the lattice parameters and the positions of all atoms (except hydrogen), and show that [WO2F4](2-) ions can form a superposition of dynamic and static orientational disorders in the anionic sublattice. A determination of the orientational position of [NH4](+) ions calls for the combined method of elastic and inelastic neutron scattering. Inelastic neutron scattering is used to determine the state of hindered rotation for ammonium ions in the G (0) phase. Powder neutron diffraction shows that the orientational disorder of NH4 ions can adequately be described within the free-rotation approximation. C1 [Novak, D. M.; Smirnov, L. S.] Joint Inst Nucl Res, Frank Neutron Phys Lab, Dubna 141980, Moscow Oblast, Russia. [Novak, D. M.] Adam Mickiewicz Univ, Inst Phys, PL-60769 Poznan, Poland. [Smirnov, L. S.] FSUE GNTs RF Inst Theoret & Expt Phys, Moscow, Russia. [Kolesnikov, A. I.] Oak Ridge Natl Lab, Neutron Scattering Sci Div, Oak Ridge, TN USA. [Voronin, V. I.; Berger, I. F.] Russian Acad Sci, Ural Branch, Inst Met Phys, Ekaterinburg 620041, Russia. [Berger, I. F.; Laptash, N. M.] Russian Acad Sci, Inst Chem, Far Eastern Branch, Vladivostok 690022, Russia. [Vasil'ev, A. D.; Flerov, I. N.] Russian Acad Sci, Siberian Branch, Kirensky Inst Phys, Krasnoyarsk 660036, Russia. RP Novak, DM (reprint author), Joint Inst Nucl Res, Frank Neutron Phys Lab, Dubna 141980, Moscow Oblast, Russia. EM dmn@nf.jinr.ru RI Voronin, Vladimir/J-7733-2013; Kolesnikov, Alexander/I-9015-2012 OI Voronin, Vladimir/0000-0002-3901-9812; Kolesnikov, Alexander/0000-0003-1940-4649 FU DOE-BES [DE-AC05-00OR22725]; Office of General Sciences on Energy, Division of Materials Science of the U.S. DOE [AC02-06CH11357] FX The work at ORNL was supported by the DOE-BES and managed by UT-Battelle, LLC, for DOE under Contract DE-AC05-00OR22725. The measurements at ANL were supported by the Office of General Sciences on Energy, Division of Materials Science of the U.S. DOE (contract DE-AC02-06CH11357). NR 14 TC 1 Z9 1 U1 0 U2 13 PU MAIK NAUKA/INTERPERIODICA/SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013-1578 USA SN 1063-7745 J9 CRYSTALLOGR REP+ JI Crystallogr. Rep. PD JAN PY 2013 VL 58 IS 1 BP 129 EP 134 DI 10.1134/S1063774513010240 PG 6 WC Crystallography SC Crystallography GA 077YQ UT WOS:000314065700018 ER PT J AU Tian, J Liu, J Liu, J Thallapally, PK AF Tian, Jian Liu, Jian Liu, Jun Thallapally, Praveen K. TI Identification of solid-state forms of cucurbit[6]uril for carbon dioxide capture SO CRYSTENGCOMM LA English DT Article ID METAL-ORGANIC FRAMEWORKS; MOLECULAR POROUS MATERIAL; HIGH SURFACE-AREAS; SORPTION PROPERTIES; PERMANENT POROSITY; CAGE COMPOUNDS; CRYSTAL; ADSORPTION; NITROGEN AB Three novel crystalline forms of cucurbit[6]uril (CB[6], 1) have been identified by fine control of the mixing process of a hydrochloride solution of CB[6] with ethanol. The form that exists in nanoplate particles shows permanent porosity upon desolvation and the highest CO2 uptake (15 wt%) at 298 K and 1 bar among any known solid-state forms of CB[6]. C1 [Tian, Jian; Liu, Jian; Liu, Jun; Thallapally, Praveen K.] Pacific NW Natl Lab, Energy & Environm Directorate, Richland, WA 99352 USA. RP Tian, J (reprint author), Pacific NW Natl Lab, Energy & Environm Directorate, Richland, WA 99352 USA. EM Jian.Tian@pnnl.gov; Praveen.Thallapally@pnnl.gov RI Tian, Jian/I-8637-2012; thallapally, praveen/I-5026-2014; Liu, Jian/C-4707-2011; Liu, Jian/D-3393-2009 OI thallapally, praveen/0000-0001-7814-4467; Liu, Jian/0000-0001-5329-7408; Liu, Jian/0000-0001-5329-7408 FU Office of Basic Energy Sciences, Division of Materials Sciences and Engineering [KC020105-FWP12152]; U. S. Department of Energy [DE-AC05-76RL01830] FX We thank the Office of Basic Energy Sciences, Division of Materials Sciences and Engineering, for their support under award KC020105-FWP12152. We also thank Scott J. Dalgarno of Heriot-Watt University for his assistance in X-ray crystallography. Pacific Northwest National Laboratory is a multiprogram national laboratory operated by Battelle Memorial Institute for the U. S. Department of Energy under contract DE-AC05-76RL01830. NR 32 TC 10 Z9 10 U1 2 U2 35 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 2013 VL 15 IS 8 BP 1528 EP 1531 DI 10.1039/c3ce27017c PG 4 WC Chemistry, Multidisciplinary; Crystallography SC Chemistry; Crystallography GA 080TB UT WOS:000314265100010 ER PT J AU Guillo, P Fasulo, ME Lipschutz, MI Tilley, TD AF Guillo, Pascal Fasulo, Meg E. Lipschutz, Michael I. Tilley, T. Don TI Synthesis and characterization of tantalum silsesquioxane complexes SO DALTON TRANSACTIONS LA English DT Article ID SURFACE ORGANOMETALLIC CHEMISTRY; CARBON-MONOXIDE CLEAVAGE; HIGHLY-ACTIVE CATALYSTS; EPOXIDATION CATALYSTS; SILOXIDE COMPLEXES; SILICA; METATHESIS; HYDRIDES; ALKANES; MODELS AB Tantalum polyhedral oligosilsesquioxane (POSS) complexes have been synthesised and characterized. X-ray structures of these complexes revealed that the coordination number of the tantalum center greatly affects the cube-like silsesquioxane framework. C1 [Guillo, Pascal; Fasulo, Meg E.; Lipschutz, Michael I.; Tilley, T. Don] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Guillo, Pascal; 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 US Department of Energy [DE-AC02-05CH11231] FX This work was supported by the Director, Office of Science, Office of Basic Energy Sciences of the US Department of Energy under contract no. DE-AC02-05CH11231. The authors are grateful to Dr Frank J. Feher for helpful discussions. NR 40 TC 5 Z9 5 U1 4 U2 49 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1477-9226 J9 DALTON T JI Dalton Trans. PY 2013 VL 42 IS 6 BP 1991 EP 1995 DI 10.1039/c2dt32601a PG 5 WC Chemistry, Inorganic & Nuclear SC Chemistry GA 071TN UT WOS:000313617500009 PM 23283146 ER PT J AU Liu, JB Wang, ZM Luo, ZP Bashir, S AF Liu, Jingbo Wang, Zhimin Luo, Zhiping Bashir, Sajid TI Effective bactericidal performance of silver-decorated titania nano-composites SO DALTON TRANSACTIONS LA English DT Article ID ENERGY-LOSS SPECTROSCOPY; ESCHERICHIA-COLI; STAPHYLOCOCCUS-AUREUS; LIGHT IRRADIATION; TIO2 PARTICLES; NANOPARTICLES; DISINFECTION; AG/TIO2; DEGRADATION; RESISTANCE AB Transition metal oxide based disinfectants offer an effective approach for water purification. The present discovery found that silver (Ag) decorated titania (TiO2) nano-composites displayed high potency at 2.5 ppm within 4 h co-incubation, proved to be effective at 100% inactivation. The composite disinfectant was effective against both Gram-negative and Gram-positive bacteria, Escherichia coli and Staphylococcus aureus, found in drinking water. The mechanism of action is through nanocomposite catalysed photocatalytic oxidation and possible depolarization of the bacterial outer membrane, resulting in disinfection under visible-light conditions. C1 [Liu, Jingbo; Bashir, Sajid] Texas A&M Univ, Dept Chem, Kingsville, TX 78363 USA. [Liu, Jingbo] Texas A&M Univ, Dept Chem, College Stn, TX 77842 USA. [Wang, Zhimin] Heilongjiang Univ, Dept Chem & Mat Sci, Harbin 150001, Heilongjiang, Peoples R China. [Luo, Zhiping] Fayetteville State Univ, Dept Chem & Phys, Microscopy & Imaging Ctr, College Stn, TX 77843 USA. [Luo, Zhiping] Texas A&M Univ, Mat Sci & Engn Program, College Stn, TX 77843 USA. [Bashir, Sajid] Texas A&M Univ, Chem Biol Res Grp, Kingsville, TX 78363 USA. [Bashir, Sajid] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Bashir, S (reprint author), Texas A&M Univ, Dept Chem, MSC 161,700 Univ Blvd, Kingsville, TX 78363 USA. EM jingbo.liu@chem.tamu.edu; zhimin.wang@hlju.edu.cn; zluo@uncfsu.edu; br9@tamuk.edu RI Luo, Zhiping/C-4435-2014 OI Luo, Zhiping/0000-0002-8264-6424 FU Texas A&M University-Kingsville (TAMUK); University Research Award; College of Arts and Sciences, Research and Development Funds [160315-00014, 160336-00002]; Robert A. Welch Departmental Grant [AC-0006]; National Science Foundation [CBET-0821370] FX Work is supported by Texas A&M University-Kingsville (TAMUK), University Research Award, the College of Arts and Sciences, Research and Development Funds (160315-00014 and 160336-00002), and Robert A. Welch Departmental Grant (AC-0006). The National Science Foundation Major Research Instrumentation program (CBET-0821370) is duly acknowledged for its financial support. Lastly, Dr Perez-Ballestero and Dr Massa (Biological and Health Sciences TAMUK) are acknowledged for their assistance and comments on the biochemical assay and biosafety compliance. Author contribution is summarized in ESI. NR 56 TC 5 Z9 5 U1 1 U2 44 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1477-9226 J9 DALTON T JI Dalton Trans. PY 2013 VL 42 IS 6 BP 2158 EP 2166 DI 10.1039/c2dt31648j PG 9 WC Chemistry, Inorganic & Nuclear SC Chemistry GA 071TN UT WOS:000313617500025 PM 23188226 ER PT J AU Belonoshko, AB Lukinov, T Burakovsky, L Preston, DL Rosengren, A AF Belonoshko, Anatoly B. Lukinov, Timofei Burakovsky, Leonid Preston, Dean L. Rosengren, Anders TI Melting of a polycrystalline material SO EUROPEAN PHYSICAL JOURNAL-SPECIAL TOPICS LA English DT Article ID ARGON AB Calculating the melting temperature of a solid with a known model of interaction between atoms is nowadays a comparatively simple task. However, when one simulates a single crystal by molecular dynamics method, it does not normally melt at the melting temperature. Instead, one has to significantly overheat it. Yet, a real material melts at the melting point. Here we investigate the impact of the defects and the grain boundaries on melting. We demonstrate that defects and grain boundaries have similar impact and make it possible to simulate melting in close vicinity of thermodynamic melting temperature. We also show that the Z method might be non-applicable in discriminating a stable submelting phase. C1 [Belonoshko, Anatoly B.; Lukinov, Timofei; Rosengren, Anders] KTH Royal Inst Technol, AlbaNova Univ Ctr, S-10691 Stockholm, Sweden. [Burakovsky, Leonid] Los Alamos Natl Lab, Div Theoret Phys, Los Alamos, NM 87545 USA. [Preston, Dean L.] Los Alamos Natl Lab, Div Appl Phys, Los Alamos, NM 87545 USA. RP Belonoshko, AB (reprint author), KTH Royal Inst Technol, AlbaNova Univ Ctr, S-10691 Stockholm, Sweden. EM anatoly@kth.se OI Belonoshko, Anatoly/0000-0001-7531-3210 FU Swedish Research Council (VR) FX Computations were performed using the facilities at the Swedish National Infrastructure for Computing (SNIC). DL_POLY package was made available by their authors [3]. A.B. wishes to thank the Swedish Research Council (VR) for financial support. NR 12 TC 7 Z9 7 U1 2 U2 18 PU SPRINGER HEIDELBERG PI HEIDELBERG PA TIERGARTENSTRASSE 17, D-69121 HEIDELBERG, GERMANY SN 1951-6355 J9 EUR PHYS J-SPEC TOP JI Eur. Phys. J.-Spec. Top. PD JAN PY 2013 VL 216 IS 1 BP 199 EP 204 DI 10.1140/epjst/e2013-01743-1 PG 6 WC Physics, Multidisciplinary SC Physics GA 082AO UT WOS:000314364300021 ER PT J AU Vaikuntanathan, S Shaffer, PR Geissler, PL AF Vaikuntanathan, Suriyanarayanan Shaffer, Patrick R. Geissler, Phillip L. TI Adsorption of solutes at liquid-vapor interfaces: insights from lattice gas models SO FARADAY DISCUSSIONS LA English DT Article ID AIR/WATER INTERFACE; SURFACE-TENSION; WATER-SURFACE; ION; ELECTROLYTES; TRANSITION; SOLVATION AB The adsorption behavior of ions at liquid-vapor interfaces exhibits several unexpected yet generic features. In particular, energy and entropy are both minimum when the solute resides near the surface, for a variety of ions in a range of polar solvents, contrary to predictions of classical theories. Motivated by this generality, and by the simple physical ingredients implicated by computational studies, we have examined interfacial solvation in highly schematic models, which resolve only coarse fluctuations in solvent density and cohesive energy. Here we show that even such lattice gas models recapitulate surprising thermodynamic trends observed in detailed simulations and experiments. Attention is focused on the case of two dimensions, for which approximate energy and entropy profiles can be calculated analytically. Simulations and theoretical analysis of the lattice gas highlight the role of capillary wave-like fluctuations in mediating adsorption. They further point to ranges of temperature and solute-solvent interaction strength where surface propensity is expected to be strongest. C1 [Vaikuntanathan, Suriyanarayanan; Geissler, Phillip L.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. [Shaffer, Patrick R.; Geissler, Phillip L.] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. RP Geissler, PL (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. FU US Department of Energy, Office of Basic Energy Sciences, through the Chemical Sciences Division (CSD) of the Lawrence Berkeley National Laboratory (LBNL) [DE-AC02-05CH11231] FX Kelsey Schuster performed preliminary simulations on the lattice gas model. We gratefully acknowledge useful discussions with Yan Levin and David Limmer. This project was supported by the US Department of Energy, Office of Basic Energy Sciences, through the Chemical Sciences Division (CSD) of the Lawrence Berkeley National Laboratory (LBNL), under Contract DE-AC02-05CH11231. NR 26 TC 12 Z9 12 U1 0 U2 30 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1359-6640 J9 FARADAY DISCUSS JI Faraday Discuss. PY 2013 VL 160 BP 63 EP 74 DI 10.1039/c2fd20106b PG 12 WC Chemistry, Physical SC Chemistry GA 074MA UT WOS:000313815400003 PM 23795493 ER PT J AU Baer, MD Mundy, CJ AF Baer, Marcel D. Mundy, Christopher J. TI An ab initio approach to understanding the specific ion effect SO FARADAY DISCUSSIONS LA English DT Article ID DENSITY-FUNCTIONAL THEORY; LIQUID WATER-SURFACE; MOLECULAR-DYNAMICS SIMULATIONS; SODIUM-HALIDE INTERFACES; AIR/WATER INTERFACE; AQUEOUS-SOLUTION; VAPOR INTERFACE; SOLVATION SHELL; FREE-ENERGY; BULK WATER AB Although there is a consensus that large, polarizable anions will adsorb to the air-water interface, the precise interactions that give rise to surface enhancement are still being debated. Previously, we have demonstrated that there is a significant dependence on the choice of molecular interaction potential for I- adsorption at the air-water interface. Specifically, density functional theory (DFT) based interaction potentials lead to significantly less adsorption than empirical interaction potentials that include polarization. We have also demonstrated that DFT based interaction potentials can accurately capture the structure of the first solvation shell of both simple and polyatomic anions as compared to multi-edge X-ray absorption fine structure (XAFS) experiments. We utilize DFT to examine the local hydration structure of SCN- and IO3- that exhibit both chaotropic and kosmotropic characteristics. We compare and contrast the solvation structure of the polyatomic anions with the series of halide anions. A picture emerges where we can correlate local solvation structure to the ions' position in the Hofmeister series. C1 [Baer, Marcel D.; Mundy, Christopher J.] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Mundy, CJ (reprint author), Pacific NW Natl Lab, Richland, WA 99352 USA. EM chris.mundy@pnnl.gov RI Baer, Marcel/K-7664-2012 FU U.S. Department of Energy's (DOE) Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences; Linus Pauling Distinguished Postdoctoral Fellowship Program at PNNL; Office of Science of the U.S. Department of Energy [DE-AC05-00OR22725] FX We acknowledge Abe Stern and Shawn Kathmann for a careful reading of this manuscript. This work was supported by the U.S. Department of Energy's (DOE) Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences. Pacific Northwest National Laboratory (PNNL) is operated for the Department of Energy by Battelle. The SCN- calculations presented herein were performed with PNNL Institutional Computing. MDB is grateful for the support of the Linus Pauling Distinguished Postdoctoral Fellowship Program at PNNL. Parts of the research described in this paper was conducted under the Laboratory Directed Research and Development Program at PNNL. The surface calculations for IO3- were carried out under an INCITE 2008-2012 award, using the resources of the Oak Ridge Leadership Computing Facility at the Oak Ridge National Laboratory, which is supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC05-00OR22725. Cluster calculations were performed using the CRAY XT5 at NERSC at Lawrence Berkeley National Laboratory. NR 111 TC 22 Z9 22 U1 1 U2 89 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1359-6640 EI 1364-5498 J9 FARADAY DISCUSS JI Faraday Discuss. PY 2013 VL 160 BP 89 EP 101 DI 10.1039/c2fd20113e PG 13 WC Chemistry, Physical SC Chemistry GA 074MA UT WOS:000313815400005 PM 23795495 ER PT J AU Luo, Y Jiang, W Yu, HB MacKerell, AD Roux, B AF Luo, Yun Jiang, Wei Yu, Haibo MacKerell, Alexander D., Jr. Roux, Benoit TI Simulation study of ion pairing in concentrated aqueous salt solutions with a polarizable force field SO FARADAY DISCUSSIONS LA English DT Article ID MOLECULAR-DYNAMICS SIMULATIONS; MONTE-CARLO SIMULATIONS; PARTICLE MESH EWALD; GUANIDINIUM CHLORIDE; SODIUM-CHLORIDE; HYDRATED IONS; MEAN FORCE; WATER; POTENTIALS; COEFFICIENTS AB The accuracy of empirical force fields is critical for meaningful molecular dynamics simulations of concentrated ionic solutions. Current models are typically developed on the basis of single ion properties such as the monohydrate energy in the gas phase, or the absolute hydration free energy at infinite dilution. However, the failure of these models to represent accurately the properties of concentrated solutions cannot be excluded. Here, these issues are illustrated for a polarizable potential based on classical Drude oscillators. To model accurately concentrated ionic solutions, the parameters of the potential functions are optimized to reproduce osmotic pressure data. The sodium-chloride potential of mean force in solution calculated from the empirically-adjusted model is consistent with the results from that calculated from ab initio CPMD simulations. C1 [Luo, Yun; Yu, Haibo; Roux, Benoit] Univ Chicago, Dept Biochem & Mol Biol, Gordon Ctr Integrat Sci, Chicago, IL 60637 USA. [Luo, Yun; Jiang, Wei; Roux, Benoit] Argonne Natl Lab, Argonne, IL 60439 USA. [MacKerell, Alexander D., Jr.] Univ Maryland, Sch Pharm, Dept Pharmaceut Sci, Baltimore, MD 21201 USA. RP Roux, B (reprint author), Univ Chicago, Dept Biochem & Mol Biol, Gordon Ctr Integrat Sci, 929 E 57th St, Chicago, IL 60637 USA. EM roux@uchicago.edu RI Yu, Haibo/B-9750-2008; OI Yu, Haibo/0000-0002-1099-2803; MacKerell, Alex/0000-0001-8287-6804 FU National Institute of Health (NIH) [GM-072558, GM-051501]; NIH/NSI [CAO 93577]; NSF [MCB-0920261] FX This work was supported by the National Institute of Health (NIH) through grants GM-072558 and GM-051501. Computational resources were provided by the Extreme Science and Engineering Discovery Environment (XSEDE), which is generously supported by grant CAO 93577 from NIH/NSI and by grant MCB-0920261 from NSF. NR 59 TC 39 Z9 39 U1 3 U2 77 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1359-6640 EI 1364-5498 J9 FARADAY DISCUSS JI Faraday Discuss. PY 2013 VL 160 BP 135 EP 149 DI 10.1039/c2fd20068f PG 15 WC Chemistry, Physical SC Chemistry GA 074MA UT WOS:000313815400008 PM 23795497 ER PT J AU Dang, LX Sun, XQ Ginovska-Pangovska, B Annapureddy, HVR Truong, TB AF Dang, Liem X. Sun, Xiuquan Ginovska-Pangovska, Bojana Annapureddy, Harsha V. R. Tai Ba Truong TI Understanding ion-ion interactions in bulk and aqueous interfaces using molecular simulations SO FARADAY DISCUSSIONS LA English DT Article ID AIR/WATER INTERFACE; LIQUID INTERFACES; CHEMICAL-REACTIONS; SURFACE-TENSION; WATER; SPECTROSCOPY; VALIDATION; POTENTIALS; SOLVATION; REVEALS AB In addition to its scientific significance, the distribution of ions in the bulk and at aqueous interfaces is also very important for practical reasons. Providing a quantitative description of the ionic distribution, and describing interactions between ions in different environments, remains a challenge, and is the subject of current debate. In this study, we found that interionic potentials of mean force (PMFs) and interfacial properties are very sensitive to the ion-ion interaction potential models. Our study predicted a Sr2+-Cl- PMF with no contact ion-pair state and a shallow solvent-separated ion-pair state. In addition, we were able to quantitatively capture the experimental X-ray reflectivity results of the aqueous salt interface of the Sr2+-Cl- ion-pair, and provided a detailed physical description of the interfacial structure for this system. We also predicted the Xray reflectivity results for SrBr2 and SrI2 systems. C1 [Dang, Liem X.; Sun, Xiuquan; Ginovska-Pangovska, Bojana; Annapureddy, Harsha V. R.; Tai Ba Truong] Pacific NW Natl Lab, Chem & Mat Sci Div, Richland, WA 99352 USA. RP Dang, LX (reprint author), Pacific NW Natl Lab, Chem & Mat Sci Div, Richland, WA 99352 USA. EM liem.dang@pnnl.gov RI Annapureddy, Harsha V R/E-9818-2013; Truong, Ba Tai/O-4320-2014; OI Truong, Ba Tai/0000-0001-8254-181X FU U.S. Department of Energy (DOE), Office of Basic Energy Sciences (BES), Division of Chemical Sciences, Geosciences and Biosciences FX This work was supported by the U.S. Department of Energy (DOE), Office of Basic Energy Sciences (BES), Division of Chemical Sciences, Geosciences and Biosciences. Pacific Northwest National Laboratory is a multiprogram national laboratory operated for DOE by Battelle. The calculations were carried out using computer resources provided by BES. NR 34 TC 7 Z9 7 U1 1 U2 57 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1359-6640 J9 FARADAY DISCUSS JI Faraday Discuss. PY 2013 VL 160 BP 151 EP 160 DI 10.1039/c2fd20093g PG 10 WC Chemistry, Physical SC Chemistry GA 074MA UT WOS:000313815400009 PM 23795498 ER PT J AU Lafuente, A Latkowski, JF Kramer, KJ Dunne, AM AF Lafuente, A. Latkowski, J. F. Kramer, K. J. Dunne, A. M. TI Neutronic studies for the optimization of shield wall penetrations for laser IFE systems SO FUSION ENGINEERING AND DESIGN LA English DT Article DE IFE; Neutron; Pinhole; Shielding; Laser ID INERTIAL FUSION ENERGY; RADIATION; REACTOR AB Building upon the inertial confinement fusion (ICF) technology developed for the National Ignition Facility (NIF) at Lawrence Livermore National Laboratory (LLNL), a laser-driven inertial fusion energy (LIFE) power plant is being designed. In this pre-conceptual design, the final optic is exposed to a variety of threats originating from the fusion target. These include prompt neutron and gamma fluxes, x-ray and ionic emissions. While x-rays and ions are stopped by the low-density chamber fill gas (6 mu g/cc xenon), neutrons and gamma-rays are not significantly attenuated. In order to limit the consequences of such threats onto the penultimate optic and the rest of the laser systems, a shielding wall stands between the target chamber area and the laser bay. An optical telescope arrangement allows for the laser beam propagation from the penultimate to the final optic, through a pinhole in the shielding wall. These pinholes attenuate the neutron flux and reduce effective dose rates such that laser bay maintenance can be performed by humans. An optimum design of this laser pinhole requires a good understanding of the different design trade-offs that exist between shielding performance and survivability of the laser optical elements and are outlined in this work. This paper provides insight on the impact and influence of the pinholes on the radiation doses in the laser bay, which is located on the opposite side of the concrete shielding wall. After addressing the difficulties of evaluating shields containing penetrations, it establishes a guideline for the selection of different variables linked to the pinhole's design and gives a preliminary evaluation of the radiation fields in the laser bay. The study also helps identify the requirements to enable manual and/or remote maintenance during operation, by determining the minimum achievable effective dose rates for different shield wall designs. Since the ability to perform maintenance during plant operation is an important contributor to high laser availability, we will propose the use of non-aligned double shield walls with pinholes. (c) 2012 Elsevier B.V. All rights reserved. C1 [Lafuente, A.; Latkowski, J. F.; Kramer, K. J.; Dunne, A. M.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. RP Lafuente, A (reprint author), Lawrence Livermore Natl Lab, 7000 E Ave, Livermore, CA 94550 USA. EM Lafuentemazu2@llnl.gov RI Dunne, Mike/B-4318-2014 OI Dunne, Mike/0000-0001-8740-3870 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. Computing support for this work came from the Lawrence Livermore National Laboratory (LLNL) Institutional Computing Grand Challenge program.The author would like to thank John S. Hendricks for helpful comments on the use of variance reduction techniques. NR 24 TC 0 Z9 0 U1 0 U2 7 PU ELSEVIER SCIENCE SA PI LAUSANNE PA PO BOX 564, 1001 LAUSANNE, SWITZERLAND SN 0920-3796 J9 FUSION ENG DES JI Fusion Eng. Des. PD JAN PY 2013 VL 88 IS 1 BP 57 EP 64 DI 10.1016/j.fusengdes.2012.11.007 PG 8 WC Nuclear Science & Technology SC Nuclear Science & Technology GA 082ZT UT WOS:000314433200010 ER PT J AU Canup, RM Barr, AC Crawford, DA AF Canup, R. M. Barr, A. C. Crawford, D. A. TI Lunar-forming impacts: High-resolution SPH and AMR-CTH simulations SO ICARUS LA English DT Article DE Moon; Satellites, Formation; Planetary formation; Impact processes ID SMOOTHED PARTICLE HYDRODYNAMICS; GIANT IMPACT; MOON; ORIGIN; COLLISIONS; EVOLUTION; HYPOTHESIS; ACCRETION; DISKS; VARIABLES AB We present results of the highest-resolution simulations to date of potential Moon-forming impacts using a Lagrangian, particle-based method (smooth particle hydrodynamics, or SPH) and an Eulerian, grid-based method with adaptive mesh refinement (AMR-CTH). We consider a few candidate impacts advocated by recent works, directly comparing simulations performed at varying resolutions and with both numerical methods and their predictions for the properties of resulting protolunar disks. For a fixed set of impact conditions, simulations with either method and with different resolutions yield very similar results for the initial impact and the first few hours of the post-impact period. The subsequent disk properties in the similar to 5-20 h time period can vary substantially from case-to-case, depending on the orbits of and mutual interactions between large bound clumps of ejecta that often form after the initial impact. After such clumps have completed at least one orbit (which typically requires similar to 25-50 h), the predicted protolunar disk mass and its angular momentum converge to within about 10% for simulations of very similar impact conditions using different resolutions or methods. The disks produced by the CTH simulations are consistently about 10% less massive than those produced by SPH simulations, due presumably to inherent differences between the codes. The two methods predict broadly similar values for the fraction of the protolunar disk that originates from the target vs. the impactor, and for the initial disk radial surface density and temperature profiles. (C) 2012 Elsevier Inc. All rights reserved. C1 [Canup, R. M.; Barr, A. C.] SW Res Inst, Planetary Sci Directorate, Boulder, CO 80302 USA. [Barr, A. C.] Brown Univ, Dept Geol Sci, Providence, RI 02912 USA. [Crawford, D. A.] Sandia Natl Labs, Livermore, CA 94550 USA. RP Canup, RM (reprint author), SW Res Inst, Planetary Sci Directorate, 1050 Walnut St,Suite 300, Boulder, CO 80302 USA. EM robin@boulder.swri.edu FU NASA's LASER program; NASA Lunar Science Institute (NLSI); NLSI; United States Department of Energy [DE-AC04-94AL85000] FX The authors thank H.J. Melosh and E. Asphaug for detailed and helpful reviews. R.M.C. was supported by NASA's LASER program and the NASA Lunar Science Institute (NLSI); A.C.B. acknowledges support from NLSI. D.A.C. is an employee of Sandia, a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the United States Department of Energy under Contract DE-AC04-94AL85000. NR 54 TC 15 Z9 15 U1 3 U2 41 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 0019-1035 J9 ICARUS JI Icarus PD JAN PY 2013 VL 222 IS 1 BP 200 EP 219 DI 10.1016/j.icarus.2012.10.011 PG 20 WC Astronomy & Astrophysics SC Astronomy & Astrophysics GA 078FT UT WOS:000314084800015 ER PT J AU Dong, WB He, P Wang, J Zhou, ZH Wang, HX AF Dong, Weibing He, Ping Wang, Jessie Zhou, Zhaohui Wang, Hongxin TI Infrared measurements on ultraviolet photolysis products at cryogenic temperatures SO INFRARED PHYSICS & TECHNOLOGY LA English DT Article DE Mid infrared (IR) spectroscopy; Far infrared spectroscopy; Ultraviolet (UV) photolysis; IR cryostat ID RESONANCE VIBRATIONAL SPECTROSCOPY; COMPLEXES; ZIRCONIA; YTTRIA; IR AB Combination of ultraviolet (UV) photolysis with infrared (IR) spectroscopy (or UV/IR for abbreviation) is a powerful tool to study various chemical photoreactions, while cryostat and sample-cell windows define the working ranges for both UV and IR beams. Although diamond window has a very wide transmission range from UV to IR, the extreme cost, the absorptions at 1800-2600 cm(-1) and other problems prevent it from being the solution for all cases. In this paper, a gas-exchange cryostat was modified to realize a UV/mid-IR experiment at cryogenic temperatures. Several windows (including diamond) were discussed as options. A di-nitrogen iron complex trans-[Fe(DMeOPrPE)(2)(N-2)H][BPh4] [DMeOPrPE = 1,2-bis(dimethoxypropylphosphino)ethane] was studied as a real photolysis example. Alternatively, a cold-finger cryostat was modified for UV/far-IR compatible experiments. Non-photolysis samples K-5[Mo4O11 (R,S-Hhomocit)(2)]Cl center dot 5H(2)O (H(4)homocit = homocitric acid) and [(n-Bu)(4)N](2)[Fe4S4(PPh)(4)] were studied at cryogenic temperatures. Sample cell windows can also be used as a natural way for choosing photolysis wavelength (in addition to the use of optical filters). (c) 2012 Elsevier B.V. All rights reserved. C1 [Dong, Weibing; Zhou, Zhaohui; Wang, Hongxin] Univ Calif Davis, Dept Chem, Davis, CA 95616 USA. [Dong, Weibing; Zhou, Zhaohui; Wang, Hongxin] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA 94720 USA. [He, Ping] Sichuan Water Conservancy Vocat Coll, Dept Civil Engn, Dujiangyan 611830, Sichuan, Peoples R China. [Wang, Jessie] Univ Calif Santa Barbara, Dept Stat, Santa Barbara, CA 93106 USA. [Zhou, Zhaohui] Xiamen Univ, Coll Chem & Chem Engn, Xiamen 361005, Peoples R China. RP Wang, HX (reprint author), MS 6 2100 Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. EM hongxin@popper.lbl.gov RI Zhou, ZH/G-4658-2010 FU National Institutes of Health (NIH) [GM-65440]; National Science Foundation of China [21073150] FX The UC Davis/LBNL work was supported by the National Institutes of Health (NIH) (GM-65440, to Dr. S. Cramer at UC Davis/LBNL). The authors thank Dr. Cramer for his overall support for this work. We also thank Dr. D. Tyler in U. Oregon, Dr. D. Coucouvanis in U. Michigan for providing the Fe(H)N2 and [Fe4S4(PPh)4]= samples, Dr. Z. Hao/M. Martin in LBNL for assisting Bruker 66v/s and Dr. Yongqing Pan in Great Wall Gems Inc., for customizing the ZrO2 windows for our experiments. Z.H.Z acknowledges the partial support of National Science Foundation of China (21073150 to Z.H.Z). NR 20 TC 2 Z9 2 U1 3 U2 15 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 1350-4495 J9 INFRARED PHYS TECHN JI Infrared Phys. Technol. PD JAN PY 2013 VL 56 BP 51 EP 56 DI 10.1016/j.infrared.2012.10.003 PG 6 WC Instruments & Instrumentation; Optics; Physics, Applied SC Instruments & Instrumentation; Optics; Physics GA 082GX UT WOS:000314381400007 ER PT J AU Hsu, JH Zeng, H Lemke, KH Polyzos, AA Weier, JF Wang, M Lawin-O'Brien, AR Weier, HUG O'Brien, B AF Hsu, Joanne H. Zeng, Hui Lemke, Kalistyn H. Polyzos, Aris A. Weier, Jingly F. Wang, Mei Lawin-O'Brien, Anna R. Weier, Heinz-Ulrich G. O'Brien, Benjamin TI Chromosome-Specific DNA Repeats: Rapid Identification in Silico and Validation Using Fluorescence in Situ Hybridization SO INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES LA English DT Article DE molecular cytogenetics; chromosomes; heterochromatin; DNA repeats; data mining; fluorescence in situ hybridization; bacterial artificial chromosomes; DNA probes ID PREIMPLANTATION GENETIC DIAGNOSIS; SPECTRAL IMAGING ANALYSIS; ALPHA-SATELLITE PROBE; CANCER CELL-LINE; INTERPHASE CELLS; PRENATAL-DIAGNOSIS; Y-CHROMOSOME; THYROID-CANCER; HUMAN EMBRYOS; SPONTANEOUS-ABORTIONS AB Chromosome enumeration in interphase and metaphase cells using fluorescence in situ hybridization (FISH) is an established procedure for the rapid and accurate cytogenetic analysis of cell nuclei and polar bodies, the unambiguous gender determination, as well as the definition of tumor-specific signatures. Present bottlenecks in the procedure are a limited number of commercial, non-isotopically labeled probes that can be combined in multiplex FISH assays and the relatively high price and effort to develop additional probes. We describe a streamlined approach for rapid probe definition, synthesis and validation, which is based on the analysis of publicly available DNA sequence information, also known as "database mining". Examples of probe preparation for the human gonosomes and chromosome 16 as a selected autosome outline the probe selection strategy, define a timeline for expedited probe production and compare this novel selection strategy to more conventional probe cloning protocols. C1 [Hsu, Joanne H.] Univ Calif Berkeley UCB, Dept Mol & Cell Biol, Berkeley, CA 94720 USA. [Hsu, Joanne H.; Zeng, Hui; Lemke, Kalistyn H.; Polyzos, Aris A.; Weier, Jingly F.; Weier, Heinz-Ulrich G.] EO Lawrence Berkeley Natl Lab, Div Life Sci, Berkeley, CA 94720 USA. [Weier, Jingly F.] Univ Calif San Francisco UCSF, Dept Pathol, San Francisco, CA 94143 USA. [Wang, Mei] City Hope Natl Med Ctr, Dept Diabet, Duarte, CA 91010 USA. [Lawin-O'Brien, Anna R.] Whipps Cross Univ Hosp, Dept Fetal Med, Barts Hlth NHS Trust, London E11 1NR, England. [O'Brien, Benjamin] Univ London, Barts Hlth London, William Harvey Res Inst, London EC1A 7BE, England. [O'Brien, Benjamin] German Heart Inst, Dept Anesthesiol, D-13353 Berlin, Germany. RP Hsu, JH (reprint author), Univ Calif Berkeley UCB, Dept Mol & Cell Biol, Berkeley, CA 94720 USA. EM jhhsu@berkeley.edu; hzeng@lbl.gov; lemke.kalistyn@gmail.com; aapolyzos@lbl.gov; JLFung@lbl.gov; mwang@coh.org; lawinobrien@doctors.org.uk; ugweier@lbl.gov; benobrien@doctors.org.uk FU Leonard Rosenman Fund; NIH [CA123370, HD45736, CA132815, CA136685]; Earnest Orlando Lawrence Berkeley National Laboratory [DE-AC02-05CH11231] FX The skillful assistance of guests and staff of the Weier laboratory, LBNL, is gratefully acknowledged. This work was supported in part by a grant from the Leonard Rosenman Fund (BOB) and NIH grants CA123370, HD45736, CA132815 and CA136685 (HUW), carried out at the Earnest Orlando Lawrence Berkeley National Laboratory, under contract DE-AC02-05CH11231. NR 79 TC 1 Z9 1 U1 0 U2 18 PU MDPI AG PI BASEL PA POSTFACH, CH-4005 BASEL, SWITZERLAND SN 1422-0067 J9 INT J MOL SCI JI Int. J. Mol. Sci. PD JAN PY 2013 VL 14 IS 1 BP 57 EP 71 DI 10.3390/ijms14010057 PG 15 WC Biochemistry & Molecular Biology; Chemistry, Multidisciplinary SC Biochemistry & Molecular Biology; Chemistry GA 077SS UT WOS:000314048800005 PM 23344021 ER PT J AU Bahn, CB Majumdar, S Kasza, KE Shack, WJ AF Bahn, Chi Bum Majumdar, Saurin Kasza, Ken E. Shack, William J. TI Leak behaviors of steam generator tube-to-tubesheet joints from room temperature to 320 degrees C SO INTERNATIONAL JOURNAL OF PRESSURE VESSELS AND PIPING LA English DT Article AB To address concerns about excessive leakage from throughwall cracks in nuclear reactor tube-to-tubesheet joints under accident conditions, leak rates were measured experimentally by using tube-to-collar joint specimens and nitrogen gas. Rates were dependent on differential pressure between the tube internal surface and the crevice (i.e., the tube-to-collar interface region) and on temperature. As specimen temperature was raised to 320 degrees C, leak rates decreased gradually due to changes in gas properties and to differential thermal expansion between the Alloy 600 tubes and the SA508 collars. The leak rates did not change even after repeated temperature excursions to 320 degrees C, suggesting that thermally induced creep and subsequent contact pressure relaxation is negligible below that temperature. When considering factors that could increase flow resistance, such as oxidation, or debris on top of the tubesheet, the measured leak rates in this work are considered to be conservative. The test results were further used to validate the contact pressure calculation and a leak rate model. (c) 2012 Elsevier Ltd. All rights reserved. C1 [Bahn, Chi Bum; Majumdar, Saurin; Kasza, Ken E.; Shack, William J.] Argonne Natl Lab, Lemont, IL 60439 USA. RP Bahn, CB (reprint author), Argonne Natl Lab, Lemont, IL 60439 USA. EM bahn@anl.gov FU agency of the United States Government; NRC FX This article 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 employees, makes any warranty, expressed or implied, or assumes any legal liability or responsibility for any third party's use, or the results of such use, of any information, apparatus, product, or process disclosed in this report, or represents that its use by such third party would not infringe privately owned rights. The views expressed in this paper are not necessarily those of the U.S. Nuclear Regulatory Commission.; The authors are grateful to Drs. Jangyul Park and Ken Natesan of ANL and Mr. Charles Harris of the U.S. Nuclear Regulatory Commission (NRC) for helpful discussions. The tube-to-collar specimens were fabricated by B&W Canada. This work was sponsored by the NRC. NR 14 TC 1 Z9 1 U1 1 U2 10 PU ELSEVIER SCI LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, OXON, ENGLAND SN 0308-0161 J9 INT J PRES VES PIP JI Int. J. Pressure Vessels Pip. PD JAN PY 2013 VL 101 BP 45 EP 54 DI 10.1016/j.ijpvp.2012.10.003 PG 10 WC Engineering, Multidisciplinary; Engineering, Mechanical SC Engineering GA 082JL UT WOS:000314388000006 ER PT J AU Bahn, CB Majumdar, S Kasza, KE Shack, WJ AF Bahn, Chi Bum Majumdar, Saurin Kasza, Ken E. Shack, William J. TI Leak behavior of steam generator tube-to-tubesheet joints under creep condition: Experimental study SO INTERNATIONAL JOURNAL OF PRESSURE VESSELS AND PIPING LA English DT Article AB To address concerns regarding excessive leakage from throughwall cracks in steam generator tube-to-tubesheet joints under severe accident conditions, leak rate testing was conducted using tube-to-collar joint specimens. The tube interior and the interface between tube and collar (crevice) were pressurized independently using nitrogen gas. The leak rate through the crevice was almost zero when the specimens were pressurized at similar to 500 degrees C; this low leak rate is attributed to thermal mismatch effects preventing much leakage. The near zero leak rate was maintained until the onset of large leakage at higher temperatures. The leak rate behavior after the onset of the large leakage was not much affected by the crevice length or heat-to-heat variation of Alloy 600 tubes. This suggests that once the crevice gap opens, the creep rate of the low alloy steel collar becomes dominant. Specimens with different tube diameters behaved essentially the same way. To simulate a flawed steam generator tube in the tubesheet, the crevice region was pressurized through a hole in the tube. This simulation resulted in essentially the same behavior as those specimens whose tubes and crevices were pressurized independently. Oxidation of low alloy steel collars in air tests can increase the flow resistance, and thus tests using nitrogen gas would provide more conservative leak rate data. (c) 2012 Elsevier Ltd. All rights reserved. C1 [Bahn, Chi Bum; Majumdar, Saurin; Kasza, Ken E.; Shack, William J.] Argonne Natl Lab, Lemont, IL 60439 USA. RP Bahn, CB (reprint author), Argonne Natl Lab, Lemont, IL 60439 USA. EM bahn@anl.gov FU U.S. Nuclear Regillatory Commission FX Authors are grateful to Drs. Ken Natesan and Jangyul Park of ANL for the support and helpful discussions. The tube-to-collar specimens were fabricated by B&W Canada. This work was sponsored by U.S. Nuclear Regillatory Commission. NR 7 TC 0 Z9 0 U1 0 U2 10 PU ELSEVIER SCI LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, OXON, ENGLAND SN 0308-0161 J9 INT J PRES VES PIP JI Int. J. Pressure Vessels Pip. PD JAN PY 2013 VL 101 BP 55 EP 63 DI 10.1016/j.ijpvp.2012.10.002 PG 9 WC Engineering, Multidisciplinary; Engineering, Mechanical SC Engineering GA 082JL UT WOS:000314388000007 ER PT J AU Vinnikov, LY Troshina, AG Veschunov, IS Analytis, D Fisher, IR Liu, Y Lin, CT Fang, L Welp, U Kwok, WK AF Vinnikov, L. Ya. Troshina, A. G. Veschunov, I. S. Analytis, D. Fisher, I. R. Liu, Yu. Lin, C. T. Fang, L. Welp, U. Kwok, W. K. TI Vortex structure in BaFe2(As1-x P (x) )(2) single crystals SO JETP LETTERS LA English DT Article ID SUPERCONDUCTORS AB Single crystals of iron-containing Ba(FeAs)(2) superconductors doped with phosphorus have been studied. The vortex structure has been studied by means of the decoration method. Large domains of the triangular vortex structures have been observed in the phosphorus-doped single crystals of iron-containing superconductors. The effect of doping on pinning in iron-containing superconductors has been discussed. C1 [Vinnikov, L. Ya.; Troshina, A. G.; Veschunov, I. S.] Russian Acad Sci, Inst Solid State Phys, Chernogolovka 142432, Moscow Region, Russia. [Analytis, D.; Fisher, I. R.] Stanford Univ, Stanford, CA 94305 USA. [Troshina, A. G.] Moscow MV Lomonosov State Univ, Moscow 119991, Russia. [Liu, Yu.; Lin, C. T.] Max Planck Inst Solid State Res, D-70569 Stuttgart, Germany. [Fang, L.; Welp, U.; Kwok, W. K.] Argonne Natl Lab, Argonne, IL 60439 USA. RP Vinnikov, LY (reprint author), Russian Acad Sci, Inst Solid State Phys, Chernogolovka 142432, Moscow Region, Russia. EM vinnik@issp.ac.ru RI Fang, Lei /K-2017-2013 FU Ministry of Science and Technology of Israel; Russian Foundation for Basic Research [11-02-92480] FX This work was supported jointly by the Ministry of Science and Technology of Israel and the Russian Foundation for Basic Research (project no. 11-02-92480). NR 19 TC 1 Z9 1 U1 1 U2 32 PU MAIK NAUKA/INTERPERIODICA/SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013-1578 USA SN 0021-3640 J9 JETP LETT+ JI Jetp Lett. PD JAN PY 2013 VL 96 IS 10 BP 655 EP 658 DI 10.1134/S0021364012220134 PG 4 WC Physics, Multidisciplinary SC Physics GA 082SP UT WOS:000314412900010 ER PT J AU Nguyen, TD Carrillo, JMY Dobrynin, AV Brown, WM AF Trung Dac Nguyen Carrillo, Jan-Michael Y. Dobrynin, Andrey V. Brown, W. Michael TI A Case Study of Truncated Electrostatics for Simulation of Polyelectrolyte Brushes on GPU Accelerators SO JOURNAL OF CHEMICAL THEORY AND COMPUTATION LA English DT Article ID MOLECULAR-DYNAMICS SIMULATIONS; PARTICLE MESH EWALD; COULOMBIC INTERACTIONS; NONUNIFORM LIQUIDS; ATTRACTIVE FORCES; LIPID-BILAYERS; WOLF METHOD; SYSTEMS; WATER; LUBRICATION AB Numerous issues have disrupted the trend for increasing computational performance with faster CPU clock frequencies. In order to exploit the potential performance of new computers, it is becoming increasingly desirable to re-evaluate computational physics methods and models with an eye toward approaches that allow for increased concurrency and data locality. The evaluation of long-range Coulombic interactions is a common bottleneck for molecular dynamics simulations. Enhanced truncation approaches have been proposed as an alternative method and are particularly well-suited for many-core architectures and GPUs due to the inherent fine-grain parallelism that can be exploited. In this paper, we compare efficient truncation-based approximations to evaluation of electrostatic forces with the more traditional particle particle-particle-mesh ((PM)-M-3) method for the molecular dynamics simulation of polyelectrolyte brush layers. We show that with the use of GPU accelerators, large parallel simulations using (PM)-M-3 can be greater than 3 times faster due to a reduction in the mesh-size required. Alternatively, using a truncation-based scheme can improve performance even further. This approach can be up to 3.9 times faster than GPU-accelerated (PM)-M-3 for many polymer systems and results in accurate calculation of shear velocities and disjoining pressures for brush layers. For configurations with highly nonuniform charge distributions, however, we find that it is more efficient to use (PM)-M-3; for these systems, computationally efficient parametrizations of the truncation-based approach do not produce accurate counterion density profiles or brush morphologies. C1 [Trung Dac Nguyen; Brown, W. Michael] Oak Ridge Natl Lab, Natl Ctr Computat Sci, Oak Ridge, TN 37831 USA. [Carrillo, Jan-Michael Y.; Dobrynin, Andrey V.] Univ Connecticut, Inst Mat Sci, Polymer Program, Storrs, CT 06269 USA. [Carrillo, Jan-Michael Y.; Dobrynin, Andrey V.] Univ Connecticut, Dept Phys, Storrs, CT 06269 USA. RP Brown, WM (reprint author), Oak Ridge Natl Lab, Natl Ctr Computat Sci, Oak Ridge, TN 37831 USA. EM 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; Dobrynin, Andrey/0000-0002-6484-7409 FU Office of Advanced Scientific Computing Research, Office of Science, U.S. Department of Energy [DE-AC05-00OR22725]; UT-Battelle, LLC; Office of Science of the U.S. Department of Energy [DE-AC05-00OR22725] FX All of the code described in this paper is available in the open-source LAMMPS software package, available at http://lammps.sandia.gov/ or by contacting the authors. This research was conducted in part 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. This research used resources of the Leadership Computing Facility at Oak Ridge National Laboratory, which is supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC05-00OR22725 with UT-Battelle, LLC. NR 55 TC 8 Z9 8 U1 2 U2 32 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 1549-9618 J9 J CHEM THEORY COMPUT JI J. Chem. Theory Comput. PD JAN PY 2013 VL 9 IS 1 BP 73 EP 83 DI 10.1021/ct300718x PG 11 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 068PM UT WOS:000313378700011 PM 26589011 ER PT J AU Gaenko, A Windus, TL Sosonkina, M Gordon, MS AF Gaenko, Alexander Windus, Theresa L. Sosonkina, Masha Gordon, Mark S. TI Design and Implementation of Scientific Software Components to Enable Multiscale Modeling: The Effective Fragment Potential (QM/EFP) Method SO JOURNAL OF CHEMICAL THEORY AND COMPUTATION LA English DT Article ID QUANTUM-CHEMISTRY; MOLECULAR-ORBITALS; CHARGE-TRANSFER; ENERGIES; STATE; PI AB The design and development of scientific software components to provide an interface to the effective fragment potential (EFP) methods are reported. Multiscale modeling of physical and chemical phenomena demands the merging of software packages developed by research groups in significantly different fields. Componentization offers an efficient way to realize new high performance scientific methods by combining the best models available in different software packages without a need for package readaptation after the initial componentization is complete. The EFP method is an efficient electronic structure theory based model potential that is suitable for predictive modeling of intermolecular interactions in large molecular systems, such as liquids, proteins, atmospheric aerosols, and nanoparticles, with an accuracy that is comparable to that of correlated ab initio methods. The developed components make the EFP functionality accessible for any scientific component-aware software package. The performance of the component is demonstrated on a protein interaction model, and its accuracy is compared with results obtained with coupled cluster methods. C1 [Gaenko, Alexander; Windus, Theresa L.; Sosonkina, Masha; Gordon, Mark S.] Iowa State Univ, Ames Lab, Ames, IA 50011 USA. RP Gordon, MS (reprint author), Iowa State Univ, Ames Lab, Ames, IA 50011 USA. EM mark@si.msg.chem.iastate.edu FU U.S. Department of Energy Scientific Discovery Through Advanced Computing (SciDAC) grant FX This work was supported by a U.S. Department of Energy Scientific Discovery Through Advanced Computing (SciDAC) grant to the Ames Laboratory. Helpful discussions with Dr. David Bernhold are gratefully acknowledged. NR 43 TC 2 Z9 2 U1 2 U2 31 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 1549-9618 EI 1549-9626 J9 J CHEM THEORY COMPUT JI J. Chem. Theory Comput. PD JAN PY 2013 VL 9 IS 1 BP 222 EP 231 DI 10.1021/ct300614z PG 10 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 068PM UT WOS:000313378700026 PM 26589025 ER PT J AU Riccardi, D Guo, HB Parks, JM Gu, BH Liang, LY Smith, JC AF Riccardi, Demian Guo, Hao-Bo Parks, Jerry M. Gu, Baohua Liang, Liyuan Smith, Jeremy C. TI Cluster-Continuum Calculations of Hydration Free Energies of Anions and Group 12 Divalent Cations SO JOURNAL OF CHEMICAL THEORY AND COMPUTATION LA English DT Article ID ELECTRONIC-STRUCTURE CALCULATIONS; SOLVATION FREE-ENERGIES; DENSITY-FUNCTIONAL THEORY; METAL-BINDING AFFINITY; QUASI-CHEMICAL THEORY; AB-INITIO; WATER CLUSTERS; BASIS-SETS; MOLECULAR CALCULATIONS; SOLVENT CALCULATIONS AB Understanding aqueous phase processes involving group 12 metal cations is relevant to both environmental and biological sciences. Here, quantum chemical methods and polarizable continuum models are used to compute the hydration free energies of a series of divalent group 12 metal cations (Zn2+, Cd2+, and Hg2+) together with Cu2+ and the anions OH-, SH-, Cl-, and F-. A cluster-continuum method is employed, in which gas-phase clusters of the ion and explicit solvent molecules are immersed in a dielectric continuum. Two approaches to define the size of the solute-water cluster are compared, in which the number of explicit waters used is either held constant or determined variationally as that of the most favorable hydration free energy. Results obtained with various polarizable continuum models are also presented. Each leg of the relevant thermodynamic cycle is analyzed in detail to determine how different terms contribute to the observed mean signed error (MSE) and the standard deviation of the error (STDEV) between theory and experiment. The use of a constant number of water molecules for each set of ions is found to lead to predicted relative trends that benefit from error cancellation. Overall, the best results are obtained with MP2 and the Solvent Model D polarizable continuum model (SMD), with eight explicit water molecules for anions and 10 for the metal cations, yielding a STDEV of 2.3 kcal mol(-1) and MSE of 0.9 kcal mol(-1) between theoretical and experimental hydration free energies, which range from -72.4 kcal mol(-1) for SW to -505.9 kcal mol(-1) for Cu2+. Using B3PW91 with DFT-D3 dispersion corrections (B3PW91-D) and SMD yields a STDEV of 3.3 kcal mol(-1) and MSE of 1.6 kcal mol(-1), to which adding MP2 corrections from smaller divalent metal cation water molecule clusters yields very good agreement with the full MP2 results. Using B3PW91-D and SMD, with two explicit water molecules for anions and six for divalent metal cations, also yields reasonable agreement with experimental values, due in part to fortuitous error cancellation associated with the metal cations. Overall, the results indicate that the careful application of quantum chemical cluster-continuum methods provides valuable insight into aqueous ionic processes that depend on both local and long-range electrostatic interactions with the solvent. C1 [Riccardi, Demian; Guo, Hao-Bo; Parks, Jerry M.; Smith, Jeremy C.] Oak Ridge Natl Lab, UT ORNL Ctr Mol Biophys, Oak Ridge, TN 37831 USA. [Riccardi, Demian; Smith, Jeremy C.] Univ Tennessee, Dept Biochem & Cellular & Mol Biol, Knoxville, TN 37996 USA. [Gu, Baohua; Liang, Liyuan] Oak Ridge Natl Lab, Div Environm Sci, Oak Ridge, TN 37831 USA. RP Smith, JC (reprint author), Oak Ridge Natl Lab, UT ORNL Ctr Mol Biophys, 1 Bethel Valley Rd, Oak Ridge, TN 37831 USA. EM smithjc@ornl.gov RI Parks, Jerry/B-7488-2009; Guo, Hao-Bo/B-7486-2009; Liang, Liyuan/O-7213-2014; Gu, Baohua/B-9511-2012; smith, jeremy/B-7287-2012 OI Parks, Jerry/0000-0002-3103-9333; Guo, Hao-Bo/0000-0003-1321-1758; Liang, Liyuan/0000-0003-1338-0324; Gu, Baohua/0000-0002-7299-2956; smith, jeremy/0000-0002-2978-3227 FU Office of Biological and Environmental Research, U.S. Department of Energy (DOE); U.S. DOE [DE-AC05-00OR22725]; Office of Science of the U.S. DOE [DE-AC02-05CH11231] FX We thank the reviewers for helpful suggestions. This work was conducted as part of the mercury Scientific Focus Area research program at Oak Ridge National Laboratory (ORNL), which is sponsored by the Subsurface Biogeochemical Research Program, Office of Biological and Environmental Research, U.S. Department of Energy (DOE). ORNL is managed by UT Battelle, LLC for U.S. DOE under contract DE-AC05-00OR22725. This research used resources of the National Energy Research Scientific Computing Center, which is supported by the Office of Science of the U.S. DOE under Contract No. DE-AC02-05CH11231. NR 91 TC 16 Z9 16 U1 3 U2 65 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 1549-9618 EI 1549-9626 J9 J CHEM THEORY COMPUT JI J. Chem. Theory Comput. PD JAN PY 2013 VL 9 IS 1 BP 555 EP 569 DI 10.1021/ct300296k PG 15 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 068PM UT WOS:000313378700057 PM 26589054 ER PT J AU Gumbart, JC Roux, B Chipot, C AF Gumbart, James C. Roux, Benoit Chipot, Christophe TI Standard Binding Free Energies from Computer Simulations: What Is the Best Strategy? SO JOURNAL OF CHEMICAL THEORY AND COMPUTATION LA English DT Article ID MOLECULAR-DYNAMICS SIMULATIONS; ABSOLUTE FREE-ENERGY; HISTOGRAM ANALYSIS METHOD; LIGAND-BINDING; THERMODYNAMIC INTEGRATION; AQUEOUS-SOLUTION; ABL-SH3 DOMAIN; T4 LYSOZYME; MEAN FORCE; AFFINITY AB Accurate prediction of standard binding free energies describing protein ligand association remains a daunting computational endeavor. This challenge is rooted to a large extent in the considerable changes in conformational, translational, and rotational entropies underlying the binding process that atomistic simulations cannot easily sample. In spite of significant methodological advances, reflected in a continuously improving agreement with experiment, a characterization of alternate strategies aimed at measuring binding affinities, notably their respective advantages and drawbacks, is somewhat lacking. Here, two distinct avenues to determine the standard binding free energy are compared in the case of a short, proline-rich peptide associating to the Src homology domain 3 of tyrosine kinase Abl. These avenues, one relying upon alchemical transformations and the other on potentials of mean force (PMFs), invoke a series of geometrical restraints acting on collective variables designed to alleviate sampling limitations inherent to classical molecular dynamics simulations. The experimental binding free energy of Delta G(bind) = -7.99 kcal/niol is well reproduced by the two strategies developed herein, with Delta G(bind) = -7.7 for the alchemical route and Delta G(bind) = -7.8 kcal/mol for the alternate PMF-based route. In detailing the underpinnings of these numerical strategies devised for the accurate determination of standard binding free energies, many practical elements of the proposed rigorous, conceptual framework are clarified, thereby paving way to tackle virtually any recognition and association phenomenon. C1 [Gumbart, James C.; Roux, Benoit] Argonne Natl Lab, Biosci Div, Argonne, IL 60439 USA. [Chipot, Christophe] Univ Illinois, Beckman Inst, Urbana, IL 61801 USA. [Roux, Benoit] Univ Chicago, Dept Biochem & Mol Biol, Chicago, IL 60637 USA. [Roux, Benoit] Univ Chicago, Gordon Ctr Integrat Sci, Chicago, IL 60637 USA. [Chipot, Christophe] Univ Lorraine, Equipe Dynam Assemblages Membranaires, UMR 7565, F-54506 Vandoeuvre Les Nancy, France. RP Roux, B (reprint author), Argonne Natl Lab, Biosci Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM roux@uchicago.edu; chipot@ks.uiuc.edu FU France and Chicago Collaborating in the Sciences (FACCTS) Center; National Science Foundation (NSF) [MCB-0920261, OCI-1053575]; National Institute of Health [R01-CA093577]; Argonne National Laboratory FX The authors are grateful to the France and Chicago Collaborating in the Sciences (FACCTS) Center for their support. The research is funded by grant MCB-0920261 from the National Science Foundation (NSF) and by grant R01-CA093577 from the National Institute of Health (BR). Simulations were carried out using the Extreme Science and Engineering Discovery Environment (XSEDE), which is supported by NSF grant number OCI-1053575. The Centre Informatique National de l'Enseignement Superieur, Montpellier, is also gratefully acknowledged for generous provision of computer time. J.C.G. is supported by a Director's Postdoctoral Fellowship from Argonne National Laboratory. NR 75 TC 80 Z9 80 U1 8 U2 130 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 1549-9618 EI 1549-9626 J9 J CHEM THEORY COMPUT JI J. Chem. Theory Comput. PD JAN PY 2013 VL 9 IS 1 BP 794 EP 802 DI 10.1021/ct3008099 PG 9 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 068PM UT WOS:000313378700079 PM 23794960 ER PT J AU Zarzycki, J Axen, SD Kinney, JN Kerfeld, CA AF Zarzycki, Jan Axen, Seth D. Kinney, James N. Kerfeld, Cheryl A. TI Cyanobacterial-based approaches to improving photosynthesis in plants SO JOURNAL OF EXPERIMENTAL BOTANY LA English DT Review DE Carbon dioxide fixation; carbonic anhydrase; carboxysomes; cyanobacteria; photorespiration; photosynthesis; RubisCO; RubisCO activase ID CARBOXYSOMAL CARBONIC-ANHYDRASE; RIBULOSE-BISPHOSPHATE CARBOXYLASE; SYNECHOCOCCUS PCC7942 REVEALS; CO2 CONCENTRATING MECHANISMS; STRAIN PCC 7942; RUBISCO ACTIVASE; RIBULOSE-1,5-BISPHOSPHATE CARBOXYLASE; NDH-1 COMPLEXES; HALOTHIOBACILLUS-NEAPOLITANUS; STIMULATES PHOTOSYNTHESIS AB Plants rely on the CalvinBenson (CB) cycle for CO2 fixation. The key carboxylase of the CB cycle is ribulose-1,5-bisphosphate carboxylase/oxygenase (RubisCO). Efforts to enhance carbon fixation in plants have traditionally focused on RubisCO or on approaches that can help to remedy RubisCO's undesirable traits: its low catalytic efficiency and photorespiration. Towards reaching the goal of improving plant photosynthesis, cyanobacteria may be instrumental. Because of their evolutionary relationship to chloroplasts, they represent ideal model organisms for photosynthesis research. Furthermore, the molecular understanding of cyanobacterial carbon fixation provides a rich source of strategies that can be exploited for the bioengineering of chloroplasts. These strategies include the cyanobacterial carbon concentrating mechanism (CCM), which consists of active and passive transporter systems for inorganic carbon and a specialized organelle, the carboxysome. The carboxysome encapsulates RubisCO together with carbonic anhydrase in a protein shell, resulting in an elevated CO2 concentration around RubisCO. Moreover, cyanobacteria differ from plants in the isoenzymes involved in the CB cycle and the photorespiratory pathways as well as in mechanisms that can affect the activity of RubisCO. In addition, newly available cyanobacterial genome sequence data from the CyanoGEBA project, which has more than doubled the amount of genomic information available for cyanobacteria, increases our knowledge on the CCM and the occurrence and distribution of genes of interest. C1 [Zarzycki, Jan; Axen, Seth D.; Kinney, James N.; Kerfeld, Cheryl A.] Joint Genome Inst, Dept Energy, Walnut Creek, CA 94598 USA. [Kerfeld, Cheryl A.] Univ Calif Berkeley, Dept Plant & Microbial Biol, Berkeley, CA 94720 USA. RP Kerfeld, CA (reprint author), Joint Genome Inst, Dept Energy, 2800 Mitchell Dr, Walnut Creek, CA 94598 USA. EM ckerfeld@lbl.gov FU Office of Science of the US Department of Energy [DE-AC02 05CH11231]; National Science Foundation [EF1105897] FX The work conducted by the US Department of Energy Joint Genome Institute is supported by the Office of Science of the US Department of Energy (contract no. DE-AC02 05CH11231) and by the National Science Foundation (grant no. EF1105897). NR 87 TC 48 Z9 51 U1 7 U2 87 PU OXFORD UNIV PRESS PI OXFORD PA GREAT CLARENDON ST, OXFORD OX2 6DP, ENGLAND SN 0022-0957 J9 J EXP BOT JI J. Exp. Bot. PD JAN PY 2013 VL 64 IS 3 SI SI BP 787 EP 798 DI 10.1093/jxb/ers294 PG 12 WC Plant Sciences SC Plant Sciences GA 078WA UT WOS:000314129600008 PM 23095996 ER PT J AU Alexander, L Hoyt, C Michalczyk, R Wu, RL Thorn, DL Silks, LA AF Alexander, Lisa Hoyt, Caroline Michalczyk, Ryszard Wu, Ruilian Thorn, Dave L. Silks, L. A. 'Pete' TI Gram-scale synthesis and efficient purification of 13C-labeled levoglucosan from 13C glucose SO JOURNAL OF LABELLED COMPOUNDS & RADIOPHARMACEUTICALS LA English DT Article DE carbon-13 labeled; levoglucosan; 1; 6-anhydroglucose; large scale AB 13C-Labeled levoglucosan has been synthesized and purified in good yield, and on the gram scale in one step from commercially available 13C glucose. This one-step protocol uses 2-chloro-1,3-dimethylimidazolinium chloride that serves to selectively activate the anomeric carbon toward substitution reactions. The labeled glucose is then smoothly converted to the anhydroglucose. Purification is efficiently achieved on large scale by chromatography on silica gel. C1 [Alexander, Lisa; Hoyt, Caroline; Michalczyk, Ryszard; Wu, Ruilian; Thorn, Dave L.; Silks, L. A. 'Pete'] Los Alamos Natl Lab, Biosci Div, Bioenergy & Environm Sci Grp B8, Los Alamos, NM 87544 USA. RP Silks, LA (reprint author), Los Alamos Natl Lab, Biosci Div, Bioenergy & Environm Sci Grp B8, MS E529, Los Alamos, NM 87544 USA. EM pete-silks@lanl.gov OI Silks, Pete/0000-0002-2993-5630; Michalczyk, Ryszard/0000-0001-8839-6473 FU Los Alamos National Laboratory LDRD [20100160ER]; National Alliance for Biomass Conversion (NABC) FX We would like to thank the Los Alamos National Laboratory LDRD program (20100160ER) and the National Alliance for Biomass Conversion (NABC) for financial support. NR 4 TC 2 Z9 2 U1 0 U2 14 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0362-4803 J9 J LABELLED COMPD RAD JI J. Label. Compd. Radiopharm. PD JAN PY 2013 VL 56 IS 1 BP 27 EP 29 DI 10.1002/jlcr.2978 PG 3 WC Biochemical Research Methods; Chemistry, Medicinal; Chemistry, Analytical SC Biochemistry & Molecular Biology; Pharmacology & Pharmacy; Chemistry GA 078AN UT WOS:000314070600007 PM 24285138 ER PT J AU Arienti, M Li, X Soteriou, MC Eckett, CA Sussman, M Jensen, RJ AF Arienti, M. Li, X. Soteriou, M. C. Eckett, C. A. Sussman, M. Jensen, R. J. TI Coupled Level-Set/Volume-of-Fluid Method for Simulation of Injector Atomization SO JOURNAL OF PROPULSION AND POWER LA English DT Article; Proceedings Paper CT 46th AIAA/ASME/SAE/ASEE Joint Propulsion Conference and Exhibit CY JUL 25-29, 2010 CL Nashville, TN SP AIAA, ASME, SAE, ASEE, Israel Minist Sci, Culture & Sport ID INSTABILITY; FLOWS; SET AB This paper presents results of a multiphase computational fluid dynamics code using a coupled level-set/volume-of-fluid method to simulate liquid atomization. This interface-capturing approach combines the mass conservation properties of the volume-of-fluid method with the accurate surface reconstruction properties of the level-set method, and it includes surface tension as a volume force calculated with second-order accuracy. Developed by one of the authors, the multiphase code builds upon the combined level-set/volume-of-fluid methodology to enable bubbly flow, liquid breakup, and phase-change simulations. The extension presented in this paper couples a Lagrangian dispersed phase model for postbreakup tracking of droplets with block-structured adaptive mesh refinement on the Eulerian grid. Under an appropriate set of criteria, the transfer of droplets representation from the Eulerian to the Lagrangian discretization enables the simulation of sprays on larger domains and for longer physical times without degrading the overall accuracy of the calculation. A demonstration for like-on-like jet impingement of relevance to cold startup of liquid rocket engines is presented here at low, moderate, and high injection velocities, including validation with experimental data. C1 [Arienti, M.] Sandia Natl Labs, Thermal Fluid Sci & Engn Dept, Livermore, CA 94550 USA. [Li, X.] United Technol Res Ctr, E Hartford, CT 06108 USA. [Soteriou, M. C.] United Technol Res Ctr, Thermal & Fluid Sci Dept, E Hartford, CT 06108 USA. [Eckett, C. A.] Pratt & Whitney, Adv Programs & Technol, E Hartford, CT 06108 USA. [Sussman, M.] Florida State Univ, Dept Math, Tallahassee, FL 32306 USA. [Jensen, R. J.] Pratt & Whitney Rocketdyne, Canoga Pk, CA 91309 USA. RP Arienti, M (reprint author), Sandia Natl Labs, Thermal Fluid Sci & Engn Dept, Livermore, CA 94550 USA. NR 23 TC 10 Z9 10 U1 0 U2 26 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 2013 VL 29 IS 1 BP 147 EP 157 DI 10.2514/1.B34198 PG 11 WC Engineering, Aerospace SC Engineering GA 081OQ UT WOS:000314331900015 ER PT J AU Ogden, MD Sinkov, SI Nilson, M Lumetta, GJ Hancock, RD Nash, KL AF Ogden, Mark D. Sinkov, Serguei I. Nilson, Mikael Lumetta, Gregg J. Hancock, Robert D. Nash, Kenneth L. TI Complexation of Am(III) and Nd(III) by 1,10-Phenanthroline-2,9-Dicarboxylic Acid SO JOURNAL OF SOLUTION CHEMISTRY LA English DT Article DE Am(III); Nd(III); 1,10-Phenanthroline-2,9-diacetic acid; Stability constants; Ligand preorganization ID ION; SEPARATION; AFFINITY AB The complexant 1,10-phenanthroline-2,9-dicarboxylic acid (PDA) is a planar tetradentate ligand that is more preorganized for metal complexation than its unconstrained analogue ethylendiiminodiacetic acid (EDDA). Furthermore, the backbone nitrogen atoms of PDA are aromatic, hence are softer than the aliphatic amines of EDDA. It has been hypothesized that PDA will selectively bond to trivalent actinides over lanthanides. In this report, the results of spectrophotometric studies of the complexation of Nd(III) and Am(III) by PDA are reported. Because the complexes are moderately stable, it was necessary to conduct these titrations using competitive equilibrium methods, competitive cation complexing between PDA and diethylenetriaminepentaacetic acid, and competition between ligand protonation and complex formation. Stability constants and ligand protonation constants were determined at 0.1 mol center dot L-1 ionic strength and at 0.5 mol center dot L-1 ionic strength nitrate media at 21 +/- A 1 A degrees C. The stability constants are lower than those predicted from first principles and speciation calculations indicate that Am3+ selectivity over Nd3+ is less than that exhibited by 1,10-phenanthroline. C1 [Ogden, Mark D.; Nilson, Mikael; Nash, Kenneth L.] Washington State Univ, Dept Chem, Pullman, WA 99164 USA. [Sinkov, Serguei I.; Lumetta, Gregg J.] Pacific NW Natl Lab, Richland, WA 99354 USA. [Hancock, Robert D.] Univ N Carolina Wilmington, Dept Chem & Biochem, Wilmington, NC 28403 USA. RP Nash, KL (reprint author), Washington State Univ, Dept Chem, POB 644630, Pullman, WA 99164 USA. EM mark.ogden@ansto.gov.au; knash@wsu.edu FU U.S. Department of Energy; Office of Nuclear Energy; Nuclear Energy Research Initiative Consortium (NERI-C) program [DE-FG07-07ID14896] FX This research was conducted at WSU, UNC-W, and PNNL with funding provided by the U.S. Department of Energy, Office of Nuclear Energy, Nuclear Energy Research Initiative Consortium (NERI-C) program under project number DE-FG07-07ID14896. NR 16 TC 8 Z9 8 U1 1 U2 37 PU SPRINGER/PLENUM PUBLISHERS PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 0095-9782 J9 J SOLUTION CHEM JI J. Solut. Chem. PD JAN PY 2013 VL 42 IS 1 BP 211 EP 225 DI 10.1007/s10953-012-9940-2 PG 15 WC Chemistry, Physical SC Chemistry GA 082AV UT WOS:000314365000016 ER PT J AU Insepov, Z Norem, J AF Insepov, Zeke Norem, Jim TI Can surface cracks and unipolar arcs explain breakdown and gradient limits? SO JOURNAL OF VACUUM SCIENCE & TECHNOLOGY A LA English DT Article ID VACUUM AB The authors argue that the physics of unipolar arcs and surface cracks can help understand rf breakdown and vacuum arc data. They outline a model of the basic mechanisms involved in breakdown and explore how the physics of unipolar arcs and cracks can simplify the picture of breakdown and gradient limits in accelerators, tokamaks as well as laser ablation, micrometeorites, and other applications. Cracks are commonly seen in SEM images of arc damage and they are produced as the liquid metal cools. They can produce the required field enhancements to explain field emission data and can produce mechanical failure of the surface that would trigger breakdown events. Unipolar arcs can produce currents sufficient to short out rf structures, and can cause the sort of damage seen in SEM images. They should be unstable, and possibly self-quenching, as seen in optical fluctuations and surface damage. The authors describe some details and consider the predictions of this simple model. (C) 2013 American Vacuum Society. [http://dx.doi.org/10.1116/1.4766929] C1 [Insepov, Zeke; Norem, Jim] Argonne Natl Lab, Argonne, IL 60439 USA. RP Insepov, Z (reprint author), Argonne Natl Lab, 9700 S Cass Ave, Argonne, IL 60439 USA. EM norem@anl.gov RI Insepov, Zinetula/L-2095-2013 OI Insepov, Zinetula/0000-0002-8079-6293 FU U.S. Department of Energy Office of High Energy Physics [DE-AC02-06CH11357] FX The authors thank the staff of the Accelerator and Technical Divisions at Fermi lab and the Muon Accelerator Program (MAP) for supporting and maintaining the MAP experimental program in the MTA experimental area. The work at UChicago Argonne, LLC, Operator of Argonne National Laboratory, Argonne was supported by the U.S. Department of Energy Office of High Energy Physics under Contract No. DE-AC02-06CH11357. Figure 3, taken by T. Proslier, was obtained at the Electron Microscopy Center at Argonne National Laboratory, which was supported by the U.S. Department of Energy, Office of Science. NR 32 TC 8 Z9 10 U1 2 U2 14 PU A V S AMER INST PHYSICS PI MELVILLE PA STE 1 NO 1, 2 HUNTINGTON QUADRANGLE, MELVILLE, NY 11747-4502 USA SN 0734-2101 J9 J VAC SCI TECHNOL A JI J. Vac. Sci. Technol. A PD JAN-FEB PY 2013 VL 31 IS 1 AR 011302 DI 10.1116/1.4766929 PG 10 WC Materials Science, Coatings & Films; Physics, Applied SC Materials Science; Physics GA 076BK UT WOS:000313931300003 ER PT J AU Tobin, JA Yu, SW Chung, BW Ryzhkov, MV Mirmelstein, A AF Tobin, J. A. Yu, S. -W. Chung, B. W. Ryzhkov, M. V. Mirmelstein, A. TI Direct comparison of spectroscopic data with cluster calculations of plutonium dioxide and uranium dioxide SO JOURNAL OF VACUUM SCIENCE & TECHNOLOGY A LA English DT Article ID ADVANCED LIGHT-SOURCE; ELECTRONIC-STRUCTURE; BEAMLINE; ACTINIDE AB The density of states predicted by cluster calculations of PuO2 and UO2 is directly compared to the results from soft x-ray spectroscopy. Remarkably good agreement between the experimentally measured spectroscopic peaks and the calculated density of states of the central part of the cluster is observed. (C) 2013 American Vacuum Society. [http://dx.doi.org/10.1116/1.4772959] C1 [Tobin, J. A.; Yu, S. -W.; Chung, B. W.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. [Ryzhkov, M. V.] Russian Acad Sci, Inst Solid State Chem, Ural Div, Ekaterinburg, Russia. [Mirmelstein, A.] EI Zababakhin Inst Tech Phys VNIITF, Russian Fed Nucl Ctr, Dept Expt Phys, Snezhinsk, Russia. RP Tobin, JA (reprint author), Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. EM Tobin1@LLNL.Gov RI Chung, Brandon/G-2929-2012 FU U.S. Department of Energy, National Nuclear Security Administration [DE-AC52-07NA27344]; DOE Office of Science, Office of Basic Energy Science, Division of Materials Science and Engineering; LLNL [B590089]; VNIITF [B590089]; DOE Office of Science, Office of Basic Energy Science FX Lawrence Livermore National Laboratory is operated by Lawrence Livermore National Security, LLC, for the U.S. Department of Energy, National Nuclear Security Administration under Contract No. DE-AC52-07NA27344. J.G.T. and S.-W.Y. were supported by the DOE Office of Science, Office of Basic Energy Science, Division of Materials Science and Engineering. Work at the RAS and VNIITF was supported in part by Contract B590089 between LLNL and VNIITF. The Advanced Light Source (ALS) in Berkeley and the Stanford Synchrotron Radiation Laboratory are supported by the DOE Office of Science, Office of Basic Energy Science. NR 14 TC 1 Z9 1 U1 2 U2 21 PU A V S AMER INST PHYSICS PI MELVILLE PA STE 1 NO 1, 2 HUNTINGTON QUADRANGLE, MELVILLE, NY 11747-4502 USA SN 0734-2101 J9 J VAC SCI TECHNOL A JI J. Vac. Sci. Technol. A PD JAN-FEB PY 2013 VL 31 IS 1 AR 013001 DI 10.1116/1.4772959 PG 3 WC Materials Science, Coatings & Films; Physics, Applied SC Materials Science; Physics GA 076BK UT WOS:000313931300009 ER PT J AU Ma, RM Oulton, RF Sorger, VJ Zhang, X AF Ma, Ren-Min Oulton, Rupert F. Sorger, Volker J. Zhang, Xiang TI Plasmon lasers: coherent light source at molecular scales SO LASER & PHOTONICS REVIEWS LA English DT Review DE Surface plasmon; laser; nanophotonics; ultrafast; miniaturization ID ENHANCED RAMAN-SCATTERING; CRYSTAL NANOCAVITY LASER; SURFACE-EMITTING LASERS; SPONTANEOUS EMISSION; MICROCAVITY LASERS; WAVE-GUIDES; QUANTUM-DOT; MU-M; LASING CHARACTERISTICS; NEAR-FIELD AB Plasmon lasers are a new class of coherent optical frequency electromagnetic wave amplifiers that deliver intense, coherent and directional surface plasmons well below the diffraction barrier. The strongly confined electric fields in plasmon lasers can enhance significantly light-matter interactions and bring fundamentally new capabilities to bio-sensing, data storage, photolithography and optical communications. C1 [Ma, Ren-Min; Oulton, Rupert F.; Sorger, Volker J.; Zhang, Xiang] Univ Calif Berkeley, NSF Nanoscale Sci & Engn Ctr, Berkeley, CA 94720 USA. [Zhang, Xiang] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. [Oulton, Rupert F.] Univ London Imperial Coll Sci Technol & Med, Blackett Lab, London SW7 2AZ, England. RP Zhang, X (reprint author), Univ Calif Berkeley, NSF Nanoscale Sci & Engn Ctr, 3112 Etcheverry Hall, Berkeley, CA 94720 USA. EM xiang@berkeley.edu RI Zhang, Xiang/F-6905-2011 FU Multidisciplinary University Research Initiative grant (Air Force Office of Scientific Research) [FA9550-10-1-0264] FX This work was supported by a Multidisciplinary University Research Initiative grant (Air Force Office of Scientific Research, FA9550-10-1-0264). NR 110 TC 78 Z9 81 U1 12 U2 202 PU WILEY-V C H VERLAG GMBH PI WEINHEIM PA POSTFACH 101161, 69451 WEINHEIM, GERMANY SN 1863-8880 EI 1863-8899 J9 LASER PHOTONICS REV JI Laser Photon. Rev. PD JAN PY 2013 VL 7 IS 1 BP 1 EP 21 DI 10.1002/lpor.201100040 PG 21 WC Optics; Physics, Applied; Physics, Condensed Matter SC Optics; Physics GA 077TQ UT WOS:000314051300003 ER PT J AU Raimunda, D Padilla-Benavides, T Vogt, S Boutigny, S Tomkinson, KN Finney, LA Arguello, JM AF Raimunda, Daniel Padilla-Benavides, Teresita Vogt, Stefan Boutigny, Sylvain Tomkinson, Kaleigh N. Finney, Lydia A. Argueello, Jose M. TI Periplasmic response upon disruption of transmembrane Cu transport in Pseudomonas aeruginosa SO METALLOMICS LA English DT Article ID COPPER HOMEOSTASIS; ESCHERICHIA-COLI; PROTEIN; ATPASES; AZURIN; SPECTROSCOPY; RESPIRATION; TOLERANCE; MECHANISM; REDUCTASE AB Pseudomonas aeruginosa, an opportunistic pathogen, has two transmembrane Cu+ transport ATPases, CopA1 and CopA2. Both proteins export cytoplasmic Cu+ into the periplasm and mutation of either gene leads to attenuation of virulence. CopA1 is required for maintaining cytoplasmic copper levels, while CopA2 provides copper for cytochrome c oxidase assembly. We hypothesized that transported Cu+ ions would be directed to their destination via specific periplasmic partners and disruption of transport should affect the periplasmic copper homeostasis. Supporting this, mutation of either ATPase gene led to large increments in periplasmic cuproprotein levels. Toward identifying the proteins participating in this cellular response the periplasmic metalloproteome was resolved in non-denaturing bidimensional gel electrophoresis, followed by X-ray fluorescence visualization and identification by mass-spectrometry. A single spot containing the electron shuttle protein azurin was responsible for the observed increments in cuproprotein contents. In agreement, lack of either Cu+-ATPase induced an increase in azu transcription. This is associated with an increase in the expression of anr and rpoS oxidative stress response regulators, rather than cueR, a copper sensing regulator. We propose that azurin overexpression and accumulation in the periplasm is part of the cellular response to cytoplasmic oxidative stress in P. aeruginosa. C1 [Raimunda, Daniel; Padilla-Benavides, Teresita; Boutigny, Sylvain; Tomkinson, Kaleigh N.; Argueello, Jose M.] Worcester Polytech Inst, Dept Chem & Biochem, Worcester, MA 01605 USA. [Vogt, Stefan; Finney, Lydia A.] Argonne Natl Lab, Xray Sci Div, Adv Photon Source, Lemont, IL USA. RP Arguello, JM (reprint author), Worcester Polytech Inst, Dept Chem & Biochem, Gateway Pk,100 Inst Rd, Worcester, MA 01605 USA. EM arguello@wpi.edu RI Arguello, Jose/D-1997-2012; Padilla-Benavides, Teresita/K-1968-2012; Vogt, Stefan/B-9547-2009; Vogt, Stefan/J-7937-2013 OI Arguello, Jose/0000-0003-3940-6297; Vogt, Stefan/0000-0002-8034-5513; Vogt, Stefan/0000-0002-8034-5513 FU Department of Energy, Office of Science [DE-AC-02-06CH11357]; NSF [MCB-0743901] FX The use of the Advanced Photon Source was supported by the Department of Energy, Office of Science Contract DE-AC-02-06CH11357. This work was supported by NSF grant MCB-0743901 (JMA). The authors thank Evan Maxey for his assistance in optimizing the instrumentation for this work in its new home at 8-BM-B and Robert Le for helping with sample preparations for XRF. NR 35 TC 8 Z9 8 U1 0 U2 19 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1756-5901 J9 METALLOMICS JI Metallomics PY 2013 VL 5 IS 2 BP 144 EP 151 DI 10.1039/c2mt20191g PG 8 WC Biochemistry & Molecular Biology SC Biochemistry & Molecular Biology GA 080UI UT WOS:000314268900005 PM 23354150 ER PT J AU Guevara, G Bonito, G Trappe, JM Cazares, E Williams, G Healy, RA Schadt, C Vilgalys, R AF Guevara, Gonzalo Bonito, Gregory Trappe, James M. Cazares, Efren Williams, Gwendolyn Healy, Rosanne A. Schadt, Christopher Vilgalys, Rytas TI New North American truffles (Tuber spp.) and their ectomycorrhizal associations SO MYCOLOGIA LA English DT Article DE Ascomycota; ectomycorrhizae; hypogeous fungi; Pezizales; Pezizomycetes; phylogeny ID HYPOGEOUS FUNGI; MEXICO; IDENTIFICATION; PHYLOGENY; DIVERSITY; SEQUENCES; FORESTS; TREES; DNA AB Recent surveys of belowground fungal biodiversity in Mexico and USA have revealed many undescribed truffle species, including many in the genus Tuber. Here we describe seven new species: Tuber beyerlei, T. castilloi, T. guevarai, T. lauryi, T. mexiusanum, T. miquihuanense and T. walkeri. Phylogenetic analyses place these species within the Maculatum group, an understudied clade of small truffles with little apparent economic value. These species are among the more taxonomically challenging in the genus. We collected Tuber castilloi, T. mexiusanum and T. guevarai as fruit bodies and ectomycorrhizae on Quercus spp. in forests of eastern Mexico. Tuber mexiusanum has a particularly broad geographic range, being collected in eastern USA under Populus deltoides and in Minnesota and Iowa in mixed hardwood forests. T. walkeri is described from the upper midwestern USA, and T. lauryi and T. beyerlei occur in the western USA. C1 [Guevara, Gonzalo] Inst Tecnol Cd Victoria, Cd Victoria 87010, Tamaulipas, Mexico. [Bonito, Gregory; Williams, Gwendolyn; Vilgalys, Rytas] Duke Univ, Dept Biol, Durham, NC 27708 USA. [Trappe, James M.; Cazares, Efren] Oregon State Univ, Dept Forest Ecosyst & Soc, Corvallis, OR 97331 USA. [Healy, Rosanne A.] Univ Minnesota, Dept Plant Biol Sci, St Paul, MN 55108 USA. [Schadt, Christopher] Oak Ridge Natl Lab, Biosci Div, Oak Ridge, TN 37831 USA. RP Bonito, G (reprint author), Duke Univ, Dept Biol, Durham, NC 27708 USA. EM gmb2@duke.edu RI Schadt, Christopher/B-7143-2008; OI Schadt, Christopher/0000-0001-8759-2448; Vilgalys, Rytas/0000-0001-8299-3605 FU DGEST (Direccion General de Educacion Superior Tecnologica); SES; ANUIES; CONACyT; National Science Foundation [DBI-0098534]; U.S. Forest Service, Pacific Northwest Research Station; Department of Energy, Office of Biological and Environmental Research, Genome Science Program; Iowa Science Foundation; Minnesota Department of Natural Resources FX The senior author thanks the DGEST (Direccion General de Educacion Superior Tecnologica, SES, ANUIES and CONACyT) for financially supporting this research. Participation by Efren Cazares and James Trappe was supported by National Science Foundation award DBI-0098534 and the U.S. Forest Service, Pacific Northwest Research Station. Gregory Bonito, Rytas Vilgalys and Christopher Schadt were supported through the Department of Energy, Office of Biological and Environmental Research, Genome Science Program. Rosanne Healy was supported by the Iowa Science Foundation and the Minnesota Department of Natural Resources. We thank Hannah Reynolds for generating sequence data on Tuber ectomycorrhizae of Populus, Jesus Garcia for loans of Tuber specimens. These herbaria generously accessioned and curated our collections: Duke University, Durham, North Carolina (DUKE); Instituto Tecnologico de Ciudad Victoria, Mexico (ITCV); Iowa State University, Ames (ISC); Oregon State University, Corvallis (OSC); University of Minnesota, Ames (MIN). NR 39 TC 14 Z9 14 U1 1 U2 24 PU ALLEN PRESS INC PI LAWRENCE PA 810 E 10TH ST, LAWRENCE, KS 66044 USA SN 0027-5514 J9 MYCOLOGIA JI Mycologia PD JAN-FEB PY 2013 VL 105 IS 1 BP 194 EP 209 DI 10.3852/12-087 PG 16 WC Mycology SC Mycology GA 082JB UT WOS:000314387000016 PM 22962353 ER PT J AU Wang, ML Saha, J Hada, M Anderson, JA Pluth, JM O'Neill, P Cucinotta, FA AF Wang, Minli Saha, Janapriya Hada, Megumi Anderson, Jennifer A. Pluth, Janice M. O'Neill, Peter Cucinotta, Francis A. TI Novel Smad proteins localize to IR-induced double-strand breaks: interplay between TGF beta and ATM pathways SO NUCLEIC ACIDS RESEARCH LA English DT Article ID DNA-DAMAGE RESPONSE; GROWTH-FACTOR; IONIZING-RADIATION; GAMMA-H2AX FOCI; MESENCHYMAL TRANSITION; SIGNALING PATHWAYS; HEAVY-IONS; DSB REPAIR; IN-SITU; ACTIVATION AB Cellular damage from ionizing radiation (IR) is in part due to DNA damage and reactive oxygen species, which activate DNA damage response (DDR) and cytokine signaling pathways, including the ataxia telangiectasia mutated (ATM) and transforming growth factor (TGF)beta/Smad pathways. Using classic double-strand breaks (DSBs) markers, we studied the roles of Smad proteins in DDR and the crosstalk between TGF beta and ATM pathways. We observed co-localization of phospho-Smad2 (pSmad2) and Smad7 with DSB repair proteins following low and high linear energy transfer (LET) radiation in human fibroblasts and epithelial cells. The decays of both foci were similar to that of gamma H2AX foci. Irradiation with high LET particles induced pSmad2 and Smad7 foci tracks indicating the particle trajectory through cells. pSmad2 foci were absent in S phase cells, while Smad7 foci were present in all phases of cell cycle. pSmad2 (but not Smad7) foci were completely abolished when ATM was depleted or inactivated. In contrast, a TGF beta receptor 1 (TGF beta R1) inhibitor abrogated Smad7, but not pSmad2 foci at DSBs sites. In summary, we suggest that Smad2 and Smad7 contribute to IR-induced DSB signaling in an ATM or TGF beta R1-dependent manner, respectively. C1 [Wang, Minli; Saha, Janapriya; Hada, Megumi] USRA Div Life Sci, Houston, TX 77058 USA. [Anderson, Jennifer A.; O'Neill, Peter] Univ Oxford, Gray Inst Radiat Oncol & Biol, Oxford OX3 7DQ, England. [Pluth, Janice M.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Cucinotta, FA (reprint author), NASA, Space Radiat Program, Lyndon B Johnson Space Ctr, Houston, TX 77058 USA. EM francis.a.cucinotta@nasa.gov FU NASA Space Radiation Program; US Department of Energy [DE-AI02-10ER64969, DE-SC0002296]; NASA FX The NASA Space Radiation Program and US Department of Energy [DE-AI02-10ER64969 and DE-SC0002296]. Funding for open access charge: NASA. NR 53 TC 21 Z9 21 U1 0 U2 6 PU OXFORD UNIV PRESS PI OXFORD PA GREAT CLARENDON ST, OXFORD OX2 6DP, ENGLAND SN 0305-1048 J9 NUCLEIC ACIDS RES JI Nucleic Acids Res. PD JAN PY 2013 VL 41 IS 2 BP 933 EP 942 DI 10.1093/nar/gks1038 PG 10 WC Biochemistry & Molecular Biology SC Biochemistry & Molecular Biology GA 078SZ UT WOS:000314121100029 PM 23221633 ER PT J AU Abramson, E Imre, D Beranek, J Wilson, J Zelenyuk, A AF Abramson, Evan Imre, Dan Beranek, Josef Wilson, Jacqueline Zelenyuk, Alla TI Experimental determination of chemical diffusion within secondary organic aerosol particles SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID ULTRAFINE PARTICLES; PHASE STATE; OZONOLYSIS; EVAPORATION; VOLATILITY; PRECURSORS; ATMOSPHERE; MORPHOLOGY; EVOLUTION; DENSITY AB Formation, properties, transformations, and temporal evolution of secondary organic aerosol (SOA) particles depend strongly on SOA phase. Recent experimental evidence from both our group and several others indicates that, in contrast to common models' assumptions, SOA constituents do not form a low-viscosity, well-mixed solution, yielding instead a semisolid phase with high, but undetermined, viscosity. We find that when SOA particles are made in the presence of vapors of semi-volatile hydrophobic compounds, such molecules become trapped in the particles' interiors and their subsequent evaporation rates and thus their rates of diffusion through the SOA can be directly obtained. Using pyrene as the tracer molecule and SOA derived from alpha-pinene ozonolysis, we find that it takes similar to 24 hours for half the pyrene to evaporate. Based on the observed pyrene evaporation kinetics we estimate a diffusivity of 2.5 x 10(-21) m(2) s(-1) for pyrene in SOA. Similar measurements on SOA doped with fluoranthene and phenanthrene yield diffusivities comparable to that of pyrene. Assuming a Stokes-Einstein relation, an approximate viscosity of 10(8) Pa s can be calculated for this SOA. Such a high viscosity is characteristic of tars and is consistent with published measurements of SOA particle bounce, evaporation kinetics, and the stability of two reverse-layered morphologies. We show that a viscosity of 10(8) Pa s implies coalescence times of minutes, consistent with the findings that SOA particles formed by coagulation are spherical on the relevant experimental timescales. Measurements on aged SOA particles doped with pyrene yield an estimated diffusivity similar to 3 times smaller, indicating that hardening occurs with time, which is consistent with the increase in SOA oligomer content, decrease in water uptake, and decrease in evaporation rates previously observed with aging. C1 [Abramson, Evan] Univ Washington, Dept Earth & Space Sci, Seattle, WA 98195 USA. [Imre, Dan] Imre Consulting, Richland, WA 99352 USA. [Beranek, Josef; Wilson, Jacqueline; Zelenyuk, Alla] Pacific NW Natl Lab, Richland, WA 99354 USA. RP Zelenyuk, A (reprint author), Pacific NW Natl Lab, Richland, WA 99354 USA. EM alla.zelenyuk@pnnl.gov OI abramson, evan/0000-0001-5278-0836 FU U. S. Department of Energy Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Bioscience Division and Office of Biological and Environmental Research (Atmospheric Research Program); Department of Energy's Office of Biological and Environmental Research at Pacific Northwest National Laboratory (PNNL); US Department of Energy by Battelle Memorial Institute [DE-AC06-76RL0 1830] FX This work was supported by the U. S. Department of Energy Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Bioscience Division and Office of Biological and Environmental Research (Atmospheric Research Program). This research was performed in the Environmental Molecular Sciences Laboratory, a national scientific user facility sponsored by the Department of Energy's Office of Biological and Environmental Research at Pacific Northwest National Laboratory (PNNL). PNNL is operated by the US Department of Energy by Battelle Memorial Institute under contract No. DE-AC06-76RL0 1830. NR 38 TC 59 Z9 59 U1 6 U2 103 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2013 VL 15 IS 8 BP 2983 EP 2991 DI 10.1039/c2cp44013j PG 9 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 082BD UT WOS:000314365800044 PM 23340901 ER PT J AU Chen, F Tobimatsu, Y Jackson, L Nakashima, J Ralph, J Dixon, RA AF Chen, Fang Tobimatsu, Yuki Jackson, Lisa Nakashima, Jin Ralph, John Dixon, Richard A. TI Novel seed coat lignins in the Cactaceae: structure, distribution and implications for the evolution of lignin diversity SO PLANT JOURNAL LA English DT Article DE Cactaceae; caffeyl alcohol; lignin composition; nuclear magnetic resonance spectroscopy; seed coat; taxonomy ID CELL-WALL BIOSYNTHESIS; SEQUENCE VARIATION; ARABIDOPSIS; NMR; THIOACIDOLYSIS; MONOLIGNOLS; PHYLOGENY; ALCOHOL; POPLARS; COMT AB We have recently described a hitherto unsuspected catechyl lignin polymer (C-lignin) in the seed coats of Vanilla orchid and in cacti of one genus, Melocactus (Chen et al., Proc. Natl. Acad. Sci. USA. 2012, 109, 1772-1777.). We have now determined the lignin types in the seed coats of 130 different cactus species. Lignin in the vegetative tissues of cacti is of the normal guaiacyl/syringyl (G/S) type, but members of most genera within the subfamily Cactoidae possess seed coat lignin of the novel C-type only, which we show is a homopolymer formed by endwise beta-O-4-coupling of caffeyl alcohol monomers onto the growing polymer resulting in benzodioxane units. However, the species examined within the genera Coryphantha, Cumarinia, Escobaria and Mammillaria (Cactoideae) mostly had normal G/S lignin in their seeds, as did all six species in the subfamily Opuntioidae that were examined. Seed coat lignin composition is still evolving in the Cactaceae, as seeds of one Mammillaria species (M. lasiacantha) possess only C-lignin, three Escobaria species (E. dasyacantha, E. lloydii and E. zilziana) contain an unusual lignin composed of 5-hydroxyguaiacyl units, the first report of such a polymer that occurs naturally in plants, and seeds of some species contain no lignin at all. We discuss the implications of these findings for the mechanisms that underlie the biosynthesis of these newly discovered lignin types. C1 [Chen, Fang; Jackson, Lisa; Nakashima, Jin; Dixon, Richard A.] Samuel Roberts Noble Fdn Inc, Div Plant Biol, Ardmore, OK 73401 USA. [Tobimatsu, Yuki; Ralph, John] Univ Wisconsin, Enzyme Inst, Dept Biochem, Madison, WI 53726 USA. [Chen, Fang; Dixon, Richard A.] DOE Bioenergy Sci Ctr, Oak Ridge, TN USA. [Ralph, John] DOE Great Lakes Bioenergy Res Ctr, Madison, WI USA. [Ralph, John] Wisconsin Bioenergy Initiat, Madison, WI USA. RP Chen, F (reprint author), Samuel Roberts Noble Fdn Inc, Div Plant Biol, 2510 Sam Noble Pkwy, Ardmore, OK 73401 USA. EM fchen@noble.org; radixon@noble.org FU Samuel Roberts Noble Foundation; US Department of Energy's Bioenergy Sciences and Great Lakes Bioenergy Centers [BER DE-AC05-00OR22725]; Office of Biological and Environmental Research in the DOE Office of Science [DE-FC02-07ER64494]; Japan Society for the Promotion of Science (JSPS) FX We thank Drs Xiaoqiang Wang and Qiao Zhao for critical reading of the manuscript. This work was supported by the Samuel Roberts Noble Foundation, and the US Department of Energy's Bioenergy Sciences and Great Lakes Bioenergy Centers, supported by the Office of Biological and Environmental Research in the DOE Office of Science (BER DE-AC05-00OR22725 and DE-FC02-07ER64494, respectively). YT acknowledges Postdoctoral Fellowship support from the Japan Society for the Promotion of Science (JSPS). NR 31 TC 20 Z9 20 U1 6 U2 74 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0960-7412 J9 PLANT J JI Plant J. PD JAN PY 2013 VL 73 IS 2 BP 201 EP 211 DI 10.1111/tpj.12012 PG 11 WC Plant Sciences SC Plant Sciences GA 079PR UT WOS:000314184000003 PM 22957702 ER PT J AU Zayas, J AF Zayas, Jose TI Advancing the Development and Deployment of Ocean Renewable Energy SO SEA TECHNOLOGY LA English DT Article C1 US DOE, Wind & Water Power Technol Off, Washington, DC 20585 USA. RP Zayas, J (reprint author), US DOE, Wind & Water Power Technol Off, Washington, DC 20585 USA. NR 0 TC 1 Z9 1 U1 1 U2 5 PU COMPASS PUBLICATIONS, INC PI ARLINGTON PA 1501 WILSON BLVD., STE 1001, ARLINGTON, VA 22209-2403 USA SN 0093-3651 J9 SEA TECHNOL JI Sea Technol. PD JAN PY 2013 VL 54 IS 1 BP 16 EP 18 PG 3 WC Engineering, Ocean SC Engineering GA 082IV UT WOS:000314386400005 ER PT J AU Lin, F Gillaspie, DT Dillon, AC Richards, RM Engtrakul, C AF Lin, Feng Gillaspie, Dane T. Dillon, Anne C. Richards, Ryan M. Engtrakul, Chaiwat TI Nitrogen-doped nickel oxide thin films for enhanced electrochromic applications SO THIN SOLID FILMS LA English DT Article DE Nitrogen-doped nickel oxide; Electrochromic properties; Reversibility; Coloration efficiency; Switching kinetics; Sputtering ID PERFORMANCE; ELECTRODES; NIO AB In this work, Ni oxide and nitrogen (N)-doped Ni oxide electrochromic films were fabricated with radio frequency magnetron sputtering from a ceramic Ni oxide target. Nitrogen gas was used as the precursor for N doping. The N dopant resulted in Ni oxide films with decreased lattice parameters, increased degree of crystallinity and enhanced surface roughness. The electrochromic performance of the resulting films was evaluated in a LiClO4 electrolyte dissolved in propylene carbonate. The charge reversibility and coloration efficiency as well as the coloration and bleaching kinetics for the N-doped Ni oxide films were significantly improved relative to the undoped Ni oxide films. (C) 2012 Elsevier B. V. All rights reserved. C1 [Lin, Feng; Gillaspie, Dane T.; Dillon, Anne C.; Engtrakul, Chaiwat] Natl Renewable Energy Lab, Golden, CO 80401 USA. [Richards, Ryan M.] Colorado Sch Mines, Dept Chem & Geochem, Golden, CO 80401 USA. [Lin, Feng; Richards, Ryan M.] Colorado Sch Mines, Mat Sci Program, Golden, CO 80401 USA. RP Engtrakul, C (reprint author), Natl Renewable Energy Lab, 1617 Cole Blvd, Golden, CO 80401 USA. EM chaiwat.engtrakul@nrel.gov RI Lin, Feng/H-5027-2012; Richards, Ryan/B-3513-2008 OI Lin, Feng/0000-0001-7286-7525; FU U.S. Department of Energy [DE-AC36-08-GO28308]; Colorado School of Mines; National Renewable Energy Laboratory as part of the DOE Office of Energy Efficiency and Renewable Energy Office of Building Technologies Program FX This research was supported by the U.S. Department of Energy under contract number DE-AC36-08-GO28308 with the National Renewable Energy Laboratory as part of the DOE Office of Energy Efficiency and Renewable Energy Office of Building Technologies Program. The authors would like to acknowledge the guidance from the Sage Electrochromics, Inc. The authors also thank Prof. Tim Ohno and Harrison Wilterdink for the help with XPS data acquisition, and Dr. John Chandler for the help with SEM. F. L. and R. M. R would like to thank the support from the Colorado School of Mines. F. L. would like to thank Dr. Robert Tenent and N. Edwin Widjonarko for the thoughtful discussions. NR 26 TC 13 Z9 13 U1 4 U2 80 PU ELSEVIER SCIENCE SA PI LAUSANNE PA PO BOX 564, 1001 LAUSANNE, SWITZERLAND SN 0040-6090 J9 THIN SOLID FILMS JI Thin Solid Films PD JAN 1 PY 2013 VL 527 BP 26 EP 30 DI 10.1016/j.tsf.2012.12.031 PG 5 WC Materials Science, Multidisciplinary; Materials Science, Coatings & Films; Physics, Applied; Physics, Condensed Matter SC Materials Science; Physics GA 077OO UT WOS:000314037200005 ER PT J AU Malone, EL AF Malone, Elizabeth L. TI Climate Change and National Security SO WEATHER CLIMATE AND SOCIETY LA English DT Article ID CONFLICT AB Climate change is increasingly recognized as having national security implications, which has prompted dialogue between the climate change and national security communities with resultant advantages and differences. Climate change research has proven useful to the national security community sponsors in several ways. It has opened security discussions to consider climate as well as political factors in studies of the future. It has encouraged factoring in the stresses placed on societies by climate changes (of any kind) to help assess the potential for state stability. And it has shown that changes such as increased heat, more intense storms, longer periods without rain, and earlier spring onset call for building climate resilience as part of building stability. For the climate change research community, studies from a national security point of view have revealed research lacunae, such as the lack of usable migration studies. This has also pushed the research community to consider second- and third-order impacts of climate change, such as migration and state stability, which broadens discussion of future impacts beyond temperature increases, severe storms, and sea level rise and affirms the importance of governance in responding to these changes. The increasing emphasis in climate change science toward research in vulnerability, resilience, and adaptation also frames what the intelligence and defense communities need to know, including where there are dependencies and weaknesses that may allow climate change impacts to result in security threats and where social and economic interventions can prevent climate change impacts and other stressors from resulting in social and political instability or collapse. C1 Pacific NW Natl Lab, Joint Global Change Res Inst, College Pk, MD 20740 USA. RP Malone, EL (reprint author), Pacific NW Natl Lab, Joint Global Change Res Inst, 5825 Univ Res Court,Suite 3500, College Pk, MD 20740 USA. EM e.malone@pnnl.gov NR 17 TC 1 Z9 1 U1 2 U2 20 PU AMER METEOROLOGICAL SOC PI BOSTON PA 45 BEACON ST, BOSTON, MA 02108-3693 USA SN 1948-8327 J9 WEATHER CLIM SOC JI Weather Clim. Soc. PD JAN PY 2013 VL 5 IS 1 BP 93 EP 95 DI 10.1175/WCAS-D-12-00016.1 PG 3 WC Environmental Studies; Meteorology & Atmospheric Sciences SC Environmental Sciences & Ecology; Meteorology & Atmospheric Sciences GA 082JJ UT WOS:000314387800009 ER PT J AU Baran, R Bowen, BP Price, MN Arkin, AP Deutschbauer, AM Northen, TR AF Baran, Richard Bowen, Benjamin P. Price, Morgan N. Arkin, Adam P. Deutschbauer, Adam M. Northen, Trent R. TI Metabolic Footprinting of Mutant Libraries to Map Metabolite Utilization to Genotype SO ACS CHEMICAL BIOLOGY LA English DT Article ID SYNECHOCOCCUS-SP. PCC-7002; ESCHERICHIA-COLI; MASS-SPECTROMETRY; HIGH-THROUGHPUT; COMPARATIVE GENOMICS; GENE-PRODUCT; CELL-WALL; SEPARATION; BACTERIA; ENZYME AB The discrepancy between the pace of sequencing and functional characterization of genomes is a major challenge in understanding complex microbial metabolic processes and metabolic interactions in the environment. Here, we identified and validated genes related to the utilization of specific metabolites in bacteria by profiling metabolite utilization in libraries of mutant strains. Untargeted mass spectrometry based metabolomics was used to identify metabolites utilized by Escherichia coli and Shewanella oneidensis MR-1. Targeted high-throughput metabolite profiling of spent media of 8042 individual mutant strains was performed to link utilization to specific genes. Using this approach we identified genes of known function as well as novel transport proteins and enzymes required for the utilization of tested metabolites. Specific examples indude two subunits of a predicted ABC transporter encoded by the genes SO1043 and SO1044 required for the utilization of citrulline and a predicted histidase encoded by the gene SO3057 required for the utilization of ergothioneine by S. oneidensis. In vitro assays with purified proteins showed substrate specificity of SO3057 toward ergothioneine and histidine betaine in contrast to substrate specificity of a paralogous histidase SO0098 toward histidine. This generally applicable, high-throughput workflow has the potential both to discover novel metabolic capabilities of microorganisms and to identify the corresponding genes. C1 [Baran, Richard; Bowen, Benjamin P.; Northen, Trent R.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Life Sci, Berkeley, CA 94720 USA. [Price, Morgan N.; Arkin, Adam P.; Deutschbauer, Adam M.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA 94720 USA. RP Northen, TR (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Life Sci, 1 Cyclotron Rd, Berkeley, CA 94720 USA. EM trnorthen@lbl.gov RI Arkin, Adam/A-6751-2008; OI Arkin, Adam/0000-0002-4999-2931; Northen, Trent/0000-0001-8404-3259 FU Office of Science, Office of Biological and Environmental Research, of the U.S. Department of Energy [DE-AC02-05CH11231] FX We thank K. Wetmore for assistance in high-throughput bacterial culturing and J. Ray for assistance with protein purification. This work conducted by ENIGMA- Ecosystems and Networks Integrated with Genes and Molecular Assemblies 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. NR 50 TC 15 Z9 15 U1 1 U2 29 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 1554-8929 J9 ACS CHEM BIOL JI ACS Chem. Biol. PD JAN PY 2013 VL 8 IS 1 BP 189 EP 199 DI 10.1021/cb300477w PG 11 WC Biochemistry & Molecular Biology SC Biochemistry & Molecular Biology GA 077DL UT WOS:000314008000022 PM 23082955 ER PT J AU Dietrich, JA Shis, DL Alikhani, A Keasling, JD AF Dietrich, Jeffrey A. Shis, David L. Alikhani, Azadeh Keasling, Jay D. TI Transcription Factor-Based Screens and Synthetic Selections for Microbial Small-Molecule Biosynthesis SO ACS SYNTHETIC BIOLOGY LA English DT Article ID BIODEGRADATIVE THREONINE DEHYDRATASE; ESCHERICHIA-COLI; PSEUDOMONAS-PUTIDA; METABOLIC PATHWAYS; SUCCINATE YIELD; GENE; DATABASE; DESIGN; ACID; PRODUCTIVITY AB Continued advances in metabolic engineering are increasing the number of small molecules being targeted for microbial production. Pathway yields and productivities, however, are often suboptimal, and strain improvement remains a persistent challenge given that the majority of small molecules are difficult to screen for and their biosynthesis does not improve host fitness. In this work, we have developed a generalized approach to screen or select for improved small-molecule biosynthesis using transcription factor-based biosensors. Using a tetracycline resistance gene 3' of a small-molecule inducible promoter, host resistance, and hence growth rate, was coupled to either small-molecule concentration in the growth medium or a small-molecule production phenotype. Biosensors were constructed for two important, chemical classes, dicarboxylic acids and alcohols, using transcription factor-promoter pairs derived from Pseudomonas putida, Thauera butanivorans, or E.coli Transcription factors were selected for specific activation by either succinate, adipate, or 1-butanol, and we demonstrate pro product-dependent growth in E. coli using all three compounds. The 1-butanol biosensor was applied in a proof-of-principle liquid culture screen to optimize 1-butanol biosynthesis in engineered E. coli, identifying a pathway variant yielding a 35% increase in 1-butanol specific productivity through optimization of enzyme expression levels. Lastly, to demonstrate the capacity to select for enzymatic activity, the 1-butanol biosensor was applied as synthetic selection, coupling in vivo 1-butanol biosynthesis to E. coli fitness, and an 120-fold enrichment for a 1-butanol production phenotype was observed following a single, round, of positive selection. C1 [Dietrich, Jeffrey A.; Keasling, Jay D.] UCSF UCB Joint Grad Grp Bioengn, Berkeley, CA 94720 USA. [Dietrich, Jeffrey A.; Shis, David L.; Keasling, Jay D.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, Synthet Biol Dept, Berkeley, CA 94720 USA. [Dietrich, Jeffrey A.; Shis, David L.; Keasling, Jay D.] Joint BioEnergy Inst, Emeryville, CA 94608 USA. [Dietrich, Jeffrey A.; Alikhani, Azadeh] Lygos Inc, San Francisco, CA 94124 USA. [Keasling, Jay D.] Univ Calif Berkeley, Dept Chem & Biomol Engn, Berkeley, CA 94720 USA. [Keasling, Jay D.] Univ Calif Berkeley, Calif Inst Quantitat Biomed Res, Berkeley, CA 94720 USA. RP Keasling, JD (reprint author), UCSF UCB Joint Grad Grp Bioengn, Berkeley, CA 94720 USA. EM jdkeasling@lbl.gov RI Keasling, Jay/J-9162-2012 OI Keasling, Jay/0000-0003-4170-6088 FU DOE Joint BioEnergy Institute; U.S. Department of Energy, Office of Science, Office of Biological and Environmental Research [DE-AC02-05CH11231]; U.S. Department of Energy; Siebel Scholars Foundation; NIH Applied Biology and Bioprocess Engineering Training Grant; QB3 Biocatalyst Grant; Department of Energy [DE-SC0006469] FX This work was part of the DOE Joint BioEnergy Institute supported by the U.S. Department of Energy, Office of Science, Office of Biological and Environmental Research through the contract DE-AC02-05CH11231 between Lawrence Berkeley National Laboratory and the U.S. Department of Energy. J.A.D. acknowledges a fellowship from the Siebel Scholars Foundation, funding from the NIH Applied Biology and Bioprocess Engineering Training Grant, and a QB3 Biocatalyst Grant. The dicarboxylic acid material is based upon work supported by the Department of Energy under Award Number DE-SC0006469. We thank W. Holtz, J. Carothers, and J. Gilmore for critical reading of the manuscript. NR 61 TC 46 Z9 47 U1 7 U2 72 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 2161-5063 J9 ACS SYNTH BIOL JI ACS Synth. Biol. PD JAN PY 2013 VL 2 IS 1 BP 47 EP 58 DI 10.1021/sb300091d PG 12 WC Biochemical Research Methods SC Biochemistry & Molecular Biology GA 075XG UT WOS:000313919900005 PM 23656325 ER PT J AU Perera, M Metz, RB Kostko, O Ahmed, M AF Perera, Manori Metz, Ricardo B. Kostko, Oleg Ahmed, Musahid TI Vacuum Ultraviolet Photoionization Studies of PtCH2 and H-Pt-CH3: A Potential Energy Surface for the Pt+CH4 Reaction SO ANGEWANDTE CHEMIE-INTERNATIONAL EDITION LA English DT Article DE C-H activation; methane; photoionization; platinum; reaction intermediates ID METAL-IONS; METHANE ACTIVATION; PLATINUM; KINETICS; ATOMS; SYNCHROTRON; CLUSTERS; ALKANES; NWCHEM; CH4 C1 [Metz, Ricardo B.] Univ Massachusetts, Dept Chem, Amherst, MA 01003 USA. [Perera, Manori] Illinois Wesleyan Univ, Dept Chem, Bloomington, IL 61702 USA. [Kostko, Oleg; Ahmed, Musahid] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. RP Metz, RB (reprint author), Univ Massachusetts, Dept Chem, Amherst, MA 01003 USA. EM rbmetz@chem.umass.edu RI Ahmed, Musahid/A-8733-2009; Kostko, Oleg/B-3822-2009; OI Kostko, Oleg/0000-0003-2068-4991; Metz, Ricardo/0000-0003-1933-058X FU Office of Energy Research, Office of Basic Energy Sciences, Chemical Sciences Division of the U.S. Department of Energy [DE-AC02-05CH11231]; National Science Foundation [CHE-0911225] FX M.A., O.K., and the ALS are 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 No. DE-AC02-05CH11231. M. P. and R. B. M. gratefully acknowledge the support of the National Science Foundation under Award CHE-0911225. NR 25 TC 8 Z9 8 U1 1 U2 35 PU WILEY-V C H VERLAG GMBH PI WEINHEIM PA BOSCHSTRASSE 12, D-69469 WEINHEIM, GERMANY SN 1433-7851 J9 ANGEW CHEM INT EDIT JI Angew. Chem.-Int. Edit. PY 2013 VL 52 IS 3 BP 888 EP 891 DI 10.1002/anie.201207931 PG 4 WC Chemistry, Multidisciplinary SC Chemistry GA 072QU UT WOS:000313688100014 PM 23315902 ER PT J AU Schlicke, H Ghosh, D Fong, LK Xin, HLL Zheng, HM Alivisatos, AP AF Schlicke, Hendrik Ghosh, Debraj Fong, Lam-Kiu Xin, Huolin L. Zheng, Haimei Alivisatos, A. Paul TI Selective Placement of Faceted Metal Tips on Semiconductor Nanorods SO ANGEWANDTE CHEMIE-INTERNATIONAL EDITION LA English DT Article DE cadmium sulfide; carbon monoxide; hybrid structures; nanostructures; platinum ID CORE/SHELL NANOCRYSTALS; CDS NANORODS; GROWTH; NANOPARTICLES; HETEROSTRUCTURES; HYDROGENATION; BINARY; BRIGHT; RODS; SIZE C1 [Schlicke, Hendrik; Ghosh, Debraj; Fong, Lam-Kiu; Alivisatos, A. Paul] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Schlicke, Hendrik; Ghosh, Debraj; Fong, Lam-Kiu; Xin, Huolin L.; Zheng, Haimei; Alivisatos, A. Paul] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. RP Alivisatos, AP (reprint author), Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. EM alivis@berkeley.edu RI Foundry, Molecular/G-9968-2014; Xin, Huolin/E-2747-2010; Alivisatos , Paul /N-8863-2015 OI Xin, Huolin/0000-0002-6521-868X; Alivisatos , Paul /0000-0001-6895-9048 FU Physical Chemistry of Inorganic Nanocrystals Program, Office of Science, Office of Basic Energy Sciences, of the United States Department of Energy [DE-AC02-05CH11231]; Studienstiftung des deutschen Volkes; National Science Foundation American Competitiveness in Chemistry Post-doctoral Fellowship [0936997]; U.S. DOE Office of Science Early Career Research Program; U.S. Department of Energy (DOE) [DE-AC02-05CH11231] FX This work was supported by the Physical Chemistry of Inorganic Nanocrystals Program, Director, Office of Science, Office of Basic Energy Sciences, of the United States Department of Energy under contract DE-AC02-05CH11231. H. S. thanks the Studienstiftung des deutschen Volkes for support. D. G. was supported by the National Science Foundation American Competitiveness in Chemistry Post-doctoral Fellowship award number 0936997. H.Z. thanks the funding support of the U.S. DOE Office of Science Early Career Research Program. TEM experiments were performed at the National Center for Electron Microscopy (NCEM) of the Lawrence Berkeley National Laboratory (LBNL), which is supported by the U.S. Department of Energy (DOE) under Contract No. DE-AC02-05CH11231. We thank Brandon Beberwyck and Dr. Marcus Scheele for support with XRD measurements. Also, we thank Dr. Trevor Evers and Fadekemi Oba for helpful discussions. NR 25 TC 19 Z9 19 U1 3 U2 96 PU WILEY-V C H VERLAG GMBH PI WEINHEIM PA BOSCHSTRASSE 12, D-69469 WEINHEIM, GERMANY SN 1433-7851 J9 ANGEW CHEM INT EDIT JI Angew. Chem.-Int. Edit. PY 2013 VL 52 IS 3 BP 980 EP 982 DI 10.1002/anie.201205958 PG 3 WC Chemistry, Multidisciplinary SC Chemistry GA 072QU UT WOS:000313688100035 PM 23192900 ER PT J AU Buton, C Copin, Y Aldering, G Antilogus, P Aragon, C Bailey, S Baltay, C Bongard, S Canto, A Cellier-Holzem, F Childress, M Chotard, N Fakhouri, HK Gangler, E Guy, J Hsiao, EY Kerschhaggl, M Kowalski, M Loken, S Nugent, P Paech, K Pain, R Pecontal, E Pereira, R Perlmutter, S Rabinowitz, D Rigault, M Runge, K Scalzo, R Smadja, G Tao, C Thomas, RC Weaver, BA Wu, C AF Buton, C. Copin, Y. Aldering, G. Antilogus, P. Aragon, C. Bailey, S. Baltay, C. Bongard, S. Canto, A. Cellier-Holzem, F. Childress, M. Chotard, N. Fakhouri, H. K. Gangler, E. Guy, J. Hsiao, E. Y. Kerschhaggl, M. Kowalski, M. Loken, S. Nugent, P. Paech, K. Pain, R. Pecontal, E. Pereira, R. Perlmutter, S. Rabinowitz, D. Rigault, M. Runge, K. Scalzo, R. Smadja, G. Tao, C. Thomas, R. C. Weaver, B. A. Wu, C. CA Nearby SuperNova Factory TI Atmospheric extinction properties above Mauna Kea from the Nearby SuperNova Factory spectro-photometric data set SO ASTRONOMY & ASTROPHYSICS LA English DT Article DE atmospheric effects; instrumentation: spectrographs; methods: observational; techniques: imaging spectroscopy ID INTEGRAL-FIELD SPECTROGRAPH; ABSORPTION CROSS-SECTIONS; GROUP SITE SURVEY; OPTICAL-PROPERTIES; SKY-TRANSPARENCY; TOTAL OZONE; LA-SILLA; VARIABILITY; BRIGHTNESS; SCATTERING AB We present a new atmospheric extinction curve for Mauna Kea spanning 3200-9700 angstrom. It is the most comprehensive to date, being based on some 4285 standard star spectra obtained on 478 nights spread over a period of 7 years obtained by the Nearby SuperNova Factory using the SuperNova Integral Field Spectrograph. This mean curve and its dispersion can be used as an aid in calibrating spectroscopic or imaging data from Mauna Kea, and in estimating the calibration uncertainty associated with the use of a mean extinction curve. Our method for decomposing the extinction curve into physical components, and the ability to determine the chromatic portion of the extinction even on cloudy nights, is described and verified over the wide range of conditions sampled by our large dataset. We demonstrate good agreement with atmospheric science data obtain at nearby Mauna Loa Observatory, and with previously published measurements of the extinction above Mauna Kea. C1 [Buton, C.; Kerschhaggl, M.; Kowalski, M.; Paech, K.] Univ Bonn, Inst Phys, D-53115 Bonn, Germany. [Copin, Y.; Gangler, E.; Pereira, R.; Rigault, M.; Smadja, G.] Univ Lyon, F-69622 Villeurbanne, France. [Copin, Y.; Gangler, E.; Pereira, R.; Rigault, M.; Smadja, G.] Univ Lyon 1, F-69622 Villeurbanne, France. [Copin, Y.; Gangler, E.; Pereira, R.; Rigault, M.; Smadja, G.] Inst Phys Nucl, CNRS IN2P3, Lyon, France. [Aldering, G.; Aragon, C.; Bailey, S.; Childress, M.; Fakhouri, H. K.; Hsiao, E. Y.; Loken, S.; Perlmutter, S.; Runge, K.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Phys, Berkeley, CA 94720 USA. [Antilogus, P.; Bongard, S.; Canto, A.; Cellier-Holzem, F.; Guy, J.; Pain, R.; Wu, C.] Univ Paris 07, Univ Paris 06, Lab Phys Nucl & Hautes Energies, CNRS IN2P3, F-75252 Paris 05, France. [Baltay, C.; Rabinowitz, D.; Scalzo, R.] Yale Univ, Dept Phys, New Haven, CT 06250 USA. [Childress, M.; Fakhouri, H. K.; Perlmutter, S.] Univ Calif Berkeley, Dept Phys, Berkeley, CA 94720 USA. [Chotard, N.; Tao, C.] Tsinghua Univ, Tsinghua Ctr Astrophys, Beijing 100084, Peoples R China. [Chotard, N.; Wu, C.] Chinese Acad Sci, Natl Astron Observ, Beijing 100012, Peoples R China. [Nugent, P.; Thomas, R. C.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Computat Res Div, Computat Cosmol Ctr, Berkeley, CA 94720 USA. [Nugent, P.] Univ Calif Berkeley, Dept Astron, Berkeley, CA 94720 USA. [Pecontal, E.] Univ Lyon 1, Ctr Rech Astron Lyon, F-69561 St Genis Laval, France. [Scalzo, R.] Australian Natl Univ, Mt Stromlo & Siding Spring Observ, Res Sch Astron & Astrophys, Weston, ACT 2611, Australia. [Tao, C.] CPPM, F-13288 Marseille 09, France. [Weaver, B. A.] NYU, Ctr Cosmol & Particle Phys, New York, NY 10003 USA. RP Buton, C (reprint author), Univ Bonn, Inst Phys, Nussallee 11, D-53115 Bonn, Germany. RI Copin, Yannick/B-4928-2015; Perlmutter, Saul/I-3505-2015; OI Copin, Yannick/0000-0002-5317-7518; Perlmutter, Saul/0000-0002-4436-4661; Scalzo, Richard/0000-0003-3740-1214 FU CNRS/IN2P3; CNRS/INSU; CNRS/PNC; DFG [TRR33]; National Natural Science Foundation of China [10903010]; Office of Science, Office of High Energy and Nuclear Physics; Office of Advanced Scientific Computing Research, of the US Department of Energy (DOE) [DE-FG02-92ER40704, DE-AC02-05CH11231, DE-FG02-06ER06-04]; Gordon & Betty Moore Foundation; National Science Foundation [AST-0407297, 0087344, 0426879, AST-0838261]; Henri Chretien International Research Grant; France-Berkeley Fund; Region Rhone-Alpes FX We are grateful to the technical and scientific staff of the University of Hawaii 2.2-m telescope for their assistance in obtaining these data. D. Birchall assisted with acquisition of the data presented here. We also thank the people of Hawaii for access to Mauna Kea. This work was supported in France by CNRS/IN2P3, CNRS/INSU, CNRS/PNC, and used the resources of the IN2P3 computer center; this work was supported by the DFG through TRR33 "The Dark Universe", and by National Natural Science Foundation of China (grant 10903010). C. WU acknowledges support from the National Natural Science Foundation of China grant 10903010. This work was also supported in part by the Director, Office of Science, Office of High Energy and Nuclear Physics and the Office of Advanced Scientific Computing Research, of the US Department of Energy (DOE) under Contract Nos. DE-FG02-92ER40704, DE-AC02-05CH11231, DE-FG02-06ER06-04, and DE-AC02-05CH11231; by a grant from the Gordon & Betty Moore Foundation; by National Science Foundation Grant Nos. AST-0407297 (QUEST), and 0087344 & 0426879 (HPWREN); by a Henri Chretien International Research Grant administrated by the American Astronomical Society; the France-Berkeley Fund; by an Explora'Doc Grant by the Region Rhone-Alpes. We thank the AERONET principal investigator Brent Holben and his staff for its effort in establishing and maintaining the AERONET sites. The Caltech Submillimeter Observatory is operated by the California Institute of Technology under cooperative agreement with the National Science Foundation (AST-0838261). NR 57 TC 21 Z9 21 U1 1 U2 7 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 0004-6361 J9 ASTRON ASTROPHYS JI Astron. Astrophys. PD JAN PY 2013 VL 549 AR A8 DI 10.1051/0004-6361/201219834 PG 21 WC Astronomy & Astrophysics SC Astronomy & Astrophysics GA 073LR UT WOS:000313745000008 ER PT J AU Vreeswijk, PM Ledoux, C Raassen, AJJ Smette, A De Cia, A Wozniak, PR Fox, AJ Vestrand, WT Jakobsson, P AF Vreeswijk, P. M. Ledoux, C. Raassen, A. J. J. Smette, A. De Cia, A. Wozniak, P. R. Fox, A. J. Vestrand, W. T. Jakobsson, P. TI Time-dependent excitation and ionization modelling of absorption-line variability due to GRB080310 SO ASTRONOMY & ASTROPHYSICS LA English DT Article DE atomic processes; radiative transfer; gamma-ray burst: individual: GRB 080310; quasars: absorption lines; radiation mechanisms: thermal; galaxies: ISM ID GAMMA-RAY BURST; PHOTOIONIZATION CROSS-SECTIONS; ATOMIC TRANSITION-PROBABILITIES; GRB HOST GALAXIES; OPTICAL AFTERGLOWS; MOLECULAR CLOUD; ANALYTIC FITS; DUSTY MEDIUM; SPECTROSCOPY; SWIFT AB We model the time-variable absorption of Fe II, Fe III, Si II, C II and Cr II detected in Ultraviolet and Visual Echelle Spectrograph (UVES) spectra of gamma-ray burst (GRB) 080310, with the afterglow radiation exciting and ionizing the interstellar medium in the host galaxy at a redshift of z = 2.42743. To estimate the rest-frame afterglow brightness as a function of time, we use a combination of the optical VRI photometry obtained by the RAPTOR-T telescope array, which is presented in this paper, and Swift's X-Ray Telescope (XRT) observations. Excitation alone, which has been successfully applied for a handful of other GRBs, fails to describe the observed column density evolution in the case of GRB080310. Inclusion of ionization is required to explain the column density decrease of all observed Fe II levels (including the ground state D-6(9/2)) and increase of the Fe III S-7(3) level. The large population of ions in this latter level (up to 10% of all Fe III) can only be explained through ionization of Fe II, as a large fraction of the ionized Fe II ions (we calculate 31% using the Flexible Atomic and Cowan codes) initially populate the S-7(3) level of Fe III rather than the ground state. This channel for producing a significant Fe III S-7(3) level population may be relevant for other objects in which absorption lines from this level, the UV34 triplet, are observed, such as broad absorption line (BAL) quasars and eta Carinae. This provides conclusive evidence for time-variable ionization in the circumburst medium, which to date has not been convincingly detected. However, the best-fit distance of the neutral absorbing cloud to the GRB is 200-400 pc, i.e. similar to GRB-absorber distance estimates for GRBs without any evidence for ionization. We find that the presence of time-varying ionization in GRB080310 is likely due to a combination of the super-solar iron abundance ([Fe/H] = +0.2) and the low H I column density (log N(H I) = 18.7) in the host of GRB080310. Finally, the modelling provides indications for the presence of an additional cloud at 10-50 pc from the GRB with log N(H I) similar to 19-20 before the burst, which became fully ionized by the radiation released during the first few tens of minutes after the GRB. C1 [Vreeswijk, P. M.; De Cia, A.; Jakobsson, P.] Univ Iceland, Inst Sci, Ctr Astrophys & Cosmol, IS-107 Reykjavik, Iceland. [Vreeswijk, P. M.] Univ Copenhagen, Niels Bohr Inst, Dark Cosmol Ctr, DK-2100 Copenhagen, Denmark. [Ledoux, C.; Smette, A.; Fox, A. J.] European So Observ, Santiago 19, Chile. [Raassen, A. J. J.] Univ Amsterdam, Astron Inst Anton Pannekoek, NL-1098 XH Amsterdam, Netherlands. [Raassen, A. J. J.] SRON Netherlands Inst Space Res, NL-3584 CA Utrecht, Netherlands. [Wozniak, P. R.; Vestrand, W. T.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Fox, A. J.] Univ Cambridge, Inst Astron, Cambridge CB3 0HA, England. [Fox, A. J.] Space Telescope Sci Inst, Baltimore, MD 21218 USA. RP Vreeswijk, PM (reprint author), Univ Iceland, Inst Sci, Ctr Astrophys & Cosmol, Dunhagi 5, IS-107 Reykjavik, Iceland. EM pmvreeswijk@gmail.com RI Jakobsson, Pall/L-9950-2015; OI Jakobsson, Pall/0000-0002-9404-5650; Wozniak, Przemyslaw/0000-0002-9919-3310 FU ESO Scientific Visitor programme in Santiago, Chile; Laboratory Directed Research and Development programme at LANL; ESO DGDF; University of Iceland Research Fund; Icelandic Research Fund; Danish National Research Foundation FX P.M.V. is grateful for the support from the ESO Scientific Visitor programme in Santiago, Chile. P. R. W. and W. T. V. acknowledge support for the RAPTOR and Thinking Telescopes projects from the Laboratory Directed Research and Development programme at LANL. A. D. C. acknowledges support from the ESO DGDF 2009, 2010 and the University of Iceland Research Fund. P.J. acknowledges support by a Project Grant from the Icelandic Research Fund. The Dark Cosmology Centre is funded by the Danish National Research Foundation. The modelling performed in this paper was mostly performed on the excellent computing facilities provided by the Danish Centre for Scientific Computing (DCSC). We kindly thank Peter Laursen for the insightful discussions on Ly alpha scattering and Gudlaugur Johannesson for use of his 24-core work station when the DCSC servers were down. Last but not least, we are grateful for the professional assistance of the VLT staff astronomers, in particular Claudio Melo and Dominique Naef, who secured the UVES observations on which this paper is based. NR 66 TC 11 Z9 11 U1 0 U2 1 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 0004-6361 J9 ASTRON ASTROPHYS JI Astron. Astrophys. PD JAN PY 2013 VL 549 AR A22 DI 10.1051/0004-6361/201219652 PG 13 WC Astronomy & Astrophysics SC Astronomy & Astrophysics GA 073LR UT WOS:000313745000022 ER PT J AU Liu, Y Li, ZT AF Liu, Yi Li, Zhan-Ting TI A Dynamic Route to Structure and Function: Recent Advances in Imine-Based Organic Nanostructured Materials SO AUSTRALIAN JOURNAL OF CHEMISTRY LA English DT Review ID TEMPLATE-DIRECTED SYNTHESIS; COMBINATORIAL CHEMISTRY; COVALENT SYNTHESIS; ONE-POT; CAGES; SELECTIVITY; CAPSULES; CO2; MACROCYCLES; FRAMEWORKS AB The chemistry of imine bond formation from simple aldehyde and amine precursors is among the most powerful dynamic covalent chemistries employed for the construction of discrete molecular objects and extended molecular frameworks. The reversible nature of the C=N bond confers error-checking and proof-reading capabilities in the self-assembly process within a multi-component reaction system. This review highlights recent progress in the self-assembly of complex organic molecular architectures that are enabled by dynamic imine chemistry, including molecular containers with defined geometry and size, mechanically interlocked molecules, and extended frameworks and polymers, from building blocks with preprogrammed steric and electronic information. The functional aspects associated with the nanometer-scale features not only place these dynamically constructed nanostructures at the frontier of materials sciences, but also bring unprecedented opportunities for the discovery of new functional materials. C1 [Liu, Yi] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA. [Li, Zhan-Ting] Fudan Univ, Dept Chem, Shanghai 200433, Peoples R China. RP Liu, Y (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA. EM yliu@lbl.gov; ztli@fudan.edu.cn RI Liu, yi/A-3384-2008; Foundry, Molecular/G-9968-2014 OI Liu, yi/0000-0002-3954-6102; FU Office of Science, Office of Basic Energy Sciences, Scientific User Facilities Division, of the USA Department of Energy [DE-AC02-05CH11231] FX This work was conducted at the Molecular Foundry, Lawrence Berkeley National Laboratory, supported by the Office of Science, Office of Basic Energy Sciences, Scientific User Facilities Division, of the USA Department of Energy under Contract No. DE-AC02-05CH11231. The authors thank Mr. David Hanifi, Mr. Andrew Pun, and Ms. Gayane Koshkakaryan for their help with the manuscript preparation. NR 67 TC 13 Z9 13 U1 1 U2 106 PU CSIRO PUBLISHING PI CLAYTON PA UNIPARK, BLDG 1, LEVEL 1, 195 WELLINGTON RD, LOCKED BAG 10, CLAYTON, VIC 3168, AUSTRALIA SN 0004-9425 EI 1445-0038 J9 AUST J CHEM JI Aust. J. Chem. PY 2013 VL 66 IS 1 BP 9 EP 22 DI 10.1071/CH12349 PG 14 WC Chemistry, Multidisciplinary SC Chemistry GA 073OS UT WOS:000313753000003 ER PT B AU Fried, DB Moris, S Xu, Q Ding, SY Baker, JO Bomble, YJ Himmel, ME Bayer, EA AF Fried, Daniel B. Moris, Sarah Xu, Qi Ding, Shi-You Baker, John O. Bomble, Yannick J. Himmel, Michael E. Bayer, Edward A. BE Rehm, BHA TI Self-assembly and Application of Cellulosomal Components SO BIONANOTECHNOLOGY: BIOLOGICAL SELF-ASSEMBLY AND ITS APPLICATIONS LA English DT Article; Book Chapter ID CARBOHYDRATE-BINDING MODULES; COHESIN-DOCKERIN INTERACTION; X-RAY ANALYSIS; CLOSTRIDIUM-THERMOCELLUM; CRYSTAL-STRUCTURE; CELL-SURFACE; BACILLUS-SUBTILIS; RUMINOCOCCUS-FLAVEFACIENS; SACCHAROMYCES-CEREVISIAE; SCAFFOLDING PROTEIN AB Cellulosomes are modular, super-molecular enzyme systems secreted by anaerobic bacteria to degrade recalcitrant plant cell wall polysaccharides to simple sugars. The components of this molecular machine include a manifold of enzymatic units and carbohydrate-binding modules, as well as the cohesin and dockerin modules responsible for the system's unique self-assembly and connectivity Known to be one of the highest affinity protein protein interactions discovered to date, the cohesin dockerin interaction is also the key to engineering the cellulosome. By mixing and matching the spare parts of the cellulosome and connecting them via cohesins and dockerins, biotechnologists have begun pursuing the concept of 'designer cellulosomes', which one day may be an important contributor to production of sustainable biomass-derived fuels. By incorporating molecules from other systems into the cellulosome paradigm, nanotechnologists have begun to harness the potential of this molecular construction kit to create diverse, self-assembling nanostructures for a broad variety of biotechnological applications. C1 [Fried, Daniel B.; Moris, Sarah; Bayer, Edward A.] Weizmann Inst Sci, Dept Biol Chem, IL-76100 Rehovot, Israel. [Xu, Qi; Ding, Shi-You; Baker, John O.; Bomble, Yannick J.; Himmel, Michael E.] Natl Renewable Energy Lab, Biosci Ctr, Golden, CO USA. RP Fried, DB (reprint author), Weizmann Inst Sci, Dept Biol Chem, IL-76100 Rehovot, Israel. EM daniel.fried@weizmann.ac.il; sarahv@weizmann.ac.il; qi.xu@nrel.gov; shi.you.ding@nrel.gov; john.baker@nrel.gov; yannick.bomble@nrel.gov; mike.himmel@nrel.gov; ed.bayer@weizmann.ac.il NR 102 TC 0 Z9 0 U1 0 U2 15 PU CAISTER ACADEMIC PRESS PI WYMONDHAM PA 32 HEWITTS LANE, WYMONDHAM NR 18 0JA, ENGLAND BN 978-1-908230-16-4 PY 2013 BP 37 EP 61 PG 25 WC Biotechnology & Applied Microbiology; Nanoscience & Nanotechnology SC Biotechnology & Applied Microbiology; Science & Technology - Other Topics GA BDH83 UT WOS:000313301400002 ER PT J AU Wang, XS Liu, J Bonefont, JM Yuan, DQ Thallapally, PK Ma, SQ AF Wang, Xi-Sen Liu, Jian Bonefont, Jean M. Yuan, Da-Qiang Thallapally, Praveen K. Ma, Shengqian TI A porous covalent porphyrin framework with exceptional uptake capacity of saturated hydrocarbons for oil spill cleanup SO CHEMICAL COMMUNICATIONS LA English DT Article ID METAL-ORGANIC FRAMEWORKS; POLYMERS; ADSORPTION; STORAGE; WATER AB A highly porous porphyrin-based organic polymer, PCPF-1, was constructed via homo-coupling reaction of the custom-designed porphyrin ligand, 5,10,15,20-tetrakis(4-bromophenyl)porphyrin. PCPF-1 possesses a large BET surface area of over 1300 m(2) g(-1) (Langmuir surface area of over 2400 m(2) g(-1)) and exhibits strong hydrophobicity with a water contact angle of 135 degrees, and these features afford it the highest adsorptive capacities for saturated hydrocarbons and gasoline among sorbent materials reported thus far, as well as render it the capability to remove oil from water. C1 [Wang, Xi-Sen; Bonefont, Jean M.; Ma, Shengqian] Univ S Florida, Dept Chem, Tampa, FL 33620 USA. [Liu, Jian; Thallapally, Praveen K.] Pacific NW Natl Lab, Energy & Environm Directorate, Richland, WA 99352 USA. [Yuan, Da-Qiang] Chinese Acad Sci, Fujian Inst Res Struct Matter, State Key Lab Struct Chem, Fuzhou 350002, Fujian, Peoples R China. RP Ma, SQ (reprint author), Univ S Florida, Dept Chem, 4202 E Fowler Ave, Tampa, FL 33620 USA. EM sqma@usf.edu RI Ma, Shengqian/B-4022-2012; wang, Xi-Sen/B-1102-2011; thallapally, praveen/I-5026-2014; Liu, Jian/C-4707-2011; Liu, Jian/D-3393-2009; Yuan, Daqiang/F-5695-2010 OI Ma, Shengqian/0000-0002-1897-7069; thallapally, praveen/0000-0001-7814-4467; Liu, Jian/0000-0001-5329-7408; Liu, Jian/0000-0001-5329-7408; Yuan, Daqiang/0000-0003-4627-072X FU University of South Florida; US Department of Energy [DE-AR0000177]; US-DOE-EERE through the Geothermal Technologies Program FX S. Ma acknowledges the University of South Florida for financial support of this work. This work was also supported, in part, by US Department of Energy (contract DE-AR0000177). P. K. T. and J. L. would like to acknowledge the support from US-DOE-EERE through the Geothermal Technologies Program. NR 26 TC 59 Z9 61 U1 18 U2 195 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1359-7345 J9 CHEM COMMUN JI Chem. Commun. PY 2013 VL 49 IS 15 BP 1533 EP 1535 DI 10.1039/c2cc38067f PG 3 WC Chemistry, Multidisciplinary SC Chemistry GA 076PE UT WOS:000313968300017 PM 23321927 ER PT J AU Assary, RS Lu, J Du, P Luo, XY Zhang, XY Ren, Y Curtiss, LA Amine, K AF Assary, Rajeev S. Lu, Jun Du, Peng Luo, Xiangyi Zhang, Xiaoyi Ren, Yang Curtiss, Larry A. Amine, Khalil TI The Effect of Oxygen Crossover on the Anode of a Li-O2 Battery using an Ether-Based Solvent: Insights from Experimental and Computational Studies SO CHEMSUSCHEM LA English DT Article DE batteries; electrochemistry; lithium; membranes; oxygen ID LITHIUM-AIR BATTERIES; CARBONATE ELECTROLYTES; ENERGY-STORAGE; ION BATTERIES; PERFORMANCE; REDUCTION; PERSPECTIVE; CHALLENGES; COMPOSITE C1 [Assary, Rajeev S.; Curtiss, Larry A.] Argonne Natl Lab, Div Mat Sci, Argonne, IL 60439 USA. [Lu, Jun; Du, Peng; Luo, Xiangyi; Amine, Khalil] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. [Zhang, Xiaoyi; Ren, Yang] Argonne Natl Lab, Xray Sci Div, Argonne, IL 60435 USA. [Luo, Xiangyi] Univ Utah, Dept Met Engn, Salt Lake City, UT 84112 USA. RP Assary, RS (reprint author), Argonne Natl Lab, Div Mat Sci, 9700 S Cass Ave, Argonne, IL 60439 USA. EM curtiss@anl.gov; amine@anl.gov RI Du, Peng/F-8336-2013; Amine, Khalil/K-9344-2013; Luo, Xiangyi/N-4709-2014; Luo, Xiangyi/K-6058-2015; Surendran Assary, Rajeev/E-6833-2012 OI Luo, Xiangyi/0000-0002-4817-1461; Luo, Xiangyi/0000-0002-4817-1461; Surendran Assary, Rajeev/0000-0002-9571-3307 FU U.S. Department of Energy [DE-AC0206CH11357]; Tailored Interfaces for Energy Storage, an Energy Frontier Research Center; U.S. Department of Energy, Office of Science, and Office of Basic Energy Sciences; Department of Energy (DOE) Office of Energy Efficiency and Renewable Energy (EERE) Postdoctoral Research Award under the EERE Vehicles Technology Program; DOE [DE-AC05-06OR23100]; U.S. Department of Energy Office of Science [DE-AC02-06CH11357] FX This work was supported by the U.S. Department of Energy under Contract DE-AC0206CH11357. This material is based upon work supported as part of the Tailored Interfaces for Energy Storage, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, and Office of Basic Energy Sciences. J. Lu was supported by the Department of Energy (DOE) Office of Energy Efficiency and Renewable Energy (EERE) Postdoctoral Research Award under the EERE Vehicles Technology Program administered by the Oak Ridge Institute for Science and Education (ORISE) for the DOE. ORISE is managed by Oak Ridge Associated Universities (ORAU) under DOE contract number DE-AC05-06OR23100. Use of the Advanced Photon Source at Argonne National Laboratory was supported by the U.S. Department of Energy Office of Science under Contract No. DE-AC02-06CH11357. Also, we acknowledge grants of computer time from EMSL, a national scientific user facility locates at the Pacific Northwest National Laboratory, the ANL Laboratory Computing Resource Center, and the ANL Center for Nanoscale Materials. NR 39 TC 82 Z9 82 U1 18 U2 185 PU WILEY-V C H VERLAG GMBH PI WEINHEIM PA BOSCHSTRASSE 12, D-69469 WEINHEIM, GERMANY SN 1864-5631 J9 CHEMSUSCHEM JI ChemSusChem PD JAN PY 2013 VL 6 IS 1 BP 51 EP 55 DI 10.1002/cssc.201200810 PG 5 WC Chemistry, Multidisciplinary; GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY SC Chemistry; Science & Technology - Other Topics GA 072VT UT WOS:000313702200007 PM 23208891 ER PT J AU Roy, LE Bridges, NJ Martin, LR AF Roy, Lindsay E. Bridges, Nicholas J. Martin, Leigh R. TI Theoretical insights into covalency driven f element separations SO DALTON TRANSACTIONS LA English DT Article ID TRIVALENT ACTINIDES; SOFT ACIDS; OPTICAL SPECTROSCOPY; ELECTRON-DENSITY; BASES HSAB; BASIS-SETS; COMPLEXES; LANTHANIDES; HARD; EXTRACTION AB Through Density Function Theory (DFT) calculations, we set out to understand the structures and stabilities of the aqueous phase complexes [M-III(DTPA)-H2O](2-) (M = Nd, Am) as well as the changes in Gibbs free energy for complexation in the gas phase and aqueous solution. All bonding analyses suggest that the preference of the DTPA(5-) ligand for Am over Nd is mainly due to electrostatic and covalent interactions from the oxygen atoms with the nitrogen chelates providing an additional, yet small, covalent interaction. These results question the exclusive use of hard and soft acids and bases (HSAB) concepts for the design of extracting reagents and suggest that hard-soft interactions may play more of a role in the separations process than previously thought. C1 [Roy, Lindsay E.] Savannah River Natl Lab, Sci & Technol Directorate, Aiken, SC 29808 USA. [Bridges, Nicholas J.] Savannah River Natl Lab, Environm Management Directorate, Aiken, SC 29808 USA. [Martin, Leigh R.] Idaho Natl Lab, Aqueous Separat & Radiochem Dept, Idaho Falls, ID 83415 USA. RP Roy, LE (reprint author), Savannah River Natl Lab, Sci & Technol Directorate, POB A, Aiken, SC 29808 USA. EM Lindsay.roy@srnl.doe.gov; Leigh.Martin@inl.gov RI Martin, Leigh/P-3167-2016 OI Martin, Leigh/0000-0001-7241-7110 FU Department of Energy/Nuclear Energy Fuel Cycle R&D Thermodynamics and Kinetics program; U.S. Department of Energy [DE-AC09-8SR22470, DE-AC07-05ID14517] FX We would like to thank Dr Enrique R. Batista (Los Alamos National Laboratory) for the Orbpop utility program. This work was supported by the Department of Energy/Nuclear Energy Fuel Cycle R&D Thermodynamics and Kinetics program. Savannah River National Laboratory is operated by Savannah River Nuclear Solutions, LLC, for the U.S. Department of Energy under Contract No. DE-AC09-8SR22470. Idaho National Laboratory is operated by Battelle Energy Alliance, for the U.S. Department of Energy under Contract No. DE-AC07-05ID14517. The United States Government retains and the publisher, by accepting this article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this work, or allow others to do so, for United States Government purposes. NR 40 TC 15 Z9 15 U1 3 U2 31 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1477-9226 J9 DALTON T JI Dalton Trans. PY 2013 VL 42 IS 7 BP 2636 EP 2642 DI 10.1039/c2dt31485a PG 7 WC Chemistry, Inorganic & Nuclear SC Chemistry GA 074HT UT WOS:000313804200040 PM 23223573 ER PT J AU Jeffers, RF Jacobson, JJ Searcy, EM AF Jeffers, Robert F. Jacobson, Jacob J. Searcy, Erin M. TI Dynamic analysis of policy drivers for bioenergy commodity markets SO ENERGY POLICY LA English DT Article DE Bioenergy markets; Modeling and simulation; Energy economics AB Biomass is increasingly being considered as a feedstock to provide a clean and renewable source of energy in the form of both liquid fuels and electric power. In the United States, the biofuels and biopower industries are regulated by different policies and have different drivers, which impact the maximum price the industries are willing to pay for biomass. This article describes a dynamic computer simulation model that analyzes future behavior of bioenergy feedstock markets given policy and technical options. The model simulates the long-term dynamics of these markets by treating advanced biomass feedstocks as a commodity and projecting the total demand of each industry, as well as the market price over time. The model is used for an analysis of the United States bioenergy feedstock market that projects supply, demand, and market price given three independent buyers: domestic biopower, domestic biofuels, and foreign exports. With base-case assumptions, the biofuels industry is able to dominate the market and meet the federal Renewable Fuel Standard (RFS) targets for advanced biofuels. Further analyses suggest that United States bioenergy studies should include estimates of export demand in their projections, and that GHG-limiting policy would partially shield both industries from export dominance. (C) 2012 Elsevier Ltd. All rights reserved. C1 [Jeffers, Robert F.; Jacobson, Jacob J.; Searcy, Erin M.] Idaho Natl Lab, Idaho Falls, ID 83415 USA. RP Jeffers, RF (reprint author), Idaho Natl Lab, Post POB 1625,2525 N Fremont Ave,MS 3710, Idaho Falls, ID 83415 USA. EM Robert.Jeffers@inl.gov; Jacob.Jacobson@inl.gov; Erin.Searcy@inl.gov FU US Government under DOE [DE-AC07-05ID14517] FX This submitted manuscript was authored by a contractor of the US Government under DOE Contract No. DE-AC07-05ID14517. Accordingly, the US Government retains and the publisher, by accepting the article for publication, acknowledges that the US Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US Government purposes. NR 33 TC 10 Z9 11 U1 0 U2 31 PU ELSEVIER SCI LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, OXON, ENGLAND SN 0301-4215 J9 ENERG POLICY JI Energy Policy PD JAN PY 2013 VL 52 BP 249 EP 263 DI 10.1016/j.enpol.2012.08.072 PG 15 WC Energy & Fuels; Environmental Sciences; Environmental Studies SC Energy & Fuels; Environmental Sciences & Ecology GA 073WZ UT WOS:000313775100022 ER PT J AU Desroches, LB Garbesi, K Kantner, C Van Buskirk, R Yang, HC AF Desroches, Louis-Benoit Garbesi, Karina Kantner, Colleen Van Buskirk, Robert Yang, Hung-Chia TI Incorporating experience curves in appliance standards analysis SO ENERGY POLICY LA English DT Article DE Efficiency standards; Experience curves; Large appliances ID STUDYING TECHNOLOGICAL-PROGRESS; ENERGY TECHNOLOGIES; LEARNING-CURVES; FUNCTIONAL-APPROACH; UNBALANCED GROWTH; RELIABILITY; DIFFUSION; PROSPECTS; RATES; POWER AB There exists considerable evidence that manufacturing costs and consumer prices of residential appliances have decreased in real terms over the last several decades. This phenomenon is generally attributable to manufacturing efficiency gained with cumulative experience producing a certain good, and is modeled by an empirical experience curve. The technical analyses conducted in support of U.S. energy conservation standards for residential appliances and commercial equipment have, until recently, assumed that manufacturing costs and retail prices remain constant during the projected 30-year analysis period. This assumption does not reflect real market price dynamics. Using price data from the Bureau of Labor Statistics, we present U.S. experience curves for room air conditioners, clothes dryers, central air conditioners, furnaces, and refrigerators and freezers. These experience curves were incorporated into recent energy conservation standards analyses for these products. Including experience curves increases the national consumer net present value of potential standard levels. In some cases a potential standard level exhibits a net benefit when considering experience, whereas without experience it exhibits a net cost. These results highlight the importance of modeling more representative market prices. (C) 2012 Elsevier Ltd. All rights reserved. C1 [Desroches, Louis-Benoit; Garbesi, Karina; Kantner, Colleen; Van Buskirk, Robert; Yang, Hung-Chia] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. RP Desroches, LB (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, 1 Cyclotron Rd, Berkeley, CA 94720 USA. EM ldesroches@lbl.gob FU U.S. Department of Energy's Office of Energy Efficiency and Renewable Energy, Building Technologies Program [DE-AC02-05CH11231] FX We wish to thank Katie Coughlin, Larry Dale, Jeffery Greenblatt, and two anonymous reviewers for helpful comments. We also thank Arpi Kupelian, who assisted us on a previous iteration of this work. The Energy Efficiency Standards group at Lawrence Berkeley National Laboratory is supported by the U.S. Department of Energy's Office of Energy Efficiency and Renewable Energy, Building Technologies Program under Contract no. DE-AC02-05CH11231. NR 56 TC 5 Z9 5 U1 0 U2 13 PU ELSEVIER SCI LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, OXON, ENGLAND SN 0301-4215 J9 ENERG POLICY JI Energy Policy PD JAN PY 2013 VL 52 BP 402 EP 416 DI 10.1016/j.enpol.2012.09.066 PG 15 WC Energy & Fuels; Environmental Sciences; Environmental Studies SC Energy & Fuels; Environmental Sciences & Ecology GA 073WZ UT WOS:000313775100034 ER PT J AU Xu, P Xu, TF Shen, PY AF Xu, Peng Xu, Tengfang Shen, Pengyuan TI Energy and behavioral impacts of integrative retrofits for residential buildings: What is at stake for building energy policy reforms in northern China? SO ENERGY POLICY LA English DT Article DE Integrative retrofits; Residential building energy; Policy reform ID DISTRICT-HEATING SYSTEM; EFFICIENCY RETROFIT; PERFORMANCE; ZONES; AREAS AB Based upon the results from extensive building monitoring and surveys on occupant's behaviors in a representative nine-story apartment building in northern China, building energy simulations were performed to evaluate the impacts of integrative retrofits implemented. Integrative retrofits required by the newer building energy standard produced significant heating-energy savings (i.e., 53%) when compared with baseline buildings commonly built in early 1980s. Taking into account district-heating-system upgrades as part of integrative retrofit measures, a representative apartment building was 66% more efficient than the baseline building. Contrary to expectation, little behavioral change was found in response to the provisions of monetary incentive, billing-method reform, or metering of heating energy use in individual apartment units. Yet this paper identified sizable energy savings potential if occupants' behavioral changes were to actually happen. This indicates that provisions of financial incentives or individual metering were insufficient for triggering substantial behavioral changes leading toward more energy savings in the current buildings. It is recommended that innovative energy policies, technology upgrades, and education would be needed to promote behavioral changes toward additional energy savings. Finally, measures and strategies to further enhance thermal integrity criteria (e.g., insulations of roof and balcony) are recommended in China's future building energy policy reforms. (C) 2012 Elsevier Ltd. All rights reserved. C1 [Xu, Peng; Shen, Pengyuan] Tongji Univ, Coll Mech Engn, Shanghai 200092, Peoples R China. [Xu, Tengfang] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Xu, TF (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, 1 Cyclotron Rd,MS 90R2000, Berkeley, CA 94720 USA. EM TTXU@LBL.gov NR 13 TC 8 Z9 9 U1 3 U2 33 PU ELSEVIER SCI LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, OXON, ENGLAND SN 0301-4215 J9 ENERG POLICY JI Energy Policy PD JAN PY 2013 VL 52 BP 667 EP 676 DI 10.1016/j.enpol.2012.10.029 PG 10 WC Energy & Fuels; Environmental Sciences; Environmental Studies SC Energy & Fuels; Environmental Sciences & Ecology GA 073WZ UT WOS:000313775100058 ER PT J AU Ni, CC AF Ni, Chun Chun TI Potential energy savings and reduction of CO2 emissions through higher efficiency standards for polyphase electric motors in Japan SO ENERGY POLICY LA English DT Article DE Polyphase electric motors; Energy efficiency; Japan AB Japan has shut down more than 70% of its nuclear power plants since the March 2011 Tohoku earthquake and the ensuing accident at the Fukushima Daiichi nuclear power plant. The country has been challenged with power shortages in the short-term and faces complex energy security decisions in the long-term. Japan has a long history of implementing energy conservation policies, such as the Top Runner Program, which covers 23 products including appliances and industrial equipment. However, Japan's efficiency policy for polyphase electric motors is considered below international standards. Polyphase electric motors accounted for about 55% of the nation's total power consumption in 2008. The aim of this study is to estimate potential energy savings and reduction in CO2 emissions (2014-2043) by examining scenarios involving adopting two different polyphase motor efficiency standards and comparing them to a base case and concludes by suggesting pathways for further policy development using the results obtained. The study finds that if level IE2 of the international efficiency standard IEC 60034-30 were implemented, it would save 8.3 TWh (or 0.03 quads) per year, which is equivalent to about 0.8% of Japan's total electric power consumption in 2010. If level IE3 of the IEC 60034-30 were implemented instead, it would save about 13.3 TWh (or 0.05 quads) per year. The corresponding cumulative energy savings and reduction in CO2 emissions for the IE2 scenario would be 249 TWh (or 0.85 quads) and 93 Mt. The corresponding cumulative energy savings and reduction in CO2 emissions for the IE3 scenario would be 398 TWh (or 1.36 quads) and 149 Mt. (C) 2012 Elsevier Ltd. All rights reserved. C1 Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. RP Ni, CC (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, 1 Cyclotron Rd,MS 90R4000, Berkeley, CA 94720 USA. EM CNi@lbl.gov NR 15 TC 3 Z9 3 U1 0 U2 24 PU ELSEVIER SCI LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, OXON, ENGLAND SN 0301-4215 J9 ENERG POLICY JI Energy Policy PD JAN PY 2013 VL 52 BP 737 EP 747 DI 10.1016/j.enpol.2012.10.035 PG 11 WC Energy & Fuels; Environmental Sciences; Environmental Studies SC Energy & Fuels; Environmental Sciences & Ecology GA 073WZ UT WOS:000313775100065 ER PT J AU Schmid, TE Grant, PG Marchetti, F Weldon, RH Eskenazi, B Wyrobek, AJ AF Schmid, Thomas E. Grant, Patrick G. Marchetti, Francesco Weldon, Rosana H. Eskenazi, Brenda Wyrobek, Andrew J. TI Elemental composition of human semen is associated with motility and genomic sperm defects among older men SO HUMAN REPRODUCTION LA English DT Article DE male aging; calcium; copper; semen; zinc ID MALE FACTOR SUBFERTILITY; PATERNAL-AGE; DNA-DAMAGE; OCCUPATIONAL EXPOSURES; CHROMATIN INTEGRITY; ANTIOXIDANT INTAKE; HUMAN-SPERMATOZOA; SEMINAL PLASMA; ADVANCING AGE; HEALTHY-MEN AB BACKGROUND: Older men tend to have poorer semen quality and are generally at higher risks for infertility and abnormal reproductive outcomes. METHODS: We employed proton-induced X-ray emission (PIXE, 3 MeV proton beam) to investigate the concentrations of zinc, copper, calcium, sulfur, chlorine, potassium, titanium, iron and nickel in washed sperm and seminal plasma from non-smoking groups of 10 older men (65-80 years old) and 10 younger men (22-28 years old) who were concurrently assayed for sperm function and genomicly defective sperm. RESULTS: The older group showed elevated zinc, copper and calcium in sperm and elevated sulfur in seminal plasma compared with the younger men. The older group also showed reduced motility as well as increased sperm DNA fragmentation, achondroplasia mutations, DNA strand breaks and chromosomal aberrations. Sperm calcium and copper were positively associated with sperm DNA fragmentation (P < 0.03). Seminal sulfur was positively associated with sperm DNA fragmentation and chromosomal aberrations (P < 0.04), and negatively associated with sperm motility (P < 0.05). Sperm calcium was negatively associated with sperm motility, independent of male age (P = 0.01). CONCLUSIONS: We identified major differences in elemental concentrations between sperm and seminal plasma and that higher sperm copper, sulfur and calcium are quantitatively associated with poorer semen quality and increased frequencies of genomic sperm defects. C1 [Schmid, Thomas E.; Marchetti, Francesco; Wyrobek, Andrew J.] Lawrence Livermore Natl Lab, Biosci Directorate, Livermore, CA 94550 USA. [Schmid, Thomas E.; Marchetti, Francesco; Wyrobek, Andrew J.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Life Sci Div, Berkeley, CA 94720 USA. [Schmid, Thomas E.; Weldon, Rosana H.; Eskenazi, Brenda] Univ Calif Berkeley, Sch Publ Hlth, CERCH, Berkeley, CA 94704 USA. [Grant, Patrick G.] Lawrence Livermore Natl Lab, Ctr Accelerator Mass Spectrometry, Livermore, CA 94550 USA. RP Wyrobek, AJ (reprint author), Lawrence Livermore Natl Lab, Biosci Directorate, Livermore, CA 94550 USA. EM ajwyrobek@lbl.gov OI Marchetti, Francesco/0000-0002-9435-4867 FU U.S. Department of Energy by LLNL [W-7405-ENG-48]; National Institute of Environmental Health Sciences [P42 ES04705]; Jennifer and Brian Maxwell Chair; LBNL [DE-AC02-05CH11231] FX The work was performed under the auspices of the U.S. Department of Energy by LLNL, contract W-7405-ENG-48, with funding support from Superfund P42 ES04705 from the National Institute of Environmental Health Sciences (Eskenazi and Wyrobek, study directors) and the Jennifer and Brian Maxwell Chair. This work was completed at LBNL contract DE-AC02-05CH11231. NR 51 TC 9 Z9 12 U1 0 U2 18 PU OXFORD UNIV PRESS PI OXFORD PA GREAT CLARENDON ST, OXFORD OX2 6DP, ENGLAND SN 0268-1161 J9 HUM REPROD JI Hum. Reprod. PD JAN PY 2013 VL 28 IS 1 BP 274 EP 282 DI 10.1093/humrep/des321 PG 9 WC Obstetrics & Gynecology; Reproductive Biology SC Obstetrics & Gynecology; Reproductive Biology GA 074SS UT WOS:000313834400030 PM 23042799 ER PT J AU Muljadi, E Samaan, N Gevorgian, V Li, J Pasupulati, S AF Muljadi, Eduard Samaan, Nader Gevorgian, Vahan Li, Jun Pasupulati, Subbaiah TI Different Factors Affecting Short Circuit Behavior of a Wind Power Plant SO IEEE TRANSACTIONS ON INDUSTRY APPLICATIONS LA English DT Article; Proceedings Paper CT Annual Meeting of the IEEE Industry-Applications-Society CY OCT 03-07, 2010 CL Houston, TX SP IEEE Ind Applicat Soc, IEEE DE Fault contribution; induction generator; protection; short circuit (SC); wind power plant (WPP); wind turbine AB A wind power plant (WPP) consists of a large number of turbines interconnected by underground cable. A pad-mounted transformer at each turbine steps up the voltage from a generating voltage (690 V) to a medium voltage (34.5 kV). All turbines in the plant are connected to the substation transformer, where the voltage is stepped up to the transmission level. An important aspect of WPP impact studies is to evaluate the short-circuit (SC) current contribution of the plant into the transmission network under different fault conditions. This task can be challenging to protection engineers due to the topology differences between different types of wind turbine generators and the conventional generating units. This paper investigates the SC behavior of a WPP for different types of faults. The impact of wind turbine types, the transformer configuration, and the reactive compensation capacitor will be investigated. The voltage response at different buses will be observed. Finally, the SC line currents will be presented along with its symmetrical components. C1 [Muljadi, Eduard; Gevorgian, Vahan] Natl Renewable Energy Lab, Golden, CO 80401 USA. [Samaan, Nader] Pacific NW Natl Lab, Richland, WA 99352 USA. [Li, Jun] EnerNex Corp, Knoxville, TN 37922 USA. [Pasupulati, Subbaiah] Oak Creek Energy Syst Inc, Mojave, CA 93501 USA. RP Muljadi, E (reprint author), Natl Renewable Energy Lab, Golden, CO 80401 USA. EM eduard.muljadi@nrel.gov; nader.samaan@pnnl.gov; vahan.gevorgian@nrel.gov; jun@enernex.com; venkata.viz@gmail.com OI Samaan, Nader/0000-0001-9478-3007 NR 12 TC 13 Z9 13 U1 0 U2 1 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 0093-9994 J9 IEEE T IND APPL JI IEEE Trans. Ind. Appl. PD JAN-FEB PY 2013 VL 49 IS 1 BP 284 EP 292 DI 10.1109/TIA.2012.2228831 PG 9 WC Engineering, Multidisciplinary; Engineering, Electrical & Electronic SC Engineering GA 073ES UT WOS:000313726900031 ER PT J AU Sen, S AF Sen, Satyabrata TI OFDM Radar Space-Time Adaptive Processing by Exploiting Spatio-Temporal Sparsity SO IEEE TRANSACTIONS ON SIGNAL PROCESSING LA English DT Article DE Adaptive waveform design; generalized eigenvalue-eigenvector; OFDM radar; residual sparse-recovery; space-time adaptive processing; spatio-temporal sparsity ID MIMO RADAR; STAP; REPRESENTATION; PERFORMANCE; PROJECTIONS; ARRAYS; FILTER AB We propose a sparsity-based space-time adaptive processing (STAP) algorithm to detect a slowly-moving target using an orthogonal frequency division multiplexing (OFDM) radar. We observe that the target and interference spectra are inherently sparse in the spatio-temporal domain. Hence, we exploit that sparsity to develop an efficient STAP technique that utilizes considerably lesser number of secondary data and produces an equivalent performance as the other existing STAP techniques. In addition, the use of an OFDM signal increases the frequency diversity of our system, as different scattering centers of a target resonate at different frequencies, and thus improves the target detectability. First, we formulate a realistic sparse-measurement model for an OFDM radar considering both the clutter and jammer as the interfering sources. Then, we apply a residual sparse-recovery technique based on the LASSO estimator to estimate the target and interference covariance matrices, and subsequently compute the optimal STAP-filter weights. Our numerical results demonstrate a comparative performance analysis of the proposed sparse-STAP algorithm with four other existing STAP methods. Furthermore, we discover that the OFDM-STAP filter-weights are adaptable to the frequency-variabilities of the target and interference responses, in addition to the spatio-temporal variabilities. Hence, by better utilizing the frequency variabilities, we propose an adaptive OFDM-waveform design technique, and consequently gain a significant amount of STAP-performance improvement. C1 Oak Ridge Natl Lab, Ctr Engn Syst Adv Res, Comp Sci & Math Div, Oak Ridge, TN 37831 USA. RP Sen, S (reprint author), Oak Ridge Natl Lab, Ctr Engn Syst Adv Res, Comp Sci & Math Div, Oak Ridge, TN 37831 USA. EM sens@ornl.gov OI Sen, Satyabrata/0000-0001-9918-4409 FU U.S. Department of Energy [DE-AC05-00OR22725] FX Manuscript received January 20, 2012; revised May 24, 2012; accepted September 18, 2012. Date of publication October 03, 2012; date of current version December 11, 2012. The associate editor coordinating the review of this manuscript and approving it for publication was Prof. Maria Sabrina Greco. This work was performed while the author was a Eugene P. Wigner Fellow and staff member with the Oak Ridge National Laboratory, managed by UT-Battelle, LLC, for the U.S. Department of Energy under Contract DE-AC05-00OR22725. NR 49 TC 20 Z9 26 U1 1 U2 28 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 1053-587X EI 1941-0476 J9 IEEE T SIGNAL PROCES JI IEEE Trans. Signal Process. PD JAN PY 2013 VL 61 IS 1 BP 118 EP 130 DI 10.1109/TSP.2012.2222387 PG 13 WC Engineering, Electrical & Electronic SC Engineering GA 075OJ UT WOS:000313896100014 ER PT J AU Latham, JP Xiang, JS Belayneh, M Nick, HM Tsang, CF Blunt, MJ AF Latham, John-Paul Xiang, Jiansheng Belayneh, Mandefro Nick, Hamidreza M. Tsang, Chin-Fu Blunt, Martin J. TI Modelling stress-dependent permeability in fractured rock including effects of propagating and bending fractures SO INTERNATIONAL JOURNAL OF ROCK MECHANICS AND MINING SCIENCES LA English DT Article DE Hydro-mechanical coupling; Deformation; Fracturing; Fracture-matrix; Fluid flow; Numerical simulation ID FINITE-ELEMENT; NUMERICAL SIMULATIONS; POROUS-MEDIA; 2-PHASE FLOW; FLUID-FLOW; TRANSPORT; APERTURE; RESERVOIRS; SINGLE; LENGTH AB The influence of in-situ stresses on flow processes in fractured rock is investigated using a novel modelling approach. The combined finite-discrete element method (FEMDEM) is used to model the deformation of a fractured rock mass. The fracture wall displacements and aperture changes are modelled in response to uniaxial and biaxial stress states. The resultant changes in flow properties of the rock mass are investigated using the Complex Systems Modelling Platform (CSMP++). CSMP++ is used to model single-phase flow through fractures with variable aperture and a permeable rock matrix. The study is based on a geological outcrop mapping of a low density fracture pattern that includes the realism of intersections, bends and segmented features. By applying far-field (boundary) stresses to a square region, geologically important phenomena are modelled including fracture-dependent stress heterogeneity, the re-activation of pre-existing fractures (i.e. opening, closing and shearing), the propagation of new fractures and the development of fault zones. Flow anisotropy is investigated under various applied stresses and matrix permeabilities. In-situ stress conditions that encourage a closing of fractures together with a more pervasive matrix-dominated flow are identified. These are compared with conditions supporting more localised flow where fractures are prone to dilatational shearing and can be more easily exploited by fluids. The natural fracture geometries modelled in this work are not perfectly straight, promoting fracture segments that dilate as they shear. We have demonstrated the introduction of several realistic processes that have an influence on natural systems: fractures can propagate with wing cracks; there is the potential for new fractures to connect with existing fractures, thus increasing the connectivity and flow; blocks can rotate when bounded by fractures, bent fractures lead to locally different aperture development; highly heterogeneous stress distributions emerge naturally. Results presented in this work provide a mechanically rigorous demonstration that a change in the stress state can cause reactivation of pre-existing fractures and channelling of flow in critically stressed fractures. (c) 2012 Elsevier Ltd. All rights reserved. C1 [Latham, John-Paul; Xiang, Jiansheng; Tsang, Chin-Fu; Blunt, Martin J.] Univ London Imperial Coll Sci Technol & Med, Dept Earth Sci & Engn, London, England. [Belayneh, Mandefro] Senergy Oil & Gas Ltd, London, England. [Nick, Hamidreza M.] Univ Utrecht, Dept Earth Sci, NL-3508 TC Utrecht, Netherlands. [Tsang, Chin-Fu] Lawrence Berkeley Lab, Berkeley, CA USA. RP Latham, JP (reprint author), Univ London Imperial Coll Sci Technol & Med, Dept Earth Sci & Engn, London, England. EM j.p.latham@imperial.ac.uk RI M. Nick, Hamidreza/N-2625-2014; OI M. Nick, Hamidreza/0000-0002-0623-6095; Blunt, Martin/0000-0002-8725-0250; Latham, John-Paul/0000-0002-9410-3945 NR 51 TC 25 Z9 30 U1 1 U2 58 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 1365-1609 EI 1873-4545 J9 INT J ROCK MECH MIN JI Int. J. Rock Mech. Min. Sci. PD JAN PY 2013 VL 57 BP 100 EP 112 DI 10.1016/j.ijrmms.2012.08.002 PG 13 WC Engineering, Geological; Mining & Mineral Processing SC Engineering; Mining & Mineral Processing GA 075LK UT WOS:000313887500010 ER PT J AU Shi, H Gutierrez, OY Haller, GL Mei, DH Rousseau, R Lercher, JA AF Shi, Hui Gutierrez, Oliver Y. Haller, Gary L. Mei, Donghai Rousseau, Roger Lercher, Johannes A. TI Structure sensitivity of hydrogenolytic cleavage of endocyclic and exocyclic C-C bonds in methylcyclohexane over supported iridium particles SO JOURNAL OF CATALYSIS LA English DT Article DE Iridium; Methylcyclohexane; Ring opening; Hydrogenolysis; Demethylation; Structure sensitivity ID RING-OPENING CATALYSTS; ETHANE HYDROGENOLYSIS; (110)-(1X2) SURFACES; ZEOLITE CATALYSTS; MODEL CATALYSTS; METAL-SUPPORT; RH CATALYSTS; METHYLCYCLOPENTANE; DECALIN; SELECTIVITY AB Structure sensitivities, H-2 pressure effects, and temperature dependencies for rates and selectivities of endo- and exocyclic C-C bond cleavage in methylcyclohexane were studied over supported Ir catalysts. The rate of endocyclic C-C bond cleavage first decreased and then increased with declining Ir dispersion from 0.65 to 0.035. The ring opening (RO) product distribution remained unchanged with varying H-2 pressure on small Ir particles, while further shifting to methylhexanes with increasing H-2 pressure on large particles. In contrast, the rate and selectivity of exocyclic C-C bond cleavage decreased monotonically with increasing H-2 pressure and decreasing Ir particle size. The distinct dependencies of endocyclic and exocyclic C-C bond cleavage pathways on Ir dispersion and H-2 pressure suggest that they are mediated by surface species with different ensemble size requirements. DFT calculations were performed on an Ir-50 cluster and an Ir(111) surface, with or without pre-adsorbed hydrogen atoms, to provide insight into the observed effects of particle size and H-2 pressure on RO pathways. On small Ir particles, the calculated dehydrogenation enthalpies for all endocyclic bonds were similar and affected to similar extents by H-2 pressure; on large particles, the selectivity to n-heptane (via substituted C-C bond cleavage) was even lower than on small particles as a result of the least favorable adsorption and dehydrogenation energetics for hindered bonds. (c) 2012 Elsevier Inc. All rights reserved. C1 [Shi, Hui; Gutierrez, Oliver Y.; Haller, Gary L.; Lercher, Johannes A.] Tech Univ Munich, Dept Chem, D-85747 Garching, Germany. [Shi, Hui; Gutierrez, Oliver Y.; Haller, Gary L.; Lercher, Johannes A.] Tech Univ Munich, Catalysis Res Ctr, D-85747 Garching, Germany. [Mei, Donghai; Rousseau, Roger; Lercher, Johannes A.] Pacific NW Natl Lab, Inst Integrated Catalysis, Richland, WA 99352 USA. RP Lercher, JA (reprint author), Tech Univ Munich, Dept Chem, Lichtenbergstr 4, D-85747 Garching, Germany. EM johannes.lercher@ch.tum.de RI Mei, Donghai/A-2115-2012; Rousseau, Roger/C-3703-2014; Shi, Hui/J-7083-2014; Mei, Donghai/D-3251-2011; OI Mei, Donghai/0000-0002-0286-4182; Gutierrez Tinoco, Oliver/0000-0001-9163-4786 FU US Department of Energy (DOE), Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences Biosciences [DE-AC05-76RL01830]; US Department of Energy's Office of Biological and Environmental Research; Elitenetzwerk Bayern NanoCat FX Hui Shi thanks the Elitenetzwerk Bayern NanoCat for a Ph.D. grant and financial support. Prof. Dr. Xuebing Li (Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, China) is gratefully acknowledged for his help in technical aspects. The authors are indebted to Dipl.-Ing. Xaver Hecht for the help with construction of the reactor setup and for conducting N2 physisorption and H2 chemisorption measurements. The theoretical part of this work was supported by the by the US Department of Energy (DOE), Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences & Biosciences under Contract DE-AC05-76RL01830. Pacific Northwest National Laboratory (PNNL) is a multiprogram national laboratory operated for DOE by Battelle. The computing time is provided by the user project from EMSL, a national scientific user facility sponsored by the US Department of Energy's Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory. Part of computing time is also provided by National Energy Research Scientific Computing Center (NERSC) at Berkeley National Laboratory. NR 46 TC 14 Z9 14 U1 2 U2 85 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 0021-9517 J9 J CATAL JI J. Catal. PD JAN PY 2013 VL 297 BP 70 EP 78 DI 10.1016/j.jcat.2012.09.018 PG 9 WC Chemistry, Physical; Engineering, Chemical SC Chemistry; Engineering GA 078YH UT WOS:000314136500008 ER PT J AU Turcu, RVF Hoyt, DW Rosso, KM Sears, JA Loring, JS Felmy, AR Hu, JZ AF Turcu, Romulus V. F. Hoyt, David W. Rosso, Kevin M. Sears, Jesse A. Loring, John S. Felmy, Andrew R. Hu, Jian Zhi TI Rotor design for high pressure magic angle spinning nuclear magnetic resonance SO JOURNAL OF MAGNETIC RESONANCE LA English DT Article DE NMR; MAS; High pressure; Sample cell; MAS rotor ID NMR-SPECTROSCOPY; CARBON-DIOXIDE; SUPERCRITICAL CO2; FORSTERITE; SEQUESTRATION; AQUIFER; SILICA; SPEED; BRINE; PROBE AB High pressure magic angle spinning (MAS) nuclear magnetic resonance (NMR) with a sample spinning rate exceeding 2.1 kHz and pressure greater than 165 bar has never been realized. In this work, a new sample cell design is reported, suitable for constructing cells of different sizes. Using a 7.5 mm high pressure MAS rotor as an example, internal pressure as high as 200 bar at a sample spinning rate of 6 kHz is achieved. The new high pressure MAS rotor is re-usable and compatible with most commercial NMR setups, exhibiting low H-1 and C-13 NMR background and offering maximal NMR sensitivity. As an example of its many possible applications, this new capability is applied to determine reaction products associated with the carbonation reaction of a natural mineral, antigorite ((Mg,Fe2+)(3)Si2O5(OH)(4)), in contact with liquid water in water-saturated supercritical CO2 (scCO(2)) at 150 bar and 50 degrees C. This mineral is relevant to the deep geologic disposal of CO2, but its iron content results in too many sample spinning sidebands at low spinning rate. Hence, this chemical system is a good case study to demonstrate the utility of the higher sample spinning rates that can be achieved by our new rotor design. We expect this new capability will be useful for exploring solid-state, including interfacial, chemistry at new levels of high-pressure in a wide variety of fields. (C) 2012 Elsevier Inc. All rights reserved. C1 [Turcu, Romulus V. F.; Hoyt, David W.; Rosso, Kevin M.; Sears, Jesse A.; Loring, John S.; Felmy, Andrew R.; Hu, Jian Zhi] Pacific NW Natl Lab, Richland, WA 99354 USA. RP Hu, JZ (reprint author), Pacific NW Natl Lab, Richland, WA 99354 USA. EM Jianzhi.Hu@pnl.gov RI Hoyt, David/H-6295-2013; Turcu, Flaviu/B-3555-2015; Hu, Jian Zhi/F-7126-2012 OI Turcu, Flaviu/0000-0002-0857-9868; FU Carbon Sequestration Initiative (CSI); Laboratory Directed Research and Development (LDRD) at Pacific Northwest National Laboratory (PNNL); DOE-BES-SISGR project; Department of Energy's Office of Biological and Environmental Research FX This research was supported by the Carbon Sequestration Initiative (CSI) funded by Laboratory Directed Research and Development (LDRD) at Pacific Northwest National Laboratory (PNNL), and in part by a DOE-BES-SISGR project. The research was performed using 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 PNNL. NR 25 TC 14 Z9 14 U1 4 U2 44 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 1090-7807 J9 J MAGN RESON JI J. Magn. Reson. PD JAN PY 2013 VL 226 BP 64 EP 69 DI 10.1016/j.jmr.2012.08.009 PG 6 WC Biochemical Research Methods; Physics, Atomic, Molecular & Chemical; Spectroscopy SC Biochemistry & Molecular Biology; Physics; Spectroscopy GA 079RU UT WOS:000314190700008 PM 23220181 ER PT J AU Straub, T Baird, C Bartholomew, RA Colburn, H Seiner, D Victry, K Zhang, L Bruckner-Lea, CJ AF Straub, Timothy Baird, Cheryl Bartholomew, Rachel A. Colburn, Heather Seiner, Derrick Victry, Kristin Zhang, Li Bruckner-Lea, Cynthia J. TI Estimated copy number of Bacillus anthracis plasmids pXO1 and pXO2 using digital PCR SO JOURNAL OF MICROBIOLOGICAL METHODS LA English DT Article DE Digital PCR; Real-time PCR; Copy number; Bacillus anthracis; Plasmids ID REAL-TIME PCR; DNA; QUANTIFICATION; SEQUENCE AB We evaluated digital PCR (dPCR) to directly enumerate plasmid and chromosome copies in three strains of Bacillus anthracis. Copy number estimates based on conventional quantitative PCR (qPCR) highlighted the variability of using qPCR to measure copy number whereas estimates based on direct sequencing are comparable to dPCR. (C) 2012 Elsevier B.V. All rights reserved. C1 [Straub, Timothy; Baird, Cheryl; Bartholomew, Rachel A.; Colburn, Heather; Seiner, Derrick; Victry, Kristin; Zhang, Li; Bruckner-Lea, Cynthia J.] Pacific NW Natl Lab, Chem & Biol Signature Sci Grp, Natl Secur Directorate, Richland, WA 99354 USA. RP Straub, T (reprint author), Pacific NW Natl Lab, Chem & Biol Signature Sci Grp, Natl Secur Directorate, POB 999,MS P750, Richland, WA 99354 USA. EM Timothy.Straub@pnnl.gov RI Baird, Cheryl/F-6569-2011 FU United States Department of Homeland Security Science and Technology Directorate [HSHQDC-08-X-00843]; U.S. Department of Energy [DE-AC06-76RLO]; DHS ST [HSHQDC-08-X-00763] FX This effort was funded by the United States Department of Homeland Security Science and Technology Directorate under contract HSHQDC-08-X-00843. Pacific Northwest National Laboratory is operated by Battelle for the U.S. Department of Energy under contract DE-AC06-76RLO. We are especially grateful to Dr. Norman Doggett at Los Alamos Laboratory for the training and the Fluidigm BioMark (TM) HD digital PCR instrument used for this research. Dr. Doggett is also funded by DHS S&T under contract HSHQDC-08-X-00763. A portion of this contract funding was used to purchase the Fluidigm instrument. NR 16 TC 8 Z9 9 U1 0 U2 25 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0167-7012 J9 J MICROBIOL METH JI J. Microbiol. Methods PD JAN PY 2013 VL 92 IS 1 BP 9 EP 10 DI 10.1016/j.mimet.2012.10.013 PG 2 WC Biochemical Research Methods; Microbiology SC Biochemistry & Molecular Biology; Microbiology GA 078BR UT WOS:000314073600002 PM 23142659 ER PT J AU Lima, E Diaz, A Guizar-Sicairos, M Gorelick, S Pernot, P Schleier, T Menzel, A AF Lima, E. Diaz, A. Guizar-Sicairos, M. Gorelick, S. Pernot, P. Schleier, T. Menzel, A. TI Cryo-scanning x-ray diffraction microscopy of frozen-hydrated yeast SO JOURNAL OF MICROSCOPY LA English DT Article DE Coherent x-ray diffraction; frozen-hydrated imaging; ptychography; scanning x-ray diffraction microscopy ID ELECTRON-MICROSCOPY; TOMOGRAPHY; RESOLUTION; CELLS; ULTRASTRUCTURE; NANOSCALE; PROTEIN AB We developed cryo-scanning x-ray diffraction microscopy, utilizing hard x-ray ptychography at cryogenic temperature, for the noninvasive, high-resolution imaging of wet, extended biological samples and report its first frozen-hydrated imaging. Utilizing phase contrast at hard x-rays, cryo-scanning x-ray diffraction microscopy provides the penetration power suitable for thick samples while retaining sensitivity to minute density changes within unstained samples. It is dose-efficient and further minimizes radiation damage by keeping the wet samples at cryogenic temperature. We demonstrate these capabilities in two dimensions by imaging unstained frozen-hydrated budding yeast cells, achieving a spatial resolution of 85 nm with a phase sensitivity of 0.0053 radians. The current work presents the feasibility of cryo-scanning x-ray diffraction microscopy for quantitative, high-resolution imaging of unmodified biological samples extending to tens of micrometres. C1 [Lima, E.] Brookhaven Natl Lab, Photon Sci Directorate, Upton, NY 11973 USA. [Diaz, A.; Guizar-Sicairos, M.; Gorelick, S.; Schleier, T.; Menzel, A.] Paul Scherrer Inst, Villigen, Switzerland. [Pernot, P.] European Synchrotron Radiat Facil, F-38043 Grenoble, France. RP Lima, E (reprint author), Brookhaven Natl Lab, Photon Sci Directorate, Upton, NY 11973 USA. EM elima@bnl.gov RI Diaz, Ana/I-4139-2013; Guizar-Sicairos, Manuel/I-4899-2013; Menzel, Andreas/C-4388-2012 OI Diaz, Ana/0000-0003-0479-4752; Menzel, Andreas/0000-0002-0489-609X FU U.S. Department of Energy, Office of Science [DE-AC02-98CH10886] FX X-ray measurements were performed at the cSAXS beamline (X12SA) of the Swiss Light Source, Paul Scherrer Institut, Villigen, Switzerland. The work at Brookhaven National Laboratory was supported by the U.S. Department of Energy, Office of Science, under Contact No. DE-AC02-98CH10886. The authors thank Roger Wepf for providing the cryo-plunging equipment and Xavier Donath for excellent technical support at the cSAXS beamline. NR 43 TC 20 Z9 20 U1 1 U2 32 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0022-2720 J9 J MICROSC-OXFORD JI J. Microsc.. PD JAN PY 2013 VL 249 IS 1 BP 1 EP 7 DI 10.1111/j.1365-2818.2012.03682.x PG 7 WC Microscopy SC Microscopy GA 076UO UT WOS:000313984000001 ER PT J AU Landau, SM Breault, C Joshi, AD Pontecorvo, M Mathis, CA Jagust, WJ Mintun, MA AF Landau, Susan M. Breault, Christopher Joshi, Abhinay D. Pontecorvo, Michael Mathis, Chester A. Jagust, William J. Mintun, Mark A. CA Alzheimer's Dis Neuroimaging TI Amyloid-beta Imaging with Pittsburgh Compound B and Florbetapir: Comparing Radiotracers and Quantification Methods SO JOURNAL OF NUCLEAR MEDICINE LA English DT Article DE amyloid-beta; Alzheimer's disease; PET imaging ID POSITRON-EMISSION-TOMOGRAPHY; MILD COGNITIVE IMPAIRMENT; ALZHEIMERS-DISEASE; F 18; PET; RADIOLIGAND; DEPOSITION; DEMENTIA AB C-11-Pittsburgh compound B (C-11-PiB) and F-18-florbetapir amyloid-beta (A beta) PET radioligands have had a substantial impact on Alzheimer disease research. Although there is evidence that both radioligands bind to fibrillar A beta in the brain, direct comparisons in the same individuals have not been reported. Here, we evaluated PiB and florbetapir in a retrospective convenience sample of cognitively normal older controls, patients with mild cognitive impairment, and patients with Alzheimer disease from the Alzheimer's Disease Neuroimaging Initiative (ADNI). Methods: From the ADNI database, 32 participants were identified who had undergone at least 1 PiB study and subsequently underwent a florbetapir study approximately 1.5 y after the last PiB study. Cortical PiB and florbetapir retention was quantified using several different methods to determine the effect of preprocessing factors (such as smoothing and reference region selection) and image processing pipelines. Results: There was a strong association between PiB and florbetapir cortical retention ratios (Spearman rho = 0.86-0.95), and these were slightly lower than cortical retention ratios for consecutive PiB scans (Spearman rho = 0.96-0.98) made approximately 1.1 y apart. Cortical retention ratios for A beta-positive subjects tended to be higher for PiB than for florbetapir images, yielding slopes for linear regression of florbetapir against PiB of 0.59-0.64. Associations between consecutive PiB scans and between PiB and florbetapir scans remained strong, regardless of processing methods such as smoothing, spatial normalization to a PET template, and use of reference regions. The PiB-florbetapir association was used to interconvert cutoffs for A beta positivity and negativity between the 2 radioligands, and these cutoffs were highly consistent in their assignment of A beta status. Conclusion: PiB and florbetapir retention ratios were strongly associated in the same individuals, and this relationship was consistent across several data analysis methods, despite scan-rescan intervals of more than a year. Cutoff thresholds for determining positive or negative A beta status can be reliably transformed from PiB to florbetapir units or vice versa using a population scanned with both radioligands. C1 [Landau, Susan M.; Jagust, William J.] Univ Calif Berkeley, Helen Wills Neurosci Inst, Berkeley, CA 94720 USA. [Landau, Susan M.; Jagust, William J.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Life Sci, Berkeley, CA 94720 USA. [Landau, Susan M.; Breault, Christopher; Joshi, Abhinay D.; Pontecorvo, Michael; Mintun, Mark A.] Avid Radiopharmaceut Inc, Philadelphia, PA USA. [Mathis, Chester A.] Univ Pittsburgh, Dept Radiol, PET Facil, Pittsburgh, PA 15260 USA. [Jagust, William J.] Univ Calif Berkeley, Sch Publ Hlth, Berkeley, CA 94720 USA. RP Landau, SM (reprint author), Univ Calif Berkeley, Helen Wills Neurosci Inst, 118 Barker Hall,MC 3190, Berkeley, CA 94720 USA. EM slandau@berkeley.edu FU ADNI (National Institutes of Health) [U01 AG024904]; Avid Radiopharmaceuticals, Inc.; NIH [U01 AG024904, P30AG010129, K01 AG030514, P30 AG010129]; Dana Foundation; National Institute on Aging, the National Institute of Biomedical Imaging and Bioengineering; Canadian Institutes of Health Research FX The costs of publication of this article were defrayed in part by the payment of page charges. Therefore, and solely to indicate this fact, this article is hereby marked "advertisement" in accordance with 18 USC section 1734. Data collection and sharing for this project was funded by the ADNI (National Institutes of Health grant U01 AG024904). This research was also supported by Avid Radiopharmaceuticals, Inc.; NIH grants P30AG010129, K01 AG030514, and U01 AG024904; and the Dana Foundation.; ADNI is funded by the National Institute on Aging, the National Institute of Biomedical Imaging and Bioengineering, and through generous contributions from the following: Abbott, Alzheimer's Association, Alzheimer's Drug Discovery Foundation, Amorfix Life Sciences Ltd., AstraZeneca, Bayer HealthCare, BioClinica, Inc., Biogen Idec Inc., Bristol-Myers Squibb Co., Eisai Inc., Elan Pharmaceuticals Inc., Eli Lilly and Company, F. Hoffmann-La Roche Ltd. and its affiliated company Genentech, Inc., GE Healthcare, Innogenetics, N.V., IXICO Ltd., Janssen Alzheimer Immunotherapy Research & Development, LLC, Johnson & Johnson Pharmaceutical Research & Development LLC, Medpace, Inc., Merck & Co., Inc., Meso Scale Diagnostics, LLC, Novartis Pharmaceuticals Corp., Pfizer Inc., Servier, Synarc Inc., and Takeda Pharmaceutical Co.. The Canadian Institutes of Health Research is providing funds to support ADNI clinical sites in Canada. Private sector contributions are facilitated by the Foundation for the National Institutes of Health (www.fnih.org). The grantee organization is the Northern California Institute for Research and Education, and the study is coordinated by the Alzheimer's Disease Cooperative Study at the University of California, San Diego. ADNI data are disseminated by the Laboratory for Neuro Imaging at the University of California, Los Angeles. This research was also supported by NIH grants P30 AG010129 and K01 AG030514. NR 20 TC 82 Z9 82 U1 2 U2 19 PU SOC NUCLEAR MEDICINE INC PI RESTON PA 1850 SAMUEL MORSE DR, RESTON, VA 20190-5316 USA SN 0161-5505 J9 J NUCL MED JI J. Nucl. Med. PD JAN PY 2013 VL 54 IS 1 BP 70 EP 77 DI 10.2967/jnumed.112.109009 PG 8 WC Radiology, Nuclear Medicine & Medical Imaging SC Radiology, Nuclear Medicine & Medical Imaging GA 071PN UT WOS:000313606800032 PM 23166389 ER PT J AU Shvartsburg, AA Seim, TA Danielson, WF Norheim, R Moore, RJ Anderson, GA Smith, RD AF Shvartsburg, Alexandre A. Seim, Tom A. Danielson, William F. Norheim, Randy Moore, Ronald J. Anderson, Gordon A. Smith, Richard D. TI High-Definition Differential Ion Mobility Spectrometry with Resolving Power up to 500 SO JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY LA English DT Article DE Ion mobility spectrometry; Differential IMS; FAIMS; High-resolution analyses ID FLIGHT MASS-SPECTROMETER; ESI-FAIMS-MS; SEPARATION PROCESS; HISTONE TAILS; RESOLUTION; ANALYZERS; GASES; SYSTEM AB As the resolution of analytical methods improves, further progress tends to be increasingly limited by instrumental parameter instabilities that were previously inconsequential. This is now the case with differential ion mobility spectrometry (FAIMS), where fluctuations of the voltages and gas pressure have become critical. A new high-definition generator for FAIMS compensation voltage reported here provides a stable and accurate output than can be scanned with negligible steps. This reduces the spectral drift and peak width, thus improving the resolving power (R) and resolution. The gain for multiply-charged peptides that have narrowest peaks is up to similar to 40 %, and R similar to 400-500 is achievable using He/N-2 or H-2/N-2 gas mixtures. C1 [Shvartsburg, Alexandre A.; Seim, Tom A.; Danielson, William F.; Norheim, Randy; Moore, Ronald J.; Anderson, Gordon A.; Smith, Richard D.] Pacific NW Natl Lab, Div Biol Sci, Richland, WA 99352 USA. RP Shvartsburg, AA (reprint author), Pacific NW Natl Lab, Div Biol Sci, Richland, WA 99352 USA. EM alexandre.shvartsburg@pnl.gov RI Smith, Richard/J-3664-2012 OI Smith, Richard/0000-0002-2381-2349 FU NIGMS [8P41 GM 103493-10]; PNNL use-at-facility funds FX The authors thank Dr. Keqi Tang for discussions and Dr. Yupeng Zheng and Professor Neil Kelleher for sharing the histone samples. This research was supported by NIGMS (8P41 GM 103493-10) and PNNL use-at-facility funds. Work was performed in the Environmental Molecular Sciences Laboratory, a US DoE OBER national scientific user facility at PNNL. NR 33 TC 23 Z9 23 U1 1 U2 58 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1044-0305 J9 J AM SOC MASS SPECTR JI J. Am. Soc. Mass Spectrom. PD JAN PY 2013 VL 24 IS 1 BP 109 EP 114 DI 10.1007/s13361-012-0517-5 PG 6 WC Biochemical Research Methods; Chemistry, Analytical; Chemistry, Physical; Spectroscopy SC Biochemistry & Molecular Biology; Chemistry; Spectroscopy GA 077RD UT WOS:000314044300013 PM 23345059 ER PT J AU Abouimrane, A Odom, SA Tavassol, H Schulmerich, MV Wu, HM Bhargava, R Gewirth, AA Moore, JS Amine, K AF Abouimrane, Ali Odom, Susan A. Tavassol, Hadi Schulmerich, Matthew V. Wu, Huiming Bhargava, Rohit Gewirth, Andrew A. Moore, Jeffrey. S. Amine, Khalil TI 3-Hexylthiophene as a Stabilizing Additive for High Voltage Cathodes in Lithium-Ion Batteries SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID ELECTROCHEMICAL-BEHAVIOR; RECHARGEABLE BATTERIES; LINI0.5MN1.5O4 SPINEL; RATE CAPABILITY; ELECTROLYTE; SPECTROSCOPY; TEMPERATURES; PERFORMANCE; INSERTION; LICOO2 AB 3-Hexylthiophene was incorporated into battery electrolyte as a life-extending additive. Upon oxidation, this monomer forms a conductive, conjugated polymer, resulting in significant increase in the cycle lifetimes of lithium half-cells containing high capacity Li1.2Ni0.15Co0.1Mn0.55O2 and high voltage LiNi0.5Mn1.5O4 cathodes. This additive significantly reduces the interfacial impedance growth observed in the cell without additive, which indicates an effective protection of the interface when using 3-hexythiophene. We also observed an improvement in safety when 3-hexylthiophene was incorporated. Electron microscopy images show the new polymer on the cathode surface, specifically poly(3-hexylthiophene) as supported by characterization of the cathode surface using vibrational spectroscopy (Raman and infrared) and mass spectrometry (MALDI). (C) 2012 The Electrochemical Society. [DOI: 10.1149/2.039302jes] All rights reserved. C1 [Abouimrane, Ali; Wu, Huiming; Amine, Khalil] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60539 USA. [Odom, Susan A.; Tavassol, Hadi; Moore, Jeffrey. S.] Univ Illinois, Dept Chem, Urbana, IL 61801 USA. [Odom, Susan A.; Schulmerich, Matthew V.; Bhargava, Rohit; Gewirth, Andrew A.; Moore, Jeffrey. S.] Univ Illinois, Beckman Inst Adv Sci & Technol, Urbana, IL 61801 USA. [Schulmerich, Matthew V.; Bhargava, Rohit] Univ Illinois, Micro & Nanotechnol Lab, Dept Bioengn, Urbana, IL 61801 USA. RP Abouimrane, A (reprint author), Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60539 USA. EM jsmoore@illinois.edu; amine@anl.gov RI Amine, Khalil/K-9344-2013; OI Bhargava, Rohit/0000-0001-7360-994X FU Center for Electrical Energy Storage, an Energy Frontier Research Center; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [919 DOE ANL 9F-31921 NS]; National Science Foundation through a National Science and Engineering Initiative [DMR-0642573]; NSF [CHE 0957849]; National Science Foundation for an American Competitiveness in Chemistry Fellowship; ARRA FX Funding for the majority of this work, including battery fabrication, electrical charactization, and SEM imaging was supported by the Center for Electrical Energy Storage, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences (Award Number 919 DOE ANL 9F-31921 NS). Support for Raman and IR imaging was provided by the National Science Foundation through a National Science and Engineering Initiative (Award Number DMR-0642573) and NSF CHE 0957849. SAO thanks the National Science Foundation for an American Competitiveness in Chemistry Fellowship funded by the ARRA. We thank Dr. Haijun Yao of Mass Spectrometry Laboratory of School of Chemical Sciences of University of Illinois for assistance with MALDI. NR 38 TC 23 Z9 25 U1 2 U2 169 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2013 VL 160 IS 2 BP A268 EP A271 DI 10.1149/2.039302jes PG 4 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA 071HJ UT WOS:000313581600010 ER PT J AU Dogan, F Joyce, C Vaughey, JT AF Dogan, Fulya Joyce, Christopher Vaughey, John T. TI Formation of Silicon Local Environments upon Annealing for Silicon Anodes: A Si-29 Solid State NMR Study SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID NUCLEAR-MAGNETIC-RESONANCE; LITHIUM-ION BATTERIES; POROUS SILICON; ELECTRODES; SURFACE; SI; SPECTROSCOPY; NANOWIRES; GROWTH; CARBON AB Si-29 magic angle spinning nuclear magnetic resonance (MAS NMR) has been used to characterize the binding interactions and interfacial phases formed between silicon and copper in a series of all-inorganic negative electrodes. The phases identified were correlated with electrochemical performance of the electrode. The electrode materials were prepared by copper deposition on silicon particles with varying Cu:Si ratios followed by heat-treatment at varying temperatures. Initial studies of the electrochemical performance of the anode materials indicated that samples with a 1:4 copper to silicon ratios and annealed at temperatures below 700 degrees C had the best cycling performance. Utilizing Si-29 MAS NMR we have been able to show that the best electrodes possess a single silicon local environment (from elemental silicon) and very little Cu3Si intermetallic formation. Electrodes with the compositions Cu:6Si and Cu:8Si annealed at certain conditions showed additional silicon resonances at -75, -92, -107 and 750 ppm and poor electrochemical performance. Combination of Si-29 Single Pulse and H-1/Si-29 Cross Polarization techniques were performed to study the nature of these silicon local environments. Preliminary assignments indicate that the presence of surface oxidation and hydration (from annealing process) are key variables that limit the electrochemical activity of the electrode. (C) 2012 The Electrochemical Society. [DOI: 10.1149/2.069302jes] All rights reserved. C1 [Dogan, Fulya; Joyce, Christopher; Vaughey, John T.] Argonne Natl Lab, Chem Sci & Engn Div, Electrochem Energy Storage Grp, Argonne, IL 60439 USA. RP Dogan, F (reprint author), Argonne Natl Lab, Chem Sci & Engn Div, Electrochem Energy Storage Grp, 9700 S Cass Ave, Argonne, IL 60439 USA. EM fdogan@anl.gov OI Vaughey, John/0000-0002-2556-6129 FU Office of Vehicle Technologies (Batteries for Advanced Transportation Technologies (BATT) Program) of the U.S. Department of Energy [DEAC02- 06CH11357] FX The authors thank Sara A. Bauer, Dr. Lynn Trahey and Dr. Baris Key for their assistance. Support to conduct this work came from the Office of Vehicle Technologies (Batteries for Advanced Transportation Technologies (BATT) Program) of the U.S. Department of Energy under Contract No. DEAC02- 06CH11357 and is gratefully acknowledged. NR 23 TC 6 Z9 7 U1 1 U2 38 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2013 VL 160 IS 2 BP A312 EP A319 DI 10.1149/2.069302jes PG 8 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA 071HJ UT WOS:000313581600018 ER PT J AU Li, JL Armstrong, BL Kiggans, J Daniel, C Wood, DL AF Li, Jianlin Armstrong, Beth L. Kiggans, Jim Daniel, Claus Wood, David L., III TI Lithium Ion Cell Performance Enhancement Using Aqueous LiFePO4 Cathode Dispersions and Polyethyleneimine Dispersant SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID LICOO2 CATHODES; ELECTROCHEMICAL PERFORMANCE; COMPOSITE ELECTRODES; CYCLIC VOLTAMMETRY; SCAN RATE; BATTERIES; BINDER; OPTIMIZATION; HOMOGENEITY; MECHANISM AB Switching manufacturing of composite battery electrodes from an organic system to an aqueous system provides both economic and environmental advantages. However, particle agglomeration of the electrode components and poor wetting of electrode dispersions to the current collectors are inherently introduced. Particle agglomeration can be mitigated by selection of appropriate dispersants. This research examines the effect of dispersant, poly(ethyleneimine) (PEI), on the associated morphology and electrochemical performance of LiFePO4. The addition of PEI reduces the agglomerate size and contributes to a more homogeneous distribution of cathode constituents, which results in a smoother, more uniform cathode surface. The LiFePO4 cathodes with PEI demonstrated a higher Li+ diffusion coefficient (1 x 10(-14) cm(2) s(-1)), better initial capacity (>142 mAh g(-1)), greater capacity retention (similar to 100%), and superior rate performance compared to the cathodes without PEI. When PEI concentration was varied, the LiFePO4 cathode with 2 wt% PEI exhibited the best performance at 167 mAh g(-1) capacity (98% of the theoretical capacity) and 100% retention after 50 cycles when discharged at 0.2C at 25 degrees C in a half cell. (C) 2012 The Electrochemical Society. [DOI: 10.1149/2.037302jes] All rights reserved. C1 [Li, Jianlin; Armstrong, Beth L.; Kiggans, Jim; Wood, David L., III] Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. [Daniel, Claus] 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 Li, JL (reprint author), Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. EM lij4@ornl.gov RI Daniel, Claus/A-2060-2008; kiggans, james/E-1588-2017; Armstrong, Beth/E-6752-2017 OI Daniel, Claus/0000-0002-0571-6054; kiggans, james/0000-0001-5056-665X; Armstrong, Beth/0000-0001-7149-3576 FU Advanced Manufacturing Office; Vehicle Technologies of the Office of Energy Efficiency and Renewable Energy; ORNL Scientific User Facilities Division FX This research was performed at Oak Ridge National Laboratory and was sponsored by the Advanced Manufacturing Office and Vehicle Technologies of the Office of Energy Efficiency and Renewable Energy. Part of the work was conducted at the Shared Research Equipment (SHaRE) user facility, which is sponsored by the ORNL Scientific User Facilities Division. The authors also thank Phostech Lithium Inc. and Timcal Corporation for supplying materials. NR 32 TC 25 Z9 25 U1 8 U2 69 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2013 VL 160 IS 2 BP A201 EP A206 DI 10.1149/2.037302jes PG 6 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA 071HJ UT WOS:000313581600001 ER PT J AU Lv, DP Xu, T Saha, P Datta, MK Gordin, ML Manivannan, A Kumta, PN Wang, DH AF Lv, Dongping Xu, Terrence Saha, Partha Datta, Moni Kanchan Gordin, Mikhail L. Manivannan, Ayyakkannu Kumta, Prashant N. Wang, Donghai TI A Scientific Study of Current Collectors for Mg Batteries in Mg(AlCl2EtBu)(2)/THF Electrolyte SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID RECHARGEABLE MAGNESIUM BATTERIES; ION BATTERIES; INTERCALATION PROPERTIES; CATHODE MATERIALS; DEPOSITION; COMPOSITES; REVERSIBILITY; DISSOLUTION; NANOTUBES; CORROSION AB The electrochemical behavior and stability of several current collectors (copper, nickel, stainless steel 316L, aluminum, titanium) potentially employed in magnesium batteries with non-aqueous Mg(AlCl2EtBu)(2)/THF electrolyte have been investigated in both three-electrode electrochemical cell and coin cell configurations. Linear sweep voltammetry and coin cell charge/discharge measurements indicate that copper, widely used in the literature as a current collector in this electrolyte, is not stable and undergoes pitting corrosion above similar to 1.8 V. Cyclic voltammetry shows that copper undergoes electrochemical oxidation and reduction in the electrolyte, which was further confirmed by inductively coupled plasma atomic emission spectroscopy (ICP-AES), scanning electron microscopy (SEM), and energy-dispersive X-ray spectroscopy (EDX) analyses. Among the current collectors studied, nickel shows excellent electrochemical stability up to similar to 2.2 V and high efficiency for magnesium deposition and dissolution processes in the electrolyte, indicating that it is a strong candidate as both cathode and anode current collectors in magnesium batteries. (C) 2012 The Electrochemical Society. [DOI: 10.1149/2.085302jes] All rights reserved. C1 [Lv, Dongping; Xu, Terrence; Gordin, Mikhail L.; Wang, Donghai] Penn State Univ, Dept Mech & Nucl Engn, University Pk, PA 16802 USA. [Saha, Partha; Datta, Moni Kanchan; Kumta, Prashant N.] Univ Pittsburgh, Dept Bioengn, Swanson Sch Engn, Pittsburgh, PA 15261 USA. [Manivannan, Ayyakkannu] US DOE NETL, Mat Performance Div, Morgantown, WV 26507 USA. [Kumta, Prashant N.] Univ Pittsburgh, Dept Chem & Petr Engn, Swanson Sch Engn, Pittsburgh, PA 15261 USA. [Kumta, Prashant N.] Univ Pittsburgh, Ctr Complex Engn Multifunct Mat, Swanson Sch Engn, Pittsburgh, PA 15261 USA. EM pkumta@pitt.edu; dwang@psu.edu RI SAHA, PARTHA/D-5508-2011; Wang, Donghai/L-1150-2013; Xu, Terrence/M-8741-2014 OI SAHA, PARTHA/0000-0002-0309-8387; Wang, Donghai/0000-0001-7261-8510; Xu, Terrence/0000-0002-9385-6881 FU National Energy Technology Laboratory's Regional University Alliance (NETL-RUA), a collaborative initiative of the NETL [4000.2.683.220.001]; Center for Complex Engineered Multifunctional Materials (CCEMM); 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 4000.2.683.220.001. Financial support of Dr. Robert Romanosky is acknowledged. In addition, PNK acknowledges the Edward R. Weidlein Chair Professorship 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. Authors Dongping Lv and Partha Saha contributed equally to this work. NR 29 TC 38 Z9 38 U1 5 U2 122 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2013 VL 160 IS 2 BP A351 EP A355 DI 10.1149/2.085302jes PG 5 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA 071HJ UT WOS:000313581600023 ER PT J AU Sethuraman, VA Srinivasan, V Newman, J AF Sethuraman, Vijay A. Srinivasan, Venkat Newman, John TI Analysis of Electrochemical Lithiation and Delithiation Kinetics in Silicon SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID LITHIUM-ION BATTERIES; SOLID-ELECTROLYTE-INTERPHASE; IN-SITU MEASUREMENTS; AMORPHOUS-SILICON; CARBON NANOTUBES; NANOSTRUCTURED SILICON; INTERFACIAL PROPERTIES; NEGATIVE ELECTRODES; SURFACE-CHEMISTRY; COMPOSITE ANODES AB Analysis of lithiation and delithiation kinetics in pulse-laser-deposited crystalline thin-film silicon (Si) electrodes is presented. Data from open-circuit relaxation experiments are used in conjunction with a model based on Tafel kinetics and double-layer capacitance to estimate the apparent transfer coefficients (alpha(a), alpha(c)) and exchange current density to capacitance ratio (i(0)/C-dl) for lithiation and delithiation reactions in a lithiated silicon (LixSi) system. Parameters estimated from data sets obtained during first-cycle amorphization of crystalline Si, as well as from cycled crystalline Si and amorphous Si thin-film electrodes do not show much variation, indicating that they are intrinsic to lithiation/delithiation in Si. A methodology to estimate the side-reaction rate on a well-cycled electrode and its role in the evolution of the open-circuit potential of the LixSi system are discussed. We conclude that the large potential offset between lithiation and delithiation reactions at any given state of charge is partially caused by a large kinetic resistance (i.e., small i(0)). Using the estimated parameters, the model is shown to predict successfully the behavior of the system under galvanostatic lithiation and delithiation. (C) 2012 The Electrochemical Society. [DOI: 10.1149/2.008303jes] All rights reserved. C1 [Sethuraman, Vijay A.; Srinivasan, Venkat; Newman, John] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. [Newman, John] Univ Calif Berkeley, Dept Chem & Biomol Engn, Berkeley, CA 94720 USA. RP Sethuraman, VA (reprint author), Brown Univ, Sch Engn, Providence, RI 02912 USA. EM vj@cal.berkeley.edu; VSrinivasan@lbl.gov RI Sethuraman, Vijay/E-5702-2010 OI Sethuraman, Vijay/0000-0003-4624-1355 FU Office of Vehicle Technologies; United States Department of Energy [DE-AC02-05CH11231]; National Center for Microscopy at LBNL FX The authors gratefully acknowledge the financial support from the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies, the United States Department of Energy under contract no. DE-AC02-05CH11231. The authors thank Dr. Robert Kostecki and Dr. Laurence J. Hardwick (LBNL) for help with Raman spectroscopy measurements; Xiaojun Zhang and Dr. Samuel S. Mao (LBNL) for help with pulse-laser deposition; Dr. Keith D. Kepler (Farasis Energy, Inc.) for help with coin-cell fabrication; Xiangyun Song (LBNL) for help with electron microscopy and X-ray measurements. The authors acknowledge the support of the National Center for Microscopy at LBNL, which is supported by the United States Department of Energy under contract no. DE-AC02-05CH11231. The authors acknowledge the Microlab at the Department of Electrical Engineering in the University of California, Berkeley, for the fabrication of amorphous Si thin films. NR 89 TC 27 Z9 27 U1 11 U2 177 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2013 VL 160 IS 2 BP A394 EP A403 DI 10.1149/2.008303jes PG 10 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA 071HJ UT WOS:000313581600030 ER PT J AU Arise, I Kawai, S Fukunaka, Y McLarnon, FR AF Arise, I. Kawai, S. Fukunaka, Y. McLarnon, F. R. TI Coupling Phenomena between Zinc Surface Morphological Variations and Ionic Mass Transfer Rate in Alkaline Solution SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID MODEL PORE ELECTRODE; NI-ZN CELLS; CONCENTRATION DISTRIBUTIONS; ANODIC-DISSOLUTION; PASSIVATION; DISCHARGE; BEHAVIOR; GROWTH; MEDIA AB A horizontal upward-facing Zn anode was electrochemically dissolved in aqueous alkaline electrolyte. A plane-parallel upward-facing Ni(OH)(2)/NiOOH cathode was combined with the Zn anode in a single cell, divided by a polymer separator. This configuration can be regarded as a single pore model inside the porous space of a Zn-NiOOH battery cell. It also insures that the ionic mass transfer rate by diffusion and migration mechanism is dominant over that by natural convection. The morphological variations of the Zn anode surface were examined during the discharge operation of the Zn-NiOOH model cell. Two-dimensional transient concentration profiles of each ion accompanying the electrochemical dissolution of Zn anode in alkaline electrolyte were numerically calculated. The surface morphological variations of the Zn anode were discussed with the aid of numerical simulation. ZnO precipitation on the Zn anode surface was confirmed to be dependent on the horizontal distance from the separator. The present numerical model provides insight to the analysis of observed morphological variations along the Zn anode surface. (C) 2012 The Electrochemical Society. [DOI: 10.1149/2.083302jes] All rights reserved. C1 [Arise, I.; Kawai, S.] Kyoto Univ, Grad Sch Energy Sci, Dept Energy Sci & Technol, Kyoto 6068501, Japan. [Fukunaka, Y.] Waseda Univ, Nano Technol Res Ctr, Tokyo 1620041, Japan. [McLarnon, F. R.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. RP Arise, I (reprint author), Kyoto Univ, Grad Sch Energy Sci, Dept Energy Sci & Technol, Kyoto 6068501, Japan. EM hirofukunaka@gmail.com NR 32 TC 7 Z9 7 U1 3 U2 39 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2013 VL 160 IS 2 BP D66 EP D74 DI 10.1149/2.083302jes PG 9 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA 071HJ UT WOS:000313581600045 ER PT J AU Papandrew, AB Chisholm, CRI Zecevic, SK Veith, GM Zawodzinski, TA AF Papandrew, Alexander B. Chisholm, Calum R. I. Zecevic, Strahinja K. Veith, Gabriel M. Zawodzinski, Thomas A., Jr. TI Activity and Evolution of Vapor Deposited Pt-Pd Oxygen Reduction Catalysts for Solid Acid Fuel Cells SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID ALKYNE HYDROGENATION; PALLADIUM CATALYSTS; L-3 EDGE; ELECTROCATALYSTS; NANOPARTICLES; MONOLAYER; CARBIDE; CARBON; PHASE; OXIDE AB The performance of hydrogen fuel cells based on the crystalline solid proton conductor CsH2PO4 is circumscribed by the mass activity of platinum oxygen reduction catalysts in the cathode. Here we report on the first application of an alloy catalyst in a solid acid fuel cell, and demonstrate a mass activity 4.5 times greater than Pt at 0.8 V. This activity enhancement was obtained with platinum-palladium alloys that were vapor-deposited directly on CsH2PO4 at 210 degrees C. Catalyst mass activity peaks at a composition of 84 at% Pd, though smaller activity enhancements are observed for catalyst compositions exceeding 50 at% Pd. Prior to fuel cell testing, Pd-rich catalysts display lattice parameter expansions of up to 2% due to the presence of interstitial carbon. After fuel cell testing, a Pt-Pd solid solution absent of lattice dilatation and depleted in carbon is recovered. The structural evolution of the catalysts is correlated with catalyst de-activation. (C) 2012 The Electrochemical Society. [DOI: 10.1149/2.002303jes] All rights reserved. C1 [Papandrew, Alexander B.; Zawodzinski, Thomas A., Jr.] Univ Tennessee, Dept Chem & Biomol Engn, Knoxville, TN 37996 USA. [Chisholm, Calum R. I.; Zecevic, Strahinja K.] SAFCell Inc, Pasadena, CA 91106 USA. [Veith, Gabriel M.; Zawodzinski, Thomas A., Jr.] Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN 37831 USA. RP Papandrew, AB (reprint author), Univ Tennessee, Dept Chem & Biomol Engn, Knoxville, TN 37996 USA. EM apapandr@utk.edu FU National Science Foundation through TN-SCORE [NSF EPS-1004083]; University of Tennessee; U.S. Department of Energy's Office of Basic Energy Science, Division of Materials Sciences and Engineering; UT-Battelle, LLC FX Partial support for this work was provided by the National Science Foundation through TN-SCORE (NSF EPS-1004083) and by the University of Tennessee's Governor's Chair Fund. A portion of this work was supported by the U.S. Department of Energy's Office of Basic Energy Science, Division of Materials Sciences and Engineering, under contract with UT-Battelle, LLC. A. B. P. thanks David Wilson for assistance with sample preparation. NR 43 TC 14 Z9 14 U1 4 U2 59 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2013 VL 160 IS 2 BP F175 EP F182 DI 10.1149/2.002303jes PG 8 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA 071HJ UT WOS:000313581600059 ER PT J AU Zheng, LJ Srouji, AK Dross, R Turhan, A Mench, MM AF Zheng, L. J. Srouji, A. K. Dross, R. Turhan, A. Mench, M. M. TI Computational Engineering of Porous Flow Field PEFCs to Enable High Temperature High Power Density Operation SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID ELECTROLYTE FUEL-CELLS; POLYMER-ELECTROLYTE; WATER-TRANSPORT; MATHEMATICAL-MODEL; BIPOLAR/END PLATES; OXYGEN REDUCTION; MEMBRANE; METHANOL; PERFORMANCE; PARAMETERS AB A comprehensive 2D + 1 multi-phase computational model has been applied to polymer electrolyte fuel cells with a porous metallic flow field to investigate operating strategies which enable high power density operation in dry, elevated temperature environment. Extensive experimental model validation has been completed under a wide range of temperature, pressure, stoichiometry and humidity conditions. Both qualitative and quantitative agreement has been achieved in regard to voltage, area-specific resistance, and net water drag coefficient. Internal water distribution predictions show that modest changes in operating parameters on the cathode side help maintain a hydrated anode stream and thus effectively push the envelope of stable operating temperature 20 degrees C higher, enabling more efficient heat dissipation in coolant system. Results also show that thermo-osmotic water flux across the membrane, as observed and measured experimentally, can be significant compared to electro-osmosis under high current (> 2 A/cm(2)) hot and dry conditions, even with thin electrolyte membranes. (C) 2012 The Electrochemical Society. [DOI: 10.1149/2.056302jes] All rights reserved. C1 [Zheng, L. J.] Penn State Univ, Dept Mech & Nucl Engn, University Pk, PA 16801 USA. [Srouji, A. K.] Penn State Univ, Dept Energy & Mineral Engn, University Pk, PA 16801 USA. [Dross, R.] Nuvera Fuel Cells Inc, Billerica, MA 01821 USA. [Turhan, A.; Mench, M. M.] Univ Tennessee, Electrochem Energy Storage & Convers Lab, Dept Mech Aerosp & Biomed Engn, Knoxville, TN 37996 USA. [Mench, M. M.] Oak Ridge Natl Lab, Energy & Transportat Sci Div, Oak Ridge, TN 37831 USA. RP Zheng, LJ (reprint author), Penn State Univ, Dept Mech & Nucl Engn, University Pk, PA 16801 USA. EM matthewmench@gmail.com FU United States Department of Energy (DOE) Energy Efficiency and Renewable Energy (EERE) Program through Nuvera Fuel Cells Inc. [DE-EE0000472] FX The authors thank Amedeo Conti from Nuvera Fuel Cells Inc. for many helpful discussions and guidance. This work is funded by the United States Department of Energy (DOE) Energy Efficiency and Renewable Energy (EERE) Program through Nuvera Fuel Cells Inc. under contract number DE-EE0000472. NR 34 TC 8 Z9 8 U1 0 U2 15 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2013 VL 160 IS 2 BP F119 EP F128 DI 10.1149/2.056302jes PG 10 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA 071HJ UT WOS:000313581600052 ER PT J AU Gallagher, KG Dees, DW Jansen, AN Abraham, DP Kang, SH AF Gallagher, Kevin G. Dees, Dennis W. Jansen, Andrew N. Abraham, Daniel P. Kang, Sun-Ho TI A Volume Averaged Approach to the Numerical Modeling of Phase-Transition Intercalation Electrodes Presented for LixC6 (vol 159, pg A2029 2012) SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Correction C1 [Gallagher, Kevin G.; Dees, Dennis W.; Jansen, Andrew N.; Abraham, Daniel P.; Kang, Sun-Ho] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. RP Gallagher, KG (reprint author), Argonne Natl Lab, Chem Sci & Engn Div, 9700 S Cass Ave, Argonne, IL 60439 USA. RI Jansen, Andrew/Q-5912-2016 OI Jansen, Andrew/0000-0003-3244-7790 NR 1 TC 0 Z9 0 U1 0 U2 15 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2013 VL 160 IS 2 BP X1 EP X1 DI 10.1149/2.073302jes PG 1 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA 071HJ UT WOS:000313581600078 ER PT J AU Cybart, SA Roediger, P Ulin-Avila, E Wu, SM Wong, TJ Dynes, RC AF Cybart, Shane A. Roediger, Peter Ulin-Avila, Erick Wu, Stephen M. Wong, Travis J. Dynes, Robert C. TI Nanometer scale high-aspect-ratio trench etching at controllable angles using ballistic reactive ion etching SO JOURNAL OF VACUUM SCIENCE & TECHNOLOGY B LA English DT Article ID NANOIMPRINT LITHOGRAPHY; DESIGN CONSIDERATIONS; IMPLANTER; CL-2 AB The authors demonstrate a low pressure reactive ion etching process capable of patterning nanometer scale angled sidewalls and three dimensional structures in photoresist. At low pressure, the plasma has a large dark space region where the etchant ions have very large highly directional mean free paths. Mounting the sample entirely within this dark space allows for etching at angles relative to the cathode with minimal undercutting, resulting in high-aspect ratio nanometer scale angled features. By reversing the initial angle and performing a second etch, the authors create three-dimensional mask profiles. (C) 2013 American Vacuum Society. [http://dx.doi.org/10.1116/1.4773919] C1 [Cybart, Shane A.; Ulin-Avila, Erick; Wu, Stephen M.; Dynes, Robert C.] Univ Calif Berkeley, Dept Phys, Berkeley, CA 94720 USA. [Cybart, Shane A.; Dynes, Robert C.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. [Roediger, Peter; Wong, Travis J.; Dynes, Robert C.] Univ Calif, Dept Phys, La Jolla, CA 92093 USA. RP Cybart, SA (reprint author), Univ Calif Berkeley, Dept Phys, Berkeley, CA 94720 USA. EM scybart@gmail.com RI Cybart, Shane/E-3518-2013; ulin-avila, erick/M-3278-2014 FU AFOSR [FA9550-07-1-0493]; ONR [N00014-11-1-0049]; Office of Science and Office of Basic Energy Sciences of the U.S. Department of Energy [DEAC02-05CH11231] FX This work was supported by AFOSR Grant FA9550-07-1-0493, ONR Grant N00014-11-1-0049, and the Office of Science and Office of Basic Energy Sciences of the U.S. Department of Energy under Contract No. DEAC02-05CH11231. NR 14 TC 3 Z9 3 U1 1 U2 13 PU A V S AMER INST PHYSICS PI MELVILLE PA STE 1 NO 1, 2 HUNTINGTON QUADRANGLE, MELVILLE, NY 11747-4502 USA SN 1071-1023 J9 J VAC SCI TECHNOL B JI J. Vac. Sci. Technol. B PD JAN PY 2013 VL 31 IS 1 AR 010604 DI 10.1116/1.4773919 PG 4 WC Engineering, Electrical & Electronic; Nanoscience & Nanotechnology; Physics, Applied SC Engineering; Science & Technology - Other Topics; Physics GA 072LN UT WOS:000313672600025 ER PT J AU Liu, L Lo, CF Xi, YY Ren, F Pearton, SJ Laboutin, O Cao, Y Johnson, JW Kravchenko, II AF Liu, Lu Lo, Chien-Fong Xi, Yuyin Ren, Fan Pearton, Stephen J. Laboutin, Oleg Cao, Yu Johnson, J. Wayne Kravchenko, Ivan I. TI Effect of buffer structures on AlGaN/GaN high electron mobility transistor reliability SO JOURNAL OF VACUUM SCIENCE & TECHNOLOGY B LA English DT Article ID FIELD-EFFECT TRANSISTORS; YELLOW LUMINESCENCE; BREAKDOWN VOLTAGE; SURFACE-STATES; GAN; THICKNESS; LAYER; PHOTOLUMINESCENCE; GROWTH; DESIGN AB AlGaN/GaN high electron mobility transistors (HEMTs) with three different types of buffer layers, including a GaN/AlGaN composite layer, or 1 or 2 mu m GaN thick layers, were fabricated and their reliability compared. The HEMTs with the thick GaN buffer layer showed the lowest critical voltage (V-cri) during off-state drain step-stress, but this was increased by around 50% and 100% for devices with the composite AlGaN/GaN buffer layers or thinner GaN buffers, respectively. The Voff-state for HEMTs with thin GaN and composite buffers were similar to 100 V, however, this degraded to 50-60V for devices with thick GaN buffers due to the difference in peak electric field near the gate edge. A similar trend was observed in the isolation breakdown voltage measurements, with the highest V-iso achieved based on thin GaN or composite buffer designs (600-700 V), while a much smaller V-iso of similar to 200V was measured on HEMTs with the thick GaN buffer layers. These results demonstrate the strong influence of buffer structure and defect density on AlGaN/GaN HEMT performance and reliability. (C) 2013 American Vacuum Society. [http://dx.doi.org/10.1116/1.4773060] C1 [Liu, Lu; Lo, Chien-Fong; Xi, Yuyin; Ren, Fan] Univ Florida, Dept Chem Engn, Gainesville, FL 32611 USA. [Pearton, Stephen J.] Univ Florida, Dept Mat Sci & Engn, Gainesville, FL 32611 USA. [Laboutin, Oleg; Cao, Yu; Johnson, J. Wayne] Kopin Corp, Taunton, MA 02780 USA. [Kravchenko, Ivan I.] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37830 USA. RP Liu, L (reprint author), Univ Florida, Dept Chem Engn, Gainesville, FL 32611 USA. EM fren@che.ufl.edu RI LIU, LU/H-2307-2013; Kravchenko, Ivan/K-3022-2015 OI LIU, LU/0000-0001-7256-3775; Kravchenko, Ivan/0000-0003-4999-5822 FU AFOSR MURI; Oak Ridge National Laboratory by the Office of Basic Energy Sciences, U.S. Department of Energy FX This work was supported by an AFOSR MURI monitored by James Hwang. A portion of this research was conducted at the Center for Nanophase Materials Sciences, which was sponsored at Oak Ridge National Laboratory by the Office of Basic Energy Sciences, U.S. Department of Energy. NR 30 TC 10 Z9 10 U1 1 U2 37 PU A V S AMER INST PHYSICS PI MELVILLE PA STE 1 NO 1, 2 HUNTINGTON QUADRANGLE, MELVILLE, NY 11747-4502 USA SN 1071-1023 J9 J VAC SCI TECHNOL B JI J. Vac. Sci. Technol. B PD JAN PY 2013 VL 31 IS 1 AR 011805 DI 10.1116/1.4773060 PG 6 WC Engineering, Electrical & Electronic; Nanoscience & Nanotechnology; Physics, Applied SC Engineering; Science & Technology - Other Topics; Physics GA 072LN UT WOS:000313672600046 ER PT J AU Song, HS Ramkrishna, D Pinchuk, GE Beliaev, AS Konopka, AE Fredrickson, JK AF Song, Hyun-Seob Ramkrishna, Doraiswami Pinchuk, Grigoriy E. Beliaev, Alexander S. Konopka, Allan E. Fredrickson, James K. TI Dynamic modeling of aerobic growth of Shewanella oneidensis. Predicting triauxic growth, flux distributions, and energy requirement for growth SO METABOLIC ENGINEERING LA English DT Article DE Shewanella oneidensis; Lumped hybrid cybernetic model (L-HCM); Dynamic metabolic model; ATP requirement for growth; C-13-MFA ID CYBERNETIC MODELS; KINETIC-MODEL; SACCHAROMYCES-CEREVISIAE; METABOLIC FUNCTION; MR-1; REDUCTION; PYRUVATE; XYLOSE; YIELD; BATCH AB A model-based analysis is conducted to investigate metabolism of Shewanella oneidensis MR-1 strain in aerobic batch culture, which exhibits an intriguing growth pattern by sequentially consuming substrate (i.e., lactate) and by-products (i.e., pyruvate and acetate). A general protocol is presented for developing a detailed network-based dynamic model for S. oneidensis based on the Lumped Hybrid Cybernetic Model (L-HCM) framework. The L-HCM, although developed from only limited data, is shown to accurately reproduce exacting dynamic metabolic shifts, and provide reasonable estimates of energy requirement for growth. Flux distributions in S. oneidensis predicted by the L-HCM compare very favorably with C-13-metabolic flux analysis results reported in the literature. Predictive accuracy is enhanced by incorporating measurements of only a few intracellular fluxes, in addition to extracellular metabolites. The L-HCM developed here for S. oneidensis is consequently a promising tool for the analysis of intracellular flux distribution and metabolic engineering. (C) 2012 Elsevier Inc. All rights reserved. C1 [Song, Hyun-Seob; Ramkrishna, Doraiswami] Purdue Univ, Sch Chem Engn, W Lafayette, IN 47907 USA. [Pinchuk, Grigoriy E.; Beliaev, Alexander S.; Konopka, Allan E.; Fredrickson, James K.] Pacific NW Natl Lab, Div Biol Sci, Richland, WA 99352 USA. RP Ramkrishna, D (reprint author), Purdue Univ, Sch Chem Engn, W Lafayette, IN 47907 USA. EM ramkrish@ecn.purdue.edu; grigoriy.pinchuk@pnnl.gov RI Beliaev, Alexander/E-8798-2016 OI Beliaev, Alexander/0000-0002-6766-4632 FU Office of Biological and Environmental Research (OBER), U.S. Department of Energy (DOE); Center for Science of Information (CSoI), NSF Science and Technology Center [CCF-0939370] FX This research was supported by the Genomic Science Program (GSP), Office of Biological and Environmental Research (OBER), U.S. Department of Energy (DOE), and is a contribution of the Pacific Northwest National Laboratory (PNNL) Foundation and Biofuels Scientific Focus Areas. Partial support was also provided by the Center for Science of Information (CSoI), an NSF Science and Technology Center, under Grant agreement CCF-0939370. NR 36 TC 8 Z9 8 U1 3 U2 46 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 1096-7176 J9 METAB ENG JI Metab. Eng. PD JAN PY 2013 VL 15 BP 25 EP 33 DI 10.1016/j.ymben.2012.08.004 PG 9 WC Biotechnology & Applied Microbiology SC Biotechnology & Applied Microbiology GA 075JW UT WOS:000313882500003 PM 23022551 ER PT J AU Ha, SJ Galazka, JM Oh, EJ Kordic, V Kim, H Jin, YS Cate, JHD AF Ha, Suk-Jin Galazka, Jonathan M. Oh, Eun Joong Kordic, Vesna Kim, Heejin Jin, Yong-Su Cate, Jamie H. D. TI Energetic benefits and rapid cellobiose fermentation by Saccharomyces cerevisiae expressing cellobiose phosphorylase and mutant cellodextrin transporters SO METABOLIC ENGINEERING LA English DT Article DE Cellobiose; Phosphorylase; beta-glucosidase; Cellodextrin transporter; Thermodynamics ID SITE-SATURATION MUTAGENESIS; CLOSTRIDIUM-THERMOCELLUM; CELLULOSIC BIOFUELS; HYDROLYSIS; YEAST; GLUCOSE; ACID; THERMODYNAMICS; PURIFICATION; RESISTANCE AB Anaerobic bacteria assimilate cellodextrins from plant biomass by using a phosphorolytic pathway to generate glucose intermediates for growth. The yeast Saccharomyces cerevisiae can also be engineered to ferment cellobiose to ethanol using a cellodextrin transporter and a phosphorolytic pathway. However, strains with an intracellular cellobiose phosphorylase initially fermented cellobiose slowly relative to a strain employing an intracellular beta-glucosidase. Fermentations by the phosphorolytic strains were greatly improved by using cellodextrin transporters with elevated rates of cellobiose transport. Furthermore under stress conditions, these phosphorolytic strains had higher biomass and ethanol yields compared to hydrolytic strains. These observations suggest that, although cellobiose phosphorolysis has energetic advantages, phosphorolytic strains are limited by the thermodynamics of cellobiose phosphorolysis (Delta G degrees = +3.6 kJ mol(-1)). A thermodynamic "push" from the reaction immediately upstream (transport) is therefore likely to be necessary to achieve high fermentation rates and energetic benefits of phosphorolysis pathways in engineered S. cerevisiae. (C) 2012 Elsevier Inc. All rights reserved. C1 [Ha, Suk-Jin; Oh, Eun Joong; Kim, Heejin; Jin, Yong-Su] Univ Illinois, Dept Food Sci & Human Nutr, Urbana, IL 61801 USA. [Ha, Suk-Jin; Oh, Eun Joong; Kim, Heejin; Jin, Yong-Su] Univ Illinois, Inst Genom Biol, Urbana, IL 61801 USA. [Galazka, Jonathan M.; Kordic, Vesna; Cate, Jamie H. D.] Univ Calif Berkeley, Dept Mol & Cell Biol, Berkeley, CA 94720 USA. [Cate, Jamie H. D.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA 94720 USA. RP Cate, JHD (reprint author), Univ Calif Berkeley, Dept Mol & Cell Biol, 229 Stanley Hall, Berkeley, CA 94720 USA. EM ysjin@illinois.edu; jcate@lbl.gov RI Jin, Yong-Su/L-4530-2013; OI Galazka, Jonathan/0000-0002-4153-0249 FU Energy Biosciences Institute FX This work was supported by funding from the Energy Biosciences Institute to Jamie Cate and Yong-Su Jin. The authors thank William Beeson, Soo Rin Kim, and Na Wei for helpful discussions, and Mara Bryan and Crystal Chan for technical support. NR 41 TC 22 Z9 23 U1 3 U2 30 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 1096-7176 J9 METAB ENG JI Metab. Eng. PD JAN PY 2013 VL 15 BP 134 EP 143 DI 10.1016/j.ymben.2012.11.005 PG 10 WC Biotechnology & Applied Microbiology SC Biotechnology & Applied Microbiology GA 075JW UT WOS:000313882500013 PM 23178501 ER PT J AU Deng, Y Olson, DG Zhou, JL Herring, CD Shaw, AJ Lynd, LR AF Deng, Yu Olson, Daniel G. Zhou, Jilai Herring, Christopher D. Shaw, A. Joe Lynd, Lee R. TI Redirecting carbon flux through exogenous pyruvate kinase to achieve high ethanol yields in Clostridium thermocellum SO METABOLIC ENGINEERING LA English DT Article DE Clostridium thermocellum; Ethanol yield; Pyruvate kinase; Malate shunt ID PHOSPHOENOLPYRUVATE CARBOXYKINASE; SACCHAROMYCES-CEREVISIAE; CARBOHYDRATE-METABOLISM; THERMOPHILIC BACTERIA; ESCHERICHIA-COLI; DNA FRAGMENTS; MALIC ENZYME; FERMENTATION; GENE; REDUCTION AB In Clostridium thermocellum, a thermophilic anaerobic bacterium able to rapidly ferment cellulose to ethanol, pyruvate kinase (EC 2.7.1.40) is absent based on both the genome sequence and enzymatic assays. Instead, a new pathway converting phosphoenolpyruvate to pyruvate via a three-step pathway involving phosphoenolpyruvate carboxykinase, NADH-linked malate dehydrogenase, and NADP-dependent malic enzyme has been found. We examined the impact of targeted modification of enzymes associated with this pathway, termed the "malate shunt", including expression of the pyruvate kinase gene from Thermoanaerobacterium saccharolyticum, mutation of the phosphoenolpyruvate carboxykinase and deletion of malic enzyme gene. Strain YD01 with exogenous pyruvate kinase, in which phosphoenolpyruvate carboxykinase expression was diminished by modifying the start codon from ATG to GTG, exhibited 3.25-fold higher ethanol yield than the wild-type strain. A second strain, YD02 with exogenous pyruvate kinase, in which the gene for malic enzyme and part of malate dehydrogenase were deleted, had over 3-fold higher ethanol yield than the wild-type strain. (C) 2012 Elsevier Inc. All rights reserved. C1 [Deng, Yu; Olson, Daniel G.; Zhou, Jilai; Herring, Christopher D.; Lynd, Lee R.] Dartmouth Coll, Thayer Sch Engn, Hanover, NH 03755 USA. [Herring, Christopher D.; Lynd, Lee R.] Mascoma Corp, Lebanon, NH 03766 USA. [Deng, Yu; Olson, Daniel G.; Zhou, Jilai; Herring, Christopher D.; Lynd, Lee R.] BioEnergy Sci Ctr, Oak Ridge, TN 37830 USA. [Shaw, A. Joe] Novogy Inc, Cambridge, MA 02138 USA. RP Lynd, LR (reprint author), Dartmouth Coll, Thayer Sch Engn Dartmouth, Engn Dr,8000 Cummings Hall, Hanover, NH 03755 USA. EM Lee.Lynd@Dartmouth.edu RI Lynd, Lee/N-1260-2013; Olson, Daniel/F-2058-2011 OI Lynd, Lee/0000-0002-5642-668X; Olson, Daniel/0000-0001-5393-6302 FU BioEnergy Science Center (BESC), a U.S. Department of Energy (DOE) Research Center; Office of Biological and Environmental Research in the DOE Office of Science; Mascoma Corporation FX The authors are grateful for the support provided by funding grants from the BioEnergy Science Center (BESC), a U.S. Department of Energy (DOE) Research Center supported by the Office of Biological and Environmental Research in the DOE Office of Science and Mascoma Corporation. NR 36 TC 34 Z9 35 U1 0 U2 39 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 1096-7176 J9 METAB ENG JI Metab. Eng. PD JAN PY 2013 VL 15 BP 151 EP 158 DI 10.1016/j.ymben.2012.11.006 PG 8 WC Biotechnology & Applied Microbiology SC Biotechnology & Applied Microbiology GA 075JW UT WOS:000313882500015 PM 23202749 ER PT J AU Ozaydin, B Burd, H Lee, TS Keasling, JD AF Oezaydin, Bilge Burd, Helcio Lee, Taek Soon Keasling, Jay D. TI Carotenoid-based phenotypic screen of the yeast deletion collection reveals new genes with roles in isoprenoid production SO METABOLIC ENGINEERING LA English DT Article DE Isoprenoids; S. cerevisiae; Carotenoids; Biofuel; Bisabolene ID SACCHAROMYCES-CEREVISIAE STRAINS; HIGH-LEVEL PRODUCTION; COENZYME-A REDUCTASE; ESCHERICHIA-COLI; MEVALONATE PATHWAY; BETA-CAROTENE; PRECURSOR; OVERPRODUCTION; EXTRACTION; GENOME AB Beside their essential cellular functions, isoprenoids have value as pharmaceuticals, nutriceuticals, pesticides, and fuel alternatives. Engineering microorganisms for production of isoprenoids is relatively easy, sustainable, and cost effective in comparison to chemical synthesis or extraction from natural producers. We introduced genes encoding carotenoid biosynthetic enzymes into the haploid yeast deletion collection to identify gene deletions that improved isoprenoid production. Deletions that showed significant improvement in carotenoid production were further screened for production of bisabolene, an isoprenoid alternative to petroleum-derived diesel. Combining those deletions with other mevalonate pathway modifications increased production of bisabolene from 40 mg/L to 800 mg/L in shake-flask cultures. In a fermentation process, this engineered strain produced 5.2 g/L of bisabolene. (C) 2012 Published by Elsevier Inc. C1 [Oezaydin, Bilge; Burd, Helcio; Lee, Taek Soon; Keasling, Jay D.] Joint BioEnergy Inst, Oakland, CA 94608 USA. [Oezaydin, Bilge; Burd, Helcio; Lee, Taek Soon; Keasling, Jay D.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA 94720 USA. [Keasling, Jay D.] Univ Calif Berkeley, Dept Chem & Biomol Engn, Berkeley, CA 94720 USA. [Keasling, Jay D.] Univ Calif Berkeley, Dept Bioengn, Berkeley, CA 94720 USA. RP Keasling, JD (reprint author), Univ Calif Berkeley, Dept Chem & Biomol Engn, Berkeley, CA 94720 USA. EM jdkeasling@lbl.gov RI Keasling, Jay/J-9162-2012 OI Keasling, Jay/0000-0003-4170-6088 FU U. S. Department of Energy, Office of Science, Office of Biological and Environmental Research [DE-AC02-05CH11231] FX We thank Nathan Hillson, Dwight Kuo, and Lane Weaver for helpful discussions and thoughtful comments on the manuscript. This work was part of the DOE Joint BioEnergy Institute (http://www.jbei.org) supported by the U. S. Department of Energy, Office of Science, Office of Biological and Environmental Research, through contract DE-AC02-05CH11231 between Lawrence Berkeley National Laboratory and the U.S. Department of Energy. NR 52 TC 28 Z9 31 U1 3 U2 59 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 1096-7176 J9 METAB ENG JI Metab. Eng. PD JAN PY 2013 VL 15 BP 174 EP 183 DI 10.1016/j.ymben.2012.07.010 PG 10 WC Biotechnology & Applied Microbiology SC Biotechnology & Applied Microbiology GA 075JW UT WOS:000313882500018 PM 22918085 ER PT J AU Barabash, RI Wang, XL Korstorz, G Fultz, B Levine, L Liaw, PK AF Barabash, R. I. Wang, Xun-Li Korstorz, G. Fultz, Brent Levine, Lyle Liaw, P. K. TI Neutron and X-Ray Studies of Advanced Materials V-Diffraction Centennial Foreword SO METALLURGICAL AND MATERIALS TRANSACTIONS A-PHYSICAL METALLURGY AND MATERIALS SCIENCE LA English DT Editorial Material C1 [Barabash, R. I.] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. [Wang, Xun-Li] City Univ Hong Kong, Kowloon, Hong Kong, Peoples R China. [Korstorz, G.] Swiss Fed Inst Technol, Zurich, Switzerland. [Fultz, Brent] CALTECH, Pasadena, CA 91125 USA. [Levine, Lyle] NIST, Gaithersburg, MD 20899 USA. [Liaw, P. K.] Univ Tennessee, Knoxville, TN USA. RP Barabash, RI (reprint author), Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. RI Wang, Xun-Li/C-9636-2010 OI Wang, Xun-Li/0000-0003-4060-8777 NR 0 TC 0 Z9 0 U1 0 U2 18 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1073-5623 J9 METALL MATER TRANS A JI Metall. Mater. Trans. A-Phys. Metall. Mater. Sci. PD JAN PY 2013 VL 44A IS 1 BP 15 EP 16 PG 2 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Materials Science; Metallurgy & Metallurgical Engineering GA 073BO UT WOS:000313718500004 ER PT J AU Fuller, MS Barabash, R Mcintyre, S Ramamurthy, S Liu, WJ AF Fuller, Marina Suominen Barabash, Rozaliya Mcintyre, Stewart Ramamurthy, Sridhar Liu, Wenjun TI Assessment of Plastic Deformation Induced by Indentation on a Large Grain on Inconel 600 Using Synchrotron Polychromatic X-ray Microdiffraction SO METALLURGICAL AND MATERIALS TRANSACTIONS A-PHYSICAL METALLURGY AND MATERIALS SCIENCE LA English DT Article ID TRANSMISSION ELECTRON-MICROSCOPY; STRUCTURAL MICROSCOPY; DISLOCATIONS; CRYSTALS AB A synchrotron-based three-dimensional (3-D) Laue technique called Differential Aperture X-ray microscopy (DAXM) was used to investigate plastic deformation of Inconel 600 induced by indentation. The DAXM technique is capable of probing up to 60 to 100 mu m into the Ni alloy, with micron resolution. A conical indenter was used to generate an indent on a large surface grain on Inconel 600. The DAXM Laue images from the uppermost grain exhibited pronounced streaking and splitting of Laue spots, which increased as the grain boundary was approached. Splitting of the Laue patterns correlates with subgrain or dislocation cell formation. A significant amount of dislocation cell formation was found within the 1-mu m voxels probed by DAXM. A change in total angle of 8.79 deg was determined for the uppermost grain from the diffraction data from depths 4 to 28 mu m, with an average misorientation angle of 2.15 deg between the dislocation cells. The next grain having a different crystallographic orientation continued to rotate in the same direction as the uppermost grain due to the large plastic deformation. DOI: 10.1007/s11661-012-1219-0 (C) The Minerals, Metals & Materials Society and ASM International 2012 C1 [Fuller, Marina Suominen; Mcintyre, Stewart] Univ Western Ontario, Dept Chem, London, ON N6A 5B7, Canada. [Liu, Wenjun] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. EM msuomine@alumni.uwo.ca FU United States Department of Energy, Office of Science, Office of Basic Energy Sciences [W-31-109-ENG-38]; United States Department of Energy, Office of Basic Energy Sciences, Materials Sciences and Engineering Division; Babcock & Wilcox Canada (BWC); Centre for Materials and Manufacturing Ontario FX Use of the Advanced Photon Source (APS) was supported by the United States Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. W-31-109-ENG-38. One of the authors (RB) is supported by the United States Department of Energy, Office of Basic Energy Sciences, Materials Sciences and Engineering Division. The authors gratefully acknowledge the funding contributions from Babcock & Wilcox Canada (BWC) and the Centre for Materials and Manufacturing Ontario. The authors also thank Mr. H. Wang, Professor Robert Klassen, and Mr. Ariful Islam, Department of Materials Engineering, University of Western Ontario, for the metallographic preparation, and Mr. Edward Lehockey, Ontario Power Generation, for many useful discussions. NR 18 TC 1 Z9 1 U1 3 U2 14 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1073-5623 J9 METALL MATER TRANS A JI Metall. Mater. Trans. A-Phys. Metall. Mater. Sci. PD JAN PY 2013 VL 44A IS 1 BP 17 EP 21 DI 10.1007/s11661-012-1219-0 PG 5 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Materials Science; Metallurgy & Metallurgical Engineering GA 073BO UT WOS:000313718500005 ER PT J AU Meng, J Wang, XL Chou, KC Li, Q AF Meng, Jie Wang, Xun-Li Chou, Kuo-Chih Li, Qian TI Hydrogen Storage Properties of Graphite-Modified Mg-Ni-Ce Composites Prepared by Mechanical Milling Followed by Microwave Sintering SO METALLURGICAL AND MATERIALS TRANSACTIONS A-PHYSICAL METALLURGY AND MATERIALS SCIENCE LA English DT Article ID ABSORPTION; KINETICS; MAGNESIUM; SYSTEM; ALLOY; DESORPTION; CARBIDE; ENERGY; MODEL AB The Mg17Ni1.5Ce0.5 hydrogen storage composites with different contents of graphite were prepared by a new method of mechanical milling and subsequent microwave sintering. The small particle size (similar to 25 mu m) and the low echo ratio of power indicate that graphite plays an important role not only as a lubricant during mechanical milling but also as a supplementary heating material during microwave sintering. As a catalyst in the hydriding/dehydriding (H/D) reaction, graphite also improved the hydrogen storage properties of the composites. The hydrogen absorption and desorption capacities of Mg17Ni1.5Ce0.5 with 5 wt pct graphite were 5.34 and 5.30 wt pct H-2 at 573 K (300 degrees C), its onset temperature of dehydriding reaction was 511 K (238 degrees C), and its activation energies of H/D reaction were 40.9 and 54.5 kJ/mol H-2, respectively. The kinetic mechanisms of the H/D reaction are also discussed. DOI: 10.1007/s11661-012-1301-7 (C) The Minerals, Metals & Materials Society and ASM International 2012 C1 [Chou, Kuo-Chih; Li, Qian] Shanghai Univ, Shanghai Key Lab Modern Met & Mat Proc, Shanghai 200072, Peoples R China. [Li, Qian] Oak Ridge Natl Lab, Neutron Scattering Sci Div, Oak Ridge, TN 37831 USA. EM shuliqian@shu.edu.cn RI Li, Qian/A-8752-2015; OI Wang, Xun-Li/0000-0003-4060-8777 FU Shanghai Rising-Star Program [11QH1400900] FX The authors thank the staff at the Instrumental Analysis and Research Center (Shanghai University) for their support of the materials testing and research. This work was financially sponsored by the Shanghai Rising-Star Program (Grant No. 11QH1400900), and QL is currently supported, in part, by an appointment of the United States Department of Energy Higher Education Research Experience Program at Oak Ridge National Laboratory, administered by the Oak Ridge Institute for Science and Education. NR 36 TC 1 Z9 1 U1 1 U2 29 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1073-5623 J9 METALL MATER TRANS A JI Metall. Mater. Trans. A-Phys. Metall. Mater. Sci. PD JAN PY 2013 VL 44A IS 1 BP 58 EP 67 DI 10.1007/s11661-012-1301-7 PG 10 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Materials Science; Metallurgy & Metallurgical Engineering GA 073BO UT WOS:000313718500010 ER PT J AU Ilavsky, J Zhang, F Allen, AJ Levine, LE Jemian, PR Long, GG AF Ilavsky, J. Zhang, F. Allen, A. J. Levine, L. E. Jemian, P. R. Long, G. G. TI Ultra-Small-Angle X-ray Scattering Instrument at the Advanced Photon Source: History, Recent Development, and Current Status SO METALLURGICAL AND MATERIALS TRANSACTIONS A-PHYSICAL METALLURGY AND MATERIALS SCIENCE LA English DT Article ID THERMAL BARRIER COATINGS; IN-SITU; CORRELATION SPECTROSCOPY; YSZ DEPOSITS; MICROSTRUCTURE; POLYETHYLENE; COMPOSITES; PARAMETERS; SUSPENSION; EVOLUTION AB The 25-year history and development of an ultra-small-angle X-ray scattering (USAXS) instrument dedicated to serving materials research is presented and discussed. The instrument's successful track record is attributed to three factors. The first, and surely the most important, is that all development has been driven by scientific research directions and opportunities. Second, the USAXS instrument is a core capability rather than an add-on facility, with measurement capability from micrometers to nanometers, which is precisely the size range where microstructures determine physical properties. The third is that the instrument's range of capabilities has continually expanded, now including 2D collimation, imaging, and dynamics. And finally, USAXS has enjoyed the benefit of a management structure that has consistently appreciated the unique experimental measurement capabilities that USAXS delivers. DOI: 10.1007/s11661-012-1431-y (C) The Minerals, Metals & Materials Society and ASM International 2012 C1 [Ilavsky, J.; Long, G. G.] Argonne Natl Lab, Xray Sci Div, Argonne, IL 60439 USA. [Zhang, F.; Allen, A. J.; Levine, L. E.; Long, G. G.] NIST, Mat Measurement Lab, Gaithersburg, MD 20899 USA. [Zhang, F.] No Illinois Univ, Dept Phys, De Kalb, IL 60115 USA. [Jemian, P. R.] Argonne Natl Lab, APS Engn Support Div, Argonne, IL 60439 USA. RP Ilavsky, J (reprint author), Argonne Natl Lab, Xray Sci Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM ilavsky@aps.anl.gov RI Ilavsky, Jan/D-4521-2013; USAXS, APS/D-4198-2013 OI Ilavsky, Jan/0000-0003-1982-8900; FU U.S. Department of Energy (DoE) [DE-AC02-98CH10886]; U.S. DOE [DEAC02-06CH11357]; National Science Foundation/Department of Energy [NSF/CHE-0822838] FX The critical support and advice in the early years from Professors Julia R. Weertman and the late Jerry B. Cohen, both of Northwestern University, are gratefully acknowledged, as well as the help and discussions with John G. Barker of Northwestern University (now at NIST) and David R. Black and Richard D. Spal of NIST. The authors thank NSLS at Brookhaven National Lab. for hosting the USAXS instrument at sector X23 until 1999. At the APS, the former UNICAT consortium members, Oak Ridge National Lab., the University of Illinois at Urbana-Champagne, and UOP LLC., are thanked for welcoming NIST to UNICAT and hosting the USAXS instrument at sector 33-ID from 1999 until 2006. The APS X-ray Science Division (XSD) is thanked for hosting the USAXS instrument at sector 32-ID from 2006 until 2010. The hosting of the USAXS instrument at APS sector 15-ID from 2010 to the present day by XSD, in partnership with the University of Chicago's ChemMatCARS, is gratefully acknowledged. The authors thank the beamline and facility staff, and our many users and collaborators who have contributed to the success of the USAXS instrument over its 25-year history. The use ofthe NSLS was supported by the U.S. Department of Energy (DoE) under contract no. DE-AC02-98CH10886. The 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, is supported by the U.S. DOE under Contract No. DEAC02-06CH11357. ChemMatCARS Sector 15 is principally supported by the National Science Foundation/Department of Energy under grant number NSF/CHE-0822838. NR 48 TC 26 Z9 26 U1 3 U2 35 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1073-5623 J9 METALL MATER TRANS A JI Metall. Mater. Trans. A-Phys. Metall. Mater. Sci. PD JAN PY 2013 VL 44A IS 1 BP 68 EP 76 DI 10.1007/s11661-012-1431-y PG 9 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Materials Science; Metallurgy & Metallurgical Engineering GA 073BO UT WOS:000313718500011 ER PT J AU Nibur, KA Somerday, BP Marchi, CS Foulk, JW Dadfarnia, M Sofronis, P AF Nibur, Kevin A. Somerday, Brian P. Marchi, Chris San Foulk, James W., III Dadfarnia, Mohsen Sofronis, Petros TI The Relationship Between Crack-Tip Strain and Subcritical Cracking Thresholds for Steels in High-Pressure Hydrogen Gas SO METALLURGICAL AND MATERIALS TRANSACTIONS A-PHYSICAL METALLURGY AND MATERIALS SCIENCE LA English DT Article ID HIGH-STRENGTH STEELS; STRESS-CORROSION CRACKING; ROOM-TEMPERATURE CREEP; VESSEL STEELS; HARDENING MATERIAL; INDUCED FRACTURE; STAINLESS-STEEL; TITANIUM-ALLOYS; QUASI-CLEAVAGE; PLASTIC SOLIDS AB Threshold stress intensity factors were measured in high-pressure hydrogen gas for a variety of low alloy ferritic steels using both constant crack opening displacement and rising crack opening displacement procedures. Thresholds for crack extension under rising displacement, K-THi, for crack extension under constant displacement, K-THi*, and for crack arrest under constant displacement K-THa, were identified. These values were not found to be equivalent, i.e. K-THi < K-THa < K-THi*. The hydrogen assisted fracture mechanism was determined to be strain controlled for all of the alloys in this study, and the micromechanics of strain controlled fracture are used to explain the observed disparities between the different threshold measurements. K-THa and K-THi differ because the strain singularity of a stationary crack is stronger than that of a propagating crack; K-THa must be larger than K-THi to achieve equivalent crack tip strain at the same distance from the crack tip. Hydrogen interacts with deformation mechanisms, enhancing strain localization and consequently altering both the nucleation and growth stages of strain controlled fracture mechanisms. The timing of load application and hydrogen exposure, i.e., sequential for constant displacement tests and concurrent for rising displacement tests, leads to differences in the strain history relative to the environmental exposure history and promotes the disparity between K-THi* and K-THi. K-THi is the only conservative measurement of fracture threshold among the methods presented here. DOI: 10.1007/s11661-012-1400-5 (C) The Minerals, Metals & Materials Society and ASM International 2012 C1 [Nibur, Kevin A.] Hy Performance Mat Testing LLC, Bend, OR USA. [Somerday, Brian P.; Marchi, Chris San] Sandia Natl Labs, Hydrogen & Met Sci Dept, Livermore, CA 94551 USA. [Somerday, Brian P.] Kyushu Univ, Int Inst Carbon Neutral Energy Res WPI I2CNER, Nishi Ku, Fukuoka 8190395, Japan. [Foulk, James W., III] Sandia Natl Labs, Mech Mat Dept, Livermore, CA 94550 USA. [Dadfarnia, Mohsen; Sofronis, Petros] Univ Illinois, Dept Mech Sci & Engn, Urbana, IL 61801 USA. RP Nibur, KA (reprint author), Hy Performance Mat Testing LLC, Bend, OR USA. EM Kevin@hy-performancetesting.com RI U-ID, Kyushu/C-5291-2016; OI Dadfarnia, Mohsen/0000-0002-5218-971X; San Marchi, Christopher/0000-0002-0862-8607 FU U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000]; US Department of Energy Fuel Cell Technologies program through the Safety, Codes and Standards sub-program element; US Department of Energy [GO15045] 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. The experimental work presented here has been supported by the US Department of Energy Fuel Cell Technologies program through the Safety, Codes and Standards sub-program element. PS and MD were supported by the US Department of Energy under Grant GO15045. The assistance of Ken Lee and Jeff Campbell in the experimental work as well as Andy Gardea, Jeff Chames and Ryan Nishimoto in metallography and microscopy is gratefully acknowledged. The authors additionally thank Gary Hayden (CP Industries) and John Felbaum (Fiba Technologies) for providing technologically relevant steels for testing. NR 88 TC 9 Z9 9 U1 2 U2 20 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1073-5623 J9 METALL MATER TRANS A JI Metall. Mater. Trans. A-Phys. Metall. Mater. Sci. PD JAN PY 2013 VL 44A IS 1 BP 248 EP 269 DI 10.1007/s11661-012-1400-5 PG 22 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Materials Science; Metallurgy & Metallurgical Engineering GA 073BO UT WOS:000313718500028 ER PT J AU Perez, E Sohn, YH Keiser, DD AF Perez, Emmanuel Sohn, Yong-Ho Keiser, Dennis D., Jr. TI Role of Si on the Diffusional Interactions Between U-Mo and Al-Si Alloys at 823 K (550 degrees C) SO METALLURGICAL AND MATERIALS TRANSACTIONS A-PHYSICAL METALLURGY AND MATERIALS SCIENCE LA English DT Article ID URANIUM-MOLYBDENUM ALLOYS; MO/AL DISPERSION FUEL; TRANSMISSION ELECTRON-MICROSCOPY; NUCLEAR-RESEARCH REACTORS; HEAVY-ION IRRADIATION; X-RAY-DIFFRACTION; GAMMA-PHASE; WT.PERCENT-MO; HIGH-DENSITY; THERMAL COMPATIBILITY AB U-Mo dispersions in Al-alloy matrix and monolithic fuels encased in Al-alloy are under development to fulfill the requirements for research and test reactors to use low-enriched molybdenum stabilized uranium alloy fuels. Significant interaction takes place between the U-Mo fuel and Al during manufacturing and in-reactor irradiation. The interaction products are Al-rich phases with physical and thermal characteristics that adversely affect fuel performance and result in premature failure. Detailed analysis of the interdiffusion and microstructural development of this system was carried through diffusion couples consisting of U-7 wt pct Mo, U-10 wt pct Mo and U-12 wt pct Mo in contact with pure Al, Al-2 wt pct Si, and Al-5 wt pct Si, annealed at 823 K (550 degrees C) for 1, 5 and 20 hours. Scanning electron microscopy and transmission electron microscopy were employed for the analysis. Diffusion couples consisting of U-Mo in contact with pure Al contained UAl3, UAl4, U6Mo4Al43, and UMo2Al20 phases. Additions of Si to the Al significantly reduced the thickness of the interdiffusion zone. The interdiffusion zones developed Al- and Si-enriched regions, whose locations and size depended on the Si and Mo concentrations in the terminal alloys. In these couples, the (U, Mo)(Al, Si) 3 phase was observed throughout the interdiffusion zone, and the U6Mo4Al43 and UMo2Al20 phases were observed only where the Si concentrations were low. DOI: 10.1007/s11661-012-1368-1 (C) The Minerals, Metals & Materials Society and ASM International 2012 C1 [Perez, Emmanuel; Keiser, Dennis D., Jr.] Idaho Natl Lab, Idaho Falls, ID 83415 USA. [Sohn, Yong-Ho] Univ Cent Florida, Dept Mech Mat & Aerosp Engn, Adv Mat Proc & Anal Ctr, Orlando, FL 32816 USA. RP Perez, E (reprint author), Idaho Natl Lab, POB 1625, Idaho Falls, ID 83415 USA. EM Emmanuel.Perez@inl.gov RI Sohn, Yongho/A-8517-2010 OI Sohn, Yongho/0000-0003-3723-4743 FU U.S. Department of Energy; U.S. Government under DOE-NE Idaho Operations Office [DE-AC07-05ID14517, 00051953]; U.S. Government FX The work described in this manuscript was supported by the U.S. Department of Energy and was authored by a contractor of the U.S. Government under DOE-NE Idaho Operations Office Contract DE-AC07-05ID14517 through a subcontract No. 00051953 administered by Battelle Energy Alliances, LLC and Idaho National Laboratory. Accordingly, the U.S. Government retains and the publisher, by accepting the article for publication, acknowledges that the U.S. Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for U.S. Government purposes. This information was prepared as an account of work sponsored by an agency of the U.S. Government. Neither the U.S. Government nor any agency thereof, nor any of their employees, makes any warranty, express or implied, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. References herein to any specific commercial product, process, or service by trade name, trademark, manufacturer, or otherwise, does not necessarily constitute or imply its endorsement, recommendation, or favoring by the U.S. Government or any agency thereof. The views and opinions of authors expressed herein do not necessarily state or reflect those of the U. S. Government or any agency thereof. NR 94 TC 9 Z9 9 U1 2 U2 14 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1073-5623 EI 1543-1940 J9 METALL MATER TRANS A JI Metall. Mater. Trans. A-Phys. Metall. Mater. Sci. PD JAN PY 2013 VL 44A IS 1 BP 584 EP 595 DI 10.1007/s11661-012-1368-1 PG 12 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Materials Science; Metallurgy & Metallurgical Engineering GA 073BO UT WOS:000313718500058 ER PT J AU Walavalkar, SS Homyk, AP Henry, MD Scherer, A AF Walavalkar, Sameer S. Homyk, Andrew P. Henry, M. David Scherer, Axel TI Three-dimensional etching of silicon for the fabrication of low-dimensional and suspended devices SO NANOSCALE LA English DT Article ID TEMPERATURES; NANOWIRES; EMISSION AB In order to expand the use of nanoscaled silicon structures we present a new etching method that allows us to shape silicon with sub-10 nm precision. This top-down, CMOS compatible etching scheme allows us to fabricate silicon devices with quantum behavior without relying on difficult lateral lithography. We utilize this novel etching process to create quantum dots, quantum wires, vertical transistors and ultra-high-aspect ratio structures. We believe that this etching technique will have broad and significant impacts and applications in nano-photonics, bio-sensing, and nano-electronics. C1 [Walavalkar, Sameer S.; Homyk, Andrew P.; Scherer, Axel] CALTECH, Kavli Nanosci Inst, Pasadena, CA 91125 USA. [Henry, M. David] Sandia Natl Labs, MESA Facil, Albuquerque, NM 87185 USA. RP Walavalkar, SS (reprint author), CALTECH, Kavli Nanosci Inst, 1200 E Calif Blvd,MC 200-36, Pasadena, CA 91125 USA. EM walavalk@caltech.edu RI Walavalkar, Sameer/B-3196-2013 OI Walavalkar, Sameer/0000-0002-7628-9600 FU Advanced Energy Commission [BEG10-07]; Boeing corporation [CT-BA-GTA-1]; National Science Foundation under NSF CIAN ERC [EEC-0812072] FX This work was supported by the Advanced Energy Commission under the BEG10-07 grant, the Boeing corporation under the CT-BA-GTA-1 grant, and by the National Science Foundation under NSF CIAN ERC (EEC-0812072). S. W. would like to thank T.K. Nelson for useful discussion and A. H. appreciates the generous support of the ARCS Foundation. The authors would like to additionally thank the staff of the Kavli Nanoscience Institute for their continued help. NR 16 TC 4 Z9 4 U1 1 U2 31 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2040-3364 J9 NANOSCALE JI Nanoscale PY 2013 VL 5 IS 3 BP 927 EP 931 DI 10.1039/c2nr32981f PG 5 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA 074HH UT WOS:000313803000015 PM 23292113 ER PT J AU Zhao, YT Zhang, WY Lin, YH Du, D AF Zhao, Yuting Zhang, Weiying Lin, Yuehe Du, Dan TI The vital function of Fe3O4@Au nanocomposites for hydrolase biosensor design and its application in detection of methyl parathion SO NANOSCALE LA English DT Article ID SELF-ASSEMBLED MONOLAYER; GOLD NANOPARTICLES; ORGANOPHOSPHORUS PESTICIDES; NERVE AGENTS; ACETYLCHOLINESTERASE; IMMOBILIZATION; SPECTROSCOPY; EXPOSURE AB A nanocomposite of gold nanoparticles (AuNPs) decorating a magnetic Fe3O4 core was synthesized using cysteamine (SH-NH2) as linker, and characterized by TEM, XPS, UV and electrochemistry. Then a hydrolase biosensor, based on self-assembly of methyl parathion hydrolase (MPH) on the Fe3O4@Au nanocomposite, was developed for sensitive and selective detection of the organophosphorus pesticide (OP) methyl parathion. The magnetic nanocomposite provides an easy way to construct the enzyme biosensor by simply exerting an external magnetic field, and also provides a simple way to renew the electrode surface by removing the magnet. Unlike inhibition-based enzyme biosensors, the hydrolase is not poisoned by OPs and thus is reusable for continuous measurement. AuNPs not only provide a large surface area, high loading efficiency and fast electron transfer, but also stabilize the enzyme through electrostatic interactions. The MPH biosensor shows rapid response and high selectivity for detection of methyl parathion, with a linear range from 0.5 to 1000 ng mL(-1) and a detection limit of 0.1 ng mL(-1). It also shows acceptable reproducibility and stability. The simplicity and ease of operation of the proposed method has great potential for on-site detection of P-S containing pesticides and provides a promising strategy to construct a robust biosensor. C1 [Zhao, Yuting; Du, Dan] Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China. [Zhang, Weiying; Lin, Yuehe] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Du, D (reprint author), Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China. EM dudan@mail.ccnu.edu.cn RI Lin, Yuehe/D-9762-2011; Du, Dan (Annie)/G-3821-2012 OI Lin, Yuehe/0000-0003-3791-7587; FU National Natural Science Foundation of China [21275062, 21075047]; self-determined research funds of CCNU from the colleges' basic research and operation of MOE [CCNU11C01002]; CounterACT Program, Office of the Director, National Institutes of Health (OD); National Institute of Neurological Disorders and Stroke (NINDS) [U01 NS058161-01]; US-DOE [DE-AC05-76RL01830] FX This work was supported by the National Natural Science Foundation of China (21275062, 21075047) and the self-determined research funds of CCNU from the colleges' basic research and operation of MOE (CCNU11C01002). Y. Lin acknowledges the financial support by the CounterACT Program, Office of the Director, National Institutes of Health (OD) and the National Institute of Neurological Disorders and Stroke (NINDS), grant number U01 NS058161-01. The contents of this publication are solely the responsibility of the authors and do not necessarily represent the official views of the NIH. Pacific Northwest National Laboratory is operated by Battelle for US-DOE under Contract DE-AC05-76RL01830. We specially thank Prof. Deli Liu in Central China Normal University for providing MPH. NR 32 TC 32 Z9 33 U1 11 U2 156 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2040-3364 J9 NANOSCALE JI Nanoscale PY 2013 VL 5 IS 3 BP 1121 EP 1126 DI 10.1039/c2nr33107a PG 6 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA 074HH UT WOS:000313803000040 PM 23280070 ER PT J AU Peters, GP Andrew, RM Boden, T Canadell, JG Ciais, P Le Quere, C Marland, G Raupach, MR Wilson, C AF Peters, Glen P. Andrew, Robbie M. Boden, Tom Canadell, Josep G. Ciais, Philippe Le Quere, Corinne Marland, Gregg Raupach, Michael R. Wilson, Charlie TI COMMENTARY: The challenge to keep global warming below 2 degrees C SO NATURE CLIMATE CHANGE LA English DT Editorial Material ID CO2 EMISSIONS; CLIMATE; SCENARIOS; GROWTH C1 [Peters, Glen P.; Andrew, Robbie M.] CICERO, N-0550 Oslo, Norway. [Boden, Tom] Oak Ridge Natl Lab, CDIAC, Oak Ridge, TN 37831 USA. [Canadell, Josep G.; Raupach, Michael R.] CSIRO Marine & Atmospher Res, Global Carbon Project, Canberra, ACT, Australia. [Ciais, Philippe] CAE CNRS UVSQ, Lab Sci Climat & Environm, F-91191 Gif Sur Yvette, France. [Le Quere, Corinne; Wilson, Charlie] Univ E Anglia, Tyndall Ctr Climate Change Res, Norwich NR4 7TJ, Norfolk, England. [Marland, Gregg] Appalachian State Univ, Inst Environm Energy & Econ, Boone, NC 28608 USA. RP Peters, GP (reprint author), CICERO, POB 1128, N-0550 Oslo, Norway. EM glen.peters@cicero.uio.no RI Peters, Glen/B-1012-2008; Canadell, Josep/E-9419-2010; Le Quere, Corinne/C-2631-2017 OI Peters, Glen/0000-0001-7889-8568; Canadell, Josep/0000-0002-8788-3218; Le Quere, Corinne/0000-0003-2319-0452 NR 24 TC 224 Z9 232 U1 17 U2 178 PU NATURE PUBLISHING GROUP PI LONDON PA MACMILLAN BUILDING, 4 CRINAN ST, LONDON N1 9XW, ENGLAND SN 1758-678X EI 1758-6798 J9 NAT CLIM CHANGE JI Nat. Clim. Chang. PD JAN PY 2013 VL 3 IS 1 BP 4 EP 6 PG 3 WC Environmental Sciences; Environmental Studies; Meteorology & Atmospheric Sciences SC Environmental Sciences & Ecology; Meteorology & Atmospheric Sciences GA 076ZZ UT WOS:000313999000005 ER PT J AU Oh, CH Kim, ES AF Oh, Chang H. Kim, Eung Soo TI ISOTHERMAL AIR-INGRESS VALIDATION EXPERIMENTS SO NUCLEAR TECHNOLOGY LA English DT Article; Proceedings Paper CT 14th International Topical Meeting on Nuclear Reactor Thermal Hydraulics (NURETH) CY SEP 25-30, 2011 CL Toronto, CANADA SP Canadian Nucl Soc, Amer Nucl Soc, Thermal Hydraul Div, Int Atom Energy Agcy, Nucl Energy Agcy, Org Econ Co-Operat & Dev DE VHTR; air ingress; stratified flow AB Idaho National Laboratory has conducted air-ingress experiments as part of a campaign to validate computational fluid dynamics (CFD) calculations for very high-temperature gas-cooled reactor (VHTR) analysis. An isothermal test loop was designed to recreate exchange or stratified flow that occurs in the lower plenum of VHTR after a break in the primary loop allows helium to leak out and reactor building air to enter the reactor core. The experiment was designed to measure stratified flow in the inlet pipe connecting to the lower plenum of the General Atomics gas turbine modular helium reactor (GT-MHR). Instead of helium and air, brine and sucrose were used as heavy fluids, and water was used as the lighter fluid to create, using scaling laws, the appropriate flow characteristics of the lower plenum immediately after depressurization. These results clearly indicate that stratified flow is established even for very small density differences. Corresponding CFD results were validated with the experimental data. A grid sensitivity study on CFD models was also performed using the Richardson extrapolation and the grid convergence index method for the numerical accuracy of CFD calculations. The calculated current speed showed very good agreement with the experimental data, indicating that current CFD methods are suitable for simulating density gradient stratified flow phenomena in an air-ingress accident. C1 [Oh, Chang H.] Idaho Natl Lab, Idaho Falls, ID 83415 USA. [Kim, Eung Soo] Seoul Natl Univ, Dept Nucl Engn, Seoul, South Korea. RP Oh, CH (reprint author), Idaho Natl Lab, POB 16125, Idaho Falls, ID 83415 USA. EM Chang.Oh@inl.gov NR 9 TC 0 Z9 0 U1 0 U2 1 PU AMER NUCLEAR SOC PI LA GRANGE PK PA 555 N KENSINGTON AVE, LA GRANGE PK, IL 60526 USA SN 0029-5450 J9 NUCL TECHNOL JI Nucl. Technol. PD JAN PY 2013 VL 181 IS 1 SI SI BP 68 EP 80 PG 13 WC Nuclear Science & Technology SC Nuclear Science & Technology GA 063CN UT WOS:000312973800007 ER PT J AU Pellegrini, M Endo, H Merzari, E Ninokata, H AF Pellegrini, M. Endo, H. Merzari, E. Ninokata, H. TI ALGEBRAIC TURBULENT HEAT FLUX MODEL FOR PREDICTION OF THERMAL STRATIFICATION IN PIPING SYSTEMS SO NUCLEAR TECHNOLOGY LA English DT Article; Proceedings Paper CT 14th International Topical Meeting on Nuclear Reactor Thermal Hydraulics (NURETH) CY SEP 25-30, 2011 CL Toronto, CANADA SP Canadian Nucl Soc, Amer Nucl Soc, Thermal Hydraul Div, Int Atom Energy Agcy, Nucl Energy Agcy, Org Econ Co-Operat & Dev DE thermal stratification; CFD; algebraic heat flux model ID PIPE-FLOW; BUOYANCY; FLUIDS AB The effect of stratification on the flow in bounded geometries is studied through computational fluid dynamics and two different modelings of the turbulent heat flux: constant turbulent Prandtl number and Algebraic Heat Flux Model (AHFM). The main feature of the work is evaluation of the effect of buoyancy on the thermal quantities, velocity field, and related pressure drop. For evaluation of the turbulent heat flux and temperature field, AHFM has been demonstrated to be superior to the simple eddy diffusivity approach. However, serious concerns remain for the prediction of the velocity field in both isothermal and nonisothermal conditions, since greater uncertainties for the obtained pressure drop and related Fanning friction factor can be introduced. Incremental pressure drop is also investigated in conditions deviating from fully developed flows, in order to study stratification effects qualitatively using an engineering method. C1 [Pellegrini, M.; Ninokata, H.] Tokyo Inst Technol, Dept Nucl Engn, Tokyo 152, Japan. [Endo, H.] Japan Nucl Energy & Safety Org, Tokyo, Japan. [Merzari, E.] Argonne Natl Lab, Nucl Engn Div, Argonne, IL 60439 USA. RP Pellegrini, M (reprint author), Tokyo Inst Technol, Dept Nucl Engn, Tokyo 152, Japan. EM mpellegrini@iae.or.jp NR 26 TC 0 Z9 0 U1 0 U2 5 PU AMER NUCLEAR SOC PI LA GRANGE PK PA 555 N KENSINGTON AVE, LA GRANGE PK, IL 60526 USA SN 0029-5450 EI 1943-7471 J9 NUCL TECHNOL JI Nucl. Technol. PD JAN PY 2013 VL 181 IS 1 SI SI BP 144 EP 156 PG 13 WC Nuclear Science & Technology SC Nuclear Science & Technology GA 063CN UT WOS:000312973800013 ER PT J AU Zhao, HH Mousseau, VA AF Zhao, Haihua Mousseau, Vincent A. TI EXTENDED FORWARD SENSITIVITY ANALYSIS FOR UNCERTAINTY QUANTIFICATION SO NUCLEAR TECHNOLOGY LA English DT Article; Proceedings Paper CT 14th International Topical Meeting on Nuclear Reactor Thermal Hydraulics (NURETH) CY SEP 25-30, 2011 CL Toronto, CANADA SP Canadian Nucl Soc, Amer Nucl Soc, Thermal Hydraul Div, Int Atom Energy Agcy, Nucl Energy Agcy, Org Econ Co-Operat & Dev DE forward sensitivity analysis; uncertainty quantification; numerical error ID COMPUTATIONAL FLUID-DYNAMICS; DIFFERENTIAL-EQUATIONS; ALGEBRAIC EQUATIONS; VERIFICATION; SYSTEMS AB This paper presents extended forward sensitivity analysis as a method to improve uncertainty quantification. By including the time step and potentially grid spacing as special sensitivity parameters, the forward sensitivity method is extended as one method to quantify numerical errors. Note that by integrating local truncation errors over the whole system through the forward sensitivity analysis process, the generated time step sensitivity information reflects global numerical errors. Discretization errors can be systematically compared against uncertainties due to other physical parameters. This extension makes the forward sensitivity method a much more powerful tool than other tools of its type to help uncertainty quantification. When the relative sensitivity of the time step to other physical parameters is known, the simulation is allowed to run at optimized time steps without affecting the confidence of the physical parameter sensitivity results. The time step forward sensitivity analysis method can also replace traditional time step convergence studies that are a key part of code verification, with much less computational cost. Two well-defined benchmark problems with manufactured solutions are utilized to demonstrate the method. C1 [Zhao, Haihua] Idaho Natl Lab, Idaho Falls, ID 83415 USA. [Mousseau, Vincent A.] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Zhao, HH (reprint author), Idaho Natl Lab, POB 1625, Idaho Falls, ID 83415 USA. EM Haihua.Zhao@inl.gov NR 18 TC 1 Z9 1 U1 0 U2 1 PU AMER NUCLEAR SOC PI LA GRANGE PK PA 555 N KENSINGTON AVE, LA GRANGE PK, IL 60526 USA SN 0029-5450 J9 NUCL TECHNOL JI Nucl. Technol. PD JAN PY 2013 VL 181 IS 1 SI SI BP 184 EP 195 PG 12 WC Nuclear Science & Technology SC Nuclear Science & Technology GA 063CN UT WOS:000312973800016 ER PT J AU Xiao, T Cui, WP Cai, M Leung, W Anderegg, JW Shinar, J Shinar, R AF Xiao, Teng Cui, Weipan Cai, Min Leung, Wai Anderegg, James W. Shinar, Joseph Shinar, Ruth TI Inverted polymer solar cells with a solution-processed cesium halide interlayer SO ORGANIC ELECTRONICS LA English DT Article DE Inverted organic solar cells; Cesium iodide (CsI) interlayer; CsF or CsCl interlayers; Molybdenum oxide interlayer; P3HT structured aggregates ID OPEN-CIRCUIT VOLTAGE; EFFICIENCY; BLENDS AB We demonstrate the utility of a low-cost cesium iodide interlayer spun from an aqueous or 2-ethoxyethanol solution on ITO in inverted polymer solar cells of the structure ITO/CsI/P3HT:PCBM/MoO3/Al, where P3HT is poly(3-hexylthiophene) and PCBM is [6,6]-phenyl-C-60-butyric acid methyl ester. The power conversion efficiency (PCE) of optimized cells was similar to 3.4%, comparable to that we obtained for inverted cells with Cs carbonate. The thickness of the CsI film was adjusted by varying the solution concentration. The concentration affected the surface morphology of P3HT:PCBM and the density of fractal-like aggregates (possibly related to the presence of Cs and film fabrication conditions) formed near the anode, as revealed by scanning electron microscopy. Auger analysis indicated a P3HT-rich surface. Optimization of the cells was achieved also by varying the thickness of the MoO3 and the drying/annealing conditions of the active layer, as was evident from the current-voltage characteristics, external quantum efficiency spectra, and PCE. The cells with the CsI interlayer were compared additionally to cells with CsCl or CsF interlayers (with a PCE of up to similar to 2.7%), which were inferior to the comparable cells with Cs2CO3 or CsI. The surface concentrations of Cs and the halide on ITO were monitored using X-ray photoelectron spectroscopy. The iodine level was low with the Cs:I ratio exceeding 8:1. In contrast, the Cs:Cl ratio was similar to 1.4:1 and the Cs:F ratio was similar to 1:1; the Cs2CO3 decomposed partially, as expected. Therefore, for CsI, as is the case for Cs2CO3 but not for CsF, Cs-O bonds are formed at the surface. Such bonds on ITO are important in modifying the ITO work function, improving the cell performance. The results indicate that spin coating solutions of the high polarity CsI is a promising and easy approach to introduce Cs-O on ITO in inverted structures for increased electron extraction from PCBM and possibly hole extraction from the P3HT-rich surface at the anode. (c) 2012 Elsevier B.V. All rights reserved. C1 [Xiao, Teng; Leung, Wai; Shinar, Ruth] Iowa State Univ, Microelect Res Ctr, Ames, IA 50011 USA. [Xiao, Teng; Cui, Weipan; Cai, Min; Leung, Wai; Anderegg, James W.; Shinar, Joseph] Iowa State Univ, Ames Lab, USDOE, Ames, IA 50011 USA. [Xiao, Teng; Cui, Weipan; Cai, Min; Shinar, Joseph] Iowa State Univ, Dept Phys & Astron, Ames, IA 50011 USA. [Shinar, Ruth] Iowa State Univ, Dept Elect & Comp Engn, Ames, IA 50011 USA. RP Shinar, J (reprint author), Iowa State Univ, Ames Lab, USDOE, Ames, IA 50011 USA. EM jshinar@iastate.edu; rshinar@iastate.edu RI Cai, Min/A-2678-2014 FU Iowa State University for the US Department of Energy (USDOE) [DE-AC 02-07CH11358]; Iowa Power Fund; EAGER NSF Grant; Basic Energy Sciences, Division of Materials Science and Engineering, USDOE FX Ames Laboratory is operated by Iowa State University for the US Department of Energy (USDOE) under Contract No. DE-AC 02-07CH11358. R.S. acknowledges partial support by the Iowa Power Fund and an EAGER NSF Grant. T.X., M.C., W.L. and J.W.A. were partially supported by the Basic Energy Sciences, Division of Materials Science and Engineering, USDOE. We thank Max Noack for helpful discussions. NR 28 TC 16 Z9 16 U1 3 U2 95 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 1566-1199 J9 ORG ELECTRON JI Org. Electron. PD JAN PY 2013 VL 14 IS 1 BP 267 EP 272 DI 10.1016/j.orgel.2012.10.020 PG 6 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA 072QB UT WOS:000313686200038 ER PT J AU Ajuria, J Chavhan, S Tena-Zaera, R Chen, JH Rondinone, AJ Sonar, P Dodabalapur, A Pacios, R AF Ajuria, Jon Chavhan, Sudam Tena-Zaera, Ramon Chen, Jihua Rondinone, Adam J. Sonar, Prashant Dodabalapur, Ananth Pacios, Roberto TI Nanomorphology influence on the light conversion mechanisms in highly efficient diketopyrrolopyrrole based organic solar cells SO ORGANIC ELECTRONICS LA English DT Article DE Low bandgap; Diketopyrrolopyrrole; Inverted organic solar cells; Nanomorphology; Charge generation and transport ID ESTER BLEND FILMS; POLYMER; PERFORMANCE; MORPHOLOGY; ELECTRON; HOLE; TRANSISTORS; DEPENDENCE AB In this work, diketopyrrolopyrrole-based polymer bulk heterojunction solar cells with inverted and regular architecture have been investigated. The influence of the polymer: fullerene ratio on the photoactive film nanomorphology has been studied in detail. Transmission Electron Microscopy and Atomic Force Microscopy reveal that the resulting film morphology strongly depends on the fullerene ratio. This fact determines the photocurrent generation and governs the transport of free charge carriers. Slight variations on the PCBM ratio respect to the polymer show great differences on the electrical behavior of the solar cell. Once the polymer: fullerene ratio is accurately adjusted, power conversion efficiencies of 4.7% and 4.9% are obtained for inverted and regular architectures respectively. Furthermore, by correlating the optical and morphological characterization of the polymer: fullerene films and the electrical behavior of solar cells, an ad hoc interpretation is proposed to explain the photovoltaic performance as a function of this polymer: blend composition. (c) 2012 Elsevier B.V. All rights reserved. C1 [Ajuria, Jon; Pacios, Roberto] IK4 IKERLAN, Dept Microsyst, E-20500 Arrasate Mondragon, Spain. [Chavhan, Sudam; Tena-Zaera, Ramon] IK4 CIDETEC, Dept Energy, E-20009 Donostia San Sebastian, Spain. [Chen, Jihua; Rondinone, Adam J.] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. [Sonar, Prashant; Dodabalapur, Ananth] Inst Mat Res & Engn, Singapore 117602, Singapore. [Sonar, Prashant; Dodabalapur, Ananth] ASTAR, Singapore 117602, Singapore. [Dodabalapur, Ananth] Univ Texas Austin, Microelect Res Ctr, Austin, TX 78758 USA. RP Tena-Zaera, R (reprint author), IK4 CIDETEC, Dept Energy, Paseo Miramon 196, E-20009 Donostia San Sebastian, Spain. EM rtena@cidetec.es; sonarp@imre.a-star.edu.sg; rpacios@ikerlan.es RI Chen, Jihua/F-1417-2011; Zhang, Jie/L-6851-2014; Tena-Zaera, Ramon/M-2413-2014; Rondinone, Adam/F-6489-2013; OI Chen, Jihua/0000-0001-6879-5936; Tena-Zaera, Ramon/0000-0002-1525-7760; Rondinone, Adam/0000-0003-0020-4612; Sonar, Prashant/0000-0002-1119-4897 FU European Community's Seventh Framework Programme (FP7) of the X10D project [287818]; "Ramon y Cajal'' Program of the Spanish MICINN; Ministerio de Educacion y Ciencia under the project HOPE [CSD2007-00007]; Visiting Investigatorship Programme (VIP) of the Agency for Science, Technology and Research (A*STAR), Republic of Singapore; Division of Scientific User Facilities, Office of Basic Energy Sciences, US Department of Energy FX JA and RP thank the European Community's Seventh Framework Programme (FP7/2007-2013) under Grant No. 287818 of the X10D project for partial financial support of this work. R. T-Z. acknowledges the support from the "Ramon y Cajal'' Program of the Spanish MICINN. Partial financial support from Ministerio de Educacion y Ciencia under the project HOPE CSD2007-00007 (Consolider-Ingenio 2010) is acknowledged. PS and Prof. AD acknowledge the Visiting Investigatorship Programme (VIP) of the Agency for Science, Technology and Research (A*STAR), Republic of Singapore for financial support. Transmission electron micrographs (TEM) images of the blend film were conducted at the Center for Nanophase Materials Sciences, which is sponsored at Oak Ridge National Laboratory by the Division of Scientific User Facilities, Office of Basic Energy Sciences, US Department of Energy. NR 37 TC 15 Z9 15 U1 0 U2 41 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 1566-1199 J9 ORG ELECTRON JI Org. Electron. PD JAN PY 2013 VL 14 IS 1 BP 326 EP 334 DI 10.1016/j.orgel.2012.11.010 PG 9 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA 072QB UT WOS:000313686200046 ER PT J AU Pantelides, ST AF Pantelides, Sokrates T. TI The role of extended defects in device degradation SO PHYSICA STATUS SOLIDI A-APPLICATIONS AND MATERIALS SCIENCE LA English DT Article DE degradation; grain boundaries; interfaces; impurities ID BIPOLAR JUNCTION TRANSISTORS; 1ST-PRINCIPLES CALCULATIONS; CRYSTALLINE SILICON; GRAIN-BOUNDARY; HYDROGEN; DIFFUSION; DEACTIVATION; RADIATION; OXYGEN; IMPURITIES AB Grain boundaries and dislocations are well known to cause trouble in electronic devices, but in most cases they can be avoided by using single crystal films and eliminating or suppressing dislocation densities. Hetero-interfaces, on the other hand, are essential features of devices. This papers reviews several topics from the author's published work, combining theoretical calculations with experimental data (microscopy, electrical measurements) to illustrate the interplay of impurities with extended defects, especially interfaces: dopant segregation in grain boundaries of polycrystalline Si, the role of hydrogen in the degradation of the SiSiO2 interface in Si-based metal-oxide-semiconductor field-effect transistors (MOSFETs), the role of carbon, nitrogen, and hydrogen in the quality and degradation of the SiCSiO2 interface in SiC-based MOSFETs, and the role of vacancies in room-temperature degradation of IIIV high-mobility electron transistors by the formation of microvoids. C1 [Pantelides, Sokrates T.] Vanderbilt Univ, Dept Phys & Astron, Nashville, TN 37235 USA. [Pantelides, Sokrates T.] Vanderbilt Univ, Dept Elect Engn & Comp Sci, Nashville, TN 37235 USA. [Pantelides, Sokrates T.] Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. RP Pantelides, ST (reprint author), Vanderbilt Univ, Dept Phys & Astron, Nashville, TN 37235 USA. EM pantelides@vanderbilt.edu FU Air Force Office of Scientific Research through the MURI program; Office of Naval Research through the MURI program; National Science Foundation; Department of Energy Basic Energy Sciences; DARPA/EPRI joint grant; McMinn Endowment at Vanderbilt University FX The work described here was partially supported by the Air Force Office of Scientific Research and the Office of Naval Research through the MURI program, by the National Science Foundation, by the Department of Energy Basic Energy Sciences, by a DARPA/EPRI joint grant, and by the McMinn Endowment at Vanderbilt University. Contributions by R. Buczko, M. F. Chisholm, G. Y. Chung, S. Dhar, G. Duscher, L. C. Feldman, D. M. Fleetwood, A. Franceschetti, A. Maiti, K. McDonald, S. J. Pennycook, Y. S. Puzyrev, S. N. Rashkeev, T. Roy, R. D. Schrimpf, X. Shen, L. Tsetseris, S. Wang, K. H. Warnick, R. A. Weller, J. R. Williams, Y. Yan are gratefully acknowledged. NR 37 TC 2 Z9 2 U1 5 U2 49 PU WILEY-V C H VERLAG GMBH PI WEINHEIM PA BOSCHSTRASSE 12, D-69469 WEINHEIM, GERMANY SN 1862-6300 J9 PHYS STATUS SOLIDI A JI Phys. Status Solidi A-Appl. Mat. PD JAN PY 2013 VL 210 IS 1 BP 175 EP 180 DI 10.1002/pssa.201200567 PG 6 WC Materials Science, Multidisciplinary; Physics, Applied; Physics, Condensed Matter SC Materials Science; Physics GA 073IN UT WOS:000313736800016 ER PT J AU Kalluri, RK Biener, MM Suss, ME Merrill, MD Stadermann, M Santiago, JG Baumann, TF Biener, J Striolo, A AF Kalluri, R. K. Biener, M. M. Suss, M. E. Merrill, M. D. Stadermann, M. Santiago, J. G. Baumann, T. F. Biener, J. Striolo, A. TI Unraveling the potential and pore-size dependent capacitance of slit-shaped graphitic carbon pores in aqueous electrolytes SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID ELECTRICAL DOUBLE-LAYER; MOLECULAR-DYNAMICS; IONIC LIQUID; ELECTROCHEMICAL CAPACITORS; COMPUTER-SIMULATION; SUPERCAPACITORS; DESALINATION; ELECTRODES; NANOTUBES; HYDRATION AB Understanding and leveraging physicochemical processes at the pore scale are believed to be essential to future performance improvements of supercapacitors and capacitive desalination (CD) cells. Here, we report on a combination of electrochemical experiments and fully atomistic simulations to study the effect of pore size and surface charge density on the capacitance of graphitic nanoporous carbon electrodes. Specifically, we used cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) to study the effect of potential and pore size on the capacitance of nanoporous carbon foams. Molecular dynamics simulations were performed to study the pore-size dependent accumulation of aqueous electrolytes in slit-shaped graphitic carbon pores of different widths (0.65 to 1.6 nm). Experimentally, we observe a pronounced increase of the capacitance of sub-nm pores as the applied potential window gets wider, from a few F g(-1) for narrow potential ranges (-0.3 to 0.3 V vs. Ag/AgCl) to similar to 40 F g(-1) for wider potential windows (-0.9 V to 0.9 V vs. Ag/AgCl). By contrast, the capacitance of wider pores does not depend significantly on the applied potential window. Molecular dynamics simulations confirm that the penetration of ions into pores becomes more difficult with decreasing pore width and increasing strength of the hydration shell. Consistent with our experimental results, we observe a pore- and ion-size dependent threshold-like charging behavior when the pore width becomes comparable to the size of the hydrated ion (0.65 nm pores for Na+ and 0.79 nm pores for Cl- ions). The observed pore-size and potential dependent accumulation of ions in slit-shaped carbon pores can be explained by the hydration structure of the ions entering the charged pores. The results are discussed in view of their effect on energy-storage and desalination efficiency. C1 [Kalluri, R. K.; Striolo, A.] Univ Oklahoma, Sch Chem Biol & Mat Engn, Norman, OK 73019 USA. [Biener, M. M.; Suss, M. E.; Merrill, M. D.; Stadermann, M.; Baumann, T. F.; Biener, J.] Lawrence Livermore Natl Lab, Nanoscale Synth & Characterizat Lab, Livermore, CA 94550 USA. [Suss, M. E.; Santiago, J. G.] Stanford Univ, Dept Mech Engn, Stanford, CA 94305 USA. RP Biener, J (reprint author), Lawrence Livermore Natl Lab, Nanoscale Synth & Characterizat Lab, Livermore, CA 94550 USA. EM biener2@llnl.gov; astriolo@ou.edu FU U.S. Department of Energy [DE-SC0001902]; US DOE by LLNL [DE-AC52-07NA27344]; LDRD Program at LLNL [12-ERD-035] FX Work at the University of Oklahoma was supported, in part, by the U.S. Department of Energy, under contract number DE-SC0001902. Work at LLNL was performed under the auspices of the US DOE by LLNL under Contract DE-AC52-07NA27344. Project 12-ERD-035 was funded by the LDRD Program at LLNL. Generous allocations of computing time were provided by the Oklahoma Supercomputer Center for Education and Research (OSCER) and by the National Energy Resources Supercomputer Center (NERSC). AS and RKK wish to thank Deepthi Konatham and Dr Naga Rajesh Tummala for helpful discussions. NR 56 TC 31 Z9 32 U1 2 U2 102 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 2013 VL 15 IS 7 BP 2309 EP 2320 DI 10.1039/c2cp43361c PG 12 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 075MR UT WOS:000313891400008 PM 23295944 ER PT J AU Szanyi, J Kwak, JH Zhu, HY Peden, CHF AF Szanyi, Janos Kwak, Ja Hun Zhu, Haiyang Peden, Charles H. F. TI Characterization of Cu-SSZ-13 NH3 SCR catalysts: an in situ FTIR study SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID EXCHANGED ZSM-5 ZEOLITES; LEAN NOX REDUCTION; NITRIC-OXIDE; CU-ZSM-5 CATALYSTS; NITROGEN MONOXIDE; REDOX CHEMISTRY; METHANE OXIDATION; CARBON-MONOXIDE; GASEOUS CUCL; DECOMPOSITION AB The adsorption of CO and NO over Cu-SSZ-13 zeolite catalysts, highly active in the selective catalytic reduction of NOx with NH3, was investigated by FTIR spectroscopy, and the results obtained were compared to those collected from other Cu-ion exchanged zeolites (Y,FAU and ZSM-5). Under low CO pressures and at room temperature (295 K), CO forms monocarbonyls exclusively on the Cu+ ions, while in the presence of gas phase CO dicarbonyls on Cu+ and adsorbed CO on Cu2+ centers form, as well. At low (cryogenic) sample temperatures, tricarbonyl formation on Cu+ sites was also observed. The adsorption of NO produces IR bands that can be assigned to nitrosyls bound to both Cu+ and Cu2+ centers, and NO+ species located in charge compensating cationic positions of the chabasite framework. On the reduced Cu-SSZ-13 samples the formation of N2O was also detected. The assignment of the adsorbed NOx species was aided by adsorption experiments with isotopically labeled (NO)-N-15. The movement of Cu ions from the sterically hindered six member ring position to the more accessible cavity positions as a result of their interaction with adsorbates (NO and H2O) was clearly evidenced. Comparisons of the spectroscopy data obtained in the static transmission IR system to those collected in the flow-through diffuse reflectance cell points out that care must be taken when general conclusions are drawn about the adsorptive and reactive properties of metal cation centers based on a set of data collected under well defined, specific experimental conditions. C1 [Szanyi, Janos; Kwak, Ja Hun; Zhu, Haiyang; Peden, Charles H. F.] Pacific NW Natl Lab, Inst Integrated Catalysis, Richland, WA 99352 USA. RP Szanyi, J (reprint author), Pacific NW Natl Lab, Inst Integrated Catalysis, Richland, WA 99352 USA. EM janos.szanyi@pnnl.gov RI Kwak, Ja Hun/J-4894-2014; OI Peden, Charles/0000-0001-6754-9928 FU US Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Program; US DOE, Office of Biological and Environmental Research FX Financial support was provided by the US Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Program. This work was performed in the Environmental Molecular Sciences Laboratory (EMSL) at Pacific Northwest National Laboratory (PNNL). The EMSL is a national scientific user facility supported by the US DOE, Office of Biological and Environmental Research. PNNL is a multi-program national laboratory operated for the US DOE by Battelle. NR 48 TC 56 Z9 58 U1 13 U2 212 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2013 VL 15 IS 7 BP 2368 EP 2380 DI 10.1039/c2cp43467a PG 13 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 075MR UT WOS:000313891400015 PM 23301245 ER PT J AU Kim, WC Ko, JH Kim, JY Kim, J Bae, HJ Han, KH AF Kim, Won-Chan Ko, Jae-Heung Kim, Joo-Yeol Kim, Jungmook Bae, Hyeun-Jong Han, Kyung-Hwan TI MYB46 directly regulates the gene expression of secondary wall-associated cellulose synthases in Arabidopsis SO PLANT JOURNAL LA English DT Article DE MYB46; cellulose; cellulose synthase; transcription factor; secondary wall; Arabidopsis ID NAC TRANSCRIPTION FACTORS; PROGRAMMED CELL-DEATH; HIGHER-PLANTS; DIRECT TARGET; BIOSYNTHESIS; THALIANA; XYLEM; DIFFERENTIATION; IDENTIFICATION; ACTIVATION AB Cellulose is the most abundant biopolymer on Earth. Three cellulose synthases (CESA4, CESA7 and CESA8) are necessary for cellulose production in the secondary cell walls of Arabidopsis. Little is known about how expression of these CESA genes is regulated. We recently identified a cis-regulatory element (M46RE) that is recognized by MYB46, which is a master switch for secondary wall formation in Arabidopsis. A genome-wide survey of promoter sequences for the presence of M46REs led to the hypothesis that MYB46 may function as a direct regulator of all three secondary wall-associated cellulose synthase genes: CESA4, CESA7 and CESA8. We tested this hypothesis using several lines of experimental evidence. All three CESA genes are highly up-regulated by both constitutive and inducible over-expression of MYB46 in planta. Using a steroid receptor-based inducible activation system, we show that MYB46 directly activates transcription of the three CESA genes. We then used an electrophoretic mobility shift assay and chromatin immunoprecipitation analysis to confirm that MYB46 protein directly binds to the promoters of the three CESA genes both in vitro and in vivo. Furthermore, ectopic up-regulation of MYB46 resulted in a significant increase of crystalline cellulose content in Arabidopsis. Taken together, we have identified MYB46 as a transcription factor that directly regulates all three secondary wall-associated CESA genes. Yeast one-hybrid screening identified additional transcription factors that regulate the CESA genes. However, none of the putative regulators appears to be regulated by MYB46, suggesting the multi-faceted nature of transcriptional regulation of secondary wall cellulose biosynthesis. C1 [Kim, Won-Chan; Kim, Joo-Yeol; Han, Kyung-Hwan] Michigan State Univ, Dept Hort, E Lansing, MI 48824 USA. [Kim, Won-Chan; Kim, Joo-Yeol; Han, Kyung-Hwan] Michigan State Univ, Dept Forestry, E Lansing, MI 48824 USA. [Kim, Won-Chan; Kim, Joo-Yeol; Han, Kyung-Hwan] Michigan State Univ, Dept Energy, Great Lakes Bioenergy Res Ctr, E Lansing, MI 48824 USA. [Ko, Jae-Heung] Kyung Hee Univ, Dept Plant & Environm New Resources, Yongin 446701, Gyeonggi Do, South Korea. [Ko, Jae-Heung] Kyung Hee Univ, Bioenergy Ctr, Yongin, South Korea. [Kim, Jungmook; Bae, Hyeun-Jong; Han, Kyung-Hwan] Chonnam Natl Univ, Dept Bioenergy Sci & Technol, Kwangju 500757, South Korea. RP Han, KH (reprint author), Michigan State Univ, Dept Hort, E Lansing, MI 48824 USA. EM hanky@msu.edu RI Han, Kyung-Hwan/G-6141-2012 OI Han, Kyung-Hwan/0000-0001-9481-4643 FU Department of Energy Great Lakes Bioenergy Research Center (Department of Energy Office of Science) [BER DR-FC02-07ER64494]; Ministry of Education, Science and Technology of Korea via the World Class University Project at Chonnam National University [R31-2009-000-20025-0]; Basic Science Research Program through the National Research Foundation of Korea [2012-0002648]; Kyung Hee University [KHU-20100611] FX This work was funded by the Department of Energy Great Lakes Bioenergy Research Center (Department of Energy Office of Science BER DR-FC02-07ER64494), in part by the Ministry of Education, Science and Technology of Korea via the World Class University Project at Chonnam National University (R31-2009-000-20025-0), and in part by the Basic Science Research Program through the National Research Foundation of Korea (2012-0002648) and a grant from Kyung Hee University (KHU-20100611). The authors would like to thank Michael Thomashow and Yong Sig Kim for providing the yeast expression library of Arabidopsis transcription factors, and Daniel Keathley (Department of Horticulture, Michigan State University), Kenneth Keegstra (DOE-Great Lakes Bioenergy Research Center, Michigan State University), Chandrashekhar Joshi (Department of Biology, Michigan Technological University) and Curtis Wilkerson (Department of Plant Biology, Michigan State University) for critical reading of the manuscript. NR 50 TC 21 Z9 27 U1 4 U2 53 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0960-7412 EI 1365-313X J9 PLANT J JI Plant J. PD JAN PY 2013 VL 73 IS 1 BP 26 EP 36 DI 10.1111/j.1365-313x.2012.05124.x PG 11 WC Plant Sciences SC Plant Sciences GA 079PM UT WOS:000314183300003 PM 26011122 ER PT J AU Wang, Y Mortimer, JC Davis, J Dupree, P Keegstra, K AF Wang, Yan Mortimer, Jennifer C. Davis, Jonathan Dupree, Paul Keegstra, Kenneth TI Identification of an additional protein involved in mannan biosynthesis SO PLANT JOURNAL LA English DT Article DE mannan biosynthesis; Golgi protein; glycosyltransferase; GT65; fenugreek; Arabidopsis ID CELLULOSE SYNTHASE-LIKE; CELL-WALL; FAMILY-MEMBERS; GENE FAMILY; ARABIDOPSIS; PLANTS; MEMBRANE; GLYCOSYLTRANSFERASES; POLYSACCHARIDES; LOCALIZATION AB Galactomannans comprise a beta-1,4-mannan backbone substituted with alpha-1,6-galactosyl residues. Genes encoding the enzymes that are primarily responsible for backbone synthesis and side-chain addition of galactomannans were previously identified and characterized. To identify additional genes involved in galactomannan biosynthesis, we previously performed deep EST profiling of fenugreek (Trigonella foenum-graecum L.) seed endosperm, which accumulates large quantities of galactomannans as a reserve carbohydrate during seed development. One of the candidate genes encodes a protein that is likely to be a glycosyltransferase. Because this protein is involved in mannan biosynthesis, we named it 'mannan synthesis-related' (MSR). Here, we report the characterization of a fenugreek MSR gene (TfMSR) and its two Arabidopsis homologs, AtMSR1 and AtMSR2. TfMSR was highly and specifically expressed in the endosperm. TfMSR, AtMSR1 and AtMSR2 proteins were all determined to be localized to the Golgi by fluorescence confocal microscopy. The level of mannosyl residues in stem glucomannans decreased by approximately 40% for Arabidopsis msr1 single T-DNA insertion mutants and by more than 50% for msr1 msr2 double mutants, but remained unchanged for msr2 single mutants. In addition, in vitro mannan synthase activity from the stems of msr1 single and msr1 msr2 double mutants also decreased. Expression of AtMSR1 or AtMSR2 in the msr1 msr2 double mutant completely or partially restored mannosyl levels. From these results, we conclude that the MSR protein is important for mannan biosynthesis, and offer some ideas about its role. C1 [Wang, Yan; Keegstra, Kenneth] Michigan State Univ, Great Lakes Bioenergy Res Ctr, E Lansing, MI 48824 USA. [Wang, Yan; Davis, Jonathan; Keegstra, Kenneth] Michigan State Univ, Plant Res Lab, Dept Energy, E Lansing, MI 48824 USA. [Mortimer, Jennifer C.; Dupree, Paul] Univ Cambridge, Dept Biochem, Cambridge CB2 1QW, England. [Davis, Jonathan; Keegstra, Kenneth] Michigan State Univ, Dept Plant Biol, E Lansing, MI 48824 USA. [Keegstra, Kenneth] Michigan State Univ, Dept Biochem & Mol Biol, E Lansing, MI 48824 USA. RP Keegstra, K (reprint author), Michigan State Univ, Great Lakes Bioenergy Res Ctr, E Lansing, MI 48824 USA. EM keegstra@msu.edu OI Mortimer, Jenny/0000-0001-6624-636X FU Department of Energy Great Lakes Bioenergy Research Center (DOE BER Office of Science) [DE-FC02-07ER64494]; UK Biotechnology and Biological Sciences Research Council [BB/G016240/1] FX We thank Linda Danhof, Robert Orler and Elizabeth Drain at the Arabidopsis Service Center of the Great Lakes Bioenergy Research Center (GLBRC) of the Department of Energy at Michigan State University for technical help in genotyping T-DNA insertion lines and transformation of Arabidopsis, Cliff Foster at the Cell Wall Analytical Platform of the Great Lakes Bioenergy Research Center at Michigan State University for technical help in analysis of matrix neutral monosaccharide composition and crystalline cellulose content, Federica Brandizzi for providing the Golgi marker ST-mRFP, and David M. Cavalier, Jacob K. Jensen, Curtis G. Wilkerson, Federica Brandizzi and Kyung-Hwan Han, as well as other members of the Keegstra laboratory and cell wall group at Michigan State University, for helpful discussions and technical advice. This work was funded in part by the Department of Energy Great Lakes Bioenergy Research Center (DOE BER Office of Science DE-FC02-07ER64494) and by a grant from the UK Biotechnology and Biological Sciences Research Council (BB/G016240/1 BBSRC Sustainable Energy Centre Cell Wall Sugars Programme) to P.D. NR 43 TC 8 Z9 8 U1 2 U2 32 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0960-7412 J9 PLANT J JI Plant J. PD JAN PY 2013 VL 73 IS 1 BP 105 EP 117 DI 10.1111/tpj.12019 PG 13 WC Plant Sciences SC Plant Sciences GA 079PM UT WOS:000314183300009 PM 22966747 ER PT J AU Lo, CT Lee, B Gao, MW Chou, PW AF Lo, Chieh-Tsung Lee, Byeongdu Gao, Mong-Wei Chou, Po-Wei TI Ordering of block copolymer/nanoparticle composite thin films SO POLYMER INTERNATIONAL LA English DT Article DE block copolymer; nanoparticle; morphology; thin film ID X-RAY-SCATTERING; DIBLOCK COPOLYMERS; POLY(METHYL METHACRYLATE); NANOPARTICLES; MIXTURES; PHASE; MICELLES; NANOCOMPOSITES; TRANSFORMATION; POLYSTYRENE AB The ordering behavior of polymer nanocomposites composed of gold nanoparticles confined in the polystyrene ( PS) domains of PS based block copolymers was investigated. The results reveal that the self-assembly of nanoparticles in the PS domains improved the ordering of microdomains. This is attributed to the presence of nanoparticles that reduced the degree of segregation of the system, causing slow phase separation. This facilitates the packing of the cylindrical microdomains, leading to awell-ordered structure of the composite. When particles were incorporated into themajor domains of cylindrically ordered block copolymer, the connectivity of the domains allowed particles to move to the top of the film to gain additional entropy of the system. In contrast, when particles were organized in parallel cylinders in the block copolymer, they were confined in the cylinders which prevented them from diffusing in the depth direction. The aggregation of nanoparticles was amplified when the composite was annealed in air. We believe that the results from this study will enable more understanding of the effects of nanoparticles on the ordering of block copolymer/nanoparticle composite thin films and will provide a tool in the fabrication of composite thin films. (C) 2012 Society of Chemical Industry C1 [Lo, Chieh-Tsung; Gao, Mong-Wei; Chou, Po-Wei] Natl Cheng Kung Univ, Dept Chem Engn, Tainan 701, Taiwan. [Lee, Byeongdu] Argonne Natl Lab, Xray Sci Div, Argonne, IL 60439 USA. RP Lo, CT (reprint author), Natl Cheng Kung Univ, Dept Chem Engn, 1 Univ Rd, Tainan 701, Taiwan. EM tsunglo@mail.ncku.edu.tw OI Lee, Byeongdu/0000-0003-2514-8805 FU US Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]; National Science Council of the Republic of China [NSC 98-2221-E-006-004-MY2] FX This work benefited by the use of argonne photon source (APS) and chemical technology division (CMT) funded by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, under contract # DE-AC02-06CH11357. The authors also appreciate financial support from the National Science Council of the Republic of China under Grant No. NSC 98-2221-E-006-004-MY2. NR 44 TC 3 Z9 3 U1 1 U2 58 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0959-8103 J9 POLYM INT JI Polym. Int. PD JAN PY 2013 VL 62 IS 1 BP 99 EP 105 DI 10.1002/pi.4303 PG 7 WC Polymer Science SC Polymer Science GA 075QX UT WOS:000313902700013 ER PT J AU Waters, KM Stenoien, DL Sowa, MB von Neubeck, C Chrisler, WB Tan, RM Sontag, RL Weber, TJ AF Waters, Katrina M. Stenoien, David L. Sowa, Marianne B. von Neubeck, Claere Chrisler, William B. Tan, Ruimin Sontag, Ryan L. Weber, Thomas J. TI Annexin A2 Modulates Radiation-Sensitive Transcriptional Programming and Cell Fate SO RADIATION RESEARCH LA English DT Article ID NF-KAPPA-B; HUMAN SKIN KERATINOCYTES; DOSE IONIZING-RADIATION; PROSTATE-CANCER CELLS; GENE-EXPRESSION; HUMAN FIBROBLASTS; ALPHA-PARTICLE; TISSUE MODEL; STEM-CELL; PROTEIN AB Waters, K. M., Stenoien, D. L., Sowa, M. B., von Neubeck, C. H., Chrisler, W. B., Tan, R., Sontag R. L. and Weber, T. J. Annexin A2 Modulates Radiation-Sensitive Transcriptional Programming and Cell Fate. Radiat. Res. 179, 53-61 (2013). We previously established annexin A2 as a radioresponsive protein associated with anchorage independent growth in murine epidermal cells. In this study, we demonstrate annexin A2 nuclear translocation in human skin organotypic culture and murine epidermal cells after exposure to X radiation (10-200 cGy), supporting a conserved nuclear function for annexin A2. Whole genome expression profiling in the presence and absence of annexin A2 [shRNA] identified fundamentally altered transcriptional programming that changes the radioresponsive transcriptome. Bioinformatics predicted that silencing ArixA2 may enhance cell death responses to stress in association with reduced activation of pro-survival signals such as nuclear factor kappa B. This prediction was validated by demonstrating a significant increase in sensitivity toward tumor necrosis factor alpha-induced cell death in annexin A2 silenced cells, relative to vector controls, associated with reduced nuclear translocation of RelA (p65) following tumor necrosis factor alpha treatment. These observations implicate an annexin A2 niche in cell fate regulation such that AnxA2 protects cells from radiation-induced apoptosis to maintain cellular homeostasis at low-dose radiation. (C) 2013 by Radiation Research Society C1 [Waters, Katrina M.; Stenoien, David L.; Sowa, Marianne B.; von Neubeck, Claere; Chrisler, William B.; Tan, Ruimin; Sontag, Ryan L.; Weber, Thomas J.] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Weber, TJ (reprint author), Pacific NW Natl Lab, 902 Battelle Blvd,J4-02, Richland, WA 99352 USA. EM Thomas.Weber@pnnl.gov FU Biological and Environmental Research Program (BER), U.S. Department of Energy [DE-AC06-76RLO]; National Aeronautics and Space Administration [NNX10AB06G]; U.S. Department of Energy [DE-AC05-76RL0 1830] FX The authors thank Dr. William Morgan and Dr. Antone Brooks for their critical review of the manuscript and helpful discussions. This work was supported by the Biological and Environmental Research Program (BER), U.S. Department of Energy [DE-AC06-76RLO] and the National Aeronautics and Space Administration [NNX10AB06G]. This manuscript has been authored by Battelle Memorial Institute, Pacific Northwest Division, under Contract no. DE-AC05-76RL0 1830 with the U.S. Department of Energy. NR 47 TC 11 Z9 11 U1 0 U2 4 PU RADIATION RESEARCH SOC PI LAWRENCE PA 810 E TENTH STREET, LAWRENCE, KS 66044 USA SN 0033-7587 J9 RADIAT RES JI Radiat. Res. PD JAN PY 2013 VL 179 IS 1 BP 53 EP 61 DI 10.1667/RR3056.1 PG 9 WC Biology; Biophysics; Radiology, Nuclear Medicine & Medical Imaging SC Life Sciences & Biomedicine - Other Topics; Biophysics; Radiology, Nuclear Medicine & Medical Imaging GA 076AG UT WOS:000313928300007 PM 23148505 ER PT J AU Dilmanian, FA Jenkins, AL Olschowka, JA Zhong, Z Park, JY Desnoyers, NR Sobotka, S Fois, GR Messina, CR Morales, M Hurley, SD Trojanczyk, L Ahmad, S Shahrabi, N Coyle, PK Meek, AG O'Banion, MK AF Dilmanian, F. Avraham Jenkins, Arthur L., III Olschowka, John A. Zhong, Zhong Park, Jane Y. Desnoyers, Nicolle R. Sobotka, Stanislaw Fois, Giovanna R. Messina, Catherine R. Morales, Marjorie Hurley, Sean D. Trojanczyk, LeeAnn Ahmad, Saffa Shahrabi, Neda Coyle, Patricia K. Meek, Allen G. O'Banion, M. Kerry TI X-Ray Microbeam Irradiation of the Contusion-Injured Rat Spinal Cord Temporarily Improves Hind-Limb Function SO RADIATION RESEARCH LA English DT Article ID CENTRAL-NERVOUS-SYSTEM; RADIATION-THERAPY; MICROPLANAR BEAMS; MOUSE-BRAIN; SYNCHROTRON-WIGGLER; LOCOMOTOR RECOVERY; TISSUE; CNS; INFLAMMATION; EXPRESSION AB Dilmanian, F. A., Jenkins, M, A. L., Olschowka, J., Zhong, Z., Park, J. Y., Desnoyers, N. R., Sobotka, S., Fois, G. R., Messina, C. R., Morales, M., Hurley, S. D., Trojanczyk, L., Ahmad, S., Shahrabi, N., Coyle, P. K., Meek, A. G. and O'Banion, M. K. X-Ray Microbeam Irradiation of the Contusion-Injured Rat Spinal Cord Temporarily Improves Hind-Limb Function. Radiat. Res. 179, 76-88 (2013). Spinal cord injury is a devastating condition with no effective treatment. The physiological processes that impede recovery include potentially detrimental immune responses and the production of reactive astrocytes. Previous work suggested that radiation treatment might be beneficial in spinal cord injury, although the method carries risk of radiation-induced damage. To overcome this obstacle we used arrays of parallel, synchrotron-generated X-ray microbeams (230 mu m with 150 mu m gaps between them) to irradiate an established model of rat spinal cord contusion injury. This technique is known to have a remarkable sparing effect in tissue, including the central nervous system. Injury was induced in adult female Long-Evans rats at the level of the thoracic vertebrae T9-T10 using 25 mm rod drop on an NYU Impactor. Microbeam irradiation was given to groups of 6-8 rats each, at either Day 10 (50 or 60 Gy in-beam entrance doses) or Day 14 (50, 60 or 70 Gy). The control group was comprised of two subgroups: one studied three months before the irradiation experiment (n = 9) and one at the time of the irradiations (it = 7). Hind-limb function was blindly scored with the Basso, Beattie and Bresnahan (BBB) rating scale on a nearly weekly basis. The scores for the rats irradiated at Day 14 post-injury, when using t test with 7-day data-averaging time bins, showed statistically significant improvement at 28-42 days post-injury (P < 0.038). H&E staining, tissue volume measurements and immunohistochemistry at day similar to 110 post-injury did not reveal obvious differences between the irradiated and nonirradiated injured rats. The same microbeam irradiation of normal rats at 70 Gy in-beam entrance dose caused no behavioral deficits and no histological effects other than minor microglia activation at 110 days. Functional improvement in the 14-day irradiated group might be due to a reduction in populations of immune cells and/or reactive astrocytes, while the Day 10/Day 14 differences may indicate time-sensitive changes in these cells and their populations. With optimizations, including those of the irradiation time(s), microbeam pattern, dose, and perhaps concomitant treatments such as immunological intervention this method may ultimately reach clinical use. (C) 2013 by Radiation Research Society C1 [Dilmanian, F. Avraham; Park, Jane Y.; Desnoyers, Nicolle R.; Fois, Giovanna R.; Morales, Marjorie; Ahmad, Saffa; Shahrabi, Neda] Brookhaven Natl Lab, Dept Med, Upton, NY 11973 USA. [Zhong, Zhong] Brookhaven Natl Lab, Natl Synchrotron Light Source, Upton, NY 11973 USA. [Dilmanian, F. Avraham] SUNY Stony Brook, Dept Radiat Oncol, Hlth Sci Ctr, Stony Brook, NY 11794 USA. [Dilmanian, F. Avraham; Coyle, Patricia K.] SUNY Stony Brook, Dept Neurol, Stony Brook, NY 11794 USA. [Messina, Catherine R.] SUNY Stony Brook, Dept Prevent Med, Stony Brook, NY 11794 USA. [Jenkins, Arthur L., III; Sobotka, Stanislaw] Mt Sinai Sch Med, Dept Neurosurg, New York, NY USA. [Olschowka, John A.; Hurley, Sean D.; Trojanczyk, LeeAnn; O'Banion, M. Kerry] Univ Rochester, Dept Neurobiol & Anat, Rochester, NY USA. [Sobotka, Stanislaw] Hackensack Univ, Med Ctr, Dept Res, Hackensack, NJ USA. [Fois, Giovanna R.] Univ Cagliari, Dept Phys, I-09042 Sardinia, Italy. RP Dilmanian, FA (reprint author), SUNY Stony Brook, Dept Radiat Oncol, Hlth Sci Ctr, Level 2, Stony Brook, NY 11794 USA. EM avraham.dilmanian@stonybrook.edu FU New York State Spinal Cord Injury Research Program, Stony Brook Foundation; Stony Brook's School of Medicine and the Office of Vice President for Research; Concerned Women of the Grove; U.S. Department of Energy, Office of Science, and Office of Basic Energy Sciences [DE-AC02-98CH10886] FX We thank Usman As lam, Kerry Bonti, Tiffany Bowman, Kaitlin Burke, Shravan Cheruku, Jessica Choi, Dean M. Connor, Jr., Faith Consiglio, Michael Frahangian, Joseph Gatz, III, John Kalef-Ezra, Joel M. Levine, Peggy L. Micca, Marta M. Nawrocky, Lynda Nwabuobi, Maryann Petry, Wojtek Sobotka, Stella E. Tsirka, Stephan Warren, Johannes Wolff, and Tom Zimmerman for assistance. Research was supported by grants from The New York State Spinal Cord Injury Research Program, Stony Brook Foundation (Allen G. Meek, P.I.), Stony Brook's School of Medicine and the Office of Vice President for Research, and Concerned Women of the Grove. Use of the NSLS, BNL was supported by the U.S. Department of Energy, Office of Science, and Office of Basic Energy Sciences, under Contract No. DE-AC02-98CH10886. NR 40 TC 4 Z9 5 U1 0 U2 5 PU RADIATION RESEARCH SOC PI LAWRENCE PA 810 E TENTH STREET, LAWRENCE, KS 66044 USA SN 0033-7587 J9 RADIAT RES JI Radiat. Res. PD JAN PY 2013 VL 179 IS 1 BP 76 EP 88 DI 10.1667/RR2921.1 PG 13 WC Biology; Biophysics; Radiology, Nuclear Medicine & Medical Imaging SC Life Sciences & Biomedicine - Other Topics; Biophysics; Radiology, Nuclear Medicine & Medical Imaging GA 076AG UT WOS:000313928300010 PM 23216524 ER PT J AU Strydom, G AF Strydom, Gerhard TI Uncertainty and Sensitivity Analyses of a Pebble Bed HTGR Loss of Cooling Event SO SCIENCE AND TECHNOLOGY OF NUCLEAR INSTALLATIONS LA English DT Article ID CODE AB The Very High Temperature Reactor Methods Development group at the Idaho National Laboratory identified the need for a defensible and systematic uncertainty and sensitivity approach in 2009. This paper summarizes the results of an uncertainty and sensitivity quantification investigation performed with the SUSA code, utilizing the International Atomic Energy Agency CRP 5 Pebble Bed Modular Reactor benchmark and the INL code suite PEBBED-THERMIX. Eight model input parameters were selected for inclusion in this study, and after the input parameters variations and probability density functions were specified, a total of 800 steady state and depressurized loss of forced cooling (DLOFC) transient PEBBED-THERMIX calculations were performed. The six data sets were statistically analyzed to determine the 5% and 95% DLOFC peak fuel temperature tolerance intervals with 95% confidence levels. It was found that the uncertainties in the decay heat and graphite thermal conductivities were the most significant contributors to the propagated DLOFC peak fuel temperature uncertainty. No significant differences were observed between the results of Simple Random Sampling (SRS) or Latin Hypercube Sampling (LHS) data sets, and use of uniform or normal input parameter distributions also did not lead to any significant differences between these data sets. C1 INL, Nucl Sci & Engn Div, Idaho Falls, ID 83415 USA. RP Strydom, G (reprint author), INL, Nucl Sci & Engn Div, 2525 N Fremont Ave, Idaho Falls, ID 83415 USA. EM gerhard.strydom@inl.gov RI Strydom, Gerhard/B-4865-2017 OI Strydom, Gerhard/0000-0002-5712-8553 FU U.S. Department of Energy under DOE Idaho Operations Office [DE-AC07-05ID14517] FX This work is supported by the U.S. Department of Energy, Assistant Secretary for the Office of Nuclear Energy, under DOE Idaho Operations Office Contract DE-AC07-05ID14517. NR 24 TC 0 Z9 0 U1 1 U2 4 PU HINDAWI PUBLISHING CORP PI NEW YORK PA 410 PARK AVENUE, 15TH FLOOR, #287 PMB, NEW YORK, NY 10022 USA SN 1687-6075 EI 1687-6083 J9 SCI TECHNOL NUCL INS JI Sci. Technol. Nucl. Install. PY 2013 AR 426356 DI 10.1155/2013/426356 PG 16 WC Nuclear Science & Technology SC Nuclear Science & Technology GA 078VZ UT WOS:000314129500001 ER PT J AU Russo, RE Mao, XL Gonzalez, JL Yoo, J AF Russo, Richard E. Mao, Xianglei Gonzalez, Jhanis L. Yoo, Jong TI Femtosecond Versus Nanosecond Laser Pulse Duration for Laser Ablation Chemical Analysis SO SPECTROSCOPY LA English DT Article ID PLASMA-MASS SPECTROMETRY; INDUCED BREAKDOWN SPECTROSCOPY; ICP-MS MEASUREMENTS; ENHANCED SENSITIVITY; SHOCK-WAVE; DYNAMICS; CARRIER; GLASS AB Laser ablation for direct solid sample chemical analysis has advanced over the past 50 years with applications in many disciplines, including environmental, geological, medical, energy, security, and others. Although the choice of laser is still highly dependent on the application requirements, there are distinct fundamental effects attributed to the laser pulse duration that drive the ablation sampling process. An overview of nanosecond and femtosecond laser ablation is presented with respect to analysis based on the optically induced plasma at the sample surface (such as laser-induced breakdown spectroscopy or laser ablation molecular isotopic spectrometry) and transport of the ablated mass aerosol to an inductively coupled plasma. C1 [Russo, Richard E.; Mao, Xianglei; Gonzalez, Jhanis L.] Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Russo, RE (reprint author), Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. FU Chemical Science Division, Office of Basic Energy Sciences; US Department of Energy (DOE) at the Lawrence Berkeley National Laboratory [DE-AC02-05CH11231]; DOE SBIR Program FX The authors-would like to thank Dr. Tim Suen for the design of the pulse-duration concept slides. R.E.R., X.L.M., and J.J.G. acknowledge support from the Chemical Science Division, Office of Basic Energy Sciences, and the Defense Nuclear Nonproliferation Research and Development Office of the US Department of Energy (DOE) under contract number DE-AC02-05CH11231 at the Lawrence Berkeley National Laboratory. J.Y. acknowledges support from the DOE SBIR Program. NR 59 TC 20 Z9 20 U1 3 U2 69 PU ADVANSTAR COMMUNICATIONS INC PI DULUTH PA 131 W 1ST STREET, DULUTH, MN 55802 USA SN 0887-6703 J9 SPECTROSCOPY-US JI Spectroscopy PD JAN PY 2013 VL 28 IS 1 BP 24 EP + PG 11 WC Spectroscopy SC Spectroscopy GA 079AG UT WOS:000314142000002 ER PT J AU Liedel, C Pester, CW Ruppel, M Lewin, C Pavan, MJ Urban, VS Shenhar, R Bosecke, P Boker, A AF Liedel, Clemens Pester, Christian W. Ruppel, Markus Lewin, Christian Pavan, Mariela J. Urban, Volker S. Shenhar, Roy Boesecke, Peter Boeker, Alexander TI Block Copolymer Nanocomposites in Electric Fields: Kinetics of Alignment SO ACS MACRO LETTERS LA English DT Article ID SYMMETRIC DIBLOCK COPOLYMERS; THIN-FILMS; POLYMER BLENDS; MICRODOMAIN ORIENTATION; UNDULATION INSTABILITY; MICROSCOPIC MECHANISM; MICROPHASE SEPARATION; DOMAIN ALIGNMENT; MAGNETIC-FIELDS; NANOPARTICLES AB We investigate the kinetics of block copolymer/nanoparticle composite alignment in an electric field using in situ transmission small-angle X-ray scattering. As a model system, we employ a lamellae forming polystyrene-block-poly(2-vinyl pyridine) block copolymer with different contents of gold nanoparticles in thick films under solvent vapor annealing. While the alignment improves with increasing nanoparticle fraction, the kinetics slows down. This is explained by changes in the degree of phase separation and viscosity. Our findings provide extended insights into the basics of nanocomposite alignment. C1 [Boeker, Alexander] Rhein Westfal TH Aachen, JARA FIT, D-52056 Aachen, Germany. [Liedel, Clemens; Pester, Christian W.; Lewin, Christian; Boeker, Alexander] DWI RWTH Aachen eV, D-52056 Aachen, Germany. [Ruppel, Markus] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. [Pavan, Mariela J.; Shenhar, Roy] Hebrew Univ Jerusalem, Inst Chem, IL-91904 Jerusalem, Israel. [Pavan, Mariela J.; Shenhar, Roy] Hebrew Univ Jerusalem, Ctr Nanosci & Nanotechnol, IL-91904 Jerusalem, Israel. [Urban, Volker S.] Oak Ridge Natl Lab, Biol & Soft Matter Div, Oak Ridge, TN 37831 USA. [Boesecke, Peter] European Synchrotron Radiat Facil, F-38043 Grenoble, France. RP Boker, A (reprint author), Rhein Westfal TH Aachen, JARA FIT, Forckenbeckstr 50, D-52056 Aachen, Germany. EM boeker@dwi.rwth-aachen.de RI Boker, Alexander/C-2055-2009; Shenhar, Roy/D-8160-2011; Urban, Volker/N-5361-2015; Liedel, Clemens/A-6671-2016 OI Boker, Alexander/0000-0002-5760-6631; Shenhar, Roy/0000-0002-0631-1542; Urban, Volker/0000-0002-7962-3408; Liedel, Clemens/0000-0002-2323-9431 FU ESRF; European Union; German Science Foundation (DFG) [BO 2475/5-1]; U.S. Department of Energy, Office of Science, Basic Energy Science, Materials Science and Engineering Division FX Our scattering experiments were performed on the ID2 beamline at the European Synchrotron Radiation Facility (ESRF), Grenoble, France. We thank Klaus Kreuels and Zhirong Fan for assistance, Theyencheri Narayanan for affording additional beam time, and we are grateful to the ESRF for financial support and provision of synchrotron beam time. C.L., C.W.P., M.J.P., RS., and A.B. thank the European Union and the German Science Foundation (DFG, BO 2475/5-1) for financial support in the framework of the ERA-NanoSci-E+ project MEMORY. M.R. and V.S.U. were supported by the U.S. Department of Energy, Office of Science, Basic Energy Science, Materials Science and Engineering Division. NR 77 TC 17 Z9 17 U1 5 U2 81 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 2161-1653 J9 ACS MACRO LETT JI ACS Macro Lett. PD JAN PY 2013 VL 2 IS 1 BP 53 EP 58 DI 10.1021/mz3005132 PG 6 WC Polymer Science SC Polymer Science GA 071PF UT WOS:000313606000014 ER PT J AU Singh, ARP Nag, S Chattopadhyay, S Ren, Y Tiley, J Viswanathan, GB Fraser, HL Banerjee, R AF Singh, A. R. P. Nag, S. Chattopadhyay, S. Ren, Y. Tiley, J. Viswanathan, G. B. Fraser, H. L. Banerjee, R. TI Mechanisms related to different generations of gamma ' precipitation during continuous cooling of a nickel base superalloy SO ACTA MATERIALIA LA English DT Article DE Nickel base superalloy; Rene 88 DT; Generations, Nucleation; Spinodal decomposition; Atom probe tomography; EFTEM ID ATOM-PROBE TOMOGRAPHY; SIZE DISTRIBUTIONS; DECOMPOSITION; ALLOYS AB This paper focuses on developing a mechanistic understanding of the process of multiple nucleation bursts leading to the formation of multiple generations (or populations) of gamma' precipitates with different size distributions, during the continuous cooling of a commercially used nickel base superalloy. This mechanistic understanding has been developed based on a number of critical experimental results: direct observation of the multiple nucleation bursts during in situ X-ray diffraction studies in the synchrotron, characterization of the size distributions associated with the different populations of gamma' precipitates by coupling multiple imaging techniques at the appropriate length scale and detailed compositional analysis of the gamma' precipitates as well as the gamma matrix using atom probe tomography. These analyses reveal that while local compositional equilibrium appears to have been achieved near the gamma'/gamma interface for the first generation of precipitates, a non-equilibrium long range diffusion profile in the gamma matrix is retained during the process of continuous cooling, which is largely responsible for the subsequent nucleation bursts at larger undercooling (or lower temperatures), leading to second and third generations of precipitates. Additionally, since these subsequent generations of precipitates are formed at larger undercoolings, they are typically finer in size scale, exhibit far-from equilibrium compositions and also have very diffuse gamma'/gamma interfaces, indicating a non-classical precipitation mechanism associated with their formation. (C) 2012 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved. C1 [Singh, A. R. P.; Nag, S.; Banerjee, R.] Univ N Texas, Ctr Adv Res & Technol, Denton, TX 76203 USA. [Singh, A. R. P.; Nag, S.; Banerjee, R.] Univ N Texas, Dept Mat Sci & Engn, Denton, TX 76203 USA. [Chattopadhyay, S.] Argonne Natl Lab, Adv Photon Source, MRCAT, CSRRI IIT, Argonne, IL 60439 USA. [Chattopadhyay, S.] IIT, Dept Phys, Chicago, IL 60616 USA. [Tiley, J.; Viswanathan, G. B.] USAF, Res Lab, Mat & Mfg Directorate, Dayton, OH USA. [Fraser, H. L.] Ohio State Univ, Ctr Accelerated Maturat Mat, Columbus, OH 43210 USA. [Fraser, H. L.] Ohio State Univ, Dept Mat Sci & Engn, Columbus, OH 43210 USA. [Ren, Y.] Argonne Natl Lab, Adv Photon Source, Xray Sci Div, Argonne, IL 60439 USA. RP Banerjee, R (reprint author), Univ N Texas, Ctr Adv Res & Technol, Denton, TX 76203 USA. EM rajarshi.banerjee@unt.edu FU US Air Force Research Laboratory (AFRL ISES) [FA8650-08-C-5226]; US Department of Energy, Office of Science, and Office of Basic Energy Science [DE-AC02-06CH11357] FX The authors would like to acknowledge the US Air Force Research Laboratory (AFRL ISES contract FA8650-08-C-5226) for providing financial support for this study. In addition, the authors also gratefully acknowledge the Center for Advanced Research and Technology (CART) at the University of North Texas and the Center for the Accelerated Maturation of Materials (CAMM) at the Ohio State University for access to the experimental facilities used for this study. The use of the Advanced Photon Source was supported by the US Department of Energy, Office of Science, and Office of Basic Energy Science under Contract No. DE-AC02-06CH11357. NR 28 TC 22 Z9 22 U1 5 U2 61 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 1359-6454 EI 1873-2453 J9 ACTA MATER JI Acta Mater. PD JAN PY 2013 VL 61 IS 1 BP 280 EP 293 DI 10.1016/j.actamat.2012.09.058 PG 14 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Materials Science; Metallurgy & Metallurgical Engineering GA 071OP UT WOS:000313604400026 ER PT J AU Qu, DD Liss, KD Sun, YJ Reid, M Almer, JD Yan, K Wang, YB Liao, XZ Shen, J AF Qu, D. D. Liss, K. -D. Sun, Y. J. Reid, M. Almer, J. D. Yan, K. Wang, Y. B. Liao, X. Z. Shen, J. TI Structural origins for the high plasticity of a Zr-Cu-Ni-Al bulk metallic glass SO ACTA MATERIALIA LA English DT Article DE Bulk metallic glass; Plasticity; In situ high-energy X-ray diffraction; Structural anisotropy ID AMORPHOUS SOLIDS; SHEAR BANDS; DEFORMATION; ANISOTROPY; ALLOYS; COMPOSITES; TRANSITION; MECHANISM AB The structural origins for the high plasticity of a Zr53Cu18.7Ni12Al16.3 (at.%) bulk metallic glass are explored. Under plastic flow conditions, in situ synchrotron high-energy X-ray diffraction reveals that the atomic strain saturates to the closest packing in the longitudinal direction of the applied load while atoms yield in the transverse plane. Scanning electron microscopy investigation reveals that global plasticity benefits from abundant shear band multiplication and interactions. Atomic level flows are seen to accompany profuse shear bands. The plasticity enhancement of this metallic glass benefits from such atomic level flows. Atomic level flow facilitates the activation of shear transformation zones that further self-assemble to promote shear band multiplication. On the other hand, it also mitigates the shear band propagation that prevents catastrophic shear band extension. (C) 2012 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved. C1 [Qu, D. D.; Shen, J.] Harbin Inst Technol, Sch Mat Sci & Engn, Harbin 150001, Peoples R China. [Liss, K. -D.; Yan, K.] Australian Nucl Sci & Technol Org, Lucas Heights, NSW 2234, Australia. [Sun, Y. J.] Tianjin Polytech Univ, Sch Sci, Dept Phys, Tianjin 300387, Peoples R China. [Reid, M.; Yan, K.] Univ Wollongong, Fac Engn, Wollongong, NSW 2522, Australia. [Almer, J. D.] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. [Wang, Y. B.; Liao, X. Z.] Univ Sydney, Sch Aerosp Mech & Mechatron Engn, Sydney, NSW 2006, Australia. RP Shen, J (reprint author), Harbin Inst Technol, Sch Mat Sci & Engn, Harbin 150001, Peoples R China. EM junshen@hit.edu.cn RI Liao, Xiaozhou/B-3168-2009; Wang, Yanbo/B-3175-2009; Liss, Klaus-Dieter/E-8548-2011; Qu, Dongdong/G-4521-2011 OI Liao, Xiaozhou/0000-0001-8565-1758; Liss, Klaus-Dieter/0000-0003-4323-0343; FU National Natural Science Foundation of China [51025415]; Australian Research Council; Commonwealth of Australia under the National Collaborative Research Infrastructure Strategy FX The X-ray diffraction was enabled through the ANSTO Senior Research Fellowship Program. The synchrotron beam time at APS was granted and travel supported through the Australian Synchrotron Research Program, funded by the Commonwealth of Australia under the National Collaborative Research Infrastructure Strategy. This work is supported by the National Natural Science Foundation of China under the Grant No. 51025415, and the Australian Research Council. We acknowledge W. Zheng and X.S. Wei for the sample preparation. NR 48 TC 12 Z9 12 U1 3 U2 107 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 1359-6454 J9 ACTA MATER JI Acta Mater. PD JAN PY 2013 VL 61 IS 1 BP 321 EP 330 DI 10.1016/j.actamat.2012.09.062 PG 10 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Materials Science; Metallurgy & Metallurgical Engineering GA 071OP UT WOS:000313604400029 ER PT J AU Yang, ZQ Chisholm, MF Duscher, G Ma, XL Pennycook, SJ AF Yang, Zhiqing Chisholm, Matthew F. Duscher, Gerd Ma, Xiuliang Pennycook, Stephen J. TI Direct observation of dislocation dissociation and Suzuki segregation in a Mg-Zn-Y alloy by aberration-corrected scanning transmission electron microscopy SO ACTA MATERIALIA LA English DT Article DE Dislocation; Stacking fault; Suzuki segregation; Strength; Mg alloy ID STACKING-FAULT ENERGIES; MAGNESIUM; DEFORMATION; 1ST-PRINCIPLES; TEMPERATURE; SUPERALLOY; STRENGTH; METALS; PHASE AB Crystal defects in a plastically deformed Mg-Zn-Y alloy have been studied on the atomic scale using aberration-corrected scanning transmission electron microscopy, providing important structural data for understanding the material's deformation behavior and strengthening mechanisms. Atomic scale structures of deformation stacking faults resulting from dissociation of different types of dislocations have been characterized experimentally, and modeled. Suzuki segregation of Zn and Y along stacking faults formed through dislocation dissociation during plastic deformation at 300 degrees C is confirmed experimentally on the atomic level. The stacking fault energy of the Mg-Zn-Y alloy is evaluated to be in the range of 4.0-10.3 mJ m(-2). The newly formed nanometer-wide stacking faults with their Zn/Y segregation in Mg grains play an important role in the superior strength of this alloy at elevated temperatures. (C) 2012 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved. C1 [Yang, Zhiqing; Ma, Xiuliang] Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China. [Yang, Zhiqing; Chisholm, Matthew F.; Duscher, Gerd; Pennycook, Stephen J.] Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. [Yang, Zhiqing; Duscher, Gerd; Pennycook, Stephen J.] Univ Tennessee, Dept Mat Sci & Engn, Knoxville, TN 37996 USA. RP Yang, ZQ (reprint author), Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China. EM yangzq34@yahoo.com RI Yang, Zhiqing/E-5188-2011; Duscher, Gerd/G-1730-2014 OI Yang, Zhiqing/0000-0003-2017-6583; Duscher, Gerd/0000-0002-2039-548X FU US Department of Energy, Office of Basic Energy Sciences, Materials Sciences and Engineering Division; NSFC [51171189]; MoST of China [2009BC623705]; NSF of Liaoning Province; Scientific User Facilities Division, Office of Basic Energy Sciences, US Department of Energy FX ZQY, MFC and SJP are supported by the US Department of Energy, Office of Basic Energy Sciences, Materials Sciences and Engineering Division. ZQY thanks the NSFC (51171189), the MoST of China (2009BC623705) and the NSF of Liaoning Province for support. Instrument access was provided by Oak Ridge National Laboratory's ShaRE User Facility, which is sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, US Department of Energy. NR 33 TC 34 Z9 35 U1 5 U2 93 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 1359-6454 J9 ACTA MATER JI Acta Mater. PD JAN PY 2013 VL 61 IS 1 BP 350 EP 359 DI 10.1016/j.actamat.2012.09.067 PG 10 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Materials Science; Metallurgy & Metallurgical Engineering GA 071OP UT WOS:000313604400032 ER PT J AU Miles, PC Li, B Li, ZS Alden, M AF Miles, Paul C. Li, Bo Li, Zhongshan Alden, Marcus TI Atmospheric Pressure Acetylene Detection by UV Photo-Fragmentation and Induced C-2 Emission SO APPLIED SPECTROSCOPY LA English DT Article DE Ultraviolet Photo-fragmentation; Acetylene detection; C-2 Swan band; Fluorescence ID VIBRATION-ROTATION CONSTANTS; X BAND SYSTEM; WAVELENGTH BANDS; PREDISSOCIATION; DISSOCIATION; SPECTROSCOPY; FLAMES; STATE; C2H2 AB Detection of C2H2 via UV photo-fragmentation, followed by monitoring the C(2)d(3)Pi(g)-a(3)Pi(u) fluorescence, is explored at atmospheric pressure and at temperatures of 295 K, 600 K, and 800 K, for excitation wavelengths 210 to 240 am using a broadband laser source (similar to 3 cm(-1) fwhm). At the lower temperature, C-2 emissions correlate closely with C2H2 (A) over tilde <- X absorption bands, and the excitation spectra suggest a higher-transition probability for the v(4)'' = 2 and 3 states than for the v(4)'' = 0 and 1 states. As temperature increases, the excitation spectra exhibit a higher nonresonant background. C1 [Miles, Paul C.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. [Li, Bo; Li, Zhongshan; Alden, Marcus] Lund Univ, Div Combust Phys, S-22100 Lund, Sweden. RP Li, ZS (reprint author), Lund Univ, Div Combust Phys, POB 118, S-22100 Lund, Sweden. EM zhongshan.li@forbrf.lth.se RI Li, Bo/M-2187-2015; OI Li, Bo/0000-0002-4436-926X; Li, Zhongshan/0000-0002-0447-2748 FU CECOST through the Energy Agency; CECOST through Foundation for Strategic Research, SSF; ERC; United States Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX This work was performed at the Department of Combustion Physics at Lund University and at the Combustion Research Facility of Sandia National Laboratories. The authors gratefully acknowledge Scania AB for financial support for this work; Joakim Bood and David Osborn for helpful technical discussions; and Oivind Andersson and Bengt Johansson of the Lund University Department of Energy Sciences for facilitating this collaboration. The Lund University authors acknowledge CECOST (through the Energy Agency and the Foundation for Strategic Research, SSF) and ERC (through the Advanced Grant 'DALDECS') for financial support. Sandia is a multi-program laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the United States Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000. NR 14 TC 3 Z9 3 U1 1 U2 10 PU SOC APPLIED SPECTROSCOPY PI FREDERICK PA 5320 SPECTRUM DRIVE SUITE C, FREDERICK, MD 21703 USA SN 0003-7028 J9 APPL SPECTROSC JI Appl. Spectrosc. PD JAN PY 2013 VL 67 IS 1 BP 66 EP 72 DI 10.1366/12-06731 PG 7 WC Instruments & Instrumentation; Spectroscopy SC Instruments & Instrumentation; Spectroscopy GA 071ON UT WOS:000313604200009 PM 23317673 ER PT J AU Zhang, W Howell, L Almgren, A Burrows, A Dolence, J Bell, J AF Zhang, W. Howell, L. Almgren, A. Burrows, A. Dolence, J. Bell, J. TI CASTRO: A NEW COMPRESSIBLE ASTROPHYSICAL SOLVER. III. MULTIGROUP RADIATION HYDRODYNAMICS SO ASTROPHYSICAL JOURNAL SUPPLEMENT SERIES LA English DT Article DE diffusion; hydrodynamics; methods: numerical; radiative transfer ID CORE-COLLAPSE SUPERNOVAE; HYPERBOLIC CONSERVATION-LAWS; SPECTRAL NEUTRINO TRANSPORT; EQUATION-OF-STATE; CIRCLE-DOT STAR; EFFICIENT IMPLEMENTATION; EDDINGTON FACTORS; NUMERICAL-METHOD; NUCLEAR-MATTER; DIFFUSION AB We present a formulation for multigroup radiation hydrodynamics that is correct to order O(v/c) using the comoving-frame approach and the flux-limited diffusion approximation. We describe a numerical algorithm for solving the system, implemented in the compressible astrophysics code, CASTRO. CASTRO uses a Eulerian grid with block-structured adaptive mesh refinement based on a nested hierarchy of logically rectangular variable-sized grids with simultaneous refinement in both space and time. In our multigroup radiation solver, the system is split into three parts: one part that couples the radiation and fluid in a hyperbolic subsystem, another part that advects the radiation in frequency space, and a parabolic part that evolves radiation diffusion and source-sink terms. The hyperbolic subsystem and the frequency space advection are solved explicitly with high-order Godunov schemes, whereas the parabolic part is solved implicitly with a first-order backward Euler method. Our multigroup radiation solver works for both neutrino and photon radiation. C1 [Zhang, W.; Almgren, A.; Bell, J.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Ctr Computat Sci & Engn, Berkeley, CA 94720 USA. [Howell, L.] Lawrence Livermore Natl Lab, Ctr Appl Sci Comp, Livermore, CA 94550 USA. [Burrows, A.; Dolence, J.] Princeton Univ, Dept Astrophys Sci, Princeton, NJ 08544 USA. RP Zhang, W (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Ctr Computat Sci & Engn, Berkeley, CA 94720 USA. OI Dolence, Joshua/0000-0003-4353-8751 FU Office of High Energy Physics; Office of Advanced Scientific Computing Research of the U.S. Department of Energy [DE-AC02-05CH11231]; SciDAC program of the U.S. Department of Energy [DE-AC52-07NA27344]; SciDAC program of DOE [DE-FG02-08ER41544]; NSF [ND201387]; NSF PetaApps program from Louisiana State University [OCI-0905046, 44592]; Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231] FX The work at LBNL was supported by the Office of High Energy Physics and the Office of Advanced Scientific Computing Research of the U.S. Department of Energy under contract No. DE-AC02-05CH11231. The work performed at LLNL was supported by the SciDAC program of the U.S. Department of Energy under the auspices of contract No. DE-AC52-07NA27344. Adam Burrows was supported by the SciDAC program of DOE under grant number DE-FG02-08ER41544, the NSF under subaward No. ND201387 to the Joint Institute for Nuclear Astrophysics, and the NSF PetaApps program, under award OCI-0905046 via a subaward No. 44592 from Louisiana State University to Princeton University. 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. The authors would like to thank S. E. Woosley for many useful comments on the manuscript. NR 68 TC 18 Z9 18 U1 0 U2 9 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 0067-0049 J9 ASTROPHYS J SUPPL S JI Astrophys. J. Suppl. Ser. PD JAN PY 2013 VL 204 IS 1 AR UNSP 7 DI 10.1088/0067-0049/204/1/7 PG 27 WC Astronomy & Astrophysics SC Astronomy & Astrophysics GA 070NN UT WOS:000313515500007 ER PT J AU Yokelson, RJ Burling, IR Gilman, JB Warneke, C Stockwell, CE de Gouw, J Akagi, SK Urbanski, SP Veres, P Roberts, JM Kuster, WC Reardon, J Griffith, DWT Johnson, TJ Hosseini, S Miller, JW Cocker, DR Jung, H Weise, DR AF Yokelson, R. J. Burling, I. R. Gilman, J. B. Warneke, C. Stockwell, C. E. de Gouw, J. Akagi, S. K. Urbanski, S. P. Veres, P. Roberts, J. M. Kuster, W. C. Reardon, J. Griffith, D. W. T. Johnson, T. J. Hosseini, S. Miller, J. W. Cocker, D. R., III Jung, H. Weise, D. R. TI Coupling field and laboratory measurements to estimate the emission factors of identified and unidentified trace gases for prescribed fires SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID BIOMASS-BURNING EMISSIONS; TRANSFORM INFRARED-SPECTROSCOPY; VOLATILE ORGANIC-COMPOUNDS; GROUND-BASED MEASUREMENTS; UNITED-STATES; PARTICLE EMISSIONS; TROPICAL FOREST; SOUTH-AFRICA; ATMOSPHERIC CHEMISTRY; MASS-SPECTROMETRY AB An extensive program of experiments focused on biomass burning emissions began with a laboratory phase in which vegetative fuels commonly consumed in prescribed fires were collected in the southeastern and southwestern US and burned in a series of 71 fires at the US Forest Service Fire Sciences Laboratory in Missoula, Montana. The particulate matter (PM2.5) emissions were measured by gravimetric filter sampling with subsequent analysis for elemental carbon (EC), organic carbon (OC), and 38 elements. The trace gas emissions were measured by an open-path Fourier transform infrared (OP-FTIR) spectrometer, proton-transfer-reaction mass spectrometry (PTRMS), proton-transfer ion-trap mass spectrometry (PIT-MS), negative-ion proton-transfer chemical-ionization mass spectrometry (NI-PT-CIMS), and gas chromatography with MS detection (GC-MS). 204 trace gas species (mostly non-methane organic compounds (NMOC)) were identified and quantified with the above instruments. Many of the 182 species quantified by the GC-MS have rarely, if ever, been measured in smoke before. An additional 153 significant peaks in the unit mass resolution mass spectra were quantified, but either could not be identified or most of the signal at that molecular mass was unaccounted for by identifiable species. In a second, "field" phase of this program, airborne and ground-based measurements were made of the emissions from prescribed fires that were mostly located in the same land management units where the fuels for the lab fires were collected. A broad variety, but smaller number of species (21 trace gas species and PM2.5) was measured on 14 fires in chaparral and oak savanna in the southwestern US, as well as pine forest understory in the southeastern US and Sierra Nevada mountains of California. The field measurements of emission factors (EF) are useful both for modeling and to examine the representativeness of our lab fire EF. The lab EF/field EF ratio for the pine understory fuels was not statistically different from one, on average. However, our lab EF for "smoldering compounds" emitted from the semiarid shrubland fuels should likely be increased by a factor of similar to 2.7 to better represent field fires. Based on the lab/field comparison, we present emission factors for 357 pyrogenic species (including unidentified species) for 4 broad fuel types: pine understory, semiarid shrublands, coniferous canopy, and organic soil. To our knowledge this is the most comprehensive measurement of biomass burning emissions to date and it should enable improved representation of smoke composition in atmospheric models. The results support a recent estimate of global NMOC emissions from biomass burning that is much higher than widely used estimates and they provide important insights into the nature of smoke. 31-72% of the mass of gas-phase NMOC species was attributed to species that we could not identify. These unidentified species are not represented in most models, but some provision should be made for the fact that they will react in the atmosphere. In addition, the total mass of gas-phase NMOC divided by the mass of co-emitted PM2.5 averaged about three (range similar to 2.0-8.7). About 35-64% of the NMOC were likely semivolatile or of intermediate volatility. Thus, the gas-phase NMOC represent a large reservoir of potential precursors for secondary formation of ozone and organic aerosol. For the single lab fire in organic soil about 28% of the emitted carbon was present as gas-phase NMOC and similar to 72% of the mass of these NMOC was unidentified, highlighting the need to learn more about the emissions from smoldering organic soils. The mass ratio of total NMOC to "NOx as NO" ranged from 11 to 267, indicating that NOx-limited O-3 production would be common in evolving biomass burning plumes. The fuel consumption per unit area was 7.0 +/- 2.3 Mg ha(-1) and 7.7 +/- 3.7 Mg ha(-1) for pine-understory and semiarid shrubland prescribed fires, respectively. C1 [Yokelson, R. J.; Burling, I. R.; Stockwell, C. E.; Akagi, S. K.] Univ Montana, Dept Chem, Missoula, MT 59812 USA. [Gilman, J. B.; Warneke, C.; de Gouw, J.; Roberts, J. M.; Kuster, W. C.] Univ Colorado, Cooperat Inst Res Environm Sci, Boulder, CO 80309 USA. [Gilman, J. B.; Warneke, C.; de Gouw, J.; Roberts, J. M.; Kuster, W. C.] Natl Ocean & Atmospher Adm, Div Chem Sci, Earth Syst Res Lab, Boulder, CO 80305 USA. [Urbanski, S. P.] US Forest Serv, USDA, Rocky Mt Res Stn, Fire Sci Lab, Missoula, MT 59808 USA. [Veres, P.] Max Planck Inst Chem, Dept Atmospher Chem, D-55128 Mainz, Germany. [Griffith, D. W. T.] Univ Wollongong, Sch Chem, Wollongong, NSW 2522, Australia. [Johnson, T. J.] Pacific NW Natl Lab, Richland, WA 99354 USA. [Jung, H.] Univ Calif Riverside, Dept Mech Engn, Riverside, CA 92521 USA. [Cocker, D. R., III; Jung, H.] Univ Calif Riverside, Coll Engn, Ctr Environm Res & Technol CE CERT, Riverside, CA 92521 USA. [Cocker, D. R., III] Univ Calif Riverside, Dept Chem & Environm Engn, Riverside, CA 92521 USA. [Weise, D. R.] US Forest Serv, USDA, Pacific SW Res Stn, Forest Fire Lab, Riverside, CA USA. RP Yokelson, RJ (reprint author), Univ Montana, Dept Chem, Missoula, MT 59812 USA. EM bob.yokelson@umontana.edu RI Veres, Patrick/E-7441-2010; Warneke, Carsten/E-7174-2010; Roberts, James/A-1082-2009; Kuster, William/E-7421-2010; Gilman, Jessica/E-7751-2010; Yokelson, Robert/C-9971-2011; Cocker, David/F-4442-2010; de Gouw, Joost/A-9675-2008; Manager, CSD Publications/B-2789-2015; OI Veres, Patrick/0000-0001-7539-353X; Roberts, James/0000-0002-8485-8172; Kuster, William/0000-0002-8788-8588; Gilman, Jessica/0000-0002-7899-9948; Yokelson, Robert/0000-0002-8415-6808; Cocker, David/0000-0002-0586-0769; de Gouw, Joost/0000-0002-0385-1826; Jung, Heejung/0000-0003-0366-7284 FU Strategic Environmental Research and Development Program (SERDP) [RC-1648, RC-1649]; National Science Foundation (NSF) [ATM 1542457]; CIRES Innovative Research Program; NOAA; NSF [ATM 0513055, ATM 0936321]; Joint Fire Science Program [08-1-6-09] FX This work was supported by the Strategic Environmental Research and Development Program (SERDP) projects RC-1648 and RC-1649 and administered partly through Forest Service Research Joint Venture Agreement 08JV11272166039, and we thank the sponsors for their support. J. Gilman, W. Kuster, P. Veres, J. M. Roberts, C. Warneke, and J. de Gouw were supported in part by National Science Foundation (NSF) Grant No. ATM 1542457, the CIRES Innovative Research Program, and NOAA's Health of the Atmosphere and Climate Goals Programs. We appreciate the efforts of Joey Chong, Bonni Corcoran, Amy Olson, Violet Holley, Signe Leirfallom, Anna Lahde, Jehn Rawling, Greg Cohen, and Emily Lincoln to sample/harvest the wildland fuels and/or assemble the laboratory fuel beds for this study. Adaptation of the USFS Twin Otter for research flights was supported primarily by NSF Grant No. ATM 0513055. R. Y., S. A., and multiple instruments aboard the Twin Otter were also supported by NSF Grant No. ATM 0936321. Shawn Urbanski was supported partially by Joint Fire Science Program grant 08-1-6-09. Special thanks to our pilots Scott Miller and Aaron Knobloch and Twin Otter mechanic Kevin Bailey. The cooperation of Dan Ardoin and personnel at Vandenberg AFB, Jeff Minetti and personnel at Ft. Hunter-Liggett, Andrew Leiendecker and personnel at Ft. Huachuca, John Maitland and personnel at Fort Jackson, and Danny Becker, Susan Cohen, and Wayne Gray at Camp Lejeune is greatly appreciated. We greatly appreciate other collaborators and support on the ground including: Gary Curcio (North Carolina Division of Forest Resources), Phillip Inman and Miller Casion (NC county rangers), Andrew Robillard (San Luis Jet Center), Jason McCarty (SBCFD), Brendan Ripley (VCFD), Angie Carl (The Nature Conservancy), and additional fuels characterization assistance from Gloria Burke, Ania Wrona, and Jesse Lozano. NR 97 TC 76 Z9 76 U1 4 U2 159 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 2013 VL 13 IS 1 BP 89 EP 116 DI 10.5194/acp-13-89-2013 PG 28 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA 070NA UT WOS:000313513700007 ER PT J AU Burrows, SM Hoose, C Poschl, U Lawrence, MG AF Burrows, S. M. Hoose, C. Poeschl, U. Lawrence, M. G. TI Ice nuclei in marine air: biogenic particles or dust? SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID SEA-SURFACE MICROLAYER; ORGANIC AEROSOL-PARTICLES; SUBMODEL SYSTEM MESSY; CENTRAL ARCTIC-OCEAN; FORMING NUCLEI; TECHNICAL NOTE; SPRAY AEROSOL; OXALIC-ACID; BACTERIAL ENRICHMENT; BIOLOGICAL PARTICLES AB Ice nuclei impact clouds, but their sources and distribution in the atmosphere are still not well known. Particularly little attention has been paid to IN sources in marine environments, although evidence from field studies suggests that IN populations in remote marine regions may be dominated by primary biogenic particles associated with sea spray. In this exploratory model study, we aim to bring attention to this long-neglected topic and identify promising target regions for future field campaigns. We assess the likely global distribution of marine biogenic ice nuclei using a combination of historical observations, satellite data and model output. By comparing simulated marine biogenic immersion IN distributions and dust immersion IN distributions, we predict strong regional differences in the importance of marine biogenic IN relative to dust IN. Our analysis suggests that marine biogenic IN are most likely to play a dominant role in determining IN concentrations in near-surface-air over the Southern Ocean, so future field campaigns aimed at investigating marine biogenic IN should target that region. Climate-related changes in the abundance and emission of biogenic marine IN could affect marine cloud properties, thereby introducing previously unconsidered feedbacks that influence the hydrological cycle and the Earth's energy balance. Furthermore, marine biogenic IN may be an important aspect to consider in proposals for marine cloud brightening by artificial sea spray production. C1 [Burrows, S. M.; Poeschl, U.; Lawrence, M. G.] Max Planck Inst Chem, D-55128 Mainz, Germany. [Hoose, C.] Karlsruhe Inst Technol, Inst Meteorol & Climate Res Atmospher Aerosol Res, D-76021 Karlsruhe, Germany. RP Burrows, SM (reprint author), Pacific NW Natl Lab, Richland, WA 99352 USA. EM susannah.burrows@pnnl.gov RI Burrows, Susannah/A-7429-2011; Hoose, Corinna/A-4295-2009; Poschl, Ulrich/A-6263-2010 OI Burrows, Susannah/0000-0002-0745-7252; Hoose, Corinna/0000-0003-2827-5789; Poschl, Ulrich/0000-0003-1412-3557 FU Max Planck Graduate Center; Johannes Gutenberg-Universitat Mainz; European Commission under PEGASOS [265148]; President's Initiative and Networking Fund of the Helmholtz Association; DOE Office of Science Biological and Environmental Research Program under their Earth System Modeling Program; DOE [DE-AC06-76RLO 1830] FX We wish to thank the EMAC development team, particularly Patrick Jockel, Holger Tost and Astrid Kerkweg, for their support in the use of the model and in trouble-shooting, Michael Schulz and coworkers for preparing and providing us with access to the AEROCOM median model data, Jean-Francois Lamarque and colleagues for preparing and making publically available the IPCC AR5 anthropogenic emissions dataset including ship emissions, and Elisabetta Vignati for providing original raw data for Fig. 2b. We would like to thank Gerhild Feyerherd for her support in preparing Fig. 1; Tasnim Pooya helped assemble the data for Fig. A1. We would like to thank Jos Lelieveld and Andy Heymsfield, and two anonymous reviewers for their comments on earlier versions of this manuscript, and Gabor Vali and an anonymous referee for comments on the ACPD manuscript version. Hailong Wang suggested the possiblity of implications for marine cloud brightening schemes. Susannah Burrows' work was supported in part by the Max Planck Graduate Center with Johannes Gutenberg-Universitat Mainz, and hosted by the International Max Planck Research School for Atmospheric Chemistry and Physics. Susannah Burrows and Ulrich Poschl acknowledge support by the European Commission under the project PEGASOS (grant no. 265148). Corinna Hoose acknowledges support by the President's Initiative and Networking Fund of the Helmholtz Association. This work was partially funded by the the DOE Office of Science Biological and Environmental Research Program under their Earth System Modeling Program. The Pacific Northwest National Laboratory is operated for DOE by Battelle Memorial Institute under contract DE-AC06-76RLO 1830. NR 146 TC 51 Z9 52 U1 5 U2 107 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 2013 VL 13 IS 1 BP 245 EP 267 DI 10.5194/acp-13-245-2013 PG 23 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA 070NA UT WOS:000313513700016 ER PT J AU Villa, A Veith, GM Ferri, D Weidenkaff, A Perry, KA Campisi, S Prati, L AF Villa, Alberto Veith, Gabriel M. Ferri, Davide Weidenkaff, Anke Perry, Kelly A. Campisi, Sebastiano Prati, Laura TI NiO as a peculiar support for metal nanoparticles in polyols oxidation SO CATALYSIS SCIENCE & TECHNOLOGY LA English DT Article ID LIQUID-PHASE OXIDATION; MODIFIED TIO2 SUPPORT; SELECTIVE OXIDATION; GOLD CATALYSTS; SOL-GEL; CARBON-MONOXIDE; ALCOHOLS; GLYCEROL; AU; HYDROGENATION AB The peculiar influence of a NiO support was studied by preparing gold catalysts supported on NiO1-x-TiO2 (x) mixed oxides. PVA protected Au nanoparticles showed high activity when supported on NiO for the selective oxidation of glycerol and ethane-1,2-diol. A detailed characterization of the resulting Au catalysts revealed a preferential deposition of the metal nanoparticles on the NiO phase. However, the activity of Au on NiO1-x-TiO2 (x) decreased with respect to pure NiO and the selectivity evolved with changes in the support. C1 [Villa, Alberto; Campisi, Sebastiano] Univ Milan, Dipartimento Chim, I-20133 Milan, Italy. [Veith, Gabriel M.; Perry, Kelly A.; Prati, Laura] Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN 37831 USA. [Ferri, Davide; Weidenkaff, Anke] Empa Lab Solid State Chem & Catalysis, CH-8600 Dubendorf, Switzerland. RP Villa, A (reprint author), Univ Milan, Dipartimento Chim, Via Golgi 19, I-20133 Milan, Italy. EM Laura.Prati@unimi.it RI Villa, Alberto/H-7355-2013; Campisi, Sebastiano/N-9722-2013; Weidenkaff, Anke/B-7808-2014; Prati, Laura/Q-3970-2016; OI Villa, Alberto/0000-0001-8656-6256; Weidenkaff, Anke/0000-0002-7021-1765; Prati, Laura/0000-0002-8227-9505; Ferri, Davide/0000-0002-9354-5231 FU Oak Ridge National Laboratory; Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy; Fondazione Cariplo; Empa FX A portion of 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 (GMV, KAP) and was performed at Oak Ridge National Laboratory's SHaRE User Facility (TEM), which is sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy. Fondazione Cariplo and Empa are also gratefully acknowledged for financial support. Dr S. Yoon and O. Brunko are thanked for XRD and XRF measurements, respectively. NR 34 TC 21 Z9 22 U1 0 U2 50 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2044-4753 EI 2044-4761 J9 CATAL SCI TECHNOL JI Catal. Sci. Technol. PY 2013 VL 3 IS 2 BP 394 EP 399 DI 10.1039/c2cy20370g PG 6 WC Chemistry, Physical SC Chemistry GA 070MW UT WOS:000313513000014 ER PT J AU Hasty, P Sharp, ZD Curiel, TJ Campisi, J AF Hasty, Paul Sharp, Zelton Dave Curiel, Tyler J. Campisi, Judith TI mTORC1 and p53 Clash of the gods? SO CELL CYCLE LA English DT Article DE mTORC1; p53; cellular senescence; cancer; aging ID GENETICALLY HETEROGENEOUS MICE; MAMMALIAN LIFE-SPAN; DNA-DAMAGE RESPONSE; PROTEIN S6 KINASE; CELL-CYCLE ARREST; TUMOR SUPPRESSION; FARNESYLTRANSFERASE INHIBITOR; EMBRYONIC LETHALITY; MDM2-DEFICIENT MICE; IN-VITRO AB A balance must be struck between cell growth and stress responses to ensure that cells proliferate without accumulating damaged DNA. This balance means that optimal cell proliferation requires the integration of pro-growth and stress-response pathways. mTOR (mechanistic target of rapamycin) is a pleiotropic kinase found in complex 1 (mTORC1). The mTORC1 pathway governs a response to mitogenic signals with high energy levels to promote protein synthesis and cell growth. In contrast, the p53 DNA damage response pathway is the arbiter of cell proliferation, restraining mTORC1 under conditions of genotoxic stress. Recent studies suggest a complicated integration of these pathways to ensure successful cell growth and proliferation without compromising genome maintenance. Deciphering this integration could be key to understanding the potential clinical usefulness of mTORC1 inhibitors like rapamycin. Here we discuss how these p53-mTORC1 interactions might play a role in the suppression of cancer and perhaps the development of cellular senescence and organismal aging. C1 [Hasty, Paul; Sharp, Zelton Dave] Univ Texas Hlth Sci Ctr San Antonio, Dept Mol Med, San Antonio, TX 78229 USA. [Hasty, Paul; Sharp, Zelton Dave] Univ Texas Hlth Sci Ctr San Antonio, Inst Biotechnol, San Antonio, TX 78229 USA. [Curiel, Tyler J.] Univ Texas Hlth Sci Ctr San Antonio, Dept Med, San Antonio, TX 78229 USA. [Hasty, Paul; Sharp, Zelton Dave; Curiel, Tyler J.] Univ Texas Hlth Sci Ctr San Antonio, Canc Therapy & Res Ctr, San Antonio, TX 78229 USA. [Campisi, Judith] Buck Inst Res Aging, Novato, CA USA. [Campisi, Judith] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Hasty, P (reprint author), Univ Texas Hlth Sci Ctr San Antonio, Dept Mol Med, San Antonio, TX 78229 USA. EM hastye@uthscsa.edu NR 66 TC 18 Z9 22 U1 0 U2 9 PU LANDES BIOSCIENCE PI AUSTIN PA 1806 RIO GRANDE ST, AUSTIN, TX 78702 USA SN 1538-4101 J9 CELL CYCLE JI Cell Cycle PD JAN 1 PY 2013 VL 12 IS 1 BP 20 EP 25 DI 10.4161/cc.22912 PG 6 WC Cell Biology SC Cell Biology GA 069DF UT WOS:000313414700012 PM 23255104 ER PT J AU Young, NJ Hay, BP AF Young, Neil J. Hay, Benjamin P. TI Structural design principles for self-assembled coordination polygons and polyhedra SO CHEMICAL COMMUNICATIONS LA English DT Article ID DE-NOVO DESIGN; HOST-GUEST INTERACTIONS; COMPUTER-AIDED-DESIGN; SUPRAMOLECULAR CHEMISTRY; CRYSTAL-STRUCTURES; RATIONAL DESIGN; BUILDING-BLOCKS; METALLOSUPRAMOLECULAR CHEMISTRY; MOLECULAR RECOGNITION; CHELATE COMPLEXES AB Strategies for the design of ligands that combine with metal ions to form high-symmetry coordination assemblies are reviewed. Evaluation of crystal structure evidence reveals that prior design approaches, based on the concept of complementary bonding vector angles, fail to predict the majority of known examples. After explaining the reasons for this failure, it is shown how an alternative approach, de novo structure-based design, provides a practical method that predicts a much wider range of component shapes encoded to direct the formation of such assemblies. C1 [Young, Neil J.; Hay, Benjamin P.] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. RP Hay, BP (reprint author), Oak Ridge Natl Lab, Div Chem Sci, POB 2008, Oak Ridge, TN 37831 USA. EM haybp@ornl.gov FU Oak Ridge National Laboratory by the Division of Chemical Sciences, Geosciences, and Biosciences, Office Basic Energy Sciences, U.S. Department of Energy FX Research was sponsored at Oak Ridge National Laboratory by the Division of Chemical Sciences, Geosciences, and Biosciences, Office Basic Energy Sciences, U.S. Department of Energy. B.P.H. is indebted to Prof. K. N. Raymond (UC-Berkeley) for an introduction to high-symmetry coordination assemblies and asking the question whether it is possible to use de novo structure-based methods to design them. NR 133 TC 78 Z9 78 U1 4 U2 73 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1359-7345 J9 CHEM COMMUN JI Chem. Commun. PY 2013 VL 49 IS 14 BP 1354 EP 1379 DI 10.1039/c2cc37776d PG 26 WC Chemistry, Multidisciplinary SC Chemistry GA 074II UT WOS:000313805700001 PM 23254364 ER PT J AU Grossman, J Livshits, B Bace, R Neville-Neil, G AF Grossman, Jeremiah Livshits, Ben Bace, Rebecca Neville-Neil, George TI Browser Security: Appearances Can Be Deceiving SO COMMUNICATIONS OF THE ACM LA English DT Editorial Material C1 [Livshits, Ben] Univ Washington, Seattle, WA 98195 USA. [Bace, Rebecca] Univ S Alabama, Ctr Forens Informat Technol & Secur, Mobile, AL 36688 USA. [Bace, Rebecca] Los Alamos Natl Lab, Comp Informat & Commun Div, Los Alamos, NM 87545 USA. NR 0 TC 0 Z9 0 U1 1 U2 3 PU ASSOC COMPUTING MACHINERY PI NEW YORK PA 2 PENN PLAZA, STE 701, NEW YORK, NY 10121-0701 USA SN 0001-0782 J9 COMMUN ACM JI Commun. ACM PD JAN PY 2013 VL 56 IS 1 BP 60 EP 67 DI 10.1145/2398356.2398372 PG 8 WC Computer Science, Hardware & Architecture; Computer Science, Software Engineering; Computer Science, Theory & Methods SC Computer Science GA 062SJ UT WOS:000312941900026 ER PT J AU Carver, J Heaton, D Hochstein, L Bartlett, R AF Carver, Jeffrey Heaton, Dustin Hochstein, Lorin Bartlett, Roscoe TI SELF-PERCEPTIONS ABOUT SOFTWARE ENGINEERING: A SURVEY OF SCIENTISTS AND ENGINEERS SO COMPUTING IN SCIENCE & ENGINEERING LA English DT Article ID CODE AB Scientists and engineers devote considerable effort to developing large, complex codes to solve important problems. However, while they often develop useful code, many scientists and engineers are frequently unaware of how various software engineering practices can help them write better code. This article presents the results of a survey on this topic. C1 [Carver, Jeffrey] Univ Alabama, Dept Comp Sci, Tuscaloosa, AL 35487 USA. [Bartlett, Roscoe] Oak Ridge Natl Lab, Oak Ridge, TN USA. RP Carver, J (reprint author), Univ Alabama, Dept Comp Sci, Tuscaloosa, AL 35487 USA. EM carver@cs.ua.edu; dwheaton@crimson.ua.edu; lorin@nimbisservices.com; bartlettra@ornl.gov NR 10 TC 3 Z9 3 U1 2 U2 8 PU IEEE COMPUTER SOC PI LOS ALAMITOS PA 10662 LOS VAQUEROS CIRCLE, PO BOX 3014, LOS ALAMITOS, CA 90720-1314 USA SN 1521-9615 J9 COMPUT SCI ENG JI Comput. Sci. Eng. PD JAN-FEB PY 2013 VL 15 IS 1 BP 7 EP 11 PG 5 WC Computer Science, Interdisciplinary Applications SC Computer Science GA 070VI UT WOS:000313540700002 ER PT J AU Santos, E Poco, J Wei, YX Liu, SS Cook, B Williams, DN Silva, CT AF Santos, Emanuele Poco, Jorge Wei, Yaxing Liu, Shishi Cook, Bob Williams, Dean N. Silva, Claudio T. TI UV-CDAT: ANALYZING CLIMATE DATASETS FROM A USER'S PERSPECTIVE SO COMPUTING IN SCIENCE & ENGINEERING LA English DT Article AB The Ultra-scale Visualization Climate Data Analysis Tools (UV-CDAT) is a new tool for analyzing and visualizing climate data. Here we provide some pointers, background information, and examples to show how the system works. C1 [Santos, Emanuele] Univ Fed Ceara, Fortaleza, Ceara, Brazil. [Poco, Jorge; Silva, Claudio T.] NYU, Polytech Inst, New York, NY 10003 USA. [Wei, Yaxing; Liu, Shishi; Cook, Bob] Oak Ridge Natl Lab, Climate Change Sci Inst, Oak Ridge, TN USA. [Williams, Dean N.] Lawrence Livermore Natl Lab, Climate Analyt Informat & Mgmt Syst Div, Livermore, CA USA. RP Santos, E (reprint author), Univ Fed Ceara, Fortaleza, Ceara, Brazil. EM emanuele@lia.ufc.br; jpocom@nyu.edu; weiy@ornl.gov; lius2@ornl.gov; cookrb@ornl.gov; williams13@llnl.gov; csilva@nyu.edu RI Wei, Yaxing/K-1507-2013; OI Wei, Yaxing/0000-0001-6924-0078; Poco, Jorge/0000-0001-9096-6287 FU US Department of Energy (DOE) Office of Biological and Environmental Research (BER); National Science Foundation [0830944]; NASA [09-TE09-07, 09-TE09-26] FX This project has been funded by the US Department of Energy (DOE) Office of Biological and Environmental Research (BER). Additional support was provided by the National Science Foundation (cooperative ageement 0830944 for DataONE) and NASA (projects 09-TE09-07 and 09-TE09-26). This is a large project involving many institutions, including the Lawrence Livermore National Laboratory, Lawrence Berkeley National Laboratory, Los Alamos, Oak Ridge National Laboratory, Kitware, the Polytechnic Institute of New York University, Scientific Computing and Imaging Institute of Utah, and NASA. NR 6 TC 6 Z9 6 U1 0 U2 11 PU IEEE COMPUTER SOC PI LOS ALAMITOS PA 10662 LOS VAQUEROS CIRCLE, PO BOX 3014, LOS ALAMITOS, CA 90720-1314 USA SN 1521-9615 J9 COMPUT SCI ENG JI Comput. Sci. Eng. PD JAN-FEB PY 2013 VL 15 IS 1 BP 94 EP 103 PG 10 WC Computer Science, Interdisciplinary Applications SC Computer Science GA 070VI UT WOS:000313540700013 ER PT J AU Hosemann, P Dickerson, R Dickerson, P Li, N Maloy, SA AF Hosemann, P. Dickerson, R. Dickerson, P. Li, N. Maloy, S. A. TI Transmission electron microscopy (TEM) on oxide layers formed on D9 stainless steel in lead bismuth eutectic (LBE) SO CORROSION SCIENCE LA English DT Article DE Stainless steel; STEM; TEM; Oxidation; High temperature corrosion; Liquid metal corrosion ID ELEVATED-TEMPERATURES; OXIDATION MECHANISM; FE-9CR-1MO STEEL; CORROSION; ALLOY; NICKEL; OXYGEN; SYSTEMS; DESIGN; SPINEL AB Fast reactors and targets in spallation neutron sources are considering lead bismuth eutectic (LBE) as a coolant. However, LBE is a rather corrosive medium for most steels and container materials. This electron microscopy study was performed to evaluate the corrosion and oxidation behavior of the Austenitic steel D9 in a flowing LBE environment. What was believed in the past to be simply a double oxide layer, is revealed here to be a more complicated structure. It was found that at least three layers can be identified while the innermost oxide layer consists of two nanostructured phases. (C) 2012 Elsevier Ltd. All rights reserved. C1 [Hosemann, P.] Univ Calif Berkeley, Dept Nucl Engn, Berkeley, CA 94720 USA. [Dickerson, R.; Dickerson, P.; Li, N.; Maloy, S. A.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Hosemann, P (reprint author), Univ Calif Berkeley, Dept Nucl Engn, 4169 Etcheverry Hall, Berkeley, CA 94720 USA. EM peterh@berkeley.edu RI Dickerson, Robert/C-9237-2013; Lujan Center, LANL/G-4896-2012; Maloy, Stuart/A-8672-2009; OI Maloy, Stuart/0000-0001-8037-1319; Hosemann, Peter/0000-0003-2281-2213 FU AFC RD DOE program; NRC faculty development grant [38-09-948] FX The Authors want to thank the IPPE institute in Obninsk Russia for providing the corrosion samples, The AFC R&D DOE program for funding as well as the NRC faculty development grant 38-09-948. Especially we want to thank Thomas M. Devine from the University of California Berkeley and Alan Bolind from the Japan Atomic Energy Agency for fruitful discussion as well as Erich Stergar from SCK-CEN for editorial suggestions. NR 47 TC 13 Z9 13 U1 2 U2 35 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0010-938X J9 CORROS SCI JI Corrosion Sci. PD JAN PY 2013 VL 66 BP 196 EP 202 DI 10.1016/j.corsci.2012.09.019 PG 7 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Materials Science; Metallurgy & Metallurgical Engineering GA 068RL UT WOS:000313383800023 ER PT J AU Keum, JK Xiao, K Ivanov, IN Hong, KL Browning, JF Smith, GS Shao, M Littrell, KC Rondinone, AJ Payzant, EA Chen, JH Hensley, DK AF Keum, Jong K. Xiao, Kai Ivanov, Ilia N. Hong, Kunlun Browning, James F. Smith, Gregory S. Shao, Ming Littrell, Kenneth C. Rondinone, Adam J. Payzant, E. Andrew Chen, Jihua Hensley, Dale K. TI Solvent quality-induced nucleation and growth of parallelepiped nanorods in dilute poly(3-hexylthiophene) (P3HT) solution and the impact on the crystalline morphology of solution-cast thin film SO CRYSTENGCOMM LA English DT Article ID TO-COIL TRANSITION; CONJUGATED POLYMER; SCATTERING; GLOBULE; CHAIN; MODEL AB Understanding the chain conformation of conjugated polymers in casting solutions and its impact on the crystalline morphology of solution-cast thin films is crucial for many electronic applications. Using small-angle neutron scattering, we show that well-dissolved poly(3-hexyl thiophene) (P3HT) chains in good solvent (chloroform) form long rectangular parallelepipeds (RPs) via nucleation and growth processes upon increasing the volume fraction of poor solvent (hexane) above a certain critical point. The growth of the RPs is due to the p-p stacking of the P3HT main backbone occurring along the long axis of the RPs. P3HT solutions prepared with different poor solvent volume fractions were drop-cast onto Si-wafers to prepare thin films, which were examined using 2D grazing-incidence X-ray scattering and 1D X-ray diffraction. The results indicate that the RPs grown in solution preferentially orient on the substrate with their two longer axes parallel to the surface after solvent evaporation, and give rise to much improved crystallinity and crystal orientation compared to the disordered chains. C1 [Keum, Jong K.; Browning, James F.; Smith, Gregory S.; Littrell, Kenneth C.; Payzant, E. Andrew] Oak Ridge Natl Lab, Neutron Sci Directorate, Oak Ridge, TN 37831 USA. [Xiao, Kai; Ivanov, Ilia N.; Hong, Kunlun; Shao, Ming; Rondinone, Adam J.; Payzant, E. Andrew; Chen, Jihua; Hensley, Dale K.] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. RP Keum, JK (reprint author), Oak Ridge Natl Lab, Neutron Sci Directorate, Oak Ridge, TN 37831 USA. EM keumjk@ornl.gov; browningjf@ornl.gov RI Smith, Gregory/D-1659-2016; Keum, Jong/N-4412-2015; Hong, Kunlun/E-9787-2015; Payzant, Edward/B-5449-2009; Xiao, Kai/A-7133-2012; Littrell, Kenneth/D-2106-2013; Chen, Jihua/F-1417-2011; ivanov, ilia/D-3402-2015; Rondinone, Adam/F-6489-2013; Hensley, Dale/A-6282-2016 OI Smith, Gregory/0000-0001-5659-1805; Keum, Jong/0000-0002-5529-1373; Hong, Kunlun/0000-0002-2852-5111; Payzant, Edward/0000-0002-3447-2060; Browning, James/0000-0001-8379-259X; Xiao, Kai/0000-0002-0402-8276; Littrell, Kenneth/0000-0003-2308-8618; Chen, Jihua/0000-0001-6879-5936; ivanov, ilia/0000-0002-6726-2502; Rondinone, Adam/0000-0003-0020-4612; Hensley, Dale/0000-0001-8763-7765 FU Office of Basic Energy Sciences, U. S. Department of Energy FX This research was conducted at the high flux isotope reactor (HFIR) and the Center for Nanophase Materials Sciences (CNMS), which are sponsored at Oak Ridge National Laboratory (ORNL) by the Office of Basic Energy Sciences, U. S. Department of Energy. SANS measurements were performed on the general purpose (GP)-SANS (CG-2) beamline at HFIR, ORNL. NR 28 TC 18 Z9 18 U1 4 U2 85 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 2013 VL 15 IS 6 BP 1114 EP 1124 DI 10.1039/c2ce26666k PG 11 WC Chemistry, Multidisciplinary; Crystallography SC Chemistry; Crystallography GA 070SU UT WOS:000313532100012 ER PT J AU Harvey, OR Qafoku, NP Cantrell, KJ Lee, G Amonette, JE Brown, CF AF Harvey, Omar R. Qafoku, Nikolla P. Cantrell, Kirk J. Lee, Giehyeon Amonette, James E. Brown, Christopher F. TI Geochemical Implications of Gas Leakage associated with Geologic CO2 Storage-A Qualitative Review SO ENVIRONMENTAL SCIENCE & TECHNOLOGY LA English DT Review ID CARBON-DIOXIDE SEQUESTRATION; NATURAL ANALOG SITE; MICROBIAL COMMUNITY; ARTIFICIAL GROUNDWATER; PRECIPITATION KINETICS; ARSENATE ADSORPTION; MINERAL CARBONATION; SEDIMENTARY BASINS; ROCK INTERACTIONS; SATURATION STATE AB Gas leakage from deep storage reservoirs is a major risk factor associated with geologic carbon sequestration (GCS). A systematic understanding of how such leakage would impact the geochemistry of potable aquifers and the vadose zone is crucial to the maintenance of environmental quality and the widespread acceptance of GCS. This paper reviews the current literature and discusses current knowledge gaps on how elevated CO2 levels could influence geochemical processes (e.g., adsorption/desorption and dissolution/precipitation) in potable aquifers and the vadose zone. The review revealed that despite an increase in research and evidence for both beneficial and deleterious consequences of CO2 migration into potable aquifers and the vaclose zone, significant knowledge gaps still exist Primary among these knowledge gaps is the role/influence of pertinent geochemical factors such as redox condition, CO2 influx rate, gas stream composition, microbial activity, and mineralogy in CO2-induced reactions. Although these factors by no means represent an exhaustive list of knowledge gaps we believe that addressing them is pivotal in advancing current scientific knowledge on how leakage from GCS may impact the environment, improving predictions of CO2-induced geochemical changes in the subsurface, and facilitating science-based decision- and policy-making on risk associated with geologic carbon sequestration. C1 [Harvey, Omar R.; Qafoku, Nikolla P.; Cantrell, Kirk J.; Brown, Christopher F.] Pacific NW Natl Lab, Geosci Grp, Richland, WA 99354 USA. [Harvey, Omar R.] Univ So Mississippi, Dept Geog & Geol, Hattiesburg, MS 39406 USA. [Lee, Giehyeon] Yonsei Univ, Dept Earth Syst Sci, Seoul 120749, South Korea. RP Harvey, OR (reprint author), Pacific NW Natl Lab, Geosci Grp, 902 Battelle Blvd,K6-81, Richland, WA 99354 USA. EM omar.harvey@usm.edu FU National Risk Assessment Partnership (NRAP) through the U.S. DOE Office of Fossil Energy's Division of Crosscutting Research [DE-AC05-76RL01830] FX Funding for this research was provided by the National Risk Assessment Partnership (NRAP) through the U.S. DOE Office of Fossil Energy's Division of Crosscutting Research under contract DE-AC05-76RL01830. We are grateful to Drs. Hongbo Shao (PNNL), Wooyong Um (PNNL), Susan Carroll (LLNL), and Nic Spycher (LBNL) who reviewed an earlier version of the manuscript and provided valuable comments and suggestions. Comments and suggestions from the Associate Editor and anonymous reviewers also improved this manuscript. NR 131 TC 43 Z9 43 U1 4 U2 121 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 0013-936X J9 ENVIRON SCI TECHNOL JI Environ. Sci. Technol. PD JAN 1 PY 2013 VL 47 IS 1 BP 23 EP 36 DI 10.1021/es3029457 PG 14 WC Engineering, Environmental; Environmental Sciences SC Engineering; Environmental Sciences & Ecology GA 066KS UT WOS:000313220300004 PM 23092162 ER PT J AU Burant, A Lowry, GV Karamalidis, AK AF Burant, Aniela Lowry, Gregory V. Karamalidis, Athanasios K. TI Partitioning Behavior of Organic Contaminants in Carbon Storage Environments: A Critical Review SO ENVIRONMENTAL SCIENCE & TECHNOLOGY LA English DT Review ID VAPOR-LIQUID-EQUILIBRIA; ENHANCED OIL-RECOVERY; POLYCYCLIC AROMATIC-HYDROCARBONS; SUPERCRITICAL-FLUID EXTRACTION; PENG-ROBINSON EQUATION; ACID-WATER MIXTURES; PHASE-EQUILIBRIA; BINARY-MIXTURES; HYDROXYBENZOIC ACID; TERNARY-SYSTEMS AB Carbon capture and storage is a promising strategy for mitigating the CO2 contribution to global climate change. The large scale implementation of the technology mandates better understanding of the risks associated with CO2 injection into geologic formations and the subsequent interactions with groundwater resources. The injected supercritical CO2 (sc-CO2) is a nonpolar solvent that can potentially mobilize organic compounds that exist at residual saturation in the formation. Here, we review the partitioning behavior of selected organic compounds typically found in depleted oil reservoirs in the residual oil-brine-sc-CO2 system under carbon storage conditions. The solubility of pure phase organic compounds in sc-CO2, and partitioning of organic compounds between water and sc-CO2 follow trends predicted based on thermodynamics. Compounds with high volatility and low aqueous solubility have the highest potential to partition to sc-CO2. The partitioning of low volatility compounds to sc-CO2 can be enhanced by cosolvency due to the presence of higher volatility compounds in the sc-CO2. The effect of temperature, pressure, salinity, pH, and dissolution of water molecules into sc-CO2 on the partitioning behavior of organic compounds in the residual oil-brine-sc-CO2 system is discussed. Data gaps and research needs for models to predict the partitioning of organic compounds in brines and from complex mixtures of oils are presented. Models need to be able to better incorporate the effect of salinity and cosolvency, which will require more experimental data from key classes of organic compounds. C1 [Burant, Aniela; Lowry, Gregory V.; Karamalidis, Athanasios K.] Reg Univ Alliance NETL RUA, Natl Energy Technol Lab, Pittsburgh, PA 15236 USA. [Burant, Aniela; Lowry, Gregory V.; Karamalidis, Athanasios K.] Carnegie Mellon Univ, Dept Civil & Environm Engn, Pittsburgh, PA 15213 USA. RP Karamalidis, AK (reprint author), Reg Univ Alliance NETL RUA, Natl Energy Technol Lab, Pittsburgh, PA 15236 USA. EM akaramal@andrew.cmu.edu FU RES [DE-FE0004000]; Jared and Maureen Cohon Graduate Fellowship in Civil and Environmental Engineering; Department of Energy, National Energy Technology Laboratory, an agency of the United States Government; URS Energy & Construction, Inc. FX As part of the National Energy Technology Laboratory's Regional University Alliance (NETL-RUA), a collaborative initiative of the NETL, this technical effort was performed under the RES contract DE-FE0004000. We thank Dr. J. Alexandra Hakala of National Energy Technology Laboratory for providing a thorough and constructive review. We also thank the Jared and Maureen Cohon Graduate Fellowship in Civil and Environmental Engineering for support. 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 129 TC 19 Z9 20 U1 4 U2 99 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 0013-936X J9 ENVIRON SCI TECHNOL JI Environ. Sci. Technol. PD JAN 1 PY 2013 VL 47 IS 1 BP 37 EP 54 DI 10.1021/es304262p PG 18 WC Engineering, Environmental; Environmental Sciences SC Engineering; Environmental Sciences & Ecology GA 066KS UT WOS:000313220300005 PM 23211055 ER PT J AU Shao, HB Thompson, CJ Qafoku, O Cantrell, KJ AF Shao, Hongbo Thompson, Christopher J. Qafoku, Odeta Cantrell, Kirk J. TI In Situ Spectrophotometric Determination of pH under Geologic CO2 Sequestration Conditions: Method Development and Application SO ENVIRONMENTAL SCIENCE & TECHNOLOGY LA English DT Article ID DEEP SALINE AQUIFERS; HYDROFLUORIC-ACID; PHENOL RED; PRESSURE; WATER; EQUILIBRIUM; SPECTRA AB CO2 injection into deep geologic formations for long-term storage will cause a decrease in aqueous pH due to CO2 dissolution into reservoir water/brine. Current studies seeking to assess chemical changes under geological CO2 sequestration (GCS) conditions rely largely on thermodynamic modeling due to the lack of reliable experimental methods. In this work, a spectrophotometric method utilizing bromophenol blue to measure pH in laboratory experiments under GCS-relevant conditions was developed. The method was tested in simulated reservoir fluids (CO2-NaCl-H2O) at different temperatures, pressures, and ionic strengths, and the results were compared with those from other experimental studies and geochemical models. Measured pH values were generally in agreement with the models, but inconsistencies were present between the models. In situ pH measurements for a basalt rock-CO2-brine system were conducted under GCS conditions. The pH increased to 3.52 during a 10-day period due to rock dissolution, compared to pH 2.95 for the CO2-brine system without rock. The calculated pH values from geochemical models were 0.22-0.25 units higher than the measured values (assuming all iron in the system was in the form of Fe2+). This work demonstrates the use of in situ spectrophotometry for pH measurement under GCS-relevant conditions. C1 [Shao, Hongbo; Thompson, Christopher J.; Qafoku, Odeta; Cantrell, Kirk J.] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Cantrell, KJ (reprint author), Pacific NW Natl Lab, Richland, WA 99352 USA. EM kirk.cantrell@pnnl.gov RI Shao, Hongbo/N-4169-2013 FU National Risk Assessment Partnership (NRAP) in the U.S. DOE Office of Fossil Energy's Carbon Sequestration Program FX Funding for this research was provided by the National Risk Assessment Partnership (NRAP) in the U.S. DOE Office of Fossil Energy's Carbon Sequestration Program. We thank Dr. Dedong Li and Dr. Kenneth Carroll for assisting with model calculations. NR 35 TC 4 Z9 4 U1 1 U2 28 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 0013-936X J9 ENVIRON SCI TECHNOL JI Environ. Sci. Technol. PD JAN 1 PY 2013 VL 47 IS 1 BP 63 EP 70 DI 10.1021/es3016793 PG 8 WC Engineering, Environmental; Environmental Sciences SC Engineering; Environmental Sciences & Ecology GA 066KS UT WOS:000313220300007 PM 22708540 ER PT J AU Steele-MacInnis, M Capobianco, RM Dilmore, R Goodman, A Guthrie, G Rimstidt, JD Bodnar, RJ AF Steele-MacInnis, Matthew Capobianco, Ryan M. Dilmore, Robert Goodman, Angela Guthrie, George Rimstidt, J. Donald Bodnar, Robert J. TI Volumetrics of CO2 Storage in Deep Saline Formations SO ENVIRONMENTAL SCIENCE & TECHNOLOGY LA English DT Article ID CARBON-DIOXIDE; 100 MPA; 647 K; CO2-H2O; SEQUESTRATION; SYSTEM; CAPACITY; AQUIFERS; SOLUBILITIES; 0-DEGREES-C AB Concern about the role of greenhouse gases in global climate change has generated interest in sequestering CO2 from fossil-fuel combustion in deep saline formations. Pore space in these formations is initially filled with brine, and space to accommodate injected CO2 must be generated by displacing brine, and to a lesser extent by compression of brine and rock. The formation volume required to store a given mass of CO2 depends on the storage mechanism. We compare the equilibrium volumetric requirements of three end-member processes: CO2 stored as a supercritical fluid (structural or stratigraphic trapping); CO2 dissolved in pre-existing brine (solubility trapping); and CO2 solubility enhanced by dissolution of calcite. For typical storage conditions, storing CO2 by solubility trapping reduces the volume required to store the same amount of CO2 by structural or stratigraphic trapping by about 50%. Accessibility of CO2 to brine determines which storage mechanism (structural/stratigraphic versus solubility) dominates at a given time, which is a critical factor in evaluating CO2 volumetric requirements and long-term storage security. C1 [Capobianco, Ryan M.; Rimstidt, J. Donald; Bodnar, Robert J.] Reg Univ Alliance NETL RUA, Natl Energy Technol Lab, Pittsburgh, PA USA. [Steele-MacInnis, Matthew; Capobianco, Ryan M.; Rimstidt, J. Donald; Bodnar, Robert J.] Virginia Tech, Dept Geosci, Blacksburg, VA 24061 USA. [Dilmore, Robert; Goodman, Angela; Guthrie, George] US DOE, Natl Energy Technol Lab NETL, Pittsburgh, PA 15236 USA. RP Steele-MacInnis, M (reprint author), Virginia Tech, Dept Geosci, Blacksburg, VA 24061 USA. EM mjmaci@vt.edu RI Rimstidt, James/N-8910-2013 FU National Energy Technology Laboratory [DE-FE-0004000]; Institute for Critical Technology and Applied Science (ICTAS) at Virginia Tech FX We thank Alexandra Hakala for valuable discussions and three anonymous reviewers for their insightful and helpful comments on an earlier version of this manuscript. We also thank David Dzombak and Daniel Giammar for their editorial advice. This research effort was partially performed in support of the National Energy Technology Laboratory under Contract DE-FE-0004000. Steele-MacInnis was funded by the Institute for Critical Technology and Applied Science (ICTAS) at Virginia Tech. NR 34 TC 9 Z9 9 U1 1 U2 35 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 0013-936X J9 ENVIRON SCI TECHNOL JI Environ. Sci. Technol. PD JAN 1 PY 2013 VL 47 IS 1 BP 79 EP 86 DI 10.1021/es301598t PG 8 WC Engineering, Environmental; Environmental Sciences SC Engineering; Environmental Sciences & Ecology GA 066KS UT WOS:000313220300009 PM 22916959 ER PT J AU Criscenti, LJ Cygan, RT AF Criscenti, Louise J. Cygan, Randall T. TI Molecular Simulations of Carbon Dioxide and Water: Cation Solvation SO ENVIRONMENTAL SCIENCE & TECHNOLOGY LA English DT Article ID CO2 SEQUESTRATION; HIGH TEMPERATURES; COMPUTER-SIMULATIONS; DYNAMICS SIMULATION; AQUEOUS-SOLUTION; CALCIUM-ION; FORCE-FIELD; METAL-IONS; MODEL; SOLUBILITY AB Proposed carbon dioxide sequestration scenarios in sedimentary reservoirs require investigation into the interactions between supercritical carbon dioxide, brines, and the mineral phases found in the basin and overlying caprock. Molecular simulations can help to understand the partitioning of metal cations between aqueous solutions and supercritical carbon dioxide where limited experimental data exist. In this effort, we used classical molecular dynamics simulations to compare the solvation of alkali and alkaline-earth metal cations in water and liquid CO2 at 300 K by combining a flexible simple point charge model for water and an accurate flexible force field for CO2. Solvation energies for these cations are larger in water than in carbon dioxide, suggesting that they will partition preferentially into water. In both aqueous and CO2 solutions, the solvation energies decrease with cation size and increase with cation charge. However, changes in solvation energy with ionic radii are smaller in CO2 than in water suggesting that the partitioning of cations into CO2 will increase with ion size. Simulations of the interface between aqueous solution and supercritical CO2 support this suggestion in that some large cations (e.g., Cs+ and K+) partition into the CO2 phase, often with a partial solvation sphere of water molecules. C1 [Criscenti, Louise J.; Cygan, Randall T.] Sandia Natl Labs, Dept Geochem, Albuquerque, NM 87185 USA. RP Criscenti, LJ (reprint author), Sandia Natl Labs, Dept Geochem, POB 5800,MS 0754, Albuquerque, NM 87185 USA. EM ljcrisc@sandia.gov FU Center for Frontiers of Subsurface Energy Security, an Energy Frontier Research Center; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC-0001114]; U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX This work was funded in part by the Center for Frontiers of Subsurface Energy Security, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Award DE-SC-0001114. Sandia National Laboratories 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 42 TC 16 Z9 17 U1 5 U2 88 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 0013-936X J9 ENVIRON SCI TECHNOL JI Environ. Sci. Technol. PD JAN 1 PY 2013 VL 47 IS 1 BP 87 EP 94 DI 10.1021/es301608c PG 8 WC Engineering, Environmental; Environmental Sciences SC Engineering; Environmental Sciences & Ecology GA 066KS UT WOS:000313220300010 PM 22779448 ER PT J AU Fernandez-Martinez, A Hu, YD Lee, B Jun, YS Waychunas, GA AF Fernandez-Martinez, Alejandro Hu, Yandi Lee, Byeongdu Jun, Young-Shin Waychunas, Glenn A. TI In Situ Determination of Interfacial Energies between Heterogeneously Nucleated CaCO3 and Quartz Substrates: Thermodynamics of CO2 Mineral Trapping SO ENVIRONMENTAL SCIENCE & TECHNOLOGY LA English DT Article ID SMALL-ANGLE SCATTERING; CALCIUM-CARBONATE; SURFACE; SEQUESTRATION; PRECIPITATION; WATER; DISSOLUTION; SILICA; GROWTH; PRINCIPLES AB The precipitation of carbonate minerals-mineral trapping-is considered one of the safest sequestration mechanisms ensuring long-term geologic storage of CO2. However, little is known about the thermodynamic factors controlling the extent of heterogeneous nucleation at mineral surfaces exposed to the fluids in porous reservoirs. The goal of this study is to determine the thermodynamic factors controlling heterogeneous nucleation of carbonate minerals on pristine quartz (100) surfaces, which are assumed representative of sandstone reservoirs. To probe CaCO3 nucleation on quartz (100) in solution and with nanoscale resolution, an in situ grazing incidence small-angle X-ray scattering technique has been utilized. With this method, a value of alpha' = 36 +/- 5 mJ/m(2) for the effective interfacial free energy governing heterogeneous nucleation of CaCO3 has been obtained by measuring nucleation rates at different solution supersaturations. This value is lower than the interfacial energy governing calcite homogeneous nucleation (alpha approximate to 120 mJ/m(2)), suggesting that heterogeneous nucleation of calcium carbonate is favored on quartz (100) at ambient pressure and temperature conditions, with nucleation barriers between 2.5% and 15% lower than those expected for homogeneous nucleation. These observations yield important quantitative parameters readily usable in reactive transport models of nucleation at the reservoir scale. C1 [Fernandez-Martinez, Alejandro; Waychunas, Glenn A.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, Berkeley, CA 94720 USA. [Hu, Yandi; Jun, Young-Shin] Washington Univ, Dept Energy Environm & Chem Engn, St Louis, MO 63130 USA. [Lee, Byeongdu] Argonne Natl Lab, Xray Sci Div, Adv Photon Source, Argonne, IL 60439 USA. RP Jun, YS (reprint author), Washington Univ, Dept Energy Environm & Chem Engn, 1 Brookings Dr, St Louis, MO 63130 USA. EM ysjun@seas.wustl.edu; GAWaychunas@lbl.gov RI Fernandez-Martinez, Alejandro/B-4042-2010; Hu, Yandi/F-7968-2011; OI Fernandez-Martinez, Alejandro/0000-0001-5073-9629; Hu, Yandi/0000-0002-8506-9335; Lee, Byeongdu/0000-0003-2514-8805 FU Center for Nanoscale Control of Geologic CO2, an Energy Frontier Research Center; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-05CH11231]; U.S. DOE [DE-AC02-06CH11357] FX We gratefully acknowledge James J. DeYoreo for numerous discussions and for his insightful comments and suggestions, as well as the constructive comments from four reviewers. Also, Jessica Ray (WUStL), Xiaobing Zuo, Janae DeBartolo and Sonke Seifert (APS, ANL) are thanked for their help during GISAXS data collection. A.F.-M. thanks Giuseppe Saldi, Damien Daval and the 'Amorphous Reading Group' for enjoyable discussions about this and other subjects over the last two years. This material is based upon work supported as part of the Center for Nanoscale Control of Geologic CO2, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Award Number DE-AC02-05CH11231. Use of the Advanced Photon Source, an Office of Science User Facility operated for the U.S. Department of Energy Office of Science by Argonne National Laboratory, was supported by the U.S. DOE under Contract No. DE-AC02-06CH11357. NR 57 TC 18 Z9 18 U1 6 U2 60 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 0013-936X J9 ENVIRON SCI TECHNOL JI Environ. Sci. Technol. PD JAN 1 PY 2013 VL 47 IS 1 BP 102 EP 109 DI 10.1021/es3014826 PG 8 WC Engineering, Environmental; Environmental Sciences SC Engineering; Environmental Sciences & Ecology GA 066KS UT WOS:000313220300012 PM 22646799 ER PT J AU Xu, M Sullivan, K VanNess, G Knauss, KG Higgins, SR AF Xu, Man Sullivan, Katie VanNess, Garrett Knauss, Kevin G. Higgins, Steven R. TI Dissolution Kinetics and Mechanisms at Dolomite-Water Interfaces: Effects of Electrolyte Specific Ionic Strength SO ENVIRONMENTAL SCIENCE & TECHNOLOGY LA English DT Article ID ATOMIC-FORCE-MICROSCOPY; AQUEOUS-SOLUTION; CALCITE DISSOLUTION; TETRAMETHYLAMMONIUM CHLORIDE; CHEMICAL CONTROLS; CRYSTAL-GROWTH; SURFACE; HYDRATION; STEP; SIMULATION AB Elucidating dissolution kinetics and mechanisms at carbonate mineral-water interfaces is essential to many environmental and geochemical processes, including geologic CO2 sequestration in deep aquifers. In the present work, effects of background electrolytes on dolomite (CaMg(CO3)(2)) reactivity were investigated by measuring step dissolution rates using in situ hydrothermal atomic force microscopy (HAFM) at 90 degrees C. Cleaved surfaces of dolomite were exposed to sodium chloride and tetramethylammonium chloride (TMACl) aqueous solutions with ionic strengths (I) ranging from 0 to 0.77 m at pH 4 and pH 9. HAFM results demonstrated that dolomite step retreat rates increased with increasing solution ionic strength and decreasing pH. Comparison of [48 (1) over bar] and [(4) over bar 41] steps revealed that the anisotropy of [48 (1) over bar] and [(4) over bar 41] step speeds became significant as solution ionic strength increased, with NaCl exerting more pronounced effects than TMACl for the same I. To interpret the different trends observed for NaCl and TMACl, a dissolution mechanism involving orientation-dependent ion adsorption and consequent edge free energy changes is proposed. C1 [Xu, Man; Sullivan, Katie; VanNess, Garrett; Higgins, Steven R.] Wright State Univ, Dept Chem, Dayton, OH 45435 USA. [Knauss, Kevin G.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, Berkeley, CA 94720 USA. RP Higgins, SR (reprint author), Wright State Univ, Dept Chem, 3640 Colonel Glenn Highway, Dayton, OH 45435 USA. EM steven.higgins@wright.edu RI Xu, Man/B-7660-2013 FU United States Department of Energy, Office of Science, Basic Energy Sciences, Chemical Sciences, Geosciences and Biosciences Division FX This research was funded by the United States Department of Energy, Office of Science, Basic Energy Sciences, Chemical Sciences, Geosciences and Biosciences Division. We thank Dr. David Dzombak, Dr. Daniel Giammar, and four anonymous reviewers for their valuable comments. NR 62 TC 8 Z9 8 U1 6 U2 67 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 0013-936X J9 ENVIRON SCI TECHNOL JI Environ. Sci. Technol. PD JAN 1 PY 2013 VL 47 IS 1 BP 110 EP 118 DI 10.1021/es301284h PG 9 WC Engineering, Environmental; Environmental Sciences SC Engineering; Environmental Sciences & Ecology GA 066KS UT WOS:000313220300013 PM 22681699 ER PT J AU Schaef, HT McGrail, BP Loring, JL Bowden, ME Arey, BW Rosso, KM AF Schaef, Herbert Todd McGrail, Bernard P. Loring, John L. Bowden, Mark E. Arey, Bruce W. Rosso, Kevin M. TI Forsterite [Mg2SiO4)] Carbonation in Wet Supercritical CO2: An in Situ High-Pressure X-ray Diffraction Study SO ENVIRONMENTAL SCIENCE & TECHNOLOGY LA English DT Article ID SEQUESTRATION; PRECIPITATION; NESQUEHONITE; TEMPERATURE; MAGNESITE; SPECTROSCOPY; REACTIVITY; DIOXIDE; LIQUID; SYSTEM AB Mechanisms controlling mineral stabilities in contact with injected supercritical fluids containing water are relatively unknown. In this paper, we discuss carbonation reactions occurring with forsterite (Mg2SiO4) exposed to variably wet supercritical CO2 (scCO(2)). Transformation reactions were tracked by in situ high-pressure X-ray diffraction in the presence of scCO(2) containing dissolved water. Under modest pressures (90 bar) and temperatures (50 degrees C), scCO(2) saturated with water converted >70 wt % forsterite to a hydrated magnesium carbonate, nesquehonite (MgCO3 center dot 3H(2)O), and magnesite (MgCO3) after 72 h. However, comparable tests with scCO(2) at only partial water saturation showed a faster carbonation rate but significantly less nesquehonite formation and no evidence of the anhydrous form (MgCO3). The presence and properties of a thin water film, observed by in situ infrared (IR) spectroscopy and with isotopically labeled oxygen (O-18), appears to be critical for this silicate mineral to carbonate in low water environments. The carbonation products formed demonstrated by temperature and water-content dependence highlights the importance of these kinds of studies to enable better predictions of the long-term fate of geologically stored CO2. C1 [Schaef, Herbert Todd; McGrail, Bernard P.; Loring, John L.; Bowden, Mark E.; Arey, Bruce W.; Rosso, Kevin M.] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Schaef, HT (reprint author), Pacific NW Natl Lab, 902 Battelle Blvd,POB 999,MSIN K6-81, Richland, WA 99352 USA. EM Todd.schaef@pnl.gov FU Carbon Sequestration Initiative, a Laboratory Directed Research and Development program at Pacific Northwest National Laboratory (PNNL); U.S. Department of Energy Office of Fossil Energy; DOE by Battelle Memorial Institute [DE-AC06-76RLO-1830] FX This work was supported by the Carbon Sequestration Initiative, a Laboratory Directed Research and Development program at Pacific Northwest National Laboratory (PNNL), and the U.S. Department of Energy Office of Fossil Energy. Part of this work was performed at EMSL, a national scientific user facility at PNNL that is managed by the DOE's office of Biological and Environmental Research. PNNL is operated for DOE by Battelle Memorial Institute under Contract DE-AC06-76RLO-1830. NR 37 TC 18 Z9 18 U1 2 U2 53 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 0013-936X EI 1520-5851 J9 ENVIRON SCI TECHNOL JI Environ. Sci. Technol. PD JAN 1 PY 2013 VL 47 IS 1 BP 174 EP 181 DI 10.1021/es301126f PG 8 WC Engineering, Environmental; Environmental Sciences SC Engineering; Environmental Sciences & Ecology GA 066KS UT WOS:000313220300021 ER PT J AU Rother, G Ilton, ES Wallacher, D Hauss, T Schaef, HT Qafoku, O Rosso, KM Felmy, AR Krukowski, EG Stack, AG Grimm, N Bodnar, RJ AF Rother, Gernot Ilton, Eugene S. Wallacher, Dirk Hauss, Thomas Schaef, Herbert T. Qafoku, Odeta Rosso, Kevin M. Felmy, Andrew R. Krukowski, Elizabeth G. Stack, Andrew G. Grimm, Nico Bodnar, Robert J. TI CO2 Sorption to Subsingle Hydration Layer Montmorillonite Clay Studied by Excess Sorption and Neutron Diffraction Measurements SO ENVIRONMENTAL SCIENCE & TECHNOLOGY LA English DT Article ID SOCIETY SOURCE CLAYS; X-RAY-DIFFRACTION; SUPERCRITICAL CARBON-DIOXIDE; BASE-LINE; SEQUESTRATION; MINERALS; STORAGE; PRESSURES; CHARGE; SMECTITES AB Geologic storage of CO2 requires that the caprock sealing the storage rock is highly impermeable to CO2. Swelling clays, which are important components of caprocks, may interact with CO2 leading to volume change and potentially impacting the seal quality. The interactions of supercritical (sc) CO2 with Na saturated montmorillonite clay containing a subsingle layer of water in the interlayer region have been studied by sorption and neutron diffraction techniques. The excess sorption isotherms show maxima at bulk CO2 densities of approximate to 0.15 g/cm(3), followed by an approximately linear decrease of excess sorption to zero and negative values with increasing CO2 bulk density. Neutron diffraction experiments on the same clay sample measured interlayer spacing and composition. The results show that limited amounts of CO2 are sorbed into the interlayer region, leading to depression of the interlayer peak intensity and an increase of the d(001) spacing by ca. 0.5 angstrom. The density of CO2 in the clay pores is relatively stable over a wide range of CO2 pressures at a given temperature, indicating the formation of a clay-CO2 phase. At the excess sorption maximum, increasing CO2 sorption with decreasing temperature is observed while the high-pressure sorption properties exhibit weak temperature dependence. C1 [Rother, Gernot; Stack, Andrew G.] Oak Ridge Natl Lab, Div Chem Sci, Geochem & Interfacial Sci Grp, Oak Ridge, TN 37831 USA. [Ilton, Eugene S.; Schaef, Herbert T.; Qafoku, Odeta; Rosso, Kevin M.; Felmy, Andrew R.] Pacific NW Natl Lab, Richland, WA 99352 USA. [Wallacher, Dirk; Hauss, Thomas] Helmholtz Zentrum Berlin Mat & Energie GmbH, D-14109 Berlin, Germany. [Krukowski, Elizabeth G.; Bodnar, Robert J.] Virginia Tech, Fluids Res Lab, Blacksburg, VA 24061 USA. RP Rother, G (reprint author), Oak Ridge Natl Lab, Div Chem Sci, Geochem & Interfacial Sci Grp, Oak Ridge, TN 37831 USA. EM rotherg@ornl.gov RI HauSS, Thomas/O-4667-2015; Stack, Andrew/D-2580-2013; Rother, Gernot/B-7281-2008 OI HauSS, Thomas/0000-0001-9325-6432; Stack, Andrew/0000-0003-4355-3679; Rother, Gernot/0000-0003-4921-6294 FU U.S. Department of Energy's Office of Basic Energy Sciences, Geosciences Program through a Single Investigator Small Group research grant; NETL-Regional University Alliance (NETL-RUA) under the RES [DE-FE0004000] FX We thank Dr. David J. Wesolowski, Dr. Andreas Busch, Yves Gensterblum, and Pieter Bertier for helpful discussions and Dr. Dzombak and anonymous reviewers for valuable comments. This work was supported by the U.S. Department of Energy's Office of Basic Energy Sciences, Geosciences Program through a Single Investigator Small Group research grant awarded to PNNL. E.G.K. and R.J.B. were supported through the NETL-Regional University Alliance (NETL-RUA) in support of the National Energy Technology Laboratory's ongoing research in carbon sequestration under the RES Contract DE-FE0004000. NR 41 TC 17 Z9 18 U1 2 U2 83 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 0013-936X J9 ENVIRON SCI TECHNOL JI Environ. Sci. Technol. PD JAN 1 PY 2013 VL 47 IS 1 BP 205 EP 211 DI 10.1021/es301382y PG 7 WC Engineering, Environmental; Environmental Sciences SC Engineering; Environmental Sciences & Ecology GA 066KS UT WOS:000313220300025 PM 22917276 ER PT J AU Wang, Y Zhang, CY Wei, N Oostrom, M Wietsma, TW Li, XC Bonneville, A AF Wang, Ying Zhang, Changyong Wei, Ning Oostrom, Mart Wietsma, Thomas W. Li, Xiaochun Bonneville, Alain TI Experimental Study of Crossover from Capillary to Viscous Fingering for Supercritical CO2-Water Displacement in a Homogeneous Pore Network SO ENVIRONMENTAL SCIENCE & TECHNOLOGY LA English DT Article ID POROUS-MEDIA; CO2 STORAGE; SCALE; WATER; MICROMODEL; INJECTION; FLOW; VISUALIZATION; AQUIFERS; MODELS AB Carbon sequestration in saline aquifers involves displacing brine from the pore space by supercritical CO2 (scCO(2)). The displacement process is considered unstable due to the unfavorable viscosity ratio between the invading scCO(2) and the resident brine. The mechanisms that affect scCO(2)-water displacement under reservoir conditions (41 degrees C, 9 MPa) were investigated in a homogeneous micromodel. A large range of injection rates, expressed as the dimensionless capillary number (Ca), was studied in two sets of experiments: discontinuous-rate injection, where the micromodel was saturated with water before each injection rate was imposed, and continuous-rate injection, where the rate was increased after quasi-steady conditions were reached for a certain rate. For the discontinuous-rate experiments, capillary fingering and viscous fingering are the dominant mechanisms for low (logCa <= -6.61) and high injection rates (logCa >= -5.21), respectively. Crossover from capillary to viscous fingering was observed for logCa = -5.91 to -5.21, resulting in a large decrease in scCO2 saturation. The discontinuous-rate experimental results confirmed the decrease in nonwetting fluid saturation during crossover from capillary to viscous fingering predicted by numerical simulations by Lenormand et al. (J. Fluid Mech. 1988, 189, 165-187). Capillary fingering was the dominant mechanism for all injection rates in the continuous-rate experiment, resulting in monotonic increase in scCO(2) saturation. C1 [Wang, Ying; Wei, Ning; Li, Xiaochun] Chinese Acad Sci, Inst Rock & Soil Mech, State Key Lab Geomech & Geotech Engn, Wuhan 430071, Peoples R China. [Zhang, Changyong; Oostrom, Mart; Wietsma, Thomas W.; Bonneville, Alain] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Zhang, CY (reprint author), Pacific NW Natl Lab, 902 Battelle Blvd,POB 999,MSIN K8-96, Richland, WA 99352 USA. EM Changyong.Zhang@pnnl.gov RI Zhang, Changyong/A-8012-2013; OI Bonneville, Alain/0000-0003-1527-1578 FU Chinese Academy of Science; Pacific Northwest National Laboratory; National Energy Technology Laboratory under framework of U.S.-China Fossil Energy Protocol, Annex VI Advanced Coal-Based Energy Systems Research, Development and Simulation; PNNL's Carbon Sequestration Initiative under its Laboratory Directed Research and Development Program FX This research was supported in part by a collaborative project between the Chinese Academy of Science, Pacific Northwest National Laboratory, and the National Energy Technology Laboratory under the framework of U.S.-China Fossil Energy Protocol, Annex VI Advanced Coal-Based Energy Systems Research, Development and Simulation, and by the PNNL's Carbon Sequestration Initiative under its Laboratory Directed Research and Development Program. All experiments were conducted in the William R. Wiley Environmental Molecular Sciences Laboratory, a United States Department of Energy (DOE) scientific user facility operated for the DOE by PNNL. NR 32 TC 20 Z9 20 U1 1 U2 64 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 0013-936X J9 ENVIRON SCI TECHNOL JI Environ. Sci. Technol. PD JAN 1 PY 2013 VL 47 IS 1 BP 212 EP 218 DI 10.1021/es3014503 PG 7 WC Engineering, Environmental; Environmental Sciences SC Engineering; Environmental Sciences & Ecology GA 066KS UT WOS:000313220300026 PM 22676368 ER PT J AU Wang, YF Bryan, C Dewers, T Heath, JE Jove-Colon, C AF Wang, Yifeng Bryan, Charles Dewers, Thomas Heath, Jason E. Jove-Colon, Carlos TI Ganglion Dynamics and Its Implications to Geologic Carbon Dioxide Storage SO ENVIRONMENTAL SCIENCE & TECHNOLOGY LA English DT Article ID POROUS-MEDIA; IMMISCIBLE DISPLACEMENT; INTERFACIAL-TENSION; OIL GANGLIA; PERCOLATION THEORY; CO2 SEQUESTRATION; BUOYANCY FORCES; 2-PHASE FLOW; WATER; MOBILIZATION AB Capillary trapping of a nonwetting fluid phase in the subsurface has been considered as an important mechanism for geologic storage of carbon dioxide (CO2). This mechanism can potentially relax stringent requirements for the integrity of cap rocks for CO2 storage and therefore can significantly enhance storage capacity and security. We here apply ganglion dynamics to understand the capillary trapping of supercritical CO2 (scCO(2)) under relevant reservoir conditions. We show that, by breaking the injected scCO(2) into small disconnected ganglia, the efficiency of capillary trapping can be greatly enhanced, because the mobility of a ganglion is inversely dependent on its size. Supercritical CO2 ganglia can be engineered by promoting CO2-water interface instability during immiscible displacement, and their size distribution can be controlled by injection mode (e.g., water-alternating-gas) and rate. We also show that a large mobile ganglion can potentially break into smaller ganglia due to CO2-brine interface instability during buoyant rise, thus becoming less mobile. The mobility of scCO(2) in the subsurface is therefore self-limited. Vertical structural heterogeneity within a reservoir can inhibit the buoyant rise of scCO(2) ganglia. The dynamics of scCO(2) ganglia described here provides a new perspective for the security and monitoring of subsurface CO2 storage. C1 [Wang, Yifeng; Bryan, Charles; Dewers, Thomas; Heath, Jason E.; Jove-Colon, Carlos] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Wang, YF (reprint author), Sandia Natl Labs, POB 5800,Mail Stop 0779, Albuquerque, NM 87185 USA. EM ywang@sandia.gov FU U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000]; DOE Sandia LDRD Program FX Sandia National Laboratories is a multiprogram laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000. This work is supported by DOE Sandia LDRD Program. NR 39 TC 2 Z9 2 U1 2 U2 30 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 0013-936X EI 1520-5851 J9 ENVIRON SCI TECHNOL JI Environ. Sci. Technol. PD JAN 1 PY 2013 VL 47 IS 1 BP 219 EP 226 DI 10.1021/es301208k PG 8 WC Engineering, Environmental; Environmental Sciences SC Engineering; Environmental Sciences & Ecology GA 066KS UT WOS:000313220300027 PM 22844874 ER PT J AU Carroll, SA Mcnab, WW Dai, ZR Torres, SC AF Carroll, Susan A. McNab, Walt W. Dai, Zurong Torres, Sharon C. TI Reactivity of Mount Simon Sandstone and the Eau Claire Shale Under CO2 Storage Conditions SO ENVIRONMENTAL SCIENCE & TECHNOLOGY LA English DT Article ID SEQUESTRATION; ROCK; SIMULATION; INJECTION; TRANSPORT; GASES; SITE; USA AB The Mount Simon sandstone and Eau Claire shale formations are target storage and cap rock formations for the Illinois Basin Decatur Geologic Carbon Sequestration Project. We reacted rock samples with brine and supercritical CO2 at 51 degrees C and 19.5 MPa to access the reactivity of these formations at storage conditions and to address the applicability of using published kinetic and thermodynamic constants to predict geochemical alteration that may occur during storage by quantifying parameter uncertainty against experimental data. Incongruent dissolution of iron-rich clays and formation of secondary clays and amorphous silica will dominate geochemical alterations at this CO2 storage site in CO2-rich brines. The surrogate iron-rich clay in the model required significant adjustments to its thermodynamic constants and inclusion of incongruent reaction terms to capture the change in solution composition under acid CO2 conditions. This result emphasizes the need for experiments that constrain the conceptual geochemical model, calibrate mean parameter values, and quantify parameter uncertainty in reactive-transport simulations that will be used to estimate long-term CO2 trapping mechanisms and changes in porosity and permeability. C1 [Carroll, Susan A.; McNab, Walt W.; Dai, Zurong; Torres, Sharon C.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. RP Carroll, SA (reprint author), Lawrence Livermore Natl Lab, 7000 East Ave, Livermore, CA 94550 USA. EM carroll6@llnl.gov FU U.S. Department of Energy, Office of Fossil Energy, Carbon Sequestration Program; U.S. Department of Energy by Lawrence Livermore National Laboratory [DE-AC52-07NA27344]; United States government FX We thank three anonymous reviewers for the constructive comments and LLNL personnel Victoria Genetti and Rachel Lindvall for ICP-MS analyses. This work was funded by the U.S. Department of Energy, Office of Fossil Energy, Carbon Sequestration Program. This work performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344. This document was prepared as an account of work sponsored by an agency of the United States government. Neither the United States government nor Lawrence Livermore National Security, LLC, 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 Lawrence Livermore National Security, LLC. The views and opinions of authors expressed herein do not necessarily state or reflect those of the United States government or Lawrence Livermore National Security, LLC, and shall not be used for advertising or product endorsement purposes. NR 25 TC 22 Z9 22 U1 0 U2 67 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 0013-936X J9 ENVIRON SCI TECHNOL JI Environ. Sci. Technol. PD JAN 1 PY 2013 VL 47 IS 1 BP 252 EP 261 DI 10.1021/es301269k PG 10 WC Engineering, Environmental; Environmental Sciences SC Engineering; Environmental Sciences & Ecology GA 066KS UT WOS:000313220300031 PM 22873684 ER PT J AU Smith, MM Sholokhova, Y Hao, Y Carroll, SA AF Smith, Megan M. Sholokhova, Yelena Hao, Yue Carroll, Susan A. TI Evaporite Caprock Integrity: An Experimental Study of Reactive Mineralogy and Pore-Scale Heterogeneity during Brine-CO2 Exposure SO ENVIRONMENTAL SCIENCE & TECHNOLOGY LA English DT Article ID WORMHOLE FORMATION; CO2 SEQUESTRATION; CARBON-DIOXIDE; POROUS-MEDIUM; OIL; FLUID; DISSOLUTION; STORAGE; MEDIA; FLOW AB We present characterization and geochemical data from a core-flooding experiment on a sample from the Three Fingers evaporite unit forming the lower extent of caprock at the Weyburn-Midale reservoir, Canada. This low-permeability sample was characterized in detail using X-ray computed microtomography before and after exposure to CO2-acidified brine, allowing mineral phase and voidspace distributions to be quantified in three dimensions. Solution chemistry indicated that CO2-acidified brine preferentially dissolved dolomite until saturation was attained, while anhydrite remained unreactive. Dolomite dissolution contributed to increases in bulk permeability through the formation of a localized channel, guided by microfractures as well as porosity and reactive phase distributions aligned with depositional bedding. An indirect effect of carbonate mineral reactivity with CO2-acidified solution is voidspace generation through physical transport of anhydrite freed from the rock matrix following dissolution of dolomite. The development of high permeability fast pathways in this experiment highlights the role of carbonate content and potential fracture orientations in evaporite caprock formations considered for both geologic carbon sequestration and CO2-enhanced oil recovery operations. C1 [Smith, Megan M.] Lawrence Livermore Natl Lab, Atmospher Earth & Energy Div, Livermore, CA 94550 USA. RP Smith, MM (reprint author), Lawrence Livermore Natl Lab, Atmospher Earth & Energy Div, L-231,7000 East Ave, Livermore, CA 94550 USA. EM megan@llnl.gov FU U.S. Department of Energy by Lawrence Livermore National Laboratory [DE-AC52-07NA27344, LLNL-JRNL-572955]; U.S. Department of Energy, Fossil Energy, Carbon Sequestration Program; Petroleum Research Technology Centre (PTRC); IEA-GHG Weyburn-Midale Monitoring and Storage Project; Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231] 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, LLNL-JRNL-572955. Funding for this work was provided from both the U.S. Department of Energy, Fossil Energy, Carbon Sequestration Program; and the Petroleum Research Technology Centre (PTRC), IEA-GHG Weyburn-Midale Monitoring and Storage Project. The authors are grateful for the efforts of LLNL personnel Rick Kemptner and Dave Ruddle (experimental fabrication), Sharon Torres (SEM data acquisition), Victoria Genetti and Rachel Lindvall (ICP-MIS analyses), and Harris Mason (image analysis assistance). The prereaction data were collected on the ID-19 beamline at the European Synchotron Radiation Facility, Grenoble, France, and we thank Paul Tafforeau at ESRF for providing assistance. The Advanced Light Source is supported by the Director, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No.DE-AC02-05CH11231, and we thank Alastair MacDowell and Dula Parkinson (ALS, LBNL) for their help with postreaction data acquisition on the 8.3.2 beamline. Ian Hutcheon and Maurice Shevalier (Univ. of Calgary) graciously shared their petrologic data. We thank the associate editor and four anonymous reviewers for their constructive comments. NR 30 TC 31 Z9 31 U1 1 U2 49 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 0013-936X EI 1520-5851 J9 ENVIRON SCI TECHNOL JI Environ. Sci. Technol. PD JAN 1 PY 2013 VL 47 IS 1 BP 262 EP 268 DI 10.1021/es3012723 PG 7 WC Engineering, Environmental; Environmental Sciences SC Engineering; Environmental Sciences & Ecology GA 066KS UT WOS:000313220300032 PM 22831758 ER PT J AU Huerta, NJ Hesse, MA Bryant, SL Strazisar, BR Lopano, CL AF Huerta, Nicolas J. Hesse, Marc A. Bryant, Steven L. Strazisar, Brian R. Lopano, Christina L. TI Experimental Evidence for Self-Limiting Reactive Flow through a Fractured Cement Core: Implications for Time-Dependent Wellbore Leakage SO ENVIRONMENTAL SCIENCE & TECHNOLOGY LA English DT Article ID GEOLOGIC SEQUESTRATION CONDITIONS; HYDROCHLORIC-ACID; ROCK FRACTURE; CO2; PRECIPITATION; DISSOLUTION; ATTACK; MEDIA; MORTAR AB We present a set of reactive transport experiments in cement fractures. The experiments simulate coupling between flow and reaction when acidic, CO2-rich fluids flow along a leaky wellbore. An analog dilute acid with a pH between 2.0 and 3.15 was injected at constant rate between 0.3 and 9.4 cm/s into a fractured cement core. Pressure differential across the core and effluent pH were measured to track flow path evolution, which was analyzed with electron microscopy after injection. In many experiments reaction was restricted within relatively narrow, tortuous channels along the fracture surface. The observations are consistent with coupling between flow and dissolution/precipitation. Injected acid reacts along the fracture surface to leach calcium from cement phases. Ahead of the reaction front, high pH pore fluid mixes with calcium-rich water and induces mineral precipitation. Increases in the pressure differential for most experiments indicate that precipitation can be sufficient to restrict flow. Experimental data from this study combined with published field evidence for mineral precipitation along cemented annuli suggests that leakage of CO2-rich fluids along a wellbore may seal the leakage pathway if the initial aperture is small and residence time allows mobilization and precipitation of minerals along the fracture. C1 [Huerta, Nicolas J.; Hesse, Marc A.] Univ Texas Austin, Jackson Sch Geosci, Austin, TX 78712 USA. [Bryant, Steven L.] Univ Texas Austin, Dept Petr & Geosyst Engn, Austin, TX 78712 USA. [Huerta, Nicolas J.; Strazisar, Brian R.; Lopano, Christina L.] US DOE, Natl Energy Technol Lab, Pittsburgh, PA 15236 USA. RP Huerta, NJ (reprint author), Univ Texas Austin, Jackson Sch Geosci, Austin, TX 78712 USA. EM njhuerta@utexas.edu RI Hesse, Marc/B-4914-2011 OI Hesse, Marc/0000-0002-2532-3274 FU Geological CO2 Storage Industrial Affiliates Program at the Center for Petroleum and Geosystems Engineering at UT-Austin; Carbon Sequestration program of the U.S. DOE National Energy Technology Laboratory FX Partial support for this work comes from the Geological CO2 Storage Industrial Affiliates Program at the Center for Petroleum and Geosystems Engineering at UT-Austin. This work was also supported by the Carbon Sequestration program of the U.S. DOE National Energy Technology Laboratory. We would also like to thank Karl Jarvis for the abstract image, Barbara Kutchko for discussions on cement chemistry and carbonic acid attack of cement, and Corinne Disenhof for help with mu XRD. NR 27 TC 26 Z9 26 U1 0 U2 37 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 0013-936X J9 ENVIRON SCI TECHNOL JI Environ. Sci. Technol. PD JAN 1 PY 2013 VL 47 IS 1 BP 269 EP 275 DI 10.1021/es3013003 PG 7 WC Engineering, Environmental; Environmental Sciences SC Engineering; Environmental Sciences & Ecology GA 066KS UT WOS:000313220300033 PM 22894832 ER PT J AU Newell, DL Carey, JW AF Newell, Dennis L. Carey, J. William TI Experimental Evaluation of Wellbore Integrity Along the Cement-rock Boundary SO ENVIRONMENTAL SCIENCE & TECHNOLOGY LA English DT Article ID GEOLOGIC SEQUESTRATION CONDITIONS; CO2; ANNULUS; WELLS AB Leakage of CO2 and brine from geologic storage reservoirs along wellbores is a major risk factor to the success of geologic carbon sequestration. We conducted multiphase [supercritical (sc)CO2-brine] coreflood experiments that simulate a leakage pathway along the cement/rock interface. A composite core constructed of oil-well cement and siltstone separated by a simulated damage zone (defect) containing ground cement and siltstone was flooded with brine + scCO(2) at 10 MPa and 60 degrees C parallel to the defect. During coinjection of scCO2, the effective brine permeability decreased from similar to 200 to 90 mD due to transition to two-phase flow and then further declined to 35 mD. CO2 injection resulted in a pH drop from 11 to 4 and carbonate-undersaturated conditions in the produced brine. Microscopy revealed leaching and erosion along the defect, a carbonation front extending 5 mm into the cement, parallel to the damage zone, and no change in the dimensions of the defect. Carbonation of cement does not appear to explain the permeability drop, which is attributed to the migration and reprecipitation of alteration products derived from cement within the defect. This study shows the potential for self-limiting flow along wellbore defects despite flow of aggressive scCO(2)-brine mixtures. C1 [Newell, Dennis L.; Carey, J. William] Los Alamos Natl Lab, Los Alamos, NM 87544 USA. RP Newell, DL (reprint author), Los Alamos Natl Lab, Los Alamos, NM 87544 USA. EM dnewell@lanl.gov FU CO2 Capture Project FX We thank the CO2 Capture Project (www.co2captureproject.org), a research partnership of major energy companies, for financial support, and Walter Crow for discussions and comments. The manuscript greatly benefited from three anonymous reviews. NR 25 TC 25 Z9 25 U1 3 U2 36 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 0013-936X J9 ENVIRON SCI TECHNOL JI Environ. Sci. Technol. PD JAN 1 PY 2013 VL 47 IS 1 BP 276 EP 282 DI 10.1021/es3011404 PG 7 WC Engineering, Environmental; Environmental Sciences SC Engineering; Environmental Sciences & Ecology GA 066KS UT WOS:000313220300034 PM 22663177 ER PT J AU Jung, HB Jansik, D Um, W AF Jung, Hun Bok Jansik, Danielle Um, Wooyong TI Imaging Wellbore Cement Degradation by Carbon Dioxide under Geologic Sequestration Conditions Using X-ray Computed Microtomography SO ENVIRONMENTAL SCIENCE & TECHNOLOGY LA English DT Article ID PORE STRUCTURE; CO2; CONCRETE; DENSITY; ATTACK; PASTE AB X-ray microtomography (XMT), a nondestructive three-dimensional imaging technique, was applied to demonstrate its capability to visualize the mineralogical alteration and microstructure changes in hydrated Portland cement exposed to carbon dioxide under geologic sequestration conditions. Steel coupons and basalt fragments were added to the cement paste in order to simulate cement-steel and cement-rock interfaces. XMT image analysis showed the changes of material density and porosity in the degradation front (density: 1.98 g/cm(3), porosity: 40%) and the carbonated zone (density: 2.27 g/cm(3), porosity: 23%) after reaction with CO2-saturated water for 5 months compared to unaltered cement (density: 2.15 g/cm(3), porosity: 30%). Three-dimensional XMT imaging was capable of displaying spatially heterogeneous alteration in cement pores, calcium carbonate precipitation in cement cracks, and preferential cement alteration along the cement-steel and cement-rock interfaces. This result also indicates that the interface between cement and host rock or steel casing is likely more vulnerable to a CO2 attack than the cement matrix in a wellbore environment. It is shown here that XMT imaging can potentially provide a new insight into the physical and chemical degradation of wellbore cement by CO2 leakage. C1 [Jung, Hun Bok; Jansik, Danielle; Um, Wooyong] Pacific NW Natl Lab, Richland, WA 99354 USA. RP Um, W (reprint author), Pacific NW Natl Lab, POB 999,P7-54,902 Battelle Blvd, Richland, WA 99354 USA. EM wooyong.um@pnnl.gov FU National Risk Assessment Partnership (NRAP) program of U.S. Department of Energy (DOE) FX We are thankful to Paul Martin for preparing the cement columns and the experiment design. This work was funded by National Risk Assessment Partnership (NRAP) program of U.S. Department of Energy (DOE). NR 33 TC 15 Z9 15 U1 2 U2 37 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 0013-936X J9 ENVIRON SCI TECHNOL JI Environ. Sci. Technol. PD JAN 1 PY 2013 VL 47 IS 1 BP 283 EP 289 DI 10.1021/es3012707 PG 7 WC Engineering, Environmental; Environmental Sciences SC Engineering; Environmental Sciences & Ecology GA 066KS UT WOS:000313220300035 PM 22823234 ER PT J AU Keating, EH Newell, DL Viswanathan, H Carey, JW Zyvoloski, G Pawar, R AF Keating, Elizabeth H. Newell, Dennis L. Viswanathan, Hari Carey, J. W. Zyvoloski, G. Pawar, Rajesh TI CO2/Brine Transport into Shallow Aquifers along Fault Zones SO ENVIRONMENTAL SCIENCE & TECHNOLOGY LA English DT Article ID COLORADO PLATEAU; CO2; USA; RESERVOIRS; SYSTEMS; STORAGE; TEXAS; WATER; FIELD AB Unintended release of CO2 from carbon sequestration reservoirs poses a well-recognized risk to groundwater quality. Research has largely focused on in situ CO2-induced pH depression and subsequent trace metal mobilization. In this paper we focus on a second mechanism: upward intrusion of displaced brine or brackish-water into a shallow aquifer as a result of CO2 injection. Studies of two natural analog sites provide insights into physical and chemical mechanisms controlling both brackish water and CO2 intrusion into shallow aquifers along fault zones. At the Chimayo, New Mexico site, shallow groundwater near the fault is enriched in CO2 and, in some places, salinity is significantly elevated. In contrast, at the Springerville, Arizona site CO2 is leaking upward through brine aquifers but does not appear to be increasing salinity in the shallow aquifer. Using multiphase transport simulations we show conditions under which significant CO2 can be transported through deep brine aquifers into shallow layers. Only a subset of these conditions favor entrainment of salinity into the shallow aquifer: high aspect-ratio leakage pathways and viscous coupling between the fluid phases. Recognition of the conditions under which salinity is favored to be cotransported with CO2 into shallow aquifers will be important in environmental risk assessments. C1 [Keating, Elizabeth H.; Newell, Dennis L.; Viswanathan, Hari; Carey, J. W.; Zyvoloski, G.; Pawar, Rajesh] Los Alamos Natl Lab, Div Earth & Environm Sci, Los Alamos, NM 87545 USA. RP Keating, EH (reprint author), Los Alamos Natl Lab, Div Earth & Environm Sci, Los Alamos, NM 87545 USA. EM ekeating@lanl.gov FU Department of Energy National Risk Assessment Program FX We are grateful to the Tuscon Electric Power Company staff for access to wells and permission to sample. This work has been funded by the Department of Energy National Risk Assessment Program. NR 26 TC 19 Z9 19 U1 2 U2 45 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 0013-936X J9 ENVIRON SCI TECHNOL JI Environ. Sci. Technol. PD JAN 1 PY 2013 VL 47 IS 1 BP 290 EP 297 DI 10.1021/es301495x PG 8 WC Engineering, Environmental; Environmental Sciences SC Engineering; Environmental Sciences & Ecology GA 066KS UT WOS:000313220300036 PM 22799449 ER PT J AU Trautz, RC Pugh, JD Varadharajan, C Zheng, LG Bianchi, M Nico, PS Spycher, NF Newell, DL Esposito, RA Wu, YX Dafflon, B Hubbard, SS Birkholzer, JT AF Trautz, Robert C. Pugh, John D. Varadharajan, Charuleka Zheng, Liange Bianchi, Marco Nico, Peter S. Spycher, Nicolas F. Newell, Dennis L. Esposito, Richard A. Wu, Yuxin Dafflon, Baptiste Hubbard, Susan S. Birkholzer, Jens T. TI Effect of Dissolved CO2 on a Shallow Groundwater System: A Controlled Release Field Experiment SO ENVIRONMENTAL SCIENCE & TECHNOLOGY LA English DT Article ID CARBON SEQUESTRATION; LEAKAGE; WATER; IRON; CHEMISTRY; MINERALS; IMPACTS; STORAGE; SITE AB Capturing carbon dioxide (CO2) emissions from industrial sources and injecting the emissions deep underground in geologic formations is one method being considered to control CO2 concentrations in the atmosphere. Sequestering CO2 underground has its own set of environmental risks, including the potential migration of CO2 out of the storage reservoir and resulting acidification and release of trace constituents in shallow groundwater. A field study involving the controlled release of groundwater containing dissolved CO2 was initiated to investigate potential groundwater impacts. Dissolution of CO2 in the groundwater resulted in a sustained and easily detected decrease of similar to 3 pH units. Several trace constituents, including As and Pb, remained below their respective detections limits and/or at background levels. Other constituents (Ba, Ca, Cr, Sr, Mg, Mn, and Fe) displayed a pulse response, consisting of an initial increase in concentration followed by either a return to background levels or slightly greater than background. This suggests a fast-release mechanism (desorption, exchange, and/or fast dissolution of small finite amounts of metals) concomitant in some cases with a slower release potentially involving different solid phases or mechanisms. Inorganic constituents regulated by the U.S. Environmental Protection Agency remained below their respective maximum contaminant levels throughout the experiment. C1 [Trautz, Robert C.] Elect Power Res Inst, Palo Alto, CA 94304 USA. [Pugh, John D.; Esposito, Richard A.] So Co Serv Inc, Birmingham, AL 35291 USA. [Varadharajan, Charuleka; Zheng, Liange; Bianchi, Marco; Nico, Peter S.; Spycher, Nicolas F.; Wu, Yuxin; Dafflon, Baptiste; Hubbard, Susan S.; Birkholzer, Jens T.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, Berkeley, CA 94720 USA. [Newell, Dennis L.] Los Alamos Natl Lab, Earth & Environm Sci Div EES 14, Los Alamos, NM 87545 USA. RP Trautz, RC (reprint author), Elect Power Res Inst, 3420 Hillview Ave, Palo Alto, CA 94304 USA. EM rtrautz@epri.com RI Birkholzer, Jens/C-6783-2011; zheng, liange/B-9748-2011; Nico, Peter/F-6997-2010; Dafflon, Baptiste/G-2441-2015; Hubbard, Susan/E-9508-2010; Spycher, Nicolas/E-6899-2010; Varadharajan, Charuleka/G-3741-2015; Wu, Yuxin/G-1630-2012 OI Birkholzer, Jens/0000-0002-7989-1912; zheng, liange/0000-0002-9376-2535; Nico, Peter/0000-0002-4180-9397; Varadharajan, Charuleka/0000-0002-4142-3224; Wu, Yuxin/0000-0002-6953-0179 FU Electric Power Research Institute; EPA, Office of Water; U.S. Department of Energy (DOE) at LBNL [DE-AC02-05CH11231]; Assistant Secretary for Fossil Energy, National Energy Technology Laboratory (NETL), National Risk Assessment Program (NRAP), of the US Department of Energy [DEAC02-05CH11231] FX This work was supported by the Electric Power Research Institute; the EPA, Office of Water, under an Interagency Agreement with the U.S. Department of Energy (DOE) at LBNL, under contract number DE-AC02-05CH11231; and the Assistant Secretary for Fossil Energy, National Energy Technology Laboratory (NETL), National Risk Assessment Program (NRAP), of the US Department of Energy under Contract No. DEAC02-05CH11231. NR 23 TC 66 Z9 67 U1 4 U2 79 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 0013-936X J9 ENVIRON SCI TECHNOL JI Environ. Sci. Technol. PD JAN 1 PY 2013 VL 47 IS 1 BP 298 EP 305 DI 10.1021/es301280t PG 8 WC Engineering, Environmental; Environmental Sciences SC Engineering; Environmental Sciences & Ecology GA 066KS UT WOS:000313220300037 PM 22950750 ER PT J AU Dafflon, B Wu, YX Hubbard, SS Birkholzer, JT Daley, TM Pugh, JD Peterson, JE Trautz, RC AF Dafflon, Baptiste Wu, Yuxin Hubbard, Susan S. Birkholzer, Jens T. Daley, Thomas M. Pugh, John D. Peterson, John E. Trautz, Robert C. TI Monitoring CO2 Intrusion and Associated Geochemical Transformations in a Shallow Groundwater System Using Complex Electrical Methods SO ENVIRONMENTAL SCIENCE & TECHNOLOGY LA English DT Article ID CONDUCTIVITY; RESISTIVITY; AQUIFER; FIELD; SITE AB The risk of CO2 leakage from a properly permitted deep geologic storage facility is expected to be very low. However, if leakage occurs it could potentially impact potable groundwater quality. Dissolved CO2 in groundwater decreases pH, which can mobilize naturally occurring trace metals commonly contained in aquifer sediments. Observing such processes requires adequate monitoring strategies. Here, we use laboratory and field experiments to explore the sensitivity of time-lapse complex resistivity responses for remotely monitoring dissolved CO2 distribution and geochemical transformations that may impact groundwater quality. Results show that electrical resistivity and phase responses correlate well with dissolved CO2 injection processes. Specifically, resistivity initially decreases due to increase of bicarbonate and dissolved species. As pH continues to decrease, the resistivity rebounds toward initial conditions due to the transition of bicarbonate into nondissociated carbonic acid, which reduces the total concentration of dissociated species and thus the water conductivity. An electrical phase decrease is also observed, which is interpreted to be driven by the decrease of surface charge density as well as potential mineral dissolution and ion exchange. Both laboratory and field experiments demonstrate the potential of field complex resistivity method for remotely monitoring changes in groundwater quality due to CO2 leakage. C1 [Dafflon, Baptiste; Wu, Yuxin; Hubbard, Susan S.; Birkholzer, Jens T.; Daley, Thomas M.; Peterson, John E.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Pugh, John D.] So Co Serv Inc, Birmingham, AL 35291 USA. [Trautz, Robert C.] Elect Power Res Inst, Palo Alto, CA 94304 USA. RP Dafflon, B (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, 1 Cyclotron Rd, Berkeley, CA 94720 USA. EM BDafflon@lbl.gov RI Birkholzer, Jens/C-6783-2011; Dafflon, Baptiste/G-2441-2015; Daley, Thomas/G-3274-2015; Hubbard, Susan/E-9508-2010; Wu, Yuxin/G-1630-2012 OI Birkholzer, Jens/0000-0002-7989-1912; Daley, Thomas/0000-0001-9445-0843; Wu, Yuxin/0000-0002-6953-0179 FU Assistant Secretary for Fossil Energy, National Energy Technology Laboratory (NETL), National Risk Assessment Program (NRAP), of the U.S. Department of Energy [DEAC02-05CH11231]; Electric Power Research Institute FX This work was funded by the Assistant Secretary for Fossil Energy, National Energy Technology Laboratory (NETL), National Risk Assessment Program (NRAP), of the U.S. Department of Energy under Contract No. DEAC02-05CH11231 in collaboration with the Electric Power Research Institute. We thank Dr. A. Kemna and M. Weigand at University of Bonn for providing the 2D complex resistivity imaging code. NR 33 TC 21 Z9 21 U1 0 U2 32 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 0013-936X J9 ENVIRON SCI TECHNOL JI Environ. Sci. Technol. PD JAN 1 PY 2013 VL 47 IS 1 BP 314 EP 321 DI 10.1021/es301260e PG 8 WC Engineering, Environmental; Environmental Sciences SC Engineering; Environmental Sciences & Ecology GA 066KS UT WOS:000313220300039 PM 22681490 ER PT J AU Karamalidis, AK Torres, SG Hakala, JA Shao, HB Cantrell, KJ Carroll, S AF Karamalidis, Athanasios K. Torres, Sharon G. Hakala, J. Alexandra Shao, Hongbo Cantrell, Kirk J. Carroll, Susan TI Trace Metal Source Terms in Carbon Sequestration Environments SO ENVIRONMENTAL SCIENCE & TECHNOLOGY LA English DT Article ID DEEP SALINE AQUIFERS; CO2 SEQUESTRATION; STORAGE; WATER; SOLUBILITY; LEAKAGE; BRINE; SITE; INJECTION; CHEMISTRY AB Carbon dioxide sequestration in deep saline and depleted oil geologic formations is feasible and promising; however, possible CO2 or CO2-saturated brine leakage to overlying aquifers may pose environmental and health impacts. The purpose of this study was to experimentally define a range of concentrations that can be used as the trace element source term for reservoirs and leakage pathways in risk simulations. Storage source terms for trace metals are needed to evaluate the impact of brines leaking into overlying drinking water aquifers. The trace metal release was measured from cements and sandstones, shales, carbonates, evaporites, and basalts from the Frio, In Salah, Illinois Basin, Decatur, Lower Tuscaloosa, Weyburn-Midale, Bass Islands, and Grand Ronde carbon sequestration geologic formations. Trace metal dissolution was tracked by measuring solution concentrations over time under conditions (e.g., pressures, temperatures, and initial brine compositions) specific to the sequestration projects. Existing metrics for maximum contaminant levels (MCLs) for drinking water as defined by the U.S. Environmental Protection Agency (U.S. EPA) were used to categorize the relative significance of metal concentration changes in storage environments because of the presence of CO2. Results indicate that Cr and Pb released from sandstone reservoir and shale cap rocks exceed the MCLs by an order of magnitude, while Cd and Cu were at or below drinking water thresholds. In carbonate reservoirs As exceeds the MCLs by an order of magnitude, while Cd, Cu, and Pb were at or below drinking water standards. Results from this study can be used as a reasonable estimate of the trace element source term for reservoirs and leakage pathways in risk simulations to further evaluate the impact of leakage on groundwater quality. C1 [Karamalidis, Athanasios K.] Carnegie Mellon Univ, Pittsburgh, PA 15213 USA. [Karamalidis, Athanasios K.; Hakala, J. Alexandra] US DOE, Natl Energy Technol Lab, Pittsburgh, PA 15236 USA. [Torres, Sharon G.; Carroll, Susan] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. [Shao, Hongbo; Cantrell, Kirk J.] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Carroll, S (reprint author), Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. EM carroll6@llnl.gov RI Shao, Hongbo/N-4169-2013 FU DOE Office of Fossil Energy's Crosscutting Research program; U.S. Department of Energy by Carnegie Mellon University and National Energy Technology Laboratory [DE-FE0004000]; Lawrence Livermore National Laboratory [DE-AC52-07NA27344]; Pacific Northwest National Laboratory; U.S. Department of Energy by Battelle Memorial Institute [DE-AC05-76RL01830] FX We wish to thank LLNL personnel Victoria Genetti, Rachel Lindvall, and Megan Smith and URS-Pittsburgh personnel for analyzing the solution compositions. This work was supported by Department of Energy, Office of Basic Energy Science. This work was completed as part of National Risk Assessment Partnership (NRAP) project. Support for this project came from the DOE Office of Fossil Energy's Crosscutting Research program. The authors wish to acknowledge Robert Romanosky (NETL Strategic Center for Coal) and Regis Conrad (DOE Office of Fossil Energy) for programmatic guidance, direction, and support. This work was performed under the auspices of the U.S. Department of Energy by Carnegie Mellon University and National Energy Technology Laboratory under contract DE-FE0004000, Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344, and Pacific Northwest National Laboratory, which is operated for U.S. Department of Energy by Battelle Memorial Institute under contract DE-AC05-76RL01830. NR 43 TC 19 Z9 19 U1 3 U2 74 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 0013-936X J9 ENVIRON SCI TECHNOL JI Environ. Sci. Technol. PD JAN 1 PY 2013 VL 47 IS 1 BP 322 EP 329 DI 10.1021/es304832m PG 8 WC Engineering, Environmental; Environmental Sciences SC Engineering; Environmental Sciences & Ecology GA 066KS UT WOS:000313220300040 PM 23215015 ER PT J AU Stewart, BD Girardot, C Spycher, N Sani, RK Peyton, BM AF Stewart, Brandy D. Girardot, Crystal Spycher, Nicolas Sani, Rajesh K. Peyton, Brent M. TI Influence of Chelating Agents on Biogenic Uraninite Reoxidation by Fe(III) (Hydr)oxides SO ENVIRONMENTAL SCIENCE & TECHNOLOGY LA English DT Article ID SULFATE-REDUCING CONDITIONS; SHEWANELLA-PUTREFACIENS; IRON(III) (HYDR)OXIDES; URANIUM REDUCTION; ORGANIC-LIGANDS; DISSOLUTION; PRECIPITATION; SEDIMENT; BACTERIA; U(VI) AB Microbially mediated reduction of soluble U(VI) to U(IV) with subsequent precipitation of uraninite, UO2(s), has been proposed as a method for limiting uranium (U) migration. However, microbially reduced UO2 may be susceptible to reoxidation by environmental factors, with Fe(III) (hydr)oxides playing a significant role. Little is known about the role that organic compounds such as Fe(III) chelators play in the stability of reduced U. Here, we investigate the impact of citrate, DFB, EDTA, and NTA on biogenic UO2 recaidation with ferrihydrite, goethite, and hematite. Experiments were conducted in anaerobic batch systems in PIPES buffer (10 mM, pH 7) with bicarbonate for approximately 80 days. Results showed EDTA accelerated UO2 reoxidation the most at an initial rate of 9.5 mu M day(-1) with ferrihydrite, 8.6 mu M day(-1) with goethite, and 8.8 mu M day(-1) with hematite. NTA accelerated UO2 reoxidation with ferrihydrite at a rate of 4.8 mu M day(-1); rates were less with goethite and hematite (0.66 and 0.71 mu M day(-1), respectively). Citrate increased UO2 reoxidation with ferrihydrite at a rate of 1.8 mu M day(-1), but did not increase the extent of reaction with goethite or hematite, with no reoxidation in this case. In all cases, bicarbonate increased the rate and extent of UO2 reoxidation with ferrihydrite in the presence and absence of chelators. The highest rate of UO2 reoxidation occurred when the chelator promoted both UO2 and Fe(III) (hydr)oxide dissolution as demonstrated with EDTA When UO2 dissolution did not occur, UO2 reoxidation likely proceeded through an aqueous Fe(III) intermediate with lower reoxidation rates observed. Reaction modeling suggests that strong Fe(II) chelators promote reoxidation whereas strong Fe (III) chelators impede it. These results indicate that chelators found in U contaminated sites may play a significant role in mobilizing U, potentially affecting bioremediation efforts. C1 [Stewart, Brandy D.; Girardot, Crystal; Peyton, Brent M.] Montana State Univ, Ctr Biofilm Engn, Bozeman, MT 59717 USA. [Spycher, Nicolas] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, Berkeley, CA 94720 USA. [Sani, Rajesh K.] S Dakota Sch Mines & Technol, Chem & Biol Engn Dept, Rapid City, SD 57701 USA. RP Peyton, BM (reprint author), Montana State Univ, Ctr Biofilm Engn, Bozeman, MT 59717 USA. EM bpeyton@coe.montana.edu RI Peyton, Brent/G-5247-2015; Spycher, Nicolas/E-6899-2010 OI Peyton, Brent/0000-0003-0033-0651; FU U.S. Department of Energy's Subsurface Biogeochemical Research program [DE-FG02-07ER-64366] FX We thank Tim Ginn for his valuable input on conceptual project design and interpretation of results. We also thank the Environmental Molecular Sciences Laboratory for imaging. This research was funded by the U.S. Department of Energy's Subsurface Biogeochemical Research program under Project No. DE-FG02-07ER-64366. NR 39 TC 6 Z9 6 U1 2 U2 57 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 0013-936X J9 ENVIRON SCI TECHNOL JI Environ. Sci. Technol. PD JAN 1 PY 2013 VL 47 IS 1 BP 364 EP 371 DI 10.1021/es303022p PG 8 WC Engineering, Environmental; Environmental Sciences SC Engineering; Environmental Sciences & Ecology GA 066KS UT WOS:000313220300047 PM 23163577 ER PT J AU Borole, AP Hamilton, CY Schell, DJ AF Borole, Abhijeet P. Hamilton, Choo Y. Schell, Daniel J. TI Conversion of Residual Organics in Corn Stover-Derived Biorefinery Stream to Bioenergy via a Microbial Fuel Cell SO ENVIRONMENTAL SCIENCE & TECHNOLOGY LA English DT Article ID ELECTRICITY-GENERATION; ETHANOL; WATER; DEGRADATION; STILLAGE; XYLOSE AB A biorefinery process typically uses about 4-10 times more water than the amount of biofuel generated. The wastewater produced in a biorefinery process contains residual sugars, 5-furfural, phenolics, and other pretreatment and fermentation byproducts. Treatment of the wastewater can reduce the need for fresh water and potentially add to the environmental benefits of the process. Use of microbial fuel cells (MFCs) for conversion of the complete range of phenolic compounds and furan aldehyde derivatives present in a postfermentation biorefinery stream is reported here. The consortium was capable of removing the molecules simultaneously with sugars, which were present at 2 orders of magnitude higher concentrations. Organic loading in a fed-batch MFC affected Coulombic efficiency, which decreased from 40% at 0.66 g/L loading to 1.8% at 66.4 g/L loading. Power density increased with loading reaching 1180 mW/m(2) at 5.3 g/L (8% dilution), but decreased thereafter. Excessive loading leads to poor electrogenic performance; therefore, operation of an MPG at an intermediate loading using dilution and recirculation of the process stream can enable effective treatment with bioenergy recovery. C1 [Borole, Abhijeet P.] Oak Ridge Natl Lab, Biosci Div, Oak Ridge, TN 37831 USA. [Borole, Abhijeet P.; Hamilton, Choo Y.] Univ Tennessee, Knoxville, TN USA. [Schell, Daniel J.] Natl Renewable Energy Lab, Golden, CO USA. RP Borole, AP (reprint author), Oak Ridge Natl Lab, Biosci Div, Oak Ridge, TN 37831 USA. EM borolea@oml.gov OI Borole, Abhijeet/0000-0001-8423-811X FU U.S. Department of Energy Office of the Biomass Program; National Renewable Energy Laboratory (NREL); Laboratory Directed Research and Development Program of Oak Ridge National Laboratory (ORNL); U.S. Department of Energy [DE AC05-00OR22725] FX This research was sponsored by the U.S. Department of Energy Office of the Biomass Program through an agreement with the National Renewable Energy Laboratory (NREL) as well as the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory (ORNL), managed by UT-Battelle, LLC, for the U.S. Department of Energy under Contract No. DE AC05-00OR22725. NR 24 TC 17 Z9 17 U1 2 U2 74 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 0013-936X J9 ENVIRON SCI TECHNOL JI Environ. Sci. Technol. PD JAN 1 PY 2013 VL 47 IS 1 BP 642 EP 648 DI 10.1021/es3023495 PG 7 WC Engineering, Environmental; Environmental Sciences SC Engineering; Environmental Sciences & Ecology GA 066KS UT WOS:000313220300082 PM 23194288 ER PT J AU Powers, RF Busse, MD McFarlane, KJ Zhang, JW Young, DH AF Powers, Robert F. Busse, Matt D. McFarlane, Karis J. Zhang, Jianwei Young, David H. TI Long-term effects of silviculture on soil carbon storage: does vegetation control make a difference? SO FORESTRY LA English DT Article ID ORGANIC-MATTER REMOVAL; PONDEROSA PINE; MINERAL SOIL; COMPETING-VEGETATION; NORTHERN CALIFORNIA; FOREST MANAGEMENT; LOGGING-DEBRIS; UNITED-STATES; PRODUCTIVITY; PLANTATIONS AB Forests and the soils beneath them are Earths largest terrestrial sinks for atmospheric carbon (C) and healthy forests provide a partial check against atmospheric rises in CO2. Consequently, there is global interest in crediting forest managers who enhance C retention. Interest centres on C acquisition and storage in trees. Less is directed to understorey management practices that affect early forest development. Even less is paid to the largest ecosystem reservoir of all the mineral soil. Understorey vegetation control is a common management practice to boost stand growth, but the consequence of this on ecosystem C storage is poorly understood. We addressed this by pooling data from five independent groups of long-term studies in the western US. Understorey control increased overstorey biomass universally, but C contents of the forest floor and top 30 cm of mineral soil largely were unaffected. Net soil C increment averaged 1.3 Mg C ha(1) year(1) in the first decade. We conclude that soil C storage is not affected adversely by vegetation management in forests under a Mediterranean climate. However, understorey shrubs can profoundly affect stand susceptibility to wildfire. We propose that C accounting systems be strengthened by assessing understorey management practices relative to wildfire risk. C1 [Powers, Robert F.; Busse, Matt D.; Zhang, Jianwei] US Forest Serv, Pacific SW Res Stn, USDA, Redding, CA 96002 USA. [McFarlane, Karis J.] Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. RP Powers, RF (reprint author), US Forest Serv, Pacific SW Res Stn, USDA, 3644 Avtech Pkwy, Redding, CA 96002 USA. EM rpowers@c-zone.net OI McFarlane, Karis/0000-0001-6390-7863 FU USDA Forest Service; USDA Forest Service National Fire Plan; Sierra-Cascade Intensive Forest Management Research Cooperative; Sierra Pacific Industries FX This work was funded primarily by congressional appropriations to the USDA Forest Service. Garden of Eden findings reported by McFarlane et al.23,24 were supported in part by grants from the USDA Forest Service National Fire Plan, Sierra-Cascade Intensive Forest Management Research Cooperative and Sierra Pacific Industries. NR 50 TC 8 Z9 9 U1 1 U2 39 PU OXFORD UNIV PRESS PI OXFORD PA GREAT CLARENDON ST, OXFORD OX2 6DP, ENGLAND SN 0015-752X J9 FORESTRY JI Forestry PD JAN PY 2013 VL 86 IS 1 BP 47 EP 58 DI 10.1093/forestry/cps067 PG 12 WC Forestry SC Forestry GA 071UA UT WOS:000313619300006 ER PT J AU Manning, VA Pandelova, I Dhillon, B Wilhelm, LJ Goodwin, SB Berlin, AM Figueroa, M Freitag, M Hane, JK Henrissat, B Holman, WH Kodira, CD Martin, J Oliver, RP Robbertse, B Schackwitz, W Schwartz, DC Spatafora, JW Turgeon, BG Yandava, C Young, S Zhou, SG Zeng, QD Grigoriev, IV Ma, LJ Ciuffetti, LM AF Manning, Viola A. Pandelova, Iovanna Dhillon, Braham Wilhelm, Larry J. Goodwin, Stephen B. Berlin, Aaron M. Figueroa, Melania Freitag, Michael Hane, James K. Henrissat, Bernard Holman, Wade H. Kodira, Chinnappa D. Martin, Joel Oliver, Richard P. Robbertse, Barbara Schackwitz, Wendy Schwartz, David C. Spatafora, Joseph W. Turgeon, B. Gillian Yandava, Chandri Young, Sarah Zhou, Shiguo Zeng, Qiandong Grigoriev, Igor V. Ma, Li-Jun Ciuffetti, Lynda M. TI Comparative Genomics of a Plant-Pathogenic Fungus, Pyrenophora tritici-repentis, Reveals Transduplication and the Impact of Repeat Elements on Pathogenicity and Population Divergence SO G3-GENES GENOMES GENETICS LA English DT Article DE wheat (Triticum aestivum); copy number variation; histone H3 transduplication; ToxA; ToxB; anastomosis ID HOST-SELECTIVE TOXIN; BERBERINE BRIDGE ENZYME; NONRIBOSOMAL PEPTIDE SYNTHETASES; BIOSYNTHETIC GENE-CLUSTER; INDUCED POINT MUTATIONS; CELL-WALL DEGRADATION; TAN SPOT; PTR-TOXA; CAUSAL AGENT; COCHLIOBOLUS-CARBONUM AB Pyrenophora tritici-repentis is a necrotrophic fungus causal to the disease tan spot of wheat, whose contribution to crop loss has increased significantly during the last few decades. Pathogenicity by this fungus is attributed to the production of host-selective toxins ( HST), which are recognized by their host in a genotype-specific manner. To better understand the mechanisms that have led to the increase in disease incidence related to this pathogen, we sequenced the genomes of three P. tritici-repentis isolates. A pathogenic isolate that produces two known HSTs was used to assemble a reference nuclear genome of approximately 40 Mb composed of 11 chromosomes that encode 12,141 predicted genes. Comparison of the reference genome with those of a pathogenic isolate that produces a third HST, and a nonpathogenic isolate, showed the nonpathogen genome to be more diverged than those of the two pathogens. Examination of gene-coding regions has provided candidate pathogen-specific proteins and revealed gene families that may play a role in a necrotrophic lifestyle. Analysis of transposable elements suggests that their presence in the genome of pathogenic isolates contributes to the creation of novel genes, effector diversification, possible horizontal gene transfer events, identified copy number variation, and the first example of transduplication by DNA transposable elements in fungi. Overall, comparative analysis of these genomes provides evidence that pathogenicity in this species arose through an influx of transposable elements, which created a genetically flexible landscape that can easily respond to environmental changes. C1 [Manning, Viola A.; Pandelova, Iovanna; Wilhelm, Larry J.; Figueroa, Melania; Holman, Wade H.; Spatafora, Joseph W.; Ciuffetti, Lynda M.] Oregon State Univ, Dept Bot & Plant Pathol, Corvallis, OR 97331 USA. [Dhillon, Braham] Univ British Columbia, Dept Forest Sci, Vancouver, BC V6T 1Z4, Canada. [Wilhelm, Larry J.] Oregon Reg Primate Res Ctr, Div Neurosci, Carbone Ferguson Labs, Beaverton, OR 97006 USA. [Goodwin, Stephen B.] Purdue Univ, USDA ARS, W Lafayette, IN 47907 USA. [Berlin, Aaron M.; Kodira, Chinnappa D.; Yandava, Chandri; Young, Sarah; Zeng, Qiandong; Ma, Li-Jun] Broad Inst, Cambridge, MA 02142 USA. [Figueroa, Melania] Oregon State Univ, USDA ARS, Forage Seed & Cereal Res Unit, Corvallis, OR 97331 USA. [Freitag, Michael] Oregon State Univ, Dept Biochem & Biophys, Corvallis, OR 97331 USA. [Freitag, Michael; Ciuffetti, Lynda M.] Oregon State Univ, Ctr Genome Res & Biocomp, Corvallis, OR 97331 USA. [Hane, James K.] CSIRO, Plant Ind, Ctr Environm & Life Sci, Floreat, WA 6014, Australia. [Henrissat, Bernard] Aix Marseille Univ, CNRS, F-13288 Marseille 9, France. [Kodira, Chinnappa D.] Roche 454, Branford, CT 06405 USA. [Martin, Joel; Schackwitz, Wendy; Grigoriev, Igor V.] US DOE Joint Genome Inst, Walnut Creek, CA 94598 USA. [Oliver, Richard P.] Curtin Univ Technol, Dept Environm & Agr, Australian Ctr Necrotroph Fungal Pathogens, Bentley, WA 6845, Australia. [Robbertse, Barbara] NIH, Natl Ctr Biotechnol Informat, Natl Lib Med, Dept Hlth & Human Serv, Bethesda, MD 20894 USA. [Schwartz, David C.; Zhou, Shiguo] Univ Wisconsin, UW Biotechnol Ctr, Dept Chem, Lab Mol & Computat Genome,Lab Genet, Madison, WI 53706 USA. [Turgeon, B. Gillian] Cornell Univ, Dept Plant Pathol & Plant Microbe Biol, Ithaca, NY 14850 USA. [Ma, Li-Jun] Univ Massachusetts, Dept Biochem & Mol Biol, Amherst, MA 01003 USA. RP Ciuffetti, LM (reprint author), Oregon State Univ, Dept Bot & Plant Pathol, Corvallis, OR 97331 USA. EM lijun@biochem.umass.edu; ciuffetL@science.oregonstate.edu RI Hane, James/A-7062-2011; Henrissat, Bernard/J-2475-2012; OI Hane, James/0000-0002-7651-0977; Ma, Li-Jun/0000-0002-2733-3708; Goodwin, Stephen/0000-0001-5708-9729 FU National Science Foundation under a Minority Postdoctoral Research Fellowship [0706881]; National Research Initiative of the U.S. Department of Agriculture Cooperative State Research, Education and Extension Service [2006-55600-16619]; Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231] FX We thank Cedar Hesse and Jeffrey Kimbrel for helpful discussion about bioinformatics and the Center of Genome Research and Biocomputing, Oregon State University, Corvallis, Oregon, for biocomputing infrastructure. We thank K. Cook, P. Martinez, and S. Ottum for microscopy. We also thank the Colletotrichum genome project (PIs-Lisa Vaillancourt, Michael Thon, and Marty Dickman) for sharing unpublished data. Funding for M. Figueroa was provided by the National Science Foundation under a Minority Postdoctoral Research Fellowship (0706881) awarded in 2007. Sequencing of the reference strain was funded by the National Research Initiative of the U.S. Department of Agriculture Cooperative State Research, Education and Extension Service, grant number (2006-55600-16619), and reviewed through the U.S. Department of Agriculture/National Science Foundation Microbial Genome Sequencing Project. Illumina sequencing work was conducted by the U.S. Department of Energy Joint Genome Institute and supported by the Office of Science of the U.S. Department of Energy (under Contract No. DE-AC02-05CH11231). NR 190 TC 48 Z9 117 U1 3 U2 69 PU GENETICS SOCIETY AMERICA PI BETHESDA PA 9650 ROCKVILLE AVE, BETHESDA, MD 20814 USA SN 2160-1836 J9 G3-GENES GENOM GENET JI G3-Genes Genomes Genet. PD JAN PY 2013 VL 3 IS 1 BP 41 EP 63 DI 10.1534/g3.112.004044 PG 23 WC Genetics & Heredity SC Genetics & Heredity GA 070ZU UT WOS:000313555200006 PM 23316438 ER PT J AU Mayes, M Jagadamma, S Ambaye, H Petridis, L Lauter, V AF Mayes, Melanie Jagadamma, Sindhu Ambaye, Haile Petridis, Loukas Lauter, Valeria TI Neutron reflectometry reveals the internal structure of organic compounds deposited on aluminum oxide SO GEODERMA LA English DT Article DE Organic carbon; Soil mineral; Neutron reflectivity; Reflectometry; Adsorption; Organo-mineral interface ID HUMIC SUBSTANCES; MATTER FRACTIONS; IRON-OXIDE; SOIL; ADSORPTION; REFLECTIVITY; DESORPTION; SURFACES; CARBON; MODEL AB Organic carbon (OC) stabilization in soils plays a significant role in the global C cycle, therefore understanding the structure and function of the OC-soil mineral interface is of high importance. To study the interface, films of simple OC compounds and natural organic matter (NOM) were deposited onto a soil mineral analogue (Al2O3) using spin coating and were exposed to humidity. The thickness, density and structure of the films were studied using a depth-sensitive, nano-scale technique of neutron reflectometry. A single homogenous layer was observed when NOM and glucose (GL) were adsorbed onto Al2O3. However, when stearic acid (SA) was added to either NOM or GL separate layers attributed to SA and either NOM or GL were detected. The formation of distinct, immiscible layers is due to insolubility of SA with NOM and GL In contrast, GL and NOM are both water-soluble, and therefore soluble with each other, forming a homogenous layer on the mineral surface. Our results suggest that the extent of complex layering formed on the OC-mineral interface may depend on the relative solubility of the compounds. (C) 2012 Elsevier B.V. All rights reserved. C1 [Mayes, Melanie; Jagadamma, Sindhu] Oak Ridge Natl Lab, Climate Change Sci Inst, Oak Ridge, TN 37831 USA. [Mayes, Melanie; Jagadamma, Sindhu] Oak Ridge Natl Lab, Div Environm Sci, Oak Ridge, TN 37831 USA. [Ambaye, Haile; Lauter, Valeria] Oak Ridge Natl Lab, Neutron Sci Directorate, Oak Ridge, TN 37831 USA. [Petridis, Loukas] Oak Ridge Natl Lab, Div Biol Sci, Oak Ridge, TN 37831 USA. RP Mayes, M (reprint author), Oak Ridge Natl Lab, Climate Change Sci Inst, POB 2008, Oak Ridge, TN 37831 USA. EM mayesma@ornl.gov RI Ambaye, Haile/D-1503-2016; Petridis, Loukas/B-3457-2009 OI Ambaye, Haile/0000-0002-8122-9952; Petridis, Loukas/0000-0001-8569-060X FU U.S. Government [DE-AC05-00OR22725]; ORNL Laboratory Research and Development Program (LDRD); Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy; U.S. Department of Energy [DE-AC05-00OR22725] FX The submitted manuscript has been authored by a contractor of the U.S. Government under contract DE-AC05-00OR22725. 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.; We thank Ilia Ivanov and Michael Kilbey at the Center for Nanophase Materials Sciences (CNMS) at Oak Ridge National Laboratory (ORNL) for their help with sample preparation, and CNMS for access to facilities via a rapid access proposal. We acknowledge two anonymous reviewers whose suggestions significantly improved the manuscript This project is funded by the ORNL Laboratory Research and Development Program (LDRD). Research at the ORNL Spallation Neutron Source was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy. ORNL is managed by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the U.S. Department of Energy. NR 32 TC 5 Z9 7 U1 1 U2 35 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0016-7061 J9 GEODERMA JI Geoderma PD JAN PY 2013 VL 192 BP 182 EP 188 DI 10.1016/j.geoderma.2012.07.025 PG 7 WC Soil Science SC Agriculture GA 065NJ UT WOS:000313154900020 ER PT J AU Portenga, EW Bierman, PR Rizzo, DM Rood, DH AF Portenga, Eric W. Bierman, Paul R. Rizzo, Donna M. Rood, Dylan H. TI Low rates of bedrock outcrop erosion in the central Appalachian Mountains inferred from in situ Be-10 SO GEOLOGICAL SOCIETY OF AMERICA BULLETIN LA English DT Article ID FISSION-TRACK THERMOCHRONOLOGY; COSMOGENIC NUCLIDES; PASSIVE MARGIN; HALF-LIFE; DENUDATION; BASIN; AL-26; SURFACES; VIRGINIA; HISTORY AB Bedrock outcrops are common on central Appalachian Mountain ridgelines. Because these ridgelines define watersheds, the rate at which they erode influences the pace of landscape evolution. To estimate ridgeline erosion rates, we sampled 72 quartz-bearing outcrops from the Potomac and Susquehanna River Basins and measured in situ produced Be-10. Ridgeline erosion rates average 9 +/- 1 m m.y.(-1) (median = 6 m m.y.(-1)), similar to Be-10-derived rates previously reported for the region. The range of erosion rates we calculated reflects the wide distribution of samples we collected and the likely inclusion of outcrops affected by episodic loss of thick slabs and periglacial activity. Outcrops on main ridgelines erode slower than those on mountainside spur ridges because ridgelines are less likely to be covered by soil, which reduces the production rate of Be-10 and increases the erosion rate of rock. Ridgeline outcrops erode slower than drainage basins in the Susquehanna and Potomac River watersheds, suggesting a landscape in disequilibrium. Erosion rates are more similar for outcrops meters to tens of meters apart than those at greater distances, yet semivariogram analysis suggests that outcrop erosion rates in the same physiographic province are similar even though they are hundreds of kilometers apart. This similarity may reflect underlying lithological and/or structural properties common to each physiographic province. Average Be-10-derived outcrop erosion rates are similar to denudation rates determined by other means (sediment flux, fission-track thermochronology, [U-Th]/He dating), indicating that the pace of landscape evolution in the central Appalachian Mountains is slow, and has been since post-Triassic rifting events. C1 [Portenga, Eric W.; Bierman, Paul R.] Univ Vermont, Dept Geol, Burlington, VT 05405 USA. [Bierman, Paul R.] Univ Vermont, Rubenstein Sch Environm & Nat Resources, Burlington, VT 05405 USA. [Rizzo, Donna M.] Univ Vermont, Coll Engn & Math Sci, Burlington, VT 05405 USA. [Rood, Dylan H.] Lawrence Livermore Natl Lab, Ctr Accelerator Mass Spectrometry, Livermore, CA 94550 USA. [Rood, Dylan H.] Univ Calif Santa Barbara, Earth Res Inst, Santa Barbara, CA 93106 USA. RP Portenga, EW (reprint author), Univ Glasgow, Sch Geog & Earth Sci, Glasgow G12 8QQ, Lanark, Scotland. EM eporteng@uvm.edu FU National Science Foundation [EAR-310208]; U.S. Geological Survey [08ERSA0582]; U.S. Department of Energy at Lawrence Livermore National Laboratory [DE-AC52-07NA27344] FX We thank R. Harriett (Harpers Ferry National Historical Park), B. Loncoski (Catoctin Mountain Park), B. Norden (Maryland Department of Natural Resources), T. Collins (George Washington National Forest), L. Tracey (Monongahela National Forest), S. Summers (West Virginia Division of Natural Resources), and G. Blackmer (Pennsylvania Department of Conservation and Natural Resources) for assistance in obtaining permits and C. Trodick Jr. for his help in collecting samples. We also thank Gregory Hancock and James Spotila for their thoughtful and constructive comments and guidance throughout the review process. This work was supported by National Science Foundation grant EAR-310208 and U.S. Geological Survey grant 08ERSA0582 and was performed in part under the auspices of the U.S. Department of Energy at Lawrence Livermore National Laboratory under contract DE-AC52-07NA27344. NR 62 TC 11 Z9 11 U1 3 U2 30 PU GEOLOGICAL SOC AMER, INC PI BOULDER PA PO BOX 9140, BOULDER, CO 80301-9140 USA SN 0016-7606 J9 GEOL SOC AM BULL JI Geol. Soc. Am. Bull. PD JAN-FEB PY 2013 VL 125 IS 1-2 BP 201 EP 215 DI 10.1130/B30559.1 PG 13 WC Geosciences, Multidisciplinary SC Geology GA 065FL UT WOS:000313133800012 ER PT J AU Gall, B Kovaleski, SD VanGordon, JA Norgard, P Benwell, A Kim, BH Kwon, JW Dale, GE AF Gall, Brady Kovaleski, Scott D. VanGordon, James A. Norgard, Peter Benwell, Andrew Kim, Baek Hyun Kwon, Jae Wan Dale, Gregory E. TI Investigation of the Piezoelectric Effect as a Means to Generate X-Rays SO IEEE TRANSACTIONS ON PLASMA SCIENCE LA English DT Article DE Electron emission; piezoelectric effect; X-ray production ID TRANSFORMER AB The piezoelectric effect is analyzed as a means to produce X-rays. A mass of crystalline piezoelectric material is used to convert a low-voltage input electrical signal into a high-voltage output signal by storing energy in a longitudinally vibrating mechanical wave. Output energy is extracted in the form of a high-voltage electron beam using a field-emission diode mounted on the surface of the crystal. The electron beam produces X-rays via bremsstrahlung interactions with a metallic surface. C1 [Gall, Brady; Kovaleski, Scott D.; VanGordon, James A.; Norgard, Peter; Kim, Baek Hyun; Kwon, Jae Wan] Univ Missouri, Dept Elect & Comp Engn, Columbia, MO 65211 USA. [Benwell, Andrew] SLAC Natl Accelerator Lab, Electrodynam Dept, RFARED, Menlo Pk, CA 94025 USA. [Dale, Gregory E.] Los Alamos Natl Lab, Accelerator & Operat Technol Div, High Power Electrodynam Grp, Los Alamos, NM 87541 USA. RP Gall, B (reprint author), Univ Missouri, Dept Elect & Comp Engn, Columbia, MO 65211 USA. EM kovaleskis@missouri.edu; abenwell@slac.stanford.edu; gedale@lanl.gov OI Norgard, Peter/0000-0002-5332-5998; Kovaleski, Scott/0000-0002-5831-6388 FU Los Alamos National Laboratory; Qynergy Corporation; Office of Naval Research FX This work was supported in part by Los Alamos National Laboratory, by Qynergy Corporation, and by the Office of Naval Research. NR 27 TC 7 Z9 7 U1 0 U2 8 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 0093-3813 J9 IEEE T PLASMA SCI JI IEEE Trans. Plasma Sci. PD JAN PY 2013 VL 41 IS 1 BP 106 EP 111 DI 10.1109/TPS.2012.2227250 PG 6 WC Physics, Fluids & Plasmas SC Physics GA 069HL UT WOS:000313425800015 ER PT J AU Coen, JL Cameron, M Michalakes, J Patton, EG Riggan, PJ Yedinak, KM AF Coen, Janice L. Cameron, Marques Michalakes, John Patton, Edward G. Riggan, Philip J. Yedinak, Kara M. TI WRF-Fire: Coupled Weather-Wildland Fire Modeling with the Weather Research and Forecasting Model SO JOURNAL OF APPLIED METEOROLOGY AND CLIMATOLOGY LA English DT Article ID DISCRETE FUEL-ELEMENTS; WIND-AIDED FIRESPREAD; GRASS FIRES; SPREAD; DYNAMICS; BEHAVIOR; SIMULATIONS; FRONTS; GROWTH; ARRAYS AB A wildland fire-behavior module, named WRF-Fire, was integrated into the Weather Research and Forecasting (WRF) public domain numerical weather prediction model. The fire module is a surface fire-behavior model that is two-way coupled with the atmospheric model. Near-surface winds from the atmospheric model are interpolated to a finer fire grid and are used, with fuel properties and local terrain gradients, to determine the fire's spread rate and direction. Fuel consumption releases sensible and latent heat fluxes into the atmospheric model's lowest layers, driving boundary layer circulations. The atmospheric model, configured in turbulence-resolving large-eddy-simulation mode, was used to explore the sensitivity of simulated fire characteristics such as perimeter shape, fire intensity, and spread rate to external factors known to influence fires, such as fuel characteristics and wind speed, and to explain how these external parameters affect the overall fire properties. Through the use of theoretical environmental vertical profiles, a suite of experiments using conditions typical of the daytime convective boundary layer was conducted in which these external parameters were varied around a control experiment. Results showed that simulated fires evolved into the expected bowed shape because of fire-atmosphere feedbacks that control airflow in and near fires. The coupled model reproduced expected differences in fire shapes and heading-region fire intensity among grass, shrub, and forest-litter fuel types; reproduced the expected narrow, rapid spread in higher wind speeds; and reproduced the moderate inhibition of fire spread in higher fuel moistures. The effects of fuel load were more complex: higher fuel loads increased the heat flux and fire-plume strength and thus the inferred fire effects but had limited impact on spread rate. C1 [Coen, Janice L.; Patton, Edward G.] Natl Ctr Atmospher Res, Boulder, CO 80301 USA. [Cameron, Marques] Natl Ctr Atmospher Res, Woodbridge, VA USA. [Michalakes, John] Natl Renewable Energy Lab, Golden, CO USA. [Riggan, Philip J.] US Forest Serv, USDA, Pacific SW Res Stn, Riverside, CA USA. [Yedinak, Kara M.] Washington State Univ, Dept Civil & Environm Engn, Pullman, WA 99164 USA. RP Coen, JL (reprint author), Natl Ctr Atmospher Res, POB 3000, Boulder, CO 80301 USA. EM janicec@ucar.edu RI Patton, Edward/K-3607-2012; OI Patton, Edward/0000-0001-5431-9541 FU National Science Foundation [0324910, 0421498, 0835598]; University Corporation for Atmospheric Research's Significant Opportunities in Atmospheric Research and Science (SOARS) program FX The National Center for Atmospheric Research is sponsored by the National Science Foundation.; This material is based upon work supported by the National Science Foundation under Awards 0324910, 0421498, and 0835598. The National Center for Atmospheric Research (NCAR) is sponsored by the National Science Foundation. Any opinions, 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. Marques Cameron was supported by the University Corporation for Atmospheric Research's Significant Opportunities in Atmospheric Research and Science (SOARS) program. WRF, including the WRF-Fire physics module, is available as public domain software at http://www.wrf-model.org. Contributions to WRF-Fire came from numerous individuals at NCAR, the U. S. Department of Agriculture Forest Service, the Australian Bureau of Meteorology, and the University of Colorado at Denver. We thank Peter Sullivan for helpful discussions during this work. We thank Alan Norton of NCAR's Computational & Information Systems Laboratory (CISL) for help with visualizations using VAPOR. NR 61 TC 27 Z9 27 U1 2 U2 42 PU AMER METEOROLOGICAL SOC PI BOSTON PA 45 BEACON ST, BOSTON, MA 02108-3693 USA SN 1558-8424 J9 J APPL METEOROL CLIM JI J. Appl. Meteorol. Climatol. PD JAN PY 2013 VL 52 IS 1 BP 16 EP 38 DI 10.1175/JAMC-D-12-023.1 PG 23 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA 071BH UT WOS:000313559900003 ER PT J AU Liu, MKP Hawkins, N Ritchie, AJ Ganusov, VV Whale, V Brackenridge, S Li, H Pavlicek, JW Cai, FP Rose-Abrahams, M Treurnicht, F Hraber, P Riou, C Gray, C Ferrari, G Tanner, R Ping, LH Anderson, JA Swanstrom, R Chavi, CB Cohen, M Karim, SSA Haynes, B Borrow, P Perelson, AS Shaw, GM Hahn, BH Williamson, C Korber, BT Gao, F Self, S McMichael, A Goonetilleke, N AF Liu, Michael K. P. Hawkins, Natalie Ritchie, Adam J. Ganusov, Vitaly V. Whale, Victoria Brackenridge, Simon Li, Hui Pavlicek, Jeffrey W. Cai, Fangping Rose-Abrahams, Melissa Treurnicht, Florette Hraber, Peter Riou, Catherine Gray, Clive Ferrari, Guido Tanner, Rachel Ping, Li-Hua Anderson, Jeffrey A. Swanstrom, Ronald Chavi, Core B. Cohen, Myron Karim, Salim S. Abdool Haynes, Barton Borrow, Persephone Perelson, Alan S. Shaw, George M. Hahn, Beatrice H. Williamson, Carolyn Korber, Bette T. Gao, Feng Self, Steve McMichael, Andrew Goonetilleke, Nilu TI Vertical T cell immunodominance and epitope entropy determine HIV-1 escape SO JOURNAL OF CLINICAL INVESTIGATION LA English DT Article ID HUMAN-IMMUNODEFICIENCY-VIRUS; HLA CLASS-I; PRIMARY INFECTION; CTL ESCAPE; VIRAL LOAD; LYMPHOCYTE RESPONSE; MAJOR DETERMINANTS; TYPE-1 INFECTION; AUTOLOGOUS VIRUS; IMMUNE CONTROL AB HIV-1 accumulates mutations in and around reactive epitopes to escape recognition and killing by CD8(+) T cells. Measurements of HIV-1 time to escape should therefore provide information on which parameters are most important for T cell-mediated in vivo control of HIV-1. Primary HIV-1 specific T cell responses were fully mapped in 17 individuals, and the time to virus escape, which ranged from days to years, was measured for each epitope. While higher magnitude of an individual T cell response was associated with more rapid escape, the most significant T cell measure was its relative immunodominance measured in acute infection. This identified subject-level or "vertical" immunodominance as the primary determinant of in vivo CD8(+) T cell pressure in HIV-1 infection. Conversely, escape was slowed significantly by lower population variability, or entropy, of the epitope targeted. Immunodominance and epitope entropy combined to explain half of all the variability in time to escape. These data explain how CD8(+) T cells can exert significant and sustained HIV-1 pressure even when escape is very slow and that within an individual, the impacts of other T cell factors on HIV-1 escape should be considered in the context of immunodominance. C1 [Liu, Michael K. P.; Ritchie, Adam J.; Whale, Victoria; Brackenridge, Simon; Tanner, Rachel; McMichael, Andrew; Goonetilleke, Nilu] Univ Oxford, Weatherall Inst Mol Med, Oxford OX3 9DS, England. [Hawkins, Natalie; Self, Steve] Univ Washington, Stat Ctr HIV AIDS Res & Prevent SCHARP, Seattle, WA 98195 USA. [Ganusov, Vitaly V.] Univ Tennessee, Dept Microbiol, Knoxville, TN 37996 USA. [Li, Hui; Shaw, George M.; Hahn, Beatrice H.] Univ Penn, Perelman Sch Med, Philadelphia, PA 19104 USA. [Pavlicek, Jeffrey W.; Cai, Fangping; Ferrari, Guido; Haynes, Barton; Gao, Feng] Duke Univ, Duke Univ Med Res, Durham, NC USA. [Rose-Abrahams, Melissa; Treurnicht, Florette; Williamson, Carolyn] Univ Cape Town, Fac Hlth Sci, Div Med Virol, ZA-7925 Cape Town, South Africa. [Hraber, Peter; Perelson, Alan S.; Korber, Bette T.] Los Alamos Natl Lab, Div Theoret, Los Alamos, NM USA. [Riou, Catherine; Gray, Clive] Univ Cape Town, Fac Hlth Sci, Inst Infect Dis & Mol Med, ZA-7925 Cape Town, South Africa. [Ping, Li-Hua; Anderson, Jeffrey A.; Swanstrom, Ronald] Univ N Carolina, UNC Ctr AIDS Res, Chapel Hill, NC USA. [Ping, Li-Hua; Anderson, Jeffrey A.; Swanstrom, Ronald] Univ N Carolina, Lineberger Comprehens Canc Ctr, Chapel Hill, NC 27599 USA. [Anderson, Jeffrey A.] Univ N Carolina, Sch Med, Div Infect Dis, Chapel Hill, NC USA. [Swanstrom, Ronald] Univ N Carolina, Dept Biochem & Biophys, Chapel Hill, NC USA. [Cohen, Myron] Univ N Carolina, HIV Prevent Trials Unit, Chapel Hill, NC USA. [Karim, Salim S. Abdool] Univ KwaZulu Natal, Ctr AIDS Programme Res S Africa, Durban, South Africa. [Borrow, Persephone] Univ Oxford, Div Expt Med, Nuffield Dept Clin Med, Oxford OX3 9DS, England. [Perelson, Alan S.; Korber, Bette T.] Santa Fe Inst, Santa Fe, NM 87501 USA. RP Goonetilleke, N (reprint author), Univ Oxford, John Radcliffe Hosp, Weatherall Inst Mol Med, Headley Way, Oxford OX3 9DS, England. EM nilu.goonetilleke@ndm.ox.ac.uk RI Abdool Karim, Salim Safurdeen/N-5947-2013; Ferrari, Guido/A-6088-2015; OI Abdool Karim, Salim Safurdeen/0000-0002-4986-2133; , Carolyn/0000-0003-0125-1226; Ganusov, Vitaly/0000-0001-6572-1691; Korber, Bette/0000-0002-2026-5757; Hraber, Peter/0000-0002-2920-4897 FU Center for HIV/AIDS Vaccine Immunology [AI067854]; Medical Research Council Human Immunology Unit, the NIH Research Oxford Biomedical Research Centre FX We thank CHAVI and Duke management, particularly Kelly Soderberg, Jennifer Kirchnerr, and Marybeth McCauley for study coordination; A. Williams, C. Margaret, C. deBoer, S.C. Heeti, and R. Thomas of SCHARP for database support; J. Roberts for administrative support; T. Rostron for HLA typing; and K. diGleria and Z. Yu for peptide synthesis. This work was supported by the Center for HIV/AIDS Vaccine Immunology grant AI067854. Additional support came from the Medical Research Council Human Immunology Unit, the NIH Research Oxford Biomedical Research Centre. P. Borrow and A.J. McMichael are Jenner Institute Investigators. NR 75 TC 72 Z9 72 U1 0 U2 20 PU AMER SOC CLINICAL INVESTIGATION INC PI ANN ARBOR PA 35 RESEARCH DR, STE 300, ANN ARBOR, MI 48103 USA SN 0021-9738 EI 1558-8238 J9 J CLIN INVEST JI J. Clin. Invest. PD JAN PY 2013 VL 123 IS 1 BP 380 EP 393 DI 10.1172/JCI65330 PG 14 WC Medicine, Research & Experimental SC Research & Experimental Medicine GA 071MV UT WOS:000313598500041 PM 23221345 ER PT J AU Kreuzer, HW West, JB Ehleringer, JR AF Kreuzer, Helen W. West, Jason B. Ehleringer, James R. TI Forensic Applications of Light-Element Stable Isotope Ratios of Ricinus communis Seeds and Ricin Preparations SO JOURNAL OF FORENSIC SCIENCES LA English DT Article DE forensic science; ricin; castor; Ricinus communis; stable isotope; sample matching; forensic signature ID MASS-SPECTROMETRY; CARBON; OXYGEN; STRONTIUM; CELLULOSE; WATER; DISCRIMINATION; FRACTIONATION; INFORMATION; METABOLITES AB Seeds of the castor plant Ricinus communis are of forensic interest because they are the source of the poison ricin. We tested whether stable isotope ratios of castor seeds and ricin preparations can be used as a forensic signature. We collected over 300 castor seed samples worldwide and measured the C, N, O, and H isotope ratios of the whole seeds and oil. We prepared ricin by three different procedures, acetone extraction, salt precipitation, and affinity chromatography, and compared their isotope ratios to those of the source seeds. The N isotope ratios of the ricin samples and source seeds were virtually identical. Therefore, N isotope ratios can be used to correlate ricin prepared by any of these methods to source seeds. Further, stable isotope ratios distinguished >99% of crude and purified ricin protein samples in pairwise comparison tests. Stable isotope ratios therefore constitute a valuable forensic signature for ricin preparations. C1 [Kreuzer, Helen W.; West, Jason B.; Ehleringer, James R.] Univ Utah, Dept Biol, Salt Lake City, UT 84112 USA. RP Kreuzer, HW (reprint author), Pacific NW Natl Lab, 999 Battelle Blvd,MSIN P7-50, Richland, WA 99352 USA. EM Helen.Kreuzer@pnnl.gov FU Federal Bureau of Investigation [BAA-0034104]; Laboratory Directed Research and Development Program at Pacific Northwest National Laboratory; U.S. Department of Energy [DE-AC05-76RL01830]; National Science Foundation [0743543] FX This work was funded by the Federal Bureau of Investigation, BAA Solicitation Number: BAA-0034104, Interest Area 103. H. W. K. also received support from the Laboratory Directed Research and Development Program at Pacific Northwest National Laboratory, a multiprogram laboratory operated by Battelle for the U.S. Department of Energy under Contract DE-AC05-76RL01830. Funding from the National Science Foundation (Grant no. 0743543) to J.B.W. provided partial support for this work. NR 54 TC 3 Z9 3 U1 1 U2 27 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0022-1198 J9 J FORENSIC SCI JI J. Forensic Sci. PD JAN PY 2013 VL 58 SU 1 SI SI BP S43 EP S51 DI 10.1111/1556-4029.12000 PG 9 WC Medicine, Legal SC Legal Medicine GA 070YK UT WOS:000313550400007 PM 23130759 ER PT J AU Hehlen, MP Greco, RR Rellergert, WG Sullivan, ST DeMille, D Jackson, RA Hudson, ER Torgerson, JR AF Hehlen, Markus P. Greco, Richard R. Rellergert, Wade G. Sullivan, Scott T. DeMille, David Jackson, Robert A. Hudson, Eric R. Torgerson, Justin R. TI Optical spectroscopy of an atomic nucleus: Progress toward direct observation of the Th-229 isomer transition SO JOURNAL OF LUMINESCENCE LA English DT Article; Proceedings Paper CT 16th International conference on luminescence and optical spectroscopy of condensed matter CY JUN 27-JUL 01, 2011 CL Ann Arbor, MI DE Vacuum ultraviolet luminescence spectroscopy; Nuclear isomer; Nuclear clock; Thorium isomer transition; Fluoride crystal ID FLUORIDE; CRYSTALS; DECAY; ASTRO-E2; LICAALF6; EMISSION; LISRALF6; STATE AB The nucleus of the thorium-229 isotope possesses a first excited nuclear state (Th-229m) at an exceptionally low energy of 7.8 +/- 0.5 eV above the nuclear ground state (Th-229g), as determined by earlier indirect measurements. This is the only nuclear excited state known that is within the range of optical spectroscopy. This paper reports progress toward detecting the Th-229m state directly by luminescence spectroscopy in the vacuum ultraviolet spectral region. The estimated natural linewidth of the Th-229g <-> Th-229m isomer transition of 2 pi x 0.1 to 2 pi x 10 mHz is expected to broaden to similar to 10 kHz for Th-229(4+) doped into a suitable crystal. The factors governing the choice of crystal system and the substantial challenges in acquiring a sufficiently large quantity of Th-229 are discussed. We show that the Th-229g <-> Th-229m transition energy can be identified to within 0.1 nm by luminescence excitation and luminescence spectroscopy using the Advanced Light Source (ALS) at Lawrence Berkeley National Laboratory. This would open the door for subsequent laser-based measurements of the isomer transition and future applications of Th-229 in nuclear clocks. We also show that U-233-doped materials should produce an intrinsic, continuous, and sufficiently high rate of Th-229m -> Th-229g luminescence and could be a useful aid in the initial direct search of the isomer transition. Published by Elsevier B.V. C1 [Hehlen, Markus P.; Greco, Richard R.; Torgerson, Justin R.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Rellergert, Wade G.; Sullivan, Scott T.; Hudson, Eric R.] Univ Calif Los Angeles, Dept Phys & Astron, Los Angeles, CA 90095 USA. [DeMille, David] Yale Univ, Dept Phys, New Haven, CT 06511 USA. [Jackson, Robert A.] Keele Univ, Sch Phys & Geog Sci, Keele ST5 5BG, Staffs, England. RP Hehlen, MP (reprint author), Los Alamos Natl Lab, Mailstop E549, Los Alamos, NM 87545 USA. EM hehlen@lanl.gov FU US DOE [DE-AC0205CH11231]; UCLRP [09-LR-04-120497-HUDE]; Los Alamos National Laboratory LDRD program; DARPA; ARO [W911NF-11-1-0369] FX The ALS is supported by the US DOE under Contract no. DE-AC0205CH11231. This work was supported by UCLRP Grant no. 09-LR-04-120497-HUDE and the Los Alamos National Laboratory LDRD program. UCLA also acknowledges support from DARPA and the ARO under grant no. W911NF-11-1-0369. UCLA also acknowledges support from DARPA and the ARO under grant no. W911NF-11-1-0369. NR 33 TC 19 Z9 19 U1 0 U2 30 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0022-2313 EI 1872-7883 J9 J LUMIN JI J. Lumines. PD JAN PY 2013 VL 133 BP 91 EP 95 DI 10.1016/j.jlumin.2011.09.037 PG 5 WC Optics SC Optics GA 070AK UT WOS:000313478000020 ER PT J AU Yukihara, EG Milliken, ED Oliveira, LC Orante-Barron, VR Jacobsohn, LG Blair, MW AF Yukihara, E. G. Milliken, E. D. Oliveira, L. C. Orante-Barron, V. R. Jacobsohn, L. G. Blair, M. W. TI Systematic development of new thermoluminescence and optically stimulated luminescence materials SO JOURNAL OF LUMINESCENCE LA English DT Article; Proceedings Paper CT 16th International conference on luminescence and optical spectroscopy of condensed matter CY JUN 27-JUL 01, 2011 CL Ann Arbor, MI DE Thermoluminescence; Optically Stimulated Luminescence; Solution Combustion Synthesis; Radioluminescence ID OSL NEUTRON DOSIMETERS; COMBUSTION SYNTHESIS; COMPUTED-TOMOGRAPHY; DETECTORS; PHOTOLUMINESCENCE; OXYORTHOSILICATE; NANOPHOSPHORS; NANOCRYSTALS; PROFILES; OXIDES AB This paper presents an overview of a systematic study to develop new thermoluminescence (TL) and optically stimulated luminescence (OSL) materials using solution combustion synthesis (SCS) for applications such as personal OSL dosimetry, 2D dose mapping, and temperature sensing. A discussion on the material requirements for these applications is included. We present X-ray diffraction (XRD) data on single phase materials obtained with SCS, as well as radioluminescence (RL), TL and OSL data of lanthanide-doped materials. The results demonstrate the possibility of producing TL and OSL materials with sensitivity similar to or approaching those of commercial TL and OSL materials used in dosimetry (e.g., LiF:Mg,Ti and Al2O3:C) using SCS. The results also show that the luminescence properties can be improved by Li co-doping and annealing. The presence of an atypical TL background and anomalous fading are discussed and deserve attention in future investigations. We hope that these preliminary results on the use of SCS for production of TL and OSL materials are helpful to guide future efforts towards the development of new luminescence materials for different applications. (c) 2011 Elsevier B.V. All rights reserved. C1 [Yukihara, E. G.; Milliken, E. D.; Oliveira, L. C.] Oklahoma State Univ, Dept Phys, Stillwater, OK 74078 USA. [Orante-Barron, V. R.] Univ Sonora, Dept Invest Polimeros & Mat, Hermosillo 83000, Sonora, Mexico. [Jacobsohn, L. G.] Clemson Univ, COMSET, Clemson, SC USA. [Jacobsohn, L. G.] Clemson Univ, Sch Mat Sci & Engn, Clemson, SC USA. [Blair, M. W.] Los Alamos Natl Lab, Mat Sci & Technol Div, Los Alamos, NM 87545 USA. RP Yukihara, EG (reprint author), Oklahoma State Univ, Dept Phys, Stillwater, OK 74078 USA. EM eduardo.yukihara@okstate.edu RI Yukihara, Eduardo/F-1345-2014; OI Yukihara, Eduardo/0000-0002-4615-6698; Jacobsohn, Luiz/0000-0001-8991-3903 FU Oklahoma Center for the Advancement of Science and Technology (OCAST) through OHRS [HR09-104]; US Defense Threat Reduction Agency (DTRA) [HDTRA1-10-1-0007] FX The authors thank Jim Puckette (Boone Pickens School of Geology, Oklahoma State University, Stillwater, OK) for the use of the Phillips Analytical X-ray diffractometer, and Gregoire Denis for discussions and suggestions. This work was supported by the Oklahoma Center for the Advancement of Science and Technology (OCAST) through OHRS award project number HR09-104, and by the US Defense Threat Reduction Agency (DTRA) through contract HDTRA1-10-1-0007. NR 47 TC 29 Z9 30 U1 8 U2 72 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0022-2313 EI 1872-7883 J9 J LUMIN JI J. Lumines. PD JAN PY 2013 VL 133 BP 203 EP 210 DI 10.1016/j.jlumin.2011.12.018 PG 8 WC Optics SC Optics GA 070AK UT WOS:000313478000043 ER PT J AU Cook, JB Kim, C Xu, LP Cabana, J AF Cook, John B. Kim, Chunjoong Xu, Linping Cabana, Jordi TI The Effect of Al Substitution on the Chemical and Electrochemical Phase Stability of Orthorhombic LiMnO2 SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID RECHARGEABLE LITHIUM BATTERIES; MANGANESE OXIDE CATHODES; LI-ION BATTERIES; LAYERED LIMNO2; INTERCALATION COMPOUNDS; HYDROTHERMAL SYNTHESIS; NEUTRON-DIFFRACTION; STACKING-FAULTS; SPINEL; TEMPERATURE AB LiMnO2 is of interest as positive electrode material in Li-ion batteries because of its high theoretical specific capacity, low material cost and toxicity. However, this material suffers from a cycling-induced transformation from a layered crystal structure to a spinel-like that induces a reduction in specific capacity during the first few cycles. Computational predictions suggested this drawback could be overcome by aluminum substitution for manganese. Using a hydrothermal synthesis method, extensive aluminum substitution in o-LiMnO2 was achieved. Even at such high levels, preservation of the orthorhombic over the monoclinic polytype was found. This strategy was unsuccessful in preventing the structural evolution of the layered to a spinel phase during electrochemical cycling, as evidenced by in situ synchrotron X-ray diffraction for a material with 25% aluminum. This sample showed the best cycling performance with a first charge capacity and coulombic efficiency of 160 mAh/g and similar to 100%, respectively. The structural transformation during cycling was correlated with a rapid decay of specific capacity over ten cycles, for a retention of 67%. (C) 2012 The Electrochemical Society. [DOI: 10.1149/2.048301jes] All rights reserved. C1 [Cook, John B.; Kim, Chunjoong; Xu, Linping; Cabana, Jordi] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. [Cook, John B.] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. RP Cook, JB (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. EM jcabana@lbl.gov RI Cabana, Jordi/G-6548-2012; Cook, John/J-3730-2016 OI Cabana, Jordi/0000-0002-2353-5986; Cook, John/0000-0002-2886-3276 FU Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the U.S. Department of Energy [DE-AC02-05CH11231]; LBNL through Community College Internship program from Department of Energy FX This work was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the U. S. Department of Energy under Contract No. DE-AC02-05CH11231, as part of the Batteries for Advanced Transportation Technologies (BATT) Program. Portions of this research were carried out at the Stanford Synchrotron Radiation Lightsource, a Directorate of SLAC National Accelerator Laboratory and an Office of Science User Facility operated for the U.S. Department of Energy Office of Science by Stanford University. JBC was partially supported by LBNL through the Community College Internship program from the Department of Energy. The authors thank Dr. Kristin A. Persson, Michael Kocher and Marca M. Doeff (LBNL, USA), as well as Kerry Wang (Rice University, USA) for useful discussions. Dr. Doeff is also acknowledged for providing access to laboratory facilities. NR 58 TC 8 Z9 9 U1 6 U2 100 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2013 VL 160 IS 1 BP A46 EP A52 DI 10.1149/2.048301jes PG 7 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA 071GM UT WOS:000313578400007 ER PT J AU Dubarry, M Truchot, C Liaw, BY Gering, K Sazhin, S Jamison, D Michelbacher, C AF Dubarry, Matthieu Truchot, Cyril Liaw, Bor Yann Gering, Kevin Sazhin, Sergiy Jamison, David Michelbacher, Christopher TI Evaluation of Commercial Lithium-Ion Cells Based on Composite Positive Electrode for Plug-In Hybrid Electric Vehicle Applications III. Effect of Thermal Excursions without Prolonged Thermal Aging SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID LOW-TEMPERATURE PERFORMANCE; ELEVATED-TEMPERATURES; NONAQUEOUS SOLVENTS; GRAPHITE ELECTRODE; CHARGED CATHODES; LIMITING FACTORS; BATTERIES; POWER; DEGRADATION; IMPEDANCE AB Understanding the behavior of lithium-ion batteries exposed to thermal excursion is of great interest to plug-in hybrid electric vehicle (PHEV) applications, because vehicles often endure wide weather conditions in operation. Here we investigate a composite {LixMn(2)O(4) + LixNi(1/3)Mn(1/3)Co(1/3)O(2)}-based commercial cell design to assess performance and degradation under thermal excursion from 25 degrees C; through -20 degrees C, -5 degrees C, 10 degrees C, 25 degrees C, 40 degrees C, and 60 degrees C; to 25 degrees C. In each isothermal regime, a reference performance test with charge and discharge cycles at C/25, C/5, C/2, 1C, and 2C is conducted to quantify cell capacity, rate capability, and other performance variations. The capacity fade caused by the thermal excursion is attributed to origins including loss of active material, degradation in reaction kinetics, and the ohmic resistance increases. Using electrochemical inference techniques, we found that thermal excursion in the range of -5 degrees C to 40 degrees C is benign to capacity fade. Exposure to -20 degrees C and 60 degrees C respectively leads to irreversible fade. The capacity fade at -20 degrees C induced Li inventory loss and did not cause kinetic degradation, whereas the exposure at 60 degrees C resulted in degradation in reaction kinetics. The evaluation protocols and results are helpful in assisting the study of path dependence of cell degradation in thermal aging. (C) 2012 The Electrochemical Society. [DOI:10.1149/2.063301jes] All rights reserved. C1 [Dubarry, Matthieu; Truchot, Cyril; Liaw, Bor Yann] Univ Hawaii Manoa, Hawaii Nat Energy Inst, SOEST, Honolulu, HI 96822 USA. [Gering, Kevin; Sazhin, Sergiy; Jamison, David; Michelbacher, Christopher] Idaho Natl Lab, Idaho Falls, ID 83415 USA. RP Dubarry, M (reprint author), Univ Hawaii Manoa, Hawaii Nat Energy Inst, SOEST, Honolulu, HI 96822 USA. EM bliaw@hawaii.edu RI Dubarry, Matthieu/B-4333-2012 OI Dubarry, Matthieu/0000-0002-3228-1834 FU U.S. Department of Energy, the Energy Efficiency and Renewable Energy Office (EERE) [DE-AC07-05ID14517] FX The authors thank the funding support from the U.S. Department of Energy, the Energy Efficiency and Renewable Energy Office (EERE), under the Advanced Battery Research (ABR) program (Contract No. DE-AC07-05ID14517). NR 38 TC 16 Z9 20 U1 5 U2 79 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2013 VL 160 IS 1 BP A191 EP A199 DI 10.1149/2.063301jes PG 9 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA 071GM UT WOS:000313578400027 ER PT J AU Kim, D Sandi, G Croy, JR Gallagher, KG Kang, SH Lee, E Slater, MD Johnson, CS Thackeray, MM AF Kim, Donghan Sandi, Giselle Croy, Jason R. Gallagher, Kevin G. Kang, Sun-Ho Lee, Eungje Slater, Michael D. Johnson, Christopher S. Thackeray, Michael M. TI Composite 'Layered-Layered-Spinel' Cathode Structures for Lithium-Ion Batteries SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID MANGANESE OXIDE ELECTRODES; LI-ION; HIGH-CAPACITY; NEUTRON-DIFFRACTION; LICOO2 CATHODE; CO ELECTRODES; NI; MN; LIMNO2; MG AB The concept of embedding a spinel component in high capacity, composite xLi(2)MnO(3)center dot(1-x)LiMO2 (M = Mn, Ni) 'layered-layered' structures to improve their electrochemical properties and cycling stability has been exploited. In this paper, we report the preparation and electrochemical characterization of three-component 'layered-layered-spinel' electrodes, synthesized by lowering the lithium content of a parent 'layered-layered' 0.3Li(2)MnO(3)center dot 0.7LiMn(0.5)Ni(0.5)O(2) material while maintaining a Mn: Ni ratio of 0.65:0.35; such compounds can be designated generically by the system, LixMn(0.65)Ni(0.35)O(y), for which the end members are 0.3Li(2)MnO(3)center dot 0.7LiMn(0.5)Ni(0.5)O(2) (x = 1.3; y = 2.3), in which the average manganese and nickel oxidation states are 4+ and 2+, respectively, and LiMn1.3Ni0.7O4 (x = 0.5; y = 2) in which the corresponding average oxidation states are expected to lie between 4+ and 3.77+ for Mn, and 2.57+ and 3+ for Ni, respectively. For this study, compounds with a lithium content of x = 1.3, i.e., the parent 'layered-layered' composition, and 1.25 were selected for detailed and comparative investigation, the latter value corresponding to a targeted spinel content of 6%. The beneficial effects of 1) using Mg2+ as a dopant ion and 2) treating the electrode particle surface with an acidic solution of AlF3 to enhance cycling stability, reduce first-cycle capacity loss, and to slow voltage decay on cycling are discussed. (C) 2012 The Electrochemical Society. [DOI: 10.1149/2.049301jes] All rights reserved. C1 [Kim, Donghan; Sandi, Giselle; Croy, Jason R.; Gallagher, Kevin G.; Kang, Sun-Ho; Lee, Eungje; Slater, Michael D.; Johnson, Christopher S.; Thackeray, Michael M.] Argonne Natl Lab, Electrochem Energy Storage Dept, Chem Sci & Engn Div, Argonne, IL 60439 USA. RP Kim, D (reprint author), Argonne Natl Lab, Electrochem Energy Storage Dept, Chem Sci & Engn Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM thackeray@anl.gov RI Slater, Michael/D-5388-2012 FU Office of Vehicle Technologies, Office of Energy Efficiency and Renewable Energy of the U.S. Department of Energy; Argonne, a U.S. Department of Energy Office of Science laboratory [DE-AC02-06CH11357] FX This work was supported by the Office of Vehicle Technologies, Office of Energy Efficiency and Renewable Energy of the U.S. Department of Energy. Bonil Koo and Soongu Kwon (Center of Nanoscale Materials (CNM), Argonne National Laboratory) are thanked for collecting the TEM/SEM image data. Facilities at CNM are supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences.; 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 39 TC 57 Z9 57 U1 13 U2 267 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2013 VL 160 IS 1 BP A31 EP A38 DI 10.1149/2.049301jes PG 8 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA 071GM UT WOS:000313578400005 ER PT J AU Johnson, A Merilis, G Hastings, J Palmer, ME Fitts, JP Chidambaram, D AF Johnson, Ashley Merilis, Giorvanni Hastings, Jason Palmer, M. Elizabeth Fitts, Jeffrey P. Chidambaram, Dev TI Reductive Degradation of Organic Compounds Using Microbial Nanotechnology SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID SULFATE-REDUCING BACTERIA; FE-0/AIR PROCESS; IDENTIFICATION; NANOPARTICLES; AZOREDUCTASE; PARTICLES; PALLADIUM; AZO; PHOTODEGRADATION; TIO2 AB Members of the genus Clostridia can reduce Pd(II) ions to form metallic Pd nanoparticles (bio-Pd). Cultures of C. pasteurianum BC1 were used to generate bio-Pd, which is primarily formed on the microbial cell wall. Batch experiments using C. pasteurianum BC1 cells loaded with bio-Pd showed efficient reduction of the organic azo dyes, methyl orange and Evans blue, while little reduction of dyes was observed in control experiments using Pd-containing heat-killed microbial cultures or Pd-free viable bacterial cultures. Degradation of azo dyes was found to occur via reductive hydrogenation of the azo-linkage. Molecular hydrogen, which is concomitantly generated by C. pasteurianum, is used in the reduction reaction. The process described in this study is a potentially viable alternative to current groundwater and wastewater treatment technologies that fail to adequately degrade the large quantities of hazardous spent textile dyes that are discharged into the environment each year. (C) 2012 The Electrochemical Society. [DOI: 10.1149/2.053301jes] All rights reserved. C1 [Johnson, Ashley; Merilis, Giorvanni] Tallahassee Community Coll, Tallahassee, FL 32304 USA. [Hastings, Jason; Palmer, M. Elizabeth; Chidambaram, Dev] Univ Nevada, Reno, NV 89557 USA. [Fitts, Jeffrey P.] Brookhaven Natl Lab, Dept Environm Sci, Upton, NY 11973 USA. RP Johnson, A (reprint author), Florida A&M Univ, Tallahassee, FL 32307 USA. EM dcc@unr.edu RI Fitts, Jeffrey/J-3633-2012 FU Office of Vice President for Research at UNR; DOE Office of Science, Office of Biological and Environmental Research [KPCH137]; UNR Graduate School FX This work was supported by the start-up funds provided to DC from the Office of Vice President for Research at UNR and the DOE Office of Science, Office of Biological and Environmental Research, under project KPCH137. JH acknowledges the ACCESS scholarship provided to him by the UNR Graduate School. We thank Dr. Jim Quinn (Department of Materials Science and Engineering at the State University of New York at Stony Brook, NY) for technical assistance with Scanning Electron Microscopy. AJ and GM thank the BNL Office of Educational Programs for the summer internships. NR 25 TC 4 Z9 4 U1 3 U2 44 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2013 VL 160 IS 1 BP G27 EP G31 DI 10.1149/2.053301jes PG 5 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA 071GM UT WOS:000313578400058 ER PT J AU Wang, W Choi, DW Yang, ZG AF Wang, Wei Choi, Daiwon Yang, Zhenguo TI Li-Ion Battery with LiFePO4 Cathode and Li4Ti5O12 Anode for Stationary Energy Storage SO METALLURGICAL AND MATERIALS TRANSACTIONS A-PHYSICAL METALLURGY AND MATERIALS SCIENCE LA English DT Article ID ELECTRODES AB Li-ion batteries based on commercially available LiFePO4 cathode and Li4Ti5O12 anode were investigated for potential stationary energy storage applications. The full cell that operated at flat 1.85 V demonstrated stable cycling up to 200 cycles followed by a rapid fade. A Li-ion full cell with Ketjen black modified LiFePO4 cathode and an unmodified Li4Ti5O12 anode exhibited negligible fade after more than 1200 cycles with a capacity of similar to 130 mAh/g at C/2. The improved stability, along with its cost-effectiveness, environmental benignity, and safety, make the LiFePO4/Li4Ti5O12 combination Li-ion battery a promising option for storing renewable energy. DOI: 10.1007/s11661-012-1284-4 (C) The Minerals, Metals & Materials Society and ASM International (outside the USA) 2012 C1 [Wang, Wei; Choi, Daiwon] Pacific NW Natl Lab, Richland, WA 99354 USA. [Yang, Zhenguo] UniEnergy Technol LLC, Mukilteo, WA 98275 USA. RP Wang, W (reprint author), Pacific NW Natl Lab, 902 Battelle Blvd,POB 999, Richland, WA 99354 USA. EM wei.wang@pnnl.gov; daiwon.choi@pnnl.gov RI Wang, Wei/F-4196-2010; Choi, Daiwon/B-6593-2008 OI Wang, Wei/0000-0002-5453-4695; FU Office of Vehicle Technologies of the United States Department of Energy [DE-AC02-05CH11231, 24134]; United States Department of Energy [DE-AC05-76RL01830] FX This work was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the United States Department of Energy, under Contract No. DE-AC02-05CH11231, Subcontract No. 24134 under the Batteries for Advanced Transportation Technologies (BATT) Program. Pacific Northwest National Laboratory is a multiprogram national laboratory operated by Battelle Memorial Institute for the United States Department of Energy under Contract No. DE-AC05-76RL01830. NR 14 TC 9 Z9 9 U1 5 U2 78 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1073-5623 J9 METALL MATER TRANS A JI Metall. Mater. Trans. A-Phys. Metall. Mater. Sci. PD JAN PY 2013 VL 44A SU 1 BP 21 EP 25 DI 10.1007/s11661-012-1284-4 PG 5 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Materials Science; Metallurgy & Metallurgical Engineering GA 073AT UT WOS:000313716300003 ER PT J AU Li, DS Sun, X Khaleel, M AF Li, Dongsheng Sun, Xin Khaleel, Mohammad TI Comparison of Different Upscaling Methods for Predicting Thermal Conductivity of Complex Heterogeneous Materials System: Application on Nuclear Waste Forms SO METALLURGICAL AND MATERIALS TRANSACTIONS A-PHYSICAL METALLURGY AND MATERIALS SCIENCE LA English DT Article ID FUKUSHIMA AB To develop strategies for determining thermal conductivity based on the prediction of a complex heterogeneous materials system and loaded nuclear waste forms, the computational efficiency and accuracy of different upscaling methods has been evaluated. The effective thermal conductivity, obtained from microstructure information and local thermal conductivity of different components, is critical in predicting the life and performance of waste forms during storage. Several methods, including the Taylor model, Sachs model, self-consistent model, and statistical upscaling method, were developed and implemented. Microstructure-based finite-element method (FEM) prediction results were used to as a benchmark to determine the accuracy of the different upscaling methods. Micrographs from waste forms with varying waste loadings were used in the prediction of thermal conductivity in FEM and homogenization methods. Prediction results demonstrated that in term of efficiency, boundary models (e. g., Taylor model and Sachs model) are stronger than the self-consistent model, statistical upscaling method, and finite-element method. However, when balancing computational efficiency and accuracy, statistical upscaling is a useful method in predicting effective thermal conductivity for nuclear waste forms. DOI: 10.1007/s11661-012-1269-3 (C) The Minerals, Metals & Materials Society and ASM International 2012 C1 [Li, Dongsheng; Sun, Xin; Khaleel, Mohammad] Pacific NW Natl Lab, Fundamental & Computat Sci Directorate, Richland, WA 99352 USA. RP Li, DS (reprint author), Pacific NW Natl Lab, Fundamental & Computat Sci Directorate, Richland, WA 99352 USA. EM dongsheng.li@pnl.gov OI khaleel, mohammad/0000-0001-7048-0749 FU DOE's Nuclear Energy Advanced Modeling and Simulation (NEAMS) program; DOE [DE-AC05-76RL01830] FX This work was funded by DOE's Nuclear Energy Advanced Modeling and Simulation (NEAMS) program. Pacific Northwest National Laboratory is operated by Battelle for the DOE under contract DE-AC05-76RL01830. NR 21 TC 3 Z9 3 U1 0 U2 5 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1073-5623 J9 METALL MATER TRANS A JI Metall. Mater. Trans. A-Phys. Metall. Mater. Sci. PD JAN PY 2013 VL 44A SU 1 BP 61 EP 69 DI 10.1007/s11661-012-1269-3 PG 9 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Materials Science; Metallurgy & Metallurgical Engineering GA 073AT UT WOS:000313716300007 ER PT J AU Anderoglu, O Byun, TS Toloczko, M Maloy, SA AF Anderoglu, Osman Byun, Thak Sang Toloczko, Mychailo Maloy, Stuart A. TI Mechanical Performance of Ferritic Martensitic Steels for High Dose Applications in Advanced Nuclear Reactors SO METALLURGICAL AND MATERIALS TRANSACTIONS A-PHYSICAL METALLURGY AND MATERIALS SCIENCE LA English DT Article ID IRRADIATED FERRITIC/MARTENSITIC STEELS; LOW-TEMPERATURE IRRADIATION; REDUCED-ACTIVATION; TENSILE PROPERTIES; STRUCTURAL-MATERIALS; FRACTURE-TOUGHNESS; NEUTRON-IRRADIATION; IMPACT PROPERTIES; STAINLESS-STEEL; DEGREES-C AB Ferritic/martensitic (F/M) steels are considered for core applications and pressure vessels in Generation IV reactors as well as first walls and blankets for fusion reactors. There are significant scientific data on testing and industrial experience in making this class of alloys worldwide. This experience makes F/M steels an attractive candidate. In this article, tensile behavior, fracture toughness and impact property, and creep behavior of the F/M steels under neutron irradiations to high doses with a focus on high Cr content (8 to 12) are reviewed. Tensile properties are very sensitive to irradiation temperature. Increase in yield and tensile strength (hardening) is accompanied with a loss of ductility and starts at very low doses under irradiation. The degradation of mechanical properties is most pronounced at <0.3T(M) (T-M is melting temperature) and up to 10 dpa (displacement per atom). Ferritic/martensitic steels exhibit a high fracture toughness after irradiation at all temperatures even below 673 K (400 degrees C), except when tested at room temperature after irradiations below 673 K (400 degrees C), which shows a significant reduction in fracture toughness. Creep studies showed that for the range of expected stresses in a reactor environment, the stress exponent is expected to be approximately one and the steady state creep rate in the absence of swelling is usually better than austenitic stainless steels both in terms of the creep rate and the temperature sensitivity of creep. In short, F/M steels show excellent promise for high dose applications in nuclear reactors. DOI: 10.1007/s11661-012-1565-y (C) The Minerals, Metals & Materials Society and ASM International (outside the USA) 2012 C1 [Anderoglu, Osman; Maloy, Stuart A.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Byun, Thak Sang] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. [Toloczko, Mychailo] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Anderoglu, O (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM oanderoglu@gmail.com RI Lujan Center, LANL/G-4896-2012; Maloy, Stuart/A-8672-2009 OI Maloy, Stuart/0000-0001-8037-1319 NR 111 TC 9 Z9 9 U1 3 U2 53 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1073-5623 EI 1543-1940 J9 METALL MATER TRANS A JI Metall. Mater. Trans. A-Phys. Metall. Mater. Sci. PD JAN PY 2013 VL 44A SU 1 BP 70 EP 83 DI 10.1007/s11661-012-1565-y PG 14 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Materials Science; Metallurgy & Metallurgical Engineering GA 073AT UT WOS:000313716300008 ER PT J AU Byun, TS Li, MM Farrell, K AF Byun, Thak Sang Li, Meimei Farrell, Kenneth TI Dose Dependence of Strength After Low-Temperature Irradiation in Metallic Materials SO METALLURGICAL AND MATERIALS TRANSACTIONS A-PHYSICAL METALLURGY AND MATERIALS SCIENCE LA English DT Article ID AUSTENITIC STAINLESS-STEELS; COPPER SINGLE CRYSTALS; NEUTRON-IRRADIATION; PLASTIC INSTABILITY; DEFORMATION MICROSTRUCTURE; RADIATION-EMBRITTLEMENT; POLYCRYSTALLINE METALS; MECHANICAL-PROPERTIES; DEFECT ACCUMULATION; TENSILE PROPERTIES AB This study intends to review and characterize the low-temperature (<473 K [200 degrees C]) irradiation-hardening behaviors in metallic materials and to propose new interpretations on the dose dependence of strength, particularly in the prehardening and saturation regimes. The analysis of results of yield stress-dose curves indicate that four dose-dependence regimes exist: the prehardening, main hardening, saturation, and embrittlement regimes. The semilog plots of yield stress vs dose data revealed that the prehardening regime displaying zero hardening or softening was common at least for the alloys with low-dose data available. It was observed that the dose range of the prehardening regime increased with the strength of material, which indicates that slower initiation in irradiation hardening is expected when strength is higher. For the majority of the metallic materials analyzed, it was reconfirmed that the exponent of the power-law hardening function was evaluated to be about 0.5 in the main hardening regime and about 0.1 in the saturation regime. In these positive hardening regimes, the low strength pure metals such as Fe, Ta, Cu, and Zr displayed lower hardening exponents. The minimum dose to the saturation of irradiation hardening was in the range of 0.003 to 0.08 dpa, depending on the category of materials. It was also reaffirmed that there exists a strong relationship between the saturation in irradiation hardening and the occurrence of plastic instability at yield. DOI: 10.1007/s11661-012-1309-z (C) The Minerals, Metals & Materials Society and ASM International (outside the USA) 2012 C1 [Byun, Thak Sang; Li, Meimei; Farrell, Kenneth] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. RP Byun, TS (reprint author), Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. EM byunts@ornl.gov FU U.S. Department of Energy, Offices of Nuclear Energy and Basic Energy Science [DE-AC05-00OR22725]; UT-Battelle, LLC FX This research was sponsored by U.S. Department of Energy, Offices of Nuclear Energy and Basic Energy Science, under Contract DE-AC05-00OR22725 with UT-Battelle, LLC. The authors express special thanks to Drs. J. T. Busby and C.S. Shin for their thorough reviews and thoughtful comments. NR 49 TC 2 Z9 2 U1 1 U2 22 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1073-5623 J9 METALL MATER TRANS A JI Metall. Mater. Trans. A-Phys. Metall. Mater. Sci. PD JAN PY 2013 VL 44A SU 1 BP 84 EP 93 DI 10.1007/s11661-012-1309-z PG 10 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Materials Science; Metallurgy & Metallurgical Engineering GA 073AT UT WOS:000313716300009 ER PT J AU Kant, ME Siriruk, A Penumadu, D Garlea, E Vogel, SC Yu, X Parish, CM AF Kant, Matthew E. Siriruk, Akawut Penumadu, Dayakar Garlea, Elena Vogel, Sven C. Yu, X. Parish, Chad M. TI Multi-Axial Mechanical Behavior of Zircaloy-702 and Effect on Initial Texture SO METALLURGICAL AND MATERIALS TRANSACTIONS A-PHYSICAL METALLURGY AND MATERIALS SCIENCE LA English DT Article ID ZIRCONIUM AB Zircaloy-702 (Zr-702 or UNS R60702) cylindrical tubes are commonly used for applications requiring mechanical stability in extreme environments. Owing to its crystal structure and processing techniques, significant texture and anisotropic mechanical properties are possible. In the current study, combined axial-torsional testing is employed to probe macroscopic stress-strain behavior in three dimensions, and corresponding yield surface in octahedral plane is obtained. Zr-702 tube samples are characterized under pure tension, torsion, and combined (tension and torsion) loading. Three-dimensional digital image correlation using VIC-3D system was implemented to determine surface deformation patterns for identification of strain localizations. Neutron diffraction-based texture analysis is performed to obtain an understanding of the effect of loading path on the material texture compared with the as-received, initial grain orientation. Pole figures for Zr-702 tubes are obtained for each loading path. DOI: 10.1007/s11661-012-1564-z (C) The Minerals, Metals & Materials Society and ASM International 2012 C1 [Kant, Matthew E.; Siriruk, Akawut; Penumadu, Dayakar] Univ Tennessee, Knoxville, TN 37996 USA. [Vogel, Sven C.; Yu, X.] Los Alamos Natl Lab, Los Alamos, NM USA. [Parish, Chad M.] Oak Ridge Natl Lab, Oak Ridge, TN USA. RP Kant, ME (reprint author), Univ Tennessee, Knoxville, TN 37996 USA. EM dpenumad@utk.edu RI Lujan Center, LANL/G-4896-2012; Parish, Chad/J-8381-2013; OI Vogel, Sven C./0000-0003-2049-0361 FU Y-12 National Security Complex's Plant Directed Research and Development program; U.S. Department of Energy [DE-AC05-00OR22800]; Oak Ridge National Laboratory's ShaRE User Facility; Scientific User Facilities Division, the Office of Basic Energy Sciences, the U.S. Department of Energy; United States Government FX The funding for this research was provided by the Y-12 National Security Complex's Plant Directed Research and Development program. This research was also supported in part by the U.S. Department of Energy under contract DE-AC05-00OR22800. Texture measurements were obtained through Los Alamos Neutron Science Center (LANSCE) user project of Dr. Penumadu. This research was also supported in part by Oak Ridge National Laboratory's ShaRE User Facility, which is sponsored by the Scientific User Facilities Division, the Office of Basic Energy Sciences, the U.S. Department of Energy.; This paper was prepared as an account of study 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 or any agency thereof. NR 21 TC 0 Z9 0 U1 0 U2 17 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1073-5623 J9 METALL MATER TRANS A JI Metall. Mater. Trans. A-Phys. Metall. Mater. Sci. PD JAN PY 2013 VL 44A SU 1 BP 94 EP 108 DI 10.1007/s11661-012-1564-z PG 15 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Materials Science; Metallurgy & Metallurgical Engineering GA 073AT UT WOS:000313716300010 ER PT J AU Mizia, RE Clark, DE Glazoff, MV Lister, TE Trowbridge, TL AF Mizia, Ronald E. Clark, Denis E. Glazoff, Michael V. Lister, Tedd E. Trowbridge, Tammy L. TI Optimizing the Diffusion Welding Process for Alloy 800H: Thermodynamic, Diffusion Modeling, and Experimental Work SO METALLURGICAL AND MATERIALS TRANSACTIONS A-PHYSICAL METALLURGY AND MATERIALS SCIENCE LA English DT Article ID COUPLES AB A research effort was made to evaluate the usefulness of modern thermodynamic and diffusion computational tools, Thermo-Calc and Dictra (Thermo_Calc Software, Inc., McMurray, PA), in optimizing the parameters for diffusion welding of Alloy 800H. This would achieve a substantial reduction in the overall number of experiments required to achieve optimal welding and post-weld heat treatment conditions. This problem is important because diffusion-welded components of Alloy 800H are being evaluated for use in assembling compact, micro-channel heat exchangers that are being proposed in the design of a high-temperature, gas-cooled reactor by the U.S. Department of Energy. The modeling was done in close contact with experimental work. The latter included using the Gleeble 3500 System (Dynamic Systems, Inc., Poestenkill, NY) for welding simulation, mechanical property measurement, and light optical and scanning electron microscopy. The modeling efforts suggested a temperature of 1423 K (1150 degrees C) for 1 hour with an applied pressure of 5 MPa using a 15-mu m Ni foil as joint filler to reduce chromium oxidation on the welded surfaces. Good agreement between modeled and experimentally determined concentration gradients was achieved, and model refinements to account for the complexity of actual alloy materials are suggested. DOI: 10.1007/s11661-011-0991-6 (C) The Minerals, Metals & Materials Society and ASM International 2011 C1 [Mizia, Ronald E.; Clark, Denis E.; Lister, Tedd E.; Trowbridge, Tammy L.] Idaho Natl Lab, Div Mat Sci, Idaho Falls, ID USA. RP Mizia, RE (reprint author), Idaho Natl Lab, Div Mat Sci, Idaho Falls, ID USA. EM Michael.Glazoff@inl.gov FU U.S. Department of Energy, Office of Nuclear Energy, Science, and Technology under DOE Idaho Operations Office [DE-AC0799ID13727]; U.S. Government under DOE [DE-AC07-05ID14517]; U.S. Government FX The authors would like to express gratitude to the Next Generation Nuclear Plant (NGNP) Program Management (Messrs Michael Patterson and Charles Park) at INL for their continuous support of this research effort. The work was supported through the U.S. Department of Energy, Office of Nuclear Energy, Science, and Technology, under DOE Idaho Operations Office Contract DE-AC0799ID13727. The authors would like to acknowledge Todd Morris for metallurgical support. One of the authors (M. V. G.) would like to extend his most sincere gratitude to Dr. Carolyn Campbell (NIST) for her generous support of our initial modeling efforts. We are also very grateful to Prof. Zi-Kui Liu and Prof. Long-Qing Chen (both of Penn State University) for the valuable discussions, and to Prof. John E. Morral (of Ohio State University) for the useful discussion of the obtained results. This submitted manuscript was authored by a contractor of the U.S. Government under DOE Contract No. DE-AC07-05ID14517. Accordingly, the U. S. Government retains and the publisher, by accepting the article for publication, acknowledges that the U. S. Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for U. S. Government purposes.; This information was prepared as an account of work sponsored by an agency of the U.S. Government. Neither the U. S. Government nor any agency thereof, nor any of their employees, makes any warranty, express or implied, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. References herein to any specific commercial product, process, or service by trade name, trademark, manufacturer, or otherwise, does not necessarily constitute or imply its endorsement, recommendation, or favoring by the U.S. Government or any agency thereof. The views and opinions of authors expressed herein do not necessarily state or reflect those of the U. S. Government or any agency thereof. NR 20 TC 3 Z9 4 U1 2 U2 24 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1073-5623 J9 METALL MATER TRANS A JI Metall. Mater. Trans. A-Phys. Metall. Mater. Sci. PD JAN PY 2013 VL 44A SU 1 BP 154 EP 161 DI 10.1007/s11661-011-0991-6 PG 8 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Materials Science; Metallurgy & Metallurgical Engineering GA 073AT UT WOS:000313716300014 ER PT J AU Joshi, VV Choi, JP Darsell, J Meier, A Weil, KS AF Joshi, Vineet V. Choi, Jung-Pyung Darsell, Jens Meier, Alan Weil, K. Scott TI Reactive Air Aluminizing of Nicrofer-6025HT for Use in Advanced Coal-Based Power Plants SO METALLURGICAL AND MATERIALS TRANSACTIONS A-PHYSICAL METALLURGY AND MATERIALS SCIENCE LA English DT Article ID OXIDATION AB Nicrofer-6025HT (Nicrofer) has been selected as a potential manifold material for advanced air separation units that use mixed ionic and electronic conductors (MIECs). Reactive air brazing (RAB) is a recently developed joining technique that has the potential to obtain high-quality joints with the required hermeticity between Nicrofer and the MIEC. Successful RAB joining of these two distinct materials requires an alumina surface layer on the Nicrofer. To aluminize the surface of Nicrofer, a recently developed reactive air aluminizing (RAA) technique was used. The current work demonstrated the feasibility of preparing RAA coatings on Nicrofer and compared the effect of aluminum powder size on the RAA process. DOI: 10.1007/s11661-012-1237-y (C) The Minerals, Metals & Materials Society and ASM International 2012 C1 [Joshi, Vineet V.; Choi, Jung-Pyung; Darsell, Jens; Weil, K. Scott] Pacific NW Natl Lab, Richland, WA 99354 USA. [Meier, Alan] Montana Tech Univ, Dept Met & Mat Engn, Butte, MT 59701 USA. RP Joshi, VV (reprint author), Pacific NW Natl Lab, Richland, WA 99354 USA. EM vineet.joshi@pnnl.gov OI Joshi, Vineet/0000-0001-7600-9317 FU U.S. Department of Energy, Office of Fossil Energy; United States Department of Energy (U.S. DOE) [DE-AC06-76RLO 1830] FX This work was supported by the U.S. Department of Energy, Office of Fossil Energy. The Pacific Northwest National Laboratory is operated by Battelle Memorial Institute for the United States Department of Energy (U.S. DOE) under Contract DE-AC06-76RLO 1830. NR 11 TC 3 Z9 3 U1 0 U2 7 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1073-5623 J9 METALL MATER TRANS A JI Metall. Mater. Trans. A-Phys. Metall. Mater. Sci. PD JAN PY 2013 VL 44A SU 1 BP 188 EP 192 DI 10.1007/s11661-012-1237-y PG 5 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Materials Science; Metallurgy & Metallurgical Engineering GA 073AT UT WOS:000313716300017 ER PT J AU Bonissone, S Gupta, N Romine, M Bradshaw, RA Pevzner, PA AF Bonissone, Stefano Gupta, Nitin Romine, Margaret Bradshaw, Ralph A. Pevzner, Pavel A. TI N-terminal Protein Processing: A Comparative Proteogenomic Analysis SO MOLECULAR & CELLULAR PROTEOMICS LA English DT Article ID TANDEM MASS-SPECTRA; SACCHAROMYCES-CEREVISIAE; POSTTRANSLATIONAL MODIFICATIONS; METHIONINE AMINOPEPTIDASE; AMINO-ACID; END RULE; IDENTIFICATION; SEQUENCE; ESCHERICHIA-COLI-K12; TRANSLATION AB N-terminal methionine excision (NME) and N-terminal acetylation (NTA) are two of the most common protein post-translational modifications. NME is a universally conserved activity and a highly specific mechanism across all life forms. NTA is very common in eukaryotes but occurs rarely in prokaryotes. By analyzing data sets from yeast, mammals and bacteria (including 112 million spectra from 57 bacterial species), the largest comparative proteogenomics study to date, it is shown that previous assumptions/perceptions about the specificity and purposes of NME are not entirely correct. Although NME, through the universal enzymatic specificity of the methionine aminopeptidases, results in the removal of the initiator Met in proteins when the second residue is Gly, Ala, Ser, Cys, Thr, Pro, or Val, the comparative genomic analyses suggest that this specificity may vary modestly in some organisms. In addition, the functional role of NME may be primarily to expose Ala and Ser rather than all seven of these residues. Although any of this group provide "stabilizing'' N termini in the N-end rule, and de facto leave the remaining 13 amino acid types that are classed as "destabilizing'' (in higher eukaryotes) protected by the initiator Met, the conservation of NME-substrate proteins through evolution suggests that the other five are not crucially important for proteins with these residues in the second position. They are apparently merely inconsequential players (their function is not affected by NME) that become exposed because their side chains are smaller or comparable to those of Ala and Ser. The importance of exposing mainly two amino acids at the N terminus, i.e. Ala and Ser, is unclear but may be related to NTA or other post-translational modifications. In this regard, these analyses also reveal that NTA is more prevalent in some prokaryotes than previously appreciated. Molecular & Cellular Proteomics 12: 10.1074/mcp.M112.019075, 14-28, 2013. C1 [Bonissone, Stefano] Univ Calif San Diego, Bioinformat Program, La Jolla, CA 92093 USA. [Romine, Margaret] Pacific NW Natl Lab, Div Biol Sci, Richland, WA 99352 USA. [Bradshaw, Ralph A.] Univ Calif San Francisco, Dept Pharmaceut Chem, San Francisco, CA USA. [Pevzner, Pavel A.] Univ Calif San Diego, Dept Comp Sci & Engn, La Jolla, CA 92093 USA. RP Bonissone, S (reprint author), Univ Calif San Diego, Bioinformat Program, La Jolla, CA 92093 USA. EM sbonisso@ucsd.edu; ppevzner@ucsd.edu RI Bradshaw, Ralph/K-1515-2013; OI Romine, Margaret/0000-0002-0968-7641; Gupta, Nitin/0000-0002-8408-3848 FU National Center for Research Resources of NIH [P-41-RR24851]; U.S. Department of Energy (DOE) Office of Biological and Environmental Research under the Genomics:GTL Program via the Shewanella Federation consortium; U.S. Department of Energy (DOE) Office of Biological and Environmental Research under the Genomics:GTL Program via and proteomics applications project; DOE [DE-AC05-76RLO1830]; NIH [8 P41 GM103481] FX The research was supported by the National Center for Research Resources of NIH via grant P-41-RR24851. RM was supported by the U.S. Department of Energy (DOE) Office of Biological and Environmental Research under the Genomics:GTL Program via the Shewanella Federation consortium and proteomics applications project. Pacific Northwest National Laboratory is operated for the DOE by Battelle Memorial Institute under Contract DE-AC05-76RLO1830. RAB is supported in part by NIH 8 P41 GM103481. NR 41 TC 33 Z9 33 U1 2 U2 30 PU AMER SOC BIOCHEMISTRY MOLECULAR BIOLOGY INC PI BETHESDA PA 9650 ROCKVILLE PIKE, BETHESDA, MD 20814-3996 USA SN 1535-9476 J9 MOL CELL PROTEOMICS JI Mol. Cell. Proteomics PD JAN PY 2013 VL 12 IS 1 BP 14 EP 28 DI 10.1074/mcp.M112.019075 PG 15 WC Biochemical Research Methods SC Biochemistry & Molecular Biology GA 071AN UT WOS:000313557600002 PM 23001859 ER PT J AU Hsieh, SI Castruita, M Malasarn, D Urzica, E Erde, J Page, MD Yamasaki, H Casero, D Pellegrini, M Merchant, SS Loo, JA AF Hsieh, Scott I. Castruita, Madeli Malasarn, Davin Urzica, Eugen Erde, Jonathan Page, M. Dudley Yamasaki, Hiroaki Casero, David Pellegrini, Matteo Merchant, Sabeeha S. Loo, Joseph A. TI The Proteome of Copper, Iron, Zinc, and Manganese Micronutrient Deficiency in Chlamydomonas reinhardtii SO MOLECULAR & CELLULAR PROTEOMICS LA English DT Article ID S-ADENOSYLHOMOCYSTEINE HYDROLASE; LIGHT-HARVESTING COMPLEX; GENE-EXPRESSION; GREEN-ALGA; COPROPORPHYRINOGEN OXIDASE; SACCHAROMYCES-CEREVISIAE; QUANTITATIVE PROTEOMICS; CHLOROPLAST RIBOSOME; CARBONIC-ANHYDRASE; ABSOLUTE PROTEIN AB Trace metals such as copper, iron, zinc, and manganese play important roles in several biochemical processes, including respiration and photosynthesis. Using a label-free, quantitative proteomics strategy (MSE), we examined the effect of deficiencies in these micronutrients on the soluble proteome of Chlamydomonas reinhardtii. We quantified >10(3) proteins with abundances within a dynamic range of 3 to 4 orders of magnitude and demonstrated statistically significant changes in similar to 200 proteins in each metal-deficient growth condition relative to nutrient-replete media. Through analysis of Pearson's coefficient, we also examined the correlation between protein abundance and transcript abundance (as determined via RNA-Seq analysis) and found moderate correlations under all nutritional states. Interestingly, in a subset of transcripts known to significantly change in abundance in metal-replete and metal-deficient conditions, the correlation to protein abundance is much stronger. Examples of new discoveries highlighted in this work include the accumulation of O-2 labile, anaerobiosis-related enzymes (Hyd1, Pfr1, and Hcp2) in copper-deficient cells; co-variation of Cgl78/Ycf54 and coprogen oxidase; the loss of various stromal and lumenal photosynthesis-related proteins, including plastocyanin, in iron-limited cells; a large accumulation (from undetectable amounts to over 1,000 zmol/cell) of two COG0523 domain-containing proteins in zinc-deficient cells; and the preservation of photosynthesis proteins in manganese-deficient cells despite known losses in photosynthetic function in this condition. Molecular & Cellular Proteomics 12: 10.1074/mcp.M112.021840, 65-86, 2013. C1 [Hsieh, Scott I.; Castruita, Madeli; Malasarn, Davin; Urzica, Eugen; Erde, Jonathan; Page, M. Dudley; Yamasaki, Hiroaki; Merchant, Sabeeha S.; Loo, Joseph A.] Univ Calif Los Angeles, Dept Chem & Biochem, Los Angeles, CA 90095 USA. [Casero, David; Pellegrini, Matteo; Merchant, Sabeeha S.; Loo, Joseph A.] Univ Calif Los Angeles, UCLA DOE Inst Genom & Prote, Los Angeles, CA 90095 USA. [Casero, David; Pellegrini, Matteo] Univ Calif Los Angeles, Dept Mol Cell & Dev Biol, Los Angeles, CA 90095 USA. [Loo, Joseph A.] Univ Calif Los Angeles, David Geffen Sch Med, Dept Biol Chem, Los Angeles, CA 90095 USA. RP Merchant, SS (reprint author), Univ Calif Los Angeles, Dept Chem & Biochem, 607 Charles E Young Dr E, Los Angeles, CA 90095 USA. EM sabeeha@chem.ucla.edu; JLoo@chem.ucla.edu RI Urzica, Eugen/B-7903-2013; Casero, David/E-7365-2010; OI Casero, David/0000-0002-7347-3330; Urzica, Eugen/0000-0002-1028-7442 FU National Institutes of Health [GM42143]; Department of Energy [DE-FD02-04ER15529, DE-FC03-02ER6342]; NIH [F32 GM086006, F32 GM083562]; Ruth L. Kirschstein National Research Service Award [T32 GM07185] FX This work was supported by the National Institutes of Health (Grant No. GM42143 to S.M. for the work on Cu and Zn) and the Department of Energy (Grant Nos. DE-FD02-04ER15529 to S.M. for the work on Fe and Mn and DE-FC03-02ER6342 to the UCLA/DOE Institute for Genomics and Proteomics). M.C. and D.M. acknowledge fellowship support from the NIH (Nos. F32 GM086006 and F32 GM083562, respectively). S.I.H. and J.E. were supported in part by a Ruth L. Kirschstein National Research Service Award (T32 GM07185) for UCLA's predoctoral Cellular and Molecular Biology Training Program. NR 95 TC 26 Z9 26 U1 4 U2 115 PU AMER SOC BIOCHEMISTRY MOLECULAR BIOLOGY INC PI BETHESDA PA 9650 ROCKVILLE PIKE, BETHESDA, MD 20814-3996 USA SN 1535-9476 J9 MOL CELL PROTEOMICS JI Mol. Cell. Proteomics PD JAN PY 2013 VL 12 IS 1 BP 65 EP 86 DI 10.1074/mcp.M112.021840 PG 22 WC Biochemical Research Methods SC Biochemistry & Molecular Biology GA 071AN UT WOS:000313557600006 PM 23065468 ER PT J AU Abraham, P Giannone, RJ Adams, RM Kalluri, U Tuskan, GA Hettich, RL AF Abraham, Paul Giannone, Richard J. Adams, Rachel M. Kalluri, Udaya Tuskan, Gerald A. Hettich, Robert L. TI Putting the Pieces Together: High-performance LC-MS/MS Provides Network-, Pathway-, and Protein-level Perspectives in Populus SO MOLECULAR & CELLULAR PROTEOMICS LA English DT Article ID SHOTGUN PROTEOMIC DATA; ARABIDOPSIS-THALIANA; MASS-SPECTROMETRY; IDENTIFICATION; GENOME; PLANTS; EXPRESSION; MODEL; PEROXIREDOXIN; CHALLENGE AB High-performance mass spectrometry (MS)-based proteomics enabled the construction of a detailed proteome atlas for Populus, a woody perennial plant model organism. Optimization of experimental procedures and implementation of current state-of-the-art instrumentation afforded the most detailed look into the predicted proteome space of Populus, offering varying proteome perspectives: (1) network-wide, (2) pathway-specific, and (3) protein-level viewpoints. Together, enhanced protein retrieval through a detergent-based lysis approach and maximized peptide sampling via the dual-pressure linear ion trap mass spectrometer (LTQ Velos), have resulted in the identification of 63,056 tryptic peptides. The technological advancements, specifically spectral-acquisition and sequencing speed, afforded the deepest look into the Populus proteome, with peptide abundances spanning 6 orders of magnitude and mapping to similar to 25% of the predicted proteome space. In total, tryptic peptides mapped to 11,689 protein assignments across four organ-types: mature (fully expanded, leaf plastichronic index (LPI) 10-12) leaf, young (juvenile, LPI 4-6) leaf, root, and stem. To resolve protein ambiguity, identified proteins were grouped by sequence similarity (>= 90%), thereby reducing the protein assignments into 7538 protein groups. In addition, this large-scale data set features the first systems-wide survey of protein expression across different Populus organs. As a demonstration of the precision and comprehensiveness of the semiquantitative analysis, we were able to contrast two stages of leaf development, mature versus young leaf. Statistical comparison through ANOVA analysis revealed 1432 protein groups that exhibited statistically significant (p <= 0.01) differences in protein abundance. Experimental validation of the metabolic circuitry expected in mature leaf (characterized by photosynthesis and carbon fixation) compared with young leaf (characterized by rapid growth and moderate photosynthetic activities) strongly testifies to the credibility of the approach. Instead of quantitatively comparing a few proteins, a systems view of all the changes associated with a given cellular perturbation could be made. Molecular & Cellular Proteomics 12: 10.1074/mcp.M112.022996, 106-119, 2013. C1 [Abraham, Paul; Adams, Rachel M.] Univ Tennessee, Grad Sch Genome Sci & Technol, Knoxville, TN 37830 USA. [Abraham, Paul; Giannone, Richard J.; Adams, Rachel M.; Hettich, Robert L.] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. [Kalluri, Udaya; Tuskan, Gerald A.] Oak Ridge Natl Lab, Biosci Div, Oak Ridge, TN 37831 USA. RP Hettich, RL (reprint author), Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. EM hettichri@ornl.gov RI Abraham, Paul/K-5599-2015; Hettich, Robert/N-1458-2016; Tuskan, Gerald/A-6225-2011; OI Hettich, Robert/0000-0001-7708-786X; Tuskan, Gerald/0000-0003-0106-1289; KALLURI, UDAYA/0000-0002-5963-8370 FU BioEnergy Science Center, a U.S. Department of Energy Bioenergy Research Facility; Office of Biological and Environmental Research, Genome Sciences program, in the DOE Office of Science; U.S. Department of Energy FX This work was suported within the BioEnergy Science Center, a U.S. Department of Energy Bioenergy Research Facility supported by the Office of Biological and Environmental Research, Genome Sciences program, in the DOE Office of Science. University of Tennessee-Battelle LLC for the Department of Energy manages Oak Ridge National Laboratory.; This manuscript has been authored by UT-Battelle, LLC, under contract 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 55 TC 11 Z9 11 U1 1 U2 31 PU AMER SOC BIOCHEMISTRY MOLECULAR BIOLOGY INC PI BETHESDA PA 9650 ROCKVILLE PIKE, BETHESDA, MD 20814-3996 USA SN 1535-9476 EI 1535-9484 J9 MOL CELL PROTEOMICS JI Mol. Cell. Proteomics PD JAN PY 2013 VL 12 IS 1 BP 106 EP 119 DI 10.1074/mcp.M112.022996 PG 14 WC Biochemical Research Methods SC Biochemistry & Molecular Biology GA 071AN UT WOS:000313557600008 PM 23073815 ER PT J AU Metin, O Ho, SF Alp, C Can, H Mankin, MN Gultekin, MS Chi, MF Sun, SH AF Metin, Oender Ho, Sally Fae Alp, Cemalettin Can, Hasan Mankin, Max N. Gultekin, Mehmet Serdar Chi, Miaofang Sun, Shouheng TI Ni/Pd core/shell nanoparticles supported on graphene as a highly active and reusable catalyst for Suzuki-Miyaura cross-coupling reaction SO NANO RESEARCH LA English DT Article DE nickel; palladium; core/shell nanoparticles; catalysis; Suzuki-Miyaura cross-coupling ID FORMIC-ACID OXIDATION; PALLADIUM NANOPARTICLES; PD NANOPARTICLES; FACILE SYNTHESIS; AMMONIA BORANE; NANOCLUSTERS; CO AB Monodisperse Ni/Pd core/shell nanoparticles (NPs) have been synthesized by sequential reduction of nickel(II) acetate and palladium(II) bromide in oleylamine (OAm) and trioctylphosphine (TOP). The Ni/Pd NPs have a narrow size distribution with a mean particle size of 10 nm and a standard deviation of 5% with respect to the particle diameter. Mechanistic studies showed that the presence of TOP was essential to control the reductive decomposition of Ni-TOP and Pd-TOP, and the formation of Ni/Pd core/shell NPs. Using the current synthetic protocol, the composition of the Ni/Pd within the core/shell structure can be readily tuned by simply controlling the initial molar ratio of the Ni and Pd salts. The as-synthesized Ni/Pd core/shell NPs were supported on graphene (G) and used as catalyst in Suzuki-Miyaura cross-coupling reactions. Among three different kinds of Ni/Pd NPs tested, the Ni/Pd (Ni/Pd = 3/2) NPs were found to be the most active catalyst for the Suzuki-Miyaura cross-coupling of arylboronic acids with aryl iodides, bromides and even chlorides in a dimethylformamide/water mixture by using K2CO3 as a base at 110 A degrees C. The G-Ni/Pd was also stable and reusable, providing 98% conversion after the 5(th) catalytic run without showing any noticeable Ni/Pd composition change. The G-Ni/Pd structure reported in this paper combines both the efficiency of a homogeneous catalyst and the durability of a heterogeneous catalyst, and is promising catalyst candidate for various Pd-based catalytic applications. C1 [Metin, Oender; Ho, Sally Fae; Mankin, Max N.; Sun, Shouheng] Brown Univ, Dept Chem, Providence, RI 02921 USA. [Metin, Oender; Alp, Cemalettin; Can, Hasan; Gultekin, Mehmet Serdar] Ataturk Univ, Dept Chem, Fac Sci, TR-25240 Erzurum, Turkey. [Chi, Miaofang] Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. [Alp, Cemalettin] Erzincan Univ, Cayirli Vocat Sch, Erzincan, Turkey. RP Metin, O (reprint author), Brown Univ, Dept Chem, Providence, RI 02921 USA. EM ometin@atauni.edu.tr; ssun@brown.edu RI Chi, Miaofang/Q-2489-2015 OI Chi, Miaofang/0000-0003-0764-1567 FU U.S. Army Research Laboratory; A.S. Army Research Office under the Multi University Research Initiative (MURI) [W911NF-11-1-0353]; Ataturk University Scientific Research Project Council [2011/93]; Office of Basic Energy Sciences, U.S. Department of Energy FX This work was supported by the U.S. Army Research Laboratory and the A.S. Army Research Office under the Multi University Research Initiative (MURI) grant No. W911NF-11-1-0353 on "Stress-Controlled Catalysis via Engineered Nanostructures" and "Ataturk University Scientific Research Project Council (Project No. 2011/93)". Microscopy research was supported in part by ORNL's Shared Research Equipment (ShaRE) User Facility, which is sponsored by the Office of Basic Energy Sciences, U.S. Department of Energy. NR 27 TC 78 Z9 78 U1 29 U2 342 PU TSINGHUA UNIV PRESS PI BEIJING PA TSINGHUA UNIV, RM A703, XUEYAN BLDG, BEIJING, 10084, PEOPLES R CHINA SN 1998-0124 J9 NANO RES JI Nano Res. PD JAN PY 2013 VL 6 IS 1 BP 10 EP 18 DI 10.1007/s12274-012-0276-4 PG 9 WC Chemistry, Physical; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA 072GW UT WOS:000313658800002 ER PT J AU Suresh, AK Pelletier, DA Doktycz, MJ AF Suresh, Anil K. Pelletier, Dale A. Doktycz, Mitchel J. TI Relating nanomaterial properties and microbial toxicity SO NANOSCALE LA English DT Article ID METAL-OXIDE NANOPARTICLES; TITANIUM-DIOXIDE NANOPARTICLES; SILVER SULFIDE NANOPARTICLES; GRAM-POSITIVE BACTERIA; CDTE QUANTUM DOTS; ANTIBACTERIAL ACTIVITY; ESCHERICHIA-COLI; PSEUDOMONAS-AERUGINOSA; ZNO NANOPARTICLES; WASTE-WATER AB Metal andmetal oxide nanoparticles are among the most commonly used nanomaterials and their potential for adversely affecting environmental systems raises concern. Complex microbial consortia underlie environmental processes, and the potential toxicity of nanoparticles to microbial systems, and the consequent impacts on trophic balances, is particularly worrisome. The diverse array of metal and metal oxides, the different sizes and shapes that can be prepared and the variety of possible surface coatings complicate assessments of toxicity. Further muddling biocidal interpretations are the diversity of microbes and their intrinsic tolerances to stresses. Here, we review a range of studies focused on nanoparticle-microbial interactions in an effort to correlate the physical-chemical properties of engineered metal and metal oxide nanoparticles to their biological response. General conclusions regarding the parent material of the nanoparticle and the nanoparticle's size and shape on potential toxicity can be made. However, the surface coating of the material, which can be altered significantly by environmental conditions, can ameliorate or promote microbial toxicity. Understanding nanoparticle transformations and how the nanoparticle surface can be designed to control toxicity represents a key area for further study. Additionally, the vast array of microbial species and the structuring of these species within communities complicate extrapolations of nanoparticle toxicity in real world settings. Ultimately, to interpret the effect and eventual fate of engineered materials in the environment, an understanding of the relationship between nanoparticle properties and responses at the molecular, cellular and community levels will be essential. C1 [Suresh, Anil K.; Pelletier, Dale A.; Doktycz, Mitchel J.] Oak Ridge Natl Lab, Biosci Div, Oak Ridge, TN 37831 USA. [Doktycz, Mitchel J.] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. RP Suresh, AK (reprint author), City Hope Natl Med Ctr, Dept Mol Med, 1500 E Duarte Rd, Duarte, CA 91010 USA. EM asuresh@coh.org; pelletierda@ornl.gov; doktyczmj@ornl.gov RI Doktycz, Mitchel/A-7499-2011; OI Doktycz, Mitchel/0000-0003-4856-8343; Pelletier, Dale/0000-0002-4321-7918 FU Office of Biological and Environmental Research, U.S. Department of Energy (DOE); Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. DOE; U. S. DOE [DE-AC05-00OR22725] FX The authors acknowledge support from the Office of Biological and Environmental Research, U.S. Department of Energy (DOE). 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. DOE. Oak Ridge National Laboratory is managed by UT-Battelle, LLC, for the U. S. DOE under contract DE-AC05-00OR22725. NR 115 TC 60 Z9 62 U1 15 U2 284 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2040-3364 J9 NANOSCALE JI Nanoscale PY 2013 VL 5 IS 2 BP 463 EP 474 DI 10.1039/c2nr32447d PG 12 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA 069HP UT WOS:000313426200001 PM 23203029 ER PT J AU Zhao, JM Pan, HL He, X Wang, YS Gu, L Hu, YS Chen, LQ Liu, HZ Dai, S AF Zhao, Junmei Pan, Huilin He, Xiang Wang, Yuesheng Gu, Lin Hu, Yong-Sheng Chen, Liquan Liu, Huizhou Dai, Sheng TI Size-controlled synthesis and morphology evolution of bismuth trifluoride nanocrystals via a novel solvent extraction route SO NANOSCALE LA English DT Article ID RARE-EARTH FLUORIDE; HYDROTHERMAL SYNTHESIS; SINGLE-CRYSTALLINE; CDSE NANOCRYSTALS; CONVERSION; MONODISPERSE; PHASE; GROWTH; SHAPE; MICROEMULSIONS AB Monodisperse orthorhombic-phase BiF3 nanocrystals with various shapes were prepared easily by a novel solvent extraction approach using an acid-base-coupled extractant. More importantly, the extractant used in this route can be recycled after synthesis. Our results show great promise for further extending the method to the preparation of other metal-fluoride nanoparticles. C1 [Zhao, Junmei; Liu, Huizhou] Chinese Acad Sci, Inst Proc Engn, Key Lab Green Proc & Engn, Beijing 100190, Peoples R China. [Pan, Huilin; He, Xiang; Wang, Yuesheng; Gu, Lin; Hu, Yong-Sheng; Chen, Liquan] Chinese Acad Sci, Inst Phys, Beijing Natl Lab Condensed Matter Phys, Beijing 100190, Peoples R China. [Dai, Sheng] Oak Ridge Natl Lab, Chem Sci Div, Oak Ridge, TN 37831 USA. RP Zhao, JM (reprint author), Chinese Acad Sci, Inst Proc Engn, Key Lab Green Proc & Engn, Beijing 100190, Peoples R China. EM jmzhao@home.ipe.ac.cn RI Gu, Lin/D-9631-2011; Hu, Yong-Sheng/H-1177-2011; Pan, Huilin/J-9298-2016; Dai, Sheng/K-8411-2015 OI Gu, Lin/0000-0002-7504-031X; Hu, Yong-Sheng/0000-0002-8430-6474; Dai, Sheng/0000-0002-8046-3931 FU NSFC [51104138, 50972164, 51090382]; "973" Project [2012CBA01202]; Chinese Academy of Sciences [KGZD-EW-201-1]; Chinese Academy of Sciences FX This work was supported by the NSFC (51104138 and 50972164), "973" Project (2012CBA01202), the Major Project of NSFC (no. 51090382), the Key Research Program of the Chinese Academy of Sciences (KGZD-EW-201-1), and Y.S.H. and L. G. acknowledge support from the 100 Talent Project of the Chinese Academy of Sciences. NR 40 TC 6 Z9 6 U1 3 U2 79 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2040-3364 J9 NANOSCALE JI Nanoscale PY 2013 VL 5 IS 2 BP 518 EP 522 DI 10.1039/c2nr33212d PG 5 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA 069HP UT WOS:000313426200008 PM 23202269 ER PT J AU Yoon, I Baker, SE Kim, K Wang, YM Esener, SC Sirbuly, DJ AF Yoon, Ilsun Baker, Sarah E. Kim, Kanguk Wang, Yinmin Esener, Sadik C. Sirbuly, Donald J. TI Profiling the evanescent field of nanofiber waveguides using self-assembled polymer coatings SO NANOSCALE LA English DT Article ID SCANNING OPTICAL MICROSCOPY; ABSORBENCY SENSOR; MULTILAYER FILMS; FLUORESCENCE; FORCE; SURFACE; SPECTROSCOPY; HYDROGEN; FIBERS; LAYERS AB Here we demonstrate a facile method of quantifying the decaying optical field surrounding free-standing tin dioxide (SnO2) nanofiber waveguides. Through the use of thin self-assembled polyelectrolyte coatings and fluorescent optical transmitters we map out the optical intensity as a function of distance with nanometer resolution. C1 [Yoon, Ilsun; Kim, Kanguk; Esener, Sadik C.; Sirbuly, Donald J.] Univ Calif San Diego, Dept NanoEngn, La Jolla, CA 92093 USA. [Baker, Sarah E.; Wang, Yinmin] Lawrence Livermore Natl Lab, Phys & Life Sci Directorate, Livermore, CA 94550 USA. [Esener, Sadik C.] Univ Calif San Diego, Dept Elect & Comp Engn, La Jolla, CA 92093 USA. RP Sirbuly, DJ (reprint author), Univ Calif San Diego, Dept NanoEngn, La Jolla, CA 92093 USA. EM dsirbuly@ucsd.edu RI Wang, Yinmin (Morris)/F-2249-2010 OI Wang, Yinmin (Morris)/0000-0002-7161-2034 FU National Science Foundation (NSF) [1150952]; American Cancer Society (ACS) [70-002]; University of California, San Diego FX This work was supported by the National Science Foundation (NSF, contract no. 1150952), the American Cancer Society-Institutional Research Grant (ACS-IRG, contract no. 70-002), and the Hellman Fellowship at the University of California, San Diego. NR 32 TC 6 Z9 6 U1 1 U2 19 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2040-3364 J9 NANOSCALE JI Nanoscale PY 2013 VL 5 IS 2 BP 552 EP 555 DI 10.1039/c2nr32831c PG 4 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA 069HP UT WOS:000313426200015 PM 23232981 ER PT J AU Wang, CD Zhou, YA He, LF Ng, TW Hong, G Wu, QH Gao, F Lee, CS Zhang, WJ AF Wang, Chundong Zhou, Yungang He, Lifang Ng, Tsz-Wai Hong, Guo Wu, Qi-Hui Gao, Fei Lee, Chun-Sing Zhang, Wenjun TI In situ nitrogen-doped graphene grown from polydimethylsiloxane by plasma enhanced chemical vapor deposition SO NANOSCALE LA English DT Article ID FEW-LAYER GRAPHENE; LARGE-AREA; RAMAN-SPECTROSCOPY; CARBON NANOTUBES; SINGLE-LAYER; FILMS; GRAPHITE; CATALYST; DEFECTS; OXIDE AB Due to its unique electronic properties and wide spectrum of promising applications, graphene has attracted much attention from scientists in various fields. Control and engineering of graphene's semiconducting properties is considered to be key to its applications in electronic devices. Here, we report a novel method to prepare in situ nitrogen-doped graphene by microwave plasma assisted chemical vapor deposition (CVD) using PDMS (polydimethylsiloxane) as a solid carbon source. Based on this approach, the concentration of nitrogen-doping can be easily controlled via the flow rate of nitrogen during the CVD process. X-ray photoelectron spectroscopy results indicated that the nitrogen atoms doped into the graphene lattice were mainly in the forms of pyridinic and pyrrolic structures. Moreover, first-principles calculations show that the incorporated nitrogen atoms can lead to p-type doping of graphene. This in situ approach provides a promising strategy to prepare graphene with controlled electronic properties. C1 [Wang, Chundong; He, Lifang; Ng, Tsz-Wai; Hong, Guo; Wu, Qi-Hui; Lee, Chun-Sing; Zhang, Wenjun] City Univ Hong Kong, Dept Phys & Mat Sci, Ctr Super Diamond & Adv Films COSDAF, Hong Kong, Hong Kong, Peoples R China. [Zhou, Yungang] Univ Elect Sci & Technol China, Dept Appl Phys, Chengdu 610054, Peoples R China. [Zhou, Yungang; Gao, Fei] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Wu, QH (reprint author), City Univ Hong Kong, Dept Phys & Mat Sci, Ctr Super Diamond & Adv Films COSDAF, Hong Kong, Hong Kong, Peoples R China. EM qihuiwu@cityu.edu.hk; apwjzh@cityu.edu.hk RI Zhang, WJ/C-6995-2012; LEE, Chun-Sing/B-6254-2013; Wang, C.D. /D-5912-2012 OI Zhang, WJ/0000-0002-4497-0688; LEE, Chun-Sing/0000-0001-6557-453X; FU National Natural Science Foundation of China (NCFC) [61176007]; Research Grants Council of the Hong Kong Special Administrative Region, China [CityU 102010]; Division of Materials Sciences and Engineering, Office of Basic Energy Sciences, US Department of Energy [DE-AC05-76RL01830] FX This work was supported by National Natural Science Foundation of China (NCFC Grant 61176007) and Research Grants Council of the Hong Kong Special Administrative Region, China (Project no. CityU 102010). F. Gao would like to acknowledge the support from the Division of Materials Sciences and Engineering, Office of Basic Energy Sciences, US Department of Energy under Contract DE-AC05-76RL01830. NR 46 TC 46 Z9 46 U1 7 U2 165 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 2013 VL 5 IS 2 BP 600 EP 605 DI 10.1039/c2nr32897f PG 6 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA 069HP UT WOS:000313426200023 PM 23203220 ER PT J AU Silva, D Natalello, A Sanii, B Vasita, R Saracino, G Zuckermann, RN Doglia, SM Gelain, F AF Silva, Diego Natalello, Antonino Sanii, Babak Vasita, Rajesh Saracino, Gloria Zuckermann, Ronald N. Doglia, Silvia Maria Gelain, Fabrizio TI Synthesis and characterization of designed BMHP1-derived self-assembling peptides for tissue engineering applications SO NANOSCALE LA English DT Article ID TRANSFORM INFRARED-SPECTROSCOPY; X-RAY-DIFFRACTION; AMYLOID FIBRILS; AGGREGATION; HYDROGELS; PROTEINS; DIFFERENTIATION; NANOSTRUCTURES; NANOTUBES; SCAFFOLDS AB The importance of self-assembling peptides (SAPs) in regenerative medicine is becoming increasingly recognized. The propensity of SAPs to form nanostructured fibers is governed by multiple forces including hydrogen bonds, hydrophobic interactions and pi-pi aromatic interactions among side chains of the amino acids. Single residue modifications in SAP sequences can significantly affect these forces. BMHP1-derived SAPs is a class of biotinylated oligopeptides, which self-assemble in beta-structured fibers to form a self-healing hydrogel. In the current study, selected modifications in previously described BMHP1-derived SAPs were designed in order to investigate the influence of modified residues on self-assembly kinetics and scaffold formation properties. The Fourier transform infrared spectroscopy (FTIR) and X-ray diffraction (XRD) analysis demonstrated the secondary structure (beta-sheet) formation in all modified SAP sequences, whereas atomic force microscopy (AFM) analysis further confirmed the presence of nanofibers. Furthermore, the fiber shape and dimension analysis by AFM showed flattened and twisted fiber morphology ranging from similar to 8 nm to similar to 70 nm. The mechanical properties of the pre-assembled and post assembled solution were investigated by rheometry. The shear-thinning behavior and rapid re-healing properties of the pre-assembled solutions make them a preferable choice for injectable scaffolds. The wide range of stiffnesses (G') -from similar to 1000 to similar to 27 000 Pa - exhibited by the post-assembled scaffolds demonstrated their potential for a variety of tissue engineering applications. The extra cellular matrix (ECM) mimicking (physically and chemically) properties of SAP scaffolds enhanced cell adhesion and proliferation. The capability of the scaffold to facilitate murine neural stem cell (mNSC) proliferation was evaluated in vitro: the increased mNSCs adhesion and proliferation demonstrated the potential of newly synthesized SAPs for regenerative medicine approaches. C1 [Silva, Diego; Saracino, Gloria; Gelain, Fabrizio] AO Osped Niguarda Ca Granda, Ctr Nanomed & Tissue Engn, I-20162 Milan, Italy. [Silva, Diego; Natalello, Antonino; Saracino, Gloria; Doglia, Silvia Maria] Univ Milano Bicocca, Biotechnol & Biosci Dept, I-20126 Milan, Italy. [Vasita, Rajesh] IRCCS Casa Sollievo Sofferenza, Opera San Pio Pietrelcina, I-71013 San Giovanni Rotondo, Italy. [Natalello, Antonino; Doglia, Silvia Maria] UdR Milano Bicocca, Consorzio Nazl Interuniv Sci Fis Mat, I-20126 Milan, Italy. [Sanii, Babak; Zuckermann, Ronald N.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA. RP Gelain, F (reprint author), AO Osped Niguarda Ca Granda, Ctr Nanomed & Tissue Engn, Piazza Ospedalemaggiore 3, I-20162 Milan, Italy. EM fabrizio.gelain@unimib.it RI Gelain, Fabrizio/K-5069-2012; Zuckermann, Ronald/A-7606-2014; Natalello, Antonino/B-9659-2012; Foundry, Molecular/G-9968-2014 OI Gelain, Fabrizio/0000-0002-2624-5853; Zuckermann, Ronald/0000-0002-3055-8860; Natalello, Antonino/0000-0002-1489-272X; FU Fondazione Cariplo [2011-0352]; RegioneLombardia; Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231]; FIRB/MIUR from the Ministry of the University and Scientific Research of Italy [RBAP10KJC5, H41J10000090001] FX This work has been mainly supported by Fondazione Cariplo, grant no. 2011-0352, and RegioneLombardia. Work at the Molecular Foundry was supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under contract no. DE-AC02-05CH11231. A.N. acknowledges a post-doctoral fellowship FIRB/MIUR from the Ministry of the University and Scientific Research of Italy (RBAP10KJC5 - project code: H41J10000090001). We also gratefully thanks Bunzow D. A., Caprini A., Cigognini D., Coletti M., and Connolly M. for their helpful suggestions, discussions and criticism. NR 44 TC 17 Z9 17 U1 3 U2 89 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2040-3364 J9 NANOSCALE JI Nanoscale PY 2013 VL 5 IS 2 BP 704 EP 718 DI 10.1039/c2nr32656f PG 15 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA 069HP UT WOS:000313426200035 PM 23223865 ER PT J AU Liu, HR Yang, JH Zhang, YY Chen, SY Walsh, A Xiang, HJ Gong, XA Wei, SH AF Liu, Heng-Rui Yang, Ji-Hui Zhang, Yue-Yu Chen, Shiyou Walsh, Aron Xiang, Hongjun Gong, Xingao Wei, Su-Huai TI Prediction of (TiO2)(x)(Cu2O)(y) alloys for efficient photoelectrochemical water splitting SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID CRYSTAL-STRUCTURE PREDICTION; TITANIUM-DIOXIDE; SINGLE-CRYSTALS; PHOTOCATALYSIS; CU2O; SEMICONDUCTORS; ABSORPTION AB The formation of (TiO2)(x)(Cu2O)(y) solid-solutions is investigated using a global optimization evolutionary algorithm. First-principles calculations based on density functional theory are then used to gain insight into the electronic properties of these alloys. We find that: (i) Ti and Cu in (TiO2)(x)(Cu2O)(y) alloys have similar local environments as in bulk TiO2 and Cu2O except for (TiO2)(Cu2O) which has some trigonal-planar Cu ions. (ii) The predicted optical band gaps are around 2.1 eV (590 nm), thus having much better performance in the absorption of visible light compared with both binary oxides. (iii) (TiO2)(2)(Cu2O) has the lowest formation energy amongst all studied alloys and the positions of its band edges are found to be suitable for solar-driven water splitting applications. C1 [Liu, Heng-Rui; Yang, Ji-Hui; Zhang, Yue-Yu; Xiang, Hongjun; Gong, Xingao] Fudan Univ, Key Lab Computat Phys Sci, Minist Educ, State Key Lab Surface Phys, Shanghai 200433, Peoples R China. [Liu, Heng-Rui; Yang, Ji-Hui; Zhang, Yue-Yu; Xiang, Hongjun; Gong, Xingao] Fudan Univ, Dept Phys, Shanghai 200433, Peoples R China. [Chen, Shiyou] E China Normal Univ, Key Lab Polar Mat & Devices MOE, Shanghai 200241, Peoples R China. [Walsh, Aron] Univ Bath, Ctr Sustainable Chem Technol, Bath BA2 7AY, Avon, England. [Walsh, Aron] Univ Bath, Dept Chem, Bath BA2 7AY, Avon, England. [Wei, Su-Huai] Natl Renewable Energy Lab, Golden, CO 80401 USA. RP Xiang, HJ (reprint author), Fudan Univ, Key Lab Computat Phys Sci, Minist Educ, State Key Lab Surface Phys, Shanghai 200433, Peoples R China. EM hxiang@fudan.edu.cn; xggong@fudan.edu.cn; suhuai.wei@nrel.gov RI Walsh, Aron/A-7843-2008; Xiang, Hongjun/I-4305-2016 OI Walsh, Aron/0000-0001-5460-7033; Xiang, Hongjun/0000-0002-9396-3214 FU Special Funds for Major State Basic Research; National Science Foundation of China; Program for Professor of Special Appointment at Shanghai Institutions of Higher Learning; FANEDD, Ministry of Education; U.S. Department of Energy [DE-AC36-08GO28308]; Royal Society; Shanghai Municipality FX This work is partially supported by the Special Funds for Major State Basic Research, National Science Foundation of China, The Program for Professor of Special Appointment at Shanghai Institutions of Higher Learning, FANEDD, Ministry of Education and Shanghai Municipality. The calculations were performed in the Supercomputer Center of Fudan University. The work at NREL was supported by the U.S. Department of Energy under Contract No. DE-AC36-08GO28308. A. W. is supported by the Royal Society University Research Fellowship scheme. NR 38 TC 11 Z9 11 U1 4 U2 163 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2013 VL 15 IS 6 BP 1778 EP 1781 DI 10.1039/c2cp44484d PG 4 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 071DN UT WOS:000313566300005 PM 23258482 ER PT J AU Bera, PP Head-Gordon, M Lee, TJ AF Bera, Partha P. Head-Gordon, Martin Lee, Timothy J. TI Association mechanisms of unsaturated C2 hydrocarbons with their cations: acetylene and ethylene SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID CYCLOBUTADIENE RADICAL-CATION; POTENTIAL-ENERGY SURFACE; FOCK PERTURBATION-THEORY; COUPLED-CLUSTER; SPIN ORBITALS; CHEMISTRY; DIAGNOSTICS; COMPOUND; DENSITY; IONS AB The ion-molecule association mechanism of acetylene and ethylene with their cations is investigated by ab initio quantum chemical methods to understand the structures, association energies, and the vibrational and electronic spectra of the products. Stable puckered cyclic isomers are found as the result of first forming less stable linear and bridge isomers. The puckered cyclic complexes are calculated to be strongly bound, by 87, 35 and 56 kcal mol(-1) for acetylene-acetylene cation, ethylene-ethylene cation and acetylene-ethylene cation, respectively. These stable complexes may be intermediates that participate in further association reactions. There are no association barriers, and no significant inter-conversion barriers, so the initial linear and bridge encounter complexes are unlikely to be observable. However, the energy gap between the bridged and cyclic puckered isomers greatly differs from complex to complex: it is 44 kcal mol(-1) in C4H4+, but only 6 kcal mol(-1) in C4H8+. The accurate CCSD(T) calculations summarized above are also compared against less computationally expensive MP2 and density functional theory (DFT) calculations for structures, relative energies, and vibrational spectra. Calculated vibrational spectra are compared against available experiments for cyclobutadiene cation. Electronic spectra are also calculated using time-dependent DFT. C1 [Bera, Partha P.; Lee, Timothy J.] NASA, Ames Res Ctr, Mountain View, CA 94035 USA. [Head-Gordon, Martin] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Head-Gordon, Martin] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. RP Lee, TJ (reprint author), NASA, Ames Res Ctr, MS 245-1, Mountain View, CA 94035 USA. EM Timothy.J.Lee@nasa.gov RI Lee, Timothy/K-2838-2012; Bera, Partha /K-8677-2012 FU NASA [10-APRA10-167]; BAERI; NASA's laboratory astrophysics 'Carbon in the Galaxy' consortium grant [NNH10ZDA001N] FX PPB gratefully acknowledges a fellowship award from the NASA postdoctoral program administered by the Oak Ridge Associated Universities (ORAU) and BAERI for funding. PPB thanks Dr Julia Rice for sharing her expertise in optimizing transition states. The authors thank Big Apple Bagel, Pleasanton, CA for treating us well over our countless meetings. The authors gratefully acknowledge support from the NASA grant 10-APRA10-167 and support from NASA's laboratory astrophysics 'Carbon in the Galaxy' consortium grant (NNH10ZDA001N). NR 43 TC 11 Z9 11 U1 1 U2 28 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2013 VL 15 IS 6 BP 2012 EP 2023 DI 10.1039/c2cp43740f PG 12 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 071DN UT WOS:000313566300033 PM 23258256 ER PT J AU Sun, L Li, CL Xue, ZJ Simmons, BA Singh, S AF Sun, Lan Li, Chenlin Xue, Zhengjun Simmons, Blake A. Singh, Seema TI Unveiling high-resolution, tissue specific dynamic changes in corn stover during ionic liquid pretreatment SO RSC ADVANCES LA English DT Article ID SULFURIC-ACID PRETREATMENT; FIBER EXPANSION AFEX; ENZYMATIC-HYDROLYSIS; LIME PRETREATMENT; ORGANOSOLV PRETREATMENT; CELLULOSE DISSOLUTION; WHEAT-STRAW; POPLAR WOOD; DILUTE-ACID; BIOMASS AB Confocal Raman microscopy and confocal fluorescence microscopy were used to understand the mechanism of ionic liquid (IL) pretreatment of corn stover stem using 1-ethyl-3-methylimidazolium acetate. Three different cell types including tracheids, sclerenchyma cells and parenchyma cells were analyzed during IL pretreatment. We have established a direct correlation between changes in both the morphology and chemical composition of these plant cell walls during IL pretreatment as well as specific cell type information. It was observed that cell wall swelling occurs primarily in the secondary plant cell walls and the IL had little effect on compound middle lamella in terms of swelling. Accordingly, more significant cell wall swelling and distortion was observed in sclerenchyma cells and tracheids than in parenchyma cells, which contain primary plant cell walls. Lignin dissolution was faster in the secondary cell walls, while there was no preferential cellulose dissolution. Surprisingly, with a much thicker cell wall and a much higher original lignin content than parenchyma cells, tracheids showed much faster lignin and cellulose dissolution and cell wall swelling. Sclerenchyma cells showed an intermediate rate of lignin dissolution, while the cellulose dissolution rate and degree of cell wall swelling was comparable to that observed for tracheids. These results suggest that there is a synergistic mechanism of lignocellulose dissolution regarding cellulose and lignin dissolution and cell wall swelling that occurs during IL pretreatment. This study provides valuable new insights towards the mechanism of ionic liquid pretreatment and can potentially assist researchers in cell wall engineering for efficient cell wall deconstruction using ILs, and the methods established can be easily extended to other systems. C1 [Sun, Lan; Li, Chenlin; Simmons, Blake A.; Singh, Seema] Lawrence Berkeley Natl Lab, Phys Biosci Div, Joint BioEnergy Inst, Emeryville, CA 94608 USA. [Sun, Lan; Li, Chenlin; Simmons, Blake A.; Singh, Seema] Sandia Natl Labs, Biomass Sci & Convers Technol Dept, Livermore, CA 94551 USA. [Xue, Zhengjun] Univ Calif Davis, Dept Biol & Agr Engn, Davis, CA 95616 USA. RP Sun, L (reprint author), Lawrence Berkeley Natl Lab, Phys Biosci Div, Joint BioEnergy Inst, 5885 Hollis St, Emeryville, CA 94608 USA. EM seesing@sandia.gov RI Sun, Lan/C-7321-2012; OI Li, Chenlin/0000-0002-0793-0505; Simmons, Blake/0000-0002-1332-1810 FU Office of Science, Office of Biological and Environmental Research, of the US Department of Energy [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 US Department of Energy under Contract No. DE-AC02-05CH11231. NR 38 TC 21 Z9 24 U1 3 U2 58 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2046-2069 J9 RSC ADV JI RSC Adv. PY 2013 VL 3 IS 6 BP 2017 EP 2027 DI 10.1039/c2ra20706k PG 11 WC Chemistry, Multidisciplinary SC Chemistry GA 070MZ UT WOS:000313513400059 ER PT J AU Kim, J Tsouris, C Mayes, RT Oyola, Y Saito, T Janke, CJ Dai, S Schneider, E Sachde, D AF Kim, Jungseung Tsouris, Costas Mayes, Richard T. Oyola, Yatsandra Saito, Tomonori Janke, Christopher J. Dai, Sheng Schneider, Erich Sachde, Darshan TI Recovery of Uranium from Seawater: A Review of Current Status and Future Research Needs SO SEPARATION SCIENCE AND TECHNOLOGY LA English DT Article DE uranium adsorbents; uranium adsorption; uranium from seawater ID INDUCED GRAFT-POLYMERIZATION; HYDROUS TITANIUM(IV) OXIDE; MACRORETICULAR CHELATING RESIN; AMIDOXIME-FIBER ADSORBENTS; MESOPOROUS CARBON MATERIALS; SOLID-PHASE EXTRACTION; SEA-WATER; ACTIVATED CARBON; METAL-IONS; URANYL IONS AB The recovery of uranium (U) from seawater has been investigated for over six decades in efforts to secure uranium sources for future energy production. The majority of the research activities have focused on inorganic materials, chelating polymers, and nanomaterials. Previous studies of uranium adsorption from aqueous solutions, mainly seawater, are reviewed here with a focus on various adsorbent materials, adsorption parameters, adsorption characterization, and marine studies. Continuous progress has been made over several decades, with adsorbent loadings approaching 3.2 mg U/g adsorbent in equilibrium with seawater. Further research is needed to improve first, the viability including improved capacity, selectivity, and kinetics, and second, the sorbent regeneration for multicycle use. An overview of the status of the uranium adsorption technology is provided and future research needs to make this technology commercially competitive are discussed. C1 [Kim, Jungseung; Tsouris, Costas; Mayes, Richard T.; Oyola, Yatsandra; Saito, Tomonori; Janke, Christopher J.; Dai, Sheng] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. [Schneider, Erich; Sachde, Darshan] Univ Texas Austin, Nucl & Radiat Engn Program, Austin, TX 78712 USA. RP Tsouris, C (reprint author), Oak Ridge Natl Lab, POB 2008, Oak Ridge, TN 37831 USA. EM tsourisc@ornl.gov RI Tsouris, Costas/C-2544-2016; Saito, Tomonori/M-1735-2016; Dai, Sheng/K-8411-2015; Mayes, Richard/G-1499-2016; Janke, Christopher/E-1598-2017 OI Tsouris, Costas/0000-0002-0522-1027; Saito, Tomonori/0000-0002-4536-7530; Dai, Sheng/0000-0002-8046-3931; Mayes, Richard/0000-0002-7457-3261; Janke, Christopher/0000-0002-6076-7188 FU U.S. DOE Office of Nuclear Energy [DE-AC05-00OR22725]; Oak Ridge National Laboratory FX This research was conducted at the Oak Ridge National Laboratory and supported by the U.S. DOE Office of Nuclear Energy, under Contract DE-AC05-00OR22725 with Oak Ridge National Laboratory, managed by UT-Battelle, LLC. Comments by David W. DePaoli are gratefully acknowledged. NR 232 TC 109 Z9 114 U1 26 U2 258 PU TAYLOR & FRANCIS INC PI PHILADELPHIA PA 530 WALNUT STREET, STE 850, PHILADELPHIA, PA 19106 USA SN 0149-6395 EI 1520-5754 J9 SEP SCI TECHNOL JI Sep. Sci. Technol. PD JAN 1 PY 2013 VL 48 IS 3 BP 367 EP 387 DI 10.1080/01496395.2012.712599 PG 21 WC Chemistry, Multidisciplinary; Engineering, Chemical SC Chemistry; Engineering GA 072OF UT WOS:000313681000001 ER PT J AU Ramirez-Hernandez, A Muller, M de Pablo, JJ AF Ramirez-Hernandez, Abelardo Mueller, Marcus de Pablo, Juan J. TI Theoretically informed entangled polymer simulations: linear and non-linear rheology of melts SO SOFT MATTER LA English DT Article ID MOLECULAR-WEIGHT DISTRIBUTION; CHAIN NETWORK MODEL; SLIP-LINK MODEL; BLOCK-COPOLYMERS; NANOPATTERNED SURFACES; DIFFUSION; PREDICTIONS; MECHANISMS; REPTATION; VISCOSITY AB In recent years, there has been a resurgence in developing models and theories for the non-equilibrium behavior of polymeric liquids. The so-called "tube" models, gradually refined over decades of research, can now provide a description of the linear and non-linear rheology of entangled polymers that is qualitatively consistent with experiments. Such approaches, however, have been limited to homopolymers. Here we present a general formalism that relies on the concept of slip links to describe the dynamics of high polymers. In this work, it is shown to be capable of describing quantitatively the linear response of pure homopolymers and blends, the non-linear rheology of highly entangled systems, and the dynamics of diblock copolymers. C1 [Ramirez-Hernandez, Abelardo; de Pablo, Juan J.] Univ Chicago, Inst Mol Engn, Chicago, IL 60637 USA. [Ramirez-Hernandez, Abelardo; de Pablo, Juan J.] Argonne Natl Lab, Argonne, IL 60439 USA. [Mueller, Marcus] Univ Gottingen, Inst Theoret Phys, D-37077 Gottingen, Germany. RP de Pablo, JJ (reprint author), Univ Chicago, Inst Mol Engn, 5747 S Ellis Ave, Chicago, IL 60637 USA. EM depablo@uchicago.edu RI Ramirez-Hernandez, Abelardo/A-1717-2011; Muller, Marcus/B-9898-2009 OI Ramirez-Hernandez, Abelardo/0000-0002-3569-5223; Muller, Marcus/0000-0002-7472-973X FU National Science Foundation through the Nanoscale Science and Engineering Center at the University of Wisconsin [DMR-0832760]; Semiconductor Research Corporation; Office of Naval Research through MURI Award [N00014-11-1-0690] FX The authors are grateful to Veronica Chappa and David Morse for helpful discussions. This work is supported by the National Science Foundation through the Nanoscale Science and Engineering Center at the University of Wisconsin under Grant no. DMR-0832760, by the Semiconductor Research Corporation, and by the Office of Naval Research through MURI Award N00014-11-1-0690. NR 39 TC 16 Z9 16 U1 4 U2 58 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 2013 VL 9 IS 6 BP 2030 EP 2036 DI 10.1039/c2sm26674a PG 7 WC Chemistry, Physical; Materials Science, Multidisciplinary; Physics, Multidisciplinary; Polymer Science SC Chemistry; Materials Science; Physics; Polymer Science GA 071LM UT WOS:000313594200035 ER PT J AU Lim, SHN Isidorsson, J Sun, LZ Kwak, BL Anders, A AF Lim, Sunnie H. N. Isidorsson, Jan Sun, Lizhong Kwak, B. Leo Anders, Andre TI Modeling of optical and energy performance of tungsten-oxide-based electrochromic windows including their intermediate states SO SOLAR ENERGY MATERIALS AND SOLAR CELLS LA English DT Article DE Electrochromic windows; Smart windows; Energy simulation; Energy efficient window modeling ID ELECTRICAL-PROPERTIES; THIN-FILMS; EMISSIVITY; COATINGS; LITHIUM; INDEXES AB Tungsten-oxide-based electrochromic (EC) windows are currently the most robust and matured dynamic windows where the transmittance of visual light and near-infrared radiation can be controlled by a small applied voltage. In its standard application, the window is commonly either in its clear or colored state. In this contribution, we study the optical and energy performance of such window in the fully bleached and fully colored state as well as when it is kept in intermediate states. Different configurations in terms of placement of the EC layer stack and possible additional low-emissivity (low-E) coating within the insulated glass unit are considered. Using optical data and software tools we find that even a small coloration has a significant effect on the energy performance because the solar heat gain coefficient is readily reduced by the absorption of the EC layer stack. We compare the performance of the EC windows to commercially available solar-control (spectrally selective) low-E windows. (C) 2012 Elsevier B.V. All rights reserved. C1 [Lim, Sunnie H. N.; Anders, Andre] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Isidorsson, Jan; Sun, Lizhong; Kwak, B. Leo] Appl Mat Inc, Santa Clara, CA 95054 USA. RP Anders, A (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. EM aanders@lbl.gov RI Anders, Andre/B-8580-2009 OI Anders, Andre/0000-0002-5313-6505 FU Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Building Technology, of the US Department of Energy [DE-AC02-05CH11231]; American Reconstruction and Reinvestment Act [DE-EE0003838] FX We thank Steve Selkowitz, Christian Kohler, and Rueben Mendelsberg (all LBNL) for insightful discussions. This work was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Building Technology, of the US Department of Energy under Contract no. DE-AC02-05CH11231, and by the American Reconstruction and Reinvestment Act, under Contract DE-EE0003838. NR 20 TC 10 Z9 11 U1 3 U2 52 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0927-0248 J9 SOL ENERG MAT SOL C JI Sol. Energy Mater. Sol. Cells PD JAN PY 2013 VL 108 BP 129 EP 135 DI 10.1016/j.solmat.2012.09.010 PG 7 WC Energy & Fuels; Materials Science, Multidisciplinary; Physics, Applied SC Energy & Fuels; Materials Science; Physics GA 071PX UT WOS:000313607800020 ER PT J AU Xie, H Lu, JL Shekhar, M Elam, JW Delgass, WN Ribeiro, FH Weitz, E Poeppelmeier, KR AF Xie, Hong Lu, Junling Shekhar, Mayank Elam, Jeffery W. Delgass, W. Nicholas Ribeiro, Fabio H. Weitz, Eric Poeppelmeier, Kenneth R. TI Synthesis of Na-Stabilized Nonporous t-ZrO2 Supports and Pt/t-ZrO2 Catalysts and Application to Water-Gas-Shift Reaction SO ACS CATALYSIS LA English DT Article DE tetragonal ZrO2; hydrothermal synthesis; Na; Pt/ZrO2; water-gas-shift reaction ID ATOMIC LAYER DEPOSITION; HYDROTHERMAL CONDITIONS; TETRAGONAL PHASE; BUTANE ISOMERIZATION; ZIRCONIA POLYMORPHS; ZRO2; CRYSTALLIZATION; NANOPARTICLES; TEMPERATURE; METHANE AB t-ZrO2, synthesized under hydrothermal treatment conditions at 150 degrees C for 20 h using NaOH as the mineralizer, was phase stable up to 600 degrees C in air. The t-ZrO2 calcined at 600 degrees C (denoted as Z600) were nonporous spherical nanocrystallites with an average size of similar to 12 nm and a surface area of similar to 55 m(2)/g, which exhibited hydrothermal stability in a wide range of pH environments from acidic to basic conditions at 200 degrees C for 20 h. Monodispersed platinum nanoparticles similar to 1.5 +/- 0.3 nm were obtained on the Z600 supported Pt/t-ZrO2 catalyst by the Pt atomic layer deposition (AID) method. Na ions were found to play a crucial role in the formation of the stable t-ZrO2 by incorporating into the internal crystal structure of ZrO2 during the hydrothermal synthesis. The rate of water-gas-shift (WGS) reaction per mole of surface Pt on the Pt/Z600 catalyst was about five times higher compared to the catalysts prepared on commercial nonporous ZrO2. The incorporation of Na into the t-ZrO2 structure had a synergistic effect: stabilizing ZrO2 in the tetragonal phase and promoting the WGS reaction. C1 [Xie, Hong; Weitz, Eric; Poeppelmeier, Kenneth R.] Northwestern Univ, Dept Chem, Ctr Catalysis & Surface Sci, Evanston, IL 60208 USA. [Lu, Junling; Elam, Jeffery W.] Argonne Natl Lab, Div Energy Syst, Argonne, IL 60439 USA. [Shekhar, Mayank; Delgass, W. Nicholas; Ribeiro, Fabio H.] Purdue Univ, Sch Chem Engn, W Lafayette, IN 47907 USA. RP Poeppelmeier, KR (reprint author), Northwestern Univ, Dept Chem, Ctr Catalysis & Surface Sci, 2145 Sheridan Rd, Evanston, IL 60208 USA. EM krp@northwestern.edu RI Lu, Junling/F-3791-2010 OI Lu, Junling/0000-0002-7371-8414 FU Institute for Atom-efficient Chemical Transformations (IACT), an Energy Frontier Research Center; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences FX This material is based upon work supported as part of the Institute for Atom-efficient Chemical Transformations (IACT), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences. We thank Mr. Yuyuan Lin for helping with HRTEM images. NR 47 TC 23 Z9 24 U1 5 U2 115 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 2155-5435 J9 ACS CATAL JI ACS Catal. PD JAN PY 2013 VL 3 IS 1 BP 61 EP 73 DI 10.1021/cs300596q PG 13 WC Chemistry, Physical SC Chemistry GA 066KX UT WOS:000313220800012 ER PT J AU Lin, JD Aloni, S Altoe, V Webb, SM Ryder, MI Ho, SP AF Lin, J. D. Aloni, S. Altoe, V. Webb, S. M. Ryder, M. I. Ho, S. P. TI Elastic discontinuity due to ectopic calcification in a human fibrous joint SO ACTA BIOMATERIALIA LA English DT Article DE Ectopic calcification; Elastic discontinuity; Structure; Chemical composition; Cementum ID NANO-MECHANICAL PROPERTIES; CEMENTUM-DENTIN JUNCTION; ELECTRON-MICROSCOPY; NANOMECHANICAL PROPERTIES; PERIODONTAL-LIGAMENT; COLLAGEN FIBRILS; ENAMEL JUNCTION; CALCULUS; TISSUE; BONE AB Disease can alter natural ramp-like elastic gradients to steeper step-like profiles at soft-hard tissue interfaces. Prolonged function can further mediate mechanochemical events that alter biomechanical response within diseased organs. In this study, a human bone-tooth fibrous joint was chosen as a model system, in which the effects of bacterial-induced disease, i.e. periodontitis, on natural elastic gradients were investigated. Specifically, the effects of ectopic biomineral, i.e. calculus, on innate chemical and elastic gradients within the cementum-dentin complex, both of which are fundamental parameters to load-bearing tissues, are investigated through comparisons with a healthy complex. Complementary techniques for mapping changes in physicochemical properties as a result of disease included micro X-ray computed tomography, microprobe micro X-ray fluorescence imaging, transmission electron and atomic force microscopy (AFM) techniques, and AFM-based nanoindentation. Results demonstrated primary effects as derivatives of ectopic mineralization within the diseased fibrous joint. Ectopic mineralization with no cementum resorption, but altered cementum physicochemical properties with increasing X-ray attenuation, exhibited stratified concretion with increasing X-ray fluorescence counts of calcium and phosphorus elements in the extracellular matrix in correlation with decreased hygroscopicity, indenter displacement, and apparent strain-relieving characteristics. Disease progression, identified as concretion through the periodontal ligament (PDL)-cementum enthesis, and sometimes the originally hygroscopic cementum-dentin junction, resulted in a significantly increased indentation elastic modulus (3.16 +/- 1.19 GPa) and a shift towards a discontinuous interface compared with healthy conditions (1.54 +/- 0.83 GPa) (Student's t-test, P < 0.05). The observed primary effects could result in secondary downstream effects, such as compromised mechanobiology at the mechanically active PDL-cementum enthesis that can catalyze progression of disease. Published by Elsevier Ltd. on behalf of Acta Materialia Inc. C1 [Lin, J. D.; Ho, S. P.] Univ Calif San Francisco, Dept Prevent & Restorat Dent Sci, Div Biomat & Bioengn, San Francisco, CA 94143 USA. [Aloni, S.; Altoe, V.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA. [Webb, S. M.] SLAC Natl Accelerator Lab, Stanford Synchrotron Radiat Lightsource, Menlo Pk, CA USA. [Ryder, M. I.] Univ Calif San Francisco, Dept Orofacial Sci, San Francisco, CA 94143 USA. RP Ho, SP (reprint author), Univ Calif San Francisco, Dept Prevent & Restorat Dent Sci, Div Biomat & Bioengn, San Francisco, CA 94143 USA. EM sunita.ho@ucsf.edu RI Webb, Samuel/D-4778-2009; Foundry, Molecular/G-9968-2014; OI Webb, Samuel/0000-0003-1188-0464; Ho, Sunita/0000-0001-9999-8226 FU Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231]; NIH/NIDCR [R00DE018212, NIH/NIDCR-R01DE022032, T32 DE07306]; NIH/NCRR [S10RR026645]; Department of Preventive and Restorative Dental Sciences, UCSF; Department of Orofacial Sciences, UCSF FX The authors thank Dr. Jim De Yoreo, Molecular Foundry, LBNL, CA, and Dr. Arthur Veis, Northwestern University Medical School, IL, for the many insightful discussions. Microprobe mu-XRF imaging was performed at the Stanford Synchrotron Radiation Lightsource (SSRL), SLAC National Accelerator Laboratory, Stanford University, CA. The authors also thank Lawrence Berkeley National Laboratories, for the use of SEM and BSE, and Dr. Peter Sargent, PhD, Department of Cell and Tissue Biology, UCSF, for the use of the ultramicrotome. Work at the Molecular Foundry was supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. Support was provided by NIH/NIDCR R00DE018212, NIH/NIDCR-R01DE022032, NIH/NIDCR T32 DE07306, NIH/NCRR S10RR026645, and Departments of Preventive and Restorative Dental Sciences and Orofacial Sciences, UCSF. NR 70 TC 3 Z9 3 U1 0 U2 16 PU ELSEVIER SCI LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, OXON, ENGLAND SN 1742-7061 J9 ACTA BIOMATER JI Acta Biomater. PD JAN PY 2013 VL 9 IS 1 BP 4787 EP 4795 DI 10.1016/j.actbio.2012.08.021 PG 9 WC Engineering, Biomedical; Materials Science, Biomaterials SC Engineering; Materials Science GA 068OV UT WOS:000313376900035 PM 22917805 ER PT J AU Liu, X Rahaman, MN Fu, Q AF Liu, Xin Rahaman, Mohamed N. Fu, Qiang TI Bone regeneration in strong porous bioactive glass (13-93) scaffolds with an oriented microstructure implanted in rat calvarial defects SO ACTA BIOMATERIALIA LA English DT Article DE Bone regeneration; Bioactive glass scaffold; Rat calvarial defect model; Mineralization; Mechanical response ID CAMPHENE-BASED SUSPENSIONS; MECHANICAL-PROPERTIES; CERAMIC SCAFFOLDS; HYDROXYAPATITE; SIZE; OSTEOGENESIS; SILICATE; STRENGTH; POROSITY; INGROWTH AB There is a need for synthetic bone graft substitutes to repair large bone defects resulting from trauma, malignancy and congenital diseases. Bioactive glass has attractive properties as a scaffold material but factors that influence its ability to regenerate bone in vivo are not well understood. In the present work, the ability of strong porous scaffolds of 13-93 bioactive glass with an oriented microstructure to regenerate bone was evaluated in vivo using a rat calvarial defect model. Scaffolds with an oriented microstructure of columnar pores (porosity = 50%; pore diameter = 50-150 mu m) showed mostly osteoconductive bone regeneration, and new bone formation, normalized to the available pore area (volume) of the scaffolds, increased from 37% at 12 weeks to 55% at 24 weeks. Scaffolds of the same glass with a trabecular microstructure (porosity = 80%; pore width = 100-500 mu m), used as the positive control, showed bone regeneration in the pores of 25% and 46% at 12 and 24 weeks, respectively. The brittle mechanical response of the as-fabricated scaffolds changed markedly to an elastoplastic response in vivo at both implantation times. These results indicate that both groups of 13-93 bioactive glass scaffolds could potentially be used to repair large bone defects, but scaffolds with the oriented microstructure could also be considered for the repair of loaded bone. (C) 2012 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved. C1 [Liu, Xin; Rahaman, Mohamed N.] Missouri Univ Sci & Technol, Dept Mat Sci & Engn, Ctr Bone & Tissue Repair & Regenerat, Rolla, MO 65409 USA. [Fu, Qiang] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. RP Rahaman, MN (reprint author), Missouri Univ Sci & Technol, Dept Mat Sci & Engn, Ctr Bone & Tissue Repair & Regenerat, Rolla, MO 65409 USA. EM rahaman@mst.edu FU National Institutes of Health, National Institute of Arthritis, Musculoskeletal and Skin Diseases (NIAMS) [1R15AR056119-01]; US Army Medical Research Acquisition Activity [W81XWH-08-1-0765] FX This work was supported by the National Institutes of Health, National Institute of Arthritis, Musculoskeletal and Skin Diseases (NIAMS), Grant No. 1R15AR056119-01, and by the US Army Medical Research Acquisition Activity, under Contract No. W81XWH-08-1-0765. The authors would like to thank Mo-Sci Corp., Rolla, MO for the bioactive glass used in this work, Dr. R.F. Brown for assistance with animal surgeries, and the Advanced Light Source, Lawrence Berkeley National Lab, for use of the dedicated X-ray tomography beamline. NR 45 TC 37 Z9 40 U1 2 U2 25 PU ELSEVIER SCI LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, OXON, ENGLAND SN 1742-7061 J9 ACTA BIOMATER JI Acta Biomater. PD JAN PY 2013 VL 9 IS 1 BP 4889 EP 4898 DI 10.1016/j.actbio.2012.08.029 PG 10 WC Engineering, Biomedical; Materials Science, Biomaterials SC Engineering; Materials Science GA 068OV UT WOS:000313376900045 PM 22922251 ER PT J AU Badger, J Chie-Leon, B Logan, C Sridhar, V Sankaran, B Zwart, PH Nienaber, V AF Badger, John Chie-Leon, Barbara Logan, Cheyenne Sridhar, Vandana Sankaran, Banumathi Zwart, Peter H. Nienaber, Vicki TI Structure determination of LpxD from the lipopolysaccharide-synthesis pathway of Acinetobacter baumannii SO ACTA CRYSTALLOGRAPHICA SECTION F-STRUCTURAL BIOLOGY AND CRYSTALLIZATION COMMUNICATIONS LA English DT Article AB Acinetobacter baumannii is a Gram-negative bacterium that is resistant to many currently available antibiotics. The protein LpxD is a component of the biosynthetic pathway for lipopolysaccharides in the outer membrane of this bacterium and is a potential target for new antibacterial agents. This paper describes the structure determination of apo forms of LpxD in space groups P2(1) and P4(3)22. These crystals contained six and three copies of the protein molecule in the asymmetric unit and diffracted to 2.8 and 2.7 angstrom resolution, respectively. A comparison of the multiple protein copies in the asymmetric units of these crystals reveals a common protein conformation and a conformation in which the relative orientation between the two major domains in the protein is altered. C1 [Badger, John; Chie-Leon, Barbara; Logan, Cheyenne; Sridhar, Vandana; Nienaber, Vicki] Zenobia Therapeut Inc, La Jolla, CA 92037 USA. [Sankaran, Banumathi; Zwart, Peter H.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley Ctr Struct Biol, Phys Biosci Div, Berkeley, CA 94720 USA. RP Badger, J (reprint author), Zenobia Therapeut Inc, 505 Coast Blvd S,Suite 111, La Jolla, CA 92037 USA. EM john@zenobiatherapeutics.com FU National Institutes of Health, National Institute of General Medical Sciences; Howard Hughes Medical Institute; Office of Basic Energy Sciences of the US Department of Energy [DE-AC02-05CH11231] FX The Berkeley Center for Structural Biology is supported in part by the National Institutes of Health, National Institute of General Medical Sciences and the Howard Hughes Medical Institute. The Advanced Light Source is supported by the Director, Office of Basic Energy Sciences of the US Department of Energy under Contract No. DE-AC02-05CH11231. We thank Rick Walter and Gina Ranieri (Shamrock Structures) for data collection at the Advanced Photon Source. NR 10 TC 4 Z9 4 U1 0 U2 4 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 1744-3091 J9 ACTA CRYSTALLOGR F JI Acta Crystallogr. F-Struct. Biol. Cryst. Commun. PD JAN PY 2013 VL 69 BP 6 EP 9 DI 10.1107/S1744309112048890 PN 1 PG 4 WC Biochemical Research Methods; Biochemistry & Molecular Biology; Biophysics; Crystallography SC Biochemistry & Molecular Biology; Biophysics; Crystallography GA 064EO UT WOS:000313055000003 PM 23295477 ER PT J AU Palani, K Burley, SK Swaminathan, S AF Palani, Kandavelu Burley, Stephen K. Swaminathan, Subramanyam TI Structure of alanine racemase from Oenococcus oeni with bound pyridoxal 5 '-phosphate SO ACTA CRYSTALLOGRAPHICA SECTION F-STRUCTURAL BIOLOGY AND CRYSTALLIZATION COMMUNICATIONS LA English DT Article ID BACILLUS-STEAROTHERMOPHILUS; DRUG DESIGN; CYCLOSERINE; MECHANISM; PRODUCT; ENZYME; MUTANT; BINDS AB The crystal structure of alanine racemase from Oenococcus oeni has been determined at 1.7 angstrom resolution using the single-wavelength anomalous dispersion (SAD) method and selenium-labelled protein. The protein exists as a symmetric dimer in the crystal, with both protomers contributing to the two active sites. Pyridoxal 5'-phosphate, a cofactor, is bound to each monomer and forms a Schiff base with Lys39. Structural comparison of alanine racemase from O. oeni (Alr) with homologous family members revealed similar domain organization and cofactor binding. C1 [Palani, Kandavelu; Swaminathan, Subramanyam] Brookhaven Natl Lab, Dept Biol, Upton, NY 11973 USA. [Burley, Stephen K.] Eli Lilly & Co, San Diego, CA 92121 USA. RP Swaminathan, S (reprint author), Brookhaven Natl Lab, Dept Biol, Upton, NY 11973 USA. EM swami@bnl.gov FU National Institute of General Medical Sciences under DOE [GM074945, DEAC02-98CH10886]; Brookhaven National Laboratory FX This research was supported by a U54 award from the National Institute of General Medical Sciences to the NYSGXRC (GM074945; PI SKB) under DOE Prime Contract No. DEAC02-98CH10886 with Brookhaven National Laboratory. We gratefully acknowledge data-collection support from beamline X12C at the National Synchrotron Light Source. NR 30 TC 2 Z9 3 U1 0 U2 18 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 1744-3091 J9 ACTA CRYSTALLOGR F JI Acta Crystallogr. F-Struct. Biol. Cryst. Commun. PD JAN PY 2013 VL 69 BP 15 EP 19 DI 10.1107/S1744309112047276 PN 1 PG 5 WC Biochemical Research Methods; Biochemistry & Molecular Biology; Biophysics; Crystallography SC Biochemistry & Molecular Biology; Biophysics; Crystallography GA 064EO UT WOS:000313055000005 PM 23295479 ER PT J AU Xiao, HY Zhang, Y Weber, WJ AF Xiao, H. Y. Zhang, Y. Weber, W. J. TI Thermodynamic properties of CexTh1-xO2 solid solution from first-principles calculations SO ACTA MATERIALIA LA English DT Article DE CeO2-ThO2 solid solution; Thermal expansion; Thermal conductivity; Ab initio lattice dynamics ID LATTICE THERMAL-EXPANSION; GROUND-STATE PROPERTIES; HEAT-CAPACITIES; THORIA-URANIA; CONDUCTIVITY; THO2; CEO2; IRRADIATION; DYNAMICS; FLUORITE AB A systematic study based on first-principles calculations along with a quasi-harmonic approximation has been conducted to calculate the thermodynamic properties of the CexTh1-xO2 solid solution. The predicted density, thermal expansion coefficients, heat capacity and thermal conductivity for the CexTh1-xO2 solid solution all agree well with the available experimental data. The thermal expansion coefficient for ThO2 increases with CeO2 substitution, and complete substitution shows the highest expansion coefficient. On the other hand, the mixed CexTh1-xO2 (0 < x < 1) solid solution generally exhibits lower heat capacity and thermal conductivity than the ThO2 and CeO2 end members. Our calculations indicate a strong effect of Ce concentration on the thermodynamic properties of the CexTh1-xO2 solid solution. (c) 2012 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved. C1 [Xiao, H. Y.; Zhang, Y.; Weber, W. J.] Univ Tennessee, Dept Mat Sci & Engn, Knoxville, TN 37996 USA. [Zhang, Y.; Weber, W. J.] Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. RP Xiao, HY (reprint author), Univ Tennessee, Dept Mat Sci & Engn, Knoxville, TN 37996 USA. EM hxiao@utk.edu RI Weber, William/A-4177-2008 OI Weber, William/0000-0002-9017-7365 FU Materials Science of Actinides, an Energy Frontier Research Center; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences 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. The theoretical calculations were performed using the supercomputer resources at the Environmental Molecular Sciences Laboratory located at the Pacific Northwest National Laboratory, and the National Energy Research Scientific Computing Center located at the Lawrence Berkeley National Laboratory. NR 80 TC 19 Z9 19 U1 3 U2 63 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 1359-6454 EI 1873-2453 J9 ACTA MATER JI Acta Mater. PD JAN PY 2013 VL 61 IS 2 BP 467 EP 476 DI 10.1016/j.actamat.2012.09.050 PG 10 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Materials Science; Metallurgy & Metallurgical Engineering GA 068VI UT WOS:000313393900005 ER PT J AU Yu, LP Kokenyesi, RS Keszler, DA Zunger, A AF Yu, Liping Kokenyesi, Robert S. Keszler, Douglas A. Zunger, Alex TI Inverse Design of High Absorption Thin-Film Photovoltaic Materials SO ADVANCED ENERGY MATERIALS LA English DT Article DE hotovoltaic absorber; tandem solar cells; photovoltaics; thin film; chalcogenide semiconductor ID AUGMENTED-WAVE METHOD; SOLAR-CELLS; DEPOSITION; ENERGY C1 [Yu, Liping; Zunger, Alex] Univ Colorado, Boulder, CO 80309 USA. [Kokenyesi, Robert S.; Keszler, Douglas A.] Oregon State Univ, Dept Chem, Corvallis, OR 97331 USA. [Yu, Liping] Natl Renewable Energy Lab, Golden, CO 80401 USA. RP Yu, LP (reprint author), Univ Colorado, Boulder, CO 80309 USA. EM yuliping@gmail.com RI Yu, Liping/B-4640-2008; OI Keszler, Douglas/0000-0002-7112-1171 FU U.S. DOE, Office of Science, Energy Frontier Research Centers; U.S. DOE EERE [DEAC36-08GO28308] FX This work was supported by U.S. DOE, Office of Science, Energy Frontier Research Centers, and used capabilities of the NREL Computational Sciences Center supported by U.S. DOE EERE, under Grant No. DEAC36-08GO28308 to NREL. The "Center for Inverse Design" is a DOE Energy Frontier Research Center. NR 31 TC 72 Z9 72 U1 12 U2 156 PU WILEY-V C H VERLAG GMBH PI WEINHEIM PA BOSCHSTRASSE 12, D-69469 WEINHEIM, GERMANY SN 1614-6832 J9 ADV ENERGY MATER JI Adv. Energy Mater. PD JAN PY 2013 VL 3 IS 1 BP 43 EP 48 DI 10.1002/aenm.201200538 PG 6 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary; Physics, Applied; Physics, Condensed Matter SC Chemistry; Energy & Fuels; Materials Science; Physics GA 066SD UT WOS:000313239600006 ER PT J AU Fang, Y Pandey, AK Nardes, AM Kopidakis, N Burn, PL Meredith, P AF Fang, Yuan Pandey, Ajay K. Nardes, Alexandre M. Kopidakis, Nikos Burn, Paul L. Meredith, Paul TI A Narrow Optical Gap Small Molecule Acceptor for Organic Solar Cells SO ADVANCED ENERGY MATERIALS LA English DT Article DE photoexcited hole transfer; narrow optical gap acceptors; non-fullerene acceptors; organic solar cells; time resolved microwave conductivity ID PHOTOVOLTAIC APPLICATIONS; SEMICONDUCTING POLYMERS; CONJUGATED POLYMERS; HIGH-PERFORMANCE; CHARGE; HETEROJUNCTIONS; GENERATION; FILMS; YIELD C1 [Fang, Yuan; Pandey, Ajay K.; Burn, Paul L.; Meredith, Paul] Univ Queensland, Ctr Organ Photon & Elect, Brisbane, Qld 4072, Australia. [Nardes, Alexandre M.; Kopidakis, Nikos] Natl Renewable Energy Lab, Golden, CO 80401 USA. RP Pandey, AK (reprint author), Univ Queensland, Ctr Organ Photon & Elect, Brisbane, Qld 4072, Australia. EM a.pandey@uq.edu.au; p.burn2@uq.edu.au; meredith@physics.uq.edu.au RI Pandey, Ajay/B-5562-2008; Burn, Paul/F-5347-2010; Meredith, Paul/E-6092-2013; Nardes, Alexandre/C-8556-2012; Kopidakis, Nikos/N-4777-2015 OI Pandey, Ajay/0000-0002-6599-745X; FU Australian Research Council [FF0668728]; University of Queensland (Strategic Initiative-Centre for Organic Photonics Electronics); Queensland Government (National and International Research Alliances Program-"Queensland Organic Solar Cell Alliance"); "Molecularly Engineered Energy Materials", an Energy Frontier Research Center; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001342:001] FX PLB is recipient of an Australian Research Council Federation Fellowship (Project number FF0668728). PM is a Vice Chancellor's Senior Research Fellow. We acknowledge funding from the University of Queensland (Strategic Initiative-Centre for Organic Photonics & Electronics), the Queensland Government (National and International Research Alliances Program-"Queensland Organic Solar Cell Alliance"). This work was performed in part at the Queensland node of the Australian National Fabrication Facility (ANFF-Q). AMN and NK acknowledge funding from "Molecularly Engineered Energy Materials", an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract Number DE-SC0001342:001. NR 28 TC 61 Z9 62 U1 3 U2 121 PU WILEY-V C H VERLAG GMBH PI WEINHEIM PA BOSCHSTRASSE 12, D-69469 WEINHEIM, GERMANY SN 1614-6832 J9 ADV ENERGY MATER JI Adv. Energy Mater. PD JAN PY 2013 VL 3 IS 1 BP 54 EP 59 DI 10.1002/aenm.201200372 PG 6 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary; Physics, Applied; Physics, Condensed Matter SC Chemistry; Energy & Fuels; Materials Science; Physics GA 066SD UT WOS:000313239600008 ER PT J AU Trahey, L Karan, NK Chan, MKY Lu, J Ren, Y Greeley, J Balasubramanian, M Burrell, AK Curtiss, LA Thackeray, MM AF Trahey, Lynn Karan, Naba K. Chan, Maria K. Y. Lu, Jun Ren, Yang Greeley, Jeffrey Balasubramanian, Mahalingam Burrell, Anthony K. Curtiss, Larry A. Thackeray, Michael M. TI Synthesis, Characterization, and Structural Modeling of High-Capacity, Dual Functioning MnO2 Electrode/Electrocatalysts for Li-O2 Cells SO ADVANCED ENERGY MATERIALS LA English DT Article DE Li-O2; batteries; MnO2; electrocatalysts; electrodes ID ALPHA-MANGANESE-DIOXIDE; V LITHIUM BATTERIES; LI-AIR BATTERIES; CATALYTIC DECOMPOSITION; CARBONATE ELECTROLYTES; OXIDES; ELECTRODES; STABILITY; ION; LIMITATIONS AB It has become clear that cycling lithium-oxygen cells in carbonate electrolytes is impractical, as electrolyte decomposition, triggered by oxygen reduction products, dominates the cell chemistry. This research shows that employing an a-MnO2/ramsdellite-MnO2 electrode/electrocatalyst results in the formation of lithium-oxide-like discharge products in propylene carbonate, which has been reported to be extremely susceptible to decomposition. X-ray photoelectron data have shown that what are likely lithium oxides (Li2O2 and Li2O) appear to form and decompose on the air electrode surface, particularly at the MnO2 surface, while Li2CO3 is also formed. By contrast, cells without a-MnO2/ramsdellite-MnO2 fail rapidly in electrochemical cycling, likely due to the differences in the discharge product. Relatively high electrode capacities, up to 5000 mAh/g (carbon + electrode/electrocatalyst), have been achieved with non-optimized air electrodes. Insights into reversible insertion reactions of lithium, lithium peroxide (Li2O2) and lithium oxide (Li2O) in the tunnels of a-MnO2, and the reaction of lithium with ramsdellite-MnO2, as determined by first principles density functional theory calculations, are used to provide a possible explanation for some of the observed results. It is speculated that a Li2O-stabilized and partially-lithiated electrode component, 0.15Li2O.a-LixMnO2, that has Mn4+/3+ character may facilitate the Li2O2/Li2O discharge/charge chemistries providing dual electrode/electrocatalyst functionality. C1 [Trahey, Lynn; Lu, Jun; Burrell, Anthony K.; Thackeray, Michael M.] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. [Karan, Naba K.; Ren, Yang; Balasubramanian, Mahalingam] Argonne Natl Lab, Adv Photon Source, Xray Sci Div, Argonne, IL 60439 USA. [Chan, Maria K. Y.; Greeley, Jeffrey; Curtiss, Larry A.] Argonne Natl Lab, Ctr Nanoscale Mat, Argonne, IL 60439 USA. [Curtiss, Larry A.] Argonne Natl Lab, Div Mat Sci, Argonne, IL 60439 USA. RP Trahey, L (reprint author), Argonne Natl Lab, Chem Sci & Engn Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM trahey@anl.gov RI Chan, Maria /B-7940-2011 OI Chan, Maria /0000-0003-0922-1363 FU US Department of Energy; Center for Electrical Energy Storage: Tailored Interfaces, an Energy Frontier Research Center; US Department of Energy, Office of Science, Office of Basic Energy Sciences; Department of Energy (DOE) Office of Energy Efficiency and Renewable Energy (EERE) Postdoctoral Research Award under the EERE Vehicles Technology Program; DOE [DE-AC05-06OR23100]; US DOE, NSERC (Canada); US Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357] FX Financial support from the US Department of Energy is gratefully acknowledged. Elemental analysis using ICP-OES was provided by Argonne's Analytical Chemistry Laboratory. Jeff Fortner (TEM), Jianglan Shui (BET), and Joseph S. Gregar (custom glass chambers) are gratefully acknowledged. XAS studies were carried out at sector 20-BM (XSD/PNC) in the Advanced Photon Source. M. C. and J.G. (theoretical modeling) were supported by the Center for Electrical Energy Storage: Tailored Interfaces, an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Office of Basic Energy Sciences and gratefully acknowledge use of the Fusion cluster in the Laboratory Computing Resource Center at Argonne National Laboratory. J.L. was supported by the Department of Energy (DOE) Office of Energy Efficiency and Renewable Energy (EERE) Postdoctoral Research Award under the EERE Vehicles Technology Program administered by the Oak Ridge Institute for Science and Education (ORISE) for the DOE. ORISE is managed by Oak Ridge Associated Universities (ORAU) under DOE contract number DE-AC05-06OR23100. Work at XSD/PNC is supported by the US DOE, NSERC (Canada) and its founding institutions. Use of the Center for Nanoscale Materials was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, under contract No. DE-AC02-06CH11357. NR 47 TC 56 Z9 56 U1 30 U2 380 PU WILEY-V C H VERLAG GMBH PI WEINHEIM PA BOSCHSTRASSE 12, D-69469 WEINHEIM, GERMANY SN 1614-6832 J9 ADV ENERGY MATER JI Adv. Energy Mater. PD JAN PY 2013 VL 3 IS 1 BP 75 EP 84 DI 10.1002/aenm.201200037 PG 10 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary; Physics, Applied; Physics, Condensed Matter SC Chemistry; Energy & Fuels; Materials Science; Physics GA 066SD UT WOS:000313239600011 ER PT J AU Shingledecker, JP Pint, BA Sabau, AS Fry, AT Wright, IG AF Shingledecker, J. P. Pint, B. A. Sabau, A. S. Fry, A. T. Wright, I. G. TI Managing Steam-Side Oxidation and Exfoliation in USC Boiler Tubes SO ADVANCED MATERIALS & PROCESSES LA English DT Article AB Materials are the key enabling technology driving development of high-efficiency power plants, which requires better fundamental and practical understanding of the effects of operating environments. C1 [Shingledecker, J. P.] Elect Power Res Inst, Fossil Mat & Repair Program P87, Charlotte, NC 28262 USA. [Pint, B. A.; Sabau, A. S.] Oak Ridge Natl Lab, Oak Ridge, TN USA. [Fry, A. T.] Natl Phys Lab, Teddington TW11 0LW, Middx, England. [Wright, I. G.] Wright HT, Denver, CO USA. RP Shingledecker, JP (reprint author), Elect Power Res Inst, Fossil Mat & Repair Program P87, Charlotte, NC 28262 USA. EM jshingledecker@epri.com RI Sabau, Adrian/B-9571-2008; Pint, Bruce/A-8435-2008; Fry, Tony/E-3448-2014 OI Sabau, Adrian/0000-0003-3088-6474; Pint, Bruce/0000-0002-9165-3335; Fry, Tony/0000-0002-7925-1392 NR 4 TC 4 Z9 4 U1 1 U2 12 PU ASM INT PI MATERIALS PARK PA SUBSCRIPTIONS SPECIALIST CUSTOMER SERVICE, MATERIALS PARK, OH 44073-0002 USA SN 0882-7958 J9 ADV MATER PROCESS JI Adv. Mater. Process. PD JAN PY 2013 VL 171 IS 1 BP 23 EP 25 PG 3 WC Materials Science, Multidisciplinary SC Materials Science GA 068VU UT WOS:000313395100003 ER PT J AU Cantrell, KJ Carroll, KC Buck, EC Neiner, D Geiszler, KN AF Cantrell, Kirk J. Carroll, Kenneth C. Buck, Edgar C. Neiner, Doinita Geiszler, Keith N. TI Single-pass flow-through test elucidation of weathering behavior and evaluation of contaminant release models for Hanford tank residual radioactive waste SO APPLIED GEOCHEMISTRY LA English DT Article ID SOLUBILITY MEASUREMENTS; URANYL; PREDICTION; 241-C-204; CARBONATE; PHASES AB Contaminant release models are required to evaluate and predict long-term environmental impacts of residual amounts of high-level radioactive waste after cleanup and closure of radioactively contaminated sites such as the DOE's Hanford Site. More realistic and representative models have been developed for release of U, Tc and Cr from Hanford Site tanks C-202, C-203, and C-103 residual wastes using data collected with a single-pass flow-through test (SPFT) method. These revised models indicate that contaminant release concentrations from these residual wastes will be considerably lower than previous estimates based on batch experiments. For U, a thermodynamic solubility model provides an effective description of U release, which can account for differences in pore fluid chemistry contacting the waste that could occur through time and as a result of different closure scenarios. Under certain circumstances in the SPFT experiments various Ca-rich precipitates (Ca phosphates and calcite) form on the surfaces of the waste particles, inhibiting dissolution of the underlying U phases in the waste. This behavior was not observed in previous batch experiments. For both Tc and Cr, empirical release models were developed. In the case of Tc, release from all three wastes was modeled using an equilibrium K-d model. For Cr release, a constant concentration model was applied for all three wastes. (C) 2012 Elsevier Ltd. All rights reserved. C1 [Cantrell, Kirk J.; Carroll, Kenneth C.; Buck, Edgar C.; Neiner, Doinita; Geiszler, Keith N.] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Cantrell, KJ (reprint author), Pacific NW Natl Lab, POB 999,Mail Stop K6-81, Richland, WA 99352 USA. EM kirk.cantrell@pnnl.gov RI Buck, Edgar/N-7820-2013; Carroll, Kenneth/H-5160-2011 OI Buck, Edgar/0000-0001-5101-9084; Carroll, Kenneth/0000-0003-2097-9589 FU Washington River Protection Solutions LLC (Richland, Washington); DOE by Battelle Memorial Institute [DE-AC05-76RL01830] FX The authors acknowledge Mike Connelly and Susan Eberlein at Washington River Protection Solutions LLC (Richland, Washington) for providing project funding and technical guidance. Pacific Northwest National Laboratory is operated for DOE by Battelle Memorial Institute under contract DE-AC05-76RL01830. NR 31 TC 4 Z9 4 U1 0 U2 18 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0883-2927 J9 APPL GEOCHEM JI Appl. Geochem. PD JAN PY 2013 VL 28 BP 119 EP 127 DI 10.1016/j.apgeochem.2012.09.004 PG 9 WC Geochemistry & Geophysics SC Geochemistry & Geophysics GA 066BX UT WOS:000313196000013 ER PT J AU Tamano, K Bruno, KS Karagiosis, SA Culley, DE Deng, S Collett, JR Umemura, M Koike, H Baker, SE Machida, M AF Tamano, Koichi Bruno, Kenneth S. Karagiosis, Sue A. Culley, David E. Deng, Shuang Collett, James R. Umemura, Myco Koike, Hideaki Baker, Scott E. Machida, Masayuki TI Increased production of fatty acids and triglycerides in Aspergillus oryzae by enhancing expressions of fatty acid synthesis-related genes SO APPLIED MICROBIOLOGY AND BIOTECHNOLOGY LA English DT Article DE Fatty acid; Triglyceride; Biofuel; Productivity; Aspergillus oryzae ID PHYLOGENOMIC ANALYSIS; BIODIESEL PRODUCTION; LIPID-ACCUMULATION; GENOME SEQUENCE; NIDULANS; OVERPRODUCTION; FUMIGATUS; GROWTH; ENZYME AB Microbial production of fats and oils is being developed as a means of converting biomass to biofuels. Here we investigate enhancing expression of enzymes involved in the production of fatty acids and triglycerides as a means to increase production of these compounds in Aspergillus oryzae. Examination of the A. oryzae genome demonstrates that it contains two fatty acid synthases and several other genes that are predicted to be part of this biosynthetic pathway. We enhanced the expression of fatty acid synthesis-related genes by replacing their promoters with the promoter from the constitutively highly expressed gene tef1. We demonstrate that by simply increasing the expression of the fatty acid synthase genes we successfully increased the production of fatty acids and triglycerides by more than two-fold. Enhancement of expression of the fatty acid pathway genes ATP-citrate lyase and palmitoyl-ACP thioesterase increased productivity to a lesser extent. Increasing expression of acetyl-CoA carboxylase caused no detectable change in fatty acid levels. Increases in message level for each gene were monitored using quantitative real-time reverse transcription polymerase chain reaction. Our data demonstrate that a simple increase in the abundance of fatty acid synthase genes can increase the detectable amount of fatty acids. C1 [Tamano, Koichi; Umemura, Myco; Machida, Masayuki] Natl Inst Adv Ind Sci & Technol, Bioprod Res Inst, Toyohira Ku, Sapporo, Hokkaido 0628517, Japan. [Tamano, Koichi; Umemura, Myco; Koike, Hideaki; Machida, Masayuki] Natl Inst Adv Ind Sci & Technol, Bioprod Res Inst, Tsukuba, Ibaraki 3058566, Japan. [Bruno, Kenneth S.; Karagiosis, Sue A.; Culley, David E.; Deng, Shuang; Collett, James R.; Baker, Scott E.] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Machida, M (reprint author), Natl Inst Adv Ind Sci & Technol, Bioprod Res Inst, Toyohira Ku, 2-17-2-1 Tsukisamu Higashi, Sapporo, Hokkaido 0628517, Japan. EM m.machida@aist.go.jp FU Ministry of Economy, Trade, and Industry, Japan; Department of Energy, USA FX We appreciate the daily research-related paperwork by Ms. Debra Lee and Ms. Ana Lundeby at PNNL. We are also grateful to Dr. Osamu Yamada (National Research Institute of Brewing, Japan) for giving us information on the DNA sequences of mutations at niaD and sC loci, respectively, of A. oryzae RIB40 niaD sC strain that is called NS4 generally. And we thank Dr. Katsuya Gomi (Tohoku University) for providing A. oryzae RIB40 Delta ligD::ptrA niaD sC strain, a derivative of NS4, to construct both NS4DLP and NS4DLDP. This work was performed by the grant-in-aid of the Ministry of Economy, Trade, and Industry, Japan. Also this work was supported by the grant-in-aid of the Department of Energy, USA. NR 34 TC 28 Z9 36 U1 3 U2 43 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 0175-7598 J9 APPL MICROBIOL BIOT JI Appl. Microbiol. Biotechnol. PD JAN PY 2013 VL 97 IS 1 BP 269 EP 281 DI 10.1007/s00253-012-4193-y PG 13 WC Biotechnology & Applied Microbiology SC Biotechnology & Applied Microbiology GA 064HS UT WOS:000313065400025 PM 22733113 ER PT J AU Hastbacka, M Dieckmann, J Bouza, A AF Hastbacka, Mildred Dieckmann, John Bouza, Antonio TI ERV Technology Revisited SO ASHRAE JOURNAL LA English DT Editorial Material C1 [Hastbacka, Mildred; Dieckmann, John] TIAX LLC, Mech Syst Grp, Lexington, MA USA. [Bouza, Antonio] US DOE, Washington, DC 20585 USA. RP Hastbacka, M (reprint author), TIAX LLC, Mech Syst Grp, Lexington, MA USA. NR 5 TC 1 Z9 1 U1 0 U2 2 PU AMER SOC HEATING REFRIGERATING AIR-CONDITIONING ENG, INC, PI ATLANTA PA 1791 TULLIE CIRCLE NE, ATLANTA, GA 30329 USA SN 0001-2491 J9 ASHRAE J JI ASHRAE J. PD JAN PY 2013 VL 55 IS 1 BP 65 EP 67 PG 3 WC Thermodynamics; Construction & Building Technology; Engineering, Mechanical SC Thermodynamics; Construction & Building Technology; Engineering GA 068QO UT WOS:000313381500014 ER PT J AU Vogel, K AF Vogel, Kathleen M. TI Intelligent assessment: Putting emerging biotechnology threats in context SO BULLETIN OF THE ATOMIC SCIENTISTS LA English DT Article DE biotechnology; evolution; intelligence assessments; networks; red teaming; revolution; sociotechnical; technological determinism AB One of the problems with assessing the emerging threats from advances in biotechnology and the life sciences is that there are two competing narratives for understanding biotechnology development: one based on the notion of a biotech revolution and the other based on biotech evolution. The biotech revolution is a dystopian tale in which scientific advances lead to rapid changes in biotechnology, its applications, and its potential threats. The biotech evolution, however, describes slower and more complex trajectories for biotechnology development and threats. These two narratives are based on different assumptions and analytic methods, which lead to fundamentally different conclusions. The US intelligence and policy communities use the biotech revolution story line to make sense of today's bioweapons threats, but this approach fails to reflect the complex social, economic, scientific, and technical factors that shape biotechnology and life science developments. The author argues that more critical perspectives on biotechnology are needed in order to improve intelligence assessments of present and future bioweapons threats and policy regarding them. C1 [Vogel, Kathleen M.] Cornell Univ, Dept Sci & Technol Studies, Ithaca, NY 14853 USA. [Vogel, Kathleen M.] Cornell Univ, Judith Reppy Inst, Ithaca, NY 14853 USA. [Vogel, Kathleen M.] US Dept State, Off Proliferat Threat Reduct, Bur Int Secur & Nonproliferat, Washington, DC USA. RP Vogel, K (reprint author), Sandia Natl Labs, Cooperat Monitoring Ctr, Livermore, CA 94550 USA. NR 43 TC 1 Z9 1 U1 2 U2 14 PU SAGE PUBLICATIONS LTD PI LONDON PA 1 OLIVERS YARD, 55 CITY ROAD, LONDON EC1Y 1SP, ENGLAND SN 0096-3402 EI 1938-3282 J9 B ATOM SCI JI Bull. Atom. Scient. PD JAN-FEB PY 2013 VL 69 IS 1 BP 43 EP 52 DI 10.1177/0096340212470813 PG 10 WC International Relations; Social Issues SC International Relations; Social Issues GA 065TY UT WOS:000313173500007 ER PT J AU Scheins, S Overgaard, J Timco, GA Stash, A Chen, YS Larsen, FK Christensen, M Jorgensen, MRV Madsen, SR Schmokel, MS Iversen, BB AF Scheins, Stephan Overgaard, Jacob Timco, Grigore A. Stash, Adam Chen, Yu-Sheng Larsen, Finn K. Christensen, Mogens Jorgensen, Mads R. V. Madsen, Solveig R. Schmokel, Mette S. Iversen, Bo B. TI Pressure versus Temperature Effects on Intramolecular Electron Transfer in Mixed-Valence Complexes SO CHEMISTRY-A EUROPEAN JOURNAL LA English DT Article DE carboxylates; electron transfer; high-pressure diffraction; mixed-valent compounds; X-ray diffraction ID IRON CYANOACETATE COMPLEX; X-RAY-DIFFRACTION; SOLID-STATE; PHASE-TRANSITIONS; INTERMOLECULAR INTERACTIONS; TRINUCLEAR COMPLEXES; MOLECULAR-CRYSTALS; SOLVATE MOLECULES; ACETATE COMPLEXES; FE-57 MOSSBAUER AB Mixed-valence trinuclear carboxylates, [M3O(O2CR)(6)L-3] (M = metal, L = terminal ligand), have small differences in potential energy between the configurations (MMMIII)-M-II-M-III double left right arrow(MMMIII)-M-III-M-II double left right arrow(MMMII)-M-III-M-III, which means that small external changes can have large structural effects, owing to the differences in coordination geometry between M2+ and M3+ sites (e. g., about 0.2 angstrom for Fe-O bond lengths). It is well-established that the electron transfer (ET) between the metal sites in these mixed-valence molecules is strongly dependent on temperature and on the specific crystal environment; however, herein, for the first time, we examine the effect of pressure on the electron transfer. Based on single-crystal X-ray diffraction data that were measured at 15, 90, 100, 110, 130, 160, and 298 K on three different crystals, we first unexpectedly found that our batch of Fe3O (O2CC(CH3)(3))(6)-(C5H5N)(3) (1) exhibited a different temperature dependence of the ET process than previous studies of compound 1 have shown. We observed a phase transition at around 130 K that was related to complete valence trapping and Hirshfeld surface analysis revealed that this phase transition was governed by a subtle competition between C H center dot center dot center dot pi and pi center dot center dot center dot pi intermolecular interactions. Subsequent high-pressure single-crystal X-ray diffraction at pressures of 0.15, 0.35, 0.45, 0.74, and 0.96 GPa revealed that it was not possible to trigger the phase transition (i.e., valence trapping) by a reduction of the unit-cell volume, owing to this external pressure. We conclude that modulation of the ET process requires anisotropic changes in the intermolecular interactions, which occur when various directional chemical bonds are affected differently by changes in temperature, but not by the application of pressure. C1 [Scheins, Stephan; Overgaard, Jacob; Larsen, Finn K.; Christensen, Mogens; Jorgensen, Mads R. V.; Madsen, Solveig R.; Schmokel, Mette S.; Iversen, Bo B.] Aarhus Univ, Dept Chem, DK-8000 Aarhus C, Denmark. [Scheins, Stephan; Stash, Adam; Chen, Yu-Sheng] Argonne Natl Lab, ChemMatCARS, Argonne, IL 60439 USA. [Stash, Adam] Karpov Inst Phys Chem, Moscow 103064, Russia. [Timco, Grigore A.] Univ Manchester, Sch Chem, Lewis Magnetism Lab, Manchester M13 9PL, Lancs, England. RP Iversen, BB (reprint author), Aarhus Univ, Dept Chem, Langelandsgade 140, DK-8000 Aarhus C, Denmark. EM bo@chem.au.dk RI Jorgensen, Mads Ry Vogel/C-6109-2017; OI Jorgensen, Mads Ry Vogel/0000-0001-5507-9615; Overgaard, Jacob/0000-0001-6492-7962 FU Danish Strategic Research Council (Center for Energy Materials); Danish National Research Foundation (Center for Materials Crystallography); Danish Research Council for Nature and Universe (Danscatt); National Science Foundation; Department of Energy [NSF/CHE-0822838]; National Science Foundation-Earth Sciences [EAR-0622171]; Department of Energy-Geosciences [DE-FG02-94ER14466]; US Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357] FX The work was supported by The Danish Strategic Research Council (Center for Energy Materials), the Danish National Research Foundation (Center for Materials Crystallography) 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 number NSF/CHE-0822838. Portions of this work were performed at GeoSoilEnviroCARS (Sector 13), Advanced Photon Source (APS), the Argonne National Laboratory. GeoSoilEnviroCARS is supported by the National Science Foundation-Earth Sciences (EAR-0622171) and by the Department of Energy-Geosciences (DE-FG02-94ER14466). Use of the Advanced Photon Source was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. NR 69 TC 6 Z9 6 U1 0 U2 48 PU WILEY-V C H VERLAG GMBH PI WEINHEIM PA POSTFACH 101161, 69451 WEINHEIM, GERMANY SN 0947-6539 EI 1521-3765 J9 CHEM-EUR J JI Chem.-Eur. J. PD JAN PY 2013 VL 19 IS 1 BP 195 EP 205 DI 10.1002/chem.201201669 PG 11 WC Chemistry, Multidisciplinary SC Chemistry GA 065OG UT WOS:000313157200021 PM 23169277 ER PT J AU Guibas, L Morozov, D Merigot, Q AF Guibas, Leonidas Morozov, Dmitriy Merigot, Quentin TI Witnessed k-Distance SO DISCRETE & COMPUTATIONAL GEOMETRY LA English DT Article DE Distance function; Order-k Voronoi diagram; Geometric inference; Surface reconstruction; Wasserstein noise ID SURFACE RECONSTRUCTION; DIAGRAMS; HOMOLOGY; SAMPLES AB Distance functions to compact sets play a central role in several areas of computational geometry. Methods that rely on them are robust to the perturbations of the data by the Hausdorff noise, but fail in the presence of outliers. The recently introduced distance to a measure offers a solution by extending the distance function framework to reasoning about the geometry of probability measures, while maintaining theoretical guarantees about the quality of the inferred information. A combinatorial explosion hinders working with distance to a measure as an ordinary power distance function. In this paper, we analyze an approximation scheme that keeps the representation linear in the size of the input, while maintaining the guarantees on the inference quality close to those for the exact but costly representation. C1 [Guibas, Leonidas] Stanford Univ, Dept Comp Sci, Stanford, CA 94305 USA. [Morozov, Dmitriy] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Merigot, Quentin] Univ Grenoble, Lab Jean Kuntzmann, St Martin Dheres, France. [Merigot, Quentin] Ecole Natl Super Electrochim & Electrome Grenoble, Thermodynam & Physicochim Met Lab, CNRS, F-38402 St Martin Dheres, France. RP Morozov, D (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. EM guibas@cs.stanford.edu; dmitriy@mrzv.org; quentin.merigot@imag.fr FU French ANR [ANR-09-BLAN-0331-01]; NSF [FODAVA 0808515, CCF 1011228]; NSF/NIH [0900700]; LBNL of the DOE Office of Science, Advanced Scientific Computing Research [KJ0402-KRD047, DE-AC02-05CH11231] FX The authors would like to thank the anonymous referees for their insightful feedback. This work has been partly supported by a grant from the French ANR, ANR-09-BLAN-0331-01, NSF grants FODAVA 0808515, CCF 1011228, and NSF/NIH grant 0900700. Quentin Merigot would also like to acknowledge the support of the Fields Institute during the revision of this article. Dmitriy Morozov would like to acknowledge the support at LBNL of the DOE Office of Science, Advanced Scientific Computing Research, under award number KJ0402-KRD047, under contract number DE-AC02-05CH11231. NR 24 TC 6 Z9 6 U1 0 U2 1 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 0179-5376 J9 DISCRETE COMPUT GEOM JI Discret. Comput. Geom. PD JAN PY 2013 VL 49 IS 1 SI SI BP 22 EP 45 DI 10.1007/s00454-012-9465-x PG 24 WC Computer Science, Theory & Methods; Mathematics SC Computer Science; Mathematics GA 069LU UT WOS:000313438500003 ER PT J AU Woods, J Kozubal, E AF Woods, Jason Kozubal, Eric TI A desiccant-enhanced evaporative air conditioner: Numerical model and experiments SO ENERGY CONVERSION AND MANAGEMENT LA English DT Article DE Liquid desiccant; Air conditioning; Membrane; Model; Indirect evaporative cooling; Experiments ID MEMBRANE-CHARACTERISTICS; HEAT; MASS; DEHUMIDIFIER/REGENERATOR; PERFORMANCE; DIFFUSION; EXCHANGER; CONTACTOR AB This article presents modeling and experimental results on a recently proposed liquid desiccant air conditioner, which consists of two stages: a liquid desiccant dehumidifier and an indirect evaporative cooler. Each stage is a stack of channel pairs, where a channel pair is a process air channel separated from an exhaust air channel with a thin plastic plate. In the first stage, a liquid desiccant film, which lines the process air channels, removes moisture from the air through a porous hydrophobic membrane. An evaporating water film wets the surface of the exhaust channels and transfers the enthalpy of vaporization from the liquid desiccant into an exhaust airstream, cooling the desiccant and enabling lower outlet humidity. The second stage is a counterflow indirect evaporative cooler that siphons off and uses a portion of the cool-dry air exiting the second stage as the evaporative sink. The objectives of this article are to (1) present fluid-thermal numerical models for each stage, (2) present experimental results of prototypes for each stage, and (3) compare the modeled and experimental results. Several experiments were performed on the prototypes over a range of inlet temperatures and humidities, process and exhaust air flow rates, and desiccant concentrations and flow rates. The model predicts the experiments within +/- 10%. (C) 2012 Elsevier Ltd. All rights reserved. C1 [Woods, Jason; Kozubal, Eric] Natl Renewable Energy Lab, Golden, CO 80401 USA. RP Woods, J (reprint author), Natl Renewable Energy Lab, 15013 Denver W Pkwy, Golden, CO 80401 USA. EM jason.woods@nrel.gov OI Woods, Jason/0000-0002-7661-2658 FU US Department of Energy [DE-AC36-08-GO28308]; National Renewable Energy Laboratory FX This work was supported by the US Department of Energy under Contract No. DE-AC36-08-GO28308 with the National Renewable Energy Laboratory. We want to thank Ian Graves, Redwood Stevens, and Dylan Garrett at Synapse Product Development and Andy Lowenstein at AIL Research for their support in prototype construction. NR 33 TC 50 Z9 50 U1 4 U2 40 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0196-8904 J9 ENERG CONVERS MANAGE JI Energy Conv. Manag. PD JAN PY 2013 VL 65 SI SI BP 208 EP 220 DI 10.1016/j.enconman.2012.08.007 PG 13 WC Thermodynamics; Energy & Fuels; Mechanics SC Thermodynamics; Energy & Fuels; Mechanics GA 065FS UT WOS:000313134500024 ER PT J AU Gorton, I AF Gorton, Ian TI Cyber Dumpster Diving: Creating New Software Systems for Less SO IEEE SOFTWARE LA English DT Article C1 Pacific NW Natl Lab, Richland, WA 99352 USA. RP Gorton, I (reprint author), Pacific NW Natl Lab, Richland, WA 99352 USA. EM ian.gorton@pnnl.gov NR 2 TC 1 Z9 1 U1 0 U2 1 PU IEEE COMPUTER SOC PI LOS ALAMITOS PA 10662 LOS VAQUEROS CIRCLE, PO BOX 3014, LOS ALAMITOS, CA 90720-1314 USA SN 0740-7459 J9 IEEE SOFTWARE JI IEEE Softw. PD JAN-FEB PY 2013 VL 30 IS 1 BP 9 EP 13 PG 5 WC Computer Science, Software Engineering SC Computer Science GA 062JS UT WOS:000312916700004 ER PT J AU Denys, RV Zavaliy, IY Berezovets, VV Paul-Boncour, V Pecharsky, VK AF Denys, R. V. Zavaliy, I. Yu Berezovets, V. V. Paul-Boncour, V. Pecharsky, V. K. TI Phase equilibria in the Mg-Ti-Ni system at 500 degrees C and hydrogenation properties of selected alloys SO INTERMETALLICS LA English DT Article DE Intermetallics, miscellaneous; Ternary alloy systems; Hydrogen storage; Mechanical alloying and milling ID CRYSTAL-STRUCTURE; STORAGE ALLOYS; MAGNESIUM; HYDRIDES; SORPTION; NICKEL; MG2NI; ABSORPTION; TERNARY AB A number of ternary Mg-Ti-Ni alloys have been synthesized by high energy ball milling, followed by annealing heat treatment. On the basis of X-ray phase analysis of these alloys an isothermal section of the Mg-Ti-Ni phase diagram at 500 degrees C has been constructed. One ternary intermetallic compound with Mg3TiNi2 stoichiometry that adopts an ordered Ti2Ni-type structure has been identified. Binary cubic TiNi compound dissolves considerable amount of Mg to form a ternary phase MgxTi1-2/3xNi1-1/3x crystallizing in the CsCl-type structure and existing over the range of compositions 0 < x <= 0.5. Other binary phases do not show appreciable solubility of the third component. The hydrogenation behavior of Mg3TiNi2 compound and Mg0.5Ti0.67Ni0.83 solid solution phase has been studied. (C) 2012 Elsevier Ltd. All rights reserved. C1 [Denys, R. V.; Zavaliy, I. Yu; Berezovets, V. V.] NAS Ukraine, Physicomech Inst, UA-79601 Lvov, Ukraine. [Paul-Boncour, V.] CNRS, ICMPE, F-94320 Thiais, France. [Pecharsky, V. K.] Iowa State Univ, Ames Lab, Ames, IA 50011 USA. [Pecharsky, V. K.] Iowa State Univ, Dept Mat Sci & Engn, Ames, IA 50011 USA. RP Zavaliy, IY (reprint author), NAS Ukraine, Physicomech Inst, 5 Naukova Str, UA-79601 Lvov, Ukraine. EM zavaliy@ipm.lviv.ua RI Denys, Roman/C-8386-2012 OI Denys, Roman/0000-0002-5479-8279 FU US Civilian Research and Development Foundation (CRDF) [UKC2-2970-LV-09]; Office of Basic Energy Sciences, Materials Sciences and Engineering Division of the Office of Science, U.S. Department of Energy [DE-AC02-07CH11358]; Iowa State University FX Work at the Physico-Mechanical Institute of NAS of Ukraine was supported by the US Civilian Research and Development Foundation (CRDF), Grant UKC2-2970-LV-09. Work at Ames Laboratory was supported by the Office of Basic Energy Sciences, Materials Sciences and Engineering Division of the Office of Science, U.S. Department of Energy under contract No. DE-AC02-07CH11358 with Iowa State University. NR 44 TC 3 Z9 3 U1 2 U2 38 PU ELSEVIER SCI LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, OXON, ENGLAND SN 0966-9795 J9 INTERMETALLICS JI Intermetallics PD JAN PY 2013 VL 32 BP 167 EP 175 DI 10.1016/j.intermet.2012.09.010 PG 9 WC Chemistry, Physical; Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Chemistry; Materials Science; Metallurgy & Metallurgical Engineering GA 065JV UT WOS:000313145500025 ER PT J AU Wu, X Baker, I Miller, MK More, KL Bei, H Wu, H AF Wu, X. Baker, I. Miller, M. K. More, K. L. Bei, H. Wu, H. TI Microstructure and mechanical behavior of directionally solidified Fe35Ni15Mn25Al25 SO INTERMETALLICS LA English DT Article DE Nanostructured intermetallics; Mechanical properties at ambient temperature; Atom microprobe; Electron microscopy, transmission ID SPINODAL FE30NI20MN25AL25 ALLOY; STRENGTH; MODEL AB The effects of directional solidification (DS) processing on the microstructure and hardness of Fe35Ni15Mn25Al25 are examined. The microstructure consists of (Fe, Mn)-enriched B2-ordered (ordered b.c.c.) and (Ni, Al)-enriched L2(1)-ordered (Heusler) phases aligned along <100> directions in a complex percolating morphology. Because of the slow cooling rate during DS processing, the phase size in the DS alloy was approximately 3 times greater than that of an arc-melted alloy. Precipitates were found within both phases of the as-DS alloy, but not in the as-arc-melted alloy. Upon annealing, the phase size increased but with no significant change in the composition of the phases, while the interphase interfaces appeared to become sharper. The hardness of the DS alloy increased monotonically upon annealing, and showed an inverse relationship with the phase size before the formation of large beta-Mn-structured precipitates. Several theoretical models are considered that might explain this variation of hardness with phase width. Longer annealing resulted in growth of the beta-Mn-structured precipitates, causing a further 50% hardness increase. (C) 2012 Elsevier Ltd. All rights reserved. C1 [Wu, X.; Baker, I.] Dartmouth Coll, Thayer Sch Engn, Hanover, NH 03755 USA. [Miller, M. K.; More, K. L.; Bei, H.] Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN 37831 USA. [Wu, H.] Cent S Univ, State Key Lab Powder Met, Changsha 410083, Hunan, Peoples R China. RP Baker, I (reprint author), Dartmouth Coll, Thayer Sch Engn, Hanover, NH 03755 USA. EM Ian.Baker@Dartmouth.edu RI More, Karren/A-8097-2016; OI More, Karren/0000-0001-5223-9097; Bei, Hongbin/0000-0003-0283-7990 FU US Department of Energy, Office of Basic Energy Sciences (DOE) [DE-FG02-07ER46392]; Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy; U.S. Department of Energy, Basic Energy Sciences, Materials Sciences and Engineering Division FX This research was supported by the US Department of Energy, Office of Basic Energy Sciences (DOE grant DE-FG02-07ER46392). Research at the ORNL ShaRE User Facility was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy (Dr. M. K. Miller and Dr. K. L More). Dr. H. Bei was supported by the U.S. Department of Energy, Basic Energy Sciences, Materials Sciences and Engineering Division. The authors gratefully acknowledge Dr. Easo George of Oak Ridge National Lab for provision of the large ingots for DS, and K. F. Russell for technical assistance. NR 30 TC 2 Z9 2 U1 0 U2 26 PU ELSEVIER SCI LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, OXON, ENGLAND SN 0966-9795 J9 INTERMETALLICS JI Intermetallics PD JAN PY 2013 VL 32 BP 413 EP 422 DI 10.1016/j.intermet.2012.07.032 PG 10 WC Chemistry, Physical; Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Chemistry; Materials Science; Metallurgy & Metallurgical Engineering GA 065JV UT WOS:000313145500056 ER PT J AU Tseng, CHT Paul, BK Chang, CH Engelhard, MH AF Tseng, Chih Heng T. Paul, Brian K. Chang, Chih-Hung Engelhard, Mark H. TI Continuous precipitation of ceria nanoparticles from a continuous flow micromixer SO INTERNATIONAL JOURNAL OF ADVANCED MANUFACTURING TECHNOLOGY LA English DT Article DE Continuous flow synthesis; Ceria; Nanoparticles; Microreactor; Micromixer ID ULTRAVIOLET-ABSORPTION SPECTRA; CDSE NANOCRYSTALS; CEO2 NANOPARTICLES; BLUE-SHIFT; PARTICLES; CERIUM(IV); SIZE; PYROLYSIS; BEHAVIOR; POWDERS AB Cerium oxide nanoparticles were continuously precipitated from a solution of cerium(III) nitrate and ammonium hydroxide using a static microchannel T-mixer. T-mixer synthesis results were compared with synthesis results from batch precipitation. Findings show that the method of mixing is important in the ceria precipitation process. Uniform porous film structures and nanorods were produced when the particle chemistry was synthesized using T-mixing followed by spin coating. Batch mixing, when using higher NH4OH feed concentrations followed by spin coating, was characterized by the heavy agglomeration of nanoparticles. Similar, high aspect ratio nanorods were produced when feed conditions in both batch mixing and T-mixing were identical demonstrating that the momentum effects of continuous microchannel T-mixing did not impact the synthesis process. In addition, it was found that the micromixing approach reduced the exposure of the Ce(OH)(3) precipitates to oxygen, yielding hydroxide precipitates in place of CeO2 precipitates. The key advantage of the micro-scale T-mixing approach is higher throughput which is important for the scaling of ceria nanoparticle production. C1 [Tseng, Chih Heng T.; Paul, Brian K.] Oregon State Univ, Sch Mech Ind & Mfg Engn, Corvallis, OR 97331 USA. [Chang, Chih-Hung] Oregon State Univ, Sch Chem Biol & Environm Engn, Corvallis, OR 97331 USA. [Engelhard, Mark H.] Pacific NW Natl Lab, Environm Mol Sci Lab, Richland, WA 99352 USA. RP Paul, BK (reprint author), Oregon State Univ, Sch Mech Ind & Mfg Engn, 204 Rogers Hall, Corvallis, OR 97331 USA. EM brian.paul@oregonstate.edu OI Engelhard, Mark/0000-0002-5543-0812 FU DARPA RIMS program; National Science Foundation [CBET-0654434]; Department of Energy's Office of Biological and Environmental Research located at Pacific Northwest National Laboratory FX This research was funded by the DARPA RIMS program and National Science Foundation under grant CBET-0654434. The authors would like to thank Dr. Chunfei Li at PSU for his assistance in obtaining the TEM images. The XPS portion of this manuscript was performed using 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. NR 35 TC 3 Z9 3 U1 3 U2 64 PU SPRINGER LONDON LTD PI LONDON PA 236 GRAYS INN RD, 6TH FLOOR, LONDON WC1X 8HL, ENGLAND SN 0268-3768 J9 INT J ADV MANUF TECH JI Int. J. Adv. Manuf. Technol. PD JAN PY 2013 VL 64 IS 1-4 BP 579 EP 586 DI 10.1007/s00170-012-4428-1 PG 8 WC Automation & Control Systems; Engineering, Manufacturing SC Automation & Control Systems; Engineering GA 069BS UT WOS:000313410500048 ER PT J AU Harris, JK Caporaso, JG Walker, JJ Spear, JR Gold, NJ Robertson, CE Hugenholtz, P Goodrich, J McDonald, D Knights, D Marshall, P Tufo, H Knight, R Pace, NR AF Harris, J. Kirk Caporaso, J. Gregory Walker, Jeffrey J. Spear, John R. Gold, Nicholas J. Robertson, Charles E. Hugenholtz, Philip Goodrich, Julia McDonald, Daniel Knights, Dan Marshall, Paul Tufo, Henry Knight, Rob Pace, Norman R. TI Phylogenetic stratigraphy in the Guerrero Negro hypersaline microbial mat SO ISME JOURNAL LA English DT Article DE Guerrero Negro; rRNA phylogeny; microbial mats; microbial ecology; QIIME ID DETRENDED CORRESPONDENCE-ANALYSIS; PUTTING THINGS; DIVERSITY; COMMUNITY; BIOGEOCHEMISTRY; ECOSYSTEMS; COMPLEXITY; SEQUENCES; SULFUR; ORDER AB The microbial mats of Guerrero Negro (GN), Baja California Sur, Mexico historically were considered a simple environment, dominated by cyanobacteria and sulfate-reducing bacteria. Culture-independent rRNA community profiling instead revealed these microbial mats as among the most phylogenetically diverse environments known. A preliminary molecular survey of the GN mat based on only similar to 1500 small subunit rRNA gene sequences discovered several new phylum-level groups in the bacterial phylogenetic domain and many previously undetected lower-level taxa. We determined an additional similar to 119 000 nearly full-length sequences and 28 000 >200 nucleotide 454 reads from a 10-layer depth profile of the GN mat. With this unprecedented coverage of long sequences from one environment, we confirm the mat is phylogenetically stratified, presumably corresponding to light and geochemical gradients throughout the depth of the mat. Previous shotgun metagenomic data from the same depth profile show the same stratified pattern and suggest that metagenome properties may be predictable from rRNA gene sequences. We verify previously identified novel lineages and identify new phylogenetic diversity at lower taxonomic levels, for example, thousands of operational taxonomic units at the family-genus levels differ considerably from known sequences. The new sequences populate parts of the bacterial phylogenetic tree that previously were poorly described, but indicate that any comprehensive survey of GN diversity has only begun. Finally, we show that taxonomic conclusions are generally congruent between Sanger and 454 sequencing technologies, with the taxonomic resolution achieved dependent on the abundance of reference sequences in the relevant region of the rRNA tree of life. The ISME Journal (2013) 7, 50-60; doi:10.1038/ismej.2012.79; published online 26 July 2012 C1 [Harris, J. Kirk] Univ Colorado Denver, Sch Med, Dept Pediat, Aurora, CO USA. [Caporaso, J. Gregory] No Arizona Univ, Dept Comp Sci, Flagstaff, AZ 86011 USA. [Walker, Jeffrey J.; Gold, Nicholas J.; Robertson, Charles E.; Pace, Norman R.] Univ Colorado, Dept Mol Cellular & Dev Biol, Boulder, CO 80309 USA. [Walker, Jeffrey J.] SomaLogic Inc, Boulder, CO USA. [Spear, John R.] Colorado Sch Mines, Dept Civil & Environm Engn, Golden, CO 80401 USA. [Hugenholtz, Philip] DOE Joint Genome Inst, Walnut Creek, CA USA. [Hugenholtz, Philip] Univ Queensland, Australian Ctr Ecogen, Sch Chem & Mol Biosci, St Lucia, Qld, Australia. [Hugenholtz, Philip] Univ Queensland, Inst Mol Biosci, St Lucia, Qld, Australia. [Goodrich, Julia] Cornell Univ, Dept Mol Biol & Genet, Ithaca, NY USA. [McDonald, Daniel; Knights, Dan; Knight, Rob] Univ Colorado, Biofrontiers Inst, Boulder, CO 80309 USA. [Knights, Dan; Marshall, Paul; Tufo, Henry] Univ Colorado, Dept Comp Sci, Boulder, CO 80309 USA. [Knight, Rob] Univ Colorado, Howard Hughes Med Inst, Boulder, CO 80309 USA. [Knight, Rob] Univ Colorado, Dept Chem & Biochem, Boulder, CO 80309 USA. RP Pace, NR (reprint author), Univ Colorado, Dept Mol Cellular & Dev Biol, Boulder, CO 80309 USA. EM norman.pace@colorado.edu RI Hugenholtz, Philip/G-9608-2011; Knight, Rob/D-1299-2010; OI ROBERTSON, CHARLES/0000-0002-4136-4121; Spear, John/0000-0002-4664-7438 FU NSF Microbial Biology Postdoctoral start-up fund; National Institutes of Health; Howard Hughes Medical Institute; NASA Astrobiology Institute; Office of Science of the US Department of Energy [DE-AC02-05CH11231] FX We thank the Exportadora de Sal SA for access and assistance in working on-site. We are grateful for the enabling support of David DesMarais, Brad Bebout and Tori Hoehler, NASA Ames, Moffat Field, CA. Sanger sequencing was provided by the Joint Genome Institute Community Sequencing Program. JRS was supported by an NSF Microbial Biology Postdoctoral start-up fund. Work in the Knight lab was supported in part by the National Institutes of Health and the Howard Hughes Medical Institute. Work in the Pace laboratory was supported by grants from the NASA Astrobiology Institute. The work conducted by the US Department of Energy Joint Genome Institute is supported by the Office of Science of the US Department of Energy under Contract no. DE-AC02-05CH11231. NR 40 TC 53 Z9 53 U1 3 U2 73 PU NATURE PUBLISHING GROUP PI LONDON PA MACMILLAN BUILDING, 4 CRINAN ST, LONDON N1 9XW, ENGLAND SN 1751-7362 J9 ISME J JI ISME J. PD JAN PY 2013 VL 7 IS 1 BP 50 EP 60 DI 10.1038/ismej.2012.79 PG 11 WC Ecology; Microbiology SC Environmental Sciences & Ecology; Microbiology GA 066QT UT WOS:000313236000005 PM 22832344 ER PT J AU Garcia, SL McMahon, KD Martinez-Garcia, M Srivastava, A Sczyrba, A Stepanauskas, R Grossart, HP Woyke, T Warnecke, F AF Garcia, Sarahi L. McMahon, Katherine D. Martinez-Garcia, Manuel Srivastava, Abhishek Sczyrba, Alexander Stepanauskas, Ramunas Grossart, Hans-Peter Woyke, Tanja Warnecke, Falk TI Metabolic potential of a single cell belonging to one of the most abundant lineages in freshwater bacterioplankton SO ISME JOURNAL LA English DT Article DE freshwater Actinobacteria; metabolic potential; single-cell genomics ID COMMUNITY COMPOSITION; BACTERIAL COMMUNITY; SEQUENCE DATA; HUMIC LAKE; RNA GENES; ACTINOBACTERIA; GENOME; POPULATIONS; DIVERSITY; ECOLOGY AB Actinobacteria within the acI lineage are often numerically dominating in freshwater ecosystems, where they can account for >50% of total bacteria in the surface water. However, they remain uncultured to date. We thus set out to use single-cell genomics to gain insights into their genetic make-up, with the aim of learning about their physiology and ecological niche. A representative from the highly abundant acI-B1 group was selected for shotgun genomic sequencing. We obtained a draft genomic sequence in 75 larger contigs (sum = 1.16 Mb), with an unusually low genomic G + C mol% (similar to 42%). Actinobacteria core gene analysis suggests an almost complete genome recovery. We found that the acI-B1 cell had a small genome, with a rather low percentage of genes having no predicted functions (similar to 15%) as compared with other cultured and genome-sequenced microbial species. Our metabolic reconstruction hints at a facultative aerobe microorganism with many transporters and enzymes for pentoses utilization (for example, xylose). We also found an actinorhodopsin gene that may contribute to energy conservation under unfavorable conditions. This project reveals the metabolic potential of a member of the global abundant freshwater Actinobacteria. The ISME Journal (2013) 7, 137-147; doi:10.1038/ismej.2012.86; published online 19 July 2012 C1 [Warnecke, Falk] Univ Jena, Microbial Ecol Grp, Jena Sch Microbial Commun JSMC, D-07743 Jena, Germany. [McMahon, Katherine D.] Univ Wisconsin, Dept Civil & Environm Engn, Madison, WI 53706 USA. [McMahon, Katherine D.] Univ Wisconsin, Dept Bacteriol, Madison, WI 53706 USA. [Martinez-Garcia, Manuel; Stepanauskas, Ramunas] Bigelow Lab Ocean Sci, E Boothbay, ME USA. [Srivastava, Abhishek; Grossart, Hans-Peter] Leibniz Inst Freshwater Ecol & Inland Fisheries, Dept Limnol Stratified Lakes, Stechlin, Germany. [Sczyrba, Alexander] Univ Bielefeld, Ctr Biotechnol CeBiTec, D-33615 Bielefeld, Germany. [Sczyrba, Alexander; Woyke, Tanja] DOE Joint Genome Inst, Walnut Creek, CA USA. [Grossart, Hans-Peter] Postdam Univ, Inst Biochem & Biol, Potsdam, Germany. RP Warnecke, F (reprint author), Univ Jena, Microbial Ecol Grp, Jena Sch Microbial Commun JSMC, Philosophenweg 12, D-07743 Jena, Germany. EM falk.warnecke@uni-jena.de OI Garcia, Sarahi L./0000-0002-8622-0308; Stepanauskas, Ramunas/0000-0003-4458-3108; McMahon, Katherine D./0000-0002-7038-026X FU NSF [DEB-841933, OCE-821374]; German Science foundation [DFG GR 1540/17-1]; JSMC; Office of Science of the US Department of Energy [DE-AC02-05CH11231]; United States National Science Foundation [MCB-0702395, NTL-LTER DEB-0822700, CBET-0738309]; Swedish Wenner-Gren Foundation FX This work was supported by NSF grants DEB-841933 and OCE-821374 to RS. HPG and Abhishek Srivastava were supported by a grant given by the German Science foundation (DFG GR 1540/17-1). SLG and FW thank JSMC for funding and support. We also thank Drs Rohit Ghai and Francisco Rodriguez-Valera at the Universidad Miguel Hernandez, Alicante, Spain, for access to custom perl scripts. We thank Todd Miller for collecting the lake water sample used to recover the SAG sequence. The work conducted by the US Department of Energy Joint Genome Institute is supported by the Office of Science of the US Department of Energy under Contract No. DE-AC02-05CH11231. KDM acknowledges funding from the United States National Science Foundation Microbial Observatories program (MCB-0702395), the Long Term Ecological Research program (NTL-LTER DEB-0822700), a CAREER award (CBET-0738309) and the Swedish Wenner-Gren Foundation. NR 65 TC 33 Z9 33 U1 0 U2 68 PU NATURE PUBLISHING GROUP PI LONDON PA MACMILLAN BUILDING, 4 CRINAN ST, LONDON N1 9XW, ENGLAND SN 1751-7362 J9 ISME J JI ISME J. PD JAN PY 2013 VL 7 IS 1 BP 137 EP 147 DI 10.1038/ismej.2012.86 PG 11 WC Ecology; Microbiology SC Environmental Sciences & Ecology; Microbiology GA 066QT UT WOS:000313236000012 PM 22810059 ER PT J AU Malmstrom, RR Rodrigue, S Huang, KH Kelly, L Kern, SE Thompson, A Roggensack, S Berube, PM Henn, MR Chisholm, SW AF Malmstrom, Rex R. Rodrigue, Sebastien Huang, Katherine H. Kelly, Libusha Kern, Suzanne E. Thompson, Anne Roggensack, Sara Berube, Paul M. Henn, Matthew R. Chisholm, Sallie W. TI Ecology of uncultured Prochlorococcus clades revealed through single-cell genomics and biogeographic analysis SO ISME JOURNAL LA English DT Article DE HNLC; Prochlorococcus; siderophore ID NORTH-ATLANTIC OCEAN; MARINE CYANOBACTERIUM PROCHLOROCOCCUS; PHOSPHATE ACQUISITION GENES; NATURAL ORGANIC-LIGANDS; MICROBIAL ASSEMBLAGES; EQUATORIAL PACIFIC; QUANTITATIVE PCR; ECOTYPES; IRON; TIME AB Prochlorococcus is the numerically dominant photosynthetic organism throughout much of the world's oceans, yet little is known about the ecology and genetic diversity of populations inhabiting tropical waters. To help close this gap, we examined natural Prochlorococcus communities in the tropical Pacific Ocean using a single-cell whole-genome amplification and sequencing. Analysis of the gene content of just 10 single cells from these waters added 394 new genes to the Prochlorococcus pan-genome-that is, genes never before seen in a Prochlorococcus cell. Analysis of marker genes, including the ribosomal internal transcribed sequence, from dozens of individual cells revealed several representatives from two uncultivated clades of Prochlorococcus previously identified as HNLC1 and HNLC2. While the HNLC clades can dominate Prochlorococcus communities under certain conditions, their overall geographic distribution was highly restricted compared with other clades of Prochlorococcus. In the Atlantic and Pacific oceans, these clades were only found in warm waters with low Fe and high inorganic P levels. Genomic analysis suggests that at least one of these clades thrives in low Fe environments by scavenging organic-bound Fe, a process previously unknown in Prochlorococcus. Furthermore, the capacity to utilize organic-bound Fe appears to have been acquired horizontally and may be exchanged among other clades of Prochlorococcus. Finally, one of the single Prochlorococcus cells sequenced contained a partial genome of what appears to be a prophage integrated into the genome. The ISME Journal (2013) 7, 184-198; doi:10.1038/ismej.2012.89; published online 16 August 2012 C1 [Malmstrom, Rex R.; Rodrigue, Sebastien; Huang, Katherine H.; Kelly, Libusha; Kern, Suzanne E.; Thompson, Anne; Roggensack, Sara; Berube, Paul M.; Chisholm, Sallie W.] MIT, Dept Civil & Environm Engn, Cambridge, MA 02139 USA. [Malmstrom, Rex R.] US DOE, Joint Genome Inst, Walnut Creek, CA USA. [Rodrigue, Sebastien] Univ Sherbrooke, Dept Biol, Sherbrooke, PQ J1K 2R1, Canada. [Huang, Katherine H.; Henn, Matthew R.] Broad Inst MIT & Harvard, Cambridge, MA USA. RP Chisholm, SW (reprint author), MIT, Dept Civil & Environm Engn, 15 Vassar St, Cambridge, MA 02139 USA. EM chisholm@mit.edu FU Gordon and Betty Moore Foundation; NSF Center for Microbial Oceanography Research and Education; Natural Sciences and Engineering Research Council of Canada; Fonds quebecois de la recherche sur la nature et les technologies FX We thank Doug Rusch and Nyree West for providing sequence data, and C Mark Moore and Malcolm Woodward for providing nutrient data for the Atlantic Meridional Transect 17. Greg Kettler assisted with identifying genomic islands in Prochlorococcus MIT9202. We thank the Broad Institute Genome Sequencing Platform for their contributions to the generation of genomic data. This work was supported buy the Gordon and Betty Moore Foundation (SWC and MRH) and the NSF Center for Microbial Oceanography Research and Education (SWC). Sebastien Rodrigue was supported by postdoctoral fellowships from the Natural Sciences and Engineering Research Council of Canada and the 'Fonds quebecois de la recherche sur la nature et les technologies.' NR 69 TC 28 Z9 30 U1 1 U2 66 PU NATURE PUBLISHING GROUP PI LONDON PA MACMILLAN BUILDING, 4 CRINAN ST, LONDON N1 9XW, ENGLAND SN 1751-7362 J9 ISME J JI ISME J. PD JAN PY 2013 VL 7 IS 1 BP 184 EP 198 DI 10.1038/ismej.2012.89 PG 15 WC Ecology; Microbiology SC Environmental Sciences & Ecology; Microbiology GA 066QT UT WOS:000313236000016 PM 22895163 ER PT J AU Randeniya, DIB Hilliard, MR AF Randeniya, Duminda I. B. Hilliard, Michael R. TI Tracking and Predicting Barge Locations on Inland Waterways SO JOURNAL OF COMPUTING IN CIVIL ENGINEERING LA English DT Article DE Marine navigation; Predicting and tracking barges; Kalman filtering; Locally weighted polynomials; Inverse distance function; Transportation systems modeling ID NAVIGATION; RIVER AB In efforts to improve efficiency, safety, and security, several groups involved in inland waterway navigation have an interest in improving tracking of barges moving on waterways. Automated tracking devices have inherent limitations, and there is a need to predict locations over the next several hours. This paper presents a nonlinear, probabilistic prediction model developed and implemented to track spatial location and other navigation characteristics of a barge traveling on the inland waterway system. A prefilter to check the validity of the measurements, a nonlinear speed estimation process, and a Kalman filter to predict the navigation solution of the barge are developed in this work. Due to the complex dynamics involved in the barge navigation system, a nonlinear stochastic model was developed in state space to represent the process and measurement processes. The algorithm was verified using actual measurements obtained from multiple barges on multiple rivers acquired from different sensors. The results show a reliable and robust prediction algorithm for tracking inland waterway barges. DOI: 10.1061/(ASCE)CP.1943-5487.0000191. (C) 2013 American Society of Civil Engineers. C1 [Randeniya, Duminda I. B.; Hilliard, Michael R.] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. RP Randeniya, DIB (reprint author), Oak Ridge Natl Lab, 1 Bethel Valley Rd,MS 6054, Oak Ridge, TN 37831 USA. EM dumindar@yahoo.com RI Hilliard, Michael/C-3270-2016 OI Hilliard, Michael/0000-0002-4450-9250 FU U.S. Department of Homeland Security under U.S. Department of Energy [43WT10301]; U.S. Department of Energy [DE-AC05-00OR22725] FX This material is based on work supported by the U.S. Department of Homeland Security under U.S. Department of Energy Interagency Agreement 43WT10301. The views and conclusions contained in this document are those of the authors and should not be interpreted as necessarily representing the official policies, either expressed or implied, of the U.S. Department of Homeland Security. 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 nonexclusive, paidup, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. NR 16 TC 0 Z9 0 U1 1 U2 11 PU ASCE-AMER SOC CIVIL ENGINEERS PI RESTON PA 1801 ALEXANDER BELL DR, RESTON, VA 20191-4400 USA SN 0887-3801 J9 J COMPUT CIVIL ENG JI J. Comput. Civil. Eng. PD JAN-FEB PY 2013 VL 27 IS 1 BP 27 EP 35 DI 10.1061/(ASCE)CP.1943-5487.0000191 PG 9 WC Computer Science, Interdisciplinary Applications; Engineering, Civil SC Computer Science; Engineering GA 067KR UT WOS:000313293400004 ER PT J AU Zhou, L Liu, DY Karney, B Zhang, QF AF Zhou, Ling Liu, Deyou Karney, Bryan Zhang, Qinfen TI Closure to "Influence of Entrapped Air Pockets on Hydraulic Transients in Water Pipelines" by Ling Zhou, Deyou Liu, Bryan Karney, and Qinfen Zhang December 2011, Vol. 137, No. 12, pp. 1686-1692. DOI: 10.1061/(ASCE)HY.1943-7900.0000460 SO JOURNAL OF HYDRAULIC ENGINEERING-ASCE LA English DT Editorial Material ID MODEL; PIPE; FLOW C1 [Zhou, Ling; Liu, Deyou] Hohai Univ, Coll Water Conservancy & Hydropower Engn, Nanjing 210098, Jiangsu, Peoples R China. [Karney, Bryan] Univ Toronto, Dept Civil Engn, Toronto, ON M5S 1A4, Canada. [Zhang, Qinfen] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. RP Zhou, L (reprint author), Hohai Univ, Coll Water Conservancy & Hydropower Engn, 1 Xikang Rd, Nanjing 210098, Jiangsu, Peoples R China. EM zlhhu@163.com; Liudyhhuc@163.com; karney@ecf.utoronto.ca; zhangq1@ornl.gov NR 3 TC 3 Z9 3 U1 2 U2 14 PU ASCE-AMER SOC CIVIL ENGINEERS PI RESTON PA 1801 ALEXANDER BELL DR, RESTON, VA 20191-4400 USA SN 0733-9429 J9 J HYDRAUL ENG-ASCE JI J. Hydraul. Eng.-ASCE PD JAN PY 2013 VL 139 IS 1 BP 107 EP 108 DI 10.1061/(ASCE)HY.1943-7900.0000654 PG 2 WC Engineering, Civil; Engineering, Mechanical; Water Resources SC Engineering; Water Resources GA 068IY UT WOS:000313361400021 ER PT J AU Zhu, ZW Wang, XQ Dai, S Huang, BS He, Q AF Zhu, Zhenwei Wang, Xiqing Dai, Sheng Huang, Baoshan He, Qiang TI Fractional Characteristics of Coal Fly Ash for Beneficial Use SO JOURNAL OF MATERIALS IN CIVIL ENGINEERING LA English DT Article DE Fly ash; Surface properties; Sorption; Particle size distribution ID SIZE DISTRIBUTION; UNBURNED CARBON; METHYLENE-BLUE; COMBUSTION; ADSORPTION; MECHANISM; CONCRETE; FORMS AB As a primary by-product of coal combustion produced in large quantities, coal fly ash is a material receiving considerable interest for potential large-scale engineering applications. However, the beneficial use of coal fly ash in concrete production and contaminant removal, which have divergent constraints to sorption capacity, requires a more complete understanding of the surface and sorptive characteristics of fly ash. A systematic analysis of fly ash particle size fractions established linkages between particle size, particle morphology, unburned carbon content, surface area, and sorption capacity. Unburned carbon was enriched in fly ash fractions of the largest particle sizes and associated with irregularly shaped particles. Further, most of the surface area and sorption capacity of fly ash could be attributed to unburned carbon. More importantly, unburned carbon content, specific surface area, and methylene blue sorption capacity were shown to strongly correlate to one another, providing a potentially quantitative basis for understanding the surface properties of fly ash and developing more effective process options to enhance the fly ash sorption behavior desirable for specific engineering applications. DOI: 10.1061/(ASCE)MT.1943-5533.0000550. (C) 2013 American Society of Civil Engineers. C1 [Zhu, Zhenwei; He, Qiang] Univ Tennessee, Dept Civil & Environm Engn, Sci & Engn Res Facil 702, Knoxville, TN 37996 USA. [Wang, Xiqing; Dai, Sheng] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. RP He, Q (reprint author), Univ Tennessee, Dept Civil & Environm Engn, Sci & Engn Res Facil 702, 57A Perkins Hall, Knoxville, TN 37996 USA. EM zzhu3@utk.edu; wangx1@ornl.gov; dais@ornl.gov; bhuang@utk.edu; qianghe@utk.edu RI He, Qiang/G-9061-2011; Wang, Xiqing/E-3062-2010; Huang, Baoshan/G-4974-2011; Dai, Sheng/K-8411-2015 OI He, Qiang/0000-0002-7155-6474; Wang, Xiqing/0000-0002-1843-008X; Huang, Baoshan/0000-0001-8551-0082; Dai, Sheng/0000-0002-8046-3931 FU Southeastern Transportation Center at the University of Tennessee FX Zhenwei Zhu was partly supported by a graduate assistanship from the Southeastern Transportation Center at the University of Tennessee. NR 26 TC 0 Z9 0 U1 2 U2 16 PU ASCE-AMER SOC CIVIL ENGINEERS PI RESTON PA 1801 ALEXANDER BELL DR, RESTON, VA 20191-4400 USA SN 0899-1561 J9 J MATER CIVIL ENG JI J. Mater. Civ. Eng. PD JAN PY 2013 VL 25 IS 1 BP 63 EP 69 DI 10.1061/(ASCE)MT.1943-5533.0000550 PG 7 WC Construction & Building Technology; Engineering, Civil; Materials Science, Multidisciplinary SC Construction & Building Technology; Engineering; Materials Science GA 067KZ UT WOS:000313294300008 ER PT J AU Scharf, TW Prasad, SV AF Scharf, T. W. Prasad, S. V. TI Solid lubricants: a review SO JOURNAL OF MATERIALS SCIENCE LA English DT Review ID DIAMOND-LIKE CARBON; HYDROGENATED AMORPHOUS-CARBON; TUNGSTEN DISULFIDE FILMS; ATOMIC LAYER DEPOSITION; HEXAGONAL BORON-NITRIDE; PULSED-LASER DEPOSITION; FRICTION BEHAVIOR; NANOCOMPOSITE COATINGS; TRIBOLOGICAL BEHAVIOR; SUPERLOW FRICTION AB The fundamental mechanisms of solid lubrication are reviewed with examples from well-known solid lubricants like the transition metal dichalcogenides and diamond-like carbon families of coatings. Solid lubricants are applied either as surface coatings or as fillers in self-lubricating composites. Tribological (friction and wear) contacts with solid lubricant coatings typically result in transfer of a thin layer of material from the surface of the coating to the counterface, commonly known as a transfer film or tribofilm. The wear surfaces can exhibit different chemistry, microstructure, and crystallographic texture from those of the bulk coating due to surface chemical reactions with the surrounding environment. As a result, solid lubricant coatings that give extremely low friction and long wear life in one environment can fail to do so in a different environment. Most solid lubricants exhibit non-Amontonian friction behavior with friction coefficients decreasing with increasing contact stress. The main mechanism responsible for low friction is typically governed by interfacial sliding between the worn coating and the transfer film. Strategies are discussed for the design of novel coating architectures to adapt to varying environments. C1 [Scharf, T. W.; Prasad, S. V.] Sandia Natl Labs, Mat Sci & Engn Ctr, Albuquerque, NM 87185 USA. RP Prasad, SV (reprint author), Sandia Natl Labs, Mat Sci & Engn Ctr, POB 5800, Albuquerque, NM 87185 USA. EM svprasa@sandia.gov FU U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000]; The National Science Foundation [CMMI-0700828, CMMI-1100648] FX Sandia National Laboratories is a multiprogram laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy's National Nuclear Security Administration under Contract DE-AC04-94AL85000. The authors thank Joe Michael, Michael Rye, Paul Kotula, Dick Grant, and Bonnie McKenzie for their assistance in electron microscopy, and Jill Glass and Robert Grubbs for their critical reviews. TWS would also like to acknowledge partial support of this work from The National Science Foundation (Grant Numbers: CMMI-0700828 and CMMI-1100648). NR 101 TC 71 Z9 76 U1 21 U2 306 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 0022-2461 J9 J MATER SCI JI J. Mater. Sci. PD JAN PY 2013 VL 48 IS 2 BP 511 EP 531 DI 10.1007/s10853-012-7038-2 PG 21 WC Materials Science, Multidisciplinary SC Materials Science GA 062FA UT WOS:000312903400001 ER PT J AU Bjork, R Tikare, V Frandsen, HL Pryds, N AF Bjork, Rasmus Tikare, Veena Frandsen, Henrik Lund Pryds, Nini TI The Effect of Particle Size Distributions on the Microstructural Evolution During Sintering SO JOURNAL OF THE AMERICAN CERAMIC SOCIETY LA English DT Article ID GRAIN-GROWTH; SIMULATION; ALUMINA; SPHERES; COORDINATION; DIFFUSION AB Microstructural evolution and sintering behavior of powder compacts composed of spherical particles with different particle size distributions (PSDs) were simulated using a kinetic Monte Carlo model of solid-state sintering. Compacts of monosized particles, normal PSDs with fixed mean particle radii and a range of standard deviations, and log-normal PSDs with fixed mode and a range of skewness values were studied. Densification rate and final relative density were found to be inversely proportional to initial PSD width. Grain growth was faster during the early stages of sintering for broad PSDs, but the final grain sizes were smaller. These behaviors are explained by the smallest grains in the broader PSDs being consumed very quickly by larger neighboring grains. The elimination of the small grains reduces both the total number of necks and the neck area between particles, which in turn reduces the regions where vacancies can be annihilated, leading to slower densification rates. The loss of neck area causes grain growth by surface diffusion to become the dominant microstructural evolution mechanism, leading to poor densification. Finally, pore size was shown to increase with the width of PSDs, which also contributes to the lower densification rates. C1 [Bjork, Rasmus; Frandsen, Henrik Lund; Pryds, Nini] Tech Univ Denmark DTU, Dept Energy Convers & Storage, DK-4000 Roskilde, Denmark. [Tikare, Veena] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Bjork, R (reprint author), Tech Univ Denmark DTU, Dept Energy Convers & Storage, Frederiksborgvej 399, DK-4000 Roskilde, Denmark. EM rabj@dtu.dk RI Frandsen, Henrik/C-4826-2013; OI Frandsen, Henrik/0000-0001-8336-6363; Bjork, Rasmus/0000-0002-3728-2326; Pryds, Nini/0000-0002-5718-7924 FU Danish Council for Independent Research Technology and Production Sciences' (FTP) part of The Danish Agency for Science, Technology and Innovation (FI) [09-072888]; U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX The authors thank the Danish Council for Independent Research Technology and Production Sciences' (FTP), which is part of The Danish Agency for Science, Technology and Innovation (FI) (Project # 09-072888) for sponsoring the OPTIMAC research work. 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 26 TC 15 Z9 15 U1 3 U2 58 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0002-7820 J9 J AM CERAM SOC JI J. Am. Ceram. Soc. PD JAN PY 2013 VL 96 IS 1 BP 103 EP 110 DI 10.1111/jace.12100 PG 8 WC Materials Science, Ceramics SC Materials Science GA 066XC UT WOS:000313254300016 ER PT J AU Vignes, RM Soules, TF Stolken, JS Settgast, RR Elhadj, S Matthews, MJ AF Vignes, Ryan M. Soules, Thomas F. Stolken, James S. Settgast, Randolph R. Elhadj, Selim Matthews, Manyalibo J. TI Thermomechanical Modeling of Laser-Induced Structural Relaxation and Deformation of Glass: Volume Changes in Fused Silica at High Temperatures SO JOURNAL OF THE AMERICAN CERAMIC SOCIETY LA English DT Article ID THERMAL-CONDUCTIVITY; FICTIVE TEMPERATURE; VITREOUS SILICA; CO2-LASER; SURFACE; IRRADIATION; ALGORITHMS; DEPENDENCE; DENSITY; SIO2 AB A fully coupled thermomechanical model of the nanoscale deformation in amorphous SiO2 due to laser heating is presented. Direct measurement of the transient, nonuniform temperature profiles was used to first validate a nonlinear thermal transport model. Densification due to structural relaxation above the glass transition point was modeled using the Tool-Narayanaswamy (TN) formulation for the evolution of structural relaxation times and fictive temperature. TN relaxation parameters were derived from spatially resolved confocal Raman scattering measurements of SiOSi stretching mode frequencies. Together, these thermal and microstructural data were used to simulate fictive temperatures which are shown to scale nearly linearly with density, consistent with previous measurements from Shelby et al. Volumetric relaxation coupled with thermal expansion occurring in the liquid-like and solid-like glassy states lead to residual stresses and permanent deformation which could be quantified. However, experimental surface deformation profiles between 1700 and 2000 K could only be reconciled with our simulation by assuming a roughly 2 x larger liquid thermal expansion for a-SiO2 with a temperature of maximum density 150 K higher than previously estimated by Bruckner et al. Calculated stress fields agreed well with recent laser-induced critical fracture measurements, demonstrating accurate material response prediction under processing conditions of practical interest. C1 [Vignes, Ryan M.; Soules, Thomas F.; Stolken, James S.; Settgast, Randolph R.; Elhadj, Selim; Matthews, Manyalibo J.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. RP Matthews, MJ (reprint author), Lawrence Livermore Natl Lab, 7000 East Ave, Livermore, CA 94550 USA. EM ibo@llnl.gov FU U.S. Department of Energy by Lawrence Livermore National Laboratory [DE-AC52-07NA27344] 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. NR 50 TC 23 Z9 23 U1 3 U2 48 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0002-7820 J9 J AM CERAM SOC JI J. Am. Ceram. Soc. PD JAN PY 2013 VL 96 IS 1 BP 137 EP 145 DI 10.1111/jace.12110 PG 9 WC Materials Science, Ceramics SC Materials Science GA 066XC UT WOS:000313254300021 ER PT J AU Yeo, K Romps, DM AF Yeo, Kyongmin Romps, David M. TI Measurement of Convective Entrainment Using Lagrangian Particles SO JOURNAL OF THE ATMOSPHERIC SCIENCES LA English DT Article ID SIMULATED CUMULUS ENSEMBLE; ICE-PHASE MICROPHYSICS; LARGE-EDDY SIMULATION; BOUNDARY-LAYER; DISPERSION; CLOUD; MODEL; PARAMETERIZATION; BUDGET; LES AB Lagrangian particle tracking is used in a large-eddy simulation to study an individual cumulus congestus. This allows for the direct measurement of the convective entrainment rate and of the residence times of entrained parcels within the cloud. The entrainment rate obtained by Lagrangian direct measurement is found to be higher than that obtained using the recently introduced method of Eulerian direct measurement. This discrepancy is explained by the fast recirculation of air in and out of cloudy updrafts, which Eulerian direct measurement is unable to resolve. By filtering these fast recirculations, the Lagrangian calculation produces a result in very good agreement with the Eulerian calculation. The Lagrangian method can also quantify some aspects of entrainment that cannot be probed with Eulerian methods. For instance, it is found that more than half of the air that is entrained by the cloud during its lifetime is air that was previously detrained by the cloud. Nevertheless, the cloud is highly diluted by entrained air: for cloudy air above 2 km, its mean height of origin is well above the cloud base. This paints a picture of a cloud that rapidly entrains both environmental air and its own detritus. C1 [Yeo, Kyongmin] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, Berkeley, CA 94720 USA. Univ Calif Berkeley, Dept Earth & Planetary Sci, Berkeley, CA 94720 USA. RP Yeo, K (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, 1 Cyclotron Rd, Berkeley, CA 94720 USA. EM kyeo@lbl.gov RI Romps, David/F-8285-2011 FU Laboratory Directed Research and Development Program of Lawrence Berkeley National Laboratory under U.S. Department of Energy [DE-AC02-05CH11231]; Office of Science, Office of Biological and Environmental Research of the U.S. Department of Energy [DE-AC02-05CH11231]; Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]; National Science Foundation [OCI-1053575] FX This work was supported by the Laboratory Directed Research and Development Program of Lawrence Berkeley National Laboratory under U.S. Department of Energy Contract DE-AC02-05CH11231. This research was also supported in part by the director, Office of Science, Office of Biological and Environmental Research of the U.S. Department of Energy under Contract DE-AC02-05CH11231 as part of their Atmospheric System Research Program. This research used computing resources of the National Energy Research Scientific Computing Center (NERSC), which is supported by the Office of Science of the U.S. Department of Energy under Contract DE-AC02-05CH11231, and computing resources of the Extreme Science and Engineering Discovery Environment (XSEDE), which is supported by National Science Foundation Grant OCI-1053575. Feedback from three anonymous reviewers helped improve this manuscript. NR 24 TC 11 Z9 11 U1 0 U2 21 PU AMER METEOROLOGICAL SOC PI BOSTON PA 45 BEACON ST, BOSTON, MA 02108-3693 USA SN 0022-4928 J9 J ATMOS SCI JI J. Atmos. Sci. PD JAN PY 2013 VL 70 IS 1 BP 266 EP 277 DI 10.1175/JAS-D-12-0144.1 PG 12 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA 068KH UT WOS:000313365100017 ER PT J AU Sirimamilla, PA Furmanski, J Rimnac, CM AF Sirimamilla, P. Abhiram Furmanski, Jevan Rimnac, Clare M. TI Application of viscoelastic fracture model and non-uniform crack initiation at clinically relevant notches in crosslinked UHMWPE SO JOURNAL OF THE MECHANICAL BEHAVIOR OF BIOMEDICAL MATERIALS LA English DT Article ID MOLECULAR-WEIGHT POLYETHYLENE; TOTAL JOINT REPLACEMENTS; ACETABULAR LINERS; THERMOMECHANICAL BEHAVIOR; FATIGUE RESISTANCE; PROPAGATION; POLYMERS; CRITERIA; STERILIZATION; DEFORMATION AB The mechanism of crack initiation from a clinically relevant notch is not well-understood for crosslinked ultra high molecular weight polyethylene (UHMWPE) used in total joint replacement components. Static mode driving forces, rather than the cyclic mode conditions typically associated with fatigue processes, have been shown to drive crack propagation in this material. Thus, in this study, crack initiation in a notched specimen under a static load was investigated. A video microscope was used to monitor the notch surface of the specimen and crack initiation time was measured from the video by identifying the onset of crack initiation at the notch. Crack initiation was considered using a viscoelastic fracture theory. It was found that the mechanism of crack initiation involved both single layer and a distributed multi-layer phenomenon and that multi-layer crack initiation delayed the crack initiation time for all loading conditions examined. The findings of this study support that the viscoelastic fracture theory governs fracture mechanics in crosslinked UHMWPE. The findings also support that crack initiation from a notch in UHMWPE is a more complex phenomenon than treated by traditional fracture theories for polymers. (C) 2012 Elsevier Ltd. All rights reserved. C1 [Sirimamilla, P. Abhiram; Rimnac, Clare M.] Case Western Reserve Univ, Dept Mech & Aerosp Engn, Cleveland, OH 44106 USA. [Furmanski, Jevan] Los Alamos Natl Lab, Struct Property Relat Grp, Los Alamos, NM USA. RP Rimnac, CM (reprint author), Case Western Reserve Univ, Dept Mech & Aerosp Engn, Cleveland, OH 44106 USA. EM clare.rimnac@case.edu FU NIAMS NIH HHS [R01 AR047192, T32AR00750, T32 AR007505, R01AR047192] NR 41 TC 1 Z9 1 U1 2 U2 20 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 1751-6161 EI 1878-0180 J9 J MECH BEHAV BIOMED JI J. Mech. Behav. Biomed. Mater. PD JAN PY 2013 VL 17 BP 11 EP 21 DI 10.1016/j.jmbbm.2012.07.008 PG 11 WC Engineering, Biomedical; Materials Science, Biomaterials SC Engineering; Materials Science GA 066OP UT WOS:000313230400002 PM 23127638 ER PT J AU McKenna, SA Vugrin, ED Hart, DB Aumer, R AF McKenna, Sean A. Vugrin, Eric D. Hart, David B. Aumer, Robert TI Multivariate Trajectory Clustering for False Positive Reduction in Online Event Detection SO JOURNAL OF WATER RESOURCES PLANNING AND MANAGEMENT-ASCE LA English DT Article DE Water quality; Event detection; Trajectory clustering; Contaminant warning system AB Online monitoring of multivariate water quality data is becoming a practical means of improving distribution network management and meeting water security goals. Changes in water quality are often due to changes in the hydraulic operations of the network. These operational changes create patterns of water quality change that are similar, but not exactly the same, from one instance to the next. Classification of multivariate change patterns through trajectory clustering is introduced in this paper to create a pattern library from historical water quality data and as an online process with the goal of reducing false positive water quality event detections. Prior to event declaration, a short sequence of the preceding multivariate data is compared against the pattern library to assess its similarity to a previously observed pattern. A fuzzy clustering algorithm is utilized to assign multivariate pattern memberships for water quality patterns associated with water quality events in both the offline and online modes of operation. The utility of trajectory clustering for multivariate pattern recognition in time-series data is demonstrated with two example applications. The first example uses observed water quality with simulated patterns and events. The pattern matching reduces the number of false positive event detections by 91% relative to the case of not using the pattern matching. The same false positive event reduction is achieved when both patterns and separate water quality events are added and 100% event detection is achieved. The second example uses observed water quality data from a metropolitan distribution system in the United States. The pattern matching approach developed in this paper is able to reduce the false positive event detections by 68%. DOI: 10.1061/(ASCE)WR.1943-5452.0000240. (C) 2013 American Society of Civil Engineers. C1 [McKenna, Sean A.; Hart, David B.; Aumer, Robert] Sandia Natl Labs, Natl Secur Applicat Dept, Albuquerque, NM 87185 USA. [Vugrin, Eric D.] Sandia Natl Labs, Resilience & Regulatory Effects Dept, Albuquerque, NM 87185 USA. RP McKenna, SA (reprint author), Sandia Natl Labs, Natl Secur Applicat Dept, POB 5800,MS 0751, Albuquerque, NM 87185 USA. EM samcken@sandia.gov FU U.S. EPA [DW89921928]; Singapore National Water Authority (PUB); U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX This work was performed under interagency agreement DW89921928 with the U.S. EPA and under contract with the Singapore National Water Authority (PUB). 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. The authors appreciate the efforts of three anonymous reviewers that greatly improved this paper. NR 23 TC 2 Z9 3 U1 0 U2 20 PU ASCE-AMER SOC CIVIL ENGINEERS PI RESTON PA 1801 ALEXANDER BELL DR, RESTON, VA 20191-4400 USA SN 0733-9496 J9 J WATER RES PL-ASCE JI J. Water Resour. Plan. Manage.-ASCE PD JAN-FEB PY 2013 VL 139 IS 1 BP 3 EP 12 DI 10.1061/(ASCE)WR.1943-5452.0000240 PG 10 WC Engineering, Civil; Water Resources SC Engineering; Water Resources GA 068GL UT WOS:000313354200002 ER PT J AU Shabalovskaya, SA Siegismund, D Heurich, E Rettenmayr, M AF Shabalovskaya, Svetlana A. Siegismund, Daniel Heurich, Erik Rettenmayr, Markus TI Evaluation of wettability and surface energy of native Nitinol surfaces in relation to hemocompatibility SO MATERIALS SCIENCE & ENGINEERING C-MATERIALS FOR BIOLOGICAL APPLICATIONS LA English DT Article DE Nitinol; Contact angle; Wettability; Surface energy ID PROTEIN ADSORPTION; MEDICAL APPLICATIONS; CONTACT-ANGLE; SHAPE-MEMORY; TITANIUM; ALLOYS; NICKEL; WIRES; BIOCOMPATIBILITY; ACTIVATION AB In the present study the dependence of Nitinol contact angles and surface energy on surface treatment is explored in order to better understand the material hemocompatibility that was evaluated in our previous studies. It is found that in the group of surfaces: (1) mechanically polished, (2) additionally heat treated, (3) chemically etched, and (4) additionally boiled in water, and (5) further heat treated, the contact angle could vary in the 50 degrees-80 degrees hydrophobic range and the total surface free energy in the 34-53 mN/m range. The polar surface energy, varying from 5 to 29 mN/m, constitutes a decisive contribution to the total energy change, and it seems to be a direct function of the Nitinol surface chemistry. Based on the complex analysis of surface energy together with the earlier results on electrochemistry and hemocompatibility it is concluded that the alteration of the polar component of surface energy and thrombogenicity is due to changes of the electron-acceptor/electron-donor character of native Nitinol surfaces during surface treatments. (c) 2012 Elsevier By. All rights reserved. C1 [Shabalovskaya, Svetlana A.] Iowa State Univ, Ames Lab DOE, Ames, IA 50011 USA. [Shabalovskaya, Svetlana A.; Siegismund, Daniel; Heurich, Erik; Rettenmayr, Markus] Univ Jena, Inst Mat Sci & Technol, D-07743 Jena, Germany. [Siegismund, Daniel] Univ Jena, Dept Bioinformat, D-07743 Jena, Germany. RP Rettenmayr, M (reprint author), Univ Jena, Inst Mat Sci & Technol, Lobdergraben 32, D-07743 Jena, Germany. EM M.Rettenmayr@uni-jena.de FU Iowa State University of Science and Technology [DE-AC02-07CH11358]; U.S. Department of Energy; Jena School for Microbial Communication (JSMC) FX The authors would like to thank McD Schetky and Paul Adler for providing the material for the studies, as well as to acknowledge K.D. Jandt and B. Harmon for their interest in the study. This manuscript has been also authored by the Iowa State University of Science and Technology under Contract No. DE-AC02-07CH11358 with the U.S. Department of Energy. One of the authors (D.S.) acknowledges financial support by the Jena School for Microbial Communication (JSMC). NR 44 TC 9 Z9 10 U1 4 U2 39 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0928-4931 EI 1873-0191 J9 MAT SCI ENG C-MATER JI Mater. Sci. Eng. C-Mater. Biol. Appl. PD JAN 1 PY 2013 VL 33 IS 1 BP 127 EP 132 DI 10.1016/j.msec.2012.08.018 PG 6 WC Materials Science, Biomaterials SC Materials Science GA 065NP UT WOS:000313155500019 PM 25428053 ER PT J AU Sercu, B Jones, ADG Wu, CH Escobar, MH Serlin, CL Knapp, TA Andersen, GL Holden, PA AF Sercu, Bram Jones, Antony D. G. Wu, Cindy H. Escobar, Mauricio H. Serlin, Carol L. Knapp, Timothy A. Andersen, Gary L. Holden, Patricia A. TI The Influence of In Situ Chemical Oxidation on Microbial Community Composition in Groundwater Contaminated with Chlorinated Solvents SO MICROBIAL ECOLOGY LA English DT Article ID FRACTURED BASALT AQUIFER; REDUCTIVE DECHLORINATION; DNAPL SOURCE; COMETABOLIC DEGRADATION; PERMANGANATE OXIDATION; RIBOSOMAL DNA; TRICHLOROETHENE; BACTERIA; DIVERSITY; SEDIMENT AB In situ chemical oxidation with permanganate has become an accepted remedial treatment for groundwater contaminated with chlorinated solvents. This study focuses on the immediate and short-term effects of sodium permanganate (NaMnO4) on the indigenous subsurface microbial community composition in groundwater impacted by trichloroethylene (TCE). Planktonic and biofilm microbial communities were studied using groundwater grab samples and reticulated vitreous carbon passive samplers, respectively. Microbial community composition was analyzed by terminal restriction fragment length polymorphism and a high-density phylogenetic microarray (PhyloChip). Significant reductions in microbial diversity and biomass were shown during NaMnO4 exposure, followed by recovery within several weeks after the oxidant concentrations decreased to < 1 mg/L. Bray-Curtis similarities and nonmetric multidimensional scaling showed that microbial community composition before and after NaMnO4 was similar, when taking into account the natural variation of the microbial communities. Also, 16S rRNA genes of two reductive dechlorinators (Desulfuromonas spp. and Sulfurospirillum spp.) and diverse taxa capable of cometabolic TCE oxidation were detected in similar quantities by PhyloChip across all monitoring wells, irrespective of NaMnO4 exposure and TCE concentrations. However, minimal biodegradation of TCE was observed in this study, based on oxidized conditions, concentration patterns of chlorinated and nonchlorinated hydrocarbons, geochemistry, and spatiotemporal distribution of TCE-degrading bacteria. C1 [Sercu, Bram; Holden, Patricia A.] Univ Calif Santa Barbara, Earth Res Inst, Santa Barbara, CA 93106 USA. [Sercu, Bram; Holden, Patricia A.] Univ Calif Santa Barbara, Donald Bren Sch Environm Sci & Management, Santa Barbara, CA 93106 USA. [Jones, Antony D. G.; Serlin, Carol L.; Knapp, Timothy A.] ENVIRON Int Corp, Irvine, CA 92612 USA. [Wu, Cindy H.; Andersen, Gary L.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, Berkeley, CA 94720 USA. [Escobar, Mauricio H.] ENVIRON Int Corp, Los Angeles, CA 90017 USA. RP Sercu, B (reprint author), Cty Ventura, Watershed Protect Dist, 800 S Victoria Ave, Ventura, CA 93006 USA. EM Bram.Sercu@Ventura.org RI Andersen, Gary/G-2792-2015 OI Andersen, Gary/0000-0002-1618-9827 FU US Department of Energy by the University of California, Lawrence Berkeley National Laboratory [DE-AC02-05CH11231] FX Microbiological field research and molecular analysis of field samples was performed by UCSB, and PhyloChip analysis was performed by the Lawrence Berkeley National Laboratory, through a research contract with ENVIRON International Corporation. Part of the work at Lawrence Berkeley National Laboratory was performed under the auspices of the US Department of Energy by the University of California, Lawrence Berkeley National Laboratory, under Contract DE-AC02-05CH11231. Groundwater sampling with geochemical analysis was performed by ENVIRON International Corporation through a private contract. The authors acknowledge the help of Annie Corbett and Kevin Huniu for field sampling and laboratory analysis. NR 54 TC 9 Z9 9 U1 5 U2 67 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 0095-3628 J9 MICROB ECOL JI Microb. Ecol. PD JAN PY 2013 VL 65 IS 1 BP 39 EP 49 DI 10.1007/s00248-012-0092-0 PG 11 WC Ecology; Marine & Freshwater Biology; Microbiology SC Environmental Sciences & Ecology; Marine & Freshwater Biology; Microbiology GA 068MD UT WOS:000313369900005 PM 22864851 ER PT J AU Costa, R Keller-Costa, T Gomes, NCM da Rocha, UN van Overbeek, L van Elsas, JD AF Costa, Rodrigo Keller-Costa, Tina Gomes, Newton C. M. da Rocha, Ulisses Nunes van Overbeek, Leo van Elsas, Jan Dirk TI Evidence for Selective Bacterial Community Structuring in the Freshwater Sponge Ephydatia fluviatilis SO MICROBIAL ECOLOGY LA English DT Article ID 16S RIBOSOMAL-RNA; PHYLOGENETIC DIVERSITY; MARINE SPONGES; PSEUDOCERATINA-CLAVATA; NUCLEOTIDE-SEQUENCES; MICROBIAL COMMUNITY; PSEUDOMONAS; RHIZOSPHERE; SYMBIONTS; SOIL AB To understand the functioning of sponges, knowledge of the structure of their associated microbial communities is necessary. However, our perception of sponge-associated microbiomes remains mainly restricted to marine ecosystems. Here, we report on the molecular diversity and composition of bacteria in the freshwater sponge Ephydatia fluviatilis inhabiting the artificial lake Vinkeveense Plassen, Utrecht, The Netherlands. Polymerase chain reaction-denaturing gradient gel electrophoresis (PCR-DGGE) fingerprints revealed that the apparent diversities within the domain Bacteria and the phylum Actinobacteria were lower in E. fluviatilis than in bulk water. Enrichment of specific PCR-DGGE bands in E. fluviatilis was detected. Furthermore, sponge- and bulk water-derived bacterial clone libraries differed with respect to bacterial community composition at the phylum level. E. fluviatilis-derived sequences were affiliated with six recognized phyla, i.e., Proteobacteria, Planctomycetes, Actinobacteria, Bacteroidetes, Chlamydiae and Verrucomicrobia, in order of relative abundance; next to the uncultured candidate phylum TM7 and one deeply rooted bacterial lineage of undefined taxonomy (BLUT). Actinobacteria, Proteobacteria, and Bacteroidetes were the dominant bacterial phyla in the freshwater clone library whereas sequences affiliated with Planctomycetes, Verrucomicrobia, Acidobacteria and Armatimonadetes were found at lower frequencies. Fine-tuned phylogenetic inference showed no or negligible overlaps between the E. fluviatilis and water-derived phylotypes within bacterial taxa such as Alphaproteobacteria, Bacteroidetes and Actinobacteria. We also ascertained the status of two alphaproteobacterial lineages as freshwater sponge-specific phylogenetic clusters, and report on high distinctiveness of other E. fluviatilis specific phylotypes, especially within the Bacteroidetes, Planctomycetes and Chlamydia taxa. This study supports the contention that the composition and diversity of bacteria in E. fluviatilis is partially driven by the host organism. C1 [Costa, Rodrigo] Univ Algarve, Ctr Marine Sci CCMAR CIMAR, Microbial Ecol & Evolut Res Grp, P-8005139 Faro, Portugal. [Keller-Costa, Tina] Univ Algarve, Ctr Marine Sci CCMAR CIMAR, P-8005139 Faro, Portugal. [Gomes, Newton C. M.] Univ Aveiro, CESAM, P-3810193 Aveiro, Portugal. [Gomes, Newton C. M.] Univ Aveiro, Dept Biol, P-3810193 Aveiro, Portugal. [da Rocha, Ulisses Nunes] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Ctr Environm Biotechnol, Berkeley, CA 94720 USA. [van Overbeek, Leo] Plant Res Int, Wageningen, Netherlands. [van Elsas, Jan Dirk] Univ Groningen, Ctr Ecol & Evolutionary Studies, Dept Microbial Ecol, NL-9747 AG Groningen, Netherlands. RP Costa, R (reprint author), Univ Algarve, Ctr Marine Sci CCMAR CIMAR, Microbial Ecol & Evolut Res Grp, P-8005139 Faro, Portugal. EM rscosta@ualg.pt RI Keller Costa, Tina/M-6165-2013; Nunes da Rocha, Ulisses/M-7467-2013; Costa, Rodrigo/N-7274-2013; UALG, CCMAR/N-7071-2013; Gomes, Newton/F-7430-2012; CESAM, UA/M-3762-2015 OI Keller Costa, Tina/0000-0003-3702-9192; Nunes da Rocha, Ulisses/0000-0001-6972-6692; Costa, Rodrigo/0000-0002-5932-4101; Gomes, Newton/0000-0003-1934-0091; FU Soil Biotechnology Foundation; Portuguese Foundation of Science and Technology (FCT); Federation of European Microbiological Societies (FEMS) FX R. Costa was supported by the Soil Biotechnology Foundation and by the Portuguese Foundation of Science and Technology (FCT). T. Keller-Costa received a research fellowship from the Federation of European Microbiological Societies (FEMS) to perform this work. We thank Dr. Joana B.T. Xavier for the identification of the sponge specimens collected in this study. We are grateful to the late Niels Cox and Albert Ellens for their assistance during sampling. NR 60 TC 16 Z9 17 U1 1 U2 45 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 0095-3628 J9 MICROB ECOL JI Microb. Ecol. PD JAN PY 2013 VL 65 IS 1 BP 232 EP 244 DI 10.1007/s00248-012-0102-2 PG 13 WC Ecology; Marine & Freshwater Biology; Microbiology SC Environmental Sciences & Ecology; Marine & Freshwater Biology; Microbiology GA 068MD UT WOS:000313369900023 PM 22903086 ER PT J AU Farkas, ME Aanei, IL Behrens, CR Tong, GJ Murphy, ST O'Neil, JP Francis, MB AF Farkas, Michelle E. Aanei, Ioana L. Behrens, Christopher R. Tong, Gary J. Murphy, Stephanie T. O'Neil, James P. Francis, Matthew B. TI PET Imaging and Biodistribution of Chemically Modified Bacteriophage MS2 SO MOLECULAR PHARMACEUTICS LA English DT Article DE drug delivery; modified viruses; nanoparticles; PEGylation; protein modification; PET imaging ID COWPEA MOSAIC-VIRUS; FREE VIRAL CAPSIDS; IN-VIVO; GENETIC-CODE; CANCER-CELLS; NANOPARTICLES; DELIVERY; CARRIERS; PROTEIN; PHAGE AB The fields of nanotechnology and medicine have merged in the development of new imaging and drug delivery agents based on nanoparticle platforms. As one example, a mutant of bacteriophage MS2 can be differentially modified on the exterior and interior surfaces for the concurrent display of targeting functionalities and payloads, respectively. In order to realize their potential for use in in vivo applications, the biodistribution and circulation properties of this class of agents must first be investigated. A means of modulating and potentially improving the characteristics of nanoparticle agents is the appendage of PEG chains. Both MS2 and MS2-PEG capsids possessing interior DOTA chelators were labeled with Cu-64 and injected intravenously into mice possessing tumor xenografts. Dynamic imaging of the agents was performed using PET-CT on a single animal per sample, and the biodistribution at the terminal time point (24 h) was assessed by gamma counting of the organs ex vivo for 3 animals per agent. Compared to other viral capsids of similar size, the MS2 agents showed longer circulation times. Both MS2 and MS2-PEG bacteriophage behaved similarly, although the latter agent showed significantly less uptake in the spleen. This effect may be attributed to the ability of the PEG chains to mask the capsid charge. Although the tumor uptake of the agents may result from the enhanced permeation and retention (EPR) effect, selective tumor imaging may be achieved in the future by using exterior targeting groups. C1 [Farkas, Michelle E.; Aanei, Ioana L.; Behrens, Christopher R.; Tong, Gary J.; Francis, Matthew B.] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Murphy, Stephanie T.] Univ Calif San Francisco, Dept Radiol & Biomed Imaging, San Francisco, CA 94107 USA. [O'Neil, James P.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Life Sci, Berkeley, CA 94720 USA. [Francis, Matthew B.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. RP Francis, MB (reprint author), Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. EM mbfrancis@berkeley.edu FU DOD Breast Cancer Research Program [BC061995]; DOD BCRP Grant [BC100159]; UC Berkeley Chemical Biology Graduate Program (Genentech Fellowship); DOE California Alliance for Radiotracer Education Grant [DESC0002061]; UC Berkeley Chemical Biology Graduate Program [1 T32 GMO66698] FX These studies were generously supported by the DOD Breast Cancer Research Program (BC061995). M.E.F. was supported by DOD BCRP Grant BC100159, and C.R.B. and I.LA. were supported by the UC Berkeley Chemical Biology Graduate Program (Genentech Fellowship). C.R.B. was supported by DOE California Alliance for Radiotracer Education Grant DESC0002061 and the UC Berkeley Chemical Biology Graduate Program (Training Grant 1 T32 GMO66698). The authors would like to thank Youngho Seo, Ph.D., for helpful discussions, and Byron Hann, M.D., Ph.D., and the UCSF Preclinical Therapeutics Core for assistance with the generation of tumored animals and MCF7cl18 cells. Nick Vandehey is gratefully acknowledged for his assistance with 64Cu handling and for many helpful discussions. Stacy Capehart is thanked for assistance with DLS studies. NR 35 TC 25 Z9 25 U1 5 U2 48 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 1543-8384 J9 MOL PHARMACEUT JI Mol. Pharm. PD JAN PY 2013 VL 10 IS 1 BP 69 EP 76 DI 10.1021/mp3003754 PG 8 WC Medicine, Research & Experimental; Pharmacology & Pharmacy SC Research & Experimental Medicine; Pharmacology & Pharmacy GA 065NV UT WOS:000313156100010 PM 23214968 ER PT J AU Berg, LK Gustafson, WI Kassianov, EI Deng, LP AF Berg, Larry K. Gustafson, William I., Jr. Kassianov, Evgueni I. Deng, Liping TI Evaluation of a Modified Scheme for Shallow Convection: Implementation of CuP and Case Studies SO MONTHLY WEATHER REVIEW LA English DT Article ID BOUNDARY-LAYER; PART I; PARAMETERIZATION; DISTRIBUTIONS; VARIABILITY; NCAR; SITE AB A new treatment for shallow clouds has been introduced into the Weather Research and Forecasting Model (WRF). The new scheme, called the cumulus potential (CuP) scheme, replaces the ad hoc trigger function used in the Kain-Fritsch cumulus parameterization with a trigger function related to the distribution of temperature and humidity in the convective boundary layer via probability density functions (PDFs). An additional modification to the default version of WRF is the computation of a cumulus cloud fraction based on the time scales relevant for shallow cumuli. Results from three case studies over the U. S. Department of Energy's Atmospheric Radiation Measurement (ARM) site in north-central Oklahoma are presented. These cases were selected because of the presence of shallow cumuli over the ARM site. The modified version of WRF does a much better job predicting the cloud fraction and the downwelling shortwave irradiance than control simulations utilizing the default Kain-Fritsch scheme. The modified scheme includes a number of additional free parameters, including the number and size of bins used to define the PDF, the minimum frequency of a bin within the PDF before that bin is considered for shallow clouds to form, and the critical cumulative frequency of bins required to trigger deep convection. A series of tests were undertaken to evaluate the sensitivity of the simulations to these parameters. Overall, the scheme was found to be relatively insensitive to each of the parameters. C1 [Berg, Larry K.; Gustafson, William I., Jr.; Kassianov, Evgueni I.; Deng, Liping] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Berg, LK (reprint author), POB 999,K9-30, Richland, WA 99352 USA. EM larry.berg@pnl.gov RI Gustafson, William/A-7732-2008; Berg, Larry/A-7468-2016 OI Gustafson, William/0000-0001-9927-1393; Berg, Larry/0000-0002-3362-9492 FU Office of Biological and Environmental Research (OBER) of the U.S. Department of Energy (DOE); DOE [DE-A06-76RLO 1830] FX We thank Dr. Richard Easter for numerous discussions related to this work and Dr. Minghuai Wang for his careful review of an earlier version of the manuscript. This work has been supported by the Office of Biological and Environmental Research (OBER) of the U.S. Department of Energy (DOE) as part of the Atmospheric Radiation Measurement (ARM) and Atmospheric System Research (ASR) Programs. The Pacific Northwest National Laboratory (PNNL) is operated by Battelle for the DOE under Contract DE-A06-76RLO 1830. A portion of the research was performed using PNNL Institutional Computing. NR 26 TC 10 Z9 13 U1 0 U2 10 PU AMER METEOROLOGICAL SOC PI BOSTON PA 45 BEACON ST, BOSTON, MA 02108-3693 USA SN 0027-0644 J9 MON WEATHER REV JI Mon. Weather Rev. PD JAN PY 2013 VL 141 IS 1 BP 134 EP 147 DI 10.1175/MWR-D-12-00136.1 PG 14 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA 064MH UT WOS:000313078900007 ER PT J AU Lang, MR He, L Kou, XF Upadhyaya, P Fan, YB Chu, H Jiang, Y Bardarson, JH Jiang, WJ Choi, ES Wang, Y Yeh, NC Moore, J Wang, KL AF Lang, Murong He, Liang Kou, Xufeng Upadhyaya, Pramey Fan, Yabin Chu, Hao Jiang, Ying Bardarson, Jens H. Jiang, Wanjun Choi, Eun Sang Wang, Yong Yeh, Nai-Chang Moore, Joel Wang, Kang L. TI Competing Weak Localization and Weak Antilocalization in Ultrathin Topological Insulators SO NANO LETTERS LA English DT Article DE Topological insulator; ambipolar effect; surface states hybridization; ultrathin films; weak localization; weak antilocalization ID SURFACE-STATES; BI2SE3; NANORIBBONS; CONDUCTION; TRANSPORT; BI2TE3; LIMIT AB We demonstrate evidence of a surface gap opening in topological insulator (TI) thin films of (Bi0.57Sb0.43)(2)Te-3 below six quintuple layers through transport and scanning tunneling spectroscopy measurements. By effective tuning the Fermi level via gate-voltage control, we unveil a striking competition between weak localization and weak antilocalization at low magnetic fields in nonmagnetic ultrathin films, possibly owing to the change of the net Berry phase. Furthermore, when the Fermi level is swept into the surface gap of ultrathin samples, the overall unitary behaviors are revealed at higher magnetic fields, which are in contrast to the pure WAL signals obtained in thicker films. Our findings show an exotic phenomenon characterizing the gapped TI surface states and point to the future realization of quantum spin Hall effect and dissipationless TI-based applications. C1 [Lang, Murong; He, Liang; Kou, Xufeng; Upadhyaya, Pramey; Fan, Yabin; Jiang, Wanjun; Wang, Kang L.] Univ Calif Los Angeles, Dept Elect Engn, Los Angeles, CA 90095 USA. [Bardarson, Jens H.; Moore, Joel] Univ Calif Berkeley, Dept Phys, Berkeley, CA 94720 USA. [Bardarson, Jens H.; Moore, Joel] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. [Jiang, Ying; Wang, Yong] Zhejiang Univ, Dept Mat Sci & Engn, Ctr Elect Microscopy, State Key Lab Silicon Mat, Hangzhou 310027, Zhejiang, Peoples R China. [Chu, Hao; Yeh, Nai-Chang] CALTECH, Dept Phys, Pasadena, CA 91125 USA. [Choi, Eun Sang] Natl High Magnet Field Lab, Tallahassee, FL 32310 USA. RP He, L (reprint author), Univ Calif Los Angeles, Dept Elect Engn, Los Angeles, CA 90095 USA. EM heliang@ee.ucla.edu; wang@ee.ucla.edu RI He, Liang/E-5935-2012; Jiang, Wanjun/E-6994-2011; Wang, Yong/A-7766-2010; Moore, Joel/O-4959-2016; OI Jiang, Wanjun/0000-0003-0918-3862; Wang, Yong/0000-0002-9893-8296; Moore, Joel/0000-0002-4294-5761; Kou, Xufeng/0000-0002-8860-5105 FU Defense Advanced Research Projects Agency (DARPA); Focus Center Research Program-Center on Functional Engineered Nano Architectonics (FENA); NSF [DMR-0654118]; State of Florida; Department of Energy (DOE); Natural Science Foundation of China [11174244]; Zhejiang Provincial Natural Science Foundation of China [LR12A04002]; National Young 1000 Talents Plan FX The authors acknowledge helpful discussions with R. Mong from UC Berkeley and technical support from X. Yu, M. Wang, J. Tang, and L. Chang from the Device Research Laboratory at UCLA. This work was in part supported by Defense Advanced Research Projects Agency (DARPA), Focus Center Research Program-Center on Functional Engineered Nano Architectonics (FENA). A portion of this work was performed at the National High Magnetic Field Laboratory, which is supported by NSF Cooperative Agreement No. DMR-0654118, by the State of Florida, and by the Department of Energy (DOE). Y.W. acknowledges the support from Natural Science Foundation of China (11174244) and Zhejiang Provincial Natural Science Foundation of China (LR12A04002) and National Young 1000 Talents Plan. NR 46 TC 44 Z9 44 U1 9 U2 133 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 1530-6984 J9 NANO LETT JI Nano Lett. PD JAN PY 2013 VL 13 IS 1 BP 48 EP 53 DI 10.1021/nl303424n PG 6 WC Chemistry, Multidisciplinary; Chemistry, Physical; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied; Physics, Condensed Matter SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA 065IP UT WOS:000313142300009 PM 23198980 ER PT J AU Choi, S Deslippe, J Capaz, RB Louie, SG AF Choi, SangKook Deslippe, Jack Capaz, Rodrigo B. Louie, Steven G. TI An Explicit Formula for Optical Oscillator Strength of Excitons in Semiconducting Single-Walled Carbon Nanotubes: Family Behavior SO NANO LETTERS LA English DT Article DE Single-walled carbon nanotubes; extended Hubbard model; oscillator strength; family behavior; GW approximation; Bethe-Salpeter equation ID QUASI-PARTICLE ENERGIES; INSULATORS; SPECTRA AB The sensitive structural dependence of the optical properties of single-walled carbon nanotubes, which are dominated by excitons and tunable by changing diameter and chirality, makes them excellent candidates for optical devices. Because of strong many-electron interaction effects, the detailed dependence of the optical oscillator strength f(s) of excitons on nanotube diameter d, chiral angle theta, and electronic subband index P (the so-called family behavior), however, has been unclear. In this study, based on results from an extended Hubbard Hamiltonian with parameters derived from ab initio GW plus Bethe-Salpeter equation (GW-BSE) calculations, we have obtained an explicit formula for the family behavior of the oscillator strengths of excitons in semiconducting single-walled carbon nanotubes (SWCNTs), incorporating environmental screening. The formula explains recent measurements well and is expected to be useful in the understanding and design of possible SWCNT optical and optoelectronic devices. C1 [Choi, SangKook; Deslippe, Jack; Capaz, Rodrigo B.; Louie, Steven G.] Univ Calif Berkeley, Dept Phys, Berkeley, CA 94720 USA. [Choi, SangKook; Deslippe, Jack; Capaz, Rodrigo B.; Louie, Steven G.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. [Capaz, Rodrigo B.] Univ Fed Rio de Janeiro, Inst Fis, BR-21941972 Rio De Janeiro, Brazil. [Capaz, Rodrigo B.] Inst Nacl Metrol Normalizacao & Qualidade Ind INM, Div Mat Metrol, BR-25250020 Rio De Janeiro, RJ, Brazil. RP Louie, SG (reprint author), Univ Calif Berkeley, Dept Phys, Berkeley, CA 94720 USA. RI B, Rodrigo/N-7595-2014 FU ASCR Office in the DOE Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division, U.S. Department of Energy [DE-AC02-05CH11231]; National Science Foundation [DMR10-1006184]; Samsung Foundation; CNPq; FAPERJ; INCT-Nanomateriais de Carbono FX We thank F. Wang, K. Liu, and X. Hong for providing the experimental data. Ab initio GW-BSE calculations were supported by the Director, the ASCR Office in the DOE Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division, U.S. Department of Energy under Contract No. DE-AC02-05CH11231. Extended Hubbard model formulation and calculations were supported by the National Science Foundation Grant No. DMR10-1006184. S.C. acknowledges partial support from the Samsung Foundation. R.B.C. acknowledges financial support from Brazilian funding agencies CNPq, FAPERJ and INCT-Nanomateriais de Carbono. Computational resources were provided by NSF through TeraGrid resources at NICS and DOE at the Lawrence Berkeley National Laboratory's NERSC facility. NR 36 TC 9 Z9 9 U1 2 U2 45 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 1530-6984 EI 1530-6992 J9 NANO LETT JI Nano Lett. PD JAN PY 2013 VL 13 IS 1 BP 54 EP 58 DI 10.1021/nl303426q PG 5 WC Chemistry, Multidisciplinary; Chemistry, Physical; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied; Physics, Condensed Matter SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA 065IP UT WOS:000313142300010 PM 23210547 ER PT J AU van Schooten, KJ Huang, J Baker, WJ Talapin, DV Boehme, C Lupton, JM AF van Schooten, Kipp J. Huang, Jing Baker, William J. Talapin, Dmitri V. Boehme, Christoph Lupton, John M. TI Spin-Dependent Exciton Quenching and Spin Coherence in CdSe/CdS Nanocrystals SO NANO LETTERS LA English DT Article DE CdSe/CdS nanocrystals; spin coherence; electron-spin resonance; light harvesting; trap states; blinking ID CORE-SHELL NANOCRYSTALS; QUANTUM DOTS; MAGNETIC-RESONANCE; SURFACE TRAPS; RELAXATION; DYNAMICS; BLINKING; LIGHT; DARK; CDS AB Large surface-to-volume ratios of semiconductor nanocrystals cause susceptibility to charge trapping, which can modify luminescence yields and induce single-particle blinking. Optical spectroscopies cannot differentiate between bulk and surface traps in contrast to spin-resonance techniques, which in principle avail chemical information on such trap sites. Magnetic resonance detection via spin-controlled photoluminescence enables the direct observation of interactions between emissive excitons and trapped charges. This approach allows the discrimination of three radical species located in two functionally different trap states in CdSe/CdS nanocrystals, underlying the fluorescence quenching and thus blinking mechanisms: a spin-dependent Auger process in charged particles; and a charge-separated state pair process, which leaves the particle neutral. The paramagnetic trap centers offer control of the energy transfer yield from the wide-gap CdS to the narrow-gap CdSe, that is, light harvesting within the heterostructure. Coherent spin motion within the trap states of the CdS arms of nanocrystal tetrapods is reflected by spatially remote luminescence from CdSe cores with surprisingly long coherence times of >300 ns at 3.5 K, illustrating coherent control of light harvesting. C1 [van Schooten, Kipp J.; Baker, William J.; Boehme, Christoph; Lupton, John M.] Univ Utah, Dept Phys & Astron, Salt Lake City, UT 84112 USA. [Huang, Jing; Talapin, Dmitri V.] Univ Chicago, Dept Chem, Chicago, IL 60637 USA. [Talapin, Dmitri V.] Argonne Natl Lab, Ctr Nanoscale Mat, Argonne, IL 60439 USA. [Lupton, John M.] Univ Regensburg, Inst Expt & Angew Phys, D-93040 Regensburg, Germany. RP Boehme, C (reprint author), Univ Utah, Dept Phys & Astron, 115 South 1400 East, Salt Lake City, UT 84112 USA. EM boehme@physics.utah.edu; john.lupton@physik.uni-regensburg.de FU Department of Energy [DESC0000909]; National Science Foundation through MRSEC [1121252, 0213745]; David and Lucile Packard Foundation; National Science Foundation CAREER [0953225, 0847535] FX An acknowledgment is made to the Department of Energy (Grant No. DESC0000909) for the funding of this research. We thank the National Science Foundation for support through MRSEC Projects Nos. 1121252 and 0213745. J.M.L. and D.V.T. are indebted to the David and Lucile Packard Foundation for providing fellowships. C.B. and D.V.T. acknowledge support by National Science Foundation CAREER grants (Nos. 0953225 and 0847535, respectively). NR 40 TC 10 Z9 10 U1 3 U2 123 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 1530-6984 EI 1530-6992 J9 NANO LETT JI Nano Lett. PD JAN PY 2013 VL 13 IS 1 BP 65 EP 71 DI 10.1021/nl303459a PG 7 WC Chemistry, Multidisciplinary; Chemistry, Physical; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied; Physics, Condensed Matter SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA 065IP UT WOS:000313142300012 PM 23189974 ER PT J AU Hughes, SM Alivisatos, AP AF Hughes, Steven M. Alivisatos, A. Paul TI Anisotropic Formation and Distribution of Stacking Faults in II-VI Semiconductor Nanorods SO NANO LETTERS LA English DT Article DE Nanocrystal; nanorod; stacking fault; CdSe; orientation; heterostructure ID NANOCRYSTAL QUANTUM DOTS; LIGHT-EMITTING-DIODES; CDSE NANOCRYSTALS; SHELL NANORODS; SEEDED-GROWTH; NANOHETEROSTRUCTURES; CDSE/CDS/ZNS; PERFORMANCE; POLYTYPISM; ENERGY AB Nanocrystals of cadmium selenide exhibit a form of polytypism with stable forms in both the wurtzite and zinc blende crystal structures. As a result, wurtzite nanorods of cadmium selenide tend to form stacking faults of zinc blende along the c-axis. These faults were found to preferentially form during the growth of the (001) face, which accounts for 40% of the rod's total length. Since II-VI semiconductor nanorods lack inversion symmetry along the c-axis of the particle, the two ends of the nanorod may be identified by this anisotropic distribution of faults. C1 Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. RP Hughes, SM (reprint author), Whitman Coll, Dept Chem, Walla Walla, WA 99362 USA. EM hughess2@whitman.edu RI Alivisatos , Paul /N-8863-2015 OI Alivisatos , Paul /0000-0001-6895-9048 FU Office of Science, Office of Basic Energy Sciences, of the United States Department of Energy [DE-AC02-05CH11231] FX The authors of this work would like to extend their thanks to H. Liu, B. Sadtler, D. Milliron, A. Mastroianni, P. Trudeau, and J. Owen for their indispensable conversations and constructive feedback throughout the development of this work. Part of the TEM work presented here was performed with a user grant at the National Center of Electron Microscopy (NCEM), which is funded by the Director, Office of Science, Office of Basic Energy Sciences, of the United States Department of Energy under contract DE-AC02-05CH11231. Work on stacking fault characterization by Steven Hughes and A. P. Alivisatos was supported by the Director, Office of Science, Office of Basic Energy Sciences, of the United States Department of Energy under contract DE-AC02-05CH11231. NR 32 TC 19 Z9 19 U1 4 U2 96 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 1530-6984 J9 NANO LETT JI Nano Lett. PD JAN PY 2013 VL 13 IS 1 BP 106 EP 110 DI 10.1021/nl3036417 PG 5 WC Chemistry, Multidisciplinary; Chemistry, Physical; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied; Physics, Condensed Matter SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA 065IP UT WOS:000313142300019 PM 23252712 ER PT J AU Qiao, ZA Guo, BK Binder, AJ Chen, JH Veith, GM Dai, S AF Qiao, Zhen-An Guo, Bingkun Binder, Andrew J. Chen, Jihua Veith, Gabriel M. Dai, Sheng TI Controlled Synthesis of Mesoporous Carbon Nanostructures via a "Silica-Assisted" Strategy SO NANO LETTERS LA English DT Article DE Mesoporous carbon nanospheres; hollow nanospheres; yolk-shell; silica-assisted; supercapacitors ID STOBER METHOD; ONE-STEP; NANOPARTICLES; SPHERES; NANOSPHERES; POLYMER; NANOCOMPOSITES; PARTICLES; CHEMISTRY; TEMPLATE AB We have established a facile and generalizable "silica-assisted" synthesis for diverse carbon spheres-a category that covers mesoporous carbon nanospheres, hollow mesoporous carbon nanospheres, and yolk-shell mesoporous carbon nanospheres-by using phenolic resols as a polymer precursor, silicate oligomers as an inorganic precursor, and hexadecyl trimethylammoniumchloride as a template. The particle sizes of the carbon nanospheres are uniform and easily controlled in a wide range of 180-850 nm by simply varying the ethanol concentrations. All three types of mesoporous carbon nanospheres have high surface areas and large pore volumes and exhibit promising properties for supercapacitors with high capacitance and favorable capacitance retention. C1 [Qiao, Zhen-An; Guo, Bingkun; Dai, Sheng] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. [Binder, Andrew J.; Dai, Sheng] Univ Tennessee, Dept Chem, Knoxville, TN 37996 USA. [Chen, Jihua] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. [Veith, Gabriel M.] Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. RP Dai, S (reprint author), Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. EM dais@ornl.gov RI Chen, Jihua/F-1417-2011; Guo, Bingkun/J-5774-2014; Dai, Sheng/K-8411-2015; OI Chen, Jihua/0000-0001-6879-5936; Dai, Sheng/0000-0002-8046-3931; Binder, Andrew/0000-0003-3221-2887; Qiao, Zhen-An/0000-0001-6064-9360 FU Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, US Department of Energy [DE-AC05-00OR22725]; Oak Ridge National Laboratory by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy; Materials Sciences and Engineering Division, Office of Basic Energy Sciences, U.S. Department of Energy; UT-Battelle, LLC (GMV-XPS) FX The research was sponsored by the Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, US Department of Energy, under contract no. DE-AC05-00OR22725 with Oak Ridge National Laboratory managed and operated by UT-Battelle, LLC. 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, and Materials Sciences and Engineering Division, Office of Basic Energy Sciences, U.S. Department of Energy under contract with UT-Battelle, LLC (GMV-XPS). NR 38 TC 86 Z9 87 U1 24 U2 401 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 1530-6984 J9 NANO LETT JI Nano Lett. PD JAN PY 2013 VL 13 IS 1 BP 207 EP 212 DI 10.1021/nl303889h PG 6 WC Chemistry, Multidisciplinary; Chemistry, Physical; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied; Physics, Condensed Matter SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA 065IP UT WOS:000313142300036 PM 23256449 ER PT J AU Sutter, P Lahiri, J Zahl, P Wang, B Sutter, E AF Sutter, P. Lahiri, J. Zahl, P. Wang, B. Sutter, E. TI Scalable Synthesis of Uniform Few-Layer Hexagonal Boron Nitride Dielectric Films SO NANO LETTERS LA English DT Article DE Layered materials; boron nitride; ultrathin dielectric films; thin film growth; reactive magnetron sputtering; tunneling ID CHEMICAL-VAPOR-DEPOSITION; HIGH-QUALITY; LARGE-AREA; GRAPHENE ELECTRONICS; HETEROSTRUCTURES; GROWTH; NANOSHEETS; SURFACES; DEVICE AB Two-dimensional or ultrathin layered materials are attracting broad interest in both fundamental science and applications. While exfoliation can provide high-quality single- and few-layer flakes with nanometer to micrometer size, the development of wafer-scale synthesis methods is important for realizing the full potential of ultrathin layered materials. Here we demonstrate the growth of high quality few-layer boron nitride (BN) films with controlled thickness by magnetron sputtering of B in N-2/Ar, a scalable process using only benign, nontoxic reagents. BN films up to two atomic layers are synthesized by reactive deposition at high substrate temperatures. Thicker monocrystalline BN films with an arbitrary number of atomic layers are achieved in a two-step process comprising cycles of alternating room temperature deposition and annealing. Tunneling transport across these BN films shows pinhole-free insulating behavior on mu m(2) scales, demonstrating the realization of high quality ultrathin dielectrics. C1 [Sutter, P.; Lahiri, J.; Zahl, P.; Sutter, E.] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. [Wang, B.] Vanderbilt Univ, Dept Phys & Astron, Nashville, TN 37235 USA. RP Sutter, P (reprint author), Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. RI Wang, Bin/E-8301-2011 OI Wang, Bin/0000-0001-8246-1422 FU U.S. Department of Energy, Office of Basic Energy Sciences [DE-AC02-98CH10886] FX This research has been 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. The authors thank Kim Kiss linger for technical support, and Dmytro Nykypanchuk for measuring UV-vis spectra. NR 49 TC 47 Z9 47 U1 16 U2 296 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 1530-6984 EI 1530-6992 J9 NANO LETT JI Nano Lett. PD JAN PY 2013 VL 13 IS 1 BP 276 EP 281 DI 10.1021/nl304080y PG 6 WC Chemistry, Multidisciplinary; Chemistry, Physical; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied; Physics, Condensed Matter SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA 065IP UT WOS:000313142300047 PM 23244762 ER PT J AU Galland, C Brovelli, S Bae, WK Padilha, LA Meinardi, F Klimov, VI AF Galland, Christophe Brovelli, Sergio Bae, Wan Ki Padilha, Lazaro A. Meinardi, Francesco Klimov, Victor I. TI Dynamic Hole Blockade Yields Two-Color Quantum and Classical Light from Dot-in-Bulk Nanocrystals SO NANO LETTERS LA English DT Article DE Dot-in-bulk nanocrystal quantum dots; single photon emitter; dynamic Coulomb blockade; single-dot spectroscopy ID SEMICONDUCTOR NANOCRYSTALS; BLINKING; CDSE AB Semiconductor nanocrystals (NCs) are an emerging class of color-tunable, solution-processable, room-temperature single-photon sources. Photon antibunching in NCs arises from suppression of rnultiphoton emission by nonradiative Auger recombination. Here, we demonstrate a new antibunching mechanism-dynamic Coulomb blockade-which allows for generating both quantum and classical light from the same NC without detrimental effects of Auger decay. This mechanism is realized in novel dot-in-bulk (DiB) nanostructures comprising a quantum-confined CdSe core overcoated with a thick, bulk-like CdS shell. The presence of one hole in the core suppresses the capture of the second hole forcing it to recombine in the shell region. Under weak excitation, these NCs emit red antibunched light (core emission). At higher pump levels they exhibit an additional green band (shell emission) with bulk-like, Poissonian photon statistics. The unusual versatility of these novel nanoscale light sources, that combine mutually correlated channels for quantum and classical emission and additionally allow for facile tunability of effective color, opens new interesting opportunities for a range of applications from quantum optics to sensing and nanoscale imaging. C1 [Galland, Christophe; Brovelli, Sergio; Bae, Wan Ki; Padilha, Lazaro A.; Klimov, Victor I.] Los Alamos Natl Lab, Div Chem, Los Alamos, NM 87545 USA. [Galland, Christophe; Brovelli, Sergio; Bae, Wan Ki; Padilha, Lazaro A.; Klimov, Victor I.] Los Alamos Natl Lab, Ctr Adv Solar Photophys, Los Alamos, NM 87545 USA. [Galland, Christophe] Univ Delaware, Dept Elect & Comp Engn, Newark, DE 19716 USA. [Brovelli, Sergio; Meinardi, Francesco] Univ Milano Bicocca, Dipartimento Sci Mat, I-20125 Milan, Italy. RP Klimov, VI (reprint author), Los Alamos Natl Lab, Div Chem, POB 1663, Los Alamos, NM 87545 USA. EM klimov@lanl.gov RI Galland, Christophe/A-1075-2013; Padilha, Lazaro/G-1523-2013; OI Galland, Christophe/0000-0001-5627-0796; Brovelli, Sergio/0000-0002-5993-855X; Klimov, Victor/0000-0003-1158-3179 FU Center for Advanced Solar Photophysics (CASP); Energy Frontier Research Center; U.S. Department of Energy (DOE), Office of Science (OS), Office of Basic Energy Sciences (BES); Chemical Sciences, Biosciences and Geosciences Division of BES, OS, DOE; Los Alamos National Laboratory Directed Research and Development Program FX C.G. and V.I.K. acknowledge support from the Center for Advanced Solar Photophysics (CASP), an Energy Frontier Research Center funded by the U.S. Department of Energy (DOE), Office of Science (OS), Office of Basic Energy Sciences (BES). W.K.B. is supported by the Chemical Sciences, Biosciences and Geosciences Division of BES, OS, DOE. S.B. is supported by the Los Alamos National Laboratory Directed Research and Development Program. Author contributions are as follows: W.K.B. synthesized and characterized the NC materials. CC., S.B., LAP., and F.M. performed the optical measurements. CC, S.B., and V.I.K. analyzed the data and wrote the manuscript. NR 29 TC 27 Z9 27 U1 1 U2 65 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 16TH ST, NW, WASHINGTON, DC 20036 USA SN 1530-6984 J9 NANO LETT JI Nano Lett. PD JAN PY 2013 VL 13 IS 1 BP 321 EP 328 DI 10.1021/nl3045316 PG 8 WC Chemistry, Multidisciplinary; Chemistry, Physical; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied; Physics, Condensed Matter SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA 065IP UT WOS:000313142300054 PM 23252581 ER PT J AU Roberts, NA Fowlkes, JD Magel, GA Rack, PD AF Roberts, Nicholas A. Fowlkes, Jason D. Magel, Gregory A. Rack, Philip D. TI Enhanced material purity and resolution via synchronized laser assisted electron beam induced deposition of platinum SO NANOSCALE LA English DT Article ID FABRICATION; PT(PF3)(4); PRECURSOR; GROWTH; REPAIR; NANOPILLARS; NANOTUBES; DEVICES; MASKS; FILMS AB We introduce a laser assisted electron beam induced deposition (LAEBID) process which is a nanoscale direct write synthesis method that integrates an electron beam induced deposition process with a synchronized pulsed laser step to induce thermal desorption of reaction by-products. Localized, spatially overlapping electron and photon pulses enable the thermal desorption of the reaction by-product while mitigating issues associated with bulk substrate heating, which can shorten the precursor residence time and distort pattern fidelity due to thermal drift. Current results demonstrate purification of platinum deposits (reduced carbon content by similar to 50%) with the addition of synchronized laser pulses as well as a significant reduction in deposit resistivity. Measured resistivities from platinum LAEBID structures (4 x 10(3) mu Omega cm) are nearly 4 orders of magnitude lower than standard EBID platinum structures (2.2 x 10(7) mu Omega cm) from the same precursor and are lower than the lowest reported EBID platinum resistivity with post-deposition annealing (1.4 x 10(4) mu Omega cm). Finally the LAEBID process demonstrates improved deposit resolution by similar to 25% compared to EBID structures under the conditions investigated in this work. C1 [Roberts, Nicholas A.; Magel, Gregory A.] Omniprobe Inc, Dallas, TX USA. [Roberts, Nicholas A.; Rack, Philip D.] Univ Tennessee, Dept Mat Sci & Engn, Knoxville, TN 37996 USA. [Fowlkes, Jason D.; Rack, Philip D.] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN USA. RP Rack, PD (reprint author), Univ Tennessee, Dept Mat Sci & Engn, Knoxville, TN 37996 USA. EM prack@utk.edu RI Roberts, Nicholas/H-3275-2014; OI Roberts, Nicholas/0000-0002-6490-9454; Rack, Philip/0000-0002-9964-3254 FU National Science Foundation [IIP-0956765, IIP-1059286]; Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy FX The authors acknowledge that 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. Omniprobe acknowledges that the laser probe development was supported in part by the National Science Foundation under Small Business Innovation Research Grant # IIP-0956765 to Omniprobe, and under Grant # IIP-1059286 to the American Society for Engineering Education. The authors gratefully acknowledge J. Chen at CNMS for TEM imaging and C. M. Gonzalez at UT for electrical measurements. NR 55 TC 30 Z9 30 U1 3 U2 39 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2040-3364 J9 NANOSCALE JI Nanoscale PY 2013 VL 5 IS 1 BP 408 EP 415 DI 10.1039/c2nr33014h PG 8 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA 068EF UT WOS:000313347200051 PM 23184056 ER PT J AU Trumbore, SE Angert, A Kunert, N Muhr, J Chambers, JQ AF Trumbore, Susan E. Angert, Alon Kunert, Norbert Muhr, Jan Chambers, Jeffrey Q. TI What's the flux? Unraveling how CO2 fluxes from trees reflect underlying physiological processes SO NEW PHYTOLOGIST LA English DT Editorial Material DE isotope labeling; respiration; sapflux; soil respiration; stem CO2 efflux ID STEM RESPIRATION; EFFLUX; TRANSPIRATION; TRANSPORT; AMAZON; BRAZIL; FATE C1 [Trumbore, Susan E.; Kunert, Norbert; Muhr, Jan] Max Planck Inst Biogeochem, D-07745 Jena, Germany. [Angert, Alon] Hebrew Univ Jerusalem, Inst Earth Sci, IL-91904 Jerusalem, Israel. [Chambers, Jeffrey Q.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Climate Sci Dept, Berkeley, CA 94720 USA. RP Trumbore, SE (reprint author), Max Planck Inst Biogeochem, D-07745 Jena, Germany. EM trumbore@bgc-jena.mpg.de RI Chambers, Jeffrey/J-9021-2014; OI Chambers, Jeffrey/0000-0003-3983-7847; Kunert, Norbert/0000-0002-5602-6221 NR 17 TC 13 Z9 16 U1 4 U2 89 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0028-646X J9 NEW PHYTOL JI New Phytol. PD JAN PY 2013 VL 197 IS 2 BP 353 EP 355 DI 10.1111/nph.12065 PG 3 WC Plant Sciences SC Plant Sciences GA 067AY UT WOS:000313265600001 PM 23253327 ER PT J AU Zeppel, MJB Anderegg, WRL Adams, HD AF Zeppel, Melanie J. B. Anderegg, William R. L. Adams, Henry D. TI Forest mortality due to drought: latest insights, evidence and unresolved questions on physiological pathways and consequences of tree death SO NEW PHYTOLOGIST LA English DT Editorial Material DE biosphere-atmosphere interactions; carbon cycling; carbon starvation; climate change; forest die-off; hydraulic failure; plant hydraulics ID CLIMATE-CHANGE; MECHANISMS; RESPONSES C1 [Zeppel, Melanie J. B.] Macquarie Univ, Dept Biol Sci, Ctr Climate Futures, N Ryde, NSW 2109, Australia. [Anderegg, William R. L.] Stanford Univ, Dept Biol, Stanford, CA 94305 USA. [Adams, Henry D.] Los Alamos Natl Lab, Earth & Environm Sci Div, Los Alamos, NM USA. RP Zeppel, MJB (reprint author), Macquarie Univ, Dept Biol Sci, Ctr Climate Futures, N Ryde, NSW 2109, Australia. EM melanie.zeppel@mq.edu.au RI Adams, Henry/A-8742-2010; OI Adams, Henry/0000-0002-6403-5304; Zeppel, Melanie/0000-0002-5510-0936 NR 16 TC 19 Z9 20 U1 6 U2 122 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0028-646X J9 NEW PHYTOL JI New Phytol. PD JAN PY 2013 VL 197 IS 2 BP 372 EP 374 DI 10.1111/nph.12090 PG 3 WC Plant Sciences SC Plant Sciences GA 067AY UT WOS:000313265600007 PM 23253331 ER PT J AU Battipaglia, G Saurer, M Cherubini, P Calfapietra, C McCarthy, HR Norby, RJ Cotrufo, MF AF Battipaglia, Giovanna Saurer, Matthias Cherubini, Paolo Calfapietra, Carlo McCarthy, Heather R. Norby, Richard J. Cotrufo, M. Francesca TI Elevated CO2 increases tree-level intrinsic water use efficiency: insights from carbon and oxygen isotope analyses in tree rings across three forest FACE sites SO NEW PHYTOLOGIST LA English DT Article DE climate change; dendro-ecology; Liquidambar styraciflua; Pinus taeda; Populus alba; Populus nigra; Populus x euramericana ID RISING ATMOSPHERIC CO2; STOMATAL CONDUCTANCE; DIOXIDE CONCENTRATION; POPLAR PLANTATION; ENRICHMENT FACE; PHOTOSYNTHETIC RESPONSES; TEMPERATE FOREST; DECIDUOUS FOREST; N-FERTILIZATION; STABLE-ISOTOPES AB Elevated CO2 increases intrinsic water use efficiency (WUEi) of forests, but the magnitude of this effect and its interaction with climate is still poorly understood. We combined tree ring analysis with isotope measurements at three Free Air CO2 Enrichment (FACE, POP-EUROFACE, in Italy; Duke FACE in North Carolina and ORNL in Tennessee, USA) sites, to cover the entire life of the trees. We used delta C-13 to assess carbon isotope discrimination and changes in water-use efficiency, while direct CO2 effects on stomatal conductance were explored using delta O-18 as a proxy. Across all the sites, elevated CO2 increased C-13-derived water-use efficiency on average by 73% for Liquidambar styraciflua, 77% for Pinus taeda and 75% for Populus sp., but through different ecophysiological mechanisms. Our findings provide a robust means of predicting water-use efficiency responses from a variety of tree species exposed to variable environmental conditions over time, and species-specific relationships that can help modelling elevated CO2 and climate impacts on forest productivity, carbon and water balances. C1 [Battipaglia, Giovanna] Univ Naples 2, Dept Environm Sci, I-81100 Caserta, Italy. [Battipaglia, Giovanna] Univ Montpellier 2, Ctr Bioarcheol & Ecol, Ecole Prat Hautes Etud PALECO EPHE, Inst Bot, F-34090 Montpellier, France. [Saurer, Matthias] PSI Paul Scherrer Inst, CH-5232 Villigen, Switzerland. [Cherubini, Paolo] WSL Swiss Fed Inst Forest Snow & Landscape Res, CH-8903 Birmensdorf, Switzerland. [Calfapietra, Carlo] CNR, IBAF Inst Agroenvironm & Forest Biol, Porano, Italy. [McCarthy, Heather R.] Univ Oklahoma, Dept Microbiol & Plant Biol, Norman, OK 73019 USA. [Norby, Richard J.] Oak Ridge Natl Lab, Div Environm Sci, Oak Ridge, TN 37831 USA. [Cotrufo, M. Francesca] Colorado State Univ, Dept Soil & Crop Sci, Ft Collins, CO 80523 USA. RP Battipaglia, G (reprint author), Univ Naples 2, Dept Environm Sci, I-81100 Caserta, Italy. EM giovanna.battipaglia@unina2.it RI Norby, Richard/C-1773-2012; Cotrufo, M. Francesca/C-1614-2013; Cherubini, Paolo/N-9702-2013; Calfapietra, Carlo/E-2269-2015 OI Norby, Richard/0000-0002-0238-9828; Cotrufo, M. Francesca/0000-0002-6191-8953; Battipaglia, Giovanna/0000-0003-1741-3509; Cherubini, Paolo/0000-0002-9809-250X; FU IBIMET CNR FX We thank David Frank, Rolf T. Siegwolf and Ram Oren for useful comments and encouragement for this work. We gratefully acknowledge Keith Lewin for sharing with us his experience on the performance of the DUKE FACE facility. We are grateful for logistic and technical support offered by Duke, ORNL and POP-EUROFACE. We thank the editor and the three anonymous referees for their valuable comments. The Duke and ORNL FACE experiments were supported by the United States Department of Energy, Office of Science, Biological and Environmental Research Program. Funding for the sampling campaign was provided by IBIMET CNR. NR 71 TC 64 Z9 65 U1 19 U2 275 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0028-646X J9 NEW PHYTOL JI New Phytol. PD JAN PY 2013 VL 197 IS 2 BP 544 EP 554 DI 10.1111/nph.12044 PG 11 WC Plant Sciences SC Plant Sciences GA 067AY UT WOS:000313265600024 PM 23215904 ER PT J AU Darrow, DS Crocker, N Fredrickson, ED Gorelenkov, NN Gorelenkova, M Kubota, S Medley, SS Podesta, M Shi, L White, RB AF Darrow, D. S. Crocker, N. Fredrickson, E. D. Gorelenkov, N. N. Gorelenkova, M. Kubota, S. Medley, S. S. Podesta, M. Shi, L. White, R. B. TI Stochastic orbit loss of neutral beam ions from NSTX due to toroidal Alfven eigenmode avalanches SO NUCLEAR FUSION LA English DT Article ID PLASMAS AB Short toroidal Alfven eigenmode (TAE) avalanche bursts in the National Spherical Torus Experiment (NSTX) cause a drop in the neutron rate and sometimes a loss of neutral beam ions at or near the full injection energy over an extended range of pitch angles. The simultaneous loss of wide ranges of pitch angle suggests stochastic transport of the beam ions occurs. When beam ion orbits are followed with a guiding centre code that incorporates the plasma's magnetic equilibrium plus the measured modes, the predicted ranges of lost pitch angle are similar to those seen in the experiment, with distinct populations of trapped and passing orbits lost. These correspond to domains where the stochasticity extends in the orbit phase space from the region of beam ion deposition to the loss boundary and the trajectories along which modes may transport particles extend from the deposition volume to the loss boundary. C1 [Darrow, D. S.; Fredrickson, E. D.; Gorelenkov, N. N.; Gorelenkova, M.; Medley, S. S.; Podesta, M.; Shi, L.; White, R. B.] Princeton Plasma Phys Lab, Princeton, NJ 08543 USA. [Crocker, N.; Kubota, S.] Univ Calif Los Angeles, Dept Phys, Los Angeles, CA 90024 USA. RP Darrow, DS (reprint author), Princeton Plasma Phys Lab, POB 451, Princeton, NJ 08543 USA. EM ddarrow@pppl.gov RI White, Roscoe/D-1773-2013 OI White, Roscoe/0000-0002-4239-2685 FU US DoE [DE-ACO2-09CH11466, DE-FG02-99ER54527] FX This work supported by US DoE contracts DE-ACO2-09CH11466 and DE-FG02-99ER54527. NR 13 TC 5 Z9 5 U1 0 U2 7 PU INT ATOMIC ENERGY AGENCY PI VIENNA PA WAGRAMERSTRASSE 5, PO BOX 100, A-1400 VIENNA, AUSTRIA SN 0029-5515 J9 NUCL FUSION JI Nucl. Fusion PD JAN PY 2013 VL 53 IS 1 AR 013009 DI 10.1088/0029-5515/53/1/13009 PG 8 WC Physics, Fluids & Plasmas SC Physics GA 067LJ UT WOS:000313295600011 ER PT J AU Fredrickson, ED Crocker, NA Darrow, DS Gorelenkov, NN Kramer, GJ Kubota, S Podesta, M White, RB Bortolon, A Gerhardt, SP Bell, RE Diallo, A LeBlanc, B Levinton, FM Yuh, H AF Fredrickson, E. D. Crocker, N. A. Darrow, D. S. Gorelenkov, N. N. Kramer, G. J. Kubota, S. Podesta, M. White, R. B. Bortolon, A. Gerhardt, S. P. Bell, R. E. Diallo, A. LeBlanc, B. Levinton, F. M. Yuh, H. TI Fast-ion energy loss during TAE avalanches in the National Spherical Torus Experiment SO NUCLEAR FUSION LA English DT Article ID FUSION TEST REACTOR; COMPRESSIONAL ALFVEN EIGENMODES; NEUTRAL BEAM INJECTION; ASPECT-RATIO PLASMAS; DIII-D; TOROIDAL PLASMAS; TOKAMAK; DRIVEN; INSTABILITIES; MODES AB Strong toroidal Alfven eigenmode (TAE) avalanches on NSTX, the National Spherical Torus Experiment (Ono et al 2000 Nucl. Fusion 40 557) are typically correlated with drops in the neutron rate in the range 5-15%. In previous studies of avalanches in L-mode plasmas, these neutron drops were found to be consistent with modelled losses of fast ions. Here we expand the study to TAE avalanches in NSTX H-mode plasmas with improved analysis techniques. At the measured TAE mode amplitudes, simulations with the ORBIT code predict that fast ion losses are negligible. However, the simulations predict that the TAE scatter the fast ions in energy, resulting in a small (approximate to 5-6%) drop in fast ion beta. The net decrease in energy of the fast ions is sufficient to account for about 50% of the drop in neutron rate, redistribution for approximate to 40%, and fast ion losses account for only approximate to 10%. This loss of energy from the fast ion population is comparable to the estimated energy lost by damping from the Alfven wave during the burst. The previously studied TAE avalanches in L-mode are re-evaluated using an improved calculation of the potential fluctuations in the ORBIT code near the separatrix. C1 [Fredrickson, E. D.; Crocker, N. A.; Darrow, D. S.; Gorelenkov, N. N.; Kramer, G. J.; Kubota, S.; Podesta, M.; White, R. B.; Bortolon, A.; Gerhardt, S. P.; Bell, R. E.; Diallo, A.; LeBlanc, B.; Levinton, F. M.; Yuh, H.] Princeton Plasma Phys Lab, Princeton, NJ 08543 USA. [Crocker, N. A.; Kubota, S.] Univ Calif Los Angeles, Dept Phys & Astron, Los Angeles, CA 90095 USA. [Bortolon, A.] Univ Calif Irvine, Dept Phys & Astron, Irvine, CA 92697 USA. [Levinton, F. M.; Yuh, H.] Nova Photon, Princeton, NJ 08543 USA. RP Fredrickson, ED (reprint author), Princeton Plasma Phys Lab, POB 451, Princeton, NJ 08543 USA. RI White, Roscoe/D-1773-2013; Bortolon, Alessandro/H-5764-2015 OI White, Roscoe/0000-0002-4239-2685; Bortolon, Alessandro/0000-0002-0094-0209 FU US DOE [DE-AC02-09CH11466, DE-FG03-99ER54527, DE-FG02-06ER54867, DE-FG02-99ER54527] FX Work supported by US DOE Contracts DE-AC02-09CH11466, DE-FG03-99ER54527, DE-FG02-06ER54867 and DE-FG02-99ER54527. NR 64 TC 17 Z9 17 U1 1 U2 13 PU INT ATOMIC ENERGY AGENCY PI VIENNA PA WAGRAMERSTRASSE 5, PO BOX 100, A-1400 VIENNA, AUSTRIA SN 0029-5515 J9 NUCL FUSION JI Nucl. Fusion PD JAN PY 2013 VL 53 IS 1 AR 013006 DI 10.1088/0029-5515/53/1/013006 PG 10 WC Physics, Fluids & Plasmas SC Physics GA 067LJ UT WOS:000313295600008 ER PT J AU Stoschus, H Lehnen, M Schmitz, O Reiser, D Unterberg, B Samm, U AF Stoschus, H. Lehnen, M. Schmitz, O. Reiser, D. Unterberg, B. Samm, U. CA TEXTOR Res Team TI Rotation dependent ion fluxes in front of resonant magnetic perturbation coils SO NUCLEAR FUSION LA English DT Article ID DYNAMIC ERGODIC DIVERTOR; TEXTOR; TRANSPORT AB Ion fluxes to the first wall of TEXTOR are modulated during application of a fast rotating resonant magnetic perturbation (RMP) field. The modulation in front of the RMP coils matches the magnetic topology modelled in vacuum approximation for low relative rotation of f(rel) = -0.2kHz between the RMP field and toroidal plasma rotation. With increasing relative rotation, the ion flux pattern is shifted linearly in counter-B-t direction. The shift is correlated to a displacement Delta phi = pi/2 of the electron density modulation at the outermost resonant flux surface caused by an internal plasma response. This indicates a competition between the near magnetic field of the RMP coils and the net magnetic field at the resonant flux surface. C1 [Stoschus, H.; Lehnen, M.; Schmitz, O.; Reiser, D.; Unterberg, B.; Samm, U.] Forschungszentrum Julich, Assoc EURATOM FZJ, Inst Energy & Climate Res Plasma Phys, Trilateral Euregio Cluster, D-52425 Julich, Germany. RP Stoschus, H (reprint author), Oak Ridge Inst Sci & Educ, Oak Ridge, TN 37831 USA. EM stoschus@fusion.gat.com OI Reiser, Dirk/0000-0002-2667-4818; Unterberg, Bernhard/0000-0003-0866-957X FU German Research Foundation (DFG) [UN 65/1-1, GRK 1203.] FX This work is supported by the German Research Foundation (DFG) under grant no. UN 65/1-1 and GRK 1203. authors thank A. Strothe for his enthusiastic commitment to this project. NR 25 TC 5 Z9 5 U1 1 U2 3 PU INT ATOMIC ENERGY AGENCY PI VIENNA PA WAGRAMERSTRASSE 5, PO BOX 100, A-1400 VIENNA, AUSTRIA SN 0029-5515 J9 NUCL FUSION JI Nucl. Fusion PD JAN PY 2013 VL 53 IS 1 AR 012001 DI 10.1088/0029-5515/53/1/012001 PG 5 WC Physics, Fluids & Plasmas SC Physics GA 067LJ UT WOS:000313295600002 ER PT J AU Kinoshita, N Paul, M Alcorta, M Bowers, M Collon, P Deibel, CM DiGiovine, B Goriely, S Greene, JP Henderson, DJ Jiang, CL Kashiv, Y Kay, BP Lee, HY Marley, ST Nakanishi, T Pardo, RC Patel, N Rehm, KE Robertson, D Scott, R Schmitt, C Tang, XD Ugalde, C Vondrasek, R AF Kinoshita, N. Paul, M. Alcorta, M. Bowers, M. Collon, P. Deibel, C. M. DiGiovine, B. Goriely, S. Greene, J. P. Henderson, D. J. Jiang, C. L. Kashiv, Y. Kay, B. P. Lee, H. Y. Marley, S. T. Nakanishi, T. Pardo, R. C. Patel, N. Rehm, K. E. Robertson, D. Scott, R. Schmitt, C. Tang, X. D. Ugalde, C. Vondrasek, R. TI New AMS method to measure the atom ratio Sm-146/Sm-147 for a half-life determination of Sm-146 SO NUCLEAR INSTRUMENTS & METHODS IN PHYSICS RESEARCH SECTION B-BEAM INTERACTIONS WITH MATERIALS AND ATOMS LA English DT Article; Proceedings Paper CT 12th International Conference on Accelerator Mass Spectrometry (AMS) CY MAR 20-25, 2011 CL GNS Sci, Wellington, NEW ZEALAND SP GNS Sci, Natl Isotope Ctr, Australian Nucl Sci & Technol Org, High Voltage Engn, Natl Electrostat Corp HO GNS Sci DE Accelerator mass spectrometry; Sm-146; ECR ion source; Superconducting linear accelerator ID ION-SOURCE AB The extinct p-process nuclide Sm-146 (t(1/2) = 103 +/- 5 Myr) is known to have been present in the Early-Solar System and has been proposed as an astrophysical chronometer. Sm-146 is also intensely used to date meteorite and planetary differentiation processes, enhancing the importance of an accurate knowledge of the Sm-146 half-life. We are engaged in a new determination of the Sm-146 half-life in which the Sm-146/Sm-147 atom ratio is determined by accelerator mass spectrometry at the ATLAS facility of Argonne National Laboratory. In order to reduce systematic errors in the AMS determination of the Sm-146/Sm-147 ratios (in the range of 10(-7)-10(-9)), Sm-146 and Sm-147 ions were alternately counted in the same detector in the focal plane of a gas-filled magnet, respectively in continuous-wave and attenuated mode. Quantitative attenuation is obtained with the 12 MHz pulsed and ns-bunched ATLAS beam by chopping beam pulses with an RF sweeper in a ratio (digitally determined) down to 1:10(6). The experiments and preliminary results are discussed. (C) 2012 Elsevier B.V. All rights reserved. C1 [Kinoshita, N.] Univ Tsukuba, Res Facil, Ctr Sci & Technol, Tsukuba, Ibaraki 305, Japan. [Paul, M.] Hebrew Univ Jerusalem, Racah Inst Phys, IL-91904 Jerusalem, Israel. [Alcorta, M.; Deibel, C. M.; DiGiovine, B.; Greene, J. P.; Henderson, D. J.; Jiang, C. L.; Kay, B. P.; Lee, H. Y.; Marley, S. T.; Pardo, R. C.; Patel, N.; Rehm, K. E.; Scott, R.; Ugalde, C.; Vondrasek, R.] Argonne Natl Lab, Div Phys, Argonne, IL 60439 USA. [Bowers, M.; Collon, P.; Kashiv, Y.; Robertson, D.; Schmitt, C.; Tang, X. D.] Univ Notre Dame, Dept Phys, Notre Dame, IN 46556 USA. [Deibel, C. M.] Michigan State Univ, Joint Inst Nucl Astrophys, E Lansing, MI 48824 USA. [Goriely, S.] Univ Libre Brussels, B-1050 Brussels, Belgium. [Nakanishi, T.] Kanazawa Univ, Fac Chem, Inst Sci & Engn, Kanazawa, Ishikawa 9201192, Japan. RP Paul, M (reprint author), Hebrew Univ Jerusalem, Racah Inst Phys, IL-91904 Jerusalem, Israel. EM paul@vms.huji.ac.il RI Kay, Benjamin/F-3291-2011; Alcorta, Martin/G-7107-2011; Tang, Xiaodong /F-4891-2016 OI Kay, Benjamin/0000-0002-7438-0208; Alcorta, Martin/0000-0002-6217-5004; NR 12 TC 2 Z9 2 U1 0 U2 16 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0168-583X J9 NUCL INSTRUM METH B JI Nucl. Instrum. Methods Phys. Res. Sect. B-Beam Interact. Mater. Atoms PD JAN PY 2013 VL 294 BP 143 EP 146 DI 10.1016/j.nimb.2012.01.013 PG 4 WC Instruments & Instrumentation; Nuclear Science & Technology; Physics, Atomic, Molecular & Chemical; Physics, Nuclear SC Instruments & Instrumentation; Nuclear Science & Technology; Physics GA 066QC UT WOS:000313234300027 ER PT J AU Paul, M Pardo, R Ahmad, I Greene, J Henderson, D Janssens, RVF Jiang, CL Rehm, KE Scott, R Seweryniak, D Vondrasek, R AF Paul, M. Pardo, R. Ahmad, I. Greene, J. Henderson, D. Janssens, R. V. F. Jiang, C. L. Rehm, K. E. Scott, R. Seweryniak, D. Vondrasek, R. TI High-sensitivity detection of Pu-244 via electron-cyclotron resonance ionization and linear acceleration SO NUCLEAR INSTRUMENTS & METHODS IN PHYSICS RESEARCH SECTION B-BEAM INTERACTIONS WITH MATERIALS AND ATOMS LA English DT Article; Proceedings Paper CT 12th International Conference on Accelerator Mass Spectrometry (AMS) CY MAR 20-25, 2011 CL GNS Sci, Wellington, NEW ZEALAND SP GNS Sci, Natl Isotope Ctr, Australian Nucl Sci & Technol Org, High Voltage Engn, Natl Electrostat Corp HO GNS Sci DE Accelerator mass spectrometry; Linear accelerator; Electron cyclotron resonance ion source; Actinides ID SOLAR-SYSTEM; ION-SOURCE; ATLAS; NUCLEI; AMS AB The r-process nuclide Pu-244 (t(1/2) = 80.8 Myr) was extant in the Early Solar System and is presently considered as extinct. However, fresh Pu-244 produced in the Galaxy, may reach the Solar System and Earth through influx of interstellar dust or as direct ejecta from supernovae. Detection of such traces requires high sensitivity, discrimination power and efficiency. Accelerator mass spectrometry (AMS), despite low efficiency, is the method of choice. We report on the successful detection of Pu-244 by AMS, using highly-charged positive ions produced in an Electron Cyclotron Resonance (ECR) ion source and accelerated with the superconducting heavy-ion linear accelerator ATLAS at Argonne National Laboratory. Pu-244(34+,35+,36+) ions with a final energy of 0.7 MeV/u were dispersed in m/q using the Argonne Fragment Mass Analyzer (FMA) and are well discriminated from parasitic ions. A count rate of 0.7 Pu-244 counts/min was observed for a sample containing 2.7 x 10(8) Pu-244 atoms/mg. The technique described here is presently used, with improved setup and accelerator conditions, for the measurement of neutron capture cross sections in the actinide region. (c) 2012 Elsevier B.V. All rights reserved. C1 [Paul, M.] Hebrew Univ Jerusalem, Racah Inst Phys, IL-91904 Jerusalem, Israel. [Pardo, R.; Ahmad, I.; Greene, J.; Henderson, D.; Janssens, R. V. F.; Jiang, C. L.; Rehm, K. E.; Scott, R.; Seweryniak, D.; Vondrasek, R.] Argonne Natl Lab, Div Phys, Argonne, IL 60439 USA. RP Paul, M (reprint author), Hebrew Univ Jerusalem, Racah Inst Phys, IL-91904 Jerusalem, Israel. EM paul@vms.huji.ac.il NR 13 TC 2 Z9 2 U1 0 U2 5 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0168-583X J9 NUCL INSTRUM METH B JI Nucl. Instrum. Methods Phys. Res. Sect. B-Beam Interact. Mater. Atoms PD JAN PY 2013 VL 294 BP 165 EP 167 DI 10.1016/j.nimb.2012.01.016 PG 3 WC Instruments & Instrumentation; Nuclear Science & Technology; Physics, Atomic, Molecular & Chemical; Physics, Nuclear SC Instruments & Instrumentation; Nuclear Science & Technology; Physics GA 066QC UT WOS:000313234300031 ER PT J AU Pardo, RC Kondev, FG Kondrashev, S Nair, C Palchan, T Scott, R Seweryniak, D Vondrasek, R Paul, M Collon, P Deibel, C Youinou, G Salvatores, M Palmotti, G Berg, J Fonnesbeck, J Imel, G AF Pardo, R. C. Kondev, F. G. Kondrashev, S. Nair, C. Palchan, T. Scott, R. Seweryniak, D. Vondrasek, R. Paul, M. Collon, P. Deibel, C. Youinou, G. Salvatores, M. Palmotti, G. Berg, J. Fonnesbeck, J. Imel, G. TI Toward laser ablation Accelerator Mass Spectrometry of actinides SO NUCLEAR INSTRUMENTS & METHODS IN PHYSICS RESEARCH SECTION B-BEAM INTERACTIONS WITH MATERIALS AND ATOMS LA English DT Article; Proceedings Paper CT 12th International Conference on Accelerator Mass Spectrometry (AMS) CY MAR 20-25, 2011 CL GNS Sci, Wellington, NEW ZEALAND SP GNS Sci, Natl Isotope Ctr, Australian Nucl Sci & Technol Org, High Voltage Engn, Natl Electrostat Corp HO GNS Sci DE Accelerator Mass Spectrometry; Laser ablation; Actinide Mass Spectrometry; Integral neutron capture cross-section; ECR ion source; Superconducting linear accelerator ID RESONANCE ION-SOURCE; SOLID MATERIAL; ATLAS; AMS AB A project to measure neutron capture cross sections of a number of actinides in a reactor environment by Accelerator Mass Spectrometry (AMS) at the ATLAS facility of Argonne National Laboratory is underway. This project will require the precise and accurate measurement of produced actinide isotopes in many (>30) samples irradiated in the Advanced Test Reactor at Idaho National Laboratory with neutron fluxes having different energy distributions. The AMS technique at ATLAS is based on production of highly-charged positive ions in an electron cyclotron resonance (ECR) ion source followed by acceleration in the ATLAS linac and mass-to-charge (m/q) measurement at the focus of the Fragment Mass Analyzer. Laser ablation was selected as the method of feeding the actinide material into the ion source because we expect it will have higher efficiency and lower chamber contamination than either the oven or sputtering techniques, because of a much narrower angular distribution of emitted material. In addition, a new multi-sample holder/changer to allow quick change between samples and a computer-controlled routine allowing fast tuning of the accelerator for different beams, are being developed. An initial test run studying backgrounds, detector response, and accelerator scaling repeatability was conducted in December 2010. The project design, schedule, and results of the initial test run to study backgrounds are discussed. (C) 2012 Elsevier B.V. All rights reserved. C1 [Pardo, R. C.; Kondev, F. G.; Kondrashev, S.; Nair, C.; Palchan, T.; Scott, R.; Seweryniak, D.; Vondrasek, R.; Deibel, C.] Argonne Natl Lab, Argonne, IL 60439 USA. [Paul, M.] Hebrew Univ Jerusalem, Racah Inst Phys, IL-91904 Jerusalem, Israel. [Collon, P.] Univ Notre Dame, Nucl Struct Lab, Notre Dame, IN 46556 USA. [Deibel, C.] Michigan State Univ, Joint Inst Nucl Astrophys, E Lansing, MI 48824 USA. [Youinou, G.; Salvatores, M.; Palmotti, G.; Berg, J.; Fonnesbeck, J.] Idaho Natl Lab, Idaho Falls, ID 83415 USA. [Imel, G.] Idaho State Univ, Pocatello, ID 83209 USA. RP Pardo, RC (reprint author), Argonne Natl Lab, 9700 S Cass Ave, Argonne, IL 60439 USA. EM pardo@phy.anl.gov NR 14 TC 3 Z9 3 U1 2 U2 12 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0168-583X J9 NUCL INSTRUM METH B JI Nucl. Instrum. Methods Phys. Res. Sect. B-Beam Interact. Mater. Atoms PD JAN PY 2013 VL 294 BP 281 EP 286 DI 10.1016/j.nimb.2012.01.047 PG 6 WC Instruments & Instrumentation; Nuclear Science & Technology; Physics, Atomic, Molecular & Chemical; Physics, Nuclear SC Instruments & Instrumentation; Nuclear Science & Technology; Physics GA 066QC UT WOS:000313234300055 ER PT J AU Salazar, G Ognibene, T AF Salazar, Gary Ognibene, Ted TI Design of a secondary ionization target for direct production of a C- beam from CO2 pulses for online AMS SO NUCLEAR INSTRUMENTS & METHODS IN PHYSICS RESEARCH SECTION B-BEAM INTERACTIONS WITH MATERIALS AND ATOMS LA English DT Article; Proceedings Paper CT 12th International Conference on Accelerator Mass Spectrometry (AMS) CY MAR 20-25, 2011 CL GNS Sci, Wellington, NEW ZEALAND SP GNS Sci, Natl Isotope Ctr, Australian Nucl Sci & Technol Org, High Voltage Engn, Natl Electrostat Corp HO GNS Sci DE AMS; Gas ion source; CO2 direct ionization; Gas target; COMSOL simulation ID ACCELERATOR MASS-SPECTROMETRY; GAS ION-SOURCE; SPUTTER SOURCE; GC-AMS; C-14; ADSORPTION; PROGRESS; SYSTEM; MODEL AB We designed and optimized a novel device "target" that directs a CO2 gas pulse onto a Ti surface where a Cs+ beam generates C- from the CO2. This secondary ionization target enables an accelerator mass spectrometer to ionize pulses of CO2 in the negative mode to measure C-14/C-12 isotopic ratios in real time. The design of the targets were based on computational flow dynamics, ionization mechanism and empirical optimization. As part of the ionization mechanism, the adsorption of CO2 on the Ti surface was fitted with the Jovanovic-Freundlich isotherm model using empirical and simulation data. The inferred adsorption constants were in good agreement with other works. The empirical optimization showed that amount of injected carbon and the flow speed of the helium carrier gas improve the ionization efficiency and the amount of C-12(-) produced until reaching a saturation point. Linear dynamic range between 150 and 1000 ng of C and optimum carrier gas flow speed of around 0.1 mL/min were shown. It was also shown that the ionization depends on the area of the Ti surface and Cs+ beam cross-section. A range of ionization efficiency of 1-2.5% was obtained by optimizing the described parameters. Published by Elsevier B.V. C1 [Salazar, Gary; Ognibene, Ted] Lawrence Livermore Natl Lab, Ctr Accelerator Mass Spectrometry, Livermore, CA 94550 USA. RP Salazar, G (reprint author), Lawrence Livermore Natl Lab, Ctr Accelerator Mass Spectrometry L397, 7000 East Ave, Livermore, CA 94550 USA. EM salazarquint1@llnl.gov FU NCRR NIH HHS [P41 RR013461]; NIGMS NIH HHS [P41 GM103483] NR 29 TC 2 Z9 2 U1 1 U2 7 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0168-583X EI 1872-9584 J9 NUCL INSTRUM METH B JI Nucl. Instrum. Methods Phys. Res. Sect. B-Beam Interact. Mater. Atoms PD JAN PY 2013 VL 294 BP 300 EP 306 DI 10.1016/j.nimb.2012.03.039 PG 7 WC Instruments & Instrumentation; Nuclear Science & Technology; Physics, Atomic, Molecular & Chemical; Physics, Nuclear SC Instruments & Instrumentation; Nuclear Science & Technology; Physics GA 066QC UT WOS:000313234300059 PM 24860204 ER PT J AU Ognibene, TJ Salazar, GA AF Ognibene, T. J. Salazar, G. A. TI Installation of hybrid ion source on the 1-MV LLNL BioAMS spectrometer SO NUCLEAR INSTRUMENTS & METHODS IN PHYSICS RESEARCH SECTION B-BEAM INTERACTIONS WITH MATERIALS AND ATOMS LA English DT Article; Proceedings Paper CT 12th International Conference on Accelerator Mass Spectrometry (AMS) CY MAR 20-25, 2011 CL GNS Sci, Wellington, NEW ZEALAND SP GNS Sci, Natl Isotope Ctr, Australian Nucl Sci & Technol Org, High Voltage Engn, Natl Electrostat Corp HO GNS Sci DE AMS; Ion sources; CO2 gas; Graphite; Moving-wire ID ACCELERATOR MASS-SPECTROMETRY; BIOCHEMICAL SAMPLES; MC-SNICS; AMS; GAS; SYSTEM AB A second ion source was recently installed onto the LLNL 1-MV AMS spectrometer, which is dedicated to the quantification of C-14 and H-3 within biochemical samples. This source is unique among the other LLNL cesium sputter ion sources in that it can ionize both gaseous and solid samples. Also, the injection beam line has been designed to directly measure C-14/C-12 isotope ratios without the need for electrostatic bouncing. Preliminary tests show that this source can ionize transient CO2 gas pulses containing less than 1 pig carbon with approximately 1.5% efficiency. We demonstrate that the measured C-14/C-12 isotope ratio is largely unaffected by small drifts in the argon stripper gas density. We also determine that a tandem accelerating voltage of 670 kV enables the highest C-14 transmission through the system. Finally, we describe a series of performance tests using solid graphite targets spanning nearly 3 orders in magnitude dynamic range and compare the results to our other ion source. (C) 2011 Elsevier B.V. All rights reserved. C1 [Ognibene, T. J.; Salazar, G. A.] Lawrence Livermore Natl Lab, Ctr Accelerator Mass Spectrometry, Livermore, CA 94551 USA. RP Ognibene, TJ (reprint author), Lawrence Livermore Natl Lab, Ctr Accelerator Mass Spectrometry, 7000 East Ave, Livermore, CA 94551 USA. EM ognibene1@llnl.gov FU NCRR NIH HHS [P41 RR013461-14, P41 RR013461]; NIGMS NIH HHS [P41 GM103483] NR 13 TC 6 Z9 6 U1 4 U2 13 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0168-583X J9 NUCL INSTRUM METH B JI Nucl. Instrum. Methods Phys. Res. Sect. B-Beam Interact. Mater. Atoms PD JAN PY 2013 VL 294 BP 311 EP 314 DI 10.1016/j.nimb.2011.11.029 PG 4 WC Instruments & Instrumentation; Nuclear Science & Technology; Physics, Atomic, Molecular & Chemical; Physics, Nuclear SC Instruments & Instrumentation; Nuclear Science & Technology; Physics GA 066QC UT WOS:000313234300061 PM 23467295 ER PT J AU Tumey, SJ Brown, TA Finkel, RC Rood, DH AF Tumey, Scott J. Brown, Thomas A. Finkel, Robert C. Rood, Dylan H. TI The feasibility of isobaric suppression of Mg-26 via post-accelerator foil stripping for the measurement of Al-26 SO NUCLEAR INSTRUMENTS & METHODS IN PHYSICS RESEARCH SECTION B-BEAM INTERACTIONS WITH MATERIALS AND ATOMS LA English DT Article; Proceedings Paper CT 12th International Conference on Accelerator Mass Spectrometry (AMS) CY MAR 20-25, 2011 CL GNS Sci, Wellington, NEW ZEALAND SP GNS Sci, Natl Isotope Ctr, Australian Nucl Sci & Technol Org, High Voltage Engn, Natl Electrostat Corp HO GNS Sci DE Accelerator mass spectrometry; Al-26; Mg suppression ID FORMULAS; IONS AB Most accelerator mass spectrometry measurements of Al-26 utilize the Al- ion despite lower source currents compared with AlO- since the stable isobar Mg-26 does not form elemental negative ions. A gas-filled magnet allows sufficient suppression of Mg-26 thus enabling the use of the more intense (AlO-)-Al-26 ion. However, most AMS systems do not include a gas-filled magnet. We therefore explored the feasibility of suppressing Mg-26 by using a post-accelerator stripping foil. With this approach, combined with the use of alternative cathode matrices, we were able to suppress Mg-26 by a factor of 20. This suppression was insufficient to enable the use of (AlO-)-Al-26, however further refinement of our system may permit its use in the future. (C) 2012 Elsevier B.V. All rights reserved. C1 [Tumey, Scott J.; Brown, Thomas A.; Rood, Dylan H.] Lawrence Livermore Natl Lab, Ctr Accelerator Mass Spectrometry, Livermore, CA 94551 USA. [Finkel, Robert C.] Univ Calif Berkeley, Dept Earth & Planetary Sci, Berkeley, CA 94720 USA. [Rood, Dylan H.] Univ Calif Santa Barbara, Earth Res Inst, Santa Barbara, CA 93196 USA. RP Tumey, SJ (reprint author), Lawrence Livermore Natl Lab, Ctr Accelerator Mass Spectrometry, POB 808,L-397, Livermore, CA 94551 USA. EM tumey2@llnl.gov NR 9 TC 0 Z9 0 U1 1 U2 1 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0168-583X J9 NUCL INSTRUM METH B JI Nucl. Instrum. Methods Phys. Res. Sect. B-Beam Interact. Mater. Atoms PD JAN PY 2013 VL 294 BP 406 EP 409 DI 10.1016/j.nimb.2012.08.040 PG 4 WC Instruments & Instrumentation; Nuclear Science & Technology; Physics, Atomic, Molecular & Chemical; Physics, Nuclear SC Instruments & Instrumentation; Nuclear Science & Technology; Physics GA 066QC UT WOS:000313234300079 ER PT J AU Rood, DH Brown, TA Finkel, RC Guilderson, TP AF Rood, Dylan H. Brown, Thomas A. Finkel, Robert C. Guilderson, Thomas P. TI Poisson and non-Poisson uncertainty estimations of Be-10/Be-9 measurements at LLNL-CAMS SO NUCLEAR INSTRUMENTS & METHODS IN PHYSICS RESEARCH SECTION B-BEAM INTERACTIONS WITH MATERIALS AND ATOMS LA English DT Article; Proceedings Paper CT 12th International Conference on Accelerator Mass Spectrometry (AMS) CY MAR 20-25, 2011 CL GNS Sci, Wellington, NEW ZEALAND SP GNS Sci, Natl Isotope Ctr, Australian Nucl Sci & Technol Org, High Voltage Engn, Natl Electrostat Corp HO GNS Sci DE Accelerator mass spectrometry; Be-10; Uncertainties ID HOLOCENE GLACIER FLUCTUATIONS; NEW-ZEALAND; ION-SOURCE; AMS; CAMS/LLNL AB We quantify the routine performance and uncertainties of Be-10 measurements made on the CAMS FN accelerator mass spectrometer in combination with the CAMS high-intensity cesium sputter source. Our analysis compiles data from 554 primary and secondary standard targets measured on 47 different wheels in nine different run campaigns over a 1-year interval (September 2009-September 2010). The series includes 87, 86, and 85 measurements of each of three different secondary standards and 296 measurements of our primary standard, KNSTD3110 (01-5-4). The average initial Be-9(3+) beam current is 22 +/- 3 mu A (1 standard deviation). Secondary standard targets, which are measured as unknowns in each of the wheels, have average statistical uncertainties based on counting statistics of 1.8%, 1.3%, and 0.8% (1 sigma) (September 2009-March 2010) and 1.3%, 1.0%, and 0.6% (April 2010-September 2010) for standard materials with Be-10/Be-9 = 5.35 x 10(-13), 9.72 x 10(-13), and 8.56 x 10(-12), respectively. The mean measured ratio for each of the secondary standards (normalized to the primary standard) falls within the 1.1% uncertainties of the reported values for each standard material. The weighted standard deviation around the mean of this large number of runs is 2.5%, 2.0%, and 1.2% (September 2009-March 2010) and 1.5%, 1.1%, and 1.2% (April 2010-September 2010) for each secondary standard. These data indicate an additional source of uncertainty, 0.9-1.8% (April 2010-September 2010) and 0.2-1.0% (April 2010-September 2010), above that calculated from counting statistics alone. These Be-10 AMS results demonstrate the precision and accuracy of the LLNL-CAMS system. (C) 2012 Elsevier B.V. All rights reserved. C1 [Rood, Dylan H.; Brown, Thomas A.; Finkel, Robert C.; Guilderson, Thomas P.] Lawrence Livermore Natl Lab, Ctr Accelerator Mass Spectrometry, Livermore, CA 94550 USA. [Rood, Dylan H.] Univ Calif Santa Barbara, Earth Res Inst, Santa Barbara, CA 93106 USA. [Finkel, Robert C.] Univ Calif Berkeley, Dept Earth & Planetary Sci, Berkeley, CA 94720 USA. [Guilderson, Thomas P.] Univ Calif Santa Cruz, Dept Ocean Sci, Santa Cruz, CA 95064 USA. RP Rood, DH (reprint author), SUERC, AMS Lab, E Kilbride G75 0QF, Lanark, Scotland. EM Dylan.Rood@glasgow.ac.uk NR 20 TC 17 Z9 17 U1 1 U2 5 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0168-583X J9 NUCL INSTRUM METH B JI Nucl. Instrum. Methods Phys. Res. Sect. B-Beam Interact. Mater. Atoms PD JAN PY 2013 VL 294 BP 426 EP 429 DI 10.1016/j.nimb.2012.08.039 PG 4 WC Instruments & Instrumentation; Nuclear Science & Technology; Physics, Atomic, Molecular & Chemical; Physics, Nuclear SC Instruments & Instrumentation; Nuclear Science & Technology; Physics GA 066QC UT WOS:000313234300083 ER PT J AU Caffee, MW Nishiizumi, K Sisterson, JM Ullmann, J Welten, KC AF Caffee, M. W. Nishiizumi, K. Sisterson, J. M. Ullmann, J. Welten, K. C. TI Cross section measurements at neutron energies 71 and 112 MeV and energy integrated cross section measurements (0.1 < E-n < 750 MeV) for the neutron induced reactions O(n,x)Be-10, Si(n,x)Be-10, and Si(n,x)Al-26 SO NUCLEAR INSTRUMENTS & METHODS IN PHYSICS RESEARCH SECTION B-BEAM INTERACTIONS WITH MATERIALS AND ATOMS LA English DT Article; Proceedings Paper CT 12th International Conference on Accelerator Mass Spectrometry (AMS) CY MAR 20-25, 2011 CL GNS Sci, Wellington, NEW ZEALAND SP GNS Sci, Natl Isotope Ctr, Australian Nucl Sci & Technol Org, High Voltage Engn, Natl Electrostat Corp HO GNS Sci DE Neutron induced reaction; Cross sections; Cosmogenic nuclides; Long-lived nuclides; Accelerator mass spectrometry ID COSMOGENIC-NUCLIDE PRODUCTION; ACCELERATOR MASS-SPECTROMETRY; PRODUCTION-RATES; AMS STANDARDS; AL-26; BE-10; SOLAR; SIMULATIONS; CL-36 AB The cross sections for the reactions O(n,x)Be-10, Si(n,x)Be-10, and Si(n,x)Al-26 were measured at neutron energies 71 and 112 MeV. The neutron cross sections for O(n,x)10Be are higher than the corresponding proton cross sections at 70-110 MeV and the neutron induced cross section for Si(n,x)Be-10 at 112 MeV is slightly higher than the corresponding proton cross section. Cross sections for the production of Al-26 from Si are similar to those from protons at low energies (<40 MeV) while at higher energies the measured neutron cross sections for Si(n,x)Al-26 are lower than the corresponding proton cross sections. Energy integrated (average) cross sections for these reactions were measured using 'white' neutron beams (0.1 < E-n < 750 MeV). The Al-26/Be-10 production rate ratio from SiO2 measured using 'white' neutrons is considerably lower than that observed in terrestrial quartz (SiO2). (C) 2012 Elsevier B.V. All rights reserved. C1 [Caffee, M. W.] Purdue Univ, Dept Phys, W Lafayette, IN 47907 USA. [Nishiizumi, K.; Welten, K. C.] Univ Calif Berkeley, Space Sci Lab, Berkeley, CA 94720 USA. [Sisterson, J. M.] Massachusetts Gen Hosp, Francis H Burr Proton Therapy Ctr, Boston, MA 02114 USA. [Ullmann, J.] Los Alamos Natl Lab, LANSCE, Los Alamos, NM 87545 USA. RP Caffee, MW (reprint author), Purdue Univ, Dept Phys, W Lafayette, IN 47907 USA. EM mcaffee@purdue.edu RI Caffee, Marc/K-7025-2015 OI Caffee, Marc/0000-0002-6846-8967 NR 21 TC 5 Z9 5 U1 0 U2 8 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0168-583X J9 NUCL INSTRUM METH B JI Nucl. Instrum. Methods Phys. Res. Sect. B-Beam Interact. Mater. Atoms PD JAN PY 2013 VL 294 BP 479 EP 483 DI 10.1016/j.nimb.2012.07.011 PG 5 WC Instruments & Instrumentation; Nuclear Science & Technology; Physics, Atomic, Molecular & Chemical; Physics, Nuclear SC Instruments & Instrumentation; Nuclear Science & Technology; Physics GA 066QC UT WOS:000313234300093 ER PT J AU Buchholz, BA Fallon, SJ Zermeno, P Bench, G Schichtel, BA AF Buchholz, Bruce A. Fallon, Stewart J. Zermeno, Paula Bench, Graham Schichtel, Bret A. TI Anomalous elevated radiocarbon measurements of PM2.5 SO NUCLEAR INSTRUMENTS & METHODS IN PHYSICS RESEARCH SECTION B-BEAM INTERACTIONS WITH MATERIALS AND ATOMS LA English DT Article; Proceedings Paper CT 12th International Conference on Accelerator Mass Spectrometry (AMS) CY MAR 20-25, 2011 CL GNS Sci, Wellington, NEW ZEALAND SP GNS Sci, Natl Isotope Ctr, Australian Nucl Sci & Technol Org, High Voltage Engn, Natl Electrostat Corp HO GNS Sci DE PM2.5; Elevated C-14; Source apportionment; Particulate matter ID PARTICULATE MATTER; AMBIENT AEROSOL; CARBON; C-14; HYDROCARBONS; FOREST; FOSSIL AB Two-component models are often used to determine the contributions made by fossil fuel and natural sources of carbon in airborne particulate matter (PM). The models reduce thousands of actual sources to two end members based on isotopic signature. Combustion of fossil fuels produces PM free of carbon-14 (C-14). Wood or charcoal smoke, restaurant fryer emissions, and natural emissions from plants produce PM with the contemporary concentration of C-14 approximately 1.2 x 10(-12) C-14/C. Such data can be used to estimate the relative contributions of fossil fuels and biogenic aerosols to the total aerosol loading and radiocarbon analysis is becoming a popular source apportionment method. Emissions from incinerators combusting medical or biological wastes containing tracer C-14 can skew the C-14/C ratio of PM, however, so critical analysis of sampling sites for possible sources of elevated PM needs to be completed prior to embarking on sampling campaigns. Results are presented for two ambient monitoring sites in different areas of the United States where C-14 contamination is apparent. Our experience suggests that such contamination is uncommon but is also not rare (similar to 10%) for PM sampling sites. (C) 2012 Elsevier B.V. All rights reserved. C1 [Buchholz, Bruce A.; Fallon, Stewart J.; Zermeno, Paula; Bench, Graham] Lawrence Livermore Natl Lab, Ctr Accelerator Mass Spectrometry, Livermore, CA 94551 USA. [Fallon, Stewart J.] Australian Natl Univ, Res Sch Earth Sci, Radiocarbon Dating Lab, Canberra, ACT 0200, Australia. [Schichtel, Bret A.] Colorado State Univ, Cooperat Inst Res Atmosphere, Ft Collins, CO 80523 USA. RP Buchholz, BA (reprint author), Lawrence Livermore Natl Lab, Ctr Accelerator Mass Spectrometry, Mail Stop L-397,POB 808, Livermore, CA 94551 USA. EM buchholz2@llnl.gov RI Fallon, Stewart/G-6645-2011; Buchholz, Bruce/G-1356-2011 OI Fallon, Stewart/0000-0002-8064-5903; NR 26 TC 6 Z9 6 U1 1 U2 24 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0168-583X J9 NUCL INSTRUM METH B JI Nucl. Instrum. Methods Phys. Res. Sect. B-Beam Interact. Mater. Atoms PD JAN PY 2013 VL 294 BP 631 EP 635 DI 10.1016/j.nimb.2012.05.021 PG 5 WC Instruments & Instrumentation; Nuclear Science & Technology; Physics, Atomic, Molecular & Chemical; Physics, Nuclear SC Instruments & Instrumentation; Nuclear Science & Technology; Physics GA 066QC UT WOS:000313234300122 ER PT J AU Kristo, MJ Tumey, SJ AF Kristo, Michael J. Tumey, Scott J. TI The state of nuclear forensics SO NUCLEAR INSTRUMENTS & METHODS IN PHYSICS RESEARCH SECTION B-BEAM INTERACTIONS WITH MATERIALS AND ATOMS LA English DT Article; Proceedings Paper CT 12th International Conference on Accelerator Mass Spectrometry (AMS) CY MAR 20-25, 2011 CL GNS Sci, Wellington, NEW ZEALAND SP GNS Sci, Natl Isotope Ctr, Australian Nucl Sci & Technol Org, High Voltage Engn, Natl Electrostat Corp HO GNS Sci DE Nuclear forensics; Accelerator mass spectrometry; Nuclear Smuggling International Technical Working Group; Uranium ore concentrate attribution ID ACCELERATOR MASS-SPECTROMETRY; URANIUM; CA-41 AB Nuclear terrorism has been identified as one of the most serious security threats facing the world today. Many countries, including the United States, have incorporated nuclear forensic analysis as a component of their strategy to prevent nuclear terrorism. Nuclear forensics involves the laboratory analysis of seized illicit nuclear materials or debris from a nuclear detonation to identify the origins of the material or weapon. Over the years, a number of forensic signatures have been developed to improve the confidence with which forensic analysts can draw conclusions. These signatures are validated and new signatures are discovered through research and development programs and in round-robin exercises among nuclear forensic laboratories. The recent Nuclear Smuggling International Technical Working Group Third Round Robin Exercise and an on-going program focused on attribution of uranium ore concentrate provide prime examples of the current state of nuclear forensics. These case studies will be examined and the opportunities for accelerator mass spectrometry to play a role in nuclear forensics will be discussed. (C) 2012 Elsevier B.V. All rights reserved. C1 [Kristo, Michael J.] Lawrence Livermore Natl Lab, Div Chem Sci, Livermore, CA 94551 USA. [Tumey, Scott J.] Lawrence Livermore Natl Lab, Ctr Accelerator Mass Spectrometry, Livermore, CA 94551 USA. RP Tumey, SJ (reprint author), Lawrence Livermore Natl Lab, Ctr Accelerator Mass Spectrometry, POB 808,L-397, Livermore, CA 94551 USA. EM tumey2@llnl.gov NR 26 TC 28 Z9 28 U1 4 U2 55 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0168-583X J9 NUCL INSTRUM METH B JI Nucl. Instrum. Methods Phys. Res. Sect. B-Beam Interact. Mater. Atoms PD JAN PY 2013 VL 294 BP 656 EP 661 DI 10.1016/j.nimb.2012.07.047 PG 6 WC Instruments & Instrumentation; Nuclear Science & Technology; Physics, Atomic, Molecular & Chemical; Physics, Nuclear SC Instruments & Instrumentation; Nuclear Science & Technology; Physics GA 066QC UT WOS:000313234300127 ER PT J AU Falso, MJS Buchholz, BA AF Falso, Miranda J. Sarachine Buchholz, Bruce A. TI Bomb pulse biology SO NUCLEAR INSTRUMENTS & METHODS IN PHYSICS RESEARCH SECTION B-BEAM INTERACTIONS WITH MATERIALS AND ATOMS LA English DT Article; Proceedings Paper CT 12th International Conference on Accelerator Mass Spectrometry (AMS) CY MAR 20-25, 2011 CL GNS Sci, Wellington, NEW ZEALAND SP GNS Sci, Natl Isotope Ctr, Australian Nucl Sci & Technol Org, High Voltage Engn, Natl Electrostat Corp HO GNS Sci DE Bomb pulse; 14C; Cell biology; Cell turnover ID AGE CALIBRATION; CELL TURNOVER; BONE-COLLAGEN; AMINO-ACIDS; STEM-CELLS; RADIOCARBON; C-14; HUMANS; CONTAMINATION; POPULATION AB The past decade has seen an explosion in use of the C-14 bomb pulse to do fundamental cell biology. Studies in the 1960s used decay counting to measure tissue turnover when the atmospheric C-14/C concentration was changing rapidly. Today bulk tissue measurements are of marginal interest since most of the carbon in the tissue resides in proteins, lipids and carbohydrates that turn over rapidly. Specific cell types with specialized functions are the focus of cell turnover investigations. Tissue samples need to be fresh or frozen. Fixed or preserved samples contain petroleum-derived carbon that has not been successfully removed. Cell or nuclear surface markers are used to sort specific cell types, typically by fluorescence-activated cell sorting (FACS). Specific biomolecules need to be isolated with high purity and accelerator mass spectrometry (AMS) measurements must accommodate samples that generally contain less than 40 mu g of carbon. Furthermore, all separations must not add carbon to the sample. Independent means such as UV absorbance must be used to confirm molecule purity. Approaches for separating specific proteins and DNA and combating contamination of undesired molecules are described. (C) 2012 Elsevier B.V. All rights reserved. C1 [Falso, Miranda J. Sarachine; Buchholz, Bruce A.] Lawrence Livermore Natl Lab, Ctr Accelerator Mass Spectrometry, Livermore, CA 94551 USA. RP Buchholz, BA (reprint author), Lawrence Livermore Natl Lab, Ctr Accelerator Mass Spectrometry, Mail Stop L-397,POB 808, Livermore, CA 94551 USA. EM buchholz2@llnl.gov RI Buchholz, Bruce/G-1356-2011 NR 43 TC 6 Z9 6 U1 4 U2 20 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0168-583X J9 NUCL INSTRUM METH B JI Nucl. Instrum. Methods Phys. Res. Sect. B-Beam Interact. Mater. Atoms PD JAN PY 2013 VL 294 BP 666 EP 670 DI 10.1016/j.nimb.2012.08.045 PG 5 WC Instruments & Instrumentation; Nuclear Science & Technology; Physics, Atomic, Molecular & Chemical; Physics, Nuclear SC Instruments & Instrumentation; Nuclear Science & Technology; Physics GA 066QC UT WOS:000313234300129 ER PT J AU Geier, M Shaddix, CR Holzleithner, F AF Geier, M. Shaddix, C. R. Holzleithner, F. TI A mechanistic char oxidation model consistent with observed CO2/CO production ratios SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Char oxidation; CO2/CO production ratio; Pressure effects; Intrinsic reaction kinetics ID CARBON-OXYGEN REACTION; SURFACE OXIDES; COMBUSTION; BEHAVIOR AB Reliable prediction of char conversion, heat release, and particle temperature during heterogeneous char oxidation relies upon quantitative calculation of the CO2/CO production ratio. This ratio depends strongly on the surface temperature, but also on the local partial pressure of oxygen and thus becomes more important in simulations of oxy-fuel or pressurized combustion systems. Existing semi-empirical intrinsic kinetic models of char combustion have been calibrated against the temperature-dependence of the CO2/CO production ratio, but have neglected the effect of the local oxygen concentration. In this study we employ steady-state analysis to demonstrate the limitations of the existing 3-step semi-global kinetics models and to show the necessity of using a 5-step model to adequately capture the temperature-and oxygen-dependence of the CO2/CO production ratio. A suitable 5-step heterogeneous reaction mechanism is developed and its rate parameters fit to match CO2/CO production data, global reaction orders, and activation energies reported in the literature. The model predictions are interrogated for a broad range of conditions characteristic of pressurized, oxy-fuel, and conventional high-temperature char combustion, for which essentially no experimental information on the CO2/CO production ratio is available. The results suggest that the CO2/CO production ratio may be considerably lower than that estimated with existing power-law correlations for oxygen partial pressures less than 10 kPa and surface temperatures higher than 1600 K. To assist with implementation of the mechanistic CO2/CO production ratio results, an analytical procedure for calculating the CO2/CO production ratio is presented. (C) 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Geier, M.; Shaddix, C. R.] Sandia Natl Labs, Livermore, CA 94551 USA. [Holzleithner, F.] Vienna Univ Technol, A-1060 Vienna, Austria. RP Shaddix, CR (reprint author), Sandia Natl Labs, Livermore, CA 94551 USA. EM mgeier@sandia.gov; crshadd@sandia.gov; franz.holzleith-ner@tuwien.ac.at FU U.S. Department of Energy through the National Energy Technology Laboratory's Power Systems Advanced Research Program; United States Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX This research was sponsored by the U.S. Department of Energy through the National Energy Technology Laboratory's Power Systems Advanced Research Program, managed by Dr. Robert Romanosky. 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 26 TC 14 Z9 15 U1 2 U2 39 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 2411 EP 2418 DI 10.1016/j.proci.2012.07.009 PN 2 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065ES UT WOS:000313131800060 ER PT J AU Sjoberg, M Reuss, DL AF Sjoeberg, Magnus Reuss, David L. TI High-speed imaging of spray-guided DISI engine combustion with near-TDC injection of E85 for ultra-low NO and soot SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE E85; Stratified charge; Spark ignition; Low NOx AB Using E85 fuel, this work demonstrates the use of near-TDC injection and highly turbulent combustion to achieve ultra-low emissions of NO and soot from a DISI engine with a spray-guided, stratified-charge combustion system. Despite the low NO emissions, both combustion efficiency and stability remain relatively high. One striking aspect of engine operation with near-TDC injection is the need to initiate the spark prior to fuel injection. Using E85 fuel, such early spark timing leads to stable ignition. For gasoline, however, such early spark timing leads to misfire under the conditions studied, thereby preventing the use of near-TDC fuel injection to achieve low exhaust emissions of NO. High-speed imaging shows that the early spark timing for E85 allows the spark plasma to develop prior to interacting with one of the fuel jets adjacent to the spark plug, and this contributes to misfire-free operation. The spark-spray interactions generate a very fast spread of either weak or thin flames throughout a large fraction of the piston bowl prior to the main combustion event. The short delay between the near-TDC fuel injection and the combustion event are believed to enhance the mixing rates during the combustion compared to the use of earlier injection, which may contribute to the low NO emissions. (C) 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Sjoeberg, Magnus; Reuss, David L.] Sandia Natl Labs, Livermore, CA 94551 USA. RP Sjoberg, M (reprint author), Sandia Natl Labs, MS 9053,POB 969, Livermore, CA 94551 USA. EM mgsjobe@sandia.gov FU U.S. Department of Energy, Office of Vehicle Technologies; United States Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX Financial support was provided by the U.S. Department of Energy, Office of Vehicle Technologies. Sandia is a multiprogram laboratory operated by the Sandia Corporation, a Lockheed Martin Company, for the United States Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000. NR 13 TC 11 Z9 11 U1 1 U2 17 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 2933 EP 2940 DI 10.1016/j.proci.2012.05.033 PN 2 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065ES UT WOS:000313131800120 ER PT J AU Yoo, CS Luo, ZY Lu, TF Kim, H Chen, JH AF Yoo, Chun Sang Luo, Zhaoyu Lu, Tianfeng Kim, Hongjip Chen, Jacqueline H. TI A DNS study of ignition characteristics of a lean iso-octane/air mixture under HCCI and SACI conditions SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE DNS; HCCI; Spark-assisted compression ignition (SACI); Iso-octane/air reduced mechanism; Thermal stratification ID DIRECT NUMERICAL-SIMULATION; FRONT PROPAGATION; TEMPERATURE INHOMOGENEITIES; REDUCED MECHANISM; AIR COUNTERFLOW; CONSTANT VOLUME; HEATED COFLOW; JET FLAME; HYDROGEN; STABILIZATION AB The effect of thermal stratification, spark-ignition, and turbulence on the ignition of a lean homogeneous iso-octane/air mixture at constant volume and high pressure is investigated by direct numerical simulations (DNS) with a new 99-species reduced kinetic mechanism developed for very lean mixtures from a detailed mechanism. Two-dimensional DNS are performed in a fixed volume with two-dimensional isotropic velocity spectrums, temperature fluctuations, and an ignition source superimposed on the initial scalar fields. The influence of variations in the initial temperature field imposed by changing the variance of temperature, the ignition-timing by changing the time at which the ignition source is superimposed, and the turbulence intensity and length scale on ignition of a lean iso-octane/air mixture is elucidated. The mean heat release rate increases more slowly and ignition delay decreases with increasing thermal stratification under homogeneous charge compression-ignition (HCCI) conditions since the present mean temperature lies far outside of the negative temperature coefficient (NTC) regime. The spark-ignition induces relatively short ignition delay under spark-assisted compression ignition (SACI) conditions while mildly spreading out the mean heat release rate. For SACI combustion, high turbulence intensity decreases the ignition delay more by increasing the turbulent flame area. Displacement speed and Damkohler number analyses reveal that the high degree of thermal stratification induces deflagration at the reaction fronts, and hence, the mean heat release rate is smoother subsequent to thermal runaway occurring at the highest temperature regions in the domain. For SACI combustion, the heat release rate occurs solely by deflagration prior to the occurrence of the maximum heat release rate and subsequently by mixed modes of deflagration and spontaneous ignition. These results suggest that thermal stratification provides smooth operation of HCCI engines and moreover, spark-ignition can precisely control the ignition timing for SACI combustion. (C) 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Yoo, Chun Sang] Ulsan Natl Inst Sci & Technol UNIST, Sch Mech & Adv Mat Engn, Ulsan 689798, South Korea. [Luo, Zhaoyu; Lu, Tianfeng] Univ Connecticut, Dept Mech Engn, Storrs, CT 06269 USA. [Kim, Hongjip] Chungnam Natl Univ, Dept Mech Engn, Taejon 305764, South Korea. [Chen, Jacqueline H.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. RP Yoo, CS (reprint author), Ulsan Natl Inst Sci & Technol UNIST, Sch Mech & Adv Mat Engn, Ulsan 689798, South Korea. EM csyoo@unist.ac.kr RI Yoo, Chun Sang/E-5900-2010; Lu, Tianfeng/D-7455-2014 OI Yoo, Chun Sang/0000-0003-1094-4016; Lu, Tianfeng/0000-0001-7536-1976 FU Basic Science Research Program through the National Research Foundation of Korea (NRF); Ministry of Education, Science and Technology [2011-0008201, 2012-0001550]; Human Resources Development of the Korea Institute of Energy Technology Evaluation and Planning (KETEP); Korea government Ministry of Knowledge Economy [20114030200010]; Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences; Office of Advanced Scientific Computing Research of the US Department of Energy; Combustion Energy Frontier Research Center, an Energy Frontier Research Center; US Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001198]; National Science Foundation [0904771] FX The work at Ulsan National Institute of Science and Technology was supported by Basic Science Research Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Education, Science and Technology (No. 2011-0008201) and the Human Resources Development of the Korea Institute of Energy Technology Evaluation and Planning (KETEP) grant funded by the Korea government Ministry of Knowledge Economy (No. 20114030200010). The work at Sandia National Laboratories (SNL) was supported by the Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, and Office of Advanced Scientific Computing Research of the US Department of Energy. JHC was also supported as part of the Combustion Energy Frontier Research Center, an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Office of Basic Energy Sciences under Award Number DE-SC0001198. The work at University of Connecticut was supported by the National Science Foundation under Grant 0904771. The work at Chungnam National University was supported by Basic Science Research Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Education, Science and Technology (No. 2012-0001550). NR 33 TC 32 Z9 32 U1 3 U2 51 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 2985 EP 2993 DI 10.1016/j.proci.2012.05.019 PN 2 PG 9 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065ES UT WOS:000313131800126 ER PT J AU Westbrook, CK Pitz, WJ Sarathy, SM Mehl, M AF Westbrook, C. K. Pitz, W. J. Sarathy, S. M. Mehl, M. TI Detailed chemical kinetic modeling of the effects of C=C double bonds on the ignition of biodiesel fuels SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Reaction mechanisms; Ignition; Diesel engines; Biodiesel fuels ID JET-STIRRED REACTOR; N-HEPTANE OXIDATION; METHYL OLEATE; REACTION-MECHANISM; LOW-TEMPERATURE; SHOCK-TUBE; COMBUSTION; HYDROCARBONS; AUTOIGNITION; ALKANES AB A detailed chemical kinetic reaction mechanism previously developed to study combustion of soy and rapeseed oil methyl ester biodiesel fuels is used to simulate combustion of many other biodiesel fuels derived from different vegetable oils and animal fats. All of these biodiesel fuels consist of unique mixtures of the same five individual, single-component methyl esters, including methyl stearate, methyl oleate, methyl linoleate, methyl linolenate, and methyl palmitate. The stearate and palmitate molecules are saturated, while the oleate, linoleate and linolenate have one, two and three C=C double bonds, respectively. Each plant-or fat-derived biodiesel fuel that is made from the same five components has variations in combustion properties that depend on differences in the relative fractions of these five components. The present study focuses on ignition properties of these oil-and fat-derived biodiesel fuels and on their cetane numbers (CN), which measure relative ignition rates under diesel engine operating conditions. A key factor determining differences in ignition properties and CN of the many methyl ester diesel fuels is shown to be the number of C=C double bonds in the long carbon chains of each component molecule, with each C=C double bond reducing the CN value by a significant amount. Each C=C double bond provides allylic sites where H atoms are easily abstracted, but these allylic radical sites are shown to be weak bonding sites for molecular oxygen that do not support subsequent isomerization reactions that lead to low temperature reactivity and ignition. This reduced rate of low temperature reactivity is responsible for the reductions in CN due to the presence of these C=C double bonds. The amount of reduction in low temperature reactivity is roughly proportional to the number of C=C double bonds in each biodiesel fuel molecule, relative to the saturated components of biodiesel fuel. (C) 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Westbrook, C. K.] Lawrence Livermore Natl Lab, Phys & Life Sci Directorate, Livermore, CA 94551 USA. RP Westbrook, CK (reprint author), Lawrence Livermore Natl Lab, Phys & Life Sci Directorate, 7000 East Ave,POB 808, Livermore, CA 94551 USA. EM westbrookck@earthlink.net RI Sarathy, S. Mani/M-5639-2015; Mehl, Marco/A-8506-2009 OI Sarathy, S. Mani/0000-0002-3975-6206; Mehl, Marco/0000-0002-2227-5035 FU US Department of Energy, Office of Vehicle Technologies; Office of Basic Energy Sciences; US Department of Energy by Lawrence Livermore National Laboratory [DE-AC52-07NA27344] FX The authors are grateful for valuable discussions with Dr. C. V. Naik, Prof. A. M. Dean, and Dr. S. Klippenstein. This work was supported by the US Department of Energy, Office of Vehicle Technologies and the Office of Basic Energy Sciences, and the authors thank program managers Gurpreet Singh, Kevin Stork, and Wade Sisk. This work was performed under the auspices of the US Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344. NR 27 TC 33 Z9 34 U1 7 U2 62 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 3049 EP 3056 DI 10.1016/j.proci.2012.05.025 PN 2 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065ES UT WOS:000313131800133 ER PT J AU Lee, KO Seong, H Choi, SM AF Lee, Kyeong O. Seong, Heeje Choi, Seung M. TI Detailed analysis of kinetic reactions in soot oxidation by simulated diesel exhaust emissions SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Diesel emissions; DPF; Soot oxidation; Kinetic parameters; Activation energy ID THERMOGRAVIMETRIC ANALYSIS; OXYGEN; PARAMETERS; DPF; NO2 AB Development of an advanced diesel particulate filter system requires efficient regeneration strategies, which, in turn, require a comprehensive understanding of soot oxidation kinetics. A goal of this study is first to define the effect of inert balance gases and heating rates used for thermogravimetric analyses on soot oxidation, with applying different analytic methodologies to the calculation of kinetic parameters. We identified an inert gas-independent activation energy value of surrogate soot to be 155 kJ/mole, evaluated at a heating rate of 1 degrees C/min, and proposed the differential method for evaluating kinetic parameters. Using the results, we conducted subsequent non-isothermal soot oxidation experiments to characterize the effects of reactant gases (NO, NO2, CO2, and O-2) in the various compositions of gas mixtures simulating diesel exhaust emissions. Notable results include the following. With no O-2 in the mixtures, NO gases rarely affected soot oxidation, while CO2 effects also appeared to be minor. In the presence of a constant NO2 concentration, the increased O-2 concentration (particularly up to 4%) significantly enhanced soot oxidation. In the case of a constant O-2 concentration, increasing the NO2 concentration promoted soot oxidation in a fairly low temperature range of 200-580 degrees C. These O-2 and NO2 effects turned out to be quite significant and temperature dependent. Overall, a higher degree of oxidation was observed with the mixture composition simulated for the higher engine load. The Arrhenius plots exhibited two distinct linear regression lines as NO2 was present in the mixture, where the low temperature linearity range was extended with increasing NO2 concentration. The activation energy quite significantly decreased from 153 to 39 kJ/mole in the low temperature range, as NO2 concentration increased from 0 to 1250 ppm. In the high temperature range, however, the activation energy changed only slightly between 153 and 159 kJ/mole, indicating negligible dependence on mixture compositions. (C) 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Lee, Kyeong O.; Seong, Heeje; Choi, Seung M.] Argonne Natl Lab, Transportat Technol R&D Ctr, Argonne, IL 60439 USA. RP Lee, KO (reprint author), Argonne Natl Lab, Transportat Technol R&D Ctr, 9700 S Cass Ave, Argonne, IL 60439 USA. EM klee@anl.gov FU Advanced Engine Combustion Program FX This work is supported by the Advanced Engine Combustion Program operated by the Office of Vehicle Technologies of the U.S. Department of Energy. NR 20 TC 9 Z9 10 U1 5 U2 43 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 3057 EP 3065 DI 10.1016/j.proci.2012.06.121 PN 2 PG 9 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065ES UT WOS:000313131800134 ER PT J AU Davis, DW Therkelsen, PL Littlejohn, D Cheng, RK AF Davis, D. W. Therkelsen, P. L. Littlejohn, D. Cheng, R. K. TI Effects of hydrogen on the thermo-acoustics coupling mechanisms of low-swirl injector flames in a model gas turbine combustor SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Gas turbines; Combustion oscillations; Hydrogen; Lean premixed; Swirl ID PREMIXED FLAMES; OSCILLATIONS; DYNAMICS AB The effects of hydrogen on the dynamic response of self-excited oscillations in a model low-swirl injector (LSI) gas turbine combustor have been studied by high-speed imaging of flame light emissions and OH* chemiluminescence on two thermoacoustically coupled unsteady flames burning CH4 (113 kW) and a fuel blend of 0.9H2/0.1CH(4) (74 kW). The two flames have different shapes. The CH4 flame is lifted and bowl-shaped and the 0.9H2/0.1CH(4) flame is attached and M-shaped. From phase-resolved PIV, the dominant unsteady flow structures of both flames are ring vortices shed from the LSI exit rim. The vortices of the CH4 flame burn intermittently and those in the 0.9H2/0.1CH(4) flame burn consistently. Proper orthogonal decomposition analysis of OH* and calculation of Rayleigh indices show different flame structures are responsible for generating flame oscillations and acoustic coupling. CH4 flame oscillations are associated with flame folding near the standing ring vortex below the trailing edge of the lifted flame, intermittent burning of the shear layer, and irregular acoustic driving. The 0.9H2/0.1CH(4) flame has regular and stronger forcing. A key contributor to the 0.9H2/0.1CH(4) flame driving is merging of the central flat flame with the reacting rolled-up vortices, resulting in an instantaneous narrow band of localized high heat release density that is in phase with the pressure oscillation. Cyclic variations in the flow of the reactants also contribute to non-linear effects. High reactivity of H-2 generates a situation where the geometry of the attached shear layer flame and central disk-shaped flame creates a very favorable situation for exciting higher-pressure oscillations at a lower total heat release than CH4 flames. To control combustion oscillations in a fuel-flexible LSI gas turbine combustor, the mitigation of flame attachment and/or formation of the outer shear layer would be necessary. (C) 2012 United Technologies Corporation and The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Davis, D. W.] United Technol Res Ctr, E Hartford, CT 06108 USA. [Therkelsen, P. L.; Littlejohn, D.; Cheng, R. K.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Cheng, RK (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, MS 70-108B,1 Cyclotron Rd, Berkeley, CA 94720 USA. EM RKCheng@lbl.gov FU Assistant Secretary for Fossil Energy, Advanced Turbines Program, of the U. S. Department of Energy [DE-AC02-05CH11231] FX This work was supported by the Assistant Secretary for Fossil Energy, Advanced Turbines Program, of the U. S. Department of Energy under Contract No. DE-AC02-05CH11231. NR 30 TC 9 Z9 10 U1 4 U2 27 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 3135 EP 3143 DI 10.1016/j.proci.2012.05.050 PN 2 PG 9 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065ES UT WOS:000313131800143 ER PT J AU Gao, Y Bohlin, A Seeger, T Bengtsson, PE Kliewer, CJ AF Gao, Yi Bohlin, Alexis Seeger, Thomas Bengtsson, Per-Erik Kliewer, Christopher J. TI In situ determination of N-2 broadening coefficients in flames for rotational CARS thermometry SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Time-resolved spectroscopy; Raman linewidths; CARS; Ultrafast; Soot ID STOKES-RAMAN SCATTERING; LASER-INDUCED INCANDESCENCE; SINGLE-SHOT THERMOMETRY; TEMPERATURE-MEASUREMENTS; Q BRANCH; SPECTROSCOPY; SOOT; SPECTRA; MIXTURES; O-2 AB Total N-2 S-branch broadening coefficients have been measured in situ as a function of radial position in a highly sooting ethylene diffusion flame by the use of time-resolved dual-broadband picosecond pure rotational CARS (RCARS). Time-domain measurements of the J-dependent N-2 rotational coherence decays in the flame were used to determine the broadening coefficients, and these coefficients were then used in the spectral fitting routine for the determination of temperature and [O-2]/[N-2] ratio in the flame. Corrections of up to 125 K are found when compared to spectral fitting using an ECS self-broadened N-2 linewidth model. The presented technique effectively takes into account contributions to the N-2 linewidths from all collision partners without any a priori knowledge of relative species concentrations. Published by Elsevier Inc. on behalf of The Combustion Institute. C1 [Gao, Yi; Seeger, Thomas] Univ Erlangen Nurnberg, Inst Engn Thermodynam LTT, D-91058 Erlangen, Germany. [Gao, Yi; Seeger, Thomas] Univ Erlangen Nurnberg, Erlangen Grad Sch Adv Opt Technol, D-91058 Erlangen, Germany. [Bohlin, Alexis; Bengtsson, Per-Erik] Lund Univ, Div Combust Phys, S-22100 Lund, Sweden. [Seeger, Thomas] Univ Siegen, Lehrstuhl Tech Thermodynam, D-57072 Siegen, Germany. [Kliewer, Christopher J.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. RP Kliewer, CJ (reprint author), Sandia Natl Labs, Combust Res Facil, POB 969,MS 9055, Livermore, CA 94551 USA. EM cjkliew@sandia.gov RI Kliewer, Christopher/E-4070-2010; Bohlin, Alexis/L-8973-2015; Seeger, Thomas/C-3951-2017 OI Kliewer, Christopher/0000-0002-2661-1753; Bohlin, Alexis/0000-0003-4383-8332; Seeger, Thomas/0000-0002-9145-5910 FU U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences; U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000]; Swedish Energy Agency; Centre of Combustion Science and Technology (CE-COST); Erlangen Graduate School in Advanced Optical Technologies (SAOT) by German National Science Foundation (DFG) FX Primary funding provided by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences. 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-AC04-94AL85000. AB acknowledges the financial support of the Swedish Energy Agency and the Centre of Combustion Science and Technology (CE-COST). YG acknowledges the funding of the Erlangen Graduate School in Advanced Optical Technologies (SAOT) by German National Science Foundation (DFG) in the framework of the German excellence initiative. NR 32 TC 7 Z9 7 U1 1 U2 21 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 3637 EP 3644 DI 10.1016/j.proci.2012.05.010 PN 2 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065ES UT WOS:000313131800198 ER PT J AU Kopeliovich, BZ Morfin, JG Schmidt, I AF Kopeliovich, Boris Z. Morfin, Jorge G. Schmidt, Ivan TI Nuclear shadowing in electro-weak interactions SO PROGRESS IN PARTICLE AND NUCLEAR PHYSICS LA English DT Review DE Lepton; Nucleus; Shadowing ID INELASTIC MUON SCATTERING; STRUCTURE-FUNCTION RATIOS; PARTON DISTRIBUTION-FUNCTIONS; TOTAL CROSS-SECTIONS; R=SIGMA-L/SIGMA-T; HIGH-ENERGY COLLISIONS; COLOR DIPOLE PICTURE; GLOBAL QCD ANALYSIS; DRELL-YAN PROCESS; SMITH SUM-RULE AB Shadowing is a quantum phenomenon leading to a non-additivity of electroweak cross sections on nucleons bound in a nucleus. It occurs due to destructive interference of amplitudes on different nucleons. Although the current experimental evidence for shadowing is dominated by charged-lepton-nucleus scattering, studies of neutrino-nucleus scattering have recently begun and revealed unexpected results. (c) 2012 Elsevier B.V. All rights reserved. C1 [Kopeliovich, Boris Z.; Schmidt, Ivan] Univ Tecn Federico Santa Maria, Dept Fis, Valparaiso, Chile. [Kopeliovich, Boris Z.; Schmidt, Ivan] Inst Estudios Avanzados Ciencias & Ingn, Valparaiso, Chile. [Kopeliovich, Boris Z.; Schmidt, Ivan] Ctr Cient Tecnol Valparaiso, Valparaiso, Chile. [Morfin, Jorge G.] Fermilab Natl Accelerator Lab, Batavia, IL 60510 USA. RP Morfin, JG (reprint author), Fermilab Natl Accelerator Lab, Batavia, IL 60510 USA. EM morfin@fnal.gov RI sebastianovitsch, stepan/G-8507-2013 FU Fondecyt (Chile) [1090291, 1100287]; Alliance Program of the Helmholtz Association [HA216/EMMI]; Fermi Research Alliance, LLC with the United States Department of Energy [De-AC02-07CH11359] FX This work was supported in part by Fondecyt (Chile) grants 1090291 and 1100287. The work of B.Z.K. was supported also by the Alliance Program of the Helmholtz Association, contract HA216/EMMI "Extremes of Density and Temperature: Cosmic Matter in the Laboratory". Fermilab is operated by Fermi Research Alliance, LLC under Contract No. De-AC02-07CH11359 with the United States Department of Energy. NR 239 TC 10 Z9 10 U1 0 U2 3 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0146-6410 EI 1873-2224 J9 PROG PART NUCL PHYS JI Prog. Part. Nucl. Phys. PD JAN PY 2013 VL 68 BP 314 EP 372 DI 10.1016/j.ppnp.2012.09.004 PG 59 WC Physics, Nuclear; Physics, Particles & Fields SC Physics GA 059ET UT WOS:000312687900006 ER PT J AU Yuan, SH Chen, MJ Mao, XH Alshawabkeh, AN AF Yuan, Songhu Chen, Mingjie Mao, Xuhui Alshawabkeh, Akram N. TI A three-electrode column for Pd-catalytic oxidation of TCE in groundwater with automatic pH-regulation and resistance to reduced sulfur compound foiling SO WATER RESEARCH LA English DT Article DE Pd; Electrolytic; TCE; Groundwater remediation; Reduced sulfur compounds ID DIAMOND FILM ELECTRODES; HYDROXYL RADICALS; ELECTROCHEMICAL OXIDATION; HYDROGEN-PEROXIDE; WATER-TREATMENT; HYDRODECHLORINATION; DECHLORINATION; TRICHLOROETHYLENE; DEGRADATION; GENERATION AB A hybrid electrolysis and Pd-catalytic oxidation process is evaluated for degradation of trichloroethylene (TCE) in groundwater. A three-electrode, one anode and two cathodes, column is employed to automatically develop a low pH condition in the Pd vicinity and a neutral effluent. Simulated groundwater containing up to 5 mM bicarbonate can be acidified to below pH 4 in the Pd vicinity using a total of 60 mA with 20 mA passing through the third electrode. By packing 2 g of Pd/Al2O3 pellets in the developed acidic region, the column efficiency for TCE oxidation in simulated groundwater (5.3 mg/L TCE) increases from 44 to 59 and 68% with increasing Fe(II) concentration from 0 to 5 and 10 mg/L, respectively. Different from Pd-catalytic hydrodechlorination under reducing conditions, this hybrid electrolysis and Pd-catalytic oxidation process is advantageous in controlling the fouling caused by reduced sulfur compounds (RSCs) because the in situ generated reactive oxidizing species, i.e., O-2, H2O2 and center dot OH, can oxidize RSCs to some extent. In particular, sulfite at concentrations less than 1 mM even greatly increases TCE oxidation by the production of SO4 center dot-, a strong oxidizing radical, and more center dot OH. (C) 2012 Elsevier Ltd. All rights reserved. C1 [Yuan, Songhu] China Univ Geosci, State Key Lab Biogeol & Environm Geol, Wuhan 430074, Peoples R China. [Yuan, Songhu; Mao, Xuhui; Alshawabkeh, Akram N.] Northeastern Univ, Dept Civil & Environm Engn, Boston, MA 02115 USA. [Chen, Mingjie] Lawrence Livermore Natl Lab, Atmospher Earth & Energy Div, Livermore, CA 94550 USA. RP Yuan, SH (reprint author), Northeastern Univ, Dept Civil & Environm Engn, 400 Snell Engn,360 Huntington Ave, Boston, MA 02115 USA. EM yuansonghu622@hotmail.com; aalsha@coe.neu.edu OI Mao, Xuhui/0000-0003-1720-255X FU US National Institute of Environmental Health Sciences (NIEHS) [P42ES017198]; Natural Science Foundation of China (NSFC) [41172220]; Fundamental Research Funds for the Central Universities, China University of Geosciences (Wuhan) [CUGL110608] FX This work was supported by the US National Institute of Environmental Health Sciences (NIEHS, Grant No. P42ES017198), the Natural Science Foundation of China (NSFC, No. 41172220), and the Fundamental Research Funds for the Central Universities, China University of Geosciences (Wuhan) (No. CUGL110608). We appreciate the assistance in ESR assay by Prof. David Budil and Mr. Xianzhe Wang in Department of Chemistry & Chemical Biology, Northeastern University. The content is solely the responsibility of the authors and does not necessarily represent the official views of the NIEHS, the National Institutes of Health or Lawrence Livermore National Security, LLC. NR 48 TC 23 Z9 23 U1 9 U2 75 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0043-1354 J9 WATER RES JI Water Res. PD JAN 1 PY 2013 VL 47 IS 1 BP 269 EP 278 DI 10.1016/j.watres.2012.10.009 PG 10 WC Engineering, Environmental; Environmental Sciences; Water Resources SC Engineering; Environmental Sciences & Ecology; Water Resources GA 068SK UT WOS:000313386300028 PM 23121896 ER PT J AU Baker, EN Dauter, Z AF Baker, Edward N. Dauter, Zbigniew TI Celebrating biological crystallography: Acta D twenty years on SO ACTA CRYSTALLOGRAPHICA SECTION D-BIOLOGICAL CRYSTALLOGRAPHY LA English DT Editorial Material C1 [Baker, Edward N.] Univ Auckland, Sch Biol Sci, Auckland 1, New Zealand. [Dauter, Zbigniew] Argonne Natl Lab, Biosci Div, Argonne, IL 60439 USA. RP Baker, EN (reprint author), Univ Auckland, Sch Biol Sci, Private Bag 92-019, Auckland 1, New Zealand. NR 0 TC 0 Z9 0 U1 0 U2 0 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0907-4449 J9 ACTA CRYSTALLOGR D JI Acta Crystallogr. Sect. D-Biol. Crystallogr. PD JAN PY 2013 VL 69 BP 1 EP 1 DI 10.1107/S0907444912051190 PN 1 PG 1 WC Biochemical Research Methods; Biochemistry & Molecular Biology; Biophysics; Crystallography SC Biochemistry & Molecular Biology; Biophysics; Crystallography GA 061RU UT WOS:000312866500001 ER PT J AU Dauter, Z AF Dauter, Zbigniew TI Placement of molecules in (not out of) the cell SO ACTA CRYSTALLOGRAPHICA SECTION D-BIOLOGICAL CRYSTALLOGRAPHY LA English DT Editorial Material AB To uniquely describe a crystal structure, it is sufficient to specify the crystal unit cell and symmetry, and describe the unique structural motif which is repeated by the space-group symmetry throughout the whole crystal. It is somewhat arbitrary how such a unique motif can be defined and positioned with respect to the unit-cell origin. As a result of such freedom, some isomorphous structures are presented in the Protein Data Bank in different locations and appear as if they have different atomic coordinates, despite being completely equivalent structurally. This may easily confuse those users of the PDB who are less familiar with crystallographic symmetry transformations. It would therefore be beneficial for the community of PDB users to introduce standard rules for locating crystal structures of macromolecules in the unit cells of various space groups. C1 NCI, Synchrotron Radiat Res Sect, Argonne Natl Lab, Argonne, IL 60439 USA. RP Dauter, Z (reprint author), NCI, Synchrotron Radiat Res Sect, Argonne Natl Lab, Argonne, IL 60439 USA. EM dauter@anl.gov NR 5 TC 3 Z9 3 U1 0 U2 2 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0907-4449 J9 ACTA CRYSTALLOGR D JI Acta Crystallogr. Sect. D-Biol. Crystallogr. PD JAN PY 2013 VL 69 BP 2 EP 4 DI 10.1107/S0907444912044794 PN 1 PG 3 WC Biochemical Research Methods; Biochemistry & Molecular Biology; Biophysics; Crystallography SC Biochemistry & Molecular Biology; Biophysics; Crystallography GA 061RU UT WOS:000312866500002 PM 23275157 ER PT J AU Culp, L Caucci, L AF Culp, Lindsay Caucci, Lisa TI State Adolescent Consent Laws and Implications for HIV Pre-Exposure Prophylaxis SO AMERICAN JOURNAL OF PREVENTIVE MEDICINE LA English DT Review AB Background: Recent large clinical trials have found that pre-exposure prophylaxis (PrEP) reduced HIV infection among men who have sex with men (MSM), but efforts to provide clinical care to minors, including young MSM, may be complicated by a lack of clarity regarding parental consent requirements with respect to medical services. Purpose: The goal of this paper was to analyze law related to a minor's ability to consent to medical care, including HIV diagnostic testing and treatment, and its implications for PrEP. Methods: Analysis was performed in 2012 on laws current as of December 31, 2011. Public Health Law Program staff collected all statutes and regulations pertaining to an adolescent's ability to consent to HIV diagnostic testing and treatment and sexually transmitted infection (STI) diagnostic testing, treatment, and prevention. Results: No state expressly prohibits minors' access to PrEP or other HIV prevention methods. All jurisdictions expressly allow some minors to consent to medical care for the diagnosis or treatment of STIs, but only eight jurisdictions allow consent to preventive or prophylactic services. Thirty-four states either expressly allow minors to consent to HIV services or allow consent to STI or communicable disease services and classify HIV as an STI or communicable disease. Seventeen jurisdictions allow minors to consent to STI testing and treatment, but they do not have an express HIV provision nor classify HIV as an STI or communicable disease. Conclusions: Minors' access to PrEP without parental consent is unclear, and further analysis is needed to evaluate how state law may relate to the provision of clinical interventions for the prevention of HIV infection. (Am J Prev Med 2013;44(1S2):S119-S124) Published by Elsevier Inc. on behalf of American Journal of Preventive Medicine C1 [Culp, Lindsay] CDC, Publ Hlth Law Program, Off Tribal Local & Territorial Support, Atlanta, GA 30341 USA. [Caucci, Lisa] Oak Ridge Inst Sci & Educ, Atlanta, GA USA. RP Culp, L (reprint author), CDC, Publ Hlth Law Program, Off Tribal Local & Territorial Support, 4770 Buford Highway,MS E-70, Atlanta, GA 30341 USA. EM lculp@cdc.gov FU CDC through the Association for Prevention Teaching and Research (CDC-APTR) [11-NCHHSTP-01] FX Publication of this article was supported by the CDC through the Association for Prevention Teaching and Research (CDC-APTR) Cooperative Agreement number 11-NCHHSTP-01. NR 11 TC 9 Z9 9 U1 0 U2 4 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 0749-3797 J9 AM J PREV MED JI Am. J. Prev. Med. PD JAN PY 2013 VL 44 IS 1 SU 2 BP S119 EP S124 DI 10.1016/j.amepre.2012.09.044 PG 6 WC Public, Environmental & Occupational Health; Medicine, General & Internal SC Public, Environmental & Occupational Health; General & Internal Medicine GA 056YL UT WOS:000312528000011 PM 23253751 ER PT J AU Chakoumakos, BC Horita, J Garlea, VO AF Chakoumakos, Bryan C. Horita, Juske Garlea, Vasile O. TI H/D isotope effects in brucite at low temperatures SO AMERICAN MINERALOGIST LA English DT Article DE Rietveld refinement; brucite; neutron diffraction; isotope effect ID NEUTRON-DIFFRACTION; HIGH-PRESSURE; STRUCTURAL REFINEMENT; COMPRESSION MECHANISM; THERMAL-EXPANSION; MG(OH)(2); GPA; PORTLANDITE; PHASE; WATER AB Joint refinement of powder neutron diffraction data of hydrogenated and deuterated brucite over the temperature range of 10-295 K clearly shows significant isotope effects in the structural parameters. Mg(OH)(2) has a 0.31% larger volume than that of Mg(OD)(2) at room temperature, which is mostly due to the c-axis expansion of Mg(OH)(2) as compared to Mg(OD)(2). The isotope effect in the a-axis has the opposite, but smaller, behavior as compared to the c-axis. These differences are slightly enhanced with reduction of the cell volume upon cooling. The temperature dependence of the isotropic atomic displacement parameters (ADPs) with the single site model show that the ADP of the H atom is approximately larger than that of the D atom by the amount expected from the reduced-mass difference, but this difference is not evident with the split site model. Despite the shorter c-axis of the deuterated form, nearest-neighbor D center dot center dot center dot D distances are longer than the H center dot center dot center dot H distances, because the O-H distances are longer than the O-D distances, which necessarily places the H atoms closer together by 0.03 angstrom or more within the interlayer space. This study showcases an example of when a joint Rietveld refinement is ideally suited, by combining data for the deuterated and hydrogenated forms of brucite. The approach reduces the number of least-squares variables, and reduces the systematic errors. It can be a general method to analyze isotope effects in materials studied by neutron diffraction. C1 [Chakoumakos, Bryan C.; Garlea, Vasile O.] Oak Ridge Natl Lab, Quantum Condensed Matter Div, Oak Ridge, TN 37831 USA. [Horita, Juske] Texas Tech Univ, Dept Geosci, Lubbock, TX 79409 USA. RP Chakoumakos, BC (reprint author), Oak Ridge Natl Lab, Quantum Condensed Matter Div, POB 2008, Oak Ridge, TN 37831 USA. EM chakoumakobc@ornl.gov RI Garlea, Vasile/A-4994-2016; Chakoumakos, Bryan/A-5601-2016 OI Garlea, Vasile/0000-0002-5322-7271; Chakoumakos, Bryan/0000-0002-7870-6543 FU Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy FX Research at Oak Ridge National Laboratory's High Flux Isotope Reactor was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy. NR 37 TC 5 Z9 5 U1 0 U2 30 PU MINERALOGICAL SOC AMER PI CHANTILLY PA 3635 CONCORDE PKWY STE 500, CHANTILLY, VA 20151-1125 USA SN 0003-004X J9 AM MINERAL JI Am. Miner. PD JAN PY 2013 VL 98 IS 1 BP 1 EP 6 DI 10.2138/am.2013.4202 PG 6 WC Geochemistry & Geophysics; Mineralogy SC Geochemistry & Geophysics; Mineralogy GA 065KZ UT WOS:000313148500001 ER PT J AU Xiong, YL AF Xiong, Yongliang TI A thermodynamic model for silica and aluminum in alkaline solutions with high ionic strength at elevated temperatures up to 100 degrees C: Applications to zeolites SO AMERICAN MINERALOGIST LA English DT Article DE Pitzer equation; solution chemistry; sodium silicates; hydrothermal synthesis ID HOT SODIUM-HYDROXIDE; EQUILIBRIUM-CONSTANTS; ACTIVITY-COEFFICIENTS; TANK WASTE; SOLUBILITY; DISSOLUTION; KINETICS; ACID; CRYSTALLIZATION; 300-DEGREES-C AB In this study, a thermodynamic model for silica and aluminum in high ionic strength solutions at elevated temperatures up to 100 degrees C is constructed. Pitzer equations are utilized for the thermodynamic model construction. This model is valid up to ionic strengths of similar to 24 molal (m) in NaOH solutions with silicate concentrations up to similar to 1.5 m. The speciation of silica (including monomers and polymers) and aluminum at elevated temperatures is taken into account. Also, the equilibrium constants for silicic acid and its polymer species (H4SiO4, H5Si2O7-, H4Si2O3-, and H5Si3O3-) at elevated temperatures up to 100 degrees C, are obtained based on theoretical calculations. Using this thermodynamic model, thermodynamic properties, including equilibrium constants, and respective reaction enthalpies are obtained for sodium silicates, zeolite A, and the amorphous form of zeolite A, based on solubility experiments at elevated temperatures. The equilibrium constants for zeolite A and amorphous precursor of zeolite A regarding the following reactions up to 100 degrees C, NaAlSiO4 center dot 2.25H(2)O(cr) + 4H(+) = Na+ + Al3+ + H4SiO4(aq) + 2.25H(2)O(1) (1) and NaAlSiO4-2.25H(2)O(am) + 4H(+) = Na+ + Al3+ + H4SiO4(aq) + 2.25H(2)O(1) (2) can be expressed as follows log K-1 = 7963 +/- 327/T - 16.46 +/- 0.96 and log K-2 = 12971 +/- 160/T - 30.80 +/- 0.50 where T is temperature in Kelvin. The enthalpy of formation from elements, Gibbs free energy of formation from elements, and standard entropy derived for zeolite A and the amorphous form of zeolite A with the chemical formulas mentioned above at 25 degrees C and 1 bar are -2738 +/- 5 kJ/mol, -2541 +/- 2 kJ/mol, 373 +/- 10 J/(K.mol); and -2642 +/- 3 kJ/mol, -2527 +/- 2 kJ/mol, and 648 +/- 10 J/(K.mol), respectively. The enthalpy of formation from elements for zeolite A derived in this study based on solubility experiments in hydrothermal solutions agrees well with those obtained by calorimetric measurements and by theoretical calculations. C1 Sandia Natl Labs, Carlsbad Programs Grp, Carlsbad, NM 88220 USA. RP Xiong, YL (reprint author), Sandia Natl Labs, Carlsbad Programs Grp, 4100 Natl Pk Highway, Carlsbad, NM 88220 USA. EM yxiong@sandia.gov FU U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX Sandia National Laboratories is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000. The author thanks Bill Bourcier, Philip Neuhoff, and an anonymous reviewer for their detailed and insightful reviews, which have significantly improved the quality of the presentation. The journal editors, Jenny Thomson, Keith Putirka, and the associate editor, Rick Wilkin, are thanked for their editorial efforts. NR 60 TC 3 Z9 3 U1 4 U2 37 PU MINERALOGICAL SOC AMER PI CHANTILLY PA 3635 CONCORDE PKWY STE 500, CHANTILLY, VA 20151-1125 USA SN 0003-004X J9 AM MINERAL JI Am. Miner. PD JAN PY 2013 VL 98 IS 1 BP 141 EP 153 DI 10.2138/am.2013.4089 PG 13 WC Geochemistry & Geophysics; Mineralogy SC Geochemistry & Geophysics; Mineralogy GA 065KZ UT WOS:000313148500014 ER PT J AU Jeitner, TM Battaile, K Cooper, AJL AF Jeitner, Thomas M. Battaile, Kevin Cooper, Arthur J. L. TI gamma-Glutamylamines and neurodegenerative diseases SO AMINO ACIDS LA English DT Review DE gamma-Glutamylamine; Transglutaminase; Neurodegeneration; gamma-Glutamylamine cyclotransferase ID CATALYZED CROSS-LINKING; MOUSE EPIDERMAL-CELLS; TISSUE TRANSGLUTAMINASE; PARKINSONS-DISEASE; HUNTINGTONS-DISEASE; ALPHA-SYNUCLEIN; SUBSTANTIA-NIGRA; ALZHEIMERS-DISEASE; POLYGLUTAMINE DOMAINS; NEURONAL DEATH AB Transglutaminases catalyze the formation of gamma-glutamylamines utilizing glutamyl residues and amine-bearing compounds such as lysyl residues and polyamines. These gamma-glutamylamines can be released from proteins by proteases in an intact form. The free gamma-glutamylamines can be catabolized to 5-oxo-L-proline and the free amine by gamma-glutamylamine cyclotransferase. Free gamma-glutamylamines, however, accumulate in the CSF and affected areas of Huntington Disease brain. This observation suggests transglutaminase-derived gamma-glutamylamines may play a more significant role in neurodegeneration than previously thought. The following monograph reviews the metabolism of gamma-glutamylamines and examines the possibility that these species contribute to neurodegeneration. C1 [Jeitner, Thomas M.] Winthrop Univ Hosp, Biomed Res Core, Mineola, NY 11501 USA. [Battaile, Kevin] Argonne Natl Lab, IMCA CAT, Adv Photon Source, Argonne, IL 60439 USA. [Cooper, Arthur J. L.] New York Med Coll, Dept Biochem & Mol Biol, Valhalla, NY 10595 USA. RP Jeitner, TM (reprint author), Winthrop Univ Hosp, Biomed Res Core, 222 Stn Plaza N, Mineola, NY 11501 USA. EM tjeitner@winthrop.org; battaile@anl.gov; arthur_cooper@nymc.edu RI Cooper, Arthur/H-5171-2016; OI Battaile, Kevin/0000-0003-0833-3259 FU Theresa Santmann-Patnode award; Burke Program [2P01 AG14930] FX The authors would like to acknowledge the pertinent comments of Dr. J. Keillor with regard to the reversibility of the reactions catalyzed by transglutaminases. Support for the writing of this review came from the Theresa Santmann-Patnode award to TMJ and from Burke Program Project-2P01 AG14930 to AJLC. We are indebted to Jack Folk for his willingness to synthesize for us several of the gamma-glutamylpolyamines mentioned in the text. Without his help our studies on the levels of gamma-glutamylpolyamines in CSF would not have been possible. Jack was always courteous and helpful. With his passing, the field has lost a superb chemist and biochemist. NR 105 TC 9 Z9 9 U1 0 U2 14 PU SPRINGER WIEN PI WIEN PA SACHSENPLATZ 4-6, PO BOX 89, A-1201 WIEN, AUSTRIA SN 0939-4451 J9 AMINO ACIDS JI Amino Acids PD JAN PY 2013 VL 44 IS 1 BP 129 EP 142 DI 10.1007/s00726-011-1209-3 PG 14 WC Biochemistry & Molecular Biology SC Biochemistry & Molecular Biology GA 063QW UT WOS:000313015900015 PM 22407484 ER PT J AU Lian, YJ Huber, T Hesp, KD Bergman, RG Ellman, JA AF Lian, Yajing Huber, Tatjana Hesp, Kevin D. Bergman, Robert G. Ellman, Jonathan A. TI Rhodium(III)-Catalyzed Alkenyl C-H Bond Functionalization: Convergent Synthesis of Furans and Pyrroles SO ANGEWANDTE CHEMIE-INTERNATIONAL EDITION LA English DT Article DE annulation; C-H activation; heterocycles; rhodium; synthetic methods ID SUBSTITUTED FURANS; INTERNAL ALKYNES; POLYSUBSTITUTED FURANS; CATALYZED ANNULATION; ACTIVATION; CLEAVAGE; ALDEHYDES; ARYL; BENZAMIDES; DERIVATIVES C1 [Lian, Yajing; Huber, Tatjana; Hesp, Kevin D.; Ellman, Jonathan A.] Yale Univ, Dept Chem, New Haven, CT 06520 USA. [Bergman, Robert G.] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Bergman, Robert G.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Ellman, JA (reprint author), Yale Univ, Dept Chem, 225 Prospect St, New Haven, CT 06520 USA. EM jonathan.ellman@yale.edu RI Lian, Yajing/F-9157-2011; Ellman, Jonathan/C-7732-2013 FU NIH [GM069559]; Office of Energy Research, Office of Basic Energy Sciences, Chemical Sciences Division, U.S. Department of Energy [DE-AC02-05CH11231]; National Sciences and Engineering Research Council of Canada (NSERC) FX This work was supported by the NIH Grant GM069559 (to J.A.E.). R. G. B. acknowledges funding from The Director, Office of Energy Research, Office of Basic Energy Sciences, Chemical Sciences Division, U.S. Department of Energy, under Contract DE-AC02-05CH11231. K. D. H. is grateful to the National Sciences and Engineering Research Council of Canada (NSERC) for a postdoctoral fellowship. NR 80 TC 95 Z9 95 U1 0 U2 125 PU WILEY-V C H VERLAG GMBH PI WEINHEIM PA BOSCHSTRASSE 12, D-69469 WEINHEIM, GERMANY SN 1433-7851 J9 ANGEW CHEM INT EDIT JI Angew. Chem.-Int. Edit. PY 2013 VL 52 IS 2 BP 629 EP 633 DI 10.1002/anie.201207995 PG 5 WC Chemistry, Multidisciplinary SC Chemistry GA 062SQ UT WOS:000312942900022 PM 23172703 ER PT J AU Kamali, S Wang, HX Mitra, D Ogata, H Lubitz, W Manor, BC Rauchfuss, TB Byrne, D Bonnefoy, V Jenney, FE Adams, MWW Yoda, Y Alp, E Zhao, JY Cramer, SP AF Kamali, Saeed Wang, Hongxin Mitra, Devrani Ogata, Hideaki Lubitz, Wolfgang Manor, Brian C. Rauchfuss, Thomas B. Byrne, Deborah Bonnefoy, Violaine Jenney, Francis E., Jr. Adams, Michael W. W. Yoda, Yoshitaka Alp, Ercan Zhao, Jiyong Cramer, Stephen P. TI Observation of the Fe-CN and Fe-CO Vibrations in the Active Site of [NiFe] Hydrogenase by Nuclear Resonance Vibrational Spectroscopy SO ANGEWANDTE CHEMIE-INTERNATIONAL EDITION LA English DT Article DE FeS clusters; hydrogenases; NiFe acvite site; spectroscopic methods; vibrational spectroscopy ID DESULFOVIBRIO-VULGARIS MIYAZAKI; NORMAL-MODE ANALYSIS; DYNAMICS; RAMAN; IRON; ACTIVATION; MYOGLOBIN; CLUSTER; FTIR; NRVS C1 [Kamali, Saeed; Wang, Hongxin; Mitra, Devrani; Cramer, Stephen P.] Univ Calif Davis, Dept Chem, Davis, CA 95616 USA. [Wang, Hongxin; Cramer, Stephen P.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA 94720 USA. [Ogata, Hideaki; Lubitz, Wolfgang] Max Planck Inst Chem Energiekonvers, D-45470 Mulheim, Germany. [Manor, Brian C.; Rauchfuss, Thomas B.] Univ Illinois Champaign Urbana, Dept Chem, Urbana, IL 61801 USA. [Byrne, Deborah] Aix Marseille Univ, Inst Microbiol Mediterranee, F-13009 Marseille, France. [Bonnefoy, Violaine] CNRS, Chim Bacterienne Lab, IMM, F-13277 Marseille 20, France. [Jenney, Francis E., Jr.] Philadelphia Coll Osteopath Med, Suwanee, GA 30024 USA. [Adams, Michael W. W.] Univ Georgia, Dept Biochem & Mol Biol, Athens, GA 30602 USA. [Yoda, Yoshitaka] JASRI, Sayo, Hyogo 6795198, Japan. [Alp, Ercan; Zhao, Jiyong] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. RP Lubitz, W (reprint author), Max Planck Inst Chem Energiekonvers, D-45470 Mulheim, Germany. EM Wolfgang.Lubitz@cec.mpg.de; spjcramer@ucdavis.edu RI Ogata, Hideaki/J-4975-2013 FU National Institutes of Health [GM-65440, GM-061153]; DOE Office of Biological and Environmental Research; BMBF [03SF0355C]; EU/Energy Network project SOLAR-H2 [212508]; Max Planck Society; DOE Office of Basic Energy Sciences FX This work was funded by the National Institutes of Health GM-65440 (S.P.C.) and GM-061153 (T.B.R.), the DOE Office of Biological and Environmental Research (S.P.C.), BMBF (03SF0355C), EU/Energy Network project SOLAR-H2 (FP7 contract 212508), and Max Planck Society (W.L. and H.O.). A.P.S. is supported by the DOE Office of Basic Energy Sciences. The proposal number in SPring-8 is 2010B0032-2012 A0032. NR 40 TC 22 Z9 23 U1 1 U2 75 PU WILEY-V C H VERLAG GMBH PI WEINHEIM PA BOSCHSTRASSE 12, D-69469 WEINHEIM, GERMANY SN 1433-7851 J9 ANGEW CHEM INT EDIT JI Angew. Chem.-Int. Edit. PY 2013 VL 52 IS 2 BP 724 EP 728 DI 10.1002/anie.201204616 PG 5 WC Chemistry, Multidisciplinary SC Chemistry GA 062SQ UT WOS:000312942900042 PM 23136119 ER PT J AU Beller, HR Han, RY Karaoz, U Lim, H Brodie, EL AF Beller, Harry R. Han, Ruyang Karaoz, Ulas Lim, HsiaoChien Brodie, Eoin L. TI Genomic and Physiological Characterization of the Chromate-Reducing, Aquifer-Derived Firmicute Pelosinus sp Strain HCF1 SO APPLIED AND ENVIRONMENTAL MICROBIOLOGY LA English DT Article ID SP NOV.; BIOCHEMICAL-CHARACTERIZATION; PARACOCCUS-DENITRIFICANS; SPOROTALEA-PROPIONICA; PSEUDOMONAS-PUTIDA; CHROMIUM COMPOUNDS; METHYLMALONYL-COA; ESCHERICHIA-COLI; REDUCTASE; IRON AB Pelosinus spp. are fermentative firmicutes that were recently reported to be prominent members of microbial communities at contaminated subsurface sites in multiple locations. Here we report metabolic characteristics and their putative genetic basis in Pelosinus sp. strain HCF1, an isolate that predominated anaerobic, Cr(VI)-reducing columns constructed with aquifer sediment. Strain HCF1 ferments lactate to propionate and acetate (the methylmalonyl-coenzyme A [CoA] pathway was identified in the genome), and its genome encodes two [NiFe]- and four [FeFe]-hydrogenases for H-2 cycling. The reduction of Cr(VI) and Fe(III) may be catalyzed by a flavoprotein with 42 to 51% sequence identity to both ChrR and FerB. This bacterium has unexpected capabilities and gene content associated with reduction of nitrogen oxides, including dissimilatory reduction of nitrate to ammonium (two copies of NrfH and NrfA were identified along with NarGHI) and a nitric oxide reductase (NorCB). In this strain, either H2 or lactate can act as a sole electron donor for nitrate, Cr(VI), and Fe(III) reduction. Transcriptional studies demonstrated differential expression of hydrogenases and nitrate and nitrite reductases. Overall, the unexpected metabolic capabilities and gene content reported here broaden our perspective on what biogeochemical and ecological roles this species might play as a prominent member of microbial communities in subsurface environments. C1 [Beller, Harry R.; Han, Ruyang; Karaoz, Ulas; Lim, HsiaoChien; Brodie, Eoin L.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, Berkeley, CA 94720 USA. RP Beller, HR (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, Berkeley, CA 94720 USA. EM HRBeller@lbl.gov RI Beller, Harry/H-6973-2014; Brodie, Eoin/A-7853-2008; Karaoz, Ulas/J-7093-2014 OI Brodie, Eoin/0000-0002-8453-8435; FU U.S. Department of Energy, Office of Science, Office of Biological and Environmental Research [DE-AC02-05CH11231] FX This work was supported as part of the Subsurface Biogeochemical Research Scientific Focus Area funded by the U.S. Department of Energy, Office of Science, Office of Biological and Environmental Research, under award number DE-AC02-05CH11231. NR 47 TC 15 Z9 16 U1 0 U2 48 PU AMER SOC MICROBIOLOGY PI WASHINGTON PA 1752 N ST NW, WASHINGTON, DC 20036-2904 USA SN 0099-2240 J9 APPL ENVIRON MICROB JI Appl. Environ. Microbiol. PD JAN PY 2013 VL 79 IS 1 BP 63 EP 73 DI 10.1128/AEM.02496-12 PG 11 WC Biotechnology & Applied Microbiology; Microbiology SC Biotechnology & Applied Microbiology; Microbiology GA 062PK UT WOS:000312931600008 PM 23064329 ER PT J AU Hunt, DE Lin, YJ Church, MJ Karl, DM Tringe, SG Izzo, LK Johnson, ZI AF Hunt, Dana E. Lin, Yajuan Church, Matthew J. Karl, David M. Tringe, Susannah G. Izzo, Lisa K. Johnson, Zackary I. TI Relationship between Abundance and Specific Activity of Bacterioplankton in Open Ocean Surface Waters SO APPLIED AND ENVIRONMENTAL MICROBIOLOGY LA English DT Article ID MICROBIAL COMMUNITY STRUCTURE; RIBOSOMAL-RNA CONTENT; PROCHLOROCOCCUS ECOTYPES; MARINE-BACTERIA; SEQUENCE DATA; REAL-TIME; GROWTH; DIVERSITY; GENOMICS; PACIFIC AB Marine microbial communities are complex and dynamic, and their ecology impacts biogeochemical cycles in pelagic ecosystems. Yet, little is known about the relative activities of different microbial populations within genetically diverse communities. We used rRNA as a proxy for activity to quantify the relative specific activities (rRNA/ribosomal DNA [rDNA or rRNA genes]) of the eubacterial populations and to identify locations or clades for which there are uncouplings between specific activity and abundance. After analyzing 1.6 million sequences from 16S rDNA and rRNA (cDNA) libraries from two euphotic depths from a representative site in the Pacific Ocean, we show that although there is an overall positive relationship between the abundances (rDNAs) and activities (rRNAs) among populations of the bacterial community, for some populations these measures are uncoupled. Different ecological strategies are exemplified by the two numerically dominant clades at this site: the cyanobacterium Prochlorococcus is abundant but disproportionately more active, while the heterotrophic SAR11 is abundant but less active. Other rare populations, such as Alteromonas, have high specific activities in spite of their low abundances, suggesting intense population regulation. More detailed analyses using a complementary quantitative PCR (qPCR)-based approach of measuring relative specific activity for Prochlorococcus populations in the Pacific and Atlantic Oceans also show that specific activity, but not abundance, reflects the key drivers of light and nutrients in this system; our results also suggest substantial top-down regulation (e.g., grazing, viruses, or organismal interactions) or transport (e.g., mixing, immigration, or emigration) of these populations. Thus, we show here that abundance and specific activity can be uncoupled in open ocean systems and that describing both is critical to characterizing microbial communities and predicting marine ecosystem functioning and responses to change. C1 [Hunt, Dana E.; Lin, Yajuan; Izzo, Lisa K.; Johnson, Zackary I.] Duke Univ, Marine Lab, Nicholas Sch Environm, Beaufort, NC 28516 USA. [Church, Matthew J.; Karl, David M.] Univ Hawaii, Dept Oceanog, Honolulu, HI 96822 USA. [Tringe, Susannah G.] Joint Genome Inst, Dept Energy DOE, Walnut Creek, CA USA. RP Johnson, ZI (reprint author), Duke Univ, Marine Lab, Nicholas Sch Environm, Beaufort, NC 28516 USA. EM zij@duke.edu RI Hunt, Dana/A-2051-2012; Johnson, Zackary/E-4601-2011; OI Johnson, Zackary/0000-0003-0793-8512; Hunt, Dana/0000-0002-8801-9624 FU U.S. National Science Foundation [OCE10-31064]; Gordon and Betty Moore Foundation; Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231] FX This work was funded in part by funds from the U.S. National Science Foundation (number OCE10-31064 to Z.I.J.) and the Gordon and Betty Moore Foundation (to D.M.K.). Sequencing was conducted in part by the U.S. Department of Energy Joint Genome Institute and was supported by the Office of Science of the U.S. Department of Energy under contract no. DE-AC02-05CH11231. NR 46 TC 44 Z9 44 U1 2 U2 92 PU AMER SOC MICROBIOLOGY PI WASHINGTON PA 1752 N ST NW, WASHINGTON, DC 20036-2904 USA SN 0099-2240 J9 APPL ENVIRON MICROB JI Appl. Environ. Microbiol. PD JAN PY 2013 VL 79 IS 1 BP 177 EP 184 DI 10.1128/AEM.02155-12 PG 8 WC Biotechnology & Applied Microbiology; Microbiology SC Biotechnology & Applied Microbiology; Microbiology GA 062PK UT WOS:000312931600020 PM 23087033 ER PT J AU Carter, L Lindsey, LA Grim, CJ Sathyamoorthy, V Jarvis, KG Gopinath, G Lee, C Sadowski, JA Trach, L Pava-Ripoll, M McCardell, BA Tall, BD Hu, L AF Carter, L. Lindsey, L. A. Grim, C. J. Sathyamoorthy, V. Jarvis, K. G. Gopinath, G. Lee, C. Sadowski, J. A. Trach, L. Pava-Ripoll, M. McCardell, B. A. Tall, B. D. Hu, L. TI Multiplex PCR Assay Targeting a Diguanylate Cyclase-Encoding Gene, cgcA, To Differentiate Species within the Genus Cronobacter SO APPLIED AND ENVIRONMENTAL MICROBIOLOGY LA English DT Article ID ENTEROBACTER-SAKAZAKII; SEQUENCE AB In a comparison to the widely used Cronobacter rpoB PCR assay, a highly specific multiplexed PCR assay based on cgcA, a diguanylate cyclase gene, that identified all of the targeted six species among 305 Cronobacter isolates was designed. This assay will be a valuable tool for identifying suspected Cronobacter isolates from food-borne investigations. C1 [Carter, L.; Lindsey, L. A.; Grim, C. J.; Sathyamoorthy, V.; Jarvis, K. G.; Gopinath, G.; Lee, C.; Sadowski, J. A.; Trach, L.; McCardell, B. A.; Tall, B. D.; Hu, L.] US FDA, CFSAN, Laurel, MD USA. [Grim, C. J.; Hu, L.] Oak Ridge Inst Sci & Educ, Oak Ridge, TN USA. [Pava-Ripoll, M.] US FDA, CFSAN, College Pk, MD USA. RP Hu, L (reprint author), US FDA, CFSAN, Laurel, MD USA. EM lan16686@yahoo.com OI Tall, Ben/0000-0003-0399-3629 FU National Association for Equal Opportunity in Higher Education internship program fellowship, Washington, DC; oint Institute of Food Safety and Applied Nutrition student internship program, University of Maryland, College Park, MD FX L. A. Lindsey was a recipient of a 2011 National Association for Equal Opportunity in Higher Education internship program fellowship, Washington, DC. C. Lee, L. Trach, and J. A. Sadowski were supported by the Joint Institute of Food Safety and Applied Nutrition student internship program, University of Maryland, College Park, MD. NR 19 TC 16 Z9 17 U1 0 U2 10 PU AMER SOC MICROBIOLOGY PI WASHINGTON PA 1752 N ST NW, WASHINGTON, DC 20036-2904 USA SN 0099-2240 J9 APPL ENVIRON MICROB JI Appl. Environ. Microbiol. PD JAN PY 2013 VL 79 IS 2 BP 734 EP 737 DI 10.1128/AEM.02898-12 PG 4 WC Biotechnology & Applied Microbiology; Microbiology SC Biotechnology & Applied Microbiology; Microbiology GA 062SI UT WOS:000312941800039 PM 23144142 ER PT J AU Phuoc, TX Chen, RH AF Phuoc, Tran X. Chen, Ruey-Hung TI Spontaneous ignition of low-concentration nano-sized Al-water slurry SO APPLIED ENERGY LA English DT Article DE Spontaneous ignition; Al-water slurry ID COMBUSTION; ALUMINUM; NANOFLUIDS; HYDROGEN; ENERGY AB Spontaneous ignition of a nano-sized aluminum (Al) particles-water slurry using a hot plate was investigated. The aluminum weight fractions were 17% and 27%. The hot plate temperatures ranged from 303 to 343 K. For all experimental conditions used, ignition was observed to occur at about 321 K and it was followed by a rapid temperature increase to above the boiling temperature of the water. Although the thermal runaway condition did not occur until the slurry reached a temperature of 321 K. it was able to react at a temperature as low as 303 K and develops sufficient heat for the slurry to reach the ignition condition. The ignition kinetic data were determined showing that E/R = 28619.66 (K) and k = 1.2644 x 10(37) K/s for the slurry containing 17% aluminum and, the value of k was about 2.398 x 10m(37) K/s for those having 27% aluminum by weight. Published by Elsevier Ltd. C1 [Phuoc, Tran X.] US DOE, Natl Energy Technol Lab, Pittsburgh, PA 15261 USA. [Chen, Ruey-Hung] Univ Cent Florida, Dept Mech Mat & Aerosp Engn, Orlando, FL 32816 USA. RP Phuoc, TX (reprint author), US DOE, Natl Energy Technol Lab, POB 10940,MS 84-340, Pittsburgh, PA 15261 USA. EM tran@netl.doe.gov; chenrh@mail.ucf.edu FU agency of the United States Government FX "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 15 TC 2 Z9 2 U1 1 U2 13 PU ELSEVIER SCI LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, OXON, ENGLAND SN 0306-2619 J9 APPL ENERG JI Appl. Energy PD JAN PY 2013 VL 101 SI SI BP 567 EP 571 DI 10.1016/j.apenergy.2012.06.033 PG 5 WC Energy & Fuels; Engineering, Chemical SC Energy & Fuels; Engineering GA 058ER UT WOS:000312617400063 ER PT J AU Pratt, JW Klebanoff, LE Munoz-Ramos, K Akhil, AA Curgus, DB Schenkman, BL AF Pratt, Joseph W. Klebanoff, Leonard E. Munoz-Ramos, Karina Akhil, Abbas A. Curgus, Dita B. Schenkman, Benjamin L. TI Proton exchange membrane fuel cells for electrical power generation on-board commercial airplanes SO APPLIED ENERGY LA English DT Article DE PEM fuel cell; More electric airplane; Heat recovery; System design; Airplane performance ID HYDROGEN STORAGE AB Deployed on a commercial airplane, proton exchange membrane (PEM) fuel cells may offer emissions reductions, thermal efficiency gains, and enable locating the power near the point of use. This work seeks to understand whether on-board fuel cell systems are technically feasible, and, if so, if they could offer a performance advantage for the airplane when using today's off-the-shelf technology. We also examine the effects of the fuel cell system on airplane performance with (I) different electrical loads, (2) different locations on the airplane, and (3) expected advances in fuel cell and hydrogen storage technologies. Through hardware analysis and thermodynamic simulation, we found that an additional fuel cell system on a commercial airplane is technically feasible using current technology. Although applied to a Boeing 787-type airplane, the method presented is applicable to other airframes as well. Recovery and on-board use of the heat and water that is generated by the fuel cell is an important method to increase the benefit of such a system. The best performance is achieved when the fuel cell is coupled to a load that utilizes the full output of the fuel cell for the entire flight. The effects of location are small and location may be better determined by other considerations such as safety and modularity. Although the PEM fuel cell generates power more efficiently than the gas turbine generators currently used, when considering the effect of the fuel cell system on the airplane's overall performance we found that an overall performance penalty (i.e., the airplane will burn more jet fuel) would result if using current technology for the fuel cell and hydrogen storage. However, we found that with expected developments in PEM fuel cell and hydrogen storage technology, PEM fuel cell systems can provide an overall benefit to airplane performance. (C) 2012 Elsevier Ltd. All rights reserved. C1 [Pratt, Joseph W.; Klebanoff, Leonard E.; Curgus, Dita B.] Sandia Natl Labs Calif, Livermore, CA 94551 USA. [Munoz-Ramos, Karina; Akhil, Abbas A.; Schenkman, Benjamin L.] Sandia Natl Labs New Mexico, Albuquerque, NM 87185 USA. RP Pratt, JW (reprint author), POB 969,MS-9409, Livermore, CA 94551 USA. EM jwpratt@sandia.gov FU Department of Energy (DOE) - Energy Efficiency & Renewable Energy (EERE) - Fuel Cell Technologies (FCT) - Market Transformation group; US Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX Special thanks to the Boeing Commercial Airplanes staff: Joe Breit, Andy Bayliss, Trevor Laib, Farhad Nozari, and Casey Roberts for their assistance with understanding airplane configuration, electrical systems, and performance. This work was sponsored by Department of Energy (DOE) - Energy Efficiency & Renewable Energy (EERE) - Fuel Cell Technologies (FCT) - Market Transformation group - thanks to Pete Devlin for his support.; Sandia National Laboratories is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the US Department of Energy's National Nuclear Security Administration under Contract DE-AC04-94AL85000. NR 39 TC 21 Z9 21 U1 4 U2 32 PU ELSEVIER SCI LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, OXON, ENGLAND SN 0306-2619 J9 APPL ENERG JI Appl. Energy PD JAN PY 2013 VL 101 SI SI BP 776 EP 796 DI 10.1016/j.apenergy.2012.08.003 PG 21 WC Energy & Fuels; Engineering, Chemical SC Energy & Fuels; Engineering GA 058ER UT WOS:000312617400084 ER PT J AU Dunner, R Hasselfield, M Marriage, TA Sievers, J Acquaviva, V Addison, GE Ade, PAR Aguirre, P Amiri, M Appel, JW Barrientos, LF Battistelli, ES Bond, JR Brown, B Burger, B Calabrese, E Chervenak, J Das, S Devlin, MJ Dicker, SR Doriese, WB Dunkley, J Essinger-Hileman, T Fisher, RP Gralla, MB Fowler, JW Hajian, A Halpern, M Hernandez-Monteagudo, C Hilton, GC Hilton, M Hincks, AD Hlozek, R Huffenberger, KM Hughes, DH Hughes, JP Infante, L Irwin, KD Juin, JB Kaul, M Klein, J Kosowsky, A Lau, JM Limon, M Lin, YT Louis, T Lupton, RH Marsden, D Martocci, K Mauskopf, P Menanteau, F Moodley, K Moseley, H Netterfield, CB Niemack, MD Nolta, MR Page, LA Parker, L Partridge, B Quintana, H Reid, B Sehgal, N Sherwin, BD Spergel, DN Staggs, ST Swetz, DS Switzer, ER Thornton, R Trac, H Tucker, C Warne, R Wilson, G Wollack, E Zhao, Y AF Duenner, Rolando Hasselfield, Matthew Marriage, Tobias A. Sievers, Jon Acquaviva, Viviana Addison, Graeme E. Ade, Peter A. R. Aguirre, Paula Amiri, Mandana Appel, John William Felipe Barrientos, L. Battistelli, Elia S. Bond, J. Richard Brown, Ben Burger, Bryce Calabrese, Erminia Chervenak, Jay Das, Sudeep Devlin, Mark J. Dicker, Simon R. Doriese, W. Bertrand Dunkley, Joanna Essinger-Hileman, Thomas Fisher, Ryan P. Gralla, Megan B. Fowler, Joseph W. Hajian, Amir Halpern, Mark Hernandez-Monteagudo, Carlos Hilton, Gene C. Hilton, Matt Hincks, Adam D. Hlozek, Renee Huffenberger, Kevin M. Hughes, David H. Hughes, John P. Infante, Leopoldo Irwin, Kent D. Baptiste Juin, Jean Kaul, Madhuri Klein, Jeff Kosowsky, Arthur Lau, Judy M. Limon, Michele Lin, Yen-Ting Louis, Thibaut Lupton, Robert H. Marsden, Danica Martocci, Krista Mauskopf, Phil Menanteau, Felipe Moodley, Kavilan Moseley, Harvey Netterfield, Calvin B. Niemack, Michael D. Nolta, Michael R. Page, Lyman A. Parker, Lucas Partridge, Bruce Quintana, Hernan Reid, Beth Sehgal, Neelima Sherwin, Blake D. Spergel, David N. Staggs, Suzanne T. Swetz, Daniel S. Switzer, Eric R. Thornton, Robert Trac, Hy Tucker, Carole Warne, Ryan Wilson, Grant Wollack, Ed Zhao, Yue TI THE ATACAMA COSMOLOGY TELESCOPE: DATA CHARACTERIZATION AND MAPMAKING SO ASTROPHYSICAL JOURNAL LA English DT Article DE cosmic background radiation; cosmology: observations; instrumentation: miscellaneous ID SOUTH-POLE TELESCOPE; BACKGROUND POWER SPECTRUM; PROBE WMAP OBSERVATIONS; 148 GHZ; GALAXY CLUSTERS; MICROWAVE; ANISOTROPY; ACT; PARAMETERS; ARRAY AB We present a description of the data reduction and mapmaking pipeline used for the 2008 observing season of the Atacama Cosmology Telescope (ACT). The data presented here at 148 GHz represent 12% of the 90 TB collected by ACT from 2007 to 2010. In 2008 we observed for 136 days, producing a total of 1423 hr of data (11 TB for the 148 GHz band only), with a daily average of 10.5 hr of observation. From these, 1085 hr were devoted to an 850 deg(2) stripe (11.2 hr by 9 degrees.1) centered on a declination of -52 degrees.7, while 175 hr were devoted to a 280 deg(2) stripe (4.5 hr by 4 degrees.8) centered at the celestial equator. The remaining 163 hr correspond to calibration runs. We discuss sources of statistical and systematic noise, calibration, telescope pointing, and data selection. For the 148 GHz band, out of 1260 survey hours and 1024 detectors in the array, 816 hr and 593 effective detectors remain after data selection, yielding a 38% survey efficiency. The total sensitivity in 2008, determined from the noise level between 5 Hz and 20 Hz in the time-ordered data stream (TOD), is 32 mu K root s in cosmic microwave background units. Atmospheric brightness fluctuations constitute the main contaminant in the data and dominate the detector noise covariance at low frequencies in the TOD. The maps were made by solving the least-squares problem using the Preconditioned Conjugate Gradient method, incorporating the details of the detector and noise correlations. Simulations, as well as cross-correlations with Wilkinson Microwave Anisotropy Probe sky maps on large angular scales, reveal that our maps are unbiased at multipoles l > 300. This paper accompanies the public release of the 148 GHz southern stripe maps from 2008. The techniques described here will be applied to future maps and data releases. C1 [Duenner, Rolando; Aguirre, Paula; Felipe Barrientos, L.; Infante, Leopoldo; Baptiste Juin, Jean; Lin, Yen-Ting; Quintana, Hernan] Pontificia Univ Catolica Chile, Fac Fis, Dept Astron & Astrofis, Santiago 22, Chile. [Hasselfield, Matthew; Amiri, Mandana; Battistelli, Elia S.; Burger, Bryce; Halpern, Mark] Univ British Columbia, Dept Phys & Astron, Vancouver, BC V6T 1Z4, Canada. [Marriage, Tobias A.; Acquaviva, Viviana; Das, Sudeep; Dunkley, Joanna; Hajian, Amir; Hlozek, Renee; Lin, Yen-Ting; Lupton, Robert H.; Sehgal, Neelima; Spergel, David N.; Trac, Hy] Princeton Univ, Dept Astrophys Sci, Princeton, NJ 08544 USA. [Marriage, Tobias A.; Gralla, Megan B.] Johns Hopkins Univ, Dept Phys & Astron, Baltimore, MD 21218 USA. [Sievers, Jon; Appel, John William; Das, Sudeep; Dunkley, Joanna; Essinger-Hileman, Thomas; Fisher, Ryan P.; Fowler, Joseph W.; Hajian, Amir; Hincks, Adam D.; Lau, Judy M.; Limon, Michele; Martocci, Krista; Niemack, Michael D.; Page, Lyman A.; Parker, Lucas; Reid, Beth; Sherwin, Blake D.; Staggs, Suzanne T.; Switzer, Eric R.; Zhao, Yue] Princeton Univ, Joseph Henry Labs Phys, Princeton, NJ 08544 USA. [Sievers, Jon; Bond, J. Richard; Hincks, Adam D.; Nolta, Michael R.; Switzer, Eric R.] Univ Toronto, Canadian Inst Theoret Astrophys, Toronto, ON M5S 3H8, Canada. [Acquaviva, Viviana; Hughes, John P.; Menanteau, Felipe] Rutgers State Univ, Dept Phys & Astron, Piscataway, NJ 08854 USA. [Addison, Graeme E.; Calabrese, Erminia; Dunkley, Joanna; Hlozek, Renee; Louis, Thibaut] Univ Oxford, Dept Astrophys, Oxford OX1 3RH, England. [Ade, Peter A. R.; Mauskopf, Phil; Tucker, Carole] Cardiff Univ, Sch Phys & Astron, Cardiff CF24 3AA, S Glam, Wales. [Battistelli, Elia S.] Univ Roma La Sapienza, Dept Phys, I-00185 Rome, Italy. [Brown, Ben; Kosowsky, Arthur] Univ Pittsburgh, Dept Phys & Astron, Pittsburgh, PA 15260 USA. [Chervenak, Jay; Moseley, Harvey; Wollack, Ed] NASA, Goddard Space Flight Ctr, Greenbelt, MD 20771 USA. [Das, Sudeep; Reid, Beth] Univ Calif Berkeley, Berkeley Ctr Cosmol Phys, LBL, Berkeley, CA 94720 USA. [Das, Sudeep; Reid, Beth] Univ Calif Berkeley, Dept Phys, Berkeley, CA 94720 USA. [Devlin, Mark J.; Dicker, Simon R.; Kaul, Madhuri; Klein, Jeff; Limon, Michele; Swetz, Daniel S.; Thornton, Robert] Univ Penn, Dept Phys & Astron, Philadelphia, PA 19104 USA. [Doriese, W. Bertrand; Fowler, Joseph W.; Hilton, Gene C.; Irwin, Kent D.; Niemack, Michael D.; Swetz, Daniel S.] NIST, Quantum Devices Grp, Boulder, CO 80305 USA. [Hajian, Amir; Netterfield, Calvin B.] Univ Toronto, Dept Phys, Toronto, ON M5S 1A7, Canada. [Hernandez-Monteagudo, Carlos] Max Planck Inst Astrophys, D-85741 Garching, Germany. [Hilton, Matt; Moodley, Kavilan; Warne, Ryan] Univ KwaZulu Natal, Sch Math Sci, Astrophys & Cosmol Res Unit, ZA-4041 Durban, South Africa. [Hilton, Matt] Univ Nottingham, Sch Phys & Astron, Ctr Astron & Particle Theory, Nottingham NG7 2RD, England. [Huffenberger, Kevin M.] Univ Miami, Dept Phys, Coral Gables, FL 33124 USA. [Hughes, David H.] INAOE, Puebla, Mexico. [Limon, Michele] Columbia Univ, Columbia Astrophys Lab, New York, NY 10027 USA. [Lin, Yen-Ting] Univ Tokyo, Inst Phys & Math Universe, Kashiwa, Chiba 2778568, Japan. [Lin, Yen-Ting] Acad Sinica, Inst Astron & Astrophys, Taipei 115, Taiwan. [Marsden, Danica] Univ Calif Santa Barbara, Dept Phys, Santa Barbara, CA 93106 USA. [Martocci, Krista] Kavli Inst Cosmol Phys, Lab Astrophys & Space Res, Chicago, IL 60637 USA. [Moodley, Kavilan] Ctr High Performance Comp, Cape Town, South Africa. [Partridge, Bruce] Haverford Coll, Dept Phys & Astron, Haverford, PA 19041 USA. [Thornton, Robert] W Chester Univ Penn, Dept Phys, W Chester, PA 19383 USA. [Trac, Hy] Harvard Univ, Harvard Smithsonian Ctr Astrophys, Cambridge, MA 02138 USA. [Wilson, Grant] Univ Massachusetts, Dept Astron, Amherst, MA 01003 USA. RP Dunner, R (reprint author), Pontificia Univ Catolica Chile, Fac Fis, Dept Astron & Astrofis, Casilla 306, Santiago 22, Chile. RI Klein, Jeffrey/E-3295-2013; Spergel, David/A-4410-2011; Hilton, Matthew James/N-5860-2013; Trac, Hy/N-8838-2014; Wollack, Edward/D-4467-2012; OI Trac, Hy/0000-0001-6778-3861; Wollack, Edward/0000-0002-7567-4451; Limon, Michele/0000-0002-5900-2698; Huffenberger, Kevin/0000-0001-7109-0099; Menanteau, Felipe/0000-0002-1372-2534; Sievers, Jonathan/0000-0001-6903-5074; Tucker, Carole/0000-0002-1851-3918 FU U.S. National Science Foundation [AST-0408698, AST-0965625, PHY-0855887, PHY-1214379]; Princeton University; University of Pennsylvania; Canada Foundation for Innovation (CFI) award; Comision Nacional de Investigacion Cientifica y Tecnologica de Chile (CONICYT); CFI under Compute Canada; Government of Ontario; Ontario Research Fund-Research Excellence; University of Toronto; CONICYT scholarship; MECESUP; Fundacion Andes; Centro de Astrofisica y Tecnologias Afines CATA del Proyecto Financiamiento Basal [PFB06]; Centro de Astrofisica FONDAP [15010003]; U.S. Department of Energy [DE-AC3-76SF00515]; NSF [1102762]; NSF Physics Frontier Center [PHY-0114422]; Rhodes Trust; Christ Church; [FONDECYT-11100147]; [NSF-AST-0807790] FX This work was supported by the U.S. National Science Foundation through awards AST-0408698 and AST-0965625 for the ACT project, and PHY-0855887 and PHY-1214379. Funding was also provided by Princeton University, the University of Pennsylvania, and a Canada Foundation for Innovation (CFI) award to UBC. ACT operates in the Parque Astronomico Atacama in northern Chile under the auspices of the Comision Nacional de Investigacion Cientifica y Tecnologica de Chile (CONICYT). Computations were performed on the GPC supercomputer at the SciNet HPC Consortium. SciNet is funded by the CFI under the auspices of Compute Canada, the Government of Ontario, the Ontario Research Fund-Research Excellence; and the University of Toronto. We specially thank Astro-Norte, Masao Uehara, Felipe Rojas, Patricio Gallardo, Omelan Strysak, Bill Page, Katerina Visnjic, Ben Schmidt, David Faber, and Benjamin Walter. R.D. received additional support from a CONICYT scholarship, from MECESUP, from Fundacion Andes, from FONDECYT-11100147, from Centro de Astrofisica y Tecnologias Afines CATA del Proyecto Financiamiento Basal PFB06, and from Centro de Astrofisica FONDAP 15010003. N.S. is supported by the U.S. Department of Energy contract to SLAC no. DE-AC3-76SF00515 and by the NSF under Award No. 1102762. E.R.S. acknowledges support by NSF Physics Frontier Center grant PHY-0114422 to the Kavli Institute of Cosmological Physics. A.K. has been supported by NSF-AST-0807790 for work on ACT. R.H. acknowledges funding from the Rhodes Trust and Christ Church. We are grateful for the assistance we received at various times from the ALMA, APEX, ASTE, CBI/QUIET, and NANTEN2 groups. NR 59 TC 31 Z9 31 U1 0 U2 11 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 0004-637X J9 ASTROPHYS J JI Astrophys. J. PD JAN 1 PY 2013 VL 762 IS 1 AR 10 DI 10.1088/0004-637X/762/1/10 PG 19 WC Astronomy & Astrophysics SC Astronomy & Astrophysics GA 063NY UT WOS:000313007900010 ER PT J AU Kampczyk, P Lilly, SJ de Ravel, L Le Fevre, O Bolzonella, M Carollo, CM Diener, C Knobel, C Kovac, K Maier, C Renzini, A Sargent, MT Vergani, D Abbas, U Bardelli, S Bongiorno, A Bordoloi, R Caputi, K Contini, T Coppa, G Cucciati, O de la Torre, S Franzetti, P Garilli, B Iovino, A Kneib, JP Koekemoer, AM Lamareille, F Le Borgne, JF Le Brun, V Leauthaud, A Mainieri, V Mignoli, M Pello, R Peng, Y Montero, EP Ricciardelli, E Scodeggio, M Silverman, JD Tanaka, M Tasca, L Tresse, L Zamorani, G Zucca, E Bottini, D Cappi, A Cassata, P Cimatti, A Fumana, M Guzzo, L Kartaltepe, J Marinoni, C McCracken, HJ Memeo, P Meneux, B Oesch, P Porciani, C Pozzetti, L Scaramella, R AF Kampczyk, P. Lilly, S. J. de Ravel, L. Le Fevre, O. Bolzonella, M. Carollo, C. M. Diener, C. Knobel, C. Kovac, K. Maier, C. Renzini, A. Sargent, M. T. Vergani, D. Abbas, U. Bardelli, S. Bongiorno, A. Bordoloi, R. Caputi, K. Contini, T. Coppa, G. Cucciati, O. de la Torre, S. Franzetti, P. Garilli, B. Iovino, A. Kneib, J. -P. Koekemoer, A. M. Lamareille, F. Le Borgne, J. -F. Le Brun, V. Leauthaud, A. Mainieri, V. Mignoli, M. Pello, R. Peng, Y. Montero, E. Perez Ricciardelli, E. Scodeggio, M. Silverman, J. D. Tanaka, M. Tasca, L. Tresse, L. Zamorani, G. Zucca, E. Bottini, D. Cappi, A. Cassata, P. Cimatti, A. Fumana, M. Guzzo, L. Kartaltepe, J. Marinoni, C. McCracken, H. J. Memeo, P. Meneux, B. Oesch, P. Porciani, C. Pozzetti, L. Scaramella, R. TI ENVIRONMENTAL EFFECTS IN THE INTERACTION AND MERGING OF GALAXIES IN zCOSMOS SO ASTROPHYSICAL JOURNAL LA English DT Article DE galaxies: evolution; galaxies: general; galaxies: interactions; galaxies: starburst ID STAR-FORMATION RATES; SIMILAR-TO 1; CNOC2 REDSHIFT SURVEY; MERGER RATE EVOLUTION; DIGITAL SKY SURVEY; COSMOS FIELD; CLOSE PAIRS; DISK GALAXIES; MORPHOLOGICAL TRANSFORMATION; FORMATION HISTORY AB We analyze the environments and galactic properties (morphologies and star formation histories) of a sample of 153 close kinematic pairs in the redshift range 0.2 < z < 1 identified in the zCOSMOS-bright 10 k spectroscopic sample of galaxies. Correcting for projection effects, the fraction of close kinematic pairs is three times higher in the top density quartile than in the lowest one. This translates to a three times higher merger rate because the merger timescales are shown, from mock catalogs based on the Millennium simulation, to be largely independent of environment once the same corrections for projection are applied. We then examine the morphologies and stellar populations of galaxies in the pairs, comparing them to control samples that are carefully matched in environment so as to remove as much of the well-known effects of environment on the properties of the parent population of galaxies as possible. Once the environment is properly taken into account in this way, we find that the early-late morphology mix is the same as for the parent population, but that the fraction of irregular galaxies is boosted by 50%-75%, with a disproportionate increase in the number of irregular-irregular pairs (factor of 4-8 times), due to the disturbance of disk galaxies. Future dry mergers, involving elliptical galaxies comprise less than 5% of all close kinematic pairs. In the closest pairs, there is a boost in the specific star formation rates of star-forming galaxies of a factor of 2-4, and there is also evidence for an increased incidence of post-starburst galaxies. Although significant for the galaxies involved, the "excess" star formation associated with pairs represents only about 5% of the integrated star formation activity in the parent sample. Although most pair galaxies are in dense environments, the effects of interaction appear to be largest in the lower density environments. By preferentially bringing more pairs into the sample in lower density environments, this could dilute the dependence of pair fraction on environment and may introduce other biases into the observational study of mergers, especially those based on morphological criteria. C1 [Kampczyk, P.; Lilly, S. J.; Carollo, C. M.; Diener, C.; Knobel, C.; Kovac, K.; Maier, C.; Bordoloi, R.; Peng, Y.; Oesch, P.; Porciani, C.] ETH, Inst Astron, CH-8093 Zurich, Switzerland. [de Ravel, L.; Le Fevre, O.; Cucciati, O.; Kneib, J. -P.; Le Brun, V.; Tresse, L.] Univ Provence, UMR CNRS 6110, Lab Astrophys Marseille, F-13376 Marseille 12, France. [de Ravel, L.] Univ Edinburgh, Royal Observ, Inst Astron, Edinburgh EH93 HJ, Midlothian, Scotland. [Bolzonella, M.; Vergani, D.; Bardelli, S.; Coppa, G.; Mignoli, M.; Zamorani, G.; Zucca, E.; Cappi, A.; Cimatti, A.; Pozzetti, L.] INAF Osservatorio Astron Bologna, I-40127 Bologna, Italy. [Maier, C.] Univ Vienna, Dept Astron, A-1180 Vienna, Austria. [Renzini, A.] INAF Osservatorio Astron Padova, I-35122 Padua, Italy. [Sargent, M. T.] Univ Paris Diderot, Lab AIM, Irfu Serv Astrophys, CEA,DSM,CNRS,CEA Saclay, F-91191 Gif Sur Yvette, France. [Abbas, U.; Leauthaud, A.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley Lab, Berkeley, CA 94720 USA. [Abbas, U.; Leauthaud, A.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley Ctr Cosmol Phys, Berkeley, CA 94720 USA. [Bongiorno, A.; Coppa, G.; Meneux, B.] Max Planck Inst Extraterr Phys, D-84571 Garching, Germany. [Caputi, K.] Univ Edinburgh, Royal Observ, SUPA, Inst Astron, Edinburgh EH9 3HJ, Midlothian, Scotland. [Contini, T.; Lamareille, F.; Le Borgne, J. -F.; Pello, R.; Montero, E. Perez] CNRS, Inst Rech Astrophys & Planetol, F-31400 Toulouse, France. [Contini, T.; Lamareille, F.; Le Borgne, J. -F.; Pello, R.; Montero, E. Perez] Univ Toulouse, IRAP, UPS OMP, F-31400 Toulouse, France. [Coppa, G.] Univ Bologna, Dipartmento Astron, I-40126 Bologna, Italy. [de la Torre, S.; Iovino, A.; Guzzo, L.] INAF Osservatorio Astron Brera, Milan, Italy. [Franzetti, P.; Garilli, B.; Tasca, L.; Bottini, D.; Fumana, M.; Memeo, P.] INAF IASF Milano, Milan, Italy. [Koekemoer, A. M.] Space Telescope Sci Inst, Baltimore, MD 21218 USA. [Mainieri, V.] European So Observ, D-85748 Garching, Germany. [Montero, E. Perez; Scodeggio, M.] CSIC, Inst Astrofis Andalucia, E-18080 Granada, Spain. [Ricciardelli, E.] Univ Padua, Dipartimento Astron, I-35122 Padua, Italy. [Silverman, J. D.; Tanaka, M.] Univ Tokyo, IPMU, Kashiwa, Chiba 2778568, Japan. [Cassata, P.] Univ Massachusetts, Dept Astron, Amherst, MA 01003 USA. [Kartaltepe, J.] Natl Opt Astron Observ, Tucson, AZ 85719 USA. [Marinoni, C.] Ctr Phys Theor, F-13288 Marseille, France. [McCracken, H. J.] Univ Paris 06, Inst Astrophys Paris, UMR7095CNRS, F-75014 Paris, France. [Meneux, B.] Univ Sternwarte, D-81679 Munich, Germany. [Scaramella, R.] Osserv Astron Roma, INAF, I-00040 Monte Porzio Catone, Italy. RP Kampczyk, P (reprint author), ETH, Inst Astron, CH-8093 Zurich, Switzerland. EM kampczyk@phys.ethz.ch RI Kneib, Jean-Paul/A-7919-2015; Bardelli, Sandro/O-9369-2015; Cappi, Alberto/O-9391-2015; Zucca, Elena/O-9396-2015; Mignoli, Marco/O-9426-2015; Bolzonella, Micol/O-9495-2015; OI bottini, dario/0000-0001-6917-041X; Pozzetti, Lucia/0000-0001-7085-0412; Scodeggio, Marco/0000-0002-2282-5850; Franzetti, Paolo/0000-0002-6986-0127; Vergani, Daniela/0000-0003-0898-2216; Scaramella, Roberto/0000-0003-2229-193X; Oesch, Pascal/0000-0001-5851-6649; Maier, Christian/0000-0001-6405-2182; Garilli, Bianca/0000-0001-7455-8750; Kneib, Jean-Paul/0000-0002-4616-4989; Bardelli, Sandro/0000-0002-8900-0298; Cappi, Alberto/0000-0002-9200-7167; Zucca, Elena/0000-0002-5845-8132; Mignoli, Marco/0000-0002-9087-2835; Bolzonella, Micol/0000-0003-3278-4607; Bongiorno, Angela/0000-0002-0101-6624; Fumana, Marco/0000-0001-6787-5950; Iovino, Angela/0000-0001-6958-0304; Zamorani, Giovanni/0000-0002-2318-301X; Perez Montero, E/0000-0003-3985-4882; Koekemoer, Anton/0000-0002-6610-2048 FU Swiss National Science Foundation FX The zCOSMOS survey was undertaken at the ESO VLT as Large Program 175. A-0839. We gratefully acknowledge the work of many individuals, not appearing as authors of this paper, whose work has enabled large surveys such as COSMOS and zCOSMOS. We thank an anonymous referee for the useful feedback. The Millennium Simulation databases used in this paper and the Web application providing online access to them were constructed as part of the activities of the German Astrophysical Virtual Observatory. This work has been supported in part by the Swiss National Science Foundation. NR 97 TC 18 Z9 18 U1 0 U2 4 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 0004-637X J9 ASTROPHYS J JI Astrophys. J. PD JAN 1 PY 2013 VL 762 IS 1 AR 43 DI 10.1088/0004-637X/762/1/43 PG 16 WC Astronomy & Astrophysics SC Astronomy & Astrophysics GA 063NY UT WOS:000313007900043 ER PT J AU Perez-Gonzalez, PG Cava, A Barro, G Villar, V Cardiel, N Ferreras, I Rodriguez-Espinosa, JM Alonso-Herrero, A Balcells, M Cenarro, J Cepa, J Charlot, S Cimatti, A Conselice, CJ Daddi, E Donley, J Elbaz, D Espino, N Gallego, J Gobat, R Gonzalez-Martin, O Guzman, R Hernan-Caballero, A Munoz-Tunon, C Renzini, A Rodriguez-Zaurin, J Tresse, L Trujillo, I Zamorano, J AF Perez-Gonzalez, Pablo G. Cava, Antonio Barro, Guillermo Villar, Victor Cardiel, Nicolas Ferreras, Ignacio Miguel Rodriguez-Espinosa, Jose Alonso-Herrero, Almudena Balcells, Marc Cenarro, Javier Cepa, Jordi Charlot, Stephane Cimatti, Andrea Conselice, Christopher J. Daddi, Emmanuele Donley, Jennifer Elbaz, David Espino, Nestor Gallego, Jesus Gobat, R. Gonzalez-Martin, Omaira Guzman, Rafael Hernan-Caballero, Antonio Munoz-Tunon, Casiana Renzini, Alvio Rodriguez-Zaurin, Javier Tresse, Laurence Trujillo, Ignacio Zamorano, Jaime TI SHARDS: AN OPTICAL SPECTRO-PHOTOMETRIC SURVEY OF DISTANT GALAXIES SO ASTROPHYSICAL JOURNAL LA English DT Article DE galaxies: high-redshift; galaxies: photometry; galaxies: starburst; infrared: galaxies ID STAR-FORMING GALAXIES; SUBARU DEEP FIELD; ALPHA LUMINOSITY FUNCTION; SIMILAR-TO 2; OLD STELLAR POPULATIONS; DUST-OBSCURED GALAXIES; FORMATION RATE DENSITY; BARYON ACOUSTIC-OSCILLATIONS; EXTRAGALACTIC LEGACY SURVEY; PROBE WMAP OBSERVATIONS AB We present the Survey for High-z Absorption Red and Dead Sources (SHARDS), an ESO/GTC Large Program carried out using the OSIRIS instrument on the 10.4 m Gran Telescopio Canarias (GTC). SHARDS is an ultra-deep optical spectro-photometric survey of the GOODS-N field covering 130 arcmin(2) at wavelengths between 500 and 950 nm with 24 contiguous medium-band filters (providing a spectral resolution R similar to 50). The data reach an AB magnitude of 26.5 (at least at a 3 sigma level) with sub-arcsec seeing in all bands. SHARDS' main goal is to obtain accurate physical properties of intermediate-and high-z galaxies using well-sampled optical spectral energy distributions (SEDs) with sufficient spectral resolution to measure absorption and emission features, whose analysis will provide reliable stellar population and active galactic nucleus (AGN) parameters. Among the different populations of high-z galaxies, SHARDS' principal targets are massive quiescent galaxies at z > 1, whose existence is one of the major challenges facing current hierarchical models of galaxy formation. In this paper, we outline the observational strategy and include a detailed discussion of the special reduction and calibration procedures which should be applied to the GTC/OSIRIS data. An assessment of the SHARDS data quality is also performed. We present science demonstration results on the detection and study of emission-line galaxies (star-forming objects and AGNs) at z = 0-5. We also analyze the SEDs for a sample of 27 quiescent massive galaxies with spectroscopic redshifts in the range 1.0 < z less than or similar to 1.4. We discuss the improvements introduced by the SHARDS data set in the analysis of their star formation history and stellar properties. We discuss the systematics arising from the use of different stellar population libraries, typical in this kind of study. Averaging the results from the different libraries, we find that the UV-to-MIR SEDs of the massive quiescent galaxies at z = 1.0-1.4 are well described by an exponentially decaying star formation history with scale t = 100-200 Myr, age around 1.5-2.0 Gyr, solar or slightly sub-solar metallicity, and moderate extinction, A(V) similar to 0.5 mag. We also find that galaxies with masses above M* are typically older than lighter galaxies, as expected in a downsizing scenario of galaxy formation. This trend is, however, model dependent, i.e., it is significantly more evident in the results obtained with some stellar population synthesis libraries, and almost absent in others. C1 [Perez-Gonzalez, Pablo G.; Cava, Antonio; Barro, Guillermo; Villar, Victor; Cardiel, Nicolas; Espino, Nestor; Gallego, Jesus; Zamorano, Jaime] Univ Complutense Madrid, Fac CC Fis, Dept Astrofis, E-28040 Madrid, Spain. [Barro, Guillermo] Univ Calif Santa Cruz, Dept Astron & Astrophys, UCO Lick Observ, Santa Cruz, CA 95064 USA. [Ferreras, Ignacio] Univ Coll London, Mullard Space Sci Lab, Dorking RH5 6NT, Surrey, England. [Miguel Rodriguez-Espinosa, Jose; Balcells, Marc; Cepa, Jordi; Gonzalez-Martin, Omaira; Munoz-Tunon, Casiana; Rodriguez-Zaurin, Javier; Trujillo, Ignacio] Inst Astrofis Canarias, E-38200 Tenerife, Spain. [Miguel Rodriguez-Espinosa, Jose; Balcells, Marc; Cepa, Jordi; Gonzalez-Martin, Omaira; Munoz-Tunon, Casiana; Rodriguez-Zaurin, Javier; Trujillo, Ignacio] Univ La Laguna, Dept Astrofis, E-38205 Tenerife, Spain. [Alonso-Herrero, Almudena; Hernan-Caballero, Antonio] Univ Cantabria, CSIC, Inst Fis Cantabria, E-39005 Santander, Spain. [Balcells, Marc] Isaac Newton Grp Telescopes, E-38700 Santa Cruz De La Palma, Spain. [Cenarro, Javier] Ctr Estudios Fis Cosmos Aragon, E-44001 Teruel, Spain. [Charlot, Stephane] Univ Paris 06, CNRS, Inst Astrophys Paris, UMR 7095, F-75014 Paris, France. [Cimatti, Andrea] Univ Bologna, Dipartimento Astron, I-40127 Bologna, Italy. [Conselice, Christopher J.] Univ Nottingham, Sch Phys & Astron, Nottingham NG7 2RD, England. [Daddi, Emmanuele; Elbaz, David] CEA, Lab AIM, Irfu SAp, F-91191 Gif Sur Yvette, France. [Donley, Jennifer] Los Alamos Natl Lab, Los Alamos, NM USA. [Gobat, R.] Univ Paris Diderot, Irfu Serv Astrophys, Lab AIM Paris Saclay, CEA,DSM,CNRS,CEA Saclay, F-91191 Gif Sur Yvette, France. [Guzman, Rafael] Univ Florida, Dept Astron, Bryant Space Sci Ctr 211, Gainesville, FL 32611 USA. [Renzini, Alvio] Osserv Astron Padova, INAF, I-35122 Padua, Italy. [Tresse, Laurence] Aix Marseille Univ, CNRS, LAM, UMR 7326, F-13388 Marseille, France. [Perez-Gonzalez, Pablo G.] Univ Arizona, Steward Observ, Tucson, AZ 85721 USA. RP Perez-Gonzalez, PG (reprint author), Univ Complutense Madrid, Fac CC Fis, Dept Astrofis, E-28040 Madrid, Spain. RI Cava, Antonio/C-5274-2017; Conselice, Christopher/B-4348-2013; Daddi, Emanuele/D-1649-2012; Zamorano, Jaime/K-7706-2014; Cardiel, Nicolas/F-1030-2016; Perez-Gonzalez, Pablo/J-2871-2016; Alonso-Herrero, Almudena/H-1426-2015; OI Cava, Antonio/0000-0002-4821-1275; Ferreras, Ignacio/0000-0003-4584-3127; Daddi, Emanuele/0000-0002-3331-9590; Zamorano, Jaime/0000-0002-8993-5894; Cardiel, Nicolas/0000-0002-9334-2979; Perez-Gonzalez, Pablo/0000-0003-4528-5639; Alonso-Herrero, Almudena/0000-0001-6794-2519; Conselice, Christopher/0000-0003-1949-7638 FU Spanish Programa Nacional de Astronomia y Astrofisica [AYA2009-07723-E, AYA2009-10368]; Spanish MICINN/MINECO under the Consolider-Ingenio 2010 Program [CSD2006-00070]; Universidad de Cantabria through the Augusto G. Linares Program [AYA2010-21887-C04-04] FX We acknowledge support from the Spanish Programa Nacional de Astronomia y Astrofisica under grants AYA2009-07723-E and AYA2009-10368. SHARDS has been funded by the Spanish MICINN/MINECO under the Consolider-Ingenio 2010 Program grant CSD2006-00070: First Science with the GTC. O.G.-M., C.M.-T., J.M.R.-E., and J.R.-Z. wish to acknowledge support from grant AYA2010-21887-C04-04. A.A.-H. and A.H.-C. acknowledge financial support from the Universidad de Cantabria through the Augusto G. Linares Program. This work has made use of the Rainbow Cosmological Surveys Database, which is operated by the Universidad Complutense de Madrid (UCM). This research has made use of the VizieR catalogue access tool, CDS, Strasbourg, France. Based on observations made with the Gran Telescopio Canarias (GTC), installed at the Spanish Observatorio del Roque de los Muchachos of the Instituto de Astrofisica de Canarias, in the island of La Palma. We thank all the GTC Staff for their support and enthusiasm with the SHARDS project, and we especially acknowledge the help from Antonio Cabrera and Rene Rutten. The work is also based on observations collected at the Centro Astronomico Hispano Aleman (CAHA) at Calar Alto, operated jointly by the Max-Planck-Institut fur Astronomie and the Instituto de Astrofisica de Andalucia (CSIC). We thank the referee for her/his very useful and positive comments. NR 189 TC 20 Z9 20 U1 0 U2 9 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 0004-637X EI 1538-4357 J9 ASTROPHYS J JI Astrophys. J. PD JAN 1 PY 2013 VL 762 IS 1 AR 46 DI 10.1088/0004-637X/762/1/46 PG 24 WC Astronomy & Astrophysics SC Astronomy & Astrophysics GA 063NY UT WOS:000313007900046 ER PT J AU Pignatari, M Hirschi, R Wiescher, M Gallino, R Bennett, M Beard, M Fryer, C Herwig, F Rockefeller, G Timmes, FX AF Pignatari, M. Hirschi, R. Wiescher, M. Gallino, R. Bennett, M. Beard, M. Fryer, C. Herwig, F. Rockefeller, G. Timmes, F. X. CA NuGrid Collaboration TI THE C-12+C-12 REACTION AND THE IMPACT ON NUCLEOSYNTHESIS IN MASSIVE STARS SO ASTROPHYSICAL JOURNAL LA English DT Article DE stars: abundances; stars: evolution; stars: interiors ID S-PROCESS NUCLEOSYNTHESIS; THERMONUCLEAR REACTION-RATES; NEUTRINO-DRIVEN WINDS; GIANT BRANCH STARS; GALACTIC CHEMICAL EVOLUTION; CORE-COLLAPSE SUPERNOVAE; WEAK INTERACTION RATES; HIGH-ENTROPY-WIND; P-PROCESS NUCLEI; STELLAR EVOLUTION AB Despite much effort in the past decades, the C-burning reaction rate is uncertain by several orders of magnitude, and the relative strength between the different channels C-12(C-12, alpha)Ne-20, C-12(C-12, p)Na-23, and C-12(C-12, n)Mg-23 is poorly determined. Additionally, in C-burning conditions a high C-12+C-12 rate may lead to lower central C-burning temperatures and to C-13(alpha, n)O-16 emerging as a more dominant neutron source than Ne-22(alpha, n)Mg-25, increasing significantly the s-process production. This is due to the chain C-12(p,gamma)N-13 followed by N-13(beta+)C-13, where the photodisintegration reverse channel N-13(gamma, p)C-12 is strongly decreasing with increasing temperature. Presented here is the impact of the C-12+C-12 reaction uncertainties on the s-process and on explosive p-process nucleosynthesis in massive stars, including also fast rotating massive stars at low metallicity. Using various C-12+C-12 rates, in particular an upper and lower rate limit of similar to 50,000 higher and similar to 20 lower than the standard rate at 5 x 10(8) K, five 25M(circle dot) stellar models are calculated. The enhanced s-process signature due to C-13(alpha, n)O-16 activation is considered, taking into account the impact of the uncertainty of all three C-burning reaction branches. Consequently, we show that the p-process abundances have an average production factor increased up to about a factor of eight compared with the standard case, efficiently producing the elusive Mo and Ru proton-rich isotopes. We also show that an s-process being driven by C-13(alpha, n)O-16 is a secondary process, even though the abundance of C-13 does not depend on the initial metal content. Finally, implications for the Sr-peak elements inventory in the solar system and at low metallicity are discussed. C1 [Pignatari, M.] Univ Basel, Dept Phys, CH-4056 Basel, Switzerland. [Hirschi, R.; Bennett, M.] Univ Keele, Astrophys Grp, EPSAM Inst, Keele ST5 5BG, Staffs, England. [Hirschi, R.] Univ Tokyo, Inst Phys & Math Universe, Kashiwa, Chiba 2778583, Japan. [Wiescher, M.; Beard, M.] Univ Notre Dame, Dept Phys, Notre Dame, IN 46556 USA. [Wiescher, M.; Beard, M.; Timmes, F. X.] Joint Inst Nucl Astrophys, Notre Dame, IN 46556 USA. [Gallino, R.] Univ Turin, I-10126 Turin, Italy. [Fryer, C.; Rockefeller, G.] LANL, Computat Phys & Methods CCS 2, Los Alamos, NM 87545 USA. [Herwig, F.] Univ Victoria, Dept Phys & Astron, Victoria, BC V8P 5C2, Canada. [Timmes, F. X.] Arizona State Univ, SESE, Tempe, AZ 85287 USA. RP Pignatari, M (reprint author), Univ Basel, Dept Phys, Klingelbergstr 82, CH-4056 Basel, Switzerland. EM marco.pignatari@unibas.ch OI Pignatari, Marco/0000-0002-9048-6010 FU NSF [PHY 02-16783, PHY 09-22648]; EU [MIRG-CT-2006-046520]; STFC (UK); NSERC Discovery grant (Canada); Ambizione grant of the SNSF (Switzerland); (Canada) Department of Physics and Astronomy at the University of Victoria; Core project Eurogenesis FX NuGrid acknowledges significant support from NSF grants PHY 02-16783 and PHY 09-22648 (Joint Institute for Nuclear Astrophysics, JINA) and EU MIRG-CT-2006-046520. The continued work on codes and in disseminating data is made possible through funding from STFC (R.H., UK), an NSERC Discovery grant (F.H., Canada), and an Ambizione grant of the SNSF (M.P., Switzerland). NuGrid computations were performed at the Arizona Advanced Computing Center (USA), the high-performance computer KHAOS at EPSAM Institute at Keele University (UK) as well as CFI (Canada) funded computing resources at the Department of Physics and Astronomy at the University of Victoria and through Computing Time Resource Allocation through the Compute Canada WestGrid consortium. M.P. also thanks the support from Core project Eurogenesis. NR 137 TC 37 Z9 37 U1 1 U2 16 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 0004-637X EI 1538-4357 J9 ASTROPHYS J JI Astrophys. J. PD JAN 1 PY 2013 VL 762 IS 1 AR 31 DI 10.1088/0004-637X/762/1/31 PG 23 WC Astronomy & Astrophysics SC Astronomy & Astrophysics GA 063NY UT WOS:000313007900031 ER PT J AU Martin, KR Barua, D Kauffman, AL Westrate, LM Posner, RG Hlavacek, WS MacKeigan, JP AF Martin, Katie R. Barua, Dipak Kauffman, Audra L. Westrate, Laura M. Posner, Richard G. Hlavacek, William S. MacKeigan, Jeffrey P. TI Computational model for autophagic vesicle dynamics in single cells SO AUTOPHAGY LA English DT Article DE computational; mathematical; autophagy; single cell; quantitative biology; microscopy; live-cell imaging; systems biology; Gillespie's method; LC3 ID COMPUTER-SIMULATION; SYSTEMS BIOLOGY; HUMAN CANCER; PROTEIN; ASSOCIATION; ENDOSOMES; FUSION; ATG9; LC3; BIOGENESIS AB Macroautophagy (autophagy) is a cellular recycling program essential for homeostasis and survival during cytotoxic stress. This process, which has an emerging role in disease etiology and treatment, is executed in four stages through the coordinated action of more than 30 proteins. An effective strategy for studying complicated cellular processes, such as autophagy, involves the construction and analysis of mathematical or computational models. When developed and refined from experimental knowledge, these models can be used to interrogate signaling pathways, formulate novel hypotheses about systems, and make predictions about cell signaling changes induced by specific interventions. Here, we present the development of a computational model describing autophagic vesicle dynamics in a mammalian system. We used time-resolved, live-cell microscopy to measure the synthesis and turnover of autophagic vesicles in single cells. The stochastically simulated model was consistent with data acquired during conditions of both basal and chemically-induced autophagy. The model was tested by genetic modulation of autophagic machinery and found to accurately predict vesicle dynamics observed experimentally. Furthermore, the model generated an unforeseen prediction about vesicle size that is consistent with both published findings and our experimental observations. Taken together, this model is accurate and useful and can serve as the foundation for future efforts aimed at quantitative characterization of autophagy. C1 [Martin, Katie R.; Kauffman, Audra L.; Westrate, Laura M.; MacKeigan, Jeffrey P.] Van Andel Res Inst, Lab Syst Biol, Grand Rapids, MI USA. [Barua, Dipak; Hlavacek, William S.] Los Alamos Natl Lab, Ctr Nonlinear Studies, Los Alamos, NM 87545 USA. [Barua, Dipak; Hlavacek, William S.] Los Alamos Natl Lab, Theoret Biol & Biophys Grp, Div Theoret, Los Alamos, NM 87545 USA. [Westrate, Laura M.] Van Andel Inst Grad Sch, Grand Rapids, MI USA. [Posner, Richard G.; Hlavacek, William S.] Translat Genom Res Inst, Clin Translat Res Div, Scottsdale, AZ USA. RP MacKeigan, JP (reprint author), Van Andel Res Inst, Lab Syst Biol, Grand Rapids, MI USA. EM jeff.mackeigan@vai.org OI Hlavacek, William/0000-0003-4383-8711 FU Department of Defense Prostate Cancer Research Program of the Office of Congressionally Directed Medical Research Programs [PC081089]; National Cancer Institute [R01CA138651]; NIH [GM085273]; DOE [DE-AC52-06NA25396]; Randy Pausch Scholars Program; TGen Foundation; Howard Young; globalCure National Advisory Council FX We thank Srabanti Chaudhury and Nikolai A. Sinitsyn for helpful discussions. This work was supported by the Department of Defense Prostate Cancer Research Program of the Office of Congressionally Directed Medical Research Programs PC081089 to J.P.M. J.P.M. is also supported by Award Number R01CA138651 from the National Cancer Institute. This work was also supported by NIH grant GM085273 and by DOE contract DE-AC52-06NA25396. W. S. H. was supported by the Randy Pausch Scholars Program, which is sponsored by the TGen Foundation, Howard Young and the globalCure National Advisory Council. The funders had no role in study design, data collection and analysis, decision to publish or preparation of the manuscript. NR 62 TC 8 Z9 8 U1 1 U2 25 PU LANDES BIOSCIENCE PI AUSTIN PA 1806 RIO GRANDE ST, AUSTIN, TX 78702 USA SN 1554-8627 J9 AUTOPHAGY JI Autophagy PD JAN PY 2013 VL 9 IS 1 BP 74 EP 92 DI 10.4161/auto.22532 PG 19 WC Cell Biology SC Cell Biology GA 064LY UT WOS:000313077900006 PM 23196898 ER PT J AU Perez-Pimienta, JA Lopez-Ortega, MG Varanasi, P Stavila, V Cheng, G Singh, S Simmons, BA AF Perez-Pimienta, Jose A. Lopez-Ortega, Monica G. Varanasi, Patanjali Stavila, Vitalie Cheng, Gang Singh, Seema Simmons, Blake A. TI Comparison of the impact of ionic liquid pretreatment on recalcitrance of agave bagasse and switchgrass SO BIORESOURCE TECHNOLOGY LA English DT Article DE Agave bagasse; Switchgrass; Biomass pretreatment; Ionic liquid ID ENZYMATIC DIGESTIBILITY; LIGNOCELLULOSIC BIOMASS; CELLULOSE; HYDROLYSIS; LIGNIN; ACID; SACCHARIFICATION; DISSOLUTION; FEATURES AB Lignocellulose represents a sustainable source of carbon for transformation into biofuels. Effective biomass to sugar conversion strategies are needed to lower processing cost without degradation of polysaccharides. Since ionic liquids (ILs) are excellent solvents for pretreatment/dissolution of biomass, IL pretreatment was carried out on agave bagasse (AGB-byproduct of tequila industry) and digestibility and sugar yield was compared with that obtained with switchgrass (SWG). The IL pretreatment was conducted using ([C2mim][OAc]) at 120 and 160 degrees C for 3 h and 15% biomass loading. While pretreatment using [C2mim][OAc] was very effective in improving the digestibility of both feedstocks, IL pretreatment at 160 degrees C resulted in higher delignification for AGB (45.5%) than for SWG (38.4%) when compared to 120 degrees C (AGB-16.6%, SWG-8.2%), formation of a highly amorphous cellulose structure and a significant enhancement of enzyme kinetics. These results highlight the potential of AGB as a biofuel feedstock that can produce high sugar yields with IL pretreatment. (C) 2012 Elsevier Ltd. All rights reserved. C1 [Perez-Pimienta, Jose A.; Lopez-Ortega, Monica G.] Univ Autonoma Nayarit, Dept Chem Engn, Tepic, Mexico. [Varanasi, Patanjali; Cheng, Gang; Singh, Seema; Simmons, Blake A.] Lawrence Berkeley Natl Lab, Joint BioEnergy Inst, Phys Biosci Div, Emeryville, CA USA. [Varanasi, Patanjali; Cheng, Gang; Singh, Seema; Simmons, Blake A.] Sandia Natl Labs, Biomass Sci & Convers Technol Dept, Livermore, CA USA. [Stavila, Vitalie] Sandia Natl Labs, Energy Nanomat Dept, Livermore, CA USA. RP Perez-Pimienta, JA (reprint author), Univ Autonoma Nayarit, Dept Chem Engn, Tepic, Mexico. EM joseantoniopimienta@gmail.com RI Stavila, Vitalie/B-6464-2008; OI Stavila, Vitalie/0000-0003-0981-0432; Perez-Pimienta, Jose A./0000-0002-1370-8716; Simmons, Blake/0000-0002-1332-1810 FU US Department of Energy, Office of Science, Office of Biological and Environmental Research [DE-AC02-05CH11231] FX The authors thank Novozymes for the gift of the cellulase cocktails and the laboratory of Dr. Daniel Putnam at UC-Davis for the switchgrass used in this work. This work was part of the DOE Joint BioEnergy Institute (http://www.jbei.org) supported by the US Department of Energy, Office of Science, Office of Biological and Environmental Research, through Contract DE-AC02-05CH11231 between Lawrence Berkeley National Laboratory and the US Department of Energy. NR 30 TC 26 Z9 27 U1 2 U2 110 PU ELSEVIER SCI LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, OXON, ENGLAND SN 0960-8524 J9 BIORESOURCE TECHNOL JI Bioresour. Technol. PD JAN PY 2013 VL 127 BP 18 EP 24 DI 10.1016/j.biortech.2012.09.124 PG 7 WC Agricultural Engineering; Biotechnology & Applied Microbiology; Energy & Fuels SC Agriculture; Biotechnology & Applied Microbiology; Energy & Fuels GA 062NK UT WOS:000312926400003 PM 23131619 ER PT J AU Wang, CW Peng, JH Li, H Bi, XTT Legros, R Lim, CJ Sokhansanj, S AF Wang, Congwei Peng, Jianghong Li, Hui Bi, Xiaotao T. Legros, Robert Lim, C. J. Sokhansanj, Shahab TI Oxidative torrefaction of biomass residues and densification of torrefied sawdust to pellets SO BIORESOURCE TECHNOLOGY LA English DT Article DE Oxidative torrefaction; Fluidized bed; Sawdust; Kinetics; Pellets ID COMBUSTION CHARACTERISTICS; LIGNOCELLULOSIC BIOMASS; THERMAL PRETREATMENT; MOISTURE-CONTENT; WHEAT-STRAW; WOOD; PELLETIZATION; TEMPERATURE; DURABILITY; SPRUCE AB Oxidative torrefaction of sawdust with a carrier gas containing 3-6% O-2 was investigated in a TG and a fluidized bed reactor, with the properties of the torrefied sawdust and pellets compared with traditional torrefaction without any O-2, as well as the dry raw material. It is found that the oxidative torrefaction process produced torrefied sawdust and pellets of similar properties as normally torrefied sawdust and corresponding pellets, especially on the density, energy consumption for pelletization, higher heating value and energy yield. For moisture absorption and hardness of the torrefied pellets, the oxidative torrefaction process showed slightly poor but negligible performance. Therefore, it is feasible to use oxygen laden combustion flue gases as the carrier gas for torrefaction of biomass. Besides, torrefied sawdust can be made into dense and strong pellets of high hydrophobicity at a higher die temperature than normally used in the production of traditional control pellets. (C) 2012 Elsevier Ltd. All rights reserved. C1 [Wang, Congwei] Chinese Acad Sci, Guangzhou Inst Energy Convers, Key Lab Renewable Energy & Gas Hydrate, Guangzhou 510640, Guangdong, Peoples R China. [Wang, Congwei; Peng, Jianghong; Li, Hui; Bi, Xiaotao T.; Legros, Robert; Lim, C. J.; Sokhansanj, Shahab] Univ British Columbia, Dept Chem & Biol Engn, Clean Energy Res Ctr, Vancouver, BC V6T 1Z3, Canada. [Li, Hui] Hunan Acad Forestry, Changsha 410004, Hunan, Peoples R China. [Li, Hui] Biodiesel Engn Res Ctr Hunan Prov, Changsha 410004, Hunan, Peoples R China. [Legros, Robert] Ecole Polytech, Dept Chem Engn, Montreal, PQ H3C 3A7, Canada. [Sokhansanj, Shahab] Oak Ridge Natl Lab, Div Environm Sci, Oak Ridge, TN 37831 USA. RP Bi, XTT (reprint author), Univ British Columbia, Dept Chem & Biol Engn, Clean Energy Res Ctr, Vancouver, BC V6T 1Z3, Canada. EM xbi@chbe.ubc.ca FU NSERC; Agriculture Canada ABIN program; China Scholarship Council FX The authors are grateful to the financial support from a NSERC Discovery Grant and the Agriculture Canada ABIN program, as well as a scholarship from the China Scholarship Council. NR 37 TC 39 Z9 40 U1 0 U2 74 PU ELSEVIER SCI LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, OXON, ENGLAND SN 0960-8524 J9 BIORESOURCE TECHNOL JI Bioresour. Technol. PD JAN PY 2013 VL 127 BP 318 EP 325 DI 10.1016/j.biortech.2012.09.092 PG 8 WC Agricultural Engineering; Biotechnology & Applied Microbiology; Energy & Fuels SC Agriculture; Biotechnology & Applied Microbiology; Energy & Fuels GA 062NK UT WOS:000312926400044 PM 23131655 ER PT J AU Jia, JJ Yao, W Amugongo, S Shahnazari, M Dai, WW Lay, YAE Olvera, D Zimmermann, EA Ritchie, RO Li, CS Alliston, T Lane, NE AF Jia, Junjing Yao, Wei Amugongo, Sarah Shahnazari, Mohammad Dai, Weiwei Lay, Yu-An E. Olvera, Diana Zimmermann, Elizabeth A. Ritchie, Robert O. Li, Chin-Shang Alliston, Tamara Lane, Nancy E. TI Prolonged alendronate treatment prevents the decline in serum TGF-beta 1 levels and reduces cortical bone strength in long-term estrogen deficiency rat model SO BONE LA English DT Article DE Alendronate; TGF-beta 1; Cortical bone; Bone quality ID GROWTH-FACTOR-BETA; NITROGEN-CONTAINING BISPHOSPHONATES; MICRO-COMPUTED TOMOGRAPHY; MESENCHYMAL STEM-CELLS; 3-AND 5-YEAR TREATMENT; OSTEOBLAST-LIKE CELLS; TGF-BETA; TRABECULAR BONE; IN-VITRO; MECHANICAL-PROPERTIES AB Introduction: While the anti-resorptive effects of the bisphosphonates (BPS) are well documented, many questions remain about their mechanisms of action, particularly following long-term use. This study evaluated the effects of alendronate (Ale) treatment on TGF-beta 1 signaling in mesenchymal stem cells (MSCs) and osteocytes, and the relationship between prolonged alendronate treatment on systemic TGF-beta 1 levels and bone strength. Methods: TGF-beta 1 expression and signaling were evaluated in MSCs and osteocytic MLO-Y4 cells following Ale treatment Serum total TGF-beta 1 levels, a bone resorption marker (DPD/Cr), three-dimensional microCT scans and biomechanical tests from both the trabecular and cortical bone were measured in ovariectomized rats that either received continuous Ale treatment for 360 days or Ale treatment for 120 days followed by 240 days of vehicle. Linear regression tests were performed to determine the association of serum total TGF-beta 1 levels and both the trabecular (vertebrae) and cortical (tibiae) bone strength. Results: Ale increased TGF-beta 1 signaling in the MSCs but not in the MLO-Y4 cells. Ale treatment increased serum TGF-beta 1 levels and the numbers of TGF-beta 1-positive osteocytes and periosteal cells in cortical bone. Serum TGF-beta 1 levels were not associated with vertebral maximum load and strength but was negatively associated with cortical bone maximum load and ultimate strength. Conclusions: The increase of serum TGF-beta 1 levels during acute phase of estrogen deficiency is likely due to increased osteoclast-mediated release of matrix-derived latent TGF-beta 1. Long-term estrogen-deficiency generally results in a decline in serum TGF-beta 1 levels that are maintained by Ale treatment Measuring serum total TGF-beta 1 levels may help to determine cortical bone quality following alendronate treatment. (C) 2012 Elsevier Inc. All rights reserved. C1 [Jia, Junjing; Yao, Wei; Amugongo, Sarah; Shahnazari, Mohammad; Dai, Weiwei; Lay, Yu-An E.; Lane, Nancy E.] Univ Calif Davis Med Ctr, Musculoskeletal Res Unit, Dept Med, Sacramento, CA 95817 USA. [Olvera, Diana; Zimmermann, Elizabeth A.; Ritchie, Robert O.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. [Ritchie, Robert O.] Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA. [Shahnazari, Mohammad] Univ Calif San Francisco, Vet Adm Med Ctr, San Francisco, CA 94121 USA. [Li, Chin-Shang] Univ Calif Davis, Div Biostat, Dept Publ Hlth Sci, Davis, CA 95616 USA. [Alliston, Tamara] Univ Calif San Francisco, Dept Orthopaed Surg, San Francisco, CA 94143 USA. RP Lane, NE (reprint author), UC Davis Hlth Syst, 4625 2nd Ave,Suite 1002, Sacramento, CA 95817 USA. EM nelane@ucdavis.edu RI Ritchie, Robert/A-8066-2008; Zimmermann, Elizabeth/A-4010-2015 OI Ritchie, Robert/0000-0002-0501-6998; FU National Institutes of Health (NIH) [R01 AR043052, 1K12HD05195801, 5K24AR048841-09, UL1 TR000002]; National Institutes of Health (NIH/NIDCR) [5R01 DE015633]; National Institute of Health (NIH/NIDCR) [R01 DE019284] FX This work was funded by National Institutes of Health (NIH) grants nos. R01 AR043052 and 1K12HD05195801, and 5K24AR048841-09. The statistical analyses were supported by the National Center for Advancing Translational Sciences (NCATS), National Institutes of Health (NIH), through grant no. UL1 TR000002. The involvement of ROR was supported by National Institutes of Health (NIH/NIDCR) under grant no. 5R01 DE015633 to the Lawrence Berkeley National Laboratory (LBNL). The involvement of TA was supported by National Institute of Health (NIH/NIDCR) under grant R01 DE019284. NR 76 TC 6 Z9 7 U1 0 U2 16 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 8756-3282 J9 BONE JI Bone PD JAN PY 2013 VL 52 IS 1 BP 424 EP 432 DI 10.1016/j.bone.2012.10.017 PG 9 WC Endocrinology & Metabolism SC Endocrinology & Metabolism GA 060BK UT WOS:000312750700051 PM 23088940 ER PT J AU Faillace, ME Phipps, RJ Miller, LM AF Faillace, Meghan E. Phipps, Roger J. Miller, Lisa M. TI Fourier Transform Infrared Imaging as a Tool to Chemically and Spatially Characterize Matrix-Mineral Deposition in Osteoblasts SO CALCIFIED TISSUE INTERNATIONAL LA English DT Article DE Bisphosphonates; Collagen; Fourier transform infrared imaging; Mineralization; Osteoblasts; Risedronate ID FTIR MICROSPECTROSCOPIC ANALYSIS; GROWTH PLATE CHONDROCYTES; MARROW STROMAL CELLS; ILIAC CREST BIOPSIES; NON-RESORBING CELLS; IN-VITRO; CALCIUM-PHOSPHATE; EXTRACELLULAR-MATRIX; GENE-EXPRESSION; BONE-FORMATION AB Mineralizing osteoblasts are regularly used to study osteogenesis and model in vivo bone formation. Thus, it is important to verify that the mineral and matrix being formed in situ are comparable to those found in vivo. However, it has been shown that histochemical techniques alone are not sufficient for identifying calcium phosphate-containing mineral. The goal of the present study was to demonstrate the use of Fourier transform infrared imaging (FTIRI) as a tool for characterizing the spatial distribution and colocalization of the collagen matrix and the mineral phase during the mineralization process of osteoblasts in situ. MC3T3-E1 mouse osteoblasts were mineralized in culture for 28 days and FTIRI was used to evaluate the collagen content, collagen cross-linking, mineralization level and speciation, and mineral crystallinity in a spatially resolved fashion as a function of time. To test whether FTIRI could detect subtle changes in the mineralization process, cells were treated with risedronate (RIS). Results showed that collagen deposition and mineralization progressed over time and that the apatite mineral was associated with a collagenous matrix rather than ectopic mineral. The process was temporarily slowed by RIS, where the inhibition of osteoblast function caused slowed collagen production and cross-linking, leading to decreased mineralization. This study demonstrates that FTIRI is a complementary tool to histochemistry for spatially correlating the collagen matrix distribution and the nature of the resultant mineral during the process of osteoblast mineralization. It can further be used to detect small perturbations in the osteoid and mineral deposition process. C1 [Faillace, Meghan E.; Miller, Lisa M.] Brookhaven Natl Lab, Natl Synchrotron Light Source, Upton, NY 11973 USA. [Faillace, Meghan E.; Miller, Lisa M.] SUNY Stony Brook, Dept Biomed Engn, Stony Brook, NY 11790 USA. [Phipps, Roger J.] Husson Univ, Sch Pharm, Bangor, ME USA. RP Miller, LM (reprint author), Brookhaven Natl Lab, Natl Synchrotron Light Source, Upton, NY 11973 USA. EM lmiller@bnl.gov FU Alliance for Better Bone Health; BNL Laboratory-Directed Research and Development (LDRD) grant [05-048]; United States Department of Energy [DE-AC02-98CH10886] FX M. F. was supported by the Alliance for Better Bone Health and a BNL Laboratory-Directed Research and Development (LDRD) grant (05-048). The NSLS is supported by the United States Department of Energy under contract DE-AC02-98CH10886. Procter & Gamble Pharmaceuticals Inc. Kindly provided the risedronate. NR 84 TC 2 Z9 2 U1 0 U2 15 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 0171-967X J9 CALCIFIED TISSUE INT JI Calcif. Tissue Int. PD JAN PY 2013 VL 92 IS 1 BP 50 EP 58 DI 10.1007/s00223-012-9667-5 PG 9 WC Endocrinology & Metabolism SC Endocrinology & Metabolism GA 059OL UT WOS:000312714800008 PM 23143076 ER PT J AU Gupta, S Hlova, IZ Kobayashi, T Denys, RV Chen, F Zavaliy, IY Pruski, M Pecharsky, VK AF Gupta, Shalabh Hlova, Ihor Z. Kobayashi, Takeshi Denys, Roman V. Chen, Fu Zavaliy, Ihor Y. Pruski, Marek Pecharsky, Vitalij K. TI Facile synthesis and regeneration of Mg(BH4)(2) by high energy reactive ball milling of MgB2 SO CHEMICAL COMMUNICATIONS LA English DT Article ID HYDROGEN STORAGE; DEHYDROGENATION; SAMPLES AB We report direct hydrogenation of MgB2 in a planetary ball mill. Magnesium borohydride, Mg(BH4)(2), and various polyhedral borane anion salts have been synthesized at pressures between 50 and 350 bar H-2 without the need for subsequent isothermal hydrogenation at elevated temperature and pressure. The obtained products release similar to 4 wt% H-2 below 390 degrees C, and a major portion of Mg(BH4)(2) transforms back to MgB2 at around 300 degrees C, demonstrating the possibility of reversible hydrogen storage in an Mg(BH4)(2)-MgB2 system. C1 [Gupta, Shalabh; Hlova, Ihor Z.; Kobayashi, Takeshi; Chen, Fu; Pruski, Marek; Pecharsky, Vitalij K.] Iowa State Univ, Ames Lab, Ames, IA 50011 USA. [Hlova, Ihor Z.; Pecharsky, Vitalij K.] Iowa State Univ, Dept Mat Sci & Engn, Ames, IA 50011 USA. [Denys, Roman V.; Zavaliy, Ihor Y.] NAS Ukraine, Phys Mech Inst, UA-79601 Lvov, Ukraine. [Pruski, Marek] Iowa State Univ, Dept Chem, Ames, IA 50011 USA. RP Pruski, M (reprint author), Iowa State Univ, Ames Lab, Ames, IA 50011 USA. EM mpruski@iastate.edu; vitkp@ameslab.gov RI Denys, Roman/C-8386-2012 OI Denys, Roman/0000-0002-5479-8279 FU U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering [DE-AC02-07CH11358]; US Civilian Research and Development Foundation (CRDF) [UKC2-2970-LV-09] FX Research was supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering under Contract No. DE-AC02-07CH11358. RD and IZ were supported by the US Civilian Research and Development Foundation (CRDF), Grant UKC2-2970-LV-09. NR 21 TC 16 Z9 16 U1 5 U2 61 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1359-7345 J9 CHEM COMMUN JI Chem. Commun. PY 2013 VL 49 IS 8 BP 828 EP 830 DI 10.1039/c2cc36580d PG 3 WC Chemistry, Multidisciplinary SC Chemistry GA 056QG UT WOS:000312505500021 PM 23235431 ER PT J AU Yeh, YC Muller, J Bi, CH Hillson, NJ Beller, HR Chhabra, SR Singer, SW AF Yeh, Yi-Chun Mueller, Jana Bi, Changhao Hillson, Nathan J. Beller, Harry R. Chhabra, Swapnil R. Singer, Steven W. TI Functionalizing bacterial cell surfaces with a phage protein SO CHEMICAL COMMUNICATIONS LA English DT Article ID RECEPTOR-BINDING PROTEIN; ESCHERICHIA-COLI; FHUA; PB5; BACTERIOPHAGE-T5; CHEMISTRY; SEQUENCE; LAMBDA AB Functionalization of bacterial cell surfaces has the potential to introduce new activities by chemical modification. Here we show that a bacteriophage-receptor complex can be used to functionalize the surface of two Gram-negative proteobacteria, Escherichia coli and Ralstonia eutropha with CdSe/ZnS nanoparticles. This work highlights the potential for using microbe-phage interactions to generate new functions on living cells. C1 [Yeh, Yi-Chun; Mueller, Jana; Bi, Changhao; Hillson, Nathan J.; Chhabra, Swapnil R.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA 94720 USA. [Beller, Harry R.; Singer, Steven W.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, Berkeley, CA 94720 USA. RP Yeh, YC (reprint author), Natl Taiwan Normal Univ, Dept Chem, 88,Sect 4,Tingzhou Rd, Taipei 11677, Taiwan. EM yichuny@ntnu.edu.tw; swsinger@lbl.gov RI Hillson, Nathan/F-9957-2012; Beller, Harry/H-6973-2014 OI Hillson, Nathan/0000-0002-9169-3978; FU Department of Energy, Advanced Research Projects Agency-Energy Electrofuels Program [DE-0000206-1577]; Department of Energy, Office of Science, Office of Biological and Environmental Research [DEAC02-5CH11231] FX This work was funded by the Department of Energy, Advanced Research Projects Agency-Energy Electrofuels Program, contract #DE-0000206-1577. This work was performed at the Joint BioEnergy Institute in Emeryville, CA, which is funded by the Department of Energy, Office of Science, Office of Biological and Environmental Research under contract DEAC02-5CH11231 to Lawrence Berkeley National Laboratory. We thank Vivek Mutalik for providing access to the Guava easyCyte Flow cytometry. NR 18 TC 4 Z9 4 U1 1 U2 14 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1359-7345 J9 CHEM COMMUN JI Chem. Commun. PY 2013 VL 49 IS 9 BP 910 EP 912 DI 10.1039/c2cc37883c PG 3 WC Chemistry, Multidisciplinary SC Chemistry GA 062TF UT WOS:000312944700019 PM 23247551 ER PT J AU Parsell, TH Owen, BC Klein, I Jarrell, TM Marcum, CL Haupert, LJ Amundson, LM Kenttamaa, HI Ribeiro, F Miller, JT Abu-Omar, MM AF Parsell, Trenton H. Owen, Benjamin C. Klein, Ian Jarrell, Tiffany M. Marcum, Christopher L. Haupert, Laura J. Amundson, Lucas M. Kenttaemaa, Hilkka I. Ribeiro, Fabio Miller, Jeffrey T. Abu-Omar, Mahdi M. TI Cleavage and hydrodeoxygenation (HDO) of C-O bonds relevant to lignin conversion using Pd/Zn synergistic catalysis SO CHEMICAL SCIENCE LA English DT Article ID HYDROGENOLYSIS; DEPOLYMERIZATION; CHEMICALS; POLYMERS; MODEL AB The development of chemical methods for the direct catalytic conversion of biomass to high value organic molecules is an area of increasing interest. The plant matter component known as lignin is a polymer consisting of aromatic rings that could provide a means of obtaining aromatic materials currently derived solely from petroleum. This report describes a bimetallic Pd/C and Zn catalytic system that can perform selective hydrodeoxygenation (HDO) of monomeric lignin surrogates as well as successfully cleave the beta-O-4 linkages found in dimeric lignin model complexes and synthetic lignin polymers with near quantitative conversions and yields between 80-90%. The reaction with lignin polymer was highly selective affording methoxy substituted propylphenol as the major product. These reactions were performed in a Parr reactor operating at relatively mild temperature (150 degrees C) and pressure (20 bar H-2) using methanol as a solvent. Reaction products were characterized using high-pressure liquid chromatography coupled to a linear quadrupole ion trap mass spectrometer equipped with an electrospray ionization source using negative ion mode. Hydroxide ions were doped into the analyte solutions to encourage negative ion formation. This method ionizes all the mixture components to yield a single ion/analyte with no fragmentation. The catalyst is fully recyclable without the need for additional zinc. X-ray absorption spectroscopy (EXAFS) is consistent with Pd nanoparticles (4-5 nm) and no evidence of Pd-Zn alloy formation. A mechanistic hypothesis on the synergy between Pd and Zn is presented. C1 [Parsell, Trenton H.; Owen, Benjamin C.; Klein, Ian; Jarrell, Tiffany M.; Marcum, Christopher L.; Haupert, Laura J.; Amundson, Lucas M.; Kenttaemaa, Hilkka I.; Abu-Omar, Mahdi M.] Purdue Univ, Dept Chem, Brown Lab, W Lafayette, IN 47907 USA. [Parsell, Trenton H.; Owen, Benjamin C.; Klein, Ian; Jarrell, Tiffany M.; Marcum, Christopher L.; Haupert, Laura J.; Amundson, Lucas M.; Kenttaemaa, Hilkka I.; Ribeiro, Fabio; Abu-Omar, Mahdi M.] Purdue Univ, Ctr Direct Catalyt Convers Biomass Biofuels C3Bio, W Lafayette, IN 47907 USA. [Ribeiro, Fabio; Miller, Jeffrey T.] Purdue Univ, Sch Chem Engn, W Lafayette, IN 47907 USA. [Miller, Jeffrey T.] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. RP Abu-Omar, MM (reprint author), Purdue Univ, Dept Chem, Brown Lab, 560 Oval Dr, W Lafayette, IN 47907 USA. EM mabuomar@purdue.edu OI Marcum, Christopher/0000-0001-5157-8337 FU Center for Direct Catalytic Conversion of Biomass to Biofuels (C3Bio), an Energy Frontier Research Center (EFRC); U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0000997] FX This work was supported as part of the Center for Direct Catalytic Conversion of Biomass to Biofuels (C3Bio), an Energy Frontier Research Center (EFRC) funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Award Number DE-SC0000997. NR 21 TC 106 Z9 108 U1 27 U2 288 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2041-6520 J9 CHEM SCI JI Chem. Sci. PY 2013 VL 4 IS 2 BP 806 EP 813 DI 10.1039/c2sc21657d PG 8 WC Chemistry, Multidisciplinary SC Chemistry GA 062TX UT WOS:000312946500034 ER PT J AU Matthieu, DE Brusseau, ML Johnson, GR Artiola, JL Bowden, ML Curry, JE AF Matthieu, D. E., III Brusseau, M. L. Johnson, G. R. Artiola, J. L. Bowden, M. L. Curry, J. E. TI Intercalation of trichloroethene by sediment-associated clay minerals SO CHEMOSPHERE LA English DT Article DE Smectite; Montmorillonite; Clay; Sorption; X-ray diffraction ID X-RAY-DIFFRACTION; SMECTITE CLAYS; ADSORPTION; SORPTION; WATER AB The objective of this research was to examine the potential for intercalation of trichloroethene (ICE) by clay minerals associated with aquifer sediments. Sediment samples were collected from a field site in Tucson, AZ. Two widely used Montmorillonite specimen clays were employed as controls. X-ray diffraction, conducted with a controlled-environment chamber, was used to characterize smectite interlayer d-spacing for three treatments (bulk air-dry sample, sample mixed with synthetic groundwater, sample mixed with ICE-saturated synthetic groundwater). The results show that the d-spacing measured for the samples treated with TCE-saturated synthetic groundwater are larger (similar to 26%) than those of the untreated samples for all field samples as well as the specimen clays. These results indicate that TCE was intercalated by the clay minerals, which may have contributed to the extensive elution tailing observed in prior miscible-displacement experiments conducted with this sediment. (C) 2012 Elsevier Ltd. All rights reserved. C1 [Matthieu, D. E., III; Brusseau, M. L.; Artiola, J. L.; Curry, J. E.] Univ Arizona, Sch Earth & Environm Sci, Soil Water & Environm Sci Dept, Tucson, AZ 85721 USA. [Matthieu, D. E., III; Brusseau, M. L.] Univ Arizona, Hydrol & Water Resources Dept, Tucson, AZ 85721 USA. [Johnson, G. R.] Portland State Univ, Dept Civil & Environm Engn, Portland, OR 97207 USA. [Bowden, M. L.] Pacific NW Natl Lab, Environm Mol Sci Lab, Richland, WA 99352 USA. RP Brusseau, ML (reprint author), Univ Arizona, Sch Earth & Environm Sci, Soil Water & Environm Sci Dept, Tucson, AZ 85721 USA. EM brusseau@email.arizona.edu FU US DOD Strategic Environmental Research and Development Program [ER-1614]; NIEHS Superfund Research Program [ES04940]; Department of Energy's Office of Biological and Environmental Research FX This research was supported by funding provided by the US DOD Strategic Environmental Research and Development Program (ER-1614) and the NIEHS Superfund Research Program (ES04940). The XRD analysis was performed at the Environmental Molecular Science Laboratory, 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 in Richland, Washington. The authors would like to thank Dr. Mercer Meding at the Center for Environmental Physics and Mineralogy (CEPM) at the University of Arizona. NR 11 TC 7 Z9 8 U1 2 U2 28 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0045-6535 EI 1879-1298 J9 CHEMOSPHERE JI Chemosphere PD JAN PY 2013 VL 90 IS 2 BP 459 EP 463 DI 10.1016/j.chemosphere.2012.07.061 PG 5 WC Environmental Sciences SC Environmental Sciences & Ecology GA 058FA UT WOS:000312618300044 PM 22921434 ER PT J AU Wehner, MF AF Wehner, Michael F. TI Very extreme seasonal precipitation in the NARCCAP ensemble: model performance and projections SO CLIMATE DYNAMICS LA English DT Article DE Extreme precipitation; Climate models; Return value; Uncertainty; High resolution ID REGIONAL SPECTRAL MODEL; GLOBAL COUPLED MODEL; CLIMATE-CHANGE; HYDROLOGICAL CYCLE; SIMULATIONS; TEMPERATURE; INCREASES; EVENTS; UPDATE; OCEAN AB Seasonal extreme daily precipitation is analyzed in the ensemble of NARCAPP regional climate models. Significant variation in these models' abilities to reproduce observed precipitation extremes over the contiguous United States is found. Model performance metrics are introduced to characterize overall biases, seasonality, spatial extent and the shape of the precipitation distribution. Comparison of the models to gridded observations that include an elevation correction is found to be better than to gridded observations without this correction. A complicated model weighting scheme based on model performance in simulating observations is found to cause significant improvements in ensemble mean skill only if some of the models are poorly performing outliers. The effect of lateral boundary conditions are explored by comparing the integrations driven by reanalysis to those driven by global climate models. Projected mid-century future changes in seasonal precipitation means and extremes are presented and discussions of the sources of uncertainty and the mechanisms causing these changes are presented. C1 Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Wehner, MF (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, 1 Cyclotron Rd MS50F, Berkeley, CA 94720 USA. EM mfwehner@lbl.gov FU Regional and Global Climate Modeling Program; Earth System Modeling Program of the Office of Biological and Environmental Research in the Department of Energy Office of Science [DE-AC02-05CH11231]; National Science Foundation; US Department of Energy; National Oceanic and Atmospheric Administration; US Environmental Protection Agency Office of Research and Development FX This work was supported by the Regional and Global Climate Modeling Program and the Earth System Modeling Program of the Office of Biological and Environmental Research in the Department of Energy Office of Science under contract number DE-AC02-05CH11231. NCEP Reanalysis data provided by the NOAA/OAR/ESRL PSD, Boulder, Colorado, USA, from their Web site at http://www.esrl.noaa.gov/psd/. The (NARCCAP) for provided the data used in this paper through the Earth System Grid data portal at http://www.earthsystemgrid.org. NARCCAP is funded by the National Science Foundation, the US Department of Energy, the National Oceanic and Atmospheric Administration, and the US Environmental Protection Agency Office of Research and Development. CPC US Unified Precipitation data is provided by the NOAA/OAR/ESRL PSD, Boulder, Colorado, USA, from their web site at http://www.cdc.noaa.gov/. The author wishes to thank Charles Doutriaux, Peter Gleckler and Karl Taylor (Lawrence Livermore National Laboratory) with their help in producing the performance portraits and Taylor diagrams. NR 53 TC 39 Z9 39 U1 2 U2 34 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 0930-7575 J9 CLIM DYNAM JI Clim. Dyn. PD JAN PY 2013 VL 40 IS 1-2 BP 59 EP 80 DI 10.1007/s00382-012-1393-1 PG 22 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA 063WQ UT WOS:000313033100004 ER PT J AU Lansbergen, G Rahman, R Tettamanzi, GC Verduijn, J Hollenberg, LCL Klimeck, G Rogge, S AF Lansbergen, G. Rahman, R. Tettamanzi, G. C. Verduijn, J. Hollenberg, L. C. L. Klimeck, G. Rogge, S. BE Collaert, N TI Dopant Metrology in Advanced FinFETs SO CMOS NANOELECTRONICS: INNOVATIVE DEVICES, ARCHITECTURES, AND APPLICATIONS LA English DT Article; Book Chapter ID QUANTUM DOTS; SINGLE; ATOM C1 [Lansbergen, G.; Tettamanzi, G. C.; Verduijn, J.; Rogge, S.] Delft Univ Technol, Kavli Inst Nanosci, NL-2628 CJ Delft, Netherlands. [Rahman, R.] Sandia Natl Labs, Albuquerque, NM 87185 USA. [Tettamanzi, G. C.; Verduijn, J.; Rogge, S.] Univ New S Wales, CQC2T, Sydney, NSW 2052, Australia. [Hollenberg, L. C. L.] Univ Melbourne, Sch Phys, CQC2T, Melbourne, Vic 3010, Australia. [Klimeck, G.] Purdue Univ, Network Computat Nanotechnol, W Lafayette, IN 47907 USA. [Klimeck, G.] CALTECH, Jet Prop Lab, Pasadena, CA 91109 USA. RP Lansbergen, G (reprint author), Delft Univ Technol, Kavli Inst Nanosci, Lorentzweg 1, NL-2628 CJ Delft, Netherlands. EM g.tettamanzi@unsw.edu.au RI Rogge, Sven/G-3709-2010 NR 21 TC 0 Z9 0 U1 0 U2 4 PU PAN STANFORD PUBLISHING PTE LTD PI SINGAPORE PA PENTHOUSE LEVEL, SUNTEC TOWER 3, 8 TEMASEK BLVD, SINGAPORE, 038988, SINGAPORE BN 978-981-4364-03-4 PY 2013 BP 399 EP 412 D2 10.4032/9789814364034 PG 14 WC Engineering, Electrical & Electronic; Nanoscience & Nanotechnology SC Engineering; Science & Technology - Other Topics GA BDB52 UT WOS:000312484100012 ER PT J AU Banerjee, B Walsh, TF Aquino, W Bonnet, M AF Banerjee, Biswanath Walsh, Timothy F. Aquino, Wilkins Bonnet, Marc TI Large scale parameter estimation problems in frequency-domain elastodynamics using an error in constitutive equation functional SO COMPUTER METHODS IN APPLIED MECHANICS AND ENGINEERING LA English DT Article DE Error in constitutive equation; Inverse problems; Parameter estimation; Elastodynamics; Successive over-relaxation ID INVERSE PROBLEMS; IDENTIFICATION STRATEGY; RECONSTRUCTION METHOD; IMAGE-RECONSTRUCTION; ELASTOGRAPHY; ELASTICITY; ALGORITHM; MODULUS AB This paper presents the formulation and implementation of an Error in Constitutive Equations (ECE) method suitable for large-scale inverse identification of linear elastic material properties in the context of steady-state elastodynamics. In ECE-based methods, the inverse problem is postulated as an optimization problem in which the cost functional measures the discrepancy in the constitutive equations that connect kinematically admissible strains and dynamically admissible stresses. Furthermore, in a more recent modality of this methodology introduced by Feissel and Allix [17], referred to as the Modified ECE (MECE), the measured data is incorporated into the formulation as a quadratic penalty term. We show that a simple and efficient continuation scheme for the penalty term, suggested by the theory of quadratic penalty methods, can significantly accelerate the convergence of the MECE algorithm. Furthermore, a (block) successive over-relaxation (SOR) technique is introduced, enabling the use of existing parallel finite element codes with minimal modification to solve the coupled system of equations that arises from the optimality conditions in MECE methods. Our numerical results demonstrate that the proposed methodology can successfully reconstruct the spatial distribution of elastic material parameters from partial and noisy measurements in as few as ten iterations in a 20 example and fifty in a 3D example. We show (through numerical experiments) that the proposed continuation scheme can improve the rate of convergence of MECE methods by at least an order of magnitude versus the alternative of using a fixed penalty parameter. Furthermore, the proposed block SOR strategy coupled with existing parallel solvers produces a computationally efficient MECE method that can be used for large scale materials identification problems, as demonstrated on a 3D example involving about 400,000 unknown moduli. Finally, our numerical results suggest that the proposed MECE approach can be significantly faster than the conventional approach of L-2 minimization using quasi-Newton methods. (c) 2012 Elsevier B.V. All rights reserved. C1 [Banerjee, Biswanath] Cornell Univ, Sch Civil & Environm Engn, Ithaca, NY 14853 USA. [Walsh, Timothy F.] Sandia Natl Labs, Albuquerque, NM 87185 USA. [Aquino, Wilkins] Duke Univ, Dept Civil & Environm Engn, Durham, NC 27708 USA. [Bonnet, Marc] ENSTA, Dept Appl Math, POems, INRIA,CNRS,UMR 7231, Paris, France. RP Aquino, W (reprint author), Duke Univ, Dept Civil & Environm Engn, Durham, NC 27708 USA. EM bb435@cornell.edu; tfwalsh@sandia.gov; wa20@duke.edu; mbonnet@ensta.fr RI Banerjee, Biswanath/E-4591-2010 FU United States National Institute for Biomedical Imaging and Bioengineering [5R01EB002640-13]; CSAR Program at Sandia National Laboratories; United States Department of Energy [DE-AC04-94AL85000] FX The work of Biswanath Banerjee and Wilkins Aquino was partially supported by the United States National Institute for Biomedical Imaging and Bioengineering, Grant# 5R01EB002640-13. The work of Wilkins Aquino was also supported by the CSAR 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 (DE-AC04-94AL85000). NR 34 TC 26 Z9 26 U1 0 U2 7 PU ELSEVIER SCIENCE SA PI LAUSANNE PA PO BOX 564, 1001 LAUSANNE, SWITZERLAND SN 0045-7825 J9 COMPUT METHOD APPL M JI Comput. Meth. Appl. Mech. Eng. PD JAN 1 PY 2013 VL 253 BP 60 EP 72 DI 10.1016/j.cma.2012.08.023 PG 13 WC Engineering, Multidisciplinary; Mathematics, Interdisciplinary Applications; Mechanics SC Engineering; Mathematics; Mechanics GA 065FT UT WOS:000313134600005 PM 23180893 ER PT J AU Muth, DJ Bryden, KM AF Muth, D. J., Jr. Bryden, K. M. TI An integrated model for assessment of sustainable agricultural residue removal limits for bioenergy systems SO ENVIRONMENTAL MODELLING & SOFTWARE LA English DT Article DE Bioenergy; Agricultural residues; Soil erosion; Soil organic carbon; Model integration ID GREENHOUSE-GAS FLUX; CORN STOVER; SOIL QUALITY; CROPPING SYSTEMS; WATER-QUALITY; EROSION; METHODOLOGY; FRAMEWORK; DAYCENT; SUBMODEL AB Agricultural residues have been identified as a significant potential resource for bioenergy production, but serious questions remain about the sustainability of harvesting residues. Agricultural residues play an important role in limiting soil erosion from wind and water and in maintaining soil organic carbon. Because of this, multiple factors must be considered when assessing sustainable residue harvest limits. Validated and accepted modeling tools for assessing these impacts include the Revised Universal Soil Loss Equation Version 2 (RUSLE2), the Wind Erosion Prediction System (WEPS), and the Soil Conditioning Index. Currently, these models do not work together as a single integrated model. Rather, use of these models requires manual interaction and data transfer. As a result, it is currently not feasible to use these computational tools to perform detailed sustainable agricultural residue availability assessments across large spatial domains or to consider a broad range of land management practices. This paper presents an integrated modeling strategy that couples existing datasets with the RUSLE2 water erosion, WEPS wind erosion, and Soil Conditioning Index soil carbon modeling tools to create a single integrated residue removal modeling system. This enables the exploration of the detailed sustainable residue harvest scenarios needed to establish sustainable residue availability. Using this computational tool, an assessment study of residue availability for the state of Iowa was performed. This study included all soil types in the state of Iowa, four representative crop rotation schemes, variable crop yields, three tillage management methods, and five residue removal methods. The key conclusions of this study are that under current management practices and crop yields nearly 26.5 million Mg of agricultural residue are sustainably accessible in the state of Iowa, and that through the adoption of no till practices residue removal could sustainably approach 40 million Mg. However, when considering the economics and logistics of residue harvest, yields below 2.25 Mg ha(-1) are generally considered to not be viable for a commercial bioenergy system. Applying this constraint, the total agricultural residue resource available in Iowa under current management practices is 19 million Mg. Previously published results have shown residue availability from 22 million Mg to over 50 million Mg in Iowa. Published by Elsevier Ltd. C1 [Muth, D. J., Jr.] Idaho Natl Lab, Biofuels & Renewable Energy Technol Div, Idaho Falls, ID 83415 USA. [Bryden, K. M.] Iowa State Univ, Dept Mech Engn, Ames, IA 50011 USA. RP Muth, DJ (reprint author), Idaho Natl Lab, Biofuels & Renewable Energy Technol Div, POB 1625,MS 2025, Idaho Falls, ID 83415 USA. EM David.Muth@inl.gov RI Bryden, Kenneth/G-6918-2012 FU DOE's Office of Biomass Programs; Sun Grant Initiative through the Biomass Regional Feedstock Partnership; DOE [DE-AC07-05ID14517] FX The authors gratefully acknowledge Daniel Yoder and Jim Lyon at the University of Tennessee for their support with the RUSLE2 API and model integration process; Dr. Larry Wagner and Dr. John Tatarko with the USDA ARS at the Wind Erosion Research Unit in Manhattan, KS, for their support on the integration of the WEPS model; and Doug McCorkle with Ames National Laboratory for his support with VE-Suite. The authors also gratefully acknowledge the funding support from DOE's Office of Biomass Programs, as well as the significant support from all partners in the DOE Biomass Regional Feedstock Partnership Program. Professor Bryden acknowledges the funding support of the Sun Grant Initiative through the Biomass Regional Feedstock Partnership.; This submitted manuscript was authored by a contractor of the US Government under DOE Contract No. DE-AC07-05ID14517. Accordingly, the US Government and the publisher, by accepting the article for publication, acknowledges that the US Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US Government purposes. NR 83 TC 18 Z9 18 U1 2 U2 62 PU ELSEVIER SCI LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, OXON, ENGLAND SN 1364-8152 J9 ENVIRON MODELL SOFTW JI Environ. Modell. Softw. PD JAN PY 2013 VL 39 SI SI BP 50 EP 69 DI 10.1016/j.envsoft.2012.04.006 PG 20 WC Computer Science, Interdisciplinary Applications; Engineering, Environmental; Environmental Sciences SC Computer Science; Engineering; Environmental Sciences & Ecology GA 056UP UT WOS:000312517200005 ER PT J AU Rucker, DF Myers, DA Cubbage, B Levitt, MT Noonan, GE McNeill, M Henderson, C Lober, RW AF Rucker, Dale F. Myers, David A. Cubbage, Brian Levitt, Marc T. Noonan, Gillian E. McNeill, Michael Henderson, Colin Lober, Robert W. TI Surface geophysical exploration: developing noninvasive tools to monitor past leaks around Hanford's tank farms SO ENVIRONMENTAL MONITORING AND ASSESSMENT LA English DT Article DE Geophysics; Hanford; Tank farms; Characterization; Monitoring ID VADOSE ZONE; ELECTRICAL-RESISTIVITY; SITE; INVERSION; URANIUM; TOMOGRAPHY; ELECTRODES; RADIATION; MIGRATION; IMPACT AB A characterization program has been developed at Hanford to image past leaks in and around the underground storage tank facilities. The program is based on electrical resistivity, a geophysical technique that maps the distribution of electrical properties of the subsurface. The method was shown to be immediately successful in open areas devoid of underground metallic infrastructure, due to the large contrast in material properties between the highly saline waste and the dry sandy host environment. The results in these areas, confirmed by a limited number of boreholes, demonstrate a tendency for the lateral extent of the underground waste plume to remain within the approximate footprint of the disposal facility. In infrastructure-rich areas, such as tank farms, the conventional application of electrical resistivity using small point-source surface electrodes initially presented a challenge for the resistivity method. The method was then adapted to directly use the buried infrastructure, specifically the steel-cased wells that surround the tanks, as "long" electrodes for both transmission of electrical current and measurements of voltage. Overcoming the drawbacks of the long electrode method has been the focus of our work over the past 7 years. The drawbacks include low vertical resolution and limited lateral coverage. The lateral coverage issue has been improved by supplementing the long electrodes with surface electrodes in areas devoid of infrastructure. The vertical resolution has been increased by developing borehole electrode arrays that can fit within the small-diameter drive casing of a direct push rig. The evolution of the program has led to some exceptional advances in the application of geophysical methods, including logistical deployment of the technology in hazardous areas, development of parallel processing resistivity inversion algorithms, and adapting the processing tools to accommodate electrodes of all shapes and locations. The program is accompanied by a full set of quality assurance procedures that cover the layout of sensors, measurement strategies, and software enhancements while insuring the integrity of stored data. The data have been shown to be useful in identifying previously unknown contaminant sources and defining the footprint of precipitation recharge barriers to retard the movement of existing contamination. C1 [Rucker, Dale F.; Noonan, Gillian E.] HydroGEOPHYSICS Inc, Tucson, AZ 85745 USA. [Myers, David A.] Washington River Protect Solut LLC, Richland, WA USA. [Cubbage, Brian; Levitt, Marc T.; McNeill, Michael] HydroGEOPHYSICS Inc, Richland, WA USA. [Henderson, Colin] Columbia Energy & Environm Serv, Richland, WA USA. [Lober, Robert W.] US DOE, Richland, WA USA. RP Rucker, DF (reprint author), HydroGEOPHYSICS Inc, 2302 N Forbes Blvd, Tucson, AZ 85745 USA. EM druck8240@gmail.com; David_A_Dave_Myers@RL.gov; bcubbage@hgiworld.com; mlevitt@hgiworld.com; gnoonan@hgiworld.com; mmcneill@hgiworld.com; chenderson@columbia-energy.com; robert_w_lober@rl.gov OI Rucker, Dale/0000-0002-8930-2747 NR 52 TC 2 Z9 2 U1 2 U2 11 PU SPRINGER PI DORDRECHT PA VAN GODEWIJCKSTRAAT 30, 3311 GZ DORDRECHT, NETHERLANDS SN 0167-6369 J9 ENVIRON MONIT ASSESS JI Environ. Monit. Assess. PD JAN PY 2013 VL 185 IS 1 BP 995 EP 1010 DI 10.1007/s10661-012-2609-x PG 16 WC Environmental Sciences SC Environmental Sciences & Ecology GA 061GB UT WOS:000312835300079 PM 22476969 ER PT J AU Sannan, S Weydahl, T Kerstein, AR AF Sannan, Sigurd Weydahl, Torleif Kerstein, Alan R. TI Stochastic Simulation of Scalar Mixing Capturing Unsteadiness and Small-scale Structure Based on Mean-flow Properties SO FLOW TURBULENCE AND COMBUSTION LA English DT Article DE Linear Eddy Model; Turbulent mixing; Subgrid scalar closure; Turbulent reactive flows ID ONE-DIMENSIONAL TURBULENCE; PREMIXED FLAMES; TRANSPORT; COMBUSTION; REGIME; FIELDS; MODEL; JET AB A key limitation of Reynolds-Average Navier-Stokes (RANS) simulation of mixing and reaction in turbulent flows is the lack of resolution of small-scale structure and associated unsteadiness. Various subgrid models formulated in state space have been developed to complement the RANS solution in this regard. We here introduce a physical-space formulation that captures unsteady advective and diffusive processes at all scales of the turbulent flow. The approach is a 3D construction based on the Linear Eddy Model (LEM), involving three orthogonally intersecting arrays of 1D LEM domains, and coupled so as to capture the 3D character of fluid trajectories. To illustrate the model performance of the 3D LEM-based formulation, here termed LEM3D, multi-stream mixing in a turbulent round jet is simulated using measured mean-flow properties as input. Comparison to scalar cross-correlation coefficients and other measured properties of this mixing configuration indicate that the LEM3D approach, in conjunction with flow properties that are provided by steady-state models, is a useful representation of complex turbulent mixing processes that would otherwise be difficult to capture within a steady-state CFD framework. C1 [Sannan, Sigurd; Weydahl, Torleif] SINTEF Energy Res, N-7465 Trondheim, Norway. [Kerstein, Alan R.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. RP Sannan, S (reprint author), SINTEF Energy Res, N-7465 Trondheim, Norway. EM sigurd.sannan@sintef.no FU Research Council of Norway [178004/I30, 176059/I30]; Gassnova [182070]; StatoilHydro; ALSTOM; GE Global Research; Statkraft; Aker Kvaerner; Shell; TOTAL; ConocoPhillips; European Community's Seventh Framework Programme [211971]; Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, US Department of Energy; United States Department of Energy [DE-AC04-94-AL85000] FX This work forms part of the BIGCO2 project supported by the Research Council of Norway (178004/I30 and 176059/I30) and Gassnova (182070). The authors acknowledge the partners StatoilHydro, ALSTOM, GE Global Research, Statkraft, Aker Kvaerner, Shell, TOTAL, and ConocoPhillips for their support. The work has also received funding from the European Community's Seventh Framework Programme (FP7/2007-2013) under grant agreement No. 211971 (the DECARBit project).; The work was partially supported by the Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, US Department of Energy. Sandia National Laboratories is a multi-program laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the United States Department of Energy under contract DE-AC04-94-AL85000. NR 22 TC 3 Z9 3 U1 0 U2 8 PU SPRINGER PI DORDRECHT PA VAN GODEWIJCKSTRAAT 30, 3311 GZ DORDRECHT, NETHERLANDS SN 1386-6184 J9 FLOW TURBUL COMBUST JI Flow Turbul. Combust. PD JAN PY 2013 VL 90 IS 1 BP 189 EP 216 DI 10.1007/s10494-012-9436-6 PG 28 WC Thermodynamics; Mechanics SC Thermodynamics; Mechanics GA 063UO UT WOS:000313027700007 ER PT J AU Hu, TT Eisen, MB Thornton, KR Andolfatto, P AF Hu, Tina T. Eisen, Michael B. Thornton, Kevin R. Andolfatto, Peter TI A second-generation assembly of the Drosophila simulans genome provides new insights into patterns of lineage-specific divergence SO GENOME RESEARCH LA English DT Article ID EFFECTIVE POPULATION-SIZE; AMINO-ACID SUBSTITUTION; MOLECULAR EVOLUTION; NUCLEOTIDE VARIATION; MAXIMUM-LIKELIHOOD; NATURAL-SELECTION; NONCODING DNA; MELANOGASTER; POLYMORPHISM; CHROMOSOMES AB We create a new assembly of the Drosophila simulans genome using 142 million paired short-read sequences and previously published data for strain w(501). Our assembly represents a higher-quality genomic sequence with greater coverage, fewer misassemblies, and, by several indexes, fewer sequence errors. Evolutionary analysis of this genome reference sequence reveals interesting patterns of lineage-specific divergence that are different from those previously reported. Specifically, we find that Drosophila melanogaster evolves faster than D. simulans at all annotated classes of sites, including putatively neutrally evolving sites found in minimal introns. While this may be partly explained by a higher mutation rate in D. melanogaster, we also find significant heterogeneity in rates of evolution across classes of sites, consistent with historical differences in the effective population size for the two species. Also contrary to previous findings, we find that the X chromosome is evolving significantly faster than autosomes for nonsynonymous and most noncoding DNA sites and significantly slower for synonymous sites. The absence of a X/A difference for putatively neutral sites and the robustness of the pattern to Gene Ontology and sex-biased expression suggest that partly recessive beneficial mutations may comprise a substantial fraction of noncoding DNA divergence observed between species. Our results have more general implications for the interpretation of evolutionary analyses of genomes of different quality. C1 [Hu, Tina T.; Andolfatto, Peter] Princeton Univ, Dept Ecol & Evolutionary Biol, Princeton, NJ 08544 USA. [Hu, Tina T.; Andolfatto, Peter] Princeton Univ, Lewis Sigler Inst Integrat Genom, Princeton, NJ 08544 USA. [Eisen, Michael B.] Univ Calif Berkeley, Howard Hughes Med Inst, Berkeley, CA 94720 USA. [Eisen, Michael B.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Thornton, Kevin R.] Univ Calif Irvine, Dept Ecol & Evolutionary Biol, Irvine, CA 92617 USA. RP Hu, TT (reprint author), Princeton Univ, Dept Ecol & Evolutionary Biol, Princeton, NJ 08544 USA. EM tthu@princeton.edu OI Eisen, Michael/0000-0002-7528-738X FU NIH [R01-GM085183, R01-GM083228] FX We thank Molly Przeworski and David Stern for useful discussions and Ying Zhen for useful comments. We also thank Stephen Wright for use of his server to run the Velvet assembly. This work was funded in part by NIH grant R01-GM085183 to K.R.T. and R01-GM083228 to P.A. NR 53 TC 52 Z9 52 U1 1 U2 31 PU COLD SPRING HARBOR LAB PRESS, PUBLICATIONS DEPT PI COLD SPRING HARBOR PA 1 BUNGTOWN RD, COLD SPRING HARBOR, NY 11724 USA SN 1088-9051 J9 GENOME RES JI Genome Res. PD JAN PY 2013 VL 23 IS 1 BP 89 EP 98 DI 10.1101/gr.141689.112 PG 10 WC Biochemistry & Molecular Biology; Biotechnology & Applied Microbiology; Genetics & Heredity SC Biochemistry & Molecular Biology; Biotechnology & Applied Microbiology; Genetics & Heredity GA 062ZJ UT WOS:000312963400008 PM 22936249 ER PT J AU McBride, J Zhao, X Nichols, T Vagnini, V Munro, N Berry, D Jiang, Y AF McBride, J. Zhao, X. Nichols, T. Vagnini, V. Munro, N. Berry, D. Jiang, Y. TI Scalp EEG-Based Discrimination of Cognitive Deficits After Traumatic Brain Injury Using Event-Related Tsallis Entropy Analysis SO IEEE TRANSACTIONS ON BIOMEDICAL ENGINEERING LA English DT Article DE Biomedical signal processing; EEG; medical diagnosis; traumatic brain injury (TBI) ID CLOSED-HEAD INJURY; BIOPHYSICAL LINKAGE; INFORMATION; ATTENTION; INDEX; TIME; TBI; MRI AB Traumatic brain injury (TBI) is the leading cause of death and disability in children and adolescents in the U. S. This is a pilot study, which explores the discrimination of chronic TBI from normal controls using scalp EEG during a memory task. Tsallis entropies are computed for responses during an old-new memory recognition task. A support vector machinemodel is constructed to discriminate between normal andmoderate/severe TBI individuals using Tsallis entropies as features. Numerical analyses of 30 records (15 normal and 15 TBI) show amaximum discrimination accuracy of 93% (p-value = 7.8557E-5) using four features. These results suggest the potential of scalp EEG as an efficacious method for noninvasive diagnosis of TBI. C1 [McBride, J.; Zhao, X.] Univ Tennessee, Dept Mech Aerosp & Biomed Engn, Knoxville, TN 37996 USA. [Nichols, T.; Munro, N.] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. [Vagnini, V.; Jiang, Y.] Univ Kentucky, Coll Med, Dept Behav Sci, Lexington, KY 40536 USA. [Berry, D.] Univ Kentucky, Dept Psychol, Lexington, KY 40536 USA. RP Zhao, X (reprint author), Univ Tennessee, Dept Mech Aerosp & Biomed Engn, Knoxville, TN 37996 USA. EM jmcbrid4@utk.edu; xzhao9@utk.edu; nicholstl@ornl.gov; tory.vagnini@gmail.com; munronb@ornl.gov; dtrb@pop.uky.edu; yjiang@uky.edu RI Zhao, Xiaopeng/A-4419-2008 OI Zhao, Xiaopeng/0000-0003-1207-5379 FU National Science Foundation [CMMI-0845753]; Department of Behavioral Science, University of Kentucky College of Medicine FX Manuscript received May 22, 2012; revised July 20, 2012 and September 1, 2012; accepted September 23, 2012. Date of publication October 10, 2012; date of current version December 14, 2012. This work was supported in part by the National Science Foundation under Grant CMMI-0845753 and in part by a pilot grant from the Department of Behavioral Science, University of Kentucky College of Medicine. Asterisk indicates corresponding author. NR 30 TC 8 Z9 8 U1 0 U2 10 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 0018-9294 EI 1558-2531 J9 IEEE T BIO-MED ENG JI IEEE Trans. Biomed. Eng. PD JAN PY 2013 VL 60 IS 1 BP 90 EP 96 DI 10.1109/TBME.2012.2223698 PN 1 PG 7 WC Engineering, Biomedical SC Engineering GA 062CV UT WOS:000312897600012 PM 23070292 ER PT J AU McCloy, JS Korolev, K Crum, JV Afsar, MN AF McCloy, John S. Korolev, Konstantin Crum, Jarrod V. Afsar, Mohammed N. TI Millimeter-Wave Absorption as a Quality Control Tool for M-Type Hexaferrite Nanopowders SO IEEE TRANSACTIONS ON MAGNETICS LA English DT Article DE Absorbing media; ferrimagnetic materials; gyromagnetism; magnetic anisotropy; millimeter wave measurements ID COMPLEX MAGNETIC-PERMEABILITY; BARIUM FERRITE; FERROMAGNETIC-RESONANCE; SINGLE CRYSTALS; NANOPARTICLES; ANISOTROPY; PARTICLES; ABSORBER; PERMITTIVITY; FERRIMAGNETS AB Millimeter wave (MMW) absorption measurements have been conducted on commercial samples of large (micrometer-sized) and small (nanometer-sized) particles of and using a quasi-optical MMW spectrometer and a series of backwards wave oscillators encompassing the 30-120 GHz range. Effective anisotropy of the particles calculated from the resonant absorption frequency indicates lower overall anisotropy in the nano-particles. Due to their high magnetocrystalline anisotropy, both and are expected to have spin resonances in the 45-55 GHz range. Several of the sampled powders did not have MMW absorptions, so they were further investigated by DC magnetization and x-ray diffraction to assess magnetic behavior and structure. The samples with absent MMW absorption contained primarily iron oxides, suggesting that MMWabsorption could be used for quality control in hexaferrite powder manufacture. C1 [McCloy, John S.; Crum, Jarrod V.] Pacific NW Natl Lab, Richland, WA 99352 USA. [Korolev, Konstantin; Afsar, Mohammed N.] Tufts Univ, Dept Elect & Comp Engn, Medford, MA 02155 USA. [Korolev, Konstantin] Extremely High Frequency Med & Tech Assoc, Moscow 125009, Russia. RP McCloy, JS (reprint author), Pacific NW Natl Lab, Richland, WA 99352 USA. EM john.mc-cloy@pnl.gov RI Afsar, Mohammed/H-5930-2013; McCloy, John/D-3630-2013 OI McCloy, John/0000-0001-7476-7771 FU Defense Threat Reduction Agency, U.S. Department of Defense [IACRO 10-4951I]; U.S. Department of Energy by Battelle [DE-AC05-76RL01830] FX The authors would like to thank A. Goel for help with the XRD and B. Johnson for the SEM. This work was supported in part by the Defense Threat Reduction Agency, U.S. Department of Defense, IACRO 10-4951I. The Pacific Northwest National Laboratory (PNNL) is operated for the U.S. Department of Energy by Battelle under Contract DE-AC05-76RL01830. NR 42 TC 1 Z9 2 U1 3 U2 25 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 0018-9464 J9 IEEE T MAGN JI IEEE Trans. Magn. PD JAN PY 2013 VL 49 IS 1 BP 546 EP 551 DI 10.1109/TMAG.2012.2208651 PN 3 PG 6 WC Engineering, Electrical & Electronic; Physics, Applied SC Engineering; Physics GA 061FD UT WOS:000312832700011 ER PT J AU Bachovchin, KD Hoburg, JF Post, RF AF Bachovchin, Kevin D. Hoburg, James F. Post, Richard F. TI Stable Levitation of a Passive Magnetic Bearing SO IEEE TRANSACTIONS ON MAGNETICS LA English DT Article DE Halbach array stabilizer; magnetic bearings; magnetic levitation; magnetization surface charge ID FIELDS; FORCES AB A design for a passive magnetic bearing system that can stably levitate a rotor in all directions is described. The bearing system consists of levitation magnets coupled with a Halbach array stabilizer, which induces currents in stabilization coils, in order to overcome the inherent instability of a system composed only of permanent magnets. The levitation magnet system consists of two pairs of annular ring magnets which provide an upward magnetic levitation force to counteract the downward gravitational force of the rotor. The Halbach array stabilizer consists of two stabilization coils shifted in angular position with respect to one another and centered in the vertical direction between two rotating Halbach arrays. Magnetic fields from permanent magnets are calculated using superposition of fields due to patches of magnetization charge at surfaces where the magnetization is discontinuous. Induced currents in the stabilization coils are calculated by computing the time derivative of the magnetic flux through those coils. Magnetic forces on the rotor are computed using a superposition of forces on each patch of magnetization charge. The entire magnetic bearing system, consisting of both the levitation magnets and the Halbach array stabilizer, is stable to both vertical and lateral displacements. Results are compared with a simpler straightened approximation of the Halbach array stabilizer. C1 [Bachovchin, Kevin D.; Hoburg, James F.] Carnegie Mellon Univ, Dept Elect & Comp Engn, Pittsburgh, PA 15213 USA. [Post, Richard F.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. RP Bachovchin, KD (reprint author), Carnegie Mellon Univ, Dept Elect & Comp Engn, Pittsburgh, PA 15213 USA. EM kbachovc@andrew.cmu.edu FU U.S. Department of Energy, National Nuclear Security Administration [DE-AC52-07NA27344] FX Lawrence Livermore National Laboratory is operated by Lawrence Livermore National Security, LLC, for the U.S. Department of Energy, National Nuclear Security Administration under Contract DE-AC52-07NA27344. NR 14 TC 28 Z9 30 U1 4 U2 37 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 0018-9464 J9 IEEE T MAGN JI IEEE Trans. Magn. PD JAN PY 2013 VL 49 IS 1 BP 609 EP 617 DI 10.1109/TMAG.2012.2209123 PN 3 PG 9 WC Engineering, Electrical & Electronic; Physics, Applied SC Engineering; Physics GA 061FD UT WOS:000312832700020 ER PT J AU Chard, K Bubendorfer, K AF Chard, Kyle Bubendorfer, Kris TI High Performance Resource Allocation Strategies for Computational Economies SO IEEE TRANSACTIONS ON PARALLEL AND DISTRIBUTED SYSTEMS LA English DT Article DE Economic resource allocation; utility computing; cloud computing; Grid computing ID OVERBOOKING; AUCTIONS; INTERNET; MARKET; TIME AB Utility computing models have long been the focus of academic research, and with the recent success of commercial cloud providers, computation and storage is finally being realized as the fifth utility. Computational economies are often proposed as an efficient means of resource allocation, however adoption has been limited due to a lack of performance and high overheads. In this paper, we address the performance limitations of existing economic allocation models by defining strategies to reduce the failure and reallocation rate, increase occupancy and thereby increase the obtainable utilization of the system. The high-performance resource utilization strategies presented can be used by market participants without requiring dramatic changes to the allocation protocol. The strategies considered include overbooking, advanced reservation, just-in-time bidding, and using substitute providers for service delivery. The proposed strategies have been implemented in a distributed metascheduler and evaluated with respect to Grid and cloud deployments. Several diverse synthetic workloads have been used to quantity both the performance benefits and economic implications of these strategies. C1 [Chard, Kyle] Univ Chicago, Computat Inst, Chicago, IL 60637 USA. [Chard, Kyle] Argonne Natl Lab, Chicago, IL 60637 USA. [Bubendorfer, Kris] Victoria Univ Wellington, Sch Engn & Comp Sci, Wellington 6140, New Zealand. RP Chard, K (reprint author), Univ Chicago, Computat Inst, 5735 S Ellis Ave, Chicago, IL 60637 USA. EM kyle@ci.uchicago.edu; kris.bubendorfer@ecs.vuw.ac.nz NR 26 TC 12 Z9 15 U1 0 U2 25 PU IEEE COMPUTER SOC PI LOS ALAMITOS PA 10662 LOS VAQUEROS CIRCLE, PO BOX 3014, LOS ALAMITOS, CA 90720-1314 USA SN 1045-9219 J9 IEEE T PARALL DISTR JI IEEE Trans. Parallel Distrib. Syst. PD JAN PY 2013 VL 24 IS 1 BP 72 EP 84 DI 10.1109/TPDS.2012.102 PG 13 WC Computer Science, Theory & Methods; Engineering, Electrical & Electronic SC Computer Science; Engineering GA 061GV UT WOS:000312837400007 ER PT J AU Li, D de Supinski, BR Schulz, M Nikolopoulos, DS Cameron, KW AF Li, Dong de Supinski, Bronis R. Schulz, Martin Nikolopoulos, Dimitrios S. Cameron, Kirk W. TI Strategies for Energy-Efficient Resource Management of Hybrid Programming Models SO IEEE TRANSACTIONS ON PARALLEL AND DISTRIBUTED SYSTEMS LA English DT Article DE Power management; hybrid parallel programming models; dynamic concurrency throttling; dynamic voltage and frequency scaling AB Many scientific applications are programmed using hybrid programming models that use both message passing and shared memory, due to the increasing prevalence of large-scale systems with multicore, multisocket nodes. Previous work has shown that energy efficiency can be improved using software-controlled execution schemes that consider both the programming model and the power-aware execution capabilities of the system. However, such approaches have focused on identifying optimal resource utilization for one programming model, either shared memory or message passing, in isolation. The potential solution space, thus the challenge, increases substantially when optimizing hybrid models since the possible resource configurations increase exponentially. Nonetheless, with the accelerating adoption of hybrid programming models, we increasingly need improved energy efficiency in hybrid parallel applications on large-scale systems. In this work, we present new software-controlled execution schemes that consider the effects of dynamic concurrency throttling (DCT) and dynamic voltage and frequency scaling (DVFS) in the context of hybrid programming models. Specifically, we present predictive models and novel algorithms based on statistical analysis that anticipate application power and time requirements under different concurrency and frequency configurations. We apply our models and methods to the NPB MZ benchmarks and selected applications from the ASC Sequoia codes. Overall, we achieve substantial energy savings (8.74 percent on average and up to 13.8 percent) with some performance gain (up to 7.5 percent) or negligible performance loss. C1 [Li, Dong] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. [de Supinski, Bronis R.; Schulz, Martin] Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. [Nikolopoulos, Dimitrios S.] Queens Univ Belfast, Sch Elect Elect Engn & Comp Sci, Belfast BT9 5BN, Antrim, North Ireland. [Nikolopoulos, Dimitrios S.] Fdn Res & Technol Hellas, Inst Comp Sci FORTH ICS, Hellas, Greece. [Cameron, Kirk W.] Virginia Polytech Inst & State Univ, Dept Comp Sci, Blacksburg, VA 24060 USA. RP Li, D (reprint author), Oak Ridge Natl Lab, 1 Bethel Valley Rd,Bldg 5100,MS-6173, Oak Ridge, TN 37831 USA. EM lid1@ornl.gov; desupinski1@llnl.gov; schulz6@llnl.gov; dsn@ics.forth.gr; cameron@cs.vt.edu FU European Commission under the I-CORES [224759]; US National Science Foundation (NSF) [CNS-0905187, CNS-0910784, CCF-0848670, CNS-0709025, CNS-0720750]; US Department of Energy (DOE) by Lawrence Livermore National Laboratory [DEAC52-07NA27344]; U.S. Government [DE-AC05-00OR22725] FX This work has been partially supported by the European Commission under the I-CORES project (FP7 MCFIRG Contract #224759) and by the US National Science Foundation (NSF) (CNS-0905187, CNS-0910784, CCF-0848670, CNS-0709025, CNS-0720750). Portions of this work were performed under the auspices of the US Department of Energy (DOE) by Lawrence Livermore National Laboratory under Contract DEAC52-07NA27344 (LLNL-JRNL-XXXXXX). The paper has been authored, in part, by Oak Ridge National Laboratory, which is managed by UT-Battelle, LLC under Contract #DE-AC05-00OR22725 to the U.S. Government. Accordingly, the US Government retains a nonexclusive, royalty-free license to publish or reproduce the published form of this contribution, or allow others to do so, for US Government purposes. NR 28 TC 19 Z9 19 U1 0 U2 14 PU IEEE COMPUTER SOC PI LOS ALAMITOS PA 10662 LOS VAQUEROS CIRCLE, PO BOX 3014, LOS ALAMITOS, CA 90720-1314 USA SN 1045-9219 EI 1558-2183 J9 IEEE T PARALL DISTR JI IEEE Trans. Parallel Distrib. Syst. PD JAN PY 2013 VL 24 IS 1 BP 144 EP 157 DI 10.1109/TPDS.2012.95 PG 14 WC Computer Science, Theory & Methods; Engineering, Electrical & Electronic SC Computer Science; Engineering GA 061GV UT WOS:000312837400013 ER PT J AU Einstein, DR Kuprat, AP Jiao, XM Carson, JP Einstein, DM Jacob, RE Corley, RA AF Einstein, Daniel R. Kuprat, Andrew P. Jiao, Xiangmin Carson, James P. Einstein, David M. Jacob, Richard E. Corley, Richard A. TI An efficient algorithm for mapping imaging data to 3D unstructured grids in computational biomechanics SO INTERNATIONAL JOURNAL FOR NUMERICAL METHODS IN BIOMEDICAL ENGINEERING LA English DT Article DE multiscale modeling; imaging; computed tomography; MRI; histology ID MOUSE-BRAIN; LUNG; SIMULATION; RESOLUTION; AIRWAYS; MODELS; ATLAS; FLOW AB Geometries for organ scale and multiscale simulations of organ function are now routinely derived from imaging data. However, medical images may also contain spatially heterogeneous information other than geometry that are relevant to such simulations either as initial conditions or in the form of model parameters. In this manuscript, we present an algorithm for the efficient and robust mapping of such data to imaging-based unstructured polyhedral grids in parallel. We then illustrate the application of our mapping algorithm to three different mapping problems: (i) the mapping of MRI diffusion tensor data to an unstructured ventricular grid; (ii) the mapping of serial cyrosection histology data to an unstructured mouse brain grid; and (iii) the mapping of computed tomography-derived volumetric strain data to an unstructured multiscale lung grid. Execution times and parallel performance are reported for each case. Copyright (C) 2012 John Wiley & Sons, Ltd. C1 [Einstein, Daniel R.; Kuprat, Andrew P.; Carson, James P.; Jacob, Richard E.; Corley, Richard A.] Pacific NW Natl Lab, Richland, WA 99352 USA. [Jiao, Xiangmin] SUNY Stony Brook, Dept Appl Math & Stat, Stony Brook, NY 11794 USA. [Einstein, David M.] Univ Massachusetts, Lowell, MA USA. RP Einstein, DR (reprint author), Pacific NW Natl Lab, Richland, WA 99352 USA. EM daniel.einstein@pnnl.gov OI Jiao, Xiangmin/0000-0002-7111-9813; Kuprat, Andrew/0000-0003-4159-918X FU National Institutes of Health Bioengineering Research [R01-HL073598]; DOE LDRD [90001] FX We gratefully acknowledge Dr. Edward Hsu for the cardiac DTI data. We also thank Stewart J. Mosso for providing the FORTRAN 90 subroutines PLANEPOLYINT3D and VOLMPOLY3D. This work was financially supported by the National Institutes of Health Bioengineering Research Partnership Grant R01-HL073598 (Richard A. Corley, PI) and by DOE LDRD 90001 (Kerstin Kleese-Van Dam, PI). NR 35 TC 0 Z9 0 U1 1 U2 19 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 2040-7939 J9 INT J NUMER METH BIO JI Int. J. Numer. Meth. Biomed. PD JAN PY 2013 VL 29 IS 1 BP 1 EP 16 DI 10.1002/cnm.2489 PG 16 WC Engineering, Biomedical; Mathematical & Computational Biology; Mathematics, Interdisciplinary Applications SC Engineering; Mathematical & Computational Biology; Mathematics GA 065AC UT WOS:000313117500001 PM 23293066 ER PT J AU Chou, YS Stevenson, JW Choi, JP AF Chou, Yeong-Shyung Stevenson, Jeffry W. Choi, Jung-Pyung TI Evaluation of a Single Cell and Candidate Materials with High Water Content Hydrogen in a Generic Solid Oxide Fuel Cell Stack Test Fixture, Part II: Materials and Interface Characterization SO INTERNATIONAL JOURNAL OF APPLIED CERAMIC TECHNOLOGY LA English DT Article ID FERRITIC STAINLESS-STEEL; SOFC CATHODE DEGRADATION; NI-YSZ ANODE; INTERCONNECT APPLICATIONS; CHEMICAL COMPATIBILITY; CONTAINING ALLOY; SEALING GLASSES; PERFORMANCE; ELECTRODES AB A generic solid oxide fuel cell (SOFC) test fixture was developed to evaluate candidate materials under realistic operating conditions. A commercial 50 mm x 50 mm NiO-YSZ anode-supported thin YSZ electrolyte cell with lanthanum strontium manganite (LSM)/YSZ cathode was tested to evaluate the stability of candidate materials. The cell was tested in two stages at 800 degrees C: stage I with low ( 3% H2O) humidity and stage II with high ( 30% H2O) humidity hydrogen fuel in constant voltage or constant current mode. Part I of the work, published previously, provided information regarding the generic test fixture design, materials, cell performance, and optical post-mortem analysis. In part II, detailed microstructure and interfacial characterizations are reported regarding the SOFC candidate materials: (Mn,Co)-spinel conductive coating, alumina coating for sealing area, ferritic stainless steel interconnect, refractory sealing glass, and their interactions with each other. Overall, the (Mn,Co)-spinel coating was very effective in minimizing Cr migration. No Cr was identified in the cathode after 1720 h at 800 degrees C. Aluminization of metallic interconnects also proved to be chemically compatible with alkaline-earth silicate sealing glass. The details of interfacial reaction and microstructure development are discussed. C1 [Chou, Yeong-Shyung; Stevenson, Jeffry W.; Choi, Jung-Pyung] Pacific NW Natl Lab, Energy & Efficiency Div, Richland, WA 99354 USA. RP Chou, YS (reprint author), Pacific NW Natl Lab, Energy & Efficiency Div, K2-44,POB 999, Richland, WA 99354 USA. EM yeong-shyung.chou@pnl.gov FU US Department of Energy's Solid-State Energy Conversion Alliance (SECA) Core Technology Program; US Department of Energy [DE-AC06-76RLO 1830] FX The authors thank S. Carlson for SEM sample preparation, and J. Coleman for SEM analysis. This work summarized in this article was funded by the US Department of Energy's Solid-State Energy Conversion Alliance (SECA) Core Technology Program. The authors also thank Wayne Surdoval and Briggs White from NETL for helpful discussions. Pacific Northwest National Laboratory is operated by Battelle Memorial Institute for the US Department of Energy under Contract no. DE-AC06-76RLO 1830. NR 29 TC 3 Z9 3 U1 2 U2 36 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 1546-542X J9 INT J APPL CERAM TEC JI Int. J. Appl. Ceram. Technol. PD JAN-FEB PY 2013 VL 10 IS 1 BP 97 EP 106 DI 10.1111/j.1744-7402.2012.02753.x PG 10 WC Materials Science, Ceramics SC Materials Science GA 063JC UT WOS:000312992100013 ER PT J AU Portune, AR Hilton, CD AF Portune, Andrew R. Hilton, Corydon D. TI Determination of Uncertainty in Transition Velocity Estimates for Ceramic Materials SO INTERNATIONAL JOURNAL OF APPLIED CERAMIC TECHNOLOGY LA English DT Article ID INTERFACE DEFEAT; PENETRATION; PROJECTILES AB The uncertainty of transition velocity estimates made for five armor ceramic materials was quantified by applying Bayesian hypothesis testing to the McCauley Wilantewicz method. Likelihood functions of the ceramic plasticity parameter and estimated transition velocity for each material were determined through analysis of loadhardness probability spaces. Parameters of these functions were analyzed to quantify variability in expected material performance. The applied statistical methodology enabled formation of probability of penetration curves that indicated how the certainty of interface defeat varied as a function of impact velocity. Qualitative and quantitative analysis of results increases the utility of the McCauley Wilantewicz method as a screening tool for ceramic materials by providing additional information regarding the variability of expected material performance. Information revealed by this statistical approach could potentially be harnessed to drive future material development by indicating microstructural states more likely to result in desirable material behavior. C1 [Portune, Andrew R.; Hilton, Corydon D.] ORISE, Aberdeen, MD 21005 USA. RP Portune, AR (reprint author), ORISE, Aberdeen, MD 21005 USA. EM aportune@gmail.com FU U.S. Army Research Laboratory; U.S. Department of Energy; USARL FX This research was supported in part by an appointment to the Postgraduate Research Participation Program at the U.S. Army Research Laboratory administered by the Oak Ridge Institute for Science and Education through an interagency agreement between the U.S. Department of Energy and USARL. NR 11 TC 2 Z9 2 U1 0 U2 9 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 1546-542X J9 INT J APPL CERAM TEC JI Int. J. Appl. Ceram. Technol. PD JAN-FEB PY 2013 VL 10 IS 1 BP 107 EP 113 DI 10.1111/j.1744-7402.2012.02807.x PG 7 WC Materials Science, Ceramics SC Materials Science GA 063JC UT WOS:000312992100014 ER PT J AU Kobayashi, H Lorente, S Anderson, R Bejan, A AF Kobayashi, H. Lorente, S. Anderson, R. Bejan, A. TI Trees and serpentines in a conducting body SO INTERNATIONAL JOURNAL OF HEAT AND MASS TRANSFER LA English DT Article DE Constructal; Tree structure; Vascular design; Dendritic; Ground heat pump; Evolutionary design ID GROUND HEAT-EXCHANGERS; CONSTRUCTAL LAW; PUMP SYSTEMS; OPERATION; EVOLUTION; DESIGN; ENERGY; WELLS AB Here we document comparatively the performance of three flow architectures for heat transfer between a buried flow structure and a conducting medium: trees with Y-shaped bifurcations, trees with T-shaped bifurcations, and classical U-shaped and serpentine designs. The competing designs occupy the same volume fraction. The tree architectures have up to four levels of bifurcation (N). We found that the heat transfer performance depends greatly on the flow configuration. The tree shaped designs yield improvements in heat transfer density as N increases from 0 to 4. The Y-shaped design is the best of the three architectures. The scale analysis of tree-in-solid heat transfer anticipates correctly the key features of the thermal performance of the architecture. The paper also shows that the tree architecture, which is derived from minimizing flow resistance, also has the property that it distributes uniformly the flow resistance time throughout the structure. This is true for both laminar and turbulent flow. (C) 2012 Elsevier Ltd. All rights reserved. C1 [Kobayashi, H.; Bejan, A.] Duke Univ, Dept Mech Engn & Mat Sci, Durham, NC 27708 USA. [Kobayashi, H.] Ajinomoto Co Inc, R&D Planning Dept, Chuo Ku, Tokyo 1048315, Japan. [Lorente, S.] Univ Toulouse, INSA, Lab Mat & Durabil Construct, F-31077 Toulouse 04, France. [Anderson, R.] Natl Renewable Energy Lab, Golden, CO 80401 USA. RP Bejan, A (reprint author), Duke Univ, Dept Mech Engn & Mat Sci, Box 90300, Durham, NC 27708 USA. EM abejan@duke.edu FU Ajinomoto Co., Inc.; National Renewable Energy Laboratory, Golden, Colorado, USA [XXL-1-40325-01] FX We thank Ajinomoto Co., Inc. for supporting Mr. H. Kobayashi's work at Duke University. Profs. Bejan and Lorente's work was supported by a subcontract (XXL-1-40325-01) from the National Renewable Energy Laboratory, Golden, Colorado, USA. NR 23 TC 8 Z9 8 U1 0 U2 21 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0017-9310 J9 INT J HEAT MASS TRAN JI Int. J. Heat Mass Transf. PD JAN 1 PY 2013 VL 56 IS 1-2 BP 488 EP 494 DI 10.1016/j.ijheatmasstransfer.2012.09.012 PG 7 WC Thermodynamics; Engineering, Mechanical; Mechanics SC Thermodynamics; Engineering; Mechanics GA 058HR UT WOS:000312625200047 ER PT J AU Bojanowski, C Kwasniewski, L Wekezer, JW AF Bojanowski, Cezary Kwasniewski, Leslaw Wekezer, Jerry W. TI Comprehensive rollover testing of paratransit buses SO INTERNATIONAL JOURNAL OF HEAVY VEHICLE SYSTEMS LA English DT Article DE rollover test; UN-ECE Regulation 66; ECE-R66; crashworthiness; paratransit bus; finite element analysis; heavy vehicle systems AB The paper presents verification and validation procedures for the originally developed FE model of a paratransit bus, which was built for rollover test simulation. Verification of the FE model is primarily performed through analysis of the energy balance during rollover test. Series of validation experiments were designed and performed in hierarchical (multi-scale) manner. The verified and validated FE model was used to perform sensitivity analysis of the bus response to changes in material properties as well as initial conditions of the test. A measure named Deformation Index (DI) was proposed as a new quantifier of the overall deformation for easier interpretation and comparison of the rollover test results. Safety margin of the bus is estimated based on this new concept. C1 [Bojanowski, Cezary] Argonne Natl Lab, Div Energy Syst, Transportat Res & Anal Comp Ctr, Argonne, IL 60439 USA. [Kwasniewski, Leslaw] Warsaw Univ Technol, Dept Civil Engn, PL-00637 Warsaw, Poland. [Wekezer, Jerry W.] FAMU FSU Coll, Dept Civil & Environm Engn, Tallahassee, FL 32310 USA. RP Bojanowski, C (reprint author), Argonne Natl Lab, Div Energy Syst, Transportat Res & Anal Comp Ctr, 9700 S Cass Ave,Bldg 222, Argonne, IL 60439 USA. EM cbojanowski@anl.gov; l.kwasniewski@il.pw.edu.pl; jwekezer@fsu.edu FU Transit Office of FDOT; FSU Project [018679]; FDOT project [BDD 30]; Federal Transit Administration (FTA) [FL-26-7103-00, FL-26-7103-01, FL-26-7103.2009.1] FX The study reported in this paper was supported by a grant from the Transit Office of the FDOT titled: "Crashworthiness Assessment of Paratransit Buses", FSU Project No. 018679, FDOT project BDD 30. Opinions and views expressed in this paper are those of the authors and not necessarily those of the sponsoring agency. The authors would like to express their appreciation for this generous support and wish to acknowledge the assistance and support from Robert Westbrook and Erin Schepers, the Project Managers.; This work was partially supported by the Federal Transit Administration (FTA) under the Cooperative Agreements No. FL-26-7103-00 and FL-26-7103-01 (Final Report No. FL-26-7103.2009.1) with Mr. Roy Chen as a Project Manager. Computing resources were made available by the Transportation Research and Analysis Computing Center, Energy Systems Division, Argonne National Laboratory and by High Performance Computing at the Florida State University free of charge. This support is also appreciated. NR 19 TC 1 Z9 1 U1 2 U2 12 PU INDERSCIENCE ENTERPRISES LTD PI GENEVA PA WORLD TRADE CENTER BLDG, 29 ROUTE DE PRE-BOIS, CASE POSTALE 856, CH-1215 GENEVA, SWITZERLAND SN 1744-232X J9 INT J HEAVY VEH SYST JI Int. J. Heavy Veh. Syst. PY 2013 VL 20 IS 1 BP 76 EP 98 DI 10.1504/IJHVS.2013.051103 PG 23 WC Engineering, Mechanical; Transportation Science & Technology SC Engineering; Transportation GA 059PN UT WOS:000312717600005 ER PT J AU Crawford, CL Fugate, GA Cable-Dunlap, PR Wall, NA Siems, WF Hill, HH AF Crawford, Christina L. Fugate, Glenn A. Cable-Dunlap, Paula R. Wall, Nathalie A. Siems, William F. Hill, Herbert H., Jr. TI The novel analysis of uranyl compounds by electrospray-ion mobility-mass spectrometry SO INTERNATIONAL JOURNAL OF MASS SPECTROMETRY LA English DT Article DE IMS; Electrospray ionization; Uranyl; MS; Forensics ID COLLISION-INDUCED DISSOCIATION; AGENT DEGRADATION-PRODUCTS; LASER-INDUCED FLUORESCENCE; GAS-PHASE; IONIZATION; COMPLEXES; TIME; SPECIATION; EXPLOSIVES; ESI AB This study relates the first mass identification of mobility peaks associated with uranyl species. These uranyl species were introduced into the gas phase by electrospray ionization and detected by ion mobility-mass spectrometry (IM-MS) to obtain rapid chemical information from uranyl compounds. Uranyl compound analysis in nuclear forensic science is typically performed using alpha, gamma, and mass spectrometry after extensive sample preparation and purification. Although providing highly sensitive isotopic and concentration information, these methods do not provide chemical information during the initial stages of analysis. Ion mobility spectrometry, when coupled with mass spectrometry, provides chemical information, including mass-identified mobility values, for analyte identification. In this study, uranyl compounds were detected in both the positive and negative ionization modes by electrosprayion mobility-time of flight mass spectrometry (ESI-IM-TOFMS). The results showed that the sample type influenced the analyte ions that formed in the negative mode and that ESI solvent composition was the main factor that influenced analyte ion formation in the positive mode analysis. These results indicate that ESI-IM-TOFMS can be used to obtain rapid, chemical information for the initial analysis of a sample containing uranyl compounds. (c) 2012 Elsevier B.V. All rights reserved. C1 [Crawford, Christina L.; Wall, Nathalie A.; Siems, William F.; Hill, Herbert H., Jr.] Washington State Univ, Dept Chem, Pullman, WA 99164 USA. [Fugate, Glenn A.] Savannah River Natl Lab, Aiken, SC 29808 USA. [Cable-Dunlap, Paula R.] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. RP Hill, HH (reprint author), Washington State Univ, Dept Chem, POB 644630, Pullman, WA 99164 USA. EM hhhill@wsu.edu RI Fugate, Glenn/O-9752-2016 OI Fugate, Glenn/0000-0001-7100-690X FU National Nuclear Security Administration [SR-09-266-PD01] FX This work was supported by the National Nuclear Security Administration under contract SR-09-266-PD01. NR 49 TC 4 Z9 4 U1 3 U2 51 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 1387-3806 J9 INT J MASS SPECTROM JI Int. J. Mass Spectrom. PD JAN 1 PY 2013 VL 333 BP 21 EP 26 DI 10.1016/j.ijms.2012.08.004 PG 6 WC Physics, Atomic, Molecular & Chemical; Spectroscopy SC Physics; Spectroscopy GA 060EN UT WOS:000312759400004 ER PT J AU Barabash, RI AF Barabash, Rozaliya I. TI Diffraction Across the Length Scale SO JOM LA English DT Article ID RAY; MICROSCOPY C1 Oak Ridge Natl Lab, MST Div, Oak Ridge, TN 37831 USA. RP Barabash, RI (reprint author), Oak Ridge Natl Lab, MST Div, Oak Ridge, TN 37831 USA. EM barabashr@ornl.gov NR 10 TC 0 Z9 0 U1 0 U2 10 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1047-4838 J9 JOM-US JI JOM PD JAN PY 2013 VL 65 IS 1 BP 18 EP 20 DI 10.1007/s11837-012-0500-4 PG 3 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering; Mineralogy; Mining & Mineral Processing SC Materials Science; Metallurgy & Metallurgical Engineering; Mineralogy; Mining & Mineral Processing GA 064HJ UT WOS:000313064500003 ER PT J AU Yu, ZZ Barabash, R Barabash, O Liu, WJ Feng, ZL AF Yu, Zhenzhen Barabash, Rozaliya Barabash, Oleg Liu, Wenjun Feng, Zhili TI Microscopic Deformation in Individual Grains in an Advanced High-Strength Steel SO JOM LA English DT Article ID DUAL-PHASE STEELS; NI-BASED SUPERALLOY; X-RAY; BEHAVIOR; FERRITE; STRESS; DISLOCATIONS; DIFFRACTION; MARTENSITE AB In situ synchrotron microbeam x-ray diffraction experiments were carried out to study the microscopic deformation within individual ferrite grains in a martensite/ferrite dual-phase steel (DP980) under incremental tensile loading. The differential aperture x-ray microscopy technique was used to resolve the strain variations as a function of depth up to 100 mu m deep from the sample surface. The highly inhomogeneous distributions of the lattice strain, which is associated with the elastic deformation and stresses inside the grains, were determined by means of monochromatic energy diffraction, whereas insights to the plastic deformation were revealed by polychromatic energy diffraction. C1 [Yu, Zhenzhen; Barabash, Rozaliya; Feng, Zhili] Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. [Barabash, Oleg] Univ Tennessee, Knoxville, TN 37996 USA. [Liu, Wenjun] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. RP Yu, ZZ (reprint author), Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. EM fengz@ornl.gov RI Feng, Zhili/H-9382-2012 OI Feng, Zhili/0000-0001-6573-7933 FU U.S. Department of Energy (DOE), Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies as part of the Lightweight Materials Program; DOE Basic Energy Sciences, Materials Sciences and Engineering Division [DE-AC05-00OR22725]; UT-Battelle, LLC; U. S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357] FX This research was sponsored by the U.S. Department of Energy (DOE), Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies as part of the Lightweight Materials Program, and by the DOE Basic Energy Sciences, Materials Sciences and Engineering Division, under Contract DE-AC05-00OR22725 with UT-Battelle, LLC. The work benefited from the use of the Advanced Photon Source, supported by the U. S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. The authors acknowledge the assistance of Dongxiao Qiao of Oak Ridge National Laboratory in DIC data analysis and Wei Wu of the University of Tennessee in supporting the experiment. NR 20 TC 9 Z9 9 U1 0 U2 29 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1047-4838 J9 JOM-US JI JOM PD JAN PY 2013 VL 65 IS 1 BP 21 EP 28 DI 10.1007/s11837-012-0494-y PG 8 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering; Mineralogy; Mining & Mineral Processing SC Materials Science; Metallurgy & Metallurgical Engineering; Mineralogy; Mining & Mineral Processing GA 064HJ UT WOS:000313064500004 ER PT J AU McIntyre, NS Barabash, RI Qin, J Kunz, M Tamura, N Bei, H AF McIntyre, N. S. Barabash, R. I. Qin, J. Kunz, M. Tamura, N. Bei, H. TI Acquisition, Sharing, and Processing of Large Data Sets for Strain Imaging: An Example of an Indented Ni3Al/Mo Composite SO JOM LA English DT Article ID X-RAY MICRODIFFRACTION; DISLOCATIONS AB The local effects of stress from a mechanical indentation have been studied on a Ni3Al single crystal containing submicron inclusions of molybdenum fibers. X-ray microdiffraction (PXM) was used to measure elastic and plastic deformations near the indents. An analysis of freshly acquired massive sets of PXM data has been carried out over the Science Studio network using parallel processing software called FOXMAS. This network and the FOXMAS software have greatly improved the efficiency of the data processing task. The analysis was successfully applied to study lattice orientation distribution and strain tensor components for both the Ni3Al and the Mo phases, particularly around eight indents patterned at the longitudinal section of the alloy. C1 [McIntyre, N. S.; Qin, J.] Univ Western Ontario, London, ON N6A 5B7, Canada. [Barabash, R. I.; Bei, H.] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. [Kunz, M.; Tamura, N.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. RP McIntyre, NS (reprint author), Univ Western Ontario, London, ON N6A 5B7, Canada. EM smcintyr@uwo.ca OI Bei, Hongbin/0000-0003-0283-7990 FU U.S. Department of Energy, Basic Energy Sciences, Materials Sciences and Engineering Division; Network Enabled Platforms project of CANARIE; Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231] FX RB and HB were supported by the U.S. Department of Energy, Basic Energy Sciences, Materials Sciences and Engineering Division. NSM and JQ were supported by the Network Enabled Platforms project of CANARIE. 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. Mr. Nathaniel Sherry is thanked for processing assistance. NR 8 TC 1 Z9 1 U1 0 U2 19 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1047-4838 J9 JOM-US JI JOM PD JAN PY 2013 VL 65 IS 1 BP 29 EP 34 DI 10.1007/s11837-012-0496-9 PG 6 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering; Mineralogy; Mining & Mineral Processing SC Materials Science; Metallurgy & Metallurgical Engineering; Mineralogy; Mining & Mineral Processing GA 064HJ UT WOS:000313064500005 ER PT J AU Pramanick, A Wang, XL AF Pramanick, Abhijit Wang, Xun-Li TI Characterization of Magnetoelastic Coupling in Ferromagnetic Shape Memory Alloys Using Neutron Diffraction SO JOM LA English DT Article ID NI-MN-GA; FIELD-INDUCED STRAIN; NI2MNGA SINGLE-CRYSTALS; MARTENSITIC PHASE; MAGNETIC-FIELDS; TRANSFORMATION; DEFORMATION; DEPENDENCE; ACTUATORS; DYNAMICS AB Ferromagnetic shape memory alloys (FSMA) are a new class of smart materials with unique properties and applications. The shape memory properties of FSMAs are due to a strong coupling between their elastic and magnetic properties. Understanding the physical origins of magnetoelastic coupling is therefore critical for future materials development and device design. To this end, a thorough study is required of the atomistic and microscopic structural arrangements and how these structural arrangements are related to the orientation of the magnetic moments. The different characterization techniques developed recently to probe these features are reviewed. A special emphasis is placed on in situ techniques such as neutron diffraction through which the microscopic origins of the collective material behavior could be ascertained. C1 [Pramanick, Abhijit] Oak Ridge Natl Lab, Chem & Engn Mat Div, Oak Ridge, TN 37831 USA. [Wang, Xun-Li] City Univ Hong Kong, Dept Phys & Mat Sci, Kowloon, Hong Kong, Peoples R China. RP Pramanick, A (reprint author), Oak Ridge Natl Lab, Chem & Engn Mat Div, Oak Ridge, TN 37831 USA. EM pramanicka@ornl.gov RI Pramanick, Abhijit/D-9578-2011; Wang, Xun-Li/C-9636-2010 OI Pramanick, Abhijit/0000-0003-0687-4967; Wang, Xun-Li/0000-0003-4060-8777 NR 58 TC 1 Z9 1 U1 1 U2 49 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1047-4838 J9 JOM-US JI JOM PD JAN PY 2013 VL 65 IS 1 BP 54 EP 64 DI 10.1007/s11837-012-0497-8 PG 11 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering; Mineralogy; Mining & Mineral Processing SC Materials Science; Metallurgy & Metallurgical Engineering; Mineralogy; Mining & Mineral Processing GA 064HJ UT WOS:000313064500008 ER PT J AU Yu, ZZ Feng, ZL Woo, WC David, S AF Yu, Zhenzhen Feng, Zhili Woo, Wan Chuck David, Stan TI Application of In Situ Neutron Diffraction to Characterize Transient Material Behavior in Welding SO JOM LA English DT Article ID X-RAY-DIFFRACTION; HIGH-STRENGTH STEELS; RESIDUAL-STRESSES; PHASE-TRANSFORMATIONS; SYNCHROTRON DIFFRACTION; INTERNAL STRAIN; ALUMINUM-ALLOY; MG ALLOY; TEXTURE; MICROSTRUCTURE AB A fundamental understanding of the transient and nonequilibrium material behavior during welding is essential in the pursuit of process control and optimization to produce defect-free, structurally sound, and reliable welds. The deep penetration capability of neutrons into most metallic materials makes neutron diffraction a unique and powerful tool in understanding the material structures and properties. However, the inadequate neutron flux limits its application in time-resolved study of transient material behavior. This article highlights recent developments toward in situ time-resolved neutron diffraction measurement of material behavior during welding with two examples: (I) measurement of the transient temperature and thermal stresses during friction-stir welding of an aluminum alloy and (II) measurement of the solid-state phase transformation behavior of an advanced high-strength steel under thermal conditions comparable to the welding processes. These newly developed experimental approaches can be broadly applied to other welding or thermomechanical processes for time-resolved measurement of the fast-changing material state in structural metals. C1 [Yu, Zhenzhen; Feng, Zhili; David, Stan] Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. [Woo, Wan Chuck] Korea Atom Energy Res Inst, Div Neutron Sci, Taejon 305353, South Korea. RP Yu, ZZ (reprint author), Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. EM fengz@ornl.gov RI Feng, Zhili/H-9382-2012; OI Feng, Zhili/0000-0001-6573-7933; WOO, Wanchuck/0000-0003-0350-5357 FU Laboratory Directed Research and Development Program of Oak Ridge National Laboratory; Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy 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. This work benefitted from the use of the Lujan Neutron Scattering Center at Los Alamos National Laboratory, and the Spallation Neutron Source at Oak Ridge National Laboratory, both of which are sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy. The authors thank Drs. Ke An, Xun-Li Wang, and Wei Zhang of Oak Ridge National Laboratory; Drs. Bjorn Clausen, Thomas Sisneros, and Donald W. Brown of Los Alamos National Laboratory; for their support and discussions. NR 54 TC 1 Z9 1 U1 3 U2 52 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1047-4838 J9 JOM-US JI JOM PD JAN PY 2013 VL 65 IS 1 BP 65 EP 72 DI 10.1007/s11837-012-0495-x PG 8 WC Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering; Mineralogy; Mining & Mineral Processing SC Materials Science; Metallurgy & Metallurgical Engineering; Mineralogy; Mining & Mineral Processing GA 064HJ UT WOS:000313064500009 ER PT J AU Dashiff, C Suzuki-Crumly, J Kracke, B Britton, L Moreland, E AF Dashiff, Carol Suzuki-Crumly, Julie Kracke, Beverly Britton, Lacrecia Moreland, Elaine TI Cystic fibrosis-related diabetes in older adolescents: Parental support and self-management SO JOURNAL FOR SPECIALISTS IN PEDIATRIC NURSING LA English DT Article DE Adolescent; autonomy support; competence; cystic fibrosis; cystic fibrosis-related diabetes; parents; self-care; self-management ID INTRINSIC MOTIVATION; GLYCEMIC CONTROL; CHRONIC ILLNESS; AUTONOMY; CARE; CHILDREN; COMPETENCE; EPIDEMIOLOGY; CHILDHOOD; ADHERENCE AB Purpose The purpose of this study was to describe the experience of cystic fibrosis-related diabetes (CFRD), parental support of adolescent self-management, and the relationship of parental autonomy support with disease self-management. Design and Methods Semi-structured interviews and questionnaires were employed in a study conducted with 10 adolescents and their parents. Results Parents and adolescents lacked confidence to manage CFRD. Mothers' autonomy support was associated with adolescents' CFRD competence and cystic fibrosis self-care. Fathers' autonomy support was associated with mothers' reports of adolescent cystic fibrosis self-care. Practice Implications Education about CFRD management and support of adolescent autonomy in disease management is needed. C1 [Dashiff, Carol; Kracke, Beverly] Univ Alabama Birmingham, Sch Nursing, Birmingham, AL 35294 USA. [Suzuki-Crumly, Julie] Oak Ridge Associated Univ, Oak Ridge, TN USA. [Britton, Lacrecia] Childrens Hosp Alabama, Cyst Fibrosis Care Ctr, Birmingham, AL USA. [Moreland, Elaine] Univ S Carolina, Sch Med, Columbia, SC USA. RP Dashiff, C (reprint author), Univ Alabama Birmingham, Sch Nursing, Birmingham, AL 35294 USA. EM carol.dashiff@me.com FU James Gregory Fleming Cystic Fibrosis Center, University of Alabama at Birmingham FX This research was funded by a grant from the James Gregory Fleming Cystic Fibrosis Center, University of Alabama at Birmingham. NR 38 TC 3 Z9 3 U1 2 U2 20 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 1539-0136 J9 J SPEC PEDIATR NURS JI J. Spec. Pediatr. Nurs. PD JAN PY 2013 VL 18 IS 1 BP 42 EP 53 DI 10.1111/jspn.12010 PG 12 WC Nursing; Pediatrics SC Nursing; Pediatrics GA 064ZL UT WOS:000313114800006 PM 23289454 ER PT J AU Ostoja-Starzewski, M Demmie, PN Zubelewicz, A AF Ostoja-Starzewski, M. Demmie, P. N. Zubelewicz, A. TI On Thermodynamic Restrictions in Peridynamics SO JOURNAL OF APPLIED MECHANICS-TRANSACTIONS OF THE ASME LA English DT Article AB This note examines restrictions imposed by the second law of thermodynamics on peridynamics in both the bond-based and the state-based formulations. Our study was carried out in the framework of thermomechanics with internal variables. In bond-based peridynamics, there are two possible thermomechanical interpretations of the dissipation function. One interpretation only admits a thermodynamic orthogonality of Ziegler, while the other admits powerless forces within a representation theory of Edelen. The latter interpretation is admissible in state-based peridynamics. Since the dissipation function of peridynamics is set up in velocity space, a link to statistical mechanics of irreversible phenomena does not appear possible. [DOI: 10.1115/1.4006945] C1 [Ostoja-Starzewski, M.] Univ Illinois, Dept Mech Sci & Engn, Inst Condensed Matter Theory, Urbana, IL 61801 USA. [Ostoja-Starzewski, M.] Univ Illinois, Beckman Inst, Urbana, IL 61801 USA. [Demmie, P. N.] Sandia Natl Labs, Albuquerque, NM 87185 USA. [Zubelewicz, A.] Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. RP Ostoja-Starzewski, M (reprint author), Univ Illinois, Dept Mech Sci & Engn, Inst Condensed Matter Theory, Urbana, IL 61801 USA. EM martinos@illinois.edu; pndemmi@sandia.gov; alek@lanl.gov OI Ostoja-Starzewski, Martin/0000-0002-3493-363X FU United States Department of Energy [DE-AC04-94AL85000]; Sandia-Defense Threat Reduction Agency (DTRA) [HDTRA1-08-10-BRCWMD]; Los Alamos National Laboratory [129493, PBX9502]; National Science Foundation [CMMI-1030940] FX Sandia National Laboratories is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the United States Department of Energy under Contract DE-AC04-94AL85000. This research was made possible by the support from Sandia-Defense Threat Reduction Agency (DTRA) (Grant HDTRA1-08-10-BRCWMD), the Los Alamos National Laboratory (Subcontract 129493 for PBX9502), and the National Science Foundation (Grant CMMI-1030940). NR 8 TC 1 Z9 1 U1 1 U2 14 PU ASME-AMER SOC MECHANICAL ENG PI NEW YORK PA THREE PARK AVE, NEW YORK, NY 10016-5990 USA SN 0021-8936 J9 J APPL MECH-T ASME JI J. Appl. Mech.-Trans. ASME PD JAN PY 2013 VL 80 IS 1 AR 014502 DI 10.1115/1.4006945 PG 3 WC Mechanics SC Mechanics GA 063VF UT WOS:000313029400031 ER PT J AU Liliental-Weber, Z Dos Reis, R Levander, AX Yu, KM Walukiewicz, W Novikov, SV Foxon, CT AF Liliental-Weber, Z. Dos Reis, R. Levander, A. X. Yu, K. M. Walukiewicz, W. Novikov, S. V. Foxon, C. T. TI Microstructure of GaN1-xBix SO JOURNAL OF ELECTRONIC MATERIALS LA English DT Article DE Microstructure; TEM; GaNBi; highly mismatched semiconductors; absorption; bandgap ID MOLECULAR-BEAM EPITAXY; ALLOYS; GAAS1-XBIX; BISMUTH; GAP AB In this paper we describe detailed transmission electron microscopy studies of GaN1-x Bi (x) with 0.05 < x < 0.18 grown by low-temperature molecular beam epitaxy under Ga-rich conditions. Microstructural transformation from columnar growth separated by thin amorphous areas in the films with lowest Bi content (5%) to pseudo-amorphous structure with crystalline grains embedded in the amorphous matrix in the samples with higher Bi content (13% to 18%) was observed. In addition, metallic Bi segregation occurred in the samples with the highest Bi concentration. An abrupt decrease in absorption edge energy is found in samples with higher Bi content. C1 [Liliental-Weber, Z.; Dos Reis, R.; Levander, A. X.; Yu, K. M.; Walukiewicz, W.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. [Dos Reis, R.] Univ Fed Rio Grande do Sul, Inst Fis, BR-91501970 Porto Alegre, RS, Brazil. [Levander, A. X.] Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA. [Novikov, S. V.; Foxon, C. T.] Univ Nottingham, Sch Phys & Astron, Nottingham NG7 2RD, England. RP Liliental-Weber, Z (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. EM z_liliental-weber@lbl.gov RI dos Reis, Roberto/E-9486-2012; Yu, Kin Man/J-1399-2012; Foundry, Molecular/G-9968-2014; OI dos Reis, Roberto/0000-0002-6011-6078; Yu, Kin Man/0000-0003-1350-9642; Novikov, Sergei/0000-0002-3725-2565 FU Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division, of the U.S. Department of Energy [DE-AC02-05CH11231]; EPSRC [EP/I004203/1] FX This work was supported by the Director, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. The synthesis work at the University of Nottingham was undertaken with support from the EPSRC (Grant No. EP/I004203/1). The use of the facility of the National Center for Electron Microscopy of the Lawrence Berkeley National Laboratory in Berkeley, CA is highly appreciated. NR 12 TC 1 Z9 1 U1 0 U2 30 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 0361-5235 J9 J ELECTRON MATER JI J. Electron. Mater. PD JAN PY 2013 VL 42 IS 1 BP 26 EP 32 DI 10.1007/s11664-012-2323-z PG 7 WC Engineering, Electrical & Electronic; Materials Science, Multidisciplinary; Physics, Applied SC Engineering; Materials Science; Physics GA 058UN UT WOS:000312660100005 ER PT J AU Harlow, FH AF Harlow, Francis H. TI Spinoff Challenges for Computational Fluid Dynamics SO JOURNAL OF HEAT TRANSFER-TRANSACTIONS OF THE ASME LA English DT Article DE crowds of people; mob dynamics; biological evolution; origin of the universe; turbulence computations ID 2-POINT DESCRIPTION AB This paper describes extensions of computational fluid dynamics (CFD) to fields of analysis lying well beyond their current realms of application. In particular, three examples are presented. The first is to the collective behavior of mobs of people interacting with sources of danger and/or opportunity to which each individual responds by actions that depend strongly on the inducement of fear and/or excitement, depending on the intrinsic susceptibilities of the person. This behavior results in both individual activities (agent-based) and collective behaviors (crowd-based stochastic) with consequences of potentially great significance. Extensions are also described for which various other emotional developments are important to the behavior of a mob. The second example is to the processes of biological evolution, in particular to the driving forces that influence the directions of species alterations through a succession of characteristics that are tested for survivability in classical Darwinian fashion. The key to the analysis lies in the newly emerging field of epigenetics, in which numerous important experimental studies are producing astonishing results leading to major challenges to the creation of computational models of the collective fluid-like dynamics of interacting biological species. The third example explores an alternative to the Big Bang theory for describing the origin of our universe. The idea is that a parent universe exists, being composed of energy, matter, and antimatter in various forms. In some region a perturbation occurs, which locally has an excess of matter over antimatter. An enormous gravitational buildup of matter and energy in the region leads to a black hole, in which there is distortion in the fourth dimension. The result then leads to an offspring entity (universe) that becomes completely detached from the parent. To apply computational fluid dynamics to the analysis of this process requires formulations that include a major component of relevant physical representations. In all three of these examples, instabilities, fluctuations, and turbulence play major roles. These arise naturally in agent-based numerical formulations (the first and second of our examples), but are much more challenging to describe in a stochastic representation (e.g., the Navier-Stokes equations). Some promising spectral analysis extensions for stochastic formulations are included in this paper. [DOI: 10.1115/1.4007648] C1 [Harlow, Francis H.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Harlow, FH (reprint author), 1407 11th St, Los Alamos, NM 87544 USA. EM francisharlow@comcast.net NR 9 TC 0 Z9 0 U1 1 U2 13 PU ASME-AMER SOC MECHANICAL ENG PI NEW YORK PA THREE PARK AVE, NEW YORK, NY 10016-5990 USA SN 0022-1481 J9 J HEAT TRANS-T ASME JI J. Heat Transf.-Trans. ASME PD JAN PY 2013 VL 135 IS 1 AR 011001 DI 10.1115/1.4007648 PG 7 WC Thermodynamics; Engineering, Mechanical SC Thermodynamics; Engineering GA 063IW UT WOS:000312991100002 ER PT J AU Marcus, PS Asay-Davis, X Wong, MH de Pater, I AF Marcus, Philip S. Asay-Davis, Xylar Wong, Michael H. de Pater, Imke TI Jupiter's Red Oval BA: Dynamics, Color, and Relationship to Jovian Climate Change SO JOURNAL OF HEAT TRANSFER-TRANSACTIONS OF THE ASME LA English DT Article DE Jupiter; chaotic mixing; climate change; vortices; secondary circulations; zonal winds; red oval ID WHITE OVALS; GEOSTROPHIC TURBULENCE; VERTICAL STRUCTURE; THERMAL STRUCTURE; HIGH-RESOLUTION; ATMOSPHERE; SPOT; VORTICES; MODEL; FLOW AB Jupiter now has a second red spot, the Oval BA. The first red spot, the Great Red Spot (GRS), is at least 180 yr old. The Oval BA formed in 2000 was originally white, but part turned red in 2005. Unlike the Great Red Spot, the red color of the Oval BA is confined to an annulus. The Oval's horizontal velocity and shape and the elevation of the haze layer above it were unchanged between 2000 and 2006. These observations, coupled with Jupiter's rapid rotation and stratification, are shown to imply that the Oval BA's 3D properties, such as its vertical thickness, were also unchanged. Therefore, neither a change in size nor velocity caused the Oval BA to turn partially red. An atmospheric warming can account for both the timing of the color change of the Oval BA as well as the persistent confinement of its red color to an annulus. [DOI: 10.1115/1.4007666] C1 [Marcus, Philip S.] Univ Calif Berkeley, Dept Mech Engn, Berkeley, CA 94720 USA. [Asay-Davis, Xylar] Los Alamos Natl Lab, Ctr Nonlinear Studies, Los Alamos, NM 87545 USA. [de Pater, Imke] Univ Calif Berkeley, Dept Astron, Berkeley, CA 94720 USA. RP Marcus, PS (reprint author), Univ Calif Berkeley, Dept Mech Engn, Berkeley, CA 94720 USA. EM pmarcus@me.berkeley.edu; xylar@lanl.gov; mikewong@astro.berkeley.edu; imke@berkeley.edu OI Asay-Davis, Xylar/0000-0002-1990-892X FU NASA Planetary Atmospheres Program; NSF AST Program; NSF ATI Program; National Science Foundation [OCI-1053575]; NASA through Space Telescope Science Institute; NASA [NAS 5-26555]; HST Programs [GO/DD 10782, GO 11102] FX This work was supported by the NASA Planetary Atmospheres Program and by the NSF AST and ATI Programs. This work used an allocation of computer resources from the Extreme Science and Engineering Discovery Environment (XSEDE), which was supported by National Science Foundation Grant No. OCI-1053575. The observations of the Jovian clouds are associated with HST Programs GO/DD 10782 and GO 11102, with support provided by NASA through a grant from the Space Telescope Science Institute, which is operated by the Association of Universities for Research in Astronomy, Inc., under NASA Contract NAS 5-26555. We thank P. Hassanzadeh and C.-H. Jiang for help with the computer simulations. NR 67 TC 2 Z9 2 U1 1 U2 13 PU ASME PI NEW YORK PA TWO PARK AVE, NEW YORK, NY 10016-5990 USA SN 0022-1481 J9 J HEAT TRANS-T ASME JI J. Heat Transf.-Trans. ASME PD JAN PY 2013 VL 135 IS 1 AR 011007 DI 10.1115/1.4007666 PG 9 WC Thermodynamics; Engineering, Mechanical SC Thermodynamics; Engineering GA 063IW UT WOS:000312991100008 ER PT J AU Pepper, DW Wang, XL Carrington, DB AF Pepper, Darrell W. Wang, Xiuling Carrington, D. B. TI A Meshless Method for Modeling Convective Heat Transfer SO JOURNAL OF HEAT TRANSFER-TRANSACTIONS OF THE ASME LA English DT Article DE numerical heat transfer; meshless method; convection; modeling ID BACKWARD-FACING STEP; GALERKIN MLPG METHOD; NATURAL-CONVECTION; NUMERICAL-SOLUTION; SQUARE CAVITY; EQUATIONS; FLOW; ELEMENT AB A meshless method is used in a projection-based approach to solve the primitive equations for fluid flow with heat transfer. The method is easy to implement in a matlab format. Radial basis functions are used to solve two benchmark test cases: natural convection in a square enclosure and flow with forced convection over a backward facing step. The results are compared with two popular and widely used commercial codes: comsol, a finite element-based model, and fluent, a finite volume-based model. [DOI: 10.1115/1.4007650] C1 [Pepper, Darrell W.] UNLV, NCACM, Las Vegas, NV 89154 USA. [Wang, Xiuling] Purdue Univ Calumet, Dept Mech Engn, Hammond, IN 46323 USA. [Carrington, D. B.] LANL, Fluid Dynam & Solid Mech Grp T3, Los Alamos, NM 87545 USA. RP Pepper, DW (reprint author), USAF Acad, Colorado Springs, CO 80840 USA. EM darrell.pepper@unlv.edu; wangx@purduecal.edu; dcarring@lanl.gov NR 32 TC 0 Z9 0 U1 2 U2 20 PU ASME-AMER SOC MECHANICAL ENG PI NEW YORK PA THREE PARK AVE, NEW YORK, NY 10016-5990 USA SN 0022-1481 J9 J HEAT TRANS-T ASME JI J. Heat Transf.-Trans. ASME PD JAN PY 2013 VL 135 IS 1 AR 011003 DI 10.1115/1.4007650 PG 9 WC Thermodynamics; Engineering, Mechanical SC Thermodynamics; Engineering GA 063IW UT WOS:000312991100004 ER PT J AU Farkas, J Chung, DW Cha, M Copeland, J Grayeski, P Westpheling, J AF Farkas, Joel Chung, Daehwan Cha, Minseok Copeland, Jennifer Grayeski, Philip Westpheling, Janet TI Improved growth media and culture techniques for genetic analysis and assessment of biomass utilization by Caldicellulosiruptor bescii SO JOURNAL OF INDUSTRIAL MICROBIOLOGY & BIOTECHNOLOGY LA English DT Article DE Caldicellulosiruptor; Biomass utilization; Defined growth media ID THERMOPHILUM DSM 6725; NOV SP-NOV; CELLULOLYTIC BACTERIUM; HYDROGEN-PRODUCTION; PLANT BIOMASS; GEN-NOV; THERMOANAEROBIUM-ACETIGENUM; ANAEROBIC BACTERIUM; SACCHAROLYTICUS; CONVERSION AB Methods for efficient growth and manipulation of relatively uncharacterized bacteria facilitate their study and are essential for genetic manipulation. We report new growth media and culture techniques for Caldicellulosiruptor bescii, the most thermophilic cellulolytic bacterium known. A low osmolarity defined growth medium (LOD) was developed that avoids problems associated with precipitates that form in previously reported media allowing the monitoring of culture density by optical density at 680 nm (OD680) and more efficient DNA transformation by electroporation. This is a defined minimal medium and does not support growth when a carbon source is omitted, making it suitable for selection of nutritional markers as well as the study of biomass utilization by C. bescii. A low osmolarity complex growth medium (LOC) was developed that dramatically improves growth and culture viability during storage, making it a better medium for routine growth and passaging of C. bescii. Both media contain significantly lower solute concentration than previously published media, allowing for flexibility in developing more specialized media types while avoiding the issues of growth inhibition and cell lysis due to osmotic stress. Plating on LOD medium solidified by agar results in 1,000-fold greater plating efficiency than previously reported and allows the isolation of discrete colonies. These new media represent a significant advance for both genetic manipulation and the study of biomass utilization in C. bescii, and may be applied broadly across the Caldicellulosiruptor genus. C1 [Farkas, Joel; Chung, Daehwan; Cha, Minseok; Copeland, Jennifer; Grayeski, Philip; Westpheling, Janet] Univ Georgia, Dept Genet, Athens, GA 30602 USA. [Farkas, Joel; Chung, Daehwan; Cha, Minseok; Copeland, Jennifer; Grayeski, Philip; Westpheling, Janet] Oak Ridge Natl Lab, Dept Energy, BioEnergy Sci Ctr, Oak Ridge, TN USA. RP Westpheling, J (reprint author), Univ Georgia, Dept Genet, Athens, GA 30602 USA. EM janwest@uga.edu FU BioEnergy Science Center; U.S. Department of Energy Bioenergy Research Center; Office of Biological and Environmental Research in the DOE Office of Science; predoctoral Graduate Training In Genetics grant [NIH 5T32GM007103-30] FX We thank Irina Kataeva for helpful discussions during the course of this work. This work was supported by The BioEnergy Science Center supported by a U.S. Department of Energy Bioenergy Research Center supported by the Office of Biological and Environmental Research in the DOE Office of Science. JF was supported by a predoctoral Graduate Training In Genetics grant (NIH 5T32GM007103-30) to the Genetics Department of the University of Georgia. NR 30 TC 23 Z9 23 U1 5 U2 40 PU SPRINGER HEIDELBERG PI HEIDELBERG PA TIERGARTENSTRASSE 17, D-69121 HEIDELBERG, GERMANY SN 1367-5435 J9 J IND MICROBIOL BIOT JI J. Ind. Microbiol. Biotechnol. PD JAN PY 2013 VL 40 IS 1 BP 41 EP 49 DI 10.1007/s10295-012-1202-1 PG 9 WC Biotechnology & Applied Microbiology SC Biotechnology & Applied Microbiology GA 063SC UT WOS:000313019300005 PM 23149625 ER PT J AU Zhou, ZH Wang, HX Yu, P Olmstead, MM Cramer, SP AF Zhou, Zhao-Hui Wang, Hongxin Yu, Ping Olmstead, Marilyn M. Cramer, Stephen P. TI Structure and spectroscopy of a bidentate bis-homocitrate dioxo-molybdenum (VI) complex: Insights relevant to the structure and properties of the FeMo-cofactor in nitrogenase SO JOURNAL OF INORGANIC BIOCHEMISTRY LA English DT Article DE Homocitrate; FeMo-cofactor; Nitrogenase; Crystal structure ID MOFE-PROTEIN; KLEBSIELLA-PNEUMONIAE; AZOTOBACTER-VINELANDII; SUBSTRATE-BINDING; BIOSYNTHESIS; ANALOGS; ENZYME; MUTANT; CARBON; ENDOR AB Direct reaction of potassium molybdate (with natural abundance Mo or enriched with Mo-92 or Mo-100) with excess hydrolyzed homocitric acid-gamma-lactone in acidic solution resulted in the isolation of a cis-dioxo bis-homocitrato molybdenum(VI) complex, K-2[*MoO2(R,S-H(2)homocit)(2)]center dot 2H(2)O (1) (*Mo=Mo, 1; Mo-92, 2; Mo-100, 3; H(4)homocit=homocitric add-gamma-lactone center dot H2O) and K-2[MoO2(O-18-R,S-H(2)homocit)(2)]center dot 2H(2)O (4). The complex has been characterized by elemental analysis. FT-IR, solid and solution C-13 NMR, and single crystal x-ray diffraction analysis. The molybdenum atom in (1) is quasi-octahedrally coordinated by two cis oxo groups and two bidentate homocitrate ligands. The latter coordinates via its alpha-alkoxy and alpha-carboxy groups, while the beta- and gamma-carboxylic acid groups remain uncomplexed, similar to the coordination mode of homocitrate in the Mo-cofactor of nitrogenase. In the IR spectra, the Mo=O stretching modes near 900 cm(-1) show 2-3 cm(-1) red- and blue-shifts for the Mo-92-complex (2) and Mo-100-complex (3) respectively compared with the natural abundance version (1). At lower frequencies, bands at 553 and 540 cm(-1) are assigned to v(Mo-O) vibrations involving the alkoxide ligand. At higher frequencies, bands in the 1700-1730 cm(-1) region are assigned to stretching modes of protonated carboxylates. In addition, a band at 1675 cm(-1) was observed that may be analogous to a band seen at 1677 cm(-1) in nitrogenase photolysis studies. The solution behavior of (1) in D2O was probed with H-1 and C-13 NMR spectra. An obvious dissociation of homocitrate was found, even though bound to the high valent Mo(VI). This suggests the likely lability of coordinated homocitrate in the FeMo-cofactor with its lower valence Mo(IV). (C) 2012 Elsevier Inc. All rights reserved. C1 [Zhou, Zhao-Hui; Wang, Hongxin; Olmstead, Marilyn M.; Cramer, Stephen P.] Univ Calif Davis, Dept Chem, Davis, CA 95616 USA. [Zhou, Zhao-Hui; Wang, Hongxin; Cramer, Stephen P.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA 94720 USA. [Zhou, Zhao-Hui] Xiamen Univ, State Key Lab Phys Chem Solid Surfaces, Xiamen 361005, Peoples R China. [Yu, Ping] Univ Calif Davis, NMR Facil, Davis, CA 95616 USA. RP Zhou, ZH (reprint author), Univ Calif Davis, Dept Chem, Davis, CA 95616 USA. EM zhzhou@xmu.edu.cn; spjcramer@ucdavis.edu RI Zhou, ZH/G-4658-2010 FU (US) National Institute of General Medical Sciences [GM-65440]; US DOE Office of Biological and Environmental Research; National Science Foundation of China [21073150]; DOE [DE-AC02-05CH11231] FX This work was supported by (US) National Institute of General Medical Sciences (GM-65440 to SPC), US DOE Office of Biological and Environmental Research (SPC) and the National Science Foundation of China (21073150 to ZHZ). The LBNL work is under DOE contract DE-AC02-05CH11231. NR 27 TC 4 Z9 5 U1 1 U2 59 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 0162-0134 J9 J INORG BIOCHEM JI J. Inorg. Biochem. PD JAN PY 2013 VL 118 BP 100 EP 106 DI 10.1016/j.jinorgbio.2012.10.001 PG 7 WC Biochemistry & Molecular Biology; Chemistry, Inorganic & Nuclear SC Biochemistry & Molecular Biology; Chemistry GA 065JN UT WOS:000313144700013 PM 23147649 ER PT J AU Doll, C Finn, E Cantaloub, M Greenwood, L Kephart, J Kephart, RF AF Doll, Charles Finn, Erin Cantaloub, Michael Greenwood, Larry Kephart, Jeremy Kephart, Rosara F. TI Comparison of impurities in charcoal sorbents found by neutron activation analysis SO JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY LA English DT Article DE Neutron activation; NAA; Gas adsorption media; Activated carbon ID CHEMICAL ACTIVATION; CARBON AB Neutron activation of gas samples in a reactor often requires a medium to retain sufficient amounts of the gas for analysis. Charcoal is commonly used to adsorb gas and hold it for activation; however, the amount of activated sodium in the charcoal after irradiation swamps most signals of interest. Neutron activation analysis was performed on several commonly available charcoal samples in an effort to determine the activation background. The results for several elements, including the dominant sodium element, are reported. It was found that ECN charcoal had the lowest elemental background, containing sodium at 2.65 +/- A 0.05 ppm, as well as trace levels of copper and tungsten. C1 [Doll, Charles; Finn, Erin; Cantaloub, Michael; Greenwood, Larry; Kephart, Jeremy; Kephart, Rosara F.] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Doll, C (reprint author), Pacific NW Natl Lab, POB 999, Richland, WA 99352 USA. EM Charles.Doll@pnnl.gov NR 9 TC 1 Z9 1 U1 0 U2 4 PU SPRINGER PI DORDRECHT PA VAN GODEWIJCKSTRAAT 30, 3311 GZ DORDRECHT, NETHERLANDS SN 0236-5731 J9 J RADIOANAL NUCL CH JI J. Radioanal. Nucl. Chem. PD JAN PY 2013 VL 295 IS 1 BP 331 EP 334 DI 10.1007/s10967-012-2239-3 PG 4 WC Chemistry, Analytical; Chemistry, Inorganic & Nuclear; Nuclear Science & Technology SC Chemistry; Nuclear Science & Technology GA 060NE UT WOS:000312784200045 ER PT J AU Warkentin, M Hopkins, JB Badeau, R Mulichak, AM Keefe, LJ Thorne, RE AF Warkentin, Matthew Hopkins, Jesse B. Badeau, Ryan Mulichak, Anne M. Keefe, Lisa J. Thorne, Robert E. TI Global radiation damage: temperature dependence, time dependence and how to outrun it SO JOURNAL OF SYNCHROTRON RADIATION LA English DT Article; Proceedings Paper CT 7th International Workshop on X-Ray Damage to Biological Crystalline Samples CY MAR 14-16, 2012 CL ENGLAND DE protein crystallography; radiation damage; room temperature; dose rate; temperature dependence ID X-RAY CRYSTALLOGRAPHY; PROTEIN CRYSTALS; MACROMOLECULAR CRYSTALLOGRAPHY; CRYOGENIC TEMPERATURES; GLASS-TRANSITION; DIFFRACTION DATA; DATA-COLLECTION; ANGSTROM RESOLUTION; ENZYME CATALYSIS; WATER-MOLECULES AB A series of studies that provide a consistent and illuminating picture of global radiation damage to protein crystals, especially at temperatures above similar to 200 K, are described. The radiation sensitivity shows a transition near 200 K, above which it appears to be limited by solvent-coupled diffusive processes. Consistent with this interpretation, a component of global damage proceeds on timescales of several minutes at 180 K, decreasing to seconds near room temperature. As a result, data collection times of order 1 s allow up to half of global damage to be outrun at 260 K. Much larger damage reductions near room temperature should be feasible using larger dose rates delivered using microfocused beams, enabling a significant expansion of structural studies of proteins under more nearly native conditions. C1 [Warkentin, Matthew; Hopkins, Jesse B.; Badeau, Ryan; Thorne, Robert E.] Cornell Univ, Dept Phys, Ithaca, NY 14853 USA. [Mulichak, Anne M.; Keefe, Lisa J.] Argonne Natl Lab, IMCA CAT, Argonne, IL 60439 USA. RP Thorne, RE (reprint author), Cornell Univ, Dept Phys, Ithaca, NY 14853 USA. EM ret6@cornell.edu FU NCRR NIH HHS [P41 RR001646, RR-01646]; NIGMS NIH HHS [GM065981, R01 GM065981] NR 80 TC 24 Z9 24 U1 2 U2 18 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0909-0495 J9 J SYNCHROTRON RADIAT JI J. Synchrot. Radiat. PD JAN PY 2013 VL 20 BP 7 EP 13 DI 10.1107/S0909049512048303 PN 1 PG 7 WC Instruments & Instrumentation; Optics; Physics, Applied SC Instruments & Instrumentation; Optics; Physics GA 057KE UT WOS:000312561300002 PM 23254651 ER PT J AU Borek, D Dauter, Z Otwinowski, Z AF Borek, Dominika Dauter, Zbigniew Otwinowski, Zbyszek TI Identification of patterns in diffraction intensities affected by radiation exposure SO JOURNAL OF SYNCHROTRON RADIATION LA English DT Article; Proceedings Paper CT 7th International Workshop on X-Ray Damage to Biological Crystalline Samples CY MAR 14-16, 2012 CL ENGLAND DE radiation damage; matrix singular value decomposition; experimental phasing; radiolysis ID SINGULAR-VALUE DECOMPOSITION; PROTEIN CRYSTALS; MACROMOLECULAR CRYSTALS; SYNCHROTRON-RADIATION; CRYSTALLOGRAPHIC DATA; STRUCTURAL-CHANGES; ELECTRON-TRANSFER; DATA REDUCTION; X-RAYS; DAMAGE AB In an X-ray diffraction experiment, the structure of molecules and the crystal lattice changes owing to chemical reactions and physical processes induced by the absorption of X-ray photons. These structural changes alter structure factors, affecting the scaling and merging of data collected at different absorbed doses. Many crystallographic procedures rely on the analysis of consistency between symmetry-equivalent reflections, so failure to account for the drift of their intensities hinders the structure solution and the interpretation of structural results. The building of a conceptual model of radiation-induced changes in macromolecular crystals is the first step in the process of correcting for radiation-induced inconsistencies in diffraction data. Here the complexity of radiation-induced changes in real and reciprocal space is analysed using matrix singular value decomposition applied to multiple complete datasets obtained from single crystals. The model consists of a resolution-dependent decay correction and a uniform-per-unique-reflection term modelling specific radiation-induced changes. This model is typically sufficient to explain radiation-induced effects observed in diffraction intensities. This analysis will guide the parameterization of the model, enabling its use in subsequent crystallographic calculations. C1 [Borek, Dominika; Otwinowski, Zbyszek] UT SW Med Ctr Dallas, Dept Biophys, Dallas, TX 75390 USA. [Borek, Dominika; Otwinowski, Zbyszek] UT SW Med Ctr Dallas, Dept Biochem, Dallas, TX 75390 USA. [Dauter, Zbigniew] NCI, Macromol Crystallog Lab, Synchrotron Radiat Res Sect, Argonne Natl Lab,Biosci Div, Argonne, IL 60439 USA. RP Otwinowski, Z (reprint author), UT SW Med Ctr Dallas, Dept Biophys, 5323 Harry Hines Blvd, Dallas, TX 75390 USA. EM zbyszek@work.swmed.edu RI Borek, Dominika/D-2943-2011 OI Borek, Dominika/0000-0002-4321-6253 FU NIGMS NIH HHS [R01 GM053163, GM053163] NR 57 TC 8 Z9 8 U1 0 U2 10 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0909-0495 J9 J SYNCHROTRON RADIAT JI J. Synchrot. Radiat. PD JAN PY 2013 VL 20 BP 37 EP 48 DI 10.1107/S0909049512048807 PN 1 PG 12 WC Instruments & Instrumentation; Optics; Physics, Applied SC Instruments & Instrumentation; Optics; Physics GA 057KE UT WOS:000312561300005 PM 23254654 ER PT J AU Gog, T Casa, DM Said, AH Upton, MH Kim, J Kuzmenko, I Huang, XR Khachatryan, R AF Gog, Thomas Casa, Diego M. Said, Ayman H. Upton, Mary H. Kim, Jungho Kuzmenko, Ivan Huang, XianRong Khachatryan, Ruben TI Spherical analyzers and monochromators for resonant inelastic hard X-ray scattering: a compilation of crystals and reflections SO JOURNAL OF SYNCHROTRON RADIATION LA English DT Article; Proceedings Paper CT 7th International Workshop on X-Ray Damage to Biological Crystalline Samples CY MAR 14-16, 2012 CL ENGLAND DE resonant inelastic X-ray scattering (RIXS); spherical diced analyzers AB Resonant inelastic X-ray scattering (RIXS) experiments require special sets of near-backscattering spherical diced analyzers and high-resolution monochromators for every distinct absorption-edge energy and emission line. For the purpose of aiding the design and planning of efficient RIXS experiments, comprehensive lists of suitable analyzer reflections for silicon, germanium, alpha-quartz, sapphire and lithium niobate crystals were compiled for a multitude of absorption edges and emission lines. Analyzers made from lithium niobate, sapphire or alpha-quartz offer many choices of reflections with intrinsic resolutions currently unattainable from silicon or germanium. In some cases these materials offer higher intensities at comparable resolutions. While lithium niobate, sapphire or alpha-quartz analyzers are still in an early stage of development, the present compilation can serve as a computational basis for assessing expected and actual performance. With regard to high-resolution monochromators, bandpass and throughput calculations for combinations of double-crystal, high-heat-load and near-backscattering high-resolution channel-cuts were assembled. The compilation of these analyzer and monochromator data is publicly available on a website. C1 [Gog, Thomas; Casa, Diego M.; Said, Ayman H.; Upton, Mary H.; Kim, Jungho; Kuzmenko, Ivan; Huang, XianRong; Khachatryan, Ruben] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. RP Gog, T (reprint author), Argonne Natl Lab, Adv Photon Source, 9700 S Cass Ave, Argonne, IL 60439 USA. EM gog@aps.anl.gov RI Casa, Diego/F-9060-2016 NR 18 TC 16 Z9 16 U1 2 U2 39 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0909-0495 J9 J SYNCHROTRON RADIAT JI J. Synchrot. Radiat. PD JAN PY 2013 VL 20 BP 74 EP 79 DI 10.1107/S0909049512043154 PN 1 PG 6 WC Instruments & Instrumentation; Optics; Physics, Applied SC Instruments & Instrumentation; Optics; Physics GA 057KE UT WOS:000312561300009 PM 23254658 ER PT J AU Yan, HF Chu, YS AF Yan, Hanfei Chu, Yong S. TI Optimization of multilayer Laue lenses for a scanning X-ray microscope SO JOURNAL OF SYNCHROTRON RADIATION LA English DT Article; Proceedings Paper CT 7th International Workshop on X-Ray Damage to Biological Crystalline Samples CY MAR 14-16, 2012 CL ENGLAND DE X-ray; nanofocusing; multilayer Laue lens; apodization; monochromaticity ID FUEL-CELL ANODE; SUPERRESOLUTION; NANOPROBE AB Multilayer Laue lenses (MLLs) have demonstrated great capabilities for efficiently focusing hard X-rays down to the nanometer scale. Optimized use of MLLs in a scanning X-ray microscope requires careful consideration of a number of practical parameters other than resolution and efficiency in order to optimize the microscope's performance and scientific throughput. Here, relationships among the apodization effect owing to the presence of a beamstop, the monochromaticity requirement and the allowable working distance are discussed, as well as their impacts on the performance of the optics. Based on these discussions, optimal MLL schemes aiming at 10 nm resolution for a scanning X-ray microscope for the Hard X-ray Nanoprobe (HXN) beamline at National Synchrotron Light Source II are presented. C1 [Yan, Hanfei; Chu, Yong S.] Brookhaven Natl Lab, Natl Synchrotron Light Source 2, Upton, NY 11973 USA. RP Yan, HF (reprint author), Brookhaven Natl Lab, Natl Synchrotron Light Source 2, Upton, NY 11973 USA. EM hyan@bnl.gov RI Yan, Hanfei/F-7993-2011 OI Yan, Hanfei/0000-0001-6824-0367 NR 34 TC 12 Z9 12 U1 0 U2 18 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0909-0495 J9 J SYNCHROTRON RADIAT JI J. Synchrot. Radiat. PD JAN PY 2013 VL 20 BP 89 EP 97 DI 10.1107/S0909049512044883 PN 1 PG 9 WC Instruments & Instrumentation; Optics; Physics, Applied SC Instruments & Instrumentation; Optics; Physics GA 057KE UT WOS:000312561300011 PM 23254660 ER PT J AU Lee, SS Fenter, P Park, C AF Lee, Sang Soo Fenter, Paul Park, Changyong TI Optimizing a flow-through X-ray transmission cell for studies of temporal and spatial variations of ion distributions at mineral-water interfaces SO JOURNAL OF SYNCHROTRON RADIATION LA English DT Article; Proceedings Paper CT 7th International Workshop on X-Ray Damage to Biological Crystalline Samples CY MAR 14-16, 2012 CL ENGLAND DE X-ray transmission flow-through cell; X-ray reflectivity; crystal truncation rod; resonant anomalous X-ray reflectivity; muscovite; interfacial thermodynamics and kinetics ID MUSCOVITE (001)-SOLUTION INTERFACE; ATOMIC-FORCE MICROSCOPY; FULVIC-ACID; HYDRATION FORCES; 001 SURFACE; REFLECTIVITY; ADSORPTION; SCATTERING; SPECIATION; HEMATITE AB The optimization of an X-ray transmission-cell design for high-resolution X-ray reflectivity measurements of the kinetics and thermodynamics of reactions at mineral-solution interfaces is presented. The transmission cell is equipped with a liquid flow system consisting of a pair of automated syringe pumps whose relative flow rates control the composition of a solution injected into the cell with similar to 1% precision. The reflectivity measurements from the muscovite-(001)-solution interface at photon energies of 15-16.5 keV show that the cell is useful for probing interfacial ion adsorption-desorption experiments at a time scale of several seconds or slower. The time resolution is achieved with a small-volume (similar to 0.22 ml) reaction chamber to facilitate fast solution exchange. Additional reductions in reaction chamber volume will improve both the data quality by reducing X-ray absorption through the solution and the time resolution by increasing the solution exchange rate in the cell. C1 [Lee, Sang Soo; Fenter, Paul; Park, Changyong] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. RP Lee, SS (reprint author), Argonne Natl Lab, Chem Sci & Engn Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM sslee@anl.gov RI Park, Changyong/A-8544-2008 OI Park, Changyong/0000-0002-3363-5788 NR 42 TC 8 Z9 8 U1 2 U2 39 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0909-0495 J9 J SYNCHROTRON RADIAT JI J. Synchrot. Radiat. PD JAN PY 2013 VL 20 BP 125 EP 136 DI 10.1107/S0909049512041568 PN 1 PG 12 WC Instruments & Instrumentation; Optics; Physics, Applied SC Instruments & Instrumentation; Optics; Physics GA 057KE UT WOS:000312561300016 PM 23254665 ER PT J AU Xi, FC Shi, T Fan, QY Prestemon, S Wan, WS An, ZH Qiao, S AF Xi, Fuchun Shi, Tan Fan, Qingyan Prestemon, Soren Wan, Weishi An, Zhenghua Qiao, S. TI A preliminary design of a knot undulator SO JOURNAL OF SYNCHROTRON RADIATION LA English DT Article; Proceedings Paper CT 7th International Workshop on X-Ray Damage to Biological Crystalline Samples CY MAR 14-16, 2012 CL ENGLAND DE novel undulator; beam dynamics ID GLOBAL DYNAMICS; POLARIZATION CONTROL; FIGURE-8 UNDULATOR; FREQUENCY-ANALYSIS; LIGHT-SOURCE; RADIATION; SYSTEMS AB The magnetic field configuration of the previously proposed knot undulator [Qiao et al. (2009). Rev. Sci. Instrum. 80, 085108] is realised in the design of a hybridized elliptically polarized undulator, which is presented. Although the details of the field distribution are not the same as those in the theoretical proposal, it is demonstrated that the practical knot undulator could work perfectly. In order to understand the minor discrepancies of the two, mathematical formulae of the synchrotron radiation are derived based on the Fourier transform of the magnetic field. From the results of calculations by simulation program, the discrepancies could be well interpreted by the corresponding formulae. The results show the importance of optimization of the end sections of the knot undulator to suppress the on-axis heat load. Furthermore, a study of the impact of the undulator on beam dynamics of the storage ring was conducted using the Shanghai Synchrotron Radiation Facility as an example and the results show that the knot undulator has little effect on the beam. C1 [Xi, Fuchun; Shi, Tan; Fan, Qingyan; An, Zhenghua; Qiao, S.] Fudan Univ, Dept Phys, Adv Mat Lab, Shanghai 200433, Peoples R China. [Xi, Fuchun; Shi, Tan; Fan, Qingyan; An, Zhenghua; Qiao, S.] Fudan Univ, Surface Phys Lab, Natl Key Lab, Shanghai 200433, Peoples R China. [Prestemon, Soren; Wan, Weishi] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. RP Qiao, S (reprint author), Fudan Univ, Dept Phys, Adv Mat Lab, 220 Handan Rd, Shanghai 200433, Peoples R China. EM qiaoshan@fudan.edu.cn NR 19 TC 1 Z9 1 U1 1 U2 10 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0909-0495 J9 J SYNCHROTRON RADIAT JI J. Synchrot. Radiat. PD JAN PY 2013 VL 20 BP 145 EP 152 DI 10.1107/S0909049512039301 PN 1 PG 8 WC Instruments & Instrumentation; Optics; Physics, Applied SC Instruments & Instrumentation; Optics; Physics GA 057KE UT WOS:000312561300018 PM 23254667 ER PT J AU Miller, WEB Kastengren, AL AF Miller, William E. B. Kastengren, Alan L. TI Measurements of spatial variations in response of ionization chambers SO JOURNAL OF SYNCHROTRON RADIATION LA English DT Article; Proceedings Paper CT 7th International Workshop on X-Ray Damage to Biological Crystalline Samples CY MAR 14-16, 2012 CL ENGLAND DE ionization chambers; spatial variations ID SATURATION CURVES; SYNCHROTRON-RADIATION; ION RECOMBINATION; TRANSPORT AB Measurements of the spatial variations in the response of three ionization chamber (IC) designs were tested as a function of chamber bias voltage, incident X-ray flux and fill gas. Two components of spatial variation are seen. When the ionization chambers are near saturation, spatial variations exist that are tied to the chamber geometry. While the response of some chambers is relatively flat, others show significant variation across the IC. These variations appear to be inherent in the response of each IC at saturation. When the chamber is far from saturation, large spatial variations in response are present when N-2 is used as a fill gas, but not when ambient air is used as a fill gas. These appear to be tied to space charge effects. C1 [Miller, William E. B.; Kastengren, Alan L.] Argonne Natl Lab, Ctr Transportat Res, Argonne, IL 60439 USA. RP Kastengren, AL (reprint author), Argonne Natl Lab, Ctr Transportat Res, 9700 S Cass Ave, Argonne, IL 60439 USA. EM akastengren@anl.gov NR 14 TC 1 Z9 1 U1 1 U2 5 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0909-0495 J9 J SYNCHROTRON RADIAT JI J. Synchrot. Radiat. PD JAN PY 2013 VL 20 BP 160 EP 165 DI 10.1107/S0909049512041337 PN 1 PG 6 WC Instruments & Instrumentation; Optics; Physics, Applied SC Instruments & Instrumentation; Optics; Physics GA 057KE UT WOS:000312561300020 PM 23254669 ER PT J AU Kanitpanyacharoen, W Parkinson, DY De Carlo, F Marone, F Stampanoni, M Mokso, R MacDowell, A Wenk, HR AF Kanitpanyacharoen, Waruntorn Parkinson, Dilworth Y. De Carlo, Francesco Marone, Federica Stampanoni, Marco Mokso, Rajmund MacDowell, Alastair Wenk, Hans-Rudolf TI A comparative study of X-ray tomographic microscopy on shales at different synchrotron facilities: ALS, APS and SLS SO JOURNAL OF SYNCHROTRON RADIATION LA English DT Article; Proceedings Paper CT 7th International Workshop on X-Ray Damage to Biological Crystalline Samples CY MAR 14-16, 2012 CL ENGLAND DE X-ray tomographic microscopy; shale; porosity; microstructure ID ADVANCED PHOTON SOURCE; QUANTITATIVE-ANALYSIS; MICROTOMOGRAPHY SYSTEM; PREFERRED ORIENTATION; COMPUTED-TOMOGRAPHY; ELASTIC PROPERTIES; MICROSTRUCTURE; ANISOTROPY; NANOSCALE; IMAGES AB Synchrotron radiation X-ray tomographic microscopy (SRXTM) was used to characterize the three-dimensional microstructure, geometry and distribution of different phases in two shale samples obtained from the North Sea (sample N1) and the Upper Barnett Formation in Texas (sample B1). Shale is a challenging material because of its multiphase composition, small grain size, low but significant amount of porosity, as well as strong shape-and lattice-preferred orientation. The goals of this round-robin project were to (i) characterize microstructures and porosity on the micrometer scale, (ii) compare results measured at three synchrotron facilities, and (iii) identify optimal experimental conditions of high-resolution SRXTM for fine-grained materials. SRXTM data of these shales were acquired under similar conditions at the Advanced Light Source (ALS) of Lawrence Berkeley National Laboratory, USA, the Advanced Photon Source (APS) of Argonne National Laboratory, USA, and the Swiss Light Source (SLS) of the Paul Scherrer Institut, Switzerland. The data reconstruction of all datasets was handled under the same procedures in order to compare the data quality and determine phase proportions and microstructures. With a 10x objective lens the spatial resolution is approximately 2 mm. The sharpness of phase boundaries in the reconstructed data collected from the APS and SLS was comparable and slightly more refined than in the data obtained from the ALS. Important internal features, such as pyrite (high-absorbing), and low-density features, including pores, fractures and organic matter or kerogen (low-absorbing), were adequately segmented on the same basis. The average volume fractions of low-density features for sample N1 and B1 were estimated at 6.3 (6)% and 4.5 (4)%, while those of pyrite were calculated to be 5.6 (6)% and 2.0 (3)%, respectively. The discrepancy of data quality and volume fractions were mainly due to different types of optical instruments and varying technical set-ups at the ALS, APS and SLS. C1 [Kanitpanyacharoen, Waruntorn; Wenk, Hans-Rudolf] Univ Calif Berkeley, Dept Earth & Planetary Sci, Berkeley, CA 94720 USA. [Parkinson, Dilworth Y.; MacDowell, Alastair] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. [De Carlo, Francesco] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. [Marone, Federica; Stampanoni, Marco; Mokso, Rajmund] Paul Scherrer Inst, Swiss Light Source, CH-5232 Villigen, Switzerland. [Stampanoni, Marco] Univ Zurich, Inst Biomed Engn, CH-8092 Zurich, Switzerland. [Stampanoni, Marco] ETH, CH-8092 Zurich, Switzerland. RP Wenk, HR (reprint author), Univ Calif Berkeley, Dept Earth & Planetary Sci, Berkeley, CA 94720 USA. EM wenk@berkeley.edu RI Marone, Federica/J-4420-2013; mokso, rajmund/J-5557-2013; Parkinson, Dilworth/A-2974-2015; Stampanoni, Marco/J-4099-2013 OI Parkinson, Dilworth/0000-0002-1817-0716; Stampanoni, Marco/0000-0001-7486-6681 NR 49 TC 17 Z9 18 U1 3 U2 36 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0909-0495 J9 J SYNCHROTRON RADIAT JI J. Synchrot. Radiat. PD JAN PY 2013 VL 20 BP 172 EP 180 DI 10.1107/S0909049512044354 PN 1 PG 9 WC Instruments & Instrumentation; Optics; Physics, Applied SC Instruments & Instrumentation; Optics; Physics GA 057KE UT WOS:000312561300022 PM 23254671 ER PT J AU Brown, DW Almer, JD Clausen, B Mosbrucker, PL Sisneros, TA Vogel, SC AF Brown, D. W. Almer, J. D. Clausen, B. Mosbrucker, P. L. Sisneros, T. A. Vogel, S. C. TI Twinning and de-twinning in beryllium during strain path changes SO MATERIALS SCIENCE AND ENGINEERING A-STRUCTURAL MATERIALS PROPERTIES MICROSTRUCTURE AND PROCESSING LA English DT Article DE Beryllium; Twinning; Diffraction; Strain path change ID SITU NEUTRON-DIFFRACTION; AZ31 MAGNESIUM ALLOY; CLOSE-PACKED METALS; HARDENING EVOLUTION; TEXTURED MAGNESIUM; STRESS-RELAXATION; HEXAGONAL METALS; DEFORMATION; TEMPERATURE; SLIP AB Rolled beryllium samples in the form of rectangular parallelepipeds were deformed at strain rates of 0.001/s and 5/s through multiple strain paths. Samples were initially deformed in-plane nominally -0.22 in compression at a rate of 5/s to populate the microstructure with twins and then reoriented and deformed a second time either in the through-thickness direction or the other in-plane direction. The microstructure (texture and internal strain) were monitored through in-situ and ex-situ diffraction measurements using neutron diffraction on the HIPPO diffractometer at LANSCE, and high energy X-ray diffraction on the 1-ID-C beamline at the APS. Twin reversal is observed when the sample is reoriented and deformed a second time in the TT direction. The twin reversal is strain rate independent in contrast to the strong strain rate dependence observed during twinning in beryllium. Deformation twinning is also observed during secondary compression in the second in-plane direction, but from the current data set we cannot determine with certainty if these twins originate from the parent orientation or the twins formed during primary in-plane compression. As a whole, this data set creates a very demanding test for the development of polycrystalline plasticity models of deformation in hexagonal metals. (C) 2012 Elsevier B.V. All rights reserved. C1 [Brown, D. W.; Clausen, B.; Sisneros, T. A.; Vogel, S. C.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Almer, J. D.] Argonne Natl Lab, Argonne, IL 60439 USA. [Mosbrucker, P. L.] Kinectr Inc, Unit 2, Toronto, ON M8Z 5G5, Canada. RP Brown, DW (reprint author), Los Alamos Natl Lab, MS H805, Los Alamos, NM 87545 USA. EM dbrown@lanl.gov RI Lujan Center, LANL/G-4896-2012; Clausen, Bjorn/B-3618-2015; OI Clausen, Bjorn/0000-0003-3906-846X; Mosbrucker, Paula/0000-0003-0262-7117; Vogel, Sven C./0000-0003-2049-0361 FU Office of Basic Energy Sciences (DOE); DOE [DE-AC52-06NA25396]; U.S. Department of Energy, Office of Basic Energy Sciences [DE-AC02-06CH11357] FX 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). Los Alamos National Laboratory is operated by Los Alamos National Security LLC under DOE Contract DE-AC52-06NA25396. Use of the Advanced Photon Source was supported by the U.S. Department of Energy, Office of Basic Energy Sciences under Contract No. DE-AC02-06CH11357. NR 48 TC 13 Z9 15 U1 1 U2 46 PU ELSEVIER SCIENCE SA PI LAUSANNE PA PO BOX 564, 1001 LAUSANNE, SWITZERLAND SN 0921-5093 J9 MAT SCI ENG A-STRUCT JI Mater. Sci. Eng. A-Struct. Mater. Prop. Microstruct. Process. PD JAN 1 PY 2013 VL 559 BP 29 EP 39 DI 10.1016/j.msea.2012.07.087 PG 11 WC Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Science & Technology - Other Topics; Materials Science; Metallurgy & Metallurgical Engineering GA 058HB UT WOS:000312623600005 ER PT J AU Kim, JH Byun, TS Hoelzer, DT Kim, SW Lee, BH AF Kim, Jeoung Han Byun, Thak Sang Hoelzer, David T. Kim, Seong-Woong Lee, Bong Ho TI Temperature dependence of strengthening mechanisms in the nanostructured ferritic alloy 14YWT: Part I-Mechanical and microstructural observations SO MATERIALS SCIENCE AND ENGINEERING A-STRUCTURAL MATERIALS PROPERTIES MICROSTRUCTURE AND PROCESSING LA English DT Article DE Ultrafine grained microstructure; Yield phenomena; Mechanical alloying; Dislocation structure ID FRACTURE CHARACTERISTICS; STEELS; RECRYSTALLIZATION; DEFORMATION; DIFFRACTION; NUCLEATION; ENERGY AB This paper presents experimental results on the mechanical and microstructural behaviors of the nanostructured ferritic alloy 14YWT and provides discussion relevant to deformation mechanisms over a wide range of temperature. The temperature dependence of strength was investigated over a wide temperature range of -196 to 1000 degrees C. Detailed microstructural characterization before and after deformation was conducted to obtain the key information on deformation mechanisms; microstructural information before and after tensile deformation, including crystallographic texture, dislocation structures, and nanoclusters, was obtained from the focused ion beam lift-out specimens using EBSD. TEM, and APT techniques. Multiple deformation stages could be identified in the yield strength versus temperature curve. The dislocation structures in the specimens deformed at room temperature and at 900 C were found to be significantly different. EBSD results were used to elucidate changes in the crystallographic textures of the specimens before and after deformation at 900 degrees C. (C) 2012 Elsevier B.V. All rights reserved. C1 [Kim, Jeoung Han; Kim, Seong-Woong] Korea Inst Mat Sci, Special Alloys Grp, Chang Won 642831, Sangnam Dong, South Korea. [Byun, Thak Sang; Hoelzer, David T.] Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN 37831 USA. [Lee, Bong Ho] Pohang Univ Sci & Technol POSTECH, NCNT, Pohang, South Korea. RP Kim, JH (reprint author), Korea Inst Mat Sci, Special Alloys Grp, Chang Won 642831, Sangnam Dong, South Korea. EM kjh1754@kims.re.kr RI Hoelzer, David/L-1558-2016 FU Korea Institute of Materials Science; US Department of Energy, Office of Nuclear Energy [DE-AC05-00OR22725]; UT-Battelle, LLC FX This research was sponsored by the in-house research project of the Korea Institute of Materials Science. It was also sponsored by the US Department of Energy, Office of Nuclear Energy under Contract DE-AC05-00OR22725 with UT-Battelle, LLC. National Center for Nanomaterials Technology at POSTECH assisted APT work. NR 28 TC 23 Z9 23 U1 2 U2 34 PU ELSEVIER SCIENCE SA PI LAUSANNE PA PO BOX 564, 1001 LAUSANNE, SWITZERLAND SN 0921-5093 J9 MAT SCI ENG A-STRUCT JI Mater. Sci. Eng. A-Struct. Mater. Prop. Microstruct. Process. PD JAN 1 PY 2013 VL 559 BP 101 EP 110 DI 10.1016/j.msea.2012.08.042 PG 10 WC Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Science & Technology - Other Topics; Materials Science; Metallurgy & Metallurgical Engineering GA 058HB UT WOS:000312623600012 ER PT J AU Kim, JH Byun, TS Hoelzer, DT Park, CH Yeom, JT Hong, JK AF Kim, Jeoung Han Byun, Thak Sang Hoelzer, David T. Park, Chan Hee Yeom, Jong Taek Hong, Jae Keun TI Temperature dependence of strengthening mechanisms in the nanostructured ferritic alloy 14YWT: Part II-Mechanistic models and predictions SO MATERIALS SCIENCE AND ENGINEERING A-STRUCTURAL MATERIALS PROPERTIES MICROSTRUCTURE AND PROCESSING LA English DT Article DE Ultrafine grained microstructure; Modeling; Yield phenomena; Mechanical alloying; Dislocation structure ID STEELS; DISLOCATION; MICROSTRUCTURE; STRESS; DEFORMATION; CRYSTALS; BEHAVIOR; IRON; FLOW AB The temperature dependence of strengthening mechanisms in the nanocluster-strengthened 14YWT alloy was investigated to elucidate the relative significance of contributing mechanisms in different temperature ranges. This study was also aimed at providing the prediction capability of yield strength for the nanostructured ferritic alloys over a wide range of temperature. The four major strengthening mechanisms: the Peierls stress, grain boundary strengthening, direct nanocluster strengthening, and dislocation forest hardening, were taken into account in the calculation, and their roles and characteristics in different temperature ranges were extensively discussed. The results indicated that the contribution of grain boundary strengthening to total strengthening was the most significant component. Yield strength calculation was made by combining all the strengthening components and the results were compared with the experimental data. Further, the validation of the proposed approach was attempted by applying to the yield strength of other alloys. (C) 2012 Elsevier BM. All rights reserved. C1 [Kim, Jeoung Han; Park, Chan Hee; Yeom, Jong Taek; Hong, Jae Keun] Korea Inst Mat Sci, Special Alloys Grp, Chang Won 642831, Sangnamdong, South Korea. [Byun, Thak Sang; Hoelzer, David T.] Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN 37831 USA. RP Kim, JH (reprint author), Korea Inst Mat Sci, Special Alloys Grp, Chang Won 642831, Sangnamdong, South Korea. EM kjh1754@kims.re.kr RI Hoelzer, David/L-1558-2016 FU Korea Institute of Materials Science; U.S. Department of Energy, Office of Nuclear Energy [DE-AC05-00OR22725]; UT-Battelle, LLC FX This research was sponsored by the in-house research project of the Korea Institute of Materials Science. It was also sponsored by U.S. Department of Energy, Office of Nuclear Energy under Contract DE-AC05-00OR22725 with UT-Battelle, LLC. A special thanks to S.M. Woo for sincere help and support. NR 55 TC 37 Z9 37 U1 0 U2 31 PU ELSEVIER SCIENCE SA PI LAUSANNE PA PO BOX 564, 1001 LAUSANNE, SWITZERLAND SN 0921-5093 J9 MAT SCI ENG A-STRUCT JI Mater. Sci. Eng. A-Struct. Mater. Prop. Microstruct. Process. PD JAN 1 PY 2013 VL 559 BP 111 EP 118 DI 10.1016/j.msea.2012.08.041 PG 8 WC Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Science & Technology - Other Topics; Materials Science; Metallurgy & Metallurgical Engineering GA 058HB UT WOS:000312623600013 ER PT J AU Schneider, AS Kiener, D Yakacki, CM Maier, HJ Gruber, PA Tamura, N Kunz, M Minor, AM Frick, CP AF Schneider, A. S. Kiener, D. Yakacki, C. M. Maier, H. J. Gruber, P. A. Tamura, N. Kunz, M. Minor, A. M. Frick, C. P. TI Influence of bulk pre-straining on the size effect in nickel compression pillars SO MATERIALS SCIENCE AND ENGINEERING A-STRUCTURAL MATERIALS PROPERTIES MICROSTRUCTURE AND PROCESSING LA English DT Article DE Nickel; Plasticity; Dislocations; Size effect; Micropillar compression; Electron microscopy ID X-RAY MICRODIFFRACTION; SINGLE-CRYSTALS; DISLOCATION NUCLEATION; MECHANICAL-PROPERTIES; YIELD STRENGTH; MICRO-PILLARS; SMALL-SCALE; PLASTICITY; DEFORMATION; FCC AB Micro-compression tests were performed on pre-strained nickel (Ni) single crystals in order to investigate the influence of the initial dislocation arrangement on the size dependence of small-scale metal structures. A bulk Ni sample was grown using the Czochralski method and sectioned into four compression samples, which were then pre-strained to nominal strains of 5, 10, 15 and 20%. Bulk samples were then characterized using transmission electron microscopy (TEM), micro-Laue diffraction, and electron backscatter diffraction. TEM results show that a dislocation cell structure was present for all deformed samples, and Laue diffraction demonstrated that the internal strain increased with increased amount of pre-straining. Small-scale pillars with diameters from 200 nm to 5 pm were focused ion beam (FIB) machined from each of the four deformed bulk samples and further compressed via a nanoindenter equipped with a flat diamond punch. Results demonstrate that bulk pre-straining inhibits the sample size effect. For heavily pre-strained bulk samples, the deformation history does not affect the stress-strain behavior, as the pillars demonstrated elevated strength and rather low strain hardening over the whole investigated size range. In situ TEM and micro-Laue diffraction measurements of pillars confirmed little change in dislocation density during pillar compression. Thus, the dislocation cell walls created by heavy bulk pre-straining become the relevant internal material structure controlling the mechanical properties, dominating the sample size effect observed in the low dislocation density regime. (C) 2012 Elsevier B.V. All rights reserved. C1 [Schneider, A. S.] INM Leibniz Inst New Mat, D-66123 Saarbrucken, Germany. [Kiener, D.] Univ Leoben, Dept Mat Phys, A-8700 Leoben, Austria. [Yakacki, C. M.] Univ Colorado, Dept Mech Engn, Denver, CO 80217 USA. [Maier, H. J.] Univ Paderborn, Lehrstuhl Werkstoffkunde Mat Sci, D-33098 Paderborn, Germany. [Gruber, P. A.] Karlsruhe Inst Technol, Inst Appl Mat, D-76131 Karlsruhe, Germany. [Tamura, N.; Kunz, M.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. [Minor, A. M.] Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA. [Minor, A. M.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Natl Ctr Electron Microscopy, Berkeley, CA 94720 USA. [Frick, C. P.] Univ Wyoming, Dept Mech Engn, Laramie, WY 82071 USA. RP Schneider, AS (reprint author), INM Leibniz Inst New Mat, Campus D2 2, D-66123 Saarbrucken, Germany. EM Andreas.schneider@inm-gmbh.de RI Foundry, Molecular/G-9968-2014; Kiener, Daniel/B-2202-2008 OI Kiener, Daniel/0000-0003-3715-3986 FU Wyoming NASA Space Grant Consortium, NASA [NNG05G165H]; Office of Science, Office of Basic Energy Sciences, US Department of Energy [DE-AC02-05CH11231]; Austrian Science Fund (FWF) through the Erwin Schrodinger fellowship [J2834-N20] FX Special thanks to Arnold Waible from the Max Planck Institute for Intelligent Systems (formerly Max Planck Institute for Metals Research) for growing the Ni single crystal. CPF gratefully thanks Wyoming NASA Space Grant Consortium, NASA Grant no. NNG05G165H, for partial funding of this work. The in situ TEM experiments were performed at the National Center for Electron Microscopy (NCEM), Lawrence Berkeley National Laboratory (LBNL). Synchrotron experiments were conducted at the Advanced Light Source (ALS) at LBNL Both NCEM and ALS are supported by the Director, Office of Science, Office of Basic Energy Sciences, US Department of Energy under contract number DE-AC02-05CH11231. DR gratefully acknowledges financial support of the Austrian Science Fund (FWF) through the Erwin Schrodinger fellowship J2834-N20. NR 67 TC 28 Z9 28 U1 2 U2 111 PU ELSEVIER SCIENCE SA PI LAUSANNE PA PO BOX 564, 1001 LAUSANNE, SWITZERLAND SN 0921-5093 EI 1873-4936 J9 MAT SCI ENG A-STRUCT JI Mater. Sci. Eng. A-Struct. Mater. Prop. Microstruct. Process. PD JAN 1 PY 2013 VL 559 BP 147 EP 158 DI 10.1016/j.msea.2012.08.055 PG 12 WC Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Science & Technology - Other Topics; Materials Science; Metallurgy & Metallurgical Engineering GA 058HB UT WOS:000312623600018 ER PT J AU Garlea, E Bridges, RL Garlea, VO Carpenter, DA Hemphill, MA Morrell, JS AF Garlea, E. Bridges, R. L. Garlea, V. O. Carpenter, D. A. Hemphill, M. A. Morrell, J. S. TI Characterization of a grain size refinement process in cast uranium SO MATERIALS SCIENCE AND ENGINEERING A-STRUCTURAL MATERIALS PROPERTIES MICROSTRUCTURE AND PROCESSING LA English DT Article DE Cast uranium; Grain refinement; Microstructure; Twinning; Neutron diffraction; Residual strain ID SINGLE CRYSTALS; DEFORMATION; TEMPERATURE AB The refinement of coarse grains in cast uranium can lead to wrought-like properties. In this study, a beta-quenched process is coupled with a shock-loading technique and alpha-annealing to manipulate uranium's grain size and the resulting microstructures have been characterized. Neutron powder diffraction has been used to evaluate the residual strain accumulated from the thermo-mechanical treatments. Optical microscopy and electron backscattering (EBSD) in scanning electron microscopy have been employed to evaluate the grain size variation and the nature of deformation mechanisms, respectively. Large strain anisotropy at the lattice level was observed on shock-loaded specimens. The final stress relief annealing did not eliminate all the residual strain. Slip and twinning were observed optically on the shocked specimens while EBSD indicates that although {130}, {172}, and {112} deformation twins were identified, an unusual type of twinning '{1176}' < 512 > was found to be dominant. It is believed that the magnitude of energy applied favored the occurrence of the {176} twin in the polycrystalline uranium. Average grain size of cast uranium underwent a significant reduction to similar to 92 mu m at the end of the process. The overall results indicate the shock-loading approach as a promising step toward controlling cast uranium grain size and thus its mechanical properties. (C) 2012 Elsevier B.V. All rights reserved. C1 [Garlea, E.; Bridges, R. L.; Carpenter, D. A.; Morrell, J. S.] Dept Dev, Oak Ridge, TN USA. [Garlea, V. O.] Oak Ridge Natl Lab, Neutron Scattering Sci Div, Oak Ridge, TN USA. [Hemphill, M. A.] Univ Tennessee, Dept Mat Sci & Engn, Knoxville, TN 37996 USA. RP Garlea, E (reprint author), Dept Dev, Y-12 Natl Secur Complex, Oak Ridge, TN USA. EM garleae@y12.doe.gov RI Garlea, Vasile/A-4994-2016 OI Garlea, Vasile/0000-0002-5322-7271 FU Y-12 National Security Complex's Plant Directed Research and Development program; US Department of Energy, Office of Basic Energy Sciences, Scientific User Facilities Division; US Government [DE-AC0500OR-22800] FX Funding for this research was provided by the Y-12 National Security Complex's Plant Directed Research and Development program. The work at Oak Ridge National Laboratory's High Flux Isotope Reactor was sponsored by the US Department of Energy, Office of Basic Energy Sciences, Scientific User Facilities Division. E.G. would like to thank Dr. J.H. Leckey and Mr. R.M. Landis, at Y-12, for reviewing the manuscript and providing valuable suggestions.; Copyright notice: The submitted manuscript has been authored by a subcontractor of the US Government under contract DE-AC0500OR-22800. Accordingly, the US Government retains a paid-up, nonexclusive, irrevocable, worldwide license to publish or reproduce the published form of this contribution, prepare derivative works, distribute copies to the public, and perform publicly and display publicly, or allow others to do so, for US Government purposes. NR 29 TC 4 Z9 4 U1 1 U2 21 PU ELSEVIER SCIENCE SA PI LAUSANNE PA PO BOX 564, 1001 LAUSANNE, SWITZERLAND SN 0921-5093 J9 MAT SCI ENG A-STRUCT JI Mater. Sci. Eng. A-Struct. Mater. Prop. Microstruct. Process. PD JAN 1 PY 2013 VL 559 BP 210 EP 216 DI 10.1016/j.msea.2012.08.082 PG 7 WC Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Science & Technology - Other Topics; Materials Science; Metallurgy & Metallurgical Engineering GA 058HB UT WOS:000312623600026 ER PT J AU McRae, R Lai, B Fahrni, CJ AF McRae, Reagan Lai, Barry Fahrni, Christoph J. TI Subcellular redistribution and mitotic inheritance of transition metals in proliferating mouse fibroblast cells SO METALLOMICS LA English DT Article ID X-RAY-FLUORESCENCE; LABILE INTRACELLULAR ZINC; THYMIDINE KINASE-ACTIVITY; SUPPRESSES TUMOR-GROWTH; STIMULATES PROLIFERATION; EXTRACELLULAR ZINC; COPPER DEFICIENCY; MICROSCOPY; ANGIOGENESIS; CANCER AB Synchrotron X-ray fluorescence microscopy of non-synchronized NIH 3T3 fibroblasts revealed an intriguing redistribution dynamics that defines the inheritance of trace metals during mitosis. At metaphase, the highest density areas of Zn and Cu are localized in two distinct regions adjacent to the metaphase plate. As the sister chromatids are pulled towards the spindle poles during anaphase, Zn and Cu gradually move to the center and partition into the daughter cells to yield a pair of twin pools during cytokinesis. Colocalization analyses demonstrated high spatial correlations between Zn, Cu, and S throughout all mitotic stages, while Fe showed consistently different topographies characterized by high-density spots distributed across the entire cell. Whereas the total amount of Cu remained similar compared to interphase cells, mitotic Zn levels increased almost 3-fold, suggesting a prominent physiological role that lies beyond the requirement of Zn as a cofactor in metalloproteins or messenger in signaling pathways. C1 [McRae, Reagan; Fahrni, Christoph J.] Georgia Inst Technol, Sch Chem & Biochem, Petit Inst Bioengn & Biosci, Atlanta, GA 30332 USA. [Lai, Barry] Argonne Natl Lab, Adv Photon Source, Xray Sci Div, Argonne, IL 60439 USA. RP Fahrni, CJ (reprint author), Georgia Inst Technol, Sch Chem & Biochem, Petit Inst Bioengn & Biosci, 901 Atlantic Dr, Atlanta, GA 30332 USA. EM blai@aps.anl.gov; fahrni@chemistry.gatech.edu FU National Institutes of Health [GM067169]; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357] FX We thank Stefan Vogt (Argonne National Laboratory) for providing support with the MAPS software. Financial support from the National Institutes of Health (GM067169) is gratefully acknowledged. 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 90 TC 15 Z9 15 U1 4 U2 39 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1756-5901 J9 METALLOMICS JI Metallomics PY 2013 VL 5 IS 1 BP 52 EP 61 DI 10.1039/c2mt20176c PG 10 WC Biochemistry & Molecular Biology SC Biochemistry & Molecular Biology GA 058UG UT WOS:000312659400005 PM 23212029 ER PT J AU Allen, FI Ercius, P Modestino, MA Segalman, RA Balsara, NP Minor, AM AF Allen, Frances I. Ercius, Peter Modestino, Miguel A. Segalman, Rachel A. Balsara, Nitash P. Minor, Andrew M. TI Deciphering the three-dimensional morphology of free-standing block copolymer thin films by transmission electron microscopy SO MICRON LA English DT Review DE Electron tomography; Energy-filtered TEM; Block copolymer morphology; PS-b-PEO thin films; Salt doping; Casting solvent ID TRIBLOCK COPOLYMERS; PHASE-BEHAVIOR; DIFFUSION; POLYMERS AB Block copolymer thin films with distinct morphologies are prepared by spin casting a nominally lamellar assay of poly(styrene-block-ethylene oxide) from a variety of solvents with and without salt doping. The 3-D morphologies of free-standing thin-film regions, which are obtained by casting directly onto holey substrates, are investigated in detail using various energy-filtering transmission electron microscopy techniques and by electron tomography. Surface characterization is achieved by atomic force microscopy. Our results demonstrate that in order to fully characterize the unique 3-D morphologies of the block copolymer thin films, a multi-method approach is required. When casting from a binary solvent, an unexpected layered honeycomb-type morphology is revealed, which likely results from an expansion of the poly(ethylene oxide) phase. A dramatic effect of selective cation coordination on the morphology of the as-cast block copolymer films is also directly observed. Published by Elsevier Ltd. C1 [Allen, Frances I.; Ercius, Peter; Minor, Andrew M.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Natl Ctr Electron Microscopy, Berkeley, CA 94720 USA. [Allen, Frances I.; Minor, Andrew M.] Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA. [Modestino, Miguel A.; Segalman, Rachel A.; Balsara, Nitash P.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. [Modestino, Miguel A.; Segalman, Rachel A.; Balsara, Nitash P.] Univ Calif Berkeley, Dept Chem & Biomol Engn, Berkeley, CA 94720 USA. RP Allen, FI (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Natl Ctr Electron Microscopy, Berkeley, CA 94720 USA. EM FIAllen@lbl.gov RI Foundry, Molecular/G-9968-2014; OI Segalman, Rachel/0000-0002-4292-5103 FU Electron Microscopy of Soft Matter Program; Office of Science, Office of Basic Energy Sciences, Materials Science and Engineering Division, of the U.S. Department of Energy [DE-AC02-05CH11231]; Office of Science, Office of Basic Energy Sciences, Scientific User Facilities Division, of the U.S. Department of Energy [DE-AC02-05CH11231] FX Financial support for this work was provided through the Electron Microscopy of Soft Matter Program supported by the Director, Office of Science, Office of Basic Energy Sciences, Materials Science and Engineering Division, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. The TEM experiments were performed as user projects at the National Center for Electron Microscopy and the Molecular Foundry, Lawrence Berkeley National Laboratory, which are supported by the Office of Science, Office of Basic Energy Sciences, Scientific User Facilities Division, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. We thank Dr. Mohit Singh for the synthesis of the block copolymer. F.I.A would also like to thank Professor Enrique Gomez, Dr. Sergey Yakovlev and and Dr. Daniel Hallinan for helpful discussions. NR 27 TC 3 Z9 3 U1 0 U2 80 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0968-4328 J9 MICRON JI Micron PD JAN PY 2013 VL 44 BP 442 EP 450 DI 10.1016/j.micron.2012.09.010 PG 9 WC Microscopy SC Microscopy GA 062NA UT WOS:000312925300048 PM 23092928 ER PT J AU Dixon, RK AF Dixon, Robert K. TI Algae based biofuels SO MITIGATION AND ADAPTATION STRATEGIES FOR GLOBAL CHANGE LA English DT Editorial Material DE Energy security; Environmental protection; Economic growth; Biotechnology; Algae; Biofuels C1 US DOE, Off Energy Efficiency & Renewable Energy, Washington, DC 20585 USA. RP Dixon, RK (reprint author), US DOE, Off Energy Efficiency & Renewable Energy, 1000 Independence Ave SW, Washington, DC 20585 USA. EM rdixon1@thegef.org NR 10 TC 2 Z9 2 U1 3 U2 72 PU SPRINGER PI DORDRECHT PA VAN GODEWIJCKSTRAAT 30, 3311 GZ DORDRECHT, NETHERLANDS SN 1381-2386 J9 MITIG ADAPT STRAT GL JI Mitig. Adapt. Strateg. Glob. Chang. PD JAN PY 2013 VL 18 IS 1 SI SI BP 1 EP 4 DI 10.1007/s11027-012-9412-4 PG 4 WC Environmental Sciences SC Environmental Sciences & Ecology GA 060NL UT WOS:000312784900001 ER PT J AU Frank, ED Elgowainy, A Han, J Wang, ZC AF Frank, Edward D. Elgowainy, Amgad Han, Jeongwoo Wang, Zhichao TI Life cycle comparison of hydrothermal liquefaction and lipid extraction pathways to renewable diesel from algae SO MITIGATION AND ADAPTATION STRATEGIES FOR GLOBAL CHANGE LA English DT Article DE Algae; Life cycle analysis; Hydrothermal liquefaction; Greenhouse gas emissions; Renewable diesel ID PRESSURE AQUEOUS ENVIRONMENTS; BIODIESEL PRODUCTION; ANAEROBIC-DIGESTION; NANNOCHLOROPSIS SP; MICROALGAE; GASIFICATION; OIL; FEEDSTOCKS; CATALYSTS; AMMONIUM AB Algae biomass is an attractive biofuel feedstock when grown with high productivity on marginal land. Hydrothermal liquefaction (HTL) produces more oil from algae than lipid extraction (LE) does because protein and carbohydrates are converted, in part, to oil. Since nitrogen in the algae biomass is incorporated into the HTL oil, and since lipid extracted algae for generating heat and electricity are not co-produced by HTL, there are questions regarding implications for emissions and energy use. We studied the HTL and LE pathways for renewable diesel (RD) production by modeling all essential operations from nutrient manufacturing through fuel use. Our objective was to identify the key relationships affecting HTL energy consumption and emissions. LE, with identical upstream growth model and consistent hydroprocessing model, served as reference. HTL used 1.8 fold less algae than did LE but required 5.2 times more ammonia when nitrogen incorporated in the HTL oil was treated as lost. HTL RD had life cycle emissions of 31,000 gCO(2) equivalent (gCO(2)e) compared to 21,500 gCO(2)e for LE based RD per million BTU of RD produced. Greenhouse gas (GHG) emissions increased when yields exceeded 0.4 g HTL oil/g algae because insufficient carbon was left for biogas generation. Key variables in the analysis were the HTL oil yield, the hydrogen demand during upgrading, and the nitrogen content of the HTL oil. Future work requires better data for upgrading renewable oils to RD and requires consideration of nitrogen recycling during upgrading. C1 [Frank, Edward D.; Elgowainy, Amgad; Han, Jeongwoo; Wang, Zhichao] Argonne Natl Lab, Ctr Transportat Res, Argonne, IL 60439 USA. RP Frank, ED (reprint author), Argonne Natl Lab, Ctr Transportat Res, 9700 S Cass Ave, Argonne, IL 60439 USA. EM efrank@anl.gov; aelgowainy@anl.gov; jhan@anl.gov; wangz@anl.gov RI Frank, Edward/A-8865-2012 FU Office of Biomass Program in the U.S. Department of Energy Office of Energy Efficiency and Renewable Energy; [DE-AC02-06CH11357] FX E.D. Frank, A. Elgowainy, J. Han, and Z. Wang performed this work for UChicago Argonne LLC, the author in fact, as a Works Made for Hire (17 USC 201(b)). This work was sponsored by the Office of Biomass Program in the U.S. Department of Energy Office of Energy Efficiency and Renewable Energy. Argonne National Laboratory is a DOE laboratory managed by UChicago Argonne, LLC, under Contract No. DE-AC02-06CH11357. The authors thank K. C. Das (University of Georgia, Athens), Ryan Davis (National Renewable Energy Laboratory), Jeff Miller and Meltem Urgun-Demirtas (Argonne National Laboratory), George Oyler (Genifuel Corp.), Y. Zhang, and G. Yu (University of Illinois) for helpful discussions. NR 42 TC 65 Z9 65 U1 6 U2 185 PU SPRINGER PI DORDRECHT PA VAN GODEWIJCKSTRAAT 30, 3311 GZ DORDRECHT, NETHERLANDS SN 1381-2386 J9 MITIG ADAPT STRAT GL JI Mitig. Adapt. Strateg. Glob. Chang. PD JAN PY 2013 VL 18 IS 1 SI SI BP 137 EP 158 DI 10.1007/s11027-012-9395-1 PG 22 WC Environmental Sciences SC Environmental Sciences & Ecology GA 060NL UT WOS:000312784900009 ER PT J AU Fensin, SJ Valone, SM Cerreta, EK Escobedo-Diaz, JP Gray, GT Kang, K Wang, J AF Fensin, S. J. Valone, S. M. Cerreta, E. K. Escobedo-Diaz, J. P. Gray, G. T., III Kang, K. Wang, J. TI Effect of grain boundary structure on plastic deformation during shock compression using molecular dynamics SO MODELLING AND SIMULATION IN MATERIALS SCIENCE AND ENGINEERING LA English DT Article ID STRAIN-RATE RESPONSE; MECHANICAL-PROPERTIES; SPALL DAMAGE; COPPER; BEHAVIOR; FRACTURE; FAILURE; DUCTILE; SOLIDS; METALS AB Grain boundaries (GBs) can play an important role in governing the mechanical behavior and damage evolution of a material during both quasistatic and dynamic loading. However, the general consensus of the shock physics community has been that minute details about the GB structure should not affect the response of a material to dynamic loading. In this paper, we present results of molecular-dynamics simulations investigating whether or not small changes in boundary structure are 'recognized' by the shock wave and can in turn affect the spall strength of a material. As a test case, we study a Sigma 11 asymmetric tilt GB in copper with an ordered and a disordered structure. The results are also compared with face-centered-cubic single crystals which correspond to the crystal orientations of the two grains in the bi-crystal. These results show that ordered and disordered boundaries undergo dissimilar amounts of plastic deformation during shock loading, which leads to spall strengths that vary by 12%, likely due to differences in the GB structures. C1 [Fensin, S. J.; Valone, S. M.; Cerreta, E. K.; Escobedo-Diaz, J. P.; Gray, G. T., III; Kang, K.; Wang, J.] Los Alamos Natl Lab, Los Alamos, NM USA. RP Fensin, SJ (reprint author), Los Alamos Natl Lab, MST 8, Los Alamos, NM USA. EM saryuj@lanl.gov RI Wang, Jian/F-2669-2012; OI Wang, Jian/0000-0001-5130-300X; Kang, Keonwook/0000-0002-8428-8288; Escobedo-Diaz, Juan/0000-0003-2413-7119 FU US Department of Energy [DE-AC52-06NA25396]; office of Basic Energy Sciences Advanced Simulations; Energy Frontier Research Center of Materials at irradiation and mechanical extremes (CNIME); DOD/DOE Joint Munitions Program; LDRD-DR [20100026] FX Los Alamos National Laboratory is operated by LANS, LLC, for the NNSA and the US Department of Energy under contract DE-AC52-06NA25396. This work has been supported by the office of Basic Energy Sciences Advanced Simulations and the Energy Frontier Research Center of Materials at irradiation and mechanical extremes (CNIME), as well as the DOD/DOE Joint Munitions Program and LDRD-DR 20100026. SJF and SMV also want to acknowledge helpful discussions with R G Hoagland. NR 46 TC 9 Z9 10 U1 3 U2 54 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 0965-0393 J9 MODEL SIMUL MATER SC JI Model. Simul. Mater. Sci. Eng. PD JAN PY 2013 VL 21 IS 1 AR 015011 DI 10.1088/0965-0393/21/1/015011 PG 12 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA 058YV UT WOS:000312672100011 ER PT J AU Tucker, GJ Aitken, ZH Greer, JR Weinberger, CR AF Tucker, Garritt J. Aitken, Zachary H. Greer, Julia R. Weinberger, Christopher R. TI The mechanical behavior and deformation of bicrystalline nanowires SO MODELLING AND SIMULATION IN MATERIALS SCIENCE AND ENGINEERING LA English DT Article ID TILT GRAIN-BOUNDARIES; MOLECULAR-DYNAMICS SIMULATION; DISLOCATION NUCLEATION; NANOCRYSTALLINE COPPER; FCC METALS; ATOMISTIC SIMULATIONS; PLASTIC-DEFORMATION; MICRON SCALE; STRENGTH; ALUMINUM AB The competition between free surfaces and internal grain boundaries as preferential sites for dislocation nucleation during plastic deformation in aluminum bicrystalline nanowires is investigated using molecular dynamics simulations at room temperature. A number of nanowires containing various minimum energy interfaces are studied under uniaxial compression at a constant applied strain rate to provide a broad, inclusive look at the competition between the two types of sources. In addition, we conduct a detailed study on the role of the grain boundaries to act as a source, sink, or obstacle for lattice dislocations, as a function of grain boundary structure. This work compares the behavior of bicrystalline nanowires containing both random high-angle boundaries and a series of symmetric tilt grain boundaries to further elucidate the effect of interface structure on its behavior. The results show that grain boundaries in nanowires can be preferred nucleation sites for dislocations and twin boundaries, in addition to efficient sinks and pinning points for migrating dislocations. Plastic deformation behavior at high imposed strains is linked to the underlying deformation processes, such as twinning, dislocation pinning, or dislocation exhaustion/starvation. We also detail some important reactions between lattice dislocations and grain boundaries observed in the simulations, along with the activation of a single-arm source. This work suggests that the cooperation of numerous mechanisms and the structure of internal grain boundaries are crucial in understanding the deformation of bicrystalline nanowires. Online supplementary data available from stacks.iop.org/MSMSE/21/015004/mmedia C1 [Tucker, Garritt J.; Weinberger, Christopher R.] Sandia Natl Labs, Computat Mat Sci & Engn Dept, Albuquerque, NM 87185 USA. [Aitken, Zachary H.; Greer, Julia R.] CALTECH, Div Engn & Appl Sci, Pasadena, CA 91125 USA. RP Tucker, GJ (reprint author), Sandia Natl Labs, Computat Mat Sci & Engn Dept, POB 5800,MS 1411, Albuquerque, NM 87185 USA. EM gtucker@sandia.gov RI Weinberger, Christopher/E-2602-2011; Tucker, Garritt/A-1954-2016 OI Weinberger, Christopher/0000-0001-9550-6992; Tucker, Garritt/0000-0002-4011-450X FU US Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000]; NSF through CAREER grant [DMR-0748267] 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 US Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000. JRG gratefully acknowledges the financial support of NSF through CAREER grant (DMR-0748267). NR 71 TC 8 Z9 8 U1 3 U2 69 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 0965-0393 J9 MODEL SIMUL MATER SC JI Model. Simul. Mater. Sci. Eng. PD JAN PY 2013 VL 21 IS 1 AR 015004 DI 10.1088/0965-0393/21/1/015004 PG 18 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA 058YV UT WOS:000312672100004 ER PT J AU Ulz, MH Mandadapu, KK Papadopoulos, P AF Ulz, Manfred H. Mandadapu, Kranthi K. Papadopoulos, Panayiotis TI On the estimation of spatial averaging volume for determining stress using atomistic methods SO MODELLING AND SIMULATION IN MATERIALS SCIENCE AND ENGINEERING LA English DT Article ID DYNAMICS; METALS AB The estimation of stress at a continuum point from the atomistic scale requires volume averaging over a region that contains this point. A hypothesis is put forth to obtain a lower bound for the size of this region based on an analogy to the Ising model. This hypothesis is tested on copper using two classical elasticity problems. C1 [Papadopoulos, Panayiotis] Univ Calif Berkeley, Dept Mech Engn, Berkeley, CA 94720 USA. [Mandadapu, Kranthi K.] Sandia Natl Labs, Livermore, CA 94551 USA. [Ulz, Manfred H.] Graz Univ Technol, Inst Strength Mat, A-8010 Graz, Austria. RP Papadopoulos, P (reprint author), Univ Calif Berkeley, Dept Mech Engn, Berkeley, CA 94720 USA. EM panos@berkeley.edu OI Ulz, Manfred/0000-0002-9240-3688 NR 26 TC 5 Z9 6 U1 0 U2 4 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 0965-0393 EI 1361-651X J9 MODEL SIMUL MATER SC JI Model. Simul. Mater. Sci. Eng. PD JAN PY 2013 VL 21 IS 1 AR 015010 DI 10.1088/0965-0393/21/1/015010 PG 15 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA 058YV UT WOS:000312672100010 ER PT J AU Bokulich, NA Subramanian, S Faith, JJ Gevers, D Gordon, JI Knight, R Mills, DA Caporaso, JG AF Bokulich, Nicholas A. Subramanian, Sathish Faith, Jeremiah J. Gevers, Dirk Gordon, Jeffrey I. Knight, Rob Mills, David A. Caporaso, J. Gregory TI Quality-filtering vastly improves diversity estimates from Illumina amplicon sequencing SO NATURE METHODS LA English DT Article AB High-throughput sequencing has revolutionized microbial ecology, but read quality remains a considerable barrier to accurate taxonomy assignment and alpha-diversity assessment for microbial communities. We demonstrate that high-quality read length and abundance are the primary factors differentiating correct from erroneous reads produced by Illumina GAIIx, HiSeq and MiSeq instruments. We present guidelines for user-defined quality-filtering strategies, enabling efficient extraction of high-quality data and facilitating interpretation of Illumina sequencing results. C1 [Caporaso, J. Gregory] Argonne Natl Lab, Inst Genom & Syst Biol, Argonne, IL 60439 USA. [Bokulich, Nicholas A.; Mills, David A.] Univ Calif Davis, Dept Viticulture & Enol, Davis, CA 95616 USA. [Bokulich, Nicholas A.; Mills, David A.] Univ Calif Davis, Dept Food Sci & Technol, Davis, CA 95616 USA. [Bokulich, Nicholas A.; Mills, David A.] Univ Calif Davis, Foods Hlth Inst, Davis, CA 95616 USA. [Subramanian, Sathish; Faith, Jeremiah J.; Gordon, Jeffrey I.] Washington Univ, Sch Med, Ctr Genome Sci & Syst Biol, St Louis, MO USA. [Gevers, Dirk] Broad Inst MIT & Harvard, Microbial Syst & Communities Genome Sequencing &, Cambridge, MA USA. [Knight, Rob] Univ Colorado, Dept Chem & Biochem, Boulder, CO 80309 USA. [Knight, Rob] Univ Colorado, Howard Hughes Med Inst, Boulder, CO 80309 USA. [Caporaso, J. Gregory] No Arizona Univ, Dept Comp Sci, Flagstaff, AZ 86011 USA. RP Caporaso, JG (reprint author), Argonne Natl Lab, Inst Genom & Syst Biol, 9700 S Cass Ave, Argonne, IL 60439 USA. EM gregcaporaso@gmail.com RI Knight, Rob/D-1299-2010 FU US National Institutes of Health [NIH DK78669, NIH R01HD059127, NIH U54HG004969]; Juvenile Diabetes Research Fund; Crohn's and Colitis Foundation of America; Howard Hughes Medical Institute; Dannon Probiotics Fellow Program (The Dannon Company); Wine Spectator scholarship FX We thank G. Giannoukos (Broad Institute of MIT and Harvard), I. Rasolonjatovo (Illumina), M. Gebert (University of Colorado, Boulder) and L. Wegener Parfrey (University of Colorado, Boulder) for contributing mock community sequencing data used in this study, and S. Huse and A. Gonzalez for useful feedback and discussions of this manuscript. This work was supported in part by grants from the US National Institutes of Health (NIH DK78669 to J.I.G., NIH R01HD059127 to D.A.M. and NIH U54HG004969 to D.G.), the Juvenile Diabetes Research Fund (D.G.), the Crohn's and Colitis Foundation of America (J.I.G. and D.G.), and the Howard Hughes Medical Institute. N.A.B. was supported by the 2012-2013 Dannon Probiotics Fellow Program (The Dannon Company) and a Wine Spectator scholarship. NR 15 TC 265 Z9 274 U1 17 U2 233 PU NATURE PUBLISHING GROUP PI LONDON PA MACMILLAN BUILDING, 4 CRINAN ST, LONDON N1 9XW, ENGLAND SN 1548-7091 J9 NAT METHODS JI Nat. Methods PD JAN PY 2013 VL 10 IS 1 BP 57 EP U11 DI 10.1038/NMETH.2276 PG 4 WC Biochemical Research Methods SC Biochemistry & Molecular Biology GA 060WW UT WOS:000312810100036 PM 23202435 ER PT J AU Kyoung, MJ Zhang, YX Diao, JJ Chu, S Brunger, AT AF Kyoung, Minjoung Zhang, Yunxiang Diao, Jiajie Chu, Steven Brunger, Axel T. TI Studying calcium-triggered vesicle fusion in a single vesicle-vesicle content and lipid-mixing system SO NATURE PROTOCOLS LA English DT Article ID MEMBRANE-FUSION; SNARE COMPLEX; IN-VITRO; NEUROTRANSMITTER RELEASE; CENTRAL SYNAPSE; EXOCYTOSIS; MOLECULE; PROTEINS; DOCKING; CELLS AB This protocol describes a single vesicle-vesicle microscopy system to study Ca2+-triggered vesicle fusion. Donor vesicles contain reconstituted synaptobrevin and synaptotagmin-1. Acceptor vesicles contain reconstituted syntaxin and synaptosomal-associated protein 25 (SNAP-25), and they are tethered to a PEG-coated glass surface. Donor vesicles are mixed with the tethered acceptor vesicles and incubated for several minutes at a zero-Ca2+ concentration, resulting in a collection of single interacting vesicle pairs. The donor vesicles also contain two spectrally distinct fluorophores that allow simultaneous monitoring of temporal changes of the content and membrane. Upon Ca2+ injection into the sample chamber, our system therefore differentiates between hemifusion and complete fusion of interacting vesicle pairs and determines the temporal sequence of these events on a sub-100-millisecond time scale. Other factors such as complexin can be easily added. Our system is unique in that it monitors both content and lipid mixing and starts from a metastable state of interacting vesicle pairs before Ca2+ injection. C1 [Kyoung, Minjoung; Zhang, Yunxiang; Diao, Jiajie; Brunger, Axel T.] Stanford Univ, Dept Mol & Cellular Physiol, Stanford, CA 94305 USA. [Kyoung, Minjoung; Zhang, Yunxiang; Diao, Jiajie; Brunger, Axel T.] Stanford Univ, Dept Neurol & Neurol Sci, Stanford, CA 94305 USA. [Kyoung, Minjoung; Zhang, Yunxiang; Diao, Jiajie; Brunger, Axel T.] Stanford Univ, Dept Biol Struct, Stanford, CA 94305 USA. [Kyoung, Minjoung; Zhang, Yunxiang; Diao, Jiajie; Brunger, Axel T.] Stanford Univ, Dept Photon Sci, Stanford, CA 94305 USA. [Kyoung, Minjoung; Diao, Jiajie; Brunger, Axel T.] Stanford Univ, Howard Hughes Med Inst, Stanford, CA 94305 USA. [Zhang, Yunxiang; Chu, Steven] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Zhang, Yunxiang; Chu, Steven] Univ Calif Berkeley, Dept Phys, Berkeley, CA 94720 USA. [Zhang, Yunxiang; Chu, Steven] Univ Calif Berkeley, Dept Mol & Cell Biol, Berkeley, CA 94720 USA. RP Brunger, AT (reprint author), Stanford Univ, Dept Mol & Cellular Physiol, Stanford, CA 94305 USA. EM brunger@stanford.edu RI Diao, Jiajie/A-3425-2008; OI Diao, Jiajie/0000-0003-4288-3203; Brunger, Axel/0000-0001-5121-2036 FU US National Institutes of Health [R37-MH63105] FX This work was supported by US National Institutes of Health grant no. R37-MH63105 to A.T.B. We thank M. Padolina for making the video of the acceptor and donor vesicle preparation; and D. Cipriano, R. Garland and M. Padolina for critical reading of the manuscript. NR 42 TC 28 Z9 28 U1 6 U2 65 PU NATURE PUBLISHING GROUP PI LONDON PA MACMILLAN BUILDING, 4 CRINAN ST, LONDON N1 9XW, ENGLAND SN 1754-2189 EI 1750-2799 J9 NAT PROTOC JI Nat. Protoc. PD JAN PY 2013 VL 8 IS 1 BP 1 EP 16 DI 10.1038/nprot.2012.134 PG 16 WC Biochemical Research Methods SC Biochemistry & Molecular Biology GA 064DO UT WOS:000313051300001 PM 23222454 ER PT J AU Volkow, ND Kim, SW Wang, GJ Alexoff, D Logan, J Muench, L Shea, C Telang, F Fowler, JS Wong, C Benveniste, H Tomasi, D AF Volkow, Nora D. Kim, Sung Won Wang, Gene-Jack Alexoff, David Logan, Jean Muench, Lisa Shea, Colleen Telang, Frank Fowler, Joanna S. Wong, Christopher Benveniste, Helene Tomasi, Dardo TI Acute alcohol intoxication decreases glucose metabolism but increases acetate uptake in the human brain SO NEUROIMAGE LA English DT Article DE Glia; PET; FDG; Alcoholism; Withdrawal; Acetate ID ETHANOL WITHDRAWAL SYNDROME; CEREBRAL-BLOOD-FLOW; RAT-BRAIN; IN-VIVO; ASTROCYTES; TRANSPORT; STIMULATION; MARKER; PET; CONSEQUENCES AB Alcohol intoxication results in marked reductions in brain glucose metabolism, which we hypothesized reflect not just its GABAergic enhancing effects but also the metabolism of acetate as an alternative brain energy source. To test this hypothesis we separately assessed the effects of alcohol intoxication on brain glucose and acetate metabolism using Positron Emission Tomography (PET). We found that alcohol intoxication significantly decreased whole brain glucose metabolism (measured with FOG) with the largest decrements in cerebellum and occipital cortex and the smallest in the thalamus. In contrast, alcohol intoxication caused a significant increase in [1-C-11]acetate brain uptake (measured as standard uptake value, SUV), with the largest increases occurring in the cerebellum and the smallest in the thalamus. In heavy alcohol drinkers [1-C-11]acetate brain uptake during alcohol challenge tended to be higher than in occasional drinkers (p<0.06) and the increases in [1-C-11]acetate uptake in cerebellum with alcohol were positively associated with the reported amount of alcohol consumed (r=0.66, p<0.01). Our findings corroborate a reduction of brain glucose metabolism during intoxication and document an increase in brain acetate uptake. The opposite changes observed between regional brain metabolic decrements and regional increases in [1-C-11]acetate uptake support the hypothesis that during alcohol intoxication the brain may rely on acetate as an alternative brain energy source and provides preliminary evidence that heavy alcohol exposures may facilitate the use of acetate as an energy substrate. These findings raise the question of the potential therapeutic benefits that increasing plasma acetate concentration (i.e. ketogenic diets) may have in alcoholics undergoing alcohol detoxification. (C) 2012 Published by Elsevier Inc. C1 [Volkow, Nora D.] NIDA, Bethesda, MD 20892 USA. [Volkow, Nora D.; Kim, Sung Won; Muench, Lisa; Telang, Frank; Wong, Christopher; Tomasi, Dardo] NIAAA, Bethesda, MD 20892 USA. [Wang, Gene-Jack; Alexoff, David; Logan, Jean; Shea, Colleen; Fowler, Joanna S.] Brookhaven Natl Lab, Dept Med, Upton, NY 11973 USA. [Benveniste, Helene] SUNY Stony Brook, Dept Anesthesiol, Stony Brook, NY 11794 USA. RP Volkow, ND (reprint author), NIDA, 6001 Execut Blvd 6001,Room 5274, Bethesda, MD 20892 USA. EM nvolkow@nida.nih.gov RI Tomasi, Dardo/J-2127-2015 FU NIH's Intramural Research Program (NIAAA); DOE [DE-AC01-76CH00016] FX We thank David Schlyer, Paul Vaska, Youwen Xu, Pauline Carter, Millard Jayne and Karen Apelskog for their contributions and Ruben Baler for editorial assistance. Research was supported by NIH's Intramural Research Program (NIAAA) and by DOE (DE-AC01-76CH00016). NR 52 TC 22 Z9 23 U1 0 U2 23 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 1053-8119 EI 1095-9572 J9 NEUROIMAGE JI Neuroimage PD JAN 1 PY 2013 VL 64 BP 277 EP 283 DI 10.1016/j.neuroimage.2012.08.057 PG 7 WC Neurosciences; Neuroimaging; Radiology, Nuclear Medicine & Medical Imaging SC Neurosciences & Neurology; Radiology, Nuclear Medicine & Medical Imaging GA 056PU UT WOS:000312504200026 PM 22947541 ER PT J AU Burr, T Williams, B Croft, S White, M Hanson, K AF Burr, Tom Williams, Brian Croft, Stephen White, Morgan Hanson, Ken TI Meta-Analysis Options for Inconsistent Nuclear Measurements SO NUCLEAR SCIENCE AND ENGINEERING LA English DT Article ID MODELS AB Meta-analysis aims to combine results from multiple experiments. For example, a neutron reaction rate or cross section is typically measured in multiple experiments, and a single estimate and its uncertainty are provided for users of the estimated reaction rate. It is often difficult to combine estimates from multiple laboratories because there can be important differences in experimental protocols among laboratories and because laboratories do not always provide all the information needed to assess the estimate's uncertainty, particularly if total uncertainty (random and systematic) is required. The paper illustrates that explicit measurement error models are essential for understanding measurement processes and for guiding how to combine multiple measurements, whether the measurements are consistent or not. We emphasize that both the consensus estimate and its estimated uncertainty depend on the assumed measurement error model, and we investigate measurement error model selection options for two examples. C1 [Burr, Tom; Williams, Brian; Croft, Stephen; White, Morgan; Hanson, Ken] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Burr, T (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM tburr@lanl.gov NR 22 TC 1 Z9 1 U1 0 U2 6 PU AMER NUCLEAR SOC PI LA GRANGE PK PA 555 N KENSINGTON AVE, LA GRANGE PK, IL 60526 USA SN 0029-5639 J9 NUCL SCI ENG JI Nucl. Sci. Eng. PD JAN PY 2013 VL 173 IS 1 BP 15 EP 27 PG 13 WC Nuclear Science & Technology SC Nuclear Science & Technology GA 064RB UT WOS:000313092000002 ER PT J AU Roberts, JA Rearden, BT Wilson, PPH AF Roberts, Jeremy A. Rearden, Bradley T. Wilson, Paul P. H. TI Determination and Application of Partial Biases in Criticality Safety Validation SO NUCLEAR SCIENCE AND ENGINEERING LA English DT Article ID SENSITIVITY AB This paper presents a method for determining partial biases and bias uncertainties for application in fission product burnup credit criticality safety analysis. The contribution of each nuclide to the overall system k(eff) bias and the bias uncertainty are determined via the generalized linear least squares method. Where experimental benchmarks are available to validate specific nuclides, sensitivity and uncertainty analysis is used to project biases observed in the benchmarks to biases appropriate for the safety system. Two weighting schemes are proposed to produce an overall bias in the safety system from several single partial biases. Finally, these methods are used to determine partial biases for Sm-149 and Rh-103 from two experiment series and to apply these biases to a representative used fuel safety system. The biases obtained are compared to bounding estimates, and the sensitivity of the results to relevant assumptions is addressed. C1 [Roberts, Jeremy A.; Wilson, Paul P. H.] Univ Wisconsin, Dept Engn Phys, Madison, WI 53706 USA. [Rearden, Bradley T.] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. RP Roberts, JA (reprint author), Univ Wisconsin, Dept Engn Phys, 1500 Engn Dr, Madison, WI 53706 USA. EM robertsj@mit.edu FU U.S. Department of Energy's (DOE's) Advanced Fuel Cycle Initiative University Fellowship Program; DOE's Nuclear Criticality Safety Program FX The first author was supported by the U.S. Department of Energy's (DOE's) Advanced Fuel Cycle Initiative University Fellowship Program. The second author was supported by DOE's Nuclear Criticality Safety Program. NR 19 TC 0 Z9 0 U1 0 U2 4 PU AMER NUCLEAR SOC PI LA GRANGE PK PA 555 N KENSINGTON AVE, LA GRANGE PK, IL 60526 USA SN 0029-5639 EI 1943-748X J9 NUCL SCI ENG JI Nucl. Sci. Eng. PD JAN PY 2013 VL 173 IS 1 BP 43 EP 57 PG 15 WC Nuclear Science & Technology SC Nuclear Science & Technology GA 064RB UT WOS:000313092000004 ER PT J AU Piet, SJ AF Piet, Steven J. TI When Is the Simple Radiotoxicity Approach Useful for Advanced Fuel Cycle System Assessments Given the Existence of Complex Performance Dose Assessments? SO NUCLEAR SCIENCE AND ENGINEERING LA English DT Article ID FUSION-REACTORS; EBR-II; SAFETY; WASTE AB Engineers often face the general question of which approximations are appropriate for a given analytical task. In particular, when is a simpler model useful if a more complex model also exists? This paper explores this question in the domain of radiotoxicity relative to geologic disposal performance dose assessments. Criterion 1 requires that the simpler approach, radiotoxicity, must be calculated correctly. The concept of ingestion radiotoxic inventories is analogous to the inventory of toxic chemicals in other industries. From a decision analysis perspective, it is also somewhat analogous to the nuclear reactor safety concept of "passive safety." This paper explains some of the issues in calculating radio toxicity, motivated by the author's observations of errors in the literature: not accounting for radioactive progeny, misunderstanding natural "ore," and focusing on transuranic (TRU) isotopes without adequate attention to actinide decay products. For example, Th/U-233 fuel cycles do have lower amounts of TRU isotopes than U/Pu-239 fuel cycles, but that does not necessarily mean lower long-term hazard. Criterion 2 requires that the uncertainties in the more complex approach, performance dose assessments, must raise issues for the assessments' intended purposes in which case, radiotoxic inventory may be of assistance until those issues are resolved. Performance dose assessments were developed for, and are legally the way to show, compliance with regulations, but the uncertainties are large. Less obvious is the degree to which dose assessments are applicable to other purposes-comparing fuel cycle options prior to site selection and showing the safety of a fuel cycle and waste management approach to the public. In the last sense especially, performance dose assessments are analogous to probabilistic risk assessments for nuclear reactor safety. The United States lacks a selected consensus site, selected fuel cycle approach (direct disposal versus recycling), and selected waste form. Thus, the paper does not intend to discuss all the issues with performance dose assessments but rather intends to focus on only those performance dose uncertainties that raise issues when comparing fuel cycles. Uncertainties associated with whether a generic geological environment is attractive or a specific location meets requirements are beyond the scope of this paper. Ingestion radiotoxicity correlates with heat, gamma, and inhalation radiotoxicity. Thus, options that are relatively high in ingestion radiotoxicity tend to be high in other parameters. Therefore, reduction in ingestion radiotoxicity means both that the potential source term for release is lower but also that one driving force for release (heat) is also lower. However, the most important time frames differ as heat is mainly an issue in decades and centuries after reactor discharge, but ingestion radio toxicity is mainly an issue during longer time periods. Ingestion radiotoxicity points to the importance of actinides in long-term waste management, followed by specific fission products such as Tc-99, I-129, Zr-93, Cs-135, and Se-79. TRU isotopes were important in four of five generic geologic environments recently studied independently with used fuel disposal experts as were the same fission products as noted from radiotoxicity in part because waste assessments must include multiple exposure pathways including human intrusion and drilling into the waste. Dose calculations that were made for used fuel disposal may be misleading if extrapolated to disposal of only the remnants of used fuel separation because the chemistry of waste will differ. Radiotoxicity can be misleading if used to strictly rank order among individual isotopes if a specific disposal option is well known. Hybrid approaches that incorporate radiotoxicity and features of full performance assessments may have value. C1 Idaho Natl Lab, Idaho Falls, ID 83415 USA. RP Piet, SJ (reprint author), Idaho Natl Lab, Mail Stop 3870,2525 N Fremont, Idaho Falls, ID 83415 USA. EM pietsteven@hotmail.com FU DOE Idaho Operations Office [DE-AC07-05ID14517] FX This paper was prepared for the U.S. DOE Office of Nuclear Energy, Science, and Technology under DOE Idaho Operations Office contract DE-AC07-05ID14517. The author thanks his many colleagues over the past several years for helpful conversations on this topic, including B. Dixon, S. Bays, R. Weiner, M. Nutt, N. Soelberg., P. Swift, and two anonymous reviewers of the manuscript. NR 57 TC 3 Z9 3 U1 0 U2 6 PU AMER NUCLEAR SOC PI LA GRANGE PK PA 555 N KENSINGTON AVE, LA GRANGE PK, IL 60526 USA SN 0029-5639 J9 NUCL SCI ENG JI Nucl. Sci. Eng. PD JAN PY 2013 VL 173 IS 1 BP 58 EP 81 PG 24 WC Nuclear Science & Technology SC Nuclear Science & Technology GA 064RB UT WOS:000313092000005 ER PT J AU Tanaka, K Henry, CS Zinner, JF Jolivet, E Cohoon, MP Xia, FF Bidnenko, V Ehrlich, SD Stevens, RL Noirot, P AF Tanaka, Kosei Henry, Christopher S. Zinner, Jenifer F. Jolivet, Edmond Cohoon, Matthew P. Xia, Fangfang Bidnenko, Vladimir Ehrlich, S. Dusko Stevens, Rick L. Noirot, Philippe TI Building the repertoire of dispensable chromosome regions in Bacillus subtilis entails major refinement of cognate large-scale metabolic model SO NUCLEIC ACIDS RESEARCH LA English DT Article ID ESCHERICHIA-COLI GENOME; REDUCED-GENOME; RNASE-P; TRANSCRIPTIONAL REGULATION; THERMODYNAMIC ANALYSIS; SYNTHETIC BIOLOGY; GENE; ESSENTIALITY; PATHWAY; CELL AB The nonessential regions in bacterial chromosomes are ill-defined due to incomplete functional information. Here, we establish a comprehensive repertoire of the genome regions that are dispensable for growth of Bacillus subtilis in a variety of media conditions. In complex medium, we attempted deletion of 157 individual regions ranging in size from 2 to 159 kb. A total of 146 deletions were successful in complex medium, whereas the remaining regions were subdivided to identify new essential genes (4) and coessential gene sets (7). Overall, our repertoire covers similar to 76% of the genome. We screened for viability of mutant strains in rich defined medium and glucose minimal media. Experimental observations were compared with predictions by the iBsu1103 model, revealing discrepancies that led to numerous model changes, including the large-scale application of model reconciliation techniques. We ultimately produced the iBsu1103V2 model and generated predictions of metabolites that could restore the growth of unviable strains. These predictions were experimentally tested and demonstrated to be correct for 27 strains, validating the refinements made to the model. The iBsu1103V2 model has improved considerably at predicting loss of viability, and many insights gained from the model revisions have been integrated into the Model SEED to improve reconstruction of other microbial models. C1 [Tanaka, Kosei; Jolivet, Edmond; Bidnenko, Vladimir; Ehrlich, S. Dusko; Noirot, Philippe] INRA, UMR Micalis 1319, F-78350 Jouy En Josas, France. [Tanaka, Kosei; Bidnenko, Vladimir; Ehrlich, S. Dusko; Noirot, Philippe] AgroParisTech, UMR Micalis, F-78350 Jouy En Josas, France. [Henry, Christopher S.; Zinner, Jenifer F.; Xia, Fangfang; Stevens, Rick L.] Argonne Natl Lab, Dept Math & Comp Sci, Argonne, IL 60439 USA. [Cohoon, Matthew P.; Stevens, Rick L.] Univ Chicago, Computat Inst, Chicago, IL 60637 USA. RP Noirot, P (reprint author), INRA, UMR Micalis 1319, F-78350 Jouy En Josas, France. EM chenry@mcs.anl.gov; philippe.noirot@jouy.inra.fr FU U.S. Department of Energy [DE-ACO2-06CH11357]; European Commission [FP7-244093] FX The U.S. Department of Energy [under contract DE-ACO2-06CH11357]; European Commission 7th Framework project BaSynthec [FP7-244093]. Funding for open access charge: European Commission 7th Framework project BaSynthec [FP7-244093]. NR 51 TC 26 Z9 27 U1 1 U2 27 PU OXFORD UNIV PRESS PI OXFORD PA GREAT CLARENDON ST, OXFORD OX2 6DP, ENGLAND SN 0305-1048 J9 NUCLEIC ACIDS RES JI Nucleic Acids Res. PD JAN PY 2013 VL 41 IS 1 BP 687 EP 699 DI 10.1093/nar/gks963 PG 13 WC Biochemistry & Molecular Biology SC Biochemistry & Molecular Biology GA 061ZW UT WOS:000312889900089 PM 23109554 ER PT J AU Blake, JA Dolan, M Drabkin, H Hill, DP Ni, L Sitnikov, D Bridges, S Burgess, S Buza, T McCarthy, F Peddinti, D Pillai, L Carbon, S Dietze, H Ireland, A Lewis, SE Mungall, CJ Gaudet, P Chisholm, RL Fey, P Kibbe, WA Basu, S Siegele, DA McIntosh, BK Renfro, DP Zweifel, AE Hu, JC Brown, NH Tweedie, S Alam-Faruque, Y Apweiler, R Auchinchloss, A Axelsen, K Bely, B Blatter, MC Bonilla, C Bougueleret, L Boutet, E Breuza, L Bridge, A Chan, WM Chavali, G Coudert, E Dimmer, E Estreicher, A Famiglietti, L Feuermann, M Gos, A Gruaz-Gumowski, N Hieta, R Hinz, U Hulo, C Huntley, R James, J Jungo, F Keller, G Laiho, K Legge, D Lemercier, P Lieberherr, D Magrane, M Martin, MJ Masson, P Mutowo-Muellenet, P O'Donovan, C Pedruzzi, I Pichler, K Poggioli, D Millan, PP Poux, S Rivoire, C Roechert, B Sawford, T Schneider, M Stutz, A Sundaram, S Tognolli, M Xenarios, I Foulger, R Lomax, J Roncaglia, P Khodiyar, VK Lovering, RC Talmud, PJ Chibucos, M Giglio, MG Chang, HY Hunter, S McAnulla, C Mitchell, A Sangrador, A Stephan, R Harris, MA Oliver, SG Rutherford, K Wood, V Bahler, J Lock, A Kersey, PJ McDowall, MD Staines, DM Dwinell, M Shimoyama, M Laulederkind, S Hayman, T Wang, SJ Petri, V Lowry, T D'Eustachio, P Matthews, L Balakrishnan, R Binkley, G Cherry, JM Costanzo, MC Dwight, SS Engel, SR Fisk, DG Hitz, BC Hong, EL Karra, K Miyasato, SR Nash, RS Park, J Skrzypek, MS Weng, S Wong, ED Berardini, TZ Li, D Huala, E Mi, H Thomas, PD Chan, J Kishore, R Sternberg, P Van Auken, K Howe, D Westerfield, M AF Blake, J. A. Dolan, M. Drabkin, H. Hill, D. P. Ni, Li Sitnikov, D. Bridges, S. Burgess, S. Buza, T. McCarthy, F. Peddinti, D. Pillai, L. Carbon, S. Dietze, H. Ireland, A. Lewis, S. E. Mungall, C. J. Gaudet, P. Chisholm, R. L. Fey, P. Kibbe, W. A. Basu, S. Siegele, D. A. McIntosh, B. K. Renfro, D. P. Zweifel, A. E. Hu, J. C. Brown, N. H. Tweedie, S. Alam-Faruque, Y. Apweiler, R. Auchinchloss, A. Axelsen, K. Bely, B. Blatter, M-C. Bonilla, C. Bougueleret, L. Boutet, E. Breuza, L. Bridge, A. Chan, W. M. Chavali, G. Coudert, E. Dimmer, E. Estreicher, A. Famiglietti, L. Feuermann, M. Gos, A. Gruaz-Gumowski, N. Hieta, R. Hinz, U. Hulo, C. Huntley, R. James, J. Jungo, F. Keller, G. Laiho, K. Legge, D. Lemercier, P. Lieberherr, D. Magrane, M. Martin, M. J. Masson, P. Mutowo-Muellenet, P. O'Donovan, C. Pedruzzi, I. Pichler, K. Poggioli, D. Millan, P. Porras Poux, S. Rivoire, C. Roechert, B. Sawford, T. Schneider, M. Stutz, A. Sundaram, S. Tognolli, M. Xenarios, I. Foulger, R. Lomax, J. Roncaglia, P. Khodiyar, V. K. Lovering, R. C. Talmud, P. J. Chibucos, M. Giglio, M. Gwinn Chang, H-Y. Hunter, S. McAnulla, C. Mitchell, A. Sangrador, A. Stephan, R. Harris, M. A. Oliver, S. G. Rutherford, K. Wood, V. Bahler, J. Lock, A. Kersey, P. J. McDowall, M. D. Staines, D. M. Dwinell, M. Shimoyama, M. Laulederkind, S. Hayman, T. Wang, S-J Petri, V. Lowry, T. D'Eustachio, P. Matthews, L. Balakrishnan, R. Binkley, G. Cherry, J. M. Costanzo, M. C. Dwight, S. S. Engel, S. R. Fisk, D. G. Hitz, B. C. Hong, E. L. Karra, K. Miyasato, S. R. Nash, R. S. Park, J. Skrzypek, M. S. Weng, S. Wong, E. D. Berardini, T. Z. Li, D. Huala, E. Mi, H. Thomas, P. D. Chan, J. Kishore, R. Sternberg, P. Van Auken, K. Howe, D. Westerfield, M. CA Gene Ontology Consortium TI Gene Ontology Annotations and Resources SO NUCLEIC ACIDS RESEARCH LA English DT Article AB The Gene Ontology (GO) Consortium (GOC, http://www.geneontology.org) is a community-based bioinformatics resource that classifies gene product function through the use of structured, controlled vocabularies. Over the past year, the GOC has implemented several processes to increase the quantity, quality and specificity of GO annotations. First, the number of manual, literature-based annotations has grown at an increasing rate. Second, as a result of a new 'phylogenetic annotation' process, manually reviewed, homology-based annotations are becoming available for a broad range of species. Third, the quality of GO annotations has been improved through a streamlined process for, and automated quality checks of, GO annotations deposited by different annotation groups. Fourth, the consistency and correctness of the ontology itself has increased by using automated reasoning tools. Finally, the GO has been expanded not only to cover new areas of biology through focused interaction with experts, but also to capture greater specificity in all areas of the ontology using tools for adding new combinatorial terms. The GOC works closely with other ontology developers to support integrated use of terminologies. The GOC supports its user community through the use of e-mail lists, social media and web-based resources. C1 [Balakrishnan, R.; Binkley, G.; Cherry, J. M.; Costanzo, M. C.; Dwight, S. S.; Engel, S. R.; Fisk, D. G.; Hitz, B. C.; Hong, E. L.; Karra, K.; Miyasato, S. R.; Nash, R. S.; Park, J.; Skrzypek, M. S.; Weng, S.; Wong, E. D.] Stanford Univ, Dept Genet, SGD, Stanford, CA 94305 USA. [Blake, J. A.; Dolan, M.; Drabkin, H.; Hill, D. P.; Ni, Li; Sitnikov, D.] Jackson Lab, MGI, Bar Harbor, ME 04609 USA. [Bridges, S.; Burgess, S.; Buza, T.; McCarthy, F.; Peddinti, D.; Pillai, L.] Mississippi State Univ, AgBase, Starkville, MS USA. [Carbon, S.; Dietze, H.; Ireland, A.; Lewis, S. E.; Mungall, C. J.] LBNL, BBOP, Berkeley, CA USA. [Gaudet, P.; Chisholm, R. L.; Fey, P.; Kibbe, W. A.; Basu, S.] Northwestern Univ, DictyBase, Chicago, IL 60611 USA. [Siegele, D. A.; McIntosh, B. K.; Renfro, D. P.; Zweifel, A. E.; Hu, J. C.] Texas A&M Univ, Dept Biochem & Biophys, EcoliWiki, College Stn, TX 77843 USA. [Siegele, D. A.; McIntosh, B. K.; Renfro, D. P.; Zweifel, A. E.; Hu, J. C.] Texas A&M Univ, Dept Biol, EcoliWiki, College Stn, TX 77843 USA. [Brown, N. H.; Tweedie, S.] Univ Cambridge, Gurdon Inst, FlyBase, Cambridge, England. [Brown, N. H.; Tweedie, S.] Univ Cambridge, Dept Genet, Cambridge CB2 3EH, England. [Alam-Faruque, Y.; Apweiler, R.; Auchinchloss, A.; Axelsen, K.; Bely, B.; Blatter, M-C.; Bonilla, C.; Bougueleret, L.; Boutet, E.; Breuza, L.; Bridge, A.; Chan, W. M.; Chavali, G.; Coudert, E.; Dimmer, E.; Estreicher, A.; Famiglietti, L.; Feuermann, M.; Gos, A.; Gruaz-Gumowski, N.; Hieta, R.; Hinz, U.; Hulo, C.; Huntley, R.; James, J.; Jungo, F.; Keller, G.; Laiho, K.; Legge, D.; Lemercier, P.; Lieberherr, D.; Magrane, M.; Martin, M. J.; Masson, P.; Mutowo-Muellenet, P.; O'Donovan, C.; Pedruzzi, I.; Pichler, K.; Poggioli, D.; Millan, P. Porras; Poux, S.; Rivoire, C.; Roechert, B.; Sawford, T.; Schneider, M.; Stutz, A.; Sundaram, S.; Tognolli, M.; Xenarios, I.] UniProtKB EBI, Hinxton, Cambs, England. [Alam-Faruque, Y.; Apweiler, R.; Auchinchloss, A.; Axelsen, K.; Bely, B.; Blatter, M-C.; Bonilla, C.; Bougueleret, L.; Boutet, E.; Breuza, L.; Bridge, A.; Chan, W. M.; Chavali, G.; Coudert, E.; Dimmer, E.; Estreicher, A.; Famiglietti, L.; Feuermann, M.; Gos, A.; Gruaz-Gumowski, N.; Hieta, R.; Hinz, U.; Hulo, C.; Huntley, R.; James, J.; Jungo, F.; Keller, G.; Laiho, K.; Legge, D.; Lemercier, P.; Lieberherr, D.; Magrane, M.; Martin, M. J.; Masson, P.; Mutowo-Muellenet, P.; O'Donovan, C.; Pedruzzi, I.; Pichler, K.; Poggioli, D.; Millan, P. Porras; Poux, S.; Rivoire, C.; Roechert, B.; Sawford, T.; Schneider, M.; Stutz, A.; Sundaram, S.; Tognolli, M.; Xenarios, I.] Swiss Inst Bioinformat, SIB, Geneva, Switzerland. [Alam-Faruque, Y.; Apweiler, R.; Auchinchloss, A.; Axelsen, K.; Bely, B.; Blatter, M-C.; Bonilla, C.; Bougueleret, L.; Boutet, E.; Breuza, L.; Bridge, A.; Chan, W. M.; Chavali, G.; Coudert, E.; Dimmer, E.; Estreicher, A.; Famiglietti, L.; Feuermann, M.; Gos, A.; Gruaz-Gumowski, N.; Hieta, R.; Hinz, U.; Hulo, C.; Huntley, R.; James, J.; Jungo, F.; Keller, G.; Laiho, K.; Legge, D.; Lemercier, P.; Lieberherr, D.; Magrane, M.; Martin, M. J.; Masson, P.; Mutowo-Muellenet, P.; O'Donovan, C.; Pedruzzi, I.; Pichler, K.; Poggioli, D.; Millan, P. Porras; Poux, S.; Rivoire, C.; Roechert, B.; Sawford, T.; Schneider, M.; Stutz, A.; Sundaram, S.; Tognolli, M.; Xenarios, I.] PIR Georgetown, Washington, DC USA. [Foulger, R.; Lomax, J.; Roncaglia, P.] GO EBI, Hinxton, Cambs, England. [Khodiyar, V. K.; Lovering, R. C.; Talmud, P. J.] UCL, Inst Cardiovasc Sci, London, England. [Chibucos, M.; Giglio, M. Gwinn] Univ Maryland, Sch Med, Inst Genome Sci, Baltimore, MD 21201 USA. [Chang, H-Y.; Hunter, S.; McAnulla, C.; Mitchell, A.; Sangrador, A.] EBI, InterPro, Hinxton, Cambs, England. [Stephan, R.] MTBBASE, Berlin, Germany. [Harris, M. A.; Oliver, S. G.; Rutherford, K.; Wood, V.] Univ Cambridge, PomBase, Cambridge, England. [Bahler, J.; Lock, A.] UCL, PomBase, London, England. [Kersey, P. J.; McDowall, M. D.; Staines, D. M.] EBI, PomBase, Hinxton, Cambs, England. [Dwinell, M.; Shimoyama, M.; Laulederkind, S.; Hayman, T.; Wang, S-J; Petri, V.; Lowry, T.] Med Coll Wisconsin, RGD, Milwaukee, WI 53226 USA. [D'Eustachio, P.; Matthews, L.] NYU, Sch Med, Dept Biochem, Reactome, New York, NY 10016 USA. [Berardini, T. Z.; Li, D.; Huala, E.] Carnegie Inst Sci, Dept Plant Biol, TAIR, Stanford, CA USA. [Mi, H.; Thomas, P. D.] USC, Los Angeles, CA USA. [Chan, J.; Kishore, R.; Sternberg, P.; Van Auken, K.] CALTECH, WormBase, Pasadena, CA 91125 USA. [Howe, D.; Westerfield, M.] Univ Oregon, ZFIN, Eugene, OR 97403 USA. RP Balakrishnan, R (reprint author), Stanford Univ, Dept Genet, SGD, Stanford, CA 94305 USA. EM ramab@stanford.edu RI Bahler, Jurg/B-4572-2009; Pedruzzi, Ivo/O-7423-2015; Huntley, Rachael/R-1036-2016; Kibbe, Warren/B-2106-2010; OI Chibucos, Marcus/0000-0001-9586-0780; Hunter, Sarah/0000-0003-2453-0770; Mutowo, Prudence/0000-0002-4646-4172; D'Eustachio, Peter/0000-0002-5494-626X; Magrane, Michele/0000-0003-3544-996X; Kersey, Paul/0000-0002-7054-800X; Breuza, Lionel/0000-0002-8075-8625; Xenarios, Ioannis/0000-0002-3413-6841; Martin, Maria-Jesus/0000-0001-5454-2815; Poux, Sylvain/0000-0001-7299-6685; Bridge, Alan/0000-0003-2148-9135; O'Donovan, Claire/0000-0001-8051-7429; Sangrador, Amaia/0000-0001-6688-429X; Rutherford, Kim/0000-0001-6277-726X; Engel, Stacia/0000-0001-5472-917X; Matthews, Lisa/0000-0001-5707-3065; Wood, Valerie/0000-0001-6330-7526; Siegele, Deborah/0000-0001-8935-0696; Lomax, Jane/0000-0001-8865-4321; Cherry, J. Michael/0000-0001-9163-5180; Talmud, Philippa/0000-0002-5560-1933; Lewis, Suzanna/0000-0002-8343-612X; Tweedie, Susan/0000-0003-1818-8243; Bahler, Jurg/0000-0003-4036-1532; Pedruzzi, Ivo/0000-0001-8561-7170; Huntley, Rachael/0000-0001-6718-3559; Kibbe, Warren/0000-0001-5622-7659; Staines, Daniel/0000-0002-7564-9125; Khodiyar, Varsha/0000-0002-2743-6918; Apweiler, Rolf/0000-0001-7078-200X; McDowall, Mark/0000-0002-6666-602X; Pichler, Klemens/0000-0001-6099-8931; Bely, Benoit/0000-0002-0029-9693; Foulger, Rebecca/0000-0001-8682-8754 FU National Human Genome Research Institute (NHGRI) [U41HG002273, 1U41HG006104-03]; British Heart Foundation [SP/07/007/23671]; NHGRI FX National Human Genome Research Institute (NHGRI) [U41HG002273 to the Gene Ontology Consortium, 1U41HG006104-03 to the European Bioinformatics Institute]; British Heart Foundation [SP/07/007/23671]. Funding for open access charge: NHGRI. NR 15 TC 165 Z9 167 U1 8 U2 43 PU OXFORD UNIV PRESS PI OXFORD PA GREAT CLARENDON ST, OXFORD OX2 6DP, ENGLAND SN 0305-1048 J9 NUCLEIC ACIDS RES JI Nucleic Acids Res. PD JAN PY 2013 VL 41 IS D1 BP D530 EP D535 DI 10.1093/nar/gks1050 PG 6 WC Biochemistry & Molecular Biology SC Biochemistry & Molecular Biology GA 062BE UT WOS:000312893300075 ER PT J AU Chivian, D Dehal, PS Keller, K Arkin, AP AF Chivian, Dylan Dehal, Paramvir S. Keller, Keith Arkin, Adam P. TI metaMicrobesOnline: phylogenomic analysis of microbial communities SO NUCLEIC ACIDS RESEARCH LA English DT Article ID ENVIRONMENTAL GENOMICS; METAGENOMICS; METABOLISM; PROTEINS; DATABASE AB The metaMicrobesOnline database (freely available at http://meta.MicrobesOnline.org) offers phylogenetic analysis of genes from microbial genomes and metagenomes. Gene trees are constructed for canonical gene families such as COG and Pfam. Such gene trees allow for rapid homologue analysis and subfamily comparison of genes from multiple metagenomes and comparisons with genes from microbial isolates. Additionally, the genome browser permits genome context comparisons, which may be used to determine the closest sequenced genome or suggest functionally associated genes. Lastly, the domain browser permits rapid comparison of protein domain organization within genes of interest from metagenomes and complete microbial genomes. C1 [Chivian, Dylan; Dehal, Paramvir S.; Keller, Keith; Arkin, Adam P.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Phys Biosci, Berkeley, CA 94720 USA. [Arkin, Adam P.] Univ Calif Berkeley, Dept Bioengn, Berkeley, CA 94720 USA. RP Chivian, D (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Phys Biosci, Berkeley, CA 94720 USA. EM DCChivian@lbl.gov; APArkin@lbl.gov RI Arkin, Adam/A-6751-2008 OI Arkin, Adam/0000-0002-4999-2931 FU Office of Science, Office of Biological and Environmental Research, of the U.S. Department of Energy [DE-AC02-05CH11231]; U.S. Department of Energy FX This work, performed by the Joint BioEnergy Institute (JBEI), 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] between Lawrence Berkeley National Laboratory and the U.S. Department of Energy. Funding for open access charge: U.S. Department of Energy. NR 25 TC 3 Z9 4 U1 3 U2 18 PU OXFORD UNIV PRESS PI OXFORD PA GREAT CLARENDON ST, OXFORD OX2 6DP, ENGLAND SN 0305-1048 J9 NUCLEIC ACIDS RES JI Nucleic Acids Res. PD JAN PY 2013 VL 41 IS D1 BP D648 EP D654 DI 10.1093/nar/gks1202 PG 7 WC Biochemistry & Molecular Biology SC Biochemistry & Molecular Biology GA 062BE UT WOS:000312893300091 PM 23203984 ER PT J AU Yang, S Sleight, SC Sauro, HM AF Yang, Song Sleight, Sean C. Sauro, Herbert M. TI Rationally designed bidirectional promoter improves the evolutionary stability of synthetic genetic circuits SO NUCLEIC ACIDS RESEARCH LA English DT Article ID ESCHERICHIA-COLI; BIOLOGY; GENOME; ADAPTATION; EXPRESSION; SYSTEMS; PARTS AB One problem with synthetic genes in genetically engineered organisms is that these foreign DNAs will eventually lose their functions over evolutionary time in absence of selective pressures. This general limitation can restrain the long-term study and industrial application of synthetic genetic circuits. Previous studies have shown that because of their crucial regulatory functions, prokaryotic promoters in synthetic genetic circuits are especially vulnerable to mutations. In this study, we rationally designed robust bidirectional promoters (BDPs), which are self-protected through the complementarity of their overlapping forward and backward promoter sequences on DNA duplex. When the transcription of a target non-essential gene (e. g. green fluorescent protein) was coupled to the transcription of an essential gene (e. g. antibiotic resistance gene) through the BDP, the evolutionary half-time of the gene of interest increases 4-10 times, depending on the strain and experimental conditions used. This design of using BDPs to increase the mutational stability of genetic circuits can be potentially applied to synthetic biology applications in general. C1 [Yang, Song] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Genom Div, Berkeley, CA 94720 USA. [Sleight, Sean C.; Sauro, Herbert M.] Univ Washington, Dept Bioengn, Seattle, WA 98195 USA. RP Yang, S (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Genom Div, 1 Cyclotron Rd,Mail Stop 84-363, Berkeley, CA 94720 USA. EM songyang@lbl.gov OI Sauro, Herbert/0000-0002-3659-6817 FU Oxford University Press FX Funding for open access charge: Waived by Oxford University Press. NR 28 TC 12 Z9 12 U1 1 U2 29 PU OXFORD UNIV PRESS PI OXFORD PA GREAT CLARENDON ST, OXFORD OX2 6DP, ENGLAND SN 0305-1048 J9 NUCLEIC ACIDS RES JI Nucleic Acids Res. PD JAN PY 2013 VL 41 IS 1 AR e33 DI 10.1093/nar/gks972 PG 7 WC Biochemistry & Molecular Biology SC Biochemistry & Molecular Biology GA 061ZW UT WOS:000312889900033 PM 23093602 ER PT J AU Moyes, AB Castanha, C Germino, MJ Kueppers, LM AF Moyes, Andrew B. Castanha, Cristina Germino, Matthew J. Kueppers, Lara M. TI Warming and the dependence of limber pine (Pinus flexilis) establishment on summer soil moisture within and above its current elevation range SO OECOLOGIA LA English DT Article DE Limber pine; Treeline; Experimental warming; Moisture stress ID ABIES-LASIOCARPA SEEDLINGS; MARIANA MILL. BSP; SUB-ALPINE FOREST; CLIMATE-CHANGE; THERMAL-ACCLIMATION; PICEA-ENGELMANNII; CONIFER SEEDLINGS; LEAF RESPIRATION; ROCKY MOUNTAINS; WATER RELATIONS AB Continued changes in climate are projected to alter the geographic distributions of plant species, in part by affecting where individuals can establish from seed. We tested the hypothesis that warming promotes uphill redistribution of subalpine tree populations by reducing cold limitation at high elevation and enhancing drought stress at low elevation. We seeded limber pine (Pinus flexilis) into plots with combinations of infrared heating and water addition treatments, at sites positioned in lower subalpine forest, the treeline ecotone, and alpine tundra. In 2010, first-year seedlings were assessed for physiological performance and survival over the snow-free growing season. Seedlings emerged in midsummer, about 5-8 weeks after snowmelt. Low temperature was not observed to limit seedling photosynthesis or respiration between emergence and October, and thus experimental warming did not appear to reduce cold limitation at high elevation. Instead, gas exchange and water potential from all sites indicated a prevailing effect of summer moisture stress on photosynthesis and carbon balance. Infrared heaters raised soil growing degree days (base 5 A degrees C, p < 0.001) and August-September mean soil temperature (p < 0.001). Despite marked differences in vegetation cover and meteorological conditions across sites, volumetric soil moisture content (theta) at 5-10 cm below 0.16 and 0.08 m(3) m(-3) consistently corresponded with moderate and severe indications of drought stress in midday stem water potential, stomatal conductance, photosynthesis, and respiration. Seedling survival was greater in watered plots than in heated plots (p = 0.01), and negatively related to soil growing degree days and duration of exposure to theta < 0.08 m(3) m(-3) in a stepwise linear regression model (p < 0.0001). We concluded that seasonal moisture stress and high soil surface temperature imposed a strong limitation to limber pine seedling establishment across a broad elevation gradient, including at treeline, and that these limitations are likely to be enhanced by further climate warming. C1 [Moyes, Andrew B.; Kueppers, Lara M.] Univ Calif Merced, Sch Nat Sci, Merced, CA 95343 USA. [Castanha, Cristina] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Germino, Matthew J.] US Geol Survey, Forest & Rangeland Ecosyst Sci Ctr, Boise, ID 83706 USA. [Germino, Matthew J.] Idaho State Univ, Dept Biol Sci, Pocatello, ID 83209 USA. RP Moyes, AB (reprint author), Univ Calif Merced, Sch Nat Sci, 5200 N Lake Rd, Merced, CA 95343 USA. EM amoyes@ucmerced.edu RI Moyes, Andrew/B-4800-2013; Germino, Matthew/F-6080-2013; Kueppers, Lara/M-8323-2013; Moyes, Andrew/J-3339-2016; Castanha, Cristina/D-3247-2015 OI Kueppers, Lara/0000-0002-8134-3579; Moyes, Andrew/0000-0002-9137-8118; Castanha, Cristina/0000-0001-7327-5169 FU Office of Science (BER), U.S. Department of Energy FX This research was supported by the Office of Science (BER), U.S. Department of Energy. We thank the Mountain Research Station and Niwot Ridge LTER at the University of Colorado, Boulder for logistical support. M. Barlerin, S. Barlerin, J. Beauregard, J. Darrow, S. Ferrenberg, S. Love-Stowell, A. Peterson, and K. Riddell set up and/or maintained the treatment and microclimate sensing infrastructure, and D. Billesbach, D. Christensen, and J. Norris assisted with microclimate data retrieval, quality assurance, and archiving. J. B. Curtis, M. Daly, A. Faist, A. P. Farnham, H. Finkel, E. Flemming, C. Foster, R. Gaffney, A. Howell, A. Qubain, M. Redmond, A. Slominski, S. Sawyer, S. Taylor Smith, and F. Zust collected and sowed seeds and/or conducted germination and survival surveys. Thanks to K. Reinhardt for valuable discussions and helpful feedback on early drafts of the manuscript. Any use of trade, product, or firm names is for descriptive purposes only and does not imply endorsement by the U. S. Government. NR 64 TC 27 Z9 27 U1 6 U2 144 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 0029-8549 EI 1432-1939 J9 OECOLOGIA JI Oecologia PD JAN PY 2013 VL 171 IS 1 BP 271 EP 282 DI 10.1007/s00442-012-2410-0 PG 12 WC Ecology SC Environmental Sciences & Ecology GA 064MI UT WOS:000313079100025 PM 22875149 ER PT J AU Wanger, G Gorby, Y El-Naggar, MY Yuzvinsky, TD Schaudinn, C Gorur, A Sedghizadeh, PP AF Wanger, Greg Gorby, Yuri El-Naggar, Mohamed Y. Yuzvinsky, Thomas D. Schaudinn, Christoph Gorur, Amita Sedghizadeh, Parish P. TI Electrically conductive bacterial nanowires in bisphosphonate-related osteonecrosis of the jaw biofilms SO ORAL SURGERY ORAL MEDICINE ORAL PATHOLOGY ORAL RADIOLOGY LA English DT Article ID MICROBIAL BIOFILMS; EXTRACELLULAR DNA; SECONDARY; THERAPY; MATRIX; MR-1 AB Objective. Bacterial biofilms play a role in the pathogenesis of bisphosphonate-related osteonecrosis of the jaw (BRONJ). The purpose of this preliminary study was to test the hypothesis that the extracellular filaments observed in biofilms associated with BRONJ contain electrically conductive nanowires. Study Design. Bone samples of patients affected by BRONJ were evaluated for conductive nanowires by scanning electron microscopy (SEM) and conductive probe atomic force microscopy (CP-AFM). We created nanofabricated electrodes to measure electrical transport along putative nanowires. Results. SEM revealed large-scale multispecies biofilms containing numerous filamentous structures throughout necrotic bone. CP-AFM analysis revealed that these structures were electrically conductive nanowires with resistivities on the order of 20 Omega.cm. Nanofabricated electrodes spaced along the nanowires confirmed their ability to transfer electrons over micron-scale lengths. Conclusions. Electrically conductive bacterial nanowires to date have been described only in environmental isolates. This study shows for the first time that these nanowires can also be found in clinically relevant biofilm-mediated diseases, such as BRONJ, and may represent an important target for therapy. (Oral Surg Oral Med Oral Pathol Oral Radiol 2013;115:71-78) C1 [Sedghizadeh, Parish P.] Univ So Calif, Ctr Biofilms, Los Angeles, CA 90089 USA. [Wanger, Greg] J Craig Venter Inst, Electromicrobiol Grp, San Diego, CA USA. [Gorby, Yuri] Univ So Calif, Dept Biol Sci, Los Angeles, CA 90089 USA. [El-Naggar, Mohamed Y.; Yuzvinsky, Thomas D.] Univ So Calif, Dept Phys, Los Angeles, CA 90089 USA. [Schaudinn, Christoph] Robert Koch Inst, Ctr Biol Secur, Berlin, Germany. [Gorur, Amita] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Life Sci, Berkeley, CA 94720 USA. RP Sedghizadeh, PP (reprint author), Univ So Calif, USC Ctr Biofilms, Herman Ostrow Sch Dent, 925 W 34th St 4110, Los Angeles, CA 90089 USA. EM sedghiza@usc.edu OI Yuzvinsky, Thomas/0000-0001-5708-2877; Sedghizadeh, Parish/0000-0003-4190-0497 NR 25 TC 13 Z9 13 U1 3 U2 32 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 2212-4403 J9 OR SURG OR MED OR PA JI Oral Surg. Oral Med. Oral Pathol. Oral Radiol. PD JAN PY 2013 VL 115 IS 1 BP 71 EP 78 DI 10.1016/j.oooo.2012.08.446 PG 8 WC Dentistry, Oral Surgery & Medicine SC Dentistry, Oral Surgery & Medicine GA 060UX UT WOS:000312804800021 PM 23217537 ER PT J AU Chang, LL Chen, ZQ Liu, X Wang, HJ AF Chang, Linlin Chen, Zhiqiang Liu, Xi Wang, Hejing TI Expansivity and compressibility of wadeite-type K2Si4O9 determined by in situ high T/P experiments, and their implication SO PHYSICS AND CHEMISTRY OF MINERALS LA English DT Article DE Compressibility; Thermal expansivity; Thermodynamic calculation; Wadeite-type K2Si4O9; X-ray diffraction ID X-RAY-DIFFRACTION; EQUATION-OF-STATE; TEMPERATURE HEAT-CAPACITY; HIGH-PRESSURE TRANSITIONS; LOWER MANTLE CONDITIONS; EARTHS LOWER MANTLE; THERMODYNAMIC PROPERTIES; KALSI3O8 HOLLANDITE; PHASE-EQUILIBRIA; SYSTEM KALSI3O8-NAALSI3O8 AB Wadeite-type K2Si4O9 was synthesized with a cubic press at 5.4 GPa and 900 A degrees C for 3 h. Its unit-cell parameters were measured by in situ high-T powder X-ray diffraction up to 600 A degrees C at ambient P. The T-V data were fitted with a polynomial expression for the volumetric thermal expansion coefficient (alpha(T) = a (0) + a (1) T), yielding a (0) = 2.47(21) x 10(-5) K-1 and a (1) = 1.45(36) x 10(-8) K-2. Compression experiments at ambient T were conducted up to 10.40 GPa with a diamond-anvil cell combined with synchrotron X-ray radiation. A second-order Birch-Murnaghan equation of state was used to fit the P-V data, yielding K (T) = 97(3) GPa and V (0) = 360.55(9) (3). These newly determined thermal expansion data and compression data were used to thermodynamically calculate the P-T curves of the following reactions: 2 sanidine (KAlSi3O8) = wadeite (K2Si4O9) + kyanite (Al2SiO5) + coesite (SiO2) and wadeite (K2Si4O9) + kyanite (Al2SiO5) + coesite/stishovite (SiO2) = 2 hollandite (KAlSi3O8). The calculated phase boundaries are generally consistent with previous experimental determinations. C1 [Chang, Linlin; Liu, Xi; Wang, Hejing] Peking Univ, Key Lab Orogen Belts & Crustal Evolut, Minist Educ China MOE, Beijing 100871, Peoples R China. [Chang, Linlin; Liu, Xi; Wang, Hejing] Peking Univ, Sch Earth & Space Sci, Beijing 100871, Peoples R China. [Chen, Zhiqiang] Brookhaven Natl Lab, Natl Synchrotron Light Source, Upton, NY 11973 USA. RP Liu, X (reprint author), Peking Univ, Key Lab Orogen Belts & Crustal Evolut, Minist Educ China MOE, Beijing 100871, Peoples R China. EM xi.liu@pku.edu.cn RI chen, zhiqiang/C-9134-2013; Liu, Xi/K-9845-2015 FU National Natural Science Foundation of China [41090371]; State Key Laboratory of Ore Deposit Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences [201114] FX We thank Professors Yingwei Fei and Youxue Zhang for their very constructive discussions. We are grateful to the useful comments on our manuscript from Dr Matteo Alvaro and an anonymous reviewer, and to the patience from Professor Masanori Matsui who editorially handled our paper. This investigation was financially supported by the National Natural Science Foundation of China (Grant #41090371) and the State Key Laboratory of Ore Deposit Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences (Grant #201114). NR 57 TC 4 Z9 7 U1 0 U2 31 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 0342-1791 J9 PHYS CHEM MINER JI Phys. Chem. Miner. PD JAN PY 2013 VL 40 IS 1 BP 29 EP 40 DI 10.1007/s00269-012-0543-7 PG 12 WC Materials Science, Multidisciplinary; Mineralogy SC Materials Science; Mineralogy GA 064EC UT WOS:000313053300005 ER PT J AU Wagner, A Tobimatsu, Y Goeminne, G Phillips, L Flint, H Steward, D Torr, K Donaldson, L Boerjan, W Ralph, J AF Wagner, Armin Tobimatsu, Yuki Goeminne, Geert Phillips, Lorelle Flint, Heather Steward, Diane Torr, Kirk Donaldson, Lloyd Boerjan, Wout Ralph, John TI Suppression of CCR impacts metabolite profile and cell wall composition in Pinus radiata tracheary elements SO PLANT MOLECULAR BIOLOGY LA English DT Article DE Pinus radiata; Cinnamoyl-CoA reductase; Tracheary elements; Lignin; Pyrolysis; Thioacidolysis ID CINNAMOYL COA REDUCTASE; THERMAL-DEGRADATION PRODUCTS; MASS-SPECTROMETRIC CHARACTERIZATION; POLYSACCHARIDE DERIVED PRODUCTS; GAS-CHROMATOGRAPHIC SEPARATION; DOWN-REGULATION; OBTAINING 1,6-ANHYDROSACCHARIDES; ALCOHOL-DEHYDROGENASE; LIGNIN COMPOSITION; FAST PYROLYSIS AB Suppression of the lignin-related gene cinnamoyl-CoA reductase (CCR) in the Pinus radiata tracheary element (TE) system impacted both the metabolite profile and the cell wall matrix in CCR-RNAi lines. UPLC-MS/MS-based metabolite profiling identified elevated levels of p-coumaroyl hexose, caffeic acid hexoside and ferulic acid hexoside in CCR-RNAi lines, indicating a redirection of metabolite flow within phenylpropanoid metabolism. Dilignols derived from coniferyl alcohol such as G(8-5)G, G(8-O-4)G and isodihydrodehydrodiconiferyl alcohol (IDDDC) were substantially depleted, providing evidence for CCR's involvement in coniferyl alcohol biosynthesis. Severe CCR suppression almost halved lignin content in TEs based on a depletion of both H-type and G-type lignin, providing evidence for CCR's involvement in the biosynthesis of both lignin types. 2D-NMR studies revealed minor changes in the H:G-ratio and consequently a largely unchanged interunit linkage distribution in the lignin polymer. However, unusual cell wall components including ferulate and unsaturated fatty acids were identified in TEs by thioacidolysis, pyrolysis-GC/MS and/or 2D-NMR in CCR-RNAi lines, providing new insights into the consequences of CCR suppression in pine. Interestingly, CCR suppression substantially promoted pyrolytic breakdown of cell wall polysaccharides, a phenotype most likely caused by the incorporation of acidic compounds into the cell wall matrix in CCR-RNAi lines. C1 [Wagner, Armin; Phillips, Lorelle; Flint, Heather; Steward, Diane; Torr, Kirk; Donaldson, Lloyd] Scion, Rotorua, New Zealand. [Tobimatsu, Yuki; Ralph, John] Univ Wisconsin, Dept Biochem, Madison, WI 53705 USA. [Goeminne, Geert; Boerjan, Wout] Univ Ghent VIB, Dept Plant Syst Biol, B-9052 Ghent, Belgium. [Goeminne, Geert; Boerjan, Wout] UGhent, Dept Plant Biotechnol & Bioinformat, B-9052 Ghent, Belgium. [Ralph, John] Wisconsin Bioenergy Initiat, DOE Great Lakes Bioenergy Res Ctr, Madison, WI USA. RP Wagner, A (reprint author), Scion, Private Bag 3020, Rotorua, New Zealand. EM armin.wagner@scionresearch.com OI Boerjan, Wout/0000-0003-1495-510X FU New Zealand Ministry of Science and Innovation [C04X0207, C04X0703]; DOE Great Lakes Bioenergy Research Center (DOE Office of Science BER) [DE-FC02-07ER64494]; Japan Society for the Promotion of Science; Research Foundation Flanders [G.0352.05N] FX This work was funded in part by grants C04X0207 and C04X0703 from the New Zealand Ministry of Science and Innovation. Funding for J.R. was from the DOE Great Lakes Bioenergy Research Center (DOE Office of Science BER DE-FC02-07ER64494). Y.T. was supported by a Postdoctoral Fellowship for Research Abroad provided by the Japan Society for the Promotion of Science. G.G. and W.B. thank the Research Foundation Flanders (Grant no. G.0352.05N). The authors would like to thank Elspeth MacRae for critical reading of this manuscript. NR 38 TC 21 Z9 21 U1 2 U2 62 PU SPRINGER PI DORDRECHT PA VAN GODEWIJCKSTRAAT 30, 3311 GZ DORDRECHT, NETHERLANDS SN 0167-4412 J9 PLANT MOL BIOL JI Plant Mol.Biol. PD JAN PY 2013 VL 81 IS 1-2 BP 105 EP 117 DI 10.1007/s11103-012-9985-z PG 13 WC Biochemistry & Molecular Biology; Plant Sciences SC Biochemistry & Molecular Biology; Plant Sciences GA 061UC UT WOS:000312872900008 PM 23131896 ER PT J AU Gerken, HG Donohoe, B Knoshaug, EP AF Gerken, Henri G. Donohoe, Bryon Knoshaug, Eric P. TI Enzymatic cell wall degradation of Chlorella vulgaris and other microalgae for biofuels production SO PLANTA LA English DT Article DE Growth inhibition; Permeability; Lysozyme; Nitrogen depletion ID ACIDIC POLYSACCHARIDE; SUGAR COMPOSITION; GREEN MICROALGAE; ALGAE; CHLOROPHYTA; EXTRACTION; PHYTOPLANKTON; CONSTITUENTS; RESISTANCE; DIVERSITY AB Cell walls of microalgae consist of a polysaccharide and glycoprotein matrix providing the cells with a formidable defense against its environment. We characterized enzymes that can digest the cell wall and weaken this defense for the purpose of protoplasting or lipid extraction. A growth inhibition screen demonstrated that chitinase, lysozyme, pectinase, sulfatase, beta-glucuronidase, and laminarinase had the broadest effect across the various Chlorella strains tested and also inhibited Nannochloropsis and Nannochloris strains. Chlorella is typically most sensitive to chitinases and lysozymes, both enzymes that degrade polymers containing N-acetylglucosamine. Using a fluorescent DNA stain, we developed rapid methodology to quantify changes in permeability in response to enzyme digestion and found that treatment with lysozyme in conjunction with other enzymes has a drastic effect on cell permeability. Transmission electron microscopy of enzymatically treated Chlorella vulgaris indicates that lysozyme degrades the outer surface of the cell wall and removes hair-like fibers protruding from the surface, which differs from the activity of chitinase. This action on the outer surface of the cell causes visible protuberances on the cell surface and presumably leads to the increased settling rate when cells are treated with lysozyme. We demonstrate radical ultrastructural changes to the cell wall in response to treatment with various enzyme combinations which, in some cases, causes a greater than twofold increase in the thickness of the cell wall. The enzymes characterized in this study should prove useful in the engineering and extraction of oils from microalgae. C1 [Gerken, Henri G.; Knoshaug, Eric P.] Natl Renewable Energy Lab, Natl Bioenergy Ctr, Golden, CO 80401 USA. [Gerken, Henri G.] Arizona State Univ, Lab Algae Res & Biotechnol, Mesa, AZ USA. [Donohoe, Bryon] Natl Renewable Energy Lab, Biosci Ctr, Golden, CO USA. RP Knoshaug, EP (reprint author), Natl Renewable Energy Lab, Natl Bioenergy Ctr, 15013 Denver W Pkwy, Golden, CO 80401 USA. EM eric.knoshaug@nrel.gov FU NREL's Laboratory Directed Research and Development program FX The authors would like to thank Jonathan Meuser for help with 18S RNA gene sequencing, Ben Smith for help with quantification of settling, Todd Vinzant and the Biomass Surface Characterization Laboratory at NREL for help in SEM image acquisition, and Philip Pienkos for technical discussions and manuscript review. This project was funded by NREL's Laboratory Directed Research and Development program. NR 53 TC 73 Z9 74 U1 18 U2 213 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 0032-0935 J9 PLANTA JI Planta PD JAN PY 2013 VL 237 IS 1 BP 239 EP 253 DI 10.1007/s00425-012-1765-0 PG 15 WC Plant Sciences SC Plant Sciences GA 063VP UT WOS:000313030400018 PM 23011569 ER PT J AU Goldsmith, CF Tomlin, AS Klippenstein, SJ AF Goldsmith, C. Franklin Tomlin, Alison S. Klippenstein, Stephen J. TI Uncertainty propagation in the derivation of phenomenological rate coefficients from theory: A case study of n-propyl radical oxidation SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Uncertainty analysis; Master equation; Propane oxidation; Sensitivity analysis; Ab initio transition state theory ID GLOBAL SENSITIVITY; MODEL REPRESENTATIONS; COMBUSTION; KINETICS; HDMR; O-2; AUTOIGNITION; OPTIMIZATION; CHEMISTRY AB Global uncertainty and sensitivity analysis is used to study the propagation of uncertainties in fundamental theoretical parameters through to uncertainties in the predicted temperature and pressure dependent phenomenological rate coefficients. Predictions are obtained from ab initio transition state theory based master equation calculations. The fundamental parameters for these rate predictions include barrier heights, well depths, vibrational frequencies, collision frequency, and energy transfer parameters. A random sampling high-dimensional model representation (HDMR) approach is used to perform the global sensitivity analysis. This approach determines the predicted distributions of the phenomenological rate coefficients based on a quasi-random sample of the fundamental parameters within their uncertainty range. Sensitivity analysis then identifies the main parameters which contribute to variance in the predicted distributions. Here the approach is applied to a study of the oxidation of the propyl radical, employing the parameters derived in our recent theoretical study. We find rates at 3 sigma variances that typically differ from the most frequent values by factors of 4-6, with the uncertainties decreasing with increasing temperature. For the well skipping reactions there are more parameters that contribute significantly to the variance, the second-order sensitivities are greater, and the uncertainties increased with increasing pressure. For the other reactions, the uncertainties tend to decrease with increasing pressure. (C) 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Goldsmith, C. Franklin] Fritz Haber Inst, Dept Inorgan Chem, D-14195 Berlin, Germany. [Tomlin, Alison S.] Univ Leeds, Sch Proc Environm & Mat Engn, Energy Res Inst, Leeds LS2 9JT, W Yorkshire, England. [Klippenstein, Stephen J.] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. RP Klippenstein, SJ (reprint author), Argonne Natl Lab, Chem Sci & Engn Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM sjk@anl.gov OI Klippenstein, Stephen/0000-0001-6297-9187 FU Division of Chemical Sciences, Geosciences, and Biosciences, the Office of Basic Energy Sciences, the U.S. Department of Energy through FWP [DE-AC02-06CH11357, 2009 ANL 59044]; Alexander von Humboldt Foundation FX The work at Argonne was supported by the Division of Chemical Sciences, Geosciences, and Biosciences, the Office of Basic Energy Sciences, the U.S. Department of Energy, under contract number DE-AC02-06CH11357 through FWP # 2009 ANL 59044. CFG acknowledges financial support from the Alexander von Humboldt Foundation. NR 31 TC 28 Z9 29 U1 3 U2 52 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 177 EP 185 DI 10.1016/j.proci.2012.05.091 PN 1 PG 9 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065CN UT WOS:000313125400007 ER PT J AU Labbe, NJ Seshadri, V Kasper, T Hansen, N Osswald, P Westmoreland, PR AF Labbe, Nicole J. Seshadri, Vikram Kasper, Tina Hansen, Nils Osswald, Patrick Westmoreland, Phillip R. TI Flame chemistry of tetrahydropyran as a model heteroatomic biofuel SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Molecular-beam mass spectrometry; Kinetics; Flat flame; Modeling; Quantum chemistry ID PHOTOIONIZATION MASS-SPECTROMETRY; TEMPERATURE OXIDATION; COMBUSTION CHEMISTRY AB The flame chemistry of tetrahydropyran (THP), a cyclic ether, has been examined using vacuum-ultraviolet (VUV)-photoionization molecular-beam mass spectrometry (PI-MBMS) and flame modeling, motivated by the need to understand and predict the combustion of oxygen-containing, biomass-derived fuels. Species identifications and mole-fraction profiles are presented for a fuel-rich (Phi = 1.75), laminar premixed THP-oxygen-argon flame at 2.66 kPa (20.0 Torr). Flame species with up to six heavy atoms have been detected. A detailed reaction set was developed for THP combustion that captures relevant features of the THP flame quite well, allowing analysis of the dominant kinetic pathways for THP combustion. Necessary rate coefficients and transport parameters were calculated or were estimated by analogies with a recent reaction set [Li et al., Combust. Flame 158 (2011) 2077-2089], and necessary thermochemical properties were computed using the CBS-QB3 method. Our results show that under the low-pressure conditions, THP destruction is dominated by H-abstraction, and the three resulting THP-yl radicals decompose primarily by beta-scissions to two-and four-heavy-atom species that are generally destroyed by beta-scission, abstraction, or oxidation. (C) 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Labbe, Nicole J.] Univ Massachusetts, Amherst, MA 01003 USA. [Westmoreland, Phillip R.] N Carolina State Univ, Dept Chem & Biomol Engn, Raleigh, NC 27695 USA. [Kasper, Tina] Univ Duisburg Essen, Duisburg, Germany. [Hansen, Nils] Sandia Natl Labs, Livermore, CA USA. [Osswald, Patrick] Univ Bielefeld, D-33615 Bielefeld, Germany. RP Westmoreland, PR (reprint author), N Carolina State Univ, Dept Chem & Biomol Engn, Engn Bldg 1,Box 7905, Raleigh, NC 27695 USA. EM phil.westmoreland@ncsu.edu RI Hansen, Nils/G-3572-2012; Osswald, Patrick/N-3377-2013; Kasper, Tina/A-2975-2017 OI Osswald, Patrick/0000-0002-2257-2988; Kasper, Tina/0000-0003-3993-5316 FU U.S. Department of Energy [DE-FG02-91ER14192]; Department of Defense (DoD) through a National Defense Science & Engineering Graduate Fellowship; National Center for Supercomputing Applications [TG-CTS090056]; U.S. Department of Energy, Office of Basic Energy Sciences under the Energy Frontier Research Center for Combustion Science [DE-SC0001198]; National Nuclear Security Administration [DE-AC04-94-AL85000]; US DOE/BES [DE-AC02-05CH11231] FX This work was supported in part by the U.S. Department of Energy (P.R.W.) under contract DE-FG02-91ER14192 and by the Department of Defense (DoD) through a National Defense Science & Engineering Graduate Fellowship (N.J.L.). This work was partially supported by the National Center for Supercomputing Applications under grant number TG-CTS090056 using the Cobalt supercomputer (N.J.L. and P.R.W.). NH is supported in part by the U.S. Department of Energy, Office of Basic Energy Sciences under the Energy Frontier Research Center for Combustion Science (Grant No. DE-SC0001198). Sandia is a multi-program laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the National Nuclear Security Administration under contract DE-AC04-94-AL85000. PI-MBMS measurements were performed within the "Flame Team" collaboration at the Advanced Light Source, Lawrence Berkeley National Laboratory, which is supported by the US DOE/BES under DE-AC02-05CH11231. The experiments have benefitted from the able support of technicians, doctoral students, and postdocs, including Wenjun Li and Bin Yang, and the valued contributions of Prof. Katharina Kohse-Hoinghaus and the late Terrill Cool. NR 25 TC 11 Z9 11 U1 3 U2 41 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 259 EP 267 DI 10.1016/j.proci.2012.07.027 PN 1 PG 9 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065CN UT WOS:000313125400016 ER PT J AU Jasper, AW Hansen, N AF Jasper, Ahren W. Hansen, Nils TI Hydrogen-assisted isomerizations of fulvene to benzene and of larger cyclic aromatic hydrocarbons SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Benzene; Fulvene; Naphthalene; PAH; Theoretical chemical kinetics ID THERMAL UNIMOLECULAR REACTIONS; MASTER EQUATION; LOW-PRESSURES; RADICALS; FLAMES; KINETICS; MECHANISMS; ACETYLENE; DYNAMICS; SURFACES AB The H-assisted isomerization of fulvene to benzene is characterized in detail using quantum chemistry, transition state theory, classical trajectory, and master equation calculations. This multistep isomerization involves 10 transition states, nine of which are found to contribute non-negligibly to the overall kinetics. Calculated temperature- and pressure-dependent rate coefficients are presented for H + fulvene --> products, with care taken to quantify uncertainties in the theoretical predictions arising from various aspects of the calculation. The rate coefficients agree with past theoretical work within these estimated uncertainties. This fast isomerization proceeds via a cyclopropylcarbinyl intermediate-a substituted cyclopropyl group adjacent to a radical carbon-that provides a facile route for the carbon bonding rearrangement. Analogous H-assisted isomerization pathways involving cyclopropylcarbinyl intermediates are characterized using quantum chemistry calculations for four second-ring isomers of naphthalene: fulvalene, azulene, 1-methyleneindene, and 2-methyleneindene. These processes, and those for larger polycyclic aromatic hydrocarbons (PAHs), may be characterized in a general way as occurring in five steps: H additions, H shifts, cyclopropylcarbinyl intermediate formation, cyclopropylcarbinyl intermediate ring opening, and H-atom regeneration. Trends in the energetics of each of these steps with respect to PAH size and composition are discussed. (C) 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Jasper, Ahren W.; Hansen, Nils] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. RP Jasper, AW (reprint author), Sandia Natl Labs, Combust Res Facil, POB 969, Livermore, CA 94551 USA. EM ajasper@sandia.gov RI Hansen, Nils/G-3572-2012; Jasper, Ahren/A-5292-2011 FU Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy [DE-AC04-94-AL85000] FX This work is supported by the Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy (DE-AC04-94-AL85000). NR 47 TC 21 Z9 21 U1 9 U2 66 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 279 EP 287 DI 10.1016/j.proci.2012.06.165 PN 1 PG 9 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065CN UT WOS:000313125400018 ER PT J AU Wang, WJ Li, ZH Oehlschlaeger, MA Healy, D Curran, HJ Sarathy, SM Mehl, M Pitz, WJ Westbrook, CK AF Wang, Weijing Li, Zhenhua Oehlschlaeger, Matthew A. Healy, Darren Curran, Henry J. Sarathy, S. Mani Mehl, Marco Pitz, William J. Westbrook, Charles K. TI An experimental and modeling study of the autoignition of 3-methylheptane SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE 3-Methylheptane; Shock tube; Rapid compression machine; Chemical kinetic modeling ID RAPID COMPRESSION MACHINE; SHOCK-TUBE; COMBUSTION; OXIDATION; ISOMERS; HEPTANE; IGNITION; OCTANE AB An experimental and kinetic modeling study of the autoignition of 3-methylheptane, a compound representative of the high molecular weight lightly branched alkanes found in large quantities in conventional and synthetic aviation kerosene and diesel fuels, is reported. Shock tube and rapid compression machine ignition delay time measurements are reported over a wide range of conditions of relevance to combustion engine applications: temperatures from 678 to 1356 K; pressures of 6.5, 10, 20, and 50 atm; and equivalence ratios of 0.5, 1.0, and 2.0. The wide range of temperatures examined provides observation of autoignition in three reactivity regimes, including the negative temperature coefficient (NTC) regime characteristic of paraffinic fuels. Comparisons made between the current ignition delay measurements for 3-methylheptane and previous results for n-octane and 2-methylheptane quantifies the influence of a single methyl substitution and its location on the reactivity of alkanes. It is found that the three C-8 alkane isomers have indistinguishable high-temperature ignition delay but their ignition delay times deviate in the NTC and low-temperature regimes in correlation with their research octane numbers. The experimental results are compared with the predictions of a proposed kinetic model that includes both high-and low-temperature oxidation chemistry. The model mechanistically explains the differences in reactivity for n-octane, 2-methylheptane, and 3-methylheptane in the NTC through the influence of the methyl substitution on the rates of isomerization reactions in the low-temperature chain branching pathway, that ultimately leads to keto-hydroperoxide species, and the competition between low-temperature chain branching and the formation of cyclic ethers, in a chain propagating pathway. (C) 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Wang, Weijing; Li, Zhenhua; Oehlschlaeger, Matthew A.] Rensselaer Polytech Inst, Troy, NY USA. [Li, Zhenhua] Shanghai Jiao Tong Univ, Shanghai 200030, Peoples R China. [Healy, Darren; Curran, Henry J.] Natl Univ Ireland, Galway, Ireland. [Sarathy, S. Mani; Mehl, Marco; Pitz, William J.; Westbrook, Charles K.] Lawrence Livermore Natl Lab, Livermore, CA USA. RP Oehlschlaeger, MA (reprint author), 110 8th St,JEC 2049, Troy, NY 12180 USA. EM oehlsm@rpi.edu RI Sarathy, S. Mani/M-5639-2015; Mehl, Marco/A-8506-2009; OI Sarathy, S. Mani/0000-0002-3975-6206; Mehl, Marco/0000-0002-2227-5035; Curran, Henry/0000-0002-5124-8562 FU U.S. Air Force Office of Scientific Research [FA9550-11-1-0261]; US Department of Energy [DE-AC52-07NA27344]; Office of Naval Research; US Department of Energy, Office of Vehicle Technologies; NSERC of Canada FX The Rensselaer group was supported by the U.S. Air Force Office of Scientific Research (Grant No. FA9550-11-1-0261) with Dr. Chiping Li as technical monitor. The work at LLNL was performed under the auspices of the US Department of Energy under Contract DE-AC52-07NA27344. The LLNL group was supported by the Office of Naval Research (program manager Sharon Beermann-Curtin) and the US Department of Energy, Office of Vehicle Technologies (program manager Gurpreet Singh). Coauthor SMS acknowledges fellowship support from NSERC of Canada. NR 24 TC 9 Z9 10 U1 3 U2 23 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 335 EP 343 DI 10.1016/j.proci.2012.06.001 PN 1 PG 9 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065CN UT WOS:000313125400024 ER PT J AU Kukkadapu, G Kumar, K Sung, CJ Mehl, M Pitz, WJ AF Kukkadapu, Goutham Kumar, Kamal Sung, Chih-Jen Mehl, Marco Pitz, William J. TI Autoignition of gasoline and its surrogates in a rapid compression machine SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Gasoline; Surrogates; Autoignition; Ignition delay; Rapid compression machine ID MIXTURES; FUEL AB The analysis and interpretation of the combustion chemistry is greatly simplified by using simple mixtures of pure components, referred to as surrogates, in lieu of fully-blended transportation fuels, such as gasoline. Recognizing that the ability to model autoignition chemistry is critical to understanding the operation of Homogeneous Charged Compression Ignition engines, this work is an attempt to experimentally and computationally assess the autoignition responses of research grade gasoline and two of its proposed surrogates reported in the literature using a rapid compression machine (RCM), for the low-to-intermediate temperature range and at high pressures. The first surrogate studied is a three-component mixture of iso-octane, n-heptane, and toluene. The second is a four-component mixture that includes an olefin (2-pentene), in addition to the ones noted above. Ignition delay times of stoichiometric mixtures, for gasoline and the two surrogates in air, are measured using an RCM for pressures of 20 and 40 bar, and in the temperature range of 650-900 K. The four-component surrogate is found to emulate the ignition delay times of gasoline more closely when compared to the three-component surrogate. Additionally, the experimental data are compared against the computed results from a recently developed surrogate model for gasoline combustion. A good agreement between the experimental and computed results is observed, while discrepancies are also identified and discussed. (C) 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Kukkadapu, Goutham; Kumar, Kamal; Sung, Chih-Jen] Univ Connecticut, Dept Mech Engn, Storrs, CT 06269 USA. [Mehl, Marco; Pitz, William J.] Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. RP Sung, CJ (reprint author), Univ Connecticut, Dept Mech Engn, Room 484,United Technol Engn Bldg, Storrs, CT 06269 USA. EM cjsung@engr.uconn.edu RI Mehl, Marco/A-8506-2009; OI Mehl, Marco/0000-0002-2227-5035; Kumar, Kamal/0000-0002-3923-8740 FU National Science Foundation [0932559]; U.S. Department of Energy, Office of Vehicle Technologies; U.S. Department of Energy [DE-AC52-07NA27344] FX The work at UCONN was supported by the National Science Foundation under Grant No. 0932559, while the work at LLNL was supported by the U.S. Department of Energy, Office of Vehicle Technologies (program manager GurpreetSingh) and performed under the auspices of the U.S. Department of Energy under Contract DE-AC52-07NA27344. The authors would like to thank Dr. John Dec of the Sandia National Laboratory for supplying the fuel sample of RD387. NR 13 TC 28 Z9 28 U1 4 U2 48 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 345 EP 352 DI 10.1016/j.proci.2012.06.135 PN 1 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065CN UT WOS:000313125400025 ER PT J AU Eskola, AJ Welz, O Savee, JD Osborn, DL Taatjes, CA AF Eskola, Arkke J. Welz, Oliver Savee, John D. Osborn, David L. Taatjes, Craig A. TI Synchrotron photoionization measurements of fundamental autoignition reactions: Product formation in low-temperature isobutane oxidation SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Isobutane; Photoionization; Mass spectrometry; Low-temperature oxidation; Kinetics ID ALKYL PLUS O-2; COMBUSTION CHEMISTRY; RADICALS; DECOMPOSITION; OXYGEN; OH; CYCLOHEXYL; PATHWAYS; PROPYL; HO2 AB Product formation in laser-photolytic Cl-initiated low-temperature (550-700 K) oxidation of isobutane in a slow-flow reactor was investigated by tunable synchrotron photoionization mass spectrometry. These experiments probed the time-resolved formation of products following photolytic initiation of the oxidation, and identify isomeric species by their photoionization spectra. The relative yields of oxygenated product isomers (2,2-dimethyloxirane, methylpropanal, and 3-methyloxetane) are in reasonable concord with measurements from Walker and co-workers (J. Chem. Soc. Faraday Trans. 74 (1) (1978) 2229-2251) at higher temperature. Oxidation of isotopically labeled isobutane, (CH3)(3)CD, suggests that methylpropanal formation can proceed from both (CH3)(2)CCH2OOH and CH3CH(CH2)CH2OOH isomers. Bimodal time behavior is observed for product formation; the initial prompt formation reflects "formally direct" channels, principally chemical activation, and the longer-timescale "delayed" component arises from dissociation of thermalized ROO and QOOH radicals. The proportion of prompt to delayed signal is smaller for the oxygenated products than for the isobutene product. This channel-specific behavior can be qualitatively understood by considering the different energetic distributions of ROO and QOOH in formally direct vs. thermal channels and the fact that the transition states involved in the formation of oxygenated products are "tighter" than that for isobutene formation. (C) 2012 Published by Elsevier Inc. on behalf of The Combustion Institute. C1 [Eskola, Arkke J.; Welz, Oliver; Savee, John D.; 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, 7011 East Ave,MS 9055, Livermore, CA 94551 USA. EM cataatj@sandia.gov RI Welz, Oliver/C-1165-2013 OI Welz, Oliver/0000-0003-1978-2412 FU Saudi Aramco "Kinetics Cluster of Excellence"; Sandia National Laboratories; Aramco Services Company, a U.S.-based subsidiary of Saudi Aramco, the state-owned national oil company of Saudi Arabia, ASC [CRADA SC10/01773.00, 6500007287]; Office of Science, Office of Basic Energy Sciences of the U. S. Department of Energy (BES/USDOE) [DE-AC02-05CH11231]; Division of Chemical Sciences, Geosciences, and Biosciences, BES/USDOE; National Nuclear Security Administration; [DE-AC04-94-AL85000] FX This work was supported as part of the Saudi Aramco "Kinetics Cluster of Excellence" under a cooperative research and development agreement (CRADA) between Sandia National Laboratories and Aramco Services Company, a U.S.-based subsidiary of Saudi Aramco, the state-owned national oil company of Saudi Arabia (CRADA SC10/01773.00, ASC Contract No. 6500007287). The Advanced Light Source is supported by the Director, Office of Science, Office of Basic Energy Sciences of the U. S. Department of Energy (BES/USDOE) under Contract No. DE-AC02-05CH11231 at Lawrence Berkeley National Laboratory. JDS and DLO are supported by the Division of Chemical Sciences, Geosciences, and Biosciences, BES/USDOE. Sandia is a multi-program laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the National Nuclear Security Administration under contract DE-AC04-94-AL85000. NR 29 TC 3 Z9 3 U1 3 U2 41 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 385 EP 392 DI 10.1016/j.proci.2012.06.116 PN 1 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065CN UT WOS:000313125400030 ER PT J AU Liu, W Sivaramakrishnan, R Davis, MJ Som, S Longman, DE Lu, TF AF Liu, W. Sivaramakrishnan, R. Davis, Michael J. Som, S. Longman, D. E. Lu, T. F. TI Development of a reduced biodiesel surrogate model for compression ignition engine modeling SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Ab initio; Transition state theory; Mechanism reduction; Methyl butanoate; Diesel spray combustion ID CHEMICAL KINETIC MECHANISMS; TRANSITION-STATE-THEORY; METHYL BUTANOATE; RATE CONSTANTS; AB-INITIO; THERMAL-DECOMPOSITION; FLAME PROPAGATION; PREMIXED FLAMES; SHOCK-TUBE; COMBUSTION AB Methylbutanoate (MB), a C-4 methyl ester, represents the simplest surrogate that captures the chemical effects of the ester moiety in biodiesel and biodiesel surrogates. An updated chemical kinetic model has been developed to characterize the ignition and flame characteristics of MB. The mechanistic elements within this model that relate to the MB and smaller ester/oxygenate sub-mechanisms are drawn from the prototypical Fisher et al. model and from more recent theory and modeling efforts. The MB model development which is based on an iterative procedure involving global sensitivity analyses to identify elementary reactions that govern ignition and subsequent high level ab initio based theoretical updates to these reaction rates are presented. The MB model makes reasonable predictions of ignition delays and laminar flame speeds. The C-5-C-7 submechanisms from the LLNL n-heptane (NH) model were merged with the present MB model to obtain a detailed chemical kinetics model for a surrogate blend representing biodiesel. The detailed MB-NH model (661 species) was reduced using graph based techniques. The robust reduction techniques employed result in a reduced model (145 species) that is in good agreement with the detailed model over a wide range of conditions. 3-D compression ignition (CI) engine simulations utilizing this reduced chemistry model for MB-NH blends as a surrogate for biodiesel show good agreement with the experimental data suggesting the utility of this model for predictions of combustion and emission characteristics of biodiesel in realistic CI engine simulations. (C) 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Liu, W.; Sivaramakrishnan, R.; Davis, Michael J.] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. [Som, S.; Longman, D. E.] Argonne Natl Lab, Div Energy Syst, Argonne, IL 60439 USA. [Lu, T. F.] Univ Connecticut, Dept Mech Engn, Storrs, CT 06269 USA. RP Sivaramakrishnan, R (reprint author), Argonne Natl Lab, Chem Sci & Engn Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM raghu@anl.gov; ssom@anl.gov RI SIVARAMAKRISHNAN, RAGHU/C-3481-2008; Lu, Tianfeng/D-7455-2014 OI SIVARAMAKRISHNAN, RAGHU/0000-0002-1867-1254; Lu, Tianfeng/0000-0001-7536-1976 FU U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences [DE-AC02-06CH11357]; National Science Foundation [0904771] FX This work was supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences, under Contract No. DE-AC02-06CH11357. The work at UConn was supported by the National Science Foundation under Grant 0904771. NR 60 TC 26 Z9 26 U1 4 U2 50 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 401 EP 409 DI 10.1016/j.proci.2012.05.090 PN 1 PG 9 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065CN UT WOS:000313125400032 ER PT J AU Darcy, D Mehl, M Simmie, JM Wurmel, J Metcalfe, WK Westbrook, CK Pitz, WJ Curran, HJ AF Darcy, D. Mehl, M. Simmie, J. M. Wuermel, J. Metcalfe, W. K. Westbrook, C. K. Pitz, W. J. Curran, H. J. TI An experimental and modeling study of the shock tube ignition of a mixture of n-heptane and n-propylbenzene as a surrogate for a large alkyl benzene SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Shock tube; Oxidation; n-Propylbenzene; n-Heptane; Alkylbenzene ID HIGH-PRESSURE; AUTO-IGNITION; OXIDATION; BUTYLBENZENE; TEMPERATURES; AUTOIGNITION; PROPENE AB Alkyl aromatics are an important chemical class in gasoline, jet and diesel fuels. In the present work, an n-propylbenzene and n-heptane mixture is studied as a possible surrogate for large alkyl benzenes contained in diesel fuels. To evaluate it as a surrogate, ignition delay times have been measured in a heated high pressure shock tube (HPST) for a mixture of 57% n-propylbenzene/43% n-heptane in air (approximate to 21% O-2, approximate to 79% N-2) at equivalence ratios of 0.29, 0.49, 0.98 and 1.95 and compressed pressures of 1, 10 and 30 atm over a temperature range of 1000-1600 K. The effects of reflected-shock pressure and equivalence ratio on ignition delay time were determined and common trends highlighted. A combined n-propylbenzene and n-heptane reaction mechanism was assembled and simulations of the shock tube experiments were carried out. The simulation results showed very good agreement with the experimental data for ignition delay times. Sensitivity and reaction pathway analyses have been performed to reveal the important reactions responsible for fuel oxidation under the shock tube conditions studied. It was found that at 1000 K, the main consumption pathways for n-propylbenzene are abstraction reactions on the alkyl chain, with particular selectivity to the allylic site. In comparison at 1500 K, the unimolecular decomposition of the fuel is the main consumption pathway. (C) 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Darcy, D.] NUI Galway, Sch Chem, Combust Chem Ctr, Galway, Ireland. [Mehl, M.; Westbrook, C. K.; Pitz, W. J.] Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. RP Darcy, D (reprint author), NUI Galway, Sch Chem, Combust Chem Ctr, Galway, Ireland. EM d.darcy2@nuigalway.ie RI Mehl, Marco/A-8506-2009; OI Mehl, Marco/0000-0002-2227-5035; Curran, Henry/0000-0002-5124-8562 FU Saudi Arabian Oil Company; US Department of Energy by Lawrence Livermore National Laboratory [DE-AC52-07NA27344]; US Department of Energy, Office of Vehicle Technologies FX NUIG acknowledge the financial support of the Saudi Arabian Oil Company. The LLNL work was performed under the auspices of the US Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344 and was supported by the US Department of Energy, Office of Vehicle Technologies (program manager Gurpreet Singh). NR 30 TC 11 Z9 11 U1 0 U2 31 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 411 EP 418 DI 10.1016/j.proci.2012.06.131 PN 1 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065CN UT WOS:000313125400033 ER PT J AU Campbell, MF Davidson, DF Hanson, RK Westbrook, CK AF Campbell, M. F. Davidson, D. F. Hanson, R. K. Westbrook, C. K. TI Ignition delay times of methyl oleate and methyl linoleate behind reflected shock waves SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Biodiesel fuel; Aerosol shock tube; Ignition delay time; Methyl oleate; Methyl linoleate ID JET-STIRRED REACTOR; BIODIESEL; OXIDATION; PRESSURE; DIESEL; FUELS; AUTOIGNITION; COMBUSTION; MECHANISMS; PYROLYSIS AB Ignition delay times for methyl oleate (C19H36O2, CAS: 112-62-9) and methyl linoleate (C19H34O2, CAS: 112-63-0) were measured for the first time behind reflected shock waves, using an aerosol shock tube. The aerosol shock tube enabled study of these very-low-vapor-pressure fuels by introducing a spatially-uniform fuel aerosol/4% oxygen/argon mixture into the shock tube and employing the incident shock wave to produce complete fuel evaporation, diffusion, and mixing. Reflected shock conditions covered temperatures from 1100 to 1400 K, pressures of 3.5 and 7.0 atm, and equivalence ratios from 0.6 to 2.4. Ignition delay times for both fuels were found to be similar over a wide range of conditions. The most notable trend in the observed ignition delay times was that the pressure and equivalence ratio scaling were a strong function of temperature, and exhibited cross-over temperatures at which there was no sensitivity to either parameter. Data were also compared to the biodiesel kinetic mechanism of Westbrook et al. (2011) [10], which underpredicts ignition delay times by about 50%. Differences between experimental and computed ignition delay times were strongly related to existing errors and uncertainties in the thermochemistry of the large methyl ester species, and when these were corrected, the kinetic simulations agreed significantly better with the experimental measurements. (C) 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Campbell, M. F.; Davidson, D. F.; Hanson, R. K.] Stanford Univ, Dept Mech Engn, Stanford, CA 94305 USA. [Westbrook, C. K.] Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. RP Campbell, MF (reprint author), 452 Escondido Mall,Bldg 520,Room 520I, Stanford, CA 94305 USA. EM matthew.campbell@stanford.edu RI Campbell, Matthew/C-2525-2015 OI Campbell, Matthew/0000-0002-7611-0332 FU Combustion Energy Frontier Research Center; U.S. Department of Energy, Office of Basic Energy Sciences [DE-SC0001198]; Air Force Office of Scientific Research; National Defense Science and Engineering Graduate (NDSEG) Fellowship [32 CFR 168a]; U.S. Department of Energy by Lawrence Livermore National Laboratory [DE-AC52-07NA27344] FX This work was supported by the Combustion Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Basic Energy Sciences under Award Number DE-SC0001198, and the Air Force Office of Scientific Research. FC is supported by a National Defense Science and Engineering Graduate (NDSEG) Fellowship, 32 CFR 168a. Part of this work (CKW) was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344. NR 25 TC 25 Z9 25 U1 1 U2 29 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 419 EP 425 DI 10.1016/j.proci.2012.05.084 PN 1 PG 7 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065CN UT WOS:000313125400034 ER PT J AU Yang, B Westbrook, CK Cool, TA Hansen, N Kohse-Hoinghaus, K AF Yang, B. Westbrook, C. K. Cool, T. A. Hansen, N. Kohse-Hoeinghaus, K. TI Photoionization mass spectrometry and modeling study of premixed flames of three unsaturated C5H8O2 esters SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Unsaturated esters; C5H8O2 isomers; Photoionization mass spectrometry; Premixed flames ID LOW-PRESSURE FLAMES; CROSS-SECTIONS; METHYL BUTANOATE; COMBUSTION CHEMISTRY; BIODIESEL SURROGATE; ETHYL PROPANOATE; DIESEL-ENGINES; RICH FLAMES; OXIDATION; ISOMERS AB The detailed chemical structures of low-pressure premixed laminar flames fueled by three simple unsaturated C5H8O2 esters, the methyl crotonate (MC), methyl methacrylate (MMA), and ethyl propenoate (EPE), are investigated using tunable synchrotron vacuum ultraviolet (VUV) photoionization mass spectrometry. Significant differences in the compositions of key reaction intermediates between these flames under similar flame conditions are observed. The results enable further refinement and validation of a detailed chemical kinetic reaction mechanism, which is largely based on a previous model for saturated esters. Detailed kinetic modeling describes how these differences are related to molecular structures, leading to unique fuel destruction pathways for each of these isomers. Meanwhile, the effect of carbon carbon double bonds on the combustion chemistry of small fatty acid esters is addressed. (C) 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Yang, B.; Cool, T. A.] Cornell Univ, Sch Appl & Engn Phys, Ithaca, NY 14853 USA. [Westbrook, C. K.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. [Hansen, N.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. [Kohse-Hoeinghaus, K.] Univ Bielefeld, Dept Chem, D-33615 Bielefeld, Germany. RP Westbrook, CK (reprint author), Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. EM westbrookck@earthlink.net RI Hansen, Nils/G-3572-2012; Kohse-Hoinghaus, Katharina/A-3867-2012; Yang, Bin/A-7158-2008 OI Yang, Bin/0000-0001-7333-0017 FU Office of Basic Energy Sciences (BES), U.S. Department of Energy (USDOE) [DE-FG02-01ER1518, DE-AC52-07NA27344]; Deutsche Forschungsgemeinschaft [KO 1363/18-3]; Sandia Corporation [DE-AC04-94-AL85000]; USDOE, Office of Basic Energy Sciences under the Energy Frontier Research Center for Combustion Science [DE-SC0001198]; Office of Science, BES/USDOE [DE-AC02-05CH11231] FX We thank Paul Fugazzi and Sarah Ferrell for expert technical assistance and Juan Wang, Tina Kasper, Patrick Osswald and Wenjun Li for experimental assistance. This work is supported by the Office of Basic Energy Sciences (BES), U.S. Department of Energy (USDOE), under grant DE-FG02-01ER1518 at Cornell University (TAC), under contract DE-AC52-07NA27344 at the Lawrence Livermore National Laboratory (CKW), by the Deutsche Forschungsgemeinschaft under KO 1363/18-3 (KKH) and by the Sandia Corporation for NNSA under contract DE-AC04-94-AL85000. BY and NH are also supported by the USDOE, Office of Basic Energy Sciences under the Energy Frontier Research Center for Combustion Science (Grant No. DE-SC0001198). The Advanced Light Source is supported by the Director, Office of Science, BES/USDOE under Contract No. DE-AC02-05CH11231. NR 47 TC 15 Z9 15 U1 5 U2 59 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 443 EP 451 DI 10.1016/j.proci.2012.05.034 PN 1 PG 9 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065CN UT WOS:000313125400037 ER PT J AU Peukert, SL Sivaramakrishnan, R Su, MC Michael, JV AF Peukert, S. L. Sivaramakrishnan, R. Su, M. -C. Michael, J. V. TI High temperature rate constants for H/D plus methyl formate and methyl acetate SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Shock tube; Abstraction; Ab initio; Transition state theory; Kinetic isotope effects ID TRANSITION-STATE-THEORY; PRESSURE RATE-CONSTANT; COEFFICIENTS; PHOTOLYSIS; MOLECULES; KINETICS; FLASH; H-2 AB The reactions of D/H with methyl formate (MF) and methyl acetate (MA) have been studied with both shock-tube experiments and ab initio transition state theoretical calculations. D-atom profiles were measured behind reflected shock waves using D-atom atomic resonance absorption spectrometry (ARAS) over the temperature range 1050-1270 K, at pressures congruent to 0.5 atm. The title reactions have been theoretically studied at the CCSD(T)/cc-pv infinity z//MP2/aug-cc-pvtz and CCSD(T)/cc-pv infinity z//B3LYP/6-311++ G(d, p) levels of theory. Theoretical calculations suggest the dominance of the abstraction processes in comparison to addition processes in the 300-2000 K T-range. Over the T-range of the present experiments, the theoretically predicted isotope effects, k(D)/k(H), are near unity. D-atom depletion in the present experiments is sensitive only to the reactions, D + CH3OC(O)H -> products (A) D + CH3OC(O)CH3 -> products (B) Simulations of the measured D-atom profiles allow for determinations of total rate constants for the processes (A) and (B). In combination with results obtained from recent H-ARAS experiments from our laboratory on MF decomposition, total experimental rate constants k(A) can be described by the Arrhenius equation, k(A) = (4.47 +/- 1.54) x 10(-10) exp(-5843 +/- 416 K/T) cm(3) molecule(-1) s(-1) (1050-1270) For H/D + MF, total experimental rate constants, k(A), and branching ratios agree well with theoretical predictions. For D/H + MA, total rate constants predicted by theory are in reasonable agreement with the experimental data. The theoretical predictions are preferred for use, with k(B) represented by the modified Arrhenius equation, k(B) = 3.078 x 10 T-19(2.78) exp(-3261 K/T) cm(3) molecule(-1) s(-1) (500-2000 K) To our knowledge, the present experiments are the first direct measurements for the title reactions and the rate constants from this combined experimental/theoretical effort are recommended for use in combustion modeling. (C) 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Peukert, S. L.; Sivaramakrishnan, R.; Su, M. -C.; Michael, J. V.] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. RP Sivaramakrishnan, R (reprint author), Argonne Natl Lab, Chem Sci & Engn Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM raghu@anl.gov; jmichael@anl.gov RI SIVARAMAKRISHNAN, RAGHU/C-3481-2008; Michael, Joe/E-3907-2010 OI SIVARAMAKRISHNAN, RAGHU/0000-0002-1867-1254; FU U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences [DE-AC02-06CH11357] FX This work was supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences, under Contract No. DE-AC02-06CH11357. NR 31 TC 7 Z9 7 U1 4 U2 24 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 463 EP 471 DI 10.1016/j.proci.2012.06.006 PN 1 PG 9 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065CN UT WOS:000313125400039 ER PT J AU Welz, O Savee, JD Eskola, AJ Sheps, L Osborn, DL Taatjes, CA AF Welz, Oliver Savee, John D. Eskola, Arkke J. Sheps, Leonid Osborn, David L. Taatjes, Craig A. TI Low-temperature combustion chemistry of biofuels: Pathways in the low-temperature (550-700 K) oxidation chemistry of isobutanol and tert-butanol SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Low-temperature oxidation; Synchrotron photoionization mass spectrometry; Alcohols; Butanol; Kinetics ID N-BUTANOL; OXYGENATED HYDROCARBONS; ELEMENTARY REACTIONS; MASS-SPECTROMETRY; LOW-PRESSURE; RADICALS; KINETICS; IGNITION; O-2; DECOMPOSITION AB Butanol isomers are promising next-generation biofuels. Their use in internal combustion applications, especially those relying on low-temperature autoignition, requires an understanding of their low-temperature combustion chemistry. Whereas the high-temperature oxidation chemistry of all four butanol isomers has been the subject of substantial experimental and theoretical efforts, their low-temperature oxidation chemistry remains underexplored. In this work we report an experimental study on the fundamental low-temperature oxidation chemistry of two butanol isomers, tert-butanol and isobutanol, in low-pressure (4-5.1 Torr) experiments at 550 and 700 K. We use pulsed-photolytic chlorine atom initiation to generate hydroxyalkyl radicals derived from tert-butanol and isobutanol, and probe the chemistry of these radicals in the presence of an excess of O-2 by multiplexed time-resolved tunable synchrotron photoionization mass spectrometry. Isomer-resolved yields of stable products are determined, providing insight into the chemistry of the different hydroxyalkyl radicals. In isobutanol oxidation, we find that the reaction of the alpha-hydroxyalkyl radical with O-2 is predominantly linked to chain-terminating formation of HO2. The Waddington mechanism, associated with chain-propagating formation of OH, is the main product channel in the reactions of O-2 with beta-hydroxyalkyl radicals derived from both tert-butanol and isobutanol. In the tert-butanol case, direct HO2 elimination is not possible in the beta-hydroxyalkyl + O-2 reaction because of the absence of a beta C-H bond; this channel is available in the beta-hydroxyalkyl + O-2 reaction for isobutanol, but we find that it is strongly suppressed. Observed evolution of the main products from 550 to 700 K can be qualitatively explained by an increasing role of hydroxyalkyl radical decomposition at 700 K. (C) 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Welz, Oliver; Savee, John D.; Eskola, Arkke J.; Sheps, Leonid; Osborn, David L.; Taatjes, Craig A.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. RP Welz, O (reprint author), Sandia Natl Labs, Combust Res Facil, Mail Stop 9055, Livermore, CA 94551 USA. EM onwelz@sandia.gov; cataatj@sandia.gov RI Welz, Oliver/C-1165-2013 OI Welz, Oliver/0000-0003-1978-2412 FU Division of Chemical Sciences, Geosciences, and Biosciences, the Office of Basic Energy Sciences, United States Department of Energy (U.S. DOE); U.S. DOE [DE-AC04-94AL85000]; Office of Science, Office of Basic Energy Sciences, Materials Sciences Division, of the U.S. DOE [DE-AC02-05CH11231]; Lawrence Berkeley National Laboratory; U.S. DOE FX We thank Howard Johnsen (Sandia) and the staff at the Chemical Dynamics Beamline for technical support. This work is funded by the Division of Chemical Sciences, Geosciences, and Biosciences, the Office of Basic Energy Sciences, United States Department of Energy (U.S. DOE). Sandia is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the U.S. DOE, under contract DE-AC04-94AL85000. The Advanced Light Source is supported by the Director, Office of Science, Office of Basic Energy Sciences, Materials Sciences Division, of the U. S. DOE, also under contract DE-AC02-05CH11231 between Lawrence Berkeley National Laboratory and the U.S. DOE. NR 38 TC 25 Z9 25 U1 4 U2 57 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 493 EP 500 DI 10.1016/j.proci.2012.05.058 PN 1 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065CN UT WOS:000313125400042 ER PT J AU Zhou, CW Klippenstein, SJ Simmie, JM Curran, HJ AF Zhou, Chong-Wen Klippenstein, Stephen J. Simmie, John M. Curran, Henry J. TI Theoretical kinetics for the decomposition of iso-butanol and related (CH3)(2) (C) over dotH plus (C) over dotH(2)OH reactions SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Iso-butanol; Thermal decomposition; Ab initio; Variable-reaction-coordinate transition state theory ID TRANSITION-STATE THEORY; GAUSSIAN-BASIS SETS; THERMAL-DECOMPOSITION; MOLECULAR CALCULATIONS; PREDICTIVE THEORY; REACTION-PATH; LOOSENESS; RADICALS; ETHANOL; DISSOCIATIONS AB The potential energy surface for the thermal decomposition of iso-butanol has been investigated using high level ab initio electronic structure methods. Temperature and pressure dependent rate coefficients for the three channels with the lower energy barriers, forming (CH3)(2)(C)over dotH + (C) over dotH(2)OH (k(1)), CH3(C)over dotHCH(2)OH + (C) over dotH(3) (k(2)) and (CH3)(2)C=CH2 + H2O (k(3)) were computed with the master equation method employing ab initio transition state theory estimates for the microcanonical rate coefficients. The two radical forming channels were treated with variable-reaction-coordinate transition state theory employing directly sampled CASPT2(2e, 2o)/cc-pVDZ orientation dependent interaction energies coupled with one-dimensional basis set and relaxation corrections. The other channel was treated with conventional TST including Eckart tunneling and one-dimensional hindered rotor corrections. For temperatures higher than 1000 K and pressures of 1 Torr or greater, the direct C-C bond fission forming (CH3)(2)(C) over dotH + CH2OH is dominant, while the formations of CH3(C)HCH2OH vertical bar (C) over dot H-3 and (CH3)(2)C = CH2 + H-2 together contribute less than 20%. The bi-molecular recombination of (CH3)(2) (C) over dotH + (C) over dotH(2)OH has also been investigated, with the formation of iso-butanol found to be dominant at high pressure and the production of CH3(C) over dotHCH(2)OH + (C) over dot H-3 favored at low pressure. (C) 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Zhou, Chong-Wen; Simmie, John M.; Curran, Henry J.] NUI Galway, Combust Chem Ctr, Galway, Ireland. [Klippenstein, Stephen J.] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. RP Zhou, CW (reprint author), NUI Galway, Combust Chem Ctr, Galway, Ireland. EM chongwen.zhou@nuigalway.ie FU Science Foundation Ireland [08/IN1./I2055]; Combustion Energy Frontier Research Center by the Division of Chemical Sciences, Geosciences, and Biosciences, the Office of Basic Energy Sciences, the U.S. Department of Energy [DE-SC0001198, DE-AC02-06CH11357] FX This material is based upon works supported by Science Foundation Ireland under Grant No. [08/IN1./I2055]. Computational resources were provided by the e-Irish National Infra Structure, e-INIS, programme, and, the Irish Centre for High-End Computing, ICHEC. The work at Argonne was supported as part of the Combustion Energy Frontier Research Center under award number DE-SC0001198 by the Division of Chemical Sciences, Geosciences, and Biosciences, the Office of Basic Energy Sciences, the U.S. Department of Energy, under contract number DE-AC02-06CH11357. NR 41 TC 11 Z9 11 U1 1 U2 37 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 501 EP 509 DI 10.1016/j.proci.2012.06.034 PN 1 PG 9 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065CN UT WOS:000313125400043 ER PT J AU Zador, J Miller, JA AF Zador, Judit Miller, James A. TI Unimolecular dissociation of hydroxypropyl and propoxy radicals SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Propanol; Master equation; Pressure-dependence; Formally direct; Alcohol ID TRANSITION-STATE THEORY; STIRRED REACTOR JSR; RATE CONSTANTS; COMBUSTION BOMB; MASTER EQUATION; N-PROPANOL; DECOMPOSITION; TEMPERATURE; OH; AUTOIGNITION AB Unimolecular pressure- and temperature-dependent decomposition rate coefficients of radicals derived from n- and i-propanol by H-atom abstraction are calculated using a time-dependent master equation in the 300-2000 K temperature range. The calculations are based on a C3H7O potential energy surface, which was previously tested successfully for the propene + OH reaction. All rate coefficients are obtained with internal consistency with particular attention paid to shallow wells. After minor adjustments very good agreement with the few available experimental results is obtained. Several interesting pathways are uncovered, such as the catalytic dehydration, well-skipping reactions and reactions forming enols. The results of the calculations can be readily used in CHEMKIN simulations or to assess important channels for higher alcohols. (C) 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Zador, Judit] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. [Miller, James A.] Argonne Natl Lab, Div Chem, Argonne, IL 60439 USA. RP Zador, J (reprint author), Sandia Natl Labs, Combust Res Facil, Mail Stop 9055, Livermore, CA 94551 USA. EM jzador@sandia.gov RI Zador, Judit/A-7613-2008 OI Zador, Judit/0000-0002-9123-8238 FU Division of Chemical Sciences, Geosciences, and Biosciences, the Office of Basic Energy Sciences, the U.S. Department of Energy under DOE [DE-AC04-94AL85000]; ASC-HPCC [DE-AC02-2006CH11357, 59044] FX 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 under DOE Contract Number DE-AC04-94AL85000. J. A. M. is supported under Contract Number DE-AC02-2006CH11357 of the same agency as part of the ASC-HPCC (ANL FWP # 59044). Sandia is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the National Nuclear Security Administration. NR 36 TC 5 Z9 5 U1 1 U2 33 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 519 EP 526 DI 10.1016/j.proci.2012.06.172 PN 1 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065CN UT WOS:000313125400045 ER PT J AU Burke, MP Klippenstein, SJ Harding, LB AF Burke, Michael P. Klippenstein, Stephen J. Harding, Lawrence B. TI A quantitative explanation for the apparent anomalous temperature dependence of OH + HO2 = H2O + O-2 through multi-scale modeling SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Optimization; Uncertainty quantification; Multi-scale modeling; Hydrogen peroxide; Ab initio transition state theory ID DETAILED KINETIC-MODEL; RATE-CONSTANT; SHOCK-TUBE; PRESSURE-DEPENDENCE; COMBUSTION; HO2; OPTIMIZATION; UNCERTAINTY; PARAMETERS; METHANE AB Kinetic models for complex chemical mechanisms are comprised of tens to thousands of reactions with rate constants informed by data from a wide variety of sources - rate constant measurements, global combustion experiments, and theoretical kinetics calculations. In order to integrate information from distinct data types in a self-consistent manner, a framework for combustion model development is presented that encapsulates behavior across a wide range of chemically relevant scales from fundamental molecular interactions to global combustion phenomena. The resulting kinetic model consists of a set of theoretical kinetics parameters (with constrained uncertainties), which are related through kinetics calculations to temperature/pressure/bath-gas-dependent rate constants (with propagated uncertainties), which in turn are related through physical models to combustion behavior (with propagated uncertainties). Direct incorporation of theory in combustion model development is expected to yield more reliable extrapolation of limited data to conditions outside the validation set, which is particularly useful for extrapolating to engine-relevant conditions where relatively limited data are available. Several key features of the approach are demonstrated for the H2O2 decomposition mechanism, where a number of its constituent reactions continue to have large uncertainties in their temperature and pressure dependence despite their relevance to high-pressure, low-temperature combustion of a variety of fuels. Here, we use the approach to provide a quantitative explanation for the apparent anomalous temperature dependence of OH + HO2 = H2O + O-2 - in a manner consistent with experimental data from the entire temperature range and ab initio transition-state theory within their associated uncertainties. Interestingly, we do find a rate minimum near 1200 K, although the temperature dependence is substantially less pronounced than previously suggested. (C) 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Burke, Michael P.; Klippenstein, Stephen J.; Harding, Lawrence B.] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. RP Burke, MP (reprint author), Argonne Natl Lab, Chem Sci & Engn Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM mpburke@anl.gov OI Klippenstein, Stephen/0000-0001-6297-9187 FU Argonne National Lab; U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences [DE-AC02-06CH11357] FX This work was supported by a Director's Post-doctoral Fellowship from Argonne National Lab and by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences, under Contract No. DE-AC02-06CH11357. The authors would also like to thank Dr. Zekai Hong for providing the raw data from [27,36,37]. NR 51 TC 24 Z9 24 U1 2 U2 61 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 547 EP 555 DI 10.1016/j.proci.2012.05.041 PN 1 PG 9 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065CN UT WOS:000313125400048 ER PT J AU Prager, J Najm, HN Zador, J AF Prager, Jens Najm, Habib N. Zador, Judit TI Uncertainty quantification in the ab initio rate-coefficient calculation for the CH3CH(OH)CH3 + OH -> CH3C center dot(OH)CH3 + H2O reaction SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Uncertainty analysis; Bayesian inference; H-abstraction; Alcohol; Autoignition ID MOLECULE REACTIONS; CHEMICAL KINETICS; OH; DECOMPOSITION; 2-PROPANOL; ALCOHOLS; ETHANOL; MODEL AB Theoretical methods to obtain rate coefficients are essential to fundamental combustion chemistry research, yet the associated uncertainties are largely unexplored in a systematic manner. In this paper we focus on the study of parametric uncertainties for a hydrogen-atom-abstraction reaction, CH3CH(OH)CH3 + OH -> CH3C center dot(OH)CH3 + H2O, which bears significant importance in low-temperature alcohol combustion and especially in autoignition models. After identifying the parameters causing significant uncertainty in the rate-coefficient calculations, Bayesian inference is employed to determine the joint probability density function (PDF) thereof using the experimental data of Dunlop and Tully (1993) [6] on isopropanol + OH. The inferred PDFs are compared to the various parameter values obtained from high-level electronic-structure calculations in order to assess the limitations of current methodologies. To gain insight on modeling the kinetic isotope effect (KIE), the reaction of the hydroxyl radical with deuterated isopropanol is also investigated. (C) 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Prager, Jens; Najm, Habib N.; Zador, Judit] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. RP Zador, J (reprint author), Sandia Natl Labs, Combust Res Facil, Mail Stop 9055, Livermore, CA 94551 USA. EM jzador@sandia.gov RI Zador, Judit/A-7613-2008 OI Zador, Judit/0000-0002-9123-8238 FU Division of Chemical Sciences, Geosciences, and Biosciences, the Office of Basic Energy Sciences, the U.S. Department of Energy under DOE [DE-AC02-06CH11357] FX This work is supported by the Division of Chemical Sciences, Geosciences, and Biosciences, the Office of Basic Energy Sciences, the U.S. Department of Energy under DOE Contract Numbers DE-AC02-06CH11357. Sandia is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the National Nuclear Security Administration. The authors thank Dr. Khachik Sargsyan for providing the software library used for the Bayesian analysis, and JZ is grateful for the stimulating discussions with Dr. Ahren W. Jasper. NR 31 TC 13 Z9 13 U1 4 U2 38 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 583 EP 590 DI 10.1016/j.proci.2012.06.078 PN 1 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065CN UT WOS:000313125400052 ER PT J AU Tranter, RS Lynch, PT Yang, XL AF Tranter, Robert S. Lynch, Patrick T. Yang, Xueliang TI Dissociation of dimethyl ether at high temperatures SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Dimethyl ether; Shock tube; Roaming ID THERMAL-DECOMPOSITION; SHOCK-WAVES; REACTION-KINETICS; FLOW REACTORS; PYROLYSIS; OXIDATION; TUBE; RADICALS AB The decomposition of dimethyl ether (CH3OCH3) has been investigated behind incident shock waves in a diaphragmless shock tube using laser schlieren densitometry, LS (T = 1500-2450 K, P = 57 +/- 4, 125 +/- 5 and 253 +/- 12 Torr). The LS density gradient profiles were simulated and excellent agreement was found between the simulations and experimental profiles. Rate coefficients for CH3OCH3 -> CH3O + CH3 were obtained. They showed strong fall-off, and at the lower end of the experimental temperature range are close to the low pressure limit. First order rate coefficient expressions were determined over 1500 < T < 2450 K. k(57Torr) = (3.10 +/- 1.0) x 10(79)T(-19.03) exp(-54417/T) s(-1), k(125Torr) = (1.12 +/- 0.3) x 10(83) T-19.94 exp(-55554/T) s(-1) and k(253Torr) = (1.02 +/- 0.3) x 10(73)T(-17.09) exp(-51500/T) s(-1). The effect of a roaming channel for decomposition of dimethyl ether was assessed and the best agreement was obtained with 1% dissociation of DME via the roaming path. (C) 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Tranter, Robert S.; Lynch, Patrick T.; Yang, Xueliang] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. RP Tranter, RS (reprint author), Argonne Natl Lab, Chem Sci & Engn Div, Bldg 200, Argonne, IL 60439 USA. EM tranter@anl.gov FU Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences, U.S. Department of Energy [DE-AC02-06CH11357] FX This work was performed under the auspices of the Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences, U.S. Department of Energy, under contract number DE-AC02-06CH11357. NR 27 TC 9 Z9 9 U1 1 U2 52 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 591 EP 598 DI 10.1016/j.proci.2012.05.021 PN 1 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065CN UT WOS:000313125400053 ER PT J AU Veloo, PS Dagaut, P Togbe, C Dayma, G Sarathy, SM Westbrook, CK Egolfopoulos, FN AF Veloo, P. S. Dagaut, P. Togbe, C. Dayma, G. Sarathy, S. M. Westbrook, C. K. Egolfopoulos, F. N. TI Jet-stirred reactor and flame studies of propanal oxidation SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Kinetics; Jet-stirred reactor; Flame propagation; Modeling; Propanal ID GAS-PHASE; COMBUSTION; PROPIONALDEHYDE; 1-PROPANOL; ALDEHYDES AB There is a strong drive towards utilizing oxygenated biofuels in blends with existing fossil fuels. Improving the kinetic modeling of the oxidation of these bio-derived oxygenates requires further investigation of their key stable intermediates such as the aldehydes. In this study, an experimental and chemical kinetic modeling investigation of propanal oxidation was carried out. Experiments were conducted in a jet stirred reactor and in counterflow flames over a wide range of equivalence ratios, temperatures, and ambient pressures. Stable species concentration profiles were measured in the jet stirred reactor and laminar flame speeds were measured. A detailed chemical kinetic reaction model was validated using the present experimental results and existing literature data. The model was used also to provide insight into the controlling reaction pathways for propanal oxidation in both the low- and high-temperature kinetic regimes. (C) 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Veloo, P. S.] Princeton Univ, Dept Mech & Aerosp Engn, Princeton, NJ 08544 USA. [Dagaut, P.; Togbe, C.; Dayma, G.] CNRS INSIS, 1C, F-45071 Orleans 2, France. [Sarathy, S. M.; Westbrook, C. K.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. [Egolfopoulos, F. N.] Univ So Calif, Dept Aerosp & Mech Engn, Los Angeles, CA 90089 USA. RP Veloo, PS (reprint author), Princeton Univ, Dept Mech & Aerosp Engn, Princeton, NJ 08544 USA. EM pveloo@princeton.edu RI Veloo, Peter/G-1196-2010; Dagaut, Philippe/C-1709-2008; Sarathy, S. Mani/M-5639-2015; OI Veloo, Peter/0000-0003-1135-4018; Dagaut, Philippe/0000-0003-4825-3288; Sarathy, S. Mani/0000-0002-3975-6206; Egolfopoulos, Fokion/0000-0002-7115-5304; Dayma, Guillaume/0000-0003-2761-657X FU ERC [291049-2G-Csafe]; U.S. Department of Energy [DE-AC52-07NA27344]; CEFRC, an Energy Frontier Research Center; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001198] FX The work at CNRS was supported by the ERC Advanced Researcher Grant No. 291049-2G-Csafe. The work at LLNL was performed under the auspices of the U.S. Department of Energy under Contract DE-AC52-07NA27344. The work performed at USC was supported as part of the CEFRC, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Award Number DE-SC0001198. Discussions with Drs. Pascal Dievart and David A. Sheen are greatly appreciated. NR 30 TC 22 Z9 22 U1 3 U2 37 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 599 EP 606 DI 10.1016/j.proci.2012.06.138 PN 1 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065CN UT WOS:000313125400054 ER PT J AU Goos, E Sickfeld, C Mauss, F Seidel, L Ruscic, B Burcat, A Zeuch, T AF Goos, Elke Sickfeld, Christina Mauss, Fabian Seidel, Lars Ruscic, Branko Burcat, Alexander Zeuch, Thomas TI Prompt NO formation in flames: The influence of NCN thermochemistry SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE NCN heat of formation; NCN thermochemistry; Prompt NO formation; Methane flames; Acetylene flame ID CHEMISTRY-GUIDED-REDUCTION; INITIO CHEMICAL-KINETICS; AB-INITIO; COMBUSTION CHEMISTRY; REACTION-MECHANISM; RATE-CONSTANT; OXIDATION; PRESSURE; SINGLET; TABLES AB The influence of the route via the NCN radical on NO formation in flames was examined from a thermochemistry and reaction kinetics perspective. A detailed analysis of available experimental and theoretical thermochemical data combined with an Active Thermochemical Tables analysis suggests a heat of formation of 457.8 +/- 2.0 kJ/mol for NCN, consistent with carefully executed theoretical work of Harding et al. (2008) [5]. This value is significantly different from other previously reported experimental and theoretical values. A combination of an extensively validated comprehensive hydrocarbon oxidation model extended by the GDFkin3.0_NCN-NOx sub-mechanism reproduced NCN and NO mole fraction profiles in a recently characterized fuel-rich methane flame only when heat of formation values in the range of 445-453 kJ/mol are applied. Sensitivity analysis revealed that the sensitivities of contributing steps to NO and NCN formation are strongly dependent on the absolute value of the heat of formation of NCN being used. In all flames under study the applied NCN thermochemistry highly influences simulated NO and NCN mole fractions. The results of this work illustrate the thermochemistry constraints in the context of NCN chemistry which have to be taken into account for improving model predictions of NO concentrations in flames. (C) 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Goos, Elke] DLR, German Aerosp Ctr, Inst Combust Technol, D-70569 Stuttgart, Germany. [Sickfeld, Christina; Zeuch, Thomas] Univ Gottingen, Inst Phys Chem, D-37077 Gottingen, Germany. [Mauss, Fabian; Seidel, Lars] Brandenburg Tech Univ Cottbus, D-03046 Cottbus, Germany. [Ruscic, Branko] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. [Burcat, Alexander] Technion Israel Inst Technol, Fac Aerosp Engn, IL-32000 Haifa, Israel. RP Goos, E (reprint author), DLR, German Aerosp Ctr, Inst Combust Technol, Pfaffenwaldring 38-40, D-70569 Stuttgart, Germany. EM Elke.Goos@dlr.de; tzeuch1@gwdg.de RI Goos, Elke/D-5372-2009; Ruscic, Branko/A-8716-2008 OI Ruscic, Branko/0000-0002-4372-6990 FU Energy Program of the German Aerospace Center (DLR); Fonds der Chemischen Industrie; U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences [DE-AC02-06CH11357]; COST Action [CM0901] FX Funding by the Energy Program of the German Aerospace Center (DLR) is gratefully acknowledged by E.G. Funding by the Fonds der Chemischen Industrie is gratefully acknowledged by T.Z. The work at Argonne National Laboratory was performed under the auspices of the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences, under Contract No. DE-AC02-06CH11357. E.G., F.M., L.S. and T.Z. acknowledge support from COST Action CM0901: "Detailed chemical kinetic models for cleaner combustion". NR 65 TC 13 Z9 14 U1 0 U2 17 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 657 EP 666 DI 10.1016/j.proci.2012.06.128 PN 1 PG 10 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065CN UT WOS:000313125400061 ER PT J AU Goldsborough, SS Mittal, G Banyon, C AF Goldsborough, S. S. Mittal, G. Banyon, C. TI Methodology to account for multi-stage ignition phenomena during simulations of RCM experiments SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Multi-stage ignition; RCM; Reduced order model ID RAPID-COMPRESSION MACHINE; TEMPERATURE-FIELDS; ELEVATED PRESSURES; JET FUEL; AUTOIGNITION; OXIDATION; COMBUSTION; MECHANISM; SURROGATE; MIXTURES AB RCM experiments are used to investigate the ignition behavior of fuels at engine relevant conditions. Modern designs utilize pistons with crevice volumes machined around the circumference of the crown in order to suppress boundary layer effects during the volumetric compression process. While piston crevices have been successful in controlling heat loss from the reaction chamber gases and improving the overall homogeneity of the reacting mixture, multi-stage ignition events can be sufficiently perturbed by spatial non-uniformities and there can be substantial gas flow into the crevice volume due to the preliminary, or low-temperature heat releases. Ignition delay times can be lengthened by up to 25% as a result of these effects. These features are difficult to incorporate into 0D chemical kinetic simulations where volumetric expansion curves from non-reacting experiments are often used to prescribe the heat loss characteristics of reacting chamber mixtures. A new methodology is presented here to account for multi-stage ignition phenomena during simulations of RCM experiments. The approach and a range of demonstrative examples are presented in this study. (C) 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Goldsborough, S. S.] Argonne Natl Lab, Div Energy Syst, Argonne, IL 60439 USA. [Mittal, G.] Univ Akron, Dept Mech Engn, Akron, OH 44325 USA. [Goldsborough, S. S.; Banyon, C.] Marquette Univ, Dept Mech Engn, Milwaukee, WI 53201 USA. RP Goldsborough, SS (reprint author), Argonne Natl Lab, Div Energy Syst, 9700 S Cass Ave, Argonne, IL 60439 USA. EM scott.goldsborough@anl.gov FU NSF [CBET-0968080]; University of Akron, College of Engineering; Argonne, a U.S. Department of Energy Office of Science laboratory [DE-AC02-06CH11357] FX Funding for this work has been provided in part through NSF CBET-0968080 and the University of Akron, College of Engineering. This manuscript has been created in part by UChicago Argonne, LLC, Operator of Argonne National Laboratory ("Argonne"). Argonne, a U.S. Department of Energy Office of Science laboratory, is operated under Contract No. DE-AC02-06CH11357. the U.S. Government retains for itself, and others acting on its behalf, a paid-up non-exclusive, irrevocable worldwide license in said article to reproduce, prepare derivative works, distribute copies to the public, and perform publicly and display publicly, by or on behalf of the Government. NR 50 TC 9 Z9 9 U1 1 U2 13 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 685 EP 693 DI 10.1016/j.proci.2012.05.094 PN 1 PG 9 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065CN UT WOS:000313125400064 ER PT J AU Ji, CS Zhao, RH Li, B Egolfopoulos, FN AF Ji, Chunsheng Zhao, Runhua Li, Bo Egolfopoulos, Fokion N. TI Propagation and extinction of cyclopentadiene flames SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Flame propagation; Flame extinction; Cyclopentadiene; Aromatics; Kinetics ID SURROGATE MIXTURES; CHEMICAL-KINETICS; DIFFUSION FLAMES; FLOW REACTOR; SHOCK-TUBE; COMBUSTION; OXIDATION; JP-8; DECOMPOSITION; DERIVATIVES AB Laminar flame speeds and extinction strain rates of cyclopentadiene/air mixture were determined in the counterflow configuration at atmospheric pressure, unburned mixture temperature of 353 K, and for a wide range of equivalence ratios. The experiments were modeled using recently developed kinetic models. Sensitivity analyses showed that both flame propagation and extinction of cyclopentadiene/air mixtures flames depend notably on the fuel kinetics and subsequent intermediates such as cyclopentadienyl, cyclopentadienone, and cyclopentadienoxy. Analyses of the computed flame structures revealed that the high temperature oxidation of cyclopentadiene depends in general on the kinetics of first few intermediates in the oxidation process following the fuel consumption. The potential reaction pathways of the consumption of cyclopentadienyl radicals were discussed and further investigation and validation is recommended for two relevant reactions that could improve the high temperature oxidation kinetic model of cyclopentadiene. The experimental flame data of this study are the first ones to be reported. (C) 2012 Published by Elsevier Inc. on behalf of The Combustion Institute. C1 [Ji, Chunsheng; Zhao, Runhua; Li, Bo; Egolfopoulos, Fokion N.] Univ So Calif, Dept Aerosp & Mech Engn, Los Angeles, CA 90089 USA. [Ji, Chunsheng] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. RP Ji, CS (reprint author), Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. EM cji@sandia.gov OI Egolfopoulos, Fokion/0000-0002-7115-5304 FU Air Force Office of Scientific Research [FA9550-10-1-0087, FA9550-11-1-0217] FX The work was performed under the support on the Air Force Office of Scientific Research (Grants Nos. FA9550-10-1-0087 and FA9550-11-1-0217) under the technical supervision of Dr. Chiping Li. The authors thank Prof. R. P. Lindstedt and Dr. S.-W. Park of Imperial College London for providing their simulation results, as well as Prof. H. Wang of the University of Southern California for useful discussions regarding both the experimental and modeling aspects of this study. NR 41 TC 2 Z9 2 U1 5 U2 25 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 787 EP 794 DI 10.1016/j.proci.2012.07.047 PN 1 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065CN UT WOS:000313125400076 ER PT J AU Zhang, HY Hawkes, ER Chen, JH Kook, S AF Zhang, Haoyang Hawkes, Evatt R. Chen, Jacqueline H. Kook, Sanghoon TI A numerical study of the autoignition of dimethyl ether with temperature inhomogeneities SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Autoignition; Dimethyl ether; Direct numerical simulation; Homogeneous charge compression ignition; Thermal stratification ID IGNITION FRONT PROPAGATION; HYDROGEN-AIR MIXTURE; CONSTANT VOLUME; SIMULATION; ENGINES AB The autoignition of dimethyl ether (DME) with temperature inhomogeneities is investigated by one-dimensional numerical simulations with detailed chemistry at high pressure and a constant volume. The primary purpose of the study is to provide an understanding of the autoignition of DME in a simplified configuration that is relevant to homogeneous charge compression ignition (HCCI) engines. The ignition structure and the negative temperature coefficient (NTC) behaviour are characterised in a homogeneous domain and one-dimensional domains with thermal stratification, at different initial mean temperatures and length scales. The thermal stratification is shown to strongly affect the spatial structure and temporal progress of ignition. The importance of diffusion and conduction on the ignition progress is assessed. It is shown that the effects of molecular diffusion decay relative to those of chemical reaction as the length-scale increases. This is to be expected, however the present study shows that these characteristics also depend on the mean temperature due to NTC behaviour. For the range of conditions studied here, which encompass a range of stratification length scales expected in HCCI engines, the effects of molecular transport are found to be small compared with chemical reaction effects for mean temperatures within the NTC regime. This is in contrast to previous work with fuels with single-stage ignition behaviour where practically realisable temperature gradients can lead to molecular transport effects becoming important. In addition, thermal stratification is demonstrated to result in significant reductions of the pressure-rise rate (PRR), even for the present fuel with two-stage ignition and NTC behaviour. The reduction of PRR is however strongly dependent on the mean initial temperature. The stratification length-scale is also shown to have an important influence on the pressure oscillations, with large-amplitude oscillations possible for larger length scales typical of integral scales in HCCI engines. (C) 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Zhang, Haoyang; Hawkes, Evatt R.] Univ New S Wales, Sch Photovolta & Renewable Energy Engn, Sydney, NSW 2052, Australia. [Chen, Jacqueline H.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. [Hawkes, Evatt R.; Kook, Sanghoon] Univ New S Wales, Sch Mech & Mfg Engn, Sydney, NSW 2052, Australia. RP Zhang, HY (reprint author), Univ New S Wales, Sch Photovolta & Renewable Energy Engn, Sydney, NSW 2052, Australia. EM haoyang.zhang@unsw.edu.au RI Kook, Sanghoon/C-5372-2009; Hawkes, Evatt/C-5307-2012 OI Kook, Sanghoon/0000-0002-7620-9789; Hawkes, Evatt/0000-0003-0539-7951 FU Australian Research Council [DP110104763, FT100100536] FX This work was supported by the Australian Research Council under Grant numbers DP110104763 and FT100100536. In addition, this research benefited from the resources of the National Computational Infrastructure, Australia. NR 31 TC 14 Z9 15 U1 1 U2 29 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 803 EP 812 DI 10.1016/j.proci.2012.07.026 PN 1 PG 10 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065CN UT WOS:000313125400078 ER PT J AU Liu, N Sarathy, SM Westbrook, CK Egolfopoulos, FN AF Liu, Ning Sarathy, S. Mani Westbrook, Charles K. Egolfopoulos, Fokion N. TI Ignition of non-premixed counterflow flames of octane and decane isomers SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Flame ignition; Octane isomers; Decane isomers; Non-premixed flames; Kinetic modeling ID CONCENTRATION-TIME HISTORIES; SHOCK-TUBE MEASUREMENTS; HCCI ENGINE COMBUSTION; ISOOCTANE IGNITION; RAPID COMPRESSION; CHEMICAL-KINETICS; HEPTANE; FUELS; INTERMEDIATE; AUTOIGNITION AB Ignition temperatures of non-premixed flames of octane and decane isomers were determined in the counterflow configuration at atmospheric pressure, a free-stream fuel/N-2 mixture temperature of 401 K, a local strain rate of 130 s(-1), and fuel mole fractions ranging from 1% to 6%. The experiments were modeled using detailed chemical kinetic mechanisms for all isomers that were combined with established H-2, CO, and n-alkane models, and close agreements were found for all flames considered. The results confirmed that increasing the degree of branching lowers the ignition propensity. On the other hand, increasing the straight chain length by two carbons was found to have no measurable effect on flame ignition for symmetric branched fuel structures. Detailed sensitivity analyses showed that flame ignition is sensitive primarily to the H-2/CO and C-1-C-3 hydrocarbon kinetics for low degrees of branching, and to fuel-related reactions for the more branched molecules. (C) 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Liu, Ning; Egolfopoulos, Fokion N.] Univ So Calif, Dept Aerosp & Mech Engn, Los Angeles, CA 90089 USA. [Sarathy, S. Mani; Westbrook, Charles K.] Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. RP Liu, N (reprint author), Univ So Calif, Dept Aerosp & Mech Engn, Los Angeles, CA 90089 USA. EM ningl@usc.edu RI Sarathy, S. Mani/M-5639-2015; OI Sarathy, S. Mani/0000-0002-3975-6206; Egolfopoulos, Fokion/0000-0002-7115-5304 FU Air Force Office of Scientific Research [FA9550-10-1-0087, FA9550-11-1-0217]; U.S. Department of Energy by Lawrence Livermore National Laboratory [DE-AC52-07NA27344]; US Department of Energy; Office of Vehicle Technologies; Office of Naval Research FX The work was performed under the support on the Air Force Office of Scientific Research (Grants Nos. FA9550-10-1-0087 and FA9550-11-1-0217) under the technical supervision of Dr. Chiping Li, and under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory (Contract DE-AC52-07NA27344), with additional support from the US Department of Energy, Office of Vehicle Technologies (program manager Gurpreet Singh), and the Office of Naval Research (program manager Sharon Beermann-Curtin). NR 51 TC 12 Z9 13 U1 1 U2 21 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 903 EP 910 DI 10.1016/j.proci.2012.05.040 PN 1 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065CN UT WOS:000313125400090 ER PT J AU Sarathy, SM Niemann, U Yeung, C Gehmlich, R Westbrook, CK Plomer, M Luo, ZY Mehl, M Pitz, WJ Seshadri, K Thomson, MJ Lu, TF AF Sarathy, S. Mani Niemann, Ulrich Yeung, Coleman Gehmlich, Ryan Westbrook, Charles K. Plomer, Max Luo, Zhaoyu Mehl, Marco Pitz, William J. Seshadri, Kalyanasundaram Thomson, Murray J. Lu, Tianfeng TI A counterflow diffusion flame study of branched octane isomers SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE 3-Methylheptane; 2,5-Dimethylhexane; Counterflow diffusion flame; Ignition; Extinction ID NON-PREMIXED FLOWS; RAPID COMPRESSION; HEPTANE; SURROGATES; EXTINCTION; COMBUSTION; MECHANISM; IGNITION AB Conventional petroleum, Fischer-Tropsch (FT), and other alternative hydrocarbon fuels typically contain a high concentration of lightly methylated iso-alkanes. However, until recently little work has been done on this important class of hydrocarbon components. In order to better understand the combustion characteristics of real fuels, this study presents new experimental data for 3-methylheptane and 2,5-dimethylhexane in counterflow diffusion flames. This new dataset includes flame ignition, extinction, and speciation profiles. The high temperature oxidation of these fuels has been modeled using an extended transport database and a high temperature skeletal chemical kinetic model. The skeletal model is generated from a detailed model reduced using the directed relation graph with expert knowledge (DRG-X) methodology. The proposed skeletal model contains sufficient chemical fidelity to accurately predict the experimental speciation data in flames. The predictions are compared to elucidate the effects of number and location of the methyl substitutions. The location is found to have little effect on ignition and extinction in these counterflow diffusion flames. However, increasing the number of methyl substitutions was found to inhibit ignition and promote extinction. Chemical kinetic modelling simulations were used to correlate a fuel's extinction propensity with its ability to populate the H radical concentration. Species composition measurements indicate that the location and number of methyl substitutions was found to particularly affect the amount and type of alkenes observed. Published by Elsevier Inc. on behalf of The Combustion Institute. C1 [Sarathy, S. Mani; Westbrook, Charles K.; Mehl, Marco; Pitz, William J.] Lawrence Livermore Natl Lab, Phys & Life Sci Directorate, Div Chem Sci, Livermore, CA USA. [Niemann, Ulrich; Gehmlich, Ryan; Seshadri, Kalyanasundaram] Univ Calif San Diego, San Diego, CA 92103 USA. [Yeung, Coleman; Thomson, Murray J.] Univ Toronto, Dept Mech & Ind Engn, Toronto, ON M5S 1A1, Canada. [Plomer, Max; Luo, Zhaoyu; Lu, Tianfeng] Univ Connecticut, Storrs, CT USA. RP Sarathy, SM (reprint author), 7000 E Ave,L-367, Livermore, CA 94658 USA. EM sarathy1@llnl.gov RI Lu, Tianfeng/D-7455-2014; Niemann, Ulrich/E-4737-2015; Sarathy, S. Mani/M-5639-2015; Mehl, Marco/A-8506-2009; OI Lu, Tianfeng/0000-0001-7536-1976; Niemann, Ulrich/0000-0001-9268-5040; Sarathy, S. Mani/0000-0002-3975-6206; Mehl, Marco/0000-0002-2227-5035; Gehmlich, Ryan/0000-0003-0903-2992 FU US. Department of Energy by Lawrence Livermore National Laboratory [DE-AC52-07NA27344]; Office of Vehicle Technologies; Office of Naval Research; US Army Research Office Grant [W911NF-09-1-0108]; NSERC of Canada; National Science Foundation [0904771] FX We express gratitude to Dr. Sang Hee Won for fruitful discussions. This work was performed under the auspices of the US. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344 and acknowledges the support of the Office of Vehicle Technologies (program manager Gurpreet Singh) and the Office of Naval Research (program manager Sharon Beermann-Curtin). The research at the University of California at San Diego is supported by the US Army Research Office Grant #W911NF-09-1-0108 (Program Manager Dr. Ralph A. Anthenien Jr.) The co-authors S.M.S., C.Y., and M.J.T. acknowledge support from NSERC of Canada. The work at University of Connecticut was supported by the National Science Foundation under Grant 0904771. NR 16 TC 16 Z9 16 U1 3 U2 22 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 1015 EP 1023 DI 10.1016/j.proci.2012.05.106 PN 1 PG 9 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065CN UT WOS:000313125400103 ER PT J AU Skeen, SA Yang, B Michelsen, HA Miller, JA Violi, A Hansen, N AF Skeen, S. A. Yang, B. Michelsen, H. A. Miller, J. A. Violi, A. Hansen, N. TI Studies of laminar opposed-flow diffusion flames of acetylene at low-pressures with photoionization mass spectrometry SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Non-premixed opposed-flow flames; Flame-sampling molecular-beam mass spectrometry; Acetylene combustion chemistry; Low-pressure combustion ID RESONANCE-STABILIZED RADICALS; CROSS-SECTIONS; COMBUSTION CHEMISTRY; BENZENE FORMATION; ALIPHATIC FUELS; HYDROCARBONS; EXTINCTION; PROPANE AB We have designed an opposed-flow flame system to investigate the chemical composition of non-premixed flames using in situ flame-sampling molecular-beam mass spectrometry with synchrotron-generated tunable vacuum-ultraviolet light as an ionization source. This paper provides details of the experimental apparatus, sampling method, and data-reduction procedures. To test the system, we have investigated the chemical composition of three low-pressure (30-50 Torr), non-premixed, opposed-flow acetylene(Ar)/O-2(Ar) flames. We measured quantitative mole-fraction profiles as a function of the distance from the fuel outlet for the major species and several intermediates, including the methyl and propargyl radicals. We determined the temperature profiles of these flames by normalizing a sampling-instrument function to thermocouple measurements near the fuel outlet. A comparison of the experimental temperature and major species profiles with modeling results indicates that flame perturbations caused by the sampling probe are minimal. The observed agreement between experimental and modeled results, apparent for most combustion species, is similar to corresponding studies of premixed flames. (C) 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Skeen, S. A.; Michelsen, H. A.; Hansen, N.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. [Yang, B.] Princeton Univ, Combust Energy Frontier Res Ctr, Princeton, NJ 08540 USA. [Miller, J. A.] Argonne Natl Lab, Div Chem, Argonne, IL 60439 USA. [Violi, A.] Univ Michigan, Dept Mech Engn, Ann Arbor, MI 48109 USA. RP Hansen, N (reprint author), PO 969 MS 9055, Livermore, CA 94551 USA. EM nhansen@sandia.gov RI Hansen, Nils/G-3572-2012; Yang, Bin/A-7158-2008; OI Yang, Bin/0000-0001-7333-0017; Skeen, Scott/0000-0002-4444-0759 FU U.S Department of Energy (DOE), Office of Basic Energy Sciences (BES) under the Single Investigator Small Group Research (SISGR) [DE-SC0002619]; National Nuclear Security Administration [DE-AC04-94-AL85000]; ASC-HPCC [DE-AC02-2006CH11357, 59044]; Office of Science, BES of the DOE [DE-AC02-05CH11231] FX We gratefully acknowledge the expert technical assistance of Sarah Ferrell and Paul Fugazzi. This work was supported by the U.S Department of Energy (DOE), Office of Basic Energy Sciences (BES) under the Single Investigator Small Group Research (SISGR, Grant No. DE-SC0002619) and under separate grants to Sandia and Argonne from the Division of Chemical Sciences, Geosciences, and Biosciences. Sandia is a multi-program laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the National Nuclear Security Administration under contract DE-AC04-94-AL85000. The work at Argonne was supported under contract no. DE-AC02-2006CH11357 as part of the ASC-HPCC (ANL FWP # 59044). The measurements were performed at the Advanced Light Source (ALS) of the Lawrence Berkeley National Laboratory. The ALS is supported by the Director, Office of Science, BES of the DOE under Contract no. DE-AC02-05CH11231. NR 43 TC 5 Z9 8 U1 3 U2 53 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 1067 EP 1075 DI 10.1016/j.proci.2012.06.075 PN 1 PG 9 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065CN UT WOS:000313125400108 ER PT J AU Chakraborty, N Kolla, H Sankaran, R Hawkes, ER Chen, JH Swaminathan, N AF Chakraborty, N. Kolla, H. Sankaran, R. Hawkes, E. R. Chen, J. H. Swaminathan, N. TI Determination of three-dimensional quantities related to scalar dissipation rate and its transport from two-dimensional measurements: Direct Numerical Simulation based validation SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Scalar dissipation rate (SDR); Two-dimensional experimental measurements; Direct Numerical Simulation; Isotropy; Reynolds-Averaged Navier-Stokes (RANS) simulation ID TURBULENT PREMIXED FLAMES; SURFACE-DENSITY; LEWIS NUMBER; STRAIN-RATE; COMBUSTION; EQUATION; CURVATURE; EVOLUTION; GRADIENT; MODEL AB Three-dimensional compressible Direct Numerical Simulation (DNS) data of freely propagating statistically planar and statistically stationary slot-jet turbulent premixed flames has been used to assess the accuracy of the isotropy-derived correction factors, which relate the two-dimensional projections of the different terms of the Favre-averaged scalar dissipation rate transport equation with their corresponding actual three-dimensional counterparts. The accuracy of these correction factors is assessed using both simplified and detailed chemistry-based DNS data, for a range of values of Karlovitz number Ka, heat release parameter tau, and turbulent Reynolds number Re-t. It is shown that the isotropic distribution of the probability density function (pdf) of the angle, phi, between the normal vectors of the measurement plane and of the flame surface provides a simple algebraic relation between the scalar dissipation rates evaluated in two and three dimensions (i.e. (N) over tilde (c) and (N) over tilde (2D)(c)), independent of the considered values of Ka, tau and Re-t. The isotropic relations between two-dimensional and three-dimensional counterparts of the curvature and propagation terms in the transport equation of (N) over tilde (c) are also found to work well for all the values of Ka, tau and Re-t considered here. However, the relation between the value obtained from two-dimensional projection and the true three-dimensional value for the strain rate term in the (N) over tilde (c) transport equation works well only for large values of Re-t and the reasons for this behaviour are explained in detail. It is found that the threshold value of Ret above which the assumption of isotropy yields an accurate relation between two-dimensional projection and three-dimensional values for the strain rate term of the dissipation rate transport equation depends on the regime of the prevailing combustion process. (C) 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Chakraborty, N.] Newcastle Univ, Sch Mech & Syst Engn, Newcastle Upon Tyne NE1 7RU, Tyne & Wear, England. [Kolla, H.; Chen, J. H.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. [Sankaran, R.] Oak Ridge Natl Lab, Natl Ctr Computat Sci, Oak Ridge, TN 37831 USA. [Hawkes, E. R.] Univ New S Wales, Sch Photovolta & Renewable Energy Engn, Sydney, NSW 2052, Australia. [Hawkes, E. R.] Univ New S Wales, Sch Mech & Mfg Engn, Sydney, NSW 2052, Australia. [Swaminathan, N.] Univ Cambridge, Dept Engn, Cambridge CB2 1PZ, England. RP Kolla, H (reprint author), Sandia Natl Labs, Combust Res Facil, MS 9051,POB 969, Livermore, CA 94551 USA. EM nilanjan.chakraborty@ncl.ac.uk; hnkolla@sandia.gov; sankaranr@ornl.gov; evatt.hawkes.unsw@gmail.com; jhchen@sandia.gov; ns341@eng.cam.ac.uk RI Swaminathan, N/A-7468-2008; Kolla, Hemanth/L-2142-2013; Sankaran, Ramanan/D-9254-2015; Hawkes, Evatt/C-5307-2012; OI Swaminathan, N/0000-0003-3338-0698; Kolla, Hemanth/0000-0003-4969-5870; Sankaran, Ramanan/0000-0002-5352-9915; Hawkes, Evatt/0000-0003-0539-7951; Chakraborty, Nilanjan/0000-0003-1690-2036 FU ESPRC; Division of Chemical Sciences, Geosciences and Biosciences, the Office of Basic Energy Sciences, the U. S. Department of Energy (DOE); Office of Science of the DOE [DE-AC05-00OR22725]; Australian Research Council FX NC and NS acknowledge the support of ESPRC. The work at Sandia National Laboratories was supported by the Division of Chemical Sciences, Geosciences and Biosciences, the Office of Basic Energy Sciences, the U. S. Department of Energy (DOE). This research used resources of the National Center for Computational Sciences at Oak Ridge National Laboratory (NCCS/ORNL) which is supported by the Office of Science of the DOE under contract No. DE-AC05-00OR22725. ERH acknowledges the support of the Australian Research Council. NR 37 TC 12 Z9 12 U1 1 U2 23 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 1151 EP 1162 DI 10.1016/j.proci.2012.06.040 PN 1 PG 12 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065CN UT WOS:000313125400118 ER PT J AU Bell, JB Day, MS Lijewski, MJ AF Bell, J. B. Day, M. S. Lijewski, M. J. TI Simulation of nitrogen emissions in a premixed hydrogen flame stabilized on a low swirl burner SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Turbulent premixed combustion; Low Mach number flow; Adaptive mesh refinement; Emissions ID NUMERICAL-SIMULATION; TURBULENT FLAMES; METHANE; COMBUSTION; CHEMISTRY; MIXTURES; INJECTOR AB There is considerable interest in developing fuel-flexible, low emissions turbines for power generation. One approach is based on burning a variety of lean premixed fuels with relatively low flame temperatures. Such flames can be stabilized in a low swirl burner configuration, for example, using a variety of fuels such as pure hydrogen and hydrogen-seeded hydrocarbon mixtures. However, many hydrogen-rich fuels are thermodiffusively unstable and burn in cellular flame structures, which can have a significant impact on the local nitrogen chemistry. These cellular burning patterns are characterized by a local enhancement of fuel concentration and a corresponding increase in local flame temperature just downstream. In turn, these regions become sites for enhanced thermal NOx production. The structure of these cells, and their impact on the net emissions of a flame is influenced by the global flame stabilization mechanisms and by local turbulence properties. Here we investigate the role of thermodiffusive instabilities on NOx emissions in the context of a laboratory-scale low swirl burner fueled with a lean hydrogen-air mixture at atmospheric pressure. The simulations show how the cellular burning structures characteristic of lean premixed hydrogen combustion lead to local and global enhancements in the NOx emissions. We quantify the chemical pathways that lead to the formation of NO and N2O, and how they are enhanced within local regions of intense burning. (C) 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Bell, J. B.; Day, M. S.; Lijewski, M. J.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Bell, JB (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mail Stop 50A-1148,1 Cyclotron Rd, Berkeley, CA 94720 USA. EM JBBell@lbl.gov FU DOE Office of Advanced Scientific Computing Research under the U.S. Department of Energy [DE-AC02-05CH11231] FX This work was supported by the DOE Applied Mathematics Research Program of the DOE Office of Advanced Scientific Computing Research under the U.S. Department of Energy Contract No. DE-AC02-05CH11231. The authors thank Peter Glarborg for providing them with the emissions chemistry used in this work. NR 22 TC 7 Z9 7 U1 0 U2 21 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 1173 EP 1182 DI 10.1016/j.proci.2012.07.046 PN 1 PG 10 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065CN UT WOS:000313125400120 ER PT J AU Yang, Y Wang, HF Pope, SB Chen, JH AF Yang, Yue Wang, Haifeng Pope, Stephen B. Chen, Jacqueline H. TI Large-eddy simulation/probability density function modeling of a non-premixed CO/H-2 temporally evolving jet flame SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Large-eddy simulation; Probability density function methods; Turbulent non-premixed jet flame; Multi-scalar mixing ID DIRECT NUMERICAL SIMULATIONS; TURBULENT REACTING FLOWS; SCALAR DISSIPATION; MIXING MODELS; COMBUSTION; FORMULATION; CHEMISTRY; DIFFUSION; SCHEME AB We report a large-eddy simulation (LES)/probability density function (PDF) study of a non-premixed CO/H-2 temporally-evolving turbulent planar jet flame, which has previously been studied using direct numerical simulations (DNS) with a skeletal chemical mechanism. The flame exhibits strong turbulence-chemistry interactions resulting in local extinction followed by re-ignition. In this study, the filtered velocity field in LES and the PDF transport equations with the interaction-by-exchange with the mean (IEM) mixing model (with molecular transport) are solved by the highly-scalable NGA/HPDF codes with second-order accuracy in space and time. The performance of the hybrid LES/PDF methodology is assessed through detailed a posteriori comparisons with DNS of the same flame. The comparison shows overall good agreement of the temporal evolution of the temperature and mass fractions of major chemical species, as well as the prediction of local extinction and re-ignition. The modeling of multi-scalar mixing is analyzed using the DNS and LES/PDF results. The DNS results exhibit an attracting manifold of the streamlines of the diffusion velocity in composition space, and the LES/PDF results show qualitative agreement on the manifold and joint PDFs of compositions. (C) 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Yang, Yue; Wang, Haifeng; Pope, Stephen B.] Cornell Univ, Sibley Sch Mech & Aerosp Engn, Ithaca, NY 14853 USA. [Yang, Yue; Chen, Jacqueline H.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 96551 USA. RP Yang, Y (reprint author), Cornell Univ, Sibley Sch Mech & Aerosp Engn, 138 Upson Hall, Ithaca, NY 14853 USA. EM yy463@cornell.edu RI Yang, Yue/C-7873-2009; Wang, Haifeng/H-9529-2013 OI Wang, Haifeng/0000-0003-0285-8783 FU US Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences [DE-SC0001198]; Office of Science of the US DOE [DE-AC05-00OR22725] FX The authors are grateful to O. Desjardins for the help of the NGA code, E.R. Hawkes and H. Kolla for the support on the post-processing of the DNS data, and P.P. Popov for the help of the two-way coupling algorithm. This research is supported by the Combustion Energy Frontier Research Center, an Energy Frontier Research Center funded by the US Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences under Award No. DE-SC0001198. Computer allocations were awarded by DOE's Innovative and Novel Computational Impact on Theory and Experiments (INCITE) Program. This research used resources of the National Center for Computational Sciences at Oak Ridge National Laboratory (NCCS/ORNL) which is supported by the Office of Science of the US DOE under Contract No. DE-AC05-00OR22725. NR 35 TC 22 Z9 23 U1 5 U2 30 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 1241 EP 1249 DI 10.1016/j.proci.2012.08.015 PN 1 PG 9 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065CN UT WOS:000313125400127 ER PT J AU Kaul, CM Raman, V Knudsen, E Richardson, ES Chen, JH AF Kaul, Colleen M. Raman, Venkat Knudsen, Edward Richardson, Edward S. Chen, Jacqueline H. TI Large eddy simulation of a lifted ethylene flame using a dynamic nonequilibrium model for subfilter scalar variance and dissipation rate SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Large eddy simulation; Subfilter modeling; Dynamic modeling; Lifted flame ID CONDITIONAL MOMENT CLOSURE; TURBULENT REACTING FLOWS; HIGHLY-HEATED COFLOW; DENSITY-FUNCTION; DIFFERENTIAL DIFFUSION; JET FLAME; COMBUSTION; FORMULATION; VELOCITY; SCHEME AB Accurate prediction of nonpremixed turbulent combustion using large eddy simulation (LES) requires detailed modeling of the mixing between fuel and oxidizer at scales finer than the LES filter resolution. In conserved scalar combustion models, the small scale mixing process is quantified by two parameters, the subfilter scalar variance and the subfilter scalar dissipation rate. The most commonly used models for these quantities assume a local equilibrium exists between production and dissipation of variance. Such an assumption has limited validity in realistic, technically relevant flow configurations. However, nonequilibrium models for variance and dissipation rate typically contain a model coefficient whose optimal value is unknown a priori for a given simulation. Furthermore, conventional dynamic procedures are not useful for estimating the value of this coefficient. In this work, an alternative dynamic procedure based on the transport equation for subfilter scalar variance is presented. This dynamic nonequilibrium modeling approach is used for simulation of a turbulent lifted ethylene flame, previously studied using DNS by Yoo et al. (2011). The predictions of the new model are compared to those of a static nonequilibrium modeling approach using an assumed model coefficient, as well as those of the equilibrium modeling approach. The equilibrium models are found to systematically underpredict both subfilter scalar variance and dissipation rate. Use of the dynamic procedure is shown to increase the accuracy of the nonequilibrium modeling approach. However, numerical errors that arise as a consequence of grid-based implicit filtering appear to degrade the accuracy of all three modeling options. Thus, while these results confirm the usefulness of the new dynamic model, they also show that the quality of subfilter model predictions depends on several factors extrinsic to the formulation of the subfilter model itself. (C) 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Kaul, Colleen M.; Raman, Venkat] Univ Texas Austin, Dept Aerosp Engn & Engn Mech, Austin, TX 78712 USA. [Kaul, Colleen M.] Stanford Univ, Ctr Turbulence Res, Stanford, CA 94305 USA. [Knudsen, Edward] Stanford Univ, Dept Mech Engn, Stanford, CA 94305 USA. [Richardson, Edward S.] Univ Southampton, Fac Engn & Environm, Southampton, Hants, England. [Chen, Jacqueline H.] Sandia Natl Labs, Combust Res Facil, Livermore, CA USA. RP Kaul, CM (reprint author), Stanford Univ, Ctr Turbulence Res, Bldg 500, Stanford, CA 94305 USA. EM cmkaul@stanford.edu RI Raman, Venkat/F-5744-2011 FU NASA [NNX07AB92A, NNX08AB41A]; US Department of Energy, the Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences; Office of Advanced Scientific Computing Research FX Support from NASA through grants NNX07AB92A and NNX08AB41A and resources provided by the High Performance Computing Center at Stanford University are gratefully acknowledged.; The work at Sandia National Laboratories (SNL) was supported by the US Department of Energy, the Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, and Office of Advanced Scientific Computing Research. NR 34 TC 11 Z9 11 U1 2 U2 37 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 1289 EP 1297 DI 10.1016/j.proci.2012.06.079 PN 1 PG 9 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065CN UT WOS:000313125400132 ER PT J AU Dunn, MJ Barlow, RS AF Dunn, Matthew J. Barlow, Robert S. TI Effects of preferential transport and strain in bluff body stabilized lean and rich premixed CH4/air flames SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Turbulent premixed flames; Bluff-body flames; Differential diffusion; Preferential transport; Multiscalar diagnostics ID METHANE-AIR FLAMES; TURBULENT COMBUSTION; RAMAN/RAYLEIGH SCATTERING; STRATIFIED FLAMES; LEWIS NUMBER; TEMPERATURES; DIFFUSION; LAMINAR AB The effects of preferential transport and strain on the scalar structure of turbulent premixed bluff body stabilized flames are examined using Raman-Rayleigh-LIF diagnostics. Bulk flowrate and equivalence ratio are varied parametrically. Comparisons with laminar flame calculations are used both to validate the quality of the experimental measurements and to facilitate interpretation of the measured response of the bluff body flames to changes in equivalence ratio and flow conditions. Strong effects of preferential species transport on the internal flame structure and the product composition of the recirculation zone are observed in lean, stoichiometric, and rich flames. Contrary to the standard view of differential diffusion effects in turbulent flow becoming negligible at sufficiently high Reynolds number, the preferential diffusion effects in the premixed bluff body flames reported here initially increase with the Reynolds number then saturate and persist at higher Reynolds numbers. Measurements in a rich bluff body flame are suggestive of high strain, but instantaneous profiles in the turbulent flame for this shear-flow geometry are thicker than calculated for an unstrained laminar flame. (C) 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Dunn, Matthew J.; Barlow, Robert S.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94550 USA. RP Dunn, MJ (reprint author), Univ Sydney, AMME, Blg J07, Sydney, NSW 2006, Australia. EM matthewdunn2009@gmail.com RI Barlow, Robert/C-2364-2013 FU Division of Chemical Sciences, Geosciences and Biosciences, Office of Basic Energy Sciences, US Department of Energy; United States Department of Energy [DE-AC04-94-AL85000] FX Work was supported by the Division of Chemical Sciences, Geosciences and Biosciences, Office of Basic Energy Sciences, US Department of Energy. Sandia National Laboratories is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the United States Department of Energy under contract DE-AC04-94-AL85000. Contributions by Bob Harmon in support of these experiments are gratefully acknowledged. NR 23 TC 14 Z9 15 U1 0 U2 12 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 1411 EP 1419 DI 10.1016/j.proci.2012.06.070 PN 1 PG 9 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065CN UT WOS:000313125400145 ER PT J AU Dahms, RN Manin, J Pickett, LM Oefelein, JC AF Dahms, Rainer N. Manin, Julien Pickett, Lyle M. Oefelein, Joseph C. TI Understanding high-pressure gas-liquid interface phenomena in Diesel engines SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Direct injection; Diesel engine; Supercritical flow; Real fluid model ID LINEAR GRADIENT THEORY; LARGE-EDDY SIMULATION; BINARY-MIXTURES; SURFACE-TENSION; SUPERCRITICAL ENVIRONMENTS; CORRESPONDING STATES; TRANSPORT-PROPERTIES; CRYOGENIC FLAMES; MIXING LAYERS; PURE FLUIDS AB Injection of liquid fuel (or oxidizer in the case of liquid rockets) in systems where the working fluid exceeds the thermodynamic critical condition of the liquid phase is not well understood. Under some conditions when operating pressures exceed the liquid phase critical pressure, surface tension forces become diminished so that the classical low-pressure gas-liquid interface is replaced by a diffusion dominated mixing layer. These two extremes have been well recognized in the liquid rocket community for years. In other systems, however, the significance of surface tension forces is not clear. Here we focus on this topic in the context of Diesel engine fuel injection processes. We derive a coupled model to obtain a theoretical analysis that quantifies under what conditions the interfacial dynamics transition between the classical non-continuum "jump" conditions associated with two phase flows and a continuous gas-liquid interfacial diffusion layer. We present high-speed imaging from the Sandia non-reacting n-dodecane experiment that provides corroborating evidence that continuous gas-liquid interfacial mixing dynamics occur at high-pressure Diesel engine conditions. At constant chamber density and supercritical fuel pressures, liquid structures affected by surface tension such as ligaments and drops develop at low ambient temperatures. But at engine-relevant high-temperature conditions, a different, more diffusive mixture preparation process without measurable fuel drops is found. These two conditions are studied using our model. It applies a real-fluid model that accounts for the relevant thermodynamic non-ideal multicomponent mixture states in the system and combines this with Linear Gradient Theory, which facilitates the calculation of the detailed vapor-liquid interfacial structure. At high ambient temperature, our model shows interfaces with substantially increased thicknesses in comparison to the low temperature condition. Our analysis reveals that gas-liquid interfacial diffusion layers develop, contrary to conventional wisdom, not necessarily because of vanishing surface tension forces, but because of the combination of a reduction in mean free molecular path and broadening interfaces, which then enter the continuum length scale regime. Then, instead of inter-molecular forces, transport processes dominate. (C) 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Dahms, Rainer N.; Manin, Julien; Pickett, Lyle M.; Oefelein, Joseph C.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94550 USA. RP Dahms, RN (reprint author), Sandia Natl Labs, Combust Res Facil, 7011 E Ave,MS9051, Livermore, CA 94550 USA. EM Rndahms@sandia.gov FU US Department of Energy, Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Program; United States Department of Energy's National Nuclear Security Administration [DE-AC-94AL85000] FX Support provided by the US Department of Energy, Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Program, is gratefully acknowledged. This research was performed at the Combustion Research Facility, Sandia National Laboratories, Livermore, CA. Sandia is a multiprogramming laboratory operated by the Sandia Corporation, a Lockheed Martin Company, for the United States Department of Energy's National Nuclear Security Administration under contract DE-AC-94AL85000. NR 40 TC 33 Z9 34 U1 7 U2 58 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 1667 EP 1675 DI 10.1016/j.proci.2012.06.169 PN 1 PG 9 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065CN UT WOS:000313125400175 ER PT J AU Edwards, DE You, XQ Zubarev, DY Lester, WA Frenklach, M AF Edwards, David E. You, Xiaoqing Zubarev, Dmitry Yu. Lester, William A., Jr. Frenklach, Michael TI Thermal decomposition of graphene armchair oxyradicals SO PROCEEDINGS OF THE COMBUSTION INSTITUTE LA English DT Article DE Soot; Graphene; PAH; Oxidation; Reaction mechanisms ID SOOT FORMATION; EDGE GROWTH; AROMATIC-HYDROCARBONS; LAYER GROWTH; FLAMES; SIMULATIONS; CHEMISTRY; MECHANISM; MIGRATION; OXIDATION AB Energetics and kinetics of the thermal decomposition of oxyradicals with oxygen bonded to a graphene armchair edge were investigated. Phenanthrene, benzoperylene, and an 11-ring polycyclic aromatic hydrocarbon (PAH) were selected as substrates to model the armchair edge, with a total of five different oxyradicals studied. The elementary steps of the reaction pathways were analyzed using density functional theory. Rate coefficients over the ranges of 1500-2500 K and 0.01-10 atm were obtained by solving the master equations. The computed rate coefficients were found to be temperature, pressure, and substrate-size dependent. The results revealed that the decomposition rate of an oxyradical with oxygen positioned on the outside of a corner armchair edge is faster than the rate with oxygen positioned to the inside of the edge. The trends in the computed oxyradical decomposition rates could be rationalized by the structural characteristics of the substrates. The decomposition rates computed for the armchair edge oxyradicals are shown to be similar to those previously obtained for corner zigzag edge oxyradicals. This implies that given an arbitrary shaped PAH, oxidation should preferentially occur at armchair and corner-zigzag sites, leaving resistant to oxidation inner zigzag sites essentially intact. Considering that growth of both armchair and zigzag edges proceeds at effectively the same rate, we expect to find proliferation of zigzag-edge surfaces on soot particles formed in flame environments. (C) 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. C1 [Edwards, David E.; You, Xiaoqing; Frenklach, Michael] Univ Calif Berkeley, Dept Mech Engn, Berkeley, CA 94720 USA. [Edwards, David E.; Frenklach, Michael] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. [Zubarev, Dmitry Yu.; Lester, William A., Jr.] Univ Calif Berkeley, Dept Chem, Kenneth S Pitzer Ctr Theoret Chem, Berkeley, CA 94720 USA. [Lester, William A., Jr.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. RP Edwards, DE (reprint author), Univ Calif Berkeley, Dept Mech Engn, 244 Hesse Hall, Berkeley, CA 94720 USA. EM david.edwards@berkeley.edu RI You, Xiaoqing/B-1240-2015 FU US Army Corps of Engineers, Humphreys Engineering Center Support Activity [W912HQ-07-C-0044]; National Science Foundation [NSF CHE-0809969]; Office of Energy Research, Office of Basic Energy Sciences, Chemical Sciences, Geosciences and Biosciences Division of the US Department of Energy [DE-AC03-76F00098]; Office of Science of the US Department of Energy [DE-AC02-05CH11231] FX XY and MF were supported by the US Army Corps of Engineers, Humphreys Engineering Center Support Activity, under Contract No. W912HQ-07-C-0044. DYZ was supported by the National Science Foundation under grant NSF CHE-0809969. DEE, WAL, and MF were supported by the Director, Office of Energy Research, Office of Basic Energy Sciences, Chemical Sciences, Geosciences and Biosciences Division of the US Department of Energy, under Contract No. DE-AC03-76F00098. This research used computational resources of the National Energy Research Scientific Computing Center, which is supported by the Office of Science of the US Department of Energy under Contract No. DE-AC02-05CH11231. The authors are indebted to Professors David Golden and John Barker for their help with the use of the MultiWell code. NR 37 TC 8 Z9 8 U1 0 U2 27 PU ELSEVIER SCIENCE INC PI NEW YORK PA 360 PARK AVE SOUTH, NEW YORK, NY 10010-1710 USA SN 1540-7489 EI 1873-2704 J9 P COMBUST INST JI Proc. Combust. Inst. PY 2013 VL 34 BP 1759 EP 1766 DI 10.1016/j.proci.2012.05.031 PN 1 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Chemical; Engineering, Mechanical SC Thermodynamics; Energy & Fuels; Engineering GA 065CN UT WOS:000313125400183 ER PT J AU Leigh, J Johnson, A Renambot, L Peterka, T Jeong, B Sandin, DJ Talandis, J Jagodic, R Nam, S Hur, H Sun, YW AF Leigh, Jason Johnson, Andrew Renambot, Luc Peterka, Tom Jeong, Byungil Sandin, Daniel J. Talandis, Jonas Jagodic, Ratko Nam, Sungwon Hur, Hyejung Sun, Yiwen TI Scalable Resolution Display Walls SO PROCEEDINGS OF THE IEEE LA English DT Article DE Computer graphics; stereo vision; virtual reality; visualization ID COLLABORATIVE VISUALIZATION AB This article will describe the progress since 2000 on research and development in 2-D and 3-D scalable resolution display walls that are built from tiling individual lower resolution flat panel displays. The article will describe approaches and trends in display hardware construction, middleware architecture, and user-interaction design. The article will also highlight examples of use cases and the benefits the technology has brought to their respective disciplines. C1 [Leigh, Jason; Johnson, Andrew; Renambot, Luc; Sandin, Daniel J.; Talandis, Jonas; Jagodic, Ratko; Nam, Sungwon; Hur, Hyejung; Sun, Yiwen] Univ Illinois, Elect Visualizat Lab, Chicago, IL 60607 USA. [Peterka, Tom] Argonne Natl Lab, Argonne, IL 60439 USA. [Jeong, Byungil] Texas Adv Comp Ctr, Austin, TX 78758 USA. RP Leigh, J (reprint author), Univ Illinois, Elect Visualizat Lab, Chicago, IL 60607 USA. EM spiff@uic.edu FU National Science Foundation [CNS-0935919, 0959053]; King Abdullah University of Science and Technology (KAUST) [US-2008-107/SA-C0064]; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357] FX This work was supported in part by the National Science Foundation under Awards CNS-0935919 and 0959053, and by the King Abdullah University of Science and Technology (KAUST) under Award US-2008-107/SA-C0064. Work at the Center for Nanoscale Materials was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract DE-AC02-06CH11357. NR 38 TC 11 Z9 11 U1 0 U2 8 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 0018-9219 EI 1558-2256 J9 P IEEE JI Proc. IEEE PD JAN PY 2013 VL 101 IS 1 SI SI BP 115 EP 129 DI 10.1109/JPROC.2012.2191609 PG 15 WC Engineering, Electrical & Electronic SC Engineering GA 063MI UT WOS:000313002800011 ER PT J AU Hay, BP Chagnes, A Cote, G AF Hay, Benjamin P. Chagnes, Alexandre Cote, Gerard TI On the Metal Ion Selectivity of Oxoacid Extractants SO SOLVENT EXTRACTION AND ION EXCHANGE LA English DT Article DE Liquid-liquid extraction; cation exchange; ligand basicity; metal ion acidity; LFER ID PREDICTING STABILITY-CONSTANTS; COMPLEXATION; HYDROLYSIS; ACIDS AB Relationships between metal chelate stability, ligand basicity, and metal ion acidity are reviewed and the general applicability is illustrated by linear correlations between aqueous stability constants and ligand pKa values for 35 metals with 26 ligands. The results confirm that most individual ligands of this type exhibit a stability ordering that correlates with the Lewis acidity of the metal ion. It is concluded that the general metal ion selectivity exhibited by liquid-liquid oxoacid extractants such as carboxylic acids, beta-diketones, and organophosphorus acids reflects the intrinsic affinity of the metal ion for the negative oxygen donor ligand. C1 [Hay, Benjamin P.] Oak Ridge Natl Lab, Div Chem Sci, Chem Separat Grp, Oak Ridge, TN 37831 USA. [Chagnes, Alexandre; Cote, Gerard] Chim ParisTech, LECIME, Paris, France. [Chagnes, Alexandre; Cote, Gerard] CNRS, Paris, France. RP Hay, BP (reprint author), Oak Ridge Natl Lab, Div Chem Sci, Chem Separat Grp, Oak Ridge, TN 37831 USA. EM haybp@ornl.gov RI CHAGNES, Alexandre/A-7441-2011 OI CHAGNES, Alexandre/0000-0002-4345-6812 FU Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, U.S. DOE at Oak Ridge National Laboratory FX BPH was supported by the Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, U.S. DOE at Oak Ridge National Laboratory. NR 20 TC 3 Z9 3 U1 2 U2 18 PU TAYLOR & FRANCIS INC PI PHILADELPHIA PA 325 CHESTNUT ST, SUITE 800, PHILADELPHIA, PA 19106 USA SN 0736-6299 J9 SOLVENT EXTR ION EXC JI Solvent Extr. Ion Exch. PD JAN 1 PY 2013 VL 31 IS 1 BP 95 EP 105 DI 10.1080/07366299.2012.709452 PG 11 WC Chemistry, Multidisciplinary SC Chemistry GA 052GW UT WOS:000312186700006 ER PT J AU Harp, DR Vesselinov, VV AF Harp, Dylan R. Vesselinov, Velimir V. TI Contaminant remediation decision analysis using information gap theory SO STOCHASTIC ENVIRONMENTAL RESEARCH AND RISK ASSESSMENT LA English DT Article DE Hydrogeology; Decision analysis; Information gap theory; Transport ID RADIOACTIVE-WASTES; UNCERTAINTY; MANAGEMENT; MODELS; PERSPECTIVE; TRANSPORT; CRITERIA AB Decision making under severe lack of information is a ubiquitous situation in nearly every applied field of engineering, policy, and science. A severe lack of information precludes our ability to determine a frequency of occurrence of events or conditions that impact the decision; therefore, decision uncertainties due to a severe lack of information cannot be characterized probabilistically. To circumvent this problem, information gap (info-gap) theory has been developed to explicitly recognize and quantify the implications of a severe lack of information in decision making. This paper presents a decision analysis based on info-gap theory developed for a contaminant remediation scenario. The analysis provides decision support in determining the fraction of contaminant mass to remove from the environment. An info-gap uncertainty model is developed to characterize uncertainty due to a lack of information concerning the contaminant flux. The info-gap uncertainty model groups nested, convex sets of functions defining contaminant flux over time based on their level of deviation from a nominal contaminant flux. The nominal contaminant flux defines a best estimate of contaminant flux over time based on existing, though incomplete, information. A robustness function is derived to quantify the maximum level of deviation from nominal that still ensures compliance for alternative decisions. An opportuneness function is derived to characterize the possibility of meeting a desired contaminant concentration level. The decision analysis evaluates how the robustness and opportuneness change as a function of time since remediation and as a function of the fraction of contaminant mass removed. C1 [Harp, Dylan R.; Vesselinov, Velimir V.] Los Alamos Natl Lab, Los Alamos, NM USA. RP Harp, DR (reprint author), Los Alamos Natl Lab, TA-3,Bldg 261,Room F200E, Los Alamos, NM USA. EM dharp@lanl.gov; vvv@lanl.gov RI Vesselinov, Velimir/P-4724-2016; OI Vesselinov, Velimir/0000-0002-6222-0530; Harp, Dylan/0000-0001-9777-8000 FU Environmental Programs Directorate of the Los Alamos National Laboratory FX This research was funded by the Environmental Programs Directorate of the Los Alamos National Laboratory. The authors extend their gratitude to Phoolendra K. Mishra, Greg M. Chavez, James R. Langenbrunner, Yakov Ben-Haim, Andy Wolfsberg, and Kay Birdsell for constructive discussions during the development of this paper. NR 30 TC 8 Z9 8 U1 0 U2 3 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1436-3240 J9 STOCH ENV RES RISK A JI Stoch. Environ. Res. Risk Assess. PD JAN PY 2013 VL 27 IS 1 BP 159 EP 168 DI 10.1007/s00477-012-0573-1 PG 10 WC Engineering, Environmental; Engineering, Civil; Environmental Sciences; Statistics & Probability; Water Resources SC Engineering; Environmental Sciences & Ecology; Mathematics; Water Resources GA 059UH UT WOS:000312730500012 ER PT J AU Iacovella, CR Varga, G Sallai, J Mukherjee, S Ledeczi, A Cummings, PT AF Iacovella, Christopher R. Varga, Gergely Sallai, Janos Mukherjee, Siladitya Ledeczi, Akos Cummings, Peter T. TI A model-integrated computing approach to nanomaterials simulation SO THEORETICAL CHEMISTRY ACCOUNTS LA English DT Article DE Model integrated computing; Nanoparticles; Polymers; Phase equilibria ID POLYHEDRAL OLIGOMERIC SILSESQUIOXANES; MOLECULAR-DYNAMICS SIMULATIONS; GOLD NANOPARTICLES; AGGREGATION BEHAVIOR; CRYSTALLIZATION; HYBRIDIZATION; AMPHIPHILES; NANOSPHERES; PREDICTIONS; ALGORITHMS AB The functionalization of nanoparticles with polymers to form "tethered nanoparticles'' (TNPs) is a promising approach to control the structure and properties of nanomaterials. However, the vast landscape of possible building blocks makes predicting the final behavior of tethered nanoparticles a priori a challenging task. Concepts from the computer science field of modeling integrated computing may provide an efficient means to optimize this complex design problem. Here, we investigate the use of model integrated computing for the simulation of tethered nanoparticles. We outline our development of a "meta-programming'' tool that enables the creation of a domain specific modeling language for tethered nanoparticle simulation and also provides tools for the creation and synthesis of simulation workflows. To test these tools and provide insight into their behavior, we report calculations of the vapor-liquid equilibrium of tethered nanoparticles as a function of grafting density and grafting length. C1 [Iacovella, Christopher R.; Mukherjee, Siladitya; Cummings, Peter T.] Vanderbilt Univ, Dept Chem & Biomol Engn, Nashville, TN 37212 USA. [Varga, Gergely; Sallai, Janos; Ledeczi, Akos] Vanderbilt Univ, Inst Software Integrated Syst, Nashville, TN USA. [Ledeczi, Akos] Vanderbilt Univ, Dept Elect Engn & Comp Sci, Nashville, TN USA. [Cummings, Peter T.] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN USA. RP Iacovella, CR (reprint author), Vanderbilt Univ, Dept Chem & Biomol Engn, Nashville, TN 37212 USA. EM christopher.r.iacovella@vanderbilt.edu; gergely.varga@vanderbilt.edu; janos.sallai@vanderbilt.edu; siladitya.mukherjee@vanderbilt.edu; akos.ledeczi@vanderbilt.edu; peter.cummings@vanderbilt.edu RI Iacovella, Christopher/D-2050-2011; Cummings, Peter/B-8762-2013 OI Cummings, Peter/0000-0002-9766-2216 FU National Science Foundation [NSF CBET-1028374]; National Institute for Computational Sciences [UT-TNEDU014]; US Civilian Research and Development Foundation CREST [UKC1-9201-LV-09] FX Funding provided by the National Science Foundation grant NSF CBET-1028374, with computational time provided by the National Institute for Computational Sciences, Project ID UT-TNEDU014 and US Civilian Research and Development Foundation CREST II Junior Scientist Research Collaboration Program Grant, Award Number UKC1-9201-LV-09. NR 56 TC 0 Z9 0 U1 1 U2 43 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1432-881X J9 THEOR CHEM ACC JI Theor. Chem. Acc. PD JAN PY 2013 VL 132 IS 1 AR 1315 DI 10.1007/s00214-012-1315-7 PG 9 WC Chemistry, Physical SC Chemistry GA 062BZ UT WOS:000312895400012 ER PT J AU Kullgren, B Jarvis, EE An, DD Abergel, RJ AF Kullgren, Birgitta Jarvis, Erin E. An, Dahlia D. Abergel, Rebecca J. TI Actinide chelation: biodistribution and in vivo complex stability of the targeted metal ions SO TOXICOLOGY MECHANISMS AND METHODS LA English DT Article DE Actinides; internal contamination; decorporation; in vivo distribution; chelating agents ID DECORPORATION AGENTS; HYDROXYPYRIDINONATE LIGANDS; PU(IV); 3,4,3-LI(1,2-HOPO); PLUTONIUM; NP-237; MOUSE; NP(V) AB Because of the continuing use of nuclear fuel sources and heightened threats of nuclear weapon use, the amount of produced and released radionuclides is increasing daily, as is the risk of larger human exposure to fission product actinides. A rodent model was used to follow the in vivo distribution of representative actinides, administered as free metal ions or complexed with chelating agents including diethylenetriamine pentaacetic acid ( DTPA) and the hydroxypyridinonate ligands 3,4,3-LI(1,2-HOPO) and 5-LIO(Me-3,2-HOPO). Different metabolic pathways for the different metal ions were evidenced, resulting in intricate ligand- and metal-dependent decorporation mechanisms. While the three studied chelators are known for their unrivaled actinide decorporation efficiency, the corresponding metal complexes may undergo in vivo decomposition and release metal ions in various biological pools. This study sets the basis to further explore the metabolism and in vivo coordination properties of internalized actinides for the future development of viable therapeutic chelating agents. C1 [Kullgren, Birgitta; Jarvis, Erin E.; An, Dahlia D.; Abergel, Rebecca J.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Glenn T Seaborg Ctr, Berkeley, CA 94720 USA. RP Abergel, RJ (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Glenn T Seaborg Ctr, 1 Cyclotron Rd,MS 70A-1150, Berkeley, CA 94720 USA. EM rjabergel@lbl.gov FU National Institutes of Health from the National Institute of Allergy and Infectious Diseases [1RC2AI087604-01, 5RC2AI087604-02] FX This work was supported by National Institutes of Health grants 1RC2AI087604-01 and 5RC2AI087604-02 from the National Institute of Allergy and Infectious Diseases. NR 32 TC 10 Z9 10 U1 1 U2 24 PU INFORMA HEALTHCARE PI LONDON PA TELEPHONE HOUSE, 69-77 PAUL STREET, LONDON EC2A 4LQ, ENGLAND SN 1537-6516 J9 TOXICOL MECH METHOD JI Toxicol. Mech. Methods PD JAN PY 2013 VL 23 IS 1 BP 18 EP 26 DI 10.3109/15376516.2012.728641 PG 9 WC Toxicology SC Toxicology GA 059MH UT WOS:000312709100004 PM 22957518 ER PT J AU Park, JM Liu, XY Leung, W Constant, K Russell, A Ho, KM AF Park, Joong-Mok Liu, Xinyu Leung, Wai Constant, Kristen Russell, Alan Ho, Kai-Ming BE Rahman, F TI High-Aspect-Ratio Metallic Nanostructures for Transparent Electrodes SO VISTAS IN NANOFABRICATION LA English DT Article; Book Chapter ID GRAIN-GROWTH; NANOWIRES AB Metallic nanowire arrays having high optical transmission and electric conductivity show promise for use as transparent electrodes. Transparent electrodes require high transmission of visible light and good electrical conductivity for charge transfer. High-aspect-ratio metallic nanowires for transparent electrode applications can be fabricated by e-beam angular deposition on polymer templates. These polymer templates are made with interference holography and nanoimprinting using a polydimethylsiloxane (PDMS) mold. The details of the fabrication processes including interference holography, micro-transfer molding, nanoimprint, and shadow angle depositions will be discussed. C1 [Park, Joong-Mok; Liu, Xinyu; Leung, Wai; Constant, Kristen; Russell, Alan; Ho, Kai-Ming] US DOE, Ames Lab, Ames, IA 50011 USA. [Constant, Kristen; Russell, Alan] Iowa State Univ, Dept Mat Sci, Ames, IA 50011 USA. [Ho, Kai-Ming] Iowa State Univ Sci & Technol, Dept Phys & Astron, Ames, IA 50011 USA. RP Park, JM (reprint author), US DOE, Ames Lab, Ames, IA 50011 USA. EM joongmok@iastate.edu RI Constant, Kristen/C-3673-2014 OI Constant, Kristen/0000-0001-7138-9365 NR 16 TC 0 Z9 0 U1 0 U2 1 PU PAN STANFORD PUBLISHING PTE LTD PI SINGAPORE PA PENTHOUSE LEVEL, SUNTEC TOWER 3, 8 TEMASEK BLVD, SINGAPORE, 038988, SINGAPORE BN 978-981-4364-57-7 PY 2013 BP 133 EP 146 PG 14 WC Nanoscience & Nanotechnology; Materials Science, Multidisciplinary SC Science & Technology - Other Topics; Materials Science GA BDD30 UT WOS:000312771400008 ER PT J AU Urgun-Demirtas, M Gillenwater, P Negri, MC Lin, YP Snyder, S Doctor, R Pierce, L Alvarado, J AF Urgun-Demirtas, Meltem Gillenwater, Patricia Negri, M. Cristina Lin, YuPo Snyder, Seth Doctor, Richard Pierce, Linda Alvarado, Jorge TI Achieving the Great Lakes Initiative Mercury Limits in Oil Refinery Effluent SO WATER ENVIRONMENT RESEARCH LA English DT Article DE low level mercury removal; refinery wastewater; Great Lakes Initiative mercury (Hg) criterion ID SEPARATION; MEMBRANE AB To meet the stringent Great Lakes Initiative (GLI) wastewater discharge mercury (Hg) limit of 1.3 ppt (ng /L), mercury removal technologies need to be identified and investigated. The goals of this study were to (1) identify and assess available wastewater treatment technologies for mercury removal from an oil refinery wastewater; and (2) conduct bench-scale tests to provide comparable, transparent, and uniform results to assess their performance at low mercury concentrations. The study found that many tested technologies were able to achieve the GLI mercury target concentration at the bench- scale, albeit with different efficiencies and engineering implications. These results demonstrate that at this scale there is no fundamental physical or chemical barrier to achieving,1.3 ng Hg/L in the tested wastewater. The study also found that some technologies were effective on particulate mercury whereas others were effective on dissolved mercury. One emerging treatment technology was found to be effective on both particulate and dissolved mercury. Three mercury-removal technologies-ultrafiltration (particulate mercury), adsorption (dissolved mercury), and an emerging reactive filtration technology (particulate and dissolved mercury)-are recommended for further study. This research offers treatment alternatives for different forms of mercury in an oil refinery wastewater, which might be applicable to other types of mercury-containing wastewater. Water Environ. Res., 85, 77 (2013). C1 [Urgun-Demirtas, Meltem; Gillenwater, Patricia; Negri, M. Cristina; Lin, YuPo; Snyder, Seth; Doctor, Richard; Pierce, Linda] Argonne Natl Lab, Div Energy Syst, Argonne, IL 60439 USA. [Alvarado, Jorge] Argonne Natl Lab, Div Environm Sci, Argonne, IL 60439 USA. RP Urgun-Demirtas, M (reprint author), Argonne Natl Lab, Div Energy Syst, 9700 S Cass Ave, Argonne, IL 60439 USA. EM negri@anl.gov FU Purdue University by BP North America, Inc. [85V09]; University of Chicago, Argonne LLC. [85V09]; Argonne, a U.S. Department of Energy Office of Science Laboratory [DE-AC02-06CH11357] FX This research was sponsored via Purdue University by BP North America, Inc. through Agreement No. 85V09 with the University of Chicago, Argonne LLC. This paper was prepared 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 24 TC 0 Z9 0 U1 1 U2 15 PU WATER ENVIRONMENT FEDERATION PI ALEXANDRIA PA 601 WYTHE ST, ALEXANDRIA, VA 22314-1994 USA SN 1061-4303 J9 WATER ENVIRON RES JI Water Environ. Res. PD JAN PY 2013 VL 85 IS 1 BP 77 EP 86 DI 10.2175/106143012X13373575831033 PG 10 WC Engineering, Environmental; Environmental Sciences; Limnology; Water Resources SC Engineering; Environmental Sciences & Ecology; Marine & Freshwater Biology; Water Resources GA 058WW UT WOS:000312666600008 PM 23409456 ER PT J AU Mason, TE Gawne, TJ Nagler, SE Nestor, MB Carpenter, JM AF Mason, T. E. Gawne, T. J. Nagler, S. E. Nestor, M. B. Carpenter, J. M. TI The early development of neutron diffraction: science in the wings of the Manhattan Project SO ACTA CRYSTALLOGRAPHICA SECTION A LA English DT Article ID SLOW-NEUTRONS; URANIUM; ICE AB Although neutron diffraction was first observed using radioactive decay sources shortly after the discovery of the neutron, it was only with the availability of higher intensity neutron beams from the first nuclear reactors, constructed as part of the Manhattan Project, that systematic investigation of Bragg scattering became possible. Remarkably, at a time when the war effort was singularly focused on the development of the atomic bomb, groups working at Oak Ridge and Chicago carried out key measurements and recognized the future utility of neutron diffraction quite independent of its contributions to the measurement of nuclear cross sections. Ernest O. Wollan, Lyle B. Borst and Walter H. Zinn were all able to observe neutron diffraction in 1944 using the X-10 graphite reactor and the CP-3 heavy water reactor. Subsequent work by Wollan and Clifford G. Shull, who joined Wollan's group at Oak Ridge in 1946, laid the foundations for widespread application of neutron diffraction as an important research tool. C1 [Mason, T. E.; Gawne, T. J.; Nagler, S. E.; Nestor, M. B.] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. [Carpenter, J. M.] Argonne Natl Lab, Argonne, IL 60439 USA. RP Mason, TE (reprint author), Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. EM masont@ornl.gov RI Mason, Thomas/M-5809-2014; Nagler, Stephen/E-4908-2010 OI Mason, Thomas/0000-0003-1880-3971; Nagler, Stephen/0000-0002-7234-2339 FU US Department of Energy [DE-AC05-00OR22725, DE-AC02-06CH11357]; US Department of Energy Office of Basic Energy Sciences, Division of Scientific User Facilities FX Oak Ridge National Laboratory is managed by UT-Battelle, LLC for the US Department of Energy under contract DE-AC05-00OR22725. Argonne National Laboratory is managed by UChicago Argonne, LLC for the US Department of Energy under contract DE-AC02-06CH11357. SEN is supported by the US Department of Energy Office of Basic Energy Sciences, Division of Scientific User Facilities. NR 60 TC 10 Z9 10 U1 2 U2 34 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0108-7673 J9 ACTA CRYSTALLOGR A JI Acta Crystallogr. Sect. A PD JAN PY 2013 VL 69 BP 37 EP 44 DI 10.1107/S0108767312036021 PN 1 PG 8 WC Chemistry, Multidisciplinary; Crystallography SC Chemistry; Crystallography GA 057JZ UT WOS:000312560800008 PM 23250059 ER PT J AU Srivatsan, TS Manigandan, K Petraroli, M Trejo, RM Sudarshan, TS AF Srivatsan, T. S. Manigandan, K. Petraroli, M. Trejo, Rosa M. Sudarshan, T. S. TI Influence of size of nanoparticles and plasma pressure compaction on microstructural development and hardness of bulk tungsten samples SO ADVANCED POWDER TECHNOLOGY LA English DT Article DE Tungsten; Nanosize powders; Consolidation; Plasma pressure compaction; Microstructure; Microhardness; Nano-hardness ID GRAIN-SIZE; NANOCRYSTALLINE MATERIALS; MECHANICAL-PROPERTIES; NANOSTRUCTURED METAL; TIB2-B4C COMPOSITE; CONSOLIDATION; POWDERS; DUCTILITY; COPPER; TEMPERATURE AB Bulk tungsten samples were prepared by consolidating nanosize tungsten powders using the technique of plasma pressure compaction. This innovative sintering technique offers the intrinsic capability of producing bulk samples having near theoretical density. Five different powder particle sizes, in the nanoscale, were chosen and bulk samples obtained by consolidating the powders under identical conditions of temperature, pressure and time using the technique of plasma pressure compaction. Microstructural observations and density measurement provide evidence for the presence of minimal porosity following consolidation. The influence of initial size of the powder particles on microstructural development to include the presence and distribution of porosity, density, micro-hardness, stiffness and nano-hardness is presented and discussed. (C) 2012 Published by Elsevier B.V. on behalf of The Society of Powder Technology Japan. All rights reserved. C1 [Srivatsan, T. S.; Manigandan, K.] Univ Akron, Dept Mech Engn, Akron, OH 44325 USA. [Petraroli, M.] Timken Res, Canton, OH 44706 USA. [Trejo, Rosa M.] Oak Ridge Natl Lab, High Temp Mat Lab, Oak Ridge, TN 37831 USA. [Sudarshan, T. S.] Mat Modificat Inc, Fairfax, VA 22031 USA. RP Srivatsan, TS (reprint author), Univ Akron, Dept Mech Engn, Akron, OH 44325 USA. EM srivatsants@yahoo.com FU Department of Mechanical Engineering at The University of Akron FX Mr. K. Manigandan (Graduate student: Department of Mechanical Engineering at The University of Akron) acknowledges support of the University through a Graduate Teaching Assistantship during the course of this research study. NR 48 TC 8 Z9 8 U1 2 U2 27 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0921-8831 J9 ADV POWDER TECHNOL JI Adv. Powder Technol. PD JAN PY 2013 VL 24 IS 1 BP 190 EP 199 DI 10.1016/j.apt.2012.05.008 PG 10 WC Engineering, Chemical SC Engineering GA 056EW UT WOS:000312472200024 ER PT J AU Abreu, P Aglietta, M Ahlers, M Ahn, EJ Albuquerque, IFM Allard, D Allekotte, I Allen, J Allison, P Almela, A Castillo, JA Alvarez-Muniz, J Batista, RA Ambrosio, M Aminaei, A Anchordoqui, L Andringa, S Antici'c, T Aramo, C Arganda, E Arqueros, F Asorey, H Assis, P Aublin, J Ave, M Avenier, M Avila, G Badescu, AM Balzer, M Barber, KB Barbosa, AF Bardenet, R Barroso, SLC Baughman, B Baeuml, J Baus, C Beatty, JJ Becker, KH Belletoile, A Bellido, JA BenZvi, S Berat, C Bertou, X Biermann, PL Billoir, P Blanco, F Blanco, M Bleve, C Blumer, H Bohacova, M Boncioli, D Bonifazi, C Bonino, R Borodai, N Brack, J Brancus, I Brogueira, P Brown, WC Bruijn, R Buchholz, P Bueno, A Buroker, L Burton, RE Caballero-Mora, KS Caccianiga, B Caramete, L Caruso, R Castellina, A Catalano, O Cataldi, G Cazon, L Cester, R Chauvin, J Cheng, SH Chiavassa, A Chinellato, JA Diaz, JC Chudoba, J Cilmo, M Clay, RW Cocciolo, G Collica, L Coluccia, MR Conceicao, R Contreras, F Cook, H Cooper, MJ Coppens, J Cordier, A Coutu, S Covault, CE Creusot, A Criss, A Cronin, J Curutiu, A Dagoret-Campagne, S Dallier, R Daniel, B Dasso, S Daumiller, K Dawson, BR de Almeida, RM De Domenico, M De Donato, C de Jong, SJ De La Vega, G de Mello, WJM Neto, JRTD De Mitri, I de Souza, V de Vries, KD del Peral, L del Rio, M Deligny, O Dembinski, H Dhital, N Di Giulio, C Castro, MLD Diep, PN Diogo, F Dobrigkeit, C Docters, W D'Olivo, JC Dong, PN Dorofeev, A dos Anjos, JC Dova, MT D'Urso, D Dutan, I Ebr, J Engel, R Erdmann, M Escobar, CO Espadanal, J Etchegoyen, A San Luis, P Falcke, H Fang, K Farrar, G Fauth, AC Fazzini, N Ferguson, AP Fick, B Figueira, JM Filevich, A Filipcic, A Fliescher, S Fracchiolla, CE Fraenkel, ED Fratu, O Froehlich, U Fuchs, B Gaior, R Gamarra, RF Gambetta, S Garcia, B Roca, STG Garcia-Gamez, D Garcia-Pinto, D Garilli, G Bravo, AG Gemmeke, H Ghia, PL Giller, M Gitto, J Glass, H Gold, MS Golup, G Albarracin, FG Berisso, MG Vitale, PF Goncalves, P Gonzalez, JG Gookin, B Gorgi, A Gouffon, P Grashorn, E Grebe, S Griffith, N Grillo, AF Guardincerri, Y Guarino, F Guedes, GP Hansen, P Harari, D Harrison, TA Harton, JL Haungs, A Hebbeker, T Heck, D Herve, AE Hill, GC Hojvat, C Hollon, N Holmes, VC Homola, P Horandel, JR Horvath, P Hrabovsky, M Huber, D Huege, T Insolia, A Ionita, F Italiano, A Jansen, S Jarne, C Jiraskova, S Josebachuili, M Kadija, K Kampert, KH Karhan, P Kasper, P Katkov, I Kegl, B Keilhauer, B Keivani, A Kelley, JL Kemp, E Kieckhafer, RM Klages, HO Kleifges, M Kleinfeller, J Knapp, J Koang, DH Kotera, K Krohm, N Kroemer, O Kruppke-Hansen, D Kuempel, D Kulbartz, JK Kunka, N La Rosa, G Lachaud, C LaHurd, D Latronico, L Lauer, R Lautridou, P Le Coz, S Leao, MSAB Lebrun, D Lebrun, P de Oliveira, MAL Letessier-Selvon, A Lhenry-Yvon, I Link, K Lopez, R Aguera, AL Louedec, K Bahilo, JL Lu, L Lucero, A Ludwig, M Lyberis, H Maccarone, MC Macolino, C Maldera, S Maller, J Mandat, D Mantsch, P Mariazzi, AG Marin, J Marin, V Maris, IC Falcon, HRM Marsella, G Martello, D Martin, L Martinez, H Bravo, OM Martraire, D Meza, JJM Mathes, HJ Matthews, J Matthews, JAJ Matthiae, G Maurel, D Maurizio, D Mazur, PO Medina-Tanco, G Melissas, M Melo, D Menichetti, E Menshikov, A Mertsch, P Messina, S Meurer, C Meyhandan, R Mi'canovi'c, S Micheletti, MI Minaya, IA Miramonti, L Molina-Bueno, L Mollerach, S Monasor, M Ragaigne, DM Montanet, F Morales, B Morello, C Moreno, E Moreno, JC Mostafa, M Moura, CA Muller, MA Mueller, G Muenchmeyer, M Mussa, R Navarra, G Navarro, JL Navas, S Necesal, P Nellen, L Nelles, A Neuser, J Nhung, PT Niechciol, M Niemietz, L Nierstenhoefer, N Nitz, D Nosek, D Nozka, L Oehlschlaeger, J Olinto, A Ortiz, M Pacheco, N Selmi-Dei, DP Palatka, M Pallotta, J Palmieri, N Parente, G Parizot, E Parra, A Pastor, S Paul, T Pech, M Pekala, J Pelayo, R Pepe, IM Perrone, L Pesce, R Petermann, E Petrera, S Petrolini, A Petrov, Y Pfendner, C Piegaia, R Pierog, T Pieroni, P Pimenta, M Pirronello, V Platino, M Plum, M Ponce, VH Pontz, M Porcelli, A Privitera, P Prouza, M Quel, EJ Querchfeld, S Rautenberg, J Ravel, O Ravignani, D Revenu, B Ridky, J Riggi, S Risse, M Ristori, P Rivera, H Rizi, V Roberts, J de Carvalho, WR Rodriguez, G Cabo, IR Martino, JR Rojo, J Rodriguez-Frias, MD Ros, G Rosado, J Rossler, T Roth, M Rouille-d'Orfeuil, B Roulet, E Rovero, AC Ruehle, C Saftoiu, A Salamida, F Salazar, H Greus, FS Salina, G Sanchez, F Santo, CE Santos, E Santos, EM Sarazin, F Sarkar, B Sarkar, S Sato, R Scharf, N Scherini, V Schieler, H Schiffer, P Schmidt, A Scholten, O Schoorlemmer, H Schovancova, J Schovanek, P Schroeder, F Schuster, D Sciutto, SJ Scuderi, M Segreto, A Settimo, M Shadkam, A Shellard, RC Sidelnik, I Sigl, G Lopez, HHS Sima, O 'Smiallkowski, A Smida, R Snow, GR Sommers, P Sorokin, J Spinka, H Squartini, R Srivastava, YN Stanic, S Stapleton, J Stasielak, J Stephan, M Stutz, A Suarez, F Suomijaervi, T Supanitsky, AD Susa, T Sutherland, MS Swain, J Szadkowski, Z Szuba, M Tapia, A Tartare, M Tascau, O Tcaciuc, R Thao, NT Thomas, D Tiffenberg, J Timmermans, C Tkaczyk, W Peixoto, CJT Toma, G Tomankova, L Tome, B Tonachini, A Elipe, GT Travnicek, P Tridapalli, DB Tristram, G Trovato, E Tueros, M Ulrich, R Unger, M Urban, M Galicia, JFV Valino, I Valore, L van Aar, G van den Berg, AM van Velzen, S van Vliet, A Varela, E Cardenas, BV Vazquez, JR Vazquez, RA Veberic, D Verzi, V Vicha, J Videla, M Villasenor, L Wahlberg, H Wahrlich, P Wainberg, O Walz, D Watson, AA Weber, M Weidenhaupt, K Weindl, A Werner, F Westerhoff, S Whelan, BJ Widom, A Wieczorek, G Wiencke, L Wilczynska, B Wilczynski, H Will, M Williams, C Winchen, T Wommer, M Wundheiler, B Yamamoto, T Yapici, T Younk, P Yuan, G Yushkov, A Garcia, BZ Zas, E Zavrtanik, D Zavrtanik, M Zaw, I Zepeda, A Zhou, J Zhu, Y Silva, MZ Ziolkowski, M AF Abreu, P. Aglietta, M. Ahlers, M. Ahn, E. J. Albuquerque, I. F. M. Allard, D. Allekotte, I. Allen, J. Allison, P. Almela, A. Alvarez Castillo, J. Alvarez-Muniz, J. Alves Batista, R. Ambrosio, M. Aminaei, A. Anchordoqui, L. Andringa, S. Antici'c, T. Aramo, C. Arganda, E. Arqueros, F. Asorey, H. Assis, P. Aublin, J. Ave, M. Avenier, M. Avila, G. Badescu, A. M. Balzer, M. Barber, K. B. Barbosa, A. F. Bardenet, R. Barroso, S. L. C. Baughman, B. Baeuml, J. Baus, C. Beatty, J. J. Becker, K. H. Belletoile, A. Bellido, J. A. BenZvi, S. Berat, C. Bertou, X. Biermann, P. L. Billoir, P. Blanco, F. Blanco, M. Bleve, C. Bluemer, H. Bohacova, M. Boncioli, D. Bonifazi, C. Bonino, R. Borodai, N. Brack, J. Brancus, I. Brogueira, P. Brown, W. C. Bruijn, R. Buchholz, P. Bueno, A. Buroker, L. Burton, R. E. Caballero-Mora, K. S. Caccianiga, B. Caramete, L. Caruso, R. Castellina, A. Catalano, O. Cataldi, G. Cazon, L. Cester, R. Chauvin, J. Cheng, S. H. Chiavassa, A. Chinellato, J. A. Chirinos Diaz, J. Chudoba, J. 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CA Pierre Auger Collaboration TI CONSTRAINTS ON THE ORIGIN OF COSMIC RAYS ABOVE 10(18) eV FROM LARGE-SCALE ANISOTROPY SEARCHES IN DATA OF THE PIERRE AUGER OBSERVATORY SO ASTROPHYSICAL JOURNAL LETTERS LA English DT Article DE astroparticle physics; cosmic rays ID MAGNETIC-FIELDS AB A thorough search for large-scale anisotropies in the distribution of arrival directions of cosmic rays detected above 10(18) eV at the Pierre Auger Observatory is reported. For the first time, these large-scale anisotropy searches are performed as a function of both the right ascension and the declination and expressed in terms of dipole and quadrupole moments. Within the systematic uncertainties, no significant deviation from isotropy is revealed. Upper limits on dipole and quadrupole amplitudes are derived under the hypothesis that any cosmic ray anisotropy is dominated by such moments in this energy range. 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[Anchordoqui, L.; Buroker, L.] Univ Wisconsin, Milwaukee, WI 53201 USA. [Antici'c, T.; Kadija, K.; Mi'canovi'c, S.; Susa, T.] Rudjer Boskovic Inst, Zagreb 10000, Croatia. [Arganda, E.; Dova, M. T.; Gomez Albarracin, F.; Hansen, P.; Jarne, C.; Mariazzi, A. G.; Moreno, J. C.; Sciutto, S. J.; Wahlberg, H.] Univ Nacl La Plata, IFLP, La Plata, Buenos Aires, Argentina. [Arganda, E.; Dasso, S.; Dova, M. T.; Gomez Albarracin, F.; Guardincerri, Y.; Hansen, P.; Jarne, C.; Mariazzi, A. G.; Masias Meza, J. J.; Moreno, J. C.; Piegaia, R.; Pieroni, P.; Sciutto, S. J.; Tiffenberg, J.; Wahlberg, H.] Consejo Nacl Invest Cient & Tecn, La Plata, Buenos Aires, Argentina. [Arganda, E.; Arqueros, F.; Blanco, F.; Garcia-Pinto, D.; Minaya, I. A.; Ortiz, M.; Rosado, J.; Vazquez, J. R.] Univ Complutense Madrid, Madrid, Spain. [Aublin, J.; Billoir, P.; Blanco, M.; Bonifazi, C.; Gaior, R.; Ghia, P. L.; Letessier-Selvon, A.; Macolino, C.; Maris, I. C.; Muenchmeyer, M.] Univ Paris 06, LPNHE, Paris, France. [Ave, M.; Baus, C.; Bluemer, H.; Dembinski, H.; Fuchs, B.; Huber, D.; Katkov, I.; Link, K.; Ludwig, M.; Melissas, M.; Palmieri, N.] Karlsruhe Inst Technol, Inst Expt Kernphys IEKP, Karlsruhe, Germany. [Avenier, M.; Berat, C.; Chauvin, J.; Koang, D. -H.; Le Coz, S.; Lebrun, D.; Louedec, K.; Montanet, F.; Stutz, A.; Tartare, M.] Univ Grenoble 1, Grenoble INP, CNRS, IN2P3,LPSC, F-38041 Grenoble, France. [Avila, G.; Contreras, F.; del Rio, M.; Gomez Vitale, P. F.; Kleinfeller, J.; Marin, J.; Rodriguez Martino, J.; Rodriguez Rojo, J.; Sato, R.; Squartini, R.] Observ Pierre Auger, Malargue, Argentina. [Avila, G.; Gomez Vitale, P. F.] Comis Nacl Energia Atom, Malargue, Argentina. [Badescu, A. M.; Fratu, O.] Univ Politehn Bucuresti, Bucharest, Romania. [Balzer, M.; Gemmeke, H.; Kleifges, M.; Kroemer, O.; Kunka, N.; Menshikov, A.; Ruehle, C.; Schmidt, A.; Weber, M.; Zhu, Y.] Karlsruhe Inst Technol, Inst Prozessdatenverarbeitung & Elekt, Karlsruhe, Germany. [Barber, K. B.; Bellido, J. A.; Clay, R. W.; Cooper, M. J.; Dawson, B. R.; Harrison, T. A.; Herve, A. E.; Hill, G. C.; Holmes, V. C.; Sorokin, J.; Wahrlich, P.; Whelan, B. J.] Univ Adelaide, Adelaide, SA, Australia. [Barbosa, A. F.; Diaz Castro, M. L.; dos Anjos, J. C.; Maurizio, D.; Shellard, R. C.] Ctr Brasileiro Pesquisas Fis, Rio De Janeiro, RJ, Brazil. [Bardenet, R.; Cordier, A.; Dagoret-Campagne, S.; Garcia-Gamez, D.; Kegl, B.; Louedec, K.; Monnier Ragaigne, D.; Urban, M.] Univ Paris 11, CNRS, IN2P3, LAL, Paris, France. [Barroso, S. L. C.] Univ Estadual Sudoeste Bahia, Vitoria Da Conquista, BA, Brazil. [Baeuml, J.; Bluemer, H.; Daumiller, K.; Engel, R.; Gonzalez, J. G.; Haungs, A.; Heck, D.; Huege, T.; Keilhauer, B.; Klages, H. O.; Kleinfeller, J.; Mathes, H. J.; Maurel, D.; Oehlschlaeger, J.; Pierog, T.; Porcelli, A.; Roth, M.; Schieler, H.; Schroeder, F.; Smida, R.; Szuba, M.; Ulrich, R.; Unger, M.; Weindl, A.; Werner, F.; Will, M.; Wommer, M.] Karlsruhe Inst Technol, Inst Kernphys, Karlsruhe, Germany. [Becker, K. H.; Bleve, C.; Kampert, K. H.; Krohm, N.; Kruppke-Hansen, D.; Neuser, J.; Niemietz, L.; Nierstenhoefer, N.; Querchfeld, S.; Rautenberg, J.; Sarkar, B.; Tascau, O.; Zimbres Silva, M.] Berg Univ Wuppertal, Wuppertal, Germany. [Belletoile, A.; Dallier, R.; Lautridou, P.; Maller, J.; Marin, V.; Martin, L.; Ravel, O.; Revenu, B.] Univ Nantes, CNRS, IN2P3, Ecole Mines Nantes,SUBATECH, F-44035 Nantes, France. [Biermann, P. L.; Caramete, L.; Curutiu, A.; Dutan, I.] Max Planck Inst Radioastron, Bonn, Germany. [Blanco, M.; del Peral, L.; Pacheco, N.; Rodriguez-Frias, M. D.; Ros, G.] Univ Alcala de Henares, Alcala De Henares, Madrid, Spain. [Bohacova, M.; Chudoba, J.; Ebr, J.; Hrabovsky, M.; Mandat, D.; Necesal, P.; Nozka, L.; Palatka, M.; Pech, M.; Prouza, M.; Ridky, J.; Schovancova, J.; Schovanek, P.; Tomankova, L.; Travnicek, P.; Vicha, J.] Acad Sci Czech Republic, Inst Phys, Prague, Czech Republic. [Boncioli, D.; del Rio, M.; Di Giulio, C.; Matthiae, G.; Salina, G.; Verzi, V.] Univ Roma Tor Vergata, I-00173 Rome, Italy. [Boncioli, D.; del Rio, M.; Di Giulio, C.; Matthiae, G.; Salina, G.; Verzi, V.] Sezione Ist Nazl Fis Nucl, Rome, Italy. [Bonifazi, C.; de Mello Neto, J. R. T.; Lyberis, H.; Santos, E. M.] Univ Fed Rio de Janeiro, Inst Fis, Rio De Janeiro, RJ, Brazil. [Borodai, N.; Homola, P.; Pekala, J.; Stasielak, J.; Wilczynska, B.; Wilczynski, H.] Inst Nucl Phys PAN, Krakow, Poland. [Brack, J.; Dorofeev, A.; Fracchiolla, C. E.; Gookin, B.; Harton, J. L.; Mostafa, M.; Petrov, Y.; Salesa Greus, F.; Thomas, D.] Colorado State Univ, Ft Collins, CO 80523 USA. [Brancus, I.; Saftoiu, A.; Toma, G.] Horia Hulubei Natl Inst Phys & Nucl Engn, Bucharest, Romania. [Brown, W. C.] Colorado State Univ, Pueblo, CO USA. [Bruijn, R.; Cook, H.; Knapp, J.; Lu, L.; Watson, A. A.] Univ Leeds, Sch Phys & Astron, Leeds LS2 9JT, W Yorkshire, England. [Buchholz, P.; Froehlich, U.; Kuempel, D.; Niechciol, M.; Pontz, M.; Risse, M.; Settimo, M.; Tcaciuc, R.; Younk, P.; Ziolkowski, M.] Univ Siegen, Siegen, Germany. [Bueno, A.; Gascon Bravo, A.; Lozano Bahilo, J.; Molina-Bueno, L.; Navarro, J. L.; Navas, S.; Zamorano Garcia, B.] Univ Granada, Granada, Spain. [Bueno, A.; Gascon Bravo, A.; Lozano Bahilo, J.; Molina-Bueno, L.; Navarro, J. L.; Navas, S.; Zamorano Garcia, B.] CAFPE, Granada, Spain. [Burton, R. E.; Covault, C. E.; Ferguson, A. P.; LaHurd, D.] Case Western Reserve Univ, Cleveland, OH 44106 USA. [Caballero-Mora, K. S.; Cheng, S. H.; Coutu, S.; Criss, A.; Sommers, P.; Whelan, B. J.] Penn State Univ, University Pk, PA 16802 USA. [Caccianiga, B.; Collica, L.; Miramonti, L.; Rivera, H.; Scherini, V.] Univ Milan, Milan, Italy. [Caccianiga, B.; Collica, L.; Miramonti, L.; Rivera, H.; Scherini, V.] Sezione Ist Nazl Fis Nucl, Milan, Italy. [Caruso, R.; De Domenico, M.; Garilli, G.; Insolia, A.; Italiano, A.; Pirronello, V.; Scuderi, M.; Trovato, E.] Univ Catania, Catania, Italy. [Caruso, R.; De Domenico, M.; Garilli, G.; Insolia, A.; Italiano, A.; Pirronello, V.; Scuderi, M.; Trovato, E.] Sezione Ist Nazl Fis Nucl, Catania, Italy. [Catalano, O.; La Rosa, G.; Maccarone, M. C.; Segreto, A.] Ist Astrofis Spaziale & Fis Cosm Palermo INAF, Palermo, Italy. [Chirinos Diaz, J.; Dhital, N.; Fick, B.; Kieckhafer, R. M.; Nitz, D.; Yapici, T.] Michigan Technol Univ, Houghton, MI 49931 USA. [Coppens, J.; de Jong, S. J.; Falcke, H.; Grebe, S.; Hoerandel, J. R.; Jansen, S.; Nelles, A.; Schoorlemmer, H.; Timmermans, C.] NIKHEF H, NL-1009 DB Amsterdam, Netherlands. [Cronin, J.; Facal San Luis, P.; Fang, K.; Hollon, N.; Ionita, F.; Kotera, K.; Monasor, M.; Olinto, A.; Privitera, P.; Rouille-d'Orfeuil, B.; Williams, C.; Yamamoto, T.; Zhou, J.] Univ Chicago, Enrico Fermi Inst, Chicago, IL 60637 USA. [Dasso, S.; Rovero, A. 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F.] Ist Nazl Fis Nucl, Lab Nazl Gran Sasso, Laquila, Italy. [Diep, P. N.; Dong, P. N.; Nhung, P. T.; Thao, N. T.] Inst Nucl Sci & Technol, Hanoi, Vietnam. [Erdmann, M.; Fliescher, S.; Hebbeker, T.; Kuempel, D.; Meurer, C.; Mueller, G.; Plum, M.; Scharf, N.; Schiffer, P.; Stephan, M.; Walz, D.; Weidenhaupt, K.; Winchen, T.] Rhein Westfal TH Aachen, Phys Inst A3, Aachen, Germany. [Falcke, H.] ASTRON, Dwingeloo, Netherlands. [Filipcic, A.; Veberic, D.; Zavrtanik, D.; Zavrtanik, M.] Jozef Stefan Inst, Ljubljana, Slovenia. [Filipcic, A.; Stanic, S.; Veberic, D.; Zavrtanik, D.; Zavrtanik, M.] Univ Nova Gorica, Lab Astroparticle Phys, Nova Gorica, Slovenia. [Gambetta, S.; Pesce, R.; Petrolini, A.] Univ Genoa, Dipartimento Fis, Genoa, Italy. [Gambetta, S.; Pesce, R.; Petrolini, A.] Ist Nazl Fis Nucl, I-16146 Genoa, Italy. [Giller, M.; 'Smiallkowski, A.; Szadkowski, Z.; Tkaczyk, W.; Wieczorek, G.] Univ Lodz, PL-90131 Lodz, Poland. [Gold, M. S.; Lauer, R.; Matthews, J. A. J.] Univ New Mexico, Albuquerque, NM 87131 USA. [Horvath, P.; Hrabovsky, M.; Rossler, T.] Palacky Univ, RCPTM, CR-77147 Olomouc, Czech Republic. [Karhan, P.; Nosek, D.] Charles Univ Prague, Fac Math & Phys, Inst Particle & Nucl Phys, Prague, Czech Republic. [Keivani, A.; Matthews, J.; Shadkam, A.; Sutherland, M. S.; Yuan, G.] Louisiana State Univ, Baton Rouge, LA 70803 USA. [Kulbartz, J. K.; Schiffer, P.; Sigl, G.; van Vliet, A.] Univ Hamburg, Hamburg, Germany. [Leao, M. S. A. B.; Leigui de Oliveira, M. A.; Moura, C. A.] Univ Fed ABC, Santo Andre, SP, Brazil. [Lopez, R.; Martinez Bravo, O.; Moreno, E.; Pelayo, R.; Salazar, H.; Varela, E.] Benemerita Univ Autonoma Puebla, Puebla, Mexico. [Marquez Falcon, H. R.; Villasenor, L.] Univ Michoacana, Morelia, Michoacan, Mexico. [Martinez, H.; Zepeda, A.] IPN CINVESTAV, Ctr Invest & Estudios Avanzados, Mexico City, DF, Mexico. [Mertsch, P.; Sarkar, S.] Univ Oxford, Rudolf Peierls Ctr Theoret Phys, Oxford, England. [Meyhandan, R.] Univ Hawaii, Honolulu, HI 96822 USA. [Micheletti, M. I.] UNR, CONICET, Inst Fis Rosario IFIR, Rosario, Santa Fe, Argentina. [Micheletti, M. I.] UNR, Fac Ciencias Bioquim & Farmaceut, Rosario, Santa Fe, Argentina. [Pallotta, J.; Quel, E. J.; Ristori, P.] CITEDEF, Ctr Invest Laseres& Aplicac, Buenos Aires, DF, Argentina. [Pastor, S.] Univ Valencia, CSIC, Inst Fis Corpuscular, Valencia, Spain. [Paul, T.; Srivastava, Y. N.; Swain, J.; Widom, A.] Northeastern Univ, Boston, MA 02115 USA. [Pepe, I. M.] Univ Fed Bahia, Salvador, BA, Brazil. [Petermann, E.; Snow, G. R.] Univ Nebraska, Lincoln, NE USA. [Sarazin, F.; Schuster, D.; Wiencke, L.] Colorado Sch Mines, Golden, CO 80401 USA. [Sima, O.] Univ Bucharest, Dept Phys, Bucharest, Romania. [Spinka, H.] Argonne Natl Lab, Argonne, IL 60439 USA. [Younk, P.] Los Alamos Natl Lab, Los Alamos, NM USA. RP Abreu, P (reprint author), Univ Tecn Lisboa, LIP, Lisbon, Portugal. RI Rodriguez Frias, Maria /A-7608-2015; Inst. of Physics, Gleb Wataghin/A-9780-2017; De Mitri, Ivan/C-1728-2017; Rodriguez Fernandez, Gonzalo/C-1432-2014; Nosek, Dalibor/F-1129-2017; Moura Santos, Edivaldo/K-5313-2016; Gouffon, Philippe/I-4549-2012; de Almeida, Rogerio/L-4584-2016; De Domenico, Manlio/B-5826-2014; Abreu, Pedro/L-2220-2014; Navas, Sergio/N-4649-2014; Blanco, Francisco/F-1131-2015; Sao Carlos Institute of Physics, IFSC/USP/M-2664-2016; Conceicao, Ruben/L-2971-2014; Bueno, Antonio/F-3875-2015; Beatty, James/D-9310-2011; Bonino, Raffaella/S-2367-2016; Espadanal, Joao/I-6618-2015; De Donato, Cinzia/J-9132-2015; Vazquez, Jose Ramon/K-2272-2015; Martello, Daniele/J-3131-2012; Insolia, Antonio/M-3447-2015; Petrolini, Alessandro/H-3782-2011; de Mello Neto, Joao/C-5822-2013; Lozano-Bahilo, Julio/F-4881-2016; scuderi, mario/O-7019-2014; zas, enrique/I-5556-2015; Arqueros, Fernando/K-9460-2014; Guarino, Fausto/I-3166-2012; Brogueira, Pedro/K-3868-2012; Alves Batista, Rafael/K-6642-2012; Dutan, Ioana/C-2337-2011; Sima, Octavian/C-3565-2011; Torralba Elipe, Guillermo/A-9524-2015; Di Giulio, Claudio/B-3319-2015; Albuquerque, Ivone/H-4645-2012; Parente, Gonzalo/G-8264-2015; Alvarez-Muniz, Jaime/H-1857-2015; Valino, Ines/J-8324-2012; Carvalho Jr., Washington/H-9855-2015; Travnicek, Petr/G-8814-2014; Smida, Radomir/G-6314-2014; Ridky, Jan/H-6184-2014; Chudoba, Jiri/G-7737-2014; Horvath, Pavel/G-6334-2014; Garcia Pinto, Diego/J-6724-2014; Pastor, Sergio/J-6902-2014; Rosado, Jaime/K-9109-2014; Espirito Santo, Maria Catarina/L-2341-2014; Pimenta, Mario/M-1741-2013; Ros, German/L-4764-2014; Yushkov, Alexey/A-6958-2013; Bleve, Carla/J-2521-2012; Falcke, Heino/H-5262-2012; Fauth, Anderson/F-9570-2012; Sarkar, Subir/G-5978-2011; Caramete, Laurentiu/C-2328-2011; Nierstenhofer, Nils/H-3699-2013; Chinellato, Carola Dobrigkeit /F-2540-2011; Badescu, Alina/B-6087-2012; de souza, Vitor/D-1381-2012; Ebr, Jan/H-8319-2012; Anjos, Joao/C-8335-2013; Goncalves, Patricia /D-8229-2013; Assis, Pedro/D-9062-2013; Tome, Bernardo/J-4410-2013; dos Santos, Eva/N-6351-2013; Todero Peixoto, Carlos Jose/G-3873-2012; Prouza, Michael/F-8514-2014; Mandat, Dusan/G-5580-2014; Pech, Miroslav/G-5760-2014; Bohacova, Martina/G-5898-2014; Cazon, Lorenzo/G-6921-2014; Schovanek, Petr/G-7117-2014; Vicha, Jakub/G-8440-2014 OI Del Peral, Luis/0000-0003-2580-5668; Dembinski, Hans/0000-0003-3337-3850; Salamida, Francesco/0000-0002-9306-8447; Ravignani, Diego/0000-0001-7410-8522; Mussa, Roberto/0000-0002-0294-9071; Ulrich, Ralf/0000-0002-2535-402X; Kampert, Karl-Heinz/0000-0002-2805-0195; Zamorano, Bruno/0000-0002-4286-2835; Bonino, Raffaella/0000-0002-4264-1215; Knapp, Johannes/0000-0003-1519-1383; La Rosa, Giovanni/0000-0002-3931-2269; Asorey, Hernan/0000-0002-4559-8785; Rizi, Vincenzo/0000-0002-5277-6527; Petrera, Sergio/0000-0002-6029-1255; Andringa, Sofia/0000-0002-6397-9207; Aramo, Carla/0000-0002-8412-3846; Maccarone, Maria Concetta/0000-0001-8722-0361; Kothandan, Divay/0000-0001-9048-7518; Castellina, Antonella/0000-0002-0045-2467; maldera, simone/0000-0002-0698-4421; Matthews, James/0000-0002-1832-4420; Mertsch, Philipp/0000-0002-2197-3421; Marsella, Giovanni/0000-0002-3152-8874; Gomez Berisso, Mariano/0000-0001-5530-0180; Catalano, Osvaldo/0000-0002-9554-4128; Segreto, Alberto/0000-0001-7341-6603; Aglietta, Marco/0000-0001-8354-5388; Rodriguez Frias, Maria /0000-0002-2550-4462; De Mitri, Ivan/0000-0002-8665-1730; Rodriguez Fernandez, Gonzalo/0000-0002-4683-230X; Nosek, Dalibor/0000-0001-6219-200X; de Jong, Sijbrand/0000-0002-3120-3367; Sigl, Guenter/0000-0002-4396-645X; Cataldi, Gabriella/0000-0001-8066-7718; Navarro Quirante, Jose Luis/0000-0002-9915-1735; Mantsch, Paul/0000-0002-8382-7745; Moura Santos, Edivaldo/0000-0002-2818-8813; Gouffon, Philippe/0000-0001-7511-4115; de Almeida, Rogerio/0000-0003-3104-2724; De Domenico, Manlio/0000-0001-5158-8594; Abreu, Pedro/0000-0002-9973-7314; Navas, Sergio/0000-0003-1688-5758; Blanco, Francisco/0000-0003-4332-434X; Conceicao, Ruben/0000-0003-4945-5340; Bueno, Antonio/0000-0002-7439-4247; Beatty, James/0000-0003-0481-4952; Espadanal, Joao/0000-0002-1301-8061; De Donato, Cinzia/0000-0002-9725-1281; Vazquez, Jose Ramon/0000-0001-9217-5219; Martello, Daniele/0000-0003-2046-3910; Insolia, Antonio/0000-0002-9040-1566; Petrolini, Alessandro/0000-0003-0222-7594; de Mello Neto, Joao/0000-0002-3234-6634; Lozano-Bahilo, Julio/0000-0003-0613-140X; scuderi, mario/0000-0001-9026-5317; zas, enrique/0000-0002-4430-8117; Arqueros, Fernando/0000-0002-4930-9282; Guarino, Fausto/0000-0003-1427-9885; Brogueira, Pedro/0000-0001-6069-4073; Alves Batista, Rafael/0000-0003-2656-064X; Torralba Elipe, Guillermo/0000-0001-8738-194X; Di Giulio, Claudio/0000-0002-0597-4547; Albuquerque, Ivone/0000-0001-7328-0136; Parente, Gonzalo/0000-0003-2847-0461; Alvarez-Muniz, Jaime/0000-0002-2367-0803; Valino, Ines/0000-0001-7823-0154; Carvalho Jr., Washington/0000-0002-2328-7628; Ridky, Jan/0000-0001-6697-1393; Horvath, Pavel/0000-0002-6710-5339; Garcia Pinto, Diego/0000-0003-1348-6735; Rosado, Jaime/0000-0001-8208-9480; Espirito Santo, Maria Catarina/0000-0003-1286-7288; Pimenta, Mario/0000-0002-2590-0908; Ros, German/0000-0001-6623-1483; Falcke, Heino/0000-0002-2526-6724; Fauth, Anderson/0000-0001-7239-0288; Sarkar, Subir/0000-0002-3542-858X; Chinellato, Carola Dobrigkeit /0000-0002-1236-0789; Ebr, Jan/0000-0001-8807-6162; Goncalves, Patricia /0000-0003-2042-3759; Assis, Pedro/0000-0001-7765-3606; Tome, Bernardo/0000-0002-7564-8392; dos Santos, Eva/0000-0002-0474-8863; Todero Peixoto, Carlos Jose/0000-0003-3669-8212; Prouza, Michael/0000-0002-3238-9597; Cazon, Lorenzo/0000-0001-6748-8395; FU Comision Nacional de Energia Atomica; Fundacion Antorchas; Gobierno De La Provincia de Mendoza; Municipalidad de Malargue; NDM Holdings; Valle Las Lenas; Australian Research Council; Conselho Nacional de Desenvolvimento Cientifico e Tecnologico (CNPq); Financiadora de Estudos e Projetos (FINEP); Fundacao de Amparo a Pesquisa do Estado de Rio de Janeiro (FAPERJ); Fundacao de Amparo a Pesquisa do Estado de Sao Paulo (FAPESP); Ministerio de Ciencia e Tecnologia (MCT), Brazil; AVCR [AV0Z10100502, AV0Z10100522]; GAAV [KJB100100904]; MSMT-CR [LA08016, LG11044, MEB111003, MSM0021620859, LA08015]; TACR, Czech Republic [TA01010517]; Centre de Calcul IN2P3/CNRS; Centre National de la Recherche Scientifique (CNRS); Conseil Regional Ile-de-France; Departement Physique Nucleaire et Corpusculaire (PNC-IN2P3/CNRS); Departement Sciences de l'Univers (SDU-INSU/CNRS), France; Bundesministerium fur Bildung und Forschung (BMBF); Deutsche Forschungsgemeinschaft (DFG); Finanzministerium Baden-Wurttemberg; Helmholtz-Gemeinschaft Deutscher Forschungszentren (HGF); Ministerium fur Wissenschaft und Forschung; Nordrhein-Westfalen; Ministerium fur Wissenschaft; Forschung und Kunst; Baden-Wurttemberg, Germany; Istituto Nazionale di Fisica Nucleare (INFN); Ministero dell'Istruzione, dell'Universita e della Ricerca (MIUR), Italy; Consejo Nacional de Ciencia y Tecnologia (CONACYT), Mexico; Ministerie van Onderwijs, Cultuur en Wetenschap; Nederlandse Organisatie voor Wetenschappelijk Onderzoek (NWO); Stichting voor Fundamenteel Onderzoek der Materie (FOM), Netherlands; Ministry of Science and Higher Education, Poland [N N202 200239, N N202 207238]; Portuguese national funds; FEDER funds within COMPETE - Programa Operacional Factores de Competitividade through Fundacao para a Ciencia e a Tecnologia, Portugal; Romanian Authority for Scientific Research, UEFICDI, Romania [Ctr.Nr.1/ASPERA2 ERA-NET]; Ministry for Higher Education, Science, and Technology; Slovenian Research Agency, Slovenia; Comunidad de Madrid; FEDER funds; Ministerio de Ciencia e Innovacion and Consolider-Ingenio (CPAN), Xunta de Galicia, Spain; Science and Technology Facilities Council, United Kingdom; Department of Energy [DE-AC02-07CH11359, DE-FR02-04ER41300]; National Science Foundation [0450696]; Grainger Foundation USA; NAFOSTED, Vietnam; Marie Curie-IRSES/EPLANET, European Particle Physics Latin American Network, European Union 7th Framework Program [PIRSES-2009-GA-246806]; UNESCO FX We are very grateful to the following agencies and organizations for financial support: Comision Nacional de Energia Atomica, Fundacion Antorchas, Gobierno De La Provincia de Mendoza, Municipalidad de Malargue, NDM Holdings, and Valle Las Lenas, in gratitude for their continuing cooperation over land access, Argentina; the Australian Research Council; Conselho Nacional de Desenvolvimento Cientifico e Tecnologico (CNPq), Financiadora de Estudos e Projetos (FINEP), Fundacao de Amparo a Pesquisa do Estado de Rio de Janeiro (FAPERJ), Fundacao de Amparo a Pesquisa do Estado de Sao Paulo (FAPESP), Ministerio de Ciencia e Tecnologia (MCT), Brazil; AVCR AV0Z10100502 and AV0Z10100522, GAAV KJB100100904, MSMT-CR LA08016, LG11044, MEB111003, MSM0021620859, LA08015 and TACR TA01010517, Czech Republic; Centre de Calcul IN2P3/CNRS, Centre National de la Recherche Scientifique (CNRS), Conseil Regional Ile-de-France, Departement Physique Nucleaire et Corpusculaire (PNC-IN2P3/CNRS), Departement Sciences de l'Univers (SDU-INSU/CNRS), France; Bundesministerium fur Bildung und Forschung (BMBF), Deutsche Forschungsgemeinschaft (DFG), Finanzministerium Baden-Wurttemberg, Helmholtz-Gemeinschaft Deutscher Forschungszentren (HGF), Ministerium fur Wissenschaft und Forschung, Nordrhein-Westfalen, Ministerium fur Wissenschaft, Forschung und Kunst, Baden-Wurttemberg, Germany; Istituto Nazionale di Fisica Nucleare (INFN), Ministero dell'Istruzione, dell'Universita e della Ricerca (MIUR), Italy; Consejo Nacional de Ciencia y Tecnologia (CONACYT), Mexico; Ministerie van Onderwijs, Cultuur en Wetenschap, Nederlandse Organisatie voor Wetenschappelijk Onderzoek (NWO), Stichting voor Fundamenteel Onderzoek der Materie (FOM), Netherlands; Ministry of Science and Higher Education, grant Nos. N N202 200239 and N N202 207238, Poland; Portuguese national funds and FEDER funds within COMPETE - Programa Operacional Factores de Competitividade through Fundacao para a Ciencia e a Tecnologia, Portugal; Romanian Authority for Scientific Research, UEFICDI, Ctr.Nr.1/ASPERA2 ERA-NET, Romania; Ministry for Higher Education, Science, and Technology, Slovenian Research Agency, Slovenia; Comunidad de Madrid, FEDER funds, Ministerio de Ciencia e Innovacion and Consolider-Ingenio 2010 (CPAN), Xunta de Galicia, Spain; Science and Technology Facilities Council, United Kingdom; Department of Energy, Contract Nos. DE-AC02-07CH11359, DE-FR02-04ER41300, National Science Foundation, grant No. 0450696, The Grainger Foundation USA; NAFOSTED, Vietnam; Marie Curie-IRSES/EPLANET, European Particle Physics Latin American Network, European Union 7th Framework Program, grant No. PIRSES-2009-GA-246806; and UNESCO. NR 24 TC 14 Z9 15 U1 4 U2 90 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 2041-8205 J9 ASTROPHYS J LETT JI Astrophys. J. Lett. PD JAN 1 PY 2013 VL 762 IS 1 AR L13 DI 10.1088/2041-8205/762/1/L13 PG 8 WC Astronomy & Astrophysics SC Astronomy & Astrophysics GA 056KS UT WOS:000312488400013 ER PT J AU Whalen, DJ Fryer, CL Holz, DE Heger, A Woosley, SE Stiavelli, M Even, W Frey, LH AF Whalen, Daniel J. Fryer, Chris L. Holz, Daniel E. Heger, Alexander Woosley, S. E. Stiavelli, Massimo Even, Wesley Frey, Lucille H. TI SEEING THE FIRST SUPERNOVAE AT THE EDGE OF THE UNIVERSE WITH JWST SO ASTROPHYSICAL JOURNAL LETTERS LA English DT Article DE early universe; galaxies: high-redshift; hydrodynamics; radiative transfer; stars: early-type; supernovae: general ID PAIR-INSTABILITY SUPERNOVAE; POPULATION III STARS; SHOCK BREAKOUT; PRIMORDIAL SUPERNOVAE; MASSIVE STARS; LIGHT CURVES; EVOLUTION; BINARIES; REDSHIFT AB The first stars ended the cosmic dark ages and created the first heavy elements necessary for the formation of planets and life. The properties of these stars remain uncertain, and it may be decades before individual Population III (Pop III) stars are directly observed. Their masses, however, can be inferred from their supernova explosions, which may soon be found in both deep-field surveys by the James Webb Space Telescope (JWST) and in all-sky surveys by the Wide Field Infrared Survey Telescope (WFIRST). We have performed radiation hydrodynamical simulations of the near-infrared signals of Pop III pair-instability supernovae in realistic circumstellar environments with Lyman absorption by the neutral intergalactic medium. We find that JWST and WFIRST will detect these explosions out to z similar to 30 and 20, respectively, unveiling the first generation of stars in the universe. C1 [Whalen, Daniel J.] Carnegie Mellon Univ, Dept Phys, Pittsburgh, PA 15213 USA. [Fryer, Chris L.] Los Alamos Natl Lab, CCS 2, Los Alamos, NM 87545 USA. [Holz, Daniel E.] Univ Chicago, Dept Phys, Enrico Fermi Inst, Chicago, IL 60637 USA. [Holz, Daniel E.] Univ Chicago, Kavli Inst Cosmol Phys, Chicago, IL 60637 USA. [Heger, Alexander] Monash Univ, Monash Ctr Astrophys, Clayton, Vic 3800, Australia. [Woosley, S. E.] Univ Calif Santa Cruz, Dept Astron & Astrophys, Santa Cruz, CA 95064 USA. [Stiavelli, Massimo] Space Telescope Sci Inst, Baltimore, MD 21218 USA. [Even, Wesley; Frey, Lucille H.] Los Alamos Natl Lab, XTD 6, Los Alamos, NM 87545 USA. [Frey, Lucille H.] Univ New Mexico, Dept Comp Sci, Albuquerque, NM 87131 USA. RP Whalen, DJ (reprint author), Carnegie Mellon Univ, Dept Phys, Pittsburgh, PA 15213 USA. OI Frey, Lucille/0000-0002-5478-2293; Even, Wesley/0000-0002-5412-3618 FU Bruce and Astrid McWilliams Center for Cosmology at Carnegie Mellon University; National Science Foundation [PHY-1151836, AST 0909129]; US Department of Energy [DE-FC02-01ER41176, FC02-09ER41618, DE-FG02-87ER40328]; NASA Theory Program [NNX09AK36G]; NASA JWST [NAG5-12458]; National Nuclear Security Administration of the U.S. Department of Energy at Los Alamos National Laboratory [DE-AC52-06NA25396] FX The authors thank the anonymous referee, whose comments improved the quality of this Letter. D.J.W. was supported by the Bruce and Astrid McWilliams Center for Cosmology at Carnegie Mellon University. D. E. H. acknowledges support from the National Science Foundation CAREER grant PHY-1151836. A. H. was supported by the US Department of Energy under contracts DE-FC02-01ER41176, FC02-09ER41618 (SciDAC), and DE-FG02-87ER40328. S. E. W. was supported by the National Science Foundation grant AST 0909129 and the NASA Theory Program grant NNX09AK36G. M. S. thanks Marcia Rieke for making available the NIRCam filter curves, and was partially supported by NASA JWST grant NAG5-12458. Work at LANL was done 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 29 TC 37 Z9 37 U1 1 U2 11 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 2041-8205 J9 ASTROPHYS J LETT JI Astrophys. J. Lett. PD JAN 1 PY 2013 VL 762 IS 1 AR L6 DI 10.1088/2041-8205/762/1/L6 PG 5 WC Astronomy & Astrophysics SC Astronomy & Astrophysics GA 056KS UT WOS:000312488400006 ER PT J AU Zhang, L Tong, HM Garewal, M Ren, G AF Zhang, Lei Tong, Huimin Garewal, Mark Ren, Gang TI Optimized negative-staining electron microscopy for lipoprotein studies SO BIOCHIMICA ET BIOPHYSICA ACTA-GENERAL SUBJECTS LA English DT Review DE Protein structure; Lipoprotein structure; Electron microscopy; Negative-staining; Optimized negative-staining protocol; Individual-particle electron tomography ID HIGH-DENSITY-LIPOPROTEIN; ESTER TRANSFER PROTEIN; APOLIPOPROTEIN-A-I; LECITHIN-CHOLESTEROL ACYLTRANSFERASE; LIMPET HEMOCYANIN KLH; LIPID-BINDING; VITREOUS ICE; CRYOELECTRON MICROSCOPY; PHOSPHOTUNGSTIC ACID; STRUCTURAL-ANALYSIS AB Background: Negative-staining (NS), a rapid, simple and conventional technique of electron microscopy (EM), has been commonly used to initially study the morphology and structure of proteins for half a century. Certain NS protocols however can cause artifacts, especially for structurally flexible or lipid-related proteins, such as lipoproteins. Lipoproteins were often observed in the form of rouleau as lipoprotein particles appeared to be stacked together by conventional NS protocols. The flexible components of lipoproteins, i.e. lipids and amphipathic apolipoproteins, resulted in the lipoprotein structure being sensitive to the NS sample preparation parameters, such as operational procedures, salt concentrations, and the staining reagents. Scope of review: The most popular NS protocols that have been used to examine lipoprotein morphology and structure were reviewed. Major conclusions: The comparisons show that an optimized NS (OpNS) protocol can eliminate the rouleau artifacts of lipoproteins, and that the lipoproteins are similar in size and shape as statistically measured from two EM methods, OpNS and cryo-electron microscopy (cryo-EM). OpNS is a high-throughput, high-contrast and high-resolution (near 1 nm, but rarely better than 1 nm) method which has been used to discover the mechanics of a small protein, 53 kDa cholesterol ester transfer protein (CETP), and the structure of an individual particle of a single protein by individual-particle electron tomography (IPET), i.e. a 14 angstrom-resolution IgG antibody three-dimensional map. General significance: It is suggested that OpNS can be used as a general protocol to study the structure of proteins, especially highly dynamic proteins with equilibrium-fluctuating structures. Published by Elsevier B.V. C1 [Zhang, Lei; Tong, Huimin; Garewal, Mark; Ren, Gang] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA. RP Ren, G (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA. EM gren@lbl.gov RI Foundry, Molecular/G-9968-2014; Zhang, Lei/G-6427-2012 OI Zhang, Lei/0000-0002-4880-824X FU Office of Science, Office of Basic Energy Sciences of the United States Department of Energy [DE-AC02-05CH11231]; National Heart, Lung, And Blood Institute of the National Institutes of Health [R01HL115153] FX We thank Mr. Matthew J. Rames for editing comments. This work was supported by the Office of Science, Office of Basic Energy Sciences of the United States Department of Energy (contract no. DE-AC02-05CH11231) and the National Heart, Lung, And Blood Institute of the National Institutes of Health (no. R01HL115153). NR 93 TC 11 Z9 11 U1 5 U2 34 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0304-4165 J9 BBA-GEN SUBJECTS JI Biochim. Biophys. Acta-Gen. Subj. PD JAN PY 2013 VL 1830 IS 1 BP 2150 EP 2159 DI 10.1016/j.bbagen.2012.09.016 PG 10 WC Biochemistry & Molecular Biology; Biophysics SC Biochemistry & Molecular Biology; Biophysics GA 056EE UT WOS:000312470400005 PM 23032862 ER PT J AU Surace, C Archibald, R Saxena, R AF Surace, Cecilia Archibald, Richard Saxena, Rishu TI On the use of the polynomial annihilation edge detection for locating cracks in beam-like structures SO COMPUTERS & STRUCTURES LA English DT Article DE Cracked cantilever beam; Bending vibration; Mode shapes first derivative; Discontinuity; Polynomial annihilation edge detection ID WAVELET-BASED APPROACH; DAMAGE DETECTION; MODE SHAPES; IDENTIFICATION; FREQUENCY; ROTATION AB A crack in a structure causes a discontinuity in the first derivative of the mode shapes: On this basis, a numerical method for detecting discontinuities in smooth piecewise functions and their derivatives, based on a polynomial annihilation technique, has been applied to the problem of crack detection and localisation in beam-like structures for which only post-damage mode shapes are available. Using a finite-element model of a cracked beam, the performance of this methodology has been analysed for different crack depths and increasing amounts of noise. Given the crack position, a procedure to estimate its depth is also proposed and corresponding results shown. (C) 2012 Elsevier Ltd. All rights reserved. C1 [Surace, Cecilia] Politecn Torino, Dept Struct Bldg & Geotech Engn, I-10129 Turin, Italy. [Archibald, Richard] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. [Saxena, Rishu] Univ Calif San Diego, Dept Math, La Jolla, CA 92093 USA. RP Surace, C (reprint author), Politecn Torino, Dept Struct Bldg & Geotech Engn, I-10129 Turin, Italy. EM cecilia.surace@polito.it RI Archibald, Rick/I-6238-2016 OI Archibald, Rick/0000-0002-4538-9780 NR 28 TC 12 Z9 12 U1 0 U2 14 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0045-7949 J9 COMPUT STRUCT JI Comput. Struct. PD JAN PY 2013 VL 114 BP 72 EP 83 DI 10.1016/j.compstruc.2012.10.008 PG 12 WC Computer Science, Interdisciplinary Applications; Engineering, Civil SC Computer Science; Engineering GA 056DC UT WOS:000312467600007 ER PT J AU Houde, S Todd, A Sudarshan, A Flora, JA Armel, KC AF Houde, Sebastien Todd, Annika Sudarshan, Anant Flora, June A. Armel, K. Carrie TI Real-time Feedback and Electricity Consumption: A Field Experiment Assessing the Potential for Savings and Persistence SO ENERGY JOURNAL LA English DT Article DE Feedback Technology; Residential Electricity Consumption; Field Experiment ID ENERGY AB Real-time information feedback delivered via technology has been reported to produce up to 20 percent declines in residential energy consumption. There are however large differences in estimates of the effect of real-time feedback technologies on energy use. In this study, we conduct a field experiment to obtain an estimate of the impact of a real-time feedback technology. Access to feedback leads to an average reduction in household electricity consumption of 5.7 percent. Significant declines persist for up to four weeks. In examining time of day reduction effects, we find that the largest reductions were observed initially at all times of the day but as time passes, morning and evening intervals show larger reductions. We find no convincing evidence that household characteristics explain heterogeneity in our treatment effects; we examine demographics, housing characteristics and psychological variables. C1 [Houde, Sebastien] Stanford Univ, Dept Management Sci & Engn, Stanford, CA 94305 USA. [Todd, Annika] Lawrence Berkeley Natl Lab, Berkeley, CA 94703 USA. [Sudarshan, Anant] Harvard Univ, Harvard Kenney Sch Govt, Cambridge, MA 02138 USA. [Flora, June A.] Stanford Univ, H STAR Human Sci & Technol Adv Res Inst, Stanford, CA 94305 USA. [Armel, K. Carrie] Stanford Univ, Precourt Energy Efficiency Ctr, Stanford, CA 94305 USA. RP Houde, S (reprint author), Stanford Univ, Dept Management Sci & Engn, Stanford, CA 94305 USA. EM shoude@stanford.edu; ATodd@lbl.gov; anant_sudarshan@hks.harvard.edu; j.flora@sitia.org; kcarmel@stanford.edu RI Houde, Sebastien/C-1335-2015 OI Houde, Sebastien/0000-0002-2889-6692 NR 10 TC 11 Z9 11 U1 2 U2 27 PU INT ASSOC ENERGY ECONOMICS PI CLEVELAND PA 28790 CHAGRIN BLVD, STE 210, CLEVELAND, OH 44122 USA SN 0195-6574 J9 ENERG J JI Energy J. PY 2013 VL 34 IS 1 BP 87 EP 102 DI 10.5547/01956574.34.1.4 PG 16 WC Economics; Energy & Fuels; Environmental Studies SC Business & Economics; Energy & Fuels; Environmental Sciences & Ecology GA 056CP UT WOS:000312466300004 ER PT J AU Balbus, JM Boxall, ABA Fenske, RA McKone, TE Zeise, L AF Balbus, John M. Boxall, Alistair B. A. Fenske, Richard A. McKone, Thomas E. Zeise, Lauren TI Implications of global climate change for the assessment and management of human health risks of chemicals in the natural environment SO ENVIRONMENTAL TOXICOLOGY AND CHEMISTRY LA English DT Review DE Toxicology; Exposure pathway; Risk assessment; Vulnerability ID SAN-FRANCISCO BAY; POLYCHLORINATED-BIPHENYLS; PARTICULATE MATTER; AIR-POLLUTION; TEMPERATURE MODIFY; UNITED-STATES; NMMAPS DATA; HEAT-WAVE; MORTALITY; OZONE AB Global climate change (GCC) is likely to alter the degree of human exposure to pollutants and the response of human populations to these exposures, meaning that risks of pollutants could change in the future. The present study, therefore, explores how GCC might affect the different steps in the pathway from a chemical source in the environment through to impacts on human health and evaluates the implications for existing risk-assessment and management practices. In certain parts of the world, GCC is predicted to increase the level of exposure of many environmental pollutants due to direct and indirect effects on the use patterns and transport and fate of chemicals. Changes in human behavior will also affect how humans come into contact with contaminated air, water, and food. Dietary changes, psychosocial stress, and coexposure to stressors such as high temperatures are likely to increase the vulnerability of humans to chemicals. These changes are likely to have significant implications for current practices for chemical assessment. Assumptions used in current exposure-assessment models may no longer apply, and existing monitoring methods may not be robust enough to detect adverse episodic changes in exposures. Organizations responsible for the assessment and management of health risks of chemicals therefore need to be more proactive and consider the implications of GCC for their procedures and processes. Environ. Toxicol. Chem. 2013;32:6278. (c) 2012 SETAC C1 [Balbus, John M.] NIEHS, Bethesda, MD USA. [Boxall, Alistair B. A.] Univ York, Dept Environm, York YO10 5DD, N Yorkshire, England. [Fenske, Richard A.] Univ Washington, Sch Publ Hlth, Seattle, WA 98195 USA. [McKone, Thomas E.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Zeise, Lauren] Calif Environm Protect Agcy, Off Environm Hlth Hazard Assessment, Sacramento, CA USA. RP Balbus, JM (reprint author), NIEHS, Bethesda, MD USA. EM john.balbus@nih.gov FU U.S. Department of Energy (DOE) [DE-AC02-05CH11231]; American Chemistry Council; Conestoga-Rover and Associates; E.I. du Pont de Nemours Co.; Environ Corp; Exponent; NIEHS Superfund Research Program; National Oceanic and Atmospheric Administration; National Council for Air and Stream Improvement; Norwegian Institute for Water Research; Research Council of Norway; Society of Environ Toxicol Chem; Johnson Foundation at Wingspread; Unilever; U.S. Department of Interior Natural Resource Damage Assessment and Restoration Program; U.S. Environmental Protection Agency; U.S. Fish and Wildlife Service; U.S. Geological Survey FX This article is the work of an employee or group of employees of the National Institute of Environmental Health Sciences (NIEHS), National Institutes of Health (NIH), the California Office of Environmental Health Hazard Assessment (OEHHA), and the Lawrence Berkeley National Laboratory, which is operated by the U.S. Department of Energy (DOE) under contract DE-AC02-05CH11231; however, the statements, opinions, or conclusions contained here do not necessarily represent the statements, opinions, or conclusions of the NIEHS, NIH, DOE, U.S. government, OEHHA, California Environmental Protection Agency, or the state of California. The authors acknowledge funding for the Society of Environmental Toxicology and Chemistry international workshop, The Influence of Global Climate Change, on the Scientific Foundations and Applications of Environ Toxicol Chem, which was provided by the American Chemistry Council, Conestoga-Rover and Associates, E.I. du Pont de Nemours & Co., Environ Corp, Exponent, NIEHS Superfund Research Program, National Oceanic and Atmospheric Administration, National Council for Air and Stream Improvement, Norwegian Institute for Water Research, Research Council of Norway, Society of Environ Toxicol Chem, Johnson Foundation at Wingspread, Unilever, U.S. Department of Interior Natural Resource Damage Assessment and Restoration Program, U.S. Environmental Protection Agency, U.S. Fish and Wildlife Service, and U.S. Geological Survey. The authors would like to thank J. Lee of MDB, Inc. for her outstanding assistance with manuscript preparation and submission. NR 105 TC 27 Z9 28 U1 5 U2 128 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0730-7268 J9 ENVIRON TOXICOL CHEM JI Environ. Toxicol. Chem. PD JAN PY 2013 VL 32 IS 1 BP 62 EP 78 DI 10.1002/etc.2046 PG 17 WC Environmental Sciences; Toxicology SC Environmental Sciences & Ecology; Toxicology GA 057EQ UT WOS:000312545700009 PM 23147420 ER PT J AU Marsh, GE AF Marsh, Gerald E. TI The problem of the 'prebiotic and never born proteins' SO INTERNATIONAL JOURNAL OF ASTROBIOLOGY LA English DT Article DE Protein evolution; RNA-world ID RNA; CHEMISTRY; EVOLUTION; ENZYMES AB It has been argued that the limited set of proteins used by life as we know could not have arisen by the process of Darwinian selection from all possible proteins. This probabilistic argument has a number of implicit assumptions that may not be warranted. A variety of considerations are presented to show that the number of amino acid sequences that need to have been sampled during the evolution of proteins is far smaller than assumed by the argument. C1 [Marsh, Gerald E.] Argonne Natl Lab, Chicago, IL 60615 USA. EM gemarsh@uchicago.edu NR 25 TC 1 Z9 1 U1 3 U2 16 PU CAMBRIDGE UNIV PRESS PI NEW YORK PA 32 AVENUE OF THE AMERICAS, NEW YORK, NY 10013-2473 USA SN 1473-5504 J9 INT J ASTROBIOL JI Int. J. Astrobiol. PD JAN PY 2013 VL 12 IS 1 BP 94 EP 98 DI 10.1017/S1473550412000468 PG 5 WC Astronomy & Astrophysics; Biology; Geosciences, Multidisciplinary SC Astronomy & Astrophysics; Life Sciences & Biomedicine - Other Topics; Geology GA 056YE UT WOS:000312526700013 ER PT J AU Burnett, JD Xu, TH Sorescu, M Strohmeier, BR Sturgeon, J Gourdon, O Baroudi, K Yao, JL Aitken, JA AF Burnett, Johanna D. Xu, Tianhong Sorescu, Monica Strohmeier, Brian R. Sturgeon, Jacqueline Gourdon, Olivier Baroudi, Kristen Yao, Jin-lei Aitken, Jennifer A. TI Location and oxidation state of iron in Fe-substituted CuInS2 chalcopyrites SO JOURNAL OF SOLID STATE CHEMISTRY LA English DT Article DE CuInS2; X-ray powder diffraction; Neutron powder diffraction; XPS; Mossbauer; Oxidation state ID X-RAY PHOTOELECTRON; THIN-FILMS; ELECTRONIC-STRUCTURE; SEMICONDUCTORS; SPECTROSCOPY; SPECTRA; XPS; MN; CUIN1-ZFEZS2; SPINTRONICS AB CuIn1-xFexS2(x=0-0.30) was synthesized via high-temperature, solid-state synthesis. Phase-pure materials were found in samples where x=0-0.15, after which a secondary phase became apparent. The materials were characterized with the use of X-ray powder diffraction (XRPD), and Reitveld refinement revealed a linear decrease in unit cell volume as the amount of iron substitution increases in accordance with Vegard's Law. Inductively coupled plasma (ICP) confirms that the actual stoichiometry is close to the nominal composition of the materials. The temperature for both the chalcopyrite-to-sphalerite and the sphalerite-to-wurtzite phase transitions decreases with increasing iron substitution for indium. These findings suggest that the Fe is being randomly incorporated into the crystal structure of the CuInS2. X-ray photoelectron spectroscopy (XPS) measurements were used to determine the oxidation state of the ions (Cu1+, In3+, and S2-), and Fe-57 Mossbauer spectroscopy verified that the iron is in the 3(+) oxidation state. Band gaps of the solid solution were estimated to be in the range of 0.70-0.85 eV. Rietveld refinement of neutron diffraction data indicates that the iron is occupying the In site within the chalcopyrite structure. (C) 2012 Elsevier Inc. All rights reserved. C1 [Burnett, Johanna D.; Baroudi, Kristen; Yao, Jin-lei; Aitken, Jennifer A.] Duquesne Univ, Dept Chem & Biochem, Pittsburgh, PA 15282 USA. [Xu, Tianhong; Sorescu, Monica] Duquesne Univ, Dept Phys, Pittsburgh, PA 15282 USA. [Strohmeier, Brian R.; Sturgeon, Jacqueline] RJ Lee Grp Inc, Monroeville, PA 15146 USA. [Strohmeier, Brian R.] Thermo Fisher Sci, Madison, WI 53711 USA. [Gourdon, Olivier] Oak Ridge Natl Lab, Spallat Neutron Source, Chem & Engn Mat Div, Oak Ridge, TN 37831 USA. RP Aitken, JA (reprint author), Duquesne Univ, Dept Chem & Biochem, 600 Forbes Ave, Pittsburgh, PA 15282 USA. EM aitkenj@duq.edu RI Yao, Jinlei/D-4977-2012; OI Aitken, Jennifer/0000-0001-8281-5091 FU Scientific User Facilities Division, Office of Basic Energy Sciences, U. S. Department of Energy; National Science Foundation (NSF) [DMR-0511444, DMR-1201729] FX The authors thank Oak Ridge National Laboratory's (ORNL) Spallation Neutron Source (SNS) which is sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, U. S. Department of Energy. POWGEN workshop, IPTS-5857. We also thank Ashfia Huq from ORNL's SNS for her valuable help. This work has been made possible through the following grants: National Science Foundation (NSF), Grant No. DMR-0511444 (providing funds for the X-ray powder diffractometer), and DMR-1201729. NR 61 TC 9 Z9 9 U1 1 U2 58 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 0022-4596 EI 1095-726X J9 J SOLID STATE CHEM JI J. Solid State Chem. PD JAN PY 2013 VL 197 BP 279 EP 287 DI 10.1016/j.jssc.2012.08.043 PG 9 WC Chemistry, Inorganic & Nuclear; Chemistry, Physical SC Chemistry GA 053NZ UT WOS:000312281000040 ER PT J AU Nichols, EJ Shi, JWJ Huq, A Vogel, SC Misture, ST AF Nichols, Eric J. Shi, Jiawanjun Huq, Ashfia Vogel, Sven C. Misture, Scott T. TI Controlling structure distortions in 3-layer ferroelectric Aurivillius oxides SO JOURNAL OF SOLID STATE CHEMISTRY LA English DT Article DE Aurivillius; Ferroelectric; Photocatalyst; Multiferroic; Octahedral distortion ID NEUTRON POWDER DIFFRACTION; CATION DISORDER; VISIBLE-LIGHT; PHOTOCATALYTIC ACTIVITIES; NIOBATE NANOSHEETS; CRYSTAL-STRUCTURES; LAYERED TITANATE; THIN-FILMS; PHASES; CA AB Combined Rietveld refinements of x-ray and neutron powder diffraction data were used to understand the subtle structure distortions in 3-layer Aurivillius oxides that yield off-centering displacements in ferroelectric and multiferroic compositions. Ferroelectric phases including Bi(2)A(2)Ti(3)O(12) (A=La, Pr, Nd, La/Pr, La/Nd, Pr/Nd), Bi(2)A(2)TiNb(2)O(12) (A=Ca/Sr, Sr. and Sr/Ba) and Bi(2)A(2)TiTa(2)O(12) (A=Ca/Sr, and Sr/Ba) were studied to separate the effects of cation size and charge on the structure distortions and properties. A new approach to describing the local coordination around the Ti, Nb, and/or Ta ions is presented, where the oxygen octahedra are characterized as containing kinks in three dimensions. The kink angles follow trends with the A-site ionic radius and the ferroelectric polarization. The driving force for extensive cation site mixing between the Bi and A-site cations has been clearly established, with site mixing required to maintain interlayer bonding. (C) 2012 Elsevier Inc. All rights reserved. C1 [Nichols, Eric J.; Shi, Jiawanjun; Misture, Scott T.] Alfred Univ, Kazuo Inamori Sch Engn, Alfred, NY 14802 USA. [Huq, Ashfia] Oak Ridge Natl Lab, Neutron Scattering Sci Div, Oak Ridge, TN 37831 USA. [Vogel, Sven C.] Los Alamos Natl Lab, Manuel Lujan Jr Neutron Scattering Ctr, Los Alamos, NM 87545 USA. RP Misture, ST (reprint author), Alfred Univ, Kazuo Inamori Sch Engn, Alfred, NY 14802 USA. EM misture@alfred.edu RI Lujan Center, LANL/G-4896-2012; Huq, Ashfia/J-8772-2013; OI Huq, Ashfia/0000-0002-8445-9649; Vogel, Sven C./0000-0003-2049-0361 FU National Science Foundation [DMR 0606246]; US Department of Energy [W-7405-ENG-36]; US Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-98CH10886]; Scientific User Facilities Division, Office of Basic Energy Sciences, US Department of Energy FX This material is based upon work supported by the National Science Foundation under Grant no. DMR 0606246. This work has benefited from the use of the Los Alamos Neutron Science Center (LANSCE) at the Los Alamos National Laboratory. LANSCE is funded by the US Department of Energy under Contract W-7405-ENG-36. Use of the National Synchrotron Light Source, Brookhaven National Laboratory, was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract no. DE-AC02-98CH10886. The research at Oak Ridge National Laboratory's Spallation Neutron Source was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, US Department of Energy. NR 62 TC 3 Z9 3 U1 3 U2 90 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 0022-4596 J9 J SOLID STATE CHEM JI J. Solid State Chem. PD JAN PY 2013 VL 197 BP 475 EP 482 DI 10.1016/j.jssc.2012.09.025 PG 8 WC Chemistry, Inorganic & Nuclear; Chemistry, Physical SC Chemistry GA 053NZ UT WOS:000312281000068 ER PT J AU Curtis, T Daran, JM Pronk, JT Frey, J Jansson, JK Robbins-Pianka, A Knight, R Schnurer, A Smets, BF Smid, EJ Abee, T Vicente, M Zengler, K AF Curtis, Tom Daran, Jean-Marc Pronk, Jack T. Frey, Joachim Jansson, Janet K. Robbins-Pianka, Adam Knight, Rob Schnurer, Anna Smets, Barth F. Smid, E. J. Abee, T. Vicente, Miguel Zengler, Karsten TI Crystal ball-2013 SO MICROBIAL BIOTECHNOLOGY LA English DT Article ID ESCHERICHIA-COLI; CELL-DIVISION; LISTERIA-MONOCYTOGENES; YEAST TRANSFORMATION; PROTEIN; GENOME; MODEL; FTSZ; DNA; RECOMBINATION C1 [Curtis, Tom] Newcastle Univ, Sch Civil Engn & Geosci, Newcastle Upon Tyne NE1 7RU, Tyne & Wear, England. Delft Univ Technol, Dept Biotechnol, NL-2628 BC Delft, Netherlands. Kluyver Ctr Genom Ind Fermentat, NL-2628 BC Delft, Netherlands. [Frey, Joachim] Univ Bern, Inst Vet Bacteriol, CH-3001 Bern, Switzerland. [Jansson, Janet K.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Dept Ecol, Div Earth Sci, Berkeley, CA 94720 USA. [Knight, Rob] Howard Hughes Med Inst, Boulder, CO 80309 USA. [Knight, Rob] Univ Colorado, Dept Comp Sci, BioFrontiers Inst, Dept Chem & Biochem, Boulder, CO 80309 USA. [Schnurer, Anna] Swedish Univ Agr Sci, Dept Microbiol, Bioctr, S-75007 Uppsala, Sweden. [Smets, Barth F.] Tech Univ Denmark, Dept Environm Engn, DK-2800 Lyngby, Denmark. [Smid, E. J.; Abee, T.] Wageningen Univ, Food Microbiol Lab, NL-6700 EV Wageningen, Netherlands. [Vicente, Miguel] CNB CSIC, E-28049 Madrid, Spain. [Zengler, Karsten] Tech Univ Denmark, Novo Nordisk Fdn, Ctr Biosustainabil, DK-2800 Lyngby, Denmark. [Zengler, Karsten] Univ Calif San Diego, Dept Bioengn, San Diego, CA 92103 USA. RP Curtis, T (reprint author), Newcastle Univ, Sch Civil Engn & Geosci, Newcastle Upon Tyne NE1 7RU, Tyne & Wear, England. RI Smets, Barth/A-5076-2014; Knight, Rob/D-1299-2010 OI Smets, Barth/0000-0003-4119-6292; NR 75 TC 6 Z9 6 U1 0 U2 67 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 1751-7907 J9 MICROB BIOTECHNOL JI Microb. Biotechnol. PD JAN PY 2013 VL 6 IS 1 BP 3 EP 16 DI 10.1111/1751-7915.12014 PG 14 WC Biotechnology & Applied Microbiology; Microbiology SC Biotechnology & Applied Microbiology; Microbiology GA 058TK UT WOS:000312656900002 ER PT J AU Shao, XM Lay, EH Jacobson, AR AF Shao, Xuan-Min Lay, Erin H. Jacobson, Abram R. TI Reduction of electron density in the night-time lower ionosphere in response to a thunderstorm SO NATURE GEOSCIENCE LA English DT Article ID GRAVITY-WAVES; IONIZATION; DISCHARGES AB Tropospheric thunderstorms have been reported to disturb the lower ionosphere, at altitudes of 65-90 km, by convective atmospheric gravity waves(1-5) and by electric field changes produced by lightning discharges(6-15). Theoretical simulations suggest that lightning electric fields enhance electron attachment to O-2 and reduce electron density in the lower ionosphere(7,8). Owing to the low electron density in the lower ionosphere, active probing of its electron distribution is difficult(16,17), and the various perturbative effects are poorly understood. However, it is now possible to probe the lower ionosphere in a spatially and temporally resolved manner by using remotely detected time waveforms of lightning radio signals(4,5,18,19). Here we report such observations of the night-time ionosphere above a small thunderstorm. We find that electron density in the lower ionosphere decreased in response to lightning discharges. The extent of the reduction is closely related in time and space to the rate of lightning discharges, supporting the idea that the enhanced electron attachment is responsible for the reduction. We conclude that ionospheric electron density variations corresponding to lightning discharges should be considered in future simulations of the ionosphere and the initiation of sprite discharges. C1 [Shao, Xuan-Min; Lay, Erin H.] Los Alamos Natl Lab, Space & Remote Sensing Grp, Los Alamos, NM 87545 USA. [Jacobson, Abram R.] Univ Washington, Earth & Space Sci Dept, Seattle, WA 98195 USA. RP Shao, XM (reprint author), Los Alamos Natl Lab, Space & Remote Sensing Grp, ISR-2,MS D436, Los Alamos, NM 87545 USA. EM xshao@lanl.gov OI Lay, Erin/0000-0002-1310-9035 FU Los Alamos National Laboratory by Laboratory Directed Research and Development project [20110184ER] FX This research was supported by the Los Alamos National Laboratory by Laboratory Directed Research and Development project 20110184ER. We thank P.Colestock and J.Zinn for useful discussions on air chemistry. NR 30 TC 18 Z9 21 U1 2 U2 23 PU NATURE PUBLISHING GROUP PI NEW YORK PA 75 VARICK ST, 9TH FLR, NEW YORK, NY 10013-1917 USA SN 1752-0894 J9 NAT GEOSCI JI Nat. Geosci. PD JAN PY 2013 VL 6 IS 1 BP 29 EP 33 DI 10.1038/NGEO1668 PG 5 WC Geosciences, Multidisciplinary SC Geology GA 058KQ UT WOS:000312633000023 ER PT J AU Bale, HA Haboub, A MacDowell, AA Nasiatka, JR Parkinson, DY Cox, BN Marshall, DB Ritchie, RO AF Bale, Hrishikesh A. Haboub, Abdel MacDowell, Alastair A. Nasiatka, James R. Parkinson, Dilworth Y. Cox, Brian N. Marshall, David B. Ritchie, Robert O. TI Real-time quantitative imaging of failure events in materials under load at temperatures above 1,600 degrees C SO NATURE MATERIALS LA English DT Article ID STRENGTH DISTRIBUTION; FIBER COMPOSITES; MATRIX CRACKING; TOMOGRAPHY AB Ceramic matrix composites are the emerging material of choice for structures that will see temperatures above similar to 1,500 degrees C in hostile environments, as for example in next-generation gas turbines and hypersonic-flight applications. The safe operation of applications depends on how small cracks forming inside the material are restrained by its microstructure. As with natural tissue such as bone and seashells, the tailored microstructural complexity of ceramic matrix composites imparts them with mechanical toughness, which is essential to avoiding failure. Yet gathering three-dimensional observations of damage evolution in extreme environments has been a challenge. Using synchrotron X-ray computed microtomography, we have fully resolved sequences of microcrack damage as cracks grow under load at temperatures up to 1,750 degrees C. Our observations are key ingredients for the high-fidelity simulations used to compute failure risks under extreme operating conditions. C1 [Bale, Hrishikesh A.; Ritchie, Robert O.] Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA. [Haboub, Abdel; MacDowell, Alastair A.; Nasiatka, James R.; Parkinson, Dilworth Y.; Ritchie, Robert O.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Cox, Brian N.; Marshall, David B.] Teledyne Sci Co, Thousand Oaks, CA 91360 USA. RP Ritchie, RO (reprint author), Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA. EM roritchie@lbl.gov RI Ritchie, Robert/A-8066-2008; Parkinson, Dilworth/A-2974-2015 OI Ritchie, Robert/0000-0002-0501-6998; Parkinson, Dilworth/0000-0002-1817-0716 FU Air Force Office of Scientific Research; NASA under the National Hypersonics Science Center for Materials and Structures (AFOSR) [FA9550-09-1-0477]; Office of Science of the US Department of Energy [DE-AC02-05CH11231] FX Work supported by the Air Force Office of Scientific Research (A. Sayir) and NASA (A. Calomino) under the National Hypersonics Science Center for Materials and Structures (AFOSR Contract No. FA9550-09-1-0477). We acknowledge the use of the X-ray synchrotron micro-tomography beam line (8.3.2) at the Advanced Light Source (ALS) at the Lawrence Berkeley National Laboratory, which is supported by the Office of Science of the US Department of Energy under contract no. DE-AC02-05CH11231. NR 23 TC 39 Z9 40 U1 7 U2 128 PU NATURE PUBLISHING GROUP PI LONDON PA MACMILLAN BUILDING, 4 CRINAN ST, LONDON N1 9XW, ENGLAND SN 1476-1122 EI 1476-4660 J9 NAT MATER JI Nat. Mater. PD JAN PY 2013 VL 12 IS 1 BP 40 EP 46 DI 10.1038/NMAT349 PG 7 WC Chemistry, Physical; Materials Science, Multidisciplinary; Physics, Applied; Physics, Condensed Matter SC Chemistry; Materials Science; Physics GA 057WA UT WOS:000312593600018 PM 23223124 ER PT J AU Shi, XY Logvenov, G Bollinger, AT Bozovic, I Panagopoulos, C Popovic, D AF Shi, Xiaoyan Logvenov, G. Bollinger, A. T. Bozovic, I. Panagopoulos, C. Popovic, Dragana TI Emergence of superconductivity from the dynamically heterogeneous insulating state in La2-xSrxCuO4 SO NATURE MATERIALS LA English DT Article ID TEMPERATURE; TRANSITION; MAGNETORESISTANCE; RESISTANCE; OXIDES; FIELD AB A central issue for copper oxides is the nature of the insulating ground state at low carrier densities and the emergence of high-temperature superconductivity from that state with doping. Even though this superconductor-insulator transition (SIT) is a zero-temperature transition, measurements are not usually carried out at low temperatures. Here we use magnetoresistance to probe both the insulating state at very low temperatures and the presence of superconducting fluctuations in La2-xSrxCuO4 films, for doping levels that range from the insulator to the superconductor (x = 0.03-0.08). We observe that the charge glass behaviour, characteristic of the insulating state, is suppressed with doping, but it coexists with superconducting fluctuations that emerge already on the insulating side of the SIT. The unexpected quenching of the superconducting fluctuations by the competing charge order at low temperatures provides a new perspective on the mechanism for the SIT. C1 [Shi, Xiaoyan; Popovic, Dragana] Florida State Univ, Natl High Magnet Field Lab, Tallahassee, FL 32310 USA. [Shi, Xiaoyan; Popovic, Dragana] Florida State Univ, Dept Phys, Tallahassee, FL 32310 USA. [Logvenov, G.; Bollinger, A. T.; Bozovic, I.] Brookhaven Natl Lab, Upton, NY 11973 USA. [Logvenov, G.] Max Planck Inst Solid State Res, D-70569 Stuttgart, Germany. [Panagopoulos, C.] Univ Crete, Dept Phys, GR-71003 Iraklion, Greece. [Panagopoulos, C.] FORTH, GR-71003 Iraklion, Greece. [Panagopoulos, C.] Nanyang Technol Univ, Div Phys & Appl Phys, Singapore 637371, Singapore. RP Popovic, D (reprint author), Florida State Univ, Natl High Magnet Field Lab, Tallahassee, FL 32310 USA. EM dragana@magnet.fsu.edu RI PANAGOPOULOS, CHRISTOS/G-8754-2011; Shi, Xiaoyan/L-4893-2015 OI Shi, Xiaoyan/0000-0002-9974-4637 FU NHMFL; State of Florida; US Department of Energy, Basic Energy Sciences, Materials Sciences and Engineering; EURYI [MEXT-CT-2006-039047]; National Research Foundation, Singapore; [NSF/DMR-0905843]; [NSF/DMR-0654118] FX We thank V. Dobrosavljevic for discussions. The work by X.S. and D.P. was supported by NSF/DMR-0905843 and the NHMFL, which is supported by NSF/DMR-0654118 and the State of Florida. I.B., G.L. and A.T.B. were supported by the US Department of Energy, Basic Energy Sciences, Materials Sciences and Engineering. C.P. was supported by EURYI, MEXT-CT-2006-039047 and the National Research Foundation, Singapore. NR 37 TC 17 Z9 17 U1 4 U2 108 PU NATURE PUBLISHING GROUP PI LONDON PA MACMILLAN BUILDING, 4 CRINAN ST, LONDON N1 9XW, ENGLAND SN 1476-1122 J9 NAT MATER JI Nat. Mater. PD JAN PY 2013 VL 12 IS 1 BP 47 EP 51 DI 10.1038/NMAT3487 PG 5 WC Chemistry, Physical; Materials Science, Multidisciplinary; Physics, Applied; Physics, Condensed Matter SC Chemistry; Materials Science; Physics GA 057WA UT WOS:000312593600019 PM 23160270 ER PT J AU Jailaubekov, AE Willard, AP Tritsch, JR Chan, WL Sai, N Gearba, R Kaake, LG Williams, KJ Leung, K Rossky, PJ Zhu, XY AF Jailaubekov, Askat E. Willard, Adam P. Tritsch, John R. Chan, Wai-Lun Sai, Na Gearba, Raluca Kaake, Loren G. Williams, Kenrick J. Leung, Kevin Rossky, Peter J. Zhu, X-Y. TI Hot charge-transfer excitons set the time limit for charge separation at donor/acceptor interfaces in organic photovoltaics SO NATURE MATERIALS LA English DT Article ID HETEROJUNCTION SOLAR-CELLS; OPEN-CIRCUIT VOLTAGE; TRANSIENT ABSORPTION; TRANSFER STATE; ENERGY; POLYMER; DISSOCIATION; GENERATION; BETAINE-30; DYNAMICS AB Photocurrent generation in organic photovoltaics (OPVs) relies on the dissociation of excitons into free electrons and holes at donor/acceptor heterointerfaces. The low dielectric constant of organic semiconductors leads to strong Coulomb interactions between electron-hole pairs that should in principle oppose the generation of free charges. The exact mechanism by which electrons and holes overcome this Coulomb trapping is still unsolved, but increasing evidence points to the critical role of hot charge-transfer (CT) excitons in assisting this process. Here we provide a real-time view of hot CT exciton formation and relaxation using femtosecond nonlinear optical spectroscopies and non-adiabatic mixed quantum mechanics/molecular mechanics simulations in the phthalocyanine-fullerene model OPV system. For initial excitation on phthalocyanine, hot CT excitons are formed in 10(-13) s, followed by relaxation to lower energies and shorter electron-hole distances on a 10(-12) s timescale. This hot CT exciton cooling process and collapse of charge separation sets the fundamental time limit for competitive charge separation channels that lead to efficient photocurrent generation. C1 [Leung, Kevin] Sandia Natl Labs, Albuquerque, NM 87185 USA. [Jailaubekov, Askat E.; Willard, Adam P.; Tritsch, John R.; Chan, Wai-Lun; Sai, Na; Gearba, Raluca; Kaake, Loren G.; Williams, Kenrick J.; Rossky, Peter J.; Zhu, X-Y.] Univ Texas Austin, Energy Frontier Res Ctr EFRC CST, Austin, TX 78712 USA. RP Zhu, XY (reprint author), Columbia Univ, Dept Chem, New York, NY 10027 USA. EM peter.rossky@austin.utexas.edu; xyzhu@columbia.edu RI Chan, Wai-Lun/A-7833-2008 OI Chan, Wai-Lun/0000-0001-8697-9894 FU Understanding Charge Separation and Transfer at Interfaces in Energy Materials (EFRC:CST), an Energy Frontier Research Center; US Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001091]; US Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX The results reported here were based on work 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. Sandia National Laboratories is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the US Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000. Computational resources were provided by TACC and NERSC. NR 45 TC 268 Z9 270 U1 28 U2 611 PU NATURE PUBLISHING GROUP PI LONDON PA MACMILLAN BUILDING, 4 CRINAN ST, LONDON N1 9XW, ENGLAND SN 1476-1122 EI 1476-4660 J9 NAT MATER JI Nat. Mater. PD JAN PY 2013 VL 12 IS 1 BP 66 EP 73 DI 10.1038/NMAT3500 PG 8 WC Chemistry, Physical; Materials Science, Multidisciplinary; Physics, Applied; Physics, Condensed Matter SC Chemistry; Materials Science; Physics GA 057WA UT WOS:000312593600022 PM 23223125 ER PT J AU Volkow, ND Wang, GJ Tomasi, D Baler, RD AF Volkow, N. D. Wang, G. -J. Tomasi, D. Baler, R. D. TI Obesity and addiction: neurobiological overlaps SO OBESITY REVIEWS LA English DT Review DE Addiction; dopamine; obesity; prefrontal cortex ID VENTRAL TEGMENTAL AREA; BODY-MASS INDEX; DOPAMINE D2 RECEPTORS; NUCLEUS-ACCUMBENS DOPAMINE; MESSENGER-RNA EXPRESSION; DIET-INDUCED OBESITY; HIGH-CALORIE FOODS; ORBITOFRONTAL CORTEX; PREFRONTAL CORTEX; CENTRAL AMYGDALA AB Drug addiction and obesity appear to share several properties. Both can be defined as disorders in which the saliency of a specific type of reward (food or drug) becomes exaggerated relative to, and at the expense of others rewards. Both drugs and food have powerful reinforcing effects, which are in part mediated by abrupt dopamine increases in the brain reward centres. The abrupt dopamine increases, in vulnerable individuals, can override the brain's homeostatic control mechanisms. These parallels have generated interest in understanding the shared vulnerabilities between addiction and obesity. Predictably, they also engendered a heated debate. Specifically, brain imaging studies are beginning to uncover common features between these two conditions and delineate some of the overlapping brain circuits whose dysfunctions may underlie the observed deficits. The combined results suggest that both obese and drug-addicted individuals suffer from impairments in dopaminergic pathways that regulate neuronal systems associated not only with reward sensitivity and incentive motivation, but also with conditioning, self-control, stress reactivity and interoceptive awareness. In parallel, studies are also delineating differences between them that centre on the key role that peripheral signals involved with homeostatic control exert on food intake. Here, we focus on the shared neurobiological substrates of obesity and addiction. C1 [Volkow, N. D.; Baler, R. D.] NIDA, NIH, Bethesda, MD 20892 USA. [Wang, G. -J.; Tomasi, D.] Brookhaven Natl Lab, Dept Med, Upton, NY 11973 USA. RP Volkow, ND (reprint author), NIDA, NIH, 6001 Execut Blvd,Room 5274, Bethesda, MD 20892 USA. EM nvokowl@nida.nih.gov RI Tomasi, Dardo/J-2127-2015 FU Intramural NIH HHS [ZIA AA000550-09] NR 225 TC 182 Z9 185 U1 10 U2 119 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 1467-7881 J9 OBES REV JI Obes. Rev. PD JAN PY 2013 VL 14 IS 1 BP 2 EP 18 DI 10.1111/j.1467-789X.2012.01031.x PG 17 WC Endocrinology & Metabolism SC Endocrinology & Metabolism GA 057FB UT WOS:000312546900002 PM 23016694 ER PT J AU Meier, D Lilienblum, M Becker, P Bohaty, L Spaldin, NA Ramesh, R Fiebig, M AF Meier, D. Lilienblum, M. Becker, P. Bohaty, L. Spaldin, N. A. Ramesh, R. Fiebig, M. TI Translation domains in multiferroics SO PHASE TRANSITIONS LA English DT Article DE multiferroics; domains; order parameter; antiferromagnetic; improper ferroelectric ID BILBAO CRYSTALLOGRAPHIC SERVER; 2ND-HARMONIC GENERATION; PHASE; CRYSTALS; WALLS; YMNO3; SYMMETRY; ORIGIN AB We describe the behavior of translation domains that is domains resulting from the breaking of translation rather than point symmetries in multiferroics with simultaneous magnetic and ferroelectric order. First, we review the structure of order parameters describing translation domains. Then, we report our spatially resolved measurements of translation domains using piezoresponse force microscopy and optical second harmonic generation in two types of multiferroics. In the split-order-parameter multiferroic hexagonal YMnO3, we show that commensurate structural translation domains are rigidly coupled to the ferroelectric orientation domains so that the orientation domains adopt the translation domain structure. In contrast, in the joint-order-parameter multiferroic MnWO4, incommensurate magnetic translation domains are largely decoupled from the ferroelectric orientation but nevertheless limited by stability criteria. These pronounced manifestations of the generally hidden translation domains emphasize that their presence should be taken into account when discussing the physical properties and functionalities of multiferroics. C1 [Lilienblum, M.; Spaldin, N. A.; Fiebig, M.] ETH, Dept Mat, CH-8093 Zurich, Switzerland. [Meier, D.; Ramesh, R.] Univ Calif Berkeley, Dept Phys, Berkeley, CA 94720 USA. [Meier, D.; Ramesh, R.] Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA. [Becker, P.; Bohaty, L.] Univ Cologne, Inst Kristallog, D-50939 Cologne, Germany. [Ramesh, R.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. RP Fiebig, M (reprint author), ETH, Dept Mat, Wolfgang Pauli Str 10, CH-8093 Zurich, Switzerland. EM manfred.fiebig@mat.ethz.ch RI Spaldin, Nicola/A-1017-2010 OI Spaldin, Nicola/0000-0003-0709-9499 FU IMI Program of the National Science Foundation [DMR-0843934]; Alexander von Humboldt Foundation; NSF Science and Technology Center (E3S); DFG [SFB 608] FX The authors thank Pierre Toledano and Morgan Trassin for many fruitful discussions and helpful comments. M.F. thanks the IMI Program of the National Science Foundation under Award No. DMR-0843934, managed by the International Center for Materials Research, UC Santa Barbara, for sabbatical support. D.M. acknowledges support by the Alexander von Humboldt Foundation and the NSF Science and Technology Center (E3S). M. F. and M. L. thank the SFB 608 of the DFG for financial support. NR 67 TC 10 Z9 10 U1 4 U2 122 PU TAYLOR & FRANCIS LTD PI ABINGDON PA 4 PARK SQUARE, MILTON PARK, ABINGDON OX14 4RN, OXON, ENGLAND SN 0141-1594 EI 1029-0338 J9 PHASE TRANSIT JI Phase Transit. PD JAN 1 PY 2013 VL 86 IS 1 SI SI BP 33 EP 52 DI 10.1080/01411594.2012.696116 PG 20 WC Crystallography; Physics, Condensed Matter SC Crystallography; Physics GA 057TK UT WOS:000312586700005 ER PT J AU Seidel, J Singh-Bhalla, G He, Q Yang, SY Chu, YH Ramesh, R AF Seidel, Jan Singh-Bhalla, Guneeta He, Qing Yang, Seung-Yeul Chu, Ying-Hao Ramesh, Ramamoorthy TI Domain wall functionality in BiFeO3 SO PHASE TRANSITIONS LA English DT Article DE ferroelectrics; domain walls; scanning probe methods; optics; photovoltaics; nanoscale characterization ID ROOM-TEMPERATURE; SINGLE-CRYSTALS; DOPED BIFEO3; CONDUCTION; PHYSICS; FILMS; FERROELECTRICS; MULTIFERROICS; POLARIZATION; MODULATION AB In this article we provide an overview of phenomena involving domain walls in BiFeO3 as nanoscale functional elements. Because ferroelectric domain walls can be routinely modified using electric fields, our results suggest a new degree of flexibility for domain boundary engineering and oxide-based nanoelectronics. C1 [Seidel, Jan; Singh-Bhalla, Guneeta; He, Qing; Ramesh, Ramamoorthy] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. [Seidel, Jan; Ramesh, Ramamoorthy] Univ Calif Berkeley, Dept Phys, Berkeley, CA 94720 USA. [Seidel, Jan] Univ New S Wales, Sch Mat Sci & Engn, Sydney, NSW, Australia. [Yang, Seung-Yeul; Ramesh, Ramamoorthy] Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA. [Chu, Ying-Hao] Natl Chiao Tung Univ, Hsinchu, Taiwan. RP Seidel, J (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. EM jan.seidel@unsw.edu.au RI Ying-Hao, Chu/A-4204-2008; He, Qing/E-3202-2010 OI Ying-Hao, Chu/0000-0002-3435-9084; FU Office of Science, Office of Basic Energy Sciences, Materials Sciences Division of the US Department of Energy [DE-AC02-05CH1123]; Alexander von Humboldt Foundation FX This work was supported by the Director, Office of Science, Office of Basic Energy Sciences, Materials Sciences Division of the US Department of Energy under contract No DE-AC02-05CH1123. J.S. acknowledges support from the Alexander von Humboldt Foundation. NR 61 TC 23 Z9 23 U1 3 U2 113 PU TAYLOR & FRANCIS LTD PI ABINGDON PA 4 PARK SQUARE, MILTON PARK, ABINGDON OX14 4RN, OXON, ENGLAND SN 0141-1594 J9 PHASE TRANSIT JI Phase Transit. PD JAN 1 PY 2013 VL 86 IS 1 SI SI BP 53 EP 66 DI 10.1080/01411594.2012.695371 PG 14 WC Crystallography; Physics, Condensed Matter SC Crystallography; Physics GA 057TK UT WOS:000312586700006 ER PT J AU Yakovlev, S Downing, KH AF Yakovlev, Sergey Downing, Kenneth H. TI Visualization of clusters in polymer electrolyte membranes by electron microscopy SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID X-RAY-SCATTERING; PERFLUORINATED IONOMER MEMBRANES; SULFONATED POLYSTYRENE IONOMERS; ENERGY-LOSS SPECTROSCOPY; SOFT MATERIALS; NAFION MEMBRANES; ACID) IONOMERS; FUEL-CELLS; MORPHOLOGY; ANGLE AB The morphology of ionic clusters that form in polyelectrolyte membranes has a strong effect on transport and electrical properties. In spite of considerable research effort the link between morphology and properties has not been clearly established, mainly due to difficulties in assessing nanoscale morphology. Electron microscopy (EM) has the potential to visualize morphology. However success in visualization has so far been moderate. In this review we focus on the potential of EM techniques to characterize the ionic domains. We use both experimental data and models to compare the capabilities of several EM techniques: BF TEM, HAADF, core-loss EELS, and low-loss EELS in projection imaging and STEM modes. The main problems common for all these EM modes are radiation damage and overlap of features in projection. Our models show that core loss EELS with exposures that are below the typical damage threshold is incapable of resolving 2 nm diameter sulfur-rich clusters in PEMs. While low loss EELS requires lower exposure, the insight it can provide is quite limited. HAADF and BF TEM present the most effective modes for imaging the sulfur clusters in PEMs. While BF TEM uses scattered electrons more efficiently, HAADF using slightly higher doses can provide unique information due to in-focus imaging and transparent interpretation of the images. Fortunately, in at least some interesting cases the clusters themselves are much more radiation resistant than the polymer and can be studied at exposures high enough to obtain clear images. Our simulations also show that tomographic 3D reconstruction provides the best approach for solving the overlap problem. In spite of the abilities of electron tomography, data obtained from all EM techniques improve if thin sections are studied. We briefly discuss methods for obtaining such sections. C1 [Downing, Kenneth H.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Life Sci, Berkeley, CA 94720 USA. [Yakovlev, Sergey] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. RP Downing, KH (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Life Sci, 1 Cyclotron Rd, Berkeley, CA 94720 USA. EM syakovlev@lbl.gov; khdowning@lbl.gov RI Foundry, Molecular/G-9968-2014 FU U.S. Department of Energy [DE-AC02-05CH11231]; Office of Basic Energy Sciences, Materials Sciences and Engineering Division; Office of Science, Office of Basic Energy Sciences of the U.S. Department of Energy [DE-AC02-05CH11231] FX Funding for this work was provided by the U.S. Department of Energy under Contract No. DE-AC02-05CH11231 through the Electron Microscopy of Soft Matter Program (electrolyte imaging) supported by the Office of Basic Energy Sciences, Materials Sciences and Engineering Division. Part of this work was performed at National Center for Electron Microscopy and the Molecular Foundry at Lawrence Berkeley National Lab, which 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. NR 58 TC 6 Z9 6 U1 3 U2 86 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2013 VL 15 IS 4 BP 1052 EP 1064 DI 10.1039/c2cp42969a PG 13 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 056BR UT WOS:000312462400001 PM 23165242 ER PT J AU Li, B Zhang, JM Kaspar, T Shutthanandan, V Ewing, RC Lian, J AF Li, Bin Zhang, Jiaming Kaspar, Tiffany Shutthanandan, Vaithiyalingam Ewing, Rodney C. Lian, Jie TI Multilayered YSZ/GZO films with greatly enhanced ionic conduction for low temperature solid oxide fuel cells SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID YTTRIA-STABILIZED ZIRCONIA; DOPED CERIA; ELECTROLYTES; FABRICATION; CHALLENGES; BATTERIES; TRANSPORT; SOFCS AB Strain confinement in heterostructured films significantly affects ionic conductivity of the electrolytes for solid oxide fuel cells based on a multi-layered design strategy. Nearly ideal tensile strain can be achieved by a dedicated manipulation of the lattice mismatch between adjacent layers and fine control of the layer thicknesses to minimize the formation of dislocations and thus to achieve optimized ionic conduction. This strategy was demonstrated by a model system of multilayered 8 mol%Y2O3 stabilized ZrO2 (YSZ) with Gd2Zr2O7 (GZO) films, which were epitaxially grown on Al2O3 (0001) substrates by pulsed laser deposition (PLD) with the {111} planes of YSZ/GZO along the Al2O3 [0 1 -1 0] direction. The tensile strain (3%) resulting from the lattice mismatch can be confined in individual YSZ layers with the formation of a coherent, dislocation-free interface upon the manipulation of the layer thickness below a critical value, e. g., down to 5 nm. The strained heterostructure displays a two order-of-magnitude increase in oxide-ion conductivity as compared with bulk YSZ, and a high ionic conductivity of 0.01 S cm(-1) at 475 degrees C can be achieved, five times greater than that of Gd-doped ceria/zirconia. The approach of strain confinement by fine control of lattice mismatch and layer thickness represents a promising strategy in developing advanced electrolytes enabling the miniaturization of solid-state ionic devices that can be operated at low temperatures below 500 degrees C. C1 [Li, Bin; Lian, Jie] Rensselaer Polytech Inst, Dept Mech Aerosp & Nucl Engn, Troy, NY 12180 USA. [Li, Bin] Pacific NW Natl Lab, Phys Sci Lab, Richland, WA 99352 USA. [Zhang, Jiaming; Ewing, Rodney C.] Univ Michigan, Dept Earth & Environm Sci, Ann Arbor, MI 48109 USA. [Zhang, Jiaming; Ewing, Rodney C.] Univ Michigan, Dept Mat Sci & Engn, Ann Arbor, MI 48109 USA. [Kaspar, Tiffany; Shutthanandan, Vaithiyalingam] Pacific NW Natl Lab, Environm Mol Sci Lab, Richland, WA 99352 USA. RP Lian, J (reprint author), Rensselaer Polytech Inst, Dept Mech Aerosp & Nucl Engn, Troy, NY 12180 USA. EM lianj@rpi.edu RI Albe, Karsten/F-1139-2011 FU NSF DMR Ceramic program under the award of DMR [0906349]; NSF career award of DMR [1151028] FX This work was financially supported by the NSF DMR Ceramic program under the award of DMR 0906349 and a NSF career award of DMR 1151028. The synthesis of multilayered heterostructured film by pulsed laser deposition was supported by user proposal 46398 at Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory. NR 33 TC 26 Z9 26 U1 3 U2 100 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2013 VL 15 IS 4 BP 1296 EP 1301 DI 10.1039/c2cp42964k PG 6 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 056BR UT WOS:000312462400029 PM 23232452 ER PT J AU Dewar, RL Hudson, SR Gibson, AM AF Dewar, R. L. Hudson, S. R. Gibson, A. M. TI Generalized action-angle coordinates defined on island chains SO PLASMA PHYSICS AND CONTROLLED FUSION LA English DT Article; Proceedings Paper CT 18th International Stellarator Hellotron Workshop and 10th Asia Pacific Plasma Theory Conference CY JAN 30-FEB 03, 2012 CL Australian Natl Univ, Canberra, AUSTRALIA SP Ampegon, Australian Inst Nucl Sci & Engn, Australian Nucl Sci & Technol Org, Int Atom Energy Agcy (IAEA) HO Australian Natl Univ ID MAGNETIC-SURFACES; FIELDS AB Straight-field-line coordinates are very useful for representing magnetic fields in toroidally confined plasmas, but fundamental problems arise regarding their definition in 3D geometries because of the formation of islands and chaotic field regions, i.e. non-integrability. In Hamiltonian dynamical systems terminology these coordinates are similar to action-angle variables, but these are normally defined only for integrable systems. In order to describe 3D magnetic field systems, a generalization of this concept was proposed recently by the present authors that unified the concepts of ghost surfaces and quadratic-flux-minimizing (QFMin) surfaces. This was based on a simple canonical transformation generated by a change of variable theta = theta(Theta, zeta), where theta and zeta are poloidal and toroidal angles, respectively, with Theta a new poloidal angle chosen to give pseudo-orbits that are (a) straight when plotted in the zeta, Theta plane and (b) QFMin pseudo-orbits in the transformed coordinate. These two requirements ensure that the pseudo-orbits are also (c) ghost pseudo-orbits. In this paper, it is demonstrated that these requirements do not uniquely specify the transformation owing to a relabelling symmetry. A variational method of solution that removes this lack of uniqueness is proposed. C1 [Dewar, R. L.; Hudson, S. R.; Gibson, A. M.] Australian Natl Univ, Res Sch Phys & Engn, Canberra, ACT 0200, Australia. [Dewar, R. L.; Hudson, S. R.; Gibson, A. M.] Princeton Plasma Phys Lab, Princeton, NJ 08543 USA. RP Dewar, RL (reprint author), Australian Natl Univ, Res Sch Phys & Engn, GPO Box 4, Canberra, ACT 0200, Australia. EM robert.dewar@anu.edu.au RI Hudson, Stuart/H-7186-2013; Dewar, Robert/B-1300-2008 OI Hudson, Stuart/0000-0003-1530-2733; Dewar, Robert/0000-0002-9518-7087 NR 15 TC 1 Z9 1 U1 1 U2 7 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 0741-3335 J9 PLASMA PHYS CONTR F JI Plasma Phys. Control. Fusion PD JAN PY 2013 VL 55 IS 1 AR 014004 DI 10.1088/0741-3335/55/1/014004 PG 5 WC Physics, Fluids & Plasmas SC Physics GA 057TD UT WOS:000312586000006 ER PT J AU Geiger, J Wolf, RC Beidler, C Cardella, A Chlechowitz, E Erckmann, V Gantenbein, G Hathiramani, D Hirsch, M Kasparek, W Kisslinger, J Konig, R Kornejew, P Laqua, HP Lechte, C Lore, J Lumsdaine, A Maassberg, H Marushchenko, NB Michel, G Otte, M Peacock, A Pedersen, TS Thumm, M Turkin, Y Werner, A Zhang, D AF Geiger, J. Wolf, R. C. Beidler, C. Cardella, A. Chlechowitz, E. Erckmann, V. Gantenbein, G. Hathiramani, D. Hirsch, M. Kasparek, W. Kisslinger, J. Koenig, R. Kornejew, P. Laqua, H. P. Lechte, C. Lore, J. Lumsdaine, A. Maassberg, H. Marushchenko, N. B. Michel, G. Otte, M. Peacock, A. Pedersen, T. Sunn Thumm, M. Turkin, Y. Werner, A. Zhang, D. CA W7-X Team TI Aspects of steady-state operation of the Wendelstein 7-X stellarator SO PLASMA PHYSICS AND CONTROLLED FUSION LA English DT Article; Proceedings Paper CT 18th International Stellarator Hellotron Workshop and 10th Asia Pacific Plasma Theory Conference CY JAN 30-FEB 03, 2012 CL Australian Natl Univ, Canberra, AUSTRALIA SP Ampegon, Australian Inst Nucl Sci & Engn, Australian Nucl Sci & Technol Org, Int Atom Energy Agcy (IAEA) HO Australian Natl Univ ID PHYSICS; W7-X; OPTIMIZATION AB The objective of Wendelstein 7-X is to demonstrate steady-state operation at beta-values of up to 5%, at ion temperatures of several keV and plasma densities of up to 2 x 10(20) m(-3). The second operational phase foresees a fully steady-state high heat flux (HHF) divertor. Preparations are underway to cope with residual bootstrap currents, either by electron cyclotron current drive or by HHF protection elements. The main steady-state heating system is an electron cyclotron resonance heating facility. Various technical improvements of the gyrotrons have been implemented recently. They enable a reliable operation at the 1 MW power level. Some of the technical issues preparing plasma diagnostics for steady-state operation are exemplified. This includes the protection against non-absorbed microwave radiation. C1 [Geiger, J.; Wolf, R. C.; Beidler, C.; Cardella, A.; Chlechowitz, E.; Erckmann, V.; Hathiramani, D.; Hirsch, M.; Kisslinger, J.; Koenig, R.; Kornejew, P.; Laqua, H. P.; Maassberg, H.; Marushchenko, N. B.; Michel, G.; Otte, M.; Peacock, A.; Pedersen, T. Sunn; Turkin, Y.; Werner, A.; Zhang, D.] Max Planck Inst Plasma Phys, EURATOM Assoc, D-8046 Garching, Germany. [Geiger, J.; Wolf, R. C.; Beidler, C.; Cardella, A.; Chlechowitz, E.; Erckmann, V.; Hathiramani, D.; Hirsch, M.; Kisslinger, J.; Koenig, R.; Kornejew, P.; Laqua, H. P.; Maassberg, H.; Marushchenko, N. B.; Michel, G.; Otte, M.; Peacock, A.; Pedersen, T. Sunn; Turkin, Y.; Werner, A.; Zhang, D.] Max Planck Inst Plasma Phys, EURATOM Assoc, Greifswald, Germany. [Gantenbein, G.; Thumm, M.] EURATOM, Karlsruhe Inst Technol, IHM, Karlsruhe, Germany. [Kasparek, W.; Lechte, C.] Univ Stuttgart, Inst Plasma Res, Stuttgart, Germany. [Lore, J.; Lumsdaine, A.] Oak Ridge Natl Lab, Oak Ridge, TN USA. RP Geiger, J (reprint author), Max Planck Inst Plasma Phys, EURATOM Assoc, Boltzmannstr 2, D-8046 Garching, Germany. EM robert.wolf@ipp.mpg.de OI Marushchenko, Nikolai/0000-0002-5110-9343; Lore, Jeremy/0000-0002-9192-465X NR 22 TC 9 Z9 9 U1 0 U2 15 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 0741-3335 J9 PLASMA PHYS CONTR F JI Plasma Phys. Control. Fusion PD JAN PY 2013 VL 55 IS 1 AR 014006 DI 10.1088/0741-3335/55/1/014006 PG 6 WC Physics, Fluids & Plasmas SC Physics GA 057TD UT WOS:000312586000008 ER PT J AU Gorelenkov, NN White, RB AF Gorelenkov, N. N. White, R. B. TI Perturbative study of energetic particle redistribution by Alfven eigenmodes in ITER SO PLASMA PHYSICS AND CONTROLLED FUSION LA English DT Article ID CODE AB The modification of particle distributions by magnetohydrodynamic modes is an important topic for magnetically confined plasmas. Low amplitude modes are known to be capable of producing significant modification of injected neutral beam profiles. Flattening of a distribution due to phase mixing in an island or due to portions of phase space becoming stochastic is a process extremely rapid on the time scale of equilibrium parameter changes in an experiment. In this paper, we examine the effect of toroidal Alfven eigenmodes (TAE) and reversed shear Alfven eigenmodes (RSAE) in ITER on alpha particle and injected beam distributions using theoretically predicted mode amplitudes using perturbative linear theory. It is found that for the equilibrium of a hybrid scenario even at ten times the predicted saturation level the modes have negligible effect on these distributions. A strongly reversed shear (or advanced) scenario, having a spectrum of modes that are much more global, is somewhat more susceptible to induced loss due to mode resonance, with alpha particle losses of over 1% with predicted amplitudes and somewhat larger with the assistance of toroidal field ripple. The elevated q profile contributes to stronger TAE (RSAE) drive and more unstable modes. An analysis of the existing mode-particle resonances is carried out to determine which modes are responsible for the profile modification and induced loss. We find that losses are entirely due to resonance with the counter-moving and trapped particle populations, with co-moving passing particles participating in resonances only deep within the plasma core and not leading to loss. C1 [Gorelenkov, N. N.; White, R. B.] Princeton Univ, Plasma Phys Lab, Princeton, NJ 08543 USA. RP Gorelenkov, NN (reprint author), Princeton Univ, Plasma Phys Lab, POB 451, Princeton, NJ 08543 USA. RI White, Roscoe/D-1773-2013 OI White, Roscoe/0000-0002-4239-2685 NR 21 TC 6 Z9 6 U1 0 U2 6 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 0741-3335 EI 1361-6587 J9 PLASMA PHYS CONTR F JI Plasma Phys. Control. Fusion PD JAN PY 2013 VL 55 IS 1 AR 015007 DI 10.1088/0741-3335/55/1/015007 PG 9 WC Physics, Fluids & Plasmas SC Physics GA 057TD UT WOS:000312586000027 ER PT J AU Hole, MJ Blackwell, BD Zarnstorff, M AF Hole, M. J. Blackwell, B. D. Zarnstorff, M. TI Selected papers from the Joint 18th International Stellarator Heliotron Workshop and the 10th Asia Pacific Plasma Theory Conference SO PLASMA PHYSICS AND CONTROLLED FUSION LA English DT Editorial Material C1 [Hole, M. J.; Blackwell, B. D.] Australian Natl Univ, Canberra, ACT 0200, Australia. [Zarnstorff, M.] Princeton Plasma Phys Lab, Princeton, NJ USA. RP Hole, MJ (reprint author), Australian Natl Univ, Canberra, ACT 0200, Australia. RI Blackwell, Boyd/M-2717-2015 OI Blackwell, Boyd/0000-0002-9091-9269 NR 0 TC 0 Z9 0 U1 1 U2 2 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 0741-3335 J9 PLASMA PHYS CONTR F JI Plasma Phys. Control. Fusion PD JAN PY 2013 VL 55 IS 1 AR 010201 DI 10.1088/0741-3335/55/1/010201 PG 1 WC Physics, Fluids & Plasmas SC Physics GA 057TD UT WOS:000312586000001 ER PT J AU Bhat, KS Birdsell, SA Hamada, MS AF Bhat, K. Sham Birdsell, Stephen A. Hamada, Michael S. TI The Interplay Between Science and Statistics in Modeling Stress-Strain Curve Data SO QUALITY ENGINEERING LA English DT Article DE Bayesian analysis; exploratory data analysis; prediction AB Data obtained from an archived 9-year aging study on S5370 foam were used to develop a stressstrain aging model using a strategy that first fits separate stressstrain curve data based on a form from polymer science. Then, exploratory data analysis of the model coefficients from these separate fits was used to develop a full model. This article illustrates this strategy and demonstrates how the full model can be fit and subsequent predictions can be made. C1 [Bhat, K. Sham; Hamada, Michael S.] Los Alamos Natl Lab, Comp Computat & Stat Sci Div, Stat Sci Grp, Los Alamos, NM 87545 USA. [Birdsell, Stephen A.] Los Alamos Natl Lab, Mat Sci & Technol Div, Polymers & Coatings Grp, Los Alamos, NM 87545 USA. RP Hamada, MS (reprint author), Los Alamos Natl Lab, Comp Computat & Stat Sci Div, Stat Sci Grp, MS F600, Los Alamos, NM 87545 USA. EM hamada@lanl.gov FU National Nuclear Security Administration through the Enhanced Surveillance Campaign at Los Alamos National Laboratory FX We thank C. C. Essix for her support and encouragement of this work. This work was funded by the National Nuclear Security Administration through the Enhanced Surveillance Campaign at Los Alamos National Laboratory. We thank an anonymous referee for helpful comments that improved the exposition of this article. NR 7 TC 1 Z9 1 U1 1 U2 2 PU TAYLOR & FRANCIS INC PI PHILADELPHIA PA 325 CHESTNUT ST, SUITE 800, PHILADELPHIA, PA 19106 USA SN 0898-2112 J9 QUAL ENG JI Qual. Eng. PY 2013 VL 25 IS 1 BP 11 EP 22 DI 10.1080/08982112.2012.725494 PG 12 WC Engineering, Industrial; Statistics & Probability SC Engineering; Mathematics GA 055YM UT WOS:000312454000003 ER PT J AU Snee, RD Piepel, GF AF Snee, Ronald D. Piepel, Greg F. TI Assessing Component Effects in Formulation Systems SO QUALITY ENGINEERING LA English DT Article DE component effects; component effect directions; formulation systems; mixture experiment models; mixture experiments; Scheffe linear mixture model ID MIXTURES AB The purpose of Snee () was to discuss and illustrate how using Six Sigma concepts and approaches can lead to a better understanding of formulation systems. Central to the recommended approach is estimating and interpreting the effects of the components in the formulation on the response variable. Knowledge of components that have no effect, small or large effects (positive or negative), and similar effects is very helpful in understanding how the formulation system works. This understanding helps one decide (1) which components having large effects should be increased or decreased and (2) what to do about components with no effects or similar effects. Correspondence between the authors following Snee (), along with further review of the literature, has pointed out that the approaches discussed in Snee (), and the interpretation of component effects in general, need further clarification. That is the focus of this article. C1 [Snee, Ronald D.] Snee Associates LLC, Newark, DE 19711 USA. [Piepel, Greg F.] Pacific NW Natl Lab, Appl Stat & Computat Modeling Grp, Richland, WA 99352 USA. RP Snee, RD (reprint author), Snee Associates LLC, 10 Creek Crossing, Newark, DE 19711 USA. EM Ron@SneeAssociates.com NR 11 TC 1 Z9 1 U1 0 U2 3 PU TAYLOR & FRANCIS INC PI PHILADELPHIA PA 325 CHESTNUT ST, SUITE 800, PHILADELPHIA, PA 19106 USA SN 0898-2112 J9 QUAL ENG JI Qual. Eng. PY 2013 VL 25 IS 1 BP 46 EP 53 DI 10.1080/08982112.2012.731628 PG 8 WC Engineering, Industrial; Statistics & Probability SC Engineering; Mathematics GA 055YM UT WOS:000312454000006 ER PT J AU Cooper, CA Cooley, LD AF Cooper, C. A. Cooley, L. D. TI Mirror-smooth surfaces and repair of defects in superconducting RF cavities by mechanical polishing SO SUPERCONDUCTOR SCIENCE & TECHNOLOGY LA English DT Article ID NIOBIUM; DEPOSITION AB Mechanical techniques for polishing the inside surface of niobium superconducting radio-frequency (SRF) cavities have been systematically explored. By extending known techniques to fine polishing, mirror-like finishes were produced, with <15 nm RMS (root mean square) roughness over 1 mm(2) scan area. This is an order of magnitude less than the typical roughness produced by the electropolishing of niobium cavities. The extended mechanical polishing (XMP) process was applied to several SRF cavities which exhibited equator defects that caused quench at <20 MV m(-1) and were not improved by further electropolishing. Cavity optical inspection equipment verified the complete removal of these defects, and minor acid processing, which dulled the mirror finish, restored performance of the defective cells to the high gradients and quality factors measured for adjacent cells when tested with other harmonics. This innate repair feature of XMP could be used to increase manufacturing yield. Excellent superconducting properties resulted after initial process optimization, with quality factor Q of 3 x 10(10) and accelerating gradient of 43 MV m(-1) being attained for a single-cell TESLA cavity, which are both close to practical limits. Several repaired nine-cell cavities also attained Q > 8 x 10(9) at 35 MV m(-1), which is the specification for the International Linear Collider. Future optimization of the process and pathways for eliminating requirements for acid processing are also discussed. C1 [Cooper, C. A.; Cooley, L. D.] Fermilab Natl Accelerator Lab, Batavia, IL 60510 USA. RP Cooper, CA (reprint author), Fermilab Natl Accelerator Lab, POB 500, Batavia, IL 60510 USA. EM ccooper@fnal.gov RI Cooley, Lance/E-7377-2015 OI Cooley, Lance/0000-0003-3488-2980 FU Fermi Research Alliance, LLC [DE-AC02-07CH11359]; United States Department of Energy FX This work was performed in accordance with Fermi Research Alliance, LLC under Contract No. DE-AC02-07CH11359 with the United States Department of Energy. The authors thank D Burk, G Steuer, C Thompson, D Sergatskov, E Toropov, M Champion, C Ginsburg, and J Ozelis for technical assistance, characterization assistance, and testing. Reidar Hahn of Fermilab took the photograph seen in figure 4(b). We also express our thanks to numerous colleagues in the ILC Americas Regional Team and the TESLA Technology Collaboration for motivation and guidance. NR 36 TC 3 Z9 3 U1 2 U2 13 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 0953-2048 J9 SUPERCOND SCI TECH JI Supercond. Sci. Technol. PD JAN PY 2013 VL 26 IS 1 AR 015011 DI 10.1088/0953-2048/26/1/015011 PG 9 WC Physics, Applied; Physics, Condensed Matter SC Physics GA 053EJ UT WOS:000312253200012 ER PT J AU Solovyov, V Dimitrov, IK Li, Q AF Solovyov, Vyacheslav Dimitrov, Ivo K. Li, Qiang TI Growth of thick YBa2Cu3O7 layers via a barium fluoride process SO SUPERCONDUCTOR SCIENCE & TECHNOLOGY LA English DT Review ID CRITICAL-CURRENT DENSITY; YBCO COATED CONDUCTORS; EX-SITU CONVERSION; TFA-MOD PROCESS; POSTDEPOSITION REACTION PROCESS; ELECTRON-BEAM EVAPORATION; 2ND-GENERATION HTS WIRES; RESEARCH-AND-DEVELOPMENT; HIGH CRITICAL CURRENTS; PRECURSOR FILMS AB The ex situ process has emerged as a popular technology for growing epitaxial YBa2Cu3O7 (YBCO) for the second generation of coated conductors. The process combines low cost, ease of scale-up, the possibility of achieving high critical currents in relatively thick YBCO layers, as well as high tolerances to substrate misalignment. All of these factors explain why the process is increasingly becoming adapted by manufacturing companies for the production of YBCO wires. Studies of the barium fluoride variant of the ex situ process have offered rare insights into the structure, chemistry and pinning in ultra-thick, 5 mu m, ex situ YBCO layers. The transition to thick YBCO layers is viewed as one of the key ingredients of the commercial success of the YBCO wire technology, which makes these studies especially relevant. This review is intended to be a comprehensive introduction into the history, physics and chemistry of barium fluoride processing, discussed concomitantly with recent results and trends in this field. Furthermore, comparisons are made between YBCO films made by ex situ and in situ deposition processes. C1 [Solovyov, Vyacheslav; Dimitrov, Ivo K.; Li, Qiang] Brookhaven Natl Lab, Condensed Matter Phys & Mat Sci Dept, Upton, NY 11973 USA. RP Solovyov, V (reprint author), Brookhaven Natl Lab, Condensed Matter Phys & Mat Sci Dept, 76 Cornell Ave, Upton, NY 11973 USA. EM solov@bnl.gov OI Solovyov, Vyacheslav/0000-0003-1879-9802 FU Brookhaven Science Associates, LLC [DE-AC02-98CH10886]; New York State Energy Research and Development Authority (NYSERDA) [NF-10-21]; US Department of Energy, Office of Basic Energy Science, Materials Sciences and Engineering Division FX This manuscript has been authored by Brookhaven Science Associates, LLC under Contract No. DE-AC02-98CH10886 with the US Department of Energy. The work at Brookhaven National Laboratory was supported by New York State Energy Research and Development Authority (NYSERDA) under agreement NF-10-21 (VFS) and the US Department of Energy, Office of Basic Energy Science, Materials Sciences and Engineering Division (IKD and QL). The authors wish to thank Ron Feenstra for valuable comments and corrections. NR 149 TC 16 Z9 18 U1 5 U2 76 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 0953-2048 J9 SUPERCOND SCI TECH JI Supercond. Sci. Technol. PD JAN PY 2013 VL 26 IS 1 AR 013001 DI 10.1088/0953-2048/26/1/013001 PG 19 WC Physics, Applied; Physics, Condensed Matter SC Physics GA 053EJ UT WOS:000312253200001 ER PT J AU Srinivasan, G Lipnikov, K AF Srinivasan, G. Lipnikov, K. TI On the Reconstruction of Darcy Velocity in Finite-Volume Methods SO TRANSPORT IN POROUS MEDIA LA English DT Article DE Mimetic finite differences; Streamlines; Velocity reconstruction; Finite volume ID POLYHEDRAL MESHES; DIFFUSION-PROBLEMS; ELEMENT-METHOD; TRANSPORT; GRIDS; STREAMLINES; MECHANISMS AB The accuracy of particle tracking methods for advective transport in porous media depends in turn upon the accuracy of the computed velocity. In many advanced finite-volume methods used in practical applications, the velocity field is often only accurate up to the first order, and is typically defined only on mesh edges. We develop an inexpensive method for reconstructing a quasi-optimal accuracy-preserving velocity field inside the elements of a polygonal mesh. Numerical verification on quadrilateral meshes shows reduction of L (2)-error in comparison with conventional reconstruction strategies. C1 [Srinivasan, G.; Lipnikov, K.] Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. RP Srinivasan, G (reprint author), Los Alamos Natl Lab, Div Theoret, POB 1663, Los Alamos, NM 87545 USA. EM gowri@lanl.gov FU Los Alamos National Laboratory; DOE Office of Science Advanced Scientific Computing Research (ASCR) program in Applied Mathematical Sciences FX This research was performed under the auspices of the Los Alamos National Laboratory and supported by the DOE Office of Science Advanced Scientific Computing Research (ASCR) program in Applied Mathematical Sciences. NR 22 TC 1 Z9 1 U1 1 U2 4 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 0169-3913 J9 TRANSPORT POROUS MED JI Transp. Porous Media PD JAN PY 2013 VL 96 IS 2 BP 337 EP 351 DI 10.1007/s11242-012-0091-0 PG 15 WC Engineering, Chemical SC Engineering GA 058KY UT WOS:000312633800008 ER PT J AU Dawson, KS Schlegel, DJ Ahn, CP Anderson, SF Aubourg, E Bailey, S Barkhouser, RH Bautista, JE Beifiori, A Berlind, AA Bhardwaj, V Bizyaev, D Blake, CH Blanton, MR Blomqvist, M Bolton, AS Borde, A Bovy, J Brandt, WN Brewington, H Brinkmann, J Brown, PJ Brownstein, JR Bundy, K Busca, NG Carithers, W Carnero, AR Carr, MA Chen, YM Comparat, J Connolly, N Cope, F Croft, RAC Cuesta, AJ da Costa, LN Davenport, JRA Delubac, T de Putter, R Dhital, S Ealet, A Ebelke, GL Eisenstein, DJ Escoffier, S Fan, XH Ak, NF Finley, H Font-Ribera, A Genova-Santos, R Gunn, JE Guo, H Haggard, D Hall, PB Hamilton, JC Harris, B Harris, DW Ho, S Hogg, DW Holder, D Honscheid, K Huehnerhoff, J Jordan, B Jordan, WP Kauffmann, G Kazin, EA Kirkby, D Klaene, MA Kneib, JP Le Goff, JM Lee, KG Long, DC Loomis, CP Lundgren, B Lupton, RH Maia, MAG Makler, M Malanushenko, E Malanushenko, V Mandelbaum, R Manera, M Maraston, C Margala, D Masters, KL McBride, CK McDonald, P McGreer, ID McMahon, RG Mena, O Miralda-Escude, J Montero-Dorta, AD Montesano, F Muna, D Myers, AD Naugle, T Nichol, RC Noterdaeme, P Nuza, SE Olmstead, MD Oravetz, A Oravetz, DJ Owen, R Padmanabhan, N Palanque-Delabrouille, N Pan, K Parejko, JK Paris, I Percival, WJ Perez-Fournon, I Perez-Rafols, I Petitjean, P Pfaffenberger, R Pforr, J Pieri, MM Prada, F Price-Whelan, AM Raddick, MJ Rebolo, R Rich, J Richards, GT Rockosi, CM Roe, NA Ross, AJ Ross, NP Rossi, G Rubino-Martin, JA Samushia, L Sanchez, AG Sayres, C Schmidt, SJ Schneider, DP Scoccola, CG Seo, HJ Shelden, A Sheldon, E Shen, Y Shu, YP Slosar, A Smee, SA Snedden, SA Stauffer, F Steele, O Strauss, MA Streblyanska, A Suzuki, N Swanson, MEC Tal, T Tanaka, M Thomas, D Tinker, JL Tojeiro, R Tremonti, CA Magana, MV Verde, L Viel, M Wake, DA Watson, M Weaver, BA Weinberg, DH Weiner, BJ West, AA White, M Wood-Vasey, WM Yeche, C Zehavi, I Zhao, GB Zheng, Z AF Dawson, Kyle S. Schlegel, David J. Ahn, Christopher P. Anderson, Scott F. Aubourg, Eric Bailey, Stephen Barkhouser, Robert H. Bautista, Julian E. Beifiori, Alessandra Berlind, Andreas A. Bhardwaj, Vaishali Bizyaev, Dmitry Blake, Cullen H. Blanton, Michael R. Blomqvist, Michael Bolton, Adam S. Borde, Arnaud Bovy, Jo Brandt, W. N. Brewington, Howard Brinkmann, Jon Brown, Peter J. Brownstein, Joel R. Bundy, Kevin Busca, N. G. Carithers, William Carnero, Aurelio R. Carr, Michael A. Chen, Yanmei Comparat, Johan Connolly, Natalia Cope, Frances Croft, Rupert A. C. Cuesta, Antonio J. da Costa, Luiz N. Davenport, James R. A. Delubac, Timothee de Putter, Roland Dhital, Saurav Ealet, Anne Ebelke, Garrett L. Eisenstein, Daniel J. Escoffier, S. Fan, Xiaohui Ak, N. Filiz Finley, Hayley Font-Ribera, Andreu Genova-Santos, R. Gunn, James E. Guo, Hong Haggard, Daryl Hall, Patrick B. Hamilton, Jean-Christophe Harris, Ben Harris, David W. Ho, Shirley Hogg, David W. Holder, Diana Honscheid, Klaus Huehnerhoff, Joe Jordan, Beatrice Jordan, Wendell P. Kauffmann, Guinevere Kazin, Eyal A. Kirkby, David Klaene, Mark A. Kneib, Jean-Paul Le Goff, Jean-Marc Lee, Khee-Gan Long, Daniel C. Loomis, Craig P. Lundgren, Britt Lupton, Robert H. Maia, Marcio A. G. Makler, Martin Malanushenko, Elena Malanushenko, Viktor Mandelbaum, Rachel Manera, Marc Maraston, Claudia Margala, Daniel Masters, Karen L. McBride, Cameron K. McDonald, Patrick McGreer, Ian D. McMahon, Richard G. Mena, Olga Miralda-Escude, Jordi Montero-Dorta, Antonio D. Montesano, Francesco Muna, Demitri Myers, Adam D. Naugle, Tracy Nichol, Robert C. Noterdaeme, Pasquier Nuza, Sebastian E. Olmstead, Matthew D. Oravetz, Audrey Oravetz, Daniel J. Owen, Russell Padmanabhan, Nikhil Palanque-Delabrouille, Nathalie Pan, Kaike Parejko, John K. Paris, Isabelle Percival, Will J. Perez-Fournon, Ismael Perez-Rafols, Ignasi Petitjean, Patrick Pfaffenberger, Robert Pforr, Janine Pieri, Matthew M. Prada, Francisco Price-Whelan, Adrian M. Raddick, M. Jordan Rebolo, Rafael Rich, James Richards, Gordon T. Rockosi, Constance M. Roe, Natalie A. Ross, Ashley J. Ross, Nicholas P. Rossi, Graziano Rubino-Martin, J. A. Samushia, Lado Sanchez, Ariel G. Sayres, Conor Schmidt, Sarah J. Schneider, Donald P. Scoccola, C. G. Seo, Hee-Jong Shelden, Alaina Sheldon, Erin Shen, Yue Shu, Yiping Slosar, Anze Smee, Stephen A. Snedden, Stephanie A. Stauffer, Fritz Steele, Oliver Strauss, Michael A. Streblyanska, Alina Suzuki, Nao Swanson, Molly E. C. Tal, Tomer Tanaka, Masayuki Thomas, Daniel Tinker, Jeremy L. Tojeiro, Rita Tremonti, Christy A. Magana, M. Vargas Verde, Licia Viel, Matteo Wake, David A. Watson, Mike Weaver, Benjamin A. Weinberg, David H. Weiner, Benjamin J. West, Andrew A. White, Martin Wood-Vasey, W. M. Yeche, Christophe Zehavi, Idit Zhao, Gong-Bo Zheng, Zheng TI THE BARYON OSCILLATION SPECTROSCOPIC SURVEY OF SDSS-III SO ASTRONOMICAL JOURNAL LA English DT Article DE cosmology: observations; surveys ID DIGITAL-SKY-SURVEY; LY-ALPHA FOREST; BROAD-ABSORPTION-LINE; LUMINOUS RED GALAXIES; ACTIVE GALACTIC NUCLEI; LARGE-AREA TELESCOPE; PRINCIPAL COMPONENT ANALYSIS; QUASAR TARGET SELECTION; HIGH-REDSHIFT QUASARS; PROBING DARK ENERGY AB The Baryon Oscillation Spectroscopic Survey (BOSS) is designed to measure the scale of baryon acoustic oscillations (BAO) in the clustering of matter over a larger volume than the combined efforts of all previous spectroscopic surveys of large-scale structure. BOSS uses 1.5 million luminous galaxies as faint as i = 19.9 over 10,000 deg(2) to measure BAO to redshifts z < 0.7. Observations of neutral hydrogen in the Ly alpha forest in more than 150,000 quasar spectra (g < 22) will constrain BAO over the redshift range 2.15 < z < 3.5. Early results from BOSS include the first detection of the large-scale three-dimensional clustering of the Ly alpha forest and a strong detection from the Data Release 9 data set of the BAO in the clustering of massive galaxies at an effective redshift z = 0.57. We project that BOSS will yield measurements of the angular diameter distance d(A) to an accuracy of 1.0% at redshifts z = 0.3 and z = 0.57 and measurements of H(z) to 1.8% and 1.7% at the same redshifts. Forecasts for Ly alpha forest constraints predict a measurement of an overall dilation factor that scales the highly degenerate D-A(z) and H-1(z) parameters to an accuracy of 1.9% at z similar to 2.5 when the survey is complete. Here, we provide an overview of the selection of spectroscopic targets, planning of observations, and analysis of data and data quality of BOSS. C1 [Dawson, Kyle S.; Ahn, Christopher P.; Bolton, Adam S.; Brown, Peter J.; Brownstein, Joel R.; Harris, David W.; Montero-Dorta, Antonio D.; Olmstead, Matthew D.; Shu, Yiping; Zheng, Zheng] Univ Utah, Dept Phys & Astron, Salt Lake City, UT 84112 USA. [Schlegel, David J.; Bailey, Stephen; Carithers, William; Font-Ribera, Andreu; Ho, Shirley; McDonald, Patrick; Roe, Natalie A.; Ross, Nicholas P.; Suzuki, Nao; White, Martin] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Anderson, Scott F.; Bhardwaj, Vaishali; Davenport, James R. A.; Owen, Russell; Sayres, Conor; Schmidt, Sarah J.] Univ Washington, Dept Astron, Seattle, WA 98195 USA. [Aubourg, Eric; Bautista, Julian E.; Busca, N. G.; Hamilton, Jean-Christophe; Magana, M. Vargas] Univ Paris Diderot, APC, CNRS, IN2P3,IRFU,CEA,Observ Paris,Sorbonne Paris Cite, Paris, France. [Barkhouser, Robert H.; Smee, Stephen A.] Johns Hopkins Univ, Dept Phys & Astron, Baltimore, MD 21218 USA. [Beifiori, Alessandra; Montesano, Francesco; Sanchez, Ariel G.] Max Planck Inst Extraterr Phys, D-85748 Garching, Germany. [Berlind, Andreas A.; Dhital, Saurav] Vanderbilt Univ, Dept Phys & Astron, Nashville, TN 37235 USA. [Bizyaev, Dmitry; Brewington, Howard; Brinkmann, Jon; Cope, Frances; Ebelke, Garrett L.; Harris, Ben; Holder, Diana; Huehnerhoff, Joe; Jordan, Beatrice; Jordan, Wendell P.; Klaene, Mark A.; Long, Daniel C.; Malanushenko, Elena; Malanushenko, Viktor; Naugle, Tracy; Oravetz, Audrey; Oravetz, Daniel J.; Pan, Kaike; Pfaffenberger, Robert; Shelden, Alaina; Snedden, Stephanie A.; Stauffer, Fritz] Apache Point Observ, Sunspot, NM 88349 USA. [Blake, Cullen H.; Carr, Michael A.; Gunn, James E.; Loomis, Craig P.; Lupton, Robert H.; Mandelbaum, Rachel; Strauss, Michael A.] Princeton Univ, Dept Astrophys Sci, Princeton, NJ 08544 USA. [Blanton, Michael R.; Hogg, David W.; Muna, Demitri; Tinker, Jeremy L.; Weaver, Benjamin A.] NYU, Dept Phys, Ctr Cosmol & Particle Phys, New York, NY 10003 USA. [Blomqvist, Michael; Kirkby, David; Margala, Daniel] Univ Calif Irvine, Dept Phys & Astron, Irvine, CA 92697 USA. [Borde, Arnaud; Delubac, Timothee; Le Goff, Jean-Marc; Palanque-Delabrouille, Nathalie; Rich, James; Yeche, Christophe] CEA, Ctr Saclay, Irfu SPP, F-91191 Gif Sur Yvette, France. [Bovy, Jo] Inst Adv Study, Princeton, NJ 08540 USA. [Brandt, W. N.; Ak, N. Filiz; Schneider, Donald P.] Penn State Univ, Dept Astron & Astrophys, Davey Lab 525, University Pk, PA 16802 USA. [Brandt, W. N.; Ak, N. Filiz; Schneider, Donald P.] Penn State Univ, Inst Gravitat & Cosmos, University Pk, PA 16802 USA. [Brown, Peter J.] Texas A&M Univ, Dept Phys & Astron, George P & Cynthia Woods Mitchell Inst Fundamenta, College Stn, TX 77843 USA. [Bundy, Kevin; Tanaka, Masayuki] Univ Tokyo, Kavli Inst Phys & Math Universe, Todai Inst Adv Study, Kashiwa, Chiba 2778583, Japan. [Carnero, Aurelio R.; da Costa, Luiz N.; Maia, Marcio A. G.] Observ Nacl, BR-20921400 Rio De Janeiro, RJ, Brazil. [Carnero, Aurelio R.; da Costa, Luiz N.; Maia, Marcio A. G.; Makler, Martin] LIneA, BR-20921400 Rio De Janeiro, RJ, Brazil. [Chen, Yanmei] Nanjing Univ, Dept Astron, Nanjing 210093, Jiangsu, Peoples R China. [Chen, Yanmei] Nanjing Univ, Minist Educ, Key Lab Modern Astron & Astrophys, Nanjing 210093, Jiangsu, Peoples R China. [Comparat, Johan; Kneib, Jean-Paul] Aix Marseille Univ, CNRS, LAM, UMR 7326, F-13388 Marseille, France. [Connolly, Natalia] Hamilton Coll, Dept Phys, Clinton, NY 13323 USA. [Croft, Rupert A. C.; Ho, Shirley; Mandelbaum, Rachel] Carnegie Mellon Univ, Dept Phys, Bruce & Astrid McWilliams Ctr Cosmol, Pittsburgh, PA 15213 USA. [Cuesta, Antonio J.; Lundgren, Britt; Padmanabhan, Nikhil; Parejko, John K.] Yale Univ, Yale Ctr Astron & Astrophys, New Haven, CT 06520 USA. [de Putter, Roland; Miralda-Escude, Jordi; Perez-Rafols, Ignasi; Verde, Licia] Univ Barcelona, IEEC, Inst Ciencies Cosmos, E-08028 Barcelona, Spain. [de Putter, Roland; Mena, Olga] Univ Valencia, CSIC, Inst Fis Corpuscular, E-46971 Valencia, Spain. [Dhital, Saurav; West, Andrew A.] Boston Univ, Dept Astron, Boston, MA 02215 USA. [Ealet, Anne; Escoffier, S.] Aix Marseille Univ, CNRS, IN2P3, Ctr Phys Particules Marseille, F-13288 Marseille, France. [Eisenstein, Daniel J.; McBride, Cameron K.; Shen, Yue; Swanson, Molly E. C.] Harvard Univ, Harvard Smithsonian Ctr Astrophys, Cambridge, MA 02138 USA. [Fan, Xiaohui; McGreer, Ian D.; Weiner, Benjamin J.] Univ Arizona, Steward Observ, Tucson, AZ 85721 USA. [Finley, Hayley; Noterdaeme, Pasquier; Paris, Isabelle; Petitjean, Patrick] Inst Astrophys Paris, UPMC CNRS, UMR7095, F-75014 Paris, France. [Font-Ribera, Andreu] Univ Zurich, Inst Theoret Phys, CH-8057 Zurich, Switzerland. [Genova-Santos, R.; Perez-Fournon, Ismael; Rebolo, Rafael; Rubino-Martin, J. A.; Scoccola, C. G.; Streblyanska, Alina] Inst Astrofis Canarias, E-38200 San Cristobal la Laguna, Tenerife, Spain. [Genova-Santos, R.; Perez-Fournon, Ismael; Rubino-Martin, J. A.; Scoccola, C. G.; Streblyanska, Alina] Univ La Laguna, Dpto Astrofis, E-38206 Tenerife, Spain. [Guo, Hong; Zehavi, Idit] Case Western Reserve Univ, Dept Astron, Cleveland, OH 44106 USA. [Haggard, Daryl] Northwestern Univ, Dept Phys & Astron, Ctr Interdisciplinary Explorat & Res Astrophys, Evanston, IL 60208 USA. [Hall, Patrick B.] York Univ, Dept Phys & Astron, Toronto, ON M3J 1P3, Canada. [Honscheid, Klaus] Ohio State Univ, Dept Phys, Columbus, OH 43210 USA. [Honscheid, Klaus; Weinberg, David H.] Ohio State Univ, Ctr Cosmol & Astroparticle Phys, Columbus, OH 43210 USA. [Kauffmann, Guinevere] Max Planck Inst Astrophys, D-85748 Garching, Germany. [Kazin, Eyal A.] Swinburne Univ Technol, Ctr Astrophys & Supercomp, Hawthorn, Vic 3122, Australia. [Lee, Khee-Gan] Max Planck Inst Astron, D-69117 Heidelberg, Germany. [Makler, Martin] ICRA Ctr Brasileiro Pesquisas Fis, BR-22290180 Rio De Janeiro, RJ, Brazil. [Manera, Marc; Maraston, Claudia; Masters, Karen L.; Nichol, Robert C.; Percival, Will J.; Pforr, Janine; Pieri, Matthew M.; Ross, Ashley J.; Samushia, Lado; Steele, Oliver; Thomas, Daniel; Tojeiro, Rita; Zhao, Gong-Bo] Univ Portsmouth, Inst Cosmol & Gravitat, Portsmouth PO1 3FX, Hants, England. [McMahon, Richard G.] Univ Cambridge, Inst Astron, Cambridge CB3 0HA, England. [McMahon, Richard G.] Univ Cambridge, Kavli Inst Cosmol, Cambridge CB3 0HA, England. [Miralda-Escude, Jordi; Verde, Licia] Inst Catalana Recerca & Estudis Avancats, E-08010 Barcelona, Spain. [Montero-Dorta, Antonio D.; Prada, Francisco] Inst Astrofis Andalucia CSIC, E-18080 Granada, Spain. [Myers, Adam D.] Univ Wyoming, Dept Phys & Astron, Laramie, WY 82071 USA. [Nuza, Sebastian E.] Leibniz Inst Astrophys Potsdam AIP, D-14482 Potsdam, Germany. [Paris, Isabelle] Univ Chile, Dept Astron, Santiago, Chile. [Pforr, Janine] Natl Opt Astron Observ, Tucson, AZ 85719 USA. [Prada, Francisco] Campus Int Excellence UAM CSIC, E-28049 Madrid, Spain. [Prada, Francisco] Univ Autonoma Madrid, Inst Fis Teor, UAM CSIC, E-28049 Madrid, Spain. [Price-Whelan, Adrian M.] Columbia Univ, Dept Astron, New York, NY 10027 USA. [Raddick, M. Jordan] Johns Hopkins Univ, Dept Phys & Astron, Ctr Astrophys Sci, Baltimore, MD 21218 USA. [Rebolo, Rafael] CSIC, E-28006 Madrid, Spain. [Richards, Gordon T.] Drexel Univ, Dept Phys, Philadelphia, PA 19104 USA. [Rockosi, Constance M.] Univ Calif Santa Cruz, UCO Lick Observ, Santa Cruz, CA 95064 USA. [Rossi, Graziano] Korea Inst Adv Study, Sch Phys, Seoul 130722, South Korea. [Samushia, Lado] Ilia State Univ, Natl Abastumani Astrophys Observ, GE-1060 Tbilisi, Rep of Georgia. [Seo, Hee-Jong] Univ Calif Berkeley, LBL, Berkeley Ctr Cosmol Phys, Berkeley, CA 94720 USA. [Seo, Hee-Jong; Suzuki, Nao; White, Martin] Univ Calif Berkeley, Dept Phys, Berkeley, CA 94720 USA. [Sheldon, Erin; Slosar, Anze] Brookhaven Natl Lab, Upton, NY 11973 USA. [Tal, Tomer; Wake, David A.] Yale Univ, Dept Astron, New Haven, CT 06520 USA. [Tremonti, Christy A.] Univ Wisconsin Madison, Dept Astron, Madison, WI 53703 USA. [Viel, Matteo] Osserv Astron Trieste, INAF, I-34131 Trieste, Italy. [Viel, Matteo] INFN Natl Inst Nucl Phys, I-34127 Trieste, Italy. [Watson, Mike] Univ Leicester, Dept Phys & Astron, Leicester LE1 7RH, Leics, England. [Weinberg, David H.] Ohio State Univ, Dept Astron, Columbus, OH 43210 USA. [White, Martin] Univ Calif Berkeley, Dept Astron, Berkeley, CA 94720 USA. [Wood-Vasey, W. M.] Univ Pittsburgh, Dept Phys & Astron, PITT PACC, Pittsburgh, PA 15260 USA. [Zhao, Gong-Bo] Chinese Acad Sci, Natl Astron Observ, Beijing 100012, Peoples R China. RP Dawson, KS (reprint author), Univ Utah, Dept Phys & Astron, Salt Lake City, UT 84112 USA. EM kdawson@astro.utah.edu RI Guo, Hong/J-5797-2015; Le Goff, Jean-Marc/E-7629-2013; West, Andrew/H-3717-2014; Mandelbaum, Rachel/N-8955-2014; Ho, Shirley/P-3682-2014; Makler, Martin/G-2639-2012; White, Martin/I-3880-2015; Brandt, William/N-2844-2015; Croft, Rupert/N-8707-2014; Filiz Ak, Nurten/C-9686-2015; Kneib, Jean-Paul/A-7919-2015; Pforr, Janine/J-3967-2015; OI Rubino-Martin, Jose Alberto/0000-0001-5289-3021; Kirkby, David/0000-0002-8828-5463; Viel, Matteo/0000-0002-2642-5707; Escoffier, Stephanie/0000-0002-2847-7498; Masters, Karen/0000-0003-0846-9578; Schmidt, Sarah/0000-0002-7224-7702; Finley, Hayley/0000-0002-1216-8914; Cuesta Vazquez, Antonio Jose/0000-0002-4153-9470; Bovy, Jo/0000-0001-6855-442X; Verde, Licia/0000-0003-2601-8770; McMahon, Richard/0000-0001-8447-8869; Guo, Hong/0000-0003-4936-8247; Mandelbaum, Rachel/0000-0003-2271-1527; Ho, Shirley/0000-0002-1068-160X; Makler, Martin/0000-0003-2206-2651; White, Martin/0000-0001-9912-5070; Brandt, William/0000-0002-0167-2453; Croft, Rupert/0000-0003-0697-2583; Miralda-Escude, Jordi/0000-0002-2316-8370; Filiz Ak, Nurten/0000-0003-3016-5490; Kneib, Jean-Paul/0000-0002-4616-4989; Pforr, Janine/0000-0002-3414-8391; Hogg, David/0000-0003-2866-9403; Davenport, James/0000-0002-0637-835X; McDonald, Patrick/0000-0001-8346-8394 FU Alfred P. Sloan Foundation; University of Arizona; Brazilian Participation Group; Brookhaven National Laboratory; University of Cambridge; Carnegie Mellon University; University of Florida; French Participation Group; German Participation Group; Harvard University; Instituto de Astrofisica de Canarias; Michigan State/Notre Dame/JINA Participation Group; Johns Hopkins University; Lawrence Berkeley National Laboratory; Max Planck Institute for Astrophysics; Max Planck Institute for Extraterrestrial Physics; New Mexico State University; New York University; Ohio State University; Pennsylvania State University; University of Portsmouth; Princeton University; Spanish Participation Group; University of Tokyo; University of Utah; Vanderbilt University; University of Virginia; University of Washington; Yale University; National Science Foundation; U.S. Department of Energy Office of Science FX Funding for SDSS-III has been provided by the Alfred P. Sloan Foundation, the Participating Institutions, the National Science Foundation, and the U.S. Department of Energy Office of Science. The SDSS-III Web site is http://www.sdss3.org/.; SDSS-III is managed by the Astrophysical Research Consortium for the Participating Institutions of the SDSS-III Collaboration including the University of Arizona, the Brazilian Participation Group, Brookhaven National Laboratory, University of Cambridge, Carnegie Mellon University, University of Florida, the French Participation Group, the German Participation Group, Harvard University, the Instituto de Astrofisica de Canarias, the Michigan State/Notre Dame/JINA Participation Group, Johns Hopkins University, Lawrence Berkeley National Laboratory, Max Planck Institute for Astrophysics, Max Planck Institute for Extraterrestrial Physics, New Mexico State University, New York University, Ohio State University, Pennsylvania State University, University of Portsmouth, Princeton University, the Spanish Participation Group, University of Tokyo, University of Utah, Vanderbilt University, University of Virginia, University of Washington, and Yale University. NR 222 TC 502 Z9 503 U1 7 U2 64 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 0004-6256 EI 1538-3881 J9 ASTRON J JI Astron. J. PD JAN PY 2013 VL 145 IS 1 AR 10 DI 10.1088/0004-6256/145/1/10 PG 41 WC Astronomy & Astrophysics SC Astronomy & Astrophysics GA 053DQ UT WOS:000312251100010 ER PT J AU Lapidus, SH Manson, JL Park, H Clement, AJ Ghannadzadeh, S Goddard, P Lancaster, T Moller, JS Blundell, SJ Telling, MTF Kang, J Whangbo, MH Schlueter, JA AF Lapidus, Saul H. Manson, Jamie L. Park, Hyunsoo Clement, Alexander J. Ghannadzadeh, Saman Goddard, Paul Lancaster, Tom Moeller, Johannes S. Blundell, Stephen J. Telling, Mark T. F. Kang, Jinhee Whangbo, Myung-Hwan Schlueter, John A. TI Antiferromagnetic ordering through a hydrogen-bonded network in the molecular solid CuF2(H2O)(2)(3-chloropyridine) SO CHEMICAL COMMUNICATIONS LA English DT Article ID MAGNETIC MODEL SYSTEMS; PYRAZINE; PHYSICS; PYZ AB CuF2(H2O)(2)(3-chloropyridine) possesses a five-coordinate Cu2+ center with a slightly distorted trigonal bypyramidal coordination geometry. Strong intermolecular F center dot center dot center dot H-O hydrogen bonds enable the formation of 2D layers and provide the primary magnetic exchange path that leads to the stabilization of long-range antiferromagnetic (AFM) order below T-N = 2.1 K. C1 [Lapidus, Saul H.; Park, Hyunsoo; Clement, Alexander J.; Schlueter, John A.] Argonne Natl Lab, Div Mat Sci, Argonne, IL 60439 USA. [Manson, Jamie L.] Eastern Washington Univ, Dept Chem & Biochem, Cheney, WA 99004 USA. [Ghannadzadeh, Saman; Goddard, Paul; Moeller, Johannes S.; Blundell, Stephen J.] Univ Oxford, Dept Phys, Clarendon Lab, Oxford OX1 3PU, England. [Lancaster, Tom] Univ Durham, Ctr Phys Mat, Durham DH1 3LE, England. [Telling, Mark T. F.] Rutherford Appleton Lab, ISIS Facil, Chilton OX11 0QX, Oxon, England. [Telling, Mark T. F.] Univ Oxford, Dept Mat, Oxford OX1 3PH, England. [Kang, Jinhee; Whangbo, Myung-Hwan] N Carolina State Univ, Dept Chem, Raleigh, NC 27695 USA. RP Schlueter, JA (reprint author), Argonne Natl Lab, Div Mat Sci, 9700 S Cass Ave, Argonne, IL 60439 USA. EM JASchlueter@anl.gov RI Moller, Johannes/A-4093-2012; Goddard, Paul/A-8638-2015; Telling, Mark/F-3294-2014 OI Moller, Johannes/0000-0003-4369-3890; Goddard, Paul/0000-0002-0666-5236; FU UChicago Argonne, LLC; U.S. National Science Foundation [DMR-1005825]; EPSRC; U.S. Department of Energy Office of Science laboratory [DE-AC02-06CH11357] FX Work at Argonne National Laboratory was supported by UChicago Argonne, LLC, Operator of Argonne National Laboratory ("Argonne"). Argonne, a U.S. Department of Energy Office of Science laboratory, is operated under Contract No. DE-AC02-06CH11357. Work at EWU was supported by the U.S. National Science Foundation under Grant No. DMR-1005825. Work in the UK is funded by the EPSRC and a beamtime allocation from the STFC ISIS Facility. MHW thanks the NERSC Center and the HPC Center of NCSU for computing resources. NR 13 TC 8 Z9 8 U1 0 U2 20 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1359-7345 J9 CHEM COMMUN JI Chem. Commun. PY 2013 VL 49 IS 5 BP 499 EP 501 DI 10.1039/c2cc37444g PG 3 WC Chemistry, Multidisciplinary SC Chemistry GA 052JE UT WOS:000312193100019 PM 23203152 ER PT J AU Haso, F Fang, XK Yin, PC Li, D Ross, JL Liu, TB AF Haso, Fadi Fang, Xikui Yin, Panchao Li, Dong Ross, Jennifer L. Liu, Tianbo TI The self-assembly of a macroion with anisotropic surface charge density distribution SO CHEMICAL COMMUNICATIONS LA English DT Article ID POLYOXOMETALATE; POLYELECTROLYTES; ASSOCIATION; MACROANIONS; TRANSITION; VESICLES; CLUSTERS; METAL AB A macroion, having anisotropic surface charge density distribution, shows unique self-assembly behaviour in polar solvents. Regular "blackberry"-like assemblies form in methanol-water mixtures due to counter-ion mediated attraction and the strong contribution of hydrogen bonding. However, rod-like assemblies form in acetone-water mixtures as the charge inhomogeneity effect overcomes the non-directional hydrogen bonding. C1 [Haso, Fadi; Yin, Panchao; Li, Dong; Ross, Jennifer L.; Liu, Tianbo] Lehigh Univ, Dept Chem, Bethlehem, PA 18015 USA. [Fang, Xikui] Iowa State Univ, US DOE, Ames Lab, Ames, IA 50011 USA. [Fang, Xikui] Iowa State Univ, Dept Phys & Astron, Ames, IA 50011 USA. RP Liu, TB (reprint author), Lehigh Univ, Dept Chem, Bethlehem, PA 18015 USA. EM xfang@Ameslab.gov; Liu@Lehigh.edu RI Yin, Panchao/J-3322-2013; Li, Dong/D-9221-2015; Liu, Tianbo/D-8915-2017 OI Yin, Panchao/0000-0003-2902-8376; Li, Dong/0000-0002-5282-6918; Liu, Tianbo/0000-0002-8181-1790 FU NSF [CHE1026505]; Department of Energy-Basic Energy Sciences [DE-AC02-07CH11358] FX We acknowledge the support of NSF (CHE1026505) and the Department of Energy-Basic Energy Sciences (Contract No. DE-AC02-07CH11358). NR 27 TC 11 Z9 11 U1 2 U2 64 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1359-7345 J9 CHEM COMMUN JI Chem. Commun. PY 2013 VL 49 IS 6 BP 609 EP 611 DI 10.1039/c2cc37235e PG 3 WC Chemistry, Multidisciplinary SC Chemistry GA 052JN UT WOS:000312194000022 PM 23212390 ER PT J AU Rivest, JB Jain, PK AF Rivest, Jessy B. Jain, Prashant K. TI Cation exchange on the nanoscale: an emerging technique for new material synthesis, device fabrication, and chemical sensing SO CHEMICAL SOCIETY REVIEWS LA English DT Review ID SOLID PHASE-TRANSITION; CORE/SHELL NANOCRYSTALS; CDSE NANOCRYSTALS; SEEDED GROWTH; QUANTUM DOTS; COLLOIDAL NANOCRYSTALS; IONIC NANOCRYSTALS; SIZE DEPENDENCE; II-VI; NANORODS AB Cation exchange is an age-old technique for the chemical conversion of liquids or extended solids by place-exchanging the cations in an ionic material with a different set of cations. The technique is undergoing a major revival with the advent of high-quality nanocrystals: researchers are now able to overcome the limitations in bulk systems and fully exploit cation exchange for materials synthesis and discovery via rapid, low-temperature transformations in the solid state. In this tutorial review, we discuss cation exchange as a promising materials synthesis and discovery tool. Exchange on the nanoscale exhibits some unique attributes: rapid kinetics at room temperature (orders of magnitude faster than in the bulk) and the tuning of reactivity via control of nanocrystal size, shape, and surface faceting. These features make cation exchange a convenient tool for accessing nanocrystal compositions and morphologies for which conventional synthesis may not be established. A simple exchange reaction allows extension of nanochemistry to a larger part of the periodic table, beyond the typical gamut of II-VI, IV-VI, and III-V materials. Cation exchange transformations in nanocrystals can be topotactic and size-and shape-conserving, allowing nanocrystals synthesized by conventional methods to be used as templates for production of compositionally novel, multicomponent, or doped nanocrystals. Since phases and compositions resulting from an exchange reaction can be kinetically controlled, rather than governed by the phase diagram, nanocrystals of metastable and hitherto inaccessible compositions are attainable. Outside of materials synthesis, applications for cation exchange exist in water purification, chemical staining, and sensing. Since nanoscale cation exchange occurs rapidly at room temperature, it can be integrated with sensitive environments such as those in biological systems. Cation exchange is already allowing access to a variety of new materials and processes. With better mechanistic understanding and control, researchers may be able to advance the field to a stage where a custom nanostructure of arbitrary complexity would be achievable by simple cation exchange chemistry and a basic understanding of the periodic table. C1 [Jain, Prashant K.] Univ Illinois, Dept Chem, Urbana, IL 61801 USA. [Jain, Prashant K.] Univ Illinois, Beckman Inst Adv Sci & Technol, Urbana, IL 61801 USA. [Rivest, Jessy B.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Mol Foundry, Berkeley, CA 94720 USA. RP Jain, PK (reprint author), Univ Illinois, Dept Chem, 1209 W Calif St, Urbana, IL 61801 USA. EM jain@illinois.edu RI Jain, Prashant/A-4779-2009 OI Jain, Prashant/0000-0002-7306-3972 FU UIUC Beckman Institute FX P. K. Jain thanks UIUC Beckman Institute for support. We acknowledge the research contributions of A. P. Alivisatos, L.-K. Fong, B. Sadtler, B. Beberwyck, L. Amirav, and J. Luther. G. Girolami and E. Chan provided helpful reading of the manuscript. NR 59 TC 154 Z9 154 U1 16 U2 331 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 2013 VL 42 IS 1 BP 89 EP 96 DI 10.1039/c2cs35241a PG 8 WC Chemistry, Multidisciplinary SC Chemistry GA 049FV UT WOS:000311968700007 PM 22968228 ER PT J AU Zou, GF Zhao, J Luo, HM McCleskey, TM Burrell, AK Jia, QX AF Zou, G. F. Zhao, J. Luo, H. M. McCleskey, T. M. Burrell, A. K. Jia, Q. X. TI Polymer-assisted-deposition: a chemical solution route for a wide range of materials SO CHEMICAL SOCIETY REVIEWS LA English DT Review ID OXIDE THIN-FILMS; VAPOR-DEPOSITION; EPITAXIAL STABILIZATION; GROWTH; SILICON; TEMPERATURE; FABRICATION; NITRIDES; CARBIDE; SCIENCE AB In this tutorial article, the recent development of polymer assisted deposition (PAD) for the growth of a wide range of materials, in particular in thin films, is reviewed. Specifically, we describe the unique chemistry and processes of PAD for the deposition of metals, metal-oxides, metal-nitrides, metal-carbides, and their derived composites. Many examples are given not only to illustrate the powerfulness of PAD for high quality coatings, but also to give readers an opportunity to evaluate this technique for specific applications. The challenging issues related to PAD, based on the authors' experience, are also discussed in this review article. C1 [Zou, G. F.; Zhao, J.] Soochow Univ, Sch Energy, Jiangsu Key Lab Thin Films, Suzhou, Peoples R China. [Luo, H. M.] New Mexico State Univ, Dept Chem Engn, Las Cruces, NM 88003 USA. [McCleskey, T. M.; Jia, Q. X.] Los Alamos Natl Lab, Ctr Integrated Nanotechnol, Los Alamos, NM 87545 USA. [Burrell, A. K.] Argonne Natl Lab, Div Chem, Dept CSE, Electctrochem Energy Storage Dept, Argonne, IL 60439 USA. RP Zou, GF (reprint author), Soochow Univ, Sch Energy, Jiangsu Key Lab Thin Films, Suzhou, Peoples R China. EM zouguifu@suda.edu.cn RI Jie, Zhao/B-9939-2013; ZOU, GUIFU/C-8498-2011; Jia, Q. X./C-5194-2008; OI Mccleskey, Thomas/0000-0003-3750-3245 FU National Natural Science Foundation of China [21101110]; Key Program of Science and Technology of Ministry of Education of China [212063]; "Jiangsu Specially-Appointed Professor'' Program [SR1080042]; Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD); U.S. Department of Energy (DOE) through the LANL/LDRD program; Center for Integrated Nanotechnologies, a U.S. Department of Energy, Office of Basic Energy Sciences user facility at Los Alamos National Laboratory [DE-AC52-06NA25396]; NSF [1131290] FX This work was supported by the National Natural Science Foundation of China (21101110), Key Program of Science and Technology of Ministry of Education of China (212063), "Jiangsu Specially-Appointed Professor'' Program (SR1080042), and the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD). The work at Los Alamos was supported by the U.S. Department of Energy (DOE) through the LANL/LDRD program and 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). HL acknowledges funding support from NSF under award number 1131290. NR 58 TC 28 Z9 29 U1 9 U2 161 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 0306-0012 J9 CHEM SOC REV JI Chem. Soc. Rev. PY 2013 VL 42 IS 2 BP 439 EP 449 DI 10.1039/c2cs35283d PG 11 WC Chemistry, Multidisciplinary SC Chemistry GA 056AZ UT WOS:000312460600002 PM 23038606 ER PT J AU Luo, W Neiner, D Karkamkar, A Parab, K Garner, EB Dixon, DA Matson, D Autrey, T Liu, SY AF Luo, Wei Neiner, Doinita Karkamkar, Abhi Parab, Kshitij Garner, Edward B., III Dixon, David A. Matson, Dean Autrey, Tom Liu, Shih-Yuan TI 3-Methyl-1,2-BN-cyclopentane: a promising H-2 storage material? SO DALTON TRANSACTIONS LA English DT Article ID CHEMICAL HYDROGEN STORAGE; AMMONIA BORANE; THERMAL-DECOMPOSITION; BASIS-SETS; DENSITY; FUEL; REGENERATION; EXCHANGE; SYSTEMS; BORON AB We provide detailed characterization of properties for 3-methyl-1,2-BN-cyclopentane 1 that are relevant to H-2 storage applications such as viscosity, thermal stability, H-2 gas stream purity, and polarity. The viscosity of 1 at room temperature is 25 +/- 5 cP, about one fourth the viscosity of olive oil. TGA/MS analysis indicates that liquid carrier 1 is thermally stable at 30 degrees C but decomposes slowly at 50 degrees C. RGA data suggest that the H-2 desorption from 1 is a clean process, producing relatively pure H-2 gas. Compound 1 is a polar zwitterionic-type liquid consistent with theoretical predictions and solvatochromic studies. C1 [Luo, Wei; Liu, Shih-Yuan] Univ Oregon, Dept Chem, Eugene, OR 97403 USA. [Neiner, Doinita; Karkamkar, Abhi; Parab, Kshitij; Matson, Dean; Autrey, Tom] Pacific NW Natl Lab, Richland, WA 99352 USA. [Garner, Edward B., III; Dixon, David A.] Univ Alabama, Dept Chem, Tuscaloosa, AL 35487 USA. RP Liu, SY (reprint author), Univ Oregon, Dept Chem, Eugene, OR 97403 USA. EM lsy@uoregon.edu RI Liu, Shih-Yuan/J-7813-2012 OI Liu, Shih-Yuan/0000-0003-3148-9147 FU U.S. Department of Energy [DE-EE-0005658]; NSF [CHE-0923589]; Fuel Cell Technology Program at U.S. DOE, Office of Energy Efficiency and Renewable Energy; University of Alabama FX S.-Y.L. and D. A. D. gratefully acknowledge the U.S. Department of Energy (DE-EE-0005658) for financial support. Funding for the University of Oregon Chemistry Research and Instrumentation Services was furnished in part by the NSF (CHE-0923589). T. A. acknowledges support from the Fuel Cell Technology Program at U.S. DOE, Office of Energy Efficiency and Renewable Energy. Pacific Northwest National Laboratory is operated by Battelle. D. A. D. thanks the Robert Ramsay Chair Fund of The University of Alabama for support. NR 39 TC 16 Z9 16 U1 0 U2 53 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1477-9226 J9 DALTON T JI Dalton Trans. PY 2013 VL 42 IS 3 BP 611 EP 614 DI 10.1039/c2dt31617j PG 4 WC Chemistry, Inorganic & Nuclear SC Chemistry GA 052TF UT WOS:000312220700003 PM 22992627 ER PT J AU Karkamkar, A Parab, K Camaioni, DM Neiner, D Cho, HM Nielsen, TK Autrey, T AF Karkamkar, Abhi Parab, Kshitij Camaioni, Donald M. Neiner, Doinita Cho, Herman Nielsen, Thomas K. Autrey, Tom TI A thermodynamic and kinetic study of the heterolytic activation of hydrogen by frustrated borane-amine Lewis pairs SO DALTON TRANSACTIONS LA English DT Article ID FREE CATALYTIC-HYDROGENATION; H-2 ACTIVATION; DIHYDROGEN ACTIVATION; REACTIVITY AB Calorimetry is used to measure the reaction enthalpies of hydrogen (H-2) activation by 2,6-lutidine (Lut), 2,2,6,6-tetramethylpiperidine (TMP), N-methyl-2,2,6,6-tetramethylpiperidine (MeTMP), and tri-tert-butylphosphine (TBP) with tris(pentafluorophenyl) borane (BCF). At 6.6 bar H-2 the conversion of the Lewis acid Lewis base pair to the corresponding ionic pair in bromobenzene at 294 K was quantitative in under 60 min. Integration of the heat release from the reaction of the Frustrated Lewis Pair (FLP) with H-2 as a function of time yields a relative rate of hydrogenation in addition to the enthalpy of hydrogenation. The half-lives of hydrogenation range from 230 s with TMP, Delta H-H2 = -31.5(0.2) kcal mol(-1), to 1400 s with Lut, Delta H-H2 = -23.4(0.4) kcal mol(-1). The B-11 nuclear magnetic resonance (NMR) spectrum of B(C6F5)(3) in bromobenzene exhibits three distinct traits depending on the sterics of the Lewis base; (1) in the presence of pyridine, only the dative bond adduct pyridine-B(C6F5)(3) is observed; (2) in the presence of TMP and MeTMP, only the free B(C6F5)(3) is observed; and (3) in the presence of Lut, both the free B(C6F5)(3) and the Lut-B(C6F5)(3) adduct appear in equilibrium. A measure of the change in K-eq of Lut + B(C6F5)(3) double left right arrow Lut-B(C6F5)(3) as a function of temperature provides thermodynamic properties of the Lewis acid Lewis base adduct, Delta H = -17.9(1.0) kcal mol(-1) and a Delta S = -49.2(2.5) cal mol(-1) K, suggesting the Lut-B(C6F5)(3) adduct is more stable in bromobenzene than in toluene. C1 [Karkamkar, Abhi; Parab, Kshitij; Camaioni, Donald M.; Neiner, Doinita; Cho, Herman; Autrey, Tom] Pacific NW Natl Lab, Richland, WA 99354 USA. [Nielsen, Thomas K.] Aarhus Univ, Dept Chem, DK-8000 Aarhus, Denmark. RP Autrey, T (reprint author), Pacific NW Natl Lab, 902 Battelle Blvd, Richland, WA 99354 USA. EM tom.autrey@pnnl.gov FU U.S. Department of Energy's Basic Energy Sciences, Division of Chemical Sciences, Biosciences and Geosciences; Laboratory Directed Research and Development Program at Pacific Northwest National Laboratory (PNNL); DOE Office of Biological and Environmental Research FX This research was supported by the U.S. Department of Energy's Basic Energy Sciences, Division of Chemical Sciences, Biosciences and Geosciences. D. M. C. and A. K. acknowledge support by the Laboratory Directed Research and Development Program at Pacific Northwest National Laboratory (PNNL), which provided funding for the kinetic analyses of the calorimetry data. The work was performed in part at the Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility sponsored by the DOE Office of Biological and Environmental Research. EMSL is located at Pacific Northwest National Laboratory (PNNL), which is operated by Battelle for DOE. The authors are grateful to Drs I. Papai (Hungarian Academy of Sciences), T. Repo (Univ. of Helsinki), D. W. Stephan (Univ. of Toronto) and Z.M. Heiden (PNNL) for many insightful discussions. NR 24 TC 22 Z9 22 U1 1 U2 56 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1477-9226 J9 DALTON T JI Dalton Trans. PY 2013 VL 42 IS 3 BP 615 EP 619 DI 10.1039/c2dt31628e PG 5 WC Chemistry, Inorganic & Nuclear SC Chemistry GA 052TF UT WOS:000312220700004 PM 22996636 ER PT J AU Nielsen, TK Karkamkar, A Bowden, M Besenbacher, F Jensen, TR Autrey, T AF Nielsen, Thomas K. Karkamkar, Abhi Bowden, Mark Besenbacher, Flemming Jensen, Torben R. Autrey, Tom TI Methods to stabilize and destabilize ammonium borohydride SO DALTON TRANSACTIONS LA English DT Article ID HYDROGEN-STORAGE MATERIALS; ACTIVATION; BORANE; RELAXATION; COMPLEXES; KINETICS; RELEASE; VOLUMES; LIBH4 AB Ammonium borohydride, NH4BH4, has a high hydrogen content of rho(m) = 24.5 wt% H-2 and releases 18 wt% H-2 below T = 160 degrees C. However, the half-life of bulk NH4BH4 at ambient temperatures and pressures, similar to 6 h, is insufficient for practical applications. The decomposition of NH4BH4 (ABH(2)) was studied at variable hydrogen and argon back pressures to investigate possible pressure mediated stabilization effects. The hydrogen release rate from solid ABH(2) at ambient temperatures is reduced by similar to 16% upon increasing the hydrogen back pressure from 5 to 54 bar. Similar results were obtained using argon pressure and the observed stabilization may be explained by a positive volume of activation, ca. 73 +/- 17 cc mol(-1), in the transition state leading to hydrogen release. Nanoconfinement in mesoporous silica, MCM-41, was investigated as alternative means to stabilize NH4BH4. However, other factors appear to significantly destabilize NH4BH4 and it rapidly decomposes at ambient temperatures into [(NH3)(2)BH2][BH4] (DADB) in accordance with the bulk reaction scheme. The hydrogen desorption kinetics from nanoconfined [(NH3)(2)BH2][BH4] is moderately enhanced as evidenced by a reduction in the DSC decomposition peak temperature of Delta T = -13 degrees C as compared to the bulk material. Finally, we note a surprising result, storage of DADB at temperature <-30 degrees C transformed, reversibly, the [(NH3)(2)BH2][BH4] into a new low temperature polymorph as revealed by both XRD and solid state MAS B-11 MAS NMR. C1 [Karkamkar, Abhi; Bowden, Mark; Autrey, Tom] Pacific NW Natl Lab, Richland, WA 99354 USA. [Nielsen, Thomas K.; Jensen, Torben R.] Aarhus Univ, Ctr Energy Mat, Interdisciplinary Nanosci Ctr iNano, DK-8000 Aarhus, Denmark. [Nielsen, Thomas K.; Jensen, Torben R.] Aarhus Univ, Dept Chem, DK-8000 Aarhus, Denmark. [Besenbacher, Flemming] Aarhus Univ, Interdisciplinary Nanosci Ctr iNANO, DK-8000 Aarhus C, Denmark. [Besenbacher, Flemming] Aarhus Univ, Dept Phys & Astron, DK-8000 Aarhus C, Denmark. RP Autrey, T (reprint author), Pacific NW Natl Lab, Richland, WA 99354 USA. EM tom.autrey@pnnl.gov OI Jensen, Torben Rene/0000-0002-4278-3221 FU Danish Strategic Research Council (Centre for Energy Materials); U.S. Department of Energy's Basic Energy Sciences, Division of Chemical Sciences, Biosciences and Geosciences; DOE Office of Biological and Environmental Research FX TKN was supported by the Danish Strategic Research Council (Centre for Energy Materials). TA, AK and MB were supported by the U.S. Department of Energy's Basic Energy Sciences, Division of Chemical Sciences, Biosciences and Geosciences. TA thanks for useful discussion. The work was performed in part at the Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility sponsored by the DOE Office of Biological and Environmental Research. EMSL is located at Pacific Northwest National Laboratory (PNNL), which is operated by Battelle for DOE. The authors are grateful to Drs H. Hagemann (University Geneva) and C. Ratcliffe (NRC) for useful discussion. NR 33 TC 5 Z9 5 U1 2 U2 44 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1477-9226 J9 DALTON T JI Dalton Trans. PY 2013 VL 42 IS 3 BP 680 EP 687 DI 10.1039/c2dt31591b PG 8 WC Chemistry, Inorganic & Nuclear SC Chemistry GA 052TF UT WOS:000312220700012 PM 22976038 ER PT J AU Saiz, E Zimmermann, EA Lee, JS Wegst, UGK Tomsia, AP AF Saiz, Eduardo Zimmermann, Elizabeth A. Lee, Janice S. Wegst, Ulrike G. K. Tomsia, Antoni P. TI Perspectives on the role of nanotechnology in bone tissue engineering SO DENTAL MATERIALS LA English DT Article DE Bone; Nanotechnology; Bone scaffolds; Composites; Drug delivery; Cell seeding ID MESENCHYMAL STEM-CELL; DRUG-DELIVERY SYSTEMS; 3-DIMENSIONAL BIOMIMETIC MINERALIZATION; GLYCOL) FUMARATE) HYDROGELS; GROWTH-FACTOR DELIVERY; BIOACTIVE GLASS; IN-VITRO; CALCIUM-PHOSPHATE; TRANSFORMING GROWTH-FACTOR-BETA-1; OSTEOBLAST DIFFERENTIATION AB Objective. This review surveys new developments in bone tissue engineering, specifically focusing on the promising role of nanotechnology and describes future avenues of research. Methods. The review first reinforces the need to fabricate scaffolds with multi-dimensional hierarchies for improved mechanical integrity. Next, new advances to promote bioactivity by manipulating the nanolevel internal surfaces of scaffolds are examined followed by an evaluation of techniques using scaffolds as a vehicle for local drug delivery to promote bone regeneration/integration and methods of seeding cells into the scaffold. Results. Through a review of the state of the field, critical questions are posed to guide future research toward producing materials and therapies to bring state-of-the-art technology to clinical settings. Significance. The development of scaffolds for bone regeneration requires a material able to promote rapid bone formation while possessing sufficient strength to prevent fracture under physiological loads. Success in simultaneously achieving mechanical integrity and sufficient bioactivity with a single material has been limited. However, the use of new tools to manipulate and characterize matter down to the nano-scale may enable a new generation of bone scaffolds that will surpass the performance of autologous bone implants. Published by Elsevier Ltd on behalf of Academy of Dental Materials. C1 [Zimmermann, Elizabeth A.; Tomsia, Antoni P.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. [Saiz, Eduardo] Univ London Imperial Coll Sci Technol & Med, Dept Mat, Ctr Adv Struct Ceram, London SW7 2AZ, England. [Lee, Janice S.] Univ Calif San Francisco, Dept Oral & Maxillofacial Surg, San Francisco, CA 94143 USA. [Wegst, Ulrike G. K.] Dartmouth Coll, Thayer Sch Engn, Hanover, NH 03755 USA. RP Tomsia, AP (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, 1 Cyclotron Rd,Bldg 62-219, Berkeley, CA 94720 USA. EM aptomsia@lbl.gov RI Zimmermann, Elizabeth/A-4010-2015; OI Wegst, Ulrike G.K./0000-0002-9057-415X; Zimmermann, Elizabeth/0000-0001-9927-3372 FU National Institute of Health (NIH/NIDCR) [5R01 DE015633] FX This work was supported by the National Institute of Health (NIH/NIDCR) under grant No. 5R01 DE015633. NR 133 TC 36 Z9 37 U1 3 U2 103 PU ELSEVIER SCI LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, OXON, ENGLAND SN 0109-5641 J9 DENT MATER JI Dent. Mater. PD JAN PY 2013 VL 29 IS 1 BP 103 EP 115 DI 10.1016/j.dental.2012.08.001 PG 13 WC Dentistry, Oral Surgery & Medicine; Materials Science, Biomaterials SC Dentistry, Oral Surgery & Medicine; Materials Science GA 053KA UT WOS:000312269000009 PM 22901861 ER PT J AU Alonso, DM Wettstein, SG Mellmer, MA Gurbuz, EI Dumesic, JA AF Alonso, David Martin Wettstein, Stephanie G. Mellmer, Max A. Gurbuz, Elif I. Dumesic, James A. TI Integrated conversion of hemicellulose and cellulose from lignocellulosic biomass SO ENERGY & ENVIRONMENTAL SCIENCE LA English DT Article ID LEVULINIC ACID; GAMMA-VALEROLACTONE; SELECTIVE HYDROGENATION; CATALYTIC CONVERSION; FURFURYL ALCOHOL; CORN STOVER; LIQUID; PRETREATMENT; BIOFUELS; TECHNOLOGIES AB Using gamma-valerolactone (GVL) as solvent, the cellulosic fraction of lignocellulosic biomass can be converted into levulinic acid (LA), while at the same conditions the hemicellulose fraction can be converted into furfural. This process allows for the conversion of hemicellulose and cellulose simultaneously in a single reactor, thus eliminating pre-treatment steps to fractionate biomass and simplifying product separation. C1 [Alonso, David Martin; Wettstein, Stephanie G.; Mellmer, Max A.; Gurbuz, Elif I.; Dumesic, James A.] Univ Wisconsin, Dept Chem & Biol Engn, Madison, WI 53706 USA. [Wettstein, Stephanie G.; Mellmer, Max A.; Gurbuz, Elif I.; Dumesic, James A.] Univ Wisconsin, DOE Great Lakes Bioenergy Res Ctr, Madison, WI 53706 USA. RP Alonso, DM (reprint author), Univ Wisconsin, Dept Chem & Biol Engn, 1415 Engn Dr, Madison, WI 53706 USA. EM dumesic@engr.wisc.edu FU DOE Great Lakes Bioenergy Research Center (DOE Office of Science) [BER DE-FC02-07ER64494]; Defense Advanced Research Projects Agency (Surf-cat: Catalysts for Production of JP-8 range molecules from Lignocellulosic Biomass) FX This work was funded in part by the DOE Great Lakes Bioenergy Research Center (DOE Office of Science BER DE-FC02-07ER64494). In addition, this work was supported through funding from the Defense Advanced Research Projects Agency (Surf-cat: Catalysts for Production of JP-8 range molecules from Lignocellulosic Biomass). The views, opinions, and/or findings contained in this article are those of the author and should not be interpreted as representing the official views or policies, either expressed or implied, of the Defense Advanced Research Projects Agency or the Department of Defense. The authors would like to thank Prof. David Hodge from Michigan State University for providing the AHP corn stover and thank Hui Chin Wong and Jher Hau Yeap for performing experiments reported in this paper. NR 30 TC 105 Z9 105 U1 14 U2 273 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1754-5692 J9 ENERG ENVIRON SCI JI Energy Environ. Sci. PD JAN PY 2013 VL 6 IS 1 BP 76 EP 80 DI 10.1039/c2ee23617f PG 5 WC Chemistry, Multidisciplinary; Energy & Fuels; Engineering, Chemical; Environmental Sciences SC Chemistry; Energy & Fuels; Engineering; Environmental Sciences & Ecology GA 054IR UT WOS:000312337700008 ER PT J AU Bae, TH Hudson, MR Mason, JA Queen, WL Dutton, JJ Sumida, K Micklash, KJ Kaye, SS Brown, CM Long, JR AF Bae, Tae-Hyun Hudson, Matthew R. Mason, Jarad A. Queen, Wendy L. Dutton, Justin J. Sumida, Kenji Micklash, Ken J. Kaye, Steven S. Brown, Craig M. Long, Jeffrey R. TI Evaluation of cation-exchanged zeolite adsorbents for post-combustion carbon dioxide capture SO ENERGY & ENVIRONMENTAL SCIENCE LA English DT Article ID METAL-ORGANIC FRAMEWORKS; NEUTRON PROFILE REFINEMENT; CO2 CAPTURE; FLUE-GAS; ADSORPTION EQUILIBRIA; CRYSTAL-STRUCTURE; CH4; STORAGE; 5A; COORDINATION AB A series of zeolite adsorbents has been evaluated for potential application in post-combustion CO2 capture using a new high-throughput gas adsorption instrument capable of measuring 28 samples in parallel. Among the zeolites tested, Ca-A exhibits the highest CO2 uptake (3.72 mmol g(-1) and 5.63 mmol cm(-3)) together with an excellent CO2 selectivity over N-2 under conditions relevant to capture from the dry flue gas stream of a coal-fired power plant. The large initial isosteric heat of adsorption of -58 kJ mol(-1) indicates the presence of strong interactions between CO2 and the Ca-A framework. Neutron and X-ray powder diffraction studies reveal the precise location of the adsorption sites for CO2 in Ca-A and Mg-A. A detailed study of CO2 adsorption kinetics further shows that the performance of Ca-A is not limited by slow CO2 diffusion within the pores. Significantly, Ca-A exhibited a higher volumetric CO2 uptake and CO2/N-2 selectivity than Mg-2(dobdc) (dobdc(4-) = 1,4-dioxido-2,5-benzenedicarboxylate; Mg-MOF-74, CPO-27-Mg), one of the best performing adsorbents. The exceptional performance of Ca-A was maintained in CO2 breakthrough simulations. C1 [Bae, Tae-Hyun; Mason, Jarad A.; Sumida, Kenji; Long, Jeffrey R.] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Bae, Tae-Hyun; Mason, Jarad A.; Sumida, Kenji; Long, Jeffrey R.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. [Hudson, Matthew R.; Queen, Wendy L.; Brown, Craig M.] NIST, Ctr Neutron Res, Gaithersburg, MD 20899 USA. [Hudson, Matthew R.] Univ Maryland, Dept Mat Sci & Engn, College Pk, MD 20742 USA. [Dutton, Justin J.; Micklash, Ken J.; Kaye, Steven S.] Wildcat Discovery Technol Inc, San Diego, CA 92121 USA. RP Bae, TH (reprint author), Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. EM jrlong@berkeley.edu RI Bae, Tae-Hyun/B-9839-2012; Brown, Craig/B-5430-2009; OI Bae, Tae-Hyun/0000-0003-0033-2526; Brown, Craig/0000-0002-9637-9355; Queen, Wendy/0000-0002-8375-2341; Sumida, Kenji/0000-0003-0215-5922 FU Advanced Research Projects Agency-Energy (ARPA-E), U.S. Department of Energy (DoE); U.S. DoE [DE-AC02-06CH11357]; NSF; NIST National Research Council Postdoctoral Fellowship Research Associate program FX This research was funded by the Advanced Research Projects Agency-Energy (ARPA-E), U.S. Department of Energy (DoE). Use of the Advanced Photon Source (APS), an Office of Science User Facility operated for the U.S. DoE Office of Science by Argonne National Laboratory, was supported by the U.S. DoE under Contract DE-AC02-06CH11357. We thank Dr Greg Halder for help with the diffraction data collection on 1-BM-C at the APS and Dr Trudy Bolin and Dr Michael Pape for the use of the helium glovebox in APS Sector 9. We also thank NSF for providing graduate fellowship support for J.A.M., and the NIST National Research Council Postdoctoral Fellowship Research Associate program for support of M.R.H. and W.L.Q. NR 75 TC 95 Z9 96 U1 12 U2 211 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1754-5692 J9 ENERG ENVIRON SCI JI Energy Environ. Sci. PD JAN PY 2013 VL 6 IS 1 BP 128 EP 138 DI 10.1039/c2ee23337a PG 11 WC Chemistry, Multidisciplinary; Energy & Fuels; Engineering, Chemical; Environmental Sciences SC Chemistry; Energy & Fuels; Engineering; Environmental Sciences & Ecology GA 054IR UT WOS:000312337700017 ER PT J AU Wu, YB Lazic, P Hautier, G Persson, K Ceder, G AF Wu, Yabi Lazic, Predrag Hautier, Geoffroy Persson, Kristin Ceder, Gerbrand TI First principles high throughput screening of oxynitrides for water-splitting photocatalysts SO ENERGY & ENVIRONMENTAL SCIENCE LA English DT Article ID VISIBLE-LIGHT-DRIVEN; AUGMENTED-WAVE METHOD; LI-ION BATTERIES; ELECTRONIC-STRUCTURE; METAL-OXIDES; BAND; IRRADIATION; CATHODES; DESIGN; ZRO2 AB In this paper, we present a first principles high throughput screening system to search for new water-splitting photocatalysts. We use the approach to screen through nitrides and oxynitrides. Most of the known photocatalytic materials in the screened chemical space are reproduced. In addition, sixteen new materials are suggested by the screening approach as promising photocatalysts, including three binary nitrides, two ternary oxynitrides and eleven quaternary oxynitrides. C1 [Wu, Yabi; Lazic, Predrag; Hautier, Geoffroy; Ceder, Gerbrand] MIT, Dept Mat Sci & Engn, Cambridge, MA 02139 USA. [Persson, Kristin] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Wu, YB (reprint author), MIT, Dept Mat Sci & Engn, Cambridge, MA 02139 USA. RI Hautier, Geoffroy/A-8357-2011; Lazic, Predrag/K-1908-2012 FU Eni S.p.A. under the Eni-MIT Alliance Solar Frontiers Program; National Science Foundation through TeraGrid resources; Pittsburgh Supercomputing Center; Department of Energy [DE-FG02-96ER4557]; Texas Advanced Computing Center [TG-DMR970008S] FX This work was supported by Eni S.p.A. under the Eni-MIT Alliance Solar Frontiers Program, and the National Science Foundation through TeraGrid resources provided by the Pittsburgh Supercomputing Center and Texas Advanced Computing Center under grant number TG-DMR970008S. Some methodological work has been supported by the Department of Energy under contract DE-FG02-96ER4557. NR 67 TC 59 Z9 59 U1 16 U2 158 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1754-5692 EI 1754-5706 J9 ENERG ENVIRON SCI JI Energy Environ. Sci. PD JAN PY 2013 VL 6 IS 1 BP 157 EP 168 DI 10.1039/c2ee23482c PG 12 WC Chemistry, Multidisciplinary; Energy & Fuels; Engineering, Chemical; Environmental Sciences SC Chemistry; Energy & Fuels; Engineering; Environmental Sciences & Ecology GA 054IR UT WOS:000312337700020 ER PT J AU Arruda, TM Heon, M Presser, V Hillesheim, PC Dai, S Gogotsi, Y Kalinin, SV Balke, N AF Arruda, Thomas M. Heon, Min Presser, Volker Hillesheim, Patrick C. Dai, Sheng Gogotsi, Yury Kalinin, Sergei V. Balke, Nina TI In situ tracking of the nanoscale expansion of porous carbon electrodes SO ENERGY & ENVIRONMENTAL SCIENCE LA English DT Article ID ATOMIC-FORCE MICROSCOPY; CARBIDE-DERIVED CARBON; DOUBLE-LAYER CAPACITORS; NANOPOROUS CARBON; IONIC LIQUIDS; TITANIUM CARBIDE; ELECTROLYTES; INTERFACE; DILATOMETRY; ADSORPTION AB Electrochemical double layer capacitors (EDLC) are rapidly emerging as a promising energy storage technology offering extremely large power densities. Despite significant experimental progress, nanoscale operation mechanisms of the EDLCs remain poorly understood and it is difficult to separate processes at multiple time and length scales involved in operation including that of double layer charging and ionic mass transport. Here we explore the functionality of EDLC microporous carbon electrodes using a combination of classical electrochemical measurements and scanning probe microscopy based dilatometry, thus separating individual stages in charge/discharge processes based on strain generation. These methods allowed us to observe two distinct modes of EDLC charging, one fast charging of the double layer unassociated with strain, and another much slower mass transport related charging exhibiting significant sample volume changes. These studies open the pathway for the exploration of electrochemical systems with multiple processes involved in the charge and discharge, and investigation of the kinetics of those processes. C1 [Arruda, Thomas M.; Kalinin, Sergei V.; Balke, Nina] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. [Heon, Min; Presser, Volker; Gogotsi, Yury] Drexel Univ, Dept Mat Sci & Engn, Philadelphia, PA 19104 USA. [Heon, Min; Presser, Volker; Gogotsi, Yury] Drexel Univ, AJ Drexel Nanotechnol Inst, Philadelphia, PA 19104 USA. [Presser, Volker] INM Leibniz Inst New Mat, Energy Mat Grp, D-66123 Saarbrucken, Germany. [Hillesheim, Patrick C.; Dai, Sheng] Oak Ridge Natl Lab, Chem Sci Div, Oak Ridge, TN 37831 USA. RP Arruda, TM (reprint author), Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. EM balken@ornl.gov RI Presser, Volker/F-1975-2010; Gogotsi, Yury/B-2167-2008; Kalinin, Sergei/I-9096-2012; Arruda, Thomas/C-6134-2012; Balke, Nina/Q-2505-2015; Dai, Sheng/K-8411-2015 OI Presser, Volker/0000-0003-2181-0590; Gogotsi, Yury/0000-0001-9423-4032; Kalinin, Sergei/0000-0001-5354-6152; Arruda, Thomas/0000-0002-6165-2024; Balke, Nina/0000-0001-5865-5892; Dai, Sheng/0000-0002-8046-3931 FU Fluid Interface Reactions, Structures and Transport (FIRST), a National Laboratory Energy Frontier Research Center; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences; Center for Nanophase Materials Sciences; Oak Ridge National Laboratory by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy; German Federal Ministry for Research and Education (BMBF); nanoEES3D project [03EK3013] FX Support was provided by the Fluid Interface Reactions, Structures and Transport (FIRST), a National Laboratory Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences and 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. VP acknowledges funding from the German Federal Ministry for Research and Education (BMBF) in support of the nanoEES3D project (award number 03EK3013) as part of the strategic funding initiative energy storage framework. We are thankful to J. Hettinger (Rowan University) for help with TiC film sputtering. The authors would also like to thank Jennifer M. Black for insightful discussions. NR 39 TC 26 Z9 26 U1 5 U2 118 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1754-5692 J9 ENERG ENVIRON SCI JI Energy Environ. Sci. PD JAN PY 2013 VL 6 IS 1 BP 225 EP 231 DI 10.1039/c2ee23707e PG 7 WC Chemistry, Multidisciplinary; Energy & Fuels; Engineering, Chemical; Environmental Sciences SC Chemistry; Energy & Fuels; Engineering; Environmental Sciences & Ecology GA 054IR UT WOS:000312337700027 ER PT J AU Lu, XC Kirby, BW Xu, W Li, GS Kim, JY Lemmon, JP Sprenkle, VL Yang, ZG AF Lu, Xiaochuan Kirby, Brent W. Xu, Wu Li, Guosheng Kim, Jin Y. Lemmon, John P. Sprenkle, Vincent L. Yang, Zhenguo TI Advanced intermediate-temperature Na-S battery SO ENERGY & ENVIRONMENTAL SCIENCE LA English DT Article ID SODIUM-SULFUR BATTERIES; RAMAN-SPECTROSCOPY; BETA ALUMINA; ENERGY; CHALLENGES; CONVERSION; ANIONS AB In this study, we reported an intermediate-temperature (similar to 150 degrees C) sodium-sulfur (Na-S) battery. With a relatively low operating temperature, this novel battery could reduce the cost and safety issues associated with the conventional high-temperature (300-350 degrees C) Na- S battery. A dense beta ''-Al2O3 solid membrane and tetraglyme were utilized as the electrolyte separator and catholyte solvent in this battery. Solubility tests indicated that a cathode mixture of Na2S4 and S exhibited extremely high solubility in tetraglyme (e.g., >4.1 M for Na2S4 + 4 S). CV scans of Na2S4 in tetraglyme revealed two pairs of redox couples with peaks at around 2.22 and 1.75 V, corresponding to the redox reactions of polysulfide species. The discharge/charge profiles of the Na-S battery showed a slope region and a plateau, indicating multiple steps and cell reactions. In situ Raman measurements during battery operation suggested that polysulfide species were formed in the sequence of Na2S5 + S -> Na2S5 + Na2S4 -> Na2S4 + Na2S2 during discharge and in a reverse order during charge. This battery showed dramatic improvement in rate capacity and cycling stability over room-temperature Na- S batteries, which makes it more attractive for renewable energy integration and other grid related applications. C1 [Lu, Xiaochuan; Kirby, Brent W.; Xu, Wu; Li, Guosheng; Kim, Jin Y.; Lemmon, John P.; Sprenkle, Vincent L.; Yang, Zhenguo] Pacific NW Natl Lab, Energy & Environm Directorate, Richland, WA 99354 USA. RP Lu, XC (reprint author), Pacific NW Natl Lab, Energy & Environm Directorate, Richland, WA 99354 USA. EM Xiaochuan.Lu@pnnl.gov; Jin.Kim@pnnl.gov OI Xu, Wu/0000-0002-2685-8684 FU Laboratory-Directed Research and Development (LDRD) Program of the Pacific Northwest National Laboratory (PNNL); U.S. Department of Energy's (DOE's) Office of Electricity Delivery & Energy Reliability (OE); Department of Energy [DE-AC05-76RL01830] FX The work was supported by the Laboratory-Directed Research and Development (LDRD) Program of the Pacific Northwest National Laboratory (PNNL) and the U.S. Department of Energy's (DOE's) Office of Electricity Delivery & Energy Reliability (OE). We appreciate useful discussions with Dr Imre Gyuk of the DOE-OE Grid Storage Program. PNNL is a multi-program laboratory operated by Battelle Memorial Institute for the Department of Energy under contract DE-AC05-76RL01830. NR 30 TC 30 Z9 33 U1 18 U2 228 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1754-5692 J9 ENERG ENVIRON SCI JI Energy Environ. Sci. PD JAN PY 2013 VL 6 IS 1 BP 299 EP 306 DI 10.1039/c2ee23606k PG 8 WC Chemistry, Multidisciplinary; Energy & Fuels; Engineering, Chemical; Environmental Sciences SC Chemistry; Energy & Fuels; Engineering; Environmental Sciences & Ecology GA 054IR UT WOS:000312337700034 ER PT J AU Waller, BH Olson, DG Currie, DH Guss, AM Lynd, LR AF Waller, Benjamin H. Olson, Daniel G. Currie, Devin H. Guss, Adam M. Lynd, Lee R. TI Exchange of type II dockerin-containing subunits of the Clostridium thermocellum cellulosome as revealed by SNAP-tags SO FEMS MICROBIOLOGY LETTERS LA English DT Article DE dockerin; cohesin; cellulosome; Clostridium thermocellum; SNAP-tag ID QUANTITATIVE PROTEOMIC ANALYSIS; EXPRESSION; CELLULASE; ETHANOL; GENES AB Clostridium thermocellum is a thermophilic anaerobic bacterium which efficiently hydrolyzes and metabolizes cellulose to ethanol through the action of its cellulosome, a multiprotein enzymatic complex. A fluorescent protein probe, consisting of a type II dockerin module fused to a SNAP-tag, was developed in order to gain insight into the quaternary configuration of the cellulosome and to investigate the effect of deleting cipA, the protein scaffold on which the cellulosome is built. Fluorescence microscopy suggested that the probe had localized to polycellulosomal protuberances on the cell surface. Surprisingly, fluorescence intensity did not substantially change in the cipA deletion mutants. Sequential labeling experiments suggested that this was a result of bound type II dockerins from CipA being replaced by unbound type II dockerins from the fluorophore-SNAP-XDocII probe. This mechanism of dockerin exchange could represent an efficient means for modifying cellulosome composition. C1 [Waller, Benjamin H.; Currie, Devin H.; Lynd, Lee R.] Dartmouth Coll, Dept Biol Sci, Hanover, NH 03755 USA. [Waller, Benjamin H.; Olson, Daniel G.; Currie, Devin H.; Guss, Adam M.; Lynd, Lee R.] BioEnergy Sci Ctr, Oak Ridge, TN USA. [Olson, Daniel G.; Lynd, Lee R.] Dartmouth Coll, Thayer Sch Engn, Hanover, NH 03755 USA. [Guss, Adam M.] Oak Ridge Natl Lab, Biosci Div, Oak Ridge, TN USA. RP Lynd, LR (reprint author), Dartmouth Coll, Dept Biol Sci, Hanover, NH 03755 USA. EM lee.r.lynd@dartmouth.edu RI Lynd, Lee/N-1260-2013; Guss, Adam/A-6204-2011; Olson, Daniel/F-2058-2011 OI Lynd, Lee/0000-0002-5642-668X; Guss, Adam/0000-0001-5823-5329; Olson, Daniel/0000-0001-5393-6302 NR 21 TC 6 Z9 7 U1 0 U2 21 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0378-1097 J9 FEMS MICROBIOL LETT JI FEMS Microbiol. Lett. PD JAN PY 2013 VL 338 IS 1 BP 46 EP 53 DI 10.1111/1574-6968.12029 PG 8 WC Microbiology SC Microbiology GA 053WA UT WOS:000312304700007 PM 23082914 ER PT J AU Freed, AD Einstein, DR AF Freed, Alan D. Einstein, Daniel R. TI An implicit elastic theory for lung parenchyma SO INTERNATIONAL JOURNAL OF ENGINEERING SCIENCE LA English DT Article DE Biomechanics; Soft solids; Compressible solids; Constitutive equations; Deviatoric strain; Elastic moduli; Tangent moduli; Thermodynamics ID CONSTITUTIVE LAW; MODEL; MECHANICS; DISTORTION; BIOMEMBRANES; DEFORMATION; RESPIRATION; MEMBRANE; STRESS; STRAIN AB The airways and parenchyma of lung experience large deformations during normal respiration. Spatially accurate predictions of airflow patterns and aerosol transport therefore require respiration to be modeled as a fluid-structure interaction problem. Such computational models in turn require constitutive models for the parencyhma that are both accurate and efficient. Herein, an implicit theory of elasticity is derived from thermodynamics to meet this need, leading to a generic template for strain-energy that is shown to be an exact analogue for the well-known Fung model that is the root of modern constitutive theory of tissues. To support this theory, we also propose a novel definition of Lagrangian strain rate. Unlike the classic definition of Lagrangian strain rate, this new definition is separable into volumetric and deviatoric terms, a separation that is both mathematically and physically justified. Within this framework, a novel material model capable of describing the elastic contribution of the nonlinear response of parenchyma is constructed and characterized against published data. (C) 2012 Elsevier Ltd. All rights reserved. C1 [Freed, Alan D.] Saginaw Valley State Univ, Dept Mech Engn, University Ctr, MI 48710 USA. [Einstein, Daniel R.] Pacific NW Natl Lab, Olympia, WA 98502 USA. RP Freed, AD (reprint author), Saginaw Valley State Univ, Dept Mech Engn, 202 Pioneer Hall,7400 Bay Rd, University Ctr, MI 48710 USA. EM adfreed@svsu.edu; daniel.einstein@pnnl.gov OI Freed, Alan/0000-0002-3492-0628 FU National Heart, Lung, and Blood Institute [R01HL073598] FX The project described was supported by Award Number R01HL073598 from the National Heart, Lung, and Blood Institute. The content is solely the responsibility of the authors and does not necessarily reflect the official views of the National Heart, Lung, and Blood Institute or the National Institutes of Health. NR 48 TC 15 Z9 15 U1 5 U2 20 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0020-7225 J9 INT J ENG SCI JI Int. J. Eng. Sci. PD JAN PY 2013 VL 62 BP 31 EP 47 DI 10.1016/j.ijengsci.2012.08.003 PG 17 WC Engineering, Multidisciplinary SC Engineering GA 055MZ UT WOS:000312422300004 PM 23144500 ER PT J AU Borg, JP Morrissey, MP Perich, CA Vogler, TJ Chhabildas, LC AF Borg, J. P. Morrissey, M. P. Perich, C. A. Vogler, T. J. Chhabildas, L. C. TI In situ velocity and stress characterization of a projectile penetrating a sand target: Experimental measurements and continuum simulations SO INTERNATIONAL JOURNAL OF IMPACT ENGINEERING LA English DT Article DE Penetration dynamics; Sand; Particle image velocimetry; Hydrodynamic simulations ID IMPACT; DYNAMICS; CONCRETE; EQUATION; MEDIA AB Understanding the impact, penetration and cavity formation of heterogeneous granular systems is of fundamental importance to a wide variety of research endeavors. In this work a series of experiments were conducted in order to investigate the penetration dynamics of loose dry sand. High-speed photography coupled with a particle image velocimetry (PIV) technique was used to capture both the grain and bulk response of the penetration event, while buried quartz gages simultaneously recorded transmitted stress wave profiles. Depth of penetration was measured via postmortem examination. Experiments were conducted over a velocity range of 30-200 m/s using both cylindrical and spherical projectiles in a unique semi-infinite experimental configuration in order to directly observe a cross-section of the impact and penetration event. The experimental results are compared to simple continuum Eulerian hydrocode simulations and an analytic penetration model. The simulations are not able to resolve both stress and velocity measurements. However, the simulations do reproduce the depth of penetration for a wide variety of penetration experiments. (C) 2012 Elsevier Ltd. All rights reserved. C1 [Borg, J. P.; Morrissey, M. P.; Perich, C. A.] Marquette Univ, Dept Mech Engn, Milwaukee, WI 53233 USA. [Vogler, T. J.] Sandia Natl Labs, Livermore, CA 94550 USA. [Chhabildas, L. C.] USAF, AFRL RW, Eglin, FL 32542 USA. RP Borg, JP (reprint author), Marquette Univ, Dept Mech Engn, 1515 W Wisconsin Ave, Milwaukee, WI 53233 USA. EM john.borg@mu.edu FU Defense Threat Reduction Agency [HDTRA1-09-0045] FX Funding for this work was provided by the Defense Threat Reduction Agency under grant HDTRA1-09-0045. We would like to acknowledge Wisconsin Space Grant Consortium (WSGC) for providing summer support for the students to collect preliminary data, without which this research could not have been initiated. NR 53 TC 16 Z9 17 U1 3 U2 25 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0734-743X EI 1879-3509 J9 INT J IMPACT ENG JI Int. J. Impact Eng. PD JAN PY 2013 VL 51 BP 23 EP 35 DI 10.1016/j.ijimpeng.2012.07.009 PG 13 WC Engineering, Mechanical; Mechanics SC Engineering; Mechanics GA 053OM UT WOS:000312282300004 ER PT J AU Ahmed, S AF Ahmed, Shahid TI Transient analysis of printed lines using finite-difference time-domain method SO INTERNATIONAL JOURNAL OF NUMERICAL MODELLING-ELECTRONIC NETWORKS DEVICES AND FIELDS LA English DT Article DE ultra-wideband; digital pulse; electromagnetic coupling (EMC); electromagnetic interference (EMI); finite-difference time-domain (FDTD); microstrip lines; crosstalk ID MULTILAYER STRUCTURES; TRANSMISSION-LINES; MICROSTRIP LINES; LAYERED MEDIA; CROSSTALK; DISTORTION; CIRCUITS; INTERCONNECTS; PROPAGATION; DISPERSION AB Comprehensive studies of ultra-wideband pulses and electromagnetic coupling on printed coupled lines have been performed using full-wave 3D finite-difference time-domain analysis. Effects of unequal phase velocities of coupled modes, coupling between line traces, and the frequency dispersion on the waveform fidelity and crosstalk have been investigated in detail. To discriminate the contributions of different mechanisms into pulse evolution, single and coupled microstrip lines without (?r?=?1) and with (?r?>?1) dielectric substrates have been examined. To consistently compare the performance of the coupled lines with substrates of different permittivities and transients of different characteristic times, a generic metric similar to the electrical wavelength has been introduced. The features of pulse propagation on coupled lines with layered and pedestal substrates and on the irregular traces have been explored. Physical interpretations of the simulation results are discussed in the paper. Copyright (C) 2012 John Wiley & Sons, Ltd. C1 Thomas Jefferson Natl Accelerator Facil, Newport News, VA 23606 USA. RP Ahmed, S (reprint author), Thomas Jefferson Natl Accelerator Facil, 12050 Jefferson Ave,Suite 704, Newport News, VA 23606 USA. EM shahid.ahmed@ieee.org NR 27 TC 0 Z9 0 U1 1 U2 12 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0894-3370 J9 INT J NUMER MODEL EL JI Int. J. Numer. Model.-Electron. Netw. Device Fields PD JAN-FEB PY 2013 VL 26 IS 1 BP 74 EP 86 DI 10.1002/jnm.1838 PG 13 WC Engineering, Electrical & Electronic; Mathematics, Interdisciplinary Applications SC Engineering; Mathematics GA 055US UT WOS:000312443900007 ER PT J AU Cerreta, EK Bingert, JF Gray, GT Trujillo, CP Lopez, MF Bronkhorst, CA Hansen, BL AF Cerreta, E. K. Bingert, J. F. Gray, G. T., III Trujillo, C. P. Lopez, M. F. Bronkhorst, C. A. Hansen, B. L. TI Microstructural examination of quasi-static and dynamic shear in high-purity iron SO INTERNATIONAL JOURNAL OF PLASTICITY LA English DT Article DE Dynamic fracture; Microstructures; Thermo-mechanical processes; Shear texture ID HIGH-STRAIN RATES; STAINLESS-STEEL; MECHANICAL-BEHAVIOR; BAND FORMATION; TEXTURE DEVELOPMENT; PLASTIC-FLOW; LOCALIZATION; DEFORMATION; FE; INSTABILITY AB Numerous studies have examined the microstructural evolution of adiabatic shear bands through the utilization of the forced shear or "tophat" test specimen. While the geometry of this specimen does not allow for the microstructure to play a dominant role in the location of a shear band, the forced shear specimen has been shown to be particularly useful for characterizing the influence of parameters such as strain rate, temperature, strain, and load on the microstructural evolution within a shear band. Additionally, many studies have also utilized this geometry to advance the understanding of shear band development in a number of materials. In this study we systematically examine the influence of integrated loading states on the dynamic shear localization response of high-purity Fe by varying the geometry of the forced shear specimen. Post-mortem characterization was performed to quantify the width of the localizations and to examine the microstructural and textural evolution of shear deformation in a body centered cubic (BCC) metal. Increased instability in mechanical response is strongly correlated with development of enhanced intergranular misorientations and high angle boundary evolution. Stress state was also critical to the localization process. Single-component, simple shear configurations were found to promote instability over multi-component stress states. In addition, these geometries resulted in traditional BCC deformation shear textures, while multi-component stress states led to less developed textures. Published by Elsevier Ltd. C1 [Cerreta, E. K.; Bingert, J. F.; Gray, G. T., III; Trujillo, C. P.; Lopez, M. F.; Bronkhorst, C. A.; Hansen, B. L.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Cerreta, EK (reprint author), Los Alamos Natl Lab, MST-8 MSG755, Los Alamos, NM 87545 USA. EM ecerreta@lanl.gov RI Bronkhorst, Curt/B-4280-2011 OI Bronkhorst, Curt/0000-0002-2709-1964 FU Department of Defense (DoD); Department of Energy (DOE) FX This work has been performed under the auspices of the United States Department of Energy and was supported by the Joint Department of Defense (DoD) and Department of Energy (DOE) Munitions Technology Development Program. NR 50 TC 11 Z9 11 U1 1 U2 45 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0749-6419 J9 INT J PLASTICITY JI Int. J. Plast. PD JAN PY 2013 VL 40 BP 23 EP 38 DI 10.1016/j.ijplas.2012.06.005 PG 16 WC Engineering, Mechanical; Materials Science, Multidisciplinary; Mechanics SC Engineering; Materials Science; Mechanics GA 052WJ UT WOS:000312230400002 ER PT J AU WoldeGabriel, G Endale, T White, TD Thouveny, N Hart, WK Renne, PR Asfaw, B AF WoldeGabriel, Giday Endale, Tamrat White, Tim D. Thouveny, Nicolas Hart, William K. Renne, Paul R. Asfaw, Berhane TI The role of tephra studies in African paleoanthropology as Hakoma Tuff SO JOURNAL OF AFRICAN EARTH SCIENCES LA English DT Article DE Tephra; Paleoanthropology; Afar Rift; Main Ethiopian Rift; Hominids ID MIDDLE-AWASH VALLEY; PLEISTOCENE HOMO-SAPIENS; EARLY PLIOCENE HOMINIDS; KOOBI-FORA FORMATION; MAIN ETHIOPIAN RIFT; WEST-CENTRAL AFAR; TULU BOR TUFF; HADAR FORMATION; SOUTHERN ETHIOPIA; TURKANA-BASIN AB Beginning in the 1960s, geological and paleoanthropological exploration of the Ethiopian rift system's basins have led to the discovery and assembly of the most comprehensive record of human biological and technological change during the last 6 million years. The hominid fossils, including partial skeletons, were primarily discovered in the Afar Rift, the Main Ethiopian Rift, and in the Omo Basin of the broadly rifted zone of SW Ethiopia. The paleoanthropological research areas within the SW Afar Rift that have yielded many diverse hominid species and the oldest stone tools are, from north to south, Woranso-Mille (aff. Ardipithecus and Au. afarensis), Hadar (Au. afarensis, Homo sp.), Dikika (Au. afarensis), Gona (Ar. kadabba, Ar. ramidus, H. erectus, and oldest stone tools), Middle Awash (Ar. kadabba, Ar. ramidus, Au. anamensis, Au. afarensis, Au. garhi, H. erectus, H. rhodesiensis, H. sapiens idaltu, and the oldest paleo-butchery locality), and Galili (Au. afarensis). Additional hominid remains were discovered at Melka Kunture on the banks of the Awash River near its source along the western margin of the central part of the Main Ethiopian Rift (H. erectus), at Konso (H. erectus and A. boisei), and at the southern end of the MER, and in the Omo Basin (Au. anamensis, Au. afarensis, Au. aethiopicus, Au. boisei, H. habilis, and H. erectus). Distal and sometimes proximal tephra units interbedded within fossilifeous sedimentary deposits have become key elements in this work by providing chronological and correlative control and depositional contexts. Several regional tephra markers have been identified within the northern half of the eastern African rift valley in Ethiopia and Kenya, and in marine sediments of the Gulf of Aden Rift and the NW Indian Ocean. Out of the many regional tephra stratigraphic markers that range in age from the early Pliocene (3.97 Ma) to the late Pleistocene (0.16 Ma), the Sidi Hakoma Tuff (SHT) has been more widely identified and thoroughly characterized than any of the others. An age of 3.446 +/- 0.041 Ma was determined on the SHT according to the most recent calibration, and it is the only regional stratigraphic marker whose source has been traced to a buried caldera in the central sector of the Main Ethiopian Rift. This paper describes new SHT occurrences and presents chemical and chronological results in the context of a broader review of the importance of this key marker. Moreover, the geographic distributions, probable dispersal mechanisms, and importance of regional tephra units in determining the tectonic and sedimentological processes in the different rift basins of the eastern African rift valleys are considered. Published by Elsevier Ltd. C1 [WoldeGabriel, Giday] Los Alamos Natl Lab, Earth Environm Sci Div, Los Alamos, NM 87545 USA. [Endale, Tamrat; Thouveny, Nicolas] CEREGE, F-13545 Aix En Provence 04, France. [White, Tim D.] Univ Calif Berkeley, Dept Integrat Biol, Berkeley, CA 94720 USA. [White, Tim D.] Univ Calif Berkeley, Human Evolut Res Ctr, Berkeley, CA 94720 USA. [Hart, William K.] Miami Univ, Dept Geol & Environm Earth Sci, Oxford, OH 45056 USA. [Renne, Paul R.] Berkeley Geochronol Ctr, Berkeley, CA 94709 USA. [Renne, Paul R.] Univ Calif Berkeley, Dept Earth & Planetary Sci, Berkeley, CA 94720 USA. [Asfaw, Berhane] Rift Valley Res Serv, Addis Ababa, Ethiopia. RP WoldeGabriel, G (reprint author), Los Alamos Natl Lab, Earth Environm Sci Div, POB 1663, Los Alamos, NM 87545 USA. EM wgiday@lanl.gov OI THOUVENY, Nicolas/0000-0001-6601-856X FU National Science Foundation; Institute of Geophysics and Planetary Physics at Los Alamos National Laboratory FX The National Science Foundation and the Institute of Geophysics and Planetary Physics at Los Alamos National Laboratory primarily funded the geological and paleoanthropological investigations in the past. We thank the Authority for Research and Conservation of the Cultural Heritage of the Ministry of Culture and Tourism, the Afar Regional Government, and the Afar people of the Middle Awash for permission and facilitation of the fieldwork. Many other field and laboratory workers have contributed to the data collection and analysis. Jim Aronson, one of the pioneers in geological investigations at paleoanthroplogical localities in the eastern African rift provided a thoughtful and detailed review and comments that greatly improved the manuscript. The comments of an anonymous reviewer were also very useful. Finally, we would like to thank Tim Horscroft and Pat Eriksson of the Journal of the African Earth Sciences for patiently waiting for this review paper to materialize. NR 125 TC 5 Z9 5 U1 2 U2 28 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 1464-343X J9 J AFR EARTH SCI JI J. Afr. Earth Sci. PD JAN PY 2013 VL 77 BP 41 EP 58 DI 10.1016/j.jafrearsci.2012.09.004 PG 18 WC Geosciences, Multidisciplinary SC Geology GA 052BX UT WOS:000312173800005 ER PT J AU Golan, A Ahmed, M Mebel, AM Kaiser, RI AF Golan, Amir Ahmed, Musahid Mebel, Alexander M. Kaiser, Ralf I. TI A VUV photoionization study of the multichannel reaction of phenyl radicals with 1,3-butadiene under combustion relevant conditions SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID POLYCYCLIC AROMATIC-HYDROCARBONS; SINGLE-COLLISION CONDITIONS; AB INITIO/RRKM-ME; 1,2-BUTADIENE; KINETICS; PROPYNE; INDENE; ISOMERIZATION; PYROLYSIS; ETHYLENE AB We studied the reaction of phenyl radicals (C6H5) with 1,3-butadiene (H2CCHCHCH2) exploiting a high temperature chemical reactor under combustion-like conditions (300 Torr, 873 K). The reaction products were probed in a supersonic beam by utilizing VUV radiation from the Advanced Light Source and by recording the experimental PIE curves at mass-to-charge ratios of m/z = 130 (C10H10+), 116 (C9H8+), and 104 (C8H8+). Our data suggest that the atomic hydrogen (H), methyl (CH3), and vinyl (C2H3) losses are open with estimated branching ratios of about 86 +/- 4%, 8 +/- 2%, and 6 +/- 2%, respectively. The isomer distributions were probed further by fitting the experimentally recorded PIE curves with a linear combination of the PIE curves of individual C10H10, C9H8, and C8H8 isomers. These fits indicate the formation of three C10H10 isomers (trans-1,3-butadienylbenzene, 1,4-dihydronaphthalene, 1-methylindene), three C9H8 isomers (indene, phenylallene, 1-phenyl-1-methylacetylene), and a C8H8 isomer (styrene). A comparison with results from recent crossed molecular beam studies of the 1,3-butadiene-phenyl radical reaction and electronic structure calculations suggests that trans-1,3-butadienylbenzene (130 amu), 1,4-dihydronaphthalene (130 amu), and styrene (104 amu) are reaction products formed as a consequence of a bimolecular reaction between the phenyl radical and 1,3-butadiene. 1-Methylindene (130 amu), indene (116 amu), phenylallene (116 amu), and 1-phenyl-1-methylacetylene (116 amu) are synthesized upon reaction of the phenyl radical with three C4H6 isomers: 1,2-butadiene (H2CCCH(CH3)), 1-butyne (HCCC2H5), and 2-butyne (CH3CCCH3); these C4H6 isomers can be formed from 1,3-butadiene via hydrogen atom assisted isomerization reactions or via thermal rearrangements of 1,3-butadiene involving hydrogen shifts in the high temperature chemical reactor. C1 [Kaiser, Ralf I.] Univ Hawaii Manoa, Dept Chem, Honolulu, HI 96822 USA. [Golan, Amir; Ahmed, Musahid] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. [Mebel, Alexander M.] Florida Int Univ, Dept Chem & Biochem, Miami, FL 33199 USA. RP Kaiser, RI (reprint author), Univ Hawaii Manoa, Dept Chem, Honolulu, HI 96822 USA. EM ralfk@hawaii.edu RI Ahmed, Musahid/A-8733-2009; Mebel, Alexander/A-5234-2009 FU US Department of Energy, Basic Energy Sciences [DE-FG02-03ER15411, DE-FG02-04ER15570]; Office of Science, Office of Basic Energy Sciences, of the US Department of Energy through the Chemical Sciences Division [DE-AC02-05CH11231]; 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 US Department of Energy, Basic Energy Sciences (DE-FG02-03ER15411 to the University of Hawaii and DE-FG02-04ER15570 to Florida International University). MA and AG are supported by the Office of Science, Office of Basic Energy Sciences, of the US Department of Energy under Contract No. DE-AC02-05CH11231, through the Chemical Sciences Division. 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. We thank Dr Fangtong Zhang (University of Hawaii) for his assistance with the experiments. NR 33 TC 14 Z9 14 U1 4 U2 56 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2013 VL 15 IS 1 BP 341 EP 347 DI 10.1039/c2cp42848b PG 7 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 049DW UT WOS:000311963200034 PM 23165625 ER PT J AU Bell, F Zimmerman, PM Casanova, D Goldey, M Head-Gordon, M AF Bell, Franziska Zimmerman, Paul M. Casanova, David Goldey, Matthew Head-Gordon, Martin TI Restricted active space spin-flip (RAS-SF) with arbitrary number of spin-flips SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID DENSITY-MATRIX RENORMALIZATION; COUPLED-CLUSTER THEORY; DIMENSIONAL ORGANIC FERROMAGNETS; TRANSITION-METAL-COMPLEXES; CONSISTENT WAVE-FUNCTIONS; BROKEN SYMMETRY APPROACH; QUANTUM-CHEMISTRY; CONFIGURATION-INTERACTION; BOND-BREAKING; SIZE-CONSISTENT AB The restricted active space spin-flip (RAS-SF) approach is a multistate, spin-complete, variational and size consistent method applicable to systems featuring electronic (near-) degeneracies. In contrast to CASSCF it does not involve orbital optimizations and so avoids issues such as root-flipping and state averaging. This also makes RAS-SF calculations roughly 100-1000 times faster. In this paper RAS-SF method is extended to include variable orbital active spaces and three or more spin-flips, which allows the study of polynuclear metal systems, triple bond dissociations and organic polyradicals featuring more than four unpaired electrons. Benchmark calculations on such systems are carried out and comparison to other wave-function based, multi-reference methods, such as CASSCF and DMRG yield very good agreement, provided that the same active space is employed. Where experimental values are available, RAS-SF is found to substantially underestimate the exchange coupling constants, if the minimal active space is chosen. However, the correct ground state is always obtained. Not surprisingly, inclusion of bridge orbitals into the active space can cause the magnitude of the coupling constants to increase substantially. Importantly, the ratio of exchange couplings in related systems is in much better agreement with experiment than the magnitude of the coupling. Nevertheless, the results indicate the need for the inclusion of dynamic correlation to obtain better accuracy in minimal active spaces. C1 [Bell, Franziska; Zimmerman, Paul M.; Goldey, Matthew; Head-Gordon, Martin] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. [Bell, Franziska; Zimmerman, Paul M.; Goldey, Matthew; Head-Gordon, Martin] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Casanova, David] Univ Barcelona, Dept Quim Fis, E-08028 Barcelona, Spain. [Casanova, David] Univ Barcelona, Inst Quim Teor & Computac IQTCUB, E-08028 Barcelona, Spain. RP Head-Gordon, M (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. EM m_headgordon@berkeley.edu RI Casanova, David/F-9752-2011 OI Casanova, David/0000-0002-8893-7089 FU Scientific Discovery through Advanced Computing (SciDAC) program; U.S. Department of Energy, Office of Science, Advanced Scientific Computing Research, and Basic Energy Sciences FX Support for this work was provided through the Scientific Discovery through Advanced Computing (SciDAC) program funded by the U.S. Department of Energy, Office of Science, Advanced Scientific Computing Research, and Basic Energy Sciences. NR 90 TC 24 Z9 24 U1 1 U2 39 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2013 VL 15 IS 1 BP 358 EP 366 DI 10.1039/c2cp43293e PG 9 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 049DW UT WOS:000311963200036 PM 23169047 ER PT J AU Clayton, DA McPherson, TE Pan, SL Chen, MY Dixon, DA Hu, DH AF Clayton, Daniel A. McPherson, Tyler E. Pan, Shanlin Chen, Mingyang Dixon, David A. Hu, Dehong TI Spatial and temporal variation of surface-enhanced Raman scattering at Ag nanowires in aqueous solution SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID SILVER NANOWIRE; HOT-SPOTS; SINGLE MOLECULES; SPECTROSCOPY; POLARIZATION; FILM; SPECTROELECTROCHEMISTRY; NANOPARTICLES; TRANSPARENT; ELECTRODES AB The spatial and temporal variation of local field enhanced Raman scattering (SERS) at Ag nanowires (NWs) in aqueous solution is presented for an improved understanding of the NW structure-SERS enhancement capability relationship. Crossed Ag NWs and Ag NW bundles are found to have SERS enhancement factors much higher than single Ag NWs because of the higher density of interstitials formed by strong surface plasmon coupling when the wires are close to each other. The role of the interstitials of Ag NWs is enhanced by using unpurified Ag NWs containing Ag nanoparticles or decorating the Ag NWs surface with gold nanoparticles using galvanic replacement reaction and electroless deposition methods. This leads to an improved SERS enhancement capability as compared to purified single Ag NWs. Raman imaging reveals a different temporal response of the SERS signal in aqueous solution in comparison to the photoluminescence background of Ag NWs in the absence of Raman-active molecules. Such a different temporal response can be potentially used to separate the SERS signal from the fluorescence background. The Discrete Dipole Approximation (DDA) method is used for the first time to calculate the local field intensity of two crossed and parallel Ag NWs. Heterogeneities in the SERS spatial distribution of the interstitials and their incident-light polarization dependence are illustrated by comparing the SEM image of a selected unpurified Ag NW bundle with its Raman image. C1 [Clayton, Daniel A.; McPherson, Tyler E.; Pan, Shanlin; Chen, Mingyang; Dixon, David A.] Univ Alabama, Dept Chem, Tuscaloosa, AL 35487 USA. [Hu, Dehong] Pacific NW Natl Lab, Fundamental & Computat Sci Directorate, Richland, WA 99352 USA. RP Pan, SL (reprint author), Univ Alabama, Dept Chem, Box 870336, Tuscaloosa, AL 35487 USA. EM span1@bama.ua.edu; dadixon@as.ua.edu RI Hu, Dehong/B-4650-2010 OI Hu, Dehong/0000-0002-3974-2963 FU Department of Energy [DE-SC0005392]; University of Alabama RGC award; National Science Foundation [CHE-1004098]; U.S. Department of Energy, Office of Basic Energy Sciences; Argonne National Laboratory; Robert Ramsay Fund of The University of Alabama; Department of Energy's Office of Biological and Environmental Research FX This work was supported in part by the Department of Energy under Award Number (s) DE-SC0005392 and University of Alabama 2010 RGC award. We thank Dr Yan Zhu for helping to prepare Ag NWs. T. McPherson would like to acknowledge the National Science Foundation for funding his research through the REU program at The University of Alabama (CHE-1004098). D. A. Dixon thanks the U.S. Department of Energy, Office of Basic Energy Sciences (catalysis center program), Argonne National Laboratory, and the Robert Ramsay Fund of The University of Alabama for partial support of this work. A portion of the work was 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 The Pacific Northwest National Laboratory. The Pacific Northwest National Laboratory is operated by Battelle Memorial Institute. NR 44 TC 8 Z9 8 U1 6 U2 79 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 2013 VL 15 IS 3 BP 850 EP 859 DI 10.1039/c2cp43424e PG 10 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 052RY UT WOS:000312217200017 PM 23202361 ER PT J AU Lee, L Wooldridge, P Nah, T Wilson, K Cohen, R AF Lee, Lance Wooldridge, Paul Nah, Theodora Wilson, Kevin Cohen, Ronald TI Observation of rates and products in the reaction of NO3 with submicron squalane and squalene aerosol SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID SECONDARY ORGANIC AEROSOL; GENERATING PARTICLE BEAMS; OLEIC-ACID PARTICLES; HETEROGENEOUS OXIDATION; CONTROLLED DIMENSIONS; ATMOSPHERIC AEROSOLS; AERODYNAMIC LENSES; HYDROXYL RADICALS; NOZZLE EXPANSIONS; RATE CONSTANTS AB The reactive uptake coefficients g, for nitrate radical, NO3, on similar to 100 nm diameter squalane and squalene aerosol were measured (1 atm pressure of N-2 and 293 K). For squalane, a branched alkane, gamma(NO3) of 2.8 x 10(-3) was estimated. For squalene which contains 6 double bonds, gNO3 was found to be a function of degree of oxidation with an initial value of 0.18 +/- 0.03 on fresh particles increasing to 0.82 +/- 0.11 on average of over 3 NO3 reactions per squalene molecule in the aerosol. Synchrotron VUV-ionization aerosol mass spectrometry was used to detect the particle phase oxidation products that include as many as 3 NO3 subunits added to the squalene backbone. The fraction of squalene remaining in the aerosol follows first order kinetics under oxidation, even at very high oxidation equivalents, which suggests that the matrix remains a liquid upon oxidation. Our calculation indicates a much shorter chemical lifetime for squalene-like particle with respect to NO3 than its atmospheric lifetime to deposition or wet removal. C1 [Lee, Lance; Wooldridge, Paul; Nah, Theodora; Cohen, Ronald] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Wilson, Kevin] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Cohen, R (reprint author), Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. EM rccohen@berkeley.edu RI Cohen, Ronald/A-8842-2011 OI Cohen, Ronald/0000-0001-6617-7691 FU National Science Foundation [1120076]; Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231]; Office of Energy Research, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division of the U.S. Department of Energy [DE-AC02-05CH11231] FX The Berkeley author is supported by National Science Foundation grant, award number 1120076. 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. K. R. W. and T.N. are also supported by the Director, Office of Energy Research, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. NR 44 TC 9 Z9 9 U1 2 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 2013 VL 15 IS 3 BP 882 EP 892 DI 10.1039/c2cp42500a PG 11 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 052RY UT WOS:000312217200021 PM 23202880 ER PT J AU Ileri, N Faller, R Palazoglu, A Letant, SE Tringe, JW Stroeve, P AF Ileri, Nazar Faller, Roland Palazoglu, Ahmet Letant, Sonia E. Tringe, Joseph W. Stroeve, Pieter TI Molecular transport of proteins through nanoporous membranes fabricated by interferometric lithography SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID SELF-ASSEMBLED MONOLAYERS; SILICON-NITRIDE; ANODIC ALUMINA; PORES; SIZE; MACROMOLECULES; NANOPARTICLES; SEPARATION; DIFFUSION; ARRAYS AB Millimeter sized arrays of uniformly-distributed nanopores (180-220 nm) were created in thin (200 nm) silicon nitride membranes using interferometric lithography. Molecular transport properties of the fabricated devices were investigated experimentally and compared with those of state-of-the-art polycarbonate track etched membranes. Two similarly-sized proteins, bovine serum albumin (BSA) and bovine hemoglobin (BHb), were used as permeates in the transport experiments. Up to 40 fold higher pore fluxes were achieved with unmodified silicon nitride membranes relative to thicker commercial nanoporous membranes. Similarly, in mixed protein experiments, similar to 5.0 and 1.9 fold higher BSA and BHb selectivities were obtained with fabricated thin membranes at pH 4.7 and 7.0, respectively, relative to the commercial nanoporous membranes. C1 [Ileri, Nazar; Faller, Roland; Palazoglu, Ahmet; Stroeve, Pieter] Univ Calif Davis, Davis, CA 95616 USA. [Ileri, Nazar; Letant, Sonia E.; Tringe, Joseph W.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. RP Stroeve, P (reprint author), Univ Calif Davis, Davis, CA 95616 USA. EM pstroeve@ucdavis.edu FU University of California [2007-03]; LLNL LDRD [FS-07-001]; U.S. Department of Energy by Lawrence Livermore National Laboratory [DE-AC52-07NA27344] FX This work was supported by the University of California System-wide Biotechnology Research & Education Program GREAT Training grant 2007-03 and by LLNL LDRD FS-07-001. Special thanks are expressed to Harold Levi, Saleem Zaidi and Phillipe Renaud. Parts of this work were performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344. NR 28 TC 5 Z9 5 U1 0 U2 43 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2013 VL 15 IS 3 BP 965 EP 971 DI 10.1039/c2cp43400h PG 7 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 052RY UT WOS:000312217200030 PM 23211956 ER PT J AU Studier, W AF Studier, William TI In memoriam: John Dunn, Scientist Extraordinaire (May 29, 1944-July 13, 2012): Reminiscences of John's 40 years of exhilarating scientific research at BNL SO PROTEIN EXPRESSION AND PURIFICATION LA English DT Biographical-Item C1 Brookhaven Natl Lab, Dept Biol, Upton, NY 11973 USA. RP Studier, W (reprint author), Brookhaven Natl Lab, Dept Biol, Upton, NY 11973 USA. NR 1 TC 0 Z9 0 U1 0 U2 3 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 1046-5928 J9 PROTEIN EXPRES PURIF JI Protein Expr. Purif. PD JAN PY 2013 VL 87 IS 1 BP 1 EP 2 DI 10.1016/j.pep.2012.09.005 PG 2 WC Biochemical Research Methods; Biochemistry & Molecular Biology; Biotechnology & Applied Microbiology SC Biochemistry & Molecular Biology; Biotechnology & Applied Microbiology GA 052ZG UT WOS:000312238600001 PM 23323273 ER PT J AU Koech, PK Zhang, J Kutnyakov, IV Cosimbescu, L Lee, SJ Bowden, ME Smurthwaite, TD Heldebrant, DJ AF Koech, Phillip K. Zhang, Jian Kutnyakov, Igor V. Cosimbescu, Lelia Lee, Suh-Jane Bowden, Mark E. Smurthwaite, Tricia D. Heldebrant, David J. TI Low viscosity alkanolguanidine and alkanolamidine liquids for CO2 capture SO RSC ADVANCES LA English DT Article ID IONIC LIQUIDS; SILYLATION; AMIDINES; DIAMINES; ANIONS AB Global carbon dioxide (CO2) emission is expected to increase tremendously with the shift to coal-powered plants for energy generation. Capture and sequestration of CO2 are needed to mitigate environmental effects. Solvents currently used for this are the energy-intensive aqueous amines. Here we present 10 advanced solvents called alkanolguanidines and alkanolamidines that are potentially energy-efficient CO2-capture solvents. These solvents were synthesized in 1-3 steps from commercially available materials. One alkanolamidine derived from a 1,8-diazabicyclo[5.4.0]-undec-7-ene (DBU) base core has a low vapor pressure and a high viscosity, resulting in low CO2 uptake capacity at standard temperature and pressure (STP). Three imidazoline base derived alkanolamidines were non-viscous but do not bind CO2 at STP, however, under mild pressure they effectively capture 7-10 wt%, making them suitable for high-pressure CO2 capture. Six novel alkanolguanidine molecules have low vapor pressure and low viscosity (<10 cP) which enable high CO2 uptake at STP. These compounds bind CO2 chemically via the alcohol moiety forming zwitterionic guanidinium and amidinium alkylcarbonate ionic liquids. These materials can be regenerated thermally by heating the alkylcarbonate to 75 degrees C. CO2 binding capacities of up to 12 wt% were achieved using several of these compounds at STP. Through this study we found that alkanolguanidines have low viscosity, are non-volatile, have high CO2 uptake at STP and are tolerant to water; thus we selected one compound for physical property testing. C1 [Koech, Phillip K.; Zhang, Jian; Kutnyakov, Igor V.; Cosimbescu, Lelia; Lee, Suh-Jane; Bowden, Mark E.; Smurthwaite, Tricia D.; Heldebrant, David J.] Pacific NW Natl Lab, Energy Proc & Mat Div, Richland, WA 99352 USA. RP Koech, PK (reprint author), Pacific NW Natl Lab, Energy Proc & Mat Div, Richland, WA 99352 USA. EM david.heldebrant@pnnl.gov OI Lee, Suh-Jane/0000-0002-3396-5859; Koech, Phillip/0000-0003-2996-0593 FU Pacific Northwest National Laboratory (PNNL) Directed Research and Development; U.S. Department of Energy's Office of Fossil Energy [DE-0007466] FX The authors acknowledge internal funding from Pacific Northwest National Laboratory (PNNL) Directed Research and Development and the U.S. Department of Energy's Office of Fossil Energy (Award DE-0007466) managed by the National Energy Technology Laboratory. PNNL is proudly operated by Battelle for the U.S. Department of Energy. We also thank Dr Rui Zhang for high resolution mass spectroscopy analysis. We thank Rubin J. McDougal and Louis V. Jasperson (Wiltec Research Co., Inc.) for density and vapor pressure measurements and Dale Hume (ThermTest Inc) NR 24 TC 16 Z9 16 U1 3 U2 93 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 2013 VL 3 IS 2 BP 566 EP 572 DI 10.1039/c2ra22801g PG 7 WC Chemistry, Multidisciplinary SC Chemistry GA 052KN UT WOS:000312196600037 ER PT J AU Chen, HH Grassian, VH Saraf, LV Laskin, A AF Chen, Haihan Grassian, Vicki H. Saraf, Laxmikant V. Laskin, Alexander TI Chemical imaging analysis of environmental particles using the focused ion beam/scanning electron microscopy technique: microanalysis insights into atmospheric chemistry of fly ash SO ANALYST LA English DT Article ID X-RAY-MICROANALYSIS; IRON SOLUBILITY; DUST PARTICLES; MINERAL DUST; AEROSOLS; CLIMATE; OCEAN; SEM AB Airborne fly ash from coal combustion may represent a source of bioavailable iron (Fe) in the open ocean. However, few studies have focused on Fe speciation and distribution in coal fly ash. In this study, chemical imaging of fly ash has been performed using a dual-beam focused ion beam/scanning electron microscope (FIB/SEM) system for a better understanding of how simulated atmospheric processing can modify the morphology, chemical composition and element distribution within individual particles. A novel approach has been applied for cross-sectioning fly ash particles with the FIB in order to explore element distribution within the interior of individual particles. Our results indicate that simulated atmospheric processing can cause disintegration of aluminosilicate glass, a dominant material in fly ash particles. Fe present in the inner core of fly ash spheres within the aluminosilicate phase is more easily mobilized compared with Fe oxides present as surface aggregates on the exterior of fly ash spheres. Fe dissolution depends strongly on Fe speciation in fly ash particles. The approach for preparation of a cross-sectioned specimen described here opens up new opportunities for particle microanalysis, particularly with respect to inorganic refractive materials like fly ash and mineral dust. C1 [Saraf, Laxmikant V.; Laskin, Alexander] Pacific NW Natl Lab, WR Wiley Environm Mol Sci Lab, Richland, WA 99352 USA. [Chen, Haihan; Grassian, Vicki H.] Univ Iowa, Dept Chem & Biochem Engn, Iowa City, IA 52242 USA. [Grassian, Vicki H.] Univ Iowa, Dept Chem, Iowa City, IA 52242 USA. RP Laskin, A (reprint author), Pacific NW Natl Lab, WR Wiley Environm Mol Sci Lab, Richland, WA 99352 USA. EM Alexander.Laskin@pnnl.gov RI Chen, Haihan/F-3264-2014; Laskin, Alexander/I-2574-2012 OI Chen, Haihan/0000-0001-6360-2947; Laskin, Alexander/0000-0002-7836-8417 FU National Science foundation [CHE1012037]; Chemical Imaging Initiative under the Laboratory Directed Research and Development funds of Pacific Northwest National Laboratory (PNNL); DOE's Office of Biological and Environmental Research at PNNL; U.S. Department of Energy [DE-AC06-76RLO 1830] FX The UI group acknowledges support by the National Science foundation under Grant no. CHE1012037. The PNNL group acknowledges support by the Chemical Imaging Initiative under the Laboratory Directed Research and Development funds of Pacific Northwest National Laboratory (PNNL). Any opinions, findings, and conclusions or recommendations expressed in this material are those of the authors and do not reflect the views of the funding agencies. The CCSEM/EDX analysis was performed at the William R. Wiley Environmental Molecular Sciences Laboratory, a national scientific user facility sponsored by the DOE's Office of Biological and Environmental Research and located at PNNL. PNNL is operated for the U.S. Department of Energy by Battelle Memorial Institute under Contract no. DE-AC06-76RLO 1830. NR 31 TC 9 Z9 9 U1 2 U2 80 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 0003-2654 J9 ANALYST JI Analyst PY 2013 VL 138 IS 2 BP 451 EP 460 DI 10.1039/c2an36318f PG 10 WC Chemistry, Analytical SC Chemistry GA 050SM UT WOS:000312074300010 PM 23207643 ER PT J AU Nguyen, TB Nizkorodov, SA Laskin, A Laskin, J AF Nguyen, Tran B. Nizkorodov, Sergey A. Laskin, Alexander Laskin, Julia TI An approach toward quantification of organic compounds in complex environmental samples using high-resolution electrospray ionization mass spectrometry SO ANALYTICAL METHODS LA English DT Article ID GAS-PHASE BASICITIES; PROTON AFFINITIES; ISOPRENE PHOTOOXIDATION; EFFICIENCY SCALE; ALPHA-PINENE; ESI-MS; SECONDARY; AEROSOL; MATRIX; MOLECULES AB Quantitative analysis of individual compounds in complex mixtures using high-resolution electrospray ionization mass spectrometry (HR-ESI-MS) is complicated by differences in the ionization efficiencies of analyte molecules, mainly resulting in signal suppression during ionization. However, the ability to obtain concentration estimates of compounds in environmental samples is important for data interpretation and comparison. We introduce an approach for estimating mass concentrations of analytes observed in a multicomponent mixture by HR-ESI-MS, without prior separation. The approach relies, in part, on a matrix-matched calibration of the instrument using appropriate standards added to the analyte matrix. An illustration of how the proposed calibration can be applied in practice is provided for aqueous extracts of isoprene photooxidation secondary organic aerosol, with multifunctional organic acid standards. We show that the observed ion sensitivities in ESI are positively correlated with the "adjusted mass," defined as a product of the molecular mass and the H/C ratio in the molecule (adjusted mass = H/C x molecular mass). The correlation of the observed ESI sensitivity with adjusted mass is associated with the trends of the physical and chemical properties of organic compounds that affect ionization in the positive ion mode, i.e., gas-phase basicity, polarizability, and molecular size. C1 [Nguyen, Tran B.; Nizkorodov, Sergey A.] Univ Calif Irvine, Dept Chem, Irvine, CA 92697 USA. [Laskin, Alexander] Pacific NW Natl Lab, Environm Mol Sci Lab, Richland, WA 99352 USA. [Laskin, Julia] Pacific NW Natl Lab, Chem & Mat Sci Div, Richland, WA 99352 USA. RP Nizkorodov, SA (reprint author), Univ Calif Irvine, Dept Chem, Irvine, CA 92697 USA. EM nizkorod@uci.edu; Julia.Laskin@pnnl.gov RI Laskin, Julia/H-9974-2012; Laskin, Alexander/I-2574-2012; Nizkorodov, Sergey/I-4120-2014 OI Laskin, Julia/0000-0002-4533-9644; Laskin, Alexander/0000-0002-7836-8417; Nizkorodov, Sergey/0000-0003-0891-0052 FU NSF [AGS-1227579, CHEM-0909227]; Chemical Sciences Division, Office of Basic Energy Sciences of the U.S. DOE; intramural research and development program of the W.R. Wiley Environmental Molecular Sciences Laboratory (EMSL); Office of Biological and Environmental Research of the U.S.; Battelle Memorial Institute [DE-AC06-76RL0 1830] FX The UCI group acknowledges support by the NSF grants AGS-1227579 (SAN) and CHEM-0909227 (TBN). The PNNL group acknowledges support from the Chemical Sciences Division (JL), Office of Basic Energy Sciences of the U.S. DOE, and the intramural research and development program of the W.R. Wiley Environmental Molecular Sciences Laboratory (EMSL). All HR-ESI-MS analyses were performed at EMSL - a national scientific user facility located at PNNL, and sponsored by the Office of Biological and Environmental Research of the U.S. PNNL is operated for US DOE by Battelle Memorial Institute under Contract No. DE-AC06-76RL0 1830. NR 50 TC 10 Z9 10 U1 0 U2 58 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1759-9660 J9 ANAL METHODS-UK JI Anal. Methods PY 2013 VL 5 IS 1 BP 72 EP 80 DI 10.1039/c2ay25682g PG 9 WC Chemistry, Analytical; Food Science & Technology; Spectroscopy SC Chemistry; Food Science & Technology; Spectroscopy GA 049FO UT WOS:000311968000009 ER PT J AU Waidmann, CR Pierpont, AW Batista, ER Gordon, JC Martin, RL Silks, LA West, RM Wu, RL AF Waidmann, Christopher R. Pierpont, Aaron W. Batista, Enrique R. Gordon, John C. Martin, Richard L. Silks, L. A. Pete West, Ryan M. Wu, Ruilian TI Functional group dependence of the acid catalyzed ring opening of biomass derived furan rings: an experimental and theoretical study SO CATALYSIS SCIENCE & TECHNOLOGY LA English DT Article ID SOLVATION FREE-ENERGIES; SET MODEL CHEMISTRY; TRANSPORTATION FUELS; CARBONYL-COMPOUNDS; LEVULINIC ACID; FAST PYROLYSIS; LIQUID FUELS; HARTREE-FOCK; GAS-PHASE; DERIVATIVES AB We describe studies of Bronsted acid catalyzed ring opening of substituted furans contained within biomass derived C-8- and C-9-molecules. Ring opening occurs homogeneously under relatively mild conditions of 80 degrees C using catalytic hydrochloric acid. In the case of 4-(5-methyl-2-furyl)-2-butanone (1a), the reaction proceeds to a single product in up to 92% yield after 24 hours. For 4-(2-furanyl)-2-butanone (1b) and 4-(5-hydroxymethyl)-2-furanyl-2-butanone (1c), however, multiple products are observed, illustrating the significant influence of furan ring substituents on the reactivity of this class of compounds. The generality of these reaction pathways was tested using several other similar substrates. Kinetics experiments indicate that ring opening of 1a occurs via specific acid catalysis, and computations elucidate the effect of initial protonation on the reaction pathway. Calculated pK(a) values were calibrated against experimentally measured values and are consistent with observed reactivities. Inclusion of explicit, hydrogen-bonded water molecules in addition to the SMD solvent model is necessary when studying protonation of alcohol and ketone groups. C1 [Waidmann, Christopher R.; Gordon, John C.] Los Alamos Natl Lab, Div Chem, Los Alamos, NM 87545 USA. [Pierpont, Aaron W.; Batista, Enrique R.; Martin, Richard L.] Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. [Silks, L. A. Pete; Wu, Ruilian] Los Alamos Natl Lab, Biosci Div, Los Alamos, NM 87545 USA. [West, Ryan M.] Procter & Gamble, W Chester, OH 45069 USA. RP Waidmann, CR (reprint author), Los Alamos Natl Lab, Div Chem, POB 1663, Los Alamos, NM 87545 USA. EM jgordon@lanl.gov OI Silks, Pete/0000-0002-2993-5630 FU Laboratory Directed Research and Development Program at LANL FX This work was supported by the Laboratory Directed Research and Development Program at LANL. NR 89 TC 29 Z9 33 U1 1 U2 68 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2044-4753 J9 CATAL SCI TECHNOL JI Catal. Sci. Technol. PY 2013 VL 3 IS 1 BP 106 EP 115 DI 10.1039/c2cy20395b PG 10 WC Chemistry, Physical SC Chemistry GA 049FZ UT WOS:000311969200012 ER PT J AU Netirojjanakul, C Witus, LS Behrens, CR Weng, CH Iavarone, AT Francis, MB AF Netirojjanakul, Chawita Witus, Leah S. Behrens, Christopher R. Weng, Chih-Hisang Iavarone, Anthony T. Francis, Matthew B. TI Synthetically modified Fc domains as building blocks for immunotherapy applications SO CHEMICAL SCIENCE LA English DT Article ID BIOMIMETIC TRANSAMINATION REACTION; MONOCLONAL-ANTIBODIES; PROTEIN MODIFICATION; PULMONARY DELIVERY; CANCER-THERAPY; EMERGING CLASS; BINDING-SITE; LIVE CELLS; HUMAN IGG1; APTAMERS AB Chemically based protein modification methods could provide useful strategies for the generation of antibody mimics. However, the highly complex structures of antibody domains make it exceptionally difficult to modify these proteins in a single or small number of locations. This complexity includes the presence of multiple polypeptide chains, extensive disulfide networks, and critically important glycosylation patterns, all of which must remain intact to obtain biological function. In this work, we have created novel antibody mimics by installing synthetic molecules at the N-termini of crystallizable fragment domains (Fc's) via a chemical modification approach. First, a pyridoxal 5'-phosphate (PLP) mediated N-terminal transamination reaction provided a compatible method for site-selectively installing ketones as reactive handles on Fc domains. High levels of conversion were achieved. For elaboration of the newly installed chemical handles, we used two strategies for the ligation of our desired compounds to the protein. In the first, we used alpha-effect amines to create oxime or hydrazone linkages. Alternatively, we used the ketone as a site to introduce a second reaction handle: an aniline group that can participate in a recently reported oxidative coupling reaction. The oxidative coupling provides a highly efficient ligation strategy requiring very short reaction times (two min or less) at room temperature. By combining the advantages of synthetic targeting agents (e.g. high stability, low cost, and facile and reproducible production and discovery) with the ability of Fc domains to mediate targeted cell death and extend plasma half-life, these new hybrid agents may possess the best qualities of both. As an initial proof of concept, Fc domains were functionalized with DNA aptamers. The specificity of the aptamers for binding their cellular targets was demonstrated, as was the ability of the modified Fc domains to bind to complement proteins. The full assessment of the immunological properties of these hybrid constructs is currently underway. C1 [Netirojjanakul, Chawita; Witus, Leah S.; Behrens, Christopher R.; Weng, Chih-Hisang; Iavarone, Anthony T.; Francis, Matthew B.] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Iavarone, Anthony T.] Univ Calif Berkeley, Inst QB3, Berkeley, CA 94720 USA. [Francis, Matthew B.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. RP Francis, MB (reprint author), Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. EM mbfrancis@berkeley.edu FU DOD Breast Cancer Research Program [BC016995]; HHMI International Student Research Fellowship; Abramson Graduate Scholarship; DOE CARE (California Alliance for Radiotracer Education) [DESC0002061]; UC Berkeley Chemical Biology Graduate Program [1 T32 GMO66698] FX These studies were generously supported by the DOD Breast Cancer Research Program (BC016995). CN was supported by a HHMI International Student Research Fellowship and an Abramson Graduate Scholarship. CRB was supported by DOE CARE (California Alliance for Radiotracer Education) grant DESC0002061. The UC Berkeley Chemical Biology Graduate Program (Training Grant 1 T32 GMO66698) is also acknowledged for their support of CRB and LSW. We would also like to thank Dr Michelle Farkas and Samuel Sternberg for helpful discussion. NR 57 TC 15 Z9 15 U1 1 U2 45 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2041-6520 J9 CHEM SCI JI Chem. Sci. PY 2013 VL 4 IS 1 BP 266 EP 272 DI 10.1039/c2sc21365f PG 7 WC Chemistry, Multidisciplinary SC Chemistry GA 049GT UT WOS:000311971500028 ER PT J AU Schultz, BJ Jaye, C Lysaght, PS Fischer, DA Prendergast, D Banerjee, S AF Schultz, Brian J. Jaye, Cherno Lysaght, Patrick S. Fischer, Daniel A. Prendergast, David Banerjee, Sarbajit TI On chemical bonding and electronic structure of graphene-metal contacts SO CHEMICAL SCIENCE LA English DT Article ID SPECTROSCOPY; SURFACES; MICROSCOPY; SCATTERING; DEVICES; LAYERS; FILMS AB The nature of chemical bonding at graphene-metal interfaces is intriguing from a fundamental perspective and has great relevance for contacts to novel spintronics and high-frequency electronic devices. Here, we use near-edge X-ray absorption fine structure (NEXAFS) spectroscopy in conjunction with Raman spectroscopy and first-principles density functional theory to examine chemical bonding and perturbation of the pi-electron cloud at graphene-metal interfaces. Graphene-metal bonding has been contrasted for graphene interfaced with single-crystalline metals, polycrystalline metal foils, and with evaporated metal overlayers and is seen to be strongest at the last noted interface. Strong covalent metal-d-graphene-pi hybridization and hole doping of graphene is observed upon deposition of Ni and Co metal contacts onto graphene/SiO2 and is significantly stronger for these metals in comparison to Cu. Of single-crystalline substrates, the most commensurate (111) facets exhibit the strongest interactions with the graphene lattice. First-principles electronic structure simulations, validated by direct comparison of simulated spectra with NEXAFS measurements, suggest that metal deposition induces a loss of degeneracy between the alpha- and beta-graphene sublattices and that spin-majority and spin-minority channels are distinctly coupled to graphene, contributing to splitting of the characteristic pi* resonance. Finally, the electronic structure of graphene is found to be far less perturbed by metal deposition when the p cloud is pinned to an underlying substrate; this remarkable behaviour of "sandwich" structures has been attributed to electronic accessibility of only one face of graphene and illustrates the potential for anisotropic functionalization. C1 [Schultz, Brian J.; Banerjee, Sarbajit] SUNY Buffalo, Dept Chem, Buffalo, NY 14260 USA. [Jaye, Cherno; Fischer, Daniel A.] NIST, Mat Measurement Lab, Gaithersburg, MD 20899 USA. [Lysaght, Patrick S.] SEMATECH, Front End Proc Div, Austin, TX 78741 USA. [Prendergast, David] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA. RP Banerjee, S (reprint author), SUNY Buffalo, Dept Chem, Buffalo, NY 14260 USA. EM sb244@buffalo.edu RI Foundry, Molecular/G-9968-2014 FU Office of Science, Office of Basic Energy Sciences, of the U. S. Department of Energy [DE-AC02-05CH11231] FX We acknowledge the New York State Energy Research and Development Authority for partial support of this work. Certain commercial names are presented in this manuscript for purposes of illustration and do not constitute an endorsement by NIST. Density functional theory simulations 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 U. S. Department of Energy, under Contract No. DE-AC02-05CH11231. NR 51 TC 32 Z9 32 U1 4 U2 151 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2041-6520 J9 CHEM SCI JI Chem. Sci. PY 2013 VL 4 IS 1 BP 494 EP 502 DI 10.1039/c2sc21018e PG 9 WC Chemistry, Multidisciplinary SC Chemistry GA 049GT UT WOS:000311971500059 ER PT J AU Guo, WD Lim, CJ Bi, XT Sokhansanj, S Melin, S AF Guo, Wendi Lim, C. Jim Bi, Xiaotao Sokhansanj, Shahab Melin, Staffan TI Determination of effective thermal conductivity and specific heat capacity of wood pellets SO FUEL LA English DT Article DE Effective thermal conductivity; Specific heat capacity; Moisture content; Wood pellets; Self-heating ID SOFTWOOD CHAR; TEMPERATURE; PARTICLES; PYROLYSIS; BARK AB Effective thermal conductivity and specific heat capacity are important properties for studying the self-heating during wood pellets storage. A modified line heat source within a wood pellets container was used to determine the thermal conductivity and specific heat capacity of wood pellets with moisture content ranging from 1.4% to 9% w.b. A second order partial differential equation describing transient temperature distribution within the test container was numerically solved for temporal and spatial temperatures. The difference between experimental and numerical temperatures was minimized to estimate an effective thermal conductivity and specific heat capacity for the bulk pellets. The estimated thermal conductivity ranged from 0.146 to 0.192 W/(m K) increasing with moisture content. An empirical relationship among effective thermal conductivity, moisture content and porosity was developed. The dependence of effective thermal conductivity on pellets size was negligible. The estimated specific heat capacity of pellets ranged from 1.074 to 1.253 kJ/(kg K) in the tested range. A relation between specific heat capacity and moisture content was developed for general wood pellets. (C) 2012 Elsevier Ltd. All rights reserved. C1 [Guo, Wendi; Lim, C. Jim; Bi, Xiaotao; Sokhansanj, Shahab; Melin, Staffan] Univ British Columbia, Dept Chem & Biol Engn, Vancouver, BC V6T 1Z3, Canada. [Sokhansanj, Shahab] Oak Ridge Natl Lab, Div Environm Sci, Oak Ridge, TN 37831 USA. RP Lim, CJ (reprint author), Univ British Columbia, Dept Chem & Biol Engn, Vancouver, BC V6T 1Z3, Canada. EM cjlim@chbe.ubc.ca FU Natural Sciences and Engineering Research Council of Canada (NSERC-CRD) [CRDPJ342219-06]; Wood Pellet Association of Canada [11R42500]; Office of Biomass Program of the US Department of Energy FX This research is funded in parts by the Natural Sciences and Engineering Research Council of Canada (NSERC-CRD Grant: CRDPJ342219-06); Wood Pellet Association of Canada (Grant-11R42500). We acknowledge the support from Office of Biomass Program of the US Department of Energy. NR 34 TC 20 Z9 20 U1 2 U2 30 PU ELSEVIER SCI LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, OXON, ENGLAND SN 0016-2361 EI 1873-7153 J9 FUEL JI Fuel PD JAN PY 2013 VL 103 BP 347 EP 355 DI 10.1016/j.fuel.2012.08.037 PG 9 WC Energy & Fuels; Engineering, Chemical SC Energy & Fuels; Engineering GA 048SF UT WOS:000311932200044 ER PT J AU Clarkson, CR Solano, N Bustin, RM Bustin, AMM Chalmers, GRL He, L Melnichenko, YB Radlinski, AP Blach, TP AF Clarkson, C. R. Solano, N. Bustin, R. M. Bustin, A. M. M. Chalmers, G. R. L. He, L. Melnichenko, Y. B. Radlinski, A. P. Blach, T. P. TI Pore structure characterization of North American shale gas reservoirs using USANS/SANS, gas adsorption, and mercury intrusion SO FUEL LA English DT Article DE Shale gas; Pore structure; Small-angle neutron scattering; Gas adsorption; Mercury intrusion ID ANGLE NEUTRON-SCATTERING; BITUMINOUS COAL; ROCKS; MICROSTRUCTURE; DISTRIBUTIONS; PRESSURE; POROSITY; METHANE; VOLUME; SANS AB Small-angle and ultra-small-angle neutron scattering (SANS and USANS), low-pressure adsorption (N-2 and CO2), and high-pressure mercury intrusion measurements were performed on a suite of North American shale reservoir samples providing the first ever comparison of all these techniques for characterizing the complex pore structure of shales. The techniques were used to gain insight into the nature of the pore structure including pore geometry, pore size distribution and accessible versus inaccessible porosity. Reservoir samples for analysis were taken from currently-active shale gas plays including the Barnett, Marcellus, Haynesville, Eagle Ford, Woodford, Muskwa, and Duvernay shales. Low-pressure adsorption revealed strong differences in BET surface area and pore volumes for the sample suite, consistent with variability in composition of the samples. The combination of CO2 and N-2 adsorption data allowed pore size distributions to be created for micro-meso-macroporosity up to a limit of similar to 1000 angstrom. Pore size distributions are either uni- or multi-modal. The adsorption-derived pore size distributions for some samples are inconsistent with mercury intrusion data, likely owing to a combination of grain compression during high-pressure intrusion, and the fact that mercury intrusion yields information about pore throat rather than pore body distributions. SANS/USANS scattering data indicate a fractal geometry (power-law scattering) for a wide range of pore sizes and provide evidence that nanometer-scale spatial ordering occurs in lower mesopore-micropore range for some samples, which may be associated with inter-layer spacing in clay minerals. SANS/USANS pore radius distributions were converted to pore volume distributions for direct comparison with adsorption data. For the overlap region between the two methods, the agreement is quite good. Accessible porosity in the pore size (radius) range 5 nm-10 mu m was determined for a Barnett shale sample using the contrast matching method with pressurized deuterated methane fluid. The results demonstrate that accessible porosity is pore-size dependent. (C) 2012 Elsevier Ltd. All rights reserved. C1 [Clarkson, C. R.; Solano, N.] Univ Calgary, Dept Geosci, Calgary, AB T2N 1N4, Canada. [Bustin, R. M.; Bustin, A. M. M.; Chalmers, G. R. L.] Dept Earth & Ocean Sci, Vancouver, BC V62 1Z4, Canada. [He, L.; Melnichenko, Y. B.] Oak Ridge Natl Lab, Neutron Scattering Sci Div, Oak Ridge, TN 37831 USA. [Radlinski, A. P.; Blach, T. P.] Griffith Univ, Queensland Micro & Nanotechnol Ctr, Brisbane, Qld 4111, Australia. [Radlinski, A. P.] Indiana Univ, Indiana Geol Survey, Bloomington, IN USA. RP Clarkson, CR (reprint author), Univ Calgary, Dept Geosci, 2500 Univ Dr NW, Calgary, AB T2N 1N4, Canada. EM clarksoc@ucalgary.ca OI Chalmers, Gareth/0000-0001-6648-5619; He, Lilin/0000-0002-9560-8101 FU Society of Petroleum Engineers Canada Region STAR Fellowship; Geoscience BC; Laboratory Directed Research and Development Program; Scientific User Facilities Division, Office of Basic Energy Sciences, US Department of Energy; ORNL Postdoctoral Research Associates Program; National Science Foundation [DMR-0454672] FX Chris Clarkson would like to acknowledge Encana for support of his Chair position in Unconventional Gas at the University of Calgary. Funding for Nisael Solano's work was provided in part by a Society of Petroleum Engineers Canada Region STAR Fellowship provided to Solano as well as by the sponsors of the Tight Oil Consortium, hosted at the University of Calgary.; Marc Bustin would like to acknowledge Geoscience BC for a grant provided to support this research.; The authors would also like to acknowledge D.F.R. Mildner for his help during USANS experiments. The research at Oak Ridge National Laboratory's High Flux Isotope Reactor was sponsored by the Laboratory Directed Research and Development Program and the Scientific User Facilities Division, Office of Basic Energy Sciences, US Department of Energy. This research was supported in part by the ORNL Postdoctoral Research Associates Program, administered jointly by the ORNL and the Oak Ridge Institute for Science and Education. The elements of this work utilizing the BT-5 instrument at the NCNR were supported in part by the National Science Foundation under agreement No. DMR-0454672. NR 29 TC 197 Z9 225 U1 30 U2 329 PU ELSEVIER SCI LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, OXON, ENGLAND SN 0016-2361 EI 1873-7153 J9 FUEL JI Fuel PD JAN PY 2013 VL 103 BP 606 EP 616 DI 10.1016/j.fuel.2012.06.119 PG 11 WC Energy & Fuels; Engineering, Chemical SC Energy & Fuels; Engineering GA 048SF UT WOS:000311932200076 ER PT J AU MacDonald, ME Davidson, DF Hanson, RK Pitz, WJ Mehl, M Westbrook, CK AF MacDonald, Megan E. Davidson, David F. Hanson, Ronald K. Pitz, William J. Mehl, Marco Westbrook, Charles K. TI Formulation of an RP-1 pyrolysis surrogate from shock tube measurements of fuel and ethylene time histories SO FUEL LA English DT Article DE Rocket propellant RP-1; Laser absorption; Shock tubes; Pyrolysis; Ethylene time-histories ID HIGH-TEMPERATURE STABILIZERS; SIMILAR HYDROCARBON MIXTURES; PHASE THERMAL-DECOMPOSITION; IGNITION DELAY TIMES; N-DODECANE; JET FUELS; REFERENCE COMPONENTS; REACTION-MECHANISM; AVIATION FUELS; KINETIC-MODEL AB RP-1 and ethylene time histories have been measured during RP-1 pyrolysis, allowing determination of ethylene yields and overall fuel decomposition rates for RP-1 near 20 atm and between 1050 K and 1500 K. A decomposition surrogate for RP-1 was formulated using the components n-dodecane, methylcyclohexane, and iso-cetane by targeting three decomposition characteristics of the fuel: compound class, overall fuel decomposition rate, and ethylene yield. Decomposition of this surrogate mixture was modeled using a newly developed detailed mechanism and the simulations are compared to the experimentally measured RP-1 and ethylene time histories. Comparisons between modeled and measured ethylene yields and overall fuel decomposition rates are also reported. (C) 2012 Elsevier Ltd. All rights reserved. C1 [MacDonald, Megan E.; Davidson, David F.; Hanson, Ronald K.] Stanford Univ, Stanford, CA 94305 USA. [Pitz, William J.; Mehl, Marco; Westbrook, Charles K.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. RP Davidson, DF (reprint author), Stanford Univ, Stanford, CA 94305 USA. EM dfd@stanford.edu RI Mehl, Marco/A-8506-2009 OI Mehl, Marco/0000-0002-2227-5035 FU ERC Incorporated at the Air Force Research Laboratory FX This work was supported by ERC Incorporated at the Air Force Research Laboratory, with Dr. David Campbell as program manager and Matthew Billingsley as contract monitor. Model development work by CKW, WJP and MM was supported by the U.S. Department of Energy through the Lawrence Livermore National Laboratory. These input files for the LLNL - mix model are available as Supplementary material to this publication and from the LLNL website at: https://www-pls.llnl.gov/?url=science_and_technology-chemistry-combustio n. NR 68 TC 5 Z9 5 U1 5 U2 36 PU ELSEVIER SCI LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, OXON, ENGLAND SN 0016-2361 EI 1873-7153 J9 FUEL JI Fuel PD JAN PY 2013 VL 103 BP 1051 EP 1059 DI 10.1016/j.fuel.2012.10.008 PG 9 WC Energy & Fuels; Engineering, Chemical SC Energy & Fuels; Engineering GA 048SF UT WOS:000311932200131 ER PT J AU Bruno, G Wheaton, BR Clausen, B Sisneros, T AF Bruno, Giovanni Wheaton, Bryan R. Clausen, Bjorn Sisneros, Thomas TI Microstress partitioning in porous and microcracked synthetic cordierite SO SCRIPTA MATERIALIA LA English DT Article DE Cordierite; Microstrains and stresses; Neutron diffraction; Coefficient of thermal expansion; Anisotropy ID THERMAL-EXPANSION; ELASTICITY; STRAIN AB diffraction allowed us to observe lattice strains as a function of temperature. The transfer of grain microstrain (and stress) between the main (orthorhombic) cordierite phase and the minority spinel phase could be experimentally captured and rationalized by simple stress balance equations. (C) 2012 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved. C1 [Bruno, Giovanni; Wheaton, Bryan R.] Corning Inc, S&T, Corning, NY 14831 USA. [Clausen, Bjorn] Los Alamos Natl Lab, LANSCE LC, Los Alamos, NM 87545 USA. RP Bruno, G (reprint author), Corning Inc, S&T, CMP SP FR06, Corning, NY 14831 USA. EM brunog@coming.com RI Lujan Center, LANL/G-4896-2012; Bruno, Giovanni/E-2817-2013; Clausen, Bjorn/B-3618-2015 OI Clausen, Bjorn/0000-0003-3906-846X FU Department of Energy's Office of Basic Energy Sciences; Los Alamos National Security LLC under DOE [DE-AC52-06NA25396] FX This work has benefited from the use of the Lujan Neutron Scattering Center at LANSCE, 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-AC52-06NA25396. NR 25 TC 2 Z9 2 U1 0 U2 13 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 1359-6462 J9 SCRIPTA MATER JI Scr. Mater. PD JAN PY 2013 VL 68 IS 2 BP 100 EP 103 DI 10.1016/j.scriptamat.2012.09.015 PG 4 WC Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Science & Technology - Other Topics; Materials Science; Metallurgy & Metallurgical Engineering GA 050MU UT WOS:000312058200002 ER PT J AU Zhang, RF Germann, TC Wang, J Liu, XY Beyerlein, IJ AF Zhang, R. F. Germann, T. C. Wang, J. Liu, X-Y. Beyerlein, I. J. TI Role of interface structure on the plastic response of Cu/Nb nanolaminates under shock compression: Non-equilibrium molecular dynamics simulations SO SCRIPTA MATERIALIA LA English DT Article DE Cu/Nb; Nanocomposites; Molecular dynamics; Shock compression; Dislocation nucleation ID COMPOSITES; STRENGTH; METALS; DEFORMATION; MECHANISMS AB We utilize non-equilibrium molecular dynamics simulations to reveal the dislocation processes underlying the recently observed pronounced effect of bimetal interface structures on the plastic response of Cu/Nb nanolayered composites to shock compression. Critical shock pressures to nucleate and transmit dislocations across an atomically flat interface are shown to be substantially higher than those from a faceted interface, due to atomic-level interface characteristics that cause these two types of interfaces to nucleate, absorb and transmit dislocations by significantly different mechanisms. (C) 2012 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved. C1 [Zhang, R. F.; Germann, T. C.; Beyerlein, I. J.] Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. [Wang, J.; Liu, X-Y.] Los Alamos Natl Lab, Mat Sci & Technol Div, Los Alamos, NM 87545 USA. RP Germann, TC (reprint author), Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. EM tcg@lanl.gov; irene@lanl.gov RI Beyerlein, Irene/A-4676-2011; Wang, Jian/F-2669-2012; OI Wang, Jian/0000-0001-5130-300X; Germann, Timothy/0000-0002-6813-238X FU LANL; 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] FX R.F.Z. would like to acknowledge support by a LANL Director's Postdoctoral Fellowship. I.J.B., T.C.G. and J.W. were supported 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 No. 2008LANL1026. NR 27 TC 29 Z9 29 U1 3 U2 60 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 1359-6462 J9 SCRIPTA MATER JI Scr. Mater. PD JAN PY 2013 VL 68 IS 2 BP 114 EP 117 DI 10.1016/j.scriptamat.2012.09.022 PG 4 WC Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Science & Technology - Other Topics; Materials Science; Metallurgy & Metallurgical Engineering GA 050MU UT WOS:000312058200006 ER PT J AU Wu, D Zhang, JY Huang, JC Bei, H Nieh, TG AF Wu, D. Zhang, Junyan Huang, J. C. Bei, H. Nieh, T. G. TI Grain-boundary strengthening in nanocrystalline chromium and the Hall-Petch coefficient of body-centered cubic metals SO SCRIPTA MATERIALIA LA English DT Article DE Grain boundaries; Nanocrystalline metal; Nanoindentation; Hall-Petch effect ID STRAIN-RATE SENSITIVITY; MECHANICAL-PROPERTIES; SINGLE-CRYSTALS; FLOW-STRESS; TEMPERATURE-DEPENDENCE; PLASTIC-DEFORMATION; THIN-FILMS; SIZE; BEHAVIOR; IRON AB Nanocrystalline Cr (nc-Cr) was synthesized by electrodeposition. Samples with various grain sizes (19-57 nm) were prepared by annealing the as-deposited sample. Microstructures were examined using X-ray and electron microscopy, and the mechanical properties were evaluated using nanoindentation. The strength of nc-Cr samples apparently obeyed the classical Hall-Petch relationship. It was found that hardening potency caused by grain refinement was generally higher in body-centered cubic metals than that in face-centered cubic and hexagonal close-packed metals. A possible explanation was offered. (C) 2012 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved. C1 [Wu, D.; Nieh, T. G.] Univ Tennessee, Dept Mat Sci & Engn, Knoxville, TN 37996 USA. [Zhang, Junyan] Chinese Acad Sci, Lanzhou Inst Chem Phys, State Key Lab Solid Lubricat, Lanzhou 730000, Peoples R China. [Huang, J. C.] Natl Sun Yat Sen Univ, Dept Mat & Optoelect Sci, Kaohsiung 804, Taiwan. [Bei, H.] Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN 37831 USA. RP Nieh, TG (reprint author), Univ Tennessee, Dept Mat Sci & Engn, Knoxville, TN 37996 USA. EM tnieh@utk.edu RI Bei, Hongbin/I-6576-2012; Nieh, Tai-Gang/G-5912-2011; Huang, J. /C-4276-2013; Wu, Dong/H-2817-2015; OI Nieh, Tai-Gang/0000-0002-2814-3746; Wu, Dong/0000-0001-6465-6138; Bei, Hongbin/0000-0003-0283-7990 FU National Science Foundation [DMR-0905979]; US Department of Energy, Basic Energy Sciences, Materials Sciences and Engineering Division FX This work was supported by the National Science Foundation under Contract DMR-0905979 (T.G.N. and D.W.). H.B. was supported by the US Department of Energy, Basic Energy Sciences, Materials Sciences and Engineering Division. We would like to thank Dr. Ian Liu, NSYSU, for his technical contribution of the TEM work. NR 49 TC 38 Z9 39 U1 6 U2 64 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 1359-6462 J9 SCRIPTA MATER JI Scr. Mater. PD JAN PY 2013 VL 68 IS 2 BP 118 EP 121 DI 10.1016/j.scriptamat.2012.09.025 PG 4 WC Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Science & Technology - Other Topics; Materials Science; Metallurgy & Metallurgical Engineering GA 050MU UT WOS:000312058200007 ER PT J AU Cheng, GM Yuan, H Jian, WW Xu, WZ Millett, PC Zhu, YT AF Cheng, G. M. Yuan, H. Jian, W. W. Xu, W. Z. Millett, P. C. Zhu, Y. T. TI Deformation-induced omega phase in nanocrystalline Mo SO SCRIPTA MATERIALIA LA English DT Article DE Phase transformation; Nanocrystalline; Body-centered cubic; Deformation mechanism; High-pressure torsion ID HIGH-PRESSURE TORSION; TENSILE DUCTILITY; FCC METALS; TRANSFORMATION; ALLOYS; BETA; STRENGTH; TANTALUM AB A deformation-induced hexagonal omega phase was first observed in pure nanocrystalline body-centered cubic (bcc) Mo using high-resolution transmission electron microscopy. As the grains were refined into nanometer sizes by deformation using high-pressure torsion under a pressure of similar to 4 GPa at room temperature, the omega phase formed at the grain boundaries of bcc Mo with a crystallographic relationship close to the {1 1 2}< 1 1 1 > twin orientation. Its formation was mainly attributed to the shear deformation on {1 1 2} planes in bcc Mo. Published by Elsevier Ltd. on behalf of Acta Materialia Inc. C1 [Cheng, G. M.; Yuan, H.; Jian, W. W.; Xu, W. Z.; Zhu, Y. T.] N Carolina State Univ, Dept Mat Sci & Engn, Raleigh, NC 27695 USA. [Millett, P. C.] Idaho Natl Lab, Idaho Falls, ID 83415 USA. RP Zhu, YT (reprint author), N Carolina State Univ, Dept Mat Sci & Engn, Box 7907, Raleigh, NC 27695 USA. EM ytzhu@ncsu.edu RI Zhu, Yuntian/B-3021-2008; Jian, Weiwei/F-1200-2013; Yuan, Hao/J-6139-2012; Xu, Weizong/G-3328-2014; Cheng, Guangming/F-8999-2010 OI Zhu, Yuntian/0000-0002-5961-7422; Yuan, Hao/0000-0002-4879-3420; Xu, Weizong/0000-0003-0030-8606; Cheng, Guangming/0000-0001-5852-1341 FU Laboratory Directed Research and Development Program Office of the Idaho National Laboratory FX This work was supported by the Laboratory Directed Research and Development Program Office of the Idaho National Laboratory. The authors wish to thank Dr. Dieter Wolf, whose insight and discussions with the authors inspired and initiated the current study of bcc metals. NR 28 TC 16 Z9 16 U1 6 U2 52 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 1359-6462 J9 SCRIPTA MATER JI Scr. Mater. PD JAN PY 2013 VL 68 IS 2 BP 130 EP 133 DI 10.1016/j.scriptamat.2012.09.033 PG 4 WC Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering SC Science & Technology - Other Topics; Materials Science; Metallurgy & Metallurgical Engineering GA 050MU UT WOS:000312058200010 ER PT J AU Vaska, P Cao, TY AF Vaska, Paul Cao, Tuoyu TI The State of Instrumentation for Combined Positron Emission Tomography and Magnetic Resonance Imaging SO SEMINARS IN NUCLEAR MEDICINE LA English DT Review ID TIME-OF-FLIGHT; RESOLUTION RESEARCH TOMOGRAPH; SIMULTANEOUS PET-MRI; PERFORMANCE EVALUATION; SIMULTANEOUS PET/MRI; INITIAL EXPERIENCES; OPTICAL-FIBERS; SCANNER; SYSTEM; BRAIN AB Efforts at developing instrumentation for combined positron emission tomography and magnetic resonance imaging have gained considerable momentum in recent years, propelled in particular by new photosensor technologies. Small preclinical prototype systems developed in academia have been scaled up to full-scale small-animal imagers, and commercial whole-body clinical positron emission tomography-magnetic resonance imaging systems are now available. A wide variety of architectures are reviewed, from sequential to simultaneous and preclinical to clinical. Whereas scintillators retain their role for gamma-ray conversion, light guides, photosensors, and electronic readout methods vary widely. Common themes relating to the technical challenges are presented, including electromagnetic interference and shielding. Technological directions that will likely gain in importance in the future are discussed, such as the ability to measure time of flight and depth of interaction. Semin Nucl Med 43:11-18 (C) 2013 Elsevier Inc. All rights reserved. C1 [Vaska, Paul] Brookhaven Natl Lab, Dept Med, Upton, NY 11973 USA. [Vaska, Paul; Cao, Tuoyu] SUNY Stony Brook, Dept Biomed Engn, Stony Brook, NY 11794 USA. RP Vaska, P (reprint author), Brookhaven Natl Lab, Dept Med, Bldg 490,POB 5000, Upton, NY 11973 USA. EM paul.vaska@stonybrook.edu NR 63 TC 11 Z9 12 U1 2 U2 22 PU W B SAUNDERS CO-ELSEVIER INC PI PHILADELPHIA PA 1600 JOHN F KENNEDY BOULEVARD, STE 1800, PHILADELPHIA, PA 19103-2899 USA SN 0001-2998 J9 SEMIN NUCL MED JI Semin. Nucl. Med. PD JAN PY 2013 VL 43 IS 1 BP 11 EP 18 DI 10.1053/j.semnuclmed.2012.08.003 PG 8 WC Radiology, Nuclear Medicine & Medical Imaging SC Radiology, Nuclear Medicine & Medical Imaging GA 050GT UT WOS:000312041900003 PM 23178085 ER PT J AU Murnen, HK Rosales, AM Dobrynin, AV Zuckermann, RN Segalman, RA AF Murnen, Hannah K. Rosales, Adrianne M. Dobrynin, Andrey V. Zuckermann, Ronald N. Segalman, Rachel A. TI Persistence length of polyelectrolytes with precisely located charges SO SOFT MATTER LA English DT Article ID X-RAY-SCATTERING; ANGLE NEUTRON-SCATTERING; EXCLUDED-VOLUME; LIGHT-SCATTERING; IONIC-STRENGTH; CONJUGATED POLYELECTROLYTE; COUNTERION CONDENSATION; COLLIGATIVE PROPERTIES; INTRINSIC-VISCOSITY; AQUEOUS-SOLUTIONS AB The conformation of polyelectrolytes in aqueous salt solutions is closely related to their self-assembly properties. In particular, the persistence length has a large impact on how the chain can arrange itself. In this work, biomimetic poly N-substituted glycines (polypeptoids) have been designed to position charged side chains at precise distances from each other to elucidate the relationship between the spacing of the charges along the backbone, the ionic strength, and the persistence length. Using small angle neutron scattering (SANS), it is shown that at low ionic strength, polypeptoids with charged groups located closer to each other along the polymer backbone are stiffer than those with the charged groups spaced further apart. At high ionic strength, the total persistence length decreases for both macromolecules because the electrostatic repulsions between ionized groups are screened. The measured persistence lengths were compared to those calculated using a discrete chain model with bending rigidity, and it is shown that the electrostatic persistence length scales quadratically with the Debye screening length. It is also shown that the bare persistence length of a molecule with alternating ionizable and hydrophilic groups is larger than that of a molecule containing 100% ionizable groups. This difference can be attributed to the longer hydrophilic side chains that may induce local chain stiffening. C1 [Murnen, Hannah K.; Rosales, Adrianne M.; Segalman, Rachel A.] Univ Calif Berkeley, Dept Chem & Biomol Engn, Berkeley, CA 94720 USA. [Dobrynin, Andrey V.] Univ Connecticut, Inst Mat Sci, Storrs, CT 06269 USA. [Zuckermann, Ronald N.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA. RP Segalman, RA (reprint author), Univ Calif Berkeley, Dept Chem & Biomol Engn, Berkeley, CA 94720 USA. EM segalman@berkeley.edu RI Dobrynin, Andrey/B-9472-2013; Zuckermann, Ronald/A-7606-2014; Foundry, Molecular/G-9968-2014; OI Dobrynin, Andrey/0000-0002-6484-7409; Zuckermann, Ronald/0000-0002-3055-8860; Segalman, Rachel/0000-0002-4292-5103 FU Office of Naval Research; National Science Foundation [DMR-0454672]; Department of Defense; Office of Science, Office of Basic Energy Sciences, U.S. Department of Energy [DE-AC02-05CH11231]; Office of Biological and Environmental Research; DOE [DE-AC05-00OR22725] FX We gratefully acknowledge funding from the Office of Naval Research via a Presidential Early Career Award in Science and Engineering. A. M. R. and H. K. M also gratefully acknowledge the National Science Foundation and the Department of Defense for graduate fellowships (respectively). Polypeptoid synthesis and associated chemical characterization were performed at the Molecular Foundry, a Lawrence Berkeley National Laboratory user facility supported by the Office of Science, Office of Basic Energy Sciences, U.S. Department of Energy, under Contract DE-AC02-05CH11231. A portion of the neutron scattering in this work is based on activities at the NIST Center for Neutron Research, which is supported in part by the National Science Foundation under Agreement no. DMR-0454672. Certain trade names and company products are identified to adequately specify the experimental procedure. In no case does such identification imply recommendation or endorsement by the National Institute of Standards and Technology, nor does it imply that the products are necessarily best for the purpose. The authors thank Dr Steven Kline for assistance on SANS data collection. A portion of this research was also performed at Oak Ridge National Laboratory. The authors thank Dr Volker S. Urban at Oak Ridge National Laboratory for assistance on SANS data collection. The SANS studies at Oak Ridge National Laboratory's Center for Structural Molecular Biology were supported by the Office of Biological and Environmental Research, using facilities supported by the DOE, managed by UT-Battelle, LLC, under Contract no. DE-AC05-00OR22725. We also would like to thank Dr J.-M. Carrillo for help with data fitting. NR 63 TC 13 Z9 13 U1 0 U2 79 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1744-683X J9 SOFT MATTER JI Soft Matter PY 2013 VL 9 IS 1 BP 90 EP 98 DI 10.1039/c2sm26849c PG 9 WC Chemistry, Physical; Materials Science, Multidisciplinary; Physics, Multidisciplinary; Polymer Science SC Chemistry; Materials Science; Physics; Polymer Science GA 049EF UT WOS:000311964200010 ER PT J AU Zhuk, A Xu, L Ankner, JF Sukhishvili, SA AF Zhuk, Aliaksandr Xu, Li Ankner, John F. Sukhishvili, Svetlana A. TI Selective water uptake within micelle-containing layer-by-layer films of various architectures: a neutron reflectometry study SO SOFT MATTER LA English DT Article ID POLYELECTROLYTE MULTILAYERS; BLOCK-COPOLYMER; WEAK POLYELECTROLYTES; OPTICAL-PROPERTIES; SWELLING BEHAVIOR; THIN-FILMS; REFLECTIVITY; SURFACES; RELEASE AB Swelling of micelle-containing layer-by-layer (LbL) films of various architectures has been studied by neutron reflectometry (NR). Multilayers of the first type were constructed using poly(2-(dimethylamino) ethyl methacrylate)-block-poly(N-isopropylacrylamide) (PNIPAM-b-PDMA) block copolymer micelles (BCMs) alternately assembled with poly(4-styrene sulfonate) (PSS). NR data showed that the films maintained their layered structure, but deuterated PSS (dPSS), deposited within every 5th layer as a marker, was highly interdiffused into neighboring layers. In situ NR measurements demonstrated that the films swelled homogeneously by similar to 35% in an aqueous environment. The second type of multilayer contained three zones: bottom and top stacks consisting of PDMA/dPSS homopolymer assemblies, and BCMs deposited in the middle stack as (BCM/dPSS)(n), where n is the number of deposition cycles, equal to 1 or 2. The individual micellar layer deposited in a single deposition step (n = 1) only partially covered the surface, whereas a complete layer of micelles was achieved after two deposition cycles. In situ NR study of these stacked films revealed different degrees of water uptake by film internal strata. While layers of assembled micelles took up similar to 38% water by volume when dry films were exposed to an aqueous environment at 25 degrees C, the bottom homopolymer stack was able to take up only 11-20% water. In addition, the film architecture and the degree of surface coverage by BCMs were found to be important factors enabling the study of selective swelling of film strata. NR-enabled observations of selective swelling of assembled amphiphilic BCMs allow one to correlate film swelling on the nanoscale with internal structure, and present a powerful approach for future studies of BCM-containing systems, which are useful in actuation, sensing, and controlled delivery applications. C1 [Ankner, John F.] Oak Ridge Natl Lab, Spallat Neutron Source, Oak Ridge, TN 37831 USA. [Zhuk, Aliaksandr; Xu, Li; Sukhishvili, Svetlana A.] Stevens Inst Technol, Dept Chem Chem Biol & Biochem Engn, Hoboken, NJ 07030 USA. RP Ankner, JF (reprint author), Oak Ridge Natl Lab, Spallat Neutron Source, Oak Ridge, TN 37831 USA. EM ssukhish@stevens.edu OI Ankner, John/0000-0002-6737-5718 FU National Science Foundation [DMR-0906474] FX This work was supported by the National Science Foundation under Award DMR-0906474. NR 37 TC 5 Z9 6 U1 0 U2 26 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1744-683X J9 SOFT MATTER JI Soft Matter PY 2013 VL 9 IS 2 BP 410 EP 417 DI 10.1039/c2sm26583d PG 8 WC Chemistry, Physical; Materials Science, Multidisciplinary; Physics, Multidisciplinary; Polymer Science SC Chemistry; Materials Science; Physics; Polymer Science GA 049EK UT WOS:000311964800009 ER PT S AU del Rio, MS Bianchi, D Pikuz, TA Faenov, AY Pikuz, SA Delgado-Aparicio, L Pablant, N Bitter, M Hill, K AF del Rio, M. Sanchez Bianchi, D. Pikuz, T. A. Faenov, A. Ya Pikuz, S. A., Jr. Delgado-Aparicio, L. Pablant, N. Bitter, M. Hill, K. BE Susini, J Dumas, P TI Stigmatic X-ray imaging using a single spherical Laue crystal SO 11TH INTERNATIONAL CONFERENCE ON SYNCHROTRON RADIATION INSTRUMENTATION (SRI 2012) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 11th International Conference on Synchrotron Radiation Instrumentation (SRI) CY JUL 09-13, 2012 CL Lyon, FRANCE SP ESRF, SOLEIL ID OPTICS AB We propose a crystal configuration using a single Laue spherical crystal for imaging applications. A crystal in Laue geometry set to focus a divergent beam in the meridional (diffraction) plane, but does not focus in the sagittal plane. A transmission object placed in the beam is imaged with different horizontal and vertical aspect ratio, but it is possible to find a configuration with similar aspect ratio. This system is studied using ray tracing, which permit to reproduce preliminary experimental data [1]. The concept of a stigmatic focusing by a single optical element may have applications in imaging, like in transmission microscopy or for hard X-ray backlighting and self-imaging in high energy density plasma experiments. Inertial confinement fusion experiments and large tokamak projects such as ITER may benefit from this optical configuration. C1 [del Rio, M. Sanchez] European Synchrotron Radiat Facil, BP 220, F-38043 Grenoble, France. [Bianchi, D.] Vienna Univ Technol, A-1040 Vienna, Austria. [Faenov, A. Ya] Japan Atom Energy Agcy, Quantum Beam Sci Directorate, Kyoto, Kizugawa 6190215, Japan. [Pikuz, T. A.; Faenov, A. Ya; Pikuz, S. A., Jr.] Russian Acad Sci, Joint Inst High Temp, Moscow 125412, Russia. [Delgado-Aparicio, L.; Pablant, N.; Bitter, M.; Hill, K.] Princeton Plasma Phys Lab, Princeton, NJ 08543 USA. RP del Rio, MS (reprint author), European Synchrotron Radiat Facil, BP 220, F-38043 Grenoble, France. EM srio@esrf.eu RI Pikuz, Sergey/F-7768-2014 OI Pikuz, Sergey/0000-0003-2529-1142 NR 5 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 2013 VL 425 AR UNSP 192021 DI 10.1088/1742-6596/425/19/192021 PG 4 WC Instruments & Instrumentation; Physics, Applied; Physics, Multidisciplinary SC Instruments & Instrumentation; Physics GA BFL51 UT WOS:000320403700266 ER PT S AU Abercrombie, RK Schlicher, BG Sheldon, FT AF Abercrombie, Robert K. Schlicher, Bob G. Sheldon, Frederick T. BE Gorraiz, J Schiebel, E Gumpenberger, C Horlesberger, M Moed, H TI ANALYSIS OF SEARCH RESULTS FOR THE CLARIFICATION AND IDENTIFICATION OF TECHNOLOGY EMERGENCE (AR-CITE) SO 14TH INTERNATIONAL SOCIETY OF SCIENTOMETRICS AND INFORMETRICS CONFERENCE (ISSI) SE Proceedings of the International Conference on Scientometrics and Informetrics LA English DT Proceedings Paper CT 14th International-Society-of-Scientometrics-and-Informetrics Conference (ISSI) CY JUL 15-20, 2013 CL Vienna, AUSTRIA SP Int Soc Sceintometr & Infometr, ASIS & T, Elsevier B V, EBSCO Informat Serv, Fed Minist Sci & Res, Fed Minist Transport Innovat & Technol, Informat Assistant Verein Informat Management, ORCID, Sci Metrix R & D Reports, Swets Informat Serv, Thomson Reuters, ZSI - Ctr Social Innovat C1 [Abercrombie, Robert K.; Schlicher, Bob G.; Sheldon, Frederick T.] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. RP Abercrombie, RK (reprint author), Oak Ridge Natl Lab, 1 Bethel Valley Rd, Oak Ridge, TN 37831 USA. EM abercrombier@ornl.gov; schlicherbg@ornl.gov; sheldonft@ornl.gov OI Abercrombie, Robert/0000-0003-0949-4070; Sheldon, Frederick/0000-0003-1241-2750 NR 2 TC 0 Z9 0 U1 0 U2 0 PU INT SOC SCIENTOMETRICS & INFORMETRICS-ISSI PI LEUVEN PA KATHOLIEKE UNIV LEUVEN, FACULTEIT E T E W, DEKENSTRAAT 2, LEUVEN, B-3000, BELGIUM SN 2175-1935 BN 978-3-200-03135-7 J9 PRO INT CONF SCI INF PY 2013 BP 1854 EP 1856 PG 3 WC Information Science & Library Science SC Information Science & Library Science GA BC6IG UT WOS:000353961700147 ER PT S AU Ahrenkiel, RK Feldman, A Lehman, J Johnston, SW AF Ahrenkiel, R. K. Feldman, A. Lehman, J. Johnston, S. W. GP IEEE TI Novel Free-Carrier Pump-Probe Analysis of Carrier Transport in Semiconductors SO 2012 IEEE 38TH PHOTOVOLTAIC SPECIALISTS CONFERENCE (PVSC), VOL 2 SE IEEE Photovoltaic Specialists Conference LA English DT Proceedings Paper CT 38th IEEE Photovoltaic Specialists Conference (PVSC) CY JUN 03-08, 2012 CL Austin, TX SP IEEE, IEEE Electron Devides Soc (EDS), IEEE Photon Soc, IEEE Power & Energy Soc (PES), HelioVolt Corp, SunShot, US Dept Energy DE Charge-carrier lifetime; free carrier absorption; photoconductive decay AB We have developed a pump-probe configuration to measure the carrier lifetime using the transient free-carrier density. The free-carrier absorption varies as lambda(2)Delta n/mu, where lambda is 10.6 mu m in this paper. We measure the transient photoconductive decay that is proportional to Delta n * mu. The data product gives Delta alpha * Delta sigma similar to lambda(2) Delta n(t)(2). The mobility variation is nullified by multiplying the data from the two parallel measurements. From the product data, both Delta n(t) and mu(Delta n) can be determined. A large increase in Delta alpha and decrease in mu are observed and caused by space-charge effects in regions of high injection. These data show the unexpected and remarkable result that the lifetime is relatively constant up to an injection level of about three times the doping level. However, the mobility decreases by about a factor of six over the same injection range. C1 [Ahrenkiel, R. K.; Feldman, A.] Colorado Sch Mines, Golden, CO 80401 USA. [Ahrenkiel, R. K.; Johnston, S. W.] Natl Renewable Energy Lab, Golden, CO 80402 USA. [Feldman, A.; Lehman, J.] NIST, Boulder, CO 80302 USA. RP Ahrenkiel, RK (reprint author), Colorado Sch Mines, Golden, CO 80401 USA. EM rahren@mac.com; ari1127@gmail.com; lehman@boulder.nist.gov; steve.johnston@nrel.gov NR 7 TC 0 Z9 0 U1 0 U2 0 PU IEEE PI NEW YORK PA 345 E 47TH ST, NEW YORK, NY 10017 USA SN 0160-8371 J9 IEEE PHOT SPEC CONF PY 2013 DI 10.1109/JPHOTOV.2012.2215581 PG 5 WC Energy & Fuels; Engineering, Electrical & Electronic SC Energy & Fuels; Engineering GA BC7HM UT WOS:000354881800025 ER PT S AU Ahsan, N Miyashita, N Islam, MM Yu, KM Walukiewicz, W Okada, Y AF Ahsan, Nazmul Miyashita, Naoya Islam, Muhammad M. Yu, Kin Man Walukiewicz, Wladek Okada, Yoshitaka GP IEEE TI Effect of Sb on GaNAs Intermediate Band Solar Cells SO 2012 IEEE 38TH PHOTOVOLTAIC SPECIALISTS CONFERENCE (PVSC), VOL 2 SE IEEE Photovoltaic Specialists Conference LA English DT Proceedings Paper CT 38th IEEE Photovoltaic Specialists Conference (PVSC) CY JUN 03-08, 2012 CL Austin, TX SP IEEE, IEEE Electron Devides Soc (EDS), IEEE Photon Soc, IEEE Power & Energy Soc (PES), HelioVolt Corp, SunShot, US Dept Energy DE Intermediate band solar cell; dilute nitride; two-step photon excitation; molecular beam epitaxy ID EFFICIENCY; LASERS AB We present a comparative study on the material properties and two photon excitation (TPE) experiments involving three bands between a GaNAs and a GaNAsSb absorber designed for intermediate band solar cells. The absorber layers were sandwiched between p-AIGaAs emitter layers and n-AIGaAs IB barrier layers. This permits production of above the bandgap electron-hole pairs by TPE involving two subband photons with the intermediate band as the stepping stone. A recovery in the carrier population in the intermediate band of the GaNAsSb absorber was realized due to an improved material quality. An enhancement in the photocurrent production due to TPE, and an associated improvement in the open circuit voltage were observed. C1 [Ahsan, Nazmul; Miyashita, Naoya; Islam, Muhammad M.; Okada, Yoshitaka] Univ Tokyo, Res Ctr Adv Sci & Technol, Tokyo 1538904, Japan. [Yu, Kin Man; Walukiewicz, Wladek] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. RP Ahsan, N (reprint author), Univ Tokyo, Res Ctr Adv Sci & Technol, Tokyo 1538904, Japan. EM ahsan@mbe.rcast.u-tokyo.ac.jp; miyashita@mbe.rcast.u-tokyo.ac.jp; monirul@mbe.rcast.u-tokyo.ac.jp; KMYu@lbl.gov; W_Walukiewicz@lbl.gov; okada@mbe.rcast.u-tokyo.ac.jp NR 25 TC 0 Z9 0 U1 0 U2 1 PU IEEE PI NEW YORK PA 345 E 47TH ST, NEW YORK, NY 10017 USA SN 0160-8371 J9 IEEE PHOT SPEC CONF PY 2013 PG 8 WC Energy & Fuels; Engineering, Electrical & Electronic SC Energy & Fuels; Engineering GA BC7HM UT WOS:000354881800026 ER PT S AU Deceglie, MG Ferry, VE Alivisatos, AP Atwater, HA AF Deceglie, Michael G. Ferry, Vivian E. Alivisatos, A. Paul Atwater, Harry A. GP IEEE TI Accounting for Localized Defects in the Optoelectronic Design of Thin-Film Solar Cells SO 2012 IEEE 38TH PHOTOVOLTAIC SPECIALISTS CONFERENCE (PVSC), VOL 2 SE IEEE Photovoltaic Specialists Conference LA English DT Proceedings Paper CT 38th IEEE Photovoltaic Specialists Conference (PVSC) CY JUN 03-08, 2012 CL Austin, TX SP IEEE, IEEE Electron Devides Soc (EDS), IEEE Photon Soc, IEEE Power & Energy Soc (PES), HelioVolt Corp, SunShot, US Dept Energy DE Light trapping; plasmon; simulation; thin-film solar cell ID OPEN-CIRCUIT VOLTAGE; SURFACE-MORPHOLOGY; PHOTONIC CRYSTAL; ABSORPTION; EFFICIENCY; DEVICES AB Controlled nanostructuring of thin-film solar cells offers a promising route toward increased efficiency through improved light trapping. Many such light trapping designs involve structuring of the active region itself. Optimization of these designs is aided by the use of computer simulations that account for both the optics and electronics of the device. We describe such a simulation-based approach that accounts for experimental trade-offs between high-aspect ratio structuring and electronic material quality. Our model explicitly accounts for localized regions of degraded material quality that is induced by light trapping structures in n-i-p a-Si: H solar cells. We find that the geometry of the defects couples to the geometry of light absorption profiles in the active region and that this coupling impacts the spectral response of the device. Our approach yields insights into the nanoscale device physics that is associated with localized geometry-induced defects and provides a framework for full optoelectronic optimization. C1 [Deceglie, Michael G.; Atwater, Harry A.] CALTECH, Thomas J Watson Lab Appl Phys, Pasadena, CA 91125 USA. [Ferry, Vivian E.; Alivisatos, A. Paul] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. [Ferry, Vivian E.; Alivisatos, A. Paul] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. RP Deceglie, MG (reprint author), CALTECH, Thomas J Watson Lab Appl Phys, Pasadena, CA 91125 USA. EM deceglie@caltech.edu; veferry@lbl.gov; apalivisatos@lbl.gov; haa@caltech.edu NR 34 TC 0 Z9 0 U1 0 U2 1 PU IEEE PI NEW YORK PA 345 E 47TH ST, NEW YORK, NY 10017 USA SN 0160-8371 J9 IEEE PHOT SPEC CONF PY 2013 DI 10.1109/JPHOTOV.2013.2240764 PG 6 WC Energy & Fuels; Engineering, Electrical & Electronic SC Energy & Fuels; Engineering GA BC7HM UT WOS:000354881800042 ER EF