FN Thomson Reuters Web of Science™ VR 1.0 PT S AU Pan, YS De Carlo, F AF Pan, Yongsheng De Carlo, Francesco BE Nishikawa, RM Whiting, BR Hoeschen, C TI A New Padding Scheme for Local Tomograpy in Tomographic Microscopy SO MEDICAL IMAGING 2013: PHYSICS OF MEDICAL IMAGING SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Medical Imaging - Physics of Medical Imaging CY FEB 11-14, 2013 CL Lake Buena Vista, FL SP SPIE, Aeroflex Inc, Univ Cent Florida, CREOL Coll Opt & Photon, DQE Instruments Inc, Medtronic Inc, PIXELTEQ DE Tomographic microscopy; local tomography; boundary-value padding; zero-value padding AB Tomographic microscopy using synchrotron radiation provides high-resolution structure details on the scale of microns. The field of view (FOV) of the microscopy system, however, is usually limited by the detector size. For example, a typical CCD camera used for data acquisition is of size 2048 by 2048. In many cases this CCD camera is not large enough to provide complete information required for accurate reconstruction, and the local tomography problem hereby arises. On the other hand, the huge dataset generated by tomographic microscopy asks for a highly efficient solution with no a priori information necessary. A new padding scheme is therefore proposed for the local tomography issue. It first pads the projection data using the boundary value inside the FOV, which is specified by the detector size, followed by a zero-value padding to 1.5 times the FOV length. The boundary-value padding removes the energy deposition and cupping artifact in reconstruction results from local tomography, while the zero-value padding reduces the drift of the intensity values caused by fully boundary padding. The combination of two padding schemes keeps advantages of fully zero-value padding and fully boundary-value padding, while avoiding their disadvantages. Quantitative analysis using synthetic data shows that the proposed method outperforms fully zero-value padding and fully boundary-value padding in terms of accuracy and ease for post processing. Experimental results for real data are also provided to demonstrate the effectiveness of the proposed method. C1 [Pan, Yongsheng; De Carlo, Francesco] Argonne Natl Lab, Xray Sci Div, Adv Photon Source, Argonne, IL 60439 USA. RP Pan, YS (reprint author), Argonne Natl Lab, Xray Sci Div, Adv Photon Source, 2-BM B,9700 South Cass Ave, Argonne, IL 60439 USA. NR 2 TC 0 Z9 0 U1 0 U2 0 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9442-9 J9 PROC SPIE PY 2013 VL 8668 AR 86683B DI 10.1117/12.2001550 PG 6 WC Optics; Physics, Applied; Radiology, Nuclear Medicine & Medical Imaging SC Optics; Physics; Radiology, Nuclear Medicine & Medical Imaging GA BFZ77 UT WOS:000322002700112 ER PT J AU Wang, WC Chen, SY Glans, PA Guo, JH Chen, RJ Fong, KW Chen, CL Gloter, A Chang, CL Chan, TS Chen, JM Lee, JF Dong, CL AF Wang, Wei-Cheng Chen, Shih-Yun Glans, Per-Anders Guo, Jinghua Chen, Ren-Jie Fong, Kang-Wei Chen, Chi-Liang Gloter, Alexandre Chang, Ching-Lin Chan, Ting-Shan Chen, Jin-Ming Lee, Jyh-Fu Dong, Chung-Li TI Towards understanding the electronic structure of Fe-doped CeO2 nanoparticles with X-ray spectroscopy SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID ROOM-TEMPERATURE FERROMAGNETISM; CERIUM OXIDE; OXYGEN VACANCY; OXIDATION; NANOSTRUCTURES; SEMICONDUCTORS; CHEMISTRY; STATES; MODEL AB This study reports on the electronic structure of Fe-doped CeO2 nanoparticles (NPs), determined by coupled X-ray absorption spectroscopy and X-ray emission spectroscopy. A comparison of the local electronic structure around the Ce site with that around the Fe site indicates that the Fe substitutes for the Ce. The oxygen K-edge spectra that originated from the hybridization between cerium 4f and oxygen 2p states are sensitive to the oxidation state and depend strongly on the concentration of Fe doping. The Ce M-4,M-5-edges and the Fe L-2,L-3-edges reveal the variations of the charge states of Ce and Fe upon doping, respectively. The band gap is further obtained from the combined absorption-emission spectrum and decreased upon Fe doping, implying Fe doping introduces vacancies. The oxygen vacancies are induced by Fe doping and the spectrum reveals the charge transfer between Fe and Ce. Fe3+ doping has two major effects on the formation of ferromagnetism in CeO2 nanoparticles. The first, at an Fe content of below 5%, is that the formation of Fe3+-Vo-Ce3+ introduces oxygen deficiencies favoring ferromagnetism. The other, at an Fe content of over 5%, is the formation of Fe3+-Vo-Fe3+, which favors antiferromagnetism, reducing the Ms. The defect structures Fe3+-Vo-Ce3+ and Fe3+-Vo-Fe3+ are crucial to the magnetism in these NPs and the change in Ms can be described as the effect of competitive interactions of magnetic polarons and paired ions. C1 [Wang, Wei-Cheng; Chang, Ching-Lin] Tamkang Univ, Dept Phys, Tamsui 25137, Taiwan. [Wang, Wei-Cheng; Glans, Per-Anders; Guo, Jinghua] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. [Chen, Shih-Yun; Chen, Ren-Jie; Fong, Kang-Wei] Natl Taiwan Univ Sci & Technol, Dept Mat Sci & Engn, Taipei, Taiwan. [Chen, Ren-Jie; Chan, Ting-Shan; Chen, Jin-Ming; Lee, Jyh-Fu; Dong, Chung-Li] Natl Synchrotron Radiat Res Ctr, Hsinchu 30076, Taiwan. [Chen, Chi-Liang] Acad Sinica, Inst Phys, Taipei 11529, Taiwan. [Gloter, Alexandre] Univ Paris 11, CNRS, Phys Solides Lab, UMR 8502, F-91405 Orsay, France. RP Chang, CL (reprint author), Tamkang Univ, Dept Phys, Tamsui 25137, Taiwan. EM clchang@mail.tku.edu.tw; dong.cl@nsrrc.org.tw RI Glans, Per-Anders/G-8674-2016; OI Gloter, Alexandre/0000-0002-4813-3799 FU National Science Council of Taiwan [NSC 100-2911-I-213-501-MY2, NSC 101-2112-M-213-004-MY3, NSC 100-2112-M-032-004]; Office of Science, Office of Basic Energy Sciences, of the Department of Energy [DE-AC02-05CH11231] FX This work was supported by the National Science Council of Taiwan under contracts NSC 100-2911-I-213-501-MY2 (C.L.D.), NSC 101-2112-M-213-004-MY3 (C.L.D.), and NSC 100-2112-M-032-004 (C.L.C.). The wok at the ALS was supported by the Director, Office of Science, Office of Basic Energy Sciences, of the Department of Energy under Contract No. DE-AC02-05CH11231. NR 41 TC 15 Z9 15 U1 4 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 35 BP 14701 EP 14707 DI 10.1039/c3cp52054d PG 7 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 202EQ UT WOS:000323196800017 PM 23900724 ER PT J AU Fu, Q Yao, YX Guo, XG Wei, MM Ning, YX Liu, HY Yang, F Liu, Z Bao, XH AF Fu, Qiang Yao, Yunxi Guo, Xiaoguang Wei, Mingming Ning, Yanxiao Liu, Hongyang Yang, Fan Liu, Zhi Bao, Xinhe TI Reversible structural transformation of FeOx nanostructures on Pt under cycling redox conditions and its effect on oxidation catalysis SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID TEMPERATURE CO OXIDATION; OXIDE-FILMS; PHOTOELECTRON-SPECTROSCOPY; FERROUS CENTERS; PT(111) SURFACE; IN-SITU; NANOPARTICLES; CHEMISTRY; AU(111); GROWTH AB Understanding dynamic changes of catalytically active nanostructures under reaction conditions is a pivotal challenge in catalysis research, which has been extensively addressed in metal nanoparticles but is less explored in supported oxide nanocatalysts. Here, structural changes of iron oxide (FeOx) nanostructures supported on Pt in a gaseous environment were examined by scanning tunneling microscopy, ambient pressure X-ray photoelectron spectroscopy, and in situ X-ray absorption spectroscopy using both model systems and real catalysts. O-Fe (FeO) bilayer nanostructures can be stabilized on Pt surfaces in reductive environments such as vacuum conditions and H-2-rich reaction gas, which are highly active for low temperature CO oxidation. In contrast, exposure to H-2-free oxidative gases produces a less active O-Fe-O (FeO2) trilayer structure. Reversible transformation between the FeO bilayer and FeO2 trilayer structures can be achieved under alternating reduction and oxidation conditions, leading to oscillation in the catalytic oxidation performance. C1 [Fu, Qiang; Yao, Yunxi; Guo, Xiaoguang; Wei, Mingming; Ning, Yanxiao; Liu, Hongyang; Yang, Fan; Bao, Xinhe] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China. [Liu, Hongyang] Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China. [Liu, Zhi] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. RP Fu, Q (reprint author), Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China. EM qfu@dicp.ac.cn; xhbao@dicp.ac.cn RI Yao, Yunxi/F-3451-2013; li, haobo/P-5373-2014; Liu, Zhi/B-3642-2009; Fu, Qiang/E-7109-2015; YANG, FAN/J-2706-2012 OI Yao, Yunxi/0000-0002-0814-6675; li, haobo/0000-0002-9215-3754; Liu, Zhi/0000-0002-8973-6561; Fu, Qiang/0000-0001-5316-6758; YANG, FAN/0000-0002-1406-9717 FU National Natural Science Foundation of China [21222305, 11079005, 20923001]; Ministry of Science and Technology of China [2011CBA00503, 2013CB933100]; Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231] FX This work was financially supported by the National Natural Science Foundation of China (No. 21222305, 11079005, and 20923001), and Ministry of Science and Technology of China (No. 2011CBA00503, and 2013CB933100). We acknowledge the fruitful discussions with Prof. Ding Ma and Prof. Weixue Li. The Advanced Light Source is supported by the Director, Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. NR 45 TC 20 Z9 20 U1 6 U2 97 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 35 BP 14708 EP 14714 DI 10.1039/c3cp52587b PG 7 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 202EQ UT WOS:000323196800018 PM 23900259 ER PT J AU Pilli, SK Janarthanan, R Deutsch, TG Furtak, TE Brown, LD Turner, JA Herring, AM AF Pilli, Satyananda Kishore Janarthanan, Rajeswari Deutsch, Todd G. Furtak, Thomas E. Brown, Logan D. Turner, John A. Herring, Andrew M. TI Efficient photoelectrochemical water oxidation over cobalt-phosphate (Co-Pi) catalyst modified BiVO4/1D-WO3 heterojunction electrodes SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID OXYGEN-EVOLVING CATALYST; TUNGSTEN TRIOXIDE; VISIBLE-LIGHT; ENERGY FUTURE; SOLAR-ENERGY; HYDROGEN; WO3; FILMS; PHOTOANODES; NANORODS AB We report the design, synthesis and photoelectrochemical characterization of cobalt phosphate (Co-Pi) oxygen evolution catalyst modified heterojunction photoelectrodes consisting of one-dimensional WO3 nanorods (1D-WO3) and highly porous BiVO4 layers. The 1D-WO3 nanorods were prepared by the decomposition of the tetrabutylammonium decatungstate precursor in the presence of poly(ethylene glycol) as a binding agent. The porous BiVO4 layers were spray deposited using a surfactant assisted metal-organic decomposition method. The Co-Pi oxygen evolution catalyst was deposited onto the BiVO4/1D-WO3/FTO heterojunction electrode using a photoassisted electrodeposition method. The Co-Pi catalyst modified heterojunction electrodes exhibited a sustained enhancement in the photocurrent compared to the unmodified BiVO4/1D-WO3/FTO heterojunction electrodes. The improved photoelectrochemical properties profited from the enhanced charge carrier separation achieved through the integration of highly porous BiVO4 layers on top of 1D-WO3 nanorods and from the superior kinetics due to the presence of the Co-Pi oxygen evolution catalyst on top of BiVO4/1D-WO3/FTO heterojunction electrodes. C1 [Pilli, Satyananda Kishore; Janarthanan, Rajeswari; Brown, Logan D.; Herring, Andrew M.] Colorado Sch Mines, Dept Chem & Biol Engn, Golden, CO 80401 USA. [Deutsch, Todd G.] Natl Renewable Energy Lab, Hydrogen Technol & Syst Ctr, Golden, CO 80401 USA. [Furtak, Thomas E.] Colorado Sch Mines, Dept Phys, Golden, CO 80401 USA. [Turner, John A.] Natl Renewable Energy Lab, Golden, CO 80401 USA. RP Herring, AM (reprint author), Colorado Sch Mines, Dept Chem & Biol Engn, Golden, CO 80401 USA. EM spilli@mines.edu; aherring@mines.edu OI Deutsch, Todd/0000-0001-6577-1226; Herring, Andrew/0000-0001-7318-5999 FU Center for Revolutionary Solar Photoconversion FX We thank the Center for Revolutionary Solar Photoconversion for a seed grant. NR 40 TC 36 Z9 37 U1 9 U2 188 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 35 BP 14723 EP 14728 DI 10.1039/c3cp52401a PG 6 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 202EQ UT WOS:000323196800020 PM 23900229 ER PT S AU Benioff, P AF Benioff, Paul BE Donkor, E Pirich, AR Brandt, HE TI Effects of gauge theory based number scaling on geometry SO QUANTUM INFORMATION AND COMPUTATION XI SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Quantum Information and Computation XI CY MAY 02-03, 2013 CL Baltimore, MD SP SPIE DE Mathematics is local; Number scaling; Scalar boson field; Scaled path lengths; Black and white scaling holes ID COHERENT THEORY; MATHEMATICS; PHYSICS; UNIVERSE AB Effects of local availability of mathematics (LAM) and space time dependent number scaling on physics and, especially, geometry are described. LAM assumes separate mathematical systems as structures at each space time point. Extension of gauge theories to include freedom of choice of scaling for number structures, and other structures based on numbers, results in a space time dependent scaling factor based on a scalar boson field. Scaling has no effect on comparison of experimental results with one another or with theory computations. With LAM all theory expressions are elements of mathematics at some reference point. Changing the reference point introduces (external) scaling. Theory expressions with integrals or derivatives over space or time include scaling factors (internal scaling) that cannot be removed by reference point change. Line elements and path lengths, as integrals over space and/or time, show the effect of scaling on geometry. In one example, the scaling factor goes to 0 as the time goes to 0, the big bang time. All path lengths, and values of physical quantities, are crushed to 0 as t goes to 0. Other examples have spherically symmetric scaling factors about some point, x. In one type, a black scaling hole, the scaling factor goes to infinity as the distance, d, between any point y and x goes to 0. For scaling white holes, the scaling factor goes to 0 as d goes to 0. For black scaling holes, path lengths from a reference point, z, to y become infinite as y approaches x. For white holes, path lengths approach a value much less than the unscaled distance from z to x. C1 Argonne Natl Lab, Div Phys, Argonne, IL 60439 USA. RP Benioff, P (reprint author), Argonne Natl Lab, Div Phys, Argonne, IL 60439 USA. EM pbenioff@anl.gov NR 25 TC 0 Z9 0 U1 0 U2 0 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9540-2 J9 PROC SPIE PY 2013 VL 8749 AR UNSP 87490F DI 10.1117/12.2014360 PG 16 WC Computer Science, Interdisciplinary Applications; Optics SC Computer Science; Optics GA BGK64 UT WOS:000323339700009 ER PT J AU Dash, A Knapp, FF Pillai, MRA AF Dash, Ashutosh Knapp, F. F. (Russ), Jr. Pillai, M. R. A. TI Industrial radionuclide generators: a potential step towards accelerating radiotracer investigations in industry SO RSC ADVANCES LA English DT Review ID INORGANIC-ION-EXCHANGERS; HIGH-LEVEL WASTE; AMMONIUM HETEROPOLYACID SALTS; POSITRON-EMISSION-TOMOGRAPHY; ACIDIC NITRATE MEDIA; RADIOISOTOPE GENERATOR; GE-68/GA-68 GENERATOR; SOLVENT-EXTRACTION; MACROCYCLIC POLYETHERS; GE-68-GA-68 GENERATOR AB The novel use of industrial radionuclide generators (IRG) ensures onsite availability of short-lived radionuclides and is expected to contribute significantly to industrial radiotracer investigations. While IRG technology is in its infancy, the use of generator-derived radioisotopes is expected to have broad potential impact on industrial radiotracer investigations. The optimal combination of suitable IRGs and appropriate radiotracer agents will form the basis of such industrial radiotracer investigations. Development of IRGs customized for specific applications is currently under development and the utility of such systems is expected to pave the way for a variety of industry related applications in the areas of residence time distribution (RTD) study, flow rate measurement, leak detection, etc. In this review, we discuss the principles of radionuclide generators, assess major parent/daughter pairs of interest for IRG, and identify the expected utility of potentially useful IRGs. Availability of the parent radionuclides required for IRG fabrication is an important criterion and hence their production is also reviewed. This overview outlines a critical assessment of recent developments, the contemporary status, and key challenges and apertures to the near future. Increase in the knowledge and use of IRGs utilizing available resources will encourage expanded use of these systems for expected future industrial radiotracer studies. C1 [Dash, Ashutosh; Pillai, M. R. A.] Bhabha Atom Res Ctr, Radiopharmaceut Div, Bombay 400085, Maharashtra, India. [Knapp, F. F. (Russ), Jr.] Oak Ridge Natl Lab, Isotope Dev Grp, Med Isotopes Program, Oak Ridge, TN 37831 USA. RP Dash, A (reprint author), Bhabha Atom Res Ctr, Radiopharmaceut Div, Bombay 400085, Maharashtra, India. EM adash@barc.gov.in OI Dash, Ashutosh/0000-0001-7541-7298 FU US Department of Energy [DE-AC05-00OR22725]; UT-Battelle, LLC. FX Research at the Bhabha Atomic Research Centre is part of the ongoing activities of the Department of Atomic Energy, India and is fully supported by government funding. Research at the Oak Ridge National Laboratory is supported by the US Department of Energy under contract DE-AC05-00OR22725 with UT-Battelle, LLC. NR 154 TC 4 Z9 4 U1 2 U2 19 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2046-2069 J9 RSC ADV JI RSC Adv. PY 2013 VL 3 IS 35 BP 14890 EP 14909 DI 10.1039/c3ra41639a PG 20 WC Chemistry, Multidisciplinary SC Chemistry GA 201HU UT WOS:000323132100002 ER PT J AU Wang, L Fu, YB Battaglia, VS Liu, G AF Wang, Lei Fu, Yanbao Battaglia, Vincent S. Liu, Gao TI SBR-PVDF based binder for the application of SLMP in graphite anodes SO RSC ADVANCES LA English DT Article ID LITHIUM-ION BATTERIES; ELECTRODES; PERFORMANCE; CELLS AB A styrene butadiene rubber (SBR)-polyvinylidene difluoride (PVDF) based binder system has been developed for an electrochemical system that is not compatible with the conventional N-methyl pyrrolidinone (NMP) solvent used to cast most Li-ion electrode slurries. This polymer system's binding properties decouple the mechanical and ionic-transport properties. It demonstrates comparable mechanical properties to SBR-based electrodes and cell performance to traditional PVDF-based electrodes. This new binder design however enables the incorporation of stabilized lithium metal powder (SLMP) into a graphite anode to improve its first cycle coulombic efficiency. C1 [Wang, Lei; Fu, Yanbao; Battaglia, Vincent S.; Liu, Gao] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. RP Wang, L (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. EM wanglei@lbl.gov RI Fu, Yanbao/F-9583-2011 OI Fu, Yanbao/0000-0001-7752-680X FU Office of Vehicle Technologies of the U.S. Department of Energy as part of the Industry-Laboratory Integrated Research Program out of the Office of Vehicle Technologies [DE-AC03-76SF00098] FX This research was funded by the Assistant Secretary for Energy Efficiency, Office of Vehicle Technologies of the U.S. Department of Energy under contract no. DE-AC03-76SF00098 as part of the Industry-Laboratory Integrated Research Program out of the Office of Vehicle Technologies. FMC-Lithium Inc. is a partner on this project. NR 19 TC 16 Z9 16 U1 10 U2 62 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 35 BP 15022 EP 15027 DI 10.1039/c3ra42773k PG 6 WC Chemistry, Multidisciplinary SC Chemistry GA 201HU UT WOS:000323132100022 ER PT J AU Rosales, AM Segalman, RA Zuckermann, RN AF Rosales, Adrianne M. Segalman, Rachel A. Zuckermann, Ronald N. TI Polypeptoids: a model system to study the effect of monomer sequence on polymer properties and self-assembly SO SOFT MATTER LA English DT Review ID GENETICALLY DIRECTED SYNTHESES; SELECTIVE RADICAL-ADDITION; BLOCK-RANDOM COPOLYMERS; TO-GLOBULE TRANSITION; SOLID-PHASE SYNTHESIS; AROMATIC SIDE-CHAINS; PEPTOID OLIGOMERS; MULTIBLOCK COPOLYMERS; PERIODIC POLYPEPTIDES; GRADIENT COPOLYMERS AB As the ability to control the monomer sequence of synthetic polymers increases, new relationships between sequence, polymer structure, and functional properties are being discovered. Recent advances in the sequence control of traditional copolymers, such as polyethylenes and polystyrenes, have led to well controlled primary structures ranging from periodic to more precise sequences. As a result, this unprecedented control in the chemical structure of the polymer has necessitated a reexamination of the role of monomer sequence on polymer properties, such as crystallization and self-assembly. In this review, we summarize the developments in establishing a relationship between a polymer's sequence and its properties, and we focus on one sequence-specific polymer system in particular: N-substituted glycines, or polypeptoids. Polypeptoid self-assembly has demonstrated remarkably tunable, hierarchical structures, and through this lens, we look to the future "designability" of sequence-specific polymers in general. C1 [Rosales, Adrianne M.; Segalman, Rachel A.] Univ Calif Berkeley, Dept Chem Engn, Berkeley, CA 94720 USA. [Segalman, Rachel A.; Zuckermann, Ronald N.] Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA USA. [Zuckermann, Ronald N.] Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA USA. RP Rosales, AM (reprint author), Univ Calif Berkeley, Dept Chem Engn, Berkeley, CA 94720 USA. EM adrianne.rosales@gmail.com RI Zuckermann, Ronald/A-7606-2014; Foundry, Molecular/G-9968-2014; OI Zuckermann, Ronald/0000-0002-3055-8860; Segalman, Rachel/0000-0002-4292-5103 FU Office of Naval Research (ONR); Molecular Foundry, a Lawrence Berkeley National Laboratory user facility; Office of Science, Office of Basic Energy Sciences, U.S. Department of Energy [DE-AC02-05CH11231] FX This work was supported by the Office of Naval Research (ONR) in the form of a Presidential Early Career Award (PECASE) in Science and Engineering for R. A. S. This work was also supported by 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. NR 150 TC 40 Z9 40 U1 9 U2 123 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 35 BP 8400 EP 8414 DI 10.1039/c3sm51421h PG 15 WC Chemistry, Physical; Materials Science, Multidisciplinary; Physics, Multidisciplinary; Polymer Science SC Chemistry; Materials Science; Physics; Polymer Science GA 203DB UT WOS:000323269400001 ER PT J AU Phillips, CL Voth, GA AF Phillips, Carolyn L. Voth, Gregory A. TI Discovering crystals using shape matching and machine learning SO SOFT MATTER LA English DT Article ID BINARY NANOPARTICLE SUPERLATTICES; PARTICLES; ORDER; CRYSTALLIZATION; STATISTICS; HISTOGRAMS; NUCLEATION; DISTANCE; LATTICE; DESIGN AB As the rate at which data can be amassed through computational simulation or experimental techniques accelerates, the pace of discovery becomes limited by the rate at which data can be analyzed. In this paper, a method is introduced by which new types of crystalline structures can be automatically identified from large data sets of coordinates. By deploying a hierarchy of pattern analysis techniques using shape matching and machine learning algorithms, local structures are extracted, classified, and then used to partition a data set into groups of common crystals. This method requires no a priori knowledge of what might be present in the data set. The method is applied to two data sets that contain both simple and complex crystals, including quasicrystals. We show how phase diagrams can be automatically generated and identify a crystal phase missed in prior analyses. By integrating shape matching and machine learning techniques to analyze rapidly produced databases, the discovery of new crystal structures and materials can be accelerated. This method is especially applicable to soft matter systems, where particle interactions can be exquisitely tuned and designed to drive the self-assembly of mesoscale materials with exotic structures. C1 [Phillips, Carolyn L.; Voth, Gregory A.] Argonne Natl Lab, Computat Inst, Argonne, IL 60439 USA. [Voth, Gregory A.] Univ Chicago, Dept Chem, James Franck Inst, Inst Biophys Dynam, Chicago, IL 60637 USA. [Voth, Gregory A.] Univ Chicago, Computat Inst, Chicago, IL 60637 USA. RP Phillips, CL (reprint author), Argonne Natl Lab, Computat Inst, 9700 S Cass Ave, Argonne, IL 60439 USA. EM cphillips@anl.gov FU Office of Naval Research; U.S. Department of Energy, Office of Science [DE-AC02-06CH11357]; Office of the Director through the Named Postdoctoral Fellowship Program (Aneesur Rahman Postdoctoral Fellowship), Argonne National Laboratory FX This research was supported in part by a grant from the Office of Naval Research and in part by the U.S. Department of Energy, Office of Science, under Contract DE-AC02-06CH11357. C. L. P. was funded by the Office of the Director through the Named Postdoctoral Fellowship Program (Aneesur Rahman Postdoctoral Fellowship), Argonne National Laboratory. We acknowledge numerous useful discussions with Michael Engel, Aaron Keys, and Jens Kleinjung. We thank Michael Engel for providing the Injavis so. ware package, Aaron Keys for the SMAC so. ware package, and Jens Kleinjung for providing the OPTICS code. NR 58 TC 9 Z9 9 U1 2 U2 18 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1744-683X EI 1744-6848 J9 SOFT MATTER JI Soft Matter PY 2013 VL 9 IS 35 BP 8552 EP 8568 DI 10.1039/c3sm51449h PG 17 WC Chemistry, Physical; Materials Science, Multidisciplinary; Physics, Multidisciplinary; Polymer Science SC Chemistry; Materials Science; Physics; Polymer Science GA 203DB UT WOS:000323269400018 ER PT J AU Stackebrandt, E Zeytun, A Lapidus, A Nolan, M Lucas, S Hammon, N Deshpande, S Cheng, JF Tapia, R Goodwin, LA Pitluck, S Liolios, K Pagani, I Ivanova, N Mavromatis, K Mikhailova, N Huntemann, M Pati, A Chen, A Palaniappan, K Chang, YJ Land, M Hauser, L Rohde, M Pukall, R Goker, M Detter, JC Woyke, T Bristow, J Eisen, JA Markowitz, V Hugenholtz, P Kyrpides, NC Klenk, HP AF Stackebrandt, Erko Zeytun, Ahmet Lapidus, Alla Nolan, Matt Lucas, Susan Hammon, Nancy Deshpande, Shweta Cheng, Jan-Fang Tapia, Roxanne Goodwin, Lynne A. Pitluck, Sam Liolios, Konstantinos Pagani, Ioanna Ivanova, Natalia Mavromatis, Konstantinos Mikhailova, Natalia Huntemann, Marcel Pati, Amrita Chen, Amy Palaniappan, Krishna Chang, Yun-juan Land, Miriam Hauser, Loren Rohde, Manfred Pukall, Ruediger Goeker, Markus Detter, John C. Woyke, Tanja Bristow, James Eisen, Jonathan A. Markowitz, Victor Hugenholtz, Philip Kyrpides, Nikos C. Klenk, Hans-Peter TI Complete genome sequence of Coriobacterium glomerans type strain (PW2(T)) from the midgut of Pyrrhocoris apterus L. (red soldier bug) SO STANDARDS IN GENOMIC SCIENCES LA English DT Article DE Gram-positive; non-motile; non-sporulating; obligatory anaerobic; chemoorganotroph; mesophile; endosymbiont; insect intestinal tract; Coriobacteriaceae; Actinobacteria; GEBA ID PROPOSAL; BACTERIA; ARCHAEA; SYSTEM; NOV; ACTINOBACTERIA; CLASSIFICATION; ATOPOBIUM; DATABASE; GRAPHS AB Coriobacterium glomerans Haas and Konig 1988, is the only species of the genus Coriobacterium, family Coriobacteriaceae, order Coriobacteriales, phylum Actinobacteria. The bacterium thrives as an endosymbiont of pyrrhocorid bugs, i.e. the red fire bug Pyrrhocoris apterus L. The rationale for sequencing the genome of strain PW2(T) is its endosymbiotic life style which is rare among members of Actinobacteria. Here we describe the features of this symbiont, together with the complete genome sequence and its annotation. This is the first complete genome sequence of a member of the genus Coriobacterium and the sixth member of the order Coriobacteriales for which complete genome sequences are now available. The 2,115,681 bp long single replicon genome with its 1,804 protein-coding and 54 RNA genes is part of the Genomic Encyclopedia of Bacteria and Archaea project. C1 [Stackebrandt, Erko; Goeker, Markus; Klenk, Hans-Peter] Leibniz Inst DSMZ German Collect Microorganisms &, Braunschweig, Germany. [Zeytun, Ahmet; Tapia, Roxanne; Goodwin, Lynne A.; Detter, John C.] Los Alamos Natl Lab, Biosci Div, Los Alamos, NM USA. [Zeytun, Ahmet; Lapidus, Alla; Nolan, Matt; Lucas, Susan; Hammon, Nancy; Deshpande, Shweta; Cheng, Jan-Fang; Tapia, Roxanne; Goodwin, Lynne A.; Pitluck, Sam; Liolios, Konstantinos; Pagani, Ioanna; Ivanova, Natalia; Mavromatis, Konstantinos; Mikhailova, Natalia; Huntemann, Marcel; Pati, Amrita; Chang, Yun-juan; Land, Miriam; Hauser, Loren; Woyke, Tanja; Bristow, James; Eisen, Jonathan A.; Hugenholtz, Philip; Kyrpides, Nikos C.] DOE Joint Genome Inst, Walnut Creek, CA USA. [Chen, Amy; Palaniappan, Krishna; Markowitz, Victor] Lawrence Berkeley Natl Lab, Biol Data Management & Technol Ctr, Berkeley, CA USA. [Chang, Yun-juan; Land, Miriam; Hauser, Loren] Oak Ridge Natl Lab, Oak Ridge, TN USA. [Rohde, Manfred] HZI Helmholtz Ctr Infect Res, Braunschweig, Germany. [Eisen, Jonathan A.] Univ Calif Davis, Genome Ctr, Davis, CA 95616 USA. [Hugenholtz, Philip] Univ Queensland, Sch Chem & Mol Biosci, Australian Ctr Ecogen, Brisbane, Qld, Australia. RP Klenk, HP (reprint author), Leibniz Inst DSMZ German Collect Microorganisms &, Braunschweig, Germany. RI Land, Miriam/A-6200-2011; Kyrpides, Nikos/A-6305-2014; Lapidus, Alla/I-4348-2013; OI Land, Miriam/0000-0001-7102-0031; Kyrpides, Nikos/0000-0002-6131-0462; Lapidus, Alla/0000-0003-0427-8731; Eisen, Jonathan A./0000-0002-0159-2197 FU US Department of Energy Office of Science, Biological and Environmental Research Program; University of California, Lawrence Berkeley National Laboratory [DE-AC02-05CH11231]; University of California, Lawrence Livermore National Laboratory [DE-AC52-07NA27344]; University of California, Los Alamos National Laboratory [DE-AC02-06NA25396]; UT-Battelle and Oak Ridge National Laboratory [DE-AC05-00OR22725] FX We would like to gratefully acknowledge the help of Gabriele Gehrich-Schroter for growing C. glomerans cultures, and Susanne Schneider for DNA extraction and quality control (both at DSMZ). This work was performed under the auspices of the US Department of Energy Office of Science, Biological and Environmental Research Program, and by the University of California, Lawrence Berkeley National Laboratory under contract No. DE-AC02-05CH11231, Lawrence Livermore National Laboratory under Contract No. DE-AC52-07NA27344, and Los Alamos National Laboratory under contract No. DE-AC02-06NA25396, UT-Battelle and Oak Ridge National Laboratory under contract DE-AC05-00OR22725. NR 47 TC 2 Z9 3 U1 0 U2 7 PU GENOMIC STAND CONSORT PI EAST LANSING PA MICHIGAN STATE UNIV, GEEO GARRITY, DEPT MICROBIOL, 6162 BIOMED & PHYS SCI BLDG, EAST LANSING, MI 48824 USA SN 1944-3277 J9 STAND GENOMIC SCI JI Stand. Genomic Sci. PY 2013 VL 8 IS 1 BP 15 EP 25 DI 10.4056/sigs.3507020 PG 11 WC Genetics & Heredity; Microbiology SC Genetics & Heredity; Microbiology GA 203WP UT WOS:000323325500002 PM 23961308 ER PT J AU Mavromatis, K Stackebrandt, E Munk, C Lapidus, A Nolan, M Lucas, S Hammon, N Deshpande, S Cheng, JF Tapia, R Goodwin, LA Pitluck, S Liolios, K Pagani, I Ivanova, N Mikhailova, N Huntemann, M Pati, A Chen, A Palaniappan, K Land, M Hauser, L Rohde, M Gronow, S Gooker, M Detter, JC Bristow, J Eisen, JA Markowitz, V Hugenholtz, P Kyrpides, NC Klenk, HP Woyke, T AF Mavromatis, Konstantinos Stackebrandt, Erko Munk, Christine Lapidus, Alla Nolan, Matt Lucas, Susan Hammon, Nancy Deshpande, Shweta Cheng, Jan-Fang Tapia, Roxanne Goodwin, Lynne A. Pitluck, Sam Liolios, Konstantinos Pagani, Ioanna Ivanova, Natalia Mikhailova, Natalia Huntemann, Marcel Pati, Amrita Chen, Amy Palaniappan, Krishna Land, Miriam Hauser, Loren Rohde, Manfred Gronow, Sabine Goeker, Markus Detter, John C. Bristow, James Eisen, Jonathan A. Markowitz, Victor Hugenholtz, Philip Kyrpides, Nikos C. Klenk, Hans-Peter Woyke, Tanja TI Complete genome sequence of the bile-resistant pigment-producing anaerobe Alistipes finegoldii type strain (AHN2437(T)) SO STANDARDS IN GENOMIC SCIENCES LA English DT Article DE Gram-negative; rod-shaped; non-sporulating; non-motile; mesophile; strictly anaerobic; chemoorganotrophic; Rikenellaceae; GEBA ID SP-NOV.; BACTERIA; ARCHAEA; RECLASSIFICATION; ALGORITHM; DATABASE; SYSTEM; GRAPHS; TOOL AB Alistipes finegoldii Rautio et al. 2003 is one of five species of Alistipes with a validly published name: family Rikenellaceae, order Bacteroidetes, class Bacteroidia, phylum Bacteroidetes. This rod-shaped and strictly anaerobic organism has been isolated mostly from human tissues. Here we describe the features of the type strain of this species, together with the complete genome sequence, and annotation. A. finegoldii is the first member of the genus Alistipes for which the complete genome sequence of its type strain is now available. The 3,734,239 bp long single replicon genome with its 3,302 protein-coding and 68 RNA genes is part of the Genomic Encyclopedia of Bacteria and Archaea project. C1 [Mavromatis, Konstantinos; Munk, Christine; Lapidus, Alla; Nolan, Matt; Lucas, Susan; Hammon, Nancy; Deshpande, Shweta; Cheng, Jan-Fang; Tapia, Roxanne; Goodwin, Lynne A.; Pitluck, Sam; Liolios, Konstantinos; Pagani, Ioanna; Ivanova, Natalia; Mikhailova, Natalia; Huntemann, Marcel; Pati, Amrita; Land, Miriam; Hauser, Loren; Bristow, James; Eisen, Jonathan A.; Hugenholtz, Philip; Kyrpides, Nikos C.; Woyke, Tanja] DOE Joint Genome Inst, Walnut Creek, CA USA. [Stackebrandt, Erko; Gronow, Sabine; Klenk, Hans-Peter] Leibniz Inst DSMZ German Collect Microorganisms, Braunschweig, Germany. [Munk, Christine; Hammon, Nancy; Deshpande, Shweta; Tapia, Roxanne; Goodwin, Lynne A.; Detter, John C.] Los Alamos Natl Lab, Biosci Div, Los Alamos, NM USA. [Chen, Amy; Palaniappan, Krishna; Markowitz, Victor] Lawrence Berkeley Natl Lab, Biol Data Management & Technol Ctr, Berkeley, CA USA. [Land, Miriam; Hauser, Loren] Oak Ridge Natl Lab, Oak Ridge, TN USA. [Rohde, Manfred] HZI Helmholtz Ctr Infect Res, Braunschweig, Germany. [Eisen, Jonathan A.] Univ Calif Davis, Genome Ctr, Davis, CA 95616 USA. [Hugenholtz, Philip] Univ Queensland, Sch Chem & Mol Biosci, Australian Ctr Ecogen, Brisbane, Qld, Australia. RP Klenk, HP (reprint author), Leibniz Inst DSMZ German Collect Microorganisms, Braunschweig, Germany. RI Land, Miriam/A-6200-2011; Kyrpides, Nikos/A-6305-2014; Lapidus, Alla/I-4348-2013; OI Land, Miriam/0000-0001-7102-0031; Kyrpides, Nikos/0000-0002-6131-0462; Lapidus, Alla/0000-0003-0427-8731; Eisen, Jonathan A./0000-0002-0159-2197 FU US Department of Energy Office of Science, Biological and Environmental Research Program; University of California, Lawrence Berkeley National Laboratory [DE-AC02-05CH11231]; University of California, Lawrence Livermore National Laboratory [DE-AC52-07NA27344]; University of California, Los Alamos National Laboratory [DE-AC02-06NA25396]; UT-Battelle and Oak Ridge National Laboratory [DE-AC05-00OR22725] FX We would like to gratefully acknowledge the help of Sabine Welnitz for growing A. finegoldii cultures, and Evelyne-Marie Brambilla for DNA extraction and quality control (both at DSMZ). This work was performed under the auspices of the US Department of Energy Office of Science, Biological and Environmental Research Program, and by the University of California, Lawrence Berkeley National Laboratory under contract No. DE-AC02-05CH11231, Lawrence Livermore National Laboratory under Contract No. DE-AC52-07NA27344, and Los Alamos National Laboratory under contract No. DE-AC02-06NA25396, UT-Battelle and Oak Ridge National Laboratory under contract DE-AC05-00OR22725. NR 41 TC 2 Z9 2 U1 1 U2 6 PU GENOMIC STAND CONSORT PI EAST LANSING PA MICHIGAN STATE UNIV, GEEO GARRITY, DEPT MICROBIOL, 6162 BIOMED & PHYS SCI BLDG, EAST LANSING, MI 48824 USA SN 1944-3277 J9 STAND GENOMIC SCI JI Stand. Genomic Sci. PY 2013 VL 8 IS 1 BP 26 EP 36 DI 10.4056/sigs.3527032 PG 11 WC Genetics & Heredity; Microbiology SC Genetics & Heredity; Microbiology GA 203WP UT WOS:000323325500003 PM 23961309 ER PT J AU Stackebrandt, E Chertkov, O Lapidus, A Nolan, M Lucas, S Han, C Cheng, JF Tapia, R Goodwin, LA Bruce, D Pitluck, S Liolios, K Mavromatis, K Pagani, I Ivanova, N Mikhailova, N Huntemann, M Pati, A Chen, A Palaniappan, K Rohde, M Tindall, BJ Goker, M Woyke, T Detter, JC Bristow, J Eisen, JA Markowitz, V Hugenholtz, P Klenk, HP Kyrpides, NC AF Stackebrandt, Erko Chertkov, Olga Lapidus, Alla Nolan, Matt Lucas, Susan Han, Cliff Cheng, Jan-Fang Tapia, Roxanne Goodwin, Lynne A. Bruce, David Pitluck, Sam Liolios, Konstantinos Mavromatis, Konstantinos Pagani, Ioanna Ivanova, Natalia Mikhailova, Natalia Huntemann, Marcel Pati, Amrita Chen, Amy Palaniappan, Krishna Rohde, Manfred Tindall, Brian J. Goeker, Markus Woyke, Tanja Detter, John C. Bristow, James Eisen, Jonathan A. Markowitz, Victor Hugenholtz, Philip Klenk, Hans-Peter Kyrpides, Nikos C. TI High-quality-draft genome sequence of the yellow-pigmented flavobacterium Joostella marina type strain (En5(T)) SO STANDARDS IN GENOMIC SCIENCES LA English DT Article DE Gram-negative; non-motile; aerobic; mesophile; Flavobacteriaceae; Bacteroidetes; GEBA ID FAMILY FLAVOBACTERIACEAE; SP-NOV.; EMENDED DESCRIPTION; BACTERIA; ARCHAEA; MEMBER; CLASSIFICATION; ALGORITHM; DATABASE; PROPOSAL AB At present, Joostella marina Quan et al. 2008 is the sole species with a validly published name in the genus Joostella, family Flavobacteriacae, phylum Bacteriodetes. It is a yellow-pigmented, aerobic, marine organism about which little has been reported other than the chemotaxonomic features required for initial taxonomic description. The genome of J. marina strain En5(T) complements a list of 16 Flavobacteriaceae strains for which complete genomes and draft genomes are currently available. Here we describe the features of this bacterium, together with the complete genome sequence, and annotation. This is the first member of the genus Joostella for which a complete genome sequence becomes available. The 4,508,243 bp long single replicon genome with its 3,944 protein-coding and 60 RNA genes is part of the Genomic Encyclopedia of Bacteria and Archaea project. C1 [Stackebrandt, Erko; Tindall, Brian J.; Goeker, Markus; Klenk, Hans-Peter] Leibniz Inst DSMZ German Collect Microorganisms &, Braunschweig, Germany. [Chertkov, Olga; Lapidus, Alla; Nolan, Matt; Lucas, Susan; Han, Cliff; Cheng, Jan-Fang; Tapia, Roxanne; Goodwin, Lynne A.; Bruce, David; Pitluck, Sam; Liolios, Konstantinos; Mavromatis, Konstantinos; Pagani, Ioanna; Ivanova, Natalia; Mikhailova, Natalia; Huntemann, Marcel; Pati, Amrita; Woyke, Tanja; Bristow, James; Eisen, Jonathan A.; Hugenholtz, Philip; Kyrpides, Nikos C.] DOE Joint Genome Inst, Walnut Creek, CA USA. [Chertkov, Olga; Han, Cliff; Tapia, Roxanne; Goodwin, Lynne A.; Bruce, David; Detter, John C.] Los Alamos Natl Lab, Biosci Div, Los Alamos, NM USA. [Chen, Amy; Palaniappan, Krishna; Markowitz, Victor] Lawrence Berkeley Natl Lab, Biol Data Management & Technol Ctr, Berkeley, CA USA. [Rohde, Manfred] HZI Helmholtz Ctr Infect Res, Braunschweig, Germany. [Eisen, Jonathan A.] Univ Calif Davis, Genome Ctr, Davis, CA 95616 USA. [Hugenholtz, Philip] Univ Queensland, Sch Chem & Mol Biosci, Australian Ctr Ecogen, Brisbane, Qld, Australia. RP Klenk, HP (reprint author), Leibniz Inst DSMZ German Collect Microorganisms &, Braunschweig, Germany. RI Kyrpides, Nikos/A-6305-2014; Lapidus, Alla/I-4348-2013; OI Kyrpides, Nikos/0000-0002-6131-0462; Lapidus, Alla/0000-0003-0427-8731; Eisen, Jonathan A./0000-0002-0159-2197 FU US Department of Energy Office of Science, Biological and Environmental Research Program; University of California, Lawrence Berkeley National Laboratory [DE-AC02-05CH11231]; University of California, Lawrence Livermore National Laboratory [DE-AC52-07NA27344]; University of California, Los Alamos National Laboratory [DE-AC02-06NA25396]; UT-Battelle and Oak Ridge National Laboratory [DE-AC05-00OR22725] FX We would like to gratefully acknowledge the help of Helga Pomrenke for growing J. marina cultures, and Evelyne-Marie Brambilla for DNA extraction and quality control (both at DSMZ). This work was performed under the auspices of the US Department of Energy Office of Science, Biological and Environmental Research Program, and by the University of California, Lawrence Berkeley National Laboratory under contract No. DE-AC02-05CH11231, Lawrence Livermore National Laboratory under Contract No. DE-AC52-07NA27344, and Los Alamos National Laboratory under contract No. DE-AC02-06NA25396, UT-Battelle and Oak Ridge National Laboratory under contract DE-AC05-00OR22725. NR 46 TC 2 Z9 2 U1 1 U2 6 PU GENOMIC STAND CONSORT PI EAST LANSING PA MICHIGAN STATE UNIV, GEEO GARRITY, DEPT MICROBIOL, 6162 BIOMED & PHYS SCI BLDG, EAST LANSING, MI 48824 USA SN 1944-3277 J9 STAND GENOMIC SCI JI Stand. Genomic Sci. PY 2013 VL 8 IS 1 BP 37 EP 46 DI 10.4056/sigs.3537045 PG 10 WC Genetics & Heredity; Microbiology SC Genetics & Heredity; Microbiology GA 203WP UT WOS:000323325500004 PM 23961310 ER PT J AU Mavromatis, K Stackebrandt, E Held, B Lapidus, A Nolan, M Lucas, S Hammon, N Deshpande, S Cheng, JF Tapia, R Goodwin, LA Pitluck, S Liolios, K Pagani, I Ivanova, N Mikhailova, N Huntemann, M Pati, A Chen, A Palaniappan, K Land, M Rohde, M Spring, S Goker, M Woyke, T Detter, JC Bristow, J Eisen, JA Markowitz, V Hugenholtz, P Klenk, HP Kyrpides, NC AF Mavromatis, Konstantinos Stackebrandt, Erko Held, Brittany Lapidus, Alla Nolan, Matt Lucas, Susan Hammon, Nancy Deshpande, Shweta Cheng, Jan-Fang Tapia, Roxanne Goodwin, Lynne A. Pitluck, Sam Liolios, Konstantinos Pagani, Ioanna Ivanova, Natalia Mikhailova, Natalia Huntemann, Marcel Pati, Amrita Chen, Amy Palaniappan, Krishna Land, Miriam Rohde, Manfred Spring, Stefan Goeker, Markus Woyke, Tanja Detter, John C. Bristow, James Eisen, Jonathan A. Markowitz, Victor Hugenholtz, Philip Klenk, Hans-Peter Kyrpides, Nikos C. TI Complete genome sequence of the moderate thermophile Anaerobaculum mobile type strain (NGA(T)) SO STANDARDS IN GENOMIC SCIENCES LA English DT Article DE Gram-negative; rod-shaped; motile; flagellum; non-spore forming; anaerobic; chemoorganotrophic; crotonate-reducer; Synergistetes; Synergistaceae; GEBA ID EMENDED DESCRIPTION; GENUS ANAEROBACULUM; SP NOV.; BACTERIUM; ARCHAEA; ALGORITHM; DATABASE; GLUCOSE; SYSTEM; GRAPHS AB Anaerobaculum mobile Menes and Muxi 2002 is one of three described species of the genus Anaerobaculum, family Synergistaceae, phylum Synergistetes. This anaerobic and motile bacterium ferments a range of carbohydrates and mono- and dicarboxylic acids with acetate, hydrogen and CO2 as end products. A. mobile NGA(T) is the first member of the genus Anaerobaculum and the sixth member of the phylum Synergistetes with a completely sequenced genome. Here we describe the features of this bacterium, together with the complete genome sequence, and annotation. The 2,160,700 bp long single replicon genome with its 2,053 protein-coding and 56 RNA genes is part of the Genomic Encyclopedia of Bacteria and Archaea project. C1 [Mavromatis, Konstantinos; Held, Brittany; Lapidus, Alla; Nolan, Matt; Lucas, Susan; Hammon, Nancy; Deshpande, Shweta; Cheng, Jan-Fang; Tapia, Roxanne; Goodwin, Lynne A.; Pitluck, Sam; Liolios, Konstantinos; Pagani, Ioanna; Ivanova, Natalia; Mikhailova, Natalia; Huntemann, Marcel; Pati, Amrita; Land, Miriam; Woyke, Tanja; Bristow, James; Eisen, Jonathan A.; Hugenholtz, Philip; Kyrpides, Nikos C.] DOE Joint Genome Inst, Walnut Creek, CA USA. [Stackebrandt, Erko; Spring, Stefan; Goeker, Markus; Klenk, Hans-Peter] Leibniz Inst DSMZ German Collect Microorganisms &, Braunschweig, Germany. [Held, Brittany; Hammon, Nancy; Deshpande, Shweta; Tapia, Roxanne; Goodwin, Lynne A.; Detter, John C.] Los Alamos Natl Lab, Biosci Div, Los Alamos, NM USA. [Chen, Amy; Palaniappan, Krishna] Lawrence Berkeley Natl Lab, Biol Data Management & Technol Ctr, Berkeley, CA USA. [Land, Miriam] Oak Ridge Natl Lab, Oak Ridge, TN USA. [Rohde, Manfred] HZI Helmholtz Ctr Infect Res, Braunschweig, Germany. [Eisen, Jonathan A.] Univ Calif Davis, Genome Ctr, Davis, CA USA. [Hugenholtz, Philip] Univ Queensland, Sch Chem & Mol Biosci, Australian Ctr Ecogen, Brisbane, Qld, Australia. RP Klenk, HP (reprint author), Leibniz Inst DSMZ German Collect Microorganisms &, Braunschweig, Germany. RI Spring, Stefan/N-6933-2013; Land, Miriam/A-6200-2011; Kyrpides, Nikos/A-6305-2014; Lapidus, Alla/I-4348-2013; OI Spring, Stefan/0000-0001-6247-0938; Land, Miriam/0000-0001-7102-0031; Kyrpides, Nikos/0000-0002-6131-0462; Lapidus, Alla/0000-0003-0427-8731; Eisen, Jonathan A./0000-0002-0159-2197 FU US Department of Energy Office of Science, Biological and Environmental Research Program; University of California, Lawrence Berkeley National Laboratory [DE-AC02-05CH11231]; University of California, Lawrence Livermore National Laboratory [DE-AC52-07NA27344]; University of California, Los Alamos National Laboratory [DE-AC02-06NA25396]; UT-Battelle and Oak Ridge National Laboratory [DE-AC05-00OR22725] FX We would like to gratefully acknowledge the help of Maren Schroder for growing A. mobile cultures, Evelyne-Marie Brambilla for DNA extraction and quality control, and Cathrin Sproer and Rudiger Pukall for helpful comments (all at DSMZ). This work was performed under the auspices of the US Department of Energy Office of Science, Biological and Environmental Research Program, and by the University of California, Lawrence Berkeley National Laboratory under contract No. DE-AC02-05CH11231, Lawrence Livermore National Laboratory under Contract No. DE-AC52-07NA27344, and Los Alamos National Laboratory under contract No. DE-AC02-06NA25396, UT-Battelle and Oak Ridge National Laboratory under contract DE-AC05-00OR22725. NR 38 TC 6 Z9 7 U1 0 U2 4 PU GENOMIC STAND CONSORT PI EAST LANSING PA MICHIGAN STATE UNIV, GEEO GARRITY, DEPT MICROBIOL, 6162 BIOMED & PHYS SCI BLDG, EAST LANSING, MI 48824 USA SN 1944-3277 J9 STAND GENOMIC SCI JI Stand. Genomic Sci. PY 2013 VL 8 IS 1 BP 47 EP 57 DI 10.4056/sigs.3547050 PG 11 WC Genetics & Heredity; Microbiology SC Genetics & Heredity; Microbiology GA 203WP UT WOS:000323325500005 PM 23961311 ER PT J AU Visser, M Worm, P Muyzer, G Pereira, IAC Schaap, PJ Plugge, CM Kuever, J Parshina, SN Nazina, TN Ivanova, AE Bernier-Latmani, R Goodwin, LA Kyrpides, NC Woyke, T Chain, P Davenport, KW Spring, S Klenk, HP Stams, AJM AF Visser, Michael Worm, Petra Muyzer, Gerard Pereira, Ines A. C. Schaap, Peter J. Plugge, Caroline M. Kuever, Jan Parshina, Sofiya N. Nazina, Tamara N. Ivanova, Anna E. Bernier-Latmani, Rizlan Goodwin, Lynne A. Kyrpides, Nikos C. Woyke, Tanja Chain, Patrick Davenport, Karen W. Spring, Stefan Klenk, Hans-Peter Stams, Alfons J. M. TI Genome analysis of Desulfotomaculum kuznetsovii strain 17(T) reveals a physiological similarity with Pelotomaculum thermopropionicum strain SIT SO STANDARDS IN GENOMIC SCIENCES LA English DT Article DE Thermophilic spore-forming anaerobes; sulfate reduction; autotrophic; methylotrophic; Peptococcaceae; Clostridiales ID SULFATE-REDUCING BACTERIA; CLOSTRIDIUM-THERMOACETICUM; CARBON-MONOXIDE; GEN. NOV.; SEQUENCE; PREDICTION; BIOSYNTHESIS; OXIDATION; METHANOL; ENZYMES AB Desulfotomaculum kuznetsovii is a moderately thermophilic member of the polyphyletic spore-forming genus Desulfotomaculum in the family Peptococcaceae. This species is of interest because it originates from deep subsurface thermal mineral water at a depth of about 3,000 m. D. kuznetsovii is a rather versatile bacterium as it can grow with a large variety of organic substrates, including short-chain and long-chain fatty acids, which are degraded completely to carbon dioxide coupled to the reduction of sulfate. It can grow methylotrophically with methanol and sulfate and autotrophically with H-2 + CO2 and sulfate. For growth it does not require any vitamins. Here, we describe the features of D. kuznetsovii together with the genome sequence and annotation. The chromosome has 3,601,386 bp organized in one contig. A total of 3,567 candidate protein-encoding genes and 58 RNA genes were identified. Genes of the acetyl-CoA pathway, possibly involved in heterotrophic growth with acetate and methanol, and in CO2 fixation during autotrophic growth are present. Genomic comparison revealed that D. kuznetsovii shows a high similarity with Pelotomaculum thermopropionicum. Genes involved in propionate metabolism of these two strains show a strong similarity. However, main differences are found in genes involved in the electron acceptor metabolism. C1 [Visser, Michael; Worm, Petra; Plugge, Caroline M.; Stams, Alfons J. M.] Wageningen Univ, Microbiol Lab, NL-6700 AP Wageningen, Netherlands. [Muyzer, Gerard] Univ Amsterdam, Inst Biodivers & Ecosyst Dynam, Dept Aquat Microbiol, Amsterdam, Netherlands. [Pereira, Ines A. C.] Univ Nova Lisboa, Inst Tecnol Quim & Biol, Oeiras, Portugal. [Schaap, Peter J.] Wageningen Univ, Lab Syst & Synthet Biol, NL-6700 AP Wageningen, Netherlands. [Kuever, Jan] Bremen Inst Mat Testing, Dept Microbiol, Bremen, Germany. [Parshina, Sofiya N.; Nazina, Tamara N.; Ivanova, Anna E.] Russian Acad Sci, Winogradsky Inst Microbiol, Moscow, Russia. [Bernier-Latmani, Rizlan] Ecole Polytech Fed Lausanne, Lausanne, Switzerland. [Goodwin, Lynne A.; Kyrpides, Nikos C.; Woyke, Tanja; Chain, Patrick; Davenport, Karen W.] DOE Joint Genome Inst, Walnut Creek, CA USA. [Goodwin, Lynne A.; Chain, Patrick; Davenport, Karen W.] Los Alamos Natl Lab, Biosci Div, Los Alamos, NM USA. [Spring, Stefan; Klenk, Hans-Peter] Leibniz Inst DSMZ German Collect Microorganisms &, Braunschweig, Germany. [Stams, Alfons J. M.] Univ Minho, Ctr Biol Engn, Braga, Portugal. RP Visser, M (reprint author), Wageningen Univ, Microbiol Lab, NL-6700 AP Wageningen, Netherlands. RI Bernier-Latmani, Rizlan/E-4398-2011; Spring, Stefan/N-6933-2013; Pereira, Ines/C-2748-2009; Kyrpides, Nikos/A-6305-2014; Stams, Alfons/C-8167-2014; OI Bernier-Latmani, Rizlan/0000-0001-6547-722X; Spring, Stefan/0000-0001-6247-0938; Chain, Patrick/0000-0003-3949-3634; Pereira, Ines/0000-0003-3283-4520; Kyrpides, Nikos/0000-0002-6131-0462; Stams, Alfons/0000-0001-7840-6500; Muyzer, Gerard/0000-0002-2422-0732 FU Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]; Netherlands Science Foundation (NWO) [CW-TOP 700.55.343, ALW 819.02.014]; European Research Council [323009] 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, and was also supported by grants CW-TOP 700.55.343 and ALW 819.02.014 of the Netherlands Science Foundation (NWO) and grant 323009 of the European Research Council. NR 52 TC 10 Z9 10 U1 1 U2 13 PU GENOMIC STAND CONSORT PI EAST LANSING PA MICHIGAN STATE UNIV, GEEO GARRITY, DEPT MICROBIOL, 6162 BIOMED & PHYS SCI BLDG, EAST LANSING, MI 48824 USA SN 1944-3277 J9 STAND GENOMIC SCI JI Stand. Genomic Sci. PY 2013 VL 8 IS 1 BP 69 EP 87 DI 10.4056/sigs.3627141 PG 19 WC Genetics & Heredity; Microbiology SC Genetics & Heredity; Microbiology GA 203WP UT WOS:000323325500007 PM 23961313 ER PT J AU Abt, B Goker, M Scheuner, C Han, C Lu, MG Misra, M Lapidus, A Nolan, M Lucas, S Hammon, N Deshpande, S Cheng, JF Tapia, R Goodwin, LA Pitluck, S Liolios, K Pagani, I Ivanova, N Mavromatis, K Mikhailova, N Huntemann, M Pati, A Chen, A Palaniappan, K Land, M Hauser, L Jeffries, CD Rohde, M Spring, S Gronow, S Detter, JC Bristow, J Eisen, JA Markowitz, V Hugenholtz, P Kyrpides, NC Woyke, T Klenk, HP AF Abt, Birte Goeker, Markus Scheuner, Carmen Han, Cliff Lu, Megan Misra, Monica Lapidus, Alla Nolan, Matt Lucas, Susan Hammon, Nancy Deshpande, Shweta Cheng, Jan-Fang Tapia, Roxanne Goodwin, Lynne A. Pitluck, Sam Liolios, Konstantinos Pagani, Ioanna Ivanova, Natalia Mavromatis, Konstantinos Mikhailova, Natalia Huntemann, Marcel Pati, Amrita Chen, Amy Palaniappan, Krishna Land, Miriam Hauser, Loren Jeffries, Cynthia D. Rohde, Manfred Spring, Stefan Gronow, Sabine Detter, John C. Bristow, James Eisen, Jonathan A. Markowitz, Victor Hugenholtz, Philip Kyrpides, Nikos C. Woyke, Tanja Klenk, Hans-Peter TI Genome sequence of the thermophilic fresh-water bacterium Spirochaeta caldaria type strain (H1(T)), reclassification of Spirochaeta caldaria, Spirochaeta stenostrepta, and Spirochaeta zuelzerae in the genus Treponema as Treponema caldaria comb. nov., Treponema stenostrepta comb. nov., and Treponema zuelzerae comb. nov., and emendation of the genus Treponema SO STANDARDS IN GENOMIC SCIENCES LA English DT Article DE obligately anaerobic; thermophilic; spiral-shaped; motile; periplasmic flagella; Gram-negative; chemoorganotrophic; Spirochaetaceae; Spirochaeta; Treponema; GEBA ID STANDARD OPERATING PROCEDURE; CLASSIFICATION; ARCHAEA; SYSTEM; NAMES; PERIODONTITIS; NOMENCLATURE; PHYLOGENY; ALGORITHM; DATABASE AB Spirochaeta caldaria Pohlschroeder et al. 1995 is an obligately anaerobic, spiral-shaped bacterium that is motile via periplasmic flagella. The type strain, H1(T), was isolated in 1990 from cyanobacterial mat samples collected at a freshwater hot spring in Oregon, USA, and is of interest because it enhances the degradation of cellulose when grown in co-culture with Clostridium thermocellum. Here we provide a taxonomic re-evaluation for S. caldaria based on phylogenetic analyses of 16S rRNA sequences and whole genomes, and propose the reclassification of S. caldaria and two other Spirochaeta species as members of the emended genus Treponema. Whereas genera such as Borrelia and Sphaerochaeta possess well-distinguished genomic features related to their divergent lifestyles, the physiological and functional genomic characteristics of Spirochaeta and Treponema appear to be intermixed and are of little taxonomic value. The 3,239,340 bp long genome of strain H1(T) with its 2,869 protein-coding and 59 RNA genes is a part of the Genomic Encyclopedia of Bacteria and Archaea project. C1 [Abt, Birte; Goeker, Markus; Scheuner, Carmen; Spring, Stefan; Gronow, Sabine; Klenk, Hans-Peter] Leibniz Inst DSMZ German Collect Microorganisms &, Braunschweig, Germany. [Han, Cliff; Lu, Megan; Misra, Monica; Lapidus, Alla; Nolan, Matt; Lucas, Susan; Hammon, Nancy; Deshpande, Shweta; Cheng, Jan-Fang; Tapia, Roxanne; Goodwin, Lynne A.; Pitluck, Sam; Liolios, Konstantinos; Pagani, Ioanna; Ivanova, Natalia; Mavromatis, Konstantinos; Mikhailova, Natalia; Huntemann, Marcel; Pati, Amrita; Land, Miriam; Hauser, Loren; Jeffries, Cynthia D.; Bristow, James; Eisen, Jonathan A.; Hugenholtz, Philip; Kyrpides, Nikos C.; Woyke, Tanja] DOE Joint Genome Inst, Walnut Creek, CA USA. [Han, Cliff; Lu, Megan; Misra, Monica; Tapia, Roxanne; Goodwin, Lynne A.; Detter, John C.] Los Alamos Natl Lab, Biosci Div, Los Alamos, NM USA. [Chen, Amy; Palaniappan, Krishna; Markowitz, Victor] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Biol Data Management & Technol Ctr, Berkeley, CA 94720 USA. [Land, Miriam; Hauser, Loren; Jeffries, Cynthia D.] Oak Ridge Natl Lab, Oak Ridge, TN USA. [Rohde, Manfred] HZI Helmholtz Ctr Infect Res, Braunschweig, Germany. [Eisen, Jonathan A.] Univ Calif Davis, Genome Ctr, Davis, CA 95616 USA. [Hugenholtz, Philip] Univ Queensland, Sch Chem & Mol Biosci, Australian Ctr Ecogenom, Brisbane, Qld, Australia. RP Woyke, T (reprint author), DOE Joint Genome Inst, Walnut Creek, CA USA. EM T_Woyke@lbl.gov; hpk@dsmz.de RI Kyrpides, Nikos/A-6305-2014; Lapidus, Alla/I-4348-2013; Spring, Stefan/N-6933-2013; Land, Miriam/A-6200-2011 OI Kyrpides, Nikos/0000-0002-6131-0462; Lapidus, Alla/0000-0003-0427-8731; Spring, Stefan/0000-0001-6247-0938; Land, Miriam/0000-0001-7102-0031 FU US Department of Energy Office of Science, Biological and Environmental Research Program; University of California, Lawrence Berkeley National Laboratory [DE-AC02-05CH11231]; University of California, Lawrence Livermore National Laboratory [DE-AC52-07NA27344]; University of California, Los Alamos National Laboratory [DE-AC02-06NA25396]; UT-Battelle and Oak Ridge National Laboratory [DE-AC05-00OR22725]; German Research Foundation (DFG) [INST 599/1-2] FX We would like to gratefully acknowledge the help of Maren Schroder for growing S. caldaria cultures and Evelyne-Marie Bramilla for DNA extraction and quality control (both at DSMZ). This work was performed under the auspices of the US Department of Energy Office of Science, Biological and Environmental Research Program, and by the University of California, Lawrence Berkeley National Laboratory under contract No. DE-AC02-05CH11231, Lawrence Livermore National Laboratory under Contract No. DE-AC52-07NA27344, and Los Alamos National Laboratory under contract No. DE-AC02-06NA25396, UT-Battelle and Oak Ridge National Laboratory under contract DE-AC05-00OR22725, as well as German Research Foundation (DFG) INST 599/1-2. NR 72 TC 14 Z9 14 U1 3 U2 20 PU BIOMED CENTRAL LTD PI LONDON PA 236 GRAYS INN RD, FLOOR 6, LONDON WC1X 8HL, ENGLAND SN 1944-3277 J9 STAND GENOMIC SCI JI Stand. Genomic Sci. PY 2013 VL 8 IS 1 BP 88 EP 105 DI 10.4056/sigs.3096473 PG 18 WC Genetics & Heredity; Microbiology SC Genetics & Heredity; Microbiology GA 203WP UT WOS:000323325500008 PM 23961314 ER PT J AU Smith, D Alverdy, J An, G Coleman, M Garcia-Houchins, S Green, J Keegan, K Kelley, ST Kirkup, BC Kociolek, L Levin, H Landon, E Olsiewski, P Knight, R Siegel, J Weber, S Gilbert, J AF Smith, Daniel Alverdy, John An, Gary Coleman, Maureen Garcia-Houchins, Sylvia Green, Jessica Keegan, Kevin Kelley, Scott T. Kirkup, Benjamin C. Kociolek, Larry Levin, Hal Landon, Emily Olsiewski, Paula Knight, Rob Siegel, Jeffrey Weber, Stephen Gilbert, Jack TI The Hospital Microbiome Project: Meeting Report for the 1st Hospital Microbiome Project Workshop on sampling design and building science measurements, Chicago, USA, June 7th-8th 2012 SO STANDARDS IN GENOMIC SCIENCES LA English DT Article AB This report details the outcome of the 1st Hospital Microbiome Project workshop held on June 7th-8th, 2012 at the University of Chicago, USA. The workshop was arranged to determine the most appropriate sampling strategy and approach to building science measurement to characterize the development of a microbial community within a new hospital pavilion being built at the University of Chicago Medical Center. The workshop made several recommendations and led to the development of a full proposal to the Alfred P. Sloan Foundation as well as to the creation of the Hospital Microbiome Consortium. C1 [Smith, Daniel; Keegan, Kevin; Gilbert, Jack] Argonne Natl Lab, Argonne, IL 60439 USA. [Alverdy, John; An, Gary] Univ Chicago, Dept Surg, Chicago, IL 60637 USA. [Coleman, Maureen] Univ Chicago, Dept Geophys Sci, Chicago, IL 60637 USA. [Garcia-Houchins, Sylvia; Weber, Stephen] Univ Chicago UCMC Infect Control, Chicago, IL 60637 USA. [Green, Jessica] Univ Oregon, Inst Ecol & Evolut, Eugene, OR 97403 USA. [Kelley, Scott T.] San Diego State Univ, Dept Biol, San Diego, CA 92182 USA. [Kirkup, Benjamin C.] Walter Reed Army Inst Res, Dept Wound Infect, Silver Spring, MD 20910 USA. [Kirkup, Benjamin C.] Uniformed Serv Univ Hlth Sci, F Edward Hebert Sch Med, Bethesda, MD 20814 USA. [Kociolek, Larry] Ann & Robert H Lurie Childrens Hosp Chicago, Div Infect Dis, Dept Pediat, Chicago, IL 60611 USA. [Levin, Hal] Bldg Ecol Res Grp, Santa Cruz, CA 95060 USA. [Landon, Emily] Univ Chicago, Med Ctr, Chicago, IL 60637 USA. [Olsiewski, Paula] Alfred P Sloan Fdn, New York, NY 10111 USA. [Knight, Rob] Univ Colorado, Howard Hughes Med Inst, Boulder, CO 80309 USA. [Knight, Rob] Univ Colorado, Dept Chem & Biochem, Boulder, CO 80309 USA. [Siegel, Jeffrey] Univ Texas Austin, Civil Archectural & Environm Engn Dept, Austin, TX 78712 USA. [Gilbert, Jack] Univ Chicago, Dept Ecol & Evolut, Chicago, IL 60637 USA. RP Smith, D (reprint author), Argonne Natl Lab, 9700 S Cass Ave, Argonne, IL 60439 USA. RI Kirkup, Benjamin/C-3610-2009; Knight, Rob/D-1299-2010; OI Kirkup, Benjamin/0000-0002-8722-6218; Kociolek, Larry/0000-0002-8756-3417; An, Gary/0000-0003-4549-9004 FU APSF; US Dept. of Energy [DE-AC02-06CH11357]; Argonne, a US Department of Energy Office of Science laboratory [DE-AC02-06CH11357] FX We acknowledge the APSF for funding this workshop. This work was supported in part by the US Dept. of Energy under Contract DE-AC02-06CH11357. The submitted manuscript has been created in part by UChicago Argonne, LLC, Operator of Argonne National Laboratory ("Argonne"). Argonne, a US Department of Energy Office of Science laboratory, is operated under Contract No. DE-AC02-06CH11357. The US 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 6 TC 6 Z9 6 U1 0 U2 19 PU GENOMIC STAND CONSORT PI EAST LANSING PA MICHIGAN STATE UNIV, GEEO GARRITY, DEPT MICROBIOL, 6162 BIOMED & PHYS SCI BLDG, EAST LANSING, MI 48824 USA SN 1944-3277 J9 STAND GENOMIC SCI JI Stand. Genomic Sci. PY 2013 VL 8 IS 1 BP 112 EP 117 DI 10.4056/sigs.3717348 PG 6 WC Genetics & Heredity; Microbiology SC Genetics & Heredity; Microbiology GA 203WP UT WOS:000323325500010 PM 23961316 ER PT J AU Bates, ST Ahrendt, S Bik, HM Bruns, TD Caporaso, JG Cole, J Dwan, M Fierer, N Gu, D Houston, S Knight, R Leff, J Lewis, C Maestre, JP McDonald, D Nilsson, RH Porras-Alfaro, A Robert, V Schoch, C Scott, J Taylor, DL Parfrey, LW Stajich, JE AF Bates, Scott T. Ahrendt, Steven Bik, Holly M. Bruns, Thomas D. Caporaso, J. Gregory Cole, James Dwan, Michael Fierer, Noah Gu, Dai Houston, Shawn Knight, Rob Leff, Jon Lewis, Christopher Maestre, Juan P. McDonald, Daniel Nilsson, R. Henrik Porras-Alfaro, Andrea Robert, Vincent Schoch, Conrad Scott, James Taylor, D. Lee Parfrey, Laura Wegener Stajich, Jason E. TI Meeting Report: Fungal ITS Workshop (October 2012) SO STANDARDS IN GENOMIC SCIENCES LA English DT Article ID DATABASE; CLASSIFICATION; SEQUENCES C1 [Bates, Scott T.; Fierer, Noah; Leff, Jon] Univ Colorado, Cooperat Inst Res Environm Sci, Boulder, CO 80309 USA. [Ahrendt, Steven; Gu, Dai; Stajich, Jason E.] Univ Calif Riverside, Dept Plant Pathol & Microbiol, Riverside, CA 92521 USA. [Bik, Holly M.] Univ Calif Davis, UC Davis Genome Ctr, Davis, CA 95616 USA. [Bruns, Thomas D.] Univ Calif Berkeley, Dept Plant & Microbial Biol, Berkeley, CA 94720 USA. [Caporaso, J. Gregory] No Arizona Univ, Dept Comp Sci, Flagstaff, AZ 86011 USA. [Caporaso, J. Gregory] Argonne Natl Labs, Argonne, IL USA. [Cole, James] Michigan State Univ, Dept Microbiol & Mol Genetet, E Lansing, MI 48824 USA. [Dwan, Michael] TGen North, Ctr Microbi & Human Hlth, Flagstaff, AZ USA. [Houston, Shawn] Univ Minnesota, Minnesota Supercomp Inst, Minneapolis, MN USA. [Knight, Rob; McDonald, Daniel] Univ Colorado, Dept Chem & Biochem, Boulder, CO 80309 USA. [Knight, Rob; Parfrey, Laura Wegener] Univ Colorado, Howard Hughes Med Inst, Boulder, CO 80309 USA. [Lewis, Christopher] Agr & Agri Food Canada, Eastern Cereals & Oilseed Res Ctr, Ottawa, ON, Canada. [Maestre, Juan P.] Univ Texas Austin, Dept Civil Architecture & Environm Engn, Austin, TX 78712 USA. [McDonald, Daniel] Univ Colorado, Biofrontiers Inst, Boulder, CO 80309 USA. [Nilsson, R. Henrik] Univ Gothenburg, Dept Biol & Environm Sci, Gothenburg, Sweden. [Porras-Alfaro, Andrea] Western Illinois Univ, Dept Biol Sci, Macomb, IL 61455 USA. [Robert, Vincent] Royal Netherlands Acad Arts & Sci, Cent Bureau Schimmelcultures, Utrecht, Netherlands. [Schoch, Conrad] NIH, Natl Ctr Biotechnol Informat, Natl Lib Med, Bethesda, MD 20892 USA. [Scott, James] Univ Toronto, Dalla Lana Sch Publ Hlth, Div Occupat & Environm Hlth, Toronto, ON, Canada. [Taylor, D. Lee] Univ Alaska, Inst Arctic Biol, Fairbanks, AK 99775 USA. RP Bates, ST (reprint author), Univ Colorado, Cooperat Inst Res Environm Sci, Boulder, CO 80309 USA. RI Scott, James/A-8598-2011; Stajich, Jason/C-7297-2008; Knight, Rob/D-1299-2010; OI Scott, James/0000-0002-5073-0832; Stajich, Jason/0000-0002-7591-0020; Taylor, Donald/0000-0002-5985-9210; Porras-Alfaro, Andrea/0000-0002-9053-7973; Nilsson, Henrik/0000-0002-8052-0107 FU Paula Olsiewski; Alfred P. Sloan Foundation FX The workshop would not have been possible without the intellectual and financial support of Paula Olsiewski and the Alfred P. Sloan Foundation. We thank Jason Stajich, for organizing the meeting, as well as all the workshop participants for their valuable contributions. NR 17 TC 12 Z9 12 U1 0 U2 13 PU GENOMIC STAND CONSORT PI EAST LANSING PA MICHIGAN STATE UNIV, GEEO GARRITY, DEPT MICROBIOL, 6162 BIOMED & PHYS SCI BLDG, EAST LANSING, MI 48824 USA SN 1944-3277 J9 STAND GENOMIC SCI JI Stand. Genomic Sci. PY 2013 VL 8 IS 1 BP 118 EP 123 PG 6 WC Genetics & Heredity; Microbiology SC Genetics & Heredity; Microbiology GA 203WP UT WOS:000323325500011 PM 23961317 ER PT J AU DeAngelis, KM D'Haeseleer, P Chivian, D Simmons, B Arkin, AP Mavromatis, K Malfatti, S Tringe, S Hazen, TC AF DeAngelis, Kristen M. D'Haeseleer, Patrik Chivian, Dylan Simmons, Blake Arkin, Adam P. Mavromatis, Konstantinos Malfatti, Stephanie Tringe, Susannah Hazen, Terry C. TI Metagenomes of tropical soil-derived anaerobic switchgrass-adapted consortia with and without iron SO STANDARDS IN GENOMIC SCIENCES LA English DT Article DE Anaerobic decomposition; switchgrass; Panicum virgatum; tropical forest soil; feedstock-adapted consortia; bacteria; archaea; metagenomics ID MICROBIAL COMMUNITIES; GENOME SEQUENCE; REDUCTION; DATABASE; MICROORGANISMS; IDENTIFICATION; ENVIRONMENTS; RECOGNITION; STRATEGIES; PATTERNS AB Tropical forest soils decompose litter rapidly with frequent episodes of anoxia, making it likely that bacteria using alternate terminal electron acceptors (TEAs) such as iron play a large role in supporting decomposition under these conditions. The prevalence of many types of metabolism in litter deconstruction makes these soils useful templates for improving biofuel production. To investigate how iron availability affects decomposition, we cultivated feedstock-adapted consortia (FACs) derived from iron-rich tropical forest soils accustomed to experiencing frequent episodes of anaerobic conditions and frequently fluctuating redox. One consortium was propagated under fermenting conditions, with switchgrass as the sole carbon source in minimal media (SG only FACs), and the other consortium was treated the same way but received poorly crystalline iron as an additional terminal electron acceptor (SG + Fe FACs). We sequenced the metagenomes of both consortia to a depth of about 150 Mb each, resulting in a coverage of 26x for the more diverse SG + Fe FACs, and 81 x for the relatively less diverse SG only FACs. Both consortia were able to quickly grow on switchgrass, and the iron-amended consortium exhibited significantly higher microbial diversity than the unamended consortium. We found evidence of higher stress in the unamended FACs and increased sugar transport and utilization in the iron-amended FACs. This work provides metagenomic evidence that supplementation of alternative TEAs may improve feedstock deconstruction in biofuel production. C1 [DeAngelis, Kristen M.] Univ Massachusetts, Dept Microbiol, Amherst, MA 01003 USA. [DeAngelis, Kristen M.; D'Haeseleer, Patrik; Simmons, Blake; Hazen, Terry C.] Joint BioEnergy Inst, Deconstruct Div, Microbial Communities Grp, Emeryville, CA USA. [D'Haeseleer, Patrik] Lawrence Livermore Natl Lab, Livermore, CA USA. [Chivian, Dylan; Arkin, Adam P.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA 94720 USA. [Chivian, Dylan; Arkin, Adam P.] Joint BioEnergy Inst, Div Technol, Emeryville, CA USA. [Simmons, Blake] Sandia Natl Labs, Livermore, CA USA. [Mavromatis, Konstantinos; Malfatti, Stephanie; Tringe, Susannah] Joint Genome Inst, Dept Energy, Walnut Creek, CA USA. [Hazen, Terry C.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, Dept Ecol, Berkeley, CA 94720 USA. [Hazen, Terry C.] Univ Tennessee, Dept Civil & Environm Engn, Knoxville, TN USA. [Hazen, Terry C.] Oak Ridge Natl Lab, Biosci Div, Oak Ridge, TN USA. RP DeAngelis, KM (reprint author), Univ Massachusetts, Dept Microbiol, Amherst, MA 01003 USA. EM kristen@post.harvard.edu RI Arkin, Adam/A-6751-2008; Hazen, Terry/C-1076-2012; OI Arkin, Adam/0000-0002-4999-2931; Hazen, Terry/0000-0002-2536-9993; 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 work conducted in part by the US Department of Energy Joint Genome Institute and in part by the Joint BioEnergy Institute (http://www.jbei.org) supported by the US Department of Energy, Office of Science, Office of Biological and Environmental Research, under Contract No. DE-AC02-05CH11231. We would like to thank Dr. Ken Vogel (USDA, ARS, Lincoln, NE) for providing samples of switchgrass (MPV 2 cultivar) for use in these studies. We are also grateful to Albert Barberan for guidance in constructing the community networks. NR 48 TC 6 Z9 6 U1 2 U2 24 PU GENOMIC STAND CONSORT PI EAST LANSING PA MICHIGAN STATE UNIV, GEEO GARRITY, DEPT MICROBIOL, 6162 BIOMED & PHYS SCI BLDG, EAST LANSING, MI 48824 USA SN 1944-3277 J9 STAND GENOMIC SCI JI Stand. Genomic Sci. PY 2013 VL 7 IS 3 BP 382 EP 398 DI 10.4056/sigs.3377516 PG 17 WC Genetics & Heredity; Microbiology SC Genetics & Heredity; Microbiology GA 203VY UT WOS:000323323500004 PM 24019987 ER PT J AU Murugapiran, SK Huntemann, M Wei, CL Han, J Detter, JC Han, C Erkkila, TH Teshima, H Chen, A Kyrpides, N Mavrommatis, K Markowitz, V Szeto, E Ivanova, N Pagani, I Pati, A Goodwin, L Peters, L Pitluck, S Lam, J McDonald, AI Dodsworth, JA Woyke, T Hedlund, BP AF Murugapiran, Senthil K. Huntemann, Marcel Wei, Chia-Lin Han, James Detter, J. C. Han, Cliff Erkkila, Tracy H. Teshima, Hazuki Chen, Amy Kyrpides, Nikos Mavrommatis, Konstantinos Markowitz, Victor Szeto, Ernest Ivanova, Natalia Pagani, Ioanna Pati, Amrita Goodwin, Lynne Peters, Lin Pitluck, Sam Lam, Jenny McDonald, Austin I. Dodsworth, Jeremy A. Woyke, Tanja Hedlund, Brian P. TI Thermus oshimai JL-2 and T. thermophilus JL-18 genome analysis illuminates pathways for carbon, nitrogen, and sulfur cycling SO STANDARDS IN GENOMIC SCIENCES LA English DT Article DE Thermus; Thermus oshimai; Thermus thermophilus; thermophiles; hot springs; denitrification; nitrous oxide; Great Basin ID HOT-SPRINGS; NITRATE RESPIRATION; EXTREME THERMOPHILE; GREAT-BASIN; DISSIMILATORY REDUCTION; WOLINELLA-SUCCINOGENES; ELECTRON-ACCEPTORS; NITRITE REDUCTASE; DNA TRANSPORT; COMB-NOV AB The complete genomes of Thermus oshimai JL-2 and T. thermophilus JL-18 each consist of a circular chromosome, 2.07 Mb and 1.9 Mb, respectively, and two plasmids ranging from 0.27 Mb to 57.2 kb. Comparison of the T. thermophilus JL-18 chromosome with those from other strains of T. thermophilus revealed a high degree of synteny, whereas the megaplasmids from the same strains were highly plastic. The T. oshimai JL-2 chromosome and megaplasmids shared little or no synteny with other sequenced Thermus strains. Phylogenomic analyses using a concatenated set of conserved proteins confirmed the phylogenetic and taxonomic assignments based on 16S rRNA phylogenetics. Both chromosomes encode a complete glycolysis, tricarboxylic acid (TCA) cycle, and pentose phosphate pathway plus glucosidases, glycosidases, proteases, and peptidases, highlighting highly versatile heterotrophic capabilities. Megaplasmids of both strains contained a gene cluster encoding enzymes predicted to catalyze the sequential reduction of nitrate to nitrous oxide; however, the nitrous oxide reductase required for the terminal step in denitrification was absent, consistent with their incomplete denitrification phenotypes. A sox gene cluster was identified in both chromosomes, suggesting a mode of chemolithotrophy. In addition, nrf and psr gene clusters in T. oshmai JL-2 suggest respiratory nitrite ammonification and polysulfide reduction as possible modes of anaerobic respiration. C1 [Murugapiran, Senthil K.; Lam, Jenny; McDonald, Austin I.; Dodsworth, Jeremy A.; Hedlund, Brian P.] Univ Nevada Las Vegas, Sch Life Sci, Las Vegas, NV 89154 USA. [Huntemann, Marcel; Wei, Chia-Lin; Han, James; Chen, Amy; Kyrpides, Nikos; Mavrommatis, Konstantinos; Markowitz, Victor; Szeto, Ernest; Ivanova, Natalia; Pagani, Ioanna; Pati, Amrita; Peters, Lin; Pitluck, Sam; Woyke, Tanja] Joint Genome Inst, Dept Energy, Walnut Creek, CA USA. [Detter, J. C.; Han, Cliff; Erkkila, Tracy H.; Teshima, Hazuki; Goodwin, Lynne] Los Alamos Natl Lab, Los Alamos, NM USA. RP Murugapiran, SK (reprint author), Univ Nevada Las Vegas, Sch Life Sci, Las Vegas, NV 89154 USA. RI Kyrpides, Nikos/A-6305-2014 OI Kyrpides, Nikos/0000-0002-6131-0462 FU Office of Science of the US Department of Energy [DE-AC02-05CH11231]; NSF [MCB-0546865, EPS-9977809]; Greg Fullmer through the UNLV Foundation 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 under Contract No. DE-AC02-05CH11231. Additional support was supported by NSF Grant Numbers MCB-0546865 and EPS-9977809. We are also grateful for support from Greg Fullmer through the UNLV Foundation. NR 72 TC 9 Z9 9 U1 3 U2 14 PU GENOMIC STAND CONSORT PI EAST LANSING PA MICHIGAN STATE UNIV, GEEO GARRITY, DEPT MICROBIOL, 6162 BIOMED & PHYS SCI BLDG, EAST LANSING, MI 48824 USA SN 1944-3277 J9 STAND GENOMIC SCI JI Stand. Genomic Sci. PY 2013 VL 7 IS 3 BP 449 EP 468 DI 10.4056/sigs.3667269 PG 20 WC Genetics & Heredity; Microbiology SC Genetics & Heredity; Microbiology GA 203VY UT WOS:000323323500009 PM 24019992 ER PT J AU Bollmann, A Sedlacek, CJ Norton, J Laanbroek, HJ Suwa, Y Stein, LY Klotz, MG Arp, D Sayavedra-Soto, L Lu, M Bruce, D Detter, C Tapia, R Han, J Woyke, T Lucas, SM Pitluck, S Pennacchio, L Nolan, M Land, ML Huntemann, M Deshpande, S Han, C Chen, A Kyrpides, N Mavromatis, K Markowitz, V Szeto, E Ivanova, N Mikhailova, N Pagani, I Pati, A Peters, L Ovchinnikova, G Goodwin, LA AF Bollmann, Annette Sedlacek, Christopher J. Norton, Jeanette Laanbroek, Hendrikus J. Suwa, Yuichi Stein, Lisa Y. Klotz, Martin G. Arp, Daniel Sayavedra-Soto, Luis Lu, Megan Bruce, David Detter, Chris Tapia, Roxanne Han, James Woyke, Tanja Lucas, Susan M. Pitluck, Sam Pennacchio, Len Nolan, Matt Land, Miriam L. Huntemann, Marcel Deshpande, Shweta Han, Cliff Chen, Amy Kyrpides, Nikos Mavromatis, Konstantinos Markowitz, Victor Szeto, Ernest Ivanova, Natalia Mikhailova, Natalia Pagani, Ioanna Pati, Amrita Peters, Lin Ovchinnikova, Galina Goodwin, Lynne A. TI Complete genome sequence of Nitrosomonas sp. Is79, an ammonia oxidizing bacterium adapted to low ammonium concentrations SO STANDARDS IN GENOMIC SCIENCES LA English DT Article DE Nitrosomonas; Ammonia-oxidizing bacteria; Ammonia oxidation; nitrification; nitrogen cycle; freshwater; oligotrophic ID DIFFERENT SENSITIVITIES; KDP-ATPASE; RNA GENES; NOV-SP; EUROPAEA; NICHE; MODEL; PROTEOBACTERIA; MULTIFORMIS; EXPRESSION AB Nitrosomonas sp. Is79 is a chemolithoautotrophic ammonia-oxidizing bacterium that belongs to the family Nitrosomonadaceae within the phylum Proteobacteria. Ammonia oxidation is the first step of nitrification, an important process in the global nitrogen cycle ultimately resulting in the production of nitrate. Nitrosomonas sp. Is79 is an ammonia oxidizer of high interest because it is adapted to low ammonium and can be found in freshwater environments around the world. The 3,783,444-bp chromosome with a total of 3,553 protein coding genes and 44 RNA genes was sequenced by the DOE-Joint Genome Institute Program CSP 2006. C1 [Bollmann, Annette; Sedlacek, Christopher J.] Miami Univ, Oxford, OH 45056 USA. [Norton, Jeanette] Utah State Univ, Logan, UT 84322 USA. [Laanbroek, Hendrikus J.] Netherlands Inst Ecol, Wageningen, Netherlands. [Suwa, Yuichi] Chuo Univ, Tokyo 112, Japan. [Stein, Lisa Y.] Univ Alberta, Edmonton, AB, Canada. [Klotz, Martin G.] Univ N Carolina, Charlotte, NC 28223 USA. [Arp, Daniel; Sayavedra-Soto, Luis] Oregon State Univ, Corvallis, OR 97331 USA. [Lu, Megan; Bruce, David; Detter, Chris; Tapia, Roxanne; Han, Cliff; Goodwin, Lynne A.] Los Alamos Natl Lab, Biosci Div, Los Alamos, NM USA. [Han, James; Woyke, Tanja; Lucas, Susan M.; Pitluck, Sam; Pennacchio, Len; Nolan, Matt; Huntemann, Marcel; Deshpande, Shweta; Chen, Amy; Kyrpides, Nikos; Mavromatis, Konstantinos; Markowitz, Victor; Szeto, Ernest; Ivanova, Natalia; Mikhailova, Natalia; Pagani, Ioanna; Pati, Amrita; Peters, Lin; Ovchinnikova, Galina] DOE Joint Genome Inst, Walnut Creek, CA USA. [Land, Miriam L.] Oak Ridge Natl Lab, Oak Ridge, TN USA. RP Bollmann, A (reprint author), Miami Univ, Oxford, OH 45056 USA. RI Norton, Jeanette/G-2633-2011; Land, Miriam/A-6200-2011; Klotz, Martin/D-2091-2009; Laanbroek, Hendrikus J./C-3830-2008; Stein, Lisa/E-6374-2016; Kyrpides, Nikos/A-6305-2014; OI Norton, Jeanette/0000-0002-6596-8691; Land, Miriam/0000-0001-7102-0031; Klotz, Martin/0000-0002-1783-375X; Laanbroek, Hendrikus J./0000-0003-2400-3399; Stein, Lisa/0000-0001-5095-5022; Kyrpides, Nikos/0000-0002-6131-0462; Sedlacek, Christopher/0000-0002-6002-4982 FU Department of Energy Joint Genome Institute (DOE-JGI) Community Sequencing Program; Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]; NSF Research Coordination Network grant (Nitrification Network) [0541797] FX This research was funded by a grant of the Department of Energy Joint Genome Institute (DOE-JGI) Community Sequencing Program 2006 to JMN. 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. The collaborative project was supported by NSF Research Coordination Network grant 0541797 (Nitrification Network). NR 66 TC 9 Z9 10 U1 7 U2 46 PU GENOMIC STAND CONSORT PI EAST LANSING PA MICHIGAN STATE UNIV, GEEO GARRITY, DEPT MICROBIOL, 6162 BIOMED & PHYS SCI BLDG, EAST LANSING, MI 48824 USA SN 1944-3277 J9 STAND GENOMIC SCI JI Stand. Genomic Sci. PY 2013 VL 7 IS 3 BP 469 EP 482 DI 10.4056/sigs.3517166 PG 14 WC Genetics & Heredity; Microbiology SC Genetics & Heredity; Microbiology GA 203VY UT WOS:000323323500010 PM 24019993 ER PT S AU Torrontegui, E Ibanez, S Martinez-Garaot, S Modugno, M del Campo, A Guery-Odelin, D Ruschhaupt, A Chen, X Muga, JG AF Torrontegui, Erik Ibanez, Sara Martinez-Garaot, Sofia Modugno, Michele del Campo, Adolfo Guery-Odelin, David Ruschhaupt, Andreas Chen, Xi Gonzalo Muga, Juan BE Arimondo, E Berman, PR Lin, CC TI Shortcuts to Adiabaticity SO ADVANCES IN ATOMIC, MOLECULAR, AND OPTICAL PHYSICS, VOL 62 SE Advances In Atomic Molecular and Optical Physics LA English DT Review; Book Chapter ID BOSE-EINSTEIN CONDENSATE; MULTIMODE WAVE-GUIDES; TIME-DEPENDENT TRAPS; POPULATION TRANSFER; MODE CONVERSION; GEOMETRIC PHASE; WIGNER FUNCTION; HARMONIC TRAPS; QUANTUM STATES; DYNAMICS AB Quantum adiabatic processes that keep constant the populations in the instantaneous eigenbasis of a time-dependent Hamiltonian are very useful to prepare and manipulate states, but take typically a long time. This is often problematic because decoherence and noise may spoil the desired final state, or because some applications require many repetitions. "Shortcuts to adiabaticity" are alternative fast processes which reproduce the same final populations, or even the same final state, as the adiabatic process in a finite, shorter time. Since adiabatic processes are ubiquitous, the shortcuts span a broad range of applications in atomic, molecular, and optical physics, such as fast transport of ions or neutral atoms, internal population control, and state preparation (for nuclear magnetic resonance or quantum information), cold atom expansions and other manipulations, cooling cycles, wavepacket splitting, and many-body state engineering or correlations microscopy. Shortcuts are also relevant to clarify fundamental questions such as a precise quantification of the third principle of thermodynamics and quantum speed limits. We review different theoretical techniques proposed to engineer the shortcuts, the experimental results, and the prospects. C1 [Torrontegui, Erik; Ibanez, Sara; Martinez-Garaot, Sofia; Chen, Xi; Gonzalo Muga, Juan] Univ Basque Country, Dept Quim Fis, Euskal Herriko Unibertsitatea, E-48080 Bilbao, Spain. [Modugno, Michele] Univ Basque Country, Dept Fis Teor & Hist Ciencia, Euskal Herriko Unibertsitatea, E-48080 Bilbao, Spain. [Modugno, Michele] Basque Fdn Sci, IKERBASQUE, Bilbao 48011, Spain. [del Campo, Adolfo] Los Alamos Natl Lab, Div Theoret, Los Alamos, NM USA. [del Campo, Adolfo] Los Alamos Natl Lab, Ctr Nonlinear Studies, Los Alamos, NM 87545 USA. [Guery-Odelin, David] Univ Toulouse 3, Lab Collis Agregats React, CNRS UMR 5589, IRSAMC, F-31062 Toulouse 4, France. [Ruschhaupt, Andreas] Natl Univ Ireland Univ Coll Cork, Dept Phys, Cork, Ireland. [Chen, Xi; Gonzalo Muga, Juan] Shanghai Univ, Dept Phys, Shanghai 200444, Peoples R China. RP Torrontegui, E (reprint author), Univ Basque Country, Dept Quim Fis, Euskal Herriko Unibertsitatea, Apdo 644, E-48080 Bilbao, Spain. RI Guery-Odelin, David/G-6311-2012; del Campo, Adolfo/B-8439-2009; Modugno, Michele/A-6218-2009 OI del Campo, Adolfo/0000-0003-2219-2851; Modugno, Michele/0000-0002-0532-1423 NR 167 TC 174 Z9 175 U1 11 U2 68 PU ELSEVIER ACADEMIC PRESS INC PI SAN DIEGO PA 525 B STREET, SUITE 1900, SAN DIEGO, CA 92101-4495 USA SN 1049-250X BN 978-0-12-408090-4 J9 ADV ATOM MOL OPT PHY JI Adv. Atom. Mol. Opt. Phys. PY 2013 VL 62 BP 117 EP 169 DI 10.1016/B978-0-12-408090-4.00002-5 PG 53 WC Optics; Physics, Atomic, Molecular & Chemical SC Optics; Physics GA BGI23 UT WOS:000323088400003 ER PT S AU Young, AL Kemme, SA Wendt, JR Carter, TR Samora, S AF Young, A. L. Kemme, S. A. Wendt, J. R. Carter, T. R. Samora, S. BE Hasan, ZU Hemmer, PR Lee, H Santori, CM TI High Numerical Aperture Diffractive Optical Elements for Neutral Atom Quantum Computing SO ADVANCES IN PHOTONICS OF QUANTUM COMPUTING, MEMORY, AND COMMUNICATION VI SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Advances in Photonics of Quantum Computing, Memory, and Communication VI CY FEB 04-07, 2013 CL San Francisco, CA SP SPIE DE diffractive optical elements; large numerical aperture; quantum computing; quantum information processing; neutral atom trapping; scalability ID MICROSCOPIC DIPOLE TRAP; BOTTLE BEAM TRAP; SINGLE ATOMS; ARRAYS AB The viability of neutral atom based quantum computers is dependent upon scalability to large numbers of qubits. Diffractive optical elements (DOEs) offer the possibility to scale up to many qubit systems by enabling the manipulation of light to collect signal or deliver a tailored spatial trapping pattern. DOEs have an advantage over refractive micro-optics since they do not have measurable surface sag, making significantly larger numerical apertures (NA) accessible with a smaller optical component. The smaller physical size of a DOE allows the micro-lenses to be placed in vacuum with the atoms, reducing aberration effects that would otherwise be introduced by the cell walls of the vacuum chamber. The larger collection angle accessible with DOEs enable faster quantum computation speeds. We have designed a set of DOEs for collecting the 852 nm fluorescence from the D2 transition in trapped cesium atoms, and compare these DOEs to several commercially available refractive micro-lenses. The largest DOE is able to collect over 20% of the atom's radiating sphere whereas the refractive micro-optic is able to collect just 8% of the atom's radiating sphere. C1 [Young, A. L.; Kemme, S. A.; Wendt, J. R.; Carter, T. R.; Samora, S.] Sandia Natl Labs, Albuquerque, NM 87111 USA. RP Young, AL (reprint author), Sandia Natl Labs, Albuquerque, NM 87111 USA. NR 25 TC 0 Z9 0 U1 1 U2 8 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9404-7 J9 PROC SPIE PY 2013 VL 8635 AR 86350L DI 10.1117/12.2005388 PG 12 WC Optics; Physics, Multidisciplinary SC Optics; Physics GA BGH35 UT WOS:000322965700009 ER PT J AU Hsieh, WC Collins, WD Liu, Y Chiang, JCH Shie, CL Caldeira, K Cao, L AF Hsieh, W. -C. Collins, W. D. Liu, Y. Chiang, J. C. H. Shie, C. -L. Caldeira, K. Cao, L. TI Climate response due to carbonaceous aerosols and aerosol-induced SST effects in NCAR community atmospheric model CAM3.5 SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID CIRCULATION; MONSOON; SATELLITE; IMPACTS; CLOUDS; CYCLE AB This study used the Community Atmospheric Model 3.5 (CAM3.5) to investigate the effects of carbonaceous aerosols on climate. The simulations include control runs with 3 times the mass of carbonaceous aerosols as compared to the model's default carbonaceous aerosol mass, as well as no-carbon runs in which carbonaceous aerosols were removed. The slab ocean model (SOM) and the fixed sea surface temperature (SST) were used to examine effects of ocean boundary conditions. Throughout this study, climate response induced by aerosol forcing was mainly analyzed in the following three terms: (1) aerosol radiative effects under fixed SST, (2) effects of aerosol-induced SST feedbacks, and (3) total effects including effects of aerosol forcing and SST feedbacks. The change of SST induced by aerosols has large impacts on distribution of climate response; the magnitudes in response patterns such as temperature, precipitation, zonal winds, mean meridional circulation, radiative fluxes, and cloud coverage are different between the SOM and fixed SST runs. Moreover, different spatial responses between the SOM and fixed SST runs can also be seen in some local areas. This implies the importance of SST feedbacks on simulated climate response. The aerosol dimming effects cause a cooling predicted at low layers near the surface in most carbonaceous aerosol source regions. The temperature response shows a warming (cooling) predicted in the north (south) high latitudes, suggesting that aerosol forcing can cause climate change in regions far away from its origins. Our simulation results show that direct and semidirect radiative forcing due to carbonaceous aerosols decreases rainfall in the tropics. This implies that carbonaceous aerosols have possibly strong influence on weakening of the tropical circulation. Most changes in precipitation are negatively correlated with changes of radiative fluxes at the top of model. The changes in radiative fluxes at top of model are physically consistent with the response patterns in cloud fields. On global average, low-level cloud coverage increases, and mid-and high-level cloud coverage decreases in response to changes in radiative energy induced by aerosol forcing. An approximated moisture budget equation was analyzed in order to understand physical mechanism of precipitation changes induced by carbonaceous aerosols. Our results show that changes in tropical precipitation are mainly dominated are mainly dominated by the dynamic effect (i.e., vertical moisture transport carried by the perturbed flow). C1 [Hsieh, W. -C.; Collins, W. D.] Univ Calif Berkeley, Dept Earth & Planetary Sci, Berkeley, CA 94720 USA. [Collins, W. D.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Liu, Y.; Chiang, J. C. H.] Univ Calif Berkeley, Dept Geog, Berkeley, CA 94720 USA. [Liu, Y.; Chiang, J. C. H.] Univ Calif Berkeley, Berkeley Atmospher Sci Ctr, Berkeley, CA 94720 USA. [Shie, C. -L.] Univ Maryland Baltimore Cty, Joint Ctr Earth Syst Technol, Baltimore, MD 21228 USA. [Caldeira, K.] Carnegie Inst Sci, Dept Global Ecol, Stanford, CA 94305 USA. [Cao, L.] Zhejiang Univ, Dept Earth Sci, Hangzhou 310027, Zhejiang, Peoples R China. RP Hsieh, WC (reprint author), Univ Calif Berkeley, Dept Earth & Planetary Sci, Berkeley, CA 94720 USA. EM hsiehweichun@gmail.com RI Collins, William/J-3147-2014; Caldeira, Ken/E-7914-2011 OI Collins, William/0000-0002-4463-9848; FU Contractor Supporting Research (CSR); Berkeley Lab; Office of Science, of the US Department of Energy [DE-AC02-05CH11231]; National Science Foundation Science and Technology Center for Multiscale Modeling of Atmospheric Processes, CMMAP [ATM-0425247]; NSF FX This work was supported by Contractor Supporting Research (CSR) funding from Berkeley Lab, provided by the director, Office of Science, of the US Department of Energy under contract no. DE-AC02-05CH11231. This material is also supported by the National Science Foundation Science and Technology Center for Multiscale Modeling of Atmospheric Processes, CMMAP, managed by Colorado State University under cooperative agreement no. ATM-0425247. The National Center for Atmospheric Research is sponsored by the NSF. We would also like to acknowledge support for high-performance computing provided by NCAR's Computational and Information Systems Laboratory, sponsored by the NSF. We thank the editors for their comments and the reviewers for their suggestions, which largely improved the content of this paper. NR 30 TC 7 Z9 7 U1 3 U2 12 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1680-7316 J9 ATMOS CHEM PHYS JI Atmos. Chem. Phys. PY 2013 VL 13 IS 15 BP 7489 EP 7510 DI 10.5194/acp-13-7489-2013 PG 22 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA 200XE UT WOS:000323103900015 ER PT J AU Takahashi, Y Furukawa, T Kanai, Y Uematsu, M Zheng, G Marcus, MA AF Takahashi, Y. Furukawa, T. Kanai, Y. Uematsu, M. Zheng, G. Marcus, M. A. TI Seasonal changes in Fe species and soluble Fe concentration in the atmosphere in the Northwest Pacific region based on the analysis of aerosols collected in Tsukuba, Japan SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID IRON SOLUBILITY; CHEMICAL-CHARACTERIZATION; ANTHROPOGENIC SOURCES; STABILITY-CONSTANTS; FINE PARTICLES; MINERAL DUST; SPECIATION; TRANSPORT; OCEAN; SPECTROSCOPY AB Atmospheric iron (Fe) can be a significant source of nutrition for phytoplankton inhabiting remote oceans, which in turn has a large influence on the Earth's climate. The bioavailability of Fe in aerosols depends mainly on the fraction of soluble Fe (=[Fe-Sol]/[Fe-Total], where [FeSol] and [FeTotal] are the atmospheric concentrations of soluble and total Fe, respectively). However, the numerous factors affecting the soluble Fe fraction have not been fully understood. In this study, the Fe species, chemical composition, and soluble Fe concentrations in aerosols collected in Tsukuba, Japan were investigated over a year (nine samples from December 2002 to October 2003) to identify the factors affecting the amount of soluble Fe supplied into the ocean. The soluble Fe concentration in aerosols is correlated with those of sulfate and oxalate originated from anthropogenic sources, suggesting that soluble Fe is mainly derived from anthropogenic sources. Moreover, the soluble Fe concentration is also correlated with the enrichment factors of vanadium and nickel emitted by fossil fuel combustion. These results suggest that the degree of Fe dissolution is influenced by the magnitude of anthropogenic activity, such as fossil fuel combustion. X-ray absorption fine structure (XAFS) spectroscopy was performed in order to identify the Fe species in aerosols. Fitting of XAFS spectra coupled with micro X-ray fluorescence analysis (mu-XRF) showed the main Fe species in aerosols in Tsukuba to be illite, ferrihydrite, hornblende, and Fe(III) sulfate. Moreover, the soluble Fe fraction in each sample measured by leaching experiments is closely correlated with the Fe(III) sulfate fraction determined by the XAFS spectrum fitting, suggesting that Fe(III) sulfate is the main soluble Fe in the ocean. Another possible factor that can control the amount of soluble Fe supplied into the ocean is the total Fe(III) concentration in the atmosphere, which was high in spring due to the high mineral dust concentrations during spring in East Asia. However, this factor does not contribute to the amount of soluble Fe to a larger degree than the effect of Fe speciation, or more strictly speaking the presence of Fe(III) sulfate. Therefore, based on these results, the most significant factor influencing the amount of soluble Fe in the North Pacific region is the concentration of anthropogenic Fe species such as Fe(III) sulfate that can be emitted from megacities in Eastern Asia. C1 [Takahashi, Y.; Furukawa, T.] Hiroshima Univ, Grad Sch Sci, Dept Earth & Planetary Syst Sci, Hiroshima 7398526, Japan. [Takahashi, Y.; Uematsu, M.] Univ Tokyo, Atmosphere & Ocean Res Inst, Kashiwa, Chiba 2778564, Japan. [Takahashi, Y.; Zheng, G.] Chinese Acad Sci, Key Lab Petr Resources, Lanzhou 730000, Peoples R China. [Kanai, Y.] Natl Inst Adv Ind Sci & Technol, Geol Survey Japan, Tsukuba, Ibaraki 3058567, Japan. [Marcus, M. A.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. RP Takahashi, Y (reprint author), Hiroshima Univ, Grad Sch Sci, Dept Earth & Planetary Syst Sci, Hiroshima 7398526, Japan. EM ytakaha@hiroshima-u.ac.jp RI Takahashi, Yoshio/F-6733-2011 FU Director of the Office of Science, Office of Basic Energy Sciences, US Department of Energy [DE-AC02-05CH11231]; Chinese Academy of Sciences Visiting Professorship for Senior International Scientists [2012T1Z0035]; National Natural Science Foundation of China [41273112] FX We are grateful to H. Kamioka, S. Yabuki, and A. Ohta for collecting the aerosol samples for the ADEC project. This research was supported by a Grant-in-Aid for Scientific Research in Priority Areas, "Western Pacific Air-Sea Interaction Study (W-PASS)." This work was performed with the approval of KEK-PF (2011G197, 2011G644, and 2012G111) and SPring-8 (2012A1240 and 2002B1428). This research is a contribution to the Surface Ocean Lower Atmosphere Study (SOLAS). The operations of the Advanced Light Source at the Lawrence Berkeley National Laboratory are supported by the Director of the Office of Science, Office of Basic Energy Sciences, US Department of Energy under contract number DE-AC02-05CH11231. This study was also partially supported by Chinese Academy of Sciences Visiting Professorship for Senior International Scientists (Grant No. 2012T1Z0035) and National Natural Science Foundation of China (No. 41273112). NR 66 TC 11 Z9 11 U1 6 U2 37 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1680-7316 EI 1680-7324 J9 ATMOS CHEM PHYS JI Atmos. Chem. Phys. PY 2013 VL 13 IS 15 BP 7695 EP 7710 DI 10.5194/acp-13-7695-2013 PG 16 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA 200XE UT WOS:000323103900027 ER PT J AU Jin, HJ Daly, DS Marks, JR Zangar, RC AF Jin, Hongjun Daly, Don S. Marks, Jeffrey R. Zangar, Richard C. TI Oxidatively modified proteins as plasma biomarkers in breast cancer SO CANCER BIOMARKERS LA English DT Article DE Breast cancer; biomarkers; reactive oxygen species; protein adducts; hydroxynonenal; glutathione; plasma ID MAMMARY EPITHELIAL-CELLS; GROWTH-FACTOR RECEPTOR; CARCINOGENESIS; MICROARRAYS; AUTOCRINE; OXIDANTS; PROMAT; TOOL AB BACKGROUND: Post-translational protein modifications (PTMs) are increased in breast tumors. OBJECTIVE: We explored whether PTMs on proteins secreted by the breast could be detected in plasma and potentially used for the early detection of breast cancer. METHODS: We used a custom ELISA microarray platform to measure 4-hydroxynonenal (HNE), glutathione (GSH), nitrotyrosine and halotyrosine adducts in 27 secreted proteins, for a total of 108 candidate biomarkers. Two independent sets of human plasma samples were measured, for a total of 160 samples. The results were analyzed for consistent cancer-associated changes across the two sample sets. Plasma samples for both cases and benign controls were collected at the time of tissue diagnosis after referral from a positive screen (such as mammography). The results from both studies were evaluated using ANOVA and t-tests or receiver operator curves (ROC). RESULTS: Levels of GSH-modified ceruloplasmin and HNE-modified PDGF were significantly altered in plasma samples from cancer patients relative to benign controls. Healthy controls, which were only included in the first set of samples, were similar to the benign controls for both of these markers. A combination of three glutathionylated proteins produced the best area under the ROC curve, with a value of 76%. CONCLUSIONS: Specific PTMs in individual proteins may be useful for distinguishing between women with breast cancer and those with benign breast disease. These oxidative changes in plasma proteins may reflect redox changes in breast cancer. Additional studies on oxidative modifications in individual proteins are warranted. C1 [Jin, Hongjun; Daly, Don S.; Zangar, Richard C.] Pacific NW Natl Lab, Richland, WA 99352 USA. [Jin, Hongjun] Washington Univ, Sch Med, Div Radiol Sci, St Louis, MO USA. [Marks, Jeffrey R.] Duke Univ, Med Ctr, Dept Surg, Durham, NC 27710 USA. RP Zangar, RC (reprint author), Pacific NW Natl Lab, POB 999, Richland, WA 99352 USA. EM richard.zangar@pnnl.gov FU NIH [U01 CA117378, UO1 CA084955]; US Department of Defense BCRP Postdoctoral Fellowship [W81XWH-10-1-0031] FX This research was supported by NIH U01 CA117378 (RCZ), NIH UO1 CA084955 (JRM), and a US Department of Defense BCRP Postdoctoral Fellowship W81XWH-10-1-0031 (HJ). NR 31 TC 3 Z9 3 U1 0 U2 2 PU IOS PRESS PI AMSTERDAM PA NIEUWE HEMWEG 6B, 1013 BG AMSTERDAM, NETHERLANDS SN 1574-0153 EI 1875-8592 J9 CANCER BIOMARK JI Cancer Biomark. PY 2013 VL 13 IS 3 BP 193 EP 200 DI 10.3233/CBM-130349 PG 8 WC Oncology SC Oncology GA 195QQ UT WOS:000322719100008 PM 23912491 ER PT J AU Britt, D AF Britt, David TI Comment on "Nickel nanoparticles catalyse reversible hydration of carbon dioxide for mineralization carbon capture and storage" by G. Bhaduri and L. Siller, Catal. Sci. Technol., 2013, 3, 1234 SO CATALYSIS SCIENCE & TECHNOLOGY LA English DT Editorial Material C1 Lawrence Berkeley Natl Lab, Berkeley, CA 94530 USA. RP Britt, D (reprint author), Lawrence Berkeley Natl Lab, 1 Cyclotron Rd, Berkeley, CA 94530 USA. EM DavidKBritt@gmail.com NR 2 TC 3 Z9 3 U1 5 U2 28 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 9 BP 2195 EP 2196 DI 10.1039/c3cy00142c PG 2 WC Chemistry, Physical SC Chemistry GA 196MR UT WOS:000322780200003 ER PT J AU Lu, J Martinez-Macias, C Aydin, C Browning, ND Gates, BC AF Lu, Jing Martinez-Macias, Claudia Aydin, Ceren Browning, Nigel D. Gates, Bruce C. TI Zeolite-supported bimetallic catalyst: controlling selectivity of rhodium complexes by nearby iridium complexes SO CATALYSIS SCIENCE & TECHNOLOGY LA English DT Article ID DEALUMINATED Y-ZEOLITE; CHEMISTRY; HYDROGENATION; ISOMERIZATION; SPECTROSCOPY; SPILLOVER; STRATEGY; CLUSTERS; ALUMINA; MGO AB Rh(C2H4)(2) complexes supported on HY zeolite selectively catalyze ethylene dimerization in the presence of H-2, but iridium complexes anchored near the rhodium alter the selectivity by spilling over hydrogen that limits the adsorption of ethylene on Al-OH sites that act in concert with the rhodium sites, thereby triggering the rhodium complexes to operate as hydrogenation rather than dimerization catalysts. C1 [Lu, Jing; Martinez-Macias, Claudia; Aydin, Ceren; Browning, Nigel D.; Gates, Bruce C.] Univ Calif Davis, Dept Chem Engn & Mat Sci, Davis, CA 95616 USA. [Browning, Nigel D.] Pacific NW Natl Lab, Fundamental & Computat Sci Div, Richland, WA 99352 USA. RP Lu, J (reprint author), Univ Calif Davis, Dept Chem Engn & Mat Sci, Davis, CA 95616 USA. EM bcgates@ucdavis.edu RI ID, MRCAT/G-7586-2011; OI Browning, Nigel/0000-0003-0491-251X FU Department of Energy (DOE), Office of Science, Basic Energy Sciences [DE-FG02-04ER15513, DE-FG02-03ER46057]; University of California Lab Fee Program; UC MEXUS-CONACYT doctoral fellowship program FX This work was supported by the Department of Energy (DOE), Office of Science, Basic Energy Sciences, Grant Nos. DE-FG02-04ER15513 (J.L. and C.M.M.) and DE-FG02-03ER46057 (C.A.), and the University of California Lab Fee Program. C.M.M was partially supported by the UC MEXUS-CONACYT doctoral fellowship program. We acknowledge beam time and the support of the DOE Division of Materials Sciences for its role in the operation and development of beamline MR-CAT at the Advanced Photon Source at Argonne National Laboratory. We thank the beamline staff for valuable support. NR 36 TC 5 Z9 5 U1 1 U2 17 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 9 BP 2199 EP 2203 DI 10.1039/c3cy00113j PG 5 WC Chemistry, Physical SC Chemistry GA 196MR UT WOS:000322780200005 ER PT J AU Hoffert, WA Roberts, JAS Bullock, RM Helm, ML AF Hoffert, Wesley A. Roberts, John A. S. Bullock, R. Morris Helm, Monte L. TI Production of H-2 at fast rates using a nickel electrocatalyst in water-acetonitrile solutions SO CHEMICAL COMMUNICATIONS LA English DT Article ID HYDROGEN-PRODUCTION; CATALYTIC RATES; PENDANT AMINES; ACTIVE-SITE; COMPLEXES; COBALT; OXIDATION; GENERATION; REDUCTION AB We report a synthetic nickel complex containing proton relays, [Ni((P2N2C6H4OH)-N-Ph)(2)](BF4)(2) ((P2N2C6H4OH)-N-Ph = 1,5-bis(p-hydroxyphenyl)-3,7- diphenyl-1,5-diaza-3,7-diphosphacyclo-octane), that catalyzes the production of H-2 in aqueous acetonitrile with turnover frequencies of 750-170 000 s(-1) at experimentally determined overpotentials of 310-470 mV. C1 [Hoffert, Wesley A.; Roberts, John A. S.; Bullock, R. Morris; Helm, Monte L.] Pacific NW Natl Lab, Div Phys Sci, Ctr Mol Electrocatalysis, Richland, WA 99352 USA. RP Helm, ML (reprint author), Pacific NW Natl Lab, Div Phys Sci, Ctr Mol Electrocatalysis, POB 999K2-57, Richland, WA 99352 USA. EM Monte.Helm@pnnl.gov RI Bullock, R. Morris/L-6802-2016 OI Bullock, R. Morris/0000-0001-6306-4851 FU Center for Molecular Electrocatalysis, an Energy Frontier Research Center; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences FX We thank Dr Jonathan M. Darmon and Dr Charles J. Weiss for their assistance with the graphical abstract. This research was supported as part of the Center for Molecular Electrocatalysis, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences. Pacific Northwest National Laboratory is operated by Battelle for the U.S. Department of Energy. NR 31 TC 38 Z9 38 U1 2 U2 37 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1359-7345 EI 1364-548X J9 CHEM COMMUN JI Chem. Commun. PY 2013 VL 49 IS 71 BP 7767 EP 7769 DI 10.1039/c3cc43203c PG 3 WC Chemistry, Multidisciplinary SC Chemistry GA 198IF UT WOS:000322915200001 PM 23743801 ER PT J AU Grubbs, RB Sun, Z AF Grubbs, Robert B. Sun, Zhe TI Shape-changing polymer assemblies SO CHEMICAL SOCIETY REVIEWS LA English DT Review ID SPHERE-TO-ROD; AMPHIPHILIC BLOCK-COPOLYMERS; TRIBLOCK COPOLYMER; AQUEOUS-SOLUTIONS; MICELLE TRANSITION; WORMLIKE MICELLES; MEMORY POLYMERS; CANCER-THERAPY; OXIDE) BLOCK; NANOPARTICLES AB A panoply of stimuli-sensitive polymorphic polymer assemblies has been constructed through the intentional synthesis of amphiphilic block copolymers comprising hydrophilic, stimulus-responsive, and hydrophobic blocks. Transformations among canonical micellar forms of polymer assemblies-spherical micelles, wormlike micelles, and vesicles (polymersomes)-have been demonstrated with a number of synthetic systems. This review discusses recent progress in the development and understanding of these systems with a focus on open questions about kinetics of shape change, effects of block copolymer architecture on the rate and nature of the transformation, and potential applications. C1 [Grubbs, Robert B.; Sun, Zhe] SUNY Stony Brook, Dept Chem, Stony Brook, NY 11794 USA. [Grubbs, Robert B.] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. RP Grubbs, RB (reprint author), SUNY Stony Brook, Dept Chem, Stony Brook, NY 11794 USA. EM robert.grubbs@stonybrook.edu FU NSF [DMR-1105622] FX The NSF (DMR-1105622) is acknowledged for partial financial support of the work from our group described in this review. NR 69 TC 31 Z9 31 U1 5 U2 150 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 17 BP 7436 EP 7445 DI 10.1039/c3cs60079c PG 10 WC Chemistry, Multidisciplinary SC Chemistry GA 196NQ UT WOS:000322782700022 PM 23801143 ER PT J AU Rumberger, EMW Ahn, HS Bell, AT Tilley, TD AF Rumberger, Evan M. W. Ahn, Hyun S. Bell, Alexis T. Tilley, T. Don TI Water oxidation catalysis via immobilization of the dimanganese complex [Mn-2(mu-O)(2)Cl(mu-O2CCH3)-(bpy)(2)(H2O)](NO3)(2) onto silica SO DALTON TRANSACTIONS LA English DT Article ID OXYGEN-EVOLVING COMPLEX; SOLAR-ENERGY CONVERSION; O BOND FORMATION; PHOTOSYSTEM-II; ELECTRONIC-STRUCTURE; MANGANESE CATALASE; FUNCTIONAL-MODEL; ARTIFICIAL PHOTOSYNTHESIS; RENEWABLE ENERGY; CLAY COMPOUNDS AB Adsorption of a dinuclear mu-oxo bridged Mn complex onto mesoporous silica was observed when SBA15 was treated with an acetonitrile solution of [Mn-2(mu-O)(2)Cl(mu-O2CCH3)(H2O)(bpy)(2)](NO3)(2) (1). This complex was immobilized via the displacement of NO3- into solution, and characterization by spectroscopic (DRIFTS and DRUV-vis) and magnetic data indicates that the intact dication is electrostatically bound to the silica surface. Loadings of up to 4.1% by weight of [Mn-2(mu-O)(2)Cl(mu-O2CCH3)(H2O)(bpy)(2)](2+) were achieved. TEM images of the grafted material revealed retention of the mesoporous structure of SBA15, and no clusters of manganese greater than ca. 10 nm were observed. The SBA15-supported dimanganese complex functions as a catalyst for the oxidation of H2O with (NH4)(2)Ce(NO3)(6) as stoichiometric oxidant. In contrast, homogenous aqueous solutions of 1 do not evolve oxygen upon treatment with (NH4)(2)Ce(NO3)(6). Labeling studies with (H2O)-O-18 confirm that the oxygen formed in this catalysis is derived from water. Monitoring the O-2 evolution allowed determination of an initial rate for the catalysis (TOFi = 1.1 x 10(-3) s(-1)). These studies also reveal a first order dependence on manganese surface concentration, and a zero order rate dependence for (NH4)Ce(NO3)(6). Spectroscopic investigations were employed to investigate the difference in activities between dissolved and supported dimanganese complexes. C1 [Rumberger, Evan M. W.; Ahn, Hyun S.; Bell, Alexis T.; Tilley, T. Don] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Rumberger, Evan M. W.; Ahn, Hyun S.; Bell, Alexis T.; Tilley, T. Don] Univ Calif Berkeley, Dept Chem Engn, Berkeley, CA 94720 USA. [Rumberger, Evan M. W.; Ahn, Hyun S.; Bell, Alexis T.; Tilley, T. Don] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. RP Bell, AT (reprint author), Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. EM bell@cchem.berkeley.edu; tdtilley@berkeley.edu FU 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 . NR 71 TC 6 Z9 6 U1 2 U2 32 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 34 BP 12238 EP 12247 DI 10.1039/c3dt51472b PG 10 WC Chemistry, Inorganic & Nuclear SC Chemistry GA 196MP UT WOS:000322780000023 PM 23861177 ER PT J AU Garsany, Y Epshteyn, A More, KL Swider-Lyons, KE AF Garsany, Yannick Epshteyn, Albert More, Karren L. Swider-Lyons, Karen E. TI Oxygen Electroreduction on Nanoscale Pt/[TaOPO4/VC] and Pt/[Ta2O5/VC] in Alkaline Electrolyte SO ECS ELECTROCHEMISTRY LETTERS LA English DT Article ID ROTATING-DISC ELECTRODE; TANTALUM OXYPHOSPHATE; PLATINUM-ELECTRODES; REDUCTION ACTIVITY; ELECTROCATALYSIS; CATALYSTS; NANOPARTICLES; SURFACES; CARBON; MEDIA AB The ORR on Pt in an alkaline electrolyte is studied for the impact of support effects. Platinum nanoparticles are supported on nanoscale tantalum oxyphosphate or tantalum oxide films on Vulcan carbon (VC) to make either Pt/[TaOPO4/VC] or Pt/[Ta2O5/VC] electrocatalysts, which were then characterized with BF-STEM. Their ORR activity was determined by RDE methodology in 0.10 M KOH electrolyte. The Pt mass activities of the Pt/[TaOPO4/VC] and Pt/[Ta2O5/VC] electrocatalysts are both approximately 250 mA mg(Pt)(-1) at 0.925 V, or about 2 x greater than that of a commercial Pt/VC electrocatalyst (120 mA mg(Pt)(-1)), implying a substantial effect of the Ta-based support films. (c) 2013 The Electrochemical Society. All rights reserved. C1 [Garsany, Yannick] Excet Inc, Springfield, VA 22151 USA. [Garsany, Yannick; Epshteyn, Albert; Swider-Lyons, Karen E.] US Naval Res Lab, Washington, DC 20375 USA. [More, Karren L.] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. RP Garsany, Y (reprint author), Excet Inc, Springfield, VA 22151 USA. EM yannick.garsany.ctr.fr@nrl.navy.mil RI More, Karren/A-8097-2016 OI More, Karren/0000-0001-5223-9097 FU Office of Naval Research; Oak Ridge National Laboratory's Shared Research Equipment (ShaRE) User Facility; Office of Basic Energy Sciences, the U.S. Department of Energy FX The authors are grateful to the Office of Naval Research for financial support of this project. Electron microscopy was supported by Oak Ridge National Laboratory's Shared Research Equipment (ShaRE) User Facility, which is sponsored by the Office of Basic Energy Sciences, the U.S. Department of Energy. NR 20 TC 2 Z9 2 U1 3 U2 12 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 2162-8726 J9 ECS ELECTROCHEM LETT JI ECS Electrochem. Lett. PY 2013 VL 2 IS 10 BP H46 EP H50 DI 10.1149/2.012310eel PG 5 WC Electrochemistry; Materials Science, Multidisciplinary SC Electrochemistry; Materials Science GA 199JW UT WOS:000322991800012 ER PT S AU Peters, DW Boye, RR Kemme, SA AF Peters, David W. Boye, Robert R. Kemme, Shanalyn A. BE ChangHasnain, CJ Koyama, F Willner, AE Zhou, W TI Angular sensitivity of guided mode resonant filters in classical and conical mounts SO HIGH CONTRAST METASTRUCTURES II SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on High Contrast Metastructures II CY FEB 05-07, 2013 CL San Francisco, CA SP SPIE DE guided mode resonance; subwavelength; filter ID SUBWAVELENGTH GRATINGS; NARROW-BAND; BIOSENSORS AB The angular sensitivity of guided mode resonant filters (GMRF) is well known. While at times useful for angle tuning of the response, this sensitivity can also be a major detriment as angular changes of tenths of a degree can shift the wavelength response in a narrow bandwidth device by an amount greater than the width of the resonance peak. We identify geometries where the resonance is more angularly stable, demonstrating high reflectivity at the design wavelength for several degrees in both azimuth and inclination angular directions with virtually no change in lineshape of the response. The investigation of GMRFs in both classical and conical mounts through simulation using rigorous coupled wave analysis reveals that there are preferred mounts for greater angular tolerance. We simulate a grating at telecom wavelengths using a design that we have previously fabricated. The identical grating placed in different mounts can exhibit angular tolerances that differ by well over an order of magnitude (60x). The most commonly used classical mount has a much more sensitive angular tolerance than does the conical mount. The lineshape of the resonant response shows only negligible changes across the angular band. The angular band for the sample grating is simulated to be several degrees in the conical mount as opposed to a tenth of a degree in the classical mount. We could thus expand the application space for narrow-band GMRFs into areas where angular tolerance cannot be controlled to the degree that we have believed required in the past. C1 [Peters, David W.; Boye, Robert R.; Kemme, Shanalyn A.] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Peters, DW (reprint author), Sandia Natl Labs, POB 5800, Albuquerque, NM 87185 USA. NR 16 TC 3 Z9 3 U1 0 U2 4 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9402-3 J9 PROC SPIE PY 2013 VL 8633 AR 86330W DI 10.1117/12.2005122 PG 6 WC Optics; Physics, Multidisciplinary SC Optics; Physics GA BGH39 UT WOS:000322969400021 ER PT S AU Bingham, P Polsky, Y Anovitz, L AF Bingham, Philip Polsky, Yarom Anovitz, Lawrence BE Bingham, PR Lam, EY TI Neutron imaging for geothermal energy systems SO IMAGE PROCESSING: MACHINE VISION APPLICATIONS VI SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Image Processing - Machine Vision Applications VI CY FEB 05-06, 2013 CL Burlingame, CA SP Soc Imaging Sci & Technol (IS&T), SPIE, Qualcomm Inc DE Neutron radiography; Geothermal Energy ID RADIOGRAPHY AB Geothermal systems extract heat energy from the interior of the earth using a working fluid, typically water. Three components are required for a commercially viable geothermal system: heat, fluid, and permeability. Current commercial electricity production using geothermal energy occurs where the three main components exist naturally. These are called hydrothermal systems. In the US, there is an estimated 30 GW of base load electrical power potential for hydrothermal sites. Next generation geothermal systems, named Enhanced Geothermal Systems (EGS), have an estimated potential of 4500 GW. EGSs lack in-situ fluid, permeability or both. As such, the heat exchange system must be developed or "engineered" within the rock. The envisioned method for producing permeability in the EGS reservoir is hydraulic fracturing, which is rarely practiced in the geothermal industry, and not well understood for the rocks typically present in geothermal reservoirs. High costs associated with trial and error learning in the field have led to an effort to characterize fluid flow and fracturing mechanisms in the laboratory to better understand how to design and manage EGS reservoirs. Neutron radiography has been investigated for potential use in this characterization. An environmental chamber has been developed that is suitable for reproduction of EGS pressures and temperatures and has been tested for both flow and precipitations studies with success for air/liquid interface imaging and 3D reconstruction of precipitation within the core. C1 [Bingham, Philip; Polsky, Yarom; Anovitz, Lawrence] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. RP Bingham, P (reprint author), Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. RI Anovitz, Lawrence/P-3144-2016; OI Anovitz, Lawrence/0000-0002-2609-8750; Bingham, Philip/0000-0003-4616-6084 NR 4 TC 0 Z9 0 U1 0 U2 7 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9434-4 J9 PROC SPIE PY 2013 VL 8661 AR 86610K DI 10.1117/12.2004617 PG 8 WC Computer Science, Artificial Intelligence; Computer Science, Cybernetics; Optics; Imaging Science & Photographic Technology SC Computer Science; Optics; Imaging Science & Photographic Technology GA BFX76 UT WOS:000321820300018 ER PT S AU Dillard, SE Henry, MJ Bohn, S Gosink, LJ AF Dillard, Scott E. Henry, Michael J. Bohn, Shawn Gosink, Luke J. BE Bingham, PR Lam, EY TI Coherent Image Layout using an Adaptive Visual Vocabulary SO IMAGE PROCESSING: MACHINE VISION APPLICATIONS VI SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Image Processing - Machine Vision Applications VI CY FEB 05-06, 2013 CL Burlingame, CA SP Soc Imaging Sci & Technol (IS&T), SPIE, Qualcomm Inc DE Image Browsing; Hierarchical Clustering; Bag of Features AB When querying a huge image database containing millions of images, the result of the query may still contain many thousands of images that need to be presented to the user. We consider the problem of arranging such a large set of images into a visually coherent layout, one that places similar images next to each other. Image similarity is determined using a bag-of-features model, and the layout is constructed from a hierarchical clustering of the image set by mapping an in-order traversal of the hierarchy tree into a space-filling curve. This layout method provides strong locality guarantees so we are able to quantitatively evaluate performance using standard image retrieval benchmarks. Performance of the bag-of-features method is best when the vocabulary is learned on the image set being clustered. Because learning a large, discriminative vocabulary is a computationally demanding task, we present a novel method for efficiently adapting a generic visual vocabulary to a particular dataset. We evaluate our clustering and vocabulary adaptation methods on a variety of image datasets and show that adapting a generic vocabulary to a particular set of images improves performance on both hierarchical clustering and image retrieval tasks. C1 [Dillard, Scott E.; Henry, Michael J.; Bohn, Shawn; Gosink, Luke J.] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Henry, MJ (reprint author), Pacific NW Natl Lab, 902 Battelle Blvd, Richland, WA 99352 USA. EM michael.j.henry@pnnl.gov NR 33 TC 0 Z9 0 U1 1 U2 4 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9434-4 J9 PROC SPIE PY 2013 VL 8661 AR 86610Q DI 10.1117/12.2004733 PG 14 WC Computer Science, Artificial Intelligence; Computer Science, Cybernetics; Optics; Imaging Science & Photographic Technology SC Computer Science; Optics; Imaging Science & Photographic Technology GA BFX76 UT WOS:000321820300024 ER PT S AU Karakaya, M Barstow, D Santos-Villalobos, H Boehnen, C AF Karakaya, Mahmut Barstow, Del Santos-Villalobos, Hector Boehnen, Christopher BE Bingham, PR Lam, EY TI An Iris Segmentation Algorithm based on Edge Orientation for Off-angle Iris Recognition SO IMAGE PROCESSING: MACHINE VISION APPLICATIONS VI SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Image Processing - Machine Vision Applications VI CY FEB 05-06, 2013 CL Burlingame, CA SP Soc Imaging Sci & Technol (IS&T), SPIE, Qualcomm Inc DE Iris recognition; segmentation; biometrics; off-angle iris; edge orientation map; elliptical boundary AB Iris recognition is known as one of the most accurate and reliable biometrics. However, the accuracy of iris recognition systems depends on the quality of data capture and is negatively affected by several factors such as angle, occlusion, and dilation. In this paper, we present a segmentation algorithm for off-angle iris images that uses edge detection, edge elimination, edge classification, and ellipse fitting techniques. In our approach, we first detect all candidate edges in the iris image by using the canny edge detector; this collection contains edges from the iris and pupil boundaries as well as eyelash, eyelids, iris texture etc. Edge orientation is used to eliminate the edges that cannot be part of the iris or pupil. Then, we classify the remaining edge points into two sets as pupil edges and iris edges. Finally, we randomly generate subsets of iris and pupil edge points, fit ellipses for each subset, select ellipses with similar parameters, and average to form the resultant ellipses. Based on the results from real experiments, the proposed method shows effectiveness in segmentation for off-angle iris images. C1 [Karakaya, Mahmut; Barstow, Del; Santos-Villalobos, Hector; Boehnen, Christopher] Oak Ridge Natl Lab, Imaging Signals & Machine Learning Grp, Oak Ridge, TN 37831 USA. RP Karakaya, M (reprint author), Oak Ridge Natl Lab, Imaging Signals & Machine Learning Grp, Oak Ridge, TN 37831 USA. EM karakayam@ornl.gov NR 19 TC 0 Z9 0 U1 0 U2 2 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9434-4 J9 PROC SPIE PY 2013 VL 8661 AR 866108 DI 10.1117/12.2004444 PG 13 WC Computer Science, Artificial Intelligence; Computer Science, Cybernetics; Optics; Imaging Science & Photographic Technology SC Computer Science; Optics; Imaging Science & Photographic Technology GA BFX76 UT WOS:000321820300007 ER PT J AU Gundlach-Graham, A Dennis, EA Ray, SJ Enke, CG Barinaga, CJ Koppenaal, DW Hieftje, GM AF Gundlach-Graham, Alexander Dennis, Elise A. Ray, Steven J. Enke, Christie G. Barinaga, Charles J. Koppenaal, David W. Hieftje, Gary M. TI First inductively coupled plasma-distance-of-flight mass spectrometer: instrument performance with a microchannel plate/phosphor imaging detector SO JOURNAL OF ANALYTICAL ATOMIC SPECTROMETRY LA English DT Article ID CONSTANT MOMENTUM ACCELERATION; ION KINETIC ENERGIES; ISOTOPE RATIO; ELEMENTAL ANALYSIS; ICP-MS; SPECTROGRAPH; RESOLUTION; GEOMETRY; SENSITIVITY; CYTOMETRY AB Here we describe the first combination of a Distance-of-Flight Mass Spectrometry (DOFMS) instrument and an inductively coupled plasma (ICP) ion source. DOFMS is a velocity-based MS technique in which ions of a range of mass-to-charge (m/z) values are detected simultaneously along the length of a spatially selective detector. As a relative of time-of-flight (TOF) MS, DOFMS leverages benefits from both TOFMS and spatially dispersive MS. The simultaneous detection of groups of m/z values improves dynamic range by spreading ion signal across many detector elements and reduces correlated noise by signal ratioing. To ascertain the performance characteristics of the ICP-DOFMS instrument, we have employed a microchannel-plate/phosphor detection assembly with a scientific CCD to capture images of the phosphor plate. With this simple (and commercially available) detection scheme, elemental detection limits from 2-30 ng L-1 and a linear dynamic range of 5 orders of magnitude (10-10(6) ng L-1) have been demonstrated. Additionally, a competitive isotope-ratio precision of 0.1% RSD has been achieved with only a 6 s signal integration period. In addition to first figures of merit, this paper outlines technical considerations for the design of the ICP-DOFMS. C1 [Gundlach-Graham, Alexander; Dennis, Elise A.; Ray, Steven J.; Hieftje, Gary M.] Indiana Univ, Dept Chem, Bloomington, IN 47405 USA. [Enke, Christie G.] Univ New Mexico, Dept Chem, Albuquerque, NM 87131 USA. [Barinaga, Charles J.; Koppenaal, David W.] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Hieftje, GM (reprint author), Indiana Univ, Dept Chem, 800 E Kirkwood Ave, Bloomington, IN 47405 USA. EM alexgrah@indiana.edu RI Gundlach-Graham, Alexander/B-6069-2011; OI Gundlach-Graham, Alexander/0000-0003-4806-6255; Ray, Steven/0000-0001-5675-1258 FU Division of Analytical Chemistry (DAC) of the American Chemistry Society; Agilent Technologies; National Science Foundation [DBI-1062846]; US DOE by Battelle Memorial Institute [DE-AC06-76RLO-1830op]; U.S. Department of Energy [DE-FG02-09ER14980] FX The authors thank the instrument makers of the Edward Bair Mechanical Instrument Services at Indiana University for the construction of the DOFMS instrument. One author (A. G.-G.) also thanks the Division of Analytical Chemistry (DAC) of the American Chemistry Society and Agilent Technologies for sponsoring him with a DAC graduate-research fellowship. This research was supported in part by the National Science Foundation through Grant DBI-1062846 and performed in collaboration with Pacific Northwest National Laboratory, operated for the US DOE by Battelle Memorial Institute under Contract DE-AC06-76RLO-1830op. Partial salary support provided by the U.S. Department of Energy through grant DE-FG02-09ER14980. NR 63 TC 8 Z9 9 U1 1 U2 17 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 0267-9477 J9 J ANAL ATOM SPECTROM JI J. Anal. At. Spectrom. PY 2013 VL 28 IS 9 BP 1385 EP 1395 DI 10.1039/c3ja50122a PG 11 WC Chemistry, Analytical; Spectroscopy SC Chemistry; Spectroscopy GA 198KS UT WOS:000322922300004 ER PT J AU Steeb, JL Graczyk, DG Tsai, Y Mertz, CJ Essling, AM Sullivan, VS Carney, KP Finck, MR Giglio, JJ Chamberlain, DB AF Steeb, J. L. Graczyk, D. G. Tsai, Y. Mertz, C. J. Essling, A. M. Sullivan, V. S. Carney, K. P. Finck, M. R. Giglio, J. J. Chamberlain, D. B. TI Application of mass spectrometric isotope dilution methodology for Sr-90 age-dating with measurements by thermal-ionization and inductively coupled-plasma mass spectrometry SO JOURNAL OF ANALYTICAL ATOMIC SPECTROMETRY LA English DT Article ID DEAD-TIME; ICP-MS; RATIO MEASUREMENTS; BIAS; UNCERTAINTY; MODELS AB Application of an isotope-dilution method for determining Zr-90 and Sr-90 in a Sr-90 source material spiked with Sr-86 and Zr-92 is described. A miniature gas pressurized extraction chromatography (GPEC) system with a column containing Eichrom Sr Resin (TM) was used for separating the elements so isobaric isotopes could be measured by mass spectrometry. Zirconium was rinsed through the column with 3 M HNO3/trace HF and strontium was eluted with 1% acetic acid. Two mass spectrometric techniques, inductively coupled plasma mass spectrometry (ICP-MS) and thermal ionization mass spectrometry (TIMS), were used for measuring isotope ratios. Data were obtained with Sr-90 from a blood-irradiator source. Results from the TIMS measurements gave a decay time of 45.16 +/- 0.26 years, and those from the ICP-MS gave 45.24 +/- 0.20 years (uncertainties are expanded uncertainty, k = 2). Quadrupole ICP-MS is preferable to TIMS in this application if the ICP-MS data are suitably corrected for non-linearity and mass discrimination. C1 [Steeb, J. L.; Graczyk, D. G.; Tsai, Y.; Mertz, C. J.; Essling, A. M.; Sullivan, V. S.; Chamberlain, D. B.] Argonne Natl Lab, Lemont, IL USA. [Carney, K. P.; Finck, M. R.; Giglio, J. J.] Idaho Natl Lab, Idaho Falls, ID 83415 USA. RP Steeb, JL (reprint author), Argonne Natl Lab, 9700 S Cass Ave, Lemont, IL USA. EM steeb@anl.gov; kevin.carney@inl.gov OI Giglio, Jeffrey/0000-0002-0877-927X FU U.S. Department of Energy, Nuclear Energy Research and Development Program [W-31-109-ENG-38]; U.S. Department of Energy [DE-AC07-05ID14517, DE-AC02-06CH11357] FX The authors acknowledge the U.S. Department of Energy, Nuclear Energy Research and Development Program under Contract no. W-31-109-ENG-38 for funding. This manuscript has been authored by by UChicago Argonne, LLC, and Battelle Energy Alliance, LLC, under Contracts no. DE-AC07-05ID14517 and DE-AC02-06CH11357 with the U.S. Department of Energy. The United States Government retains a nonexclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. We would like to thank ORNL for providing the image of the Sr-90 blood irradiator. NR 25 TC 5 Z9 5 U1 1 U2 12 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 0267-9477 J9 J ANAL ATOM SPECTROM JI J. Anal. At. Spectrom. PY 2013 VL 28 IS 9 BP 1493 EP 1507 DI 10.1039/c3ja50136a PG 15 WC Chemistry, Analytical; Spectroscopy SC Chemistry; Spectroscopy GA 198KS UT WOS:000322922300017 ER PT J AU Wolpert, DH Bono, JW AF Wolpert, David H. Bono, James W. TI Predicting Behavior in Unstructured Bargaining with a Probability Distribution SO JOURNAL OF ARTIFICIAL INTELLIGENCE RESEARCH LA English DT Article ID NONCONVEX PROBLEMS; EXTENSION; ALTERNATIVES; FINITE AB In experimental tests of human behavior in unstructured bargaining games, typically many joint utility outcomes are found to occur, not just one. This suggests we predict the outcome of such a game as a probability distribution. This is in contrast to what is conventionally done (e.g, in the Nash bargaining solution), which is predict a single outcome. We show how to translate Nash's bargaining axioms to provide a distribution over outcomes rather than a single outcome. We then prove that a subset of those axioms forces the distribution over utility outcomes to be a power-law distribution. Unlike Nash's original result, our result holds even if the feasible set is finite. When the feasible set is convex and comprehensive, the mode of the power law distribution is the Harsanyi bargaining solution, and if we require symmetry it is the Nash bargaining solution. However, in general these modes of the joint utility distribution are not the experimentalist's Bayes-optimal predictions for the joint utility. Nor are the bargains corresponding to the modes of those joint utility distributions the modes of the distribution over bargains in general, since more than one bargain may result in the same joint utility. After introducing distributional bargaining solution concepts, we show how an external regulator can use them to optimally design an unstructured bargaining scenario. Throughout we demonstrate our analysis in computational experiments involving flight rerouting negotiations in the National Airspace System. We emphasize that while our results are formulated for unstructured bargaining, they can also be used to make predictions for noncooperative games where the modeler knows the utility functions of the players over possible outcomes of the game, but does not know the move spaces the players use to determine those outcomes. C1 [Wolpert, David H.] Santa Fe Inst, Santa Fe, NM 87501 USA. [Wolpert, David H.] Los Alamos Natl Lab, Informat Sci Grp, Los Alamos, NM 87545 USA. RP Wolpert, DH (reprint author), Santa Fe Inst, 1399 Hyde Pk Rd, Santa Fe, NM 87501 USA. EM DAVID.H.WOLPERT@GMAIL.COM; jwbono@gmail.com NR 38 TC 0 Z9 0 U1 0 U2 1 PU AI ACCESS FOUNDATION PI MARINA DEL REY PA USC INFORMATION SCIENCES INST, 4676 ADMIRALITY WAY, MARINA DEL REY, CA 90292-6695 USA SN 1076-9757 J9 J ARTIF INTELL RES JI J. Artif. Intell. Res. PY 2013 VL 46 BP 579 EP 605 PG 27 WC Computer Science, Artificial Intelligence SC Computer Science GA 199CZ UT WOS:000322973400001 ER PT J AU Pattyn, F Perichon, L Durand, G Favier, L Gagliardini, O Hindmarsh, RCA Zwinger, T Albrecht, T Cornford, S Docquier, D Furst, JJ Goldberg, D Gudmundsson, GH Humbert, A Hutten, M Huybrechts, P Jouvet, G Kleiner, T Larour, E Martin, D Morlighem, M Payne, AJ Pollard, D Ruckamp, M Rybak, O Seroussi, H Thoma, M Wilkens, N AF Pattyn, Frank Perichon, Laura Durand, Gael Favier, Lionel Gagliardini, Olivier Hindmarsh, Richard C. A. Zwinger, Thomas Albrecht, Torsten Cornford, Stephen Docquier, David Furst, Johannes J. Goldberg, Daniel Gudmundsson, G. Hilmar Humbert, Angelika Huetten, Moritz Huybrechts, Philippe Jouvet, Guillaume Kleiner, Thomas Larour, Eric Martin, Daniel Morlighem, Mathieu Payne, Anthony J. Pollard, David Rueckamp, Martin Rybak, Oleg Seroussi, Helene Thoma, Malte Wilkens, Nina TI Grounding-line migration in plan-view marine ice-sheet models: results of the ice2sea MISMIP3d intercomparison SO JOURNAL OF GLACIOLOGY LA English DT Article ID HIGHER-ORDER; PART 1; FLOW; DYNAMICS; SHELF; SENSITIVITY; ANTARCTICA; STABILITY AB Predictions of marine ice-sheet behaviour require models able to simulate grounding-line migration. We present results of an intercomparison experiment for plan-view marine ice-sheet models. Verification is effected by comparison with approximate analytical solutions for flux across the grounding line using simplified geometrical configurations (no lateral variations, no buttressing effects from lateral drag). Perturbation experiments specifying spatial variation in basal sliding parameters permitted the evolution of curved grounding lines, generating buttressing effects. The experiments showed regions of compression and extensional flow across the grounding line, thereby invalidating the boundary layer theory. Steady-state grounding-line positions were found to be dependent on the level of physical model approximation. Resolving grounding lines requires inclusion of membrane stresses, a sufficiently small grid size (<500 m), or subgrid interpolation of the grounding line. The latter still requires nominal grid sizes of <5 km. For larger grid spacings, appropriate parameterizations for ice flux may be imposed at the grounding line, but the short-time transient behaviour is then incorrect and different from models that do not incorporate grounding-line parameterizations. The numerical error associated with predicting grounding-line motion can be reduced significantly below the errors associated with parameter ignorance and uncertainties in future scenarios. C1 [Pattyn, Frank; Perichon, Laura; Docquier, David] Univ Libre Bruxelles, Lab Glaciol, Brussels, Belgium. [Durand, Gael; Favier, Lionel; Gagliardini, Olivier] UJF Grenoble I, CNRS, LGGE, Grenoble, France. [Gagliardini, Olivier] Inst Univ France, Paris, France. [Hindmarsh, Richard C. A.; Gudmundsson, G. Hilmar] British Antarctic Survey, Nat Environm Res Council, Cambridge CB3 0ET, England. [Zwinger, Thomas] CSC IT Ctr Sci Ltd, Espoo, Finland. [Albrecht, Torsten; Huetten, Moritz] Potsdam Inst Climate Impact Res, Potsdam, Germany. [Albrecht, Torsten; Huetten, Moritz] Univ Potsdam, Inst Phys, Potsdam, Germany. [Cornford, Stephen; Payne, Anthony J.] Univ Bristol, Sch Geog Sci, Bristol Glaciol Ctr, Bristol, Avon, England. [Furst, Johannes J.; Huybrechts, Philippe; Rybak, Oleg] Vrije Univ Brussel, Brussels, Belgium. [Furst, Johannes J.; Huybrechts, Philippe; Rybak, Oleg] Vrije Univ Brussel, Dept Geog, Brussels, Belgium. [Goldberg, Daniel] MIT, Dept Earth Atmospher & Planetary Sci, Cambridge, MA USA. [Humbert, Angelika; Rueckamp, Martin; Wilkens, Nina] Univ Hamburg, Inst Geophys IfG, Hamburg, Germany. [Humbert, Angelika; Kleiner, Thomas; Thoma, Malte] Alfred Wegener Inst Polar & Marine Res, Bremerhaven, Germany. [Jouvet, Guillaume] Free Univ Berlin, Inst Math, Berlin, Germany. [Larour, Eric; Seroussi, Helene] CALTECH, Jet Prop Lab, Pasadena, CA USA. [Martin, Daniel] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Morlighem, Mathieu] Univ Calif Irvine, Dept Earth Syst Sci, Irvine, CA USA. [Pollard, David] Penn State Univ, Earth & Environm Syst Inst, University Pk, PA 16802 USA. RP Pattyn, F (reprint author), Univ Libre Bruxelles, Lab Glaciol, Brussels, Belgium. EM fpattyn@ulb.ac.be RI payne, antony/A-8916-2008; Rybak, Oleg/B-7308-2014; Hindmarsh, Richard/C-1405-2012; Morlighem, Mathieu/O-9942-2014; Kleiner, Thomas/F-6821-2015; OI Gudmundsson, Gudmundur Hilmar/0000-0003-4236-5369; payne, antony/0000-0001-8825-8425; Rybak, Oleg/0000-0003-3923-7163; Hindmarsh, Richard/0000-0003-1633-2416; Zwinger, Thomas/0000-0003-3360-4401; Morlighem, Mathieu/0000-0001-5219-1310; Kleiner, Thomas/0000-0001-7825-5765; Cornford, Stephen/0000-0002-2461-1645; Thoma, Malte/0000-0002-4033-3905; Cornford, Stephen/0000-0003-1844-274X; Pattyn, Frank/0000-0003-4805-5636 FU ice2sea project from the European Union 7th Framework Programme [226375]; NASA Cryospheric Sciences Program; NASA Modeling Analysis and Prediction Program; NASA FX This work was supported by funding from the ice2sea project from the European Union 7th Framework Programme, grant No. 226375. This is ice2sea contribution No. 112. LGGE was granted access to the high-performance computing resources of CINES (Centre Informatique National de l'Enseignement Superieur, France) under allocations 2011-016066 and 2012-016066 made by GENCI (Grand Equipement National de Calcul Intensif) to perform the Elmer/Ice simulations. E. Larour and M. Morlighem are supported by the NASA Cryospheric Sciences and Modeling Analysis and Prediction Programs. H. Seroussi was supported by an appointment to the NASA Postdoctoral Program at the Jet Propulsion Laboratory, administered by Oak Ridge Associated Universities through a contract with NASA. We wish to acknowledge the helpful comments of J. Johnson and F. Saito, as well as the Scientific Editor R. Greve. NR 52 TC 60 Z9 61 U1 1 U2 33 PU CAMBRIDGE UNIV PRESS PI CAMBRIDGE PA EDINBURGH BLDG, SHAFTESBURY RD, CB2 8RU CAMBRIDGE, ENGLAND SN 0022-1430 EI 1727-5652 J9 J GLACIOL JI J. Glaciol. PY 2013 VL 59 IS 215 BP 410 EP 422 DI 10.3189/2013JoG12J129 PG 13 WC Geography, Physical; Geosciences, Multidisciplinary SC Physical Geography; Geology GA 202BX UT WOS:000323189600002 ER PT J AU Liu, XF Majzoub, EH Stavila, V Bhakta, RK Allendorf, MD Shane, DT Conradi, MS Verdal, N Udovic, TJ Hwang, SJ AF Liu, Xiangfeng Majzoub, Eric H. Stavila, Vitalie Bhakta, Raghunandan K. Allendorf, Mark D. Shane, David T. Conradi, Mark S. Verdal, Nina Udovic, Terrence J. Hwang, Son-Jong TI Probing the unusual anion mobility of LiBH4 confined in highly ordered nanoporous carbon frameworks via solid state NMR and quasielastic neutron scattering SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID HYDROGEN STORAGE PROPERTIES; COMPLEX HYDRIDES; RECENT PROGRESS; THERMODYNAMICS; DECOMPOSITION; NANOPARTICLES; NAALH4; SPECTROMETER; DYNAMICS; KINETICS AB Particle size and particle-framework interactions have profound effects on the kinetics, reaction pathways, and even thermodynamics of complex hydrides incorporated in frameworks possessing nanoscale features. Tuning these properties may hold the key to the utilization of complex hydrides in practical applications for hydrogen storage. Using carefully synthesized, highly-ordered, nanoporous carbons (NPCs), we have previously shown quantitative differences in the kinetics and reaction pathways of LiBH4 when incorporated into the frameworks. In this paper, we probe the anion mobility of LiBH4 confined in NPC frameworks by a combination of solid state NMR and quasielastic neutron scattering (QENS) and present some new insights into the nanoconfinement effect. NMR and QENS spectra of LiBH4 confined in a 4 nm pore NPC suggest that the BH4- anions nearer the LiBH4-carbon pore interface exhibit much more rapid translational and reorientational motions compared to those in the LiBH4 interior. Moreover, an overly broadened BH4- torsional vibration band reveals a disorder-induced array of BH4- rotational potentials. XRD results are consistent with a lack of LiBH4 long-range order in the pores. Consistent with differential scanning calorimetry measurements, neither NMR nor QENS detects a clear solid-solid phase transition as observed in the bulk, indicating that borohydride-framework interactions and/or nanosize effects have large roles in confined LiBH4. C1 [Liu, Xiangfeng; Majzoub, Eric H.] Univ Missouri, Dept Phys & Astron, Ctr Nanosci, St Louis, MO 63121 USA. [Liu, Xiangfeng] Univ Chinese Acad Sci, Coll Mat Sci & Optoelect Technol, Beijing 10049, Peoples R China. [Stavila, Vitalie; Bhakta, Raghunandan K.; Allendorf, Mark D.] Sandia Natl Labs, Livermore, CA 94551 USA. [Shane, David T.; Conradi, Mark S.] Washington Univ, Dept Phys, St Louis, MO 63130 USA. [Verdal, Nina; Udovic, Terrence J.] NIST, NIST Ctr Neutron Res, Gaithersburg, MD 20899 USA. [Hwang, Son-Jong] CALTECH, Div Chem & Chem Engn, Pasadena, CA 91125 USA. RP Majzoub, EH (reprint author), Univ Missouri, Dept Phys & Astron, Ctr Nanosci, St Louis, MO 63121 USA. EM liuxf@ucas.ac.cn; majzoube@umsl.edu FU U.S. Department of Energy in the Hydrogen, Fuel Cells, and Infrastructure Technologies Program through the office Energy Efficiency and Renewable Energy; DOE-EERE [DE-EE0002978]; DOE Basic Energy Sciences [DE-FG02-05ER46256]; National Science Foundation (NSF) [DMR-0944772, 9724240]; MRSEC Program of the NSF [DMR-520565]; Hundred Talents Project; National Basic Research Program of China (973 Program) [2010CB833101] FX This work was funded by the U.S. Department of Energy in the Hydrogen, Fuel Cells, and Infrastructure Technologies Program through the office Energy Efficiency and Renewable Energy. This work utilized facilities supported in part by the National Science Foundation under Agreement DMR-0944772. This work was partially supported by DOE-EERE under Agreement no. DE-EE0002978. The work at Washington University was supported by DOE Basic Energy Sciences grant DE-FG02-05ER46256. The NMR facility at Caltech was supported by the National Science Foundation (NSF) under Grant Number 9724240 and partially supported by the MRSEC Program of the NSF under Award Number DMR-520565. The work at University of Chinese Academy of Sciences was supported by "Hundred Talents Project" and the National Basic Research Program of China (973 Program, 2010CB833101). NR 52 TC 17 Z9 17 U1 3 U2 43 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 34 BP 9935 EP 9941 DI 10.1039/c3ta12051a PG 7 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA 196RJ UT WOS:000322792900050 ER PT J AU Ding, WW Lin, JP Yao, KJ Mays, JW Ramanathan, M Hong, KL AF Ding, Weiwei Lin, Jiaping Yao, Kejian Mays, Jimmy W. Ramanathan, Muruganathan Hong, Kunlun TI Building triangular nanoprisms from the bottom-up: a polyelectrolyte micellar approach SO JOURNAL OF MATERIALS CHEMISTRY B LA English DT Article ID KINETICALLY CONTROLLED SYNTHESIS; POLY(VINYL PYRROLIDONE); LANGEVIN DYNAMICS; SHAPE EVOLUTION; CRYSTALLIZATION; NANOSTRUCTURES; MINERALIZATION; NANOPARTICLES; AGGREGATION; TEMPLATE AB Charge-regulated synthesis of triangular prisms in aqueous solution using self-assembled polyelectrolyte micelles as templates is described in detail. Micelles formed from amphiphilic polystyrene-block-sulfonated poly(1,3-cyclohexadiene) (PS-b-sPCHD) serve as templates to direct the formation of novel triangular prisms of CuCl2 single crystals. We demonstrate that the edge lengths of these triangular prisms can be easily tailored at room temperature from the nanoscale to the mesoscale by simply adjusting the ratio of charged micelles to protons in the solution. This approach can be extended to the preparation of different ordered crystal structures with a precision hard to achieve via other approaches. C1 [Ding, Weiwei; Lin, Jiaping; Yao, Kejian] E China Univ Sci & Technol, Sch Mat Sci & Engn, State Key Lab Bioreactor Engn,Key Lab Ultrafine M, Minist Educ,Shanghai Key Lab Adv Polymer Mat, Shanghai 200237, Peoples R China. [Mays, Jimmy W.] Univ Tennessee, Dept Chem, Knoxville, TN 37996 USA. [Mays, Jimmy W.] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. [Ramanathan, Muruganathan; Hong, Kunlun] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. RP Lin, JP (reprint author), E China Univ Sci & Technol, Sch Mat Sci & Engn, State Key Lab Bioreactor Engn,Key Lab Ultrafine M, Minist Educ,Shanghai Key Lab Adv Polymer Mat, Shanghai 200237, Peoples R China. EM jlin@ecust.edu.cn; hongkq@ornl.gov RI Yao, Kejian/A-7486-2014; LIN, Jiaping/A-8734-2012; Hong, Kunlun/E-9787-2015 OI Hong, Kunlun/0000-0002-2852-5111 FU National Science Foundation of China [50673026, 20574018]; Doctoral Foundation of Education Ministry of China [20050251008]; Projects of Shanghai Municipality [B502, 06SU07002, 0652nm021, 082231]; Oak Ridge National Laboratory by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy FX This work was supported by the National Science Foundation of China (50673026, 20574018) and Doctoral Foundation of Education Ministry of China (Grant no. 20050251008), and Projects of Shanghai Municipality (B502, 06SU07002, 0652nm021, and 082231) are also acknowledged. A portion of this research was conducted at the Center for Nanophase Materials Sciences, which is sponsored at Oak Ridge National Laboratory by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy. NR 29 TC 7 Z9 7 U1 0 U2 26 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-750X J9 J MATER CHEM B JI J. Mat. Chem. B PY 2013 VL 1 IS 34 BP 4212 EP 4216 DI 10.1039/c3tb20765j PG 5 WC Materials Science, Biomaterials SC Materials Science GA 198IP UT WOS:000322916400002 ER PT J AU Lin, LQ Crew, E Yan, H Shan, SY Skeete, Z Mott, D Krentsel, T Yin, J Chernova, NA Luo, J Engelhard, MH Wang, CM Li, QB Zhong, CJ AF Lin, Liqin Crew, Elizabeth Yan, Hong Shan, Shiyao Skeete, Zakiya Mott, Derrick Krentsel, Tatiana Yin, Jun Chernova, Natasha A. Luo, Jin Engelhard, Mark H. Wang, Chongmin Li, Qingbiao Zhong, Chuan-Jian TI Bifunctional nanoparticles for SERS monitoring and magnetic intervention of assembly and enzyme cutting of DNAs SO JOURNAL OF MATERIALS CHEMISTRY B LA English DT Article ID ENHANCED RAMAN-SCATTERING; CORE-SHELL NANOPARTICLES; IRON-OXIDE NANOPARTICLES; GOLD NANOPARTICLES; SILVER NANOPARTICLES; SEPARATION; NANOPROBES; PATHOGENS; PROTEIN; PROBES AB The ability to harness the nanoscale structural properties is essential for the exploration of functional properties of nanomaterials. This report demonstrates a novel strategy exploring bifunctional nanoparticles for spectroscopic detection and magnetic intervention of DNA assembly, disassembly, and enzyme cutting processes in a solution phase. In contrast to existing single-function based approaches, this strategy exploits magnetic MnZn ferrite nanoparticles decorated with gold or silver on the surface to retain adequate magnetization while producing sufficient plasmonic resonance features to impart surface-enhanced Raman scattering (SERS) functions. The decoration of MnZn ferrite nanoparticles with Au or Ag (MZF/Au or MZF/Ag) was achieved by thermally activated deposition of Au or Ag atoms/nanoparticles on MZF nanoparticles. Upon interparticle double-stranded DNA linkage of the MZF/Au (or MZF/Ag) nanoparticles with gold nanoparticles labeled with a Raman reporter, the resulting interparticle "hot spots" are shown to enable real time SERS monitoring of the DNA assembly, disassembly, or enzyme cutting processes, where the magnetic component provides an effective means for intervention of the biomolecular processes in the solution. The unique bifunctional combination of the SERS "hot spots" and the magnetic separation capability serves as the first example of bifunctional nanoprobes for biomolecular recognition and intervention. C1 [Lin, Liqin; Crew, Elizabeth; Yan, Hong; Shan, Shiyao; Skeete, Zakiya; Krentsel, Tatiana; Yin, Jun; Chernova, Natasha A.; Luo, Jin; Zhong, Chuan-Jian] SUNY Binghamton, Dept Chem, Binghamton, NY 13902 USA. [Lin, Liqin; Li, Qingbiao] Xiamen Univ, Coll Environm & Ecol, Environm Sci Res Ctr, Xiamen 361005, Peoples R China. [Mott, Derrick] Japan Adv Inst Sci & Technol, Sch Mat Sci, Nomi, Ishikawa 9231292, Japan. [Engelhard, Mark H.; Wang, Chongmin] Pacific NW Natl Lab, EMSL, Richland, WA 99352 USA. RP Lin, LQ (reprint author), SUNY Binghamton, Dept Chem, Binghamton, NY 13902 USA. EM cjzhong@binghamton.edu RI Li, QB/G-4616-2010; Yan, Hong/D-1937-2014; Zhong, Chuan-Jian/D-3394-2013 OI Engelhard, Mark/0000-0002-5543-0812; FU National Science Foundation [CHE 0848701, CMMI 1100736]; National Natural Science Foundation of China [21036004]; DOE FX This work is supported by the National Science Foundation (CHE 0848701, CMMI 1100736) and in part by the National Natural Science Foundation of China (no. 21036004). The XPS and part of TEM measurements were performed using EMSL, a national scientific user facility sponsored by the DOE and located at PNNL. NR 53 TC 13 Z9 13 U1 3 U2 49 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-750X J9 J MATER CHEM B JI J. Mat. Chem. B PY 2013 VL 1 IS 34 BP 4320 EP 4330 DI 10.1039/c3tb20446d PG 11 WC Materials Science, Biomaterials SC Materials Science GA 198IP UT WOS:000322916400016 ER PT J AU Hellerich, ES Intemann, JJ Cai, M Liu, R Ewan, MD Tlach, BC Jeffries-EL, M Shinar, R Shinar, J AF Hellerich, Emily S. Intemann, Jeremy J. Cai, Min Liu, Rui Ewan, Monique D. Tlach, Brian C. Jeffries-EL, Malika Shinar, Ruth Shinar, Joseph TI Fluorescent polymer guest:small molecule host solution-processed OLEDs SO JOURNAL OF MATERIALS CHEMISTRY C LA English DT Article ID LIGHT-EMITTING-DIODES; HIGH-EFFICIENCY; ELECTROPHOSPHORESCENT DEVICES; TRANSPORTING MATERIALS; ENERGY-TRANSFER; PERFORMANCE; SINGLE; LAYER; MOBILITY AB Solution-processed OLEDs with polymer hosts and polymer or small-molecule guests have been studied extensively. More recently, efficient solution-processed OLEDs with small molecule hosts and small molecule guests were also reported. However, small molecule hosts of polymer guests in solution-processed fluorescent OLEDs have not been investigated. In this work guest: host systems consisting of the small molecule 4,4'-bis(9-carbazolyl)-biphenyl (CBP) as host to polymer guests such as novel benzobisoxazole (BBO)-containing copolymers and well-known poly(2-methoxy-5-(2'-ethyl-hexyloxy)1,4-phenylene vinylene) (MEH-PPV) are compared to those with poly(N-vinyl carbazole) (PVK) host, which previously yielded highly efficient phosphorescent OLEDs. In the case of MEH-PPV, guest: host OLEDs are also compared to those with a neat MEH-PPV emitting layer. It is found that replacing the polymer host PVK with the small molecule host CBP improves efficiencies by up to 100%. A blue emissive BBO-polymer: CBP device reaches a luminous efficiency (eta(L,max)) of 3.4 cd A(-1) (external quantum efficiency eta(ext) = 2.4%), while the PVK-based device exhibits eta(L,max) 1.7 cd A(-1) (eta(ext) = 1.2%). A green emissive BBO:CBP OLED exhibits eta(L,max) = 5.7 cd A(-1) (eta(ext) = 2.1%), while that in the PVK host is 3.1 cd A(-1) (eta(ext) = 1.1%). For MEH-PPV: CBP these values are 3.7 cd A(-1) (eta(ext) = 1.4%), compared to 2.9 cd A(-1) (eta(ext) = 1.0%) for MEH-PPV:PVK and 0.7 cd A(-1) (eta(ext) = 0.4%) for the neat MEH-PPV device. Possible origins of the improvement are discussed, including increased charge mobility, smoother film morphology, and the potential effect of multiple non-coiling host small molecules (in contrast to the likely coiled PVK) surrounding a polymer guest. C1 [Hellerich, Emily S.; Cai, Min; Liu, Rui; Shinar, Joseph] US DOE, Ames Lab, Ames, IA 50011 USA. [Hellerich, Emily S.; Cai, Min; Liu, Rui; Shinar, Joseph] Iowa State Univ, Dept Phys & Astron, Ames, IA 50011 USA. [Intemann, Jeremy J.; Ewan, Monique D.; Tlach, Brian C.; Jeffries-EL, Malika] Iowa State Univ, Dept Chem, Ames, IA 50011 USA. [Shinar, Ruth] Iowa State Univ, Microelect Res Ctr, Ames, IA 50011 USA. [Shinar, Ruth] Iowa State Univ, Dept Elect & Comp Engn, Ames, IA 50011 USA. RP Shinar, J (reprint author), US DOE, Ames Lab, Ames, IA 50011 USA. EM rshinar@iastate.edu; jshinar@iastate.edu RI Cai, Min/A-2678-2014 FU US Department of Energy (USDOE) [DE-AC 02-07CH11358]; Basic Energy Sciences, Division of Materials Science and Engineering, USDOE; National Science Foundation [DMR-0846607] FX Ames Laboratory is operated by Iowa State University for the US Department of Energy (USDOE) under Contract no. DE-AC 02-07CH11358. The research was partially supported by Basic Energy Sciences, Division of Materials Science and Engineering, USDOE. JJI, MDE, BCT and MJE thank the National Science Foundation (DMR-0846607) for partial support of this work. NR 35 TC 12 Z9 12 U1 4 U2 62 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7526 J9 J MATER CHEM C JI J. Mater. Chem. C PY 2013 VL 1 IS 34 BP 5191 EP 5199 DI 10.1039/c3tc31019a PG 9 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA 198HB UT WOS:000322911900002 ER PT J AU Kim, Y Kim, Y Han, H Jesse, S Hyun, S Lee, W Kalinin, SV Kim, JK AF Kim, Youngsuk Kim, Yunseok Han, Hee Jesse, Stephen Hyun, Seung Lee, Woo Kalinin, Sergei V. Kim, Jin Kon TI Towards the limit of ferroelectric nanostructures: switchable sub-10 nm nanoisland arrays SO JOURNAL OF MATERIALS CHEMISTRY C LA English DT Article ID BLOCK-COPOLYMER MICELLES; ULTRAHIGH-DENSITY ARRAY; THIN-FILMS; ULTRAFINE PARTICLES; DOMAIN-STRUCTURE; POLARIZATION; PBTIO3; SIZE; NANOPARTICLES; FABRICATION AB Ultrahigh density arrays of ferroelectric PbTiO3 (PTO) nanoislands with various feature sizes were epitaxially grown by utilizing block copolymer micelles. Piezoresponse and ferroelectric properties were clearly observed in the PTO nanoislands by band excitation piezoresponse force microscopy. In particular, PTO nanoislands were fully switchable even with a volume as small as 79 nm(3). Accordingly, it is expected that the volume of the switchable ferroelectric nanoislands can be further decreased. The obtained results show that an areal density of over 10 Tb in(-2) for the ferroelectric memory devices would be possible. C1 [Kim, Youngsuk; Hyun, Seung; Kim, Jin Kon] Pohang Univ Sci & Technol POSTECH, Natl Creat Res Initiat Ctr Block Copolymer Self A, Pohang 790784, Kyungbuk, South Korea. [Kim, Youngsuk; Hyun, Seung; Kim, Jin Kon] Pohang Univ Sci & Technol POSTECH, Dept Chem Engn, Pohang 790784, Kyungbuk, South Korea. [Kim, Yunseok; Jesse, Stephen; Kalinin, Sergei V.] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. [Kim, Yunseok] Sungkyunkwan Univ, Sch Adv Mat Sci & Engn, Suwon 440746, Gyeonggi Do, South Korea. [Han, Hee; Lee, Woo] KRISS, Taejon 305340, South Korea. RP Kim, JK (reprint author), Pohang Univ Sci & Technol POSTECH, Natl Creat Res Initiat Ctr Block Copolymer Self A, Pohang 790784, Kyungbuk, South Korea. EM yunseokkim@skku.edu; jkkim@postech.ac.kr RI Lee, Woo/B-5268-2008; Kalinin, Sergei/I-9096-2012; Jesse, Stephen/D-3975-2016 OI Lee, Woo/0000-0003-4560-8901; Kalinin, Sergei/0000-0001-5354-6152; Jesse, Stephen/0000-0002-1168-8483 FU National Creative Research Initiative Program; National Research Foundation of Korea (NRF); Center for Advanced Soft Electronics under the Global Frontier Research Program of the Ministry of Science, ICT & Future Planning, Korea [2011-0031635]; U.S. Department of Energy, Basic Energy Sciences, Materials Sciences and Engineering Division; Oak Ridge National Laboratory by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy; POSCO; NRF FX This research was supported by the National Creative Research Initiative Program supported by the National Research Foundation of Korea (NRF) and a grant (Code no. 2011-0031635) from the Center for Advanced Soft Electronics under the Global Frontier Research Program of the Ministry of Science, ICT & Future Planning, Korea. The research was also supported (S. V. K., Y.K.) by the U.S. Department of Energy, Basic Energy Sciences, Materials Sciences and Engineering Division. A portion of this research was conducted at the Center for Nanophase Materials Sciences (S. V. K.), which is sponsored at Oak Ridge National Laboratory by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy. XRD experiments were performed at PLS beamlines 3C2 and 10C1 supported by POSCO and NRF. NR 30 TC 7 Z9 7 U1 1 U2 27 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7526 J9 J MATER CHEM C JI J. Mater. Chem. C PY 2013 VL 1 IS 34 BP 5299 EP 5302 DI 10.1039/c3tc30971a PG 4 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA 198HB UT WOS:000322911900015 ER PT J AU Yeates, TO Jorda, J Bobik, TA AF Yeates, Todd O. Jorda, Julien Bobik, Thomas A. TI The Shells of BMC-Type Microcompartment Organelles in Bacteria SO JOURNAL OF MOLECULAR MICROBIOLOGY AND BIOTECHNOLOGY LA English DT Article DE Bacterial microcompartments; Carboxysome; Shell proteins ID B-12-DEPENDENT 1,2-PROPANEDIOL DEGRADATION; HALOTHIOBACILLUS-NEAPOLITANUS CARBOXYSOMES; SALMONELLA-TYPHIMURIUM LT2; PENTAMERIC VERTEX PROTEINS; THIOBACILLUS-NEAPOLITANUS; PDU MICROCOMPARTMENT; CARBONIC-ANHYDRASE; ESCHERICHIA-COLI; ETHANOLAMINE; ENTERICA AB Bacterial microcompartments are large proteinaceous structures that act as metabolic organelles in many bacterial cells. A shell or capsid, which is composed of a few thousand protein subunits, surrounds a series of sequentially acting enzymes and controls the diffusion of substrates and products into and out of the lumen. The carboxysome and the propanediol utilization microcompartment represent two well-studied systems among seven or more distinct types that can be delineated presently. Recent structural studies have highlighted a number of sophisticated mechanisms that underlie the function of bacterial microcompartment shell proteins. This review updates our understanding of bacterial microcompartment shells, how they are assembled, and how they carry out their functions in molecular transport and enzyme organization. Copyright (C) 2013 S. Karger AG, Basel C1 [Yeates, Todd O.] Univ Calif Los Angeles, Dept Chem & Biochem, Los Angeles, CA 90095 USA. [Jorda, Julien] Univ Calif Los Angeles, UCLA DOE Inst Genom & Prote, Los Angeles, CA 90095 USA. [Bobik, Thomas A.] Iowa State Univ, Dept Biochem Biophys & Mol Biol, Ames, IA USA. RP Yeates, TO (reprint author), Univ Calif Los Angeles, Dept Chem & Biochem, Los Angeles, CA 90095 USA. EM yeates@mbi.ucla.edu OI Yeates, Todd/0000-0001-5709-9839 FU NIAID NIH HHS [R01 AI081146] NR 58 TC 18 Z9 18 U1 0 U2 17 PU KARGER PI BASEL PA ALLSCHWILERSTRASSE 10, CH-4009 BASEL, SWITZERLAND SN 1464-1801 J9 J MOL MICROB BIOTECH JI J. Mol. Microbiol. Biotechnol. PY 2013 VL 23 IS 4-5 BP 290 EP 299 DI 10.1159/000351347 PG 10 WC Biotechnology & Applied Microbiology; Microbiology SC Biotechnology & Applied Microbiology; Microbiology GA 197YL UT WOS:000322888700004 PM 23920492 ER PT S AU Choi, J Cruz-Cabrera, AA Tanbakuchi, A AF Choi, Junoh Cruz-Cabrera, Alvaro A. Tanbakuchi, Anthony BE Maher, MA Resnick, PJ TI Practical Implementation of Broadband Diffractive Optical Elements SO MICROMACHINING AND MICROFABRICATION PROCESS TECHNOLOGY XVIII SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Micromachining and Microfabrication Process Technology XVIII CY FEB 05-07, 2013 CL San Francisco, CA SP SPIE, VUZIX Corp DE Diffractive optical element; broadband diffractive AB Diffractive optical elements (DOEs), with their thin profile and unique dispersion properties, have been studied and utilized in a number of optical systems, often yielding smaller and lighter systems. Despite the interest in and study of DOEs, the application of DOEs has been limited to narrow spectral bands. This is due to DOEs depths, which are optimized for optical path differences of only a single wavelength, consequently leading to rapid decline in efficiency as the working wavelength shifts away from the design wavelength. Various broadband DOE design methodologies have recently been developed that improve spectral diffraction efficiency and expand the working bandwidth of diffractive elements. Two such extended bandwidth diffractive designs have been modeled and fabricated. The diffraction efficiency test result for one broadband DOE design is presented. C1 [Choi, Junoh; Cruz-Cabrera, Alvaro A.; Tanbakuchi, Anthony] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Choi, J (reprint author), Sandia Natl Labs, POB 5800,MS 0406, Albuquerque, NM 87185 USA. NR 3 TC 1 Z9 1 U1 0 U2 1 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9381-1 J9 PROC SPIE PY 2013 VL 8612 AR 86120G DI 10.1117/12.2013204 PG 12 WC Optics; Physics, Applied SC Optics; Physics GA BGG96 UT WOS:000322910000013 ER PT J AU Vishnyakov, EA Voronov, DL Gullikson, EM Kondratenko, VV Kopylets, IA Luginin, MS Pirozhkov, AS Ragozin, EN Shatokhin, AN AF Vishnyakov, E. A. Voronov, D. L. Gullikson, E. M. Kondratenko, V. V. Kopylets, I. A. Luginin, M. S. Pirozhkov, A. S. Ragozin, E. N. Shatokhin, A. N. TI Normal-incidence Sb/B4C multilayer mirrors for the 80 angstrom < lambda < 120 angstrom wavelength range SO QUANTUM ELECTRONICS LA English DT Article DE soft X-ray range; multilayer mirrors; antimony; aperiodic structures; normal radiation incidence ID PLASMA RADIATION SOURCE; PULSED XENON-JET; X-RAY RADIATION; REFLECTION; SPECTROSCOPY; DISPERSION; OPTICS AB Periodic and aperiodic Sb/B4C multilayer structures have been theoretically calculated and synthesised for the first time for the application in soft X-ray optics in the 80 angstrom < lambda < 120 angstrom range. The reflection spectra of the periodic multilayer mirrors are measured using synchrotron radiation and laser plasma-generated radiation. The experimental spectra are theoretically interpreted with the inclusion of transition layers and substrate roughness. The density of antimony layers is supposedly rho(Sb) = 6.0 g cm(-3), and the thickness of transition layers (if any) in the Sb/B4C multilayer structures does not exceed 10 angstrom. A peak reflectivity of 19% is attained at a wavelength of 85 angstrom. An aperiodic mirror optimised for maximum uniform reflectivity in the 100 - 120 angstrom range is tested employing the laser plasma radiation source. C1 [Vishnyakov, E. A.; Luginin, M. S.; Ragozin, E. N.; Shatokhin, A. N.] State Univ, Moscow Inst Phys & Technol, Dolgoprudnyi 141700, Moscow Region, Russia. [Vishnyakov, E. A.; Ragozin, E. N.; Shatokhin, A. N.] Russian Acad Sci, PN Lebedev Phys Inst, Moscow 119991, Russia. [Voronov, D. L.; Gullikson, E. M.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Ctr Xray Opt, Berkeley, CA 94720 USA. [Kondratenko, V. V.; Kopylets, I. A.] Natl Tech Univ, Kharkov Polytech Inst, UA-61002 Kharkov, Ukraine. [Pirozhkov, A. S.] JAEA, Adv Beam Technol Div, Kizugawa, Kyoto 6190215, Japan. RP Vishnyakov, EA (reprint author), State Univ, Moscow Inst Phys & Technol, Inst Per 9, Dolgoprudnyi 141700, Moscow Region, Russia. EM juk301@mail.ru; enragozin@gmail.com RI Vishnyakov, Eugene/M-3106-2015; Ragozin, Eugene/M-3139-2015; Shatokhin, Alexey/C-3534-2016 FU 'Fundamental Optical Spectroscopy and its Applications' Programme of the Physical Sciences Division, RAS; Educational-Scientific Complex of the LPI FX The authors express their appreciation to N.N. Salashchenko and P.V. Sasorov for fruitful discussions. This work was supported by the 'Fundamental Optical Spectroscopy and its Applications' Programme of the Physical Sciences Division, RAS, and the Educational-Scientific Complex of the LPI. NR 38 TC 4 Z9 4 U1 0 U2 2 PU TURPION LTD PI BRISTOL PA C/O TURPION LTD, IOP PUBLISHING, TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6HG, ENGLAND SN 1063-7818 EI 1468-4799 J9 QUANTUM ELECTRON+ JI Quantum Electron. PY 2013 VL 43 IS 7 BP 666 EP 673 DI 10.1070/QE2013v043n07ABEH015128 PG 8 WC Engineering, Electrical & Electronic; Physics, Applied SC Engineering; Physics GA 196XJ UT WOS:000322810400013 ER PT J AU Wang, L Lei, HW Lee, J Chen, SL Tang, J Ahring, B AF Wang, Lu Lei, Hanwu Lee, John Chen, Shulin Tang, Juming Ahring, Birgitte TI Aromatic hydrocarbons production from packed-bed catalysis coupled with microwave pyrolysis of Douglas fir sawdust pellets SO RSC ADVANCES LA English DT Article ID BIO-OIL; ASSISTED PYROLYSIS; BIOMASS; FUEL; TEMPERATURE; CONVERSION; ZEOLITES; PHENOLS; REACTOR; ENERGY AB The direct catalytic cracking of biomass pyrolysis vapour into aromatics derived from Douglas fir sawdust pellets was tested using an upfront microwave pyrolysis process coupled with a packed-bed catalysis process using a ZSM-5 Zeolite catalyst. A central composite experimental design (CCD) was used to optimize the bio-oil and syngas yields. The effects of temperature and inverse weight hourly space velocity (WHSV)(-1) on the bio-oil composition were determined. The gas chromatography-mass spectrometry (GC-MS) analysis results showed that the bio-oil contained aromatic hydrocarbons. The aromatic hydrocarbons were enriched and became the most abundant compounds accounting for about 15-92.6% in upgraded bio-oils, depending on the catalytic pyrolysis conditions. The aromatic hydrocarbons were mainly composed of benzene, toluene, xylene, naphthalene, and their derivatives. When the effect of the reaction temperature on the bio-oil chemical compositions was analysed with a fixed (WHSV)(-1) (0.048 h), we found that the aromatic hydrocarbons increased from 0.72% in raw bio-oil (no catalyst added) to around 92.6% when the catalysis temperature was 500 degrees C, clearly demonstrating that a high temperature with the ZSM-5 Zeolite catalyst favoured the production of aromatic hydrocarbons. At a lower temperature fixed at 375 degrees C, the aromatic hydrocarbon content was increased from 0.72% to 78.1% with a (WHSV)(-1) increase from 0 to 0.075. C1 [Wang, Lu; Lei, Hanwu; Chen, Shulin; Tang, Juming; Ahring, Birgitte] Washington State Univ, Bioprod Sci & Engn Lab, Dept Biol Syst Engn, Richland, WA 99354 USA. [Lee, John] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Lei, HW (reprint author), Washington State Univ, Bioprod Sci & Engn Lab, Dept Biol Syst Engn, Richland, WA 99354 USA. EM hlei@tricity.wsu.edu FU Office of Research; Department of Biological Systems Engineering at Washington State University FX This work was supported in partial by the Office of Research and Department of Biological Systems Engineering at Washington State University. NR 36 TC 12 Z9 13 U1 5 U2 23 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2046-2069 J9 RSC ADV JI RSC Adv. PY 2013 VL 3 IS 34 BP 14609 EP 14615 DI 10.1039/c3ra23104f PG 7 WC Chemistry, Multidisciplinary SC Chemistry GA 195XP UT WOS:000322737400056 ER PT S AU Coslovich, G Huber, B Lee, WS Chuang, YD Zhu, Y Sasagawa, T Hussain, Z Bechtel, HA Martin, MC Schoenlein, RW Shen, ZX Kaindl, RA AF Coslovich, G. Huber, B. Lee, W. -S. Chuang, Y. -D. Zhu, Y. Sasagawa, T. Hussain, Z. Bechtel, H. A. Martin, M. C. Schoenlein, R. W. Shen, Z. -X. Kaindl, R. A. BE Betz, M Elezzabi, AY Song, JJ Tsen, KT TI Ultrafast Mid-infrared Spectroscopy of the Charge- and Spin-ordered Nickelates SO ULTRAFAST PHENOMENA AND NANOPHOTONICS XVII SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Ultrafast Phenomena and Nanophotonics XVII CY FEB 03-06, 2013 CL San Francisco, CA SP SPIE, Femtolasers Inc DE ultrafast dynamics; mid-infrared spectroscopy; strongly-correlated materials; electronic stripes; nickelates AB We discuss the mid-infrared optical response of a charge and spin-ordered nickelate in the ultrafast time domain. A strong photo-induced modulation of the optical reflectivity is observed on the sub-picosecond timescale, indicating the transient filling and recovery of the pseudogap in the mid-infrared charge transport. A variational Kramers-Kronig analysis of equilibrium reflectivity data is extended to time-resolved experiments, allowing us to extract the optical conductivity despite a comparatively limited frequency range of tunable femtosecond parametric sources. The fast dynamics of the spectral weight transfer supports an electronic origin of the mid-infrared pseudogap in nickelates. C1 [Coslovich, G.; Huber, B.; Zhu, Y.; Schoenlein, R. W.; Kaindl, R. A.] Lawrence Berkeley Natl Lab, Div Sci Mat, Berkeley, CA 94720 USA. [Lee, W. -S.; Shen, Z. -X.] Stanford Univ, SLAC Natl Accelerat Lab, SIMES, Menlo Pk, CA 94025 USA. [Chuang, Y. -D.; Hussain, Z.; Bechtel, H. A.; Martin, M. C.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. [Sasagawa, T.] Tokyo Inst Technol, Mat & Struct Lab, Kanagawa 226, Japan. RP Coslovich, G (reprint author), Lawrence Berkeley Natl Lab, Div Sci Mat, Berkeley, CA 94720 USA. EM GCoslovich@lbl.gov RI Schoenlein, Robert/D-1301-2014; Sasagawa, Takao/E-6666-2014 OI Schoenlein, Robert/0000-0002-6066-7566; Sasagawa, Takao/0000-0003-0149-6696 FU U.S. Department of Energy, Office of Basic Energy Sciences (DOE BES), Division of Materials Sciences and Engineering [DE-AC02-05CH11231]; Division of Materials Sciences and Engineering, DOE-BES [DE-AC02-76SF00515]; German Academic Exchange Service (DAAD) FX This research was supported by the U.S. Department of Energy, Office of Basic Energy Sciences (DOE BES), Division of Materials Sciences and Engineering under contract DE-AC02-05CH11231 at Lawrence Berkeley National Laboratory (G.C., B.H., Y.Z., R.W.S., R.A.K.). The Advanced Light Source is supported by DOE BES under the same contract (Y.D.C., H.B., M.M., Z.H.). W.S.L. and Z.X.S. acknowledge funding from the Division of Materials Sciences and Engineering, DOE-BES under contract DE-AC02-76SF00515 at SLAC National Accelerator Laboratory and Stanford Institute for Materials and Energy Sciences. B.H. acknowledges fellowship support from the German Academic Exchange Service (DAAD) and participation in an exchange program with the U.C. Berkeley Nanosciences and Nanoengineering Institute. NR 12 TC 1 Z9 1 U1 0 U2 6 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9392-7 J9 PROC SPIE PY 2013 VL 8623 AR 862308 DI 10.1117/12.2005366 PG 6 WC Nanoscience & Nanotechnology; Optics; Physics, Applied SC Science & Technology - Other Topics; Optics; Physics GA BGG42 UT WOS:000322829300006 ER PT S AU Li, CY Seletskiy, DV Cederberg, JG Sheik-Bahae, M AF Li, Chia-Yeh Seletskiy, Denis V. Cederberg, Jeffrey G. Sheik-Bahae, Mansoor BE Betz, M Elezzabi, AY Song, JJ Tsen, KT TI Observation of strong and broadband terahertz induced electroabsorption in multiple quantum wells SO ULTRAFAST PHENOMENA AND NANOPHOTONICS XVII SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Ultrafast Phenomena and Nanophotonics XVII CY FEB 03-06, 2013 CL San Francisco, CA SP SPIE, Femtolasers Inc DE Electroabsorption; Terahertz; Quantum Well; Franz-Keldysh Effect AB We report the observation of strong terahertz-induced electroabsoption (EA) modulation in in multiple double quantum well (MDQW) structures Broadband terahertz generated by two-color laser induced plasma is focused (similar to 1MV/cm) onto the MQW and spectro-temporal response is probed in transmission geometry, where up to 60% modulation signals are observed. EAS signal is attributed to several mechanisms, including observed qualitative agreement with the twodimensional Franz-Keldysh response. Utilizing strong EA signals, we present a simple THz imaging scheme using conventional imagers. C1 [Li, Chia-Yeh; Seletskiy, Denis V.; Sheik-Bahae, Mansoor] Univ New Mexico, Dept Phys & Astron, Albuquerque, NM 87131 USA. [Cederberg, Jeffrey G.] Sandia Natl Labs, Albuquerque, NM USA. [Seletskiy, Denis V.] Univ Konstanz, Ctr Appl Photon, Dept Phys, Constance, Germany. RP Li, CY (reprint author), Univ New Mexico, Dept Phys & Astron, Albuquerque, NM 87131 USA. FU University of New Mexico is provided by Nation Science Foundation (NSF) [1207489]; Defense Threat Reduction Agency (DTRA); U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000]; National Science Foundation [1160764] FX The funding of this research at University of New Mexico is provided by Nation Science Foundation (NSF) Award No. 1207489, and Defense Threat Reduction Agency (DTRA). 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. D.V.S acknowledges support by the National Science Foundation under Award No. 1160764. NR 9 TC 0 Z9 0 U1 0 U2 0 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9392-7 J9 PROC SPIE PY 2013 VL 8623 AR 86230O DI 10.1117/12.2004633 PG 8 WC Nanoscience & Nanotechnology; Optics; Physics, Applied SC Science & Technology - Other Topics; Optics; Physics GA BGG42 UT WOS:000322829300013 ER PT S AU Luo, CW Chen, HJ Wang, HJ Ku, SA Wu, KH Uen, TM Juang, JY Lin, JY Young, BL Kobayashi, T Sankar, R Chou, FC Berger, H Gu, GD AF Luo, C. W. Chen, H. -J. Wang, H. J. Ku, S. A. Wu, K. H. Uen, T. M. Juang, J. Y. Lin, J. -Y. Young, B. L. Kobayashi, T. Sankar, R. Chou, F. C. Berger, H. Gu, G. D. BE Betz, M Elezzabi, AY Song, JJ Tsen, KT TI Ultrafast dynamics in topological insulators SO ULTRAFAST PHENOMENA AND NANOPHOTONICS XVII SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Ultrafast Phenomena and Nanophotonics XVII CY FEB 03-06, 2013 CL San Francisco, CA SP SPIE, Femtolasers Inc DE Ultrafast dynamics; topological insulators; pump-probe spectroscopy ID SURFACE; TRANSPORT; BI2SE3 AB Ultrafast dynamics of carriers and phonons in topological insulators CuxBi2Se3-y (x= 0, 0.1, 0.125, y= 0, 1) was studied using femtosecond optical pump-probe spectroscopy. One damped oscillation was clearly observed in the transient reflectivity changes (Delta R/R), which is assigned to the coherent optical phonon (A(1g)(1)). According to the red shift of A(1g)(1) phonon frequency, the Cu atoms in CuxBi2Se3 crystals may predominantly intercalated between pair of the quintuple layers. Moreover, the carrier dynamics in the Dirac-cone surface state is significantly different from that in bulk state, which was investigated using optical pump mid-infrared (mid-IR) probe spectroscopy. The rising time and decay time of the negative component in Delta R/R, which is assigned to carrier relaxation in Dirac cone, is 1.62 ps and 20.5 ps, respectively. C1 [Luo, C. W.; Chen, H. -J.; Wang, H. J.; Ku, S. A.; Wu, K. H.; Uen, T. M.; Juang, J. Y.; Young, B. L.; Kobayashi, T.] Natl Chiao Tung Univ, Dept Electrophys, Hsinchu 300, Taiwan. [Lin, J. -Y.] Natl Chiao Tung Univ, Inst Phys, Hsinchu 300, Taiwan. [Sankar, R.; Chou, F. C.] Natl Taipei Univ Technol, Ctr Condensed Matter Sci, Taipei 106, Taiwan. [Berger, H.] Ecole Polytech Fed Lausanne, Inst Phys Complex Matter, CH-1015 Lausanne, Switzerland. [Gu, G. D.] Brookhaven Natl Lab, Dept Condensed Matter Phys & Mat Sci, Upton, NY 11973 USA. RP Luo, CW (reprint author), Natl Chiao Tung Univ, Dept Electrophys, Hsinchu 300, Taiwan. EM cwluo@g2.nctu.edu.tw RI Luo, Chih Wei/D-3485-2013 OI Luo, Chih Wei/0000-0002-6453-7435 FU National Science Council [NSC 98-2112-M-009-006-MY3, NSC98-2112-M-009-008-MY3, NSC 101-2112-M-009-016-MY2]; Ministry of Education (MOE ATU program at NCTU) of Taiwan, R.O.C FX This project is financially sponsored by the National Science Council (grant no. NSC 98-2112-M-009-006-MY3, NSC 98-2112-M-009-008-MY3 and NSC 101-2112-M-009-016-MY2) and the Ministry of Education (MOE ATU program at NCTU) of Taiwan, R.O.C. NR 27 TC 0 Z9 0 U1 3 U2 14 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9392-7 J9 PROC SPIE PY 2013 VL 8623 AR 86230D DI 10.1117/12.2001954 PG 7 WC Nanoscience & Nanotechnology; Optics; Physics, Applied SC Science & Technology - Other Topics; Optics; Physics GA BGG42 UT WOS:000322829300009 ER PT J AU Mariani, Z Strong, K Palm, M Lindenmaier, R Adams, C Zhao, X Savastiouk, V McElroy, CT Goutail, F Drummond, JR AF Mariani, Z. Strong, K. Palm, M. Lindenmaier, R. Adams, C. Zhao, X. Savastiouk, V. McElroy, C. T. Goutail, F. Drummond, J. R. TI Year-round retrievals of trace gases in the Arctic using the Extended-range Atmospheric Emitted Radiance Interferometer SO ATMOSPHERIC MEASUREMENT TECHNIQUES LA English DT Article ID TOTAL OZONE MEASUREMENTS; GROUND-BASED FTIR; INFRARED MEASUREMENTS; EMISSION-SPECTROSCOPY; COLUMN MEASUREMENTS; CARBON-MONOXIDE; WATER-VAPOR; EUREKA; VALIDATION; CANADA AB The Extended-range Atmospheric Emitted Radiance Interferometer (E-AERI) was installed at the Polar Environment Atmospheric Research Laboratory (PEARL) at Eureka, Nunavut, Canada in October 2008. Spectra from the E-AERI provide information about the radiative balance and budgets of trace gases in the Canadian high Arctic. Measurements are taken every 7 min year-round, including polar night when the solar-viewing spectrometers at PEARL are not operated. This allows E-AERI measurements to fill the gap in the PEARL dataset during the four months of polar night. Measurements were taken year-round in 2008-2009 at the PEARL Ridge Lab, which is 610 m a.s.l. (above sea-level), and from 2011 onwards at the Zero-Altitude PEARL Auxiliary Lab (0PAL), which is at sea level 15 km from the Ridge Lab. Total columns of O-3, CO, CH4, and N2O have been retrieved using a modified version of the SFIT2 retrieval algorithm adapted for emission spectra. This provides the first ground-based nighttime measurements of these species at Eureka. Changes in the total columns driven by photochemistry and dynamics are observed. Analyses of E-AERI retrievals indicate accurate spectral fits (root-mean-square residuals consistent with noise) and a 10-15% uncertainty in the total column, depending on the trace gas. O-3 comparisons between the E-AERI and a Bruker IFS 125HR Fourier transform infrared (FTIR) spectrometer, three Brewer spectrophotometers, two UV-visible ground-based spectrometers, and a System D'Analyse par Observations Zenithales (SAOZ) at PEARL are made from 2008-2009 and for 2011. 125HR CO, CH4, and N2O columns are also compared with the E-AERI measurements. Mean relative differences between the E-AERI and the other spectrometers are 1-10% (14% is for the un-smoothed profiles), which are less than the E-AERI's total column uncertainties. The E-AERI O-3 and CO measurements are well correlated with the other spectrometers (r > 0.92 with the 125HR). The 24 h diurnal cycle and 365-day seasonal cycle of CO are observed and their amplitudes are quantified by the E-AERI (6-12 and 46 %, respectively). The seasonal variability of H2O has an impact on the retrievals, leading to larger uncertainties in the summer months. Despite increased water vapour at the lower-altitude site 0PAL, measurements at 0PAL are consistent with measurements at PEARL. C1 [Mariani, Z.; Strong, K.; Lindenmaier, R.; Adams, C.; Zhao, X.] Univ Toronto, Dept Phys, Toronto, ON, Canada. [Palm, M.] Univ Bremen, Dept Phys, Bremen, Germany. [Lindenmaier, R.] Los Alamos Natl Lab, Div Phys, Los Alamos, NM 87545 USA. [Adams, C.] Univ Saskatoon, Dept Phys & Engn, Saskatoon, SK, Canada. [Savastiouk, V.] Full Spectrum Sci Inc, Toronto, ON, Canada. [McElroy, C. T.] York Univ, Dept Earth & Space Sci & Engn, Toronto, ON M3J 2R7, Canada. [Goutail, F.] Univ Versailles St Quentin, CNRS, LATMOS, Guyancourt, France. [Drummond, J. R.] Dalhousie Univ, Dept Phys & Atmospher Sci, Halifax, NS, Canada. RP Mariani, Z (reprint author), Univ Toronto, Dept Phys, Toronto, ON, Canada. EM zmariani@atmosp.physics.utoronto.ca; strong@atmosp.physics.utoronto.ca; mathias@iup.physik.uni-bremen.de; rodica@atmosp.physics.utoronto.ca; cadams@physics.utoronto.ca; xizhao@atmosp.physics.utoronto.ca; volodya@io3.ca; c.t.mcelroy@gmail.com; florence.goutail@aerov.jussieu.fr; james.drummond@dal.ca RI Drummond, James/O-7467-2014; OI Palm, Mathias/0000-0001-7191-6911 FU Arctic Research Infrastructure Fund; Atlantic Innovation Fund/Nova Scotia Research Innovation Trust; Canadian Foundation for Climate and Atmospheric Science; Canadian Foundation for Innovation; Canadian Space Agency (CSA); Environment Canada (EC); Government of Canada International Polar Year; Natural Sciences and Engineering Research Council (NSERC); Ontario Innovation Trust; Ontario Research Fund; Indian and Northern Affairs Canada; Polar Continental Shelf Program; CSA; NSERC; NSERC CREATE Training Program in Arctic Atmospheric Science; Northern Student Training Program FX The Polar Environment Atmospheric Research Laboratory (PEARL) is operated by the Canadian Network for the Detection of Atmospheric Change (CANDAC). CANDAC/PEARL funding partners are: the Arctic Research Infrastructure Fund, Atlantic Innovation Fund/Nova Scotia Research Innovation Trust, Canadian Foundation for Climate and Atmospheric Science, Canadian Foundation for Innovation, Canadian Space Agency (CSA), Environment Canada (EC), Government of Canada International Polar Year, Natural Sciences and Engineering Research Council (NSERC), Ontario Innovation Trust, Ontario Research Fund, Indian and Northern Affairs Canada, and the Polar Continental Shelf Program. Spring visits to PEARL were made as part of the Canadian Arctic ACE Validation Campaigns, led by Kaley A. Walker and supported by CSA, EC, NSERC, NSERC CREATE Training Program in Arctic Atmospheric Science, and the Northern Student Training Program. Thanks to David Hudak at Environment Canada for providing MMCR data. Thanks to PEARL site manager Pierre Fogal and CANDAC operators Ashley Harrett, Alexei Khmel, Paul Loewen, Oleg Mikhailov, Keith MacQuarrie and Matt Okraszewski who have helped with the E-AERI measurements at PEARL. Thanks to Stephane Lantagne and Guillaume Gamache from ABB for their work installing the E-AERI, Dan Weaver for his help analyzing water vapour data, and Simone Chaudhary for her help with automating SFIT2. Thanks also to the staff at the Eureka Weather Station for their support and hospitality. NR 43 TC 1 Z9 1 U1 0 U2 6 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1867-1381 J9 ATMOS MEAS TECH JI Atmos. Meas. Tech. PY 2013 VL 6 IS 6 BP 1549 EP 1565 DI 10.5194/amt-6-1549-2013 PG 17 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA 193FX UT WOS:000322545400007 ER PT J AU Shim, JH Powers, HH Meyer, CW Knohl, A Dawson, TE Riley, WJ Pockman, WT McDowell, N AF Shim, J. H. Powers, H. H. Meyer, C. W. Knohl, A. Dawson, T. E. Riley, W. J. Pockman, W. T. McDowell, N. TI Hydrologic control of the oxygen isotope ratio of ecosystem respiration in a semi-arid woodland SO BIOGEOSCIENCES LA English DT Article ID TUNABLE DIODE-LASER; GLOBAL 3-DIMENSIONAL MODEL; BOREAL FOREST ECOSYSTEMS; ATMOSPHERIC WATER-VAPOR; LEAF WATER; RESPIRED CO2; SOIL-WATER; STABLE-ISOTOPE; CARBON-DIOXIDE; STOMATAL CONDUCTANCE AB We conducted high frequency measurements of the delta O-18 value of atmospheric CO2 from a juniper (Juniperus monosperma) woodland in New Mexico, USA, over a four-year period to investigate climatic and physiological regulation of the delta O-18 value of ecosystem respiration (delta(R)). Rain pulses reset delta(R) with the dominant water source isotope composition, followed by progressive enrichment of delta(R). Transpiration (E-T) was significantly related to post-pulse delta(R) enrichment because the leaf water delta O-18 value showed strong enrichment with increasing vapor pressure deficit that occurs following rain. Post-pulse delta(R) enrichment was correlated with both E-T and the ratio of E-T to soil evaporation (E-T/E-S). In contrast, the soil water delta O-18 value was relatively stable and delta(R) enrichment was not correlated with E-S. Model simulations captured the large post-pulse delta(R) enrichments only when the offset between xylem and leaf water delta O-18 value was modeled explicitly and when a gross flux model for CO2 retro-diffusion was included. Drought impacts delta(R) through the balance between evaporative demand, which enriches delta(R), and low soil moisture availability, which attenuates delta(R) enrichment through reduced E-T. The net result, observed throughout all four years of our study, was a negative correlation of post-precipitation delta(R) enrichment with increasing drought. C1 [Shim, J. H.; Powers, H. H.; Meyer, C. W.; McDowell, N.] Los Alamos Natl Lab, Div Earth & Environm Sci, Los Alamos, NM 87545 USA. [Knohl, A.] Univ Gottingen, Chair Bioclimatol, D-37073 Gottingen, Germany. [Dawson, T. E.] Univ Calif Berkeley, Dept Integrat Biol, Berkeley, CA 94720 USA. [Riley, W. J.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, Berkeley, CA 94720 USA. [Pockman, W. T.] Univ New Mexico, Dept Biol, Albuquerque, NM 87131 USA. RP Shim, JH (reprint author), Los Alamos Natl Lab, Div Earth & Environm Sci, MS-J495, Los Alamos, NM 87545 USA. EM jeehshim@gmail.com RI Pockman, William/D-4086-2014; Knohl, Alexander/F-9453-2014; Riley, William/D-3345-2015 OI Pockman, William/0000-0002-3286-0457; Knohl, Alexander/0000-0002-7615-8870; Riley, William/0000-0002-4615-2304 FU LANL-Laboratory Directed Research and Development (LDRD); Institute for Geophysical and Planetary Research (IGPP); Department of Energy, Office of Science, Office of Biological and Environmental Research (DOE-BER) FX We appreciate the technical and field support provided by Steve Sargent, Karen Brown, and numerous undergraduate interns during the four years of this study. Funding for this project was derived from LANL-Laboratory Directed Research and Development (LDRD), the Institute for Geophysical and Planetary Research (IGPP), and the Department of Energy, Office of Science, Office of Biological and Environmental Research (DOE-BER). NR 87 TC 3 Z9 3 U1 3 U2 19 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1726-4170 EI 1726-4189 J9 BIOGEOSCIENCES JI Biogeosciences PY 2013 VL 10 IS 7 BP 4937 EP 4956 DI 10.5194/bg-10-4937-2013 PG 20 WC Ecology; Geosciences, Multidisciplinary SC Environmental Sciences & Ecology; Geology GA 189BT UT WOS:000322242700035 ER PT S AU Mourant, JR Marina, OC Sanders, CK AF Mourant, Judith R. Marina, Oana C. Sanders, Claire K. BE Wax, AP Backman, V TI The contribution of specific organelles to side scatter SO BIOMEDICAL APPLICATIONS OF LIGHT SCATTERING VII SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Biomedical Applications of Light Scattering VII CY FEB 02-04, 2013 CL San Francisco, CA SP SPIE DE light scattering; flow cytometry; fluorescence; mitochondria; lysosomes; nuclei ID LIGHT-SCATTERING; RAT-LIVER; CELLS; TISSUE AB Knowledge of which cellular structures scatter light is needed to fully utilize the information available from light scattering measurements of cells and tissues. To determine how specific organelles contribute to light scattering, wide angle side scattering was imaged simultaneously with fluorescence from specific organelles for thousands of cells using flow cytometry. Images were obtained with different depth of field conditions and analyzed with different assumptions. Both sets of data demonstrated that mitochondria and lysosomes, contribute similarly to side scatter. The nucleus contributes as much or more light scatter than either the mitochondria or the lysosomes. C1 [Mourant, Judith R.; Marina, Oana C.; Sanders, Claire K.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Mourant, JR (reprint author), Los Alamos Natl Lab, MS M888, Los Alamos, NM 87545 USA. EM jmourant@lanl.gov RI Backman, Vadim/B-6689-2009 NR 15 TC 0 Z9 0 U1 0 U2 2 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9361-3 J9 PROC SPIE PY 2013 VL 8592 AR 85920L DI 10.1117/12.2008437 PG 7 WC Engineering, Biomedical; Optics SC Engineering; Optics GA BFX99 UT WOS:000321858000008 ER PT J AU Prozument, K Shaver, RG Ciuba, MA Muenter, JS Park, GB Stanton, JF Guo, H Wong, BM Perry, DS Field, RW AF Prozument, Kirill Shaver, Rachel Glyn Ciuba, Monika A. Muenter, John S. Park, G. Barratt Stanton, John F. Guo, Hua Wong, Bryan M. Perry, David S. Field, Robert W. TI A new approach toward transition state spectroscopy SO FARADAY DISCUSSIONS LA English DT Article ID EXCITED VIBRATIONAL-STATES; LARGE-AMPLITUDE MOTIONS; PHOTOELECTRON-SPECTROSCOPY; WAVE SPECTROSCOPY; ACETYLENE; VINYLIDENE; ISOMERIZATION; ENERGY; CM(-1); HCN AB Chirped-Pulse millimetre-Wave (CPmmW) rotational spectroscopy provides a new class of information about photolysis transition state(s). Measured intensities in rotational spectra determine species-isomer-vibrational populations, provided that the rotational populations can be thermalized. The formation and detection of S-0 vinylidene is discussed in the limits of low and high initial rotational excitation. CPmmW spectra of 193 nm photolysis of vinyl cyanide (acrylonitrile) contain J = 0-1 transitions in more than 20 vibrational levels of HCN and HNC, but no transitions in vinylidene or highly excited local-bender vibrational levels of acetylene. Reasons for the non-observation of the vinylidene co-product of HCN are discussed. C1 [Prozument, Kirill; Shaver, Rachel Glyn; Park, G. Barratt; Field, Robert W.] MIT, Dept Chem, Cambridge, MA 02139 USA. [Ciuba, Monika A.] Arizona State Univ, Dept Chem & Biochem, Tempe, AZ 85287 USA. [Muenter, John S.] Univ Rochester, Dept Chem, Rochester, NY 14627 USA. [Stanton, John F.] Univ Texas Austin, Dept Chem & Biochem, Austin, TX 78712 USA. [Guo, Hua] Univ New Mexico, Dept Chem, Albuquerque, NM 87131 USA. [Wong, Bryan M.] Sandia Natl Labs, Dept Chem Mat, Livermore, CA 94550 USA. [Perry, David S.] Univ Akron, Dept Chem, Akron, OH 44325 USA. RP Field, RW (reprint author), MIT, Dept Chem, Cambridge, MA 02139 USA. EM kuyanov@mit.edu; rshaver@mit.edu; monika.ciuba@asu.edu; muenter@chem.rochester.edu; barratt@mit.edu; jfstanton@mail.utexas.edu; hguo@unm.edu; usagi@alum.mit.edu; dperry@uakron.edu; rwfield@mit.edu RI Wong, Bryan/B-1663-2009; Prozument, Kirill/F-7865-2013; Guo, Hua/J-2685-2014; OI Wong, Bryan/0000-0002-3477-8043; Prozument, Kirill/0000-0003-3045-8429; Guo, Hua/0000-0001-9901-053X; Park, Barratt/0000-0002-8716-220X FU Department of Energy [DEFG0287ER13671]; Petroleum Research Fund [50650-ND6]; Air Force Office of Scientific Research [FA9550-09-1-0330]; National Science Foundation [1126380] FX We are grateful to Dr. Gabriel Just and to Prof. T. A. Miller at The Ohio State University for sharing their expertise on the slit jet design, and to Dr. Michel Costes at the University of Bordeaux for providing us with the multi-channel IOTA ONE driver. RWF thanks the Department of Energy (grant #DEFG0287ER13671) for primary support of this work (equipment and personnel support for KP, RGS, GBP, BMW), the Petroleum Research Fund (grant #50650-ND6) for the support of KP, the Air Force Office of Scientific Research (contract #FA9550-09-1-0330) for the support of MC, and the National Science Foundation (grant #1126380) for equipment and for partial support of GBP. We thank Joshua Baraban for many experimental and theoretical contributions. NR 48 TC 18 Z9 18 U1 0 U2 37 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 163 BP 33 EP 57 DI 10.1039/c3fd20160k PG 25 WC Chemistry, Physical SC Chemistry GA 187LN UT WOS:000322120500002 PM 24020195 ER PT J AU King, SB Yandell, MA Neumark, DM AF King, Sarah B. Yandell, Margaret A. Neumark, Daniel M. TI Time-resolved photoelectron imaging of the iodide-thymine and iodide-uracil binary cluster systems SO FARADAY DISCUSSIONS LA English DT Article ID DISSOCIATIVE ELECTRON-ATTACHMENT; NUCLEIC-ACID BASES; DNA-STRAND BREAKS; AB-INITIO; IONIZATION-POTENTIALS; PYRIMIDINE-BASES; RARE TAUTOMERS; NEGATIVE-IONS; ANIONS; SPECTROSCOPY AB The energetics and dynamics of thymine and uracil transient negative ions were examined using femtosecond time-resolved photoelectron imaging. The vertical detachment energies (VDEs) of these systems were found to be 4.05 eV and 4.11 eV for iodide-thymine (I-center dot T) and iodide-uracil (I-center dot U) clusters, respectively. An ultraviolet pump pulse was used to promote intracluster charge transfer from iodide to the nucleobase. Subsequent electron detachment using an infrared probe pulse monitored the dynamics of the resulting transient negative ion. Photoelectron spectra reveal two primary features: a near-zero electron kinetic energy signal attributed to autodetachment and a transient feature representing photodetachment from the excited anion state. The transient state exhibits biexponential decay in both thymine and uracil complexes with short and long decay time constants ranging from 150-600 fs and 1-50 ps, respectively, depending on the excitation energy. However, both time constants are systematically shorter for I-center dot T. Vibrational autodetachment and iodine loss are identified as the primary decay mechanisms of the transient negative ions of thymine and uracil. C1 [King, Sarah B.; Yandell, Margaret A.; Neumark, Daniel M.] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Neumark, Daniel M.] Lawrence Berkeley Natl Lab, Chem Sci Div, Berkeley, CA 94702 USA. RP Neumark, DM (reprint author), Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. EM dneumark@berkeley.edu RI Neumark, Daniel/B-9551-2009 OI Neumark, Daniel/0000-0002-3762-9473 FU National Science Foundation (NSF) [CHE-1011819]; NSF FX This research is supported by the National Science Foundation (NSF) under grant CHE-1011819. S.B.K. and M.A.Y. are grateful for funding through NSF Graduate Research Fellowships. NR 55 TC 17 Z9 17 U1 5 U2 37 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 163 BP 59 EP 72 DI 10.1039/c3fd20158a PG 14 WC Chemistry, Physical SC Chemistry GA 187LN UT WOS:000322120500003 PM 24020196 ER PT J AU Kelley, ST Gilbert, JA AF Kelley, Scott T. Gilbert, Jack A. TI Studying the microbiology of the indoor environment SO GENOME BIOLOGY LA English DT Review ID RIBOSOMAL-RNA GENE; HUMAN SKIN MICROBIOTA; BACTERIAL COMMUNITIES; PHYLOGENETIC DIVERSITY; MOLECULAR ANALYSIS; QUANTITATIVE PCR; CULTURE; WATER; AIR; METAGENOMICS AB The majority of people in the developed world spend more than 90% of their lives indoors. Here, we examine our understanding of the bacteria that co-inhabit our artificial world and how they might influence human health. C1 [Kelley, Scott T.] San Diego State Univ, Dept Biol, San Diego, CA 92182 USA. [Gilbert, Jack A.] Argonne Natl Lab, Argonne, IL 60439 USA. [Gilbert, Jack A.] Univ Chicago, Dept Ecol & Evolut, Chicago, IL 60637 USA. RP Kelley, ST (reprint author), San Diego State Univ, Dept Biol, 5500 Campanile Dr, San Diego, CA 92182 USA. EM skelley@mail.sdsu.edu FU Alfred P Sloan Foundation; US Department of Energy [DE-AC02-06CH11357] FX This work was supported in part by a grant from the Alfred P Sloan Foundation and the US Department of Energy under Contract DE-AC02-06CH11357. NR 77 TC 35 Z9 36 U1 3 U2 64 PU BIOMED CENTRAL LTD PI LONDON PA 236 GRAYS INN RD, FLOOR 6, LONDON WC1X 8HL, ENGLAND SN 1465-6906 J9 GENOME BIOL JI Genome Biol. PY 2013 VL 14 IS 2 AR 202 DI 10.1186/gb-2013-14-2-202 PG 9 WC Biotechnology & Applied Microbiology; Genetics & Heredity SC Biotechnology & Applied Microbiology; Genetics & Heredity GA 191BY UT WOS:000322388800014 PM 23514020 ER PT J AU Lu, AH Dai, S AF Lu, An-Hui Dai, Sheng TI Themed issue on porous carbon materials SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Editorial Material C1 [Lu, An-Hui] Dalian Univ Technol, Sch Chem Engn, State Key Lab Fine Chem, Dalian 116024, Peoples R China. [Dai, Sheng] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. RP Lu, AH (reprint author), Dalian Univ Technol, Sch Chem Engn, State Key Lab Fine Chem, LingGong Rd 2, Dalian 116024, Peoples R China. EM anhuilu@dlut.edu.cn; dais@ornl.gov RI Dai, Sheng/K-8411-2015 OI Dai, Sheng/0000-0002-8046-3931 NR 0 TC 3 Z9 3 U1 0 U2 31 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 33 BP 9326 EP 9326 DI 10.1039/c3ta90211k PG 1 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA 192HT UT WOS:000322475600001 ER PT J AU Adcock, JL Fulvio, PF Dai, S AF Adcock, Jamie L. Fulvio, Pasquale F. Dai, Sheng TI Towards the selective modification of soft-templated mesoporous carbon materials by elemental fluorine for energy storage devices SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID LOW-TEMPERATURE FLUORINATION; LITHIUM-ION BATTERIES; ELECTROCHEMICAL PROPERTIES; ELECTRODE MATERIALS; BLOCK-COPOLYMERS; PETROLEUM COKES; GRAPHITE; STABILITY; FULLERENE; TRANSFORMATION AB Graphite fluoride is classified into (CF)(n) and (C2F)(n) types based on its structure and composition. The former (CF) n has been widely prepared and commercially utilized as electrodes in primary lithium ion batteries (LIBs). Porous electrodes, i.e. templated mesoporous carbons, can greatly improve first Coulombic efficiencies. For achieving the highest discharge potentials and rate capabilities, the extent of fluorination reactions and the retention of a conductive carbon backbone are required. Hence, the choice of the starting carbon nanomaterial and of the fluorination conditions is detrimental to the design of future energy storage and conversion devices, namely LIBs and pseudosupercapacitors. C1 [Adcock, Jamie L.; Dai, Sheng] Univ Tennessee, Dept Chem, Knoxville, TN 37996 USA. [Fulvio, Pasquale F.; Dai, Sheng] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 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 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, an Energy Frontier Research Center; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences FX The authors were supported as part of the Fluid Interface Reactions, Structures, and Transport (FIRST) Center, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences (PFF and SD). NR 63 TC 8 Z9 8 U1 2 U2 60 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 33 BP 9327 EP 9331 DI 10.1039/c3ta10700k PG 5 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA 192HT UT WOS:000322475600002 ER PT J AU Morris, JR Contescu, CI Chisholm, MF Cooper, VR Guo, J He, L Ihm, Y Mamontov, E Melnichenko, YB Olsen, RJ Pennycook, SJ Stone, MB Zhang, H Gallego, NC AF Morris, J. R. Contescu, C. I. Chisholm, M. F. Cooper, V. R. Guo, J. He, L. Ihm, Y. Mamontov, E. Melnichenko, Y. B. Olsen, R. J. Pennycook, S. J. Stone, M. B. Zhang, H. Gallego, N. C. TI Modern approaches to studying gas adsorption in nanoporous carbons SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID ANGLE NEUTRON-SCATTERING; ACTIVATED CARBONS; MOLECULAR-HYDROGEN; CO2 CAPTURE; GRAPHITE; COAL; TRANSITION; GRAPHENE; PROPANE; METHANE AB Conventional approaches to understanding the gas adsorption capacity of nanoporous carbons have emphasized the relationship with the effective surface area, but more recent work has demonstrated the importance of local structures and pore-size-dependent adsorption. These developments provide new insights into local structures in nanoporous carbon and their effect on gas adsorption and uptake characteristics. Experiments and theory show that appropriately tuned pores can strongly enhance local adsorption, and that pore sizes can be used to tune adsorption characteristics. In the case of H-2 adsorbed on nanostructured carbon, quasielastic and inelastic neutron scattering probes demonstrate novel quantum effects in the motion of adsorbed molecules. C1 [Morris, J. R.; Contescu, C. I.; Chisholm, M. F.; Cooper, V. R.; Olsen, R. J.; Pennycook, S. J.; Zhang, H.; Gallego, N. C.] Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN 37831 USA. [Morris, J. R.; Guo, J.; Ihm, Y.] Univ Tennessee, Dept Mat Sci & Engn, Oak Ridge, TN 37996 USA. [He, L.; Mamontov, E.; Melnichenko, Y. B.; Stone, M. B.] Oak Ridge Natl Lab, Neutron Sci Directorate, Oak Ridge, TN 37831 USA. RP Morris, JR (reprint author), Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN 37831 USA. EM morrisj@ornl.gov; gallegonc@ornl.gov RI Stone, Matthew/G-3275-2011; Cooper, Valentino /A-2070-2012; Mamontov, Eugene/Q-1003-2015; BL18, ARCS/A-3000-2012; guo, junjie/I-3189-2012; Morris, J/I-4452-2012; OI Stone, Matthew/0000-0001-7884-9715; Cooper, Valentino /0000-0001-6714-4410; Mamontov, Eugene/0000-0002-5684-2675; guo, junjie/0000-0002-3414-3734; Morris, J/0000-0002-8464-9047; Contescu, Cristian/0000-0002-7450-3722; He, Lilin/0000-0002-9560-8101; Gallego, Nidia/0000-0002-8252-0194 FU U.S. Department of Energy (DOE), Basic Energy Sciences (BES), Materials Sciences and Engineering Division; U.S. Department of Energy Office of Energy Efficiency and Renewable Energy (DOE-EERE); Scientific User Facility Division, Office of Basic Energy Sciences, U.S. Department of Energy; DOE-BES FX JRM thanks Mina Yoon for helpful comments on the manuscript. Research by JRM, CIC, NCG, JG, MFC, VRC, SJP, HZ and YI was supported by the U.S. Department of Energy (DOE), Basic Energy Sciences (BES), Materials Sciences and Engineering Division. HZ acknowledges appointment under the ORNL Postdoctoral Associate Program administered jointly by Oak Ridge Institute for Science and Education and Oak Ridge Associated Universities. RJO was supported from the U.S. Department of Energy Office of Energy Efficiency and Renewable Energy (DOE-EERE) postdoctoral research award under the EERE Fuel Cell Technologies Program. Neutron scattering experiments were conducted at Oak Ridge National Laboratory's Spallation Neutron Source (SNS) and High Flux Isotope Reactor (HFIR), supported by the Scientific User Facility Division, Office of Basic Energy Sciences, U.S. Department of Energy. We also acknowledge computer time from the National Energy Research Scientific Computing Center (NERSC) of DOE. The microscopy was also supported through a user project with ORNL's Shared Research Equipment (ShaRE) User Program, which is also sponsored by DOE-BES. NR 54 TC 15 Z9 15 U1 6 U2 64 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 33 BP 9341 EP 9350 DI 10.1039/c3ta10701a PG 10 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA 192HT UT WOS:000322475600004 ER PT J AU Fulvio, PF Veith, GM Adcock, JL Brown, SS Mayes, RT Wang, XQ Mahurin, SM Guo, BK Sun, XG Puretzky, AA Rouleau, CM Geohegan, DB Dai, S AF Fulvio, Pasquale F. Veith, Gabriel M. Adcock, Jamie L. Brown, Suree S. Mayes, Richard T. Wang, Xiqing Mahurin, Shannon M. Guo, Bingkun Sun, Xiao-Guang Puretzky, Alex A. Rouleau, Christopher M. Geohegan, David B. Dai, Sheng TI Fluorination of "brick and mortar" soft-templated graphitic ordered mesoporous carbons for high power lithium-ion battery SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID PETROLEUM COKES; TRANSFORMATION; PERFORMANCE; FRAMEWORKS; POLYMERS; GAS AB Ordered mesoporous carbon-graphitic carbon composites prepared by the "brick and mortar" method were fluorinated using F-2 and investigated as cathodes for primary lithium batteries. The resulting materials have a rich array of C-F species, as measured by XPS, which influence conduction and voltage profiles. C1 [Fulvio, Pasquale F.; Mayes, Richard T.; Wang, Xiqing; Mahurin, Shannon M.; Guo, Bingkun; Sun, Xiao-Guang; Dai, Sheng] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. [Veith, Gabriel M.] Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN 37831 USA. [Adcock, Jamie L.; Brown, Suree S.; Dai, Sheng] Univ Tennessee, Dept Chem, Knoxville, TN 37996 USA. [Puretzky, Alex A.; Rouleau, Christopher M.; Geohegan, David B.] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, 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 Guo, Bingkun/J-5774-2014; Fulvio, Pasquale/B-2968-2014; Wang, Xiqing/E-3062-2010; Rouleau, Christopher/Q-2737-2015; Puretzky, Alexander/B-5567-2016; Dai, Sheng/K-8411-2015; Geohegan, David/D-3599-2013; Mayes, Richard/G-1499-2016 OI Fulvio, Pasquale/0000-0001-7580-727X; Wang, Xiqing/0000-0002-1843-008X; Rouleau, Christopher/0000-0002-5488-3537; Puretzky, Alexander/0000-0002-9996-4429; Dai, Sheng/0000-0002-8046-3931; Geohegan, David/0000-0003-0273-3139; Mayes, Richard/0000-0002-7457-3261 FU U.S. Department of Energy's Office of Basic Energy Science, Division of Materials Sciences and Engineering; Fluid Interface Reactions, Structures, and Transport (FIRST) Center, an Energy Frontier Research Center; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences; Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy FX This work was supported by the U.S. Department of Energy's Office of Basic Energy Science, Division of Materials Sciences and Engineering. PF and SM in synthesis of mesoporous carbons were supported by the Fluid Interface Reactions, Structures, and Transport (FIRST) Center, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences. A portion of this research was performed 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 27 TC 5 Z9 5 U1 3 U2 62 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 33 BP 9414 EP 9417 DI 10.1039/c3ta10710h PG 4 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA 192HT UT WOS:000322475600010 ER PT J AU Xiao, LF Cao, YL Xiao, J Schwenzer, B Engelhard, MH Saraf, LV Nie, ZM Exarhos, GJ Liu, J AF Xiao, Lifen Cao, Yuliang Xiao, Jie Schwenzer, Birgit Engelhard, Mark H. Saraf, Laxmikant V. Nie, Zimin Exarhos, Gregory J. Liu, Jun TI Molecular structures of polymer/sulfur composites for lithium-sulfur batteries with long cycle life SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID RAY PHOTOELECTRON-SPECTROSCOPY; IONIC LIQUID ELECTROLYTE; CATHODE MATERIALS; ELECTROCHEMICAL PROPERTIES; IMPEDANCE SPECTROSCOPY; CARBON COMPOSITES; S BATTERIES; POLYANILINE; PERFORMANCE; NANOTUBES AB Vulcanized polyaniline/sulfur (SPANI/S) nanostructures were investigated for Li-S battery applications, but the detailed molecular structures of such composites have not been fully illustrated. In this paper, we synthesize SPANI/S composites with different S content in a nanorod configuration. FTIR, Raman, XPS, XRD, SEM and elemental analysis methods are used to characterize the molecular structure of the materials. We provide clear evidence that a portion of S was grafted on PANI during heating and connected the PANI chains with disulfide bonds to form a crosslinked network and the rest of S was encapsulated within it. Polysulfides and elementary S nanoparticles are physically trapped inside the polymer network and are not chemically bound to the polymer. The performance of the composites is further improved by reducing the particle size. After 200 cycles, a capacity retention rate of 80.4, 80.5, 87.6, and 90.0% is observed at 0.1, 0.2, 0.5 and 1 C respectively in the SPANI/S composite with 55% S content. C1 [Xiao, Lifen] Cent China Normal Univ, Coll Chem, Wuhan 430079, Peoples R China. [Cao, Yuliang] Wuhan Univ, Coll Chem & Mol Sci, Wuhan 430072, Peoples R China. [Xiao, Lifen; Cao, Yuliang; Xiao, Jie; Schwenzer, Birgit; Engelhard, Mark H.; Saraf, Laxmikant V.; Nie, Zimin; Exarhos, Gregory J.; Liu, Jun] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Cao, YL (reprint author), Wuhan Univ, Coll Chem & Mol Sci, Wuhan 430072, Peoples R China. EM ylcao@whu.edu.cn; Jun.Liu@pnnl.gov OI Schwenzer, Birgit/0000-0002-7872-1372; Engelhard, Mark/0000-0002-5543-0812 FU U.S. Department of Energy (DOE), Office of Basic Energy Sciences, Division of Materials Sciences and Engineering [KC020105-FWP12152]; National Natural Science Foundation of China [21273090]; Department of Energy's Office of Biological and Environmental Research; DOE by Battelle [DE-AC05-76RL01830] FX This research is supported by the U.S. Department of Energy (DOE), Office of Basic Energy Sciences, Division of Materials Sciences and Engineering under Award KC020105-FWP12152. Xiao would like to acknowledge the support by the National Natural Science Foundation of China (no. 21273090). The TEM and XPS were conducted at the Environmental and Molecular Sciences Laboratory, 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 (PNNL) is a multiprogram national laboratory operated for DOE by Battelle under Contract DE-AC05-76RL01830. NR 51 TC 34 Z9 34 U1 11 U2 141 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 33 BP 9517 EP 9526 DI 10.1039/c3ta10865a PG 10 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA 192HT UT WOS:000322475600025 ER PT J AU Torok, J Del Re, R Herbol, H Das, S Bocharova, I Paolucci, A Ocola, LE Ventrice, C Lifshin, E Denbeaux, G Brainard, RL AF Torok, Justin Del Re, Ryan Herbol, Henry Das, Sanjana Bocharova, Irina Paolucci, Angela Ocola, Leonidas E. Ventrice, Carl, Jr. Lifshin, Eric Denbeaux, Greg Brainard, Robert L. TI Secondary Electrons in EUV Lithography SO JOURNAL OF PHOTOPOLYMER SCIENCE AND TECHNOLOGY LA English DT Article ID ENERGY-LOSS SPECTROSCOPY; CHEMICALLY AMPLIFIED RESISTS; X-RAY-LITHOGRAPHY; INELASTIC INTERACTIONS; ACID YIELD; SIMULATION; BEAM; MICROSCOPY; SOLIDS; RANGE AB Secondary electrons play critical roles in several imaging technologies, including extreme ultraviolet (EUV) lithography. At longer wavelengths of light (e.g. 193 and 248 nm), the photons are directly involved in the photochemistry occurring during photolysis. EUV light (13.5 um, 92 eV), however, first creates a photoelectron, and this electron, or its subsequent daughter electrons create most of the chemical changes that occur during exposure. Despite the importance of these electrons, the details surrounding the chemical events leading to acid production remain poorly understood. Previously reported experimental results using high PAG-loaded resists have demonstrated that up to five or six photoacids can be generated per incident photon. Until recently, only electron recombination events were thought to play a role in acid generation, requiring that at least as many secondary electrons are produced to yield a given number of acid molecules. However, the initial results we have obtained using a Monte Carlo-based modeling program, LESiS, demonstrate that only two to three secondary electrons are made per absorbed EUV photon. A more comprehensive understanding of EUV-induced acid generation is therefore needed for the development of higher performance resists. C1 [Torok, Justin; Del Re, Ryan; Herbol, Henry; Das, Sanjana; Bocharova, Irina; Paolucci, Angela; Ventrice, Carl, Jr.; Lifshin, Eric; Denbeaux, Greg; Brainard, Robert L.] SUNY Albany, Coll Nanoscale Sci & Engn, Albany, NY 12222 USA. [Ocola, Leonidas E.] Argonne Natl Lab, Argonne, IL 60439 USA. RP Torok, J (reprint author), SUNY Albany, Coll Nanoscale Sci & Engn, Albany, NY 12222 USA. OI Ocola, Leonidas/0000-0003-4990-1064 FU U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]; College of Nanoscale Science and Engineering (CNSE) FX We thank the College of Nanoscale Science and Engineering (CNSE) and specifically, Senior Vice President Alain Kaleyeros for financial support of this project. We also thank the supplier of our commercial resist. Additionally, we thank Brian Cardineau, Bill Earley, Yudhishthir Kandel, Tim Groves, and Alain Diebold for helpful discussions. The use of the Center for Nanoscale Materials, Argonne National Laboratory was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. NR 39 TC 15 Z9 15 U1 0 U2 19 PU TECHNICAL ASSOC PHOTOPOLYMERS,JAPAN PI CHIBA PA CHIBA UNIV, FACULTY ENGINEERING, YAYOICHO, CHIBA, 263-8522, JAPAN SN 0914-9244 J9 J PHOTOPOLYM SCI TEC JI J. Photopolym Sci. Technol. PY 2013 VL 26 IS 5 BP 625 EP 634 PG 10 WC Polymer Science SC Polymer Science GA 192RW UT WOS:000322504000009 ER PT J AU Fujita, EM Campbell, DE Stockwell, WR Lawson, DR AF Fujita, Eric M. Campbell, David E. Stockwell, William R. Lawson, Douglas R. TI Past and future ozone trends in California's South Coast Air Basin: Reconciliation of ambient measurements with past and projected emission inventories SO JOURNAL OF THE AIR & WASTE MANAGEMENT ASSOCIATION LA English DT Article ID WEEKDAY; QUALITY; TUNNEL; NOX AB This paper updates the historic trends (1980-2010) in ambient ozone and ozone precursor concentrations in the South Coast Air Basin (SoCAB) and examines the evolution of the ozone-precursor relationship in the Basin. Whereas reductions in NOx (oxide of nitrogen) emissions have decreased nitrate and PM2.5 (particulate matter with an aerodynamic diameter 2.5 m) concentrations in the Basin during the past decade, ozone levels have increased at the central basin locations since about 2005 following a reversal in the decline of volatile organic compound (VOC)/NOx ratios during the previous two decades. A chemical box model was used to simulate the effects of changes in precursor concentrations on ozone formation using day-of-week-specific initial precursor concentrations that were derived from measurements and projected to 2020 based on expected emission reductions from 2005 (-10% VOC and-50% NOx). Results show that peak ozone formation rates in 2020 will increase on weekdays by a factor of 3 relative to 2005 and will be comparable to 1995 weekday and 2005 Sunday rates. Ozone production will become precursor limited on Sundays in 2020, but with higher initial rates than 2005. Although a greater NOx reduction scenario in 2020 of-75% will result in even higher initial ozone formation rates, precursor limitation is reached quickly, leading to a further shift westward in the location of peak ozone levels. However, ozone levels will likely be lower in downwind areas where transport is more important than local production of ozone. The ambient versus emission inventory reconciliation indicates a factor of 2 underestimation of VOC emissions in 2009 relative to NOx. Other analyses suggest that there is an overall increase in VOC emissions on hot days that is not fully accounted for by emission inventory estimates. Air quality models using emission inventories that underestimate VOC emissions relative to NOx may lead to inaccurate forecasting of the consequence of emission reductions. Implications: The rate and efficiency of ozone formation and accumulation in the SoCAB is more rapid than would be indicated by air quality model simulations based on the current inventory. Projected reductions in NOx emissions without concurrent reductions in VOC emissions will likely cause ozone to increase during the next decade within central regions of the SoCAB compared with a flat or slightly declining trend in far downwind locations. Air quality statistics that are commonly used to track progress toward attainment, such as basin-wide ozone design value and standard exceedances mask these varying trends within the Basin. C1 [Fujita, Eric M.; Campbell, David E.] Nevada Syst Higher Educ, Desert Res Inst, Div Atmospher Sci, Reno, NV USA. [Stockwell, William R.] Howard Univ, Dept Chem, Washington, DC 20059 USA. [Lawson, Douglas R.] Natl Renewable Energy Lab, Golden, CO USA. RP Fujita, EM (reprint author), Desert Res Inst, Div Atmospher Sci, 2215 Raggio Pkwy, Reno, NV 89512 USA. EM Eric.Fujita@dri.edu OI Stockwell, William/0000-0002-7509-6575 FU Department of Energy Office of Vehicle Technologies through the National Renewable Energy Laboratory FX This project was funded by the Department of Energy Office of Vehicle Technologies (Dr. James Eberhardt, Chief Scientist) through the National Renewable Energy Laboratory. The authors thank Joe Cassmasi and Xinqiu Zhang of the South Coast Air Quality Management District for the modeling emission inventory data. NR 32 TC 11 Z9 11 U1 4 U2 28 PU TAYLOR & FRANCIS INC PI PHILADELPHIA PA 325 CHESTNUT ST, SUITE 800, PHILADELPHIA, PA 19106 USA SN 1096-2247 J9 J AIR WASTE MANAGE JI J. Air Waste Manage. Assoc. PD JAN 1 PY 2013 VL 63 IS 1 BP 54 EP 69 DI 10.1080/10962247.2012.735211 PG 16 WC Engineering, Environmental; Environmental Sciences; Meteorology & Atmospheric Sciences SC Engineering; Environmental Sciences & Ecology; Meteorology & Atmospheric Sciences GA 194LZ UT WOS:000322636100007 PM 23447864 ER PT S AU Hehlen, MP Mueller, AH Weisse-Bernstein, NR Epstein, RI AF Hehlen, Markus P. Mueller, Alexander H. Weisse-Bernstein, Nina R. Epstein, Richard I. BE Epstein, RI Seletskiy, DV SheikBahae, M TI Electrocaloric refrigerator using electrohydrodynamic flows in dielectric fluids SO LASER REFRIGERATION OF SOLIDS VI SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Laser Refrigeration of Solids VI CY FEB 06-07, 2013 CL San Francisco, CA SP SPIE DE Electrocaloric refrigerator; electrohydrodynamic (EHD) flow; dielectric fluid; thin film heat switch ID THERMAL-CONDUCTIVITY; ROOM-TEMPERATURE; HEAT-TRANSFER; FILM; EFFICIENCY; PUMP AB Heat switches are a key enabling element of efficient refrigerators that are based on the electrocaloric effect. We demonstrate a new concept for a heat switch that is based on micro-scale electrohydrodynamic (EHD) flows in thin layers of dielectric fluids. In this device, convective flow of the fluid is controlled by applying an electric field across the fluid layer. This creates a heat switch that can be cycled between a "closed" state with efficient convective heat transport and an "open" state with less efficient conductive heat transport. Substantial switching of the thermal transport coefficient was achieved in 500 mu m thick layers of commercial hydrofluoroethers and bias voltages of typically 390 V. The efficacy of the heat switch varied by almost four orders of magnitude for different biasing schemes. The highest efficacy was achieved by biasing a patterned strip electrode and using a planar ground electrode. A preliminary experiment found a thermal conductivity contrast of 4.7 +/- 1.1 for the switch in the closed vs. open state. We also characterize the electrocaloric response of commercial multilayer ceramic chip capacitors and show that they can serve as serve as a useful surrogate material for first-generation electrocaloric refrigerators until higher performing multilayer structures of ferroelectric polymers are available. C1 [Hehlen, Markus P.; Mueller, Alexander H.; Weisse-Bernstein, Nina R.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Hehlen, MP (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. OI Epstein, Richard/0000-0002-3929-4363 NR 36 TC 1 Z9 1 U1 0 U2 9 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9407-8 J9 PROC SPIE PY 2013 VL 8638 AR 86380D DI 10.1117/12.2004009 PG 13 WC Optics; Physics, Applied SC Optics; Physics GA BFX97 UT WOS:000321854200008 ER PT J AU Woodson, LE Wells, BK Weber, PK MacFarlane, RB Whitman, GE Johnson, RC AF Woodson, Lindsay E. Wells, Brian K. Weber, Peter K. MacFarlane, R. Bruce Whitman, George E. Johnson, Rachel C. TI Size, growth, and origin-dependent mortality of juvenile Chinook salmon Oncorhynchus tshawytscha during early ocean residence SO MARINE ECOLOGY PROGRESS SERIES LA English DT Article DE Critical period; Otolith; California Current; Hatchery; Gulf of the Farralones ID SELECTIVE MORTALITY; CALIFORNIA CURRENT; BRITISH-COLUMBIA; CENTRAL VALLEY; CHUM SALMON; COHO SALMON; PINK SALMON; OTOLITH MICROSTRUCTURE; MARINE MORTALITY; SOCKEYE-SALMON AB Selective mortality during early life history stages can have significant population-level consequences, yet critical periods when selective mortality occurs, the strength of selection, and under what environmental conditions can be difficult to identify. Here, we used otolith microstructure and chemistry to examine the factors potentially linked to selective mortality of juvenile fall-run Chinook salmon Oncorhynchus tshawytscha from California's Central Valley during early ocean residence. Back-calculated size and growth rates of the population were compared across 3 sample periods: as juveniles exited the San Francisco Bay estuary (estuary-exit), after their first month at sea (summer-ocean) and 5 mo after ocean entry (fall-ocean). We compared mortality dynamics during years of exceptional recruitment (addition of individuals to harvestable population; 2000 and 2001) to a year of poor recruitment (2005). Otoliths from 2005 were also analyzed for sulfur isotopes to discern hatchery from naturally spawned stock. Significant size and growth-rate selective mortality were detected during the first month at sea in the low recruitment year of 2005, but not in 2000 and 2001. Individuals that were larger and growing faster during freshwater and estuarine rearing were more likely to survive to summer and fall in the low recruitment year. There was a slight, but insignificant, increase in the proportion of hatchery to naturally spawned individuals from estuary-exit to fall-ocean, suggesting that fish from neither origin were overwhelmingly favored. Our results suggest that Central Valley Chinook salmon can be subject to significant size and growth-rate selective mortality resulting in low adult abundance, and this mortality appears independent of origin. C1 [Woodson, Lindsay E.; Wells, Brian K.; MacFarlane, R. Bruce] NOAA, Fisheries Ecol Div, Southwest Fisheries Sci Ctr, Natl Marine Fisheries Serv, Santa Cruz, CA 95060 USA. [Weber, Peter K.] Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. [Whitman, George E.; Johnson, Rachel C.] Univ Calif Santa Cruz, Inst Marine Sci, Santa Cruz, CA 95064 USA. [Johnson, Rachel C.] US Bur Reclamat, Bay Delta Off, Sacramento, CA 95825 USA. RP Woodson, LE (reprint author), NOAA, Fisheries Ecol Div, Southwest Fisheries Sci Ctr, Natl Marine Fisheries Serv, 110 Shaffer Rd, Santa Cruz, CA 95060 USA. EM lindsay.e.woodson@gmail.com FU California Sea Grant; Bureau of Reclamation for the Central Valley Aquatic Ecosystem Investigations , alifornia Cooperative Ecosystem Studies Unit; NOAA fisheries Southwest Fisheries Science Center FX We acknowledge the essential support of the Delta Science Fellows Program administered by California Sea Grant and funded by the Bureau of Reclamation for the Central Valley Aquatic Ecosystem Investigations as part of the California Cooperative Ecosystem Studies Unit. This publication was prepared by L.E.W. under USBR Agreement R09AC20043, California Sea Grant College Program Project R/SFBR-31. The statements, findings, conclusions, and recommendations are those of the author(s) and do not necessarily reflect the views of California Sea Grant, Bureau of Reclamation or the US Department of the Interior. We thank A. Schmitt and K. McKeegan for invaluable assistance and use of the secondary ion mass spectrometer at the University of California, Los Angeles, WM Keck Foundation Center for Isotope Geochemistry for otolith sulfur isotopic analyses, F. Loge for providing laboratory space and use of equipment at the University of California Davis, and NOAA fisheries Southwest Fisheries Science Center for additional funding. Thank you to the SWFSC Salmon Ecology team for the collection and preservation of the historical data sets. We thank C. Grimes, C. Michel, C. Phillis, and 3 anonymous reviewers whose comments greatly improved this manuscript. We are particularly grateful to P. Koch, E. Van Nieuwenhuyse, J. Hannon, and S. Oh for their support and assistance in making this project possible. NR 62 TC 25 Z9 24 U1 1 U2 38 PU INTER-RESEARCH PI OLDENDORF LUHE PA NORDBUNTE 23, D-21385 OLDENDORF LUHE, GERMANY SN 0171-8630 EI 1616-1599 J9 MAR ECOL PROG SER JI Mar. Ecol.-Prog. Ser. PY 2013 VL 487 BP 163 EP 175 DI 10.3354/meps10353 PG 13 WC Ecology; Marine & Freshwater Biology; Oceanography SC Environmental Sciences & Ecology; Marine & Freshwater Biology; Oceanography GA 193QV UT WOS:000322577400014 ER PT S AU Jameson, JR Albert, CI Busse, B Smith, PA Harris, GF AF Jameson, John R. Albert, Carolyne I. Busse, Bjoern Smith, Peter A. Harris, Gerald F. BE Weaver, JB Molthen, RC TI 3D micron-scale imaging of the cortical bone canal network in human osteogenesis imperfecta (OI) SO MEDICAL IMAGING 2013: BIOMEDICAL APPLICATIONS IN MOLECULAR, STRUCTURAL, AND FUNCTIONAL IMAGING SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Medical Imaging - Biomedical Applications in Molecular, Structural, and Functional Imaging CY FEB 10-13, 2013 CL Lake Buena Vista, FL SP SPIE, Aeroflex Inc, Univ Cent Florida, CREOL Coll Opt & Photon, DQE Instruments Inc, Medtronic Inc, PIXELTEQ DE Osteogenesis imperfecta; brittle bone disease; micro-computed tomography; synchrotron; cortical porosity; bone microstructure; strength; pediatric bone ID SYNCHROTRON-RADIATION MICROTOMOGRAPHY; HISTOMORPHOMETRY; ADULTS; TOUGHNESS; CHILDREN; IMAGEJ AB Osteogenesis imperfecta (OI) is a genetic disorder leading to increased bone fragility. Recent work has shown that the hierarchical structure of bone plays an important role in determining its mechanical properties and resistance to fracture. The current study represents one of the first attempts to characterize the 3D structure and composition of cortical bone in OI at the micron-scale. A total of 26 pediatric bone fragments from 18 individuals were collected during autopsy (N-c=5) or routing orthopaedic procedures (N-OI=13) and imaged by microtomography with a synchrotron light source (SR mu CT) for several microstructural parameters including cortical porosity (Ca.V/TV), canal surface to tissue volume (Ca.S/TV), canal diameter (Ca.Dm), canal separation (Ca.Sp), canal connectivity density (Ca.ConnD), and volumetric tissue mineral density (TMD). Results indicated significant differences in all imaging parameters between pediatric controls and OI tissue, with OI bone showing drastically increased cortical porosity, canal diameter, and connectivity. Preliminary mechanical testing revealed a possible link between cortical porosity and strength. Together these results suggest that the pore network in OI contributes greatly to its reduced mechanical properties. C1 [Jameson, John R.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. RP Jameson, JR (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, 1 Cyclotron Rd, Berkeley, CA 94720 USA. RI Busse, Bjorn/O-8462-2016 OI Busse, Bjorn/0000-0002-3099-8073 NR 25 TC 0 Z9 0 U1 1 U2 4 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9446-7 J9 PROC SPIE PY 2013 VL 8672 AR 86721L DI 10.1117/12.2007209 PG 9 WC Engineering, Biomedical; Optics; Radiology, Nuclear Medicine & Medical Imaging SC Engineering; Optics; Radiology, Nuclear Medicine & Medical Imaging GA BFY76 UT WOS:000321907600053 ER PT S AU Williams, AC Hitt, A Voisin, S Tourassi, G AF Williams, Alex C. Hitt, Austin Voisin, Sophie Tourassi, Georgia BE Novak, CL Aylward, S TI Automated assessment of bilateral breast volume asymmetry as a breast cancer biomarker during mammographic screening SO MEDICAL IMAGING 2013: COMPUTER-AIDED DIAGNOSIS SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Medical Imaging - Computer-Aided Diagnosis CY FEB 12-14, 2013 CL Lake Buena Vista, FL SP SPIE, Aeroflex Inc, Univ Cent Florida, CREOL Coll Opt & Photon, DQE Instruments Inc, Medtronic Inc, PIXELTEQ DE mammography; breast cancer; diagnosis; fluctuating asymmetry; imaging biomarker ID COMPUTERIZED DETECTION; DIGITIZED MAMMOGRAMS; LOBULAR CARCINOMA; MASSES; SIZE; SUBTRACTION AB The biological concept of bilateral symmetry as a marker of developmental stability and good health is well established. Although most individuals deviate slightly from perfect symmetry, humans are essentially considered bilaterally symmetrical. Consequently, increased fluctuating asymmetry of paired structures could be an indicator of disease. There are several published studies linking bilateral breast size asymmetry with increased breast cancer risk. These studies were based on radiologists' manual measurements of breast size from mammographic images. We aim to develop a computerized technique to assess fluctuating breast volume asymmetry in screening mammograms and investigate whether it correlates with the presence of breast cancer. Using a large database of screening mammograms with known ground truth we applied automated breast region segmentation and automated breast size measurements in CC and MLO views using three well established methods. All three methods confirmed that indeed patients with breast cancer have statistically significantly higher fluctuating asymmetry of their breast volumes. However, statistically significant difference between patients with cancer and benign lesions was observed only for the MLO views. The study suggests that automated assessment of global bilateral asymmetry could serve as a breast cancer risk biomarker for women undergoing mammographic screening. Such biomarker could be used to alert radiologists or computer-assisted detection (CAD) systems to exercise increased vigilance if higher than normal cancer risk is suspected. C1 [Voisin, Sophie; Tourassi, Georgia] Oak Ridge Natl Lab, Biomed Sci & Engn Ctr, Oak Ridge, TN 37831 USA. RP Williams, AC (reprint author), Middle Tennessee State Univ, Dept Comp Sci, Murfreesboro, TN 37132 USA. EM tourassig@ornl.gov OI Voisin, Sophie/0000-0002-9726-4605; Tourassi, Georgia/0000-0002-9418-9638 NR 23 TC 0 Z9 0 U1 0 U2 5 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9444-3 J9 PROC SPIE PY 2013 VL 8670 AR 86701A DI 10.1117/12.2008019 PG 6 WC Engineering, Electrical & Electronic; Optics; Radiology, Nuclear Medicine & Medical Imaging SC Engineering; Optics; Radiology, Nuclear Medicine & Medical Imaging GA BGC32 UT WOS:000322261500044 ER PT J AU Jiang, DE AF Jiang, De-en TI The expanding universe of thiolated gold nanoclusters and beyond SO NANOSCALE LA English DT Article ID STRUCTURAL EVOLUTION; PROTECTED AU-38; ELECTRONIC-STRUCTURE; KDA GOLD; OPTICAL-PROPERTIES; MASS-SPECTROMETRY; CRYSTAL-STRUCTURE; 1ST PRINCIPLES; CLUSTERS; NANOPARTICLES AB Thiolated gold nanoclusters form a universe of their own. Researchers in this field are constantly pushing the boundary of this universe by identifying new compositions and in a few "lucky" cases, solving their structures. Such solved structures, even if there are only few, provide important hints for predicting the many identified compositions that are yet to be crystallized or structure determined. Structure prediction is the most pressing issue for a computational chemist in this field. The success of the density functional theory method in gauging the energetic ordering of isomers for thiolated gold clusters has been truly remarkable, but to predict the most stable structure for a given composition remains a great challenge. In this feature article from a computational chemist's point of view, the author shows how one understands and predicts structures for thiolated gold nanoclusters based on his old and new results. To further entertain the reader, the author also offers several "imaginative" structures, claims, and challenges for this field. C1 Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. RP Jiang, DE (reprint author), Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. EM jiangd@ornl.gov RI Jiang, De-en/D-9529-2011 OI Jiang, De-en/0000-0001-5167-0731 FU Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy; Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231] FX This work was supported by the Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy. 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. As usual in a scientific endeavor, the author benefited greatly from collaborations, discussions, and suggestions from many colleagues in the field of thiolated gold nanoclusters over the years. NR 101 TC 88 Z9 88 U1 6 U2 69 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 16 BP 7149 EP 7160 DI 10.1039/c3nr34192e PG 12 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA 190CP UT WOS:000322315600003 PM 23629814 ER PT J AU Kang, HC Yan, HF Chu, YS Lee, SY Kim, J Nazaretski, E Kim, C Seo, O Noh, DY Macrander, AT Stephenson, GB Maser, J AF Kang, Hyon Chol Yan, Hanfei Chu, Yong S. Lee, Su Yong Kim, Jungdae Nazaretski, Evgeny Kim, Chan Seo, Okkyun Noh, Do Young Macrander, Albert T. Stephenson, G. Brian Maser, Joerg TI Oxidation of PtNi nanoparticles studied by a scanning X-ray fluorescence microscope with multi-layer Laue lenses SO NANOSCALE LA English DT Article ID COALESCENCE; NANOSCALE; NANOCRYSTALS; NANOPROBE; CATALYST; BEAMLINE; SURFACES; DESIGN AB We report a study of the oxidation process of individual PtNi nanoparticles (NPs) conducted with a novel scanningmulti-layer Laue lens X-ray microscope. The elemental maps reveal that alloyed PtNi NPs were transformed into Pt/NiO core-shell NPs by thermal oxidation. The observations furthermore indicate that a coalescence of Pt/NiO core-shell NPs occurred during oxidation. C1 [Kang, Hyon Chol] Chosun Univ, Dept Adv Engn Mat, Kwangju 501759, South Korea. [Yan, Hanfei; Chu, Yong S.; Kim, Jungdae; Nazaretski, Evgeny] Brookhaven Natl Lab, Natl Synchrotron Light Source 2, Upton, NY 11973 USA. [Lee, Su Yong; Kim, Chan; Seo, Okkyun; Noh, Do Young] Gwangju Inst Sci & Technol, Sch Mat Sci & Engn, Dept Photon & Appl Phys, Dept Nanobio Mat & Elect, Kwangju 500712, South Korea. [Macrander, Albert T.; Stephenson, G. Brian; Maser, Joerg] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. [Macrander, Albert T.; Stephenson, G. Brian; Maser, Joerg] Argonne Natl Lab, Ctr Nanoscale Mat, Argonne, IL 60439 USA. RP Kang, HC (reprint author), Chosun Univ, Dept Adv Engn Mat, Kwangju 501759, South Korea. EM kanghc@chosun.ac.kr RI Maser, Jorg/K-6817-2013; Yan, Hanfei/F-7993-2011 OI Yan, Hanfei/0000-0001-6824-0367 FU Korean National Research Foundation through the NCRC [R15-2008-006-00000-0]; WCU [R31-2008-000-10026-0]; Department of Energy, Office of Basic Energy Sciences [DE-AC-02-06CH11357, DE-AC-02-98CH10886]; [2010-0023604] FX The authors thank R. Conley, N. Bouet, and J. Zhou for producing MLL optics. We wish to thank D. Shu, who developed the SMM. This work was partially supported by the Korean National Research Foundation through the NCRC (R15-2008-006-00000-0), WCU (R31-2008-000-10026-0), and basic research program (2010-0023604). We also acknowledge the GIST Top Brand grant. Work at Argonne, including the use of the Advanced Photon Source and Center for Nanoscale Materials, was supported by the Department of Energy, Office of Basic Energy Sciences under contract DE-AC-02-06CH11357. Work at Brookhaven was supported by the Department of Energy, Office of Basic Energy Sciences under contract DE-AC-02-98CH10886. NR 25 TC 10 Z9 10 U1 2 U2 25 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 16 BP 7184 EP 7187 DI 10.1039/c3nr00396e PG 4 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA 190CP UT WOS:000322315600006 PM 23674261 ER PT J AU Petkov, V Shan, SY Chupas, P Yin, J Yang, LF Luo, J Zhong, CJ AF Petkov, Valeri Shan, Shiyao Chupas, Peter Yin, Jun Yang, Lefu Luo, Jin Zhong, Chuan-Jian TI Noble-transition metal nanoparticle breathing in a reactive gas atmosphere SO NANOSCALE LA English DT Article ID PAIR DISTRIBUTION FUNCTION; OXYGEN REDUCTION REACTION; X-RAY-DIFFRACTION; LATTICE-PARAMETER; NANOCRYSTALS; SURFACES; ENERGY; STRAIN; ALLOYS; ELECTROCATALYSTS AB In situ high-energy X-ray diffraction coupled to atomic pair distribution function analysis is used to obtain fundamental insight into the effect of the reactive gas environment on the atomic-scale structure of metallic particles less than 10 nm in size. To substantiate our recent discovery we investigate a wide range of noble-transition metal nanoparticles and confirm that they expand and contract radially when treated in oxidizing (O-2) and reducing (H-2) atmospheres, respectively. The results are confirmed by supplementary XAFS experiments. Using computer simulations guided by the experimental diffraction data we quantify the effect in terms of both relative lattice strain and absolute atomic displacements. In particular, we show that the effect leads to a small percent of extra surface strain corresponding to several tenths of Angstrom displacements of the atoms at the outmost layer of the particles. The effect then gradually decays to zero within 4 atomic layers inside the particles. We also show that, reminiscent of a breathing type structural transformation, the effect is reproducible and reversible. We argue that because of its significance and widespread occurrence the effect should be taken into account in nanoparticle research. C1 [Petkov, Valeri] Cent Michigan Univ, Dept Phys, Mt Pleasant, MI 48859 USA. [Shan, Shiyao; Yin, Jun; Yang, Lefu; Luo, Jin; Zhong, Chuan-Jian] SUNY Binghamton, Dept Chem, Binghamton, NY 13902 USA. [Chupas, Peter] Argonne Natl Lab, Adv Photon Source, Xray Sci Div, Argonne, IL 60439 USA. RP Petkov, V (reprint author), Cent Michigan Univ, Dept Phys, Mt Pleasant, MI 48859 USA. EM petko1vg@cmich.edu; chupas@aps.anl.gov; cjzhong@binghamton.edu RI Zhong, Chuan-Jian/D-3394-2013 FU DOE [DESC0006877, DE-AC02-06CH11357] FX This work was supported by DOE Grant No. DESC0006877. Work at APS is supported by the DOE under Contract No. DE-AC02-06CH11357. NR 52 TC 11 Z9 11 U1 3 U2 21 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 16 BP 7379 EP 7387 DI 10.1039/c3nr02582a PG 9 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA 190CP UT WOS:000322315600036 PM 23828235 ER PT J AU Li, Q Xu, P Zhang, B Wu, G Zhao, HT Fu, EG Wang, HL AF Li, Qing Xu, Ping Zhang, Bin Wu, Gang Zhao, Hongtao Fu, Engang Wang, Hsing-Lin TI Self-supported Pt nanoclusters via galvanic replacement from Cu2O nanocubes as efficient electrocatalysts SO NANOSCALE LA English DT Article ID POROUS PLATINUM NANOPARTICLES; SHAPE-CONTROLLED SYNTHESIS; OXYGEN-REDUCTION; ENHANCED PERFORMANCE; SINGLE-CRYSTALLINE; FUEL-CELLS; NANOWIRES; NANOTUBES; NANOCRYSTALS; GROWTH AB A novel synthesis method for self-supported Pt nanoclusters (Pt NCs) comprised of interconnected 2-3 nm Pt nanoparticles was developed by employing the galvanic replacement process between Cu2O nanocubes and PtCl42- ions. This discovered synthesis procedure eliminates the use of any polymer capping agents and enables a catalytically clean Pt surface. It is determined that the presence of H+ ions is crucial for initializing the galvanic replacement reaction. The electrocatalytic performances of the Pt NCs were tested for both oxygen reduction and methanol oxidation reactions, which showed higher electrochemical activity and greater long-term durability as compared with commercial Pt materials. C1 [Li, Qing; Xu, Ping; Zhang, Bin; Zhao, Hongtao] Harbin Inst Technol, Dept Chem, Harbin 150001, Peoples R China. [Xu, Ping; Wang, Hsing-Lin] Los Alamos Natl Lab, Div Chem, Los Alamos, NM 87545 USA. [Li, Qing; Wu, Gang; Fu, Engang] Los Alamos Natl Lab, Mat Phys & Applicat Div, Los Alamos, NM 87545 USA. RP Xu, P (reprint author), Harbin Inst Technol, Dept Chem, Harbin 150001, Peoples R China. EM pxu@hit.edu.cn; hwang@lanl.gov RI Wu, Gang/E-8536-2010; Li, Qing/G-4502-2011; Xu, Ping/I-1910-2013 OI Wu, Gang/0000-0003-4956-5208; Li, Qing/0000-0003-4807-030X; Xu, Ping/0000-0002-1516-4986 FU China Postdoctor Fund; NSFC [21203045, 21101041, 21003029, 21071037, 91122002]; Fundamental Research Funds for the Central Universities [HIT.NSRIF. 2010065, 2011017, HIT.BRETIII. 201223]; LANL; Laboratory Directed Research and Development (LDRD) fund under the auspices of DOE; Basic Energy Science (BES), Biomaterials program, Materials Sciences and Engineering Division FX PX thanks support from the China Postdoctor Fund, NSFC (no. 21203045, 21101041, 21003029, 21071037, 91122002), Fundamental Research Funds for the Central Universities (no. HIT.NSRIF. 2010065 and 2011017, and HIT.BRETIII. 201223), and Director's Postdoctoral Fellow from LANL. HLW acknowledges the financial support from the Laboratory Directed Research and Development (LDRD) fund under the auspices of DOE. This work is partially supported by Basic Energy Science (BES), Biomaterials program, Materials Sciences and Engineering Division. NR 31 TC 26 Z9 26 U1 5 U2 112 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 16 BP 7397 EP 7402 DI 10.1039/c3nr02243a PG 6 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA 190CP UT WOS:000322315600038 PM 23828129 ER PT J AU Sharma, R Xu, YW Kim, SW Schueller, MJ Alexoff, D Smith, SD Wang, W Schlyer, D AF Sharma, Ramesh Xu, Youwen Kim, Sung Won Schueller, Michael J. Alexoff, David Smith, S. David Wang, Wei Schlyer, David TI Carbon-11 radiolabeling of iron-oxide nanoparticles for dual-modality PET/MR imaging SO NANOSCALE LA English DT Article ID POSITRON-EMISSION-TOMOGRAPHY; CU-64-LABELED MAGNETIC NANOPARTICLES; IN-VIVO; FUNCTIONALIZED SILICA; BIODISTRIBUTION; F-18; PARTICLES; CANCER AB Dual-modality imaging, using Magnetic Resonance Imaging (MRI) and Positron Emission Tomography (PET) simultaneously, is a powerful tool to gain valuable information correlating structure with function in biomedicine. The advantage of this dual approach is that the strengths of one modality can balance the weaknesses of the other. However, success of this technique requires developing imaging probes suitable for both. Here, we report on the development of a nanoparticle labeling procedure via covalent bonding with carbon-11 PET isotope. Carbon-11 in the form of [C-11] methyl iodide was used as a methylation agent to react with carboxylic acid (-COOH) and amine (-NH2) functional groups of ligands bound to the nanoparticles (NPs). The surface coating ligands present on superparamagnetic iron-oxide nanoparticles (SPIO NPs) were radiolabeled to achieve dual-modality PET/MR imaging capabilities. The proof-of-concept dual-modality PET/MR imaging using the radiolabeled SPIO NPs was demonstrated in an in vivo experiment. C1 [Sharma, Ramesh; Xu, Youwen; Kim, Sung Won; Schueller, Michael J.; Alexoff, David; Smith, S. David; Schlyer, David] Brookhaven Natl Lab, Upton, NY 11973 USA. [Sharma, Ramesh] Battelle Mem Inst, Columbus, OH 43201 USA. [Wang, Wei] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. RP Sharma, R (reprint author), Brookhaven Natl Lab, Upton, NY 11973 USA. EM ramesharma26@gmail.com; schlyer@bnl.gov RI Wang, Wei/B-5924-2012 FU U.S. Department of Energy Office of Biological and Environmental Research [DE-AC02-98CH10886]; Battelle Memorial Institute FX This work was carried out at Brookhaven National Laboratory supported by the U.S. Department of Energy Office of Biological and Environmental Research under contract DE-AC02-98CH10886. R.S. was supported by the Battelle Memorial Institute. Lihua Zhang is acknowledged for assistance with TEM data acquisition. NR 50 TC 12 Z9 13 U1 5 U2 45 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 16 BP 7476 EP 7483 DI 10.1039/c3nr02519e PG 8 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA 190CP UT WOS:000322315600048 PM 23832243 ER PT J AU Kronawitter, CX Zegkinoglou, I Shen, SH Guo, JH Himpsel, FJ Mao, SS Vayssieres, L AF Kronawitter, Coleman X. Zegkinoglou, Ioannis Shen, Shaohua Guo, Jinghua Himpsel, Franz J. Mao, Samuel S. Vayssieres, Lionel TI On the orbital anisotropy in hematite nanorod-based photoanodes SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID X-RAY-ABSORPTION; ELECTRONIC-STRUCTURE; SOLAR-CELLS; ALPHA-FE2O3; POLARIZATION; SCATTERING; ARRAYS; FILMS; PHOTOELECTRODES; DEPENDENCE AB The orbital anisotropy of hematite (alpha-Fe2O3) nanorod arrays, an engineered structure commonly investigated for applications in solar water oxidation photoanodes, is probed using polarization-dependent soft X-ray absorption spectroscopy at the O K-edge and at the Fe L-2,L-3-edge. Thereby the unoccupied states of alpha-Fe2O3 are examined. In the lowest energy region these are found to be strongly-hybridized Fe 3d (a(1g)) orbitals and O2- ligand 2p orbitals, oriented along the c-axis. For [110]-oriented alpha-Fe2O3 nanocrystals the observed direction of strong hybridization is parallel to the substrate surface (perpendicular to the direction of electron conduction and light propagation in operating electrodes). The Fe L-3-edge line shape and aspects of polarization dependence can be reproduced by crystal field atomic multiplet calculations of 2p-to-3d transitions for Fe3+ in the D-3d point group symmetry of metal ions in the corundum structure. Both the O K-edge and Fe L-3-edge spectra possess features that may be related to the high density of surface atoms in this nanoscale system. They are associated with partial coordination and therefore reduced symmetry compared to that for Fe3+ in bulk crystals. C1 [Kronawitter, Coleman X.; Mao, Samuel S.] Univ Calif Berkeley, Dept Mech Engn, Berkeley, CA 94720 USA. [Kronawitter, Coleman X.; Shen, Shaohua; Mao, Samuel S.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. [Zegkinoglou, Ioannis; Himpsel, Franz J.] Univ Wisconsin, Dept Phys, Madison, WI 53706 USA. [Zegkinoglou, Ioannis; Guo, Jinghua] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. [Shen, Shaohua; Vayssieres, Lionel] Xi An Jiao Tong Univ, Int Res Ctr Renewable Energy, State Key Lab Multiphase Flow Power Engn, Xian 710049, Peoples R China. [Guo, Jinghua] Univ Calif Santa Cruz, Dept Chem & Biochem, Santa Cruz, CA 95064 USA. RP Mao, SS (reprint author), Univ Calif Berkeley, Dept Mech Engn, Berkeley, CA 94720 USA. EM ssmao@lbl.gov; lionelv@xjtu.edu.cn RI Shen, Shaohua/E-9507-2011; Zegkinoglou, Ioannis/H-2343-2013 FU NSF/CMMI [1036076]; U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy; Office of Basic Energy Sciences [DE-SC0006931, DE-AC02-05CH11231, DE-FG02-01ER45917]; International Research Center for Renewable Energy, State Key Laboratory of Multiphase Flow in Power Engineering, Xian Jiaotong University; Thousand Talents plan; National Natural Science Foundation of China [51121092] FX This research has been supported by NSF/CMMI under grant #1036076, by the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy; and by the Office of Basic Energy Sciences under the Contracts DE-SC0006931, DE-AC02-05CH11231 (ALS), DE-FG02-01ER45917 (end station) and by the International Research Center for Renewable Energy, State Key Laboratory of Multiphase Flow in Power Engineering, Xian Jiaotong University, the Thousand Talents plan and the National Natural Science Foundation of China (no. 51121092). NR 44 TC 11 Z9 11 U1 4 U2 62 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 32 BP 13483 EP 13488 DI 10.1039/c3cp52527a PG 6 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 191GQ UT WOS:000322401600025 PM 23839223 ER PT J AU Duan, YH Pfeiffer, H Li, BY Romero-Ibarra, IC Sorescu, DC Luebke, DR Halley, JW AF Duan, Yuhua Pfeiffer, Heriberto Li, Bingyun Romero-Ibarra, Issis C. Sorescu, Dan C. Luebke, David R. Halley, J. Woods TI CO2 capture properties of lithium silicates with different ratios of Li2O/SiO2: an ab initio thermodynamic and experimental approach SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID HIGH-TEMPERATURE; CARBON-DIOXIDE; CRYSTAL-STRUCTURE; ALPHA-QUARTZ; STRUCTURAL-PROPERTIES; ELECTRONIC-PROPERTIES; MOLECULAR-DYNAMICS; REACTION-MECHANISM; KINETIC-ANALYSIS; PARTICLE-SIZE AB The lithium silicates have attracted scientific interest due to their potential use as high-temperature sorbents for CO2 capture. The electronic properties and thermodynamic stabilities of lithium silicates with different Li2O/SiO2 ratios (Li2O, Li8SiO6, Li4SiO4, Li6Si2O7, Li2SiO3, Li2Si2O5, Li2Si3O7, and alpha-SiO2) have been investigated by combining first-principles density functional theory with lattice phonon dynamics. All these lithium silicates examined are insulators with band-gaps larger than 4.5 eV. By decreasing the Li2O/SiO2 ratio, the first valence bandwidth of the corresponding lithium silicate increases. Additionally, by decreasing the Li2O/SiO2 ratio, the vibrational frequencies of the corresponding lithium silicates shift to higher frequencies. Based on the calculated energetic information, their CO2 absorption capabilities were extensively analyzed through thermodynamic investigations on these absorption reactions. We found that by increasing the Li2O/SiO2 ratio when going from Li2Si3O7 to Li8SiO6, the corresponding lithium silicates have higher CO2 capture capacity, higher turnover temperatures and heats of reaction, and require higher energy inputs for regeneration. Based on our experimentally measured isotherms of the CO2 chemisorption by lithium silicates, we found that the CO2 capture reactions are two-stage processes: (1) a superficial reaction to form the external shell composed of Li2CO3 and a metal oxide or lithium silicate secondary phase and (2) lithium diffusion from bulk to the surface with a simultaneous diffusion of CO2 into the shell to continue the CO2 chemisorption process. The second stage is the rate determining step for the capture process. By changing the mixing ratio of Li2O and SiO2, we can obtain different lithium silicate solids which exhibit different thermodynamic behaviors. Based on our results, three mixing scenarios are discussed to provide general guidelines for designing new CO2 sorbents to fit practical needs. C1 [Duan, Yuhua; Li, Bingyun; Sorescu, Dan C.; Luebke, David R.] US DOE, Natl Energy Technol Lab, Pittsburgh, PA 15236 USA. [Pfeiffer, Heriberto; Romero-Ibarra, Issis C.] Univ Nacl Autonoma Mexico, Inst Invest Mat, Mexico City 04510, DF, Mexico. [Li, Bingyun] W Virginia Univ, Sch Med, Morgantown, WV 26506 USA. [Halley, J. Woods] Univ Minnesota, Sch Phys & Astron, Minneapolis, MN 55455 USA. RP Duan, YH (reprint author), US DOE, Natl Energy Technol Lab, 236 Cochrans Mill Rd, Pittsburgh, PA 15236 USA. EM yuhua.duan@netl.doe.gov RI Duan, Yuhua/D-6072-2011; OI Duan, Yuhua/0000-0001-7447-0142; Pfeiffer, Heriberto/0000-0002-6217-3420 NR 96 TC 28 Z9 28 U1 8 U2 63 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 32 BP 13538 EP 13558 DI 10.1039/c3cp51659h PG 21 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 191GQ UT WOS:000322401600032 PM 23824271 ER PT J AU McGrath, MJ Kuo, IFW Ngouana, WBF Ghogomu, JN Mundy, CJ Marenich, AV Cramer, CJ Truhlar, DG Siepmann, JI AF McGrath, Matthew J. Kuo, I-F. Will Ngouana, Brice F. W. Ghogomu, Julius N. Mundy, Christopher J. Marenich, Aleksandr V. Cramer, Christopher J. Truhlar, Donald G. Siepmann, J. Ilja TI Calculation of the Gibbs free energy of solvation and dissociation of HCl in water via Monte Carlo simulations and continuum solvation models SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID HYDROCHLORIC-ACID SOLUTIONS; VAPOR-LIQUID-EQUILIBRIA; MOLECULAR-DYNAMICS SIMULATION; DENSITY-FUNCTIONAL THEORY; HENRY LAW CONSTANT; AQUEOUS-SOLUTION; AB-INITIO; HYDROGEN-CHLORIDE; 1ST PRINCIPLES; PHASE-EQUILIBRIA AB The Gibbs free energy of solvation and dissociation of hydrogen chloride in water is calculated through a combined molecular simulation/quantum chemical approach at four temperatures between T = 300 and 450 K. The Gibbs free energy is first decomposed into the sum of two components: the Gibbs free energy of transfer of molecular HCl from the vapor to the aqueous liquid phase and the standard-state Gibbs free energy of acid dissociation of HCl in aqueous solution. The former quantity is calculated using Gibbs ensemble Monte Carlo simulations using either Kohn-Sham density functional theory or a molecular mechanics force field to determine the system's potential energy. The latter Gibbs free energy contribution is computed using a continuum solvation model utilizing either experimental reference data or micro-solvated clusters. The predicted combined solvation and dissociation Gibbs free energies agree very well with available experimental data. C1 [McGrath, Matthew J.] CEA Orme Merisiers, Lab Sci Climat & Environm, F-91191 Gif Sur Yvette, France. [McGrath, Matthew J.; Marenich, Aleksandr V.; Cramer, Christopher J.; Truhlar, Donald G.; Siepmann, J. Ilja] Univ Minnesota, Chem Theory Ctr, Dept Chem, Minneapolis, MN 55455 USA. [McGrath, Matthew J.; Marenich, Aleksandr V.; Cramer, Christopher J.; Truhlar, Donald G.; Siepmann, J. Ilja] Univ Minnesota, Supercomp Inst, Minneapolis, MN 55455 USA. [Kuo, I-F. Will] Lawrence Livermore Natl Lab, Phys & Life Sci Directorate, Livermore, CA 94550 USA. [Ngouana, Brice F. W.; Ghogomu, Julius N.] Univ Dschang, Dept Chem, Dschang, Cameroon. [Ngouana, Brice F. W.] Lab Subatech, F-44307 Nantes 3, France. [Cramer, Christopher J.] Pacific NW Natl Lab, Div Phys Sci, Richland, WA 99352 USA. [Siepmann, J. Ilja] Univ Minnesota, Dept Chem Engn & Mat Sci, Minneapolis, MN 55455 USA. RP McGrath, MJ (reprint author), CEA Orme Merisiers, Lab Sci Climat & Environm, F-91191 Gif Sur Yvette, France. EM matthew.mcgrath@lsce.ipsl.fr RI Truhlar, Donald/G-7076-2015; Cramer, Christopher/B-6179-2011 OI Truhlar, Donald/0000-0002-7742-7294; Cramer, Christopher/0000-0001-5048-1859 FU National Science Foundation [OISE-0853294, CBET-0756641, CBET-1159837]; U.S. Army Research Laboratory [W911NF09-100377]; U.S. Department of Energy by the University of California Lawrence Livermore National Laboratory (LLNL) [W-7405-Eng-48]; US Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences Biosciences; NSF under CDI [CHE-1051396] FX MJM gratefully acknowledges support from a National Science Foundation International Research grant (OISE-0853294). Part of this work was performed during a Peace Corps assignment of MJM at the University of Dschang. Additional financial support from the National Science Foundation (CBET-0756641 and CBET-1159837) and the U.S. Army Research Laboratory under Grant No. W911NF09-100377. Part of this work was performed under the auspices of the U.S. Department of Energy by the University of California Lawrence Livermore National Laboratory (LLNL) under contract No. W-7405-Eng-48. CJM was supported by the US Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences & Biosciences. Pacific Northwest National Laboratory is operated by Battelle for the U.S. Department of Energy. This work was also supported in part by the NSF under CDI Grant No. CHE-1051396. Computer resources were provided by Livermore Computing and the Minnesota Supercomputing Institute. NR 89 TC 10 Z9 10 U1 1 U2 47 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2013 VL 15 IS 32 BP 13578 EP 13585 DI 10.1039/c3cp51762d PG 8 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 191GQ UT WOS:000322401600035 PM 23831584 ER PT J AU Langan, P Chen, JCH AF Langan, Paul Chen, Julian C. -H. TI Seeing the chemistry in biology with neutron crystallography SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID BARRIER HYDROGEN-BOND; PHOTOACTIVE YELLOW PROTEIN; JOINT X-RAY; HIGH-RESOLUTION NEUTRON; PURE-SPERMINE FORM; Z-DNA; CRYSTAL-STRUCTURE; DIISOPROPYL FLUOROPHOSPHATASE; FIBER DIFFRACTION; MACROMOLECULAR CRYSTALLOGRAPHY AB New developments in macromolecular neutron crystallography have led to an increasing number of structures published over the last decade. Hydrogen atoms, normally invisible in most X-ray crystal structures, become visible with neutrons. Using X-rays allows one to see structure, while neutrons allow one to reveal the chemistry inherent in these macromolecular structures. A number of surprising and sometimes controversial results have emerged; because it is difficult to see or predict hydrogen atoms in X-ray structures, when they are seen by neutrons they can be in unexpected locations with important chemical and biological consequences. Here we describe examples of chemistry seen with neutrons for the first time in biological macromolecules over the past few years. C1 [Langan, Paul] Oak Ridge Natl Lab, Biol & Soft Matter Div, Oak Ridge, TN 37831 USA. [Langan, Paul; Chen, Julian C. -H.] Univ Toledo, Dept Chem, Toledo, OH 43606 USA. RP Langan, P (reprint author), Oak Ridge Natl Lab, Biol & Soft Matter Div, Oak Ridge, TN 37831 USA. EM langanpa@ornl.gov RI Langan, Paul/N-5237-2015 OI Langan, Paul/0000-0002-0247-3122 FU Center for Structural Molecular Biology; US Office of Biological and Environmental Research, US Department of Energy [FWP ERKP752]; NIH-NIGMS [R01GM071939]; Scientific User Facilities Division, Office of Basic Energy Sciences, US Department of Energy FX This work was partly supported by the Center for Structural Molecular Biology supported by the US Office of Biological and Environmental Research, US Department of Energy, under FWP ERKP752. PL was partly supported by an NIH-NIGMS funded consortium (R01GM071939) between ORNL and LBNL to develop computational tools for neutron protein crystallography. This research used facilities sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, US Department of Energy. NR 59 TC 4 Z9 4 U1 0 U2 19 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 33 BP 13705 EP 13712 DI 10.1039/c3cp51760h PG 8 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 192WH UT WOS:000322517800002 PM 23852376 ER PT J AU Chatman, S Zarzycki, P Rosso, KM AF Chatman, Shawn Zarzycki, Piotr Rosso, Kevin M. TI Surface potentials of (001), (012), (113) hematite (alpha-Fe2O3) crystal faces in aqueous solution SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID PHOTOELECTROCHEMICAL WATER OXIDATION; ZERO CHARGE; SOLUTION INTERFACE; ELECTRON-AFFINITY; PROTON ADSORPTION; PH; POINTS; OXIDE; UPDATE; MODEL AB Hematite (alpha-Fe2O3) is an important candidate electrode for energy system technologies such as photoelectrochemical water splitting. Conversion efficiency issues with this material are presently being addressed through nanostructuring, doping, and surface modification. However, key electrochemical properties of hematite/electrolyte interfaces remain poorly understood at a fundamental level, in particular those of crystallographically well-defined hematite faces likely present as interfacial components at the grain scale. We report a combined measurement and theory study that isolates and evaluates the equilibrium surface potentials of three nearly defect-free single crystal faces of hematite, titrated from pH 3 to 11.25. We link measured surface potentials with atomic-scale surface topology, namely the ratio and distributions of surface protonation-deprotonation site types expected from the bulk structure. The data reveal face-specific points of zero potential (PZP) relatable to points of zero net charge (PZC) that lie within a small pH window (8.35-8.85). Over the entire pH range the surface potentials show strong non-Nernstian charging at pH extremes separated by a wide central plateau in agreement with surface complexation modeling predictions, but with important face-specific distinctions. We introduce a new surface complexation model based on fitting the entire data set that depends primarily only on the proton affinities of two site types and the two associated electrical double layer capacitances. The data and model show that magnitudes of surface potential biases at the pH extremes are on the order of 100 mV, similar to the activation energy for electron hopping mobility. An energy band diagram for hematite crystallites with specific face expression and pH effects is proposed that could provide a baseline for understanding water splitting performance enhancement effects from nanostructuring, and guide morphology targets and pH for systematic improvements in efficiency. C1 [Chatman, Shawn; Rosso, Kevin M.] Pacific NW Natl Lab, Div Phys Sci, Richland, WA 99352 USA. [Zarzycki, Piotr] Polish Acad Sci, Inst Phys Chem, Warsaw, Poland. RP Chatman, S (reprint author), Pacific NW Natl Lab, Div Phys Sci, Richland, WA 99352 USA. EM shawnm.chatman@pnnl.gov; Kevin.Rosso@pnnl.gov FU U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences Biosciences; U.S. Department of Energy's Office of Biological and Environmental Research; MNiSW [IP2012 059872] FX This work was supported by the Geosciences Research Program in the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences & Biosciences. A portion of this research was performed using EMSL, a national scientific user facility sponsored by the U.S. Department of Energy's Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory. Pacific Northwest National Laboratory (PNNL) is a multi-program national laboratory operated for DOE by Battelle. P.Z. also thanks MNiSW (IP2012 059872) for support. NR 72 TC 25 Z9 25 U1 13 U2 120 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 33 BP 13911 EP 13921 DI 10.1039/c3cp52592a PG 11 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 192WH UT WOS:000322517800024 PM 23846741 ER PT J AU Lewandowska-Andralojc, A Polyansky, DE Zong, RF Thummel, RP Fujita, E AF Lewandowska-Andralojc, Anna Polyansky, Dmitry E. Zong, Ruifa Thummel, Randolph P. Fujita, Etsuko TI Enabling light-driven water oxidation via a low-energy Ru-IV=O intermediate SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID MONONUCLEAR RUTHENIUM COMPLEXES; INDUCED ELECTRON-TRANSFER; CATALYST; LIGANDS; REDOX; SITE; MECHANISM; RADICALS; KINETICS; ANALOGS AB The discovery of catalysts capable of driving water oxidation at relatively low overpotential is a key challenge for efficient photoinduced water oxidation. The mononuclear Ru(II) polypyridyl complex (1) [Ru(NPM)(H2O)(pic)(2)](2+) (NPM = 4-tert-butyl-2,6-di-(1',8'-naphthyrid-2'-yl)-pyridine, pic = 4-picoline) has been examined as a catalyst for visible-light-driven water oxidation in a three-component homogeneous system containing [Ru(bpy)(3)](2+) as a photosensitizer, persulfate as a sacrificial electron acceptor and catalyst 1. In contrast to the well-established water oxidation mechanism via the nucleophilic attack of a water molecule on the high-energy [Ru-V=O](3+) species, a lower-energy "direct pathway" for O-O bond formation via a [Ru-V=O](2+) intermediate was proposed for the first time for the catalyst 1 (Polyansky et al., J. Am. Chem. Soc., 2011, 133, 14649). In this report we successfully demonstrate that this unique proton-coupled low-energy pathway actually takes place with the use of a mild oxidant such as the photogenerated [Ru(bpy)(3)](3+) (1.26 V vs. NHE) to drive water oxidation. The overall quantum yield of 9%, TOF of 0.12 s(-1) and TON of 103 (limited solely by a drop in pH) were found for photochemical water oxidation with 1 using [Ru(bpy)(3)](2+) as a photosensitizer and [S2O8](2-) as a sacrificial electron acceptor. These values render catalyst 1 as one of the most active mononuclear ruthenium-based catalysts for light-driven water oxidation in a homogeneous system. The utilization of a pH-dependent pathway for water oxidation is a new and promising direction as a low-energy pathway. Furthermore, the detailed analysis of individual photochemical steps leading to O-2 evolution provides benchmarks for future mechanistic studies of photo-induced water oxidation catalysis. C1 [Lewandowska-Andralojc, Anna; Polyansky, Dmitry E.; Fujita, Etsuko] Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA. [Zong, Ruifa; Thummel, Randolph P.] Univ Houston, Dept Chem, Houston, TX 77204 USA. RP Polyansky, DE (reprint author), Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA. EM dmitriyp@bnl.gov; fujita@bnl.gov RI Polyansky, Dmitry/C-1993-2009; Lewandowska-Andralojc, Anna/A-8149-2012 OI Polyansky, Dmitry/0000-0002-0824-2296; FU Brookhaven National Laboratory (BNL) [DE-AC02-98CH10886]; U.S. Department of Energy [DE-FG02-07ER15888]; Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences; U.S. Department of Energy under BES Hydrogen Fuel Initiative; Robert A. Welch Foundation [E-621] FX We thank Dr Norman Sutin and Dr Carol Creutz for fruitful discussions, and Dr James T. Muckerman for careful reading of this manuscript. The work at Brookhaven National Laboratory (BNL) was carried out under contract DE-AC02-98CH10886 and the work at Houston was carried out under contract DE-FG02-07ER15888 with the U.S. Department of Energy and supported by its Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences. The BNL authors also thank the U.S. Department of Energy for funding under the BES Hydrogen Fuel Initiative. RZ and RPT also thank the Robert A. Welch Foundation (E-621). NR 51 TC 17 Z9 17 U1 2 U2 38 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2013 VL 15 IS 33 BP 14058 EP 14068 DI 10.1039/c3cp52038b PG 11 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 192WH UT WOS:000322517800038 PM 23860663 ER PT J AU Hearon, K Singhal, P Horn, J Small, W Olsovsky, C Maitland, KC Wilson, TS Maitland, DJ AF Hearon, Keith Singhal, Pooja Horn, John Small, Ward Olsovsky, Cory Maitland, Kristen C. Wilson, Thomas S. Maitland, Duncan J. TI Porous Shape-Memory Polymers SO POLYMER REVIEWS LA English DT Review DE shape memory polymer foam; porous active material; stimuli-responsive polymers ID SELF-DEPLOYABLE STRUCTURES; SYNTACTIC FOAM; THERMOMECHANICAL CHARACTERIZATION; BIOMEDICAL APPLICATIONS; POLYURETHANE FOAMS; SPACE APPLICATIONS; CROSS-LINKING; BEHAVIOR; FABRICATION; NANOCOMPOSITES AB Porous shape memory polymers (SMPs) include foams, scaffolds, meshes, and other polymeric substrates that possess porous three-dimensional macrostructures. Porous SMPs exhibit active structural and volumetric transformations and have driven investigations in fields ranging from biomedical engineering to aerospace engineering to the clothing industry. The present review article examines recent developments in porous SMPs, with focus given to structural and chemical classification, methods of characterization, and applications. We conclude that the current body of literature presents porous SMPs as highly interesting smart materials with potential for industrial use. C1 [Hearon, Keith; Singhal, Pooja; Horn, John; Olsovsky, Cory; Maitland, Kristen C.; Maitland, Duncan J.] Texas A&M Univ, Dept Biomed Engn, College Stn, TX 77843 USA. [Singhal, Pooja; Small, Ward; Wilson, Thomas S.] Lawrence Livermore Natl Lab, Livermore, CA USA. RP Maitland, DJ (reprint author), Texas A&M Univ, Mailstop 3120,5045 Emerging Technol Bldg, College Stn, TX 77843 USA. EM djmaitland@tamu.edu RI Maitland, Kristen/D-6961-2011 OI Maitland, Kristen/0000-0003-0931-0622 FU NIBIB NIH HHS [R01 EB000462] NR 98 TC 27 Z9 27 U1 14 U2 145 PU TAYLOR & FRANCIS INC PI PHILADELPHIA PA 325 CHESTNUT ST, SUITE 800, PHILADELPHIA, PA 19106 USA SN 1558-3724 J9 POLYM REV JI Polym. Rev. PD JAN 1 PY 2013 VL 53 IS 1 BP 41 EP 75 DI 10.1080/15583724.2012.751399 PG 35 WC Polymer Science SC Polymer Science GA 189ZF UT WOS:000322306100003 PM 23646038 ER PT J AU Kang, SH Neale, NR Zhu, K Halverson, AF Yan, YF Frank, AJ AF Kang, Soon Hyung Neale, Nathan R. Zhu, Kai Halverson, Adam F. Yan, Yanfa Frank, Arthur J. TI The effect of a metallic Ni core on charge dynamics in CdS-sensitized p-type NiO nanowire mesh photocathodes SO RSC ADVANCES LA English DT Article ID SOLAR-CELLS; COLLECTION EFFICIENCIES; REDOX COUPLE; FILMS; ELECTROLYTES; TRANSPORT; MECHANISM; SULFIDE; ARRAYS AB We report on the synthesis and photoelectrochemical characterization of photocathodes based on CdS-sensitized Ni-NiO core-shell nanowire mesh inverse opals (IOs). Compared to the NiO-CdS nanowire mesh IO electrode, the hole diffusion coefficient of the CdS-sensitized Ni-NiO core-shell nanowire mesh IO photocathode was one order of magnitude larger, indicating that the Ni core facilitated hole transfer in nanostructured p-type electrodes. As a result, the charge-collection efficiency of the Ni-NiO core-shell nanowire mesh IO electrode was shown to be essentially 100%. C1 [Kang, Soon Hyung; Neale, Nathan R.; Zhu, Kai; Halverson, Adam F.; Yan, Yanfa; Frank, Arthur J.] Natl Renewable Energy Lab, Golden, CO 80401 USA. [Kang, Soon Hyung] Chonnam Natl Univ, Dept Chem Educ, Kwangju 500757, South Korea. [Halverson, Adam F.] GE Global Res, New York, NY 12309 USA. [Yan, Yanfa] Univ Toledo, Dept Phys & Astron, Toledo, OH 43606 USA. RP Kang, SH (reprint author), Natl Renewable Energy Lab, 1617 Cole Blvd, Golden, CO 80401 USA. EM Kai.Zhu@nrel.gov; Arthur.Frank@nrel.gov FU Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy [DE-AC36-08GO28308] FX This work was supported by the Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy, under contract No. DE-AC36-08GO28308. NR 37 TC 0 Z9 0 U1 3 U2 45 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 32 BP 13342 EP 13347 DI 10.1039/c3ra41216d PG 6 WC Chemistry, Multidisciplinary SC Chemistry GA 186TN UT WOS:000322068400041 ER PT J AU Peng, Q Wen, XD De, S AF Peng, Qing Wen, Xiaodong De, Suvranu TI Mechanical stabilities of silicene SO RSC ADVANCES LA English DT Article ID HEXAGONAL BORON-NITRIDE; ELASTIC PROPERTIES; AB-INITIO; GRAPHENE; MONOLAYER; 1ST-PRINCIPLES; CHEMISTRY; GRAPHITE; CRYSTALS AB The mechanical stabilities of planar (g) and low-buckled (b) honeycomb monolayer structures of silicon under various large strains are investigated using density functional theory (DFT). The mechanical properties, including the ultimate stresses, ultimate strains, and high order elastic constants of silicene are predicted, as well as the structure evolutions. Both g-Si and b-Si can sustain large strains (eta >= 0.15) for armchair, zigzag, and biaxial deformation. The third, fourth, and fifth order elastic constants are indispensable for accurate modeling of the mechanical properties under strains larger than 0.03, 0.06, and 0.08 respectively. The second order elastic constants, including in-plane stiffness, are predicted to monotonically increase with pressure while the Poisson ratio monotonically decreases with increasing pressure. Our results on the positive ultimate strengths and strains, second order elastic constants, and the in-plane Young's modulus indicate that both g-Si and b-Si are mechanically stable. C1 [Peng, Qing; De, Suvranu] Rensselaer Polytech Inst, Dept Mech Aerosp & Nucl Engn, Troy, NY 12180 USA. [Wen, Xiaodong] Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. RP Peng, Q (reprint author), Rensselaer Polytech Inst, Dept Mech Aerosp & Nucl Engn, Troy, NY 12180 USA. EM qpeng.org@gmail.com RI Wen, Xiaodong/G-5227-2011; Peng, Qing/F-4246-2010 OI Wen, Xiaodong/0000-0001-8161-9742; Peng, Qing/0000-0002-8281-8636 FU Defense Threat Reduction Agency (DTRA) [BRBAA08-C-2-0130, HDTRA1-13-1-0025] FX The authors would like to acknowledge the generous financial support from the Defense Threat Reduction Agency (DTRA) Grant # BRBAA08-C-2-0130 and # HDTRA1-13-1-0025. NR 56 TC 43 Z9 43 U1 7 U2 51 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 33 BP 13772 EP 13781 DI 10.1039/c3ra41347k PG 10 WC Chemistry, Multidisciplinary SC Chemistry GA 192DO UT WOS:000322464500033 ER PT J AU Rong, G Liu, G Hou, D Zhou, CB AF Rong, Guan Liu, Guang Hou, Di Zhou, Chuang-bing TI Effect of Particle Shape on Mechanical Behaviors of Rocks: A Numerical Study Using Clumped Particle Model SO SCIENTIFIC WORLD JOURNAL LA English DT Article ID STRENGTH; ANGLE; COMPRESSION; DILATANCY; FRICTION; MASSES; DAMAGE AB Since rocks are aggregates of mineral particles, the effect of mineral microstructure on macroscopic mechanical behaviors of rocks is inneglectable. Rock samples of four different particle shapes are established in this study based on clumped particle model, and a sphericity index is used to quantify particle shape. Model parameters for simulation in PFC are obtained by triaxial compression test of quartz sandstone, and simulation of triaxial compression test is then conducted on four rock samples with different particle shapes. It is seen from the results that stress thresholds of rock samples such as crack initiation stress, crack damage stress, and peak stress decrease with the increasing of the sphericity index. The increase of sphericity leads to a drop of elastic modulus and a rise in Poisson ratio, while the decreasing sphericity usually results in the increase of cohesion and internal friction angle. Based on volume change of rock samples during simulation of triaxial compression test, variation of dilation angle with plastic strain is also studied. C1 [Rong, Guan; Liu, Guang; Hou, Di; Zhou, Chuang-bing] Wuhan Univ, State Key Lab Water Resources & Hydropower Engn, Wuhan 430072, Hubei, Peoples R China. [Rong, Guan] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, Berkeley, CA 94720 USA. [Liu, Guang] Wuhan Univ, Minist Educ, Key Lab Rock Mech Hydraul Struct Engn, Wuhan 430072, Peoples R China. RP Rong, G (reprint author), Wuhan Univ, State Key Lab Water Resources & Hydropower Engn, Wuhan 430072, Hubei, Peoples R China. EM rg_mail@163.com RI Zhou, Chuangbing/A-6964-2015; Zhou, Chuang-Bing/B-4254-2017 OI Zhou, Chuangbing/0000-0002-0114-735X; FU National Basic Research Program of China ("973" Program) [2011CB013501, 2010CB732005]; National Natural Science Foundation of China [50979081]; Program for New Century Excellent Talents in University [NCET-11-0406] FX The research work presented in this paper is sponsored by the National Basic Research Program of China ("973" Program) (Grant nos. 2011CB013501 and 2010CB732005), the National Natural Science Foundation of China (Grant no. 50979081) and Program for New Century Excellent Talents in University (Grant no. NCET-11-0406). The authors would like to thank their support. NR 34 TC 5 Z9 5 U1 5 U2 33 PU HINDAWI PUBLISHING CORPORATION PI NEW YORK PA 410 PARK AVENUE, 15TH FLOOR, #287 PMB, NEW YORK, NY 10022 USA SN 1537-744X J9 SCI WORLD J JI Sci. World J. PY 2013 AR 589215 DI 10.1155/2013/589215 PG 12 WC Multidisciplinary Sciences SC Science & Technology - Other Topics GA 195KQ UT WOS:000322701500001 ER PT S AU Kelly, JH Shvydky, A Marozas, JA Guardalben, MJ Kruschwitz, BE Waxer, LJ Dorrer, C Hill, E Okishev, AV Di Nicola, JM AF Kelly, J. H. Shvydky, A. Marozas, J. A. Guardalben, M. J. Kruschwitz, B. E. Waxer, L. J. Dorrer, C. Hill, E. Okishev, A. V. Di Nicola, J. -M. BE Awwal, AAS TI Simulations of the propagation of multiple-FM smoothing by spectral dispersion on OMEGA EP SO HIGH POWER LASERS FOR FUSION RESEARCH II SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on High Power Lasers for Fusion Research II CY FEB 07, 2013 CL San Francisco, CA SP SPIE, NIF DE Fusion lasers; beam smoothing; SSD; polar-drive; dispersion; Miro; simulations; B-integral; beam conditioning ID NATIONAL IGNITION FACILITY; AM CONVERSION; LASER; LIGHT AB A one-dimensional (1-D) smoothing by spectral dispersion (SSD) system for smoothing focal-spot nonuniformities using multiple modulation frequencies has been commissioned on one long-pulse beamline of OMEGA EP, the first use of such a system in a high-energy laser. Frequency modulation (FM) to amplitude modulation (AM) conversion in the infrared (IR) output, frequency conversion, and final optics affected the accumulation of B-integral in that beamline. Modeling of this FM-to-AM conversion using the code Miro [Morice, O., "Miro: Complete modeling and software for pulse amplification and propagation in high-power laser systems," Opt. Eng. 42(6), 1530-1541 (2003).] was used as input to set the beamline performance limits for picket (short) pulses with multi-FM SSD applied. This article first describes that modeling. The 1-D SSD analytical model of Chuang [Chuang, Y.-H., "Amplification of broad-bandwidth phase-modulated laser counterpropagating light waves in homogeneous plasma," Ph.D. thesis, University of Rochester (September 1991).] is first extended to the case of multiple modulators and then used to benchmark Miro simulations. Comparison is also made to an alternative analytic model developed by Hocquet et al. [Hocquet, S., Penninckx, D., Bordenave, E., Gouedard, C. and Jaouen, Y., "FM-to-AM conversion in high-power lasers," Appl. Opt. 47(18), 3338-3349 (2008).] With the confidence engendered by this benchmarking, Miro results for multi-FM SSD applied on OMEGA EP are then presented. The relevant output section(s) of the OMEGA EP Laser System are described. The additional B-integral in OMEGA EP IR components upstream of the frequency converters due to AM is modeled. The importance of locating the image of the SSD dispersion grating at the frequency converters is demonstrated. Finally, since frequency conversion is not performed in OMEGA EP's target chamber, the additional AM due to propagation to the target chamber's vacuum window is modeled. C1 [Kelly, J. H.; Shvydky, A.; Marozas, J. A.; Guardalben, M. J.; Kruschwitz, B. E.; Waxer, L. J.; Dorrer, C.; Hill, E.; Okishev, A. V.] Univ Rochester, Laser Energet Lab, 250 E River Rd, Rochester, NY 14623 USA. [Di Nicola, J. -M.] Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. RP Kelly, JH (reprint author), Univ Rochester, Laser Energet Lab, 250 E River Rd, Rochester, NY 14623 USA. FU U.S. Department of Energy Office of Inertial Confinement Fusion [DE-FC52-08NA28302]; University of Rochester; New York State Energy Research and Development Authority; DOE FX This work was supported by the U.S. Department of Energy Office of Inertial Confinement Fusion under Cooperative Agreement No. DE-FC52-08NA28302, the University of Rochester, and the New York State Energy Research and Development Authority. The support of DOE does not constitute an endorsement by DOE of the views expressed in this article. NR 29 TC 0 Z9 0 U1 0 U2 7 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9371-2 J9 PROC SPIE PY 2013 VL 8602 AR UNSP 86020D DI 10.1117/12.2003209 PG 17 WC Optics; Physics, Fluids & Plasmas SC Optics; Physics GA BEX24 UT WOS:000318517700008 ER PT S AU Chen, CH AF Chen, Chin-Hao BE Li, BA Natowitz, JB TI Measurement of the Higher Order Azimuthal Anisotropy for Charged Hadrons at RHIC-PHENIX SO 11TH INTERNATIONAL CONFERENCE ON NUCLEUS-NUCLEUS COLLISIONS (NN2012) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 11th International Conference on Nucleus-Nucleus Collisions (NN) CY MAY 27-JUN 01, 2012 CL Texas A&M Univ, Cyclotron Inst, San Antonio, TX SP Texas A&M Univ-Commerce, Dept Phys and Astron HO Texas A&M Univ, Cyclotron Inst AB Measuring the azimuthal anisotropy of particles produced in relativistic heavy ion collisions has been considered as a powerful probe for investigating the characteristics of the quark-gluon plasma (QGP), which is the phase in QCD matter of de-confined quarks and gluons. The event anisotropy (v(2), v(3), v(4)) are measured in Au+Au collisions in various energies in PHENIX. The results of these higher-order event anisotropy constrain the initial geometrical eccentricity and viscosity that are used in hydrodynamical models. We present the latest results of v(2), v(3), v(4) measurement and discuss the simultaneous description with the hydrodynamical calculations C1 Brookhaven Natl Lab, RIKEN BNL Res Ctr, Upton, NY 11973 USA. RP Chen, CH (reprint author), Brookhaven Natl Lab, RIKEN BNL Res Ctr, Upton, NY 11973 USA. EM chchen@bnl.gov RI Natowitz, Joseph/D-4160-2015 NR 12 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 420 AR 012037 DI 10.1088/1742-6596/420/1/012037 PG 6 WC Physics, Nuclear SC Physics GA BEW69 UT WOS:000318430800037 ER PT S AU Das, JJ Carter, HK Beene, JR Sherrill, BM AF Das, J. J. Carter, H. K. Beene, J. R. Sherrill, B. M. BE Li, BA Natowitz, JB TI Helium jet ion source in FRIB era SO 11TH INTERNATIONAL CONFERENCE ON NUCLEUS-NUCLEUS COLLISIONS (NN2012) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 11th International Conference on Nucleus-Nucleus Collisions (NN) CY MAY 27-JUN 01, 2012 CL Texas A&M Univ, Cyclotron Inst, San Antonio, TX SP Texas A&M Univ-Commerce, Dept Phys and Astron HO Texas A&M Univ, Cyclotron Inst ID ONLINE ISOTOPE-SEPARATION; FACILITY AB Gas stopping of reaction products has a key feature, fixed holdup time independent of element, making it possible to provide ion beams of essentially all element. Two classes of gas stopping have been developed over the last 40+ years, broadly classified as He Jet and Ion guide. A primary difference between these two techniques is the physical separation of the stopping cell and the ionization cell in the He Jet technique. In this paper we point out two applications of current interest where this physical separation is crucial: 1) ionization (ion beam intensity) is independent of primary beam intensity and 2) multiuser capability for accelerator facilities. Specific examples will be described. C1 [Das, J. J.; Carter, H. K.] ORISE, UNIRIB, Oak Ridge, TN 37830 USA. RP Das, JJ (reprint author), ORISE, UNIRIB, Oak Ridge, TN 37830 USA. EM dasjj@ornl.gov RI Natowitz, Joseph/D-4160-2015 FU Office of Nuclear Physics, US Department of Energy [DE-AC05-06OR23100, DE-AC05-00OR22725]; National Nuclear Security Administration under the Stewardship Science Academic Alliances program through U.S. DOE Cooperative Agreement [DE-FG52-08NA28552] FX This research is sponsored by the Office of Nuclear Physics, US Department of Energy under contracts DE-AC05-06OR23100, DE-AC05-00OR22725 and the National Nuclear Security Administration under the Stewardship Science Academic Alliances program through U.S. DOE Cooperative Agreement No. DE-FG52-08NA28552 with Rutgers University. We also sincerely acknowledge scientific and technical help received D.W. Stracener, C. Reed, B. Griffith, Mark E. Whitley, D. Bunch, Frank Smith, Trevor Register, A.J. Mendez, G. D. Alton, Nate Foster, John Wills, B. A. Tatum, E. H. Spejewski and R.L. Varner. NR 12 TC 1 Z9 1 U1 0 U2 1 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 420 AR 012165 DI 10.1088/1742-6596/420/1/012165 PG 10 WC Physics, Nuclear SC Physics GA BEW69 UT WOS:000318430800165 ER PT S AU Gandolfi, S AF Gandolfi, Stefano BE Li, BA Natowitz, JB TI The equation of state of neutron star matter and the symmetry energy SO 11TH INTERNATIONAL CONFERENCE ON NUCLEUS-NUCLEUS COLLISIONS (NN2012) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 11th International Conference on Nucleus-Nucleus Collisions (NN) CY MAY 27-JUN 01, 2012 CL Texas A&M Univ, Cyclotron Inst, San Antonio, TX SP Texas A&M Univ-Commerce, Dept Phys and Astron HO Texas A&M Univ, Cyclotron Inst ID MONTE-CARLO CALCULATIONS; NUCLEI AB We present an overview of microscopic calculations of the Equation of State (EOS) of neutron matter performed using Quantum Monte Carlo techniques. We focus on the role of the model of the three-neutron force in the high-density part of the EOS up to a few times the saturation density. We also discuss the interplay between the symmetry energy and the neutron star mass-radius relation. The combination of theoretical models of the EOS with recent neutron star observations permits us to constrain the value of the symmetry energy and its slope. We show that astrophysical observations are starting to provide important insights into the properties of neutron star matter. C1 Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. RP Gandolfi, S (reprint author), Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. EM stefano@lanl.gov RI Natowitz, Joseph/D-4160-2015; OI Gandolfi, Stefano/0000-0002-0430-9035 NR 28 TC 1 Z9 1 U1 0 U2 1 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 420 AR 012150 DI 10.1088/1742-6596/420/1/012150 PG 7 WC Physics, Nuclear SC Physics GA BEW69 UT WOS:000318430800150 ER PT S AU Jiang, CL Albers, M Almaraz-Calderon, S Alcorta, M Back, BB Bertone, P Bucher, B Collon, P Courtin, S Deibel, CM DiGiovine, B Esbensen, H Fang, X Greene, J Haas, F Henderson, DJ Janssens, RVF Lauritsen, T Lefebvre-Schuhl, A Lister, CJ Marley, ST Pardo, R Paul, M Rehm, KE Seweryniak, D Tang, XD Ugalde, C Zhu, S AF Jiang, C. L. Albers, M. Almaraz-Calderon, S. Alcorta, M. Back, B. B. Bertone, P. Bucher, B. Collon, P. Courtin, S. Deibel, C. M. DiGiovine, B. Esbensen, H. Fang, X. Greene, J. Haas, F. Henderson, D. J. Janssens, R. V. F. Lauritsen, T. Lefebvre-Schuhl, A. Lister, C. J. Marley, S. T. Pardo, R. Paul, M. Rehm, K. E. Seweryniak, D. Tang, X. D. Ugalde, C. Zhu, S. BE Li, BA Natowitz, JB TI Study of the fusion reaction C-12+C-12 at low beam energy SO 11TH INTERNATIONAL CONFERENCE ON NUCLEUS-NUCLEUS COLLISIONS (NN2012) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 11th International Conference on Nucleus-Nucleus Collisions (NN) CY MAY 27-JUN 01, 2012 CL Texas A&M Univ, Cyclotron Inst, San Antonio, TX SP Texas A&M Univ-Commerce, Dept Phys and Astron HO Texas A&M Univ, Cyclotron Inst ID OR-EQUAL-TO; CROSS-SECTIONS; SUBCOULOMB ENERGIES; ELASTIC-SCATTERING; COULOMB BARRIER; C-12&C-12; C-12; C-13&C-13; NUCLEI AB In this article we discuss two aspects related to the C-12 + C-12 fusion reaction at low energies for carbon burning in supermassive stars. First we present plausible arguments for the notion that the observed resonance structures at the lowest measured energies arise from the relatively large spacing and narrow width of Mg-24 compound levels at the corresponding excitation energy region. We thus point out that the Incoming Wave Boundary Condition is inappropriate for calculating the fusion cross section under these situations. Secondly, we report on a particle-gamma coincidence technique that has been used for the first time to measure the fusion cross section in the system C-12 + C-12 at low beam energies. Based on these results, it should be possible to measure this important fusion cross section down to the 10 pb level within a reasonable length of time. C1 [Jiang, C. L.; Albers, M.; Almaraz-Calderon, S.; Alcorta, M.; Back, B. B.; Bertone, P.; Deibel, C. M.; DiGiovine, B.; Esbensen, H.; Greene, J.; Henderson, D. J.; Janssens, R. V. F.; Lauritsen, T.; Lister, C. J.; Marley, S. T.; Pardo, R.; Rehm, K. E.; Seweryniak, D.; Ugalde, C.; Zhu, S.] Argonne Natl Lab, Div Phys, Argonne, IL 60439 USA. RP Jiang, CL (reprint author), Argonne Natl Lab, Div Phys, Argonne, IL 60439 USA. EM jiang@phy.anl.gov RI Alcorta, Martin/G-7107-2011; Natowitz, Joseph/D-4160-2015; Tang, Xiaodong /F-4891-2016 OI Alcorta, Martin/0000-0002-6217-5004; NR 38 TC 4 Z9 4 U1 0 U2 7 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 420 AR 012120 DI 10.1088/1742-6596/420/1/012120 PG 14 WC Physics, Nuclear SC Physics GA BEW69 UT WOS:000318430800120 ER PT S AU Lee, IY AF Lee, I-Yang BE Li, BA Natowitz, JB TI Gamma-ray energy tracking array: GRETINA SO 11TH INTERNATIONAL CONFERENCE ON NUCLEUS-NUCLEUS COLLISIONS (NN2012) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 11th International Conference on Nucleus-Nucleus Collisions (NN) CY MAY 27-JUN 01, 2012 CL Texas A&M Univ, Cyclotron Inst, San Antonio, TX SP Texas A&M Univ-Commerce, Dept Phys and Astron HO Texas A&M Univ, Cyclotron Inst ID RADIOACTIVE BEAMS; DETECTORS AB A Gamma-ray energy tracking array can provide higher efficiency, better peak-to-total ratio and higher position resolution than the current generation of detector arrays. Particularly, the capability of reconstructing the position of the interaction with millimetre resolution is needed to fully exploit the physics opportunities provided by current and next generation radioactive beam facilities. This paper presents the basic concepts of energy tracking, examples of physics opportunities, and the status of the GRETINA/GRETA project. C1 Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Nucl Sci, Berkeley, CA 94720 USA. RP Lee, IY (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Nucl Sci, 1 Cyclotron Rd, Berkeley, CA 94720 USA. EM IYLee@lbl.gov RI Natowitz, Joseph/D-4160-2015 NR 14 TC 0 Z9 0 U1 0 U2 1 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 420 AR 012156 DI 10.1088/1742-6596/420/1/012156 PG 5 WC Physics, Nuclear SC Physics GA BEW69 UT WOS:000318430800156 ER PT S AU Liang, JF AF Liang, J. F. BE Li, BA Natowitz, JB TI Unexpected results in neutron-rich radioactive beams induced fusion SO 11TH INTERNATIONAL CONFERENCE ON NUCLEUS-NUCLEUS COLLISIONS (NN2012) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 11th International Conference on Nucleus-Nucleus Collisions (NN) CY MAY 27-JUN 01, 2012 CL Texas A&M Univ, Cyclotron Inst, San Antonio, TX SP Texas A&M Univ-Commerce, Dept Phys and Astron HO Texas A&M Univ, Cyclotron Inst ID EVEN-EVEN NUCLIDES; COULOMB BARRIER; ION-BEAMS; ENERGIES; FISSION AB The fission-fragment beams at HRIBF provide a unique opportunity for studying the mechanisms of fusion involving nuclei with large neutron excess. To explore the role of transfer couplings, fusion excitation functions have been measured using neutron-rich radioactive Sn-132 beams incident on Ca-40 and Ni-58 targets. The sub-barrier fusion enhancement for Sn-132+Ca-40 is larger than that for Sn-132+Ni-58 although the neutron transfer Q-values are similar for the two reactions. The fusion excitation function for Ti-46+Sn-124 has been measured in an attempt to resolve the differences observed in Sn-132+Ca-40 and Sn-132+Ni-58. C1 Oak Ridge Natl Lab, Div Phys, Oak Ridge, TN 37831 USA. RP Liang, JF (reprint author), Oak Ridge Natl Lab, Div Phys, Oak Ridge, TN 37831 USA. RI Natowitz, Joseph/D-4160-2015 NR 19 TC 2 Z9 2 U1 0 U2 0 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 420 AR 012125 DI 10.1088/1742-6596/420/1/012125 PG 8 WC Physics, Nuclear SC Physics GA BEW69 UT WOS:000318430800125 ER PT S AU Morrison, D AF Morrison, David CA PHENIX Collaboration BE Li, BA Natowitz, JB TI Jet Measurements in Heavy Ion Collisions with an Upgraded PHENIX Detector SO 11TH INTERNATIONAL CONFERENCE ON NUCLEUS-NUCLEUS COLLISIONS (NN2012) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 11th International Conference on Nucleus-Nucleus Collisions (NN) CY MAY 27-JUN 01, 2012 CL Texas A&M Univ, Cyclotron Inst, San Antonio, TX SP Texas A&M Univ-Commerce, Dept Phys and Astron HO Texas A&M Univ, Cyclotron Inst ID QUARK-GLUON PLASMA; COLLABORATION; PERSPECTIVE AB The PHENIX Collaboration is pursuing an upgrade to the PHENIX detector to enable investigations of specific, outstanding questions that will advance our understanding of the strongly coupled quark-gluon plasma (sQGP). The greatly upgraded detector, called sPHENIX, consists of a superconducting solenoid and electromagnetic and hadronic calorimeters with a fiducial acceptance of Delta phi = 2 pi and |eta| < 1 around an existing silicon tracking detector, the VTX. It will have excellent capabilities for measuring an important set of jet observables. These measurements, in conjunction with similar measurements at the LHC, will provide information about energy loss, transport coefficients, and the fundamental constituents of the sQGP in the domain of strongest coupling, near T-c. C1 [Morrison, David; PHENIX Collaboration] Brookhaven Natl Lab, Upton, NY 11973 USA. RP Morrison, D (reprint author), Brookhaven Natl Lab, Upton, NY 11973 USA. EM morrison@bnl.gov RI Natowitz, Joseph/D-4160-2015 NR 27 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 420 AR 012025 DI 10.1088/1742-6596/420/1/012025 PG 10 WC Physics, Nuclear SC Physics GA BEW69 UT WOS:000318430800025 ER PT S AU Nouicer, R AF Nouicer, Rachid CA PHENIX Collaboration BE Li, BA Natowitz, JB TI Heavy Flavor Physics in PHENIX SO 11TH INTERNATIONAL CONFERENCE ON NUCLEUS-NUCLEUS COLLISIONS (NN2012) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 11th International Conference on Nucleus-Nucleus Collisions (NN) CY MAY 27-JUN 01, 2012 CL Texas A&M Univ, Cyclotron Inst, San Antonio, TX SP Texas A&M Univ-Commerce, Dept Phys and Astron HO Texas A&M Univ, Cyclotron Inst ID NUCLEUS-NUCLEUS COLLISIONS; STRIPIXEL DETECTOR; MATTER; COLLABORATION AB Heavy quarks are good probes of the hot and dense medium created in relativistic heavy ion collisions since they are mainly generated early in the collision and interact with the medium in all collision stages. In addition, heavy flavor quarkonia production is thought to be uniquely sensitive to the deconfined medium of the Quark Gluon Plasma (QGP) through color screening. Heavy quark production has been studied by the PHENIX experiment at RHIC via measurements of single leptons from semi-leptonic decays, in both the electron channel at mid-rapidity and in the muon channel at forward rapidity. Large suppression and azimuthal anisotropy of single electrons have been observed in Au+Au collisions at root s(NN) = 200 GeV. These results suggest a large energy loss and strong flow of the heavy quarks in the hot, dense matter. The PHENIX experiment has also measured J/psi, production in p+p, d+Au, Cu+Cu, and Au+Au collisions at energies up to root s(NN) = 200 GeV. In central Au+Au at 200 GeV, more suppression is observed at forward rapidity than at central rapidity. This can be interpreted either as a sign of quark recombination, or as a hint of additional cold nuclear matter effects. Selected PHENIX results on open heavy flavor and heavy quarkonia production in p+p, d+Au, Cu+Cu, and Au+Au collisions are presented. The status of the recent PHENIX upgrade of the central Silicon Vertex Tracker (VTX) and its performance are elucidated. C1 [Nouicer, Rachid; PHENIX Collaboration] Brookhaven Natl Lab, Dept Phys, Upton, NY 11973 USA. RP Nouicer, R (reprint author), Brookhaven Natl Lab, Dept Phys, Upton, NY 11973 USA. EM rachid.nouicer@bnl.gov RI Natowitz, Joseph/D-4160-2015 NR 35 TC 2 Z9 2 U1 0 U2 0 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 420 AR 012021 DI 10.1088/1742-6596/420/1/012021 PG 8 WC Physics, Nuclear SC Physics GA BEW69 UT WOS:000318430800021 ER PT S AU Rubert, J Dorvaux, O Gall, BJP Greenlees, PT Asfari, Z Piot, J Andersson, LL Asai, M Cox, DM Dechery, F Grahn, T Hauschild, K Henning, G Herzan, A Herzberg, RD Hessberger, FP Jakobsson, U Jones, P Julin, R Juutinen, S Ketelhut, S Khoo, TL Leino, M Ljungvall, J Lopez-Martens, A Lozeva, R Nieminen, P Pakarinen, J Papadakis, P Parr, E Peura, P Rahkila, P Rinta-Antila, S Ruotsalainen, P Sandzelius, M Saren, J Scholey, C Seweryniak, D Sorri, J Sulignano, B Theisen, C Uusitalo, J Venhart, M AF Rubert, J. Dorvaux, O. Gall, B. J. P. Greenlees, P. T. Asfari, Z. Piot, J. Andersson, L. L. Asai, M. Cox, D. M. Dechery, F. Grahn, T. Hauschild, K. Henning, G. Herzan, A. Herzberg, R-D Hessberger, F. P. Jakobsson, U. Jones, P. Julin, R. Juutinen, S. Ketelhut, S. Khoo, T-L Leino, M. Ljungvall, J. Lopez-Martens, A. Lozeva, R. Nieminen, P. Pakarinen, J. Papadakis, P. Parr, E. Peura, P. Rahkila, P. Rinta-Antila, S. Ruotsalainen, P. Sandzelius, M. Saren, J. Scholey, C. Seweryniak, D. Sorri, J. Sulignano, B. Theisen, Ch Uusitalo, J. Venhart, M. BE Li, BA Natowitz, JB TI First prompt in-beam gamma-ray spectroscopy of a superheavy element: the (256)Rf SO 11TH INTERNATIONAL CONFERENCE ON NUCLEUS-NUCLEUS COLLISIONS (NN2012) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 11th International Conference on Nucleus-Nucleus Collisions (NN) CY MAY 27-JUN 01, 2012 CL Texas A&M Univ, Cyclotron Inst, San Antonio, TX SP Texas A&M Univ-Commerce, Dept Phys and Astron HO Texas A&M Univ, Cyclotron Inst ID ECR ION-SOURCE; TOTAL DATA READOUT; ISOTOPES; NUCLEI AB Using state-of-the-art gamma-ray spectroscopic techniques, the first rotational band of a superheavy element, extending up to a spin of 20 (h) over bar, was discovered in the nucleus (256)Rf. To perform such an experiment at the limits of the present instrumentation, several developments were needed. The most important of these developments was of an intense isotopically enriched Ti-50 beam using the MIVOC method. The experimental set-up and subsequent analysis allowed the (256)Rf ground-state band to be revealed. The rotational properties of the band are discussed and compared with neighboring transfermium nuclei through the study of their moments of inertia. These data suggest that there is no evidence of a significant deformed shell gap at Z = 104. C1 [Rubert, J.; Dorvaux, O.; Gall, B. J. P.; Asfari, Z.; Lozeva, R.] Univ Strasbourg, Inst Pluridisciplinaire Hubert Curien, 23 Rue Loess, F-67037 Strasbourg, France. [Greenlees, P. T.; Grahn, T.; Herzan, A.; Julin, R.; Juutinen, S.; Ketelhut, S.; Peura, P.; Rahkila, P.; Rinta-Antila, S.; Ruotsalainen, P.; Sandzelius, M.; Saren, J.; Scholey, C.; Uusitalo, J.] Univ Jyvaskyla, Dept Phys, FIN-40014 Jyvaskyla, Finland. [Andersson, L. L.; Cox, D. M.; Herzberg, R-D; Papadakis, P.; Parr, E.] Univ Liverpool, Dept Phys, Liverpool L69 7ZE, Merseyside, England. [Asai, M.] Japan Atom Energy Agcy, Adv Sci Res Ctr, Tokai, Ibaraki 3191195, Japan. [Dechery, F.; Sulignano, B.; Theisen, Ch] CEA, Saclay Ctr, IRFU, Serv Phys Nucl, F-91191 Gif Sur Yvette, France. [Hauschild, K.; Henning, G.; Lopez-Martens, A.] CNRS, IN2P3, CSNSM, F-91405 Orsay, France. [Henning, G.; Khoo, T-L; Seweryniak, D.] Argonne Natl Lab, Argonne, IL 60439 USA. [Hessberger, F. P.] GSI Helmholtzzentrum Schwerionenforsch GmbH, D-64291 Darmstadt, Germany. [Pakarinen, J.] CERN, ISOLDE, CH-1211 Geneva, Switzerland. [Venhart, M.] Slovak Acad Sci, Inst Phys, Bratislava SK-84511, Slovakia. [Piot, J.] GANIL, CEA, DSM CNRS, IN2P3, Caen, France. RP Rubert, J (reprint author), Univ Strasbourg, Inst Pluridisciplinaire Hubert Curien, 23 Rue Loess, F-67037 Strasbourg, France. EM jerome.rubert@iphc.cnrs.fr RI Herzberg, Rolf-Dietmar/E-1558-2011; Scholey, Catherine/G-2720-2014; Hauschild, Karl/A-6726-2009; THEISEN, Christophe/A-9343-2015; Natowitz, Joseph/D-4160-2015 OI Scholey, Catherine/0000-0002-8743-6071; THEISEN, Christophe/0000-0002-8509-1022; FU EU [262010]; Academy of Finland [131665]; European Research Council [203481]; EURONS (European Commission) [506065]; UK STFC; Slovak Grant Agency VEGA [2/0105/11]; U.S. Department of Energy, Office of Nuclear Physics [DEAC02-06CH11357] FX This work has been supported by the EU-FP7-IA project ENSAR (No. 262010), the Academy of Finland (CoE in Nuclear ad Accelerator Based Physics, Grant to T.G contract No. 131665), the European Research Council through the project SHESTRUCT (Grant Agreement No. 203481), EURONS (European Commission Contract No. 506065), the UK STFC, the Slovak Grant Agency VEGA (Contract No. 2/0105/11) and the U.S. Department of Energy, Office of Nuclear Physics, under Contract No. DEAC02-06CH11357. The GAMMAPOOL European Spectroscopy Resource is thanked for the loan of detectors for JUROGAM II. NR 24 TC 0 Z9 0 U1 0 U2 8 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 420 AR 012010 DI 10.1088/1742-6596/420/1/012010 PG 10 WC Physics, Nuclear SC Physics GA BEW69 UT WOS:000318430800010 ER PT S AU Videbaek, F AF Videbaek, Flemming CA STAR Collaboration BE Li, BA Natowitz, JB TI Heavy Flavor Physics in STAR SO 11TH INTERNATIONAL CONFERENCE ON NUCLEUS-NUCLEUS COLLISIONS (NN2012) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 11th International Conference on Nucleus-Nucleus Collisions (NN) CY MAY 27-JUN 01, 2012 CL Texas A&M Univ, Cyclotron Inst, San Antonio, TX SP Texas A&M Univ-Commerce, Dept Phys and Astron HO Texas A&M Univ, Cyclotron Inst ID CHARM AB In relativistic heavy ion collisions at RHIC, heavy quarks are primarily created from initial hard scatterings. Since their large masses are not easily affected by the strong interaction with QCD medium they may carry information from the system at early stage. The interaction between heavy quarks and the medium is sensitive to the medium dynamics; therefore heavy quarks are suggested as an ideal probe to quantify the properties of the strongly interacting QCD matter. The STAR Collaboration should complete the Heavy Flavor Tracker (HFT) and the Muon Telescope Detector (MTD) upgrades by 2014. These detectors will greatly enhance the STAR physics capability to measure heavy quark collectivity and correlations using topologically reconstructed charmed hadrons and heavy quark decay electron-muon correlations. In addition, measurements of the quarkonium muon decay channels will enable us to separate Upsilon 1S from 2S and 3S states in p + p and A+A collisions. Selected STAR results on open charm and quarkonia production in p + p and Au+Au collisions at 200 GeV are presented. An overview of the upgrades, their expected performance and current status is presented. C1 [Videbaek, Flemming; STAR Collaboration] Brookhaven Natl Lab, Upton, NY 11973 USA. RP Videbaek, F (reprint author), Brookhaven Natl Lab, Upton, NY 11973 USA. EM videbaek@bnl.gov RI Natowitz, Joseph/D-4160-2015 NR 16 TC 0 Z9 0 U1 0 U2 1 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 420 AR 012024 DI 10.1088/1742-6596/420/1/012024 PG 9 WC Physics, Nuclear SC Physics GA BEW69 UT WOS:000318430800024 ER PT S AU Wong, CY AF Wong, Cheuk-Yin BE Li, BA Natowitz, JB TI Feynman Amplitude Approach to study the Passage of a Jet in a Medium SO 11TH INTERNATIONAL CONFERENCE ON NUCLEUS-NUCLEUS COLLISIONS (NN2012) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 11th International Conference on Nucleus-Nucleus Collisions (NN) CY MAY 27-JUN 01, 2012 CL Texas A&M Univ, Cyclotron Inst, San Antonio, TX SP Texas A&M Univ-Commerce, Dept Phys and Astron HO Texas A&M Univ, Cyclotron Inst ID HIGH-ENERGY SCATTERING; COLLISIONS; QCD; DIAGRAMS; STAR AB In the Feynman amplitude approach for coherent collisions of a jet with medium partons, the Bose-Einstein symmetry with respect to the interchange of the exchanged bosons leads to a destructive interference of the amplitudes in most regions of the phase space but a constructive interference in some other regions. As a consequence, there is a collective longitudinal momentum transfer to the scatterers along the jet direction, each scatterer carrying a substantial fraction of the incident jet longitudinal momentum. The manifestation of the Bose-Einstein interference may have been observed in angular correlations of hadrons associated with a high-p(T) trigger in high-energy collisions at RHIC and LHC. C1 Oak Ridge Natl Lab, Div Phys, Oak Ridge, TN 37831 USA. RP Wong, CY (reprint author), Oak Ridge Natl Lab, Div Phys, Oak Ridge, TN 37831 USA. EM wongc@ornl.gov RI Natowitz, Joseph/D-4160-2015; OI Wong, Cheuk-Yin/0000-0001-8223-0659 NR 57 TC 0 Z9 0 U1 0 U2 8 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 420 AR UNSP 012028 DI 10.1088/1742-6596/420/1/012028 PG 10 WC Physics, Nuclear SC Physics GA BEW69 UT WOS:000318430800028 ER PT B AU Bierbaum, RL Robertson, AA AF Bierbaum, Rene L. Robertson, Alix A. GP IEEE TI Defect Types and Surveillance Strategies for One-Shot Items SO 59TH ANNUAL RELIABILITY AND MAINTAINABILITY SYMPOSIUM (RAMS) LA English DT Proceedings Paper CT 59th Annual Reliability and Maintainability Symposium (RAMS) CY JAN 28-31, 2013 CL Orlando, FL SP IIE, IEST, AIAA, IEEE Reliabil Soc, SAE Int, Soc Reliabil Engineers (SRE), SSS, ASQ, Elect & Commun Div, ASQ, Reliabil Div DE one-shot items; surveillance; defect taxonomy AB This paper will describe some of the challenges and strategies for sampling and testing of complex one-shot systems. A taxonomy for defect types will be offered that informs the nature of the testing and analysis that should be done. In addition, some options for balancing and articulating risk will be summarized for the various surveillance programs described. C1 [Bierbaum, Rene L.; Robertson, Alix A.] Sandia Natl Labs, Livermore, CA 94551 USA. RP Bierbaum, RL (reprint author), Sandia Natl Labs, POB 969,MS9007, Livermore, CA 94551 USA. EM rlbierb@sandia.gov; aarober@sandia.gov NR 8 TC 0 Z9 0 U1 0 U2 0 PU IEEE PI NEW YORK PA 345 E 47TH ST, NEW YORK, NY 10017 USA BN 978-1-4673-4711-2 PY 2013 PG 6 WC Engineering, Industrial; Engineering, Electrical & Electronic; Operations Research & Management Science SC Engineering; Operations Research & Management Science GA BFW62 UT WOS:000321693500016 ER PT S AU Westbrook, CK AF Westbrook, Charles K. BE Johnson, MA Martinez, TJ TI Biofuels Combustion SO ANNUAL REVIEW OF PHYSICAL CHEMISTRY, VOL 64 SE Annual Review of Physical Chemistry LA English DT Review; Book Chapter DE ethanol; iso-pentanol; biodiesel; methyl esters; combustion ID LOW-TEMPERATURE COMBUSTION; IGNITION DELAY TIMES; KINETIC REACTION-MECHANISMS; INJECTION DIESEL-ENGINE; PRESSURE RATE RULES; AEROSOL SHOCK-TUBE; BIODIESEL FUELS; METHYL OLEATE; CHEMICAL-KINETICS; LIQUID BIOFUELS AB This review describes major features of current research in renewable fuels derived from plants and from fatty acids. Recent and ongoing fundamental studies of biofuel molecular structure, oxidation reactions, and biofuel chemical properties are reviewed, in addition to combustion applications of biofuels in the major types of engines in which biofuels are used. Biofuels and their combustion are compared with combustion features of conventional petroleum-based fuels. Two main classes of biofuels are described, those consisting of small, primarily alcohol, fuels ( particularly ethanol, n-butanol, and iso-pentanol) that are used primarily to replace or supplement gasoline and those derived from fatty acids and used primarily to replace or supplement conventional diesel fuels. Research efforts on so-called second- and third-generation biofuels are discussed briefly. C1 Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. RP Westbrook, CK (reprint author), Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. EM Westbrook1@llnl.gov NR 115 TC 43 Z9 44 U1 13 U2 133 PU ANNUAL REVIEWS PI PALO ALTO PA 4139 EL CAMINO WAY, PO BOX 10139, PALO ALTO, CA 94303-0897 USA SN 0066-426X BN 978-0-8243-1064-6 J9 ANNU REV PHYS CHEM JI Annu. Rev. Phys. Chem. PY 2013 VL 64 BP 201 EP 219 DI 10.1146/annurev-physchem-040412-110009 PG 19 WC Chemistry, Physical SC Chemistry GA BFX47 UT WOS:000321771600010 PM 23298249 ER PT S AU Geissler, PL AF Geissler, Phillip L. BE Johnson, MA Martinez, TJ TI Water Interfaces, Solvation, and Spectroscopy SO ANNUAL REVIEW OF PHYSICAL CHEMISTRY, VOL 64 SE Annual Review of Physical Chemistry LA English DT Review; Book Chapter DE liquid water; interfaces; ion solvation; isosbestic behavior; vibrational spectroscopy ID SUM-FREQUENCY GENERATION; ULTRAFAST INFRARED-SPECTROSCOPY; ECHO CORRELATION SPECTROSCOPY; HYDROGEN-BOND DYNAMICS; ATMOSPHERICALLY RELEVANT IONS; LIQUID-VAPOR INTERFACE; 3-PULSE PHOTON-ECHOES; GAUSSIAN FIELD MODEL; OH STRETCHING BAND; RAMAN LINE-SHAPES AB Liquid water consistently expands our appreciation of the rich statistical mechanics that can emerge from simple molecular constituents. Here I review several interrelated areas of recent work on aqueous systems that aim to explore and explain this richness by revealing molecular arrangements, their thermodynamic origins, and the timescales on which they change. Vibrational spectroscopy of OH stretching features prominently in these discussions, with an emphasis on efforts to establish connections between spectroscopic signals and statistics of intermolecular structure. For bulk solutions, the results of these efforts largely verify and enrich existing physical pictures of hydrogen-bond network connectivity, dynamics, and response. For water at interfaces, such pictures are still emerging. As an important example I discuss the solvation of small ions at the air-water interface, whose surface propensities challenge a basic understanding of how aqueous fluctuations accommodate solutes in heterogeneous environments. C1 [Geissler, Phillip L.] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Geissler, Phillip L.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. RP Geissler, PL (reprint author), Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. EM geissler@berkeley.edu NR 115 TC 43 Z9 43 U1 7 U2 88 PU ANNUAL REVIEWS PI PALO ALTO PA 4139 EL CAMINO WAY, PO BOX 10139, PALO ALTO, CA 94303-0897 USA SN 0066-426X BN 978-0-8243-1064-6 J9 ANNU REV PHYS CHEM JI Annu. Rev. Phys. Chem. PY 2013 VL 64 BP 317 EP 337 DI 10.1146/annurev-physchem-040412-110153 PG 21 WC Chemistry, Physical SC Chemistry GA BFX47 UT WOS:000321771600015 PM 23298244 ER PT S AU Tobias, DJ Stern, AC Baer, MD Levin, Y Mundy, CJ AF Tobias, Douglas J. Stern, Abraham C. Baer, Marcel D. Levin, Yan Mundy, Christopher J. BE Johnson, MA Martinez, TJ TI Simulation and Theory of Ions at Atmospherically Relevant Aqueous Liquid-Air Interfaces SO ANNUAL REVIEW OF PHYSICAL CHEMISTRY, VOL 64 SE Annual Review of Physical Chemistry LA English DT Review; Book Chapter DE atmospheric chemistry; interfacial chemistry; specific ion effects; molecular dynamics; dielectric continuum theory ID MOLECULAR-DYNAMICS SIMULATIONS; SUM-FREQUENCY GENERATION; DENSITY-FUNCTIONAL THEORY; POLARIZABLE FORCE-FIELD; VAPOR INTERFACE; SURFACE-TENSION; SALT-SOLUTIONS; AIR/WATER INTERFACE; VIBRATIONAL SPECTROSCOPY; WATER-SURFACE AB Chemistry occurring at or near the surface of aqueous droplets and thin films in the atmosphere influences air quality and climate. Molecular dynamics simulations are becoming increasingly useful for gaining atomic-scale insight into the structure and reactivity of aqueous interfaces in the atmosphere. Here we review simulation studies of atmospherically relevant aqueous liquid-air interfaces, with an emphasis on ions that play important roles in the chemistry of atmospheric aerosols. In addition to surveying results from simulation studies, we discuss challenges to the refinement and experimental validation of the methodology for simulating ion adsorption to the air-water interface and recent advances in elucidating the driving forces for adsorption. We also review the recent development of a dielectric continuum theory capable of reproducing simulation and experimental data on ion behavior at aqueous interfaces. C1 [Tobias, Douglas J.; Stern, Abraham C.] Univ Calif Irvine, Dept Chem, Irvine, CA 92697 USA. [Baer, Marcel D.; Mundy, Christopher J.] Pacific NW Natl Lab, Chem & Mat Sci Div, Richland, WA 99352 USA. [Levin, Yan] Univ Fed Rio Grande do Sul, Inst Fis, BR-91501970 Porto Alegre, RS, Brazil. RP Tobias, DJ (reprint author), Univ Calif Irvine, Dept Chem, Irvine, CA 92697 USA. EM dtobias@uci.edu; acstern@uci.edu; marcel.baer@pnnl.gov; levin@if.ufrgs.br; chris.mundy@pnnl.gov RI Baer, Marcel/K-7664-2012; Levin, Yan/H-5589-2012; Tobias, Douglas/B-6799-2015 NR 132 TC 53 Z9 53 U1 8 U2 126 PU ANNUAL REVIEWS PI PALO ALTO PA 4139 EL CAMINO WAY, PO BOX 10139, PALO ALTO, CA 94303-0897 USA SN 0066-426X BN 978-0-8243-1064-6 J9 ANNU REV PHYS CHEM JI Annu. Rev. Phys. Chem. PY 2013 VL 64 BP 339 EP 359 DI 10.1146/annurev-physchem-040412-110049 PG 21 WC Chemistry, Physical SC Chemistry GA BFX47 UT WOS:000321771600016 PM 23331311 ER PT S AU Gordon, MS Smith, QA Xu, P Slipchenko, LV AF Gordon, Mark S. Smith, Quentin A. Xu, Peng Slipchenko, Lyudmila V. BE Johnson, MA Martinez, TJ TI Accurate First Principles Model Potentials for Intermolecular Interactions SO ANNUAL REVIEW OF PHYSICAL CHEMISTRY, VOL 64 SE Annual Review of Physical Chemistry LA English DT Review; Book Chapter DE effective fragment potential; EFP; charge transfer; dispersion; exchange repulsion; QM/EFP ID MOLECULAR-ORBITAL METHODS; EFFECTIVE FRAGMENT METHOD; QUANTUM-MECHANICAL CALCULATIONS; ENERGY DECOMPOSITION ANALYSIS; ADAPTED PERTURBATION-THEORY; CLOSED-SHELL MOLECULES; WATER CLUSTERS; CHARGE-TRANSFER; AB-INITIO; AQUEOUS-SOLUTION AB The general effective fragment potential (EFP) method provides model potentials for any molecule that is derived from first principles, with no empirically fitted parameters. The EFP method has been interfaced with most currently used ab initio single-reference and multireference quantum mechanics (QM) methods, ranging from Hartree-Fock and coupled cluster theory to multireference perturbation theory. The most recent innovations in the EFP model have been to make the computationally expensive charge transfer term much more efficient and to interface the general EFP dispersion and exchange repulsion interactions with QM methods. Following a summary of the method and its implementation in generally available computer programs, these most recent new developments are discussed. C1 [Gordon, Mark S.; Smith, Quentin A.; Xu, Peng] Iowa State Univ, Dept Chem, Ames, IA 50011 USA. [Gordon, Mark S.; Smith, Quentin A.; Xu, Peng] Iowa State Univ, Ames Lab, Ames, IA 50011 USA. [Slipchenko, Lyudmila V.] Purdue Univ, Dept Chem, W Lafayette, IN 47907 USA. RP Gordon, MS (reprint author), Iowa State Univ, Dept Chem, Ames, IA 50011 USA. EM mark@si.msg.chem.iastate.edu; schrodinator@gmail.com; pxu@iastate.edu; lslipchenko@purdue.edu NR 138 TC 52 Z9 52 U1 3 U2 66 PU ANNUAL REVIEWS PI PALO ALTO PA 4139 EL CAMINO WAY, PO BOX 10139, PALO ALTO, CA 94303-0897 USA SN 0066-426X BN 978-0-8243-1064-6 J9 ANNU REV PHYS CHEM JI Annu. Rev. Phys. Chem. PY 2013 VL 64 BP 553 EP 578 DI 10.1146/annurev-physchem-040412-110031 PG 26 WC Chemistry, Physical SC Chemistry GA BFX47 UT WOS:000321771600025 PM 23561011 ER PT S AU Shu, JY Panganiban, B Xu, T AF Shu, Jessica Y. Panganiban, Brian Xu, Ting BE Johnson, MA Martinez, TJ TI Peptide-Polymer Conjugates: From Fundamental Science to Application SO ANNUAL REVIEW OF PHYSICAL CHEMISTRY, VOL 64 SE Annual Review of Physical Chemistry LA English DT Review; Book Chapter DE hybrid biomaterial; self-assembly; polymer conformation; protein-polymer interaction ID HYBRID BLOCK-COPOLYMERS; SOLID-STATE STRUCTURE; DIBLOCK COPOLYMERS; GIANT AMPHIPHILES; DRUG-DELIVERY; GENE DELIVERY; POLY(ETHYLENE GLYCOL); COFACTOR RECONSTITUTION; RADICAL POLYMERIZATION; SYNTHETIC STRATEGIES AB Peptide/protein-polymer conjugates make up a new class of soft matter comprising natural and synthetic building blocks. They have the potential to combine the advantages of proteins and synthetic polymers (i.e., the precise chemical structure and diverse functionalities of biomolecules and the stability and processability of synthetic polymers) to generate hybrid materials with properties yet to be realized with either component alone. Here we briefly discuss recent developments in the design, fundamental understanding, and self-assembly of various peptide-polymer conjugates, as well as emerging biological and nonbiological applications that range from nanomedicine, to separation, and beyond. C1 [Shu, Jessica Y.; Panganiban, Brian; Xu, Ting] Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA. [Xu, Ting] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Xu, Ting] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. RP Shu, JY (reprint author), Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA. EM tingxu@berkeley.edu NR 142 TC 67 Z9 68 U1 11 U2 158 PU ANNUAL REVIEWS PI PALO ALTO PA 4139 EL CAMINO WAY, PO BOX 10139, PALO ALTO, CA 94303-0897 USA SN 0066-426X BN 978-0-8243-1064-6 J9 ANNU REV PHYS CHEM JI Annu. Rev. Phys. Chem. PY 2013 VL 64 BP 631 EP 657 DI 10.1146/annurev-physchem-040412-110108 PG 27 WC Chemistry, Physical SC Chemistry GA BFX47 UT WOS:000321771600028 PM 23331303 ER PT J AU Yan, XQ Wang, XJ Tang, Y Ma, GC Zou, SH Li, RH Peng, XG Dai, S Fan, J AF Yan, Xiaoqing Wang, Xiaojuan Tang, Yu Ma, Guicen Zou, Shihui Li, Renhong Peng, Xiaogang Dai, Sheng Fan, Jie TI Ordered, extra-large mesopores with highly loaded gold nanoparticles: a new sintering- and coking-resistant catalyst system SO CHEMICAL COMMUNICATIONS LA English DT Article ID OXIDATION; PHASE; DEACTIVATION; ALCOHOLS; N2O AB Ordered, extra-large mesopores with highly loaded gold nanoparticles (AuNPs) exhibits unique sintering- and coking-resistant properties in gas-phase, cyclohexanol selective aerobic oxidation. C1 [Yan, Xiaoqing; Wang, Xiaojuan; Tang, Yu; Ma, Guicen; Zou, Shihui; Li, Renhong; Peng, Xiaogang; Fan, Jie] Zhejiang Univ, Key Lab Appl Chem Zhejiang Prov, Dept Chem, Hangzhou 310003, Zhejiang, Peoples R China. [Dai, Sheng] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. RP Fan, J (reprint author), Zhejiang Univ, Key Lab Appl Chem Zhejiang Prov, Dept Chem, Hangzhou 310003, Zhejiang, Peoples R China. EM jfan@zju.edu.cn RI Fan, Jie/B-3740-2008; Li, Renhong/G-7778-2016; Zou, Shihui/H-9607-2012; Dai, Sheng/K-8411-2015 OI Fan, Jie/0000-0002-8380-6338; Li, Renhong/0000-0002-8327-5506; Zou, Shihui/0000-0001-5564-4151; Dai, Sheng/0000-0002-8046-3931 NR 23 TC 4 Z9 4 U1 8 U2 98 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 66 BP 7274 EP 7276 DI 10.1039/c3cc39196e PG 3 WC Chemistry, Multidisciplinary SC Chemistry GA 187UE UT WOS:000322145300001 PM 23615685 ER PT J AU Fulvio, PF Hillesheim, PC Oyola, Y Mahurin, SM Veith, GM Dai, S AF Fulvio, Pasquale F. Hillesheim, Patrick C. Oyola, Yatsandra Mahurin, Shannon M. Veith, Gabriel M. Dai, Sheng TI A new family of fluidic precursors for the self-templated synthesis of hierarchical nanoporous carbons SO CHEMICAL COMMUNICATIONS LA English DT Article ID DOUBLE-LAYER CAPACITORS; IONIC LIQUIDS; MESOPOROUS CARBONS; BLOCK-COPOLYMERS; POROUS CARBON; NITROGEN; FLUORINATION; PERFORMANCE; STORAGE AB Hierarchical nanoporous nitrogen-doped carbons were prepared from task specific ionic liquids having a bis-imidazolium motif linked with various organic groups. While ethyl chains linking the imidazolium ions afforded microporous-mesoporous carbons, long or aromatic groups resulted in microporous samples. C1 [Fulvio, Pasquale F.; Hillesheim, Patrick C.; Oyola, Yatsandra; Mahurin, Shannon M.; Dai, Sheng] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. [Veith, Gabriel M.] Oak Ridge Natl Lab, Mat Sci & Technol Div, 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 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, an Energy Frontier Research Center; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences (Carbons, BET, CV, TEM); Division of Chemical Sciences, Geosciences, and Biosciences (ILs, NMR, MS, TEM); GMV Division of Materials Sciences and Engineering (XPS, BET); U.S. Department of Energy's Office of Basic Energy Science FX PFF and SD were supported as part of the Fluid Interface Reactions, Structures, and Transport (FIRST) Center, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences (Carbons, BET, CV, TEM). PCH, YO, and SMM were sponsored by Division of Chemical Sciences, Geosciences, and Biosciences (ILs, NMR, MS, TEM) and GMV Division of Materials Sciences and Engineering (XPS, BET), U.S. Department of Energy's Office of Basic Energy Science. NR 31 TC 15 Z9 15 U1 3 U2 72 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1359-7345 EI 1364-548X J9 CHEM COMMUN JI Chem. Commun. PY 2013 VL 49 IS 66 BP 7289 EP 7291 DI 10.1039/c3cc44175j PG 3 WC Chemistry, Multidisciplinary SC Chemistry GA 187UE UT WOS:000322145300006 PM 23846510 ER PT J AU Hubaud, AA Schroeder, DJ Key, B Ingram, BJ Dogan, F Vaughey, JT AF Hubaud, Aude A. Schroeder, David J. Key, Baris Ingram, Brian J. Dogan, Fulya Vaughey, John T. TI Low temperature stabilization of cubic (Li7-xAlx/3) La3Zr2O12: role of aluminum during formation SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID GARNET-TYPE LI7LA3ZR2O12; SOLID-ELECTROLYTE; TETRAGONAL LI7LA3ZR2O12; AL; STATE; CONDUCTIVITY; BATTERIES; CERAMICS AB The lithium lanthanum zirconium oxide garnet, Li7La3Zr2O12 (LLZ), has received significant attention in recent years due to its high room temperature lithium ion conductivity and its stability against lithium metal. Together these features make it a promising electrolyte candidate for a high energy all solid-state battery. Previous studies have shown that incorporation of aluminum cations during the synthesis stabilizes the higher conductivity cubic phase of LLZ; however the incorporation process and its effect on the phase transition are still unclear. In the present study, we have combined powder X-ray diffraction (XRD), Al-27 and Li-7 MAS NMR and high-resolution X-ray diffraction (HRXRD) to determine the disposition of Al cations during the formation of low temperature cubic LLZ. At temperatures as low as 700 degrees C, the aluminum is incorporated into amorphous or nanocrystalline grain boundary phases. Above 700 degrees C, the Al cations are associated with a poorly crystalline anti-fluorite phase Li5AlO4, composed of molecular [AlO4](5-) anions. This phase then reacts with tetragonal LLZ to form cubic LLZ over a 25 hour period at 850 degrees C. Although the reaction appears complete by powder X-ray diffraction, Al-27 NMR spectra showed overlapping resonances suggesting multiple Al environments due to uneven substitution of the 24d Li(1) site. This was confirmed by high-resolution XRD and was consistent with a series of closely related cubic LLZ phases with slightly different Al concentrations, indicating the slower Al(III) diffusion within the lattice has not reached equilibrium in the time allotted. The disorder over the two crystallographic tetrahedral sites by lithium and aluminum cations at this temperature contributes to the observed lattice enlargement associated with the low temperature cubic phase. C1 [Hubaud, Aude A.; Key, Baris; Ingram, Brian J.; Dogan, Fulya; Vaughey, John T.] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. [Schroeder, David J.] No Illinois Univ, Dept Engn Technol, Coll Engn & Engn Technol, De Kalb, IL 60115 USA. RP Hubaud, AA (reprint author), Argonne Natl Lab, Chem Sci & Engn Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM vaughey@anl.gov OI Vaughey, John/0000-0002-2556-6129 FU Integrated Laboratory Industry Research Program (ILIRP), Office of Vehicle Technologies, Office of Energy Efficiency and Renewable Energy (EERE) of the U.S. Department of Energy by UChicago Argonne LLC [DE-AC02-06CH11357] FX The authors would like to thank Dr Martin Bettge for helpful discussion and assistance with the conductivity measurements. Support for this work came from Integrated Laboratory Industry Research Program (ILIRP), Office of Vehicle Technologies, Office of Energy Efficiency and Renewable Energy (EERE) of the U.S. Department of Energy under Contract no. DE-AC02-06CH11357 by UChicago Argonne LLC and is gratefully acknowledged. NR 24 TC 40 Z9 41 U1 4 U2 124 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 31 BP 8813 EP 8818 DI 10.1039/c3ta11338h PG 6 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA 184CN UT WOS:000321864300017 ER PT J AU Yin, Z Chi, MF Zhu, QJ Ma, D Sun, JM Bao, XH AF Yin, Zhen Chi, Miaofang Zhu, Qingjun Ma, Ding Sun, Junming Bao, Xinhe TI Supported bimetallic PdAu nanoparticles with superior electrocatalytic activity towards methanol oxidation SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID TRANSMISSION ELECTRON-MICROSCOPY; ALCOHOL FUEL-CELLS; CATALYTIC-ACTIVITY; HYDROGEN-PEROXIDE; OXYGEN REDUCTION; ALKALINE MEDIA; ELECTROCHEMICAL OXIDATION; ALLOY ELECTROCATALYSTS; PALLADIUM CATALYSTS; AU AB Monodispersed bimetallic PdAu nanoparticles with controlled composition are prepared by an emulsion-assisted synthetic strategy with ternary metal precursors in the surfactants of oleic acid and oleylamine. The PdAu nanoparticles are loaded on a carbon support, and their electrocatalytic activities are tested for methanol oxidation in alkaline media. The bimetallic PdAu nanoparticles show superior electrocatalytic activities for methanol oxidation compared with the pure Pd nanoparticles prepared by the same method. The most active Pd30Au70 nanoparticles, with significantly low Pd content, even show remarkably higher activities than the commercial Pt/C catalyst. Various characterization techniques such as TEM, XPS and UV-vis are applied to study the nature of the catalysts. It is concluded that the increased activity is dependant on the unique Pd-rich shell and Au-rich core structure of such bimetallic PdAu particles as well as the nature of the Pd species on the catalyst surface. C1 [Yin, Zhen] Tianjin Polytech Univ, Sch Environm & Chem Engn, Tianjin 300387, Peoples R China. [Chi, Miaofang] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. [Zhu, Qingjun] Natl Inst Clean & Low Carbon Energy, Beijing 102209, Peoples R China. [Ma, Ding] Peking Univ, Coll Chem & Mol Engn, Beijing Natl Lab Mol Sci, Beijing 100871, Peoples R China. [Sun, Junming] Washington State Univ, Sch Chem Engn & Bioengn, Pullman, WA 99164 USA. [Bao, Xinhe] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China. RP Ma, D (reprint author), Peking Univ, Coll Chem & Mol Engn, Beijing Natl Lab Mol Sci, Beijing 100871, Peoples R China. EM dma@pku.edu.cn RI Sun, Junming/B-3019-2011; li, haobo/P-5373-2014; Yin, Zhen/I-6356-2015; Chi, Miaofang/Q-2489-2015 OI Sun, Junming/0000-0002-0071-9635; li, haobo/0000-0002-9215-3754; Yin, Zhen/0000-0002-1252-7809; Chi, Miaofang/0000-0003-0764-1567 FU National Natural Science Foundation of China [21173009, 21222306]; 973 Project [2011CB201402, 2013CB933100]; High School Science & Technology Fund Planning Project of Tianjin [20120513]; Chinese Academy of Science; Division of Scientific User Facilities, Office of Basic Energy Sciences, U. S. Department of Energy FX This work was supported by the National Natural Science Foundation of China (21173009, 21222306), 973 Project (2011CB201402, 2013CB933100), and High School Science & Technology Fund Planning Project of Tianjin (20120513). D. M. thanks the Chinese Academy of Science for financial support through the Bairen project. We gratefully acknowledge the contributions of Professor Jian Chen and Dr Yining Zhang for assistance and discussion on the electrochemical measurements, Dr Rentao Mu for discussion on the XPS spectra, from Dalian Institute of Chemical Physics, the Chinese Academy of Science. Part of the STEM work was performed at ORNL SHaRE User Facility, which is supported by the Division of Scientific User Facilities, Office of Basic Energy Sciences, U. S. Department of Energy. NR 53 TC 29 Z9 29 U1 5 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 32 BP 9157 EP 9163 DI 10.1039/c3ta11592e PG 7 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA 187LT UT WOS:000322121300021 ER PT J AU Won, J Vernon, LJ Karakuscu, A Dickerson, RM Cologna, M Raj, R Wang, YQ Yoo, SJ Lee, SH Misra, A Uberuaga, BP AF Won, Jonghan Vernon, Louis J. Karakuscu, Aylin Dickerson, Robert M. Cologna, Marco Raj, Rishi Wang, Yongqiang Yoo, Seung Jo Lee, Seok-Hoon Misra, Amit Uberuaga, Blas P. TI The role of non-stoichiometric defects in radiation damage evolution of SrTiO3 SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID RUDDLESDEN-POPPER PHASES; THIN-FILMS; AMORPHIZATION; BOUNDARY; OXIDES; STOICHIOMETRY; SIMULATIONS; IRRADIATION; PEROVSKITE; RESISTANCE AB The response of polycrystalline SrTiO3, fabricated by the flash sintering method, to ion beam irradiation was investigated by means of transmission electron microscopy (TEM) and atomic scale modeling. The samples were implanted with 250 keV Ne ions at fluences between 1.11 x 10(16) and 2.25 x 10(16) ions per cm(2) at room temperature and then characterized using scanning transmission electron microscopy and high voltage TEM. We observed that this material has a large number of Ruddlesden-Popper (RP) faults, related to the non-stoichiometry of the material, in a random and sometimes complicated arrangement. These faults have a significant impact on the radiation damage evolution of the material. In particular, the faults amorphize more quickly than the surrounding SrTiO3 matrix. We examined the interaction of point defects with the RP faults using atomistic modeling and determined that both the thermodynamic and kinetic properties of defects are significantly influenced by the presence of the faults, providing insight into the experimental observations. We conclude that planar defects such as RP faults can have a significant impact on the radiation damage evolution of SrTiO3 and might be one avenue for controlling radiation tolerance in complex materials. C1 [Won, Jonghan; Vernon, Louis J.; Karakuscu, Aylin; Dickerson, Robert M.; Wang, Yongqiang; Uberuaga, Blas P.] Los Alamos Natl Lab, Div Mat Sci & Technol, Los Alamos, NM 87545 USA. [Misra, Amit] Los Alamos Natl Lab, Ctr Integrated Nanotechnol, Los Alamos, NM 87545 USA. [Cologna, Marco; Raj, Rishi] Univ Colorado, Dept Mech Engn, Boulder, CO 80309 USA. [Won, Jonghan; Yoo, Seung Jo; Lee, Seok-Hoon] Korea Basic Sci Inst, Div Electron Microscop Res, Taejon 305333, South Korea. RP Uberuaga, BP (reprint author), Los Alamos Natl Lab, Div Mat Sci & Technol, Los Alamos, NM 87545 USA. EM jhwon@kbsi.re.kr; blas@lanl.gov RI Misra, Amit/H-1087-2012; Vernon, Louis/K-9729-2016; OI Vernon, Louis/0000-0001-5379-7488; RAJ, RISHI/0000-0001-8556-9797; won, Jonghan/0000-0002-7612-1322 FU Center for Materials at Irradiation and Mechanical Extremes, an Energy Frontier Research Center; U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences [2008LANL1026]; National Nuclear Security Administration of the U.S. DOE [DE-AC52-06NA25396]; Korea Basic Science Institute [T33526] FX The authors wish to acknowledge K. E. Sickafus and X.-M. Bai for helpful discussions. We also thank A. F. Voter for the use of his CLSMAN simulation code. This work was supported as part of the Center for Materials at Irradiation and Mechanical Extremes, an Energy Frontier Research Center funded by the U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences under Award number 2008LANL1026. Los Alamos National Laboratory, an affirmative action equal opportunity employer, is operated by Los Alamos National Security, LLC, for the National Nuclear Security Administration of the U.S. DOE under contract DE-AC52-06NA25396. Some of the microscopy reported in Fig. 3 was performed by J. W. as part of his new employment at the Korea Basic Science Institute. J. W., S. J. Y., and S. H. L. acknowledge support from the Korea Basic Science Institute, grant number T33526. NR 44 TC 4 Z9 4 U1 7 U2 37 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 32 BP 9235 EP 9245 DI 10.1039/c3ta11046j PG 11 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA 187LT UT WOS:000322121300031 ER PT J AU Nikiforov, MP Strzalka, J Jiang, Z Darling, SB AF Nikiforov, Maxim P. Strzalka, Joseph Jiang, Zhang Darling, Seth B. TI Lanthanides: new metallic cathode materials for organic photovoltaic cells SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID POLYMER SOLAR-CELLS; CONVERSION EFFICIENCY; LAYER; INTERFACE; ENERGY; TRANSMISSION; DEPOSITION; SCATTERING; BLOCKING; ANODE AB Organic photovoltaics (OPVs) are compliant with inexpensive, scalable, and environmentally benign manufacturing technologies. While substantial attention has been focused on optimization of active layer chemistry, morphology, and processing, far less research has been directed to understanding charge transport at the interfaces between the electrodes and the active layer. Electrical properties of these interfaces not only impact efficiency, but also play a central role in stability of organic solar cells. Low work function metals are the most widely used materials for the electron transport layer with Ca being the most common material. In bulk heterojunction OPV devices, low work function metals are believed to mirror the role they play in OLEDs, where such metals are used to control carrier selectivity, transport, extraction, and blocking, as well as interface band bending. Despite their advantages, low work function materials are generally prone to reactions with water, oxygen, nitrogen, and carbon dioxide from air leading to rapid device degradation. Here we discuss the search for a new metallic cathode interlayer material that increases device stability and still provides device efficiency similar to that achieved with a Ca interlayer. C1 [Nikiforov, Maxim P.; Darling, Seth B.] Argonne Natl Lab, Ctr Nanoscale Mat, Lemont, IL 60439 USA. [Strzalka, Joseph; Jiang, Zhang] Argonne Natl Lab, Xray Sci Div, Lemont, IL 60439 USA. [Darling, Seth B.] Univ Chicago, Inst Mol Engn, Chicago, IL 60637 USA. RP Nikiforov, MP (reprint author), Argonne Natl Lab, Ctr Nanoscale Mat, 9700 S Cass Ave, Lemont, IL 60439 USA. EM maximnik@gmail.com; darling@anl.gov RI Jiang, Zhang/A-3297-2012 OI Jiang, Zhang/0000-0003-3503-8909 FU U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences User Facility [DE-AC02-06CH11357]; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]; Director's Fellowship Program FX This work was performed, in part, at the Center for Nanoscale Materials, a U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences User Facility under Contract No. DE-AC02-06CH11357. Use of the Advanced Photon Source (APS) at Argonne National Laboratory was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. MPN is grateful to the Director's Fellowship Program for financial support. NR 48 TC 5 Z9 5 U1 3 U2 47 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 31 BP 13052 EP 13060 DI 10.1039/c3cp52327f PG 9 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 185GF UT WOS:000321954200031 PM 23817556 ER PT J AU Zhang, LL Huang, XY Qin, CY Brinkman, K Gong, YH Wang, SW Huang, K AF Zhang, Lingling Huang, Xinyu Qin, Changyong Brinkman, Kyle Gong, Yunhui Wang, Siwei Huang, Kevin TI First spectroscopic identification of pyrocarbonate for high CO2 flux membranes containing highly interconnected three dimensional ionic channels SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID CARBON-DIOXIDE SEPARATION; AB-INITIO CALCULATIONS; RAMAN-SPECTROSCOPY; HIGH-TEMPERATURE; CAPTURE TECHNOLOGY; ALKALI CARBONATES; POWER-GENERATION; EUTECTIC MIXTURE; BASIS-SET; CO2/CH4 AB Identification of the existence of pyrocarbonate ion C2O52- in molten carbonates exposed to a CO2 atmosphere provides key support for a newly established bi-ionic transport model that explains the mechanisms of high CO2 permeation flux observed in mixed oxide-ion and carbonate-ion conducting (MOCC) membranes containing highly interconnected three dimensional ionic channels. Here we report the first Raman spectroscopic evidence of C2O52- as an active species involved in the CO2-transport process of MOCC membranes exposed to a CO2 atmosphere. The two new broad peaks centered at 1317 cm(-1) and 1582 cm(-1) are identified as the characteristic frequencies of the C2O52- species. The measured characteristic Raman frequencies of C2O52- are in excellent agreement with the DFT-model consisting of six overlapping individual theoretical bands calculated from Li2C2O5 and Na2C2O5. C1 [Zhang, Lingling; Huang, Xinyu; Gong, Yunhui; Wang, Siwei; Huang, Kevin] Univ S Carolina, Dept Mech Engn, Columbia, SC 29201 USA. [Qin, Changyong] Benedict Coll, Dept Biol Chem & Environm Hlth Sci, Columbia, SC 29204 USA. [Brinkman, Kyle] Savannah River Natl Lab, Aiken, SC 29808 USA. RP Huang, K (reprint author), Univ S Carolina, Dept Mech Engn, Columbia, SC 29201 USA. EM kevin.huang@sc.edu RI Wang, Siwei/A-9048-2012; Qin, Changyong/F-5753-2016; OI Qin, Changyong/0000-0003-2717-3131; Brinkman, Kyle/0000-0002-2219-1253 FU U.S. Army Research Laboratory; U.S. Army Research Office [W911NF-10-R-006] FX This work is supported by the U.S. Army Research Laboratory and the U.S. Army Research Office under grant number W911NF-10-R-006. NR 53 TC 11 Z9 11 U1 3 U2 19 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 31 BP 13147 EP 13152 DI 10.1039/c3cp52362d PG 6 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 185GF UT WOS:000321954200042 PM 23824146 ER PT J AU Mehta, VK Aslam, O Dale, L Miller, N Purkey, DR AF Mehta, Vishal K. Aslam, Omar Dale, Larry Miller, Norman Purkey, David R. TI Scenario-based water resources planning for utilities in the Lake Victoria region SO PHYSICS AND CHEMISTRY OF THE EARTH LA English DT Article DE Lake Victoria; Utilities; Climate change; Water resources; Planning; WEAP ID DECISION-SUPPORT-SYSTEM; SACRAMENTO VALLEY; MANAGEMENT; IMPACTS; BASIN AB Urban areas in the Lake Victoria (LV) region are experiencing the highest growth rates in Africa. As efforts to meet increasing demand accelerate, integrated water resources management (IWRM) tools provide opportunities for utilities and other stakeholders to develop a planning framework comprehensive enough to include short term (e.g. landuse change), as well as longer term (e.g. climate change) scenarios. This paper presents IWRM models built using the Water Evaluation And Planning (WEAP) decision support system, for three towns in the LV region - Bukoba (Tanzania), Masaka (Uganda), and Kisii (Kenya). Each model was calibrated under current system performance based on site visits, utility reporting and interviews. Projected water supply, demand, revenues and costs were then evaluated against a combination of climate, demographic and infrastructure scenarios up to 2050. Our results show that water supply in all three towns is currently infrastructure limited; achieving existing design capacity could meet most projected demand until 2020s in Masaka beyond which new supply and conservation strategies would be needed. In Bukoba, reducing leakages would provide little performance improvement in the short-term, but doubling capacity would meet all demands until 2050. In Kisii, major infrastructure investment is urgently needed. In Masaka, streamflow simulations show that wetland sources could satisfy all demand until 2050, but at the cost of almost no water downstream of the intake. These models demonstrate the value of IWRM tools for developing water management plans that integrate hydroclimatology-driven supply to demand projections on a single platform. (c) 2013 Elsevier Ltd. All rights reserved. C1 [Mehta, Vishal K.; Purkey, David R.] Stockholm Environm Inst US, Davis, CA 95616 USA. [Aslam, Omar; Dale, Larry; Miller, Norman] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Mehta, Vishal K.; Aslam, Omar; Dale, Larry; Miller, Norman; Purkey, David R.] Univ Calif Berkeley, Dept Geog, Berkeley, CA 94720 USA. RP Mehta, VK (reprint author), Stockholm Environm Inst US, 400 F St, Davis, CA 95616 USA. EM vishal.mehta@sei-us.org; oaslam@lbl.gov; lldale@lbl.gov; nlmiller@lbl.gov; vishal.mehta@sei-us.org FU UN-Habitat FX Financial support from UN-Habitat is greatfully acknowledged. The authors would like to thank all the utility staff of NWSC, KWS and BUWASA, and project partners Alliance to Save Energy (ASE), Re Solve and ClimateXL. NR 25 TC 1 Z9 1 U1 1 U2 25 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 1474-7065 J9 PHYS CHEM EARTH JI Phys. Chem. Earth PY 2013 VL 61-62 BP 22 EP 31 DI 10.1016/j.pce.2013.02.007 PG 10 WC Geosciences, Multidisciplinary; Meteorology & Atmospheric Sciences; Water Resources SC Geology; Meteorology & Atmospheric Sciences; Water Resources GA 193JX UT WOS:000322557200003 ER PT S AU Cole, DR Ok, S Phan, A Rother, G Striolo, A Vlcek, L AF Cole, D. R. Ok, Salim Phan, A. Rother, G. Striolo, A. Vlcek, L. BE Hellmann, R Pitsch, H TI Carbon-bearing fluids at nanoscale interfaces SO PROCEEDINGS OF THE FOURTEENTH INTERNATIONAL SYMPOSIUM ON WATER-ROCK INTERACTION, WRI 14 SE Procedia Earth and Planetary Science LA English DT Proceedings Paper CT 14th International Symposium on Water-Rock Interaction (WRI) CY JUN 09-14, 2013 CL Avignon, FRANCE SP Int Assoc Geochemistry, Int Assoc Geochemistry (IAGC), Water Rock Interact Working Grp, French Geol Survey (BRGM), French Alternat Energy & Atom Energy Commiss, French Inst Radioprotect & Nucl Safety (IRSN), US Army Engineer Res & Dev Ctr DE carbon-bearing fluids; nanoscale interfaces; nanopores; neutron scattering; molecular dynamics ID NEUTRON-SCATTERING; CO2 AB The behaviour of fluids at mineral surfaces or in confined geometries (pores, fractures) typically differs from their bulk behaviour in many ways due to the effects of large internal surfaces and geometrical confinement. We summarize research performed on C-O-H fluids at nanoscale interfaces in materials of interest to the earth and material sciences (e.g., silica, alumina, zeolites, clays, rocks, etc.), emphasizing those techniques that assess microstructural modification and/or dynamical behaviour such as gravimetric analysis, small-angle (SANS) neutron scattering, and nuclear magnetic resonance (NMR). Molecular dynamics (MD) simulations will be described that provide atomistic characterization of interfacial and confined fluid behaviour as well as aid in the interpretation of the neutron scattering results. (C) 2013 The Authors. Published by Elsevier B.V. Selection and/or peer-review under responsibility of Organizing and Scientific Committee of WRI 14 - 2013 C1 [Cole, D. R.; Ok, Salim] Ohio State Univ, Columbus, OH 43210 USA. [Rother, G.; Vlcek, L.] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. [Phan, A.; Striolo, A.] Univ Oklahoma, Norman, OK 73019 USA. RP Cole, DR (reprint author), Ohio State Univ, Columbus, OH 43210 USA. RI Rother, Gernot/B-7281-2008; Vlcek, Lukas/N-7090-2013 OI Rother, Gernot/0000-0003-4921-6294; Vlcek, Lukas/0000-0003-4782-7702 FU Dept. of Energy Office; Basic Energy Sciences, Geosciences Program; Deep Carbon Observatory through Sloan Foundation; DOE BES EFRC Nanoscale Control of Geologic CO2 FX Support for DRC, SO, AP and AS comes from the Dept. of Energy Office, Basic Energy Sciences, Geosciences Program and the Deep Carbon Observatory through a grant from the A.P. Sloan Foundation.Support for GR and VC comes from the DOE BES EFRC Nanoscale Control of Geologic CO2. NR 8 TC 3 Z9 3 U1 0 U2 15 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA SARA BURGERHARTSTRAAT 25, PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 1878-5220 J9 PROCED EARTH PLAN SC PY 2013 VL 7 BP 175 EP 178 DI 10.1016/j.proeps.2013.03.226 PG 4 WC Geosciences, Multidisciplinary SC Geology GA BFW45 UT WOS:000321664000043 ER PT S AU Evans, WC Hurwitz, S Bergfeld, D Lewicki, J Huebner, MA Williams, CF Brown, ST AF Evans, W. C. Hurwitz, S. Bergfeld, D. Lewicki, J. Huebner, M. A. Williams, C. F. Brown, S. T. BE Hellmann, R Pitsch, H TI Water-rock interaction in the Long Valley Caldera (USA) SO PROCEEDINGS OF THE FOURTEENTH INTERNATIONAL SYMPOSIUM ON WATER-ROCK INTERACTION, WRI 14 SE Procedia Earth and Planetary Science LA English DT Proceedings Paper CT 14th International Symposium on Water-Rock Interaction (WRI) CY JUN 09-14, 2013 CL Avignon, FRANCE SP Int Assoc Geochemistry, Int Assoc Geochemistry (IAGC), Water Rock Interact Working Grp, French Geol Survey (BRGM), French Alternat Energy & Atom Energy Commiss, French Inst Radioprotect & Nucl Safety (IRSN), US Army Engineer Res & Dev Ctr DE Long Valley; geothermal; geothermometry; carbon dioxide ID HYDROTHERMAL SYSTEM; CALIFORNIA AB Water-rock interactions within the main thermal aquifer in the Long Valley Caldera are evaluated using water chemistry data from a new suite of samples. The results reflect the impact of increased geothermal production and major CO2 loss, which appears to drive calcite precipitation in the aquifer. The study provides qualitative information on the rates of mineral reactions and the response times of chemical geothermometers to declining temperatures. (C) 2012 The Authors. Published by Elsevier B. V. Selection and/or peer-review under responsibility of Organizing and Scientific Committee of WRI 14 - 2013 C1 [Evans, W. C.; Hurwitz, S.; Bergfeld, D.; Lewicki, J.; Huebner, M. A.; Williams, C. F.] US Geol Survey, 345 Middlefield Rd, Menlo Pk, CA 94025 USA. [Brown, S. T.] Lawrence Berkeley Natl Lab, Berkeley, CA USA. RP Evans, WC (reprint author), US Geol Survey, 345 Middlefield Rd, Menlo Pk, CA 94025 USA. EM wcevans@usgs.gov NR 8 TC 1 Z9 1 U1 0 U2 6 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA SARA BURGERHARTSTRAAT 25, PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 1878-5220 J9 PROCED EARTH PLAN SC PY 2013 VL 7 BP 252 EP 255 DI 10.1016/j.proeps.2013.03.186 PG 4 WC Geosciences, Multidisciplinary SC Geology GA BFW45 UT WOS:000321664000062 ER PT S AU Icenhower, JP Saldi, GD Knauss, KG AF Icenhower, Jonathan P. Saldi, Giuseppe D. Knauss, Kevin G. BE Hellmann, R Pitsch, H TI Contrasts in the geochemical behavior of carbonate and siliciclastic rocks during carbon storage and sequestration SO PROCEEDINGS OF THE FOURTEENTH INTERNATIONAL SYMPOSIUM ON WATER-ROCK INTERACTION, WRI 14 SE Procedia Earth and Plantetary Science LA English DT Proceedings Paper CT 14th International Symposium on Water-Rock Interaction (WRI) CY JUN 09-14, 2013 CL Avignon, FRANCE SP Int Assoc Geochemistry, Int Assoc Geochemistry (IAGC), Water Rock Interact Working Grp, French Geol Survey (BRGM), French Alternat Energies & Atom Energy Commiss (CEA), French Inst Radioprotect & Nucl Safety (IRSN), US Army Engineer Res & Dev Ctr DE carbon sequestration; experimental geochemistry; dissolution ID DIOXIDE; FLUID; GAS; CO2 AB In order to better understand the geochemical behavior of carbonate and siliciclastic materials that may host carbon dioxide in the subsurface, we carried out experiments using a dolostone from the Weyburn formation and an arkosic sandstone from the Newark Basin. Synthetic brine (0.7 m NaCl) saturated with CO2 with or without CH4 reacted with the powdered materials for 30 to 60 days at 100 bars pressure and 50 - 150 degrees C. The reactivity of the material was monitored by release of elements from the rock to solution over time. A subset of experiments were carried out in which an acidic heavy metals solution was injected into a Weyburn experiment in order to simulate the release of metals to solution through injection of CO2-saturated brines. The results show that the heavy metals do not stay in solution and rapidly decrease in concentration to pre-injection levels after a few days' time. (C) 2012 The Authors. Published by Elsevier B.V. C1 [Icenhower, Jonathan P.; Saldi, Giuseppe D.; Knauss, Kevin G.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Icenhower, JP (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, 1 Cyclotron Rd,Bldg 74, Berkeley, CA 94720 USA. EM jpicenhower@lbl.gov NR 6 TC 0 Z9 0 U1 4 U2 9 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA SARA BURGERHARTSTRAAT 25, PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 1878-5220 J9 PROCED EARTH PLAN SC PY 2013 VL 7 BP 377 EP 380 DI 10.1016/j.proeps.2013.03.150 PG 4 WC Geosciences, Multidisciplinary SC Geology GA BFW45 UT WOS:000321664000092 ER PT S AU Peiffer, L Wanner, C Spycher, N Sonnenthal, E Kennedy, BM AF Peiffer, L. Wanner, C. Spycher, N. Sonnenthal, E. Kennedy, B. M. BE Hellmann, R Pitsch, H TI Multicomponent vs. classical geothermometry: an evaluation using reactive transport modeling SO PROCEEDINGS OF THE FOURTEENTH INTERNATIONAL SYMPOSIUM ON WATER-ROCK INTERACTION, WRI 14 SE Procedia Earth and Plantetary Science LA English DT Proceedings Paper CT 14th International Symposium on Water-Rock Interaction (WRI) CY JUN 09-14, 2013 CL Avignon, FRANCE SP Int Assoc Geochemistry, Int Assoc Geochemistry (IAGC), Water Rock Interact Working Grp, French Geol Survey (BRGM), French Alternat Energies & Atom Energy Commiss (CEA), French Inst Radioprotect & Nucl Safety (IRSN), US Army Engineer Res & Dev Ctr DE geothermometer; geothermal exploration; reactive transport; multicomponent; modeling ID MINERAL EQUILIBRIA; WATERS AB Reactive transport simulations were used to examine the chemical evolution of deep geothermal fluids as they ascend to the surface, and to assess constraints on the application of solute geothermometers. Al and Mg concentrations of deep fluids are sensitive to precipitation-dissolution processes, affecting reservoir temperatures estimated with multicomponent geothermometry. The concentrations of major elements such as Na, K, and SiO2 are less sensitive to reequilibration, and thus geothermometers based on these elements are often reliable, but fail when dilution or mixing with saline waters occurs. For these cases, multicomponent geothermometry coupled with optimization provides a more reliable approach to reconstruct the fluid composition at depth and estimate reservoir temperatures. (C) 2012 The Authors. Published by Elsevier B.V. Selection and/or peer-review under responsibility of Organizing and Scientific Committee of WRI 14 - 2013. C1 [Peiffer, L.; Wanner, C.; Spycher, N.; Sonnenthal, E.; Kennedy, B. M.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Peiffer, L (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. EM lpeiffer@lbl.gov NR 10 TC 0 Z9 0 U1 0 U2 3 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA SARA BURGERHARTSTRAAT 25, PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 1878-5220 J9 PROCED EARTH PLAN SC PY 2013 VL 7 BP 665 EP 668 DI 10.1016/j.proeps.2013.03.103 PG 4 WC Geosciences, Multidisciplinary SC Geology GA BFW45 UT WOS:000321664000162 ER PT S AU Um, W Wang, GH Serne, RJ AF Um, Wooyong Wang, Guohui Serne, R. Jeffrey BE Hellmann, R Pitsch, H TI The effects of secondary mineral precipitates on Sr-90 mobility at the Hanford Site, USA SO PROCEEDINGS OF THE FOURTEENTH INTERNATIONAL SYMPOSIUM ON WATER-ROCK INTERACTION, WRI 14 SE Procedia Earth and Plantetary Science LA English DT Proceedings Paper CT 14th International Symposium on Water-Rock Interaction (WRI) CY JUN 09-14, 2013 CL Avignon, FRANCE SP Int Assoc Geochemistry, Int Assoc Geochemistry (IAGC), Water Rock Interact Working Grp, French Geol Survey (BRGM), French Alternat Energies & Atom Energy Commiss (CEA), French Inst Radioprotect & Nucl Safety (IRSN), US Army Engineer Res & Dev Ctr DE radioactive strontium; secondary precipitate; retardation; colloids; Hanford site AB The effects of secondary precipitates on Sr-90 transport at the Hanford Site were investigated using quartz column experiments with simulated caustic tank waste leachates (STWL). Significantly enhanced retardation of Sr transport was observed in the column contacted with STWL due to Sr sorption and co-precipitation with neo-formed nitrate-cancrinite. However, the column results also suggest that neo-formed secondary precipitates could behave like native mobile colloids that can enhance Sr transport. Initially immobilized Sr within secondary precipitates could remobilize given a change in the porewater background conditions. The mobility of the neo-formed Sr-bearing precipitates increased with increased solution flow rate. In the field, porewater contents and flow rates can be changed by snowmelt (or storm water) events or artificial infiltration. The increased porewater flow rate caused by these events could affect the mobility of Sr-90-containing secondary precipitates, which can be a potential source for facilitated Sr transport in Hanford Site subsurface environments. (C) 2013 The Authors. Published by Elsevier B. V. Selection and/or peer-review under responsibility of the Organizing and Scientific Committee of WRI 14-2013 C1 [Um, Wooyong; Wang, Guohui; Serne, R. Jeffrey] Pacific NW Natl Lab, Richland, WA 99354 USA. RP Um, W (reprint author), Pacific NW Natl Lab, 902 Battelle Blvd,MSIN P7-54, Richland, WA 99354 USA. EM wooyong.um@pnnl.gov NR 0 TC 0 Z9 0 U1 1 U2 2 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA SARA BURGERHARTSTRAAT 25, PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 1878-5220 J9 PROCED EARTH PLAN SC PY 2013 VL 7 BP 855 EP 858 DI 10.1016/j.proeps.2013.03.032 PG 4 WC Geosciences, Multidisciplinary SC Geology GA BFW45 UT WOS:000321664000209 ER PT S AU Wanner, C Peiffer, L Sonnenthal, E Spycher, N Iovenitti, J Kennedy, BM AF Wanner, Christoph Peiffer, Loic Sonnenthal, Eric Spycher, Nicolas Iovenitti, Joe Kennedy, Burton M. BE Hellmann, R Pitsch, H TI On the use of chemical geothermometry: A reactive transport modeling study of the Dixie Valley geothermal area SO PROCEEDINGS OF THE FOURTEENTH INTERNATIONAL SYMPOSIUM ON WATER-ROCK INTERACTION, WRI 14 SE Procedia Earth and Planetary Science LA English DT Proceedings Paper CT 14th International Symposium on Water-Rock Interaction (WRI) CY JUN 09-14, 2013 CL Avignon, FRANCE SP Int Assoc Geochemistry, Int Assoc Geochemistry (IAGC), Water Rock Interact Working Grp, French Geol Survey (BRGM), French Alternat Energy & Atom Energy Commiss, French Inst Radioprotect & Nucl Safety (IRSN), US Army Engineer Res & Dev Ctr DE geothermal systems; geothermometry; reactive transport modeling; Dixie Valley; geothermal exploration ID WATERS AB A 2D reactive transport model of the Dixie Valley geothermal field in Nevada, USA was developed to assess the conditions under which chemical geothermometers operate as powerful exploration tools. Model concentrations read out at the surface were processed by multicomponent geothermometry to compare inferred reservoir temperatures with true reservoir temperatures of the model. Varying reactive fracture surface areas revealed that re-equilibration does not occur if the effective fracture surface area is 1-3 orders of magnitude lower than the corresponding geometric surface area. Moreover, it could be shown that a full re-equilibration is hindered if the fluid velocity within a fracture is on the order of 1 m/day. It was concluded that such upflow rates and relatively low reactive fracture surface areas are likely occurring at a wide series of geothermal fields, confirming that geothermometers can be used as powerful geochemical exploration tools. (C) 2013 The Authors. Published by Elsevier B.V. C1 [Wanner, Christoph; Peiffer, Loic; Sonnenthal, Eric; Spycher, Nicolas; Kennedy, Burton M.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Earth Sci Div, 1 Cyclotron Rd, Berkeley, CA 94720 USA. [Iovenitti, Joe] AltaRockEnergy Inc, Sausalito, CA USA. RP Wanner, C (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Earth Sci Div, 1 Cyclotron Rd, Berkeley, CA 94720 USA. EM cwanner@lbl.gov FU U.S. Department of Energy; Geothermal Technologies Program, Energy Efficiency and Renewable Energy Office [DE-EE0002765, DE-AC02-05CH11231] FX This work was supported by the U.S. Department of Energy, Geothermal Technologies Program, Energy Efficiency and Renewable Energy Office, Award No DE-EE0002765 and DE-AC02-05CH11231. NR 9 TC 0 Z9 0 U1 0 U2 1 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA SARA BURGERHARTSTRAAT 25, PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 1878-5220 J9 PROCED EARTH PLAN SC PY 2013 VL 7 BP 884 EP 887 DI 10.1016/j.proeps.2013.03.107 PG 4 WC Geosciences, Multidisciplinary SC Geology GA BFW45 UT WOS:000321664000216 ER PT S AU Lund, KR Lynn, KG Weber, MH Okuniewski, MA AF Lund, K. R. Lynn, K. G. Weber, M. H. Okuniewski, M. A. BE Alam, A Coleman, P Dugdale, S Roussenova, M TI Vacancy Formation Enthalpy in Polycrystalline Depleted Uranium SO 16TH INTERNATIONAL CONFERENCE ON POSITRON ANNIHILATION (ICPA-16) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 16th International Conference on Positron Annihilation (ICPA) CY AUG 19-24, 2012 CL Univ Bristol, H H Wills Phys Lab, Bristol, ENGLAND SP Ortech, Canberra, Univ Bristol HO Univ Bristol, H H Wills Phys Lab ID POSITRON-ANNIHILATION; SPECTROSCOPY AB Positron Annihilation Spectroscopy was performed as a function of temperature and beam energy on polycrystalline depleted uranium (DU) foil. Samples were run with varying heat profiles all starting at room temperature. While collecting Doppler-Broadening data, the temperature of the sample was cycled several times. The first heat cycle shows an increasing S-parameter near temperatures of 400K to 500K much lower than the first phase transition of 941K indicating increasing vacancies possibly due to oxygen diffusion from the bulk to the surface. Vacancy formation enthalpies were calculated fitting a model to the data to be 1.6 +/- 0.16 eV. Results are compared to previous work [3,4]. C1 [Lund, K. R.; Lynn, K. G.; Weber, M. H.] Washington State Univ, Ctr Mat Res, Pullman, WA 99164 USA. [Okuniewski, M. A.] Idaho Natl Lab, Idaho Falls, ID USA. RP Lund, KR (reprint author), Washington State Univ, Ctr Mat Res, Pullman, WA 99164 USA. EM kasey.lund@email.wsu.edu FU Idaho National Laboratory [00014002] FX We would like to acknowledge Idaho National Laboratory for funding under contract number 00014002, as well as Narendra Parmar and Ryan Stewart for their discussions and help in the lab. NR 8 TC 3 Z9 3 U1 1 U2 4 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 443 AR 012021 DI 10.1088/1742-6596/443/1/012021 PG 4 WC Physics, Atomic, Molecular & Chemical; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFX12 UT WOS:000321739400021 ER PT S AU Patil, K Sellaiyan, S Rajkhowa, R Tsuzuki, T Lin, T Smith, SV Wang, X Uedono, A AF Patil, K. Sellaiyan, S. Rajkhowa, R. Tsuzuki, T. Lin, T. Smith, S. V. Wang, X. Uedono, A. BE Alam, A Coleman, P Dugdale, S Roussenova, M TI Positron annihilation lifetime spectroscopy of mechanically milled protein fibre powders and their free volume aspects SO 16TH INTERNATIONAL CONFERENCE ON POSITRON ANNIHILATION (ICPA-16) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 16th International Conference on Positron Annihilation (ICPA) CY AUG 19-24, 2012 CL Univ Bristol, H H Wills Phys Lab, Bristol, ENGLAND SP Ortech, Canberra, Univ Bristol HO Univ Bristol, H H Wills Phys Lab ID POLYMERS AB The present study reports the fabrication of ultra-fine powders from animal protein fibres such as cashmere guard hair, merino wool and eri silk along with their free volume aspects. The respectively mechanically cleaned, scoured and degummed cashmere guard hair, wool and silk fibres were converted into dry powders by a process sequence: Chopping, Attritor Milling, and Spray Drying. The fabricated protein fibre powders were characterised by scanning electron microscope, particle size distribution and positron annihilation lifetime spectroscopy (PALS). The PALS results indicated that the average free volume size in protein fibres increased on their wet mechanical milling with a decrease in the corresponding intensities leading to a resultant decrease in their fractional free volumes. C1 [Patil, K.; Rajkhowa, R.; Tsuzuki, T.; Lin, T.; Wang, X.] Deakin Univ, Inst Frontier Mat, Geelong, Vic 3217, Australia. [Sellaiyan, S.] Australian Nucl Sci & Technol Org, Ctr Excellence Antimatter Matter Studies, Kirrawee 2232, Australia. [Sellaiyan, S.] Australian Natl Univ, Ctr Excellence Antimatter Matter Studies, Res Sch Phys & Engn, Canberra, ACT 0200, Australia. [Sellaiyan, S.] Univ Tsukuba, Tandem Accelerator Complex, Ibaraki 3058577, Japan. [Smith, S. V.] Brookhaven Natl Lab, Collider Accelerator Dept, Upton, NY 11973 USA. [Uedono, A.] Univ Tsukuba, Fac Pure & Appl Sci, Div Appl Phys, Tsukuba, Ibaraki 3058573, Japan. RP Patil, K (reprint author), Deakin Univ, Inst Frontier Mat, Geelong, Vic 3217, Australia. EM selva2d@yahoo.co.in RI Lin, Tong/A-3505-2008; Tsuzuki, Takuya/A-7058-2009 OI Lin, Tong/0000-0002-1003-0671; Tsuzuki, Takuya/0000-0002-2002-3758 FU Australian Research Council [1094979] FX Financial support from Australian Research Council (DP 1094979) is acknowledged. NR 13 TC 0 Z9 0 U1 0 U2 3 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 443 AR 012054 DI 10.1088/1742-6596/443/1/012054 PG 4 WC Physics, Atomic, Molecular & Chemical; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFX12 UT WOS:000321739400054 ER PT B AU Abdollahy, S Mammoli, A Cheng, F Ellis, A Johnson, J AF Abdollahy, S. Mammoli, A. Cheng, F. Ellis, A. Johnson, J. GP IEEE TI Distributed Compensation of a Large Intermittent Energy Resource in a Distribution Feeder SO 2013 IEEE PES INNOVATIVE SMART GRID TECHNOLOGIES (ISGT) LA English DT Proceedings Paper CT Conference of the IEEE PES on Innovative Smart Grid Technologies (ISGT) CY FEB 24-27, 2013 CL Washington, DC SP IEEE PES DE distributed energy resources(DER); microgrid; Demand-Response(DR); State of Charge(SoC) AB In a smart grid demonstration project in New Mexico, a combination of a 500kW PV farm and a 1MWh utility scale storage system which consists of a 500kW ultra fast smoothing battery and a 250kW shifting battery are installed. At a nearby location, a micro grid demonstration which incorporates a 240kW natural gas-powered generator, a 80kW fuel cell, a 50kW PV generator, a lead-acid battery storage system, and hot and cold thermal storage is installed. With the current configuration, the storage system associated with the 500kW PV is able to smooth PV output, to shift the peak generation to the time of peak consumption and also to firm the PV resource as a fixed amount of power. The problem is how the system would be managed in presence of several distributed resources with different ramp rates and capacities and different operation costs, which would reduce the stress placed on the battery. In this paper, the results of the different studies on the system model are discussed. A complete feeder model in GridLAB-D is used to demonstrate several control algorithms. In one scenario, all other available generations are planned to compensate the PV generation ramp rate based on their individual capacity. Each agent will compensate the ramp rate of the total generation of the higher priority agents based on its own capacity. In another scenario, individual agents try to compensate the deficit in power generation scheduled for the whole system. Every particular agent is responsible for compensating the difference between the scheduled and the total generation of the higher priority agents. C1 [Abdollahy, S.; Cheng, F.] Univ New Mexico, Dept Elect & Comp Engn, Albuquerque, NM 87131 USA. [Mammoli, A.] Univ New Mexico, Mech Engn Dept, Albuquerque, NM USA. [Johnson, J.] Sandia Natl Labs, Albuquerque, NM USA. RP Abdollahy, S (reprint author), Univ New Mexico, Dept Elect & Comp Engn, Albuquerque, NM 87131 USA. EM shahinab@unm.edu FU Department of Energy [DE-OE0000230, EPRI P.A. EP_P32412/C15054] FX This material is based upon work supported partially by the Department of Energy under award number DE-OE0000230 and EPRI P.A. EP_P32412/C15054 . NR 4 TC 0 Z9 0 U1 0 U2 0 PU IEEE PI NEW YORK PA 345 E 47TH ST, NEW YORK, NY 10017 USA BN 978-1-4673-4896-6; 978-1-4673-4894-2 PY 2013 PG 6 WC Computer Science, Theory & Methods; Engineering, Electrical & Electronic SC Computer Science; Engineering GA BFM26 UT WOS:000320500800122 ER PT J AU Kirkham, H AF Kirkham, H. GP IEEE TI The Digital Revolution in Measurements SO 2013 IEEE PES INNOVATIVE SMART GRID TECHNOLOGIES (ISGT) LA English DT Proceedings Paper CT Conference of the IEEE PES on Innovative Smart Grid Technologies (ISGT) CY FEB 24-27, 2013 CL Washington, DC SP IEEE PES DE Measurements; digital measurements; abstraction; data compression; measurand definition AB This paper considers what it means to make a measurement, and the changes in measurement technology over the years. The impact of the latest changes, which have resulted in most electrical measurements being done digitally, is explored. It is argued that the process of measurement can be considered equivalent to one of data compression. The smart grid will certainly result in many more signals being made available, and therefore a great deal of data compression will be taking place. Measurements will be made in parts of the power system presently unmonitored, as well as parts that are already well covered by instrumentation. The smart grid engineer must decide what it means to have "useful" information. Unless care is taken, the signal processing may furnish information that is not useful, and may not even make sense. The paper concludes by examining the possibilities of data compression from multiple separate signals. C1 Pacific NW Natl Lab, Richland, WA 99352 USA. RP Kirkham, H (reprint author), Pacific NW Natl Lab, Richland, WA 99352 USA. EM Harold.Kirklham@pnnl.gov NR 10 TC 0 Z9 0 U1 0 U2 1 PU IEEE PI NEW YORK PA 345 E 47TH ST, NEW YORK, NY 10017 USA BN 978-1-4673-4896-6 PY 2013 PG 6 WC Computer Science, Theory & Methods; Engineering, Electrical & Electronic SC Computer Science; Engineering GA BFM26 UT WOS:000320500800086 ER PT J AU Kirkham, H Marinovici, C AF Kirkham, Harold Marinovici, Cristina GP IEEE TI Technology Readiness and the Smart Grid SO 2013 IEEE PES INNOVATIVE SMART GRID TECHNOLOGIES (ISGT) LA English DT Proceedings Paper CT Conference of the IEEE PES on Innovative Smart Grid Technologies (ISGT) CY FEB 24-27, 2013 CL Washington, DC SP IEEE PES DE smart grid; standards; technology readiness; TRL; SGL AB Technology Readiness Levels (TRLs) originated as a way for the National Aeronautics and Space Administration (NASA) to monitor the development of systems being readied for space. The technique has found wide application as part of the more general topic of system engineering. In this paper, we consider the applicability of TRLs to systems being readied for the smart grid. We find that there are many useful parallels, and much to be gained by this application. However, TRLs were designed for a developer who was also a user. That is not usually the case for smart grid developments. We consider the matter from the point of view of the company responsible for implementation, typically a utility, and we find that there is a need for connecting the many standards in the industry. That connection is explored, and some new considerations are introduced. C1 [Kirkham, Harold; Marinovici, Cristina] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Kirkham, H (reprint author), Pacific NW Natl Lab, Richland, WA 99352 USA. EM harold.kirkham@pnnl.gov; cristina_marinovici@pnnl.gov NR 14 TC 0 Z9 0 U1 0 U2 6 PU IEEE PI NEW YORK PA 345 E 47TH ST, NEW YORK, NY 10017 USA BN 978-1-4673-4896-6 PY 2013 PG 6 WC Computer Science, Theory & Methods; Engineering, Electrical & Electronic SC Computer Science; Engineering GA BFM26 UT WOS:000320500800019 ER PT J AU MacDonald, D Clements, SL Patrick, SW Perkins, C Muller, G Lancaster, MJ Hutton, W AF MacDonald, Doug Clements, Samuel L. Patrick, Scott W. Perkins, Casey Muller, George Lancaster, Mary J. Hutton, Will GP IEEE TI Cyber/Physical Security Vulnerability Assessment Integration SO 2013 IEEE PES INNOVATIVE SMART GRID TECHNOLOGIES (ISGT) LA English DT Proceedings Paper CT Conference of the IEEE PES on Innovative Smart Grid Technologies (ISGT) CY FEB 24-27, 2013 CL Washington, DC SP IEEE PES DE Risk analysis; Security; Modeling; Simulation; Power Industry AB Securing high value and critical assets is one of the biggest challenges facing this nation and others around the world. In modern integrated systems, there are four potential modes of attack available to an adversary: physical only attack, cyber only attack, physical-enabled cyber attack, cyber-enabled physical attack. Blended attacks involve an adversary working in one domain to reduce system effectiveness in another domain. This enables the attacker to penetrate further into the overall layered defenses. Existing vulnerability assessment (VA) processes and software tools which predict facility vulnerabilities typically evaluate the physical and cyber domains separately. Vulnerabilities which result from the integration of cyber-physical control systems are not well characterized and are often overlooked by existing assessment approaches. In this paper, we modified modification of the timely detection methodology, used for decades in physical security VAs, to include cyber components. The Physical and Cyber Risk Analysis Tool (PACRAT) prototype illustrates an integrated vulnerability assessment that includes cyber-physical interdependencies. Information about facility layout, network topology, and emplaced safeguards is used to evaluate how well suited a facility is to detect, delay, and respond to attacks, to identify the pathways most vulnerable to attack, and to evaluate how often safeguards are compromised for a given threat or adversary type. We have tested the PACRAT prototype on critical infrastructure facilities and the results are promising. Future work includes extending the model to prescribe the recommended security improvements via an automated cost-benefit analysis. C1 [MacDonald, Doug; Clements, Samuel L.; Patrick, Scott W.; Perkins, Casey; Muller, George; Lancaster, Mary J.; Hutton, Will] Pacific NW Natl Lab, Richland, WA 99352 USA. RP MacDonald, D (reprint author), Pacific NW Natl Lab, Richland, WA 99352 USA. NR 5 TC 0 Z9 0 U1 1 U2 4 PU IEEE PI NEW YORK PA 345 E 47TH ST, NEW YORK, NY 10017 USA BN 978-1-4673-4896-6 PY 2013 PG 6 WC Computer Science, Theory & Methods; Engineering, Electrical & Electronic SC Computer Science; Engineering GA BFM26 UT WOS:000320500800094 ER PT B AU Marinovici, MC Kirkham, H Glass, KA Carlsen, LC AF Marinovici, M. C. Kirkham, H. Glass, K. A. Carlsen, L. C. GP IEEE TI Modeling Power System Operation with Intermittent Resources SO 2013 IEEE PES INNOVATIVE SMART GRID TECHNOLOGIES (ISGT) LA English DT Proceedings Paper CT Conference of the IEEE PES on Innovative Smart Grid Technologies (ISGT) CY FEB 24-27, 2013 CL Washington, DC SP IEEE PES DE economic dispatch; load following; multi objective optimization problem; renewable energies; unit commitment AB Electricity generating companies and power system operators face the need to minimize total fuel cost and maximize total profit over a given time period. These issues become optimization problems subject to a large number of constraints that must be satisfied simultaneously. The grid updates due to smart-grid technologies, plus the penetration of intermittent re-sources in electrical grid, introduce additional complexity to the optimization problem. The Renewable Integration Model (RIM) is a computer model of an interconnected power system. It is intended to provide insight and advice on complex power systems management, as well as answers to questions relating to the integration of renewable energy. This paper describes the RIM basic design concept, solution method, and the initial suite of modules that it supports. C1 [Marinovici, M. C.; Kirkham, H.; Glass, K. A.; Carlsen, L. C.] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Marinovici, MC (reprint author), Pacific NW Natl Lab, Richland, WA 99352 USA. EM cristina.marinovici@pnnl.gov; harold.kirkham@pnnl.gov; kevin.glass@pnnl.gov; leif.carlsen@pnnl.gov NR 6 TC 0 Z9 0 U1 2 U2 2 PU IEEE PI NEW YORK PA 345 E 47TH ST, NEW YORK, NY 10017 USA BN 978-1-4673-4896-6; 978-1-4673-4894-2 PY 2013 PG 6 WC Computer Science, Theory & Methods; Engineering, Electrical & Electronic SC Computer Science; Engineering GA BFM26 UT WOS:000320500800053 ER PT B AU McKinnon, AD Thompson, SR Doroshchuk, RA Fink, GA Fulp, EW AF McKinnon, A. David Thompson, Seth R. Doroshchuk, Ruslan A. Fink, Glenn A. Fulp, Errin W. GP IEEE TI Bio-Inspired Cyber Security for Smart Grid Deployments SO 2013 IEEE PES INNOVATIVE SMART GRID TECHNOLOGIES (ISGT) LA English DT Proceedings Paper CT Conference of the IEEE PES on Innovative Smart Grid Technologies (ISGT) CY FEB 24-27, 2013 CL Washington, DC SP IEEE PES DE Agents; Bio-inspired; Computer security; Cyber security; Smart Grid; Smart meters AB Smart Grid technologies are transforming the electric power system in ways that will significantly impact electric distribution systems and result in greater efficiency. However, the increased scale of the grid and the new types of information it will transmit introduce security risks that cannot be addressed by traditional, centralized security techniques. We propose a scalable approach inspired by the complex-adaptive control systems of social insects, such as ants and bees. These systems emerge from inter-agent communication and the collective application of simple rules. The Digital Ants framework is a bio-inspired framework that uses lightweight, mobile agents. The agents communicate using digital pheromones which enable the agents to alert each other of possible cyber security issues. All communication and coordination is both localized and decentralized thereby allowing the framework to scale across the large numbers of devices that will exist in the Smart Grid. Furthermore, being lightweight makes the agents suitable for implementation on devices with limited computational resources. This paper will provide a brief overview of the Digital Ants framework and then present results from testbed-based demonstrations that show how Digital Ants can identify a cyber security attack scenario against smart meter deployments. C1 [McKinnon, A. David; Thompson, Seth R.; Doroshchuk, Ruslan A.; Fink, Glenn A.] Pacific Northwest Natl Lab, Secure Cyber Syst Grp, Richland, WA 99352 USA. [Fulp, Errin W.] Wake Forest Univ, Dept Comp Sci, Winston Salem, NC USA. RP McKinnon, AD (reprint author), Pacific Northwest Natl Lab, Secure Cyber Syst Grp, Richland, WA 99352 USA. EM david.mckinnon@pnnl.gov; fulp@wfu.edu FU U. S. Department of Energy [DEAC0576RL01830] FX This research was supported, in part, by the U.S. Department of Energy under U. S. Department of Energy Contract DEAC0576RL01830. NR 15 TC 0 Z9 0 U1 0 U2 0 PU IEEE PI NEW YORK PA 345 E 47TH ST, NEW YORK, NY 10017 USA BN 978-1-4673-4896-6; 978-1-4673-4894-2 PY 2013 PG 6 WC Computer Science, Theory & Methods; Engineering, Electrical & Electronic SC Computer Science; Engineering GA BFM26 UT WOS:000320500800091 ER PT B AU Tesfaye, M Castello, CC AF Tesfaye, M. Castello, C. C. GP IEEE TI Minimization of Impact from Electric Vehicle Supply Equipment to the Electric Grid Using a Dynamically Controlled Battery Bank for Peak Load Shaving SO 2013 IEEE PES INNOVATIVE SMART GRID TECHNOLOGIES (ISGT) LA English DT Proceedings Paper CT Conference of the IEEE PES on Innovative Smart Grid Technologies (ISGT) CY FEB 24-27, 2013 CL Washington, DC SP IEEE PES DE Battery Management Systems; Control System; Scheduling Algorithm; Electric Vehicles; Power System Control AB This research presents a comparison of two control systems for peak load shaving using local solar power generation (i.e., photovoltaic array) and local energy storage (i.e., battery bank). The purpose is to minimize load demand of electric vehicle supply equipment (EVSE) on the electric grid. Static and dynamic control systems are compared to decrease demand from EVSE. Static control of the battery bank is based on charging and discharging to the electric grid at fixed times. Dynamic control, with 15-minute resolution, forecasts EVSE load based on data analysis of collected data. In the proposed dynamic control system, the sigmoid function is used to shave peak loads while limiting scenarios that can quickly drain the battery bank. These control systems are applied to Oak Ridge National Laboratory's (ORNL) solar-assisted electric vehicle (EV) charging stations. This installation is composed of three independently grid-tied sub-systems: (1) 25 EVSE; (2) a 47 kW photovoltaic (PV) array; and (3) a 60 kWh battery bank. The dynamic control system achieved the greatest peak load shaving, up to 34% on a cloudy day and 38% on a sunny day. The static control system was not ideal; peak load shaving was 14.6% on a cloudy day and 12.7% on a sunny day. Simulations based on ORNL data show solar-assisted EV charging stations combined with the proposed dynamic battery control system can negate up to 89% of EVSE load demand on sunny days. C1 [Tesfaye, M.] Tennessee State Univ, Nashville, TN 37209 USA. [Castello, C. C.] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. RP Tesfaye, M (reprint author), Tennessee State Univ, Nashville, TN 37209 USA. EM mekbibtesfaye@yahoo.com; castellocc@ornl.gov FU U.S. Department of Energy's (DOE); American Recovery and Reinvestment Act (ARRA) [DE-EE0002194]; U.S. DOE [DE-ACOS-000R2272S] FX This work was supported by the U.S. Department of Energy's (DOE) American Recovery and Reinvestment Act (ARRA) under Grant DE-EE0002194. Oak Ridge National Laboratory (ORNL) is managed by UT-Battelle, LLC, for the U.S. DOE under contract DE-ACOS-000R2272S. NR 9 TC 0 Z9 0 U1 0 U2 2 PU IEEE PI NEW YORK PA 345 E 47TH ST, NEW YORK, NY 10017 USA BN 978-1-4673-4896-6; 978-1-4673-4894-2 PY 2013 PG 6 WC Computer Science, Theory & Methods; Engineering, Electrical & Electronic SC Computer Science; Engineering GA BFM26 UT WOS:000320500800029 ER PT B AU Ton, D Biviji, MA Nagypal, E Wang, JH AF Ton, Dan Biviji, Mustafa A. Nagypal, Eva Wang, Jianhui GP IEEE TI Tool for Determining Price Elasticity of Electricity Demand and Designing Dynamic Price Program SO 2013 IEEE PES INNOVATIVE SMART GRID TECHNOLOGIES (ISGT) LA English DT Proceedings Paper CT Conference of the IEEE PES on Innovative Smart Grid Technologies (ISGT) CY FEB 24-27, 2013 CL Washington, DC SP IEEE PES DE Load Management; Smart Grids; Dynamic Pricing; Electric Utilities AB A tool has been developed to determine the price elasticity of electricity demand using data from dynamic pricing pilots with time of use and/or critical peak pricing rates. Elasticity values are derived from an augmented Constant Elasticity of Substitution model. Using the calculated elasticity values, the tool can further project changes in electricity loads as a function of electricity prices and temperatures as specified by utilities; conversely, the tool is capable of calculating the pricing structure necessary to achieve utility-defined objectives for peak load reduction and revenue, under a given set of temperatures. Data from the California Statewide Pricing Pilot study was used for tool development and testing. Tool testing was conducted by comparing the loads and shift in loads, calculated from the tool versus observed from the pilot study, resulting in close agreements. Furthermore, use of this tool under three likely scenarios of interest to utilities is presented. C1 [Ton, Dan] US DOE, Washington, DC 20585 USA. [Biviji, Mustafa A.] Energy & Environm Resources Grp LLC, Pittsburgh, PA 15237 USA. [Nagypal, Eva; Wang, Jianhui] Argonne Natl Lab, Argonne, IL 60439 USA. RP Ton, D (reprint author), US DOE, Washington, DC 20585 USA. EM dan.ton@hq.doe.gov; mustafa@e2rg.com; enagypal@anl.gov; jianhui.wang@anl.gov NR 11 TC 0 Z9 0 U1 0 U2 1 PU IEEE PI NEW YORK PA 345 E 47TH ST, NEW YORK, NY 10017 USA BN 978-1-4673-4896-6; 978-1-4673-4894-2 PY 2013 PG 6 WC Computer Science, Theory & Methods; Engineering, Electrical & Electronic SC Computer Science; Engineering GA BFM26 UT WOS:000320500800060 ER PT J AU Zhang, Y Lu, N AF Zhang, Yu Lu, Ning GP IEEE TI Demand-side Management of Air Conditioning Cooling Loads for Intra-hour Load Balancing SO 2013 IEEE PES INNOVATIVE SMART GRID TECHNOLOGIES (ISGT) LA English DT Proceedings Paper CT Conference of the IEEE PES on Innovative Smart Grid Technologies (ISGT) CY FEB 24-27, 2013 CL Washington, DC SP IEEE PES DE demand response; load management; direct load control; thermostatically controlled appliances; ancillary service; renewable integration; smart grid; optimal parameter selection AB This paper evaluates the performance of a centralized load controller designed to provide intra-hour load balancing services (LBSs) using air conditioning (a/c) units in their cooling modes. First, thermal models of a/c units and the control logic of the central controller are presented. The objective is to control the aggregated consumption of the thermostatically controlled appliances (TCAs) to follow a desired load profile for providing LBSs. The simulations are carried out in a MATLAB/Simulink environment. A total of 1000 a/c units in their cooling modes are modeled to provide a realistic +/- 1 MW load balancing signal for 24 hours for baseline settings. The impacts of lockout times, ambient temperatures, heat gains, and two-way communication delays on the demand-side management (DSM) performance are modeled. The cost of communication between the TCAs and the central controller, customer comfort, device life cycles, and control errors are used as metrics to evaluate the DSM performance. The results demonstrate that the DSM controller precisely controls the aggregated heating, ventilating, and air conditioning load shapes while maintaining load diversity. The controllable and the measurable load services that the controller provides can be used for many other demand response applications, such as peak shaving, load shifting, and arbitrage. C1 [Zhang, Yu; Lu, Ning] Pacific NW Natl Lab, Energy Sci & Technol Div, Richland, WA 99352 USA. RP Zhang, Y (reprint author), Pacific NW Natl Lab, Energy Sci & Technol Div, Richland, WA 99352 USA. EM Yu.Zhang@pnnl.gov; ninglu134@gmail.com NR 14 TC 0 Z9 0 U1 0 U2 0 PU IEEE PI NEW YORK PA 345 E 47TH ST, NEW YORK, NY 10017 USA BN 978-1-4673-4896-6 PY 2013 PG 6 WC Computer Science, Theory & Methods; Engineering, Electrical & Electronic SC Computer Science; Engineering GA BFM26 UT WOS:000320500800116 ER PT S AU Benner, R Echeverria, VTE Onunkwo, U Patel, J Zage, D AF Benner, Robert Echeverria, Victor T. E. Onunkwo, Uzoma Patel, Jay Zage, David GP IEEE TI Harnessing Many-core Processors for Scalable, Highly Efficient, and Adaptable Firewall Solutions SO 2013 INTERNATIONAL CONFERENCE ON COMPUTING, NETWORKING AND COMMUNICATIONS (ICNC) SE International Conference on Computer Networking and Communications LA English DT Proceedings Paper CT International Conference on Computing, Networking and Communications (ICNC) CY JAN 28-31, 2013 CL San Diego, CA AB Many-core processors have become the mainstay of today's computing systems. This fact and their ease of accessibility is now broadening the horizons of computational advances. In this work, we demonstrate the use of many-core processing platforms to provide scalable, efficient, and easily configurable firewall implementations on many-core processors. Our work has made possible, to the best of our knowledge, a first-known pipelined and scalable implementation of a stateful firewall on many-core processors. We discuss the results of our work and highlight areas for future considerations and improvements. Although this work focuses on the firewall as an exemplar network protection tool, the ideas developed apply to other network processing applications like network intrusion detection systems. C1 [Benner, Robert; Echeverria, Victor T. E.; Onunkwo, Uzoma; Patel, Jay; Zage, David] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Benner, R (reprint author), Sandia Natl Labs, POB 5800, Albuquerque, NM 87185 USA. EM rebenne@sandia.gov; vtechev@sandia.gov; uonunkw@sandia.gov; jaypate@sandia.gov; djzage@sandia.gov NR 13 TC 0 Z9 0 U1 0 U2 0 PU IEEE PI NEW YORK PA 345 E 47TH ST, NEW YORK, NY 10017 USA SN 2325-2626 BN 978-1-4673-0009-4 J9 INT CONF COMPUT NETW PY 2013 PG 5 WC Computer Science, Hardware & Architecture; Telecommunications SC Computer Science; Telecommunications GA BFT23 UT WOS:000321210800119 ER PT S AU Dobrovitski, VV Fuchs, GD Falk, AL Santori, C Awschalom, DD AF Dobrovitski, V. V. Fuchs, G. D. Falk, A. L. Santori, C. Awschalom, D. D. BE Langer, JS TI Quantum Control over Single Spins in Diamond SO ANNUAL REVIEW OF CONDENSED MATTER PHYSICS, VOL 4 SE Annual Review of Condensed Matter Physics LA English DT Review; Book Chapter DE nitrogen; vacancy; qubit; information; defect; coherence; diamond ID SOLID-STATE SPIN; NITROGEN-VACANCY CENTER; N-V CENTER; NUCLEAR-SPIN; ROOM-TEMPERATURE; NANOSCALE RESOLUTION; ELECTRONIC-STRUCTURE; COHERENT DYNAMICS; COLOR-CENTERS; FIELD AB Nitrogen-vacancy (NV) centers in diamond have recently emerged as a unique platform for fundamental studies in quantum information and nanoscience. The special properties of these impurity centers allow robust, room-temperature operation of solid-state qubits and have enabled several remarkable demonstrations in quantum information processing and precision nanoscale sensing. This article reviews the recent advances in magnetic and optical manipulation of the NV center's quantum spin and their importance for prospective applications. We discuss how quantum control of individual centers can be harnessed for the protection of NV-center spin coherence, for multiqubit quantum operations in the presence of decoherence, and for high-fidelity initialization and readout. We also discuss the progress in resonant optical control, which has led to interfaces between spin and photonic qubits and may lead to spin networks based on diamond photonics. Many of these recently developed diamond-based technologies constitute critical components for the future leap toward practical multiqubit devices. C1 [Dobrovitski, V. V.] Iowa State Univ, Ames Lab, Ames, IA 50011 USA. [Fuchs, G. D.] Cornell Univ, Sch Appl & Engn Phys, Ithaca, NY 14853 USA. [Falk, A. L.; Awschalom, D. D.] Univ Calif Santa Barbara, Ctr Spintron & Quantum Computat, Santa Barbara, CA 93106 USA. [Santori, C.] Hewlett Packard Labs, Palo Alto, CA 94304 USA. RP Dobrovitski, VV (reprint author), Iowa State Univ, Ames Lab, Ames, IA 50011 USA. EM awsch@physics.ucsb.edu NR 169 TC 43 Z9 43 U1 8 U2 113 PU ANNUAL REVIEWS PI PALO ALTO PA 4139 EL CAMINO WAY, PO BOX 10139, PALO ALTO, CA 94303-0897 USA SN 1947-5454 BN 978-0-8243-5004-8 J9 ANNU REV CONDEN MA P JI Annu. Rev. Condens. Matter Phys. PY 2013 VL 4 BP 23 EP 50 DI 10.1146/annurev-conmatphys-030212-184238 PG 28 WC Physics, Condensed Matter SC Physics GA BFW64 UT WOS:000321694300003 ER PT S AU Maiti, A AF Maiti, Amitesh BE Fitzgerald, G Govind, N TI Ionic Liquids for Carbon Capture: Solubility Computation Using an Implicit Solvent Model SO APPLICATIONS OF MOLECULAR MODELING TO CHALLENGES IN CLEAN ENERGY SE ACS Symposium Series LA English DT Proceedings Paper CT Symposium on Applications of Computational Methods to Environmentally Sustainable Solutions at ACS National Spring Meeting CY MAR 25-29, 2012 CL San Diego, CA SP ACS, Div Comp Chem ID PRESSURE PHASE-BEHAVIOR; COSMO-RS; CO2 CAPTURE; BASIS-SETS; DIOXIDE; PREDICTION; SELECTIVITY; SYSTEMS; ENERGY; GAS AB Through a large number of solubility measurements over the last decade and a half, Ionic Liquids (ILs) have been demonstrated as a great medium for the physical dissolution of CO2. However, there are numerous possible variations on the component ions of an IL, only a small fraction of which has actually been synthesized so far. In order to screen for the best solvents it is necessary to adopt a theoretical approach that can quickly compute the CO2 solubility with reasonable quantitative accuracy. Here we report a theoretical prescription that involves computing the chemical potential of CO2 in the solvent phase with a density-functional-theory-based implicit solvation code (COSMO-RS) and computing the gas fugacity with a cubic equation of state. The approach yields excellent agreement with a large volume of experimental data on CO2 solubility in diverse classes of ILs over a wide range of temperatures and pressures. The resulting quantitative trends can be used to discover solvents with much higher CO2 uptake per kg of solvent than has been experimentally achieved so far. C1 Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. RP Maiti, A (reprint author), Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. EM amaiti@llnl.gov NR 46 TC 0 Z9 0 U1 1 U2 11 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 SIXTEENTH ST NW, WASHINGTON, DC 20036 USA SN 0097-6156 BN 978-0-8412-2820-7 J9 ACS SYM SER JI ACS Symp. Ser. PY 2013 VL 1133 BP 19 EP 30 PG 12 WC Chemistry, Multidisciplinary; Computer Science, Interdisciplinary Applications; Energy & Fuels SC Chemistry; Computer Science; Energy & Fuels GA BFX60 UT WOS:000321806600002 ER PT S AU Yoon, Y AF Yoon, Yeohoon BE Fitzgerald, G Govind, N TI Characterization of CO2 Behavior on Rutile TiO2 (110) Surface SO APPLICATIONS OF MOLECULAR MODELING TO CHALLENGES IN CLEAN ENERGY SE ACS Symposium Series LA English DT Proceedings Paper CT Symposium on Applications of Computational Methods to Environmentally Sustainable Solutions at ACS National Spring Meeting CY MAR 25-29, 2012 CL San Diego, CA SP ACS, Div Comp Chem ID CARBON-DIOXIDE; MOLECULAR-DYNAMICS; TIO2(110) SURFACE; CHEMISTRY; DIFFUSION AB The dynamic behavior of carbon dioxide (CO2) adsorbed on the rutile TiO2 (110) surface is studied by dispersion corrected density functional theory (DFT) and combined ab initio molecular dynamics (AIMD) simulation. Understanding the behavior of CO2 is important regarding possible applications for treating CO2 in current environmental problems along with the consideration as a renewable energy source. Concerning the ability as a reducible support of TiO2 surface, a fundamental understanding of the interaction between CO2 and TiO2 surface will help extending the possible applications. In the current study, CO2 interaction and dynamic behavior on the TiO2 surface is characterized including the effect of the oxygen vacancy (O-v) defect. Also the coverage dependence of CO2 behavior is investigated since more contribution of the intermolecular interaction among CO2 molecules can be expected as the coverage increasing. C1 Pacific NW Natl Lab, Fundamental & Computat Sci Directorate, Richland, WA 99352 USA. RP Yoon, Y (reprint author), Pacific NW Natl Lab, Fundamental & Computat Sci Directorate, Richland, WA 99352 USA. EM yeohoon.yoon@pnnl.gov RI Yoon, Yeohoon/D-4934-2014 NR 39 TC 0 Z9 0 U1 0 U2 5 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 SIXTEENTH ST NW, WASHINGTON, DC 20036 USA SN 0097-6156 BN 978-0-8412-2820-7 J9 ACS SYM SER JI ACS Symp. Ser. PY 2013 VL 1133 BP 51 EP 66 PG 16 WC Chemistry, Multidisciplinary; Computer Science, Interdisciplinary Applications; Energy & Fuels SC Chemistry; Computer Science; Energy & Fuels GA BFX60 UT WOS:000321806600004 ER PT S AU Ho, MH Chen, ST Rousseau, R Dupuis, M Bullock, RM Raugei, S AF Ho, Ming-Hsun Chen, Shentan Rousseau, Roger Dupuis, Michel Bullock, R. Morris Raugei, Simone BE Fitzgerald, G Govind, N TI Bio-Inspired Molecular Catalysts for Hydrogen Oxidation and Hydrogen Production SO APPLICATIONS OF MOLECULAR MODELING TO CHALLENGES IN CLEAN ENERGY SE ACS Symposium Series LA English DT Proceedings Paper CT Symposium on Applications of Computational Methods to Environmentally Sustainable Solutions at ACS National Spring Meeting CY MAR 25-29, 2012 CL San Diego, CA SP ACS, Div Comp Chem ID OUTER-COORDINATION SPHERE; PENDANT NITROGEN BASES; FRUSTRATED LEWIS PAIRS; H-2 PRODUCTION; IRON HYDROGENASE; CORRELATION-ENERGY; ACTIVE-SITE; ELECTRON-TRANSFER; COMPLEXES; DENSITY AB Recent advances in Ni-based bio-inspired catalysts obtained in the Center for Molecular Electrocatalysis, an Energy Frontier Research Center (EFRC) led by the Pacific Northwest National Laboratory, demonstrated the possibility of cleaving H-2 or generating H-2 heterolytically with turnover frequencies comparable or superior to those of hydrogenase enzymes. In these catalysts the transformation between H-2 and protons proceeds via an interplay between proton, hydride and electron transfer steps, and involves the interaction of a dihydrogen molecule with both a Ni(II) center and pendent amine bases incorporated in six-membered rings, which function as proton relays. These catalytic platforms are well designed in that when protons are correctly positioned (endo) toward the metal center, catalysis proceeds at very high rates. We show here that the proton removal from the molecular catalysts (for H-2 oxidation) and proton delivery to the molecular catalysts (for H-2 production) are often the rate-determining steps. Furthermore, the presence of multiple protonation sites gives rise to reaction intermediates with protons incorrectly positioned (exo relative to the metal center). These isomers are kinetically easily accessible and are detrimental to catalysis because the isomerization processes necessary to convert them to the catalytically competent endo isomers are slow. In this chapter we give an overview of the major findings of our computational investigation of proton relays for H-2 chemistry and provide guidelines for the design of catalysts with enhanced activity. C1 [Ho, Ming-Hsun; Chen, Shentan; Rousseau, Roger; Dupuis, Michel; Bullock, R. Morris; Raugei, Simone] Pacific NW Natl Lab, Ctr Mol Electrocatalysis, Richland, WA 99352 USA. RP Ho, MH (reprint author), Pacific NW Natl Lab, Ctr Mol Electrocatalysis, POB 999,K1-83, Richland, WA 99352 USA. EM simone.raugei@pnl.gov RI Rousseau, Roger/C-3703-2014; Bullock, R. Morris/L-6802-2016 OI Bullock, R. Morris/0000-0001-6306-4851 NR 74 TC 6 Z9 6 U1 0 U2 14 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 SIXTEENTH ST NW, WASHINGTON, DC 20036 USA SN 0097-6156 BN 978-0-8412-2820-7 J9 ACS SYM SER JI ACS Symp. Ser. PY 2013 VL 1133 BP 89 EP 111 PG 23 WC Chemistry, Multidisciplinary; Computer Science, Interdisciplinary Applications; Energy & Fuels SC Chemistry; Computer Science; Energy & Fuels GA BFX60 UT WOS:000321806600006 ER PT S AU Ferguson, G Curtiss, LA AF Ferguson, Glen Curtiss, Larry A. BE Fitzgerald, G Govind, N TI Atomic-Level Modeling of Organic Electrolytes in Lithium-Ion Batteries SO APPLICATIONS OF MOLECULAR MODELING TO CHALLENGES IN CLEAN ENERGY SE ACS Symposium Series LA English DT Proceedings Paper CT Symposium on Applications of Computational Methods to Environmentally Sustainable Solutions at ACS National Spring Meeting CY MAR 25-29, 2012 CL San Diego, CA SP ACS, Div Comp Chem ID DENSITY-FUNCTIONAL THEORY; UNDERSTAND SURFACE-CHEMISTRY; MOLECULAR-DYNAMICS; ETHYLENE CARBONATE; GENETIC ALGORITHM; PROPYLENE CARBONATE; REDUCTIVE DECOMPOSITIONS; GEOMETRY OPTIMIZATION; POLYMER ELECTROLYTES; VINYLENE CARBONATE AB Lithium-ion (Li-ion) batteries are a widely used and important technology. Recent expansion of Li-ion batteries into automotive applications has resulted in intense scientific interest. In Li-ion batteries the multitude of reactions occurring under harsh conditions along with difficulties in characterization have made calculations and simulations an important part of this research. Application of atomic level methods has expanded the knowledge concerning the basic chemistry of the Li-ion battery, especially as applied to electrolytes and their relationship to the solid electrolyte interphase (SET), a key component of many Li-ion batteries. In this chapter we review methods for atomic-level computations and simulations of Li-ion battery electrolytes with a focus on the chemistry of the organic solvents of the electrolyte. Each section includes a short overview of computational methodology and some applications, followed by a highlight of recent work. The first section describes how quantum chemical methods can be used to interrogate problems in Li-ion batteries. The highlighted work in this section is a study of the reactions of organic solvent on model systems to form an oligomeric SEI layer. In the next section the use of classical and ab initio molecular dynamics to simulate reactions in the SEI layer is reviewed and two studies are highlighted. The final method is the use of data from ab initio calculations to screen electrolytes for improved reactivity. The chapter closes with a section on the future outlook of atomic-level modeling of Li-ion electrolytes. C1 [Ferguson, Glen; Curtiss, Larry A.] Argonne Natl Lab, Div Mat Sci, Argonne, IL 60439 USA. RP Ferguson, G (reprint author), Argonne Natl Lab, Div Mat Sci, 9700 S Cass Ave, Argonne, IL 60439 USA. EM gferguson@anl.gov NR 105 TC 4 Z9 4 U1 3 U2 25 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 SIXTEENTH ST NW, WASHINGTON, DC 20036 USA SN 0097-6156 BN 978-0-8412-2820-7 J9 ACS SYM SER JI ACS Symp. Ser. PY 2013 VL 1133 BP 217 EP 233 PG 17 WC Chemistry, Multidisciplinary; Computer Science, Interdisciplinary Applications; Energy & Fuels SC Chemistry; Computer Science; Energy & Fuels GA BFX60 UT WOS:000321806600012 ER PT J AU Wang, D Jia, W Olsen, SC Wuebbles, DJ Dubey, MK Rockett, AA AF Wang, D. Jia, W. Olsen, S. C. Wuebbles, D. J. Dubey, M. K. Rockett, A. A. TI Impact of a future H-2-based road transportation sector on the composition and chemistry of the atmosphere - Part 1: Tropospheric composition and air quality SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID CMAQ MODELING SYSTEM; HYDROGEN ECONOMY; MOLECULAR-HYDROGEN; CARBON-MONOXIDE; VERSION 4.5; H-2; EMISSIONS; CLIMATE; OZONE; SOIL AB Vehicles burning fossil fuel emit a number of substances that change the composition and chemistry of the atmosphere, and contribute to global air and water pollution and climate change. For example, nitrogen oxides and volatile organic compounds (VOCs) emitted as byproducts of fossil fuel combustion are key precursors to ground-level ozone and aerosol formation. In addition, on-road vehicles are major CO2 emitters. In order to tackle these problems, molecular hydrogen (H-2) has been proposed as an energy carrier to substitute for fossil fuels in the future. However, before implementing any such strategy it is crucial to evaluate its potential impacts on air quality and climate. Here, we evaluate the impact of a future (2050) H-2-based road transportation sector on tropospheric chemistry and air quality for several possible growth and technology adoption scenarios. The growth scenarios are based on the high and low emissions Intergovernmental Panel on Climate Change Special Report on Emissions Scenarios, A1FI and B1, respectively. The technological adoption scenarios include H-2 fuel cell and H-2 internal combustion engine options. The impacts are evaluated with the Community Atmospheric Model Chemistry global chemistry transport model (CAM-Chem). Higher resolution simulations focusing on the contiguous United States are also carried out with the Community Multiscale Air Quality Modeling System (CMAQ) regional chemistry transport model. For all scenarios future air quality improves with the adoption of a H-2-based road transportation sector; however, the magnitude and type of improvement depend on the scenario. Model results show that the adoption of H-2 fuel cells would decrease tropospheric burdens of ozone (7%), CO (14%), NOx (16%), soot (17%), sulfate aerosol (4%), and ammonium nitrate aerosol (12%) in the A1FI scenario, and would decrease those of ozone (5%), CO (4%), NOx (11%), soot (7%), sulfate aerosol (4%), and ammonium nitrate aerosol (9%) in the B1 scenario. The adoption of H-2 internal combustion engines would decrease tropospheric burdens of ozone (1%), CO (18%), soot (17%), and sulfate aerosol (3%) in the A1FI scenario, and would decrease those of ozone (1%), CO (7%), soot (7%), and sulfate aerosol (3%) in the B1 scenario. In the future, people residing in the contiguous United States could expect to experience significantly fewer days of elevated levels of pollution if a H-2 fuel cell road transportation sector were to be adopted. Health benefits of transitioning to a H-2 economy for citizens in developing nations, like China and India, will be much more dramatic, particularly in megacities with severe, intensifying air-quality problems. C1 [Wang, D.; Jia, W.; Olsen, S. C.; Wuebbles, D. J.] Univ Illinois, Dept Atmospher Sci, Urbana, IL USA. [Dubey, M. K.] Los Alamos Natl Lab, Los Alamos, NM USA. [Rockett, A. A.] Univ Illinois, Dept Mat Sci & Engn, Urbana, IL USA. RP Wuebbles, DJ (reprint author), Univ Illinois, Dept Atmospher Sci, Urbana, IL USA. EM wuebbles@atmos.uiuc.edu RI Dubey, Manvendra/E-3949-2010; Rockett, Angus/B-5539-2013 OI Dubey, Manvendra/0000-0002-3492-790X; Rockett, Angus/0000-0001-9759-8421 FU United States Department of Energy [DE-FC36-07GO17109] FX The authors thank Hugh Pitcher for providing projections of energy efficiency. Funding for this study was provided by the United States Department of Energy through award number DE-FC36-07GO17109 to the University of Illinois project "Evaluation of the Potential Environmental Impacts from Large-Scale Use and Production of Hydrogen in Energy and Transportation Applications". MKD thanks Los Alamos National Laboratory's LDRD and IGPP for nurturing this research. NR 49 TC 4 Z9 4 U1 3 U2 19 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 13 BP 6117 EP 6137 DI 10.5194/acp-13-6117-2013 PG 21 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA 182TL UT WOS:000321767200001 ER PT J AU Wang, D Jia, W Olsen, SC Wuebbles, DJ Dubey, MK Rockett, AA AF Wang, D. Jia, W. Olsen, S. C. Wuebbles, D. J. Dubey, M. K. Rockett, A. A. TI Impact of a future H-2-based road transportation sector on the composition and chemistry of the atmosphere - Part 2: Stratospheric ozone SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID HYDROGEN ECONOMY; NITROGEN-OXIDES; MODEL; TROPOSPHERE; METHANE; CLIMATE; O-3 AB The prospective future adoption of molecular hydrogen (H-2) to power the road transportation sector could greatly improve tropospheric air quality but also raises the question of whether the adoption would have adverse effects on the stratospheric ozone. The possibility of undesirable impacts must be fully evaluated to guide future policy decisions. Here we evaluate the possible impact of a future (2050) H-2-based road transportation sector on stratospheric composition and chemistry, especially on the stratospheric ozone, with the MOZART (Model for OZone And Related chemical Tracers) model. Since future growth is highly uncertain, we evaluate the impact of two world evolution scenarios, one based on an IPCC (Intergovernmental Panel on Climate Change) high-emitting scenario (A1FI) and the other on an IPCC low-emitting scenario (B1), as well as two technological options: H-2 fuel cells and H-2 internal combustion engines. We assume a H-2 leakage rate of 2.5% and a complete market penetration of H-2 vehicles in 2050. The model simulations show that a H-2-based road transportation sector would reduce stratospheric ozone concentrations as a result of perturbed catalytic ozone destruction cycles. The magnitude of the impact depends on which growth scenario evolves and which H-2 technology option is applied. For the evolution growth scenario, stratospheric ozone decreases more in the H-2 fuel cell scenarios than in the H-2 internal combustion engine scenarios because of the NOx emissions in the latter case. If the same technological option is applied, the impact is larger in the A1FI emission scenario. The largest impact, a 0.54% decrease in annual average global mean stratospheric column ozone, is found with a H-2 fuel cell type road transportation sector in the A1FI scenario; whereas the smallest impact, a 0.04% increase in stratospheric ozone, is found with applications of H-2 internal combustion engine vehicles in the B1 scenario. The impacts of the other two scenarios fall between the above two boundary scenarios. However, the magnitude of these changes is much smaller than the increases in 2050 stratospheric ozone projected, as stratospheric ozone is expected to recover due to the limits in ozone depleting substance emissions imposed in the Montreal Protocol. C1 [Wang, D.; Jia, W.; Olsen, S. C.; Wuebbles, D. J.] Univ Illinois, Dept Atmospher Sci, Urbana, IL USA. [Dubey, M. K.] Los Alamos Natl Lab, Los Alamos, NM USA. [Rockett, A. A.] Univ Illinois, Dept Mat Sci & Engn, Urbana, IL USA. RP Wuebbles, DJ (reprint author), Univ Illinois, Dept Atmospher Sci, Urbana, IL USA. EM wuebbles@atmos.uiuc.edu RI Dubey, Manvendra/E-3949-2010; Rockett, Angus/B-5539-2013 OI Dubey, Manvendra/0000-0002-3492-790X; Rockett, Angus/0000-0001-9759-8421 FU United States Department of Energy [DE-FC36-07GO17109]; LANL's IGPP program FX The authors thank Hugh Pitcher for providing projections of energy efficiency. Funding for this study was provided by the United States Department of Energy through award number DE-FC36-07GO17109 to the University of Illinois project "Evaluation of the Potential Environmental Impacts from Large-Scale Use and Production of Hydrogen in Energy and Transportation Applications". MKD would like to thank LANL's IGPP program for support. NR 26 TC 1 Z9 1 U1 0 U2 10 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1680-7316 J9 ATMOS CHEM PHYS JI Atmos. Chem. Phys. PY 2013 VL 13 IS 13 BP 6139 EP 6150 DI 10.5194/acp-13-6139-2013 PG 12 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA 182TL UT WOS:000321767200002 ER PT J AU Huang, Y Wu, S Dubey, MK French, NHF AF Huang, Y. Wu, S. Dubey, M. K. French, N. H. F. TI Impact of aging mechanism on model simulated carbonaceous aerosols SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID GENERAL-CIRCULATION MODEL; ORGANIC AEROSOL; BLACK CARBON; ELEMENTAL CARBON; TRANSPORT; UNCERTAINTIES; DEPOSITION; PARTICLES; CHEMISTRY; EMISSIONS AB Carbonaceous aerosols including organic carbon and black carbon have significant implications for both climate and air quality. In the current global climate or chemical transport models, a fixed hydrophobic-to-hydrophilic conversion lifetime for carbonaceous aerosol (tau) is generally assumed, which is usually around one day. We have implemented a new detailed aging scheme for carbonaceous aerosols in a chemical transport model (GEOS-Chem) to account for both the chemical oxidation and the physical condensation-coagulation effects, where tau is affected by local atmospheric environment including atmospheric concentrations of water vapor, ozone, hydroxyl radical and sulfuric acid. The updated tau exhibits large spatial and temporal variations with the global average (up to 11 km altitude) calculated to be 2.6 days. The chemical aging effects are found to be strongest over the tropical regions driven by the low ozone concentrations and high humidity there. The tau resulted from chemical aging generally decreases with altitude due to increases in ozone concentration and decreases in humidity. The condensation-coagulation effects are found to be most important for the high-latitude areas, in particular the polar regions, where the tau values are calculated to be up to 15 days. When both the chemical aging and condensation-coagulation effects are considered, the total atmospheric burdens and global average lifetimes of BC, black carbon, (OC, organic carbon) are calculated to increase by 9% (3 %) compared to the control simulation, with considerable enhancements of BC and OC concentrations in the Southern Hemisphere. Model evaluations against data from multiple datasets show that the updated aging scheme improves model simulations of carbonaceous aerosols for some regions, especially for the remote areas in the Northern Hemisphere. The improvement helps explain the persistent low model bias for carbonaceous aerosols in the Northern Hemisphere reported in literature. Further model sensitivity simulations focusing on the continental outflow of carbonaceous aerosols demonstrate that previous studies using the old aging scheme could have significantly underestimated the intercontinental transport of carbonaceous aerosols. C1 [Huang, Y.] Michigan Technol Univ, Dept Geol & Min Engn & Sci, Houghton, MI 49931 USA. [Wu, S.] Michigan Technol Univ, Dept Geol & Min Engn & Sci, Dept Civil & Environm Engn, Atmospher Sci Program, Houghton, MI 49931 USA. [Dubey, M. K.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [French, N. H. F.] Michigan Technol Univ, Michigan Tech Res Inst, Ann Arbor, MI 48105 USA. RP Wu, S (reprint author), Michigan Technol Univ, Dept Geol & Min Engn & Sci, Dept Civil & Environm Engn, Atmospher Sci Program, Houghton, MI 49931 USA. EM slwu@mtu.edu RI Dubey, Manvendra/E-3949-2010; Chem, GEOS/C-5595-2014; OI Dubey, Manvendra/0000-0002-3492-790X; French, Nancy/0000-0002-2389-3003 FU US EPA [R83428601]; NIH [1 RC1 ES018612] FX This work was supported by US EPA (grant # R83428601) and NIH (grant #1 RC1 ES018612). We thank Robert Page at Michigan Tech for his help on programming. We would like to thank people contributing to the multiple datasets including ACE-Asia, HIPPO1, IMPROVE, EMEP, and CAWNET. We thank Joshua Schwarz for help on the HIPPO1 data. We thank the Editor and two anonymous reviewers for their helpful comments. NR 54 TC 14 Z9 14 U1 0 U2 21 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1680-7316 EI 1680-7324 J9 ATMOS CHEM PHYS JI Atmos. Chem. Phys. PY 2013 VL 13 IS 13 BP 6329 EP 6343 DI 10.5194/acp-13-6329-2013 PG 15 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA 182TL UT WOS:000321767200013 ER PT J AU Wang, J McGraw, RL Kuang, C AF Wang, J. McGraw, R. L. Kuang, C. TI Growth of atmospheric nano-particles by heterogeneous nucleation of organic vapor SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID AEROSOL FORMATION; BOREAL FOREST; INITIAL STEPS; SULFURIC-ACID; NUCLEI; RATES; CONDENSATION; EVENTS; CRITERION; POLLUTION AB Atmospheric aerosols play critical roles in air quality, public health, and visibility. In addition, they strongly influence climate by scattering solar radiation and by changing the reflectivity and lifetime of clouds. One major but still poorly understood source of atmospheric aerosols is new particle formation, which consists of the formation of thermodynamically stable clusters from trace gas molecules (homogeneous nucleation) followed by growth of these clusters to a detectable size (similar to 3 nm). Because freshly nucleated clusters are most susceptible to loss due to high rate of coagulation with pre-existing aerosol population, the initial growth rate strongly influences the rate of new particle formation and ambient aerosol population. Whereas many field observations and modeling studies indicate that organics enhance the initial growth of the clusters and therefore new particle formation, thermodynamic considerations would suggest that the strong increase of equilibrium vapor concentration due to cluster surface curvature (Kelvin effect) may prevent ambient organics from condensing on these small clusters. Here, the contribution of organics to the initial cluster growth is described as heterogeneous nucleation of organic molecules onto these clusters. We find that the strong gradient in cluster population with respect to its size leads to positive cluster number flux. This positive flux drives the growth of clusters substantially smaller than the Kelvin diameter, conventionally considered the minimum particle size that can be grown through condensation. The conventional approach neglects the contribution from the cluster concentration gradient, and underestimates the cluster survival probabilities by a factor of up to 60 if early growth of clusters is due to both condensation of sulfuric acid and heterogeneous nucleation of organic vapors. C1 [Wang, J.; McGraw, R. L.; Kuang, C.] Brookhaven Natl Lab, Div Atmospher Sci, Upton, NY 11973 USA. RP Wang, J (reprint author), Brookhaven Natl Lab, Div Atmospher Sci, Upton, NY 11973 USA. EM jian@bnl.gov RI Wang, Jian/G-9344-2011; Kuang, Chongai/E-4446-2013 FU U.S. Department of Energy's Atmospheric Science Program (Office of Science, OBER) [DE-AC02-98CH10886] FX This work was supported by the U.S. Department of Energy's Atmospheric Science Program (Office of Science, OBER) under contract DE-AC02-98CH10886. NR 49 TC 6 Z9 6 U1 0 U2 32 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1680-7316 J9 ATMOS CHEM PHYS JI Atmos. Chem. Phys. PY 2013 VL 13 IS 13 BP 6523 EP 6531 DI 10.5194/acp-13-6523-2013 PG 9 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA 182TL UT WOS:000321767200027 ER PT J AU Lee, YH Lamarque, JF Flanner, MG Jiao, C Shindell, DT Berntsen, T Bisiaux, MM Cao, J Collins, WJ Curran, M Edwards, R Faluvegi, G Ghan, S Horowitz, LW McConnell, JR Ming, J Myhre, G Nagashima, T Naik, V Rumbold, ST Skeie, RB Sudo, K Takemura, T Thevenon, F Xu, B Yoon, JH AF Lee, Y. H. Lamarque, J. -F. Flanner, M. G. Jiao, C. Shindell, D. T. Berntsen, T. Bisiaux, M. M. Cao, J. Collins, W. J. Curran, M. Edwards, R. Faluvegi, G. Ghan, S. Horowitz, L. W. McConnell, J. R. Ming, J. Myhre, G. Nagashima, T. Naik, V. Rumbold, S. T. Skeie, R. B. Sudo, K. Takemura, T. Thevenon, F. Xu, B. Yoon, J-H TI Evaluation of preindustrial to present-day black carbon and its albedo forcing from Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) (vol 13, pg 2607, 2013) SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Correction C1 [Lee, Y. H.; Shindell, D. T.; Faluvegi, G.] NASA, Goddard Inst Space Studies, New York, NY 10025 USA. [Lee, Y. H.; Shindell, D. T.; Faluvegi, G.] Columbia Earth Inst, New York, NY USA. [Lamarque, J. -F.] Natl Ctr Atmospher Res NCAR, Boulder, CO USA. [Flanner, M. G.; Jiao, C.] Univ Michigan, Dept Atmospher Ocean & Space Sci, Ann Arbor, MI 48109 USA. [Berntsen, T.] Univ Oslo, CICERO, Oslo, Norway. [Berntsen, T.] Univ Oslo, Dept Geosci, Oslo, Norway. [Bisiaux, M. M.; McConnell, J. R.] Nevada Syst Higher Educ, Desert Res Inst, Reno, NV USA. [Cao, J.] Chinese Acad Sci, Inst Earth Environm, State Key Lab Loess & Quaternary Geol, Xian, Peoples R China. [Collins, W. J.; Rumbold, S. T.] Hadley Ctr, Met Off, Exeter, Devon, England. [Edwards, R.] Curtin Univ, Dept Imaging & Appl Phys, Bentley, WA, Australia. [Ghan, S.; Yoon, J-H] Pacific NW Natl Lab, Richland, WA 99352 USA. [Horowitz, L. W.] NOAA, Geophys Fluid Dynam Lab, Princeton, NJ USA. [Ming, J.] China Meteorol Adm, Natl Climate Ctr, Beijing, Peoples R China. [Myhre, G.] CICERO, Oslo, Norway. [Nagashima, T.; Skeie, R. B.] Natl Inst Environm Studies, Tsukuba, Ibaraki, Japan. [Naik, V.] NOAA, UCAR, Geophys Fluid Dynam Lab, Princeton, NJ USA. [Sudo, K.] Nagoya Univ, Grad Sch Environm Studies, Dept Earth & Environm Sci, Nagoya, Aichi 4648601, Japan. [Takemura, T.] Kyushu Univ, Res Inst Appl Mech, Fukuoka 812, Japan. [Thevenon, F.] Univ Geneva, FA Forel Inst, Versoix, Switzerland. [Xu, B.] Chinese Acad Sci, Inst Tibetan Plateau Res, Key Lab Tibetan Environm Changes & Land Surface P, Beijing, Peoples R China. RP Lee, YH (reprint author), NASA, Goddard Inst Space Studies, New York, NY 10025 USA. EM yunha.lee@nasa.gov RI Shindell, Drew/D-4636-2012; Horowitz, Larry/D-8048-2014; Ghan, Steven/H-4301-2011; Edwards, Ross/B-1433-2013; Lee, Yunha/Q-7222-2016; Cao, Junji/D-3259-2014; Naik, Vaishali/A-4938-2013; Lamarque, Jean-Francois/L-2313-2014; Kyushu, RIAM/F-4018-2015; Myhre, Gunnar/A-3598-2008; U-ID, Kyushu/C-5291-2016 OI Horowitz, Larry/0000-0002-5886-3314; Ghan, Steven/0000-0001-8355-8699; Edwards, Ross/0000-0002-9233-8775; Lee, Yunha/0000-0001-7478-2672; Cao, Junji/0000-0003-1000-7241; Naik, Vaishali/0000-0002-2254-1700; Lamarque, Jean-Francois/0000-0002-4225-5074; Myhre, Gunnar/0000-0002-4309-476X; NR 1 TC 1 Z9 1 U1 0 U2 19 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1680-7316 J9 ATMOS CHEM PHYS JI Atmos. Chem. Phys. PY 2013 VL 13 IS 13 BP 6553 EP 6554 DI 10.5194/acp-13-6553-2013 PG 2 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA 182TL UT WOS:000321767200029 ER PT J AU Wang, JJ Chen-Wiegart, YCK Wang, J AF Wang, Jiajun Chen-Wiegart, Yu-chen Karen Wang, Jun TI In situ chemical mapping of a lithium-ion battery using full-field hard X-ray spectroscopic imaging SO CHEMICAL COMMUNICATIONS LA English DT Article ID NANO-TOMOGRAPHY; MICROSCOPY; LITHIATION AB In situ tracking of chemical phase transformation, mapping, and composition information of a battery with CuO as the anode was performed with quantitative analysis at sub-30 nm resolution with a 40 x 40 mu m field of view using transmission X-ray microscopy combined with spectroscopy. A size-dependent and core-shell lithiation-delithiation mechanism was suggested for the electrochemical reaction. C1 [Wang, Jiajun; Chen-Wiegart, Yu-chen Karen; Wang, Jun] Brookhaven Natl Lab, Photon Sci Directorate, Upton, NY 11973 USA. RP Wang, J (reprint author), Brookhaven Natl Lab, Photon Sci Directorate, 75 Brookhaven Ave Bldg 725D, Upton, NY 11973 USA. EM junwang@bnl.gov RI wang, jiajun/H-3315-2012; wang, jiajun/H-5683-2016 FU U.S. Department of Energy, Office of Basic Energy Sciences [DE-AC02-98CH10886] FX This work was performed at NSLS and the Center for Functional Nanomaterials, BNL, which is supported by the U.S. Department of Energy, Office of Basic Energy Sciences under Contract No. DE-AC02-98CH10886. We also acknowledge Drs Jianming Bai and Dong Su for XRD and TEM measurements. NR 13 TC 39 Z9 39 U1 1 U2 56 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1359-7345 EI 1364-548X J9 CHEM COMMUN JI Chem. Commun. PY 2013 VL 49 IS 58 BP 6480 EP 6482 DI 10.1039/c3cc42667j PG 3 WC Chemistry, Multidisciplinary SC Chemistry GA 170VT UT WOS:000320883500003 PM 23685635 ER PT J AU Collins, MS Carnes, ME Sather, AC Berryman, OB Zakharov, LN Teat, SJ Johnson, DW AF Collins, Mary S. Carnes, Matthew E. Sather, Aaron C. Berryman, Orion B. Zakharov, Lev N. Teat, Simon J. Johnson, Darren W. TI Pnictogen-directed synthesis of discrete disulfide macrocycles SO CHEMICAL COMMUNICATIONS LA English DT Article ID BIOLOGICAL RECOGNITION; AROMATIC RINGS; IODINE AB Cyclic disulfide macrocycles were rapidly synthesized cleanly and selectively from rigid dithiols via oxidation with iodine when activated by pnictogen additives (As and Sb). Macrocycles were confirmed by H-1-NMR spectroscopy and X-ray crystallography. A p-xylyl-based disulfide trimer and tetramer crystallized in hollow, stacked columns stabilized by intermolecular, sulfur center dot center dot center dot sulfur close contacts. C1 [Collins, Mary S.; Carnes, Matthew E.; Sather, Aaron C.; Berryman, Orion B.; Johnson, Darren W.] Univ Oregon, Eugene, OR 97403 USA. [Collins, Mary S.; Carnes, Matthew E.; Sather, Aaron C.; Berryman, Orion B.; Johnson, Darren W.] Univ Oregon, Inst Mat Sci, Eugene, OR 97403 USA. [Zakharov, Lev N.] Univ Oregon, CAMCOR Ctr Adv Mat Characterizat Oregon, Eugene, OR 97403 USA. [Teat, Simon J.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Johnson, DW (reprint author), Univ Oregon, Eugene, OR 97403 USA. EM dwj@uoregon.edu FU University of Oregon; Research Corporation for Science Advancement [20317]; Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231] FX The authors thank the University of Oregon for partial support of this work. D.W.J. is a Scialog Fellow of Research Corporation for Science Advancement (Award ID 20317). The Advanced Light Source is supported by the Director, Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. NR 20 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 59 BP 6599 EP 6601 DI 10.1039/c3cc43524e PG 3 WC Chemistry, Multidisciplinary SC Chemistry GA 172OE UT WOS:000321012900007 PM 23770675 ER PT J AU Plonka, AM Banerjee, D Woerner, WR Zhang, ZJ Li, J Parise, JB AF Plonka, Anna M. Banerjee, Debasis Woerner, William R. Zhang, Zhijuan Li, Jing Parise, John B. TI Effect of ligand geometry on selective gas-adsorption: the case of a microporous cadmium metal organic framework with a V-shaped linker SO CHEMICAL COMMUNICATIONS LA English DT Article ID CARBON-DIOXIDE CAPTURE; ZEOLITIC IMIDAZOLATE FRAMEWORKS; CO2 CAPTURE; COORDINATION POLYMERS; SWING ADSORPTION; SEPARATION; TEMPERATURE; CAPACITY; HYDROGEN; CO2/N-2 AB A microporous cadmium metal organic framework is synthesized and structurally characterized. The material possesses a 3-D framework with a 1-D sinusoidal chain and shows high selectivity for CO2 over N-2. The selectivity is attributed to CO2 interacting with two phenyl rings of a V-shaped linker as estimated by the in situ XRD-DSC study. C1 [Plonka, Anna M.; Woerner, William R.; Parise, John B.] SUNY Stony Brook, Dept Geosci, Stony Brook, NY 11794 USA. [Banerjee, Debasis; Zhang, Zhijuan; Li, Jing] Rutgers State Univ, Dept Chem & Chem Biol, Piscataway, NJ 08854 USA. [Parise, John B.] Brookhaven Natl Lab, Photon Sci Div, Upton, NY 11973 USA. RP Li, J (reprint author), Rutgers State Univ, Dept Chem & Chem Biol, 610 Taylor Rd, Piscataway, NJ 08854 USA. EM Jingli@rutgers.edu; john.parise@stonybrook.edu RI Banerjee, Debasis/B-2439-2008 FU U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-FG02-09ER46650, DE-AC02-06CH11357, DE-FG02-08ER46491]; National Science Foundation/Department of Energy [NSF/CHE-0822838] FX The synthesis, DSC-XRD characterization work and analysis of synchrotron data at Stony Brook is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under contract DE-FG02-09ER46650. The structure of 1 was determined in ChemMatCars (Sector 15), Advanced Photon Source (APS), principally supported by the National Science Foundation/Department of Energy (NSF/CHE-0822838). Use of APS was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under contract no. DE-AC02-06CH11357. The RU team acknowledges the partial support for the gas adsorption work and IAST calculations by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences through Grant DE-FG02-08ER46491. NR 31 TC 17 Z9 17 U1 1 U2 41 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1359-7345 J9 CHEM COMMUN JI Chem. Commun. PY 2013 VL 49 IS 63 BP 7055 EP 7057 DI 10.1039/c3cc43299h PG 3 WC Chemistry, Multidisciplinary SC Chemistry GA 182QH UT WOS:000321758300011 PM 23811783 ER PT J AU Whitehead, GFS Cross, B Carthy, L Milway, VA Rath, H Fernandez, A Heath, SL Muryn, CA Pritchard, RG Teat, SJ Timco, GA Winpenny, REP AF Whitehead, George F. S. Cross, Bryony Carthy, Laura Milway, Victoria A. Rath, Harapriya Fernandez, Antonio Heath, Sarah L. Muryn, Christopher A. Pritchard, Robin G. Teat, Simon J. Timco, Grigore A. Winpenny, Richard E. P. TI Rings and threads as linkers in metal-organic frameworks and poly-rotaxanes SO CHEMICAL COMMUNICATIONS LA English DT Article ID INORGANIC ROTAXANES AB Coordination polymers and metal-organic rotaxane frameworks are reported where the organic linker is replaced by functionalised inorganic clusters that act as bridging ligands. C1 [Whitehead, George F. S.; Cross, Bryony; Carthy, Laura; Milway, Victoria A.; Rath, Harapriya; Fernandez, Antonio; Heath, Sarah L.; Muryn, Christopher A.; Pritchard, Robin G.; Timco, Grigore A.; Winpenny, Richard E. P.] Univ Manchester, Sch Chem, Manchester M13 9PL, Lancs, England. [Whitehead, George F. S.; Cross, Bryony; Carthy, Laura; Milway, Victoria A.; Rath, Harapriya; Fernandez, Antonio; Heath, Sarah L.; Muryn, Christopher A.; Pritchard, Robin G.; Timco, Grigore A.; Winpenny, Richard E. P.] Univ Manchester, Photon Sci Inst, Manchester M13 9PL, Lancs, England. [Teat, Simon J.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. RP Winpenny, REP (reprint author), Univ Manchester, Sch Chem, Oxford Rd, Manchester M13 9PL, Lancs, England. EM richard.winpenny@manchester.ac.uk RI Whitehead, George/E-6639-2017 OI Whitehead, George/0000-0003-1949-4250 FU EPSRC (UK); European Commission; Royal Society (Newton Fellowship); Office of Science, Office of Basic Energy Sciences, of the US Department of Energy [DE-AC02-05CH11231]; Royal Society FX This research was funded by the EPSRC (UK) and the European Commission (Marie Curie Intra-European Fellowship to A.F.) and the Royal Society (Newton Fellowship to H.R.). The ALS is supported by the Director, Office of Science, Office of Basic Energy Sciences, of the US Department of Energy under contract no. DE-AC02-05CH11231. R.E.P.W. holds a Royal Society Wolfson Research Merit Award. NR 15 TC 18 Z9 18 U1 1 U2 41 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1359-7345 J9 CHEM COMMUN JI Chem. Commun. PY 2013 VL 49 IS 65 BP 7195 EP 7197 DI 10.1039/c3cc42300j PG 3 WC Chemistry, Multidisciplinary SC Chemistry GA 185GX UT WOS:000321956400003 PM 23788112 ER PT J AU Driscoll, PF Deunf, E Rubin, L Arnold, J Kerr, JB AF Driscoll, Peter F. Deunf, Elise Rubin, Leah Arnold, John Kerr, John B. TI Electrochemical Redox Catalysis for Electrochemical Dehydrogenation of Liquid Hydrogen Carrier Fuels for Energy Storage and Conversion SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID FERROCENE DERIVATIVES; OXIDATION; REDUCTION; HALIDES; LOHC AB The application of redox catalysis to the electrochemical dehydrogenation of organic molecules is of interest for a hybrid flow battery/fuel cell system for energy storage. The process of redox catalysis has been known and well studied theoretically and experimentally for several decades. Studies of redox catalysis can be instrumental in determining mechanistic aspects of electrochemical reactions and in measuring basic thermodynamic and kinetic parameters. Redox catalysis has the ability to reduce the overpotential of the dehydrogenation reaction used in such a system as well as to alter the course of the reaction to achieve higher efficiencies. The mechanism of catalysis can involve an ECE-type reaction or a CEE-type reaction. In either case the acid-base chemistry of the medium is critical. Preliminary results of catalytic current measurements as a function of redox catalyst, base concentration, and base strength are described along with possible reaction mechanisms. (C) 2013 The Electrochemical Society. All rights reserved. C1 [Driscoll, Peter F.; Deunf, Elise; Rubin, Leah; Arnold, John; Kerr, John B.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. [Deunf, Elise; Rubin, Leah; Arnold, John] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. RP Driscoll, PF (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. EM jbkerr@lbl.gov RI Arnold, John/F-3963-2012 OI Arnold, John/0000-0001-9671-227X FU Center for Electrocatalysis, Transport Phenomena, and Materials (CETM) for Innovative Energy Storage, an Energy Frontier Research Center (EFRC); U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC00001055]; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under DOE [DE-AC02-05CH11231] FX This material is based upon work supported as part of the Center for Electrocatalysis, Transport Phenomena, and Materials (CETM) for Innovative Energy Storage, 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-SC00001055 and under DOE Contract No DE-AC02-05CH11231. NR 25 TC 3 Z9 3 U1 1 U2 25 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 7 BP G3152 EP G3158 DI 10.1149/2.024307jes PG 7 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA 183DQ UT WOS:000321794600025 ER PT J AU Strack, G Babanova, S Farrington, KE Luckarift, HR Atanassov, P Johnson, GR AF Strack, Guinevere Babanova, Sofia Farrington, Karen E. Luckarift, Heather R. Atanassov, Plamen Johnson, Glenn R. TI Enzyme-Modified Buckypaper for Bioelectrocatalysis SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID DIRECT ELECTRON-TRANSFER; GLUCOSE-DEHYDROGENASE; CARBON ELECTRODES; CELL; BIOSENSORS AB Direct bioelectrocatalysis was demonstrated-with pyrroloquinoline quinone-dependent glucose dehydrogenase (PQQ-GDH) tethered to a range of carbon nanotube (CNT) materials, as evidenced by the generation of anodic current in the presence of glucose. Physical and electrochemical characterization of CNT paper (buckypaper) reveals marked differences attributed to changes in CNT dimensions, including conductivity, packing density, and electrochemically accessible surface area. By using single-walled CNTs as the electrode material, higher current densities per geometric area and lower electron transfer resistances were achieved. In comparison, electrodes made of oxidized CNTs enhanced in the physical adsorption of PQQ, but displayed voltage drops associated with activation losses. In addition, electrode longevity tests revealed that electrochemical activity was retained for two days but decreased by 50% on the third day. PQQ-GDH enzymatic electrodes show potential application as biological fuel cell anodes and will oxidize a range of mono- and disaccharide substrates. (C) 2013 The Electrochemical Society. C1 [Strack, Guinevere; Farrington, Karen E.; Luckarift, Heather R.; Johnson, Glenn R.] Air Force Res Lab, Airbase Technol Div, Tyndall AFB, FL 32403 USA. [Strack, Guinevere] Oak Ridge Inst Sci & Engn, Oak Ridge, TN 37831 USA. [Babanova, Sofia; Atanassov, Plamen] Univ New Mexico, Ctr Emerging Energy Technol, Albuquerque, NM 87131 USA. [Farrington, Karen E.; Luckarift, Heather R.] Univ Technol Corp, Dayton, OH 45432 USA. RP Strack, G (reprint author), Air Force Res Lab, Airbase Technol Div, Tyndall AFB, FL 32403 USA. EM glenn.johnson@i3-corps.com FU U.S. Department of Energy; Air Force Research Laboratory, Materials and Manufacturing Directorate, Airbase Technologies Division (AFRL/RXQ); NSF-CRET FX The authors acknowledge Buckeye Composites for manufacturing made-to-order BP and providing detailed characterization of the material. This research was supported in part by an appointment to the Postgraduate Research Participation Program at the Air Force Research Laboratory administered by the Oak Ridge Institute for Science and Education (ORISE) through an interagency agreement between the U.S. Department of Energy and the Air Force Research Laboratory, Materials and Manufacturing Directorate, Airbase Technologies Division (AFRL/RXQ). University of New Mexico work was supported by funding from the NSF-CRET Biosensing Program: Collaborative Research: Supramolecular Bio-Nano-Architectures as Biosensing Platforms. NR 25 TC 17 Z9 17 U1 3 U2 29 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 EI 1945-7111 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2013 VL 160 IS 7 BP G3178 EP G3182 DI 10.1149/2.028307jes PG 5 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA 183DQ UT WOS:000321794600029 ER PT S AU Nekoogar, F Dowla, F AF Nekoogar, Faranak Dowla, Farid BE Akopian, D Creutzburg, R Georgiev, TG Kennedy, LS Lumsdaine, A Matherson, KJ Sebe, N Snoek, CGM Wuller, D TI Location-Based Tracking Using Long Range Passive RFID and Ultra-wideband Communications SO MULTIMEDIA CONTENT AND MOBILE DEVICES SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Multimedia Content and Mobile Devices CY FEB 04-06, 2013 CL Burlingame, CA SP Soc Imaging Sci & Technol (IS&T), SPIE, Qualcomm Inc DE RF tracking; mobile platform; passive RFID; UWB; first responders; emergency response AB Reliable positioning capability is a crucial need for first responders in emergency and disaster situations. Lack of a dependable positioning system can result in disruptions in the situational awareness between the local responders in the field and the emergency command and control centers. Indoor localization and navigation poses many challenges for search and rescue teams (i.e. firefighters) such as inability to determine their exact location and communicate with the incident commander outside the building. Although RF navigation and tracking systems have many advantages over other technologies, the harsh indoor RF environment demands new ways of developing and using RF sensor and communication systems. A new approach, proposed recently [1-4], employs passive RFID for geo-location and tracking of a first responder. However, because conventional passive RFID tags have limited communications ranges, a very large number of these tags will be required to fully cover a large multi-storied building without any dead spots. Another technical challenge for conventional RF communications is the transmission of data from the mobile RFID platform (the tag reader) to the outside command and control node, as the buildings walls impose challenges such as attenuation and multipath. In this paper, we introduce a mobile platform architecture that makes optimal use of long-range passive tags, and takes advantage of the frequency diversity of Ultra-wideband (UWB) communication systems for a reliable, robust and yet low-cost infrastructure C1 [Nekoogar, Faranak; Dowla, Farid] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. RP Nekoogar, F (reprint author), Lawrence Livermore Natl Lab, 7000 East Ave L-183, Livermore, CA 94550 USA. NR 8 TC 0 Z9 0 U1 1 U2 9 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9440-5 J9 PROC SPIE PY 2013 VL 8667 AR 86670M DI 10.1117/12.2008706 PG 8 WC Engineering, Electrical & Electronic; Optics SC Engineering; Optics GA BFW66 UT WOS:000321695100019 ER PT J AU Moon, GH Shin, Y Choi, D Arey, BW Exarhos, GJ Wang, C Choi, W Liu, J AF Moon, Gun-hee Shin, Yongsoon Choi, Daiwon Arey, Bruce W. Exarhos, Gregory J. Wang, Chongmin Choi, Wonyong Liu, Jun TI Catalytic templating approaches for three-dimensional hollow carbon/graphene oxide nano-architectures SO NANOSCALE LA English DT Article ID REDUCED GRAPHENE OXIDE; HIGH-POWER SUPERCAPACITORS; CARBON NANOTUBES; HIGH-ENERGY; ELECTRODES; FILMS; PERFORMANCE; NANOSHEETS; REDUCTION; GRAPHITE AB We report a catalytic templating method to synthesize well-controlled three-dimensional carbon nano-architectures. Depending on graphene oxide content, the morphology can be systematically tuned from layered composites to 3D hollow structures to microporous materials. The composites with high surface area and high porosity induce a significant enhancement to its capacitance at high current density. C1 [Moon, Gun-hee; Shin, Yongsoon; Choi, Daiwon; Arey, Bruce W.; Exarhos, Gregory J.; Wang, Chongmin; Liu, Jun] Pacific NW Natl Lab, Div Chem & Mat Sci, Richland, WA 99354 USA. [Moon, Gun-hee; Choi, Wonyong] Pohang Univ Sci & Technol POSTECH, Dept Chem Engn, Pohang 790784, South Korea. RP Shin, Y (reprint author), Pacific NW Natl Lab, Div Chem & Mat Sci, 902 Battelle Blvd, Richland, WA 99354 USA. EM Yongsoon.shin@pnnl.gov; wchoi@postech.ac.kr; jun.liu@pnnl.gov RI Choi, Wonyong/F-8206-2010; Choi, Daiwon/B-6593-2008; Moon, Gun-hee/A-3279-2017 OI Choi, Wonyong/0000-0003-1801-9386; FU U.S. Department of Energy's (DOE) Office of Basic Energy Sciences, Division of Materials Sciences and Engineering; DOE's Office of Biological and Environmental Research; DOE [DE-AC05-76RL01830]; KOSEF NRL program; Korean government (MEST) [R0A-2008-000-20068-0]; KOSEF EPB Center [R11-2008-052-02002]; Fundamental R&D Program for Core Technology of Materials; Ministry of Knowledge Economy, South Korea FX This work was supported by the U.S. Department of Energy's (DOE) Office of Basic Energy Sciences, Division of Materials Sciences and Engineering. The research was performed using the William R. Wiley Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility sponsored by DOE's Office of Biological and Environmental Research and located at PNNL. PNNL is operated by Battelle for the DOE under Contract DE-AC05-76RL01830. This work also was supported by the KOSEF NRL program funded by the Korean government (MEST) (no. R0A-2008-000-20068-0); the KOSEF EPB Center (no. R11-2008-052-02002); and the Fundamental R&D Program for Core Technology of Materials funded by the Ministry of Knowledge Economy, South Korea. NR 52 TC 16 Z9 16 U1 1 U2 85 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 14 BP 6291 EP 6296 DI 10.1039/c3nr01387a PG 6 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA 172OW UT WOS:000321014900013 PM 23740334 ER PT J AU Mortensen, NP Hurst, GB Wang, W Foster, CM Nallathamby, PD Retterer, ST AF Mortensen, Ninell P. Hurst, Gregory B. Wang, Wei Foster, Carmen M. Nallathamby, Prakash D. Retterer, Scott T. TI Dynamic development of the protein corona on silica nanoparticles: composition and role in toxicity SO NANOSCALE LA English DT Article ID IN-VITRO TOXICITY; SHOTGUN PROTEOMICS; OXIDATIVE STRESS; PLASMA-PROTEINS; DOSIMETRY; DELIVERY; BIOCOMPATIBILITY; IDENTIFICATIONS; CYTOTOXICITY; MECHANISMS AB The formation and composition of the protein corona on silica (SiO2) nanoparticles (NP) with different surface chemistries was evaluated over time. Native SiO2, amine (-NH2) and carboxy (-COO-) modified NP were examined following incubation in mammalian growth media containing fetal bovine serum (FBS) for 1, 4, 24 and 48 hours. The protein corona transition from its early dynamic state to the later more stable corona was evaluated using mass spectrometry. The NP diameter was 22.4 +/- 2.2 nm measured by scanning transmission electron microscopy (STEM). Changes in hydrodynamic diameter and agglomeration kinetics were studied using dynamic light scattering (DLS). The initial surface chemistry of the NP played an important role in the development and final composition of the protein corona, impacting agglomeration kinetics and NP toxicity. Particle toxicity, indicated by changes in membrane integrity and mitochondrial activity, was measured by lactate dehydrogenase (LDH) release and tetrazolium reduction (MTT), respectively, in mouse alveolar macrophages (RAW264.7) and mouse lung epithelial cells (C10). SiO2-COO- NP had a slower agglomeration rate, formed smaller aggregates, and exhibited lower cytotoxicity compared to SiO2 and SiO2-NH2. Composition of the protein corona for each of the three NP was unique, indicating a strong dependence of corona development on NP surface chemistry. This work underscores the need to understand all aspects of NP toxicity, particularly the influence of agglomeration on effective dose and particle size. Furthermore, the interplay between materials and local biological environment is emphasized and highlights the need to conduct toxicity profiling under physiologically relevant conditions that provide an appropriate estimation of material modifications that occur during exposure in natural environments. C1 [Mortensen, Ninell P.; Foster, Carmen M.; Retterer, Scott T.] Oak Ridge Natl Lab, Biosci Div, Biol & Nanoscale Syst Grp, Oak Ridge, TN 37831 USA. [Mortensen, Ninell P.; Retterer, Scott T.] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci Div, Oak Ridge, TN 37831 USA. [Hurst, Gregory B.] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. [Wang, Wei] Oak Ridge Natl Lab, Div Environm Sci, Oak Ridge, TN 37831 USA. [Mortensen, Ninell P.; Nallathamby, Prakash D.; Retterer, Scott T.] Battelle Mem Inst, Battelle Ctr Fundamental & Appl Syst Toxicol, B FAST, Columbus, OH 43201 USA. [Mortensen, Ninell P.] RTI Int, Ctr Aerosol & Nanomat Engn, Nanotoxicol & Nanopharmacol, Res Triangle Pk, NC 27709 USA. RP Retterer, ST (reprint author), Oak Ridge Natl Lab, Biosci Div, Biol & Nanoscale Syst Grp, Oak Ridge, TN 37831 USA. EM rettererst@ornl.gov RI Wang, Wei/B-5924-2012; Retterer, Scott/A-5256-2011; OI Retterer, Scott/0000-0001-8534-1979; Hurst, Gregory/0000-0002-7650-8009 FU B-FAST, Battelle Center for Fundamental and Applied Systems Toxicology, Mult-Scale Toxicity Initiative; Center for Nanophase Materials Sciences; Division of Scientific User Facilities, US Department of Energy; US DOE [DE-AC05-00OR22725] FX This research was supported by the B-FAST, Battelle Center for Fundamental and Applied Systems Toxicology, Mult-Scale Toxicity Initiative. STR would like to acknowledge funding from the Center for Nanophase Materials Sciences, which is sponsored at Oak Ridge National Laboratory by the Division of Scientific User Facilities, US Department of Energy. This work was performed at the Oak Ridge National Laboratory, managed by UT-Battelle, LLC, for the US DOE under Contract No. DE-AC05-00OR22725. NR 50 TC 45 Z9 45 U1 8 U2 77 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 14 BP 6372 EP 6380 DI 10.1039/c3nr33280b PG 9 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA 172OW UT WOS:000321014900027 PM 23736871 ER PT J AU Liu, FQ Wu, HM Li, T Grabstanowicz, LR Amine, K Xu, T AF Liu, Fa-Qian Wu, Huiming Li, Tao Grabstanowicz, Lauren R. Amine, Khalil Xu, Tao TI Three-dimensional conducting oxide nanoarchitectures: morphology-controllable synthesis, characterization, and applications in lithium-ion batteries SO NANOSCALE LA English DT Article ID SENSITIZED SOLAR-CELLS; TIN OXIDE; HOLLOW SPHERES; ELECTRICAL-CONDUCTIVITY; STANNOUS SALTS; HIGH-CAPACITY; THIN-FILMS; TRANSPARENT; NANOPARTICLES; GRAPHENE AB We report the synthesis, characterization and applications in Li-ion batteries of a set of 3-dimensional (3-D) nanostructured conducting oxides including fluorinated tin oxide (FTO) and aluminum zinc oxide (AZO). The morphology of these 3-D conducting oxide nanoarchitectures can be directed towards either mono-dispersed hollow nanobead matrix or mono-dispersed sponge-like nanoporous matrix by controlling the surface charge of the templating polystyrene (PS) nanobeads, the steric hindrance and hydrolysis rates of the precursors, pH of the solvents etc. during the evaporative co-assembly of the PS beads. These 3-D nanostructured conducting oxide matrices possess high surface area (over 100 m(2) g(-1)) and accessible interconnected pores extending in all three spatial dimensions. By optimizing the temperature profile during calcination, we can obtain large area (of a few cm(2)) and crack-free nanoarchitectured films with thickness over 60 mu m. As such, the sheet resistance of these nanoarchitectured films on FTO glass can reach below 20 Omega per square. The nanoarchitectured FTO electrodes were used as anodes in Li-ion batteries, and they showed an enhanced cycling performance and stability over pure SnO2. C1 [Liu, Fa-Qian; Grabstanowicz, Lauren R.; Xu, Tao] No Illinois Univ, Dept Chem & Biochem, De Kalb, IL 60115 USA. [Wu, Huiming; Amine, Khalil] Argonne Natl Lab, Argonne, IL 60439 USA. [Li, Tao] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. RP Xu, T (reprint author), No Illinois Univ, Dept Chem & Biochem, De Kalb, IL 60115 USA. EM txu@niu.edu RI Amine, Khalil/K-9344-2013; li, tao/K-8911-2012 OI li, tao/0000-0001-5454-1468 FU National Science Foundation [CBET-1150617]; U.S. Department of Energy, Vehicle Technologies Office; U.S. Department of Energy by UChicago Argonne, LLC [DE-AC02-06CH11357]; U.S. Department of Energy Office of Science Laboratory by U of Chicago Argonne, LLC [DE-AC02-06CH11357] FX TX acknowledges the support from the National Science Foundation (CBET-1150617). The battery research at Argonne National Laboratory was supported by U.S. Department of Energy, Vehicle Technologies Office. Argonne National Laboratory is operated for the U.S. Department of Energy by UChicago Argonne, LLC, under contract DE-AC02-06CH11357. The electron microscopy study was conducted at the Electron Microscopy Center for Materials Research at Argonne National Laboratory, a U.S. Department of Energy Office of Science Laboratory operated under Contract no. DE-AC02-06CH11357 by U of Chicago Argonne, LLC. NR 44 TC 8 Z9 8 U1 13 U2 127 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 14 BP 6422 EP 6429 DI 10.1039/c3nr01844j PG 8 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA 172OW UT WOS:000321014900033 PM 23740404 ER PT J AU Puretzky, AA Geohegan, DB Pannala, S Rouleau, CM Regmi, M Thonnard, N Eres, G AF Puretzky, Alexander A. Geohegan, David B. Pannala, Sreekanth Rouleau, Christopher M. Regmi, Murari Thonnard, Norbert Eres, Gyula TI Real-time optical diagnostics of graphene growth induced by pulsed chemical vapor deposition SO NANOSCALE LA English DT Article ID SITU RAMAN-SPECTROSCOPY; WALLED CARBON NANOTUBES; SINGLE-LAYER GRAPHENE; LARGE-AREA; BILAYER GRAPHENE; HIGH-QUALITY; POLYCRYSTALLINE NI; FILMS; CU; TEMPERATURE AB The kinetics and mechanisms of graphene growth on Ni films at 720-880 degrees C have been measured using fast pulses of acetylene and real-time optical diagnostics. In situ UV-Raman spectroscopy was used to unambiguously detect isothermal graphene growth at high temperatures, measure the growth kinetics with similar to 1 s temporal resolution, and estimate the fractional precipitation upon cooldown. Optical reflectivity and videography provided much faster temporal resolution. Both the growth kinetics and the fractional isothermal precipitation were found to be governed by the C2H2 partial pressure in the CVD pulse for a given film thickness and temperature, with up to similar to 94% of graphene growth occurring isothermally within 1 second at 800 degrees C at high partial pressures. At lower partial pressures, isothermal graphene growth is shown to continue 10 seconds after the gas pulse. These flux-dependent growth kinetics are described in the context of a dissolution/precipitation model, where carbon rapidly dissolves into the Ni film and later precipitates driven by gradients in the chemical potential. The combination of pulsed-CVD and real-time optical diagnostics opens new opportunities to understand and control the fast, sub-second growth of graphene on various substrates at high temperatures. C1 [Puretzky, Alexander A.; Geohegan, David B.; Pannala, Sreekanth; Rouleau, Christopher M.; Regmi, Murari; Thonnard, Norbert; Eres, Gyula] Oak Ridge Natl Lab, Oak Ridge, TN USA. RP Puretzky, AA (reprint author), Oak Ridge Natl Lab, Oak Ridge, TN USA. EM puretzkya@ornl.gov RI Pannala, Sreekanth/F-9507-2010; Rouleau, Christopher/Q-2737-2015; Puretzky, Alexander/B-5567-2016; Geohegan, David/D-3599-2013; Eres, Gyula/C-4656-2017 OI Rouleau, Christopher/0000-0002-5488-3537; Puretzky, Alexander/0000-0002-9996-4429; Geohegan, David/0000-0003-0273-3139; Eres, Gyula/0000-0003-2690-5214 FU Materials Sciences and Engineering (MSE) Division, Office of Basic Energy Sciences, U.S. Department of Energy; Scientific User Facilities (SUF) Division, U.S. Department of Energy FX Synthesis science sponsored by the Materials Sciences and Engineering (MSE) Division, Office of Basic Energy Sciences, U.S. Department of Energy. Characterization science including Raman spectroscopy and SEM part of this research was conducted at the Center for Nanophase Materials Sciences user facility, which is sponsored at Oak Ridge National Laboratory by the Scientific User Facilities (SUF) Division, U.S. Department of Energy. NR 55 TC 8 Z9 8 U1 1 U2 43 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2040-3364 J9 NANOSCALE JI Nanoscale PY 2013 VL 5 IS 14 BP 6507 EP 6517 DI 10.1039/c3nr01436c PG 11 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA 172OW UT WOS:000321014900044 PM 23752798 ER PT J AU Pettibone, JM Osborn, WA Rykaczewski, K Talin, AA Bonevich, JE Hudgens, JW Allendorf, MD AF Pettibone, John M. Osborn, William A. Rykaczewski, Konrad Talin, A. Alec Bonevich, John E. Hudgens, Jeffrey W. Allendorf, Mark D. TI Surface mediated assembly of small, metastable gold nanoclusters SO NANOSCALE LA English DT Article ID CO OXIDATION; CLUSTERS; SIZE; MONODISPERSE; IDENTIFICATION; NANOPARTICLES; TEMPERATURE; REACTIVITY; DEPOSITION; CATALYSTS AB The unique properties of metallic nanoclusters are attractive for numerous commercial and industrial applications but are generally less stable than nanocrystals. Thus, developing methodologies for stabilizing nanoclusters and retaining their enhanced functionality is of great interest. We report the assembly of PPh3-protected Au-9 clusters from a heterogeneous mixture into films consisting of sub 3 nm nanocluster assemblies. The depositing nanoclusters are metastable in solution, but the resulting nanocluster assemblies are stabilized indefinitely in air or fresh solvent. The films exhibit distinct structure from Au nanoparticles observed by X-ray diffraction, and film dissolution data support the preservation of small nanoclusters. UV-Vis spectroscopy, electrospray ionization mass spectrometry, X-ray photoelectron spectroscopy and electron microscopy are used to elucidate information regarding the nanocluster formation and assembly mechanism. Preferential deposition of nanocluster assemblies can be achieved on multiple substrates, including polymer, Cr, Si, SiO2, SiNx, and metal-organic frameworks (MOFs). Unlike other vapor phase coating processes, nanocluster assembly on the MIL-68(In) MOF crystal is capable of preferentially coating the external surface and stabilizing the crystal structure in hydrothermal conditions, which should enhance their storage, separation and delivery capabilities. C1 [Pettibone, John M.; Osborn, William A.; Rykaczewski, Konrad; Bonevich, John E.; Hudgens, Jeffrey W.] NIST, Mat Measurement Lab, Gaithersburg, MD 20899 USA. [Talin, A. Alec] NIST, Ctr Nanoscale Sci & Technol, Gaithersburg, MD 20899 USA. [Allendorf, Mark D.] Sandia Natl Labs, Livermore, CA USA. RP Pettibone, JM (reprint author), NIST, Mat Measurement Lab, Gaithersburg, MD 20899 USA. EM john.pettibone@nist.gov RI Osborn, Will/G-4526-2012 FU Sandia Laboratory Directed Research and Development Program; United States Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX The authors thank K. Steffens for help with XPS measurements and M. Martin for help synthesizing the gold nanoparticles. MDA was supported by the Sandia Laboratory Directed Research and Development Program. 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 41 TC 6 Z9 6 U1 14 U2 142 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 14 BP 6558 EP 6566 DI 10.1039/c3nr01708g PG 9 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA 172OW UT WOS:000321014900051 PM 23759958 ER PT S AU Akl, TJ Wilson, MA Ericson, MN Cote, GL AF Akl, Tony J. Wilson, Mark A. Ericson, M. Nance Cote, Gerard L. BE Cote, GL TI Optical Modeling toward Optimizing Monitoring of Intestinal Perfusion in Trauma Patients SO OPTICAL DIAGNOSTICS AND SENSING XIII: TOWARD POINT-OF-CARE DIAGNOSTICS SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Optical Diagnostics and Sensing XIII - Toward Point-of-Care Diagnostics CY FEB 06, 2013 CL San Francisco, CA SP SPIE DE Perfusion monitoring; Photoplethysmography; Trauma; Oximetry; Telemetry ID TISSUE; RESUSCITATION; PENETRATION; DEPTH; SHOCK AB Trauma is the number one cause of death for people between the ages 1 and 44 years in the United States. In addition, according to the Centers of Disease Control and Prevention, injury results in over 31 million emergency department visits annually. Minimizing the resuscitation period in major abdominal injuries increases survival rates by correcting impaired tissue oxygen delivery. Optimization of resuscitation requires a monitoring method to determine sufficient tissue oxygenation. Oxygenation can be assessed by determining the adequacy of tissue perfusion. In this work, we present the design of a wireless perfusion and oxygenation sensor based on photoplethysmography. Through optical modeling, the benefit of using the visible wavelengths 470, 525 and 590nm (around the 525nm hemoglobin isobestic point) for intestinal perfusion monitoring is compared to the typical near infrared (NIR) wavelengths (805nm isobestic point) used in such sensors. Specifically, NIR wavelengths penetrate through the thin intestinal wall (similar to 4mm) leading to high background signals. However, these visible wavelengths have two times shorter penetration depth that the NIR wavelengths. Monte-Carlo simulations show that the transmittance of the three selected wavelengths is lower by 5 orders of magnitude depending on the perfusion state. Due to the high absorbance of hemoglobin in the visible range, the perfusion signal carried by diffusely reflected light is also enhanced by an order of magnitude while oxygenation signal levels are maintained. In addition, short source-detector separations proved to be beneficial for limiting the probing depth to the thickness of the intestinal wall. C1 [Akl, Tony J.; Cote, Gerard L.] Texas A&M Univ, Dept Biomed Engn, College Stn, TX 77843 USA. [Wilson, Mark A.] Univ Pittsburgh, Dept Surg, Pittsburgh, PA 15260 USA. [Wilson, Mark A.] VA Pittsburgh Healthcare Syst, Pittsburgh, PA 15260 USA. [Cote, Gerard L.] Oak Ridge Natl Lab, Oak Ridge, TN USA. RP Akl, TJ (reprint author), Texas A&M Univ, Dept Biomed Engn, College Stn, TX 77843 USA. RI Ericson, Milton/H-9880-2016 OI Ericson, Milton/0000-0002-6628-4865 FU NIH [5R01-GM077150] FX This research was funded by a bioengineering research partnership (BRP) grant from NIH, (#5R01-GM077150). NR 21 TC 0 Z9 0 U1 0 U2 0 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9360-6 J9 PROC SPIE PY 2013 VL 8591 AR 859106 DI 10.1117/12.2003352 PG 6 WC Engineering, Biomedical; Optics SC Engineering; Optics GA BFX14 UT WOS:000321740300006 ER PT J AU Mitri, FG AF Mitri, F. G. TI Vector wave analysis of an electromagnetic high-order Bessel vortex beam of fractional type alpha: II. The cases of standing and quasi-standing waves SO OPTIK LA English DT Article DE Bessel beams; Diffraction theory; Electromagnetic optics; Optical laser tweezers; (Quasi-)standing waves ID DIELECTRIC SPHERE; SCATTERING AB Stemming from the vector Maxwell's equations and Lorenz' gauge condition, a full vector-wave derivation for the electric and magnetic fields components of a high-order Bessel vortex beam of fractional type a (HOBVB-F alpha) is provided. The field corresponds to the most generalized case of quasi-standing waves that reduce to perfect (i.e. equi-amplitude) standing waves or progressive waves with appropriate choice of the quasi-standing wave coefficient Y. The results are of particular importance in the study of the optical/electromagnetic wave scattering, radiation force and torque in optical tweezers operating with this fractional type of non-diffracting vortex beams. (C) 2012 Elsevier GmbH. All rights reserved. C1 Los Alamos Natl Lab, Acoust & Sensors Technol Team, MPA 11, Los Alamos, NM 87545 USA. RP Mitri, FG (reprint author), Los Alamos Natl Lab, Acoust & Sensors Technol Team, MPA 11, MS D429, Los Alamos, NM 87545 USA. EM mitri@lanl.gov FU Los Alamos National Laboratory (LDRD-X9N9) [20100595PRD1] FX The financial support provided through a Director's fellowship (LDRD-X9N9, Project # 20100595PRD1) from the Los Alamos National Laboratory is gratefully acknowledged. NR 17 TC 6 Z9 6 U1 0 U2 4 PU ELSEVIER GMBH, URBAN & FISCHER VERLAG PI JENA PA OFFICE JENA, P O BOX 100537, 07705 JENA, GERMANY SN 0030-4026 J9 OPTIK JI Optik PY 2013 VL 124 IS 13 BP 1469 EP 1471 DI 10.1016/j.ijleo.2012.04.024 PG 3 WC Optics SC Optics GA 173PG UT WOS:000321090800020 ER PT S AU Schunck, N AF Schunck, Nicolas GP IOP TI Microscopic description of induced fission SO 10TH INTERNATIONAL CONFERENCE ON CLUSTERING ASPECTS OF NUCLEAR STRUCTURE AND DYNAMICS (CLUSTER'12) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 10th International Conference on Clustering Aspects of Nuclear Structure and Dynamics (CLUSTER) CY SEP 24-28, 2012 CL MTA Inst Nucl Res, Debrecen, HUNGARY SP Hungarian Acad Sci, Paks Nucl Power Ltd, HMP Log Ltd, Int Workshop Theoret Phys, Univ Debrecen HO MTA Inst Nucl Res AB Selected aspects of the description of neutron-induced fission in Pu-240 in the framework of the nuclear energy density functional theory at finite temperature are presented. In particular, we discuss aspects pertaining to the choice of thermodynamic state variables, the evolution of fission barriers as function of the incident neutron energy, and the temperatures of the fission fragments. C1 Lawrence Livermore Natl Lab, Div Phys, Livermore, CA 94551 USA. RP Schunck, N (reprint author), Lawrence Livermore Natl Lab, Div Phys, Livermore, CA 94551 USA. EM schunck1@llnl.gov OI Schunck, Nicolas/0000-0002-9203-6849 NR 15 TC 6 Z9 6 U1 0 U2 4 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 436 AR UNSP 012058 DI 10.1088/1742-6596/436/1/012058 PG 5 WC Physics, Multidisciplinary; Physics, Nuclear SC Physics GA BFK64 UT WOS:000320267700057 ER PT S AU Bahrdt, J Ivanyushenkov, Y AF Bahrdt, J. Ivanyushenkov, Y. BE Susini, J Dumas, P TI Short Period Undulators for Storage Rings and Free Electron Lasers 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 SUPERCONDUCTING UNDULATOR; FIELD; FABRICATION AB Short period undulators have the potential to enhance the spectral performance of synchrotron radiation sources significantly. These devices open the range of brilliant hard X-rays at medium energy storage rings, their implementation may reduce the facility length of linac based FELs and they are an essential prerequisite for laser plasma accelerator based FELs. The development of cryogenic permanent magnet undulators has started and the first devices, employing period lengths around 18mm, have been installed in 3rd generation storage rings. Ambitious magnet designs permit even smaller period lengths which improve their performance further. The paper discusses the performance of cryogenic permanent magnet undulators in comparison with superconducting undulators. C1 [Bahrdt, J.] Helmholtzzentrum Berlin Mat & Energie, Glienicker Str 100, D-14109 Berlin, Germany. [Ivanyushenkov, Y.] Argonne Natl Lab, Argonne, IL 60439 USA. RP Bahrdt, J (reprint author), Helmholtzzentrum Berlin Mat & Energie, Glienicker Str 100, D-14109 Berlin, Germany. EM Johannes.Bahrdt@helmholtz-berlin.de NR 41 TC 5 Z9 5 U1 0 U2 8 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 425 AR UNSP 032001 DI 10.1088/1742-6596/425/3/032001 PG 6 WC Instruments & Instrumentation; Physics, Applied; Physics, Multidisciplinary SC Instruments & Instrumentation; Physics GA BFL51 UT WOS:000320403700026 ER PT S AU Benson, SV Douglas, DR Evtushenko, P Hannon, FE Hernandez-Garcia, C Klopf, JM Legg, RA Neil, GR Shinn, MD Tennant, CD Zhang, S Williams, GP AF Benson, S. V. Douglas, D. R. Evtushenko, P. Hannon, F. E. Hernandez-Garcia, C. Klopf, J. M. Legg, R. A. Neil, G. R. Shinn, M. D. Tennant, C. D. Zhang, S. Williams, G. P. BE Susini, J Dumas, P TI Photon Source Capabilities of the Jefferson Lab FEL 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 AB Jefferson Lab operates a superconducting energy recovered linac which is operated with CW RF and which powers oscillator-based IR and UV Free-Electron Lasers (FELs) with diffraction limited sub-picosecond pulses with >10(13) photons per pulse (1.0%BW) at pulse repetition frequencies up to 75 MHz. Useful harmonics extend into the vacuum ultraviolet (VUV). Based on FEL model calculations validated using this facility, we have designed both an oscillator-based VUV-FEL that would produce 6 x 10(12) coherent (0.5% BW) 100 eV photons per pulse at multi-MHz repetition rates in the fundamental, and a dual FEL configuration that would allow simultaneous lasing lasing at THz and UV wavelengths. The VUV-FEL would utilize a novel high gain, low Q cavity, while the THz source would be an FEL oscillator with a short wiggler providing diffraction limited pulses with pulse energy exceeding 50 microJoules. The THz source would use the exhaust beam from a UV FEL. Such multiphoton capabilities would provide unique opportunities for out of equilibrium dynamical studies at time-scales down to 50 fs. The fully coherent nature of all these sources results in peak and average brightness values that are many orders of magnitude higher than storage rings. C1 [Benson, S. V.; Douglas, D. R.; Evtushenko, P.; Hannon, F. E.; Hernandez-Garcia, C.; Klopf, J. M.; Legg, R. A.; Neil, G. R.; Shinn, M. D.; Tennant, C. D.; Zhang, S.; Williams, G. P.] Jefferson Lab, Newport News, VA 23606 USA. RP Benson, SV (reprint author), Jefferson Lab, 12000 Jefferson Ave, Newport News, VA 23606 USA. EM gwyn@jlab.org NR 7 TC 1 Z9 1 U1 1 U2 8 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 425 AR UNSP 072002 DI 10.1088/1742-6596/425/7/072002 PG 5 WC Instruments & Instrumentation; Physics, Applied; Physics, Multidisciplinary SC Instruments & Instrumentation; Physics GA BFL51 UT WOS:000320403700120 ER PT S AU Borland, M AF Borland, M. BE Susini, J Dumas, P TI Progress Toward an Ultimate Storage Ring Light Source 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 AB Developments such as the low emittance NSLS-II storage ring, followed by the even lower emittance MAX IV ring, indicate that the technology of storage ring light sources has not reached full maturity. Indeed, these new sources are paving the way toward realizing diffraction-limited angstrom-wavelength storage ring light sources in the not-too-distant future. In this paper, we survey ongoing work around the world to develop concepts and designs for so-called "ultimate" storage ring light sources. Several of these designs target horizontal emittances that are two or more orders of magnitude less than present machines, and thus brightness and coherent fraction that is several orders of magnitude better than existing storage ring light sources. C1 Argonne Natl Lab, Argonne, IL 60439 USA. RP Borland, M (reprint author), Argonne Natl Lab, 9700 S Cass Ave, Argonne, IL 60439 USA. EM borland@aps.anl.gov NR 35 TC 13 Z9 13 U1 1 U2 15 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 425 AR UNSP 042016 DI 10.1088/1742-6596/425/4/042016 PG 6 WC Instruments & Instrumentation; Physics, Applied; Physics, Multidisciplinary SC Instruments & Instrumentation; Physics GA BFL51 UT WOS:000320403700065 ER PT S AU Cai, YQ Coburn, DS Cunsolo, A Keister, JW Honnicke, MG Huang, XR Kodituwakku, CN Stetsko, Y Suvorov, A Hiraoka, N Tsuei, KD Wille, HC AF Cai, Yong Q. Coburn, D. S. Cunsolo, A. Keister, J. W. Honnicke, M. G. Huang, X. R. Kodituwakku, C. N. Stetsko, Y. Suvorov, A. Hiraoka, N. Tsuei, K. D. Wille, H. C. BE Susini, J Dumas, P TI The Ultrahigh Resolution IXS Beamline of NSLS-II: Recent Advances and Scientific Opportunities 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 GRADED MULTILAYER MIRROR; MONOCHROMATOR AB The ultrahigh resolution IXS beamline of NSLS-II is designed to probe a region of dynamic response that requires an ultrahigh energy and momentum resolution of up to 0.1 meV and < 0.1 nm(-1), respectively, which is currently still beyond the reach of existing low and high frequency inelastic scattering probes. Recent advances at NSLS-II in developing the required x-ray optics and instrumentation based on the use of extremely asymmetric Bragg back reflections of Si have allowed us to achieve sub-meV energy resolution with sharp tails and high efficiency at a medium energy of around 9.1 keV, thereby validating the optical design of the beamline for the baseline scope and paving the way for further development towards the ultimate goal of 0.1 meV. The IXS beamline is expected to provide a broad range of scientific opportunities, particularly in areas of liquid, disordered and bio-molecular systems. C1 [Cai, Yong Q.; Coburn, D. S.; Cunsolo, A.; Keister, J. W.; Honnicke, M. G.; Huang, X. R.; Kodituwakku, C. N.; Stetsko, Y.; Suvorov, A.] Brookhaven Natl Lab, Upton, NY 11973 USA. [Wille, H. C.] Deutsches Elektronen Synchrotron, PETRA 3, D-22607 Hamburg, Germany. [Tsuei, K. D.] Natl Synchrotron Radiat Res Ctr, Hsinchu 30076, Taiwan. RP Cai, YQ (reprint author), Brookhaven Natl Lab, Upton, NY 11973 USA. EM cai@bnl.gov RI Cai, Yong/C-5036-2008; Honnicke, Marcelo/I-8624-2012 OI Cai, Yong/0000-0002-9957-6426; FU JASRI [2011A4262]; NSRRC [2011-1-002]; U.S. Department of Energy, Office of Basic Energy Science, [DE-AC02-98CH10886] FX We are grateful to Q. Shen and T. Ishikawa for support and encouragement throughout the project. We are indebted to A. Kuczewski and D.P. Siddons for support in detectors, D. Chabot and K. Gofron in controls, L. Reffi in mechanical design of the prototype instrument, W. Struble and R. Conley in crystal optics fabrication, and H. Yavas, F.U. Dill (PETRA III) and Y. Kohmura (SPring-8) for experimental support. M. Krisch (ESRF), A. Baron (SPring-8) and Yu. Shvyd'ko (APS) are acknowledged for providing the performance data for their respective facilities in Table 1. We thank members of the Beamline Advisory Team including C. Burns, S.H. Chen, J. Hill, M. Krisch, H.K. Mao, T. Scopigno, S. Shapiro and Yu. Shvyd'ko for their valuable contributions to the project. W. Sturhahn, T. Toellner and D. Shu are acknowledged for stimulating discussions. Experiments at BL12XU/SPring-8 were performed under the approvals from JASRI (No. 2011A4262) and NSRRC (No. 2011-1-002). This work was supported by the U.S. Department of Energy, Office of Basic Energy Science, under Contract No. DE-AC02-98CH10886. NR 14 TC 16 Z9 16 U1 0 U2 13 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 425 AR UNSP 202001 DI 10.1088/1742-6596/425/20/202001 PG 7 WC Instruments & Instrumentation; Physics, Applied; Physics, Multidisciplinary SC Instruments & Instrumentation; Physics GA BFL51 UT WOS:000320403700271 ER PT S AU Canestrari, N Chubar, O del Rio, MS AF Canestrari, Niccolo Chubar, Oleg del Rio, Manuel Sanchez BE Susini, J Dumas, P TI Improved models for synchrotron radiation sources in SHADOW 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 AB A technique to improve the description of synchrotron sources is proposed and applied to the ray tracing code SHADOW. Using a dedicated synchrotron radiation calculation code, it is possible to calculate the single electron emission, as well as the thick electron beam emission. Two methods will be introduced. The first simulates synchrotron radiation using the spatial electron distribution for the positions of the rays and the thick electron beam spectral-angular distribution in the far field for their directions and their energies. The second method derives the variation of the single electron spectral-angular distribution with respect to the electron direction and the electron energy, and simulates the rays emitted by each electron. A preprocessor for SHADOW has been developed to read the intensity distribution from an HDF5 file generated by SRW. The final rays have been used to simulate future beamlines and have been cross checked with the wavefront propagation method. C1 [Canestrari, Niccolo; Chubar, Oleg] Brookhaven Natl Lab, Upton, NY 11973 USA. [Canestrari, Niccolo; del Rio, Manuel Sanchez] European Synchrotron Radiat Fac, Grenoble, France. RP Canestrari, N (reprint author), Brookhaven Natl Lab, Upton, NY 11973 USA. EM ncanestrari@bnl.gov RI Chubar, Oleg/B-6286-2014 FU National Laboratory Research Scholar Program [P-1-01957, 8668704]; European Synchrotron Radiation Facility; University Joseph Fourier in Grenoble FX The present work has been finaced by the Brookhaven National Laboratory Research Scholar Program grant P-1-01957 No. 8668704, and was made in collaboration with the European Synchrotron Radiation Facility and the University Joseph Fourier in Grenoble. NR 4 TC 1 Z9 1 U1 0 U2 0 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 425 AR UNSP 162007 DI 10.1088/1742-6596/425/16/162007 PG 4 WC Instruments & Instrumentation; Physics, Applied; Physics, Multidisciplinary SC Instruments & Instrumentation; Physics GA BFL51 UT WOS:000320403700229 ER PT S AU Chubar, O Fluerasu, A Berman, L Kaznatcheev, K Wiegart, L AF Chubar, O. Fluerasu, A. Berman, L. Kaznatcheev, K. Wiegart, L. BE Susini, J Dumas, P TI Wavefront propagation simulations for beamlines and experiments with "Synchrotron Radiation Workshop" 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 INFRARED BEAMLINE; FACILITY SOLEIL; COMPUTATION; CODE; FEL AB An overview of the basic principles, the approach to fully- and partially-coherent synchrotron radiation wavefront propagation simulations, implemented in the "Synchrotron Radiation Workshop" (SRW) computer code, and simulation examples for different types of sources, including undulator and wiggler, different beamlines and experiments, are presented. Recent developments, such as the support of parallel calculations, which considerably increase the efficiency of partially-coherent wavefront propagation calculations, are described. C1 [Chubar, O.; Fluerasu, A.; Berman, L.; Kaznatcheev, K.; Wiegart, L.] Brookhaven Natl Lab, Photon Sci Directorate, Upton, NY 11973 USA. RP Chubar, O (reprint author), Brookhaven Natl Lab, Photon Sci Directorate, Upton, NY 11973 USA. EM chubar@bnl.gov RI Chubar, Oleg/B-6286-2014 NR 24 TC 8 Z9 9 U1 1 U2 13 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 425 AR UNSP 162001 DI 10.1088/1742-6596/425/16/162001 PG 6 WC Instruments & Instrumentation; Physics, Applied; Physics, Multidisciplinary SC Instruments & Instrumentation; Physics GA BFL51 UT WOS:000320403700223 ER PT S AU Chubar, O Fluerasu, A Chu, YS Berman, L Wiegart, L Lee, WK Baltser, J AF Chubar, O. Fluerasu, A. Chu, Y. S. Berman, L. Wiegart, L. Lee, W-K Baltser, J. BE Susini, J Dumas, P TI Experimental characterization of X-ray transverse coherence in the presence of beam transport optics 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 SYNCHROTRON-RADIATION AB A simple Boron fiber based interference scheme [1] and other similar schemes are currently routinely used for X-ray coherence estimation at 3rd generation synchrotron radiation sources. If such a scheme is applied after a perfect monochromator and without any focusing/transport optics in the optical path, the interpretation of the measured interference pattern is relatively straightforward and can be done in terms of the basic parameters of the source [2]. However, if the interference scheme is used after some focusing optics, e. g. close to the X-ray beam waist, the visibility of fringes can be significantly affected by the new shape of the focused beam phase-space. At the same time, optical element imperfections still have a negative impact on the transverse coherence. In such situations, which are frequently encountered in experiments at beamlines, the quantitative interpretation of a measured interference pattern is not straightforward. Here we show that this can nevertheless be done by using partially-coherent synchrotron radiation wavefront propagation simulations. The results obtained from measurements, performed at the 32-ID undulator beamline of the Advanced Photon Source, and wavefront propagation based simulations show, in particular, that new generation 1D Beryllium Compound Refractive Lenses [3, 4] do not reduce the X-ray transverse coherence in any significant manner. C1 [Chubar, O.; Fluerasu, A.; Chu, Y. S.; Berman, L.; Wiegart, L.; Lee, W-K] Brookhaven Natl Lab, Photon Sci Directorate, Upton, NY 11973 USA. [Baltser, J.] Univ Copenhagen, Niels Bohr Inst, DK-1168 Copenhagen, Denmark. RP Chubar, O (reprint author), Brookhaven Natl Lab, Photon Sci Directorate, Upton, NY 11973 USA. EM chubar@bnl.gov RI Chubar, Oleg/B-6286-2014 FU US DOE [DE-AC02-98CH10886, DE-AC02-06CH11357] FX This work has been supported by US DOE, Contract No. DE-AC02-98CH10886 and the use of Advanced Photon Source is supported by US DOE Contract No. DE-AC02-06CH11357. NR 13 TC 3 Z9 3 U1 0 U2 5 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 425 AR UNSP 052028 DI 10.1088/1742-6596/425/5/052028 PG 4 WC Instruments & Instrumentation; Physics, Applied; Physics, Multidisciplinary SC Instruments & Instrumentation; Physics GA BFL51 UT WOS:000320403700096 ER PT S AU Chubar, O Bengtsson, J Blednykh, A Kitegi, C Rakowsky, G Tanabe, T Clarke, J AF Chubar, O. Bengtsson, J. Blednykh, A. Kitegi, C. Rakowsky, G. Tanabe, T. Clarke, J. BE Susini, J Dumas, P TI Segmented Adaptive-Gap In-Vacuum Undulators - Potential Solution for Beamlines Requiring High Hard X-Ray Flux and Brightness in Medium Energy Synchrotron Sources? 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 AB We propose an approach to the optimization of segmented in-vacuum undulators, in which different segments along an undulator may have different gaps and periods. This enables close matching between the gaps and the vertical "envelope" of electron beam motion in a storage ring straight section (carefully satisfying the associated vertical "stay clear" constraint) and, at the same time, precise tuning of all the segments to the same fundamental photon energy. Placing together undulator segments with different periods may introduce small kicks to electron trajectories at the segment junctions, which can be easily compensated, without introducing any significant radiation phase error, by active correction magnets or by special design of terminating magnets in the segments. Thanks to this, the entire multi-segment structure can operate as one long undulator. On the other hand, since the vertical gaps in segments located close to straight section center can be smaller than at extremities, such structure can offer better magnetic performance, compared to the case of a standard undulator with constant gap (and period) over its length. We present magnetic field, radiation flux and brightness calculation results for such segmented adaptive-gap in-vacuum undulators if used in low-beta straight sections of NSLS-II, and demonstrate their gain in spectral performance, especially in hard X-ray range, over standard room-temperature and even cryo-cooled in-vacuum undulators. C1 [Chubar, O.; Bengtsson, J.; Blednykh, A.; Kitegi, C.; Rakowsky, G.; Tanabe, T.] Brookhaven Natl Lab, Photon Sci Directorate, Upton, NY 11973 USA. [Clarke, J.] ASTeC, STFC, Daresbury Lab, Warrington, Cheshire, England. RP Chubar, O (reprint author), Brookhaven Natl Lab, Photon Sci Directorate, Upton, NY 11973 USA. EM chubar@bnl.gov RI Chubar, Oleg/B-6286-2014 FU US DOE [DE-AC02-98CH10886] FX We would also like to thank S. Dierker and F. Willeke for encouragement.; Work supported by US DOE, Contract No. DE-AC02-98CH10886. NR 11 TC 1 Z9 1 U1 0 U2 7 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 425 AR UNSP 032005 DI 10.1088/1742-6596/425/3/032005 PG 4 WC Instruments & Instrumentation; Physics, Applied; Physics, Multidisciplinary SC Instruments & Instrumentation; Physics GA BFL51 UT WOS:000320403700030 ER PT S AU Fayard, B Pouyet, E Berruyer, G Bugnazet, D Cornu, C Cotte, M De Andrade, V Di Chiaro, F Hignette, O Kieffer, J Martin, T Papillon, E Salome, M Sole, VA AF Fayard, B. Pouyet, E. Berruyer, G. Bugnazet, D. Cornu, C. Cotte, M. De Andrade, V. Di Chiaro, F. Hignette, O. Kieffer, J. Martin, T. Papillon, E. Salome, M. Sole, V. A. BE Susini, J Dumas, P TI The new ID21 XANES full-field end-station at ESRF 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 AB A new X-ray absorption near-edge spectroscopy (XANES) full-field imaging station has been developed, installed and tested on beamline ID21 at the European Synchrotron Radiation Facility (ESRF). The set-up operates in the 2-9 keV energy range and allows for the simultaneous acquisition of up to 4.10(6) XANES spectra over large sample areas with preserved sub-micron spatial resolution. The versatile set-up is compatible with various types of cameras and magnifying objectives. It accommodates spatial resolutions ranging from 0.3 mu m to 1.4 mu m and fields of view from 600 mu m up to 2 mm. The range of potential applications is broad: from geology, cultural heritage, environmental sciences to medicine. C1 [Fayard, B.] Univ Paris 11, UMR CNRS 8502, Lab Phys Solides, Bat 510, F-91405 Orsay, France. [Fayard, B.; Pouyet, E.; Berruyer, G.; Bugnazet, D.; Cornu, C.; Cotte, M.; Di Chiaro, F.; Hignette, O.; Kieffer, J.; Martin, T.; Papillon, E.; Salome, M.] European Synchrotron Radiat Fac, F-38043 Grenoble, France. [De Andrade, V.] Brookhaven Natl Lab, Natl Synchrotron Light Source, Upton, NY 11973 USA. [Di Chiaro, F.] Inst Laue Langevin, F-38042 Grenoble 9, France. RP Fayard, B (reprint author), Univ Paris 11, UMR CNRS 8502, Lab Phys Solides, Bat 510, F-91405 Orsay, France. EM barbara.fayard@u-psud.fr NR 6 TC 17 Z9 17 U1 1 U2 16 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 425 AR UNSP 192001 DI 10.1088/1742-6596/425/19/192001 PG 4 WC Instruments & Instrumentation; Physics, Applied; Physics, Multidisciplinary SC Instruments & Instrumentation; Physics GA BFL51 UT WOS:000320403700246 ER PT S AU Feng, Y Zhu, D Lemke, H Chollet, M Fritz, DM Robert, A Hastings, JB Feldkamp, M Cammarata, M Moeller, S Yabashi, M Tono, K Huang, X AF Feng, Y. Zhu, D. Lemke, H. Chollet, M. Fritz, D. M. Robert, A. Hastings, J. B. Feldkamp, M. Cammarata, M. Moeller, S. Yabashi, M. Tono, K. Huang, X. BE Susini, J Dumas, P TI Experimental Measurements of Ultra-Thin Bragg Crystals for LCLS Beam-Sharing Operation 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 AB The successful lasing and operation of the LCLS hard X-ray FEL has brought tremendous interest to the user community spanning a wide range of scientific disciplines including physics, chemistry, structural biology, and material science. It created demand on beam time that is often left unfulfilled. Here we report experimental measurements of ultra-thin silicon single-crystal membranes for potentially beam-sharing the LCLS beam. The samples included the (111), (220), and (400) orientations with thicknesses ranging from 5 to 20 m. Both high-resolution rocking curves and topographic data were first obtained using synchrotron X-rays, demonstrating near ideal diffraction qualities. Subsequent tests using the full LCLS beam revealed lattice distortions from beam-induced membrane vibrations, which were shown to be effectively reduced by ambient air and smaller membrane dimensions. High diffraction quality thin-diamonds in the (111) orientation are also being pursued as a parallel effort. Both approaches are paving a way for a practical beam-sharing implementation at LCLS in the near future. C1 [Feng, Y.; Zhu, D.; Lemke, H.; Chollet, M.; Fritz, D. M.; Robert, A.; Hastings, J. B.; Feldkamp, M.; Cammarata, M.; Moeller, S.] SLAC Natl Accelerator Lab, Linac Coherent Light Source, Menlo Pk, CA 94025 USA. [Yabashi, M.; Tono, K.] RIKEN, SPring 8, Mikazuki, Hyogo 6795148, Japan. [Huang, X.] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. RP Feng, Y (reprint author), SLAC Natl Accelerator Lab, Linac Coherent Light Source, Menlo Pk, CA 94025 USA. EM yfeng@SLAC.stanford.edu RI Zhu, Diling/D-1302-2013; Lemke, Henrik Till/N-7419-2016 OI Lemke, Henrik Till/0000-0003-1577-8643 FU Linac Coherent Light Source (LCLS) at SLAC National Accelerator Laboratory; U.S. Department of Energy Office of Science by Stanford University FX Y Feng wishes to give special thanks to SSRL staff members C. Knotts, B. Johnson and T. Hostetler for their continuing support. Portions of this research were carried out at the Linac Coherent Light Source (LCLS) at SLAC National Accelerator Laboratory. LCLS is an Office of Science User Facility operated for the U.S. Department of Energy Office of Science by Stanford University. NR 2 TC 5 Z9 5 U1 1 U2 1 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 425 AR UNSP 052002 DI 10.1088/1742-6596/425/5/052002 PG 4 WC Instruments & Instrumentation; Physics, Applied; Physics, Multidisciplinary SC Instruments & Instrumentation; Physics GA BFL51 UT WOS:000320403700070 ER PT S AU Ilinski, P AF Ilinski, P. BE Susini, J Dumas, P TI Optimization of NSLS-II Blade X-ray Beam Position Monitors: from Photoemission type to Diamond Detector 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 AB Optimization of blade type X-ray Beam Position Monitors (XBPM) was performed for NSLS-II undulator IVU20. Blade material, configuration and operation principle was analyzed to improve XBPM performance. Optimization is based on calculation of the XBPM signal spatial distribution. Along with standard photoemission blades, Diamond Detector Blade (DDB) was analyzed as XBPM signal source. Analyses revealed, that Diamond Detector Blade XBPM would allow overcoming drawbacks of the photoemission type XBPMs. C1 Brookhaven Natl Lab, Upton, NY 11973 USA. RP Ilinski, P (reprint author), Brookhaven Natl Lab, Upton, NY 11973 USA. EM pilinski@bnl.gov NR 3 TC 1 Z9 1 U1 0 U2 3 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 425 AR UNSP 042006 DI 10.1088/1742-6596/425/4/042006 PG 4 WC Instruments & Instrumentation; Physics, Applied; Physics, Multidisciplinary SC Instruments & Instrumentation; Physics GA BFL51 UT WOS:000320403700055 ER PT S AU Ivanyushenkov, Y Abliz, M Doose, C Fuerst, J Hasse, Q Kasa, M Lev, V Mezentsev, N Syrovatin, V Trakhtenberg, E Tsukanov, V Vasserman, I Gluskin, E AF Ivanyushenkov, Y. Abliz, M. Doose, C. Fuerst, J. Hasse, Q. Kasa, M. Lev, V. Mezentsev, N. Syrovatin, V. Trakhtenberg, E. Tsukanov, V. Vasserman, I. Gluskin, E. BE Susini, J Dumas, P TI Development of a superconducting undulator for the APS 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 AB As the western hemisphere's premier x-ray synchrotron radiation source, the Advanced Photon Source (APS) continues to advance the state of the art in insertion device technology in order to maintain record high brightness, especially in the hard x-ray wavelength region. Due to the unique bunch pattern used for normal APS operations and its ultimate capabilities, the APS has chosen superconducting technology for its future hard x-ray undulator sources. In the last several years, the APS in collaboration with the Budker Institute of Nuclear Physics has being developing the technology for planar, small-period superconducting undulators (SCUs). These developments include the design and construction of several prototypes and the construction of the necessary mechanical, vacuum, and cryogenic infrastructure at the APS site. Several prototypes of the SCU magnetic structure have been built and tested. The first SCU is assembled and will be installed in the APS storage ring at the end of 2012. Expected SCU performance in terms of x-ray brightness should noticeably exceed that of existing APS undulators. Immediately after commissioning, the SCU will be used at APS Sector 6 as the radiation source for high-energy x-ray studies. C1 [Ivanyushenkov, Y.; Abliz, M.; Doose, C.; Fuerst, J.; Hasse, Q.; Kasa, M.; Trakhtenberg, E.; Vasserman, I.; Gluskin, E.] Argonne Natl Lab, Adv Photon Source, 9700 S Cass Ave, Argonne, IL 40439 USA. [Lev, V.; Mezentsev, N.; Syrovatin, V.; Tsukanov, V.] Budker Inst Nucl Phys, Novosibirsk 630090, Russia. RP Ivanyushenkov, Y (reprint author), Argonne Natl Lab, Adv Photon Source, 9700 S Cass Ave, Argonne, IL 40439 USA. EM yury@aps.anl.gov FU U.S. Department of Energy, Office of Science [DE-AC02-06CH11357] FX The authors are thankful to the technical staff from Magnetic Device, Survey and Alignment, Vacuum Systems and Design and Drafting Groups of the Advanced Photon Source for their significant contributions to the success of the project. The work at Argonne was supported by the U.S. Department of Energy, Office of Science, under Contract No. DE-AC02-06CH11357. NR 3 TC 3 Z9 3 U1 1 U2 6 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 425 AR UNSP 032007 DI 10.1088/1742-6596/425/3/032007 PG 4 WC Instruments & Instrumentation; Physics, Applied; Physics, Multidisciplinary SC Instruments & Instrumentation; Physics GA BFL51 UT WOS:000320403700032 ER PT S AU Kaznatcheev, K Chubar, O Keister, JW Idir, M AF Kaznatcheev, K. Chubar, O. Keister, J. W. Idir, M. BE Susini, J Dumas, P TI Optical design of the NSLS-II metrology beamline 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 RAY; RESOLUTION AB The article describes the optical design of the NSLS-II test beamline, dedicated to at-wavelength metrology, in situ surface figuring, crystal optics, radiometry, detectors and instrumentation testing. A key aspect of the beamline design is configuration flexibility, providing as wide as possible range of photon energy, beam size, and divergence, including the optimum trading of SR flux to a required degree of coherence. For this application we propose to use the chromatic properties of compound refractive lens (for hard x-ray) or zone plate (for soft x-ray) to provide band-pass energy filtering and variable spatial coherence. Using such a scheme, it is possible to efficiently vary the transverse coherence from 10 mu m to 10 mm at similar to 1% monochromaticity. The flux extracted permits real-time phase imaging and at-wavelength metrology, even at the bending magnet beamline. C1 [Kaznatcheev, K.; Chubar, O.; Keister, J. W.; Idir, M.] Brookhaven Natl Lab, Photon Sci Directorate, Upton, NY 11973 USA. RP Kaznatcheev, K (reprint author), Brookhaven Natl Lab, Photon Sci Directorate, Upton, NY 11973 USA. EM kaznatch@bnl.gov RI Chubar, Oleg/B-6286-2014 NR 13 TC 0 Z9 0 U1 0 U2 4 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 425 AR UNSP 162009 DI 10.1088/1742-6596/425/16/162009 PG 4 WC Instruments & Instrumentation; Physics, Applied; Physics, Multidisciplinary SC Instruments & Instrumentation; Physics GA BFL51 UT WOS:000320403700231 ER PT S AU Keister, JW Suvorov, A Coburn, DS Cunsolo, A Kodituwakku, CN Stetsko, Y Cai, YQ AF Keister, J. W. Suvorov, A. Coburn, D. S. Cunsolo, A. Kodituwakku, C. N. Stetsko, Y. Cai, Y. Q. BE Susini, J Dumas, P TI Realizing an Analyzer Instrument for Medium-energy Sub-meV IXS 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 AB For the past few years, silicon (800) asymmetric back-diffraction at 9.13 keV has been investigated for use in inelastic x-ray scattering (IXS) analyzer with <1 meV resolution and > 100 mu rad acceptance. While the basic principles have been described and proven, attractive results have become consistently achievable only recently, with particular attention paid to key execution details, including crystal quality (substrate purity, orientation, surface flatness and strain), positioning (resolution, repeatability, and stability of critical axes), thermal environment stability and control, and x-ray diagnostics. While methods for positioning, diagnostics, and thermal stabilization have been refined in our work, crystal quality remains a critical limitation of ultimate performance. An overview of the implementation details is provided in the context of prototype x-ray beam test results collected in preparation for final design of the analyzer instrument to be incorporated into the IXS beamline of NSLS-II. C1 [Keister, J. W.; Suvorov, A.; Coburn, D. S.; Cunsolo, A.; Kodituwakku, C. N.; Stetsko, Y.; Cai, Y. Q.] Brookhaven Natl Lab, Photon Sci Directorate, Upton, NY 11973 USA. RP Keister, JW (reprint author), Brookhaven Natl Lab, Photon Sci Directorate, Upton, NY 11973 USA. EM jkeister@bnl.gov RI Cai, Yong/C-5036-2008 OI Cai, Yong/0000-0002-9957-6426 NR 5 TC 2 Z9 2 U1 0 U2 3 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 425 AR UNSP 052032 DI 10.1088/1742-6596/425/5/052032 PG 4 WC Instruments & Instrumentation; Physics, Applied; Physics, Multidisciplinary SC Instruments & Instrumentation; Physics GA BFL51 UT WOS:000320403700100 ER PT S AU Khounsary, A Kenesei, P Collins, J Navrotski, G Nudell, J AF Khounsary, A. Kenesei, P. Collins, J. Navrotski, G. Nudell, J. BE Susini, J Dumas, P TI High Energy X-ray Micro-tomography for the characterization of thermally fatigued GlidCop specimen 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 MICROTOMOGRAPHY AB The expected increases in the thermal power of X-ray beams produced at the third-generation synchrotron radiation facilities may exceed the heat-load capabilities of the existing high-heat-load components with which the beams interact. An X-ray beam shutter is an example of such components. Typically made of GlidCop, it is used, as needed, to block the X-ray beam from entering the experimental area. Analyses show that the planned 50% increase in storage ring beam current (and thus beam heat load) at the Advanced Photon Source (APS) will result in plastic strain in the shutter limiting its operational life. In order to develop a predictive model to estimate the number of cycles to failure, cooled GlidCop samples were thermally cycled 10,000 times under the high heat load of an X-ray beam from two inline APS undulators. Samples are examined for cracks, and crack size information is extracted for use in the model. In this paper, following some introductory remarks, we report on the characterization of the micron-size fatigue cracks in a sample GlidCop using high-energy X-ray absorption and phase-contrast tomography. It is shown that the current set up at beamline 1-ID at the APS is capable of nondestructive reconstruction of internal structure of the fatigued part with a resolution of 3 mu m, which may further be improved to about 1 mu m. C1 [Khounsary, A.; Kenesei, P.; Collins, J.; Navrotski, G.; Nudell, J.] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. RP Khounsary, A (reprint author), Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. EM amk@aps.anl.gov NR 15 TC 2 Z9 2 U1 0 U2 2 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 425 AR UNSP 212015 DI 10.1088/1742-6596/425/21/212015 PG 7 WC Instruments & Instrumentation; Physics, Applied; Physics, Multidisciplinary SC Instruments & Instrumentation; Physics GA BFL51 UT WOS:000320403700297 ER PT S AU Kujala, NG Macrander, AT Ramanathan, M Dufresne, EM Navrotski, G Marathe, S Assoufid, L Mills, DM Mancini, DC AF Kujala, N. G. Macrander, A. T. Ramanathan, M. Dufresne, E. M. Navrotski, G. Marathe, S. Assoufid, L. Mills, D. M. Mancini, D. C. BE Susini, J Dumas, P TI High-heat-load studies of cryogenically internally cooled silicon double crystal monochromator above and away from cooling channels 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 DE High-heat-load optics; X-ray silicon crystal monochromator; X-ray optics; cryogenic cooling AB High-heat-load studies on Si double crystal monochromator that is internally cooled with liquid nitrogen flow were performed as APS-Upgrade planned to increase ring current to 150 mA. The monochromator consists of two separated Si crystals with diffraction surfaces oriented along (111), diffracting vertically to produce a fixed 35 mm beam offset. Rocking curves were measured for the beam footprint on the first crystal lying both above and away from cooling channels. The beam was produced by two collinear APS undulators type A, each 2.4 m long with 3.3 cm period. Most of the data were obtained for a monochromator set to Bragg diffract at 8 keV for the Si (111) reflection. Through the use of aluminium filters between two sequential ion chambers, we also measured the Si (333) reflection diffracting at 24 keV. We measured the FWHM of rocking curves with either one or both undulators tuned so that the energy of the 1st harmonic matched the Si (111) Bragg energy. Our results show sensitivity to the distance between the beam footprint above and away from cooling channels under high power conditions. C1 [Kujala, N. G.; Macrander, A. T.; Ramanathan, M.; Dufresne, E. M.; Navrotski, G.; Marathe, S.; Assoufid, L.; Mills, D. M.; Mancini, D. C.] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. RP Kujala, NG (reprint author), Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. EM kujala@aps.anl.gov NR 7 TC 0 Z9 0 U1 0 U2 4 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 425 AR UNSP 052006 DI 10.1088/1742-6596/425/5/052006 PG 4 WC Instruments & Instrumentation; Physics, Applied; Physics, Multidisciplinary SC Instruments & Instrumentation; Physics GA BFL51 UT WOS:000320403700074 ER PT S AU Laundy, D Sutter, JP Wagner, UH Rau, C Thomas, CA Sawhney, KJS Chubar, O AF Laundy, D. Sutter, J. P. Wagner, U. H. Rau, C. Thomas, C. A. Sawhney, K. J. S. Chubar, O. BE Susini, J Dumas, P TI Parallel simulations of partially coherent wave front propagation from a finite emittance electron beam 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 AB Hard X-ray undulator radiation at 3rd generation storage rings falls between the geometrical and the fully coherent limit. This is a result of the small but finite emittance of the electron beam source and means that the radiation cannot be completely modelled by incoherent ray tracing or by fully coherent wave propagation. We have developed using the wavefront propagation code Synchrotron Radiation Workshop (SRW) running in a Python environment, a parallel computer program using the Monte Carlo method for modelling the partially coherent emission from electron beam sources taking into account the finite emittance of the source. Using a parallel computing cluster with in excess of 500 cores and each core calculating the wavefront from in excess of a 1000 electrons, a source containing millions of electrons could be simulated. We have applied this method to the Diamond X-ray Imaging and Coherence beamline (113). C1 [Laundy, D.; Sutter, J. P.; Wagner, U. H.; Rau, C.; Thomas, C. A.; Sawhney, K. J. S.] Diamond Light Source, Harwell Sci & Innovat Campus, Didcot OX11 0DE, Oxon, England. [Chubar, O.] Brookhaven Natl Lab, Photon Sci Directorate, Upton, NY 11973 USA. RP Laundy, D (reprint author), Diamond Light Source, Harwell Sci & Innovat Campus, Didcot OX11 0DE, Oxon, England. EM david.laundy@diamond.ac.uk RI Chubar, Oleg/B-6286-2014 NR 6 TC 2 Z9 2 U1 0 U2 4 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 425 AR UNSP 162002 DI 10.1088/1742-6596/425/16/162002 PG 4 WC Instruments & Instrumentation; Physics, Applied; Physics, Multidisciplinary SC Instruments & Instrumentation; Physics GA BFL51 UT WOS:000320403700224 ER PT S AU Potier, J Mercere, P Da Silva, P Idir, M AF Potier, J. Mercere, P. Da Silva, P. Idir, M. BE Susini, J Dumas, P TI Experimental comparison of full and partial coherent illumination in coherent diffraction imaging reconstructions 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 X-RAY CRYSTALLOGRAPHY AB In this paper, we will present coherent diffraction imaging reconstruction of a well-known object by use of a Hybrid Input-Output algorithm. The sample was imaged at 400 nm wavelength with a fully coherent laser source and at 0.41 nm wavelength in partially coherent illumination. The comparison of the two experiments, completed with theoretical simulations, will highlight the influence of the degree of spatial coherence in the reconstruction process. C1 [Potier, J.; Mercere, P.; Da Silva, P.] Synchrotron SOLEIL, BP 48, F-91192 Gif Sur Yvette, France. [Idir, M.] Brookhaven Natl Lab, NSLS 2, Upton, NY USA. RP Potier, J (reprint author), Synchrotron SOLEIL, BP 48, F-91192 Gif Sur Yvette, France. EM potier@synchrotron-soleil.fr NR 11 TC 0 Z9 0 U1 0 U2 3 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 425 AR UNSP 192009 DI 10.1088/1742-6596/425/19/192009 PG 4 WC Instruments & Instrumentation; Physics, Applied; Physics, Multidisciplinary SC Instruments & Instrumentation; Physics GA BFL51 UT WOS:000320403700254 ER PT S AU Rizzi, J Mercere, P Idir, M Guerineau, N Sakat, E Haidar, R Vincent, G Da Silva, P Primot, J AF Rizzi, J. Mercere, P. Idir, M. Guerineau, N. Sakat, E. Haidar, R. Vincent, G. Da Silva, P. Primot, J. BE Susini, J Dumas, P TI X-ray phase contrast imaging using a broadband X-ray beam and a single phase grating used in its achromatic and propagation-invariant regime. 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 LATERAL SHEARING INTERFEROMETRY AB Recently, Onera developed a new interferometer for X-ray phase contrast imaging. This device uses a single phase grating and takes advantage of the incident light spectral bandwidth to create an achromatic and propagation-invariant pattern. This very simple setup produces highly contrasted interferograms after a certain distance of propagation. Our first quantitative images are presented in this paper and the performances of the device are discussed. C1 [Rizzi, J.; Guerineau, N.; Sakat, E.; Haidar, R.; Vincent, G.; Primot, J.] Off Natl Etud & Rech Aerosp, French Aerospace Lab, Chemin Huniere, F-91128 Palaiseau, France. [Mercere, P.; Da Silva, P.] Synchrotron Soleil, F-91192 Gif Sur Yvette, France. [Idir, M.] Brookhaven Natl Lab, NSLS2, Upton, NY 11973 USA. RP Rizzi, J (reprint author), Off Natl Etud & Rech Aerosp, French Aerospace Lab, Chemin Huniere, F-91128 Palaiseau, France. EM Julien.rizzi@onera.fr RI VINCENT, Gregory/A-8140-2012 OI VINCENT, Gregory/0000-0003-1636-3853 FU Triangle de la Physique and by the US Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC-02-98CH10886] FX The research presented here is supported by Triangle de la Physique and by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, under contract No. DE-AC-02-98CH10886. NR 11 TC 4 Z9 4 U1 0 U2 6 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 425 AR UNSP 192002 DI 10.1088/1742-6596/425/19/192002 PG 4 WC Instruments & Instrumentation; Physics, Applied; Physics, Multidisciplinary SC Instruments & Instrumentation; Physics GA BFL51 UT WOS:000320403700247 ER PT S AU Sanchez-Hanke, C Hulbert, SL Shapiro, D Reininger, R AF Sanchez-Hanke, C. Hulbert, S. L. Shapiro, D. Reininger, R. BE Susini, J Dumas, P TI High coherent flux at the NSLS-II coherent soft x-ray beamline 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 AB The optical design of the coherent soft x-ray (CSX) and fast polarization switching beamline at NSLS-II has been optimized to deliver photon flux in the range of 10(12) - 10(13) ph/s in the energy range from 200 to 2000 eV. Two identical APPLE-II undulators will be operated in two different modes: canted and phased. In the canted mode, one beam will be directed to the coherence branch and the other to the fast polarization switching branch. In the phased mode, the two undulators will be operated as a single device to deliver the highest coherence flux to the coherence branch. The monochromator for the coherence branch is a focusing variable line spacing plane grating monochromator designed to deliver a moderate resolving power (2000 to 3000). The horizontal focusing onto the exit slit will be performed with a cylindrical bendable mirror located downstream of the monochromator and having similar demagnification as the monochromator. C1 [Sanchez-Hanke, C.; Hulbert, S. L.; Shapiro, D.; Reininger, R.] Brookhaven Natl Lab, NSLS 2, Upton, NY 11973 USA. RP Sanchez-Hanke, C (reprint author), Brookhaven Natl Lab, NSLS 2, Upton, NY 11973 USA. EM hanke@bnl.gov NR 8 TC 0 Z9 0 U1 0 U2 8 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 425 AR UNSP 152017 DI 10.1088/1742-6596/425/15/152017 PG 4 WC Instruments & Instrumentation; Physics, Applied; Physics, Multidisciplinary SC Instruments & Instrumentation; Physics GA BFL51 UT WOS:000320403700217 ER PT S AU Schmah, A AF Schmah, Alexander CA STAR Collaboration BE Susini, J Dumas, P TI The Beam Energy Scan at RHIC: Recent Results from STAR 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 AB The first phase of the beam energy scan (BES) program at RHIC was successfully completed in the years 2010 and 2011. The main goals are the search for the QCD critical point and to find signatures for a phase transition between the hadron gas and the QGP phase. For this purpose several observables like higher moments of net-proton distributions, RCP of charged hadrons or the elliptic flow v(2) are studied. Further new observations and results like the centrality dependence of chemical freeze-out parameters (T-ch and mu B) or di-electron spectra in comparison with model calculations are discussed. C1 [Schmah, Alexander; STAR Collaboration] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Schmah, A (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, 1 Cyclotron Rd, Berkeley, CA 94720 USA. EM aschmah@lbl.gov NR 15 TC 0 Z9 0 U1 0 U2 2 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 425 AR UNSP 012007 DI 10.1088/1742-6596/426/1/012007 PG 5 WC Instruments & Instrumentation; Physics, Applied; Physics, Multidisciplinary SC Instruments & Instrumentation; Physics GA BFL51 UT WOS:000320403700007 ER PT S AU Shapiro, D Roy, S Celestre, R Chao, W Doering, D Howells, M Kevan, S Kilcoyne, D Kirz, J Marchesini, S Seu, KA Schirotzek, A Spence, J Tyliszczak, T Warwick, T Voronov, D Padmore, HA AF Shapiro, D. Roy, S. Celestre, R. Chao, W. Doering, D. Howells, M. Kevan, S. Kilcoyne, D. Kirz, J. Marchesini, S. Seu, K. A. Schirotzek, A. Spence, J. Tyliszczak, T. Warwick, T. Voronov, D. Padmore, H. A. BE Susini, J Dumas, P TI Development of coherent scattering and diffractive imaging and the COSMIC facility at the Advanced Light Source 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 AB A new facility is described that is being constructed for coherent scattering and microscopy at the Advanced Light Source. The undulator beamline delivers maximum coherent flux to two experiment programs. One is for soft x-ray coherent scattering and correlation studies, the other is for soft x-ray diffractive imaging using ptychographic reconstruction techniques. The energy resolution is sufficient for NEXAFS spectroscopy with full polarization control, from below the carbon edge to 2500eV. New instrumentation is planned for wavelength limited 2D imaging and 3D imaging at spatial resolution better than 10nm and for coherent scattering studies with a variety of sample environments including strong magnetic fields and cryogenic temperatures. High speed CCD detectors will make optimum use of the available flux on dedicated data transmission networks. C1 [Shapiro, D.; Roy, S.; Celestre, R.; Doering, D.; Howells, M.; Kevan, S.; Kilcoyne, D.; Kirz, J.; Marchesini, S.; Seu, K. A.; Schirotzek, A.; Tyliszczak, T.; Warwick, T.; Voronov, D.; Padmore, H. A.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. [Chao, W.] Ctr X ray Opt, Berkeley, CA 94720 USA. [Spence, J.] Arizona State Univ, Dept Phys, Tempe, AZ 85287 USA. RP Shapiro, D (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. EM warwick@lbl.gov RI Kevan, Stephen/F-6415-2010 OI Kevan, Stephen/0000-0002-4621-9142 NR 7 TC 1 Z9 1 U1 1 U2 7 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 425 AR UNSP 192011 DI 10.1088/1742-6596/425/19/192011 PG 4 WC Instruments & Instrumentation; Physics, Applied; Physics, Multidisciplinary SC Instruments & Instrumentation; Physics GA BFL51 UT WOS:000320403700256 ER PT S AU Shu, D Kearney, S Preissner, C AF Shu, D. Kearney, S. Preissner, C. BE Susini, J Dumas, P TI Design of a precision flexural linear stage system with sub-nanometer resolution and 12-mm travel range 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 AB Precision ball-bearing-based or roller-bearing-based positioning stage systems are capable of providing a large travel range. However, it is not possible to meet requirements in sub-nanometer positioning resolution, high tilting stiffness, and microradian-level straightness of trajectory repeatability with a simple rolling element guiding system. To meet those requirements and still allow for large travel range, we have designed a novel precision flexural linear stage. It is capable of sub-nanometer positioning resolution and 12-mm travel range for synchrotron radiation instrumentation applications. The design and preliminary test results for a prototype stage system are discussed in this paper. C1 [Shu, D.; Kearney, S.; Preissner, C.] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. RP Shu, D (reprint author), Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. EM shu@aps.anl.gov NR 4 TC 2 Z9 2 U1 0 U2 3 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 425 AR UNSP 212011 DI 10.1088/1742-6596/425/21/212011 PG 4 WC Instruments & Instrumentation; Physics, Applied; Physics, Multidisciplinary SC Instruments & Instrumentation; Physics GA BFL51 UT WOS:000320403700293 ER PT S AU Shu, D Stoupin, S Khachatryan, R Goetze, KA Roberts, T Mundboth, K Collins, S Shvyd'ko, Y AF Shu, D. Stoupin, S. Khachatryan, R. Goetze, K. A. Roberts, T. Mundboth, K. Collins, S. Shvyd'ko, Y. BE Susini, J Dumas, P TI Precision mechanical design of an ultrahigh-resolution inelastic x-ray scattering spectrometer system with CDFDW optics at the APS 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 AB There are many scientific applications, especially involving topics related to the equilibrium atomic-scale dynamics of condensed matter, that require both a narrower and a steeper resolution function and access to a broader dynamic range than are currently available. To meet these important scientific needs, a prototype of a novel ultrahigh-resolution inelastic x-ray scattering spectrometer system has been designed and constructed at undulator-based beamline 30-ID at the Advanced Photon Source, Argonne National Laboratory. This prototype is designed to meet challenging mechanical and optical specifications for performing so-called CDFDW angular-dispersive x-ray crystal optics, which include a central ultra-thin CFW crystal and a pair of dispersing elements. The abbreviation CDFDW stands for: C - collimating crystal, D - dispersing-element crystal (two D-crystals are used in each CDFDW), F - anomalous transmission filter, and W - wavelength-selector crystal [1]. The mechanical design of the ultrahigh-resolution inelastic x-ray scattering spectrometer, as well as the preliminary test results of its precision positioning performance are presented in this paper. C1 [Shu, D.; Stoupin, S.; Khachatryan, R.; Goetze, K. A.; Roberts, T.; Shvyd'ko, Y.] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. [Mundboth, K.; Collins, S.] Diamond Light Source Ltd, Didcot OX11 0DE, Oxon, England. RP Shu, D (reprint author), Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. EM shu@aps.anl.gov FU U.S. Department of Energy, Office of Science [DE-AC02-06CH11357] FX The authors would like to thank R. Ranay, T. Buffington from Argonne National Laboratory, and S. Kearney and J. Anton from Argonne National Laboratory and the University of Illinois at Chicago for their help with the CDFDW-optics-based IXS spectrometer prototype development. The authors would also like to thank L. Young for supporting this project and stimulating interest. This work was supported by the U.S. Department of Energy, Office of Science, under Contract No. DE-AC02-06CH11357. 11th International Conference on Synchrotron Radiation Instrumentation (SRI 2012) IOP Publishing Journal of Physics: Conference Series 425 (2013) 052031 doi:10.1088/1742-6596/425/5/052031 NR 10 TC 4 Z9 4 U1 1 U2 1 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 425 AR UNSP 052031 DI 10.1088/1742-6596/425/5/052031 PG 4 WC Instruments & Instrumentation; Physics, Applied; Physics, Multidisciplinary SC Instruments & Instrumentation; Physics GA BFL51 UT WOS:000320403700099 ER PT S AU Shu, D Shvyd'ko, Y Amann, J Emma, P Stoupin, S Quintana, J AF Shu, D. Shvyd'ko, Y. Amann, J. Emma, P. Stoupin, S. Quintana, J. BE Susini, J Dumas, P TI Design of a diamond-crystal monochromator for the LCLS hard x-ray self-seeding project 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 AB As the result of collaborations between the Advanced Photon Source (APS), Argonne National Laboratory, and the Linac Coherent Light Source (LCLS) at SLAC National Accelerator Laboratory, we have designed and constructed a diamond crystal monochromator for the LCLS hard x-ray self-seeding project. The novel monochromator is ultrahigh-vacuum compatible to meet the LCLS linear accelerator vacuum environmental requirement. A special graphite holder was designed for strain-free mount of the 110-mu m thin synthetic diamond crystal plate provided by Technological Institute for Super-hard and Novel Carbon Materials of Russia (TISNCM). An in-vacuum multi-axis precision positioning mechanism is designed to manipulate the thin-film diamond holder with resolutions and stabilities required by the hard x-ray self-seeding physics. Optical encoders, limit switches, and hardware stops are established in the mechanism to ensure system reliability and to meet the accelerator personal and equipment safety interlock requirements. Molybdenum shields are installed in the monochromator to protect the encoders and associated electronics from radiation damage. Mechanical specifications, designs, and preliminary test results of the diamond monochromator are presented in this paper. C1 [Shu, D.; Shvyd'ko, Y.; Stoupin, S.; Quintana, J.] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. [Amann, J.; Emma, P.] SLAC Natl Accelerator Lab, Linac Coherent Light Source, Menlo Pk, CA 94025 USA. RP Shu, D (reprint author), Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. EM shu@aps.anl.gov FU U.S. Department of Energy, Office of Science [DEAC02-06CH11357] FX The authors would like to thank A. Zholents, W. Berg, R. Ranay, and T. Buffington from Argonne National Laboratory, S. Kearney and J. Anton from Argonne National Laboratory and the University of Illinois at Chicago, J. Hastings, Y. Feng, H. Huang, and engineers in the LCLS HXRSS team from SLAC National Accelerator Laboratory for their help with the monochromator development, This work was supported by the U.S. Department of Energy, Office of Science, under Contract No. DEAC02-06CH11357. NR 4 TC 11 Z9 11 U1 1 U2 5 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 425 AR UNSP 052004 DI 10.1088/1742-6596/425/5/052004 PG 4 WC Instruments & Instrumentation; Physics, Applied; Physics, Multidisciplinary SC Instruments & Instrumentation; Physics GA BFL51 UT WOS:000320403700072 ER PT S AU Shu, D Kuan, CK Sheng, IC Chen, JR AF Shu, D. Kuan, C-K Sheng, I. C. Chen, J-R BE Susini, J Dumas, P TI Development of an x-ray beam position monitor for TPS EPU beamline front ends 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 AB In order to develop state-of-the-art x-ray beam position monitors (XBPMs) for the Taiwan Photon Source (TPS) project, the National Synchrotron Radiation Research Center (NSRRC) and the Advance Photon Source have established a collaboration project to design and test various XBPMs for the TPS beamline front ends. One of the XBPM prototypes is dedicated to the elliptically polarized undulator (EPU) beamline front ends to be constructed at the TPS. In this paper, we present the design of the XBPM prototype. Preliminary test results for the prototype are also discussed. C1 [Shu, D.] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. [Kuan, C-K; Sheng, I. C.; Chen, J-R] Natl Synchrotron Radiat Res Ctr, Hsinchu 30076, Taiwan. RP Shu, D (reprint author), Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. EM shu@aps.anl.gov FU U.S. Department of Energy, Office of Science [DE-AC02-06CH11357] FX The authors would like to thank Shih-Chun Chung, Hok-Sum Fung, Jyun Yan Jhuang, Po-An Lin, Bor-Yuan Shew, Cheng-Hao Ko, and Ching-Shiang Hwang from NSRRC. R. Raney from ANL, and S. Kearney from ANL and the University of Illinois at Chicago for their help with the XBPM development. This work was supported by the U.S. Department of Energy, Office of Science, under Contract No. DE-AC02-06CH11357. NR 4 TC 0 Z9 0 U1 0 U2 3 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 425 AR UNSP 042003 DI 10.1088/1742-6596/425/4/042003 PG 4 WC Instruments & Instrumentation; Physics, Applied; Physics, Multidisciplinary SC Instruments & Instrumentation; Physics GA BFL51 UT WOS:000320403700052 ER PT S AU Stepanov, S Hilgart, M Makarov, O Pothineni, SB Yoder, D Ogata, C Sanishvili, R Venugopalan, N Becker, M Clift, M Smith, JL Fischetti, RF AF Stepanov, S. Hilgart, M. Makarov, O. Pothineni, S. B. Yoder, D. Ogata, C. Sanishvili, R. Venugopalan, N. Becker, M. Clift, M. Smith, J. L. Fischetti, R. F. BE Susini, J Dumas, P TI JBluIce-EPICS: a fast and flexible open-source beamline control system for macromolecular crystallography 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 AB This paper overviews recent advances in the JBluIce-EPICS open-source control system designed at the macromolecular crystallography beamlines of the National Institute of General Medical Sciences and National Cancer Institute at the Advanced Photon Source (GM/CA@APS). We discuss some technical highlights of this system distinguishing it from the competition, such as reduction of software layers to only two, possibility to operate JBluIce in parallel with other beamline controls, plugin-enabled architecture where the plugins can be written in any programming language, and utilization of the whole power of the Java integrated development environment in the Graphical User Interface. Then, we demonstrate how these highlights help to make JBluIce fast, easily adaptable to new beamline developments, and intuitive for users. In particular, we discuss several recent additions to the system including a bridge between crystal rastering and data collection, automatic detection of raster polygons from optical crystal centering, background data processing, and a pathway to a fully automated pipeline from crystal screening to solving crystal structure. C1 [Stepanov, S.; Hilgart, M.; Makarov, O.; Pothineni, S. B.; Yoder, D.; Ogata, C.; Sanishvili, R.; Venugopalan, N.; Becker, M.; Smith, J. L.; Fischetti, R. F.] Argonne Natl Lab, Adv Photon Source, GM CA Struct Biol Facil, Argonne, IL 60439 USA. [Clift, M.] Australian Synchrotron, Clayton, Vic 3168, Australia. [Smith, J. L.] Univ Michigan, Dept Biol Chem, Inst Life Sci, Ann Arbor, MI 48109 USA. RP Stepanov, S (reprint author), Argonne Natl Lab, Adv Photon Source, GM CA Struct Biol Facil, Argonne, IL 60439 USA. EM sstepanov@anl.gov FU National Cancer Institute [Y1-CO-1020]; National Institute of General Medical Sciences [Y1-GM-1104]; US Department of Energy, Basic Energy Sciences, Office of Science [DE-AC02-06CH1135] FX GM/CA@APS is supported in whole or in part by Federal funds from the National Cancer Institute (Y1-CO-1020) and the National Institute of General Medical Sciences (Y1-GM-1104). Use of the Advanced Photon Source was supported by the US Department of Energy, Basic Energy Sciences, Office of Science under contract No. DE-AC02-06CH1135. NR 10 TC 0 Z9 0 U1 0 U2 1 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 425 AR UNSP 012019 DI 10.1088/1742-6596/425/1/012019 PG 4 WC Instruments & Instrumentation; Physics, Applied; Physics, Multidisciplinary SC Instruments & Instrumentation; Physics GA BFL51 UT WOS:000320403700019 ER PT S AU Stepanov, S AF Stepanov, Sergey BE Susini, J Dumas, P TI Cybersecurity, massive data processing, community interaction, and other developments at WWW-based computational X-ray Server 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 DIFFRACTION; SOFTWARE AB X-Ray Server (x-server.gmca.aps.anl.gov) is a WWW-based computational server for modeling of X-ray diffraction, reflection and scattering data. The modeling software operates directly on the server and can be accessed remotely either from web browsers or from user software. In the later case the server can be deployed as a software library or a data fitting engine. As the server recently surpassed the milestones of 15 years online and 1.5 million calculations, it accumulated a number of technical solutions that are discussed in this paper. The developed approaches to detecting physical model limits and user calculations failures, solutions to spam and firewall problems, ways to involve the community in replenishing databases and methods to teach users automated access to the server programs may be helpful for X-ray researchers interested in using the server or sharing their own software online. C1 Argonne Natl Lab, Adv Photon Source, GM CA Struct Biol Facil, Argonne, IL 60439 USA. RP Stepanov, S (reprint author), Argonne Natl Lab, Adv Photon Source, GM CA Struct Biol Facil, Argonne, IL 60439 USA. EM sstepanov@anl.gov NR 5 TC 0 Z9 0 U1 0 U2 2 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 425 AR UNSP 162006 DI 10.1088/1742-6596/425/16/162006 PG 5 WC Instruments & Instrumentation; Physics, Applied; Physics, Multidisciplinary SC Instruments & Instrumentation; Physics GA BFL51 UT WOS:000320403700228 ER PT S AU Voronov, DL Anderson, EH Cambie, R Gawlitza, P Goray, LI Gullikson, EM Salmassi, F Warwick, T Yashchuk, VV Padmore, HA AF Voronov, D. L. Anderson, E. H. Cambie, R. Gawlitza, P. Goray, L. I. Gullikson, E. M. Salmassi, F. Warwick, T. Yashchuk, V. V. Padmore, H. A. BE Susini, J Dumas, P TI Development of near atomically perfect diffraction gratings for EUV and soft x-rays with very high efficiency and resolving power 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 EXTREME-ULTRAVIOLET; MULTILAYER AB Multilayer-coated Blazed Gratings (MBG) can offer high diffraction efficiency in a very high diffraction order and are therefore of great interest for high-resolution EUV and soft x-ray spectroscopy techniques such as Resonance Inelastic X-ray Scattering. However, realization of the MBG concept requires nano-scale precision in fabrication of a saw-tooth substrate with atomically smooth facets, and reproduction of the blazed groove profile in the course of conformal growth of a multilayer coating. We report on recent progress achieved in the development, fabrication, and characterization of ultra-dense MBGs for EUV and soft x-rays. As a result of thorough optimization of all steps of the fabrication process, an absolute diffraction efficiency as high as 44% and 12.7% was achieved for a 5250 l/mm grating in the EUV and soft x-ray regions respectively. This work now shows a direct route to achieving high diffraction efficiency in high order at wavelengths throughout the soft x-ray energy range with revolutionary applications in synchrotron science. C1 [Voronov, D. L.; Anderson, E. H.; Cambie, R.; Gullikson, E. M.; Salmassi, F.; Warwick, T.; Yashchuk, V. V.; Padmore, H. A.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, 1 Cyclotron Rd, Berkeley, CA 94720 USA. [Gawlitza, P.] Fraunhofer Inst Mat & Beam Technol, D-01277 Dresden, Germany. [Goray, L. I.] St Petersburg Acad Univ, St Petersburg 194021, Russia. RP Voronov, DL (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, 1 Cyclotron Rd, Berkeley, CA 94720 USA. EM dlvoronov@lbl.gov RI Goray, Leonid/D-4426-2013 OI Goray, Leonid/0000-0002-0381-9607 FU US Department of Energy [DEAC02-05CH11231] FX The work was supported by the US Department of Energy under contract number DEAC02-05CH11231. NR 9 TC 2 Z9 2 U1 3 U2 6 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 425 AR UNSP 152006 DI 10.1088/1742-6596/425/15/152006 PG 4 WC Instruments & Instrumentation; Physics, Applied; Physics, Multidisciplinary SC Instruments & Instrumentation; Physics GA BFL51 UT WOS:000320403700206 ER PT S AU Ward, MJ Regier, TZ Vogt, JM Gordon, RA Han, WQ Sham, TK AF Ward, M. J. Regier, T. Z. Vogt, J. M. Gordon, R. A. Han, W-Q Sham, T. K. BE Susini, J Dumas, P TI Time-resolved X-ray excited optical luminescence using an optical streak camera 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 AB We report the development of a time-resolved XEOL (TR-XEOL) system that employs an optical streak camera. We have conducted TR-XEOL experiments at the Canadian Light Source (CLS) operating in single bunch mode with a 570 ns dark gap and 35 ps electron bunch pulse, and at the Advanced Photon Source (APS) operating in top-up mode with a 153 ns dark gap and 33.5 ps electron bunch pulse. To illustrate the power of this technique we measured the TR-XEOL of solid-solution nanopowders of gallium nitride - zinc oxide, and for the first time have been able to resolve near-band-gap (NBG) optical luminescence emission from these materials. Herein we will discuss the development of the streak camera TR-XEOL technique and its application to the study of these novel materials. C1 [Ward, M. J.; Sham, T. K.] Univ Western Ontario, Dept Chem, London, ON N6A 5B7, Canada. [Regier, T. Z.; Vogt, J. M.; Gordon, R. A.] Canadian Light Source Inc, Saskatoon, SK S7N 0X4, Canada. [Gordon, R. A.] Pacific Nortwestern Consortium Adv Photo Source, Argonne, IL 60439 USA. [Han, W-Q] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. RP Ward, MJ (reprint author), Univ Western Ontario, Dept Chem, London, ON N6A 5B7, Canada. EM tsham@uwo.ca FU US Department of Energy (DOE) - Basic Energy Sciences; NSERC; University of Washington; CLS; APS; U.S. DOE [DE-AC02-06CH11357]; NRC; CIHR; Province of Saskatchewan; Western Economic Diversification Canada; University of Saskatchewan; University of Western Ontario; CRC; CFI; OIT; Center for Functional Nanomaterials; Brookhaven National Laboratory; Office of Basic Energy Sciences [DE-AC0298CH10886]; QEIIGSST; OGS FX PNC/XSD facilities at the APS, and research at these facilities, are supported by the US Department of Energy (DOE) - Basic Energy Sciences, a Major Resources Support grant from NSERC, the University of Washington, the CLS, and the APS. Use of the APS was supported by the U.S. DOE under Contract No. DE-AC02-06CH11357. Research at the CLS was supported by the NSERC, NRC, CIHR, the Province of Saskatchewan, Western Economic Diversification Canada, and the University of Saskatchewan. Research at The University of Western Ontario was supported by NSERC, CRC, CFI, and OIT. Research carried out at the Center for Functional Nanomaterials, Brookhaven National Laboratory, was supported by the U.S. DOE, Office of Basic Energy Sciences, under contract No. DE-AC0298CH10886. M.J.W. acknowledges the financial support of the QEIIGSST and OGS scholarship programs. We thank Dale Brewe for assistance with the timing setup at 20BM PNC/XSD. NR 9 TC 0 Z9 0 U1 0 U2 8 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 425 DI 10.1088/1742-6596/425/9/092006 PG 4 WC Instruments & Instrumentation; Physics, Applied; Physics, Multidisciplinary SC Instruments & Instrumentation; Physics GA BFL51 UT WOS:000320403700151 ER PT S AU Yashchuk, VV Merthe, DJ Goldberg, KA Artemiev, NA Celestre, R Domning, EE Kunz, M McKinney, WR Morrison, GY Smith, BV Tamura, N AF Yashchuk, V. V. Merthe, D. J. Goldberg, K. A. Artemiev, N. A. Celestre, R. Domning, E. E. Kunz, M. McKinney, W. R. Morrison, G. Y. Smith, B. V. Tamura, N. BE Susini, J Dumas, P TI Experimental methods for optimal tuning of bendable mirrors for diffraction-limited soft x-ray focusing 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 METROLOGY AB We report on hands-on experimental methods developed at the Advanced Light Source (ALS) for optimal tuning of mechanically bendable x-ray mirrors for diffraction-limited soft x-ray nano-focusing. For ex situ tuning of the benders for optimal beam-line performance, we use a revised version of the method of characteristic functions recently developed at the ALS optical metrology laboratory. At-wavelength optimal tuning of bendable optics consists of a series of wavefront-sensing tests with increasing accuracy and sensitivity, including modified scanning-slit Hartmann tests. The methods have been experimentally validated at ALS test beamline 5.3.1 and the micro-diffraction beamline 12.3.2 in applications to optimally set bendable Kirkpatrick-Baez mirrors designed for sub-micron focusing. C1 [Yashchuk, V. V.; Merthe, D. J.; Artemiev, N. A.; Celestre, R.; Kunz, M.; McKinney, W. R.; Tamura, N.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. [Goldberg, K. A.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Ctr for X ray Opt, Berkeley, CA 94720 USA. [Domning, E. E.; Morrison, G. Y.; Smith, B. V.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Engn, Berkeley, CA 94720 USA. RP Yashchuk, VV (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. EM VVYashchuk@lbl.gov RI McKinney, Wayne/F-2027-2014 OI McKinney, Wayne/0000-0003-2586-3139 FU Director, Office of Science; Office of Basic Energy Sciences; Material Science Division; U.S. Department of Energy [DE-AC02-05CH11231] FX The Advanced Light Source is supported by the Director, Office of Science, Office of Basic Energy Sciences, Material Science Division, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231 at Lawrence Berkeley National Laboratory. NR 11 TC 6 Z9 6 U1 0 U2 3 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 425 AR UNSP 152003 DI 10.1088/1742-6596/425/15/152003 PG 4 WC Instruments & Instrumentation; Physics, Applied; Physics, Multidisciplinary SC Instruments & Instrumentation; Physics GA BFL51 UT WOS:000320403700203 ER PT S AU Yashchuk, VV Morrison, GY Church, M Artemiev, NA Celestre, R Domning, EE Howells, M Kunz, M McKinney, WR Merthe, DJ Smith, BV Tamura, N Padmore, HA AF Yashchuk, V. V. Morrison, G. Y. Church, M. Artemiev, N. A. Celestre, R. Domning, E. E. Howells, M. Kunz, M. McKinney, W. R. Merthe, D. J. Smith, B. V. Tamura, N. Padmore, H. A. BE Susini, J Dumas, P TI Bendable Kirkpatrick-Baez mirrors for the ALS micro-diffraction beamline 12.3.2: optimal tuning and alignment for multiple focusing geometries 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 AB Using an example of Kirkpatrick-Baez mirrors for the micro-diffraction beamline 12.3.2, we present the recent development of bendable x-ray optics and experimental techniques used for focusing of beams of soft and hard x-rays at the Advanced Light Source (ALS). We briefly review the nature of the bending and analyze a generalized solution of the bending equation for a side-profiled elliptically bent mirror substrate. A scaling rule is derived to understand a range of reliable tunability of the bendable optics for different applications (e.g., different focal distances and grazing incidence angles). Original design approaches are developed for assembly of bendable mirrors with minimal spurious stress and misalignment and for final precision compensation of the residual stress, substrate twist, and roll-off misalignment of the mirrors. Procedures used for optimal shaping and alignment of bendable optics at the ALS optical metrology laboratory are also briefly reviewed. C1 [Yashchuk, V. V.; Church, M.; Artemiev, N. A.; Celestre, R.; Howells, M.; Kunz, M.; McKinney, W. R.; Merthe, D. J.; Tamura, N.; Padmore, H. A.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. [Morrison, G. Y.; Domning, E. E.; Smith, B. V.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Engn, Berkeley, CA 94720 USA. RP Yashchuk, VV (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. EM VVYashchuk@lbl.gov RI McKinney, Wayne/F-2027-2014 OI McKinney, Wayne/0000-0003-2586-3139 FU Director, Office of Science, Office of Basic Energy Sciences; Material Science Division; U.S. Department of Energy [DE-AC02-05CH11231] FX The Advanced Light Source is supported by the Director, Office of Science, Office of Basic Energy Sciences, Material Science Division, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231 at Lawrence Berkeley National Laboratory. NR 10 TC 4 Z9 4 U1 1 U2 7 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 425 AR UNSP 152004 DI 10.1088/1742-6596/425/15/152004 PG 4 WC Instruments & Instrumentation; Physics, Applied; Physics, Multidisciplinary SC Instruments & Instrumentation; Physics GA BFL51 UT WOS:000320403700204 ER PT S AU Gaur, A Shrivastava, BD Khalid, S AF Gaur, A. Shrivastava, B. D. Khalid, S. BE Wu, ZY TI Study of XAFS spectroscopic methods of speciation using mixtures of Cu(I) and Cu(II) chlorides SO 15TH INTERNATIONAL CONFERENCE ON X-RAY ABSORPTION FINE STRUCTURE (XAFS15) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 15th International Conference on X-Ray Absorption Fine Structure (XAFS) CY JUL 22-28, 2012 CL Beijing, PEOPLES R CHINA SP Chinese Acad Sci (CAS), Natl Nat Sci Fdn China (NSFC), China Ctr Adv Sci & Technol World Lab, Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Chinese Acad Sci, Inst High Energy Phys, AREVA, Xian Act Power Elect Co, Ltd ID COPPER; OXIDATION; STATE AB Speciation concerns determination of the chemical forms along with the relative quantities of the different species in a given sample. The aim of the present work is to make a comparative study of the different methods of speciation using X-ray absorption fine structure (XAFS) spectroscopy. For this purpose, mixtures have been prepared by mixing CuCl2 and CuCl in different proportions. The X-ray absorption spectra have been recorded at the copper K-edge in the mixtures and the two chlorides separately. The different characteristic features of the XANES spectra of the two chlorides, useful for speciation, have been identified. Firstly, Principal component analysis (PCA) and target transformation (TT) methods have been used to check the number and identity of components in the mixtures. After the identification of the components, the percentages of the species in the mixtures have been quantitatively determined by linear combination fitting (LCF) of XANES, derivative XANES, and EXAFS (k(3)chi and k(2)chi) spectra. The other methods of speciation which have been employed are normalized difference absorption edge spectra analysis (NDAES), methods based on derivative XANES spectra of species and the method based on the relative position of the absorption edge. Results obtained from these methods have been compared and their relative merits discussed. It is probably for the first time that such a study has been done. The first section in your paper C1 [Gaur, A.; Shrivastava, B. D.] Vikram Univ, Sch Studies Phys, Ujjain 456010, Madhya Pradesh, India. [Khalid, S.] Brookhaven Natl Lab, NSLS, Upton, NY 11973 USA. RP Gaur, A (reprint author), Vikram Univ, Sch Studies Phys, Ujjain 456010, Madhya Pradesh, India. EM abhijeetgaur9@gmail.com FU Madhya Pradesh Council of Science & Technology (MPCST), Bhopal (India) FX Thanks are due to Madhya Pradesh Council of Science & Technology (MPCST), Bhopal (India) for a research grant. NR 9 TC 3 Z9 3 U1 1 U2 12 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 430 AR UNSP 012045 DI 10.1088/1742-6596/430/1/012045 PG 4 WC Physics, Condensed Matter; Spectroscopy SC Physics; Spectroscopy GA BFM11 UT WOS:000320464300045 ER PT S AU Heald, S Alshammari, MS Alfehaid, S Alotaibi, M Feng, Q Hakimi, AMHR AF Heald, Steve Alshammari, Marzook S. Alfehaid, S. Alotaibi, M. Feng, Qi Hakimi, A. M. H. R. BE Wu, ZY TI XAFS Study of metal-doped In2O3 SO 15TH INTERNATIONAL CONFERENCE ON X-RAY ABSORPTION FINE STRUCTURE (XAFS15) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 15th International Conference on X-Ray Absorption Fine Structure (XAFS) CY JUL 22-28, 2012 CL Beijing, PEOPLES R CHINA SP Chinese Acad Sci (CAS), Natl Nat Sci Fdn China (NSFC), China Ctr Adv Sci & Technol World Lab, Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Chinese Acad Sci, Inst High Energy Phys, AREVA, Xian Act Power Elect Co, Ltd ID THIN-FILMS AB In2O3 has attracted interest recently because of its favorable properties for potential applications as diluted magnetic semiconductors. For these applications the material must be doped to produce the desired magnetic properties, and it is essential to determine the fate of the dopants in order to optimize the materials and understand the magnetic measurements. This paper summarizes some recent XAFS studies of a series of In2O3 films doped with V, Cr, Co, and Fe. XAFS is shown to be a powerful tool to characterize these materials, providing valence information, and detecting both substitutional doping as well as second phase formation. V and Cr are found to take up well ordered substitutional sites with no evidence for second phase formation. For Co the substitutional sites were much more disordered than for V or Cr. Fe doped samples also displayed a range of results with well-ordered substitutional sites in some samples, while others showed extensive second phase formation including magnetite and Fe metal. C1 [Heald, Steve] Argonne Natl Lab, Xray Sci Div, 9700 S Cass Ave, Argonne, IL 60439 USA. [Alshammari, Marzook S.; Alfehaid, S.; Alotaibi, M.] KACST, Natl Ctr Nanotechnol, Riyadh 11442, Saudi Arabia. [Alshammari, Marzook S.; Feng, Qi] Univ Sheffield, Dept Phys & Astron, Sheffield S10 2TN, S Yorkshire, England. [Hakimi, A. M. H. R.] Univ Cambridge, Dept Mat Sci & Met, Cambridge CB2 1TN, England. RP Heald, S (reprint author), Argonne Natl Lab, Xray Sci Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM heald@aps.anl.gov FU U.S. DOE [DE-AC02-06CH11357]; UK Engineering and Physical Sciences Research Council; KACST (Saudi Arabia) FX Use of the Advanced Photon Source, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science by Argonne National Laboratory, was supported by the U.S. DOE under Contract No. DE-AC02-06CH11357.This research was also funded by the UK Engineering and Physical Sciences Research Council and also KACST (Saudi Arabia). NR 8 TC 3 Z9 3 U1 3 U2 9 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 430 AR UNSP 012081 DI 10.1088/1742-6596/430/1/012081 PG 4 WC Physics, Condensed Matter; Spectroscopy SC Physics; Spectroscopy GA BFM11 UT WOS:000320464300081 ER PT S AU Newville, M AF Newville, Matthew BE Wu, ZY TI Larch: An Analysis Package for XAFS and Related Spectroscopies SO 15TH INTERNATIONAL CONFERENCE ON X-RAY ABSORPTION FINE STRUCTURE (XAFS15) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 15th International Conference on X-Ray Absorption Fine Structure (XAFS) CY JUL 22-28, 2012 CL Beijing, PEOPLES R CHINA SP Chinese Acad Sci, Natl Nat Sci Fdn China, China Ctr Adv Sci & Technol World Lab, Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Chinese Acad Sci, Inst High Energy Phys, AREVA, Xian Act Power Elect Co, Ltd ID RAY-ABSORPTION SPECTROSCOPY; IN-SITU; SPECTRA; DETECTOR; IFEFFIT; FEFF AB LARCH, a package of analysis tools for XAFS and related spectroscopies is presented. A complete rewrite of the IFEFFIT package, the initial release of LARCH preserves the core XAFS analysis procedures such as normalization, background subtraction, Fourier transforms, fitting of XANES spectra, and fitting of experimental spectra to a sum of FEFF Paths, with few algorithmic changes made in comparison to IFEFFIT. LARCH is written using Python and its packages for scientific programming, which gives significant improvements over IFEFFIT in the ability to handle multi-dimensional and large data sets, write complex analysis scripts, visualize data, add new functionality, and customize existing capabilities. Like the earlier version, LARCH can run from an interactive command line or in batch-mode, but LARCH can also be run as a server and accessed from clients using standard inter-process communication techniques available in a variety of computer languages. LARCH is freely available under an open source license. Examples of using LARCH are shown, future directions for development are discussed, and collaborations for adding new capabilities are actively sought. C1 Univ Chicago, Ctr Adv Radiat Studies, Argonne Natl Lab, Argonne, IL 60439 USA. RP Newville, M (reprint author), Univ Chicago, Ctr Adv Radiat Studies, Argonne Natl Lab, Bldg 434A, Argonne, IL 60439 USA. EM newville@cars.uchicago.edu NR 28 TC 11 Z9 11 U1 0 U2 11 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 430 AR UNSP 012007 DI 10.1088/1742-6596/430/1/012007 PG 7 WC Physics, Condensed Matter; Spectroscopy SC Physics; Spectroscopy GA BFM11 UT WOS:000320464300007 ER PT S AU Sham, TK Ward, MJ Murphy, MW Liu, LJ Han, WQ AF Sham, T. K. Ward, M. J. Murphy, M. W. Liu, L. J. Han, W. Q. BE Wu, ZY TI Pt L-3,L-2-edge whiteline anomaly and its implications for the chemical behaviour of Pt 5d(5/2) and 5d(3/2) electronic states - a study of Pt-Au nanowires and nanoparticles SO 15TH INTERNATIONAL CONFERENCE ON X-RAY ABSORPTION FINE STRUCTURE (XAFS15) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 15th International Conference on X-Ray Absorption Fine Structure (XAFS) CY JUL 22-28, 2012 CL Beijing, PEOPLES R CHINA SP Chinese Acad Sci (CAS), Natl Nat Sci Fdn China (NSFC), China Ctr Adv Sci & Technol World Lab, Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Chinese Acad Sci, Inst High Energy Phys, AREVA, Xian Act Power Elect Co, Ltd ID X-RAY-ABSORPTION AB We report the L-3,L-2-edge whiteline anomaly observed in PtAu nanowire, PtAu and Pt nanoparticles deposited on Si nanowire, and their comparison with that of Pt metal. It is found that charge redistribution upon the formation of these materials can indeed be tracked with the L-3,L-2 whiteline intensity. The implications of these findings are discussed. C1 [Sham, T. K.; Ward, M. J.; Murphy, M. W.; Liu, L. J.] Univ Western Ontario, Dept Chem, London, ON N6A 5B7, Canada. [Han, W. Q.] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. RP Sham, TK (reprint author), Univ Western Ontario, Dept Chem, London, ON N6A 5B7, Canada. EM tsham@uwo.ca FU NSERC; CRC; CFI of Canada; OIT (Ontario); US Department of Energy (DOE); Basic Energy Sciences; Major Resource Support (NSERC); University of Washington; Simon Fraser University FX Research at Western is supported by NSERC, CRC, and CFI of Canada and OIT (Ontario); PNC/XSD at APS is supported by the US Department of Energy (DOE), Basic Energy Sciences, the Major Resource Support (NSERC), the University of Washington, and Simon Fraser University. Technical assistance of Robert Gordon is greatly appreciated. NR 8 TC 2 Z9 2 U1 0 U2 8 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 430 AR UNSP 012018 DI 10.1088/1742-6596/430/1/012018 PG 4 WC Physics, Condensed Matter; Spectroscopy SC Physics; Spectroscopy GA BFM11 UT WOS:000320464300018 ER PT S AU Christophersen, JP Morrison, JL Morrison, WH AF Christophersen, Jon P. Morrison, John L. Morrison, William H. GP IEEE TI Acquiring Impedance Spectra from Diode-Coupled Primary Batteries to Determine Health and State of Charge SO 2013 IEEE AEROSPACE CONFERENCE SE IEEE Aerospace Conference Proceedings LA English DT Proceedings Paper CT IEEE Aerospace Conference CY MAR 02-09, 2013 CL Big Sky, MT SP IEEE ID MANAGEMENT-SYSTEMS; PART 2; PACKS AB The U. S. Army uses BA5590 Lithium Sulfur Dioxide primary batteries for portable electronic systems. There remains a need, however, for technology that can rapidly assess these batteries and estimate their remaining state of health after being used without degrading them to determine if there is remaining useful life for additional missions. This allows the full range of charge to be consumed before the battery is recycled or disposed. Impedance spectroscopy measurements have been shown to be a useful diagnostic tool, but standard methods cannot be applied to the BA5590 batteries because of the up-front electronics. The BA5590 module is diode-coupled and a charge-neutral excitation signal would be half-wave rectified and completely corrupt the results. However, a rapid impedance spectrum measurement technique has been developed that can be used for the BA5590s based on the addition of a small discharge bias load superimposed on the sinusoidal excitation signal. The feasibility of this approach was initially simulated and then successfully applied to cell strings on four fresh BA5590 modules. The results clearly showed consistent and repeatable impedance spectra with no significant impact on the SOC as a result of the measurement. Details of this measurement technique and discussion of the preliminary results are presented. C1 [Christophersen, Jon P.] Idaho Natl Lab, POB 1625, Idaho Falls, ID 83415 USA. RP Christophersen, JP (reprint author), Idaho Natl Lab, POB 1625, Idaho Falls, ID 83415 USA. EM Jon.Christophersen@inl.gov; jmorrison@mtech.edu; morrison.theta.sigma@gmail.com FU United States Government under U.S. DOE [DE-AC0705I14517]; U.S. DOE Office of Vehicle Technologies; Idaho National Laboratory [00095510]; U.S. Government FX The authors gratefully acknowledge Jeff Ross at the Fort Polk Joint Readiness Training Center (JRTC) for providing the BA5590 module samples for this effort. This work was prepared as an account of work sponsored by an agency of the United States Government under U.S. DOE Contract DE-AC0705I14517. Funding for this work was provided by the U.S. DOE Office of Vehicle Technologies. Montana Tech was supported in part by Idaho National Laboratory Contract 00095510. 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. Views and opinions of the authors expressed herein do not necessarily state or reflect those of the U.S. Government or any agency thereof NR 17 TC 0 Z9 0 U1 1 U2 6 PU IEEE PI NEW YORK PA 345 E 47TH ST, NEW YORK, NY 10017 USA SN 1095-323X BN 978-1-4673-1811-2 J9 AEROSP CONF PROC PY 2013 PG 10 WC Engineering, Aerospace; Engineering, Electrical & Electronic SC Engineering GA BFJ62 UT WOS:000320123903049 ER PT S AU Hughart, DR Dalton, SM Mickel, PR Dodd, PE Shaneyfelt, MR Bielejec, E Vizkelethy, G Marinella, MJ AF Hughart, D. R. Dalton, S. M. Mickel, P. R. Dodd, P. E. Shaneyfelt, M. R. Bielejec, E. Vizkelethy, G. Marinella, M. J. GP IEEE TI Total Ionizing Dose and Displacement Damage Effects on TaOx Memristive Memories SO 2013 IEEE AEROSPACE CONFERENCE SE IEEE Aerospace Conference Proceedings LA English DT Proceedings Paper CT IEEE Aerospace Conference CY MAR 02-09, 2013 CL Big Sky, MT SP IEEE ID ELECTRICAL CHARACTERISTICS; RADIATION; MECHANISM; DEVICE AB The effects of ionizing radiation and displacement damage on TaOx memristors are evaluated. Devices show little response to 10 keV x-rays up to 10 Mrad(Si). Co-60 gamma rays and 4.5 MeV protons did not change the resistances significantly at levels up to 2.5 Mrad(Si) and 5 Mrad(Si) respectively. 105 MeV and 480 MeV protons cause switching of the memristors from high to low resistance states in some cases, but do not exhibit a consistent degradation. 800 keV silicon ions are observed to cause resistance degradation, with an inverse dependence of resistance on oxygen vacancy density. Variation between different devices appears to be a key factor in determining the electrical response resulting from irradiation. The proposed degradation mechanism likely involves the creation of oxygen vacancies, but a better fundamental understanding of switching is needed before a definitive understanding of radiation degradation can be achieved. C1 [Hughart, D. R.; Dalton, S. M.; Mickel, P. R.; Dodd, P. E.; Shaneyfelt, M. R.; Bielejec, E.; Vizkelethy, G.; Marinella, M. J.] Sandia Natl Labs, Albuquerque, NM 87123 USA. RP Hughart, DR (reprint author), Sandia Natl Labs, Albuquerque, NM 87123 USA. EM dhughar@sandia.gov; mmarine@sandia.gov NR 16 TC 0 Z9 0 U1 0 U2 9 PU IEEE PI NEW YORK PA 345 E 47TH ST, NEW YORK, NY 10017 USA SN 1095-323X BN 978-1-4673-1811-2 J9 AEROSP CONF PROC PY 2013 PG 10 WC Engineering, Aerospace; Engineering, Electrical & Electronic SC Engineering GA BFJ62 UT WOS:000320123903044 ER PT S AU Kimball, J Duchaineau, M Kuester, F AF Kimball, Jason Duchaineau, Mark Kuester, Falko GP IEEE TI Interactive Visualization of Large Scale Atomistic and Cosmological Particle Simulation SO 2013 IEEE AEROSPACE CONFERENCE SE IEEE Aerospace Conference Proceedings LA English DT Proceedings Paper CT IEEE Aerospace Conference CY MAR 02-09, 2013 CL Big Sky, MT SP IEEE AB In this paper we present a method for interactive high-quality visualization of large and time-varying 3D unstructured data from particle simulations. To help design next-generation materials for aerospace systems, understanding the physics of material structures at the atomic scale is achieved through molecular dynamics simulations run on tens to hundreds of millions of atoms. Similarly, to understand the formation of the cosmos, galaxy formation simulations are run using tens to hundreds of millions of particles. From the atomically small to the astronomically large, these simulations produce immense amounts of data. While these simulations have been shown to produce excellent results matching real-world observations, the daunting Big Data that they produce can be difficult to work with. Numerical analysis is useful for processing this large quantity of data, but visual analysis is also important in the search for identifying interesting results and formulating new hypotheses to explore. Though many level-of-detail techniques exist for structured and geometric data, allowing scalable interactive visualization, unstructured particle data is not suitable for these techniques. Therefore, we have developed a new technique for scalable visualization of massive particle datasets. The technique is different from previous level-of-detail techniques which create progressive approximations of the data itself. Instead, the technique creates a volumetric representation of the data first and then creates a hierarchy of progressive approximations of the volumetric representation. An adaptive volume rendering technique is also presented that progressively refines the volume hierarchy depending on the view of the data and the time available to load data. The technique provides a scalable framework, allowing various levels of detail to be loaded while maintaining interactivity. This paper describes the rendering techniques used to produce the 3D volume hierarchy as well as the adaptive volume renderer used for interactive visualization. Three case studies are discussed as examples of interactive visualization. Two are from a molecular dynamics simulation, one containing approximately 22 million particles per time-step over 100 time-steps and one containing a range of particles containing a total of 230 million particles over 9 time steps. The third example is a single time step containing 128 million particle from a cosmology simulation. C1 [Kimball, Jason] Univ Calif San Diego, Dept Comp Sci & Engn, La Jolla, CA 92093 USA. [Duchaineau, Mark] Lawrence Livermore Natl Lab, Ctr Appl Sci Comp, Livermore, CA 94550 USA. [Kuester, Falko] Univ Calif San Diego, Dept Struct Engn, La Jolla, CA 92093 USA. RP Kimball, J (reprint author), Univ Calif San Diego, Dept Comp Sci & Engn, La Jolla, CA 92093 USA. EM jkimball@ucsd.edu; duchaine@google.com; fkuester@ucsd.edu FU U.S. Department of Energy by Lawrence Livermore National Laboratory [DE-AC5207NA27344] FX We would like to thank Lawrence Livermore National Laboratory for providing the atomistic datasets.; This work was performed in part under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC5207NA27344. NR 14 TC 0 Z9 0 U1 0 U2 2 PU IEEE PI NEW YORK PA 345 E 47TH ST, NEW YORK, NY 10017 USA SN 1095-323X BN 978-1-4673-1811-2 J9 AEROSP CONF PROC PY 2013 PG 9 WC Engineering, Aerospace; Engineering, Electrical & Electronic SC Engineering GA BFJ62 UT WOS:000320123903082 ER PT S AU Marinella, M AF Marinella, Matthew GP IEEE TI The Future of Memory SO 2013 IEEE AEROSPACE CONFERENCE SE IEEE Aerospace Conference Proceedings LA English DT Proceedings Paper CT IEEE Aerospace Conference CY MAR 02-09, 2013 CL Big Sky, MT SP IEEE AB In the not too distant future, the traditional memory and storage hierarchy of may be replaced by a single Storage Class Memory (SCM) device integrated on or near the logic processor. Traditional magnetic hard drives, NAND flash, DRAM, and higher level caches (L2 and up) will be replaced with a single high performance memory device. The Storage Class Memory paradigm will require high speed (< 100 ns read/write), excellent endurance (> 1012), nonvolatility (retention > 10 years), and low switching energies (< 10 pJ per switch). The International Technology Roadmap for Semiconductors (ITRS) has recently evaluated several potential candidates SCM technologies, including Resistive (or Redox) RAM, Spin Torque Transfer RAM (STT-MRAM), and phase change memory (PCM). All of these devices show potential well beyond that of current flash technologies and research efforts are underway to improve the endurance, write speeds, and scalabilities to be on-par with DRAM. This progress has interesting implications for space electronics: each of these emerging device technologies show excellent resistance to the types of radiation typically found in space applications. Commercially developed, high density storage class memory-based systems may include a memory that is physically radiation hard, and suitable for space applications without major shielding efforts. This paper reviews the Storage Class Memory concept, emerging memory devices, and possible applicability to radiation hardened electronics for space. C1 Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Marinella, M (reprint author), Sandia Natl Labs, POB 5800,MS 1084, Albuquerque, NM 87185 USA. EM mmarine@sandia.gov NR 24 TC 0 Z9 0 U1 1 U2 14 PU IEEE PI NEW YORK PA 345 E 47TH ST, NEW YORK, NY 10017 USA SN 1095-323X BN 978-1-4673-1811-2 J9 AEROSP CONF PROC PY 2013 PG 11 WC Engineering, Aerospace; Engineering, Electrical & Electronic SC Engineering GA BFJ62 UT WOS:000320123903097 ER PT S AU Guo, TF Wang, SQ Samulyak, R AF Guo, Tongfei Wang, Shuqiang Samulyak, Roman BE Alexandrov, V Lees, M Krzhizhanovskaya, V Dongarra, J Sloot, PMA TI Sharp Interface Algorithm for Large Density Ratio Incompressible Multiphase Magnetohydrodynamic Flows SO 2013 INTERNATIONAL CONFERENCE ON COMPUTATIONAL SCIENCE SE Procedia Computer Science LA English DT Proceedings Paper CT 13th Annual International Conference on Computational Science (ICCS) CY JUN 05-07, 2013 CL Barcelona, SPAIN SP Univ Amsterdam, Univ Tennessee, Nanyang Technol Univ, Barcelona Super Comp Ctr DE Front tracking; multiphase MHD; liquid metal MHD ID EMBEDDED BOUNDARY METHOD; NAVIER-STOKES EQUATIONS; FRONT-TRACKING METHOD; IRREGULAR DOMAINS; POISSONS-EQUATION; HEAT-EQUATION; SYSTEMS AB A numerical algorithm and the corresponding paralleled implementation for the study of magnetohydrodynamics (MHD) of large density ratio, three-dimensional multiphase flows at low magnetic Reynolds numbers have been developed. The algorithm employs the method of front tracking for the propagation of material interfaces and the embedded interface method for solving elliptic-parabolic problems associated with approximations of incompressible fluids and low magnetic Reynolds numbers. The use of embedded interface method supports arbitrary discontinuities of density and other physics properties across interfaces and significantly improves methods that smear interface discontinuities across several grid cells. The numerical algorithm has been implemented as an MHD extension of FronTier, a parallel front tracking hydrodynamic code, verified using asymptotic solutions and validated through the comparison with experiments on liquid metal jets. The FronTier-MHD code has been used for simulations of liquid mercury targets for the proposed muon collider/neutrino factory, ablation of pellets in tokamaks, and processes in hybrid magnetoinertial fusion. C1 [Guo, Tongfei; Samulyak, Roman] SUNY Stony Brook, Dept Appl Math & Stat, Stony Brook, NY 11794 USA. [Wang, Shuqiang; Samulyak, Roman] Brookhaven Natl Lab, Computat Sci Ctr, Upton, NY 11973 USA. RP Samulyak, R (reprint author), SUNY Stony Brook, Dept Appl Math & Stat, Stony Brook, NY 11794 USA. EM roman.samulyak@stonybrook.edu RI Dongarra, Jack/E-3987-2014 FU Muon Accelerator Program of the US Department of Energy FX This work was supported in part by the Muon Accelerator Program of the US Department of Energy. NR 26 TC 0 Z9 0 U1 0 U2 7 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA SARA BURGERHARTSTRAAT 25, PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 1877-0509 J9 PROCEDIA COMPUT SCI PY 2013 VL 18 BP 511 EP 520 DI 10.1016/j.procs.2013.05.215 PG 10 WC Computer Science, Theory & Methods SC Computer Science GA BFR52 UT WOS:000321051200052 ER PT S AU Chen, J Li, TLH AF Chen, Jie Li, Tom L. H. BE Alexandrov, V Lees, M Krzhizhanovskaya, V Dongarra, J Sloot, PMA TI Parallelizing the conjugate gradient algorithm for multilevel Toeplitz systems SO 2013 INTERNATIONAL CONFERENCE ON COMPUTATIONAL SCIENCE SE Procedia Computer Science LA English DT Proceedings Paper CT 13th Annual International Conference on Computational Science (ICCS) CY JUN 05-07, 2013 CL Barcelona, SPAIN SP Univ Amsterdam, Univ Tennessee, Nanyang Technol Univ, Barcelona Super Comp Ctr DE Toeplitz; conjugate gradient; FFT; all-reduction ID LINEAR-EQUATIONS; MATRICES; PRECONDITIONERS AB Multilevel Toeplitz linear systems appear in a wide range of scientific and engineering applications. While several fast direct solvers exist for the basic 1-level Toeplitz matrices, in the multilevel case an iterative solver provides the most general and practical solution. This paper proposes several parallelization techniques that enable an efficient implementation of the conjugate gradient algorithm for solving multilevel Toeplitz systems on distributed-memory machines. The two major differences between this implementation and that for a general sparse linear solver are (1) a communication-efficient approach to handle data expansion and truncation and data transpose simultaneously; (2) the interleaving of matrix-vector multiplications and vector inner product calculations to reduce synchronization cost and latency. Similar ideas can be applied to the implementation of other iterative methods for Toeplitz systems that are not necessarily symmetric positive definite. Scaling results are shown to demonstrate the usefulness of the proposed techniques. C1 [Chen, Jie] Argonne Natl Lab, Div Math & Comp Sci, Argonne, IL 60517 USA. [Li, Tom L. H.] Univ Missouri, Dept Math & Comp Sci, St Louis, MO 63121 USA. RP Chen, J (reprint author), Argonne Natl Lab, Div Math & Comp Sci, Argonne, IL 60517 USA. EM jiechen@mcs.anl.gov; ll9n8@mail.umsl.edu RI Dongarra, Jack/E-3987-2014 FU U.S. Department of Energy [DE-AC02-06CH11357] FX This work was supported by the U.S. Department of Energy under Contract DE-AC02-06CH11357. We gratefully acknowledge use of the Fusion cluster in the Laboratory Computing Resource Center at Argonne National Laboratory. NR 31 TC 3 Z9 3 U1 0 U2 1 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA SARA BURGERHARTSTRAAT 25, PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 1877-0509 J9 PROCEDIA COMPUT SCI PY 2013 VL 18 BP 571 EP 580 DI 10.1016/j.procs.2013.05.221 PG 10 WC Computer Science, Theory & Methods SC Computer Science GA BFR52 UT WOS:000321051200058 ER PT S AU Jacob, R Krishna, J Xu, XB Tautges, T Grindeanu, I Latham, R Peterson, K Bochev, P Haley, M Brown, D Brownrigg, R Shea, D Huang, W Middleton, D AF Jacob, Robert Krishna, Jayesh Xu, Xiabing Tautges, Tim Grindeanu, Iulian Latham, Rob Peterson, Kara Bochev, Pavel Haley, Mary Brown, David Brownrigg, Richard Shea, Dennis Huang, Wei Middleton, Don BE Alexandrov, V Lees, M Krzhizhanovskaya, V Dongarra, J Sloot, PMA TI ParNCL and ParGAL: Data-parallel tools for postprocessing of large-scale Earth science data SO 2013 INTERNATIONAL CONFERENCE ON COMPUTATIONAL SCIENCE SE Procedia Computer Science LA English DT Proceedings Paper CT 13th Annual International Conference on Computational Science (ICCS) CY JUN 05-07, 2013 CL Barcelona, SPAIN SP Univ Amsterdam, Univ Tennessee, Nanyang Technol Univ, Barcelona Super Comp Ctr DE data analysis; data parallelism; postprocessing ID PERFORMANCE; EQUATIONS; MODEL AB Earth science high-performance applications often require extensive analysis of their output in order to complete the scientific goals or produce a visual image or animation. Often this analysis cannot be done in situ because it requires calculating time-series statistics from state sampled over the entire length of the run or analyzing the relationship between similar time series from previous simulations or observations. Many of the tools used for this postprocessing are not themselves high-performance applications, but the new Parallel Gridded Analysis Library (ParGAL) provides high-performance data-parallel versions of several common analysis algorithms for data from a structured or unstructured grid simulation. The library builds on several scalable systems, including the Mesh Oriented DataBase (MOAB), a library for representing mesh data that supports structured, unstructured finite element, and polyhedral grids; the Parallel-NetCDF (PNetCDF) library; and Intrepid, an extensible library for computing operators (such as gradient, curl, and divergence) acting on discretized fields. We have used ParGAL to implement a parallel version of the NCAR Command Language (NCL) a scripting language widely used in the climate community for analysis and visualization. The data-parallel algorithms in ParGAL/ParNCL are both higher performing and more flexible than their serial counterparts. C1 [Jacob, Robert; Krishna, Jayesh; Xu, Xiabing; Tautges, Tim; Grindeanu, Iulian; Latham, Rob] Argonne Natl Lab, 9700 S Cass Ave, Argonne, IL 60439 USA. [Peterson, Kara; Bochev, Pavel] Sandia Natl Labs, Albuquerque, NM 87123 USA. [Haley, Mary; Brown, David; Brownrigg, Richard; Shea, Dennis; Huang, Wei; Middleton, Don] Natl Ctr Atmospher Res, Boulder, CO 80307 USA. RP Jacob, R (reprint author), Argonne Natl Lab, 9700 S Cass Ave, Argonne, IL 60439 USA. EM jacob@mcs.anl.gov RI Dongarra, Jack/E-3987-2014; OI Jacob, Robert/0000-0002-9444-6593 FU Office of Biological and Environmental Research of the U.S. Department of Energy's Office of Science [AC02-06CH11357]; U.S. National Science Foundation via contributions from the National Center for Atmospheric Research, Boulder, CO; U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX This work is part of the Parallel Analysis Tools and New Visualization Techniques for Ultra-Large Climate Data Sets (ParVis) project supported by the Earth System Modeling Program of the Office of Biological and Environmental Research of the U.S. Department of Energys Office of Science under contract DE-AC02-06CH11357. The project is co-sponsored by the U.S. National Science Foundation via contributions from the National Center for Atmospheric Research, Boulder, CO. We gratefully acknowledge the computing resources provided on Fusion, a 320-node computing cluster operated by the Laboratory Computing Resource Center at Argonne National Laboratory. 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 Energys National Nuclear Security Administration under contract DE-AC04-94AL85000. NR 24 TC 2 Z9 2 U1 0 U2 10 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA SARA BURGERHARTSTRAAT 25, PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 1877-0509 J9 PROCEDIA COMPUT SCI PY 2013 VL 18 BP 1245 EP 1254 DI 10.1016/j.procs.2013.05.291 PG 10 WC Computer Science, Theory & Methods SC Computer Science GA BFR52 UT WOS:000321051200128 ER PT S AU Utke, J Rearden, BT Lefebvre, RA AF Utke, Jean Rearden, Bradley T. Lefebvre, Robert A. BE Alexandrov, V Lees, M Krzhizhanovskaya, V Dongarra, J Sloot, PMA TI Sensitivity analysis for mixed-language numerical models SO 2013 INTERNATIONAL CONFERENCE ON COMPUTATIONAL SCIENCE SE Procedia Computer Science LA English DT Proceedings Paper CT 13th Annual International Conference on Computational Science (ICCS) CY JUN 05-07, 2013 CL Barcelona, SPAIN SP Univ Amsterdam, Univ Tennessee, Nanyang Technol Univ, Barcelona Super Comp Ctr DE sensitivity analysis; mixed-programming languages; algorithmic differentiation ID AUTOMATIC DIFFERENTIATION; DERIVATIVE TENSORS AB The separation of concerns in the development of numerical models not only leads to a separation into components but, based on their purpose, these components may also be written in different programming languages. The sensitivity analysis of a numerical model provides quantitative information about the dependencies of the model outputs with respect to its inputs. An analysis of mixed-language models using derivatives computed with algorithmic (or automatic) differentiation needs to comprehensively handle all the involved components and the respective interfaces in a mixed-language environment. We describe the issues arising in the context of the sensitivity analysis, present a solution implemented with the algorithmic differentiation tool Rapsodia for C++ and Fortran, and discuss its practical use in a large-scale engineering application. C1 [Utke, Jean] Argonne Natl Lab, MCS, 9700 S Cass Ave, Argonne, IL 60437 USA. [Rearden, Bradley T.; Lefebvre, Robert A.] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. RP Utke, J (reprint author), Argonne Natl Lab, MCS, 9700 S Cass Ave, Argonne, IL 60437 USA. EM utke@mcs.anl.gov RI Dongarra, Jack/E-3987-2014 FU U.S. Department of Energy [DE-AC02-06CH11357] FX Utke was supported by the U.S. Department of Energy, under contract DE-AC02-06CH11357. NR 18 TC 1 Z9 1 U1 0 U2 0 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA SARA BURGERHARTSTRAAT 25, PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 1877-0509 J9 PROCEDIA COMPUT SCI PY 2013 VL 18 BP 1794 EP 1803 DI 10.1016/j.procs.2013.05.348 PG 10 WC Computer Science, Theory & Methods SC Computer Science GA BFR52 UT WOS:000321051200185 ER PT S AU Bazilevs, Y Hsu, MC Bement, MT AF Bazilevs, Y. Hsu, M. -C. Bement, M. T. BE Alexandrov, V Lees, M Krzhizhanovskaya, V Dongarra, J Sloot, PMA TI Adjoint-Based Control of Fluid-Structure Interaction for Computational Steering Applications SO 2013 INTERNATIONAL CONFERENCE ON COMPUTATIONAL SCIENCE SE Procedia Computer Science LA English DT Proceedings Paper CT 13th Annual International Conference on Computational Science (ICCS) CY JUN 05-07, 2013 CL Barcelona, SPAIN SP Univ Amsterdam, Univ Tennessee, Nanyang Technol Univ, Barcelona Super Comp Ctr DE Fluid-structure interaction; adjoint FSI formulation; adjoint-based control; isogeometric analysis; computational steering; DDDAS AB The primal and adjoint, time-dependent fluid-structure interaction (FSI) formulations are presented. A simple control strategy for FSI problems is formulated based on the information provided by the solution of the adjoint FSI problem. A well-known benchmark FSI problem is computed to demonstrate the effectiveness of the proposed technique. Such control strategies as proposed in this paper are useful for computational steering or so-called Dynamics Data Driven Application System (DDDAS) simulations, in which the computational model is adjusted to include the information coming from the measurement data, and control strategies may be employed to computationally steer the physical system toward desired behavior. C1 [Bazilevs, Y.] Univ Calif San Diego, Dept Struct Engn, La Jolla, CA 92093 USA. [Hsu, M. -C.] Univ Texas Austin, Inst Computat Engn & Sci, Austin, TX 78712 USA. [Bement, M. T.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Bazilevs, Y (reprint author), Univ Calif San Diego, Dept Struct Engn, La Jolla, CA 92093 USA. EM yuri@ucsd.edu RI Dongarra, Jack/E-3987-2014; Hsu, Ming-Chen/J-1881-2012 OI Hsu, Ming-Chen/0000-0001-8062-8612 FU Air Force Office of Scientific Research [FA9550-12-1-0005]; Los AlamosUC San Diego Educational Collaboration Fellowship FX The lead author acknowledges the support of the Air Force Office of Scientific Research Award FA9550-12-1-0005. M.-C. Hsu was supported through the Los AlamosUC San Diego Educational Collaboration Fellowship. NR 16 TC 13 Z9 13 U1 0 U2 4 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA SARA BURGERHARTSTRAAT 25, PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 1877-0509 J9 PROCEDIA COMPUT SCI PY 2013 VL 18 BP 1989 EP 1998 DI 10.1016/j.procs.2013.05.368 PG 10 WC Computer Science, Theory & Methods SC Computer Science GA BFR52 UT WOS:000321051200205 ER PT S AU Sisneros, R Huang, J Ostrouchov, G Ahern, S Semeraro, BD AF Sisneros, Robert Huang, Jian Ostrouchov, George Ahern, Sean Semeraro, B. David BE Alexandrov, V Lees, M Krzhizhanovskaya, V Dongarra, J Sloot, PMA TI Contrasting Climate Ensembles: A Model-Based Visualization Approach for Analyzing Extreme Events SO 2013 INTERNATIONAL CONFERENCE ON COMPUTATIONAL SCIENCE SE Procedia Computer Science LA English DT Proceedings Paper CT 13th Annual International Conference on Computational Science (ICCS) CY JUN 05-07, 2013 CL Barcelona, SPAIN SP Univ Amsterdam, Univ Tennessee, Nanyang Technol Univ, Barcelona Super Comp Ctr DE visualization; climate ensembles; multivariate classification ID PROJECTIONS AB The use of increasingly sophisticated means to simulate and observe natural phenomena has led to the production of larger and more complex data. As the size and complexity of this data increases, the task of data analysis becomes more challenging. Determining complex relationships among variables requires new algorithm development. Addressing the challenge of handling large data necessitates that algorithm implementations target high performance computing platforms. In this work we present a technique that allows a user to study the interactions among multiple variables in the same spatial extents as the underlying data. The technique is implemented in an existing parallel analysis and visualization framework in order that it be applicable to the largest datasets. The foundation of our approach is to classify data points via inclusion in, or distance to, multivariate representations of relationships among a subset of the variables of a dataset. We abstract the space in which inclusion is calculated and through various space transformations we alleviate the necessity to consider variables' scales and distributions when making comparisons. We apply this approach to the problem of highlighting variations in climate model ensembles. C1 [Sisneros, Robert; Semeraro, B. David] Univ Illinois, Natl Ctr Supercomp Applicat, Urbana, IL 61801 USA. [Huang, Jian] Univ Tennessee, Knoxville, TN 37996 USA. [Ostrouchov, George; Ahern, Sean] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. RP Sisneros, R (reprint author), Univ Illinois, Natl Ctr Supercomp Applicat, Urbana, IL 61801 USA. EM sisneros@illinois.edu RI Dongarra, Jack/E-3987-2014 NR 37 TC 3 Z9 3 U1 0 U2 8 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA SARA BURGERHARTSTRAAT 25, PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 1877-0509 J9 PROCEDIA COMPUT SCI PY 2013 VL 18 BP 2347 EP 2356 DI 10.1016/j.procs.2013.05.406 PG 10 WC Computer Science, Theory & Methods SC Computer Science GA BFR52 UT WOS:000321051200243 ER PT S AU Smith, B Ricciuto, DM Thornton, PE Shipman, G Steed, CA Williams, D Wehner, M AF Smith, Brian Ricciuto, Daniel M. Thornton, Peter E. Shipman, Galen Steed, Chad A. Williams, Dean Wehner, Michael BE Alexandrov, V Lees, M Krzhizhanovskaya, V Dongarra, J Sloot, PMA TI ParCAT: Parallel Climate Analysis Toolkit SO 2013 INTERNATIONAL CONFERENCE ON COMPUTATIONAL SCIENCE SE Procedia Computer Science LA English DT Proceedings Paper CT 13th Annual International Conference on Computational Science (ICCS) CY JUN 05-07, 2013 CL Barcelona, SPAIN SP Univ Amsterdam, Univ Tennessee, Nanyang Technol Univ, Barcelona Super Comp Ctr DE Parallel Climate Analysis ParCAT AB Climate science is employing increasingly complex models and simulations to analyze the past and predict the future of Earth's climate. This growth in complexity is creating a widening gap between the data being produced and the ability to analyze the datasets. Parallel computing tools are necessary to analyze, compare, and interpret the simulation data. The Parallel Climate Analysis Toolkit (ParCAT) provides basic tools to efficiently use parallel computing techniques to make analysis of these datasets manageable. The toolkit provides the ability to compute spatio-temporal means, differences between runs or differences between averages of runs, and histograms of the values in a data set. ParCAT is implemented as a command-line utility written in C. This allows for easy integration in other tools and allows for use in scripts. This also makes it possible to run ParCAT on many platforms from laptops to supercomputers. ParCAT outputs NetCDF files so it is compatible with existing utilities such as Panoply and UV-CDAT. This paper describes ParCAT and presents results from some example runs on the Titan system at ORNL. (C) 2013 The Authors. Published by Elsevier B.V. Selection and peer review under responsibility of the organizers of the 2013 International Conference on Computational Science C1 [Smith, Brian; Ricciuto, Daniel M.; Thornton, Peter E.; Shipman, Galen; Steed, Chad A.] Oak Ridge Natl Lab, 1 Bethel Valley Rd, Oak Ridge, TN 37830 USA. [Williams, Dean] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. [Wehner, Michael] Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Smith, B (reprint author), Oak Ridge Natl Lab, 1 Bethel Valley Rd, Oak Ridge, TN 37830 USA. EM smithbe@ornl.gov RI Dongarra, Jack/E-3987-2014; Thornton, Peter/B-9145-2012; Ricciuto, Daniel/I-3659-2016; OI Thornton, Peter/0000-0002-4759-5158; Ricciuto, Daniel/0000-0002-3668-3021; Steed, Chad/0000-0002-3501-909X FU U.S. Department of Energy; Oak Ridge National Laboratory [DE-AC05-00OR22725]; Office of Science of the U.S. Department of Energy [DE-AC05-0OR22725] FX This work is sponsored by the Office of Biological and Environmental Research; U.S. Department of Energy. The work was performed at the Oak Ridge National Laboratory, which is managed by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725. This research used resources of the Oak Ridge Leadership Computing Facility at Oak Ridge National Laboratory, which is supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC05-0OR22725. NR 6 TC 5 Z9 5 U1 0 U2 11 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA SARA BURGERHARTSTRAAT 25, PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 1877-0509 J9 PROCEDIA COMPUT SCI PY 2013 VL 18 BP 2367 EP 2375 DI 10.1016/j.procs.2013.05.408 PG 9 WC Computer Science, Theory & Methods SC Computer Science GA BFR52 UT WOS:000321051200245 ER PT S AU Mills, RT Kumar, J Hoffman, FM Hargrove, WW Spruce, JP Norman, SP AF Mills, Richard Tran Kumar, Jitendra Hoffman, Forrest M. Hargrove, William W. Spruce, Joseph P. Norman, Steven P. BE Alexandrov, V Lees, M Krzhizhanovskaya, V Dongarra, J Sloot, PMA TI Identification and visualization of dominant patterns and anomalies in remotely sensed vegetation phenology using a parallel tool for principal components analysis SO 2013 INTERNATIONAL CONFERENCE ON COMPUTATIONAL SCIENCE SE Procedia Computer Science LA English DT Proceedings Paper CT 13th Annual International Conference on Computational Science (ICCS) CY JUN 05-07, 2013 CL Barcelona, SPAIN SP Univ Amsterdam, Univ Tennessee, Nanyang Technol Univ, Barcelona Super Comp Ctr DE phenology; MODIS; NDVI; remote sensing; principal components analysis; singular value decomposition; data mining; anomaly detection; high performance computing; parallel computing ID DATA SETS; NETWORK; DELINEATION AB We investigated the use of principal components analysis (PCA) to visualize dominant patterns and identify anomalies in a multi-year land surface phenology data set (231 m x 231 m normalized difference vegetation index (NDVI) values derived from the Moderate Resolution Imaging Spectroradiometer (MODIS)) used for detecting threats to forest health in the conterminous United States (CONUS). Our goal is to find ways that PCA can be used with this massive data set to automate the process of detecting forest disturbance and attributing it to particular agents. We briefly describe the parallel computational approaches we used to make PCA feasible, and present some examples in which we have used it to visualize the seasonal vegetation phenology for the CONUS and to detect areas where anomalous NDVI traces suggest potential threats to forest health. C1 [Mills, Richard Tran; Kumar, Jitendra; Hoffman, Forrest M.] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. RP Mills, RT (reprint author), Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. EM rmills@ornl.gov RI Dongarra, Jack/E-3987-2014; Kumar, Jitendra/G-8601-2013; Hoffman, Forrest/B-8667-2012 OI Kumar, Jitendra/0000-0002-0159-0546; Hoffman, Forrest/0000-0001-5802-4134 NR 13 TC 3 Z9 3 U1 1 U2 9 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA SARA BURGERHARTSTRAAT 25, PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 1877-0509 J9 PROCEDIA COMPUT SCI PY 2013 VL 18 BP 2396 EP 2405 DI 10.1016/j.procs.2013.05.411 PG 10 WC Computer Science, Theory & Methods SC Computer Science GA BFR52 UT WOS:000321051200248 ER PT J AU Senesi, AJ Eichelsdoerfer, DJ Macfarlane, RJ Jones, MR Auyeung, E Lee, B Mirkin, CA AF Senesi, Andrew J. Eichelsdoerfer, Daniel J. Macfarlane, Robert J. Jones, Matthew R. Auyeung, Evelyn Lee, Byeongdu Mirkin, Chad A. TI Stepwise Evolution of DNA-Programmable Nanoparticle Superlattices SO ANGEWANDTE CHEMIE-INTERNATIONAL EDITION LA English DT Article DE colloidal crystals; DNA; nanomaterials; nanoparticle superlattice; X-ray diffraction ID NANOCRYSTAL SUPERLATTICES; THIN-FILMS; COLLOIDAL CRYSTALS; BUILDING-BLOCKS; CRYSTALLIZATION; GROWTH; PARTICLES; LAYERS C1 [Senesi, Andrew J.; Eichelsdoerfer, Daniel J.; Macfarlane, Robert J.; Mirkin, Chad A.] Northwestern Univ, Dept Chem, Evanston, IL 60208 USA. [Jones, Matthew R.; Auyeung, Evelyn; Mirkin, Chad A.] Northwestern Univ, Dept Mat Sci & Engn, Evanston, IL 60208 USA. [Lee, Byeongdu] Argonne Natl Lab, Xray Sci Div, Argonne, IL 60439 USA. RP Lee, B (reprint author), Argonne Natl Lab, Xray Sci Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM blee@anl.gov; chadnano@northwestern.edu RI Mirkin, Chad/E-3911-2010; OI Lee, Byeongdu/0000-0003-2514-8805; Jones, Matthew/0000-0002-9289-291X FU AFOSR [FA9550-11-1-0275, FA9550-09-1-0294, FA2386-10-1-4065]; Department of the Navy/ONR [N00014-11-1-0729]; DoD/NSSEFF/NPS [N00244-09-1-0012, N00244-09-1-0071]; Non-Equilibrium Energy Research Center (NERC), an Energy Frontier Research Center; DoE/Office of Science/Office of Basic Energy Sciences [DE-SC0000989]; DoD, Air Force Office of Scientific Research, National Defense Science and Engineering Graduate (NDSEG) [32 CFR 168a]; NSF; U.S. DOE [DE-AC02-06CH11357] FX C. A. M. acknowledges support from AFOSR Awards FA9550-11-1-0275 and FA9550-09-1-0294, AOARD Award FA2386-10-1-4065, Department of the Navy/ONR Award N00014-11-1-0729, DoD/NSSEFF/NPS Awards N00244-09-1-0012 and N00244-09-1-0071, and the Non-Equilibrium Energy Research Center (NERC), an Energy Frontier Research Center funded by DoE/Office of Science/Office of Basic Energy Sciences Award DE-SC0000989. D.J.E. and E.A. acknowledge support from the DoD, Air Force Office of Scientific Research, National Defense Science and Engineering Graduate (NDSEG) Fellowship, 32 CFR 168a. M.R.J. acknowledges a Graduate Research Fellowship from the NSF. Portions of this work were carried out at beamline 12-ID-B at the Advance Photon Source (APS). Use of the APS, an Office of Science User Facility operated for the U. S. Department of Energy (DOE) Office of Science by Argonne National Laboratory, was supported by the U.S. DOE under contract no. DE-AC02-06CH11357. Electron microscopy was performed at the EPIC facility of the NUANCE Center at Northwestern University. NR 38 TC 36 Z9 36 U1 5 U2 102 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 26 BP 6624 EP 6628 DI 10.1002/anie.201301936 PG 5 WC Chemistry, Multidisciplinary SC Chemistry GA 168VJ UT WOS:000320733600009 PM 23681747 ER PT J AU Li, T Zan, XJ Winans, RE Wang, Q Lee, B AF Li, Tao Zan, Xingjie Winans, Randall E. Wang, Qian Lee, Byeongdu TI Biomolecular Assembly of Thermoresponsive Superlattices of the Tobacco Mosaic Virus with Large Tunable Interparticle Distances SO ANGEWANDTE CHEMIE-INTERNATIONAL EDITION LA English DT Article DE depletion force; self-assembly; stimulus-responsive materials; superlattices; viruses ID AQUEOUS-SOLUTION; NANOPARTICLE SUPERLATTICES; CARBOXYMETHYL CELLULOSE; PERSISTENCE LENGTH; LIGHT-SCATTERING; ELECTRIC-FIELD; DNA; CRYSTALLIZATION; PARTICLES; GELS C1 [Li, Tao; Winans, Randall E.; Lee, Byeongdu] Argonne Natl Lab, Xray Sci Div, Lemont, IL 60439 USA. [Zan, Xingjie; Wang, Qian] Univ S Carolina, Dept Chem & Biochem, Columbia, SC 29208 USA. RP Wang, Q (reprint author), Univ S Carolina, Dept Chem & Biochem, Columbia, SC 29208 USA. EM wang263@mailbox.sc.edu; blee@aps.anl.gov RI li, tao/K-8911-2012; OI li, tao/0000-0001-5454-1468; Lee, Byeongdu/0000-0003-2514-8805 FU US DOE [DE-AC02-06CH11357, DE-SC0001477]; US NSF [CHE-0748690]; US DSF [DMR-0706431]; US DoD [W911NF-09-1-0236]; W. M. Keck Foundation FX T.L. and B. L. are thankful for the use of the Advanced Photon Source, an Office of Science User Facility operated for the US Department of Energy (DOE) Office of Science by Argonne National Laboratory; the use of this facility was supported by the US DOE under Contract No. DE-AC02-06CH11357. Q. W. is grateful for financial support from the US NSF (CHE-0748690), the US DSF (DMR-0706431), the US DoD (W911NF-09-1-0236), the US DOE (DE-SC0001477), and the W. M. Keck Foundation. We thank Dr. A. J. Senesi for helpful discussions. NR 48 TC 20 Z9 20 U1 4 U2 41 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 26 BP 6638 EP 6642 DI 10.1002/anie.201209299 PG 5 WC Chemistry, Multidisciplinary SC Chemistry GA 168VJ UT WOS:000320733600012 PM 23681591 ER PT S AU Wilson, RC Doudna, JA AF Wilson, Ross C. Doudna, Jennifer A. BE Dill, KA TI Molecular Mechanisms of RNA Interference SO ANNUAL REVIEW OF BIOPHYSICS, VOL 42 SE Annual Review of Biophysics LA English DT Review; Book Chapter DE miRNA; siRNA; RNAi; dsRNA; Argonaute; Dicer; RISC; ribonucleoproteins; crystallography ID MEDIATED TRANSLATIONAL REPRESSION; EUKARYOTIC ARGONAUTE PROTEIN; RISC-LOADING COMPLEX; CRYSTAL-STRUCTURE; HUMAN DICER; STRUCTURAL INSIGHTS; STRAND SELECTION; PIRNA BIOGENESIS; RIBONUCLEASE-III; HELICASE DOMAIN AB Small RNA molecules regulate eukaryotic gene expression during development and in response to stresses including viral infection. Specialized ribonucleases and RNA-binding proteins govern the production and action of small regulatory RNAs. After initial processing in the nucleus by Drosha, precursor microRNAs (pre-miRNAs) are transported to the cytoplasm, where Dicer cleavage generates mature microRNAs (miRNAs) and short interfering RNAs (siRNAs). These double-stranded products assemble with Argonaute proteins such that one strand is preferentially selected and used to guide sequence-specific silencing of complementary target mRNAs by endonucleolytic cleavage or translational repression. Molecular structures of Dicer and Argonaute proteins, and of RNA-bound complexes, have offered exciting insights into the mechanisms operating at the heart of RNA-silencing pathways. C1 [Doudna, Jennifer A.] Univ Calif Berkeley, Howard Hughes Med Inst, Berkeley, CA 94720 USA. [Wilson, Ross C.; Doudna, Jennifer A.] Univ Calif Berkeley, Dept Mol & Cell Biol, Berkeley, CA 94720 USA. [Doudna, Jennifer A.] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Doudna, Jennifer A.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA 94720 USA. RP Wilson, RC (reprint author), Univ Calif Berkeley, Dept Mol & Cell Biol, 229 Stanley Hall, Berkeley, CA 94720 USA. EM doudna@berkeley.edu FU NIGMS NIH HHS [F32GM096689] NR 103 TC 218 Z9 231 U1 27 U2 176 PU ANNUAL REVIEWS PI PALO ALTO PA 4139 EL CAMINO WAY, PO BOX 10139, PALO ALTO, CA 94303-0897 USA SN 1936-122X BN 978-0-8243-1842-0 J9 ANNU REV BIOPHYS JI Annu. Rev. Biophys. PY 2013 VL 42 BP 217 EP 239 DI 10.1146/annurev-biophys-083012-130404 PG 23 WC Biophysics SC Biophysics GA BFW68 UT WOS:000321695700011 PM 23654304 ER PT S AU Adams, PD Baker, D Brunger, AT Das, R DiMaio, F Read, RJ Richardson, DC Richardson, JS Terwilliger, TC AF Adams, Paul D. Baker, David Brunger, Axel T. Das, Rhiju DiMaio, Frank Read, Randy J. Richardson, David C. Richardson, Jane S. Terwilliger, Thomas C. BE Dill, KA TI Advances, Interactions, and Future Developments in the CNS, Phenix, and Rosetta Structural Biology Software Systems SO ANNUAL REVIEW OF BIOPHYSICS, VOL 42 SE Annual Review of Biophysics LA English DT Review; Book Chapter DE molecular replacement; experimental phasing; structure refinement; model building; validation; physically realistic potential functions; low resolution ID CRYSTALLOGRAPHIC STRUCTURE REFINEMENT; PROTEIN-STRUCTURE REFINEMENT; X-RAY CRYSTALLOGRAPHY; MOLECULAR-REPLACEMENT; STRUCTURE PREDICTION; CRYSTAL-STRUCTURE; ANOMALOUS DIFFRACTION; LOW-RESOLUTION; STRUCTURE VALIDATION; TRYPSIN-INHIBITOR AB Advances in our understanding of macromolecular structure come from experimental methods, such as X-ray crystallography, and also computational analysis of the growing number of atomic models obtained from such experiments. The later analyses have made it possible to develop powerful tools for structure prediction and optimization in the absence of experimental data. In recent years, a synergy between these computational methods for crystallographic structure determination and structure prediction and optimization has begun to be exploited. We review some of the advances in the algorithms used for crystallographic structure determination in the Phenix and Crystallography & NMR System software packages and describe how methods from ab initio structure prediction and refinement in Rosetta have been applied to challenging crystallographic problems. The prospects for future improvement of these methods are discussed. C1 [Adams, Paul D.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Adams, Paul D.] Univ Calif Berkeley, Dept Bioengn, Berkeley, CA 94720 USA. [Baker, David; DiMaio, Frank] Univ Washington, Dept Biochem, Seattle, WA 98195 USA. [Brunger, Axel T.] Stanford Univ, Howard Hughes Med Inst, Stanford, CA 94305 USA. [Brunger, Axel T.] Stanford Univ, Dept Mol & Cellular Physiol, Stanford, CA 94305 USA. [Brunger, Axel T.] Stanford Univ, Dept Neurol & Neurol Sci, Stanford, CA 94305 USA. [Brunger, Axel T.] Stanford Univ, Dept Biol Struct, Stanford, CA 94305 USA. [Brunger, Axel T.] Stanford Univ, Dept Photon Sci, Stanford, CA 94305 USA. [Das, Rhiju] Stanford Univ, Dept Biochem, Stanford, CA 94305 USA. [Das, Rhiju] Stanford Univ, Dept Phys, Stanford, CA 94305 USA. [Read, Randy J.] Cambridge Inst Med Res, Cambridge CB2 0XY, England. [Richardson, David C.; Richardson, Jane S.] Duke Univ, Dept Biochem, Durham, NC 27710 USA. [Terwilliger, Thomas C.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Adams, PD (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. EM PDAdams@lbl.gov; dabaker@u.washington.edu; brunger@stanford.edu; rhiju@stanford.edu; dimaio@u.washington.edu; rjr27@cam.ac.uk; dcrjsr@kinemage.biochem.duke.edu; terwilliger@lanl.gov RI Read, Randy/L-1418-2013; Terwilliger, Thomas/K-4109-2012; Adams, Paul/A-1977-2013; Baker, David/K-8941-2012; OI Read, Randy/0000-0001-8273-0047; Terwilliger, Thomas/0000-0001-6384-0320; Adams, Paul/0000-0001-9333-8219; Baker, David/0000-0001-7896-6217; Brunger, Axel/0000-0001-5121-2036 FU NIGMS NIH HHS [P01 GM063210, GM063210, GM092802-03, R21 GM102716, R21 GM102718-01]; Wellcome Trust [082961] NR 101 TC 26 Z9 26 U1 1 U2 49 PU ANNUAL REVIEWS PI PALO ALTO PA 4139 EL CAMINO WAY, PO BOX 10139, PALO ALTO, CA 94303-0897 USA SN 1936-122X BN 978-0-8243-1842-0 J9 ANNU REV BIOPHYS JI Annu. Rev. Biophys. PY 2013 VL 42 BP 265 EP 287 DI 10.1146/annurev-biophys-083012-130253 PG 23 WC Biophysics SC Biophysics GA BFW68 UT WOS:000321695700013 PM 23451892 ER PT S AU Rambo, RP Tainer, JA AF Rambo, Robert P. Tainer, John A. BE Dill, KA TI Super-Resolution in Solution X-Ray Scattering and Its Applications to Structural Systems Biology SO ANNUAL REVIEW OF BIOPHYSICS, VOL 42 SE Annual Review of Biophysics LA English DT Review; Book Chapter DE macromolecular flexibility; macromolecular interactions; dynamic complexes; X-ray scattering data analysis; SAXS model validation; solution structure quality control metrics ID SMALL-ANGLE SCATTERING; INTRINSICALLY DISORDERED PROTEINS; RESIDUAL DIPOLAR COUPLINGS; LARGE RNA MOLECULES; LOW-RESOLUTION DATA; ESCHERICHIA-COLI; DEOXYRIBONUCLEIC-ACID; NEUTRON-SCATTERING; RIBOSOMAL-SUBUNIT; MACROMOLECULAR STRUCTURES AB Small-angle X-ray scattering (SAXS) is a robust technique for the comprehensive structural characterizations of biological macromolecular complexes in solution. Here, we present a coherent synthesis of SAXS theory and experiment with a focus on analytical tools for accurate, objective, and high-throughput investigations. Perceived SAXS limitations are considered in light of its origins, and we present current methods that extend SAXS data analysis to the super-resolution regime. In particular, we discuss hybrid structural methods, illustrating the role of SAXS in structure refinement with NMR and ensemble refinement with single-molecule FRET. High-throughput genomics and proteomics are far outpacing macromolecular structure determinations, creating information gaps between the plethora of newly identified genes, known structures, and the structure-function relationship in the underlying biological networks. SAXS can bridge these information gaps by providing a reliable, high-throughput structural characterization of macromolecular complexes under physiological conditions. C1 [Rambo, Robert P.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA 94720 USA. [Tainer, John A.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Life Sci, Berkeley, CA 94720 USA. [Tainer, John A.] Scripps Res Inst, Dept Mol Biol, La Jolla, CA 92037 USA. [Tainer, John A.] Scripps Res Inst, Skaggs Inst Chem Biol, La Jolla, CA 92037 USA. RP Rambo, RP (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA 94720 USA. EM rprambo@lbl.gov; jat@scripps.edu FU NCI NIH HHS [P01 CA092584]; NIGMS NIH HHS [R01 GM105404, R01GM105404] NR 132 TC 66 Z9 67 U1 2 U2 55 PU ANNUAL REVIEWS PI PALO ALTO PA 4139 EL CAMINO WAY, PO BOX 10139, PALO ALTO, CA 94303-0897 USA SN 1936-122X BN 978-0-8243-1842-0 J9 ANNU REV BIOPHYS JI Annu. Rev. Biophys. PY 2013 VL 42 BP 415 EP 441 DI 10.1146/annurev-biophys-083012-130301 PG 27 WC Biophysics SC Biophysics GA BFW68 UT WOS:000321695700019 PM 23495971 ER PT J AU Garrett, TJ Zhao, C AF Garrett, T. J. Zhao, C. TI Ground-based remote sensing of thin clouds in the Arctic SO ATMOSPHERIC MEASUREMENT TECHNIQUES LA English DT Article ID MIXED-PHASE CLOUDS; LIQUID WATER; PART I; RADIATION PROPERTIES; OPTICAL-CONSTANTS; BEAUFORT SEA; ICE-CLOUD; SURFACE; SHEBA; STRATUS AB This paper describes a method for using interferometer measurements of downwelling thermal radiation to retrieve the properties of single-layer clouds. Cloud phase is determined from ratios of thermal emission in three "micro-windows" at 862.5 cm(-1), 935.8 cm(-1), and 988.4cm(-1) where absorption by water vapour is particularly small. Cloud microphysical and optical properties are retrieved from thermal emission in the first two of these micro-windows, constrained by the transmission through clouds of primarily stratospheric ozone emission at 1040 cm(-1). Assuming a cloud does not approximate a blackbody, the estimated 95 % confidence retrieval errors in effective radius r(e), visible optical depth tau, number concentration N, and water path WP are, respectively, 10%, 20%, 38 % (55 % for ice crystals), and 16%. Applied to data from the Atmospheric Radiation Measurement programme (ARM) North Slope of Alaska Adjacent Arctic Ocean (NSA-AAO) site near Barrow, Alaska, retrievals show general agreement with both ground-based microwave radiometer measurements of liquid water path and a method that uses combined shortwave and microwave measurements to retrieve r(e), tau and N. Compared to other retrieval methods, advantages of this technique include its ability to characterise thin clouds year round, that water vapour is not a primary source of retrieval error, and that the retrievals of microphysical properties are only weakly sensitive to retrieved cloud phase. The primary limitation is the inapplicability to thicker clouds that radiate as blackbodies and that it relies on a fairly comprehensive suite of ground based measurements. C1 [Garrett, T. J.] Univ Utah, Dept Atmospher Sci, Salt Lake City, UT 84112 USA. [Zhao, C.] Lawrence Livermore Natl Lab, Livermore, CA USA. [Zhao, C.] Beijing Normal Univ, Coll Global Change & Earth Syst Sci, Beijing 100875, Peoples R China. RP Garrett, TJ (reprint author), Univ Utah, Dept Atmospher Sci, Salt Lake City, UT 84112 USA. EM tim.garrett@utah.edu RI Zhao, Chuanfeng/G-8546-2013 FU National Science Foundation [0303962, 0649570]; Clean Air Task Force, through NOAA [2308014]; Ministry of Science and Technology of China [2013CB955804] FX This work was supported by the National Science Foundation through grants 0303962 and 0649570, the Clean Air Task Force, through NOAA by grant 2308014, and the Ministry of Science and Technology of China through grant 2013CB955804. We are grateful to the late P. V. Hobbs for having provided aircraft data, the Word Data Center for Remote Sensing of the Atmosphere for ozone profile data, X. Dong for his cloud retrieval product, and Jay Mace and Sally Benson for plots of the lidar and radar signals. NR 71 TC 9 Z9 9 U1 0 U2 15 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1867-1381 J9 ATMOS MEAS TECH JI Atmos. Meas. Tech. PY 2013 VL 6 IS 5 BP 1227 EP 1243 DI 10.5194/amt-6-1227-2013 PG 17 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA 181OU UT WOS:000321679200009 ER PT J AU Nabat, P Somot, S Mallet, M Chiapello, I Morcrette, JJ Solmon, F Szopa, S Dulac, F Collins, W Ghan, S Horowitz, LW Lamarque, JF Lee, YH Naik, V Nagashima, T Shindell, D Skeie, R AF Nabat, P. Somot, S. Mallet, M. Chiapello, I. Morcrette, J. J. Solmon, F. Szopa, S. Dulac, F. Collins, W. Ghan, S. Horowitz, L. W. Lamarque, J. F. Lee, Y. H. Naik, V. Nagashima, T. Shindell, D. Skeie, R. TI A 4-D climatology (1979-2009) of the monthly tropospheric aerosol optical depth distribution over the Mediterranean region from a comparative evaluation and blending of remote sensing and model products SO ATMOSPHERIC MEASUREMENT TECHNIQUES LA English DT Article ID GLOBAL 3-DIMENSIONAL MODEL; SAHARAN DUST; ATMOSPHERIC CORRECTION; CARBONACEOUS AEROSOLS; AERONET OBSERVATIONS; SYSTEM MODEL; OCEAN; SATELLITE; SIMULATIONS; SEAWIFS AB Since the 1980s several spaceborne sensors have been used to retrieve the aerosol optical depth (AOD) over the Mediterranean region. In parallel, AOD climatologies coming from different numerical model simulations are now also available, permitting to distinguish the contribution of several aerosol types to the total AOD. In this work, we perform a comparative analysis of this unique multiyear database in terms of total AOD and of its apportionment by the five main aerosol types (soil dust, sea-salt, sulfate, black and organic carbon). We use 9 different satellite-derived monthly AOD products: NOAA/AVHRR, SeaWiFS (2 products), TERRA/MISR, TERRA/MODIS, AQUA/MODIS, ENVISAT/MERIS, PARASOL/POLDER and MSG/SEVIRI, as well as 3 more historical datasets: NIMBUS7/CZCS, TOMS (onboard NIMBUS7 and Earth- Probe) and METEOSAT/MVIRI. Monthly model datasets include the aerosol climatology from Tegen et al. (1997), the climate-chemistry models LMDz-OR-INCA and RegCM-4, the multi-model mean coming from the ACCMIP exercise, and the reanalyses GEMS and MACC. Ground-based Level-2 AERONET AOD observations from 47 stations around the basin are used here to evaluate the model and satellite data. The sensor MODIS (on AQUA and TERRA) has the best average AOD scores over this region, showing a relevant spatio-temporal variability and highlighting high dust loads over Northern Africa and the sea (spring and summer), and sulfate aerosols over continental Europe (summer). The comparison also shows limitations of certain datasets (especially MERIS and SeaWiFS standard products). Models reproduce the main patterns of the AOD variability over the basin. The MACC reanalysis is the closest to AERONET data, but appears to underestimate dust over Northern Africa, where RegCM-4 is found closer to MODIS thanks to its interactive scheme for dust emissions. The vertical dimension is also investigated using the CALIOP instrument. This study confirms differences of vertical distribution between dust aerosols showing a large vertical spread, and other continental and marine aerosols which are confined in the boundary layer. From this compilation, we propose a 4-D blended product from model and satellite data, consisting in monthly time series of 3-D aerosol distribution at a 50 km horizontal resolution over the Euro-Mediterranean marine and continental region for the 2003-2009 period. The product is based on the total AOD from AQUA/MODIS, apportioned into sulfates, black and organic carbon from the MACC reanalysis, and into dust and sea-salt aerosols from RegCM-4 simulations, which are distributed vertically based on CALIOP climatology. We extend the 2003-2009 reconstruction to the past up to 1979 using the 2003-2009 average and applying the decreasing trend in sulfate aerosols from LMDz-OR-INCA, whose AOD trends over Europe and the Mediterranean are median among the ACCMIP models. Finally optical properties of the different aerosol types in this region are proposed from Mie calculations so that this reconstruction can be included in regional climate models for aerosol radiative forcing and aerosol-climate studies. C1 [Nabat, P.; Somot, S.] Meteo France, CNRS CNRM GAME, UMR3589, Ctr Natl Rech Meteorol, F-31057 Toulouse 1, France. [Mallet, M.] Lab Aerol, UMR 5560, F-31400 Toulouse, France. [Chiapello, I.] Univ Lille 1, CNRS, UMR 8518, Opt Atmospher Lab, F-59655 Villeneuve Dascq, France. [Morcrette, J. J.] European Ctr Medium Range Weather Forecasts, Reading, Berks, England. [Solmon, F.] Abdus Salam Int Ctr Theroret Phys, I-34100 Trieste, Italy. [Szopa, S.; Dulac, F.] CEA CNRS UVSQ, LSCE IPSL, Lab Sci Climat & Environm, F-91191 Gif Sur Yvette, France. [Collins, W.] Univ Reading, Dept Meteorol, Reading RG6 2AH, Berks, England. [Ghan, S.] Pacific NW Natl Lab, Richland, WA 99352 USA. [Horowitz, L. W.] NOAA, Geophys Fluid Dynam Lab, Princeton, NJ USA. [Lamarque, J. F.] Natl Ctr Atmospher Res, NCAR Earth Syst Lab, Boulder, CO 80307 USA. [Lee, Y. H.; Shindell, D.] NASA, Goddard Inst Space Studies, New York, NY 10025 USA. [Lee, Y. H.; Shindell, D.] NASA, Columbia Earth Inst, New York, NY 10025 USA. [Naik, V.] NOAA, UCAR, Geophys Fluid Dynam Lab, Princeton, NJ USA. [Nagashima, T.] Natl Inst Environm Studies, Tsukuba, Ibaraki, Japan. [Skeie, R.] CICERO, Oslo, Norway. RP Nabat, P (reprint author), Meteo France, CNRS CNRM GAME, UMR3589, Ctr Natl Rech Meteorol, 42 Ave G Coriolis, F-31057 Toulouse 1, France. EM pierre.nabat@meteo.fr RI Collins, William/A-5895-2010; Szopa, Sophie/F-8984-2010; Shindell, Drew/D-4636-2012; Horowitz, Larry/D-8048-2014; Naik, Vaishali/A-4938-2013; Lamarque, Jean-Francois/L-2313-2014; Skeie, Ragnhild/K-1173-2015; Ghan, Steven/H-4301-2011; Lee, Yunha/Q-7222-2016 OI Somot, Samuel/0000-0002-5066-2921; Collins, William/0000-0002-7419-0850; Szopa, Sophie/0000-0002-8641-1737; Horowitz, Larry/0000-0002-5886-3314; Naik, Vaishali/0000-0002-2254-1700; Lamarque, Jean-Francois/0000-0002-4225-5074; Skeie, Ragnhild/0000-0003-1246-4446; Ghan, Steven/0000-0001-8355-8699; Lee, Yunha/0000-0001-7478-2672 FU French National Research Agency (ANR) project ADRIMED [ANR-11-BS56-0006]; FP7 European Commission project CLIMRUN [FP7-ENV-2010-265192]; European Commission [SIP4-CT-2004-516099]; MACC [218793]; National Science Foundation; Office of Science (BER) of the US Department of Energy FX We would like to thank Meteo-France for the financial support of the first author. This work is part of the Med-CORDEX initiative (www.medcordex.eu) and a contribution to the HyMeX and ChArMEx programmes. This new AOD climatology is indeed available on the ChArMEx database (http://mistrals.sedoo.fr/ChArMEx). This research has received funding from the French National Research Agency (ANR) project ADRIMED (contract ANR-11-BS56-0006) and from the FP7 European Commission project CLIMRUN (contract FP7-ENV-2010-265192). MODIS and MERIS data used in this paper were retrieved from the Giovanni online data system, developed and maintained by the NASA GES DISC. MISR and CALIOP data were obtained from the NASA Langley Research Center Atmospheric Science Data Center, SeaWiFS and CZCS data from the NASA Ocean Biology Processing Group, AVHRR data from the NOAA/National Climatic Data Center and TOMS data from the NASA/GSFC TOMS group. We also thank the ICARE Data and Services Center for providing access to the PARASOL and SEVIRI data used in this study, and Cyril Moulin for providing his historical MVIRI data. We thank the PI investigators of the different AERONET stations and their staff for establishing and maintaining all the sites used in this investigation. GEMS was funded by the European Commission between 2004 and 2009 as part of the 6th Framework Programme under contract number SIP4-CT-2004-516099, and MACC was funded between 2009 and 2011 as part of the 7th Framework Programme, pilot core GMES Atmospheric Service under contract number 218793. We thank all the people taking part in the ACCMIP project, notably other scientists involved in the development of models, namely Toshihiko Takemura and Kengo Sudo for MIROC-CHEM, Stig Dalsoren for CICERO-OsloCTM2, and Greg Faluvegi for GISS-E2-R. The CESM project (which includes NCAR-CAM3.5 and NCAR-CAM5.1) is supported by the National Science Foundation and the Office of Science (BER) of the US Department of Energy. The National Center for Atmospheric Research is operated by the University Corporation for Atmospheric Research under sponsorship of the National Science Foundation. NR 124 TC 33 Z9 33 U1 2 U2 35 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1867-1381 EI 1867-8548 J9 ATMOS MEAS TECH JI Atmos. Meas. Tech. PY 2013 VL 6 IS 5 BP 1287 EP 1314 DI 10.5194/amt-6-1287-2013 PG 28 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA 181OU UT WOS:000321679200013 ER PT J AU Morgado, L Dantas, JM Simoes, T Londer, YY Pokkuluri, PR Salgueiro, CA AF Morgado, Leonor Dantas, Joana M. Simoes, Telma Londer, Yuri Y. Raj Pokkuluri, P. Salgueiro, Carlos A. TI Role of Met(58) in the regulation of electron/proton transfer in trihaem cytochrome PpcA from Geobacter sulfurreducens SO BIOSCIENCE REPORTS LA English DT Article DE electron transfer; Geobacter; multihaem cytochrome; NMR site-directed mutagenesis ID C-TYPE CYTOCHROME; ESCHERICHIA-COLI; THERMODYNAMIC CHARACTERIZATION; SUBSURFACE ENVIRONMENTS; DESULFOVIBRIO-VULGARIS; RESIDUE F-15; C(7); FAMILY; REDUCTION; FE(III) AB The bacterium Gs (Geobacter sulfurreducens) is capable of oxidizing a large variety of compounds relaying electrons out of the cytoplasm and across the membranes in a process designated as extracellular electron transfer. The trihaem cytochrome PpcA is highly abundant in Gs and is most probably the reservoir of electrons destined for the outer surface. In addition to its role in electron transfer pathways, we have previously shown that this protein could perform e(-)/H+ energy transduction. This mechanism is achieved by selecting the specific redox states that the protein can access during the redox cycle and might be related to the formation of proton electrochemical potential gradient across the periplasmic membrane. The regulatory role of haem III in the functional mechanism of PpcA was probed by replacing Met(58), a residue that controls the solvent accessibility of haem III, with serine, aspartic acid, asparagine or lysine. The data obtained from the mutants showed that the preferred e(-)/H+ transfer pathway observed for PpcA is strongly dependent on the reduction potential of haem III. It is striking to note that one residue can fine tune the redox states that can be accessed by the trihaem cytochrome enough to alter the functional pathways. C1 [Morgado, Leonor; Dantas, Joana M.; Simoes, Telma; Salgueiro, Carlos A.] Univ Nova Lisboa, Fac Ciencias & Tecnol, Dept Quim, Requimte CQFB, P-2829516 Caparica, Portugal. [Londer, Yuri Y.; Raj Pokkuluri, P.] Argonne Natl Lab, Biosci Div, Argonne, IL 60439 USA. RP Salgueiro, CA (reprint author), Univ Nova Lisboa, Fac Ciencias & Tecnol, Dept Quim, Requimte CQFB, Campus Caparica, P-2829516 Caparica, Portugal. EM csalgueiro@fct.unl.pt RI Caparica, cqfb_staff/H-2611-2013; REQUIMTE, AL/H-9106-2013; Salgueiro, Carlos/A-4522-2013; REQUIMTE, UCIBIO/N-9846-2013; Caparica, PTNMR/E-5112-2013; Morgado, Leonor/D-7387-2013; Dantas, Joana/B-8275-2017 OI Salgueiro, Carlos/0000-0003-1136-809X; Morgado, Leonor/0000-0002-3760-5180; Dantas, Joana/0000-0002-4852-7608 FU Fundacao para a Ciencia e Tecnologia (Portugal) [PTDC/QUI/70182/2006, PEst-C/EQB/LA006/2011]; Fundacao para a Ciencia e a Tecnologia (FCT); U.S. Department of Energy Office of Biological and Environmental Research [DE-AC02-06CH11357]; division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences of the U.S. Department of Energy [DE-AC02-06CH11357] FX This work was supported by the Fundacao para a Ciencia e Tecnologia (Portugal) [grant numbers PTDC/QUI/70182/2006, PEst-C/EQB/LA006/2011]. The NMR spectrometers are part of the National NMR Network (RNRMN) and are funded by the Fundacao para a Ciencia e a Tecnologia (FCT). The Met58 mutants were produced at ANL with support from U.S. Department of Energy Office of Biological and Environmental Research [grant number DE-AC02-06CH11357]. The structural analysis of the mutants is supported by the division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences of the U.S. Department of Energy [grant number DE-AC02-06CH11357]. NR 34 TC 7 Z9 7 U1 0 U2 5 PU PORTLAND PRESS LTD PI LONDON PA THIRD FLOOR, EAGLE HOUSE, 16 PROCTER STREET, LONDON WC1V 6 NX, ENGLAND SN 0144-8463 J9 BIOSCIENCE REP JI Biosci. Rep. PY 2013 VL 33 BP 11 EP U28 AR UNSP e00002 DI 10.1042/BSR20120086 PN 1 PG 16 WC Biochemistry & Molecular Biology; Cell Biology SC Biochemistry & Molecular Biology; Cell Biology GA 175PJ UT WOS:000321242600002 PM 23030844 ER PT J AU He, YB Furukawa, H Wu, CD O'Keeffe, M Krishna, R Chen, BL AF He, Yabing Furukawa, Hiroyasu Wu, Chuande O'Keeffe, Michael Krishna, Rajamani Chen, Banglin TI Low-energy regeneration and high productivity in a lanthanide-hexacarboxylate framework for high-pressure CO2-CH4-H-2 separation SO CHEMICAL COMMUNICATIONS LA English DT Article ID METAL-ORGANIC FRAMEWORKS; CARBON-DIOXIDE CAPTURE; SMALL HYDROCARBONS; NATURAL-GAS; CO2 UPTAKE; PURIFICATION; ADSORPTION; THERMODYNAMICS; TRICARBOXYLATE; HYDROGEN AB A porous lanthanide-organic framework UTSA-62a of a jjt-a topology has been synthesized from a hexacarboxylate and structurally characterized, exhibiting significant potential for use in CO2-CH4-H-2 separation (H-2 purification) processes with high productivities and low regeneration costs when operating at high pressure and room temperature. C1 [He, Yabing] Zhejiang Normal Univ, Coll Chem & Life Sci, Jinhua 321004, Peoples R China. [Furukawa, Hiroyasu] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Dept Chem, Div Mat Sci, Berkeley, CA 94720 USA. [Wu, Chuande] Zhejiang Univ, Dept Chem, Hangzhou 310027, Zhejiang, Peoples R China. [O'Keeffe, Michael] Arizona State Univ, Dept Chem & Biochem, Tempe, AZ 85287 USA. [Krishna, Rajamani] Univ Amsterdam, Vant Hoff Inst Mol Sci, NL-1098 XH Amsterdam, Netherlands. [Chen, Banglin] Univ Texas San Antonio, Dept Chem, San Antonio, TX 78249 USA. RP He, YB (reprint author), Zhejiang Normal Univ, Coll Chem & Life Sci, Jinhua 321004, Peoples R China. EM heyabing@gmail.com; r.krishna@nva.nl; banglin.chen@utsa.edu RI Chen, Banglin/F-5461-2010; Krishna, Rajamani/A-1098-2012; Wu, Chuan-De/B-7546-2013; He, Yabing/H-3314-2012; Furukawa, Hiroyasu/C-5910-2008 OI Chen, Banglin/0000-0001-8707-8115; Krishna, Rajamani/0000-0002-4784-8530; Furukawa, Hiroyasu/0000-0002-6082-1738 NR 34 TC 31 Z9 31 U1 4 U2 70 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 60 BP 6773 EP 6775 DI 10.1039/c3cc43196g PG 3 WC Chemistry, Multidisciplinary SC Chemistry GA 175DJ UT WOS:000321209800022 PM 23783245 ER PT J AU Butcher, DR Zhu, ZW Mao, BH Wang, HL Liu, Z Salmeron, M Somorjai, GA AF Butcher, Derek R. Zhu, Zhongwei Mao, Baohua Wang, Hailiang Liu, Zhi Salmeron, Miquel Somorjai, Gabor A. TI Mobility on the reconstructed Pt(100)-hex surface in ethylene and in its mixture with hydrogen and carbon monoxide SO CHEMICAL COMMUNICATIONS LA English DT Article ID SCANNING-TUNNELING-MICROSCOPY; PT(111); CO; PLATINUM; COADSORPTION; ADSORPTION; SPECTROSCOPY; CATALYST; COVERAGE; STM AB By using high-pressure scanning tunneling microscopy and ambient-pressure X-ray photoelectron spectroscopy, we studied the mobility along with composition, structure and reactivity on the Pt(100)-hex surface. Adsorbates are mobile under 1 Torr of C2H4 and C2H4-H-2 mixtures, but adding 3 mTorr of CO quenches the mobility. Ethylene-related adsorbates can also weaken Pt-Pt bonds and thus facilitate displacements in the hexagonal layer. C1 [Butcher, Derek R.; Zhu, Zhongwei; Wang, Hailiang; Somorjai, Gabor A.] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Butcher, Derek R.; Zhu, Zhongwei; Wang, Hailiang; Salmeron, Miquel; Somorjai, Gabor A.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. [Mao, Baohua; Liu, Zhi] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. [Salmeron, Miquel] Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA. RP Salmeron, M (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. EM mbsamelron@lbl.gov; somorjai@berkeley.edu RI Liu, Zhi/B-3642-2009 OI Liu, Zhi/0000-0002-8973-6561 FU Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division, of the U.S. Department of Energy [DE-AC02-05CH11231]; Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231]; Philomathia Postdoctoral Fellowship 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 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. H.W. acknowledges support from the Philomathia Postdoctoral Fellowship. NR 22 TC 4 Z9 4 U1 0 U2 31 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 61 BP 6903 EP 6905 DI 10.1039/c3cc42312c PG 3 WC Chemistry, Multidisciplinary SC Chemistry GA 177OH UT WOS:000321384200026 PM 23800761 ER PT J AU Summerscales, OT Gordon, JC AF Summerscales, Owen T. Gordon, John C. TI Regeneration of ammonia borane from spent fuel materials SO DALTON TRANSACTIONS LA English DT Article ID CHEMICAL HYDROGEN STORAGE; THERMODYNAMIC PROPERTIES; THERMAL-DECOMPOSITION; COMPLEXES M; LARGE-SCALE; HIGH-YIELD; THERMOCHEMISTRY; HYDRIDE; ROUTE; DEHYDROGENATION AB A shift to the hydrogen economy requires the development of an effective hydrogen fuel carrier with high volumetric and gravimetric storage capacity. Ammonia borane (AB) has emerged as a leading candidate due to its light weight and multiple protic (N-H) and hydridic (B-H) hydrogens. As a consequence, much work has been directed towards fine tuning the release of H-2 from AB, in addition to its regeneration from the dehydrogenated "spent fuel" materials. This review summarizes the development of these regeneration methodologies. C1 [Summerscales, Owen T.; Gordon, John C.] Los Alamos Natl Lab, Div Chem, MS J582, Los Alamos, NM 87545 USA. RP Gordon, JC (reprint author), Los Alamos Natl Lab, Div Chem, MS J582, POB 1663, Los Alamos, NM 87545 USA. EM jgordon@lanl.gov NR 65 TC 24 Z9 25 U1 2 U2 58 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 28 BP 10075 EP 10084 DI 10.1039/c3dt50475a PG 10 WC Chemistry, Inorganic & Nuclear SC Chemistry GA 170ST UT WOS:000320874600001 PM 23571860 ER PT J AU Kreller, CR Wilson, MS Mukundan, R Brosha, EL Garzon, FH AF Kreller, Cortney R. Wilson, Mahlon S. Mukundan, Rangachary Brosha, Eric L. Garzon, Fernando H. TI Stability and Conductivity of In3+-Doped SnP2O7 with Varying Phosphorous to Metal Ratios SO ECS ELECTROCHEMISTRY LETTERS LA English DT Article ID PROTONIC CONDUCTORS AB In-doped tin pyrophosphate materials were synthesized with varying metal to phosphate ratios to assess the influence of an excess amorphous polyphosphate phase on conductivity. Total conductivity at 250 degrees C increased with phosphorus to metal (P:M) ratio, with the 2.81 P:M ratio material exhibiting maximum conductivity of 10(-2) and 10(-1) Scm(-1) in dry and humidified N-2. XRD measurements revealed no systematic change in lattice parameter with increasing P:M. These results combined with supporting spectroscopy, suggest that a grain-boundary polyphosphate phase is required to achieve high conductivity in the low-intermediate temperature range. The materials were relatively stable and provided steady conductivities at 250 degrees C. (c) 2013 The Electrochemical Society. C1 [Kreller, Cortney R.; Wilson, Mahlon S.; Mukundan, Rangachary; Brosha, Eric L.; Garzon, Fernando H.] Los Alamos Natl Lab, Sensors & Electrochem Devices Grp, Los Alamos, NM 87545 USA. RP Kreller, CR (reprint author), Los Alamos Natl Lab, Sensors & Electrochem Devices Grp, POB 1663, Los Alamos, NM 87545 USA. EM ckreller@lanl.gov OI Kreller, Cortney/0000-0003-2180-2494; Wilson, Mahlon/0000-0002-5944-2650; Mukundan, Rangachary/0000-0002-5679-3930 NR 18 TC 4 Z9 4 U1 1 U2 16 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 2162-8726 J9 ECS ELECTROCHEM LETT JI ECS Electrochem. Lett. PY 2013 VL 2 IS 9 BP F61 EP F63 DI 10.1149/2.002309eel PG 3 WC Electrochemistry; Materials Science, Multidisciplinary SC Electrochemistry; Materials Science GA 182PE UT WOS:000321755400004 ER PT J AU Shenai, K Dudley, M Davis, RF AF Shenai, Krishna Dudley, Michael Davis, Robert F. TI Current Status and Emerging Trends in Wide Bandgap (WBG) Semiconductor Power Switching Devices SO ECS JOURNAL OF SOLID STATE SCIENCE AND TECHNOLOGY LA English DT Article ID CARBIDE SINGLE-CRYSTALS; P-N-JUNCTION; SILICON-CARBIDE; MATERIAL DEFECTS; BIPOLAR-DEVICES; LARGE-AREA; GROWTH; DIODES; BULK; GAN AB The current state-of-the-art of wide bandgap (WBG) semiconductor material technology is reviewed for the manufacturing of high-performance and reliable power electronics switching devices. In particular, silicon carbide (SiC) and gallium nitride (GaN) material and device technologies are evaluated when compared to conventional silicon power switching devices. For commercial applications above 400 volts, SiC stands out as a viable near-term commercial opportunity especially for single-chip current ratings in excess of 20 amps. For voltage ratings below 900 volts and smaller currents (below 20 amps), lateral GaN power transistors that utilize two-dimensional electron gas (2DEG) are promising candidates. At the time of this writing, field-reliability of WBG power devices is yet to be demonstrated in power converter applications. The exact role of high-density of material defects in both SiC and GaN semiconductors, primarily in the drift-region of the device, is not known from manufacturing and reliability considerations. This fundamental understanding is critical in order for WBG power devices to rapidly penetrate the vast commercial and strategic markets. (C) 2013 The Electrochemical Society. All rights reserved. C1 [Shenai, Krishna] Argonne Natl Lab, Div Energy Syst, Argonne, IL 60439 USA. [Dudley, Michael] SUNY Stony Brook, Dept Mat Sci & Engn, Stony Brook, NY 11794 USA. [Davis, Robert F.] Carnegie Mellon Univ, Dept Mat Sci & Engn, Pittsburgh, PA 15213 USA. RP Shenai, K (reprint author), Argonne Natl Lab, Div Energy Syst, 9700 S Cass Ave, Argonne, IL 60439 USA. EM kshenai@anl.gov RI Davis, Robert/A-9376-2011 OI Davis, Robert/0000-0002-4437-0885 FU U.S. Department of Energy Office of Science laboratory [DE-AC02-06CH11357] FX The submitted manuscript has been created by UChicago Argonne, LLC, Operator of Argonne National Laboratory ("Argonne"). Argonne, a U.S. Department of Energy Office of Science laboratory, is operated under Contract 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 69 TC 13 Z9 13 U1 2 U2 27 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 2162-8769 J9 ECS J SOLID STATE SC JI ECS J. Solid State Sci. Technol. PY 2013 VL 2 IS 8 BP N3055 EP N3063 DI 10.1149/2.012308jss PG 9 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA 180TJ UT WOS:000321619700008 ER PT J AU Lieten, RR Douhard, B Stesmans, A Jivanescu, M Beeman, JW Simoen, E Vandervorst, W Haller, EE Locquet, JP AF Lieten, R. R. Douhard, B. Stesmans, A. Jivanescu, M. Beeman, J. W. Simoen, E. Vandervorst, W. Haller, E. E. Locquet, J. -P. TI Implantation and Activation of Phosphorus in Amorphous and Crystalline Germanium Layers SO ECS JOURNAL OF SOLID STATE SCIENCE AND TECHNOLOGY LA English DT Article ID ION-IMPLANTATION; DIFFUSION; JUNCTIONS; REGROWTH; GE AB We have investigated phosphorus implantation and activation in amorphous and crystalline Ge layers, deposited on Si substrates. The structure of the Ge layer has only limited influence on the dopant profile and diffusion after annealing. Surprisingly, crystalline Ge layers show better electrical results after implantation and dopant activation. For the amorphous layer, the solid phase epitaxy process is influenced in the neighborhood of P, leading to point defects, which inhibit electrical activation. This result implies that when a crystalline Ge layer is amorphized during implantation of high doses, the dopant activation can be significantly reduced. Reduced temperature ramping improves activation of P in amorphous Ge layers. (C) 2013 The Electrochemical Society. All rights reserved. C1 [Lieten, R. R.; Stesmans, A.; Jivanescu, M.; Vandervorst, W.; Locquet, J. -P.] Katholieke Univ Leuven, Dept Phys & Astron, Louvain, Belgium. [Lieten, R. R.; Beeman, J. W.; Haller, E. E.] Lawrence Berkeley Natl Lab, Div Sci Mat, Berkeley, CA 94704 USA. [Lieten, R. R.; Douhard, B.; Simoen, E.; Vandervorst, W.] IMEC, B-3001 Louvain, Belgium. [Haller, E. E.] Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94704 USA. RP Lieten, RR (reprint author), Katholieke Univ Leuven, Dept Phys & Astron, Louvain, Belgium. EM ruben.lieten@gmail.com FU Belgian American Educational Foundation (BAEF); Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division, of the U.S. DOE [DE-AC02-05CH11231] FX R.R.L acknowledges support as Research Fellow of the Research Foundation - Flanders (FWO) and support of the Belgian American Educational Foundation (BAEF). Some of the authors (R. R. Lieten, J.W Beeman, and E. E. Haller) acknowledge support by the Director, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division, of the U.S. DOE under Contract No. DE-AC02-05CH11231. NR 22 TC 0 Z9 0 U1 2 U2 11 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 2162-8769 J9 ECS J SOLID STATE SC JI ECS J. Solid State Sci. Technol. PY 2013 VL 2 IS 9 BP P346 EP P350 DI 10.1149/2.011309jss PG 5 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA 180TQ UT WOS:000321620800009 ER PT J AU Ramprasad, S Su, YW Chang, CH Paul, BK Palo, DR AF Ramprasad, Sudhir Su, Yu-Wei Chang, Chih-Hung Paul, Brian K. Palo, Daniel R. TI Continuous Microreactor-Assisted Solution Deposition for Scalable Production of CdS Films SO ECS JOURNAL OF SOLID STATE SCIENCE AND TECHNOLOGY LA English DT Article ID CHEMICAL BATH DEPOSITION; CONTINUOUS-FLOW MICROREACTOR; CUIN1-XGA(X)SE-2-BASED PHOTOVOLTAIC CELLS; CADMIUM-SULFIDE FILMS; SOLAR-CELLS; THIN-FILMS; PRECURSOR FILMS; TELLURIDE; KINETICS; GROWTH AB Solution deposition offers an attractive, low temperature option in the cost effective production of thin film solar cells. Continuous microreactor-assisted solution deposition (MASD) was used to produce nanocrystalline cadmium sulfide (CdS) films on fluorine doped tin oxide (FTO) coated glass substrates with excellent uniformity. We report a novel liquid coating technique using a ceramic rod to efficiently and uniformly apply reactive solution to large substrates (152 mm x 152 mm). This technique represents an inexpensive approach to utilize the MASD on the substrate for uniform growth of CdS films. Nano-crystalline CdS films have been produced from liquid phase at similar to 90 degrees C, with average thicknesses of 70 nm to 230 nm and with a 5 to 12% thickness variation. The CdS films produced were characterized by UV-Vis spectroscopy, transmission electron microscopy, and X-Ray diffraction to demonstrate their suitability to thin-film solar technology. (C) 2013 The Electrochemical Society. All rights reserved. C1 [Ramprasad, Sudhir; Palo, Daniel R.] Pacific NW Natl Lab, Energy Proc & Mat Div, Corvallis, OR 97330 USA. [Ramprasad, Sudhir; Su, Yu-Wei; Chang, Chih-Hung; Paul, Brian K.; Palo, Daniel R.] Microprod Breakthrough Inst, Corvallis, OR 97330 USA. [Ramprasad, Sudhir; Su, Yu-Wei; Chang, Chih-Hung; Paul, Brian K.; Palo, Daniel R.] Oregon Proc Innovat Ctr, Corvallis, OR 97330 USA. [Su, Yu-Wei; Chang, Chih-Hung] Oregon State Univ, Sch Chem Biol & Environm Engn, Corvallis, OR 97331 USA. [Paul, Brian K.] Oregon State Univ, Sch Mech Ind & Mfg Engn, Corvallis, OR 97331 USA. RP Ramprasad, S (reprint author), Pacific NW Natl Lab, Energy Proc & Mat Div, Corvallis, OR 97330 USA. EM sudhir.ramprasad@pnnl.gov FU U.S. Department of Energy, Industrial Technologies Program [NT08847, DE-AC-05-RL01830]; Oregon Nanoscience and Microtechnologies Institute (ONAMI) FX The work described herein was funded by the U.S. Department of Energy, Industrial Technologies Program, through award #NT08847, under contract DE-AC-05-RL01830 to PNNL. Additional funds were received from the Oregon Nanoscience and Microtechnologies Institute (ONAMI) under a matching grant to Oregon State University. The facilities and equipment resident at the Microproducts Breakthrough Institute and the Oregon Process Innovation Center were crucial in conducting this study. Furthermore, we extend our thanks to Don Higgins and to Dr. Jair Lizarazo-Adarme for their assistance with set up of data acquisition and control. We are thankful to the staff at Oregon State University Microscope Facility for their assistance with TEM imaging. NR 32 TC 1 Z9 1 U1 0 U2 12 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 2162-8769 J9 ECS J SOLID STATE SC JI ECS J. Solid State Sci. Technol. PY 2013 VL 2 IS 9 BP P333 EP P337 DI 10.1149/2.003309jss PG 5 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA 180TQ UT WOS:000321620800007 ER PT J AU Moreira, AS Horgan, FG Murray, TE Kakouli-Duarte, T AF Moreira, Antonio S. Horgan, Finbarr G. Murray, Tomas E. Kakouli-Duarte, Thomais TI Bumblebee (Hymenoptera: Apidae) sample storage for a posteriori molecular studies: Interactions between sample storage and DNA-extraction techniques SO EUROPEAN JOURNAL OF ENTOMOLOGY LA English DT Article DE Hymenoptera; Apidae; Bombus terrestris; acetone; commercial kit; DNA quality; entomological pins; freezing; phenol-extraction ID BOMBUS-TERRESTRIS; BEES BOMBUS; PRESERVATION; SPECIMENS; CONSERVATION; COLLECTION; DIVERSITY; TAXONOMY; FLIES; PCR AB A global decline in pollinator abundance and diversity has demanded increased research attention to the ecology and genetics of bumblebees. However, as progressively more restrictions are placed on sampling for insects, researchers are increasingly obliged to use archival specimens collected for purposes other than genetic analyses. In this study we assessed the suitability, for population genetic studies, of popular, low-cost methods for preservation and storage of bumblebee specimens. Specimens of Bombus terrestris L. were held under six storage regimes for up to two years. DNA was extracted from the samples using three extraction protocols and the quality of the DNA was examined using PCR amplification of a mitochondrial and a nuclear gene. All extraction and storage methods provided sufficient DNA for successful PCR amplification. However, samples preserved in acetone or at freezing temperatures yielded the highest DNA concentrations. DNA yields from pinned specimens at room temperature declined over time, particularly when using standard extraction techniques. DNA concentrations were significantly lower from specimens preserved in 70% ethanol compared to all other extraction techniques and declined linearly over the two years of storage. These results indicate that two of the most popular insect storage methods (pinning and storage in ethanol) should be avoided for the long-term preservation of genetic material for future studies. We suggest that optimal insect preservation methods should be incorporated into research protocols in order to best capitalise on limited collection opportunities. C1 [Moreira, Antonio S.; Kakouli-Duarte, Thomais] Inst Technol Carlow, Carlow, County Carlow, Ireland. [Moreira, Antonio S.; Horgan, Finbarr G.; Murray, Tomas E.] TEAGASC, Agri Res & Advisory Author, Oak Pk Res Ctr, Carlow, County Carlow, Ireland. RP Moreira, AS (reprint author), Inst Technol Carlow, Kilkenny Rd, Carlow, County Carlow, Ireland. EM Antonio.Moreira@itcarlow.ie; f.horgan@irri.org; tomas.murray@zoologie.uni-halle.de; thomae.kakouli@itcarlow.ie RI Murray, Tomas/C-5540-2013 FU Irish Department of Agriculture, Food and the Marine [RSF 06 348] FX Funding for this research was provided by the Irish Department of Agriculture, Food and the Marine as part of a research stimulus grant (RSF 06 348). We thank S. Boyle for his support during early stages of this research and anonymous reviewers for several helpful comments that improved the manuscript. NR 38 TC 3 Z9 3 U1 2 U2 26 PU CZECH ACAD SCI, INST ENTOMOLOGY PI CESKE BUDEJOVICE PA BRANISOVSKA 31, CESKE BUDEJOVICE 370 05, CZECH REPUBLIC SN 1210-5759 J9 EUR J ENTOMOL JI Eur. J. Entomol. PY 2013 VL 110 IS 3 BP 419 EP 425 PG 7 WC Entomology SC Entomology GA 173XW UT WOS:000321117200004 ER PT J AU Beaumont, SK Alayoglu, S Pushkarev, VV Liu, Z Kruse, N Somorjai, GA AF Beaumont, Simon K. Alayoglu, Selim Pushkarev, Vladimir V. Liu, Zhi Kruse, Norbert Somorjai, Gabor A. TI Exploring surface science and restructuring in reactive atmospheres of colloidally prepared bimetallic CuNi and CuCo nanoparticles on SiO2 in situ using ambient pressure X-ray photoelectron spectroscopy SO FARADAY DISCUSSIONS LA English DT Article ID CORE-SHELL NANOPARTICLES; OXIDE FUEL-CELLS; SEGREGATION; OXIDATION; CATALYSTS; ALLOYS; NANOCATALYSTS; CHEMISTRY; EVOLUTION; METHANE AB Bimetallic nanoparticles (similar to 11 nm diameter) of CuNi and CuCo were prepared by a new synthetic route and the 1 : 1 atomic ratio of their constituent elements confirmed using STEM-EDS at a single particle level. These nanoparticles, supported on the native oxide layer of a silicon wafer, were studied in situ in a series of reactive gas atmospheres (H-2 -> CO or CO/H-2 -> O-2 -> H-2) using ambient pressure X-ray photoelectron spectroscopy (AP-XPS). Despite the deliberate similarity of nickel and cobalt with respect to copper, their restructuring behaviour is different. CuNi nanoparticles were found to surface segregate nickel in H-2, but copper in O-2 reversibly, while CuCo nanoparticles were found to surface segregate copper irreversibly when exposed to O-2, such that the surface remains copper rich when re-exposed to H-2. Both systems also restructure in opposition to the behaviour predicted by the surface free energies and enthalpies of oxide formation of the elements from which they are comprised - factors that are seen to control restructuring and surface segregation in many similar systems. C1 [Beaumont, Simon K.; Alayoglu, Selim; Pushkarev, Vladimir V.; Somorjai, Gabor A.] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Somorjai, Gabor A.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. [Liu, Zhi] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. [Kruse, Norbert] Univ Libre Brussels, B-1050 Brussels, Belgium. RP Somorjai, GA (reprint author), Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. EM somorjai@berkeley.edu RI Liu, Zhi/B-3642-2009; Foundry, Molecular/G-9968-2014; Beaumont, Simon/F-5272-2012 OI Liu, Zhi/0000-0002-8973-6561; Beaumont, Simon/0000-0002-1973-9783 FU Office of Sciences, Office of Basic Energy Sciences, Division of Material Sciences of the US Department of Energy (DOE) [DE-AC02-05CH11231]; Total, France; Office of Science, Office of Basic Energy Sciences, of the US Department of Energy [DE-AC02-05CH11231] FX GAS acknowledges support from the Director, Office of Sciences, Office of Basic Energy Sciences, Division of Material Sciences of the US Department of Energy (DOE) under contract DE-AC02-05CH11231. NK gratefully acknowledges funding from Total, France. The user work at the Advanced Light Source and Molecular Foundry is 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 also grateful to Rui Chang at Beamline 9.3.2 for his practical assistance. NR 40 TC 14 Z9 14 U1 5 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 162 BP 31 EP 44 DI 10.1039/c2fd20145c PG 14 WC Chemistry, Physical SC Chemistry GA 180JW UT WOS:000321591000002 PM 24015574 ER PT J AU Yim, CM Pang, CL Humphrey, DS Muryn, CA Schulte, K Perez, R Thornton, G AF Yim, Chi Ming Pang, Chi Lun Humphrey, David S. Muryn, Christopher A. Schulte, Karina Perez, Ruben Thornton, Geoff TI CO and O overlayers on Pd nanocrystals supported on TiO2(110) SO FARADAY DISCUSSIONS LA English DT Article ID DENSITY-FUNCTIONAL THEORY; TOTAL-ENERGY CALCULATIONS; WAVE BASIS-SET; SURFACE-STRUCTURES; MODEL CATALYST; PD(111); ADSORPTION; RESOLUTION; STM; SPECTROSCOPY AB We have prepared a model catalytic system by depositing Pd onto a TiO2(110) surface held at similar to 720 K. Scanning tunneling microscopy (STM) reveals well-defined Pd nanocrystals consisting of (111) top facets with {111} and {100} side facets. The Pd nanocrystals go down to about 10 nm in width and 1.3 nm in height. Top facets can be imaged with atomic resolution, indicating the absence of TiOx encapsulation. The model catalyst was probed by exposure to CO and O-2. By varying the CO exposure, different CO overlayers were formed on the (111) top facets, with coverages ranging from 0.33 to 0.75 of a monolayer. Near edge X-ray absorption fine structure (NEXAFS) measurements at 300 K reveal that at around 0.5 ML coverage, CO is oriented with the molecular axis more or less normal to TiO2(110). Dosing small amounts of O-2 separately on a Pd/TiO2(110) surface led to an overlayer of p(2 x 2)-O formed on the (111) top facet of the Pd nanocrystals at 190 K. C1 [Yim, Chi Ming; Pang, Chi Lun; Humphrey, David S.; Thornton, Geoff] UCL, Dept Chem, London WC1H 0AH, England. [Yim, Chi Ming; Pang, Chi Lun; Humphrey, David S.; Thornton, Geoff] UCL, London Ctr Nanotechnol, London WC1H 0AH, England. [Muryn, Christopher A.] Univ Manchester, Sch Chem, Manchester M13 9PL, Lancs, England. [Muryn, Christopher A.] Univ Manchester, Photon Sci Inst, Manchester M13 9PL, Lancs, England. [Schulte, Karina] Lund Univ, MAX Lab 4, S-22100 Lund, Sweden. [Perez, Ruben] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Perez, Ruben] Univ Autonoma Madrid, Dept Fis Teor Mat Condensada, Fac Ciencias, E-28049 Madrid, Spain. RP Thornton, G (reprint author), UCL, Dept Chem, 17-19 Gordon St, London WC1H 0AH, England. EM g.thornton@ucl.ac.uk RI Perez, Ruben/F-1849-2010; COST, CM1104/I-8057-2015; Pang, Chi Lun/M-1105-2016; OI Perez, Ruben/0000-0001-5896-541X; Pang, Chi Lun/0000-0002-5222-9734; Yim, Chi Ming/0000-0003-3339-4571 FU EPSRC (UK) [COST1104]; European Research Council; Spanish Project MINECO [MAT2011-023627]; Spanish Project MEC [PR2011-0402]; Fundacion CajaMadrid FX This work was supported by EPSRC (UK), COST1104 and European Research Council Advanced Grant ENERGYSURF. RP acknowledges the support of the Spanish Projects MAT2011-023627 (MINECO), PR2011-0402 (MEC) and Fundacion CajaMadrid. NR 30 TC 5 Z9 5 U1 1 U2 32 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 162 BP 191 EP 200 DI 10.1039/c2fd20137b PG 10 WC Chemistry, Physical SC Chemistry GA 180JW UT WOS:000321591000011 PM 24015584 ER PT J AU Wania, R Melton, JR Hodson, EL Poulter, B Ringeval, B Spahni, R Bohn, T Avis, CA Chen, G Eliseev, AV Hopcroft, PO Riley, WJ Subin, ZM Tian, H van Bodegom, PM Kleinen, T Yu, ZC Singarayer, JS Zurcher, S Lettenmaier, DP Beerling, DJ Denisov, SN Prigent, C Papa, F Kaplan, JO AF Wania, R. Melton, J. R. Hodson, E. L. Poulter, B. Ringeval, B. Spahni, R. Bohn, T. Avis, C. A. Chen, G. Eliseev, A. V. Hopcroft, P. O. Riley, W. J. Subin, Z. M. Tian, H. van Bodegom, P. M. Kleinen, T. Yu, Z. C. Singarayer, J. S. Zuercher, S. Lettenmaier, D. P. Beerling, D. J. Denisov, S. N. Prigent, C. Papa, F. Kaplan, J. O. TI Present state of global wetland extent and wetland methane modelling: methodology of a model inter-comparison project (WETCHIMP) SO GEOSCIENTIFIC MODEL DEVELOPMENT LA English DT Article ID INCREASED N DEPOSITION; NATURAL WETLANDS; ATMOSPHERIC CO2; TERRESTRIAL ECOSYSTEMS; BIOGEOCHEMISTRY MODEL; VEGETATION MODEL; PRIMARY PRODUCTIVITY; CLIMATE FEEDBACKS; NORTH-AMERICA; RICE PADDIES AB The Wetland and Wetland CH4 Intercomparison of Models Project (WETCHIMP) was created to evaluate our present ability to simulate large-scale wetland characteristics and corresponding methane (CH4) emissions. A multi-model comparison is essential to evaluate the key uncertainties in the mechanisms and parameters leading to methane emissions. Ten modelling groups joined WETCHIMP to run eight global and two regional models with a common experimental protocol using the same climate and atmospheric carbon dioxide (CO2) forcing datasets. We reported the main conclusions from the intercomparison effort in a companion paper (Melton et al., 2013). Here we provide technical details for the six experiments, which included an equilibrium, a transient, and an optimized run plus three sensitivity experiments (temperature, precipitation, and atmospheric CO2 concentration). The diversity of approaches used by the models is summarized through a series of conceptual figures, and is used to evaluate the wide range of wetland extent and CH4 fluxes predicted by the models in the equilibrium run. We discuss relationships among the various approaches and patterns in consistencies of these model predictions. Within this group of models, there are three broad classes of methods used to estimate wetland extent: prescribed based on wetland distribution maps, prognostic relationships between hydrological states based on satellite observations, and explicit hydrological mass balances. A larger variety of approaches was used to estimate the net CH4 fluxes from wetland systems. Even though modelling of wetland extent and CH4 emissions has progressed significantly over recent decades, large uncertainties still exist when estimating CH4 emissions: there is little consensus on model structure or complexity due to knowledge gaps, different aims of the models, and the range of temporal and spatial resolutions of the models. C1 [Wania, R.] Univ Montpellier 2, CNRS, UMR5554, Inst Sci Evolut, F-34090 Montpellier, France. [Melton, J. R.; Kaplan, J. O.] Ecole Polytech Fed Lausanne, ARVE Grp, CH-1015 Lausanne, Switzerland. [Hodson, E. L.] Swiss Fed Res Inst WSL, Zurich, Switzerland. [Poulter, B.; Ringeval, B.] UVSQ, CNRS CEA, Lab Sci Climat & Environm, Gif Sur Yvette, France. [Ringeval, B.; Hopcroft, P. O.; Singarayer, J. S.] Univ Bristol, Sch Geog Sci, BRIDGE, Bristol BS8 1TH, Avon, England. [Ringeval, B.] Vrije Univ Amsterdam, Dept Earth Sci, Amsterdam, Netherlands. [Spahni, R.; Zuercher, S.] Univ Bern, Inst Phys, CH-3012 Bern, Switzerland. [Spahni, R.; Zuercher, S.] Univ Bern, Oeschger Ctr Climate Change Res, CH-3012 Bern, Switzerland. [Bohn, T.; Lettenmaier, D. P.] Univ Washington, Dept Civil & Environm Engn, Seattle, WA 98195 USA. [Avis, C. A.] Univ Victoria, Sch Earth & Ocean Sci, Victoria, BC V8W 2Y2, Canada. [Chen, G.; Tian, H.] Auburn Univ, Int Ctr Climate & Global Change Res, Auburn, AL 36849 USA. [Chen, G.; Tian, H.] Auburn Univ, Sch Forestry & Wildlife Sci, Auburn, AL 36849 USA. [Eliseev, A. V.; Denisov, S. N.] Russian Acad Sci, AM Obukhov Inst Atmospher Phys, Moscow 117901, Russia. [Eliseev, A. V.] Kazan Volga Reg Fed Univ, Kazan, Russia. [Riley, W. J.; Subin, Z. M.] Lawrence Berkeley Natl Lab, ESD, Berkeley, CA USA. [Kleinen, T.] Max Planck Inst Meteorol, D-20146 Hamburg, Germany. [van Bodegom, P. M.] Vrije Univ Amsterdam, Dept Ecol Sci, Amsterdam, Netherlands. [Yu, Z. C.] Lehigh Univ, Dept Earth & Environm Sci, Bethlehem, PA USA. [Beerling, D. J.] Univ Sheffield, Dept Anim & Plant Sci, Sheffield S10 2TN, S Yorkshire, England. [Prigent, C.] Observ Paris, CNRS LERMA, F-75014 Paris, France. [Papa, F.] IRD, LEGOS, F-31400 Toulouse, France. RP Melton, JR (reprint author), Environm Canada, Canadian Ctr Climate Modelling & Anal, Victoria, BC V8W 2Y2, Canada. EM joe.melton.sci@gmail.com RI Eliseev, Alexey V./L-8707-2013; Tian, Hanqin/A-6484-2012; lettenmaier, dennis/F-8780-2011; Denisov, Sergey/N-2700-2013; Papa, Fabrice/D-3695-2009; Yu, Zicheng/D-4108-2012; Subin, Zachary/K-5168-2012; Bohn, Theodore/K-4494-2012; van Bodegom, Peter/N-8150-2015; Riley, William/D-3345-2015; Kaplan, Jed/P-1796-2015; Hopcroft, Peter/H-4957-2016 OI Ringeval, Bruno/0000-0001-8405-1304; Eliseev, Alexey V./0000-0001-7288-7649; Tian, Hanqin/0000-0002-1806-4091; lettenmaier, dennis/0000-0003-3317-1327; Papa, Fabrice/0000-0001-6305-6253; Subin, Zachary/0000-0002-9257-9288; Bohn, Theodore/0000-0002-1880-9129; van Bodegom, Peter/0000-0003-0771-4500; Riley, William/0000-0002-4615-2304; Kaplan, Jed/0000-0001-9919-7613; Hopcroft, Peter/0000-0003-3694-9181 FU COST Action [ES0805 TERRABITES]; Swiss Ministry for Research and Education [C09.0054]; Swiss National Science Foundation [PP0022_119049, PP00P2_139193]; Office of Science, Office of Biological and Environmental Research, Climate and Environmental Science Division, of the US Department of Energy [DE-AC02-05CH11231]; NASA's ROSES program [NNX08AH97G]; US NSF [ARC-1107981]; The Max Planck Society (Germany); Russian Foundation for Basic Research; Russian Academy of Sciences; Swiss National Science Foundation; European Research Council under European Community [226172]; NERC UK [NE/I010912/1]; NERC UK/INSU France QUEST-DESIRE project; ETH Competence Center Environment and Sustainability's grant MAIOLICA; [5467.2012.5] FX The authors are grateful to the COST Action ES0805 TERRABITES for providing support for the WETCHIMP workshop. We thank Sylvia Houston and Olga Petrikova for assistance with organizing the project meeting and Kristen Krumhardt for assistance producing the figures. J. R. M. was supported by the Swiss Ministry for Research and Education (grant C09.0054). J. O. K. acknowledges support from the Swiss National Science Foundation (grants PP0022_119049 and PP00P2_139193). The contributions of W. J. R. and Z. M. S. were supported by the Director, Office of Science, Office of Biological and Environmental Research, Climate and Environmental Science Division, of the US Department of Energy under Contract No. DE-AC02-05CH11231 to Berkeley Lab (IMPACTS and C-Climate Uncertainties projects). The contributions of T. J. B. and D. P. L. were supported by NASA's ROSES program, grant NNX08AH97G. The contribution of Z. C. Y. was supported by a US NSF grant (ARC-1107981) and a grant from The Max Planck Society (Germany). A. V. E. and S. N. D. were supported by the the President of Russia grant 5467.2012.5, by the Russian Foundation for Basic Research, and by the programs of the Russian Academy of Sciences. The contributions of R. S. and S. Z. were supported by the Swiss National Science Foundation and by the European Research Council advanced grant MATRICs (ERC grant agreement no. 226172) under the European Community's Seventh Framework Programme. P. O. H. is supported by a NERC UK grant NE/I010912/1 and previously through NERC UK/INSU France QUEST-DESIRE project. E. L. H. was supported by ETH Competence Center Environment and Sustainability's grant MAIOLICA. We also thank Steve Frolking and one anonymous reviewer for their comments which have improved our manuscript. NR 123 TC 42 Z9 43 U1 8 U2 74 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1991-959X EI 1991-9603 J9 GEOSCI MODEL DEV JI Geosci. Model Dev. PY 2013 VL 6 IS 3 BP 617 EP 641 DI 10.5194/gmd-6-617-2013 PG 25 WC Geosciences, Multidisciplinary SC Geology GA 174EU UT WOS:000321137700003 ER PT J AU Wan, H Giorgetta, MA Zangl, G Restelli, M Majewski, D Bonaventura, L Frohlich, K Reinert, D Ripodas, P Kornblueh, L Forstner, J AF Wan, H. Giorgetta, M. A. Zaengl, G. Restelli, M. Majewski, D. Bonaventura, L. Froehlich, K. Reinert, D. Ripodas, P. Kornblueh, L. Foerstner, J. TI The ICON-1.2 hydrostatic atmospheric dynamical core on triangular grids - Part 1: Formulation and performance of the baseline version SO GEOSCIENTIFIC MODEL DEVELOPMENT LA English DT Article ID SHALLOW-WATER EQUATIONS; BAROTROPIC VORTICITY EQUATION; SEMI-LAGRANGIAN ADVECTION; AQUA-PLANET SIMULATIONS; FINITE-VOLUME; NUMERICAL-INTEGRATION; GENERAL-CIRCULATION; TRANSPORT SCHEMES; STANDARD TEST; MODEL AB As part of a broader effort to develop next-generation models for numerical weather prediction and climate applications, a hydrostatic atmospheric dynamical core is developed as an intermediate step to evaluate a finite-difference discretization of the primitive equations on spherical icosahedral grids. Based on the need for mass-conserving discretizations for multi-resolution modelling as well as scalability and efficiency on massively parallel computing architectures, the dynamical core is built on triangular C-grids using relatively small discretization stencils. This paper presents the formulation and performance of the baseline version of the new dynamical core, focusing on properties of the numerical solutions in the setting of globally uniform resolution. Theoretical analysis reveals that the discrete divergence operator defined on a single triangular cell using the Gauss theorem is only first-order accurate, and introduces grid-scale noise to the discrete model. The noise can be suppressed by fourth-order hyper-diffusion of the horizontal wind field using a time-step and grid-size-dependent diffusion coefficient, at the expense of stronger damping than in the reference spectral model. A series of idealized tests of different complexity are performed. In the deterministic baroclinic wave test, solutions from the new dynamical core show the expected sensitivity to horizontal resolution, and converge to the reference solution at R2B6 (35 km grid spacing). In a dry climate test, the dynamical core correctly reproduces key features of the meridional heat and momentum transport by baroclinic eddies. In the aqua-planet simulations at 140 km resolution, the new model is able to reproduce the same equatorial wave propagation characteristics as in the reference spectral model, including the sensitivity of such characteristics to the meridional sea surface temperature profile. These results suggest that the triangular-C discretization provides a reasonable basis for further development. The main issues that need to be addressed are the grid-scale noise from the divergence operator which requires strong damping, and a phase error of the baroclinic wave at medium and low resolutions. C1 [Wan, H.; Giorgetta, M. A.; Froehlich, K.; Kornblueh, L.] Max Planck Inst Meteorol, D-20146 Hamburg, Germany. [Zaengl, G.; Majewski, D.; Froehlich, K.; Reinert, D.; Ripodas, P.; Foerstner, J.] German Weather Serv, Offenbach, Germany. [Restelli, M.; Bonaventura, L.] Politecn Milan, MOX Dept Math F Brioschi, I-20133 Milan, Italy. [Wan, H.] Int Max Planck Res Sch Earth Syst Modelling, Hamburg, Germany. RP Wan, H (reprint author), Pacific NW Natl Lab, Richland, WA 99352 USA. EM hui.wan@zmaw.de RI Wan, Hui/J-4701-2013; Bonaventura, Luca/A-8058-2010 OI Bonaventura, Luca/0000-0002-1994-0217 FU ZEIT Foundation "Ebelin and Gerd Bucerius"; Pacific Northwest National Laboratory FX The authors are indebted to Almut Gassmann (now at IAP-Kuhlungsborn), Christiane Jablonowski (University of Michigan), David Williamson (NCAR), Frank Giraldo (Naval Postgraduate School), Rupert Klein (Freie Universitat Berlin), Hans-Joachim Herzog (German Weather Service), Werner Bauer (MPI-M), and Leonidas Linardakis (MPI-M) for valuable and inspiring discussions. We also thank Almut Gassmann, Hilary Weller and the anonymous referees, whose comments and suggestions helped to improve the paper. Hui Wan was recipient of a PhD fellowship from the ZEIT Foundation "Ebelin and Gerd Bucerius" through their support to the International Max Planck Research School on Earth System Modelling in Hamburg, Germany. Preparation of this manuscript was partially supported by the Linus Pauling Distinguished Postdoctoral Fellowship of the Pacific Northwest National Laboratory, a multiprogram national laboratory operated by Battelle Memorial Institute for the US Department of Energy. The computing resources used in this work were provided by the German Climate Computing Center (Deutsches Klimarechenzentrum, DKRZ). NR 83 TC 17 Z9 18 U1 0 U2 8 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1991-959X J9 GEOSCI MODEL DEV JI Geosci. Model Dev. PY 2013 VL 6 IS 3 BP 735 EP 763 DI 10.5194/gmd-6-735-2013 PG 29 WC Geosciences, Multidisciplinary SC Geology GA 174EU UT WOS:000321137700007 ER PT J AU Wang, H Easter, RC Rasch, PJ Wang, M Liu, X Ghan, SJ Qian, Y Yoon, JH Ma, PL Vinoj, V AF Wang, H. Easter, R. C. Rasch, P. J. Wang, M. Liu, X. Ghan, S. J. Qian, Y. Yoon, J-H Ma, P-L Vinoj, V. TI Sensitivity of remote aerosol distributions to representation of cloud-aerosol interactions in a global climate model SO GEOSCIENTIFIC MODEL DEVELOPMENT LA English DT Article ID COMMUNITY ATMOSPHERE MODEL; BLACK CARBON; SEASONAL CYCLE; AIR-POLLUTION; PNNL-MMF; AEROCOM; EMISSIONS; IMPACTS; GASES; SNOW AB Many global aerosol and climate models, including the widely used Community Atmosphere Model version 5 (CAM5), have large biases in predicting aerosols in remote regions such as the upper troposphere and high latitudes. In this study, we conduct CAM5 sensitivity simulations to understand the role of key processes associated with aerosol transformation and wet removal affecting the vertical and horizontal long-range transport of aerosols to the remote regions. Improvements are made to processes that are currently not well represented in CAM5, which are guided by surface and aircraft measurements together with results from a multi-scale aerosol-climate model that explicitly represents convection and aerosol-cloud interactions at cloud-resolving scales. We pay particular attention to black carbon (BC) due to its importance in the Earth system and the availability of measurements. We introduce into CAM5 a new unified scheme for convective transport and aerosol wet removal with explicit aerosol activation above convective cloud base. This new implementation reduces the excessive BC aloft to better simulate observed BC profiles that show decreasing mixing ratios in the mid- to upper-troposphere. After implementing this new unified convective scheme, we examine wet removal of submicron aerosols that occurs primarily through cloud processes. The wet removal depends strongly on the subgrid-scale liquid cloud fraction and the rate of conversion of liquid water to precipitation. These processes lead to very strong wet removal of BC and other aerosols over mid- to high latitudes during winter months. With our improvements, the Arctic BC burden has a 10-fold (5-fold) increase in the winter (summer) months, resulting in a much-better simulation of the BC seasonal cycle as well. Arctic sulphate and other aerosol species also increase but to a lesser extent. An explicit treatment of BC aging with slower aging assumptions produces an additional 30-fold (5-fold) increase in the Arctic winter (summer) BC burden. This BC aging treatment, however, has minimal effect on other underpredicted species. Interestingly, our modifications to CAM5 that aim at improving prediction of high-latitude and upper-tropospheric aerosols also produce much-better aerosol optical depth (AOD) over various other regions globally when compared to multi-year AERONET retrievals. The improved aerosol distributions have impacts on other aspects of CAM5, improving the simulation of global mean liquid water path and cloud forcing. C1 [Wang, H.; Easter, R. C.; Rasch, P. J.; Wang, M.; Liu, X.; Ghan, S. J.; Qian, Y.; Yoon, J-H; Ma, P-L; Vinoj, V.] Pacific NW Natl Lab, Atmospher Sci & Global Change Div, Richland, WA 99352 USA. RP Wang, H (reprint author), Pacific NW Natl Lab, Atmospher Sci & Global Change Div, Richland, WA 99352 USA. EM hailong.wang@pnnl.gov RI qian, yun/E-1845-2011; Wang, Minghuai/E-5390-2011; Vinoj, V./C-3241-2008; Wang, Hailong/B-8061-2010; YOON, JIN-HO/A-1672-2009; Liu, Xiaohong/E-9304-2011; Ma, Po-Lun/G-7129-2015; Ghan, Steven/H-4301-2011 OI Wang, Minghuai/0000-0002-9179-228X; Vinoj, V./0000-0001-8573-6073; Wang, Hailong/0000-0002-1994-4402; YOON, JIN-HO/0000-0002-4939-8078; Liu, Xiaohong/0000-0002-3994-5955; Ma, Po-Lun/0000-0003-3109-5316; Ghan, Steven/0000-0001-8355-8699 FU Office of Science of the US Department of Energy (DOE) as part of the Earth System Modeling Program; DOE [DE-AC05-76RLO1830]; National Science Foundation; DOE Office of Science; NASA [NNX07AI56G]; DOE Office of Science, Decadal and Regional Climate Prediction using Earth System Models (EaSM) program FX This research was supported by the Office of Science of the US Department of Energy (DOE) as part of the Earth System Modeling Program. The Pacific Northwest National Laboratory (PNNL) is operated for DOE by Battelle Memorial Institute under contract DE-AC05-76RLO1830. The CESM project is supported by the National Science Foundation and the DOE Office of Science. The development of the PNNL-MMF was supported by the NASA Interdisciplinary Science Program under grant NNX07AI56G and the DOE Office of Science, Decadal and Regional Climate Prediction using Earth System Models (EaSM) program. We thank D. Koch for providing BC profiles and helpful discussion, J. P. Schwarz for providing the HIPPO BC profiles, and many scientists, engineers and support staff for their efforts in making all the datasets available for our model evaluation. Computational resources were provided by the National Energy Research Scientific Computing Center (NERSC), a national scientific user facility located at Lawrence Berkeley National Laboratory in Berkeley, California. NERSC is the flagship scientific computing facility for the Office of Science in DOE. NR 61 TC 44 Z9 44 U1 4 U2 35 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1991-959X EI 1991-9603 J9 GEOSCI MODEL DEV JI Geosci. Model Dev. PY 2013 VL 6 IS 3 BP 765 EP 782 DI 10.5194/gmd-6-765-2013 PG 18 WC Geosciences, Multidisciplinary SC Geology GA 174EU UT WOS:000321137700008 ER PT J AU Wan, H Rasch, PJ Zhang, K Kazil, J Leung, LR AF Wan, H. Rasch, P. J. Zhang, K. Kazil, J. Leung, L. R. TI Numerical issues associated with compensating and competing processes in climate models: an example from ECHAM-HAM SO GEOSCIENTIFIC MODEL DEVELOPMENT LA English DT Article ID COMMUNITY ATMOSPHERE MODEL; NONLINEAR VERTICAL DIFFUSION; CLOUD MICROPHYSICS SCHEME; SIZE DISTRIBUTIONS; SULFURIC-ACID; SINGLE-COLUMN; AEROSOL; SENSITIVITY; IMPLEMENTATION; REPRESENTATION AB The purpose of this paper is to draw attention to the need for appropriate numerical techniques to represent process interactions in climate models. In two versions of the ECHAM-HAM model, different time integration methods are used to solve the sulfuric acid (H2SO4) gas evolution equation, which lead to substantially different results in the H2SO4 gas concentration and the aerosol nucleation rate. Using convergence tests and sensitivity simulations performed with various time stepping schemes, it is confirmed that numerical errors in the second model version are significantly smaller than those in version one. The use of sequential operator splitting in combination with a long time step is identified as the main reason for the large systematic biases in the old model. The remaining errors of nucleation rate in version two, related to the competition between condensation and nucleation, have a clear impact on the simulated concentration of cloud condensation nuclei (CCN) in the lower troposphere. These errors can be significantly reduced by employing solvers that handle production, condensation and nucleation at the same time. Lessons learned in this work underline the need for more caution when treating multi-timescale problems involving compensating and competing processes, a common occurrence in current climate models. C1 [Wan, H.; Rasch, P. J.; Zhang, K.; Leung, L. R.] Pacific NW Natl Lab, Richland, WA 99352 USA. [Kazil, J.] Univ Colorado, CIRES, Boulder, CO 80309 USA. [Kazil, J.] NOAA, ESRL, Boulder, CO USA. RP Wan, H (reprint author), Pacific NW Natl Lab, Richland, WA 99352 USA. EM hui.wan@pnnl.gov RI Kazil, Jan/B-7652-2013; Wan, Hui/J-4701-2013; Zhang, Kai/F-8415-2010; Manager, CSD Publications/B-2789-2015 OI Kazil, Jan/0000-0003-3271-2451; Zhang, Kai/0000-0003-0457-6368; FU Pacific Northwest National Laboratory (PNNL); US Department of Energy (DOE) [DE-AC05-76RL01830]; DOE Office of Science as part of the Earth System Modeling Program (Aerosol Clouds and Precipitation Science Focus Area); Scientific Discovery Through Advanced Computing (SciDAC) project on Multiscale Methods for Accurate, Efficient, and Scale-Aware Models of the Earth System FX The authors thank Harri Kokkola (FMI), Xiaohong Liu (PNNL), Dick Easter (PNNL), Peter Caldwell (LLNL), Declan O'Donnell (FMI), Philip Stier (Oxford University) and Stefan Kinne (MPI-M) for valuable discussions. We also thank Luca Bonaventura and an anonymous reviewer, whose comments helped to improve the paper. H. Wan is grateful for the support of the Linus Pauling Distinguished Postdoctoral Fellowship of the Pacific Northwest National Laboratory (PNNL), a multiprogram laboratory operated for the US Department of Energy (DOE) by Battelle Memorial Institute under contract DE-AC05-76RL01830. The study described in this paper was conducted under the PNNL Laboratory Directed Research and Development Program. P. J. Rasch was supported by the DOE Office of Science as part of the Earth System Modeling Program (the Aerosol Clouds and Precipitation Science Focus Area), and the Scientific Discovery Through Advanced Computing (SciDAC) project on Multiscale Methods for Accurate, Efficient, and Scale-Aware Models of the Earth System. The ECHAM-HAM simulations presented in this paper were performed at the German Climate Computing Center (Deutsches Klimarechenzentrum, DKRZ). NR 54 TC 4 Z9 4 U1 0 U2 7 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1991-959X EI 1991-9603 J9 GEOSCI MODEL DEV JI Geosci. Model Dev. PY 2013 VL 6 IS 3 BP 861 EP 874 DI 10.5194/gmd-6-861-2013 PG 14 WC Geosciences, Multidisciplinary SC Geology GA 174EU UT WOS:000321137700014 ER PT J AU Zhao, C Bruck, T Lercher, JA AF Zhao, Chen Brueck, Thomas Lercher, Johannes A. TI Catalytic deoxygenation of microalgae oil to green hydrocarbons SO GREEN CHEMISTRY LA English DT Review ID WASTE COOKING OIL; SOLID ACID CATALYSTS; FREE FATTY-ACIDS; BIODIESEL PRODUCTION; VEGETABLE-OILS; STEARIC-ACID; CANOLA OIL; PALM OIL; MESOPOROUS CARBON; DIESEL FUEL AB Microalgae are high potential raw biomass material for triglyceride feedstock, due to their high oil content and rapid growth rate, and because algae cultivation does not compete with edible food on arable land. This review addresses first the microalgae cultivation with an overview of the productivity and growth of microalgae, the recovery of lipids from the microalgae, and chemical compositions of microalgae biomass and microalgal oil. Second, three basic approaches are discussed to downstream processing for the production of green gasoline and diesel hydrocarbons from microalgae oil, including cracking with zeolite, hydrotreating with supported sulfided catalysts and hydrodeoxygenation with non-sulfide metal catalysts. For the triglyceride derived bio-fuels, only "drop-in" gasoline and diesel range components are discussed in this review. C1 [Zhao, Chen; Brueck, Thomas; Lercher, Johannes A.] Tech Univ Munich, Dept Chem, D-85747 Garching, Germany. [Zhao, Chen; Lercher, Johannes A.] Tech Univ Munich, Catalysis Res Ctr, D-85747 Garching, Germany. [Lercher, Johannes A.] Pacific NW Natl Lab, Inst Integrated Catalysis, Richland, WA 99352 USA. RP Zhao, C (reprint author), Tech Univ Munich, Dept Chem, D-85747 Garching, Germany. EM chenzhao@mytum.de; johannes.lercher@ch.tum.de RI Bruck, Prof.Dr. Thomas/B-6018-2016 OI Bruck, Prof.Dr. Thomas/0000-0002-2113-6957 NR 174 TC 71 Z9 73 U1 19 U2 200 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9262 J9 GREEN CHEM JI Green Chem. PY 2013 VL 15 IS 7 BP 1720 EP 1739 DI 10.1039/c3gc40558c PG 20 WC Chemistry, Multidisciplinary; GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY SC Chemistry; Science & Technology - Other Topics GA 169LH UT WOS:000320781200002 ER PT J AU Wall, AJ Capo, RC Stewart, BW Phan, TT Jain, JC Hakala, JA Guthrie, GD AF Wall, Andrew J. Capo, Rosemary C. Stewart, Brian W. Phan, Thai T. Jain, Jinesh C. Hakala, J. Alexandra Guthrie, George D. TI High throughput method for Sr extraction from variable matrix waters and Sr-87/Sr-86 isotope analysis by MC-ICP-MS SO JOURNAL OF ANALYTICAL ATOMIC SPECTROMETRY LA English DT Article ID UTILIZATION BY-PRODUCTS; ACID-MINE DRAINAGE; STRONTIUM-ISOTOPE; CHROMATOGRAPHIC RESIN; PRECISE DETERMINATION; MASS-SPECTROMETRY; COAL-MINE; SEPARATION; RATIOS; USA AB Natural isotope tracers, such as strontium (Sr), can facilitate the tracking of brine migration caused by CO2 injection in carbon storage sites and assist in identifying the origin of formation waters associated with oil and gas exploration. However, it might be necessary to analyze tens of samples with complex chemical compositions over a short period to identify subsurface reactions and respond to unexpected fluid movement in the host formation. These conditions require streamlined Sr separation chemistry for samples ranging from pristine groundwaters to those containing high total dissolved solids, followed by rapid measurement of isotope ratios with high analytical precision. Here we describe a method useful for the separation of Sr from energy related geofluids and the rapid measurements of Sr isotopic ratios by MC-ICP-MS. Existing vacuum-assisted Sr separation procedures were modified by using inexpensive disposable parts that also eliminate cross contamination. These improvements will allow an operator to independently prepare samples for Sr isotope analysis using fast, low cost separation procedures and commercially available components. We optimized the elution chemistry by adjusting acid normality and elution rates to provide better separation of Sr from problematic matrices (e. g. Rb, Ca, Ba, K) associated with oilfield brines and formation waters. The separation procedure is designed for high sample throughputs that are ready for immediate Sr isotope measurements by MC-ICP-MS. Precise Sr isotope results can be achieved by MC-ICP-MS with a throughput of 4 to 5 samples per hour. Fluids from a range of geologic environments analyzed by this method yielded results within the analytical uncertainty of Sr-87/Sr-86 ratios previously determined by standard column separation and TIMS. This method provides a fast and effective way to use isolate Sr in a variety of geologic fluids for isotopic analysis by MC-ICP-MS. C1 [Wall, Andrew J.; Hakala, J. Alexandra; Guthrie, George D.] US DOE, Natl Energy Technol Lab, Pittsburgh, PA 15236 USA. [Capo, Rosemary C.; Stewart, Brian W.; Phan, Thai T.] Univ Pittsburgh, Natl Energy Technol Lab, Reg Univ Alliance, Pittsburgh, PA 15260 USA. [Capo, Rosemary C.; Stewart, Brian W.; Phan, Thai T.] Univ Pittsburgh, Dept Geol & Planetary Sci, Pittsburgh, PA 15260 USA. [Jain, Jinesh C.] Natl Energy Technol Lab, URS Washington Div, Pittsburgh, PA 15236 USA. RP Wall, AJ (reprint author), US DOE, Natl Energy Technol Lab, Pittsburgh, PA 15236 USA. EM Andrew.Wall@CONTR.NETL.DOE.GOV OI Phan, Thai/0000-0003-2491-749X FU U.S. Department of Energy, Office of Fossil Energy, under the Office of Oil and Natural Gas; Office of Clean Coal (Geologic Carbon Storage); National Energy Technology Laboratory's ongoing research under the RES [DE-FE0004000]; agency of the United States Government FX This work was supported by the U.S. Department of Energy, Office of Fossil Energy, under the Office of Oil and Natural Gas (Energy Policy Act of 2005, Section 999 Complementary Program Research) and the Office of Clean Coal (Geologic Carbon Storage), as performed through the Oak Ridge Institute for Science and Education at the National Energy Technology Laboratory (AW) and the National Energy Technology Laboratory's ongoing research under the RES contract DE-FE0004000 (RCC and BWS). The authors would like to thank Dan Bain for assistance with ICP-MS analysis, and three anonymous reviewers for detailed comments which improved the manuscript. Disclaimer: 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 36 TC 7 Z9 7 U1 2 U2 31 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 0267-9477 J9 J ANAL ATOM SPECTROM JI J. Anal. At. Spectrom. PY 2013 VL 28 IS 8 BP 1338 EP 1344 DI 10.1039/c3ja30350k PG 7 WC Chemistry, Analytical; Spectroscopy SC Chemistry; Spectroscopy GA 181NO UT WOS:000321674600020 ER PT J AU Abdallah, J Adragna, P Alexa, C Alves, R Amaral, P Ananiev, A Anderson, K Andresen, X Antonaki, A Batusov, V Bednar, P Bergeaas, E Biscarat, C Blanch, O Blanchot, G Bohm, C Boldea, V Bosi, F Bosman, M Bromberg, C Budagov, J Calvet, D Cardeira, C Carli, T Carvalho, J Cascella, M Castillo, MV Costelo, J Cavalli-Sforza, M Cavasinni, V Cerqueira, AS Clement, C Cobal, M Cogswell, F Constantinescu, S Costanzo, D Da Silva, P David, M Davidek, T Dawson, J De, K Del Prete, T Diakov, E Di Girolamo, B Dita, S Dolejsi, J Dolezal, Z Dotti, A Downing, R Drake, G Efthymiopoulos, I Errede, D Errede, S Farbin, A Fassouliotis, D Feng, E Fenyuk, A Ferdi, C Ferreira, BC Ferrer, A Flaminio, V Flix, J Francavilla, P Fullana, E Garde, V Gellerstedt, K Giakoumopoulou, V Giangiobbe, V Gildemeister, O Gilewsky, V Giokaris, N Gollub, N Gomes, A Gonzalez, V Gouveia, J Grenier, P Gris, P Guarino, V Guicheney, C Gupta, A Hakobyan, H Haney, M Hellman, S Henriques, A Higon, E Hill, N Holmgren, S Hruska, I Hurwitz, M Huston, J Plante, IJL Jon-And, K Junk, T Karyukhin, A Khubua, J Klereborn, J Konstantinov, V Kopikov, S Korolkov, I Krivkova, P Kulchitsky, Y Kurochkin, Y Kuzhir, P Lapin, V LeCompte, T Lefevre, R Leitner, R Li, J Liablin, M Lokajicek, M Lomakin, Y Lourtie, P Lovas, L Lupi, A Maidantchik, C Maio, A Maliukov, S Manousakis, A Marques, C Marroquim, F Martin, F Mazzoni, E Merritt, F Miagkov, A Miller, R Minashvili, I Miralles, L Montarou, G Nemecek, S Nessi, M Nikitine, I Nodulman, L Norniella, O Onofre, A Oreglia, M Palan, B Pallin, D Pantea, D Pereira, A Pilcher, J Pina, J Pinhao, J Pod, E Podlyski, F Portell, X Poveda, J Pribyl, L Price, E Proudfoot, J Ramalho, M Ramstedt, M Raposeiro, L Reis, J Richards, R Roda, C Romanov, V Rosnet, P Roy, P Ruiz, A Rumiantsau, V Russakovich, N Da Costa, JS Salto, O Salvachua, B Sanchis, E Sanders, H Santoni, C Santos, J Saraiva, JG Sarri, F Says, LP Schlager, G Schlereth, J Seixas, JM Sellden, B Shalanda, N Shevtsov, P Shochet, M Silva, J Simaitis, V Simonyan, M Sissakian, A Sjoelin, J Solans, C Solodkov, A Solovianov, O Sosebee, M Spano, F Speckmeyer, P Stanek, R Starchenko, E Starovoitov, P Suk, M Sykora, I Tang, F Tas, P Teuscher, R Tischenko, M Tokar, S Topilin, N Torres, J Underwood, D Usai, G Valero, A Valkar, S Valls, JA Vartapetian, A Vazeille, F Vellidis, C Ventura, F Vichou, I Vivarelli, I Volpi, M White, A Zaitsev, A Zaytsev, Y Zenin, A Zenis, T Zenonos, Z Zenz, S Zilka, B AF Abdallah, J. Adragna, P. Alexa, C. Alves, R. Amaral, P. Ananiev, A. Anderson, K. Andresen, X. Antonaki, A. Batusov, V. Bednar, P. Bergeaas, E. Biscarat, C. Blanch, O. Blanchot, G. Bohm, C. Boldea, V. Bosi, F. Bosman, M. Bromberg, C. Budagov, J. Calvet, D. Cardeira, C. Carli, T. Carvalho, J. Cascella, M. Castillo, M. V. Costelo, J. Cavalli-Sforza, M. Cavasinni, V. Cerqueira, A. S. Clement, C. Cobal, M. Cogswell, F. Constantinescu, S. Costanzo, D. Da Silva, P. David, M. Davidek, T. Dawson, J. De, K. Del Prete, T. Diakov, E. Di Girolamo, B. Dita, S. Dolejsi, J. Dolezal, Z. Dotti, A. Downing, R. Drake, G. Efthymiopoulos, I. Errede, D. Errede, S. Farbin, A. Fassouliotis, D. Feng, E. Fenyuk, A. Ferdi, C. Ferreira, B. C. Ferrer, A. Flaminio, V. Flix, J. Francavilla, P. Fullana, E. Garde, V. Gellerstedt, K. Giakoumopoulou, V. Giangiobbe, V. Gildemeister, O. Gilewsky, V. Giokaris, N. Gollub, N. Gomes, A. Gonzalez, V. Gouveia, J. Grenier, P. Gris, P. Guarino, V. Guicheney, C. Gupta, A. Hakobyan, H. Haney, M. Hellman, S. Henriques, A. Higon, E. Hill, N. Holmgren, S. Hruska, I. Hurwitz, M. Huston, J. Plante, I. Jen-La Jon-And, K. Junk, T. Karyukhin, A. Khubua, J. Klereborn, J. Konstantinov, V. Kopikov, S. Korolkov, I. Krivkova, P. Kulchitsky, Y. Kurochkin, Yu Kuzhir, P. Lapin, V. LeCompte, T. Lefevre, R. Leitner, R. Li, J. Liablin, M. Lokajicek, M. Lomakin, Y. Lourtie, P. Lovas, L. Lupi, A. Maidantchik, C. Maio, A. Maliukov, S. Manousakis, A. Marques, C. Marroquim, F. Martin, F. Mazzoni, E. Merritt, F. Miagkov, A. Miller, R. Minashvili, I. Miralles, L. Montarou, G. Nemecek, S. Nessi, M. Nikitine, I. Nodulman, L. Norniella, O. Onofre, A. Oreglia, M. Palan, B. Pallin, D. Pantea, D. Pereira, A. Pilcher, J. Pina, J. Pinhao, J. Pod, E. Podlyski, F. Portell, X. Poveda, J. Pribyl, L. Price, E. Proudfoot, J. Ramalho, M. Ramstedt, M. Raposeiro, L. Reis, J. Richards, R. Roda, C. Romanov, V. Rosnet, P. Roy, P. Ruiz, A. Rumiantsau, V. Russakovich, N. Da Costa, J. Sa Salto, O. Salvachua, B. Sanchis, E. Sanders, H. Santoni, C. Santos, J. Saraiva, J. G. Sarri, F. Says, L. -P. Schlager, G. Schlereth, J. Seixas, J. M. Sellden, B. Shalanda, N. Shevtsov, P. Shochet, M. Silva, J. Simaitis, V. Simonyan, M. Sissakian, A. Sjoelin, J. Solans, C. Solodkov, A. Solovianov, O. Sosebee, M. Spano, F. Speckmeyer, P. Stanek, R. Starchenko, E. Starovoitov, P. Suk, M. Sykora, I. Tang, F. Tas, P. Teuscher, R. Tischenko, M. Tokar, S. Topilin, N. Torres, J. Underwood, D. Usai, G. Valero, A. Valkar, S. Valls, J. A. Vartapetian, A. Vazeille, F. Vellidis, C. Ventura, F. Vichou, I. Vivarelli, I. Volpi, M. White, A. Zaitsev, A. Zaytsev, Yu Zenin, A. Zenis, T. Zenonos, Z. Zenz, S. Zilka, B. CA ATLAS Tile Calorimeter Community TI The optical instrumentation of the ATLAS Tile Calorimeter SO JOURNAL OF INSTRUMENTATION LA English DT Article DE Calorimeters; Calorimeter methods; Scintillators, scintillation and light emission processes (solid, gas and liquid scintillators) ID HADRON CALORIMETER AB The Tile Calorimeter, covering the central region of the ATLAS experiment up to pseudorapidities of +/-1.7, is a sampling device built with scintillating tiles that alternate with iron plates. The light is collected in wave-length shifting (WLS) fibers and is read out with photomultipliers. In the characteristic geometry of this calorimeter the tiles lie in planes perpendicular to the beams, resulting in a very simple and modular mechanical and optical layout. This paper focuses on the procedures applied in the optical instrumentation of the calorimeter, which involved the assembly of about 460,000 scintillator tiles and 550,000 WLS fibers. The outcome is a hadronic calorimeter that meets the ATLAS performance requirements, as shown in this paper. C1 [Dawson, J.; Drake, G.; Guarino, V.; Hill, N.; LeCompte, T.; Nodulman, L.; Price, E.; Proudfoot, J.; Schlereth, J.; Stanek, R.; Underwood, D.] Argonne Natl Lab, Argonne, IL 60439 USA. [De, K.; Li, J.; Sosebee, M.; Vartapetian, A.; White, A.] Univ Texas Arlington, Arlington, TX 76019 USA. [Antonaki, A.; Fassouliotis, D.; Giakoumopoulou, V.; Giokaris, N.; Manousakis, A.; Vellidis, C.] Univ Athens, Athens, Greece. [Blanch, O.; Blanchot, G.; Bosman, M.; Cavalli-Sforza, M.; Flix, J.; Korolkov, I.; Miralles, L.; Norniella, O.; Portell, X.; Salto, O.; Volpi, M.] Univ Autonoma Barcelona, Inst Fis Altes Energies, E-08193 Barcelona, Spain. [Bednar, P.; Lovas, L.; Sykora, I.; Tokar, S.; Zenis, T.; Zilka, B.] Comenius Univ, Bratislava, Slovakia. [Alexa, C.; Boldea, V.; Constantinescu, S.; Dita, S.; Pantea, D.] Nat Inst Phys & Nucl Engn, Bucharest, Romania. [Anderson, K.; Farbin, A.; Feng, E.; Gupta, A.; Hurwitz, M.; Plante, I. Jen-La; Merritt, F.; Oreglia, M.; Pilcher, J.; Pod, E.; Sanders, H.; Shochet, M.; Tang, F.; Teuscher, R.; Zenz, S.] Univ Chicago, Chicago, IL 60637 USA. [Biscarat, C.; Calvet, D.; Ferdi, C.; Garde, V.; Gris, P.; Guicheney, C.; Lefevre, R.; Martin, F.; Montarou, G.; Pallin, D.; Podlyski, F.; Rosnet, P.; Roy, P.; Santoni, C.; Says, L. -P.; Vazeille, F.] Univ Clermont Ferrand, CNRS IN2P3, LPC Clermont Ferrand, Clermont Ferrand, France. [Batusov, V.; Budagov, J.; Khubua, J.; Kulchitsky, Y.; Liablin, M.; Lomakin, Y.; Maliukov, S.; Minashvili, I.; Romanov, V.; Russakovich, N.; Sissakian, A.; Topilin, N.] Joint Inst Nucl Res Dubna, Dubna, Russia. [Bromberg, C.; Huston, J.; Miller, R.; Richards, R.] Michigan State Univ, E Lansing, MI 48824 USA. [Amaral, P.; Andresen, X.; Carli, T.; Clement, C.; Cobal, M.; Davidek, T.; Di Girolamo, B.; Efthymiopoulos, I.; Farbin, A.; Gildemeister, O.; Gollub, N.; Grenier, P.; Henriques, A.; Martin, F.; Nessi, M.; Schlager, G.; Spano, F.; Speckmeyer, P.] CERN, Geneva, Switzerland. [Amaral, P.; Andresen, X.; David, M.; Gomes, A.; Maio, A.; Marques, C.; Pina, J.; Santos, J.; Saraiva, J. G.; Silva, J.] LIP & FCUL Univ Lisbon, Lisbon, Portugal. [Alves, R.; Carvalho, J.; Pereira, A.; Pinhao, J.] LIP & FCTUC Univ Coimbra, Coimbra, Portugal. [Onofre, A.] LIP & Univ Catolica Figueira Foz, Foz, Portugal. [Gilewsky, V.; Kulchitsky, Y.; Kurochkin, Yu] Natl Acad Sci, Inst Phys, Minsk, Byelarus. [Kuzhir, P.; Rumiantsau, V.; Shevtsov, P.; Starovoitov, P.] Nat Ctr Particles & High Energy Phys, Minsk, Byelarus. [Adragna, P.; Bosi, F.; Cascella, M.; Cavasinni, V.; Costanzo, D.; Del Prete, T.; Dotti, A.; Flaminio, V.; Francavilla, P.; Giangiobbe, V.; Lupi, A.; Mazzoni, E.; Roda, C.; Sarri, F.; Spano, F.; Usai, G.; Vivarelli, I.; Zenonos, Z.] Univ Pisa, Pisa, Italy. [Adragna, P.; Bosi, F.; Cascella, M.; Cavasinni, V.; Costanzo, D.; Del Prete, T.; Dotti, A.; Flaminio, V.; Francavilla, P.; Giangiobbe, V.; Lupi, A.; Mazzoni, E.; Roda, C.; Sarri, F.; Spano, F.; Usai, G.; Vivarelli, I.; Zenonos, Z.] Ist Nazl Fis Nucl, Pisa, Italy. [Davidek, T.; Dolejsi, J.; Dolezal, Z.; Krivkova, P.; Leitner, R.; Suk, M.; Tas, P.; Valkar, S.] Charles Univ Prague, Prague, Czech Republic. [Hruska, I.; Lokajicek, M.; Nemecek, S.; Palan, B.; Pribyl, L.] Acad Sci Czech Republic, Inst Phys, Prague, Czech Republic. [Fenyuk, A.; Karyukhin, A.; Konstantinov, V.; Kopikov, S.; Lapin, V.; Miagkov, A.; Nikitine, I.; Shalanda, N.; Solodkov, A.; Solovianov, O.; Starchenko, E.; Zaitsev, A.; Zenin, A.] Inst High Energy Phys, Protvino, Russia. [Cerqueira, A. S.; Da Silva, P.; Ferreira, B. C.; Maidantchik, C.; Marroquim, F.; Seixas, J. M.] COPPE EE UFRJ, Rio De Janeiro, Brazil. [Bergeaas, E.; Bohm, C.; Clement, C.; Gellerstedt, K.; Hellman, S.; Holmgren, S.; Jon-And, K.; Klereborn, J.; Ramstedt, M.; Sellden, B.; Sjoelin, J.] Stockholm Univ, S-10691 Stockholm, Sweden. [Khubua, J.] Tbilisi State Univ, HEPI, GE-380086 Tbilisi, Rep of Georgia. [Cogswell, F.; Downing, R.; Errede, D.; Errede, S.; Haney, M.; Junk, T.; Simaitis, V.; Vichou, I.] Univ Illinois, Urbana, IL 61801 USA. [Abdallah, J.; Castillo, M. V.; Costelo, J.; Ferrer, A.; Fullana, E.; Gonzalez, V.; Higon, E.; Poveda, J.; Ruiz, A.; Salvachua, B.; Sanchis, E.; Solans, C.; Torres, J.; Valero, A.; Valls, J. A.] Univ Valencia, Ctr Mixto, CSIC, IFIC, E-46100 Burjassot, Valencia, Spain. [Hakobyan, H.; Simonyan, M.] Yerevan Phys Inst, Yerevan 375036, Armenia. [Diakov, E.; Tischenko, M.; Zaytsev, Yu] SIA Luch, Podolsk, Russia. [Ananiev, A.; Cardeira, C.; Gouveia, J.; Lourtie, P.; Ramalho, M.; Raposeiro, L.; Reis, J.; Da Costa, J. Sa; Ventura, F.] LIP & IDMEC IST, Lisbon, Portugal. RP Davidek, T (reprint author), Charles Univ Prague, Prague, Czech Republic. EM Tomas.Davidek@cern.ch RI Gonzalez Millan, Vicente/J-3023-2012; Solodkov, Alexander/B-8623-2017; Zaitsev, Alexandre/B-8989-2017; Cardeira, Carlos/K-9502-2013; Sanchis Peris, Enrique/J-7348-2016; Karyukhin, Andrey/J-3904-2014; Ananiev, Anani/D-9383-2015; Kuzhir, Polina/H-8653-2012; De, Kaushik/N-1953-2013; Ferrer, Antonio/H-2942-2015; Carvalho, Joao/M-4060-2013; Flix, Josep/G-5414-2012; Sa da Costa, Jose/N-6961-2013; Nemecek, Stanislav/G-5931-2014; Lokajicek, Milos/G-7800-2014; Bosman, Martine/J-9917-2014; Torres, Jose/H-3231-2015; Cavalli-Sforza, Matteo/H-7102-2015; Cascella, Michele/B-6156-2013; OI Gonzalez Millan, Vicente/0000-0001-6014-2586; Solodkov, Alexander/0000-0002-2737-8674; Zaitsev, Alexandre/0000-0002-4961-8368; Cardeira, Carlos/0000-0002-7966-4648; Sanchis Peris, Enrique/0000-0002-9689-9131; Maio, Amelia/0000-0001-9099-0009; Karyukhin, Andrey/0000-0001-9087-4315; Gomes, Agostinho/0000-0002-5940-9893; Reis, Joao/0000-0002-7586-6269; Ananiev, Anani/0000-0002-5925-1379; Kuzhir, Polina/0000-0003-3689-0837; De, Kaushik/0000-0002-5647-4489; Ferrer, Antonio/0000-0003-0532-711X; Carvalho, Joao/0000-0002-3015-7821; Flix, Josep/0000-0003-2688-8047; Sa da Costa, Jose/0000-0001-9773-9896; Bosman, Martine/0000-0002-7290-643X; Torres, Jose/0000-0002-1525-1828; Cascella, Michele/0000-0003-2091-2501; Mendes Saraiva, Joao Gentil/0000-0002-7006-0864; Pina, Joao /0000-0001-8959-5044 FU Ministry of Economical Development and Trade, Armenia; State Committee on Science & Technologies of the Republic of Belarus; CNPq, Brazil; FINEP, Brazil; CERN; Ministry of Education, Youth and Sports of the Czech Republic; Ministry of Industry and Trade of the Czech Republic; Committee for Collaboration of the Czech Republic; IN2P3, France; Georgian Academy of Sciences; GSRT, Greece; NKUA/SARG, Greece; INFN, Italy; GRICES, Portugal; FCT, Portugal; Ministry of Education and Research, Romania; Ministry of Education and Science of the Russian Federation; Russian Federal Agency of Science and Innovations; Russian Federal Agency of Atomic Energy; JINR; Ministry Department of International Science and Technology Cooperation; Ministry of Education of the Slovak Republic; Ministerio de Educacion y Ciencia (MEC), Spain; Swedish Research Council, Sweden; Knut and Alice Wallenberg Foundation, Sweden; DOE, United States of America; NSF, United States of America FX We acknowledge the support of The Ministry of Economical Development and Trade, Armenia; State Committee on Science & Technologies of the Republic of Belarus; CNPq and FINEP, Brazil; CERN; Ministry of Education, Youth and Sports of the Czech Republic, Ministry of Industry and Trade of the Czech Republic, and Committee for Collaboration of the Czech Republic with CERN; IN2P3, France; Georgian Academy of Sciences; GSRT and NKUA/SARG, Greece; INFN, Italy; GRICES and FCT, Portugal; Ministry of Education and Research, Romania; Ministry of Education and Science of the Russian Federation, Russian Federal Agency of Science and Innovations, and Russian Federal Agency of Atomic Energy; JINR; Ministry Department of International Science and Technology Cooperation, Ministry of Education of the Slovak Republic; Ministerio de Educacion y Ciencia (MEC), Spain; The Swedish Research Council, The Knut and Alice Wallenberg Foundation, Sweden; DOE and NSF, United States of America. NR 15 TC 0 Z9 0 U1 1 U2 20 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 1748-0221 J9 J INSTRUM JI J. Instrum. PD JAN PY 2013 VL 8 AR P01005 DI 10.1088/1748-0221/8/01/P01005 PG 21 WC Instruments & Instrumentation SC Instruments & Instrumentation GA 167WF UT WOS:000320665400062 ER PT J AU Alvarez, V Bandac, I Bettini, A Borges, FIGM Carcel, S Castel, J Cebrian, S Cervera, A Conde, CAN Dafni, T Dias, THVT Diaz, J Egorov, M Esteve, R Evtoukhovitch, P Fernandes, LMP Ferrario, P Ferreira, AL Freitas, EDC Gehman, VM Gil, A Goldschmidt, A Gomez, H Gomez-Cadenas, JJ Gonzalez-Diaz, D Gutierrez, RM Hauptman, J Morata, JAH Herrera, DC Iguaz, FJ Irastorza, IG Jinete, MA Labarga, L Laing, A Liubarsky, I Lopes, JAM Lorca, D Losada, M Luzon, G Mari, A Martin-Albo, J Martinez, A Miller, T Moiseenko, A Monrabal, F Monteiro, CMB Mora, FJ Moutinho, LM Vidal, JM da Luz, HN Navarro, G Nebot-Guinot, M Nygren, D Oliveira, CAB de Solorzano, AO Palma, R Perez, J Aparicio, JLP Renner, J Ripoll, L Rodriguez, A Rodriguez, J Santos, FP dos Santos, JMF Segui, L Serra, L Shuman, D Simon, A Sofka, C Sorel, M Toledo, JF Tomas, A Torrent, J Tsamalaidze, Z Vazquez, D Veloso, JFCA Villar, JA Webb, RC White, JT Yahlali, N AF Alvarez, V. Bandac, I. Bettini, A. Borges, F. I. G. M. Carcel, S. Castel, J. Cebrian, S. Cervera, A. Conde, C. A. N. Dafni, T. Dias, T. H. V. T. Diaz, J. Egorov, M. Esteve, R. Evtoukhovitch, P. Fernandes, L. M. P. Ferrario, P. Ferreira, A. L. Freitas, E. D. C. Gehman, V. M. Gil, A. Goldschmidt, A. Gomez, H. Gomez-Cadenas, J. J. Gonzalez-Diaz, D. Gutierrez, R. M. Hauptman, J. Hernando Morata, J. A. Herrera, D. C. Iguaz, F. J. Irastorza, I. G. Jinete, M. A. Labarga, L. Laing, A. Liubarsky, I. Lopes, J. A. M. Lorca, D. Losada, M. Luzon, G. Mari, A. Martin-Albo, J. Martinez, A. Miller, T. Moiseenko, A. Monrabal, F. Monteiro, C. M. B. Mora, F. J. Moutinho, L. M. Munoz Vidal, J. da Luz, H. Natal Navarro, G. Nebot-Guinot, M. Nygren, D. Oliveira, C. A. B. Ortiz de Solorzano, A. Palma, R. Perez, J. Perez Aparicio, J. L. Renner, J. Ripoll, L. Rodriguez, A. Rodriguez, J. Santos, F. P. dos Santos, J. M. F. Segui, L. Serra, L. Shuman, D. Simon, A. Sofka, C. Sorel, M. Toledo, J. F. Tomas, A. Torrent, J. Tsamalaidze, Z. Vazquez, D. Veloso, J. F. C. A. Villar, J. A. Webb, R. C. White, J. T. Yahlali, N. TI Radiopurity control in the NEXT-100 double beta decay experiment: procedures and initial measurements SO JOURNAL OF INSTRUMENTATION LA English DT Article DE Radiation calculations; Time projection Chambers (TPC); Gamma detectors (scintillators, CZT, HPG, HgI etc) ID LOW RADIOACTIVITY LEVELS; SEARCH; SPECTROMETRY; SELECTION; GERDA; MASS AB The "Neutrino Experiment with a Xenon Time-Projection Chamber" (NEXT) is intended to investigate the neutrinoless double beta decay of Xe-136, which requires a severe suppression of potential backgrounds. An extensive screening and material selection process is underway for NEXT since the control of the radiopurity levels of the materials to be used in the experimental set-up is a must for rare event searches. First measurements based on Glow Discharge Mass Spectrometry and gamma-ray spectroscopy using ultra-low background germanium detectors at the Laboratorio Subterraneo de Canfranc (Spain) are described here. Activity results for natural radioactive chains and other common radionuclides are summarized, being the values obtained for some materials like copper and stainless steel very competitive. The implications of these results for the NEXT experiment are also discussed. C1 [Alvarez, V.; Carcel, S.; Cervera, A.; Diaz, J.; Ferrario, P.; Gil, A.; Gomez-Cadenas, J. J.; Laing, A.; Liubarsky, I.; Lorca, D.; Martin-Albo, J.; Martinez, A.; Monrabal, F.; Munoz Vidal, J.; Nebot-Guinot, M.; Rodriguez, J.; Serra, L.; Simon, A.; Sorel, M.; Yahlali, N.] CSIC, Inst Fis Corpuscular IFIC, Valencia 46980, Spain. [Alvarez, V.; Carcel, S.; Cervera, A.; Diaz, J.; Ferrario, P.; Gil, A.; Gomez-Cadenas, J. J.; Laing, A.; Liubarsky, I.; Lorca, D.; Martin-Albo, J.; Martinez, A.; Monrabal, F.; Munoz Vidal, J.; Nebot-Guinot, M.; Rodriguez, J.; Serra, L.; Simon, A.; Sorel, M.; Yahlali, N.] Univ Valencia, Valencia 46980, Spain. [Bandac, I.; Bettini, A.; Castel, J.; Cebrian, S.; Dafni, T.; Gomez, H.; Gonzalez-Diaz, D.; Herrera, D. C.; Iguaz, F. J.; Irastorza, I. G.; Luzon, G.; Ortiz de Solorzano, A.; Rodriguez, A.; Segui, L.; Tomas, A.; Villar, J. A.] Lab Subterraneo Canfranc, Canfranc Estn 22880, Huesca, Spain. [Bettini, A.] Univ Padua, Dipartimento Fis, I-35131 Padua, Italy. [Bettini, A.] INFN Sect, I-35131 Padua, Italy. [Borges, F. I. G. M.; Conde, C. A. N.; Dias, T. H. V. T.; Fernandes, L. M. P.; Freitas, E. D. C.; Lopes, J. A. M.; Monteiro, C. M. B.; da Luz, H. Natal; Santos, F. P.; dos Santos, J. M. F.] Univ Coimbra, Dept Fis, P-3004516 Coimbra, Portugal. [Castel, J.; Cebrian, S.; Dafni, T.; Gomez, H.; Gonzalez-Diaz, D.; Herrera, D. C.; Iguaz, F. J.; Irastorza, I. G.; Luzon, G.; Ortiz de Solorzano, A.; Rodriguez, A.; Segui, L.; Tomas, A.; Villar, J. A.] Univ Zaragoza, Lab Fis Nucl & Astroparticulas, E-50009 Zaragoza, Spain. [Egorov, M.; Gehman, V. M.; Goldschmidt, A.; Miller, T.; Nygren, D.; Oliveira, C. A. B.; Renner, J.; Shuman, D.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Esteve, R.; Mari, A.; Mora, F. J.; Toledo, J. F.] Univ Politecn Valencia, Inst Instrumentac Imagen Mol I3M, Valencia 46022, Spain. [Evtoukhovitch, P.; Moiseenko, A.; Tsamalaidze, Z.] Joint Inst Nucl Res, Dubna 141980, Russia. [Ferreira, A. L.; Moutinho, L. M.; Veloso, J. F. C. A.] Univ Aveiro, Inst Nanostruct Nanomodelling & Nanofabricat I3N, P-3810193 Aveiro, Portugal. [Gutierrez, R. M.; Jinete, M. A.; Losada, M.; Navarro, G.] Univ Antonio Narino, Ctr Invest Ciencias Basicas & Aplicadas, Bogota, Colombia. [Hauptman, J.] Iowa State Univ, Dept Phys & Astron, Ames, IA 50011 USA. [Hernando Morata, J. A.; Vazquez, D.] Univ Santiago de Compostela, Inst Gallego Fis Altas Energias, Santiago De Compostela 15782, Spain. [Labarga, L.] Univ Autonoma Madrid, Dept Fis Teor, E-28049 Madrid, Spain. [Palma, R.; Perez Aparicio, J. L.] Univ Politecn Valencia, Dept Mecan Medios Continuos & Teor Estruct, E-46071 Valencia, Spain. [Perez, J.] UAM CSIC, Inst Fis Teor, Madrid 28049, Spain. [Ripoll, L.; Torrent, J.] Univ Girona, Escola Politecn Super, Girona 17071, Spain. [Sofka, C.; Webb, R. C.; White, J. T.] Texas A&M Univ, Dept Phys & Astron, College Stn, TX 77843 USA. RP Cebrian, S (reprint author), Lab Subterraneo Canfranc, Paseo Ayerbe S-N, Canfranc Estn 22880, Huesca, Spain. EM gomez@mail.cern.ch RI veloso, joao/J-4478-2013; Irastorza, Igor/B-2085-2012; Gomez Cadenas, Juan Jose/L-2003-2014; Moutinho, Luis/J-6021-2013; Diaz, Jose/B-3454-2012; Dafni, Theopisti /J-9646-2012; AMADE Research Group, AMADE/B-6537-2014; Balanzat, Josep Costa/C-1017-2014; matias-lopes, jose/H-6074-2012; Villar, Jose Angel/K-6630-2014; Gonzalez Diaz, Diego/K-7265-2014; Hernando Morata, Jose Angel/L-7642-2014; Gil Ortiz, Alejandro/M-1671-2014; YAHLALI, NADIA/L-1880-2014; Monrabal, Francesc/A-5880-2015; Ripoll, Lluis/A-8413-2015; dos Santos, Joaquim/B-3058-2015; Perez-Aparicio, Jose/H-7053-2015; Natal da Luz, Hugo/F-6460-2013; Fernandes, Luis/E-2372-2011; Iguaz Gutierrez, Francisco Jose/F-4117-2016 OI Irastorza, Igor/0000-0003-1163-1687; Gomez Cadenas, Juan Jose/0000-0002-8224-7714; Moutinho, Luis/0000-0001-9074-4449; Diaz, Jose/0000-0002-7239-223X; Dafni, Theopisti /0000-0002-8921-910X; AMADE Research Group, AMADE/0000-0002-5778-3291; matias-lopes, jose/0000-0002-6366-2963; Villar, Jose Angel/0000-0003-0228-7589; Gonzalez Diaz, Diego/0000-0002-6809-5996; Sorel, Michel/0000-0003-2141-9508; Toledo Alarcon, Jose Francisco/0000-0002-9782-4510; Freitas, Elisabete/0000-0001-8235-3229; Santos, Filomena/0000-0002-0214-4185; Martin-Albo, Justo/0000-0002-7318-1469; Veloso, Joao/0000-0002-7107-7203; Munoz Vidal, Javier/0000-0002-9649-2251; Dias, Teresa/0000-0001-5101-4902; Borges Soares, Filipa/0000-0001-5790-173X; Ferreira, Antonio /0000-0002-8696-3590; dos Santos, Joaquim Marques Ferreira/0000-0002-8841-6523; Conde, Carlos/0000-0002-1387-2161; Monteiro, Cristina Maria Bernardes/0000-0002-1912-2804; Palma, Roberto/0000-0002-4047-381X; Luzon Marco, Gloria/0000-0002-5352-1884; Hernando Morata, Jose Angel/0000-0002-8683-5142; Gil Ortiz, Alejandro/0000-0002-0852-412X; YAHLALI, NADIA/0000-0003-2184-0132; Monrabal, Francesc/0000-0002-4047-5620; Ripoll, Lluis/0000-0001-8194-5396; Perez-Aparicio, Jose/0000-0003-2884-6991; Natal da Luz, Hugo/0000-0003-1177-870X; Fernandes, Luis/0000-0002-7061-8768; Iguaz Gutierrez, Francisco Jose/0000-0001-6327-9369 FU Spanish Ministerio de Economia y Competitividad [CONSOLIDER-Ingenio 2010 CSD2008-0037, Consolider-Ingenio 2010 CSD2007-00042, FPA2008-03456, FPA2009-13697-C04-04]; FCT(Lisbon) and FEDER [PTDC/FIS/103860/2008]; European Commission under the European Research Council T-REX Starting Grant of the IDEAS program of the 7th EU Framework Program [ERC-2009-StG-240054]; Office of Science, Office of Basic Energy Sciences, of the US Department of Energy [DE-AC02-05CH11231]; European Regional Development Fund (ERDF/FEDER); US DOE NNSA Stewardship Science Graduate Fellowship [DE-FC52-08NA28752]; Eurotalents program FX We deeply acknowledge LSC directorate and staff for their strong support for performing the measurements at the LSC Radiopurity Service. The NEXT Collaboration acknowledges funding support from the following agencies and institutions: the Spanish Ministerio de Economia y Competitividad under grants CONSOLIDER-Ingenio 2010 CSD2008-0037 (CUP), Consolider-Ingenio 2010 CSD2007-00042 (CPAN), and under contracts ref. FPA2008-03456, FPA2009-13697-C04-04; FCT(Lisbon) and FEDER under grant PTDC/FIS/103860/2008; the European Commission under the European Research Council T-REX Starting Grant ref. ERC-2009-StG-240054 of the IDEAS program of the 7th EU Framework Program; Director, Office of Science, Office of Basic Energy Sciences, of the US Department of Energy under contract no. DE-AC02-05CH11231. Part of these grants are funded by the European Regional Development Fund (ERDF/FEDER). J. Renner (LBNL) acknowledges the support of a US DOE NNSA Stewardship Science Graduate Fellowship under contract no. DE-FC52-08NA28752. F.I. acknowledges the support from the Eurotalents program. NR 32 TC 17 Z9 17 U1 2 U2 14 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 1748-0221 J9 J INSTRUM JI J. Instrum. PD JAN PY 2013 VL 8 AR T01002 DI 10.1088/1748-0221/8/01/T01002 PG 19 WC Instruments & Instrumentation SC Instruments & Instrumentation GA 167WF UT WOS:000320665400083 ER PT J AU Choong, WS Peng, Q Vu, CQ Turko, BT Moses, WW AF Choong, W. -S. Peng, Q. Vu, C. Q. Turko, B. T. Moses, W. W. TI High-performance electronics for time-of-flight PET systems SO JOURNAL OF INSTRUMENTATION LA English DT Article DE Analogue electronic circuits; Gamma camera, SPECT, PET PET/CT, coronary CT angiography (CTA); Front-end electronics for detector readout ID RESOLUTION AB We have designed and built a high-performance readout electronics system for time-of-flight positron emission tomography (TOF PET) cameras. The electronics architecture is based on the electronics for a commercial whole-body PET camera (Siemens/CPS Cardinal electronics), modified to improve the timing performance. The fundamental contributions in the electronics that can limit the timing resolution include the constant fraction discriminator (CFD), which converts the analog electrical signal from the photo-detector to a digital signal whose leading edge is time-correlated with the input signal, and the time-to-digital converter (TDC), which provides a time stamp for the CFD output. Coincident events are identified by digitally comparing the values of the time stamps. In the Cardinal electronics, the front-end processing electronics are performed by an Analog subsection board, which has two application-specific integrated circuits (ASICs), each servicing a PET block detector module. The ASIC has a built-in CFD and TDC. We found that a significant degradation in the timing resolution comes from the ASIC's CFD and TDC. Therefore, we have designed and built an improved Analog subsection board that replaces the ASIC's CFD and TDC with a high-performance CFD (made with discrete components) and TDC (using the CERN high-performance TDC ASIC). The improved Analog subsection board is used in a custom single-ring LSO-based TOF PET camera. The electronics system achieves a timing resolution of 60 ps FWHM. Prototype TOF detector modules are read out with the electronics system and give coincidence timing resolutions of 259 ps FWHM and 156 ps FWHM for detector modules coupled to LSO and LaBr3 crystals respectively. C1 [Choong, W. -S.; Peng, Q.; Vu, C. Q.; Turko, B. T.; Moses, W. W.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Choong, WS (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. EM wschoong@lbl.gov RI peng, qiyu/G-1586-2013 FU Office of Science, Office of Biological and Environmental Research, Biological Systems Science Division of the U.S. Department of Energy [DE-AC02-05CH11231]; National Institutes of Health, National Institute of Biomedical Imaging and Bioengineering [R01EB006085] FX The authors would like to thank Mike Casey and John Young of Siemens Medical Solutions, Knoxville, TN, for their support with the Siemens/CPS Cardinal electronics. This work was supported in part by the Director, Office of Science, Office of Biological and Environmental Research, Biological Systems Science Division of the U.S. Department of Energy under contract no. DE-AC02-05CH11231, and in part by the National Institutes of Health, National Institute of Biomedical Imaging and Bioengineering, under Grant Number R01EB006085. NR 5 TC 5 Z9 5 U1 1 U2 12 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 1748-0221 J9 J INSTRUM JI J. Instrum. PD JAN PY 2013 VL 8 AR T01006 DI 10.1088/1748-0221/8/01/T01006 PG 10 WC Instruments & Instrumentation SC Instruments & Instrumentation GA 167WF UT WOS:000320665400087 PM 24575149 ER PT J AU Jones, BJP VanGemert, JK Conrad, JM Pla-Dalmau, A AF Jones, B. J. P. VanGemert, J. K. Conrad, J. M. Pla-Dalmau, A. TI Photodegradation mechanisms of tetraphenyl butadiene coatings for liquid argon detectors SO JOURNAL OF INSTRUMENTATION LA English DT Article DE Noble-liquid detectors (scintillation, ionization two-phase); Scintillators, scintillation and light emission processes (solid, gas and liquid scintillators); Photon detectors for UV, visible and IR photons (gas) (gas-photocathodes, solid-photocathodes) AB We report on studies of degradation mechanisms of tetraphenyl butadiene (TPB) coatings of the type used in neutrino and dark matter liquid argon experiments. Using gas chromatography coupled to mass spectrometry we have detected the ultraviolet-blocking impurity benzophenone. We monitored the drop in performance and increase of benzophenone concentration in TPB plates with exposure to ultraviolet (UV) light, and demonstrate the correlation between these two variables. Based on the presence and initially exponential increase in the concentration of benzophenone observed, we propose that TPB degradation is a free radical-mediated photooxidation reaction, which is subsequently confirmed by displaying delayed degradation using a free radical inhibitor. Finally we show that the performance of wavelength-shifting coatings of the type envisioned for the LBNE experiment can be improved by 10-20%, with significantly delayed UV degradation, by using a 20% admixture of 4-tert-Butylcatechol. C1 [Jones, B. J. P.; Conrad, J. M.] MIT, Cambridge, MA 02139 USA. [VanGemert, J. K.; Pla-Dalmau, A.] Fermilab Natl Accelerator Lab, Batavia, IL 60510 USA. RP Jones, BJP (reprint author), MIT, 77 Massachusetts Ave, Cambridge, MA 02139 USA. EM bjpjones@mit.edu FU National Science Foundation [NSF-PHY-084784]; Department Of Energy [DE-FG02-91ER40661]; Fermi National Accelerator Laboratory; United States Department of Energy [De-AC02-07CH11359] FX We would like to thank Christie Chiu for her help in performing preliminary studies related to this paper. The authors thank the National Science Foundation (NSF-PHY-084784) and Department Of Energy (DE-FG02-91ER40661). This work was supported by the Fermi National Accelerator Laboratory, which is operated by the Fermi Research Alliance, LLC under Contract No. De-AC02-07CH11359 with the United States Department of Energy. NR 16 TC 12 Z9 12 U1 0 U2 3 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 1748-0221 J9 J INSTRUM JI J. Instrum. PD JAN PY 2013 VL 8 AR P01013 DI 10.1088/1748-0221/8/01/P01013 PG 13 WC Instruments & Instrumentation SC Instruments & Instrumentation GA 167WF UT WOS:000320665400070 ER PT J AU Mekkaoui, A Garcia-Sciveres, M Gnani, D AF Mekkaoui, A. Garcia-Sciveres, M. Gnani, D. TI Results of 65 nm pixel readout chip demonstrator array SO JOURNAL OF INSTRUMENTATION LA English DT Article; Proceedings Paper CT Topical Workshop on Electronics for Particle Physics CY SEP 17-21, 2012 CL Oxford, ENGLAND SP US Dept Engergy, U S Natl Sci Fdn, U K Sci and Technol Facilities Council DE Analogue electronic circuits; Radiation-hard electronics; Front-end electronics for detector readout; VLSI circuits AB Complex and challenging instrumentation projects (LHC upgrades, HL LHC, new Detector concepts) will require the adoption of ever more empowering and complex IC technologies. We clearly see that by moving only two nodes from the current 130 nm CMOS to 65 nm, substantial processing power could be embedded in the front-end system. We have designed and fabricated a prototype pixel readout chip to explore 65 nm CMOS as a potential integrated circuit technology for future particle physics applications. Not only the reported functional test results are very encouraging, but we also found that the process is fundamentally tolerant to radiation doses higher than 600 Mrad. C1 [Mekkaoui, A.; Garcia-Sciveres, M.; Gnani, D.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Mekkaoui, A (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, 1 Cyclotron Rd Mail Stop 50A6134, Berkeley, CA 94720 USA. EM amekkaoui@lbl.gov RI Gnani, Dario/J-6426-2012 OI Gnani, Dario/0000-0003-0464-9176 NR 2 TC 5 Z9 5 U1 0 U2 2 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 1748-0221 J9 J INSTRUM JI J. Instrum. PD JAN PY 2013 VL 8 AR C01055 DI 10.1088/1748-0221/8/01/C01055 PG 7 WC Instruments & Instrumentation SC Instruments & Instrumentation GA 167WF UT WOS:000320665400055 ER PT J AU Wu, J AF Wu, J. TI A digitization scheme of sub-microampere current using a commercial comparator with hysteresis and FPGA-based wave union TDC SO JOURNAL OF INSTRUMENTATION LA English DT Article; Proceedings Paper CT Topical Workshop on Electronics for Particle Physics CY SEP 17-21, 2012 CL Oxford, ENGLAND SP US Dept Engergy, U S Natl Sci Fdn, U K Sci and Technol Facilities Council DE Front-end electronics for detector readout; Digital electronic circuits ID READOUT; SENSOR; ADC AB A digitization scheme of sub-microampere current using a commercial comparator with adjustable hysteresis and FPGA-based Wave Union TDC has been tested. The comparator plus a few passive components forms a current controlled oscillator and the input current is sent into the hysteresis control pin. The input current is converted into the transition times of the oscillations, which are digitized with a Wave Union TDC in FPGA and the variation of the transition times reflects the variation of the input current. Preliminary tests show that input charges <25 fC can be measured at > 50M samples/s without a preamplifier. C1 Fermilab Natl Accelerator Lab, Batavia, IL 60510 USA. RP Wu, J (reprint author), Fermilab Natl Accelerator Lab, POB 500, Batavia, IL 60510 USA. EM jywu168@fnal.gov NR 12 TC 0 Z9 0 U1 1 U2 4 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 1748-0221 J9 J INSTRUM JI J. Instrum. PD JAN PY 2013 VL 8 AR C01019 DI 10.1088/1748-0221/8/01/C01019 PG 9 WC Instruments & Instrumentation SC Instruments & Instrumentation GA 167WF UT WOS:000320665400019 ER PT J AU Yarema, R Deptuch, G Hoff, J Khalid, F Lipton, R Shenai, A Trimpl, M Zimmerman, T AF Yarema, R. Deptuch, G. Hoff, J. Khalid, F. Lipton, R. Shenai, A. Trimpl, M. Zimmerman, T. TI Vertically integrated circuit development at Fermilab for detectors SO JOURNAL OF INSTRUMENTATION LA English DT Article; Proceedings Paper CT Topical Workshop on Electronics for Particle Physics CY SEP 17-21, 2012 CL Oxford, ENGLAND SP US Dept Engergy, U S Natl Sci Fdn, U K Sci and Technol Facilities Council DE VLSI circuits; Electronic detector readout concepts (solid-state); Front-end electronics for detector readout AB Today vertically integrated circuits, (a.k.a. 3D integrated circuits) is a popular topic in many trade journals. The many advantages of these circuits have been described such as higher speed due to shorter trace lenghts, the ability to reduce cross talk by placing analog and digital circuits on different levels, higher circuit density without the going to smaller feature sizes, lower interconnect capacitance leading to lower power, reduced chip size, and different processing for the various layers to optimize performance. There are some added advantages specifically for MAPS (Monolithic Active Pixel Sensors) in High Energy Physics: four side buttable pixel arrays, 100% diode fill factor, the ability to move PMOS transistors out of the diode sensing layer, and a increase in channel density. Fermilab began investigating 3D circuits in 2006. Many different bonding processes have been described for fabricating 3D circuits [1]. Fermilab has used three different processes to fabricate several circuits for specific applications in High Energy Physics and X-ray imaging. This paper covers some of the early 3D work at Fermilab and then moves to more recent activities. The major processes we have used are discussed and some of the problems encountered are described. An overview of pertinent 3D circuit designs is presented along with test results thus far. C1 [Yarema, R.; Deptuch, G.; Hoff, J.; Khalid, F.; Lipton, R.; Shenai, A.; Trimpl, M.; Zimmerman, T.] Fermilab Natl Accelerator Lab, Batavia, IL 60510 USA. RP Yarema, R (reprint author), Fermilab Natl Accelerator Lab, POB 500, Batavia, IL 60510 USA. EM yarema@fnal.gov NR 9 TC 2 Z9 2 U1 0 U2 7 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 1748-0221 J9 J INSTRUM JI J. Instrum. PD JAN PY 2013 VL 8 AR C01052 DI 10.1088/1748-0221/8/01/C01052 PG 11 WC Instruments & Instrumentation SC Instruments & Instrumentation GA 167WF UT WOS:000320665400052 ER PT J AU Ramezanipour, F Shishkin, M Singh, K Hodges, JP Ziegler, T Thangadurai, V AF Ramezanipour, Farshid Shishkin, Maxim Singh, Kalpana Hodges, Jason P. Ziegler, Tom Thangadurai, Venkataraman TI Interstitial oxygens and cation deficiency in Mo-doped ceria, an anode material for SOFCs SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID OXIDE FUEL-CELLS; TOTAL-ENERGY CALCULATIONS; AUGMENTED-WAVE METHOD; ELECTRICAL-PROPERTIES; TRANSPORT MECHANISMS; IONIC CONDUCTORS; DEFECT STRUCTURE; BASIS-SET; ELECTROLYTES; GADOLINIUM AB Density functional theory studies show that it is energetically possible for oxygen atoms to reside on the interstitial sites in Mo-doped ceria. This is also studied experimentally using neutron diffraction experiments that show small concentration of oxygens on two intestinal sites, as well as cation deficiency in the Ce1-xMoxO2+delta (x similar to 0.07) lattice. C1 [Ramezanipour, Farshid; Shishkin, Maxim; Singh, Kalpana; Ziegler, Tom; Thangadurai, Venkataraman] Univ Calgary, Dept Chem, Calgary, AB T2N 1N4, Canada. [Hodges, Jason P.] Oak Ridge Natl Lab, Instrument & Source Design Div, Oak Ridge, TN 37831 USA. RP Thangadurai, V (reprint author), Univ Calgary, Dept Chem, 2500 Univ Dr NW, Calgary, AB T2N 1N4, Canada. EM vthangad@ucalgary.ca RI Shishkin, Maxim/I-3308-2013; Hodges, Jason/K-1421-2013 FU Natural Science and Engineering Research Council (NSERC); Scientific User Facilities Division, Office of Basic Energy Sciences, U. S. Department of Energy [DEAC05-00OR22725]; UT-Battelle, LLC FX One of us (V. T.) thanks the Natural Science and Engineering Research Council (NSERC) for funding through the Discovery Grants to support his research program on novel solid electrolytes for solid state ionic devices, including solid oxide fuel cells and solid state Li ion batteries. The authors also 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 under contract DEAC05-00OR22725 with UT-Battelle, LLC. NR 36 TC 2 Z9 2 U1 0 U2 16 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 29 BP 8344 EP 8347 DI 10.1039/c3ta11464c PG 4 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA 176NA UT WOS:000321310200005 ER PT J AU Huda, MN Deutsch, TG Sarker, P Turner, JA AF Huda, Muhammad N. Deutsch, Todd G. Sarker, Pranab Turner, John A. TI Electronic structure study of N, O related defects in GaP for photoelectrochemical applications SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID TOTAL-ENERGY CALCULATIONS; AUGMENTED-WAVE METHOD; HYDROGEN GENERATION; GALLIUM-PHOSPHIDE; BASIS-SET; WATER; RESONANCE; ALLOYS; OXIDE; BAND AB It is known that the stability of GaP as a photocatalyst in electrolytes can be enhanced by nitrogen doping, GaP:N. However, both GaP (indirect gap) and GaP:N (direct gap) have poor optical absorption properties across their fundamental band gap. To enhance optical absorption as well as the photocurrent, we have examined by density functional theory the favorability of oxygen and hydrogen impurities in conjunction with N doping in bulk GaP. It has been found here that O-related defects are more favorable, whereas H with N substitution is not very favorable. These O-N related defects create a global effect in the GaP lattice by both volume and band gap reduction. Enhancement of optical absorption was also found due to these types of complex doping. C1 [Huda, Muhammad N.; Sarker, Pranab] Univ Texas Arlington, Dept Phys, Arlington, TX 76019 USA. [Deutsch, Todd G.; Turner, John A.] Natl Renewable Energy Lab, Golden, CO 80401 USA. RP Huda, MN (reprint author), Univ Texas Arlington, Dept Phys, POB 19059, Arlington, TX 76019 USA. EM huda@uta.edu RI Huda, Muhammad/C-1193-2008; OI Huda, Muhammad/0000-0002-2655-498X; Deutsch, Todd/0000-0001-6577-1226 FU National Renewable Energy Laboratory [XEJ-9-99042-01]; U.S. Department of Energy Fuel Cell Technologies Office [DE-AC36-08-G028303] FX MNH was supported by National Renewable Energy Laboratory sub-contract no. XEJ-9-99042-01. TGD and JAT were supported by the U.S. Department of Energy Fuel Cell Technologies Office under Contract no. DE-AC36-08-G028303 with the National Renewable Energy Laboratory. NR 29 TC 0 Z9 0 U1 4 U2 38 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 29 BP 8425 EP 8431 DI 10.1039/c3ta11475a PG 7 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA 176NA UT WOS:000321310200017 ER PT J AU Zheng, JM Gu, M Chen, HH Meduri, P Engelhard, MH Zhang, JG Liu, J Xiao, J AF Zheng, Jianming Gu, Meng Chen, Honghao Meduri, Praveen Engelhard, Mark H. Zhang, Ji-Guang Liu, Jun Xiao, Jie TI Ionic liquid-enhanced solid state electrolyte interface (SEI) for lithium-sulfur batteries SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID ELECTROCHEMICAL PERFORMANCE; CARBON COMPOSITES; CATHODE; SURFACE; CELLS; EFFICIENCY; SALTS AB Li-S batteries are a complicated system with many challenges existing before their final market penetration. While most of the reported work for Li-S batteries is focused on the cathode design, we demonstrate in this work that the anode consumption accelerated by corrosive polysulfide solution also critically determines the Li-S cell performance. To validate this hypothesis, ionic liquid (IL) N-methyl-N-butylpyrrolidinium bis(trifluoromethylsulfonyl)imide (Py14TFSI) has been employed to modify the properties of the SEI layer formed on the Li metal surface in Li-S batteries. It is found that the IL-enhanced passivation film on the lithium anode surface exhibits very different morphology and chemical composition, effectively protecting lithium metal from continuous attack by soluble polysulfides. Therefore, both the cell impedance and the irreversible consumption of polysulfides on lithium metal are reduced. As a result, the Coulombic efficiency and the cycling stability of Li-S batteries have been greatly improved. After 120 cycles, the Li-S battery cycled in the electrolyte containing 75% IL demonstrates a high capacity retention of 94.3% at 0.1 C rate. These results reveal one of the main failure mechanisms in Li-S batteries and shine the light on new approaches to improve the reversible capacity and cyclability of Li-S batteries. This work provides important clues for the understanding and thus the improvement of Li-S battery systems through a different point of view. C1 [Zheng, Jianming; Gu, Meng; Chen, Honghao; Meduri, Praveen; Engelhard, Mark H.; Zhang, Ji-Guang; Liu, Jun; Xiao, Jie] Pacific NW Natl Lab, Richland, WA 99354 USA. RP Xiao, J (reprint author), Pacific NW Natl Lab, Richland, WA 99354 USA. EM jie.xiao@pnnl.gov RI Gu, Meng/B-8258-2013; Zheng, Jianming/F-2517-2014; OI Zheng, Jianming/0000-0002-4928-8194; Engelhard, Mark/0000-0002-5543-0812 FU Department of Energy's Office of Biological and Environmental Research; DOE by Battelle [DE-AC05-76RL01830]; Office of Vehicle Technologies of the U.S. Department of Energy FX This work is supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the U.S. Department of Energy. The SEM and XPS were conducted at the Environmental and Molecular Sciences 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. PNNL is a multi-program national laboratory operated for DOE by Battelle under Contract DE-AC05-76RL01830. NR 28 TC 75 Z9 77 U1 31 U2 182 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 29 BP 8464 EP 8470 DI 10.1039/c3ta11553d PG 7 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA 176NA UT WOS:000321310200022 ER PT J AU Woo, JJ Zhang, ZC Rago, NLD Lu, WQ Amine, K AF Woo, Jung-Je Zhang, Zhengcheng Rago, Nancy L. Dietz Lu, Wenquan Amine, Khalil TI A high performance separator with improved thermal stability for Li-ion batteries SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article AB A thermally stable separator based on a poly( phenylene oxide)/SiO2 composite is prepared using a dry phase inversion method. The separator endures up to 250 degrees C without obvious thermal deformation. A LiNi1/3Mn1/3Co1/3O2/graphite cell using the composite separator showed excellent cycling performance, especially at high C-rates. C1 [Woo, Jung-Je; Zhang, Zhengcheng; Rago, Nancy L. Dietz; Lu, Wenquan; Amine, Khalil] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. RP Zhang, ZC (reprint author), Argonne Natl Lab, Chem Sci & Engn Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM zzhang@anl.gov RI Amine, Khalil/K-9344-2013 FU Vehicle Technology Program, Integrated Laboratory/Industry Research Project (ILIRP); Department of Energy; U. S. Department of Energy Office of Science Laboratory [DE-AC02-06CH11357] FX This work was supported by the Vehicle Technology Program, Integrated Laboratory/Industry Research Project (ILIRP) and Department of Energy. Argonne National Laboratory, a U. S. Department of Energy Office of Science Laboratory, is operated under Contract no. DE-AC02-06CH11357. NR 20 TC 6 Z9 9 U1 5 U2 35 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 30 BP 8538 EP 8540 DI 10.1039/c3ta12154b PG 3 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA 180TV UT WOS:000321622300006 ER PT J AU Qiao, L Xiao, HY Heald, SM Bowden, ME Varga, T Exarhos, GJ Biegalski, MD Ivanov, IN Weber, WJ Droubay, TC Chambers, SA AF Qiao, L. Xiao, H. Y. Heald, S. M. Bowden, M. E. Varga, T. Exarhos, G. J. Biegalski, M. D. Ivanov, I. N. Weber, W. J. Droubay, T. C. Chambers, S. A. TI The impact of crystal symmetry on the electronic structure and functional properties of complex lanthanum chromium oxides SO JOURNAL OF MATERIALS CHEMISTRY C LA English DT Article ID RAY-ABSORPTION SPECTRA; PRE-EDGE; K-EDGE; TRANSITION; PEROVSKITE; HETEROSTRUCTURES; HETEROJUNCTIONS; LEVEL; FILMS AB Complex oxides exhibit a wide range of crystal structures, chemical compositions and physical properties. The underlying drivers determining the complicated structure-composition-property phase diagrams are the relative positions and orbital overlaps between the metal cations and the oxygen anions. Here we report a combined experimental and theoretical investigation of the structure and bonding in a series of lanthanum chromium oxides prepared by molecular beam epitaxy. Of particular interest is the charge state and local coordination of the Cr. We have stabilized LaCrO3, LaCrO4 and La2CrO6 films by controlling the three elemental fluxes during deposition, and have carried out X-ray diffraction, X-ray photoemission, and X-ray absorption spectroscopy, as well as first-principles calculations, to determine structure, charge state, chemical bonding, and electronic structure. Significant changes in bonding character and orbital interaction are revealed with decreasing ligand symmetry from octahedral to tetrahedral Cr coordination. Both LaCrO4 and La2CrO6 with tetrahedrally coordinated Cr show strong pre-edge features in the Cr K-edge near-edge structure whereas LaCrO3 with octahedrally coordinated Cr exhibits very weak pre-edge features. The origin of these pre-edge features is discussed based on various selection rules and ligand symmetry. We also demonstrate an increase in cation-anion orbital hybridization and a decrease in long-range ligand coupling induced by this symmetry reduction. These in turn result in dramatic modifications of the macroscopic optical and magnetic properties. C1 [Qiao, L.; Exarhos, G. J.; Droubay, T. C.; Chambers, S. A.] Pacific NW Natl Lab, Fundamental & Computat Sci Directorate, Richland, WA 99352 USA. [Qiao, L.; Biegalski, M. D.; Ivanov, I. N.] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN USA. [Xiao, H. Y.; Weber, W. J.] Univ Tennessee, Dept Mat Sci & Engn, Knoxville, TN 37996 USA. [Heald, S. M.] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. [Bowden, M. E.; Varga, T.] Pacific NW Natl Lab, Environm Mol Sci Lab, Richland, WA 99352 USA. RP Qiao, L (reprint author), Pacific NW Natl Lab, Fundamental & Computat Sci Directorate, Richland, WA 99352 USA. EM sa.chambers@pnnl.gov RI Qiao, Liang/A-8165-2012; Weber, William/A-4177-2008; ivanov, ilia/D-3402-2015; Droubay, Tim/D-5395-2016 OI Weber, William/0000-0002-9017-7365; ivanov, ilia/0000-0002-6726-2502; Droubay, Tim/0000-0002-8821-0322 FU U.S. Department of Energy, Office of Science, Division of Materials Sciences and Engineering [10122]; Division of Chemical Sciences [48526]; Department of Energy's Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory; Oak Ridge National Laboratory by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy; US DOE [DE-AC02-06CH11357]; U.S. Department of Energy, Office of Science, Basic Energy Science, Materials Sciences and Engineering Division; National Natural Science Foundation of China [11004023] FX This work was supported by the U.S. Department of Energy, Office of Science, Division of Materials Sciences and Engineering under Award #10122, and Division of Chemical Sciences under Award #48526. The work was performed in the Environmental Molecular Sciences Laboratory, a national science user facility sponsored by the Department of Energy's Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory. A portion of this research was conducted at the Center for Nanophase Materials Sciences, which is sponsored at Oak Ridge National Laboratory by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy. Use of the Advanced Photon Source, an Office of Science User Facility operated for the US DOE Office of Science by Argonne National Laboratory, was supported by the US DOE under Contract no. DE-AC02-06CH11357. H. Y. Xiao and W. J. Weber were supported by the U.S. Department of Energy, Office of Science, Basic Energy Science, Materials Sciences and Engineering Division. H. Y. Xiao also acknowledges the partial support of the National Natural Science Foundation of China (Grant no. 11004023). The theoretical calculations were performed using the supercomputer resources at the Environmental Molecular Sciences Laboratory (EMSL) located at the Pacific Northwest National Laboratory. NR 66 TC 12 Z9 12 U1 3 U2 59 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7526 J9 J MATER CHEM C JI J. Mater. Chem. C PY 2013 VL 1 IS 30 BP 4527 EP 4535 DI 10.1039/c3tc30883a PG 9 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA 181JO UT WOS:000321664100003 ER PT S AU Gecys, P Markauskas, E Raciukaitis, G Repins, I Beall, C AF Gecys, P. Markauskas, E. Raciukaitis, G. Repins, I. Beall, C. BE Emmelmann, C Zaeh, MF Graf, T Schmidt, M TI Selective front side patterning of CZTS thin-film solar cells by picosecond laser induced material lift-off process SO LASERS IN MANUFACTURING (LIM 2013) SE Physics Procedia LA English DT Proceedings Paper CT 7th International WLT Conference on Lasers in Manufacturing (LiM) CY MAY 13-16, 2013 CL Munich, GERMANY SP German Sci Laser Soc (WLT), Hamburg Univ Technol (TUHH), Inst Laser & Syst Technologies (ILAS), Ruhr Univ Bochum (RUB), Appl Laser Technol (LAT), Tech Univ Hamburg Harburg (TUHH), Ruhr Univ Bochum (RUB) DE CZTS; thin-film; picosecond laser scribing; material lift-off AB The thin-film Cu-chalcopyrite based solar cell technologies become more attractive due to their lower cost and optimal performance. Efficiency of cells with a large area might be maintained if small segments are interconnected in series in order to reduce photocurrent in thin films and resistance losses, and laser scribing is crucial for performance of the device. We present our results on the material lift-off effect investigations in the CZTS thin-film solar cell structures which can be applied for the damage-free front-side scribing processes. The results of the P2 and P3 type scribe formation with the fundamental harmonics of a picosecond laser are presented. (C) 2013 The Authors. Published by Elsevier B.V. C1 [Gecys, P.; Markauskas, E.; Raciukaitis, G.] Ctr Phys Sci & Technol, Savanoriu Ave 231, LT-2300 Vilnius, Lithuania. [Repins, I.; Beall, C.] Natl Renewable Energy Lab, Golden, CO 80401 USA. RP Gecys, P (reprint author), Ctr Phys Sci & Technol, Savanoriu Ave 231, LT-2300 Vilnius, Lithuania. EM p.gecys@ar.fi.lt FU National Programme "An improvement of the skills of researchers"; Lithuanian Ministry of Education and Science FX The work was carried out within the project VP1-3.1-g MM-08-K-01-009 that is partly supported by the National Programme "An improvement of the skills of researchers" launched by the Lithuanian Ministry of Education and Science. NR 7 TC 1 Z9 1 U1 1 U2 13 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA SARA BURGERHARTSTRAAT 25, PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 1875-3892 J9 PHYSCS PROC PY 2013 VL 41 BP 734 EP 738 DI 10.1016/j.phpro.2013.03.142 PG 5 WC Engineering, Manufacturing; Physics, Applied SC Engineering; Physics GA BFR27 UT WOS:000321039300099 ER PT J AU Zhang, HZ Finnegan, MP Banfield, JF AF Zhang, Hengzhong Finnegan, Michael P. Banfield, Jillian F. TI Titania nanorods curve to lower their energy SO NANOSCALE LA English DT Article ID NANOCRYSTALLINE TITANIA; ORIENTED ATTACHMENT; PHASE-STABILITY; CRYSTAL-GROWTH; TIO2; INSIGHTS; ANATASE; RUTILE; BEHAVIOR AB Spontaneous formation of curved nanorods is generally unexpected, since curvature introduces strain energy. However, electron microscopy shows that under hydrothermal conditions, some nanorods grown by oriented attachment of small anatase particles on {101} surfaces are curved and dislocation free. Molecular dynamics simulations show that the lattice energy of a curved anatase rod is actually lower than that of a linear rod due to more attractive long-range interatomic Coulombic interactions among atoms in the curved rod. The thermodynamic driving force stemming from lattice energy could be harnessed to produce asymmetric morphologies unexpected from classical Ostwald ripening with unusual shapes and properties. C1 [Zhang, Hengzhong; Finnegan, Michael P.; Banfield, Jillian F.] Univ Calif Berkeley, Dept Earth & Planetary Sci, Berkeley, CA 94720 USA. [Banfield, Jillian F.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, Berkeley, CA 94720 USA. RP Zhang, HZ (reprint author), Univ Calif Berkeley, Dept Earth & Planetary Sci, Berkeley, CA 94720 USA. EM heng@eps.berkeley.edu; jban.eld@berkeley.edu FU National Science Foundation [CHE-1213835, EAR-0920921]; U.S. Department of Energy [DE-AC02-05CH11231] FX The TEM work was performed in the National Center for Electron Microscopy, Lawrence Berkeley National Laboratory. This research was supported by the National Science Foundation (Grant nos CHE-1213835 and EAR-0920921) and U.S. Department of Energy (Grant no. DE-AC02-05CH11231). NR 25 TC 6 Z9 6 U1 1 U2 28 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2040-3364 J9 NANOSCALE JI Nanoscale PY 2013 VL 5 IS 15 BP 6742 EP 6746 DI 10.1039/c3nr02616g PG 5 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA 181NY UT WOS:000321675600013 PM 23794056 ER PT J AU Azoz, S Jiang, J Keskar, G McEnally, C Alkas, A Ren, F Marinkovic, N Haller, GL Ismail-Beigi, S Pfefferle, LD AF Azoz, Seyla Jiang, Jie Keskar, Gayatri McEnally, Charles Alkas, Alp Ren, Fang Marinkovic, Nebojsa Haller, Gary L. Ismail-Beigi, Sohrab Pfefferle, Lisa D. TI Mechanism for strong binding of CdSe quantum dots to multiwall carbon nanotubes for solar energy harvesting SO NANOSCALE LA English DT Article ID PHOTOINDUCED CHARGE-TRANSFER; SHAPE CONTROL; NANOCRYSTALS; CELLS; ATTACHMENT; POLYMER; NANOPARTICLES; ASSEMBLIES; EFFICIENCY; DEFECTS AB As hybrid nanomaterials have myriad of applications in modern technology, different functionalization strategies are being intensely sought for preparing nanocomposites with tunable properties and structures. Multi-Walled Carbon Nanotube (MWNT)/CdSe Quantum Dot (QD) heterostructures serve as an important example for an active component of solar cells. The attachment mechanism of CdSe QDs and MWNTs is known to affect the charge transfer between them and consequently to alter the efficiency of solar cell devices. In this study, we present a novel method that enables the exchange of some of the organic capping agents on the QDs with carboxyl functionalized MWNTs upon ultrasonication. This produces a ligand-free covalent attachment of the QDs to the MWNTs. EXAFS characterization reveals direct bond formation between the CdSe QDs and the MWNTs. The amount of oleic acid exchanged is quantified by temperature-programmed decomposition; the results indicate that roughly half of the oleic acid is removed from the QDs upon functionalized MWNT addition. Additionally, we characterize the optical and structural properties of the QD-MWNT heterostructures and investigate how these properties are affected by the attachment. The steady state photoluminescence response of QDs is completely quenched. The lifetime of the PL of the QDs measured with time resolved photoluminescence shows a significant decrease after they are covalently bonded to functionalized MWNTs, suggesting a fast charge transfer between QDs and MWNTs. Our theoretical calculations are consistent with and support these experimental findings and provide microscopic models for the QD binding mechanisms. C1 [Azoz, Seyla; Keskar, Gayatri; McEnally, Charles; Ren, Fang; Haller, Gary L.; Pfefferle, Lisa D.] Yale Univ, Mason Lab, New Haven, CT 06520 USA. [Jiang, Jie; Ismail-Beigi, Sohrab] Yale Univ, Dept Appl Phys, New Haven, CT 06520 USA. [Alkas, Alp] European Retail Capital Markets Jones Lang LaSall, London W1B 5NH, England. [Marinkovic, Nebojsa] Brookhaven Natl Lab, Natl Synchrotron Light Source, Upton, NY 11973 USA. RP Pfefferle, LD (reprint author), Yale Univ, Mason Lab, 9 Hillhouse Ave, New Haven, CT 06520 USA. EM alp.alkas@eu.jll.com; lisa.pfefferle@yale.edu RI Ismail-Beigi, Sohrab/F-2382-2014; Marinkovic, Nebojsa/A-1137-2016; McEnally, Charles/N-9999-2016 OI Ismail-Beigi, Sohrab/0000-0002-7331-9624; Marinkovic, Nebojsa/0000-0003-3579-3453; McEnally, Charles/0000-0002-6820-921X FU NSF [DMR-0934520 Solar] FX The authors gratefully acknowledge financial support from NSF DMR-0934520 Solar. We thank the NSLS beam lines X18B, U4B and U7A at Brookhaven National Laboratory for use of their facilities and acknowledge Dr Cherno Jaye and Dr Dario Arena for their support in collecting the NEXAFS data. We acknowledge Dr Stephen Golledge, and Dr Abhinav Nath for their contribution towards the work. NR 39 TC 11 Z9 12 U1 2 U2 58 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 15 BP 6893 EP 6900 DI 10.1039/c3nr00928a PG 8 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA 181NY UT WOS:000321675600033 PM 23783269 ER PT J AU Wang, CJ Ranasingha, O Natesakhawat, S Ohodnicki, PR Andio, M Lewis, JP Matranga, C AF Wang, Congjun Ranasingha, Oshadha Natesakhawat, Sittichai Ohodnicki, Paul R., Jr. Andio, Mark Lewis, James P. Matranga, Christopher TI Visible light plasmonic heating of Au-ZnO for the catalytic reduction of CO2 SO NANOSCALE LA English DT Article ID CHEMICAL-VAPOR-DEPOSITION; METAL NANOPARTICLES; OXIDE NANOCRYSTALS; CHARGE-CARRIERS; GOLD; SURFACE; WATER; NANOSTRUCTURES; ABSORPTION; OXIDATION AB Plasmonic excitation of Au nanoparticles attached to the surface of ZnO catalysts using low power 532 nm laser illumination leads to significant heating of the catalyst and the conversion of CO2 and H-2 reactants to CH4 and CO products. Temperature-calibrated Raman spectra of ZnO phonons show that intensity-dependent plasmonic excitation can controllably heat Au-ZnO from 30 to similar to 600 degrees C and simultaneously tune the CH4 : CO product ratio. The laser induced heating and resulting CH4 : CO product distribution agrees well with predictions from thermodynamic models and temperature-programmed reaction experiments indicating that the reaction is a thermally driven process resulting from the plasmonic heating of the Au-ZnO. The apparent quantum yield for CO2 conversion under continuous wave (cw) 532 nm laser illumination is 0.030%. The Au-ZnO catalysts are robust and remain active after repeated laser exposure and cycling. The light intensity required to initiate CO2 reduction is low (similar to 2.5 x 10(5) W m(-2)) and achievable with solar concentrators. Our results illustrate the viability of plasmonic heating approaches for CO2 utilization and other practical thermal catalytic applications. C1 [Wang, Congjun; Ranasingha, Oshadha; Natesakhawat, Sittichai; Ohodnicki, Paul R., Jr.; Andio, Mark; Lewis, James P.; Matranga, Christopher] US DOE, Natl Energy Technol Lab, Pittsburgh, PA 15236 USA. [Wang, Congjun] URS Corp, South Pk, PA 15129 USA. [Ranasingha, Oshadha; Lewis, James P.] W Virginia Univ, Dept Phys, Morgantown, WV 26506 USA. [Natesakhawat, Sittichai] Univ Pittsburgh, Dept Chem & Petr Engn, Pittsburgh, PA 15261 USA. RP Wang, CJ (reprint author), US DOE, Natl Energy Technol Lab, 626 Cochrans Mill Rd, Pittsburgh, PA 15236 USA. EM congjun.wang@netl.doe.gov RI Matranga, Christopher/E-4741-2015 OI Matranga, Christopher/0000-0001-7082-5938 FU National Energy Technology Laboratory under the RES [DE-FE0004000]; Department of Energy, National Energy Technology Laboratory, an agency of the United States Government; URS Energy & Construction, Inc. FX This technical effort was performed in support of the National Energy Technology Laboratory's ongoing research into CO2 capture under the RES contract DE-FE0004000. We thank Dr Phuoc Tran for assistance with the pulsed laser experiment and Dr Junseok Lee for stimulating discussions. 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 50 TC 40 Z9 40 U1 10 U2 134 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 15 BP 6968 EP 6974 DI 10.1039/c3nr02001k PG 7 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA 181NY UT WOS:000321675600043 PM 23794025 ER PT J AU Duffey, KC Shih, O Wong, NL Drisdell, WS Saykally, RJ Cohen, RC AF Duffey, Kaitlin C. Shih, Orion Wong, Nolan L. Drisdell, Walter S. Saykally, Richard J. Cohen, Ronald C. TI Evaporation kinetics of aqueous acetic acid droplets: effects of soluble organic aerosol components on the mechanism of water evaporation SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID MASS ACCOMMODATION COEFFICIENT; MOLECULAR-DYNAMICS SIMULATIONS; SUM-FREQUENCY SPECTROSCOPY; LIQUID-GAS INTERFACE; CONDENSATION COEFFICIENT; ATMOSPHERIC PARTICLES; AIR/WATER INTERFACE; CARBOXYLIC-ACIDS; GROWTH-KINETICS; CLOUD DROPLETS AB The presence of organic surfactants in atmospheric aerosol may lead to a depression of cloud droplet growth and evaporation rates affecting the radiative properties and lifetime of clouds. Both the magnitude and mechanism of this effect, however, remain poorly constrained. We have used Raman thermometry measurements of freely evaporating micro-droplets to determine evaporation coefficients for several concentrations of acetic acid, which is ubiquitous in atmospheric aerosol and has been shown to adsorb strongly to the air-water interface. We find no suppression of the evaporation kinetics over the concentration range studied (1-5 M). The evaporation coefficient determined for 2 M acetic acid is 0.53 +/- 0.12, indistinguishable from that of pure water (0.62 +/- 0.09). C1 [Duffey, Kaitlin C.; Shih, Orion; Wong, Nolan L.; Saykally, Richard J.; Cohen, Ronald C.] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Duffey, Kaitlin C.; Shih, Orion; Saykally, Richard J.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. [Drisdell, Walter S.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. [Cohen, Ronald C.] Univ Calif Berkeley, Dept Earth & Planetary Sci, Berkeley, CA 94720 USA. RP Saykally, RJ (reprint author), Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. EM saykally@berkeley.edu; rccohen@berkeley.edu RI Cohen, Ronald/A-8842-2011 OI Cohen, Ronald/0000-0001-6617-7691 FU National Science Foundation [ATM 0639847]; Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231] FX The authors thank Dr. Patrick Varilly for insightful discussions about evaporation and for his input regarding our temperature calibrations and cooling model. We also thank Frank Liu and Michael Angell for their assistance in collecting data. This work was supported by National Science Foundation Grant ATM 0639847 and the Director, Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract DE-AC02-05CH11231. NR 48 TC 10 Z9 10 U1 4 U2 60 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2013 VL 15 IS 28 BP 11634 EP 11639 DI 10.1039/c3cp51148k PG 6 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 175AN UT WOS:000321201500006 PM 23677455 ER PT J AU Sharma, K Bilheux, HZ Walker, LMH Voisin, S Mayes, RT Kiggans, JO Yiacoumi, S DePaoli, DW Dai, S Tsouris, C AF Sharma, Ketki Bilheux, Hassina Z. Walker, Lakeisha M. H. Voisin, Sophie Mayes, Richard T. Kiggans, Jim O., Jr. Yiacoumi, Sotira DePaoli, David W. Dai, Sheng Tsouris, Costas TI Neutron imaging of ion transport in mesoporous carbon materials SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID COMPOSITE FILM ELECTRODES; PEM FUEL-CELLS; CAPACITIVE DEIONIZATION; WATER DISTRIBUTION; LIQUID WATER; LITHIUM BATTERIES; AQUEOUS-SOLUTIONS; ROOT-GROWTH; ELECTROSORPTION; RADIOGRAPHY AB Neutron imaging is presented as a tool for quantifying the diffusion of ions inside porous materials, such as carbon electrodes used in the desalination process via capacitive deionization and in electro-chemical energy-storage devices. Monolithic mesoporous carbon electrodes of similar to 10 nm pore size were synthesized based on a soft-template method. The electrodes were used with an aqueous solution of gadolinium nitrate in an electrochemical flow-through cell designed for neutron imaging studies. Sequences of neutron images were obtained under various conditions of applied potential between the electrodes. The images revealed information on the direction and magnitude of ion transport within the electrodes. From the time-dependent concentration profiles inside the electrodes, the average value of the effective diffusion coefficient for gadolinium ions was estimated to be 2.09 +/- 0.17 x 10(-11) m(2) s(-1) at 0 V and 1.42 +/- 0.06 x 10(-10) m(2) s(-1) at 1.2 V. The values of the effective diffusion coefficient obtained from neutron imaging experiments can be used to evaluate model predictions of the ion transport rate in capacitive deionization and electrochemical energy-storage devices. C1 [Sharma, Ketki; Yiacoumi, Sotira] Georgia Inst Technol, Atlanta, GA 30332 USA. [Bilheux, Hassina Z.; Walker, Lakeisha M. H.; Voisin, Sophie; Mayes, Richard T.; Kiggans, Jim O., Jr.; DePaoli, David W.; Dai, Sheng; Tsouris, Costas] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. RP Tsouris, C (reprint author), Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. EM tsourisc@ornl.gov RI Bilheux, Hassina/H-4289-2012; Tsouris, Costas/C-2544-2016; Dai, Sheng/K-8411-2015; Mayes, Richard/G-1499-2016; kiggans, james/E-1588-2017; OI Bilheux, Hassina/0000-0001-8574-2449; Tsouris, Costas/0000-0002-0522-1027; Dai, Sheng/0000-0002-8046-3931; Mayes, Richard/0000-0002-7457-3261; kiggans, james/0000-0001-5056-665X; Voisin, Sophie/0000-0002-9726-4605 FU U.S. DOE Office of Energy Efficiency and Renewable Energy (EERE) [DE-AC05-0096OR22725]; Oak Ridge National Laboratory; Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy; Campbell Applied Physics, Inc.; National Science Foundation [CBET-0651683] FX This research was conducted at the Oak Ridge National Laboratory and supported by the U.S. DOE Office of Energy Efficiency and Renewable Energy (EERE), under Contract DE-AC05-0096OR22725 with Oak Ridge National Laboratory, managed by UT-Battelle, LLC. A portion of this 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. Partial support to S. Yiacoumi and K. Sharma was provided by Campbell Applied Physics, Inc., and the National Science Foundation under Grant No. CBET-0651683. The authors are thankful to Charles R. Schaich for constructing the flow-through neutron cell and Bob Campbell, Bill Bourcier, Tom Dorow, Sunita Kaushik, and Fred Seamon of Campbell Applied Physics, Inc., for frequent discussions on capacitive deionization. NR 55 TC 8 Z9 8 U1 1 U2 57 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 28 BP 11740 EP 11747 DI 10.1039/c3cp51310f PG 8 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 175AN UT WOS:000321201500019 PM 23756558 ER PT J AU Rodriguez, JA Hanson, JC Stacchiola, D Senanayake, SD AF Rodriguez, Jose A. Hanson, Jonathan C. Stacchiola, Dario Senanayake, Sanjaya D. TI In situ/operando studies for the production of hydrogen through the water-gas shift on metal oxide catalysts SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID X-RAY-ABSORPTION; TIME-RESOLVED CHARACTERIZATION; LOW-TEMPERATURE; HETEROGENEOUS CATALYSIS; SITU CHARACTERIZATION; PARTICLE-SIZE; ACTIVE-SITE; CUO-CEO2 CATALYSTS; RAMAN-SPECTROSCOPY; REACTION-MECHANISM AB In this perspective article, we show how a series of in situ techniques {X-ray diffraction (XRD), pair-distribution-function analysis (PDF), X-ray absorption fine structure (XAFS), environmental transmission electron microscopy (ETEM), infrared spectroscopy (IR), ambient-pressure X-ray photoelectron spectroscopy (AP-XPS)} can be combined to perform detailed studies of the structural, electronic and chemical properties of metal oxide catalysts used for the production of hydrogen through the water-gas shift reaction (WGS, CO + H2O -> H-2 + CO2). Under reaction conditions most WGS catalysts undergo chemical transformations that drastically modify their composition with respect to that obtained during the synthesis process. Experiments of time-resolved in situ XRD, XAFS, and PDF indicate that the active phase of catalysts which combine Cu, Au or Pt with oxides such as ZnO, CeO2, TiO2, CeOx/TiO2 and Fe2O3 essentially involves nanoparticles of the reduced noble metals. The oxide support undergoes partial reduction and is not a simple spectator, facilitating the dissociation of water and in some cases modifying the chemical properties of the supported metal. Therefore, to optimize the performance of these catalysts one must take into consideration the properties of the metal and oxide phases. IR and AP-XPS have been used to study the reaction mechanism for the WGS on metal oxide catalysts. Data of IR spectroscopy indicate that formate species are not necessarily involved in the main reaction path for the water-gas shift on Cu-, Au- and Pt-based catalysts. Thus, a pure redox mechanism or associative mechanisms that involve either carbonate-like (CO3, HCO3) or carboxyl (HOCO) species should be considered. In the last two decades, there have been tremendous advances in our ability to study catalytic materials under reaction conditions and we are moving towards the major goal of fully understanding how the active sites for the production of hydrogen through the WGS actually work. C1 [Rodriguez, Jose A.; Hanson, Jonathan C.; Stacchiola, Dario; Senanayake, Sanjaya D.] Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA. RP Rodriguez, JA (reprint author), Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA. EM rodrigez@bnl.gov RI Stacchiola, Dario/B-1918-2009; Senanayake, Sanjaya/D-4769-2009 OI Stacchiola, Dario/0000-0001-5494-3205; Senanayake, Sanjaya/0000-0003-3991-4232 FU US Department of Energy (DOE), Chemical Sciences Division [DE-AC02-98CH10086]; Divisions of Materials and Chemical Sciences of US-DOE FX Many of the in situ studies described above were done in collaboration with past and current members of the Catalysis Group at BNL. We are grateful to all of them: X. Wang, W. Wen, L. Barrio, M. Estrella, G. Zhou, R. Si and W. Xu. Our in situ work has benefited from thought-provoking conversations with scientists studying different aspects of the water-gas shift reaction: C. T. Campbell, J. Hrbek, P. Liu, J. Evans, M. Fernandez-Garcia, A. Martinez-Arias, J. Graciani, J. Fernandez-Sanz, F. Illas, J. Ciston, R. M. Navarro, J. L. G. Fierro, H. Idriss and M. Flytzani-Stephanopoulos. The work at BNL was financed by the US Department of Energy (DOE), Chemical Sciences Division (DE-AC02-98CH10086). The National Synchrotron Light Source is supported by the Divisions of Materials and Chemical Sciences of US-DOE. NR 126 TC 37 Z9 37 U1 16 U2 228 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 29 BP 12004 EP 12025 DI 10.1039/c3cp50416f PG 22 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 175ZB UT WOS:000321271300003 PM 23660768 ER PT J AU Li, ZJ Kay, BD Dohnalek, Z AF Li, Zhenjun Kay, Bruce D. Dohnalek, Zdenek TI Dehydration and dehydrogenation of ethylene glycol on rutile TiO2(110) SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID O-H; ALIPHATIC-ALCOHOLS; MOLECULAR-OXYGEN; SURFACE SCIENCE; BOND SCISSION; ADSORPTION; REACTIVITY; CHEMISTRY; DEFECTS; WATER AB The interactions of ethylene glycol with a partially reduced rutile TiO2(110) surface have been studied using temperature programmed desorption (TPD). The saturation coverage on surface Ti rows is determined to be 0.43 monolayer (ML), slightly less than one ethylene glycol per two Ti sites. Most of the adsorbed ethylene glycol (similar to 80%) undergoes further reactions to yield other products. Two major channels are observed, dehydration yielding ethylene and water and dehydrogenation yielding acetaldehyde and hydrogen. Hydrogen formation is rather surprising as it has not been observed previously on TiO2(110) from simple organic molecules. The coverage dependent yields of ethylene and acetaldehyde correlate well with those of water and hydrogen, respectively. Dehydration dominates at lower ethylene glycol coverages (<0.2 ML) and plateaus as the coverage is increased to saturation. Dehydrogenation is observed primarily at higher ethylene glycol coverages (>0.2 ML). Our results suggest that the observed dehydration and dehydrogenation reactions proceed via different surface intermediates. C1 [Kay, Bruce D.] Pacific NW Natl Lab, Phys Sci Directorate, Richland, WA 99352 USA. Pacific NW Natl Lab, Inst Integrated Catalysis, Richland, WA 99352 USA. RP Kay, BD (reprint author), Pacific NW Natl Lab, Phys Sci Directorate, POB 999, Richland, WA 99352 USA. EM Bruce.Kay@pnnl.gov; Zdenek.Dohnalek@pnnl.gov OI Dohnalek, Zdenek/0000-0002-5999-7867 FU US Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences Biosciences FX This work was supported by the US Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences & Biosciences, and performed in the Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility sponsored by the Department of Energy's Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory (PNNL). PNNL is a multiprogram national laboratory operated for the DOE by Battelle. NR 38 TC 8 Z9 8 U1 5 U2 48 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 29 BP 12180 EP 12186 DI 10.1039/c3cp50687h PG 7 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 175ZB UT WOS:000321271300022 PM 23764541 ER PT J AU Baber, AE Mudiyanselage, K Senanayake, SD Beatriz-Vidal, A Luck, KA Sykes, ECH Liu, P Rodriguez, JA Stacchiola, DJ AF Baber, Ashleigh E. Mudiyanselage, Kumudu Senanayake, Sanjaya D. Beatriz-Vidal, Alba Luck, Kyle A. Sykes, E. Charles H. Liu, Ping Rodriguez, Jose A. Stacchiola, Dario J. TI Assisted deprotonation of formic acid on Cu(111) and self-assembly of 1D chains SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID GAS SHIFT REACTION; TEMPERATURE-PROGRAMMED DESORPTION; SCANNING-TUNNELING-MICROSCOPY; METHANOL SYNTHESIS; STRUCTURE SENSITIVITY; THERMAL-DESORPTION; CO2 HYDROGENATION; COPPER SURFACES; ACTIVE-SITE; FORMATE AB Formic acid (HCOOH) deprotonates on the open surfaces of Cu(110) and Cu(100) when exposed at 300 K. However, this does not occur on the close-packed surface of clean Cu(111). In this study, we show that the deprotonation of formic acid on atomically flat Cu(111) surfaces can be induced by pre-adsorbing polymeric formic acid clusters at low temperatures, and then annealing the system to break the acidic O-H bond of HCOOH adsorbed on the edges of the polymeric clusters. The thermal activation of HCOOH to bidentate formate was studied using a combination of infrared reflection absorption spectroscopy, scanning tunneling microscopy, X-ray photoelectron spectroscopy, and near edge X-ray absorption fine structure spectroscopy. Extended 1D formate structures self-assemble due to a templating effect introduced by the formation of long alpha-polymeric formic acid chains commensurate with the substrate. C1 [Baber, Ashleigh E.; Mudiyanselage, Kumudu; Senanayake, Sanjaya D.; Beatriz-Vidal, Alba; Luck, Kyle A.; Rodriguez, Jose A.; Stacchiola, Dario J.] Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA. [Sykes, E. Charles H.] Tufts Univ, Dept Chem, Medford, MA 02155 USA. [Liu, Ping] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. RP Stacchiola, DJ (reprint author), Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA. EM djs@bnl.gov RI Stacchiola, Dario/B-1918-2009; Mudiyanselage, Kumudu/B-2277-2013; Senanayake, Sanjaya/D-4769-2009 OI Stacchiola, Dario/0000-0001-5494-3205; Mudiyanselage, Kumudu/0000-0002-3539-632X; Senanayake, Sanjaya/0000-0003-3991-4232 FU US Department of Energy (Chemical Sciences Division) [DE-AC02-98CH10886]; National Science Foundation [CBET-1159882] FX The work carried out at Brookhaven National Laboratory was supported by the US Department of Energy (Chemical Sciences Division, DE-AC02-98CH10886). E.C.H.S. thanks the National Science Foundation (CBET-1159882) for support. NR 64 TC 7 Z9 7 U1 1 U2 60 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2013 VL 15 IS 29 BP 12291 EP 12298 DI 10.1039/c3cp51533h PG 8 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 175ZB UT WOS:000321271300034 PM 23775138 ER PT J AU Politi, JRD Vines, F Rodriguez, JA Illas, F AF dos Santos Politi, Jose Roberto Vines, Francesc Rodriguez, Jose A. Illas, Francesc TI Atomic and electronic structure of molybdenum carbide phases: bulk and low Miller-index surfaces SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID TRANSITION-METAL CARBIDES; DENSITY-FUNCTIONAL THEORY; AU-C INTERACTIONS; AUGMENTED-WAVE METHOD; GAS-SHIFT REACTION; CHARGE POLARIZATION; TUNGSTEN CARBIDE; ADSORPTION; CATALYSTS; DISSOCIATION AB The geometric and electronic structure of catalytically relevant molybdenum carbide phases (cubic delta-MoC, hexagonal alpha-MoC, and orthorhombic beta-Mo2C) and their low Miller-index surfaces have been investigated by means of periodic density functional theory (DFT) based calculations with the Perdew-Burke-Ernzerhof (PBE) exchange-correlation functional. Comparison to available experimental data indicates that this functional is particularly well suited to study these materials. The calculations reveal that beta-Mo2C has a stronger metallic character than the other two polymorphs, both beta-Mo2C and d-MoC have a large ionic contribution, and delta- and alpha-MoC exhibit the strongest covalent character. Among the various surfaces explored, the calculations reveal the high stability of the delta-MoC(001) nonpolar surface, Mo- and C-terminated (001) polar surfaces of alpha-MoC, and the nonpolar (011) surface of beta-Mo2C. A substantially low work function of only 3.4 eV is predicted for beta-Mo2C(011), suggesting that this system is particularly well suited for (electro) catalytic processes where surface -> adsorbate electron transfer is essential. The overall implications for heterogeneously catalysed reactions by these molybdenum carbide nanoparticles are also discussed. C1 [dos Santos Politi, Jose Roberto; Vines, Francesc; Illas, Francesc] Univ Barcelona, Dept Quim Fis, E-08028 Barcelona, Spain. [dos Santos Politi, Jose Roberto; Vines, Francesc; Illas, Francesc] Univ Barcelona, Inst Quim Teor & Computac IQTCUB, E-08028 Barcelona, Spain. [dos Santos Politi, Jose Roberto] Univ Brasilia, Inst Quim, Lab Quim Computac, BR-70904970 Brasilia, DF, Brazil. [Rodriguez, Jose A.] Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA. RP Illas, F (reprint author), Univ Barcelona, Dept Quim Fis, C Marti & Franques 1, E-08028 Barcelona, Spain. EM francesc.illas@ub.edu RI Illas, Francesc /C-8578-2011; Politi, Jose Roberto/K-7105-2013; OI Illas, Francesc /0000-0003-2104-6123; Politi, Jose Roberto/0000-0001-8202-6586; Vines, Francesc/0000-0001-9987-8654 FU Spanish MICINN [FIS2008-02238, CTQ2012-30751]; Generalitat de Catalunya [2009SGR1041, XRQTC]; US Department of Energy [DE-AC02-98CH10886]; MINECO [JCI-2010-06372]; CNPq Brasil; ICREA Academia award for excellence in research FX This work was supported by the Spanish MICINN (grants FIS2008-02238 and CTQ2012-30751), Generalitat de Catalunya (grants 2009SGR1041 and XRQTC) and US Department of Energy (DE-AC02-98CH10886). F. V. thanks the MINECO for a postdoctoral Juan de la Cierva grant (JCI-2010-06372), J.R.S.P. is thankful to CNPq Brasil for his postdoctoral fellowship and F. I. acknowledges additional support through the 2009 ICREA Academia award for excellence in research. Computational time at the MARENOSTRUM supercomputer has been generously provided by the Barcelona Supercomputing Centre. NR 77 TC 27 Z9 27 U1 13 U2 119 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 30 BP 12617 EP 12625 DI 10.1039/c3cp51389k PG 9 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 180TW UT WOS:000321622500028 PM 23787949 ER PT J AU Kamath, G Deshmukh, SA Baker, GA Mancini, DC Sankaranarayanan, SKRS AF Kamath, Ganesh Deshmukh, Sanket A. Baker, Gary A. Mancini, Derrick C. Sankaranarayanan, Subramanian K. R. S. TI Thermodynamic considerations for solubility and conformational transitions of poly-N-isopropyl-acrylamide SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID CRITICAL SOLUTION TEMPERATURE; MOLECULAR-DYNAMICS; FREE-ENERGIES; FORCE-FIELD; POLY(N-ISOPROPYLACRYLAMIDE) HYDROGELS; PARTITION-COEFFICIENTS; PHASE-EQUILIBRIA; WATER; ISOPROPYLACRYLAMIDE; POTENTIALS AB Thermodynamic considerations based on the free energy of hydration, free energy of solvation and partition coefficient predictions of the monomer N-isopropyl-acrylamide (NIPAM) determined using various intermolecular potentials are used to elucidate the origin of hydrophobicity/hydrophilicity across the lower critical solution temperature (LCST). Thermodynamic properties are predicted for NIPAM using adaptive bias force-molecular dynamics and various popular force-fields (AMBER, OPLS-AA, CHARMM and GROMOS) at four different temperatures: below the LCST (275 K and 300 K) and above the LCST (310 K and 330 K). The effect of changes in the thermodynamic properties of the monomer NIPAM at various temperatures below and above LCST on the kinetics of conformational transition of thermo-sensitive polymers is discussed. Our findings provide encouraging prospects for understanding the LCST transition in the hydrogel poly-N-isopropylacrylamide which shows temperature-dependent conformational changes in part due to the complex interplay of hydrophilic/hydrophobic interactions. C1 [Kamath, Ganesh; Baker, Gary A.] Univ Missouri, Dept Chem, Columbia, MO 65211 USA. [Deshmukh, Sanket A.; Mancini, Derrick C.; Sankaranarayanan, Subramanian K. R. S.] Argonne Natl Lab, Argonne, IL 60439 USA. RP Mancini, DC (reprint author), Argonne Natl Lab, 9700 S Cass Ave, Argonne, IL 60439 USA. EM mancini@anl.gov; skrssank@anl.gov RI Baker, Gary/H-9444-2016 OI Baker, Gary/0000-0002-3052-7730 FU U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]; [2F32501-ANL] FX Use of the Center for Nanoscale Materials was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. The authors thank the computational facilities provided by CNM-ANL (CNM-31237) and the University of Missouri-Bioinformatics Consortium. Financial support from subcontract No. 2F32501-ANL to University of Missouri (GK and GAB) is gratefully acknowledged. NR 29 TC 5 Z9 5 U1 2 U2 54 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 30 BP 12667 EP 12673 DI 10.1039/c3cp44076a PG 7 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 180TW UT WOS:000321622500033 PM 23793265 ER PT S AU Lechman, JB Yarrington, C Erikson, W Noble, DR AF Lechman, Jeremy B. Yarrington, Cole Erikson, William Noble, David R. BE Yu, A Dong, K Yang, R Luding, S TI Thermal Conduction in Particle Packs via Finite Elements SO POWDERS AND GRAINS 2013 SE AIP Conference Proceedings LA English DT Proceedings Paper CT 7th International Conference on Micromechanics of Granular Media (Powders and Grains) CY JUL 08-12, 2013 CL Sydney, AUSTRALIA SP Assoc Study Micromechan Granular Media (AEMMG), Univ New S Wales (UNSW), Lab Simulat & Modelling Particulate Syst (SIMPAS), Curtin Univ (CU), Dept Chemical Engn, Univ Twente (UT), Multi Scale Mech Grp (CTW & MESA+), JMBC Res Sch Fluid Mechan, Elsevier, Univ New S Wales (UNSW), Sch Mat Sci & Engn DE Finite Element; thermal conduction; granular ID SPHERES; FLOW; SUSPENSIONS; SIMULATION; LATTICES AB Conductive transport in heterogeneous materials composed of discrete particles is a fundamental problem for a number of applications. While analytical results and rigorous bounds on effective conductivity in mono-sized particle dispersions are well established in the literature, the methods used to arrive at these results often fail when the average size of particle clusters becomes large (i.e., near the percolation transition where particle contact networks dominate the bulk conductivity). Our aim is to develop general, efficient numerical methods that would allow us to explore this behavior and compare to a recent microstructural description of conduction in this regime. To this end, we present a finite element analysis approach to modeling heat transfer in granular media with the goal of predicting effective bulk thermal conductivities of particle-based heterogeneous composites. Our approach is verified against theoretical predictions for random isotropic dispersions of mono-disperse particles at various volume fractions up to close packing. Finally, we present results for the probability distribution of the effective conductivity in particle dispersions generated by Brownian dynamics, and suggest how this might be useful in developing stochastic models of effective properties based on the dynamical process involved in creating heterogeneous dispersions. C1 [Lechman, Jeremy B.; Yarrington, Cole; Erikson, William] Sandia Natl Labs, Nanoscale & React Proc Dept, POB 5800, Albuquerque, NM 87185 USA. [Noble, David R.] Sandia Natl Labs, Thermal & Fluid Proc Dept, Albuquerque, NM USA. RP Lechman, JB (reprint author), Sandia Natl Labs, Nanoscale & React Proc Dept, POB 5800, Albuquerque, NM 87185 USA. FU Sandia National Laboratories is a multi-program laboratory; Sandia Corporation; Lockheed Martin Corporation; 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 Energys National Nuclear Security Administration under contract DE-AC04- 94AL85000. NR 23 TC 0 Z9 0 U1 0 U2 7 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1166-1 J9 AIP CONF PROC PY 2013 VL 1542 BP 539 EP 542 DI 10.1063/1.4811987 PG 4 WC Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Science & Technology - Other Topics; Materials Science; Physics GA BFQ84 UT WOS:000321003200130 ER PT S AU Perton, M Levesque, D Monchalin, JP Lord, M Smith, JA Rabin, BH AF Perton, M. Levesque, D. Monchalin, J-P Lord, M. Smith, J. A. Rabin, B. H. BE Thompson, DO Chimenti, DE TI LASER SHOCKWAVE TECHNIQUE FOR CHARACTERIZATION OF NUCLEAR FUEL PLATE INTERFACES SO REVIEW OF PROGRESS IN QUANTITATIVE NONDESTRUCTIVE EVALUATION, VOLS 32A AND 32B SE AIP Conference Proceedings LA English DT Proceedings Paper CT 39th Annual Review of Progress in Quantitative Nondestructive Evaluation (QNDE) CY JUL 15-20, 2012 CL Denver, CO SP QNDE Programs, AF Res Lab, Army Res Lab, Amer Soc Nondestruct Testing (ASNT), Dept Energy, AMES Lab, Fed Aviat Adm (FAA), Natl Aeronaut & Space Adm (NASA), Natl Sci Fdn (NSF), Ind/Univ Cooperat Res Ctr, Iowa State Univ, Ctr Nondestruct Evaluat DE Laser Ultrasonics; Shock Waves; Adhesion Testing; Nuclear Fuel Plate AB The US National Nuclear Security Agency is tasked with minimizing the worldwide use of high-enriched uranium. One aspect of that effort is the conversion of research reactors to monolithic fuel plates of low-enriched uranium. The manufacturing process includes hot isostatic press bonding of an aluminum cladding to the fuel foil. The Laser Shockwave Technique (LST) is here evaluated for characterizing the interface strength of fuel plates using depleted Uranium/Mo foils. LST is a non-contact method that uses lasers for the generation and detection of large amplitude acoustic waves and is therefore well adapted to the quality assurance of this process. Preliminary results show a clear signature of well-bonded and debonded interfaces and the method is able to classify/rank the bond strength of fuel plates prepared under different HIP conditions. C1 [Perton, M.; Levesque, D.; Monchalin, J-P; Lord, M.] Natl Res Council Canada, 75 de Mortagne Blvd, Boucherville, PQ J4B 6Y4, Canada. [Smith, J. A.; Rabin, B. H.] Idaho Natl Lab, Idaho Falls, ID 83415 USA. RP Perton, M (reprint author), Natl Res Council Canada, 75 de Mortagne Blvd, Boucherville, PQ J4B 6Y4, Canada. EM jean-pierre.monchalin@cnrc-nrc.gc.ca; James.Smith@INL.gov NR 7 TC 2 Z9 2 U1 0 U2 2 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1129-6 J9 AIP CONF PROC PY 2013 VL 1511 BP 345 EP 352 DI 10.1063/1.4789068 PG 8 WC Materials Science, Characterization & Testing SC Materials Science GA BFM02 UT WOS:000320452600042 ER PT S AU Sun, JG AF Sun, J. G. BE Thompson, DO Chimenti, DE TI EVOLUTION OF IMAGE PROCESSING METHODS FOR PULSED THERMAL IMAGING SO REVIEW OF PROGRESS IN QUANTITATIVE NONDESTRUCTIVE EVALUATION, VOLS 32A AND 32B SE AIP Conference Proceedings LA English DT Proceedings Paper CT 39th Annual Review of Progress in Quantative Nondestructive Evaluation (QNDE) CY JUL 15-20, 2012 CL Denver, CO SP QNDE Programs, AF Res Lab, Army Res Lab, Amer Soc Nondestruct Testing (ASNT), Dept Energy, AMES Lab, Fed Aviat Adm (FAA), Natl Aeronaut & Space Adm (NASA), Natl Sci Fdn (NSF), Ind/Univ Cooperat Res Ctr, Iowa State Univ, Ctr Nondestruct Evaluat DE Image Processing Methods; Pulsed Thermal Imaging; Nondestructive Evaluation ID THERMOGRAPHY; DIFFUSIVITY; ENHANCEMENT AB Pulsed thermal imaging is a commonly used infrared thermal imaging technology for nondestructive evaluation of engineering materials. It provides a complete interrogation and therefore a potentially complete quantification of the thermal properties of a test material. Two distinct applications have been pursued in the development of data/imaging processing methods: one for material property measurement and the other for flaw or discontinuity detection. For property measurement, theoretical models for one-and multi-layer materials are used to determine thickness-averaged material properties. For flaw detection, various image-processing methods are developed to enhance and extract the thermal contrast induced by subsurface flaw/discontinuities. This study examines the evolution of these methods and compares the differences of flaw-detection methods for detection and characterization of delamination flaws. C1 Argonne Natl Lab, Nucl Engn Div, Argonne, IL 60439 USA. RP Sun, JG (reprint author), Argonne Natl Lab, Nucl Engn Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM sun@anl.gov NR 15 TC 0 Z9 0 U1 0 U2 2 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1129-6 J9 AIP CONF PROC PY 2013 VL 1511 BP 691 EP 698 DI 10.1063/1.4789113 PG 8 WC Materials Science, Characterization & Testing SC Materials Science GA BFM02 UT WOS:000320452600087 ER PT S AU Bakhtiari, S Wang, K Elmer, TW Koehl, E Raptis, AC AF Bakhtiari, S. Wang, K. Elmer, T. W. Koehl, E. Raptis, A. C. BE Thompson, DO Chimenti, DE TI DEVELOPMENT OF A NOVEL ULTRASONIC TEMPERATURE PROBE FOR LONG-TERM MONITORING OF DRY CASK STORAGE SYSTEMS SO REVIEW OF PROGRESS IN QUANTITATIVE NONDESTRUCTIVE EVALUATION, VOLS 32A AND 32B SE AIP Conference Proceedings LA English DT Proceedings Paper CT 39th Annual Review of Progress in Quantative Nondestructive Evaluation (QNDE) CY JUL 15-20, 2012 CL Denver, CO SP QNDE Programs, AF Res Lab, Army Res Lab, Amer Soc Nondestruct Testing (ASNT), Dept Energy, AMES Lab, Fed Aviat Adm (FAA), Natl Aeronaut & Space Adm (NASA), Natl Sci Fdn (NSF), Ind/Univ Cooperat Res Ctr, Iowa State Univ, Ctr Nondestruct Evaluat DE Dry Cask Storage System; Ultrasonic Temperature Probe; Long-term Temperature Monitoring ID THERMOMETRY AB With the recent cancellation of the Yucca Mountain repository and the limited availability of wet storage utilities for spent nuclear fuel (SNF), more attention has been directed toward dry cask storage systems (DCSSs) for long-term storage of SNF. Consequently, more stringent guidelines have been issued for the aging management of dry storage facilities that necessitate monitoring of the conditions of DCSSs. Continuous health monitoring of DCSSs based on temperature variations is one viable method for assessing the integrity of the system. In the present work, a novel ultrasonic temperature probe (UTP) is being tested for long-term online temperature monitoring of DCSSs. Its performance was evaluated and compared with type N thermocouple (NTC) and resistance temperature detector (RTD) using a small-scale dry storage canister mockup. Our preliminary results demonstrate that the UTP system developed at Argonne is able to achieve better than 0.8 degrees C accuracy, tested at temperatures of up to 400 degrees C. The temperature resolution is limited only by the sampling rate of the current system. The flexibility of the probe allows conforming to complex geometries thus making the sensor particularly suited to measurement scenarios where access is limited. C1 [Bakhtiari, S.; Wang, K.; Elmer, T. W.; Koehl, E.; Raptis, A. C.] Argonne Natl Lab, Nucl Engn Div, Argonne, IL 60439 USA. RP Bakhtiari, S (reprint author), Argonne Natl Lab, Nucl Engn Div, 9700 S Cass Ave,Bldg 308, Argonne, IL 60439 USA. EM kwang@anl.gov NR 11 TC 1 Z9 1 U1 0 U2 3 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1129-6 J9 AIP CONF PROC PY 2013 VL 1511 BP 1526 EP 1533 DI 10.1063/1.4789223 PG 8 WC Materials Science, Characterization & Testing SC Materials Science GA BFM02 UT WOS:000320452600197 ER PT S AU Meyer, RM Ramuhalli, P Doctor, SR Bond, LJ AF Meyer, R. M. Ramuhalli, P. Doctor, S. R. Bond, L. J. BE Thompson, DO Chimenti, DE TI QUALIFICATION REQUIREMENTS OF GUIDED ULTRASONIC WAVES FOR INSPECTION OF PIPING IN LIGHT WATER REACTORS SO REVIEW OF PROGRESS IN QUANTITATIVE NONDESTRUCTIVE EVALUATION, VOLS 32A AND 32B SE AIP Conference Proceedings LA English DT Proceedings Paper CT 39th Annual Review of Progress in Quantitative Nondestructive Evaluation (QNDE) CY JUL 15-20, 2012 CL Denver, CO SP QNDE Programs, AF Res Lab, Army Res Lab, Amer Soc Nondestruct Testing (ASNT), Dept Energy, AMES Lab, Fed Aviat Adm (FAA), Natl Aeronaut & Space Adm (NASA), Natl Sci Fdn (NSF), Ind/Univ Cooperat Res Ctr, Iowa State Univ, Ctr Nondestruct Evaluat DE Guided Ultrasonic Waves; Performance Demonstration; Qualification; Nuclear Power Plant ID DEFECTS; NOTCHES; PIPES; MODE AB It is anticipated that guided ultrasonic wave (GUW) techniques will eventually see widespread application in the nuclear power industry as there are several near-term and future needs that could benefit from the availability of GUW technologies. Already, GUW techniques are receiving consideration for inspecting buried piping at nuclear power plants and future applications may include several Class 1 and 2 components. To accept the results of a nondestructive examination of safety critical components, the U. S. Nuclear Regulatory Commission requires that the examinations be performed using qualified equipment, personnel, and procedures. As the use of GUW techniques becomes more frequent, qualification may be required. Performance demonstration has been the approach to qualifying conventional NDE methods in the nuclear power industry. This paper highlights potential issues and research needs associated with facilitating GUW qualification for the nuclear power industry. Parametric studies of essential inspection parameters are necessary to understand their influence on inspection performance. The large volume sampling capability introduces several challenges for qualifying GUW techniques including the quantification of performance, potential interference caused by the presence of multiple flaws in the inspection region, and the practicality of manufacturing several large qualification specimens. Computer simulation may have a significant role in reducing the experimental burden associated with qualifying GUW techniques for nuclear power plant examinations. C1 [Meyer, R. M.; Ramuhalli, P.; Doctor, S. R.] Pacific Northwest Natl Lab, Richland, WA 99352 USA. [Bond, L. J.] Iowa State Univ, Ctr Nondestruct Evaluat, Ames, IA 50011 USA. RP Meyer, RM (reprint author), Pacific Northwest Natl Lab, Richland, WA 99352 USA. FU Reactor Aging Management (RAM) Focus Area of Pacific Northwest National Laboratory (PNNL); Sustainable Nuclear Power Initiative (SNPI); US Department of Energy [DE-AC06-76RLO 1830] FX This work was supported through the Reactor Aging Management (RAM) Focus Area of the Pacific Northwest National Laboratory (PNNL) Sustainable Nuclear Power Initiative (SNPI). PNNL is a multi-program national laboratory operated by Battelle Memorial Institute for the US Department of Energy under DE-AC06-76RLO 1830. NR 26 TC 0 Z9 0 U1 0 U2 3 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1129-6 J9 AIP CONF PROC PY 2013 VL 1511 BP 1662 EP 1669 DI 10.1063/1.4789241 PG 8 WC Materials Science, Characterization & Testing SC Materials Science GA BFM02 UT WOS:000320452600215 ER PT S AU Schley, RS Hurley, DH Hua, ZA AF Schley, R. S. Hurley, D. H. Hua, Z. A. BE Thompson, DO Chimenti, DE TI OPTICAL FIBER TECHNIQUE FOR IN-REACTOR MECHANICAL PROPERTIES MEASUREMENT SO REVIEW OF PROGRESS IN QUANTITATIVE NONDESTRUCTIVE EVALUATION, VOLS 32A AND 32B SE AIP Conference Proceedings LA English DT Proceedings Paper CT 39th Annual Review of Progress in Quantative Nondestructive Evaluation (QNDE) CY JUL 15-20, 2012 CL Denver, CO SP QNDE Programs, AF Res Lab, Army Res Lab, Amer Soc Nondestruct Testing (ASNT), Dept Energy, AMES Lab, Fed Aviat Adm (FAA), Natl Aeronaut & Space Adm (NASA), Natl Sci Fdn (NSF), Ind/Univ Cooperat Res Ctr, Iowa State Univ, Ctr Nondestruct Evaluat DE Irradiation Testing; Material Properties; Optical Fiber ID INTERNAL-FRICTION; YOUNGS MODULUS; IRRADIATION; COPPER AB In-reactor measurement of material properties is required for a better understanding of radiation effects on materials. We present an optical fiber based technique for measuring changes in elastic properties which involves exciting and measuring flexural vibrations in a thin cantilever beam. By exciting the beam and measuring the resonant frequency, changes in the modulus of elasticity can be monitored. The technique is demonstrated by monitoring the elastic property changes of a beam fabricated from copper, as the copper undergoes recrystallization at elevated temperature. C1 [Schley, R. S.; Hurley, D. H.; Hua, Z. A.] Idaho Natl Lab, Dept Mat Sci, Idaho Falls, ID 83415 USA. RP Schley, RS (reprint author), Idaho Natl Lab, Dept Mat Sci, POB 1625, Idaho Falls, ID 83415 USA. EM robert.schley@inl.gov RI Schley, Robert/B-9124-2017 OI Schley, Robert/0000-0001-8907-6535 NR 18 TC 0 Z9 0 U1 0 U2 5 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1129-6 J9 AIP CONF PROC PY 2013 VL 1511 BP 1701 EP 1708 DI 10.1063/1.4789246 PG 8 WC Materials Science, Characterization & Testing SC Materials Science GA BFM02 UT WOS:000320452600220 ER PT S AU McCloy, JS Ramuhalli, P Henager, C AF McCloy, J. S. Ramuhalli, Pradeep Henager, Charles, Jr. BE Thompson, DO Chimenti, DE TI USE OF FIRST ORDER REVERSAL CURVE MEASUREMENTS TO UNDERSTAND BARKHAUSEN NOISE EMISSION IN NUCLEAR STEEL SO REVIEW OF PROGRESS IN QUANTITATIVE NONDESTRUCTIVE EVALUATION, VOLS 32A AND 32B SE AIP Conference Proceedings LA English DT Proceedings Paper CT 39th Annual Review of Progress in Quantitative Nondestructive Evaluation (QNDE) CY JUL 15-20, 2012 CL Denver, CO SP QNDE Programs, AF Res Lab, Army Res Lab, Amer Soc Nondestruct Testing (ASNT), Dept Energy, AMES Lab, Fed Aviat Adm (FAA), Natl Aeronaut & Space Adm (NASA), Natl Sci Fdn (NSF), Ind/Univ Cooperat Res Ctr, Iowa State Univ, Ctr Nondestruct Evaluat DE Barkhausen; First Order Reversal Curves; Reversible Magnetization; Reactor Steel ID MAGNETIC-PROPERTIES; HYSTERESIS; DIAGRAMS; MODEL AB A prototypical ferritic/martensitic alloy, HT-9, of interest to the nuclear materials community was investigated for microstructure effects on Barkhausen noise emission and first-order reversal curve (FORC) analysis for three different heat-treated samples. It was observed that Barkhausen noise emission and reversible component of magnetization, computed from the FORC data, decreased with increasing measured mechanical hardness. The results are discussed in terms of the use of magnetic signatures for use in nondestructive interrogation of radiation damage and other microstructural changes in ferritic/martensitic alloys. FORC analysis is shown to be particularly useful for detailed characterization of defect density and pinning, which can be correlated to bulk nondestructive evaluation field measurements such as Barkhausen noise emission. C1 [McCloy, J. S.; Ramuhalli, Pradeep; Henager, Charles, Jr.] Pacific NW Natl Lab, Richland, WA 99352 USA. RP McCloy, JS (reprint author), Pacific NW Natl Lab, Richland, WA 99352 USA. EM pradeep.ramuhalli@pnl.gov NR 27 TC 3 Z9 3 U1 1 U2 8 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1129-6 J9 AIP CONF PROC PY 2013 VL 1511 BP 1709 EP 1716 DI 10.1063/1.4789247 PG 8 WC Materials Science, Characterization & Testing SC Materials Science GA BFM02 UT WOS:000320452600221 ER PT J AU Le, VQ Cochis, A Rimondini, L Pourroy, G Stanic, V Palkowski, H Carrado, A AF Van Quang Le Cochis, Andrea Rimondini, Lia Pourroy, Genevieve Stanic, Vesna Palkowski, Heinz Carrado, Adele TI Biomimetic calcium-phosphates produced by an auto-catalytic route on stainless steel 316L and bio-inert polyolefin SO RSC ADVANCES LA English DT Article ID HYDROXYAPATITE COATINGS; CELL-CULTURES; IN-VITRO; BIOCOMPATIBILITY; TITANIUM; BONE; IMPLANTS; SURFACE; CORROSION; METALS AB A melange of hydroxyapatite and calcium phosphate hydrate coatings have been deposited on the surfaces of 316L type stainless steel and polyolefin (PP-PE), both components of 316L/PP-PE/316L sandwich, by an auto-catalytic route using an acidic bath. Coatings on 316L are made of spherules size ranged from 100 nm to 1 mu m while those observed on PP-PE are smaller in the 50-600 nm range. Cell viability is much higher in samples with novel auto-catalytic layer of Ca-P than in the uncoated ones. Furthermore, our results show that the Ca-P coating produced by an auto-catalytic route act as promoter for osteoblasts proliferation. Osteoblasts morphology investigated by immunofluorescence proves that they are attached and well spread confirming the cytocompatibility. C1 [Van Quang Le; Pourroy, Genevieve; Carrado, Adele] Inst Phys & Chim Mat Strasbourg, UMR UDS CNRS 7504, F-67034 Strasbourg 2, France. [Cochis, Andrea; Rimondini, Lia] Univ Piemonte Orientale Amedeo Avogadro, Dept Hlth Sci, Lab Biomed & Dent Mat, I-28100 Novara, Italy. [Stanic, Vesna] Brookhaven Natl Lab, Photon Sci Directorate, Upton, NY 11973 USA. [Palkowski, Heinz] Clausthal Univ Technol TUC, Inst Met IMET Met Forming & Proc, D-38678 Clausthal Zellerfeld, Germany. RP Carrado, A (reprint author), Inst Phys & Chim Mat Strasbourg, UMR UDS CNRS 7504, 23 Rue Loess,BP 43, F-67034 Strasbourg 2, France. EM adele.carrado@ipcms.unistra.fr RI Carrado, Adele/B-6542-2014; stanic, vesna/J-9013-2012 OI Carrado, Adele/0000-0003-1094-4075; stanic, vesna/0000-0003-0318-9454 FU German Research Foundation DFG; DAAD [D/0707603]; EGIDE (PHC PROCOPE) [17895XK]; APIC-DEU-PICS [5245]; US Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-98CH10886] FX The authors are grateful for the support of the German Research Foundation DFG, DAAD (D/0707603), EGIDE (PHC PROCOPE No. 17895XK), and APIC-DEU-PICS (No. 5245) for funding this research. Moreover, we thank ThyssenKrupp Nirosta for supporting us with the steel material. 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 authors take pleasure in acknowledging M. Dris Ihiawakrim, M. Jacques Faerber and Dr Enrico Catalano for TEM, SEM and immunofluorescent observations respectively. NR 43 TC 5 Z9 5 U1 1 U2 10 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 28 BP 11255 EP 11262 DI 10.1039/c3ra23385e PG 8 WC Chemistry, Multidisciplinary SC Chemistry GA 169LU UT WOS:000320782500021 ER PT J AU Burr, T Hamada, MS Howell, J Skurikhin, M Ticknor, L Weaver, B AF Burr, Tom Hamada, Michael S. Howell, John Skurikhin, Misha Ticknor, Larry Weaver, Brian TI Estimating Alarm Thresholds for Process Monitoring Data under Different Assumptions about the Data Generating Mechanism SO SCIENCE AND TECHNOLOGY OF NUCLEAR INSTALLATIONS LA English DT Article ID CONTROL CHARTS; RUN-LENGTH; (X)OVER-BAR; LIMITS; QUANTILES; MODELS; FUEL AB Process monitoring (PM) for nuclear safeguards sometimes requires estimation of thresholds corresponding to small false alarm rates. Threshold estimation dates to the 1920s with the Shewhart control chart; however, because possible new roles for PM are being evaluated in nuclear safeguards, it is timely to consider modern model selection options in the context of threshold estimation. One of the possible new PM roles involves PM residuals, where a residual is defined as residual = data - prediction. This paper reviews alarm threshold estimation, introduces model selection options, and considers a range of assumptions regarding the data-generating mechanism for PM residuals. Two PM examples from nuclear safeguards are included to motivate the need for alarm threshold estimation. The first example involves mixtures of probability distributions that arise in solution monitoring, which is a common type of PM. The second example involves periodic partial cleanout of in-process inventory, leading to challenging structure in the time series of PM residuals. C1 [Burr, Tom; Hamada, Michael S.; Skurikhin, Misha; Ticknor, Larry; Weaver, Brian] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Howell, John] Univ Glasgow, Dept Mech Engn, Glasgow G12 8QQ, Lanark, Scotland. RP Burr, T (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM tburr@lanl.gov OI Ticknor, Lawrence/0000-0002-7967-7908 NR 47 TC 1 Z9 1 U1 0 U2 0 PU HINDAWI PUBLISHING CORPORATION PI NEW YORK PA 410 PARK AVENUE, 15TH FLOOR, #287 PMB, NEW YORK, NY 10022 USA SN 1687-6075 J9 SCI TECHNOL NUCL INS JI Sci. Technol. Nucl. Install. PY 2013 AR 705878 DI 10.1155/2013/705878 PG 18 WC Nuclear Science & Technology SC Nuclear Science & Technology GA 180YN UT WOS:000321635300001 ER PT J AU Lee, J AF Lee, Jungho TI TWO DOMAIN DECOMPOSITION METHODS FOR AUXILIARY LINEAR PROBLEMS OF A MULTIBODY ELLIPTIC VARIATIONAL INEQUALITY SO SIAM JOURNAL ON SCIENTIFIC COMPUTING LA English DT Article DE domain decomposition; variational inequalities; one-level finite element tearing and interconnecting; dual-primal finite element tearing and interconnecting; balanced domain decomposition by constraints ID ACTIVE SET STRATEGY; FETI-DP ALGORITHM; PRIMAL SUBSTRUCTURING METHOD; CONTACT PROBLEMS; LAGRANGE MULTIPLIERS; ENERGY MINIMIZATION; PART I; CONVERGENCE; ELASTICITY; CONSTRAINTS AB Elliptic variational inequalities with multiple bodies in two dimensions are considered. It is assumed that an active set method is used to handle the nonlinearity of the inequality constraint, which results in auxiliary linear problems. For solving such linear problems we study two domain decomposition methods called the finite element tearing and interconnecting (FETI-FETI) and hybrid methods in this paper. Bodies are decomposed into several subdomains in both methods. The FETI-FETI method combines the one-level FETI and the dual-primal FETI (FETI-DP) methods. We present a proof that this combined method has a condition number that depends linearly on the number of subdomains across each body and polylogarithmically on the number of elements across each subdomain. Our numerical results, and those of others, suggest that this is the best possible bound. The hybrid method combines the one-level FETI and the balanced domain decomposition by constraints (BDDC) methods; we prove that the condition number of this method has two polylogarithmic factors depending on the number of elements across each subdomain and across each body. We present numerical results confirming this theoretical finding. C1 Argonne Natl Lab, Div Math & Comp Sci, Argonne, IL 60439 USA. RP Lee, J (reprint author), Argonne Natl Lab, Div Math & Comp Sci, 9700 S Cass Ave, Argonne, IL 60439 USA. EM julee@mcs.anl.gov FU Office of Advanced Scientific Computing Research, Office of Science, U.S. Department of Energy [DE-AC02-06CH11357] FX This work was supported by the Office of Advanced Scientific Computing Research, Office of Science, U.S. Department of Energy, under contract DE-AC02-06CH11357. NR 46 TC 0 Z9 0 U1 0 U2 1 PU SIAM PUBLICATIONS PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA SN 1064-8275 J9 SIAM J SCI COMPUT JI SIAM J. Sci. Comput. PY 2013 VL 35 IS 3 BP A1350 EP A1375 DI 10.1137/100783753 PG 26 WC Mathematics, Applied SC Mathematics GA 172YX UT WOS:000321044800006 ER PT J AU Cyr, EC Shadid, JN Tuminaro, RS Pawlowski, RP Chacon, L AF Cyr, Eric C. Shadid, John N. Tuminaro, Raymond S. Pawlowski, Roger P. Chacon, Luis TI A NEW APPROXIMATE BLOCK FACTORIZATION PRECONDITIONER FOR TWO-DIMENSIONAL INCOMPRESSIBLE (REDUCED) RESISTIVE MHD SO SIAM JOURNAL ON SCIENTIFIC COMPUTING LA English DT Article DE block preconditioning; magnetohydrodynamics; stabilized finite element; large-scale parallel; multilevel preconditioner; fully implicit ID NAVIER-STOKES EQUATIONS; NEWTON-KRYLOV METHODS; ALGEBRAIC MULTILEVEL PRECONDITIONER; DRIFT-DIFFUSION; SYSTEMS; IMPLICIT; PERFORMANCE; FLUID; FLOW; SIMULATIONS AB The one-fluid visco-resistive MHD model provides a description of the dynamics of a charged fluid under the influence of an electromagnetic field. This model is strongly coupled, highly nonlinear, and characterized by physical mechanisms that span a wide range of interacting time scales. Solutions of this system can include very fast component time scales to slowly varying dynamical time scales that are long relative to the normal modes of the model equations. Fully implicit time stepping is attractive for simulating this type of wide-ranging physical phenomena. However, it is essential that one has effective preconditioning strategies so that the overall fully implicit methodology is both efficient and scalable. In this paper, we propose and explore the performance of several candidate block preconditioners for this system. One of these preconditioners is based on an operator-split approximation. This method reduces the 3 x 3 system (momentum, continuity, and magnetics) into two 2 x 2 operators: a Navier-Stokes operator (momentum and continuity) and a magnetics-velocity operator (momentum and magnetics) which takes into account the critical Lorentz force coupling. Using previously developed preconditioners for Navier-Stokes, and an initial Schur-complement approximation for the magnetics-velocity system, we show that the split preconditioner is scalable and competitive with other preconditioners, including a fully coupled algebraic multigrid method. C1 [Cyr, Eric C.; Shadid, John N.; Tuminaro, Raymond S.; Pawlowski, Roger P.] Sandia Natl Labs, Albuquerque, NM 87185 USA. [Chacon, Luis] Oak Ridge Natl Lab, Oak Ridge, TN 37837 USA. RP Cyr, EC (reprint author), Sandia Natl Labs, POB 5800, Albuquerque, NM 87185 USA. EM eccyr@sandia.gov; jnshadi@sandia.gov; rstumin@sandia.gov; rppawlo@sandia.gov; chacon@lanl.gov FU DOE Office of Science AMR program at Oak Ridge National Laboratory [DE-AC05-00OR22725]; Sandia National Laboratories [DE-AC04-94AL85000]; U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX This work was partially supported by the DOE Office of Science AMR program at Oak Ridge National Laboratory under contract DE-AC05-00OR22725, and Sandia National Laboratories under contract DE-AC04-94AL85000. 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 57 TC 14 Z9 14 U1 0 U2 15 PU SIAM PUBLICATIONS PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA SN 1064-8275 J9 SIAM J SCI COMPUT JI SIAM J. Sci. Comput. PY 2013 VL 35 IS 3 BP B701 EP B730 DI 10.1137/12088879X PG 30 WC Mathematics, Applied SC Mathematics GA 172YX UT WOS:000321044800030 ER PT J AU Peterson, JL Hammett, GW AF Peterson, J. L. Hammett, G. W. TI POSITIVITY PRESERVATION AND ADVECTION ALGORITHMS WITH APPLICATIONS TO EDGE PLASMA TURBULENCE SO SIAM JOURNAL ON SCIENTIFIC COMPUTING LA English DT Article DE numerical simulation; fluid; advection; positivity; high-order upwind ID DISCONTINUOUS GALERKIN METHOD; TIME-SPLITTING METHODS; CONSERVATION-LAWS; 2-DIMENSIONAL TURBULENCE; FINITE-DIFFERENCES; SCHEMES; ACCURACY; EQUATIONS; DYNAMICS; FLOWS AB The unique conditions of edge tokamak plasmas motivate the employment of efficient numerical methods that can robustly handle steep temperature and density gradients. To that end, we compare an Arakawa finite difference technique with some recent high-resolution upwind methods that are designed to minimize nonmonotonic overshoots while preserving the accuracy of solutions at smooth extrema. Versions of these algorithms are able to rigorously preserve positivity when that is physically relevant (such as for the advection of particle density or temperature). We explain in detail the use of these methods for the nonlinear Poisson bracket, an operator applicable to neutral fluid, gyrofluid, gyrokinetic, and general Hamiltonian simulations. For one-dimensional passive advection, the high-resolution upwind techniques maintain monotonicity and approach minimal levels of phase error and dissipation, especially at long wavelengths. In a two-dimensional incompressible Navier-Stokes vortex merging problem we find that extrema-preserving methods can resolve details at lower resolution than the Arakawa technique, are less dissipative than traditional finite volume methods while still minimizing overshoots and ensuring positivity, and model nonlinear cascade behavior fairly well without additional subgrid damping. C1 [Peterson, J. L.] Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. [Hammett, G. W.] Princeton Univ, Princeton Plasma Phys Lab, Princeton, NJ 08543 USA. RP Peterson, JL (reprint author), Lawrence Livermore Natl Lab, 7000 East Ave, Livermore, CA 94551 USA. EM peterson76@llnl.gov; hammett@pppl.gov RI Hammett, Gregory/D-1365-2011 OI Hammett, Gregory/0000-0003-1495-6647 FU U.S. Department of Energy [DE-AC52-07NA27344, DE-AC02-09CH11466]; Center for the Study of Plasma Microturbulence, a U.S. Department of Energy Scientific Discovery Through Advanced Computing project FX This work was supported by the Center for the Study of Plasma Microturbulence, a U.S. Department of Energy Scientific Discovery Through Advanced Computing project. This work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under contract DE-AC52-07NA27344 and by the Princeton Plasma Physics Laboratory under contract DE-AC02-09CH11466. NR 35 TC 2 Z9 2 U1 1 U2 16 PU SIAM PUBLICATIONS PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA SN 1064-8275 EI 1095-7197 J9 SIAM J SCI COMPUT JI SIAM J. Sci. Comput. PY 2013 VL 35 IS 3 BP B576 EP B605 DI 10.1137/120888053 PG 30 WC Mathematics, Applied SC Mathematics GA 172YX UT WOS:000321044800025 ER PT J AU Kokot, G Snezhko, A Aranson, IS AF Kokot, Gasper Snezhko, Alexey Aranson, Igor S. TI Emergent coherent states and flow rectification in active magnetic colloidal monolayers SO SOFT MATTER LA English DT Article AB We report on an emergent coherent behavior of a ferromagnetic colloidal monolayer suspended at a liquid-air interface and powered by a single-axis alternating in-plane magnetic field. Large-scale coherent states are manifested by formation of dynamic vortex arrays within the colloidal monolayer. Emergence of the dynamic coherence and self-organized patterns in this non-equilibrium colloidal system is attributed to a spontaneous symmetry breaking due to subtle interplay between magnetic, steric, and hydrodynamic forces acting on individual colloidal particles. Collective response of the magnetic colloidal monolayer induces in-plane rectified hydrodynamic surface flows which in turn entrains the particles, resulting in a variety of coherent states. C1 [Kokot, Gasper] Jozef Stefan Inst, Complex Matter Dept, Ljubljana 1000, Slovenia. [Snezhko, Alexey; Aranson, Igor S.] Argonne Natl Lab, Div Mat Sci, Argonne, IL 60439 USA. RP Snezhko, A (reprint author), Argonne Natl Lab, Div Mat Sci, 9700 S Cass Ave, Argonne, IL 60439 USA. EM snezhko@anl.gov RI Aranson, Igor/I-4060-2013 FU U.S. DOE, Office of Basic Energy Sciences, Division of Materials Science and Engineering [DE AC02-06CH11357] FX The research was supported by the U.S. DOE, Office of Basic Energy Sciences, Division of Materials Science and Engineering, under the Contract no. DE AC02-06CH11357. NR 24 TC 7 Z9 7 U1 0 U2 13 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 29 BP 6757 EP 6760 DI 10.1039/c3sm00136a PG 4 WC Chemistry, Physical; Materials Science, Multidisciplinary; Physics, Multidisciplinary; Polymer Science SC Chemistry; Materials Science; Physics; Polymer Science GA 175ZR UT WOS:000321273000020 ER PT J AU Haxton, TK Whitelam, S AF Haxton, Thomas K. Whitelam, Stephen TI Do hierarchical structures assemble best via hierarchical pathways? SO SOFT MATTER LA English DT Article ID PROTEIN CRYSTAL; GERM-FORMATION; S-LAYER; KINETICS; GROWTH; RULE; NUCLEATION; PHASE; TIME AB Hierarchically structured natural materials possess functionalities unattainable to the same components organized or mixed in simpler ways. For instance, the bones and teeth of mammals are far stronger and more durable than the mineral phases from which they are derived because their constituents are organized hierarchically from the molecular scale to the macroscale. Making similarly functional synthetic hierarchical materials will require an understanding of how to promote the self-assembly of structure on multiple length scales, without falling foul of numerous possible kinetic traps. Here we use computer simulation to study the self-assembly of a simple hierarchical structure, a square crystal lattice whose repeat unit is a tetramer. Although the target material is organized hierarchically, it self-assembles most reliably when its dynamic assembly pathway consists of the sequential addition of monomers to a single structure. Hierarchical dynamic pathways via dimer and tetramer intermediates are also viable modes of assembly, but result in general in lower yield: these intermediates have a stronger tendency than monomers to associate in ways not compatible with the target structure. In addition, assembly via tetramers results in a kinetic trap whereby material is sequestered in trimers that cannot combine to form the target crystal. We use analytic theory to relate dynamical pathways to the presence of equilibrium phases close in free energy to the target structure, and to identify the thermodynamic principles underpinning optimum self-assembly in this model: (1) make the free energy gap between the target phase and the most stable fluid phase of order kBT, and (2) ensure that no other dense phases (liquids or close-packed solids of monomers or oligomers) or fluids of incomplete building blocks fall within this gap. C1 [Haxton, Thomas K.; Whitelam, Stephen] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA. RP Whitelam, S (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA. EM swhitelam@lbl.gov 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 This work was performed at the Molecular Foundry, Lawrence Berkeley National Laboratory, used resources of the National Energy Research Scientific Computing Center, and was supported by the Director, Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. NR 56 TC 14 Z9 14 U1 1 U2 40 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 29 BP 6851 EP 6861 DI 10.1039/c3sm27637f PG 11 WC Chemistry, Physical; Materials Science, Multidisciplinary; Physics, Multidisciplinary; Polymer Science SC Chemistry; Materials Science; Physics; Polymer Science GA 175ZR UT WOS:000321273000030 ER PT S AU Appavoo, K Brady, NF Seo, M Nag, J Prasankumar, RP Hilton, DJ Haglund, RF AF Appavoo, K. Brady, N. F. Seo, M. Nag, J. Prasankumar, R. P. Hilton, D. J. Haglund, R. F., Jr. BE Chergui, M Taylor, A Cundiff, S DeVivieRiedle, R Yamagouchi, K TI Ultrafast Phase Transition in Vanadium Dioxide Driven by Hot-Electron Injection SO XVIIITH INTERNATIONAL CONFERENCE ON ULTRAFAST PHENOMENA SE EPJ Web of Conferences LA English DT Proceedings Paper CT 18th International Conference on Ultrafast Phenomena CY JUL 08-13, 2012 CL Ecole Polytechnique Fed Lausanne (EPFL), Lausanne, SWITZERLAND HO Ecole Polytechnique Fed Lausanne (EPFL) AB We present a novel all-optical method of triggering the phase transition in vanadium dioxide by means of ballistic electrons injected across the interface between a mesh of Au nanoparticles coveringd VO2 nanoislands. By performing non-degenerate pump-probe transmission spectroscopy on this hybrid plasmonic/phase-changing nanostructure, structural and electronic dynamics can be retrieved and compared. C1 [Appavoo, K.; Haglund, R. F., Jr.] Vanderbilt Univ, Interdisciplinary Mat Sci Program, 221 Kirkland Hall, Nashville, TN 37235 USA. [Brady, N. F.; Hilton, D. J.] Univ Alabama Birmingham, Dept Phys, Birmingham, AL 35924 USA. [Seo, M.; Prasankumar, R. P.] Los Alamos Natl Lab, Ctr Integrated Nanotechnol, Los Alamos, NM 87545 USA. [Nag, J.; Haglund, R. F., Jr.] Vanderbilt Univ, Dept Phys & Astron, Nashville, TN 37235 USA. RP Appavoo, K (reprint author), Vanderbilt Univ, Interdisciplinary Mat Sci Program, 221 Kirkland Hall, Nashville, TN 37235 USA. NR 6 TC 0 Z9 0 U1 0 U2 10 PU E D P SCIENCES PI CEDEX A PA 17 AVE DU HOGGAR PARC D ACTIVITES COUTABOEUF BP 112, F-91944 CEDEX A, FRANCE SN 2100-014X BN 978-2-7598-0956-1 J9 EPJ WEB CONF PY 2013 VL 41 AR UNSP 03026 DI 10.1051/epjconf/20134103026 PG 3 WC Physics, Multidisciplinary SC Physics GA BFM57 UT WOS:000320558600083 ER PT S AU Biggs, JD Zhang, Y Healion, D Govind, N Mukamel, S AF Biggs, Jason D. Zhang, Yu Healion, Daniel Govind, Niranjan Mukamel, Shaul BE Chergui, M Taylor, A Cundiff, S DeVivieRiedle, R Yamagouchi, K TI Dissecting X-Ray Raman Resonances Using Four-Wave Mixing SO XVIIITH INTERNATIONAL CONFERENCE ON ULTRAFAST PHENOMENA SE EPJ Web of Conferences LA English DT Proceedings Paper CT 18th International Conference on Ultrafast Phenomena CY JUL 08-13, 2012 CL Ecole Polytechnique Fed Lausanne (EPFL), Lausanne, SWITZERLAND HO Ecole Polytechnique Fed Lausanne (EPFL) AB The stimulated x-ray Raman signal has been calculated for the amino acid cysteine using broadband (FWHM similar or equal to 14.2eV, 128 as) pulses tuned to the nitrogen K-edge. Peaks correspond to those valence excited states and reveal electronic Frank-Condon overlaps between canonical valence orbitals and relaxed orbitals in the presence of the core hole. The coupling between excited states with valence- and core-holes is further explored using a coherent, wave-vector matched photon echo technique, where it is possible to eliminate stimulated emission and excited-state absorption by taking the waiting time to be longer the lifetime of the core hole (similar to 7.1 fs for nitrogen). C1 [Biggs, Jason D.; Zhang, Yu; Healion, Daniel; Mukamel, Shaul] Univ Calif Irvine, Dept Chem, Irvine, CA 92697 USA. [Govind, Niranjan] Pacific NW Natl Lab, Wiiliam R Wiley Environm Mol Sci Lab, Richland, WA 99352 USA. RP Biggs, JD (reprint author), Univ Calif Irvine, Dept Chem, Irvine, CA 92697 USA. EM mukamel@uci.edu NR 6 TC 0 Z9 0 U1 0 U2 3 PU E D P SCIENCES PI CEDEX A PA 17 AVE DU HOGGAR PARC D ACTIVITES COUTABOEUF BP 112, F-91944 CEDEX A, FRANCE SN 2100-014X BN 978-2-7598-0956-1 J9 EPJ WEB CONF PY 2013 VL 41 AR UNSP 05040 DI 10.1051/epjconf/20134105040 PG 3 WC Physics, Multidisciplinary SC Physics GA BFM57 UT WOS:000320558600160 ER PT S AU Brady, NF Appavoo, K Seo, M Nag, J Prasankumar, RP Haglund, RF Hilton, DJ AF Brady, N. F. Appavoo, K. Seo, M. Nag, J. Prasankumar, R. P. Haglund, R. F. Hilton, D. J. BE Chergui, M Taylor, A Cundiff, S DeVivieRiedle, R Yamagouchi, K TI Ultrafast Dynamics of the VO2 Insulator-to-Metal Transition Observed by Nondegenerate Pump-Probe Spectroscopy SO XVIIITH INTERNATIONAL CONFERENCE ON ULTRAFAST PHENOMENA SE EPJ Web of Conferences LA English DT Proceedings Paper CT 18th International Conference on Ultrafast Phenomena CY JUL 08-13, 2012 CL Ecole Polytechnique Fed Lausanne (EPFL), Lausanne, SWITZERLAND HO Ecole Polytechnique Fed Lausanne (EPFL) AB Non-degenerate pump (1.5 eV)-probe (0.4 eV) transmission spectroscopy on vanadium dioxide films grown on glass and three different sapphire substrates shows systematic variations with substrate that correlate with VO2 grain size and laser fluence. Temperature dependent measurements showed changes in the electronic response that is proportional to the metallic fraction. C1 [Brady, N. F.; Hilton, D. J.] Univ Alabama Birmingham, Birmingham, AL 35294 USA. [Appavoo, K.; Nag, J.; Haglund, R. F.] Vanderbilt Univ, Nashville, TN USA. [Seo, M.; Prasankumar, R. P.] Los Alamos Natl Lab, Ctr Integrated Nanotechnol, Los Alamos, NM 87545 USA. RP Brady, NF (reprint author), Univ Alabama Birmingham, Birmingham, AL 35294 USA. FU U.S. Department of Energy; Office of Basic Energy Sciences user facility at Los Alamos National Laboratory [DE-AC52-06NA25396]; Sandia National Laboratories [DE-AC04- 94AL85000]; US Dept. Education GAANN Fellowship [P200A090143]; Office of Science; U. S. Department of Energy [DE-FG02-01ER45916] FX This work was performed, in part, at the Center for Integrated Nanotechnologies, a U.S. Department of Energy, Office of Basic Energy Sciences user facility at Los Alamos National Laboratory (Contract DE-AC52-06NA25396) and Sandia National Laboratories (Contract DE-AC04- 94AL85000). NFB acknowledges support from the US Dept. Education GAANN Fellowship (P200A090143). KA, JN and RFH acknowledge support from the Office of Science, U. S. Department of Energy (DE-FG02-01ER45916). NR 6 TC 0 Z9 0 U1 1 U2 7 PU E D P SCIENCES PI CEDEX A PA 17 AVE DU HOGGAR PARC D ACTIVITES COUTABOEUF BP 112, F-91944 CEDEX A, FRANCE SN 2100-014X BN 978-2-7598-0956-1 J9 EPJ WEB CONF PY 2013 VL 41 AR UNSP 03006 DI 10.1051/epjconf/20134103006 PG 3 WC Physics, Multidisciplinary SC Physics GA BFM57 UT WOS:000320558600063 ER PT S AU Caviezel, A Staub, U Johnson, SL Mariager, SO Ingold, G Mohr-Vorobeva, E Garganourakis, M Huang, SW Milne, CJ Jia, QX Cheong, SW Beaud, P AF Caviezel, A. Staub, U. Johnson, S. L. Mariager, S. O. Ingold, G. Moehr-Vorobeva, E. Garganourakis, M. Huang, S. W. Milne, C. J. Jia, Q. X. Cheong, S. -W. Beaud, P. BE Chergui, M Taylor, A Cundiff, S DeVivieRiedle, R Yamagouchi, K TI Optical and x-ray time resolved study of the structural transition in mixed valence manganites SO XVIIITH INTERNATIONAL CONFERENCE ON ULTRAFAST PHENOMENA SE EPJ Web of Conferences LA English DT Proceedings Paper CT 18th International Conference on Ultrafast Phenomena CY JUL 08-13, 2012 CL Ecole Polytechnique Fed Lausanne (EPFL), Lausanne, SWITZERLAND HO Ecole Polytechnique Fed Lausanne (EPFL) ID PHASE AB Time resolved optical reflectivity and x-ray diffraction techniques are employed to study the laser-induced structural response in two charge and orbitally ordered manganites. Optical data indicate a non-thermal nature of the laser-triggered phase transition via the disappearance of an optical phonon related to the charge and orbitally ordered phase. The x-ray diffraction measurements on superlattice reflections confirm the non-thermal time scale of the initial step of this phase transition but also show that the complete change of structural symmetry is not instantaneous. C1 [Caviezel, A.; Staub, U.; Mariager, S. O.; Ingold, G.; Moehr-Vorobeva, E.; Garganourakis, M.; Huang, S. W.; Beaud, P.] Paul Scherrer Inst, Swiss Light Source, CH-5232 Villigen, Switzerland. [Johnson, S. L.] ETH, Inst Quantum Elect, Dept Phys, CH-8093 Zurich, Switzerland. [Milne, C. J.] Ecole Polytech Fed Lausanne, Lab Spectroscopie Ultrarapide, CH-1015 Lausanne, Switzerland. [Jia, Q. X.] LANL, Ctr Integrated Nanotechnol, Los Alamos, NM 87545 USA. [Cheong, S. -W.] Rutgers State Univ, Rutgers Ctr Emergent Mat, Piscataway, NJ 08854 USA. RP Caviezel, A (reprint author), Paul Scherrer Inst, Swiss Light Source, CH-5232 Villigen, Switzerland. RI Johnson, Steven/B-3252-2008; Beaud, Paul/A-8178-2008; Milne, Christopher/C-6883-2008; Staub, Urs/C-4914-2015 OI Johnson, Steven/0000-0001-6074-4894; Beaud, Paul/0000-0001-5028-9138; Milne, Christopher/0000-0003-4714-9139; NR 12 TC 0 Z9 0 U1 0 U2 22 PU E D P SCIENCES PI CEDEX A PA 17 AVE DU HOGGAR PARC D ACTIVITES COUTABOEUF BP 112, F-91944 CEDEX A, FRANCE SN 2100-014X BN 978-2-7598-0956-1 J9 EPJ WEB CONF PY 2013 VL 41 AR UNSP 03002 DI 10.1051/epjconf/20134103002 PG 3 WC Physics, Multidisciplinary SC Physics GA BFM57 UT WOS:000320558600059 ER PT S AU Coslovich, G Huber, B Lee, WS Chuang, YD Zhu, Y Sasagawa, T Hussain, Z Bechtel, HA Martin, MC Schoenlein, RW Shen, ZX Kaindl, RA AF Coslovich, G. Huber, B. Lee, W. -S. Chuang, Y. -D. Zhu, Y. Sasagawa, T. Hussain, Z. Bechtel, H. A. Martin, M. C. Schoenlein, R. W. Shen, Z. -X. Kaindl, R. A. BE Chergui, M Taylor, A Cundiff, S DeVivieRiedle, R Yamagouchi, K TI Ultrast Mid-infrared Spectroscopy of the Charge- and Spin-Ordered Nickelate La1.75Sr0.25NiO4 SO XVIIITH INTERNATIONAL CONFERENCE ON ULTRAFAST PHENOMENA SE EPJ Web of Conferences LA English DT Proceedings Paper CT 18th International Conference on Ultrafast Phenomena CY JUL 08-13, 2012 CL Ecole Polytechnique Fed Lausanne (EPFL), Lausanne, SWITZERLAND HO Ecole Polytechnique Fed Lausanne (EPFL) AB We present the first ultrafast mid-infrared study of charge and spin-ordered nickelates. A sub-picosecond modulation of the optical reflectivity is observed, indicating the filling and subsequent re-establishment of the pseudogap in the time-domain. C1 [Coslovich, G.; Huber, B.; Zhu, Y.; Schoenlein, R. W.; Kaindl, R. A.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. [Lee, W. -S.; Shen, Z. -X.] Stanford Univ, SLAC Natl Accelerator Lab, SIMES, Menlo Pk, CA 94025 USA. [Chuang, Y. -D.; Hussain, Z.; Bechtel, H. A.; Martin, M. C.] Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. [Sasagawa, T.] Tokyo Inst Technol, Mat & Struct Lab, Kanagawa 2268503, Japan. RP Coslovich, G (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. EM GCoslovich@lbl.gov RI Schoenlein, Robert/D-1301-2014; Sasagawa, Takao/E-6666-2014 OI Schoenlein, Robert/0000-0002-6066-7566; Sasagawa, Takao/0000-0003-0149-6696 NR 10 TC 0 Z9 0 U1 0 U2 0 PU E D P SCIENCES PI CEDEX A PA 17 AVE DU HOGGAR PARC D ACTIVITES COUTABOEUF BP 112, F-91944 CEDEX A, FRANCE SN 2100-014X BN 978-2-7598-0956-1 J9 EPJ WEB CONF PY 2013 VL 41 AR UNSP 03016 DI 10.1051/epjconf/20134103016 PG 3 WC Physics, Multidisciplinary SC Physics GA BFM57 UT WOS:000320558600073 ER PT S AU De Re, E Schlau-Cohen, GS Huxter, VM Leverenz, RL Mathies, RA Fleming, GR AF De Re, E. Schlau-Cohen, G. S. Huxter, V. M. Leverenz, R. L. Mathies, R. A. Fleming, G. R. BE Chergui, M Taylor, A Cundiff, S DeVivieRiedle, R Yamagouchi, K TI Comparing the photophysics of the two forms of the Orange Carotenoid Protein using 2D electronic spectroscopy SO XVIIITH INTERNATIONAL CONFERENCE ON ULTRAFAST PHENOMENA SE EPJ Web of Conferences LA English DT Proceedings Paper CT 18th International Conference on Ultrafast Phenomena CY JUL 08-13, 2012 CL Ecole Polytechnique Fed Lausanne (EPFL), Lausanne, SWITZERLAND HO Ecole Polytechnique Fed Lausanne (EPFL) ID CYANOBACTERIA AB Broadband two-dimensional electronic spectroscopy is applied to investigate the photophysics of the photoactive orange carotenoid protein, which is involved in nonphotochemical quenching in cyanobacteria. Differences in dynamics between the light and dark forms arise from the different structure of the carotenoid in the protein pocket, with consequences for the biological role of the two forms. C1 [De Re, E.; Fleming, G. R.] Univ Calif Berkeley, Appl Sci & Technol Grad Grp, Berkeley, CA 94720 USA. [Schlau-Cohen, G. S.; Huxter, V. M.; Leverenz, R. L.; Mathies, R. A.; Fleming, G. R.] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [De Re, E.; Schlau-Cohen, G. S.; Huxter, V. M.; Fleming, G. R.] Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA 94720 USA. RP De Re, E (reprint author), Univ Calif Berkeley, Appl Sci & Technol Grad Grp, Berkeley, CA 94720 USA. FU Office of Science; Office of Basic Energy Sciences; U.S. Department of Energy [DE-AC02-05CH11231, DE-AC03-76SF000098]; Division of Chemical Sciences, Geosciences, and Biosciences FX This work was supported by the Director, Office of Science, and Office of Basic Energy Sciences of the U.S. Department of Energy under contract DE-AC02-05CH11231 and by the Division of Chemical Sciences, Geosciences, and Biosciences and Office of Basic Energy Sciences of the U.S. Department of Energy through grant DE-AC03-76SF000098. NR 7 TC 1 Z9 1 U1 0 U2 8 PU E D P SCIENCES PI CEDEX A PA 17 AVE DU HOGGAR PARC D ACTIVITES COUTABOEUF BP 112, F-91944 CEDEX A, FRANCE SN 2100-014X BN 978-2-7598-0956-1 J9 EPJ WEB CONF PY 2013 VL 41 AR UNSP 08008 DI 10.1051/epjconf/20134108008 PG 3 WC Physics, Multidisciplinary SC Physics GA BFM57 UT WOS:000320558600205 ER PT S AU Guggenmos, A Hofstetter, M Rauhut, R Spath, C Hertrich, S Nickel, B Yang, S Gullikson, EM Schmidt, J Seibald, M Schnick, W Krausz, F Kleineberg, U AF Guggenmos, A. Hofstetter, M. Rauhut, R. Spaeth, C. Hertrich, S. Nickel, B. Yang, S. Gullikson, E. M. Schmidt, J. Seibald, M. Schnick, W. Krausz, F. Kleineberg, U. BE Chergui, M Taylor, A Cundiff, S DeVivieRiedle, R Yamagouchi, K TI Broadband multilayer mirror and diffractive optics for attosecond pulse shaping in the 280-500 eV photon energy range SO XVIIITH INTERNATIONAL CONFERENCE ON ULTRAFAST PHENOMENA SE EPJ Web of Conferences LA English DT Proceedings Paper CT 18th International Conference on Ultrafast Phenomena CY JUL 08-13, 2012 CL Ecole Polytechnique Fed Lausanne (EPFL), Lausanne, SWITZERLAND HO Ecole Polytechnique Fed Lausanne (EPFL) AB Chirped broadband multilayer mirrors are key components to shape attosecond pulses in the XUV range. Compressing high harmonic pulses to their Fourier limit is the major goal for attosecond physics utilizing short pulse pump-probe experiments. Here, we report about the first implementation of multilayers and diffractive optics fulfilling these requirements in the "water-window" spectral range. C1 [Guggenmos, A.; Hofstetter, M.; Rauhut, R.; Spaeth, C.; Schmidt, J.; Krausz, F.; Kleineberg, U.] Univ Munich, Fak Phys, Coulombwall 1, Garching, Germany. [Guggenmos, A.; Hofstetter, M.; Krausz, F.; Kleineberg, U.] Max Plank Inst Quantenoptik, Garching, Germany. [Hertrich, S.; Nickel, B.] Ludwig Maximilians Univ Munchen, Ctr Nanosci, Munich, Germany. [Yang, S.; Gullikson, E. M.] Lawrence Berkeley Natl Lab, Ctr Xray Opt, Berkeley, CA 94720 USA. [Seibald, M.; Schnick, W.] Ludwing Maximilians Univ Munchen, Fak Chem, Munich, Germany. RP Guggenmos, A (reprint author), Univ Munich, Fak Phys, Coulombwall 1, Garching, Germany. RI Nickel, Bert/A-2095-2009 OI Nickel, Bert/0000-0002-0254-8841 NR 6 TC 0 Z9 0 U1 1 U2 9 PU E D P SCIENCES PI CEDEX A PA 17 AVE DU HOGGAR PARC D ACTIVITES COUTABOEUF BP 112, F-91944 CEDEX A, FRANCE SN 2100-014X BN 978-2-7598-0956-1 J9 EPJ WEB CONF PY 2013 VL 41 AR UNSP 01011 DI 10.1051/epjconf/20134101011 PG 3 WC Physics, Multidisciplinary SC Physics GA BFM57 UT WOS:000320558600011 ER PT S AU Huse, N Van Kuiken, BE Cho, H Strader, ML Kim, TK Khalil, M Schoenlein, RW AF Huse, Nils Van Kuiken, Benjamin E. Cho, Hana Strader, Matthew L. Kim, Tae Kyu Khalil, Munira Schoenlein, Robert W. BE Chergui, M Taylor, A Cundiff, S DeVivieRiedle, R Yamagouchi, K TI Elucidating Charge Delocalization in the High-Spin State of aqueous Fe-II Spin-Crossover Compounds via Time-Resolved Spectroscopy in the X-ray Water Window SO XVIIITH INTERNATIONAL CONFERENCE ON ULTRAFAST PHENOMENA SE EPJ Web of Conferences LA English DT Proceedings Paper CT 18th International Conference on Ultrafast Phenomena CY JUL 08-13, 2012 CL Ecole Polytechnique Fed Lausanne (EPFL), Lausanne, SWITZERLAND HO Ecole Polytechnique Fed Lausanne (EPFL) ID COMPLEXES; DYNAMICS AB We report the first time-resolved spectroscopy of aqueous solution in the X-ray water window. Nitrogen K-edge spectra, combined with ab initio calculations, reveal distinct charge delocalization, shedding light on the origins of ultrafast spin crossover. C1 [Huse, Nils] Univ Hamburg, Max Planck Res Dept Struct Dynam, D-22607 Hamburg, Germany. [Huse, Nils; Cho, Hana; Strader, Matthew L.; Schoenlein, Robert W.] Lawrence Berkeley Natl Lab, Div Chem Sci, Ultra Xray sci Lab, Berkeley, CA 94720 USA. [Van Kuiken, Benjamin E.; Khalil, Munira] Univ Washington, Dept Chem, Seattle, WA 98195 USA. [Cho, Hana; Kim, Tae Kyu] Pusan Natl Univ, Dept Chem, Pusan 609735, South Korea. RP Huse, N (reprint author), Univ Hamburg, Max Planck Res Dept Struct Dynam, D-22607 Hamburg, Germany. EM nils.huse@mpsd.cfel.de RI Schoenlein, Robert/D-1301-2014 OI Schoenlein, Robert/0000-0002-6066-7566 NR 9 TC 0 Z9 0 U1 0 U2 5 PU E D P SCIENCES PI CEDEX A PA 17 AVE DU HOGGAR PARC D ACTIVITES COUTABOEUF BP 112, F-91944 CEDEX A, FRANCE SN 2100-014X BN 978-2-7598-0956-1 J9 EPJ WEB CONF PY 2013 VL 41 AR UNSP 05037 DI 10.1051/epjconf/20134105037 PG 3 WC Physics, Multidisciplinary SC Physics GA BFM57 UT WOS:000320558600157 ER PT S AU Huxter, VM Oliver, TAA Budker, D Fleming, GR AF Huxter, V. M. Oliver, T. A. A. Budker, D. Fleming, G. R. BE Chergui, M Taylor, A Cundiff, S DeVivieRiedle, R Yamagouchi, K TI Vibrational and electronic ultrafast relaxation of the nitrogen-vacancy centers in diamond SO XVIIITH INTERNATIONAL CONFERENCE ON ULTRAFAST PHENOMENA SE EPJ Web of Conferences LA English DT Proceedings Paper CT 18th International Conference on Ultrafast Phenomena CY JUL 08-13, 2012 CL Ecole Polytechnique Fed Lausanne (EPFL), Lausanne, SWITZERLAND HO Ecole Polytechnique Fed Lausanne (EPFL) ID DYNAMICS; SPIN AB Two dimensional electronic spectroscopy and transient grating measurements were performed, for the first time, on nitrogen-vacancy centers in diamond. These measurements reveal energy transfer and vibrational pathways with consequences for spin coherence. C1 [Huxter, V. M.; Oliver, T. A. A.; Fleming, G. R.] Univ Calif Berkeley, Dept Chem, Berkeley & Phys Biosci Div, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Budker, D.] Univ Calif Berkeley, Dept Phys, Berkeley & Nucl Sci Div, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Huxter, VM (reprint author), Univ Calif Berkeley, Dept Chem, Berkeley & Phys Biosci Div, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RI Budker, Dmitry/F-7580-2016 OI Budker, Dmitry/0000-0002-7356-4814 FU National Science and Engineering Research Council of Canada for a postdoctoral fellowship; NSF [CHE-1012168]; IMOD; AFOSR/DARPA QuASAR program FX The authors thank Adam Gali for suggesting ultrafast measurements with NV-diamond and Andrey Jarmola for preparing the NV-diamond sample. V.M.H. thanks the National Science and Engineering Research Council of Canada for a postdoctoral fellowship. D.B. was supported by NSF, IMOD, and the AFOSR/DARPA QuASAR program. The work by V.M.H., T.A.A.O. and G.R.F. was supported by NSF grant CHE-1012168. NR 9 TC 0 Z9 0 U1 1 U2 9 PU E D P SCIENCES PI CEDEX A PA 17 AVE DU HOGGAR PARC D ACTIVITES COUTABOEUF BP 112, F-91944 CEDEX A, FRANCE SN 2100-014X BN 978-2-7598-0956-1 J9 EPJ WEB CONF PY 2013 VL 41 AR UNSP 04009 DI 10.1051/epjconf/20134104009 PG 3 WC Physics, Multidisciplinary SC Physics GA BFM57 UT WOS:000320558600092 ER PT S AU Koralek, JD Yang, L Tibbetts, DR Reno, JL Lilly, MP Orenstein, J AF Koralek, J. D. Yang, L. Tibbetts, D. R. Reno, J. L. Lilly, M. P. Orenstein, J. BE Chergui, M Taylor, A Cundiff, S DeVivieRiedle, R Yamagouchi, K TI Doppler velocimetry of spin and charge currents in the 2D Fermi gas SO XVIIITH INTERNATIONAL CONFERENCE ON ULTRAFAST PHENOMENA SE EPJ Web of Conferences LA English DT Proceedings Paper CT 18th International Conference on Ultrafast Phenomena CY JUL 08-13, 2012 CL Ecole Polytechnique Fed Lausanne (EPFL), Lausanne, SWITZERLAND HO Ecole Polytechnique Fed Lausanne (EPFL) ID 2-DIMENSIONAL ELECTRON-GAS AB Phase-sensitive transient grating spectroscopy was used to measure the Doppler shift of light diffracted off moving spin and charge density waves, allowing complete characterization of spin and charge transport in the 2D Fermi gas. C1 [Koralek, J. D.; Yang, L.; Orenstein, J.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. [Yang, L.; Orenstein, J.] Univ Calif Berkeley, Dept Phys, Berkeley, CA 94720 USA. [Tibbetts, D. R.; Reno, J. L.; Lilly, M. P.] Sandia Natl Labs, Albuquerque, NM 87123 USA. RP Koralek, JD (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. RI Orenstein, Joseph/I-3451-2015 NR 5 TC 0 Z9 0 U1 0 U2 5 PU E D P SCIENCES PI CEDEX A PA 17 AVE DU HOGGAR PARC D ACTIVITES COUTABOEUF BP 112, F-91944 CEDEX A, FRANCE SN 2100-014X BN 978-2-7598-0956-1 J9 EPJ WEB CONF PY 2013 VL 41 AR UNSP 03017 DI 10.1051/epjconf/20134103017 PG 2 WC Physics, Multidisciplinary SC Physics GA BFM57 UT WOS:000320558600074 ER PT S AU Lawrie, BJ Mu, R Haglund, RF AF Lawrie, B. J. Mu, R. Haglund, R. F., Jr. BE Chergui, M Taylor, A Cundiff, S DeVivieRiedle, R Yamagouchi, K TI Ultrafast Surface-Plasmon Enhancement of Exciton and Defect Luminescence in ZnO Thin Films SO XVIIITH INTERNATIONAL CONFERENCE ON ULTRAFAST PHENOMENA SE EPJ Web of Conferences LA English DT Proceedings Paper CT 18th International Conference on Ultrafast Phenomena CY JUL 08-13, 2012 CL Ecole Polytechnique Fed Lausanne (EPFL), Lausanne, SWITZERLAND HO Ecole Polytechnique Fed Lausanne (EPFL) AB Femtosecond pump-probe and photoluminescence measurements in transmission and reflection show that ultraviolet band-edge and visible defect luminescence in ZnO films can be selectively enhanced by coupling to Ag surface-plasmon polaritons or localized surface plasmon resonances. C1 [Lawrie, B. J.] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. RP Lawrie, BJ (reprint author), Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. RI Lawrie, Benjamin/B-7182-2016 OI Lawrie, Benjamin/0000-0003-1431-066X NR 5 TC 0 Z9 0 U1 0 U2 14 PU E D P SCIENCES PI CEDEX A PA 17 AVE DU HOGGAR PARC D ACTIVITES COUTABOEUF BP 112, F-91944 CEDEX A, FRANCE SN 2100-014X BN 978-2-7598-0956-1 J9 EPJ WEB CONF PY 2013 VL 41 AR UNSP 04016 DI 10.1051/epjconf/20134104016 PG 3 WC Physics, Multidisciplinary SC Physics GA BFM57 UT WOS:000320558600099 ER PT S AU Li, T Patz, A Yan, J Lograsso, TA Perakis, IE Wang, J AF Li, T. Patz, A. Yan, J. Lograsso, T. A. Perakis, I. E. Wang, J. BE Chergui, M Taylor, A Cundiff, S DeVivieRiedle, R Yamagouchi, K TI Photoinduced femtosecond formation of ferromagnetism in a strongly correlated antiferromagentic manganite SO XVIIITH INTERNATIONAL CONFERENCE ON ULTRAFAST PHENOMENA SE EPJ Web of Conferences LA English DT Proceedings Paper CT 18th International Conference on Ultrafast Phenomena CY JUL 08-13, 2012 CL Ecole Polytechnique Fed Lausanne (EPFL), Lausanne, SWITZERLAND HO Ecole Polytechnique Fed Lausanne (EPFL) ID PULSES AB We report a pump threshold behavior in fs photoinduced magnetization in a strongly correlated manganite, which indicates the establishment of thermally-inaccessible ferromagnetic ground state and build-up of new magnetic order parameters at fs time scales. C1 [Li, T.; Patz, A.; Yan, J.; Lograsso, T. A.; Wang, J.] Iowa State Univ, Dept Phys & Astron, Ames, IA 50011 USA. [Li, T.; Patz, A.; Wang, J.] Ames Lab, USDOE, Ames, IA USA. [Perakis, I. E.] Univ Crete, Dept Phys, Iraklion, Greece. RP Li, T (reprint author), Iowa State Univ, Dept Phys & Astron, Ames, IA 50011 USA. RI Li, Tianqi/C-5142-2014 OI Li, Tianqi/0000-0002-5238-8540 FU National Science Foundation [DMR-1055352]; U.S. Department of Energy-Basic Energy Sciences [DE-AC02-7CH11358] FX This work was also supported by the National Science Foundation Contract No. DMR-1055352. Material synthesis at the Ames Laboratory was supported by the U.S. Department of Energy-Basic Energy Sciences under Contract No. DE-AC02-7CH11358 NR 8 TC 0 Z9 0 U1 0 U2 3 PU E D P SCIENCES PI CEDEX A PA 17 AVE DU HOGGAR PARC D ACTIVITES COUTABOEUF BP 112, F-91944 CEDEX A, FRANCE SN 2100-014X BN 978-2-7598-0956-1 J9 EPJ WEB CONF PY 2013 VL 41 AR UNSP 03004 DI 10.1051/epjconf/20134103004 PG 3 WC Physics, Multidisciplinary SC Physics GA BFM57 UT WOS:000320558600061 ER PT S AU Patz, A Li, T Ran, S Bud'ko, S Canfield, P Wang, J AF Patz, A. Li, T. Ran, S. Bud'ko, S. Canfield, P. Wang, J. BE Chergui, M Taylor, A Cundiff, S DeVivieRiedle, R Yamagouchi, K TI Photoinduced femtosecond relaxation of antiferromagnetic orders in the iron pnictides revealed by ultrafast laser ellipsometry SO XVIIITH INTERNATIONAL CONFERENCE ON ULTRAFAST PHENOMENA SE EPJ Web of Conferences LA English DT Proceedings Paper CT 18th International Conference on Ultrafast Phenomena CY JUL 08-13, 2012 CL Ecole Polytechnique Fed Lausanne (EPFL), Lausanne, SWITZERLAND HO Ecole Polytechnique Fed Lausanne (EPFL) AB We report ultrafast softening of the antiferromagnetic order, similar to 150fs after the electron thermalization, which follows a two-step recovery pathway to reveal a distinct interplay of magnetism and the nematic order in iron pnictides. C1 [Patz, A.; Li, T.; Ran, S.; Bud'ko, S.; Canfield, P.; Wang, J.] Iowa State Univ, Ames Lab, Ames, IA 50011 USA. RP Patz, A (reprint author), Iowa State Univ, Ames Lab, Ames, IA 50011 USA. RI Li, Tianqi/C-5142-2014 OI Li, Tianqi/0000-0002-5238-8540 NR 3 TC 0 Z9 0 U1 1 U2 5 PU E D P SCIENCES PI CEDEX A PA 17 AVE DU HOGGAR PARC D ACTIVITES COUTABOEUF BP 112, F-91944 CEDEX A, FRANCE SN 2100-014X BN 978-2-7598-0956-1 J9 EPJ WEB CONF PY 2013 VL 41 AR UNSP 03011 DI 10.1051/epjconf/20134103011 PG 3 WC Physics, Multidisciplinary SC Physics GA BFM57 UT WOS:000320558600068 ER PT S AU Perkins, BG Hwang, HY Grady, NK Yan, L Trugman, D Jia, Q Chen, HT Taylor, AJ Nelson, KA AF Perkins, B. G., Jr. Hwang, H. Y. Grady, N. K. Yan, L. Trugman, D. Jia, Q. Chen, H. T. Taylor, A. J. Nelson, K. A. BE Chergui, M Taylor, A Cundiff, S DeVivieRiedle, R Yamagouchi, K TI Nonlinear ultrafast dynamics of high temperature YBa2Cu3O7-delta superconductors probed with THz pump / THz probe spectroscopy SO XVIIITH INTERNATIONAL CONFERENCE ON ULTRAFAST PHENOMENA SE EPJ Web of Conferences LA English DT Proceedings Paper CT 18th International Conference on Ultrafast Phenomena CY JUL 08-13, 2012 CL Ecole Polytechnique Fed Lausanne (EPFL), Lausanne, SWITZERLAND HO Ecole Polytechnique Fed Lausanne (EPFL) ID QUASI-PARTICLE DYNAMICS AB High power THz pulses induce near transparency in superconductive YBCO thin films below the critical temperature. THz pump/THz probe measurements reveal a decay of the induced transparency on the time scale of a few picoseconds. C1 [Perkins, B. G., Jr.; Hwang, H. Y.; Nelson, K. A.] MIT, Dept Chem, Cambridge, MA 02139 USA. [Grady, N. K.; Yan, L.; Trugman, D.; Jia, Q.; Chen, H. T.; Taylor, A. J.] Los Alamos Natl Lab, Ctr Integrated Nanotechnol, Los Alamos, NM 87545 USA. RP Perkins, BG (reprint author), MIT, Dept Chem, Cambridge, MA 02139 USA. OI Chen, Hou-Tong/0000-0003-2014-7571 FU ONR [N00014-09-1-1103]; NSF American Competitiveness in Chemistry Fellowship [1041979]; LANL/LDRD program; Center for Integrated Nanotechnologies; U.S. Department of Energy; Office of Basic Energy Sciences; Los Alamos National Security; LLC; National Nuclear Security Administration of the U.S. Department of Energy [DE-AC52-06NA25396] FX Funding for this work is provided by ONR grant N00014-09-1-1103 and NSF American Competitiveness in Chemistry Fellowship 1041979. We acknowledge partial support from LANL/LDRD program. Additionally, this work was performed, in part, at the Center for Integrated Nanotechnologies, a U.S. Department of Energy, Office of Basic Energy Sciences user facility. Los Alamos National Laboratory, an affirmative action equal opportunity employer, is operated by Los Alamos National Security, LLC, for the National Nuclear Security Administration of the U.S. Department of Energy under contract DE-AC52-06NA25396. NR 8 TC 0 Z9 0 U1 0 U2 4 PU E D P SCIENCES PI CEDEX A PA 17 AVE DU HOGGAR PARC D ACTIVITES COUTABOEUF BP 112, F-91944 CEDEX A, FRANCE SN 2100-014X BN 978-2-7598-0956-1 J9 EPJ WEB CONF PY 2013 VL 41 AR UNSP 03010 DI 10.1051/epjconf/20134103010 PG 3 WC Physics, Multidisciplinary SC Physics GA BFM57 UT WOS:000320558600067 ER PT S AU Seo, MA Yoo, J Perea, DE Dayeh, SA Picraux, ST Taylor, AJ Prasankumar, RP AF Seo, M. A. Yoo, J. Perea, D. E. Dayeh, S. A. Picraux, S. T. Taylor, A. J. Prasankumar, R. P. BE Chergui, M Taylor, A Cundiff, S DeVivieRiedle, R Yamagouchi, K TI Tracking Ultrafast Carrier Dynamics in Single Semiconductor Nanowire Heterostructures SO XVIIITH INTERNATIONAL CONFERENCE ON ULTRAFAST PHENOMENA SE EPJ Web of Conferences LA English DT Proceedings Paper CT 18th International Conference on Ultrafast Phenomena CY JUL 08-13, 2012 CL Ecole Polytechnique Fed Lausanne (EPFL), Lausanne, SWITZERLAND HO Ecole Polytechnique Fed Lausanne (EPFL) AB An understanding of non-equilibrium carrier dynamics in silicon (Si) nanowires (NWs) and NW heterostructures is very important due to their many nanophotonic and nanoelectronics applications. Here, we describe the first measurements of ultrafast carrier dynamics and diffusion in single heterostructured Si nanowires, obtained using ultrafast optical microscopy. By isolating individual nanowires, we avoid complications resulting from the broad size and alignment distribution in nanowire ensembles, allowing us to directly probe ultrafast carrier dynamics in these quasi-one-dimensional systems. Spatially-resolved pump-probe spectroscopy demonstrates the influence of surface-mediated mechanisms on carrier dynamics in a single NW, while polarization-resolved femtosecond pump-probe spectroscopy reveals a clear anisotropy in carrier lifetimes measured parallel and perpendicular to the NW axis, due to density-dependent Auger recombination. Furthermore, separating the pump and probe spots along the NW axis enabled us to track space and time dependent carrier diffusion in radial and axial NW heterostructures. These results enable us to reveal the influence of radial and axial interfaces on carrier dynamics and charge transport in these quasi-one-dimensional nanosystems, which can then be used to tailor carrier relaxation in a single nanowire heterostructure for a given application. C1 [Seo, M. A.; Yoo, J.; Perea, D. E.; Dayeh, S. A.; Picraux, S. T.; Taylor, A. J.; Prasankumar, R. P.] Los Alamos Natl Lab, Ctr Integrated Nanotechnol, Los Alamos, NM 87545 USA. RP Seo, MA (reprint author), Los Alamos Natl Lab, Ctr Integrated Nanotechnol, POB 1663, Los Alamos, NM 87545 USA. NR 5 TC 0 Z9 0 U1 2 U2 9 PU E D P SCIENCES PI CEDEX A PA 17 AVE DU HOGGAR PARC D ACTIVITES COUTABOEUF BP 112, F-91944 CEDEX A, FRANCE SN 2100-014X BN 978-2-7598-0956-1 J9 EPJ WEB CONF PY 2013 VL 41 AR UNSP 04030 DI 10.1051/epjconf/20134104030 PG 3 WC Physics, Multidisciplinary SC Physics GA BFM57 UT WOS:000320558600113 ER PT S AU Sheu, YM Trugman, SA Xiong, J Park, YS Lee, S Yi, HT Cheong, SW Jia, QX Taylor, AJ Prasankumar, RP AF Sheu, Y. M. Trugman, S. A. Xiong, J. Park, Y. -S. Lee, S. Yi, H. T. Cheong, S. -W. Jia, Q. X. Taylor, A. J. Prasankumar, R. P. BE Chergui, M Taylor, A Cundiff, S DeVivieRiedle, R Yamagouchi, K TI Ultrafast carrier dynamics and radiative recombination in multiferroic BiFeO3 single crystals and thin films SO XVIIITH INTERNATIONAL CONFERENCE ON ULTRAFAST PHENOMENA SE EPJ Web of Conferences LA English DT Proceedings Paper CT 18th International Conference on Ultrafast Phenomena CY JUL 08-13, 2012 CL Ecole Polytechnique Fed Lausanne (EPFL), Lausanne, SWITZERLAND HO Ecole Polytechnique Fed Lausanne (EPFL) AB We report a detailed comparison of ultrafast carrier dynamics in single crystals and thin films of multiferroic BiFeO3 (BFO). Using degenerate femtosecond optical pump-probe spectroscopy, we find that the observed dynamics are qualitatively similar in both samples. After photoexcitation, electrons relax to the conduction band minimum through electron-phonon coupling, with subsequent carrier relaxation proceeding via various recombination pathways that extend to a nanosecond timescale. Subtle differences observed in our measurements indicate that BFO films have a higher band gap than single crystals. Overall, our results demonstrate that carrier relaxation in BFO is analogous to that in bulk semiconductors. C1 [Sheu, Y. M.; Trugman, S. A.; Xiong, J.; Park, Y. -S.; Jia, Q. X.; Taylor, A. J.; Prasankumar, R. P.] Los Alamos Natl Lab, Ctr Integrated Nanotechnol, MS K771, Los Alamos, NM 87545 USA. [Lee, S.] Korea Atom Energy Res Inst, Taejon 305353, South Korea. [Yi, H. T.; Cheong, S. -W.] Rutgers State Univ, Rutgers Ctr Emergent Mat, Dept Phys & Astron, Piscataway, NJ 08854 USA. RP Sheu, YM (reprint author), Los Alamos Natl Lab, Ctr Integrated Nanotechnol, MS K771, Los Alamos, NM 87545 USA. OI Trugman, Stuart/0000-0002-6688-7228 NR 7 TC 0 Z9 0 U1 1 U2 18 PU E D P SCIENCES PI CEDEX A PA 17 AVE DU HOGGAR PARC D ACTIVITES COUTABOEUF BP 112, F-91944 CEDEX A, FRANCE SN 2100-014X BN 978-2-7598-0956-1 J9 EPJ WEB CONF PY 2013 VL 41 AR UNSP 03018 DI 10.1051/epjconf/20134103018 PG 3 WC Physics, Multidisciplinary SC Physics GA BFM57 UT WOS:000320558600075 ER PT S AU Tobey, RI Wall, S Forst, M Bromberger, H Khanna, V Turner, JJ Schlotter, W Trigo, M Krupin, O Lee, WS Chuang, YD Moore, R Cavalieri, AL Wilkins, SB Zeng, H Mitchell, JF Dhesi, SS Cavalleri, A Hill, JP AF Tobey, R. I. Wall, S. Foerst, M. Bromberger, H. Khanna, V. Turner, J. J. Schlotter, W. Trigo, M. Krupin, O. Lee, W. S. Chuang, Y. -D. Moore, R. Cavalieri, A. L. Wilkins, S. B. Zeng, H. Mitchell, J. F. Dhesi, S. S. Cavalleri, A. Hill, J. P. BE Chergui, M Taylor, A Cundiff, S DeVivieRiedle, R Yamagouchi, K TI Measuring 3D magnetic correlations during the photo-induced melting of electronic order in La0.5Sr1.5MnO4 SO XVIIITH INTERNATIONAL CONFERENCE ON ULTRAFAST PHENOMENA SE EPJ Web of Conferences LA English DT Proceedings Paper CT 18th International Conference on Ultrafast Phenomena CY JUL 08-13, 2012 CL Ecole Polytechnique Fed Lausanne (EPFL), Lausanne, SWITZERLAND HO Ecole Polytechnique Fed Lausanne (EPFL) AB Time-resolved x-ray diffraction measures the dynamics of antiferromagnetic correlations by reconstructing the reciprocal-space scattering volume for the magnetic Bragg peak. Modifications in the scattering line shape along the three principal reciprocal lattice directions are measured. C1 [Tobey, R. I.] Univ Groningen, Zernike Inst Adv Mat, NL-9747 AG Groningen, Netherlands. [Tobey, R. I.; Wilkins, S. B.; Hill, J. P.] Brookhaven Natl Lab, Condensed Matter Phys & Mat Sci, Upton, NY 11973 USA. [Wall, S.] Max Planck Gesell, Fritz Haber Inst, Berlin, Germany. [Foerst, M.; Bromberger, H.; Khanna, V.; Cavalieri, A. L.] Univ Hamburg, Ctr Free Electron Laser Sci, Max Planck Dept Struct Dynam, Hamburg, Germany. [Khanna, V.; Dhesi, S. S.] Diamond Light Source, Oxford OX11 0DE, England. [Khanna, V.; Cavalleri, A.] Univ Oxford, Dept Phys, Clarendon Lab, Oxford OX1 2JD, England. [Turner, J. J.; Schlotter, W.; Krupin, O.] SLAC Natl Accelerator Lab, PULSE Inst, Menlo Pk, CA 94025 USA. [Trigo, M.] SLAC Natl Accelerator Lab, PULSE Inst, Menlo Pk, CA 94025 USA. [Krupin, O.] European XFEL GmbH, Hamburg, Germany. [Lee, W. S.; Moore, R.] SLAC Natl Accelerator Lab, SIMES, Menlo Pk, CA 94025 USA. [Chuang, Y. -D.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Zeng, H.; Mitchell, J. F.] Argonne Natl Lab, Dept Mat Sci, Argonne, IL 69439 USA. RP Tobey, RI (reprint author), Univ Groningen, Zernike Inst Adv Mat, NL-9747 AG Groningen, Netherlands. OI Wall, Simon/0000-0002-6136-0224 NR 5 TC 0 Z9 0 U1 0 U2 9 PU E D P SCIENCES PI CEDEX A PA 17 AVE DU HOGGAR PARC D ACTIVITES COUTABOEUF BP 112, F-91944 CEDEX A, FRANCE SN 2100-014X BN 978-2-7598-0956-1 J9 EPJ WEB CONF PY 2013 VL 41 AR UNSP 03003 DI 10.1051/epjconf/20134103003 PG 3 WC Physics, Multidisciplinary SC Physics GA BFM57 UT WOS:000320558600060 ER PT S AU Zaks, J Sun, J Kirmayer, S Urban, JJ Tilley, TD Segalman, RA Fleming, GR AF Zaks, J. Sun, J. Kirmayer, S. Urban, J. J. Tilley, T. D. Segalman, R. A. Fleming, G. R. BE Chergui, M Taylor, A Cundiff, S DeVivieRiedle, R Yamagouchi, K TI Effect of bridge on energy transfer and photoinduced charge sepration in perylene-diimide-naphthalene-bisimide-hexathiophene based donor-bridge-acceptor triads SO XVIIITH INTERNATIONAL CONFERENCE ON ULTRAFAST PHENOMENA SE EPJ Web of Conferences LA English DT Proceedings Paper CT 18th International Conference on Ultrafast Phenomena CY JUL 08-13, 2012 CL Ecole Polytechnique Fed Lausanne (EPFL), Lausanne, SWITZERLAND HO Ecole Polytechnique Fed Lausanne (EPFL) AB Femtosecond transient absorption spectroscopy is performed to assess bridge effects on energy transfer and charge separation in molecular junctions. A short, conjugated bridge can facilitate charge separation from both donor and acceptor, whereas in longer bridges charge separation only occurs from the excited donor. C1 [Zaks, J.; Segalman, R. A.; Fleming, G. R.] Univ Calif Berkeley, Appl Sci & Technol Grad Grp, Berkeley, CA 94720 USA. [Sun, J.; Tilley, T. D.; Fleming, G. R.] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Sun, J.; Kirmayer, S.; Segalman, R. A.] Univ Calif Berkeley, Dept Chem & Biomol Engn, Berkeley, CA 94720 USA. [Zaks, J.; Fleming, G. R.] Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA USA. [Kirmayer, S.; Urban, J. J.; Segalman, R. A.] Lawrence Berkeley Natl Lab, Mat Sci Div, Mol Foundry, Berkeley, CA USA. RP Zaks, J (reprint author), Univ Calif Berkeley, Appl Sci & Technol Grad Grp, Berkeley, CA 94720 USA. FU Helios Solar Energy Research Center; Director, Office of Science, Office of Basic Energy Sciences of the U.S. Department of Energy [DE-AC02-05CH11231] FX We thank Dr. Ying-Zhong Ma and Dr. Matthew Graham for assistance with the experimental apparatus. This work was funded by the Helios Solar Energy Research Center, which is supported by the Director, Office of Science, Office of Basic Energy Sciences of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. NR 9 TC 0 Z9 0 U1 0 U2 10 PU E D P SCIENCES PI CEDEX A PA 17 AVE DU HOGGAR PARC D ACTIVITES COUTABOEUF BP 112, F-91944 CEDEX A, FRANCE SN 2100-014X BN 978-2-7598-0956-1 J9 EPJ WEB CONF PY 2013 VL 41 AR UNSP 05011 DI 10.1051/epjconf/20134105011 PG 3 WC Physics, Multidisciplinary SC Physics GA BFM57 UT WOS:000320558600131 ER PT S AU Lorenzo-Martin, C Ajayi, OO Torrel, S Demas, N Fenske, GR AF Lorenzo-Martin, C. Ajayi, O. O. Torrel, S. Demas, N. Fenske, G. R. BE Zhu, D Lin, HT Zhou, Y Hwang, T Halbig, M Mathur, S TI EFFECT OF HARD THIN FILM COATINGS ON TRIBOCHEMICAL FILM BEHAVIOR UNDER LUBRICATED SLIDING CONTACT SO ADVANCED CERAMIC COATINGS AND MATERIALS FOR EXTREME ENVIRONMENTS II SE Ceramic Engineering and Science Proceedings LA English DT Proceedings Paper CT 36th International Conference and Expo on Advanced Ceramics and Composites CY JAN 22-27, 2012 CL Daytona Beach, FL SP Amer Ceram Soc (ACerS), Amer Ceram Soc (ACerS), Engn Ceram Div (ECD) ID DIAMOND-LIKE CARBON; SURFACES AB Most of tribological components such as gears and bearings which are engaged in sliding or rolling contacts are made of ferrous materials. In order to reduce friction and wear, lubricants are usually applied to components. The lubricants are normally formulated with functional additives such as anti-wear, friction modifier, anti-oxidant, etc. These additives react with the ferrous materials surface to form tribochemical surface films. A variety of hard thin-film coatings are increasingly being used in tribological components. These coatings can enhance the friction and wear behavior of the components. The impacts of thin film coatings on surface reactions by lubricant additives, and hence their effectiveness in reducing friction and wear is currently unclear. In this study, we evaluated the friction and wear behavior of several commercially available thin-film ceramic coatings when lubricated with unformulated and fully formulated synthetic oils. In tests with unformulated lubricant, friction coefficient behavior is similar to the uncoated steel. While in tests with fully formulated lubricants, a variety of behaviors were observed for different coatings. These behaviors are explained in terms of the differences in tribochemical film formation and properties on the coatings surfaces. C1 [Lorenzo-Martin, C.; Ajayi, O. O.; Torrel, S.; Demas, N.; Fenske, G. R.] Argonne Natl Lab, Div Energy Syst, Argonne, IL 60439 USA. RP Lorenzo-Martin, C (reprint author), Argonne Natl Lab, Div Energy Syst, 9700 S Cass Ave, Argonne, IL 60439 USA. NR 7 TC 0 Z9 0 U1 0 U2 1 PU AMER CERAMIC SOC PI WESTERVILLE PA 735 CERAMIC PLACE, WESTERVILLE, OH 43081-8720 USA SN 0196-6219 BN 978-1-118-21747-4 J9 CERAM ENG SCI PROC PY 2013 BP 47 EP 55 PG 9 WC Materials Science, Ceramics SC Materials Science GA BFK97 UT WOS:000320335000005 ER PT J AU Chavez, DE Hanson, SK Veauthier, JM Parrish, DA AF Chavez, David E. Hanson, Susan K. Veauthier, Jacqueline M. Parrish, Damon A. TI Electroactive Explosives: Nitrate Ester-Functionalized 1,2,4,5-Tetrazines SO ANGEWANDTE CHEMIE-INTERNATIONAL EDITION LA English DT Article DE electroactive compounds; explosives; fluorescence; heterocycles; tetrazines ID S-TETRAZINES; MOLECULES; FLUORESCENCE; PETN C1 [Chavez, David E.; Hanson, Susan K.; Veauthier, Jacqueline M.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Parrish, Damon A.] Naval Res Lab, Struct Matter Lab, Washington, DC 20375 USA. RP Chavez, DE (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM dechavez@lanl.gov OI Veauthier, Jacqueline/0000-0003-2206-7786 FU DOE Science Campaign 2; U.S. Department of Energy [DE-AC52-06A25396]; Office of Naval Research [N00014-11-AF-0-0002] FX The authors would like to thank the DOE Science Campaign 2 for funding, Anna Giambra, Daniel Preston, Mary Sandstrom, Jose Archuleta for performing the sensitivity characterization and testing, and David Morris for helpful discussions. Los Alamos National Laboratory is operated by Los Alamos National Security (LANS, LLC) under contract No. DE-AC52-06A25396 for the U.S. Department of Energy. The authors also thank the Office of Naval Research (Award No. N00014-11-AF-0-0002). NR 28 TC 25 Z9 26 U1 0 U2 32 PU WILEY-V C H VERLAG GMBH PI WEINHEIM PA BOSCHSTRASSE 12, D-69469 WEINHEIM, GERMANY SN 1433-7851 EI 1521-3773 J9 ANGEW CHEM INT EDIT JI Angew. Chem.-Int. Edit. PY 2013 VL 52 IS 27 BP 6876 EP 6879 DI 10.1002/anie.201302128 PG 4 WC Chemistry, Multidisciplinary SC Chemistry GA 169JS UT WOS:000320776900010 PM 23681779 ER PT J AU Gong, Y Hu, HS Tian, GX Rao, LF Li, J Gibson, JK AF Gong, Yu Hu, Han-Shi Tian, Guoxin Rao, Linfeng Li, Jun Gibson, John K. TI A Tetrapositive Metal Ion in the Gas Phase: Thorium(IV) Coordinated by Neutral Tridentate Ligands SO ANGEWANDTE CHEMIE-INTERNATIONAL EDITION LA English DT Article DE actinides; density functional calculations; gas-phase chemistry; mass spectrometry; polycations ID MULTIPLY-CHARGED IONS; ACTINIDE SEPARATIONS; COMPLEXES; TRICATIONS; GENERATION; REACTIVITY; STABILITY; CHEMISTRY; PLUTONYL; HYDROLYSIS C1 [Gong, Yu; Tian, Guoxin; Rao, Linfeng; Gibson, John K.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. [Hu, Han-Shi; Li, Jun] Tsinghua Univ, Dept Chem, Beijing, Peoples R China. [Hu, Han-Shi; Li, Jun] Tsinghua Univ, Lab Organ Optoelect & Mol Engn, Minist Educ, Beijing, Peoples R China. [Li, Jun] Pacific NW Natl Lab, William R Wiley Environm Mol Sci Lab, Richland, WA 99352 USA. RP Li, J (reprint author), Tsinghua Univ, Dept Chem, Beijing, Peoples R China. EM junli.thu@gmail.com; jkgibson@lbl.gov RI Li, Jun/E-5334-2011 OI Li, Jun/0000-0002-8456-3980 FU U.S. Department of Energy, Office of Basic Energy Sciences, Heavy Element Chemistry, at LBNL [DE-AC02-05CH11231]; U.S. Department of Energy, Office of Basic Energy Sciences, Heavy Element Chemistry, at PNNL [DE-AC05-76RL01830]; NSFC of China [20933003, 91026003] FX This work was supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Heavy Element Chemistry, at LBNL under Contract No. DE-AC02-05CH11231 (Y.G., G. T., L. R., J.K.G.) and at PNNL under Contract No. DE-AC05-76RL01830 (J.L.). The theoretical work by H. S. H. and J.L. was also supported by NSFC (20933003 and 91026003) of China. The calculations were done using Tsinghua National Laboratory for Information Science and Technology and the Molecular Science Computing capability at the EMSL, a National scientific user facility located at the PNNL, operated for the Department of Energy by Battelle. NR 49 TC 12 Z9 13 U1 3 U2 47 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 27 BP 6885 EP 6888 DI 10.1002/anie.201302212 PG 4 WC Chemistry, Multidisciplinary SC Chemistry GA 169JS UT WOS:000320776900012 PM 23650148 ER PT J AU Cassata, WS Renne, PR AF Cassata, William S. Renne, Paul R. TI Kinetics of argon diffusion in calcite SO CHEMIE DER ERDE-GEOCHEMISTRY LA English DT Article DE Diffusion; Calcite; Noble gas; Argon; Cosmogenic ID NOBLE-GASES; THERMOCHRONOMETRY; MINERALS; PYROXENE AB Here we present results of detailed diffusion experiments on Ar-37 in laser-heated calcite crystals. The data define linear Arrhenius arrays that yield an average apparent activation energy of 417.4 +/- 4.3 kJ/mol and average frequency factor of 43.2 +/- 0.6 ln(s(-1)), which correspond to a closure temperature of 385 +/- 2 degrees C (for a 10 degrees C/Ma cooling rate). These results indicate that calcite quantitatively retains trapped atmospheric and in situ produced cosmogenic argon at Earth surface and upper crustal temperatures over geologic time. Furthermore, these are the first reported data on argon diffusion in a rhombohedral or carbonate mineral, an important constraint on models of noble gas diffusion kinetics in crystalline materials. 0 2012 Elsevier GmbH. All rights reserved. C1 [Cassata, William S.; Renne, Paul R.] Univ Calif Berkeley, Dept Earth & Planetary Sci, Berkeley, CA 94720 USA. [Cassata, William S.; Renne, Paul R.] Berkeley Geochronol Ctr, Berkeley, CA 94709 USA. RP Cassata, WS (reprint author), Lawrence Livermore Natl Lab, 7000 East Ave, Livermore, CA 94550 USA. EM cassata2@llnl.gov; prenne@bgc.org NR 21 TC 0 Z9 0 U1 1 U2 12 PU ELSEVIER GMBH, URBAN & FISCHER VERLAG PI JENA PA OFFICE JENA, P O BOX 100537, 07705 JENA, GERMANY SN 0009-2819 J9 CHEM ERDE-GEOCHEM JI Chem Erde-Geochem. PY 2013 VL 73 IS 1 BP 113 EP 115 DI 10.1016/j.chemer.2012.10.001 PG 3 WC Geochemistry & Geophysics SC Geochemistry & Geophysics GA 173MK UT WOS:000321083400008 ER PT J AU Kim, EH Johnson, JR Lee, DH Pyo, YS AF Kim, Eun-Hwa Johnson, Jay R. Lee, Dong-Hun Pyo, Yoo Surn TI Field-line resonance structures in Mercury's multi-ion magnetosphere SO EARTH PLANETS AND SPACE LA English DT Article; Proceedings Paper CT Workshop on Physical Processes in NonUniform Finite Magnetospheric Systems CY SEP 12-15, 2011 CL Fukuoka, JAPAN DE Mercury; field line resonance; wave absorption; multi-ion effects; ULF waves ID ULF WAVES; MESSENGER OBSERVATIONS; MAGNETIC-FIELD; FREQUENCY; EXOSPHERE; PLASMAS AB Recently, MESSENGER spacecraft detected transverse waves at Mercury's inner magnetosphere. The magnetic field fluctuations of theses waves are approximately perpendicular to the gradient of magnetic field magnitude which is similar to the field-line resonance characteristics predicted by numerical simulations in two-ion plasmas. In this paper, we perform a wave simulation in a three-ion plasma to consider the effect of multiple heavy ions at Mercury. Because recently observed wave frequencies are near the He+, He2+ and H+, we adopt multi-ion plasmas that contain H+, He2+, and He+. The simulation results show that several resonant waves between the ion gyrofrequencies can occur at the same location and also show the modulation of amplitude in time histories. Therefore, the simulation results suggest that it could be possible to observe two or three different resonant frequencies at certain locations in Mercury's magnetosphere. C1 [Kim, Eun-Hwa; Johnson, Jay R.] Princeton Univ, Princeton Plasma Phys Lab, Princeton, NJ 08543 USA. [Lee, Dong-Hun] Kyung Hee Univ, Sch Space Res, Yongin 449701, Gyeonggi, South Korea. [Lee, Dong-Hun; Pyo, Yoo Surn] Kyung Hee Univ, Sch Space Res, Dept Astron & Space Sci, Yongin 449701, Gyeonggi, South Korea. RP Kim, EH (reprint author), Princeton Univ, Princeton Plasma Phys Lab, POB 451, Princeton, NJ 08543 USA. EM ehkim@pppl.gov FU NASA [NNH09AM53I, NNH09AK63I, NNH11AQ46I]; NSF [ATM0902730]; DOE [DE-AC02-09CH11466]; WCU program through NRF; MEST of Korea [R31-10016]; [KRF-2008-31-C00375] FX The work at the Princeton University was supported by NASA grants (NNH09AM53I, NNH09AK63I, and NNH11AQ46I), NSF grant ATM0902730, and DOE contract DE-AC02-09CH11466. The work at the Kyung Hee University was supported by KRF-2008-31-C00375 and the WCU program through NRF funded by MEST of Korea (R31-10016). Eun-Hwa Kim thanks to Peter Damiano for useful discussions. NR 24 TC 5 Z9 5 U1 0 U2 8 PU SPRINGER HEIDELBERG PI HEIDELBERG PA TIERGARTENSTRASSE 17, D-69121 HEIDELBERG, GERMANY SN 1880-5981 J9 EARTH PLANETS SPACE JI Earth Planets Space PY 2013 VL 65 IS 5 BP 447 EP 451 DI 10.5047/eps.2012.08.004 PG 5 WC Geosciences, Multidisciplinary SC Geology GA 171MS UT WOS:000320934100007 ER PT J AU Zhang, HF Parikh, HM Bapat, J Lin, YH Surratt, JD Kamens, RM AF Zhang, Haofei Parikh, Harshal M. Bapat, Jyoti Lin, Ying-Hsuan Surratt, Jason D. Kamens, Richard M. TI Modelling of secondary organic aerosol formation from isoprene photooxidation chamber studies using different approaches SO ENVIRONMENTAL CHEMISTRY LA English DT Article DE gas-particle partitioning; isoprene-derived epoxides; kinetic models; reactive uptake ID VOLATILITY BASIS-SET; AQUEOUS-PHASE; SOA FORMATION; 2-METHYLGLYCERIC ACID; CHEMICAL-COMPOSITION; RELATIVE-HUMIDITY; KINETIC MECHANISM; MASS-SPECTROMETRY; NATURAL SUNLIGHT; UNITED-STATES AB Secondary organic aerosol (SOA) formation from the photooxidation of isoprene was simulated against smog chamber experiments with varied concentrations of isoprene, nitrogen oxides (NOx = NO + NO2) and ammonium sulfate seed aerosols. A semi-condensed gas-phase isoprene chemical mechanism (ISO-UNC) was coupled with different aerosol-phase modelling frameworks to simulate SOA formation, including: (1) the Odum two-product approach, (2) the 1-D volatility basis-set (VBS) approach and (3) a new condensed kinetic model based upon the gas-particle partitioning theory and reactive uptake processes. The first two approaches are based upon empirical parameterisations from previous studies. The kinetic model uses a gas-phase mechanism to explicitly predict the major intermediate precursors, namely the isoprene-derived epoxides, and hence simulate SOA formation. In general, they all tend to significantly over predict SOA formation when semivolatile concentrations are higher because more semivolatiles are forced to produce SOA in the models to maintain gas-particle equilibrium; yet the data indicate otherwise. Consequently, modified dynamic parameterised models, assuming non-equilibrium partitioning, were incorporated and could improve the model performance. In addition, the condensed kinetic model was expanded by including an uptake limitation representation so that reactive uptake processes slow down or even stop; this assumes reactive uptake reactions saturate seed aerosols. The results from this study suggest that isoprene SOA formation by reactive uptake of gas-phase precursors is likely limited by certain particle-phase features, and at high gas-phase epoxide levels, gas-particle equilibrium is not obtained. The real cause of the limitation needs further investigation; however, the modified kinetic model in this study could tentatively be incorporated in large-scale SOA models given its predictive ability. C1 [Zhang, Haofei; Parikh, Harshal M.; Bapat, Jyoti; Lin, Ying-Hsuan; Surratt, Jason D.; Kamens, Richard M.] Univ N Carolina, Dept Environm Sci & Engn, Gillings Sch Global Publ Hlth, Chapel Hill, NC 27599 USA. RP Zhang, HF (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. EM hfzhang@lbl.gov RI Surratt, Jason/D-3611-2009; Lin, Ying-Hsuan/J-4023-2014 OI Surratt, Jason/0000-0002-6833-1450; Lin, Ying-Hsuan/0000-0001-8904-1287 FU National Science Foundation [ATM-0711097]; US Environmental Protection Agency [EP-W-09023]; Electric Power Research Institute (EPRI); UNC Graduate School FX This research was supported by National Science Foundation (ATM-0711097) and US Environmental Protection Agency (number EP-W-09023, Project Officer: Deborah Luecken) to the University of North Carolina. J.D. Surratt and Y.-H. Lin were supported in part by the Electric Power Research Institute (EPRI). Y.-H. Lin also acknowledges a Dissertation Completion Fellowship from the UNC Graduate School. The authors thank Professor Harvey E. Jeffries (UNC) for useful discussions. The authors thank Yang Zhou, Elias P. Rosen and Weruka Rattanavaraha for help with experimental design. NR 66 TC 3 Z9 3 U1 4 U2 64 PU CSIRO PUBLISHING PI COLLINGWOOD PA 150 OXFORD ST, PO BOX 1139, COLLINGWOOD, VICTORIA 3066, AUSTRALIA SN 1448-2517 EI 1449-8979 J9 ENVIRON CHEM JI Environ. Chem. PY 2013 VL 10 IS 3 SI SI BP 194 EP 209 DI 10.1071/EN13029 PG 16 WC Chemistry, Analytical; Environmental Sciences SC Chemistry; Environmental Sciences & Ecology GA 173FU UT WOS:000321064400007 ER PT J AU Noel, JK Sanbonmatsu, KY Whitford, PC AF Noel, Jeffrey K. Sanbonmatsu, Karissa Y. Whitford, Paul C. TI The energy landscapes of ribosome function SO JOURNAL OF BIOMOLECULAR STRUCTURE & DYNAMICS LA English DT Meeting Abstract C1 [Noel, Jeffrey K.] Rice Univ, Ctr Theoret Biol Phys, Houston, TX 77005 USA. [Sanbonmatsu, Karissa Y.] Los Alamos Natl Lab, Theoret Biol & Biophys Grp, Los Alamos, NM 87545 USA. [Whitford, Paul C.] Northeastern Univ, Dept Phys, Boston, MA 02115 USA. EM p.whitford@neu.edu NR 0 TC 0 Z9 0 U1 0 U2 2 PU TAYLOR & FRANCIS INC PI PHILADELPHIA PA 325 CHESTNUT ST, SUITE 800, PHILADELPHIA, PA 19106 USA SN 0739-1102 J9 J BIOMOL STRUCT DYN JI J. Biomol. Struct. Dyn. PD JAN 1 PY 2013 VL 31 SU 1 SI SI MA 35 BP 21 EP 22 DI 10.1080/07391102.2013.786468 PG 2 WC Biochemistry & Molecular Biology; Biophysics SC Biochemistry & Molecular Biology; Biophysics GA 160VU UT WOS:000320149400035 ER PT J AU Alexandrov, BS Rasmussen, KO Bishop, AR Usheva, A AF Alexandrov, Boian S. Rasmussen, Kim O. Bishop, Alan R. Usheva, Anny TI Protein-DNA binding and breathing dynamics of DNA SO JOURNAL OF BIOMOLECULAR STRUCTURE & DYNAMICS LA English DT Meeting Abstract ID TRANSCRIPTION FACTOR; YY1 C1 [Alexandrov, Boian S.; Rasmussen, Kim O.; Bishop, Alan R.] Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. [Alexandrov, Boian S.; Usheva, Anny] Harvard Univ, Beth Israel Deaconess Med Ctr, Sch Med, Boston, MA 02215 USA. EM boian@lanl.gov RI Alexandrov, Boian/D-2488-2010 OI Alexandrov, Boian/0000-0001-8636-4603 NR 8 TC 0 Z9 0 U1 0 U2 6 PU TAYLOR & FRANCIS INC PI PHILADELPHIA PA 325 CHESTNUT ST, SUITE 800, PHILADELPHIA, PA 19106 USA SN 0739-1102 J9 J BIOMOL STRUCT DYN JI J. Biomol. Struct. Dyn. PD JAN 1 PY 2013 VL 31 SU 1 SI SI MA 76 BP 49 EP 50 DI 10.1080/07391102.2013.786510 PG 2 WC Biochemistry & Molecular Biology; Biophysics SC Biochemistry & Molecular Biology; Biophysics GA 160VU UT WOS:000320149400078 ER PT J AU Zhang, L Ren, G AF Zhang, Lei Ren, Gang TI Individual-particle electron tomography: a method for studying macromolecule dynamics SO JOURNAL OF BIOMOLECULAR STRUCTURE & DYNAMICS LA English DT Meeting Abstract C1 [Zhang, Lei; Ren, Gang] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA. EM gren@lbl.gov RI Zhang, Lei/G-6427-2012 OI Zhang, Lei/0000-0002-4880-824X NR 4 TC 0 Z9 0 U1 0 U2 4 PU TAYLOR & FRANCIS INC PI PHILADELPHIA PA 325 CHESTNUT ST, SUITE 800, PHILADELPHIA, PA 19106 USA SN 0739-1102 J9 J BIOMOL STRUCT DYN JI J. Biomol. Struct. Dyn. PD JAN 1 PY 2013 VL 31 SU 1 SI SI MA 108 BP 68 EP 69 DI 10.1080/07391102.2013.786350 PG 2 WC Biochemistry & Molecular Biology; Biophysics SC Biochemistry & Molecular Biology; Biophysics GA 160VU UT WOS:000320149400110 ER PT J AU Cantara, WA Vendeix, FAP Murphy, FV Leszcynska, G Harris, K Gustilo, EM Sproat, B Kaiser, R Malkiewicz, A Agris, PF AF Cantara, William A. Vendeix, Franck A. P. Murphy, Franck V. Leszcynska, Grazyna Harris, Kimberly Gustilo, Estella M. Sproat, Brian Kaiser, Rob Malkiewicz, Andrzej Agris, Paul F. TI The importance of being modified: tautomeric forms of pyrimidines provide expanded use of the genetic code SO JOURNAL OF BIOMOLECULAR STRUCTURE & DYNAMICS LA English DT Meeting Abstract C1 [Cantara, William A.; Vendeix, Franck A. P.; Murphy, Franck V.; Leszcynska, Grazyna; Harris, Kimberly; Gustilo, Estella M.; Sproat, Brian; Kaiser, Rob; Malkiewicz, Andrzej; Agris, Paul F.] SUNY Albany, Dept Biol Sci, RNA Inst, Albany, NY 12222 USA. [Cantara, William A.; Vendeix, Franck A. P.; Murphy, Franck V.; Leszcynska, Grazyna; Harris, Kimberly; Gustilo, Estella M.; Sproat, Brian; Kaiser, Rob; Malkiewicz, Andrzej; Agris, Paul F.] SUNY Albany, Dept Chem, RNA Inst, Albany, NY 12222 USA. [Cantara, William A.; Vendeix, Franck A. P.; Murphy, Franck V.; Leszcynska, Grazyna; Harris, Kimberly; Gustilo, Estella M.; Sproat, Brian; Kaiser, Rob; Malkiewicz, Andrzej; Agris, Paul F.] Argonne Natl Lab, Northeastern Collaborat Access Team, Argonne, IL 60439 USA. [Cantara, William A.; Vendeix, Franck A. P.; Murphy, Franck V.; Leszcynska, Grazyna; Harris, Kimberly; Gustilo, Estella M.; Sproat, Brian; Kaiser, Rob; Malkiewicz, Andrzej; Agris, Paul F.] Brown Univ, Dept Mol Biol Cell Biol & Biochem, Providence, RI 02912 USA. [Cantara, William A.; Vendeix, Franck A. P.; Murphy, Franck V.; Leszcynska, Grazyna; Harris, Kimberly; Gustilo, Estella M.; Sproat, Brian; Kaiser, Rob; Malkiewicz, Andrzej; Agris, Paul F.] Tech Univ Lodz, PL-90924 Lodz, Poland. [Cantara, William A.; Vendeix, Franck A. P.; Murphy, Franck V.; Leszcynska, Grazyna; Harris, Kimberly; Gustilo, Estella M.; Sproat, Brian; Kaiser, Rob; Malkiewicz, Andrzej; Agris, Paul F.] Dharmacon, Thermo Fisher, CO USA. EM pagris@albany.edu NR 2 TC 0 Z9 0 U1 1 U2 1 PU TAYLOR & FRANCIS INC PI PHILADELPHIA PA 325 CHESTNUT ST, SUITE 800, PHILADELPHIA, PA 19106 USA SN 0739-1102 J9 J BIOMOL STRUCT DYN JI J. Biomol. Struct. Dyn. PD JAN 1 PY 2013 VL 31 SU 1 SI SI MA 112 BP 71 EP 72 DI 10.1080/07391102.2013.786354 PG 2 WC Biochemistry & Molecular Biology; Biophysics SC Biochemistry & Molecular Biology; Biophysics GA 160VU UT WOS:000320149400113 ER PT J AU Meduri, P Chen, HH Xiao, J Martinez, JJ Carlson, T Zhang, JG Deng, ZD AF Meduri, Praveen Chen, Honghao Xiao, Jie Martinez, Jayson J. Carlson, Thomas Zhang, Ji-Guang Deng, Z. Daniel TI Tunable electrochemical properties of fluorinated graphene SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID PRIMARY LITHIUM BATTERIES; GRAPHITE FLUORIDE; CARBON-MONOFLUORIDE; POROUS GRAPHENE; CATHODE; PERFORMANCE; ATMOSPHERE AB The structural and electrochemical properties of fluorinated graphene have been investigated by using a series of graphene fluorides (CFx, x = 0.47, 0.66, 0.89). Fluorinated graphene exhibited high capacity retentions of 75-81% of theoretical capacity at moderate rates as cathode materials for primary lithium batteries. Specifically, CF0.47 maintained a capacity of 356 mAh g (1) at a 5 C rate, superior to that of traditional fluorinated graphite. The discharged graphene fluorides also provide an electrochemical tool to probe the chemical bonding on the parent graphene substrate. C1 [Meduri, Praveen; Chen, Honghao; Xiao, Jie; Martinez, Jayson J.; Carlson, Thomas; Zhang, Ji-Guang; Deng, Z. Daniel] Pacific NW Natl Lab, Energy & Environm Directorate, Richland, WA 99352 USA. RP Deng, ZD (reprint author), Pacific NW Natl Lab, Energy & Environm Directorate, Richland, WA 99352 USA. EM jie.xiao@pnnl.gov; zhiqun.deng@pnnl.gov RI Deng, Daniel/A-9536-2011 OI Deng, Daniel/0000-0002-8300-8766 FU U.S. Army Corps of Engineers (USACE), Portland District; Battelle for the U.S. Department of Energy (DOE) [DE-AC05-76RL01830]; DOE, Office of Biological and Environmental Research FX This research is supported by the U.S. Army Corps of Engineers (USACE), Portland District, as part of the injectable acoustic microtransmitter development project. Brad Eppard is the technical lead for USACE and we greatly appreciate his involvement and oversight. The study was conducted at the Pacific Northwest National Laboratory (PNNL) in Richland, Washington, which is operated by Battelle for the U.S. Department of Energy (DOE) under Contract DE-AC05-76RL01830. The authors thank Vorbeck Materials Corporation and Prof. Ilhan A. Aksay of Princeton University, Princeton for providing the graphene. The authors also thank Suree Brown, J. L. Adcock and Sheng Dai of The University of Tennessee, Knoxville for their help in fluorination of graphene. The authors thank Xiaolin Li and Libor Kovarik of PNNL for the XRD and TEM characterization, respectively. The TEM work was performed at the Environmental Molecular Sciences Laboratory (EMSL) located at PNNL, a national scientific user facility sponsored by the DOE, Office of Biological and Environmental Research. NR 34 TC 21 Z9 21 U1 8 U2 57 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 27 BP 7866 EP 7869 DI 10.1039/c3ta11710c PG 4 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA 166JR UT WOS:000320551200002 ER PT J AU Wang, XQ Liu, CG Neff, D Fulvio, PF Mayes, RT Zhamu, A Fang, Q Chen, GR Meyer, HM Jang, BZ Dai, S AF Wang, Xiqing Liu, Chen-Guang Neff, David Fulvio, Pasquale F. Mayes, Richard T. Zhamu, Aruna Fang, Qing Chen, Guorong Meyer, Harry M. Jang, Bor Z. Dai, Sheng TI Nitrogen-enriched ordered mesoporous carbons through direct pyrolysis in ammonia with enhanced capacitive performance SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID POROUS CARBON; DOPED CARBON; CO2 CAPTURE; SUPERCAPACITOR PERFORMANCE; BLOCK-COPOLYMERS; OXYGEN REDUCTION; POLYMERS; TRANSFORMATION; NANOCOMPOSITE; ELECTROLYTE AB Self-assembly of phenolic resins and a Pluronic block copolymer via the soft-template method enables the formation of well-organized polymeric mesostructures, providing an easy way for preparation of ordered mesoporous carbons (OMCs). However, direct synthesis of OMCs with high nitrogen content remains a significant challenge due to the limited availability of nitrogen precursors capable of co-polymerizing with phenolic resins without deterioration of the order of mesostructural arrangement and significant diminishment of nitrogen content during carbonization. In this work, we demonstrate pyrolysis of the soft-templated polymeric composites in ammonia as a direct, facile way towards nitrogen-enriched OMCs (N-OMCs). This approach does not require any nitrogen-containing carbon precursors or post-treatment, but takes advantage of the preferential reaction and/ or replacement of oxygen with nitrogen species, generated by decomposition of ammonia at elevated temperatures, in oxygen-rich polymers during pyrolysis. It combines carbonization, nitrogen functionalization, and activation into one simple process, generating N-OMCs with a uniform pore size, large surface area (up to 1400 m(2) g(-1)), and high nitrogen content (up to 9.3 at%). More importantly, the ordering of the meso-structure is well-maintained as long as the heating temperature does not exceed 800 degrees C, above which (e. g., 850 degrees C) a slight structural degradation is observed. When being used as electrode materials for symmetric electric double layer capacitors, N-OMCs demonstrate enhanced capacitance (6.8 mu F cm(-2) vs. 3.2 mu F cm(-2)) and reduced ion diffusion resistance compared to the non-NH3-treated sample. C1 [Wang, Xiqing; Fulvio, Pasquale F.; Mayes, Richard T.; Dai, Sheng] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. [Wang, Xiqing; Liu, Chen-Guang; Neff, David; Fang, Qing; Chen, Guorong; Jang, Bor Z.] Nanotek Instruments Inc, Dayton, OH 45404 USA. [Zhamu, Aruna] Angstron Mat Inc, Dayton, OH 45404 USA. [Meyer, Harry M.] Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN 37831 USA. [Dai, Sheng] Univ Tennessee, Dept Chem, Knoxville, TN 37996 USA. RP Dai, S (reprint author), Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. EM xiqing.wang@gmail.com; bor.jang@wright.edu; dais@ornl.gov RI FANG, QING/C-9498-2013; Fulvio, Pasquale/B-2968-2014; Wang, Xiqing/E-3062-2010; Dai, Sheng/K-8411-2015; Mayes, Richard/G-1499-2016 OI Fulvio, Pasquale/0000-0001-7580-727X; Wang, Xiqing/0000-0002-1843-008X; Dai, Sheng/0000-0002-8046-3931; Mayes, Richard/0000-0002-7457-3261 FU Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy, [DE-AC05-OR22725]; Fluid Interface Reactions, Structures, and Transport (FIRST) Center; Energy Frontier Research Center; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences; Nanotek Instruments, Inc.; Ohio Third Frontier Advanced Energy Program [OTFAEP 11-303] FX The main part of this work was supported by the Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy, under contract DE-AC05-OR22725 with Oak Ridge National Laboratory, managed and operated by UT-Battelle, LLC. S. D. and P. F. F. was supported as part of the Fluid Interface Reactions, Structures, and Transport (FIRST) Center, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences. The work done at Nanotek Instruments, Inc. was supported by the Ohio Third Frontier Advanced Energy Program under award OTFAEP 11-303. NR 43 TC 38 Z9 39 U1 11 U2 130 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 27 BP 7920 EP 7926 DI 10.1039/c3ta11342f PG 7 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA 166JR UT WOS:000320551200011 ER PT J AU Baggetto, L Ganesh, P Sun, CN Meisner, RA Zawodzinski, TA Veith, GM AF Baggetto, Loic Ganesh, P. Sun, Che-Nan Meisner, Roberta A. Zawodzinski, Thomas A. Veith, Gabriel M. TI Intrinsic thermodynamic and kinetic properties of Sb electrodes for Li-ion and Na-ion batteries: experiment and theory SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID AUGMENTED-WAVE METHOD; HIGH-CAPACITY; LITHIUM; STORAGE; SODIUM; MOSSBAUER; SYSTEMS; ANODE AB A detailed comparative study between the electrochemical lithiation and sodiation of pure antimony (Sb), relating changes in structural, thermodynamic, kinetic and electrochemical properties has been carried out. For this purpose, a wide range of measurements using electrochemical (galvanostatic cycling, GITT, PITT), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) methods as well as density functional theory (DFT) based investigations have been undertaken. Assessment of the thermodynamics reveals that the reaction proceeds identically during the first and second cycles for Li whereas it differs between the first and subsequent cycles for Na as the reaction with Na proceeds through a different pathway associated with the formation of amorphous NaxSb phases. For the first time we rationalize the amorphization of NaxSb phases by the long ranged strain propagation due to Na-vacancy compared to Li-3-Sb. At full discharge, our XRD results show for the first time that a minor fraction of hexagonal Li3Sb forms concomitantly with cubic Li3Sb. The XRD results confirm that Sb crystallizes into hexagonal Na3Sb at full sodiation. The kinetics of the reaction is assessed by rate performance tests which highlight that both Li and Na can diffuse rapidly throughout micron thick films at room temperature. However, it is found that the (de) insertion of Li provides lower overpotentials and larger storage capacities compared to Na. The difference in rate performance is complemented by diffusion coefficient determinations near the 0 V region where both materials are crystallized into M3Sb (M Li, Na). Interestingly, calculations show that the energy barrier for near-neighbor vacancy migration, predominant in these close-packed phases, is about twice for Na than for Li. Our analysis tries to relate the lower intrinsic diffusivity of Na compared to Li with the long-range strain propagation induced by the former, thereby leading to an intrinsic origin of differences in rates, mechanical properties and amorphization. Finally, the surface chemistry of Sb electrodes cycled in NaClO4 dissolved in pure PC with(out) the addition of 5 wt% EC or FEC shows presence of ethers and NaF for the EC- and FEC-based electrolytes, respectively, and SEI films rich in Na-based carbonates. C1 [Baggetto, Loic; Sun, Che-Nan; Meisner, Roberta A.; Zawodzinski, Thomas A.; Veith, Gabriel M.] Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. [Ganesh, P.] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. [Meisner, Roberta A.] Univ Tennessee, Dept Mat Sci & Engn, Knoxville, TN 37996 USA. [Zawodzinski, Thomas A.] Univ Tennessee, Dept Chem & Biomol Engn, Knoxville, TN 37996 USA. RP Baggetto, L (reprint author), Oak Ridge Natl Lab, Div Mat Sci & Technol, 1 Bethel Valley Rd, Oak Ridge, TN 37831 USA. EM baggettol@ornl.gov; ganeshp@ornl.gov; veithgm@ornl.gov RI Sun, Che-Nan/I-3871-2013; Ganesh, Panchapakesan/L-5571-2013; Ganesh, Panchapakesan/E-3435-2012; Baggetto, Loic/D-5542-2017 OI Ganesh, Panchapakesan/0000-0002-7170-2902; Baggetto, Loic/0000-0002-9029-2363 FU U.S. Department of Energy (DOE); Basic Energy Sciences (BES); Materials Sciences and Engineering Division; DOE-BES FX This work was supported by the U.S. Department of Energy (DOE), Basic Energy Sciences (BES), Materials Sciences and Engineering Division. Computations performed at the Center for Nanophase Materials Sciences (CNMS) are sponsored by DOE-BES. NR 23 TC 79 Z9 79 U1 31 U2 194 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 27 BP 7985 EP 7994 DI 10.1039/c3ta11568b PG 10 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA 166JR UT WOS:000320551200020 ER PT J AU Hsu, HM Cheng, PK Chen, WF Kuo, MH Chen, CC Kuo, PL AF Hsu, Huang-Ming Cheng, Ping-Kai Chen, Wei-Fu Kuo, Meng-Hsin Chen, Chi-Chang Kuo, Ping-Lin TI Highly conductive, crosslinked ionomers based on poly(styrene-co-maleic anhydride) for water electrolysis SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID METHANOL FUEL-CELLS; PROTON-EXCHANGE MEMBRANES; POLYHEDRAL OLIGOSILSESQUIOXANE; TEMPERATURES; DEGRADATION; PERFORMANCE; COPOLYMERS; TRANSPORT; NETWORK; MONOMER AB Hydrogen production through water electrolysis calls for a low-cost non-fluoro membrane to make the process economically viable due to the high cost and environmental concerns of the current fluorinated ionomers. Here, we present such an ionomer with high proton conductivity based on the hybrid of commercially available poly(styrene-co-maleic anhydride) and polyhedral oligomeric silsesquioxane (POSS). The three-dimensional POSS framework, which does not only act as a robust scaffold but also provides binding sites for water, contributes to the amount of bound water, high proton conductivity and good oxidative stability. C1 [Hsu, Huang-Ming; Cheng, Ping-Kai; Kuo, Meng-Hsin; Chen, Chi-Chang; Kuo, Ping-Lin] Natl Cheng Kung Univ, Dept Chem Engn, Tainan, Taiwan. [Chen, Wei-Fu] Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA. RP Chen, WF (reprint author), Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA. EM wfchen@bnl.gov; plkuo@mail.ncku.edu.tw NR 38 TC 2 Z9 2 U1 3 U2 29 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 28 BP 8093 EP 8096 DI 10.1039/c3ta11059a PG 4 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA 170TG UT WOS:000320876000002 ER PT J AU Shao, M Das, S Xiao, K Chen, JH Keum, JK Ivanov, IN Gu, G Durant, W Li, DW Geohegan, DB AF Shao, Ming Das, Sanjib Xiao, Kai Chen, Jihua Keum, Jong K. Ivanov, Ilia N. Gu, Gong Durant, William Li, Dawen Geohegan, David B. TI High-performance organic field-effect transistors with dielectric and active layers printed sequentially by ultrasonic spraying SO JOURNAL OF MATERIALS CHEMISTRY C LA English DT Article ID HIGH-MOBILITY; ULTRADILUTE SOLUTION; POLYMER; DEPOSITION; SEMICONDUCTORS; FABRICATION; CIRCUITS; CELLS; FILMS AB High-performance organic field-effect transistors (OFETs) are reported with dielectric and active layers sequentially deposited by ultrasonic spray-printing. A cross-linkable insulator and a soluble small molecule semiconductor are developed which are both printable and highly robust. Using plastic with pre-patterned indium tin oxide gate contacts as required for display applications, two different layers are sequentially spray-printed: the semiconductor 6,13-bis(trisopropylsilylethynyl)pentacene (TIPS-PEN), and the insulator poly-4-vinylphenol (PVP). OFETs printed in ambient air with a bottom-gate/top-contact geometry are shown to achieve on/off ratios of >10(4) and mobilities up to 0.35 cm(2) V-1 s(-1). These rival the characteristics of the best solution-processable small molecule FETs fabricated by other processing methods such as drop casting and ink-jet printing. C1 [Shao, Ming; Xiao, Kai; Chen, Jihua; Keum, Jong K.; Ivanov, Ilia N.; Geohegan, David B.] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. [Das, Sanjib; Gu, Gong] Univ Tennessee, Dept Elect Engn & Comp Sci, Knoxville, TN 37931 USA. [Keum, Jong K.] Oak Ridge Natl Lab, Neutron Scattering Sci Div, Oak Ridge, TN 37831 USA. [Durant, William; Li, Dawen] Univ Alabama, Dept Elect & Comp Engn, Tuscaloosa, AL 35487 USA. RP Xiao, K (reprint author), Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, 1 Bethel Valley Rd, Oak Ridge, TN 37831 USA. EM xiaok@ornl.gov RI Chen, Jihua/F-1417-2011; ivanov, ilia/D-3402-2015; Gu, Gong/L-5919-2015; Keum, Jong/N-4412-2015; Geohegan, David/D-3599-2013; Das, Sanjib/A-9255-2017 OI Chen, Jihua/0000-0001-6879-5936; ivanov, ilia/0000-0002-6726-2502; Xiao, Kai /0000-0002-0402-8276; Gu, Gong/0000-0002-3888-1427; Keum, Jong/0000-0002-5529-1373; Geohegan, David/0000-0003-0273-3139; Das, Sanjib/0000-0002-5281-4458 FU Division of Scientific User Facilities, U.S. Department of Energy; Higher Education Research Experiences (HERE) summer intern program at ORNL; DOE [08-0217] FX This research was conducted at the Center for Nanophase Materials Sciences (CNMS), which is sponsored at Oak Ridge National Laboratory by the Division of Scientific User Facilities, U.S. Department of Energy, managed by UT-Battelle, LLC, for the U.S. Department of Energy. K. X. and W. D. acknowledge support from the Higher Education Research Experiences (HERE) summer intern program at ORNL, and D. L. acknowledges partial support from DOE travel fund (08-0217). NR 35 TC 14 Z9 14 U1 4 U2 53 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7526 J9 J MATER CHEM C JI J. Mater. Chem. C PY 2013 VL 1 IS 28 BP 4384 EP 4390 DI 10.1039/c3tc30535j PG 7 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA 172PD UT WOS:000321015700011 ER PT J AU Cuennet, JG Vasdekis, AE Psaltis, D AF Cuennet, J. G. Vasdekis, A. E. Psaltis, D. TI Optofluidic-tunable color filters and spectroscopy based on liquid-crystal microflows SO LAB ON A CHIP LA English DT Article ID LIGHT-EMITTING-DIODES; ON-A-CHIP; FLUORESCENCE DETECTION; CAPILLARY-ELECTROPHORESIS; MICROFLUIDICS; INTEGRATION; ABSORPTION; PLATFORM; SYSTEMS; ARRAYS AB The integration of color filters with microfluidics has attracted substantial attention in recent years, for on-chip absorption, fluorescence, or Raman analysis. We describe such tunable filters based on the micro-flow of liquid crystals. The filter operation is based on the wavelength-dependent liquid crystal birefringence that can be tuned by modifying the flow velocity field in the microchannel. The latter is possible both temporally and spatially by varying the inlet pressure and the channel geometry, respectively. We explored the use of these optofluidic filters for on-chip absorption spectroscopy in poly(dimethylsiloxane) microfluidic systems; by integrating the distance-dependent color filter with a dye-filled micro-channel, the absorption spectrum of a dye could be measured. Liquid crystal microflows substantially simplify the optofluidic integration, actuation and tuning of color filters for lab-on-a-chip spectroscopic applications. C1 [Cuennet, J. G.; Psaltis, D.] Ecole Polytech Fed Lausanne, Sch Engn, Opt Lab, CH-1015 Lausanne, Switzerland. [Vasdekis, A. E.] Pacific NW Natl Lab, Environm Mol Sci Lab, Richland, WA 99354 USA. RP Vasdekis, AE (reprint author), Pacific NW Natl Lab, Environm Mol Sci Lab, Richland, WA 99354 USA. EM andreas.vasdekis@pnnl.gov OI Vasdekis, Andreas/0000-0003-4315-1047 FU Laboratory Directed Research and Development funds [PN12005/2406] FX The experimental work and data analysis was performed at the Ecole Polytechnique Federale de Lausanne, Optics Laboratory. For the partial writing of the manuscript, A. E. V. gratefully acknowledges funding from the Laboratory Directed Research and Development funds administered by Pacific Northwest National Laboratory (project PN12005/2406). NR 34 TC 7 Z9 7 U1 0 U2 42 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 14 BP 2721 EP 2726 DI 10.1039/c3lc50501d PG 6 WC Biochemical Research Methods; Chemistry, Multidisciplinary; Nanoscience & Nanotechnology SC Biochemistry & Molecular Biology; Chemistry; Science & Technology - Other Topics GA 166KG UT WOS:000320552700010 PM 23752198 ER PT J AU Wang, WH Muckerman, JT Fujita, E Himeda, Y AF Wang, Wan-Hui Muckerman, James T. Fujita, Etsuko Himeda, Yuichiro TI Hydroxy-substituted pyridine-like N-heterocycles: versatile ligands in organometallic catalysis SO NEW JOURNAL OF CHEMISTRY LA English DT Article ID REVERSIBLE DEHYDROGENATION-HYDROGENATION; HALF-SANDWICH COMPLEXES; ACID-BASE-EQUILIBRIUM; ASTERISK-IR COMPLEX; CARBON-DIOXIDE; RUTHENIUM(II) COMPLEXES; COORDINATION CHEMISTRY; IRIDIUM CATALYST; WATER SOLUBILITY; AQUEOUS-MEDIA AB Bio-inspired complexes with hydroxy-substituted pyridine-like N-heterocyclic ligands have been applied in homogeneous catalysis, especially in transformations related to hydrogen storage. The hydroxy functional group has a significant effect on catalyst activation by acting as an electron donor and/or pendent base. This article presents the design and synthesis of new complexes with pyridine-like N-heterocyclic ligands bearing versatile hydroxy functional groups. Their application for the activation of small molecules such as H-2, CO2, and alcohols and their potential contribution to the hydrogen economy are highlighted. C1 [Wang, Wan-Hui; Himeda, Yuichiro] Natl Inst Adv Ind Sci & Technol, Tsukuba, Ibaraki 3058565, Japan. [Wang, Wan-Hui; Himeda, Yuichiro] ACT C, JST, Kawaguchi, Saitama 3320012, Japan. [Muckerman, James T.; Fujita, Etsuko] Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA. RP Himeda, Y (reprint author), Natl Inst Adv Ind Sci & Technol, Tsukuba Cent 5-2,1-1-1 Higashi, Tsukuba, Ibaraki 3058565, Japan. EM himeda.y@aist.go.jp RI Himeda, Yuichiro/E-8613-2014; Wang, Wan-Hui/J-8773-2012 OI Wang, Wan-Hui/0000-0002-5943-4589 FU JST, ACT-C; U.S. Department of Energy [DE-AC02-98CH10886]; Brookhaven National Laboratory FX Y.H. and W.-H.W. acknowledge JST, ACT-C for financial support. J.T.M. and E. F. thank the U.S. Department of Energy and its Division of Chemical Sciences, Geosciences, & Biosciences, Office of Basic Energy Sciences for funding under contract DE-AC02-98CH10886 with Brookhaven National Laboratory. NR 55 TC 24 Z9 24 U1 3 U2 51 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1144-0546 J9 NEW J CHEM JI New J. Chem. PY 2013 VL 37 IS 7 BP 1860 EP 1866 DI 10.1039/c3nj41146j PG 7 WC Chemistry, Multidisciplinary SC Chemistry GA 165ET UT WOS:000320466600001 ER PT S AU Cheng, L Curtiss, LA AF Cheng, Lei Curtiss, Larry A. BE BravoSuarez, JJ Kidder, MK Schwartz, V TI Computational Studies of Structure and Catalytic Activity of Vanadia for Propane Oxidative Dehydrogenation SO NOVEL MATERIALS FOR CATALYSIS AND FUELS PROCESSING SE ACS Symposium Series LA English DT Proceedings Paper CT Symposium on Novel Materials for Catalysis and Fuels Processing / 243rd American-Chemical-Society National Meeting CY MAR 25-29, 2012 CL San Diego, CA ID X-RAY-ABSORPTION; DENSITY-FUNCTIONAL THEORY; SITU RAMAN-SPECTROSCOPY; METAL OXIDE CATALYSTS; SUPPORTED VANADIA; TITANIA CATALYSTS; V2O5-TIO2-ANATASE CATALYST; MOLECULAR-STRUCTURE; REACTION-MECHANISM; SURFACE-STRUCTURE AB Understanding catalysis at a molecular level is the key to improving catalytic activity and the rational design of the next generation of catalysts. Despite the development of new surface science research techniques, characterization of surface catalytic sites still remain challenging due to the complexities of catalytic surfaces. Computational chemistry provides reaction studies at the molecular level and has become a very powerful tool for investigating catalysis. In this chapter, we review computational studies of supported vanadium oxide as a catalyst for the propane oxidative dehydrogenation reaction. The determination of the structure of active catalytic sites, elucidation of reaction mechanisms, and structure-activity relationships will be reviewed. C1 [Cheng, Lei; Curtiss, Larry A.] Argonne Natl Lab, Div Mat Sci, Argonne, IL 60439 USA. RP Cheng, L (reprint author), Argonne Natl Lab, Div Mat Sci, 9700 S Cass Ave, Argonne, IL 60439 USA. EM curtiss@anl.gov NR 51 TC 0 Z9 0 U1 2 U2 14 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 SIXTEENTH ST NW, WASHINGTON, DC 20036 USA SN 0097-6156 BN 978-0-8412-2811-5 J9 ACS SYM SER JI ACS Symp. Ser. PY 2013 VL 1132 BP 71 EP 82 PG 12 WC Chemistry, Physical; Energy & Fuels SC Chemistry; Energy & Fuels GA BFS61 UT WOS:000321160400002 ER PT S AU Formo, EV Wu, ZL Mahurin, SM Dai, S AF Formo, Eric V. Wu, Zili Mahurin, Shannon M. Dai, Sheng BE BravoSuarez, JJ Kidder, MK Schwartz, V TI Utilizing Surface Enhanced Raman Spectroscopy for the Study of Interfacial Phenomena: Probing Interactions on an Alumina Surface SO NOVEL MATERIALS FOR CATALYSIS AND FUELS PROCESSING SE ACS Symposium Series LA English DT Proceedings Paper CT Symposium on Novel Materials for Catalysis and Fuels Processing / 243rd American-Chemical-Society National Meeting CY MAR 25-29, 2012 CL San Diego, CA ID ATOMIC LAYER DEPOSITION; METAL-OXIDE CATALYSTS; HETEROGENEOUS CATALYSIS; VIBRATIONAL INVESTIGATIONS; KEGGIN STRUCTURE; SITU; MOLYBDENUM(VI); TEMPERATURE; CHEMISTRY; ACID AB Herein is a discussion of new developments in expanding Surface Enhanced Raman Spectroscopy (SERS) into probing a catalyst's structure and interface interactions. To accomplish this, robust SERS substrates were generated by depositing a protective alumina coating on top of silver nanowires (NWs) via atomic layer deposition (ALD). In situ studies of catalytic systems were conducted by analyzing the effects of heating a solid acid on the alumina surface in various environments at temperatures up to 400 degrees C. Interestingly, the distance-dependent decay of the SERS effect allowed us to probe with enhanced detail the interfacial region. Further, we monitored adsorbate interface interactions between the adsorption-desorption of pyridine on the acidic sites of a solid acid. C1 [Formo, Eric V.; Wu, Zili; Dai, Sheng] Oak Ridge Natl Lab, Ctr Nanophase Mat, Oak Ridge, TN 37831 USA. RP Formo, EV (reprint author), Oak Ridge Natl Lab, Ctr Nanophase Mat, POB 2008 MS6493, Oak Ridge, TN 37831 USA. EM wuz1@ornl.gov; dais@ornl.gov RI Wu, Zili/F-5905-2012; Dai, Sheng/K-8411-2015 OI Wu, Zili/0000-0002-4468-3240; Dai, Sheng/0000-0002-8046-3931 NR 32 TC 0 Z9 0 U1 1 U2 15 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 SIXTEENTH ST NW, WASHINGTON, DC 20036 USA SN 0097-6156 BN 978-0-8412-2811-5 J9 ACS SYM SER JI ACS Symp. Ser. PY 2013 VL 1132 BP 101 EP 114 PG 14 WC Chemistry, Physical; Energy & Fuels SC Chemistry; Energy & Fuels GA BFS61 UT WOS:000321160400004 ER PT S AU Chai, SH Howe, JY Kidder, M Wang, X Schwartz, V Overbury, SH Dai, S Jiang, DE AF Chai, Song-Hai Howe, Jane Y. Kidder, Michelle Wang, Xiqing Schwartz, Viviane Overbury, Steven H. Dai, Sheng Jiang, De-en BE BravoSuarez, JJ Kidder, MK Schwartz, V TI Rhodium Nanoparticles Confined in Ordered Mesoporous Carbon: Microscopic Characterization and Catalytic Application for Synthesis Gas Conversion to Ethanol SO NOVEL MATERIALS FOR CATALYSIS AND FUELS PROCESSING SE ACS Symposium Series LA English DT Proceedings Paper CT Symposium on Novel Materials for Catalysis and Fuels Processing / 243rd American-Chemical-Society National Meeting CY MAR 25-29, 2012 CL San Diego, CA ID RH CATALYSTS; SYNGAS; CO; HYDROGENATION; ADSORPTION AB Rh nanoparticles (2-4 nm) confined in the nanopores (6.5 nm) of ordered mesoporous carbon (OMC) were characterized by scanning transmission electron microscopy imaging on the cross-section of OMC grains generated using state-of-the-art focused ion beam lift-out technique. The catalytic activity (turnover frequency) and ethanol selectivity of Rh/OMC for synthesis gas conversion to ethanol are enhanced greatly when triply promoted with Mn, Li, and Fe oxides. Compared with traditional mesoporous silica having similar pore size, OMC as the support of promoted Rh catalyst increases the ethanol selectivity along with suppressing the formation of undesired hydrocarbons, although its overall activity is lowered to some extent. C1 [Chai, Song-Hai; Kidder, Michelle; Wang, Xiqing; Overbury, Steven H.; Dai, Sheng; Jiang, De-en] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. RP Chai, SH (reprint author), Oak Ridge Natl Lab, Div Chem Sci, 1 Bethel Valley Rd, Oak Ridge, TN 37831 USA. EM chais@ornl.gov; jiangd@ornl.gov RI Jiang, De-en/D-9529-2011; Chai, Song-Hai/A-9299-2012; Overbury, Steven/C-5108-2016; Howe, Jane/G-2890-2011; Dai, Sheng/K-8411-2015; OI Jiang, De-en/0000-0001-5167-0731; Chai, Song-Hai/0000-0002-4152-2513; Overbury, Steven/0000-0002-5137-3961; Dai, Sheng/0000-0002-8046-3931; Wang, Xiqing/0000-0002-1843-008X NR 24 TC 0 Z9 0 U1 0 U2 8 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 SIXTEENTH ST NW, WASHINGTON, DC 20036 USA SN 0097-6156 BN 978-0-8412-2811-5 J9 ACS SYM SER JI ACS Symp. Ser. PY 2013 VL 1132 BP 231 EP 243 PG 13 WC Chemistry, Physical; Energy & Fuels SC Chemistry; Energy & Fuels GA BFS61 UT WOS:000321160400009 ER PT S AU Schwartz, V Overbury, SH Liang, CD AF Schwartz, Viviane Overbury, Steven H. Liang, Chengdu BE BravoSuarez, JJ Kidder, MK Schwartz, V TI Carbon-Mediated Catalysis: Oxidative Dehydrogenation on Graphitic Carbon SO NOVEL MATERIALS FOR CATALYSIS AND FUELS PROCESSING SE ACS Symposium Series LA English DT Proceedings Paper CT Symposium on Novel Materials for Catalysis and Fuels Processing / 243rd American-Chemical-Society National Meeting CY MAR 25-29, 2012 CL San Diego, CA ID ACTIVATED CARBON; HETEROGENEOUS CATALYSIS; ETHYLBENZENE; NANOTUBES; STYRENE; OXYDEHYDROGENATION; SELECTIVITY; ISOBUTANE; OXIDE; CHEMISTRY AB Although carbon has been widely used in catalytic processes as a support material, very little is known about its function as an active catalyst. The scientific challenge is to achieve a detailed mechanistic understanding of the structural or chemical sites of the carbon that are catalytically active especially because of the very heterogeneous nature of carbon surfaces. This problem is complicated by the fact that there are limited tools to characterize the surface chemical and structural properties of carbon materials. This review highlights recent efforts from our group in utilizing well-defined synthetic nanostructure carbons in which surface properties can be controlled and systematically varied in order to identify their function for oxidative dehydrogenation reactions. Manipulation of exposed edge sites and oxygen functionalities are some of the aspects studied for controlling activity and selectivity on carbon catalysis. C1 [Schwartz, Viviane; Overbury, Steven H.; Liang, Chengdu] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. RP Schwartz, V (reprint author), Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, POB 2008 MS6493, Oak Ridge, TN 37831 USA. EM schwartzv@ornl.gov RI Overbury, Steven/C-5108-2016 OI Overbury, Steven/0000-0002-5137-3961 NR 40 TC 3 Z9 3 U1 1 U2 11 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 SIXTEENTH ST NW, WASHINGTON, DC 20036 USA SN 0097-6156 BN 978-0-8412-2811-5 J9 ACS SYM SER JI ACS Symp. Ser. PY 2013 VL 1132 BP 247 EP 258 PG 12 WC Chemistry, Physical; Energy & Fuels SC Chemistry; Energy & Fuels GA BFS61 UT WOS:000321160400010 ER PT S AU Kandel, K Althaus, SM Pruski, M Slowing, II AF Kandel, Kapil Althaus, Stacey M. Pruski, Marek Slowing, Igor I. BE BravoSuarez, JJ Kidder, MK Schwartz, V TI Supported Hybrid Enzyme-Organocatalysts for Upgrading the Carbon Content of Alcohols SO NOVEL MATERIALS FOR CATALYSIS AND FUELS PROCESSING SE ACS Symposium Series LA English DT Proceedings Paper CT Symposium on Novel Materials for Catalysis and Fuels Processing / 243rd American-Chemical-Society National Meeting CY MAR 25-29, 2012 CL San Diego, CA ID MESOPOROUS SILICA; ETHANOL; OXIDASE; FUNCTIONALIZATION; CONVERSION; ENGINE; YEAST; FUEL AB A bicatalytic system was prepared by the immobilization of alcohol oxidase enzyme and an alkylamine organocatalyst in distinct locations of mesoporous nanoparticles. The resulting nanocomposites were able to perform a sequence of oxidation and aldol coupling reactions, which transformed short chain alcohols into longer chain molecules. The process takes place at low temperatures, but requires additional enzyme (catalase) to prevent inactivation of the catalyst. This qualitative study introduces a model of a hybrid multicomponent nanomaterial that resembles the behavior of multienzymatic systems within confined spaces. C1 [Kandel, Kapil] US DOE, Ames Lab, Ames, IA 50011 USA. RP Kandel, K (reprint author), US DOE, Ames Lab, Ames, IA 50011 USA. EM islowing@iastate.edu OI Slowing, Igor/0000-0002-9319-8639 NR 17 TC 2 Z9 2 U1 1 U2 6 PU AMER CHEMICAL SOC PI WASHINGTON PA 1155 SIXTEENTH ST NW, WASHINGTON, DC 20036 USA SN 0097-6156 BN 978-0-8412-2811-5 J9 ACS SYM SER JI ACS Symp. Ser. PY 2013 VL 1132 BP 261 EP 271 PG 11 WC Chemistry, Physical; Energy & Fuels SC Chemistry; Energy & Fuels GA BFS61 UT WOS:000321160400011 ER PT J AU Kirilovsky, D Kerfeld, CA AF Kirilovsky, Diana Kerfeld, Cheryl A. TI The Orange Carotenoid Protein: a blue-green light photoactive protein SO PHOTOCHEMICAL & PHOTOBIOLOGICAL SCIENCES LA English DT Article ID SYNECHOCYSTIS PCC 6803; PHOTOSYSTEM-II; ENERGY-DISSIPATION; PHYCOBILISOME FLUORESCENCE; PHOTOPROTECTIVE MECHANISM; MOLECULAR SWITCH; SP PCC-6803; CYANOBACTERIUM; COMPLEX; OCP AB This review focuses on the Orange Carotenoid Protein (OCP) which is the first photoactive protein identified containing a carotenoid as the photoresponsive chromophore. This protein is essential for the triggering of a photoprotective mechanism in cyanobacteria which decreases the excess absorbed energy arriving at the photosynthetic reaction centers by increasing thermal dissipation at the level of the phycobilisomes, the cyanobacterial antenna. Blue-green light causes structural changes within the carotenoid and the protein, converting the orange inactive form into a red active form. The activated red form interacts with the phycobilisome and induces the decrease of phycobilisome fluorescence emission and of the energy arriving to the photosynthetic reaction centers. The OCP is the light sensor, the signal propagator and the energy quencher. A second protein, the Fluorescence Recovery Protein (FRP), is needed to detach the red OCP from the phycobilisome and its reversion to the inactive orange form. In the last decade, in vivo and in vitro mechanistic studies combined with structural and genomic data resulted in both the discovery and a detailed picture of the function of the OCP and OCP-mediated photoprotection. Recent structural and functional results are emphasized and important previous results will be reviewed. Similarities to other blue-light responsive proteins will be discussed. C1 [Kirilovsky, Diana] CEA, Inst Biol & Technol Saclay iBiTec S, F-91191 Gif Sur Yvette, France. [Kirilovsky, Diana] CNRS, UMR 8221, F-91191 Gif Sur Yvette, France. [Kerfeld, Cheryl A.] US Dept Energy Joint Genome Inst, Walnut Creek, CA 94598 USA. [Kerfeld, Cheryl A.] Univ Calif Berkeley, Dept Plant & Microbial Biol, Berkeley, CA 94720 USA. [Kerfeld, Cheryl A.] Berkeley Synthet Biol Inst, Berkeley, CA 94720 USA. RP Kirilovsky, D (reprint author), CEA, Inst Biol & Technol Saclay iBiTec S, F-91191 Gif Sur Yvette, France. EM diana.kirilovsky@cea.fr FU National Science Foundation [MCB0851070]; Commissariat a l'Energie Atomique; Centre National de la Recherche Scientifique; Agence Nationale de la Recherche; EU network HARVEST FX The authors thank Ryan Leverenz and Seth Axen for assistance with data compilation and figures. C. A. K. was supported by National Science Foundation grant MCB0851070. The research of DK and her group was supported by the "Commissariat a l'Energie Atomique", the "Centre National de la Recherche Scientifique" and the "Agence Nationale de la Recherche" (project CAROPROTECT). The work was also partially supported by EU network HARVEST. NR 57 TC 54 Z9 60 U1 5 U2 51 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1474-905X J9 PHOTOCH PHOTOBIO SCI JI Photochem. Photobiol. Sci. PY 2013 VL 12 IS 7 BP 1135 EP 1143 DI 10.1039/c3pp25406b PG 9 WC Biochemistry & Molecular Biology; Biophysics; Chemistry, Physical SC Biochemistry & Molecular Biology; Biophysics; Chemistry GA 166MD UT WOS:000320557800003 PM 23396391 ER PT S AU Lupinacci, A Shapiro, AA Suh, JO Minor, AM AF Lupinacci, A. Shapiro, A. A. Suh, J. O. Minor, A. M. GP IEEE TI A study of solder alloy ductility for cryogenic applications SO 2013 IEEE INTERNATIONAL SYMPOSIUM ON ADVANCED PACKAGING MATERIALS (APM) SE International Symposium on Advanced Packaging Materials-Processes, Properties, and Interfaces LA English DT Proceedings Paper CT IEEE International Symposium on Advanced Packaging Materials (APM) CY FEB 27-MAR 01, 2013 CL Irvine, CA SP IEEE ID TIN; CRYSTALS AB For aerospace applications it is important to understand the mechanical performance of components at the extreme temperature conditions seen in service. For solder alloys used in microelectronics, cryogenic temperatures can prove problematic. At low temperatures Sn-based solders undergo a ductile to brittle transition that leads to brittle cracks, which can result in catastrophic failure of electronic components, assemblies and spacecraft payloads. As industrial processes begin to move away from Pb-Sn solder, it is even more critical to characterize the behavior of alternative Sn-based solders. Here we report on initial investigations using a modified Charpy test apparatus to characterize the ductile to brittle transformation temperature of nine different solder systems. C1 [Shapiro, A. A.; Suh, J. O.] CALTECH, Jet Prop Lab, 4800 Oak Grove Dr, Pasadena, CA 91109 USA. [Lupinacci, A.; Minor, A. M.] Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA. [Lupinacci, A.; Minor, A. M.] Natl Ctr Electron Microscopy, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Shapiro, AA (reprint author), CALTECH, Jet Prop Lab, 4800 Oak Grove Dr, Pasadena, CA 91109 USA. EM Andrew.A.Shapiro@jpl.nasa.gov NR 10 TC 0 Z9 0 U1 1 U2 11 PU IEEE PI NEW YORK PA 345 E 47TH ST, NEW YORK, NY 10017 USA SN 1550-5723 BN 978-1-4673-6091-3; 978-1-4673-6093-7 J9 INT SYM ADV PKG MAT PY 2013 PG 6 WC Engineering, Electrical & Electronic; Materials Science, Multidisciplinary SC Engineering; Materials Science GA BFN19 UT WOS:000320594100010 ER PT S AU Su, J Liu, WP Shu, NC Yan, SQ Smith, MS Wang, JS Yang, YY Li, XQ He, C Li, ZH Guo, B Huang, WZ Zeng, S Li, ET Jin, SJ Liu, X Wang, YB Lian, G Li, YJ Chen, YS Bai, XX AF Su, J. Liu, W. P. Shu, N. C. Yan, S. Q. Smith, M. S. Wang, J. S. Yang, Y. Y. Li, X. Q. He, C. Li, Z. H. Guo, B. Huang, W. Z. Zeng, S. Li, E. T. Jin, S. J. Liu, X. Wang, Y. B. Lian, G. Li, Y. J. Chen, Y. S. Bai, X. X. BE Liu, W Hatanaka, K Zhu, S Aoi, N TI The half-lives of Mn-50, Fe-51, Co-52,Co-53, and Ni-53,Ni-54 SO 8TH CHINA-JAPAN JOINT NUCLEAR PHYSICS SYMPOSIUM (CJJNPS2012) SE AIP Conference Proceedings LA English DT Proceedings Paper CT 8th China-Japan Joint Nuclear Physics Symposium (CJJNPS) CY OCT 15-19, 2012 CL China Inst Atom Energy (CIAE), Beijing, PEOPLES R CHINA SP Natl Nat Sci Fdn China (NSFC), China Ctr Adv Sci & Technol, Chinese Nucl Phys Soc, Peking Univ, State Key Lab Nucl Phys & Technol, CAS, Inst Modern Phys, CAS, Shanghai Inst Appl Phys HO China Inst Atom Energy (CIAE) DE beta decay; half-life; rp-process ID FERMI BETA-DECAY; X-RAY-BURSTS; RP-PROCESS; SC-42; SOLAR; V-46 AB We have measured the beta decay half-lives of Mn-50, Fe-51, Co-52,Co-53, and Ni-53,Ni-54 produced via the Ni-58 projectile fragmentation. The uncertainty of Co-52 half-life was reduced by a factor of 3 compared to the previous result. The half- lives were evaluated with the previous values and used as inputs of nucleosynthesis calculations of the rapid proton-capture process in an x-ray burst. C1 [Su, J.; Liu, W. P.; Shu, N. C.; Yan, S. Q.; Li, Z. H.; Guo, B.; Huang, W. Z.; Zeng, S.; Li, E. T.; Jin, S. J.; Liu, X.; Wang, Y. B.; Lian, G.; Li, Y. J.; Chen, Y. S.; Bai, X. X.] China Inst Atom Energy, POB 275 10, Beijing 102413, Peoples R China. [Smith, M. S.] Oak Ridge Natl Lab, Div Phys, Oak Ridge, TN 37831 USA. [Wang, J. S.; Yang, Y. Y.] Chinese Acad Sci, Inst Modern Phys, Lanzhou 730000, Peoples R China. [Li, X. Q.; He, C.] Peking Univ, Sch Phys, State Key Lab Nucl Phys & Technol, Beijing 100871, Peoples R China. RP Su, J (reprint author), China Inst Atom Energy, POB 275 10, Beijing 102413, Peoples R China. FU National Natural Science Foundation of China [11021504, 10979026, 11105228]; 973 Program [2013CB834406] FX This work is supported by the National Natural Science Foundation of China under Grant Nos. 11021504, 10979026, 11105228, the 973 Program under Grand No. 2013CB834406. NR 20 TC 0 Z9 0 U1 0 U2 1 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1157-9 J9 AIP CONF PROC PY 2013 VL 1533 BP 78 EP 83 DI 10.1063/1.4806780 PG 6 WC Physics, Applied; Physics, Nuclear SC Physics GA BFO83 UT WOS:000320779500011 ER PT J AU Liu, QH Turhan, A Zawodzinski, TA Mench, MM AF Liu, Qinghua Turhan, Ahmet Zawodzinski, Thomas A. Mench, Matthew M. TI In situ potential distribution measurement in an all-vanadium flow battery SO CHEMICAL COMMUNICATIONS LA English DT Article ID SCALE ENERGY-STORAGE; PERFORMANCE; ELECTRODE; CELL; PROGRESS; MODEL AB An experimental method for measurement of local redox potential within multilayer electrodes was developed and applied to all-vanadium redox flow batteries (VRFBs). Through-plane measurement at the positive side reveals several important phenomena including potential distribution, concentration distribution of active species and the pre-dominant reaction location within the porous carbon electrodes. C1 [Liu, Qinghua; Turhan, Ahmet; Zawodzinski, Thomas A.; Mench, Matthew M.] Univ Tennessee, BRANE Lab, Dept Mech Aerosp & Biomed Engn, Knoxville, TN 37996 USA. [Liu, Qinghua; Turhan, Ahmet; Zawodzinski, Thomas A.; Mench, Matthew M.] Univ Tennessee, Dept Chem & Biomol Engn, Knoxville, TN 37996 USA. [Zawodzinski, Thomas A.; Mench, Matthew M.] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. RP Mench, MM (reprint author), Univ Tennessee, BRANE Lab, Dept Mech Aerosp & Biomed Engn, Knoxville, TN 37996 USA. EM mmench@utk.edu FU NSF [0644811]; TN-Score [NSF EPS-1004083] FX This work was partially funded by the NSF Early Career Development Award #0644811. Partial support of this work was also provided through TN-Score (NSF EPS-1004083). NR 25 TC 16 Z9 16 U1 3 U2 103 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 56 BP 6292 EP 6294 DI 10.1039/c3cc42092b PG 3 WC Chemistry, Multidisciplinary SC Chemistry GA 166LJ UT WOS:000320555800014 PM 23736771 ER PT J AU Starr, DE Liu, Z Havecker, M Knop-Gericke, A Bluhm, H AF Starr, D. E. Liu, Z. Haevecker, M. Knop-Gericke, A. Bluhm, H. TI Investigation of solid/vapor interfaces using ambient pressure X-ray photoelectron spectroscopy SO CHEMICAL SOCIETY REVIEWS LA English DT Review ID IN-SITU XPS; PREFERENTIAL CO OXIDATION; CATALYZED ALKYNE HYDROGENATION; CATALYTICALLY ACTIVE STATES; OXIDE ELECTROCHEMICAL-CELLS; CERIA-SUPPORTED CATALYSTS; DENSITY-FUNCTIONAL THEORY; SUM-FREQUENCY GENERATION; CARBON NANOTUBE GROWTH; GAS SHIFT REACTION AB Heterogeneous chemical reactions at vapor/solid interfaces play an important role in many processes in the environment and technology. Ambient pressure X-ray photoelectron spectroscopy (APXPS) is a valuable tool to investigate the elemental composition and chemical specificity of surfaces and adsorbates on the molecular scale at pressures of up to 130 mbar. In this review we summarize the historical development of APXPS since its introduction over forty years ago, discuss different approaches to minimize scattering of electrons by gas molecules, and give a comprehensive overview about the experimental systems (vapor/solid interfaces) that have been studied so far. We also present several examples for the application of APXPS to environmental science, heterogeneous catalysis, and electrochemistry. C1 [Starr, D. E.] Helmholtz Zentrum Berlin Mat & Energie GmbH, Solar Energy Res, EMIL, D-12489 Berlin, Germany. [Liu, Z.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. [Haevecker, M.; Knop-Gericke, A.] Max Planck Gesell, Fritz Haber Inst, Dept Inorgan Chem, D-14195 Berlin, Germany. [Haevecker, M.] Helmholtz Zentrum Berlin Mat & Energie GmbH, Catalysis Energy, Grp E GKAT, D-12489 Berlin, Germany. [Bluhm, H.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. RP Bluhm, H (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. EM hbluhm@lbl.gov RI Liu, Zhi/B-3642-2009 OI Liu, Zhi/0000-0002-8973-6561 FU Office of Energy Research, Office of Basic Energy Sciences, and Chemical Sciences Division of the U.S. Department of Energy [DE-AC02-05CH11231]; Office of Science, Biological and Environmental Research, Environmental Remediation Sciences Division (ERSD), U.S. Department of Energy [DE-AC02-05CH11231]; Silicon In situ Spectroscopy@the Sychrotron (SISSY) project within the Bundesministerium fur Bildung und Forschung (BMBF) [03SF0403]; European Union (Technotubes Project) FX The Advanced Light Source and beamline 11.0.2 are supported by the Director, Office of Energy Research, Office of Basic Energy Sciences, and Chemical Sciences Division of the U.S. Department of Energy under contracts No. DE-AC02-05CH11231. This work was also supported by the Office of Science, Biological and Environmental Research, Environmental Remediation Sciences Division (ERSD), U.S. Department of Energy under Contract No. DE-AC02-05CH11231. DES acknowledges support through the Silicon In situ Spectroscopy@the Sychrotron (SISSY) project within the Bundesministerium fur Bildung und Forschung (BMBF project number 03SF0403). The Helmholtz-Zentrum Berlin (Electron Storage Ring BESSY II) is acknowledged for provision of synchrotron radiation at beamline ISISS. Part of the work was supported by the European Union (Technotubes Project). NR 249 TC 106 Z9 106 U1 25 U2 259 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 13 BP 5833 EP 5857 DI 10.1039/c3cs60057b PG 25 WC Chemistry, Multidisciplinary SC Chemistry GA 160LC UT WOS:000320120000011 PM 23598709 ER PT J AU Wang, WH Suna, Y Himeda, Y Muckerman, JT Fujita, E AF Wang, Wan-Hui Suna, Yuki Himeda, Yuichiro Muckerman, James T. Fujita, Etsuko TI Functionalized cyclopentadienyl rhodium(III) bipyridine complexes: synthesis, characterization, and catalytic application in hydrogenation of ketones SO DALTON TRANSACTIONS LA English DT Article ID MULTIPLY SUBSTITUTED CYCLOPENTADIENES; ASYMMETRIC TRANSFER HYDROGENATION; HETEROCYCLIC CARBENE COMPLEXES; ELECTROCHEMICAL PROPERTIES; IRIDIUM CATALYST; CARBON-DIOXIDE; RUTHENIUM; LIGANDS; GENERATION; EXCHANGE AB A series of highly functionalized cyclopentadienyl rhodium(III) complexes, [Cp'Rh(bpy) Br](ClO4) (Cp' = substituted cyclopentadienyl), was synthesized from various multi-substituted cyclopentadienes (Cp'H). [Rh(cod) Cl] 2 and Cp'H were firstly converted to [Cp'Rh(cod)] complexes, which were then treated with Br-2 to give the rhodium(III) dibromides [Cp'RhBr2](2). The novel complexes [Cp'Rh(bpy) Br](ClO4) were obtained readily by the reaction of 2,2'-bipyridine with [Cp'RhBr2](2). These rhodium complexes [Cp'Rh(bpy) Br](ClO4) were fully characterized and utilized in the hydrogenation of cyclohexanone and acetophenone with generally high yields, but they did not exhibit the same reactivity trends for the two substrate ketones. The different activity of these complexes for the different substrates may be due to the influence of the substituents on the Cp' rings. C1 [Wang, Wan-Hui; Suna, Yuki; Himeda, Yuichiro] Natl Inst Adv Ind Sci & Technol, Tsukuba, Ibaraki 3058565, Japan. [Wang, Wan-Hui; Himeda, Yuichiro] JST, ACT C, Kawaguchi, Saitama 3320012, Japan. [Muckerman, James T.; Fujita, Etsuko] Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA. RP Himeda, Y (reprint author), Natl Inst Adv Ind Sci & Technol, Tsukuba Cent 5-2,1-1-1 Higashi, Tsukuba, Ibaraki 3058565, Japan. EM himeda.y@aist.go.jp RI Himeda, Yuichiro/E-8613-2014; Wang, Wan-Hui/J-8773-2012 OI Wang, Wan-Hui/0000-0002-5943-4589 FU JST; ACT-C; U.S. Department of Energy Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences [DE-AC02-98CH10886]; Brookhaven National Laboratory FX Y.H. and W.-H. W. acknowledge JST, ACT-C for financial support. J.T.M. and E.F. thank the U.S. Department of Energy and its Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences for funding under contract DE-AC02-98CH10886 with Brookhaven National Laboratory. We thank Dr Midori Goto and Dr Hide Kambayashi for X-ray crystallography. NR 49 TC 1 Z9 1 U1 1 U2 64 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 26 BP 9628 EP 9636 DI 10.1039/c3dt50445j PG 9 WC Chemistry, Inorganic & Nuclear SC Chemistry GA 162DZ UT WOS:000320246200028 PM 23677258 ER PT J AU Villa, EM Juan, DW Alekseev, EV Depmeier, W Albrecht-Schmitt, TE AF Villa, Eric M. Juan Diwu Alekseev, Evgeny V. Depmeier, Wulf Albrecht-Schmitt, Thomas E. TI Structural changes within the alkaline earth uranyl phosphites SO DALTON TRANSACTIONS LA English DT Article ID CRYSTAL-STRUCTURE; URANIUM PHOSPHITES; HYDROTHERMAL SYNTHESES; STRUCTURE VALIDATION; HEXAVALENT URANIUM; SOLID-SOLUTIONS; LEACHING TESTS; U6+ MINERALS; PLUTONIUM; CHEMISTRY AB Three new alkaline earth (AE) uranyl phosphites and one barium uranium(IV) phosphate were synthesized under hydrothermal conditions. The carbonate salts of the AE's were employed both as cation sources and as pH regulators. Despite having very similar formulas and uranyl building units, the Ca2+, Sr2+ and Ba2+ uranyl phosphites have three different extended networks. The calcium compound also contains a Ca2+/UO22+ mixed cation position. The four structure types will be presented herein with the AE cations generating distinct structural transformations. C1 [Villa, Eric M.; Albrecht-Schmitt, Thomas E.] Florida State Univ, Dept Chem & Biochem, Tallahassee, FL 32306 USA. [Villa, Eric M.; Juan Diwu; Albrecht-Schmitt, Thomas E.] Univ Notre Dame, Dept Civil & Environm Engn & Earth Sci, Notre Dame, IN 46556 USA. [Villa, Eric M.; Juan Diwu; Albrecht-Schmitt, Thomas E.] Univ Notre Dame, Dept Chem & Biochem, Notre Dame, IN 46556 USA. [Juan Diwu] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. [Juan Diwu] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Alekseev, Evgeny V.] Forschungszentrum Julich, Inst Energy & Climate Res IEK 6, D-52428 Julich, Germany. [Alekseev, Evgeny V.] Rhein Westfal TH Aachen, Inst Kristallog, D-52066 Aachen, Germany. [Depmeier, Wulf] Univ Kiel, Inst Geowissensch, D-24118 Kiel, Germany. RP Albrecht-Schmitt, TE (reprint author), Florida State Univ, Dept Chem & Biochem, 102 Vars Way, Tallahassee, FL 32306 USA. EM e.alekseev@fz-juelich.de; talbrechtschmitt@gmail.com RI Villa, Eric/B-5305-2016; OI Villa, Eric/0000-0001-9883-1993; Alekseev, Evgeny/0000-0002-4919-5211 FU Materials Science of Actinides; Energy Frontier Research Center; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001089]; Helmholtz Association [VH-NG-815] FX The authors are grateful for support provided 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 under Award Number DE-SC0001089. We would also like to thank the Center for Sustainable Energy at Notre Dame for the use of their instrumentation. EVA was supported by VH-NG-815 grant of the Helmholtz Association. NR 56 TC 4 Z9 4 U1 1 U2 15 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 26 BP 9637 EP 9644 DI 10.1039/c3dt50769f PG 8 WC Chemistry, Inorganic & Nuclear SC Chemistry GA 162DZ UT WOS:000320246200029 PM 23677038 ER PT S AU Aarts, G Allton, C Kelly, A Skullerud, JI Kim, S Harris, T Ryan, SM Lombardo, MP Oktay, MB Sinclair, DK AF Aarts, G. Allton, C. Kelly, A. Skullerud, J. -I. Kim, S. Harris, T. Ryan, S. M. Lombardo, M. P. Oktay, M. B. Sinclair, D. K. GP Institute of Physics TI Bottomonium from lattice QCD as a probe of the Quark-Gluon Plasma SO EXTREME QCD 2012 (XQCD) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 10th Extreme QCD Conference (xQCD) CY AUG 21-23, 2012 CL George Washington Univ, Washington, DC HO George Washington Univ AB We study the temperature dependence of bottomonium for temperatures in the range 0.4T(c) < T < 2.1T(c), using non-relativistic dynamics for the bottom quark and full relativistic lattice QCD simulations for N (f) - 2 light flavors. We consider the behaviour of the correlators in Euclidean space, we analyze the associated spectral functions and we study the dependence on the momentum. Our results are amenable to a successful comparison with effective field theories. They help build a coherent picture of the behaviour of bottomonium in the plasma, consistent which the current LHC results. C1 [Aarts, G.; Allton, C.] Swansea Univ, Dept Phys, Swansea, West Glam, Wales. [Kelly, A.; Skullerud, J. -I.] Natl Univ Ireland Maynooth, Dept Math Phys, Maynooth, Kildare, Ireland. [Kim, S.] Sejong Univ, Dept Phys, Seoul 143747, South Korea. [Harris, T.; Ryan, S. M.] Trinity Coll Dublin, Sch Math, Dublin 2, Ireland. [Lombardo, M. P.] Ist Nazl Fis Nucl, Lab Nazl Frascati, I-00044 Frascati, Italy. [Oktay, M. B.] Univ Utah, Dept Phys, Salt Lake City, UT 84112 USA. [Sinclair, D. K.] Argonne Natl Lab, HEP Div, Argonne, IL 60439 USA. RP Aarts, G (reprint author), Swansea Univ, Dept Phys, Swansea, West Glam, Wales. OI Skullerud, Jon-Ivar/0000-0002-8255-0043; Aarts, Gert/0000-0002-6038-3782 NR 23 TC 2 Z9 2 U1 0 U2 0 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 432 AR UNSP 012014 DI 10.1088/1742-6596/432/1/012014 PG 10 WC Physics, Particles & Fields SC Physics GA BFM51 UT WOS:000320537200014 ER PT S AU Bazavov, A Petreczky, P AF Bazavov, A. Petreczky, P. GP Institute of Physics TI Static quark correlators and quarkonium properties at non-zero temperature SO EXTREME QCD 2012 (XQCD) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 10th Extreme QCD Conference (xQCD) CY AUG 21-23, 2012 CL George Washington Univ, Washington, DC HO George Washington Univ ID FINITE-TEMPERATURE; SPECTRAL FUNCTIONS; HEAVY QUARKONIUM; FIELD-THEORIES; QCD AB We discuss different static quark correlators, including Wilson loops in 2+1 flavor QCD at non-zero temperature and their relation to in-medium quarkonium properties. We present lattice results on static correlation functions obtained with highly improved staggered fermion action and their implications for potential models. C1 [Bazavov, A.; Petreczky, P.] Brookhaven Natl Lab, Dept Phys, Upton, NY 11973 USA. RP Bazavov, A (reprint author), Brookhaven Natl Lab, Dept Phys, Upton, NY 11973 USA. EM bazavov@bnl.gov; petreczk@bnl.gov NR 38 TC 2 Z9 2 U1 0 U2 2 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 432 AR UNSP 012003 DI 10.1088/1742-6596/432/1/012003 PG 10 WC Physics, Particles & Fields SC Physics GA BFM51 UT WOS:000320537200003 ER PT S AU Ding, HT AF Ding, Heng-Tong GP Institute of Physics TI Exploring QCD phase diagram at vanishing baryon density on the lattice SO EXTREME QCD 2012 (XQCD) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 10th Extreme QCD Conference (xQCD) CY AUG 21-23, 2012 CL George Washington Univ, Washington, DC HO George Washington Univ ID CHIRAL CRITICAL-POINT; FINITE-TEMPERATURE; 3-FLAVOR QCD; CHROMODYNAMICS; TRANSITION AB I report on the current status of QCD phase diagram at vanishing baryon density. I focus on the QCD phase diagram with three degenerate quark flavor using Highly Improved Staggered Quarks on N-tau = 6 lattices. No evidence of a first order phase transition in the pion mass window of 80 less than or similar to m(pi) less than or similar to 230 MeV is found. The pion mass at the critical point where the chiral first order phase transition ends is estimated to be m(pi)(c) less than or similar to 45 MeV. C1 Brookhaven Natl Lab, Dept Phys, Upton, NY 11973 USA. RP Ding, HT (reprint author), Brookhaven Natl Lab, Dept Phys, Upton, NY 11973 USA. EM htding@quarkphy.bnl.gov OI Ding, Heng-Tong/0000-0003-0590-081X NR 26 TC 1 Z9 1 U1 0 U2 0 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2013 VL 432 AR UNSP 012027 DI 10.1088/1742-6596/432/1/012027 PG 5 WC Physics, Particles & Fields SC Physics GA BFM51 UT WOS:000320537200027 ER PT S AU Dumitru, A AF Dumitru, Adrian GP Institute of Physics TI Effective matrix models for deconfinement in SU(N) and G(2) gauge theories SO EXTREME QCD 2012 (XQCD) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 10th Extreme QCD Conference (xQCD) CY AUG 21-23, 2012 CL George Washington Univ, Washington, DC HO George Washington Univ AB I present a simple matrix model for the deconfined phase of SU(N) theories at temperatures just above T-c. The model is designed to reproduce the anomaly, in particular the flatness of (e - 3p)/T-2 above similar to 1.2T(c) observed by lattice simulations with up to six colors. Furthermore, it predicts the existence of an adjoint Higgs phase where the masses of diagonal and off-diagonal gluons split and that the phase transition of SU(N) with three or more colors, and for exceptional groups with a trivial center such as G(2), is generically of first order. For G(2) gauge group, a small value of the Polyakov loop at T-c(-) can be obtained with a non-perturbative potential summed over the roots of SU(7) rather than G(2), which implements the principle of maximal eigenvalue repulsion. C1 Brookhaven Natl Lab, RIKEN BNL Res Ctr, Upton, NY 11973 USA. RP Dumitru, A (reprint author), Brookhaven Natl Lab, RIKEN BNL Res Ctr, Upton, NY 11973 USA. EM adrian.dumitru@baruch.cuny.edu NR 9 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 432 AR UNSP 012006 DI 10.1088/1742-6596/432/1/012006 PG 5 WC Physics, Particles & Fields SC Physics GA BFM51 UT WOS:000320537200006 ER PT S AU Maezawa, Y AF Maezawa, Yu GP Institute of Physics TI Anomaly-induced charges in nucleons SO EXTREME QCD 2012 (XQCD) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 10th Extreme QCD Conference (xQCD) CY AUG 21-23, 2012 CL George Washington Univ, Washington, DC HO George Washington Univ ID SKYRME MODEL AB We suggest a novel charge structure inside nucleons in electromagnetic field due to the chiral anomaly. We use Skyrmions, where nucleons appear as solitons of mesons, to calculate the charge distributions in a single nucleon and find that an additional non-integer charge proportional to the magnetic field would be produced. This might look surprising, but the magnitude of the induced charge is evaluated to be tiny enough to have not been observed yet. C1 Brookhaven Natl Lab, Dept Phys, Upton, NY 11973 USA. RP Maezawa, Y (reprint author), Brookhaven Natl Lab, Dept Phys, Upton, NY 11973 USA. EM ymaezawa@bnl.gov NR 8 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 432 AR UNSP 012030 DI 10.1088/1742-6596/432/1/012030 PG 5 WC Physics, Particles & Fields SC Physics GA BFM51 UT WOS:000320537200030 ER PT S AU Skokov, V AF Skokov, Vladimir GP Institute of Physics TI Photon azimuthal anizotropy and magnetic field in heavy-ion collisions SO EXTREME QCD 2012 (XQCD) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 10th Extreme QCD Conference (xQCD) CY AUG 21-23, 2012 CL George Washington Univ, Washington, DC HO George Washington Univ ID QUARK-GLUON PLASMA; ANOMALIES; EVENT AB Recent measurements of the azimuthal anisotropy of direct photons in heavy-ion collisions at the energies of RHIC showed that it is of the same order as the hadronic one. This finding appears to contradict the expected dominance of photon production from a quark-gluon plasma at an early stage of a heavy-ion collision. A possible explanation of the strong azimuthal anisotropy of the photons, given recently, is based on the presence of a large magnetic field in the early phase of a collision. In this talk, we consider a novel photon production mechanism stemming from the conformal anomaly of QCDxQED and the existence of strong (electro)magnetic fields in heavy ion collisions. Using the hydrodynamical description of the bulk modes of QCD plasma, we show that this mechanism leads to the photon production yield that is comparable to the yield from conventional sources. The comparison of the results to the data from the PHENIX collaboration, show that this mechanism might be the most responsible for the observed azimuthal anisotropy of photons. C1 Brookhaven Natl Lab, Dept Phys, Upton, NY 11973 USA. RP Skokov, V (reprint author), Brookhaven Natl Lab, Dept Phys, Upton, NY 11973 USA. EM VSkokov@bnl.gov OI Skokov, Vladimir/0000-0001-7619-1796 NR 26 TC 3 Z9 3 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 432 AR UNSP 012021 DI 10.1088/1742-6596/432/1/012021 PG 5 WC Physics, Particles & Fields SC Physics GA BFM51 UT WOS:000320537200021 ER PT J AU Chen, R Song, J Lin, TY Aizin, GR Kawano, Y Aoki, N Ochiai, Y Whiteside, VR McCombe, BD Thomas, D Einhorn, M Reno, JL Strasser, G Bird, JP AF Chen, Rui Song, Jungwoo Lin, Teng-Yin Aizin, Gregory R. Kawano, Yukio Aoki, Nobuyuki Ochiai, Yuichi Whiteside, Vincent R. McCombe, Bruce D. Thomas, David Einhorn, Mike Reno, John L. Strasser, Gottfried Bird, Jonathan P. TI Terahertz Detection With Nanoscale Semiconductor Rectifiers SO IEEE SENSORS JOURNAL LA English DT Article DE Nanoelectronics; rectifiers; terahertz science; terahertz technology ID QUANTUM; PERFORMANCE AB In this paper, we describe our ongoing research on CMOS-compatible semiconductor nanosensors for broadband terahertz (THz) detection. We review the results of earlier work, which reveal the promise of THz rectification by nanoconstrictions, and present proof-of-concept results showing efficient THz detection at room temperature. C1 [Chen, Rui; Song, Jungwoo; Lin, Teng-Yin; Bird, Jonathan P.] SUNY Buffalo, Dept Elect Engn, Buffalo, NY 14260 USA. [Aizin, Gregory R.] CUNY, Kingsborough Community Coll, Dept Phys Sci, Brooklyn, NY 11235 USA. [Kawano, Yukio] Tokyo Inst Technol, Dept Phys Elect, Tokyo 1528552, Japan. [Aoki, Nobuyuki; Ochiai, Yuichi] Chiba Univ, Grad Sch Adv Integrat Sci, Chiba 2638522, Japan. [Whiteside, Vincent R.; McCombe, Bruce D.] SUNY Buffalo, Dept Phys, Buffalo, NY 14260 USA. [Thomas, David; Einhorn, Mike] Div AEgis Technol Inc, Nanogenesis, Huntsville, AL 35806 USA. [Reno, John L.] Sandia Natl Labs, CINT, Albuquerque, NM 87185 USA. [Strasser, Gottfried] Vienna Univ Technol, Ctr Micro & Nanostruct, A-1040 Vienna, Austria. [Strasser, Gottfried] Vienna Univ Technol, Inst Solid State Elect, A-1040 Vienna, Austria. RP Chen, R (reprint author), SUNY Buffalo, Dept Elect Engn, Buffalo, NY 14260 USA. EM rchen8@buffalo.edu; jungwoossong@gmail.com; eblreservation@gmail.com; gaizin@kbcc.cuny.edu; kawano@pe.titech.ac.jp; n-aoki@faculty.chiba-u.jp; ochiai@faculty.chiba-u.jp; vrw@buffalo.edu; mccombe@buffalo.edu; dthomas@nanogenesisgroup.com; meinhorn@nanogenesisgroup.com; jlreno@sandia.gov; gottfried.strasser@tuwien.ac.at; jbird@buffalo.edu RI Bird, Jonathan/G-4068-2010; Strasser, Gottfried/E-3274-2010 OI Bird, Jonathan/0000-0002-6966-9007; Strasser, Gottfried/0000-0003-0147-0883 FU NSF [ECS-0609146]; DoE [DE-FG03-01ER45920]; PSC-CUNY [62040-00 40]; AFOSR STTR [FA9550-10-C-0118]; U.S. Department of Energy's National Nuclear Security Administration [AC04-94AL85000] FX This work was supported by the NSF Grant ECS-0609146, DoE Grant DE-FG03-01ER45920, PSC-CUNY Grant 62040-00 40, and AFOSR STTR Grant FA9550-10-C-0118. This work was performed in part at the Center for Integrated Nanotechnologies, a U.S. Department of Energy, an Office of Basic Energy Sciences user facility. 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 associate editor coordinating the review of this paper and approving it for publication was Dr. Francis P. Hindle. NR 23 TC 1 Z9 1 U1 0 U2 4 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 1530-437X EI 1558-1748 J9 IEEE SENS J JI IEEE Sens. J. PD JAN PY 2013 VL 13 IS 1 DI 10.1109/JSEN.2012.2216522 PG 7 WC Engineering, Electrical & Electronic; Instruments & Instrumentation; Physics, Applied SC Engineering; Instruments & Instrumentation; Physics GA 166ZB UT WOS:000320598600004 ER PT J AU Margulis, GY Lim, B Hardin, BE Unger, EL Yum, JH Feckl, JM Fattakhova-Rohlfing, D Bein, T Gratzel, M Sellinger, A McGehee, MD AF Margulis, George Y. Lim, Bogyu Hardin, Brian E. Unger, Eva L. Yum, Jun-Ho Feckl, Johann M. Fattakhova-Rohlfing, Dina Bein, Thomas Graetzel, Michael Sellinger, Alan McGehee, Michael D. TI Highly soluble energy relay dyes for dye-sensitized solar cells SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID MESOPOROUS TITANIA FILMS; RUTHENIUM DYES; ORGANIC-DYE; EFFICIENCY; COSENSITIZATION; RECOMBINATION; PERFORMANCE; IMPROVEMENT; STRATEGY; ELECTRON AB High solubility is a requirement for energy relay dyes (ERDs) to absorb a large portion of incident light and significantly improve the efficiency of dye-sensitized solar cells (DSSCs). Two benzonitrile-soluble ERDs, BL302 and BL315, were synthesized, characterized, and resulted in a 65% increase in the efficiency of TT1-sensitized DSSCs. The high solubility (180 mM) of these ERDs allows for absorption of over 95% of incident light at their peak wavelength. The overall power conversion efficiency of DSSCs with BL302 and BL315 was found to be limited by their energy transfer efficiency of approximately 70%. Losses due to large pore size, dynamic collisional quenching of the ERD, energy transfer to desorbed sensitizing dyes and static quenching by complex formation were investigated and it was found that a majority of the losses are caused by the formation of statically quenched ERDs in solution. C1 [Margulis, George Y.] Stanford Univ, Dept Appl Phys, Stanford, CA 94305 USA. [Lim, Bogyu; Unger, Eva L.; McGehee, Michael D.] Stanford Univ, Dept Mat Sci & Engn, Stanford, CA 94305 USA. [Hardin, Brian E.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA. [Yum, Jun-Ho; Graetzel, Michael] Ecole Polytech Fed Lausanne, Lab Photon & Interfaces, CH-1015 Lausanne, Switzerland. [Feckl, Johann M.; Fattakhova-Rohlfing, Dina; Bein, Thomas] Univ Munich, Dept Chem, D-81377 Munich, Germany. [Feckl, Johann M.; Fattakhova-Rohlfing, Dina; Bein, Thomas] Univ Munich, Ctr NanoSci CeNS, D-81377 Munich, Germany. [Sellinger, Alan] Colorado Sch Mines, Dept Chem & Geochem, Golden, CO 80401 USA. RP Sellinger, A (reprint author), Colorado Sch Mines, Dept Chem & Geochem, Coolbaugh Hall,1012 14th St, Golden, CO 80401 USA. EM bein@lmu.de; michael.graetzel@epfl.ch; aselli@mines.edu; mmcgehee@stanford.edu RI Fattakhova-Rohlfing, Dina/E-7967-2012; Bein, Thomas/G-7686-2014; Lim, Bogyu/A-6737-2011; Unger, Eva/N-6230-2014; Sellinger, Alan/C-6250-2015; YUM, Jun-Ho/N-6183-2016 OI Fattakhova-Rohlfing, Dina/0000-0003-2008-0151; Bein, Thomas/0000-0001-7248-5906; Unger, Eva/0000-0002-3343-867X; Sellinger, Alan/0000-0001-6705-1548; FU Office of Naval Research (ONR) [N000141110244]; ABB Stanford Graduate Fellowship in Science and Engineering FX This work was supported by the Office of Naval Research (ONR) under grant N000141110244. G.Y.M. would like to acknowledge the support of the ABB Stanford Graduate Fellowship in Science and Engineering. We would like to thank Professor Tomas Torres (Universidad Autonoma de Madrid) for providing TT1 dye. NR 38 TC 17 Z9 17 U1 1 U2 53 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 27 BP 11306 EP 11312 DI 10.1039/c3cp51018b PG 7 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 166MB UT WOS:000320557600015 PM 23733016 ER PT S AU Meyer, FW Harris, PR Meyer, HM Hijazi, H Barghouty, AF AF Meyer, F. W. Harris, P. R. Meyer, H. M., III Hijazi, H. Barghouty, A. F. BE Zank, GP Borovsky, J Bruno, R Cirtain, J Cranmer, S Elliott, H Giacalone, J Gonzalez, W Li, G Marsch, E Moebius, E Pogorelov, N Spann, J Verkhoglyadova, O TI Kinetic And Potential Sputtering Of Lunar Regolith: The Contribution Of The Heavy (Minority) Solar Wind Ions SO PROCEEDINGS OF THE THIRTEENTH INTERNATIONAL SOLAR WIND CONFERENCE (SOLAR WIND 13) SE AIP Conference Proceedings LA English DT Proceedings Paper CT 13th International Solar Wind Conference (Solar Wind) CY JUN 17-22, 2012 CL HI SP Natl Sci Fdn (NSF), Int Conf & Networking Solut (ICNS) DE Solar wind; Sputtering; Lunar regolith; Ion-surface interactions ID HYDROGEN; SURFACE; POLES AB In this paper the sputtering of lunar regolith by protons and solar wind heavy ions is considered. From preliminary measurements of H+, Ar+1, Ar+6 and Ar+9 ion sputtering of JSC-1A AGGL lunar regolith simulant at solar wind velocities, and TRIM simulations of kinetic sputtering yields, the relative contributions of kinetic and potential sputtering contributions are estimated. An 80-fold enhancement of oxygen sputtering by Ar+ over same-velocity H+, and an additional x2 increase for Ar+9 over same-velocity Ar+ was measured. This enhancement persisted to the maximum fluences investigated (similar to 10(16)/cm(2)). Modeling studies including the enhanced oxygen ejection by potential sputtering due to the minority heavy ion multicharged ion solar wind component, and the kinetic sputtering contribution of all solar wind constituents, as determined from TRIM sputtering simulations, indicate an overall 35% reduction of near-surface oxygen abundance. XPS analyses of simulant samples exposed to singly and multicharged Ar ions show the characteristic signature of reduced (metallic) Fe, consistent with the preferential ejection of oxygen atoms that can occur in potential sputtering of some metal oxides. C1 [Meyer, F. W.; Harris, P. R.; Hijazi, H.] Oak Ridge Natl Lab, Div Phys, Oak Ridge, TN 37831 USA. RP Meyer, FW (reprint author), Oak Ridge Natl Lab, Div Phys, POB 2008, Oak Ridge, TN 37831 USA. EM meyerfw@ornl.gov NR 14 TC 0 Z9 0 U1 0 U2 4 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1163-0 J9 AIP CONF PROC PY 2013 VL 1539 BP 410 EP 413 DI 10.1063/1.4811072 PG 4 WC Energy & Fuels; Physics, Applied SC Energy & Fuels; Physics GA BFQ76 UT WOS:000320997100097 ER PT J AU Sturzbecher-Hoehne, M Deblonde, GJP Abergel, RJ AF Sturzbecher-Hoehne, M. Deblonde, G. J. -P. Abergel, R. J. TI Solution thermodynamic evaluation of hydroxypyridinonate chelators 3,4,3-LI(1,2-HOPO) and 5-LIO(Me-3,2-HOPO) for UO2(VI) and Th(IV) decorporation SO RADIOCHIMICA ACTA LA English DT Article DE Spectrophotometric titration; Actinide decorporation; Hydroxypyridinonate ligands; UO2 complexes; Th complexes ID SEQUESTERING AGENTS; EQUILIBRIUM-CONSTANTS; ACTINIDE CHELATORS; COMPLEX-FORMATION; LIGANDS; PROGRAM; THORIUM(IV); STABILITY; EFFICACY; IONS AB Solution thermodynamic studies were performed to characterize the coordination of U(VI) and Th(IV) by the multidentate hydroxypyridinonate chelating agents 3,4,3-LI(1,2-HOPO) and 5-LIO(Me-3,2-HOPO). Species distribution and conditional stability pM profiles were calculated based on the determined formation constants, showing that both ligands form extremely stable uranyl and thorium complexes in solution. At physiological pH, the formation of 1:1 ligand : uranyl complexes is favored for both ligands, while a 2:1 ligand : thorium complex is predominant with the tetradentate 5-LIO(Me-3,2-HOPO). Comparisons with functionally similar bidentate ligands as well as with the common actinide chelator diethylenetriamine pentaacetic acid emphasized the superior affinity for U(VI) and Th(IV) of both experimental compounds over a wide pH range. These analytical results corroborate the in vivo chelation efficacy of 3,4,3-LI(1,2-HOPO) and 5-LIO(Me-3,2-HOPO) and validate their selection for further development as therapeutic actinide decorporation agents. C1 [Sturzbecher-Hoehne, M.; Deblonde, G. J. -P.; Abergel, R. 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, Berkeley, CA 94720 USA. EM rjabergel@lbl.gov RI Deblonde, Gauthier/O-3881-2014 OI Deblonde, Gauthier/0000-0002-0825-8714 FU National Institutes of Health from the National Institute of Allergy and Infectious Diseases [1RC2AI087604-01, 5RC2AI087604-02]; E. O. Lawrence Berkeley National Laboratory, a U.S. Department of Energy Laboratory [DE-AC02-05CH11231] FX The authors are grateful to Prof. Kenneth N. Raymond for helpful discussions and for his support of the actinide decorporation program at the Lawrence Berkeley National Laboratory. This research was supported by National Institutes of Health grants 1RC2AI087604-01 and 5RC2AI087604-02 from the National Institute of Allergy and Infectious Diseases. The work was performed at the E. O. Lawrence Berkeley National Laboratory, a U.S. Department of Energy Laboratory under Contract No. DE-AC02-05CH11231. NR 34 TC 11 Z9 11 U1 3 U2 28 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 6 SI SI BP 359 EP 366 DI 10.1524/ract.2013.2047 PG 8 WC Chemistry, Inorganic & Nuclear; Nuclear Science & Technology SC Chemistry; Nuclear Science & Technology GA 172UJ UT WOS:000321030100003 ER PT J AU Lucchini, JF Borkowski, M Richmann, MK Reed, DT AF Lucchini, J. -F. Borkowski, M. Richmann, M. K. Reed, D. T. TI Uranium(VI) solubility in carbonate-free WIPP brine SO RADIOCHIMICA ACTA LA English DT Article DE Uranium; Solubility; WIPP; Carbonate; Borate ID NUCLEAR-WASTE; HYDROLYSIS; SPECIATION; ENVIRONMENT; ACTINIDES; SCHOEPITE; COMPLEXES; PLUTONIUM; CHEMISTRY; INSIGHTS AB The solubility of uranium(VI) was determined in WIPP-relevant brines as a function of pC(H+) and ionic strength, in the absence of carbonate. Carbonate concentration was below 2 x 10(-5) M, measured using the gas chromatography method. In the absence of carbonate, the uranium(VI) solubilities were about 10(-6) M in GWB at pC(H+) >= 7 and about 10(-8)-10(-)7 M in ERDA-6 brine at pC(H+) >= 8. Solubility of uranium(VI) was also measured in NaCl media at the same levels as in ERDA-6 brine. The data established a uranium solubility that was 10-100 times lower than published results from Diaz-Arocas and Grambow [13], and they are in good agreement with modeling results and other literature data [11, 12]. In the absence of carbonate, hydrolysis was the main complexation and precipitation mechanisms for uranium(VI) solubility at high ionic strength and pC(H+) >= 7. However, the effect of borate complexation was noticeable at pC(H+) similar to 8-9. C1 [Lucchini, J. -F.; Borkowski, M.; Richmann, M. K.; Reed, D. T.] Los Alamos Natl Lab, Earth & Environm Sci Div, Carlsbad, NM 88220 USA. RP Lucchini, JF (reprint author), Los Alamos Natl Lab, Earth & Environm Sci Div, 115 N Main, Carlsbad, NM 88220 USA. EM lucchini@lanl.gov NR 35 TC 1 Z9 1 U1 0 U2 14 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 6 SI SI BP 391 EP 398 DI 10.1524/ract.2013.2029 PG 8 WC Chemistry, Inorganic & Nuclear; Nuclear Science & Technology SC Chemistry; Nuclear Science & Technology GA 172UJ UT WOS:000321030100007 ER PT J AU Shim, YS Moon, HG Kim, DH Zhang, LH Yoon, SJ Yoon, YS Kang, CY Jang, HW AF Shim, Young-Seok Moon, Hi Gyu Kim, Do Hong Zhang, Lihua Yoon, Seok-Jin Yoon, Young Soo Kang, Chong-Yun Jang, Ho Won TI Au-decorated WO3 cross-linked nanodomes for ultrahigh sensitive and selective sensing of NO2 and C2H5OH SO RSC ADVANCES LA English DT Article ID SEMICONDUCTOR GAS SENSORS; SURFACE-CHEMISTRY; ELECTRONIC NOSE; EXHALED BREATH; LUNG-CANCER; THIN-FILMS; GOLD; CATALYSIS; NANORODS; CLUSTERS AB Au-decorated WO3 cross-linked nanodomes are fabricated using soft templates composed of highly ordered polystyrene beads and self-agglomeration of Au. The distribution and size of Au nanoparticles on the surface of WO3 cross-linked nanodomes are controlled by varying the thickness of the initial Au film. The responses of Au-decorated WO3 cross-linked nanodomes to various gases such as NO2, CH3COCH3, C2H5OH, NH3, CO, H-2, and C6H6 are at least 5 times higher than those of bare WO3 cross-linked nanodomes. The response enhancement by Au decoration is dependent on the target gas, which is attributed to an interplay between electronic and chemical sensitizations. In particular, the Au-decorated WO3 cross-linked nanodomes exhibit extremely high sensitivities and selectivities, and ppt-level detection limits to NO2 and C2H5OH at 250 degrees C and 450 degrees C, respectively. These results suggest that Au-decorated WO3 cross-linked nanodomes are very promising for use in breath analysers to diagnose both asthma and lung cancer from exhaled human breath. C1 [Shim, Young-Seok; Kim, Do Hong; Jang, Ho Won] Seoul Natl Univ, Res Inst Adv Mat, Dept Mat Sci & Engn, Seoul 151744, South Korea. [Shim, Young-Seok; Moon, Hi Gyu; Yoon, Seok-Jin; Kang, Chong-Yun] Korea Inst Sci & Technol, Elect Mat Res Ctr, Seoul 136791, South Korea. [Shim, Young-Seok; Yoon, Young Soo] Yonsei Univ, Dept Mat Sci & Engn, Seoul 120749, South Korea. [Zhang, Lihua] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. [Kang, Chong-Yun] Korea Univ, KU KIST Grad Sch Converging Sci & Technol, Seoul 136701, South Korea. [Yoon, Young Soo] Gachon Univ, Dept Environm & Energy Engn, Gyeonggi Do 461710, South Korea. RP Shim, YS (reprint author), Seoul Natl Univ, Res Inst Adv Mat, Dept Mat Sci & Engn, Seoul 151744, South Korea. EM benedicto@gachon.ac.kr; cykang@kist.re.kr; hwjang@snu.ac.kr RI Zhang, Lihua/F-4502-2014; Jang, Ho Won/D-9866-2011; OI Jang, Ho Won/0000-0002-6952-7359; Kang, Chong-Yun/0000-0002-4516-8160 FU Korea Ministry of Intelligence and Economy; Korea Institute of Science and Technology; Korea Ministry of Environment; Hi Seoul Science Fellowship from the Seoul Scholarship Foundation FX The authors gratefully acknowledge support from the Korea Ministry of Intelligence and Economy, the Korea Institute of Science and Technology, and a research program of the Korea Ministry of Environment. S.Y.S. is supported by a Hi Seoul Science Fellowship from the Seoul Scholarship Foundation. H. W. J. is grateful to the Fusion Research Program for Green Technologies through the National Research Foundation of Korea. NR 41 TC 22 Z9 23 U1 3 U2 55 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2046-2069 J9 RSC ADV JI RSC Adv. PY 2013 VL 3 IS 26 BP 10452 EP 10459 DI 10.1039/c3ra41331d PG 8 WC Chemistry, Multidisciplinary SC Chemistry GA 160LQ UT WOS:000320121500053 ER PT J AU Gartia, MR Hsiao, A Pokhriyal, A Seo, S Kulsharova, G Cunningham, BT Bond, TC Liu, GL AF Gartia, Manas Ranjan Hsiao, Austin Pokhriyal, Anusha Seo, Sujin Kulsharova, Gulsim Cunningham, Brian T. Bond, Tiziana C. Liu, Gang Logan TI Colorimetric Plasmon Resonance Imaging Using Nano Lycurgus Cup Arrays SO ADVANCED OPTICAL MATERIALS LA English DT Article ID REFRACTIVE-INDEX SENSITIVITY C1 [Kulsharova, Gulsim; Cunningham, Brian T.; Liu, Gang Logan] Univ Illinois, Dept Elect & Comp Engn, Urbana, IL 61801 USA. [Gartia, Manas Ranjan] Univ Illinois, Dept Nucl Plasma & Radiol Engn, Urbana, IL 61801 USA. [Bond, Tiziana C.] Lawrence Livermore Natl Lab, Meso Micro & Nano Technol Ctr, Livermore, CA 94550 USA. [Cunningham, Brian T.; Liu, Gang Logan] Univ Illinois, Dept Bioengn, Urbana, IL 61801 USA. [Pokhriyal, Anusha] Univ Illinois, Dept Phys, Urbana, IL 61801 USA. [Seo, Sujin] Univ Illinois, Dept Mat Sci & Engn, Urbana, IL 61801 USA. [Gartia, Manas Ranjan; Hsiao, Austin; Pokhriyal, Anusha; Seo, Sujin; Kulsharova, Gulsim; Cunningham, Brian T.; Liu, Gang Logan] Univ Illinois, Micro & Nano Technol Lab, Urbana, IL 61801 USA. RP Liu, GL (reprint author), Univ Illinois, Dept Elect & Comp Engn, Urbana, IL 61801 USA. EM loganliu@illinois.edu FU U.S. Department of Energy [DE-FG02-07ER46453, DE-FG02-07ER46471] FX The authors thank Jing Jiang and Te-Wei Chang for help with the SEM. We thank Hoang Nguyen, Cindy Larson for the preparation of master nanopillar mold. Transmission experiments were carried out in the Frederick Seitz Materials Research Laboratory Central Facilities, University of Illinois, which are partially supported by the U.S. Department of Energy under Grants DE-FG02-07ER46453 and DE-FG02-07ER46471. NR 32 TC 42 Z9 42 U1 6 U2 38 PU WILEY-V C H VERLAG GMBH PI WEINHEIM PA BOSCHSTRASSE 12, D-69469 WEINHEIM, GERMANY SN 2195-1071 J9 ADV OPT MATER JI Adv. Opt. Mater. PD JAN PY 2013 VL 1 IS 1 BP 68 EP 76 DI 10.1002/adom.201200040 PG 9 WC Materials Science, Multidisciplinary; Optics SC Materials Science; Optics GA 172IZ UT WOS:000320997600008 ER PT J AU Wheeler, EK Baker, BR Piggott, WT Mabery, SL Hara, CA DeOtte, J Benett, W Mukerjee, EV Dzenitis, J Beer, NR AF Wheeler, E. K. Baker, B. R. Piggott, W. T. Mabery, S. L. Hara, C. A. DeOtte, J. Benett, W. Mukerjee, E. V. Dzenitis, J. Beer, N. R. TI On-chip laser-induced DNA dehybridization SO ANALYST LA English DT Article ID POLYMERASE-CHAIN-REACTION; MICROARRAY; AMPLIFICATION; SELECTION; SYSTEM AB Detection of pathogens and relevant genetic markers using their nucleic acid signatures is extremely common due to the inherent specificity genomic sequences provide. One approach for assaying a sample simultaneously for many different targets is the DNA microarray, which consists of several million short nucleic acid sequences (probes) bound to an inexpensive transparent substrate. Typically, complex samples hybridize to the microarray and the pattern of fluorescing probes on the microarray's surface identifies the detected targets. In the case of evolving or newly emergent organisms, a hybridization pattern can occur that differs from any previously known sources. When this happens it can be useful to recover the hybridized DNA from the binding locations of interest for sequencing. Here we present the novel utilization of a focused Infrared (IR) laser to heat user-selected spots on the DNA microarray surface, causing only localized dehybridization and recovery of the desired DNA into an elution buffer where it is available for subsequent amplification or sequencing. The introduction of a focused dehybridization method for spots of interest suppresses the amount of background DNA to be analyzed from downstream processes, and should reduce subsequent sequence assembly errors. This technique could also be applied to high-density protein microarrays where the desire to locally heat spots for release of bound molecules is desired. C1 [Wheeler, E. K.; DeOtte, J.; Benett, W.; Mukerjee, E. V.; Dzenitis, J.; Beer, N. R.] LLNL, Ctr Micro & Nano Technol, Livermore, CA USA. [Baker, B. R.; Mabery, S. L.; Hara, C. A.] Lawrence Livermore Natl Lab, Phys & Life Sci Directorate, Livermore, CA USA. [Piggott, W. T.] LLNL, Comp Engn Div, Livermore, CA USA. RP Beer, NR (reprint author), LLNL, Ctr Micro & Nano Technol, Livermore, CA USA. EM beer2@llnl.gov RI Baker, Brian/C-1628-2009 FU U.S. Department of Energy by Lawrence Livermore National Laboratory [DE-AC52-07NA27344]; [LDRD 08-ERD-064] FX The authors wish to acknowledge Kelly Spruiell and John Breneman for their assistance. This work was funded by LDRD 08-ERD-064. This work performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344. NR 14 TC 2 Z9 2 U1 3 U2 16 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 13 BP 3692 EP 3696 DI 10.1039/c3an00288h PG 5 WC Chemistry, Analytical SC Chemistry GA 157DT UT WOS:000319876800017 PM 23689934 ER PT J AU Chan, MN Nah, T Wilson, KR AF Chan, Man Nin Nah, Theodora Wilson, Kevin R. TI Real time in situ chemical characterization of sub-micron organic aerosols using Direct Analysis in Real Time mass spectrometry (DART-MS): the effect of aerosol size and volatility SO ANALYST LA English DT Article ID LIQUID PHASE-SEPARATION; VAPOR-PRESSURES; ION-SOURCE; PARTICLES; MORPHOLOGY; COMPONENT; SPLAT AB Direct Analysis in Real Time (DART) mass spectrometry is an atmospheric pressure ionization technique suitable for in situ chemical analysis of organic aerosols. Here, mass spectra are obtained by introducing a stream of nanometer-sized aerosols into the ionization region, which is an open space between the ion source and the atmospheric inlet of mass spectrometer. Model single component aerosols are used to show how the aerosol size and volatility influence the measured ion signals at different DART gas temperatures. The results show that for equivalent aerosol mass concentrations, the ion signal scales with particle surface area, with smaller diameter oleic acid aerosols yielding higher ion signals relative to larger diameter aerosols. For the aerosols of the same size, but different vapor pressures, the ion signal is larger for more volatile succinic acid aerosols than less volatile adipic and suberic acid particles. From the measured changes in aerosol size, produced by the DART source, the radial probing depth for these model aerosols range from 1 to 10 nm, the magnitude of which depends upon the physiochemical properties of the aerosols and DART gas temperature. An aerosol evaporation model reveals that the ion signal is correlated with changes in aerosol size and depends upon the total quantity of evaporated aerosol mass, consistent with a mechanism in which gas-phase molecules are first desorbed from the aerosol surface prior to ionization. The results of this work serve as a basis for future investigations of the mass spectra, ionization pathways, and probing depth of the aerosols using DART. C1 [Chan, Man Nin; Nah, Theodora; Wilson, Kevin R.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. [Nah, Theodora] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. RP Wilson, KR (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. EM krwilson@lbl.gov FU Department of Energy, Office of Science Early Career Research Program through the Chemical Sciences, Geosciences, and Biosciences Division of the U.S. Department of Energy [DE-AC02-05CH11231] FX This work was supported by the Department of Energy, Office of Science Early Career Research Program through the Chemical Sciences, Geosciences, and Biosciences Division of the U.S. Department of Energy under Contract no. DE-AC02-05CH11231. NR 31 TC 16 Z9 16 U1 7 U2 72 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 13 BP 3749 EP 3757 DI 10.1039/c3an00168g PG 9 WC Chemistry, Analytical SC Chemistry GA 157DT UT WOS:000319876800025 PM 23687648 ER PT S AU Lee, TG Pindzola, MS Colgan, J AF Lee, Teck-Ghee Pindzola, M. S. Colgan, J. BE McDaniel, FD Doyle, BL Glass, GA Wang, Y TI Time-Dependent Close-Coupling Study of Antiproton-Impact Ionization of Atoms and Molecules SO APPLICATION OF ACCELERATORS IN RESEARCH AND INDUSTRY SE AIP Conference Proceedings LA English DT Proceedings Paper CT 22nd International Conference on the Application of Accelerators in Research and Industry (CAARI) CY AUG 05-10, 2012 CL Fort Worth, TX SP Sandia Natl Labs, Univ N Texas, Los Alamos Natl Lab, Pacific NW Natl Lab, High Voltage Engn Europa B V, Kurt J Lester Co, Natl Electrostat Corp DE atomic collisions; matter-antimatter interaction; antiproton-impact ionization ID HYDROGEN; HELIUM AB We present our progress in the investigations of atomic and molecular ionization due to antiproton-impact using the time-dependent close-coupling (TDCC) methods. We show some examples of our energy-dependent ionization cross sections for H, He, Li, H-2(+) and H-2 and compare them with the available theoretical and experimental data. C1 [Lee, Teck-Ghee; Pindzola, M. S.] Auburn Univ, Dept Phys, Auburn, AL 36849 USA. [Colgan, J.] Los Alamos Natl Lab, Theoret Div, Los Alamos, NM 87545 USA. RP Lee, TG (reprint author), Auburn Univ, Dept Phys, Auburn, AL 36849 USA. OI Colgan, James/0000-0003-1045-3858 FU US Department of Energy and US National Science Foundation; National Energy Research Scientific Computing Center (NESRC) in Oakland, California; National Institute for Computational Science (NICS) in Knoxville FX This work is supported by the US Department of Energy and US National Science Foundation. The computational work was carried out at the National Energy Research Scientific Computing Center (NESRC) in Oakland, California, USA, and at the National Institute for Computational Science (NICS) in Knoxville, Tennessee, USA. NR 21 TC 0 Z9 0 U1 0 U2 4 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1148-7 J9 AIP CONF PROC PY 2013 VL 1525 BP 32 EP 35 DI 10.1063/1.4802284 PG 4 WC Physics, Applied; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFI58 UT WOS:000319997900005 ER PT S AU Morgan, K Andrianarijaona, V Draganic, IN Defay, X Fogle, M Galindo-Uribarri, A Guillen, CI Havener, CC Hokin, M McCammon, D Nader, DJ Romano, SL Carcoba, FS Sauter, P Seely, D Stancil, PC Vane, CR Vassantachart, AK Wulf, D AF Morgan, K. Andrianarijaona, V. Draganic, I. N. Defay, X. Fogle, M. Galindo-Uribarri, A. Guillen, C. I. Havener, C. C. Hokin, M. McCammon, D. Nader, D. J. Romano, S. L. Salces Carcoba, F. Sauter, P. Seely, D. Stancil, P. C. Vane, C. R. Vassantachart, A. K. Wulf, D. BE McDaniel, FD Doyle, BL Glass, GA Wang, Y TI Charge Exchange X-Ray Emission: Astrophysical Observations And Potential Diagnostics SO APPLICATION OF ACCELERATORS IN RESEARCH AND INDUSTRY SE AIP Conference Proceedings LA English DT Proceedings Paper CT 22nd International Conference on the Application of Accelerators in Research and Industry (CAARI) CY AUG 05-10, 2012 CL Fort Worth, TX SP Sandia Natl Labs, Univ N Texas, Los Alamos Natl Lab, Pacific NW Natl Lab, High Voltage Engn Europa B V, Kurt J Lester Co, Natl Electrostat Corp DE charge transfer; state-selective; laboratory astrophysics; X-ray spectra; interstellar medium ID SOLAR-WIND; INTERSTELLAR NEUTRALS; ROCKET; COMETS; LIMITS; GAS AB Interest in astrophysical sources of charge exchange X-rays has been growing steadily since the discovery of X-ray emission from the comet Hyakutake with ROSAT in 1996. Since then, charge exchange has been observed between solar wind ions and neutrals in the geocorona and in the atmospheres of Mars and Jupiter. Charge exchange with interstellar neutrals within the heliosphere between solar wind ions and neutral hydrogen and helium from the interstellar medium is now acknowledged as contributing a considerable (although currently unknown) fraction of the soft X-ray background. We make a brief survey of the heliospheric, Galactic, and extragalactic systems in which charge exchange has been observed or is predicted to take place. Experiments measuring velocity dependent cross-section and line ratios for Lyman-series lines and He-like triplets are needed to check current theoretical models of charge exchange emission and aid interpretation of observations. We point out a number of systems that are of astrophysical interest that could be the subject of future laboratory investigations, particularly velocity dependent line ratios of the X-ray emission produced by charge exchange between highly ionized common elements (such as O, C, Ne, and Fe) and atomic hydrogen and helium. To begin to address the need for laboratory data we have measured velocity dependent Ly-series line ratios for C6+ ions interacting with H-2, He, and Kr gas targets at Oak Ridge National Laboratory's Ion-Atom Merged-Beams Apparatus C1 [Morgan, K.; Defay, X.; Hokin, M.; McCammon, D.; Sauter, P.; Wulf, D.] Univ Wisconsin, Dept Phys, 1150 Univ Ave, Madison, WI 53706 USA. [Draganic, I. N.; Galindo-Uribarri, A.; Havener, C. C.; Vane, C. R.] Oak Ridge Natl Lab, Div Phys, Oak Ridge, TN 37831 USA. [Andrianarijaona, V.; Guillen, C. I.; Romano, S. L.; Vassantachart, A. K.] Pacific Union Coll, Dept Phys, Angwin, CA 94508 USA. [Salces Carcoba, F.] Univ Autonoma San Luis Potosi, Fac Ciencias, San Luis Potosi 78290, Mexico. [Nader, D. J.] Univ Veracruzana, Fac Fis, Skopje 91000, Macedonia. [Fogle, M.] Auburn Univ, Dept Phys, Auburn, AL 36849 USA. [Seely, D.] Albion Coll, Dept Phys, Albion, MI 49224 USA. [Stancil, P. C.] Univ Georgia, Dept Phys, Athens, GA 30602 USA. RP Morgan, K (reprint author), Univ Wisconsin, Dept Phys, 1150 Univ Ave, Madison, WI 53706 USA. RI Morgan, Kelsey/J-5053-2016 OI Morgan, Kelsey/0000-0002-6597-1030 NR 37 TC 1 Z9 1 U1 0 U2 5 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1148-7 J9 AIP CONF PROC PY 2013 VL 1525 BP 49 EP 54 DI 10.1063/1.4802288 PG 6 WC Physics, Applied; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFI58 UT WOS:000319997900009 ER PT S AU Beiersdorfer, P Brown, GV Clementson, J Kilbourne, CA Kelley, RL Leutenegger, MA Porter, FS Schweikhard, L AF Beiersdorfer, P. Brown, G. V. Clementson, J. Kilbourne, C. A. Kelley, R. L. Leutenegger, M. A. Porter, F. S. Schweikhard, L. BE McDaniel, FD Doyle, BL Glass, GA Wang, Y TI Unresolved Puzzles In The X-Ray Emission Produced By Charge Exchange Measured On Electron Beam Ion Traps SO APPLICATION OF ACCELERATORS IN RESEARCH AND INDUSTRY SE AIP Conference Proceedings LA English DT Proceedings Paper CT 22nd International Conference on the Application of Accelerators in Research and Industry (CAARI) CY AUG 05-10, 2012 CL Fort Worth, TX SP Sandia Natl Labs, Univ N Texas, Los Alamos Natl Lab, Pacific NW Natl Lab, High Voltage Engn Europa B V, Kurt J Lester Co, Natl Electrostat Corp (NEC) DE Charge exchange; x-ray spectra ID MAGNETIC TRAPPING MODE; SOLAR-WIND; NEUTRAL HYDROGEN; EXCITED-STATES; SPECTROMETER; COMETS; POPULATION; ENERGY AB Charge exchange recombination, the transfer of one or more electrons from an atomic or molecular system to a positive ion, is a common phenomenon affecting laboratory and astrophysical plasmas. Controlled studies of this process in electron beam ion traps during the past one and a half decades have produced multiple observations that are difficult to explain with available spectral models. Some of the most recent observations are so puzzling that they bring in doubt the existence of a coherent predictive capability for line formation by charge exchange, making investigations of charge exchange a fertile ground for continued measurements and theoretical development. C1 [Beiersdorfer, P.; Brown, G. V.; Clementson, J.] Lawrence Livermore Natl Lab, Div Phys, Livermore, CA 94550 USA. [Schweikhard, L.] Ernst Moritz Arndt Univ Greifswald, Inst Phys, D-17487 Greifswald, Germany. RP Beiersdorfer, P (reprint author), Lawrence Livermore Natl Lab, Div Phys, 7000 East Ave, Livermore, CA 94550 USA. RI Porter, Frederick/D-3501-2012 OI Porter, Frederick/0000-0002-6374-1119 NR 27 TC 0 Z9 0 U1 0 U2 2 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1148-7 J9 AIP CONF PROC PY 2013 VL 1525 BP 60 EP 63 DI 10.1063/1.4802290 PG 4 WC Physics, Applied; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFI58 UT WOS:000319997900011 ER PT S AU Clementson, J Beiersdorfer, P Lennartsson, T AF Clementson, J. Beiersdorfer, P. Lennartsson, T. BE McDaniel, FD Doyle, BL Glass, GA Wang, Y TI Atomic Data Of Tungsten For Current And Future Uses In Fusion And Plasma Science SO APPLICATION OF ACCELERATORS IN RESEARCH AND INDUSTRY SE AIP Conference Proceedings LA English DT Proceedings Paper CT 22nd International Conference on the Application of Accelerators in Research and Industry (CAARI) CY AUG 05-10, 2012 CL Fort Worth, TX SP Sandia Natl Labs, Univ N Texas, Los Alamos Natl Lab, Pacific NW Natl Lab, High Voltage Engn Europa B V, Kurt J Lester Co, Natl Electrostat Corp DE spectroscopic plasma diagnostics; atomic data; tungsten; tokamak; ITER; EBIT ID BEAM ION-TRAP; X-RAY SPECTROSCOPY; SPECTRA; SPECTROMETER; RADIATION; ENERGIES; KRYPTON; LINES; CODE AB Atomic physics has played an important role throughout the history of experimental plasma physics. For example, accurate knowledge of atomic properties has been crucial for understanding the plasma energy balance and for diagnostic development. With the shift in magnetic fusion research toward high-temperature burning plasmas like those expected to be produced in the ITER tokamak, the atomic physics of tungsten has become important. Tungsten will be a constituent of ITER plasmas because of its use as a plasma-facing material able to withstand high heat loads with lower tritium retention than other possible materials. Already, ITER diagnostics are being developed based on using tungsten radiation. In particular, the ITER Core Imaging X-ray Spectrometer (CIXS), which is designed to measure the core ion temperature and bulk plasma motion, is being based on the x-ray emission of neonlike tungsten ions (W64+). In addition, tungsten emission will at ITER be measured by extreme ultraviolet (EUV) and optical spectrometers to determine its concentration in the plasma and to assess power loss and tungsten sputtering rates. On present-day tokamaks tungsten measurements are therefore being performed in preparation of ITER. Tungsten has very complex spectra and most are still unknown. The WOLFRAM project at Livermore aims to produce data for tungsten in various spectral bands: L-shell x-ray emission for CIXS development, soft x-ray and EUV M-and N-shell tungsten emission for understanding the edge radiation from ITER plasmas as well as from contemporary tokamaks, and O-shell emission for developing spectral diagnostics of the ITER divertor. C1 [Clementson, J.; Beiersdorfer, P.] Lawrence Livermore Natl Lab, Div Phys, POB 808, Livermore, CA 94551 USA. RP Clementson, J (reprint author), Lawrence Livermore Natl Lab, Div Phys, POB 808, Livermore, CA 94551 USA. NR 51 TC 8 Z9 9 U1 1 U2 17 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1148-7 J9 AIP CONF PROC PY 2013 VL 1525 BP 78 EP 83 DI 10.1063/1.4802294 PG 6 WC Physics, Applied; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFI58 UT WOS:000319997900015 ER PT S AU Vainionpaa, JH Harris, JL Piestrup, MA Gary, CK Williams, DL Apodaca, MD Cremer, JT Ji, Q Ludewigt, BA Jones, G AF Vainionpaa, J. H. Harris, J. L. Piestrup, M. A. Gary, C. K. Williams, D. L. Apodaca, M. D. Cremer, J. T. Ji, Qing Ludewigt, B. A. Jones, G. BE McDaniel, FD Doyle, BL Glass, GA Wang, Y TI High Yield Neutron Generators Using The DD Reaction SO APPLICATION OF ACCELERATORS IN RESEARCH AND INDUSTRY SE AIP Conference Proceedings LA English DT Proceedings Paper CT 22nd International Conference on the Application of Accelerators in Research and Industry (CAARI) CY AUG 05-10, 2012 CL Fort Worth, TX SP Sandia Natl Labs, Univ N Texas, Los Alamos Natl Lab, Pacific NW Natl Lab, High Voltage Engn Europa B V, Kurt J Lester Co, Natl Electrostat Corp DE Neutron generators; ion sources; neutron tubes; electron cyclotron resonance AB A product line of high yield neutron generators has been developed at Adelphi technology inc. The generators use the D-D fusion reaction and are driven by an ion beam supplied by a microwave ion source. Yields of up to 5 x 10(9) n/s have been achieved, which are comparable to those obtained using the more efficient D-T reaction. The microwave-driven plasma uses the electron cyclotron resonance (ECR) to produce a high plasma density for high current and high atomic ion species. These generators have an actively pumped vacuum system that allows operation at reduced pressure in the target chamber, increasing the overall system reliability. Since no radioactive tritium is used, the generators can be easily serviced, and components can be easily replaced, providing essentially an unlimited lifetime. Fast neutron source size can be adjusted by selecting the aperture and target geometries according to customer specifications. Pulsed and continuous operation has been demonstrated. Minimum pulse lengths of 50 mu s have been achieved. Since the generators are easily serviceable, they offer a long lifetime neutron generator for laboratories and commercial systems requiring continuous operation. Several of the generators have been enclosed in radiation shielding/moderator structures designed for customer specifications. These generators have been proven to be useful for prompt gamma neutron activation analysis (PGNAA), neutron activation analysis (NAA) and fast neutron radiography. Thus these generators make excellent fast, epithermal and thermal neutron sources for laboratories and industrial applications that require neutrons with safe operation, small footprint, low cost and small regulatory burden. C1 [Vainionpaa, J. H.; Harris, J. L.; Piestrup, M. A.; Gary, C. K.; Williams, D. L.; Apodaca, M. D.; Cremer, J. T.] Adelphi Technol, 2003 E Bayshore Rd 94061, Redwood City, CA 94063 USA. [Ji, Qing; Ludewigt, B. A.] Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Jones, G.] G&J Enterprise, Pleasanton, CA 94566 USA. RP Vainionpaa, JH (reprint author), Adelphi Technol, 2003 E Bayshore Rd 94061, Redwood City, CA 94063 USA. FU DOE [DE-FG02-04ER86177, DE-FG02-04ER86294]; DHS [HSHQDC-10-C-00196, HSHQDC-09-C-0008] FX Much of the technology used in these generators was developed under DOE grants DE-FG02-04ER86177 and DE-FG02-04ER86294, and DHS grants HSHQDC-10-C-00196 and HSHQDC-09-C-0008. NR 9 TC 2 Z9 2 U1 2 U2 12 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1148-7 J9 AIP CONF PROC PY 2013 VL 1525 BP 118 EP 122 DI 10.1063/1.4802303 PG 5 WC Physics, Applied; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFI58 UT WOS:000319997900024 ER PT S AU Sy, A Ji, Q Persaud, A Ludewigt, BA Schenkel, T AF Sy, A. Ji, Q. Persaud, A. Ludewigt, B. A. Schenkel, T. BE McDaniel, FD Doyle, BL Glass, GA Wang, Y TI Ion Source And Beam Guiding Studies For An API Neutron Generator SO APPLICATION OF ACCELERATORS IN RESEARCH AND INDUSTRY SE AIP Conference Proceedings LA English DT Proceedings Paper CT 22nd International Conference on the Application of Accelerators in Research and Industry (CAARI) CY AUG 05-10, 2012 CL Fort Worth, TX SP Sandia Natl Labs, Univ N Texas, Los Alamos Natl Lab, Pacific NW Natl Lab, High Voltage Engn Europa B V, Kurt J Lester Co, Natl Electrostat Corp (NEC) DE Penning ion source; Associated particle imaging; Neutron generator ID TAPERED GLASS-CAPILLARY; SYSTEM; RADIOGRAPHY AB Recently developed neutron imaging methods require high neutron yields for fast imaging times and small beam widths for good imaging resolution. For ion sources with low current density to be viable for these types of imaging methods, large extraction apertures and beam focusing must be used. We present recent work on the optimization of a Penning-type ion source for neutron generator applications. Two multi-cusp magnet configurations have been tested and are shown to increase the extracted ion current density over operation without multi-cusp magnetic fields. The use of multi-cusp magnetic confinement and gold electrode surfaces have resulted in increased ion current density, up to 2.2 mA/cm(2). Passive beam focusing using tapered dielectric capillaries has been explored due to its potential for beam compression without the cost and complexity issues associated with active focusing elements. Initial results from first experiments indicate the possibility of beam compression. Further work is required to evaluate the viability of such focusing methods for associated particle imaging (API) systems. C1 [Sy, A.; Ji, Q.; Persaud, A.; Ludewigt, B. A.; Schenkel, T.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Sy, A (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, 1 Cyclotron Rd, Berkeley, CA 94720 USA. NR 12 TC 0 Z9 0 U1 3 U2 8 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1148-7 J9 AIP CONF PROC PY 2013 VL 1525 BP 123 EP 127 DI 10.1063/1.4802304 PG 5 WC Physics, Applied; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFI58 UT WOS:000319997900025 ER PT S AU Ellsworth, JL Tang, V Falabella, S Naranjo, B Putterman, S AF Ellsworth, J. L. Tang, V. Falabella, S. Naranjo, B. Putterman, S. BE McDaniel, FD Doyle, BL Glass, GA Wang, Y TI Neutron Production Using A Pyroelectric Driven Target Coupled With A Gated Field Ionization Source SO APPLICATION OF ACCELERATORS IN RESEARCH AND INDUSTRY SE AIP Conference Proceedings LA English DT Proceedings Paper CT 22nd International Conference on the Application of Accelerators in Research and Industry (CAARI) CY AUG 05-10, 2012 CL Fort Worth, TX SP Sandia Natl Labs, Univ N Texas, Los Alamos Natl Lab, Pacific NW Natl Lab, High Voltage Engn Europa B V, Kurt J Lester Co, Natl Electrostat Corp DE Neutron source; pyroelectric crystal; field ionization ID CRYSTAL AB A palm sized, portable neutron source would be useful for widespread implementation of detection systems for shielded, special nuclear material. We present progress towards the development of the components for an ultra-compact neutron generator using a pulsed, meso-scale field ionization source, a deuterated (or tritiated) titanium target driven by a negative high voltage lithium tantalate crystal. Neutron production from integrated tests using an ion source with a single, biased tungsten tip and a 3x1 cm, vacuum insulated crystal with a plastic deuterated target are presented. Component testing of the ion source with a single tip produces up to 3 nA of current. Dielectric insulation of the lithium tantalate crystals appears to reduce flashover, which should improve the robustness. The field emission losses from a 3 cm diameter crystal with a plastic target and 6 cm diameter crystal with a metal target are compared. C1 [Ellsworth, J. L.; Tang, V.; Falabella, S.] Lawrence Livermore Natl Lab, 7000 East Ave, Livermore, CA 94550 USA. [Naranjo, B.; Putterman, S.] Univ Calif Los Angeles, Los Angeles, CA 90095 USA. RP Ellsworth, JL (reprint author), Lawrence Livermore Natl Lab, 7000 East Ave, Livermore, CA 94550 USA. FU U.S. Department of Energy by Lawrence Livermore National Laboratory [DE-AC52-07NA27344]; U.S. Department of Energy NA-22 Office of Nonproliferation Research and Development under the Special Nuclear Materials Movement Detection portfolio FX The authors would like to thank Phil Kerr for assistance with the calibration of the neutron backpack diagnostic. This work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344 and supported by the U.S. Department of Energy NA-22 Office of Nonproliferation Research and Development under the Special Nuclear Materials Movement Detection portfolio. NR 12 TC 4 Z9 4 U1 0 U2 5 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1148-7 J9 AIP CONF PROC PY 2013 VL 1525 BP 128 EP 132 DI 10.1063/1.4802305 PG 5 WC Physics, Applied; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFI58 UT WOS:000319997900026 ER PT S AU Field, KG Wetteland, CJ Cao, G Maier, BR Dickerson, C Gerczak, TJ Field, CR Kriewaldt, K Sridharan, K Allen, TR AF Field, K. G. Wetteland, C. J. Cao, G. Maier, B. R. Dickerson, C. Gerczak, T. J. Field, C. R. Kriewaldt, K. Sridharan, K. Allen, T. R. BE McDaniel, FD Doyle, BL Glass, GA Wang, Y TI University of Wisconsin Ion Beam Laboratory: A Facility for Irradiated Materials and Ion Beam Analysis SO APPLICATION OF ACCELERATORS IN RESEARCH AND INDUSTRY SE AIP Conference Proceedings LA English DT Proceedings Paper CT 22nd International Conference on the Application of Accelerators in Research and Industry (CAARI) CY AUG 05-10, 2012 CL Fort Worth, TX SP Sandia Natl Labs, Univ N Texas, Los Alamos Natl Lab, Pacific NW Natl Lab, High Voltage Engn Europa B V, Kurt J Lester Co, Natl Electrostat Corp DE Ion Beam; TORVIS; Nuclear Materials; Radiation Damage ID MECHANICAL-PROPERTIES; CARBIDE; MICROSTRUCTURE; COATINGS AB The University of Wisconsin Ion Beam Laboratory (UW-IBL) has recently undergone significant infrastructure upgrades to facilitate graduate level research in irradiated materials phenomena and ion beam analysis. A National Electrostatics Corp. (NEC) Torodial Volume Ion Source (TORVIS), the keystone upgrade for the facility, can produce currents of hydrogen ions and helium ions up to similar to 200 mu A and similar to 5 mu A, respectively. Recent upgrades also include RBS analysis packages, end station developments for irradiation of relevant material systems, and the development of an in-house touch screen based graphical user interface for ion beam monitoring. Key research facilitated by these upgrades includes irradiation of nuclear fuels, studies of interfacial phenomena under irradiation, and clustering dynamics of irradiated oxide dispersion strengthened steels. The UW-IBL has also partnered with the Advanced Test Reactor National Scientific User Facility (ATR-NSUF) to provide access to the irradiation facilities housed at the UW-IBL as well as access to post irradiation facilities housed at the UW Characterization Laboratory for Irradiated Materials (CLIM) and other ATR-NSUF partner facilities. Partnering allows for rapid turnaround from proposed research to finalized results through the ATR-NSUF rapid turnaround proposal system. An overview of the UW-IBL including CLIM and relevant research is summarized. C1 [Field, K. G.; Wetteland, C. J.; Cao, G.; Maier, B. R.; Gerczak, T. J.; Kriewaldt, K.; Sridharan, K.; Allen, T. R.] Univ Wisconsin, Madison, WI 53706 USA. [Dickerson, C.] Argonne Natl Lab, Argonne, IL 60439 USA. [Field, C. R.] Naval Res Lab, Washington, DC 20375 USA. RP Field, KG (reprint author), Univ Wisconsin, Madison, WI 53706 USA. RI Field, Kevin/K-1942-2013; OI Field, Kevin/0000-0002-3105-076X; Allen, Todd/0000-0002-2372-7259; Gerczak, Tyler/0000-0001-9967-3579 NR 20 TC 2 Z9 3 U1 0 U2 11 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1148-7 J9 AIP CONF PROC PY 2013 VL 1525 BP 159 EP 164 DI 10.1063/1.4802311 PG 6 WC Physics, Applied; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFI58 UT WOS:000319997900032 ER PT S AU Potter, JM Krawczyk, FL AF Potter, James M. Krawczyk, Frank L. BE McDaniel, FD Doyle, BL Glass, GA Wang, Y TI Resonant Coupling Applied To Superconducting Accelerator Structures SO APPLICATION OF ACCELERATORS IN RESEARCH AND INDUSTRY SE AIP Conference Proceedings LA English DT Proceedings Paper CT 22nd International Conference on the Application of Accelerators in Research and Industry (CAARI) CY AUG 05-10, 2012 CL Fort Worth, TX SP Sandia Natl Labs, Univ N Texas, Los Alamos Natl Lab, Pacific NW Natl Lab, High Voltage Engn Europa B V, Kurt J Lester Co, Natl Electrostat Corp DE linear accelerator; superconducting accelerator; resonant coupling AB The concept of resonant coupling and the benefits that accrue from its application is well known in the world of room temperature coupled cavity linacs. Design studies show that it can be applied successfully between sections of conventional elliptical superconducting coupled cavity accelerator structures and internally to structures with spoked cavity resonators. The coupling mechanisms can be designed without creating problems with high field regions or multipactoring. The application of resonant coupling to superconducting accelerators eliminates the need for complex cryogenic mechanical tuners and reduces the time needed to bring a superconducting accelerator into operation. C1 [Potter, James M.] JP Accelerator Works Inc, 2245 47th St, Los Alamos, NM 87544 USA. [Krawczyk, Frank L.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Potter, JM (reprint author), JP Accelerator Works Inc, 2245 47th St, Los Alamos, NM 87544 USA. OI Krawczyk, Frank/0000-0001-8306-2562 FU Los Alamos National Laboratory with the Office of Naval Research [N00014-10-M-0328] FX This work was done by JP Accelerator Works, Inc. and Los Alamos National Laboratory under contract N00014-10-M-0328 with the Office of Naval Research. NR 3 TC 0 Z9 0 U1 0 U2 1 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1148-7 J9 AIP CONF PROC PY 2013 VL 1525 BP 184 EP 189 DI 10.1063/1.4802316 PG 6 WC Physics, Applied; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFI58 UT WOS:000319997900037 ER PT S AU Sooby, E Adams, M Baty, A Gerity, J McIntyre, P Melconian, K Phongikaroon, S Pogue, N Sattarov, A Simpson, M Tripathy, P Tsevkov, P AF Sooby, Elizabeth Adams, Marvin Baty, Austin Gerity, James McIntyre, Peter Melconian, Karie Phongikaroon, Supathorn Pogue, Nathaniel Sattarov, Akhdiyor Simpson, Michael Tripathy, Prabhat Tsevkov, Pavel BE McDaniel, FD Doyle, BL Glass, GA Wang, Y TI Molten Salt Considerations For Accelerator-Driven Subcritical Fission To Close The Nuclear Fuel Cycle SO APPLICATION OF ACCELERATORS IN RESEARCH AND INDUSTRY SE AIP Conference Proceedings LA English DT Proceedings Paper CT 22nd International Conference on the Application of Accelerators in Research and Industry (CAARI) CY AUG 05-10, 2012 CL Fort Worth, TX SP Sandia Natl Labs, Univ N Texas, Los Alamos Natl Lab, Pacific NW Natl Lab, High Voltage Engn Europa B V, Kurt J Lester Co, Natl Electrostat Corp DE Accelerator Driven System (ADS); Molten Salt Reactor (MSR); Used Nuclear Fuel (UNF); Transuranic (TRU) Waste; Long-Lived Fission Products; Neutronics ID IONS AB The host salt selection, molecular modeling, physical chemistry, and processing chemistry are presented here for an accelerator-driven subcritical fission in a molten salt core (ADSMS). The core is fueled solely with the transuranics (TRU) and long-lived fission products (LFP) from used nuclear fuel. The neutronics and salt composition are optimized to destroy the transuranics by fission and the long-lived fission products by transmutation. The cores are driven by proton beams from a strong-focusing cyclotron stack. One such ADSMS system can destroy the transuranics in the used nuclear fuel produced by a 1GWe conventional reactor. It uniquely provides a method to close the nuclear fuel cycle for green nuclear energy. C1 [Sooby, Elizabeth; Baty, Austin; Gerity, James; McIntyre, Peter; Melconian, Karie; Pogue, Nathaniel; Sattarov, Akhdiyor] Texas A&M Univ, Dept Phys & Astron, 4242 TAMU, College Stn, TX 77843 USA. [Adams, Marvin; Tsevkov, Pavel] Texas A&M Univ, Nucl Engn, College Stn, TX 77843 USA. [Phongikaroon, Supathorn] Univ Idaho, Ctr Adv Energy Studies, Idaho Falls, ID 83401 USA. [Simpson, Michael; Tripathy, Prabhat] Idaho Natl Lab, Idaho Falls, ID 83415 USA. RP Sooby, E (reprint author), Texas A&M Univ, Dept Phys & Astron, 4242 TAMU, College Stn, TX 77843 USA. RI Melconian, Karie/H-9518-2013 OI Melconian, Karie/0000-0003-2006-0441 FU Mitchell Family Foundation; State of Texas ASE Fund FX This work is supported by grants from the Mitchell Family Foundation and the State of Texas ASE Fund. Special thanks to Dr. Mathieu Salanne of the University of Pierre and Marie Currie, Paris, France, Prof. Paul Madden, The University of Oxford at Queens College, and Ondrej Benes, Institute of Transuranium elements, Karlsruhe, Germany for their help with both the modeling work presented here as well as their conceptual input in the development of these system-specific models. NR 12 TC 0 Z9 0 U1 0 U2 12 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1148-7 J9 AIP CONF PROC PY 2013 VL 1525 BP 230 EP 235 DI 10.1063/1.4802325 PG 6 WC Physics, Applied; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFI58 UT WOS:000319997900046 ER PT S AU Takahashi, K Okamura, M Sekine, M Cushing, E Jandovitz, P AF Takahashi, Kazumasa Okamura, Masahiro Sekine, Megumi Cushing, Eric Jandovitz, Peter BE McDaniel, FD Doyle, BL Glass, GA Wang, Y TI Effect Of Solenoidal Magnetic Field On Drifting Laser Plasma SO APPLICATION OF ACCELERATORS IN RESEARCH AND INDUSTRY SE AIP Conference Proceedings LA English DT Proceedings Paper CT 22nd International Conference on the Application of Accelerators in Research and Industry (CAARI) CY AUG 05-10, 2012 CL Fort Worth, TX SP Sandia Natl Labs, Univ N Texas, Los Alamos Natl Lab, Pacific NW Natl Lab, High Voltage Engn Europa B V, Kurt J Lester Co, Natl Electrostat Corp DE laser ion source; solenoid; ablation plasma AB An ion source for accelerators requires to provide a stable waveform with a certain pulse length appropriate to the application. The pulse length of laser ion source is easy to control because it is expected to be proportional to plasma drifting distance. However, current density decay is proportional to the cube of the drifting distance, so large current loss will occur under unconfined drift. We investigated the stability and current decay of a Nd:YAG laser generated copper plasma confined by a solenoidal field using a Faraday cup to measure the current waveform. It was found that the plasma was unstable at certain magnetic field strengths, so a baffle was introduced to limit the plasma diameter at injection and improve the stability. Magnetic field, solenoid length, and plasma diameter were varied in order to find the conditions that minimize current decay and maximize stability. C1 [Takahashi, Kazumasa; Sekine, Megumi] Tokyo Inst Technol, Yokohama, Kanagawa 2268502, Japan. [Okamura, Masahiro] Brookhaven Natl Lab, Upton, NY 11973 USA. [Okamura, Masahiro] RIKEN, Wako, Saitama 3510198, Japan. [Cushing, Eric] Penn State Univ, University Pk, PA 16802 USA. [Jandovitz, Peter] Cornell Univ, Ithaca, NY 14853 USA. RP Takahashi, K (reprint author), Tokyo Inst Technol, Yokohama, Kanagawa 2268502, Japan. NR 8 TC 9 Z9 9 U1 1 U2 3 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1148-7 J9 AIP CONF PROC PY 2013 VL 1525 BP 241 EP 244 DI 10.1063/1.4802327 PG 4 WC Physics, Applied; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFI58 UT WOS:000319997900048 ER PT S AU Sattarov Assadi, S Badgley, K Baty, A Comeaux, J Gerity, J Kellams, J Mcintyre, P Pogue, N Sooby, E Tsvetkov, P Rosaire, G Mann, T AF Sattarov Assadi, S. Badgley, K. Baty, A. Comeaux, J. Gerity, J. Kellams, J. Mcintyre, P. Pogue, N. Sooby, E. Tsvetkov, P. Rosaire, G. Mann, T. BE McDaniel, FD Doyle, BL Glass, GA Wang, Y TI Neutronics Of Accelerator-Driven Subcritical Fission For Burning Transuranics In Used Nuclear Fuel SO APPLICATION OF ACCELERATORS IN RESEARCH AND INDUSTRY SE AIP Conference Proceedings LA English DT Proceedings Paper CT 22nd International Conference on the Application of Accelerators in Research and Industry (CAARI) CY AUG 05-10, 2012 CL Fort Worth, TX SP Sandia Natl Labs, Univ N Texas, Los Alamos Natl Lab, Pacific NW Natl Lab, High Voltage Engn Europa B V, Kurt J Lester Co, Natl Electrostat Corp DE fission; ADS; molten salt; subcritical AB We report the development of a conceptual design for accelerator-driven subcritical fission in a molten salt core (ADSMS). ADSMS is capable of destroying all of the transuranics at the same rate and proportion as they are produced in a conventional nuclear power plant. The ADSMS core is fueled solely by transuranics extracted from used nuclear fuel and reduces its radiotoxicity by a factor 10,000. ADSMS offers a way to close the nuclear fuel cycle so that the full energy potential in the fertile fuels uranium and thorium can be recovered. C1 [Sattarov; Assadi, S.; Badgley, K.; Comeaux, J.; Gerity, J.; Kellams, J.; Mcintyre, P.; Pogue, N.; Sooby, E.; Tsvetkov, P.; Rosaire, G.] Texas A&M Univ, College Stn, TX 77845 USA. [Mann, T.] Argonne Natl Lab, Argone, IL USA. RP Sattarov (reprint author), Texas A&M Univ, College Stn, TX 77845 USA. RI Melconian, Karie/H-9518-2013 OI Melconian, Karie/0000-0003-2006-0441 NR 1 TC 0 Z9 0 U1 0 U2 2 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1148-7 J9 AIP CONF PROC PY 2013 VL 1525 BP 245 EP 250 DI 10.1063/1.4802328 PG 6 WC Physics, Applied; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFI58 UT WOS:000319997900049 ER PT S AU Rajasekhara, S Doyle, BL Enos, DG Clark, BG AF Rajasekhara, S. Doyle, B. L. Enos, D. G. Clark, B. G. BE McDaniel, FD Doyle, BL Glass, GA Wang, Y TI Hydrogen Uptake In Zircaloy-2 Reactor Fuel Claddings Studied With Elastic Recoil Detection SO APPLICATION OF ACCELERATORS IN RESEARCH AND INDUSTRY SE AIP Conference Proceedings LA English DT Proceedings Paper CT 22nd International Conference on the Application of Accelerators in Research and Industry (CAARI) CY AUG 05-10, 2012 CL Fort Worth, TX SP Sandia Natl Labs, Univ N Texas, Los Alamos Natl Lab, Pacific NW Natl Lab, High Voltage Engn Europa B V, Kurt J Lester Co, Natl Electrostat Corp (NEC) DE Elastic recoil detection; hydrogen uptake; nuclear cladding; spent nuclear fuel; Zircaloy-2; transmission electron microscopy ID ALPHA-ZIRCONIUM; ION-BEAM; DIFFUSION; KINETICS; ABSORPTION; SOLUBILITY; CORROSION; MECHANISM; ALLOYS; TUBES AB The recent trend towards a high burn-up discharge spent nuclear fuel necessitates a thorough understanding of hydrogen uptake in Zr-based cladding materials that encapsulate spent nuclear fuel. Although it is challenging to experimentally replicate exact conditions in a nuclear reactor that lead to hydrogen uptake in claddings, in this study we have attempted to understand the kinetics of hydrogen uptake by first electrolytically charging Zircaloy-2 (Zr-2) cladding material for various durations (100 to 2,600 s), and subsequently examining hydrogen ingress with elastic recoil detection (ERD) and transmission electron microscopy (TEM). To understand the influence of irradiation damage defects on hydrogen uptake, an analogous study was performed on ion - irradiated (0.1, 1 and 25 dpa) Zr-2. Analysis of ERD data from the un-irradiated Zr-2 suggests that the growth of the hydride layer is diffusion controlled, and preliminary TEM results support this assertion. In un-irradiated Zr-2, the diffusivity of hydrogen in the hydride phase was found to be approximately 1.1 x 10(-11) cm(2)/s, while the diffusivity in the hydride phase for lightly irradiated (0.1 and 1 dpa) Zr-2 is an order of magnitude lower. Irradiation to 25 dpa results in a hydrogen diffusivity that is comparable to the un-irradiated Zr-2. These results are compared with existing literature on hydrogen transport in Zr - based materials. C1 [Rajasekhara, S.; Doyle, B. L.; Enos, D. G.; Clark, B. G.] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Rajasekhara, S (reprint author), Sandia Natl Labs, POB 5800, Albuquerque, NM 87185 USA. NR 35 TC 0 Z9 0 U1 3 U2 18 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1148-7 J9 AIP CONF PROC PY 2013 VL 1525 BP 270 EP 275 DI 10.1063/1.4802332 PG 6 WC Physics, Applied; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFI58 UT WOS:000319997900053 ER PT S AU Gregory, E Chemerisov, SD Vandegrift, GF Woloshun, KA Kelsey, CT Tkac, P Makarashvili, V Jonah, CD Olivas, ER Holloway, MA Hurtle, KP Romero, FP Dalmas, DA Harvey, JT AF Dale, Gregory E. Chemerisov, Sergey D. Vandegrift, George F. Woloshun, Keith A. Kelsey, Charles T. Tkac, Peter Makarashvili, Vakho Jonah, Charles D. Olivas, Eric R. Holloway, Michael A. Hurtle, Ken P. Romero, Frank P. Dalmas, Dale A. Harvey, James T. BE McDaniel, FD Doyle, BL Glass, GA Wang, Y TI Design and Experimental Activities Supporting Commercial US Electron Accelerator Production of Mo-99 SO APPLICATION OF ACCELERATORS IN RESEARCH AND INDUSTRY SE AIP Conference Proceedings LA English DT Proceedings Paper CT 22nd International Conference on the Application of Accelerators in Research and Industry (CAARI) CY AUG 05-10, 2012 CL Fort Worth, TX SP Sandia Natl Labs, Univ N Texas, Los Alamos Natl Lab, Pacific NW Natl Lab, High Voltage Engn Europa B V, Kurt J Lester Co, Natl Electrostat Corp DE Accelerator Production of Medical Radioisotopes; Accelerator Target Design; Accelerator Target Cooling AB Tc-99m, the daughter isotope of Mo-99, is the most commonly used radioisotope for nuclear medicine in the United States. Under the direction of the National Nuclear Security Administration (NNSA), Los Alamos National Laboratory (LANL) and Argonne National Laboratory (ANL) are partnering with NorthStar Medical Technologies to demonstrate the viability of large-scale Mo-99 production using electron accelerators. In this process, Mo-99 is produced in an enriched Mo-100 target through the Mo-100(gamma,n)Mo-99 reaction. Five experiments have been performed to date at ANL to demonstrate this process. This paper reviews the current status of these activities, specifically the design and performance of the helium gas target cooling system. C1 [Dale, Gregory E.; Woloshun, Keith A.; Kelsey, Charles T.; Olivas, Eric R.; Holloway, Michael A.; Hurtle, Ken P.; Romero, Frank P.; Dalmas, Dale A.] Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. [Chemerisov, Sergey D.; Vandegrift, George F.; Tkac, Peter; Makarashvili, Vakho; Jonah, Charles D.] Argonne Natl Lab, LLC, Argonne, IL 60439 USA. [Harvey, James T.] NorthStar Med Technol, LLC, Madison, WI 53718 USA. RP Gregory, E (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM gedale@lanl.gov; chemerisov@anl.gov; jharvey@northstarnm.com OI Olivas, Eric/0000-0002-7721-6622 FU National Nuclear Security Administration FX This work was funded by the National Nuclear Security Administrations Global Threat Reduction Initiative. NR 3 TC 0 Z9 0 U1 2 U2 5 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1148-7 J9 AIP CONF PROC PY 2013 VL 1525 BP 355 EP 359 DI 10.1063/1.4802350 PG 5 WC Physics, Applied; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFI58 UT WOS:000319997900071 ER PT S AU Sun, ZJ Wells, D Starovoitova, V Segebade, C AF Sun, Z. J. Wells, D. Starovoitova, V. Segebade, C. BE McDaniel, FD Doyle, BL Glass, GA Wang, Y TI Testing The Quasi-Absolute Method In Photon Activation Analysis SO APPLICATION OF ACCELERATORS IN RESEARCH AND INDUSTRY SE AIP Conference Proceedings LA English DT Proceedings Paper CT 22nd International Conference on the Application of Accelerators in Research and Industry (CAARI) CY AUG 05-10, 2012 CL Fort Worth, TX SP Sandia Natl Labs, Univ N Texas, Los Alamos Natl Lab, Pacific NW Natl Lab, High Voltage Engn Europa B V, Kurt J Lester Co, Natl Electrostat Corp DE Photon Activation Analysis (PAA); Nuclear Analysis; Simulation; LINAC ID MONTE-CARLO-SIMULATION; THICK TARGETS; BREMSSTRAHLUNG AB In photon activation analysis (PAA), relative methods are widely used because of their accuracy and precision. Absolute methods, which are conducted without any assistance from calibration materials, are seldom applied for the difficulty in obtaining photon flux in measurements. This research is an attempt to perform a new absolute approach in PAA - quasi-absolute method - by retrieving photon flux in the sample through Monte Carlo simulation. With simulated photon flux and database of experimental cross sections, it is possible to calculate the concentration of target elements in the sample directly. The QA/QC procedures to solidify the research are discussed in detail. Our results show that the accuracy of the method for certain elements is close to a useful level in practice. Furthermore, the future results from the quasi-absolute method can also serve as a validation technique for experimental data on cross sections. The quasi-absolute method looks promising. C1 [Sun, Z. J.] Argonne Natl Lab, Chem Sci & Engn Div, 9700 S Cass Ave, Argonne, IL 60439 USA. [Wells, D.] South Dakota Sch Mines & Technol, Dept Phys, Rapid City, SD 57701 USA. [Starovoitova, V.; Segebade, C.] Idaho State Univ, Idaho Accelerator Ctr, Pocatello, ID 83209 USA. RP Sun, ZJ (reprint author), Argonne Natl Lab, Chem Sci & Engn Div, 9700 S Cass Ave, Argonne, IL 60439 USA. FU U.S. Department of Energy, Basic Energy Sciences, Office of Science [DE-AC02-06CH11357] FX This work is supported by the U.S. Department of Energy, Basic Energy Sciences, Office of Science, under contract # DE-AC02-06CH11357. NR 9 TC 2 Z9 2 U1 0 U2 3 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1148-7 J9 AIP CONF PROC PY 2013 VL 1525 BP 412 EP 416 DI 10.1063/1.4802360 PG 5 WC Physics, Applied; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFI58 UT WOS:000319997900081 ER PT S AU Shavorskiy, A Cordones, A Vura-Weis, J Siefermann, K Slaughter, D Sturm, F Weise, F Bluhm, H Strader, M Cho, HN Lin, MF Bacellar, C Khurmi, C Hertlein, M Guo, JH Tyliszczak, T Prendergast, D Coslovich, G Robinson, J Kaindl, RA Schoenlein, RW Belkacem, A Weber, T Neumark, DM Leone, SR Nordlund, D Ogasawara, H Nilsson, AR Krupin, O Turner, JJ Schlotter, WF Holmes, MR Heimann, PA Messerschmidt, M Minitti, MP Beye, M Gul, S Zhang, JZ Huse, N Gessner, O AF Shavorskiy, Andrey Cordones, Amy Vura-Weis, Josh Siefermann, Katrin Slaughter, Daniel Sturm, Felix Weise, Fabian Bluhm, Hendrik Strader, Matthew Cho, Hana Lin, Ming-Fu Bacellar, Camila Khurmi, Champak Hertlein, Marcus Guo, Jinghua Tyliszczak, Tolek Prendergast, David Coslovich, Giacomo Robinson, Joseph Kaindl, Robert A. Schoenlein, Robert W. Belkacem, Ali Weber, Thorsten Neumark, Daniel M. Leone, Stephen R. Nordlund, Dennis Ogasawara, Hirohito Nilsson, Anders R. Krupin, Oleg Turner, Joshua J. Schlotter, William F. Holmes, Michael R. Heimann, Philip A. Messerschmidt, Marc Minitti, Michael P. Beye, Martin Gul, Sheraz Zhang, Jin Z. Huse, Nils Gessner, Oliver BE McDaniel, FD Doyle, BL Glass, GA Wang, Y TI Time-Resolved X-Ray Photoelectron Spectroscopy Techniques For Real-Time Studies Of Interfacial Charge Transfer Dynamics SO APPLICATION OF ACCELERATORS IN RESEARCH AND INDUSTRY SE AIP Conference Proceedings LA English DT Proceedings Paper CT 22nd International Conference on the Application of Accelerators in Research and Industry (CAARI) CY AUG 05-10, 2012 CL Fort Worth, TX SP Sandia Natl Labs, Univ N Texas, Los Alamos Natl Lab, Pacific NW Natl Lab, High Voltage Engn Europa B V, Kurt J Lester Co, Natl Electrostat Corp DE Ultrafast Spectroscopy; X-ray Photoelectron Spectroscopy; Dye-Sensitized Nanostructures; Free Electron Lasers ID ELECTRON INJECTION; RECOMBINATION; LASER AB X-ray based spectroscopy techniques are particularly well suited to gain access to local oxidation states and electronic dynamics in complex systems with atomic pinpoint accuracy. Traditionally, these techniques are applied in a quasi-static fashion that usually highlights the steady-state properties of a system rather than the fast dynamics that often define the system function on a molecular level. Novel x-ray spectroscopy techniques enabled by free electron lasers (FELs) and synchrotron based pump-probe schemes provide the opportunity to monitor intramolecular and interfacial charge transfer processes in real-time and with element and chemical specificity. Two complementary time-domain x-ray photoelectron spectroscopy techniques are presented that are applied at the Linac Coherent Light Source (LCLS) and the Advanced Light Source (ALS) to study charge transfer processes in N3 dye-sensitized ZnO semiconductor nanocrystals, which are at the heart of emerging light-harvesting technologies. C1 [Shavorskiy, Andrey; Hertlein, Marcus; Guo, Jinghua; Tyliszczak, Tolek] Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. [Cordones, Amy; Vura-Weis, Josh; Lin, Ming-Fu; Bacellar, Camila; Neumark, Daniel M.; Leone, Stephen R.] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Siefermann, Katrin; Slaughter, Daniel; Sturm, Felix; Weise, Fabian; Lin, Ming-Fu; Bacellar, Camila; Khurmi, Champak; Schoenlein, Robert W.; Belkacem, Ali; Weber, Thorsten; Neumark, Daniel M.; Leone, Stephen R.; Gessner, Oliver] Lawrence Berkeley Natl Lab, Ultrafast Xray Sci Lab, Div Chem Sci, Berkeley, CA 94720 USA. [Bluhm, Hendrik] Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. [Strader, Matthew; Cho, Hana; Coslovich, Giacomo; Robinson, Joseph; Kaindl, Robert A.] Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. [Prendergast, David] Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA. [Robinson, Joseph; Krupin, Oleg; Turner, Joshua J.; Schlotter, William F.; Holmes, Michael R.; Heimann, Philip A.; Messerschmidt, Marc; Minitti, Michael P.] SLAC Natl Accelerator Lab, Linac Coherent Light Source, Menlo Pk, CA 94025 USA. [Leone, Stephen R.] Univ Calif Berkeley, Dept Phys, Berkeley, CA 94720 USA. [Nordlund, Dennis; Ogasawara, Hirohito; Nilsson, Anders R.] SLAC Natl Accelerator Lab, Menlo Pk, CA 94025 USA. [Krupin, Oleg] European XFEL GmbH, Schenefeld, Germany. [Beye, Martin] Helmholtz Zentrum Berlin, Mat & Energie GmbH, Berlin, Germany. [Gul, Sheraz; Zhang, Jin Z.] Univ Calif Santa Cruz, Dept Chem & Biochem, Santa Cruz, CA 95064 USA. [Huse, Nils] Univ Hamburg, CFEL, Max Planck Res Dept Struct Dynam, Hamburg, Germany. RP Shavorskiy, A (reprint author), Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. RI Messerschmidt, Marc/F-3796-2010; Schoenlein, Robert/D-1301-2014; Nordlund, Dennis/A-8902-2008; Beye, Martin/F-1165-2011; Foundry, Molecular/G-9968-2014; Ogasawara, Hirohito/D-2105-2009; Neumark, Daniel/B-9551-2009 OI Messerschmidt, Marc/0000-0002-8641-3302; Schoenlein, Robert/0000-0002-6066-7566; Nordlund, Dennis/0000-0001-9524-6908; Beye, Martin/0000-0002-3924-2993; Ogasawara, Hirohito/0000-0001-5338-1079; Neumark, Daniel/0000-0002-3762-9473 FU U.S. Department of Energy [DEAC02-05CH11231]; Department of Energy Office of Science Early Career Research Program; Basic Energy Sciences Division of the US DOE [DE-FG02-ER46232]; consortium whose membership includes the LCLS; Stanford University through the Stanford Institute for Materials Energy Sciences (SIMES); Lawrence Berkeley National Laboratory (LBNL); University of Hamburg through the BMBF [FSP 301]; Center for Free Electron Laser Science (CFEL) FX The authors would like to acknowledge the outstanding support from the staff at the Advanced Light Source, Lawrence Berkeley National Laboratory, and the Linac Coherent Light Source, SLAC National Accelerator Laboratory. This work was supported by the Director, Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract no. DEAC02-05CH11231. O.G. was supported by the Department of Energy Office of Science Early Career Research Program. J.Z.Z. is grateful for support by the Basic Energy Sciences Division of the US DOE (DE-FG02-ER46232). Portions of this research were carried out on the SXR Instrument at the Linac Coherent Light Source (LCLS), a division of SLAC National Accelerator Laboratory and an Office of Science user facility operated by Stanford University for the U.S. Department of Energy. The SXR Instrument is funded by a consortium whose membership includes the LCLS, Stanford University through the Stanford Institute for Materials Energy Sciences (SIMES), Lawrence Berkeley National Laboratory (LBNL), University of Hamburg through the BMBF priority program FSP 301, and the Center for Free Electron Laser Science (CFEL) NR 12 TC 2 Z9 2 U1 2 U2 35 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1148-7 J9 AIP CONF PROC PY 2013 VL 1525 BP 475 EP 479 DI 10.1063/1.4802374 PG 5 WC Physics, Applied; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFI58 UT WOS:000319997900095 ER PT S AU Ratkiewicz, A Pain, SD Cizewski, JA Bardayan, DW Blackmon, JC Chipps, KA Hardy, S Jones, KL Kozub, RL Lister, CJ Manning, B Matos, M Peters, WA Seweryniak, D Shand, C AF Ratkiewicz, A. Pain, S. D. Cizewski, J. A. Bardayan, D. W. Blackmon, J. C. Chipps, K. A. Hardy, S. Jones, K. L. Kozub, R. L. Lister, C. J. Manning, B. Matos, M. Peters, W. A. Seweryniak, D. Shand, C. BE McDaniel, FD Doyle, BL Glass, GA Wang, Y TI Coupling Gammasphere and ORRUBA SO APPLICATION OF ACCELERATORS IN RESEARCH AND INDUSTRY SE AIP Conference Proceedings LA English DT Proceedings Paper CT 22nd International Conference on the Application of Accelerators in Research and Industry (CAARI) CY AUG 05-10, 2012 CL Fort Worth, TX SP Sandia Natl Labs, Univ N Texas, Los Alamos Natl Lab, Pacific NW Natl Lab, High Voltage Engn Europa B V, Kurt J Lester Co, Natl Electrostat Corp DE Radioactive ion beams; Neutron transfer reactions; Silicon detectors; HPGe gamma-ray detectors AB The coincident detection of particles and gamma rays allows the study of the structure of exotic nuclei via inverse kinematics reactions using radioactive ion beams and thick targets. We report on the status of the project to couple the high-resolution charged-particle detector ORRUBA to Gammasphere, a high-efficiency, high-resolution gamma ray detector. C1 [Ratkiewicz, A.; Cizewski, J. A.; Hardy, S.; Manning, B.; Shand, C.] Rutgers State Univ, Dept Phys & Astron, New Brunswick, NJ 08903 USA. [Pain, S. D.; Bardayan, D. W.] Div Phys, Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. [Blackmon, J. C.; Matos, M.] Louisiana State Univ, Dept Phys & Astron, Baton Rouge, LA 70803 USA. [Chipps, K. A.] Colorado Sch Mines, Dept Phys, Golden, CO 80401 USA. [Hardy, S.; Shand, C.] Univ Surrey, Dept Phys, Surrey, England. [Jones, K. L.] Univ Tennessee, Dept Phys & Astron, Knoxville, TN 37996 USA. [Kozub, R. L.] Tennessee Technol Univ, Dept Phys, Cookeville, TN 38505 USA. [Lister, C. J.; Seweryniak, D.] Argonne Natl Lab, Div Phys, Argonne, IL 60439 USA. [Lister, C. J.] Univ Massachusetts Lowell, Dept Phys & Appl Phys, Lowell, MA 01854 USA. [Peters, W. A.] Oak Ridge Associated Univ, Oak Ridge, TN 37830 USA. RP Ratkiewicz, A (reprint author), Rutgers State Univ, Dept Phys & Astron, New Brunswick, NJ 08903 USA. RI Jones, Katherine/B-8487-2011; Pain, Steven/E-1188-2011; Peters, William/B-3214-2012; OI Jones, Katherine/0000-0001-7335-1379; Pain, Steven/0000-0003-3081-688X; Peters, William/0000-0002-3022-4924; Chipps, Kelly/0000-0003-3050-1298 FU U.S. Department of Energy National Nuclear Security Administration under the Stewardship Science Academic Alliances program through DOE [DE-FG52-08NA28552]; Rutgers, ORAU; DOE Office of Nuclear Physics; ORNL [DE-AC05-00OR22725]; UT [DE-FG02-96ER40983]; CSM [DEFG03-93ER40789]; ANL [DE-AC02-06CH11357]; TTU [DE-FG02-96ER40955]; National Science Foundation FX This research was supported in part by the U.S. Department of Energy National Nuclear Security Administration under the Stewardship Science Academic Alliances program through DOE Cooperative Agreement No. DE-FG52-08NA28552 (Rutgers, ORAU); the DOE Office of Nuclear Physics under Contract Nos. DE-AC05- 00OR22725 (ORNL), DE-FG02-96ER40983 (UT), DEFG03-93ER40789 (CSM), DE-AC02-06CH11357 (ANL), DE-FG02-96ER40955 (TTU); and the National Science Foundation. The authors gratefully acknowledge the contributions of M. Carpenter and S. Zhu towards the design and testing of this project. NR 8 TC 4 Z9 4 U1 0 U2 3 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1148-7 J9 AIP CONF PROC PY 2013 VL 1525 BP 487 EP 491 DI 10.1063/1.4802376 PG 5 WC Physics, Applied; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFI58 UT WOS:000319997900097 ER PT S AU Benitez, J Hodgkinson, A Johnson, M Loew, T Lyneis, C Phair, L AF Benitez, Janilee Hodgkinson, Adrian Johnson, Mike Loew, Tim Lyneis, Claude Phair, Larry BE McDaniel, FD Doyle, BL Glass, GA Wang, Y TI Development Of Ion Beams For Space Effects Testing Using An ECR Ion Source SO APPLICATION OF ACCELERATORS IN RESEARCH AND INDUSTRY SE AIP Conference Proceedings LA English DT Proceedings Paper CT 22nd International Conference on the Application of Accelerators in Research and Industry (CAARI) CY AUG 05-10, 2012 CL Fort Worth, TX SP Sandia Natl Labs, Univ N Texas, Los Alamos Natl Lab, Pacific NW Natl Lab, High Voltage Engn Europa B V, Kurt J Lester Co, Natl Electrostat Corp (NEC) DE ion sources; radiation effects facility; VENUS; AECR-U; Cocktail beams AB At LBNL's 88-Inch Cyclotron and Berkeley Accelerator Space Effects (BASE) Facility, a range of ion beams at energies from 1 to 55 MeV/nucleon are used for radiation space effects testing. By bombarding a component with ion beams the radiation component of the space environment can be simulated and single event effects (SEEs) determined. The performance of electronic components used in space flight and high altitude aircraft can then be evaluated. The 88-Inch Cyclotron is coupled to the three electron cyclotron resonance ion sources (ECR, AECR-U, VENUS). These ion sources provide a variety of ion species, ranging from protons to heavy ions such as bismuth, for these tests. In particular the ion sources have been developed to provide "cocktails", a mixture of ions of similar mass-to-charge ratio, which can be simultaneously injected into the cyclotron, but selectively extracted from it. The ions differ in both their linear energy transfer (LET) deposited to the part and in their penetration depth into the tested part. The current heavy ion cocktails available are the 4.5, 10, 16, and 30 MeV per nucleon. To provide the optimum range of LET a variety of ion beams and charge states is required. In order to produce a broad range of heavy ion cocktails, several methods to inject various metals and gases simultaneously have been developed, including sputter probes and ovens. Cocktail beams, first developed in 1985 in Berkeley, continue to evolve along with the capabilities of the accelerator system. The newest ECR source at Berkeley, VENUS, is capable of producing very high charge state heavy ions, delivering heavier ions with increased range and LET. The most recent example is the acceleration of Bi56+ to 9.5 MeV per nucleon. This paper will discuss the progress and gains still underway with the ECR ion sources and how they support radiation space effects testing. C1 [Benitez, Janilee; Hodgkinson, Adrian; Johnson, Mike; Loew, Tim; Lyneis, Claude; Phair, Larry] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Nucl Sci, Berkeley, CA 94720 USA. RP Benitez, J (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Nucl Sci, 1 Cyclotron Rd, Berkeley, CA 94720 USA. NR 7 TC 0 Z9 0 U1 0 U2 0 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1148-7 J9 AIP CONF PROC PY 2013 VL 1525 BP 503 EP 506 DI 10.1063/1.4802379 PG 4 WC Physics, Applied; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFI58 UT WOS:000319997900100 ER PT S AU Winklehner, D Lemut, A Leitner, D Couder, M Hodgkinson, A Wiescher, M AF Winklehner, Daniel Lemut, Alberto Leitner, Daniela Couder, Manoel Hodgkinson, Adrian Wiescher, Michael BE McDaniel, FD Doyle, BL Glass, GA Wang, Y TI DIANA - A Deep Underground Accelerator For Nuclear Astrophysics Experiments SO APPLICATION OF ACCELERATORS IN RESEARCH AND INDUSTRY SE AIP Conference Proceedings LA English DT Proceedings Paper CT 22nd International Conference on the Application of Accelerators in Research and Industry (CAARI) CY AUG 05-10, 2012 CL Fort Worth, TX SP Sandia Natl Labs, Univ N Texas, Los Alamos Natl Lab, Pacific NW Natl Lab, High Voltage Engn Europa B V, Kurt J Lester Co, Natl Electrostat Corp DE Ion Sources; Electrostatic Accelerators; Simulations ID CROSS-SECTION AB DIANA (Dakota Ion Accelerator for Nuclear Astrophysics) is a proposed facility designed to be operated deep underground. The DIANA collaboration includes nuclear astrophysics groups from Lawrence Berkeley National Laboratory, Michigan State University, Western Michigan University, Colorado School of Mines, and the University of North Carolina, and is led by the University of Notre Dame. The scientific goals of the facility are measurements of low energy nuclear cross-sections associated with sun and pre-supernova stars in a laboratory setup at energies that are close to those in stars. Because of the low stellar temperatures associated with these environments, and the high Coulomb barrier, the reaction cross-sections are extremely low. Therefore these measurements are hampered by small signal to background ratios. By going underground the background due to cosmic rays can be reduced by several orders of magnitude. We report on the design status of the DIANA facility with focus on the 3 MV electrostatic accelerator. C1 [Winklehner, Daniel; Leitner, Daniela] Michigan State Univ, 640 S Shaw Lane, E Lansing, MI 48824 USA. [Lemut, Alberto; Hodgkinson, Adrian] Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Couder, Manoel; Wiescher, Michael] Univ Notre Dame, Notre Dame, IN 46556 USA. RP Winklehner, D (reprint author), Michigan State Univ, 640 S Shaw Lane, E Lansing, MI 48824 USA. RI Couder, Manoel/B-1439-2009 OI Couder, Manoel/0000-0002-0636-744X FU National Science Foundation [NSF-09-500, 091728]; Office of Science; Office of Basic Energy Sciences, of U.S. Department of Energy [DE-AC02-05CH11231]; Assistant Secretary for Energy Efficiency and Renewable Energy; U.S. Department of Energy [DE-AC02-05CH11231] FX This work is supported by the National Science Foundation NSF-09-500 grant, proposal ID 091728. This work was supported by the Director, Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. This work was 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. NR 10 TC 1 Z9 1 U1 1 U2 4 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1148-7 J9 AIP CONF PROC PY 2013 VL 1525 BP 516 EP 519 DI 10.1063/1.4802382 PG 4 WC Physics, Applied; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFI58 UT WOS:000319997900103 ER PT S AU Jost, CU Griswold, JR Bruffey, SH Mirzadeh, S Stracener, DW Williams, CL AF Jost, C. U. Griswold, J. R. Bruffey, S. H. Mirzadeh, S. Stracener, D. W. Williams, C. L. BE McDaniel, FD Doyle, BL Glass, GA Wang, Y TI Measurement Of Cross Sections For The Th-232 (P, 4n) Pa-229 Reaction At Low Proton Energies SO APPLICATION OF ACCELERATORS IN RESEARCH AND INDUSTRY SE AIP Conference Proceedings LA English DT Proceedings Paper CT 22nd International Conference on the Application of Accelerators in Research and Industry (CAARI) CY AUG 05-10, 2012 CL Fort Worth, TX SP Sandia Natl Labs, Univ N Texas, Los Alamos Natl Lab, Pacific NW Natl Lab, High Voltage Engn Europa B V, Kurt J Lester Co, Natl Electrostat Corp DE Medical isotopes; Thorium; accelerator ID HRIBF; CU AB The alpha-emitters Ac-225 and Bi-213 are of great interest for alpha-radioimmunotherapy which uses radioisotopes attached to cancer-seeking antibodies to efficiently treat various types of cancers. Both radioisotopes are daughters of the long-lived Th-229 (t(1/2) = 7880y). Th-229 can be produced by proton irradiation of Th-232 and Th-230, either directly or through production of isobars that beta-decay into Th-229. To obtain excitation functions, Th-232 and Th-230 have been irradiated at the On-Line Test Facility at the Holifield Radioactive Ion Beam Facility at ORNL. Benchmark tests conducted with Cu and Ni foils show very good agreement with literature results. The experiments with thorium targets were focused on the production of Pa-229 and its daughter Ac-225 from both Th-232 and Th-230. Differential cross-sections for production of Pa-229 and other Pa isotopes have been obtained. C1 [Jost, C. U.] Univ Tennessee, Dept Phys & Astron, Knoxville, TN 37996 USA. [Griswold, J. R.] Univ Tennessee, Dept Nuclear Engn, Knoxville, TN 37996 USA. [Griswold, J. R.; Bruffey, S. H.; Mirzadeh, S.] Oak Ridge Natl Lab, Fuel Cycle & Isotope Div, Oak Ridge, TN 37831 USA. [Stracener, D. W.] Oak Ridge Natl Lab, Div Phys, Oak Ridge, TN 37831 USA. [Williams, C. L.] Oak Ridge Associated Univ, Oak Ridge, TN 37831 USA. RP Jost, CU (reprint author), Univ Tennessee, Dept Phys & Astron, Knoxville, TN 37996 USA. FU Office of Nuclear Physics of U.S. Department of Energy (DOE); UT-Battelle LLC [DE-AC05-00OR22725]; US Department of Energy FX Research supported by the Office of Nuclear Physics of the U.S. Department of Energy (DOE). The authors gratefully acknowledge the efforts of the HRIBF staff in delivering the high-quality proton beams that made this study possible. This manuscript has been authored by UT-Battelle LLC under Contract No. DE-AC05-00OR22725 with the US Department of Energy. The US Government retains and the publisher, by accepting the article for publication, acknowledges that the US Government retains a non-exclusive, paid-up, 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 12 TC 4 Z9 4 U1 0 U2 3 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1148-7 J9 AIP CONF PROC PY 2013 VL 1525 BP 520 EP 524 DI 10.1063/1.4802383 PG 5 WC Physics, Applied; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFI58 UT WOS:000319997900104 ER PT S AU Manning, B Cizewski, JA Kozub, RL Ahn, S Allmond, JM Bardayan, DW Beene, JR Chae, KY Chipps, KA Galindo-Uribarri, A Howard, ME Jones, KL Liang, JF Matos, M Nesaraja, CD O'Malley, PD Pain, SD Padilla-Rodal, E Peters, WA Pittman, ST Radford, DC Ratkiewicz, A Schmitt, KT Shapira, D Smith, MS AF Manning, B. Cizewski, J. A. Kozub, R. L. Ahn, S. Allmond, J. M. Bardayan, D. W. Beene, J. R. Chae, K. Y. Chipps, K. A. Galindo-Uribarri, A. Howard, M. E. Jones, K. L. Liang, J. F. Matos, M. Nesaraja, C. D. O'Malley, P. D. Pain, S. D. Padilla-Rodal, E. Peters, W. A. Pittman, S. T. Radford, D. C. Ratkiewicz, A. Schmitt, K. T. Shapira, D. Smith, M. S. BE McDaniel, FD Doyle, BL Glass, GA Wang, Y TI Single-Neutron Levels Near The N=82 Shell Closure SO APPLICATION OF ACCELERATORS IN RESEARCH AND INDUSTRY SE AIP Conference Proceedings LA English DT Proceedings Paper CT 22nd International Conference on the Application of Accelerators in Research and Industry (CAARI) CY AUG 05-10, 2012 CL Fort Worth, TX SP Sandia Natl Labs, Univ N Texas, Los Alamos Natl Lab, Pacific NW Natl Lab, High Voltage Engn Europa B V, Kurt J Lester Co, Natl Electrostat Corp DE Transfer Reactions; Single-Particle States; Shell Model; Radioactive Ion Beams ID COULOMB-EXCITATION; BEAMS; HRIBF AB The (d,p) reaction was measured with the radioactive ion beams of Sn-126 and Sn-128 in inverse kinematics at the Holifield Radioactive Ion Beam Facility at Oak Ridge National Laboratory, utilizing the SuperORRUBA silicon detector array. Angular distributions of reaction protons were measured for several states in Sn-127 and Sn-129 to determine angular momentum transfers and deduce spectroscopic factors. Such information is critical for calculating direct (n,gamma) cross sections for the r-process as well as for constraining shell model parameters in the A approximate to 130 region. Combined with previous experiments on Sn-130 and Sn-132, these results will provide a complete set of (d, p) reaction data on even tin isotopes between stable Sn-124 and doubly-magic Sn-132. C1 [Manning, B.; Cizewski, J. A.; Howard, M. E.; O'Malley, P. D.; Ratkiewicz, A.] Rutgers State Univ, Dept Phys & Astron, POB 849, Piscataway, NJ 08854 USA. [Kozub, R. L.] Tennessee Technol Univ, Dept Phys, Cookeville, TN 38505 USA. [Ahn, S.; Galindo-Uribarri, A.; Jones, K. L.] Univ Tennessee, Dept Phys & Astron, Knoxville, TN 37996 USA. [Allmond, J. M.] JIHIR, Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. [Bardayan, D. W.; Beene, J. R.; Galindo-Uribarri, A.; Nesaraja, C. D.; Pain, S. D.; Pittman, S. T.; Radford, D. C.; Schmitt, K. T.; Shapira, D.] Oak Ridge Natl Lab, Div Phys, Oak Ridge, TN 37831 USA. [Chae, K. Y.] Sungkyunkwan Univ, Dept Phys, Suwon, South Korea. [Chipps, K. A.] Colorado Sch Mines, Dept Phys, Golden, CO 80401 USA. [Matos, M.] Louisiana State Univ, Dept Phys & Astron, Baton Rouge, LA 70803 USA. [Padilla-Rodal, E.] Univ Nacl Autonoma Mexico, Inst Nucl Sci, Mexico City 04510, DF, Mexico. [Peters, W. A.] Oak Ridge Associated Univ, Oak Ridge, TN 37830 USA. RP Manning, B (reprint author), Rutgers State Univ, Dept Phys & Astron, POB 849, Piscataway, NJ 08854 USA. RI radford, David/A-3928-2015; Jones, Katherine/B-8487-2011; Pain, Steven/E-1188-2011; OI Jones, Katherine/0000-0001-7335-1379; Pain, Steven/0000-0003-3081-688X; Nesaraja, Caroline/0000-0001-5571-8341; Chipps, Kelly/0000-0003-3050-1298; Allmond, James Mitchell/0000-0001-6533-8721 FU U.S. Department of Energy; National Science Foundation FX We would like to thank Dan Stracener and Cara Jost who provided critical accelerator physics expertise in support of these experiments. This work is supported in part by the U.S. Department of Energy and National Science Foundation. NR 17 TC 0 Z9 0 U1 0 U2 1 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1148-7 J9 AIP CONF PROC PY 2013 VL 1525 BP 548 EP 551 DI 10.1063/1.4802388 PG 4 WC Physics, Applied; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFI58 UT WOS:000319997900109 ER PT S AU Laptev, AB Tovesson, F Hill, TS AF Laptev, A. B. Tovesson, F. Hill, T. S. BE McDaniel, FD Doyle, BL Glass, GA Wang, Y TI Neutron-Induced Fission Cross Section Measurements For Uranium Isotopes U-236 And U-234 At LANSCE SO APPLICATION OF ACCELERATORS IN RESEARCH AND INDUSTRY SE AIP Conference Proceedings LA English DT Proceedings Paper CT 22nd International Conference on the Application of Accelerators in Research and Industry (CAARI) CY AUG 05-10, 2012 CL Fort Worth, TX SP Sandia Natl Labs, Univ N Texas, Los Alamos Natl Lab, Pacific NW Natl Lab, High Voltage Engn Europa B V, Kurt J Lester Co, Natl Electrostat Corp DE Fission; cross section; actinides; fast neutrons; time-of-flight ID SCIENCE AB A well established program of neutron-induced fission cross section measurement at Los Alamos Neutron Science Center (LANSCE) is supporting the Fuel Cycle Research program (FC R&D). The incident neutron energy range spans from sub-thermal up to 200 MeV by combining two LANSCE facilities, the Lujan Center and the Weapons Neutron Research facility (WNR). The time-of-flight method is implemented to measure the incident neutron energy. A parallel-plate fission ionization chamber was used as a fission fragment detector. The event rate ratio between the investigated foil and a standard U-235 foil is converted into a fission cross section ratio. In addition to previously measured data new measurements include U-236 data which is being analyzed, and U-234 data acquired in the 2011-2012 LANSCE run cycle. The new data complete the full suite of Uranium isotopes which were investigated with this experimental approach. Obtained data are presented in comparison with existing evaluations and previous data. C1 [Laptev, A. B.; Tovesson, F.] Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. RP Laptev, AB (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. RI Laptev, Alexander/D-4686-2009 OI Laptev, Alexander/0000-0002-9759-9907 FU US Department of Energy and operated by Los Alamos National Security; LLC [DE-AC52-06NA25396]; US Department of Energy; operated by Los Alamos National Security, LLC [DE-AC52-06NA25396] FX This work has benefited from the use of the Los Alamos Neutron Science Center at the Los Alamos National Laboratory. This facility is funded by the US Department of Energy and operated by Los Alamos National Security, LLC under contract DE-AC52-06NA25396. NR 11 TC 0 Z9 0 U1 0 U2 3 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1148-7 J9 AIP CONF PROC PY 2013 VL 1525 BP 563 EP 566 DI 10.1063/1.4802391 PG 4 WC Physics, Applied; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFI58 UT WOS:000319997900112 ER PT S AU Boswell, MS Elliott, SR Guiseppe, V Kidd, M Rundberg, B Tybo, J AF Boswell, M. S. Elliott, S. R. Guiseppe, V. Kidd, M. Rundberg, B. Tybo, J. BE McDaniel, FD Doyle, BL Glass, GA Wang, Y TI Neutron-Induced Reactions In The Hohlraum To Study Reaction In Flight Neutrons SO APPLICATION OF ACCELERATORS IN RESEARCH AND INDUSTRY SE AIP Conference Proceedings LA English DT Proceedings Paper CT 22nd International Conference on the Application of Accelerators in Research and Industry (CAARI) CY AUG 05-10, 2012 CL Fort Worth, TX SP Sandia Natl Labs, Univ N Texas, Los Alamos Natl Lab, Pacific NW Natl Lab, High Voltage Engn Europa B V, Kurt J Lester Co, Natl Electrostat Corp DE Diagnostic; National Ignition Facility (NIF); gold; Reaction In Flight (RIF); explosions; plasma diagnostics; neutron sources AB We are currently developing the physics necessary to measure the Reaction In Flight (RIF) neutron flux from a NIF capsule. A measurement of the RIF neutron flux from a NIF capsule could be used to deduce the stopping power in the cold fuel of the NIF capsule. A foil irradiated at the Omega laser at LLE was counted at the LANL low-background counting facility at WIPP. The estimated production rate of Au-195 was just below our experimental sensitivity. We have made several improvements to our counting facility in recent months. These improvements are designed to increase our sensitivity, and include installing two new low-background detectors, and taking steps to reduce noise in the signals. C1 [Boswell, M. S.; Elliott, S. R.; Tybo, J.] Los Alamos Natl Lab, Div Phys, Los Alamos, NM 87545 USA. RP Boswell, MS (reprint author), Los Alamos Natl Lab, Div Phys, Los Alamos, NM 87545 USA. FU US Department of Energy [DEAC52-06NA25396]; LANL/LDRD Program FX support of the US Department of Energy under contract DEAC52-06NA25396,and the LANL/LDRD Program.We also wish to thank the technical staff at WIPP fortheir hospitality and assistance getting the laboratory together. NR 5 TC 0 Z9 0 U1 0 U2 4 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1148-7 J9 AIP CONF PROC PY 2013 VL 1525 BP 567 EP 569 DI 10.1063/1.4802392 PG 3 WC Physics, Applied; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFI58 UT WOS:000319997900113 ER PT S AU Baramsai, B Mitchell, GE Walker, CL Bredeweg, TA Couture, A Haight, RC Jandel, M Mosb, S O'Donnell, JM Rundberg, RS Rusev, G Ullmann, JL Vieira, DJ Becvar, F Krticka, M Kroll, J Agvaanluvsan, U Dashdorj, D Erdenehuluun, B Tsend-Ayush, T AF Baramsai, B. Mitchell, G. E. Walker, C. L. Bredeweg, T. A. Couture, A. Haight, R. C. Jandel, M. Mosb, S. O'Donnell, J. M. Rundberg, R. S. Rusev, G. Ullmann, J. L. Vieira, D. J. Becvar, F. Krticka, M. Kroll, J. Agvaanluvsan, U. Dashdorj, D. Erdenehuluun, B. Tsend-Ayush, T. BE McDaniel, FD Doyle, BL Glass, GA Wang, Y TI (n,gamma) Experiments On Tin Isotopes SO APPLICATION OF ACCELERATORS IN RESEARCH AND INDUSTRY SE AIP Conference Proceedings LA English DT Proceedings Paper CT 22nd International Conference on the Application of Accelerators in Research and Industry (CAARI) CY AUG 05-10, 2012 CL Fort Worth, TX SP Sandia Natl Labs, Univ N Texas, Los Alamos Natl Lab, Pacific NW Natl Lab, High Voltage Engn Europa B V, Kurt J Lester Co, Natl Electrostat Corp DE Neutron capture; Tin; gamma-ray multiplicity; resonance spin and parity AB Neutron capture experiments on highly enriched Sn-117,Sn- 119 isotopes were performed with the DANCE detector array located at the Los Alamos Neutron Science Center. The DANCE detector provides detailed information about the multi-step gamma-ray cascade following neutron capture. Analysis of the experimental data provides important information to improve understanding of the neutron capture reaction, including a test of the statistical model, the assignment of spins and parities of neutron resonances, and information concerning the Photon Strength Function (PSF) and Level Density (LD) below the neutron separation energy. Preliminary results for the (n,gamma) reaction on Sn-117,Sn- 119 are presented. Resonance spins of the odd-A tin isotopes were almost completely unknown. Resonance spins and parities have been assigned via analysis of the multi-step gamma-ray spectra and directional correlations. C1 [Baramsai, B.; Mitchell, G. E.; Walker, C. L.; Rusev, G.] N Carolina State Univ, Raleigh, NC 27695 USA. [Baramsai, B.; Mitchell, G. E.; Walker, C. L.; Rusev, G.] Triangle Univ Nucl Lab, Durham, NC 27708 USA. [Bredeweg, T. A.; Couture, A.; Haight, R. C.; Jandel, M.; O'Donnell, J. M.; Rundberg, R. S.; Ullmann, J. L.; Vieira, D. J.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Becvar, F.; Krticka, M.; Kroll, J.] Charles Univ Prague, Prague 18000, Czech Republic. [Agvaanluvsan, U.; Dashdorj, D.; Erdenehuluun, B.; Tsend-Ayush, T.] MonAme Scientif Res Ctr, Ulaanbaatar, Mongol Peo Rep. RP Baramsai, B (reprint author), N Carolina State Univ, Raleigh, NC 27695 USA. FU U. S. Department of Energy [DE-FG52-09NA29460, DE-FG02-97-ER41042]; U.S. DOE [DE-AC52-06NA25396] FX This work was supported in part by the U. S. Department of Energy Grants No. DE-FG52-09NA29460 and No. DE-FG02-97-ER41042 and performed under the auspices of the U.S. DOE under contracts No. DE-AC52-06NA25396. NR 8 TC 0 Z9 0 U1 1 U2 7 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1148-7 J9 AIP CONF PROC PY 2013 VL 1525 BP 577 EP 580 DI 10.1063/1.4802394 PG 4 WC Physics, Applied; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFI58 UT WOS:000319997900115 ER PT S AU Harwood, L AF Harwood, Leigh BE McDaniel, FD Doyle, BL Glass, GA Wang, Y TI Upgrade Of CEBAF From 6 Gev To 12 Gev: Status SO APPLICATION OF ACCELERATORS IN RESEARCH AND INDUSTRY SE AIP Conference Proceedings LA English DT Proceedings Paper CT 22nd International Conference on the Application of Accelerators in Research and Industry (CAARI) CY AUG 05-10, 2012 CL Fort Worth, TX SP Sandia Natl Labs, Univ N Texas, Los Alamos Natl Lab, Pacific NW Natl Lab, High Voltage Engn Europa B V, Kurt J Lester Co, Natl Electrostat Corp (NEC) DE Electron accelerator; linac; srf; upgrade AB The CEBAF accelerator is being upgraded from 6 GeV to 12 GeV by the US Department of Energy. The accelerator upgrade is being done within the existing tunnel footprint. The accelerator upgrade includes: 10 new srf-based high-performance cryomodules plus RF systems, doubling the 2K helium plant's capability, upgrading the existing beamlines to operate at nearly double the original performance envelope, and adding a beamline to a new experimental area. Construction is over 75% complete with final completion projected for late FY13. Details of the upgrade and status of the work will be presented. C1 Jefferson Lab, Newport News, VA 23606 USA. RP Harwood, L (reprint author), Jefferson Lab, 12000 Jefferson Ave, Newport News, VA 23606 USA. NR 6 TC 0 Z9 0 U1 0 U2 0 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1148-7 J9 AIP CONF PROC PY 2013 VL 1525 BP 595 EP 599 DI 10.1063/1.4802397 PG 5 WC Physics, Applied; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFI58 UT WOS:000319997900118 ER PT S AU Boswell, MS Young, AR Ejiri, H AF Boswell, M. S. Young, A. R. Ejiri, H. BE McDaniel, FD Doyle, BL Glass, GA Wang, Y TI Gamow-Teller Strength Studied Through Gamma-Excitation Of Isobaric Analog States SO APPLICATION OF ACCELERATORS IN RESEARCH AND INDUSTRY SE AIP Conference Proceedings LA English DT Proceedings Paper CT 22nd International Conference on the Application of Accelerators in Research and Industry (CAARI) CY AUG 05-10, 2012 CL Fort Worth, TX SP Sandia Natl Labs, Univ N Texas, Los Alamos Natl Lab, Pacific NW Natl Lab, High Voltage Engn Europa B V, Kurt J Lester Co, Natl Electrostat Corp DE double beta decay; free electron lasers; nuclear structure; Gamow-Teller transitions; beta decay AB We consider a measurement of isobaric analog states (IAS) of 76As in 76Se as a method for measuring the Gamow-Teller (GT) strength important to constrain and possibly help normalize calculations of double beta (beta beta) decay matrix elements. We show that photo-nuclear reactions via IAS can provide valuable information about the parent and daughter states of beta beta-decay not currently available from measurements of charge exchange reactions. Several experiments have been proposed at the HI square S facility at the Triangle Nuclear Research Laboratory in Durham, NC, the first of which will measure the lowest 1(-), 1(+) and 2(+) IAS in Se-76. C1 [Boswell, M. S.] Los Alamos Natl Lab, Div Phys, Los Alamos, NM 87545 USA. RP Boswell, MS (reprint author), Los Alamos Natl Lab, Div Phys, Los Alamos, NM 87545 USA. FU US Department of Energy through the LANL/LDRD Program; U.S. Department of Energy; Office of Nuclear Physics [2011LANLE9BW] FX We gratefully acknowledge the support of the US Department of Energy through the LANL/LDRD Program for part of this work. We also acknowledge the support of the U.S. Department of Energy, Office of Nuclear Physics under Contract No. 2011LANLE9BW. NR 17 TC 0 Z9 0 U1 0 U2 1 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1148-7 J9 AIP CONF PROC PY 2013 VL 1525 BP 600 EP 603 DI 10.1063/1.4802398 PG 4 WC Physics, Applied; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFI58 UT WOS:000319997900119 ER PT S AU Allmond, JM AF Allmond, J. M. BE McDaniel, FD Doyle, BL Glass, GA Wang, Y TI Direct-Reaction Studies By Particle-gamma Coincidence Spectroscopy Using Csi-Hpge And Si-Hpge Arrays SO APPLICATION OF ACCELERATORS IN RESEARCH AND INDUSTRY SE AIP Conference Proceedings LA English DT Proceedings Paper CT 22nd International Conference on the Application of Accelerators in Research and Industry (CAARI) CY AUG 05-10, 2012 CL Fort Worth, TX SP Sandia Natl Labs, Univ N Texas, Los Alamos Natl Lab, Pacific NW Natl Lab, High Voltage Engn Europa B V, Kurt J Lester Co, Natl Electrostat Corp DE direct reaction; transfer reaction; particle-gamma coincidence spectroscopy; angular correlation ID SURROGATE REACTION TECHNIQUE; SILICON DETECTOR ARRAY; REX-ISOLDE; INVERSE KINEMATICS; BEAM; SPECTROMETER; RAY; GAMMASPHERE; SCATTERING; NUCLEI AB Particle-gamma and particle-gamma-gamma coincidence spectroscopy has several advantages in the study of direct reactions (particularly in inverse kinematics) since it can generally allow determination of: decay paths; high-precision level energies; multipolarities of transitions; and cross sections. Techniques for studying direct reactions by particle-gamma coincidence spectroscopy are presented for two cases: (1) heavy-ion reactions with CsI-HPGe, and (2) light-ion reactions with Si-HPGe. Future direct-reaction studies with radioactive ion beams (RIBs) will mostly involve low beam intensities and inverse kinematics (i.e., A(beam)>A(target)), which eliminates the traditional use of magnetic spectrometers. Particle-gamma coincidence spectroscopy currently provides the most viable method to study direct reactions with nuclei of any level density. In the present study, the capabilities and limitations of the technique are explored. C1 Oak Ridge Natl Lab, Joint Inst Heavy Ion Res, Oak Ridge, TN 37831 USA. RP Allmond, JM (reprint author), Oak Ridge Natl Lab, Joint Inst Heavy Ion Res, Oak Ridge, TN 37831 USA. OI Allmond, James Mitchell/0000-0001-6533-8721 NR 57 TC 1 Z9 1 U1 0 U2 1 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1148-7 J9 AIP CONF PROC PY 2013 VL 1525 BP 610 EP 615 DI 10.1063/1.4802400 PG 6 WC Physics, Applied; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFI58 UT WOS:000319997900121 ER PT S AU Rajasekhara, S Ferreira, PJ Hattar, K AF Rajasekhara, S. Ferreira, P. J. Hattar, K. BE McDaniel, FD Doyle, BL Glass, GA Wang, Y TI Microstructural Evolution Of Nanocrystalline Nickel Thin Films Due To High-Energy Heavy-Ion Irradiation SO APPLICATION OF ACCELERATORS IN RESEARCH AND INDUSTRY SE AIP Conference Proceedings LA English DT Proceedings Paper CT 22nd International Conference on the Application of Accelerators in Research and Industry (CAARI) CY AUG 05-10, 2012 CL Fort Worth, TX SP Sandia Natl Labs, Univ N Texas, Los Alamos Natl Lab, Pacific NW Natl Lab, High Voltage Engn Europa B V, Kurt J Lester Co, Natl Electrostat Corp (NEC) DE Nanocrystalline nickel; ion irradiation; precession electron diffraction microscopy ID ELECTRON-DIFFRACTION INTENSITIES; LASER DEPOSITED NICKEL; ABNORMAL GRAIN-GROWTH; RADIATION-DAMAGE; BOMBARDMENT; HE AB This initial feasibility study demonstrates that recent advancements in precession electron diffraction microscopy can be applied to nanostructured metals exposed to high displacement damage from a Tandem accelerator. In this study, high purity, nanocrystalline, free-standing nickel thin films produced by pulsed laser deposition were irradiated with approximately 3 x 10(14) ions/cm(2) of 35 MeV Ni6+ ions resulting in an approximately uniform damage profile to approximately 16 dpa. Pristine and ion-irradiated regions of the nanocrystalline Ni films were characterized by conventional transmission electron microscopy and precession electron diffraction microscopy. Precession electron diffraction microscopy provided additional insight into the texture, phase, and grain boundary distribution resulting from the displacement damage that could not be obtained from traditional electron microscopy techniques. For the nanocrystalline nickel film studied, this included the growth in number and percentage of a metastable hexagonal closed packed phase grains and the formation of large < 001 > textured face centered cubic grains. The application of precession electron diffraction microscopy to characterize other nanocrystalline metals, which are being considered for radiation tolerant applications, will permit a comparison of materials that goes beyond the dominant length scale to consider the effects of local phase, texture, and grain boundary or interface information. C1 [Rajasekhara, S.; Hattar, K.] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Rajasekhara, S (reprint author), Sandia Natl Labs, POB 5800 MS 1056, Albuquerque, NM 87185 USA. NR 31 TC 1 Z9 1 U1 3 U2 22 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1148-7 J9 AIP CONF PROC PY 2013 VL 1525 BP 630 EP 635 DI 10.1063/1.4802404 PG 6 WC Physics, Applied; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFI58 UT WOS:000319997900125 ER PT S AU Quinn, H AF Quinn, Heather BE McDaniel, FD Doyle, BL Glass, GA Wang, Y TI The Use Of Accelerated Radiation Testing For Avionics SO APPLICATION OF ACCELERATORS IN RESEARCH AND INDUSTRY SE AIP Conference Proceedings LA English DT Proceedings Paper CT 22nd International Conference on the Application of Accelerators in Research and Industry (CAARI) CY AUG 05-10, 2012 CL Fort Worth, TX SP Sandia Natl Labs, Univ N Texas, Los Alamos Natl Lab, Pacific NW Natl Lab, High Voltage Engn Europa B V, Kurt J Lester Co, Natl Electrostat Corp (NEC) DE neutron radiation; single-event effects; accelerated facilities AB In recent years, the use of unmanned aerial vehicles (UAVs) for military and national security applications has been increasing. One possible use of these vehicles is as remote sensing platforms, where the UAV carries several sensors to provide real-time information about biological, chemical or radiological agents that might have been released into the environment. One such UAV, the Global Hawk, has a payload space that can carry nearly one ton of sensing equipment, which makes these platforms significantly larger than many satellites. Given the size of the potential payload and the heightened radiation environment at high altitudes, these systems could be affected by the radiation-induced failure mechanisms from the naturally occurring terrestrial environment. In this paper, we will explore the use of accelerated radiation testing to prepare UAV payloads for deployment. C1 Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Quinn, H (reprint author), Los Alamos Natl Lab, ISR-3 MS D440, Los Alamos, NM 87545 USA. NR 5 TC 0 Z9 0 U1 0 U2 0 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1148-7 J9 AIP CONF PROC PY 2013 VL 1525 BP 643 EP 648 DI 10.1063/1.4802406 PG 6 WC Physics, Applied; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFI58 UT WOS:000319997900127 ER PT S AU McCloy, JS Jiang, WL Sundararajan, JA Qiang, Y Burks, E Liu, K AF McCloy, John S. Jiang, Weilin Sundararajan, Jennifer A. Qiang, You Burks, Edward Liu, Kai BE McDaniel, FD Doyle, BL Glass, GA Wang, Y TI Structure And Magnetic Properties Of Irradiated Fe-Fe Oxide Core-Shell Nanoclusters SO APPLICATION OF ACCELERATORS IN RESEARCH AND INDUSTRY SE AIP Conference Proceedings LA English DT Proceedings Paper CT 22nd International Conference on the Application of Accelerators in Research and Industry (CAARI) CY AUG 05-10, 2012 CL Fort Worth, TX SP Sandia Natl Labs, Univ N Texas, Los Alamos Natl Lab, Pacific NW Natl Lab, High Voltage Engn Europa B V, Kurt J Lester Co, Natl Electrostat Corp (NEC) DE nanocluster; granular magnetite film; ion irradiation; first-order reversal curve ID PARTICLES AB A cluster deposition method was used to produce a film of loosely aggregated particles of Fe-Fe3O4 core-shell nanoclusters with an 8 nm iron core size and 2 nm oxide shell thickness. The film of particles on a silicon substrate was irradiated with 5.5 MeV Si2+ ions to a fluence of 10(16) cm(-2) near room temperature, and computer simulations based on the SRIM (Stopping and Range of Ions in Matter) code show that the implanted Si species stops near the film-substrate interface. The ion irradiation creates a structural change in the film with corresponding chemical and magnetic changes. X-ray diffraction shows that the core size and chemistry stay the same but the shell becomes FeO that grows to a thickness of 17 nm. Helium ion microscopy shows that the previously separate particles have densified into a nearly continuous film. Major loop magnetic hysteresis measurements show a decrease in saturation magnetization that we attribute to the presence of the antiferromagnetic (AFM) FeO shell. First-order reversal curve measurements on the irradiated film performed with a vibrating sample magnetometer show that the AFM shell prevents the particles from interacting magnetically, leading to low coercivity from the iron core and little bias field from the core interactions. These results, and others reported previously on different compositions (Fe3O4 or FeO + Fe3N nanoclusters), show that the ion irradiation behavior of nanocluster films such as these depends strongly on the initial nanostructure and chemistry. C1 [McCloy, John S.; Jiang, Weilin] Pacific NW Natl Lab, Richland, WA 99352 USA. RP McCloy, JS (reprint author), Pacific NW Natl Lab, 902 Battelle Blvd,POB 999, Richland, WA 99352 USA. RI McCloy, John/D-3630-2013; Liu, Kai/B-1163-2008 OI McCloy, John/0000-0001-7476-7771; Jiang, Weilin/0000-0001-8302-8313; Liu, Kai/0000-0001-9413-6782 NR 18 TC 3 Z9 3 U1 1 U2 14 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1148-7 J9 AIP CONF PROC PY 2013 VL 1525 BP 659 EP 662 DI 10.1063/1.4802409 PG 4 WC Physics, Applied; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFI58 UT WOS:000319997900130 ER PT S AU Tang, V Rusnak, B Falabella, S Hawkins, S McCarrick, JF Wang, H Hall, JM Ellsworth, J AF Tang, V. Rusnak, B. Falabella, S. Hawkins, S. McCarrick, J. F. Wang, H. Hall, J. M. Ellsworth, J. BE McDaniel, FD Doyle, BL Glass, GA Wang, Y TI Accelerator Driven Gamma And Fast Neutron Radiography Test-Bed At Lawrence Livermore National Laboratory SO APPLICATION OF ACCELERATORS IN RESEARCH AND INDUSTRY SE AIP Conference Proceedings LA English DT Proceedings Paper CT 22nd International Conference on the Application of Accelerators in Research and Industry (CAARI) CY AUG 05-10, 2012 CL Fort Worth, TX SP Sandia Natl Labs, Univ N Texas, Los Alamos Natl Lab, Pacific NW Natl Lab, High Voltage Engn Europa B V, Kurt J Lester Co, Natl Electrostat Corp (NEC) DE fusion gammas; neutrons; radiography; NDE; imaging ID 12C(D AB Accelerator driven fusion gammas and fast neutrons could provide unique radiography capabilities due to their ability to produce both high and low energy mono-energetic gammas and neutrons compared with broadband bremsstrahlung based x-ray sources. The possibility of simultaneously obtaining both gamma and neutron radiographs using one source could allow complex objects composed of a large range of low to high Z materials to be imaged. In this paper we review a 4 MV RFQ accelerator driven radiography test-bed at LLNL designed to study the physics involved in applying these dual output fusion reactions for radiography applications. First experimental neutron images from a carbon target are presented. C1 [Tang, V.; Rusnak, B.; Falabella, S.; Hawkins, S.; McCarrick, J. F.; Wang, H.; Hall, J. M.; Ellsworth, J.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. RP Tang, V (reprint author), Lawrence Livermore Natl Lab, 7000 East Ave, Livermore, CA 94550 USA. NR 11 TC 1 Z9 1 U1 1 U2 5 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1148-7 J9 AIP CONF PROC PY 2013 VL 1525 BP 714 EP 719 DI 10.1063/1.4802420 PG 6 WC Physics, Applied; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFI58 UT WOS:000319997900141 ER PT S AU Chen, AX Antolak, AJ Leung, KN Raber, TN Morse, DH AF Chen, A. X. Antolak, A. J. Leung, K. -N. Raber, T. N. Morse, D. H. BE McDaniel, FD Doyle, BL Glass, GA Wang, Y TI Pulsed Pyroelectric Crystal-Powered Gamma Source SO APPLICATION OF ACCELERATORS IN RESEARCH AND INDUSTRY SE AIP Conference Proceedings LA English DT Proceedings Paper CT 22nd International Conference on the Application of Accelerators in Research and Industry (CAARI) CY AUG 05-10, 2012 CL Fort Worth, TX SP Sandia Natl Labs, Univ N Texas, Los Alamos Natl Lab, Pacific NW Natl Lab, High Voltage Engn Europa B V, Kurt J Lester Co, Natl Electrostat Corp (NEC) DE pyroelectric; gamma source; RF source; d-Be reaction ID ION-SOURCE; DRIVEN AB A compact pulsed gamma generator is being developed to replace radiological sources used in commercial, industrial and medical applications. Mono-energetic gammas are produced in the 0.4 - 1.0 MeV energy range using nuclear reactions such as Be-9(d,n gamma)B-10. The gamma generator employs an RF-driven inductively coupled plasma ion source to produce deuterium ion current densities up to 2 mA/mm(2) and ampere-level current pulses can be attained by utilizing an array extraction grid. The extracted deuterium ions are accelerated to approximately 300 keV via a compact stacked pyroelectric crystal system and then bombard the beryllium target to generate gammas. The resulting microsecond pulse of gammas is equivalent to a radiological source with curie-level activity. C1 [Chen, A. X.; Antolak, A. J.; Leung, K. -N.; Raber, T. N.; Morse, D. H.] Sandia Natl Labs, Livermore, CA 94550 USA. RP Chen, AX (reprint author), Sandia Natl Labs, Livermore, CA 94550 USA. NR 15 TC 2 Z9 2 U1 0 U2 6 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1148-7 J9 AIP CONF PROC PY 2013 VL 1525 BP 720 EP 724 DI 10.1063/1.4802421 PG 5 WC Physics, Applied; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFI58 UT WOS:000319997900142 ER PT S AU Norgard, P Kovaleski, SD VanGordon, JA Baxter, EA Gall, BB Kwon, JW Kim, BH Dale, GE AF Norgard, P. Kovaleski, S. D. VanGordon, J. A. Baxter, E. A. Gall, B. B. Kwon, Jae Wan Kim, Baek Hyun Dale, G. E. BE McDaniel, FD Doyle, BL Glass, GA Wang, Y TI A Compact Ion Source And Accelerator Based On A Piezoelectric Driver SO APPLICATION OF ACCELERATORS IN RESEARCH AND INDUSTRY SE AIP Conference Proceedings LA English DT Proceedings Paper CT 22nd International Conference on the Application of Accelerators in Research and Industry (CAARI) CY AUG 05-10, 2012 CL Fort Worth, TX SP Sandia Natl Labs, Univ N Texas, Los Alamos Natl Lab, Pacific NW Natl Lab, High Voltage Engn Europa B V, Kurt J Lester Co, Natl Electrostat Corp DE Piezoelectric transformer; compact neutron source; piezoelectric transformer plasma source AB Compact ion sources and accelerators using piezoelectric devices for the production of energetic ion beams are being evaluated. A coupled source-accelerator is being tested as a neutron source to be incorporated into oil-well logging diagnostics. Two different ion sources are being investigated, including a piezoelectric transformer-based plasma source and a silicon-based field ion source. The piezoelectric transformer plasma ion source uses a cylindrical, resonantly driven piezoelectric crystal to produce high voltage inside a confined volume filled with low pressure deuterium gas. The plasma generated in the confined chamber is ejected through a small aperture into an evacuated drift region. The silicon field ion source uses localized electric field enhancement produced by an array of sharp emitters etched into a silicon blank to produce ions through field desorption ionization. A second piezoelectric device of a different design is used to generate an accelerating potential on the order of 130 kV; this potential is applied to a deuterated target plate positioned perpendicular to the ion stream produced by either plasma source. This paper discusses the results obtained by the individual components as they relate to the final neutron source. C1 [Norgard, P.; Kovaleski, S. D.; VanGordon, J. A.; Baxter, E. A.; Gall, B. B.; Kwon, Jae Wan; Kim, Baek Hyun] Univ Missouri, Elect & Comp Engn Dept, 349 Engn Bldg West, Columbia, MO 65211 USA. [Dale, G. E.] Los Alamos Natl Lab, High Power Electdynam Grp, Los Alamos, NM 87545 USA. RP Norgard, P (reprint author), Univ Missouri, Elect & Comp Engn Dept, 349 Engn Bldg West, Columbia, MO 65211 USA. OI Norgard, Peter/0000-0002-5332-5998; Kovaleski, Scott/0000-0002-5831-6388 FU Qynergy and Los Alamos National Laboratory FX This work was supported by Qynergy and Los Alamos National Laboratory NR 10 TC 0 Z9 0 U1 0 U2 1 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1148-7 J9 AIP CONF PROC PY 2013 VL 1525 BP 725 EP 730 DI 10.1063/1.4802422 PG 6 WC Physics, Applied; Physics, Nuclear; Physics, Particles & Fields SC Physics GA BFI58 UT WOS:000319997900143 ER PT J AU Burrows, SM Rayner, PJ Butler, T Lawrence, MG AF Burrows, S. M. Rayner, P. J. Butler, T. Lawrence, M. G. TI Estimating bacteria emissions from inversion of atmospheric transport: sensitivity to modelled particle characteristics SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID CHEMISTRY-CLIMATE MODEL; SUBMODEL SYSTEM MESSY; TRACER TRANSPORT; TECHNICAL NOTE; CONVECTION PARAMETERISATIONS; DIFFERENT ECOSYSTEMS; GLOBAL SIMULATIONS; AEROSOL-PARTICLES; IMPLEMENTATION; FORMULATIONS AB Model-simulated transport of atmospheric trace components can be combined with observed concentrations to obtain estimates of ground-based sources using various inversion techniques. These approaches have been applied in the past primarily to obtain source estimates for long-lived trace gases such as CO2. We consider the application of similar techniques to source estimation for atmospheric aerosols, using as a case study the estimation of bacteria emissions from different ecosystem regions in the global atmospheric chemistry and climate model ECHAM5/MESSy-Atmospheric Chemistry (EMAC). Source estimation via Markov Chain Monte Carlo is applied to a suite of sensitivity simulations, and the global mean emissions are estimated for the example problem of bacteria-containing aerosol particles. We present an analysis of the uncertainties in the global mean emissions, and a partitioning of the uncertainties that are attributable to particle size, activity as cloud condensation nuclei (CCN), the ice nucleation scavenging ratios for mixed-phase and cold clouds, and measurement error. \ For this example, uncertainty due to CCN activity or to a 1 mu m error in particle size is typically between 10% and 40% of the uncertainty due to observation uncertainty, as measured by the 5-95th percentile range of the Monte Carlo ensemble. Uncertainty attributable to the ice nucleation scavenging ratio in mixed-phase clouds is as high as 10-20% of that attributable to observation uncertainty. Taken together, the four model parameters examined contribute about half as much to the uncertainty in the estimated emissions as do the observations. This was a surprisingly large contribution from model uncertainty in light of the substantial observation uncertainty, which ranges from 81-870% of the mean for each of ten ecosystems for this case study. The effects of these and other model parameters in contributing to the uncertainties in the transport of atmospheric aerosol particles should be treated explicitly and systematically in both forward and inverse modelling studies. C1 [Burrows, S. M.; Butler, T.; Lawrence, M. G.] Max Planck Inst Chem, D-55128 Mainz, Germany. [Rayner, P. J.] Univ Melbourne, Sch Earth Sci, Melbourne, Vic, Australia. RP Burrows, SM (reprint author), Pacific NW Natl Lab, Richland, WA 99352 USA. EM susannah.burrows@pnnl.gov RI Burrows, Susannah/A-7429-2011 OI Burrows, Susannah/0000-0002-0745-7252 FU U. S. Department of Energy; Australian Professorial Fellowship [DP1096309] FX Susannah Burrows was supported in part by the U. S. Department of Energy as part of the Earth System Modeling Program. Peter Rayner is in receipt of an Australian Professorial Fellowship (DP1096309). We gratefully acknowledge the efforts of the EMAC development team to develop and make available the EMAC modelling system. NR 55 TC 5 Z9 5 U1 1 U2 17 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1680-7316 J9 ATMOS CHEM PHYS JI Atmos. Chem. Phys. PY 2013 VL 13 IS 11 BP 5473 EP 5488 DI 10.5194/acp-13-5473-2013 PG 16 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA 164AD UT WOS:000320380200004 ER PT J AU Jin, H Won, N Ahn, B Kwag, J Heo, K Oh, JW Sun, YT Cho, SG Lee, SW Kim, S AF Jin, Ho Won, Nayoun Ahn, Boeun Kwag, Jungheon Heo, Kwang Oh, Jin-Woo Sun, Yintao Cho, Soo Gyeong Lee, Seung-Wuk Kim, Sungjee TI Quantum dot-engineered M13 virus layer-by-layer composite films for highly selective and sensitive turn-on TNT sensors SO CHEMICAL COMMUNICATIONS LA English DT Article ID NANOCRYSTALS; FLUORESCENCE; EXPLOSIVES; HYBRID; QDS; CDS AB We developed quantum dot-engineered M13 virus layer-by-layer hybrid composite films with incorporated fluorescence quenchers. TNT is designed to displace the quenchers and turn on the quantum dot fluorescence. TNT was detected at the sub ppb level with a high selectivity. C1 [Jin, Ho; Won, Nayoun; Ahn, Boeun; Kim, Sungjee] Pohang Univ Sci & Technol POSTECH, Dept Chem, Pohang 790784, South Korea. [Kwag, Jungheon; Kim, Sungjee] POSTECH, Sch Interdisciplinary Biosci & Bioengn, Pohang, South Korea. [Heo, Kwang; Oh, Jin-Woo; Sun, Yintao; Lee, Seung-Wuk] Univ Calif Berkeley, Dept Bioengn, Berkeley, CA 94720 USA. [Heo, Kwang; Oh, Jin-Woo; Sun, Yintao; Lee, Seung-Wuk] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA 94720 USA. [Cho, Soo Gyeong] Agcy Def Dev, Def Adv R&D Ctr, Taejon 305600, South Korea. RP Kim, S (reprint author), Pohang Univ Sci & Technol POSTECH, Dept Chem, Pohang 790784, South Korea. EM sungjee@postech.ac.kr RI Heo, Kwang/B-1133-2015; OI Kim, Sungjee/0000-0002-1289-1926 FU Defense Acquisition Program Administration; Agency for Defense Development [ADD-08-11-03]; KOSEF grant; MOST [20120006280, 2009-0094036]; NRF; Center of Integrated Nanomechanical Systems (COINS) of the National Science Foundation [EEC-0832819] FX This work was supported by Defense Acquisition Program Administration and Agency for Defense Development under the contract ADD-08-11-03, KOSEF grant funded by MOST (20120006280), and Basic Science Research Program through NRF funded by MOST (2009-0094036). LWS acknowledges support from Center of Integrated Nanomechanical Systems (COINS) of the National Science Foundation (Grant No. EEC-0832819). NR 22 TC 8 Z9 9 U1 1 U2 57 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1359-7345 J9 CHEM COMMUN JI Chem. Commun. PY 2013 VL 49 IS 54 BP 6045 EP 6047 DI 10.1039/c3cc42032a PG 3 WC Chemistry, Multidisciplinary SC Chemistry GA 161ND UT WOS:000320199000012 PM 23722503 ER PT J AU Carraher, JM Bakac, A AF Carraher, Jack M. Bakac, Andreja TI Alkyl group versus hydrogen atom transfer from metal alkyls to macrocyclic rhodium complexes SO CHEMICAL COMMUNICATIONS LA English DT Article ID LIVING RADICAL POLYMERIZATION; HOMOLYTIC SUBSTITUTION; ORGANIC RADICALS; VINYL-ACETATE; CARBON BONDS; COBALT; INVERSION; KINETICS; ABSTRACTION; DIALKYLZINC AB Macrocyclic rhodium(II) complexes LRh(H2O)(2+) react with (dmgH)(2)-(H2O)CoR and with (H2O)(5)CrR2+ by alkyl transfer for R = CH3 to generate L(H2O)RhCH32+. When R = C2H5, C3H7 or C4H9, the reaction takes place by hydrogen atom abstraction from the coordinated alkyl and produces L(H2O)RhH2+ and an alpha-olefin. C1 [Bakac, Andreja] Iowa State Univ, Ames Lab, Ames, IA 50011 USA. Iowa State Univ, Dept Chem, Ames, IA 50011 USA. RP Bakac, A (reprint author), Iowa State Univ, Ames Lab, Ames, IA 50011 USA. EM carraher@iastate.edu; bakac@ameslab.gov FU U.S. Department of Energy, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division through the Ames Laboratory; U.S. Department of Energy [DE-AC02-07CH11358] FX This research was supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division through the Ames Laboratory. The Ames Laboratory is operated for the U.S. Department of Energy by Iowa State University under Contract No. DE-AC02-07CH11358. NR 28 TC 1 Z9 1 U1 0 U2 8 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 54 BP 6099 EP 6101 DI 10.1039/c3cc43472a PG 3 WC Chemistry, Multidisciplinary SC Chemistry GA 161ND UT WOS:000320199000030 PM 23727728 ER PT J AU Cernusak, LA Winter, K Dalling, JW Holtum, JAM Jaramillo, C Korner, C Leakey, ADB Norby, RJ Poulter, B Turner, BL Wright, SJ AF Cernusak, Lucas A. Winter, Klaus Dalling, James W. Holtum, Joseph A. M. Jaramillo, Carlos Koerner, Christian Leakey, Andrew D. B. Norby, Richard J. Poulter, Benjamin Turner, Benjamin L. Wright, S. Joseph TI Tropical forest responses to increasing atmospheric CO2: current knowledge and opportunities for future research SO FUNCTIONAL PLANT BIOLOGY LA English DT Review DE carbon storage; CO2 enrichment; liana; phosphorus; succession; water use efficiency ID WATER-USE EFFICIENCY; ELEVATED CARBON-DIOXIDE; AMAZON RAIN-FOREST; SOIL ORGANIC PHOSPHORUS; GLOBAL VEGETATION MODEL; BARRO-COLORADO ISLAND; BASIN-WIDE VARIATIONS; FICUS-INSIPIDA WILLD; STOMATAL CONDUCTANCE; LONG-TERM AB Elevated atmospheric CO2 concentrations (ca) will undoubtedly affect the metabolism of tropical forests worldwide; however, critical aspects of how tropical forests will respond remain largely unknown. Here, we review the current state of knowledge about physiological and ecological responses, with the aim of providing a framework that can help to guide future experimental research. Modelling studies have indicated that elevated ca can potentially stimulate photosynthesis more in the tropics than at higher latitudes, because suppression of photorespiration by elevated ca increases with temperature. However, canopy leaves in tropical forests could also potentially reach a high temperature threshold under elevated ca that will moderate the rise in photosynthesis. Belowground responses, including fine root production, nutrient foraging and soil organic matter processing, will be especially important to the integrated ecosystem response to elevated ca. Water use efficiency will increase as ca rises, potentially impacting upon soil moisture status and nutrient availability. Recruitment may be differentially altered for some functional groups, potentially decreasing ecosystem carbon storage. Whole-forest CO2 enrichment experiments are urgently needed to test predictions of tropical forest functioning under elevated ca. Smaller scale experiments in the understorey and in gaps would also be informative, and could provide stepping stones towards stand-scale manipulations. C1 [Cernusak, Lucas A.] James Cook Univ, Sch Marine & Trop Biol, Cairns, Qld 4878, Australia. [Winter, Klaus; Holtum, Joseph A. M.; Jaramillo, Carlos; Turner, Benjamin L.] Smithsonian Trop Res Inst, Balboa, Ancon, Panama. [Dalling, James W.; Leakey, Andrew D. B.] Univ Illinois, Dept Plant Biol, Urbana, IL 61801 USA. [Holtum, Joseph A. M.] James Cook Univ, Sch Marine & Trop Biol, Townsville, Qld 4811, Australia. [Koerner, Christian] Univ Basel, Inst Bot, CH-4056 Basel, Switzerland. [Norby, Richard J.] Oak Ridge Natl Lab, Div Environm Sci, Oak Ridge, TN 37831 USA. [Norby, Richard J.] Oak Ridge Natl Lab, Climate Change Sci Inst, Oak Ridge, TN 37831 USA. [Poulter, Benjamin] Univ Versailles St Quentin, F-91191 Versailles, France. RP Cernusak, LA (reprint author), James Cook Univ, Sch Marine & Trop Biol, Cairns, Qld 4878, Australia. EM lcernusak@gmail.com RI Cernusak, Lucas/A-6859-2011; Turner, Benjamin/E-5940-2011; Korner, Christian/B-6592-2014; James Cook University, TESS/B-8171-2012; Wright, Stuart/M-3311-2013; Research ID, CTBCC /O-3564-2014; Norby, Richard/C-1773-2012; Leakey, Andrew/Q-9889-2016 OI Poulter, Benjamin/0000-0002-9493-8600; Cernusak, Lucas/0000-0002-7575-5526; Turner, Benjamin/0000-0002-6585-0722; Wright, Stuart/0000-0003-4260-5676; Norby, Richard/0000-0002-0238-9828; Leakey, Andrew/0000-0001-6251-024X FU Smithsonian Tropical Research Institute; Australian Research Council [FT100100329] FX This review resulted from a symposium held at the Smithsonian Tropical Research Institute on 31 March and 1 April 2011. Funding for the symposium was provided by the Smithsonian Tropical Research Institute. LAC was supported by a Future Fellowship from the Australian Research Council (FT100100329). NR 243 TC 31 Z9 32 U1 9 U2 142 PU CSIRO PUBLISHING PI COLLINGWOOD PA 150 OXFORD ST, PO BOX 1139, COLLINGWOOD, VICTORIA 3066, AUSTRALIA SN 1445-4408 J9 FUNCT PLANT BIOL JI Funct. Plant Biol. PY 2013 VL 40 IS 6 BP 531 EP 551 DI 10.1071/FP12309 PG 21 WC Plant Sciences SC Plant Sciences GA 162NH UT WOS:000320271400001 ER PT S AU Li, H Li, ST AF Li, Hui Li, Shengtai BE Barge, P Jorda, L TI 3D Simulations of Type-I Migration in Nearly Laminar Disks SO INSTABILITIES AND STRUCTURES IN PROTO-PLANETARY DISKS SE EPJ Web of Conferences LA English DT Proceedings Paper CT Workshop on Instabilities and Structures in Proto-Planetary Disks CY SEP 17-20, 2012 CL Marseille, FRANCE SP AMU, Lab Astrophysique Marseille (LAM) ID PLANET MIGRATION; COROTATION; TORQUES AB We report results from 3D hydrodynamic disk simulations with an embedded planet. We examine the planet's migration dependence on the disk viscosity. We find that the Type I migration can be slowed down significantly in low viscosity disks. The density feedback effect that was studied in 2D simulations still exists in 3D disks and causes the slowing down of Type I. Future work will address further the quantitative differences between 3D and 2D in slowing down the migration. C1 [Li, Hui; Li, Shengtai] Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. RP Li, H (reprint author), Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. EM hli@lanl.gov; sli@lanl.gov OI Li, Shengtai/0000-0002-4142-3080 NR 13 TC 0 Z9 0 U1 0 U2 0 PU E D P SCIENCES PI CEDEX A PA 17 AVE DU HOGGAR PARC D ACTIVITES COUTABOEUF BP 112, F-91944 CEDEX A, FRANCE SN 2100-014X BN 978-2-7598-0983-7 J9 EPJ WEB CONF PY 2013 VL 46 AR UNSP 05003 DI 10.1051/epjconf/20134605003 PG 4 WC Astronomy & Astrophysics SC Astronomy & Astrophysics GA BFH95 UT WOS:000319936900020 ER PT J AU Gaynor, JD Karakoti, AS Inerbaev, T Sanghavi, S Nachimuthu, P Shutthanandan, V Seal, S Thevuthasan, S AF Gaynor, James D. Karakoti, Ajay S. Inerbaev, Talgat Sanghavi, Shail Nachimuthu, P. Shutthanandan, V. Seal, S. Thevuthasan, S. TI Enzyme-free detection of hydrogen peroxide from cerium oxide nanoparticles immobilized on poly(4-vinylpyridine) self-assembled monolayers SO JOURNAL OF MATERIALS CHEMISTRY B LA English DT Article ID OXIDATIVE STRESS; REACTIVE OXYGEN; NEURODEGENERATIVE DISEASES; ALZHEIMERS-DISEASE; FLUORESCENT-PROBES; SURFACE; CANCER; CELLS AB A simple enzyme-free spectrophotometric detection of hydrogen peroxide is demonstrated based on its colorimetric reaction with oxygen deficient cerium oxide nanoparticles (CNPs). This colorimetric sensitivity of CNPs towards H2O2 increases significantly with decreasing crystallite size due to an increase in the surface area as well as the concentration of Ce3+ on the surface. The origin of this colorimetric reaction was studied using DFT that suggests the adsorption of peroxide and oxygen molecules on ceria nanoparticles creates new states in the electronic structure leading to transitions absorbing in the visible region of the electromagnetic spectrum. For detection, a single layer of nanoparticles was immobilized on transparent microscopic glass slides using self-assembled monolayers (SAMs) of poly(4-vinylpyridine) (PVP). Cluster-free and uniform immobilization of nanoparticles was confirmed from atomic force microscopy (AFM) and helium ion microscopy (HIM). UV-Visible absorption measurements showed a concentration dependent increase in absorbance from immobilized CNPs that were exposed to increasing concentrations (10-400 mu M) of hydrogen peroxide. The immobilized CNPs can be baked at 80 degrees C after initial use to regenerate the sensor for reuse. The development of a direct, reusable, enzyme-free and dye-free peroxide sensing technology is possible and can be immediately applied in various areas, including biomedicine and national security. C1 [Gaynor, James D.] Univ Portland, Dept Chem, Portland, OR 97203 USA. [Gaynor, James D.; Sanghavi, Shail; Nachimuthu, P.; Shutthanandan, V.; Thevuthasan, S.] Pacific NW Natl Lab, EMSL, Richland, WA 99352 USA. [Karakoti, Ajay S.] Battelle Sci & Technol Pvt Ltd, Pune 411057, Maharashtra, India. [Inerbaev, Talgat] Gumilyov Eurasian Natl Univ, Astana 010008, Kazakhstan. [Seal, S.] Univ Cent Florida, Nanosci & Technol Ctr, Adv Mat Proc Anal Ctr, Orlando, FL 32826 USA. RP Karakoti, AS (reprint author), Battelle Sci & Technol Pvt Ltd, 302 Panchshil Technol Pk, Pune 411057, Maharashtra, India. EM Ajay.Karakoti@battelle-india.com FU Department of Energy's Office of Biological and Environmental Research; EMSL Intramural program; DOE Office of Science's SULI undergraduate research program; NSF-NIRT Program FX The research was performed using EMSL, a national scientific user facility sponsored by the Department of Energy's Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory and supported by the EMSL Intramural program. J. D. Gaynor was also supported by the DOE Office of Science's SULI undergraduate research program. Additional support from the NSF-NIRT Program supplemented this research as well. NR 34 TC 10 Z9 11 U1 3 U2 60 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-750X J9 J MATER CHEM B JI J. Mat. Chem. B PY 2013 VL 1 IS 28 BP 3443 EP 3450 DI 10.1039/c3tb20204f PG 8 WC Materials Science, Biomaterials SC Materials Science GA 171TJ UT WOS:000320951700002 ER PT J AU Wu, T Tyson, TA Bai, JM Pandya, K Jaye, C Fischer, D AF Wu, Tao Tyson, Trevor A. Bai, Jianming Pandya, Kaumudi Jaye, Cherno Fischer, Daniel TI On the origin of enhanced thermoelectricity in Fe doped Ca3Co4O9 SO JOURNAL OF MATERIALS CHEMISTRY C LA English DT Article ID MISFIT-LAYERED COBALTITE; SINGLE-CRYSTALS; THIN-FILMS; TRANSPORT-PROPERTIES; BI-SUBSTITUTION; GROWTH; OXIDES AB Resistivity and Seebeck coefficient measurements on Ca3Co4-xFexO9 (x = 0, 0.05, 0.1, 0.2 and 0.25) reveal enhanced thermoelectric performance with an optimal x value of 0.2. X-ray diffraction measurements show continuous Fe doping into the host lattice, while X-ray absorption experiments reveal that Fe substitutes for Co in the Ca2CoO3 (rock salt) block. The Fe substitution for Co produces electron doping. The local structure around Fe in the Ca2CoO3 block becomes disordered, while the structure in the conducting CoO2 layer becomes more ordered. The structural change in the CoO2 layer plays the key role to enhance the electron transport. The highest ordered structure is achieved at x = 0.2 with the lowest resistivity. Soft X-ray absorption measurements find no Co site spin-state change with Fe doping. Thermoelectric property enhancement associated with doping induced structural change points to a new approach for creating materials with improved ZT in complex oxide systems. C1 [Wu, Tao; Tyson, Trevor A.] New Jersey Inst Technol, Dept Phys, Newark, NJ 07102 USA. [Bai, Jianming] Brookhaven Natl Lab, Natl Synchrotron Light Source, Upton, NY 11973 USA. [Pandya, Kaumudi] Brookhaven Natl Lab, SAIC, Upton, NY 11973 USA. [Jaye, Cherno; Fischer, Daniel] Natl Inst Stand & Technol, Mat Sci & Engn Lab, Gaithersburg, MD 20899 USA. RP Tyson, TA (reprint author), New Jersey Inst Technol, Dept Phys, Newark, NJ 07102 USA. EM tyson@njit.edu RI Bai, Jianming/O-5005-2015 FU DOE [DE-FG02-07ER46402]; NSF MRI [DMR-0923032]; U.S. Department of Energy FX This work is supported by DOE Grant DE-FG02-07ER46402. The Physical Properties Measurements System was acquired under NSF MRI Grant DMR-0923032 (ARRA award). X-ray diffraction and X-ray absorption data acquisition were performed at Brookhaven National Laboratory's National Synchrotron Light Source (NSLS) which is funded by the U.S. Department of Energy. We are indebted to Prof. M. Croft of Rutgers University, for useful discussion on the structural changes accompanying doping and for providing the spectra for Fe K-edge XANES standards. NR 48 TC 17 Z9 17 U1 1 U2 61 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7526 J9 J MATER CHEM C JI J. Mater. Chem. C PY 2013 VL 1 IS 26 BP 4114 EP 4121 DI 10.1039/c3tc30481g PG 8 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA 163IX UT WOS:000320330600007 ER PT J AU Lu, HL Song, SQ Gu, XF He, SL Chen, CL Song, GB Cai, ZH Guo, HM Gao, HJ Sun, L AF Lu, Hongliang Song, Shuangqi Gu, Xiaofeng He, Shuli Chen, Chonglin Song, Gangbing Cai, Zhonghou Guo, Haiming Gao, Hongjun Sun, Li TI Piezoresponse Force Microscopy Study of Ferroelectric BaTiO3 Thin Film Directly Deposited on Si(001) by Magnetron Sputtering SO JOURNAL OF NANO RESEARCH LA English DT Article DE Ferroelectric; Thin Film; BaTiO3; Magnetron Sputtering ID PULSED-LASER DEPOSITION; OXIDE; SILICON; PHYSICS AB Direct integration of ferroelectrics with semiconductors is critical to lower the cost and simplify the production procedures for data storage/processing components and miniature sensor/actuator development. By optimizing magnetron sputtering parameters, highly <001> preferential growth of BaTiO3 thin films with reproducible ferroelectric responses have been achieved on Si(001) substrates. The thin film ferroelectric characteristics were systematically studied by piezoresponse force microscopy, and a piezoelectric coefficient d(33) of 24pm/V has been measured. It is found that the scanning tip sidewall angle and cantilever tilt affect the contour and size of polarized area. C1 [Lu, Hongliang; Song, Shuangqi; Song, Gangbing; Sun, Li] Univ Houston, Dept Mech Engn, Houston, TX 77204 USA. [Lu, Hongliang; Guo, Haiming; Gao, Hongjun] Chinese Acad Sci, Inst Phys, Beijing 100190, Peoples R China. [Gu, Xiaofeng] Jiangnan Univ, Dept Elect Engn, Minist Educ, Key Lab Adv Proc Control Light Ind, Wuxi 214122, Peoples R China. [He, Shuli] Capital Normal Univ, Dept Phys, Beijing 100037, Peoples R China. [Chen, Chonglin; Sun, Li] Univ Houston, Texas Ctr Superconduct, Houston, TX 77204 USA. [Chen, Chonglin] Univ Texas San Antonio, Dept Phys & Astron, San Antonio, TX 78249 USA. [Cai, Zhonghou] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. RP Lu, HL (reprint author), Univ Houston, Dept Mech Engn, Houston, TX 77204 USA. EM lsun4@uh.edu RI Gu, Xiaofeng/E-8287-2013 OI Gu, Xiaofeng/0000-0001-8299-6451 FU DOD TATRC award through the Alliance for Nano Health [W81XWH-09-2-0139]; 111 Project [B12018]; PAPD of Jiangsu Higher Education Institutions; U.S. Department of Energy Sciences, Office of Science [W-31-109-ENG-38] FX Financial support from DOD TATRC award W81XWH-09-2-0139 through the Alliance for Nano Health is gratefully acknowledged. XFG wants to thank the 111 Project (B12018) and PAPD of Jiangsu Higher Education Institutions for support. Use of the Advanced Photon Source is supported by the U.S. Department of Energy Sciences, Office of Science, under contract No. W-31-109-ENG-38. NR 28 TC 1 Z9 1 U1 4 U2 32 PU TRANS TECH PUBLICATIONS LTD PI STAFA-ZUERICH PA LAUBISRUTISTR 24, STAFA-ZUERICH, CH-8712, SWITZERLAND SN 1662-5250 J9 J NANO RES-SW JI J. Nano Res. PY 2013 VL 22 BP 23 EP 30 DI 10.4028/www.scientific.net/JNanoR.22.23 PG 8 WC Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Science & Technology - Other Topics; Materials Science; Physics GA 165MI UT WOS:000320487600003 ER PT J AU Fang, H Liang, G Zhao, L Wallace, T Arava, H Zhang, LL Ignatov, A Croft, MC AF Fang, Hui Liang, Gan Zhao, Liang Wallace, Timothy Arava, Hanu Zhang, Lu-Lu Ignatov, Alexander Croft, Mark C. TI Electrochemical Properties of Cathode Material LiFePO4 with Ti Substitution SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID LITHIUM IRON PHOSPHATE; ALIOVALENT SUBSTITUTIONS; ELECTRODE MATERIALS; IMPACT; BATTERIES AB Ti substituted LiFePO4 with nominal composition Li1-4yTiyFePO4 (y = 0, 0.01, 0.02, 0.03, 0.04, and 0.05) cathode materials were prepared by solid-state reaction. The as-prepared samples were characterized by X-ray diffraction, X-ray absorption spectroscopy, cyclic charge-discharge, cyclic voltammograms, and electrochemical impendence spectroscopy. The X-ray diffraction results indicate that the increase of Ti4+ amount leads to the expansion of the LiFePO4 lattice monotonically, but the XAS reveals that small amount of doped Ti can also form TiO2-anatase impurities. At 0.1 C rate, doping of Ti causes a decrease in charge and discharge capacities. However, at higher C rate, the charge/discharge capacities are improved. Li0.96Ti0.01FePO4 exhibits the optimized electrochemical performance. (C) 2013 The Electrochemical Society. C1 [Fang, Hui; Liang, Gan; Wallace, Timothy; Arava, Hanu] Sam Houston State Univ, Dept Phys, Huntsville, TX 77341 USA. [Zhao, Liang] Rice Univ, Dept Phys & Astron, Houston, TX 77005 USA. [Zhang, Lu-Lu] Huazhong Univ Sci & Technol, Sch Mat Sci & Engn, State Key Lab Mat Proc & Die & Mold Technol, Wuhan 430074, Hubei, Peoples R China. [Ignatov, Alexander; Croft, Mark C.] Rutgers State Univ, Dept Phys & Astron, Piscataway, NJ 08854 USA. [Croft, Mark C.] Brookhaven Natl Lab, NSLS, Upton, NY 11973 USA. RP Fang, H (reprint author), Sam Houston State Univ, Dept Phys, Huntsville, TX 77341 USA. EM hfang@shsu.edu FU National Science Foundation [CHE-0718482]; Research Corporation for Science Advancement; ERG grant from Sam Houston State University FX This work was supported by National Science Foundation under Grants (No. CHE-0718482), an award from Research Corporation for Science Advancement, and an ERG grant from Sam Houston State University NR 17 TC 6 Z9 6 U1 8 U2 46 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 5 BP A3148 EP A3152 DI 10.1149/2.024305jes PG 5 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA 161OI UT WOS:000320202800025 ER PT J AU Kim, Y Dudney, NJ Chi, MF Martha, SK Nanda, J Veith, GM Liang, CD AF Kim, Yoongu Dudney, Nancy J. Chi, Miaofang Martha, Surendra K. Nanda, Jagjit Veith, Gabriel M. Liang, Chengdu TI A Perspective on Coatings to Stabilize High-Voltage Cathodes: LiMn1.5Ni0.5O4 with Sub-Nanometer Lipon Cycled with LiPF6 Electrolyte SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID LITHIUM-ION BATTERIES; ATOMIC LAYER DEPOSITION; SPUTTERED THIN-FILM; LICOO2 CATHODES; ELECTROCHEMICAL PROPERTIES; LIPF6-BASED ELECTROLYTES; LINI0.5MN1.5O4 SPINEL; RECHARGEABLE BATTERIES; THERMAL-DECOMPOSITION; PHOSPHORUS OXYNITRIDE AB High voltage Li-ion cathodes push the limits of stability for both cathode and electrolyte. Here sub-nanometer coatings of an amorphous thin-film electrolyte (Lipon) improved the room temperature and 60 degrees C cycling stability of a LiMn1.5Ni0.5O4 spinel cathode when charged to 4.9 V with a standard LiPF6 carbonate electrolyte. The cathodes delivered superior C-rate performances up to a 5C discharge, when compared to the uncoated cathodes. Enhanced performance extended for at least 100 cycles. Electrochemical impedance spectroscopy indicates that Lipon slows the increase of interface resistance. Thicker 1-3 nm Lipon coatings are sufficiently insulating as to block electronic transport to the cathode particles. Thick coatings also slow Mn dissolution. Results suggest that Lipon may act to scavenge impurities or block active sites that promote electrolyte decomposition. While greatly improved by the Lipon coating, cycling is not yet sufficiently stable for applications requiring thousands of cycles or prolonged operation at higher temperatures. Further work is needed to assess what surface properties of coatings will ultimately stabilize the high voltage cathodes in carbonate liquid electrolyte cells. Comments include insight from other studies of Lipon-coated cathodes and the focus for future research. (C) 2013 The Electrochemical Society. C1 [Kim, Yoongu; Dudney, Nancy J.; Chi, Miaofang; Martha, Surendra K.; Nanda, Jagjit; Veith, Gabriel M.] Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN 37831 USA. [Liang, Chengdu] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. RP Kim, Y (reprint author), Infinite Power Solut, Littleton, CO 80127 USA. EM ygkim90@gmail.com; dudneynj@ornl.gov RI Chi, Miaofang/Q-2489-2015; Dudney, Nancy/I-6361-2016 OI Chi, Miaofang/0000-0003-0764-1567; Dudney, Nancy/0000-0001-7729-6178 FU Division of Materials Sciences and Engineering, Office of Basic Energy Sciences, U.S. Department of Energy; Division of Scientific User Facilities, U.S. Department of Energy FX Research sponsored by the Division of Materials Sciences and Engineering, Office of Basic Energy Sciences, U.S. Department of Energy. This includes fabrication, electrochemistry, and characterization by YGK, NJD, MFC, GMV. Electron microscopy was conducted at the Shared Research Equipment (SHaRE) user facility, which is sponsored by the Division of Scientific User Facilities, U.S. Department of Energy. Contributions of Raman spectroscopy by SKM and JN and assistance with cycle tests were supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office Of Vehicle Technologies of the U.S. Department of Energy. The raw materials were provided by nGimat Co. (GA, USA) for this research. NR 83 TC 22 Z9 22 U1 5 U2 148 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 EI 1945-7111 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2013 VL 160 IS 5 BP A3113 EP A3125 DI 10.1149/2.017305jes PG 13 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA 161OI UT WOS:000320202800020 ER PT J AU Li, Y Bettge, M Polzin, B Zhu, Y Balasubramanian, M Abraham, DP AF Li, Y. Bettge, M. Polzin, B. Zhu, Y. Balasubramanian, M. Abraham, D. P. TI Understanding Long-Term Cycling Performance of Li1.2Ni0.15Mn0.55Co0.1O2-Graphite Lithium-Ion Cells SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID X-RAY-ABSORPTION; CATHODE MATERIALS; HIGH-POWER; ELECTRODE MATERIALS; ELECTROCHEMICAL INTERCALATION; RAMAN-SPECTROSCOPY; LOCAL-STRUCTURE; ENERGY-STORAGE; HIGH-CAPACITY; OXYGEN LOSS AB Lithium-ion cells containing lithium and manganese rich layered-oxides (LMR-NMC) have gained significant attention in recent years because of their ability to deliver high energy densities. In this article we report on a comprehensive performance and degradation study of cells, containing Li1.2Ni1.5Mn0.55Co0.1O2 based positive electrodes and graphite based negative electrodes, on extended cycling. In addition to electrochemical measurements on full cells, characterization data on harvested electrodes by techniques that include scanning electron microscopy (SEM), X-ray diffraction (XRD), X-ray absorption spectroscopy (XAS), Raman spectroscopy, and secondary ion mass spectrometry (SIMS) are discussed. Our data show that cell capacity fade mainly results from lithium trapping in the solid electrolyte interphase (SEI) of the negative electrode. In addition, cell impedance rise and voltage fade mainly arise at the positive electrode and result from degradation processes in its oxide and carbon constituents. Processes that include the accumulation of transition metal elements at the negative electrode, and increasing misalignment of electrode capacity windows on extended cycling, also have a deleterious effect on cell performance. Identifying sources of performance degradation has enabled strategies to extend cell life, which include improved cell fabrication protocols, positive electrode coatings, and bifunctional electrolyte additives. (C) 2013 The Electrochemical Society. C1 [Li, Y.; Bettge, M.; Polzin, B.; Zhu, Y.; Balasubramanian, M.; Abraham, D. P.] Argonne Natl Lab, Argonne, IL 60439 USA. [Li, Y.] Univ Rochester, Rochester, NY 14627 USA. RP Li, Y (reprint author), Argonne Natl Lab, 9700 S Cass Ave, Argonne, IL 60439 USA. EM abraham@anl.gov RI Li, Yan/H-2957-2012 OI Li, Yan/0000-0002-9801-7243 FU U.S. Department of Energy's Vehicle Technologies Program; DOE Vehicle Technologies Program (VTP) within Applied Battery Research (ABR) for Transportation Program; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]; Argonne, a U.S. Department of Energy Office of Science laboratory [DE-AC02-06CH11357] FX Support from the U.S. Department of Energy's Vehicle Technologies Program, specifically from Peter Faguy and Dave Howell, is gratefully acknowledged. We are grateful to A. Jansen and S. Trask from the U.S. Department of Energy's (DOE) Cell Fabrication Facility (CFF), Argonne. The CFF is fully supported by the DOE Vehicle Technologies Program (VTP) within the core funding of the Applied Battery Research (ABR) for Transportation Program. Use of the Advanced Photon Source (APS), and use of the Center for Nanoscale Materials at Argonne, was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. We are grateful to Matt Suchomel at APS beam dine 11-BM for help with the high-resolution powder diffraction experiments, and to Naba Karan for assistance with the X-ray absorption spectroscopy experiments performed at the APS PNC-XOR bending magnet beam line 20-BM. A part of this work was carried out at the Frederick Seitz Materials Research Laboratory Central Facilities, University of Illinois at Urbana-Champaign (UIUC). We gratefully acknowledge the assistance and valuable discussions with R. Haasch, T, Spila, E. Sammann (UIUC), D. Dees, N. Dietz, J. Bareno, and W. Lu (Argonne). Y. Li is grateful to Prof. James Li at the University of Rochester for support and encouragement during the course of this-work.; 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 52 TC 75 Z9 75 U1 14 U2 138 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 5 BP A3006 EP A3019 DI 10.1149/2.002305jes PG 14 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA 161OI UT WOS:000320202800004 ER PT J AU Takeuchi, KJ Yau, SZ Subramanian, A Marschilok, AC Takeuchi, ES AF Takeuchi, Kenneth J. Yau, Shali Z. Subramanian, Aditya Marschilok, Amy C. Takeuchi, Esther S. TI The Electrochemistry of Silver Hollandite Nanorods, AgxMn8O16: Enhancement of Electrochemical Battery Performance via Dimensional and Compositional Control SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID CRYSTALLITE SIZE CONTROL; MANGANESE OXIDE; MAGNETITE; IONS AB The reflux synthetic approach for silver hollandite, AgxMn8O16, enabled the preparation of pure silver hollandite over a range of silver (x) content, 1.0 <= x <= 1.8. It was demonstrated that the crystallite size increased along with the silver content in the product. This finding led to the ability to synthetically control material properties enabling the systematic exploration. of the electrochemistry of silver hollandite at a variety of crystallite sizes. Results from battery electrochemical testing, including constant current discharge, pulse testing, Galvanostatic Intermittent Titration Type Testing and cycle testing, are reported herein where all tests, demonstrated improved performance of the smaller crystallite materials relative to the larger crystallite materials. Notably, a 5 fold decrease in calculated DC cell resistance and a doubling of the delivered capacity as a result of crystallite size reduction were demonstrated. Overall, these results illustrate an important paradigm in battery electrochemistry, that the electrochemistry of active electrode materials can be positively affected and controlled by variation in crystal size. (C) 2013 The Electrochemical Society. C1 [Takeuchi, Kenneth J.; Marschilok, Amy C.; Takeuchi, Esther S.] SUNY Stony Brook, Dept Chem, Stony Brook, NY 11794 USA. [Yau, Shali Z.] SUNY Buffalo, Dept Chem, Buffalo, NY 14260 USA. [Subramanian, Aditya] SUNY Buffalo, Dept Chem & Biol Engn, Buffalo, NY 14260 USA. [Marschilok, Amy C.; Takeuchi, Esther S.] SUNY Stony Brook, Dept Mat Sci & Engn, Stony Brook, NY 11794 USA. [Takeuchi, Esther S.] Brookhaven Natl Lab, Global & Reg Solut Directorate, Upton, NY 11973 USA. RP Takeuchi, KJ (reprint author), SUNY Stony Brook, Dept Chem, Stony Brook, NY 11794 USA. EM kenneth.takeuchi.1@stonybrook.edu; amy.marschilok@stonybrook.edu; esther.takeuchi@stonybrook.edu RI Takeuchi, Esther/D-1825-2014; Marschilok, Amy/D-1821-2014 FU Department of Energy, Office of Basic Energy Sciences [DE-SC0008512]; National Institutes of Health from the National Heart, Lung, and Blood Institute [1R01HL093044-01A1] FX This work was supported by the Department of Energy, Office of Basic Energy Sciences, under grant DE-SC0008512. Galvanostatic discharge and galvanostatic intermittent titration-type (GITT) testing for possible use as a primary cell was supported by National Institutes of Health under grant 1R01HL093044-01A1 from the National Heart, Lung, and Blood Institute. NR 23 TC 13 Z9 13 U1 4 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 5 BP A3090 EP A3094 DI 10.1149/2.014305jes PG 5 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA 161OI UT WOS:000320202800016 ER PT J AU Wang, DP Belharouak, I Zhou, GW Amine, K AF Wang, Dapeng Belharouak, Ilias Zhou, Guangwen Amine, Khalil TI Synthesis of Lithium and Manganese-Rich Cathode Materials via an Oxalate Co-Precipitation Method SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID SITU X-RAY; ION BATTERIES; SECONDARY BATTERIES; LOCAL-STRUCTURE; ELECTRODES; LINI0.5MN0.5O2; DECOMPOSITION; DIFFRACTION; NICKEL; MN AB The synthesis of Li- and Mn- rich cathode materials with oxalate co-precipitation method was comprehensively investigated. Thermodynamic calculation arid advanced characterizations were conducted to study the effects of reaction pH and precipitation agent on the morphology and composition of the precipitates. It was found that manganese oxalate has a higher solubility compared to nickel oxalate, especially at low reaction pH. In addition, the different capability of Ni2+ and Mn2+ to form transition metal ammonia complexes led to a composition discrepancy in the precipitation. The desired nickel manganese oxalate precursor composition could only be achieved when these factors were considered, and cathode materials synthesized based on this precursor exhibited satisfactory electrochemical performance (about 220 mAh . g(-1) over 70 cycles under C/10 rate). (C) 2013 The Electrochemical Society. C1 [Wang, Dapeng; Belharouak, Ilias; Amine, Khalil] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. [Wang, Dapeng; Zhou, Guangwen] SUNY Binghamton, Binghamton, NY 13902 USA. RP Wang, DP (reprint author), Argonne Natl Lab, Chem Sci & Engn Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM belharouak@anl.gov RI Amine, Khalil/K-9344-2013; OI Belharouak, Ilias/0000-0002-3985-0278 FU U.S. Department of Energy; Freedom CAR; Vehicle Technologies Office; U.S. Department of Energy Office of Science Laboratory by UChicago Argonne, LLC [DE-AC02-06CH11357] FX This research was funded by the U.S. Department of Energy, Freedom CAR, and Vehicle Technologies Office. The electron microscopy was accomplished at the-Electron Microscopy Center for Materials Research at Argonne National Laboratory, a U.S. Department of Energy Office of Science Laboratory operated under Contract No. DE-AC02-06CH11357 by UChicago Argonne, LLC. NR 30 TC 11 Z9 11 U1 3 U2 61 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 5 BP A3108 EP A3112 DI 10.1149/2.016305jes PG 5 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA 161OI UT WOS:000320202800019 ER PT S AU Sun, JG AF Sun, J. G. BE Singh, D Salem, J Halbig, M Mathur, S TI NONDESTRUCTIVE EVALUATION OF THERMAL BARRIER COATINGS BY OPTICAL AND THERMAL IMAGING METHODS SO MECHANICAL PROPERTIES AND PERFORMANCE OF ENGINEERING CERAMICS AND COMPOSITES VII SE Ceramic Engineering and Science Proceedings LA English DT Proceedings Paper CT Mechanical Behavior and Performance of Ceramics and Composites Symposium CY JAN 22-27, 2012 CL Daytona Beach, FL SP Amer Ceram Soc (ACerS), Amer Ceram Soc (ACerS), Engn Ceram Div (ECD) AB Thermal barrier coatings (TBCs) are widely used to improve the performance and extend the life of combustor and gas turbine components. As TBCs become prime reliant, it becomes important to determine their conditions nondestructively to assure the reliability of the components. Nondestructive evaluation (NDE) methods may be used to assess TBC condition for quality control as well as to monitor TBC degradation during service. Several NDE methods were developed for these applications, including laser backscatter, mid-IR reflectance (MIRR), and thermal imaging based on a multilayer analysis method. Both laser backscatter and MIRR are optical imaging methods and have been investigated for TBC health monitoring. The thermal imaging method is new and can measure TBCs thermal properties with high accuracy. Because TBC properties change with life, a model for TBC health monitoring based on the property change is proposed. This paper describes these NDE methods and presents preliminary experimental results related to TBC health monitoring. C1 Argonne Natl Lab, Argonne, IL 60439 USA. RP Sun, JG (reprint author), Argonne Natl Lab, 9700 S Cass Ave, Argonne, IL 60439 USA. NR 15 TC 0 Z9 0 U1 0 U2 3 PU AMER CERAMIC SOC PI WESTERVILLE PA 735 CERAMIC PLACE, WESTERVILLE, OH 43081-8720 USA SN 0196-6219 BN 978-1-118-21746-7; 978-1-118-20588-4 J9 CERAM ENG SCI PROC PY 2013 BP 27 EP 34 PG 8 WC Materials Science, Ceramics SC Materials Science GA BFH88 UT WOS:000319911600004 ER PT J AU Parkes, MV Staiger, CL Perry, JJ Allendorf, MD Greathouse, JA AF Parkes, Marie V. Staiger, Chad L. Perry, John J. Allendorf, Mark D. Greathouse, Jeffery A. TI Screening metal-organic frameworks for selective noble gas adsorption in air: effect of pore size and framework topology SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID UNITED-ATOM DESCRIPTION; ZEOLITIC-IMIDAZOLATE FRAMEWORKS; CANONICAL MONTE-CARLO; HIGH H-2 ADSORPTION; MOLECULAR-ORBITAL METHODS; VAPOR-LIQUID-EQUILIBRIA; TRANSFERABLE POTENTIALS; PHASE-EQUILIBRIA; CU-BTC; METHANE ADSORPTION AB The adsorption of noble gases and nitrogen by sixteen metal-organic frameworks (MOFs) was investigated using grand canonical Monte Carlo simulation. The MOFs were chosen to represent a variety of net topologies, pore dimensions, and metal centers. Three commercially available MOFs (HKUST-1, AlMIL-53, and ZIF-8) and PCN-14 were also included for comparison. Experimental adsorption isotherms, obtained from volumetric and gravimetric methods, were used to compare krypton, argon, and nitrogen uptake with the simulation results. Simulated trends in gas adsorption and predicted selectivities among the commercially available MOFs are in good agreement with experiment. In the low pressure regime, the expected trend of increasing adsorption with increasing noble gas polarizabilty is seen. For each noble gas, low pressure adsorption correlates with several MOF properties, including free volume, topology, and metal center. Additionally, a strong correlation exists between the Henry's constant and the isosteric heat of adsorption for all gases and MOFs considered. Finally, we note that the simulated and experimental gas selectivities demonstrated by this small set of MOFs show improved performance compared to similar values reported for zeolites. C1 [Parkes, Marie V.; Greathouse, Jeffery A.] Sandia Natl Labs, Dept Geochem, Albuquerque, NM 87185 USA. [Staiger, Chad L.] Sandia Natl Labs, Mat Devices & Energy Technol Dept, Albuquerque, NM 87185 USA. [Perry, John J.; Allendorf, Mark D.] Sandia Natl Labs, Energy Nanomat Dept, Livermore, CA 94551 USA. RP Greathouse, JA (reprint author), Sandia Natl Labs, Dept Geochem, POB 5800, Albuquerque, NM 87185 USA. EM jagreat@sandia.gov RI Perry IV, John/C-9155-2011 OI Perry IV, John/0000-0001-9393-5451 FU U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000]; U.S. Department of Energy FX We would like to thank Todd Zeitler for calculating pore-limiting diameters. This work was funded by the U.S. Department of Energy. 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 107 TC 36 Z9 37 U1 10 U2 126 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 23 BP 9093 EP 9106 DI 10.1039/c3cp50774b PG 14 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 148YN UT WOS:000319285000026 PM 23646358 ER PT J AU Nelson, T Fernandez-Alberti, S Roitberg, AE Tretiak, S AF Nelson, Tammie Fernandez-Alberti, Sebastian Roitberg, Adrian E. Tretiak, Sergei TI Conformational disorder in energy transfer: beyond Forster theory SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID PHOTOSYNTHETIC PURPLE BACTERIA; CONJUGATED POLYMERS; TEMPERATURE-DEPENDENCE; EXCITATION TRANSFER; MOLECULAR-DYNAMICS; ANTENNA SYSTEM; MEH-PPV; LH2; FLUORESCENCE; EXCITONS AB Energy transfer in donor-acceptor chromophore pairs, where the absorption of each species is well separated while donor emission and acceptor absorption overlap, can be understood through a Forster resonance energy transfer model. The picture is more complex for organic conjugated polymers, where the total absorption spectrum can be described as a sum of the individual contributions from each subunit (chromophore), whose absorption is not well separated. Although excitations in these systems tend to be well localized, traditional donors and acceptors cannot be defined and energy transfer can occur through various pathways where each subunit (chromophore) is capable of playing either role. In addition, fast torsional motions between individual monomers can break conjugation and lead to reordering of excited state energy levels. Fast torsional fluctuations occur on the same timescale as electronic transitions leading to multiple trivial unavoided crossings between excited states during dynamics. We use the non-adiabatic excited state molecular dynamics (NA-ESMD) approach to simulate energy transfer between two poly-phenylene vinylene (PPV) oligomers composed of 3-rings and 4-rings, respectively, separated by varying distances. The change in the spatial localization of the transient electronic transition density, initially localized on the donors, is used to determine the transfer rate. Our analysis shows that evolution of the intramolecular transition density can be decomposed into contributions from multiple transfer pathways. Here we present a detailed analysis of ensemble dynamics as well as a few representative trajectories which demonstrate the intertwined role of electronic and conformational processes. Our study reveals the complex nature of energy transfer in organic conjugated polymer systems and emphasizes the caution that must be taken in performing such an analysis when a single simple unidirectional pathway is unlikely. C1 [Nelson, Tammie; Tretiak, Sergei] Los Alamos Natl Lab, Div Theoret, Ctr Nonlinear Studies CNLS, Los Alamos, NM 87545 USA. [Nelson, Tammie; Tretiak, Sergei] Los Alamos Natl Lab, Ctr Integrated Nanotechnol CINT, Los Alamos, NM 87545 USA. [Fernandez-Alberti, Sebastian] Univ Nacl Quilmes, Bernal, Argentina. [Roitberg, Adrian E.] Univ Florida, Dept Phys, Quantum Theory Project, Gainesville, FL 32611 USA. [Roitberg, Adrian E.] Univ Florida, Dept Chem, Quantum Theory Project, Gainesville, FL 32611 USA. RP Tretiak, S (reprint author), Los Alamos Natl Lab, Div Theoret, Ctr Nonlinear Studies CNLS, Los Alamos, NM 87545 USA. EM serg@lanl.gov RI Tretiak, Sergei/B-5556-2009; Roitberg, Adrian/A-2378-2009 OI Tretiak, Sergei/0000-0001-5547-3647; FU Los Alamos National Laboratory (LANL); CONICET; UNQ; ANPCyT [PICT-2010-2375]; NSF [CHE-0239120, CHE-0808910]; National Nuclear Security Administration of the U.S. Department of Energy [DE-AC52-06NA25396]; Center for Integrated Nanotechnology (CINT); Center for Nonlinear Studies (CNLS) FX We acknowledge support of Directed Research and Development Fund at Los Alamos National Laboratory (LANL). A. E. R. and S. F.-A. acknowledge support of CONICET, UNQ, ANPCyT (PICT-2010-2375), NSF Grants CHE-0239120 and CHE-0808910. Los Alamos National Laboratory 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. We acknowledge support of Center for Integrated Nanotechnology (CINT) and Center for Nonlinear Studies (CNLS). NR 69 TC 9 Z9 9 U1 3 U2 50 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 23 BP 9245 EP 9256 DI 10.1039/c3cp50857a PG 12 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 148YN UT WOS:000319285000044 PM 23657784 ER PT J AU Hensel-Bielowka, S Sangoro, JR Wojnarowska, Z Hawelek, L Paluch, M AF Hensel-Bielowka, S. Sangoro, J. R. Wojnarowska, Z. Hawelek, L. Paluch, M. TI The behavior and origin of the excess wing in DEET (N,N-diethyl-3-methylbenzamide) SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID GLASS-FORMING LIQUIDS; SECONDARY RELAXATION; ALPHA-RELAXATION; DIELECTRIC-SPECTROSCOPY; INTERACTING ARRAYS; BETA-RELAXATION; PRESSURE; DYNAMICS; FORMERS; TEMPERATURE AB Broadband dielectric spectroscopy along with a high pressure technique and quantum-mechanical calculations are employed to study in detail the behavior and to reveal the origin of the excess wing (EW) in neat N,N-diethyl-3-methylbenzamide (DEET). Our analysis of dielectric spectra again corroborates the idea that the EW is a hidden beta-relaxation peak. Moreover, we found that the position frequency of the beta peak corresponds to the position of the primitive relaxation of the Coupling Model. We also studied the possible intramolecular rotations in DEET by means of DFT calculation. On that basis we were able to describe the EW as the JG beta-relaxation and find the possible origin of the gamma-relaxation visible in DEET dielectric spectra at very low temperatures. C1 [Hensel-Bielowka, S.] Univ Silesia, Inst Chem, PL-40006 Katowice, Poland. [Sangoro, J. R.] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37830 USA. [Wojnarowska, Z.; Hawelek, L.; Paluch, M.] Univ Silesia, Inst Phys, PL-40007 Katowice, Poland. [Hawelek, L.] Inst Nonferrous Met, PL-44100 Gliwice, Poland. RP Hensel-Bielowka, S (reprint author), Univ Silesia, Inst Chem, Szkolna 9, PL-40006 Katowice, Poland. EM stella.hensel-bielowka@us.edu.pl RI Sangoro, Joshua/A-6573-2011 OI Sangoro, Joshua/0000-0002-5483-9528 FU National Science Centre within the framework of the Maestro2 project [DEC-2012/04/A/ST3/00337]; FNP START; DOE BES; Alexander von Humboldt FX The authors M. P. and Z.W. are deeply grateful for the financial support from the National Science Centre within the framework of the Maestro2 project (Grant No. DEC-2012/04/A/ST3/00337). Z.W. acknowledges financial assistance from FNP START (2013). JRS acknowledges financial support from the DOE BES and the Alexander von Humboldt for the Feodor-Lynen Research Fellowship. NR 34 TC 3 Z9 3 U1 1 U2 23 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 23 BP 9300 EP 9307 DI 10.1039/c3cp50975c PG 8 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 148YN UT WOS:000319285000051 PM 23660993 ER PT J AU Siahrostami, S Bjorketun, ME Strasser, P Greeley, J Rossmeisl, J AF Siahrostami, Samira Bjorketun, Marten E. Strasser, Peter Greeley, Jeff Rossmeisl, Jan TI Tandem cathode for proton exchange membrane fuel cells SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID OXYGEN REDUCTION REACTION; DENSITY-FUNCTIONAL THEORY; H2O2 ACID-SOLUTIONS; HYDROGEN-PEROXIDE; ELECTROCHEMICAL REDUCTION; GRAPHITE-ELECTRODES; DIOXYGEN REDUCTION; COBALT PORPHYRINS; TRANSITION-METALS; CARBON CATHODE AB The efficiency of proton exchange membrane fuel cells is limited mainly by the oxygen reduction reaction at the cathode. The large cathodic overpotential is caused by correlations between binding energies of reaction intermediates in the reduction of oxygen to water. This work introduces a novel tandem cathode design where the full oxygen reduction, involving four electron-transfer steps, is divided into formation (equilibrium potential 0.70 V) followed by reduction (equilibrium potential 1.76 V) of hydrogen peroxide. The two part reactions contain only two electron-transfer steps and one reaction intermediate each, and they occur on different catalyst surfaces. As a result they can be optimized independently and the fundamental problem associated with the four-electron catalysis is avoided. A combination of density functional theory calculations and published experimental data is used to identify potentially active and selective materials for both catalysts. Co-porphyrin is recommended for the first step, formation of hydrogen peroxide, and three different metal oxides - SrTiO3(100), CaTiO3(100) and WO3(100) - are suggested for the subsequent reduction step. C1 [Siahrostami, Samira; Bjorketun, Marten E.; Rossmeisl, Jan] Tech Univ Denmark, Dept Phys, CAMD, DK-2800 Lyngby, Denmark. [Strasser, Peter] Tech Univ Berlin, Div Chem Engn, Dept Chem, D-16123 Berlin, Germany. [Greeley, Jeff] Argonne Natl Lab, Ctr Nanoscale Mat, Argonne, IL 60439 USA. RP Rossmeisl, J (reprint author), Tech Univ Denmark, Dept Phys, CAMD, DK-2800 Lyngby, Denmark. EM Jan.Rossmeisl@fysik.dtu.dk RI Rossmeisl, Jan/A-5714-2011; Bjorketun, Marten/L-4396-2013; Strasser, Peter/A-1868-2012 OI Rossmeisl, Jan/0000-0001-7749-6567; FU Danish Center for Scientific Computing [HDW-1103-06]; Catalysis for Sustainable Energy initiative; Danish Ministry of Science, Technology and Innovation; Danish Council for Strategic Research's Programme Commission on Strategic Growth-Technologies (NABIIT); center of excellence in catalysis UNICAT; DFG FX The authors acknowledge support from the Danish Center for Scientific Computing through grant HDW-1103-06, from the Catalysis for Sustainable Energy initiative funded by the Danish Ministry of Science, Technology and Innovation, and from the Danish Council for Strategic Research's Programme Commission on Strategic Growth-Technologies (NABIIT). Peter Strasser acknowledges support from the center of excellence in catalysis UNICAT funded by DFG and managed by the TU Berlin. NR 82 TC 8 Z9 8 U1 6 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 23 BP 9326 EP 9334 DI 10.1039/c3cp51479j PG 9 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 148YN UT WOS:000319285000054 PM 23661187 ER PT J AU Ramanathan, M Shrestha, LK Mori, T Ji, QM Hill, JP Ariga, K AF Ramanathan, Muruganathan Shrestha, Lok Kumar Mori, Taizo Ji, Qingmin Hill, Jonathan P. Ariga, Katsuhiko TI Amphiphile nanoarchitectonics: from basic physical chemistry to advanced applications SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID LANGMUIR-BLODGETT BILAYERS; DENSITY-FUNCTIONAL THEORY; LIQUID-LIQUID INTERFACE; ENHANCED OIL-RECOVERY; BLACK FOAM FILMS; BY-LAYER FILMS; HYDROPHOBICALLY ASSOCIATING POLYACRYLAMIDE; MESOPOROUS NANOCOMPARTMENT FILMS; MOLECULAR-DYNAMICS SIMULATIONS; SURFACTANT ADSORPTION-KINETICS AB Amphiphiles, either synthetic or natural, are structurally simple molecules with the unprecedented capacity to self-assemble into complex, hierarchical geometries in nanospace. Effective self-assembly processes of amphiphiles are often used to mimic biological systems, such as assembly of lipids and proteins, which has paved a way for bottom-up nanotechnology with bio-like advanced functions. Recent developments in nanostructure formation combine simple processes of assembly with the more advanced concept of nanoarchitectonics. In this perspective, we summarize research on self-assembly of amphiphilic molecules such as lipids, surfactants or block copolymers that are a focus of interest for many colloid, polymer, and materials scientists and which have become increasingly important in emerging nanotechnology and practical applications, latter of which are often accomplished by amphiphile-like polymers. Because the fundamental science of amphiphiles was initially developed for their solution assembly then transferred to assemblies on surfaces as a development of nanotechnological techniques, this perspective attempts to mirror this development by introducing solution systems and progressing to interfacial systems, which are roughly categorized as (i) basic properties of amphiphiles, (ii) self-assembly of amphiphiles in bulk phases, (iii) assembly on static surfaces, (iv) assembly at dynamic interfaces, and (v) advanced topics from simulation to application. This progression also represents the evolution of amphiphile science and technology from simple assemblies to advanced assemblies to nanoarchitectonics. C1 [Ramanathan, Muruganathan] Oak Ridge Natl Lab, CNMS, Oak Ridge, TN 37831 USA. [Shrestha, Lok Kumar; Mori, Taizo; Ji, Qingmin; Hill, Jonathan P.; Ariga, Katsuhiko] NIMS, WPI, Res Ctr Mat Nanoarchitecton MANA, Tsukuba, Ibaraki 3050044, Japan. [Mori, Taizo; Hill, Jonathan P.; Ariga, Katsuhiko] Japan Sci & Technol Agcy JST, Tsukuba, Ibaraki 3050044, Japan. RP Ramanathan, M (reprint author), Oak Ridge Natl Lab, CNMS, Oak Ridge, TN 37831 USA. EM nmr@ornl.gov; Lokkumar@nims.go.jp; ARIGA.Katsuhiko@nims.go.jp RI ARIGA, Katsuhiko/H-2695-2011; Mori, Taizo/N-9374-2016; Shrestha, Lok Kumar /B-9537-2013; OI Mori, Taizo/0000-0002-6974-5137; Hill, Jonathan/0000-0002-4229-5842 FU Center for Nanophase Materials Sciences; Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy; World Premier International Research Center Initiative (WPI Initiative), MEXT, Japan; Core Research for Evolutional Science and Technology (CREST) program of Japan Science and Technology Agency (JST), Japan FX Partial support from 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 is greatly acknowledged. This work was also partly supported by World Premier International Research Center Initiative (WPI Initiative), MEXT, Japan and the Core Research for Evolutional Science and Technology (CREST) program of Japan Science and Technology Agency (JST), Japan. NR 407 TC 104 Z9 105 U1 22 U2 186 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 26 BP 10580 EP 10611 DI 10.1039/c3cp50620g PG 32 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 163FP UT WOS:000320321600004 PM 23639971 ER PT J AU Mudiyanselage, K An, W Yang, F Liu, P Stacchiola, DJ AF Mudiyanselage, Kumudu An, Wei Yang, Fan Liu, Ping Stacchiola, Dario J. TI Selective molecular adsorption in sub-nanometer cages of a Cu2O surface oxide SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID GAS SHIFT REACTION; ATOMIC-STRUCTURE; CO ADSORPTION; AB-INITIO; CU(111); METHANOL; COPPER; OXIDATION; METALS; NANOPARTICLES AB In this study the identity of diverse adsorption sites on a 5-7 Cu2O/Cu(111) surface oxide structure has been identified. The 5-7 membered rings formed by a topological defect on stoichiometric Cu2O present different electronic structures from the originating hexagonal rings, as shown by combined bias dependent scanning tunneling microscopy (STM) and density functional theory (DFT) calculations. The adsorption of CO as a probe molecule on the 5-7 structure, studied using infrared reflection-absorption spectroscopy (IRRAS), shows the existence of special adsorption sites. By combining experimental and theoretical results, it is determined that CO molecules can be selectively confined inside the 7-membered oxide rings with internal dimensions of similar to 0.85 nm, leading to a marked different adsorbate-substrate interaction than in either clean Cu(111) or Cu2O. The implication of these newly discovered sites on the chemistry of copper for catalytic reactions is discussed. C1 [Mudiyanselage, Kumudu; An, Wei; Yang, Fan; Liu, Ping; Stacchiola, Dario J.] Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA. RP Stacchiola, DJ (reprint author), Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA. EM djs@bnl.gov RI Stacchiola, Dario/B-1918-2009; An, Wei/E-9270-2010; Mudiyanselage, Kumudu/B-2277-2013; YANG, FAN/J-2706-2012 OI Stacchiola, Dario/0000-0001-5494-3205; An, Wei/0000-0002-0760-1357; Mudiyanselage, Kumudu/0000-0002-3539-632X; YANG, FAN/0000-0002-1406-9717 FU US Department of Energy (Chemical Sciences Division) [DE-AC02-98CH10886]; Office of Science of the U.S. DOE [DE-AC02-05CH11231] FX Work carried out at Brookhaven National Laboratory was supported by the US Department of Energy (Chemical Sciences Division, DE-AC02-98CH10886). The DFT calculations were carried out at Center for Functional Nanomaterials at Brookhaven National Laboratory and National Energy Research Scientific Computing (NERSC) Center, which is supported by the Office of Science of the U.S. DOE under Contract No. DE-AC02-05CH11231. NR 41 TC 12 Z9 12 U1 5 U2 81 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 26 BP 10726 EP 10731 DI 10.1039/c3cp50522g PG 6 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 163FP UT WOS:000320321600017 PM 23685717 ER PT J AU Mamontov, E Ohl, M AF Mamontov, E. Ohl, M. TI Slow dynamics of water molecules in an aqueous solution of lithium chloride probed by neutron spin-echo SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID GLASS-FORMING LIQUIDS; LENNARD-JONES MIXTURE; MODE-COUPLING THEORY; DIELECTRIC-RELAXATION; SUPERCOOLED LIQUIDS; SILICA MATRICES; SCATTERING; CROSSOVER; TRANSITION; SPECTROSCOPY AB Aqueous solutions of lithium chloride are uniquely similar to pure water in the parameters such as glass transition temperature, T-g, yet they could be supercooled without freezing down to below 200 K even in the bulk state. This provides advantageous opportunity to study low-temperature dynamics of water molecules in water-like environment in the bulk rather than nano-confined state. Using high-resolution neutron spin-echo data, we argue that the critical temperature, T-c, which is also common between lithium chloride aqueous solutions and pure water, is associated with the split of a secondary relaxation from the main structural relaxation on cooling down. Our results do not allow distinguishing between a well-defined separate secondary relaxation process and the "excess wing" scenario, in which the temperature dependence of the secondary relaxation follows the main relaxation. Importantly, however, in either of these scenarios the secondary relaxation is associated with density-density fluctuations, measurable in a neutron scattering experiment. Neutron scattering could be the only experimental technique with the capability of providing information on the spatial characteristics of the secondary relaxation through the dependence of the signal on the scattering momentum transfer. We propose a simple method for such analysis. C1 [Mamontov, E.] Oak Ridge Natl Lab, Neutron Sci Directorate, Oak Ridge, TN 37831 USA. [Ohl, M.] Oak Ridge Natl Lab, Julich Ctr Neutron Sci, Outstn Spallat Neutron Source, Oak Ridge, TN 37831 USA. RP Mamontov, E (reprint author), Oak Ridge Natl Lab, Neutron Sci Directorate, Oak Ridge, TN 37831 USA. EM mamontove@ornl.gov; m.ohl@fz-juelich.de RI Mamontov, Eugene/Q-1003-2015 OI Mamontov, Eugene/0000-0002-5684-2675 FU Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy (DOE); U.S. DOE [DE-AC05-00OR22725] FX The neutron scattering experiments at Oak Ridge National Laboratory's (ORNL) Spallation Neutron Source were supported by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy (DOE). ORNL is managed by UTBattelle, LLC, for the U.S. DOE under Contract No. DE-AC05-00OR22725. NR 53 TC 5 Z9 5 U1 2 U2 35 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 26 BP 10732 EP 10739 DI 10.1039/c3cp51355f PG 8 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 163FP UT WOS:000320321600018 PM 23689686 ER PT J AU Zador, J Huang, HF Welz, O Zetterberg, J Osborn, DL Taatjes, CA AF Zador, Judit Huang, Haifeng Welz, Oliver Zetterberg, Johan Osborn, David L. Taatjes, Craig A. TI Directly measuring reaction kinetics of (center dot)QOOH - a crucial but elusive intermediate in hydrocarbon autoignition SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID PHOTOIONIZATION MASS-SPECTROMETRY; SET MODEL CHEMISTRY; ALKYL PLUS O-2; ELEMENTARY REACTIONS; PRODUCT FORMATION; UNIMOLECULAR REACTIONS; COMBUSTION CHEMISTRY; MASTER EQUATION; RADICALS; MOLECULES AB Hydrocarbon autoignition has long been an area of intense fundamental chemical interest, and is a key technological process for emerging clean and efficient combustion strategies. Carbon-centered radicals containing an -OOH group, commonly denoted (center dot)QOOH radicals, are produced by isomerization of the alkylperoxy radicals that are formed in the first stages of oxidation. These (center dot)QOOH radicals are among the most critical species for modeling autoignition, as their reactions with O-2 are responsible for chain branching below 1000 K. Despite their importance, no (center dot)QOOH radicals have ever been observed by any means, and only computational and indirect experimental evidence has been available on their reactivity. Here, we directly produce a (center dot)QOOH radical, 2-hydroperoxy-2-methylprop-1-yl, and experimentally determine rate coefficients for its unimolecular decomposition and its association reaction with O-2. The results are supported by high-level theoretical kinetics calculations. Our experimental strategy opens up a new avenue to study the chemistry of (center dot)QOOH radicals in isolation. C1 [Zador, Judit; Huang, Haifeng; Welz, Oliver; Zetterberg, Johan; Osborn, David L.; Taatjes, Craig A.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA. [Zetterberg, Johan] Lund Univ, Dept Phys, SE-22100 Lund, Sweden. RP Zador, J (reprint author), Sandia Natl Labs, Combust Res Facil, Mail Stop 9055, Livermore, CA 94551 USA. EM jzador@sandia.gov; cataatj@sandia.gov RI Zetterberg, Johan/C-6963-2008; Welz, Oliver/C-1165-2013; Zador, Judit/A-7613-2008 OI Zetterberg, Johan/0000-0002-0882-1482; Welz, Oliver/0000-0003-1978-2412; 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]; Lawrence Berkeley National Laboratory [DE-AC02-05CH11231]; U.S. DOE [DE-AC02-05CH11231]; Center for Combustion Science and Technology, CECOST FX This work was supported by the Division of Chemical Sciences, Geosciences, and Biosciences, the Office of Basic Energy Sciences, the U.S. Department of Energy under DOE Contract Number DE-AC04-94AL85000. Sandia is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the National Nuclear Security Administration. The Advanced Light Source is supported by the Director, Office of Science, Office of Basic Energy Sciences, of the U.S. DOE, also under contract DE-AC02-05CH11231 between Lawrence Berkeley National Laboratory and the U.S. DOE. J. Zetterberg was supported by The Center for Combustion Science and Technology, CECOST. J. Zador thanks Dr C. Franklin Goldsmith for providing information on the propyl-QOOH + O2 systems, while O. Welz thanks Dr Wayne Lukens for taking 1H-NMR spectrum of the TBHP sample. NR 41 TC 21 Z9 21 U1 9 U2 98 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 26 BP 10753 EP 10760 DI 10.1039/c3cp51185e PG 8 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 163FP UT WOS:000320321600021 PM 23689671 ER PT J AU Gu, HB Guo, J Wei, HG Huang, YD Zhao, CY Li, Y Wu, QL Haldolaarachchige, N Young, DP Wei, SY Guo, ZH AF Gu, Hongbo Guo, Jiang Wei, Huige Huang, Yudong Zhao, Cunyu Li, Ying Wu, Qingliu Haldolaarachchige, Neel Young, David P. Wei, Suying Guo, Zhanhu TI Giant magnetoresistance in non-magnetic phosphoric acid doped polyaniline silicon nanocomposites with higher magnetic field sensing sensitivity SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID LITHIUM-ION BATTERIES; ELECTRICAL-PROPERTIES; CONJUGATED POLYMERS; OPTICAL-PROPERTIES; CONDUCTING POLYANILINE; NEGATIVE PERMITTIVITY; OXIDE NANOCOMPOSITES; TRANSPORT; COMPOSITE; FILMS AB Phosphoric acid doped conductive polyaniline (PANI) polymer nanocomposites (PNCs) reinforced with silicon nanopowders have been successfully synthesized using a facile surface initiated polymerization (SIP) method. The chemical structures of the nanocomposites are characterized using Fourier transform infrared (FT-IR) spectroscopy. The enhanced thermal stability of the silicon-PANI PNCs compared with pure PANI is obtained using thermogravimetric analysis (TGA). The obtained optical band gap of the PNCs using Ultraviolet-visible diffuse reflectance spectroscopy (UV-vis DRS) decreases with increasing silicon loading. The dielectric properties of the PNCs are strongly related to the silicon loading level. Temperature dependent resistivity analysis reveals a quasi 3-D variable range hopping (VRH) electrical conduction mechanism for the synthesized PNCs. Room temperature giant magnetoresistance (GMR) is observed in the synthesized non-magnetic nanocomposites and analyzed using the wave-function shrinkage model. C1 [Gu, Hongbo; Guo, Jiang; Wei, Huige; Guo, Zhanhu] Lamar Univ, Dan F Smith Dept Chem Engn, ICL, Beaumont, TX 77710 USA. [Gu, Hongbo; Huang, Yudong] Harbin Inst Technol, Sch Chem Engn & Technol, Harbin 150001, Heilongjiang, Peoples R China. [Wei, Huige; Wei, Suying] Lamar Univ, Dept Chem & Biochem, Beaumont, TX 77710 USA. [Zhao, Cunyu; Li, Ying] Univ Wisconsin, Dept Mech Engn, Milwaukee, WI 53211 USA. [Wu, Qingliu] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. [Haldolaarachchige, Neel; Young, David P.] Louisiana State Univ, Dept Phys & Astron, Baton Rouge, LA 70803 USA. RP Wei, SY (reprint author), Lamar Univ, Dept Chem & Biochem, Beaumont, TX 77710 USA. EM suying.wei@lamar.edu; zhanhu.guo@lamar.edu RI wu, qingliu /C-7631-2012; Li, Ying/B-1830-2010; Haldolaarachchige, Neel/E-3773-2010; Wei, Huige/N-2316-2014; Zhao, Cunyu/E-9417-2015; Guo, Jiang /Q-7163-2016; OI Li, Ying/0000-0002-6775-5649; Haldolaarachchige, Neel/0000-0002-4681-4144; Wei, Huige/0000-0002-7046-798X; Guo, Zhanhu/0000-0003-0134-0210 FU Lamar University; National Science Foundation Nanoscale Interdisciplinary Research Team, and Materials Processing and Manufacturing [CMMI 10-30755]; NSF [DMR 10-05764]; China Scholarship Council (CSC) FX This project is supported by the Research Enhancement Grant of Lamar University. The support from the National Science Foundation Nanoscale Interdisciplinary Research Team, and Materials Processing and Manufacturing (CMMI 10-30755) is kindly acknowledged. D. P. Young acknowledges support from the NSF under Grant No. DMR 10-05764. H. Gu acknowledges the support from China Scholarship Council (CSC) program. NR 81 TC 20 Z9 21 U1 2 U2 39 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 26 BP 10866 EP 10875 DI 10.1039/c3cp50698c PG 10 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 163FP UT WOS:000320321600034 PM 23698645 ER PT J AU Baggetto, L Jumas, JC Gorka, J Bridges, CA Veith, GM AF Baggetto, Loic Jumas, Jean-Claude Gorka, Joanna Bridges, Craig A. Veith, Gabriel M. TI Predictions of particle size and lattice diffusion pathway requirements for sodium-ion anodes using eta-Cu6Sn5 thin films as a model system SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID X-RAY-DIFFRACTION; ELECTROCHEMICAL REACTION; LITHIUM BATTERIES; TIN ANODES; ELECTRODES; CU6SN5; LI; ETA'-CU6SN5; CAPACITY; SN AB Geometrically well-defined Cu6Sn5 thin films were used as a model system to estimate the diffusion depth and diffusion pathway requirements of Na ions in alloy anodes. Cu6Sn5 anodes have an initial reversible capacity towards Li of 545 mA h g(-1) (Li3.96Sn or 19.8 Li/Cu6Sn5), close to the theoretical 586 mA h g(-1) (Li4.26Sn), and a very low initial irreversible capacity of 1.6 Li/Cu6Sn5 (Li0.32Sn). In contrast, the reaction with Na is limited with a reversible capacity of 160 mA h g(-1) compared to the expected 516 mA h g(-1) (Na3.75Sn). X-ray diffraction and Sn-119-Mossbauer spectroscopy measurements show that this limited capacity likely results from the restricted diffusion of Na into the anode nanoparticles and not the formation of a low Na-content phase. Moreover, our results suggest that the Z-Cu6Sn5 alloy should have optimized particle sizes of nearly 10 nm diameter to increase the Na capacity significantly. An alternative system consisting of a two-phase mixture of Cu6Sn5 and Sn of nominal composition 'Cu6Sn10' has been studied and is able to deliver a larger initial reversible storage capacity of up to 400 mA h g(-1). Finally, we have demonstrated that the presence of Cu in Cu6Sn5 and 'Cu6Sn10' suppresses the anomalous electrolyte decomposition normally observed for pure Sn. C1 [Baggetto, Loic; Veith, Gabriel M.] Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. [Jumas, Jean-Claude] Univ Montpellier 2, Inst Charles Gerhardt, F-34095 Montpellier 5, France. [Gorka, Joanna; Bridges, Craig A.] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. RP Baggetto, L (reprint author), Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. EM baggettol@ornl.gov; veithgm@ornl.gov RI Baggetto, Loic/D-5542-2017 OI Baggetto, Loic/0000-0002-9029-2363 FU U.S. Department of Energy (DOE), Basic Energy Sciences (BES), Materials Sciences and Engineering Division; ORNL's Shared Research Equipment (ShaRE) User Program (Microscopy); DOE-BES; Region Languedoc-Roussillon (France) FX This work was supported by the U.S. Department of Energy (DOE), Basic Energy Sciences (BES), Materials Sciences and Engineering Division. Research supported by ORNL's Shared Research Equipment (ShaRE) User Program (Microscopy) is sponsored by DOE-BES. JCJ gratefully acknowledges Region Languedoc-Roussillon (France) for the financial support to the "X-rays and gamma-rays platform'' of Universite Montpellier II in relation with Mossbauer spectroscopy experiments. NR 25 TC 23 Z9 24 U1 2 U2 69 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 26 BP 10885 EP 10894 DI 10.1039/c3cp51657a PG 10 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 163FP UT WOS:000320321600036 PM 23698702 ER PT J AU Zhou, XW Jones, RE Duda, JC Hopkins, PE AF Zhou, X. W. Jones, R. E. Duda, J. C. Hopkins, P. E. TI Molecular dynamics studies of material property effects on thermal boundary conductance SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID ELASTIC-CONSTANTS; TRANSPORT; RESISTANCE; SIMULATION; ORDER; CONDUCTIVITY; TEMPERATURE; INTERFACES; ALUMINUM; NITROGEN AB Thermal boundary resistance (inverse of conductance) between different material layers can dominate the overall thermal resistance in nanostructures and therefore impact the performance of the thermal property limiting nano devices. Because relationships between material properties and thermal boundary conductance have not been fully understood, optimum devices cannot be developed through a rational selection of materials. Here we develop generic interatomic potentials to enable material properties to be continuously varied in extremely large molecular dynamics simulations to explore the dependence of thermal boundary conductance on the characteristic properties of materials such as atomic mass, stiffness, and interfacial crystallography. To ensure that our study is not biased to a particular model, we employ different types of interatomic potentials. In particular, both a Stillinger-Weber potential and a hybrid embedded-atom-method + Stillinger-Weber potential are used to study metal-on-semiconductor compound interfaces, and the results are analyzed considering previous work based upon a Lennard-Jones (LJ) potential. These studies, therefore, reliably provide new understanding of interfacial transport phenomena particularly in terms of effects of material properties on thermal boundary conductance. Our most important finding is that thermal boundary conductance increases with the overlap of the vibrational spectra between metal modes and the acoustic modes of the semiconductor compound, and increasing the metal stiffness causes a continuous shift of the metal modes. As a result, the maximum thermal boundary conductance occurs at an intermediate metal stiffness (best matched to the semiconductor stiffness) that maximizes the overlap of the vibrational modes. C1 [Zhou, X. W.; Jones, R. E.] Sandia Natl Labs, Mech Mat Dept, Livermore, CA 94550 USA. [Duda, J. C.; Hopkins, P. E.] Univ Virginia, Dept Mech & Aerosp Engn, Charlottesville, VA 22904 USA. RP Zhou, XW (reprint author), Sandia Natl Labs, Mech Mat Dept, Livermore, CA 94550 USA. EM xzhou@sandia.gov FU U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000]; NSF [CBET 1134311] FX Sandia National Laboratories is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000. This work was performed under a Laboratory Directed Research and Development (LDRD) project. PEH is also appreciative for funding from NSF Grant number CBET 1134311. NR 62 TC 12 Z9 12 U1 2 U2 37 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 26 BP 11078 EP 11087 DI 10.1039/c3cp51131f PG 10 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 163FP UT WOS:000320321600057 PM 23715116 ER PT J AU Carroll, KJ Qian, D Fell, C Calvin, S Veith, GM Chi, MF Baggetto, L Meng, YS AF Carroll, Kyler J. Qian, Danna Fell, Chris Calvin, Scott Veith, Gabriel M. Chi, Miaofang Baggetto, Loic Meng, Ying Shirley TI Probing the electrode/electrolyte interface in the lithium excess layered oxide Li1.2Ni0.2Mn0.6O2 SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID SITU X-RAY; ABSORPTION FINE-STRUCTURE; LI-ION BATTERIES; MULTIPLE-SCATTERING CALCULATIONS; NICKEL MANGANESE OXIDES; CATHODE MATERIALS; SURFACE-CHEMISTRY; HIGH-VOLTAGE; ELECTROCHEMICAL PERFORMANCE; SECONDARY BATTERIES AB A detailed surface investigation of the lithium-excess nickel manganese layered oxide Li1.2Ni0.2Mn0.6O2 structure was carried out using X-ray photoelectron spectroscopy (XPS), total electron yield and transmission X-ray absorption spectroscopy (XAS), and electron energy loss spectroscopy (EELS) during the first two electrochemical cycles. All spectroscopy techniques consistently showed the presence of Mn4+ in the pristine material and a surprising reduction of Mn at the voltage plateau during the first charge. The Mn reduction is accompanied by the oxygen loss revealed using EELS. Upon the first discharge, the Mn at the surface never fully recovers back to Mn4+. The electrode/electrolyte interface of this compound consists of the reduced Mn at the crystalline defect-spinel inner layer and an oxidized Mn species simultaneously with the presence of a superoxide species in the amorphous outer layer. This proposed model signifies that oxygen vacancy formation and lithium removal result in electrolyte decomposition and superoxide formation, leading to Mn activation/dissolution and surface layer-spinel phase transformation. The results also indicate that the role of oxygen is complex and significant in contributing to the extra capacity of this class of high energy density cathode materials. C1 [Carroll, Kyler J.; Qian, Danna; Meng, Ying Shirley] Univ Calif San Diego, Dept NanoEngn, La Jolla, CA 92037 USA. [Fell, Chris] Univ Florida, Dept Mat Sci & Engn, Gainesville, FL 32611 USA. [Calvin, Scott] Sarah Lawrence Coll, Dept Phys, Bronxville, NY 10708 USA. [Veith, Gabriel M.; Chi, Miaofang; Baggetto, Loic] Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN USA. RP Meng, YS (reprint author), Univ Calif San Diego, Dept NanoEngn, La Jolla, CA 92037 USA. EM shirleymeng@ucsd.edu RI Meng, Shirley /I-1276-2013; Qian, Danna/H-6580-2015; Chi, Miaofang/Q-2489-2015; Baggetto, Loic/D-5542-2017 OI Chi, Miaofang/0000-0003-0764-1567; Baggetto, Loic/0000-0002-9029-2363 FU Office of Vehicle Technologies of the U.S. Department of Energy [DE-AC02-05CH11231, 7056412]; U.S. Department of Energy's Office of Basic Energy Science, Division of Materials Sciences and Engineering under UT-Battelle, LLC; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-98CH10886]; Florida Energy System Consortium through University of Florida [80859]; Office of Basic Energy Sciences, U.S. Department of Energy FX YSM, KJC, and DQ acknowledge the support from 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, Subcontract No. 7056412 under the Batteries for Advanced Transportation Technologies (BATT) Program. GMV and LB acknowledge the support from the U.S. Department of Energy's Office of Basic Energy Science, Division of Materials Sciences and Engineering, under contract with UT-Battelle, LLC. KJC and SC acknowledge the use of the National Synchrotron Light Source, Brookhaven National Laboratory, supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under contract no. DE-AC02-98CH10886. CRF acknowledges the financial support from Florida Energy System Consortium through University of Florida under Award Number 80859. We would like to thank Dr Nancy Dudney for invaluable discussions. DQ thanks Dr Huolin Xin for providing the scripts for Mn oxidation state analysis. a-S/TEM and EELS analysis were carried out at the ORNL Shared Research Equipment (SHaRE) User Facility, which is sponsored by the Office of Basic Energy Sciences, U.S. Department of Energy. NR 65 TC 41 Z9 42 U1 6 U2 115 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 26 BP 11128 EP 11138 DI 10.1039/c3cp51927a PG 11 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 163FP UT WOS:000320321600063 PM 23722534 ER PT S AU Emiliani, F Guber, K Kopecky, S Lampoudis, C Massimi, C Schillebeeckx, P Volev, K AF Emiliani, F. Guber, K. Kopecky, S. Lampoudis, C. Massimi, C. Schillebeeckx, P. Volev, K. BE Serot, O DeSaintJean, C Litaize, O Noguere, G TI Evaluation of stable tungsten isotopes in the resolved resonance region SO WONDER-2012 - 3RD INTERNATIONAL WORKSHOP ON NUCLEAR DATA EVALUATION FOR REACTOR APPLICATIONS SE EPJ Web of Conferences LA English DT Proceedings Paper CT 3rd International Workshop on Nuclear Data Evaluation for Reactor Applications (WONDER) CY SEP 25-28, 2012 CL Aix en Provence, FRANCE AB In the last decade benchmark experiments and simulations, together with newly obtained neutron cross section data, have pointed out deficiencies in evaluated data files of W isotopes. The role of W as a fundamental structural material in different nuclear applications fully justifies a new evaluation of W-182,W- 183,W- 184,W- 186 neutron resonance parameters. In this regard transmission and capture cross section measurements on natural and enriched tungsten samples were performed at the GELINA facility of the EC-JRC-IRMM. A resonance parameter file used as input in the resonance shape analysis was prepared based on the available literature and adjusted in first instance to transmission data. C1 [Emiliani, F.; Kopecky, S.; Lampoudis, C.; Schillebeeckx, P.; Volev, K.] European Commiss, Joint Res Ctr, IRMM, Retieseweg 111, B-2440 Geel, Belgium. [Guber, K.] Oak Ridge Natl Lab, Oak Ridge, TN 37381 USA. [Massimi, C.] Univ Bologna, Sezione INFN Bologna, Dept Phys, I-40126 Bologna, Italy. [Volev, K.] Inst Nucl Res & Nucl Energy INRNE, Sofia, Bulgaria. RP Emiliani, F (reprint author), European Commiss, Joint Res Ctr, IRMM, Retieseweg 111, B-2440 Geel, Belgium. RI Massimi, Cristian/B-2401-2015; Massimi, Cristian/K-2008-2015 OI Massimi, Cristian/0000-0001-9792-3722; Massimi, Cristian/0000-0003-2499-5586 FU European Commission through the projects EUFRAT [FP7-211499]; ERINDA [FP7-269499] FX This work was partly supported by the European Commission through the projects EUFRAT (FP7-211499 and ERINDA (FP7-269499). NR 10 TC 0 Z9 0 U1 0 U2 2 PU E D P SCIENCES PI CEDEX A PA 17 AVE DU HOGGAR PARC D ACTIVITES COUTABOEUF BP 112, F-91944 CEDEX A, FRANCE SN 2100-014X BN 978-2-7598-0961-5 J9 EPJ WEB CONF PY 2013 VL 42 AR UNSP 02002 DI 10.1051/epjconf/20134202002 PG 5 WC Nuclear Science & Technology SC Nuclear Science & Technology GA BFM55 UT WOS:000320553300009 ER PT S AU Noguere, G Bouland, O Bernard, D Leconte, P Blaise, P Peneliau, Y Vidal, JF De Saint Jean, C Leal, L Schilleebeeckx, P Kopecky, S Lampoudis, C AF Noguere, G. Bouland, O. Bernard, D. Leconte, P. Blaise, P. Peneliau, Y. Vidal, J. F. De Saint Jean, C. Leal, L. Schilleebeeckx, P. Kopecky, S. Lampoudis, C. BE Serot, O DeSaintJean, C Litaize, O Noguere, G TI Improved MOX fuel calculations using new Pu-239, Am-241 and Pu-240 evaluations SO WONDER-2012 - 3RD INTERNATIONAL WORKSHOP ON NUCLEAR DATA EVALUATION FOR REACTOR APPLICATIONS SE EPJ Web of Conferences LA English DT Proceedings Paper CT 3rd International Workshop on Nuclear Data Evaluation for Reactor Applications (WONDER) CY SEP 25-28, 2012 CL Aix en Provence, FRANCE AB Several studies based on the JEFF-3.1.1 nuclear data library show a systematic overestimation of the critical keff for core configurations of MOX fuel assemblies. The present work investigates possible improvements of the C/E results by using new evaluations for Am-241, Pu-239 and Pu-240. C1 [Noguere, G.; Bouland, O.; Bernard, D.; Leconte, P.; Blaise, P.; Peneliau, Y.; Vidal, J. F.; De Saint Jean, C.] CEA, DEN, Cadarache, F-13108 St Paul Les Durance, France. [Leal, L.] Oak Ridge Natl Lab, Oak Ridge, TN 37381 USA. [Schilleebeeckx, P.; Kopecky, S.; Lampoudis, C.] IRMM, JRC EC, B-2440 Geel, Belgium. RP Noguere, G (reprint author), CEA, DEN, Cadarache, F-13108 St Paul Les Durance, France. RI De Saint Jean, Cyrille/E-8853-2011 NR 0 TC 0 Z9 0 U1 1 U2 4 PU E D P SCIENCES PI CEDEX A PA 17 AVE DU HOGGAR PARC D ACTIVITES COUTABOEUF BP 112, F-91944 CEDEX A, FRANCE SN 2100-014X BN 978-2-7598-0961-5 J9 EPJ WEB CONF PY 2013 VL 42 AR UNSP 05005 DI 10.1051/epjconf/20134205005 PG 5 WC Nuclear Science & Technology SC Nuclear Science & Technology GA BFM55 UT WOS:000320553300023 ER PT S AU Polyanskiy, MN Babzien, M Pogorelsky, I Yakimenko, V AF Polyanskiy, Mikhail N. Babzien, Marcus Pogorelsky, Igor Yakimenko, Vitaly BE Allakhverdiev, KR TI Ultrashort-pulse CO2 lasers: Ready for the race to petawatt? SO XIX INTERNATIONAL SYMPOSIUM ON HIGH-POWER LASER SYSTEMS AND APPLICATIONS 2012 SE Proceedings of SPIE LA English DT Proceedings Paper CT 19th International Symposium on High-Power Laser Systems and Applications (HPLS&A) CY SEP 10-14, 2012 CL Istanbul, TURKEY SP TUBITAK Marmara Arastirma Merkezi, European Off Aerosp Res & Dev (EOARD), OSA, Quantel, Global Analitik, Mateck GmbH, Optomek, EZAN, Laser Syst, Edinburgh Photon, Opt m, Sci Res, Star Alliance, SPIE, AF Off Sci Res, USAF Res Lab DE CO2 laser; ultrashort pulses; terawatt CO2 laser; petawatt lasers ID AMPLIFICATION AB We present an overview of recent progress in ultrahigh-peak-power CO2 laser systems and discuss a roadmap for further development. C1 [Polyanskiy, Mikhail N.; Babzien, Marcus; Pogorelsky, Igor; Yakimenko, Vitaly] Brookhaven Natl Lab, Upton, NY 11973 USA. RP Polyanskiy, MN (reprint author), Brookhaven Natl Lab, Upton, NY 11973 USA. EM polyanskiy@bnl.gov RI Polyanskiy, Mikhail/E-8406-2010 NR 6 TC 1 Z9 1 U1 0 U2 10 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9455-9 J9 PROC SPIE PY 2013 VL 8677 AR UNSP 86770G DI 10.1117/12.2013389 PG 6 WC Optics; Physics, Applied SC Optics; Physics GA BFH40 UT WOS:000319867800016 ER PT S AU Tanaka, T Miyabara, M Saito, K Guo, QX Nishio, M Yu, KM Walukiewicz, W AF Tanaka, Tooru Miyabara, Masaki Saito, Katsuhiko Guo, Qixin Nishio, Mitsuhiro Yu, Kin M. Walukiewicz, Wladek BE Zhu, S Ni, B Ju, DY TI Development of ZnTe-based solar cells SO ADVANCED MATERIALS SCIENCE AND TECHNOLOGY, (IFAMST-8) SE Materials Science Forum LA English DT Proceedings Paper CT 8th International Forum on Advanced Materials Science and Technology (IFAMST-8) CY AUG 01-04, 2012 CL Fukuoka Inst Technol, Fukuoka City, JAPAN SP Saitama Inst Technol, Chinese Mat Res Soc Japan, Chinese Acad & Profess Assoc Japan HO Fukuoka Inst Technol DE ZnTe; homojunction; heterojunction; solar cell ID EFFICIENCY AB ZnTe solar cells with homojunction and heterojunction structures have been developed. Homojunction was fabricated by thermal diffusion of Al into p-ZnTe, and the effect of the diffusion temperature on the photovoltaic (PV) properties was investigated. The highest efficiency was obtained by lowering the diffusion temperature and using p-ZnTe substrate with a low hole concentration. For the heterojunction solar cell, n-ZnO/i-ZnTe/p-ZnTe structure was fabricated, and PV properties were characterized. C1 [Tanaka, Tooru; Miyabara, Masaki; Saito, Katsuhiko; Guo, Qixin; Nishio, Mitsuhiro] Saga Univ, Dept Elect & Elect Engn, Saga 8408502, Japan. [Tanaka, Tooru] Japan Sci & Technol Agcy JST, PRESTO, Saitama 3320012, Japan. [Yu, Kin M.; Walukiewicz, Wladek] Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. RP Tanaka, T (reprint author), Saga Univ, Dept Elect & Elect Engn, Saga 8408502, Japan. EM ttanaka@cc.saga-u.ac.jp OI Tanaka, Tooru/0000-0001-5747-1717; Yu, Kin Man/0000-0003-1350-9642 FU JSPS KAKENHI [24760258]; Nippon Sheet Glass Foundation for Materials Science and Engineering FX This work is partially supported by the JST PRESTO program, JSPS KAKENHI Grant Number 24760258, and Nippon Sheet Glass Foundation for Materials Science and Engineering. NR 11 TC 3 Z9 3 U1 0 U2 8 PU TRANS TECH PUBLICATIONS LTD PI DURNTEN-ZURICH PA KREUZSTRASSE 10, 8635 DURNTEN-ZURICH, SWITZERLAND SN 0255-5476 J9 MATER SCI FORUM PY 2013 VL 750 BP 80 EP + DI 10.4028/www.scientific.net/MSF.750.80 PG 2 WC Materials Science, Multidisciplinary SC Materials Science GA BFD20 UT WOS:000319235900020 ER PT J AU Miliordos, E Ruedenberg, K Xantheas, SS AF Miliordos, Evangelos Ruedenberg, Klaus Xantheas, Sotiris S. TI Unusual Inorganic Biradicals: A Theoretical Analysis SO ANGEWANDTE CHEMIE-INTERNATIONAL EDITION LA English DT Article DE biradical character; Criegee biradicals; ozone; singlet-triplet splitting; unpaired electrons ID POTENTIAL-ENERGY SURFACES; CONFIGURATION-INTERACTION; EXCITED-STATES; BASIS-SETS; TRIMETHYLENEMETHANE; OZONE; ORBITALS; O-3 C1 [Miliordos, Evangelos; Xantheas, Sotiris S.] Pacific NW Natl Lab, Div Phys Sci, Richland, WA 99352 USA. [Ruedenberg, Klaus] Iowa State Univ, Dept Chem, Ames, IA 50011 USA. [Ruedenberg, Klaus] Iowa State Univ, Ames Lab USDOE, Ames, IA 50011 USA. RP Xantheas, SS (reprint author), Pacific NW Natl Lab, Div Phys Sci, 902 Battelle Blvd,POB 999,MS K1-83, Richland, WA 99352 USA. EM sotiris.xantheas@pnnl.gov RI Xantheas, Sotiris/L-1239-2015; OI Xantheas, Sotiris/0000-0002-6303-1037 FU US Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences & Biosciences at Pacific Northwest National Laboratory (PNNL), a multiprogram national laboratory; US Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences & Biosciences at Iowa State University through Ames Laboratory [DE-AC02-07CH11358]; Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231] FX This work was supported by the US Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences & Biosciences at Pacific Northwest National Laboratory (PNNL), a multiprogram national laboratory operated for the DOE by Battelle (for E. M. and S. S. X.) and at Iowa State University under Contract No. DE-AC02-07CH11358 through the Ames Laboratory (for K.R.). This research used resources of the National Energy Research Scientific Computing Center, which is supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. NR 27 TC 20 Z9 20 U1 2 U2 42 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 22 BP 5736 EP 5739 DI 10.1002/anie.201300654 PG 4 WC Chemistry, Multidisciplinary SC Chemistry GA 155IL UT WOS:000319741100008 PM 23606511 ER PT J AU Scarnato, BV Vahidinia, S Richard, DT Kirchstetter, TW AF Scarnato, B. V. Vahidinia, S. Richard, D. T. Kirchstetter, T. W. TI Effects of internal mixing and aggregate morphology on optical properties of black carbon using a discrete dipole approximation model SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID POROUS DUST GRAINS; LIGHT-ABSORPTION; SCATTERING PROPERTIES; AEROSOL PROPERTIES; PLANETARY-ATMOSPHERES; SATELLITE RETRIEVAL; REFLECTED SUNLIGHT; SOOT AEROSOLS; SNOW GRAINS; PARTICLES AB According to recent studies, internal mixing of black carbon (BC) with other aerosol materials in the atmosphere alters its aggregate shape, absorption of solar radiation, and radiative forcing. These mixing state effects are not yet fully understood. In this study, we characterize the morphology and mixing state of bare BC and BC internally mixed with sodium chloride (NaCl) using electron microscopy and examine the sensitivity of optical properties to BC mixing state and aggregate morphology using a discrete dipole approximation model (DDSCAT). DDSCAT is flexible in simulating the geometry and refractive index of particle aggregates. DDSCAT predicts a higher mass absorption coefficient (MAC), lower single scattering albedo (SSA), and higher absorption Angstrom exponent (AAE) for bare BC aggregates that are lacy rather than compact. Predicted values of SSA at 550 nm range between 0.16 and 0.27 for lacy and compact aggregates, respectively, in agreement with reported experimental values of 0.25 +/- 0.05. The variation in absorption with wavelength does not adhere precisely to a power law relationship over the 200 to 1000 nm range. Consequently, AAE values depend on the wavelength region over which they are computed. The MAC of BC (averaged over the 200-1000 nm range) is amplified when internally mixed with NaCl (100-300 nm in radius) by factors ranging from 1.0 for lacy BC aggregates partially immersed in NaCl to 2.2 for compact BC aggregates fully immersed in NaCl. The SSA of BC internally mixed with NaCl is higher than for bare BC and increases with the embedding in the NaCl. Internally mixed BC SSA values decrease in the 200-400 nm wavelength range, a feature also common to the optical properties of dust and organics. Linear polarization features are also predicted in DDSCAT and are dependent on particle size and morphology. This study shows that DDSCAT predicts complex morphology and mixing state dependent aerosol optical properties that have been reported previously and are relevant to radiative transfer, climate modeling, and interpretation of remote sensing measurements. C1 [Scarnato, B. V.; Vahidinia, S.] NASA, Ames Res Ctr, Bay Area Environm Res Inst, Moffett Field, CA 94035 USA. [Vahidinia, S.] NASA, Ames Res Ctr, Oak Ridge Associated Univ, Moffett Field, CA 94035 USA. [Richard, D. T.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. [Kirchstetter, T. W.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. [Kirchstetter, T. W.] Univ Calif Berkeley, Dept Civil & Environm Engn, Berkeley, CA 94720 USA. RP Scarnato, BV (reprint author), USN, Postgrad Sch, Dept Meteorol, Monterey, CA 93943 USA. EM barbara.v.scarnato@nasa.gov FU Radiation Sciences Program in the Earth Science Division of the Science Mission Directorate, National Aeronautical and Space Administration [NNH09AK98I] FX This research was supported by an appointment to the NASA Postdoctoral Program at Ames Research Center, administrated by Oak Ridge Associated Universities through a contract with NASA, and by the Radiation Sciences Program in the Earth Science Division of the Science Mission Directorate, National Aeronautical and Space Administration via award NNH09AK98I. NR 67 TC 35 Z9 35 U1 8 U2 46 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 10 BP 5089 EP 5101 DI 10.5194/acp-13-5089-2013 PG 13 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA 155LK UT WOS:000319749400001 ER PT J AU Naik, V Voulgarakis, A Fiore, AM Horowitz, LW Lamarque, JF Lin, M Prather, MJ Young, PJ Bergmann, D Cameron-Smith, PJ Cionni, I Collins, WJ Dalsoren, SB Doherty, R Eyring, V Faluvegi, G Folberth, GA Josse, B Lee, YH MacKenzie, IA Nagashima, T van Noije, TPC Plummer, DA Righi, M Rumbold, ST Skeie, R Shindell, DT Stevenson, DS Strode, S Sudo, K Szopa, S Zeng, G AF Naik, V. Voulgarakis, A. Fiore, A. M. Horowitz, L. W. Lamarque, J. -F. Lin, M. Prather, M. J. Young, P. J. Bergmann, D. Cameron-Smith, P. J. Cionni, I. Collins, W. J. Dalsoren, S. B. Doherty, R. Eyring, V. Faluvegi, G. Folberth, G. A. Josse, B. Lee, Y. H. MacKenzie, I. A. Nagashima, T. van Noije, T. P. C. Plummer, D. A. Righi, M. Rumbold, S. T. Skeie, R. Shindell, D. T. Stevenson, D. S. Strode, S. Sudo, K. Szopa, S. Zeng, G. TI Preindustrial to present-day changes in tropospheric hydroxyl radical and methane lifetime from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID MEAN OH CONCENTRATION; PAST 2 DECADES; INTERANNUAL VARIABILITY; ICE CORE; ANTHROPOGENIC EMISSIONS; OXIDIZING EFFICIENCY; METHYL CHLOROFORM; CARBON-MONOXIDE; NOX EMISSIONS; OZONE AB We have analysed time-slice simulations from 17 global models, participating in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP), to explore changes in present-day (2000) hydroxyl radical (OH) concentration and methane (CH4) lifetime relative to preindustrial times (1850) and to 1980. A comparison of modeled and observation-derived methane and methyl chloroform lifetimes suggests that the present-day global multi-model mean OH concentration is overestimated by 5 to 10% but is within the range of uncertainties. The models consistently simulate higher OH concentrations in the Northern Hemisphere (NH) compared with the Southern Hemisphere (SH) for the present-day (2000; inter-hemispheric ratios of 1.13 to 1.42), in contrast to observation-based approaches which generally indicate higher OH in the SH although uncertainties are large. Evaluation of simulated carbon monoxide (CO) concentrations, the primary sink for OH, against ground-based and satellite observations suggests low biases in the NH that may contribute to the high north-south OH asymmetry in the models. The models vary widely in their regional distribution of present-day OH concentrations (up to 34 %). Despite large regional changes, the multi-model global mean (mass-weighted) OH concentration changes little over the past 150 yr, due to concurrent increases in factors that enhance OH (humidity, tropospheric ozone, nitrogen oxide (NOx) emissions, and UV radiation due to decreases in stratospheric ozone), compensated by increases in OH sinks (methane abundance, carbon monoxide and non-methane volatile organic carbon (NMVOC) emissions). The large inter-model diversity in the sign and magnitude of preindustrial to present-day OH changes (ranging from a decrease of 12.7% to an increase of 14.6 %) indicate that uncertainty remains in our understanding of the long-term trends in OH and methane lifetime. We show that this diversity is largely explained by the different ratio of the change in global mean tropospheric CO and NOx burdens (Delta CO/Delta NOx, approximately represents changes in OH sinks versus changes in OH sources) in the models, pointing to a need for better constraints on natural precursor emissions and on the chemical mechanisms in the current generation of chemistry-climate models. For the 1980 to 2000 period, we find that climate warming and a slight increase in mean OH (3.5 +/- 2.2 %) leads to a 4.3 +/- 1.9% decrease in the methane lifetime. Analysing sensitivity simulations performed by 10 models, we find that preindustrial to present-day climate change decreased the methane lifetime by about four months, representing a negative feedback on the climate system. Further, we analysed attribution experiments performed by a subset of models relative to 2000 conditions with only one precursor at a time set to 1860 levels. We find that global mean OH increased by 46.4 +/- 12.2% in response to preindustrial to present-day anthropogenic NOx emission increases, and decreased by 17.3 +/- 2.3 %, 7.6 +/- 1.5 %, and 3.1 +/- 3.0% due to methane burden, and anthropogenic CO, and NMVOC emissions increases, respectively. C1 [Naik, V.] UCAR NOAA Geophys Fluid Dynam Lab, Princeton, NJ USA. [Voulgarakis, A.] Univ London Imperial Coll Sci Technol & Med, Dept Phys, London, England. [Fiore, A. M.] Columbia Univ, Dept Earth & Environm Sci, Palisades, NY USA. [Fiore, A. M.] Columbia Univ, Lamont Doherty Earth Observ, Palisades, NY USA. [Horowitz, L. W.; Lin, M.] NOAA Geophys Fluid Dynam Lab, Princeton, NJ USA. [Lamarque, J. -F.] Natl Ctr Atmospher Res, Boulder, CO 80307 USA. [Lin, M.] Princeton Univ, Princeton, NJ 08544 USA. [Prather, M. J.] Univ Calif Irvine, Dept Earth Syst Sci, Irvine, CA USA. [Young, P. J.] Univ Colorado, Cooperat Inst Res Environm Sci, Boulder, CO 80309 USA. [Young, P. J.] NOAA Earth Syst Res Lab, Chem Sci Div, Boulder, CO USA. [Bergmann, D.; Cameron-Smith, P. J.] Lawrence Livermore Natl Lab, Livermore, CA USA. [Cionni, I.] Agenzia Nazl Nuove Tecnol Energia & Sviluppo Econ, Bologna, Italy. [Collins, W. J.; Folberth, G. A.; Rumbold, S. T.] Hadley Ctr Climate Predict, Met Off, Exeter, Devon, England. [Dalsoren, S. B.; Skeie, R.] CICERO, Oslo, Norway. [Doherty, R.; MacKenzie, I. A.; Stevenson, D. S.] Univ Edinburgh, Sch Geosci, Edinburgh, Midlothian, Scotland. [Eyring, V.; Righi, M.] Deutsch Zentrum Luft & Raumfahrt, Inst Phys Atmosphare, Oberpfaffenhofen, Germany. [Faluvegi, G.; Lee, Y. H.; Shindell, D. T.] NASA, Goddard Inst Space Studies, New York, NY 10025 USA. [Josse, B.] CNRS, GAME CNRM, Meteofrance, Ctr Natl Rech Meteorol, Toulouse, France. [Nagashima, T.] Natl Inst Environm Studies, Tsukuba, Ibaraki, Japan. [van Noije, T. P. C.] Royal Netherlands Meteorol Inst, NL-3730 AE De Bilt, Netherlands. [Plummer, D. A.] Environm Canada, Canadian Ctr Climate Modeling & Anal, Victoria, BC, Canada. [Strode, S.] NASA, Goddard Space Flight Ctr, Greenbelt, MD 20771 USA. [Strode, S.] Univ Space Res Assoc, Columbia, MD USA. [Sudo, K.] Nagoya Univ, Dept Earth & Environm Sci, Grad Sch Environm Studies, Nagoya, Aichi 4648601, Japan. [Szopa, S.] LSCE CEA CNRS UVSQ IPSL, Lab Sci Climat & Environm, Paris, France. [Zeng, G.] Natl Inst Water & Atmospher Res, Lauder, New Zealand. RP Naik, V (reprint author), UCAR NOAA Geophys Fluid Dynam Lab, Princeton, NJ USA. EM vaishali.naik@noaa.gov RI Lin, Meiyun/D-6107-2013; Horowitz, Larry/D-8048-2014; Bergmann, Daniel/F-9801-2011; Naik, Vaishali/A-4938-2013; Strode, Sarah/H-2248-2012; Lamarque, Jean-Francois/L-2313-2014; Cameron-Smith, Philip/E-2468-2011; Young, Paul/E-8739-2010; Collins, William/A-5895-2010; Stevenson, David/C-8089-2012; Righi, Mattia/I-5120-2013; Szopa, Sophie/F-8984-2010; Shindell, Drew/D-4636-2012; Skeie, Ragnhild/K-1173-2015; Eyring, Veronika/O-9999-2016; Lee, Yunha/Q-7222-2016; Manager, CSD Publications/B-2789-2015; OI Lin, Meiyun/0000-0003-3852-3491; Horowitz, Larry/0000-0002-5886-3314; Bergmann, Daniel/0000-0003-4357-6301; Naik, Vaishali/0000-0002-2254-1700; Strode, Sarah/0000-0002-8103-1663; Lamarque, Jean-Francois/0000-0002-4225-5074; Cameron-Smith, Philip/0000-0002-8802-8627; Young, Paul/0000-0002-5608-8887; Collins, William/0000-0002-7419-0850; Stevenson, David/0000-0002-4745-5673; Szopa, Sophie/0000-0002-8641-1737; Skeie, Ragnhild/0000-0003-1246-4446; Eyring, Veronika/0000-0002-6887-4885; Lee, Yunha/0000-0001-7478-2672; Folberth, Gerd/0000-0002-1075-440X; Righi, Mattia/0000-0003-3827-5950 FU Atmospheric Chemistry and Climate (AC&C), a project of International Global Atmospheric Chemistry (IGAC) and Stratospheric Processes And their Role in Climate (SPARC) under the International Geosphere-Biosphere Project (IGBP); World Climate Research Program (WCRP); US Dept. of Energy (BER); LLNL [DE-AC52-07NA27344]; NERSC [DE-AC02-05CH11231]; Norwegian Research Council; ENEA; DLR Earth System Model Validation (ESMVal); NASA; NASA MAP program; NASA ACMAP program; DECC [GA01101]; Defra [GA01101]; Environment Research and Technology Development Fund (S-7) of the Ministry of the Environment, Japan [S-7]; National Science Foundation; Office of Science (BER) of the US Department of Energy; Office of Science and Technology through EPSRC's High End Computing Programme FX ACCMIP is organized under the auspices of Atmospheric Chemistry and Climate (AC&C), a project of International Global Atmospheric Chemistry (IGAC) and Stratospheric Processes And their Role in Climate (SPARC) under the International Geosphere-Biosphere Project (IGBP) and World Climate Research Program (WCRP). The authors are grateful to the British Atmospheric Data Centre (BADC), which is part of the NERC National Centre for Atmospheric Science (NCAS), for collecting and archiving the ACCMIP data.; For CESM-CAM-superfast, DB and PC were funded by the US Dept. of Energy (BER), performed under the auspices of LLNL under Contract DE-AC52-07NA27344, and used the supercomputing resources of NERSC under contract No. DE-AC02-05CH11231.; The CICERO-OSloCTM2 simulations were done within the projects SLAC (Short Lived Atmospheric Components) and Earth-Clim funded by the Norwegian Research Council.; For EMAC, the work of VE and MR was funded by the DLR Earth System Model Validation (ESMVal) project and used the supercomputing resources of the German Climate Computing Center (DKRZ) and the Leibniz Supercomputing Centre (LRZ), and the work of IC was funded by the ENEA National Integrated Model to support the international negotiation on atmospheric pollution (Minni) project.; The GEOSCCM work was supported by the NASA Modeling, Analysis and Prediction program, with computing resources provided by NASA's High-End Computing Program through the NASA Advanced Supercomputing Division.; AV, DTS and YHL acknowledge support from the NASA MAP and ACMAP programs.; For HadGEM2, WJC, GAF, and STR were supported by the Joint DECC and Defra Integrated Climate Programme (GA01101).; The MIROC-CHEM calculations were performed on the NIES supercomputer system (NEC SX-8R), and supported by the Environment Research and Technology Development Fund (S-7) of the Ministry of the Environment, Japan.; The CESM project, including NCAR-CAM3.5, is supported by the National Science Foundation and the Office of Science (BER) of the US Department of Energy. The National Center for Atmospheric Research is operated by the University Corporation for Atmospheric Research under sponsorship of the National Science Foundation.; The STOC-HadAM3 work made use of the facilities of HECToR, the UK's national high-performance computing service which is funded by the Office of Science and Technology through EPSRC's High End Computing Programme. NR 107 TC 81 Z9 82 U1 5 U2 90 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 10 BP 5277 EP 5298 DI 10.5194/acp-13-5277-2013 PG 22 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA 155LK UT WOS:000319749400014 ER PT J AU Liu, S Wei, Y Post, WM Cook, RB Schaefer, K Thornton, MM AF Liu, S. Wei, Y. Post, W. M. Cook, R. B. Schaefer, K. Thornton, M. M. TI The Unified North American Soil Map and its implication on the soil organic carbon stock in North America SO BIOGEOSCIENCES LA English DT Article ID GENERAL-CIRCULATION MODELS; CONTIGUOUS UNITED-STATES; BIOSPHERE MODEL; MOJAVE DESERT; DATA SET; VEGETATION; DYNAMICS; CLIMATE; ALASKA; STORAGE AB The Unified North American Soil Map (UNASM) was developed to provide more accurate regional soil information for terrestrial biosphere modeling. The UNASM combines information from state-of-the-art US STATSGO2 and Soil Landscape of Canada (SLCs) databases. The area not covered by these datasets is filled by using the Harmonized World Soil Database version 1.21 (HWSD1.21). The UNASM contains maximum soil depth derived from the data source as well as seven soil attributes (including sand, silt, and clay content, gravel content, organic carbon content, pH, and bulk density) for the topsoil layer (0-30 cm) and the subsoil layer (30-100 cm), respectively, of the spatial resolution of 0.25 degrees in latitude and longitude. There are pronounced differences in the spatial distributions of soil properties and soil organic carbon between UNASM and HWSD, but the UNASM overall provides more detailed and higher-quality information particularly in Alaska and central Canada. To provide more accurate and up-to-date estimate of soil organic carbon stock in North America, we incorporated Northern Circumpolar Soil Carbon Database (NCSCD) into the UNASM. The estimate of total soil organic carbon mass in the upper 100 cm soil profile based on the improved UNASM is 365.96 Pg, of which 23.1% is under trees, 14.1% is in shrubland, and 4.6% is in grassland and cropland. This UNASM data will provide a resource for use in terrestrial ecosystem modeling both for input of soil characteristics and for benchmarking model output. C1 [Liu, S.; Wei, Y.; Post, W. M.; Cook, R. B.; Thornton, M. M.] Oak Ridge Natl Lab, Climate Change Sci Inst, Oak Ridge, TN 37831 USA. [Schaefer, K.] Univ Colorado, Natl Snow & Ice Data Ctr, Boulder, CO 80309 USA. RP Liu, S (reprint author), Huazhong Agr Univ, Coll Resources & Environm, Wuhan 430070, Hubei, Peoples R China. EM carol.shishi@gmail.com RI Cook, Robert/I-1395-2013; Wei, Yaxing/K-1507-2013; Liu, Shuyan/M-8813-2014; OI Wei, Yaxing/0000-0001-6924-0078; Cook, Robert/0000-0001-7393-7302 FU NASA's Terrestrial Ecology Program (TEP) for the Modeling and Synthesis Thematic Data Center (MAST-DC) [09-TE09-26]; NASA TEP FX The authors would like to acknowledge the financial support from the NASA's Terrestrial Ecology Program (TEP) for the Modeling and Synthesis Thematic Data Center (MAST-DC: project 09-TE09-26). We would like to thank the core group from the NASA TEP-funded Multi-scale Synthesis and Terrestrial Model Intercomparison Project (MsTMIP) for providing helpful suggestions to this study. This study was part of the North American Carbon Program. NR 63 TC 12 Z9 12 U1 3 U2 26 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1726-4170 J9 BIOGEOSCIENCES JI Biogeosciences PY 2013 VL 10 IS 5 BP 2915 EP 2930 DI 10.5194/bg-10-2915-2013 PG 16 WC Ecology; Geosciences, Multidisciplinary SC Environmental Sciences & Ecology; Geology GA 156QT UT WOS:000319838200007 ER PT J AU Bowles, FL Olmstead, MM Beavers, CM Balch, AL AF Bowles, Faye L. Olmstead, Marilyn M. Beavers, Christine M. Balch, Alan L. TI Reshaping molecules through cocrystallization. Comparison of the structures of Hg{Co(CO)(4)}(2) and Hg{Co(CO)(4)}(2)center dot C-60 center dot toluene SO CHEMICAL COMMUNICATIONS LA English DT Article ID SOLUBLE ENDOHEDRAL FULLERENES; DICOBALT OCTACARBONYL; METAL-CARBONYL; CRYSTALLOGRAPHIC CHARACTERIZATION; CRYSTAL-STRUCTURE; TRANSITION; DISORDER; C-60 AB Cocrystallization of Hg{Co(CO)(4)}(2) with C-60 produces Hg{Co(CO)(4)}(2)center dot C-60 center dot toluene in which the geometry of the Hg{Co(CO)(4)}(2) molecule is rearranged to fit between the remarkably well ordered fullerenes. C1 [Bowles, Faye L.; Olmstead, Marilyn M.; Balch, Alan L.] Univ Calif Davis, Dept Chem, Davis, CA 95616 USA. [Beavers, Christine M.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Balch, AL (reprint author), Univ Calif Davis, Dept Chem, 1 Shields Ave, Davis, CA 95616 USA. EM albalch@ucdavis.edu RI Beavers, Christine/C-3539-2009 OI Beavers, Christine/0000-0001-8653-5513 FU NSF [CHE-1011760]; ALS; Advanced Light Source; Lawrence Berkeley Laboratory; Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231] FX Financial support from the NSF [Grant CHE-1011760 to ALB and MMO] and the ALS for a predoctoral fellowship for F.L.B. is gratefully acknowledged. We also thank the Advanced Light Source, Lawrence Berkeley Laboratory and Dr. Simon Teat, for support. The Advanced Light Source is supported by the Director, Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. NR 27 TC 1 Z9 1 U1 1 U2 5 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 53 BP 5921 EP 5923 DI 10.1039/c3cc41773e PG 3 WC Chemistry, Multidisciplinary SC Chemistry GA 158QP UT WOS:000319987600003 PM 23648829 ER PT J AU Brown, JW Henderson, BL Kiesz, MD Whalley, AC Morris, W Grunder, S Deng, HX Furukawa, H Zink, JI Stoddart, JF Yaghi, OM AF Brown, Jonathan W. Henderson, Bryana L. Kiesz, Matthew D. Whalley, Adam C. Morris, William Grunder, Sergio Deng, Hexiang Furukawa, Hiroyasu Zink, Jeffrey I. Stoddart, J. Fraser Yaghi, Omar M. TI Photophysical pore control in an azobenzene-containing metal-organic framework SO CHEMICAL SCIENCE LA English DT Article ID DRUG-DELIVERY; MESOSTRUCTURED SILICA; MOLECULAR MACHINES; HYDROGEN STORAGE; POLYMER-FILMS; PHOTOISOMERIZATION; PHOTOCHEMISTRY; NANOPARTICLES; CATALYSIS; RELEASE AB The synthesis and structure of an azobenzene functionalized isoreticular metal-organic framework (azo-IRMOF-74-III) [Mg-2(C26H16O6N2)] are described and the ability to controllably release a guest from its pores in response to an external stimulus has been demonstrated. Azo-IRMOF-74-III is an isoreticular expansion of MOF-74 with an etb topology and a 1-D hexagonal pore structure. The structure of azo-IRMOF-74-III is analogous to that of MOF-74, as demonstrated by powder X-ray diffraction, with a surface area of 2410 m(2) g(-1) BET. Each organic unit within azo-IRMOF-74-III is decorated with a photoswitchable azobenzene unit, which can be toggled between its cis and trans conformation by excitation at 408 nm. When propidium iodide dye was loaded into the MOF, spectroscopic studies showed that no release of the luminescent dye was observed under ambient conditions. Upon irradiation of the MOF at 408 nm, however, the rapid wagging motion inherent to the repetitive isomerization of the azobenzene functionality triggered the release of the dye from the pores. This light-induced release of cargo can be modulated between an on and an off state by controlling the conformation of the azobenzene with the appropriate wavelength of light. This report highlights the ability to capture and release small molecules and demonstrates the utility of self-contained photoactive switches located inside highly porous MOFs. C1 [Brown, Jonathan W.; Morris, William; Deng, Hexiang; Furukawa, Hiroyasu; Yaghi, Omar M.] Univ Calif Los Angeles, Ctr Reticular Chem, Ctr Global Mentoring, Dept Chem & Biochem, Los Angeles, CA 90095 USA. [Henderson, Bryana L.; Kiesz, Matthew D.; Zink, Jeffrey I.] Univ Calif Los Angeles, Dept Chem & Biochem, Los Angeles, CA 90095 USA. [Whalley, Adam C.; Grunder, Sergio; Stoddart, J. Fraser] Northwestern Univ, Ctr Chem Integrated Syst, Evanston, IL 60208 USA. [Whalley, Adam C.; Grunder, Sergio; Stoddart, J. Fraser] Northwestern Univ, Dept Chem, Evanston, IL 60208 USA. [Yaghi, Omar M.] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Yaghi, Omar M.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mol Foundry, Div Mat Sci, Berkeley, CA 94720 USA. RP Brown, JW (reprint author), Univ Calif Los Angeles, Ctr Reticular Chem, Ctr Global Mentoring, Dept Chem & Biochem, Los Angeles, CA 90095 USA. EM jbrown@chem.ucla.edu; yaghi@berkeley.edu RI Stoddart, James /H-1518-2011; Furukawa, Hiroyasu/C-5910-2008; OI Furukawa, Hiroyasu/0000-0002-6082-1738; Yaghi, Omar/0000-0002-5611-3325 FU DTRA/US Army Research Office [W911NF-07-1-0533] FX This work was supported by DTRA/US Army Research Office (Grant W911NF-07-1-0533). NR 44 TC 75 Z9 75 U1 43 U2 310 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 7 BP 2858 EP 2864 DI 10.1039/c3sc21659d PG 7 WC Chemistry, Multidisciplinary SC Chemistry GA 158AH UT WOS:000319940400018 ER PT J AU Wei, D Hossain, T Garces, NY Nepal, N Meyer, HM Kirkham, MJ Eddy, CR Edgar, JH AF Wei, D. Hossain, T. Garces, N. Y. Nepal, N. Meyer, H. M., III Kirkham, M. J. Eddy, C. R., Jr. Edgar, J. H. TI Influence of Atomic Layer Deposition Temperatures on TiO2/n-Si MOS Capacitor SO ECS JOURNAL OF SOLID STATE SCIENCE AND TECHNOLOGY LA English DT Article ID TIO2 FILMS; INTERFACE; GROWTH; SI AB This paper reports on the influence of deposition temperature on the structure, composition, and electrical properties of TiO2 thin films deposited on n-type silicon (100) by plasma-assisted atomic layer deposition (PA-ALD). TiO2 layers similar to 20 nm thick, deposited at temperatures ranging from 100 to 300 degrees C, were investigated. Samples deposited at 200 degrees C and 250 degrees C had the most uniform coverage as determined by atomic force microscopy. The average carbon concentration throughout the oxide layer and at the TiO2/Si interface was lowest at 200 degrees C. Metal oxide semiconductor capacitors (MOSCAPs) were fabricated, and profiled by capacitance-voltage techniques. The sample prepared at 200 degrees C had negligible hysteresis (from a capacitance-voltage plot) and the lowest interface trap density (as extracted using the conductance method). Current-voltage measurements were carried out with top-to-bottom structures. At -2 V gate bias voltage, the smallest leakage current was 1.22 x 10(-5) A/cm(2) for the 100 degrees C deposited sample. (C) 2013 The Electrochemical Society. C1 [Wei, D.; Hossain, T.; Edgar, J. H.] Kansas State Univ, Dept Chem Engn, Manhattan, KS 66506 USA. [Garces, N. Y.; Nepal, N.; Eddy, C. R., Jr.] USN, Elect Sci & Technol Div, Res Lab, Washington, DC 20375 USA. [Meyer, H. M., III; Kirkham, M. J.] Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN 37831 USA. RP Wei, D (reprint author), Kansas State Univ, Dept Chem Engn, Durland Hall, Manhattan, KS 66506 USA. EM edgarjh@ksu.edu RI Kirkham, Melanie/B-6147-2011 OI Kirkham, Melanie/0000-0001-8411-9751 FU Office of Naval Research [N00014-09-1-1160]; U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Program; Office of Naval Research FX We are grateful for the support for this project from the Office of Naval Research, grant N00014-09-1-1160, Paul Maki, program manager. XPS and XRD were conducted through the Oak Ridge National Laboratory's High Temperature Materials Laboratory User Program, sponsored by the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Program. Work at the U.S. Naval Research Laboratory is supported by the Office of Naval Research. NR 29 TC 11 Z9 11 U1 1 U2 21 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 2162-8769 J9 ECS J SOLID STATE SC JI ECS J. Solid State Sci. Technol. PY 2013 VL 2 IS 5 BP N110 EP N114 DI 10.1149/2.010305jss PG 5 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA 151KA UT WOS:000319458200004 ER PT J AU Zhou, YJ Gao, HY Mihindukulasuriya, KA La Rosa, PS Wylie, KM Vishnivetskaya, T Podar, M Warner, B Tarr, PI Nelson, DE Fortenberry, JD Holland, MJ Burr, SE Shannon, WD Sodergren, E Weinstock, GM AF Zhou, Yanjiao Gao, Hongyu Mihindukulasuriya, Kathie A. La Rosa, Patricio S. Wylie, Kristine M. Vishnivetskaya, Tatiana Podar, Mircea Warner, Barb Tarr, Phillip I. Nelson, David E. Fortenberry, J. Dennis Holland, Martin J. Burr, Sarah E. Shannon, William D. Sodergren, Erica Weinstock, George M. TI Biogeography of the ecosystems of the healthy human body SO GENOME BIOLOGY LA English DT Article DE Biogeography; Human microbiome; Biodiversity; Temporal stability ID HUMAN ORAL MICROBIOME; RARE BIOSPHERE; RIBOSOMAL-RNA; DIVERSITY; GUT; BACTERIA; COMMUNITIES; DISEASE; CHILDREN; PROJECT AB Background: Characterizing the biogeography of the microbiome of healthy humans is essential for understanding microbial associated diseases. Previous studies mainly focused on a single body habitat from a limited set of subjects. Here, we analyzed one of the largest microbiome datasets to date and generated a biogeographical map that annotates the biodiversity, spatial relationships, and temporal stability of 22 habitats from 279 healthy humans. Results: We identified 929 genera from more than 24 million 16S rRNA gene sequences of 22 habitats, and we provide a baseline of inter-subject variation for healthy adults. The oral habitat has the most stable microbiota with the highest alpha diversity, while the skin and vaginal microbiota are less stable and show lower alpha diversity. The level of biodiversity in one habitat is independent of the biodiversity of other habitats in the same individual. The abundances of a given genus at a body site in which it dominates do not correlate with the abundances at body sites where it is not dominant. Additionally, we observed the human microbiota exhibit both cosmopolitan and endemic features. Finally, comparing datasets of different projects revealed a project-based clustering pattern, emphasizing the significance of standardization of metagenomic studies. Conclusions: The data presented here extend the definition of the human microbiome by providing a more complete and accurate picture of human microbiome biogeography, addressing questions best answered by a large dataset of subjects and body sites that are deeply sampled by sequencing. C1 [Zhou, Yanjiao; Gao, Hongyu; Mihindukulasuriya, Kathie A.; Wylie, Kristine M.; Sodergren, Erica; Weinstock, George M.] Washington Univ, Sch Med, Genome Inst, St Louis, MO 63108 USA. [La Rosa, Patricio S.; Shannon, William D.] Washington Univ, Sch Med, Div Gen Med Sci, Dept Med, St Louis, MO 63110 USA. [Vishnivetskaya, Tatiana] Univ Tennessee, Knoxville, TN 37916 USA. [Nelson, David E.; Fortenberry, J. Dennis] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. [Warner, Barb] Washington Univ, Sch Med, Div Newborn Med, Dept Pediat, St Louis, MO 63110 USA. [Tarr, Phillip I.] Washington Univ, Sch Med, Div Pediat Gastroenterol, Dept Pediat, St Louis, MO 63110 USA. [Nelson, David E.] Indiana Univ, Dept Biol, Bloomington, IN 47405 USA. [Fortenberry, J. Dennis] Indiana Univ Sch Med, Dept Pediat, Sect Adolescent Med, Indianapolis, IN 46202 USA. [Holland, Martin J.; Burr, Sarah E.] Univ London London Sch Hyg & Trop Med, London WC1E 7HT, England. [Burr, Sarah E.] MRC Unit, Gambia 1000, Fajara, Gambia. RP Weinstock, GM (reprint author), Washington Univ, Sch Med, Genome Inst, St Louis, MO 63108 USA. EM gweinsto@genome.wustl.edu OI Vishnivetskaya, Tatiana/0000-0002-0660-023X; Podar, Mircea/0000-0003-2776-0205; Mihindukulasuriya, Kathie/0000-0001-9372-3758 FU National Institutes of Health [U54HG004968]; NIH-NHGRI [1R01HG004857]; Oak Ridge National Laboratory; Wellcome Trust [079246/Z/06/Z]; NIH [UH3 AI083265, 5P30 DK052574, UH3 AI094641] FX The authors are grateful to the NIH Common Fund Human Microbiome Project Consortium for generating and making available many of the datasets used in this study. The research leading to these results received funding from the National Institutes of Health, grant U54HG004968 to George Weinstock, The Genome Institute at Washington University. Tatiana Vishnivetskaya and Mircea Podar were supported by NIH-NHGRI grant 1R01HG004857 and by the Oak Ridge National Laboratory (managed by UT-Battelle, LLC, for the U.S. Department of Energy). Martin J. Holland was supported by the Wellcome Trust Grant 079246/Z/06/Z. Phillip I. Tarr was supported by NIH grants UH3 AI083265 and 5P30 DK052574 (Biobank) for the Digestive Diseases Research Core Center. J. Dennis Fortenberry was supported by NIH grant UH3 AI094641. NR 53 TC 35 Z9 37 U1 3 U2 54 PU BIOMED CENTRAL LTD PI LONDON PA 236 GRAYS INN RD, FLOOR 6, LONDON WC1X 8HL, ENGLAND SN 1465-6906 J9 GENOME BIOL JI Genome Biol. PY 2013 VL 14 IS 1 AR R1 DI 10.1186/gb-2013-14-1-r1 PG 18 WC Biotechnology & Applied Microbiology; Genetics & Heredity SC Biotechnology & Applied Microbiology; Genetics & Heredity GA 160YA UT WOS:000320155200001 PM 23316946 ER PT J AU Mernild, SH Yde, JC Malmros, JK Knudsen, NT AF Mernild, Sebastian H. Yde, Jacob C. Malmros, Jeppe K. Knudsen, Niels Tvis TI Land-terminating glacier volume changes in different Circum-Arctic areas, mid-1980s to late-2000s/2011 SO GEOGRAFISK TIDSSKRIFT-DANISH JOURNAL OF GEOGRAPHY LA English DT Article ID MITTIVAKKAT-GLETSCHER; SOUTHEAST GREENLAND; MASS-BALANCE; FUTURE C1 [Mernild, Sebastian H.; Malmros, Jeppe K.] Ctr Estudios Cient, Glaciol & Climate Change Lab, Ctr Sci Studies, Valdivia, Chile. [Mernild, Sebastian H.] Los Alamos Natl Lab, Climate Ocean & Sea Ice Modeling Grp, Los Alamos, NM USA. [Yde, Jacob C.] Sogn Fjordane Univ Coll, Fac Sci & Technol, Sogndal, Norway. [Knudsen, Niels Tvis] Aarhus Univ, Dept Geosci, Aarhus, Denmark. RP Mernild, SH (reprint author), Ctr Estudios Cient, Glaciol & Climate Change Lab, Ctr Sci Studies, Valdivia, Chile. EM mernild@cecs.cl RI Knudsen, Niels Tvis/A-2461-2014; OI Yde, Jacob Clement/0000-0002-6211-2601 NR 27 TC 3 Z9 3 U1 1 U2 3 PU ROYAL DANISH GEOGRAPHICAL SOC PI COPENHAGEN K PA OSTER VOLDGADE 10, COPENHAGEN K, DK 1350, DENMARK SN 0016-7223 EI 1903-2471 J9 GEOGR TIDSSKR-DEN JI Geogr. Tidsskr. PY 2013 VL 113 IS 1 BP 65 EP 70 DI 10.1080/00167223.2013.799311 PG 6 WC Environmental Studies; Geography SC Environmental Sciences & Ecology; Geography GA 156KU UT WOS:000319821600006 ER PT J AU Bindschadler, RA Nowicki, S Abe-Ouchi, A Aschwanden, A Choi, H Fastook, J Granzow, G Greve, R Gutowski, G Herzfeld, U Jackson, C Johnson, J Khroulev, C Levermann, A Lipscomb, WH Martin, MA Morlighem, M Parizek, BR Pollard, D Price, SF Ren, DD Saito, F Sato, T Seddik, H Seroussi, H Takahashi, K Walker, R Wang, WL AF Bindschadler, Robert A. Nowicki, Sophie Abe-Ouchi, Ayako Aschwanden, Andy Choi, Hyeungu Fastook, Jim Granzow, Glen Greve, Ralf Gutowski, Gail Herzfeld, Ute Jackson, Charles Johnson, Jesse Khroulev, Constantine Levermann, Anders Lipscomb, William H. Martin, Maria A. Morlighem, Mathieu Parizek, Byron R. Pollard, David Price, Stephen F. Ren, Diandong Saito, Fuyuki Sato, Tatsuru Seddik, Hakime Seroussi, Helene Takahashi, Kunio Walker, Ryan Wang, Wei Li TI Ice-sheet model sensitivities to environmental forcing and their use in projecting future sea level (the SeaRISE project) SO JOURNAL OF GLACIOLOGY LA English DT Article ID DIGITAL ELEVATION MODEL; SATELLITE RADAR; MASS-BALANCE; SURFACE MELT; LASER DATA; PISM-PIK; GREENLAND; ANTARCTICA; SHELF; FLOW AB Ten ice-sheet models are used to study sensitivity of the Greenland and Antarctic ice sheets to prescribed changes of surface mass balance, sub-ice-shelf melting and basal sliding. Results exhibit a large range in projected contributions to sea-level change. In most cases, the ice volume above flotation lost is linearly dependent on the strength of the forcing. Combinations of forcings can be closely approximated by linearly summing the contributions from single forcing experiments, suggesting that nonlinear feedbacks are modest. Our models indicate that Greenland is more sensitive than Antarctica to likely atmospheric changes in temperature and precipitation, while Antarctica is more sensitive to increased ice-shelf basal melting. An experiment approximating the Intergovernmental Panel on Climate Change's RCP8.5 scenario produces additional first-century contributions to sea level of 22.3 and 8.1 cm from Greenland and Antarctica, respectively, with a range among models of 62 and 14 cm, respectively. By 200 years, projections increase to 53.2 and 26.7 cm, respectively, with ranges of 79 and 43 cm. Linear interpolation of the sensitivity results closely approximates these projections, revealing the relative contributions of the individual forcings on the combined volume change and suggesting that total ice-sheet response to complicated forcings over 200 years can be linearized. C1 [Bindschadler, Robert A.; Nowicki, Sophie; Wang, Wei Li] NASA, Goddard Space Flight Ctr, Greenbelt, MD USA. [Abe-Ouchi, Ayako] Univ Tokyo, Atmosphere & Ocean Res Inst, Kashiwa, Chiba, Japan. [Aschwanden, Andy; Khroulev, Constantine] Univ Alaska Fairbanks, Inst Geophys, Fairbanks, AK 99775 USA. [Choi, Hyeungu] Sigma Space Corp, Lanham, MD USA. [Fastook, Jim] Univ Maine, Comp Sci Quaternary Inst, Orono, ME USA. [Granzow, Glen; Johnson, Jesse] Univ Montana, Coll Arts & Sci, Missoula, MT 59812 USA. [Greve, Ralf; Sato, Tatsuru; Seddik, Hakime] Hokkaido Univ, Inst Low Temp Sci, Sapporo, Hokkaido 060, Japan. [Gutowski, Gail; Jackson, Charles] Univ Texas Austin, Inst Geophys, Austin, TX USA. [Herzfeld, Ute] Univ Colorado, Dept Elect Comp & Energy Engn, Boulder, CO 80309 USA. [Herzfeld, Ute] Univ Colorado, Cooperat Inst Res Environm Sci, Boulder, CO 80309 USA. [Levermann, Anders] Univ Potsdam, Inst Phys, Potsdam, Germany. [Lipscomb, William H.; Price, Stephen F.] Los Alamos Natl Lab, Los Alamos, NM USA. [Martin, Maria A.] Potsdam Inst Climate Impact Res, Potsdam, Germany. [Morlighem, Mathieu] Univ Calif Irvine, Dept Earth Syst Sci, Irvine, CA USA. [Parizek, Byron R.] Penn State DuBois, Math & Geosci, Du Bois, PA USA. [Pollard, David] Penn State Univ, Earth & Environm Syst Inst, University Pk, PA 16802 USA. [Ren, Diandong] Curtin Univ Technol, Dept Phys, Perth, WA, Australia. [Saito, Fuyuki; Takahashi, Kunio] Japan Agcy Marine Earth Sci & Technol, Res Inst Global Change, Kanazawa Ku, Yokohama, Kanagawa, Japan. [Seroussi, Helene] CALTECH, Jet Prop Lab, Pasadena, CA USA. [Walker, Ryan] Univ Maryland, Earth Syst Sci Interdisciplinary Ctr, College Pk, MD 20742 USA. RP Bindschadler, RA (reprint author), NASA, Goddard Space Flight Ctr, Greenbelt, MD USA. EM robert.a.bindschadler@nasa.gov RI Levermann, Anders/G-4666-2011; Price, Stephen /E-1568-2013; Greve, Ralf/G-2336-2010; Abe-Ouchi, Ayako/M-6359-2013; Seddik, Hakime/F-7640-2014; Morlighem, Mathieu/O-9942-2014; Jackson, Charles/A-2202-2009; Ren, Diandong/C-8870-2013; OI Levermann, Anders/0000-0003-4432-4704; Price, Stephen /0000-0001-6878-2553; Greve, Ralf/0000-0002-1341-4777; Abe-Ouchi, Ayako/0000-0003-1745-5952; Seddik, Hakime/0000-0002-0241-590X; Morlighem, Mathieu/0000-0001-5219-1310; Jackson, Charles/0000-0002-2870-4494; Ren, Diandong/0000-0002-5757-7527; SAITO, Fuyuki/0000-0001-5935-9614 FU Japan Society for the Promotion of Science (JSPS) [22244058]; NASA [NNX11AP39G, NNX-09-AV94G, NNX-10-AI04G, 281945.02.53.02.19]; US National Science Foundation (NSF) [0531211, 0758274, 0909335]; Center for Remote Sensing of Ice Sheets (CReSIS) [0424589]; NSF [0909335, ANT-0424589, 1043018, 25-0550-0001, OCE-1202632, CReSIS 0424589]; US Department of Energy (DOE) Office of Science Office of Biological and Environmental Research; DOE's Office of Science [DE-AC02-05CH11231, DE-AC05-000R22725]; Jet Propulsion Laboratory (JPL) Research Technology and Development Program; Gary Comer Science and Education Foundation FX R. Greve, H. Seddik and T. Sato were supported by a Grant-in-Aid for Scientific Research A (No. 22244058) from the Japan Society for the Promotion of Science (JSPS).; U. Herzfeld was supported by a NASA Cryospheric Sciences Award (NNX11AP39G).; B. Parizek was supported by the US National Science Foundation (NSF) under grants 0531211, 0758274, 0909335 and the Center for Remote Sensing of Ice Sheets (CReSIS) 0424589 and by NASA under grants NNX-09-AV94G and NNX-10-AI04G.; D. Pollard was supported by NSF under grants ANT-0424589, 1043018, 25-0550-0001 and OCE-1202632.; S.F. Price and W.H. Lipscomb were supported by the US Department of Energy (DOE) Office of Science Office of Biological and Environmental Research. Simulations were conducted at the National Energy Research Scientific Computing Center (supported by DOE's Office of Science under contract No. DE-AC02-05CH11231) using time awarded through DOE's ASCR Leadership Computing Challenge allocation to the project 'Projections of Ice Sheet Evolution Using Advanced Ice and Ocean Models'. Model development and simulations were also conducted at the Oak Ridge Leadership Computing Facility at the Oak Ridge National Laboratory, supported by DOE's Office of Science under contract No. DE-AC05-000R22725. CISM development and simulations relied on additional support by K.J. Evans, P.H. Worley and J.A. Nichols (all of Oak Ridge National Laboratory) and A.G. Salinger (Sandia National Laboratories).; H. Seroussi and M. Morlighem are supported by the NASA Cryospheric Sciences Program and Modeling Analysis and Prediction Program, and a contract with the Jet Propulsion Laboratory (JPL) Research Technology and Development Program. H. Seroussi was also supported by an appointment to the NASA Postdoctoral Program at JPL, administered by Oak Ridge Associated Universities through a contract with NASA. Resources supporting this work were provided by the NASA High-End Computing (HEC) Program through the NASA Advanced Supercomputing (NAS) Division at Ames Research Center. E. Larour and E. Rignot further enabled their participation on SeaRISE.; R. Walker was supported by NSF through grants 0909335 and CReSIS 0424589, by NASA under grants NNX-09-AV94G and NNX-10-AI04G, and by the Gary Comer Science and Education Foundation.; W. Wang was supported by the NASA Cryospheric Science program (grant 281945.02.53.02.19). NR 102 TC 82 Z9 83 U1 5 U2 64 PU CAMBRIDGE UNIV PRESS PI CAMBRIDGE PA EDINBURGH BLDG, SHAFTESBURY RD, CB2 8RU CAMBRIDGE, ENGLAND SN 0022-1430 EI 1727-5652 J9 J GLACIOL JI J. Glaciol. PY 2013 VL 59 IS 214 BP 195 EP 224 DI 10.3189/2013JoG12J125 PG 30 WC Geography, Physical; Geosciences, Multidisciplinary SC Physical Geography; Geology GA 154ZV UT WOS:000319716100001 ER PT J AU Mohanty, D Sefat, AS Kalnaus, S Li, JL Meisner, RA Payzant, EA Abraham, DP Wood, DL Daniel, C AF Mohanty, Debasish Sefat, Athena S. Kalnaus, Sergiy Li, Jianlin Meisner, Roberta A. Payzant, E. Andrew Abraham, Daniel P. Wood, David L. Daniel, Claus TI Investigating phase transformation in the Li1.2Co0.1Mn0.55Ni0.15O2 lithium-ion battery cathode during high-voltage hold (4.5 V) via magnetic, X-ray diffraction and electron microscopy studies SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID ELECTROCHEMICAL-BEHAVIOR; CRYSTAL-STRUCTURE; LOCAL-STRUCTURE; SOLID-SOLUTION; LICOO2; CAPACITY; LI2MNO3; OXIDES; CELLS; INTERCALATION AB This study is the first that provides evidence of phase transformation in a Li-rich Li1.2Co0.1Mn0.55Ni0.15O2 cathode material for lithium-ion batteries (LIBs) during constant voltage charging. Diffraction and magnetic measurement techniques were successfully implemented to investigate the structural transformation in this cathode material during holding a half-cell at 4.5 V in a charged state. The results from X-ray diffraction showed a decrease in c-lattice parameters during high-voltage hold. Magnetic data revealed an increase in average effective magnetic moments of transition metal (TM) ions at constant voltage corresponding to a change in electronic states of TM ions. Analysis showed the reduction of Ni4+ to Ni2+, which was attributed to charge compensation due to oxygen loss. The appearance of the strong {1010} forbidden reflection in the single-crystal selected area electron diffraction (SAED) data was attributed to migration of transition metal ions to the octahedral vacancy sites in the lithium layer during high-voltage hold, which was in agreement with the magnetization results. After prolonged hold at 4.5 V, high-resolution transmission electron microscopy (TEM) images along with SAED results showed the presence of spinel phases in the particles, indicating a layered to spinel like phase transformation at constant voltage in agreement with the magnetic data. The results obtained from these magnetic and diffraction studies furnish the fundamental understanding of the structural transformation pathways in Li-rich cathodes at constant voltage and will be instrumental for modifying the parent structure to achieve greater stability. C1 [Mohanty, Debasish; Sefat, Athena S.; Kalnaus, Sergiy; Meisner, Roberta A.; Wood, David L.] Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN 37931 USA. [Li, Jianlin; Daniel, Claus] Oak Ridge Natl Lab, Energy & Transportat Sci Div, Oak Ridge, TN 37831 USA. [Payzant, E. Andrew] Oak Ridge Natl Lab, Chem & Engn Mat Div, Oak Ridge, TN 37831 USA. [Abraham, Daniel P.] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. [Daniel, Claus] Univ Tennessee, Bredesen Ctr Interdisciplinary Res & Grad Educ, Knoxville, TN 37996 USA. RP Mohanty, D (reprint author), Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN 37931 USA. EM mohantyd@ornl.gov RI Payzant, Edward/B-5449-2009; Mohanty, Debasish/B-6207-2012; Daniel, Claus/A-2060-2008; Li, Jianlin/D-3476-2011; Sefat, Athena/R-5457-2016 OI Payzant, Edward/0000-0002-3447-2060; Mohanty, Debasish/0000-0003-1141-0657; Daniel, Claus/0000-0002-0571-6054; Li, Jianlin/0000-0002-8710-9847; Sefat, Athena/0000-0002-5596-3504 FU U.S. Department of Energy (DOE) [DE-AC05-00OR22725]; Office of Energy Efficiency and Renewable Energy for the Vehicle Technologies Office's Applied Battery Research Program; DOE, Basic Energy Sciences, Materials Sciences and Engineering Division; ORNL's ShaRE User Facility; Scientific User Facilities Division, Office of Basic Energy Sciences, DOE; DOE Vehicle Technologies Office (VTO) FX This research at Oak Ridge National Laboratory, managed by UT Battelle, LLC, for the U.S. Department of Energy (DOE) under contract DE-AC05-00OR22725, was sponsored by the Office of Energy Efficiency and Renewable Energy for the Vehicle Technologies Office's Applied Battery Research Program (Program Managers: Peter Faguy and David Howell). Part of this research was supported by the DOE, Basic Energy Sciences, Materials Sciences and Engineering Division and by ORNL's ShaRE User Facility, which is sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, DOE. The electrodes were produced at the DOE's Cell Fabrication Facility, Argonne National Laboratory, by Andrew Jansen and Bryant Polzin. The Cell Fabrication Facility is fully supported by the DOE Vehicle Technologies Office (VTO) within the core funding of the Applied Battery Research (ABR). NR 51 TC 57 Z9 57 U1 11 U2 116 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 20 BP 6249 EP 6261 DI 10.1039/c3ta10304h PG 13 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA 135QH UT WOS:000318303100018 ER PT J AU He, H Liu, YD Liu, Q Li, ZF Xu, F Dun, C Ren, Y Wang, MX Xie, J AF He, Hao Liu, Yadong Liu, Qi Li, Zhefei Xu, Fan Dun, Clif Ren, Yang Wang, Mei-xian Xie, Jian TI Failure Investigation of LiFePO4 Cells in Over-Discharge Conditions SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID LITHIUM-ION BATTERIES; OVERCHARGE REACTION; CAPACITY FADE; CATHODE; MECHANISMS; SAFETY AB The failure mechanism of LiFePO4 cells in over-discharge conditions has been systematically studied using commercial A123 18650 cells at a 1.0 C rate and different conditions - from 5% to 20% over-discharge (DOD = 105% to 120%). SEM/EDAX, high-energy synchrotron XRD (HESXRD), and cyclic voltammetry (CV) were used to characterize the morphology, structure, and electrode potentials of cell components both in situ and ex situ. The failure behaviors of A123 18650 cells experiencing different degrees of over-discharge were found to be similar, and the 20% over-discharge process was analyzed as the representative example. The Cu electrochemical potentials in the 1.2 M LiPF6 EC/EMC electrolyte were measured during the charge/over-discharge process using CV, proving that Cu oxidation and reduction in the cell during the charge/over-discharge cycle were theoretically possible to proceed. A possible failure mechanism is proposed: during the over-discharging process, Cu foil oxidized first to Cu+, then to Cu2+ cations; next, these Cu+ and Cu2+ cations diffused to the cathode side from the anode side; and finally, these Cu2+ cations reduced to Cu+ cations, and then reduced further, back to metallic Cu. During charge/over-discharge cycling, Cu dendrites continued growing from the cathode side, penetrating through the separator and forming a copper bridge between the anode and cathode. The copper bridge caused micro-shorting and eventually led to the failure of the cell. During the charge/over-discharge cycles, the continued cell temperature increase at the end of over-discharge is evidence of the micro-shorting. (C) 2013 The Electrochemical Society. All rights reserved. C1 [He, Hao; Liu, Yadong; Liu, Qi; Li, Zhefei; Xu, Fan; Wang, Mei-xian; Xie, Jian] Indiana Univ Purdue Univ, Purdue Sch Engn & Technol, Dept Mech Engn, Indianapolis, IN 46202 USA. [Dun, Clif] Indiana Univ, Sch Dent, Indianapolis, IN 46202 USA. [Ren, Yang] Argonne Natl Lab, Xray Sci Div, Argonne, IL 60439 USA. RP He, H (reprint author), Hunan Univ, Changsha 410082, Hunan, Peoples R China. EM jianxie@iupui.edu RI Xu, Fan/L-1114-2013; Li, Zhefei/M-1106-2015 FU U.S. Navy [N00164-09-C-GS42]; U.S. Department of Energy, Office of Science, Office of Basic Energy Science [DE-AC02-06CH11357] FX This work was financially supported by the U.S. Navy under contract N00164-09-C-GS42. The authors would also like to express appreciation to A123 Systems for providing the 18650 LiFePO4 cells for testing. Use of the Advanced Photon Source was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Science, under Contract No. DE-AC02-06CH11357. NR 17 TC 7 Z9 8 U1 4 U2 64 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 6 BP A793 EP A804 DI 10.1149/2.039306jes PG 12 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA 159VF UT WOS:000320074700006 ER PT J AU Liu, B Abouimrane, A Ren, Y Neuefeind, J Fang, ZGZ Amine, K AF Liu, Bo Abouimrane, Ali Ren, Yang Neuefeind, Joerg Fang, Zhigang Z. Amine, Khalil TI Electrochemical Study and Material Characterization of xSiO center dot(1-x)Sn30Co30C40 Composite Anode Material for Lithium-Ion Batteries SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID TIN-COBALT-CARBON; NEGATIVE-ELECTRODE; ALLOYS; SYSTEM; SN AB A novel composite anode material, SiO center dot SnxCoyCz, has attracted much attention because of its good cycle life and high capacity. Seven compositions of xSiO center dot(1-x)Sn30Co30C40, where 0 <= x <= 1, were prepared by mechanical ball milling (SPEX). The milled materials were studied by X-ray diffraction (XRD),. pair distribution function (PDF), and electrochemical testing. The XRD and PDF data show that CoSn is the main phase and is detected in all seven samples. As the amount of SiO increases, CoSn2 is formed. Also with increasing SiO, the reversible specific capacity of the composite anode materials increases, but the cycle performance declines. The composition of 50 wt% SiO-50 wt% Sn30Co30C40 gives the best electrochemical performance, a reversible capacity of 633 mAh/g after 50 cycles. X-ray and neutron PDF techniques were used to probe the local structure of as-milled 50 wt% SiO-50 wt% Sn30CO30C40. Ex-situ XRD and PDF study for samples taken at different cutoff voltages reveals a phase transformation during charge/discharge via an intercalation/conversion reaction. The full cell (i.e., Li1.2Ni0.15Co0.10Mn0.55O2 vs. 50 wt% SiO-50 wt% Sn30Co30C40 with solid lithium metallic powder coating) achieves 72% capacity retention in 200 cycles. (C) 2013 The Electrochemical Society. All rights reserved. C1 [Liu, Bo; Abouimrane, Ali; Amine, Khalil] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. [Liu, Bo; Fang, Zhigang Z.] Univ Utah, Dept Met Engn, Salt Lake City, UT 84102 USA. [Ren, Yang] Argonne Natl Lab, Adv Photon Source, Xray Sci Div, Argonne, IL 60439 USA. [Neuefeind, Joerg] Oak Ridge Natl Lab, Neutron Scattering Sci Directorate, Oak Ridge, TN 37831 USA. RP Liu, B (reprint author), Argonne Natl Lab, Chem Sci & Engn Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM abouimrane@anl.gov; zak.fang@utah.edu; amine@anl.gov RI Amine, Khalil/K-9344-2013; Neuefeind, Joerg/D-9990-2015 OI Neuefeind, Joerg/0000-0002-0563-1544 FU Applied Battery Research for Transportation program (Department of Energy) FX Funding from the Applied Battery Research for Transportation program (Department of Energy) is gratefully acknowledged. This work has benefited from the use of the beamline 11-ID-C at the Advanced Photon Source. 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. Research conducted at the Spoliation Neutron Source of Oak Ridge National Laboratory was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy. Cathode material electrode used in this experiment was produced at the U.S. Department of Energy's (DOE) Cell Fabrication Facility, Argonne National Laboratory. NR 25 TC 8 Z9 8 U1 0 U2 22 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 6 BP A882 EP A887 DI 10.1149/2.100306jes PG 6 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA 159VF UT WOS:000320074700018 ER PT J AU Lu, WQ Wu, QL Dees, DW AF Lu, Wenquan Wu, Qingliu Dees, Dennis W. TI Electrochemical Characterization of Lithium and Manganese Rich Composite Material for Lithium Ion Batteries SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID CATHODE MATERIALS; ELECTRODES; LI2MNO3; LI; MN; NI; CO; COMPLEXITY; CAPACITY AB The analysis on the voltage profiles of lithium and manganese rich composite xLi(2)MnO(3)center dot yLiMO(2) based cells within different operating potential windows reveals that the Li2MnO3-like component (originated from activated Li2MnO3 component after initial charge process) is continuously oxidized during the whole charge process. However, this component only makes the capacity contribution as the operating potential is below 3.6 V (vs. Li/Li+) during the discharge process, while the discharge capacity above 3.6 V can be attributed to the other component (LiMO2). Investigations on the single component based cells confirm that the redox potential below 3.5 V (vs. Li/Li+) and the appearance of voltage hysteresis loop with large area comes from the Li2MnO3-like component. (C) 2013 The Electrochemical Society. All rights reserved. C1 [Lu, Wenquan; Wu, Qingliu; Dees, Dennis W.] Argonne Natl Lab, Electrochem Energy Storage Chem Sci & Engn Div, Argonne, IL 60439 USA. RP Lu, WQ (reprint author), Argonne Natl Lab, Electrochem Energy Storage Chem Sci & Engn Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM luw@anl.gov RI wu, qingliu /C-7631-2012 NR 26 TC 4 Z9 4 U1 0 U2 50 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 6 BP A950 EP A954 DI 10.1149/2.134306jes PG 5 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA 159VF UT WOS:000320074700028 ER PT J AU Tavassol, H Chan, MKY Catarello, MG Greeley, J Cahill, DG Gewirth, AA AF Tavassol, Hadi Chan, Maria K. Y. Catarello, Maria G. Greeley, Jeffery Cahill, David G. Gewirth, Andrew A. TI Surface Coverage and SEI Induced Electrochemical Surface Stress Changes during Li Deposition in a Model System for Li-Ion Battery Anodes SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID IN-SITU STRESS; SCANNING-TUNNELING-MICROSCOPY; LITHIUM UNDERPOTENTIAL DEPOSITION; NEGATIVE ELECTRODE MATERIALS; BEAM DEFLECTION METHOD; SILICON THIN-FILMS; (111)-TEXTURED AU; GOLD ELECTRODE; NANOGRAVIMETRIC MEASUREMENTS; COPPER ELECTRODEPOSITION AB We report electrochemical surface stress and potential dependent matrix assisted laser desorption ionization (MALDI)-time of flight (TOF) mass spectrometry (MS) results combined with detailed density functional theory (DFT) analysis of Li deposition on a Au model system for Li ion battery anodes. Deposition of Li on Au surfaces at potentials >0.2 V -vs. Li/Li+ occurs through the formation of a Li-Au surface alloy, a result that is predicted by DFT calculations. As the Au surface potential becomes more cathodic, compressive stress develops on the surface, a result again predicted from calculation. The compressive stress is completely removed by cycling the potential back to 2.0 V vs. Li/Li+ through delithiation of the surface alloy. Lithiation of the Au electrode during Li bulk alloy formation at potentials <0.2 V vs. Li/Li+ results in compressive stress, as expected. However, in this case residual tensile stress is observed following delithiation, the magnitude of which increases with increasing lithiation/delithiation cycles. Potential dependent MALDI-TOF MS analysis shows that solid electrolyte interphase (SEI) oligomers are formed during delithiation following Li bulk alloy formation and that these oligomers are the likely origin of the observed residual tensile stress. This residual tensile stress is not present when the carbonate solvent is replaced with an ionic liquid. These results show that surface stress is determined by Li-host atomistic interactions as well as the nature of the SEI (C) 2013 The Electrochemical Society. All rights reserved. C1 [Tavassol, Hadi; Catarello, Maria G.; Gewirth, Andrew A.] Univ Illinois, Dept Chem, Urbana, IL 61801 USA. [Chan, Maria K. Y.; Greeley, Jeffery] Argonne Natl Lab, Ctr Nanoscale Mat, Argonne, IL 60439 USA. [Cahill, David G.] Univ Illinois, Dept Mat Sci & Engn, Urbana, IL 61801 USA. RP Tavassol, H (reprint author), Univ Illinois, Dept Chem, 1209 W Calif St, Urbana, IL 61801 USA. EM agewirth@uiuc.edu RI Cahill, David/B-3495-2014 FU U.S. Department of Energy; Center for Electrical Energy Storage, an Energy Frontier Research Center; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357] FX Financial support from the U.S. Department of Energy is gratefully acknowledged. This material is based upon work supported as part of 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. Use of the Center for Nanoscale Materials at Argonne National Laboratory was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. NR 84 TC 19 Z9 20 U1 6 U2 148 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 6 BP A888 EP A896 DI 10.1149/2.068306jes PG 9 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA 159VF UT WOS:000320074700019 ER PT J AU Xun, SD Song, XY Battaglia, V Liu, G AF Xun, Shidi Song, Xiangyun Battaglia, Vincent Liu, Gao TI Conductive Polymer Binder-Enabled Cycling of Pure Tin Nanoparticle Composite Anode Electrodes for a Lithium-Ion Battery SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID SECONDARY BATTERIES; NEGATIVE ELECTRODES; C COMPOSITE; PERFORMANCE; OXIDE; NANOSPHERES; STORAGE; ALLOY; FE AB Pure tin (Sn) nanoparticles can be cycled in stable and high gravimetric capacity (>500 mAh/g) with a polyfluorene-type conductive polymer binder in composite electrodes. Crystalline Sn nanoparticles (<150 nanometers, nm) were used as anode materials in this study. The average diameter of Sn secondary particles is 270 nm, calculated based on BET surface area. The composite electrodes contain a conductive polymer binder that constitutes 2% to 10% of the material, without any conductive additives (e.g., acetylene black). The electrode containing the 5% conductive binder showed the best cycling performance, with a reversible capacity of 510 mAh/g. Crystallinity of Sn particles gradually degrades during cycling, and pulverization of particles was observed after long-term cycling, leading to the capacity fade. The conductive polymer binder shows advantages over other Conventional binders, such as Poly(vinylidene difluoride) (PVDF) and carboxymethylcellulose (CMC) binders, because it can provide electrical conductivity and strong adhesion during Sn volume change. (C) 2013 The Electrochemical Society. All rights reserved. C1 [Xun, Shidi; Song, Xiangyun; Battaglia, Vincent; Liu, Gao] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Xun, SD (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. EM gliu@lbl.gov RI Foundry, Molecular/G-9968-2014 FU Assistant Secretary for Energy Efficiency, Office of Vehicle Technologies of the U.S. Department of Energy (U.S. DOE) [DE-AC02-05CH11231]; University of California, Office of the President through the University of California Discovery grant; Office of Science, Office of Basic Energy Sciences, of the U.S. DOE [DE-AC02-05CH11231] FX This work was funded by the Assistant Secretary for Energy Efficiency, Office of Vehicle Technologies of the U.S. Department of Energy (U.S. DOE) under contract no. DE-AC02-05CH11231 under the Batteries for Advanced Transportation Technologies (BATT) Program, and by the University of California, Office of the President through the University of California Discovery grant. TEM was performed at National Center for Electron Microscopy, funded by Office of Science, Office of Basic Energy Sciences, of the U.S. DOE under Contract No. DE-AC02-05CH11231. NR 32 TC 21 Z9 21 U1 2 U2 92 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 6 BP A849 EP A855 DI 10.1149/2.087306jes PG 7 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA 159VF UT WOS:000320074700013 ER PT J AU Li, YH Gerdes, K Liu, XB AF Li, Yihong Gerdes, Kirk Liu, Xingbo TI Oxygen Transport Kinetics in Infiltrated SOFCs Cathode by Electrical Conductivity Relaxation Technique SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID OXIDE FUEL-CELLS; SURFACE EXCHANGE; DOPED CERIA; PERFORMANCE; LSM; LA0.6SR0.4COO3-DELTA; ELECTROLYTE; LSCF AB Infiltration has attracted increasing attention as an effective technique to modify SOFC cathodes to improve cell electrochemical performance while maintaining material compatibility and long-term stability. However, the infiltrated material's effect on oxygen transport is still not clear and detailed knowledge of the oxygen reduction reaction in infiltrated cathodes is lacking. In this work, the technique of electrical conductivity relaxation (ECR) is used to evaluate oxygen exchange in two common infiltrated materials, Ce0.8Sm0.2O1.9 and La0.6Sr0.4CoO3-delta. The ECR technique is also used to examine the transport processes in a composite material formed with a backbone of La0.6Sr0.4Co0.2Fe0.8O3-delta and possessing a thin, dense surface layer composed of the representative infiltrate material. Both the surface oxygen exchange process and the oxygen exchange coefficient at infiltrate/LSCF interface are reported. ECR testing results indicate that the application of infiltrate under certain oxygen partial pressure conditions produces a measureable increase in the fitted oxygen exchange parameter. It is presently only possible to generate hypotheses to explain the observation. However the correlation between improved electrochemical performance and increased oxygen transport measured by ECR is reliably demonstrated. The simple and inexpensive ECR technique is utilized as a direct method to optimize the selection of specific infiltrate/backbone material systems for superior performance. (C) 2013 The Electrochemical Society. All rights reserved. C1 [Li, Yihong; Gerdes, Kirk; Liu, Xingbo] Natl Energy Technol Lab, Morgantown, WV 26507 USA. [Li, Yihong; Liu, Xingbo] W Virginia Univ, Dept Mech & Aerosp Engn, Morgantown, WV 26506 USA. RP Li, YH (reprint author), Natl Energy Technol Lab, Morgantown, WV 26507 USA. EM xingbo.liu@mail.wvu.edu FU National Energy Technology Laboratory [DE-AC26-04NT41817] FX This technical effort was performed in support of the National Energy Technology Laboratory's on-going research in West Virginia University under contract #DE-AC26-04NT41817. The valuable technical assistance and discussion from Mingyang Gong and Greg Collins in WVU are acknowledged. The assistance of Richard Pineault, David Ruehl and Randall Gemmen from NETL in Morgantown, WV are highly appreciated. NR 29 TC 6 Z9 6 U1 2 U2 50 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 EI 1945-7111 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2013 VL 160 IS 6 BP F554 EP F559 DI 10.1149/2.056306jes PG 6 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA 159VF UT WOS:000320074700078 ER PT J AU Matanovic, I Kent, PRC Garzon, FH Henson, NJ AF Matanovic, I. Kent, P. R. C. Garzon, F. H. Henson, N. J. TI Density Functional Study of the Structure, Stability and Oxygen Reduction Activity of Ultrathin Platinum Nanowires SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID INITIO MOLECULAR-DYNAMICS; TOTAL-ENERGY CALCULATIONS; AUGMENTED-WAVE METHOD; AB-INITIO; GOLD NANOWIRES; TRANSITION-METALS; SILVER NANOWIRES; BASIS-SET; ELECTROCATALYSTS; NANOPARTICLES AB We used density functional theory to study the difference in the structure, stability and catalytic reactivity between ultrathin, 0.5-1.0 nm diameter, platinum nanotubes and nanowires. Model nanowires were formed by inserting an inner chain of platinum atoms in small diameter nanotubes. In this way more stable, non-hollow structures were formed. The difference in the electronic structure of platinum nanotubes and nanowires was examined by inspecting the density of surface states and band structure. Furthermore, reactivity toward the oxygen reduction reaction of platinum nanowires was assessed by studying the change in the chemisorption energies of oxygen, hydroxyl, and hydroperoxyl groups, induced by converting the nanotube models to nanowires. Both ultrathin platinum nanotubes and nanowires show distinct properties compared to bulk platinum. Single-wall nanotubes and platinum nanowires with diameters larger than 1 nm show promise for use as oxygen reduction catalysts. (C) 2013 The Electrochemical Society. All rights reserved. C1 [Matanovic, I.; Henson, N. J.] Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. [Kent, P. R. C.] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. [Kent, P. R. C.] Oak Ridge Natl Lab, Comp Sci & Math Div, Oak Ridge, TN 37831 USA. [Garzon, F. H.] Los Alamos Natl Lab, Mat Phys & Applicat Div, Los Alamos, NM 87545 USA. RP Matanovic, I (reprint author), Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. EM ivana@lanl.gov RI Kent, Paul/A-6756-2008; OI Kent, Paul/0000-0001-5539-4017; Henson, Neil/0000-0002-1842-7884 FU LANL LDRD; U.S. Department of Energy, Energy Efficiency and Renewable Energy; Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]; CNMS; U.S. Department of Energy [DE-AC52-06NA25396]; EMSL; Department of Energy's Office of Biological and Environmental Research FX I.M. thanks the LANL LDRD program for a postdoctoral fellowship, U.S. Department of Energy, Energy Efficiency and Renewable Energy for financial support. Part of the computational work was performed using computational resources of NERSC, supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231, CNMS, sponsored at Oak Ridge National Laboratory by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy and EMSL, a national scientific user facility sponsored by the Department of Energy's Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory.; Los Alamos National Laboratory 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. This paper has been designated LA-UR-12-22233. NR 43 TC 1 Z9 1 U1 0 U2 23 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 6 BP F548 EP F553 DI 10.1149/2.047306jes PG 6 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA 159VF UT WOS:000320074700077 ER PT J AU Mishler, J Wang, Y Lujan, R Mukundan, R Borup, RL AF Mishler, Jeffrey Wang, Yun Lujan, Roger Mukundan, Rangachary Borup, Rodney L. TI An Experimental Study of Polymer Electrolyte Fuel Cell Operation at Sub-Freezing Temperatures SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID COLD-START; BEHAVIOR; MODEL; LAYER AB The ability of polymer electrolyte fuel cells (PEFCs) to startup at subfreezing temperatures is governed by whether it is able to overcome the freezing point (0 degrees C) before product ice prevents the electrochemical reactions. In this work, we experimentally investigated the coulombs of charge Q(c) transferred in PEFCs under subfreezing operation before the output voltage drops to 0.0 V. PEFCs with various membranes and catalyst-layer thicknesses, ionomer-carbon ratios, operating current density, and initial hydration of PEFCs were studied, and their influences on cold-start performance and coulombs of charge were experimentally measured. We find that subfreezing temperature, ionomer-catalyst ratio, and catalyst-layer thickness, significantly affect the amount of charge transferred before operational failure, whereas the membrane thickness and initial hydration level have limited effect for the considered cases. (C) 2013 The Electrochemical Society. All rights reserved. C1 [Mishler, Jeffrey; Wang, Yun] Univ Calif Irvine, Dept Mech & Aerosp Engn, Renewable Energy Resources Lab, Irvine, CA 92697 USA. [Lujan, Roger; Mukundan, Rangachary; Borup, Rodney L.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Mishler, J (reprint author), Univ Calif Irvine, Dept Mech & Aerosp Engn, Renewable Energy Resources Lab, Irvine, CA 92697 USA. EM yunw@uci.edu OI Mukundan, Rangachary/0000-0002-5679-3930 FU Fuel Cell Technologies Program at the U.S. Department of Energy - Energy Efficiency and Renewable Energy FX The authors express their thanks to all those who assisted in the writing of this paper. This work was supported by the Fuel Cell Technologies Program at the U.S. Department of Energy - Energy Efficiency and Renewable Energy, Technology Development Manager: Nancy Garland. NR 21 TC 3 Z9 3 U1 2 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 6 BP F514 EP F521 DI 10.1149/2.051306jes PG 8 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA 159VF UT WOS:000320074700074 ER PT J AU Ford, DC Cooper, C Cooley, LD Thompson, C Bouchard, D Albee, B Bishnoi, S AF Ford, Denise C. Cooper, Charlie Cooley, Lance D. Thompson, Chad Bouchard, Donald Albee, Brian Bishnoi, Sandra TI Chemical Analysis of Fluorine in Niobium Electropolishing SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID HYDROFLUORIC ACID; MECHANISM; CAVITIES; SPECTRA; RAMAN AB Surface topography and chemical purity are important factors in niobium superconducting radio-frequency (SRF) cavity performance. Electropolishing (EP) is currently being used to minimize the surface roughness and to remove the damaged surface layer created during cavity manufacturing. This process is not ideal for reasons such as safety and performance consistency, so research and development is ongoing. Furthermore, the EP process specifications have been developed empirically, and a molecular level understanding of the process is not complete. The currently employed polishing solution is composed of sulfuric and hydrofluoric acids, where the fluorine ion is active in polishing the niobium. We used vibrational and nuclear magnetic resonance (NMR) spectroscopies to analyze the standard solution, and show that fluorine is bound and released by the reaction of the acid components in the solution: HF + H2SO4 <-> HFSO3 + H2O. This result implies that new recipes can possibly be developed on the principle of controlled release of fluorine by a chemical reaction, which provides a route to improve the safety and effectiveness of EP. We also show that NMR or Raman spectroscopy can be used to monitor the free fluorine when polishing with the standard EP recipe. (C) 2013 The Electrochemical Society. All rights reserved. C1 [Ford, Denise C.; Cooper, Charlie; Cooley, Lance D.; Thompson, Chad] Fermilab Natl Accelerator Lab, Batavia, IL 60510 USA. [Ford, Denise C.] Northwestern Univ, Evanston, IL 60208 USA. [Bouchard, Donald] Anasazi Instruments Inc, Indianapolis, IN 46203 USA. [Albee, Brian; Bishnoi, Sandra] IIT, Chicago, IL 60616 USA. RP Ford, DC (reprint author), Fermilab Natl Accelerator Lab, POB 500, Batavia, IL 60510 USA. EM deniseford@u.northwestern.edu RI Cooley, Lance/E-7377-2015 OI Cooley, Lance/0000-0003-3488-2980 FU U.S. Department of Energy [DE-AC02-07CH11359] FX This work was supported in part by the U.S. Department of Energy under Contract No. DE-AC02-07CH11359. We are grateful to D. N. Seidman for reading the manuscript. NR 23 TC 0 Z9 0 U1 0 U2 5 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 6 BP H398 EP H403 DI 10.1149/2.144306jes PG 6 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA 159VF UT WOS:000320074700119 ER PT J AU Deblonde, GJP Sturzbecher-Hoehne, M Mason, AB Abergel, RJ AF Deblonde, Gauthier J. -P. Sturzbecher-Hoehne, Manuel Mason, Anne B. Abergel, Rebecca J. TI Receptor recognition of transferrin bound to lanthanides and actinides: a discriminating step in cellular acquisition of f-block metals SO METALLOMICS LA English DT Article ID HUMAN-SERUM; ENDOSOMAL PH; IRON RELEASE; BINDING; MECHANISM; DECORPORATION; COMPLEXATION; SPECIATION; PLUTONIUM; TRANSPORT AB Following an internal contamination event, the transport of actinide (An) and lanthanide (Ln) metal ions through the body is facilitated by endogenous ligands such as the human iron-transport protein transferrin (Tf). The recognition of resulting metallo-transferrin complexes (M2Tf) by the cognate transferrin receptor (TfR) is therefore a critical step for cellular uptake of these metal ions. A high performance liquid chromatography-based method has been used to probe the binding of M2Tf with TfR, yielding a direct measurement of the successive thermodynamic constants that correspond to the dissociation of TfR(M2Tf)(2) and TfR(M2Tf) complexes for Fe3+, Ga3+, La3+, Nd3+, Gd3+, Yb3+, Lu3+, Th-232(4+), (UO22+)-U-238, and Pu-242(4+). Important features of this method are (i) its ability to distinguish both 1:1 and 1:2 complexes formed between the receptor and the metal-bound transferrin, and (ii) the requirement for very small amounts of each binding partner (<1 nmol of protein per assay). Consistent with previous reports, the strongest receptor affinity is found for Fe2Tf (K-d1 = 5 nM and K-d2 = 20 nM), while the lowest affinity was measured for Pu2Tf (K-d1 = 0.28 mu M and K-d2 = 1.8 mu M) binding to the TfR. Other toxic metal ions such as Th-IV and U-VI, when bound to Tf, are well recognized by the TfR. Under the described experimental conditions, the relative stabilities of TfR:(MxTf)(y) adducts follow the order Fe3+ >> Th4+ similar to UO22+ similar to Cm3+ > Ln(3+) similar to Ga3+ >>> Yb3+ similar to Pu4+. This study substantiates a role for Tf in binding lanthanide fission products and actinides, and transporting them into cells by receptor-mediated endocytosis. C1 [Deblonde, Gauthier J. -P.; Sturzbecher-Hoehne, Manuel; Abergel, Rebecca J.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Glenn T Seaborg Ctr, Div Chem Sci, Berkeley, CA 94720 USA. [Mason, Anne B.] Univ Vermont, Coll Med, Dept Biochem, Burlington, VT 05405 USA. RP Abergel, RJ (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Glenn T Seaborg Ctr, Div Chem Sci, Berkeley, CA 94720 USA. EM rjabergel@lbl.gov RI Deblonde, Gauthier/O-3881-2014 OI Deblonde, Gauthier/0000-0002-0825-8714 FU National Institutes of Health [RAI087604Z]; Laboratory Directed Research and Development Program at Lawrence Berkeley National Laboratory [DE-AC02-05CH11231]; U.S. Public Service Grant [R01 DK 21739] FX Instrument acquisition and method development for the chromatography assays were supported by the National Institutes of Health (R.J.A., RAI087604Z); the experimental work on lanthanide and actinide protein interactions was supported by the Laboratory Directed Research and Development Program at Lawrence Berkeley National Laboratory under Contract No. DE-AC02-05CH11231 (R.J.A.), and by a U.S. Public Service Grant (A.B.M., R01 DK 21739). NR 37 TC 10 Z9 10 U1 2 U2 36 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 6 BP 619 EP 626 DI 10.1039/c3mt20237b PG 8 WC Biochemistry & Molecular Biology SC Biochemistry & Molecular Biology GA 155VU UT WOS:000319777300004 PM 23446908 ER PT J AU Kozer, N Barua, D Orchard, S Nice, EC Burgess, AW Hlavacek, WS Clayton, AHA AF Kozer, Noga Barua, Dipak Orchard, Suzanne Nice, Eduoard C. Burgess, Antony W. Hlavacek, William S. Clayton, Andrew H. A. TI Exploring higher-order EGFR oligomerisation and phosphorylation-a combined experimental and theoretical approach SO MOLECULAR BIOSYSTEMS LA English DT Article ID EPIDERMAL-GROWTH-FACTOR; RECEPTOR TYROSINE KINASES; IMAGE CORRELATION SPECTROSCOPY; PLASMA-MEMBRANE; CELL-SURFACE; LIGAND-BINDING; LIVING CELLS; SIGNALING COMPLEXES; CRYSTAL-STRUCTURE; LOW-AFFINITY AB The epidermal growth factor receptor ( EGFR) kinase is generally considered to be activated by either ligand-induced dimerisation or a ligand-induced conformational change within pre-formed dimers. Ligand-induced higher-order EGFR oligomerisation or clustering has been reported but it is not clear how EGFR oligomers, as distinct from EGFR dimers, influence signaling outputs. To address this question, we combined measures of receptor clustering (microscopy; image correlation spectroscopy) and phosphorylation (Western blots) with modelling of mass-action chemical kinetics. A stable BaF/3 cell-line that contains a high proportion (>90%) of inactive dimers of EGFR-eGFP but no secreted ligand and no other detectable ErbB receptors was used as the model cell system. EGF at concentrations of greater than 1 nM was found to cluster EGFR-eGFP dimers into higher-order complexes and cause parallel increases in EGFR phosphorylation. The kinetics of EGFR clustering and phosphorylation were both rapid, plateauing within 2 minutes after stimulation with 30 nM EGF. A rule-based model was formulated to interpret the data. This model took into account ligand binding, ligand-induced conformational changes in the cytosolic tail, monomer-dimer-trimer-tetramer transitions via ectodomain- and kinase-mediated interactions, and phosphorylation. The model predicts that cyclic EGFR tetramers are the predominant phosphorylated species, in which activated receptor dimers adopt a cyclic side-by-side orientation, and that receptor kinase activation is stabilised by the intramolecular interactions responsible for cyclic tetramerization. C1 [Kozer, Noga; Clayton, Andrew H. A.] Swinburne Univ Technol, Cell Biophys Lab, Fac Engn & Ind Sci, Ctr Microphoton, Hawthorn, Vic 3122, Australia. [Barua, Dipak; Hlavacek, William S.] Los Alamos Natl Lab, Theoret Biol & Biophys Grp, Div Theoret, Los Alamos, NM 87545 USA. [Barua, Dipak; Hlavacek, William S.] Los Alamos Natl Lab, Ctr Nonlinear Studies, Los Alamos, NM 87545 USA. [Orchard, Suzanne; Nice, Eduoard C.; Burgess, Antony W.] Royal Melbourne Hosp, Ludwig Inst Canc Res, Melbourne Parkville Branch, Melbourne, Vic 3050, Australia. [Nice, Eduoard C.] Monash Univ, Dept Biochem, Clayton, Vic 3080, Australia. RP Hlavacek, WS (reprint author), Los Alamos Natl Lab, Theoret Biol & Biophys Grp, Div Theoret, Mail Stop K710, Los Alamos, NM 87545 USA. EM tburgess@wehi.edu.au; wish@lanl.gov; aclayton@swin.edu.au RI Clayton, Andrew/I-1454-2013; OI Hlavacek, William/0000-0003-4383-8711 FU Australian NHMRC [433624]; NHMRC [487922]; NIH [P50 GM085273]; DOE [DE-AC52-06NA25396] FX This work was partially supported by Australian NHMRC Project Grant no. 433624, NHMRC program Grant no. 487922, NIH grant P50 GM085273, and DOE contract DE-AC52-06NA25396. NR 67 TC 17 Z9 17 U1 0 U2 20 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1742-206X EI 1742-2051 J9 MOL BIOSYST JI Mol. Biosyst. PY 2013 VL 9 IS 7 BP 1849 EP 1863 DI 10.1039/c3mb70073a PG 15 WC Biochemistry & Molecular Biology SC Biochemistry & Molecular Biology GA 157FU UT WOS:000319882200031 PM 23629589 ER PT J AU Manera, M Scoccimarro, R Percival, WJ Samushia, L McBride, CK Ross, AJ Sheth, RK White, M Reid, BA Sanchez, AG de Putter, R Xu, XY Berlind, AA Brinkmann, J Maraston, C Nichol, B Montesano, F Padmanabhan, N Skibba, RA Tojeiro, R Weaver, BA AF Manera, Marc Scoccimarro, Roman Percival, Will J. Samushia, Lado McBride, Cameron K. Ross, Ashley J. Sheth, Ravi K. White, Martin Reid, Beth A. Sanchez, Ariel G. de Putter, Roland Xu, Xiaoying Berlind, Andreas A. Brinkmann, Jonathan Maraston, Claudia Nichol, Bob Montesano, Francesco Padmanabhan, Nikhil Skibba, Ramin A. Tojeiro, Rita Weaver, Benjamin A. TI The clustering of galaxies in the SDSS-III Baryon Oscillation Spectroscopic Survey: a large sample of mock galaxy catalogues SO MONTHLY NOTICES OF THE ROYAL ASTRONOMICAL SOCIETY LA English DT Article DE galaxies: haloes; large-scale structure of Universe ID DIGITAL SKY SURVEY; COLD DARK-MATTER; HALO OCCUPATION DISTRIBUTION; POWER-SPECTRUM ANALYSIS; LARGE-SCALE STRUCTURE; GRAVITATIONAL-INSTABILITY; REDSHIFT-SPACE; COSMOLOGICAL IMPLICATIONS; ACOUSTIC-OSCILLATIONS; LAGRANGIAN APPROACH AB We present a fast method for producing mock galaxy catalogues that can be used to compute the covariance of large-scale clustering measurements and test analysis techniques. Our method populates a second-order Lagrangian perturbation theory (2LPT) matter field, where we calibrate masses of dark matter haloes by detailed comparisons with N-body simulations. We demonstrate that the clustering of haloes is recovered at similar to 10 per cent accuracy. We populate haloes with mock galaxies using a halo occupation distribution (HOD) prescription, which has been calibrated to reproduce the clustering measurements on scales between 30 and 80 h(-1) Mpc. We compare the sample covariance matrix from our mocks with analytic estimates, and discuss differences. We have used this method to make catalogues corresponding to Data Release 9 of the Baryon Oscillation Spectroscopic Survey (BOSS), producing 600 mock catalogues of the 'CMASS' galaxy sample. These mocks have enabled detailed tests of methods and errors, and have formed an integral part of companion analyses of these galaxy data. C1 [Manera, Marc; Percival, Will J.; Samushia, Lado; Ross, Ashley J.; Maraston, Claudia; Nichol, Bob; Tojeiro, Rita] Univ Portsmouth, Inst Cosmol & Gravitat, Portsmouth PO1 3FX, Hants, England. [Scoccimarro, Roman; Weaver, Benjamin A.] NYU, Ctr Cosmol & Particle Phys, New York, NY USA. [McBride, Cameron K.] Harvard Smithsonian Ctr Astrophys, Cambridge, MA 02138 USA. [Sheth, Ravi K.] Abdus Salam Int Ctr Theoret Phys, I-34151 Trieste, Italy. [Sheth, Ravi K.] Univ Penn, Dept Phys & Astron, Philadelphia, PA 19104 USA. [White, Martin] Univ Calif Berkeley, Dept Phys & Astron, Berkeley, CA 94720 USA. [White, Martin; Reid, Beth A.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Sanchez, Ariel G.; Montesano, Francesco] Max Planck Inst Extraterr Phys, D-85748 Garching, Germany. [de Putter, Roland] Univ Valencia, CSIC, Inst Fis Corpuscular, E-46071 Valencia, Spain. [de Putter, Roland] Univ Barcelona IEEC UB, Inst Cincies Cosmos, E-08028 Barcelona, Spain. [Xu, Xiaoying; Skibba, Ramin A.] Univ Arizona, Steward Observ, Tucson, AZ 85721 USA. [Berlind, Andreas A.] Vanderbilt Univ, Dept Phys & Astron, Nashville, TN 37235 USA. [Brinkmann, Jonathan] Apache Point Observ, Sunspot, NM 88349 USA. [Padmanabhan, Nikhil] Yale Univ, Dept Phys, New Haven, CT 06520 USA. RP Manera, M (reprint author), Univ Portsmouth, Inst Cosmol & Gravitat, Dennis Sciama Bldg, Portsmouth PO1 3FX, Hants, England. EM marc.manera@port.ac.uk RI White, Martin/I-3880-2015 OI White, Martin/0000-0001-9912-5070 FU European Research Council; Alfred P. Sloan Foundation; National Science Foundation; US Department of Energy Office of Science; ICG; SEPNet; University of Portsmouth; STFC; HEFCE; SGI; NSF [AST-0607747]; 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; Princeton University; Spanish Participation Group; University of Tokyo; University of Utah; Vanderbilt University; University of Virginia; University of Washington; Yale University FX MM acknowledges support from European Research Council. Funding for SDSS-III has been provided by the Alfred P. Sloan Foundation, the Participating Institutions, the National Science Foundation, and the US Department of Energy Office of Science. The SDSS-III website 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. The analysis made use of the computing resources of the National Energy Research Scientific Computing Center, the Shared Research Computing Services Pilot of the University of California and the Laboratory Research Computing project at Lawrence Berkeley National Laboratory.; Part of the numerical computations and analyses were done on the Sciama High Performance Compute (HPC) cluster which is supported by the ICG, SEPNet and the University of Portsmouth. MM thanks Gary Burton and David Bacon for designing the system and for their help when running the mocks. Parts of the process were performed on the COSMOS supercomputer which is funded by STFC, HEFCE and SGI. This research was partially supported by grant NSF AST-0607747 NR 79 TC 98 Z9 98 U1 0 U2 6 PU OXFORD UNIV PRESS PI OXFORD PA GREAT CLARENDON ST, OXFORD OX2 6DP, ENGLAND SN 0035-8711 J9 MON NOT R ASTRON SOC JI Mon. Not. Roy. Astron. Soc. PD JAN PY 2013 VL 428 IS 2 BP 1036 EP 1054 DI 10.1093/mnras/sts084 PG 19 WC Astronomy & Astrophysics SC Astronomy & Astrophysics GA 134QO UT WOS:000318229000007 ER PT J AU Ross, AJ Percival, WJ Carnero, A Zhao, GB Manera, M Raccanelli, A Aubourg, E Bizyaev, D Brewington, H Brinkmann, J Brownstein, JR Cuesta, AJ da Costa, LAN Eisenstein, DJ Ebelke, G Guo, H Hamilton, JC Magana, MV Malanushenko, E Malanushenko, V Maraston, C Montesano, F Nichol, RC Oravetz, D Pan, KK Prada, F Sanchez, AG Samushia, L Schlegel, DJ Schneider, DP Seo, HJ Sheldon, A Simmons, A Snedden, S Swanson, MEC Thomas, D Tinker, JL Tojeiro, R Zehavi, I AF Ross, Ashley J. Percival, Will J. Carnero, Aurelio Zhao, Gong-bo Manera, Marc Raccanelli, Alvise Aubourg, Eric Bizyaev, Dmitry Brewington, Howard Brinkmann, J. Brownstein, Joel R. Cuesta, Antonio J. da Costa, Luiz A. N. Eisenstein, Daniel J. Ebelke, Garrett Guo, Hong Hamilton, Jean-Christophe Magana, Mariana Vargas Malanushenko, Elena Malanushenko, Viktor Maraston, Claudia Montesano, Francesco Nichol, Robert C. Oravetz, Daniel Pan, Kaike Prada, Francisco Sanchez, Ariel G. Samushia, Lado Schlegel, David J. Schneider, Donald P. Seo, Hee-Jong Sheldon, Alaina Simmons, Audrey Snedden, Stephanie Swanson, Molly E. C. Thomas, Daniel Tinker, Jeremy L. Tojeiro, Rita Zehavi, Idit TI The clustering of galaxies in the SDSS-III DR9 Baryon Oscillation Spectroscopic Survey: constraints on primordial non-Gaussianity SO MONTHLY NOTICES OF THE ROYAL ASTRONOMICAL SOCIETY LA English DT Article DE cosmology: observations; (cosmology:) inflation; (cosmology:) large-scale structure of Universe ID DIGITAL-SKY-SURVEY; LUMINOUS RED GALAXIES; SURVEY IMAGING DATA; DATA RELEASE; ACOUSTIC-OSCILLATIONS; REDSHIFT SURVEYS; BIAS; EVOLUTION; QUASARS; PROBE AB We analyse the density field of 264 283 galaxies observed by the Sloan Digital Sky Survey (SDSS)-III Baryon Oscillation Spectroscopic Survey (BOSS) and included in the SDSS Data Release 9 (DR9). In total, the SDSS DR9 BOSS data include spectroscopic redshifts for over 400 000 galaxies spread over a footprint of more than 3000 deg(2). We measure the power spectrum of these galaxies with redshifts 0.43 < z < 0.7 in order to constrain the amount of local non-Gaussianity, f(NL)(local), in the primordial density field, paying particular attention to the impact of systematic uncertainties. The BOSS galaxy density field is systematically affected by the local stellar density and this influences the ability to accurately measure f(NL)(local). In the absence of any correction, we find (erroneously) that the probability that f(NL)(local) is greater than zero, P(f(NL)(local) > 0), is 99.5 per cent. After quantifying and correcting for the systematic bias and including the added uncertainty, we find -45 < f(NL)(local) < 195 at 95 per cent confidence and P(f(NL)(local) > 0) = 91.0 per cent. A more conservative approach assumes that we have only learnt the k dependence of the systematic bias and allows any amplitude for the systematic correction; we find that the systematic effect is not fully degenerate with that of f(NL)(local), and we determine that - 82 < f(NL)(local) < 178 (at 95 per cent confidence) and P(f(NL)(local) > 0) = 68 per cent. This analysis demonstrates the importance of accounting for the impact of Galactic foregrounds on f(NL)(local) measurements. We outline the methods that account for these systematic biases and uncertainties. We expect our methods to yield robust constraints on f(NL)(local) for both our own and future large-scale structure investigations. C1 [Ross, Ashley J.; Percival, Will J.; Zhao, Gong-bo; Manera, Marc; Raccanelli, Alvise; Maraston, Claudia; Nichol, Robert C.; Samushia, Lado; Thomas, Daniel; Tojeiro, Rita] Univ Portsmouth, Inst Cosmol & Gravitat, Portsmouth PO1 3FX, Hants, England. [Carnero, Aurelio; da Costa, Luiz A. N.] Observ Nacl, BR-20921400 Rio De Janeiro, RJ, Brazil. [Carnero, Aurelio; da Costa, Luiz A. N.] Lab Interinst E Astron LineA, BR-20921400 Rio De Janeiro, RJ, Brazil. [Raccanelli, Alvise] CALTECH, Jet Prop Lab, Pasadena, CA 91109 USA. [Raccanelli, Alvise] CALTECH, Pasadena, CA 91125 USA. [Aubourg, Eric] Univ Paris Diderot, APC, CNRS IN2P3, CEA Irfu,Obs Paris,Sorbonne Paris Cite, Paris, France. [Bizyaev, Dmitry; Brewington, Howard; Brinkmann, J.; Ebelke, Garrett; Malanushenko, Elena; Malanushenko, Viktor; Oravetz, Daniel; Pan, Kaike; Sheldon, Alaina; Simmons, Audrey; Snedden, Stephanie] Apache Point Observ, Sunspot, NM 88349 USA. [Brownstein, Joel R.] Univ Utah, Dept Phys & Astron, Salt Lake City, UT 84112 USA. [Cuesta, Antonio J.] Yale Univ, Yale Ctr Astron & Astrophys, New Haven, CT 06511 USA. [Eisenstein, Daniel J.; Swanson, Molly E. C.] Harvard Smithsonian Ctr Astrophys, Cambridge, MA 02138 USA. [Guo, Hong; Zehavi, Idit] Case Western Reserve Univ, Dept Astron, Cleveland, OH 44106 USA. [Hamilton, Jean-Christophe; Magana, Mariana Vargas] Univ Paris 07, APC, CNRS IN2P3, CEA,Observ Paris, Paris, France. [Montesano, Francesco; Sanchez, Ariel G.] Max Planck Inst Extraterr Phys, D-85748 Garching, Germany. [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. [Samushia, Lado] Ilia State Univ, Natl Abastumani Astrophys Observ, GE-1060 Tbilisi, Rep of Georgia. [Schlegel, David J.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Schneider, Donald P.] Penn State Univ, Dept Astron & Astrophys, University Pk, PA 16802 USA. [Schneider, Donald P.] Penn State Univ, Inst Gravitat & Cosmos, University Pk, PA 16802 USA. [Seo, Hee-Jong] Univ Calif Berkeley, Berkeley Ctr Cosmol Phys, LBL, Berkeley, CA 94720 USA. [Seo, Hee-Jong] Univ Calif Berkeley, Dept Phys, Berkeley, CA 94720 USA. [Tinker, Jeremy L.] NYU, Ctr Cosmol & Particle Phys, York, NY 10003 USA. RP Ross, AJ (reprint author), Univ Portsmouth, Inst Cosmol & Gravitat, Dennis Sciama Bldg, Portsmouth PO1 3FX, Hants, England. EM ashley.ross@port.ac.uk RI Guo, Hong/J-5797-2015; OI Guo, Hong/0000-0003-4936-8247; Raccanelli, Alvise/0000-0001-6726-0438; Cuesta Vazquez, Antonio Jose/0000-0002-4153-9470 FU UK Science and Technology Facilities Council [ST/I001204/1]; UK Science and Technology Facilities Research Council; European Research Council; National Aeronautics and Space Administration; Alfred P. Sloan Foundation; National Science Foundation; US Department of Energy Office of Science; University of Arizona; Brazilian Participation Group; Brookhaven National Laboratory; Cambridge University; Carnegie Mellon University; Case Western University; University of Florida; Fermilab; French Participation Group; German Participation Group; Harvard University; UC Irvine; Instituto de Astrofisica de Andalucia; Instituto de Astrofisica de Canarias; Institucio Catalana de Recerca y Estudis Avancat, Barcelona; Instituto de Fisica Corpuscular; Michigan State/Notre Dame/JINA Participation Group; Johns Hopkins University; Korean Institute for Advanced Study; 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 Pittburgh; University of Portsmouth; Princeton University; UC Santa Cruz; Spanish Participation Group; Texas Christian University; Trieste Astrophysical Observatory; University of Tokyo/IPMU; University of Utah; Vanderbilt University; University of Virginia; University of Washington; University of Wisconson; Yale University FX We thank the anonymous referee for comments that helped improve this paper. AJR is grateful to the UK Science and Technology Facilities Council for financial support through the grant ST/I001204/1. WJP is grateful for support from the UK Science and Technology Facilities Research Council and the European Research Council.; Part of the research described in this paper was carried out at the JetPropulsion Laboratory, California Institute of Technology, under a contract with the National Aeronautics and Space Administration. Funding for SDSS-III has been provided by the Alfred P. Sloan Foundation, the Participating Institutions, the National Science Foundation and the US Department of Energy Office of Science. The SDSS-III website 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, Cambridge University, Carnegie Mellon University, Case Western University, University of Florida, Fermilab, the French Participation Group, the German Participation Group, Harvard University, UC Irvine, Instituto de Astrofisica de Andalucia, Instituto de Astrofisica de Canarias, Institucio Catalana de Recerca y Estudis Avancat, Barcelona, Instituto de Fisica Corpuscular, the Michigan State/Notre Dame/JINA Participation Group, Johns Hopkins University, Korean Institute for Advanced Study, 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 Pittburgh, University of Portsmouth, Princeton University, UC Santa Cruz, the Spanish Participation Group, Texas Christian University, Trieste Astrophysical Observatory, University of Tokyo/IPMU, University of Utah, Vanderbilt University, University of Virginia, University of Washington, University of Wisconson and Yale University. NR 64 TC 46 Z9 46 U1 1 U2 5 PU OXFORD UNIV PRESS PI OXFORD PA GREAT CLARENDON ST, OXFORD OX2 6DP, ENGLAND SN 0035-8711 J9 MON NOT R ASTRON SOC JI Mon. Not. Roy. Astron. Soc. PD JAN PY 2013 VL 428 IS 2 BP 1116 EP 1127 DI 10.1093/mnras/sts094 PG 12 WC Astronomy & Astrophysics SC Astronomy & Astrophysics GA 134QO UT WOS:000318229000012 ER PT J AU Comparat, J Kneib, JP Escoffier, S Zoubian, J Ealet, A Lamareille, F Mostek, N Steele, O Aubourg, E Bailey, S Bolton, AS Brownstein, J Dawson, K Ge, J Ilbert, O Leauthaud, A Maraston, C Percival, W Ross, NP Schimd, C Schlegel, DJ Schneider, DP Thomas, D Tinker, JL Weaver, BA AF Comparat, Johan Kneib, Jean-Paul Escoffier, Stephanie Zoubian, Julien Ealet, Anne Lamareille, Fabrice Mostek, N. Steele, Oliver Aubourg, Eric Bailey, Stephen Bolton, Adam S. Brownstein, Joel Dawson, Kyle Ge, Jian Ilbert, Olivier Leauthaud, Alexie Maraston, Claudia Percival, Will Ross, Nicholas P. Schimd, Carlo Schlegel, David J. Schneider, Donald P. Thomas, Daniel Tinker, Jeremy L. Weaver, Benjamin A. TI Investigating emission-line galaxy surveys with the Sloan Digital Sky Survey infrastructure SO MONTHLY NOTICES OF THE ROYAL ASTRONOMICAL SOCIETY LA English DT Article DE cosmology: observations; large-scale structure of Universe; galaxies: abundances ID HUBBLE-SPACE-TELESCOPE; STAR-FORMING GALAXIES; DARK ENERGY SURVEY; VLT DEEP SURVEY; OBSERVATIONS COSMOLOGICAL INTERPRETATION; BARYON ACOUSTIC-OSCILLATIONS; PHOTOMETRIC REDSHIFTS; DATA RELEASE; METALLICITY RELATION; TARGET SELECTION AB The baryon acoustic oscillation (BAO) feature in the power spectrum of galaxies provides a standard ruler to probe the accelerated expansion of the Universe. The current surveys covering a comoving volume sufficient to unveil the BAO scale are limited to redshift z less than or similar to 0.7. In this paper, we study several galaxy selection schemes aiming at building an emission-line galaxy (ELG) sample in the redshift range 0.6 < z < 1.7 that would be suitable for future BAO studies using the Baryonic Oscillation Spectroscopic Survey (BOSS) spectrograph on the Sloan Digital Sky Survey (SDSS) telescope. We explore two different colour selections using both the SDSS and the Canada-France-Hawaii Telescope Legacy Survey (CFHT-LS) photometry in the u, g, r and i bands and evaluate their performance selecting luminous ELGs. From about 2000 ELGs, we identified a selection scheme that has a 75 per cent redshift measurement efficiency. This result confirms the feasibility of massive ELG surveys using the BOSS spectrograph on the SDSS telescope for a BAO detection at z similar to 1, in particular the proposed eBOSS experiment, which plans to use the SDSS telescope to combine the use of the BAO ruler with redshift space distortions using ELGs and quasars in the redshift range 0.6 < z < 2.2. C1 [Comparat, Johan; Kneib, Jean-Paul; Zoubian, Julien; Ilbert, Olivier; Schimd, Carlo] Aix Marseille Univ, CNRS, LAM, UMR 7326, F-13388 Marseille, France. [Escoffier, Stephanie; Ealet, Anne] Univ Aix Marseille, CNRS, IN2P3, Ctr Phys Particules Marseille, F-13288 Marseille, France. [Lamareille, Fabrice] Univ Toulouse, UPS OMP, IRAP, F-31400 Toulouse, France. [Lamareille, Fabrice] CNRS, IRAP, F-31400 Toulouse, France. [Mostek, N.; Bailey, Stephen; Dawson, Kyle; Ross, Nicholas P.; Schlegel, David J.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Steele, Oliver; Maraston, Claudia; Percival, Will; Thomas, Daniel] Univ Portsmouth, ICG, Portsmouth PO1 3FX, Hants, England. [Aubourg, Eric] Univ Paris Diderot, CNRS, IN2P3, APC, F-75205 Obs De Paris, Sorbonne Paris, France. [Bolton, Adam S.; Brownstein, Joel] Univ Utah, Dept Phys & Astron, Salt Lake City, UT 84112 USA. [Ge, Jian] Univ Florida, Dept Astron, Gainesville, FL 32611 USA. [Leauthaud, Alexie] Univ Tokyo, Universe IPMU, Inst Phys & Math, Chiba 2778582, Japan. [Schneider, Donald P.] Penn State Univ, Dept Astron & Astrophys, University Pk, PA 16802 USA. [Schneider, Donald P.] Penn State Univ, Inst Gravitat & Cosmos, University Pk, PA 16802 USA. [Tinker, Jeremy L.; Weaver, Benjamin A.] NYU, Ctr Cosmol & Particle Phys, New York, NY 10003 USA. RP Comparat, J (reprint author), Aix Marseille Univ, CNRS, LAM, UMR 7326, F-13388 Marseille, France. EM johan.comparat@oamp.fr RI Kneib, Jean-Paul/A-7919-2015; OI Kneib, Jean-Paul/0000-0002-4616-4989; Escoffier, Stephanie/0000-0002-2847-7498 FU Alfred P. Sloan Foundation; National Science Foundation; US Department of Energy Office of Science; 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; Agence Nationale de la Recherche [ANR-08-BLAN-0222] FX Funding for SDSS-III has been provided by the Alfred P. Sloan Foundation, the Participating Institutions, the National Science Foundation and the US 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.; The BOSS French Participation Group is supported by Agence Nationale de la Recherche under grant ANR-08-BLAN-0222. NR 66 TC 19 Z9 19 U1 1 U2 2 PU OXFORD UNIV PRESS PI OXFORD PA GREAT CLARENDON ST, OXFORD OX2 6DP, ENGLAND SN 0035-8711 J9 MON NOT R ASTRON SOC JI Mon. Not. Roy. Astron. Soc. PD JAN PY 2013 VL 428 IS 2 BP 1498 EP 1517 DI 10.1093/mnras/sts127 PG 20 WC Astronomy & Astrophysics SC Astronomy & Astrophysics GA 134QO UT WOS:000318229000044 ER PT J AU Meyer, C Balsara, DS Aslam, TD AF Meyer, Chad Balsara, Dinshaw S. Aslam, Tariq D. TI A second-order accurate Super TimeStepping formulation for anisotropic thermal conduction (vol 422, pg 2102, 2012) SO MONTHLY NOTICES OF THE ROYAL ASTRONOMICAL SOCIETY LA English DT Correction DE conduction; MHD; methods: numerical C1 [Meyer, Chad; Balsara, Dinshaw S.] Univ Notre Dame, Dept Phys, Notre Dame, IN 46556 USA. [Aslam, Tariq D.] Los Alamos Natl Lab, WX Grp 9, Los Alamos, NM 87545 USA. RP Meyer, C (reprint author), Univ Notre Dame, Dept Phys, 225 Nieuwland Sci Hall, Notre Dame, IN 46556 USA. EM cmeyer8@nd.edu NR 1 TC 0 Z9 0 U1 0 U2 2 PU OXFORD UNIV PRESS PI OXFORD PA GREAT CLARENDON ST, OXFORD OX2 6DP, ENGLAND SN 0035-8711 J9 MON NOT R ASTRON SOC JI Mon. Not. Roy. Astron. Soc. PD JAN PY 2013 VL 428 IS 2 BP 1855 EP 1855 DI 10.1093/mnras/sts095 PG 1 WC Astronomy & Astrophysics SC Astronomy & Astrophysics GA 134QO UT WOS:000318229000071 ER PT S AU Malila, J McGraw, R Laaksonen, A Lehtinen, KEJ AF Malila, Jussi McGraw, Robert Laaksonen, Ari Lehtinen, Kari E. J. BE DeMott, PJ ODowd, CD TI Repairing the First Nucleation Theorem: Precritical Cluster Losses SO NUCLEATION AND ATMOSPHERIC AEROSOLS SE AIP Conference Proceedings LA English DT Proceedings Paper CT 19th International Conference on Nucleation and Atmospheric Aerosols (ICNAA) CY JUN 23-28, 2013 CL Colorado State Univ, Ctr Arts, Fort Collins, CO SP Comm Nucleat & Atmospher Aerosols (CNAA), Int Commiss Clouds & Precipitat (ICCP), Int Assoc Meteorol & Atmospher Sci (IAMAS), Int Union Geodesy & Geophys (IUGG), Natl Sci Fdn (NSF), Colorado State Univ, Dept Atmospher Sci, Aerodyne Res Inc, Droplet Measurement Technologies, TSI Inc HO Colorado State Univ, Ctr Arts DE clusters; nucleation theorem; losses; coagulation; diffusion; phoretic forces ID HOMOGENEOUS NUCLEATION; AEROSOL FORMATION AB We have extended the kinetic derivation of the first nucleation theorem to account for losses of precritical clusters. Model calculations with coagulation scavenging show that if unaccounted for, these losses can lead to substantial errors in the interpretation of experimental data from laboratory and field measurements. C1 [Malila, Jussi; Laaksonen, Ari; Lehtinen, Kari E. J.] Univ Eastern Finland, Dept Appl Phys, Kuopio, Finland. [McGraw, Robert] Brookhaven Natl Lab, Dept Environm Sci, Upton, NY 11973 USA. [Laaksonen, Ari] Climate Change Res, Finnish Meteorol Inst, Vantaa, Finland. [Lehtinen, Kari E. J.] Kuopio Unit, Finnish Meteorol Inst, Kuopio, Finland. RP Malila, J (reprint author), Univ Eastern Finland, Dept Appl Phys, Kuopio, Finland. FU Finnish ACCC graduate school; Academy of Finland Centre-of-Excellence [1118615] FX This work was supported by the Finnish ACCC graduate school and the Academy of Finland Centre-of-Excellence program (project no 1118615). NR 14 TC 3 Z9 3 U1 0 U2 5 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1152-4 J9 AIP CONF PROC PY 2013 VL 1527 BP 31 EP 34 DI 10.1063/1.4803197 PG 4 WC Physics, Applied SC Physics GA BFG32 UT WOS:000319766400007 ER PT S AU Kathmann, SM Sellner, B Alexander, AJ Valiev, M AF Kathmann, Shawn M. Sellner, Bernhard Alexander, Andrew J. Valiev, Marat BE DeMott, PJ ODowd, CD TI Beyond Classical Theories SO NUCLEATION AND ATMOSPHERIC AEROSOLS SE AIP Conference Proceedings LA English DT Proceedings Paper CT 19th International Conference on Nucleation and Atmospheric Aerosols (ICNAA) CY JUN 23-28, 2013 CL Colorado State Univ, Ctr Arts, Fort Collins, CO SP Comm Nucleat & Atmospher Aerosols (CNAA), Int Commiss Clouds & Precipitat (ICCP), Int Assoc Meteorol & Atmospher Sci (IAMAS), Int Union Geodesy & Geophys (IUGG), Natl Sci Fdn (NSF), Colorado State Univ, Dept Atmospher Sci, Aerodyne Res Inc, Droplet Measurement Technologies, TSI Inc HO Colorado State Univ, Ctr Arts DE nucleation; salt crystallization; charge transfer; excited states; luminescence ID WATER-ADSORPTION; NUCLEATION AB Both Classical Nucleation Theory (CNT) and ground state adiabatic descriptions of matter have taught us a great deal about nucleation phenomena. However, recent experiments have confirmed the existence of luminescence, in both the deep UV and visible regions, during crystallization of NaCl from solution - referred to as crystalloluminescence (XTL). Given the difficulty in experimentally probing the underlying nucleation mechanisms in condensed phases, the emission of radiation is characteristic of the chemical processes giving rise to that emission. This opens the possibility of using XTL as an exquisite probe of nucleation mechanisms. The inclusion of electronically excited states in the nucleation mechanism lies beyond both CNT and ground state adiabatic interactions. Here we outline the chemical physics relevant to these findings and their consequences on how we understand and model nucleation. C1 [Kathmann, Shawn M.; Sellner, Bernhard] Pacific NW Natl Lab, Phys Sci Div, Richland, WA 99352 USA. [Alexander, Andrew J.] Univ Edinburgh, Sch Chem, Edinburgh, Midlothian, Scotland. [Valiev, Marat] Pacific NW Natl Lab, Environm Mol Sci Lab, Richland, WA 99352 USA. RP Kathmann, SM (reprint author), Pacific NW Natl Lab, Phys Sci Div, Richland, WA 99352 USA. RI Alexander, Andrew/E-5330-2011 OI Alexander, Andrew/0000-0002-0897-020X FU U.S. Department of Energy, Office of Basic Energy Sciences; Division of Chemical Sciences, Geosciences, and Biosciences FX This work was supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences. Pacific Northwest National Laboratory (PNNL) is a multiprogram national laboratory operated for DOE by Battelle. NR 8 TC 0 Z9 0 U1 2 U2 7 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1152-4 J9 AIP CONF PROC PY 2013 VL 1527 BP 109 EP 112 DI 10.1063/1.4803215 PG 4 WC Physics, Applied SC Physics GA BFG32 UT WOS:000319766400025 ER PT S AU Bzdek, BR DePalma, JW Ridge, DP Laskin, J Johnston, MV AF Bzdek, Bryan R. DePalma, Joseph W. Ridge, Douglas P. Laskin, Julia Johnston, Murray V. BE DeMott, PJ ODowd, CD TI Fragmentation and Growth Energetics of Clusters Relevant to New Particle Formation SO NUCLEATION AND ATMOSPHERIC AEROSOLS SE AIP Conference Proceedings LA English DT Proceedings Paper CT 19th International Conference on Nucleation and Atmospheric Aerosols (ICNAA) CY JUN 23-28, 2013 CL Colorado State Univ, Ctr Arts, Fort Collins, CO SP Comm Nucleat & Atmospher Aerosols (CNAA), Int Commiss Clouds & Precipitat (ICCP), Int Assoc Meteorol & Atmospher Sci (IAMAS), Int Union Geodesy & Geophys (IUGG), Natl Sci Fdn (NSF), Colorado State Univ, Dept Atmospher Sci, Aerodyne Res Inc, Droplet Measurement Technologies, TSI Inc HO Colorado State Univ, Ctr Arts DE aerosol growth; ammonia; new particle formation; nucleation; sulfuric acid ID OFF-RESONANCE EXCITATION; AMMONIUM BISULFATE; RADICAL-CATION; SULFURIC-ACID; DIMETHYLAMINE AB The chemical mechanisms governing atmospheric new particle formation are not fully resolved, although this process may significantly impact cloud condensation nuclei levels. Whereas sulfuric acid is the key component, bases are also important in promoting nucleation and growth. This work utilizes a Fourier transform ion cyclotron resonance mass spectrometer (FTICR-MS) equipped with surface-induced dissociation (SID) to investigate time-and collision energy-resolved fragmentation of positively charged ammonium bisulfate clusters. Critical energies for dissociation are obtained from Rice-Ramsperger-Kassel-Marcus/Quasi-Equilibrium Theory (RRKM/QET) modeling of the experimental data and are compared to thermodynamic values. If cluster growth is considered the reverse of cluster dissociation, the results suggest that an activation barrier exists to the incorporation of ammonia into acidic clusters and that diffusion-limited cluster growth should not be assumed. C1 [Bzdek, Bryan R.; DePalma, Joseph W.; Ridge, Douglas P.; Johnston, Murray V.] Univ Delaware, Dept Chem & Biochem, Newark, DE 19716 USA. [Laskin, Julia] Pacific NW Natl Lab, Chem & Mat Sci Div, Richland, WA 99352 USA. RP Bzdek, BR (reprint author), Univ Delaware, Dept Chem & Biochem, Newark, DE 19716 USA. RI Laskin, Julia/H-9974-2012; OI Laskin, Julia/0000-0002-4533-9644; Bzdek, Bryan/0000-0003-2234-1079 FU NSF [CHE-1110554]; NSF/XSEDE [TG-ATM-100041]; U.S. Department of Energy's (DOE) Office of Basic Energy Sciences; Division of Chemical Sciences, Geosciences, and Biosciences; DOE's Office of Biological and Environmental Research; Pacific Northwest National Laboratory FX This work was supported by NSF grant no. CHE-1110554 and NSF/XSEDE supercomputing resources (Grant TG-ATM-100041). J.L. acknowledges support from the U.S. Department of Energys (DOE) Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences. The SID experiments were performed using EMSL, a national scientific user facility sponsored by the DOEs Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory. NR 11 TC 0 Z9 0 U1 0 U2 5 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1152-4 J9 AIP CONF PROC PY 2013 VL 1527 BP 177 EP 180 DI 10.1063/1.4803232 PG 4 WC Physics, Applied SC Physics GA BFG32 UT WOS:000319766400042 ER PT S AU Kuang, C Kangasluoma, J Wimmer, D Lehtipalo, K Wang, J Kulmala, M Petaja, T AF Kuang, Chongai Kangasluoma, Juha Wimmer, Daniela Lehtipalo, Katrianne Wang, Jian Kulmala, Markku Petaja, Tuukka BE DeMott, PJ ODowd, CD TI Laboratory Characterization of a Size-Resolved CPC Battery to Infer the Composition of Freshly Formed Atmospheric Nuclei SO NUCLEATION AND ATMOSPHERIC AEROSOLS SE AIP Conference Proceedings LA English DT Proceedings Paper CT 19th International Conference on Nucleation and Atmospheric Aerosols (ICNAA) CY JUN 23-28, 2013 CL Colorado State Univ, Ctr Arts, Fort Collins, CO SP Comm Nucleat & Atmospher Aerosols (CNAA), Int Commiss Clouds & Precipitat (ICCP), Int Assoc Meteorol & Atmospher Sci (IAMAS), Int Union Geodesy & Geophys (IUGG), Natl Sci Fdn (NSF), Colorado State Univ, Dept Atmospher Sci, Aerodyne Res Inc, Droplet Measurement Technologies, TSI Inc HO Colorado State Univ, Ctr Arts DE CPC calibration; heterogeneous nucleation; particle activation ID CONDENSATION PARTICLE COUNTER; 1 NM; NANOPARTICLES; CLUSTERS AB A size-resolved condensation particle counter battery (SR-CPCb) was developed to infer the composition of freshly nucleated aerosol down to 1 nm in diameter. This was accomplished by exploiting the strong dependence of CPC counting efficiency on particle composition and CPC working fluid. The SR-CPCb consists of CPCs that are optimized for sub 2 nm particle detection using the following working fluids: diethylene glycol, water, and butanol. Laboratory characterizations of the SR-CPCb were performed for challenge aerosols of various compositions down to 1 nm in diameter. C1 [Kuang, Chongai; Wang, Jian] Brookhaven Natl Lab, Div Atmospher Sci, Upton, NY 11789 USA. [Kangasluoma, Juha; Wimmer, Daniela; Lehtipalo, Katrianne; Kulmala, Markku; Petaja, Tuukka] Univ Helsinki, Dept Phys, FIN-00014 Helsinki, Finland. [Wimmer, Daniela] Goethe Univ Frankfurt, Inst Atmospher & Environm Sci, Frankfurt, Germany. [Lehtipalo, Katrianne] Airmodus Ltd, FIN-00560 Helsinki, Finland. RP Kuang, C (reprint author), Brookhaven Natl Lab, Div Atmospher Sci, Upton, NY 11789 USA. RI Petaja, Tuukka/A-8009-2008 OI Petaja, Tuukka/0000-0002-1881-9044 FU US Department of Energy (DOE) Atmospheric System Research Program (Office of Science, OBER) [DE-AC02-98CH10886]; US DOE [DE-FG-02-05ER63997]; Academy of Finland [1251427, 1139656, 141451, 133872]; Finnish Center of Excellence [1118615]; European Research Council (ATMNUCLE) FX This work was supported by the US Department of Energy (DOE) Atmospheric System Research Program (Office of Science, OBER) under contract DE-AC02-98CH10886, US DOE Grant Number DE-FG-02-05ER63997, the Academy of Finland (project nos. 1251427, 1139656, 141451, 133872), the Finnish Center of Excellence (project no. 1118615), and the European Research Council (ATMNUCLE). NR 10 TC 0 Z9 0 U1 0 U2 4 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1152-4 J9 AIP CONF PROC PY 2013 VL 1527 BP 197 EP 199 DI 10.1063/1.4803237 PG 3 WC Physics, Applied SC Physics GA BFG32 UT WOS:000319766400047 ER PT S AU Wang, J Wexler, AS AF Wang, Jian Wexler, Anthony S. BE DeMott, PJ ODowd, CD TI Adsorption of Organic Molecules May Explain Growth of Newly Nucleated Clusters and New Particle Formation SO NUCLEATION AND ATMOSPHERIC AEROSOLS SE AIP Conference Proceedings LA English DT Proceedings Paper CT 19th International Conference on Nucleation and Atmospheric Aerosols (ICNAA) CY JUN 23-28, 2013 CL Colorado State Univ, Ctr Arts, Fort Collins, CO SP Comm Nucleat & Atmospher Aerosols (CNAA), Int Commiss Clouds & Precipitat (ICCP), Int Assoc Meteorol & Atmospher Sci (IAMAS), Int Union Geodesy & Geophys (IUGG), Natl Sci Fdn (NSF), Colorado State Univ, Dept Atmospher Sci, Aerodyne Res Inc, Droplet Measurement Technologies, TSI Inc HO Colorado State Univ, Ctr Arts DE Adsorption; New particle formation; Kelvin effect ID AEROSOLS AB New particle formation consists of formation of thermodynamically stable clusters from trace gas molecules (homogeneous nucleation) followed by growth of these clusters to a detectable size. Because of the large coagulation rate of clusters smaller than 3 nm with the preexisting aerosol population, for new particle formation to take place, these clusters need to grow sufficiently fast to escape removal by coagulation. Previous studies have indicated that condensation of low-volatility organic vapor may play an important role in the initial growth of the clusters. However, due to the relatively high vapor pressure and partial molar volume of even highly oxidized organic compounds, the strong Kelvin effect may prevent typical ambient organics from condensing on these small clusters. Earlier studies did not consider that adsorption of organic molecules on the cluster surface, due to the intermolecular forces between the organic molecule and cluster, may occur and substantially alter the growth process under sub-saturated conditions. Using the Brunauer-Emmett-Teller (BET) isotherm, we show that the adsorption of organic molecules onto the surface of clusters may significantly reduce the saturation ratio required for condensation of organics to occur, and therefore may provide a physico-chemical explanation for the enhanced initial growth by condensation of organics despite the strong Kelvin effect. C1 [Wang, Jian] Brookhaven Natl Lab, Environm Sci Dept, Upton, NY 11973 USA. [Wexler, Anthony S.] Univ Calif Davis, Mech Aeronaut Engn, Davis, CA USA. RP Wang, J (reprint author), Brookhaven Natl Lab, Environm Sci Dept, Upton, NY 11973 USA. NR 11 TC 0 Z9 0 U1 0 U2 4 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1152-4 J9 AIP CONF PROC PY 2013 VL 1527 BP 258 EP 261 DI 10.1063/1.4803253 PG 4 WC Physics, Applied SC Physics GA BFG32 UT WOS:000319766400063 ER PT S AU Wang, BB Kelly, ST Sellon, R Shilling, J Tivanski, AV Moffet, RC Gilles, MK Laskin, A AF Wang, Bingbing Kelly, Stephen T. Sellon, Rachel Shilling, John Tivanski, Alexei V. Moffet, Ryan C. Gilles, Mary K. Laskin, Alexander BE DeMott, PJ ODowd, CD TI Field and Laboratory Studies of Reactions between Atmospheric Water Soluble Organic Acids and Inorganic Particles SO NUCLEATION AND ATMOSPHERIC AEROSOLS SE AIP Conference Proceedings LA English DT Proceedings Paper CT 19th International Conference on Nucleation and Atmospheric Aerosols (ICNAA) CY JUN 23-28, 2013 CL Colorado State Univ, Ctr Arts, Fort Collins, CO SP Comm Nucleat & Atmospher Aerosols (CNAA), Int Commiss Clouds & Precipitat (ICCP), Int Assoc Meteorol & Atmospher Sci (IAMAS), Int Union Geodesy & Geophys (IUGG), Natl Sci Fdn (NSF), Colorado State Univ, Dept Atmospher Sci, Aerodyne Res Inc, Droplet Measurement Technologies, TSI Inc HO Colorado State Univ, Ctr Arts DE Organic Acids; Inorganic Particles; Heterogeneous Reactions; Acid Replacement AB Atmospheric inorganic particles undergo complex heterogeneous reactions that change their physicochemical properties. Depletion of chloride in sea salt particles was reported in previous field studies and was attributed to the acid displacement of chlorides with inorganic acids, such as nitric and sulfuric acids [1-2]. Recently, we showed that NaCl can react with water soluble organic acids (WSOA) and release gaseous hydrochloric acid (HCl) resulting in formation of organic salts [3]. A similar mechanism is also applicable to mixed WSOA/nitrate particles where multi-phase reactions are driven by the volatility of nitric acid. Furthermore, secondary organic material, which is a complex mixture of carboxylic acids, exhibits the same reactivity towards chlorides and nitrates. Here, we present a systematic study of reactions between atmospheric relevant WSOA, SOM, and inorganic salts including NaCl, NaNO3, and Ca(NO3)(2) using complementary micro-spectroscopy analysis. C1 [Wang, Bingbing; Shilling, John; Laskin, Alexander] Pacific NW Natl Lab, Richland, WA 99354 USA. [Kelly, Stephen T.; Sellon, Rachel; Gilles, Mary K.] Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Sellon, Rachel; Moffet, Ryan C.] Univ Pacific, Stockton, CA 95211 USA. [Tivanski, Alexei V.] Univ Iowa, Iowa City, IA 52242 USA. RP Wang, BB (reprint author), Pacific NW Natl Lab, Richland, WA 99354 USA. RI Wang, Bingbing/B-6211-2011; Laskin, Alexander/I-2574-2012 OI Laskin, Alexander/0000-0002-7836-8417 FU Chemical Imaging Initiative; Laboratory Directed Research and Development; Laboratory Directed Research and Development at Lawrence Berkeley National Laboratory; OBER at Pacific Northwest National Laboratory; U.S. Department of Energy by Battelle Memorial Institute [DE-AC06-76RL0]; U.S. Department of Energy [DE-AC02-10 05CH11231] FX PNNL group acknowledges support from the Chemical Imaging Initiative of the Laboratory Directed Research and Development program at Pacific Northwest National Laboratory. LBNL group acknowledges support from Laboratory Directed Research and Development at Lawrence Berkeley National Laboratory. The CCSEM/EDX and micro-FTIR particle analysis was performed in the Environmental Molecular Sciences Laboratory, a national scientific user facility sponsored by OBER at Pacific Northwest National Laboratory. PNNL is operated by the U.S. Department of Energy by Battelle Memorial Institute under contract DE-AC06-76RL0. The STXM/NEXAFS particle analysis was performed at beamlines 11.0.2 and 5.3.2 at the Advanced Light Source at Lawrence Berkeley National Laboratory. The work at the Advanced Light Source was supported by the Director, Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-10 05CH11231. NR 4 TC 0 Z9 0 U1 0 U2 8 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1152-4 J9 AIP CONF PROC PY 2013 VL 1527 BP 465 EP 467 DI 10.1063/1.4803305 PG 3 WC Physics, Applied SC Physics GA BFG32 UT WOS:000319766400115 ER PT S AU Yu, H Hallar, AG Sedlacek, A Springston, S Kanawade, V You, Y Lee, YN Wang, J Kuang, CG McGraw, RL McCubbin, I Chirokova, G Mikkila, J Lee, SH AF Yu, Huan Hallar, A. Gannet Sedlacek, Arthur Springston, Stephen Kanawade, Vijay You, Yi Lee, Yin-Nan Wang, Jian Kuang, Chongai McGraw, Robert L. McCubbin, Ian Chirokova, Galina Mikkila, Jyri Lee, Shan-Hu BE DeMott, PJ ODowd, CD TI Sub-3 nm Particle Observations in the Atmosphere of Two Sites in Eastern United States SO NUCLEATION AND ATMOSPHERIC AEROSOLS SE AIP Conference Proceedings LA English DT Proceedings Paper CT 19th International Conference on Nucleation and Atmospheric Aerosols (ICNAA) CY JUN 23-28, 2013 CL Colorado State Univ, Ctr Arts, Fort Collins, CO SP Comm Nucleat & Atmospher Aerosols (CNAA), Int Commiss Clouds & Precipitat (ICCP), Int Assoc Meteorol & Atmospher Sci (IAMAS), Int Union Geodesy & Geophys (IUGG), Natl Sci Fdn (NSF), Colorado State Univ, Dept Atmospher Sci, Aerodyne Res Inc, Droplet Measurement Technologies, TSI Inc HO Colorado State Univ, Ctr Arts DE New particle formation; sulfuric acid; sub-3 nm particles; Particle Size Magnifier ID BIOGENIC IODINE EMISSIONS; BOREAL FOREST; COASTAL ENVIRONMENT; NANO-CN; NUCLEATION; EXPLANATION; CLUSTERS; GROWTH AB Direct measurement of sub-3 nm particles is crucial for understanding the new particle formation process and its contribution to cloud condensation nuclei (CCN) formation. Sub-3 nm particles measured at Long Island, New York (coastal site) and Kent, Ohio (inland continental site) show that high concentrations of nighttime sub-3 nm particles were present at the coastal site only with marine air masses, whereas nighttime sub-3 nm particle concentrations were significantly low in continental air masses and at the inland continental site. The coastal nighttime sub-3 nm particles did not grow larger. Measured sulfuric acid and Volatile Organic Compounds (VOCs) indicate that the potential source precursors of nighttime sub-3 nm particles may be unknown ocean-originated chemical species other than sulfuric acid and biogenic VOCs (isoprene and monoterpenes). C1 [Yu, Huan; Kanawade, Vijay; You, Yi; Lee, Shan-Hu] Kent State Univ, Coll Publ Hlth, Kent, OH 44242 USA. [Hallar, A. Gannet; McCubbin, Ian; Chirokova, Galina] Desert Res Inst, Storm Peak Lab, Div Atmospher Sci, Steamboat Springs, CO 80487 USA. [Sedlacek, Arthur; Springston, Stephen; Lee, Yin-Nan; Wang, Jian; Kuang, Chongai; McGraw, Robert L.] Brookhaven Natl Lab, Div Atmospher Sci, Upton, NY 11973 USA. [Mikkila, Jyri] Airmodus Oy, Helsinki, Finland. RP Yu, H (reprint author), Kent State Univ, Coll Publ Hlth, Kent, OH 44242 USA. RI Lee, Shan-Hu/F-9913-2014; Kanawade, Vijay Punjaji/C-9848-2015 OI Kanawade, Vijay Punjaji/0000-0001-5611-3029 NR 15 TC 0 Z9 0 U1 0 U2 4 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1152-4 J9 AIP CONF PROC PY 2013 VL 1527 BP 539 EP 542 DI 10.1063/1.4803327 PG 4 WC Physics, Applied SC Physics GA BFG32 UT WOS:000319766400135 ER PT S AU Chen, MD Titcombe, M Jiang, JK Jen, C Kuang, CG Fischer, ML Eisele, FL Siepmann, I Hanson, DR Zhao, J McMurry, PH AF Chen, Modi Titcombe, Mari Jiang, Jingkun Jen, Coty Kuang, Chongai Fischer, Marc L. Eisele, Fred L. Siepmann, Ilja Hanson, David R. Zhao, Jun McMurry, Peter H. BE DeMott, PJ ODowd, CD TI Acid-Base Chemical Reaction Model for Nucleation Rates In The Polluted Atmospheric Boundary Layer SO NUCLEATION AND ATMOSPHERIC AEROSOLS SE AIP Conference Proceedings LA English DT Proceedings Paper CT 19th International Conference on Nucleation and Atmospheric Aerosols (ICNAA) CY JUN 23-28, 2013 CL Colorado State Univ, Ctr Arts, Fort Collins, CO SP Comm Nucleat & Atmospher Aerosols (CNAA), Int Commiss Clouds & Precipitat (ICCP), Int Assoc Meteorol & Atmospher Sci (IAMAS), Int Union Geodesy & Geophys (IUGG), Natl Sci Fdn (NSF), Colorado State Univ, Dept Atmospher Sci, Aerodyne Res Inc, Droplet Measurement Technologies, TSI Inc HO Colorado State Univ, Ctr Arts DE Nucleation; Nanoparticles; Clusters; CCN; Sulfuric Acid; Amines; Ammonia ID SIZE; NM AB Measurements of aerosol number distributions down to one molecule have provided information that we've used to develop a new approach for modeling atmospheric nucleation rates. Measurements were carried out with the Cluster Chemical Ionization Mass Spectrometer (Cluster CIMS), the scanning mobility spectrometer using a diethylene glycol condensation particle counter as detector (DEG SMPS), and an ambient pressure proton transfer mass spectrometer for ammonia and amines (AmPMS). The model explains nucleation as a result of cluster evolution due to a sequence of acid-base reactions. We conclude that the smallest stable cluster contains four sulfuric acid molecules. The model leads to a simple analytic expression for nucleation rates that is reasonably consistent (i.e., +/- 10x) with atmospheric observations. The model predicts that nucleation rates are equal to a prefactor, P<1, times the sulfuric acid vapor collision rate, (i.e., J=P.0.5.k(11) *[H2SO4](2)). C1 [Chen, Modi; Jiang, Jingkun; Jen, Coty; Zhao, Jun; McMurry, Peter H.] Univ Minnesota, Dept Mech Engn, 111 Church St SE, Minneapolis, MN 55455 USA. [Titcombe, Mari; Siepmann, Ilja] Univ Minnesota, Dept Chem, Minneapolis, MN 55455 USA. [Titcombe, Mari] Colorado Coll, Environm Program, Colorado Springs, CO 80903 USA. [Jiang, Jingkun] Tsinghua Univ, Dept Environm Engn, Beijing, Peoples R China. [Kuang, Chongai] Dept Environm Sci, Brookhaven Natl Lab, New York, NY 10001 USA. [Fischer, Marc L.] Lawrence Berkeley Natl Lab, Sustainable Energy Syst Grp, Berkeley, CA 94720 USA. [Eisele, Fred L.; Zhao, Jun] Natl Ctr Atmospher Res, Boulder, CO 80301 USA. [Hanson, David R.] Augsburg Coll, Dept Chem, Minneapolis, MN 55402 USA. RP Chen, MD (reprint author), Univ Minnesota, Dept Mech Engn, 111 Church St SE, Minneapolis, MN 55455 USA. RI McMurry, Peter/A-8245-2008 OI McMurry, Peter/0000-0003-1609-5131 NR 9 TC 1 Z9 1 U1 1 U2 10 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1152-4 J9 AIP CONF PROC PY 2013 VL 1527 BP 647 EP 650 DI 10.1063/1.4803354 PG 4 WC Physics, Applied SC Physics GA BFG32 UT WOS:000319766400162 ER PT S AU McGraw, R AF McGraw, Robert BE DeMott, PJ ODowd, CD TI Sparse Aerosol Models Beyond the Quadrature Method of Moments SO NUCLEATION AND ATMOSPHERIC AEROSOLS SE AIP Conference Proceedings LA English DT Proceedings Paper CT 19th International Conference on Nucleation and Atmospheric Aerosols (ICNAA) CY JUN 23-28, 2013 CL Colorado State Univ, Ctr Arts, Fort Collins, CO SP Comm Nucleat & Atmospher Aerosols (CNAA), Int Commiss Clouds & Precipitat (ICCP), Int Assoc Meteorol & Atmospher Sci (IAMAS), Int Union Geodesy & Geophys (IUGG), Natl Sci Fdn, Colorado State Univ, Dept Atmospher Sci, Aerodyne Res Inc, Droplet Measurement Technologies, TSI Inc HO Colorado State Univ, Ctr Arts DE Sparse aerosol models; Aerosol physical and optical properties; Aerosol dynamics; Quadrature Method of Moments AB This study examines a class of sparse aerosol models derived from linear programming (LP). The widely used quadrature method of moments (QMOM) is shown to fall into this class. Here it is shown how other sparse aerosol models can be constructed, which are not based on moments of the particle size distribution. The new methods enable one to bound atmospheric aerosol physical and optical properties using arbitrary combinations of model parameters and measurements. Rigorous upper and lower bounds, e. g. on the number of aerosol particles that can activate to form cloud droplets, can be obtained this way from measurement constraints that may include total particle number concentration and size distribution moments. The new LP-based methods allow a much wider range of aerosol properties, such as light backscatter or extinction coefficient, which are not easily connected to particle size moments, to also be assimilated into a list of constraints. Finally, it is shown that many of these more general aerosol properties can be tracked directly in an aerosol dynamics simulation, using SAMs, in much the same way that moments are tracked directly in the QMOM. C1 Brookhaven Natl Lab, Dept Environm Sci, Div Atmospher Sci, Upton, NY 11973 USA. RP McGraw, R (reprint author), Brookhaven Natl Lab, Dept Environm Sci, Div Atmospher Sci, Upton, NY 11973 USA. NR 6 TC 1 Z9 1 U1 0 U2 1 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1152-4 J9 AIP CONF PROC PY 2013 VL 1527 BP 651 EP 654 DI 10.1063/1.4803355 PG 4 WC Physics, Applied SC Physics GA BFG32 UT WOS:000319766400163 ER PT S AU D'Andrea, SD Hakkinen, SAK Westervelt, DM Kuang, C Spracklen, DV Riipinen, I Pierce, JR AF D'Andrea, S. D. Hakkinen, S. A. K. Westervelt, D. M. Kuang, C. Spracklen, D. V. Riipinen, I. Pierce, J. R. BE DeMott, PJ ODowd, CD TI Effect of Secondary Organic Aerosol Amount and Condensational Behavior on Global Aerosol Size Distributions SO NUCLEATION AND ATMOSPHERIC AEROSOLS SE AIP Conference Proceedings LA English DT Proceedings Paper CT 19th International Conference on Nucleation and Atmospheric Aerosols (ICNAA) CY JUN 23-28, 2013 CL Colorado State Univ, Ctr Arts, Fort Collins, CO SP Comm Nucleat & Atmospher Aerosols (CNAA), Int Commiss Clouds & Precipitat (ICCP), Int Assoc Meteorol & Atmospher Sci (IAMAS), Int Union Geodesy & Geophys (IUGG), Natl Sci Fdn (NSF), Colorado State Univ, Dept Atmospher Sci, Aerodyne Res Inc, Droplet Measurement Technologies, TSI Inc HO Colorado State Univ, Ctr Arts DE Aerosols; CCN; SOA; condensation; volatility AB Recent research has shown that secondary organic aerosols (SOA) are major contributors to ultrafine particle growth to climatically relevant sizes, increasing global cloud condensation nuclei (CCN) concentrations within the continental boundary layer. Many models treat SOA solely as semivolatile, which leads to condensation of SOA proportional to the aerosol mass distribution; however, recent closure studies with field measurements show that a significant fraction of SOA condenses proportional to the aerosol surface area, which suggests a very low volatility. Additionally, while many global models contain only biogenic sources of SOA (with emissions generally 10-30 Tg yr(-1)), recent studies have shown a need for an additional source of SOA around 100 Tg yr(-1) correlated with anthropogenic carbon monoxide (CO) emissions is required to match measurements. Here, we explore the significance of these two findings using the GEOS-Chem-TOMAS global aerosol microphysics model. The percent change in the number of particles of size D-p > 40 nm (N40) within the continental boundary layer between the surface-area-and mass-distribution condensation schemes, both with the base biogenic SOA only, yielded a global increase of 8% but exceeds 100% in biogenically active regions. The percent change in N40 within the continental boundary layer between the base simulation (19 Tg yr(-1)) and the additional SOA (100 Tg yr(-1)) both using the surface area condensation scheme (very low volatility) yielded a global increase of 14%, and a global decrease in the number of particles of size D-p > 10 nm (N10) of 32%. These model simulations were compared to measured data from Hyytiala, Finland and other global locations and confirmed a decrease in the model-measurement bias. Thus, treating SOA as very low volatile as well as including additional SOA correlated with anthropogenic CO emissions causes a significant global increase in the number of climatically relevant sized particles, and therefore we must continue to refine our SOA treatments in aerosol microphysics models. C1 [D'Andrea, S. D.] Dalhousie Univ, Dept Phys & Atmospher Sci, Halifax, NS, Canada. [D'Andrea, S. D.; Pierce, J. R.] Colorado State Univ, Dept Atmospher Sci, Ft Detrick, MD 21702 USA. [Hakkinen, S. A. K.] Univ Helsinki, Dept Phys, Helsinki, Finland. [Westervelt, D. M.] Carnegie Mellon Univ, Dept Civil & Environm Engn, Pittsburgh, PA 15213 USA. [Kuang, C.] Brookhaven Natl Lab, Div Atmospher Sci, New York, NY 10005 USA. [Spracklen, D. V.] Univ Leeds, Sch Earth & Environm, Leeds LS2 9JT, W Yorkshire, England. [Riipinen, I.] Univ Stockholm, Bert Bolin Ctr Climate Res, Dept Appl Environm Sci, S-10691 Stockholm, Sweden. RP D'Andrea, SD (reprint author), Dalhousie Univ, Dept Phys & Atmospher Sci, Halifax, NS, Canada. RI Pierce, Jeffrey/E-4681-2013; Spracklen, Dominick/B-4890-2014; Chem, GEOS/C-5595-2014 OI Pierce, Jeffrey/0000-0002-4241-838X; FU Natural Science and Engineering Research Council (NSERC) of Canada FX We thank the Atlantic Computational Excellence Network (ACEnet) for the computing resources used in this study. We thank the Natural Science and Engineering Research Council (NSERC) of Canada for funding this project. NR 7 TC 0 Z9 0 U1 0 U2 5 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1152-4 J9 AIP CONF PROC PY 2013 VL 1527 BP 667 EP 670 DI 10.1063/1.4803359 PG 4 WC Physics, Applied SC Physics GA BFG32 UT WOS:000319766400167 ER PT S AU Betancourt, RM Nenes, A Liu, XH AF Betancourt, Ricardo Morales Nenes, Athanasios Liu, Xiaohong BE DeMott, PJ ODowd, CD TI Relative Contributions of Aerosol Properties to Cloud Droplet Number: Adjoint Sensitivity Approach in a GCM SO NUCLEATION AND ATMOSPHERIC AEROSOLS SE AIP Conference Proceedings LA English DT Proceedings Paper CT 19th International Conference on Nucleation and Atmospheric Aerosols (ICNAA) CY JUN 23-28, 2013 CL Colorado State Univ, Ctr Arts, Fort Collins, CO SP Comm Nucleat & Atmospher Aerosols (CNAA), Int Commiss Clouds & Precipitat (ICCP), Int Assoc Meteorol & Atmospher Sci (IAMAS), Int Union Geodesy & Geophys (IUGG), Natl Sci Fdn (NSF), Colorado State Univ, Dept Atmospher Sci, Aerodyne Res Inc, Droplet Measurement Technologies, TSI Inc HO Colorado State Univ, Ctr Arts DE Aerosol Indirect Effects; Adjoint sensitivity ID COMMUNITY ATMOSPHERE MODEL; CLIMATE MODELS; PARAMETERIZATION AB In this work we study the sensitivity of cloud droplet number concentration to aerosol characteristics in the framework of a Global Circulation Model (GCM) by using the newly developed adjoints of a number of physically based droplet activation parameterizations. The adjoint sensitivities of these activation parameterizations were implemented in the Community Atmospheric Model version 5, which includes interactive aerosols and detailed cloud microphysics. These simulations exhibit clear patterns of high-sensitivity areas to aerosol number concentration coinciding with relatively clean environments, as well as continental and relatively polluted areas showing saturation with respect to aerosol load changes. Furthermore, in order to identify process-level discrepancies between the activation schemes in the absence of feedbacks, aerosol input fields from the Global Modeling Initiative (GMI) chemical transport model were used to drive off-line comparisons between the sensitivities of the droplet number predicted by these parameterizations against predictions with detailed numerical simulations of the activation process. Important differences were observed particularly in their response to number concentration and hygroscopicity of fine and coarse mode aerosols. Overall, the parameterizations were capable of capturing the response of droplet concentrations to perturbations in aerosol number concentration, and updraft velocity better than to chemical composition variations. C1 [Betancourt, Ricardo Morales; Nenes, Athanasios] Georgia Inst Technol, Sch Earth Ans Atmospher Sci, Atlanta, GA 30332 USA. [Nenes, Athanasios] Georgia Inst Technol, Sch Biomol & Chem Engn, Atlanta, GA 30332 USA. [Liu, Xiaohong] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Betancourt, RM (reprint author), Georgia Inst Technol, Sch Earth Ans Atmospher Sci, Atlanta, GA 30332 USA. FU DOE; NASA-ACMAP; NERSC FX We acknowledge our sources of funding, DOE and NASA-ACMAP. We also thank Dr. Xiaohong Liu for providing access to the NERSC computational resources that made this work possible. NR 8 TC 0 Z9 0 U1 0 U2 6 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1152-4 J9 AIP CONF PROC PY 2013 VL 1527 BP 679 EP 682 DI 10.1063/1.4803362 PG 4 WC Physics, Applied SC Physics GA BFG32 UT WOS:000319766400170 ER PT S AU Russell, LM Sorooshian, A Seinfeld, JH Albrecht, BA Nenes, A Leaitch, WR Macdonald, AM Ahlm, L Chen, YC Coggon, M Corrigan, A Craven, JS Flagan, RC Frossard, AA Hawkins, LN Jonsson, H Jung, E Lin, JJ Metcalf, AR Modini, R Mulmenstadt, J Roberts, GC Shingler, T Song, SW Wang, Z Wonaschutz, A AF Russell, Lynn M. Sorooshian, Armin Seinfeld, John H. Albrecht, Bruce A. Nenes, Athanasios Leaitch, W. Richard Macdonald, Anne Marie Ahlm, Lars Chen, Yi-Chun Coggon, Matthew Corrigan, Ashley Craven, Jill S. Flagan, Richard C. Frossard, Amanda A. Hawkins, Lelia N. Jonsson, Haflidi Jung, Eunsil Lin, Jack J. Metcalf, Andrew R. Modini, Robin Muelmenstaedt, Johannes Roberts, Greg C. Shingler, Taylor Song, Siwon Wang, Zhen Wonaschuetz, Anna BE DeMott, PJ ODowd, CD TI Observed Aerosol Effects on Marine Cloud Nucleation and Supersaturation SO NUCLEATION AND ATMOSPHERIC AEROSOLS SE AIP Conference Proceedings LA English DT Proceedings Paper CT 19th International Conference on Nucleation and Atmospheric Aerosols (ICNAA) CY JUN 23-28, 2013 CL Colorado State Univ, Ctr Arts, Fort Collins, CO SP Comm Nucleat & Atmospher Aerosols (CNAA), Int Commiss Clouds & Precipitat (ICCP), Int Assoc Meteorol & Atmospher Sci (IAMAS), Int Union Geodesy & Geophys (IUGG), Natl Sci Fdn (NSF), Colorado State Univ, Dept Atmospher Sci, Aerodyne Res Inc, Droplet Measurement Technologies, TSI Inc HO Colorado State Univ, Ctr Arts DE Atmospheric Aerosol; Marine Aerosol; Cloud Properties; Aerosol-Cloud Interactions; Marine Boundary Layer AB Aerosol particles in the marine boundary layer include primary organic and salt particles from sea spray and combustion-derived particles from ships and coastal cities. These particle types serve as nuclei for marine cloud droplet activation, although the particles that activate depend on the particle size and composition as well as the supersaturation that results from cloud updraft velocities. The Eastern Pacific Emitted Aerosol Cloud Experiment (E-PEACE) 2011 was a targeted aircraft campaign to assess how different particle types nucleate cloud droplets. As part of E-PEACE 2011, we studied the role of marine particles as cloud droplet nuclei and used emitted particle sources to separate particle-induced feedbacks from dynamical variability. The emitted particle sources included shipboard smoke-generated particles with 0.05-1 mu m diameters (which produced tracks measured by satellite and had drop composition characteristic of organic smoke) and combustion particles from container ships with 0.05-0.2 mu m diameters (which were measured in a variety of conditions with droplets containing both organic and sulfate components) [1]. Three central aspects of the collaborative E-PEACE results are: (1) the size and chemical composition of the emitted smoke particles compared to ship-track-forming cargo ship emissions as well as background marine particles, with particular attention to the role of organic particles, (2) the characteristics of cloud track formation for smoke and cargo ships, as well as the role of multi-layered low clouds, and (3) the implications of these findings for quantifying aerosol indirect effects. For comparison with the E-PEACE results, the preliminary results of the Stratocumulus Observations of Los-Angeles Emissions Derived Aerosol-Droplets (SOLEDAD) 2012 provided evidence of the cloud-nucleating roles of both marine organic particles and coastal urban pollution, with simultaneous measurements of the effective supersaturations of the clouds in the California coastal region. C1 [Russell, Lynn M.; Ahlm, Lars; Corrigan, Ashley; Frossard, Amanda A.; Modini, Robin; Muelmenstaedt, Johannes; Roberts, Greg C.] Univ Calif San Diego, Scripps Inst Oceanog, La Jolla, CA 92093 USA. [Seinfeld, John H.; Chen, Yi-Chun; Coggon, Matthew; Craven, Jill S.; Flagan, Richard C.; Metcalf, Andrew R.] CALTECH, Pasadena, CA 91125 USA. [Sorooshian, Armin; Shingler, Taylor; Wang, Zhen] Univ Arizona, Dept Chem & Environm Engn, Tucson, AZ 85721 USA. [Nenes, Athanasios; Lin, Jack J.] Georgia Inst Technol, Sch Earth & Atmospher Sci, Atlanta, GA 30332 USA. [Albrecht, Bruce A.; Jung, Eunsil; Song, Siwon] Univ Miami, Rosenstiel Sch Marine Sci, Coral Gables, FL 33124 USA. [Jonsson, Haflidi] Ctr Interdisciplinary Remotely Poloted Aerosol St, Marina Del Rey, CA 90292 USA. [Sorooshian, Armin; Wonaschuetz, Anna] Univ Arizona, Dept Atmospher Sci, Tucson, AZ 85721 USA. Georgia Inst Technol, Dept Chem & Biomol Engn, Atlanta, GA 30332 USA. [Roberts, Greg C.] Ctr Natl Rech Sci, Toulouse, France. [Metcalf, Andrew R.] Sandia Natl Labs, Combust Res Facil, Livermore, CA 94550 USA. [Leaitch, W. Richard; Macdonald, Anne Marie] Environm Canada, Toronto, ON, Canada. [Hawkins, Lelia N.] Harvey Mudd Coll, Claremont, CA 91711 USA. RP Russell, LM (reprint author), Univ Calif San Diego, Scripps Inst Oceanog, La Jolla, CA 92093 USA. RI Modini, Rob/A-8451-2014; OI Sorooshian, Armin/0000-0002-2243-2264 FU National Science Foundation [AGS-1013423, AGS-1008848, AGS-1013381, AGS-1013319, ATM-0744636, AGS-0821599, ATM-0349015]; Office of Naval Research [N00014-11-1-0783, N00014-10-1-0811, N00014-10-1-0200, N00014-08-1-0465] FX The E-PEACE 2011 field campaign and modeling studies were funded by the National Science Foundation (AGS-1013423; AGS-1008848; AGS-1013381; AGS-1013319; ATM-0744636; AGS-0821599; ATM-0349015) and the Office of Naval Research (N00014-11-1-0783; N00014-10-1-0811; N00014-10-1-0200; N00014-08-1-0465). Sea Spray Research, Inc., provided oil for the operation of the smoke generators. The authors gratefully acknowledge the crews of the CIRPAS Twin Otter and the R/V Point Sur for their assistance during the field campaign, Tom Maggard who revived and tirelessly maintained the smoke generators during the cruise, and Spyros Pandis for providing the CCN spectrometer. The SOLEDAD 2012 field measurements shown here were a collaboration of Scripps Institution of Oceanography and Environment Canada. NR 5 TC 0 Z9 0 U1 0 U2 14 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1152-4 J9 AIP CONF PROC PY 2013 VL 1527 BP 696 EP 701 DI 10.1063/1.4803366 PG 6 WC Physics, Applied SC Physics GA BFG32 UT WOS:000319766400174 ER PT S AU Xie, SC Liu, XH Zhao, CF Zhang, YY AF Xie, Shaocheng Liu, Xiaohong Zhao, Chuanfeng Zhang, Yuying BE DeMott, PJ ODowd, CD TI Impact of Ice Nucleation Parameterizations on CAM5 Simulated Arctic Clouds and Radiation: A Sensitivity Study SO NUCLEATION AND ATMOSPHERIC AEROSOLS SE AIP Conference Proceedings LA English DT Proceedings Paper CT 19th International Conference on Nucleation and Atmospheric Aerosols (ICNAA) CY JUN 23-28, 2013 CL Colorado State Univ, Ctr Arts, Fort Collins, CO SP Comm Nucleat & Atmospher Aerosols (CNAA), Int Commiss Clouds & Precipitat (ICCP), Int Assoc Meteorol & Atmospher Sci (IAMAS), Int Union Geodesy & Geophys (IUGG), Natl Sci Fdn (NSF), Colorado State Univ, Dept Atmospher Sci, Aerodyne Res Inc, Droplet Measurement Technologies, TSI Inc HO Colorado State Univ, Ctr Arts DE ice nucleation; community atmospheric model (CAM); arctic clouds and radiation AB Sensitivity of Arctic clouds and radiation in the Community Atmospheric Model version 5 (CAM5) to ice nucleation parameterizations is examined. The physical reasons behind these changes in cloud amount and cloud microphysical properties are discussed. Model simulations of clouds and radiation are evaluated with available observations. C1 [Xie, Shaocheng; Zhao, Chuanfeng; Zhang, Yuying] Lawrence Livermore Natl Lab, Livermore, CA USA. [Liu, Xiaohong] Pacific Northwest Natl Lab, Richland, WA USA. RP Xie, SC (reprint author), Lawrence Livermore Natl Lab, Livermore, CA USA. RI Zhao, Chuanfeng/G-8546-2013; Zhang, Yuying/H-5011-2012 FU U. S. Department of Energy (DOE), Office of Science; Office of Biological and Environmental Research; Lawrence Livermore National Laboratory [DE-AC52-07NA27344]; Battelle Memorial Institute [DE-AC06-76RLO 1830] FX The contributions of S. Xie, C. Zhao, and Y. Zhang to this work were performed under the auspices of the U. S. Department of Energy (DOE), Office of Science, Office of Biological and Environmental Research by Lawrence Livermore National Laboratory under contract No. DE-AC52-07NA27344 and supported by the DOE Earth System Modeling Program and Atmospheric Radiation Measurement Program. Support for X. Liu was provided by the DOE Office of Science Atmospheric System Research (ASR) Program and Earth System Modeling Program. The Pacific Northwest National Laboratory is operated for the DOE by Battelle Memorial Institute under contract DE-AC06-76RLO 1830. NR 2 TC 0 Z9 0 U1 1 U2 3 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1152-4 J9 AIP CONF PROC PY 2013 VL 1527 BP 747 EP 750 DI 10.1063/1.4803378 PG 4 WC Physics, Applied SC Physics GA BFG32 UT WOS:000319766400186 ER PT S AU Komurcu, M Storelvmo, T Tan, I Lohmann, U Yun, YX Penner, JE Wang, Y Liu, XH Takemura, T AF Komurcu, Muge Storelvmo, Trude Tan, Ivy Lohmann, Ulrike Yun, Yuxing Penner, Joyce E. Wang, Yong Liu, Xiaohong Takemura, Toshihiko BE DeMott, PJ ODowd, CD TI Inter-Comparison of the Phase Partitioning of Cloud Water among Global Climate Models SO NUCLEATION AND ATMOSPHERIC AEROSOLS SE AIP Conference Proceedings LA English DT Proceedings Paper CT 19th International Conference on Nucleation and Atmospheric Aerosols (ICNAA) CY JUN 23-28, 2013 CL Colorado State Univ, Ctr Arts, Fort Collins, CO SP Comm Nucleat & Atmospher Aerosols (CNAA), Int Commiss Clouds & Precipitat (ICCP), Int Assoc Meteorol & Atmospher Sci (IAMAS), Int Union Geodesy & Geophys (IUGG), Natl Sci Fdn (NSF), Colorado State Univ, Dept Atmospher Sci, Aerodyne Res Inc, Droplet Measurement Technologies, TSI Inc HO Colorado State Univ, Ctr Arts DE Cloud Water Phase Partitioning; Mixed-Phase Clouds; Ice Nucleation; GCM Inter-comparison ID ICE-NUCLEATION; CAM-OSLO; DUST AB Cloud water phase partitioning of global climate models is investigated using four different models. Two simulations are done: One with the models' default heterogeneous ice nucleation and another one using a fixed ice nucleation for all models. Results show that heterogeneous ice nucleation can influence the water phase partitioning, however, its influence is not the dominant factor leading to the phase partitioning differences among models. C1 [Komurcu, Muge; Storelvmo, Trude; Tan, Ivy] Yale Univ, Dept Geol & Geophys, New Haven, CT 06520 USA. [Lohmann, Ulrike] Swiss Fed Inst Technol, Inst Atmospher & Climate Sci, Ch-8092 Zurich, Switzerland. [Yun, Yuxing; Penner, Joyce E.] Univ Michigan, Dept Atmospher Ocean & Space Sci, Ann Arbor, MI USA. [Wang, Yong; Liu, Xiaohong] Pacific NW Natl Lab, Richland, WA 99352 USA. [Takemura, Toshihiko] Kyushu Univ, Res Inst Appl Mech, Kasuga, Fukuoka 8168580, Japan. RP Komurcu, M (reprint author), Yale Univ, Dept Geol & Geophys, POB 208109, New Haven, CT 06520 USA. RI Penner, Joyce/J-1719-2012; Lohmann, Ulrike/B-6153-2009; U-ID, Kyushu/C-5291-2016; Kyushu, RIAM/F-4018-2015; OI Lohmann, Ulrike/0000-0001-8885-3785; Komurcu, Muge/0000-0001-5313-2785; Takemura, Toshihiko/0000-0002-2859-6067 NR 17 TC 1 Z9 1 U1 0 U2 8 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1152-4 J9 AIP CONF PROC PY 2013 VL 1527 BP 755 EP 758 DI 10.1063/1.4803381 PG 4 WC Physics, Applied SC Physics GA BFG32 UT WOS:000319766400189 ER PT S AU Liu, XH Wang, Y Hoose, C AF Liu, Xiaohong Wang, Yong Hoose, Corinna BE DeMott, PJ ODowd, CD TI Implement a Classical-Theory-Based Parameterization of Heterogeneous Ice Nucleation in CAM5 SO NUCLEATION AND ATMOSPHERIC AEROSOLS SE AIP Conference Proceedings LA English DT Proceedings Paper CT 19th International Conference on Nucleation and Atmospheric Aerosols (ICNAA) CY JUN 23-28, 2013 CL Colorado State Univ, Ctr Arts, Fort Collins, CO SP Comm Nucleat & Atmospher Aerosols (CNAA), Int Commiss Clouds & Precipitat (ICCP), Int Assoc Meteorol & Atmospher Sci (IAMAS), Int Union Geodesy & Geophys (IUGG), Natl Sci Fdn (NSF), Colorado State Univ, Dept Atmospher Sci, Aerodyne Res Inc, Droplet Measurement Technologies, TSI Inc HO Colorado State Univ, Ctr Arts DE classic nucleation theory (CNT); community atmospheric model (CAM); clouds; radiation ID MODEL AB We implement the Hoose et al. [2010] parameterization, which is based on the classic nucleation theory (CNT), into the Community Atmospheric Model version 5.1 (CAM5.1) to represent the ice nucleation in mixed-phase clouds in the model. With the implementation of this new heterogeneous ice nucleation in CAM5, we find that immersion freezing by mineral dust is the dominant ice formation process in mixed-phase clouds, followed by immersion freezing by soot. Compared to immersion freezing, deposition and contact nucleation by either dust or soot, are less important. We also examine the impact of this new parameterization on the global and Arctic clouds and radiation by comparing the results with those from the default CAM5.1. C1 [Liu, Xiaohong; Wang, Yong] Pacific Northwest Natl Lab, Richland, WA 99352 USA. [Hoose, Corinna] Karlsruhe Inst Technol, Meteorol Res Inst & Climate, Karlsruhe, Germany. RP Liu, XH (reprint author), Pacific Northwest Natl Lab, Richland, WA 99352 USA. FU DOE Office of Science; Battelle Memorial Institute [DE-AC06-76RLO 1830] FX Support for X. Liu and Y. Wang was provided by the DOE Office of Science Atmospheric System Research (ASR) Program and Earth System Modeling Program.; The Pacific Northwest National Laboratory is operated for the DOE by Battelle Memorial Institute under contract DE-AC06-76RLO 1830. NR 2 TC 0 Z9 0 U1 0 U2 2 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1152-4 J9 AIP CONF PROC PY 2013 VL 1527 BP 763 EP 765 DI 10.1063/1.4803383 PG 3 WC Physics, Applied SC Physics GA BFG32 UT WOS:000319766400191 ER PT S AU Raatikainen, T Nenes, A Seinfeld, JH Morales, R Moore, RH Lathem, TL Lance, S Padro, LT Lin, JJ Cerully, KM Bougiatioti, A Cozic, J Ruehl, C Chuang, PY Anderson, BE Flagan, RC Jonsson, H Mihalopoulos, N Smith, JN AF Raatikainen, T. Nenes, A. Seinfeld, J. H. Morales, R. Moore, R. H. Lathem, T. L. Lance, S. Padro, L. T. Lin, J. J. Cerully, K. M. Bougiatioti, A. Cozic, J. Ruehl, C. Chuang, P. Y. Anderson, B. E. Flagan, R. C. Jonsson, H. Mihalopoulos, N. Smith, J. N. BE DeMott, PJ ODowd, CD TI Constraining the Water Vapor Uptake Coefficient in Ambient Cloud Droplet Formation SO NUCLEATION AND ATMOSPHERIC AEROSOLS SE AIP Conference Proceedings LA English DT Proceedings Paper CT 19th International Conference on Nucleation and Atmospheric Aerosols (ICNAA) CY JUN 23-28, 2013 CL Colorado State Univ, Ctr Arts, Fort Collins, CO SP Comm Nucleat & Atmospher Aerosols (CNAA), Int Commiss Clouds & Precipitat (ICCP), Int Assoc Meteorol & Atmospher Sci (IAMAS), Int Union Geodesy & Geophys (IUGG), Natl Sci Fdn (NSF), Colorado State Univ, Dept Atmospher Sci, Aerodyne Res Inc, Droplet Measurement Technologies, TSI Inc HO Colorado State Univ, Ctr Arts DE Water uptake; kinetics; droplet formation ID SIZE-RESOLVED CCN; ACTIVATION KINETICS; GROWTH-KINETICS; HYGROSCOPICITY; AEROSOL; ENVIRONMENT; CHAMBER AB Cloud droplet formation depends on the condensation of water vapor on ambient aerosols, the rate of which is strongly affected by the condensation (or mass accommodation) coefficient, alpha(c). Estimates of alpha(c) for droplet growth from activation of ambient particles vary considerably and represent a critical source of uncertainty in estimates of global cloud droplet distributions and the aerosol indirect forcing of climate. An analysis of ten globally relevant data sets of cloud condensation nuclei is used to constrain alpha(c), and find that rapid activation kinetics (alpha(c) > 0.1) is uniformly prevalent. This means that uncertainty in water vapor accommodation on droplets is less than previously thought and resolves a long-standing issue in cloud physics. C1 [Raatikainen, T.; Nenes, A.; Morales, R.; Lathem, T. L.; Lance, S.; Lin, J. J.; Bougiatioti, A.] Georgia Inst Technol, Dept Earth & Atmospher Sci, Atlanta, GA 30332 USA. [Raatikainen, T.] Finnish Meteorol Inst, FI-00101 Helsinki, Finland. [Nenes, A.; Moore, R. H.; Padro, L. T.; Cerully, K. M.] Georgia Inst Technol, Dept Chem & Biomol Engn, Atlanta, GA 30332 USA. [Nenes, A.; Mihalopoulos, N.] Inst Chem Engn & High Temp Chem Proc, Fdn Res & Technol, Patras GR-71110, Greece. [Seinfeld, J. H.; Flagan, R. C.] CALTECH, Dept Chem Engn, Pasadena, CA 91106 USA. [Seinfeld, J. H.; Flagan, R. C.] CALTECH, Dept Environm Sci & Engn, Pasadena, CA 91106 USA. [Moore, R. H.; Anderson, B. E.] NASA, Langley Res Ctr, Hampton, VA 23681 USA. [Lathem, T. L.] Phillips Res Ctr 66, Bartlesville, OK 74003 USA. [Lance, S.] Natl Ctr Atmospher Res, Div Atmospher Chem, Boulder, CO 80305 USA. [Lance, S.] SPEC Inc, Boulder, CO 8030 USA. [Padro, L. T.] Tufts Univ, Dept Civil & Environm Engn, Medford, MA 02155 USA. [Bougiatioti, A.] Univ Crete, Dept Chem, Iraklion GR-71003, Greece. [Cozic, J.] Natl Ocean & Atmospher Adm, Div Chem Sci, Earth Syst Res Lab, Boulder, CO 80305 USA. [Cozic, J.] Lab Glaciol & Geophys Environm, F-38402 Grenoble, France. [Ruehl, C.] Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Chuang, P. Y.] Univ Calif Santa Cruz, Dept Earth & Planetary Sci, Santa Cruz, CA 95064 USA. [Jonsson, H.] US Navy, Postgrad Sch, Monterey, CA 93943 USA. RP Raatikainen, T (reprint author), Georgia Inst Technol, Dept Earth & Atmospher Sci, Atlanta, GA 30332 USA. RI Mihalopoulos, Nikolaos/H-5327-2016 OI Mihalopoulos, Nikolaos/0000-0002-1282-0896 FU Finnish Cultural Foundation; Georgia Tech Institute Fellowships; NCAR ASP; NASA; DOE Global Change Education Fellowship; NASA ESS Fellowships; NASA Postdoctoral Fellowship; NSF; DOE; Electric Power Research Institute; NSF-CAREER; NOAA FX We acknowledge support from the Finnish Cultural Foundation, Georgia Tech Institute Fellowships, a NCAR ASP Graduate Fellowship, the NASA Graduate Student Researchers Program, a DOE Global Change Education Fellowship, NASA ESS Fellowships, a NASA Postdoctoral Fellowship, and a NSF Fellowship. Funding from the DOE, the Electric Power Research Institute, a NSF-CAREER award, NOAA and NASA is also acknowledged. We thank Dr. Xiaohong Liu for advice on using the CAM 5, Charles Brock from the NOAA Earth System Research Laboratory and the NASA Langley LARGE research team. NR 18 TC 0 Z9 0 U1 0 U2 6 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1152-4 J9 AIP CONF PROC PY 2013 VL 1527 BP 812 EP 816 DI 10.1063/1.4803395 PG 5 WC Physics, Applied SC Physics GA BFG32 UT WOS:000319766400203 ER PT J AU Zhou, YG Yang, P Zu, HY Gao, F Zu, XT AF Zhou, Yungang Yang, Ping Zu, Haoyue Gao, Fei Zu, Xiaotao TI Electronic structures and magnetic properties of MoS2 nanostructures: atomic defects, nanoholes, nanodots and antidots SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID LAYER MOS2; QUANTUM DOTS; GRAPHENE; NANORIBBONS; NANOPARTICLES; MONOLAYER; LATTICES AB Developing approaches to effectively induce and control the magnetic states is critical to the use of magnetic nanostructures in quantum information devices but is still challenging. Here MoS2-based nanostructures including atomic defects, nanoholes, nanodots and antidots are characterized with spin-polarized density functional theory. The S-vacancy defect is more likely to form than the Mo-vacancy defect due to the form of Mo-Mo metallic bonds. Among different shaped nanoholes and nanodots, triangle ones associated with ferromagnetic characteristic are most energetically favorable, and exhibit unexpected large spin moments that scale linearly with edged length. In particular, S-terminated triangle nanodots show strong spin anisotropy around the Fermi level with a substantial collective characteristic of spin states at edges, enabling it to a desired spin-filtering structure. However, in the antidot, the net spin, coupled order and stability of spin states can be engineered by controlling type and distance of internal nanoholes. Based on the analysis of the spin coupled mechanism, a specific antidot structure, the only S-terminated antidot, was determined to exhibit a large net spin with long-range ferromagnetic coupling above room temperature. Given the recent achievement of graphene- and BN-based nanohole, nanodot and antidot structures, we believe that our calculated results are suitable for experimental verification and implementation opening a new path to explore MoS2-based magnetic nanostructures. C1 [Zhou, Yungang; Zu, Haoyue; Zu, Xiaotao] Univ Elect Sci & Technol China, Dept Appl Phys, Chengdu 610054, Peoples R China. [Yang, Ping; Gao, Fei] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Zhou, YG (reprint author), Univ Elect Sci & Technol China, Dept Appl Phys, Chengdu 610054, Peoples R China. EM zhouyungang1@126.com; fei.gao@pnl.gov; xtzu@uestc.edu.cn OI Yang, Ping/0000-0003-4726-2860 FU Fundamental Research Funds for the Central Universities; Environmental Molecular Sciences Laboratory (EMSL); U. S. Department of Energy's Office of Biological and Environmental Research, located at Pacific Northwest National Laboratory (PNNL) FX This work was supported by the Fundamental Research Funds for the Central Universities. Ping Yang acknowledges partial support from the Environmental Molecular Sciences Laboratory (EMSL) through its intramural program. A portion of this research was performed using the Environmental Molecular Sciences Laboratory, a national scientific user facility sponsored by the U. S. Department of Energy's Office of Biological and Environmental Research, located at Pacific Northwest National Laboratory (PNNL). PNNL is operated by Battelle for the U. S. Department of Energy. NR 74 TC 47 Z9 49 U1 17 U2 236 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 25 BP 10385 EP 10394 DI 10.1039/c3cp50381j PG 10 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 158BJ UT WOS:000319943200040 PM 23681313 ER PT B AU Segel, LA Edelstein-Keshet, L AF Segel, Lee A. Edelstein-Keshet, Leah BA Segel, LA EdelsteinKeshet, L BF Segel, LA EdelsteinKeshet, L TI A Primer on MATHEMATICAL MODELS IN BIOLOGY Introduction SO PRIMER ON MATHEMATICAL MODELS IN BIOLOGY LA English DT Editorial Material; Book Chapter C1 [Segel, Lee A.] Weizmann Inst Sci, IL-76100 Rehovot, Israel. [Segel, Lee A.] Weizmann Inst Sci, Sci Council, IL-76100 Rehovot, Israel. [Segel, Lee A.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Segel, Lee A.] Amer Assoc Advancement Sci, Washington, DC USA. [Edelstein-Keshet, Leah] Univ British Columbia, Dept Math, Vancouver, BC, Canada. NR 0 TC 0 Z9 0 U1 0 U2 1 PU SIAM PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA BN 978-1-611972-49-8 PY 2013 BP 1 EP + D2 10.1137/1.9781611972504 PG 23 WC Mathematics, Applied SC Mathematics GA BFG45 UT WOS:000319780100001 ER PT B AU Segel, LA Edelstein-Keshet, L AF Segel, Lee A. Edelstein-Keshet, Leah BA Segel, LA EdelsteinKeshet, L BF Segel, LA EdelsteinKeshet, L TI Introduction to biochemical kinetics SO PRIMER ON MATHEMATICAL MODELS IN BIOLOGY LA English DT Editorial Material; Book Chapter C1 [Segel, Lee A.] Weizmann Inst Sci, IL-76100 Rehovot, Israel. [Segel, Lee A.] Weizmann Inst Sci, Sci Council, IL-76100 Rehovot, Israel. [Segel, Lee A.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Segel, Lee A.] Amer Assoc Advancement Sci, Washington, DC USA. [Edelstein-Keshet, Leah] Univ British Columbia, Dept Math, Vancouver, BC, Canada. NR 0 TC 0 Z9 0 U1 0 U2 0 PU SIAM PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA BN 978-1-611972-49-8 PY 2013 BP 13 EP 41 D2 10.1137/1.9781611972504 PG 29 WC Mathematics, Applied SC Mathematics GA BFG45 UT WOS:000319780100002 ER PT B AU Segel, LA Edelstein-Keshet, L AF Segel, Lee A. Edelstein-Keshet, Leah BA Segel, LA EdelsteinKeshet, L BF Segel, LA EdelsteinKeshet, L TI Review of linear differential equations SO PRIMER ON MATHEMATICAL MODELS IN BIOLOGY LA English DT Review; Book Chapter C1 [Segel, Lee A.] Weizmann Inst Sci, IL-76100 Rehovot, Israel. [Segel, Lee A.] Weizmann Inst Sci, Sci Council, IL-76100 Rehovot, Israel. [Segel, Lee A.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Segel, Lee A.] Amer Assoc Advancement Sci, Washington, DC USA. [Edelstein-Keshet, Leah] Univ British Columbia, Dept Math, Vancouver, BC, Canada. NR 0 TC 0 Z9 0 U1 0 U2 0 PU SIAM PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA BN 978-1-611972-49-8 PY 2013 BP 43 EP 66 D2 10.1137/1.9781611972504 PG 24 WC Mathematics, Applied SC Mathematics GA BFG45 UT WOS:000319780100003 ER PT B AU Segel, LA Edelstein-Keshet, L AF Segel, Lee A. Edelstein-Keshet, Leah BA Segel, LA EdelsteinKeshet, L BF Segel, LA EdelsteinKeshet, L TI Introduction to nondimensionalization and scaling SO PRIMER ON MATHEMATICAL MODELS IN BIOLOGY LA English DT Editorial Material; Book Chapter C1 [Segel, Lee A.] Weizmann Inst Sci, IL-76100 Rehovot, Israel. [Segel, Lee A.] Weizmann Inst Sci, Sci Council, IL-76100 Rehovot, Israel. [Segel, Lee A.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Segel, Lee A.] Amer Assoc Advancement Sci, Washington, DC USA. [Edelstein-Keshet, Leah] Univ British Columbia, Dept Math, Vancouver, BC, Canada. NR 0 TC 0 Z9 0 U1 0 U2 0 PU SIAM PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA BN 978-1-611972-49-8 PY 2013 BP 67 EP 82 D2 10.1137/1.9781611972504 PG 16 WC Mathematics, Applied SC Mathematics GA BFG45 UT WOS:000319780100004 ER PT B AU Segel, LA Edelstein-Keshet, L AF Segel, Lee A. Edelstein-Keshet, Leah BA Segel, LA EdelsteinKeshet, L BF Segel, LA EdelsteinKeshet, L TI Qualitative behavior of simple differential equation models SO PRIMER ON MATHEMATICAL MODELS IN BIOLOGY LA English DT Editorial Material; Book Chapter C1 [Segel, Lee A.] Weizmann Inst Sci, IL-76100 Rehovot, Israel. [Segel, Lee A.] Weizmann Inst Sci, Sci Council, IL-76100 Rehovot, Israel. [Segel, Lee A.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Segel, Lee A.] Amer Assoc Advancement Sci, Washington, DC USA. [Edelstein-Keshet, Leah] Univ British Columbia, Dept Math, Vancouver, BC, Canada. NR 0 TC 0 Z9 0 U1 0 U2 1 PU SIAM PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA BN 978-1-611972-49-8 PY 2013 BP 83 EP 102 D2 10.1137/1.9781611972504 PG 20 WC Mathematics, Applied SC Mathematics GA BFG45 UT WOS:000319780100005 ER PT B AU Segel, LA Edelstein-Keshet, L AF Segel, Lee A. Edelstein-Keshet, Leah BA Segel, LA EdelsteinKeshet, L BF Segel, LA EdelsteinKeshet, L TI Developing a model from the ground up: Case study of the spread of an infection SO PRIMER ON MATHEMATICAL MODELS IN BIOLOGY LA English DT Editorial Material; Book Chapter C1 [Segel, Lee A.] Weizmann Inst Sci, IL-76100 Rehovot, Israel. [Segel, Lee A.] Weizmann Inst Sci, Sci Council, IL-76100 Rehovot, Israel. [Segel, Lee A.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Segel, Lee A.] Amer Assoc Advancement Sci, Washington, DC USA. [Edelstein-Keshet, Leah] Univ British Columbia, Dept Math, Vancouver, BC, Canada. NR 0 TC 0 Z9 0 U1 0 U2 0 PU SIAM PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA BN 978-1-611972-49-8 PY 2013 BP 103 EP 114 D2 10.1137/1.9781611972504 PG 12 WC Mathematics, Applied SC Mathematics GA BFG45 UT WOS:000319780100006 ER PT B AU Segel, LA Edelstein-Keshet, L AF Segel, Lee A. Edelstein-Keshet, Leah BA Segel, LA EdelsteinKeshet, L BF Segel, LA EdelsteinKeshet, L TI Phase plane analysis SO PRIMER ON MATHEMATICAL MODELS IN BIOLOGY LA English DT Article; Book Chapter C1 [Segel, Lee A.] Weizmann Inst Sci, IL-76100 Rehovot, Israel. [Segel, Lee A.] Weizmann Inst Sci, Sci Council, IL-76100 Rehovot, Israel. [Segel, Lee A.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Segel, Lee A.] Amer Assoc Advancement Sci, Washington, DC USA. [Edelstein-Keshet, Leah] Univ British Columbia, Dept Math, Vancouver, BC, Canada. NR 0 TC 0 Z9 0 U1 0 U2 0 PU SIAM PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA BN 978-1-611972-49-8 PY 2013 BP 115 EP 144 D2 10.1137/1.9781611972504 PG 30 WC Mathematics, Applied SC Mathematics GA BFG45 UT WOS:000319780100007 ER PT B AU Segel, LA Edelstein-Keshet, L AF Segel, Lee A. Edelstein-Keshet, Leah BA Segel, LA EdelsteinKeshet, L BF Segel, LA EdelsteinKeshet, L TI Quasi steady state and enzyme-mediated biochemical kinetics SO PRIMER ON MATHEMATICAL MODELS IN BIOLOGY LA English DT Article; Book Chapter C1 [Segel, Lee A.] Weizmann Inst Sci, IL-76100 Rehovot, Israel. [Segel, Lee A.] Weizmann Inst Sci, Sci Council, IL-76100 Rehovot, Israel. [Segel, Lee A.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Segel, Lee A.] Amer Assoc Advancement Sci, Washington, DC USA. [Edelstein-Keshet, Leah] Univ British Columbia, Dept Math, Vancouver, BC, Canada. NR 0 TC 0 Z9 0 U1 0 U2 0 PU SIAM PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA BN 978-1-611972-49-8 PY 2013 BP 145 EP 172 D2 10.1137/1.9781611972504 PG 28 WC Mathematics, Applied SC Mathematics GA BFG45 UT WOS:000319780100008 ER PT B AU Segel, LA Edelstein-Keshet, L AF Segel, Lee A. Edelstein-Keshet, Leah BA Segel, LA EdelsteinKeshet, L BF Segel, LA EdelsteinKeshet, L TI Multiple subunit enzymes and proteins: Coperativity SO PRIMER ON MATHEMATICAL MODELS IN BIOLOGY LA English DT Article; Book Chapter C1 [Segel, Lee A.] Weizmann Inst Sci, IL-76100 Rehovot, Israel. [Segel, Lee A.] Weizmann Inst Sci, Sci Council, IL-76100 Rehovot, Israel. [Segel, Lee A.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Segel, Lee A.] Amer Assoc Advancement Sci, Washington, DC USA. [Edelstein-Keshet, Leah] Univ British Columbia, Dept Math, Vancouver, BC, Canada. NR 0 TC 0 Z9 0 U1 0 U2 0 PU SIAM PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA BN 978-1-611972-49-8 PY 2013 BP 173 EP 193 D2 10.1137/1.9781611972504 PG 21 WC Mathematics, Applied SC Mathematics GA BFG45 UT WOS:000319780100009 ER PT B AU Segel, LA Edelstein-Keshet, L AF Segel, Lee A. Edelstein-Keshet, Leah BA Segel, LA EdelsteinKeshet, L BF Segel, LA EdelsteinKeshet, L TI Dynamic behavior of neuronal membranes SO PRIMER ON MATHEMATICAL MODELS IN BIOLOGY LA English DT Article; Book Chapter C1 [Segel, Lee A.] Weizmann Inst Sci, IL-76100 Rehovot, Israel. [Segel, Lee A.] Weizmann Inst Sci, Sci Council, IL-76100 Rehovot, Israel. [Segel, Lee A.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Segel, Lee A.] Amer Assoc Advancement Sci, Washington, DC USA. [Edelstein-Keshet, Leah] Univ British Columbia, Dept Math, Vancouver, BC, Canada. NR 0 TC 0 Z9 0 U1 0 U2 0 PU SIAM PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA BN 978-1-611972-49-8 PY 2013 BP 195 EP 225 D2 10.1137/1.9781611972504 PG 31 WC Mathematics, Applied SC Mathematics GA BFG45 UT WOS:000319780100010 ER PT B AU Segel, LA Edelstein-Keshet, L AF Segel, Lee A. Edelstein-Keshet, Leah BA Segel, LA EdelsteinKeshet, L BF Segel, LA EdelsteinKeshet, L TI Excitable systems and the FitzHugh-Nagumo equations SO PRIMER ON MATHEMATICAL MODELS IN BIOLOGY LA English DT Article; Book Chapter C1 [Segel, Lee A.] Weizmann Inst Sci, IL-76100 Rehovot, Israel. [Segel, Lee A.] Weizmann Inst Sci, Sci Council, IL-76100 Rehovot, Israel. [Segel, Lee A.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Segel, Lee A.] Amer Assoc Advancement Sci, Washington, DC USA. [Edelstein-Keshet, Leah] Univ British Columbia, Dept Math, Vancouver, BC, Canada. NR 0 TC 0 Z9 0 U1 0 U2 0 PU SIAM PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA BN 978-1-611972-49-8 PY 2013 BP 227 EP 250 D2 10.1137/1.9781611972504 PG 24 WC Mathematics, Applied SC Mathematics GA BFG45 UT WOS:000319780100011 ER PT B AU Segel, LA Edelstein-Keshet, L AF Segel, Lee A. Edelstein-Keshet, Leah BA Segel, LA EdelsteinKeshet, L BF Segel, LA EdelsteinKeshet, L TI Biochemical modules SO PRIMER ON MATHEMATICAL MODELS IN BIOLOGY LA English DT Article; Book Chapter C1 [Segel, Lee A.] Weizmann Inst Sci, IL-76100 Rehovot, Israel. [Segel, Lee A.] Weizmann Inst Sci, Sci Council, IL-76100 Rehovot, Israel. [Segel, Lee A.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Segel, Lee A.] Amer Assoc Advancement Sci, Washington, DC USA. [Edelstein-Keshet, Leah] Univ British Columbia, Dept Math, Vancouver, BC, Canada. NR 0 TC 0 Z9 0 U1 0 U2 0 PU SIAM PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA BN 978-1-611972-49-8 PY 2013 BP 251 EP 281 D2 10.1137/1.9781611972504 PG 31 WC Mathematics, Applied SC Mathematics GA BFG45 UT WOS:000319780100012 ER PT B AU Segel, LA Edelstein-Keshet, L AF Segel, Lee A. Edelstein-Keshet, Leah BA Segel, LA EdelsteinKeshet, L BF Segel, LA EdelsteinKeshet, L TI Discrete networks of genes and cells SO PRIMER ON MATHEMATICAL MODELS IN BIOLOGY LA English DT Article; Book Chapter C1 [Segel, Lee A.] Weizmann Inst Sci, IL-76100 Rehovot, Israel. [Segel, Lee A.] Weizmann Inst Sci, Sci Council, IL-76100 Rehovot, Israel. [Segel, Lee A.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Segel, Lee A.] Amer Assoc Advancement Sci, Washington, DC USA. [Edelstein-Keshet, Leah] Univ British Columbia, Dept Math, Vancouver, BC, Canada. NR 0 TC 0 Z9 0 U1 0 U2 0 PU SIAM PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA BN 978-1-611972-49-8 PY 2013 BP 283 EP 310 D2 10.1137/1.9781611972504 PG 28 WC Mathematics, Applied SC Mathematics GA BFG45 UT WOS:000319780100013 ER PT B AU Segel, LA Edelstein-Keshet, L AF Segel, Lee A. Edelstein-Keshet, Leah BA Segel, LA EdelsteinKeshet, L BF Segel, LA EdelsteinKeshet, L TI For further study SO PRIMER ON MATHEMATICAL MODELS IN BIOLOGY LA English DT Article; Book Chapter C1 [Segel, Lee A.] Weizmann Inst Sci, IL-76100 Rehovot, Israel. [Segel, Lee A.] Weizmann Inst Sci, Sci Council, IL-76100 Rehovot, Israel. [Segel, Lee A.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Segel, Lee A.] Amer Assoc Advancement Sci, Washington, DC USA. [Edelstein-Keshet, Leah] Univ British Columbia, Dept Math, Vancouver, BC, Canada. NR 0 TC 0 Z9 0 U1 0 U2 0 PU SIAM PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA BN 978-1-611972-49-8 PY 2013 BP 311 EP 336 D2 10.1137/1.9781611972504 PG 26 WC Mathematics, Applied SC Mathematics GA BFG45 UT WOS:000319780100014 ER PT B AU Segel, LA Edelstein-Keshet, L AF Segel, Lee A. Edelstein-Keshet, Leah BA Segel, LA EdelsteinKeshet, L BF Segel, LA EdelsteinKeshet, L TI Extended exercises and projects SO PRIMER ON MATHEMATICAL MODELS IN BIOLOGY LA English DT Article; Book Chapter C1 [Segel, Lee A.] Weizmann Inst Sci, IL-76100 Rehovot, Israel. [Segel, Lee A.] Weizmann Inst Sci, Sci Council, IL-76100 Rehovot, Israel. [Segel, Lee A.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Segel, Lee A.] Amer Assoc Advancement Sci, Washington, DC USA. [Edelstein-Keshet, Leah] Univ British Columbia, Dept Math, Vancouver, BC, Canada. NR 0 TC 0 Z9 0 U1 0 U2 0 PU SIAM PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA BN 978-1-611972-49-8 PY 2013 BP 337 EP 353 D2 10.1137/1.9781611972504 PG 17 WC Mathematics, Applied SC Mathematics GA BFG45 UT WOS:000319780100015 ER PT B AU Segel, LA Edelstein-Keshet, L AF Segel, Lee A. Edelstein-Keshet, Leah BA Segel, LA EdelsteinKeshet, L BF Segel, LA EdelsteinKeshet, L TI The Taylor approximation and Taylor series SO PRIMER ON MATHEMATICAL MODELS IN BIOLOGY LA English DT Article; Book Chapter C1 [Segel, Lee A.] Weizmann Inst Sci, IL-76100 Rehovot, Israel. [Segel, Lee A.] Weizmann Inst Sci, Sci Council, IL-76100 Rehovot, Israel. [Segel, Lee A.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Segel, Lee A.] Amer Assoc Advancement Sci, Washington, DC USA. [Edelstein-Keshet, Leah] Univ British Columbia, Dept Math, Vancouver, BC, Canada. NR 0 TC 0 Z9 0 U1 0 U2 0 PU SIAM PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA BN 978-1-611972-49-8 PY 2013 BP 355 EP 362 D2 10.1137/1.9781611972504 PG 8 WC Mathematics, Applied SC Mathematics GA BFG45 UT WOS:000319780100016 ER PT B AU Segel, LA Edelstein-Keshet, L AF Segel, Lee A. Edelstein-Keshet, Leah BA Segel, LA EdelsteinKeshet, L BF Segel, LA EdelsteinKeshet, L TI Complex numbers SO PRIMER ON MATHEMATICAL MODELS IN BIOLOGY LA English DT Article; Book Chapter C1 [Segel, Lee A.] Weizmann Inst Sci, IL-76100 Rehovot, Israel. [Segel, Lee A.] Weizmann Inst Sci, Sci Council, IL-76100 Rehovot, Israel. [Segel, Lee A.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Segel, Lee A.] Amer Assoc Advancement Sci, Washington, DC USA. [Edelstein-Keshet, Leah] Univ British Columbia, Dept Math, Vancouver, BC, Canada. NR 0 TC 0 Z9 0 U1 0 U2 0 PU SIAM PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA BN 978-1-611972-49-8 PY 2013 BP 363 EP 366 D2 10.1137/1.9781611972504 PG 4 WC Mathematics, Applied SC Mathematics GA BFG45 UT WOS:000319780100017 ER PT B AU Segel, LA Edelstein-Keshet, L AF Segel, Lee A. Edelstein-Keshet, Leah BA Segel, LA EdelsteinKeshet, L BF Segel, LA EdelsteinKeshet, L TI A review of basic theory of electricity SO PRIMER ON MATHEMATICAL MODELS IN BIOLOGY LA English DT Article; Book Chapter C1 [Segel, Lee A.] Weizmann Inst Sci, IL-76100 Rehovot, Israel. [Segel, Lee A.] Weizmann Inst Sci, Sci Council, IL-76100 Rehovot, Israel. [Segel, Lee A.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Segel, Lee A.] Amer Assoc Advancement Sci, Washington, DC USA. [Edelstein-Keshet, Leah] Univ British Columbia, Dept Math, Vancouver, BC, Canada. NR 0 TC 0 Z9 0 U1 0 U2 0 PU SIAM PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA BN 978-1-611972-49-8 PY 2013 BP 367 EP 377 D2 10.1137/1.9781611972504 PG 11 WC Mathematics, Applied SC Mathematics GA BFG45 UT WOS:000319780100018 ER PT B AU Segel, LA Edelstein-Keshet, L AF Segel, Lee A. Edelstein-Keshet, Leah BA Segel, LA EdelsteinKeshet, L BF Segel, LA EdelsteinKeshet, L TI Proofs of Boolean algebra rules SO PRIMER ON MATHEMATICAL MODELS IN BIOLOGY LA English DT Article; Book Chapter C1 [Segel, Lee A.] Weizmann Inst Sci, IL-76100 Rehovot, Israel. [Segel, Lee A.] Weizmann Inst Sci, Sci Council, IL-76100 Rehovot, Israel. [Segel, Lee A.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Segel, Lee A.] Amer Assoc Advancement Sci, Washington, DC USA. [Edelstein-Keshet, Leah] Univ British Columbia, Dept Math, Vancouver, BC, Canada. NR 0 TC 0 Z9 0 U1 0 U2 0 PU SIAM PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA BN 978-1-611972-49-8 PY 2013 BP 379 EP 383 D2 10.1137/1.9781611972504 PG 5 WC Mathematics, Applied SC Mathematics GA BFG45 UT WOS:000319780100019 ER PT B AU Segel, LA Edelstein-Keshet, L AF Segel, Lee A. Edelstein-Keshet, Leah BA Segel, LA EdelsteinKeshet, L BF Segel, LA EdelsteinKeshet, L TI XPP files for models in this book SO PRIMER ON MATHEMATICAL MODELS IN BIOLOGY LA English DT Article; Book Chapter C1 [Segel, Lee A.] Weizmann Inst Sci, IL-76100 Rehovot, Israel. [Segel, Lee A.] Weizmann Inst Sci, Sci Council, IL-76100 Rehovot, Israel. [Segel, Lee A.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Segel, Lee A.] Amer Assoc Advancement Sci, Washington, DC USA. [Edelstein-Keshet, Leah] Univ British Columbia, Dept Math, Vancouver, BC, Canada. NR 0 TC 0 Z9 0 U1 0 U2 0 PU SIAM PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA BN 978-1-611972-49-8 PY 2013 BP 385 EP 403 D2 10.1137/1.9781611972504 PG 19 WC Mathematics, Applied SC Mathematics GA BFG45 UT WOS:000319780100020 ER PT J AU Nikl, M Yoshikawa, A Kamada, K Nejezchleb, K Stanek, CR Mares, JA Blazek, K AF Nikl, M. Yoshikawa, A. Kamada, K. Nejezchleb, K. Stanek, C. R. Mares, J. A. Blazek, K. TI Development of LuAG-based scintillator crystals - A review SO PROGRESS IN CRYSTAL GROWTH AND CHARACTERIZATION OF MATERIALS LA English DT Review ID CHARGE-TRANSFER LUMINESCENCE; LU3AL5O12 SINGLE-CRYSTALS; EMISSION MAMMOGRAPHY PEM; BAND-GAP SCINTILLATORS; GAMMA-RAY DETECTION; PULLING-DOWN METHOD; GARNET CRYSTALS; YAG-CE; CZOCHRALSKI GROWTH; ENERGY-TRANSFER AB A review of research and development of Lu3Al5O12 (LuAG)-based single crystal scintillators is presented. Crystals of this type have been prepared by the micro-pulling down method at the initial stage of material screening and by Czochralski or Bridgman methods to obtain higher quality and larger size single crystals afterward. Several different activators, namely Ce3+, Pr3+, Yb3+ and Sc3+ have been reported in the literature and such doped LuAG single crystals have been extensively studied to understand a number of issues, including: the scintillation mechanism, underlying energy transfer and trapping processes including the nature and role of material defects involved in the scintillation process and their relation to manufacturing technology. Significant improvements in the understanding of aluminum garnet scintillators lead to the discovery of multicomponent garnet single crystal scintillators in 2011, which are described. These materials gave rise to new class of ultraefficient complex oxide scintillators, the light yield of which considerably exceeds the values achieved for the best Ce-doped orthosilicate scintillators. (C) 2013 Elsevier Ltd. All rights reserved. C1 [Nikl, M.; Mares, J. A.] Inst Phys AS CR, Prague, Czech Republic. [Yoshikawa, A.] Tohoku Univ, Inst Mat Res, Sendai, Miyagi, Japan. [Kamada, K.] Furukawa Co Ltd, Mat Res Lab, Tsukuba, Ibaraki, Japan. [Nejezchleb, K.; Blazek, K.] CRYTUR Spol Sro, Turnov, Czech Republic. [Stanek, C. R.] Los Alamos Natl Lab, Div Mat Sci & Technol, Los Alamos, NM 87545 USA. [Yoshikawa, A.; Kamada, K.] Tohoku Univ, New Ind Creat Hatchery Ctr, Sendai, Miyagi 980, Japan. RP Yoshikawa, A (reprint author), Tohoku Univ, Inst Mat Res, Sendai, Miyagi, Japan. EM yoshikawa@imr.tohoku.ac.jp RI Yoshikawa, Akira/B-9986-2011 FU Czech Science Foundation [P204/12/0805]; Japan society for promotion of science (JSPS); [GAAV KAN300100802]; [AV M100100910] FX This research and article preparation was supported by Czech GAAV KAN300100802, AV M100100910 and Czech Science Foundation P204/12/0805 projects. This work was partially supported by the funding program for next generation world-leading researchers, Japan society for promotion of science (JSPS). J. Tous is acknowledged for providing us photographs for Figs. 2 and 22, W. Chewpraditkul for providing the data for Fig. 6(B). NR 108 TC 69 Z9 73 U1 11 U2 135 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0960-8974 J9 PROG CRYST GROWTH CH JI Prog. Cryst. Growth Charact. Mater. PY 2013 VL 59 IS 2 BP 47 EP 72 DI 10.1016/j.pcrysgrow.2013.02.001 PG 26 WC Crystallography; Materials Science, Characterization & Testing SC Crystallography; Materials Science GA 160VF UT WOS:000320147900001 ER PT J AU Kaya, Y Piepel, GF Caniyilmaz, E AF Kaya, Yahya Piepel, Greg F. Caniyilmaz, Erdal TI Development of a Rubber-Based Product Using a Mixture Experiment: A Challenging Case Study SO PROGRESS IN RUBBER PLASTICS AND RECYCLING TECHNOLOGY LA English DT Article DE Rubber formulation; Product development; Experimental design; Mixture experiment; Mixture models; Optimization AB Many products used in daily life are made by blending two or more components. The properties of such products typically depend on the relative proportions of the components. Experimental design, modeling, and data analysis methods for mixture experiments provide for efficiently determining the component proportions that will yield a product with desired properties. This article presents a case study of the work performed to develop a new rubber formulation for an o-ring (a circular gasket) with requirements specified on 10 product properties. Each step of the study is discussed, including: 1) identifying the objective of the study and requirements for properties of the o-ring, 2) selecting the components to vary and specifying the component constraints, 3) constructing a mixture experiment design, 4) measuring the responses and assessing the data, 5) developing property-composition models, 6) selecting the new product formulation, and 7) confirming the selected formulation in manufacturing. The case study includes some challenging and new aspects, which are discussed in the article. C1 [Kaya, Yahya] Erciyes Univ, Dept Mech Engn, TR-38039 Kayseri, Turkey. [Piepel, Greg F.] Pacific NW Natl Lab, Richland, WA 99354 USA. [Caniyilmaz, Erdal] Erciyes Univ, Dept Ind Engn, TR-38039 Kayseri, Turkey. RP Kaya, Y (reprint author), Erciyes Univ, Dept Mech Engn, TR-38039 Kayseri, Turkey. EM kayayahya@gmail.com NR 17 TC 0 Z9 0 U1 1 U2 5 PU ISMITHERS-IRAPRA TECHNOLOGY LTD PI SHREWSBURY PA SHAWBURY, SHREWSBURY SY4 4NR, SHROPS, ENGLAND SN 1477-7606 J9 PROG RUBBER PLAST RE JI Prog. Rubber Plast. Recycl. Technol. PY 2013 VL 29 IS 3 BP 123 EP 149 PG 27 WC Materials Science, Composites; Polymer Science SC Materials Science; Polymer Science GA 157JX UT WOS:000319893500001 ER PT S AU Nguyen, BM Liu, Y Tang, W Picraux, ST Dayeh, SA AF Binh-Minh Nguyen Liu, Yang Tang, Wei Picraux, S. T. Dayeh, Shadi A. BE Razeghi, M Tournie, E Brown, GJ TI Ultra-short channel field effect transistors based on Ge/Si core/shell nanowires SO QUANTUM SENSING AND NANOPHOTONIC DEVICES X SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Quantum Sensing and Nanophotonic Devices X CY FEB 03-07, 2013 CL San Francisco, CA SP SPIE DE nanowires; Ge/Si core/shell; field effect transistor; ultra-short channel ID HETEROSTRUCTURES AB In recent years, transistor technology has scaled down to sub-20 nm channel length with many performance-boosting techniques at the material and device levels in order to meet the increasing demand for higher performance electronics. The nanowire (NW) device architecture has proven itself as a viable candidate for the sub-20 nm generation transistors. Compared to Si NWs, the Ge/Si core/shell NW alternative can supply larger on-current due to the increased confined hole mobility and ohmic behavior at the Ni-alloyed drain/source contacts. It is thus important to understand transport mechanisms in this core/shell structure, and develop pathway to realize ultra-short channel core/shell NW field effect transistors (FETs). In this paper, we report the growth of Ge/Si concentric NWs with precise control of Si shell thickness. Performance of FETs fabricated from core/shell NWs exhibited a clear dependence on NWs' diameters, with steeper sub-threshold slopes for smaller NWs. An 18 nm diameter Ge/Si heterostructure FET exhibited sub-threshold swing of 102 mV/decade, with a maximum transconductance of 3.4 mu S at V-DS =-100 mV. Finally, transmission electron microscopy was utilized to monitor and control the solid state reaction between Ni contacts and Ge/Si NWs, resulting in ultra-scaled channel lengths, as short as 5 nm. C1 [Binh-Minh Nguyen; Picraux, S. T.; Dayeh, Shadi A.] Los Alamos Natl Lab, Ctr Integrated Nanotechnol, Los Alamos, NM 87545 USA. RP Nguyen, BM (reprint author), Los Alamos Natl Lab, Ctr Integrated Nanotechnol, POB 1663, Los Alamos, NM 87545 USA. EM minh@lanl.gov; sdayeh@ece.ucsd.edu RI Tang, Wei/A-6917-2015 OI Tang, Wei/0000-0001-6113-7201 NR 9 TC 0 Z9 0 U1 0 U2 6 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9400-9 J9 PROC SPIE PY 2013 VL 8631 AR UNSP 863118 DI 10.1117/12.2008676 PG 10 WC Nanoscience & Nanotechnology; Optics; Spectroscopy SC Science & Technology - Other Topics; Optics; Spectroscopy GA BFG30 UT WOS:000319759100024 ER PT S AU Craig, IM Phillips, MC Taubman, MS Josberger, EE Raschke, MB AF Craig, Ian M. Phillips, Mark C. Taubman, Matthew S. Josberger, Erik E. Raschke, Markus B. BE Razeghi, M Tournie, E Brown, GJ TI Infrared scattering scanning near-field optical microscopy using an external cavity quantum cascade laser for nanoscale chemical imaging and spectroscopy of explosive residues SO QUANTUM SENSING AND NANOPHOTONIC DEVICES X SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Quantum Sensing and Nanophotonic Devices X CY FEB 03-07, 2013 CL San Francisco, CA SP SPIE DE s-SNOM; AFM; ECQCL; chemical imaging; infrared; nano-spectroscopy; tetryl ID ELASTIC LIGHT-SCATTERING; ABSORPTION-SPECTROSCOPY; TIP AB Infrared scattering scanning near-field optical microscopy (s-SNOM) is an apertureless superfocusing technique that uses the antenna properties of a conducting atomic force microscope (AFM) tip to achieve infrared spatial resolution below the diffraction limit. The instrument can be used either in imaging mode, where a fixed wavelength light source is tuned to a molecular resonance and the AFM raster scans an image, or in spectroscopy mode where the AFM is held stationary over a feature of interest and the light frequency is varied to obtain a spectrum. In either case, a strong, stable, coherent infrared source is required. Here we demonstrate the integration of a broadly tunable external cavity quantum cascade laser (ECQCL) into an s-SNOM and use it to obtain infrared spectra of microcrystals of chemicals adsorbed onto gold substrates. Residues of the explosive compound tetryl was deposited onto gold substrates. s-SNOM experiments were performed in the 1260-1400 cm(-1) tuning range of the ECQCL, corresponding to the NO2 symmetric stretch vibrational fingerprint region. Vibrational infrared spectra were collected on individual chemical domains with a collection area of similar to 500 nm(2) and compared to ensemble averaged far-field reflection-absorption infrared spectroscopy (RAIRS) results. C1 [Craig, Ian M.; Phillips, Mark C.; Taubman, Matthew S.] Pacific NW Natl Lab, EMSL, Richland, WA 99352 USA. RP Craig, IM (reprint author), Pacific NW Natl Lab, EMSL, 902 Battelle Blvd, Richland, WA 99352 USA. RI Craig, Ian/C-3799-2009; Razeghi, Manijeh/B-7265-2009; Raschke, Markus/F-8023-2013 OI Craig, Ian/0000-0003-4481-3700; NR 26 TC 2 Z9 2 U1 0 U2 16 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9400-9 J9 PROC SPIE PY 2013 VL 8631 AR UNSP 863110 DI 10.1117/12.2004954 PG 8 WC Nanoscience & Nanotechnology; Optics; Spectroscopy SC Science & Technology - Other Topics; Optics; Spectroscopy GA BFG30 UT WOS:000319759100019 ER PT S AU Phillips, MC Craig, IM Blake, TA AF Phillips, Mark C. Craig, Ian M. Blake, Thomas A. BE Razeghi, M Tournie, E Brown, GJ TI Reflection-absorption infrared spectroscopy of thin films using an external cavity quantum cascade laser SO QUANTUM SENSING AND NANOPHOTONIC DEVICES X SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Quantum Sensing and Nanophotonic Devices X CY FEB 03-07, 2013 CL San Francisco, CA SP SPIE DE Infrared spectroscopy; quantum cascade laser; tunable laser; explosives detection; complex refractive index ID METAL-SURFACES; MOLECULES AB We present experimental demonstrations using a broadly tunable external cavity quantum cascade laser (ECQCL) to perform Reflection-Absorption InfraRed Spectroscopy (RAIRS) of thin layers and residues on surfaces. The ECQCL compliance voltage was used to measure fluctuations in the ECQCL output power and improve the performance of the RAIRS measurements. Absorption spectra from self-assembled monolayers of a fluorinated alkane thiol and a thiol carboxylic acid were measured and compared with FTIR measurements. RAIRS spectra of the explosive compounds PETN, RDX, and tetryl deposited on gold substrates were also measured. Rapid measurement times and low noise were demonstrated, with <1E-3 absorbance noise for a 10 second measurement time. C1 [Phillips, Mark C.; Craig, Ian M.; Blake, Thomas A.] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Phillips, MC (reprint author), Pacific NW Natl Lab, POB 999, Richland, WA 99352 USA. RI Craig, Ian/C-3799-2009; Razeghi, Manijeh/B-7265-2009 OI Craig, Ian/0000-0003-4481-3700; NR 13 TC 2 Z9 2 U1 1 U2 8 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-0-8194-9400-9 J9 PROC SPIE PY 2013 VL 8631 AR UNSP 86310C DI 10.1117/12.2002849 PG 13 WC Nanoscience & Nanotechnology; Optics; Spectroscopy SC Science & Technology - Other Topics; Optics; Spectroscopy GA BFG30 UT WOS:000319759100005 ER PT J AU Li, C Guo, XJ He, YX Jiang, Z Wang, YX Chen, SM Fu, HY Zou, Y Dai, S Wu, GZ Xu, HJ AF Li, Cheng Guo, Xiaojing He, Yaxing Jiang, Zheng Wang, Yaxing Chen, Shimou Fu, Haiying Zou, Yang Dai, Sheng Wu, Guozhong Xu, Hongjie TI Compression of ionic liquid when confined in porous silica nanoparticles SO RSC ADVANCES LA English DT Article ID CARBON NANOTUBES; MELTING-POINT; MOLECULAR-DYNAMICS; SIMULATION; REACTIVITY; EXAFS; WATER AB [Emim]Br ionic liquid was confined in porous SiO2 nanoparticles. It is shown that the confinement in the nanopores leads to a compression of molecular size and an increase in the melting point. The pore size of SiO2 is a key factor in tuning the anion-cation distance and the melting point of the confined ionic liquids. C1 [Li, Cheng; Guo, Xiaojing; He, Yaxing; Jiang, Zheng; Wang, Yaxing; Fu, Haiying; Zou, Yang; Wu, Guozhong; Xu, Hongjie] Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai 201800, Peoples R China. [Chen, Shimou] Chinese Acad Sci, Inst Proc Engn, Beijing 100190, Peoples R China. [Dai, Sheng] Oak Ridge Natl Lab, Chem Sci Div, Oak Ridge, TN USA. RP Li, C (reprint author), Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai 201800, Peoples R China. EM wuguozhong@sinap.ac.cn RI Chen, Shimou/G-4451-2010; Dai, Sheng/K-8411-2015 OI Dai, Sheng/0000-0002-8046-3931 FU National Natural Science Foundation of China [11079007, 11005148, 20973192, 10705046]; Basic Energy Sciences, U.S. Department of Energy FX This work was supported by the National Natural Science Foundation of China No. 11079007, 11005148, 20973192 and 10705046. XAFS analysis was carried out at beamline BL14W1 (Shanghai Synchrotron Radiation Facility). SD was supported by the Basic Energy Sciences, U.S. Department of Energy. NR 26 TC 11 Z9 11 U1 7 U2 79 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2046-2069 J9 RSC ADV JI RSC Adv. PY 2013 VL 3 IS 25 BP 9618 EP 9621 DI 10.1039/c3ra40245b PG 4 WC Chemistry, Multidisciplinary SC Chemistry GA 158BE UT WOS:000319942700004 ER PT J AU Yang, X Chang, ASP Chen, B Gu, C Bond, TC AF Yang, Xuan Chang, Allan S. P. Chen, Bin Gu, Claire Bond, Tiziana C. TI High sensitivity gas sensing by Raman spectroscopy in photonic crystal fiber SO SENSORS AND ACTUATORS B-CHEMICAL LA English DT Article DE Fiber sensor; Photonic crystal fiber; Raman spectroscopy; Gas sensing ID SCATTERING; AIR AB We report the highly sensitive Raman detection of various gases (ambient nitrogen, oxygen, and carbon dioxide) and vapors (toluene, acetone, and 1,1,1-trichloroethane) using a hollow core photonic crystal fiber probe. With a sensitivity enhancement of around 3 orders of magnitude over direct detection, the minimum instrumentation-limited detectable concentrations for toluene, acetone, 1,1,1-trichloroethane vapors are 0.04%, 0.01%, 1.2%, respectively, with a 30 cm-long fiber probe. Moreover, we demonstrate its multiplexed sensing capability quantitatively using a vapor mixture. This combination of Raman spectroscopy and photonic crystal fiber provides a promising platform for gas sensing in environmental control applications. (C) 2012 Elsevier B.V. All rights reserved. C1 [Yang, Xuan; Chang, Allan S. P.; Bond, Tiziana C.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. [Yang, Xuan; Chen, Bin; Gu, Claire] Univ Calif Santa Cruz, Dept Elect Engn, Santa Cruz, CA 95064 USA. [Chen, Bin] NASA, Ames Res Ctr, Adv Studies Labs, Moffett Field, CA 94035 USA. RP Gu, C (reprint author), Univ Calif Santa Cruz, Dept Elect Engn, Santa Cruz, CA 95064 USA. EM claire@soe.ucsc.edu; bond7@llnl.gov FU National Science Foundation (NSF) [ECCS-0823921]; Lawrence Scholar Program at LLNL; U.S. Department of Energy by LLNL [DE-AC52-07NA27344, LLNL-JRNL-561331] FX We acknowledge support from the National Science Foundation (NSF), ECCS-0823921. X.Y. acknowledges financial support by the Lawrence Scholar Program at LLNL. This work was performed under the auspices of the U.S. Department of Energy by LLNL under Contract DE-AC52-07NA27344, LLNL-JRNL-561331. NR 19 TC 13 Z9 16 U1 1 U2 49 PU ELSEVIER SCIENCE SA PI LAUSANNE PA PO BOX 564, 1001 LAUSANNE, SWITZERLAND SN 0925-4005 J9 SENSOR ACTUAT B-CHEM JI Sens. Actuator B-Chem. PD JAN PY 2013 VL 176 BP 64 EP 68 DI 10.1016/j.snb.2012.09.004 PG 5 WC Chemistry, Analytical; Electrochemistry; Instruments & Instrumentation SC Chemistry; Electrochemistry; Instruments & Instrumentation GA 157AM UT WOS:000319867500010 ER PT J AU Shin, D Besmann, TM Armstrong, BL AF Shin, Dongwon Besmann, Theodore M. Armstrong, Beth L. TI Phase stability of noble metal loaded WO3 for SO2 sensor applications SO SENSORS AND ACTUATORS B-CHEMICAL LA English DT Article DE SO2; Semiconductor gas sensor; WO3; Ag/WO3; Thermodynamics; CALPHAD ID GAS SENSORS; SENSING PROPERTIES; THIN-FILMS; TIO2 AB A thermodynamic phase stability investigation of semiconductor oxide materials for SO2 gas sensing applications has been performed to provide insight into understanding the working principles for SO2 sensing. Complex phase stabilities of noble metals (Au, Ag, Pd, and Pt) loaded WO3 semiconductor oxides for SO2 sensors have been investigated through the use of the CALPHAD (CALculation of PHAse Diagram) computational thermodynamics approach. Thermodynamic descriptions for the individual phases, i.e. SO2 gas, oxides, sulfides, and metal sulfates, are obtained from the Scientific Group Thermodata Europe (SGTE) Substance Database. Calculated isothermal sections of W-S-O show a significant phase transformation for WS2 at 400 degrees C. This phase transformation agrees with the previously reported experimental findings that the SO2 response of WO3 increases notably at that temperature. Ag-loaded WO3 in equilibrium with the SO2 gas exhibits very complex phase stabilities for the binary sulfide and ternary sulfate, while the other metals (Au, Pd and Pt) did not exhibit any notable phase transformations. The thermodynamic model predicts an allotropic phase transformation of the Ag2S phase near 500 degrees C in Ag/WO3-SO2 regardless of the Ag content, which differs from the reported experimental observation that 1.0 wt% Ag/WO3 exhibited SO2 sensor response at 450 degrees C. This discrepancy may be attributed to the fact that the solubility of Ag in the WO3 phase has not been considered in the thermodynamic model. Published by Elsevier B.V-. C1 [Shin, Dongwon; Besmann, Theodore M.; Armstrong, Beth L.] Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. RP Shin, D (reprint author), Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. EM shind@ornl.gov RI Shin, Dongwon/C-6519-2008; Armstrong, Beth/E-6752-2017 OI Shin, Dongwon/0000-0002-5797-3423; Armstrong, Beth/0000-0001-7149-3576 FU US Department of Energy Office of Fossil Energy, National Energy Technology Laboratory FX The authors would like to thank the Oak Ridge National Laboratory (ORNL) sensor research team, David West, Fred Montgomery, and Dane Wilson, for their helpful discussions. This research was sponsored by the US Department of Energy Office of Fossil Energy, National Energy Technology Laboratory. NR 23 TC 3 Z9 3 U1 6 U2 65 PU ELSEVIER SCIENCE SA PI LAUSANNE PA PO BOX 564, 1001 LAUSANNE, SWITZERLAND SN 0925-4005 J9 SENSOR ACTUAT B-CHEM JI Sens. Actuator B-Chem. PD JAN PY 2013 VL 176 BP 75 EP 80 DI 10.1016/j.snb.2012.08.084 PG 6 WC Chemistry, Analytical; Electrochemistry; Instruments & Instrumentation SC Chemistry; Electrochemistry; Instruments & Instrumentation GA 157AM UT WOS:000319867500012 ER PT S AU Torres, DA De La Rosa, N Cristancho, F Tabor, SL Kaye, RA Solomon, GZ Doring, J Johns, GD Devlin, M Lerma, F Sarantites, DG Lee, IY Macchiavelli, AO Garzon, A AF Torres, D. A. De La Rosa, N. Cristancho, F. Tabor, S. L. Kaye, R. A. Solomon, G. Z. Doering, J. Johns, G. D. Devlin, M. Lerma, F. Sarantites, D. G. Lee, I. -Y. Macchiavelli, A. O. Garzon, A. BE Melquiades, FL Genezini, FA Medina, NH DosAnjos, RM Avancini, SD TI Band termination in normally deformed bands in Y-83 SO XXXV BRAZILIAN WORKSHOP ON NUCLEAR PHYSICS SE AIP Conference Proceedings LA English DT Proceedings Paper CT 35th Brazilian Workshop on Nuclear Physics CY SEP 02-06, 2012 CL Sao Sebastiao, BRAZIL SP Brazilian Phys Soc (SBF), Fundacao Amparo Pesquisa Sao Paulo (FAPESP), Fundacao Amparo Pesquisa Rio de Janeiro (FAPERJ), Conselho Nacl Desenvolvimento Cientifico & Tecnologica, Coordenacao Aperfeicoamento Pessoal Nivel Super, Eletrobras Eletronuclear, SINC Brasil DE Lifetimes; DSAM; Nuclear Deformation AB Lifetimes in the negative parity favored signature have been studied up to the I-pi = 53/2(-) state in the Y-83(39) nucleus. The reaction Ni-58(S-32,alpha 3p) at E-lab - 135 MeV was utilized to populate high-spin states in Y-83. Lifetimes were measured using the Doppler shift attenuation method with the GAMMASPHERE and MICROBALL arrays. The evolution of the transitional quadrupole values are in agreement with a possible band termination. C1 [Torres, D. A.; De La Rosa, N.; Cristancho, F.] Univ Nacl Colombia, Dept Fis, Bogota, Colombia. [Tabor, S. L.; Kaye, R. A.; Solomon, G. Z.] Florida State Univ, Dept Phys, Tallahassee, FL 32306 USA. [Doering, J.] Univ Notre Dame, Dept Phys, Notre Dame, IN 46556 USA. [Johns, G. D.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Devlin, M.; Sarantites, D. G.] Washington Univ, Dept Chem, St Louis, MO 63130 USA. [Lee, I. -Y.; Macchiavelli, A. O.] Lawrence Berkeley Natl Lab, Div Nucl Sci, Berkeley, CA 94720 USA. [Garzon, A.] Univ Sergio Arboleda, Sch Math, Bogota, Colombia. RP Torres, DA (reprint author), Univ Nacl Colombia, Dept Fis, Bogota, Colombia. RI Devlin, Matthew/B-5089-2013 OI Devlin, Matthew/0000-0002-6948-2154 NR 6 TC 0 Z9 0 U1 0 U2 0 PU AMER INST PHYSICS PI MELVILLE PA 2 HUNTINGTON QUADRANGLE, STE 1NO1, MELVILLE, NY 11747-4501 USA SN 0094-243X BN 978-0-7354-1154-8 J9 AIP CONF PROC PY 2013 VL 1529 BP 170 EP 173 DI 10.1063/1.4804112 PG 4 WC Physics, Nuclear SC Physics GA BFG29 UT WOS:000319754400039 ER PT J AU Crease, RP AF Crease, Robert P. TI Identity physics SO PHYSICS WORLD LA English DT Editorial Material C1 [Crease, Robert P.] SUNY Stony Brook, Dept Philosophy, Stony Brook, NY 11794 USA. [Crease, Robert P.] Brookhaven Natl Lab, Upton, NY 11973 USA. RP Crease, RP (reprint author), SUNY Stony Brook, Dept Philosophy, Stony Brook, NY 11794 USA. EM rcrease@notes.cc.sunysb.edu NR 0 TC 0 Z9 0 U1 0 U2 0 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 0953-8585 J9 PHYS WORLD JI Phys. World PD JAN PY 2013 VL 26 IS 1 BP 19 EP 19 PG 1 WC Physics, Multidisciplinary SC Physics GA 074UO UT WOS:000313839700018 ER PT J AU Bowman, KW Shindell, DT Worden, HM Lamarque, JF Young, PJ Stevenson, DS Qu, Z de la Torre, M Bergmann, D Cameron-Smith, PJ Collins, WJ Doherty, R Dalsoren, SB Faluvegi, G Folberth, G Horowitz, LW Josse, BM Lee, YH MacKenzie, IA Myhre, G Nagashima, T Naik, V Plummer, DA Rumbold, ST Skeie, RB Strode, SA Sudo, K Szopa, S Voulgarakis, A Zeng, G Kulawik, SS Aghedo, AM Worden, JR AF Bowman, K. W. Shindell, D. T. Worden, H. M. Lamarque, J. F. Young, P. J. Stevenson, D. S. Qu, Z. de la Torre, M. Bergmann, D. Cameron-Smith, P. J. Collins, W. J. Doherty, R. Dalsoren, S. B. Faluvegi, G. Folberth, G. Horowitz, L. W. Josse, B. M. Lee, Y. H. MacKenzie, I. A. Myhre, G. Nagashima, T. Naik, V. Plummer, D. A. Rumbold, S. T. Skeie, R. B. Strode, S. A. Sudo, K. Szopa, S. Voulgarakis, A. Zeng, G. Kulawik, S. S. Aghedo, A. M. Worden, J. R. TI Evaluation of ACCMIP outgoing longwave radiation from tropospheric ozone using TES satellite observations SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID INTERCOMPARISON PROJECT ACCMIP; BIOMASS BURNING EMISSIONS; CHEMISTRY-CLIMATE MODELS; ATMOSPHERIC CHEMISTRY; TROPICAL TROPOSPHERE; PREINDUSTRIAL TIMES; NADIR RETRIEVALS; SOUTHERN AFRICA; ZONAL STRUCTURE; CARBON-DIOXIDE AB We use simultaneous observations of tropospheric ozone and outgoing longwave radiation (OLR) sensitivity to tropospheric ozone from the Tropospheric Emission Spectrometer (TES) to evaluate model tropospheric ozone and its effect on OLR simulated by a suite of chemistry-climate models that participated in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The ensemble mean of ACCMIP models show a persistent but modest tropospheric ozone low bias (5-20 ppb) in the Southern Hemisphere (SH) and modest high bias (5-10 ppb) in the Northern Hemisphere (NH) relative to TES ozone for 2005-2010. These ozone biases have a significant impact on the OLR. Using TES instantaneous radiative kernels (IRK), we show that the ACCMIP ensemble mean tropospheric ozone low bias leads up to 120 mW m(-2) OLR high bias locally but zonally compensating errors reduce the global OLR high bias to 39 +/- 41 mW m(-2) relative to TES data. We show that there is a correlation (R-2 = 0.59) between the magnitude of the ACCMIP OLR bias and the deviation of the ACCMIP preindustrial to present day (1750-2010) ozone radiative forcing (RF) from the ensemble ozone RF mean. However, this correlation is driven primarily by models whose absolute OLR bias from tropospheric ozone exceeds 100 mW m(-2). Removing these models leads to a mean ozone radiative forcing of 394 +/- 42 mW m(-2). The mean is about the same and the standard deviation is about 30% lower than an ensemble ozone RF of 384 +/- 60 mW m(-2) derived from 14 of the 16 ACCMIP models reported in a companion ACCMIP study. These results point towards a profitable direction of combining satellite observations and chemistry-climate model simulations to reduce uncertainty in ozone radiative forcing. C1 [Bowman, K. W.; de la Torre, M.; Kulawik, S. S.; Worden, J. R.] CALTECH, Jet Prop Lab, Pasadena, CA 91125 USA. [Shindell, D. T.; Faluvegi, G.; Lee, Y. H.] NASA, Goddard Inst Space Studies, New York, NY 10025 USA. [Shindell, D. T.; Faluvegi, G.; Lee, Y. H.] Columbia Earth Inst, New York, NY USA. [Worden, H. M.; Lamarque, J. F.] Natl Ctr Atmospher Res, Boulder, CO 80307 USA. [Young, P. J.] Univ Lancaster, Lancaster Environm Ctr, Lancaster, England. [Stevenson, D. S.; Doherty, R.; MacKenzie, I. A.] Univ Edinburgh, Sch Geosci, Edinburgh, Midlothian, Scotland. [Qu, Z.] Raytheon Intelligence & Informat Syst, Pasadena, CA USA. [Bergmann, D.; Cameron-Smith, P. J.] Lawrence Livermore Natl Lab, Livermore, CA USA. [Collins, W. J.] Univ Reading, Dept Meteorol, Reading, Berks, England. [Dalsoren, S. B.; Myhre, G.; Skeie, R. B.] Ctr Int Climate & Environm Res, Oslo, Norway. [Folberth, G.; Rumbold, S. T.] Hadley Ctr, Met Off, Exeter, Devon, England. [Horowitz, L. W.] NOAA, Geophys Fluid Dynam Lab, Princeton, NJ USA. [Josse, B. M.] CNRS, GAME CNRM, Meteo France, Ctr Natl Rech Meteorol, Toulouse, France. [Nagashima, T.] Natl Inst Environm Studies, Tsukuba, Ibaraki, Japan. [Sudo, K.] Nagoya Univ, Grad Sch Environm Studies, Nagoya, Aichi 4648601, Japan. [Naik, V.] NOAA, UCAR, Geophys Fluid Dynam Lab, Princeton, NJ USA. [Plummer, D. A.] Environm Canada, Canadian Ctr Climate Modeling & Anal, Victoria, BC, Canada. [Strode, S. A.] NASA, Goddard Space Flight Ctr, Columbia, MD USA. [Strode, S. A.] Univ Space Res Assoc, Columbia, MD 90034 USA. [Szopa, S.] Lab Sci Climat & Environm, Gif Sur Yvette, France. [Zeng, G.] Natl Inst Water & Atmospher Res, Lauder, New Zealand. [Voulgarakis, A.] Univ London Imperial Coll Sci Technol & Med, Dept Phys, London, England. [Aghedo, A. M.] Rice Univ, Houston, TX USA. RP Bowman, KW (reprint author), CALTECH, Jet Prop Lab, Pasadena, CA 91125 USA. EM kevin.bowman@jpl.nasa.gov RI Lee, Yunha/Q-7222-2016; Strode, Sarah/H-2248-2012; Manager, CSD Publications/B-2789-2015; Young, Paul/E-8739-2010; Lamarque, Jean-Francois/L-2313-2014; Myhre, Gunnar/A-3598-2008; Skeie, Ragnhild/K-1173-2015; Collins, William/A-5895-2010; Stevenson, David/C-8089-2012; Cameron-Smith, Philip/E-2468-2011; Szopa, Sophie/F-8984-2010; Shindell, Drew/D-4636-2012; Horowitz, Larry/D-8048-2014; Bergmann, Daniel/F-9801-2011; Naik, Vaishali/A-4938-2013 OI Lee, Yunha/0000-0001-7478-2672; Strode, Sarah/0000-0002-8103-1663; Young, Paul/0000-0002-5608-8887; Lamarque, Jean-Francois/0000-0002-4225-5074; Myhre, Gunnar/0000-0002-4309-476X; Skeie, Ragnhild/0000-0003-1246-4446; Collins, William/0000-0002-7419-0850; Stevenson, David/0000-0002-4745-5673; Cameron-Smith, Philip/0000-0002-8802-8627; Szopa, Sophie/0000-0002-8641-1737; Horowitz, Larry/0000-0002-5886-3314; Bergmann, Daniel/0000-0003-4357-6301; Naik, Vaishali/0000-0002-2254-1700 FU NASA; National Science Foundation; NASA Aura ROSES program; International Global Atmospheric Chemistry (IGAC) and Stratospheric Processes And their Role in Climate (SPARC) under the International Geosphere-Biosphere Project (IGBP); World Climate Research Program (WCRP); Office of Science (BER) of the US Department of Energy; New Zealand Ministry of Science and Innovation; US Dept. of Energy (BER) under LLNL [DE-AC52-07NA27344, DE-AC02-05CH11231]; US Department of Energy Office of Science Decadal and Regional Climate Prediction using Earth System Models (EaSM) program; DOE [DE-AC06-76RLO 1830]; DECC [GA01101]; Defra Integrated Climate Programme [GA01101]; NASA Modeling, Analysis and Prediction program; Environment Research and Technology Development Fund of the Ministry of the Environment, Japan [S-7]; cross UK research council [NE/I008063/1]; NASA MAP program; NASA ACMAP program FX This research was carried out at the Jet Propulsion Laboratory, California Institute of Technology, under a contract with NASA. The TES monthly ozone and IRK dataset was developed using techniques from the obs4MIP activity (http://obs4mips.llnl.gov:8080/wiki/); The National Center for Atmospheric Research (NCAR) is sponsored by the National Science Foundation.; KB and HW acknowledges the support of the NASA Aura ROSES program. KB also acknowledges some useful codes from Adetutu Aghedo and Rachel Hodos in the initial processing of TES data to netcdf files.; ACCMIP is organized under the auspices of Atmospheric Chemistry and Climate (AC&C), a project of International Global Atmospheric Chemistry (IGAC) and Stratospheric Processes And their Role in Climate (SPARC) under the International Geosphere-Biosphere Project (IGBP) and World Climate Research Program (WCRP).; The CESM project is supported by the National Science Foundation and the Office of Science (BER) of the US Department of Energy.; GZ acknowledges NIWA HPCF facility and funding from New Zealand Ministry of Science and Innovation.; The work of DB and PC was funded by the US Dept. of Energy (BER), performed under the auspices of LLNL under Contract DE-AC52-07NA27344, and used the supercomputing resources of NERSC under contract No. DE-AC02-05CH11231.; Ghan was supported by the US Department of Energy Office of Science Decadal and Regional Climate Prediction using Earth System Models (EaSM) program. The Pacific Northwest National Laboratory (PNNL) is operated for the DOE by Battelle Memorial Institute under contract DE-AC06-76RLO 1830.; W. J. Collins, G. A. Folberth, F. O'Connor and S. T. Rumbold were supported by the Joint DECC and Defra Integrated Climate Programme (GA01101).; The GEOSCCM work was supported by the NASA Modeling, Analysis and Prediction program, with computing resources provided by NASA's High-End Computing Program through the NASA Advanced Supercomputing Division.; The MIROC-CHEM calculations were performed on the NIES supercomputer system (NEC SX-8R), and supported by the Environment Research and Technology Development Fund (S-7) of the Ministry of the Environment, Japan.; The STOC-HadAM3 work was supported by cross UK research council grant NE/I008063/1 and used facilities provided by the UK's national high-performance computing service, HECToR, through Computational Modelling Services (CMS), part of the NERC National Centre for Atmospheric Science (NCAS).; DS and Y. H. Lee acknowledges support from the NASA MAP and ACMAP programs. NR 86 TC 15 Z9 17 U1 2 U2 32 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1680-7316 EI 1680-7324 J9 ATMOS CHEM PHYS JI Atmos. Chem. Phys. PY 2013 VL 13 IS 8 BP 4057 EP 4072 DI 10.5194/acp-13-4057-2013 PG 16 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA 137IF UT WOS:000318428300009 ER PT J AU Li, Z Zang, Z Li, QB Chao, Y Chen, D Ye, Z Liu, Y Liou, KN AF Li, Z. Zang, Z. Li, Q. B. Chao, Y. Chen, D. Ye, Z. Liu, Y. Liou, K. N. TI A three-dimensional variational data assimilation system for multiple aerosol species with WRF/Chem and an application to PM2.5 prediction SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID STATISTICAL-INTERPOLATION; ERROR STATISTICS; MODELING SYSTEM; RETRIEVALS; CHEMISTRY; SMOOTHER; DYNAMICS; MODULE; SCHEME; OZONE AB A three-dimensional variational data assimilation (3-DVAR) algorithm for aerosols in a WRF/Chem model is presented. The WRF/Chem model uses the MOSAIC (Model for Simulating Aerosol Interactions and Chemistry) scheme, which explicitly treats eight major species (elemental/black carbon, organic carbon, nitrate, sulfate, chloride, ammonium, sodium and the sum of other inorganic, inert mineral and metal species) and represents size distributions using a sectional method with four size bins. The 3-DVAR scheme is formulated to take advantage of the MOSAIC scheme in providing comprehensive analyses of species concentrations and size distributions. To treat the large number of state variables associated with the MOSAIC scheme, this 3-DVAR algorithm first determines the analysis increments of the total mass concentrations of the eight species, defined as the sum of the mass concentrations across all size bins, and then distributes the analysis increments over four size bins according to the background error variances. The number concentrations for each size bin are adjusted based on the ratios between the mass and number concentrations of the background state. Additional flexibility is incorporated to further lump the eight mass concentrations, and five lumped species are used in the application presented. The system is evaluated using the analysis and prediction of PM2.5 in the Los Angeles basin during the CalNex 2010 field experiment, with assimilation of surface PM2.5 and speciated concentration observations. The results demonstrate that the data assimilation significantly reduces the errors in comparison with a simulation without data assimilation and improved forecasts of the concentrations of PM2.5 as well as individual species for up to 24 h. Some implementation difficulties and limitations of the system are discussed. C1 [Li, Z.] CALTECH, Jet Prop Lab, Pasadena, CA 91125 USA. [Li, Z.; Zang, Z.; Li, Q. B.; Chao, Y.; Chen, D.; Ye, Z.; Liou, K. N.] Univ Calif Los Angeles, Joint Inst Reg Earth Syst Sci & Engn, Los Angeles, CA USA. [Li, Q. B.; Liou, K. N.] Univ Calif Los Angeles, Dept Atmospher & Ocean Sci, Los Angeles, CA USA. [Liu, Y.] Brookhaven Natl Lab, Upton, NY 11973 USA. [Chao, Y.] Remote Sensing Solut Inc, Pasadena, CA USA. RP Li, Z (reprint author), CALTECH, Jet Prop Lab, Pasadena, CA 91125 USA. EM zhijin.li@jpl.nasa.gov RI Liu, Yangang/H-6154-2011; Chen, Dan/R-4486-2016 FU National Aeronautics and Space Administration (NASA); US Department of Energy Earth System Modelling (ESM) programme via the FASTER project; JPL Director's Research and Development Fund (DRDF); NASA from the Atmospheric Chemistry Modelling and Analysis Programme (ACMAP) [NNX09AF07G, NNX08AF64G] FX The research described in this publication was carried out, in part, at the Jet Propulsion Laboratory (JPL), California Institute of Technology, under a contract with the National Aeronautics and Space Administration (NASA). This research was supported in part by the US Department of Energy Earth System Modelling (ESM) programme via the FASTER project http://www.bnl.gov/faster/, the JPL Director's Research and Development Fund (DRDF), and NASA grants NNX09AF07G and NNX08AF64G from the Atmospheric Chemistry Modelling and Analysis Programme (ACMAP). The careful and constructive reviews by two anonymous referees are highly appreciated. NR 45 TC 11 Z9 12 U1 5 U2 38 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1680-7316 J9 ATMOS CHEM PHYS JI Atmos. Chem. Phys. PY 2013 VL 13 IS 8 BP 4265 EP 4278 DI 10.5194/acp-13-4265-2013 PG 14 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA 137IF UT WOS:000318428300020 ER PT J AU Newman, S Jeong, S Fischer, ML Xu, X Haman, CL Lefer, B Alvarez, S Rappenglueck, B Kort, EA Andrews, AE Peischl, J Gurney, KR Miller, CE Yung, YL AF Newman, S. Jeong, S. Fischer, M. L. Xu, X. Haman, C. L. Lefer, B. Alvarez, S. Rappenglueck, B. Kort, E. A. Andrews, A. E. Peischl, J. Gurney, K. R. Miller, C. E. Yung, Y. L. TI Diurnal tracking of anthropogenic CO2 emissions in the Los Angeles basin megacity during spring 2010 SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID FOSSIL-FUEL CO2; ION-SOURCE DEVELOPMENT; CARBON-DIOXIDE; BOUNDARY-LAYER; ATMOSPHERIC OBSERVATIONS; AIRBORNE MEASUREMENTS; AIR-POLLUTION; GAS EMISSIONS; STILT MODEL; CEILOMETER AB Attributing observed CO2 variations to human or natural cause is critical to deducing and tracking emissions from observations. We have used in situ CO2, CO, and planetary boundary layer height (PBLH) measurements recorded during the CalNex-LA (CARB et al., 2008) ground campaign of 15 May-15 June 2010, in Pasadena, CA, to deduce the diurnally varying anthropogenic component of observed CO2 in the megacity of Los Angeles (LA). This affordable and simple technique, validated by carbon isotope observations and WRF-STILT (Weather Research and Forecasting model - Stochastic Time-Inverted Lagrangian Transport model) predictions, is shown to robustly attribute observed CO2 variation to anthropogenic or biogenic origin over the entire diurnal cycle. During CalNex-LA, local fossil fuel combustion contributed up to similar to 50% of the observed CO2 enhancement overnight, and similar to 100% of the enhancement near midday. This suggests that sufficiently accurate total column CO2 observations recorded near midday, such as those from the GOSAT or OCO-2 satellites, can potentially be used to track anthropogenic emissions from the LA megacity. C1 [Newman, S.; Yung, Y. L.] CALTECH, Div Geol & Planetary Sci, Pasadena, CA 91125 USA. [Jeong, S.; Fischer, M. L.] EO Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. [Xu, X.] Univ Calif Irvine, Dept Earth Syst Sci, Irvine, CA 92697 USA. [Haman, C. L.; Lefer, B.; Alvarez, S.; Rappenglueck, B.] Univ Houston, Dept Earth & Atmospher Sci, Houston, TX 77004 USA. [Kort, E. A.; Miller, C. E.] CALTECH, Jet Prop Lab, Pasadena, CA 91109 USA. [Andrews, A. E.] NOAA ESRL Global Monitoring Div, Boulder, CO 80305 USA. [Peischl, J.] NOAA ESRL Chem Sci Div, Boulder, CO 80305 USA. [Gurney, K. R.] Arizona State Univ, Sch Life Sci, Tempe, AZ 85287 USA. RP Newman, S (reprint author), CALTECH, Div Geol & Planetary Sci, Pasadena, CA 91125 USA. EM sally@gps.caltech.edu RI Peischl, Jeff/E-7454-2010; Kort, Eric/F-9942-2012; Andrews, Arlyn/K-3427-2012; Manager, CSD Publications/B-2789-2015 OI Peischl, Jeff/0000-0002-9320-7101; Kort, Eric/0000-0003-4940-7541; FU JPL's Director's Research and Development Fund; Office of Science, of the US Department of Energy [DE-AC02-05CH11231]; Keck Institute for Space Studies FX We appreciate productive discussions with Paul Wennberg, Debra Wunch, Michael Line, Xi Zhang, Run-Lie Shia, and Joshua Kammer. WRF winds for the time-averaged footprints during the CalNex period were provided by Wayne Angevine of NOAA (Earth System Research Laboratory; ESRL). We thank Paul Novelli and Colm Sweeney of NOAA-ESRL for sharing their data that went into the NOAA background curtain product from which we calculated the time-varying background for CO. John S. Holloway (NOAA ESRL) provided the measurements of CO from the P3 aircraft profiles. As part of the CalNex-LA campaign, we gratefully acknowledge the support of Caltech and the California Air Resources Board in making the campaign successful. TCCON data (version GGG2012) were obtained from the TCCON Data Archive, operated by the California Institute of Technology, from the website at http://tccon.ipac.caltech.edu/. SN acknowledges financial support from JPL's Director's Research and Development Fund. Analysis by MLF and SJ was supported by the Director, Office of Science, of the US Department of Energy under Contract No. DE-AC02-05CH11231. We acknowledge the Keck Institute for Space Studies for financial support of publication costs and contribution by EAK. NR 64 TC 29 Z9 30 U1 2 U2 44 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1680-7316 J9 ATMOS CHEM PHYS JI Atmos. Chem. Phys. PY 2013 VL 13 IS 8 BP 4359 EP 4372 DI 10.5194/acp-13-4359-2013 PG 14 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA 137IF UT WOS:000318428300027 ER PT J AU Zhang, K Liu, X Wang, M Comstock, JM Mitchell, DL Mishra, S Mace, GG AF Zhang, K. Liu, X. Wang, M. Comstock, J. M. Mitchell, D. L. Mishra, S. Mace, G. G. TI Evaluating and constraining ice cloud parameterizations in CAM5 using aircraft measurements from the SPARTICUS campaign SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID COMMUNITY ATMOSPHERE MODEL; CIRRUS MICROPHYSICAL PROPERTIES; HOMOGENEOUS NUCLEATION RATE; UPPER-TROPOSPHERIC CLOUDS; GLOBAL CLIMATE MODEL; PART I; NUMERICAL-SIMULATION; EFFECTIVE DIAMETER; RELATIVE-HUMIDITY; VERSION-3 CAM3 AB This study uses aircraft measurements of relative humidity and ice crystal size distribution collected during the SPARTICUS (Small PARTicles In CirrUS) field campaign to evaluate and constrain ice cloud parameterizations in the Community Atmosphere Model version 5. About 200 h of data were collected during the campaign between January and June 2010, providing the longest aircraft measurements available so far for cirrus clouds in the midlatitudes. The probability density function (PDF) of ice crystal number concentration (N-i) derived from the high-frequency (1 Hz) measurements features a strong dependence on ambient temperature. As temperature decreases from -35 degrees C to -62 degrees C, the peak in the PDF shifts from 10-20 L-1 to 200-1000 L-1, while N-i shows a factor of 6-7 increase. Model simulations are performed with two different ice nucleation schemes for pure ice-phase clouds. One of the schemes can reproduce a clear increase of N-i with decreasing temperature by using either an observation-based ice nuclei spectrum or a classical-theory-based spectrum with a relatively low (5-10 %) maximum freezing ratio for dust aerosols. The simulation with the other scheme, which assumes a high maximum freezing ratio (100 %), shows much weaker temperature dependence of N-i. Simulations are also performed to test empirical parameters related to water vapor deposition and the autoconversion of ice crystals to snow. Results show that a value between 0.05 and 0.1 for the water vapor deposition coefficient, and 250 mu m for the critical diameter that distinguishes ice crystals from snow, can produce good agreement between model simulation and the SPARTICUS measurements in terms of N-i and effective radius. The climate impact of perturbing these parameters is also discussed. C1 [Zhang, K.; Liu, X.; Wang, M.; Comstock, J. M.] Pacific NW Natl Lab, Richland, WA 99352 USA. [Mitchell, D. L.; Mishra, S.] Univ Nevada, Desert Res Inst, Reno, NV 89506 USA. [Mishra, S.] CIMMS, Norman, OK USA. [Mace, G. G.] Univ Utah, Dept Meteorol, Salt Lake City, UT 84112 USA. RP Zhang, K (reprint author), Pacific NW Natl Lab, Richland, WA 99352 USA. EM kai.zhang@pnnl.gov RI Wang, Minghuai/E-5390-2011; Liu, Xiaohong/E-9304-2011; Zhang, Kai/F-8415-2010 OI Wang, Minghuai/0000-0002-9179-228X; Liu, Xiaohong/0000-0002-3994-5955; Zhang, Kai/0000-0003-0457-6368 FU NASA Modeling, Analysis and Prediction (MAP) Program; DOE Atmospheric System Research (ASR) Program; DOE Atmospheric Radiation Measurement (ARM) Program; DOE [DE-AC06-76RLO 1830] FX We thank Paul Lawson (SPEC Inc.) for his help with the ice crystal number concentration measured by the 2D-S probe and Glenn S. Diskin (NASA Langley Research Center) for the DLH water vapor measurements. We are also grateful to Xiangjun Shi (IAP/CAS), Eric Jensen (NASA Ames), Donifan Barahona (NASA GSFC), Hugh Morrison (NCAR), and Phil Rasch for helpful discussions. Comments and suggestions from Hui Wan provided through the PNNL internal review are highly appreciated. We also thank the two anonymous referees for their helpful reviews. Kai Zhang and Xiaohong Liu acknowledge support from the NASA Modeling, Analysis and Prediction (MAP) Program. Xiaohong Liu and Minghuai Wang acknowledge support from the DOE Atmospheric System Research (ASR) Program. Jennifer M. Comstock was supported by the DOE Atmospheric Radiation Measurement (ARM) Program. The Pacific Northwest National Laboratory is operated for DOE by Battelle Memorial Institute under contract DE-AC06-76RLO 1830. NR 90 TC 20 Z9 20 U1 1 U2 27 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1680-7316 J9 ATMOS CHEM PHYS JI Atmos. Chem. Phys. PY 2013 VL 13 IS 9 BP 4963 EP 4982 DI 10.5194/acp-13-4963-2013 PG 20 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA 144LR UT WOS:000318941300031 ER PT J AU Lance, S Raatikainen, T Onasch, TB Worsnop, DR Yu, XY Alexander, ML Stolzenburg, MR McMurry, PH Smith, JN Nenes, A AF Lance, S. Raatikainen, T. Onasch, T. B. Worsnop, D. R. Yu, X. -Y. Alexander, M. L. Stolzenburg, M. R. McMurry, P. H. Smith, J. N. Nenes, A. TI Aerosol mixing state, hygroscopic growth and cloud activation efficiency during MIRAGE 2006 SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID AERODYNAMIC DIAMETER MEASUREMENTS; DIFFERENTIAL MOBILITY ANALYZER; BIOMASS BURNING SMOKE; MEGA-CITY GUANGZHOU; MEXICO-CITY; CONDENSATION NUCLEI; PART 1; CCN ACTIVATION; BOREAL FOREST; DENSITY CHARACTERIZATION AB Observations of aerosol hygroscopic growth and CCN activation spectra for submicron particles are reported for the T1 ground site outside of Mexico City during the MIRAGE 2006 campaign. kappa-Kohler theory is used to evaluate the characteristic hygroscopicity parameter, kappa*, for the CCN active aerosol population using both size-resolved HTMDA and size-resolved CCNc measurements. Organic mass fractions (f(org)) are evaluated from size-resolved aerosol mass spectrometer (AMS) measurements, from which predictions of the hygroscopicity parameter are compared against kappa*. Strong diurnal changes in aerosol water uptake parameters and aerosol composition are observed. We find that new particle formation (NPF) events are correlated with an increased kappa* and CCN-active fraction during the daytime, with greater impact on smaller particles. During NPF events, the number concentration of 40 nm particles acting as CCN at 0.51%+/- 0.06% supersaturation can surpass by more than a factor of two the corresponding concentrations of 100 nm particles. We also find that at 06:00-08:00 LT throughout the campaign, fresh traffic emissions result in substantial changes to the chemical distribution of the aerosol, with on average 65% externally mixed fraction for 40 nm particles and 30% externally mixed fraction for 100 nm particles, whereas at midday nearly all particles of both sizes can be described as "internally mixed". Average activation spectra and growth factor distributions are analyzed for different time periods characterizing the daytime (with and without NPF events), the early morning "rush hour" and the entire campaign. We show that kappa* derived from CCNc measurements decreases as a function of size during all time periods, while the CCN-active fraction increases as a function of size. Size-resolved AMS measurements do not predict the observed trend for kappa* versus particle size, which can be attributed to unresolved mixing state and the presence of refractory material not measured by the AMS. Measured kappa* typically ranges from 0.2 to 0.35, and organics typically make up 60-85% of the aerosol mass in the size range studied. We show that kappa(AMS) is able to describe CCN concentrations reasonably well, provided mixing-state information is available, especially at the highest CCN concentrations. This is consistent with other CCN studies carried out in urban environments, and is partly due to the fact that the highest CCN concentrations occur during the daytime when the aerosol is internally mixed. During the early morning rush hour, however, failing to account for the aerosol mixing state results in systematic overestimation of CCN concentrations by as much as 50-100% on average. C1 [Lance, S.; Raatikainen, T.; Nenes, A.] Georgia Inst Technol, Sch Earth & Atmospher Sci, Atlanta, GA 30332 USA. [Lance, S.] NOAA, Earth Syst Res Lab, Boulder, CO USA. [Lance, S.] Univ Colorado, Cooperat Inst Res Environm Sci, Boulder, CO 80309 USA. [Lance, S.; Smith, J. N.] Natl Ctr Atmospher Res, Div Atmospher Chem, Boulder, CO 80307 USA. [Raatikainen, T.] Finnish Meteorol Inst, FIN-00101 Helsinki, Finland. [Onasch, T. B.; Worsnop, D. R.] Aerodyne Res Inc, Billerica, MA 01821 USA. [Yu, X. -Y.; Alexander, M. L.] Pacific NW Natl Lab, Richland, WA 99352 USA. [Stolzenburg, M. R.; McMurry, P. H.] Univ Minnesota, Dept Mech Engn, Minneapolis, MN 55455 USA. [Nenes, A.] Georgia Inst Technol, Sch Chem & Biomol Engn, Atlanta, GA 30332 USA. RP Nenes, A (reprint author), Georgia Inst Technol, Sch Earth & Atmospher Sci, Atlanta, GA 30332 USA. EM athanasios.nenes@gatech.edu RI Worsnop, Douglas/D-2817-2009; Smith, James/C-5614-2008; Raatikainen, Tomi/C-5410-2014; Yu, Xiao-Ying/L-9385-2013; McMurry, Peter/A-8245-2008; Manager, CSD Publications/B-2789-2015 OI Worsnop, Douglas/0000-0002-8928-8017; Smith, James/0000-0003-4677-8224; Yu, Xiao-Ying/0000-0002-9861-3109; McMurry, Peter/0000-0003-1609-5131; FU Georgia Tech Presidential Fellowship; NCAR ASP Fellowship; NSF CAREER grant; Finnish Cultural Foundation; DOE [DE-FG-02-05ER63997, DE-FG02-05ER63982]; NSF [ATM-0528170]; DOE Biological and Environmental (BER) Atmospheric System Research (ASR) grant [DE-AC05-76RLO1830/KP1701000/57131]; NOAA FX S. Lance was supported by a Georgia Tech Presidential Fellowship and NCAR ASP Fellowship. A. Nenes acknowledges support from an NSF CAREER grant. T. Raatikainen acknowledges funding support from the Finnish Cultural Foundation. University of Minnesota researchers were supported by DOE grant DE-FG-02-05ER63997. T. Onasch and D. Worsnop acknowledge DOE grant DE-FG02-05ER63982 and NSF grant ATM-0528170. Thanks to Jeff Gaffney and Nancy Marley at the University of Arkansas at Little Rock for meteorological and ultraviolet solar insolation data at the T1 site during MIRAGE 2006. X.-Y. Yu acknowledges the support from the DOE Biological and Environmental (BER) Atmospheric System Research (ASR) grant under contract DE-AC05-76RLO1830/KP1701000/57131. PNNL is operated by the US DOE by Battelle Memorial Institute. This work was also supported by NOAA climate and air quality programs. NR 42 TC 17 Z9 18 U1 1 U2 54 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1680-7316 J9 ATMOS CHEM PHYS JI Atmos. Chem. Phys. PY 2013 VL 13 IS 9 BP 5049 EP 5062 DI 10.5194/acp-13-5049-2013 PG 14 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA 144LR UT WOS:000318941300036 ER PT J AU Kasimatis, G Fitz-Gibbon, S Tomida, S Wong, M Li, HY AF Kasimatis, Gabriela Fitz-Gibbon, Sorel Tomida, Shuta Wong, Marthew Li, Huiying TI Analysis of Complete Genomes of Propionibacterium acnes Reveals a Novel Plasmid and Increased Pseudogenes in an Acne Associated Strain SO BIOMED RESEARCH INTERNATIONAL LA English DT Article ID LINEAR PLASMIDS; BORRELIA-BURGDORFERI; IMPROVE OUTCOMES; SKIN MICROBIOME; GLOBAL ALLIANCE; SEQUENCE; VIRULENCE; BACTERIA; WIDESPREAD; MANAGEMENT AB The human skin harbors a diverse community of bacteria, including the Gram-positive, anaerobic bacterium Propionibacterium acnes. P. acnes has historically been linked to the pathogenesis of acne vulgaris, a common skin disease affecting over 80% of all adolescents in the US. To gain insight into potential P. acnes pathogenic mechanisms, we previously sequenced the complete genome of a P. acnes strain HL096PA1 that is highly associated with acne. In this study, we compared its genome to the first published complete genome KPA171202. HL096PA1 harbors a linear plasmid, pIMPLE-HL096PA1. This is the first described P. acnes plasmid. We also observed a five-fold increase of pseudogenes in HL096PA1, several of which encode proteins in carbohydrate transport and metabolism. In addition, our analysis revealed a few island-like genomic regions that are unique to HL096PA1 and a large genomic inversion spanning the ribosomal operons. Together, these findings offer a basis for understanding P. acnes virulent properties, host adaptation mechanisms, and its potential role in acne pathogenesis at the strain level. Furthermore, the plasmid identified in HL096PA1 may potentially provide a new opportunity for P. acnes genetic manipulation and targeted therapy against specific disease-associated strains. C1 [Kasimatis, Gabriela; Fitz-Gibbon, Sorel; Tomida, Shuta; Wong, Marthew; Li, Huiying] Univ Calif Los Angeles, Crump Inst Mol Imaging, Dept Mol & Med Pharmacol, Los Angeles, CA 90095 USA. [Li, Huiying] Univ Calif Los Angeles, DOE Inst Genom & Prote, Los Angeles, CA 90095 USA. RP Li, HY (reprint author), Univ Calif Los Angeles, Crump Inst Mol Imaging, Dept Mol & Med Pharmacol, Los Angeles, CA 90095 USA. EM huiying@mednet.ucla.edu FU NIH Human Microbiome Project from NIAMS [UH2AR057503] FX The authors thank Lin Lin for her technical support in finishing the HL096PA1 genome. They also thank Anya Loncaric and Dr. Robert Modlin at UCLA for providing HL096PA1 strain. This research was partly funded by one of the demonstration projects by the NIH Human Microbiome Project under Grant no. UH2AR057503 from NIAMS. NR 46 TC 13 Z9 13 U1 0 U2 20 PU HINDAWI PUBLISHING CORPORATION PI NEW YORK PA 410 PARK AVENUE, 15TH FLOOR, #287 PMB, NEW YORK, NY 10022 USA SN 2314-6133 J9 BIOMED RES INT JI Biomed Res. Int. PY 2013 AR 918320 DI 10.1155/2013/918320 PG 11 WC Biotechnology & Applied Microbiology; Medicine, Research & Experimental SC Biotechnology & Applied Microbiology; Research & Experimental Medicine GA 153JC UT WOS:000319596700001 ER PT J AU Wong-Ng, W Culp, JT Chen, YS Zavalij, P Espinal, L Siderius, DW Allen, AJ Scheins, S Matranga, C AF Wong-Ng, W. Culp, J. T. Chen, Y. S. Zavalij, P. Espinal, L. Siderius, D. W. Allen, A. J. Scheins, S. Matranga, C. TI Improved synthesis and crystal structure of the flexible pillared layer porous coordination polymer: Ni(1,2-bis(4-pyridyl)ethylene)[Ni(CN)(4)] SO CRYSTENGCOMM LA English DT Article ID METAL-ORGANIC FRAMEWORKS; SPIN-CROSSOVER; SURFACE-AREAS; NICKEL CYANIDE; PORE-SIZE; ADSORPTION; NI; CONSTRUCTION; ASSEMBLIES; NETWORKS AB This paper reports our synthesis of flexible coordination polymer, Ni(L)[ Ni(CN)(4)], (L = 1,2-bis(4-pyridyl)ethylene (nicknamed bpene)), and its structural characterization using synchrotron single crystal X-ray diffraction. The structure of the purplish crystals has been determined to be monoclinic, space group P2(1)/m, a = 13.5941(12) angstrom, b = 14.3621(12) angstrom, c = 14.2561(12) angstrom, beta = 96.141(2)degrees, V = 2767.4(4) angstrom(3), Z = 4, D-c = 1.46 g cm(-1). Ni(bpene)[ Ni(CN)(4)] assumes a pillared layer structure with layers defined by Ni[ Ni(CN)(4)](n) nets and bpene ligands acting as pillars. With the present crystallization technique which involves the use of concentrated ammonium hydroxide solution and dimethyl sulfoxide (DMSO), disordered free bpene ligands and solvents of crystallization (DMSO and water molecules) occupy the pores, resulting in a formula of Ni(bpene)[ Ni(CN)(4)]center dot 1/2 bpene center dot DMSO center dot 2H(2)O, or Ni2N7C24H25SO3. Without the inclusion of free bpene ligands and solvent molecules, the free volume is approximately 61% of the total volume; this free volume fraction is reduced to 50% with the free ligands present. Pores without the free ligands were found to have a local diameter of 5.7 angstrom and a main aperture of 3.5 angstrom. Based on the successful crystal synthesis, we also devised a new bulk synthetic technique which yielded a polycrystalline material with a significantly improved CO2 uptake as compared to the originally reported powder material. The improved synthetic technique yielded a polycrystalline material with 40% higher CO2 uptake compared to the previously reported powder material. An estimated 14.4 molecules of CO2 per unit cell was obtained. C1 [Wong-Ng, W.; Espinal, L.; Siderius, D. W.; Allen, A. J.] NIST, Mat Measurement Lab, Gaithersburg, MD 20899 USA. [Culp, J. T.; Matranga, C.] US DOE, Natl Energy Technol Lab, Pittsburgh, PA 15236 USA. [Culp, J. T.] URS Corp, South Park, PA 15219 USA. [Chen, Y. S.; Scheins, S.] Univ Chicago, ChemMatCARS, Argonne, IL 60439 USA. [Zavalij, P.] Univ Maryland, Dept Chem & Biochem, College Pk, MD 20742 USA. RP Wong-Ng, W (reprint author), NIST, Mat Measurement Lab, Gaithersburg, MD 20899 USA. RI Zavalij, Peter/H-3817-2012; Matranga, Christopher/E-4741-2015 OI Zavalij, Peter/0000-0001-5762-3469; Matranga, Christopher/0000-0001-7082-5938 FU RES [DE-FE0004000]; National Science Foundation/Department of Energy [NSF/CHE-0822838]; U. S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357] FX This technical effort was performed in support of the National Energy Technology's ongoing research in CO2 capture under the RES contract DE-FE0004000. The authors gratefully acknowledge ChemMatCARS Sector 15 which is principally supported by the National Science Foundation/Department of Energy under grant number NSF/CHE-0822838. Use of the Advanced Photon Source was supported by the U. S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. NR 44 TC 7 Z9 7 U1 0 U2 29 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 23 BP 4684 EP 4693 DI 10.1039/c3ce00017f PG 10 WC Chemistry, Multidisciplinary; Crystallography SC Chemistry; Crystallography GA 148FF UT WOS:000319227900014 ER PT J AU Sun, XQ Luo, HM Dai, S AF Sun, Xiaoqi Luo, Huimin Dai, Sheng TI Mechanistic investigation of solvent extraction based on anion-functionalized ionic liquids for selective separation of rare-earth ions SO DALTON TRANSACTIONS LA English DT Article ID NITRIC-ACID MEDIUM; CROWN-ETHERS; TEMPERATURE; AMERICIUM(III); COORDINATION; GREENNESS; EXCHANGE; BEHAVIOR; DILUENT; MEDIA AB In this study, solvation has been found to be a dominant mechanism in an ionic liquid (IL)-based extraction system for rare earth elements (REEs). Trioctylmethylammonium di(2-ethylhexyl)phosphate ([TOMA][DEHP]), an anion-functionalized IL extractant, was used in 1-alkyl-3-methylimidizolium bis[(trifluoromethylsulfonyl)]imide ([C(n)mim][NTf2], n = 4, 6, 8, 10) and 1-alkyl-3-methylimidizolium bis(perfluoroethane-sulfonyl)imide ([C(n)mim][BETI], n = 4, 6, 8, 10) for the separation of REEs. Surprisingly, a very similar extraction behavior was observed even as the carbon chain length on the IL cation increased from butyl (C4) to decyl (C10). This behavior is in sharp contrast to that exhibited by the conventional molecular extractants, whose extraction efficiencies are strongly dependent on the hydrophobicity of IL cations. Furthermore, the addition of IL cations ([C(n)mim](+)) in [C(n)mim]Cl form or IL anions ([NTf2](-) or [BETI](-)) in Li[NTf2] or Li[BETI] form to the aqueous phase had a minor effect on the extraction behavior of the above extraction system, ruling out the strong involvement of the ion-exchange mechanism associated with traditional IL-based extraction systems. Results showed that the extractabilities and selectivities of REEs using [TOMA][DEHP] in [C(10)mim][NTf2]/[BETI] are several orders of magnitude better than those achieved using a conventional organic solvent, diisopropylbenzene (DIPB). This study highlights the potential of developing a comprehensive IL-based extraction strategy for REEs separations via ionic extractants. C1 [Sun, Xiaoqi; Dai, Sheng] Oak Ridge Natl Lab, Chem Sci Div, Oak Ridge, TN 37831 USA. [Sun, Xiaoqi] Chinese Acad Sci, Inst Appl Chem, State Key Lab Rare Earth Resource Utilizat, Changchun 130022, Peoples R China. [Luo, Huimin] Oak Ridge Natl Lab, Energy & Transportat Sci Div, Oak Ridge, TN 37831 USA. [Dai, Sheng] Univ Tennessee, Dept Chem, Knoxville, TN 37916 USA. RP Luo, HM (reprint author), Oak Ridge Natl Lab, Energy & Transportat Sci Div, Oak Ridge, TN 37831 USA. EM luoh@ornl.gov; dais@ornl.gov RI Dai, Sheng/K-8411-2015 OI Dai, Sheng/0000-0002-8046-3931 FU U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences [DE-AC05-0096OR22725]; Oak Ridge National Laboratory; Oak Ridge Associated Universities (ORAU) FX This research was supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences under Contract DE-AC05-0096OR22725 with Oak Ridge National Laboratory, managed by UT-Battelle, LLC. XQS acknowledge the Oak Ridge Associated Universities (ORAU) for postdoctoral fellowships. The authors would like to thank the referees for their useful comments. NR 28 TC 22 Z9 22 U1 2 U2 101 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 23 BP 8270 EP 8275 DI 10.1039/c3dt50148e PG 6 WC Chemistry, Inorganic & Nuclear SC Chemistry GA 148YY UT WOS:000319286300017 PM 23595558 ER PT J AU Shea-Rohwer, LE Martin, JE Cai, XC Kelley, DF AF Shea-Rohwer, Lauren E. Martin, James E. Cai, Xichen Kelley, David F. TI Red-Emitting Quantum Dots for Solid-State Lighting SO ECS JOURNAL OF SOLID STATE SCIENCE AND TECHNOLOGY LA English DT Article ID TEMPERATURE-DEPENDENT PHOTOLUMINESCENCE; BROAD-BAND EMISSION; RECOMBINATION DYNAMICS; NANOCRYSTALS; DIODES; COLOR; CDSE; YIELD; CDTE AB Red emitters that can be excited with blue InGaN LEDs are essential for warm white LEDs for solid-state lighting (SSL). Current red phosphors do not satisfy all of the criteria for SSL. Red-emitting CdTe-based quantum dot (QD) heterostructures meet several of these criteria, such as narrowband emission, broad blue absorption, high quantum yield (QY), and high luminous efficacy of radiation. This paper describes the synthesis of CdTe, CdTe/2CdSe, CdTe/2CdSe/CdS, and CdTe/2CdSe/CdS/5ZnS QDs and their photoluminescence. The growth of two CdSe shells on the CdTe core increases the QY to 95.5%. The shells reduce the thermal quenching above room temperature. CdTe cores that were aged for one year, exhibited thermal quenching of 73% at 100 degrees C, whereas the aged CdTe/2CdSe and CdTe/2CdSe/CdS QDs had thermal quenching of 39% and 38%, respectively at 100 degrees C. After cooling to room temperature, the QDs retained similar to 92% of their initial QYs. CdTe-based QDs have substantially less thermal quenching than CdSe/ZnSe QDs, which exhibit an 87% reduction in the QY and thermal degradation at 100 degrees C. Aging the various QDs for one year resulted in blue-shifts of the absorbance and PL emission by similar to 5-11 nm; broadening of the FWHM by similar to 0.7-4 nm; and an increase in the PL lifetimes. (C) 2012 The Electrochemical Society. C1 [Shea-Rohwer, Lauren E.; Martin, James E.] Sandia Natl Labs, Albuquerque, NM 87185 USA. [Cai, Xichen; Kelley, David F.] Univ Calif Merced, Merced, CA 95343 USA. RP Shea-Rohwer, LE (reprint author), Sandia Natl Labs, POB 5800, Albuquerque, NM 87185 USA. EM leshea@sandia.gov FU Sandia's Solid-State Lighting Science Energy Frontiers Research Center; U.S. Department of Energy, Office of Basic Energy Sciences; U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX This work was funded by Sandia's Solid-State Lighting Science Energy Frontiers Research Center, funded by the U.S. Department of Energy, Office of Basic Energy Sciences. 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 25 TC 10 Z9 10 U1 2 U2 25 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 2162-8769 J9 ECS J SOLID STATE SC JI ECS J. Solid State Sci. Technol. PY 2013 VL 2 IS 2 SI SI BP R3112 EP R3118 DI 10.1149/2.015302jss PG 7 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA 151IZ UT WOS:000319455200015 ER PT J AU Zhang, CQ Xia, Y Chen, RQ Huh, S Johnston, PA Kessler, MR AF Zhang, Chaoqun Xia, Ying Chen, Ruqi Huh, Seungmoo Johnston, Patrick A. Kessler, Michael R. TI Soy-castor oil based polyols prepared using a solvent-free and catalyst-free method and polyurethanes therefrom SO GREEN CHEMISTRY LA English DT Article ID VEGETABLE-OILS; SOYBEAN OIL; PHYSICAL-PROPERTIES; CYCLOHEXENE OXIDE; CANOLA OIL; PALM OIL; OLIGOMERIZATION; POLYMERIZATION; MECHANISM; NETWORKS AB Bio-based polyols from epoxidized soybean oil and castor oil fatty acid were developed using an environmentally friendly, solvent-free/catalyst-free method. The effects of the molar ratios of the carboxyl to the epoxy groups, reaction time, and reaction temperature on the polyols' structures were systematically studied. Subsequently, polyurethane films were prepared from these green polyols. Properties of the new, soy-castor oil based polyurethane films were compared with two other polyurethane films prepared from castor oil and methoxylated soybean oil polyol, respectively. Thermal and mechanical tests showed that the polyurethane films prepared from the new polyols exhibited higher glass transition temperatures, tensile strength, Young's modulus, and thermal stability because of the higher degree of cross-linking in the new polyols. Moreover, the novel polyols, prepared using the solvent-free and catalyst-free synthetic route, were 100% bio-based and facilitate a more environmentally friendly and economical process than conventional soy-based polyols used for polyurethane production. C1 [Zhang, Chaoqun; Xia, Ying; Chen, Ruqi; Kessler, Michael R.] Iowa State Univ, Dept Mat Sci & Engn, Ames, IA 50011 USA. [Huh, Seungmoo] Kumho Petrochem R&BD Ctr, Taejon, South Korea. [Johnston, Patrick A.] Iowa State Univ, Ctr Sustainable Environm Technol, Ames, IA USA. [Kessler, Michael R.] Iowa State Univ, Dept Mech Engn, Ames, IA USA. [Kessler, Michael R.] US DOE, Ames Lab, Ames, IA 50011 USA. RP Zhang, CQ (reprint author), Iowa State Univ, Dept Mat Sci & Engn, Ames, IA 50011 USA. EM mkessler@iastate.edu RI Kessler, Michael/C-3153-2008; Xia, Ying/G-9533-2012 OI Kessler, Michael/0000-0001-8436-3447; FU Kumho Petrochemical Co. FX This work was sponsored by Kumho Petrochemical Co. NR 29 TC 52 Z9 54 U1 9 U2 79 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9262 J9 GREEN CHEM JI Green Chem. PY 2013 VL 15 IS 6 BP 1477 EP 1484 DI 10.1039/c3gc40531a PG 8 WC Chemistry, Multidisciplinary; GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY SC Chemistry; Science & Technology - Other Topics GA 150QM UT WOS:000319405900005 ER PT J AU Li, Z Sun, YG AF Li, Zheng Sun, Yugang TI Silver chlorobromide nanoparticles with highly pure phases: synthesis and characterization SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID VISIBLE-LIGHT; PHOTOCATALYTIC DEGRADATION; AQUEOUS SUSPENSION; WATER OXIDATION; METHYLENE-BLUE; GOLD NANORODS; AGCL; SURFACE; ABSORPTION; MICROSCOPY AB Ternary silver chlorobromide (AgClxBr1-x) nanoparticles with finely tuned compositions have been successfully synthesized through a co-precipitation approach in which silver nitrate reacts with hexadecyltrimethylammonium chloride (CTAC) and hexadecyltrimethylammonium bromide (CTAB) in aqueous solutions at room temperature. The synthesized AgClxBr1-x nanoparticles exhibit highly pure crystalline phases with face-centred cubic symmetries and compositional purity without contamination of optically active silver clusters and silver nanodomains. Such high purity enables the determination of indirect bandgap energies of the AgClxBr1-x nanoparticles for the first time. Tuning the composition from chloride-to bromide-rich leads to a decrease in size and the indirect bandgap of the nanoparticles. In addition, preliminary evaluations indicate that the ternary AgClxBr1-x nanoparticles are better in the photocatalytic decomposition of methylene blue molecules with visible light in comparison with the counterpart binary AgCl and AgBr nanoparticles. C1 [Li, Zheng; Sun, Yugang] Argonne Natl Lab, Ctr Nanoscale Mat, Argonne, IL 60439 USA. RP Li, Z (reprint author), Argonne Natl Lab, Ctr Nanoscale Mat, 9700 S Cass Ave, Argonne, IL 60439 USA. EM ygsun@anl.gov RI Sun, Yugang /A-3683-2010; Li, Zheng/L-1355-2016 OI Sun, Yugang /0000-0001-6351-6977; Li, Zheng/0000-0001-5281-8101 FU Center for Nanoscale Materials, a US Department of Energy, Office of Science, Office of Basic Energy Sciences User Facility [DE-AC02-06CH11357]; Electron Microscopy Center at Argonne National Laboratory, a US Department of Energy Office of Science Laboratory by UChicago Argonne, LLC. [DE-AC02-06CH11357] FX This work was performed at the Center for Nanoscale Materials, a US Department of Energy, Office of Science, Office of Basic Energy Sciences User Facility under Contract no. DE-AC02-06CH11357. The electron microscopy and EDX was partially accomplished at the Electron Microscopy Center at Argonne National Laboratory, a US Department of Energy Office of Science Laboratory operated under Contract no. DE-AC02-06CH11357 by UChicago Argonne, LLC. The authors gratefully appreciate helpful discussions with Dr Ian McNulty and Dr Yang Ren. NR 51 TC 4 Z9 4 U1 0 U2 30 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 23 BP 6786 EP 6793 DI 10.1039/c3ta00020f PG 8 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA 148UJ UT WOS:000319272800012 ER PT J AU Cai, L Liu, ZC An, K Liang, CD AF Cai, Lu Liu, Zengcai An, Ke Liang, Chengdu TI Unraveling structural evolution of LiNi0.5Mn1.5O4 by in situ neutron diffraction SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID LITHIUM-ION BATTERY; ELECTROCHEMICAL PROPERTIES; CRYSTAL-STRUCTURE; SPINEL; ELECTRODE; CATHODE; OXYGEN; PERFORMANCE; TRANSITION; P4(3)32 AB The electrochemical properties of the spinel LiNi0.5Mn1.5O4 cathode material are influenced by the synthesis processes, which determines the impurity phase and the distribution of Ni and Mn in the spinel structure. Taking advantage of neutron's high sensitivity to Ni and Mn, in situ neutron diffraction has been employed to quantify the phase formation/structural evolution process under continuous heating/cooling and isothermal annealing conditions. The results show that the subtle Ni and Mn ordering process occurs slowly at 700 degrees C and the degree of ordering can be controlled by the annealing time. At temperatures above 750 degrees C, the LiNi0.5Mn1.5O4 spinel phase starts to decompose into the rock-salt impurity phase accompanied by the release of O-2. The rock-salt phase reverts back to the spinel phase upon cooling along with the oxygen uptake. The dynamic process of structural evolution of LiNi0.5Mn1.5O4 that was unraveled by in situ neutron diffraction is valuable for guiding the synthesis of cathode materials with desirable properties. C1 [Cai, Lu; An, Ke] Oak Ridge Natl Lab, Chem & Engn Mat Div, Oak Ridge, TN USA. [Liu, Zengcai; Liang, Chengdu] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. RP Cai, L (reprint author), Oak Ridge Natl Lab, Chem & Engn Mat Div, Oak Ridge, TN USA. EM kean@ornl.gov RI An, Ke/G-5226-2011 OI An, Ke/0000-0002-6093-429X FU U.S. Department of Energy, Basic Energy Sciences, Materials Sciences and Engineering Division; Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy FX This research is supported by the U.S. Department of Energy, Basic Energy Sciences, Materials Sciences and Engineering Division and performed at Spallation Neutron Source and Center for Nanophase Materials Sciences, DOE user facilities at Oak Ridge National Laboratory, which are sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy. LC and KA thank Ms R. Mills and Mr H. Skorpenske from SNS for their technical support for the neutron experiments. NR 32 TC 18 Z9 18 U1 4 U2 57 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 23 BP 6908 EP 6914 DI 10.1039/c3ta00145h PG 7 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA 148UJ UT WOS:000319272800027 ER PT J AU Ryan, KR Trahey, L Okasinski, JS Burrell, AK Ingram, BJ AF Ryan, Kate R. Trahey, Lynn Okasinski, John S. Burrell, Anthony K. Ingram, Brian J. TI In situ synchrotron X-ray diffraction studies of lithium oxygen batteries SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID LI-AIR BATTERIES; LI-O-2 BATTERIES; ION BATTERIES; ETHER; ELECTROLYTES; SOLVENTS; XRD; ELECTROCHEMISTRY; STABILITY; EVOLUTION AB Lithium oxygen batteries were studied in situ by synchrotron X-ray diffraction. Crystalline Li2O2 was shown to form reversibly on a plain carbon cathode under normal cycling conditions. However, if the cell was polarized to induce electrolyte decomposition before the oxygen reduction reaction was initiated, LiOH was found to cycle reversibly on the cathode instead. A mechanism linking the LiOH production to the electrolyte decomposition was proposed. C1 [Ryan, Kate R.; Trahey, Lynn; Burrell, Anthony K.; Ingram, Brian J.] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. [Okasinski, John S.] Argonne Natl Lab, Adv Photon Source, Xray Sci Div, Argonne, IL 60439 USA. RP Ryan, KR (reprint author), Univ Oxford, Dept Chem, Oxford OX1 2JD, England. EM ingram@anl.gov FU U.S. Department of Energy; U.S. DOE [DE-AC02-06CH11357] FX The authors are particularly indebted to Dr Yan Ren sector 11 of the APS for the loan of the in situ coin cell chamber. Financial support from the U.S. Department of Energy is gratefully acknowledged. Use of the Advanced Photon Source, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science by Argonne National Laboratory, was supported by the U.S. DOE under Contract no. DE-AC02-06CH11357. 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. Argonne National Laboratory assisted in meeting the publication costs of this article. NR 26 TC 14 Z9 15 U1 5 U2 89 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 23 BP 6915 EP 6919 DI 10.1039/c3ta10361g PG 5 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA 148UJ UT WOS:000319272800028 ER PT J AU Seredych, M Idrobo, JC Bandosz, TJ AF Seredych, Mykola Idrobo, Juan-Carlos Bandosz, Teresa J. TI Effect of confined space reduction of graphite oxide followed by sulfur doping on oxygen reduction reaction in neutral electrolyte SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID DENSITY-FUNCTIONAL THEORY; METAL-FREE ELECTROCATALYST; CATALYTIC-ACTIVITY; ACTIVATED CARBONS; DOPED GRAPHENE; SOLAR-ENERGY; NITROGEN; ADSORPTION; PYROLYSIS; OXIDATION AB Graphite oxide was thermally reduced within the confined space of commercial silica gel, and then the matrix was removed. The modified graphite oxide was treated with hydrogen sulfide at 800 degrees C. The treatment applied results in a specific porous texture and high hydrophobicity of the surface. 3 at.% sulfur was introduced, mainly as thiophenic groups and sulfur in aromatic rings. The reduced GO and sulfur doped was evaluated as oxygen reduction catalysts in neutral electrolytes. Even though both materials show the strong catalytic activity, the results indicate that more electrons take part in oxygen reduction reaction on reduced GO than on its sulfur modified counterpart. The high activity of our materials is linked to oxygen and surface functional groups incorporated to the graphene structure, to the high degree of surface hydrophobicity and to the specific texture consisting of micro and mesopores (replicate of silica porosity). C1 [Seredych, Mykola; Bandosz, Teresa J.] CUNY City Coll, Dept Chem, CUNY Energy Inst, New York, NY 10031 USA. [Idrobo, Juan-Carlos] Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA. RP Seredych, M (reprint author), CUNY City Coll, Dept Chem, CUNY Energy Inst, 160 Convent Ave, New York, NY 10031 USA. EM tbandosz@ccny.cuny.edu RI Idrobo, Juan/H-4896-2015 OI Idrobo, Juan/0000-0001-7483-9034 FU Oak Ridge National Laboratory' ShaRE User Facility; Scientific User Facility Division, Office of Basic Energy Sciences, U.S. Department of Energy FX The authors are grateful to Mr Jeffrey Shallenberger of Evans Analytical Group for his involvement in XPS analysis. This research was supported in part by Oak Ridge National Laboratory' ShaRE User Facility, which is sponsored by the Scientific User Facility Division, Office of Basic Energy Sciences, U.S. Department of Energy. NR 54 TC 28 Z9 28 U1 2 U2 52 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 24 BP 7059 EP 7067 DI 10.1039/c3ta10995j PG 9 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA 152IS UT WOS:000319525900012 ER PT J AU Haines, BM Grinstein, FF Schwarzkopf, JD AF Haines, Brian M. Grinstein, Fernando F. Schwarzkopf, John D. TI Reynolds-averaged Navier-Stokes initialization and benchmarking in shock-driven turbulent mixing SO JOURNAL OF TURBULENCE LA English DT Article DE large eddy simulation; Reynolds-averaged Navier-Stokes; turbulence modeling: Reynolds averaged; turbulent mixing; compressible turbulence ID RICHTMYER-MESHKOV INSTABILITY; LARGE-EDDY SIMULATION; TAYLOR-GREEN VORTEX; FLOWS; CLOSURE AB We investigate a strategy for benchmarking Reynolds-averaged Navier-Stokes (RANS) models by comparing moments extracted from averaged large eddy simulation (LES) data and those predicted directly by RANS. We consider the Besnard-Harlow-Rauenzahn (BHR) RANS approach designed for variable-density compressible flows, which has been previously applied to a wide variety of turbulence problems of interest. We focus on the model's ability to predict moments relevant to shock-driven material mixing. A prototypical inverse chevron shock tube configuration is considered, for which laboratory and previous LES studies are available for comparison and validation. We show that when appropriately initialized, BHR is capable of accurately capturing various characteristic integral measures of the flow; strategies for initialization are demonstrated while addressing sensitivity of BHR predictions to closure and initialization specifics, initial material interface conditions, and grid resolution. The reference simulations are performed using implicit LES based on the Los Alamos National Laboratory RAGE hydrodynamics code. C1 [Haines, Brian M.; Grinstein, Fernando F.; Schwarzkopf, John D.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Grinstein, FF (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM fgrinstein@lanl.gov OI Haines, Brian/0000-0002-3889-7074 FU U.S. Department of Energy, NNSA [DE-AC52-06NA25396] FX Los Alamos National Laboratory is operated by the Los Alamos National Security, LLC for the U.S. Department of Energy, NNSA under Contract No. DE-AC52-06NA25396. NR 43 TC 9 Z9 9 U1 1 U2 11 PU TAYLOR & FRANCIS LTD PI ABINGDON PA 4 PARK SQUARE, MILTON PARK, ABINGDON OX14 4RN, OXON, ENGLAND SN 1468-5248 J9 J TURBUL JI J. Turbul. PY 2013 VL 14 IS 2 BP 46 EP 70 DI 10.1080/14685248.2013.779380 PG 25 WC Mechanics; Physics, Fluids & Plasmas SC Mechanics; Physics GA 152WZ UT WOS:000319563800004 ER PT J AU Rubinstein, R Clark, TT AF Rubinstein, Robert Clark, Timothy T. TI Reassessment of the classical closures for scalar turbulence SO JOURNAL OF TURBULENCE LA English DT Article DE isotropic turbulence; homogeneous turbulence; passive scalar turbulence; solvable or simplified models; turbulent mixing ID QUANTITIES LIKE TEMPERATURE; ISOTROPIC TURBULENCE; DIFFUSION APPROXIMATION; ENERGY-TRANSFER; MODEL; FLUID; CONDUCTIVITY; DYNAMICS; FIELDS AB In deducing the consequences of the Direct Interaction Approximation, Kraichnan was sometimes led to consider the properties of special classes of nonlinear interactions in degenerate triads in which one wavevector is very small. Such interactions can be described by simplified models closely related to elementary closures for homogeneous isotropic turbulence such as the Heisenberg and Leith models. These connections can be exploited to derive considerably improved versions of the Heisenberg and Leith models that are only slightly more complicated analytically. This paper applies this approach to derive some new simplified closure models for passive scalar advection and investigates the consistency of these models with fundamental properties of scalar turbulence. Whereas some properties, such as the existence of the Kolmogorov-Obukhov range and the existence of thermal equilibrium ensembles, follow the velocity case closely, phenomena special to the scalar case arise when the diffusive and viscous effects become important at different scales of motion. These include the Batchelor and Batchelor-Howells-Townsend ranges pertaining, respectively, to high and low molecular Schmidt number. We also consider the spectrum in the diffusive range that follows the Batchelor range. We conclude that improved elementary models can be made consistent with many nontrivial properties of scalar turbulence, but that such models have unavoidable limitations. C1 [Rubinstein, Robert] NASA, Langley Res Ctr, Computat AeroSci Branch, Hampton, VA 23665 USA. [Clark, Timothy T.] Los Alamos Natl Lab, X Div Grp XCP 2, Los Alamos, NM USA. RP Clark, TT (reprint author), Los Alamos Natl Lab, X Div Grp XCP 2, Los Alamos, NM USA. EM ttc@lanl.gov NR 22 TC 2 Z9 2 U1 1 U2 1 PU TAYLOR & FRANCIS LTD PI ABINGDON PA 4 PARK SQUARE, MILTON PARK, ABINGDON OX14 4RN, OXON, ENGLAND SN 1468-5248 J9 J TURBUL JI J. Turbul. PY 2013 VL 14 IS 2 BP 71 EP 98 DI 10.1080/14685248.2013.769685 PG 28 WC Mechanics; Physics, Fluids & Plasmas SC Mechanics; Physics GA 152WZ UT WOS:000319563800005 ER PT J AU Niklas, J Mardis, KL Banks, BP Grooms, GM Sperlich, A Dyakonov, V Beaupre, S Leclerc, M Xu, T Yu, LP Poluektov, OG AF Niklas, Jens Mardis, Kristy L. Banks, Brian P. Grooms, Gregory M. Sperlich, Andreas Dyakonov, Vladimir Beaupre, Serge Leclerc, Mario Xu, Tao Yu, Luping Poluektov, Oleg G. TI Highly-efficient charge separation and polaron delocalization in polymer-fullerene bulk-heterojunctions: a comparative multi-frequency EPR and DFT study SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID PERFORMANCE SOLAR-CELLS; ZETA VALENCE QUALITY; GAUSSIAN-BASIS SETS; PHOTOVOLTAIC APPLICATIONS; CONDUCTING POLYMERS; ATOMS LI; DENSITY; ENERGY; POLY(3-HEXYLTHIOPHENE); POLY(3-ALKYLTHIOPHENES) AB The ongoing depletion of fossil fuels has led to an intensive search for additional renewable energy sources. Solar-based technologies could provide sufficient energy to satisfy the global economic demands in the near future. Photovoltaic (PV) cells are the most promising man-made devices for direct solar energy utilization. Understanding the charge separation and charge transport in PV materials at a molecular level is crucial for improving the efficiency of the solar cells. Here, we use light-induced EPR spectroscopy combined with DFT calculations to study the electronic structure of charge separated states in blends of polymers (P3HT, PCDTBT, and PTB7) and fullerene derivatives (C-60-PCBM and C-70-PCBM). Solar cells made with the same composites as active layers show power conversion efficiencies of 3.3% (P3HT), 6.1% (PCDTBT), and 7.3% (PTB7), respectively. Upon illumination of these composites, two paramagnetic species are formed due to photo-induced electron transfer between the conjugated polymer and the fullerene. They are the positive, P+, and negative, P-, polarons on the polymer backbone and fullerene cage, respectively, and correspond to radical cations and radical anions. Using the high spectral resolution of high-frequency EPR (130 GHz), the EPR spectra of these species were resolved and principal components of the g-tensors were assigned. Light-induced pulsed ENDOR spectroscopy allowed the determination of H-1 hyperfine coupling constants of photogenerated positive and negative polarons. The experimental results obtained for the different polymer-fullerene composites have been compared with DFT calculations, revealing that in all three systems the positive polaron is distributed over distances of 40-60 angstrom on the polymer chain. This corresponds to about 15 thiophene units for P3HT, approximately three units for PCDTBT, and about three to four units for PTB7. No spin density delocalization between neighboring fullerene molecules was detected by EPR. Strong delocalization of the positive polaron on the polymer donor is an important reason for the efficient charge separation in bulk heterojunction systems as it minimizes the wasteful process of charge recombination. The combination of advanced EPR spectroscopy and DFT is a powerful approach for investigation of light-induced charge dynamics in organic photovoltaic materials. C1 [Niklas, Jens; Poluektov, Oleg G.] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. [Mardis, Kristy L.; Banks, Brian P.; Grooms, Gregory M.] Chicago State Univ, Dept Chem & Phys, Chicago, IL 60628 USA. [Sperlich, Andreas; Dyakonov, Vladimir] Univ Wurzburg, D-97074 Wurzburg, Germany. [Sperlich, Andreas; Dyakonov, Vladimir] Bavarian Ctr Appl Energy Res, D-97074 Wurzburg, Germany. [Beaupre, Serge; Leclerc, Mario] Univ Laval, Dept Chem, Quebec City, PQ G1V 0A6, Canada. [Xu, Tao; Yu, Luping] Univ Chicago, Dept Chem, Chicago, IL 60637 USA. [Xu, Tao; Yu, Luping] Univ Chicago, James Franck Inst, Chicago, IL 60637 USA. RP Poluektov, OG (reprint author), Argonne Natl Lab, Chem Sci & Engn Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM Oleg@anl.gov RI Dyakonov, Vladimir/F-6862-2013; Niklas, Jens/I-8598-2016; OI Dyakonov, Vladimir/0000-0001-8725-9573; Niklas, Jens/0000-0002-6462-2680; Sperlich, Andreas/0000-0002-0850-6757; Mardis, Kristy/0000-0003-2633-9304 FU Argonne-Northwestern Solar Energy Research (ANSER) Center, an Energy Frontier Research Center; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001059]; DFG SPP "Elementary processes in organic photovoltaics" [DY18/6-1]; ANSER; Department of Defense Army Research Lab [W911NF-0820039]; National Institutes of Health [1SC2GM083717]; National Science Foundation IL-LSAMP [HRD-0413000]; GMG by the NIH/NIGMS [R25 GM059218]; Natural Sciences and Engineering Research Council (NSERC) of Canada FX This material is based upon work supported as part of the Argonne-Northwestern Solar Energy Research (ANSER) Center, 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-SC0001059 (JN, LU, and OGP) and by the DFG SPP "Elementary processes in organic photovoltaics", under contract DY18/6-1 (AS and VD). VD acknowledges financial support from ANSER during his research visit at ANL in 2012. KLM was supported by the Department of Defense Army Research Lab (W911NF-0820039) and the National Institutes of Health (Grant 1SC2GM083717). BPB was supported by the National Science Foundation IL-LSAMP (Grant HRD-0413000) and GMG by the NIH/NIGMS (R25 GM059218). We thank Alexander Fortig and Carsten Deibel (both U of Wurzburg) for solar cell fabrication and evaluation as well as for fruitful discussions. The synthesis of PCDTBT (M.L. and S.B.) was supported by the Natural Sciences and Engineering Research Council (NSERC) of Canada. NR 57 TC 56 Z9 56 U1 15 U2 216 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 24 BP 9562 EP 9574 DI 10.1039/c3cp51477c PG 13 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 153BP UT WOS:000319576500014 PM 23670645 ER PT J AU Harmon, CW Ruehl, CR Cappa, CD Wilson, KR AF Harmon, Christopher W. Ruehl, Christopher R. Cappa, Christopher D. Wilson, Kevin R. TI A statistical description of the evolution of cloud condensation nuclei activity during the heterogeneous oxidation of squalane and bis(2-ethylhexyl) sebacate aerosol by hydroxyl radicals SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID SECONDARY ORGANIC AEROSOL; SINGLE-PARAMETER REPRESENTATION; HYGROSCOPIC GROWTH; SURFACE-TENSION; CHEMICAL-COMPOSITION; INORGANIC PARTICLES; MASS-SPECTROMETER; ACTIVATION; PRODUCTS; CCN AB The heterogeneous reaction of hydroxyl radicals with chemically reduced organic aerosol comprised of either squalane or bis(2-ethylhexyl) sebacate are used as model systems to examine how cloud condensation nuclei (CCN) activity evolves with photochemical oxidation. Over the course of the reaction, the critical super-saturation evolves both by the formation of new oxygen functional groups and by changes in aerosol size through the formation of gas phase reaction products. A statistical model of the heterogeneous reaction reveals that it is the formation, volatilization, solubility, and surface activity of many generations of oxidation products that together control the average changes in aerosol hygroscopicity. The experimental observations and model demonstrate the importance of considering the underlying population or subpopulation of species within a particle and how they each uniquely contribute to the average hygroscopicity of a multi-component aerosol. To accurately predict changes in CCN activity upon oxidation requires a reduction in the surface tension of the activating droplet by a subpopulation of squalane reaction products. These results provide additional evidence that surface tension-concentration parameterizations based on macroscopic data should be modified for microscopic droplets. C1 [Harmon, Christopher W.; Ruehl, Christopher R.; Wilson, Kevin R.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. [Cappa, Christopher D.] Univ Calif Davis, Dept Civil & Environm Engn, Davis, CA 95616 USA. RP Wilson, KR (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. EM krwilson@lbl.gov FU Office of Energy Research, Office of Basic Energy Sciences, Chemical Sciences Division of the U.S. Department of Energy [DE-AC02-05CH11231]; Department of Energy, Office of Science Early Career Research Program; National Science Foundation [ATM-0837913] FX This work is 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. C.R.R. and K.R.W are supported by the Department of Energy, Office of Science Early Career Research Program. CDC was also supported by the National Science Foundation (ATM-0837913). NR 60 TC 10 Z9 10 U1 1 U2 34 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 24 BP 9679 EP 9693 DI 10.1039/c3cp50347j PG 15 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 153BP UT WOS:000319576500028 PM 23670352 ER PT J AU Duan, YH AF Duan, Yuhua TI Structural and electronic properties of Li8ZrO6 and its CO2 capture capabilities: an ab initio thermodynamic approach SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID CARBON-DIOXIDE SORPTION; LITHIUM ZIRCONATE; SOLID SORBENTS; TEMPERATURE; LI6ZR2O7; DIFFRACTION; ABSORPTION; SEPARATION; DYNAMICS; LI2ZRO3 AB The structural, electronic, and phonon properties of Li8ZrO6 are investigated with the application of density functional theory and lattice phonon dynamics. Based on the calculated data, the thermodynamics of CO2 absorption-desorption for Li8ZrO6 is analyzed and compared with those of Li2ZrO3 and Li6Zr2O7. The band gap of Li8ZrO6 is indirect along Gamma-L with a value of 4.74 eV. From the calculated thermodynamic properties of Li8ZrO6 reacting with CO2, we found that Li8ZrO6 could be regenerated at high temperatures (>1100 K). Our results indicated that the lithium zirconate with a lower Li2O/ZrO2 ratio has a lower turnover temperature. Hence, by mixing or doping two or more materials to form a new material, it is possible to find or synthesize CO2 sorbents that can fit the industrial needs for optimal performance. Although the CO2 capture capacity of Li8ZrO6 is much higher than that of Li2ZrO3, the high energy required for regeneration, the capacity loss during long absorption-desorption cycles, solid sintering at high temperature, and the material cost may affect its overall capture performance. Our results also provided some general guidelines for designing new CO2 sorbents. C1 US DOE, Natl Energy Technol Lab, Pittsburgh, PA 15236 USA. RP Duan, YH (reprint author), US DOE, Natl Energy Technol Lab, Pittsburgh, PA 15236 USA. EM yuhua.duan@netl.doe.gov RI Duan, Yuhua/D-6072-2011 OI Duan, Yuhua/0000-0001-7447-0142 NR 52 TC 16 Z9 16 U1 2 U2 38 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2013 VL 15 IS 24 BP 9752 EP 9760 DI 10.1039/c3cp51101d PG 9 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 153BP UT WOS:000319576500036 PM 23674075 ER PT J AU Delegard, CH AF Delegard, C. H. TI Effects of aging on PuO2 center dot xH(2)O particle size in alkaline solution SO RADIOCHIMICA ACTA LA English DT Article DE Hydrated plutonium oxide; Plutonium oxide; Particle size; Solubility; Hanford high-level waste; Aging ID PLUTONIUM DIOXIDE; SOLUBILITY AB Between 1944 and 1989, 54.5 metric tons of the United States' weapons-grade plutonium and an additional 12.9 metric tons of fuels-grade plutonium were produced in and separated from irradiated uranium metal fuel at the Hanford Site. Acidic high-activity wastes containing around 600 kg of plutonium were made alkaline and discharged to underground storage tanks from separations, isolation, and recycle processes to yield average plutonium concentration of about 0.003 g/L (or similar to 0.0002 wt. %) in the similar to 200 million liter tank waste volume. The plutonium is largely associated with low-solubility metal hydroxide/oxide sludges where its low concentration and intimate mixture with neutron-absorbing elements (e.g., iron) are credited in nuclear criticality safety. However, concerns have been expressed that plutonium, in the form of hydrated plutonium oxide, PuO2 center dot xH(2)O, could undergo sufficient crystal growth through dissolution and re-precipitation in the alkaline tank waste to potentially become separable from neutron absorbing constituents by settling or sedimentation. Thermodynamic considerations and laboratory studies of systems chemically analogous to tank waste show that the plutonium, precipitated in the alkaline tank waste by neutralization from acid solution, probably entered as 2-5-nm PuO2 center dot xH(2)O crystallite particles that, because of the low concentration of the neutral Pu(IV) dissolved species and opposition from radiolytic processes, grow from that point at exceedingly slow rates. C1 Pacific NW Natl Lab, Richland, WA 99352 USA. RP Delegard, CH (reprint author), Pacific NW Natl Lab, POB 999, Richland, WA 99352 USA. EM calvin.delegard@pnnl.gov OI Delegard, Calvin/0000-0001-6503-9502 NR 30 TC 5 Z9 5 U1 0 U2 12 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 5 BP 313 EP 322 DI 10.1524/ract.2013.2034 PG 10 WC Chemistry, Inorganic & Nuclear; Nuclear Science & Technology SC Chemistry; Nuclear Science & Technology GA 154ZS UT WOS:000319715800006 ER PT J AU Fassbender, ME Ballard, B Birnbaum, ER Engle, JW John, KD Maassen, JR Nortier, FM Lenz, JW Cutler, CS Ketring, AR Jurisson, SS Wilbur, DS AF Fassbender, M. E. Ballard, B. Birnbaum, E. R. Engle, J. W. John, K. D. Maassen, J. R. Nortier, F. M. Lenz, J. W. Cutler, C. S. Ketring, A. R. Jurisson, S. S. Wilbur, D. S. TI Proton irradiation parameters and chemical separation procedure for the bulk production of high-specific-activity Re-186g using WO3 targets SO RADIOCHIMICA ACTA LA English DT Article DE Rhenium-186; WO3 target; Proton induced reaction; High specific activity ID CARRIER-ADDED RE-186; EXCITATION-FUNCTIONS; NUCLEAR-REACTIONS; NATURAL TUNGSTEN; CYCLOTRON; RELEVANT; YIELDS AB Rhenium-186g (T-1/2 = 89.2 h) is a beta(-) emitter suitable for therapeutic applications. Current production methods rely on reactor production via Re-185 (n, gamma) which results in low specific activities, thereby limiting its use. Production by p, d activation of enriched W-186 results in a Re-186g product with a higher specific activity, allowing it to be used for targeted therapy with limited receptors. A test target consisting of pressed, sintered (WO3)-W-nat was proton irradiated at Los Alamos (LANL-IPF) to evaluate product yield and impurities, irradiation parameters and wet chemical Re recovery for proof-of-concept for bulk production of Re-186g. We demonstrated isolation of Re-186g in 97% yield from irradiated (WO3)-W-nat targets within 12 h of end of bombardment (BOB) via an alkaline dissolution followed by anion exchange. The recovery process has potential for automation, and WO3 can be easily recycled for recurrent irradiations. A Re-186g batch yield of 42.7 +/- 2.2 mu Ci/mu Ah or 439 +/- 23 MBq/C was obtained after 24 h in an 18.5 mu A proton beam. The target entrance energy was determined to be 15.6 MeV. The specific activity of Re-186g at BOB was measured to be 1.9 kCi (70.3 TBq) mmol(-1), which agrees well with the result of a previous Re-185,Re-186m coproduction EMPIRE and TALYS modeling study assuming similar conditions. Utilizing enriched (WO3)-W-186, we anticipate that a proton beam of 250 mu A for 24 h will provide batch yields of 256 mCi (9.5 GBq) of Re-186g at BOB with specific activities even higher than 1.9 kCi (70.3 TBq)mmol(-1), suitable for therapy applications. C1 [Fassbender, M. E.; Ballard, B.; Birnbaum, E. R.; Engle, J. W.; John, K. D.; Maassen, J. R.; Nortier, F. M.] Los Alamos Natl Lab, Div Chem, Los Alamos, NM 87545 USA. [Lenz, J. W.] John Lenz & Associates, E Lansing, MI 48823 USA. [Cutler, C. S.; Ketring, A. R.] Univ Missouri, Res Reactor Ctr, Columbia, MO 65211 USA. [Jurisson, S. S.] Univ Missouri, Dept Chem, Columbia, MO 65211 USA. [Wilbur, D. S.] Univ Washington, Radiochem Div, Seattle, WA 98105 USA. RP Fassbender, ME (reprint author), Los Alamos Natl Lab, Div Chem, POB 1663, Los Alamos, NM 87545 USA. EM mifa@lanl.gov RI Engle, Jonathan/D-7734-2012; Ballard, Beau/E-2925-2017 OI Ballard, Beau/0000-0003-1206-9358 FU United States Department of Energy, Office of Science via the Isotope Development and Production for Research and Applications subprogram in the Office of Nuclear Physics [DE-FOA-0000048] FX The authors would like to acknowledge the efforts of the LANL Isotope Production Facility and Hot Cell Facility personnel for their support in conducting target irradiations, target transportation, and for their general operational support. The study described in this paper was funded by the United States Department of Energy, Office of Science via an award from the Isotope Development and Production for Research and Applications subprogram in the Office of Nuclear Physics (Funding opportunity DE-FOA-0000048). NR 24 TC 15 Z9 15 U1 4 U2 15 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 5 BP 339 EP 346 DI 10.1524/ract.2013.2031 PG 8 WC Chemistry, Inorganic & Nuclear; Nuclear Science & Technology SC Chemistry; Nuclear Science & Technology GA 154ZS UT WOS:000319715800009 ER PT J AU Simpson, MF AF Simpson, Michael F. TI Projected Salt Waste Production from a Commercial Pyroprocessing Facility SO SCIENCE AND TECHNOLOGY OF NUCLEAR INSTALLATIONS LA English DT Article ID LIQUID CADMIUM CATHODE; MOLTEN-SALT; SPENT FUEL; ELECTROMETALLURGICAL TREATMENT; FORM; ACTINIDES; PRECIPITATION; REDUCTION; CHLORIDES; ELEMENTS AB Pyroprocessing of used nuclear fuel inevitably produces salt waste from electrorefining and/or oxide reduction unit operations. Various process design characteristics can affect the actual mass of such waste produced. This paper examines both oxide and metal fuel treatment, estimates the amount of salt waste generated, and assesses potential benefit of process options to mitigate the generation of salt waste. For reference purposes, a facility is considered in which 100 MT/year of fuel is processed. Salt waste estimates range from 8 to 20 MT/year from considering numerous scenarios. It appears that some benefit may be derived from advanced processes for separating fission products from molten salt waste, but the degree of improvement is limited. Waste form production is also considered but appears to be economically unfavorable. Direct disposal of salt into a salt basin type repository is found to be the most promising with respect to minimizing the impact of waste generation on the economic feasibility and sustainability of pyroprocessing. C1 Idaho Natl Lab, Idaho Falls, ID 83415 USA. RP Simpson, MF (reprint author), Idaho Natl Lab, POB 1625, Idaho Falls, ID 83415 USA. EM michael.simpson@inl.gov NR 17 TC 4 Z9 4 U1 1 U2 7 PU HINDAWI PUBLISHING CORPORATION PI NEW YORK PA 410 PARK AVENUE, 15TH FLOOR, #287 PMB, NEW YORK, NY 10022 USA SN 1687-6075 J9 SCI TECHNOL NUCL INS JI Sci. Technol. Nucl. Install. PY 2013 AR 945858 DI 10.1155/2013/945858 PG 8 WC Nuclear Science & Technology SC Nuclear Science & Technology GA 153IZ UT WOS:000319596400001 ER PT J AU Connors, JM Banks, JW Hittinger, JA Woodward, CS AF Connors, Jeffrey M. Banks, Jeffrey W. Hittinger, Jeffrey A. Woodward, Carol S. TI A METHOD TO CALCULATE NUMERICAL ERRORS USING ADJOINT ERROR ESTIMATION FOR LINEAR ADVECTION SO SIAM JOURNAL ON NUMERICAL ANALYSIS LA English DT Article DE a posteriori error; adjoint error; error estimation; hyperbolic conservation law ID FINITE-ELEMENT METHODS; ESSENTIALLY NONOSCILLATORY SCHEMES; HYPERBOLIC CONSERVATION-LAWS; MESH REFINEMENT; ADAPTIVITY; SIMULATIONS; EQUATIONS; SYSTEMS; VOLUME AB This paper is concerned with the computation of numerical discretization error for uncertainty quantification. An a posteriori error formula is described for a functional measurement of the solution to a scalar advection equation that is estimated by finite volume approximations. An exact error formula and computable error estimate are derived based on an abstractly defined approximation of the adjoint solution. The adjoint problem is divorced from the finite volume method used to approximate the forward solution variables and may be approximated using a low-order finite volume method. The accuracy of the computable error estimate provably satisfies an a priori error bound for sufficiently smooth solutions of the forward and adjoint problems. Computational examples are provided that show support of the theory for smooth solutions. The application to problems with discontinuities is also investigated computationally. C1 [Connors, Jeffrey M.; Banks, Jeffrey W.; Hittinger, Jeffrey A.; Woodward, Carol S.] Lawrence Livermore Natl Lab, Ctr Appl Sci Comp, Livermore, CA 94551 USA. RP Connors, JM (reprint author), Lawrence Livermore Natl Lab, Ctr Appl Sci Comp, Livermore, CA 94551 USA. EM connors4@llnl.gov; banks20@llnl.gov; hittinger1@llnl.gov; woodward6@llnl.gov RI Banks, Jeffrey/A-9718-2012; Woodward, Carol/M-4008-2014 FU U.S. Department of Energy; Lawrence Livermore National Laboratory (LLNL) [DE-AC52-07NA27344]; Uncertainty Quantification Strategic Initiative Laboratory Directed Research and Development Project at LLNL [10-SI-013, LLNL-JRNL-484291] FX This work was supported by the U.S. Department of Energy, by Lawrence Livermore National Laboratory (LLNL) under contract DE-AC52-07NA27344, and was funded by the Uncertainty Quantification Strategic Initiative Laboratory Directed Research and Development Project at LLNL under project tracking code 10-SI-013, LLNL-JRNL-484291. NR 33 TC 2 Z9 2 U1 0 U2 7 PU SIAM PUBLICATIONS PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA SN 0036-1429 EI 1095-7170 J9 SIAM J NUMER ANAL JI SIAM J. Numer. Anal. PY 2013 VL 51 IS 2 BP 894 EP 926 DI 10.1137/110845100 PG 33 WC Mathematics, Applied SC Mathematics GA 136ZZ UT WOS:000318405100007 ER PT J AU Hu, XZ Vassilevski, PS Xu, JC AF Hu, Xiaozhe Vassilevski, Panayot S. Xu, Jinchao TI COMPARATIVE CONVERGENCE ANALYSIS OF NONLINEAR AMLI-CYCLE MULTIGRID SO SIAM JOURNAL ON NUMERICAL ANALYSIS LA English DT Article DE multigrid; nonlinear AMLI-cycle multigrid; nonlinear preconditioned conjugate gradient method ID MULTILEVEL PRECONDITIONING METHODS; SMOOTHED AGGREGATION; VARIATIONAL-PROBLEMS; V-CYCLE; AMGE; ITERATION; SPACE AB The main purpose of this paper is to provide a comprehensive convergence analysis of the nonlinear algebraic multilevel iteration (AMLI)-cycle multigrid (MG) method for symmetric positive definite problems. Based on classical assumptions for approximation and smoothing properties, we show that the nonlinear AMLI-cycle MG method is uniformly convergent. Furthermore, under only the assumption that the smoother is convergent, we show that the nonlinear AMLI-cycle method is always better (or not worse) than the respective V-cycle MG method. Finally, numerical experiments are presented to illustrate the theoretical results. C1 [Hu, Xiaozhe; Xu, Jinchao] Penn State Univ, Dept Math, University Pk, PA 16802 USA. [Vassilevski, Panayot S.] Lawrence Livermore Natl Lab, Ctr Appl Sci Comp, Livermore, CA 94550 USA. RP Hu, XZ (reprint author), Penn State Univ, Dept Math, University Pk, PA 16802 USA. EM hu_x@math.psu.edu; panayot@llnl.gov; xu@math.psu.edu FU U.S. Department of Energy by Lawrence Livermore National Laboratory [DE-AC52-07NA27344]; NSF [DMS-0749202, DMS-0915153]; DOE [DE-SC0006903, B574178, B591217]; NSFC [91130011/A0117] 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.; The research of the third author was supported in part by NSF grants DMS-0749202 and DMS-0915153, DOE grant DE-SC0006903, DOE subcontracts B574178 and B591217, and NSFC grant 91130011/A0117. NR 33 TC 7 Z9 7 U1 0 U2 0 PU SIAM PUBLICATIONS PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA SN 0036-1429 J9 SIAM J NUMER ANAL JI SIAM J. Numer. Anal. PY 2013 VL 51 IS 2 BP 1349 EP 1369 DI 10.1137/110850049 PG 21 WC Mathematics, Applied SC Mathematics GA 136ZZ UT WOS:000318405100026 ER PT J AU Mitrica, B Goodman, M Szabelski, J AF Mitrica, Bogdan Goodman, Maury Szabelski, Jacek TI High Energy Physics in Underground Labs SO ADVANCES IN HIGH ENERGY PHYSICS LA English DT Editorial Material C1 [Mitrica, Bogdan] Horia Hulubei Natl Inst Phys & Nucl Engn, Magurele 077125, Romania. [Goodman, Maury] Argonne Natl Lab, Argonne, IL 60439 USA. [Szabelski, Jacek] Natl Ctr Nucl Res, PL-90137 Lodz, Poland. RP Mitrica, B (reprint author), Horia Hulubei Natl Inst Phys & Nucl Engn, Magurele 077125, Romania. EM mitrica@nipne.ro NR 0 TC 0 Z9 0 U1 1 U2 3 PU HINDAWI PUBLISHING CORPORATION PI NEW YORK PA 410 PARK AVENUE, 15TH FLOOR, #287 PMB, NEW YORK, NY 10022 USA SN 1687-7357 J9 ADV HIGH ENERGY PHYS JI Adv. High. Energy Phys. PY 2013 AR 180610 DI 10.1155/2013/180610 PG 2 WC Physics, Particles & Fields SC Physics GA 157SG UT WOS:000319918800001 ER PT J AU Kashif, MK Nippe, M Duffy, NW Forsyth, CM Chang, CJ Long, JR Spiccia, L Bach, U AF Kashif, Muhammad K. Nippe, Michael Duffy, Noel. W. Forsyth, Craig M. Chang, Christopher J. Long, Jeffrey R. Spiccia, Leone Bach, Udo TI Stable Dye-Sensitized Solar Cell Electrolytes Based on Cobalt(II)/(III) Complexes of a Hexadentate Pyridyl Ligand SO ANGEWANDTE CHEMIE-INTERNATIONAL EDITION LA English DT Article DE cobalt electrolytes; dye-sensitized solar cells; energy conversion; ligand engineering ID CHARGE RECOMBINATION; REDOX COUPLES; GENERATING HYDROGEN; ORGANIC-DYES; TIO2; EFFICIENCY; REGENERATION; PERFORMANCE; MEDIATORS; SHUTTLE C1 [Kashif, Muhammad K.; Bach, Udo] Monash Univ, Dept Mat Engn, Clayton, Vic 3800, Australia. [Nippe, Michael; Chang, Christopher J.; Long, Jeffrey R.] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Chang, Christopher J.] Univ Calif Berkeley, Dept Mol & Cell Biol, Berkeley, CA 94720 USA. [Chang, Christopher J.] Univ Calif Berkeley, Howard Hughes Med Inst, Berkeley, CA 94720 USA. [Nippe, Michael; Chang, Christopher J.; Long, Jeffrey R.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mat Chem Sci Div, Berkeley, CA 94720 USA. [Forsyth, Craig M.; Spiccia, Leone] Monash Univ, Dept Chem, Clayton, Vic 3800, Australia. [Bach, Udo] Melbourne Ctr Nanofabricat, Clayton, Vic 3168, Australia. [Bach, Udo] CSIRO, Mat Sci & Engn, Clayton, Vic 3169, Australia. [Duffy, Noel. W.] CSIRO, Energy Technol, Clayton, Vic 3169, Australia. RP Chang, CJ (reprint author), Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. EM chrischang@berkeley.edu; jrlong@berkeley.edu; leone.spiccia@monash.edu; udo.bach@monash.edu RI Duffy, Noel/G-5590-2010; Bach, Udo/F-3880-2012; Spiccia, Leone/I-8085-2013; Nippe, Michael/A-6222-2015 OI Duffy, Noel/0000-0001-9390-8402; Spiccia, Leone/0000-0003-2258-8506; Nippe, Michael/0000-0003-1091-4677 FU Australian Research Council; Australian Solar Institute, the Victorian State Government (DBI-VSA and DPI-ETIS); CSIRO; Office of Science of the U.S. Department of Energy [DE-SC0004993] FX The authors acknowledge the Australian Research Council for providing equipment and fellowship support and the Australian Solar Institute, the Victorian State Government (DBI-VSA and DPI-ETIS) for financial support. The CSIRO is acknowledged for providing support through an OCE Science Leader position (UB). Part of the synthetic work was carried out at the Joint Center for Artificial Photosynthesis supported by the Office of Science of the U.S. Department of Energy under award number DE-SC0004993. NR 49 TC 33 Z9 33 U1 12 U2 126 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 21 BP 5527 EP 5531 DI 10.1002/anie.201300070 PG 5 WC Chemistry, Multidisciplinary SC Chemistry GA 144HB UT WOS:000318929200015 PM 23606377 ER PT J AU Kundu, S Pfaff, FF Miceli, E Zaharieva, I Herwig, C Yao, SL Farquhar, ER Kuhlmann, U Bill, E Hildebrandt, P Dau, H Driess, M Limberg, C Ray, K AF Kundu, Subrata Pfaff, Florian Felix Miceli, Enrico Zaharieva, Ivelina Herwig, Christian Yao, Shenglai Farquhar, Erik R. Kuhlmann, Uwe Bill, Eckhard Hildebrandt, Peter Dau, Holger Driess, Matthias Limberg, Christian Ray, Kallol TI A High-Valent Heterobimetallic [Cu-III(mu-O)(2)Ni-III](2+) Core with Nucleophilic Oxo Groups SO ANGEWANDTE CHEMIE-INTERNATIONAL EDITION LA English DT Article DE bridging oxo ligands; copper; diamond core; nickel; nucleophilicity ID BIS(MU-OXO) COMPLEXES; DIOXYGEN ACTIVATION; ELECTRON-TRANSFER; COPPER PROTEINS; REACTIVITY; CONVERSION; NICKEL; SPECTROSCOPY; CHEMISTRY; SITES C1 [Kundu, Subrata; Pfaff, Florian Felix; Miceli, Enrico; Herwig, Christian; Limberg, Christian; Ray, Kallol] Humboldt Univ, Inst Chem, D-12489 Berlin, Germany. [Zaharieva, Ivelina; Dau, Holger] Free Univ Berlin, FB Phys, Berlin, Germany. [Yao, Shenglai; Kuhlmann, Uwe; Hildebrandt, Peter; Driess, Matthias] Tech Univ Berlin, Inst Chem, D-10623 Berlin, Germany. [Farquhar, Erik R.] Case Western Reserve Univ, Ctr Synchrotron Biosci, Cleveland, OH 44106 USA. [Farquhar, Erik R.] Brookhaven Natl Lab, Ctr Prote & Bioinformat, Upton, NY 11973 USA. [Bill, Eckhard] Max Plank Inst Chem Energiekonvers, Mulheim, Germany. RP Driess, M (reprint author), Tech Univ Berlin, Inst Chem, Str 17 Juni 135, D-10623 Berlin, Germany. EM matthias.driess@tu-berlin.de; christian.limberg@chemie.hu-berlin.de; kallol.ray@chemie.hu-berlin.de RI Zaharieva, Ivelina/H-6119-2012; Hildebrandt, Peter/J-5658-2014; Herwig, Christian/O-5946-2016; OI Zaharieva, Ivelina/0000-0002-4745-5307; Hildebrandt, Peter/0000-0003-1030-5900; Kundu, Subrata/0000-0002-3533-3206 FU Cluster of Excellence "Unifying Concepts in Catalysis", Berlin [EXC 314/1]; NIH [P30-EB-009998]; United States Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-98CH10886] FX We gratefully acknowledge financial support of this work from the Cluster of Excellence "Unifying Concepts in Catalysis" (EXC 314/1), Berlin. XAS data were obtained on beamline X3B of the National Synchrotron Light Source (Brookhaven National Laboratory) and beamline KMC-1 of BESSY, Berlin (Germany). Beamline X3B is operated by the Case Western Reserve University Center for Synchrotron Biosciences, supported by NIH Grant P30-EB-009998. NSLS is supported by the United States Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract DE-AC02-98CH10886. We also thank Prof. William B. Tolman for helpful suggestions. NR 37 TC 17 Z9 17 U1 3 U2 49 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 21 BP 5622 EP 5626 DI 10.1002/anie.201300861 PG 5 WC Chemistry, Multidisciplinary SC Chemistry GA 144HB UT WOS:000318929200036 PM 23589478 ER PT J AU Yang, X Post, WM Thornton, PE Jain, A AF Yang, X. Post, W. M. Thornton, P. E. Jain, A. TI The distribution of soil phosphorus for global biogeochemical modeling SO BIOGEOSCIENCES LA English DT Article ID HEDLEY FRACTIONATION; NEW-ZEALAND; NUTRIENT LIMITATION; TROPICAL FORESTS; IRON REDUCTION; MASS-BALANCE; RAIN-FOREST; CHRONOSEQUENCE; PEDOGENESIS; CARBON AB Phosphorus (P) is a major element required for biological activity in terrestrial ecosystems. Although the total P content in most soils can be large, only a small fraction is available or in an organic form for biological utilization because it is bound either in incompletely weathered mineral particles, adsorbed on mineral surfaces, or, over the time of soil formation, made unavailable by secondary mineral formation (occluded). In order to adequately represent phosphorus availability in global biogeochemistry-climate models, a representation of the amount and form of P in soils globally is required. We develop an approach that builds on existing knowledge of soil P processes and databases of parent material and soil P measurements to provide spatially explicit estimates of different forms of naturally occurring soil P on the global scale. We assembled data on the various forms of phosphorus in soils globally, chronosequence information, and several global spatial databases to develop a map of total soil P and the distribution among mineral bound, labile, organic, occluded, and secondary P forms in soils globally. The amount of P, to 50cm soil depth, in soil labile, organic, occluded, and secondary pools is 3.6 +/- 3, 8.6 +/- 6, 12.2 +/- 8, and 3.2 +/- 2 Pg P (Petagrams of P, 1 Pg = 1x10(15)g) respectively. The amount in soil mineral particles to the same depth is estimated at 13.0 +/- 8 Pg P for a global soil total of 40.6 +/- 18 Pg P. The large uncertainty in our estimates reflects our limited understanding of the processes controlling soil P transformations during pedogenesis and a deficiency in the number of soil P measurements. In spite of the large uncertainty, the estimated global spatial variation and distribution of different soil P forms presented in this study will be useful for global biogeochemistry models that include P as a limiting element in biological production by providing initial estimates of the available soil P for plant uptake and microbial utilization. C1 [Yang, X.; Post, W. M.; Thornton, P. E.] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. [Jain, A.] Univ Illinois, Urbana, IL 61801 USA. RP Yang, X (reprint author), Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. EM yangx2@ornl.gov RI Thornton, Peter/B-9145-2012; Yang, Xiaojuan/I-3643-2016; Jain, Atul/D-2851-2016 OI Thornton, Peter/0000-0002-4759-5158; Yang, Xiaojuan/0000-0002-2686-745X; Jain, Atul/0000-0002-4051-3228 FU US Department of Energy, Office of Science, Biological and Environmental Research (BER); US Department of Energy [DE-AC05-00OR22725]; NASA [NNX08AK75G]; Office of Science (BER), US Department of Energy [DOE-DE-SC0006706] FX This research was sponsored by the US Department of Energy, Office of Science, Biological and Environmental Research (BER) programs and performed at Oak Ridge National Laboratory (ORNL). ORNL is managed by UT-Battelle, LLC, for the US Department of Energy under Contract No. DE-AC05-00OR22725. We are grateful to Hans H. Durr for providing us the lithology data. We would like to thank Beto Quesada for his comments to improve the total P spatial pattern in Amazonia. AKJ is funded by the NASA LCLUC Program (No. NNX08AK75G) and the Office of Science (BER), US Department of Energy (DOE-DE-SC0006706). NR 51 TC 24 Z9 24 U1 8 U2 80 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1726-4170 J9 BIOGEOSCIENCES JI Biogeosciences PY 2013 VL 10 IS 4 BP 2525 EP 2537 DI 10.5194/bg-10-2525-2013 PG 13 WC Ecology; Geosciences, Multidisciplinary SC Environmental Sciences & Ecology; Geology GA 137KH UT WOS:000318434200024 ER PT J AU Bailey, DH Borwein, JM AF Bailey, David H. Borwein, Jonathan M. TI Compressed lattice sums arising from the Poisson equation SO BOUNDARY VALUE PROBLEMS LA English DT Article DE lattice sums; Poisson equation; experimental mathematics; high-precision computation ID INFINITE SERIES; PRODUCTS AB Purpose: In recent years attention has been directed to the problem of solving the Poisson equation, either in engineering scenarios (computational) or in regard to crystal structure (theoretical). Methods: In (Bailey et al. in J. Phys. A, Math. Theor. 46:115201, 2013, doi:10.1088/1751-8113/46/11/115201) we studied a class of lattice sums that amount to solutions of Poisson's equation, utilizing some striking connections between these sums and Jacobi I-function values, together with high-precision numerical computations and the PSLQ algorithm to find certain polynomials associated with these sums. We take a similar approach in this study. Results: We were able to develop new closed forms for certain solutions and to extend such analysis to related lattice sums. We also alluded to results for the compressed sum phi(2)(x,y,d) :=1/pi(2) Sigma(m,n is an element of O) cos(pi mx)cos(pi n root dy)/m(2) + dn(2) , (1) where , x, y are real numbers and denotes the odd integers. In this paper we first survey the earlier work and then discuss the sum (1) more completely. Conclusions: As in the previous study, we find some surprisingly simple closed-form evaluations of these sums. In particular, we find that in some cases these sums are given by , where A is an algebraic number. These evaluations suggest that a deep theory interconnects all such summations. : C1 [Bailey, David H.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Borwein, Jonathan M.] Univ Newcastle, Ctr Comp Assisted Res Math & Its Applicat CARMA, Callaghan, NSW 2308, Australia. RP Borwein, JM (reprint author), Univ Newcastle, Ctr Comp Assisted Res Math & Its Applicat CARMA, Callaghan, NSW 2308, Australia. EM jonathan.borwein@newcastle.edu.au FU Office of Computational and Technology Research, Division of Mathematical, Information, and Computational Sciences of the U.S. Department of Energy [DE-AC02-05CH11231]; Australian Research Council FX The authors thank many colleagues and the referees for fruitful discussions about lattice sums and theta functions. The first author supported in part by the Director, Office of Computational and Technology Research, Division of Mathematical, Information, and Computational Sciences of the U.S. Department of Energy, under contract number DE-AC02-05CH11231. The second author is supported in part by the Australian Research Council. NR 22 TC 0 Z9 0 U1 1 U2 5 PU SPRINGER INTERNATIONAL PUBLISHING AG PI CHAM PA GEWERBESTRASSE 11, CHAM, CH-6330, SWITZERLAND SN 1687-2770 J9 BOUND VALUE PROBL JI Bound. Value Probl. PY 2013 AR 75 DI 10.1186/1687-2770-2013-75 PG 18 WC Mathematics, Applied; Mathematics SC Mathematics GA 149BP UT WOS:000319293300001 ER PT J AU Chandrasekaran, A Deng, K Koh, CY Takasuka, T Bergeman, LF Fox, BG Adams, PD Singh, AK AF Chandrasekaran, Aarthi Deng, Kai Koh, Chung-Yan Takasuka, Taichi Bergeman, Lai F. Fox, Brian G. Adams, Paul D. Singh, Anup K. TI A universal flow cytometry assay for screening carbohydrate-active enzymes using glycan microspheres SO CHEMICAL COMMUNICATIONS LA English DT Article ID GLYCOSYLTRANSFERASES; LIGATION; BIOSYNTHESIS AB We describe a simple, multiplexed assay that integrates glycan synthesis, bioconjugation to microspheres, fluorescent chemical/biochemical detection and multiparameter flow cytometric analysis to screen activities of different families of carbohydrate-active enzymes. C1 [Chandrasekaran, Aarthi; Deng, Kai; Adams, Paul D.; Singh, Anup K.] Joint BioEnergy Inst, Div Technol, Emeryville, CA USA. [Chandrasekaran, Aarthi; Deng, Kai; Koh, Chung-Yan; Singh, Anup K.] Sandia Natl Labs, Biotechnol & Bioengn Dept, Livermore, CA USA. [Takasuka, Taichi; Bergeman, Lai F.; Fox, Brian G.] Univ Wisconsin, Great Lakes Bioenergy Res Ctr, Madison, WI USA. [Adams, Paul D.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA 94720 USA. RP Chandrasekaran, A (reprint author), Joint BioEnergy Inst, Div Technol, Emeryville, CA USA. EM achandrasekaran@lbl.gov; aksingh@sandia.gov RI Adams, Paul/A-1977-2013 OI Adams, Paul/0000-0001-9333-8219 FU US DOE, Office of Science, Office of Biological and Environmental Research [DE-AC02-05 CH11231, DE-FC02-07ER64494]; US DOE's Nuclear Security Administration [DE-AC04-94AL85000] FX The authors thank Dr. Rajiv Bharadwaj for insightful scientific discussions and Prof. Richmond Sarpong of UC Berkeley for using the instruments in his group. Work at the DOE Joint BioEnergy Institute and DOE Great Lakes Bioenergy Research Center (GLBRC) is supported by the US DOE, Office of Science, Office of Biological and Environmental Research, through contracts DE-AC02-05 CH11231 (LBNL) and DE-FC02-07ER64494 (GLBRC). Sandia is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for US DOE's Nuclear Security Administration under contract DE-AC04-94AL85000. NR 20 TC 0 Z9 0 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 48 BP 5441 EP 5443 DI 10.1039/c3cc39155h PG 3 WC Chemistry, Multidisciplinary SC Chemistry GA 148EU UT WOS:000319226700001 PM 23536035 ER PT J AU Mathew, KJ O'Connor, G Hasozbek, A Kraiem, M AF Mathew, K. J. O'Connor, G. Hasozbek, A. Kraiem, M. TI Total evaporation method for uranium isotope-amount ratio measurements SO JOURNAL OF ANALYTICAL ATOMIC SPECTROMETRY LA English DT Article ID IONIZATION MASS-SPECTROMETRY; PLUTONIUM; SAMPLES; UNCERTAINTY; TIMS AB Total evaporation (TE) is an analysis technique for the measurement of uranium isotopic abundance ratios using thermal ionization mass spectrometry (TIMS). A small mass dependent bias observed in this analytical technique is determined by an external correction factor using well characterized standards (most often certified reference materials, CRMs). The technique had been demonstrated to be highly precise and accurate for major isotope-amount ratio measurements of uranium and plutonium. We compare the performance of the TE analytical technique for uranium isotope ratio measurements on two TIMS instruments (TRITON and MAT261) using well characterized CRMs from NBL and investigate the dependence of the instrumental mass bias on the amount of sample analyzed. It is concluded that the mass bias during a TIMS uranium isotopic analysis by TE is independent of the amount of material analyzed. Unlike the major ratio, minor isotope ratio measurements by TE are biased high due to peak-tailing from the major isotopes. The biases in the minor isotope ratio data using TE are evaluated using well characterized NBL CRMs. C1 [Mathew, K. J.; O'Connor, G.; Hasozbek, A.; Kraiem, M.] US DOE, New Brunswick Lab, Argonne, IL 60439 USA. RP Mathew, KJ (reprint author), US DOE, New Brunswick Lab, 9800 South Cass Ave,Bldg 350, Argonne, IL 60439 USA. EM kattathu.mathew@ch.doe.gov RI Hasozbek, Altug/A-8788-2010 OI Hasozbek, Altug/0000-0001-8846-0412 NR 23 TC 12 Z9 12 U1 3 U2 19 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 0267-9477 J9 J ANAL ATOM SPECTROM JI J. Anal. At. Spectrom. PY 2013 VL 28 IS 6 BP 866 EP 876 DI 10.1039/c2ja30321c PG 11 WC Chemistry, Analytical; Spectroscopy SC Chemistry; Spectroscopy GA 144MR UT WOS:000318944300008 ER PT J AU Eguchi, H Hirata, K Kurotani, R Fukumura, H Singh, D Yamamoto, M Sato, I Umemura, M Yamamoto, M Sato, M Ishikawa, Y AF Eguchi, Haruki Hirata, Kunio Kurotani, Reiko Fukumura, Hidenobu Singh, David Yamamoto, Masahiro Sato, Itaru Umemura, Masanori Yamamoto, Masaki Sato, Mamoru Ishikawa, Yoshihiro TI Controlled drug delivery and magnetic resonance imaging with intrinsic ferromagnetic nano-particle compound SO JOURNAL OF PHARMACOLOGICAL SCIENCES LA English DT Meeting Abstract CT 86th Annual Meeting of the Japanese-Pharmacological-Society CY MAR 21-23, 2013 CL Fukuoka, JAPAN SP Japanese Pharmacol Soc C1 [Eguchi, Haruki] Res Lab IHI, Isogo Ku, Yokohama, Kanagawa 2358501, Japan. [Hirata, Kunio; Yamamoto, Masaki] RIKEN SPring8, Hyogo 6795184, Japan. [Kurotani, Reiko] Yamagata Univ, Fac Engn, Yonezawa, Yamagata 992, Japan. [Fukumura, Hidenobu; Sato, Itaru; Umemura, Masanori; Ishikawa, Yoshihiro] Yokohama City Univ, Grad Sch Med, Yokohama, Kanagawa 232, Japan. [Singh, David] Oak Ridge Natl Lab, Oak Ridge, TN USA. [Yamamoto, Masaki] Fac Sci & Engn, Kobe, Hyogo, Japan. [Sato, Mamoru] Int Grad Sch Arts & Sci, Yokohama, Kanagawa, Japan. RI Yamamoto, Masaki/B-7844-2015 OI Yamamoto, Masaki/0000-0002-1311-1768 NR 0 TC 0 Z9 0 U1 0 U2 3 PU JAPANESE PHARMACOLOGICAL SOC PI KYOTO PA EDITORIAL OFF, KANTOHYA BLDG GOKOMACHI-EBISUGAWA NAKAGYO-KU, KYOTO, 604, JAPAN SN 1347-8613 J9 J PHARMACOL SCI JI J. Pharmacol. Sci. PY 2013 VL 121 SU 1 BP 125P EP 125P PG 1 WC Pharmacology & Pharmacy SC Pharmacology & Pharmacy GA 151WL UT WOS:000319491000419 ER PT J AU Weed, AMK Dvornik, J Stefancin, JJ Gyapong, AA Svec, F Zajickova, Z AF Weed, Anna-Marie Karen Dvornik, Jill Stefancin, John Jacob Gyapong, Afua Asantewaa Svec, Frantisek Zajickova, Zuzana TI Photopolymerized organo-silica hybrid monolithic columns: Characterization of their performance in capillary liquid chromatography SO JOURNAL OF SEPARATION SCIENCE LA English DT Article DE Hybrid; Monolith; Organo-silica; Photopolymerization; Sol-gel ID SOL-GEL MONOLITHS; MASS-SPECTROMETRY; SURFACE MODIFICATION; HIGH-EFFICIENCY; ELECTROCHROMATOGRAPHY; SEPARATION; HPLC; PHASE; METHACRYLATE; BEHAVIOR AB Porous hybrid organo-silica monoliths have been prepared inside pretreated 100 mu m id UV transparent fused-silica capillaries using simultaneous sol-gel transition and polymerization of 3-(methacryloyloxy) propyl trimethoxysilane in the presence of toluene as a porogen. The sol-gel reaction was catalyzed by hydrochloric acid while various photoinitiators including azobisisobutyronitrile, 2,2-dimethoxy-2-phenylacetophenone, and Irgacure 819 were used for the photopolymerization carried out under irradiation with UV light at a wavelength of 254 or 365 nm. The chromatographic performance of photopolymerized monolithic columns in RP liquid chromatographic mode was assessed with respect to the following metrics: column efficiency, methylene and steric selectivity, effect of silanol groups, van Deemter plot, permeability, and pore size distribution. Columns with an efficiency of up to 77 000 plates/m for benzene has been achieved at a flow velocity of 0.47 mm/s. The performance of photopolymerized hybrid monolithic column was compared to the performance of columns prepared via thermally initiated polymerization. C1 [Weed, Anna-Marie Karen; Dvornik, Jill; Stefancin, John Jacob; Gyapong, Afua Asantewaa; Zajickova, Zuzana] Barry Univ, Dept Phys Sci, Miami Shores, FL 33161 USA. [Svec, Frantisek] EO Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA USA. RP Zajickova, Z (reprint author), Barry Univ, Dept Phys Sci, 11300 NE 2nd Ave, Miami Shores, FL 33161 USA. EM ZZajickova@mail.barry.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]; Department of Energy (DOE)/National Science Foundation (NSF) Faculty and Student Team (FaST) Program; National Science Foundation [CBET-1066113] FX Experimental work carried out at the Molecular Foundry, Lawrence Berkeley National Laboratory and F. S. were supported by the Office of Science, Office of Basic Energy Sciences of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. J.S. and Z.Z. were supported by the Department of Energy (DOE)/National Science Foundation (NSF) Faculty and Student Team (FaST) Program. A-M. W., J.D., A. G., and Z.Z. were also supported by the National Science Foundation CBET-1066113. Jiri Urban and Jana Krenkova are kindly acknowledged for their valuable suggestions helping implementation of this project. NR 33 TC 15 Z9 15 U1 2 U2 50 PU WILEY-V C H VERLAG GMBH PI WEINHEIM PA POSTFACH 101161, 69451 WEINHEIM, GERMANY SN 1615-9306 EI 1615-9314 J9 J SEP SCI JI J. Sep. Sci. PD JAN PY 2013 VL 36 IS 2 BP 270 EP 278 DI 10.1002/jssc.201200760 PG 9 WC Chemistry, Analytical SC Chemistry GA 156YE UT WOS:000319859500007 PM 23212714 ER PT J AU Bonner, IJ Kenney, KL AF Bonner, Ian J. Kenney, Kevin L. TI Moisture sorption characteristics and modeling of energy sorghum (Sorghum bicolor (L.) Moench) SO JOURNAL OF STORED PRODUCTS RESEARCH LA English DT Article DE Sorghum bicolor; Aerobic storage; Dynamic dew-point isotherm; Equilibrium moisture content; Monolayer moisture; Heat of sorption ID SWEET SORGHUM; THERMODYNAMIC PROPERTIES; ISOSTERIC HEATS; WATER ACTIVITY; ADSORPTION; STORAGE; DESORPTION; BIOETHANOL; FEEDSTOCK; SYSTEMS AB Long-term low cost storage of whole-stalk lignocellulosic energy sorghum biomass (specialized forage varieties of Sorghum bicolor (L) Moench) is essential for the feedstock's successful role as a dedicated energy crop for ethanol production. As an alternative to expensive ensiling methods, aerobic storage of S. bicolor (L) Moench biomass in traditional rectangular bale formats could alleviate feedstock supply costs if material deterioration in storage could be minimized. Moisture desorption and adsorption isotherms for S. bicolor (L) Moench were created at 15 degrees C, 20 degrees C, 30 degrees C, and 40 degrees C with water activities from 0.1 to 0.9 using the dynamic dew-point method. Sorption isotherms were modeled using four temperature dependent and three temperature independent equations. The relationship between equilibrium moisture content and water activity was found to decrease with increasing temperatures. GAB (Guggenheim-Anderson-de Boer) monolayer moisture content and the moisture content at which microbial activity becomes limited were found to range from 5.6% db to 10.4% dry basis (db) and 12.0% db to 18.4% db, respectively. The net isosteric heat of sorption was calculated using the Clausius-Clapeyron equation and determined to be higher for desorption than adsorption with both trends decreasing exponentially at increasing levels of moisture content. The differential entropy of S. bicolor (L) Moench was shown to exhibit a log normal relationship with moisture; peaking near the monolayer moisture content. The results of the study indicate that aerobic storage of energy sorghum biomass may be similar to other herbaceous feedstocks should extensive drying occur before entering storage. (c) 2012 Elsevier Ltd. All rights reserved. C1 [Bonner, Ian J.; Kenney, Kevin L.] Idaho Natl Lab, Idaho Falls, ID 83415 USA. RP Bonner, IJ (reprint author), Idaho Natl Lab, POB 1625, Idaho Falls, ID 83415 USA. EM ian.bonner@inl.gov FU U.S. Department of Energy, under DOE Idaho Operations Office [DE-AC07-05ID14517]; U.S. Government FX This work is supported by the U.S. Department of Energy, under DOE Idaho Operations Office Contract DE-AC07-05ID14517. Accordingly, the U.S. Government retains a nonexclusive, royalty-free license to publish or reproduce the published form of 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 is 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 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 44 TC 9 Z9 9 U1 0 U2 15 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0022-474X J9 J STORED PROD RES JI J. Stored Prod. Res. PD JAN PY 2013 VL 52 BP 128 EP 136 DI 10.1016/j.jspr.2012.11.002 PG 9 WC Entomology SC Entomology GA 150BU UT WOS:000319366000021 ER PT J AU Borkiewicz, OJ Chapman, KW Chupas, PJ AF Borkiewicz, Olaf J. Chapman, Karena W. Chupas, Peter J. TI Mapping spatially inhomogeneous electrochemical reactions in battery electrodes using high energy X-rays SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID LITHIUM-ION BATTERIES; CONVERSION REACTION AB The spatial distribution of a reaction through a lithium-ion battery electrode has been resolved using micro-beam high-energy X-ray scattering measurements coupled with Pair Distribution Function (PDF) analysis. The electrochemical reaction was most advanced at the interface between the electrode and electrolyte-soaked separator, with linear variation in reaction progress with distance from this interface. C1 [Borkiewicz, Olaf J.; Chapman, Karena W.; Chupas, Peter J.] Argonne Natl Lab, Adv Photon Source, Xray Sci Div, Argonne, IL 60439 USA. RP Chapman, KW (reprint author), Argonne Natl Lab, Adv Photon Source, Xray Sci Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM chapmank@aps.anl.gov; chupas@aps.anl.gov FU Northeastern Center for Chemical Energy Storage, an Energy Frontier Research Center; U.S. DOE, BES [DE-SC0001294]; U.S. DOE [DE-AC02-06CH11357] FX This work was supported by the Northeastern Center for Chemical Energy Storage, an Energy Frontier Research Center funded by the U.S. DOE, BES under award No. DE-SC0001294. Work done at Argonne and use of the Advanced Photon Source, an Office of Science User Facility operated for the U.S. DOE Office of Science by Argonne National Laboratory, were supported by the U.S. DOE under Contract No. DE-AC02-06CH11357. NR 16 TC 4 Z9 4 U1 0 U2 52 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 22 BP 8466 EP 8469 DI 10.1039/c3cp50590a PG 4 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 145HN UT WOS:000319006100003 PM 23598687 ER PT J AU Yang, XH Masadeh, AS McBride, JR Bozin, ES Rosenthal, SJ Billinge, SJL AF Yang, Xiaohao Masadeh, Ahmad S. McBride, James R. Bozin, Emil S. Rosenthal, Sandra J. Billinge, Simon J. L. TI Confirmation of disordered structure of ultrasmall CdSe nanoparticles from X-ray atomic pair distribution function analysis SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID CADMIUM SELENIDE NANOCRYSTALS; WHITE-LIGHT EMISSION; DIFFRACTION DATA; TRANSFORMATION AB The atomic pair distribution function (PDF) analysis of X-ray powder diffraction data has been used to study the structure of small and ultra-small CdSe nanoparticles. A method is described that uses a wurtzite and zinc-blende mixed phase model to account for stacking faults in CdSe particles. The mixed-phase model successfully describes the structure of nanoparticles larger than 2 nm yielding a stacking fault density of about 30%. However, for ultrasmall nanoparticles smaller than 2 nm, the models cannot fit the experimental PDF showing that the structure is significantly modified from that of larger particles and the bulk. The observation of a significant change in the average structure at ultra-small size is likely to explain the unusual properties of the ultrasmall particles such as their white light emitting ability. C1 [Yang, Xiaohao; Billinge, Simon J. L.] Columbia Univ, Dept Appl Phys & Appl Math, New York, NY 10027 USA. [Masadeh, Ahmad S.] Univ Jordan, Dept Phys, Amman 11942, Jordan. [McBride, James R.; Rosenthal, Sandra J.] Vanderbilt Univ, Dept Chem, Nashville, TN 37235 USA. [Bozin, Emil S.; Billinge, Simon J. L.] Brookhaven Natl Lab, Condensed Matter Phys & Mat Sci Dept, Upton, NY 11973 USA. RP Billinge, SJL (reprint author), Columbia Univ, Dept Appl Phys & Appl Math, New York, NY 10027 USA. EM sb2896@columbia.edu RI Yang, Xiaohao/H-3977-2013; McBride, James/D-2934-2012 OI Yang, Xiaohao/0000-0001-6136-3575; McBride, James/0000-0003-0161-7283 FU Center for Re-Defining Photovoltaic Efficiency Through Molecule Scale Control, an Energy Frontier Research Center; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001085]; U.S. DOE, Office of Science, Office of Basic Energy Sciences [W-31-109-Eng-38] FX We would like to acknowledge help from Pavol Juhas, Mouath Shatnawi, HyunJeong Kim and Christos Malliakas for help in collecting data. The X-ray data collection and analysis were supported as part of the Center for Re-Defining Photovoltaic Efficiency Through Molecule Scale Control, 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-SC0001085. Data were collected at the 6IDD beamline of the MUCAT sector at the Advanced Photon Source (APS). Use of the APS is supported by the U.S. DOE, Office of Science, Office of Basic Energy Sciences, under Contract No. W-31-109-Eng-38. NR 36 TC 19 Z9 19 U1 2 U2 41 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2013 VL 15 IS 22 BP 8480 EP 8486 DI 10.1039/c3cp00111c PG 7 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 145HN UT WOS:000319006100005 PM 23525376 ER PT J AU Bytchkov, A Cuello, GJ Kohara, S Benmore, CJ Price, DL Bychkov, E AF Bytchkov, Aleksei Cuello, Gabriel J. Kohara, Shinji Benmore, Chris J. Price, David L. Bychkov, Eugene TI Unraveling the atomic structure of Ge-rich sulfide glasses SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID NEUTRON-DIFFRACTION; RANGE ORDER; AMORPHOUS SOLIDS; BINARY GLASSES; S GLASSES; X-RAY; CHALCOGENIDE; SCATTERING; SYSTEMS; ALLOYS AB In contrast to the well-established structure of glassy GeS2, consisting of corner- and edge-sharing GeS4/2 tetrahedra, the structural features of Ge-rich sulfide alloys remain essentially unknown. Two contrasting points of view: (1) a tetrahedral model, and (2) a distorted NaCl approach were neither confirmed nor excluded mostly because of missing advanced structural studies. Using high-energy X-ray scattering and neutron diffraction, we show the complexity of the short and intermediate range order in GexS1-x glasses, 1/3 <= x <= 0.47, formed by corner- and edge-sharing tetrahedra with two-fold coordinated sulfur species and a variable number of Ge-Ge bonds, and Ge-S units with three-fold coordinated sulfur at x >= 0.36. C1 [Bytchkov, Aleksei; Bychkov, Eugene] Univ Littoral, F-59140 Dunkerque, France. [Bytchkov, Aleksei; Cuello, Gabriel J.] Inst Max Von Laue Paul Langevin, F-38042 Grenoble, France. [Kohara, Shinji] Japan Synchrotron Radiat Res Inst, Sayo, Hyogo 6795198, Japan. [Benmore, Chris J.] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. [Price, David L.] Univ Orleans, F-45071 Orleans 2, France. RP Bytchkov, A (reprint author), Univ Littoral, F-59140 Dunkerque, France. EM bytchkov@ill.fr RI Cuello, Gabriel/C-5831-2009; bytchkov, aleksei/F-2609-2012; OI Cuello, Gabriel/0000-0003-3844-0602; Benmore, Chris/0000-0001-7007-7749 FU Centre for Advanced Science and Technology (Japan); U.S. Department of Energy, Office of Science [DE-AC02-06CH11357]; European Commission FX The authors are grateful to M. Fourmentin, V. Tsegelnik and M. Bokova for glass synthesis, M. Milochova for DSC measurements, and D. Bowron for help with neutron diffraction measurements. The experiments at the SPring-8 were approved by the Japan Synchrotron Radiation Research Institute and supported by the Centre for Advanced Science and Technology (Japan). The work at Argonne was supported by the U.S. Department of Energy, Office of Science, under Contract No. DE-AC02-06CH11357. The work at the Universite du Littoral (France) was supported by the European Commission within the Interreg IIIA and IVA programs (CTMM and CleanTech projects). NR 51 TC 11 Z9 11 U1 0 U2 23 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 22 BP 8487 EP 8494 DI 10.1039/c3cp50536g PG 8 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 145HN UT WOS:000319006100006 PM 23615750 ER PT J AU Petkov, V Ren, Y Kabekkodu, S Murphy, D AF Petkov, V. Ren, Y. Kabekkodu, S. Murphy, D. TI Atomic pair distribution functions analysis of disordered low-Z materials SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID X-RAY-DIFFRACTION; CRYSTAL-STRUCTURE; SCATTERING; FILMS; WATER AB Results of high-energy X-ray diffraction experiments coupled to atomic pair distribution function analysis of disordered low-Z materials are presented. Several scientifically and technologically important classes of disordered low-Z materials such as small and large organic molecules, graphitic powders, polymers and liquids are intentionally explored to certify the technique's performance. Results clearly show that disordered low-Z materials can be well characterized in terms of material's phase identity, relative abundance in mixtures and atomic-scale structure. The demonstrated efficiency of the technique provides the scientific community with much needed confidence to apply it more often than now. C1 [Petkov, V.] Cent Michigan Univ, Dept Phys, Mt Pleasant, MI 48859 USA. [Ren, Y.] Argonne Natl Lab, Adv Photon Source, Xray Sci Div, Argonne, IL 60439 USA. [Kabekkodu, S.] Int Ctr Diffract Data, Newtown Sq, PA 19073 USA. [Murphy, D.] Bristol Myers Squibb Co, Drug Prod Sci & Technol, New Brunswick, NJ 08903 USA. RP Petkov, V (reprint author), Cent Michigan Univ, Dept Phys, Mt Pleasant, MI 48859 USA. EM petko1vg@cmich.edu FU DOE [DE-AC02-06CH11357] FX VP acknowledges help from DOE via DE-SC0006877, NSF and ARL. Work at APS has been supported by DOE under Contract DE-AC02-06CH11357. NR 28 TC 9 Z9 9 U1 0 U2 25 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 22 BP 8544 EP 8554 DI 10.1039/c2cp43378h PG 11 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 145HN UT WOS:000319006100011 PM 23318354 ER PT J AU Skinner, LB Benmore, CJ Weber, JKR Wilding, MC Tumber, SK Parise, JB AF Skinner, L. B. Benmore, C. J. Weber, J. K. R. Wilding, M. C. Tumber, S. K. Parise, J. B. TI A time resolved high energy X-ray diffraction study of cooling liquid SiO2 SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID VITREOUS SILICA; SCATTERING FACTORS; TEMPERATURE; GLASSES; NEUTRON AB The evolution of the X-ray structure factor and corresponding pair distribution function of SiO2 has been measured upon cooling from the melt using high energy X-ray diffraction combined with aerodynamic levitation. Small changes in the position of the average Si-O bond distance and peak width are found to occur at similar to 1500(100) K in the region of the calorimetric glass transition temperature, T-g and the observed density minima. At higher temperatures deviations from linear behavior are seen in the first sharp diffraction peak width, height and area at around 1750(50) K, which coincides with the reported density maximum around 1.2T(g). C1 [Skinner, L. B.; Benmore, C. J.; Weber, J. K. R.] Argonne Natl Lab, Adv Photon Source, Xray Sci Div, Argonne, IL 60439 USA. [Skinner, L. B.; Parise, J. B.] SUNY Stony Brook, Inst Mineral Phys, Stony Brook, NY 11794 USA. [Weber, J. K. R.; Tumber, S. K.] Mat Dev Inc, Arlington Hts, IL 60004 USA. [Wilding, M. C.] Univ Wales, Inst Math & Phys Sci, Aberystwyth SY23 3BZ, Cerdigion, Wales. [Parise, J. B.] SUNY Stony Brook, Dept Geosci, New York, NY 11794 USA. [Parise, J. B.] Brookhaven Natl Lab, Photon Sci Div, Upton, NY 11973 USA. RP Benmore, CJ (reprint author), Argonne Natl Lab, Adv Photon Source, Xray Sci Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM benmore@aps.anl.gov RI Skinner, Lawrie/I-2603-2012 OI Benmore, Chris/0000-0001-7007-7749; Skinner, Lawrie/0000-0001-7317-1642 FU US DOE Argonne National Laboratory [DE-AC02-06CH11357]; [DE-SC0004684]; [DE-SC0007564] FX Rick Spence is thanked for help with setting up the levitation equipment on beamline 11-ID-C at the APS. This work was supported by the US DOE Argonne National Laboratory under contract number DE-AC02-06CH11357. Grants DE-SC0004684, DE-SC0007564 supported JBP and LS, and DE-FG02-09ER46650 supported data collection and analysis. NR 25 TC 5 Z9 5 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 22 BP 8566 EP 8572 DI 10.1039/c3cp44347g PG 7 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 145HN UT WOS:000319006100013 PM 23588490 ER PT J AU White, CE Provis, JL Bloomer, B Henson, NJ Page, K AF White, Claire E. Provis, John L. Bloomer, Breaunnah Henson, Neil J. Page, Katharine TI In situ X-ray pair distribution function analysis of geopolymer gel nanostructure formation kinetics SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID MONTE-CARLO-SIMULATION; C-S-H; LOCAL-STRUCTURE; ZEOLITE SYNTHESIS; METAKAOLIN; EVOLUTION; CONCRETE; BLENDS; BINDER; MICROSTRUCTURE AB With the ever-increasing environmentally-driven demand for technologically advanced structural materials, geopolymer cement is fast becoming a viable alternative to traditional cements due to its proven engineering characteristics and the reduction in CO2 emitted during manufacturing (as much as 80% less CO2 emitted in manufacture, compared to ordinary Portland cement). Nevertheless, much remains unknown regarding the kinetics of reaction responsible for nanostructural evolution during the geopolymerisation process. Here, in situ X-ray total scattering measurements and pair distribution function (PDF) analysis are used to quantify the extent of reaction as a function of time for alkali-activated metakaolin/slag geopolymer binders, including the impact of various activators (alkali hydroxide/silicate) on the kinetics of the geopolymerisation reaction. Quantifying the reaction process in situ from X-ray PDF data collected during the initial ten hours can provide an estimate of the total reaction extent, but when combined with data obtained at longer times (128 days here) enables more accurate determination of the overall rate of reaction. To further assess the initial stages of the geopolymerisation reaction process, a pseudo-single step first order rate equation is fitted to the extent of reaction data, which reveals important mechanistic information regarding the role of free silica in the activators in the evolution of the binder systems. Hence, it is shown that in situ X-ray PDF analysis is an ideal experimental local structure tool to probe the reaction kinetics of complex reacting systems involving transitions between disordered/amorphous phases, of which geopolymerisation is an important example. C1 [White, Claire E.; Bloomer, Breaunnah; Page, Katharine] Los Alamos Natl Lab, Manuel Lujan Jr Neutron Scattering Ctr, Los Alamos, NM 87545 USA. [White, Claire E.; Henson, Neil J.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [White, Claire E.] Los Alamos Natl Lab, Ctr Nonlinear Studies, Los Alamos, NM 87545 USA. [Provis, John L.] Univ Sheffield, Dept Mat Sci & Engn, Sheffield, S Yorkshire, England. RP White, CE (reprint author), Los Alamos Natl Lab, Manuel Lujan Jr Neutron Scattering Ctr, Mailstop H805, Los Alamos, NM 87545 USA. EM whitece@lanl.gov RI Page, Katharine/C-9726-2009; Provis, John/A-7631-2008; White, Claire/A-1722-2011; OI Page, Katharine/0000-0002-9071-3383; Provis, John/0000-0003-3372-8922; White, Claire/0000-0002-4800-7960; Henson, Neil/0000-0002-1842-7884 FU Los Alamos National Laboratory; Los Alamos National Security LLC under DOE [DE-AC52-06NA25396]; Faculty of Engineering, University of Sheffield; U.S. Department of Energy through the LANL/LDRD Program; U.S. DOE Office of Science by Argonne National Laboratory, under U.S. DOE [DE-AC02-06CH11357] FX The authors thank Dr Karena Chapman and Kevin Beyer, ANL, for assistance with sample loading, data acquisition and data reduction on 11-ID-B at the APS, and Dr Dingwu Feng and Prof. Jannie van Deventer, University of Melbourne, for assistance in synthesis of slags and for valuable discussions. The participation of CEW, KP and NJH in this work was supported by Los Alamos National Laboratory, which is operated by Los Alamos National Security LLC under DOE Contract DE-AC52-06NA25396, and the participation of JLP was made possible by funding from the Faculty of Engineering, University of Sheffield. Furthermore, CEW gratefully acknowledges the support of the U.S. Department of Energy through the LANL/LDRD Program. The 11-ID-B beam line is located at the Advanced Photon Source, an Office of Science User Facility operated for the U.S. DOE Office of Science by Argonne National Laboratory, under U.S. DOE Contract No. DE-AC02-06CH11357. NR 56 TC 14 Z9 15 U1 2 U2 51 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 22 BP 8573 EP 8582 DI 10.1039/c3cp44342f PG 10 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 145HN UT WOS:000319006100014 PM 23450172 ER PT J AU Wilding, MC Wilson, M Benmore, CJ Weber, JKR McMillan, PF AF Wilding, Martin C. Wilson, Mark Benmore, Chris J. Weber, J. K. R. McMillan, Paul F. TI Structural changes in supercooled Al2O3-Y2O3 liquids SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID PRESSURE MOLECULAR-DYNAMICS; PHASE-TRANSITIONS; NEUTRON-DIFFRACTION; AB-INITIO; GLASS-TRANSITION; ALUMINUM-OXIDE; IONIC SYSTEMS; BOND-LATTICE; X-RAY; MODEL AB Structural changes in liquids between Al2O3 and Y2O3 are investigated as a function of the composition and during supercooling using high energy X-ray diffraction (HEXRD) techniques combined with containerless aerodynamic levitation. Many-body molecular dynamics simulation techniques utilizing potential models that incorporate anion polarization effects are applied to study the same liquid systems. The X-ray scattering experiments indicate a change in liquid structure during supercooling around a composition 20% Y2O3 (AlY20) that occurs over a narrow temperature interval. We have associated this change in structure with the onset of a liquid-liquid phase transformation. Analysis of the MD simulated structures has allowed the structure changes to be interpreted in terms of Al3+ and Y3+ coordination environments and particularly the Y3+-Y3+ structural correlations. We show that the incipient liquid-liquid phase transition behaviour is correlated with local density fluctuations that represent different coordination polyhedra surrounding oxygen ions. The difference in energy and volume associated with this sampling of high and low density basins in the underlying energy landscape is consistent with independent verifications of the volume and enthalpy differences between different amorphous forms. The differences in the high- and low-density configurations match the difference in diffraction patterns observed experimentally. C1 [Wilding, Martin C.] Aberystwyth Univ, Inst Math & Phys Sci, Aberystwyth SY23 3BZ, Dyfed, Wales. [Wilson, Mark] Univ Oxford, Phys & Theoret Chem Lab, Dept Chem, Oxford OX1 3QZ, England. [Benmore, Chris J.] Argonne Natl Lab, Xray Sci Div, Argonne, IL 60439 USA. [Weber, J. K. R.] Mat Dev Inc, Arlington Hts, IL 60004 USA. [McMillan, Paul F.] UCL, Dept Chem, London WC1H 0AJ, England. RP Wilding, MC (reprint author), Aberystwyth Univ, Inst Math & Phys Sci, Aberystwyth SY23 3BZ, Dyfed, Wales. OI Benmore, Chris/0000-0001-7007-7749 FU U.S. DOE, at the Advanced Photon Source, Argonne National Laboratory [DE-AC02-06CH11357] FX This work was supported by the U.S. DOE, at the Advanced Photon Source, Argonne National Laboratory under contract number DE-AC02-06CH11357. The authors thank Guy Jennings for technical help with the fast X-ray data acquisition. We would also like to thank Dr Stuart Kearns of the Department of Earth Sciences Department, University of Bristol for help with electron microprobe analysis. NR 74 TC 8 Z9 8 U1 1 U2 38 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2013 VL 15 IS 22 BP 8589 EP 8605 DI 10.1039/c3cp51209f PG 17 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA 145HN UT WOS:000319006100016 PM 23620162 ER EF